Rational Design of PDI-Based Linear Conjugated Polymers for Highly Effective and Long-Term Photocatalytic Oxygen Evolution
© 2023 Wiley-VCH GmbH.
| Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 25 vom: 04. Juni, Seite e2300655 |
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| 1. Verfasser: | |
| Weitere Verfasser: | , , , , , , |
| Format: | Online-Aufsatz |
| Sprache: | English |
| Veröffentlicht: |
2023
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| Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
| Schlagworte: | Journal Article build-in electric field intramolecular dipole moment linear conjugated polymers photocatalytic oxygen evolution |
| Zusammenfassung: | © 2023 Wiley-VCH GmbH. Constructed through relatively weak noncovalent forces, the stability of organic supramolecular materials has shown to be a challenge. Herein, the designing of a linear conjugated polymer is proposed through creating a chain polymer connected via bridging covalent bonds in one direction and retaining π-stacked aromatic columns in its orthogonal direction. Specifically, three analogs of linear conjugated polymers through tuning the aromatic core and its covalently linked moiety (bridging group) within the building block monomer are prepared. Cooperatively supported by strong π-π stacking interactions from the extended aromatic core of perylene and favorable dipole-dipole interactions from the bridging group, the as-expected high crystallinity, wide light absorption, and increased stability are successfully achieved for Oxamide-PDI (perylene diimide) through ordered molecular arrangement, and present a remarkable full-spectrum oxygen evolution rate of 5110.25 µmol g-1 h-1 without any cocatalyst. Notably, experimental and theoretical studies reveal that large internal dipole moments within Oxamide-PDI together with its ordered crystalline structure enable a robust built-in electric field for efficient charge carrier migration and separation. Moreover, density functional theory (DFT) calculations also reveal oxidative sites located at carbon atoms next to imide bonds and inner bay positions based on proven spatially separated photogenerated electrons and holes, thus resulting in highly efficient water photolysis into oxygen |
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| Beschreibung: | Date Completed 22.06.2023 Date Revised 22.06.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202300655 |