Decoupling Electrochromism and Energy Storage for Flexible Quasi-Solid-State Aqueous Electrochromic Batteries with High Energy Density

Currently, reported aqueous electrochromic batteries (ECBs) show only limited capacity with insufficient energy density and power density. Such a limitation is naturally imposed by the rationale that the cathode of ECBs stores charge by an ion intercalation/deintercalation mechanism, where the inherent inhibition of ion diffusion and structural collapse of cathode materials through repetitive charge/discharge cycles lead to low areal capacity and unsatisfactory electrochemical performance with short lifetime. Herein, we decouple the dual functions of electrochromism and energy storage in conventional cathodes of ECBs by introducing a polyaniline/triiodide composite cathode that is in situ formed by direct electrolysis of an iodide-based quasi-solid-state aqueous electrolyte during charging. When paired with a zinc metal anode, the composite cathode can synergistically utilize the electrochromic property of polyaniline, the high-efficiency energy storage of the Zn-I₂ system, as well as the effective anchorage of polyiodide by polyaniline to suppress the shuttle effect of triiodide. By selecting 1-butyl-3-methylimidazolium ion (BMI⁺) as the cation, a liquid-solid cathode/quasi-solid-state electrolyte interface can be achieved to facilitate the interfacial charge transfer, rendering quasi-solid-state aqueous electrochromic batteries with a high areal capacity of 1363 μAh cm^-2, energy density of 1650 μWh cm^-2, and power density of 5186 μW cm^-2.