Generating dual-active species by triple-atom sites through peroxymonosulfate activation for treating micropollutants in complex water

Proceedings of the National Academy of Sciences, Год журнала: 2023, Номер 120(13)

Опубликована: Март 23, 2023

The peroxymonosulfate (PMS)-triggered radical and nonradical active species can synergistically guarantee selectively removing micropollutants in complex wastewater; however, realizing this on heterogeneous metal-based catalysts with single sites remains challenging due to insufficient electron cycle. Herein, we design asymmetric Co-O-Bi triple-atom Co-doped Bi2O2CO3 facilitate PMS oxidation reduction simultaneously by enhancing the transfer between sites. We propose that result an density increase Bi decrease Co sites, thereby undergoes a reaction generate SO4•- •OH at site 1O2 site. suggest synergistic effect of SO4•-, •OH, enables efficient removal mineralization without interference from organic inorganic compounds under environmental background. As result, achieves almost 99.3% sulfamethoxazole degradation 3 min k-value as high 82.95 min-1 M-1, which is superior existing reported so far. This work provides structural regulation approach control catalytic function, will guide rational Fenton-like catalysts.

Язык: Английский

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MOF Derived Co−Fe nitrogen doped graphite carbon@crosslinked magnetic chitosan Micro−nanoreactor for environmental applications: Synergy enhancement effect of adsorption−PMS activation

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 319, С. 121926 - 121926

Опубликована: Сен. 1, 2022

Язык: Английский

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Different reaction mechanisms of SO4•− and •OH with organic compound interpreted at molecular orbital level in Co(II)/peroxymonosulfate catalytic activation system

Water Research, Год журнала: 2022, Номер 229, С. 119392 - 119392

Опубликована: Ноя. 19, 2022

Язык: Английский

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Linkage Microenvironment of Azoles‐Related Covalent Organic Frameworks Precisely Regulates Photocatalytic Generation of Hydrogen Peroxide

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(36)

Опубликована: Июль 18, 2023

Artificial H2 O2 photosynthesis by covalent organic frameworks (COFs) photocatalysts is promising for wastewater treatment. The effect of linkage chemistry COFs as functional basis to photoelectrochemical properties and photocatalysis remains a significant challenge. In this study, three kinds azoles-linked including thiazole-linked TZ-COF, oxazole-linked OZ-COF imidazole-linked IZ-COF were successfully synthesized. More accessible channels charge transfer constructed in TZ-COF via the donor-π-acceptor structure between thiazole pyrene linker, leading efficient suppression photoexcited recombination. Density theory calculations support experimental studies, demonstrating that more favorable formation *O2 intermediate production than oxazole imidazole linkages. real active sites located at benzene ring fragment unit azole linkage.

Язык: Английский

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Enhanced and synergistic catalytic activation by photoexcitation driven S−scheme heterojunction hydrogel interface electric field

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Окт. 23, 2023

The regulation of heterogeneous material properties to enhance the peroxymonosulfate (PMS) activation degrade emerging organic pollutants remains a challenge. To solve this problem, we synthesize S-scheme heterojunction PBA/MoS2@chitosan hydrogel achieve photoexcitation synergistic PMS activation. constructed photoexcited carriers undergo redox conversion with through transfer pathway driven by directional interface electric field. Multiple pathways greatly reactive oxygen species generation, leading significant increase in doxycycline degradation rate. Meanwhile, 3D polymer chain spatial structure chitosan is conducive rapid capture and electron transport advanced oxidation process, reducing use transition metal activator limiting leaching ions. There reason believe that regulated will provide new perspective for future design research on enhancing heterologous catalysis process.

Язык: Английский

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Oxygen vacancy-induced spin polarization of tungsten oxide nanowires for efficient photocatalytic reduction and immobilization of uranium(VI) under simulated solar light

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 324, С. 122202 - 122202

Опубликована: Ноя. 20, 2022

Язык: Английский

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Catalysis Enhancement of Co₃O₄ through the Epitaxial Growth of Inert ZnO in Peroxymonosulfate Activation: The Catalytic Mechanism of Surface Hydroxyls in Singlet Oxygen Generation

Crystal Growth & Design, Год журнала: 2024, Номер unknown

Опубликована: Дек. 16, 2024

As a prevalent Co-contained catalyst, modified Co3O4 has been widely utilized to activate peroxymonosulfate (PMS) for organic wastewater treatment due its affordability and accessibility. While the catalysis enhancement of by catalytic inert species is often attributed formation oxygen vacancies (OVs), underlying mechanism beyond OVs remains unclear. Herein, we designed one-pot pyrolysis process synthesize ZnO/Co3O4 heterojunctions featuring Zn–Co tetrahedral coordination on their interface. In PMS-advanced oxidation methylene blue (MB), epitaxial growth ZnO surface led an 88-fold increase in activity, facilitating rapid degradation dyes achieve deep mineralization effluent. Co sites hydroxyls played crucial role PMS activation, generating variety reactive species. Among these species, singlet (1O2) was identified as dominant responsible MB degradation, with assistance sulfate radical. Theoretical calculations demonstrated that Zn–OH group easier than Co–OH through polarization during chemisorption. The activated groups served novel active sites, participating activation nonradical way generate partial 1O2. This study sheds new light effect (ZnO) enhancing activity Co3O4, refining our understanding generation route 1O2 activation.

Язык: Английский

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Establishing a high-speed electron transfer channel via CuS/MIL-Fe heterojunction catalyst for photo-Fenton degradation of acetaminophen

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 320, С. 121979 - 121979

Опубликована: Сен. 16, 2022

Язык: Английский

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Co3O4 with upshifted d-band center and enlarged specific surface area by single-atom Zr doping for enhanced PMS activation

Journal of Hazardous Materials, Год журнала: 2023, Номер 448, С. 130987 - 130987

Опубликована: Фев. 10, 2023

Язык: Английский

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Cobalt-based catalysts for heterogeneous peroxymonosulfate (PMS) activation in degradation of organic contaminants: Recent advances and perspectives

Journal of Alloys and Compounds, Год журнала: 2023, Номер 958, С. 170370 - 170370

Опубликована: Апрель 30, 2023

Язык: Английский

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