Bioinspired Tetranuclear Manganese Cubane Complex as an Efficient Molecular Electrocatalyst for Two‐electron Water Oxidation Towards Hydrogen Peroxide DOI
Tongshuai Wang, Wenxiu Li, Gang Wu

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(34)

Published: May 14, 2024

Abstract Stable homogeneous two‐electron water oxidation electrocatalysts are highly demanded to understand the precise mechanism and reaction intermediates of electrochemical H 2 O production. Here we report a tetranuclear manganese complex with cubane structure which can electrocatalyze hydrogen peroxide under alkaline neutral conditions. Such demonstrates an optimal Faradaic efficiency (FE) 87 %, is amongst ( if not ) highest FE(H reported heterogeneous electrocatalysts. In addition, active species were identified co‐catalysts excluded through ESI‐MS characterization. Furthermore, binding sites isolated one‐electron intermediate by chemical catalyst in presence substrates. It evident that efficient proton‐accepting electrolytes avoid rapid proton building‐up at electrode substantially improve rate selectivity. Accordingly, propose catalytic cycle model for bioinspired molecular electrocatalyst. The present work expected provide ideal platform elucidate WOR atomic level.

Language: Английский

Advanced Porous Aromatic Frameworks: A Comprehensive Overview of Emerging Functional Strategies and Potential Applications DOI

Hamid Ali,

Yasin Orooji, Abdullah Yahya Abdullah Alzahrani

et al.

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 18, 2025

Porous aromatic frameworks (PAFs) are a fundamental group of porous materials characterized by their distinct structural features and large surface areas. These synthesized from building units linked strong carbon–carbon bonds, which confer exceptional rigidity long-term stability. PAFs functionalities may arise directly the intrinsic chemistry or through postmodification motifs using well-defined chemical processes. Compared to other traditional such as zeolites metallic-organic frameworks, demonstrate superior stability under severe treatments due robust bonding. Even in challenging environments, ease functionalization flexibility specificity. Research on has significantly expanded accelerated over past decade, necessitating comprehensive overview key advancements this field. This review provides an in-depth analysis recent advances synthesis, functionalization, dimensionality PAFs, along with distinctive properties wide-ranging applications. explores innovative methodologies strategies for functionalizing structures, manipulation tailor specific potential Similarly, application areas, including batteries, absorption, sensors, CO2 capture, photo-/electrocatalytic usages, supercapacitors, separation, biomedical discussed detail, highlighting versatility addressing modern scientific industrial challenges.

Language: Английский

Citations

3
Charge carrier controlled free radical construction efficient photocatalytic self-Fenton system DOI
Tao Sun,

Yuhang Deng,

Guanqi Wang

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 496, P. 154351 - 154351

Published: July 27, 2024

Language: Английский

Citations

12
Strong interface coupling of H-substituted graphdiyne-based promotes photocatalytic hydrogen production DOI
Xiao Ming Qian,

Xueying Yang,

Xin Guo

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 359, P. 124502 - 124502

Published: Aug. 13, 2024

Language: Английский

Citations

8
Ethynyl‐Linked Donor–Acceptor Covalent Organic Framework for Highly Efficient Photocatalytic H2O2 Production DOI
Bowen Li, Jikun Chen, Kang Wang

et al.

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

Published: Jan. 19, 2025

Abstract Photocatalytic H 2 O synthesis from and is considered to be one of the most promising alternative approaches for manufacturing . Developing highly active selective photocatalysts significant in achieving efficient photosynthesis. Herein, an ethynyl‐linked donor–acceptor covalent organic framework (COF), named EBBT‐COF, prepared condensation reaction between electron‐deficient unit 4,4′,4″‐(1,3,5‐benzenetriyltri‐2,1‐ethynediyl)tris‐benzenamine electron‐rich benzo[1,2‐b:3,4‐b′:5,6‐b″]trithiophene‐2,5,8‐tricarboxaldehyde. Powder X‐ray diffraction N adsorption isotherm unveil crystalline porous hcb network EBBT‐COF with pores size centered at ca 2.3 nm. Spectroscopic characterizations demonstrate excellent visible‐light absorption capacity enhanced photo‐induced charge separation transport efficiency owing its architecture. Density functional theory calculations electrochemical tests indicate high activity selectivity toward 2e − reduction water oxidation triethynylbenzene trithiophene moieties accelerate ‐to‐H O‐to‐H conversion, respectively. These merits enable a photocatalyst generation yield rate 5 686 µmol g −1 h , optimal apparent quantum 15.14%, solar‐to‐chemical conversion 1.17% (λ > 400 nm), representing best performance among COF‐based reported thus far.

