Organic small molecular heterostructures for enhanced photocatalytic hydrogen evolution via isomer engineering

Conjugated organic molecular heterostructures have been widely investigated as a substitute catalyst for the photocatalytic hydrogen evolution reaction (HER). The controllable replacement of pure carbon rings with heterocyclic units can significantly change the ultraviolet-visible light harvesting a...

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Bibliographic Details
Published in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2023-03, Vol.11 (11), p.5937-5944
Main Authors: Zhang, Qiankun, Li, Dongye, Zhao, Zijie, Zheng, Kunpeng, Wang, Qian, Wang, Binbin, Long, Xiaojing
Format: Article
Language:English
Subjects:
Carbon
Carbon nitride
Catalysts
Catalytic activity
Charge transfer
Chemical composition
Controllability
Heterostructures
Hydrogen
Hydrogen evolution reactions
Hydrogen production
Isomers
Molecular structure
Organic chemistry
Photocatalysis
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Summary:Conjugated organic molecular heterostructures have been widely investigated as a substitute catalyst for the photocatalytic hydrogen evolution reaction (HER). The controllable replacement of pure carbon rings with heterocyclic units can significantly change the ultraviolet-visible light harvesting and photogenerated carrier separation and transport. Thus, we introduce isomer engineering to develop efficient HER catalysts based on quinquephenyl-based molecules with the same elemental composition. Among these catalysts, the central phenyl-linked thiophene molecule P-TP, with graphitic carbon nitride, exhibits a remarkable hydrogen production rate and outstanding photocatalytic stability. Experiments and theoretical calculations reveal that the central phenyl-linked phenyl molecule P-PT is catalytically inactive, while the isomer P-TP, with a planar aromatic structure and delocalized π electrons, enables the heterostructure to have fast intermolecular charge transfer and strong binding energy, and so exhibit efficient photocatalytic activity. More importantly, the well-regulated molecular structure and catalytic activity in the organic small molecular isomeric photocatalysts highlight a new opportunity for photocatalytic HER.
ISSN:2050-7488
2050-7496
DOI:10.1039/D2TA09970E