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Atomically Dispersed Fe-N4 Site as a Conductive Bridge Enables Efficient and Stable Activation of Peroxymonosulfate: Active Site Renewal, Anti-Oxidative Capacity, and Pathway Alternation Mechanism.
Zeng, Tao; Tang, Xiaofeng; Huang, Zheqing; Chen, Hong; Jin, Sijia; Dong, Feilong; He, Jia; Song, Shuang; Zhang, Haiyan.
Afiliación
  • Zeng T; Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, Department of Environment, Zhejiang University of Technology, Zhejiang, Hangzhou 310032, P.R. China.
  • Tang X; Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, Department of Environment, Zhejiang University of Technology, Zhejiang, Hangzhou 310032, P.R. China.
  • Huang Z; Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, Department of Environment, Zhejiang University of Technology, Zhejiang, Hangzhou 310032, P.R. China.
  • Chen H; Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, Department of Environment, Zhejiang University of Technology, Zhejiang, Hangzhou 310032, P.R. China.
  • Jin S; Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Zhejiang, Hangzhou 310024, P.R. China.
  • Dong F; Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, Department of Environment, Zhejiang University of Technology, Zhejiang, Hangzhou 310032, P.R. China.
  • He J; Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, Department of Environment, Zhejiang University of Technology, Zhejiang, Hangzhou 310032, P.R. China.
  • Song S; Beijing Key Laboratory of Urban Hydrological Cycle and Sponge City Technology, College of Water Sciences, Beijing Normal University, Beijing 100875, China.
  • Zhang H; Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, Department of Environment, Zhejiang University of Technology, Zhejiang, Hangzhou 310032, P.R. China.
Environ Sci Technol ; 57(49): 20929-20940, 2023 Dec 12.
Article en En | MEDLINE | ID: mdl-37956230
Atomically dispersed metal sites anchored on nitrogen-doped carbonaceous substrates (M-NCs) have emerged as promising alternatives to conventional peroxymonosulfate (PMS) activators; however, the exact contribution of each site still remains elusive. Herein, isolated Fe-N4 active site-decorated three-dimensional NC substrates (FeSA-NC) via a micropore confinement strategy are fabricated to initiate PMS oxidation reaction, achieving a specific activity of 5.16 × 103 L·min-1·g-1 for the degradation of bisphenol A (BPA), which outperforms most of the state-of-the-art single-atom (SA) catalysts. Mechanism inquiry reveals enhanced chemisorption and electron transfer between PMS and FeSA-NC, enabling an inner electron shuttle mechanism in which Fe-N4 serves as a conductive bridge. The Fe-N4 sites reduce the energy barrier for the formation of SO5* and H*, thereby transforming the reaction pathway from directly adjacent electron transfer into reactive oxygen species (ROS)-dominated oxidation. Theoretical calculations and dynamic simulations reveal that the Fe-N4 sites induce facilitated desorption of reaction intermediates (PMS*/BPA*), which collectively contribute to the renewal of active sites and eventually enhance the catalytic durability. This work offers a reasonable interpretation for the important role of the Fe-N4 moiety in altering the activation mechanism and enhancing the antioxidative capacity of NC materials, which fundamentally furnishes theoretical support for SA material design.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Peróxidos Idioma: En Revista: Environ Sci Technol Año: 2023 Tipo del documento: Article Pais de publicación: Estados Unidos
Texto completo
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XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Peróxidos Idioma: En Revista: Environ Sci Technol Año: 2023 Tipo del documento: Article Pais de publicación: Estados Unidos