Catalytic Semi-Water-Gas Shift Reaction: A Simple Green Path to Formic Acid Fuel.

Autor: Qadir MI; Institute of Chemistry, Universidade Federal do Rio Grande do Sul, Av. Bento Gonçalves, 9500, Porto Alegre, 91501-970, RS, Brazil., Castegnaro MV; Institute of Physics, Federal University of Rio Grande do Sul, Campus Agronomia, Porto Alegre, 90650-001, Brazil., Selau FF; Institute of Physics, Federal University of Rio Grande do Sul, Campus Agronomia, Porto Alegre, 90650-001, Brazil., Samperi M; School of Chemistry, University of Nottingham, University Park, Nottingham, NG7 2RD, United Kingdom., Fernandes JA; School of Chemistry, University of Nottingham, University Park, Nottingham, NG7 2RD, United Kingdom., Morais J; Institute of Physics, Federal University of Rio Grande do Sul, Campus Agronomia, Porto Alegre, 90650-001, Brazil., Dupont J; Institute of Chemistry, Universidade Federal do Rio Grande do Sul, Av. Bento Gonçalves, 9500, Porto Alegre, 91501-970, RS, Brazil.
Jazyk: angličtina
Zdroj: ChemSusChem [ChemSusChem] 2020 Apr 07; Vol. 13 (7), pp. 1817-1824. Date of Electronic Publication: 2020 Mar 17.
DOI: 10.1002/cssc.201903417
Abstrakt: Formic acid (FA) is a promising CO and hydrogen energy carrier, and currently its generation is mainly centered on the hydrogenation of CO 2 . However, it can also be obtained by the hydrothermal conversion of CO with H 2 O at very high pressures (>100 bar) and temperatures (>200 °C), which requires days to complete. Herein, it is demonstrated that by using a nano-Ru/Fe alloy embedded in an ionic liquid (IL)-hybrid silica in the presence of the appropriate IL in water, CO can be catalytically converted into free FA (0.73 m) under very mild reactions conditions (10 bar at 80 °C) with a turnover number of up to 1269. The catalyst was prepared by simple reduction/decomposition of Ru and Fe complexes in the IL, and it was then embedded into an IL-hybrid silica {1-n-butyl-3-(3-trimethoxysilylpropyl)-imidazolium cations associated with hydrophilic (acetate, SILP-OAc) and hydrophobic [bis((trifluoromethyl)sulfonyl)amide, SILP-NTf 2 ] anions}. The location of the alloy nanoparticles on the support is strongly related to the nature of the anion, that is, in the case of hydrophilic SILP-OAc, RuFe nanoparticles are more exposed to the support surface than in the case of the hydrophobic SILP-NTf 2 , as determined by Rutherford backscattering spectrometry. This catalytic membrane in the presence of H 2 O/CO and an appropriate IL, namely, 1,2-dimethyl-3-n-butylimidazolium 2-methyl imidazolate (BMMIm⋅MeIm), is stable and recyclable for at least five runs, yielding a total of 4.34 m of free FA.
(© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)
Databáze: MEDLINE
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