Decoding Hydrogen-Bond Network of Electrolyte for Cryogenic Durable Aqueous Zinc-Ion Batteries

Abstract Aqueous zinc-ion batteries (AZIBs) hold great promise for next-generation energy storage but face challenges such as Zn dendrite growth, side reactions, and limited performance at low temperatures. Here, we propose an electrolyte design strategy that reconstructs the hydrogen-bond network through the synergistic effect of glycerol (GL) and methylsulfonamide (MSA), enabling the formation of a (100)-oriented Zn anode. This design significantly broadens the operating current and temperature windows of AZIBs. As a result, Zn||Zn symmetric cells exhibit remarkable cycling stability, achieving 4,000 h at 1 mA cm −2 and 600 h at 40 mA cm −2 (both at 1 mAh cm −2 capacity); even at −20 °C, Zn||Zn symmetric cells deliver ultra-stable cycling for over 5,400 h. Furthermore, Zn||VO 2 full cells retain 77.3% of their capacity after 2,000 cycles at 30 °C with a current density of 0.5 A g −1 and 85.4% capacity retention after 2,000 cycles at −20 °C and 0.25 A g −1 . These results demonstrate a robust pathway for enhancing the practicality and low-temperature adaptability of AZIBs.