Nanoconfinement steers nonradical pathway transition in single atom fenton-like catalysis for improving oxidant utilization

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 22, 2024

Abstract The introduction of single-atom catalysts (SACs) into Fenton-like oxidation promises ultrafast water pollutant elimination, but the limited access to pollutants and oxidant by surface catalytic sites intensive consumption still severely restrict decontamination performance. While nanoconfinement SACs allows drastically enhanced reaction kinetics, detailed regulatory mechanisms remain elusive. Here, we unveil that, apart from local enrichment reactants, pathway shift is also an important cause for reactivity enhancement nanoconfined SACs. electronic structure cobalt site altered confining it within nanopores mesostructured silica particles, which triggers a fundamental transition singlet oxygen electron transfer 4-chlorophenol oxidation. changed accelerated interfacial mass render system up 34.7-fold higher degradation rate raised peroxymonosulfate utilization efficiency (from 61.8% 96.6%) relative unconfined control. It demonstrates superior other electron-rich phenolic compounds, good environment robustness, high stability treating real lake water. Our findings deepen knowledge catalysis may inspire innovations in low-carbon purification technologies heterogeneous applications.

Language: Английский

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Tuning electronic structure of metal-free dual-site catalyst enables exclusive singlet oxygen production and in-situ utilization

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 9, 2024

Abstract Developing eco-friendly catalysts for effective water purification with minimal oxidant use is imperative. Herein, we present a metal-free and nitrogen/fluorine dual-site catalyst, enhancing the selectivity utilization of singlet oxygen ( 1 O 2 ) decontamination. Advanced theoretical simulations reveal that synergistic fluorine-nitrogen interactions modulate electron distribution polarization, creating asymmetric surface configurations electron-deficient nitrogen vacancies. These properties trigger selective generation from peroxymonosulfate (PMS) improve neighboring reactive species, facilitated by contaminant enrichment at fluorine-carbon Lewis-acid adsorption sites. Utilizing these insights, synthesize catalyst through montmorillonite (MMT)-assisted pyrolysis (NFC/M). This method leverages role MMT as an in-situ layer-stacked template, enabling controlled decomposition carbon, nitrogen, fluorine precursors resulting in enhanced structural adaptability, site accessibility, mass-transfer capacity. The NFC/M demonstrates impressive 290.5-fold increase phenol degradation efficiency than single-site analogs, outperforming most metal-based catalysts. work not only underscores potential precise electronic manipulations design but also advances development efficient sustainable solutions purification.

Language: Английский

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Ce-doped CuCoO2 delafossite with switchable PMS activation pathway for tetracycline degradation

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 481, P. 148633 - 148633

Published: Jan. 12, 2024

Language: Английский

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Fenton-like catalysis by MnO2 membrane reactor with oxygen vacancies for carbamazepine degradation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 353, P. 124106 - 124106

Published: April 22, 2024

Language: Английский

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Anthraquinone centers modified covalent organic frameworks for boosted photocatalytic O2-to-H2O2 synthesis: Inhibiting the in-situ decomposition of H2O2

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 481, P. 148494 - 148494

Published: Jan. 4, 2024

Language: Английский

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Coordination engineering of heterogeneous high-valent Fe(IV)-oxo for safe removal of pollutants via powerful Fenton-like reactions

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 19, 2024

Coordination engineering of high-valent Fe(IV)-oxo (FeIV=O) is expected to break the activity-selectivity trade-off traditional reactive oxygen species, while attempts regulate oxidation behaviors heterogeneous FeIV=O remain unexplored. Here, by coordination Fe-Nx single-atom catalysts (Fe-Nx SACs), we propose a feasible approach FeIV=O. The developed Fe-N2 SACs/peroxymonosulfate (PMS) system delivers boosted performance for generation, and thereby can selectively remove range pollutants within tens seconds. In-situ spectra theoretical simulations suggest that low-coordination SACs favor generation via PMS activation as providing more electrons facilitate desorption key *SO4H intermediate. Due their disparate attacking sites sulfamethoxazole (SMX) molecules, mediated (FeIVN2=O) oxidize SMX small molecules with less toxicity, FeIVN4=O produces series toxic azo compounds through N-N coupling complex pathways. may species but controllable remains authors alter number

Language: Английский

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Understanding the multiple roles of electrified MXene filter toward boosting the Fenton-like reaction

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 343, P. 127092 - 127092

Published: March 12, 2024

Language: Английский

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N-doped CuFe-MOF-919 derivatives in activation of peroxymonosulfate for enhanced degradation of organic pollutants: 1O2 dominated non-radical pathway

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 345, P. 127324 - 127324

Published: April 4, 2024

Language: Английский

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Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 356, P. 124216 - 124216

Published: May 18, 2024

Language: Английский

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Site-designed dual-active-center catalysts for co-catalysis in advanced oxidation processes

npj Materials Sustainability, Journal Year: 2025, Volume and Issue: 3(1)

Published: Jan. 7, 2025

Abstract Advanced Oxidation Processes (AOPs) are promising for treating persistent pollutants, yet challenges arise due to the step-wise oxidants activation process, which traditional single-active-center catalysts struggle facilitate effectively. Recently, dual-active-center have emerged as a solution by enabling synergistic reactions. This review covers advances in these catalysts, their co-catalytic mechanisms, and applications electro-Fenton, photocatalytic, peroxymonosulfate-, pollutant-as-electron-donor based Fenton-like processes, along with active site design considerations future challenges.

Language: Английский

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