人工晶体学报2025，Vol.54Issue(8)：1441-1453,13.DOI:10.16553/j.cnki.issn1000-985x.2025.0035
非化学计量比氧化钨(WO3-x)催化甲烷氧化制甲醇反应的第一性原理研究
First-Principles Study on Oxidation of Methane to Methanol Catalyzed by Non-Stoichiometric Tungsten Oxide(WO3-x)
摘要
Abstract
The key challenge in the oxidation of methane to methanol is attributed to the efficient activation of CH4 by catalysts.Non-stoichiometric WO3-x(0<x<3),recognized for its controllable oxygen vacancies along with structural stability and conductive advantages,has emerged as a research hotspot in novel catalytic materials.In this study,density functional theory(DFT)methods were employed to systematically investigate the catalytic performance of six distinct WO3-x materials for oxidation of methane to methanol.The mechanisms were elucidated through comprehensive analyses of material structures,surface active sites,methane oxidation behaviors and electronic properties.The results reveal that the WO-terminated surface of the WO2.72 catalyst demonstrates enhanced methane adsorption and activation capabilities,which are ascribed to its lower work function,hybridization between W 5d orbitals and CH4 molecules,and the strong electron-donating capacity of W atomic states.Specifically,this surface exhibits a favorable CH4 adsorption free energy(-0.62 eV)and dissociation free energy(-0.07 eV).These findings provide theoretical guidance for exploring the application of WO3-x catalysts in methane oxidation reactions.关键词
甲烷/光催化/WO3-x/第一性原理/密度泛函理论Key words
methane/photocatalysis/WO3-x/first-principle/density functional theory分类
数理科学引用本文复制引用
秦纪龙,李向远,张璐璐,刘建新,李瑞..非化学计量比氧化钨(WO3-x)催化甲烷氧化制甲醇反应的第一性原理研究[J].人工晶体学报,2025,54(8):1441-1453,13.基金项目
国家自然科学基金面上项目(22478273) （22478273）
山西省中央引导地方科技发展资金项目(YDZJSX20231A014) （YDZJSX20231A014）
山西省科技合作交流专项项目(202304041101040) （202304041101040）
