Isomerization of Covalent Organic Frameworks for Efficiently Activating Molecular Oxygen and Promoting Hydrogen Peroxide Photosynthesis

Small, Год журнала: 2024, Номер unknown

Опубликована: Сен. 27, 2024

Abstract Constitutional‐isomerized covalent organic frameworks (COFs), constructed by swapping monomers around imine bonds, have attracted attention for their distinct optoelectronic properties, which significantly impact photocatalytic performance. However, limited research has delved into the inherent relationship between isomerization and enhancement of H 2 O photosynthesis. Herein, a pair isomeric COFs linked bonds (PB‐PT‐COF PT‐PB‐COF) is synthesized, it proved that exhibit different rate‐determining steps in generation process , resulting twofold increase efficiency. Specifically, PT‐PB‐COF demonstrates effective adsorption activation molecular oxygen (O + e − → •O ), leading to significant improvement In contrast, PB‐PT‐COF exhibits robust interaction with O, enabling direct oxidation (H h ). This study provides thorough understanding intrinsic mechanism underlying constitutional‐isomerized generation, offering insights further optimizing building units.

Язык: Английский

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Quasi-One-Dimensional Zigzag Covalent Organic Frameworks for Photocatalytic Hydrogen Evolution from Water

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(38), С. 26198 - 26206

Опубликована: Сен. 10, 2024

Covalent organic frameworks (COFs) have potential applications in a wide range of fields. However, it remains critical challenge to constrain their covalent expansions the one-dimensional (1D) direction. Here, we developed general approach fabricate 15 different highly crystalline COFs with zigzag-packed 1D porous chains through condensation V-shaped ditopic linkers and X-shaped tetratopic knots. Appropriate geometrical combinations scope knots distinct aromatic cores, linkages, functionalities offer series quasi-1D dominant pore sizes 7-13 Å surface areas 116-784 m

Язык: Английский

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3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Янв. 28, 2025

Abstract Artificial photosynthesis of urea from NH 3 and CO 2 seems to remain still essentially unexplored. Herein, three isomorphic three-dimensional covalent organic frameworks with twofold interpenetrated ffc topology are functionalized by benzene, pyrazine, tetrazine active moieties, respectively. A series experiment results disclose the gradually enhanced conductivity, light-harvesting capacity, photogenerated carrier separation efficiency, co-adsorption capacity towards in order benzene-, pyrazine-, tetrazine-containing framework. This turn endows framework superior photocatalytic activity production yield 523 μmol g −1 h , 40 4 times higher than that for benzene- pyrazine-containing framework, respectively, indicating heterocyclic N microenvironment-dependent catalytic performance these photocatalysts. is further confirmed in-situ spectroscopic characterization density functional theory calculations. work lays a way sustainable urea.

Язык: Английский

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Triazine- and triphenylamine-based covalent organic frameworks as photocatalyst for the synthesis of 2-aryl-2H-indazoles by cyclization reaction

Molecular Catalysis, Год журнала: 2025, Номер 573, С. 114823 - 114823

Опубликована: Янв. 11, 2025

Язык: Английский

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Implantation of non-metal redox sites in conjugated triazine frameworks for visible-light-driven reduction of CO2 to C2+ products

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер unknown, С. 125123 - 125123

Опубликована: Фев. 1, 2025

Язык: Английский

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Nitrogen‐Doped Engineering in Covalent Organic Frameworks for Photocatalytic Synthesis of Hydrogen Peroxide^†

Chinese Journal of Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Март 21, 2025

Comprehensive Summary Photocatalytic synthesis of hydrogen peroxide (H 2 O ) from air and water presents a sustainable efficient alternative to the traditional anthraquinone method. Therefore, design photocatalysts for H production are important. In this work, we apply nitrogen‐site engineering strategy achieve high‐performance by synthesizing three imine‐ linked oligo(phenylenevinylene)‐based covalent organic frameworks (OPV‐COFs) doped with different numbers nitrogen atoms (denoted as COF‐920‐ n N, = 0, 1, 3). characterization confirmed high crystallinity porosity COFs, critical photocatalysis. Each OPV‐COF exhibited ability rapidly synthesize using water, COF‐920‐1N achieving highest rate 4288 μmol·g –1 ·h under visible light, higher than those most other reported COFs. Mechanism studies demonstrated that introduction pyridine at junction changes electronic structure electron transfer path within enhancing photogenerated mobility reducing electron‐hole recombination. This study not only pioneers class OPV‐COFs photocatalytic , but also sets foundational rational COFs in applications.

Язык: Английский

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Flexible Units in Covalent Organic Frameworks Promote Photocatalytic Uranium Extraction from Wastewater

Research Square (Research Square), Год журнала: 2025, Номер unknown

Опубликована: Апрель 29, 2025

Covalent organic frameworks (COFs) are increasingly being utilized in photocatalysis due to their programmable band gaps and pore geometries. Flexible COFs currently of interest for selective sorption, though use has received little attention date. Herein, we propose a strategy modulating the flexible units facilitate efficient charge carrier separation transfer during photocatalysis. Rotational freedom linkers our led controllable local curvature, thereby optimizing optoelectronic properties boosting photocatalytic activity. One developed (COF-3) showed excellent performance uranium removal from contaminated groundwater tap water. Mechanistic studies revealed that COF-3 photocatalytically generated H₂O₂ under visible light irradiation water, which transformed UO₂²⁺ solid (UO₂)O₂·2H₂O through redox pathway. The results demonstrate an effective design towards COF photocatalysts water potentially many other applications.

Язык: Английский

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Covalent organic framework-based surface plasmon-enhanced fluorescence sensing for real-time monitoring of cell apoptosis

Biosensors and Bioelectronics, Год журнала: 2025, Номер unknown, С. 117569 - 117569

Опубликована: Май 1, 2025

Язык: Английский

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The Role of Reticular Chemistry in Photoenzymatic Reaction

Green Chemistry, Год журнала: 2024, Номер 26(23), С. 11468 - 11489

Опубликована: Янв. 1, 2024

Photoenzymatic catalysis faces challenges like low stability and recyclability. Reticular framework materials offer solutions by enabling enzyme protection reuse. This review highlights recent advances, design strategies, future directions.

Язык: Английский

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Catalytic Applications of Organic-Inorganic Hybrid Porous Materials

Chemical Communications, Год журнала: 2024, Номер 60(91), С. 13325 - 13335

Опубликована: Янв. 1, 2024

Organic-inorganic hybrid porous materials (OIHMs) inherit the unique properties from both organic and inorganic components, flexibility in incorporation of functional groups renders OIHMs an ideal platform for construction catalytic with multiple active sites. The preparation precise locations organic-inorganic components tunable structures is one important topics application OIHMs, but it still very challenging. In this feature article, we describe our work related to

Язык: Английский

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