Construction of N-doped copper metal-organic frameworks for promoting photocatalytic carbon dioxide reduction to ethylene  

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作  者:Fan Guo Zong-Zheng He Peng Wang Xiao-Yu Zhang Hongjian Yu Qin-Chao Wang Wei-Yin Sun 

机构地区:[1]School of Chemistry and Chemical Engineering,Yangzhou University,Yangzhou 225002,China [2]Coordination Chemistry Institute,State Key Laboratory of Coordination Chemistry,School of Chemistry and Chemical Engineering,Nanjing National Laboratory of Microstructures,Collaborative Innovation Center of Advanced Microstructures,Nanjing University,Nanjing 210023,China

出  处:《Science China Chemistry》2025年第2期601-609,共9页中国科学(化学英文版)

基  金:supported by the National Natural Science Foundation of China (22101246, 22231006, and 22171131);supported by a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions

摘  要:Engineering nonmetallic atom-doped metal-organic framework(MOF)catalyst to promote C−C coupling and realize conversion of CO_(2) into C_(2 )multi-carbon hydrocarbon products is still challenging.Herein,with 2-methylimidazole as a dopant of N element,an N-doped NH_(2)-CuBDC catalyst was obtained via a facile and simple stirring procedure.Upon illumination,compared with catalytic CO_(2) reduction to C1 product of CO by original MOF,N-doped NH_(2)-CuBDC can motivate generation of C_(2)H_(4),which is difficult to achieve in photocatalytic system by MOF-based catalysts.The transfer rates of photo-generated charges have been expedited due to the high electron density around Cu catalytic sites after N-doping.More importantly,C–C coupling intermediate CO–CHO*was identified by in situ Fourier transform infrared spectroscopy during the catalytic CO_(2) reduction reaction process,which further indicates the presence of Cu–N sites in the NH_(2)-CuBDC can facilitate the formation of C2H_(4) effectively.This work uncovers a new paradigm to design photocatalysts for enhancing the reduction of CO_(2) to C_(2) products.

关 键 词:metal-organic frameworks C-C coupling DOPING photocatalytic CO_(2) reduction Cu-based catalysts 

分 类 号:TQ221.211[化学工程—有机化工] O643.36[理学—物理化学] O644.1[理学—化学]

 

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