Revealing the role of electrode potential micro-environments in single Mn atoms for carbon dioxide and oxygen electrolysis  

作　　者：Pengcheng Liu anyi Liu Kaili Wang Shuai Shi Mengmeng Jin Jingxiu Liu Tao Qin Qian Liu Xijun Liu Jia He 

机构地区：[1]Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion,School of Chemistry and Chemical Engineering,Institute of New-Energy Materials and Low-Carbon Technologies,School of Materials Science and Engineering,Tianjin University of Technology,Tianjin 300384,China [2]School of Chemistry and Chemical Engineering and Environmental Engineering,Weifang University,Weifang 261061,China [3]Department of Electrical Engineering and Automation,Luoyang Institute of Science and Technology,Luoyang 471023,China [4]Institute for Advanced Study,Chengdu University,Chengdu 610106,China [5]State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures,Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials,School of Resources,Environment and Materials,Guangxi University,Nanning 530004,China

出　　处：《Nano Research》2024年第9期7957-7966,共10页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.52073214 and 22075211);Guangxi Natural Science Fund for Distinguished Young Scholars(No.2024GXNSFFA010008).

摘　　要：Elucidation the relationship between electrode potentials and heterogeneous electrocatalytic reactions has attracted widespread attention.Herein we construct the well-defined Mn single-atom(MnSA)catalyst with four N-coordination through a simple thermal pyrolysis preparation method to investigate the electrode potential micro-environments effect on carbon dioxide reduction reactions(CO_(2)RR)and oxygen reduction reactions(ORR).MnSA catalysts generate higher CO production Faradaic efficiency of exceeding 90%at-0.9 V for CO_(2)RR and higher H_(2)O_(2)yield from 0.1 to 0.6 V with excellent ORR activity.Density functional theory(DFT)calculations based on constant potential models were performed to study the mechanism of MnSA on CO_(2)RR.The thermodynamic energy barrier of CO_(2)RR is lowest at-0.9 V vs.reversible hydrogen electrode(RHE).Similar DFT calculations on the H_(2)O_(2)yield of ORR showed that the H_(2)O_(2)yield at 0.2 V was higher.This study provides a reasonable explanation for the role of electrode potential micro-environments.

关 键 词：electrode potential micro-environments Mn single-atom catalyst carbon dioxide reduction reaction oxygen reduction reaction constant potential models 

分 类 号：O64[理学—物理化学]