Multicomponent Synthesis of Imidazole‐Linked Fully Conjugated 3D Covalent Organic Framework for Efficient Electrochemical Hydrogen Peroxide Production DOI
Yuting Zhang, Zelong Qiao, Rui Zhang

et al.

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

Published: Oct. 26, 2023

The semiconducting properties and applications of three dimensional (3D) covalent organic frameworks (COFs) are greatly hampered because their long-ranged non-conjugated skeletons relatively unstable linkages. Here, a robust imidazole-linked fully conjugated 3D framework (BUCT-COF-7) is synthesized through the one-pot multicomponent Debus-Radziszewski reaction saddle-shaped aldehyde-substituted cyclooctatetrathiophene, pyrene-4,5,9,10-tetraone, ammonium acetate. BUCT-COF-7, as metal-free catalyst, shows excellent two electron oxygen reduction (ORR) activity in alkaline medium with high hydrogen peroxide (H2 O2 ) selectivity 83.4 %. When BUCT-COF-7 cathode catalyst assembled into electrolyzer, devices showed electrochemical production rate H2 up to 326.9 mmol g-1 h-1 . accumulative amount could totally degrade dye methylene blue via Fenton for wastewater treatment. This first report about intrinsic COFs efficient synthesis , revealing promising environment-related field.

Language: Английский

Covalent Organic Framework Based Lithium–Sulfur Batteries: Materials, Interfaces, and Solid‐State Electrolytes DOI

Ben Hu,

Jie Xu, Zengjie Fan

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(10)

Published: Jan. 20, 2023

Abstract Lithium–sulfur batteries are recognized as one of the most promising next‐generation energy‐storage technologies owing to their high energy density and low cost. Nevertheless, shuttle effect polysulfide intermediates formation lithium dendrites principal reasons that restrict practical adoption current Li–S batteries. Adjustable frameworks, structural variety, functional adaptability covalent organic frameworks (COFs) have potential overcome issues associated with battery technology. Herein, a summary is presented emerging COF materials in addressing challenging problems terms sulfur hosts, modified separators, artificial solid electrolyte interphase layers, solid‐state electrolytes. This comprehensive overview focuses on design chemistry COFs used upgrade Furthermore, existing difficulties, prospective remedies, research directions for discussed, laying groundwork future advancements this class fascinating materials.

Language: Английский

Citations

165

Aggregation behaviour of pyrene-based luminescent materials, from molecular design and optical properties to application DOI
Xing Feng, Xiaohui Wang, Carl Redshaw

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(19), P. 6715 - 6753

Published: Jan. 1, 2023

This review not only highlights the progress of emission and electronic behaviour new pyrene-based luminescence molecules in aggregated state, but also provides a perspective for understanding mechanism optoelectronic properties pyrenes.

Language: Английский

Citations

142

Post-synthetic modification of covalent organic frameworks for CO2 electroreduction DOI Creative Commons
Minghao Liu, Shuai Yang, Xiubei Yang

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 26, 2023

To achieve high-efficiency catalysts for CO2 reduction reaction, various catalytic metal centres and linker molecules have been assembled into covalent organic frameworks. The amine-linkages enhance the binding ability of molecules, ionic frameworks enable to improve electronic conductivity charge transfer along However, directly synthesis with is hardly achieved due electrostatic repulsion predicament strength linkage. Herein, we demonstrate reaction by modulating linkers linkages template framework build correlation between performance structures Through double modifications, states are well tuned, resulting in controllable activity selectivity reaction. Notably, dual-functional achieves high a maximum CO Faradaic efficiency 97.32% turnover frequencies value 9922.68 h-1, which higher than those base single-modified Moreover, theoretical calculations further reveal that attributed easier formation immediate *CO from COOH*. This study provides insights developing

Language: Английский

Citations

122

Construction of Covalent Organic Frameworks via Multicomponent Reactions DOI
Qun Guan, Lele Zhou, Yu‐Bin Dong

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(3), P. 1475 - 1496

Published: Jan. 16, 2023

Multicomponent reactions (MCRs) combine at least three reactants to afford the desired product in a highly atom-economic way and are therefore viewed as efficient one-pot combinatorial synthesis tools allowing one significantly boost molecular complexity diversity. Nowadays, MCRs no longer confined organic have found applications materials chemistry. In particular, can be used prepare covalent frameworks (COFs), which crystalline porous assembled from monomers exhibit broad range of properties applications. This synthetic approach retains advantages small-molecule MCRs, not only strengthening skeletal robustness COFs, but also providing additional driving forces for their crystallization, has been series robust COFs with diverse The present perspective article provides general background discusses types employed COF date, addresses related critical challenges future perspectives inspire MCR-based design new promote further progress this emerging field.

Language: Английский

Citations

110

Highly Connected Three-Dimensional Covalent Organic Framework with Flu Topology for High-Performance Li-S Batteries DOI
Wenbo Liu, Kang Wang,

Xiaoning Zhan

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(14), P. 8141 - 8149

Published: March 29, 2023

Lithium-sulfur batteries (LSBs) have been considered as a promising candidate for next-generation energy storage devices, which however still suffer from the shuttle effect of intermediate lithium polysulfides (LiPSs). Covalent-organic frameworks (COFs) exhibited great potential sulfur hosts LSBs to solve such problem. Herein, pentiptycene-based D2h symmetrical octatopic polyaldehyde, 6,13-dimethoxy-2,3,9,10,18,19,24,25-octa(4'-formylphenyl)pentiptycene (DMOPTP), was prepared and utilized building block toward preparing COFs. Condensation DMOPTP with 4-connected tetrakis(4-aminophenyl)methane affords an expanded [8 + 4] connected network 3D-flu-COF, flu topology. The non-interpenetrated nature topology endows 3D-flu-COF high Brunauer-Emmett-Teller surface area 2860 m2 g-1, large octahedral cavities, cross-linked tunnels in framework, enabling loading capacity (∼70 wt %), strong LiPS adsorption capability, facile ion diffusion. Remarkably, when used host LSBs, delivers 1249 mA h g-1 at 0.2 C (1.0 = 1675 g-1), outstanding rate capability (764 5.0 C), excellent stability, representing one best results among thus far reported COF-based materials being competitive state-of-the-art inorganic materials.

