Résumé
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 °C exhibits a rather low reaction temperature at 75 °C 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 °C. 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.
langue originale | Anglais |
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Pages (de - à) | 1081-1090 |
Nombre de pages | 10 |
journal | Chinese Journal of Catalysis |
Volume | 41 |
Numéro de publication | 7 |
Les DOIs | |
Etat de la publication | Publié - juil. 2020 |
Financement
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).
Bailleurs de fonds | Numéro du bailleur de fonds |
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Hubei Provincial Department of Education | |
University of Cambridge | |
National Natural Science Foundation of China | 21805216, 2018AAA012, U1663225, 21902122, 21671155 |
Ministry of Education of the People's Republic of China | |
China Postdoctoral Science Foundation | 2019M652723 |
Natural Science Foundation of Hubei Province | 2018CFA054 |
Fundamental Research Funds for the Central Universities | 2019IVA116 |
Program for Changjiang Scholars and Innovative Research Team in University | IRT_15R52 |
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