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Optimizing the Structure and Electrochemical Properties of Benzoquinone-Embedded COF via Heat Treatment for a High-Energy Organic Cathode

结晶度 材料科学 阴极 电化学 化学工程 阳极 电极 石墨 锂(药物) 共价有机骨架 复合材料 物理化学 医学 化学 多孔性 工程类 内分泌学
作者
Kamran Amin,Warisha Mehmood,Jianqi Zhang,Sadia Ahmed,Lijuan Mao,Chuanfu Li,Binbin Zhang,Zhixiang Wei
出处
期刊:ACS Applied Materials & Interfaces [American Chemical Society]
被引量:1
标识
DOI:10.1021/acsami.3c11998
摘要

A benzoquinone-embedded aza-fused covalent organic framework (BQ COF) with the maximum loading of redox-active units per molecule was employed as a cathode for lithium-ion batteries (LIBs) to achieve high energy and power densities. The synthesis was optimized to obtain high crystallinity and improved electrochemical performance. Synthesis at moderate temperature followed by a solid-state reaction was found to be particularly useful for achieving good crystallinity and the activation of the COF. When used as a cathode for LIBs, very high discharge capacities of 513, 365, and 234 mAh g-1 were obtained at 0.1C, 1C, and 10C, respectively, showing a remarkable rate performance. More than 70% of the initial capacity was retained after 1000 cycles when the cathode was investigated for cyclic performance at 2.5C. We demonstrated that a straightforward heat treatment led to enhanced crystallinity, an optimized structure, and favorable morphology, resulting in enhanced electrode kinetics and an improved overall electrochemical behavior. A comparative study was conducted involving an aza-fused COF lacking carbonyl groups (TAB COF) and a small molecule containing phenazine and carbonyl (3BQ), providing useful insights into new material design. A full cell was assembled with graphite as the anode to assess the commercial feasibility of BQ COF, and a discharge capacity of 240 mAh g-1 was obtained at 0.5C. Furthermore, a pouch-type cell with a high discharge capacity and an excellent rate performance was assembled, demonstrating the practical applicability of our designed cathode. Considering the entire mass of the working electrode, a specific energy density of 492 Wh kg-1 and a power density of 492 W kg-1 were achieved at the high current density of 1C, which are comparable to those of commercially available cathodes. These results highlight the promise of organic electrode materials for next-generation lithium-ion batteries. Furthermore, this study provides a systematic approach for simultaneously designing organic materials with high power and energy densities.
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