Fenton-like activity and pathway modulation via single-atom sites and pollutants comediates the electron transfer process

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(3)

Опубликована: Янв. 8, 2024

The studies on the origin of versatile oxidation pathways toward targeted pollutants in single-atom catalysts (SACs)/peroxymonosulfate (PMS) systems were always associated with coordination structures rather than perspective pollutant characteristics, and analysis mechanism commonality is lacking. In this work, a variety (M-SACs, M: Fe, Co, Cu) fabricated via pyrolysis process using lignin as complexation agent substrate precursor. Sixteen kinds commonly detected various references selected, their ln k obs values M-SACs/PMS correlated well ( R 2 = 0.832 to 0.883) electrophilic indexes (reflecting electron accepting/donating ability pollutants) energy gap 0.801 0.840) between complexes. Both transfer (ETP) radical can be significantly enhanced systems, while was overwhelmed by ETP lower indexes. contrast, higher represented weaker electron-donating capacity complexes, which resulted accompanied noticeable oxidation. addition, different regulated gaps complexes pollutants. As result, Fenton-like activities could modulated reaction pathways, determined both sites. This work provided strategy establish PMS-based AOP tunable capacities for high-efficiency organic decontamination.

Язык: Английский

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Selective degradation of organic micropollutants by activation of peroxymonosulfate by Se@NC: Role of Se doping and nonradical pathway mechanism

Journal of Hazardous Materials, Год журнала: 2023, Номер 452, С. 131202 - 131202

Опубликована: Март 15, 2023

Язык: Английский

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Elucidation of the mechanistic origin of spin-state-dependent P-doped Fe single-atom catalysts for the oxidation of organic pollutants through peroxymonosulfate activation

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 341, С. 123289 - 123289

Опубликована: Сен. 14, 2023

Язык: Английский

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Modulating Electronic Structure Engineering of Atomically Dispersed Cobalt Catalyst in Fenton-like Reaction for Efficient Degradation of Organic Pollutants

Environmental Science & Technology, Год журнала: 2023, Номер 57(37), С. 14071 - 14081

Опубликована: Сен. 8, 2023

Currently, the lack of model catalysts limits understanding catalytic essence. Herein, we report functional group modification single atom (SACs) with an accurately regulated electronic structure for accelerating sluggish kinetics Fenton-like reaction. The amino-modified cobalt phthalocyanine anchored on graphene (CoPc/G-NH2) shows superior performance in peroxymonosulfate (PMS) based reaction Co mass-normalized pseudo-first-order rate constants (kobs, 0.2935 min-1), which is increased by 4 and 163 times compared to those CoPc/G (0.0737 min-1) Co3O4/G (0.0018 min-1). Density theory (DFT) calculations demonstrate that -NH2 narrows gap between d-band center Fermi level a atom, strengthens charge transfer at interface reduces free energy barrier activation PMS. Moreover, scale-up experiment realizes 100% phenol removal 7200-bed volumes during 240 h continuous operation without obvious decline performance. This work provides in-depth insight into mechanism reactions demonstrates engineering SACs as effective strategy improving activity achieve goal practical application.

Язык: Английский

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A Novel Dual-Channel Carbon Nitride Homojunction with Nanofibrous Carbon for Significantly Boosting Photocatalytic Hydrogen Peroxide Production

Advanced Fiber Materials, Год журнала: 2024, Номер 6(2), С. 387 - 400

Опубликована: Янв. 9, 2024

Язык: Английский

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Enhanced electron transfer-based nonradical activation of peroxymonosulfate by CoNx sites anchored on carbon nitride nanotubes for the removal of organic pollutants

Chemical Engineering Journal, Год журнала: 2023, Номер 466, С. 143155 - 143155

Опубликована: Апрель 23, 2023

Язык: Английский

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Ultrafast oxidation of refractory organics via PMS activation by Si-O doped biomimetic montmorillonite: Simultaneous enhanced radical/electron transfer pathways and efficient catalytic membrane system

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 342, С. 123428 - 123428

Опубликована: Окт. 24, 2023

Язык: Английский

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Application of 3D hierarchical porous NiCo-spinel nanosheet array for enhancement of synergistic activation of peroxymonosulfate: Degradation, Intermediates, mechanism and degradation pathway of tetracycline

Chemical Engineering Journal, Год журнала: 2024, Номер 481, С. 148506 - 148506

Опубликована: Янв. 4, 2024

Язык: Английский

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Photothermal-synergistic peroxymonosulfate activation promoting carbamazepine degradation by Porphyra-derived porous biochar composites: Performance, mechanism, transformation pathway and practical application

Chemical Engineering Journal, Год журнала: 2024, Номер 489, С. 151263 - 151263

Опубликована: Апрель 12, 2024

Язык: Английский

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Nitrogen-doped biochar/MnO2 as an efficient PMS activator for synergistic BPA degradation via non-free radical pathways in the water

Journal of environmental chemical engineering, Год журнала: 2024, Номер 12(2), С. 112446 - 112446

Опубликована: Март 8, 2024

Язык: Английский

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