Boosting zinc-ion storage performance by interlayer chemistry modulation on an organic-inorganic hybrid cathode

Aqueous zinc-ion batteries (AZIBs) have triggered a surge of scientific research due to the unique merits of high safety, volumetric specific capacity, and environmental benignity. However, the implementation of this technology is still plagued by the lack of high-performance cathodes that can output high energy density and exceptional cycle life and inadequate Zn reversibility. Here, an organic-inorganic hybrid cathode based on a poly(3,4-ethylenedioxythiophene) (PEDOT) intercalated hydrated vanadium oxide (denoted PVO), which delivers an ultrahigh discharge capacity of 513.1 mAh g^-1 (0.5 A g^-1) and an ultra-stable cycle with 95.3 % capacity retention and approximately 100 % Coulombic efficiency over 2000 cycles (20 A g^-1), is developed. Combining substantive measurements and theoretical calculations, it is demonstrated that favorable structural features with expanded interlayer galleries and robust architecture are believed to be responsible for the enhanced electrochemical performance, which can be further boosted by the improved Zn reversibility because of the introduction of maltitol electrolyte additive. This work provides a new attempt to achieve organic-inorganic composites for high-performance cathode materials of AZIBs and new insights into the charge storage behavior under the synergistic regulation of bilateral interfaces.