背景技术:
国际专利申请WO 2010/089055 A2和相应的欧洲专利申请EP 2393363 A2广泛地公开了通式(I)的含硫杂芳族酸类似物用于防治有用植物中的细菌性有害生物的用途。在20种不同的优选的具体化合物中,通式(I)尤其包含宿主防御诱导剂噻酰菌胺(tiadinil)(化合物I-1)和异噻菌胺(化合物I-15)。宿主防御诱导剂苯并噻二唑和烯丙苯噻唑(probenazole)未包含于式(I)中。此外,所述申请广泛地涉及多种细菌菌株,以及涉及待处理的多种植物。所述申请具体地仅涉及一个具体实施例,其中记载了化合物I-15(异噻菌胺)用于处理稻以抵御野油菜黄单胞菌稻致病变种(Xanthomonas campestris pv.oryzae)的用途。在WO 2010/089055 A2中未记载包含协同有效量的至少一种这类宿主防御诱导剂和至少一种生物防治剂的结合物用于防治有用植物中的细菌性有害生物的用途。本发明的发明人出乎意料地发现所述结合物在抵御植物中的细菌性有害生物方面的有益协同作用。
本申请人未公开的专利申请PCT/EP2013/050772涉及宿主防御诱导剂、优选异噻菌胺,用于防治所选择的有用植物中的所选择的细菌性有害生物的用途,且可被认为是相对于WO 2010/089055 A2的选择发明。在所述专利申请中未记载用于防治有用植物中的细菌性有害生物的包含协同有效量的至少一种宿主防御诱导剂和至少一种生物防治剂的结合物。
国际专利申请WO 98/21967 A1和相应的美国专利第5,869,042号广泛地公开了通过施用有效量的至少一种生物防治剂、例如产生抗生素的芽孢杆菌属(Bacillus sp.)细菌菌株AQ175(ATCC登录号55608)、AQ77(ATCC登录号55609)或AQ178(ATCC登录号53522)或由这些菌株产生的至少一种抗生素来预防或治疗植物中的地上真菌和细菌感染的方法。在所述申请中未提及此类芽孢杆菌属细菌菌株与至少一种宿主防御诱导剂的结合物。
此外,本申请人的若干未公开的专利申请如EP 12004160.3、EP 12197956.1、EP 12197951.2、EP 12197949.6、EP 12197945.4、EP 12197942.1、EP 12197941.3、EP 12197939.7、EP 12197141.0、EP 12197131.1、EP 12197132.9、EP 12197134.5、EP 12197135.2、EP 12197137.8、EP 12197139.4、EP 12169936.7涉及包含生物防治剂的结合物,特别是包含芽孢杆菌属细菌菌株的此类结合物,并且涉及此类生物防治剂与杀真菌剂和/或杀昆虫剂的结合物。
WO 98/50422的实施例13公开了包含枯草芽孢杆菌(Bacillus subtilis)AQ713(NRRL登录号B-21661)和嘧菌酯(azoxystrobin)的混合物的协同作用。
但是,这些专利申请均未涉及作为生物防治剂的此类芽孢杆菌属细菌菌株与至少一种宿主防御诱导剂的结合物。
现在,包含至少一种宿主防御诱导剂和至少一种生物防治剂的结合物的有益协同作用和新用途被本发明的发明人首次示出,且未被所提及的现有技术显而易见地提出。
在适宜或温暖和潮湿的气候中尤其会遭遇作为有用植物中的病原体的细菌,其在大量有用植物中导致细菌性病害,且在一些情况下造成相当大的经济损失。
例如,燕麦食酸菌(Acidovorax avenae)或荚壳伯克霍尔德氏菌(Burkholderia glumae)可感染稻,分别导致褐纹病或细菌性粒腐病。
由韧皮部杆菌属(Candidatus Liberibacter spp.)引起的柑橘绿化病害(黄龙病(HLB)、柑橘叶脉韧皮部退化(CVPD)、黄苗病、叶斑黄(在菲律宾)、libukin(在台湾)和柑橘顶枯病(在印度))可能是危害最大的柑橘病害,其极大地减产,破坏果实的经济价值并能够最终导致整株植物的死亡。韧皮部杆菌属是根瘤菌科(Rhizobiaceae)革兰氏阴性细菌的一个属。所述属的成员是植物病原体,主要依靠木虱(psyllids)传播。通过以下常见症状来区分所述病害:叶脉和邻近组织变黄;然后是整个叶片变黄或长斑;然后是过早脱叶、细枝顶枯、小根和侧根腐烂和活力降低;最终整株植物死亡。受影响的树木长得矮小、长出许多反季节花(其中大多数脱落)并产生体积小、形状不规则的果实,果皮厚而色淡,底部仍为绿色。这些树木产生的果实味苦。被感染的树木不会复原并且现在没有治愈方法。HLB的防治是基于使用内吸杀昆虫剂和接触杀昆虫剂预防性防治媒介生物(vector)。但是,这些化合物的功效和活性谱并不总是完全令人满意。新感染的树木在6-12个月的潜伏期之后表现出初期症状。此外,重要的是要根除受到感染的树木以防止木虱吸收病原体并传播病害。无法治愈黄龙病,而且因为被感染的柑橘植物难以维持、再生和研究,防治所述病害的尝试进展缓慢。农业研究局的研究者使用感染黄龙病的柠檬树来感染长春花植物以研究所述病害。长春花植物易于感染所述病害并且当在实验中用抗生素处理时其反应良好。根据将青霉素G钠和生物灭杀剂2,2-二溴-3-次氮基丙酰胺施用到被感染的长春花时观察到的阳性结果,研究者试验青霉素G钠和生物灭杀剂2,2-二溴-3-次氮基丙酰胺作为潜在的疗法对感染的柑橘植物的作用。HLB细菌仅在柑橘树木的韧皮部存活和繁殖。但是,迄今仅有几种杀细菌剂用于治疗性防治HLB,例如,国际申请WO 2011/029536A2涉及环状酮-烯醇抗韧皮部杆菌属的用途。
柑橘溃疡是一种感染柑橘物种的病害,其由细菌地毯草黄单胞菌柑橘致病变种(Xanthomonas axonopodis pv.citri)(=野油菜黄单胞菌柑橘致病变种(Xanthomonas campestris pv.citri))引起。感染导致柑橘树木(包括青柠、橙和葡萄柚)的叶、茎和果实的损害。尽管溃疡对人类无害,但是其显著影响柑橘树木的活力,导致叶和果实过早脱落;感染溃疡的果实可安全食用,但是其外表难看以致无法售出。由于在一个地区存在柑橘溃疡会引发直接的检疫管制,扰乱新鲜水果的运输,因而影响会愈发严重。柑橘溃疡被认为起源于亚洲-印度东南部。现在,柑橘溃疡也存在于日本、南非和中非、中东、孟加拉国、太平洋群岛、南美的一些国家和美国佛罗里达州。世界上的一些地区已经根除了柑橘溃疡,其他地区正在进行根除(破坏柑橘树林以尝试根除所述病害),但是所述病害在其出现的大多数地区仍在流行。由于柑橘溃疡传播迅速、对出口和国内贸易的损害和影响的可能性大,它是所有柑橘生长地区的重大威胁。
柑橘杂色褪绿病(CVC)是另一种影响整个南美(特别是巴西)的柑橘植物的柑橘病害。CVC由来自黄单胞菌科(Xanthomonadaceae)家族的细菌苛养木杆菌(Xylella fastidiosa)引起。CVC是系统性病害,其仅存活于植物木质部或其媒介生物内部。已表明苛养木杆菌可从甜橙的种子迁移到幼苗。在症状出现之前,CVC具有9-12个月的潜伏期。苛养木杆菌的自然传播通过半翅目(Hemiptera)中的几种尖头叶蝉(sharpshooter leafhopper)发生。猕猴桃产业受到假单胞菌属(Pseudomonas spp.)感染的广泛影响,例如,丁香假单胞菌猕猴桃致病变种(Pseudomonas syringae pv.actinidae,Psa)感染首先在新西兰以及日本和意大利被认定,在这些地区它极大损害了黄金猕猴桃。现在正在进行深入的研究并试验抵抗猕猴桃中Psa损害的可能的解决方案。
马铃薯块茎细菌性疮痂病(普通疮痂病)是马铃薯种植核心区的新出现的问题,其严重影响块茎质量。受影响的马铃薯块茎被评定为低劣品,在市场上价格低,在感染严重的情况下马铃薯难以售卖。农民们普遍认为,所述病害逐年增加。
例如,感染欧文氏菌属(Erwinia)可导致整个水果种植园(如苹果或梨)的死亡。还已知的是,由感染土壤杆菌而引起的马铃薯细菌软腐病、植物肿瘤形成,以及当谷物(例如,小麦或稻)、蔬菜或柑橘果实被黄单胞菌属(Xanthomonas)感染时引起的大量坏死性病害。
由假单胞菌属引起的细菌性病害、特别是蔬菜、树木果实和烟草中的病害,被认为是特别具有破坏性的。
抵抗细菌性有害生物的标准处理包括使用合成化学农药,特别是使用(常规的)抗生素,其通常是合成或半合成来源或天然来源,从活生物体中分离并纯化或被遗传工程化。这样的常规抗生素的实例包括例如链霉素、杀稻瘟菌素S或春雷霉素。这类常规抗生素的施用基本上是防治有用植物中的细菌的唯一有效方法。但是,仅在少数情况下采用这种方法,这是因为这些抗生素依赖于与人类和兽医医学中使用的抗生素相同的作用机制,因此对抗生素在植物保护中的使用有很大的保留。引起关注的是,促进抗性形成;此外,大多数常规抗生素价格昂贵并且经常尤其仅能通过使用生物技术方法来获得。
合成和半合成农药例如合成或半合成抗生素通常是非特异性的,因此能够作用于目标生物以外的生物,包括其他天然存在的有益生物。因为其化学性质,其还可能是有毒的和非生物可降解的。全世界的消费者逐渐意识到与化学物质残留相关的潜在的环境和健康问题,特别是在食品中。这导致减少使用化学(即合成的)农药或至少减少其使用量的来自消费者的压力增大。因此,需要管理食物链需求,同时仍然允许有效的害虫防治。
使用合成抗生素带来的另一个问题是重复及单独施用这类常规抗生素通常导致抗性微生物的选择。通常,这类菌株还对具有相同作用模式的其他活性成分具有交叉抗性。于是,使用所述活性化合物有效防治病原体不再可能。但是,具有新作用机制的活性成分又难以研发或研发成本昂贵。
病原体种群的抗性发展的风险以及对环境与人类健康的关注培养了在寻找用于防治植物病害的常规抗生素的替代物方面的兴趣。使用生物防治剂(生物防治剂)是一种可选方案。然而,大多数生物防治剂的有效性尚未达到与常规抗生素相同的水平,特别是在严重感染压力的情况下。因此,已知的生物防治剂、其突变体和由其产生的代谢产物并不能完全令人满意,特别是在低施用率下。
另一种用于防治植物中的细菌的方法旨在使用氧氯化铜,其是不利的,这是因为在标准处理中必须施用高剂量。氧氯化铜例如在番茄保护中用于防治丁香假单胞菌(Pseudomonas syringae)。此外,氧氯化铜被认为是植物毒性的,并且因为已知它会在土壤中累积,所以它的使用越来越受到限制。此外,氧氯化铜制剂通常会在叶和果实上留下明显的残留物,这不被消费者欣赏和接受。
因此,非常需要具有改进效果的用于防治有用植物中的细菌性病害的特别有效的方法,此外该方法仅需要少量待施用物质,此外不损害植物或不损害人类或动物健康。
在本文中,特别关注这类新型结合物的提高的杀细菌活性和协同作用,以及快速功效和长期功效的结合,以增大在施用时间以及最小化散播在环境中的化学产品的剂量以及减少处理成本方面的灵活性。
现已发现,包含协同有效量的至少一种宿主防御诱导剂(例如,优选异噻菌胺或异噻菌胺和苯并噻二唑的结合物)和至少一种生物防治剂(例如,优选枯草芽孢杆菌菌株QST713/AQ713(NRRL登录号B21661)、枯草芽孢杆菌菌株AQ153(NRRL登录号55614)、芽孢杆菌属菌株AQ175(ATCC登录号55608)、芽孢杆菌属菌株AQ177(ATCC登录号55609)、芽孢杆菌属菌株AQ178(ATCC登录号53522)和Pseudozyma aphidisin)的结合物特别适用于防治有用植物中的细菌性有害生物。
此外,发现一种处理植物的方法特别适用于防治有用植物中的细菌性有害生物,所述方法包括对待保护以免受细菌性有害生物侵袭的植物进行两个以上的依次处理区段,其中至少一个处理区段包括用至少一种宿主防御诱导剂对植物进行至少一次处理,并且至少一个处理区段包括用至少一种生物防治剂对植物进行至少一次处理。根据一个优选的实施方案,发现一种处理植物的方法特别适用于防治有用植物中的细菌性有害生物,所述方法包括对待保护以免受细菌性有害生物侵袭的植物进行两个以上的依次处理区段,其中至少一个处理区段包括用至少一种宿主防御诱导剂对植物进行至少一次处理,并且至少一个处理区段包括用至少一种生物防治剂对植物进行至少一次处理,条件是最后一个处理区段包括用至少一种生物防治剂对植物进行至少一次处理。
待解决的问题
本发明的目的是提供在防治有用植物中的细菌性有害生物方面具有优异效果的新型活性化合物结合物,以及提供新的处理方法。
技术实现要素:
本发明的问题已通过提供新型的用于防治有用植物中的细菌性有害生物的活性化合物结合物而得到解决,所述结合物包含协同有效量的
(A)至少一种宿主防御诱导剂和
(B)至少一种生物防治剂。
宿主防御诱导剂
在本发明中,宿主防御诱导剂是指这样的化合物:其特征在于能够刺激植物自身的防御机制以保护植物抵御感染。因此,宿主防御诱导剂用于诱导已知为植物防御诱导剂的早期基因和强化(strongly)基因。它们使植物在病原体侵袭后更强和/或更快地诱导防御基因。根据本发明,宿主防御诱导剂包括,例如,
苯并噻二唑:
异噻菌胺:
烯丙苯噻唑:
噻酰菌胺:
昆布多糖(Laminarin):
优选地,至少一种宿主防御诱导剂(A)选自A.1苯并噻二唑、A.2异噻菌胺、A.3烯丙苯噻唑和A.4噻酰菌胺或其组合,更优选地,至少一种宿主防御诱导剂(A)是A.2异噻菌胺。在另一个优选的实施方案中,至少一种宿主防御诱导剂(A)是A.2异噻菌胺和A.1苯并噻二唑的结合物。
如果适合,本发明的宿主防御诱导剂(A)可以以可能的多种异构形式、特别是立体异构体如旋光异构体的混合物形式存在。
生物防治剂
本文中所使用的“生物防治”被定义为通过使用第二种生物来防治植物致病生物例如病原体和/或昆虫和/或螨虫和/或线虫。已知的生物防治机制包括肠道细菌,其通过在根部表面与真菌竞争赢得空间来防治根腐病。细菌毒素如抗生素已用于防治病原体。毒素可被分离并直接施用于植物,或者给予细菌物种使其在原位产生毒素。
通常,“杀虫”意指物质提高植物害虫的死亡率或抑制植物害虫的生长速率的能力。在本文中,该术语用于描述物质对昆虫、螨虫、线虫和/或植物病原体具有活性的性质。就本发明来说,术语“害虫”包括昆虫、螨虫、线虫和/或植物致病细菌。
“杀昆虫剂”和术语“杀昆虫”是指物质提高昆虫的死亡率或抑制昆虫的生长速率的能力。本文中使用的术语“昆虫”包括“昆虫纲”的所有生物。术语“成年前”昆虫是指生物在进入成年阶段之前的任何形式,包括,例如,卵、幼虫和若虫。
“杀线虫剂”和“杀线虫”是指物质提高线虫死亡率或抑制线虫生长速率的能力。通常,术语“线虫”包括所述生物的卵、幼虫、幼体形态及成熟形态。
“杀螨剂”或“杀螨”是指物质提高属于蛛形纲、蜱螨亚纲的体外寄生虫的死亡率或抑制其生长速率的能力。
术语“代谢产物”是指具有杀虫活性的微生物发酵的任何化合物、物质或副产物。
术语“突变体”是指亲代菌株的变体,以及用来获得杀虫活性比亲代菌株表达出的杀虫活性更高的突变体或变体的方法。在本文中,“亲代菌株”定义为诱变之前的原始菌株。为了获得这样的突变体,可以使用化学品,如N-甲基-N'-硝基-N-亚硝基胍、乙基甲砜(ethylmethanesulfone),或通过γ射线、X射线或UV辐射,或通过本领域技术人员熟知的其他方法来处理亲代菌株。
“变体”是指具有如文中所示的NRRL或ATCC登录号的所有识别特征的菌株,其可被认定为具有在高严紧性条件下同NRRL或ATCC登录号的基因组杂交的基因组。
“杂交”是指其中一个或多个多核苷酸反应形成复合物的反应,所述复合物通过核苷酸残基的碱基之间的氢键而稳定。氢键可以通过Watson-Crick碱基配对、Hoogstein结合或任何其他序列特异性的方式发生。所述复合物可包括形成双链结构的两条链、形成多链复合物的三条或更多条链、可自杂交的单链、或上述的任何组合。杂交反应可在不同的“严紧性”条件下进行。通常,低严紧性杂交反应在约40℃、10×SSC中进行,或在具有相当的离子强度/温度的溶液中进行。中严紧性杂交通常在6×SSC中在约50℃下进行,并且高严紧性杂交反应通常在1×SSC中在约60℃下进行。
所示NRRL或ATCC登录号的变体还可被定义为这样的菌株,其基因组序列与所示NRRL或ATCC登录号的基因组的序列一致性大于85%,更优选大于90%或者更优选大于95%。多核苷酸或多核苷酸区域(或者多肽或多肽区域)与另一序列具有一定的“序列一致性”百分比(例如,80%、85%、90%、95%)意指,当二者排列在一起比对时,该百分比的碱基(或氨基酸)相同。所述比对和同源百分比或序列一致性可使用本领域中已知的软件程序来确定,例如,Current Protocols in Molecular Biology(F.M.Ausubel et al.,eds.,1987)Supplement 30,section 7.7.18,Table 7.7.1.中所记载的那些程序。
NRRL是美国农业研究菌种保藏中心的简称,是《国际承认用于专利程序的微生物保存布达佩斯公约》之下的用于保藏微生物菌株的国际权威保存机构,其地址是:美国伊利诺伊州Peroira市北部大学街1815号,美国农业部农业研究服务局农业应用国家中心,邮编61604。
ATCC是美国标准生物品收藏中心的简称,是《国际承认用于专利程序的微生物保存布达佩斯公约》之下用于保藏微生物菌株的国际权威保存机构,其地址是:美国弗吉尼亚州马纳萨斯市大学林荫大道10801号ATCC专利保藏中心,邮编10110。
生物防治剂特别包括细菌、真菌和/或酵母、原生动物、病毒、昆虫病原线虫、接种剂(Inoculant)和植物药(botanical),和/或具有各菌株所有识别特征的菌株突变体,和/或由各菌株产生的表现出抗细菌性有害生物、昆虫、螨虫、线虫和/或植物病原体活性的代谢产物。
根据本发明,生物防治剂(B)特别地选自1)细菌和2)真菌(包括酵母)。
1)细菌
根据本发明,被归类于术语“细菌”之下的生物防治剂包括形成孢子的根定殖细菌,或适于用作改善植物健康和生长的生物杀昆虫剂、杀线虫剂、杀螨剂、杀真菌剂或土壤改良剂的细菌及其代谢产物。根据本发明使用或利用的这类细菌的实例为(在以下全部本发明的说明书中延用编号):
B.1.1枯草芽孢杆菌,特别是菌株QST713/AQ713(可作为SERENADE MAX从Bayer CropScience LP,US获得,NRRL登录号B21661,记载于美国专利第6,060,051号中);B.1.2枯草芽孢杆菌菌株AQ153(NRRL登录号55614并记载于美国专利第5,753,222号中);B.1.3芽孢杆菌属菌株AQ175(ATCC登录号55608并记载于美国专利第5,869,042号中);B.1.4芽孢杆菌属菌株AQ177(ATCC登录号55609并记载于美国专利第5,869,042号中);B.1.5芽孢杆菌属菌株AQ178(ATCC登录号53522并记载于美国专利第5,869,042号中);B.1.6解淀粉芽孢杆菌(Bacillus amyloliquefaciens),菌株D747(可作为从Etec Crop Solutions,NZ获得,也可作为Double NickelTM从Certis,US获得,登录号FERM BP-8234,参见美国专利第7,094,592号的摘要);B.1.7短小芽孢杆菌(Bacillus pumilus),特别是菌株BU F-33(可作为Integral F-33从Becker Underwood,US获得,登录号B-50185);B.1.8解淀粉枯草芽孢杆菌变种(B.subtilis var.amyloliquefaciens)菌株FZB24(可作为从Novozymes,US获得,登录号000-00-9002);B.1.9苏云金芽孢杆菌(B.thuringiensis)菌株AQ52,其购自AgraQuest,US(登录号NRRL B-21619);B.1.10多粘类芽孢杆菌(Paenibacillus polymyxa),特别是菌株AC-1(可作为Topseed从Green Biotech Company Ltd.获得,参见WO2013010322A1);B.1.11Pseudomonas proradix(可作为从Sourcon Padena获得,登录号PRORADIX-DSM 13134(参见美国专利第6,916,650号的权利要求1);B.1.12解淀粉芽孢杆菌,特别是菌株IN937a;B.1.13产氮芽孢杆菌(Bacillus azotoformans);B.1.14斯密氏芽孢杆菌(Bacillus smithii);B.1.15枯草芽孢杆菌,特别是菌株DB 101;B.1.16抗生素溶杆菌(Lysobacter antibioticus),特别是菌株13-1(参见Biological Control 2008,45,288-296);B.1.17成团泛菌(Pantoea agglomerans),特别是菌株E325(登录号NRRL B-21856)。
优选的细菌为B.1.1枯草芽孢杆菌,特别是菌株QST713/AQ713(可作为SERENADE MAX从Bayer CropScience LP,US获得,NRRL登录号B21661,记载于美国专利第6,060,051号中);B.1.2枯草芽孢杆菌菌株AQ153(NRRL登录号55614并记载于美国专利第5,753,222号中);B.1.3芽孢杆菌属菌株AQ175(ATCC登录号55608并记载于美国专利第5,869,042号中);B.1.4芽孢杆菌属菌株AQ177(ATCC登录号55609并记载于美国专利第5,869,042号中);B.1.5芽孢杆菌属菌株AQ178(ATCC登录号53522并记载于美国专利第5,869,042号中);B.1.6解淀粉芽孢杆菌,菌株D747(可作为从Etec Crop Solutions,NZ获得,也可作为Double NickelTM从Certis,US获得);B.1.7短小芽孢杆菌,特别是菌株BU F-33(可作为Integral F-33从Becker Underwood,US获得);B.1.8解淀粉枯草芽孢杆菌变种菌株FZB24(可作为从Novozymes,US获得);B.1.9苏云金芽孢杆菌菌株AQ52,其购自AgraQuest,US(登录号NRRL B-21619);B.1.10多粘类芽孢杆菌,特别是菌株AC-1(可作为Topseed从Green Biotech Company Ltd.获得);B.1.11Pseudomonas proradix(可作为从Sourcon Padena获得)。
特别优选的细菌是B.1.1枯草芽孢杆菌,特别是菌株QST713/AQ713(可作为SERENADE MAX从Bayer CropScience LP,US获得,NRRL登录号B21661,记载于美国专利第6,060,051号中);B.1.2枯草芽孢杆菌菌株AQ153(NRRL登录号55614并记载于美国专利第5,753,222号中);B.1.3芽孢杆菌属菌株AQ175(ATCC登录号55608并记载于美国专利第5,869,042号中);B.1.4芽孢杆菌属菌株AQ177(ATCC登录号55609并记载于美国专利第5,869,042号中);B.1.5芽孢杆菌属菌株AQ178(ATCC登录号53522并记载于美国专利第5,869,042号中)。
最优选的细菌是B.1.1枯草芽孢杆菌,特别是菌株QST713/AQ713(可作为SERENADE MAX从Bayer CropScience LP,US获得,NRRL登录号B21661,记载于美国专利第6,060,051号中)。
已知,记载于WO 98/21697 A1中的细菌菌株芽孢杆菌属AQ175(ATCC登录号55608)、芽孢杆菌属AQ177(ATCC登录号55609)和芽孢杆菌属AQ178(ATCC登录号53522)在治疗和保护植物免受地上真菌和细菌感染方面是有效的。
枯草芽孢杆菌AQ713(登录号B-21661),也被命名为枯草芽孢杆菌QST713,表现出广泛的杀真菌和杀细菌活性,也表现出玉米根虫活性(WO 98/50422 A1)。该菌株的市售制剂可以商品名MAX、Soil、ASO、CPB和从Bayer CropScience LP,US(之前为AgraQuest,Inc.USA)获得。ASO是枯草芽孢杆菌菌株的液体制剂,而Max是干制剂。可相互交换使用这两种产品来抵御细菌性病害。
所述商业产品的各自配方如以下所示:
ASO:
水性悬浮液/ASO=水性悬浮液有机物
活性成分:
枯草芽孢杆菌的QST 713菌株* 1.34%
其他成分 98.66%
总计 100.00%
*包含最小1×109cfu/g
美国专利第6,060,051号、第6,103,228号、第6,291,426号和第6,417,163号关于枯草芽孢杆菌的QST 713菌株。
MAX:
可湿性粉剂
活性成分:
干燥的枯草芽孢杆菌的QST 713菌株* 14.6%
其他成分 85.4%
总计 100.0%
*包含最小7.3×109cfu/g
美国专利第6,060,051号、第6,103,228号、第6,291,426号和第6,417,163号关于枯草芽孢杆菌的QST 713菌株。
Soil:
水性悬浮液
活性成分:
干燥的枯草芽孢杆菌的QST 713菌株* 1.34%
其他成分 98.66%
总计 100.00%
*包含最小1×109cfu/g
美国专利第6,060,051号、第6,103,228号、第6,291,426号和第6,417,163号关于枯草芽孢杆菌的QST 713菌株。
已知,枯草芽孢杆菌的杀细菌活性抵御细菌性叶斑病(黄单胞菌属(Xanthemonas))、疮痂病(黑星菌属(venturia))、火疫病(欧文氏菌属(Erwinia))、假单胞菌属、细菌性萎蔫病(罗尔斯通氏菌属(Ralstonia))、溃疡(包括柑橘溃疡,由韧皮部杆菌属引起)。作用模式包括广泛的抗真菌活性、引起植物应答——ISR(诱导性系统抗性)、叶的定殖和病原体的竞争(out-competition)。可与以下物质进行桶混:例如杀真菌剂,如嘧菌酯、啶酰菌胺(boscalid)和唑菌胺酯(pyraclostrobin)、百菌清(chlorothalonil)、嘧菌环胺(cyprodinil)、异菌脲(iprodione)、腈菌唑(myclobutanil)、碳酸氢钾、硫;杀昆虫剂,如阿维菌素(abamectin)、苏云金芽孢杆菌、多杀霉素(Spinosad)。应避免与乙膦酸铝(Fosetyl-Al)的桶混,原因在于这会导致孢子沉淀。因此,在一个优选的实施方案中,排除本发明的结合物与乙膦酸铝的桶混。
WO 98/21964 A1中所记载的枯草芽孢杆菌AQ153(ATCC登录号55614)在抑制植物致病细菌和真菌的生长方面是有效的。
根据WO 98/21965 A1,产生抗生素的菌株苏云金芽孢杆菌AQ52(NRRL登录号B-21619)表现出广泛的杀真菌和杀细菌活性。
2)真菌和/或酵母
根据本发明,被归类于术语“真菌”和/或“酵母”之下的生物防治剂为例如以下生物,和/或具有各菌株全部识别特征的菌株突变体,和/或由各菌株产生的表现出抗昆虫、螨虫、线虫和/或植物病原体活性的代谢产物(在整个说明书中延用编号):
B.2.1Pseudozyma aphidis(参见WO2011151819A2);B.2.2出芽短梗霉菌(Aureobasidium pullulans),特别是菌株DSM14940的芽生孢子;B.2.3菌株DSM 14941的出芽短梗霉菌芽生孢子,或其混合物;B.2.4酿酒酵母(Saccharomyces cerevisiae),特别是菌株CNCM号I-3936;B.2.5酿酒酵母,特别是菌株CNCM号I-3937;B.2.6酿酒酵母,特别是菌株CNCM号I-3938;B.2.7酿酒酵母,特别是菌株CNCM号I-3939;B.2.8黄硬皮马勃(Scleroderma citrinum)。
优选真菌为B.2.1Pseudozyma aphidis。
因此,根据本发明,优选结合物,其中生物防治剂(B)选自
1)由B.1.1枯草芽孢杆菌,特别是菌株QST713/AQ713(可作为SERENADE MAX从Bayer CropScience LP,US获得,NRRL登录号B21661,记载于美国专利第6,060,051号中);B.1.2枯草芽孢杆菌菌株AQ153(NRRL登录号55614并记载于美国专利第5,753,222号中);B.1.3芽孢杆菌属菌株AQ175(ATCC登录号55608并记载于美国专利第5,869,042号中);B.1.4芽孢杆菌属菌株AQ177(ATCC登录号55609并记载于美国专利第5,869,042号中);B.1.5芽孢杆菌属菌株AQ178(ATCC登录号53522并记载于美国专利第5,869,042号中);B.1.6解淀粉芽孢杆菌,菌株D747(可作为从Etec Crop Solutions,NZ获得,也可作为Double NickelTM从Certis,US获得);B.1.7短小芽孢杆菌,特别是菌株BU F-33(可作为Integral F-33从Becker Underwood,US获得);B.1.8解淀粉枯草芽孢杆菌变种菌株FZB24(可作为从Novozymes,US获得);B.1.9苏云金芽孢杆菌菌株AQ52,其购自AgraQuest,US(登录号NRRL B-21619);B.1.10多粘类芽孢杆菌,特别是菌株AC-1(可作为Topseed从Green Biotech Company Ltd.获得);B.1.11Pseudomonas proradix(可作为从Sourcon Padena获得)组成的细菌;以及
2)由B.2.1Pseudozyma aphidis组成的真菌。
甚至更优选结合物,其中生物防治剂(B)选自
1)由B.1.1枯草芽孢杆菌,特别是菌株QST713/AQ713(可作为SERENADE MAX从Bayer CropScience LP,US获得,NRRL登录号B21661,记载于美国专利第6,060,051号中);B.1.2枯草芽孢杆菌菌株AQ153(NRRL登录号55614并记载于美国专利第5,753,222号中);B.1.3芽孢杆菌属菌株AQ175(ATCC登录号55608并记载于美国专利第5,869,042号中);B.1.4芽孢杆菌属菌株AQ177(ATCC登录号55609并记载于美国专利第5,869,042号中);B.1.5芽孢杆菌属菌株AQ178(ATCC登录号53522并记载于美国专利第5,869,042号中)组成的细菌;以及
2)由B.2.1Pseudozyma aphidis组成的真菌。
最优选结合物,其中生物防治剂(B)选自
1)由B.1.1枯草芽孢杆菌,特别是菌株QST713/AQ713(可作为SERENADE MAX从Bayer CropScience LP,US获得,NRRL登录号B21661,记载于美国专利第6,060,051号中)组成的细菌;以及
2)由B.2.1Pseudozyma aphidis组成的真菌。
其他生物防治剂特别包括原生动物、病毒、昆虫病原线虫和植物药,和/或其突变体。
3)原生动物
根据本发明,被归类于术语“原生动物”之下的生物防治剂为以下实例(在整个说明书中延用编号):
B.3.1蝗虫微孢子虫(Nosema locustae)(产品已知为NoloBait),B.3.2泰罗汉孢虫属火蚁(Thelohania solenopsis)和B.3.3变形孢虫属(Vairimorpha spp.)。
4)病毒
根据本发明,被归类于术语“病毒”之下的生物防治剂为以下实例。它们包括具有各菌株全部识别特征的菌株突变体,和/或由各菌株产生的表现出抗昆虫、螨虫、线虫和/或植物病原体活性的代谢产物(在整个说明书中延用编号):
B.4.1棉褐带卷蛾(Adoxophyes orana)(夏季果实卷叶蛾)颗粒体病毒(GV)(产品已知为BIOFA-),B.4.2黄地老虎(Agrotis segetum)(芜菁蛾)核型多角体病毒(NPV),B.4.3大豆夜蛾(Anticarsia gemmatalis)(Woolly pyrol moth)mNPV(产品已知为Polygen),B.4.4苜蓿银纹夜蛾(Autographa californica)(苜蓿尺蠖)mNPV(产品已知为来自Agricola El Sol的VPN80),B.4.5油桐尺蠖(Biston suppressaria)(茶尺蠖)NPV,B.4.6家蚕(Bombyx mori)(蚕)NPV,B.4.7苹果异形小卷蛾(Cryptophlebia leucotreta)(伪苹果小卷蛾(false codling moth))GV(产品已知为Cryptex),B.4.8苹果蠹蛾(Cydia pomonella)(苹果蠹蛾(Codling moth))颗粒体病毒(GV)(产品已知为Madex Plus),B.4.9马尾松毛虫(Dendrolimus punctatus)(马尾松蛾)CPV,B.4.10棉铃虫(Helicoverpa armigera)NPV(产品已知为AgBiTech-ViVUS Max),B.4.11棉铃虫(Helicoverpa zea,之前写作Heliothis zea)(玉米棉铃虫(corn earworm))NPV(产品已知为Elcar),B.4.12柳毒蛾(Leucoma salicis)(柳毒蛾(satin moth))NPV,B.4.13舞毒蛾(Lymantria dispar)(舞毒蛾(gypsy moth))NPV(产品已知为Gypcheck),B.4.14冷杉叶蜂(Neodiprion abietis)(香脂冷杉叶蜂)NPV(产品已知为Abietiv),B.4.15红头松叶蜂(Neodiprion lecontei)(红头松叶蜂(red-headed pinesawfly))NPV(产品已知为Lecontvirus),B.4.16松黄叶蜂(Neodiprion sertifer)(松黄叶蜂(Pine sawfly))NPV(产品已知为Neocheck-S),B.4.17黄杉毒蛾(Orgyia pseudotsugata)(黄杉毒蛾(Douglas-fir tussock moth))NPV(产品已知为Virtuss),B.4.18马铃薯块茎蛾(Phthorimaea operculella)(烟潜夜蛾)GV(产品已知为Matapol),B.4.19菜粉蝶(Pieris rapae)(菜粉蝶(small white))GV,B.4.20小菜蛾(Plutella xylostella)(菱形斑纹蛾)GV(产品已知为Plutec),B.4.21灰纹夜蛾(Spodoptera albula)(灰纹夜蛾)mNPV(产品已知为VPN 82),B.4.22莎草粘虫(Spodoptera exempta)(真粘虫(true armyworm))mNPV(产品已知为Spodec),B.4.23甜菜夜蛾(Spodoptera exigua)(甜菜夜蛾(sugarbeet armyworm))mNPV(产品已知为Spexit,来自Andermatt Biocontrol),B.4.24草地贪夜蛾(Spodoptera frugiperda)(草地贪夜蛾(fall armyworm))mNPV(产品已知为Baculovirus VPN),B.4.25海灰翅夜蛾(Spodoptera littoralis)(烟草夜蛾)NPV(产品已知为Spodoptrin,来自NPP Calliope France),以及B.4.26东方叶蛾(Spodoptera litura)(东方叶蛾(oriental leafworm moth))NPV(产品已知为Littovir)。
5)昆虫病原线虫
根据本发明,被归类于术语“昆虫病原线虫”之下的生物防治剂为(在整个说明书中延用编号):
B.5.1Abbreviata caucasica,B.5.2锐形线虫属(Acuaria spp.),B.5.3脱尾多索线虫(Agamermis decaudata),B.5.4腊肠形线虫属(Allantonema spp.),B.5.5两索线虫属(Amphimermis spp.),B.5.6Beddingia(=Deladenus)siridicola,B.5.7博温线虫属(Bovienema spp.),B.5.7Cameronia spp.,B.5.8Chitwoodiella ovofilamenta,B.5.9Contortylenchus spp.,B.5.10Culicimermis spp.,B.5.11双三齿线虫属(Diplotriaena spp.),B.5.12Empidomermis spp.,B.5.13Filipjevimermis leipsandra,B.5.14胃索线虫属(Gastromermis spp.),B.5.15筒线虫属(Gongylonema spp.),B.5.16Gynopoecilia pseudovipara,B.5.17异小杆线虫属(Heterorhabditis spp.),特别是异小杆线虫(Heterorhabditis bacteriophora)(产品已知为B-Green)、或Heterorhabditis baujardi、或Heterorhabditis heliothidis(产品已知为Nematon)、或Heterorhabditis indica、Heterorhabditis marelatus、Heterorhabditis megidis、Heterorhabditis zealandica,B.5.18六索线虫属(Hexamermis spp.),B.5.19水索线虫属(Hydromermis spp.),B.5.20等索线虫属(Isomermis spp.),B.5.21Limnomermis spp.,B.5.22Maupasina weissi,B.5.23黑色索线虫(Mermis nigrescens),B.5.24中索线虫属(Mesomermis spp.),B.5.25新中索线虫属(Neomesomermis spp.),B.5.26Neoparasitylenchus rugulosi,B.5.27奥克托索线虫属(Octomyomermis spp.),B.5.28寄生滑刃属(Parasitaphelenchus spp.),B.5.29Parasitorhabditis spp.,B.5.30寄生垫刃属(Parasitylenchus spp.),B.5.31蚊镒索线虫(Perutilimermis culicis),B.5.32Phasmarhabditis hermaphrodita,B.5.33泡翼线虫属(Physaloptera spp.),B.5.34Protrellatus spp.,B.5.35Pterygodermatites spp.,B.5.36罗马索线虫属(Romanomermis spp.),B.5.37Seuratum cadarachense,B.5.38园线虫属(Sphaerulariopsis spp.),B.5.39Spirura guianensis,B.5.40斯氏线虫属(Steinernema spp.)(=新线虫属(Neoaplectana spp.)),特别是小卷蛾斯氏线虫(Steinernema carpocapsae)(产品已知为Biocontrol)、或夜蛾斯氏线虫(Steinernema feltiae)(=小卷蛾新线虫(Neoaplectana carpocapsae)),(产品已知为)、或格氏线虫(Steinernema glaseri)(产品已知为Biotopia)、或锯蜂线虫(Steinernema kraussei)(产品已知为Larvesure)、或Steinernema riobrave(产品已知为Biovector)、或Steinernema scapterisci(产品已知为Nematac S)、或斯氏线虫(Steinernema scarabaei)、或Steinernema siamkayai,B.5.41Strelkovimermis peterseni,B.5.42锥尾线虫属(Subulura spp.),B.5.43Sulphuretylenchus elongatus,以及B.5.44四棱线虫属(Tetrameres spp.)。
在本发明的含义中,至少一种生物防治剂(B)不仅包括各微生物的分离的纯培养物,还包括在全培养物(whole broth culture)中的它们的悬浮液或包含代谢产物的上清液或从菌株的全培养物获得的纯化的代谢产物。“全培养物”指包含细胞和培养基的液体培养物。“上清液”指当通过离心、过滤、沉淀或本领域熟知的其他方法除去生长在培养基中的细胞后的液体培养基残余物。
以上提及的由非致病微生物产生的代谢产物包括抗生素、酶、铁载体(siderophore)和生长促进剂,例如双效菌素(zwittermicin-A)、卡那霉素水解物、多氧菌素(polyoxine)、酶(例如α-淀粉酶、几丁质酶和果胶酶),植物激素及其前体(例如植物生长素、赤霉素类化合物、细胞分裂素类化合物)、脂肽(如伊枯草菌素、plipastatins)或表面活性肽,例如,阿瓜斯他汀A(agrastatin A)、芽孢菌霉素D、杆菌溶素、地非西丁、大环内酰亚胺(macrolactin)、丰原素、杆菌溶素和bacilaene。以上列出的脂肽的优选代谢产物特别是由短小芽孢杆菌(NRRL登录号B-30087)、枯草芽孢杆菌AQ713(NRRL登录号B-21661)、枯草芽孢杆菌菌株AQ30002(aka QST30002;NRRL登录号B-50421)或枯草芽孢杆菌菌株AQ30004(aka QST30004;NRRL登录号No.B-50455)产生。
根据本发明,可利用或使用任何生理状态、例如活性的或休眠的生物防治剂。
本发明的结合物特别适用于防治细菌性有害生物。根据本发明,细菌性有害生物尤其包括对植物或植物部位造成损害的细菌。
细菌尤其包括放线菌门(Actinobacteria)和蛋白细菌门(Proteobacteria),并且选自伯克霍尔德氏菌科(Burkholderiaceae)、黄单胞菌科(Xanthomonadaceae)、假单胞菌科(Pseudomonadaceae)、肠杆菌科(Enterobacteriaceae)、微杆菌科(Microbacteriaceae)和根瘤菌科(Rhizobiaceae)。
根据本发明,所述细菌性有害生物特别选自:
