Dual donor-acceptor covalent organic frameworks for hydrogen peroxide photosynthesis

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Aug. 28, 2023

Constructing photocatalytically active and stable covalent organic frameworks containing both oxidative reductive reaction centers remain a challenge. In this study, benzotrithiophene-based with spatially separated redox are rationally designed for the photocatalytic production of hydrogen peroxide from water oxygen without sacrificial agents. The triazine-containing framework demonstrates high selectivity H2O2 photogeneration, yield rate 2111 μM h-1 (21.11 μmol 1407 g-1 h-1) solar-to-chemical conversion efficiency 0.296%. Codirectional charge transfer large energetic differences between linkages linkers verified in double donor-acceptor structures periodic frameworks. sites mainly concentrated on electron-acceptor fragments near imine bond, which regulate electron distribution adjacent carbon atoms to optimally reduce Gibbs free energy O2* OOH* intermediates during formation H2O2.

Language: Английский

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Piezo‐Photocatalytic Synergy in BiFeO₃@COF Z‐Scheme Heterostructures for High‐Efficiency Overall Water Splitting

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(44)

Published: Sept. 13, 2022

Solar-driven overall water splitting is an ideal way to generate renewable energy while still challenging. For the first time, this work combined covalent organic frameworks (COFs) and piezoelectric material by linkages form Z-scheme core@shell heterostructure for splitting. Benefiting from synergistic effect between polarized electric field photo-generated charges, as well precise adjustment of shell thickness, carrier separation utilization efficiency greatly improved. The optimal BiFeO3 @TpPa-1-COF photocatalyst revealed hydrogen (H2 ) oxygen (O2 production rates 1416.4 708.2 μmol h-1 g-1 under excitation ultrasonication coupled with light irradiation, which best performance among various piezo- COF-based photocatalysts. This provides a new sight practical application highly efficient photocatalytic

Language: Английский

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Covalent Organic Frameworks for Energy Conversion in Photocatalysis

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(34)

Published: April 24, 2023

Abstract Intensifying energy crises and severe environmental issues have led to the discovery of renewable sources, sustainable conversion, storage technologies. Photocatalysis is a green technology that converts eco‐friendly solar into high‐energy chemicals. Covalent organic frameworks (COFs) are porous materials constructed by covalent bonds show promising potential for converting chemicals owing their pre‐designable structures, high crystallinity, porosity. Herein, we highlight recent progress in synthesis COF‐based photocatalysts applications water splitting, CO 2 reduction, H O production. The challenges future opportunities rational design COFs advanced discussed. This Review expected promote further development toward photocatalysis.

Language: Английский

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Linkage Microenvironment of Azoles‐Related Covalent Organic Frameworks Precisely Regulates Photocatalytic Generation of Hydrogen Peroxide

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(36)

Published: July 18, 2023

Artificial H2 O2 photosynthesis by covalent organic frameworks (COFs) photocatalysts is promising for wastewater treatment. The effect of linkage chemistry COFs as functional basis to photoelectrochemical properties and photocatalysis remains a significant challenge. In this study, three kinds azoles-linked including thiazole-linked TZ-COF, oxazole-linked OZ-COF imidazole-linked IZ-COF were successfully synthesized. More accessible channels charge transfer constructed in TZ-COF via the donor-π-acceptor structure between thiazole pyrene linker, leading efficient suppression photoexcited recombination. Density theory calculations support experimental studies, demonstrating that more favorable formation *O2 intermediate production than oxazole imidazole linkages. real active sites located at benzene ring fragment unit azole linkage.

Language: Английский

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Covalent Organic Frameworks Enable Sustainable Solar to Hydrogen Peroxide

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(12)

Published: Dec. 6, 2023

Abstract As a chemical product with rapidly expanding demand in the field of modern energy and environmental applications, hydrogen peroxide (H 2 O ) has garnered widespread attention. However, existing industrial production H is plagued by high consumption, harmful waste emission, severe safety issues, making it difficult to satisfy environmental/economic concept. Artificial photosynthesis offers viable strategy for green sustainable since uses sunlight as an source initiate reaction oxygen water produce . Among various photocatalysts, covalent organic frameworks (COFs), featuring highly ordered skeletons well‐defined active sites, have emerged promising photocatalysts production. This review presents nascent burgeoning area photocatalytic based on COFs. First, brief overview technology provided, followed detailed introduction principles evaluation generation. Subsequently, latest research progress judicious design COFs expounded, particular emphasis manipulating electronic structures redox sites. Finally, outlook challenges future opportunities proposed, hope stimulating further explorations novel molecular‐designed photosynthesis.

Language: Английский

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Magnetic Covalent Organic Framework Composites for Wastewater Remediation

Small, Journal Year: 2023, Volume and Issue: 19(37)

Published: May 8, 2023

Abstract Covalent organic frameworks (COFs) with high specific surface area, tailored structure, easy functionalization, and excellent chemical stability have been extensively exploited as fantastic materials in various fields. However, most cases, COFs prepared powder form suffer from the disadvantages of tedious operation, strong tendency to agglomerate, poor recyclability, greatly limiting their practical application environmental remediation. To tackle these issues, fabrication magnetic (MCOFs) has attracted tremendous attention. In this review, several reliable strategies for MCOFs are summarized. addition, recent outstanding adsorbents removal contaminants including toxic metal ions, dyes, pharmaceuticals personal care products, other pollutants is discussed. Moreover, in‐depth discussions regarding structural parameters affecting potential highlighted detail. Finally, current challenges future prospects field provided expectation boost application.

Language: Английский

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Decade Milestone Advancement of Defect-Engineered g-C3N4 for Solar Catalytic Applications

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: Jan. 4, 2024

Over the past decade, graphitic carbon nitride (g-C

Language: Английский

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The Collision between g‐C₃N₄ and QDs in the Fields of Energy and Environment: Synergistic Effects for Efficient Photocatalysis

Small, Journal Year: 2023, Volume and Issue: 19(14)

Published: Jan. 2, 2023

Abstract Recently, graphitic carbon nitride (g‐C 3 N 4 ) has attracted increasing interest due to its visible light absorption, suitable energy band structure, and excellent stability. However, low specific surface area, finite response range (<460 nm), rapid photogenerated electron–hole (e − –h + pairs recombination of the pristine g‐C limit practical applications. The small size quantum dots (QDs) endows properties abundant active sites, wide absorption spectrum, adjustable bandgap, but inevitable aggregation. Studies have confirmed that integration QDs not only overcomes these limitations individual component, also successfully inherits each advantage. Encouraged by advantages, synthetic strategies fundamental QDs/g‐C composites are briefly elaborated in this review. Particularly, synergistic effects analyzed comprehensively, including enhancement photocatalytic performance avoidance Then, applications fields environment described further combined with DFT calculation reveal reaction mechanisms. Moreover, stability reusability analyzed. Finally, future development solution existing problems prospected.

Language: Английский

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Multiple path-dominated activation of peroxymonosulfate by MOF-derived Fe2O3/Mn3O4 for catalytic degradation of tetracycline

Journal of environmental chemical engineering, Journal Year: 2023, Volume and Issue: 11(5), P. 110395 - 110395

Published: June 19, 2023

Language: Английский

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Recent progress of radionuclides separation by porous materials

Science China Chemistry, Journal Year: 2024, Volume and Issue: 67(11), P. 3515 - 3577

Published: Sept. 26, 2024

Language: Английский

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