Ma Dingxuan, Zhao Huimin, Cao Fan, Zhao Huihui, Li Jixin, Wang Lei, Liu Kang
College of Chemistry and Molecular Engineering, Key Laboratory of Optic-Electric Sensing and Analytical Chemistry for Life Science, MOE, Shandong Key Laboratory of Biochemical Analysis, Qingdao University of Science and Technology Qingdao 266042 Shandong P. R. China
School of Materials Science and Engineering, Shandong Jianzhu University Jinan 250101 Shandong P. R. China.
Chem Sci. 2022 Feb 8;13(8):2385-2390. doi: 10.1039/d1sc06412f. eCollection 2022 Feb 23.
Aqueous rechargeable zinc-ion batteries (ZIBs) provide high theoretical capacity, operational safety, low-cost and environmental friendliness for large-scale energy storage and wearable electronic devices, but their future development is plagued by low capacity and poor cycle life due to the lack of suitable cathode materials. In this work, a covalent organic framework (Tp-PTO-COF) with multiple carbonyl active sites is synthesized and successfully introduced in aqueous rechargeable ZIBs for the first time. Tp-PTO-COF delivers high specific capacities of 301.4 and 192.8 mA h g at current densities of 0.2 and 5 A g, respectively, along with long-term durability and flat charge-discharge plateaus. The remarkable electrochemical performance is attributed to the abundance of nucleophilic carbonyl active sites, well defined porous structure and inherent chemical stability of Tp-PTO-COF. Moreover, the structural evolution and Zn ion intercalation mechanism are discussed and revealed by the experimental analysis and density functional theory calculations. These results highlight a new avenue to develop organic cathode materials for high performance and sustainable aqueous rechargeable ZIBs.
水系可充电锌离子电池（ZIBs）为大规模储能和可穿戴电子设备提供了高理论容量、运行安全性、低成本和环境友好性，但其未来发展因缺乏合适的正极材料而受到低容量和循环寿命差的困扰。在这项工作中，首次合成了具有多个羰基活性位点的共价有机框架（Tp-PTO-COF）并成功引入水系可充电锌离子电池中。Tp-PTO-COF在电流密度分别为0.2和5 A g时，分别具有301.4和192.8 mA h g的高比容量，同时具有长期耐久性和稳定的充放电平台。卓越的电化学性能归因于Tp-PTO-COF丰富的亲核羰基活性位点、明确的多孔结构和固有的化学稳定性。此外，通过实验分析和密度泛函理论计算对结构演变和锌离子嵌入机制进行了讨论和揭示。这些结果为开发用于高性能和可持续水系可充电锌离子电池的有机正极材料开辟了一条新途径。