燕麦食酸菌(Acidovorax avenae)(=燕麦假单胞菌(Pseudomonas avenae)、燕麦假单胞菌燕麦亚种(Pseudomonas avenae subsp.avenae)、红纹假单胞菌(Pseudomonas rubrilineans)),包括例如,燕麦食酸菌燕麦亚种(Acidovorax avenae subsp.avenae)(=燕麦假单胞菌燕麦亚种)、燕麦食酸菌卡特莱兰亚种(Acidovorax avenae subsp.cattleyae)(=卡特莱兰假单胞菌(Pseudomonas cattleyae))、燕麦食酸菌西瓜亚种(Acidovorax avenae subsp.citrulli)(=类产碱假单胞菌西瓜亚种(Pseudomonas pseudoalcaligenes subsp.citrulli)、燕麦假单胞菌西瓜亚种(Pseudomonas avenae subsp.citrulli));
伯克霍尔德氏菌属(Burkholderia spec.),包括例如,须芒草伯克霍尔德氏菌(Burkholderia andropogonis)(=须芒草假单胞菌(Pseudomonas andropogonis)、伍氏假单胞菌(Pseudomonas woodsii))、石竹伯克霍尔德氏菌(Burkholderia caryophylli)(=石竹假单胞菌(Pseudomonas caryophylli))、洋葱伯克霍尔德氏菌(Burkholderia cepacia)(=洋葱假单胞菌(Pseudomonas cepacia))、唐菖蒲伯克霍尔德氏菌(Burkholderia gladioli)(=唐菖蒲假单胞菌(Pseudomonas gladioli))、Burkholderia gladioli pv.agaricicola(=Pseudomnas gladioli pv.agaricicola)、唐菖蒲伯克霍尔德氏菌葱生致病变种(Burkholderia gladioli pv.alliicola)(=唐菖蒲假单胞菌葱生致病变种(Pseusomonas gladioli pv.alliicola))、唐菖蒲伯克霍尔德氏菌唐菖蒲致病变种(Burkholderia gladioli pv.gladioli)(=唐菖蒲假单胞菌、唐菖蒲假单胞菌唐菖蒲致病变种(Pseudomonas gladioli pv.gladioli))、荚壳伯克霍尔德氏菌(Burkholderia glumae)(=荚壳假单胞菌(Pseudomonas glumae))、植物伯克霍尔德氏菌(Burkholderia plantarii)(=植物假单胞菌(Pseudomonas plantarii))、茄伯克霍尔德氏菌(Burkholderia solanacearum)(=茄罗尔斯通氏菌(Ralstonia solanacearum))和罗尔斯通氏菌属(Ralstonia spp.);
Liberibacter属,包括韧皮部杆菌属,包括例如,非洲韧皮部杆菌(Liberibacter africanus(Laf))、美洲韧皮部杆菌(Liberibacter americanus(Lam))、亚洲韧皮部杆菌(Liberibacter asiaticus(Las))、欧洲韧皮部杆菌(Liberibacter europaeus(Leu))、Liberibacter psyllaurous、茄韧皮部杆菌(Liberibacter solanacearum(Lso));
棒杆菌属(Corynebacterium),包括例如,聚集棒杆菌(Corynebacterium fascians)、萎蔫棒杆菌萎蔫致病变种(Corynebacterium flaccumfaciens pv.flaccumfaciens)、密执安棒杆菌(Corynebacterium michiganensis)、密执安棒杆菌小麦致病变种(Corynebacterium michiganense pv.tritici)、密执安棒杆菌尼布拉斯加致病变种(Corynebacterium michiganense pv.nebraskense)、腐烂棒杆菌(Corynebacterium sepedonicum);
欧文氏菌属(Erwinia spec.),包括例如,解淀粉欧文氏菌(Erwinia amylovora)、菠萝欧文氏菌(Erwinia ananas)、胡萝卜软腐欧文氏菌(Erwinia carotovora)(=胡萝卜果胶杆菌(Pectobacterium carotovorum))、胡萝卜软腐欧文氏菌黑腐亚种(Erwinia carotovora subsp.atroseptica)、胡萝卜软腐欧文氏菌胡萝卜软腐亚种(Erwinia carotovora subsp.carotovora)、菊欧文氏菌(Erwinia chrysanthemi)、菊欧文氏菌玉米致病变种(Erwinia chrysanthemi pv.zeae)、溶解欧文氏菌(Erwinia dissolvens)、草生欧文氏菌(Erwinia herbicola)、大黄欧文氏菌(Erwinia rhapontic)、斯氏欧文氏菌(Erwinia stewartii)、嗜管欧文氏菌(Erwinia tracheiphila)、嗜夏孢欧文氏菌(Erwinia uredovora);
丁香假单胞菌(Pseudomonas syringae),包括例如,丁香假单胞菌猕猴桃致病变种(Pseudomonas syringae pv.actinidiae)(Psa)、丁香假单胞菌致黑致病变种(Pseudomonas syringae pv.atrofaciens)、丁香假单胞菌晕斑致病变种(Pseudomonas syringae pv.coronafaciens)、丁香假单胞菌大豆致病变种(Pseudomonas syringae pv.glycinea)、丁香假单胞菌黄瓜病致病变种(Pseudomonas syringae pv.lachrymans)、丁香假单胞菌斑生致病变种(Pseudomonas syringae pv.maculicola)、丁香假单胞菌疱疹致病变种(Pseudomonas syringae pv.papulans)、丁香假单胞菌条纹致病变种(Pseudomonas syringae pv.striafaciens)、丁香假单胞菌丁香致病变种(Pseudomonas syringae pv.syringae)、丁香假单胞菌番茄致病变种(Pseudomonas syringae pv.tomato)、丁香假单胞菌烟草致病变种(Pseudomonas syringae pv.Tabaci);
链霉菌属(Streptomyces spp.),包括例如,酸性疮痂链霉菌(Streptomyces acidiscabies)、微白黄链霉菌(Streptomyces albidoflavus)、纯白链霉菌(Streptomyces candidus)(=纯白放线菌(Actinomyces candidus))、Streptomyces caviscabies、山丘链霉菌(Streptomyces collinus)、Streptomyces europaeiscabiei、中间型链霉菌(Streptomyces intermedius)、甘薯链霉菌(Streptomyces ipomoeae)、Streptomyces luridiscabiei、Streptomyces niveiscabiei、Streptomyces puniciscabiei、Streptomyces retuculiscabiei、Streptomyces scabiei、疮痂病链霉菌(Streptomyces scabies)、西唐氏链霉菌(Streptomyces setonii)、Streptomyces steliiscabiei、Streptomyces turgidiscabies、威德摩尔链霉菌(Streptomyces wedmorensis);
地毯草黄单胞菌(Xanthomonas axonopodis),包括例如,地毯草黄单胞菌苜蓿致病变种(Xanthomonas axonopodis pv.alfalfae)(=苜蓿黄单胞菌(Xanthomonas alfalfae))、地毯草黄单胞菌橙致病变种(Xanthomonas axonopodis pv.aurantifolii)(=褐色黄单胞菌橙亚种(Xanthomonas fuscans subsp.Aurantifolii))、地毯草黄单胞菌蒜致病变种(Xanthomonas axonopodis pv.allii)(=野油菜黄单胞菌蒜致病变种(Xanthomonas campestris pv.allii))、地毯草黄单胞菌地毯草致病变种(Xanthomonas axonopodis pv.axonopodis)、地毯草黄单胞菌羊蹄甲致病变种(Xanthomonas axonopodis pv.bauhiniae)(=野油菜黄单胞菌羊蹄甲致病变种(Xanthomonas campestris pv.bauhiniae))、地毯草黄单胞菌秋海棠致病变种(Xanthomonas axonopodis pv.begoniae)(=野油菜黄单胞菌秋海棠致病变种(Xanthomonas campestris pv.begoniae))、地毯草黄单胞菌甜蒌叶致病变种(Xanthomonas axonopodis pv.betlicola)(=野油菜黄单胞菌甜蒌叶致病变种(Xanthomonas campestris pv.betlicola))、地毯草黄单胞菌感应草致病变种(Xanthomonas axonopodis pv.biophyti)(=野油菜黄单胞菌感应草致病变种(Xanthomonas campestris pv.biophyti))、地毯草黄单胞菌木豆致病变种(Xanthomonas axonopodis pv.cajani)(=野油菜黄单胞菌木豆致病变种(Xanthomonas campestris pv.cajani))、地毯草黄单胞菌木薯致病变种(Xanthomonas axonopodis pv.cassavae)(=木薯黄单胞菌(Xanthomonas cassavae)、野油菜黄单胞菌木薯致病变种(Xanthomonas campestris pv.cassavae))、地毯草黄单胞菌山扁豆致病变种(Xanthomonas axonopodis pv.cassiae)(=野油菜黄单胞菌山扁豆致病变种(Xanthomonas campestris pv.cassiae))、地毯草黄单胞菌柑橘致病变种(Xanthomonas axonopodis pv.citri)(=柑橘黄单胞菌(Xanthomonas citri))、地毯草黄单胞菌柑蜜致病变种(Xanthomonas axonopodis pv.citrumelo)(=苜蓿黄单胞菌柑蜜亚种(Xanthomonas alfalfae subsp.citrumelonis))、地毯草黄单胞菌蝶豆致病变种(Xanthomonas axonopodis pv.clitoriae)(=野油菜黄单胞菌蝶豆致病变种(Xanthomonas campestris pv.clitoriae))、地毯草黄单胞菌糁子致病变种(Xanthomonas axonopodis pv.coracanae)(=野油菜黄单胞菌糁子致病变种(Xanthomonas campestris pv.coracanae))、地毯草黄单胞菌瓜尔豆致病变种(Xanthomonas axonopodis pv.cyamopsidis)(=野油菜黄单胞菌瓜尔豆致病变种(Xanthomonas campestris pv.cyamopsidis))、地毯草黄单胞菌山马蝗致病变种(Xanthomonas axonopodis pv.desmodii)(=野油菜黄单胞菌山马蝗致病变种(Xanthomonas campestris pv.desmodii))、地毯草黄单胞菌恒河山马蝗致病变种(Xanthomonas axonopodis pv.desmodiigangetici)(=野油菜黄单胞菌恒河山马蝗致病变种(Xanthomonas campestris pv.desmodiigangetici))、地毯草黄单胞菌疏花山马蝗致病变种(Xanthomonas axonopodis pv.desmodiilaxiflori)(=野油菜黄单胞菌疏花山马蝗致病变种(Xanthomonas campestris pv.desmodiilaxiflori))、地毯草黄单胞菌园叶山马蝗致病变种(Xanthomonas axonopodis pv.desmodiirotundifolii)(=野油菜黄单胞菌园叶山马蝗致病变种(Xanthomonas campestris pv.desmodiirotundifolii))、地毯草黄单胞菌花叶万年青致病变种(Xanthomonas axonopodis pv.dieffenbachiae)(=野油菜黄单胞菌万年青致病变种(Xanthomonas campestris pv.dieffenbachiae))、地毯草黄单胞菌印度刺桐致病变种(Xanthomonas axonopodis pv.erythrinae)(=野油菜黄单胞菌印度刺桐致病变种(Xanthomonas campestris pv.erythrinae))、地毯草黄单胞菌簇生致病变种(Xanthomonas axonopodis pv.fascicularis)(=野油菜黄单胞菌簇生致病变种(Xanthomonas campestris pv.fasciculari))、地毯草黄单胞菌大豆致病变种(Xanthomonas axonopodis pv.glycines)(=野油菜黄单胞菌大豆致病变种(Xanthomonas campestris pv.glycines))、地毯草黄单胞菌红木致病变种(Xanthomonas axonopodis pv.khayae)(=野油菜黄单胞菌红木致病变种(Xanthomonas campestris pv.khayae))、地毯草黄单胞菌胡枝子致病变种(Xanthomonas axonopodis pv.lespedezae)(=野油菜黄单胞菌胡枝子致病变种(Xanthomonas campestris pv.lespedezae))、地毯草黄单胞菌栀子致病变种(Xanthomonas axonopodis pv.maculifoliigardeniae)(=野油菜黄单胞菌栀子致病变种(Xanthomonas campestris pv.maculifoliigardeniae))、地毯草黄单胞菌锦葵致病变种(Xanthomonas axonopodis pv.malvacearum)(=柑橘黄单胞菌锦葵亚种(Xanthomonas citri subsp.Malvacearum))、地毯草黄单胞菌木薯致病变种(Xanthomonas axonopodis pv.manihotis)(=野油菜黄单胞菌木薯致病变种(Xanthomonas campestris pv.manihotis))、地毯草黄单胞菌栖角胡麻致病变种(Xanthomonas axonopodis pv.martyniicola)(=野油菜黄单胞菌栖角胡麻致病变种(Xanthomonas campestris pv.martyniicola))、地毯草黄单胞菌梅氏致病变种(Xanthomonas axonopodis pv.melhusii)(=野油菜黄单胞菌梅氏致病变种(Xanthomonas campestris pv.melhusii))、地毯草黄单胞菌中田氏黄麻致病变种(Xanthomonas axonopodis pv.nakataecorchori)(=野油菜黄单胞菌中田氏黄麻致病变种(Xanthomonas campestris pv.nakataecorchori))、地毯草黄单胞菌西番莲致病变种(Xanthomonas axonopodis pv.passiflorae)(=野油菜黄单胞菌西番莲致病变种(Xanthomonas campestris pv.passiflorae))、地毯草黄单胞菌印度麻致病变种(Xanthomonas axonopodis pv.patelii)(=野油菜黄单胞菌印度麻致病变种(Xanthomonas campestris pv.patelii))、地毯草黄单胞菌脂麻致病变种(Xanthomonas axonopodis pv.pedalii)(=野油菜黄单胞菌脂麻致病变种(Xanthomonas campestris pv.pedalii))、地毯草黄单胞菌菜豆致病变种(Xanthomonas axonopodis pv.phaseoli)(=野油菜黄单胞菌菜豆致病变种(Xanthomonas campestris pv.phaseoli)、菜豆黄单胞菌(Xanthomonas phaseoli))、地毯草黄单胞菌菜豆致病变种褐色变种(Xanthomonas axonopodis pv.phaseoli var.fuscans)(=褐色黄单胞菌(Xanthomonas fuscans))、地毯草黄单胞菌叶下珠致病变种(Xanthomonas axonopodis pv.phyllanthi)(=野油菜黄单胞菌叶下珠致病变种(Xanthomonas campestris pv.phyllanthi))、地毯草黄单胞菌栖酸浆致病变种(Xanthomonas axonopodis pv.physalidicola)(=野油菜黄单胞菌栖酸浆致病变种(Xanthomonas campestris pv.physalidicola))、地毯草黄单胞菌栖猩猩木致病变种(Xanthomonas axonopodis pv.poinsettiicola)(=野油菜黄单胞菌栖猩猩木致病变种(Xanthomonas campestris pv.poinsettiicola))、地毯草黄单胞菌安石榴致病变种(Xanthomonas axonopodis pv.punicae)(=野油菜黄单胞菌安石榴致病变种(Xanthomonas campestris pv.punicae))、地毯草黄单胞菌鹿藿致病变种(Xanthomonas axonopodis pv.rhynchosiae)(=野油菜黄单胞菌鹿藿致病变种(Xanthomonas campestris pv.rhynchosiae))、地毯草黄单胞菌蓖麻致病变种(Xanthomonas axonopodis pv.ricini)(=野油菜黄单胞菌蓖麻致病变种(Xanthomonas campestris pv.ricini))、地毯草黄单胞菌田菁致病变种(Xanthomonas axonopodis pv.sesbaniae)(=野油菜黄单胞菌田菁致病变种(Xanthomonas campestris pv.sesbaniae))、地毯草黄单胞菌罗望子致病变种(Xanthomonas axonopodis pv.tamarindi)(=野油菜黄单胞菌罗望子致病变种(Xanthomonas campestris pv.tamarindi))、地毯草黄单胞菌维管束致病变种(Xanthomonas axonopodis pv.vasculorum)(=野油菜黄单胞菌维管束致病变种(Xanthomonas campestris pv.vasculorum))、地毯草黄单胞菌辣椒斑点病致病变种(Xanthomonas axonopodis pv.vesicatoria)(=野油菜黄单胞菌辣椒斑点病致病变种(Xanthomonas campestris pv.vesicatoria)、辣椒斑点病黄单胞菌(Xanthomonas vesicatoria))、地毯草黄单胞菌绿豆致病变种(Xanthomonas axonopodis pv.vignaeradiatae)(=野油菜黄单胞菌绿豆致病变种(Xanthomonas campestris pv.vignaeradiatae))、地毯草黄单胞菌栖豇豆致病变种(Xanthomonas axonopodis pv.vignicola)(=野油菜黄单胞菌栖豇豆致病变种(Xanthomonas campestris pv.vignicola))、地毯草黄单胞菌葡萄蔓致病变种(Xanthomonas axonopodis pv.vitians)(=野油菜黄单胞菌葡萄蔓致病变种(Xanthomonas campestris pv.vitians));
野油菜黄单胞菌香蕉致病变种(Xanthomonas campestris pv.musacearum)、野油菜黄单胞菌桃李致病变种(Xanthomonas campestris pv.pruni)(=Xanthomonas arboricola pv.pruni)、草莓黄单胞菌(Xanthomonas fragariae);
半透明黄单胞菌(Xanthomonas translucens)(=野油菜黄单胞菌大麦致病变种(Xanthomonas campestris pv.hordei)),包括例如,半透明黄单胞菌燕麦草致病变种(Xanthomonas translucens pv.arrhenatheri)(=野油菜黄单胞菌燕麦草致病变种(Xanthomonas campestris pv.arrhenatheri)、半透明黄单胞菌谷物致病变种(Xanthomonas translucens pv.cerealis)(=野油菜黄单胞菌谷物致病变种(Xanthomonas campestris pv.cerealis))、半透明黄单胞菌禾谷致病变种(Xanthomonas translucens pv.graminis)(=野油菜黄单胞菌禾谷致病变种(Xanthomonas campestris pv.graminis))、半透明黄单胞菌梯牧草属致病变种(Xanthomonas translucens pv.phlei)(=野油菜黄单胞菌梯牧草属致病变种(Xanthomonas campestris pv.phlei))、半透明黄单胞菌梯牧草致病变种(Xanthomonas translucens pv.phleipratensis)(=野油菜黄单胞菌梯牧草致病变种(Xanthomonas campestris pv.phleipratensis))、半透明黄单胞菌早熟禾致病变种(Xanthomonas translucens pv.poae)(=野油菜黄单胞菌早熟禾致病变种(Xanthomonas campestris pv.poae))、半透明黄单胞菌黑麦致病变种(Xanthomonas translucens pv.secalis)(=野油菜黄单胞菌黑麦致病变种(Xanthomonas campestris pv.secalis))、半透明黄单胞菌半透明致病变种(Xanthomonas translucens pv.translucens)(=野油菜黄单胞菌半透明致病变种(Xanthomonas campestris pv.translucens))、半透明黄单胞菌波形致病变种(Xanthomonas translucens pv.undulosa)(=野油菜黄单胞菌波形致病变种(Xanthomonas campestris pv.Undulosa));
稻黄单胞菌(Xanthomonas oryzae)、稻黄单胞菌稻致病变种(Xanthomonas oryzae pv.oryzae)(=野油菜黄单胞菌稻致病变种(Xanthomonas campestris pv.oryzae))、稻黄单胞菌水稻致病变种(Xanthomonas oryzae pv.oryzicola)(=野油菜黄单胞菌水稻致病变种(Xanthomonas campestris pv.oryzicola))。
来自黄单胞菌科(Xanthomonadaceae)家族的苛养木杆菌(Xylella fastidiosa)。
优选地,所述细菌性有害生物选自:
燕麦食酸菌燕麦亚种(=燕麦假单胞菌燕麦亚种)、燕麦食酸菌西瓜亚种(=类产碱假单胞菌西瓜亚种、燕麦假单胞菌西瓜亚种)、荚壳伯克霍尔德氏菌(=荚壳假单胞菌)、茄伯克霍尔德氏菌(=茄罗尔斯通氏菌)、密执安棒杆菌尼布拉斯加致病变种、解淀粉欧文氏菌、胡萝卜软腐欧文氏菌(=胡萝卜果胶杆菌)、胡萝卜软腐欧文氏菌黑腐亚种、胡萝卜软腐欧文氏菌胡萝卜软腐亚种、菊欧文氏菌、菊欧文氏菌玉米致病变种、草生欧文氏菌、斯氏欧文氏菌、嗜夏孢欧文氏菌、Liberibacter属、如上所定义的韧皮部杆菌属、丁香假单胞菌、丁香假单胞菌猕猴桃致病变种(Psa)、丁香假单胞菌大豆致病变种、丁香假单胞菌黄瓜病致病变种、丁香假单胞菌疱疹致病变种、丁香假单胞菌丁香致病变种、丁香假单胞菌番茄致病变种、丁香假单胞菌烟草致病变种、罗尔斯通氏菌属、疮痂病链霉菌、地毯草黄单胞菌柑橘致病变种、地毯草黄单胞菌大豆致病变种(=野油菜黄单胞菌大豆致病变种)、地毯草黄单胞菌安石榴致病变种(=野油菜黄单胞菌安石榴致病变种)、地毯草黄单胞菌辣椒斑点病致病变种(=野油菜黄单胞菌辣椒斑点病致病变种、辣椒斑点病黄单胞菌)、野油菜黄单胞菌、野油菜黄单胞菌香蕉致病变种、野油菜黄单胞菌桃李致病变种(=Xanthomonas arboricola pv.pruni)、草莓黄单胞菌、半透明黄单胞菌半透明致病变种(=野油菜黄单胞菌半透明致病变种)、稻黄单胞菌稻致病变种(=野油菜黄单胞菌稻致病变种)、苛养木杆菌。
在本发明一个更优选的方面,所述细菌性有害生物选自:
如上所定义的燕麦食酸菌(=燕麦假单胞菌、燕麦假单胞菌燕麦亚种、红纹假单胞菌)、如上所定义的伯克霍尔德氏菌属、荚壳伯克霍尔德氏菌、如上所定义的棒杆菌属、如上所定义的欧文氏菌属、解淀粉欧文氏菌、胡萝卜软腐欧文氏菌(=胡萝卜果胶杆菌)、胡萝卜软腐欧文氏菌黑腐亚种、胡萝卜软腐欧文氏菌胡萝卜软腐亚种、菊欧文氏菌、菊欧文氏菌玉米致病变种、草生欧文氏菌、斯氏欧文氏菌、嗜夏孢欧文氏菌、Liberibacter属、如上所定义的韧皮部杆菌属、如上所定义的丁香假单胞菌、丁香假单胞菌猕猴桃致病变种、丁香假单胞菌大豆致病变种、丁香假单胞菌番茄致病变种、丁香假单胞菌黄瓜病致病变种、罗尔斯通氏菌属、链霉菌属、疮痂病链霉菌、黄单胞菌属、如上所定义的地毯草黄单胞菌、地毯草黄单胞菌柑橘致病变种、地毯草黄单胞菌大豆致病变种、野油菜黄单胞菌、野油菜黄单胞菌香蕉致病变种、野油菜黄单胞菌桃李致病变种(=Xanthomonas arboricola pv.pruni)、草莓黄单胞菌和半透明黄单胞菌(=野油菜黄单胞菌大麦致病变种)、稻黄单胞菌稻致病变种(=野油菜黄单胞菌稻致病变种)和如上所定义的苛养木杆菌。
甚至更优选的是由以下组成的选择:
燕麦食酸菌、伯克霍尔德氏菌属、荚壳伯克霍尔德氏菌、棒杆菌属、欧文氏菌属、Liberibacter属、韧皮部杆菌属、丁香假单胞菌、丁香假单胞菌猕猴桃致病变种、丁香假单胞菌大豆致病变种、丁香假单胞菌番茄致病变种、丁香假单胞菌黄瓜病致病变种、罗尔斯通氏菌属、链霉菌属、黄单胞菌属、地毯草黄单胞菌、地毯草黄单胞菌柑橘致病变种、地毯草黄单胞菌大豆致病变种、野油菜黄单胞菌、野油菜黄单胞菌香蕉致病变种、野油菜黄单胞菌桃李致病变种、草莓黄单胞菌、半透明黄单胞菌、稻黄单胞菌稻致病变种(=野油菜黄单胞菌稻致病变种)和苛养木杆菌。
在本发明的一个甚至更优选的方面,所述细菌性有害生物选自:
燕麦食酸菌、伯克霍尔德氏菌属、荚壳伯克霍尔德氏菌、棒杆菌属、解淀粉欧文氏菌、胡萝卜软腐欧文氏菌、胡萝卜软腐欧文氏菌黑腐亚种、胡萝卜软腐欧文氏菌胡萝卜软腐亚种、菊欧文氏菌、菊欧文氏菌玉米致病变种、草生欧文氏菌、斯氏欧文氏菌、嗜夏孢欧文氏菌、Liberibacter属、韧皮部杆菌属、丁香假单胞菌、丁香假单胞菌猕猴桃致病变种、丁香假单胞菌大豆致病变种、丁香假单胞菌黄瓜病致病变种、丁香假单胞菌番茄致病变种、罗尔斯通氏菌属、疮痂病链霉菌、地毯草黄单胞菌、地毯草黄单胞菌柑橘致病变种、地毯草黄单胞菌大豆致病变种、野油菜黄单胞菌、野油菜黄单胞菌香蕉致病变种、野油菜黄单胞菌桃李致病变种、草莓黄单胞菌、半透明黄单胞菌、稻黄单胞菌稻致病变种(=野油菜黄单胞菌稻致病变种)和苛养木杆菌。
最优选的选择包括由以下组成的组:
荚壳伯克霍尔德氏菌、Liberibacter属、韧皮部杆菌属、地毯草黄单胞菌柑橘致病变种、丁香假单胞菌、丁香假单胞菌猕猴桃致病变种、丁香假单胞菌大豆致病变种、丁香假单胞菌黄瓜病致病变种、丁香假单胞菌番茄致病变种、罗尔斯通氏菌属、疮痂病链霉菌、地毯草黄单胞菌大豆致病变种、野油菜黄单胞菌桃李致病变种、野油菜黄单胞菌、稻黄单胞菌稻致病变种(=野油菜黄单胞菌稻致病变种)和苛养木杆菌。
因此,本发明的结合物可用于在某一处理后时期内保护植物免受以上提及的病原体的侵袭。在使用所述活性化合物处理植物之后,提供保护的时期通常持续1至10天,优选1至7天。根据施用形式,可通过靶向方法来控制活性化合物对植物的可达性(accessibility)。
所述结合物在防治植物病害所需的宿主防御诱导剂和生物防治剂浓度下的良好的植物耐受性使其可处理地上和地下植物部位、营养繁殖材料和土壤。
本发明的结合物还适用于提高产率,表现出低毒性并具有良好的植物耐受性。所述结合物特别适用于减少对植物和植物部位的总体损害,以及减少由植物致病细菌引起的采收水果或蔬菜的减产。
在本发明中,施用至植物后观察到有利的效果。
根据本发明,可处理所有植物。在本文的上下文中,植物应被理解为意指全部植物部位和植物种群,例如需要的和不需要的野生植物或作物植物(包括天然的作物植物)。作物植物可以是可通过传统育种和优化方法或通过生物技术和重组方法或这些方法的结合而获得的植物,包括转基因植物并且包括受到或不受植物育种者权利保护的植物品种。这类方法是,例如,双倍化单倍体、原生质体融合、随机或定向诱变,以及分子或遗传标记。
植物部位旨在表示植物的所有地上和地下部位,以及植物器官,例如草(herb)、假茎、芽、叶、苞片、叶鞘、叶柄、叶片(lamina)、花和根,可提及的实例为叶、针叶、秆、茎、花、子实体、果实、香蕉把(banana hand)、串和种子,以及根、块茎、根茎、分枝、吸根、次生生长。植物部位还包括作物材料和营养生殖材料和有性生殖材料,例如扦插、块茎、根茎、插枝(slip)和种子。
如以上已提及,根据本发明可处理所有的植物。在一个优选的实施方案中,处理植物物种和植物品种及其部位,其存在于野生环境或通过常规的生物育种方法(例如,杂交、分生组织培养、微繁殖、体细胞胚胎发生、直接器官发生或原生质体融合)获得。在另一优选的实施方案中,处理转基因植物和植物品种,其通过重组方法——如果适合,结合传统方法——获得(基因修饰生物),例如,通过土壤杆菌属(Agrobacterium)转化或胚胎生成细胞的粒子轰击,以及微繁殖。植物包括以上提及的全部植物部位。
特别优选根据本发明处理在各种情况下市售或使用的那些植物品种的植物。植物品种应理解为具有新特性(“性状”)的植物,所述新特性通过常规育种、通过诱变或通过重组DNA技术来获得。其可以是品种、培育品种(breed)、生物型和基因型。
本发明的处理方法可用于处理基因修饰生物(GMOs),例如植物或种子。基因修饰的植物(或转基因植物)是异源基因已稳定地整合到其基因组中的植物。表述“异源基因”基本上意指在植物体外提供或组装的基因,当将其引入细胞核、叶绿体或线粒体基因组时,通过表达目的蛋白或多肽或通过下调或沉默存在于植物中的其他基因(使用例如,反义技术、共抑制技术或RNA干扰(RNAi)技术)赋予转化植物新的或改进的农学或其他特性。位于基因组中的异源基因也被称为转基因。通过其在植物基因组中的特定位置而定义的转基因被称为转化或转基因株系。
优选待根据本发明处理的植物和植物品种包括具有赋予这些植物特别有利、有用的性状的遗传物质的所有植物(无论是通过育种和/或通过生物技术方法获得)。
可根据本发明进行处理的植物为已经表达出杂交特征或杂种活力的杂交植物,所述杂交特征或杂种活力通常带来更高的产率、更高的活力、植物更加健康和对生物和非生物胁迫因素的更好的抗性。通常将一种自交雄性不育亲系(母本)与另一种自交雄性能育亲系(父本)杂交而制得这种植物。杂交种子通常收获自雄性不育植物并出售给种植者。有时(例如在玉米中)可以通过去雄(即机械地移去雄性生殖器官或雄花)而产生雄性不育植物,但是,更通常地,雄性不育性是由植物基因组中遗传决定因子产生的。在这种情况下,特别是当种子是待从杂交植物上收获的所需产品时,通常有用的是确保杂交植物的雄性能育性完全恢复,所述杂交植物包含造成雄性不育性的遗传决定因子。这可以通过确保父本具有合适的育性恢复基因而完成,该基因能够恢复含有造成雄性不育性的遗传决定因子的杂交植物的雄性能育性。雄性不育的遗传决定因子可以位于细胞质中。细胞质雄性不育(CMS)实例例如记载于芸苔属(Brassica)物种中。然而,雄性不育的遗传决定因子也可位于细胞核基因组中。也可通过植物生物技术方法如基因工程获得雄性不育植物。一种获取雄性不育植物的特别有用的方法记载于WO 89/10396中,其中,例如,一种核糖核酸酶例如芽孢杆菌RNA酶在雄蕊中的绒毡层细胞中选择性表达。随后可以通过在绒毡层细胞中表达核糖核酸酶抑制因子如芽孢杆菌RNA酶抑制因子来恢复能育性。
还可根据本发明处理的植物或植物品种(通过植物生物技术方法如遗传工程获得)是对昆虫有抗性的转基因植物,即对某些目标昆虫的侵害有抗性的植物。可通过遗传转化或通过选择含赋予所述昆虫抗性的突变的植物而获得这类植物。
可根据本发明处理并可提及的植物是以下植物:
棉花、亚麻、葡萄藤、蔬菜和水果(例如,猕猴桃、菠萝),如蔷薇科物种(Rosaceae sp.)(例如,仁果如苹果和梨,以及核果如杏、樱桃、扁桃和桃,以及浆果如草莓),或来自石榴属(Punica)的石榴、Ribesioidae物种、胡桃科物种(Juglandaceae sp.)、桦木科物种(Betulaceae sp.)、漆树科物种(Anacardiaceae sp.)、壳斗科物种(Fagaceae sp.)、桑科物种(Moraceae sp.)、木犀科物种(Oleaceae sp.)、猕猴桃科物种(Actinidaceae sp.)、樟科物种(Lauraceae sp.)、芭蕉科物种(Musaceae sp.)(例如香蕉树和香蕉种植园,以及芭蕉)、茜草科物种(Rubiaceae sp.)(例如咖啡)、山茶科物种(Theaceae sp.)、梧桐科物种(Sterculiceae sp.)、芸香科物种(Rutaceae sp.)(例如柑橘、柠檬、橙和葡萄柚)、茄科物种(Solanaceae sp.)(例如番茄)、百合科物种(Liliaceae sp.)、菊科物种(Asteraceae sp.)(例如莴苣)、伞形科物种(Umbelliferae sp.)、十字花科物种(Cruciferae sp.)、藜科物种(Chenopodiaceae sp.)、葫芦科物种(Cucurbitaceae sp.)(例如,黄瓜、甜瓜、葫芦、南瓜)、葱科物种(Alliaceae sp.)(例如韭菜、洋葱)、蝶形花科物种(Papilionaceae sp.)(例如,豌豆);主要作物植物如禾本科物种(Gramineae sp.)(例如,玉米、草地,谷物如小麦、黑麦、稻、大麦、燕麦、高粱、小米、小黑麦)、菊科物种(Asteraceae sp.)(例如向日葵)、十字花科物种(Brassicaceae sp.)(例如,甘蓝如白球甘蓝和红球甘蓝、花椰菜、菜花、抱子甘蓝、小白菜、球茎甘蓝、小萝卜,以及油菜、芥菜、山葵和水芹)、豆科物种(Fabacae sp.)(例如,豆、花生)、蝶形花科物种(Papilionaceae sp.)(例如,大豆)、茄科物种(Solanaceae sp.)(例如马铃薯)、藜科物种(Chenopodiaceae sp.)(例如甜菜、饲用甜菜、瑞士甜菜、甜菜根);园林和森林中的有用植物和观赏植物;以及在各种情况下这些植物的遗传修饰型。
优选地,本发明的结合物用于处理选自以下的植物:
蔬菜和水果(例如,猕猴桃、甜瓜、菠萝),如蔷薇科物种(例如,仁果如苹果和梨,以及核果如杏、樱桃、扁桃和桃,以及浆果如草莓),或来自石榴属的石榴、芭蕉科物种(例如香蕉树和香蕉种植园,以及芭蕉)、芸香科物种(例如柑橘、柠檬、橙和葡萄柚);蔬菜如茄科物种(例如番茄)、葫芦科物种(例如,黄瓜、甜瓜、葫芦、南瓜);主要作物植物如禾本科物种(例如,玉米、草地,谷物如小麦、黑麦、稻、大麦、燕麦、高粱、小米和小黑麦)、十字花科物种(例如,甘蓝如白球甘蓝和红球甘蓝、花椰菜、菜花、抱子甘蓝、小白菜、球茎甘蓝、小萝卜,以及油菜、芥菜、山葵和水芹)、蝶形花科物种(例如,大豆)、茄科物种(例如马铃薯);以及在各种情况下这些植物的遗传修饰型。
甚至更优选的是处理选自水果、蔬菜、马铃薯、谷物、玉米、稻和大豆的植物。
由此进一步优选的选择涉及由以下植物组成的组:
猕猴桃,甜瓜,菠萝,仁果如苹果、梨和石榴,核果如桃,浆果如草莓,香蕉植物和香蕉种植园以及芭蕉,柑橘,柠檬,橙和葡萄柚;番茄,黄瓜,甜瓜,葫芦,玉米,谷物如小麦、稻,甘蓝,菜花,大豆,马铃薯;以及在各种情况下这些植物的遗传修饰型。
根据本发明处理的有用植物的最优选选择涉及:苹果、香蕉、柑橘、猕猴桃、甜瓜、桃、梨、菠萝、梨果、石榴、甘蓝、菜花、黄瓜、葫芦、番茄、马铃薯、小麦、稻和大豆。
进一步涉及:柑橘、猕猴桃、桃、黄瓜、番茄、马铃薯、小麦、稻和大豆。
本发明的另一个优选方面涉及包含至少一种宿主防御诱导剂和至少一种生物防治剂的结合物用于防治至少一种以下生物的用途:
稻中的燕麦食酸菌、荚壳伯克霍尔德氏菌和/或野油菜黄单胞菌稻致病变种;柑橘中的韧皮部杆菌属和/或地毯草黄单胞菌柑橘致病变种;玉米中的棒杆菌属;猕猴桃中的丁香假单胞菌猕猴桃致病变种;桃、香蕉和/或芭蕉中的野油菜黄单胞菌;石榴中的地毯草黄单胞菌;大豆中的丁香假单胞菌大豆致病变种和/或地毯草黄单胞菌;谷物中(优选在小麦中)的伯克霍尔德氏菌属和/或半透明黄单胞菌;番茄中的丁香假单胞菌、丁香假单胞菌番茄致病变种和/或野油菜黄单胞菌;黄瓜中的丁香假单胞菌和/或丁香假单胞菌黄瓜致病变种;马铃薯中的胡萝卜软腐欧文氏菌、胡萝卜软腐欧文氏菌黑腐亚种和/或疮痂病链霉菌;香蕉和/或芭蕉中的胡萝卜软腐欧文氏菌;以及柑橘中的苛养木杆菌。
其中更优选使用包含至少一种宿主防御诱导剂和至少一种生物防治剂的结合物以防治至少一种以下生物:稻中的燕麦食酸菌、伯克霍尔德氏菌属(优选荚壳伯克霍尔德氏菌)和/或野油菜黄单胞菌稻致病变种;柑橘中的韧皮部杆菌属和/或地毯草黄单胞菌(优选地毯草黄单胞菌柑橘致病变种)和/或苛养木杆菌;猕猴桃中的丁香假单胞菌(优选丁香假单胞菌猕猴桃致病变种);桃中的野油菜黄单胞菌和/或野油菜黄单胞菌桃李致病变种;大豆中的丁香假单胞菌(优选丁香假单胞菌大豆致病变种)和/或地毯草黄单胞菌(优选地毯草黄单胞菌大豆致病变种(=野油菜黄单胞菌大豆致病变种));谷物中的伯克霍尔德氏菌属和/或半透明黄单胞菌;番茄中的丁香假单胞菌(优选丁香假单胞菌番茄致病变种)和/或野油菜黄单胞菌;黄瓜中的丁香假单胞菌和/或丁香假单胞菌黄瓜致病变种;以及马铃薯中的黑腐欧文氏菌(Erwinia atroseptica)、胡萝卜软腐欧文氏菌和/或疮痂病链霉菌。
最优选使用包含至少一种宿主防御诱导剂和至少一种生物防治剂的结合物以防治以下生物:稻中的荚壳伯克霍尔德氏菌和/或野油菜黄单胞菌稻致病变种;柑橘中的韧皮部杆菌属和/或地毯草黄单胞菌柑橘致病变种和/或苛养木杆菌;猕猴桃中的丁香假单胞菌猕猴桃致病变种(Psa);大豆中的丁香假单胞菌大豆致病变种和/或地毯草黄单胞菌大豆致病变种;番茄中的丁香假单胞菌和/或丁香假单胞菌番茄致病变种;桃中的野油菜黄单胞菌和/或野油菜黄单胞菌桃李致病变种;黄瓜中的丁香假单胞菌、丁香假单胞菌黄瓜致病变种;和/或马铃薯中的疮痂病链霉菌。
结合物/制剂
包含至少一种宿主防御诱导剂(A)和至少一种生物防治剂(B)的本发明的结合物还可包含至少一种化合物(C),其选自抗微生物剂如杀细菌剂、其他(常规)抗生素、杀真菌剂、杀螨剂、杀线虫剂、杀昆虫剂、除草剂、微量营养素和包含微量营养素的化合物、安全剂、脂壳寡糖化合物(LCO)和土壤改良产品或减少植物胁迫的产品,以例如扩大作用范围或阻止抗性发展。在本发明的含义内,其他化合物(C)的组包括不属于本文定义的生物防治剂(B)组且不属于本文定义的宿主防御诱导剂(A)组的化合物。
因此,在本发明的含义内,选自已知或常规抗生素的化合物(C)包括C1.1春雷霉素、C1.2链霉素、C1.3氧四环素(oxytetracyclin)、有效霉素(validamycin)、庆大霉素(gentamycin)、金色制霉素(aureofungin)、杀稻瘟菌素-S(blasticidin-S)、放线菌酮(cycloheximide)、灰黄霉素(griseofulvin)、吗啉胍(moroxydine)、游霉素(natamycin)、多抗霉素(polyoxins)、保粒霉素(polyoxorim)及其组合。
优选的常规抗生素为C1.1春雷霉素、C1.2链霉素和C1.3氧四环素,或其组合。
在本发明的含义内,选自已知或常规杀真菌剂的化合物(C)包括:
