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

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

作     者:Zhi-Hao Yan Bo Ma Shu-Rong Li Junxue Liu Rong Chen Ming-Hao Du Shengye Jin Gui-Lin Zhuang La-Sheng Long Xiang-Jian Kong Lan-Sun Zheng 

作者机构: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 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 College of Chemical Engineering Zhejiang University of Technology Hangzhou 310032 China 

出 版 物:《Science Bulletin》 (科学通报(英文版))

年 卷 期:2019年第64卷第14期

页      面:976-985页

核心收录:

学科分类:07[理学] 08[工学] 

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) 

主  题:Metal-organic frameworks CO2 reduction Transient absorption Photocatalysis DFT calculations 

摘      要:Photocatalytic reduction of CO2 to CO is a promising strategy for reducing atmospheric CO2 levels and storing solar radiation as chemical ***,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 *** 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 *** mechanistic insights into photoreduction of CO2 have been studied based on thermodynamical,electrochemical,and spectroscopic investigation,together with density functional theory(DFT)*** work shows that encapsulating molecular catalyst into photoactive MOF highlights opportunities for designing efficient,stable and recyclable photocatalysts.

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