High-efficient peroxymonosulfate activation for rapid atrazine degradation by FeSx@MoS2 derived from MIL-88A(Fe)

Journal of Hazardous Materials, Год журнала: 2022, Номер 440, С. 129723 - 129723

Опубликована: Авг. 6, 2022

Язык: Английский

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Crystallinity engineering for overcoming the activity–stability tradeoff of spinel oxide in Fenton-like catalysis

Proceedings of the National Academy of Sciences, Год журнала: 2023, Номер 120(15)

Опубликована: Апрель 5, 2023

A precise modulation of heterogeneous catalysts in structural and surface properties promises the development more sustainable advanced oxidation water purification technologies. However, while with superior decontamination activity selectivity are already achievable, maintaining a long-term service life such materials remains challenging. Here, we propose crystallinity engineering strategy to break activity-stability tradeoff metal oxides Fenton-like catalysis. The amorphous/crystalline cobalt-manganese spinel oxide (A/C-CoMnOx) provided highly active, hydroxyl group-rich surface, moderate peroxymonosulfate (PMS)-binding affinity charge transfer energy strong pollutant adsorption, trigger concerted radical nonradical reactions for efficient mineralization, thereby alleviating catalyst passivation by intermediate accumulation. Meanwhile, surface-confined reactions, benefited from enhanced adsorption pollutants at A/C interface, rendered A/C-CoMnOx/PMS system ultrahigh PMS utilization efficiency (82.2%) unprecedented (rate constant 1.48 min-1) surpassing almost all state-of-the-art catalysts. cyclic stability environmental robustness real treatment was also demonstrated. Our work unveils critical role material modulating catalytic pathways oxides, which fundamentally improves our understanding structure-activity-selectivity relationships may inspire design application beyond.

Язык: Английский

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Derivatives of two-dimensional MXene-MOFs heterostructure for boosting peroxymonosulfate activation: Enhanced performance and synergistic mechanism

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 323, С. 122136 - 122136

Опубликована: Ноя. 1, 2022

Язык: Английский

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Nearly zero peroxydisulfate consumption for persistent aqueous organic pollutants degradation via nonradical processes supported by in-situ sulfate radical regeneration in defective MIL-88B(Fe)

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 331, С. 122699 - 122699

Опубликована: Март 27, 2023

Язык: Английский

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Activation of peroxymonosulfate with cobalt embedded in layered δ-MnO2 for degradation of dimethyl phthalate: Mechanisms, degradation pathway, and DFT calculation

Journal of Hazardous Materials, Год журнала: 2023, Номер 451, С. 130901 - 130901

Опубликована: Янв. 31, 2023

Язык: Английский

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Oxygen vacancies-rich α@δ-MnO2 mediated activation of peroxymonosulfate for the degradation of CIP: The role of electron transfer process on the surface

Chemical Engineering Journal, Год журнала: 2023, Номер 458, С. 141415 - 141415

Опубликована: Янв. 12, 2023

Язык: Английский

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

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июнь 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.

Язык: Английский

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Transformative Removal of Aqueous Micropollutants into Polymeric Products by Advanced Oxidation Processes

Environmental Science & Technology, Год журнала: 2024, Номер 58(11), С. 4844 - 4851

Опубликована: Фев. 22, 2024

This perspective presents the latest advancements in selective polymerization pathways advanced oxidation processes (AOPs) for removal of featured organic pollutants wastewater. In radical-based homogeneous reactions, SO4• –-based systems exhibit superior oxidative activity toward aromatics with electron-donating substituents via single electron transfer and radical adduct formation (RAF). The produced cations subsequently undergo coupling reactions to produce polymers. For •OH-based oxidation, metal ions facilitate production monomer radicals RAF. Additionally, heterogeneous catalysts can mediate both persulfate activation without generating inorganic radicals. Metal-based will a direct pathway polymerization. contrast, carbon-based induce low-molecular-weight oligomers (≤4 units) an process. comparison mineralization, remarkably reduce peroxide usage, quickly separate from aqueous phase, generate polymeric byproducts. Thus, AOP-driven hold significant promise reducing carbon emission realizing recycling water treatment processes.

Язык: Английский

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Size‐Dependent Catalysis in Fenton‐like Chemistry: From Nanoparticles to Single Atoms

Advanced Materials, Год журнала: 2024, Номер 36(28)

Опубликована: Апрель 24, 2024

Abstract State‐of‐the‐art Fenton‐like reactions are crucial in advanced oxidation processes (AOPs) for water purification. This review explores the latest advancements heterogeneous metal‐based catalysts within AOPs, covering nanoparticles (NPs), single‐atom (SACs), and ultra‐small atom clusters. A distinct connection between physical properties of these catalysts, such as size, degree unsaturation, electronic structure, state, their impacts on catalytic behavior efficacy reactions. In‐depth comparative analysis metal NPs SACs is conducted focusing how particle size variations metal‐support interactions affect species pathways. The highlights cutting‐edge characterization techniques theoretical calculations, indispensable deciphering complex structural characteristics active sites downsized particles. Additionally, underscores innovative strategies immobilizing onto membrane surfaces, offering a solution to inherent challenges powdered catalysts. Recent advances pilot‐scale or engineering applications Fenton‐like‐based devices also summarized first time. paper concludes by charting new research directions, emphasizing catalyst design, precise identification reactive oxygen species, in‐depth mechanistic studies. These efforts aim enhance application potential nanotechnology‐based AOPs real‐world wastewater treatment.

Язык: Английский

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Oxidative polymerization versus degradation of organic pollutants in heterogeneous catalytic persulfate chemistry

Water Research, Год журнала: 2024, Номер 255, С. 121485 - 121485

Опубликована: Март 18, 2024

Catalytic polymerization pathways in advanced oxidation processes (AOPs) have recently drawn much attention for organic pollutant elimination owing to the rapid removal kinetics, high selectivity, and recovery of carbon from wastewater. This work presents a review on regimes AOPs their applications wastewater decontamination. The mainly highlights three critical issues reactions induced by persulfate activation (Poly-PS-AOPs), including heterogeneous catalysts, pathways, properties substrates. dominant influencing factors selection reactive oxygen species, substrates are discussed detail. Moreover, we systematically demonstrate merits challenges Poly-PS-AOPs upon degradation polymer synthesis. We particularly highlight that technology could be promising treatment industrial containing heterocyclic organics synthesis polymers polymer-functionalized materials environmental energy applications.

Язык: Английский

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