Single-atom Ni-N4 sites coordinate dual nonradical oxidation pathways via peroxymonosulfate activation: Computational insights and in situ spectroscopic analyses

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 346, С. 123752 - 123752

Опубликована: Янв. 21, 2024

In this work, we revealed a dual-pathway nonradical oxidation (NRO) system catalyzed by Ni single atom catalyst (NiN4) accommodated in the carbon nitride substrate. The monatomic coordinated with four N atoms (Ni-N4) is determined as dynamic catalytic center for peroxymonosulfate (PMS) activation, showing an exceptional specific rate constant of 3.34 min-1 g-2 L-2 (29.7 times that CN/PMS system) oxidizing bisphenol A and other refractory organics. situ Raman, X-ray absorption, electrochemical analyses well theoretical simulations demonstrate Ni-N4 sites exhibit strong interaction PMS benefited from modulated electronic structures, resulting surface-bonding active complexes (NiN4-PMS*) deuterogenic high-valent Ni(IV)-Oxo species. NRO process will spontaneously coordinate both electron transfer via CN matrix direct selective organic excellent anti-interference ability adaptability.

Язык: Английский

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Deactivation of porphyrin metal-organic framework in advanced oxidation process: Photobleaching and underlying mechanism

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 346, С. 123746 - 123746

Опубликована: Янв. 16, 2024

Язык: Английский

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Electro-driven cycling Fenton catalysis through two-dimensional electroresponsive metal–organic frameworks for water purification

Nature Water, Год журнала: 2024, Номер 2(8), С. 793 - 802

Опубликована: Июль 1, 2024

Язык: Английский

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The structure-performance relationships in active center size-dependent Fenton-like catalysis: From nanoparticles to single atoms

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 355, С. 124157 - 124157

Опубликована: Май 9, 2024

Язык: Английский

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Current Mechanism of Peroxymonosulfate Activation by Cobalt-Based Heterogeneous Catalysts in Degrading Organic Compounds

ACS ES&T Engineering, Год журнала: 2023, Номер 4(1), С. 19 - 46

Опубликована: Авг. 14, 2023

Persulfate based advanced oxidation processes (PS-AOPs) have been regarded as a mainstream degradation technology of organic compounds due to their high efficiency in wastewater treatment. In particular, peroxymonosulfate (PMS) has unique structure and chemical properties, which can be efficiently activated by Co-based catalysts produce active species with potential. These usually determine the subsequent an efficient process, while intrinsic reaction mechanism behind this complex process remains unclear therefore impedes continual development scientific community. Recently, density functional theory (DFT) calculations emerged powerful means identify electronic properties distinguish energy changes PMS activation system. With assistance quantum calculation, increasing investigations conducted focusing on explaining phenomenon that occurred experiments. However, these mainly contributed part sometimes even differ from each other, lacking comprehensive summary DFT calculation results. review, we introduce main uses catalytic PMS, provide recent application examples heterogeneous different structures, then discuss detail. Finally, research results method field are summarized, future focus challenges put forward, is conducive guiding practical design further PS-AOPs creating value products.

Язык: Английский

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Carbon-based single-atom catalysts in advanced oxidation reactions for water remediation: From materials to reaction pathways

Eco-Environment & Health, Год журнала: 2023, Номер 2(2), С. 47 - 60

Опубликована: Апрель 26, 2023

Single-atom catalysts (SACs) have been widely recognized as state-of-the-art in environment remediation because of their exceptional performance, 100% metal atomic utilization, almost no secondary pollution, and robust structures. Most recently, the activation persulfate with carbon-based SACs advanced oxidation processes (AOPs) raises tremendous interest degradation emerging contaminants wastewater, owning to its efficient versatile reactive oxidant species (ROS) generation. However, comprehensive critical review unraveling underlying relationship between structures corresponding generated ROS is still rare. Herein, we systematically summarize fundamental understandings intrinsic mechanisms single atom active sites produced during AOPs. The types are firstly elaborated, presenting prior pollutants that need be degraded. Then, preparation characterization methods overviewed. material structure–ROS type persulfate-based AOPs discussed depth expound catalytic mechanisms. Finally, briefly conclude current development propose prospects for rational design synthesis on-demand performances future research.

Язык: Английский

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Conjugated Microporous Polymers‐Based Catalytic Membranes with Hierarchical Channels for High‐Throughput Removal of Micropollutants

Advanced Science, Год журнала: 2024, Номер 11(29)

Опубликована: Июнь 3, 2024

Abstract Engineering a catalytic membrane capable of efficiently removing emerging organic microcontaminants under ultrahigh flux conditions is significance for water purification. Herein, drawing inspiration from the functional attributes lymphatic vessels involved in immunosurveillance and fluid transport with minimal energy consumption, novel hierarchical porous engineered. This membrane, based on an innovative nitrogen‐rich conjugated microporous polymer (polytripheneamine, PTPA), synthesized using electrospinning coupled situ polymerization approach. The resulting bioinspired channels comprises thin layer (≈1.7 µm) crosslinked PTPA nanoparticles covering interconnected electrospun nanofibers. unique design creates intrinsic angstrom‐confined system activating peroxymonosulfate (PMS) to generate 98.7% singlet oxygen ( 1 O 2 ), enabling durable highly efficient degradation microcontaminants. Additionally, presence mesoporous structure between macroporous within interwoven nanofibers enhances mass transfer efficiency facilitates high rates. Notably, prepared demonstrates enduring high‐efficiency performance superior permeance (>95% >2500 L m −2 h −1 bar ) sustained over 100 h. work introduces pathway high‐performance membranes removal

Язык: Английский

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Two-dimensional MBene combined with cobalt nanoparticles enabling highly efficient peroxymonosulfate activation for ornidazole degradation

Separation and Purification Technology, Год журнала: 2024, Номер 354, С. 128647 - 128647

Опубликована: Июль 2, 2024

Язык: Английский

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Imine-linked covalent organic frameworks with coordinated Co single atoms for efficient Fenton-like catalysis to degrade sulfamethoxazole

Journal of environmental chemical engineering, Год журнала: 2025, Номер unknown, С. 115749 - 115749

Опубликована: Фев. 1, 2025

Язык: Английский

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Metal-organic frameworks meet synthetic polymers for water decontamination: A critical review

Chemical Engineering Journal, Год журнала: 2023, Номер 476, С. 146684 - 146684

Опубликована: Окт. 14, 2023

Язык: Английский

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