| Institution: | 1. Department of Chemistry, University of Cincinnati, P.O. Box 210172, Cincinnati, Ohio, 45221 USA
These authors contributed equally to this work.;2. Department of Chemistry, University of Tennessee, Knoxville, Tennessee, 37996-1600 USA;3. Department of Chemistry, University of Cincinnati, P.O. Box 210172, Cincinnati, Ohio, 45221 USA |
| Abstract: | 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?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. |
