《Co3O4纳米晶催化氧化甲烷的理论研究：C-H键活化的晶面效应及活性中心》.pdfVIP

ChineseJournalofCatalysis35(2014]462—467 催化学报2014年 第35卷 g4期 1www．chxb．cn 镬 a一 ab¨ e-蠢 瓣 ．sel簿 e d ee鼍．∞| 蒜 0 曩 一 臻 一 董 誊 嘶 蠢 曩一 joI¨_I a 舞：：m攀p囊g ：、^、^w。eI¨e：r {》 ／lo囊t囊，露hje Article Theoreticalstudyofthecrystalplaneeffectandion-pairactive centerforC--HbondactivationbyCo304nanocrystals YanggangWang，XiaofengYang一，LinhuaHu，YadongLia／JunLi， aDepartmentofChemistry,TsinghuaUniversity,Beqing100084,China StateKeyLaboratoryofCatasis,DalianInstituteofChemicalP sicsChineseAcademyofSciences,Dalian116023,Liaoning,China A R T IC L E IN F O A B S T R A C T Articlehistory： Methanehasattractedextensiveinterestinrecentyearsduetoitspotentialapplication asare． Received29December2013 placementofoilandafeedstockforvaluablechemicals．DuetothelargeC-Hbondenergy,thecon— Accepted20January2014 versionofmethaneintousefulproductshasbeenachallenge．Inthepresentstudy．densityfunc— Published20April2014 tionaltheory(DFT]calculationswereperformedtostudytheactivationoftheC—Hbondofmethane onthe(001)and(011)planesofCo304，whichshowedthatCH4activationonCo304nanocrystals Keywords： wasfairlyeasywithonlysmalleneryg barriers(1essthan1．1eV)．SurfaceCo-Oionpairsarethe activesiteofrC—Hbondactivation．wherethetwoionsprovideasynergisticeffectf0rtheactivation C—Hbondactivation Methaneconversion ofthestrongC—HbondandyieldsupfaceCo—CH3and0一Hspecies．TheCo304(0111surfacaisshown Crystalplaneeffect t0bemorereactiveforC—HbondactivationthantheC