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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Rational modulation of Fe single-atom electronic structure in a Fe-N2B4 configuration for preferential 1O2 generation in Fenton-like reactions

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 344, С. 123643 - 123643

Опубликована: Дек. 21, 2023

Язык: Английский

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Active Center Size-Dependent Fenton-Like Chemistry for Sustainable Water Decontamination

Environmental Science & Technology, Год журнала: 2023, Номер 57(50), С. 21416 - 21427

Опубликована: Дек. 8, 2023

Accurately controlling catalytic activity and mechanism as well identifying structure–activity–selectivity correlations in Fenton-like chemistry is essential for designing high-performance catalysts sustainable water decontamination. Herein, active center size-dependent with single cobalt atoms (CoSA), atomic clusters (CoAC), nanoparticles (CoNP) were fabricated to realize the changeover of peroxymonosulfate (PMS)-based chemistry. Catalytic durability vary change metal sizes. Besides, reducing size from significantly modulates contributions radical nonradical mechanisms, thus achieving selective/nonselective degradation. Density functional theory calculations reveal evolutions mechanisms systems over different Gibbs free energies reactive oxygen species generation. Single-atom site contact PMS preferred induce while dissociates generates radicals on nanoparticles. Differences originating reaction endow developed selectivity mineralization treating actual hospital wastewater column reactors. This work brings an in-depth understanding effects guides design intelligent fulfill demand specific scenes purification.

Язык: Английский

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Overcoming metals redox rate limitations in spinel oxide-driven Fenton-like reactions via synergistic heteroatom doping and carbon anchoring for efficient micropollutant removal

Water Research, Год журнала: 2024, Номер 261, С. 122020 - 122020

Опубликована: Июнь 29, 2024

Язык: Английский

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The structure-performance relationships in active center size-dependent Fenton-like catalysis: From nanoparticles to single atoms

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 355, С. 124157 - 124157

Опубликована: Май 9, 2024

Язык: Английский

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Electro-driven cycling Fenton catalysis through two-dimensional electroresponsive metal–organic frameworks for water purification

Nature Water, Год журнала: 2024, Номер 2(8), С. 793 - 802

Опубликована: Июль 1, 2024

Язык: Английский

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The “4 + 1” strategy fabrication of iron single-atom catalysts with selective high-valent iron-oxo species generation

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(23)

Опубликована: Май 30, 2024

Single-atom catalysts (SACs) with atomic dispersion active sites have exhibited huge potentials in peroxymonosulfate (PMS)-based Fenton-like chemistry water purification. However, four-N coordination metal (MN 4 ) moieties often suffer from such problems as low selectivity and narrow workable pH. How to construct SACs a controllable strategy optimized electronic structures is of great challenge. Herein, an innovative (i.e., the “4 + 1” fabrication) was devised precisely modulate first-shell coordinated microenvironment FeN SAC using additional N (SA-FeN 5 ). This leads almost 100% selective formation high-valent iron-oxo [Fe(IV)═O] (steady-state concentration: 2.00 × 10 −8 M) SA-FeN /PMS system. In-depth theoretical calculations unveil that configuration optimizes electron distribution monatomic Fe sites, which thus fosters PMS adsorption reduces energy barrier for Fe(IV)═O generation. then attached polyvinylidene difluoride membrane continuous flow device, showing long-term abatement microcontaminant. work furnishes general effective activation metal-oxo species generation by high N-coordination number regulation SACs, would provide guidance rational design superior environmental

Язык: Английский

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Hydrogen Peroxide as an Ideal Electron Donor for Long-Lasting Fenton Chemistry: Strong Enhancement of Fe(III) Activity by Heteroatom-Doped Nanocarbons

ACS Catalysis, Год журнала: 2024, Номер 14(9), С. 6525 - 6534

Опубликована: Апрель 15, 2024

Heteroatom doping has been demonstrated to be an effective strategy improve the catalytic activity of carbon materials. Herein, heteroatom-doped nanocarbons were found environmental protection cocatalysts for promoting Fenton oxidation. Nitrogen-doped reduced graphene oxide (N-rGO) exhibited better than sulfur-, boron-, and phosphorus-doped rGO enhancing Unlike classical electron sacrificial agents, H2O2 was employed as donor enhance oxidation during catalysis N-rGO. Electrochemical analysis nitrogen molecular model tests indicated potential Fe(III) increased with improvement in N atom content (R2 = 0.97), revealing that Fe atoms FeOH2+ on N-rGO surface are more likely abstract electrons from H2O2. In addition, delocalized π is one active sites N-rGO-boosted oxidation, could facilitate transfer along C–C/C═C structures due conductivity ability Fe(III). Moreover, density functional theory (DFT) calculations suggest pyrrole species best site, resulting higher adsorption energy stretching Fe–O bond increase species. Therefore, study findings provide insight into designing stable efficient metal-free catalysts reactivity overcoming inherent drawbacks system.

Язык: Английский

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Selective degradation of organic pollutants by highly dispersed Fe, Ni anchored on nitrogen carbon activating persulfate system: Electron transfer promotion, the impact of pollutant redox and adsorption properties

Chemical Engineering Journal, Год журнала: 2024, Номер 490, С. 151585 - 151585

Опубликована: Апрель 23, 2024

Язык: Английский

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Nano-island-encapsulated cobalt single-atom catalysts for breaking activity-stability trade-off in Fenton-like reactions

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Янв. 2, 2025

Язык: Английский

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