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Ru/FeOx catalyst performance design: Highly dispersed Ru species for selective carbon dioxide hydrogenation
Zhang, D; Luo, JJ; Wang, JJ; Xiao, X; Liu, YF; Qi, W; Su, DS; Chu, W; Chu, W (reprint author), Sichuan Univ, Dept Chem Engn, Chengdu 610065, Sichuang, Peoples R China.; Chu, W (reprint author), Sichuan Univ, Inst New Energy & Low Carbon Technol, Chengdu 610065, Sichuang, Peoples R China.; Luo, JJ (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci SYNL, Shenyang 110016, Liaoning, Peoples R China.
2018-01-18
发表期刊CHINESE JOURNAL OF CATALYSIS
ISSN1872-2067
卷号39期号:1页码:157-166
摘要A series of Ru/FeOx catalysts were synthesized for the selective hydrogenation of CO2 to CO. Detailed characterizations of the catalysts through X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and temperature-programmed techniques were performed to directly monitor the surface chemical properties and the catalytic performance to elucidate the reaction mechanism. Highly dispersed Ru species were observed on the surface of FeOx regardless of the initial Ru loading. Varying the Ru loading resulted in changes to the Ru coverage over the FeOx surface, which had a significant impact on the interaction between Ru and adsorbed H, and concomitantly, the H-2 activation capacity via the ability for H-2 dissociation. FeOx having 0.01% of Ru loading exhibited 100% selectivity toward CO resulting from the very strong interaction between Ru and adsorbed H, which limits the desorption of the activated H species and hinders over-reduction of CO to CH4. Further increasing the Ru loading of the catalysts to above 0.01% resulted in the adsorbed H to be easily dissociated, as a result of a weaker interaction with Ru, which allowed excessive CO reduction to produce CH4. Understanding how to selectively design the catalyst by tuning the initial loading of the active phase has broader implications on the design of supported metal catalysts toward preparing liquid fuels from CO2. (C) 2018, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.; A series of Ru/FeOx catalysts were synthesized for the selective hydrogenation of CO2 to CO. Detailed characterizations of the catalysts through X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and temperature-programmed techniques were performed to directly monitor the surface chemical properties and the catalytic performance to elucidate the reaction mechanism. Highly dispersed Ru species were observed on the surface of FeOx regardless of the initial Ru loading. Varying the Ru loading resulted in changes to the Ru coverage over the FeOx surface, which had a significant impact on the interaction between Ru and adsorbed H, and concomitantly, the H-2 activation capacity via the ability for H-2 dissociation. FeOx having 0.01% of Ru loading exhibited 100% selectivity toward CO resulting from the very strong interaction between Ru and adsorbed H, which limits the desorption of the activated H species and hinders over-reduction of CO to CH4. Further increasing the Ru loading of the catalysts to above 0.01% resulted in the adsorbed H to be easily dissociated, as a result of a weaker interaction with Ru, which allowed excessive CO reduction to produce CH4. Understanding how to selectively design the catalyst by tuning the initial loading of the active phase has broader implications on the design of supported metal catalysts toward preparing liquid fuels from CO2. (C) 2018, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
部门归属[zhang, di ; wang, jiajie ; xiao, xin ; chu, wei] sichuan univ, dept chem engn, chengdu 610065, sichuang, peoples r china ; [zhang, di ; wang, jiajie ; xiao, xin ; chu, wei] sichuan univ, inst new energy & low carbon technol, chengdu 610065, sichuang, peoples r china ; [zhang, di ; luo, jingjie ; qi, wei ; su, dang sheng] chinese acad sci, inst met res, shenyang natl lab mat sci synl, shenyang 110016, liaoning, peoples r china ; [liu, yuefeng ; su, dang sheng] chinese acad sci, dalian inst chem phys, dalian natl lab clean energy dnl, dalian 116023, liaoning, peoples r china
关键词Fischer-tropsch Synthesis Transient Drifts-ms Gas Shift Reaction Co2 Hydrogenation Heterogeneous Catalysis Ruthenium Catalyst Gold Nanoparticles Surface-chemistry Oxygen Vacancy Methanation
学科领域Chemistry, Applied ; Chemistry, Physical ; Engineering, Chemical
资助者National Natural Science Foundation of China [21476145, 91645117]; China Postdoctoral Science Foundation [2016M600221]
收录类别SCI
语种英语
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/79574
专题中国科学院金属研究所
通讯作者Chu, W (reprint author), Sichuan Univ, Dept Chem Engn, Chengdu 610065, Sichuang, Peoples R China.; Chu, W (reprint author), Sichuan Univ, Inst New Energy & Low Carbon Technol, Chengdu 610065, Sichuang, Peoples R China.; Luo, JJ (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci SYNL, Shenyang 110016, Liaoning, Peoples R China.
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Zhang, D,Luo, JJ,Wang, JJ,et al. Ru/FeOx catalyst performance design: Highly dispersed Ru species for selective carbon dioxide hydrogenation[J]. CHINESE JOURNAL OF CATALYSIS,2018,39(1):157-166.
APA Zhang, D.,Luo, JJ.,Wang, JJ.,Xiao, X.,Liu, YF.,...&Luo, JJ .(2018).Ru/FeOx catalyst performance design: Highly dispersed Ru species for selective carbon dioxide hydrogenation.CHINESE JOURNAL OF CATALYSIS,39(1),157-166.
MLA Zhang, D,et al."Ru/FeOx catalyst performance design: Highly dispersed Ru species for selective carbon dioxide hydrogenation".CHINESE JOURNAL OF CATALYSIS 39.1(2018):157-166.
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