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

被引:30
作者
Hu, Nian [1 ]
Li, Xiao-Yun [2 ]
Liu, Si-Ming [1 ]
Wang, Zhao [1 ]
He, Xiao-Ke [1 ]
Hou, Yue-Xin [1 ]
Wang, Yu-Xiang [1 ]
Deng, Zhao [1 ]
Chen, Li-Hua [1 ]
Su, Bao-Lian [1 ,3 ,4 ]
机构
[1] Wuhan Univ Technol, Lab Living Mat, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Hubei, Peoples R China
[2] Wuhan Univ Technol, State Key Lab Silicate Mat Architectures, Wuhan 430070, Hubei, Peoples R China
[3] Univ Namur, Lab Inorgan Mat Chem CMI, B-5000 Namur, Belgium
[4] Univ Cambridge, Clare Hall, Cambridge CB3 9AL, England
基金
中国国家自然科学基金;
关键词
Hierarchically porous structure; Catalyst; Cu/C; Selective hydrogenation; Metal organic frameworks; METAL-ORGANIC-FRAMEWORK; OXIDE NANOPARTICLES; PD NANOPARTICLES; 1,3-BUTADIENE; SINGLE; PALLADIUM; ALLOY; IDENTIFICATION; TRANSFORMATION; PERFORMANCE;
D O I
10.1016/S1872-2067(20)63570-7
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
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 degrees C exhibits a rather low reaction temperature at 75 degrees 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 degrees 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. (C) 2020, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
引用
收藏
页码:1081 / 1090
页数:10
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