Sorbitol-derived carbon overlayers encapsulated Cu nanoparticles on SiO2: Stable and efficient for the continuous hydrogenation of ethylene carbonate

Summary: An ultrastable and efficient Cu@C/SiO2 nanocatalyst was fabricated for the hydrogenation of ethylene carbonate, in which Cu nanoparticles are encapsulated by sorbitol-derived graphitized carbon overlayers. During the calcination of Cu-sorbitol/SiO2 precursors under N2 atmosphere, sorbitol d...

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Main Authors: Tongyang Song, Yuanyuan Qi, Chen Zhao, Peng Wu, Xiaohong Li
Format: Article
Language:English
Published: Elsevier 2022-10-01
Series:iScience
Subjects:
Online Access:http://www.sciencedirect.com/science/article/pii/S2589004222015115
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author Tongyang Song
Yuanyuan Qi
Chen Zhao
Peng Wu
Xiaohong Li
author_facet Tongyang Song
Yuanyuan Qi
Chen Zhao
Peng Wu
Xiaohong Li
author_sort Tongyang Song
collection DOAJ
description Summary: An ultrastable and efficient Cu@C/SiO2 nanocatalyst was fabricated for the hydrogenation of ethylene carbonate, in which Cu nanoparticles are encapsulated by sorbitol-derived graphitized carbon overlayers. During the calcination of Cu-sorbitol/SiO2 precursors under N2 atmosphere, sorbitol decomposed to CO and CO2. The in situ generated CO not only reduced Cu2+ to Cu0/Cu+, but also formed graphitized carbon overlayers on the Cu surface via the disproportionation of CO. The Cu@C/SiO2 catalyst exhibited superior catalytic performance (91% MeOH yield and 43.6 h−1 TOF) at a H2/EC molar ratio of 20. Of particular note, the Cu@C/SiO2 catalyst showed remarkable long-term stability during 736 h time-on-stream test without any deactivation. The graphitized carbon overlayers on the surface of Cu nanoparticles not only functioned synergistically with the surface Cu0/Cu+ sites to promote the EC hydrogenation but also suppressed the sintering of Cu nanoparticles. Furthermore, the interaction of Cu nanoparticles and graphitized carbon overlayers stabilized the surface Cu+/(Cu0+Cu+) ratio.
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spelling doaj.art-8c763d140e504376b270d91fc19912652022-12-22T04:31:49ZengElsevieriScience2589-00422022-10-012510105239Sorbitol-derived carbon overlayers encapsulated Cu nanoparticles on SiO2: Stable and efficient for the continuous hydrogenation of ethylene carbonateTongyang Song0Yuanyuan Qi1Chen Zhao2Peng Wu3Xiaohong Li4Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan Rd, Shanghai 200062, ChinaShanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan Rd, Shanghai 200062, ChinaShanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan Rd, Shanghai 200062, China; Institute of Eco-Chongming, Shanghai 202162, ChinaShanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan Rd, Shanghai 200062, China; Institute of Eco-Chongming, Shanghai 202162, ChinaShanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan Rd, Shanghai 200062, China; Institute of Eco-Chongming, Shanghai 202162, China; Corresponding authorSummary: An ultrastable and efficient Cu@C/SiO2 nanocatalyst was fabricated for the hydrogenation of ethylene carbonate, in which Cu nanoparticles are encapsulated by sorbitol-derived graphitized carbon overlayers. During the calcination of Cu-sorbitol/SiO2 precursors under N2 atmosphere, sorbitol decomposed to CO and CO2. The in situ generated CO not only reduced Cu2+ to Cu0/Cu+, but also formed graphitized carbon overlayers on the Cu surface via the disproportionation of CO. The Cu@C/SiO2 catalyst exhibited superior catalytic performance (91% MeOH yield and 43.6 h−1 TOF) at a H2/EC molar ratio of 20. Of particular note, the Cu@C/SiO2 catalyst showed remarkable long-term stability during 736 h time-on-stream test without any deactivation. The graphitized carbon overlayers on the surface of Cu nanoparticles not only functioned synergistically with the surface Cu0/Cu+ sites to promote the EC hydrogenation but also suppressed the sintering of Cu nanoparticles. Furthermore, the interaction of Cu nanoparticles and graphitized carbon overlayers stabilized the surface Cu+/(Cu0+Cu+) ratio.http://www.sciencedirect.com/science/article/pii/S2589004222015115Nanoparticlesnanotechnology fabricationnanomaterials
spellingShingle Tongyang Song
Yuanyuan Qi
Chen Zhao
Peng Wu
Xiaohong Li
Sorbitol-derived carbon overlayers encapsulated Cu nanoparticles on SiO2: Stable and efficient for the continuous hydrogenation of ethylene carbonate
iScience
Nanoparticles
nanotechnology fabrication
nanomaterials
title Sorbitol-derived carbon overlayers encapsulated Cu nanoparticles on SiO2: Stable and efficient for the continuous hydrogenation of ethylene carbonate
title_full Sorbitol-derived carbon overlayers encapsulated Cu nanoparticles on SiO2: Stable and efficient for the continuous hydrogenation of ethylene carbonate
title_fullStr Sorbitol-derived carbon overlayers encapsulated Cu nanoparticles on SiO2: Stable and efficient for the continuous hydrogenation of ethylene carbonate
title_full_unstemmed Sorbitol-derived carbon overlayers encapsulated Cu nanoparticles on SiO2: Stable and efficient for the continuous hydrogenation of ethylene carbonate
title_short Sorbitol-derived carbon overlayers encapsulated Cu nanoparticles on SiO2: Stable and efficient for the continuous hydrogenation of ethylene carbonate
title_sort sorbitol derived carbon overlayers encapsulated cu nanoparticles on sio2 stable and efficient for the continuous hydrogenation of ethylene carbonate
topic Nanoparticles
nanotechnology fabrication
nanomaterials
url http://www.sciencedirect.com/science/article/pii/S2589004222015115
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AT yuanyuanqi sorbitolderivedcarbonoverlayersencapsulatedcunanoparticlesonsio2stableandefficientforthecontinuoushydrogenationofethylenecarbonate
AT chenzhao sorbitolderivedcarbonoverlayersencapsulatedcunanoparticlesonsio2stableandefficientforthecontinuoushydrogenationofethylenecarbonate
AT pengwu sorbitolderivedcarbonoverlayersencapsulatedcunanoparticlesonsio2stableandefficientforthecontinuoushydrogenationofethylenecarbonate
AT xiaohongli sorbitolderivedcarbonoverlayersencapsulatedcunanoparticlesonsio2stableandefficientforthecontinuoushydrogenationofethylenecarbonate