Regulating the Topology of Covalent Organic Frameworks for Boosting Overall H₂O₂ Photogeneration

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(24)

Published: April 12, 2024

Photocatalytic oxygen reduction reactions and water oxidation are extremely promising green approaches for massive H

Language: Английский

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Structurally Locked High-Crystalline Covalent Triazine Frameworks Enable Remarkable Overall Photosynthesis of Hydrogen Peroxide

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(43), P. 29943 - 29954

Published: Oct. 17, 2024

The development of green and efficient hydrogen peroxide (H

Language: Английский

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Robust Covalent Organic Frameworks for Photosynthesis of H₂O₂: Advancements, Challenges and Strategies

Small, Journal Year: 2024, Volume and Issue: 20(44)

Published: July 6, 2024

Abstract Since 2020, covalent organic frameworks (COFs) are emerging as robust catalysts for the photosynthesis of hydrogen peroxide (H 2 O ), benefiting from their distinct advantages. However, current efficiency H production and solar‐to‐chemical energy conversion (SCC) remain suboptimal due to various constraints in reaction mechanism. Therefore, there is an imperative propose improvement strategies accelerate development this system. This comprehensive review delineates recent advances, challenges, utilizing COFs photocatalytic production. It explores fundamentals challenges (e.g., oxygen (O ) mass transfer rate, adsorption capacity, response sunlight, electron‐hole separation efficiency, charge selectivity, desorption) associated with process, well advantages, applications, classification, preparation purpose. Various enhance performance highlighted. The aims stimulate further advancements discusses potential prospects, application areas field.

Language: Английский

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One‐Pot Synthesis of Fully Conjugated Covalent Organic Frameworks via the Pictet–Spengler Reaction for Boosting H₂O₂ Photogeneration in Real Seawater

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

Published: Jan. 24, 2025

Abstract Photosynthesizing H 2 O from real seawater is a promising and green avenue but suffers salt‐deactivated effects with limitations on stability photocatalytic activity. Herein, by the Pictet–Spengler reaction, two fully conjugated thieno[3,2‐c]pyridine‐linked covalent organic frameworks (named TBA‐COF TCA‐COF) are synthesized for photoproduction first time. Without sacrificial agents in , TCA‐COF exhibit impressive generation rates of 8878 6023 µmol g −1 h solar‐to‐chemical conversion efficiency 0.62% 0.42%, respectively, superior to their Schiff base analogs. Further experimental theoretical investigations reveal that, compared imine‐linkage counterparts, one‐pot cyclized TCA‐COF, reaction improves charge carrier separation efficiency, alters photoreduction center triazine benzene parts pyridine units, modulates energy band structures drive 2e − oxygen reduction water oxidation thereby enhances photosynthetic Notably, seawater‐produced flow reactors packed can be directly utilized E. coli sterilization. The present study highlights construction robust COFs thieno[3,2‐c]pyridine linkage via sustainable producing seawater.

Language: Английский

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Reticular Ratchets for Directing Electrochemiluminescence

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(24), P. 16681 - 16688

Published: June 5, 2024

Electrochemiluminescence (ECL) involves charge transfer between electrochemical redox intermediates to produce an excited state for light emission. Ensuring precise control of is essential decoding ECL fundamentals, yet guidelines on how achieve this conventional emitters remain unexplored. Molecular ratchets offer a potential solution, as they enable the directional energy or chemicals while impeding reverse movement. Herein, we designed 10 pairs imine-based covalent organic frameworks reticular delicately manipulate intrareticular directing transduction from electric and chemical energies. Aligning donor acceptor (D–A) directions with imine dipole effectively facilitates migration, whereas reversing D–A direction impedes it. Notably, ratchet effect directionality intensified increasing contrast, resulting in remarkable 680-fold improvement efficiency. Furthermore, dipole-controlled exciton binding energy, electron/hole decay kinetics, femtosecond transient absorption spectra identified electron tendency N-end toward C-end during transduction. An exponential correlation efficiency difference was discovered. Our work provides general approach design next-generation devices.

Language: Английский

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Tandem Fields Facilitating Directional Carrier Migration in Van der Waals Heterojunction for Efficient Overall Piezo‐synthesis of H₂O₂

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(32)

Published: May 29, 2024

Piezo-synthesis of H

Language: Английский

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Bi₄O₅Br₂/COF S-Scheme Heterojunctions for Boosting H₂O₂ Photoproduction under Air and Pure Water

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(9), P. 3932 - 3940

Published: July 26, 2024

Photosynthesizing H2O2 by the oxygen reduction reaction (ORR) and water oxidation (WOR) is a promising green avenue for generation but limited charge carrier recombination rate sluggish kinetics. Herein, Bi4O5Br2/COF step-scheme (S-scheme) heterojunction (named BIT) created first time covalent organic frameworks (TTD-COF) Bi4O5Br2, with an increased separation efficiency photosynthetic activity. Under air pure water, BIT6 exhibits highest production of 5221 μmol g–1 h–1, which 20 1.7 times greater than that individual Bi4O5Br2 TTD-COF. Subsequent mechanism analysis reveals photosynthesizes through overpowering indirect 2e– ORR paths (O2–O2• ––H2O2 O2–O2• ––O21–H2O2) weak direct WOR pathways. Moreover, in situ photogeneration process can be accompanied degradation antibiotics. This study offers in-depth insights into COF-based S-scheme heterojunctions enhanced photoproduction.

Language: Английский

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Photocatalytic hydrogen peroxide production: Advances, mechanistic insights, and emerging challenges

Journal of environmental chemical engineering, Journal Year: 2024, Volume and Issue: 12(5), P. 114143 - 114143

Published: Sept. 16, 2024

Language: Английский

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S‐Scheme Heterojunction Fabricated from Covalent Organic Framework and Quantum Dot for Enhanced Photosynthesis of Hydrogen Peroxide from Water and Air

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

Published: Sept. 16, 2024

Abstract Covalent organic frameworks (COFs) with stable crystalline porous structures and flexible assembly properties contribute to the direct photocatalytic synthesis of H 2 O meet growing global demand. To address challenges insufficient redox capacity photogenerated carrier recombination COFs, S‐scheme heterojunction is constructed from COFs quantum dots (QDs) improve production . Herein, 0D ZnCdS QDs (ZCS) uniformly anchor on surface a 2D conjugated tetrathiafulvalene‐based COF (TT‐COF), affording TT‐COF/ZCS. Formation effectively prevents agglomeration ZCS, modulates energy band structure TT‐COF, enhances migration carriers ability. As total consequence, optimized (TZ‐40) able afford in yield up 5171 µmol g −1 h under visible light irradiation , much higher than those for 2520 2647 The present result demonstrates great potential COFs/QDs‐based heterojunctions applications including production.

Language: Английский

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Enhancing photocatalytic H2O2 production of donor−acceptor polymers by modulation of polymerization modes

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124856 - 124856

Published: Nov. 1, 2024

Language: Английский

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