Language: Английский

Citations

101

Covalent Organic Frameworks as Model Materials for Fundamental and Mechanistic Understanding of Organic Battery Design Principles DOI Creative Commons
Sattwick Haldar, Andreas Schneemann, Stefan Kaskel

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(25), P. 13494 - 13513

Published: June 12, 2023

Redox-active covalent organic frameworks (COFs) have recently emerged as advanced electrodes in polymer batteries. COFs provide ideal molecular precision for understanding redox mechanisms and increasing the theoretical charge-storage capacities. Furthermore, functional groups on pore surface of highly ordered easily accessible interaction sites, which can be modeled to establish a synergy between ex situ/in situ mechanism studies computational methods, permitting creation predesigned structure–property relationships. This perspective integrates categorizes functionalities COFs, providing deeper mechanistic investigation guest ion interactions Additionally, it highlights tunable electronic structural properties that influence activation reactions this promising electrode material.

Language: Английский

Citations

77

Metal-Coordinated Covalent Organic Frameworks as Advanced Bifunctional Hosts for Both Sulfur Cathodes and Lithium Anodes in Lithium–Sulfur Batteries DOI
Sen Lv, Xingkai Ma, Si‐Wen Ke

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(13), P. 9385 - 9394

Published: March 21, 2024

The shuttling of polysulfides on the cathode and uncontrollable growth lithium dendrites anode have restricted practical application lithium–sulfur (Li–S) batteries. In this study, a metal-coordinated 3D covalent organic framework (COF) with homogeneous distribution nickel–bis(dithiolene) N-rich triazine centers (namely, NiS4-TAPT) was designed synthesized, which can serve as bifunctional hosts for both sulfur cathodes anodes in Li–S abundant Ni N-sites NiS4-TAPT greatly enhance adsorption conversion polysulfides. Meanwhile, presence Ni–bis(dithiolene) enables uniform Li nucleation at anode, thereby suppressing dendrites. This work demonstrated effectiveness integrating catalytic sites to optimize chemical interactions between host materials redox-active intermediates, potentially facilitating rational design COF high-performance secondary

Language: Английский

Citations

77

Covalent organic frameworks for CO2 capture: from laboratory curiosity to industry implementation DOI
He Li,

Akhil Dilipkumar,

Saifudin Abubakar

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(18), P. 6294 - 6329

Published: Jan. 1, 2023

Synergistic developments of covalent organic frameworks and engineering processes can expedite the qualitative leap for net-zero carbon emissions.

Language: Английский

Citations

72

Covalent Organic Frameworks: Their Composites and Derivatives for Rechargeable Metal-Ion Batteries DOI Creative Commons
Bowen Sun, Zixu Sun,

Yi Yang

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 18(1), P. 28 - 66

Published: Dec. 20, 2023

Covalent organic frameworks (COFs) have attracted considerable interest in the field of rechargeable batteries owing to their three-dimensional (3D) varied pore sizes, inerratic porous structures, abundant redox-active sites, and customizable structure-adjustable frameworks. In context metal-ion batteries, these materials play a vital role electrode materials, effectively addressing critical issues such as low ionic conductivity, limited specific capacity, unstable structural integrity. However, electrochemical characteristics developed COFs still fall short practical battery requirements due inherent electronic tradeoff between capacity redox potential, unfavorable micromorphology. This review provides comprehensive overview recent advancements application COFs, COF-based composites, derivatives including lithium-ion, lithium-sulfur, sodium-ion, sodium-sulfur, potassium-ion, zinc-ion, other multivalent batteries. The operational mechanisms are elucidated, along with strategies implemented enhance properties broaden range applications.

Language: Английский

Citations

72

Rechargeable Metal-Sulfur Batteries: Key Materials to Mechanisms DOI
Weiqi Yao, K. T. Liao, Tianxing Lai

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(8), P. 4935 - 5118

Published: April 10, 2024

Rechargeable metal-sulfur batteries are considered promising candidates for energy storage due to their high density along with natural abundance and low cost of raw materials. However, they could not yet be practically implemented several key challenges: (i) poor conductivity sulfur the discharge product metal sulfide, causing sluggish redox kinetics, (ii) polysulfide shuttling, (iii) parasitic side reactions between electrolyte anode. To overcome these obstacles, numerous strategies have been explored, including modifications cathode, anode, electrolyte, binder. In this review, fundamental principles challenges first discussed. Second, latest research on is presented discussed, covering material design, synthesis methods, electrochemical performances. Third, emerging advanced characterization techniques that reveal working mechanisms highlighted. Finally, possible future directions practical applications This comprehensive review aims provide experimental theoretical guidance designing understanding intricacies batteries; thus, it can illuminate pathways progressing high-energy-density battery systems.

Language: Английский

Citations

67