Visible-Light-Driven C–N Bond Formation by a Hexanickel Cluster Substituted Polyoxometalate-Based Photocatalyst
| Autor: | Jiachen Jiao, Qiuxia Han, Ming-Xue Li, Jie Li, Jiangnan Chang |
|---|---|
| Rok vydání: | 2021 |
| Předmět: |
010405 organic chemistry
Chemistry Electron donor 010402 general chemistry Photochemistry 01 natural sciences Pyrrolidine 0104 chemical sciences Inorganic Chemistry chemistry.chemical_compound Covalent bond Excited state Polyoxometalate Photocatalysis Proton NMR Photosensitizer Physical and Theoretical Chemistry |
| Zdroj: | Inorganic Chemistry. 60:10022-10029 |
| ISSN: | 1520-510X 0020-1669 |
| DOI: | 10.1021/acs.inorgchem.1c01311 |
| Popis: | A powerful and attractive route to develop novel photocatalysts for C-N bond formation involves the use of pyrrolidine as the substrate and cocatalyst simultaneously. Herein, a new polyoxometalate (POM)-based metal-organic framework, namely, [Ni6(OH)3(H2O)9(DPNDIH)(SiW9O34)]2·2H2O (SiW9Ni6-DPNDI) (DPNDI = N,N'-di(4-pyridyl)-1,4,5,8-naphthalenediimide), was prepared by incorporating a Ni6 cluster-substituted POM anion and a photosensitizer (DPNDI) into a framework. The anion···π interactions and covalent bonds between SiW9Ni6 and DPNDI are beneficial for the consecutive electron separation and transfer. Under visible-light irradiation, DPNDI can be easily excited to generate radical species DPNDI* that could be further excited in the presence of the electron donor pyrrolidine for the inert O2 activation. SiW9Ni6-DPNDI showed a high efficiency in the photocatalysis of C-N bond formation under a mild condition by the synergy of DPNDI and SiW9Ni6. The results of the reaction were confirmed by gas chromatography and 1H NMR. In addition, SiW9Ni6-DPNDI exhibited a high sustainability without an obvious change in yields after five cycles. |
| Databáze: | OpenAIRE |
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