西北师范大学学报（自然科学版）2017，Vol.53Issue(1)：65-69,78,6.DOI:10.16783/j.cnki.nwnuz.2017.01.011
气相中Au+2催化水煤气变换循环反应的理论研究
Theory study of the water-gas shift cycle reaction catalyzed by Au+2 in the gas phase
摘要
Abstract
The mechanism of the Au+2 catalyze CO and H2 O to form CO2 and H2 of the water-gas shift (WGS)cycle reaction has been considered on doublet and quartet potential energy surfaces in the gas phase.The UB3LYP density functional theory has been used in the reaction. All geometries are completed optimized.Transition states of the reaction are confirmed by the vibration frequency calculation and the intrinsic reaction coordinate analysis.Meanwhile,the possible of the potential energy surfaces (PESs)crossing has been discussed.The turnover frequency(fTO )is computed with the energetic span model by Kozuch,and the rate states are defined of the cycle reaction.The result shows that crossing points between the different PESs does not appear.The 2 TS34 and 2 IM1 are defined as rate-determining transition states(TDTS)and rate-determining intermediates(TDI),respectively.For the cycle reaction,δE and fTO are 237.6 kJ·mol-1 and 1.440×10-29 s-1 under the temperature of 298.15 K.关键词
密度泛函/Au+2 催化/转化频率/能量跨度模型Key words
density functional theory(DFT)/Au+2 catalyze/the turnover frequency(fTO )/energetic span model分类
化学化工引用本文复制引用
王永成,李爽,王晓莉,张玉伟,马盼盼..气相中Au+2催化水煤气变换循环反应的理论研究[J].西北师范大学学报（自然科学版）,2017,53(1):65-69,78,6.基金项目
国家自然科学基金资助项目(21263023) （21263023）
