Diatomic Pd catalyst with conjugated backbone for synergistic electrochemical CO_(2)reduction  

作　　者：Wenxuan Zhang Mengran Zhang Hongjuan Wang Wen Zhang Min Zhang 

机构地区：[1]MOE International Joint Laboratory of Materials Microstructure,Institute for New Energy Materials and Low Carbon Technologies,School of Materials Science and Engineering,Tianjin University of Technology,Tianjin 300384,China [2]Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion,School of Chemistry and Chemical Engineering,Tianjin University of Technology,Tianjin 300384,China

出　　处：《Nano Research》2024年第6期4850-4855,共6页纳米研究（英文版）

基　　金：the National Natural Science Foundation of China(No.22275139);Natural Science Foundation of Tianjin(No.22JCZDJC00510).

摘　　要：Double-site catalysts have attracted widespread attention in the field of electrocatalysis due to their high metal loading,adjustable active centres,and electronic valence states.However,the development of bimetallic sites catalysts that coordinate with definite atoms is still in the exploratory stage.Here,we designed and synthesized a bimetallic palladium complex(BPB-Pd_(2))with conjugated backbone.The supported BPB-Pd_(2)was applied to electrochemical CO_(2)reduction reaction(CO_(2)RR)for the first time.The as-obtained BPB-Pd_(2)gives an exceptional Faradaic efficiency of CO(FECO)of 94.4%at−0.80 V vs.reversible hydrogen electrode(RHE),which is significantly superior to monoatomic palladium catalyst(BPB-Pd1).The density functional theory(DFT)calculations revealed that the essential reason for the outstanding activity of BPB-Pd_(2)toward CO_(2)RR was that the electronic effect between diatomic palladium reduces the free energy change for CO_(2)RR process.Thus,BPB-Pd_(2)exhibits moderate free energy change to form COOH*intermediate,which was beneficial for the generation of CO in CO_(2)RR.

关 键 词：synthesis electrocatalysis CO_(2)reduction bimetallic palladium complex synergistic catalysis 

分 类 号：O64[理学—物理化学]