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Selective Carbon Dioxide Hydrogenation Driven by Ferromagnetic RuFe Nanoparticles in Ionic Liquids

Qadir, Muhammad I.; Weilhard, Andreas; Fernandes, Jesum A.; de Pedro, Imanol; Vieira, Bruno J. C.; Waerenborgh, Jo�o C.; Dupont, Jairton

Authors

Muhammad I. Qadir

Imanol de Pedro

Bruno J. C. Vieira

Jo�o C. Waerenborgh

Jairton Dupont



Abstract

© 2018 American Chemical Society. CO2 is selectively hydrogenated to HCO2H or hydrocarbons (HCs) by RuFe nanoparticles (NPs) in ionic liquids (ILs) under mild reaction conditions. The generation of HCO2H occurs in ILs containing basic anions, whereas heavy HCs (up to C21 at 150 °C) are formed in the presence of ILs containing nonbasic anions. Remarkably, high values of TONs (400) and a TOF value of 23.52 h-1 for formic acid with a molar ratio of 2.03 per BMI·OAc IL were obtained. Moreover, these NPs exhibited outstanding abilities in the formation of long-chain HCs with efficient catalytic activity (12% conversion) in a BMI·NTf2 hydrophobic IL. The IL forms a cage around the NPs that controls the diffusion/residence time of the substrates, intermediates, and products. The distinct CO2 hydrogenation pathways (HCO2H or FT via RWGS) catalyzed by the RuFe alloy are directly related to the basicity and hydrophobicity of the IL ion pair (mainly imposed by the anion) and the composition of the metal alloy. The presence of Fe in the RuFe alloy provides enhanced catalytic performance via a metal dilution effect for the formation of HCO2H and via a synergistic effect for the generation of heavy HCs.

Journal Article Type Article
Acceptance Date Jan 4, 2018
Online Publication Date Jan 24, 2018
Publication Date Feb 2, 2018
Deposit Date Dec 4, 2018
Journal ACS Catalysis
Electronic ISSN 2155-5435
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 8
Issue 2
Pages 1621-1627
DOI https://doi.org/10.1021/acscatal.7b03804
Public URL https://nottingham-repository.worktribe.com/output/1363368
Publisher URL https://pubs.acs.org/doi/10.1021/acscatal.7b03804