Ni–Fe–S Cubanes in CO₂ Reduction Electrocatalysis: A DFT Study

In this work, we perform extensive mechanistic studies of CO₂ (electro)­reduction by analogs to the active sites of carbon monoxide dehydrogenase (CODH) enzymes. We explore structure–property relationships for different cluster compositions and interpret the results with a model for CO₂ electroreduction we recently developed and applied to transition metal catalysts. Our results validate the effectiveness of the CODH in catalyzing this important reaction and give insight into why specific cluster compositions were adopted by nature.