Rational Design of PDI‐Based Linear Conjugated Polymers for Highly Effective and Long‐Term Photocatalytic Oxygen Evolution

材料科学 共轭体系 共价键 聚合物 二亚胺 堆积 超分子聚合物 密度泛函理论 部分 光化学 单体 超分子化学 化学物理 计算化学 分子 化学 有机化学 复合材料
作者
Di Liu,Xuan Yang,Peiyan Chen,Xinling Zhang,GaoYuan Chen,Qiwei Guo,Huan Hou,Yi Li
出处
期刊:Advanced Materials [Wiley]
卷期号:35 (25) 被引量:54
标识
DOI:10.1002/adma.202300655
摘要

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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