Two-Dimensional Kagome Covalent Organic Frameworks with Single Atomic Co Sites for Superior Photocatalytic CO2 Reduction DOI
Yuhui Wang, Tingting Sun, Tianyu Zheng

et al.

ACS Materials Letters, Journal Year: 2023, Volume and Issue: 6(1), P. 140 - 152

Published: Dec. 7, 2023

Covalent organic frameworks (COFs) have attracted great attention as pivotal photocatalysts for efficient CO2 photoreduction into value-added fuels, which hold promise simultaneously mitigating global warming and the energy crisis. However, synthesis of COFs with a high crystalline state hierarchically porous structure to boost is still an enormous challenge rarely reported, probably because dependence upon monomers rigorous preparation conditions. Herein, series functional kagome (kg m) topologic 2D crystallinity porosity were synthesized based on condensation 4,4′,4″,4‴-(ethene-1,1,2,2-tetrayl)tetraaniline (ETTA) 2,2′-bipyridyl-5,5′-dialdehyde (Bpy-CHO) building units combined postmodification strategy, named ETTA-Bpy-COF-M (M = H, Fe, Co, Ni, or Cu). Stimulated by unique kg m topologized framework well-ordered hierarchical micropores mesopores, abundant exposed atomic Co sites, remarkable photoelectrical performance, ETTA-Bpy-COF-Co used photocatalyst catalyzing CO2-to-CO photoconversion exhibits CO yield rate (9398.14 μmol g–1 h–1), large selectivity (92.73%), good durability. Experimental theoretical analyses demonstrated that superior performance catalyzed was attributed desirable cooperative contribution topological hexagonal triangular pores well active can promote photoexcited charge carrier kinetics, enhance adsorption activation, reduce barriers *COOH generation desorption. This work opens new way COF photosynthesis reduction offers precious insights related studies in future.

Language: Английский

Dual Metallosalen‐based Covalent Organic Frameworks for Artificial Photosynthetic Diluted CO2 Reduction DOI Open Access
Hong Dong, Liang Fang, Kexin Chen

et al.

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

Published: Oct. 7, 2024

Directly converting CO

Language: Английский

Citations

10
Single-Atom Catalysts on Covalent Organic Frameworks for Energy Applications DOI
Yurong Wu, Rui Wang, Yoonseob Kim

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: unknown

Published: Feb. 8, 2024

Single-atom catalysts (SACs) have been investigated and applied to energy conversion devices. However, issues of metal agglomeration, low loading, substrate stability hindered realization the SACs' full potential. Recently, covalent organic framework (COF)-based SACs emerged as promising materials enable highly efficient catalytic reactions. Here, we summarize representative COF-based their wide application in clean devices reactions, such hydrogen evolution reaction, carbon dioxide reduction nitrogen oxygen reaction. Based on catalysis conditions, these reactions are categorized into photocatalyzed electrocatalyzed We also design strategies, including heteroatom inclusion, donor–acceptor pairs, pore engineering, interface etc. Although promising, more efforts, linkage functional groups, ionization, multifunctional sites for cocatalyzed systems, etc., could improve them be ideal SAC materials. At end, provide our perspectives where field will proceed next 5 years.

Language: Английский

Citations

9
Exploring high-connectivity three-dimensional covalent organic frameworks: topologies, structures, and emerging applications DOI
Fengqian Chen,

Haorui Zheng,

Yusran Yusran

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 25, 2024

The design principles, development process, structural analysis, applications, challenges, and future directions of high-connectivity 3D COFs.

Language: Английский

Citations

9
Heteropolyaromatic Covalent Organic Frameworks via One-Pot Multicomponent Reactions DOI Creative Commons
Prasenjit Das,

Gouri Chakraborty,

Nico Friese

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(25), P. 17131 - 17139

Published: June 14, 2024

Multicomponent reactions (MCRs) offer a platform to create different chemical structures and linkages for highly stable covalent organic frameworks (COFs). As an illustrative example, the multicomponent Povarov reaction generates 2,4-phenylquinoline from aldehydes amines in presence of electron-rich alkenes. In this study, we introduce new domino generate unprecedented 2,3-phenylquinoline COFs epoxystyrene. This work thus presents, first time, structural isomeric produced by reactions. Furthermore, 2,3-phenylquinolines can undergo Scholl form extended aromatic linkages. With approach, synthesize two thermally chemically MCR-COFs heteropolyaromatic using both situ The structure properties these are compared with corresponding 2,4-phenylquinoline-linked COF imine-COF, their activity toward benzene cyclohexane sorption separation is investigated. position pendant phenyl groups within pore plays crucial role facilitating industrially important over cyclohexane. study opens avenue construct via MCR

Language: Английский

Citations

8
Porphyrin‐Based Covalent Organic Frameworks for CO2 Photo/Electro‐Reduction DOI Open Access

Sun Tingting,

Zhi Wang, Yuhui Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 9, 2025

Photo/electro-catalytic CO2 reduction into high-value products are promising strategies for addressing both environmental problems and energy crisis. Duo to their advantageous visible light absorption ability, adjustable optic/electronic properties, definite active center, post-modification capability, excellent stability, porphyrin-based covalent organic frameworks (COFs) have emerged as attractive photo/electro-catalysts towards reduction. In this review, the research progress of COFs photo/electro-catalytic is summarized including design principles, catalytic performance, reaction mechanism. addition, review also presents some challenges prospects application in reduction, laying base fundamental efforts.

