Boosting thermo-photocatalytic CO<sub>2</sub> conversion activity by using photosynthesis-inspired electron-proton-transfer mediators.

Li, Yingxuan; Hui, Danping; Sun, Yuqing; Wang, Ying; Wu, Zhijian; Wang, Chuanyi; Zhao, Jincai · Nat Commun · 2021

basic_science · Level V

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Abstract

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