Stable zinc anode interface and environmentally adaptable hydrogel electrolytes for stable operation of zinc-ion hybrid supercapacitors

Abstract

Hydrogel-based zinc ion hybrid supercapacitors (ZIHS) have stood out from many energy storage device candidates due to their battery-level energy density, inherent flexibility, and safety. Nevertheless, the inevitable dendrite growth of Zn anodes and sharp capacity degradation at low-temperature seriously hinder their practical application. Herein, a dense ZnF2 solid electrolyte interface protective layer was constructed in situ on the Zn electrode surface by a simple chemical deposition method, effectively isolating the water molecules and alleviating the water-induced dendrite growth and parasitic reaction. To achieve the flexible ZIHS with environmental adaptability, a self-adhesion and anti-freezing zwitterionic hydrogel electrolyte was fabricated to afford superior ionic conductivity (97.1 mS cm−1), excellent anti-drying ability, and robust interfacial adhesion. Benefitting from the integrated merits of the as-designed electrolyte and electrode, the ZIHS delivered excellent mechanical adaptability, favorable energy density (103.9 Wh kg−1 at 270.1 W kg−1), broad operating temperature range (−40 to 40 °C), along with long-term cycling stability (12,000 cycles) with 90.3 % capacity retention at −25 °C. Notably, the unencapsulated ZIHS achieved exceptional electrochemical stability in an open environment. This finding provides valuable insights for constructing durable, flexible, and environmentally adaptable zinc-based energy storage systems.