Ethynyl‐Linked Donor–Acceptor Covalent Organic Framework for Highly Efficient Photocatalytic H₂O₂ Production

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

Abstract Photocatalytic H 2 O synthesis from and is considered to be one of the most promising alternative approaches for manufacturing . Developing highly active selective photocatalysts significant in achieving efficient photosynthesis. Herein, an ethynyl‐linked donor–acceptor covalent organic framework (COF), named EBBT‐COF, prepared condensation reaction between electron‐deficient unit 4,4′,4″‐(1,3,5‐benzenetriyltri‐2,1‐ethynediyl)tris‐benzenamine electron‐rich benzo[1,2‐b:3,4‐b′:5,6‐b″]trithiophene‐2,5,8‐tricarboxaldehyde. Powder X‐ray diffraction N adsorption isotherm unveil crystalline porous hcb network EBBT‐COF with pores size centered at ca 2.3 nm. Spectroscopic characterizations demonstrate excellent visible‐light absorption capacity enhanced photo‐induced charge separation transport efficiency owing its architecture. Density functional theory calculations electrochemical tests indicate high activity selectivity toward 2e − reduction water oxidation triethynylbenzene trithiophene moieties accelerate ‐to‐H O‐to‐H conversion, respectively. These merits enable a photocatalyst generation yield rate 5 686 µmol g −1 h , optimal apparent quantum 15.14%, solar‐to‐chemical conversion 1.17% (λ > 400 nm), representing best performance among COF‐based reported thus far.

Язык: Английский

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A Covalent Organic Framework as Photocatalyst for Smart Conversion Between Photooxidation and Photoreduction and H₂O₂ Production in Full pH Environment

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 7, 2025

Abstract Developing multifunctional photocatalysts with intelligent self‐adjusting is of great significance in the photocatalytic process. Herein, a smart covalent organic framework (Por‐HQ‐COF) phenol‐quinone conversion structure pH changes constructed for photooxidation, photoreduction, and H 2 O production. As photocatalyst, Por‐HQ‐COF can convert into Por‐BQ‐COF intelligently trigger including solution pH, vice versa. The reconstruction not only significantly alters morphologies specific surface areas COF, but also leads to an entirely change band energy charge distribution influence photoelectric properties. result, under acidic conditions, converts automatically photoreduce high concentration Cr(VI) Cr(III) efficiently. Under neutral superoxide anions (·O − ) initiate accelerate photooxidation degrade high‐concentration TC. alkaline Por‐BQ‐COF, effectively photosynthesize (1525 µmol h −1 g at λ > 420 nm) absence any sacrificial reagents, reveal strong alkalinity lower barrier hydrogen extraction from clarify active sites This work provides new strategy developing fulfill application across full environment.

Язык: Английский

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Terphenyl Functionalized Covalent Triazine Polymer as Metal‐Free Photocatalyst for Superior Hydrogen Peroxide Production

Advanced Functional Materials, Год журнала: 2024, Номер 34(32)

Опубликована: Март 25, 2024

Abstract Artificial photosynthesis of H 2 O from and by visible light is a promising approach, but the efficiency still unsatisfactory because inefficient adsorption proton supply. Here, terphenyl functionalized covalent triazine polymer (CTP‐TD) prepared for efficient production. Experimental theoretical results show that structure can promote regulating oxygen evolution (O → 1 ) improve supply accelerating water oxidation. The significantly promotes singlet ( production via intersystem crossing (ISC) process. electrophilic more easily adsorbed on catalyst surface than . Simultaneously, accumulated holes at lower oxidation energy barriers accelerate dehydrogenation This work provides valuable reference new inspiration design generation perspective reactant

Язык: Английский

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Carbazole-containing covalent triazine frameworks for efficient hydrogen peroxide photosynthesis from natural sunlight

Chemical Engineering Journal, Год журнала: 2024, Номер 490, С. 151332 - 151332

Опубликована: Апрель 16, 2024

Язык: Английский

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Covalent organic frameworks for efficient hydrogen peroxide production

EnergyChem, Год журнала: 2024, Номер 6(2), С. 100121 - 100121

Опубликована: Март 1, 2024

Язык: Английский

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Insights into Substituent Effects on the Fundamental Photocatalytic Processes of Covalent Organic Frameworks toward H₂ Evolution and H₂O₂ Production Reactions

ACS Catalysis, Год журнала: 2024, Номер 14(15), С. 11262 - 11272

Опубликована: Июль 13, 2024

Язык: Английский

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

ACS Materials Letters, Год журнала: 2024, Номер 6(9), С. 3932 - 3940

Опубликована: Июль 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.

Язык: Английский

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

Journal of environmental chemical engineering, Год журнала: 2024, Номер 12(5), С. 114143 - 114143

Опубликована: Сен. 16, 2024

Язык: Английский

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Covalent Organic Frameworks for Photocatalysis

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Дек. 9, 2024

Abstract The global energy crisis and environmental concerns are driving research into renewable sustainable conversion storage technologies. Solar energy, as an ideal resource, has significant potential to contribute the goal of net‐zero carbon emissions if effectively harnessed converted a reliable storable form energy. Photocatalysts have convert sunlight chemical carriers. In this respect, covalent organic frameworks (COFs) shown great promise due their tunable structure on different length scales, high surface areas, beneficial optical properties such broad visible light absorption. This review offers comprehensive overview key developments in COF‐based photocatalysts for various applications, including water splitting, hydrogen peroxide generation, transformations, dioxide nitrogen reduction. underlying mechanisms, essential principles material design, structure‐function relationships COFs photocatalytic applications discussed. challenges faced by also summarized strategies enhance performance explained, improving crystallinity, regulating molecular structures, tailoring linkages, incorporating cocatalysts. Finally, critical proposed utilization photocatalytically generated chemicals value‐added products.

Язык: Английский

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Donor-acceptor engineering of covalent organic frameworks for enhanced photocatalytic ammonia synthesis

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 159188 - 159188

Опубликована: Янв. 1, 2025

Язык: Английский

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