Wang Haoran, Deng Shenzhen, Wang Shuai, Li Wulong, Yuan Shixing, Han Jing, Fu Hongyan, Xu Bingang, Wei Lei
School of Electrical and Electronic Engineering, Nanyang Technological University, Singapore, 639798, Singapore.
School of Electronic Science and Engineering (National Model Microelectronics College), Xiamen University, Xiamen, 361005, China.
Angew Chem Int Ed Engl. 2025 Mar 17;64(12):e202422395. doi: 10.1002/anie.202422395. Epub 2025 Jan 2.
Aqueous zinc-ion batteries (ZIBs) are playing an increasingly important role in the field of energy storage owing to their low cost, high safety, and environmental friendliness. However, their practical applications are still handicapped by severe dendrite formation and side reactions (e.g., hydrogen evolution reaction and corrosion) on the zinc anodes. Herein, a low-concentration high-entropy (HE) electrolyte strategy is proposed to achieve high reversibility and ultra-durable zinc metal anode. Specifically, this HE electrolyte features multiple anions participating in coordination and highly disordered solvation shells, which would disrupt the intrinsic H-bond network between water molecules and suppress interfacial side reactions. Moreover, these diversified weakly solvated structures can lower the solvation energy of Zn solvation configurations and enhance zinc ion diffusion kinetics, thereby promoting uniform Zn deposition and electrode interface stability. Consequently, Zn||Zn symmetric cells exhibit over 2,000 hours of cycling stability, and Zn||Cu asymmetric cells achieve a high average Coulombic efficiency of 99.9 % over 500 cycles. Furthermore, the Zn||PANI full cell with the optimized HE-50 mM electrolyte delivers a high specific capacity of 110.7 mAh g over 2,000 cycles at 0.5 A g and a capacity retention of 70.4 % at 15 A g after 10,000 cycles. Remarkably, even at a low temperature of -20 °C, the Zn||PANI full cells equipped with HE-50 mM electrolyte still demonstrate long-term cycling stability over 600 cycles with a high-capacity retention of 93.5 %. This research provides a promising strategy for the design of aqueous electrolytes, aiding in the development of low-cost, high-safety, and high-performance aqueous batteries.
水系锌离子电池（ZIBs）因其低成本、高安全性和环境友好性，在储能领域发挥着越来越重要的作用。然而，锌负极上严重的枝晶形成和副反应（如析氢反应和腐蚀）仍然阻碍着它们的实际应用。在此，提出了一种低浓度高熵（HE）电解质策略，以实现高可逆性和超耐用的锌金属负极。具体而言，这种HE电解质具有多个参与配位的阴离子和高度无序的溶剂化壳层，这会破坏水分子之间固有的氢键网络并抑制界面副反应。此外，这些多样化的弱溶剂化结构可以降低锌溶剂化构型的溶剂化能并增强锌离子扩散动力学，从而促进锌的均匀沉积和电极界面稳定性。因此，Zn||Zn对称电池表现出超过2000小时的循环稳定性，Zn||Cu不对称电池在500次循环中实现了99.9%的高平均库仑效率。此外，采用优化的HE-50 mM电解质的Zn||PANI全电池在0.5 A g下2000次循环中提供了110.7 mAh g的高比容量，在15 A g下10000次循环后容量保持率为70.4%。值得注意的是，即使在-20°C的低温下，配备HE-50 mM电解质的Zn||PANI全电池在600次循环中仍表现出长期循环稳定性，高容量保持率为93.5%。这项研究为水系电解质的设计提供了一种有前景的策略，有助于开发低成本、高安全性和高性能的水系电池。
