Williams Caroline K, McCarver Gavin A, Chaturvedi Ashwin, Sinha Soumalya, Ang Marcus, Vogiatzis Konstantinos D, Jiang Jianbing Jimmy
Department of Chemistry, University of Cincinnati, P.O. Box 210172, Cincinnati, Ohio, 45221, USA.
Department of Chemistry, University of Tennessee, Knoxville, Tennessee, 37996-1600, USA.
Chemistry. 2022 Sep 16;28(52):e202201323. doi: 10.1002/chem.202201323. Epub 2022 Jul 25.
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/cm . 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 using 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.
电催化制氢被认为是通向碳中和能源的一条潜在途径。然而，该技术的发展受到缺乏高效、经济高效且环境友好型催化剂的阻碍。在本研究中，据报道一种基于主族元素的电催化剂SbSalen可在水介质中催化析氢反应（HER）。该异质化分子体系在相对于标准氢电极（NHE）为 -1.4 V时实现了100%的法拉第效率，最大电流密度为 -30.7 mA/cm 。电解前后催化剂负载工作电极的X射线光电子能谱证实了催化过程中分子的稳定性。通过氧化还原峰积分计算得出周转频率为43.4 s 。采用计算方法进一步研究了电催化反应的动力学和机理方面。本研究为用于多相小分子转化的主族元素电催化剂提供了机理见解。
