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

作　　者：Wenhui Liu Lingtong Ding Minmin Liu Xiao Wang Zhengrong Zhang Tian-Wen Jiang Shengjuan Huo Wen-Bin Cai 

机构地区：[1]International Joint Laboratory of Catalytic Chemistry,Department of Chemistry,Institute for Sustainable Energy,College of Sciences,Shanghai University,Shanghai 200444,China [2]Shenzhen Key Laboratory of Nanobiomechanics,Shenzhen Institute of Advanced Technology,Chinese Academy of Sciences,Shenzhen 518055,China [3]Paul C.Lauterbur Research Center for Biomedical Imaging,Shenzhen Institute of Advanced Technology,Chinese Academy of Sciences,Shenzhen 518055,China [4]Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials,Collaborative Innovation Center of Chemistry for Energy Materials,Department of Chemistry,Fudan University,Shanghai 200438,China

出　　处：《Nano Research》2023年第8期10822-10831,共10页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.22003074 and 22002087);Youth Innovation Promotion Association CAS,Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials(No.2021MCIMKF03);Baoshan Iron&Steel Co.,Ltd.(Baosteel),located in Shanghai,China.

摘　　要：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) 

分 类 号：O64[理学—物理化学]