Wang Yifan, Yan Weilin, Zhu Xuejun, Li Jinghao, Li Zhaoqian, Zhang Hong, Ren Yingke, Mo Lie, Huang Yang, Zhang Lei, Hu Linhua
Key Laboratory of Photovoltaic and Energy Conservation Materials, CAS, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei, Anhui, 230031, P.R. China.
Science Island Branch of Graduate School University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.
Angew Chem Int Ed Engl. 2025 Aug 25;64(35):e202508556. doi: 10.1002/anie.202508556. Epub 2025 Jul 26.
Hydrogel electrolytes hold great promise in tackling severe issues facing aqueous zinc-ion batteries (AZIBs). However, to satisfy the quest of flexible and eco-friendly batteries, developing low-cost and high mechanical durability hydrogel electrolyte remains a challenge. Here, employing the zincophilic solubilizer urea, we break the classical concentration limits of the low-cost Zn(Ac) salt and introduce it into the hydrogel skeleton. The "salting out" effect give the polymer chain sediments a tighter bundle and twist effect. The as-formed hydrogel electrolyte can endure 557% high elongation and 3.7 MPa compressive strength to resist repeated zinc plating/striping process and external physical stimuli. The in situ polyurea solid electrolyte interphase (SEI) layer leads to thermodynamically stable anode/electrolyte interface. Utilizing the hydrogel electrolyte, the zinc anode shows high reversibility, leading to an average Coulombic efficiency (CE) of 99.93% for 150 cycles on the Zn//Cu battery. When assembled with NHVO cathode (NVO), the full battery delivers a high capacity of 253.8 mAh g beyond 1000 cycles longevity at 1 A g. The pouch battery also shows a high capacity of 280.7 mAh g at 500 mA g and operate steadily for 90.13% retention after 200 cycles, and maintained a stable voltage even experienced bending and folding.
水凝胶电解质在解决水系锌离子电池（AZIBs）面临的严峻问题方面具有巨大潜力。然而，为了满足柔性和环保型电池的需求，开发低成本且具有高机械耐久性的水凝胶电解质仍然是一项挑战。在此，我们采用亲锌增溶剂尿素，突破了低成本Zn(Ac)盐的经典浓度限制，并将其引入水凝胶骨架中。“盐析”效应使聚合物链沉积物产生更紧密的束状和扭曲效应。所形成的水凝胶电解质能够承受557%的高伸长率和3.7 MPa的抗压强度，以抵抗反复的锌电镀/剥离过程和外部物理刺激。原位聚脲固体电解质界面（SEI）层导致阳极/电解质界面具有热力学稳定性。利用这种水凝胶电解质，锌阳极表现出高可逆性，在Zn//Cu电池上150次循环的平均库仑效率（CE）为99.93%。当与NHVO阴极（NVO）组装时，全电池在1 A g的电流下循环1000次以上，具有253.8 mAh g的高容量。软包电池在500 mA g的电流下也具有280.7 mAh g的高容量，并且在200次循环后仍能稳定运行，容量保持率为90.13%，即使经历弯曲和折叠也能保持稳定电压。
