C₂₊ Selectivity for CO₂ Electroreduction on Oxidized Cu-Based Catalysts

Designfor highly selective catalysts for CO2 electroreductionto multicarbon (C2+) fuels is pressing and important. Thereis, however, presently a poor understanding of selectivity towardC(2+) species. Here we report for the first time a methodof judiciously combined quantum chemical computations, artificial-intelligence(AI) clustering, and experiment for development of a model for therelationship between C2+ product selectivity and compositionof oxidized Cu-based catalysts. We 1) evidence that the oxidized Cusurface more significantly facilitates C-C coupling, 2) confirmthe critical potential condition(s) for this oxidation state underdifferent metal doping components via abinitio thermodynamics computation, 3) establish an inverted-volcanorelationship between experimental Faradaic efficiency and criticalpotential using multidimensional scaling (MDS) results based on physicalproperties of dopant elements, and 4) demonstrate design for electrocatalyststo selectively generate C2+ product(s) through a co-dopingstrategy of early and late transition metals. We conclude that a combinationof theoretical computation, AI clustering, and experiment can be usedto practically establish relationships between descriptors and selectivityfor complex reactions. Findings will benefit researchers in designingelectroreduction conversions of CO2 to multicarbon C2+ products.