Accurate identification of radicals by in-situ electron paramagnetic resonance in ultraviolet-based homogenous advanced oxidation processes

Water Research, Journal Year: 2022, Volume and Issue: 221, P. 118747 - 118747

Published: June 15, 2022

Language: Английский

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Dual donor-acceptor covalent organic frameworks for hydrogen peroxide photosynthesis

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Aug. 28, 2023

Constructing photocatalytically active and stable covalent organic frameworks containing both oxidative reductive reaction centers remain a challenge. In this study, benzotrithiophene-based with spatially separated redox are rationally designed for the photocatalytic production of hydrogen peroxide from water oxygen without sacrificial agents. The triazine-containing framework demonstrates high selectivity H2O2 photogeneration, yield rate 2111 μM h-1 (21.11 μmol 1407 g-1 h-1) solar-to-chemical conversion efficiency 0.296%. Codirectional charge transfer large energetic differences between linkages linkers verified in double donor-acceptor structures periodic frameworks. sites mainly concentrated on electron-acceptor fragments near imine bond, which regulate electron distribution adjacent carbon atoms to optimally reduce Gibbs free energy O2* OOH* intermediates during formation H2O2.

Language: Английский

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Linkage Microenvironment of Azoles‐Related Covalent Organic Frameworks Precisely Regulates Photocatalytic Generation of Hydrogen Peroxide

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(36)

Published: July 18, 2023

Artificial H2 O2 photosynthesis by covalent organic frameworks (COFs) photocatalysts is promising for wastewater treatment. The effect of linkage chemistry COFs as functional basis to photoelectrochemical properties and photocatalysis remains a significant challenge. In this study, three kinds azoles-linked including thiazole-linked TZ-COF, oxazole-linked OZ-COF imidazole-linked IZ-COF were successfully synthesized. More accessible channels charge transfer constructed in TZ-COF via the donor-π-acceptor structure between thiazole pyrene linker, leading efficient suppression photoexcited recombination. Density theory calculations support experimental studies, demonstrating that more favorable formation *O2 intermediate production than oxazole imidazole linkages. real active sites located at benzene ring fragment unit azole linkage.

Language: Английский

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Accelerating radical generation from peroxymonosulfate by confined variable Co species toward ciprofloxacin mineralization: ROS quantification and mechanisms elucidation

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 315, P. 121542 - 121542

Published: May 23, 2022

Language: Английский

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Efficient sacrificial-agent-free solar H2O2 production over all-inorganic S-scheme composites

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 324, P. 122227 - 122227

Published: Nov. 26, 2022

Language: Английский

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Clarification of the role of singlet oxygen for pollutant abatement during persulfate-based advanced oxidation processes: Co3O4@CNTs activated peroxymonosulfate as an example

Water Research, Journal Year: 2023, Volume and Issue: 244, P. 120480 - 120480

Published: Aug. 11, 2023

Language: Английский

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Were Persulfate-Based Advanced Oxidation Processes Really Understood? Basic Concepts, Cognitive Biases, and Experimental Details

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(24), P. 10415 - 10444

Published: June 7, 2024

Persulfate (PS)-based advanced oxidation processes (AOPs) for pollutant removal have attracted extensive interest, but some controversies about the identification of reactive species were usually observed. This critical review aims to comprehensively introduce basic concepts and rectify cognitive biases appeals pay more attention experimental details in PS-AOPs, so as accurately explore reaction mechanisms. The scientifically summarizes character, generation, different species. It then highlights complexities analysis electron paramagnetic resonance, uncertainties use probes scavengers, necessities determination scavenger concentration. importance choice buffer solution, operating mode, terminator, filter membrane is also emphasized. Finally, we discuss current challenges future perspectives alleviate misinterpretations toward mechanisms PS-AOPs.

Language: Английский

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Insights into reactive species generation and organics selective degradation in Fe-based heterogeneous Fenton-like systems: A critical review

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 454, P. 140126 - 140126

Published: Nov. 9, 2022

Language: Английский

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Trimetallic MOFs-derived Fe-Co-Cu oxycarbide toward peroxymonosulfate activation for efficient trichlorophenol degradation via high-valent metal-oxo species

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 468, P. 143444 - 143444

Published: May 11, 2023

Language: Английский

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Efficient Photosynthesis of Hydrogen Peroxide by Cyano‐Containing Covalent Organic Frameworks from Water, Air and Sunlight

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(6)

Published: Dec. 28, 2023

Abstract The insufficient exciton ( e − ‐ h + pair) separation/transfer and sluggish two‐electron water oxidation are two main factors limiting the H 2 O photosynthetic efficiency of covalent organic frameworks (COFs) photocatalysts. Herein, we present an alternative strategy to simultaneously facilitate reduce energy barrier in COFs via a dicyano functionalization. situ characterization theoretical calculations reveal that functionalization improves amount charge transfer channels between donor acceptor units from COF‐0CN without cyano three COF‐1CN with mono‐cyano four COF‐2CN functionalization, leading highest COF‐2CN. More importantly, group activates neighbouring C atom produce key *OH intermediate for effectively reducing rate‐determining photosynthesis. enhanced result high yield (1601 μmol g −1 ) oxygen using sacrificial reagent under visible‐light irradiation. can wide pH range, different real samples, scaled‐up reactor natural sunlight irradiation, continuous‐flow consecutively producing solution decontamination.

Language: Английский

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