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Research Article

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

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.

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Graphical Abstract

A diatomic synergistic modulation (DSM) strategy was developed to effectively control the separation of photo-generated carriers. Theoretical and experimental results reveal that the diatomic sites of Cr and Fe act as electron acceptor and electron donor, respectively, and then enhance the photocatalytic activity.

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

diatomic sitesMIL-53-NH2charge-carrier dynamicsphotocatalysisbenzene oxidation

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Nano Research
Volume 15 Issue 8,
August 2022
Pages 7034-7041
DOI: 10.1007/s12274-022-4357-8
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
Topics:
Photocatalytic activity

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Received: 03 March 2022
Revised: 22 March 2022
Accepted: 22 March 2022
Published: 02 May 2022
© Tsinghua University Press 2022
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