articleJournal of the American Chemical SocietyFeb 5, 2025Closed access

Tailoring CO 2 Adsorption Configuration with Spatial Confinement Switches Electroreduction Product from Formate to Acetate

Guizhou University · Huanghuai University · +3 more institutions

PubMed
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Abstract

Multi-proton-coupled electron transfer, multitudinous intermediates, and unavoidable competing hydrogen evolution reaction during CO2 electroreduction make it tricky to control high selectivity for specific products. Here, we present spatial confinement of Fe single atoms (FeN2S2) by adjacent FeS clusters (Fe4S4) to orientate the transition of CO2 adsorption configuration from C,O-side to O-end, which triggers a shift of activated CO2 from first-step protonation to C–C coupling, thus switching the target product from HCOOH in high Faraday efficiency (FE: 90.6%) on FeN2S2 to CH3COOH (FE: 82.3%) on Fe4S4/FeN2S2. The adsorption strength of *OCHO upon the solitary FeN2S2 site is linearly related to the…

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