Hybrid Metal–Organic Framework‐Derived Dual Active Site Catalysts Enabling Surface‐Enriched Cathode and Modified Zinc Anode for Long‐Life Zinc–Air Batteries

ABSTRACT The surface modification of zinc anodes and the development of effective cathode dual‐functional oxygen electrocatalysts remain of paramount interest for enhancing the cycle life of rechargeable zinc‐air batteries. The present work provides a sustainable synthesis of CoNi‐based composites that can be used as cathode and anode side catalysts in Zn‐air batteries. CoNi‐metals with hybrid‐metal organic frameworks (Hybrid‐MOFs) and MOF‐derived composites from curcumin‐melamine (C‐M) and benzene‐1,3,5‐tricarboxylic acid (BTC) were created for cathode and anode composites using reflux and hydrothermal techniques. In this instance, the cathode composite can be referred to as CoNi‐N‐C after annealing, whereas the anode composite can be referred to as CoNi‐BTC without annealing. Thereafter, the formation of CoNi‐N‐C and CoNi‐BTC composites was confirmed by microscopic, X‐ray photoelectron, and X‐ray diffraction techniques. As a result, structurally tailored CoNi‐N‐C and CoNi‐BTC composites perform efficiently in electrochemical processes such as oxygen evolution/reduction reactions (OER/ORR) and energy conversion devices (Zn‐air battery). Primarily, the CoNi‐N‐C catalyst exhibits the lowest overpotential (E i = 10 = 1.48 V) and better half‐wave potential (E 1/2 = 0.781 V) in OER/ORR reactions; secondary CoNi‐BTC composites coated on the Zn anode have the highest specific capacity (756.3 mA h g zn −1 ) and 1000‐cycle charge–discharge stability in Zn‐air batteries.