(a)麦角固醇生物合成抑制剂,例如,4-十二烷基-2,6-二甲基吗啉(aldimorph)、氧环唑(azaconazole)、双苯三唑醇(bitertanol)、糠菌唑(bromuconazole)、环唑醇(cyproconazole)、苄氯三唑醇(diclobutrazole)、苯醚甲环唑(difenoconazole)、烯唑醇(diniconazole)、R-烯唑醇(diniconazole-M)、十二环吗啉(dodemorph)、十二环吗啉乙酸盐(dodemorph acetate)、氟环唑(epoxiconazole)、乙环唑(etaconazole)、氯苯嘧啶醇(fenarimol)、腈苯唑(fenbuconazole)、环酰菌胺(fenhexamid)、苯锈啶(fenpropidin)、丁苯吗啉(fenpropimorph)、氟喹唑(fluquinconazole)、呋嘧醇(flurprimidole)、氟硅唑(flusilazole)、粉唑醇(flutriafol)、呋菌唑(furconazole)、顺呋醚唑(furconazole-cis)、己唑醇(hexaconazole)、抑霉唑(imazalil)、烯菌灵硫酸盐(imazalil sulphate)、亚胺(imibenconazole)、种菌唑(ipconazole)、叶菌唑(metconazole)、腈菌唑(myclobutanil)、萘替芬(naftifine)、氟苯嘧啶醇(nuarimol)、恶咪唑(oxpoconazole)、多效唑(paclobutrazol)、稻瘟酯(pefurazoate)、戊菌唑(penconazole)、粉病灵(piperalin)、咪鲜胺(prochloraz)、丙环唑(propiconazole)、丙硫菌唑(prothioconazole)、稗草丹(pyributicarb)、啶斑肟(pyrifenox)、唑喹菌酮(quinconazole)、硅氟唑(simeconazole)、螺环菌胺(spiroxamine)、戊唑醇(tebuconazole)、特比萘芬(terbinafine)、四氟醚唑(tetraconazole)、三唑酮(triadimefon)、唑菌醇(triadimenol)、十三吗啉(tridemorph)、氟菌唑(triflumizole)、嗪氨灵(triforine)、灭菌唑(triticonazole)、烯效唑(uniconazole)、烯效唑-p(uniconazole-p)、烯霜苄唑(viniconazole)、伏立康唑(voriconazole)、1-(4-氯苯基)-2-(1H-1,2,4-三唑-1-基)环庚醇、1-(2,2-二甲基-2,3-二氢-1H-茚-1-基)-1H-咪唑-5-羧酸甲酯、N'-{5-(二氟甲基)-2-甲基-4-[3-(三甲基甲硅烷基)丙氧基]苯基}-N-乙基-N-甲基酰亚胺基(imido)甲酰胺、N-乙基-N-甲基-N'-{2-甲基-5-(三氟甲基)-4-[3-(三甲基甲硅烷基)丙氧基]苯基}酰亚胺基甲酰胺和O-[1-(4-甲氧基苯氧基)-3,3-二甲基丁-2-基]1H-咪唑-1-硫代甲酸酯;
(b)呼吸链复合物I或II的抑制剂,例如,联苯吡菌胺(bixafen)、啶酰菌胺(boscalid)、萎锈灵(carboxin)、氟嘧菌胺(diflumetorim)、甲呋酰胺(fenfuram)、氟吡菌酰胺(fluopyram)、氟酰胺(flutolanil)、氟唑菌酰胺(fluxapyroxad)、呋吡菌胺(furametpyr)、拌种胺(furmecyclox)、吡唑萘菌胺(isopyrazam)(顺式差向异构外消旋体1RS,4SR,9RS与反式差向异构外消旋体1RS,4SR,9SR的混合物)、吡唑萘菌胺(反式差向异构外消旋体1RS,4SR,9SR)、吡唑萘菌胺(反式差向异构对映异构体1R,4S,9S)、吡唑萘菌胺(反式差向异构对映异构体1S,4R,9R)、吡唑萘菌胺(顺式差向异构外消旋体1RS,4SR,9RS)、吡唑萘菌胺(顺式差向异构对映异构体1R,4S,9R)、吡唑萘菌胺(顺式差向异构对映异构体1S,4R,9S)、灭锈胺(mepronil)、氧化萎锈灵(oxycarboxin)、C.2.2戊苯吡菌胺(penflufen)、吡噻菌胺(penthiopyrad)、sedaxane、溴氟唑菌(thifluzamide)、1-甲基-N-[2-(1,1,2,2-四氟乙氧基)苯基]-3-(三氟甲基)-1H-吡唑-4-甲酰胺、3-(二氟甲基)-1-甲基-N-[2-(1,1,2,2-四氟乙氧基)苯基]-1H-吡唑-4-甲酰胺、3-(二氟甲基)-N-[4-氟-2-(1,1,2,3,3,3-六氟丙氧基)苯基]-1-甲基-1H-吡唑-4-甲酰胺、N-[1-(2,4-二氯苯基)-1-甲氧基丙-2-基]-3-(二氟甲基)-1-甲基-1H-吡唑-4-甲酰胺、5,8-二氟-N-[2-(2-氟-4-{[4-(三氟甲基)吡啶-2-基]氧基}苯基)乙基]喹唑啉-4-胺、N-[9-(二氯亚甲基)-1,2,3,4-四氢-1,4-羟甲基(methano)萘-5-基]-3-(二氟甲基)-1-甲基-1H-吡唑-4-甲酰胺、N-[(1S,4R)-9-(二氯亚甲基)-1,2,3,4-四氢-1,4-羟甲基萘-5-基]-3-(二氟甲基)-1-甲基-1H-吡唑-4-甲酰胺和N-[(1R,4S)-9-(二氯亚甲基)-1,2,3,4-四氢-1,4-羟甲基萘-5-基]-3-(二氟甲基)-1-甲基-1H-吡唑-4-甲酰胺;
(c)呼吸链复合物III的抑制剂,例如,唑嘧菌胺(ametoctradin)、吲唑磺菌胺(amisulbrom)、C.2.4嘧菌酯(azoxystrobin)、氰霜唑(cyazofamid)、甲香菌酯(coumethoxystrobin)、丁香菌酯(coumoxystrobin)、醚菌胺(dimoxystrobin)、烯肟菌酯(enestroburin)、噁唑菌酮(famoxadone)、咪唑菌酮(fenamidone)、fenoxystrobin、氟嘧菌酯(fluoxastrobin)、醚菌酯(kresoxim-methyl)、苯氧菌胺(metominostrobin)、肟醚菌胺(orysastrobin)、啶氧菌酯(picoxystrobin)、唑菌胺酯(pyraclostrobin)、唑胺菌酯(pyrametostrobin)、唑菌酯(pyraoxystrobin)、吡菌苯威(pyribencarb)、氯啶菌酯(triclopyricarb)、C.2.3肟菌酯(trifloxystrobin)、(2E)-2-(2-{[6-(3-氯-2-甲基苯氧基)-5-氟嘧啶-4-基]氧基}苯基)-2-(甲氧基亚氨基)-N-甲基乙酰胺、(2E)-2-(甲氧基亚氨基)-N-甲基-2-(2-{[({(1E)-1-[3-(三氟甲基)苯基]亚乙基}氨基)氧基]甲基}苯基)乙酰胺、(2E)-2-(甲氧基亚氨基)-N-甲基-2-{2-[(E)-({1-[3-(三氟甲基)苯基]乙氧基}亚氨基)甲基]苯基}乙酰胺、(2E)-2-{2-[({[(1E)-1-(3-{[(E)-1-氟-2-苯基乙烯基]氧基}苯基)亚乙基]氨基}氧基)甲基]苯基}-2-(甲氧基亚氨基)-N-甲基乙酰胺、(2E)-2-{2-[({[(2E,3E)-4-(2,6-二氯苯基)丁-3-烯-2-亚基]氨基}氧基)甲基]苯基}-2-(甲氧基亚氨基)-N-甲基乙酰胺、2-氯-N-(1,1,3-三甲基-2,3-二氢-1H-茚-4-基)吡啶-3-甲酰胺、5-甲氧基-2-甲基-4-(2-{[({(1E)-1-[3-(三氟甲基)苯基]亚乙基}氨基)氧基]甲基}苯基)-2,4-二氢-3H-1,2,4-三唑-3-酮、(2E)-2-{2-[({环丙基[(4-甲氧基苯基)亚氨基]甲基}硫烷基(sulfanyl))甲基]苯基}-3-甲氧基丙-2-烯酸甲酯、N-(3-乙基-3,5,5-三甲基环己基)-3-(甲酰基氨基)-2-羟基苯甲酰胺、2-{2-[(2,5-二甲基苯氧基)甲基]苯基}-2-甲氧基-N-甲基乙酰胺和(2R)-2-{2-[(2,5-二甲基苯氧基)甲基]苯基}-2-甲氧基-N-甲基乙酰胺;
(d)有丝分裂和细胞分裂抑制剂,例如苯菌灵(benomyl)、多菌灵(carbendazim)、苯咪唑菌(chlorfenazole)、乙霉威(diethofencarb)、噻唑菌胺(ethaboxam)、氟啶酰菌胺(fluopicolide)、麦穗宁(fuberidazole)、戊菌隆(pencycuron)、噻菌灵(thiabendazole)、甲基硫菌灵(thiophanate-methyl)、硫菌灵(thiophanate)、苯酰菌胺(zoxamide)、5-氯-7-(4-甲基哌啶-1-基)-6-(2,4,6-三氟苯基)[1,2,4]三唑并[1,5-a]嘧啶和3-氯-5-(6-氯吡啶-3-基)-6-甲基-4-(2,4,6-三氟苯基)哒嗪;
(e)能够具有多位点作用的化合物,例如,波尔多混合液、敌菌丹(captafol)、克菌丹(captan)、百菌清(chlorothalonil)、氢氧化铜、环烷酸铜、氧化铜、氯氧化铜(copper oxychloride)、硫酸铜(2+)、苯氟磺胺(dichlofluanid)、二氰蒽醌(dithianon)、多果定(dodine)、多果定游离碱(dodine free base)、福美铁(ferbam)、氟灭菌丹(fluorofolpet)、灭菌丹(folpet)、双胍辛盐(guazatine)、双胍辛乙酸盐(guazatine acetate)、双胍辛胺(iminoctadine)、双胍辛烷基苯磺酸盐(iminoctadine albesilate)、双胍辛胺乙酸盐(iminoctadine triacetate)、代森锰铜(mancopper)、代森锰锌(mancozeb)、代森锰(maneb)、代森联(metiram)、代森联锌(metiram zinc)、喹啉铜(oxine-copper)、丙烷脒(propamidine)、丙森锌(propineb)、包括多硫化钙的硫和硫制剂、福美双(thiram)、甲苯氟磺胺(tolylfluanid)、代森锌(zineb)和福美锌(ziram);
(f)能诱导宿主防御的化合物,例如,苯并噻二唑(acibenzolar-S-methyl)、异噻菌胺(isotianil)、烯丙苯噻唑(probenazole)和噻酰菌胺(tiadinil);
(g)氨基酸和/或蛋白质生物合成抑制剂,例如,胺扑灭(andoprim)、杀稻瘟菌素-S(blasticidin-S)、嘧菌环胺(cyprodinil)、春雷霉素(kasugamycin)、春雷霉素盐酸盐水合物(kasugamycin hydrochloride hydrate)、嘧菌胺(mepanipyrim)、嘧霉胺(pyrimethanil)和3-(5-氟-3,3,4,4-四甲基-3,4-二氢异喹啉-1-基)喹啉;
(h)ATP产生抑制剂,例如,三苯基乙酸锡(fentin acetate)、三苯基氯化锡(fentin chloride)、毒菌锡(fentin hydroxide)和硅噻菌胺(silthiofam);
(i)细胞壁合成抑制剂,例如,苯噻菌胺(benthiavalicarb)、烯酰吗啉(dimethomorph)、氟吗啉(flumorph)、异丙菌胺(iprovalicarb)、双炔酰菌胺(mandipropamid)、多抗霉素(polyoxins)、保粒霉素(polyoxorim)、有效霉素A(validamycin A)和维芬乐特(valifenalate);
(j)脂质和膜合成抑制剂,例如,联苯、地茂散(chloroneb)、氯硝胺(dicloran)、敌瘟磷(edifenphos)、土菌灵(etridiazole)、碘代丙炔基丁基甲胺酸酯(iodocarb)、异稻瘟净(iprobenfos)、稻瘟灵(isoprothiolane)、霜霉威(propamocarb)、霜霉威盐酸盐(propamocarb hydrochloride)、胺丙威(prothiocarb)、吡菌磷(pyrazophos)、五氯硝基苯(quintozene)、四氯硝基苯(tecnazene)和甲基立枯磷(tolclofos-methyl);
(k)黑色素生物合成抑制剂,例如,环丙酰菌胺(capropamid)、双氯氰菌胺(diclocymet)、氰菌胺(fenoxanil)、四氯苯酞(phthalide)、咯喹酮(pyroquilon)、三环唑(tricyclazole)和2,2,2-三氟乙基{3-甲基-1-[(4-甲基苯甲酰基)氨基]丁-2-基}氨基甲酸酯;
(l)核酸合成抑制剂,例如,苯霜灵(benalaxyl)、精苯霜灵(benalaxyl-M(kiralaxyl))、乙嘧酚磺酸酯(bupirimate)、clozylacon、二甲嘧酚(dimethirimol)、乙嘧酚(ethirimol)、呋霜灵(furalaxyl)、恶霉灵(hymexazole)、甲霜灵(metalaxyl)、高效霜灵(metalaxyl-M)(精加霜灵(mefenoxam))、呋酰胺(ofurace)、恶霜灵(oxadixyl)和奥索利酸(oxolinic acid);
(m)信号转导抑制剂,例如,乙菌利(chlozolinate)、拌种咯(fenpiclonil)、咯菌腈(fludioxonil)、异菌脲(iprodione)、腐霉利(procymidone)、苯氧喹啉(quinoxyfen)和乙烯菌核利(vinclozolin);
(n)能作为解偶联剂的化合物,例如,乐杀螨(binapacryl)、敌螨普(dinocap)、嘧菌腙(ferimzone)、氟啶胺(fluazinam)和消螨多(meptyldinocap);
(o)其他化合物,例如,苯噻硫氰(benthiazole)、贝斯氧杂嗪(bethoxazin)、卡巴西霉素(capsimycin)、香芹酮(carvone)、灭螨猛(chinomethionat)、甲氧苯啶菌(pyriofenone)(氯酚酮(chlazafenone))、硫杂灵(cufraneb)、环氟菌胺(cyflufenamid)、霜脲氰(cymoxanil)、啶酰菌胺(cyprosulfamide)、棉隆(dazomet)、咪菌威(debacarb)、双氯酚(dichlorophen)、哒菌酮(diclomezine)、野燕枯(difenzoquat)、野燕枯甲基硫酸酯(difenzoquat methyl sulphate)、二苯胺(diphenylamine)、乙克霉特(ecomate)、胺苯吡菌酮(fenpyrazamine)、氟酰菌胺(flumetover)、唑呋草(fluoroimide)、磺菌胺(flusulfamide)、氟噻菌灵(flutianil)、C.2.1乙膦酸铝、乙膦酸钙、乙膦酸钠、六氯苯(hexachlorobenzene)、人间霉素(irumamycin)、磺菌威(methasulphocarb)、异硫氰酸甲酯(methyl isothiocyanate)、苯菌酮(metrafenone)、米多霉素(mildiomycin)、纳他霉素(natamycin)、福美镍(nickel dimethyl dithiocarbamate)、酞菌酯(nitrothal-isopropyl)、辛噻酮(octhilinone)、奥克斯莫卡宾(oxamocarb)、氧代奋欣(oxyfenthiin)、五氯苯酚(pentachlorophenol)及其盐、苯醚菊酯(phenothrin)、磷酸及其盐、霜霉威乙膦酸盐(propamocarb-fosetylate)、丙烷辛钠(propanosine-sodium)、丙氧喹啉(proquinazid)、丁吡吗啉(pyrimorph)、(2E)-3-(4-叔丁基苯基)-3-(2-氯吡啶-4-基)-1-(吗啉-4-基)丙-2-烯-1-酮、(2Z)-3-(4-叔丁基苯基)-3-(2-氯吡啶-4-基)-1-(吗啉-4-基)丙-2-烯-1-酮、硝吡咯菌素(pyrrolnitrin)、异丁乙氧喹啉(tebufloquin)、叶枯酞(tecloftalam)、甲磺菌胺(tolnifanide)、咪唑嗪(triazoxide)、水杨菌胺(trichlamide)、氰菌胺(zarilamid)、(3S,6S,7R,8R)-8-苄基-3-[({3-[(异丁酰基氧基)甲氧基]-4-甲氧基吡啶-2-基}羰基)氨基]-6-甲基-4,9-二氧代-1,5-二氧壬环(dioxonan)-7-基2-甲基丙酸盐、1-(4-{4-[(5R)-5-(2,6-二氟苯基)-4,5-二氢-1,2-噁唑-3-基]-1,3-噻唑-2-基}哌啶-1-基)-2-[5-甲基-3-(三氟甲基)-1H-吡唑-1-基]乙酮、1-(4-{4-[(5S)-5-(2,6-二氟苯基)-4,5-二氢-1,2-噁唑-3-基]-1,3-噻唑-2-基}哌啶-1-基)-2-[5-甲基-3-(三氟甲基)-1H-吡唑-1-基]乙酮、1-(4-{4-[5-(2,6-二氟苯基)-4,5-二氢-1,2-噁唑-3-基]-1,3-噻唑-2-基}哌啶-1-基)-2-[5-甲基-3-(三氟甲基)-1H-吡唑-1-基]乙酮、1-(4-甲氧基苯氧基)-3,3-二甲基丁-2-基1H-咪唑-1-羧酸酯、2,3,5,6-四氯-4-(甲基磺酰基)吡啶、2,3-二丁基-6-氯噻吩并[2,3-d]嘧啶-4(3H)-酮、2-[5-甲基-3-(三氟甲基)-1H-吡唑-1-基]-1-(4-{4-[(5R)-5-苯基-4,5-二氢-1,2-噁唑-3-基]-1,3-噻唑-2-基}哌啶-1-基)乙酮、2-[5-甲基-3-(三氟甲基)-1H-吡唑-1-基]-1-(4-{4-[(5S)-5-苯基-4,5-二氢-1,2-噁唑-3-基]-1,3-噻唑-2-基}哌啶-1-基)乙酮、2-[5-甲基-3-(三氟甲基)-1H-吡唑-1-基]-1-{4-[4-(5-苯基-4,5-二氢-1,2-噁唑-3-基)-1,3-噻唑-2-基]哌啶-1-基}乙酮、2-丁氧基-6-碘-3-丙基-4H-苯并吡喃-4-酮、2-氯-5-[2-氯-1-(2,6-二氟-4-甲氧基苯基)-4-甲基-1H-咪唑-5-基]吡啶、2-苯基苯酚和盐、3-(4,4,5-三氟-3,3-二甲基-3,4-二氢异喹啉-1-基)喹啉、3,4,5-三氯吡啶-2,6-二腈、3-[5-(4-氯苯基)-2,3-二甲基-1,2-噁唑烷-3-基]吡啶、3-氯-5-(4-氯苯基)-4-(2,6-二氟苯基)-6-甲基哒嗪、4-(4-氯苯基)-5-(2,6-二氟苯基)-3,6-二甲基哒嗪、5-氨基-1,3,4-噻二唑-2-硫醇、5-氯-N'-苯基-N'-(丙-2-炔-1-基)噻吩-2-磺酰肼、5-氟-2-[(4-氟苄基)氧基]嘧啶-4-胺、5-氟-2-[(4-甲基苄基)氧基]嘧啶-4-胺、5-甲基-6-辛基[1,2,4]三唑并[1,5-a]嘧啶-7-胺、(2Z)-3-氨基-2-氰基-3-苯基丙-2-烯酸乙酯、N'-(4-{[3-(4-氯苄基)-1,2,4-噻二唑-5-基]氧基}-2,5-二甲基苯基)-N-乙基-N-甲基酰亚胺基甲酰胺、N-(4-氯苄基)-3-[3-甲氧基-4-(丙-2-炔-1-基氧基)苯基]丙酰胺、N-[(4-氯苯基)(氰基)甲基]-3-[3-甲氧基-4-(丙-2-炔-1-基氧基)苯基]丙酰胺、N-[(5-溴-3-氯吡啶-2-基)甲基]-2,4-二氯吡啶-3-甲酰胺、N-[1-(5-溴-3-氯吡啶-2-基)乙基]-2,4-二氯吡啶-3-甲酰胺、N-[1-(5-溴-3-氯吡啶-2-基)乙基]-2-氟-4-碘吡啶-3-甲酰胺、N-{(E)-[(环丙基甲氧基)亚氨基][6-(二氟甲氧基)-2,3-二氟苯基]甲基}-2-苯基乙酰胺、N-{(Z)-[(环丙基甲氧基)亚氨基][6-(二氟甲氧基)-2,3-二氟苯基]甲基}-2-苯基乙酰胺、N'-{4-[(3-叔丁基-4-氰基-1,2-噻唑-5-基)氧基]-2-氯-5-甲基苯基}-N-乙基-N-甲基酰亚胺基甲酰胺、N-甲基-2-(1-{[5-甲基-3-(三氟甲基)-1H-吡唑-1-基]乙酰基}哌啶-4-基)-N-(1,2,3,4-四氢萘-1-基)-1,3-噻唑-4-甲酰胺、N-甲基-2-(1-{[5-甲基-3-(三氟甲基)-1H-吡唑-1-基]乙酰基}哌啶-4-基)-N-[(1R)-1,2,3,4-四氢萘-1-基]-1,3-噻唑-4-甲酰胺、N-甲基-2-(1-{[5-甲基-3-(三氟甲基)-1H-吡唑-1-基]乙酰基}哌啶-4-基)-N-[(1S)-1,2,3,4-四氢萘-1-基]-1,3-噻唑-4-甲酰胺、{6-[({[(1-甲基-1H-四唑-5-基)(苯基)亚甲基]氨基}氧基)甲基]吡啶-2-基}氨基甲酸戊酯、吩嗪-1-羧酸、喹啉-8-醇、喹啉-8-醇硫酸酯(2:1)和{6-[({[(1-甲基-1H-四唑-5-基)(苯基)亚甲基]氨基}氧基)甲基]吡啶-2-基}氨基甲酸叔丁酯;
(p)其他化合物,例如,1-甲基-3-(三氟甲基)-N-[2'-(三氟甲基)联苯-2-基]-1H-吡唑-4-甲酰胺、N-(4'-氯联苯-2-基)-3-(二氟甲基)-1-甲基-1H-吡唑-4-甲酰胺、N-(2',4'-二氯联苯-2-基)-3-(二氟甲基)-1-甲基-1H-吡唑-4-甲酰胺、3-(二氟甲基)-1-甲基-N-[4'-(三氟甲基)联苯-2-基]-1H-吡唑-4-甲酰胺、N-(2',5'-二氟联苯-2-基)-1-甲基-3-(三氟甲基)-1H-吡唑-4-甲酰胺、3-(二氟甲基)-1-甲基-N-[4'-(丙-1-炔-1-基)联苯-2-基]-1H-吡唑-4-甲酰胺、5-氟-1,3-二甲基-N-[4'-(丙-1-炔-1-基)联苯-2-基]-1H-吡唑-4-甲酰胺、2-氯-N-[4'-(丙-1-炔-1-基)联苯-2-基]吡啶-3-甲酰胺、3-(二氟甲基)-N-[4'-(3,3-二甲基丁-1-炔-1-基)联苯-2-基]-1-甲基-1H-吡唑-4-甲酰胺、N-[4'-(3,3-二甲基丁-1-炔-1-基)联苯-2-基]-5-氟-1,3-二甲基-1H-吡唑-4-甲酰胺、3-(二氟甲基)-N-(4'-乙炔基联苯-2-基)-1-甲基-1H-吡唑-4-甲酰胺、N-(4'-乙炔基联苯-2-基)-5-氟-1,3-二甲基-1H-吡唑-4-甲酰胺、2-氯-N-(4'-乙炔基联苯-2-基)吡啶-3-甲酰胺、2-氯-N-[4'-(3,3-二甲基丁-1-炔-1-基)联苯-2-基]吡啶-3-甲酰胺、4-(二氟甲基)-2-甲基-N-[4'-(三氟甲基)联苯-2-基]-1,3-噻唑-5-甲酰胺、5-氟-N-[4'-(3-羟基-3-甲基丁-1-炔-1-基)联苯-2-基]-1,3-二甲基-1H-吡唑-4-甲酰胺、2-氯-N-[4'-(3-羟基-3-甲基丁-1-炔-1-基)联苯-2-基]吡啶-3-甲酰胺、3-(二氟甲基)-N-[4'-(3-甲氧基-3-甲基丁-1-炔-1-基)联苯-2-基]-1-甲基-1H-吡唑-4-甲酰胺、5-氟-N-[4'-(3-甲氧基-3-甲基丁-1-炔-1-基)联苯-2-基]-1,3-二甲基-1H-吡唑-4-甲酰胺、2-氯-N-[4'-(3-甲氧基-3-甲基丁-1-炔-1-基)联苯-2-基]吡啶-3-甲酰胺、(5-溴-2-甲氧基-4-甲基吡啶-3-基)(2,3,4-三甲氧基-6-甲基苯基)甲酮、N-[2-(4-{[3-(4-氯苯基)丙-2-炔-1-基]氧基}-3-甲氧基苯基)乙基]-N2-(甲基磺酰基)缬氨酰胺、4-氧代-4-[(2-苯基乙基)氨基]丁酸和{6-[({[(Z)-(1-甲基-1H-四唑-5-基)(苯基)亚甲基]氨基}氧基)甲基]吡啶-2-基}氨基甲酸丁-3-炔-1-基酯,及其组合。
优选的常规杀真菌剂选自C.2.1乙膦酸铝、C.2.2戊苯吡菌胺、strobilurins,特别是C.2.3肟菌酯和C.2.4嘧菌酯。
更优选的常规杀真菌剂选自C.2.1乙膦酸铝和C.2.3肟菌酯。
在本发明的含义内,选自已知或常规的杀螨剂、杀线虫剂和杀昆虫剂的化合物(C)包括:
(a)乙酰胆碱酯酶(AChE)抑制剂,例如氨基甲酸酯类,例如,棉铃威(alanycarb)、涕灭威(aldicarb)、恶虫威(bendiocarb)、丙硫克百威(benfuracarb)、丁酮威(butocarboxim)、丁酮砜威(butoxycarboxim)、甲萘威(carbaryl)、克百威(carbofuran)、丁硫克百威(carbosulfan)、乙硫苯威(ethiofencarb)、仲丁威(fenobucarb)、伐虫脒(formetanate)、呋线威(furathiocarb)、异丙威(isoprocarb)、甲硫威(methiocarb)、灭多威(methomyl)、速灭威(metolcarb)、杀线威(oxamyl)、抗蚜威(pirimicarb)、残杀威(propoxur)、硫双威(thiodicarb)、久效威(thiofanox)、唑蚜威(triazamate)、混杀威(trimethacarb)、XMC和灭杀威(xylylcarb);或有机磷酸酯类,例如,乙酰甲胺磷(acephate)、甲基吡恶磷(azamethiphos)、益棉磷(azinphos-ethyl)、保棉磷(azinphos-methyl)、硫线磷(cadusafos)、氯氧磷(chlorethoxyfos)、毒虫畏(chlorfenvinphos)、氯甲硫磷(chlormephos)、毒死蜱(Chlorpyrifos)、甲基毒死蜱(chlorpyrifos-methyl)、蝇毒磷(coumaphos)、杀螟腈(cyanophos)、甲基内吸磷(demeton-S-methyl)、二嗪磷(diazinon)、敌敌畏/DDVP(dichlorvos/DDVP)、百治磷(dicrotophos)、乐果(dimethoate)、甲基毒虫畏(dimethylvinphos)、乙拌磷(disulphoton)、苯硫磷(EPN)、乙硫磷(ethion)、灭线磷(ethoprophos)、伐灭磷(famphur)、苯线磷(fenamiphos)、杀螟硫磷(fenitrothion)、倍硫磷(fenthion)、噻唑磷(fosthiazate)、庚烯磷(heptenophos)、imicyafos、异柳磷(isofenphos)、O-(甲氧基氨基硫代磷酰基)水杨酸异丙酯(Isopropyl O-(methoxyaminothio-phosphoryl)salicylate)、恶唑磷(isoxathion)、马拉硫磷(malathion)、灭蚜磷(mecarbam)、甲胺磷(methamidophos)、杀扑磷(methidathion)、速灭磷(mevinphos)、久效磷(monocrotophos)、二溴磷(naled)、氧乐果(omethoate)、亚砜磷(oxydemeton-methyl)、对硫磷(parathion)、甲基对硫磷(parathion-methyl)、稻丰散(phenthoate)、甲拌磷(phorate)、伏杀硫磷(phosalone)、亚胺硫磷(phosmet)、磷胺(phosphamidon)、辛硫磷(phoxim)、甲基嘧啶磷(pirimiphos-methyl)、丙溴磷(profenofos)、胺丙畏(propetamphos)、丙硫磷(prothiofos)、吡唑硫磷(pyraclofos)、哒嗪硫磷(pyridaphenthion)、喹硫磷(quinalphos)、治螟磷(sulfotep)、丁基嘧啶磷(tebupirimfos)、双硫磷(temephos)、特丁硫磷(terbufos)、杀虫畏(tetrachlorvinphos)、甲基乙拌磷(thiometon)、三唑磷(triazophos)、敌百虫(triclorfon)和蚜灭磷(vamidothion);
(b)GABA门控氯化物通道拮抗剂类,例如环戊二烯有机氯类,例如,氯丹(chlordane)和硫丹(endosulfan);或苯基吡唑类(fiproles),例如,乙虫腈(ethiprole)和氟虫腈(fipronil);
(c)钠通道调节剂/电压依赖性钠通道阻断剂,例如拟除虫菊酯类,例如,氟丙菊酯(acrinathrin)、烯丙菊酯(allethrin)、(d-顺-反)烯丙菊酯(d-cis-trans allethrin)、(d-反)烯丙菊酯(d-trans allethrin)、C.3.5氟氯氰菊酯(Betacyfluthrin)、联苯菊酯(bifenthrin)、生物烯丙菊酯(bioallethrin)、生物烯丙菊酯-S-环戊烯基异构体(Bioallethrin S-cyclopentenyl isomer)、生物苄呋菊酯(bioresmethrin)、乙氰菊酯(cycloprothrin)、氟氯氰菊酯(cyfluthrin)、β-氟氯氰菊酯(beta-cyfluthrin)、氯氟氰菊酯(cyhalothrin)、λ-氯氟氰菊酯(lambda-cyhalothrin)、γ-氯氟氰菊酯(gamma-cyhalothrin)、氯氰菊酯(cypermethrin)、α-氯氰菊酯(alpha-cypermethrin)、β-氯氰菊酯(beta-cypermethrin)、θ-氯氰菊酯(theta-cypermethrin)、ζ-氯氰菊酯(zeta-cypermethrin)、苯醚氯菊酯(cyphenothrin)(1R-反式异构体)、C.3.6溴氰菊酯(deltamethrin)、右旋烯炔菊酯(empenthrin)((EZ)-(1R)异构体)、高氰戊菊酯(esfenvalerate)、醚菊酯(etofenprox)、甲氰菊酯(fenpropathrin)、氰戊菊酯(fenvalerate)、氟氰戊菊酯(flucythrinate)、氟氯苯菊酯(flumethrin)、τ-氟胺氰菊酯(tau-fluvalinate)、苄螨醚(halfenprox)、炔咪菊酯(imiprothrin)、噻嗯菊酯(kadethrin)、氯菊酯(permethrin)、苯醚菊酯(phenothrin)((1R)-反式异构体)、炔丙菊酯(prallethrin)、除虫菊素(pyrethrine)(除虫菊(pyrethrum))、苄呋菊酯(resmethrin)、氟硅菊酯(silafluofen)、七氟菊酯(tefluthrin)、胺菊酯(tetramethrin)、胺菊酯(tetramethrin)(1R异构体)、四溴菊酯(tralomethrin)和四氟苯菊酯(transfluthrin);或DDT;或甲氧滴滴涕(methoxychlor);
(d)烟碱乙酰胆碱受体(nAChR)激动剂类,例如新烟碱类(neonicotinoids,CNI’s),例如,C.3.1啶虫脒(acetamiprid)、C.3.2噻虫胺(clothianidin)、呋虫胺(dinotefuran)、C.3.3吡虫啉(imidacloprid)、烯啶虫胺(nitenpyram)、C.3.4噻虫啉(thiacloprid)和噻虫嗪(thiamethoxam);或烟碱(nicotine);
(e)烟碱乙酰胆碱受体(nAChR)变构激活剂,例如多杀霉素类(spinosyns),例如乙基多杀霉素(spinetoram)和多杀菌素(spinosad);
(f)氯化物通道激活剂类,例如阿维菌素类(avermectins)/米尔贝霉素类(milbemycins),例如,阿维菌素(abamectin)、甲氨基阿维菌素苯甲酸盐(emamectin benzoate)、雷皮菌素(lepimectin)和米尔倍霉素(milbemycin);
(g)保幼激素模拟物,例如保幼激素类似物类,例如,烯虫乙酯(hydroprene)、烯虫炔酯(kinoprene)和烯虫酯(methoprene);或苯氧威(fenoxycarb);或吡丙醚(pyriproxifen);
(h)多种非特异性(多位点)抑制剂,例如烷基卤化物类,例如,溴甲烷(Methyl bromide)和其他烷基卤化物;或氯化苦(chloropicrin);或硫酰氟(sulfuryl fluoride);或硼砂(borax);或吐酒石(tartar emetic);
(i)选择性同翅昆虫拒食剂类,例如,吡蚜酮(pymetrozine);或氟啶虫酰胺(flonicamid);
(j)螨生长抑制剂类,例如,四螨嗪(clofentezine)、噻螨酮(hexythiazox)和氟螨嗪(diflovidazin);或乙螨唑(etoxazole);
(k)昆虫肠膜的微生物干扰剂,例如苏云金芽孢杆菌以色列亚种(Bacillus thuringiensis subspecies israelensis)、苏云金芽胞杆菌鲇泽亚种(Bacillus thuringiensis subspecies aizawai)、苏云金芽孢杆菌库尔斯塔克亚种(Bacillus thuringiensis subspecies kurstaki)、苏云金芽孢杆菌拟步行甲亚种(Bacillus thuringiensis subspecies tenebrionis),以及BT作物蛋白:Cry1Ab、Cry1Ac、Cry1Fa、Cry2Ab、mCry3A、Cry3Ab、Cry3Bb、Cry34/35Ab1;
(l)线粒体ATP合成酶抑制剂,例如丁醚脲(diafenthiuron);或有机锡杀螨剂,例如三唑锡(azocyclotin)、三环锡(cyhexatin)和苯丁锡(fenbutatin oxide);或炔螨特(propargite);或三氯杀螨砜(tetradifon);
(m)通过间断质子梯度而起作用的氧化磷酸化解偶联剂类,例如虫螨腈(chlorfenapyr)、二硝甲酚(DNOC)和氟虫胺(sulfluramid);
(n)烟碱乙酰胆碱受体(nAChR)通道阻断剂类,例如杀虫磺(bensultap)、杀螟丹盐酸盐(cartap hydrochloride)、杀虫环(thiocylam)和杀虫双(thiosultap-sodium);
(o)几丁质生物合成抑制剂类,0型,例如,双三氟虫脲(bistrifluron)、定虫隆(chlofluazuron)、氟脲杀(diflubenzuron)、氟螨脲(flucycloxuron)、氟虫脲(flufenoxuron)、氟铃脲(hexaflumuron)、氟丙氧脲(lufenuron)、双苯氟脲(novaluron)、多氟脲(noviflumuron)、伏虫磷(teflubenzuron)和杀虫隆(triflumuron);
(p)几丁质生物合成抑制剂类,1型,例如噻嗪酮(buprofezin);
(q)蜕皮干扰物,例如灭蝇胺(cyromazine);
(r)蜕皮激素受体激动剂类,例如环虫酰肼(chromafenozide)、氯虫酰肼(halofenozide)、甲氧虫酰肼(methoxyfenozide)和虫酰肼(tebufenozide);
(s)章鱼胺受体激动剂类,例如双甲脒(amitraz);
(t)线粒体复合物III电子传递抑制剂类,例如灭蚁腙(hydramethylnone);或灭螨醌(acequinocyl);或嘧螨酯(fluacrypyrim);
(u)线粒体复合物I电子传递抑制剂类,例如METI杀螨剂类,例如,喹螨醚(fenazaquin)、唑螨酯(fenpyroximate)、嘧螨醚(pyrimidifen)、哒螨灵(pyridaben)、吡螨胺(tebufenpyrad)和唑虫酰胺(tolfenpyrad);或鱼藤酮(rotenone(Derris));
(v)电压依赖性钠通道阻断剂,例如茚虫威(indoxacarb);或氰氟虫胺(metaflumizone);
(w)乙酰基-辅酶A羧化酶抑制剂类,例如特窗酸和特拉姆酸衍生物,例如,酮烯醇类(ketoenols)特别是C.3.7螺虫乙酯(spirotetramat)、C.3.8螺甲螨酯(spiromesifen)和C.3.9螺螨酯(spirodiclofen);
(x)线粒体复合物IV电子传递抑制剂,例如膦类化合物,例如,磷化铝(Aluminium phosphide)、磷化钙(Calcium phosphide)、膦(Phosphine)和磷化锌(Zinc phosphide);或氰化物(Cyanide);
(y)线粒体复合物II电子传递抑制剂类,例如唑螨氰(cyenopyrafen);
(z)兰诺定(ryanodine)受体调节剂类,例如二酰胺(diamides),例如,氯虫酰胺(chlorantraniliprole)和氟虫酰胺(flubendiamide);
其他作用方式未知或不确定的活性成分,例如磺胺螨酯(amidoflumet)、印楝素(azadirachtin)、Benclothiaz、苯螨特(benzoximate)、联苯肼酯(bifenazate)、溴螨酯(bromopropylate)、灭螨锰(chinomethionat)、冰晶石(Cryolite)、氰虫酰胺(Cyantraniliprole(Cyazypyr))、丁氟螨酯(Cyflumetofen)、三氯杀螨醇(Dicofol)、氟螨嗪(Diflovidazin)、氟噻虫砜(Fluensulfone)、嘧虫胺(Flufenerim)、丁烯氟虫腈(Flufiprole)、氟吡菌酰胺(Fluopyram)、呋喃虫酰肼(Fufenozide)、氯噻啉(Imidaclothiz)、异菌脲(Iprodione)、氯氟醚菊酯(Meperfluthrin)、啶虫丙醚(Pyridalyl)、Pyrifluquinazon、四氟醚菊酯(Tetramethylfluthrin)和碘甲烷(iodomethane);以及基于坚强芽胞杆菌(Bacillus firmus)(包括但不限于菌株CNCM I-1582,例如,VotivoTM,BioNem)的产品,或下列已知的活性化合物之一:3-溴-N-{2-溴-4-氯-6-[(1-环丙基乙基)氨基甲酰基]苯基}-1-(3-氯吡啶-2-基)-1H-吡唑-5-甲酰胺(已知于WO2005/077934)、4-{[(6-溴吡啶-3-基)甲基](2-氟乙基)氨基}呋喃-2(5H)-酮(已知于WO 2007/115644)、4-{[(6-氟吡啶-3-基)甲基](2,2-二氟乙基)氨基}呋喃-2(5H)-酮(已知于WO 2007/115644)、4-{[(2-氯-1,3-噻唑-5-基)甲基](2-氟乙基)氨基}呋喃-2(5H)-酮(已知于WO 2007/115644)、4-{[(6-氯吡啶-3-基)甲基](2-氟乙基)氨基}呋喃-2(5H)-酮(已知于WO 2007/115644)、C.3.10Flupyradifurone、4-{[(6-氯-5-氟吡啶-3-基)甲基](甲基)氨基}呋喃-2(5H)-酮(已知于WO 2007/115643)、4-{[(5,6-二氯吡啶-3-基)甲基](2-氟乙基)氨基}呋喃-2(5H)-酮(已知于WO 2007/115646)、4-{[(6-氯-5-氟吡啶-3-基)甲基](环丙基)氨基}呋喃-2(5H)-酮(已知于WO 2007/115643)、4-{[(6-氯吡啶-3-基)甲基](环丙基)氨基}呋喃-2(5H)-酮(已知于EP-A-0 539 588)、4-{[(6-氯吡啶-3-基)甲基](甲基)氨基}呋喃-2(5H)-酮(已知于EP-A-0 539 588)、{[1-(6-氯吡啶-3-基)乙基](甲基)氧代(oxido)-λ4-亚硫烷基}氨腈(已知于WO 2007/149134)及其非对映异构体{[(1R)-1-(6-氯吡啶-3-基)乙基](甲基)氧代-λ4-亚硫烷基}氨腈(A)和{[(1S)-1-(6-氯吡啶-3-基)乙基](甲基)氧代-λ4-亚硫烷基}氨腈(B)(同样已知于WO 2007/149134)以及氟啶虫胺腈(sulfoxaflor)及其非对映异构体[(R)-甲基(氧代){(1R)-1-[6-(三氟甲基)吡啶-3-基]乙基}-λ4-亚硫烷基]氨腈(A1)和[(S)-甲基(氧代){(1S)-1-[6-(三氟甲基)吡啶-3-基]乙基}-λ4-亚硫烷基]氨腈(A2),称为非对映异构体组A(已知于WO 2010/074747、WO 2010/074751),[(R)-甲基(氧代){(1S)-1-[6-(三氟甲基)吡啶-3-基]乙基}-λ4-亚硫烷基]氨腈(B1)和{(S)-甲基(氧代){(1R)-1-[6-(三氟甲基)吡啶-3-基]乙基}-λ4-亚硫烷基]氨腈(B2),称为非对映异构体组B(同样已知于WO 2010/074747、WO 2010/074751),和11-(4-氯-2,6-二甲基苯基)-12-羟基-1,4-二氧杂-9-氮杂二螺[4.2.4.2]十四-11-烯-10-酮(已知于WO 2006/089633)、3-(4'-氟-2,4-二甲基联苯-3-基)-4-羟基-8-氧杂-1-氮杂螺[4.5]癸-3-烯-2-酮(已知于WO 2008/067911)、1-{2-氟-4-甲基-5-[(2,2,2-三氟乙基)亚磺酰基]苯基}-3-(三氟甲基)-1H-1,2,4-三唑-5-胺(已知于WO 2006/043635)、[(3S,4aR,12R,12aS,12bS)-3-[(环丙基羰基)氧基]-6,12-二羟基-4,12b-二甲基-11-氧代-9-(吡啶-3-基)-1,3,4,4a,5,6,6a,12,12a,12b-十氢-2H,11H-苯并[f]吡喃并[4,3-b]苯并吡喃-4-基]甲基环丙烷羧酸盐(已知于WO2008/066153)、2-氰基-3-(二氟甲氧基)-N,N-二甲基苯磺酰胺(已知于WO 2006/056433)、2-氰基-3-(二氟甲氧基)-N-甲基苯磺酰胺(已知于WO 2006/100288)、2-氰基-3-(二氟甲氧基)-N-乙基苯磺酰胺(已知于WO 2005/035486)、4-(二氟甲氧基)-N-乙基-N-甲基-1,2-苯并噻唑-3-胺1,1-二氧化物(已知于WO 2007/057407)、N-[1-(2,3-二甲基苯基)-2-(3,5-二甲基苯基)乙基]-4,5-二氢-1,3-噻唑-2-胺(已知于WO 2008/104503)、{1'-[(2E)-3-(4-氯苯基)丙-2-烯-1-基]-5-氟杂螺[吲哚-3,4'-哌啶]-1(2H)-基}(2-氯吡啶-4-基)甲酮(已知于WO2003/106457)、3-(2,5-二甲基苯基)-4-羟基-8-甲氧基-1,8-二氮杂螺[4.5]癸-3-烯-2-酮(已知于WO2009/049851)、3-(2,5-二甲基苯基)-8-甲氧基-2-氧代-1,8-二氮杂螺[4.5]癸-3-烯-4-基乙基碳酸酯(已知于WO2009/049851)、4-(丁-2-炔-1-基氧基)-6-(3,5-二甲基哌啶-1-基)-5-氟嘧啶(已知于WO2004/099160)、(2,2,3,3,4,4,5,5-八氟戊基)(3,3,3-三氟丙基)丙二腈(已知于WO2005/063094)、(2,2,3,3,4,4,5,5-八氟戊基)(3,3,4,4,4-五氟丁基)丙二腈(已知于WO2005/063094)、8-[2-(环丙基甲氧基)-4-(三氟甲基)苯氧基]-3-[6-(三氟甲基)哒嗪-3-基]-3-氮杂双环[3.2.1]辛烷(已知于WO2007/040280)、Flometoquin、PF1364(CAS注册号1204776-60-2)(已知于JP2010/018586)、5-[5-(3,5-二氯苯基)-5-(三氟甲基)-4,5-二氢-1,2-噁唑-3-基]-2-(1H-1,2,4-三唑-1-基)苯甲腈(已知于WO2007/075459)、5-[5-(2-氯吡啶-4-基)-5-(三氟甲基)-4,5-二氢-1,2-噁唑-3-基]-2-(1H-1,2,4-三唑-1-基)苯甲腈(已知于WO2007/075459)、4-[5-(3,5-二氯苯基)-5-(三氟甲基)-4,5-二氢-1,2-噁唑-3-基]-2-甲基-N-{2-氧代-2-[(2,2,2-三氟乙基)氨基]乙基}苯甲酰胺(已知于WO2005/085216)、4-{[(6-氯吡啶-3-基)甲基](环丙基)氨基}-1,3-噁唑-2(5H)-酮、4-{[(6-氯吡啶-3-基)甲基](2,2-二氟乙基)氨基}-1,3-噁唑-2(5H)-酮、4-{[(6-氯吡啶-3-基)甲基](乙基)氨基}-1,3-噁唑-2(5H)-酮、4-{[(6-氯吡啶-3-基)甲基](甲基)氨基}-1,3-噁唑-2(5H)-酮(全部已知于WO2010/005692)、NNI-0711(已知于WO2002/096882)、1-乙酰基-N-[4-(1,1,1,3,3,3-六氟-2-甲氧基丙烷-2-基)-3-异丁基苯基]-N-异丁酰基-3,5-二甲基-1H-吡唑-4-甲酰胺(已知于WO2002/096882)、2-[2-({[3-溴-1-(3-氯吡啶-2-基)-1H-吡唑-5-基]羰基}氨基)-5-氯-3-甲基苯甲酰基]-2-甲基肼羧酸甲酯(已知于WO2005/085216)、2-[2-({[3-溴-1-(3-氯吡啶-2-基)-1H-吡唑-5-基]羰基}氨基)-5-氰基-3-甲基苯甲酰基]-2-乙基肼羧酸甲酯(已知于WO2005/085216)、2-[2-({[3-溴-1-(3-氯吡啶-2-基)-1H-吡唑-5-基]羰基}氨基)-5-氰基-3-甲基苯甲酰基]-2-甲基肼羧酸甲酯(已知于WO2005/085216)、2-[3,5-二溴-2-({[3-溴-1-(3-氯吡啶-2-基)-1H-吡唑-5-基]羰基}氨基)苯甲酰基]-1,2-二乙基肼羧酸甲酯(已知于WO2005/085216)、2-[3,5-二溴-2-({[3-溴-1-(3-氯吡啶-2-基)-1H-吡唑-5-基]羰基}氨基)苯甲酰基]-2-乙基肼羧酸甲酯(已知于WO2005/085216)、(5RS,7RS;5RS,7SR)-1-(6-氯-3-吡啶基甲基)-1,2,3,5,6,7-六氢-7-甲基-8-硝基-5-丙氧基咪唑并[1,2-a]吡啶(已知于WO2007/101369)、2-{6-[2-(5-氟吡啶-3-基)-1,3-噻唑-5-基]吡啶-2-基}嘧啶(已知于WO2010/006713)、2-{6-[2-(吡啶-3-基)-1,3-噻唑-5-基]吡啶-2-基}嘧啶(已知于WO2010/006713)、1-(3-氯吡啶-2-基)-N-[4-氰基-2-甲基-6-(甲基氨基甲酰基)苯基]-3-{[5-(三氟甲基)-1H-四唑-1-基]甲基}-1H-吡唑-5-甲酰胺(已知于WO2010/069502)、1-(3-氯吡啶-2-基)-N-[4-氰基-2-甲基-6-(甲基氨基甲酰基)苯基]-3-{[5-(三氟甲基)-2H-四唑-2-基]甲基}-1H-吡唑-5-甲酰胺(已知于WO2010/069502)、N-[2-(叔丁基氨基甲酰基)-4-氰基-6-甲基苯基]-1-(3-氯吡啶-2-基)-3-{[5-(三氟甲基)-1H-四唑-1-基]甲基}-1H-吡唑-5-甲酰胺(已知于WO2010/069502)、N-[2-(叔丁基氨基甲酰基)-4-氰基-6-甲基苯基]-1-(3-氯吡啶-2-基)-3-{[5-(三氟甲基)-2H-四唑-2-基]甲基}-1H-吡唑-5-甲酰胺(已知于WO2010/069502)、(1E)-N-[(6-氯吡啶-3-基)甲基]-N'-氰基-N-(2,2-二氟乙基)乙脒(已知于WO2008/009360)、N-[2-(5-氨基-1,3,4-噻二唑-2-基)-4-氯-6-甲基苯基]-3-溴-1-(3-氯吡啶-2-基)-1H-吡唑-5-甲酰胺(已知于CN102057925)和2-[3,5-二溴-2-({[3-溴-1-(3-氯吡啶-2-基)-1H-吡唑-5-基]羰基}氨基)苯甲酰基]-2-乙基-1-甲基肼羧酸甲酯(已知于WO2011/049233),及其组合。
