Chaotropic Salt-Aided "Water-In-Organic" Electrolyte for Highly Reversible Zinc-Ion Batteries Across a Wide Temperature Range

Aqueous zinc-ion batteries are promising alternatives to lithium-ion batteries due to their cost-effectiveness and improved safety. However, several challenges, including corrosion, dendrites, and water decomposition at the Zn anode, hinder their performance. Herein, an approach is proposed, that deviates from the conventional design by adding water into a propylene carbonate-based organic electrolyte to prepare a non-flammable "water-in-organic" electrolyte. The chaotropic salt Zn(ClO4)2 exploits the Hofmeister effect to promote the miscibility of immiscible liquid phases. Interactions between propylene carbonate and water restrict water activity and mitigate unfavorable reactions. This electrolyte facilitates preferential Zn (002) deposition and the formation of solid electrolyte interphase. Consequently, the "water-in-organic" electrolyte achieves a 99.5% Coulombic efficiency at 1 mA cm-2 over 1000 cycles in Zn/Cu cells, and constant cycling over 1000 h in Zn/Zn symmetric cells. A Na0.33V2O5/Zn battery exhibits impressive cycling stability with a capacity of 175 mAh g-1 for 800 cycles at 2 A g-1. Additionally, this electrolyte enables sustainable cycling across a wide temperature range from -20 to 50 degrees C. The design of a "water-in-organic" electrolyte employing a chaotropic salt presents a potential strategy for high-performance electrolytes in zinc-ion batteries with a large stability window and a wide temperature range. Inspired by the Hofmeister effect, Zn(ClO4)2 chaotropic salt facilitates the miscibility between water and propylene carbonate to prepare a "water-in-organic" electrolyte. This electrolyte promotes the preferential exposure of the Zn (002) facet and forms a robust inorganic solid electrolyte interphase. The tuned intermolecular interactions within the electrolyte enable the battery to cycle across a wide temperature range.image