Intelligent Chip-Controlled Smart Oxygen Electrodes for Constructing Rechargeable Zinc–Air Batteries with Excellent Energy Efficiency and Durability

High-performance rechargeable oxygen electrodes are key devices for realizing high-specific-energy batteries, including zinc–air and lithium–air batteries. However, these batteries have severe problems of premature decay in energy efficiency by serious corrosion, wide charge–discharge gap, and catalyst peeling off. Herein, we propose a “smart dual-oxygen electrode”, which is composed of an intelligent switch control module + heterostructured Fe1Ni3-LDH/PNCNF OER catalysis electrode layer + ion conductive | electronic insulating membrane + Pt/C ORR catalysis electrode layer, where OER and ORR layers are automatically switched by the intelligent switch control module as required. This smart dual-oxygen electrode offers an ultralow energy efficiency decay rate of 0.0067% after 300 cycles during cycling, much lower than that of the commercial Pt/C electrode (1.82%). The assembled rechargeable zinc–air battery (RZAB) displays a super narrow voltage gap and achieves a high energy efficiency of 71.7%, far higher than that of the existing RZABs (about 50%). Therefore, this strategy provides a complete solution for designing various high-performance metal–air secondary batteries.