Abstract
Direct electrochemical reduction of CO2 (CO2 RR) into value-added chemicals is a promising solution to reduce carbon emissions. The activity of CO2 RR is influenced deeply by the reaction microenvironment and electronic properties of the catalysts. Herein, the surface PO4 3- anions are tuned to modulate the local microenvironment and the electronic properties of indium-based catalyst with abundant metal-oxygen species enabling efficient electrochemical conversion of CO2 to HCOO- . Indium nanoparticles coupled with PO4 3- anions (PO4 3- -In NPs) achieved a high selectivity of HCOO- up to 91.4% at a low potential of -0.98 V versus reversible hydrogen electrode (vs. RHE), and a high HCOO- partial current density of 279.3 mA cm-2 at -1.1 V vs. RHE in the electrochemical flow cell. In-situ and ex-situ characterizations confirmed the PO4 3- anions kept stable on the surface of indium during CO2 RR, accelerating the generation of OCHO* intermediate. From density functional theory (DFT) calculations, PO4 3- anions enriched the metal-oxygen species on the substrate to optimize the electronic structure of the catalysts and induced a local microenvironment with massive K+ ions on the interface, thus reducing the activation energy barrier of CO2 RR. This article is protected by copyright. All rights reserved.
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