期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 10, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202114538
关键词
Electrocatalysis; Electropolymerization; Metal Nanoclusters; Nitrate Reduction; Photocatalysis
资金
- National Natural Science Foundation of China [21825106, 92061201, 21905254, 21901234]
- Central Plains Academician Fund of Henan Province [22180017]
- Henan Science Fund for Excellent Young Scholars [212300410084]
- China Postdoctoral Science Foundation [2020 M682332, 2021T140614]
- Henan Postdoctoral Foundation [202003015]
- Program for Innovative Research Team (in Science and Technology) in Universities of Henan Province [19IRTSTHN022]
- Zhengzhou University
Polymerized metal-cluster hybrid materials prepared by electropolymerization show enhanced catalytic performance due to improved electron-transfer ability and long-term recyclability compared to isolated metal clusters.
Atomically precise metal clusters are attractive as highly efficient catalysts, but suffer from continuous efficiency deactivation in the catalytic process. Here, we report the development of an efficient strategy that enhances catalytic performance by electropolymerization (EP) of metal clusters into hybrid materials. Based on carbazole ligand protection, three polymerized metal-cluster hybrid materials, namely Poly-Cu(14)cba, Poly-Cu(6)Au(6)cbz and Poly-Cu(6)Ag(4)cbz, were prepared. Compared with isolated metal clusters, metal clusters immobilizing on a biscarbazole network after EP significantly improved their electron-transfer ability and long-term recyclability, resulting in higher catalytic performance. As a proof-of-concept, Poly-Cu(14)cba was evaluated as an electrocatalyst for reducing nitrate (NO3-) to ammonia (NH3), which exhibited approximate to 4-fold NH3 yield rate and approximate to 2-fold Faraday efficiency enhancement compared to that of Cu(14)cba with good durability. Similarly, Poly-Cu(6)Au(6)cbz showed 10 times higher photocatalytic efficiency towards chemical warfare simulants degradation than the cluster counterpart.
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