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

Environmental Science & Technology, Год журнала: 2021, Номер 56(1), С. 78 - 97

Опубликована: Дек. 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.

Язык: Английский

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The Intrinsic Nature of Persulfate Activation and N-Doping in Carbocatalysis

Environmental Science & Technology, Год журнала: 2020, Номер 54(10), С. 6438 - 6447

Опубликована: Апрель 17, 2020

Persulfates activation by carbon nanotubes (CNT) has been evidenced as nonradical systems for oxidation of organic pollutants. Peroxymonosulfate (PMS) and peroxydisulfate (PDS) possess discrepant atomic structures redox potentials, while the nature their distinct behaviors in carbocatalytic not investigated. Herein, we illustrated that roles nitrogen species CNT-based persulfate are intrinsically different. In PMS mediated nitrogen-doped CNT (N-CNT), surface chemical modification (N-doping) can profoundly promote adsorption quantity PMS, consequently elevate potential derived N-CNT–PMS* complexes, boost efficiency via an electron-transfer regime. contrast, PDS was enhanced upon incorporating N into due to limited equilibrium PDS, leading a relatively lower oxidative PDS/N-CNT system mediocre degradation rate. However, with equivalent on N-CNT at low quantity, exhibited stronger oxidizing capacity than PMS/N-CNT because intrinsic higher PMS. The rates two were great linearity potentials carbon–persulfate* suggesting shared similar mechanism. Therefore, this study provides new insights heteroatom doping nanocarbons persulfates unveils principles rational design reaction-oriented carbocatalysts persulfate-based advanced processes.

Язык: Английский

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Activation of persulfates by carbonaceous materials: A review

Chemical Engineering Journal, Год журнала: 2021, Номер 418, С. 129297 - 129297

Опубликована: Март 14, 2021

Язык: 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, Год журнала: 2020, Номер 765, С. 142794 - 142794

Опубликована: Окт. 8, 2020

Язык: Английский

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Co3O4 anchored in N, S heteroatom co-doped porous carbons for degradation of organic contaminant: role of pyridinic N-Co binding and high tolerance of chloride

Applied Catalysis B Environment and Energy, Год журнала: 2020, Номер 282, С. 119484 - 119484

Опубликована: Сен. 17, 2020

Язык: Английский

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Oxygen Vacancy-Induced Nonradical Degradation of Organics: Critical Trigger of Oxygen (O₂) in the Fe–Co LDH/Peroxymonosulfate System

Environmental Science & Technology, Год журнала: 2021, Номер 55(22), С. 15400 - 15411

Опубликована: Ноя. 5, 2021

Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into activation over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective via single-electron-transfer nonradical pathway. Moreover, O2 firstly demonstrated most critical trigger system. Mechanistic studies reveal that, with abundant electrons confined vacant electron orbitals Vo, thermodynamically enabled to capture from form O2•– imprinting effect start process. Simultaneously, becomes electron-deficient withdraws sustain electrostatic balance achieve (32% Bisphenol A without PMS). Different conventional activation, collaboration kinetics thermodynamics, endowed ability donate reductant other than an oxidant 1O2. case, 1O2 act indispensable intermediate species accelerate circulation (as high 14.3 mg/L) micro area around promote nano-confinement electron-recycling process 67% improvement degradation. This study provides brand-new perspective natural environments.

Язык: Английский

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Degradation of antibiotic pollutants by persulfate activated with various carbon materials

Chemical Engineering Journal, Год журнала: 2021, Номер 429, С. 132387 - 132387

Опубликована: Сен. 10, 2021

Язык: Английский

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Simultaneous nanocatalytic surface activation of pollutants and oxidants for highly efficient water decontamination

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Май 30, 2022

Abstract Removal of organic micropollutants from water through advanced oxidation processes (AOPs) is hampered by the excessive input energy and/or chemicals as well large amounts residuals resulting incomplete mineralization. Herein, we report a new purification paradigm, direct oxidative transfer process (DOTP), which enables complete, highly efficient decontamination at very low dosage oxidants. DOTP differs fundamentally AOPs and adsorption in its pollutant removal behavior mechanisms. In DOTP, nanocatalyst can interact with persulfate to activate pollutants lowering their reductive potential energy, triggers non-decomposing bulk solution surface. By leveraging activation, stabilization, accumulation functions heterogeneous catalyst, occur spontaneously on surface enable complete pollutants. The found for diverse pollutants, oxidants, nanocatalysts, including various low-cost catalysts. Significantly, requires no external input, has oxidant consumption, produces residual byproducts, performs robustly real environmental matrices. These favorable features render an extremely promising nanotechnology platform purification.

Язык: 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, Год журнала: 2021, Номер 11(17), С. 11129 - 11159

Опубликована: Авг. 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.

Язык: 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, Год журнала: 2021, Номер 301, С. 120832 - 120832

Опубликована: Окт. 19, 2021

Язык: Английский

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