Electrochemically exfoliated covalent organic frameworks for improved photocatalytic hydrogen evolution

文献情報

出版日 2023-12-06

DOI 10.1039/D3TA06312G

インパクトファクター 12.732

著者

Ruijuan Zhang, Pengda Zhai, Xinying Liu

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要旨

Covalent organic frameworks (COFs) have recently shown great prospects for their photocatalytic applications in solar-to-hydrogen conversion. Nevertheless, most of the COFs were synthesized as crystalline bulk powders, impeding the exposure of surface catalytically active sites. Developing a noninvasive and expedient route to exfoliate COFs in liquids still remains a great challenge. Herein, two typical 1,3,5-tri(thiophen-2-yl)benzene (TTB)-based COFs (one possesses non-donor–acceptor constitution, denoted as TTB-PB, while the other possesses donor–acceptor constitution, denoted as TTB-PT) were synthesized via Schiff-base condensation reactions. Subsequently, these bulk COFs were exfoliated via a facile electrochemical strategy in aqueous systems. The obtained exfoliated COFs can not only facilitate photo-triggered exciton dissociation but also afford more accessible active sites and enhanced hydrophilicity. Consequently, the exfoliated COFs exhibited much higher photocatalytic capabilities for H2 evolution from water in sharp contrast to their unexfoliated precursors. It is to be noted that the exfoliated donor–acceptor COFs achieved a maximum H2 evolution rate of 27.24 mmol h−1 g−1, which is superior to that of the exfoliated non-donor–acceptor COF (i.e., 9.86 mmol h−1 g−1), and also ranks at the top of the state-of-the-art thiophen-based COF photocatalysts in the literature. This work enriches the fabrication approach of COF exfoliation. Furthermore, utilizing the synergetic strategy of aqueous electrochemical exfoliation and suitable molecular design, TTB-based COFs demonstrate promising photocatalytic activity.

掲載誌

Journal of Materials Chemistry A

CiteScore: 19.5

自己引用率: 4.7%

年間論文数: 2211

Journal of Materials Chemistry A, B & C cover high quality studies across all fields of materials chemistry. The journals focus on those theoretical or experimental studies that report new understanding, applications, properties and synthesis of materials. The journals have a strong history of publishing quality reports of interest to interdisciplinary communities and providing an efficient and rigorous service through peer review and publication. The journals are led by an international team of Editors-in-Chief and Associate Editors who are all active researchers in their fields. Journal of Materials Chemistry A, B & C are separated by the intended application of the material studied. Broadly, applications in energy and sustainability are of interest to Journal of Materials Chemistry A, applications in biology and medicine are of interest to Journal of Materials Chemistry B, and applications in optical, magnetic and electronic devices are of interest to Journal of Materials Chemistry C. More than one Journal of Materials Chemistry journal may be suitable for certain fields and researchers are encouraged to submit their paper to the journal that they feel best fits for their particular article. Example topic areas within the scope of Journal of Materials Chemistry A are listed below. This list is neither exhaustive nor exclusive. Artificial photosynthesis Batteries Carbon dioxide conversion Catalysis Fuel cells Gas capture/separation/storage Green/sustainable materials Hydrogen generation Hydrogen storage Photocatalysis Photovoltaics Self-cleaning materials Self-healing materials Sensors Supercapacitors Thermoelectrics Water splitting Water treatment

Electrochemically exfoliated covalent organic frameworks for improved photocatalytic hydrogen evolution

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