Electrocatalytic Hydrogen Evolution Using A Molecular Antimony Complex under Aqueous Conditions: An Experimental and Computational Study on Main‐Group Element Catalysis
Electrocatalytic Hydrogen Evolution Using A Molecular Antimony Complex under Aqueous Conditions: An Experimental and Computational Study on Main‐Group Element Catalysis
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水相条件下使用分子锑配合物电催化析氢：主族元素催化的实验和计算研究
DOI：
10.1002/chem.202201323
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Jiang, Jianbing “Jimmy”
中科院分区：
文献类型：
--
作者：
Williams, Caroline K.;McCarver, Gavin A.;Chaturvedi, Ashwin;Sinha, Soumalya;Ang, Marcus;Vogiatzis, Konstantinos D.;Jiang, Jianbing “Jimmy”
电催化氢气生产被认为是实现碳中性能源的潜在途径。然而，这项技术的发展受到缺乏高效，成本效益和环境友好催化剂的阻碍。在这项研究中，一个主族元素为基础的电催化剂，SbSalen，报道催化析氢反应（HER）在水介质中。异质化分子系统在−1.4 V vs. NHE下实现了100%的法拉第效率，最大电流密度为−30.7 mA/cm 2。 电解前后催化剂结合的工作电极的X射线光电子能谱证实了催化过程中的分子稳定性。使用氧化还原峰积分计算的转换频率为43.4 s− 1。通过计算方法进一步研究了电催化反应的动力学和机理。这项研究为非均相小分子转化的主族元素电催化剂提供了机理见解。
Electrocatalytic hydrogen gas production is considered a potential pathway towards carbon‐neutral energy sources. However, the development of this technology is hindered by the lack of efficient, cost‐effective, and environmentally benign catalysts. In this study, a main‐group‐element‐based electrocatalyst,SbSalen, is reported to catalyze the hydrogen evolution reaction (HER) in an aqueous medium. The heterogenized molecular system achieved a Faradaic efficiency of 100 % at −1.4 V vs. NHE with a maximum current density of −30.7 mA/cm2. X‐ray photoelectron spectroscopy of the catalyst‐bound working electrode before and after electrolysis confirmed the molecular stability during catalysis. The turnover frequency was calculated as 43.4 s−1using redox‐peak integration. The kinetic and mechanistic aspects of the electrocatalytic reaction were further examined by computational methods. This study provides mechanistic insights into main‐group‐element electrocatalysts for heterogeneous small‐molecule conversion.