Ultrafast degradation of emerging organic pollutants via activation of peroxymonosulfate over Fe3C/Fe@N-C-x: Singlet oxygen evolution and electron-transfer mechanisms

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 321, P. 122034 - 122034

Published: Oct. 10, 2022

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

Water Research, Journal Year: 2023, Volume and Issue: 235, P. 119925 - 119925

Published: March 28, 2023

Language: Английский

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Sustainable Fe(III)/Fe(II) cycles triggered by co-catalyst of weak electrical current in Fe(III)/peroxymonosulfate system: Collaboration of radical and non-radical mechanisms

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 317, P. 121716 - 121716

Published: July 8, 2022

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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Oxygen vacancies-enriched Cu/Co bimetallic oxides catalysts for high-efficiency peroxymonosulfate activation to degrade TC: Insight into the increase of Cu+ triggered by Co doping

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 450, P. 138302 - 138302

Published: July 25, 2022

Language: Английский

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Mechanism of the application of single-atom catalyst-activated PMS/PDS to the degradation of organic pollutants in water environment: A review

Journal of Cleaner Production, Journal Year: 2023, Volume and Issue: 397, P. 136468 - 136468

Published: Feb. 23, 2023

Language: Английский

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A multiple Kirkendall strategy for converting nanosized zero-valent iron to highly active Fenton-like catalyst for organics degradation

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(39)

Published: Sept. 19, 2023

Nanosized zero-valent iron (nZVI) is a promising persulfate (PS) activator, however, its structurally dense oxide shell seriously inhibited electrons transfer for O-O bond cleavage of PS. Herein, we introduced sulfidation and phosphorus-doped biochar breaking the pristine with formation FeS FePO 4 -containing mixed shell. In this case, faster diffusion rate atoms compared to components triggered multiple Kirkendall effects, causing inward fluxion vacancies further coalescing into radial nanocracks. Exemplified by trichloroethylene (TCE) removal, such unique “lemon-slice-like” nanocrack structure favored fast outward ferrous ions across PS activation high-efficient generation utilization reactive species, as evidenced effective dechlorination (90.6%) mineralization (85.4%) TCE. O 2 • - contributed most TCE decomposition, moreover, SnZVI@PBC gradually became electron-deficient thus extracted from achieving nonradical-based degradation. Compared nZVI/PS process, SnZVI@PBC/PS system could significantly reduce catalyst dosage (87.5%) amount (68.8%) achieve nearly complete degradation, was anti-interference, stable, pH-universal. This study advanced mechanistic understandings effects-triggered on nZVI corresponding rational design Fenton-like catalysts organics

Language: Английский

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Revealing the fundamental role of MoO2 in promoting efficient and stable activation of persulfate by iron carbon based catalysts: Efficient Fe2+/Fe3+ cycling to generate reactive species

Water Research, Journal Year: 2022, Volume and Issue: 225, P. 119142 - 119142

Published: Sept. 23, 2022

Language: Английский

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