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Nano Research 2022, 15(8): 7034-7041 https://doi.org/10.1007/s12274-022-4357-8
Research Article | Issue | Published: 02 May 2022

Constructing the separation pathway for photo-generated carriers by diatomic sites decorated on MIL-53-NH2(Al) for enhanced photocatalytic performance

Show Author's Information Gang Wang1,§,  Yan Liu1,§,  Ning Zhao1,§,  Huimei Chen1,  Wenjie Wu1,  Yueyue Li1,  Xiangwen Liu2,  Ang Li3,  Wenxing Chen4,  Junjie Mao1( )
Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, China
Institute of Analysis and Testing, Beijing Academy of Science and Technology (Beijing Center for Physical and Chemical Analysis), Beijing 100094, China
Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing 100124, China
Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China

§ Gang Wang, Yan Liu, and Ning Zhao contributed equally to this work.

Keywords:
photocatalysis, charge-carrier dynamics, benzene oxidation, diatomic sites, MIL-53-NH2
Topics:
Photocatalytic activity
Cite this article:
Wang G, Liu Y, Zhao N, et al. Constructing the separation pathway for photo-generated carriers by diatomic sites decorated on MIL-53-NH2(Al) for enhanced photocatalytic performance. Nano Research, 2022, 15(8): 7034-7041. https://doi.org/10.1007/s12274-022-4357-8
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Abstract Full text Electronic supplementary material About this article

High yield production of phenol from hydroxylation of benzene with low energy consumption is of paramount importance, but still challenging. Herein, a new strategy, consisting of using diatomic synergistic modulation (DSM) to effectively control the separation of photo-generated carriers for an enhanced production of phenol is reported. The atomic level dispersion of Fe and Cr respectively decorated on Al based MIL-53-NH2 photocatalyst (Fe1/Cr:MIL-53-NH2) is designed, in which Cr single atoms are substituted for Al3+ while Fe single atoms are coordinated by N. Notably, the Fe1/Cr:MIL-53-NH2 significantly boosts the photo-oxidation of benzene to phenol under visible light irradiation, which is much higher than those of MIL-53-NH2, Cr:MIL-53-NH2, Fe1/MIL-53-NH2, and Fe nanoparticles/Cr:MIL-53-NH2 catalysts. Theoretical and experimental results reveal that the Cr single atoms and Fe single atoms can act as electron acceptor and electron donor, respectively, during photocatalytic reaction, exhibiting a synergistic effect on the separation of the photo-generated carriers and thereby causing great enhancement on the benzene oxidation. This strategy provides new insights for rational design of advanced photocatalysts at the atomic level.


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Electronic supplementary material
About this article

Constructing the separation pathway for photo-generated carriers by diatomic sites decorated on MIL-53-NH2(Al) for enhanced photocatalytic performance

Show Author's information Gang Wang1,§, Yan Liu1,§, Ning Zhao1,§, Huimei Chen1, Wenjie Wu1, Yueyue Li1, Xiangwen Liu2, Ang Li3, Wenxing Chen4, Junjie Mao1( )
Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, China
Institute of Analysis and Testing, Beijing Academy of Science and Technology (Beijing Center for Physical and Chemical Analysis), Beijing 100094, China
Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing 100124, China
Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China

§ Gang Wang, Yan Liu, and Ning Zhao contributed equally to this work.

Abstract

High yield production of phenol from hydroxylation of benzene with low energy consumption is of paramount importance, but still challenging. Herein, a new strategy, consisting of using diatomic synergistic modulation (DSM) to effectively control the separation of photo-generated carriers for an enhanced production of phenol is reported. The atomic level dispersion of Fe and Cr respectively decorated on Al based MIL-53-NH2 photocatalyst (Fe1/Cr:MIL-53-NH2) is designed, in which Cr single atoms are substituted for Al3+ while Fe single atoms are coordinated by N. Notably, the Fe1/Cr:MIL-53-NH2 significantly boosts the photo-oxidation of benzene to phenol under visible light irradiation, which is much higher than those of MIL-53-NH2, Cr:MIL-53-NH2, Fe1/MIL-53-NH2, and Fe nanoparticles/Cr:MIL-53-NH2 catalysts. Theoretical and experimental results reveal that the Cr single atoms and Fe single atoms can act as electron acceptor and electron donor, respectively, during photocatalytic reaction, exhibiting a synergistic effect on the separation of the photo-generated carriers and thereby causing great enhancement on the benzene oxidation. This strategy provides new insights for rational design of advanced photocatalysts at the atomic level.

Keywords: photocatalysis, charge-carrier dynamics, benzene oxidation, diatomic sites, MIL-53-NH2

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Publication history
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Acknowledgements

Publication history

Received: 03 March 2022
Revised: 22 March 2022
Accepted: 22 March 2022
Published: 02 May 2022
Issue date: August 2022

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 21971002), and the Natural Science Foundation of Anhui Province (Nos. 1908085QB45 and 2008085QB81). The calculations in this paper have been done on the supercomputing system of the National Supercomputing Center in Changsha. The authors thank the BL1W1B in the Beijing Synchrotron Radiation Facility (BSRF), BL14W1 in the Shanghai Synchrotron Radiation Facility (SSRF), BL10B and BL12B in the National Synchrotron Radiation Laboratory (NSRL) for help with characterizations.

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