优选的化合物(C)选自(常规)杀昆虫剂,优选选自新烟碱类(CNI’s),特别是C.3.1啶虫脒、C.3.2噻虫胺、C.3.3吡虫啉和C.3.4噻虫啉;拟除虫菊酯类,特别是C.3.5氟氯氰菊酯和C.3.6溴氰菊酯;酮烯醇类,特别是C.3.7螺虫乙酯、C.3.8螺甲螨酯和C.3.9螺螨酯;C.3.10flupyradifurone;及其组合,特别是CNI’s和拟除虫菊酯类的组合。
更优选的常规杀昆虫剂选自C.3.3吡虫啉、C.3.4噻虫啉、C.3.5氟氯氰菊酯、C.3.6溴氰菊酯、C.3.10flupyradifurone,及其组合。
在本发明的含义内,选自微量营养素和包含微量营养素的化合物的化合物(C)包括选自包含至少一种金属离子的活性成分的化合物,所述金属离子选自锌、锰、钼、铁和铜或微量营养素硼。更优选地,这些微量营养素和包含微量营养素的化合物选自含锌化合物丙森锌、多氧菌素Z(Polyoxin Z)(锌盐)、代森锌、福美锌、噻二唑锌(zinc thiodazole)、环烷酸锌(zinc naphthenate)和代森锰锌(还包含锰),含锰化合物代森锰、代森联和代森锰铜(还包含铜),包含铁的化合物福美铁,铜(Cu)和包含铜的化合物波尔多混合液、伯更狄混合液、切欣特混合液、氧氯化铜、硫酸铜、碱性硫酸铜(例如,三碱硫酸铜)、氧化铜、辛酸铜、氢氧化铜、8-羟基喹啉铜(oxine-copper)、乙酸铜铵、环烷酸铜、螯合铜(例如,氨基酸螯合物)、代森锰铜、acypetacs-铜、乙酸铜、碱性碳酸铜、油酸铜、硅酸铜、铬酸铜锌、硫杂灵、福美铜氯(cuprobam)、噻森铜(saisentong)和噻二唑铜,及其组合。
优选地,所述微量营养素和包含微量营养素的化合物选自C.4.1铜(Cu)、C.4.2氢氧化铜、C.4.3硫酸铜、C.4.4氧氯化铜、C.4.5丙森锌和C.4.6代森锰锌。更优选地,所述微量营养素和包含微量营养素的化合物选自C.4.2氢氧化铜、C.4.3硫酸铜、C.4.5丙森锌和C.4.6代森锰锌。最优选C.4.5丙森锌和C.4.6代森锰锌。
在本发明的含义中,选自脂壳寡糖化合物(LCO)的化合物(C)包括具有通常的LCO结构的化合物,即β-1,4-连接的N-乙酰基-D-葡萄糖胺残基的低聚物骨架,其中在非还原端具有N连接的脂肪酰基链,如美国专利第5549718号、美国专利第5,646,018号、美国专利第5,175,149号和美国专利第5,321,011号中所描述。这一基本结构可包含在天然存在的LCO's结构中发现的修饰或取代,如Spaink,Critical Reviews in Plant Sciences 54:257-288,2000;D'Haeze and Holsters,Glycobiology 12:79R-105R,2002中所描述的那些修饰或取代。天然存在的LCO's被定义为可在自然界发现的化合物。这一基本结构还可包含迄今为止在天然存在的LCO's中未发现的修饰或取代。这类类似物的实例——其共轭酰胺键被苯甲酰胺键模拟或包含苄胺型官能团——是在WO 2005/063784和WO 2008/071672中所描述的以下式(I)化合物,所述文献内容以引用的方式纳入本文。LCO's化合物可直接从根瘤菌科细菌菌株的特定培养物中分离、可化学合成或可通过化学-酶法获得。通过后一种方法,寡糖骨架可通过在发酵罐中培养重组细菌菌株如大肠杆菌(Escherichia coli)来形成,然后可化学连接脂质链。本发明的实施方案中使用的LCO's可从产生LCO's的天然根瘤菌科细菌菌株中回收,或从被遗传改造以产生LCO's的细菌菌株中回收,所述天然根瘤菌科细菌菌株为例如固氮根瘤菌属(Azorhizobium)、慢生根瘤菌属(Bradyrhizobium)(包括大豆慢生根瘤菌(B.japonicum))、中间根瘤菌属(Mesorhizobium)、根瘤菌属(包括豌豆根瘤菌(R.leguminosarum))、中华根瘤菌属(Sinorhizobium)(包括苜蓿中华根瘤菌(S.meliloti))。这些方法在本领域中是已知的并记载于例如美国专利第5,549,718号和第5,646,018号中,其以引用的方式纳入本文。Hungria和Stacey(Soil Biol.Biochem.29:819-830,1997)列出了由不同根瘤菌物种产生的具体的LCO结构。LCO's可以多种纯度形式利用且可单独使用或与根瘤菌一起使用。仅提供LCO's的方法包括从LCO和根瘤菌的混合物中简单除去根瘤菌细胞,或通过LCO溶剂相分离然后进行HPLC色谱法来继续分离并纯化LCO分子,如Lerouge等人(US 5,549,718)所描述。通过重复的HPLC可提高纯化程度,纯化的LCO分子可被冻干以长期保存。这种方法适用于由根瘤菌科的所有属和种产生LCO's。可获得包含LCO's的商用产品,例如(EMD Crop BioScience)。通过化学合成和/或通过基因工程还可获得与天然存在的LCO's相同或不同的LCO化合物。在Samain et al.,Carbohydrate Research 302:35-42,1997中公开了用于通过基因工程生物构建LCO的前体寡糖分子的合成。在WO 2005/063784和WO 2008/07167中公开了制备大量LCO化合物的方法,其中寡糖骨架通过培养重组细菌菌株例如含有来自根瘤菌的异源基因的重组大肠杆菌细胞而获得,且其中脂质链通过化学方法连接,所述文献内容以引用的方式纳入本文。脂壳寡糖化合物的实例包括但不限于特别地在WO 2010/125065中公开的LCO化合物。
在本发明的含义中,选自土壤改良产品或用于减少植物胁迫的产品的化合物(C)包括例如C.5Myconate。
此外,在本发明的含义内,化合物(C)可选自至少一种选自以下的活性化合物:
乙酸(例如,萘乙酸)、过乙酸、有机酸(例如,柠檬酸、乳酸)、氨基酸(例如,L-精氨酸)、腐植酸、富里酸、硼酸、奥索利酸(oxolinic acid)、1,2,3-苯并噻二唑-7-硫代羧酸-S-甲酯、5-羟基-1,4-萘二酮、溴-氯-二甲基乙内酰脲、三氯异氰尿酸、水杨酸、双氯酚、卡那霉素、春雷霉素、链霉素、硫酸链霉素、氧四环素、庆大霉素(例如,硫酸庆大霉素水合物)、吡虫啉、戊唑醇、噻菌灵、福美双、teracep、辛噻酮、苯氧喹啉、印楝素、呋喃黄酮(furanoflavone)、氯吡脲(forchlorfenuron)、植物矿物质(例如,钙、碳酸钙、次氯酸盐、EDTA钙)、酶(例如,蛋白酶、淀粉酶、脂酶)、痕量元素和螯合的痕量元素(例如,氨基酸螯合物)、维生素和植物提取物、水杨酸衍生物、生物黄酮(bioflavonoids)和来自蔬菜和水果的有机酸、天然水果提取的多酚、苦橙皮油、柑橘提取物、壳聚糖、淀粉、海藻提取物、有机硅、有活性的离子化硅复合物蜂蜡、尿素、枯草芽孢杆菌、解淀粉芽孢杆菌、荧光假单胞菌(Pseudomonas fluorescens)、恶臭假单胞菌(Pseudomonas putida)、成团泛菌、康氏木霉(Trichoderma koningii)、哈茨木霉(Trichoderma harzianum)、氯和氯化合物(例如,经氯化的水、二氧化氯、亚氯酸钠、次氯酸钠、次氯酸、氯化铵、二癸基二甲基氯化铵、苯扎氯铵)、氧、过氧化氢(H2O2)和过氧化物、氰胺(hydrogen cyanamide)、硫酸镍(III)、过硫酸钠、亚磷酸盐(例如金属亚磷酸盐,特别是乙基亚磷酸铝)、磷酸盐、磷酸三钠、磷酸、无机氮、银和包含银的化合物(例如,胶体银)、戊二醛、鼠李糖脂
其中优选亚磷酸盐,例如金属亚磷酸盐,特别是乙基亚磷酸铝。
优选地,所述宿主防御诱导剂和生物防治剂存在于包含至少一种其他化合物(C)的结合物中,所述化合物(C)选自分别如以上所定义的(常规)杀细菌剂、(常规)抗生素、(常规)杀真菌剂、(常规)杀昆虫剂、(常规)除草剂,其分别不属于生物防治剂(B)、微量营养素和包含微量营养素的化合物,以及脂壳寡糖化合物(LCO)。
优选地,至少一种其他化合物(C)选自乙膦酸铝;金属亚磷酸盐,特别是乙基亚磷酸铝;戊苯吡菌胺;strobilurins,特别是肟菌酯;新烟碱类(CNI’s),特别是啶虫脒、噻虫胺、吡虫啉和噻虫啉;拟除虫菊酯类,特别是氟氯氰菊酯和溴氰菊酯;flupyradifurone;酮烯醇类,特别是螺虫乙酯、螺甲螨酯和螺螨酯;含铜和/或锌的化合物,特别是氢氧化铜、硫酸铜、丙森锌和代森锰锌;脂壳寡糖化合物(LCO);以及选自春雷霉素、链霉素和氧四环素的常规抗生素。
更优选地,至少一种其他化合物(C)选自乙膦酸铝、乙基亚磷酸铝、肟菌酯、吡虫啉、噻虫啉、氟氯氰菊酯、溴氰菊酯、flupyradifurone及其组合;选自春雷霉素、链霉素和氧四环素的常规抗生素。
本发明的一个特别优选的实施方案涉及一种结合物的用途,其中
(A)宿主防御诱导剂是异噻菌胺,
(B)生物防治剂选自
(1)由枯草芽孢杆菌菌株QST713/AQ713(NRRL登录号B21661)、枯草芽孢杆菌菌株AQ153(NRRL登录号55614)、芽孢杆菌属菌株AQ175(ATCC登录号55608)、芽孢杆菌属菌株AQ177(ATCC登录号55609),以及芽孢杆菌属菌株AQ178(ATCC登录号53522)组成的细菌;和
(2)由Pseudozyma aphidis组成的真菌,并且
(C)至少一种其他化合物选自乙膦酸铝、乙基亚磷酸铝、肟菌酯、吡虫啉、噻虫啉、氟氯氰菊酯、溴氰菊酯、flupyradifurone,及其组合;选自春雷霉素、链霉素和氧四环素的其他抗生素。
本发明的一个甚至更优选的实施方案涉及一种结合物的用途,其中
(A)宿主防御诱导剂是异噻菌胺和苯并噻二唑的结合物,
(B)生物防治剂选自
(1)由枯草芽孢杆菌菌株QST713/AQ713(NRRL登录号B21661)、枯草芽孢杆菌菌株AQ153(NRRL登录号55614)、芽孢杆菌属菌株AQ175(ATCC登录号55608)、芽孢杆菌属菌株AQ177(ATCC登录号55609),以及芽孢杆菌属菌株AQ178(ATCC登录号53522)组成的细菌;和
(2)由Pseudozyma aphidis组成的真菌,并且
(C)至少一种其他化合物选自乙膦酸铝、乙基亚磷酸铝、肟菌酯、吡虫啉、噻虫啉、氟氯氰菊酯、溴氰菊酯、flupyradifurone,及其组合;选自春雷霉素、链霉素和氧四环素的其他抗生素。
根据本发明,优选选自以下的二元结合物:
(A.1)+(B.1.1),(A.2)+(B.1.1),(A.3)+(B.1.1),(A.4)+(B.1.1),(A.1)+(B.1.2),(A.2)+(B.1.2),(A.3)+(B.1.2),(A.4)+(B.1.2),(A.1)+(B.1.3),(A.2)+(B.1.3),(A.3)+(B.1.3),(A.4)+(B.1.3),(A.1)+(B.1.4),(A.2)+(B.1.4),(A.3)+(B.1.4),(A.4)+(B.1.4),(A.1)+(B.1.5),(A.2)+(B.1.5),(A.3)+(B.1.5),(A.4)+(B.1.5),(A.1)+(B.1.6),(A.2)+(B.1.6),(A.3)+(B.1.6),(A.4)+(B.1.6),(A.1)+(B.1.7),(A.2)+(B.1.7),(A.3)+(B.1.7),(A.4)+(B.1.7),(A.1)+(B.1.8),(A.2)+(B.1.8),(A.3)+(B.1.8),(A.4)+(B.1.8),(A.1)+(B.1.9),(A.2)+(B.1.9),(A.3)+(B.1.9),(A.4)+(B.1.9),(A.1)+(B.1.10),(A.2)+(B.1.10),(A.3)+(B.1.10),(A.4)+(B.1.10),(A.1)+(B.1.11),(A.2)+(B.1.11),(A.3)+(B.1.11),(A.4)+(B.1.11),(A.1)+(B.1.12),(A.2)+(B.1.12),(A.3)+(B.1.12),(A.4)+(B.1.12),(A.1)+(B.1.13),(A.2)+(B.1.13),(A.3)+(B.1.13),(A.4)+(B.1.13),(A.1)+(B.1.14),(A.2)+(B.1.14),(A.3)+(B.1.14),(A.4)+(B.1.14),(A.1)+(B.1.15),(A.2)+(B.1.15),(A.3)+(B.1.15),(A.4)+(B.1.15),(A.1)+(B.1.16),(A.2)+(B.1.16),(A.3)+(B.1.16),(A.4)+(B.1.16),(A.1)+(B.1.17),(A.2)+(B.1.17),(A.3)+(B.1.17),(A.4)+(B.1.17),
(A.1)+(B.2.1),(A.2)+(B.2.1),(A.3)+(B.2.1),(A.4)+(B.2.1),(A.1)+(B.2.2),(A.2)+(B.2.2),(A.3)+(B.2.2),(A.4)+(B.2.2),(A.1)+(B.2.3),(A.2)+(B.2.3),(A.3)+(B.2.3),(A.4)+(B.2.3),(A.1)+(B.2.4),(A.2)+(B.2.4),(A.3)+(B.2.4),(A.4)+(B.2.4),(A.1)+(B.2.5),(A.2)+(B.2.5),(A.3)+(B.2.5),(A.4)+(B.2.5),(A.1)+(B.2.6),(A.2)+(B.2.6),(A.3)+(B.2.6),(A.4)+(B.2.6),(A.1)+(B.2.7),(A.2)+(B.2.7),(A.3)+(B.2.7),(A.4)+(B.2.7),(A.1)+(B.2.8),(A.2)+(B.2.8),(A.3)+(B.2.8),(A.4)+(B.2.8)。
其中甚至进一步优选以下结合物:
(A.1)+(B.1.1),(A.2)+(B.1.1),(A.1)+(B.1.2),(A.2)+(B.1.2),(A.1)+(B.1.3),(A.2)+(B.1.3),(A.1)+(B.1.4),(A.2)+(B.1.4),(A.1)+(B.1.5),(A.2)+(B.1.5),(A.1)+(B.1.6),(A.2)+(B.1.6),(A.1)+(B.1.7),(A.2)+(B.1.7),(A.1)+(B.1.8),(A.2)+(B.1.8),(A.1)+(B.1.9),(A.2)+(B.1.9),(A.1)+(B.1.10),(A.2)+(B.1.10),(A.1)+(B.1.11),(A.2)+(B.1.11),
(A.1)+(B.2.1),(A.2)+(B.2.1)。
最优选以下结合物:
(A.1)+(B.1.1),(A.2)+(B.1.1),(A.1)+(B.1.2),(A.2)+(B.1.2),(A.1)+(B.1.3),(A.2)+(B.1.3),(A.1)+(B.1.4),(A.2)+(B.1.4),(A.1)+(B.1.5),(A.2)+(B.1.5),
(A.1)+(B.2.1),(A.2)+(B.2.1)。
其中最优选的是结合物(A.2)+(B.1.1)。
以上提及的所有二元结合物可以与至少一种其他已知的杀细菌剂、抗生素、杀真菌剂、杀螨剂、杀线虫剂、除草剂、杀昆虫剂、微量营养素和包含微量营养素的化合物、安全剂、脂壳寡糖化合物(LCO)、土壤改良产品或减少植物胁迫的产品(例如Myconate)结合,以例如扩大作用范围或阻止抗性发展。
根据本发明,优选选自以下的三元结合物:
(A.1)+(A.2)+(B.1.1),(A.1)+(A.2)+(B.1.2),(A.1)+(A.2)+(B.1.3),(A.1)+(A.2)+(B.1.4),(A.1)+(A.2)+(B.1.5),(A.1)+(A.2)+(B.1.6),(A.1)+(A.2)+(B.1.7),(A.1)+(A.2)+(B.1.8),(A.1)+(A.2)+(B.1.9),(A.1)+(A.2)+(B.1.10),(A.1)+(A.2)+(B.1.11),(A.1)+(A.2)+(B.2.1.)。
还优选选自以下的四元结合物:
(A.1)+(A.2)+(B.1.1)+(C.1.1),(A.1)+(A.2)+(B.1.1)+(C.1.2),(A.1)+(A.2)+(B.1.1)+(C.1.3),(A.1)+(A.2)+(B.1.1)+(C.2.1),(A.1)+(A.2)+(B.1.1)+(C.2.3),(A.1)+(A.2)+(B.1.1)+(C.3.3),(A.1)+(A.2)+(B.1.1)+(C.3.10),(A.1)+(A.2)+(B.1.1)+(C.4.5),(A.1)+(A.2)+(B.1.1)+(C.4.6),(A.1)+(A.2)+(B.1.1)+(C.5),
(A.1)+(A.2)+(B.1.2)+(C.1.1),(A.1)+(A.2)+(B.1.2)+(C.1.2),(A.1)+(A.2)+(B.1.2)+(C.1.3),(A.1)+(A.2)+(B.1.2)+(C.2.1),(A.1)+(A.2)+(B.1.2)+(C.2.3),(A.1)+(A.2)+(B.1.2)+(C.3.3),(A.1)+(A.2)+(B.1.2)+(C.3.10),(A.1)+(A.2)+(B.1.2)+(C.4.5),(A.1)+(A.2)+(B.1.2)+(C.4.6),(A.1)+(A.2)+(B.1.2)+(C.5),
(A.1)+(A.2)+(B.1.3)+(C.1.1),(A.1)+(A.2)+(B.1.3)+(C.1.2),(A.1)+(A.2)+(B.1.3)+(C.1.3),(A.1)+(A.2)+(B.1.3)+(C.2.1),(A.1)+(A.2)+(B.1.3)+(C.2.3),(A.1)+(A.2)+(B.1.3)+(C.3.3),(A.1)+(A.2)+(B.1.3)+(C.3.10),(A.1)+(A.2)+(B.1.3)+(C.4.5),(A.1)+(A.2)+(B.1.3)+(C.4.6),(A.1)+(A.2)+(B.1.3)+(C.5),
(A.1)+(A.2)+(B.1.4)+(C.1.1),(A.1)+(A.2)+(B.1.4)+(C.1.2),(A.1)+(A.2)+(B.1.4)+(C.1.3),(A.1)+(A.2)+(B.1.4)+(C.2.1),(A.1)+(A.2)+(B.1.4)+(C.2.3),(A.1)+(A.2)+(B.1.4)+(C.3.3),(A.1)+(A.2)+(B.1.4)+(C.3.10),(A.1)+(A.2)+(B.1.4)+(C.4.5),(A.1)+(A.2)+(B.1.4)+(C.4.6),(A.1)+(A.2)+(B.1.4)+(C.5),
(A.1)+(A.2)+(B.1.5)+(C.1.1),(A.1)+(A.2)+(B.1.5)+(C.1.2),(A.1)+(A.2)+(B.1.5)+(C.1.3),(A.1)+(A.2)+(B.1.5)+(C.2.1),(A.1)+(A.2)+(B.1.5)+(C.2.3),(A.1)+(A.2)+(B.1.5)+(C.3.3),(A.1)+(A.2)+(B.1.5)+(C.3.10),(A.1)+(A.2)+(B.1.5)+(C.4.5),(A.1)+(A.2)+(B.1.5)+(C.4.6),(A.1)+(A.2)+(B.1.5)+(C.5),
(A.1)+(A.2)+(B.1.6)+(C.1.1),(A.1)+(A.2)+(B.1.6)+(C.1.2),(A.1)+(A.2)+(B.1.6)+(C.1.3),(A.1)+(A.2)+(B.1.6)+(C.2.1),(A.1)+(A.2)+(B.1.6)+(C.2.3),(A.1)+(A.2)+(B.1.6)+(C.3.3),(A.1)+(A.2)+(B.1.6)+(C.3.10),(A.1)+(A.2)+(B.1.6)+(C.4.5),(A.1)+(A.2)+(B.1.6)+(C.4.6),(A.1)+(A.2)+(B.1.6)+(C.5),
(A.1)+(A.2)+(B.1.7)+(C.1.1),(A.1)+(A.2)+(B.1.7)+(C.1.2),(A.1)+(A.2)+(B.1.7)+(C.1.3),(A.1)+(A.2)+(B.1.7)+(C.2.1),(A.1)+(A.2)+(B.1.7)+(C.2.3),(A.1)+(A.2)+(B.1.7)+(C.3.3),(A.1)+(A.2)+(B.1.7)+(C.3.10),(A.1)+(A.2)+(B.1.7)+(C.4.5),(A.1)+(A.2)+(B.1.7)+(C.4.6),(A.1)+(A.2)+(B.1.7)+(C.5),
(A.1)+(A.2)+(B.1.8)+(C.1.1),(A.1)+(A.2)+(B.1.8)+(C.1.2),(A.1)+(A.2)+(B.1.8)+(C.1.3),(A.1)+(A.2)+(B.1.8)+(C.2.1),(A.1)+(A.2)+(B.1.8)+(C.2.3),(A.1)+(A.2)+(B.1.8)+(C.3.3),(A.1)+(A.2)+(B.1.8)+(C.3.10),(A.1)+(A.2)+(B.1.8)+(C.4.5),(A.1)+(A.2)+(B.1.8)+(C.4.6),(A.1)+(A.2)+(B.1.8)+(C.5),
(A.1)+(A.2)+(B.1.9)+(C.1.1),(A.1)+(A.2)+(B.1.9)+(C.1.2),(A.1)+(A.2)+(B.1.9)+(C.1.3),(A.1)+(A.2)+(B.1.9)+(C.2.1),(A.1)+(A.2)+(B.1.9)+(C.2.3),(A.1)+(A.2)+(B.1.9)+(C.3.3),(A.1)+(A.2)+(B.1.9)+(C.3.10),(A.1)+(A.2)+(B.1.9)+(C.4.5),(A.1)+(A.2)+(B.1.9)+(C.4.6),(A.1)+(A.2)+(B.1.9)+(C.5),
(A.1)+(A.2)+(B.1.10)+(C.1.1),(A.1)+(A.2)+(B.1.10)+(C.1.2),(A.1)+(A.2)+(B.1.10)+(C.1.3),(A.1)+(A.2)+(B.1.10)+(C.2.1),(A.1)+(A.2)+(B.1.10)+(C.2.3),(A.1)+(A.2)+(B.1.10)+(C.3.3),(A.1)+(A.2)+(B.1.10)+(C.3.10),(A.1)+(A.2)+(B.1.10)+(C.4.5),(A.1)+(A.2)+(B.1.10)+(C.4.6),(A.1)+(A.2)+(B.1.10)+(C.5),
(A.1)+(A.2)+(B.1.11)+(C.1.1),(A.1)+(A.2)+(B.1.11)+(C.1.2),(A.1)+(A.2)+(B.1.11)+(C.1.3),(A.1)+(A.2)+(B.1.11)+(C.2.1),(A.1)+(A.2)+(B.1.11)+(C.2.3),(A.1)+(A.2)+(B.1.11)+(C.3.3),(A.1)+(A.2)+(B.1.11)+(C.3.10),(A.1)+(A.2)+(B.1.11)+(C.4.5),(A.1)+(A.2)+(B.1.11)+(C.4.6),(A.1)+(A.2)+(B.1.11)+(C.5),
(A.1)+(A.2)+(B.2.1)+(C.1.1),(A.1)+(A.2)+(B.2.1)+(C.1.2),(A.1)+(A.2)+(B.2.1)+(C.1.3),(A.1)+(A.2)+(B.2.1)+(C.2.1),(A.1)+(A.2)+(B.2.1)+(C.2.3),(A.1)+(A.2)+(B.2.1)+(C.3.3),(A.1)+(A.2)+(B.2.1)+(C.3.10),(A.1)+(A.2)+(B.2.1)+(C.4.5),(A.1)+(A.2)+(B.2.1)+(C.4.6),(A.1)+(A.2)+(B.2.1)+(C.5),
根据本发明,优选选自以下的三元结合物:
(A.1)+(B.1.1)+(C.1.1),(A.2)+(B.1.1)+(C.1.1),(A.3)+(B.1.1)+(C.1.1),(A.4)+(B.1.1)+(C.1.1),(A.1)+(B.1.2)+(C.1.1),(A.2)+(B.1.2)+(C.1.1),(A.3)+(B.1.2)+(C.1.1),(A.4)+(B.1.2)+(C.1.1),(A.1)+(B.1.3)+(C.1.1),(A.2)+(B.1.3)+(C.1.1),(A.3)+(B.1.3)+(C.1.1),(A.4)+(B.1.3)+(C.1.1),(A.1)+(B.1.4)+(C.1.1),(A.2)+(B.1.4)+(C.1.1),(A.3)+(B.1.4)+(C.1.1),(A.4)+(B.1.4)+(C.1.1),(A.1)+(B.1.5)+(C.1.1),(A.2)+(B.1.5)+(C.1.1),(A.3)+(B.1.5)+(C.1.1),(A.4)+(B.1.5)+(C.1.1),(A.1)+(B.1.6)+(C.1.1),(A.2)+(B.1.6)+(C.1.1),(A.3)+(B.1.6)+(C.1.1),(A.4)+(B.1.6)+(C.1.1),(A.1)+(B.1.7)+(C.1.1),(A.2)+(B.1.7)+(C.1.1),(A.3)+(B.1.7)+(C.1.1),(A.4)+(B.1.7)+(C.1.1),(A.1)+(B.1.8)+(C.1.1),(A.2)+(B.1.8)+(C.1.1),(A.3)+(B.1.8)+(C.1.1),(A.4)+(B.1.8)+(C.1.1),(A.1)+(B.1.9)+(C.1.1),(A.2)+(B.1.9)+(C.1.1),(A.3)+(B.1.9)+(C.1.1),(A.4)+(B.1.9)+(C.1.1),(A.1)+(B.1.10)+(C.1.1),(A.2)+(B.1.10)+(C.1.1),(A.3)+(B.1.10)+(C.1.1),(A.4)+(B.1.10)+(C.1.1),(A.1)+(B.1.11)+(C.1.1),(A.2)+(B.1.11)+(C.1.1),(A.3)+(B.1.11)+(C.1.1),(A.4)+(B.1.11)+(C.1.1),(A.1)+(B.1.12)+(C.1.1),(A.2)+(B.1.12)+(C.1.1),(A.3)+(B.1.12)+(C.1.1),(A.4)+(B.1.12)+(C.1.1),(A.1)+(B.1.13)+(C.1.1),(A.2)+(B.1.13)+(C.1.1),(A.3)+(B.1.13)+(C.1.1),(A.4)+(B.1.13)+(C.1.1),(A.1)+(B.1.14)+(C.1.1),(A.2)+(B.1.14)+(C.1.1),(A.3)+(B.1.14)+(C.1.1),(A.4)+(B.1.14)+(C.1.1),(A.1)+(B.1.15)+(C.1.1),(A.2)+(B.1.15)+(C.1.1),(A.3)+(B.1.15)+(C.1.1),(A.4)+(B.1.15)+(C.1.1),(A.1)+(B.1.16)+(C.1.1),(A.2)+(B.1.16)+(C.1.1),(A.3)+(B.1.16)+(C.1.1),(A.4)+(B.1.16)+(C.1.1),(A.1)+(B.1.17)+(C.1.1),(A.2)+(B.1.17)+(C.1.1),(A.3)+(B.1.17)+(C.1.1),(A.4)+(B.1.17)+(C.1.1),
(A.1)+(B.2.1)+(C.1.1),(A.2)+(B.2.1)+(C.1.1),(A.3)+(B.2.1)+(C.1.1),(A.4)+(B.2.1)+(C.1.1),(A.1)+(B.2.2)+(C.1.1),(A.2)+(B.2.2)+(C.1.1),(A.3)+(B.2.2)+(C.1.1),(A.4)+(B.2.2)+(C.1.1),(A.1)+(B.2.3)+(C.1.1),(A.2)+(B.2.3)+(C.1.1),(A.3)+(B.2.3)+(C.1.1),(A.4)+(B.2.3)+(C.1.1),(A.1)+(B.2.4)+(C.1.1),(A.2)+(B.2.4)+(C.1.1),(A.3)+(B.2.4)+(C.1.1),(A.4)+(B.2.4)+(C.1.1),(A.1)+(B.2.5)+(C.1.1),(A.2)+(B.2.5)+(C.1.1),(A.3)+(B.2.5)+(C.1.1),(A.4)+(B.2.5)+(C.1.1),(A.1)+(B.2.6)+(C.1.1),(A.2)+(B.2.6)+(C.1.1),(A.3)+(B.2.6)+(C.1.1),(A.4)+(B.2.6)+(C.1.1),(A.1)+(B.2.7)+(C.1.1),(A.2)+(B.2.7)+(C.1.1),(A.3)+(B.2.7)+(C.1.1),(A.4)+(B.2.7)+(C.1.1),(A.1)+(B.2.8)+(C.1.1),(A.2)+(B.2.8)+(C.1.1),(A.3)+(B.2.8)+(C.1.1),(A.4)+(B.2.8)+(C.1.1)。
(A.1)+(B.1.1)+(C.1.2),(A.2)+(B.1.1)+(C.1.2),(A.3)+(B.1.1)+(C.1.2),(A.4)+(B.1.1)+(C.1.2),(A.1)+(B.1.2)+(C.1.2),(A.2)+(B.1.2)+(C.1.2),(A.3)+(B.1.2)+(C.1.2),(A.4)+(B.1.2)+(C.1.2),(A.1)+(B.1.3)+(C.1.2),(A.2)+(B.1.3)+(C.1.2),(A.3)+(B.1.3)+(C.1.2),(A.4)+(B.1.3)+(C.1.2),(A.1)+(B.1.4)+(C.1.2),(A.2)+(B.1.4)+(C.1.2),(A.3)+(B.1.4)+(C.1.2),(A.4)+(B.1.4)+(C.1.2),(A.1)+(B.1.5)+(C.1.2),(A.2)+(B.1.5)+(C.1.2),(A.3)+(B.1.5)+(C.1.2),(A.4)+(B.1.5)+(C.1.2),(A.1)+(B.1.6)+(C.1.2),(A.2)+(B.1.6)+(C.1.2),(A.3)+(B.1.6)+(C.1.2),(A.4)+(B.1.6)+(C.1.2),(A.1)+(B.1.7)+(C.1.2),(A.2)+(B.1.7)+(C.1.2),(A.3)+(B.1.7)+(C.1.2),(A.4)+(B.1.7)+(C.1.2),(A.1)+(B.1.8)+(C.1.2),(A.2)+(B.1.8)+(C.1.2),(A.3)+(B.1.8)+(C.1.2),(A.4)+(B.1.8)+(C.1.2),(A.1)+(B.1.9)+(C.1.2),(A.2)+(B.1.9)+(C.1.2),(A.3)+(B.1.9)+(C.1.2),(A.4)+(B.1.9)+(C.1.2),(A.1)+(B.1.10)+(C.1.2),(A.2)+(B.1.10)+(C.1.2),(A.3)+(B.1.10)+(C.1.2),(A.4)+(B.1.10)+(C.1.2),(A.1)+(B.1.11)+(C.1.2),(A.2)+(B.1.11)+(C.1.2),(A.3)+(B.1.11)+(C.1.2),(A.4)+(B.1.11)+(C.1.2),(A.1)+(B.1.12)+(C.1.2),(A.2)+(B.1.12)+(C.1.2),(A.3)+(B.1.12)+(C.1.2),(A.4)+(B.1.12)+(C.1.2),(A.1)+(B.1.13)+(C.1.2),(A.2)+(B.1.13)+(C.1.2),(A.3)+(B.1.13)+(C.1.2),(A.4)+(B.1.13)+(C.1.2),(A.1)+(B.1.14)+(C.1.2),(A.2)+(B.1.14)+(C.1.2),(A.3)+(B.1.14)+(C.1.2),(A.4)+(B.1.14)+(C.1.2),(A.1)+(B.1.15)+(C.1.2),(A.2)+(B.1.15)+(C.1.2),(A.3)+(B.1.15)+(C.1.2),(A.4)+(B.1.15)+(C.1.2),(A.1)+(B.1.16)+(C.1.2),(A.2)+(B.1.16)+(C.1.2),(A.3)+(B.1.16)+(C.1.2),(A.4)+(B.1.16)+(C.1.2),(A.1)+(B.1.17)+(C.1.2),(A.2)+(B.1.17)+(C.1.2),(A.3)+(B.1.17)+(C.1.2),(A.4)+(B.1.17)+(C.1.2),
(A.1)+(B.2.1)+(C.1.2),(A.2)+(B.2.1)+(C.1.2),(A.3)+(B.2.1)+(C.1.2),(A.4)+(B.2.1)+(C.1.2),(A.1)+(B.2.2)+(C.1.2),(A.2)+(B.2.2)+(C.1.2),(A.3)+(B.2.2)+(C.1.2),(A.4)+(B.2.2)+(C.1.2),(A.1)+(B.2.3)+(C.1.2),(A.2)+(B.2.3)+(C.1.2),(A.3)+(B.2.3)+(C.1.2),(A.4)+(B.2.3)+(C.1.2),(A.1)+(B.2.4)+(C.1.2),(A.2)+(B.2.4)+(C.1.2),(A.3)+(B.2.4)+(C.1.2),(A.4)+(B.2.4)+(C.1.2),(A.1)+(B.2.5)+(C.1.2),(A.2)+(B.2.5)+(C.1.2),(A.3)+(B.2.5)+(C.1.2),(A.4)+(B.2.5)+(C.1.2),(A.1)+(B.2.6)+(C.1.2),(A.2)+(B.2.6)+(C.1.2),(A.3)+(B.2.6)+(C.1.2),(A.4)+(B.2.6)+(C.1.2),(A.1)+(B.2.7)+(C.1.2),(A.2)+(B.2.7)+(C.1.2),(A.3)+(B.2.7)+(C.1.2),(A.4)+(B.2.7)+(C.1.2),(A.1)+(B.2.8)+(C.1.2),(A.2)+(B.2.8)+(C.1.2),(A.3)+(B.2.8)+(C.1.2),(A.4)+(B.2.8)+(C.1.2)。
(A.1)+(B.1.1)+(C.1.3),(A.2)+(B.1.1)+(C.1.3),(A.3)+(B.1.1)+(C.1.3),(A.4)+(B.1.1)+(C.1.3),(A.1)+(B.1.2)+(C.1.3),(A.2)+(B.1.2)+(C.1.3),(A.3)+(B.1.2)+(C.1.3),(A.4)+(B.1.2)+(C.1.3),(A.1)+(B.1.3)+(C.1.3),(A.2)+(B.1.3)+(C.1.3),(A.3)+(B.1.3)+(C.1.3),(A.4)+(B.1.3)+(C.1.3),(A.1)+(B.1.4)+(C.1.3),(A.2)+(B.1.4)+(C.1.3),(A.3)+(B.1.4)+(C.1.3),(A.4)+(B.1.4)+(C.1.3),(A.1)+(B.1.5)+(C.1.3),(A.2)+(B.1.5)+(C.1.3),(A.3)+(B.1.5)+(C.1.3),(A.4)+(B.1.5)+(C.1.3),(A.1)+(B.1.6)+(C.1.3),(A.2)+(B.1.6)+(C.1.3),(A.3)+(B.1.6)+(C.1.3),(A.4)+(B.1.6)+(C.1.3),(A.1)+(B.1.7)+(C.1.3),(A.2)+(B.1.7)+(C.1.3),(A.3)+(B.1.7)+(C.1.3),(A.4)+(B.1.7)+(C.1.3),(A.1)+(B.1.8)+(C.1.3),(A.2)+(B.1.8)+(C.1.3),(A.3)+(B.1.8)+(C.1.3),(A.4)+(B.1.8)+(C.1.3),(A.1)+(B.1.9)+(C.1.3),(A.2)+(B.1.9)+(C.1.3),(A.3)+(B.1.9)+(C.1.3),(A.4)+(B.1.9)+(C.1.3),(A.1)+(B.1.10)+(C.1.3),(A.2)+(B.1.10)+(C.1.3),(A.3)+(B.1.10)+(C.1.3),(A.4)+(B.1.10)+(C.1.3),(A.1)+(B.1.11)+(C.1.3),(A.2)+(B.1.11)+(C.1.3),(A.3)+(B.1.11)+(C.1.3),(A.4)+(B.1.11)+(C.1.3),(A.1)+(B.1.12)+(C.1.3),(A.2)+(B.1.12)+(C.1.3),(A.3)+(B.1.12)+(C.1.3),(A.4)+(B.1.12)+(C.1.3),(A.1)+(B.1.13)+(C.1.3),(A.2)+(B.1.13)+(C.1.3),(A.3)+(B.1.13)+(C.1.3),(A.4)+(B.1.13)+(C.1.3),(A.1)+(B.1.14)+(C.1.3),(A.2)+(B.1.14)+(C.1.3),(A.3)+(B.1.14)+(C.1.3),(A.4)+(B.1.14)+(C.1.3),(A.1)+(B.1.15)+(C.1.3),(A.2)+(B.1.15)+(C.1.3),(A.3)+(B.1.15)+(C.1.3),(A.4)+(B.1.15)+(C.1.3),(A.1)+(B.1.16)+(C.1.3),(A.2)+(B.1.16)+(C.1.3),(A.3)+(B.1.16)+(C.1.3),(A.4)+(B.1.16)+(C.1.3),(A.1)+(B.1.17)+(C.1.3),(A.2)+(B.1.17)+(C.1.3),(A.3)+(B.1.17)+(C.1.3),(A.4)+(B.1.17)+(C.1.3),
