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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Activation of peroxymonosulfate by sludge-derived magnetic biochar for pollutant removal: Performance, applicability, and synergetic mechanism of iron species and carboxylated biochar

Chemical Engineering Journal, Год журнала: 2024, Номер 485, С. 149744 - 149744

Опубликована: Фев. 20, 2024

Язык: Английский

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Co-incorporation of nitrogen and boron into microscale zero-valent iron via mechanochemical ball-milling method improved Cr(Ⅵ) elimination: Performance and mechanism investigation

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 160050 - 160050

Опубликована: Янв. 1, 2025

Язык: Английский

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Tailoring the surface and interface structures of carbon nitride for enhanced photocatalytic self-Fenton process in pollutant degradation

Journal of Colloid and Interface Science, Год журнала: 2025, Номер 684, С. 831 - 843

Опубликована: Янв. 10, 2025

Язык: Английский

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Confinement Effect and Application in Catalytic Oxidation–Reduction Reaction of Confined Single-Atom Catalysts

ACS Catalysis, Год журнала: 2024, Номер 14(17), С. 12991 - 13014

Опубликована: Авг. 15, 2024

Single-atom catalysts (SACs) exhibit remarkable 100% atomic economy, making them highly efficient in various fields, including production processes, energy systems, and environmental remediation. However, the migration agglomeration of single atoms significantly diminish reactivity increase operating cost catalyst. Due to size effect, space confinement electron are stabilized, overall catalytic performance is also improved. The effect can be enhanced by modifying supporting materials with ordered regular pore structures improving binding mode between support atom. In this Review, confined functional structure will explained for synthesis SACs. It elucidates mechanisms formation elaborates how improves performance. This Review helpful better understanding, controlling, utilizing design SACs impressive

Язык: Английский

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Performance enhancement and mechanism of electroenhanced peroxymonosulfate activation by single-atom Fe catalyst modified electrodes

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(37)

Опубликована: Сен. 5, 2024

Peroxymonosulfate-based electrochemical advanced oxidation processes (PMS-EAOPs) have great potential for sustainable water purification, so an in-depth understanding of its catalytic mechanism is imperative to facilitate practical application. Herein, the performance enhancement and electroenhanced PMS activation by single-atom Fe catalyst modified carbon felt was investigated. Compared with anode, cathode exhibited faster bisphenol A degradation ( k = 0.073 vs. anode 0.015 min −1 ), increased consumption (98.8 10.3%), order magnitude reduction dissolution (0.068 0.787 mg L ). Mass transfer a key factor limiting activation, while electrostriction in hydrophobic region caused electric field (CEF) significantly mass coefficient m, 1.49 × 10 −4 2.68 −5 m s The enhanced synergistic result between electroactivation catalyst-activation, which controlled applied current density. 1 O 2 direct electron are main active species pathway, achieve high efficiency over pH 3 10. Density functional theory calculations prove CEF increases adsorption energy, lengthens O–O bond PMS, promotes charge transfer. flow-through convection unit achieves operation removal (99.5% 97.5%), low electrical energy (0.15 kWh log –1 –3 leaching (0.81% total single atom Fe). This work reveals critical role fields modulating Fenton-like activity, may advance development other electrocatalytic applications.

Язык: Английский

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Pore modulation of single atomic Fe sites for ultrafast Fenton-like chemistry with amplified electron migration oxidation

Water Research, Год журнала: 2024, Номер 268, С. 122545 - 122545

Опубликована: Сен. 30, 2024

Язык: Английский

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Modulating the electronic structure of Fe7S8@TCN enhancing peroxymonosulfate activation for efficient water decontamination: Importance of interfacial engineering

Separation and Purification Technology, Год журнала: 2025, Номер 362, С. 131862 - 131862

Опубликована: Янв. 31, 2025

Язык: Английский

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Overlooked Synergistic Effect Induced by Fe-Mo Dual-atom Catalyst in Water Remedation: Enhanced Electron Management and Efficient Pollutants Pre-activation

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер unknown, С. 125377 - 125377

Опубликована: Апрель 1, 2025

Язык: Английский

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Electron cycling mechanism in Fe/Mn DSAzyme accelerates BPA degradation and nanoenzyme regeneration

Journal of Hazardous Materials, Год журнала: 2024, Номер 476, С. 135228 - 135228

Опубликована: Июль 15, 2024

Язык: Английский

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