Stable Heterometallic Cluster-Based Organic Framework Catalysts for Artificial Photosynthesis

被引：218

作者：

Dong, Long-Zhang ^{[1
]}

Zhang, Lei ^{[1
]}

Liu, Jiang ^{[1
]}

Huang, Qing ^{[1
]}

Lu, Meng ^{[1
]}

Ji, Wen-Xin ^{[2
]}

Lan, Ya-Qian ^{[1
]}

机构：

[1] Nanjing Normal Univ, Sch Chem & Mat Sci, Jiangsu Key Lab New Power Batteries, Jiangsu Collaborat Innovat Ctr Biomed Funct Mat, 1 Wenyuan Rd, Nanjing 210023, Peoples R China

[2] Ningxia Univ, State Key Lab High Efficiency Coal Utilizat & Gre, Yinchuan 750021, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2020年 / 59卷 / 07期

基金：

中国博士后科学基金;

关键词：

carbon dioxide reduction; heterometallic catalysts; metal-organic frameworks; photocatalysts; PHOTOCATALYTIC CO2 REDUCTION; METAL; CONVERSION; PHOTOREDUCTION;

D O I：

10.1002/anie.201913284

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

A series of stable heterometallic Fe2M cluster-based MOFs (NNU-31-M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO2 and H2O into HCOOH and O-2 without the assistance of additional sacrificial agent and photosensitizer. The heterometallic cluster units and photosensitive ligands excited by visible light generate separated electrons and holes. Then, low-valent metal M accepts electrons to reduce CO2, and high-valent Fe uses holes to oxidize H2O. This is the first MOF photocatalyst system to finish artificial photosynthetic full reaction. It is noted that NNU-31-Zn exhibits the highest HCOOH yield of 26.3 mu mol g(-1) h(-1) (selectivity of ca. 100 %). Furthermore, the DFT calculations based on crystal structures demonstrate the photocatalytic reaction mechanism. This work proposes a new strategy for how to design crystalline photocatalyst to realize artificial photosynthetic overall reaction.

引用

页码：2659 / 2663

页数：5

共 31 条

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