Three-Dimensional Welded Mn1 Site Catalysts with nearly 100% Singlet Oxygen Fabrication for Contaminant Elimination

Xiao Ge; Donghua Xie; Rui Fen Cheng; Wenxing Chen; Cai Chen; Fangyao Zhou; Xiaozhi Wang; Jie Jie Chen; Guo Ping Sheng; Yuen Wu

doi:10.1021/prechem.2c00006

Three-Dimensional Welded Mn₁ Site Catalysts with nearly 100% Singlet Oxygen Fabrication for Contaminant Elimination

Xiao Ge, Donghua Xie, Rui Fen Cheng, Wenxing Chen, Cai Chen, Fangyao Zhou, Xiaozhi Wang, Jie Jie Chen^*, Guo Ping Sheng^*, Yuen Wu^*

^*Corresponding author for this work

School of Material Science and Engineering

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

29 Citations (Scopus)

Abstract

Reactive oxygen species (ROS) have a significant part in the elimination of recalcitrant organic pollutants and commonly coexist in one advanced oxidation system. It is difficult for us to make clear the effect of the co-instantaneous generation of radicals and nonradicals, which would cover and obscure the transformation pathway. Herein, a coordinate welding process is presented for fabricating accessible Mn₁ site catalysts (Mn SSCs) in order to clarify the nonradical (singlet oxygen/¹O₂) generated pathway and transformation in oxidative removal of contaminants. The Mn SSCs achieve nearly 100% ¹O₂ fabrication by activating peroxymonosulfate, which displays an excellent sulfamethoxazole elimination performance, super anti-anion interference, and extraordinary stability. As revealed by density functional theory calculations, the Mn SSCs with a special welded three-dimensional nanostructure could significantly boost the activation process by oxidizing the peroxymonosulfate at the interlayer of Mn SSCs and reducing dissolved oxygen on the surface of Mn SSCs. This design of Mn SSCs with a three-dimensional welded nanostructure might offer a potential approach for employing single site catalysts for environmental remediation.

Original language	English
Pages (from-to)	153-160
Number of pages	8
Journal	Precision Chemistry
Volume	1
Issue number	3
DOIs	https://doi.org/10.1021/prechem.2c00006
Publication status	Published - 22 May 2023

Keywords

advanced oxidation
nonradicals
single site catalysts
singlet oxygen
three-dimensional welded nanostructure

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10.1021/prechem.2c00006

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@article{2f1b6d7beb2d4dd582e0519bdccf3515,

title = "Three-Dimensional Welded Mn1 Site Catalysts with nearly 100% Singlet Oxygen Fabrication for Contaminant Elimination",

abstract = "Reactive oxygen species (ROS) have a significant part in the elimination of recalcitrant organic pollutants and commonly coexist in one advanced oxidation system. It is difficult for us to make clear the effect of the co-instantaneous generation of radicals and nonradicals, which would cover and obscure the transformation pathway. Herein, a coordinate welding process is presented for fabricating accessible Mn1 site catalysts (Mn SSCs) in order to clarify the nonradical (singlet oxygen/1O2) generated pathway and transformation in oxidative removal of contaminants. The Mn SSCs achieve nearly 100% 1O2 fabrication by activating peroxymonosulfate, which displays an excellent sulfamethoxazole elimination performance, super anti-anion interference, and extraordinary stability. As revealed by density functional theory calculations, the Mn SSCs with a special welded three-dimensional nanostructure could significantly boost the activation process by oxidizing the peroxymonosulfate at the interlayer of Mn SSCs and reducing dissolved oxygen on the surface of Mn SSCs. This design of Mn SSCs with a three-dimensional welded nanostructure might offer a potential approach for employing single site catalysts for environmental remediation.",

keywords = "advanced oxidation, nonradicals, single site catalysts, singlet oxygen, three-dimensional welded nanostructure",

author = "Xiao Ge and Donghua Xie and Cheng, {Rui Fen} and Wenxing Chen and Cai Chen and Fangyao Zhou and Xiaozhi Wang and Chen, {Jie Jie} and Sheng, {Guo Ping} and Yuen Wu",

note = "Publisher Copyright: {\textcopyright} 2023 The Authors. Co-published by University of Science and Technology of China and American Chemical Society.",

year = "2023",

month = may,

day = "22",

doi = "10.1021/prechem.2c00006",

language = "English",

volume = "1",

pages = "153--160",

journal = "Precision Chemistry",

issn = "2771-9316",

publisher = "American Chemical Society",

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TY - JOUR

T1 - Three-Dimensional Welded Mn1 Site Catalysts with nearly 100% Singlet Oxygen Fabrication for Contaminant Elimination

AU - Ge, Xiao

AU - Xie, Donghua

AU - Cheng, Rui Fen

AU - Chen, Wenxing

AU - Chen, Cai

AU - Zhou, Fangyao

AU - Wang, Xiaozhi

AU - Chen, Jie Jie

AU - Sheng, Guo Ping

AU - Wu, Yuen

PY - 2023/5/22

Y1 - 2023/5/22

N2 - Reactive oxygen species (ROS) have a significant part in the elimination of recalcitrant organic pollutants and commonly coexist in one advanced oxidation system. It is difficult for us to make clear the effect of the co-instantaneous generation of radicals and nonradicals, which would cover and obscure the transformation pathway. Herein, a coordinate welding process is presented for fabricating accessible Mn1 site catalysts (Mn SSCs) in order to clarify the nonradical (singlet oxygen/1O2) generated pathway and transformation in oxidative removal of contaminants. The Mn SSCs achieve nearly 100% 1O2 fabrication by activating peroxymonosulfate, which displays an excellent sulfamethoxazole elimination performance, super anti-anion interference, and extraordinary stability. As revealed by density functional theory calculations, the Mn SSCs with a special welded three-dimensional nanostructure could significantly boost the activation process by oxidizing the peroxymonosulfate at the interlayer of Mn SSCs and reducing dissolved oxygen on the surface of Mn SSCs. This design of Mn SSCs with a three-dimensional welded nanostructure might offer a potential approach for employing single site catalysts for environmental remediation.

AB - Reactive oxygen species (ROS) have a significant part in the elimination of recalcitrant organic pollutants and commonly coexist in one advanced oxidation system. It is difficult for us to make clear the effect of the co-instantaneous generation of radicals and nonradicals, which would cover and obscure the transformation pathway. Herein, a coordinate welding process is presented for fabricating accessible Mn1 site catalysts (Mn SSCs) in order to clarify the nonradical (singlet oxygen/1O2) generated pathway and transformation in oxidative removal of contaminants. The Mn SSCs achieve nearly 100% 1O2 fabrication by activating peroxymonosulfate, which displays an excellent sulfamethoxazole elimination performance, super anti-anion interference, and extraordinary stability. As revealed by density functional theory calculations, the Mn SSCs with a special welded three-dimensional nanostructure could significantly boost the activation process by oxidizing the peroxymonosulfate at the interlayer of Mn SSCs and reducing dissolved oxygen on the surface of Mn SSCs. This design of Mn SSCs with a three-dimensional welded nanostructure might offer a potential approach for employing single site catalysts for environmental remediation.

KW - advanced oxidation

KW - nonradicals

KW - single site catalysts

KW - singlet oxygen

KW - three-dimensional welded nanostructure

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M3 - Article

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Three-Dimensional Welded Mn₁ Site Catalysts with nearly 100% Singlet Oxygen Fabrication for Contaminant Elimination

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Keywords

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