(A.1)+(B.2.1)+(C.1.3),(A.2)+(B.2.1)+(C.1.3),(A.3)+(B.2.1)+(C.1.3),(A.4)+(B.2.1)+(C.1.3),(A.1)+(B.2.2)+(C.1.3),(A.2)+(B.2.2)+(C.1.3),(A.3)+(B.2.2)+(C.1.3),(A.4)+(B.2.2)+(C.1.3),(A.1)+(B.2.3)+(C.1.3),(A.2)+(B.2.3)+(C.1.3),(A.3)+(B.2.3)+(C.1.3),(A.4)+(B.2.3)+(C.1.3),(A.1)+(B.2.4)+(C.1.3),(A.2)+(B.2.4)+(C.1.3),(A.3)+(B.2.4)+(C.1.3),(A.4)+(B.2.4)+(C.1.3),(A.1)+(B.2.5)+(C.1.3),(A.2)+(B.2.5)+(C.1.3),(A.3)+(B.2.5)+(C.1.3),(A.4)+(B.2.5)+(C.1.3),(A.1)+(B.2.6)+(C.1.3),(A.2)+(B.2.6)+(C.1.3),(A.3)+(B.2.6)+(C.1.3),(A.4)+(B.2.6)+(C.1.3),(A.1)+(B.2.7)+(C.1.3),(A.2)+(B.2.7)+(C.1.3),(A.3)+(B.2.7)+(C.1.3),(A.4)+(B.2.7)+(C.1.3),(A.1)+(B.2.8)+(C.1.3),(A.2)+(B.2.8)+(C.1.3),(A.3)+(B.2.8)+(C.1.3),(A.4)+(B.2.8)+(C.1.3)。
(A.1)+(B.1.1)+(C.2.1),(A.2)+(B.1.1)+(C.2.1),(A.3)+(B.1.1)+(C.2.1),(A.4)+(B.1.1)+(C.2.1),(A.1)+(B.1.2)+(C.2.1),(A.2)+(B.1.2)+(C.2.1),(A.3)+(B.1.2)+(C.2.1),(A.4)+(B.1.2)+(C.2.1),(A.1)+(B.1.3)+(C.2.1),(A.2)+(B.1.3)+(C.2.1),(A.3)+(B.1.3)+(C.2.1),(A.4)+(B.1.3)+(C.2.1),(A.1)+(B.1.4)+(C.2.1),(A.2)+(B.1.4)+(C.2.1),(A.3)+(B.1.4)+(C.2.1),(A.4)+(B.1.4)+(C.2.1),(A.1)+(B.1.5)+(C.2.1),(A.2)+(B.1.5)+(C.2.1),(A.3)+(B.1.5)+(C.2.1),(A.4)+(B.1.5)+(C.2.1),(A.1)+(B.1.6)+(C.2.1),(A.2)+(B.1.6)+(C.2.1),(A.3)+(B.1.6)+(C.2.1),(A.4)+(B.1.6)+(C.2.1),(A.1)+(B.1.7)+(C.2.1),(A.2)+(B.1.7)+(C.2.1),(A.3)+(B.1.7)+(C.2.1),(A.4)+(B.1.7)+(C.2.1),(A.1)+(B.1.8)+(C.2.1),(A.2)+(B.1.8)+(C.2.1),(A.3)+(B.1.8)+(C.2.1),(A.4)+(B.1.8)+(C.2.1),(A.1)+(B.1.9)+(C.2.1),(A.2)+(B.1.9)+(C.2.1),(A.3)+(B.1.9)+(C.2.1),(A.4)+(B.1.9)+(C.2.1),(A.1)+(B.1.10)+(C.2.1),(A.2)+(B.1.10)+(C.2.1),(A.3)+(B.1.10)+(C.2.1),(A.4)+(B.1.10)+(C.2.1),(A.1)+(B.1.11)+(C.2.1),(A.2)+(B.1.11)+(C.2.1),(A.3)+(B.1.11)+(C.2.1),(A.4)+(B.1.11)+(C.2.1),(A.1)+(B.1.12)+(C.2.1),(A.2)+(B.1.12)+(C.2.1),(A.3)+(B.1.12)+(C.2.1),(A.4)+(B.1.12)+(C.2.1),(A.1)+(B.1.13)+(C.2.1),(A.2)+(B.1.13)+(C.2.1),(A.3)+(B.1.13)+(C.2.1),(A.4)+(B.1.13)+(C.2.1),(A.1)+(B.1.14)+(C.2.1),(A.2)+(B.1.14)+(C.2.1),(A.3)+(B.1.14)+(C.2.1),(A.4)+(B.1.14)+(C.2.1),(A.1)+(B.1.15)+(C.2.1),(A.2)+(B.1.15)+(C.2.1),(A.3)+(B.1.15)+(C.2.1),(A.4)+(B.1.15)+(C.2.1),(A.1)+(B.1.16)+(C.2.1),(A.2)+(B.1.16)+(C.2.1),(A.3)+(B.1.16)+(C.2.1),(A.4)+(B.1.16)+(C.2.1),(A.1)+(B.1.17)+(C.2.1),(A.2)+(B.1.17)+(C.2.1),(A.3)+(B.1.17)+(C.2.1),(A.4)+(B.1.17)+(C.2.1),
(A.1)+(B.2.1)+(C.2.1),(A.2)+(B.2.1)+(C.2.1),(A.3)+(B.2.1)+(C.2.1),(A.4)+(B.2.1)+(C.2.1),(A.1)+(B.2.2)+(C.2.1),(A.2)+(B.2.2)+(C.2.1),(A.3)+(B.2.2)+(C.2.1),(A.4)+(B.2.2)+(C.2.1),(A.1)+(B.2.3)+(C.2.1),(A.2)+(B.2.3)+(C.2.1),(A.3)+(B.2.3)+(C.2.1),(A.4)+(B.2.3)+(C.2.1),(A.1)+(B.2.4)+(C.2.1),(A.2)+(B.2.4)+(C.2.1),(A.3)+(B.2.4)+(C.2.1),(A.4)+(B.2.4)+(C.2.1),(A.1)+(B.2.5)+(C.2.1),(A.2)+(B.2.5)+(C.2.1),(A.3)+(B.2.5)+(C.2.1),(A.4)+(B.2.5)+(C.2.1),(A.1)+(B.2.6)+(C.2.1),(A.2)+(B.2.6)+(C.2.1),(A.3)+(B.2.6)+(C.2.1),(A.4)+(B.2.6)+(C.2.1),(A.1)+(B.2.7)+(C.2.1),(A.2)+(B.2.7)+(C.2.1),(A.3)+(B.2.7)+(C.2.1),(A.4)+(B.2.7)+(C.2.1),(A.1)+(B.2.8)+(C.2.1),(A.2)+(B.2.8)+(C.2.1),(A.3)+(B.2.8)+(C.2.1),(A.4)+(B.2.8)+(C.2.1)。
(A.1)+(B.1.1)+(C.2.2),(A.2)+(B.1.1)+(C.2.2),(A.3)+(B.1.1)+(C.2.2),(A.4)+(B.1.1)+(C.2.2),(A.1)+(B.1.2)+(C.2.2),(A.2)+(B.1.2)+(C.2.2),(A.3)+(B.1.2)+(C.2.2),(A.4)+(B.1.2)+(C.2.2),(A.1)+(B.1.3)+(C.2.2),(A.2)+(B.1.3)+(C.2.2),(A.3)+(B.1.3)+(C.2.2),(A.4)+(B.1.3)+(C.2.2),(A.1)+(B.1.4)+(C.2.2),(A.2)+(B.1.4)+(C.2.2),(A.3)+(B.1.4)+(C.2.2),(A.4)+(B.1.4)+(C.2.2),(A.1)+(B.1.5)+(C.2.2),(A.2)+(B.1.5)+(C.2.2),(A.3)+(B.1.5)+(C.2.2),(A.4)+(B.1.5)+(C.2.2),(A.1)+(B.1.6)+(C.2.2),(A.2)+(B.1.6)+(C.2.2),(A.3)+(B.1.6)+(C.2.2),(A.4)+(B.1.6)+(C.2.2),(A.1)+(B.1.7)+(C.2.2),(A.2)+(B.1.7)+(C.2.2),(A.3)+(B.1.7)+(C.2.2),(A.4)+(B.1.7)+(C.2.2),(A.1)+(B.1.8)+(C.2.2),(A.2)+(B.1.8)+(C.2.2),(A.3)+(B.1.8)+(C.2.2),(A.4)+(B.1.8)+(C.2.2),(A.1)+(B.1.9)+(C.2.2),(A.2)+(B.1.9)+(C.2.2),(A.3)+(B.1.9)+(C.2.2),(A.4)+(B.1.9)+(C.2.2),(A.1)+(B.1.10)+(C.2.2),(A.2)+(B.1.10)+(C.2.2),(A.3)+(B.1.10)+(C.2.2),(A.4)+(B.1.10)+(C.2.2),(A.1)+(B.1.11)+(C.2.2),(A.2)+(B.1.11)+(C.2.2),(A.3)+(B.1.11)+(C.2.2),(A.4)+(B.1.11)+(C.2.2),(A.1)+(B.1.12)+(C.2.2),(A.2)+(B.1.12)+(C.2.2),(A.3)+(B.1.12)+(C.2.2),(A.4)+(B.1.12)+(C.2.2),(A.1)+(B.1.13)+(C.2.2),(A.2)+(B.1.13)+(C.2.2),(A.3)+(B.1.13)+(C.2.2),(A.4)+(B.1.13)+(C.2.2),(A.1)+(B.1.14)+(C.2.2),(A.2)+(B.1.14)+(C.2.2),(A.3)+(B.1.14)+(C.2.2),(A.4)+(B.1.14)+(C.2.2),(A.1)+(B.1.15)+(C.2.2),(A.2)+(B.1.15)+(C.2.2),(A.3)+(B.1.15)+(C.2.2),(A.4)+(B.1.15)+(C.2.2),(A.1)+(B.1.16)+(C.2.2),(A.2)+(B.1.16)+(C.2.2),(A.3)+(B.1.16)+(C.2.2),(A.4)+(B.1.16)+(C.2.2),(A.1)+(B.1.17)+(C.2.2),(A.2)+(B.1.17)+(C.2.2),(A.3)+(B.1.17)+(C.2.2),(A.4)+(B.1.17)+(C.2.2),
(A.1)+(B.2.1)+(C.2.2),(A.2)+(B.2.1)+(C.2.2),(A.3)+(B.2.1)+(C.2.2),(A.4)+(B.2.1)+(C.2.2),(A.1)+(B.2.2)+(C.2.2),(A.2)+(B.2.2)+(C.2.2),(A.3)+(B.2.2)+(C.2.2),(A.4)+(B.2.2)+(C.2.2),(A.1)+(B.2.3)+(C.2.2),(A.2)+(B.2.3)+(C.2.2),(A.3)+(B.2.3)+(C.2.2),(A.4)+(B.2.3)+(C.2.2),(A.1)+(B.2.4)+(C.2.2),(A.2)+(B.2.4)+(C.2.2),(A.3)+(B.2.4)+(C.2.2),(A.4)+(B.2.4)+(C.2.2),(A.1)+(B.2.5)+(C.2.2),(A.2)+(B.2.5)+(C.2.2),(A.3)+(B.2.5)+(C.2.2),(A.4)+(B.2.5)+(C.2.2),(A.1)+(B.2.6)+(C.2.2),(A.2)+(B.2.6)+(C.2.2),(A.3)+(B.2.6)+(C.2.2),(A.4)+(B.2.6)+(C.2.2),(A.1)+(B.2.7)+(C.2.2),(A.2)+(B.2.7)+(C.2.2),(A.3)+(B.2.7)+(C.2.2),(A.4)+(B.2.7)+(C.2.2),(A.1)+(B.2.8)+(C.2.2),(A.2)+(B.2.8)+(C.2.2),(A.3)+(B.2.8)+(C.2.2),(A.4)+(B.2.8)+(C.2.2)。
(A.1)+(B.1.1)+(C.2.3),(A.2)+(B.1.1)+(C.2.3),(A.3)+(B.1.1)+(C.2.3),(A.4)+(B.1.1)+(C.2.3),(A.1)+(B.1.2)+(C.2.3),(A.2)+(B.1.2)+(C.2.3),(A.3)+(B.1.2)+(C.2.3),(A.4)+(B.1.2)+(C.2.3),(A.1)+(B.1.3)+(C.2.3),(A.2)+(B.1.3)+(C.2.3),(A.3)+(B.1.3)+(C.2.3),(A.4)+(B.1.3)+(C.2.3),(A.1)+(B.1.4)+(C.2.3),(A.2)+(B.1.4)+(C.2.3),(A.3)+(B.1.4)+(C.2.3),(A.4)+(B.1.4)+(C.2.3),(A.1)+(B.1.5)+(C.2.3),(A.2)+(B.1.5)+(C.2.3),(A.3)+(B.1.5)+(C.2.3),(A.4)+(B.1.5)+(C.2.3),(A.1)+(B.1.6)+(C.2.3),(A.2)+(B.1.6)+(C.2.3),(A.3)+(B.1.6)+(C.2.3),(A.4)+(B.1.6)+(C.2.3),(A.1)+(B.1.7)+(C.2.3),(A.2)+(B.1.7)+(C.2.3),(A.3)+(B.1.7)+(C.2.3),(A.4)+(B.1.7)+(C.2.3),(A.1)+(B.1.8)+(C.2.3),(A.2)+(B.1.8)+(C.2.3),(A.3)+(B.1.8)+(C.2.3),(A.4)+(B.1.8)+(C.2.3),(A.1)+(B.1.9)+(C.2.3),(A.2)+(B.1.9)+(C.2.3),(A.3)+(B.1.9)+(C.2.3),(A.4)+(B.1.9)+(C.2.3),(A.1)+(B.1.10)+(C.2.3),(A.2)+(B.1.10)+(C.2.3),(A.3)+(B.1.10)+(C.2.3),(A.4)+(B.1.10)+(C.2.3),(A.1)+(B.1.11)+(C.2.3),(A.2)+(B.1.11)+(C.2.3),(A.3)+(B.1.11)+(C.2.3),(A.4)+(B.1.11)+(C.2.3),(A.1)+(B.1.12)+(C.2.3),(A.2)+(B.1.12)+(C.2.3),(A.3)+(B.1.12)+(C.2.3),(A.4)+(B.1.12)+(C.2.3),(A.1)+(B.1.13)+(C.2.3),(A.2)+(B.1.13)+(C.2.3),(A.3)+(B.1.13)+(C.2.3),(A.4)+(B.1.13)+(C.2.3),(A.1)+(B.1.14)+(C.2.3),(A.2)+(B.1.14)+(C.2.3),(A.3)+(B.1.14)+(C.2.3),(A.4)+(B.1.14)+(C.2.3),(A.1)+(B.1.15)+(C.2.3),(A.2)+(B.1.15)+(C.2.3),(A.3)+(B.1.15)+(C.2.3),(A.4)+(B.1.15)+(C.2.3),(A.1)+(B.1.16)+(C.2.3),(A.2)+(B.1.16)+(C.2.3),(A.3)+(B.1.16)+(C.2.3),(A.4)+(B.1.16)+(C.2.3),(A.1)+(B.1.17)+(C.2.3),(A.2)+(B.1.17)+(C.2.3),(A.3)+(B.1.17)+(C.2.3),(A.4)+(B.1.17)+(C.2.3),
(A.1)+(B.2.1)+(C.2.3),(A.2)+(B.2.1)+(C.2.3),(A.3)+(B.2.1)+(C.2.3),(A.4)+(B.2.1)+(C.2.3),(A.1)+(B.2.2)+(C.2.3),(A.2)+(B.2.2)+(C.2.3),(A.3)+(B.2.2)+(C.2.3),(A.4)+(B.2.2)+(C.2.3),(A.1)+(B.2.3)+(C.2.3),(A.2)+(B.2.3)+(C.2.3),(A.3)+(B.2.3)+(C.2.3),(A.4)+(B.2.3)+(C.2.3),(A.1)+(B.2.4)+(C.2.3),(A.2)+(B.2.4)+(C.2.3),(A.3)+(B.2.4)+(C.2.3),(A.4)+(B.2.4)+(C.2.3),(A.1)+(B.2.5)+(C.2.3),(A.2)+(B.2.5)+(C.2.3),(A.3)+(B.2.5)+(C.2.3),(A.4)+(B.2.5)+(C.2.3),(A.1)+(B.2.6)+(C.2.3),(A.2)+(B.2.6)+(C.2.3),(A.3)+(B.2.6)+(C.2.3),(A.4)+(B.2.6)+(C.2.3),(A.1)+(B.2.7)+(C.2.3),(A.2)+(B.2.7)+(C.2.3),(A.3)+(B.2.7)+(C.2.3),(A.4)+(B.2.7)+(C.2.3),(A.1)+(B.2.8)+(C.2.3),(A.2)+(B.2.8)+(C.2.3),(A.3)+(B.2.8)+(C.2.3),(A.4)+(B.2.8)+(C.2.3)。
(A.1)+(B.1.1)+(C.3.1),(A.2)+(B.1.1)+(C.3.1),(A.3)+(B.1.1)+(C.3.1),(A.4)+(B.1.1)+(C.3.1),(A.1)+(B.1.2)+(C.3.1),(A.2)+(B.1.2)+(C.3.1),(A.3)+(B.1.2)+(C.3.1),(A.4)+(B.1.2)+(C.3.1),(A.1)+(B.1.3)+(C.3.1),(A.2)+(B.1.3)+(C.3.1),(A.3)+(B.1.3)+(C.3.1),(A.4)+(B.1.3)+(C.3.1),(A.1)+(B.1.4)+(C.3.1),(A.2)+(B.1.4)+(C.3.1),(A.3)+(B.1.4)+(C.3.1),(A.4)+(B.1.4)+(C.3.1),(A.1)+(B.1.5)+(C.3.1),(A.2)+(B.1.5)+(C.3.1),(A.3)+(B.1.5)+(C.3.1),(A.4)+(B.1.5)+(C.3.1),(A.1)+(B.1.6)+(C.3.1),(A.2)+(B.1.6)+(C.3.1),(A.3)+(B.1.6)+(C.3.1),(A.4)+(B.1.6)+(C.3.1),(A.1)+(B.1.7)+(C.3.1),(A.2)+(B.1.7)+(C.3.1),(A.3)+(B.1.7)+(C.3.1),(A.4)+(B.1.7)+(C.3.1),(A.1)+(B.1.8)+(C.3.1),(A.2)+(B.1.8)+(C.3.1),(A.3)+(B.1.8)+(C.3.1),(A.4)+(B.1.8)+(C.3.1),(A.1)+(B.1.9)+(C.3.1),(A.2)+(B.1.9)+(C.3.1),(A.3)+(B.1.9)+(C.3.1),(A.4)+(B.1.9)+(C.3.1),(A.1)+(B.1.10)+(C.3.1),(A.2)+(B.1.10)+(C.3.1),(A.3)+(B.1.10)+(C.3.1),(A.4)+(B.1.10)+(C.3.1),(A.1)+(B.1.11)+(C.3.1),(A.2)+(B.1.11)+(C.3.1),(A.3)+(B.1.11)+(C.3.1),(A.4)+(B.1.11)+(C.3.1),(A.1)+(B.1.12)+(C.3.1),(A.2)+(B.1.12)+(C.3.1),(A.3)+(B.1.12)+(C.3.1),(A.4)+(B.1.12)+(C.3.1),(A.1)+(B.1.13)+(C.3.1),(A.2)+(B.1.13)+(C.3.1),(A.3)+(B.1.13)+(C.3.1),(A.4)+(B.1.13)+(C.3.1),(A.1)+(B.1.14)+(C.3.1),(A.2)+(B.1.14)+(C.3.1),(A.3)+(B.1.14)+(C.3.1),(A.4)+(B.1.14)+(C.3.1),(A.1)+(B.1.15)+(C.3.1),(A.2)+(B.1.15)+(C.3.1),(A.3)+(B.1.15)+(C.3.1),(A.4)+(B.1.15)+(C.3.1),(A.1)+(B.1.16)+(C.3.1),(A.2)+(B.1.16)+(C.3.1),(A.3)+(B.1.16)+(C.3.1),(A.4)+(B.1.16)+(C.3.1),(A.1)+(B.1.17)+(C.3.1),(A.2)+(B.1.17)+(C.3.1),(A.3)+(B.1.17)+(C.3.1),(A.4)+(B.1.17)+(C.3.1),
(A.1)+(B.2.1)+(C.3.1),(A.2)+(B.2.1)+(C.3.1),(A.3)+(B.2.1)+(C.3.1),(A.4)+(B.2.1)+(C.3.1),(A.1)+(B.2.2)+(C.3.1),(A.2)+(B.2.2)+(C.3.1),(A.3)+(B.2.2)+(C.3.1),(A.4)+(B.2.2)+(C.3.1),(A.1)+(B.2.3)+(C.3.1),(A.2)+(B.2.3)+(C.3.1),(A.3)+(B.2.3)+(C.3.1),(A.4)+(B.2.3)+(C.3.1),(A.1)+(B.2.4)+(C.3.1),(A.2)+(B.2.4)+(C.3.1),(A.3)+(B.2.4)+(C.3.1),(A.4)+(B.2.4)+(C.3.1),(A.1)+(B.2.5)+(C.3.1),(A.2)+(B.2.5)+(C.3.1),(A.3)+(B.2.5)+(C.3.1),(A.4)+(B.2.5)+(C.3.1),(A.1)+(B.2.6)+(C.3.1),(A.2)+(B.2.6)+(C.3.1),(A.3)+(B.2.6)+(C.3.1),(A.4)+(B.2.6)+(C.3.1),(A.1)+(B.2.7)+(C.3.1),(A.2)+(B.2.7)+(C.3.1),(A.3)+(B.2.7)+(C.3.1),(A.4)+(B.2.7)+(C.3.1),(A.1)+(B.2.8)+(C.3.1),(A.2)+(B.2.8)+(C.3.1),(A.3)+(B.2.8)+(C.3.1),(A.4)+(B.2.8)+(C.3.1)。
(A.1)+(B.1.1)+(C.3.2),(A.2)+(B.1.1)+(C.3.2),(A.3)+(B.1.1)+(C.3.2),(A.4)+(B.1.1)+(C.3.2),(A.1)+(B.1.2)+(C.3.2),(A.2)+(B.1.2)+(C.3.2),(A.3)+(B.1.2)+(C.3.2),(A.4)+(B.1.2)+(C.3.2),(A.1)+(B.1.3)+(C.3.2),(A.2)+(B.1.3)+(C.3.2),(A.3)+(B.1.3)+(C.3.2),(A.4)+(B.1.3)+(C.3.2),(A.1)+(B.1.4)+(C.3.2),(A.2)+(B.1.4)+(C.3.2),(A.3)+(B.1.4)+(C.3.2),(A.4)+(B.1.4)+(C.3.2),(A.1)+(B.1.5)+(C.3.2),(A.2)+(B.1.5)+(C.3.2),(A.3)+(B.1.5)+(C.3.2),(A.4)+(B.1.5)+(C.3.2),(A.1)+(B.1.6)+(C.3.2),(A.2)+(B.1.6)+(C.3.2),(A.3)+(B.1.6)+(C.3.2),(A.4)+(B.1.6)+(C.3.2),(A.1)+(B.1.7)+(C.3.2),(A.2)+(B.1.7)+(C.3.2),(A.3)+(B.1.7)+(C.3.2),(A.4)+(B.1.7)+(C.3.2),(A.1)+(B.1.8)+(C.3.2),(A.2)+(B.1.8)+(C.3.2),(A.3)+(B.1.8)+(C.3.2),(A.4)+(B.1.8)+(C.3.2),(A.1)+(B.1.9)+(C.3.2),(A.2)+(B.1.9)+(C.3.2),(A.3)+(B.1.9)+(C.3.2),(A.4)+(B.1.9)+(C.3.2),(A.1)+(B.1.10)+(C.3.2),(A.2)+(B.1.10)+(C.3.2),(A.3)+(B.1.10)+(C.3.2),(A.4)+(B.1.10)+(C.3.2),(A.1)+(B.1.11)+(C.3.2),(A.2)+(B.1.11)+(C.3.2),(A.3)+(B.1.11)+(C.3.2),(A.4)+(B.1.11)+(C.3.2),(A.1)+(B.1.12)+(C.3.2),(A.2)+(B.1.12)+(C.3.2),(A.3)+(B.1.12)+(C.3.2),(A.4)+(B.1.12)+(C.3.2),(A.1)+(B.1.13)+(C.3.2),(A.2)+(B.1.13)+(C.3.2),(A.3)+(B.1.13)+(C.3.2),(A.4)+(B.1.13)+(C.3.2),(A.1)+(B.1.14)+(C.3.2),(A.2)+(B.1.14)+(C.3.2),(A.3)+(B.1.14)+(C.3.2),(A.4)+(B.1.14)+(C.3.2),(A.1)+(B.1.15)+(C.3.2),(A.2)+(B.1.15)+(C.3.2),(A.3)+(B.1.15)+(C.3.2),(A.4)+(B.1.15)+(C.3.2),(A.1)+(B.1.16)+(C.3.2),(A.2)+(B.1.16)+(C.3.2),(A.3)+(B.1.16)+(C.3.2),(A.4)+(B.1.16)+(C.3.2),(A.1)+(B.1.17)+(C.3.2),(A.2)+(B.1.17)+(C.3.2),(A.3)+(B.1.17)+(C.3.2),(A.4)+(B.1.17)+(C.3.2),
(A.1)+(B.2.1)+(C.3.2),(A.2)+(B.2.1)+(C.3.2),(A.3)+(B.2.1)+(C.3.2),(A.4)+(B.2.1)+(C.3.2),(A.1)+(B.2.2)+(C.3.2),(A.2)+(B.2.2)+(C.3.2),(A.3)+(B.2.2)+(C.3.2),(A.4)+(B.2.2)+(C.3.2),(A.1)+(B.2.3)+(C.3.2),(A.2)+(B.2.3)+(C.3.2),(A.3)+(B.2.3)+(C.3.2),(A.4)+(B.2.3)+(C.3.2),(A.1)+(B.2.4)+(C.3.2),(A.2)+(B.2.4)+(C.3.2),(A.3)+(B.2.4)+(C.3.2),(A.4)+(B.2.4)+(C.3.2),(A.1)+(B.2.5)+(C.3.2),(A.2)+(B.2.5)+(C.3.2),(A.3)+(B.2.5)+(C.3.2),(A.4)+(B.2.5)+(C.3.2),(A.1)+(B.2.6)+(C.3.2),(A.2)+(B.2.6)+(C.3.2),(A.3)+(B.2.6)+(C.3.2),(A.4)+(B.2.6)+(C.3.2),(A.1)+(B.2.7)+(C.3.2),(A.2)+(B.2.7)+(C.3.2),(A.3)+(B.2.7)+(C.3.2),(A.4)+(B.2.7)+(C.3.2),(A.1)+(B.2.8)+(C.3.2),(A.2)+(B.2.8)+(C.3.2),(A.3)+(B.2.8)+(C.3.2),(A.4)+(B.2.8)+(C.3.2)。
(A.1)+(B.1.1)+(C.3.3),(A.2)+(B.1.1)+(C.3.3),(A.3)+(B.1.1)+(C.3.3),(A.4)+(B.1.1)+(C.3.3),(A.1)+(B.1.2)+(C.3.3),(A.2)+(B.1.2)+(C.3.3),(A.3)+(B.1.2)+(C.3.3),(A.4)+(B.1.2)+(C.3.3),(A.1)+(B.1.3)+(C.3.3),(A.2)+(B.1.3)+(C.3.3),(A.3)+(B.1.3)+(C.3.3),(A.4)+(B.1.3)+(C.3.3),(A.1)+(B.1.4)+(C.3.3),(A.2)+(B.1.4)+(C.3.3),(A.3)+(B.1.4)+(C.3.3),(A.4)+(B.1.4)+(C.3.3),(A.1)+(B.1.5)+(C.3.3),(A.2)+(B.1.5)+(C.3.3),(A.3)+(B.1.5)+(C.3.3),(A.4)+(B.1.5)+(C.3.3),(A.1)+(B.1.6)+(C.3.3),(A.2)+(B.1.6)+(C.3.3),(A.3)+(B.1.6)+(C.3.3),(A.4)+(B.1.6)+(C.3.3),(A.1)+(B.1.7)+(C.3.3),(A.2)+(B.1.7)+(C.3.3),(A.3)+(B.1.7)+(C.3.3),(A.4)+(B.1.7)+(C.3.3),(A.1)+(B.1.8)+(C.3.3),(A.2)+(B.1.8)+(C.3.3),(A.3)+(B.1.8)+(C.3.3),(A.4)+(B.1.8)+(C.3.3),(A.1)+(B.1.9)+(C.3.3),(A.2)+(B.1.9)+(C.3.3),(A.3)+(B.1.9)+(C.3.3),(A.4)+(B.1.9)+(C.3.3),(A.1)+(B.1.10)+(C.3.3),(A.2)+(B.1.10)+(C.3.3),(A.3)+(B.1.10)+(C.3.3),(A.4)+(B.1.10)+(C.3.3),(A.1)+(B.1.11)+(C.3.3),(A.2)+(B.1.11)+(C.3.3),(A.3)+(B.1.11)+(C.3.3),(A.4)+(B.1.11)+(C.3.3),(A.1)+(B.1.12)+(C.3.3),(A.2)+(B.1.12)+(C.3.3),(A.3)+(B.1.12)+(C.3.3),(A.4)+(B.1.12)+(C.3.3),(A.1)+(B.1.13)+(C.3.3),(A.2)+(B.1.13)+(C.3.3),(A.3)+(B.1.13)+(C.3.3),(A.4)+(B.1.13)+(C.3.3),(A.1)+(B.1.14)+(C.3.3),(A.2)+(B.1.14)+(C.3.3),(A.3)+(B.1.14)+(C.3.3),(A.4)+(B.1.14)+(C.3.3),(A.1)+(B.1.15)+(C.3.3),(A.2)+(B.1.15)+(C.3.3),(A.3)+(B.1.15)+(C.3.3),(A.4)+(B.1.15)+(C.3.3),(A.1)+(B.1.16)+(C.3.3),(A.2)+(B.1.16)+(C.3.3),(A.3)+(B.1.16)+(C.3.3),(A.4)+(B.1.16)+(C.3.3),(A.1)+(B.1.17)+(C.3.3),(A.2)+(B.1.17)+(C.3.3),(A.3)+(B.1.17)+(C.3.3),(A.4)+(B.1.17)+(C.3.3),
(A.1)+(B.2.1)+(C.3.3),(A.2)+(B.2.1)+(C.3.3),(A.3)+(B.2.1)+(C.3.3),(A.4)+(B.2.1)+(C.3.3),(A.1)+(B.2.2)+(C.3.3),(A.2)+(B.2.2)+(C.3.3),(A.3)+(B.2.2)+(C.3.3),(A.4)+(B.2.2)+(C.3.3),(A.1)+(B.2.3)+(C.3.3),(A.2)+(B.2.3)+(C.3.3),(A.3)+(B.2.3)+(C.3.3),(A.4)+(B.2.3)+(C.3.3),(A.1)+(B.2.4)+(C.3.3),(A.2)+(B.2.4)+(C.3.3),(A.3)+(B.2.4)+(C.3.3),(A.4)+(B.2.4)+(C.3.3),(A.1)+(B.2.5)+(C.3.3),(A.2)+(B.2.5)+(C.3.3),(A.3)+(B.2.5)+(C.3.3),(A.4)+(B.2.5)+(C.3.3),(A.1)+(B.2.6)+(C.3.3),(A.2)+(B.2.6)+(C.3.3),(A.3)+(B.2.6)+(C.3.3),(A.4)+(B.2.6)+(C.3.3),(A.1)+(B.2.7)+(C.3.3),(A.2)+(B.2.7)+(C.3.3),(A.3)+(B.2.7)+(C.3.3),(A.4)+(B.2.7)+(C.3.3),(A.1)+(B.2.8)+(C.3.3),(A.2)+(B.2.8)+(C.3.3),(A.3)+(B.2.8)+(C.3.3),(A.4)+(B.2.8)+(C.3.3)。
(A.1)+(B.1.1)+(C.3.4),(A.2)+(B.1.1)+(C.3.4),(A.3)+(B.1.1)+(C.3.4),(A.4)+(B.1.1)+(C.3.4),(A.1)+(B.1.2)+(C.3.4),(A.2)+(B.1.2)+(C.3.4),(A.3)+(B.1.2)+(C.3.4),(A.4)+(B.1.2)+(C.3.4),(A.1)+(B.1.3)+(C.3.4),(A.2)+(B.1.3)+(C.3.4),(A.3)+(B.1.3)+(C.3.4),(A.4)+(B.1.3)+(C.3.4),(A.1)+(B.1.4)+(C.3.4),(A.2)+(B.1.4)+(C.3.4),(A.3)+(B.1.4)+(C.3.4),(A.4)+(B.1.4)+(C.3.4),(A.1)+(B.1.5)+(C.3.4),(A.2)+(B.1.5)+(C.3.4),(A.3)+(B.1.5)+(C.3.4),(A.4)+(B.1.5)+(C.3.4),(A.1)+(B.1.6)+(C.3.4),(A.2)+(B.1.6)+(C.3.4),(A.3)+(B.1.6)+(C.3.4),(A.4)+(B.1.6)+(C.3.4),(A.1)+(B.1.7)+(C.3.4),(A.2)+(B.1.7)+(C.3.4),(A.3)+(B.1.7)+(C.3.4),(A.4)+(B.1.7)+(C.3.4),(A.1)+(B.1.8)+(C.3.4),(A.2)+(B.1.8)+(C.3.4),(A.3)+(B.1.8)+(C.3.4),(A.4)+(B.1.8)+(C.3.4),(A.1)+(B.1.9)+(C.3.4),(A.2)+(B.1.9)+(C.3.4),(A.3)+(B.1.9)+(C.3.4),(A.4)+(B.1.9)+(C.3.4),(A.1)+(B.1.10)+(C.3.4),(A.2)+(B.1.10)+(C.3.4),(A.3)+(B.1.10)+(C.3.4),(A.4)+(B.1.10)+(C.3.4),(A.1)+(B.1.11)+(C.3.4),(A.2)+(B.1.11)+(C.3.4),(A.3)+(B.1.11)+(C.3.4),(A.4)+(B.1.11)+(C.3.4),(A.1)+(B.1.12)+(C.3.4),(A.2)+(B.1.12)+(C.3.4),(A.3)+(B.1.12)+(C.3.4),(A.4)+(B.1.12)+(C.3.4),(A.1)+(B.1.13)+(C.3.4),(A.2)+(B.1.13)+(C.3.4),(A.3)+(B.1.13)+(C.3.4),(A.4)+(B.1.13)+(C.3.4),(A.1)+(B.1.14)+(C.3.4),(A.2)+(B.1.14)+(C.3.4),(A.3)+(B.1.14)+(C.3.4),(A.4)+(B.1.14)+(C.3.4),(A.1)+(B.1.15)+(C.3.4),(A.2)+(B.1.15)+(C.3.4),(A.3)+(B.1.15)+(C.3.4),(A.4)+(B.1.15)+(C.3.4),(A.1)+(B.1.16)+(C.3.4),(A.2)+(B.1.16)+(C.3.4),(A.3)+(B.1.16)+(C.3.4),(A.4)+(B.1.16)+(C.3.4),(A.1)+(B.1.17)+(C.3.4),(A.2)+(B.1.17)+(C.3.4),(A.3)+(B.1.17)+(C.3.4),(A.4)+(B.1.17)+(C.3.4),
(A.1)+(B.2.1)+(C.3.4),(A.2)+(B.2.1)+(C.3.4),(A.3)+(B.2.1)+(C.3.4),(A.4)+(B.2.1)+(C.3.4),(A.1)+(B.2.2)+(C.3.4),(A.2)+(B.2.2)+(C.3.4),(A.3)+(B.2.2)+(C.3.4),(A.4)+(B.2.2)+(C.3.4),(A.1)+(B.2.3)+(C.3.4),(A.2)+(B.2.3)+(C.3.4),(A.3)+(B.2.3)+(C.3.4),(A.4)+(B.2.3)+(C.3.4),(A.1)+(B.2.4)+(C.3.4),(A.2)+(B.2.4)+(C.3.4),(A.3)+(B.2.4)+(C.3.4),(A.4)+(B.2.4)+(C.3.4),(A.1)+(B.2.5)+(C.3.4),(A.2)+(B.2.5)+(C.3.4),(A.3)+(B.2.5)+(C.3.4),(A.4)+(B.2.5)+(C.3.4),(A.1)+(B.2.6)+(C.3.4),(A.2)+(B.2.6)+(C.3.4),(A.3)+(B.2.6)+(C.3.4),(A.4)+(B.2.6)+(C.3.4),(A.1)+(B.2.7)+(C.3.4),(A.2)+(B.2.7)+(C.3.4),(A.3)+(B.2.7)+(C.3.4),(A.4)+(B.2.7)+(C.3.4),(A.1)+(B.2.8)+(C.3.4),(A.2)+(B.2.8)+(C.3.4),(A.3)+(B.2.8)+(C.3.4),(A.4)+(B.2.8)+(C.3.4)。
(A.1)+(B.1.1)+(C.3.5),(A.2)+(B.1.1)+(C.3.5),(A.3)+(B.1.1)+(C.3.5),(A.4)+(B.1.1)+(C.3.5),(A.1)+(B.1.2)+(C.3.5),(A.2)+(B.1.2)+(C.3.5),(A.3)+(B.1.2)+(C.3.5),(A.4)+(B.1.2)+(C.3.5),(A.1)+(B.1.3)+(C.3.5),(A.2)+(B.1.3)+(C.3.5),(A.3)+(B.1.3)+(C.3.5),(A.4)+(B.1.3)+(C.3.5),(A.1)+(B.1.4)+(C.3.5),(A.2)+(B.1.4)+(C.3.5),(A.3)+(B.1.4)+(C.3.5),(A.4)+(B.1.4)+(C.3.5),(A.1)+(B.1.5)+(C.3.5),(A.2)+(B.1.5)+(C.3.5),(A.3)+(B.1.5)+(C.3.5),(A.4)+(B.1.5)+(C.3.5),(A.1)+(B.1.6)+(C.3.5),(A.2)+(B.1.6)+(C.3.5),(A.3)+(B.1.6)+(C.3.5),(A.4)+(B.1.6)+(C.3.5),(A.1)+(B.1.7)+(C.3.5),(A.2)+(B.1.7)+(C.3.5),(A.3)+(B.1.7)+(C.3.5),(A.4)+(B.1.7)+(C.3.5),(A.1)+(B.1.8)+(C.3.5),(A.2)+(B.1.8)+(C.3.5),(A.3)+(B.1.8)+(C.3.5),(A.4)+(B.1.8)+(C.3.5),(A.1)+(B.1.9)+(C.3.5),(A.2)+(B.1.9)+(C.3.5),(A.3)+(B.1.9)+(C.3.5),(A.4)+(B.1.9)+(C.3.5),(A.1)+(B.1.10)+(C.3.5),(A.2)+(B.1.10)+(C.3.5),(A.3)+(B.1.10)+(C.3.5),(A.4)+(B.1.10)+(C.3.5),(A.1)+(B.1.11)+(C.3.5),(A.2)+(B.1.11)+(C.3.5),(A.3)+(B.1.11)+(C.3.5),(A.4)+(B.1.11)+(C.3.5),(A.1)+(B.1.12)+(C.3.5),(A.2)+(B.1.12)+(C.3.5),(A.3)+(B.1.12)+(C.3.5),(A.4)+(B.1.12)+(C.3.5),(A.1)+(B.1.13)+(C.3.5),(A.2)+(B.1.13)+(C.3.5),(A.3)+(B.1.13)+(C.3.5),(A.4)+(B.1.13)+(C.3.5),(A.1)+(B.1.14)+(C.3.5),(A.2)+(B.1.14)+(C.3.5),(A.3)+(B.1.14)+(C.3.5),(A.4)+(B.1.14)+(C.3.5),(A.1)+(B.1.15)+(C.3.5),(A.2)+(B.1.15)+(C.3.5),(A.3)+(B.1.15)+(C.3.5),(A.4)+(B.1.15)+(C.3.5),(A.1)+(B.1.16)+(C.3.5),(A.2)+(B.1.16)+(C.3.5),(A.3)+(B.1.16)+(C.3.5),(A.4)+(B.1.16)+(C.3.5),(A.1)+(B.1.17)+(C.3.5),(A.2)+(B.1.17)+(C.3.5),(A.3)+(B.1.17)+(C.3.5),(A.4)+(B.1.17)+(C.3.5),
