Impact of imine bond orientations on photocatalytic hydrogen generation of benzothiadiazole-based covalent organic frameworks constructed using “two-in-one” monomers DOI
Zeyang Wang, Jiaxin Guo, Shuai Sun

et al.

Journal of Materials Chemistry C, Journal Year: 2024, Volume and Issue: 12(32), P. 12249 - 12253

Published: Jan. 1, 2024

Two benzothiadiazole-based COFs, constructed using “two-in-one” monomers, exhibit significantly different photocatalytic hydrogen generation performances due to their distinct imine bond orientations.

Language: Английский

Thermally triggered topological polymerization in diacetylene-functionalized covalent organic framework toward enhanced memristive properties DOI
Pan‐Ke Zhou, Yuxing Huang, Ziyue Yu

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 3, 2025

Language: Английский

Citations

1
Pyridyl‐Imine‐Functionalized Donor–Acceptor Covalent Organic Frameworks for Optimal Photosynthesis of Hydrogen Peroxide DOI Open Access
Zixuan Li,

Bingzi Cai,

Ying Zou

et al.

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 3, 2025

Abstract The artificial photosynthesis of hydrogen peroxide (H 2 O ) using semiconductor photocatalysts is gaining attention as an eco‐friendly and energy‐efficient method. Covalent organic frameworks (COFs) show great promise in enhancing photocatalytic H production due to their tunable structures functional diversity. However, the efficiency generation close photoelectric properties COFs microenvironment active sites. Herein, synthesis pyridyl‐imine‐functionalized (PyIm‐COFs) featuring donor–acceptor (D–A) moieties improve reported. By employing benzothiadiazole (BT) units with varied fluorine substitutions, electronic environment sites, optimizing selective two‐electron (2e − oxygen reduction reaction (ORR), tuned. Among synthesized COFs, PyIm‐BT_F exhibits highest activity, achieving a rate 5342 µmol g −1 h . importance D–A rational design COF‐based photocatalysts, providing novel strategy for sustainable through optimized site environments, underscored.

Language: Английский

Citations

1
Enhanced Photocatalytic Production of Hydrogen Peroxide by Covalent Triazine Frameworks with Stepwise Electron Transfer DOI
Hao Zhang, Wenxin Wei, Kai Chi

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 17654 - 17663

Published: Nov. 15, 2024

The photosynthesis of hydrogen peroxide (H2O2) from pure water and oxygen using metal-free photocatalysts offers a renewable approach to convert solar energy storable chemical energy. However, the efficiency H2O2 is often hindered by rapid recombination photogenerated charge carriers. Herein, we present an elegantly designed covalent triazine framework (CTF) photocatalyst, denoted as Ace-asy-CTF, with stepwise electron transfer pathway for highly efficient H2O2. Notably, Ace-asy-CTF possesses localized excited-state distribution that created weakly conjugated acetenyl units in asymmetric frameworks, revealed transient spectroscopies further supported theoretical calculations. Meanwhile, introduced also serve active sites reduction reaction (ORR). simultaneously enhanced two-step 2e– ORR result excellent yield 2594 μmol g–1 h–1, directly produced without requiring any sacrificial reagents. This work paves way development next-generation catalysts, providing feasible benchmark stable

Language: Английский

Citations

8
Impact of Imine Bond Orientations and Acceptor Groups on Photocatalytic Hydrogen Generation of Donor–Acceptor Covalent Organic Frameworks DOI

Chao‐Qin Han,

Jiaxin Guo, Shuai Sun

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 9, 2024

Abstract Covalent organic frameworks (COFs) have emerged as one of the most studied photocatalysts owing to their adjustable structure and bandgaps. However, there is limited research on regulating light‐harvesting capabilities acceptor building blocks in donor–acceptor (D–A) isomer COFs with different bond orientations. This investigation crucial for elucidating structure‐property‐performance relationship COF photocatalysts. Herein, a series D–A isostructural are synthesized imine orientations using benzothiadiazole its derivatives‐based units. Extended light absorption achieved groups that strong electron‐withdrawing capacities, although this resulted decreased hydrogen generation efficiency. Photocatalytic experiments indicated dialdehyde benzothiadiazole‐based COFs, HIAM‐0015, exhibit highest rate (17.99 mmol g −1 h ), which 15 times higher than isomer. The excellent photocatalytic performance HIAM‐0015 can be attributed fast charge separation migration. work provides insights into rational design synthesis achieve efficient activity.

Language: Английский

Citations

5
The Effect of Pore Functionality in Multicomponent Covalent Organic Frameworks on Stable Long‐Term Photocatalytic H2 Production DOI Creative Commons
Prasenjit Das,

Gouri Chakraborty,

Jin Yang

et al.

