燃料化学学报2017，Vol.45Issue(12)：1473-1480,8.
Aun团簇催化水煤气变换反应机理的密度泛函理论研究
Reaction mechanism of water gas shift reaction Aun clusters: A density functional theory study
摘要
Abstract
The stability and catalytic activity of Au10 , Au13 and Au20 clusters in water gas shift reaction ( WGSR) were investigated by density functional theory ( DFT);the adsorption behavior of reaction species and the reaction mechanism of WGSR on various Aun clusters were explored. The results indicated that the stability of three Aun clusters follows the order Au10< Au13< Au20 , whereas their electron delocalization and adsorption capacity decreases in the sequence of Au13> Au10> Au20 . Three Aun clusters exhibit the same rate-determining step for WGSR, i. e. H2 O dissociation; however, they are quite different in the actual reaction routes. Over Au10 cluster, the WGSR reaction follows the carboxyl mechanism, characterized by the direct dissociation of COOH*;over Au13 cluster, the redox mechanism applies, suggested by the disproportionation of two OH*;over Au20 cluster, the WGSR reaction proceeds via the carboxyl mechanism, represented by the disproportionation of COOH* and OH*. A comparison for the optimal reaction paths over three Aun clusters suggests that the Au13 cluster has the highest catalytic activity in the WGSR reaction at low temperature.关键词
Au团簇/水煤气变换/密度泛函理论/反应机理Key words
Au cluster/water gas shift reaction/density functional theory/reaction mechanism分类
化学化工引用本文复制引用
张晓锋,薛继龙,孟跃,钱梦丹,夏盛杰,倪哲明..Aun团簇催化水煤气变换反应机理的密度泛函理论研究[J].燃料化学学报,2017,45(12):1473-1480,8.基金项目
The project was supported by the National Natural Science Foundation of China (21503188) and the Zhejiang Provincial Natural Science Foundation of China (LQ15B030002).国家自然科学基金(21503188)和浙江省自然科学基金(LQ15B030002)资助 （21503188）
