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Sonochemical engineering of highly efficient and robust Au nanoparticle-wrapped on Fe/ZrO2 nanorods and their controllable product selectivity in dimethyl oxalate hydrogenation

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Abstract

Considerable attention has been paid in last few years to the environmentally-benign hydrogenation reaction of dimethyl oxalate (DMO) to produce methyl glycolate (MG), ethylene glycol (EG) and ethanol (EtOH). Cu-Based composites and noble-metal promoted Cu-materials have been reported as highly efficient catalysts in DMO hydrogenation. In this study, for the first time, a Cu-free Fe/ZrO2 nanorod catalyst with a highly crystalline structure was synthesized in the absence of any toxic materials and through a one-pot sonochemical approach and used without the calcination step as a robust catalyst in DMO hydrogenation to produce a high EtOH yield of 94.4%. Furthermore, to control the product distribution in this multistep DMO hydrogenation and achieve a high MG selectivity of 95%, highly dispersed Au nanoparticles were nicely decorated on the surface of the Fe/ZrO2 nanorod catalyst by a facile sonochemical route which was used as a highly efficient catalyst. Moreover, the produced catalysts displayed high stability properties for a period of at least 300 h with maintained high catalytic activity. Interestingly, X-ray diffraction results for the spent catalysts demonstrated that Hägg iron carbide (Fe5C2) is the active phase for the production of ethanol using the Fe/ZrO2 catalyst, while the XPS results exhibited that the co-existence of the three oxidation states of metallic Au (Au+, Au0, and Au3+) plays the key role as the active species for the synthesis of MG with high selectivity using the Au/Fe/ZrO2 catalyst.

Graphical abstract: Sonochemical engineering of highly efficient and robust Au nanoparticle-wrapped on Fe/ZrO2 nanorods and their controllable product selectivity in dimethyl oxalate hydrogenation

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Supplementary files

Article information


Submitted
06 Dec 2019
Accepted
05 Jan 2020
First published
07 Jan 2020

Catal. Sci. Technol., 2020, Advance Article
Article type
Paper

Sonochemical engineering of highly efficient and robust Au nanoparticle-wrapped on Fe/ZrO2 nanorods and their controllable product selectivity in dimethyl oxalate hydrogenation

M. Abbas, J. Zhang and J. Chen, Catal. Sci. Technol., 2020, Advance Article , DOI: 10.1039/C9CY02469G

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