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Electrochemical conversion of carbon dioxide promises next-level paradigm shifts in sustainability. Applications will include breakthrough solutions to global crisis threatening our civilization, including energy, food, and climate change. Here, inspired by CO dehydrogenase II from Carboxyothermus hydrogenoformans, we designed a heterogeneous Fe4S4 single-cluster catalyst Ni100-Fe4S4, achieving high performance CO2 electroreduction. Combined with the experimental data and theoreticaldoi:10.26434/chemrxiv-2022-dhj14 fatcat:xeixedoqivbpnkpmbwbmc6w5ci