文献类型：期刊文献

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

作者：Cao, Xiao-Ming[1,2];Zhou, Haijin[1,2];Zhao, Liyang[1,2];Chen, Xuning[1,2];Hu, Peijun[1,2,3]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Joint Int Res Lab Precis Chem & Mol Engn, Ctr Computat Chem, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[3]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland

年份：2021

卷号：32

期号：6

起止页码：1972

外文期刊名：CHINESE CHEMICAL LETTERS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000658340900024)】；

基金：The authors gratefully acknowledge the 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) and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：Boron nitride monolayer; Density functional theory; Methane activation; Surface reactive oxygen species; Transition metal center

摘要：Methane (CH4) controllable activation is the key process for CH4 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 CH4 activation are systematically investigated during the CH4 oxidation by means of first-principles computation. The calculation results unravel the periodic variation trends for the stability of TM-BN, the adsorption strength and the kind of O-2 species, and the resulting CH4 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 CH4 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 CH4 oxidative dehydrogenation. (C) 2021 Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences. Published by Elsevier B.V. All rights reserved.