Affiliation:
1. School of Chemical & Environmental Engineering China University of Mining and Technology (Beijing) Beijing 100083 P. R. China
2. State Key Laboratory of Applied Organic Chemistry (Lanzhou University) Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province. College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 P. R. China
3. Future Science Research Institute Global Scientific and Technological Innovation Center, Zhejiang University Hangzhou 310013 P. R. China
Abstract
AbstractConstructed 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 retainingπ‐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 strongπ–πstacking 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−1without 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.
Funder
Fundamental Research Funds for the Central Universities
National Natural Science Foundation of China
Subject
Mechanical Engineering,Mechanics of Materials,General Materials Science
Cited by
13 articles.
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