Deciphering the Origin of Higher Shell Coordination on Single Iron Catalysts for Resilient Modulating Persulfate Oxidation Into Singlet Oxygen Pathway

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 28, 2025

Abstract Precise manipulation of coordination structure single‐atom sites and establishment schematic microenvironment‐oxidation pathway relations remain significant challenges in Fenton‐like chemistry. Herein, incorporating sulfur heteroatoms into the higher shell FeN 4 (Fe‐NSC) exhibited a volcano trend p ‐hydroxybenzoic acid oxidation, aligning with number positions dopant. Specifically, S moderate electronegativity larger atomic radii triggers long‐range electronic interactions, which provoke Fe 3d orbital splitting spin electron rearrangement, resulting crossover states d xy 2 yz 1 xz z 21 . As result, partial filling e g t orbitals σ/π antibonding between 2p optimized adsorption–desorption behaviors key oxygenated intermediates from peroxymonosulfate activation. Thus, optimal binding configuration weakens Fe─O bonding accelerates PMS dissociation to yield C‐S‐N Fe‐O*, subsequently couples form O nearly 100% selectivity. The Fe‐NSC‐functionalized membrane outstanding long‐term reusability continuous flow reactor further validated practical application perspective. This study provides insight at both levels for rational design spin‐polarized catalysts its functions fine‐tuning oxidation pathways environmental catalysis.

Language: Английский

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Confronting the Mysteries of Oxidative Reactive Species in Advanced Oxidation Processes: An Elephant in the Room

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(42), P. 18496 - 18507

Published: Oct. 9, 2024

Advanced oxidation processes (AOPs) are rapidly evolving but still lack well-established protocols for reliably identifying oxidative reactive species (ORSs). This Perspective presents both the radical and nonradical ORSs that have been identified or proposed, along with extensive controversies surrounding mechanisms. Conventional identification tools, such as quenchers, probes, spin trappers, might be inadequate analytical demands of systems in which multiple coexist, often yielding misleading results. Therefore, challenges these complex, short-lived, transient must fully acknowledged. Refining methods is necessary, supported by rigorous experiments innovative paradigms, particularly through kinetic analysis based on situ spectroscopic techniques multiple-probe strategies. To demystify complex ORSs, future efforts should made to develop advanced tools strategies enhance mechanism understanding. In addition, integrating real-world conditions into experimental designs will establish a reliable framework fundamental studies, providing more accurate insights effectively guiding design AOPs.

Language: Английский

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Methods and Prospects for Enhancing Heterogeneous Fenton Catalytic Activity

ChemistrySelect, Journal Year: 2025, Volume and Issue: 10(1)

Published: Jan. 1, 2025

Abstract As an advanced oxidation process that can efficiently remove organic pollutants in water, Fenton has attracted much attention recent years. Compared to homogeneous Fenton, it a wider applicability, wide pH range, higher degradation efficiency, lower environmental impact, and treatment cost. However, the heterogeneous reaction also some limitations, such as deactivation of catalyst, rate being limited by solid–liquid interface mass transfer. Therefore, development efficient stable catalytic system is focus research at present. In this paper, catalysis are introduced, construction characteristics mechanism iron base, copper transition metals their oxides, chelating agents, carbon materials, supported catalysts, photocatalysis systematically summarized. addition, strategies for formation Fe II promotion H 2 O decomposition were discussed, pathway catalyst matter summarized order provide technical support further on catalysts.

Language: Английский

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Biochar-supported MnFeO2 for heterogeneous photo-Fenton degradation of doxycycline: Collaborative promotion of electron transfer and H2O2 activation

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 159885 - 159885

Published: Jan. 1, 2025

Language: Английский

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Stability challenges of transition metal-modified cathodes for electro-Fenton process: A mini-review

Chemosphere, Journal Year: 2025, Volume and Issue: 373, P. 144159 - 144159

Published: Jan. 30, 2025

Language: Английский

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Removal of Sulfonamide Antibiotics in Peracetic Acid-Mediated Natural Polyphenol Systems via an Overlooked Polymerization Pathway: Role of ortho-Quinones

Environmental Science & Technology, Journal Year: 2025, Volume and Issue: unknown

Published: April 14, 2025

Natural polyphenols can be oxidized into reactive quinones, which might play a key role in the removal of specific contaminants natural polyphenol-related advanced oxidation processes (AOPs). In this study, peracetic acid (PAA) was employed combination with protocatechuic (PCA) to remove sulfonamide antibiotics (SAs) from water. More than 95% sulfamethoxazole (SMX) and other SAs observed PCA/PAA system, neutral pH conditions (5.0-8.0) were more conducive SMX. The system exhibited great anti-interference ability against complex water matrices. ortho-Quinone, generated PCA by PAA, played dominant SMX removal. Electrons tended transfer ortho-quinones form covalent bonds, resulting production less toxic oligomers via overlooked polymerization pathway. A reduction toxicity solution found following treatment system. interestingly, several structurally related could also facilitate using PAA as oxidant. Overall, study proposes novel strategy for developing quinones dominated AOPs robust performance, well enhances understanding contaminant an pathway AOPs.

Language: Английский

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Pyrazine-based iron metal organic frameworks (Fe-MOFs) with modulated O-Fe-N coordination for enhanced hydroxyl radical generation in Fenton-like process

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 674, P. 279 - 288

Published: June 24, 2024

Language: Английский

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Enhancing solar-driven photocatalysis: synergistic integration of biochar, semiconductors, and magnetic materials for degrading organic pollutants

Desalination and Water Treatment, Journal Year: 2024, Volume and Issue: unknown, P. 100798 - 100798

Published: Sept. 1, 2024

Language: Английский

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Fe(III) Alleviates pH Dependence of Iron-based Bimetallic/PMS System for Organic Pollutant Oxidation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 125002 - 125002

Published: Dec. 1, 2024

Language: Английский

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NH2-MIL-88B(Fe)/PVDF mixed matrix membranes: A one-stone-two-birds strategy for efficient removal of tetracycline hydrochloride from aquatic systems

Journal of environmental chemical engineering, Journal Year: 2024, Volume and Issue: 13(1), P. 115100 - 115100

Published: Dec. 12, 2024

Language: Английский

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