Variation of Chemical Microenvironment of Pores in Hydrazone‐Linked Covalent Organic Frameworks for Photosynthesis of H2O2 DOI

Zhipeng Xie,

Xiong Chen, Wenbin Wang

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(39)

Published: July 2, 2024

Abstract Photocatalytic synthesis of H 2 O is an advantageous and ecologically sustainable alternative to the conventional anthraquinone process. However, achieving high conversion efficiency without sacrificial agents remains a challenge. In this study, two covalent organic frameworks (COF−O COF−C) were prepared with identical skeletal structures but their pore walls anchored different alkyl chains. They used investigate effect chemical microenvironment pores on photocatalytic production. Experimental results reveal change hydrophilicity in COF−O, leading suppressed charge recombination, diminished transfer resistance, accelerated interfacial electron transfer. An apparent quantum yield as 10.3 % (λ=420 nm) can be achieved through oxygen reduction reaction. This among highest ever reported for polymer photocatalysts. study may provide novel avenue optimizing activity selectivity generation.

Language: Английский

Solar‐to‐H2O2 Catalyzed by Covalent Organic Frameworks DOI Creative Commons
Zi‐Jun Yong, Tianyi Ma

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(49)

Published: Aug. 14, 2023

Abstract Benefiting from the excellent structural tunability, robust framework, ultrahigh porosity, and rich active sites, covalent organic frameworks (COFs) are widely recognized as promising photocatalysts in chemical conversions, emerged hydrogen peroxide (H 2 O ) photosynthesis 2020. H , serving an environmental‐friendly oxidant a liquid fuel, has attracted increasing researchers to explore its potential. Over past few years, numerous COFs‐based developed with encouraging achievements production, whereas no comprehensive review articles exist summarize this specific significant area. Herein we provide systematic overview of advances challenges COFs photocatalytic production. We first introduce priorities photosynthesis. Then, various strategies improve efficiency discussed. The perspective outlook for future emerging field finally offered. This timely will pave way development highly efficient practical production value‐added chemicals not limited .

Language: Английский

Citations

167

Reticular framework materials for photocatalytic organic reactions DOI
Ning‐Yu Huang,

Yu‐Tao Zheng,

Di Chen

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(22), P. 7949 - 8004

Published: Jan. 1, 2023

Photocatalytic organic reactions, harvesting solar energy to produce high value-added chemicals, have attracted increasing attention as a sustainable approach address the global crisis and environmental issues. Reticular framework materials, including metal-organic frameworks (MOFs) covalent (COFs), are widely considered promising candidates for photocatalysis owing their crystallinity, tailorable pore environment extensive structural diversity. Although design synthesis of MOFs COFs been intensively developed in last 20 years, applications photocatalytic transformations still preliminary stage, making systematic summary necessary. Thus, this review aims provide comprehensive understanding useful guidelines exploration suitable MOF COF photocatalysts towards appropriate reactions. The commonly used reactions categorized facilitate identification reaction types. From practical viewpoint, fundamentals experimental design, active species, performance evaluation external conditions, discussed detail easy experimentation. Furthermore, latest advances COFs, composites, comprehensively summarized according actual sites, together with discussion structure-property relationship. We believe that study will be helpful researchers novel reticular various synthetic applications.

Language: Английский

Citations

104

Molecular‐Level Regulation Strategies Toward Efficient Charge Separation in Donor−Acceptor Type Conjugated Polymers for Boosted Energy‐Related Photocatalysis DOI
Lu Wang,

Linghao Liu,

Yan Li

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 14(5)

Published: Dec. 11, 2023

Abstract The development of efficient photocatalysts for artificial photocatalytic energy conversion is an intriguing strategy. Promisingly, conjugated polymers (CPs) have been actively investigated as alternatives to traditional inorganic semiconductors photocatalysis due their molecularly tunable optoelectronic properties, thus providing a great platform molecular design. Incorporating donor (D) and acceptor (A) units into the backbone CPs ensures adequate D−A interface, which essential facilitating charge separation. This approach also allows bandgaps leading significant progress in conversions recent years. Here, fundamentals D–A type are initially outlined, followed by advanced experimental methods density functional theory (DFT) calculations investigating carrier dynamics. Then, detailed exposition synthetic strategies carried out. Their extensive applications diverse energy‐related conversions, such hydrogen evolution, oxygen overall water splitting, CO 2 reduction, N H O evolution comprehensively presented. review provides new comprehensive insights molecular‐level design catalysts boosted conversion, expected further advance photocatalysis.

