Theoretical catalytic performance of single-atom catalysts M_(1)/PW_(12)O_(40)for alkyne hydrogenation materials  

作　　者：Shamraiz Hussain Talib Xuelian Jiang Shixiang Feng Mengdie Zhao Qi Yu 

机构地区：[1]School of Materials Science and Engineering,and Shaanxi Laboratory of Catalysis,Shaanxi University of Technology,Hanzhong 723001,China [2]Center for Catalysis and Separations,Khalifa University of Science and Technology,Abu Dhabi,P.O.Box 127788,United Arab Emirates [3]Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis,Southern University of Science and Technology,Shenzhen 518055,China [4]Joint School of National University of Singapore and Tianjin University,International Campus of Tianjin University,Binhai New City,Fuzhou 350207,China

出　　处：《Nano Research Energy》2024年第4期13-22,共10页纳米能源研究(英文)

基　　金：National Natural Science Foundation of China(No.92061109);NSFC Center for Single-Atom Catalysis(grant No.22388102);Natural Science Basic Research Program of Shaanxi(Program No.2021JCW-20 and 2022KJXX-18)。

摘　　要：Single-atom catalysts(SACs)have provoked significant curiosity in heterogeneous catalysis due to the benefits of maximum metal atoms usage,robust metal-support interaction,single-metal-atom active sites,and high catalytic efficiency.In this study,the electronic structures and catalytic mechanism of ethyne hydrogenation of SACs with the group-9 metal atoms M1(M1=Co,Rh,Ir)anchored on PTA(phosphotungstic acid)cluster have been explored by using first-principles quantum calculations.It is found that the catalytic activity of ethyne(C_(2)H_(2))hydrogenation is determined by two critical parameters:the adsorption energies of the adsorbate(H_(2),C_(2)H_(2))and the activation energy barrier of ethyne hydrogenation.We have shown that the reaction pathway of ethyne hydrogenation reaction on the experimentally characterized Rh1/PTA at room temperature consists of three steps:C_(2)H_(2) and H_(2) coadsorption on Rh1/PTA,H_(2) attacking C_(2)H_(2) to form C_(2)H_(4),then C_(2)H_(4) desorbing or further reacting with H_(2) to produce C_(2)H6 and completing the catalytic cycle.The Rh1/PTA possesses fair catalytic activity with a C_(2)H_(4) desorption energy of 1.46 eV and a 2.59 eV barrier for ethylene hydrogenation.Moreover,micro-kinetics analysis is also carried out to understand the mechanism and catalytic performance further.The work reveals that the PTA-supported SACs can be a promising catalyst for alkyne hydrogenation.

关 键 词：single-atom catalyst phosphotungstic acid alkyne hydrogenation transition metal atoms first-principles calculations 

分 类 号：O64[理学—物理化学]