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Encapsulating a Ni(Ⅱ) molecular catalyst in photoactive metal–organic framework for highly efficient photoreduction of CO2

查看全文 作　　者：Zhi-Hao [1]Yan;Bo [1]Ma;Shu-Rong [1]Li;Junxue [2]Liu;Rong [1]Chen;Ming-Hao [1]Du;Shengye [2]Jin;Gui-Lin [3]Zhuang;La-Sheng [1]Long;Xiang-Jian [1]Kong;Lan-Sun [1]Zheng 高影响力作者 机构地区：[1]Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surface and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;[2]State Key Laboratory of Molecular Reaction Dynamics and Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;[3]College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, China高影响力机构 出　　处：《Science Bulletin》索引2019年第64卷第14期,共10页高影响力期刊 基　　金：supported by the National Natural Science Foundation of China (21871224, 21673184, 21431005, and 21390391);the Fok Ying Tong Education Foundation (151013);the Fundamental Research Funds for the Central Universities (20720180032) 摘　　要：Photocatalytic reduction of CO2 to CO is a promising strategy for reducing atmospheric CO2 levels and storing solar radiation as chemical energy.Here,we demonstrate that a molecular catalyst[NiⅡ(bpet)(H2O)2]successfully encapsulated into a highly robust and visible-light responsive metal–organic framework(Ru-UiO-67)to fabricate composite catalysts for photocatalytic CO2 reduction.The composite Ni@Ru-UiO-67 photocatalysts show efficient visible-light-driven CO2 reduction to CO with a TON of 581 and a selectivity of 99% after 20-h illumination,because of the facile electron transfer from Ru-photosensitizer to Ni(Ⅱ)active sites in Ni@Ru-UiO-67 system.The mechanistic insights into photoreduction of CO2 have been studied based on thermodynamical,electrochemical,and spectroscopic investigation,together with density functional theory(DFT)calculations.This work shows that encapsulating molecular catalyst into photoactive MOF highlights opportunities for designing efficient,stable and recyclable photocatalysts. 关 键 词：METAL-ORGANIC frameworks CO2 reduction TRANSIENT absorption PHOTOCATALYSIS DFT CALCULATIONS
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