Yu Yuanze, Jia Xu, Zhang Qian, Song Hongjiang, Zhang Pengfei, Wang Fanghui, Liu Jie
Youth Innovation Team of Shandong Higher Education Institutions, College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
Weifang Key Laboratory of Green Processing of Separator for Chemical Power Sources, College of Chemistry and Engineering, Weifang Vocational College, Weifang 261108, China.
J Colloid Interface Sci. 2025 Jan;677(Pt B):748-755. doi: 10.1016/j.jcis.2024.08.092. Epub 2024 Aug 13.
The heavy by-products generated on Zn anode surface decrease the active surface of Zn anodes and thus induce uneven Zn deposition, seriously reducing the service life of aqueous Zn-ion batteries (AZIBs). Herein, we propose an elimination strategy enabled by the coordination chemistry to dissolve the main by-products (ZnSO(OH)·xHO). Urea as a proof-of-concept has been applied as the reactivator in the electrolyte to catalytically produce highly active NH on the surface of the by-products. Then the NH can powerfully coordinate with the Zn ion in the by-products to form the soluble complex [Zn(NH)]. Consequently, the proposed electrolyte can not only lead to the timely decomposition of the by-products to prevent the Zn anode from inactivation during cycling, but also repair the waste Zn anodes for reutilization. The action mechanism has been systematically demonstrated via theoretical simulation and experimental study. As a result, the high durability with ultrahigh cumulative capacity of 10,600 mAh cm for the Zn||Zn symmetric cell has been achieved at 40 mA cm. Particularly, the dead Zn||Zn symmetric cells and Zn||LiFePO full cells have been successfully reactivated. This study lights a new route to extend the cell lifespan and reuse waste Zn-ion batteries.
锌阳极表面产生的大量副产物会降低锌阳极的活性表面，从而导致锌沉积不均匀，严重缩短水系锌离子电池（AZIBs）的使用寿命。在此，我们提出一种基于配位化学的消除策略，以溶解主要副产物（ZnSO(OH)·xHO）。作为概念验证的尿素已被用作电解质中的再活化剂，以在副产物表面催化产生高活性的NH。然后，NH可以与副产物中的锌离子强烈配位，形成可溶性络合物[Zn(NH)]。因此，所提出的电解质不仅可以导致副产物及时分解，以防止锌阳极在循环过程中失活，还可以修复废弃的锌阳极以供再利用。通过理论模拟和实验研究系统地证明了其作用机制。结果，在40 mA cm下，Zn||Zn对称电池实现了10,600 mAh cm的超高累积容量的高耐久性。特别是，已成功重新激活了失效的Zn||Zn对称电池和Zn||LiFePO全电池。这项研究为延长电池寿命和再利用废弃锌离子电池开辟了一条新途径。
