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Mechanistic insight into the facet-dependent selectivity of ethylene epoxidation on Ag nanocatalysts
Zhu, Lin1; Zhang, Wei1; Zhu, Jiqin1; Cheng, Daojian1,2
2017-05-25
发表期刊APPLIED CATALYSIS A-GENERAL
ISSN0926-860X
卷号538页码:27-36
摘要

Ethylene epoxidation reaction to selectively produce the ethylene oxide (EO) is a crucial heterogeneous catalytic chemical process in industry. However, the intrinsic catalytic selectivity depending on the facet of commonly used Ag catalysts is still far from understanding. In this work, we used the periodical density functional theory (DFT) calculations to gain an atomistic insight into the facet-dependent reaction selectivity of the ethylene epoxidation on Ag catalysts. We investigated the adsorption of atomic or molecular oxygen and oxametallacycle (OMC) intermediate, and further study the dissociation of molecular oxygen and the reaction mechanism of ethylene epoxidation on (111), (110), (100), and (211) surfaces of Ag catalysts. Our results indicate that the adsorption of the 0 atom is not facet-dependent under low oxygen coverage. Moreover, although the adsorption of molecular oxygen is facet-dependent, the dissociation of molecular oxygen would not have the essential influence on selectively producing EO in the ethylene epoxidation reaction. In addition, the catalytic selectivity of ethylene epoxidation reaction is facet-dependent, following the order of (110) > (100) > (111) > (211), which is consistent with the order of the adsorption strength of the OMC intermediate. Our results show that the stability of the OMC intermediate has an essential effect on the selectivity to EO in the ethylene epoxidation reaction. We have faith in that our results can provide useful information which would guide the intellectual design of the catalysts for ethylene epoxidation by controlling their morphologies. (C) 2017 Elsevier B.V. All rights reserved.

关键词Ethylene Epoxidation Ag Catalyst Facet-dependent Selectivity Dft Calculation
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Life Sciences & Biomedicine
DOI10.1016/j.apcata.2017.03.011
收录类别SCI
语种英语
关键词[WOS]Adsorbed Species Present ; Oxygen-adsorption ; Silver Catalysts ; Covered Ag(111) ; Oxidation ; Surface ; Oxide ; Chemistry ; Model ; Size
WOS研究方向Chemistry ; Environmental Sciences & Ecology
WOS类目Chemistry, Physical ; Environmental Sciences
项目资助者National Natural Science Foundation of China(21576008 ; Open Research Fund of State Key Laboratory of Multiphase Complex Systems(MPCS-2014-D-06) ; 91634116 ; 91334203)
WOS记录号WOS:000403132600004
引用统计
被引频次:3[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/22627
专题多相复杂系统国家重点实验室
作者单位1.Beijing Univ Chem Technol, Beijing Key Lab Energy Environm Catalysis, State Key Lab Organ Inorgan Composites, Beijing 100029, Peoples R China
2.Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, Beijing, Peoples R China
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GB/T 7714
Zhu, Lin,Zhang, Wei,Zhu, Jiqin,et al. Mechanistic insight into the facet-dependent selectivity of ethylene epoxidation on Ag nanocatalysts[J]. APPLIED CATALYSIS A-GENERAL,2017,538:27-36.
APA Zhu, Lin,Zhang, Wei,Zhu, Jiqin,&Cheng, Daojian.(2017).Mechanistic insight into the facet-dependent selectivity of ethylene epoxidation on Ag nanocatalysts.APPLIED CATALYSIS A-GENERAL,538,27-36.
MLA Zhu, Lin,et al."Mechanistic insight into the facet-dependent selectivity of ethylene epoxidation on Ag nanocatalysts".APPLIED CATALYSIS A-GENERAL 538(2017):27-36.
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