Zhang Yiyang, Xu Beibei, Zhao Lingfei, Luo Qi, Tao Ying, Lei Yaojie, Lai Wei-Hong, Liu Hua-Kun, Dou Shi-Xue, Wang Yun-Xiao
Institute of Energy Materials Science, University of Shanghai for Science and Technology, Shanghai, 200093, China.
Faculty of Engineering and Information Sciences, Australian Institute of Innovative Materials, University of Wollongong, Innovation Campus, Squires Way, North Wollongong, New South Wales, 2500, Australia.
Adv Mater. 2025 Sep;37(36):e2503153. doi: 10.1002/adma.202503153. Epub 2025 Jun 10.
In contrast to high-concentration electrolyte systems, low-concentration electrolytes provide a cost-effective strategy to advance the commercialization of aqueous zinc-ion batteries (AZIBs). However, such electrolytes frequently exhibit severe dendrite formation caused by localized Zn concentration gradients, which critically compromise the cycling stability and operational safety of AZIBs. In this work, an innovative approach is proposed that involves the in situ construction of a fluoride-ion (F) enriched interfacial layer on zinc anodes. This method facilitates in-plane diffusion of zinc ions at the anode interface, resulting in accelerated lateral growth of zinc deposits rather than dendritic formation. The results indicate that this orientated growth is closely associated with an anionic layer that effectively reduces random and irregular deposition as well as undesirable side reactions. The proposed system exhibits exceptional electrochemical performance within a low-concentration electrolyte framework, achieving a battery lifespan exceeding 1500 h at a current density of 2 mA cm. Furthermore, it maintains Coulombic efficiency above 99% after 800 h of cycling. Additionally, the NaVO·3HO (NVO)//Zn full battery incorporating this additive showcases enhanced long-term cycling performance and improved capacity retention, further confirming the excellent reversibility of the plating/stripping processes for zinc anode.
与高浓度电解质体系相比,低浓度电解质为推进水系锌离子电池(AZIBs)的商业化提供了一种具有成本效益的策略。然而,这类电解质经常会因局部锌浓度梯度而出现严重的枝晶形成,这严重损害了AZIBs的循环稳定性和运行安全性。在这项工作中,提出了一种创新方法,即原位在锌阳极上构建富含氟离子(F)的界面层。这种方法促进了锌离子在阳极界面的面内扩散,导致锌沉积物的横向生长加速,而不是枝晶形成。结果表明,这种定向生长与一个阴离子层密切相关,该阴离子层有效地减少了随机和不规则沉积以及不良副反应。所提出的体系在低浓度电解质框架内表现出优异的电化学性能,在2 mA cm的电流密度下实现了超过1500 h的电池寿命。此外,在循环800 h后,其库仑效率保持在99%以上。此外,包含这种添加剂的NaVO·3HO(NVO)//Zn全电池展现出增强的长期循环性能和改善的容量保持率,进一步证实了锌阳极电镀/剥离过程的优异可逆性。