This work reports the facile synthesis of nonaqueous zinc‐ion conducting polymer electrolyte (ZIP) membranes using an ultraviolet (UV)‐light‐induced photopolymerization technique, with room temperature (RT) ionic conductivity values in the order of 10−3 S cm−1. The ZIP membranes demonstrate excellent physicochemical and electrochemical properties, including an electrochemical stability window of >2.4 V versus Zn|Zn2+ and dendrite‐free plating/stripping processes in symmetric Zn||Zn cells. Besides, a UV‐polymerization‐assisted in situ process is developed to produce ZIP (abbreviated i‐ZIP), which is adopted for the first time to fabricate a nonaqueous zinc‐metal polymer battery (ZMPB; VOPO4|i‐ZIP|Zn) and zinc‐metal hybrid polymer supercapacitor (ZMPS; activated carbon|i‐ZIP|Zn) cells. The VOPO4 cathode employed in ZMPB possesses a layered morphology, exhibiting a high average operating voltage of ≈1.2 V. As compared to the conventional polymer cell assembling approach using the ex situ process, the in situ process is simple and it enhances the overall electrochemical performance, which enables the widespread intrusion of ZMPBs and ZMPSs into the application domain. Indeed, considering the promising aspects of the proposed ZIP and its easy processability, this work opens up a new direction for the emergence of the zinc‐based energy storage technologies.

Solid-state rechargeable zinc–air batteries (ZABs) are gaining interest as a class of portable clean energy technology due to their advantages such as high theoretical energy density, intrinsic safety, and low cost. It is expected that an appropriately triple-phase boundary (TPB) engineered, bifunctional oxygen reaction (OER and ORR) electrocatalyst at the air–electrode of ZABs can redefine the performance characteristics of these systems. To explore this possibility, an electrode material consisting of manganese–cobalt-based bimetallic spinel oxide (MnCo2O4)-supported nitrogen-doped entangled graphene (MnCo2O4/NEGF) with multiple active sites responsible for facilitating both OER and ORR has been prepared. The porous 3D graphitic support significantly affects the bifunctional oxygen reaction kinetics and helps the system display a remarkable catalytic performance. The air electrode consisting of the MnCo2O4/NEGF catalyst coated over the gas diffusion layer (GDL) ensures the effective TPB, and this feature works in favor of the rechargeable ZAB system under the charging and discharging modes. As an important structural and functional attribute of the electrocatalyst, the porosity and nitrogen doping in the 3D conducting support play a decisive aspect in controlling the surface wettability (hydrophilicity/hydrophobicity) of the air electrode. The fabricated solid-state rechargeable ZAB device with the developed electrode displayed a maximum peak power density of 202 mW cm–2, which is significantly improved as compared to the one based on the Pt/C + RuO2 standard catalyst pair (124 mW cm–2). The solid-state device which displayed an initial charge–discharge voltage gap of only 0.7 V at 10 mA cm–2 showed only a small increment of 86 mV after 50 h.

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Rechargeable batteries consisting of a Zn metal anode and a suitable cathode coupled with a Zn2+ion-conducting electrolyte are recently emerging as promising energy storage devices for stationary applications. However, the...