Wang Xinyi, Liu Liyang, Hu Zewei, Han Chao, Xu Xun, Dou Shixue, Li Weijie
State Key Laboratory for Powder Metallurgy, Central South University Changsha 410083 China
Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong Wollongong 2522 Australia.
Chem Sci. 2024 Sep 20;15(42):17348-61. doi: 10.1039/d4sc04611k.
The practical application of aqueous zinc-ion batteries (AZIBs) is hindered by their low coulombic efficiency (CE) and unstable cycle life. Numerous electrolyte-additive-related studies have been performed, but most of the focus has been on the Zn plating process. In fact, practical AZIBs undergo stripping in practice rather than plating in the initial cycle, because the commonly used cathodes in the charged state do not have zinc ions, so a uniform stripping process is crucial for the cell performance of AZIBs. Here, we propose an electron-losing regulation strategy for stripping modulation by adding additives. Oxolane (OL) was chosen as the model additive to verify this assumption. It is found that OL adsorbs onto the uneven initial Zn surface and accelerates the dissolution of the Zn tips, thus providing a uniform Zn anode during the stripping process. The oxygen atoms in OL reduce the surface energy of Zn and promote the exposure of the Zn (002) surface during plating. Consequently, cells with the OL electrolyte additive maintained a long lifespan and showed superior reversibility with a high average CE. The findings of this work lead to a deep understanding of the underlying mechanism of Zn anode stripping and provide new guidance for designing electrolyte additives.
水系锌离子电池(AZIBs)的实际应用受到其低库仑效率(CE)和不稳定循环寿命的阻碍。已经进行了许多与电解质添加剂相关的研究,但大多数研究都集中在锌电镀过程上。实际上,实际的AZIBs在初始循环中经历的是脱锌过程而非镀锌过程,因为充电状态下常用的阴极不含锌离子,所以均匀的脱锌过程对AZIBs的电池性能至关重要。在此,我们提出一种通过添加添加剂来调控脱锌的电子损失调控策略。选择四氢呋喃(OL)作为模型添加剂来验证这一假设。研究发现,OL吸附在初始不均匀的锌表面上,加速了锌尖端的溶解,从而在脱锌过程中提供了均匀的锌阳极。OL中的氧原子降低了锌的表面能,并在镀锌过程中促进了Zn(002)表面的暴露。因此,添加OL电解质添加剂的电池保持了较长的寿命,并表现出优异的可逆性和高平均CE。这项工作的研究结果有助于深入理解锌阳极脱锌的潜在机制,并为设计电解质添加剂提供新的指导。