燃料化学学报2016，Vol.44Issue(8)：961-969,9.
噻吩在Au13和Pt13团簇上加氢脱硫的反应机理比较
Comparison of reaction mechanism of thiophene hydrodesulfurization on Au13 and Pt13 clusters
摘要
Abstract
The behaviors of thiophene adsorption and hydrodesulfurization on cubic octahedral M13 ( M = Au, Pt) clusters were investigated by density functional theory. The results show that the adsorption energy of thiophene on Pt13 is higher than that on Au13;on the Au13 cluster, the Hol-tri site is most stable for the thiophene adsorption with ring, whereas on the Pt13 cluster, the Hol-quadr site is most stable. By the indirect desulfurization mechanism, the desulfurization is achieved probably via the cis-hydrogenation; the removal of C-S is the rate-determining step. By the direct desulfurization mechanism, the HS hydrogenation turns to be the rate-determining step. The desulfurization is most likely via the direct desulfurization mechanism, which exhibits much lower activation energy than the indirect desulfurization mechanism. The energy change for thiophene desulfurization on the Au13 cluster is exothermic, whereas on the Pt13 cluster it is endothermic; as a result, the hydrodesulfurization on Au13 is much easier than that on Pt13 .关键词
噻吩/加氢脱硫/吸附/Au13团簇/Pt13团簇/密度泛函理论Key words
thiophene/hydrodesulfurization/adsorption/Au13 cluster/Pt13 cluster/density functional theory分类
化学引用本文复制引用
蒋军辉,曹勇勇,倪哲明,张连阳..噻吩在Au13和Pt13团簇上加氢脱硫的反应机理比较[J].燃料化学学报,2016,44(8):961-969,9.基金项目
The project was supported by the National Natural Science Foundation of China (21503188).国家自然科学基金(21503188)资助 （21503188）
