Oxidation‐Reduction Molecular Junction Covalent Organic Frameworks for Full Reaction Photosynthesis of H₂O₂

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(9)

Published: Dec. 30, 2022

The full reaction photosynthesis of H2 O2 that can combine water-oxidation and oxygen-reduction without sacrificial agents is highly demanded to maximize the light-utilization overcome complex reaction-process anthraquinone-oxidation. Here, a kind oxidation-reduction molecular junction covalent-organic-framework (TTF-BT-COF) has been synthesized through covalent-coupling tetrathiafulvalene (photo-oxidation site) benzothiazole (photo-reduction site), which presents visible-light-adsorption region, effective electron-hole separation-efficiency photo-redox sites enables generation . Specifically, record-high yield (TTF-BT-COF, ≈276 000 μM h-1 g-1 ) for achieved among porous crystalline photocatalysts. This first work design COFs , might extend scope in production.

Language: Английский

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Solar‐to‐H₂O₂ Catalyzed by Covalent Organic Frameworks

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

Published: Aug. 14, 2023

Abstract Benefiting from the excellent structural tunability, robust framework, ultrahigh porosity, and rich active sites, covalent organic frameworks (COFs) are widely recognized as promising photocatalysts in chemical conversions, emerged hydrogen peroxide (H 2 O ) photosynthesis 2020. H , serving an environmental‐friendly oxidant a liquid fuel, has attracted increasing researchers to explore its potential. Over past few years, numerous COFs‐based developed with encouraging achievements production, whereas no comprehensive review articles exist summarize this specific significant area. Herein we provide systematic overview of advances challenges COFs photocatalytic production. We first introduce priorities photosynthesis. Then, various strategies improve efficiency discussed. The perspective outlook for future emerging field finally offered. This timely will pave way development highly efficient practical production value‐added chemicals not limited .

Language: Английский

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Covalent Organic Frameworks Containing Dual O₂Reduction Centers for Overall Photosynthetic Hydrogen Peroxide Production

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(9)

Published: Dec. 28, 2022

Covalent organic frameworks (COFs) are highly desirable for achieving high-efficiency overall photosynthesis of hydrogen peroxide (H2 O2 ) via molecular design. However, precise construction COFs toward photosynthetic H2 remains a great challenge. Herein, we report the crystalline s-heptazine-based (HEP-TAPT-COF and HEP-TAPB-COF) with separated redox centers efficient production from pure water. The spatially orderly active sites in HEP-COFs can efficiently promote charge separation enhance photocatalytic production. Compared HEP-TAPB-COF, HEP-TAPT-COF exhibits higher efficiency integrating dual reduction s-heptazine triazine moieties. Accordingly, bearing remarkable solar-to-chemical energy 0.65 % high apparent quantum 15.35 at 420 nm, surpassing previously reported COF-based photocatalysts.

Language: Английский

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Enhanced Mass Transfer of Oxygen through a Gas–Liquid–Solid Interface for Photocatalytic Hydrogen Peroxide Production

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(52)

Published: Sept. 24, 2021

Abstract Solar‐driven photocatalytic oxygen reduction is a potentially sustainable route for the production of hydrogen peroxide (H 2 O ). However, this approach suffers from limited solubility and slow diffusion in water. Another problem that most systems do not work well with just They often require addition sacrificial agents such as alcohols. Here, covalent organic framework (COF)‐based photocatalyst can reduce to H efficiently pure water under visible‐light irradiation reported. A solar‐to‐chemical conversion 0.76% achieved generation. More importantly, hydrophobic mesoporous properties triphenylbenzene‐dimethoxyterephthaldehyde‐COF allow formation triphase interface (gas–liquid–solid) when loading catalyst onto porous substrate. The rate reaches ≈2.9 mmol g cat −1 h at by overcoming mass‐transfer limitation Notably, 15 times higher than diphase system (liquid–solid). photoelectrochemical tests reveal increase yield closely related enhanced interfacial concentration. Furthermore, triphenylbenzene part identified reactive site based on theoretical calculations.

Language: Английский

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Carbon nitride nanotubes with in situ grafted hydroxyl groups for highly efficient spontaneous H2O2 production

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 288, P. 119993 - 119993

Published: Feb. 16, 2021

Language: Английский

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