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Electron Localization and Lattice Strain Induced by Surface Lithium Doping Enable Ampere‐Level Electrosynthesis of Formate from CO<sub>2</sub>

Shuai Yan, Peng Chen, Chao Yang, Yangshen Chen, Junbo Zhang, Anxiang Guan, Ximeng Lv, Haozhen Wang, Zhiqiang Wang, Tsun‐Kong Sham, Qing Han, Gengfeng Zheng

2021Angewandte Chemie32 citationsDOI

Abstract

Abstract The electrochemical CO 2 conversion to formate is a promising approach for reducing CO 2 level and obtaining value‐added chemicals, but its partial current density is still insufficient to meet the industrial demands. Herein, we developed a surface‐lithium‐doped tin (s‐SnLi) catalyst by controlled electrochemical lithiation. Density functional theory calculations indicated that the Li dopants introduced electron localization and lattice strains on the Sn surface, thus enhancing both activity and selectivity of the CO 2 electroreduction to formate. The s‐SnLi electrocatalyst exhibited one of the best CO 2 ‐to‐formate performances, with a partial current density of −1.0 A cm −2 for producing formate and a corresponding Faradaic efficiency of 92 %. Furthermore, Zn–CO 2 batteries equipped with the s‐SnLi catalyst displayed one of the highest power densities of 1.24 mW cm −2 and an outstanding stability of &gt;800 cycles. Our work suggests a promising approach to incorporate electron localization and lattice strain for the catalytic sites to achieve efficient CO 2 ‐to‐formate electrosynthesis toward potential commercialization.

Topics & Concepts

FormateElectrosynthesisElectrochemistryElectrocatalystCatalysisFaraday efficiencyChemistryDopingInorganic chemistryMaterials scienceChemical engineeringNanotechnologyPhysical chemistryElectrodeOrganic chemistryOptoelectronicsEngineeringCO2 Reduction Techniques and CatalystsElectrocatalysts for Energy ConversionIonic liquids properties and applications
Electron Localization and Lattice Strain Induced by Surface Lithium Doping Enable Ampere‐Level Electrosynthesis of Formate from CO<sub>2</sub> | Litcius