Low band gap semiconducting covalent organic framework films with enhanced photocatalytic hydrogen evolution

文献情報

出版日 2023-11-20

DOI 10.1039/D3TA04552H

インパクトファクター 12.732

著者

Hüseyin Küçükkeçeci, Rajendra Prasad Paitandi, Vincent Weigelt, Veit Dippold, Shu Seki, Arne Thomas

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要旨

Semiconducting covalent organic frameworks (COFs) are emerging materials for the photocatalytic hydrogen (H2) evolution, owing to their porous periodic network of π-conjugated scaffolds with tuneable band gap and optoelectronic properties. The optoelectronic properties, for example, band gap, band position and charge carrier mobility of the COF photocatalyst, play a pivotal role in their activity in photocatalytic conversions. However, it is challenging to control the band gap and band position of COFs simultaneously. In the present manuscript, we investigate the photocatalytic performance of low band gap semiconducting COFs constructed from anthracene containing π-conjugated building blocks linked with different hydroxy functionalized 1,3,5-triformylbenzene. Along with crystalline and porous COF powders, thin COF films were synthesized successfully. Such thin COF films offer several advantages in photocatalytic applications owing to their low light scattering, scalability and reusability. It is furthermore shown that the number of hydroxy groups on the 1,3,5-triformylbenzene linker largely influences the properties of the final COFs. The COF prepared from the linker with two hydroxy groups exhibits the lowest band gap of 1.8 eV and efficient exciton migration due to the formation of J-type aggregates resulting in the maximum hydrogen evolution rate (8.4 ± 0.5 mmol g−1 h−1) in the powder state. On the other hand, for COF films a steady increase in hydrogen evolution rate is observed with increasing hydroxy-functionalization and reaches a maximum for three hydroxy groups (1.6 ± 0.2 mmol m−2 h−1) due to the enhanced charge carrier mobility.

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

Low band gap semiconducting covalent organic framework films with enhanced photocatalytic hydrogen evolution

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