Language: Английский

Citations

1
Carbon nitride with grafted benzothiadiazole as electron acceptor and active site to promote exciton dissociation for metal-free photocatalytic N2 fixation DOI

Donghui Cui,

Xue Yang,

Yu Liu

et al.

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 686, P. 795 - 806

Published: Feb. 3, 2025

Language: Английский

Citations

1
Weakness-complementing Z-scheme black phosphorus/TiO2 heterojunction with efficient charge separation and photocatalytic overall water splitting activity DOI
Xiaosong Zhou,

Jyun-Bo Liang,

Limei Xu

et al.

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 689, P. 137240 - 137240

Published: March 4, 2025

Language: Английский

Citations

1
Leveraging Phenazine and Dihydrophenazine Redox Dynamics in Conjugated Microporous Polymers for High-Efficiency Overall Photosynthesis of Hydrogen Peroxide DOI Creative Commons

Shufan Feng,

Lei Wang, Limei Tian

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(30), P. 11972 - 11980

Published: Jan. 1, 2024

Leveraging the reversible phenazine–dihydrophenazine interconversion in microporous polymers enhances photocatalytic H 2 O generation by improving reduction and charge separation, showcasing a new approach for solar-driven chemical conversion.

Language: Английский

Citations

7
Construction of Porous Aromatic Frameworks with Specifically Designed Motifs for Charge Storage and Transport DOI
Yuyang Tian, Fengchao Cui, Zheng Bian

et al.

Accounts of Chemical Research, Journal Year: 2024, Volume and Issue: 57(15), P. 2130 - 2143

Published: July 24, 2024

ConspectusPorous frameworks possess high porosity and adjustable functions. The two features conjointly create sufficient interfaces for matter exchange energy transfer within the skeletons. For crystalline porous frameworks, including metal organic (MOFs) covalent (COFs), their long-range ordered structures indeed play an important role in managing versatile physicochemical behaviors such as electron or band gap engineering. It is now feasible to predict functions based on unveiled structure-performance relationships. In contrast, (POFs) represent a member of solid family with no regularity. case POFs, randomly packed building units disordered connections hinder electronic structural consistency throughout entire networks. However, many investigations have demonstrated that POFs could also be designed originated from local motifs.In this Account, we will first provide overview design synthesis principles aromatic (PAFs), which are typical exceptional stability. Specifically, achieved by specific in-framework motifs demonstrated. This strategy particularly intuitive introduce desired PAFs, owing tolerance PAFs harsh chemical treatments synthetic conditions. can either obtained selecting suitable units, sometimes aid computational screening, emerge product coupling reactions during process. Radical incorporating persistent radical molecule unit, rigid framework may facilitate formation species trapping spins network, avoid delocalizing recombining processes. Alternatively, formed linkages. reaction plays construction functional like diacetylene. highly porous, showed significant performance anodes lithium-ion batteries. To improve charge transport framework, connecting manner were cohesively considered, fully conjugated backbone was built up. another case, explicit cross-coupling ensured precise assembly donating accepting abilities; therefore, moving direction photogenerated electrons rationally controlled. Constructing designing D-A system introduced exciting properties photovoltaic photocatalysis, stable improved applications perovskite solar cells productions. These shed light designable combination intrinsic effective storage conversion.

Language: Английский

Citations

6
Synergistic Tri‐efficiency Enhancement Utilizing Functionalized Covalent Organic Frameworks for Photocatalytic H2O2 Production DOI

Yanchi Yao,

Chao Zhu,

Renlan Liu

et al.

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

Published: Sept. 23, 2024

The overall maximization of photocatalytic H

Language: Английский

Citations

6
Isomerization of Covalent Organic Frameworks for Efficiently Activating Molecular Oxygen and Promoting Hydrogen Peroxide Photosynthesis DOI

Wenjiao Wang,

Rui Zhang,

Hongqi Chu

et al.

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

Published: Sept. 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.

Language: Английский

Citations

5