Screening performance of methane activation over atomically dispersed metal catalysts on defective boron nitride monolayers:A density functional theory study

查看全文 作　　者：Xiao-Ming [1]Cao;Haijin [1]Zhou;Liyang [1]Zhao;Xuning [1]Chen;Peijun [1,2]Hu 机构地区：[1]Joint International Research Laboratory for Precision Chemistry and Molecular Engineering,Centre for Computational Chemistry and Research Institute of Industrial Catalysis,School of Chemistry and Molecular Engineering,East China University of Science and Technology,Shanghai 200237,China;[2]School of Chemistry and Chemical Engineering,The Queen's University of Belfast,Belfast BT95AG,United Kingdom 出　　处：《Chinese Chemical Letters》索引2021年第32卷第6期,共5页 基　　金：financial support from the National Natural Science Foundation of China(NSFC,Nos.21673072 and 91845111);Program of Shanghai Subject Chief Scientist(No.17XD1401400);Shanghai Science and Technology Committee(No.17520750100);the Fundamental Research Funds for the Central Universities。 摘　　要：Methane(CH_(4))controllable activation is the key process for CH_(4)upgrading,which is sensitive to the surface oxygen species.The high thermal conductivity and superb thermal stability of the hexagonal boron nitride(h-BN)sheet makes a single transition metal atom doped hexagonal boron nitride monolayer(TM-BN)possible to be a promising material for catalyzing methane partial oxidation.The performances of 24 TM-BNs for CH_(4)activation are systematically investigated during the CH_(4)oxidation by means of first-principles computation.The calculation results unravel the periodic va riation trends for the stability of TM-BN,the adsorption strength and the kind of O_(2)species,and the resulting CH_(4)activation performance on TM-BNs.The formed peroxide O_(2)^(2-)of which the O-O bond could be broken and O-anions are found to be reactive oxygen species for CH_(4)activation under the mild conditions.It is found that the redox potential of TM center,including its valence electron number,coordination environment,and the work function of TM-BN,is the underlying reason for the formation of different oxygen species and the resulting activity for CH_(4)oxidative dehydrogenation. 关 键 词：Boron nitride monolayer Density functional theory Methane activation Surface reactive oxygen species Transition metal center