Language: Английский

Citations

48

Electric effects reinforce charge carrier behaviour for photocatalysis DOI

Aoqiang Shu,

Chencheng Qin,

Miao Li

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(14), P. 4907 - 4928

Published: Jan. 1, 2024

Recent studies on enhancing charge carrier behavior through electric effects for efficient photocatalysis are summarized, evaluating the in-depth function of these effects. This provides unique perspectives to optimize photocatalytic processes.

Language: Английский

Citations

26

Dual–Acceptor Engineering in Pyrene‐Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution DOI

Nengyi Liu,

Shuailei Xie, Yuxing Huang

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(40)

Published: July 18, 2024

Abstract The integration of electron donor (D) and acceptor (A) units into covalent organic frameworks (COFs) has received increasing interest due to its potential for efficient photocatalytic hydrogen (H 2 ) evolution from water. Nevertheless, the advancement D–A COFs is still constrained by limited investigations on engineering, which enables highly effective charge transfer pathways in deliver photoexcited electrons a preferential orientation enhance performance. Herein, two systems with D–A–A configurations based molecular engineering strategy are proposed construct three distinct COFs. Specifically, TAPPy‐DBTDP‐COF merging one pyrene‐based benzothiadiazole acceptors realized an average H rate 12.7 mmol h −1 g under visible light, among highest ever reported typical D–A‐type COF systems. combination experimental theoretical analysis signifies crucial role dual‐acceptor arrangement promoting exciton dissociation carrier migration. These findings underscore significant structural design, conducive separation holes resulting superior activities.

Language: Английский

Citations

25

Variation of Chemical Microenvironment of Pores in Hydrazone‐Linked Covalent Organic Frameworks for Photosynthesis of H2O2 DOI

Zhipeng Xie,

Xiong Chen, Wenbin Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 20, 2024

Photocatalytic synthesis of H

Language: Английский

Citations

19

Unveiling the exciton dissociation dynamics steered by built-in electric fields in conjugated microporous polymers for photoreduction of uranium (VI) from seawater DOI
Weijie Zhang, Bingxin Wang,

Haishuai Cui

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 662, P. 377 - 390

Published: Feb. 9, 2024

Language: Английский

Citations

18

Π‐Bridge Modulations in D–π–A Conjugated Microporous Polymers to Facilitate Charge Separation and Transfer Kinetics for Efficient Photocatalysis DOI
Chunlei Li,

Hetao Xu,

Hao Xiong

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(44)

Published: May 16, 2024

Abstract The burgeoning field of conjugated microporous polymers (CMPs) has generated widespread interest due to their potential as photocatalysts for hydrogen production from water. Nevertheless, photocatalytic performance is sometimes hindered by inadequate charge separation and transfer, coupled with rapid recombination. Herein, a strategy enhance via the customization π ‐bridges through modulation heteroatoms in series donor‐ ‐acceptor (D‐ ‐A) CMPs proposed. This affords optimized energy levels improved thus boosting efficiency. Among various heteroatom substitutions, S‐doped CMP (10 mg) demonstrates highest evolution rate 203 µmol h −1 (AQY 450nm = 7.4%) under visible light irradiation. Subsequent experimental analysis reveals its superior can be largely related minimized exciton binding energy, facilitated transfer efficiency, impeded recombination among these heteroatom‐doped D‐ ‐A CMPs. research paves way rational design modification organic semiconductors advanced solar‐driven photocatalysis promoting transfer.

Language: Английский

Citations

14

Insights into Substituent Effects on the Fundamental Photocatalytic Processes of Covalent Organic Frameworks toward H2 Evolution and H2O2 Production Reactions DOI
Yingying Gu, Junxia Wang, Qingqing Tang

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(15), P. 11262 - 11272

Published: July 13, 2024

Language: Английский

Citations

10

Two-dimensional porphyrin-based covalent organic frameworks for heterogeneous photocatalysis: Influence of pore size on photocatalytic performance DOI

Houchao Shan,

Ziyi Zhang, Yunfei Jiang

et al.

Separation and Purification Technology, Journal Year: 2025, Volume and Issue: unknown, P. 132102 - 132102

Published: Feb. 1, 2025

Language: Английский

Citations

1