Language: Английский

Citations

1
Selective oxidation of sulfides with oxygen over a pyrene covalent organic framework photocatalyst with TEMPO DOI
Xiaoyun Dong, Fulin Zhang,

Yuexin Wang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 345, P. 123660 - 123660

Published: Dec. 25, 2023

Language: Английский

Citations

22
Site-Selective Zn-Metalation in Poly-Triphenyl Amine-based Porous Organic Polymer for Solid–Gas Phase CO2 Photoreduction DOI
Ankita Boruah, Bishal Boro, Ratul Paul

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(27), P. 34437 - 34449

Published: June 28, 2024

Harvesting solar energy to produce value-added chemicals from carbon dioxide (CO2) presents a promising route for addressing the complexities of sustainable systems and environmental issues. In this context, development metal-coordinated porous organic polymers (POPs) offers vital avenue improving photocatalytic performance motifs. The current study metal-integrated system (namely, Zn@BP-POP) developed via one-pot Friedel–Crafts (F.C.) acylation strategy, solid–gas phase photochemical CO2 reduction CO (CO2RR). postsynthetic incorporation metal (Zn) active sites on host polymeric backbone BP-POP significantly influences catalytic activity. Notably, Zn@BP-POP demonstrates good in absence any cocatalyst photosensitizer yielding while impeding competitive hydrogen evolution reaction (HER) water. experimental findings collectively propose that observed activity selectivity arise synergistic interplay between singular zinc centers light-harvesting capacity highly conjugated backbone. Further, X-ray absorption spectroscopy (XAS) analysis has highlighted prominent role played by ZnN2O4 single framework activating gaseous molecules. time-dependent density functional theory (DFT) also reveals thermodynamic feasibility CO2RR over HER under optimized conditions. This work cumulatively an effective strategy demonstrate importance metal-active effectively establish their structure-activity relationship during photocatalysis.

Language: Английский

Citations

8
Photons, Excitons, and Electrons in Covalent Organic Frameworks DOI Creative Commons
Dominic Blätte, Frank Ortmann, Thomas Bein

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(47), P. 32161 - 32205

Published: Nov. 18, 2024

Covalent organic frameworks (COFs) are created by the condensation of molecular building blocks and nodes to form two-dimensional (2D) or three-dimensional (3D) crystalline frameworks. The diversity with different properties functionalities large number possible framework topologies open a vast space well-defined porous architectures. Besides more classical applications materials such as absorption, separation, catalytic conversions, interest in optoelectronic COFs has recently increased considerably. electronic both their linkage chemistry can be controlled tune photon absorption emission, create excitons charge carriers, use these carriers photocatalysis, luminescence, chemical sensing, photovoltaics. In this Perspective, we will discuss relationship between structural features properties, starting connectivity, layer stacking 2D COFs, control over defects morphology including thin film synthesis, exploring theoretical modeling structural, electronic, dynamic discussing recent intriguing focus on photocatalysis photoelectrochemistry. We conclude some remarks about present challenges future prospects powerful architectural paradigm.

Language: Английский

Citations

8
Reticular Materials for Photocatalysis DOI
Kang Sun, Yunyang Qian, Dandan Li

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 27, 2024

Abstract Photocatalysis leverages solar energy to overcome the thermodynamic barrier, enabling efficient chemical reactions under mild conditions. It can greatly reduce reliance on traditional sources and has attracted significant research interest. Reticular materials, including metal‐organic frameworks (MOFs) covalent organic (COFs), represent a class of crystalline materials constructed from molecular building blocks linked by coordination bonds, respectively. function as heterogeneous catalysts, combining well‐defined structures high tailorability akin homogeneous catalysts. In this review, regulation light absorption, charge separation, surface in photocatalytic process through precise molecular‐level design based features reticular is elaborated. Notably, for MOFsmicroenvironment modulation around catalytic sites affects performance delved, with emphasis their unique dynamic flexible microenvironments. For COFs, inherent excitonic effects due fully nature discussed highlight strategies regulate charge‐ and/or energy‐transfer‐mediated photocatalysis. Finally, current challenges future directions field, aiming provide comprehensive understanding how be optimized enhanced photocatalysis discussed.

Language: Английский

Citations

8
Advancements and applications of three-dimensional covalent organic frameworks DOI Open Access
Rui Wang, Jie Zhao, Qianrong Fang

et al.

Chemical Synthesis, Journal Year: 2024, Volume and Issue: 4(2)

Published: May 31, 2024

Covalent organic frameworks (COFs) represent an emerging class of crystalline porous polymers characterized by their pre-designed interconnected structures formed via dynamic covalent bonds. These materials have garnered widespread attention in recent years. While applications two-dimensional (2D) COFs been extensively investigated since 2005, practicality has impeded limited specific surface area and the robust π-π stacking interaction. In contrast, three-dimensional (3D) boast enhanced porosity, larger area, well-exposed functional groups, abundance reaction sites, positioning them at forefront material research. They find extensive diverse fields, including adsorption, separation, catalysis, so on. This featured article provides a comprehensive exploration latest advancements 3D across respective application domains. Additionally, we outline current challenges that must be addressed shed light on promising prospects for utilization COFs.

Language: Английский

Citations

7