The debatable role of singlet oxygen in persulfate-based advanced oxidation processes

Water Research, Год журнала: 2023, Номер 235, С. 119925 - 119925

Опубликована: Март 28, 2023

Язык: Английский

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Different reaction mechanisms of SO4•− and •OH with organic compound interpreted at molecular orbital level in Co(II)/peroxymonosulfate catalytic activation system

Water Research, Год журнала: 2022, Номер 229, С. 119392 - 119392

Опубликована: Ноя. 19, 2022

Язык: Английский

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Origin of the Excellent Activity and Selectivity of a Single-Atom Copper Catalyst with Unsaturated Cu-N₂ Sites via Peroxydisulfate Activation: Cu(III) as a Dominant Oxidizing Species

Environmental Science & Technology, Год журнала: 2022, Номер 56(12), С. 8765 - 8775

Опубликована: Май 12, 2022

As an efficient active oxidant for the selective degradation of pollutants in wastewater, high-valent copper species Cu(III) with persulfate activation has attracted substantial attention some Cu-based catalysts. However, systematic study a catalyst structure and mechanism about peroxydisulfate (PDS) is challenging owing to coexistence multiple Cu structural symmetry PDS. Herein, we anchored atom two pyridinic N atoms synthesize single-atom (CuSA-NC). Experimental characterizations theoretical calculations complemented each other well because uniform atomic sites. The was identified as site, unsaturated Cu-N2 configuration more conductive PDS than saturated Cu-N4 configuration. Benefiting from generation Cu(III), CuSA-NC exhibited obvious anti-interference performance pollutant complex matrix. superior catalytic activity compared that reported catalysts good durability continuous-flow experiment further revealed potential practical applications. This work strongly deepens understanding sites under develops approach actual water purification.

Язык: Английский

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Single-atom co sites confined in layered double hydroxide for selective generation of surface-bound radicals via peroxymonosulfate activation

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 340, С. 123218 - 123218

Опубликована: Авг. 25, 2023

Selective production of specific radical species with prolonged lifetime is challenging in advanced oxidation process. Herein, we constructed single-atom Co (SA-Co) catalytic sites confined layered double hydroxide (LDH) for selectively and sustainably generate via peroxymonosulfate (PMS) activation. The negatively charged PMS was stabilized by the positively LDH simultaneously activated nanoconfined sites, resulting oriented-production surface-bonded •OH SO4•− radicals long-term efficiency (up to 48 h), suppressed decomposition self-quenching. Ion competition experiments in-situ spectroscopic studies were applied monitor activation processes. SA-Co-LDH/PMS system outperforms benchmark homogeneous (Co2+/PMS) heterogeneous (Co3O4/PMS) systems degradation emerging organic contaminants (EOCs) lowest consumption highest efficiency.

Язык: Английский

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Advanced oxidation processes for water purification using percarbonate: Insights into oxidation mechanisms, challenges, and enhancing strategies

Journal of Hazardous Materials, Год журнала: 2022, Номер 442, С. 130014 - 130014

Опубликована: Сен. 17, 2022

Язык: Английский

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

Environmental Science & Technology, Год журнала: 2024, Номер 58(24), С. 10415 - 10444

Опубликована: Июнь 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.

Язык: Английский

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Strategies based on electron donors to accelerate Fe(III)/Fe(II) cycle in Fenton or Fenton-like processes

Chemical Engineering Journal, Год журнала: 2022, Номер 454, С. 140096 - 140096

Опубликована: Ноя. 1, 2022

Язык: Английский

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Degradation of Organic Contaminants by Reactive Iron/Manganese Species: Progress and Challenges

Water Research, Год журнала: 2022, Номер 221, С. 118765 - 118765

Опубликована: Июнь 16, 2022

Язык: Английский

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Constructing Hollow Multishelled Microreactors with a Nanoconfined Microenvironment for Ofloxacin Degradation through Peroxymonosulfate Activation: Evolution of High-Valence Cobalt-Oxo Species

Environmental Science & Technology, Год журнала: 2023, Номер 57(42), С. 16141 - 16151

Опубликована: Сен. 11, 2023

This study constructed hollow multishelled microreactors with a nanoconfined microenvironment for degrading ofloxacin (OFX) through peroxymonosulfate (PMS) activation in Fenton-like advanced oxidation processes (AOPs), resulting adequate contaminant mineralization. Among the microreactors, triple-shelled Co-based microsphere (TS-Co/HM) exhibited optimal performance; its OFX degradation rate was 0.598 min-1, which higher than that of Co3O4 nanoparticles by 8.97-fold. The structural tuning Co/HM promoted formation oxygen vacancies (VO), then facilitated evolution high-valence cobalt-oxo (Co(IV)═O) and shifted entire t2g orbital Co atom upward, promoting catalytic reactions. Co(IV)═O identified using phenylmethyl sulfoxide (PMSO) probe situ Raman spectroscopy, theoretical calculations were conducted to identify lower energy barrier on defect-rich catalyst. Furthermore, TS-Co/HM catalyst remarkable stability inorganic (Cl-, H2PO4-, NO3-), organic (humic acid), real water samples (tap water, river hospital water), continuous flow system microreactor. could enrich reactants cavities, prolong residence time molecules, increase utilization efficiency Co(IV)═O. work describes an process involving contaminants elimination. Our results may encourage use structures inform design catalysts AOPs.

Язык: Английский

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Insight into peroxymonosulfate assisted photocatalysis over Fe2O3 modified TiO2/diatomite composite for highly efficient removal of ciprofloxacin

Separation and Purification Technology, Год журнала: 2022, Номер 293, С. 121123 - 121123

Опубликована: Апрель 21, 2022

Язык: Английский

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