(A.1)+(B.2.1)+(C.3.5),(A.2)+(B.2.1)+(C.3.5),(A.3)+(B.2.1)+(C.3.5),(A.4)+(B.2.1)+(C.3.5),(A.1)+(B.2.2)+(C.3.5),(A.2)+(B.2.2)+(C.3.5),(A.3)+(B.2.2)+(C.3.5),(A.4)+(B.2.2)+(C.3.5),(A.1)+(B.2.3)+(C.3.5),(A.2)+(B.2.3)+(C.3.5),(A.3)+(B.2.3)+(C.3.5),(A.4)+(B.2.3)+(C.3.5),(A.1)+(B.2.4)+(C.3.5),(A.2)+(B.2.4)+(C.3.5),(A.3)+(B.2.4)+(C.3.5),(A.4)+(B.2.4)+(C.3.5),(A.1)+(B.2.5)+(C.3.5),(A.2)+(B.2.5)+(C.3.5),(A.3)+(B.2.5)+(C.3.5),(A.4)+(B.2.5)+(C.3.5),(A.1)+(B.2.6)+(C.3.5),(A.2)+(B.2.6)+(C.3.5),(A.3)+(B.2.6)+(C.3.5),(A.4)+(B.2.6)+(C.3.5),(A.1)+(B.2.7)+(C.3.5),(A.2)+(B.2.7)+(C.3.5),(A.3)+(B.2.7)+(C.3.5),(A.4)+(B.2.7)+(C.3.5),(A.1)+(B.2.8)+(C.3.5),(A.2)+(B.2.8)+(C.3.5),(A.3)+(B.2.8)+(C.3.5),(A.4)+(B.2.8)+(C.3.5)。
(A.1)+(B.1.1)+(C.3.6),(A.2)+(B.1.1)+(C.3.6),(A.3)+(B.1.1)+(C.3.6),(A.4)+(B.1.1)+(C.3.6),(A.1)+(B.1.2)+(C.3.6),(A.2)+(B.1.2)+(C.3.6),(A.3)+(B.1.2)+(C.3.6),(A.4)+(B.1.2)+(C.3.6),(A.1)+(B.1.3)+(C.3.6),(A.2)+(B.1.3)+(C.3.6),(A.3)+(B.1.3)+(C.3.6),(A.4)+(B.1.3)+(C.3.6),(A.1)+(B.1.4)+(C.3.6),(A.2)+(B.1.4)+(C.3.6),(A.3)+(B.1.4)+(C.3.6),(A.4)+(B.1.4)+(C.3.6),(A.1)+(B.1.5)+(C.3.6),(A.2)+(B.1.5)+(C.3.6),(A.3)+(B.1.5)+(C.3.6),(A.4)+(B.1.5)+(C.3.6),(A.1)+(B.1.6)+(C.3.6),(A.2)+(B.1.6)+(C.3.6),(A.3)+(B.1.6)+(C.3.6),(A.4)+(B.1.6)+(C.3.6),(A.1)+(B.1.7)+(C.3.6),(A.2)+(B.1.7)+(C.3.6),(A.3)+(B.1.7)+(C.3.6),(A.4)+(B.1.7)+(C.3.6),(A.1)+(B.1.8)+(C.3.6),(A.2)+(B.1.8)+(C.3.6),(A.3)+(B.1.8)+(C.3.6),(A.4)+(B.1.8)+(C.3.6),(A.1)+(B.1.9)+(C.3.6),(A.2)+(B.1.9)+(C.3.6),(A.3)+(B.1.9)+(C.3.6),(A.4)+(B.1.9)+(C.3.6),(A.1)+(B.1.10)+(C.3.6),(A.2)+(B.1.10)+(C.3.6),(A.3)+(B.1.10)+(C.3.6),(A.4)+(B.1.10)+(C.3.6),(A.1)+(B.1.11)+(C.3.6),(A.2)+(B.1.11)+(C.3.6),(A.3)+(B.1.11)+(C.3.6),(A.4)+(B.1.11)+(C.3.6),(A.1)+(B.1.12)+(C.3.6),(A.2)+(B.1.12)+(C.3.6),(A.3)+(B.1.12)+(C.3.6),(A.4)+(B.1.12)+(C.3.6),(A.1)+(B.1.13)+(C.3.6),(A.2)+(B.1.13)+(C.3.6),(A.3)+(B.1.13)+(C.3.6),(A.4)+(B.1.13)+(C.3.6),(A.1)+(B.1.14)+(C.3.6),(A.2)+(B.1.14)+(C.3.6),(A.3)+(B.1.14)+(C.3.6),(A.4)+(B.1.14)+(C.3.6),(A.1)+(B.1.15)+(C.3.6),(A.2)+(B.1.15)+(C.3.6),(A.3)+(B.1.15)+(C.3.6),(A.4)+(B.1.15)+(C.3.6),(A.1)+(B.1.16)+(C.3.6),(A.2)+(B.1.16)+(C.3.6),(A.3)+(B.1.16)+(C.3.6),(A.4)+(B.1.16)+(C.3.6),(A.1)+(B.1.17)+(C.3.6),(A.2)+(B.1.17)+(C.3.6),(A.3)+(B.1.17)+(C.3.6),(A.4)+(B.1.17)+(C.3.6),
(A.1)+(B.2.1)+(C.3.6),(A.2)+(B.2.1)+(C.3.6),(A.3)+(B.2.1)+(C.3.6),(A.4)+(B.2.1)+(C.3.6),(A.1)+(B.2.2)+(C.3.6),(A.2)+(B.2.2)+(C.3.6),(A.3)+(B.2.2)+(C.3.6),(A.4)+(B.2.2)+(C.3.6),(A.1)+(B.2.3)+(C.3.6),(A.2)+(B.2.3)+(C.3.6),(A.3)+(B.2.3)+(C.3.6),(A.4)+(B.2.3)+(C.3.6),(A.1)+(B.2.4)+(C.3.6),(A.2)+(B.2.4)+(C.3.6),(A.3)+(B.2.4)+(C.3.6),(A.4)+(B.2.4)+(C.3.6),(A.1)+(B.2.5)+(C.3.6),(A.2)+(B.2.5)+(C.3.6),(A.3)+(B.2.5)+(C.3.6),(A.4)+(B.2.5)+(C.3.6),(A.1)+(B.2.6)+(C.3.6),(A.2)+(B.2.6)+(C.3.6),(A.3)+(B.2.6)+(C.3.6),(A.4)+(B.2.6)+(C.3.6),(A.1)+(B.2.7)+(C.3.6),(A.2)+(B.2.7)+(C.3.6),(A.3)+(B.2.7)+(C.3.6),(A.4)+(B.2.7)+(C.3.6),(A.1)+(B.2.8)+(C.3.6),(A.2)+(B.2.8)+(C.3.6),(A.3)+(B.2.8)+(C.3.6),(A.4)+(B.2.8)+(C.3.6)。
(A.1)+(B.1.1)+(C.3.7),(A.2)+(B.1.1)+(C.3.7),(A.3)+(B.1.1)+(C.3.7),(A.4)+(B.1.1)+(C.3.7),(A.1)+(B.1.2)+(C.3.7),(A.2)+(B.1.2)+(C.3.7),(A.3)+(B.1.2)+(C.3.7),(A.4)+(B.1.2)+(C.3.7),(A.1)+(B.1.3)+(C.3.7),(A.2)+(B.1.3)+(C.3.7),(A.3)+(B.1.3)+(C.3.7),(A.4)+(B.1.3)+(C.3.7),(A.1)+(B.1.4)+(C.3.7),(A.2)+(B.1.4)+(C.3.7),(A.3)+(B.1.4)+(C.3.7),(A.4)+(B.1.4)+(C.3.7),(A.1)+(B.1.5)+(C.3.7),(A.2)+(B.1.5)+(C.3.7),(A.3)+(B.1.5)+(C.3.7),(A.4)+(B.1.5)+(C.3.7),(A.1)+(B.1.6)+(C.3.7),(A.2)+(B.1.6)+(C.3.7),(A.3)+(B.1.6)+(C.3.7),(A.4)+(B.1.6)+(C.3.7),(A.1)+(B.1.7)+(C.3.7),(A.2)+(B.1.7)+(C.3.7),(A.3)+(B.1.7)+(C.3.7),(A.4)+(B.1.7)+(C.3.7),(A.1)+(B.1.8)+(C.3.7),(A.2)+(B.1.8)+(C.3.7),(A.3)+(B.1.8)+(C.3.7),(A.4)+(B.1.8)+(C.3.7),(A.1)+(B.1.9)+(C.3.7),(A.2)+(B.1.9)+(C.3.7),(A.3)+(B.1.9)+(C.3.7),(A.4)+(B.1.9)+(C.3.7),(A.1)+(B.1.10)+(C.3.7),(A.2)+(B.1.10)+(C.3.7),(A.3)+(B.1.10)+(C.3.7),(A.4)+(B.1.10)+(C.3.7),(A.1)+(B.1.11)+(C.3.7),(A.2)+(B.1.11)+(C.3.7),(A.3)+(B.1.11)+(C.3.7),(A.4)+(B.1.11)+(C.3.7),(A.1)+(B.1.12)+(C.3.7),(A.2)+(B.1.12)+(C.3.7),(A.3)+(B.1.12)+(C.3.7),(A.4)+(B.1.12)+(C.3.7),(A.1)+(B.1.13)+(C.3.7),(A.2)+(B.1.13)+(C.3.7),(A.3)+(B.1.13)+(C.3.7),(A.4)+(B.1.13)+(C.3.7),(A.1)+(B.1.14)+(C.3.7),(A.2)+(B.1.14)+(C.3.7),(A.3)+(B.1.14)+(C.3.7),(A.4)+(B.1.14)+(C.3.7),(A.1)+(B.1.15)+(C.3.7),(A.2)+(B.1.15)+(C.3.7),(A.3)+(B.1.15)+(C.3.7),(A.4)+(B.1.15)+(C.3.7),(A.1)+(B.1.16)+(C.3.7),(A.2)+(B.1.16)+(C.3.7),(A.3)+(B.1.16)+(C.3.7),(A.4)+(B.1.16)+(C.3.7),(A.1)+(B.1.17)+(C.3.7),(A.2)+(B.1.17)+(C.3.7),(A.3)+(B.1.17)+(C.3.7),(A.4)+(B.1.17)+(C.3.7),
(A.1)+(B.2.1)+(C.3.7),(A.2)+(B.2.1)+(C.3.7),(A.3)+(B.2.1)+(C.3.7),(A.4)+(B.2.1)+(C.3.7),(A.1)+(B.2.2)+(C.3.7),(A.2)+(B.2.2)+(C.3.7),(A.3)+(B.2.2)+(C.3.7),(A.4)+(B.2.2)+(C.3.7),(A.1)+(B.2.3)+(C.3.7),(A.2)+(B.2.3)+(C.3.7),(A.3)+(B.2.3)+(C.3.7),(A.4)+(B.2.3)+(C.3.7),(A.1)+(B.2.4)+(C.3.7),(A.2)+(B.2.4)+(C.3.7),(A.3)+(B.2.4)+(C.3.7),(A.4)+(B.2.4)+(C.3.7),(A.1)+(B.2.5)+(C.3.7),(A.2)+(B.2.5)+(C.3.7),(A.3)+(B.2.5)+(C.3.7),(A.4)+(B.2.5)+(C.3.7),(A.1)+(B.2.6)+(C.3.7),(A.2)+(B.2.6)+(C.3.7),(A.3)+(B.2.6)+(C.3.7),(A.4)+(B.2.6)+(C.3.7),(A.1)+(B.2.7)+(C.3.7),(A.2)+(B.2.7)+(C.3.7),(A.3)+(B.2.7)+(C.3.7),(A.4)+(B.2.7)+(C.3.7),(A.1)+(B.2.8)+(C.3.7),(A.2)+(B.2.8)+(C.3.7),(A.3)+(B.2.8)+(C.3.7),(A.4)+(B.2.8)+(C.3.7)。
(A.1)+(B.1.1)+(C.3.8),(A.2)+(B.1.1)+(C.3.8),(A.3)+(B.1.1)+(C.3.8),(A.4)+(B.1.1)+(C.3.8),(A.1)+(B.1.2)+(C.3.8),(A.2)+(B.1.2)+(C.3.8),(A.3)+(B.1.2)+(C.3.8),(A.4)+(B.1.2)+(C.3.8),(A.1)+(B.1.3)+(C.3.8),(A.2)+(B.1.3)+(C.3.8),(A.3)+(B.1.3)+(C.3.8),(A.4)+(B.1.3)+(C.3.8),(A.1)+(B.1.4)+(C.3.8),(A.2)+(B.1.4)+(C.3.8),(A.3)+(B.1.4)+(C.3.8),(A.4)+(B.1.4)+(C.3.8),(A.1)+(B.1.5)+(C.3.8),(A.2)+(B.1.5)+(C.3.8),(A.3)+(B.1.5)+(C.3.8),(A.4)+(B.1.5)+(C.3.8),(A.1)+(B.1.6)+(C.3.8),(A.2)+(B.1.6)+(C.3.8),(A.3)+(B.1.6)+(C.3.8),(A.4)+(B.1.6)+(C.3.8),(A.1)+(B.1.7)+(C.3.8),(A.2)+(B.1.7)+(C.3.8),(A.3)+(B.1.7)+(C.3.8),(A.4)+(B.1.7)+(C.3.8),(A.1)+(B.1.8)+(C.3.8),(A.2)+(B.1.8)+(C.3.8),(A.3)+(B.1.8)+(C.3.8),(A.4)+(B.1.8)+(C.3.8),(A.1)+(B.1.9)+(C.3.8),(A.2)+(B.1.9)+(C.3.8),(A.3)+(B.1.9)+(C.3.8),(A.4)+(B.1.9)+(C.3.8),(A.1)+(B.1.10)+(C.3.8),(A.2)+(B.1.10)+(C.3.8),(A.3)+(B.1.10)+(C.3.8),(A.4)+(B.1.10)+(C.3.8),(A.1)+(B.1.11)+(C.3.8),(A.2)+(B.1.11)+(C.3.8),(A.3)+(B.1.11)+(C.3.8),(A.4)+(B.1.11)+(C.3.8),(A.1)+(B.1.12)+(C.3.8),(A.2)+(B.1.12)+(C.3.8),(A.3)+(B.1.12)+(C.3.8),(A.4)+(B.1.12)+(C.3.8),(A.1)+(B.1.13)+(C.3.8),(A.2)+(B.1.13)+(C.3.8),(A.3)+(B.1.13)+(C.3.8),(A.4)+(B.1.13)+(C.3.8),(A.1)+(B.1.14)+(C.3.8),(A.2)+(B.1.14)+(C.3.8),(A.3)+(B.1.14)+(C.3.8),(A.4)+(B.1.14)+(C.3.8),(A.1)+(B.1.15)+(C.3.8),(A.2)+(B.1.15)+(C.3.8),(A.3)+(B.1.15)+(C.3.8),(A.4)+(B.1.15)+(C.3.8),(A.1)+(B.1.16)+(C.3.8),(A.2)+(B.1.16)+(C.3.8),(A.3)+(B.1.16)+(C.3.8),(A.4)+(B.1.16)+(C.3.8),(A.1)+(B.1.17)+(C.3.8),(A.2)+(B.1.17)+(C.3.8),(A.3)+(B.1.17)+(C.3.8),(A.4)+(B.1.17)+(C.3.8),
(A.1)+(B.2.1)+(C.3.8),(A.2)+(B.2.1)+(C.3.8),(A.3)+(B.2.1)+(C.3.8),(A.4)+(B.2.1)+(C.3.8),(A.1)+(B.2.2)+(C.3.8),(A.2)+(B.2.2)+(C.3.8),(A.3)+(B.2.2)+(C.3.8),(A.4)+(B.2.2)+(C.3.8),(A.1)+(B.2.3)+(C.3.8),(A.2)+(B.2.3)+(C.3.8),(A.3)+(B.2.3)+(C.3.8),(A.4)+(B.2.3)+(C.3.8),(A.1)+(B.2.4)+(C.3.8),(A.2)+(B.2.4)+(C.3.8),(A.3)+(B.2.4)+(C.3.8),(A.4)+(B.2.4)+(C.3.8),(A.1)+(B.2.5)+(C.3.8),(A.2)+(B.2.5)+(C.3.8),(A.3)+(B.2.5)+(C.3.8),(A.4)+(B.2.5)+(C.3.8),(A.1)+(B.2.6)+(C.3.8),(A.2)+(B.2.6)+(C.3.8),(A.3)+(B.2.6)+(C.3.8),(A.4)+(B.2.6)+(C.3.8),(A.1)+(B.2.7)+(C.3.8),(A.2)+(B.2.7)+(C.3.8),(A.3)+(B.2.7)+(C.3.8),(A.4)+(B.2.7)+(C.3.8),(A.1)+(B.2.8)+(C.3.8),(A.2)+(B.2.8)+(C.3.8),(A.3)+(B.2.8)+(C.3.8),(A.4)+(B.2.8)+(C.3.8)。
(A.1)+(B.1.1)+(C.3.9),(A.2)+(B.1.1)+(C.3.9),(A.3)+(B.1.1)+(C.3.9),(A.4)+(B.1.1)+(C.3.9),(A.1)+(B.1.2)+(C.3.9),(A.2)+(B.1.2)+(C.3.9),(A.3)+(B.1.2)+(C.3.9),(A.4)+(B.1.2)+(C.3.9),(A.1)+(B.1.3)+(C.3.9),(A.2)+(B.1.3)+(C.3.9),(A.3)+(B.1.3)+(C.3.9),(A.4)+(B.1.3)+(C.3.9),(A.1)+(B.1.4)+(C.3.9),(A.2)+(B.1.4)+(C.3.9),(A.3)+(B.1.4)+(C.3.9),(A.4)+(B.1.4)+(C.3.9),(A.1)+(B.1.5)+(C.3.9),(A.2)+(B.1.5)+(C.3.9),(A.3)+(B.1.5)+(C.3.9),(A.4)+(B.1.5)+(C.3.9),(A.1)+(B.1.6)+(C.3.9),(A.2)+(B.1.6)+(C.3.9),(A.3)+(B.1.6)+(C.3.9),(A.4)+(B.1.6)+(C.3.9),(A.1)+(B.1.7)+(C.3.9),(A.2)+(B.1.7)+(C.3.9),(A.3)+(B.1.7)+(C.3.9),(A.4)+(B.1.7)+(C.3.9),(A.1)+(B.1.8)+(C.3.9),(A.2)+(B.1.8)+(C.3.9),(A.3)+(B.1.8)+(C.3.9),(A.4)+(B.1.8)+(C.3.9),(A.1)+(B.1.9)+(C.3.9),(A.2)+(B.1.9)+(C.3.9),(A.3)+(B.1.9)+(C.3.9),(A.4)+(B.1.9)+(C.3.9),(A.1)+(B.1.10)+(C.3.9),(A.2)+(B.1.10)+(C.3.9),(A.3)+(B.1.10)+(C.3.9),(A.4)+(B.1.10)+(C.3.9),(A.1)+(B.1.11)+(C.3.9),(A.2)+(B.1.11)+(C.3.9),(A.3)+(B.1.11)+(C.3.9),(A.4)+(B.1.11)+(C.3.9),(A.1)+(B.1.12)+(C.3.9),(A.2)+(B.1.12)+(C.3.9),(A.3)+(B.1.12)+(C.3.9),(A.4)+(B.1.12)+(C.3.9),(A.1)+(B.1.13)+(C.3.9),(A.2)+(B.1.13)+(C.3.9),(A.3)+(B.1.13)+(C.3.9),(A.4)+(B.1.13)+(C.3.9),(A.1)+(B.1.14)+(C.3.9),(A.2)+(B.1.14)+(C.3.9),(A.3)+(B.1.14)+(C.3.9),(A.4)+(B.1.14)+(C.3.9),(A.1)+(B.1.15)+(C.3.9),(A.2)+(B.1.15)+(C.3.9),(A.3)+(B.1.15)+(C.3.9),(A.4)+(B.1.15)+(C.3.9),(A.1)+(B.1.16)+(C.3.9),(A.2)+(B.1.16)+(C.3.9),(A.3)+(B.1.16)+(C.3.9),(A.4)+(B.1.16)+(C.3.9),(A.1)+(B.1.17)+(C.3.9),(A.2)+(B.1.17)+(C.3.9),(A.3)+(B.1.17)+(C.3.9),(A.4)+(B.1.17)+(C.3.9),
(A.1)+(B.2.1)+(C.3.9),(A.2)+(B.2.1)+(C.3.9),(A.3)+(B.2.1)+(C.3.9),(A.4)+(B.2.1)+(C.3.9),(A.1)+(B.2.2)+(C.3.9),(A.2)+(B.2.2)+(C.3.9),(A.3)+(B.2.2)+(C.3.9),(A.4)+(B.2.2)+(C.3.9),(A.1)+(B.2.3)+(C.3.9),(A.2)+(B.2.3)+(C.3.9),(A.3)+(B.2.3)+(C.3.9),(A.4)+(B.2.3)+(C.3.9),(A.1)+(B.2.4)+(C.3.9),(A.2)+(B.2.4)+(C.3.9),(A.3)+(B.2.4)+(C.3.9),(A.4)+(B.2.4)+(C.3.9),(A.1)+(B.2.5)+(C.3.9),(A.2)+(B.2.5)+(C.3.9),(A.3)+(B.2.5)+(C.3.9),(A.4)+(B.2.5)+(C.3.9),(A.1)+(B.2.6)+(C.3.9),(A.2)+(B.2.6)+(C.3.9),(A.3)+(B.2.6)+(C.3.9),(A.4)+(B.2.6)+(C.3.9),(A.1)+(B.2.7)+(C.3.9),(A.2)+(B.2.7)+(C.3.9),(A.3)+(B.2.7)+(C.3.9),(A.4)+(B.2.7)+(C.3.9),(A.1)+(B.2.8)+(C.3.9),(A.2)+(B.2.8)+(C.3.9),(A.3)+(B.2.8)+(C.3.9),(A.4)+(B.2.8)+(C.3.9)。
(A.1)+(B.1.1)+(C.3.10),(A.2)+(B.1.1)+(C.3.10),(A.3)+(B.1.1)+(C.3.10),(A.4)+(B.1.1)+(C.3.10),(A.1)+(B.1.2)+(C.3.10),(A.2)+(B.1.2)+(C.3.10),(A.3)+(B.1.2)+(C.3.10),(A.4)+(B.1.2)+(C.3.10),(A.1)+(B.1.3)+(C.3.10),(A.2)+(B.1.3)+(C.3.10),(A.3)+(B.1.3)+(C.3.10),(A.4)+(B.1.3)+(C.3.10),(A.1)+(B.1.4)+(C.3.10),(A.2)+(B.1.4)+(C.3.10),(A.3)+(B.1.4)+(C.3.10),(A.4)+(B.1.4)+(C.3.10),(A.1)+(B.1.5)+(C.3.10),(A.2)+(B.1.5)+(C.3.10),(A.3)+(B.1.5)+(C.3.10),(A.4)+(B.1.5)+(C.3.10),(A.1)+(B.1.6)+(C.3.10),(A.2)+(B.1.6)+(C.3.10),(A.3)+(B.1.6)+(C.3.10),(A.4)+(B.1.6)+(C.3.10),(A.1)+(B.1.7)+(C.3.10),(A.2)+(B.1.7)+(C.3.10),(A.3)+(B.1.7)+(C.3.10),(A.4)+(B.1.7)+(C.3.10),(A.1)+(B.1.8)+(C.3.10),(A.2)+(B.1.8)+(C.3.10),(A.3)+(B.1.8)+(C.3.10),(A.4)+(B.1.8)+(C.3.10),(A.1)+(B.1.9)+(C.3.10),(A.2)+(B.1.9)+(C.3.10),(A.3)+(B.1.9)+(C.3.10),(A.4)+(B.1.9)+(C.3.10),(A.1)+(B.1.10)+(C.3.10),(A.2)+(B.1.10)+(C.3.10),(A.3)+(B.1.10)+(C.3.10),(A.4)+(B.1.10)+(C.3.10),(A.1)+(B.1.11)+(C.3.10),(A.2)+(B.1.11)+(C.3.10),(A.3)+(B.1.11)+(C.3.10),(A.4)+(B.1.11)+(C.3.10),(A.1)+(B.1.12)+(C.3.10),(A.2)+(B.1.12)+(C.3.10),(A.3)+(B.1.12)+(C.3.10),(A.4)+(B.1.12)+(C.3.10),(A.1)+(B.1.13)+(C.3.10),(A.2)+(B.1.13)+(C.3.10),(A.3)+(B.1.13)+(C.3.10),(A.4)+(B.1.13)+(C.3.10),(A.1)+(B.1.14)+(C.3.10),(A.2)+(B.1.14)+(C.3.10),(A.3)+(B.1.14)+(C.3.10),(A.4)+(B.1.14)+(C.3.10),(A.1)+(B.1.15)+(C.3.10),(A.2)+(B.1.15)+(C.3.10),(A.3)+(B.1.15)+(C.3.10),(A.4)+(B.1.15)+(C.3.10),(A.1)+(B.1.16)+(C.3.10),(A.2)+(B.1.16)+(C.3.10),(A.3)+(B.1.16)+(C.3.10),(A.4)+(B.1.16)+(C.3.10),(A.1)+(B.1.17)+(C.3.10),(A.2)+(B.1.17)+(C.3.10),(A.3)+(B.1.17)+(C.3.10),(A.4)+(B.1.17)+(C.3.10),
(A.1)+(B.2.1)+(C.3.10),(A.2)+(B.2.1)+(C.3.10),(A.3)+(B.2.1)+(C.3.10),(A.4)+(B.2.1)+(C.3.10),(A.1)+(B.2.2)+(C.3.10),(A.2)+(B.2.2)+(C.3.10),(A.3)+(B.2.2)+(C.3.10),(A.4)+(B.2.2)+(C.3.10),(A.1)+(B.2.3)+(C.3.10),(A.2)+(B.2.3)+(C.3.10),(A.3)+(B.2.3)+(C.3.10),(A.4)+(B.2.3)+(C.3.10),(A.1)+(B.2.4)+(C.3.10),(A.2)+(B.2.4)+(C.3.10),(A.3)+(B.2.4)+(C.3.10),(A.4)+(B.2.4)+(C.3.10),(A.1)+(B.2.5)+(C.3.10),(A.2)+(B.2.5)+(C.3.10),(A.3)+(B.2.5)+(C.3.10),(A.4)+(B.2.5)+(C.3.10),(A.1)+(B.2.6)+(C.3.10),(A.2)+(B.2.6)+(C.3.10),(A.3)+(B.2.6)+(C.3.10),(A.4)+(B.2.6)+(C.3.10),(A.1)+(B.2.7)+(C.3.10),(A.2)+(B.2.7)+(C.3.10),(A.3)+(B.2.7)+(C.3.10),(A.4)+(B.2.7)+(C.3.10),(A.1)+(B.2.8)+(C.3.10),(A.2)+(B.2.8)+(C.3.10),(A.3)+(B.2.8)+(C.3.10),(A.4)+(B.2.8)+(C.3.10)。
(A.1)+(B.1.1)+(C.4.1),(A.2)+(B.1.1)+(C.4.1),(A.3)+(B.1.1)+(C.4.1),(A.4)+(B.1.1)+(C.4.1),(A.1)+(B.1.2)+(C.4.1),(A.2)+(B.1.2)+(C.4.1),(A.3)+(B.1.2)+(C.4.1),(A.4)+(B.1.2)+(C.4.1),(A.1)+(B.1.3)+(C.4.1),(A.2)+(B.1.3)+(C.4.1),(A.3)+(B.1.3)+(C.4.1),(A.4)+(B.1.3)+(C.4.1),(A.1)+(B.1.4)+(C.4.1),(A.2)+(B.1.4)+(C.4.1),(A.3)+(B.1.4)+(C.4.1),(A.4)+(B.1.4)+(C.4.1),(A.1)+(B.1.5)+(C.4.1),(A.2)+(B.1.5)+(C.4.1),(A.3)+(B.1.5)+(C.4.1),(A.4)+(B.1.5)+(C.4.1),(A.1)+(B.1.6)+(C.4.1),(A.2)+(B.1.6)+(C.4.1),(A.3)+(B.1.6)+(C.4.1),(A.4)+(B.1.6)+(C.4.1),(A.1)+(B.1.7)+(C.4.1),(A.2)+(B.1.7)+(C.4.1),(A.3)+(B.1.7)+(C.4.1),(A.4)+(B.1.7)+(C.4.1),(A.1)+(B.1.8)+(C.4.1),(A.2)+(B.1.8)+(C.4.1),(A.3)+(B.1.8)+(C.4.1),(A.4)+(B.1.8)+(C.4.1),(A.1)+(B.1.9)+(C.4.1),(A.2)+(B.1.9)+(C.4.1),(A.3)+(B.1.9)+(C.4.1),(A.4)+(B.1.9)+(C.4.1),(A.1)+(B.1.10)+(C.4.1),(A.2)+(B.1.10)+(C.4.1),(A.3)+(B.1.10)+(C.4.1),(A.4)+(B.1.10)+(C.4.1),(A.1)+(B.1.11)+(C.4.1),(A.2)+(B.1.11)+(C.4.1),(A.3)+(B.1.11)+(C.4.1),(A.4)+(B.1.11)+(C.4.1),(A.1)+(B.1.12)+(C.4.1),(A.2)+(B.1.12)+(C.4.1),(A.3)+(B.1.12)+(C.4.1),(A.4)+(B.1.12)+(C.4.1),(A.1)+(B.1.13)+(C.4.1),(A.2)+(B.1.13)+(C.4.1),(A.3)+(B.1.13)+(C.4.1),(A.4)+(B.1.13)+(C.4.1),(A.1)+(B.1.14)+(C.4.1),(A.2)+(B.1.14)+(C.4.1),(A.3)+(B.1.14)+(C.4.1),(A.4)+(B.1.14)+(C.4.1),(A.1)+(B.1.15)+(C.4.1),(A.2)+(B.1.15)+(C.4.1),(A.3)+(B.1.15)+(C.4.1),(A.4)+(B.1.15)+(C.4.1),(A.1)+(B.1.16)+(C.4.1),(A.2)+(B.1.16)+(C.4.1),(A.3)+(B.1.16)+(C.4.1),(A.4)+(B.1.16)+(C.4.1),(A.1)+(B.1.17)+(C.4.1),(A.2)+(B.1.17)+(C.4.1),(A.3)+(B.1.17)+(C.4.1),(A.4)+(B.1.17)+(C.4.1),
(A.1)+(B.2.1)+(C.4.1),(A.2)+(B.2.1)+(C.4.1),(A.3)+(B.2.1)+(C.4.1),(A.4)+(B.2.1)+(C.4.1),(A.1)+(B.2.2)+(C.4.1),(A.2)+(B.2.2)+(C.4.1),(A.3)+(B.2.2)+(C.4.1),(A.4)+(B.2.2)+(C.4.1),(A.1)+(B.2.3)+(C.4.1),(A.2)+(B.2.3)+(C.4.1),(A.3)+(B.2.3)+(C.4.1),(A.4)+(B.2.3)+(C.4.1),(A.1)+(B.2.4)+(C.4.1),(A.2)+(B.2.4)+(C.4.1),(A.3)+(B.2.4)+(C.4.1),(A.4)+(B.2.4)+(C.4.1),(A.1)+(B.2.5)+(C.4.1),(A.2)+(B.2.5)+(C.4.1),(A.3)+(B.2.5)+(C.4.1),(A.4)+(B.2.5)+(C.4.1),(A.1)+(B.2.6)+(C.4.1),(A.2)+(B.2.6)+(C.4.1),(A.3)+(B.2.6)+(C.4.1),(A.4)+(B.2.6)+(C.4.1),(A.1)+(B.2.7)+(C.4.1),(A.2)+(B.2.7)+(C.4.1),(A.3)+(B.2.7)+(C.4.1),(A.4)+(B.2.7)+(C.4.1),(A.1)+(B.2.8)+(C.4.1),(A.2)+(B.2.8)+(C.4.1),(A.3)+(B.2.8)+(C.4.1),(A.4)+(B.2.8)+(C.4.1)。
(A.1)+(B.1.1)+(C.4.2),(A.2)+(B.1.1)+(C.4.2),(A.3)+(B.1.1)+(C.4.2),(A.4)+(B.1.1)+(C.4.2),(A.1)+(B.1.2)+(C.4.2),(A.2)+(B.1.2)+(C.4.2),(A.3)+(B.1.2)+(C.4.2),(A.4)+(B.1.2)+(C.4.2),(A.1)+(B.1.3)+(C.4.2),(A.2)+(B.1.3)+(C.4.2),(A.3)+(B.1.3)+(C.4.2),(A.4)+(B.1.3)+(C.4.2),(A.1)+(B.1.4)+(C.4.2),(A.2)+(B.1.4)+(C.4.2),(A.3)+(B.1.4)+(C.4.2),(A.4)+(B.1.4)+(C.4.2),(A.1)+(B.1.5)+(C.4.2),(A.2)+(B.1.5)+(C.4.2),(A.3)+(B.1.5)+(C.4.2),(A.4)+(B.1.5)+(C.4.2),(A.1)+(B.1.6)+(C.4.2),(A.2)+(B.1.6)+(C.4.2),(A.3)+(B.1.6)+(C.4.2),(A.4)+(B.1.6)+(C.4.2),(A.1)+(B.1.7)+(C.4.2),(A.2)+(B.1.7)+(C.4.2),(A.3)+(B.1.7)+(C.4.2),(A.4)+(B.1.7)+(C.4.2),(A.1)+(B.1.8)+(C.4.2),(A.2)+(B.1.8)+(C.4.2),(A.3)+(B.1.8)+(C.4.2),(A.4)+(B.1.8)+(C.4.2),(A.1)+(B.1.9)+(C.4.2),(A.2)+(B.1.9)+(C.4.2),(A.3)+(B.1.9)+(C.4.2),(A.4)+(B.1.9)+(C.4.2),(A.1)+(B.1.10)+(C.4.2),(A.2)+(B.1.10)+(C.4.2),(A.3)+(B.1.10)+(C.4.2),(A.4)+(B.1.10)+(C.4.2),(A.1)+(B.1.11)+(C.4.2),(A.2)+(B.1.11)+(C.4.2),(A.3)+(B.1.11)+(C.4.2),(A.4)+(B.1.11)+(C.4.2),(A.1)+(B.1.12)+(C.4.2),(A.2)+(B.1.12)+(C.4.2),(A.3)+(B.1.12)+(C.4.2),(A.4)+(B.1.12)+(C.4.2),(A.1)+(B.1.13)+(C.4.2),(A.2)+(B.1.13)+(C.4.2),(A.3)+(B.1.13)+(C.4.2),(A.4)+(B.1.13)+(C.4.2),(A.1)+(B.1.14)+(C.4.2),(A.2)+(B.1.14)+(C.4.2),(A.3)+(B.1.14)+(C.4.2),(A.4)+(B.1.14)+(C.4.2),(A.1)+(B.1.15)+(C.4.2),(A.2)+(B.1.15)+(C.4.2),(A.3)+(B.1.15)+(C.4.2),(A.4)+(B.1.15)+(C.4.2),(A.1)+(B.1.16)+(C.4.2),(A.2)+(B.1.16)+(C.4.2),(A.3)+(B.1.16)+(C.4.2),(A.4)+(B.1.16)+(C.4.2),(A.1)+(B.1.17)+(C.4.2),(A.2)+(B.1.17)+(C.4.2),(A.3)+(B.1.17)+(C.4.2),(A.4)+(B.1.17)+(C.4.2),
(A.1)+(B.2.1)+(C.4.2),(A.2)+(B.2.1)+(C.4.2),(A.3)+(B.2.1)+(C.4.2),(A.4)+(B.2.1)+(C.4.2),(A.1)+(B.2.2)+(C.4.2),(A.2)+(B.2.2)+(C.4.2),(A.3)+(B.2.2)+(C.4.2),(A.4)+(B.2.2)+(C.4.2),(A.1)+(B.2.3)+(C.4.2),(A.2)+(B.2.3)+(C.4.2),(A.3)+(B.2.3)+(C.4.2),(A.4)+(B.2.3)+(C.4.2),(A.1)+(B.2.4)+(C.4.2),(A.2)+(B.2.4)+(C.4.2),(A.3)+(B.2.4)+(C.4.2),(A.4)+(B.2.4)+(C.4.2),(A.1)+(B.2.5)+(C.4.2),(A.2)+(B.2.5)+(C.4.2),(A.3)+(B.2.5)+(C.4.2),(A.4)+(B.2.5)+(C.4.2),(A.1)+(B.2.6)+(C.4.2),(A.2)+(B.2.6)+(C.4.2),(A.3)+(B.2.6)+(C.4.2),(A.4)+(B.2.6)+(C.4.2),(A.1)+(B.2.7)+(C.4.2),(A.2)+(B.2.7)+(C.4.2),(A.3)+(B.2.7)+(C.4.2),(A.4)+(B.2.7)+(C.4.2),(A.1)+(B.2.8)+(C.4.2),(A.2)+(B.2.8)+(C.4.2),(A.3)+(B.2.8)+(C.4.2),(A.4)+(B.2.8)+(C.4.2)。
(A.1)+(B.1.1)+(C.4.3),(A.2)+(B.1.1)+(C.4.3),(A.3)+(B.1.1)+(C.4.3),(A.4)+(B.1.1)+(C.4.3),(A.1)+(B.1.2)+(C.4.3),(A.2)+(B.1.2)+(C.4.3),(A.3)+(B.1.2)+(C.4.3),(A.4)+(B.1.2)+(C.4.3),(A.1)+(B.1.3)+(C.4.3),(A.2)+(B.1.3)+(C.4.3),(A.3)+(B.1.3)+(C.4.3),(A.4)+(B.1.3)+(C.4.3),(A.1)+(B.1.4)+(C.4.3),(A.2)+(B.1.4)+(C.4.3),(A.3)+(B.1.4)+(C.4.3),(A.4)+(B.1.4)+(C.4.3),(A.1)+(B.1.5)+(C.4.3),(A.2)+(B.1.5)+(C.4.3),(A.3)+(B.1.5)+(C.4.3),(A.4)+(B.1.5)+(C.4.3),(A.1)+(B.1.6)+(C.4.3),(A.2)+(B.1.6)+(C.4.3),(A.3)+(B.1.6)+(C.4.3),(A.4)+(B.1.6)+(C.4.3),(A.1)+(B.1.7)+(C.4.3),(A.2)+(B.1.7)+(C.4.3),(A.3)+(B.1.7)+(C.4.3),(A.4)+(B.1.7)+(C.4.3),(A.1)+(B.1.8)+(C.4.3),(A.2)+(B.1.8)+(C.4.3),(A.3)+(B.1.8)+(C.4.3),(A.4)+(B.1.8)+(C.4.3),(A.1)+(B.1.9)+(C.4.3),(A.2)+(B.1.9)+(C.4.3),(A.3)+(B.1.9)+(C.4.3),(A.4)+(B.1.9)+(C.4.3),(A.1)+(B.1.10)+(C.4.3),(A.2)+(B.1.10)+(C.4.3),(A.3)+(B.1.10)+(C.4.3),(A.4)+(B.1.10)+(C.4.3),(A.1)+(B.1.11)+(C.4.3),(A.2)+(B.1.11)+(C.4.3),(A.3)+(B.1.11)+(C.4.3),(A.4)+(B.1.11)+(C.4.3),(A.1)+(B.1.12)+(C.4.3),(A.2)+(B.1.12)+(C.4.3),(A.3)+(B.1.12)+(C.4.3),(A.4)+(B.1.12)+(C.4.3),(A.1)+(B.1.13)+(C.4.3),(A.2)+(B.1.13)+(C.4.3),(A.3)+(B.1.13)+(C.4.3),(A.4)+(B.1.13)+(C.4.3),(A.1)+(B.1.14)+(C.4.3),(A.2)+(B.1.14)+(C.4.3),(A.3)+(B.1.14)+(C.4.3),(A.4)+(B.1.14)+(C.4.3),(A.1)+(B.1.15)+(C.4.3),(A.2)+(B.1.15)+(C.4.3),(A.3)+(B.1.15)+(C.4.3),(A.4)+(B.1.15)+(C.4.3),(A.1)+(B.1.16)+(C.4.3),(A.2)+(B.1.16)+(C.4.3),(A.3)+(B.1.16)+(C.4.3),(A.4)+(B.1.16)+(C.4.3),(A.1)+(B.1.17)+(C.4.3),(A.2)+(B.1.17)+(C.4.3),(A.3)+(B.1.17)+(C.4.3),(A.4)+(B.1.17)+(C.4.3),
