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
Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(15), P. 8364 - 8374
Published: March 14, 2023
Two-dimensional covalent-organic frameworks (2D COFs) have recently emerged as great prospects for their applications new photocatalytic platforms in solar-to-hydrogen conversion; nevertheless, inefficient solar energy capture and fast charge recombination hinder the improvement of hydrogen production performance. Herein, two photoactive three-component donor-π-acceptor (TCDA) materials were constructed using a multicomponent synthesis strategy by introducing electron-deficient triazine electron-rich benzotrithiophene moieties into through sp2 carbon imine linkages, respectively. Compared with two-component COFs, novel TCDA-COFs are more convenient regulating inherent photophysical properties, thereby realizing outstanding activity evolution from water. Remarkably, first carbon-linked TCDA-COF displays an impressive rate 70.8 ± 1.9 mmol g-1 h-1 excellent reusability presence 1 wt % Pt under visible-light illumination (420-780 nm). Utilizing combination diversified spectroscopy theoretical prediction, we show that full π-conjugated linkage not only effectively broadens harvesting COFs but also enhances transfer separation efficiency.
Language: Английский
Citations
247
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
195
Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 475, P. 214882 - 214882
Published: Oct. 14, 2022
Language: Английский
Citations
154
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(34)
Published: April 24, 2023
Abstract Intensifying energy crises and severe environmental issues have led to the discovery of renewable sources, sustainable conversion, storage technologies. Photocatalysis is a green technology that converts eco‐friendly solar into high‐energy chemicals. Covalent organic frameworks (COFs) are porous materials constructed by covalent bonds show promising potential for converting chemicals owing their pre‐designable structures, high crystallinity, porosity. Herein, we highlight recent progress in synthesis COF‐based photocatalysts applications water splitting, CO 2 reduction, H O production. The challenges future opportunities rational design COFs advanced discussed. This Review expected promote further development toward photocatalysis.
Language: Английский
Citations
154
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(22)
Published: April 3, 2023
Conjugated polymers (CPs) represent a promising platform for photocatalytic CO2 fixation owing to their suitable band structures that meet the requirements of reduction potential value-added fuels. However, performance CPs is rather restrained by low charge transfer efficiency. Herein, we rationally designed three with more delocalized electronic transmission channel and planar molecular structure, which are regarded evidently reduce exciton binding energy (Eb ) accelerate internal process. Besides, assembly electron-output "tentacles" cocatalysts on surface could effectively facilitate interfacial electron delivery. Accordingly, optimal P-2CN exhibits an apparent quantum yield 4.6 % at 420 nm CO. Further adjusting amounts cyano groups cocatalysts, CO selectivity be obtained in range 0-80.5 %.
Language: Английский
Citations
71
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(15)
Published: Feb. 9, 2023
Photocatalytic hydrogen (H2 ) evolution represents a promising and sustainable technology. Covalent organic frameworks (COFs)-based photocatalysts have received growing attention. A 2D fully conjugated ethylene-linked COF (BTT-BPy-COF) was fabricated with dedicated designed active site. The introduced bipyridine sites enable facile post-protonation strategy to fine-tune the actives sites, which results in largely improved charge-separation efficiency increased hydrophilicity pore channels synergically. After modulating degree of protonation, optimal BTT-BPy-PCOF exhibits remarkable H2 rate 15.8 mmol g-1 h-1 under visible light, surpasses biphenyl-based 6 times. By using different types acids, is proved be potential universal for promoting photocatalytic evolution. This would provide important guidance design highly efficient semiconductor photocatalysts.
Language: Английский
Citations
69
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
63
Small, Journal Year: 2023, Volume and Issue: 19(48)
Published: Aug. 4, 2023
Abstract Covalent organic frameworks (COFs) are one type of porous materials linked by covalent bonds. COFs exhibit many outstanding characteristics such as high porosity, chemical and thermal stability, large specific surface area, efficient electron transfer efficiency, the ability for predesigned structures. These exceptional advantages enable to remarkable performance in photocatalysis. Additionally, activity photocatalysts can be significantly upgraded ion doping formation heterojunctions. This paper summarizes latest research progress on COF‐based applied photocatalytic systems. Initially, typical structures preparation methods analyzed compared. Moreover, essential principles reactions over COFs‐based developments hydrogen production, CO 2 reduction, pollutants elimination, transformation, overall water splitting indicated. At last, outlook challenges photocatalysis discussed. review is intended permit instructive guidance use based future.
Language: Английский
Citations
61
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown
Published: March 10, 2024
Abstract Covalent organic frameworks (COFs) attract significant attention due to their ordered, crystalline, porous, metal‐free, and predictable structures. These unique characteristics offer great opportunities for the diffusion transmission of photogenerated charges during photocatalysis. Currently, a considerable number COFs are used as metal‐free semiconductor photocatalysts. This review aims understand relationships between structure photocatalysis performance provides in‐depth insight into synthetic strategy improve performance. Subsequently, focuses on structural motif in sustainable photocatalytic hydrogen evolution, carbon dioxide reduction, peroxide generation, compound transformations. Last, conjunction with progress achieved challenges yet be overcome, candid discussion is undertaken regarding field COF photocatalysis, accompanied by presentation potential research avenues future directions. seeks provide readers comprehensive understanding pivotal role robust guidance innovative utilization
Language: Английский
Citations
61
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