DOI: 10.1016/j.jcou.2017.12.005
Scopus记录号: 2-s2.0-85039161226
论文题名: DFT insight into the support effect on the adsorption and activation of key species over Co catalysts for CO2 methanation
作者: Nie X. ; Wang H. ; Li W. ; Chen Y. ; Guo X. ; Song C.
刊名: Journal of CO2 Utilization
ISSN: 22129820
出版年: 2018
卷: 24 起始页码: 99
结束页码: 111
语种: 英语
英文关键词: CO2 Methanation
; Cobalt catalyst
; Density functional theory
; Support effect
; ZrO2
Scopus关键词: Adsorption
; Aluminum compounds
; Carbon dioxide
; Catalysts
; Chemical activation
; Chemical bonds
; Cobalt
; Density functional theory
; Hydrogenation
; Methanation
; Zirconium compounds
; Adsorption properties
; Adsorption strength
; Cobalt Catalyst
; Dissociative adsorption
; Enhanced adsorptions
; Metal-support interactions
; Support effects
; ZrO2
; Catalyst supports
英文摘要: Our recent experiments for CO2 methanation reveal that Co catalysts supported on ZrO2 and Al2O3 exhibit good initial activity, but the Co/ZrO2 catalyst is catalytically more active and more stable than the Co/Al2O3 catalyst. Detailed characterization demonstrated that there are notable differences in the adsorption properties of key species between the ZrO2- and Al2O3-supported catalysts and in the metal-support interactions where Co/ZrO2 shows enhanced adsorption for key species and better reducibility of the cobalt oxide. In the present work, we performed density functional theory (DFT) calculations to provide theoretical insight into the support effect over Co/ZrO2 and Co/Al2O3 for CO2 methanation in terms of adsorption and activation of key species. The relative adsorption strengths of CO2, H2, CO, and CH4 species on Co/ZrO2 and Co/Al2O3 calculated by DFT showed qualitative agreement with experimental TPD. Importantly, DFT results uncovered an energetically more favorable H2 dissociative adsorption, faster H* surface migration, and more facile Co-O bond cleavage on Co/ZrO2 than on Co/Al2O3, thus rationalizing the experimentally observed lower temperature and higher degree of cobalt oxide reduction on the ZrO2 support. © 2017 Elsevier Ltd
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/111949
Appears in Collections: 气候减缓与适应
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作者单位: State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, China; EMS Energy Institute, PSU-DUT Joint Center for Energy Research and Departments of Energy & Mineral Engineering and Chemical Engineering, Pennsylvania State University, University Park, PA 16802, United States; Network and Information Center, Dalian University of Technology, Dalian, 116024, China
Recommended Citation:
Nie X.,Wang H.,Li W.,et al. DFT insight into the support effect on the adsorption and activation of key species over Co catalysts for CO2 methanation[J]. Journal of CO2 Utilization,2018-01-01,24