Rationally Designed Double-Shell Dodecahedral Microreactors with Efficient Photoelectron Transfer: N-Doped-C-Encapsulated Ultrafine In2O3 Nanoparticles |
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Authors: | Liming Sun Rong Li Wenwen Zhan Fan Wang Yuan Zhuang Xiaojun Wang Xiguang Han |
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Institution: | 1. Jiangsu Key Laboratory of Green Synthetic Chemistry for, Functional Materials, Department of Chemistry, School of, Chemistry and Materials Science, Jiangsu Normal University, Xuzhou, 221116 P. R. China
These authors contributed equally to this work.;2. Jiangsu Key Laboratory of Green Synthetic Chemistry for, Functional Materials, Department of Chemistry, School of, Chemistry and Materials Science, Jiangsu Normal University, Xuzhou, 221116 P. R. China |
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Abstract: | It is desirable but challenging to design efficient micro-/nanoreactors for chemical reactions. In this study, we have fabricated mesoporous double-shelled hollow microreactors composed of N-doped-C-coated ultrafine In2O3 nanoparticles N-C/In2O3 HD (hollow dodecahedron)] by the thermolysis of a dodecahedral In-based framework in Ar atmosphere. The obtained N-C/In2O3 HD exhibited excellent activity in the photocatalytic oxidative hydroxylation of a series of arylboronic acid substrates. This property can be attributed to its enhanced optical absorption and efficient separation of photo-generated electron–hole pairs, imparted by the unique structure and uniformly coated N-doped C layers. Furthermore, we found O2.− to be the critical active species in the process of photocatalytic oxidative hydroxylation of arylboronic acids, and the formation mechanism of this radical is also proposed. Theoretical calculations further confirmed that the N-doped C layer serves as an electron acceptor and revealed the microscopic charge-carrier migration path through the In2O3/N-doped graphite interfaces. Thus, photo-generated electrons from hybrid states of In2O3, composed of In 5s and 2p orbitals, are transferred into the hybrid states of N-doped graphite, composed of C 2p and N 2p orbitals. The present study may be helpful for understanding and designing carbon-based micro-/nanoreactors for photocatalytic reactions, and may also be useful for investigating related micro-/nanoreactors. |
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Keywords: | In2O3 mesoporous materials microreactor nanoparticles N-doped C photocatalysis |
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