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Sorbitol-derived carbon overlayers encapsulated Cu nanoparticles on SiO2: Stable and efficient for the continuous
Tongyang Song1, Yuanyuan Qi1, Chen Zhao1,2
1Shanghai 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.
Abstract:
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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