(A.1)+(B.2.1)+(C.4.3),(A.2)+(B.2.1)+(C.4.3),(A.3)+(B.2.1)+(C.4.3),(A.4)+(B.2.1)+(C.4.3),(A.1)+(B.2.2)+(C.4.3),(A.2)+(B.2.2)+(C.4.3),(A.3)+(B.2.2)+(C.4.3),(A.4)+(B.2.2)+(C.4.3),(A.1)+(B.2.3)+(C.4.3),(A.2)+(B.2.3)+(C.4.3),(A.3)+(B.2.3)+(C.4.3),(A.4)+(B.2.3)+(C.4.3),(A.1)+(B.2.4)+(C.4.3),(A.2)+(B.2.4)+(C.4.3),(A.3)+(B.2.4)+(C.4.3),(A.4)+(B.2.4)+(C.4.3),(A.1)+(B.2.5)+(C.4.3),(A.2)+(B.2.5)+(C.4.3),(A.3)+(B.2.5)+(C.4.3),(A.4)+(B.2.5)+(C.4.3),(A.1)+(B.2.6)+(C.4.3),(A.2)+(B.2.6)+(C.4.3),(A.3)+(B.2.6)+(C.4.3),(A.4)+(B.2.6)+(C.4.3),(A.1)+(B.2.7)+(C.4.3),(A.2)+(B.2.7)+(C.4.3),(A.3)+(B.2.7)+(C.4.3),(A.4)+(B.2.7)+(C.4.3),(A.1)+(B.2.8)+(C.4.3),(A.2)+(B.2.8)+(C.4.3),(A.3)+(B.2.8)+(C.4.3),(A.4)+(B.2.8)+(C.4.3)。
(A.1)+(B.1.1)+(C.4.4),(A.2)+(B.1.1)+(C.4.4),(A.3)+(B.1.1)+(C.4.4),(A.4)+(B.1.1)+(C.4.4),(A.1)+(B.1.2)+(C.4.4),(A.2)+(B.1.2)+(C.4.4),(A.3)+(B.1.2)+(C.4.4),(A.4)+(B.1.2)+(C.4.4),(A.1)+(B.1.3)+(C.4.4),(A.2)+(B.1.3)+(C.4.4),(A.3)+(B.1.3)+(C.4.4),(A.4)+(B.1.3)+(C.4.4),(A.1)+(B.1.4)+(C.4.4),(A.2)+(B.1.4)+(C.4.4),(A.3)+(B.1.4)+(C.4.4),(A.4)+(B.1.4)+(C.4.4),(A.1)+(B.1.5)+(C.4.4),(A.2)+(B.1.5)+(C.4.4),(A.3)+(B.1.5)+(C.4.4),(A.4)+(B.1.5)+(C.4.4),(A.1)+(B.1.6)+(C.4.4),(A.2)+(B.1.6)+(C.4.4),(A.3)+(B.1.6)+(C.4.4),(A.4)+(B.1.6)+(C.4.4),(A.1)+(B.1.7)+(C.4.4),(A.2)+(B.1.7)+(C.4.4),(A.3)+(B.1.7)+(C.4.4),(A.4)+(B.1.7)+(C.4.4),(A.1)+(B.1.8)+(C.4.4),(A.2)+(B.1.8)+(C.4.4),(A.3)+(B.1.8)+(C.4.4),(A.4)+(B.1.8)+(C.4.4),(A.1)+(B.1.9)+(C.4.4),(A.2)+(B.1.9)+(C.4.4),(A.3)+(B.1.9)+(C.4.4),(A.4)+(B.1.9)+(C.4.4),(A.1)+(B.1.10)+(C.4.4),(A.2)+(B.1.10)+(C.4.4),(A.3)+(B.1.10)+(C.4.4),(A.4)+(B.1.10)+(C.4.4),(A.1)+(B.1.11)+(C.4.4),(A.2)+(B.1.11)+(C.4.4),(A.3)+(B.1.11)+(C.4.4),(A.4)+(B.1.11)+(C.4.4),(A.1)+(B.1.12)+(C.4.4),(A.2)+(B.1.12)+(C.4.4),(A.3)+(B.1.12)+(C.4.4),(A.4)+(B.1.12)+(C.4.4),(A.1)+(B.1.13)+(C.4.4),(A.2)+(B.1.13)+(C.4.4),(A.3)+(B.1.13)+(C.4.4),(A.4)+(B.1.13)+(C.4.4),(A.1)+(B.1.14)+(C.4.4),(A.2)+(B.1.14)+(C.4.4),(A.3)+(B.1.14)+(C.4.4),(A.4)+(B.1.14)+(C.4.4),(A.1)+(B.1.15)+(C.4.4),(A.2)+(B.1.15)+(C.4.4),(A.3)+(B.1.15)+(C.4.4),(A.4)+(B.1.15)+(C.4.4),(A.1)+(B.1.16)+(C.4.4),(A.2)+(B.1.16)+(C.4.4),(A.3)+(B.1.16)+(C.4.4),(A.4)+(B.1.16)+(C.4.4),(A.1)+(B.1.17)+(C.4.4),(A.2)+(B.1.17)+(C.4.4),(A.3)+(B.1.17)+(C.4.4),(A.4)+(B.1.17)+(C.4.4),
(A.1)+(B.2.1)+(C.4.4),(A.2)+(B.2.1)+(C.4.4),(A.3)+(B.2.1)+(C.4.4),(A.4)+(B.2.1)+(C.4.4),(A.1)+(B.2.2)+(C.4.4),(A.2)+(B.2.2)+(C.4.4),(A.3)+(B.2.2)+(C.4.4),(A.4)+(B.2.2)+(C.4.4),(A.1)+(B.2.3)+(C.4.4),(A.2)+(B.2.3)+(C.4.4),(A.3)+(B.2.3)+(C.4.4),(A.4)+(B.2.3)+(C.4.4),(A.1)+(B.2.4)+(C.4.4),(A.2)+(B.2.4)+(C.4.4),(A.3)+(B.2.4)+(C.4.4),(A.4)+(B.2.4)+(C.4.4),(A.1)+(B.2.5)+(C.4.4),(A.2)+(B.2.5)+(C.4.4),(A.3)+(B.2.5)+(C.4.4),(A.4)+(B.2.5)+(C.4.4),(A.1)+(B.2.6)+(C.4.4),(A.2)+(B.2.6)+(C.4.4),(A.3)+(B.2.6)+(C.4.4),(A.4)+(B.2.6)+(C.4.4),(A.1)+(B.2.7)+(C.4.4),(A.2)+(B.2.7)+(C.4.4),(A.3)+(B.2.7)+(C.4.4),(A.4)+(B.2.7)+(C.4.4),(A.1)+(B.2.8)+(C.4.4),(A.2)+(B.2.8)+(C.4.4),(A.3)+(B.2.8)+(C.4.4),(A.4)+(B.2.8)+(C.4.4)。
(A.1)+(B.1.1)+(C.4.5),(A.2)+(B.1.1)+(C.4.5),(A.3)+(B.1.1)+(C.4.5),(A.4)+(B.1.1)+(C.4.5),(A.1)+(B.1.2)+(C.4.5),(A.2)+(B.1.2)+(C.4.5),(A.3)+(B.1.2)+(C.4.5),(A.4)+(B.1.2)+(C.4.5),(A.1)+(B.1.3)+(C.4.5),(A.2)+(B.1.3)+(C.4.5),(A.3)+(B.1.3)+(C.4.5),(A.4)+(B.1.3)+(C.4.5),(A.1)+(B.1.4)+(C.4.5),(A.2)+(B.1.4)+(C.4.5),(A.3)+(B.1.4)+(C.4.5),(A.4)+(B.1.4)+(C.4.5),(A.1)+(B.1.5)+(C.4.5),(A.2)+(B.1.5)+(C.4.5),(A.3)+(B.1.5)+(C.4.5),(A.4)+(B.1.5)+(C.4.5),(A.1)+(B.1.6)+(C.4.5),(A.2)+(B.1.6)+(C.4.5),(A.3)+(B.1.6)+(C.4.5),(A.4)+(B.1.6)+(C.4.5),(A.1)+(B.1.7)+(C.4.5),(A.2)+(B.1.7)+(C.4.5),(A.3)+(B.1.7)+(C.4.5),(A.4)+(B.1.7)+(C.4.5),(A.1)+(B.1.8)+(C.4.5),(A.2)+(B.1.8)+(C.4.5),(A.3)+(B.1.8)+(C.4.5),(A.4)+(B.1.8)+(C.4.5),(A.1)+(B.1.9)+(C.4.5),(A.2)+(B.1.9)+(C.4.5),(A.3)+(B.1.9)+(C.4.5),(A.4)+(B.1.9)+(C.4.5),(A.1)+(B.1.10)+(C.4.5),(A.2)+(B.1.10)+(C.4.5),(A.3)+(B.1.10)+(C.4.5),(A.4)+(B.1.10)+(C.4.5),(A.1)+(B.1.11)+(C.4.5),(A.2)+(B.1.11)+(C.4.5),(A.3)+(B.1.11)+(C.4.5),(A.4)+(B.1.11)+(C.4.5),(A.1)+(B.1.12)+(C.4.5),(A.2)+(B.1.12)+(C.4.5),(A.3)+(B.1.12)+(C.4.5),(A.4)+(B.1.12)+(C.4.5),(A.1)+(B.1.13)+(C.4.5),(A.2)+(B.1.13)+(C.4.5),(A.3)+(B.1.13)+(C.4.5),(A.4)+(B.1.13)+(C.4.5),(A.1)+(B.1.14)+(C.4.5),(A.2)+(B.1.14)+(C.4.5),(A.3)+(B.1.14)+(C.4.5),(A.4)+(B.1.14)+(C.4.5),(A.1)+(B.1.15)+(C.4.5),(A.2)+(B.1.15)+(C.4.5),(A.3)+(B.1.15)+(C.4.5),(A.4)+(B.1.15)+(C.4.5),(A.1)+(B.1.16)+(C.4.5),(A.2)+(B.1.16)+(C.4.5),(A.3)+(B.1.16)+(C.4.5),(A.4)+(B.1.16)+(C.4.5),(A.1)+(B.1.17)+(C.4.5),(A.2)+(B.1.17)+(C.4.5),(A.3)+(B.1.17)+(C.4.5),(A.4)+(B.1.17)+(C.4.5),
(A.1)+(B.2.1)+(C.4.5),(A.2)+(B.2.1)+(C.4.5),(A.3)+(B.2.1)+(C.4.5),(A.4)+(B.2.1)+(C.4.5),(A.1)+(B.2.2)+(C.4.5),(A.2)+(B.2.2)+(C.4.5),(A.3)+(B.2.2)+(C.4.5),(A.4)+(B.2.2)+(C.4.5),(A.1)+(B.2.3)+(C.4.5),(A.2)+(B.2.3)+(C.4.5),(A.3)+(B.2.3)+(C.4.5),(A.4)+(B.2.3)+(C.4.5),(A.1)+(B.2.4)+(C.4.5),(A.2)+(B.2.4)+(C.4.5),(A.3)+(B.2.4)+(C.4.5),(A.4)+(B.2.4)+(C.4.5),(A.1)+(B.2.5)+(C.4.5),(A.2)+(B.2.5)+(C.4.5),(A.3)+(B.2.5)+(C.4.5),(A.4)+(B.2.5)+(C.4.5),(A.1)+(B.2.6)+(C.4.5),(A.2)+(B.2.6)+(C.4.5),(A.3)+(B.2.6)+(C.4.5),(A.4)+(B.2.6)+(C.4.5),(A.1)+(B.2.7)+(C.4.5),(A.2)+(B.2.7)+(C.4.5),(A.3)+(B.2.7)+(C.4.5),(A.4)+(B.2.7)+(C.4.5),(A.1)+(B.2.8)+(C.4.5),(A.2)+(B.2.8)+(C.4.5),(A.3)+(B.2.8)+(C.4.5),(A.4)+(B.2.8)+(C.4.5)。
(A.1)+(B.1.1)+(C.4.6),(A.2)+(B.1.1)+(C.4.6),(A.3)+(B.1.1)+(C.4.6),(A.4)+(B.1.1)+(C.4.6),(A.1)+(B.1.2)+(C.4.6),(A.2)+(B.1.2)+(C.4.6),(A.3)+(B.1.2)+(C.4.6),(A.4)+(B.1.2)+(C.4.6),(A.1)+(B.1.3)+(C.4.6),(A.2)+(B.1.3)+(C.4.6),(A.3)+(B.1.3)+(C.4.6),(A.4)+(B.1.3)+(C.4.6),(A.1)+(B.1.4)+(C.4.6),(A.2)+(B.1.4)+(C.4.6),(A.3)+(B.1.4)+(C.4.6),(A.4)+(B.1.4)+(C.4.6),(A.1)+(B.1.5)+(C.4.6),(A.2)+(B.1.5)+(C.4.6),(A.3)+(B.1.5)+(C.4.6),(A.4)+(B.1.5)+(C.4.6),(A.1)+(B.1.6)+(C.4.6),(A.2)+(B.1.6)+(C.4.6),(A.3)+(B.1.6)+(C.4.6),(A.4)+(B.1.6)+(C.4.6),(A.1)+(B.1.7)+(C.4.6),(A.2)+(B.1.7)+(C.4.6),(A.3)+(B.1.7)+(C.4.6),(A.4)+(B.1.7)+(C.4.6),(A.1)+(B.1.8)+(C.4.6),(A.2)+(B.1.8)+(C.4.6),(A.3)+(B.1.8)+(C.4.6),(A.4)+(B.1.8)+(C.4.6),(A.1)+(B.1.9)+(C.4.6),(A.2)+(B.1.9)+(C.4.6),(A.3)+(B.1.9)+(C.4.6),(A.4)+(B.1.9)+(C.4.6),(A.1)+(B.1.10)+(C.4.6),(A.2)+(B.1.10)+(C.4.6),(A.3)+(B.1.10)+(C.4.6),(A.4)+(B.1.10)+(C.4.6),(A.1)+(B.1.11)+(C.4.6),(A.2)+(B.1.11)+(C.4.6),(A.3)+(B.1.11)+(C.4.6),(A.4)+(B.1.11)+(C.4.6),(A.1)+(B.1.12)+(C.4.6),(A.2)+(B.1.12)+(C.4.6),(A.3)+(B.1.12)+(C.4.6),(A.4)+(B.1.12)+(C.4.6),(A.1)+(B.1.13)+(C.4.6),(A.2)+(B.1.13)+(C.4.6),(A.3)+(B.1.13)+(C.4.6),(A.4)+(B.1.13)+(C.4.6),(A.1)+(B.1.14)+(C.4.6),(A.2)+(B.1.14)+(C.4.6),(A.3)+(B.1.14)+(C.4.6),(A.4)+(B.1.14)+(C.4.6),(A.1)+(B.1.15)+(C.4.6),(A.2)+(B.1.15)+(C.4.6),(A.3)+(B.1.15)+(C.4.6),(A.4)+(B.1.15)+(C.4.6),(A.1)+(B.1.16)+(C.4.6),(A.2)+(B.1.16)+(C.4.6),(A.3)+(B.1.16)+(C.4.6),(A.4)+(B.1.16)+(C.4.6),(A.1)+(B.1.17)+(C.4.6),(A.2)+(B.1.17)+(C.4.6),(A.3)+(B.1.17)+(C.4.6),(A.4)+(B.1.17)+(C.4.6),
(A.1)+(B.2.1)+(C.4.6),(A.2)+(B.2.1)+(C.4.6),(A.3)+(B.2.1)+(C.4.6),(A.4)+(B.2.1)+(C.4.6),(A.1)+(B.2.2)+(C.4.6),(A.2)+(B.2.2)+(C.4.6),(A.3)+(B.2.2)+(C.4.6),(A.4)+(B.2.2)+(C.4.6),(A.1)+(B.2.3)+(C.4.6),(A.2)+(B.2.3)+(C.4.6),(A.3)+(B.2.3)+(C.4.6),(A.4)+(B.2.3)+(C.4.6),(A.1)+(B.2.4)+(C.4.6),(A.2)+(B.2.4)+(C.4.6),(A.3)+(B.2.4)+(C.4.6),(A.4)+(B.2.4)+(C.4.6),(A.1)+(B.2.5)+(C.4.6),(A.2)+(B.2.5)+(C.4.6),(A.3)+(B.2.5)+(C.4.6),(A.4)+(B.2.5)+(C.4.6),(A.1)+(B.2.6)+(C.4.6),(A.2)+(B.2.6)+(C.4.6),(A.3)+(B.2.6)+(C.4.6),(A.4)+(B.2.6)+(C.4.6),(A.1)+(B.2.7)+(C.4.6),(A.2)+(B.2.7)+(C.4.6),(A.3)+(B.2.7)+(C.4.6),(A.4)+(B.2.7)+(C.4.6),(A.1)+(B.2.8)+(C.4.6),(A.2)+(B.2.8)+(C.4.6),(A.3)+(B.2.8)+(C.4.6),(A.4)+(B.2.8)+(C.4.6)。
(A.1)+(B.1.1)+(C.5),(A.2)+(B.1.1)+(C.5),(A.3)+(B.1.1)+(C.5),(A.4)+(B.1.1)+(C.5),(A.1)+(B.1.2)+(C.5),(A.2)+(B.1.2)+(C.5),(A.3)+(B.1.2)+(C.5),(A.4)+(B.1.2)+(C.5),(A.1)+(B.1.3)+(C.5),(A.2)+(B.1.3)+(C.5),(A.3)+(B.1.3)+(C.5),(A.4)+(B.1.3)+(C.5),(A.1)+(B.1.4)+(C.5),(A.2)+(B.1.4)+(C.5),(A.3)+(B.1.4)+(C.5),(A.4)+(B.1.4)+(C.5),(A.1)+(B.1.5)+(C.5),(A.2)+(B.1.5)+(C.5),(A.3)+(B.1.5)+(C.5),(A.4)+(B.1.5)+(C.5),(A.1)+(B.1.6)+(C.5),(A.2)+(B.1.6)+(C.5),(A.3)+(B.1.6)+(C.5),(A.4)+(B.1.6)+(C.5),(A.1)+(B.1.7)+(C.5),(A.2)+(B.1.7)+(C.5),(A.3)+(B.1.7)+(C.5),(A.4)+(B.1.7)+(C.5),(A.1)+(B.1.8)+(C.5),(A.2)+(B.1.8)+(C.5),(A.3)+(B.1.8)+(C.5),(A.4)+(B.1.8)+(C.5),(A.1)+(B.1.9)+(C.5),(A.2)+(B.1.9)+(C.5),(A.3)+(B.1.9)+(C.5),(A.4)+(B.1.9)+(C.5),(A.1)+(B.1.10)+(C.5),(A.2)+(B.1.10)+(C.5),(A.3)+(B.1.10)+(C.5),(A.4)+(B.1.10)+(C.5),(A.1)+(B.1.11)+(C.5),(A.2)+(B.1.11)+(C.5),(A.3)+(B.1.11)+(C.5),(A.4)+(B.1.11)+(C.5),(A.1)+(B.1.12)+(C.5),(A.2)+(B.1.12)+(C.5),(A.3)+(B.1.12)+(C.5),(A.4)+(B.1.12)+(C.5),(A.1)+(B.1.13)+(C.5),(A.2)+(B.1.13)+(C.5),(A.3)+(B.1.13)+(C.5),(A.4)+(B.1.13)+(C.5),(A.1)+(B.1.14)+(C.5),(A.2)+(B.1.14)+(C.5),(A.3)+(B.1.14)+(C.5),(A.4)+(B.1.14)+(C.5),(A.1)+(B.1.15)+(C.5),(A.2)+(B.1.15)+(C.5),(A.3)+(B.1.15)+(C.5),(A.4)+(B.1.15)+(C.5),(A.1)+(B.1.16)+(C.5),(A.2)+(B.1.16)+(C.5),(A.3)+(B.1.16)+(C.5),(A.4)+(B.1.16)+(C.5),(A.1)+(B.1.17)+(C.5),(A.2)+(B.1.17)+(C.5),(A.3)+(B.1.17)+(C.5),(A.4)+(B.1.17)+(C.5),
(A.1)+(B.2.1)+(C.5),(A.2)+(B.2.1)+(C.5),(A.3)+(B.2.1)+(C.5),(A.4)+(B.2.1)+(C.5),(A.1)+(B.2.2)+(C.5),(A.2)+(B.2.2)+(C.5),(A.3)+(B.2.2)+(C.5),(A.4)+(B.2.2)+(C.5),(A.1)+(B.2.3)+(C.5),(A.2)+(B.2.3)+(C.5),(A.3)+(B.2.3)+(C.5),(A.4)+(B.2.3)+(C.5),(A.1)+(B.2.4)+(C.5),(A.2)+(B.2.4)+(C.5),(A.3)+(B.2.4)+(C.5),(A.4)+(B.2.4)+(C.5),(A.1)+(B.2.5)+(C.5),(A.2)+(B.2.5)+(C.5),(A.3)+(B.2.5)+(C.5),(A.4)+(B.2.5)+(C.5),(A.1)+(B.2.6)+(C.5),(A.2)+(B.2.6)+(C.5),(A.3)+(B.2.6)+(C.5),(A.4)+(B.2.6)+(C.5),(A.1)+(B.2.7)+(C.5),(A.2)+(B.2.7)+(C.5),(A.3)+(B.2.7)+(C.5),(A.4)+(B.2.7)+(C.5),(A.1)+(B.2.8)+(C.5),(A.2)+(B.2.8)+(C.5),(A.3)+(B.2.8)+(C.5),(A.4)+(B.2.8)+(C.5)。
其中甚至进一步优选以下结合物:
(A.1)+(B.1.1)+(C.1.1),(A.2)+(B.1.1)+(C.1.1),(A.1)+(B.1.2)+(C.1.1),(A.2)+(B.1.2)+(C.1.1),(A.1)+(B.1.3)+(C.1.1),(A.2)+(B.1.3)+(C.1.1),(A.1)+(B.1.4)+(C.1.1),(A.2)+(B.1.4)+(C.1.1),(A.1)+(B.1.5)+(C.1.1),(A.2)+(B.1.5)+(C.1.1),(A.1)+(B.1.6)+(C.1.1),(A.2)+(B.1.6)+(C.1.1),(A.1)+(B.1.7)+(C.1.1),(A.2)+(B.1.7)+(C.1.1),(A.1)+(B.1.8)+(C.1.1),(A.2)+(B.1.8)+(C.1.1),(A.1)+(B.1.9)+(C.1.1),(A.2)+(B.1.9)+(C.1.1),(A.1)+(B.1.10)+(C.1.1),(A.2)+(B.1.10)+(C.1.1),(A.1)+(B.1.11)+(C.1.1),(A.2)+(B.1.11)+(C.1.1),
(A.1)+(B.2.1)+(C.1.1),(A.2)+(B.2.1)+(C.1.1)。
(A.1)+(B.1.1)+(C.1.2),(A.2)+(B.1.1)+(C.1.2),(A.1)+(B.1.2)+(C.1.2),(A.2)+(B.1.2)+(C.1.2),(A.1)+(B.1.3)+(C.1.2),(A.2)+(B.1.3)+(C.1.2),(A.1)+(B.1.4)+(C.1.2),(A.2)+(B.1.4)+(C.1.2),(A.1)+(B.1.5)+(C.1.2),(A.2)+(B.1.5)+(C.1.2),(A.1)+(B.1.6)+(C.1.2),(A.2)+(B.1.6)+(C.1.2),(A.1)+(B.1.7)+(C.1.2),(A.2)+(B.1.7)+(C.1.2),(A.1)+(B.1.8)+(C.1.2),(A.2)+(B.1.8)+(C.1.2),(A.1)+(B.1.9)+(C.1.2),(A.2)+(B.1.9)+(C.1.2),(A.1)+(B.1.10)+(C.1.2),(A.2)+(B.1.10)+(C.1.2),(A.1)+(B.1.11)+(C.1.2),(A.2)+(B.1.11)+(C.1.2),
(A.1)+(B.2.1)+(C.1.2),(A.2)+(B.2.1)+(C.1.2)。
(A.1)+(B.1.1)+(C.1.3),(A.2)+(B.1.1)+(C.1.3),(A.1)+(B.1.2)+(C.1.3),(A.2)+(B.1.2)+(C.1.3),(A.1)+(B.1.3)+(C.1.3),(A.2)+(B.1.3)+(C.1.3),(A.1)+(B.1.4)+(C.1.3),(A.2)+(B.1.4)+(C.1.3),(A.1)+(B.1.5)+(C.1.3),(A.2)+(B.1.5)+(C.1.3),(A.1)+(B.1.6)+(C.1.3),(A.2)+(B.1.6)+(C.1.3),(A.1)+(B.1.7)+(C.1.3),(A.2)+(B.1.7)+(C.1.3),(A.1)+(B.1.8)+(C.1.3),(A.2)+(B.1.8)+(C.1.3),(A.1)+(B.1.9)+(C.1.3),(A.2)+(B.1.9)+(C.1.3),(A.1)+(B.1.10)+(C.1.3),(A.2)+(B.1.10)+(C.1.3),(A.1)+(B.1.11)+(C.1.3),(A.2)+(B.1.11)+(C.1.3),
(A.1)+(B.2.1)+(C.1.3),(A.2)+(B.2.1)+(C.1.3)。
(A.1)+(B.1.1)+(C.2.1),(A.2)+(B.1.1)+(C.2.1),(A.1)+(B.1.2)+(C.2.1),(A.2)+(B.1.2)+(C.2.1),(A.1)+(B.1.3)+(C.2.1),(A.2)+(B.1.3)+(C.2.1),(A.1)+(B.1.4)+(C.2.1),(A.2)+(B.1.4)+(C.2.1),(A.1)+(B.1.5)+(C.2.1),(A.2)+(B.1.5)+(C.2.1),(A.1)+(B.1.6)+(C.2.1),(A.2)+(B.1.6)+(C.2.1),(A.1)+(B.1.7)+(C.2.1),(A.2)+(B.1.7)+(C.2.1),(A.1)+(B.1.8)+(C.2.1),(A.2)+(B.1.8)+(C.2.1),(A.1)+(B.1.9)+(C.2.1),(A.2)+(B.1.9)+(C.2.1),(A.1)+(B.1.10)+(C.2.1),(A.2)+(B.1.10)+(C.2.1),(A.1)+(B.1.11)+(C.2.1),(A.2)+(B.1.11)+(C.2.1),
(A.1)+(B.2.1)+(C.2.1),(A.2)+(B.2.1)+(C.2.1)。
(A.1)+(B.1.1)+(C.2.3),(A.2)+(B.1.1)+(C.2.3),(A.1)+(B.1.2)+(C.2.3),(A.2)+(B.1.2)+(C.2.3),(A.1)+(B.1.3)+(C.2.3),(A.2)+(B.1.3)+(C.2.3),(A.1)+(B.1.4)+(C.2.3),(A.2)+(B.1.4)+(C.2.3),(A.1)+(B.1.5)+(C.2.3),(A.2)+(B.1.5)+(C.2.3),(A.1)+(B.1.6)+(C.2.3),(A.2)+(B.1.6)+(C.2.3),(A.1)+(B.1.7)+(C.2.3),(A.2)+(B.1.7)+(C.2.3),(A.1)+(B.1.8)+(C.2.3),(A.2)+(B.1.8)+(C.2.3),(A.1)+(B.1.9)+(C.2.3),(A.2)+(B.1.9)+(C.2.3),(A.1)+(B.1.10)+(C.2.3),(A.2)+(B.1.10)+(C.2.3),(A.1)+(B.1.11)+(C.2.3),(A.2)+(B.1.11)+(C.2.3),
(A.1)+(B.2.1)+(C.2.3),(A.2)+(B.2.1)+(C.2.3)。
(A.1)+(B.1.1)+(C.3.3),(A.2)+(B.1.1)+(C.3.3),(A.1)+(B.1.2)+(C.3.3),(A.2)+(B.1.2)+(C.3.3),(A.1)+(B.1.3)+(C.3.3),(A.2)+(B.1.3)+(C.3.3),(A.1)+(B.1.4)+(C.3.3),(A.2)+(B.1.4)+(C.3.3),(A.1)+(B.1.5)+(C.3.3),(A.2)+(B.1.5)+(C.3.3),(A.1)+(B.1.6)+(C.3.3),(A.2)+(B.1.6)+(C.3.3),(A.1)+(B.1.7)+(C.3.3),(A.2)+(B.1.7)+(C.3.3),(A.1)+(B.1.8)+(C.3.3),(A.2)+(B.1.8)+(C.3.3),(A.1)+(B.1.9)+(C.3.3),(A.2)+(B.1.9)+(C.3.3),(A.1)+(B.1.10)+(C.3.3),(A.2)+(B.1.10)+(C.3.3),(A.1)+(B.1.11)+(C.3.3),(A.2)+(B.1.11)+(C.3.3),
(A.1)+(B.2.1)+(C.3.3),(A.2)+(B.2.1)+(C.3.3)。
(A.1)+(B.1.1)+(C.3.4),(A.2)+(B.1.1)+(C.3.4),(A.1)+(B.1.2)+(C.3.4),(A.2)+(B.1.2)+(C.3.4),(A.1)+(B.1.3)+(C.3.4),(A.2)+(B.1.3)+(C.3.4),(A.1)+(B.1.4)+(C.3.4),(A.2)+(B.1.4)+(C.3.4),(A.1)+(B.1.5)+(C.3.4),(A.2)+(B.1.5)+(C.3.4),(A.1)+(B.1.6)+(C.3.4),(A.2)+(B.1.6)+(C.3.4),(A.1)+(B.1.7)+(C.3.4),(A.2)+(B.1.7)+(C.3.4),(A.1)+(B.1.8)+(C.3.4),(A.2)+(B.1.8)+(C.3.4),(A.1)+(B.1.9)+(C.3.4),(A.2)+(B.1.9)+(C.3.4),(A.1)+(B.1.10)+(C.3.4),(A.2)+(B.1.10)+(C.3.4),(A.1)+(B.1.11)+(C.3.4),(A.2)+(B.1.11)+(C.3.4),
(A.1)+(B.2.1)+(C.3.4),(A.2)+(B.2.1)+(C.3.4)。
(A.1)+(B.1.1)+(C.3.5),(A.2)+(B.1.1)+(C.3.5),(A.1)+(B.1.2)+(C.3.5),(A.2)+(B.1.2)+(C.3.5),(A.1)+(B.1.3)+(C.3.5),(A.2)+(B.1.3)+(C.3.5),(A.1)+(B.1.4)+(C.3.5),(A.2)+(B.1.4)+(C.3.5),(A.1)+(B.1.5)+(C.3.5),(A.2)+(B.1.5)+(C.3.5),(A.1)+(B.1.6)+(C.3.5),(A.2)+(B.1.6)+(C.3.5),(A.1)+(B.1.7)+(C.3.5),(A.2)+(B.1.7)+(C.3.5),(A.1)+(B.1.8)+(C.3.5),(A.2)+(B.1.8)+(C.3.5),(A.1)+(B.1.9)+(C.3.5),(A.2)+(B.1.9)+(C.3.5),(A.1)+(B.1.10)+(C.3.5),(A.2)+(B.1.10)+(C.3.5),(A.1)+(B.1.11)+(C.3.5),(A.2)+(B.1.11)+(C.3.5),
(A.1)+(B.2.1)+(C.3.5),(A.2)+(B.2.1)+(C.3.5)。
(A.1)+(B.1.1)+(C.3.6),(A.2)+(B.1.1)+(C.3.6),(A.1)+(B.1.2)+(C.3.6),(A.2)+(B.1.2)+(C.3.6),(A.1)+(B.1.3)+(C.3.6),(A.2)+(B.1.3)+(C.3.6),(A.1)+(B.1.4)+(C.3.6),(A.2)+(B.1.4)+(C.3.6),(A.1)+(B.1.5)+(C.3.6),(A.2)+(B.1.5)+(C.3.6),(A.1)+(B.1.6)+(C.3.6),(A.2)+(B.1.6)+(C.3.6),(A.1)+(B.1.7)+(C.3.6),(A.2)+(B.1.7)+(C.3.6),(A.1)+(B.1.8)+(C.3.6),(A.2)+(B.1.8)+(C.3.6),(A.1)+(B.1.9)+(C.3.6),(A.2)+(B.1.9)+(C.3.6),(A.1)+(B.1.10)+(C.3.6),(A.2)+(B.1.10)+(C.3.6),(A.1)+(B.1.11)+(C.3.6),(A.2)+(B.1.11)+(C.3.6),
(A.1)+(B.2.1)+(C.3.6),(A.2)+(B.2.1)+(C.3.6)。
(A.1)+(B.1.1)+(C.3.10),(A.2)+(B.1.1)+(C.3.10),(A.1)+(B.1.2)+(C.3.10),(A.2)+(B.1.2)+(C.3.10),(A.1)+(B.1.3)+(C.3.10),(A.2)+(B.1.3)+(C.3.10),(A.1)+(B.1.4)+(C.3.10),(A.2)+(B.1.4)+(C.3.10),(A.1)+(B.1.5)+(C.3.10),(A.2)+(B.1.5)+(C.3.10),(A.1)+(B.1.6)+(C.3.10),(A.2)+(B.1.6)+(C.3.10),(A.1)+(B.1.7)+(C.3.10),(A.2)+(B.1.7)+(C.3.10),(A.1)+(B.1.8)+(C.3.10),(A.2)+(B.1.8)+(C.3.10),(A.1)+(B.1.9)+(C.3.10),(A.2)+(B.1.9)+(C.3.10),(A.1)+(B.1.10)+(C.3.10),(A.2)+(B.1.10)+(C.3.10),(A.1)+(B.1.11)+(C.3.10),(A.2)+(B.1.11)+(C.3.10),
(A.1)+(B.2.1)+(C.3.10),(A.2)+(B.2.1)+(C.3.10)。
(A.1)+(B.1.1)+(C.4.2),(A.2)+(B.1.1)+(C.4.2),(A.1)+(B.1.2)+(C.4.2),(A.2)+(B.1.2)+(C.4.2),(A.1)+(B.1.3)+(C.4.2),(A.2)+(B.1.3)+(C.4.2),(A.1)+(B.1.4)+(C.4.2),(A.2)+(B.1.4)+(C.4.2),(A.1)+(B.1.5)+(C.4.2),(A.2)+(B.1.5)+(C.4.2),(A.1)+(B.1.6)+(C.4.2),(A.2)+(B.1.6)+(C.4.2),(A.1)+(B.1.7)+(C.4.2),(A.2)+(B.1.7)+(C.4.2),(A.1)+(B.1.8)+(C.4.2),(A.2)+(B.1.8)+(C.4.2),(A.1)+(B.1.9)+(C.4.2),(A.2)+(B.1.9)+(C.4.2),(A.1)+(B.1.10)+(C.4.2),(A.2)+(B.1.10)+(C.4.2),(A.1)+(B.1.11)+(C.4.2),(A.2)+(B.1.11)+(C.4.2),
(A.1)+(B.2.1)+(C.4.2),(A.2)+(B.2.1)+(C.4.2)。
(A.1)+(B.1.1)+(C.4.3),(A.2)+(B.1.1)+(C.4.3),(A.1)+(B.1.2)+(C.4.3),(A.2)+(B.1.2)+(C.4.3),(A.1)+(B.1.3)+(C.4.3),(A.2)+(B.1.3)+(C.4.3),(A.1)+(B.1.4)+(C.4.3),(A.2)+(B.1.4)+(C.4.3),(A.1)+(B.1.5)+(C.4.3),(A.2)+(B.1.5)+(C.4.3),(A.1)+(B.1.6)+(C.4.3),(A.2)+(B.1.6)+(C.4.3),(A.1)+(B.1.7)+(C.4.3),(A.2)+(B.1.7)+(C.4.3),(A.1)+(B.1.8)+(C.4.3),(A.2)+(B.1.8)+(C.4.3),(A.1)+(B.1.9)+(C.4.3),(A.2)+(B.1.9)+(C.4.3),(A.1)+(B.1.10)+(C.4.3),(A.2)+(B.1.10)+(C.4.3),(A.1)+(B.1.11)+(C.4.3),(A.2)+(B.1.11)+(C.4.3),
(A.1)+(B.2.1)+(C.4.3),(A.2)+(B.2.1)+(C.4.3)。
(A.1)+(B.1.1)+(C.4.5),(A.2)+(B.1.1)+(C.4.5),(A.1)+(B.1.2)+(C.4.5),(A.2)+(B.1.2)+(C.4.5),(A.1)+(B.1.3)+(C.4.5),(A.2)+(B.1.3)+(C.4.5),(A.1)+(B.1.4)+(C.4.5),(A.2)+(B.1.4)+(C.4.5),(A.1)+(B.1.5)+(C.4.5),(A.2)+(B.1.5)+(C.4.5),(A.1)+(B.1.6)+(C.4.5),(A.2)+(B.1.6)+(C.4.5),(A.1)+(B.1.7)+(C.4.5),(A.2)+(B.1.7)+(C.4.5),(A.1)+(B.1.8)+(C.4.5),(A.2)+(B.1.8)+(C.4.5),(A.1)+(B.1.9)+(C.4.5),(A.2)+(B.1.9)+(C.4.5),(A.1)+(B.1.10)+(C.4.5),(A.2)+(B.1.10)+(C.4.5),(A.1)+(B.1.11)+(C.4.5),(A.2)+(B.1.11)+(C.4.5),
(A.1)+(B.2.1)+(C.4.5),(A.2)+(B.2.1)+(C.4.5)。
(A.1)+(B.1.1)+(C.4.6),(A.2)+(B.1.1)+(C.4.6),(A.1)+(B.1.2)+(C.4.6),(A.2)+(B.1.2)+(C.4.6),(A.1)+(B.1.3)+(C.4.6),(A.2)+(B.1.3)+(C.4.6),(A.1)+(B.1.4)+(C.4.6),(A.2)+(B.1.4)+(C.4.6),(A.1)+(B.1.5)+(C.4.6),(A.2)+(B.1.5)+(C.4.6),(A.1)+(B.1.6)+(C.4.6),(A.2)+(B.1.6)+(C.4.6),(A.1)+(B.1.7)+(C.4.6),(A.2)+(B.1.7)+(C.4.6),(A.1)+(B.1.8)+(C.4.6),(A.2)+(B.1.8)+(C.4.6),(A.1)+(B.1.9)+(C.4.6),(A.2)+(B.1.9)+(C.4.6),(A.1)+(B.1.10)+(C.4.6),(A.2)+(B.1.10)+(C.4.6),(A.1)+(B.1.11)+(C.4.6),(A.2)+(B.1.11)+(C.4.6),
(A.1)+(B.2.1)+(C.4.6),(A.2)+(B.2.1)+(C.4.6)。
(A.1)+(B.1.1)+(C.5),(A.2)+(B.1.1)+(C.5),(A.1)+(B.1.2)+(C.5),(A.2)+(B.1.2)+(C.5),(A.1)+(B.1.3)+(C.5),(A.2)+(B.1.3)+(C.5),(A.1)+(B.1.4)+(C.5),(A.2)+(B.1.4)+(C.5),(A.1)+(B.1.5)+(C.5),(A.2)+(B.1.5)+(C.5),(A.1)+(B.1.6)+(C.5),(A.2)+(B.1.6)+(C.5),(A.1)+(B.1.7)+(C.5),(A.2)+(B.1.7)+(C.5),(A.1)+(B.1.8)+(C.5),(A.2)+(B.1.8)+(C.5),(A.1)+(B.1.9)+(C.5),(A.2)+(B.1.9)+(C.5),(A.1)+(B.1.10)+(C.5),(A.2)+(B.1.10)+(C.5),(A.1)+(B.1.11)+(C.5),(A.2)+(B.1.11)+(C.5),
(A.1)+(B.2.1)+(C.5),(A.2)+(B.2.1)+(C.5)。
甚至更优选以下结合物:
(A.1)+(B.1.1)+(C.1.1),(A.2)+(B.1.1)+(C.1.1),(A.1)+(B.1.2)+(C.1.1),(A.2)+(B.1.2)+(C.1.1),(A.1)+(B.1.3)+(C.1.1),(A.2)+(B.1.3)+(C.1.1),(A.1)+(B.1.4)+(C.1.1),(A.2)+(B.1.4)+(C.1.1),(A.1)+(B.1.5)+(C.1.1),(A.2)+(B.1.5)+(C.1.1),
(A.1)+(B.2.1)+(C.1.1),(A.2)+(B.2.1)+(C.1.1)。
(A.1)+(B.1.1)+(C.1.2),(A.2)+(B.1.1)+(C.1.2),(A.1)+(B.1.2)+(C.1.2),(A.2)+(B.1.2)+(C.1.2),(A.1)+(B.1.3)+(C.1.2),(A.2)+(B.1.3)+(C.1.2),(A.1)+(B.1.4)+(C.1.2),(A.2)+(B.1.4)+(C.1.2),(A.1)+(B.1.5)+(C.1.2),(A.2)+(B.1.5)+(C.1.2),
(A.1)+(B.2.1)+(C.1.2),(A.2)+(B.2.1)+(C.1.2)。
