Computational Discovery of Nickel-Based Catalysts for CO2 Reduction to Formic Acid

Electrochemical reduction of CO2 into chemical fuels is crucial to clean energy production and environment remediation. First-principles calculations are performed to elucidate reaction mechanism of CO2 reduction to formic acid on Ni-based catalysts. The origin of CO poisoning is examined and a novel design strategy is proposed to eliminate CO poisoning. Three design criteria are derived based on which computational screening is performed to identify several Ni-based near-surface-alloys (NSAs) with both high selectivity and reactivity. The effect of elastic strain on CO2 reduction is studied on these NSAs. We predict that Ni/Ti, Cu/Ni, and strained Cu/Ni NSAs could lead to highly selective and efficient production of formic acid.