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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2D N-Doped Porous Carbon Derived from Polydopamine-Coated Graphitic Carbon Nitride for Efficient Nonradical Activation of Peroxymonosulfate

Environmental Science & Technology, Год журнала: 2020, Номер 54(13), С. 8473 - 8481

Опубликована: Июнь 8, 2020

Nitrogen-doped carbon materials attract broad interest as catalysts for peroxymonosulfate (PMS) activation toward an efficient, nonradical advanced oxidation process. However, synthesis of N-rich carbocatalysts is challenging because the thermal instability desirable nitrogenous species (pyrrolic, pyridinic, and graphitic N). Furthermore, relative importance different configurations (and associated mechanisms) are unclear. Herein, we report a "coating-pyrolysis" method to synthesize porous 2D nanocarbon (PCN-x) derived from dopamine g-C3N4 in weight proportions. PCN-0.5 calcined at 800 °C had highest surface area (759 m2/g) unprecedentedly high N content (18.5 at%), displayed efficiency 4-chlorophenol (4-CP) degradation via PMS activation. A positive correlation was observed between 4-CP rates total pyridinic pyrrolic content. These dopants serve Lewis basic sites facilitate adsorption on PCN subsequent electron-transfer PMS, mediated by surface-bound complexes (PMS–PCN-0.5). The main products were chlorinated oligomers (mostly dimeric biphenolic compounds), which adsorbed deteriorated carbocatalyst. Overall, this study offers new insights rational design nitrogen-enriched carbocatalysts, advances mechanistic understanding critical role during

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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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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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, Год журнала: 2021, Номер 287, С. 119963 - 119963

Опубликована: Фев. 7, 2021

Язык: Английский

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Activation of peroxymonosulfate by biochar-based catalysts and applications in the degradation of organic contaminants: A review

Chemical Engineering Journal, Год журнала: 2021, Номер 416, С. 128829 - 128829

Опубликована: Фев. 24, 2021

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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Single-Atom Fe Catalyst Outperforms Its Homogeneous Counterpart for Activating Peroxymonosulfate to Achieve Effective Degradation of Organic Contaminants

Environmental Science & Technology, Год журнала: 2021, Номер 55(10), С. 7034 - 7043

Опубликована: Фев. 23, 2021

Recently, reactive iron species (RFeS) have shown great potential for the selective degradation of emerging organic contaminants (EOCs). However, rapid generation RFeS and efficient EOCs over a wide pH range is still challenging. Herein, we constructed FeN4 structures on carbon nanotube (CNT) to obtain single-atom catalysts (FeSA-N-CNT) generate in presence peroxymonosulfate (PMS). The obtained FeSA-N-CNT/PMS system exhibited outstanding reactivity oxidizing (3.0-9.0). Several lines evidences suggested that existing as an FeN4═O intermediate was predominant oxidant, while SO4·- HO· were secondary oxidants. Density functional theory calculation results revealed CNT played key role optimizing distribution bonding antibonding states Fe 3d orbital, resulting ability FeSA-N-CNT PMS chemical adsorption activation. Moreover, could significantly enhance by increasing overlap electrons O 2p bisphenol A near Fermi level. this study can advance understanding heterogeneous application real practice.

Язык: Английский

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Correlation of Active Sites to Generated Reactive Species and Degradation Routes of Organics in Peroxymonosulfate Activation by Co-Loaded Carbon

Environmental Science & Technology, Год журнала: 2021, Номер 55(23), С. 16163 - 16174

Опубликована: Ноя. 18, 2021

Peroxymonosulfate (PMS)-based advanced oxidation processes (PMS-AOPs) as an efficient strategy for organic degradation are highly dependent on catalyst design and structured active sites. However, the identification of sites their relationship with reaction mechanisms not fully understood a composite due to complex structure. Herein, we developed family Co encapsulated in N-doped carbons (Co-PCN) tailored types contents via manipulated pyrolysis PMS activation ciprofloxacin (CIP) degradation, focusing correlation generated reactive species routes organics. The structure-function relationships between different Co-PCN catalysts oxygen (ROS), well bond breaking position CIP, were revealed through regression analysis density functional theory calculation. Co-Nx, O-C═O, C═O, graphitic N, defects stimulate generation 1O2 oxidizing C-C piperazine ring CIP into C═O. substitution F by OH hydroxylation might be induced SO4•- •OH, whose formation was affected C-O, Co(0), defects. findings provided new insights PMS-AOP systems rational ROS-oriented pollutants.

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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