(A.1)+(B.1.1)+(C.1.3),(A.2)+(B.1.1)+(C.1.3),(A.1)+(B.1.2)+(C.1.3),(A.2)+(B.1.2)+(C.1.3),(A.1)+(B.1.3)+(C.1.3),(A.2)+(B.1.3)+(C.1.3),(A.1)+(B.1.4)+(C.1.3),(A.2)+(B.1.4)+(C.1.3),(A.1)+(B.1.5)+(C.1.3),(A.2)+(B.1.5)+(C.1.3),
(A.1)+(B.2.1)+(C.1.3),(A.2)+(B.2.1)+(C.1.3)。
(A.1)+(B.1.1)+(C.2.1),(A.2)+(B.1.1)+(C.2.1),(A.1)+(B.1.2)+(C.2.1),(A.2)+(B.1.2)+(C.2.1),(A.1)+(B.1.3)+(C.2.1),(A.2)+(B.1.3)+(C.2.1),(A.1)+(B.1.4)+(C.2.1),(A.2)+(B.1.4)+(C.2.1),(A.1)+(B.1.5)+(C.2.1),(A.2)+(B.1.5)+(C.2.1),
(A.1)+(B.2.1)+(C.2.1),(A.2)+(B.2.1)+(C.2.1)。
(A.1)+(B.1.1)+(C.2.3),(A.2)+(B.1.1)+(C.2.3),(A.1)+(B.1.2)+(C.2.3),(A.2)+(B.1.2)+(C.2.3),(A.1)+(B.1.3)+(C.2.3),(A.2)+(B.1.3)+(C.2.3),(A.1)+(B.1.4)+(C.2.3),(A.2)+(B.1.4)+(C.2.3),(A.1)+(B.1.5)+(C.2.3),(A.2)+(B.1.5)+(C.2.3),
(A.1)+(B.2.1)+(C.2.3),(A.2)+(B.2.1)+(C.2.3)。
(A.1)+(B.1.1)+(C.3.3),(A.2)+(B.1.1)+(C.3.3),(A.1)+(B.1.2)+(C.3.3),(A.2)+(B.1.2)+(C.3.3),(A.1)+(B.1.3)+(C.3.3),(A.2)+(B.1.3)+(C.3.3),(A.1)+(B.1.4)+(C.3.3),(A.2)+(B.1.4)+(C.3.3),(A.1)+(B.1.5)+(C.3.3),(A.2)+(B.1.5)+(C.3.3),
(A.1)+(B.2.1)+(C.3.3),(A.2)+(B.2.1)+(C.3.3)。
(A.1)+(B.1.1)+(C.3.10),(A.2)+(B.1.1)+(C.3.10),(A.1)+(B.1.2)+(C.3.10),(A.2)+(B.1.2)+(C.3.10),(A.1)+(B.1.3)+(C.3.10),(A.2)+(B.1.3)+(C.3.10),(A.1)+(B.1.4)+(C.3.10),(A.2)+(B.1.4)+(C.3.10),(A.1)+(B.1.5)+(C.3.10),(A.2)+(B.1.5)+(C.3.10),
(A.1)+(B.2.1)+(C.3.10),(A.2)+(B.2.1)+(C.3.10)。
(A.1)+(B.1.1)+(C.4.5),(A.2)+(B.1.1)+(C.4.5),(A.1)+(B.1.2)+(C.4.5),(A.2)+(B.1.2)+(C.4.5),(A.1)+(B.1.3)+(C.4.5),(A.2)+(B.1.3)+(C.4.5),(A.1)+(B.1.4)+(C.4.5),(A.2)+(B.1.4)+(C.4.5),(A.1)+(B.1.5)+(C.4.5),(A.2)+(B.1.5)+(C.4.5),
(A.1)+(B.2.1)+(C.4.5),(A.2)+(B.2.1)+(C.4.5)。
(A.1)+(B.1.1)+(C.4.6),(A.2)+(B.1.1)+(C.4.6),(A.1)+(B.1.2)+(C.4.6),(A.2)+(B.1.2)+(C.4.6),(A.1)+(B.1.3)+(C.4.6),(A.2)+(B.1.3)+(C.4.6),(A.1)+(B.1.4)+(C.4.6),(A.2)+(B.1.4)+(C.4.6),(A.1)+(B.1.5)+(C.4.6),(A.2)+(B.1.5)+(C.4.6),
(A.1)+(B.2.1)+(C.4.6),(A.2)+(B.2.1)+(C.4.6)。
(A.1)+(B.1.1)+(C.5),(A.2)+(B.1.1)+(C.5),(A.1)+(B.1.2)+(C.5),(A.2)+(B.1.2)+(C.5),(A.1)+(B.1.3)+(C.5),(A.2)+(B.1.3)+(C.5),(A.1)+(B.1.4)+(C.5),(A.2)+(B.1.4)+(C.5),(A.1)+(B.1.5)+(C.5),(A.2)+(B.1.5)+(C.5),
(A.1)+(B.2.1)+(C.5),(A.2)+(B.2.1)+(C.5)。
最优选以下结合物:
(A.2)+(B1.1)
(A.2)+(B.1.1)+(C.1.1),(A.2)+(B.1.1)+(C.1.2),(A.2)+(B.1.1)+(C.1.3),(A.2)+(B.1.1)+(C.2.1),(A.2)+(B.1.1)+(C.2.3),(A.2)+(B.1.1)+(C.3.3),(A.2)+(B.1.1)+(C.3.10),(A.2)+(B.1.1)+(C.4.5),(A.2)+(B.1.1)+(C.4.6),A.2)+(B.1.1)+(C.5)。
以上提及的所有三元结合物可以与至少一种其他已知的杀细菌剂、杀真菌剂、杀螨剂、杀线虫剂、除草剂、杀昆虫剂、微量营养素和包含微量营养素的化合物、安全剂、脂壳寡糖化合物(LCO)、土壤改良产品或减少植物胁迫的产品(例如Myconate)结合,以例如扩大作用范围或阻止抗性发展。
优选地,以上提及的三元和四元结合物可进一步与至少一种化合物结合,所述化合物选自(A.1)苯并噻二唑、(A.2)异噻菌胺、(A.3)烯丙苯噻唑、(A.4)噻酰菌胺、(C.2.1)乙膦酸铝、(C.2.4)嘧菌酯、(C.2.3)肟菌酯、(C.3.3)吡虫啉、(C.3.4)噻虫啉、(C.3.5)氟氯氰菊酯、(C.3.6)溴氰菊酯、(C.3.10)flupyradifurone、(C.4.1)铜(Cu)、(C.4.2)氢氧化铜、(C.4.3)硫酸铜、(C.4.4)氧氯化铜、(C.4.5)丙森锌、(C.4.6)代森锰锌和(C.5)Myconate。
本发明所有已命名的结合物配对物(partner)以及宿主防御诱导剂能够——如果其官能团能实现这一点——任选地与合适的碱或酸形成盐。
此外,本发明的宿主防御诱导剂能够与至少一种活性化合物结合,所述活性化合物选自:
乙酸(例如,萘乙酸)、过乙酸、有机酸(例如,柠檬酸、乳酸)、氨基酸(例如,L-精氨酸)、腐植酸、富烯酸、硼酸、奥索利酸、1,2,3-苯并噻二唑-7-硫代羧酸-S-甲酯、5-羟基-1,4-萘二酮、溴-氯-二甲基乙内酰脲、三氯异氰尿酸、水杨酸、双氯酚、卡那霉素、春雷霉素、链霉素、硫酸链霉素、氧四环素、庆大霉素(例如,硫酸庆大霉素水合物)、吡虫啉、戊唑醇、噻菌灵、福美双、teracep、辛噻酮、苯氧喹啉、印楝素、呋喃黄酮、氯吡脲、植物矿物质(例如,钙、碳酸钙、次氯酸盐、EDTA钙)、酶(例如,蛋白酶、淀粉酶、脂酶)、痕量元素和螯合的痕量元素(例如,氨基酸螯合物)、维生素和植物提取物、水杨酸衍生物、生物黄酮和来自蔬菜和水果的有机酸、天然水果提取的多酚、苦橙皮油、柑橘提取物、壳聚糖、淀粉、海藻提取物、有机硅、有活性的离子化硅复合物蜂蜡、尿素、枯草芽孢杆菌、解淀粉芽孢杆菌、荧光假单胞菌、恶臭假单胞菌、成团泛菌、康氏木霉、哈茨木霉、氯和氯化合物(例如,经氯化的水、二氧化氯、亚氯酸钠、次氯酸钠、次氯酸、氯化铵、二癸基二甲基氯化铵、苯扎氯铵)、氧、过氧化氢(H2O2)和过氧化物、氰胺、硫酸镍(III)、过硫酸钠、亚磷酸盐、磷酸盐、磷酸三钠、磷酸、无机氮、银和包含银的化合物(例如,胶体银)、戊二醛、鼠李糖脂
其中,优选至少一种本发明的宿主防御诱导剂和至少一种其他化合物的结合物,所述其他化合物选自:
乙膦酸铝;strobilurins,其优选选自嘧菌酯和肟菌酯;以及如本文定义的微量营养素和包含微量营养素的化合物,其优选选自铜(Cu)、氢氧化铜、硫酸铜、氧氯化铜、丙森锌和代森锰锌。
在本文中以及在本发明的含义中,术语“结合物”或“制剂”意指分别如本文定义的至少一种宿主防御诱导剂与至少一种生物防治剂和任选的至少一种化合物(C)的多种结合物,其可以以例如预混物(ready mix)、桶混物(tank mix)(其被理解为意指由单独的活性化合物的制剂通过在施用前合并和稀释而制备的喷雾浆)或其组合(例如,通过使用第三种单一物质的制剂,将以上提及的活性化合物中的两种的二元预混物制成桶混物)的形式提供。
施用形式和处理方法
根据本发明,使用活性化合物的结合物或组合物对植物和植物部位的处理使用常规处理方法直接进行或通过使用常规处理方法作用于其环境、生境或贮存空间而进行,所述处理例如通过浸泡、喷雾、雾化、灌溉、蒸发、撒粉、成雾、播撒、发泡、涂布、分散、浇水(浸湿)、滴灌溉,并且在繁殖材料的情况下,特别是在种子的情况下,将所述活性化合物的结合物或组合物作为用于干燥种子处理的粉末、用于种子处理的溶液、用于浆体处理的水溶性粉末,通过包壳、通过包覆一层或多层包衣等来进行处理。优选通过浸泡、喷雾、雾化、灌溉、蒸发、撒粉、成雾、播撒、发泡、涂布、分散、浇水(浸湿)、滴灌溉来施用。本发明还包括培育箱处理。
本发明的处理可治疗性地以及预防性地实施。
根据本发明,单独的活性化合物也可按照几小时或几天的合理间隔依次地即一个接着一个地使用,在处理种子的情况下,例如也可通过施用多个包含不同活性化合物的层而使用。优选地,单独的活性化合物的施用次序是不重要的。
在本发明的一个特别优选的实施方案中,包含宿主防御诱导剂和生物防治剂的结合物或其制剂以待喷雾施用的溶液剂、乳剂或悬浮液形式施用,以处理营养繁殖材料;或被用于根茎或叶片施用。
根据其各自的物理和/或化学特性,可将本发明结合物的选择的化合物转化为常规制剂,例如溶液、乳剂、悬浮液、粉剂、泡沫剂、糊剂(paste)、颗粒剂、囊剂(sachet)、气雾剂、聚合物质中的微胶囊剂,以及ULV冷雾剂和ULV热雾剂。
这些制剂通过已知方法制备,例如通过将宿主防御诱导剂和/或生物防治剂和/或任选的其他化合物(C)任选地在使用表面活性剂即乳化剂和/或分散剂和/或泡沫形成剂(foam former)的情况下与增量剂即液体溶剂、增压的液化气体和/或固体载体混合。如果使用水作为增量剂,则还可例如使用有机溶剂作为助溶剂。合适的液体溶剂主要有:芳族化合物,例如二甲苯、甲苯或烷基萘;氯化的芳族化合物和氯化的脂族烃,例如氯苯、氯乙烯或二氯甲烷;脂族烃,例如环己烷或石蜡,例如矿物油馏分;醇类,例如丁醇或乙二醇及其醚和酯;酮类,例如丙酮、甲基乙基酮、甲基异丁基酮或环己酮;强极性溶剂,例如二甲基甲酰胺和二甲基亚砜,以及水;以及矿物油、动物油和植物油,例如棕榈油和其他植物种子油。液化气体增量剂或载体被理解为意指在标准温度和标准压力下是气态的那些液体,例如气溶胶喷射剂,例如卤代烃,以及丁烷、丙烷、氮气和二氧化碳。
合适的固体载体是:例如,磨碎的天然矿物,如高岭土、粘土、滑石、白垩、石英、绿坡缕石、蒙脱石或硅藻土,以及磨碎的合成矿物质,如细分散的二氧化硅、矾土和硅酸盐。适用于颗粒剂的固体载体是:例如,压碎或分级的天然矿物质,例如方解石、浮石、大理石、海泡石、白云石,以及无机和有机粉料(meal)的合成颗粒,以及有机材料如锯屑、椰子壳、玉米穗轴和烟草秸秆的颗粒。合适的乳化剂和/或泡沫形成剂是,例如,非离子、阳离子和阴离子乳化剂,如聚氧化乙烯脂肪酸酯、聚氧化乙烯脂肪醇醚,例如烷基芳基聚乙二醇醚、烷基磺酸酯、烷基硫酸酯、芳基磺酸酯和蛋白水解产物。合适的分散剂是:例如,木质素亚硫酸盐废液和甲基纤维素。
在制剂中可使用胶粘剂,如羧甲基纤维素;粉状、颗粒状或胶乳状的天然或合成聚合物,例如阿拉伯树胶、聚乙烯醇、聚乙酸乙烯酯,以及天然磷脂,例如脑磷脂和卵磷脂,以及合成磷脂。其他胶粘剂可以是矿物油或植物油。
可使用着色剂,例如无机颜料,如氧化铁、氧化钛、普鲁士蓝;和有机染料,如茜素染料、偶氮染料、金属酞菁染料;以及痕量营养物,如铁盐、锰盐、硼盐、铜盐、钴盐、钼盐和锌盐。
通常,所述制剂包含0.1重量%至95重量%的活性化合物(宿主防御诱导剂、生物防治剂和/或化合物(C)),优选0.5重量%至90重量%的活性化合物。
通过处理植物的营养繁殖材料来防治选择的细菌性有害生物已被了解很长一段时间,并且是持续改进的主题。但是,营养繁殖材料处理仍涉及到一系列无法以令人满意的方式解决的问题。因此,有必要开发保护营养繁殖材料和发芽植物的方法,所述方法免去、或至少显著减少种植后或植物出苗后额外施用作物保护产品。此外,有必要优化所使用的活性化合物的量,以为营养繁殖材料和发芽植物提供尽可能好的保护,使其免受细菌性有害生物的侵袭,但所使用的活性化合物不会对植物本身造成损害。特别地,处理营养繁殖材料的方法还应该考虑转基因植物固有的特性,以实现对营养繁殖材料和发芽植物的最优保护,同时保持尽可能低的植物保护产品施用率。
因此,本发明还特别涉及通过用本发明的化合物或制剂处理种子和营养繁殖材料来保护营养繁殖材料和发芽植物免受选择的细菌性有害生物的侵袭的方法。
本发明还涉及本发明的化合物用于处理营养繁殖材料以保护营养繁殖材料和发芽植物免受选择的细菌性有害生物的侵袭的用途。
本发明的优势之一是,由于本发明化合物特有的内吸特性,使用这些化合物处理营养繁殖材料不仅保护营养繁殖材料本身,还保护其在种植后长出的植物免受细菌性有害生物的侵袭。通过这种方式,可免去在种植时或之后不久立即处理作物。
另一个优势是,本发明的化合物还可特别用于转基因营养繁殖材料。
本发明的化合物适用于保护农业、温室、森林或园艺中使用的任何植物品种的营养繁殖材料。特别是本文所定义并优选的植物的营养繁殖材料。
在本发明的范围内,将本发明的化合物单独或以合适的制剂的形式施用到营养繁殖材料。优选在营养繁殖材料处于足够稳定的状态下对其进行处理,以使在处理过程中不产生损害。通常可在采收和种植之间的任何时间点处理营养繁殖材料。通常使用已与植物分离并且去除穗轴、壳、秸秆、包衣、绒毛或果肉的营养繁殖材料。
处理营养繁殖材料时,通常必须注意的是,对施用到营养繁殖材料的本发明的化合物或制剂和/或其他添加剂的量进行选择,使营养繁殖材料的发芽不会受到不利影响,或使其长出的植物不受损害。特别是在一定施用率下活性化合物可具有植物毒性效应的情况下,必须考虑这个问题。
可直接施用本发明的化合物或制剂,即不包含其他成分并且不进行稀释。通常优选以合适的制剂形式将化合物或制剂施用于营养繁殖材料。用于处理种子和营养繁殖材料的合适的制剂和方法对技术人员而言是已知的。
根据本发明使用的化合物或制剂可转化为常规制剂,如溶液、乳剂、悬浮液、粉剂、泡沫和ULV制剂。
通过将宿主防御诱导剂、生物防治剂和任选的化合物(C)与常规添加剂混合用已知方法制备这些制剂,所述常规添加剂为例如常规增量剂,以及溶剂或稀释剂、着色剂、润湿剂、分散剂、乳化剂、消泡剂、防腐剂、二次增稠剂、胶粘剂、赤霉素、矿物油和植物油,以及水。
可存在于可根据本发明使用的制剂中的着色剂为常规用于此目的的所有着色剂。在本文中,可使用微溶于水的颜料和溶于水的染料。可提及的实例是已知的命名为若丹明B(Rhodamine B)、C.I.颜料红112和C.I.溶剂红1的着色剂。
可存在于可根据本发明使用的制剂中的润湿剂为常规用于配制农业化学活性化合物且促进润湿的所有物质。优选使用烷基萘磺酸酯,如二异丙基萘磺酸酯或二异丁基萘磺酸酯。
可存在于可根据本发明使用的制剂中的适合的分散剂和/或乳化剂是常规用于农业化学活性化合物制剂中的所有非离子、阴离子或阳离子分散剂。优选使用以下非离子或阴离子分散剂,或非离子或阴离子分散剂的混合物。可提及的合适的非离子分散剂特别是环氧乙烷-环氧丙烷嵌段聚合物、烷基酚聚乙二醇醚和三苯乙烯基酚聚乙二醇醚,及其磷酸化或硫酸化衍生物。合适的阴离子分散剂特别为木素磺酸盐、聚丙烯酸盐和芳基磺酸盐/甲醛缩合物。
可存在于可根据本发明使用的制剂中的消泡剂是常规用于农业化学活性化合物制剂中的所有泡沫抑制物质。可优选使用有机硅消泡剂和硬脂酸镁。
可存在于可根据本发明使用的制剂中的防腐剂包括可在农业化学组合物中用于此目的的所有物质。可提及的实例为二氯苯和苄醇半缩甲醛。
可存在于可根据本发明使用的制剂中的二次增稠剂是在农业化学组合物中可以用于此目的的所有物质。优选纤维素衍生物、丙烯酸衍生物、黄原胶、改性粘土以及高度分散的二氧化硅。
可存在于可根据本发明使用的制剂中的胶粘剂包括可用于媒染剂(mordant)的所有常规粘合剂。优选提及聚乙烯基吡咯烷酮、聚乙酸乙烯酯、聚乙烯醇和甲基纤维素。
可存在于可根据本发明使用的制剂中的赤霉素可优选赤霉素A1、赤霉素A3(赤霉酸)、赤霉素A4和赤霉素A7。特别优选使用赤霉酸。
赤霉素是已知的(参见R.Wegler,“Chemie der Pflanzenschutz-und”[Chemistry of plant protection and pesticide agents],第2卷,Springer Verlag,Berlin-Heidelberg-New York,1970,第401-412页)。
可根据本发明使用的制剂可以直接使用或先用水稀释后用于处理多种类型的种子。因此,浓缩液或可由其通过用水稀释而获得的制剂可用于拌种。可根据本发明使用的制剂或其稀释制剂也可用于处理转基因植物的营养繁殖材料。在此情况下,额外的协同作用也可在结合通过表达形成的物质的情况下发生。
可根据本发明使用的制剂的施用率可在大范围内变化。施用率取决于制剂中各种活性化合物的含量,以及取决于营养繁殖材料。通常,活性化合物的施用率为0.001-50克/千克营养繁殖材料,优选0.01-15克/千克营养繁殖材料。
本发明的结合物可以以本身形式、其制剂形式或由其制备的使用形式使用,所述使用形式为例如即用型溶液、悬浮液、可湿性粉剂、糊剂、可溶性粉剂、粉剂和颗粒剂。其以常规方法进行施用,例如通过灌注、喷雾、雾化、播撒、撒粉、发泡、涂布等施用。此外,还可以通过超低容量法来施用本发明的化合物或制剂,或将活性化合物制剂或活性化合物本身注射进土壤中。还可以处理植物的营养繁殖材料。
根据施用类型,施用率可以在大范围内变化。在植物部位的处理中,活性化合物的施用率通常为0.1-10000g/ha,优选10-1000g/ha。在营养繁殖材料的处理中,活性化合物的施用率通常为0.001-50克/千克营养繁殖材料,优选0.01-10克/千克营养繁殖材料。在土壤处理中,活性化合物的施用率通常为0.1-10000g/ha,优选1-5000g/ha。
本发明还涉及试剂盒结合物,其包括协同有效量的
(A)至少一种如本文所定义的宿主防御诱导剂,
(B)至少一种如本文所定义的生物防治剂,以及
(C)任选的至少一种如本文所定义的其他化合物,
用于防治有用植物中的细菌性有害生物。
这样的试剂盒包含空间上分开放置的各组分。其中,所有组分可以在空间上彼此分开,如通过A/B、A/B/C、A/A’/B/C说明(例如在包含作为宿主防御诱导剂(A)的异噻菌胺和苯并噻二唑的结合物的优选实施方案的情况下)。还可能的是,至少两种组分以混合物形式存在并且在空间上与至少一种其他组分或混合物分开,例如通过A+B/C、A+C/B、B+C/A、A+A’/B/C、A/A’+B/C、A/B/C+A’、A+B/A’/C、A/A’/B+C、A+A’/B+C等说明(各种结合相应地适用于包含至少两种生物防治剂B和B’或至少两种其他化合物C和C’等的结合物的实施方案)。在施用至植物之前,可以将至少两种空间上分开的组分或两种组分的混合物与空间上分开的第三种组分(或其他混合物)混合。或者,如本文所述的空间上分开的组分可单独使用并且在如下文定义的单独的依次处理区段中依次施用。
本发明的活性化合物制剂包含有效且非植物毒性量的活性成分,表述“有效且非植物毒性量”意指下述本发明的成分或活性结合物的量,所述量通过显著避免针对活性成分的抗性菌株的发展而足以防治或消灭存在于或易于出现在植物上的致病细菌性生物,并且在各种情况下对所述作物不产生任何明显的植物毒性症状。根据待抵抗的病原体或所防治的细菌、作物类型、气候条件和包含在本发明的杀细菌结合物中的化合物,这种量可以在宽范围内变化。所述量可通过系统的田间试验测定,所述试验在本领域技术人员的能力范围内。
因此,本发明还涉及防治有用植物中的细菌性有害生物的方法,其包括使用包含如本文定义的(A)至少一种宿主防御诱导剂和如本文定义的(B)至少一种生物防治剂和任选的如本文定义的至少一种化合物(C)的结合物处理植物。
本发明的一个优选实施方案涉及防治有用植物中的细菌性有害生物的方法,所述方法包括对待保护以免受细菌性有害生物侵袭的植物进行两个以上的依次处理区段,优选2、3或4个依次处理区段,其中至少一个处理区段包括用如本文定义的至少一种宿主防御诱导剂(A)对植物进行至少一次处理,并且至少一个处理区段包括用如本文定义的至少一种生物防治剂(B)对植物进行至少一次处理。本发明的一个甚至更优选的实施方案涉及防治有用植物中的细菌性有害生物的方法,所述方法包括对待保护以免受细菌性有害生物侵袭的植物进行两个以上的依次处理区段,优选2、3或4个依次处理区段,其中至少一个处理区段包括用如本文定义的至少一种宿主防御诱导剂(A)对植物进行至少一次处理,并且至少一个处理区段包括用如本文定义的至少一种生物防治剂(B)对植物进行至少一次处理,条件是最后一个处理区段包括使用至少一种生物防治剂对植物进行至少一次处理。
在本发明的含义内,“处理区段”是指包括一次或多次施用至少一种宿主防御诱导剂(A)或至少一种生物防治剂(B)的处理步骤。不同的处理区段通过所使用的活性化合物类型(一个处理区段包括施用至少一种宿主防御诱导剂或至少一种生物防治剂)和时间(即不同的处理区段不重叠)来区分。但是,如果有多于两个处理区段,则一个处理区段可包括用至少一种宿主防御诱导剂和至少一种生物防治剂进行的结合处理,其例如通过施用至少一种宿主防御诱导剂和至少一种生物防治剂的混合物而进行。优选地,如果有多于两个处理区段,则一个处理区段可包括用至少一种宿主防御诱导剂和至少一种生物防治剂进行的结合处理,其例如通过施用至少一种宿主防御诱导剂和至少一种生物防治剂的混合物而进行,条件是最后一个处理区段包括用至少一种生物防治剂(而非宿主防御诱导剂)对植物进行至少一次处理。然而,优选的是,处理区段不包括用至少一种宿主防御诱导剂和至少一种生物防治剂进行的结合处理;换言之,优选的是,每个处理区段包括要么施用至少一种宿主防御诱导剂,要么施用至少一种生物防治剂。
“最后一个”处理区段是在一个时期中,例如,在采收(作物处理)之前、期间或最晚之后,或在植物死亡之前(在一年生植物的情况下),成为最后一个宿主防御诱导剂处理区段的处理区段。
优选地,本发明的方法包括两个处理区段。因此,本发明优选涉及防治细菌性有害生物的方法,所述方法包括对待保护以免受植物致病细菌侵袭的植物进行两个依次处理区段,其中第一个处理区段包括用至少一种宿主防御剂对植物进行至少一次处理,且随后的第二个处理区段包括用至少一种生物防治剂对植物进行至少一次处理。在包括用至少一种宿主防御诱导剂对植物进行至少一次处理的处理区段中,不施用生物防治剂。在包括用至少一种生物防治剂对植物进行至少一次处理的处理区段中,不施用宿主防御诱导剂。在本发明的方法中,仅在前个处理区段完成后进行处理区段,即仅在第一个处理区段完成后进行第二个处理区段,如果存在第三个处理区段,则仅在第二个处理区段完成后进行第三个处理区段,等等。
优选地,在植物的不同生长阶段期间进行各处理区段。换言之,随后的处理区段之间的时间间隔优选使得当对植物进行各处理区段时植物处于不同的生长阶段,即在植物的不重叠的生长阶段中进行第一个、第二个等处理区段,第一个处理区段当然在比第二个处理区段更早的生长阶段进行,等等。在其中所述方法包括两个处理区段的本发明的优选实施方案的情况下,优选第一个和第二个处理区段之间的时间间隔使得当对植物分别进行第一个和第二个处理区段时植物处于不同的生长阶段,即优选在植物不重叠的生长阶段中进行第一个和第二个处理区段,当然在更早的生长阶段进行第一个处理区段。
本文使用的术语“生长阶段”是指根据BBCH扩充版(extended scale)(BBCH Makrostadien;Biologische Bundesanstalt fur Land-und Forstwirtschaft[BBCH Macrostages;德国联邦农林生物研究中心(German Federal BiologicalResearch Center for Agriculture and Forestry)];参见www.bba.de/veroeff/bbch/bbcheng.pdf)的生长阶段。
优选地,第一个处理区段最晚在植物达到根据BBCH扩充版的生长阶段81时结束,最后一个处理区段最早在植物处于根据BBCH扩充版的生长阶段41时开始。正如已经指出的,随后的区段始终且必须在前一个区段完成后进行;这意味着例如,如果当植物处于生长阶段81时完成第一个处理区段,则仅在第一个区段完成后、优选最早在生长阶段82进行第二个处理区段。最适合的处理时间点尤其取决于待处理的植物。
在其中所述方法包括两个处理区段的本发明的优选实施方案中,优选第一个处理区段最晚在植物达到生长阶段81时结束,且第二个处理区段最早在植物处于生长阶段41时开始。正如已经指出的,第二个区段始终且必须在第一个区段完成后进行;这意味着例如,如果当植物处于生长阶段81时完成第一个处理区段,则仅在第一个区段完成后、优选最早在生长阶段82进行第二个处理区段。最适合的处理时间点尤其取决于待处理的植物。
更优选地,第一个处理区段最晚在植物达到生长阶段79时结束,且最后一个处理区段(其优选为第二个处理区段)最早在植物处于生长阶段41时开始。甚至更优选地,当植物处于生长阶段01至79、优选10至79时进行第一个处理区段,且当植物处于生长阶段41至92时或甚至在采收后(即41至99)进行最后一个处理区段(其优选为第二个处理区段)。最适合的处理时间点尤其取决于待处理的植物。以下给出了具体植物的更具体的信息。
在下文中,举例来说,汇编了具体植物和各自的优选两个处理区段的优选时间间隔:
*GS=生长阶段
在一个具体的实施方案中,包括用至少一种宿主防御诱导剂处理的所有处理区段最晚在各植物的营养期结束时结束。换言之,在该具体的实施方案中,在营养期结束之后不使用宿主防御诱导剂处理植物。在该具体的实施方案中,用至少一种生物防治剂的处理步骤在营养期之后的采收期前进行。在其中使用至少一种宿主防御诱导剂的处理区段中,其被施用至少一次,例如1、2、3、4、5、6、7或8次,优选1、2、3、4或5次。施用频率尤其取决于病原体压力和/或气候条件。例如,促进细菌侵袭和繁殖的天气条件如极端潮湿可能比干燥和炎热天气需要更多次施用至少一种宿主防御诱导剂。如果宿主防御诱导剂的施用多于一次,则单次施用之间的时间间隔尤其取决于害虫压力、待处理的植物、天气条件,并且可由技术人员确定。通常,施用频率以及施用率对应于给定条件下各植物和各宿主防御诱导剂的常规施用频率以及施用率,除了在特定的生长阶段之后用生物防治剂处理代替宿主防御诱导剂处理。如果至少一种宿主防御诱导剂的施用多于一次,则可在不同的生长阶段进行这些施用。
在本发明的方法中,根据所使用的宿主防御诱导剂的类型,至少一种宿主防御诱导剂的单次施用率为0.0001-7kg/ha,优选0.005-5kg/ha,更优选0.05-2kg/ha。
在其中使用至少一种生物防治剂的处理区段中,其被施用至少一次,例如1、2、3、4、5、6、7或8次,优选1、2、3、4、5或6次,更优选1、2、3或4次,甚至更优选2、3或4次,特别是2或3次。类似于施用宿主防御诱导剂的情况,生物防治剂的施用频率尤其取决于病原体压力和/或气候条件。例如,促进细菌侵袭和繁殖的天气条件如极端潮湿可能比干燥和炎热天气需要更多次施用生物防治剂。如果生物防治剂的施用多于一次,则单次施用之间的时间间隔尤其取决于害虫压力、待处理的植物、天气条件等,并且可由技术人员确定。通常,施用频率以及施用率对应于给定条件下各植物和各生物防治剂的常规施用频率以及施用率,除了仅在植物达到特定的生长时期之后并且在用宿主防御诱导剂处理完成之后才开始用生物防治剂处理。如果生物防治剂的施用多于一次,则可在不同的生长阶段进行这些施用。
本发明的另一优选方法包括对植物进行本文所述的两个以上的依次处理区段并进一步用本文定义的至少一种化合物(C)进行至少一次处理。本发明的甚至更优选的方法包括对植物进行本文所述的两个以上的依次处理区段并进一步用本文定义的至少一种化合物(C)进行至少一次处理,条件是最后一个处理区段包括用至少一种生物防治剂和任选的至少一种其他化合物(C)对植物进行至少一次处理。在所述实施方案中,生物防治剂不一定在宿主防御诱导剂之后施用,而是可在至少一种其他化合物(C)之后施用。具体而言,可以以任何次序施用三种组分(A)、(B)和(C),且其中各自具有任何不同的重复处理次数。更优选地,可以以任何次序施用三种组分(A)、(B)和(C),且其中各自具有任何不同的重复处理次数,条件是最后一个(最终)处理区段包括用至少一种生物防治剂(而非宿主防御诱导剂和其他化合物(C))对植物进行至少一次处理。这意味着所述方法可包括化合物(A)、(B)和/或(C)的至少两个重复处理区段。通常,化合物(A)、(B)和/或(C)的施用频率以及施用率和重复次数对应于给定条件下各植物和各化合物(A)、(B)和(C)的常规施用频率以及施用率和重复次数,除了仅在植物达到特定的生长阶段之后并且在任何之前的处理区段的施用完成之后才开始用化合物(A)、(B)或(C)进行处理。如果化合物(A)、(B)和(C)的施用多于一次,则可在不同的生长阶段进行这些施用。
本文所述的方法全部包括转基因植物的处理。
根据本发明,当活性化合物结合物的活性超过活性化合物单独施用时的活性的总和时,则例如宿主防御诱导剂或生物防治剂的协同效应始终存在。可按照如下计算两种活性化合物的给定结合物(二元组合物)的预期活性:
其中E代表两种确定剂量(例如,分别等于x和y)的化合物的结合物抑制病害的预期百分数,x是所观察到的确定剂量(等于x)的化合物(A)抑制病害的百分数,y是所观察到的确定剂量(等于y)的化合物(B)抑制病害的百分数。当所观察到的结合物的抑制百分数大于E时,存在协同效应。
可按照如下计算三种活性化合物的给定结合物(三元结合物)的预期活性:
其中
X是以m ppm(或g/ha)的施用率施用活性化合物A时的功效,
Y是以n ppm(或g/ha)的施用率施用活性化合物B时的功效,
Z是以r ppm(或g/ha)的施用率施用活性化合物C时的功效,
E是分别以m、n和r ppm(或g/ha)的施用率施用活性化合物A、B和C时的功效。
以%表示功效的程度。0%意指相当于对照功效的功效,而100%功效意指未观察到病害。
如果实际活性超过计算值,则结合物的活性是超加和的,即存在协同效应。在这种情况下,实际观察到的功效一定大于由上述公式计算得到的预期功效(E)。
另一种表明协同效应的方法是Tammes法(参见“Isoboles,a graphic representation of synergism in pesticides”in Neth.J.Plant Path.,1964,70,73-80)。
本发明的一个优选实施方案涉及一种结合物在番茄中的用途,其中
(A)宿主防御诱导剂是异噻菌胺,
(B)生物防治剂选自
(1)由枯草芽孢杆菌菌株QST713/AQ713(NRRL登录号B21661)、枯草芽孢杆菌菌株AQ153(NRRL登录号55614)、芽孢杆菌属菌株AQ175(ATCC登录号55608)、芽孢杆菌属菌株AQ177(ATCC登录号55609),以及芽孢杆菌属菌株AQ178(ATCC登录号53522)组成的细菌;和
(2)由丁香假单胞菌番茄致病变种组成的细菌,并且
(C)至少一种其他化合物选自戊苯吡菌胺。
本发明的另一个优选的实施方案涉及一种结合物在马铃薯中作为种子处理的用途,其中
(A)宿主防御诱导剂是异噻菌胺,
(B)生物防治剂选自
(1)由枯草芽孢杆菌菌株QST713/AQ713(NRRL登录号B21661)、枯草芽孢杆菌菌株AQ153(NRRL登录号55614)、芽孢杆菌属菌株AQ175(ATCC登录号55608)、芽孢杆菌属菌株AQ177(ATCC登录号55609),以及芽孢杆菌属菌株AQ178(ATCC登录号53522)组成的细菌;和
(2)由疮痂病链霉菌组成的细菌,并且
(C)至少一种其他化合物选自戊苯吡菌胺。
实施例1:
在以下实施例中,本发明的活性化合物结合物的增加的抗细菌活性是显而易见的。尽管单独的活性化合物表现出弱的抗细菌活性,但是结合物具有超过活性简单加和的活性。
当活性化合物结合物的抗细菌活性超过活性化合物单独施用时的活性的总和时,杀细菌剂的协同效应始终存在。按照以上说明计算两种活性化合物的给定结合物的预期活性。
以%表示功效的程度。0%意指相当于对照功效的功效,而100%功效意指未观察到病害。
如果实际的抗细菌活性超过计算值,则结合物的活性是超加和的,即存在协同效应。在这种情况下,实际观察到的功效一定大于由上述公式计算得到的预期功效(E)。
通过以下实施例说明本发明。但是本发明不限于实施例。
实施例1:丁香假单胞菌番茄致病变种体内预防性试验(番茄)
溶剂:去离子水
试验化合物:异噻菌胺(SC200制剂),200/100/50g a.i./ha苯并噻二唑(Bion WG50),20/10/5g/ha Serenade Max(干燥的枯草芽孢杆菌QST 713菌株/WP/14.6%)6/3/1.2g/ha
为了测试预防性活性,用三种不同施用率的制备化合物喷洒植物幼株。施用一周后,用丁香假单胞菌番茄致病变种的水性悬浮液接种植物。将接种过的植物放置在温度为25℃、相对空气湿度为90%的温室中。
接种1周后评估试验。0%意指相当于未处理的对照功效的功效,而100%功效意指未观察到病害。
下表清楚地表明,所观察到的本发明的活性化合物结合物的活性大于计算活性,即存在协同效应。
表:对丁香假单胞菌番茄致病变种的体内预防性试验(番茄)
*实际值=实际活性
**计算值=使用Colby’s公式计算的活性
*实际值=实际活性
**计算值=使用Colby’s公式计算的活性
*实际值=实际活性
**计算值=使用Colby’s公式计算的活性
*实际值=实际活性
**计算值=使用Colby’s公式计算的活性
*实际值=实际活性
**计算值=使用Colby’s公式计算的活性
*实际值=实际活性
**计算值=使用Colby’s公式计算的活性
*实际值=实际活性
**计算值=使用Colby’s公式计算的活性
*实际值=实际活性
**计算值=使用Colby’s公式计算的活性
*实际值=实际活性
**计算值=使用Colby’s公式计算的活性
实施例2:对疮痂病链霉菌的体内预防性试验(种子生长试验)(马铃薯)
溶剂:水
测试化合物:异噻菌胺(FS200制剂),30/24/12ml/100kg马铃薯种子
戊苯吡菌胺(Emesto FS240制剂),10ml/100kg马铃薯种子
Serenade ASO(枯草芽孢杆菌QST 713菌株/SC/1.34%),5L/ha(200ml/播种100kg种子的面积)
为了测试与任选的其他杀真菌剂结合的异噻菌胺FS200和Serenade ASO SC的混合物的种子(块茎)处理活性,选择具有适当的疮痂病链霉菌感染的马铃薯块茎。使用总体积为1500ml/100kg种子的浆体,通过用手动背负式喷雾器喷洒在块茎上来处理种子。使用单独的异噻菌胺FS200以及与戊苯吡菌胺的桶混物进行种子处理。
在即将播种种子之前,将5000ml/ha的Serenade ASO SC 1.34%配制产品喷洒在犁沟中。将100kg种子播种在400m2面积上,并在该试验中使用200ml Serenade ASO配制产品。按照上述方法用异噻菌胺和任选的戊苯吡菌胺处理的种子与播种前Serenade ASO在犁沟中的土壤施用结合使用。该试验在天然田间条件的室内进行,并在采收时观察马铃薯上的疮痂病链霉菌感染。
在采收马铃薯作物时评估试验。0%意指相当于未处理的对照功效的功效,而100%功效意指未观察到病害。
下表清楚地表明,结合产物抵抗疮痂病的功效提高,同时“%等级”表明积极效应,即更大块茎的数量增加,其中异噻菌胺与Serenade和作为其他杀真菌剂的戊苯吡菌胺的结合物是特别有利的。
技术特征:
1.一种结合物用于防治有用植物中的细菌性有害生物的用途,所述结合物包含协同有效量的
(A)至少一种宿主防御诱导剂和
(B)至少一种生物防治剂,选自枯草芽孢杆菌菌株QST713/AQ713,NRRL登录号B21661;
其中,至少一种宿主防御诱导剂(A)选自苯并噻二唑、异噻菌胺;
其中,在植物部位的处理中,组分(A)和(B)的施用率为0.1-10000g/ha;在营养繁殖材料的处理中,组分(A)和(B)的施用率为0.001-50克/千克营养繁殖材料;且在土壤处理中,组分(A)和(B)的施用率为0.1-10 000g/ha,且
其中,细菌性有害生物选自假单胞菌属和链霉菌属。
2.根据权利要求1所述的用途,其中所述宿主防御诱导剂是异噻菌胺。
3.根据权利要求1所述的用途,其中所述有用植物选自苹果、香蕉、柑橘、猕猴桃、甜瓜、桃、梨、菠萝、仁果、石榴、甘蓝、菜花、黄瓜、葫芦、番茄、马铃薯、小麦、稻和大豆。
4.根据权利要求1所述的用途,用于防治番茄中的丁香假单胞菌番茄致病变种;马铃薯中的疮痂病链霉菌。
5.根据权利要求1所述的用途,其中包含(A)至少一种宿主防御诱导剂和(B)至少一种生物防治剂的结合物还包含至少一种化合物(C),其选自戊苯吡菌胺。
6.根据权利要求5所述的用途,其中
所述宿主防御诱导剂(A)是异噻菌胺,
所述生物防治剂(B)选自
枯草芽孢杆菌菌株QST713/AQ713,NRRL登录号B21661;
所述细菌性有害生物是丁香假单胞菌番茄致病变种或疮痂病链霉菌,并且
至少一种其他化合物(C)是戊苯吡菌胺。
7.根据权利要求6所述的用途,其中被处理的植物是番茄。
8.根据权利要求5所述的用途,其中
所述宿主防御诱导剂(A)是异噻菌胺,
所述生物防治剂(B)选自枯草芽孢杆菌菌株QST713/AQ713,NRRL登录号B21661,并且
至少一种其他化合物(C)选自戊苯吡菌胺。
9.根据权利要求8所述的用途,其中被处理的植物是马铃薯。
10.如权利要求1至9中任一项所表征的用于防治有用植物中的细菌性有害生物的用途,所述用途包括使用包含(A)至少一种宿主防御诱导剂和(B)至少一种生物防治剂和任选的权利要求5所定义的至少一种化合物(C)的结合物处理植物,
其中,至少一种宿主防御诱导剂(A)选自苯并噻二唑、异噻菌胺,至少一种生物防治剂(B)选自枯草芽孢杆菌菌株QST713/AQ713,NRRL登录号B21661;其中,在植物部位的处理中,组分(A)和(B)的施用率为0.1-10000g/ha;在营养繁殖材料的处理中,组分(A)和(B)的施用率为0.001-50克/千克营养繁殖材料;且在土壤处理中,组分(A)和(B)的施用率为0.1-10 000g/ha,
且其中,细菌性有害生物选自假单胞菌属和链霉菌。
11.用于防治有用植物中的细菌性有害生物的方法,所述方法包括对待保护以免受植物致病细菌侵袭的植物进行两个以上的依次处理区段,其中至少一个处理区段包括用前述权利要求中任一项所定义的至少一种宿主防御诱导剂(A)对植物进行至少一次处理,并且至少一个处理区段包括用前述权利要求中任一项所定义的至少一种生物防治剂(B)对植物进行至少一次处理,条件是最后一个处理区段包括用至少一种生物防治剂对植物进行至少一次处理,
其中,宿主防御诱导剂(A)选自苯并噻二唑、异噻菌胺,生物防治剂(B)选自枯草芽孢杆菌菌株QST713/AQ713,NRRL登录号B21661,
其中,在植物部位的处理中,组分(A)和(B)的施用率为0.1-10000g/ha;在营养繁殖材料的处理中,组分(A)和(B)的施用率为0.001-50克/千克营养繁殖材料;且在土壤处理中,组分(A)和(B)的施用率为0.1-10 000g/ha,且
其中,细菌性有害生物选自假单胞菌属和链霉菌属。
12.根据权利要求11所述的方法,还包括用权利要求5所定义的至少一种化合物(C)对植物进行至少一次处理,条件是最后一个处理区段包括用至少一种生物防治剂对植物进行至少一次处理。
13.根据权利要求11或12所述的方法,其中在植物的不同生长阶段期间进行各处理区段。
14.试剂盒,包括协同有效量的
(A)权利要求1或2所定义的至少一种宿主防御诱导剂,
(B)至少一种生物防治剂,其选自枯草芽孢杆菌菌株QST713/AQ713,NRRL登录号B21661,以及
(C)任选的权利要求5所定义的至少一种化合物,
用于防治有用植物中的细菌性有害生物,
其中,在植物部位的处理中,组分(A)和(B)的施用率为0.1-10000g/ha;在营养繁殖材料的处理中,组分(A)和(B)的施用率为0.001-50克/千克营养繁殖材料;且在土壤处理中,组分(A)和(B)的施用率为0.1-10 000g/ha,且
其中,细菌性有害生物选自假单胞菌属和链霉菌。
技术总结
本发明涉及包含协同有效量的至少一种宿主防御诱导剂和至少一种生物防治剂的结合物用于防治有用植物中的细菌性有害生物的用途。所述生物防治剂选自特定的微生物和/或具有各菌株的全部识别特征的这些菌株的突变体和/或由各菌株产生的代谢产物。在本发明的一个优选方面,所述宿主防御诱导剂是异噻菌胺或异噻菌胺和苯并噻二唑的结合物。本发明还涉及通过使用包含协同有效量的至少一种宿主防御诱导剂和至少一种生物防治剂的结合物进行处理来防治有用植物中的细菌性有害生物的方法。本发明的另一方面涉及通过对待保护以免受细菌性有害生物侵袭的植物进行两次以上的依次处理区段来防治有用植物中的细菌性有害生物的方法。
技术研发人员:K-W·明克斯;R·C·贝克尔;F·克尔兹-莫哈莱恩迪克;B·斯普林格;L·M·迪亚斯;C·N·范布鲁克伦-葛洛妮维尔德;G·拉布迪特;D·蒙克尔
受保护的技术使用者:拜耳作物科学股份公司
技术研发日:2014.07.10
技术公布日:2018.08.07
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