Tuning covalence for phosphorus-mediated C-C coupling in carbon monoxide electroreduction to multicarbon oxygenates

Résumé fourni par la source

Electrochemical carbon monoxide reduction (COR) is a promising route for sustainable production of multicarbon chemicals from CO2, as it bypasses the large carbon losses of direct CO2 electroreduction. In most electrocatalysts currently explored to tune COR selectivity towards highadded value multicarbon oxygenated molecules, like acetate and ethanol, copper is the catalytic site of C-C bond formation. Herein, we show that by designing nanoparticles of a strongly covalent copper compound, CuSi2P3, we retain isolated copper atoms during COR and trigger the intervention of phosphorus atoms as C-C coupling sites, without directly involving copper atoms. This profound change in COR mechanism results in a high selectivity towards C2 molecules (80 % Faradaic efficiency), especially oxygenates (73%), at a current density of -150 mA cm-2. This work reveals the importance of tailoring, via the crystal structure, the local environment of metal atoms, to achieve original selectivity in COR with new families of electrocatalysts.

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