Theoretical and experimental investigations on single-atom catalysis:Pt_(1)/FeO_(x) for water-gas shift reaction  

作　　者：Shan-Fei Wang Yangyang Li Haiyan Wang Jin-Xia Liang Chun Zhu Botao Qiao 

机构地区：[1]School of Chemistry and Chemical Engineering,Guizhou University,Guiyang 550025,China [2]CAS Key Laboratory of Science and Technology on Applied Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China [3]University of Chinese Academy of Sciences,Beijing 100049,China

出　　处：《Nano Research》2024年第9期8627-8637,共11页纳米研究（英文版）

基　　金：the financial support from the National Natural Science Foundation of China(NSFC,Nos.22363001 and 21963005);the NSFC Center for Single-Atom Catalysis(No.22388102);the National Key Research and Development Program of China(No.2022YFA1503900);the Natural Science Special Foundation of Guizhou University(No.202140).

摘　　要：Oxide-supported metal single-atom catalysts(SACs)have exhibited excellent catalytic performance for water-gas shift(WGS)reaction.Here,we report the single-atom catalyst Pt1/FeOx exhibits excellent medium temperature catalytic performance for WGS reactions by the density functional theory(DFT)calculations and experimental results.The calculations indicate that H_(2)O molecules are easily dissociated at oxygen vacancies,and the formed*OH and*O are adsorbed on Pt1 single atoms and the adjacent O atoms,respectively.After studying four possible reaction mechanisms,it is found that the optimal WGS reaction pathway is proceeded along the carboxyl mechanism(pathway III),in which the formation of*COOH intermediates can promote the stability of Pt_(1)/FeO_(x) SAC and the easier occurrence of WGS reaction.The energy barrier of the rate-determining step during the entire reaction cycle is only 1.16 eV,showing the high activity for the medium temperature WGS reaction on Pt_(1)/FeO_(x) SAC,which was verified by experimental results.Moreover,the calculated turnover frequencies(TOFs)of CO_(2)and H_(2)formation on Pt1/FeOx at 610 K(337℃)can reach up to 1.14×10^(-3)s^(-1)·site^(-1)through carboxyl mechanism.In this work,we further expand the application potential of Pt1/FeOx SAC in WGS reaction.

关 键 词：water-gas shift(WGS)reaction single-atom catalyst(SAC) density functional theory(DFT) thermocatalysis 

分 类 号：O64[理学—物理化学]