Origins of Electron-Transfer Regime in Persulfate-Based Nonradical Oxidation Processes

Environmental Science & Technology, Journal Year: 2021, Volume and Issue: 56(1), P. 78 - 97

Published: Dec. 21, 2021

Persulfate-based nonradical oxidation processes (PS-NOPs) are appealing in wastewater purification due to their high efficiency and selectivity for removing trace organic contaminants complicated water matrices. In this review, we showcased the recent progresses of state-of-the-art strategies electron-transfer regimes PS-NOPs, including design metal metal-free heterogeneous catalysts, situ/operando characterization/analytical techniques, insights into origins mechanisms. a typical process (ETP), persulfate is activated by catalyst form surface complexes, which directly or indirectly interact with target pollutants finalize oxidation. We discussed different analytical techniques on fundamentals tactics accurate analysis ETP. Moreover, demonstrated challenges proposed future research ETP-based systems, such as computation-enabled molecular-level investigations, rational real-scenario applications environment. Overall, review dedicates sharpening understanding ETP PS-NOPs presenting promising remediation technology green chemistry.

Language: Английский

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Facile fabrication of TaON/Bi2MoO6 core–shell S-scheme heterojunction nanofibers for boosting visible-light catalytic levofloxacin degradation and Cr(VI) reduction

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 428, P. 131158 - 131158

Published: July 7, 2021

Language: Английский

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Nonradicals induced degradation of organic pollutants by peroxydisulfate (PDS) and peroxymonosulfate (PMS): Recent advances and perspective

The Science of The Total Environment, Journal Year: 2020, Volume and Issue: 765, P. 142794 - 142794

Published: Oct. 8, 2020

Language: Английский

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Engineered carbon supported single iron atom sites and iron clusters from Fe-rich Enteromorpha for Fenton-like reactions via nonradical pathways

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 287, P. 119963 - 119963

Published: Feb. 7, 2021

Language: Английский

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Density Functional Theory Calculations for Insight into the Heterocatalyst Reactivity and Mechanism in Persulfate-Based Advanced Oxidation Reactions

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(17), P. 11129 - 11159

Published: Aug. 23, 2021

Advanced oxidation processes (AOPs) based on persulfates such as peroxymonosulfate and peroxydisulfate via heterogeneous catalysts have been a research hotspot due to their outstanding performances in removing emerging organic contaminants (OCs). In this Review, we highlight the recent advances theoretical simulations for persulfate-based AOPs (PS-AOPs) using density functional theory (DFT), with emphasis catalyst properties mechanism of persulfate activation over variety (including nanocarbons, metals, metal oxides). Moreover, OCs degradation by diverse reactive oxygen species investigated computations are also summarized. The descriptors computational studies related structure–performance relationships discussed. Finally, challenges future focuses DFT PS-AOPs proposed, including evaluation properties, elucidation mechanism, especially nonradical pathway, rational design on-demand catalysts.

Language: Английский

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Singlet oxygen-dominated activation of peroxymonosulfate by passion fruit shell derived biochar for catalytic degradation of tetracycline through a non-radical oxidation pathway

Journal of Hazardous Materials, Journal Year: 2021, Volume and Issue: 419, P. 126495 - 126495

Published: June 26, 2021

Language: Английский

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Biochar co-doped with nitrogen and boron switching the free radical based peroxydisulfate activation into the electron-transfer dominated nonradical process

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 301, P. 120832 - 120832

Published: Oct. 19, 2021

Language: Английский

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Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N₄–C Intensified Radical and Nonradical Pathways

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(16), P. 11635 - 11645

Published: July 11, 2022

Single-atom catalysts (SACs)-based peroxymonosulfate (PMS) systems are highly selective to the type of organic pollutants while mechanisms remain ambiguous. In this work, we carried out experimental and theoretical investigations reveal origins selectivity radical nonradical pathways in a designated Co–N4–C/PMS system. Two typical [bisphenol A (BPA) metronidazole (MNZ)] with different molecular structures were employed for comparison. We found that oxidation (SO4•– HO•) electron-transfer pathway (ETP) co-existed Pollutants (e.g., MNZ) high redox potential degraded primarily by free radicals rather than ETP, oxidization low-redox BPA) was dominated ETP at surface region Co–N4–C which overwhelmed contributions homogeneous phase. Intriguingly, could be manipulated PMS loading, simultaneously increased population elevated Co–N4–C-PMS* complexes ETP. Findings from work will unravel mysterious behavior SACs/PMS micropollutants.

Language: Английский

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

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

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Activation of peroxymonosulfate by single atom Co-N-C catalysts for high-efficient removal of chloroquine phosphate via non-radical pathways: Electron-transfer mechanism

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 429, P. 132245 - 132245

Published: Sept. 3, 2021

Language: Английский

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