Activating Selenium Cathode Chemistry for Aqueous Zinc‐Ion Batteries

Abstract Aqueous rechargeable zinc‐ion batteries (ARZIBs) are a promising next‐generation energy‐storage device by virtue of the superior safety and low cost of both the aqueous electrolyte and zinc‐metal anode. However, their development is hindered by the lack of suitable cathodes with high volumetric capacity that can provide both lightweight and compact size. Herein, a novel cathode chemistry based on amorphous Se doped with transition metal Ru that mitigates the resistive surface layer produced by the side reactions between the Se cathode and aqueous electrolyte is reported. This improvement can permit high volumetric capacity in this system. Distinct from the conventional conversion mechanisms between Se and ZnSe in Se||Zn cells, this strategy realizes synchronous proton and Zn ²⁺ intercalation/deintercalation in the Ru‐doped amorphous Se||Zn half cells. Moreover, an unanticipated Zn ²⁺ deposition/stripping process in this system further contributes to the superior electrochemical performance of this new cathode chemistry. Consequently, the Ru‐doped amorphous Se||Zn half cells are found to deliver a record‐high capacity of 721 mAh g ⁻¹ /3472 mAh cm ⁻³ , and superior cycling stability of over 800 cycles with only 0.015% capacity decay per cycle. This reported work opens the door for new chemistries that can further improve the gravimetric and volumetric capacity of ARZIBs.