Electrocatalytic CO2 reduction to value-added chemicals is a sustainable way to mitigate global CO2 level and reduce societal reliance on fossil fuels but hampered by the high overpotential and poor product selectivity. Designing and developing highly efficient catalysts based on earth-abundant elements with desirable selectivity towards high-value products are both challenging and rewarding. Herein, we selected Mn, Fe, and Co and explored their oxides on the NiFe alloy surface for electrocatalytic CO2 reduction. This study is built on the previously demonstrated activity of the reduced oxophilic metal oxides towards CO2 adsorption and activation (Zhao, Y et al. ACS Catalysis 2019, 9, 3187-3197). The oxide/metal interface with controlled redox properties helps to overcome/by-pass the high potential CO2 activation step and steers the reaction towards high-value products. The results of CO2 adsorption and activation on the model electrocatalysts consisting of oxides of Mn, Fe, Co on Ni and/or NiFe alloy surfaces based on results of density functional theory calculations will be reported and the mechanism of CO2 activation, hydrogenation and possible coupling of the carbon-containing species will be presented. These earth-abundant metals-based catalysts are promising for practical applications.

Earth-abundant metal/metal oxide catalysts for efficient electrochemical CO2 reduction

ACS Fall 2021

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