P-type semiconducting organic cathode materials have received extensive attention in recent years due to their high redox potential, which however suffer from the low capacity and unsatisfactory energy density. Here, two-dimensional covalent organic frameworks (COFs) namely TAPA-Pz-COF and TATTA-Pz-COF were constructed by one p-type semiconductor methylphenazine possessing high capacity with another p-type semiconductor tris-(4-aminophenyl)amine (TAPA) and 4,4′,4′'-(1,3,5-triazine-2,4,6-triayl)trainline (TATTA), respectively. Electron microscopy, powder X-ray diffraction, and N adsorption-desorption measurements demonstrate the highly ordered mesoporous structure of both COFs with a Brunauer−Emmett−Teller surface area of 472–855 m g and pore size of 3.2–3.9 nm. The cyclic voltammetry curves of these two COFs display a pair of broad redox peaks at ca. 3.15/3.05 V vs. Li/Li, revealing their p-type semiconductor nature and enabling them to be high energy density cathodes for Li-ion battery. In particular, TATTA-Pz-COF shows a high specific capacity of 324 mA h g at 100 mA g with a record-high energy density of 737 W h kg among all the organic polymer and COF electrodes. This work will help to develop high-performance and low-cost organic cathodes for energy storage.

中文翻译：

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用于高能量密度锂离子电池正极的P型半导体共价有机骨架

P型半导体有机正极材料近年来因其高氧化还原电位而受到广泛关注，但其容量低且能量密度不理想。这里，二维共价有机骨架（COF），即TAPA-Pz-COF和TATTA-Pz-COF是由一种具有高容量的p型半导体甲基吩嗪与另一种p型半导体三（4-氨基苯基）胺构建而成。分别为 TAPA) 和 4,4',4''-(1,3,5-三嗪-2,4,6-三酰基)trainline (TATTA)。电子显微镜、粉末 X 射线衍射和 N2 吸附-解吸测量表明两种 COF 具有高度有序的介孔结构，Brunauer-Emmett-Teller 表面积为 472-855 mg，孔径为 3.2-3.9 nm。这两个 COF 的循环伏安曲线在约 100 处显示出一对宽的氧化还原峰。 3.15/3.05 V 与 Li/Li，揭示了它们的 p 型半导体性质，并使它们成为锂离子电池的高能量密度阴极。特别是，TATTA-Pz-COF在100 mA g-1下表现出324 mA hg的高比容量，在所有有机聚合物和COF电极中创下了737 W h kg的最高能量密度。这项工作将有助于开发高性能和低成本的用于能量存储的有机阴极。