Covalent triazine frameworks for advanced energy storage: challenges and new opportunities

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(8), P. 3181 - 3213

Published: Jan. 1, 2023

This Review provides a comprehensive overview of recent advancements in CTF materials and CTF-based batteries. The aims to make batteries viable for next-generation high-energy battery systems.

Language: Английский

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Construction of Thiadiazole-Bridged sp²-Carbon-Conjugated Covalent Organic Frameworks with Diminished Excitation Binding Energy Toward Superior Photocatalysis

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(2), P. 1318 - 1325

Published: Jan. 5, 2024

Sp2-carbon-conjugated covalent organic frameworks (sp2c-COFs) have emerged as promising platforms for phototo–chemical energy conversion due to their tailorable optoelectronic properties, in-plane π-conjugations, and robust structures. However, the development of sp2c-COFs in photocatalysis is still highly hindered by limited linkage chemistry. Herein, we report a novel thiadiazole-bridged sp2c-COF (sp2c-COF-ST) synthesized thiadiazole-mediated aldol-type polycondensation. The resultant sp2c-COF-ST demonstrates high chemical stability under strong acids bases (12 M HCl or 12 NaOH). electro-deficient thiadiazole together with fully conjugated planar skeleton endows superior photoelectrochemical performance charge-carrier separation migration ability. As result, when employed photocathode, exhibits significant photocurrent up ∼14.5 μA cm–2 at 0.3 V vs reversible hydrogen electrode (RHE) visible-light irradiation (>420 nm), which much higher than those analogous COFs partial imine linkages (mix-COF-SNT ∼ 9.5 cm–2) full (imi-COF-SNNT 4.9 cm–2), emphasizing importance structure–property relationships. Further temperature-dependent photoluminescence spectra density functional theory calculations demonstrate that has smaller exciton binding well effective mass comparison mix-COF-SNT imi-COF-SNNT, suggests sp2c-conjugated enhances dissociation carrier light irradiation. This work highlights design preparation photocatalytic performance.

Language: Английский

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Charging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 29, 2024

Abstract Covalent organic frameworks (COFs) are ideal templates for constructing metal-free catalysts the oxygen reduction reaction due to their highly tuneable skeletons and controllable porous channels. However, development of active sites within COFs remains challenging limited electron-transfer capabilities weak binding affinities intermediates. Herein, we constructed catalytic centres by modulating electronic states pyridine nitrogen atoms incorporated into COFs. By incorporating different units (such as pyridine, ionic imidazole units), tuned various properties including dipole moments, reductive ability, hydrophilicity, towards Notably, COF ( im -PY-BPY-COF) exhibited greater activity than neutral (PY-BPY-COF) ion -PY-BPY-COF). Specifically, -PY-BPY-COF demonstrated a half-wave potential 0.80 V in 0.1 M KOH, outperforming other Theoretical calculations situ synchrotron radiation Fourier transform infrared spectroscopy confirmed that carbon rings improved facilitating intermediate OOH* promoting desorption OH*. This study provides new insights design metal-like catalysts.

Language: Английский

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Molecular Engineering for Modulating Photocatalytic Hydrogen Evolution of Fully Conjugated 3D Covalent Organic Frameworks

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(25)

Published: April 16, 2024

Covalent organic frameworks (COFs) have recently shown great potential for photocatalytic hydrogen production. Currently almost all reports are focused on two-dimensional (2D) COFs, while the 3D counterparts rarely explored due to their non-conjugated derived from sp

Language: Английский

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Covalent Organic Frameworks: Linkage Chemistry and Its Critical Role in The Evolution of π Electronic Structures and Functions

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(22)

Published: March 19, 2024

Covalent organic frameworks (COFs) provide a molecular platform for designing novel class of functional materials with well-defined structures. A crucial structural parameter is the linkage, which dictates how knot and linker units are connected to form two-dimensional polymers layer frameworks, shaping ordered π-array porous architectures. However, roles linkage in development π electronic structures functions remain fundamental yet unresolved issues. Here we report designed synthesis COFs featuring four representative linkages: hydrazone, imine, azine, C=C bonds, elucidate their impacts on evolution functions. Our observations revealed that hydrazone provides non-conjugated connection, while imine azine allow partial conjugation, bond permits full π-conjugation. Importantly, profoundly influences control functions, unraveling its pivotal role determining key properties such as band gap, frontier energy levels, light absorption, luminescence, carrier density mobility, magnetic permeability. These findings highlight significance chemistry offer general transformative guidance framework achieve

Language: Английский

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Emerging MOFs, COFs, and their derivatives for energy and environmental applications

The Innovation, Journal Year: 2025, Volume and Issue: 6(2), P. 100778 - 100778

Published: Jan. 18, 2025

Traditional fossil fuels significantly contribute to energy supply, economic development, and advancements in science technology. However, prolonged extensive use of has resulted increasingly severe environmental pollution. Consequently, it is imperative develop new, clean, pollution-free sources with high density versatility as substitutes for conventional fuels, although this remains a considerable challenge. Simultaneously, addressing water pollution critical concern. The design, optimization functional nanomaterials are pivotal advancing new solutions pollutant remediation. Emerging porous framework materials such metal-organic frameworks (MOFs) covalent organic (COFs), recognized exemplary crystalline materials, exhibit potential applications due their specific surface area, adjustable pore sizes structures, permanent porosity, customizable functionalities. This work provides comprehensive systematic review the MOFs, COFs, derivatives emerging technologies, including oxygen reduction reaction, evolution hydrogen lithium-ion batteries, remediation carbon dioxide reaction management. In addition, strategies performance adjustment structure-effect relationships these explored. Interaction mechanisms summarized based on experimental discussions, theoretical calculations, advanced spectroscopy analyses. challenges, future prospects, opportunities tailoring presented.

Language: Английский

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Application of metal-organic framework materials in supercapacitors

Journal of Energy Storage, Journal Year: 2025, Volume and Issue: 113, P. 115535 - 115535

Published: Feb. 8, 2025

Language: Английский

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Carborane-Based Three-Dimensional Covalent Organic Frameworks

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(44), P. 24202 - 24209

Published: Oct. 27, 2023

The predesignable porous structure and high structural flexibility of covalent organic frameworks (COFs) render this material desirable as a platform for addressing various cutting-edge issues. Precise control over their composition, topological structure, porosity, stability to realize tailor-made functionality still remains great challenge. In work, we developed new kind three-dimensional (3D) carborane-based COF with 7-fold interpenetrating dia diagram. resulting COFs exhibited crystallinity, exceptional strong robustness. slightly lower electronegativity boron (2.04) than that hydrogen (2.20) can lead the polarization B-H bond into Bδ+-Hδ- mode, which renders these high-performance materials adsorption separation hexane isomers through B-Hδ-···Hδ+-C interaction. Significantly, carborane content obtained reached up 54.2 wt %, gets highest rank among all reported materials. Combining surface area, robustness, carborane, work efficient adsorbents five factors. This not only enhances diversity 3D functional but also constitutes further step toward alkane isomers.

Language: Английский

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Self-derivation and reconstruction of silver nanoparticle reinforced cobalt-nickel bimetallic hydroxides through interface engineering for overall water splitting

Journal of Energy Chemistry, Journal Year: 2023, Volume and Issue: 90, P. 590 - 599

Published: Dec. 14, 2023

Language: Английский

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A fully π-conjugated covalent organic framework with dual binding sites for ultrasensitive detection and removal of divalent heavy metal ions

Journal of Hazardous Materials, Journal Year: 2023, Volume and Issue: 459, P. 132081 - 132081

Published: July 17, 2023

Language: Английский

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