摘要
Nanoporous metals show promising performances in electrochemical catalysis.In this paper,we report a self-supporting bimetallic porous heterogeneous indium/copper structure synthesized with a eutectic gallium-indium(EGaIn)material on a copper substrate.This nanoporous copper-indium heterostructure catalyst exhibits excellent performance in the reduction of carbon dioxide to syngas.The ratio of H_(2)/CO is tunable from 0.47 to 2.0 by changing working potentials.The catalyst is highly stable,showing 96%maintenance of the current density after a 70-h continuous test.Density functional theory calculations reveal that the indium/copper interface induces charge redistribution within the copper surface,leading to the formation of two distinct active sites,namely,Cu^(δ)and Cu0,and enabling a high-performance generation of CO and H_(2).This work provides a new strategy for obtaining self-supporting nanoporous metal electrode catalysts.
纳米多孔金属作为电催化剂使用时表现出了优异的性能.我们报道了一种利用共熔镓铟合金和铜基底制备而成的自支撑铜铟双金属多孔异质结构材料.该多孔铜铟异质结构电催化剂具有良好的二氧化碳转化为合成气的性能.通过调整工作电压,可以使氢气和一氧化碳的比例控制在0.47–2.0之间.且该催化剂非常稳定,经过70小时连续测试后还可以保持96%的电流密度.密度泛函理论计算表明,得益于这种铜铟异质结构的存在,铜表面电荷发生了转变,形成了Cu^(δ)和Cu0等不同位点,从而协同作用分别增强了催化剂生成一氧化碳和氢气的能力.本工作可为多孔金属异质结构电催化剂的设计提供新思路.
作者
Xingcheng Ma
Feng Wang
Dongxu Jiao
Dantong Zhang
Xiao Zhao
David JSingh
Jingxiang Zhao
Xiaoqiang Cui
Weitao Zheng
马星程;王锋;焦东旭;张丹彤;赵晓;辛格戴维;赵景祥;崔小强;郑伟涛(State Key Laboratory of Automotive Simulation and Control,School of Materials Science and Engineering,Key Laboratory of Automobile Materials of MOE,Jilin University,Changchun 130012,China;Key Laboratory of Photonic and Electronic Bandgap Materials,Ministry of Education,and College of Chemistry and Chemical Engineering,Harbin Normal University,Harbin 150025,China;Department of Physics and Astronomy and Department of Chemistry,University of Missouri,Columbia,Missouri 65211,United States;Guangdong Provincial Key Laboratory of Functional Oxide Materials and Devices,Southern University of Science and Technology,Shenzhen 518055,China)
基金
the National Natural Science Foundation of China(51872116 and 12034002)
the Project for Self-Innovation Capability Construction of Jilin Province Development and Reform Commission(2021C026)
the Program for JLU Science and Technology Innovative Research Team(JLUSTIRT-2017TD-09)
the Science and Technology Development Program of Jilin Province(20190201233JC)
the Fundamental Research Funds for the Central Universities.The work was carried out at LvLiang Cloud Computing Center of China,and the calculations were performed on TianHe-2.
