Journal
MATERIALS TODAY
Volume 61, Issue -, Pages 22-29Publisher
ELSEVIER SCI LTD
DOI: 10.1016/j.mattod.2022.10.024
Keywords
p-Conjugated; Perylene diimide; Photocatalysis; Macro-dipole; Aerobic coupling
Categories
Funding
- Guizhou Provincial Science and Technology Foundation
- Young Science and Technology Talents Development Project of Educa- tion Department in Guizhou Province
- National Natural Science Foundation of China
- [ZK2021069]
- [KY2022144]
- [22268015]
- [21938002]
- [21725602]
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This study reports on the varied intramolecular angles of PDI polymers and investigates the role of pi-conjugated non-planar molecules in photocatalysis. Results demonstrate that the vertical structure of non-planar molecules enhances the electric field and facilitates charge transfer and exciton dissociation, as well as promotes carrier migration and separation. This research provides a new interpretation for developing highly efficient photocatalysts to address sustainability issues.
pi-Conjugated supramolecular with higher delocalization of electrons has attracted considerable attention in enhancing the charge transfer in photocatalysis. However, those conjugated macro-molecules often possess varied rotational geometries, which will significantly deteriorate charge mobility but still inexplicitly. Herein, we reported diversified PDI polymers with intramolecular angles of 94.7 degrees, 149.7 degrees and 176.3 degrees to explore the role of pi-conjugated non-planar molecules. Density functional theory (DFT) calculations and experimental results show that vertical structural PDIMH has antibonding in anisotropic polarizable monomer to generate a macro-dipole, which greatly expands the built-in electric field and facilitates charge transfer and exciton dissociation. On the other hand, the vertical angle is favorable for the face-to-face overlap of the homogeneous molecules, which will create a carrier migration channel and promote carrier separation. Notably, PDIMH exhibited highly effective photocatalytic sterilization (near 100% in 2 h) and benzylamine oxidation (conversion rate up to 300 mmol g(-1)h(-1)), which is superior to other ever reported catalysts. This work provides a new interpretation for regulating molecular geometry in developing highly efficient photocatalyst to solve future sustainable issues.
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