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

Gang Wang; Yan Liu; Ning Zhao; Huimei Chen; Wenjie Wu; Yueyue Li; Xiangwen Liu; Ang Li; Wenxing Chen; Junjie Mao

doi:10.1007/s12274-022-4357-8

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

Gang Wang, Yan Liu, Ning Zhao, Huimei Chen, Wenjie Wu, Yueyue Li, Xiangwen Liu, Ang Li, Wenxing Chen, Junjie Mao^*

^*Corresponding author for this work

School of Material Science and Engineering

Research output: Contribution to journal › Article › peer-review

12 Citations (Scopus)

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. [Figure not available: see fulltext.]

Original language	English
Pages (from-to)	7034-7041
Number of pages	8
Journal	Nano Research
Volume	15
Issue number	8
DOIs	https://doi.org/10.1007/s12274-022-4357-8
Publication status	Published - Aug 2022

Keywords

MIL-53-NH
benzene oxidation
charge-carrier dynamics
diatomic sites
photocatalysis

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1007/s12274-022-4357-8

Cite this

@article{56865f5b55784af6bee074dd5adbf373,

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

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. [Figure not available: see fulltext.]",

keywords = "MIL-53-NH, benzene oxidation, charge-carrier dynamics, diatomic sites, photocatalysis",

author = "Gang Wang and Yan Liu and Ning Zhao and Huimei Chen and Wenjie Wu and Yueyue Li and Xiangwen Liu and Ang Li and Wenxing Chen and Junjie Mao",

note = "Publisher Copyright: {\textcopyright} 2022, Tsinghua University Press.",

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T1 - Constructing the separation pathway for photo-generated carriers by diatomic sites decorated on MIL-53-NH2(Al) for enhanced photocatalytic performance

AU - Wang, Gang

AU - Liu, Yan

AU - Zhao, Ning

AU - Chen, Huimei

AU - Wu, Wenjie

AU - Li, Yueyue

AU - Liu, Xiangwen

AU - Li, Ang

AU - Chen, Wenxing

AU - Mao, Junjie

PY - 2022/8

Y1 - 2022/8

N2 - 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. [Figure not available: see fulltext.]

AB - 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. [Figure not available: see fulltext.]

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