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钯装饰的 SiX（X = N、P、As、Sb、Bi）氢气进化催化剂

花匠小妙招
2025-01-08 03:40

摘要

开发单原子催化剂（SAC）是设计高效、低成本、对氢进化反应（HER）有活性的光催化剂或电催化剂的一种有前途的有用策略。在此，我们利用密度泛函理论计算探讨了钯装饰的 SiX（X = N、P、As、Sb 和 Bi）SAC 的结构、电子和氢进化催化活性。钯原子与 SiX 纳米片之间存在很强的相互作用，这种作用改变了电子特性，进而提高了导电性。在吉布斯自由能变化、d 带中心、COHP 分析和交换电流密度等描述指标的帮助下，我们系统地研究了 Pd@SiX （X = V 组）SAC 的 HER 活性。研究发现，在零外部电势（Ue = 0）和 pH 值为 0 的条件下，Pd@SiSb 和 Pd@SiBi 的吉布斯自由能（ΔGH*）分别降低到 0.96 eV 和 0.67 eV，与原始 SiSb（ΔGH* = 1.60 eV）和 SiBi（ΔGH* = 1.72 eV）相比，分别降低了近 40% 和 61%。此外，在提供的外部电位作用下，Pd@SiSb 和 Pd@SiBi SAC 的 ΔGH* 甚至分别降低到 0.23 eV 和 -0.22 eV，交换电流密度越高，HER 性能越好。因此，我们认为，在 SiX（X = V 族）二元化合物家族中，Pd@SiSb 和 Pd@SiBi SACs 是适用于 HER 的电催化剂。我们坚信，我们的研究结果将为有效利用钯等贵族元素设计 SAC 提供一些启示。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

摘要图片

Palladium-decorated SiX (X = N, P, As, Sb, Bi) catalysts for hydrogen evolution†

Developing single atom catalysts (SAC) is a promising and useful strategy for designing highly efficient and low-cost photo- or electrocatalysts that are active towards hydrogen evolution reaction (HER). Herein, we have explored the structural, electronic and HER catalytic activity of Pd-decorated SiX (X = N, P, As, Sb and Bi) SACs using density-functional theory calculations. A strong interaction exists between the Pd atom and SiX nanosheets which modifies the electronic properties which in turn increases the electrical conductivity. With the help of several descriptors, including the Gibbs free energy change, d-band center, COHP analysis and the exchange current density, we systematically investigated the HER activity of the Pd@SiX (X = group-V) SACs. It is observed that under zero external potential (Ue = 0) and at a pH of 0, the Gibbs free energy (ΔGH*) of Pd@SiSb and Pd@SiBi reduces to 0.96 eV and 0.67 eV which is nearly a 40% and 61% reduction as compared to pristine SiSb (ΔGH* = 1.60 eV) and SiBi (ΔGH* = 1.72 eV), respectively. Additionally, under the effect of supplied external potentials, the ΔGH* even reduces to 0.23 eV and −0.22 eV for the Pd@SiSb and Pd@SiBi SACs, respectively, with higher exchange current densities indicating a better HER performance. Hence we propose that, from the family of SiX (X = group-V) binary compounds, the Pd@SiSb and Pd@SiBi SACs are suitable electrocatalysts for the HER. We strongly believe that our findings will shed some light on the effective utilization of noble elements like palladium for the effective design of SACs.