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具有瞬态金属中心的金属有机框架用于增强光催化活性。

MOFs Conferred with Transient Metal Centers for Enhanced Photocatalytic Activity.

作者信息

Chen Xiaolang, Xiao Shuning, Wang Hao, Wang Wenchao, Cai Yong, Li Guisheng, Qiao Minghua, Zhu Jian, Li Hexing, Zhang Dieqing, Lu Yunfeng

机构信息

Key Laboratory of Resource Chemistry of Ministry of Education, Shanghai Key Laboratory of Rare Earth Functional Materials, College of Chemistry and Materials Science, Shanghai Normal University, Shanghai, 200234, P. R. China.

Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200433, China.

出版信息

Angew Chem Int Ed Engl. 2020 Sep 21;59(39):17182-17186. doi: 10.1002/anie.202002375. Epub 2020 Jul 27.

Abstract

Highly effective photocatalysts for the hydrogen-evolution reaction were developed by conferring the linkers of NH -MIL-125(Ti), a metal-organic framework (MOF) constructed from TiO clusters and 2-aminoterephthalic acid (linkers), with active copper centers. This design enables effective transfer of electrons from the linkers to the transient Cu /Cu centers, leading to 7000-fold and 27-fold increase of carrier density and lifetime of photogenerated charges, respectively, as well as high-rate production of H under visible-light irradiation. This work provides a novel design of a photocatalyst for hydrogen evolution using non-noble Cu /Cu as co-catalysts.

摘要

通过将NH -MIL-125(Ti)(一种由TiO簇和2-氨基对苯二甲酸(连接体)构建的金属有机框架(MOF))的连接体赋予活性铜中心,开发出了用于析氢反应的高效光催化剂。这种设计能够使电子从连接体有效地转移到瞬态Cu⁺/Cu²⁺中心,分别导致载流子密度增加7000倍和光生电荷寿命延长27倍,以及在可见光照射下高速率产氢。这项工作提供了一种使用非贵金属Cu⁺/Cu²⁺作为共催化剂的析氢光催化剂的新颖设计。

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