DOI: 10.1016/j.jcou.2018.12.010
Scopus记录号: 2-s2.0-85058891328
论文题名: Comparative computational study of CO 2 dissociation and hydrogenation over Fe-M (M = Pd, Ni, Co) bimetallic catalysts: The effect of surface metal content
作者: Nie X. ; Wang H. ; Liang Z. ; Yu Z. ; Zhang J. ; Janik M.J. ; Guo X. ; Song C.
刊名: Journal of CO2 Utilization
ISSN: 22129820
出版年: 2019
卷: 29 起始页码: 179
结束页码: 195
语种: 英语
英文关键词: Adsorption
; Bimetallic catalyst
; CO 2
; Density functional theory
; Hydrogenation
Scopus关键词: Adsorption
; Atoms
; Binary alloys
; Carbon dioxide
; Catalyst activity
; Computation theory
; Density functional theory
; Dissociation
; Hydrogenation
; Surface reactions
; Transition metals
; Bimetallic catalysts
; Bimetallic surfaces
; Calculation results
; Computational studies
; Formation pathways
; Surface atomic ratio
; Surface metals
; Transition state
; Palladium
英文摘要: Density functional theory (DFT) calculations were performed to study CO 2 adsorption, dissociation and hydrogenation over Fe-M (M = Pd, Ni, Co) bimetallic catalysts, with a focus on probing the effect of surface content of the added transition metals to Fe. Various Fe-M bimetallic surfaces were constructed with varied surface atomic ratios of Fe/(Fe + M), based on which CO 2 and atomic H∗adsorptions were systematically examined. The H∗was found to be energetically favorable adsorbed at the 4-fold hollow site of Fe-M catalysts and the adsorption stability was slightly impacted by the surface content of the introduced transition metal. For CO 2 adsorption, stable bent structures adsorbed on the 4-fold hollow sites were identified on Fe-Ni and Fe-Co surfaces, no matter at which Fe-M formulations. However, on Fe-Pd surfaces, CO 2 adsorption configurations were found to be sensitive to surface Pd content, resulting in large distinctions in adsorption stabilities of CO 2 as compared to Fe-Co and Fe-Ni surfaces. CO 2 dissociation and initial hydrogenation were comparatively investigated on Fe-M bimetallic surfaces, and the calculation results demonstrated that CO 2 conversion properties are similar over Fe-Ni and Fe-Co catalysts, with CO∗and HCOO∗as the preferred intermediates but the barriers are still above 0.8 eV. While on Fe-Pd bimetallic surfaces, CO 2 reactions exhibit significant distinctions with varying the surface Pd content, showing a dramatic preference (E act around 0.3∼0.4 eV) towards HCOO∗and CO∗formation at surface Pd/(Pd + Fe) atomic ratios of 4/9 and 5/9. The superior catalytic activities of Fe-Pd catalysts are attributed to the particular surface structures and electronic features at specific bimetallic formulations which result in unique adsorption configurations of CO 2 and facilitate the stabilization of transition states in CO∗and HCOO∗formation pathways in CO 2 conversion. © 2018 Published by Elsevier Ltd. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/117314
Appears in Collections: 气候变化与战略
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Recommended Citation:
Nie X.,Wang H.,Liang Z.,et al. Comparative computational study of CO 2 dissociation and hydrogenation over Fe-M (M = Pd, Ni, Co) bimetallic catalysts: The effect of surface metal content[J]. Journal of CO2 Utilization,2019-01-01,29