IHEP OpenIR
Active Site Dependent Reaction Mechanism over Ru/CeO2 Catalyst toward CO2 Methanation
Wang, F; He, S; Chen, H; Wang, B; Zheng, LR; Wei, M; Evans, DG; Duan, X; Zheng LR(郑黎荣)
2016
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
Volume138Issue:19Pages:6298-6305
SubtypeArticle
AbstractOxygen vacancy on the surface of metal oxides is one of the most important defects which acts as the reactive site in a variety of catalytic reactions. In this work, operando spectroscopy methodology was employed to study the CO2 methanation reaction catalyzed by Ru/CeO2 (with oxygen vacancy in CeO2) and Ru/alpha-Al2O3 (without oxygen vacancy), respectively, so as to give a thorough understanding on active site dependent reaction mechanism. In Ru/CeO2 catalyst, operando XANES, IR, and Raman were used to reveal the generation process of Ce3+, surface hydroxyl, and oxygen vacancy as well as their structural evolvements under practical reaction conditions. The steady-state isotope transient kinetic analysis (SSITKA)-type in situ DRIFT infrared spectroscopy undoubtedly substantiates that CO2 methanation undergoes formate route over Ru/CeO2 catalyst, and the formate dissociation to methanol catalyzed by oxygen vacancy is the rate-determining step. In contrast, CO2 methanation undergoes CO route over Ru surface in Ru/alpha-Al2O3 with the absence of oxygen vacancy, demonstrating active site dependent catalytic mechanism toward CO2 methanation. In addition, the catalytic activity evaluation and the oscillating reaction over Ru/CeO2 catalyst further prove that the oxygen vacancy catalyzes the rate -determining step with a much lower activation temperature compared with Ru surface in Ru/alpha-Al2O3 (125 vs 250 degrees C).
DOI10.1021/jacs.6b02762
Indexed BySCI
Language英语
WOS IDWOS:000376331000032
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ihep.ac.cn/handle/311005/248104
Collection中国科学院高能物理研究所
Recommended Citation
GB/T 7714
Wang, F,He, S,Chen, H,et al. Active Site Dependent Reaction Mechanism over Ru/CeO2 Catalyst toward CO2 Methanation[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2016,138(19):6298-6305.
APA Wang, F.,He, S.,Chen, H.,Wang, B.,Zheng, LR.,...&郑黎荣.(2016).Active Site Dependent Reaction Mechanism over Ru/CeO2 Catalyst toward CO2 Methanation.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,138(19),6298-6305.
MLA Wang, F,et al."Active Site Dependent Reaction Mechanism over Ru/CeO2 Catalyst toward CO2 Methanation".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 138.19(2016):6298-6305.
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