Pressure-Boosted C-C Coupling for CO Electroreduction to Ethanol over the Cascade Sites of Cu Single-Atom and Cu Cluster.

Tandem catalysis of the CO electroreduction reaction (CORR) offers a promising way to obtain multicarbon products (C) with high Faradaic efficiency (FE). However, the synchronously changed CO supply and consumption with potentials and the mismatch between the two potential windows of the different components in tandem catalysts impede further understanding and development of tandem catalysis. Herein, a novel strategy of pressure regulating to separately promote the CO supply and consumption is reported on the cascade sites of Cu single-atom and Cu cluster, where a near-linear relationship between CO pressure, CO supply, and ethanol FE is well established. Benefiting from the above strategy, the ethanol FE of 41.2% is achieved under 26 bar CO, which increases by ≈3 times that under ambient pressure. This work provides a new method of CO supply regulation and gives more mechanism insights into the tandem catalysis of CO electroreduction toward multicarbon products.