Electrocatalytic Hydrogen Evolution Using A Molecular Antimony Complex under Aqueous Conditions: An Experimental and Computational Study on Main‐Group Element Catalysis

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(2). 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(-1) 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.