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

Environmental Science & Technology, Journal Year: 2021, Volume and Issue: 56(1), P. 78 - 97

Published: Dec. 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.

Language: Английский

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Photo-Fenton degradation of tetracycline over Z-scheme Fe-g-C3N4/Bi2WO6 heterojunctions: Mechanism insight, degradation pathways and DFT calculation

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 310, P. 121326 - 121326

Published: March 16, 2022

Language: Английский

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Activation of peroxymonosulfate by single atom Co-N-C catalysts for high-efficient removal of chloroquine phosphate via non-radical pathways: Electron-transfer mechanism

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 429, P. 132245 - 132245

Published: Sept. 3, 2021

Language: Английский

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Recent research progress of bimetallic phosphides-based nanomaterials as cocatalyst for photocatalytic hydrogen evolution

Chinese Chemical Letters, Journal Year: 2021, Volume and Issue: 33(3), P. 1141 - 1153

Published: July 30, 2021

Language: Английский

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Oxygen doping of cobalt-single-atom coordination enhances peroxymonosulfate activation and high-valent cobalt–oxo species formation

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(16)

Published: April 11, 2023

The high-valent cobalt-oxo species (Co(IV)=O) is being increasingly investigated for water purification because of its high redox potential, long half-life, and antiinterference properties. However, generation Co(IV)=O inefficient unsustainable. Here, a cobalt-single-atom catalyst with N/O dual coordination was synthesized by O-doping engineering. O-doped (Co-OCN) greatly activated peroxymonosulfate (PMS) achieved pollutant degradation kinetic constant 73.12 min-1 g-2, which 4.9 times higher than that Co-CN (catalyst without O-doping) those most reported single-atom catalytic PMS systems. Co-OCN/PMS realized dominant oxidation pollutants increasing the steady-state concentration (1.03 × 10-10 M) 5.9 compared Co-CN/PMS. A competitive kinetics calculation showed contribution to micropollutant 97.5% during process. Density functional theory calculations influenced charge density (increased Bader transfer from 0.68 0.85 e), optimized electron distribution Co center d-band -1.14 -1.06 eV), enhanced adsorption energy -2.46 -3.03 eV, lowered barrier key reaction intermediate (*O*H2O) formation 1.12 0.98 eV. Co-OCN fabricated on carbon felt flow-through device, continuous efficient removal micropollutants (degradation efficiency >85% after 36 h operation). This study provides new protocol activation elimination through heteroatom-doping metal-oxo purification.

Language: Английский

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Modulation of Charge Trapping by Island‐like Single‐Atom Cobalt Catalyst for Enhanced Photo‐Fenton‐Like reaction

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(12)

Published: Jan. 6, 2023

Abstract Composites‐based photocatalysis relies on the interfacial electron transfer between metallic cocatalyst and photosensitizer (the semiconductor) to realize spatial separation of charge carriers. Herein, an ingenious heterojunction Co‐CN single atom catalysts (SACs) g‐C 3 N 4 is constructed for heterogeneous photo‐Fenton‐like reactions. Driven by built‐in electric field across heterojunctions, migration photogenerated carriers promoted, leading fast from SACs. Theoretical calculations transient absorption spectroscopy reveal modulated trapping in SA‐Co‐CN/g‐C heterostructure, resulting remarkably enhanced generation reactive oxygen species via peroxymonosulfate activation under light irradiation. This /PMS/vis system efficient oxidation various antibiotics with high removal efficiency (>98%), a wide operating pH range (pH 3–11) excellent stability long‐term operation. study provides new tactic rational design SACs‐based heterojunctions bridge catalysis, attaining superior photoredox activity coupling.

Language: Английский

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Outlook on Single Atom Catalysts for Persulfate-Based Advanced Oxidation

ACS ES&T Engineering, Journal Year: 2022, Volume and Issue: 2(10), P. 1776 - 1796

Published: Sept. 7, 2022

Single atom catalysts (SACs) have emerged as a promising catalyst material architecture for energy, chemical, and environmental applications. In the past several years, SACs been increasingly explored persulfate-based advanced oxidation processes (AOPs) due to their superior persulfate activation pollutant degradation performance compared benchmark dissolved ion nanoparticle catalysts. However, there still exist uncertainties on mechanism of by SACs, which involves complex interplay sulfate hydroxyl radicals, singlet oxygen, high-valent metal species, and/or mediated electron transfer. Questions also remain how ions molecularly align single site, are converted into reactive what design parameters lead higher efficiency degradation. this critical review, we examine SAC materials employed AOPs discuss they function differently counterparts. We further our discussion current limitations, opportunities, future research needs in (i) filling knowledge gaps mechanisms persulfate-SAC interactions; (ii) augmenting fundamental with theoretical simulation situ characterization techniques; (iii) improving tailored applications; (iv) proactively considering challenges associated engineering practices water matrixes.

Language: Английский

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Transition metal single-atom embedded on N-doped carbon as a catalyst for peroxymonosulfate activation: A DFT study

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 437, P. 135428 - 135428

Published: Feb. 23, 2022

Language: Английский

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Single atom Fe-dispersed graphitic carbon nitride (g-C3N4) as a highly efficient peroxymonosulfate photocatalytic activator for sulfamethoxazole degradation

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 430, P. 132937 - 132937

Published: Oct. 14, 2021

Language: Английский

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Fe-Mn oxycarbide anchored on N-doped carbon for enhanced Fenton-like catalysis: Importance of high-valent metal-oxo species and singlet oxygen

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 340, P. 123204 - 123204

Published: Aug. 22, 2023

Language: Английский

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