Pt overlayer for direct oxidation of CH_(4)to CH_(3)OH  

作　　者：Haoyu Li Wei Pei Xiaowei Yang Si Zhou Jijun Zhao 

机构地区：[1]Key Laboratory of Materials Modification by Laser,Ion and Electron Beams(Dalian University of Technology),Ministry of Education,Dalian 116024,China [2]College of Physics Science and Technology,Yangzhou University,Yangzhou 225009,China

出　　处：《Chinese Chemical Letters》2023年第11期280-284,共5页中国化学快报（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.11974068,91961204,and 12004065);the Fundamental Research Funds for the Central Universities of China(No.DUT20LAB110);the Liaoning Provincial Natural Science Foundation of China(No.2019JH3/30100002);Key Research and Development Project of Liaoning Province(No.2020JH2/10500003).

摘　　要：Highly selective conversion of methane(CH_(4))to methanol(CH_(3)OH)is an emerging attractive but challenging process for future development of hydrogen economy,which requires efficient catalysts.Herein,we systematically explore the catalytic properties of Pt(111)overlayer on transition metal oxides(TMOs)for CH_(4) conversion by first principles calculations.The Pt(111)monolayer supported by Ce-terminated CeO_(2)(111)substrate exhibits high activity and selectivity for CH_(4) conversion to CH_(3)OH,with the kinetic barrier of rate-limiting step of 1.05 eV.Intriguingly,the surface activity of Pt overlayer is governed by its d-band center relative to the energy of bonding states of adsorbed molecules,which in turn depends on the number of charge transfer between Pt(111)monolayer and underlying TMOs substrates.These results provide useful insights in the design of metal overlayers as catalysts with high-ultra performance and atomic utilization.

关 键 词：CH_(4)conversion Pt(111)overlayer d-band center 

分 类 号：O64[理学—物理化学]