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

Abstract

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

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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, Accepted Manuscript
Article type
Paper

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

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

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