Efficient Visible-Light-Driven Carbon Dioxide Reduction by a Single-Atom Implanted Metal-Organic Framework

被引：732

作者：

Zhang, Huabin ^{[1
]}

Wei, Jing ^{[4
]}

Dong, Juncai ^{[5
]}

Liu, Guigao ^{[1
]}

Shi, Li ^{[1
]}

An, Pengfei ^{[5
]}

Zhao, Guixia ^{[1
]}

Kong, Jintao ^{[4
]}

Wang, Xiaojun ^{[1
]}

Meng, Xianguang ^{[1
]}

Zhang, Jing ^{[5
]}

Ye, Jinhua ^{[1
,2
,3
]}

机构：

[1] Natl Inst Mat Sci, Int Ctr Mat Nanoarchitecton WPI MANA, 1-1 Namiki, Tsukuba, Ibaraki 3050044, Japan

[2] Tianjin Univ, Sch Mat Sci & Engn, TU NIMS Joint Res Ctr, Tianjin 300072, Peoples R China

[3] Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China

[4] Chinese Acad Sci, Fujian Inst Res Struct Matter, Fuzhou 350002, Peoples R China

[5] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2016年 / 55卷 / 46期

关键词：

active sites; CO2; reduction; heterogeneous catalysis; photocatalysis; solar-energy conversion; PHOTOCATALYTIC CO2 REDUCTION; WATER OXIDATION; HIGHLY EFFICIENT; CATALYSTS; PERFORMANCE; COBALT; MOFS;

D O I：

10.1002/anie.201608597

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Modular optimization of metal-organic frameworks (MOFs) was realized by incorporation of coordinatively unsaturated single atoms in a MOF matrix. The newly developed MOF can selectively capture and photoreduce CO2 with high efficiency under visible-light irradiation. Mechanistic investigation reveals that the presence of single Co atoms in the MOF can greatly boost the electron-hole separation efficiency in porphyrin units. Directional migration of photogenerated excitons from porphyrin to catalytic Co centers was witnessed, thereby achieving supply of long-lived electrons for the reduction of CO2 molecules adsorbed on Co centers. As a direct result, porphyrin MOF comprising atomically dispersed catalytic centers exhibits significantly enhanced photocatalytic conversion of CO2, which is equivalent to a 3.13-fold improvement in CO evolution rate (200.6 mu mol g(-1) h(-1)) and a 5.93-fold enhancement in CH4 generation rate (36.67 mu mol g(-1) h(-1)) compared to the parent MOF.

引用

页码：14308 / 14312

页数：5

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