Citation: JIANG Jun-hui, CAO Yong-yong, NI Zhe-ming, ZHANG Lian-yang. Comparison of reaction mechanism of thiophene hydrodesulfurization on Au₁₃ and Pt₁₃ clusters[J]. Journal of Fuel Chemistry and Technology, ;2016, 44(08): 961-969. shu

Comparison of reaction mechanism of thiophene hydrodesulfurization on Au₁₃ and Pt₁₃ clusters

1.
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

Corresponding author: NI Zhe-ming,
Received Date: 15 March 2016
Available Online: 25 April 2016
Fund Project:

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.
- thiophene,
- hydrodesulfurization,
- adsorption,
- Au₁₃ cluster,
- Pt₁₃ cluster,
- density functional theory
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沈阳化工大学材料科学与工程学院沈阳 110142

Comparison of reaction mechanism of thiophene hydrodesulfurization on Au13 and Pt13 clusters

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通讯作者: 陈斌, bchen63@163.com

Comparison of reaction mechanism of thiophene hydrodesulfurization on Au₁₃ and Pt₁₃ clusters