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Reverse water gas shift reaction using supported ionic liquid phase catalysts

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Title: Reverse water gas shift reaction using supported ionic liquid phase catalysts
Authors: Yasuda, Tomohiro Browse this author
Uchiage, Eriko Browse this author
Fujitani, Tadahiro Browse this author
Tominaga, Ken-ichi Browse this author
Nishida, Mayumi Browse this author
Keywords: Supported ionic liquid phase
Reverse water gas shift reaction
Ionic liquid
Catalytic cycle
Ru catalyst
Issue Date: 15-Sep-2018
Publisher: Elsevier
Journal Title: Applied Catalysis B-environmental
Volume: 232
Start Page: 299
End Page: 305
Publisher DOI: 10.1016/j.apcatb.2018.03.057
Abstract: The reverse water gas shift reaction (RWGSR) using a supported ionic liquid-phase (SILP) catalyst consisting of Ru catalyst, ionic liquid (1-butyl-3-methylimidazolium chloride ([C(4)mim]Cl)), and porous silica gel support, was investigated. The catalytic activity of the SILP catalyst toward RWGSR strongly depends on the kind of Ru catalyst and amount of IL. Among the three kinds of Ru catalysts ([RuCl2(CO)(3)](2), Ru-3(CO)(12), and RuC13), [RuCl2(CO)(3)](2) exhibits the best catalytic activity. Brunauer Emmett Teller (BET) surface area analysis and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analyses of the SILP catalyst based on [RuCl2(CO)(3)](2) and [C(4)mim]Cl revealed that both the solvation of the active catalytic Ru species and the surface area of the ionic liquid phase strongly affect catalytic activity. Hence, these factors help to determine the optimum amount of [C(4)mim]Cl in the SILP catalyst. The resulting SILP catalyst, with an optimum constitution, exhibited greater catalytic activity than the homogeneous system in which the same amounts of [RuCl2(CO)(3)](2) and [C(4)mim]Cl were employed. Catalytically active Ru species during RWGSR in both systems were investigated by means of electrospray ionization-mass spectrometry (ESI-MS). Interestingly, the rate-determining step in the two systems was different, implying that the silica support lowers the activation energy of the protonation reaction in the catalytic cycle. Therefore, the facilitation of the RWGSR by a SILP catalyst system can be realized by good mass transport, derived from the large surface area, as well as the effect of the silica support on activation energy. Furthermore, 20 cycles of the RWGSR using the SILP catalyst were accomplished.
Rights: © 2018. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/
https://creativecommons.org/licenses/by-nc-nd/4.0/
Type: article (author version)
URI: http://hdl.handle.net/2115/79275
Appears in Collections:触媒科学研究所 (Institute for Catalysis) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 安田 友洋

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