Cobalt Corrole Catalyst for Efficient Hydrogen Evolution Reaction from H2O under Ambient Conditions: Reactivity, Spectroscopy, and Density Functional Theory Calculations

摘要: The feasibility of a hydrogen-based economy relies very much on the availability catalysts for hydrogen evolution reaction (HER) that are not based Pt or other noble elements. Significant breakthroughs have been achieved with certain first row transition metal complexes in terms low overpotentials and large turnover rates, but majority reported work utilized purified deoxygenated solvents (most commonly mixtures organic solvents/acids). Realizing design earth abundant operate under truly ambient conditions remains an unresolved challenge, we now developed electronically tuned Co(III) corrole can catalyze HER from aqueous sulfuric acid at as −0.3 V vs NHE, frequency 600 s–1 ≫107 catalytic turnovers. Under aerobic conditions, using H2O naturally available sources without any pretreatment, same complex catalyzes reduction H+ Faradaic Yield (FY) 52%. Density functional theory (D...