Janus Dione-Based Conjugated Covalent Organic Frameworks with High Conductivity as Superior Cathode Materials

J Am Chem Soc. 2023 Jan 18;145(2):1022-1030. doi: 10.1021/jacs.2c10509. Epub 2022 Dec 30.

Abstract

The development of conductive covalent organic frameworks (COFs) with high stability is desirable for the practical applications in optoelectronics and energy storage. Herein, we developed a new kind of Janus dione-based COF, which is fully sp2 carbon-conjugated through the connection by olefin units. The electrical conductivity and carrier mobility reached up to 10-3 S cm-1 and 7.8 cm2 V-1 s-1, respectively. In addition, these COFs are strongly robust against various harsh conditions. The well-ordered two-dimensional crystalline structures, excellent porosity, high conductivity, and abundant redox-active carbonyl units render these COFs serviceable as high-performance cathode materials in lithium-ion batteries. It is worth noting that TFPPy-ICTO-COF exhibits a capacity of up to 338 mAh g-1 at a discharge rate of 0.1 C, which sets a new capacity record among COF-based lithium-ion batteries. Its capacity retention was as high as 100% even after 1000 cycles, demonstrating the remarkable stability of these Janus dione-based COF materials. This work not only expands the diversity of olefin-linked COFs but also makes a new breakthrough in energy storage.