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: May 2, 2025

Abstract In nature, organic molecules play a vital role in light harvesting and photosynthesis. However, regarding artificial water splitting, the research focus is primarily on inorganic semiconductors. Although photocatalysts have high structural variability, they tend to exhibit lower quantum efficiencies for splitting than their counterparts. Multicomponent reactions (MCRs) offer an attractive route introduce different functional units into covalent frameworks (COFs) enable semiconducting properties chemical stability, creating promising materials long‐term photocatalytic applications, such as H 2 production. Herein, five highly crystalline donor‐acceptor based, 4‐substituted quinoline‐linked MCR‐COFs are presented that prepared via three‐component Povarov reaction. The pore functionality varied by applying vinyl derivatives (e.g., styrene, 2‐vinyl pyridine, 4‐vinylpyridine, 4‐vinyl imidazole, 2,3,4,5,6‐pentafluorostyrene), which has strong influence obtained activity. Especially imidazole‐functionalized COF displays performance due its surface area, crystallinity, wettability. These it maintain activity even membrane support. Furthermore, display dramatically enhanced (photo)chemical stability after solar irradiation steady evolution at least 15 days.

Language: Английский

Citations

0
Strategic engineering of strong electron coupling between the ohmic junction of nanoflower-like MoWS2 and CdS for boosting photocatalytic hydrogen evolution DOI

Lu Ding,

Minjun Lei, Xiaoli Ma

et al.

Journal of Power Sources, Journal Year: 2025, Volume and Issue: 645, P. 237220 - 237220

Published: May 3, 2025

Language: Английский

Citations

0
Efficient photoresponsive one-dimensional covalent organic framework as oxidase-like enzyme for ultrasensitive detection of antioxidants DOI

Wenping Yao,

Liyi Yao,

Ze-En Wang

et al.

Talanta, Journal Year: 2025, Volume and Issue: 286, P. 127519 - 127519

Published: Jan. 4, 2025

Language: Английский

Citations

0
Construction of Covalent Triazine Framework With D‐A1‐A2 Configuration via Post‐Modification for Photocatalytic Hydrogen Evolution DOI Open Access
Yong Yang,

He Wei,

Dengmeng Song

et al.

Applied Organometallic Chemistry, Journal Year: 2025, Volume and Issue: 39(2)

Published: Jan. 9, 2025

ABSTRACT A D‐A 1 ‐A 2 type covalent triazine framework (CTF) was prepared for the photocatalytic hydrogen evolution (HER). In resulting CTF‐CZ‐Bpy 2+ , 9‐ethyl‐9 H ‐carbazole (CZ) group is used as donor, ring first acceptor, and cyclic diquat (Bpy ) moiety second acceptor. Both experimental theoretical results show that structure significantly enhances efficiency of photogenerated charge separation transfer. As a result, demonstrated outstanding HER activity with yield rate 31.1 mmol g −1 h which 7.8 times higher than nonfunctionalized CTF‐CZ‐Bpy.

Language: Английский

Citations

0
N-Position Isomerization to Enhance the Co2 Photoreduction Performance of Bipyridine-Based Covalent Organic Frameworks DOI
Yiming Li, Mingming Chu, Wenjing Sun

et al.

Published: Jan. 1, 2025

Language: Английский

Citations

0
Amidoxime‐Functionalized sp2‐Carbon‐Conjugated Covalent Organic Frameworks for Overall Photocatalytic Hydrogen Peroxide Production DOI Creative Commons

Zhiwu Yu,

Fengtao Yu,

Mei Xu

et al.

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 18, 2025

Abstract Cyano‐functionalized sp 2 ‐carbon‐conjugated covalent organic frameworks (CN‐COFs) have been considered as promising candidates for artificial photosynthesis of hydrogen peroxide (H O ). Nevertheless, the performance CN‐COFs is inherently limited by constrained oxygen capture capacity, insufficient charge separation, and rapid carrier recombination. Herein, study rationally reports a strategy integrating amidoxime groups (AO) into COF through one‐step cyano hydrolysis process to increase photocatalytic H production. Combined simulations characterizations reveal that introducing AO enhances hydrophilicity, stabilizes adsorbed Oxygen (O ) via bonding, accelerates separation transfer, well lowers energy barrier reduction reaction pathway, thus achieving an unmatched production rate 6024 µmol h −1 g . Importantly, solar‐to‐chemical conversion (SCC) efficiency PTTN‐AO reaches 0.61%, significantly surpassing natural plants (≈0.1%) most COF‐based photocatalysts. The current findings are encouraging molecular design polymers green efficient

Language: Английский

Citations

0