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Natural photosynthesis proceeded by sequential water splitting and CO 2  reduction reactions is an efficient strategy for CO 2  conversion. Here, mimicking photosynthesis to boost CO 2 -to-CO conversion is achieved by using plasmonic Bi as an electron-proton-transfer mediator. Electroreduction of H 2 O with a Bi electrode simultaneously produces O 2  and hydrogen-stored Bi (Bi-H  x  ). The obtained Bi-H  x   is subsequently used to generate electron-proton pairs under light irradiation to reduce CO 2  to CO; meanwhile, Bi-H  x   recovers to Bi, completing the catalytic cycle. This two-step strategy avoids O 2  separation and enables a CO production efficiency of 283.8 μmol g −1  h −1  without sacrificial reagents and cocatalysts, which is 9 times that on pristine Bi in H 2  gas. Theoretical/experimental studies confirm that such excellent activity is attributed to the formed Bi-H  x   intermediate that improves charge separation and reduces reaction barriers in CO 2  reduction.

Boosting thermo-photocatalytic CO2 conversion activity by using photosynthesis-inspired electron-proton-transfer mediators