CrystEngComm, Journal Year: 2023, Volume and Issue: 25(32), P. 4511 - 4520
Published: Jan. 1, 2023
The imine COFs with longer linkers exhibited higher H 2 O photoproduction rate in pure water, owing to their more negative conductor band and better separation efficiency of photogenerated carriers.
Language: Английский
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)
Published: April 29, 2023
Optimizing the electronic structure of covalent organic framework (COF) photocatalysts is essential for maximizing photocatalytic activity. Herein, we report an isoreticular family multivariate COFs containing chromenoquinoline rings in COF and electron-donating or withdrawing groups pores. Intramolecular donor-acceptor (D-A) interactions allowed tuning local charge distributions carrier separation under visible light irradiation, resulting enhanced performance. By optimizing optoelectronic properties COFs, a uranium extraction efficiency 8.02 mg/g/day was achieved using nitro-functionalized multicomponent natural seawater, exceeding performance all reported to date. Results demonstrate effective design strategy towards high-activity with intramolecular D-A structures not easily accessible traditional synthetic approaches.
Language: Английский
Citations
196
Green Chemistry, Journal Year: 2023, Volume and Issue: 25(8), P. 3069 - 3076
Published: Jan. 1, 2023
Three highly crystalline and porous COFs with promising photoredox properties have been prepared. Via a post-sulfurization process, the imine-linked were converted into thiazole-linked COFs, generating conjugated ultrastable photocatalyst for H 2 O production.
Language: Английский
Citations
79
Materials Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 7(16), P. 3298 - 3331
Published: Jan. 1, 2023
This review provides an overview of the recent advances in heterogeneous catalysis using COFs, primarily from 2020 to 2023, covering fundamentals, advantages, current challenges, and future perspectives.
Language: Английский
Citations
64
Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)
Published: Feb. 10, 2024
Abstract Developing heterogeneous photocatalysts for the applications in harsh conditions is of high importance but challenging. Herein, by converting imine linkages into quinoline groups triphenylamine incorporated covalent organic frameworks (COFs), two photosensitive COFs, namely TFPA-TAPT-COF-Q and TFPA-TPB-COF-Q, are successfully constructed. The obtained quinoline-linked COFs display improved stability photocatalytic activity, making them suitable reactions under conditions, as verified recyclable acid involving oxidative decarboxylation base benzylamine coupling. Under strong condition, show a efficiency up to 11831.6 μmol·g −1 ·h long-term usability production H 2 O , while pristine imine-linked less catalytically active easily decomposed these conditions. results demonstrate that enhancing linkage robustness photoactive promising strategy construct catalysts
Language: Английский
Citations
64
ACS Applied Materials & Interfaces, Journal Year: 2023, Volume and Issue: 15(6), P. 8066 - 8075
Published: Feb. 1, 2023
Conversing oxygen (O2) to hydrogen peroxide (H2O2) driven by solar energy is a promising H2O2 onsite production route but often short of efficient and durable photocatalysts. Herein, strong π-π conjugate polycyclic aromatic benzene acetylene units have been constructed into new covalent organic frameworks (COFs) linked imine C═N bonding. These COFs demonstrated two-dimensional hexagonal crystalline with higher crystallinity larger surface area (>600 m2 g-1). Covalent benzene-acetylene possessed appropriate visible light-responsive band structure the suppressed charge recombination rate. The -OH groups on their enable them be weakly hydrophilic. As result, it served as high-performance photocatalysts for in water-benzyl alcohol (BA) two-phase system. It delivered rate 1240 μmol h-1 gcat-1 catalytic efficiency within 60 h, comparable best COF-based catalysts. This study provides an photocatalytic system based hydrophilic imine-linked
Language: Английский
Citations
55
Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(11), P. 6230 - 6239
Published: March 9, 2023
The library of imine-linked covalent organic frameworks (COFs) has grown significantly over the last two decades, featuring a variety morphologies, pore sizes, and applications. An array synthetic methods been developed to expand scope COF functionalities; however, most these were designed introduce functional scaffolds tailored specific application. Having general approach diversify COFs via late-stage incorporation group handles would greatly facilitate transformation materials into platforms for useful Herein, we report strategy in Ugi multicomponent reaction. To demonstrate versatility this approach, have synthesized with hexagonal kagome morphologies. We then introduced azide, alkyne, vinyl groups, which could be readily utilized post-synthetic modifications. This facile enables functionalization any containing imine linkages.
Language: Английский
Citations
45
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(9)
Published: Jan. 9, 2024
Constructing uniform covalent organic framework (COF) film on substrates for electronic devices is highly desirable. Here, a simple and mild strategy developed to prepare them by polymerization solid-liquid interface. The universality of the method confirmed successful preparation five COF films with different microstructures. These have large lateral size, controllable thickness, high crystalline quality. And patterns can also be directly achieved via hydrophilic hydrophobic interface engineering, which in favor preparing device array. For application studies, PyTTA-TPA (PyTTA: 4,4',4'',4'''-(1,3,6,8-Tetrakis(4-aminophenyl)pyrene TPA: terephthalaldehyde) has photoresponsivity 59.79 μA W
Language: Английский
Citations
23
Materials Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 8(6), P. 1513 - 1535
Published: Jan. 1, 2024
Covalent organic frameworks (COFs) with permanent porosity, long-range order and rigid backbones offer a promising material platform for photocatalytic water splitting hydrogen production.
Language: Английский
Citations
16
Chemical Science, Journal Year: 2023, Volume and Issue: 14(6), P. 1543 - 1550
Published: Jan. 1, 2023
Irreversible locking of imine linkages into stable represents a promising strategy to improve the robustness and functionality covalent organic frameworks (COFs). We report, for first time, multi-component one-pot reaction (OPR) annulation construct highly nonsubstituted quinoline-bridged COFs (NQ-COFs), that equilibrium regulation reversible/irreversible cascade reactions by addition MgSO4 desiccant is crucial achieve high conversion efficiency crystallinity. The higher long-range order surface area NQ-COFs synthesized this OPR than those reported two-step post-synthetic modification (PSM) facilitate charge carrier transfer photogeneration ability superoxide radicals (O2˙-), which makes these more efficient photocatalysts O2˙- mediated synthesis 2-benzimidazole derivatives. general applicability synthetic demonstrated fabricating 12 other crystalline with diversity topologies functional groups.
Language: Английский
Citations
25
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(11)
Published: Jan. 20, 2024
Abstract Benzoxazole‐linked covalent organic frameworks (BO−COFs), despite their exceptional chemical stability, are still in infancy. This is primarily because the current prevalent methods require use of special ortho ‐hydroxyl‐substituted aromatic amines as monomers. Herein, we report an innovative strategy to access BO−COFs directly from imine‐linked COFs (Im−COFs) without pre‐embedded OH groups, using a two‐step sequential oxidation/cyclization process. The process included oxidation Im−COFs into amide‐linked COFs, followed by copper‐catalyzed oxidative cyclization. Five representative were synthesized with retained crystallinity and high oxidization efficiency, offering potential convert significant portion BO−COFs. structural advantages newly designed demonstrated through application photocatalytic transformations.
Language: Английский
Citations
15