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

被引:5
|
作者
Zhi-Hao Yan [1 ]
Bo Ma [1 ]
Shu-Rong Li [1 ]
Junxue Liu [2 ]
Rong Chen [1 ]
Ming-Hao Du [1 ]
Shengye Jin [2 ]
Gui-Lin Zhuang [3 ]
La-Sheng Long [1 ]
Xiang-Jian Kong [1 ]
Lan-Sun Zheng [1 ]
机构
[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
[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
[3] College of Chemical Engineering,Zhejiang University of Technology
基金
中国国家自然科学基金; 中央高校基本科研业务费专项资金资助;
关键词
Metal-organic frameworks; CO2; reduction; Transient absorption; Photocatalysis; DFT calculations;
D O I
暂无
中图分类号
O643.36 [催化剂]; O644.1 [光化学]; X701 [废气的处理与利用];
学科分类号
070304 ; 081704 ; 081705 ; 083002 ;
摘要
Photocatalytic reduction of COto CO is a promising strategy for reducing atmospheric COlevels and storing solar radiation as chemical energy.Here,we demonstrate that a molecular catalyst[Ni(bpet)(HO)]successfully encapsulated into a highly robust and visible-light responsive metal–organic framework(Ru-UiO-67)to fabricate composite catalysts for photocatalytic COreduction.The composite Ni@Ru-UiO-67 photocatalysts show efficient visible-light-driven COreduction 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 COhave 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.
引用
收藏
页码:976 / 985
页数:10
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