Synergistic Catalysis of Cobalt Single Atoms and Clusters Loaded on Carbon Film: Enhancing Peroxymonosulfate Activation for Degradation of Norfloxacin DOI

Chenglin Hao,

Tinghang Li,

Yanjie Xie

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 1, 2024

Abstract Many existing research focuses on the differences or performance comparisons between single‐atom small‐sized nanocluster catalysts, but there is a lack of comprehensive coupling relationship structure and activity mechanism synergy. This study investigates combined catalytic potential cobalt single atoms (SAs) nanoclusters (NCs) for enhanced peroxymonosulfate (PMS) activation to degrade norfloxacin (NFX). A novel Co SAs‐NCs /CN/TiO 2 catalyst synthesized, featuring SAs NCs uniformly dispersed carbon film wrapping TiO , degradation efficiency NFX solution almost completely degraded, with mineralization rate 76.35%. Density functional theory (DFT) calculations indicate that synergistic interaction promotes more efficient PMS adsorption significantly reduces energy barrier, which enhances electron transfer increases reactive oxygen species (ROS) generation. highlights robust versatile nature this system in addressing various contaminants. elucidates providing new ideas advanced oxidation processes (AOPs) environmental remediation, linking emphasizes practicality importance effectively long‐term remediation water pollutants.

Language: Английский

Merits and Limitations of Radical vs. Nonradical Pathways in Persulfate-Based Advanced Oxidation Processes DOI

Yiqi Yan,

Zongsu Wei, Xiaoguang Duan

et al.

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(33), P. 12153 - 12179

Published: Aug. 3, 2023

Urbanization and industrialization have exerted significant adverse effects on water quality, resulting in a growing need for reliable eco-friendly treatment technologies. Persulfate (PS)-based advanced oxidation processes (AOPs) are emerging as viable technologies to treat challenging industrial wastewaters or remediate groundwater impacted by hazardous wastes. While the generated reactive species can degrade variety of priority organic contaminants through radical nonradical pathways, there is lack systematic in-depth comparison these pathways practical implementation different scenarios. Our comparative analysis reaction rate constants vs. indicates that radical-based AOPs may achieve high removal efficiency with relatively short contact time. Nonradical feature advantages minimal matrix interference complex wastewater treatments. (e.g., singlet oxygen, high-valent metals, surface activated PS) preferentially react bearing electron-donating groups, allowing enhancement degradation known target contaminants. For byproduct formation, analytical limitations computational chemistry applications also considered. Finally, we propose holistically estimated electrical energy per order (EE/O) parameter show significantly higher requirements pathways. Overall, critical comparisons help prioritize basic research PS-based inform merits system-specific applications.

Language: Английский

Citations

261

Electron transfer-mediated enhancement of superoxide radical generation in fenton-like process: Key role of oxygen vacancy-regulated local electron density of cobalt sites DOI

Ta Cong Khiem,

Nguyễn Nhật Huy, Eilhann E. Kwon

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 343, P. 123490 - 123490

Published: Nov. 10, 2023

Language: Английский

Citations

66

NiCo2N nanosheets catalyzed peroxymonosulfate activation to generate 1O2 and SO4•- for efficient pollutant degradation: The role of nitrogen atoms DOI

Pengcheng Cai,

Xiaohui Zhang, Shuai Yang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123446 - 123446

Published: Oct. 28, 2023

Language: Английский

Citations

49

Rational modulation of Fe single-atom electronic structure in a Fe-N2B4 configuration for preferential 1O2 generation in Fenton-like reactions DOI
Yuhan Long, Zhenhua Cao,

Weiran Wu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 344, P. 123643 - 123643

Published: Dec. 21, 2023

Language: Английский

Citations

49

Generation and engineering applications of sulfate radicals in environmental remediation DOI
Jun Xie, Chunping Yang, Xiang Li

et al.

Chemosphere, Journal Year: 2023, Volume and Issue: 339, P. 139659 - 139659

Published: July 27, 2023

Language: Английский

Citations

44

Recent advances in microwave-enhanced advanced oxidation processes (MAOPs) for environmental remediation: A review DOI

Menghan Cao,

Peng Xu, Ke Tian

et al.

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 471, P. 144208 - 144208

Published: June 28, 2023

Language: Английский

Citations

42

Ultrafast oxidation of refractory organics via PMS activation by Si-O doped biomimetic montmorillonite: Simultaneous enhanced radical/electron transfer pathways and efficient catalytic membrane system DOI

Jiasheng Mao,

Kexin Yin,

Yang Zhang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123428 - 123428

Published: Oct. 24, 2023

Language: Английский

Citations

42

Precise coordination of high-loading Fe single atoms with sulfur boosts selective generation of nonradicals DOI
Xun‐Heng Jiang,

Binghui Zhou,

Weijie Yang

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(4)

Published: Jan. 17, 2024

Nonradicals are effective in selectively degrading electron-rich organic contaminants, which unfortunately suffer from unsatisfactory yield and uncontrollable composition due to the competitive generation of radicals. Herein, we precisely construct a local microenvironment carbon nitride–supported high-loading (~9 wt.%) Fe single-atom catalyst (Fe SAC) with sulfur via facile supermolecular self-assembly strategy. Short-distance S coordination boosts peroxymonosulfate (PMS) activation generates high-valent iron–oxo species IV =O) along singlet oxygen ( 1 O 2 ), significantly increasing yield, PMS utilization, p -chlorophenol reactivity by 6.0, 3.0, 8.4 times, respectively. The nonradicals is controllable simply changing content. In contrast, long-distance both radicals nonradicals, could not promote reactivity. Experimental theoretical analyses suggest that short-distance upshifts d -band center atom, i.e., being close Fermi level, changes binding mode between atom site generate =O high yield. S-coordinated SAC exhibits excellent application potential various water matrices. These findings can guide rational design robust SACs toward selective utilization.

Language: Английский

Citations

36

Single Atom Catalyst in Persulfate Oxidation Reaction: From Atom Species to Substance DOI

Daixi Zhou,

Zhi Li, Xinjiang Hu

et al.

Small, Journal Year: 2024, Volume and Issue: 20(30)

Published: March 5, 2024

Abstract With maximum utilization of active metal sites, more and researchers have reported using single atom catalysts (SACs) to activate persulfate (PS) for organic pollutants removal. In SACs, atoms (Fe, Co, Cu, Mn, etc.) different substrates (porous carbon, biochar, graphene oxide, carbon nitride, MOF, MoS 2 , others) are the basic structural. Metal atoms, substances, connected chemical bonds all a great influence on electronic structures that directly affect activation process PS degradation efficiency pollutants. However, there few relevant reviews about interaction between substances during process. this review, SACs with species summarized investigate metal−support evaluate their effects oxidation reaction Furthermore, how reactive pathways also discussed. Finally, challenges prospects in PS‐AOPs proposed.

Language: Английский

Citations

25

Single-atom Co-N3 sites induce peroxymonosulfate activation for acetaminophen degradation via nearly 100% internal electron transfer process DOI
Hong Meng, Junhui Zhou, Yongqing Zhang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125038 - 125038

Published: Jan. 1, 2025

Language: Английский

Citations

5