【摘要】 用Ｇ９４的从头计算方法对甲烷在金属氧化镁及氧化锂表面上不同氧物种Ｏ－、Ｏ２－２、Ｏ－２、Ｏ２－催化脱氢进行了理论研究，确定了过渡态的几何构型、集居分布和反应活化能．结果表明，氧物种的催化脱氢的活性顺序为，其中Ｏ－２物种由于对甲烷具有较低的氧化能力而可能是ＯＣＭ活性和高Ｃ２选择性的氧物种。另外，还讨论了氧物种对ＣＨ４脱氧活性与其电子结构的联系。更多还原

【Abstract】 Ab initio MP2 calculations have been carried out to study C-H bond catalysticactivation in CH4 Various oxygen species O-2 O2-2,O2- are assumed to be the activespecies on the oxide MgO, Li/MgO surface.Transition states(TS) geometries,MullikenPopulations and reaction activation barriers are determined.The results reveal that the sequencein the activation ability of oxygen species is O2-2 Because the activity of O-2is intermediate between the O- and O2-,O-2 whould be better species in order to oxidativecoupling of methane(OCM) to C2 hydrocarbon with higher choiceness.The relation betweenthe activity of oxygen species for C-H bond activation and their electonic structure isdiscussed.更多还原