Citation: Nian Hu, Xiao-Yun Li, Si-Ming Liu, Zhao Wang, Xiao-Ke He, Yue-Xin Hou, Yu-Xiang Wang, Zhao Deng, Li-Hua Chen, Bao-Lian Su. Enhanced stability of highly-dispersed copper catalyst supported by hierarchically porous carbon for long term selective hydrogenation[J]. Chinese Journal of Catalysis, ;2020, 41(7): 1081-1090. doi: 10.1016/S1872-2067(20)63570-7 shu

Enhanced stability of highly-dispersed copper catalyst supported by hierarchically porous carbon for long term selective hydrogenation

Nian Hu ^a, ,
Xiao-Yun Li ^b ,
Si-Ming Liu ^a ,
Zhao Wang ^a ,
Xiao-Ke He ^a ,
Yue-Xin Hou ^a ,
Yu-Xiang Wang ^a ,
Zhao Deng ^a ,
Li-Hua Chen ^a ,
Bao-Lian Su ^a,c,d

a Laboratory of Living Materials, the State Key Laboratory of Advanced Technology for Material Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, Hubei, China;
b State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, Hubei, China;
c Laboratory of Inorganic Materials Chemistry (CMI), University of Namur, B-5000 Namur, Belgium;
d Clare Hall, University of Cambridge, Cambridge CB3 9AL

Received Date: 26 November 2019

Fund Project: This work was supported by Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52) of the Chinese Ministry of Education. B. L. Su acknowledges the Chinese Ministry of Education for a “Changjiang Chaire Professor” position and a Clare Hall Life Membership, University of Cambridge. L. H. Chen acknowledges Hubei Provincial Department of Education for the “Chutian Scholar” program. This work was also financially supported by the National Natural Science Foundation of China (21671155, U1663225, 21902122, 21805216), Major programs of technical innovation in Hubei (2018AAA012), Hubei Provincial Natural Science Foundation (2018CFA054), Postdoctoral Science Foundation of China (2019M652723), and the Fundamental Research Funds for the Central Universities (2019IVA116).

Copper based catalysts have high potential for the substituent of noble-metal based catalysts as their high selectivity and moderate activity for selective hydrogenation reaction; however, achieving further high catalytic stability is very difficult. In this work, the carbonization process of Cu-based organic frameworks was explored for the synthesis of highly-dispersed Cu supported by hierarchically porous carbon with high catalytic performance for selective hydrogenation of 1,3-butadiene. The porous hierarchy of carbon support and the dispersion of copper nanoparticles can be precisely tuned by controlling the carbonization process. The resultant catalyst carbonized at 600 ℃ exhibits a rather low reaction temperature at 75 ℃ for 100% butadiene conversion with 100% selectivity to butenes, due to its reasonable porous hierarchy and highly-dispersed copper sites. More importantly, unprecedentedly stability of the corresponding Cu catalyst was firstly observed for selective 1,3-butadiene hydrogenation, with both 100% butadiene conversion and 100% butenes selectivity over 120 h of reaction at 75 ℃. This study verifies that a simply control the carbonization process of metal organic frameworks can be an effective way to obtain Cu-based catalysts with superior catalytic performance for selective hydrogenation reaction.
- Hierarchically porous structure,
- Catalyst,
- Cu/C,
- Selective hydrogenation,
- Metal organic frameworks
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