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Shape and size controlled synthesis of Cu nanoparticles-wrapped on RGO nanosheet catalyst and their outstanding stability and catalytic performance in the hydrogenation reaction of dimethyl oxalate

Abstract

Considerable interest has been paid in the last few years for the important environmental-benign catalytic hydrogenation reaction of dimethyl oxalate (DMO) to produce methyl glycolate (MG), ethylene glycol (EG) and ethanol (ETOH). SiO2-supported noble metal elements such as Au, Ag and Ru have been nominated as efficient catalysts for the production of high MG selectivity. In this work, noble-metal free, Cu nanoparticles-wrapped on RGO nanosheets were synthesized using green in-situ sonochemical method in aqueous medium and then applied without the calcination step as robust catalyst in DMO hydrogenation reaction. Moreover, the effect of ultrasound (US), ammonia (NH4OH), combine both of US and NH4OH, and Cu loading (10, 25 and 45 wt%) on the morphology and catalytic performance of the produced Cu/RGO catalysts were studied in details. Interstingly, transmission electron microscopy images revealed that a dramatically morphology evolution of cu catalysts from ultra small dots to elongated and leaf-like nanoparticles shapes were produced, depending on the simple modifications of the reaction parameters. Notably, the obtained catalytic results demonstrated that among the different produced six catalysts, the prepared Cu/RGO catalyst using 20 KHz of ultrasound and in presence of ammonia within 25 wt% of Cu loading displayed the highest MG selectivity (98.8%) at relatively low reaction temperature (210ºC), however, the synthesized Cu/RGO catalyst within 45 wt% of Cu loading exhibited the highest ETOH selectivity (94%) at 240 ºC. Moreover, both catalysts showed long term stability of at least 300 h within maintained high DMO conversion and selectivity ratio. The comprehensive characterization to the as-prepared, reduced and spent catalysts concluded that the synergistic ratio of Cu+/(Cu++Cu0), the highly dispersion of Cu nanoparticles, the defective edges, sites and electron transfer provided from RGO are the main reasons for the such superior catalytic activity and long term stability.

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Supplementary files

Publication details

The article was received on 30 Jul 2018, accepted on 11 Sep 2018 and first published on 13 Sep 2018


Article type: Paper
DOI: 10.1039/C8TA07371F
Citation: J. Mater. Chem. A, 2018, Accepted Manuscript
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    Shape and size controlled synthesis of Cu nanoparticles-wrapped on RGO nanosheet catalyst and their outstanding stability and catalytic performance in the hydrogenation reaction of dimethyl oxalate

    M. Abbas, C. Zheng and J. Chen, J. Mater. Chem. A, 2018, Accepted Manuscript , DOI: 10.1039/C8TA07371F

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