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Unraveling the interfacial effect of pdbi bimetallic catalysts on promoting CO_(2)electroreduction to formate

Nano Research 2023年第8期16卷 10822-10831页

作者： Wenhui Liu Lingtong Ding Minmin Liu Xiao Wang Zhengrong Zhang Tian-Wen Jiang Shengjuan Huo Wen-Bin Cai International Joint Laboratory of Catalytic Chemistry Department of ChemistryInstitute for Sustainable EnergyCollege of SciencesShanghai UniversityShanghai 200444China Shenzhen Key Laboratory of Nanobiomechanics Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China Paul C.Lauterbur Research Center for Biomedical Imaging Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Through interface engineering and content control strategy,a pdbi bimetallic interface structure was constructed for the first time to selectively convert CO_(2)to formate with a remarkably high Faraday efficiency(FEformate)of 94%and a partial current density(jformate)of 34 mA·cm^(−2)at−0.8 V vs.reversible hydrogen electrode(RHE)in an H-cell.Moreover,the pdbi interface electrocatalyst even exhibited a high current density of 180 mA·cm^(−2)with formate selectivity up to 92%in a flow cell and could steadily operate for at least 20 h.Electrochemical in-situ attenuated total reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS)confirmed that the pdbi interface could greatly weaken the adsorption of*CO intermediates due to electronic and geometric effects.Density functional theory(DFT)calculations also established that the pdbi interface regulated the CO_(2)-to-formate pathway by reducing the energy barrier toward HCOOH and largely weakening the adsorption of*CO intermediates on the catalyst surface.This study reveals that the unique pdbi bimetallic interface can provide a novel platform to study the reaction mechanism through combining in-situ ATR-SEIRAS and DFT calculations.

关键词： carbon dioxide reduction reaction bimetallic PdBi interface engineering formate in-situ attenuated total reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS)

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