Ni Single‐Atom Dual Catalytic Electrodes for Long Life and High Energy Efficiency Zinc‐Iodine Batteries

Abstract Zinc‐iodine batteries (Zn‐I2) are extremely attractive as the safe and cost‐effective scalable energy storage system in the stationary applications. However, the inefficient redox kinetics and “shuttling effect” of iodine species result in unsatisfactory energy efficiency and short cycle life, hindering their commercialization. In this work, Ni single atoms highly dispersed on carbon fibers is designed and synthesized as iodine anchoring sites and dual catalysts for Zn‐I2 batteries, and successfully inhibit the iodine species shuttling and boost dual reaction kinetics. Theoretical calculations indicate that the reinforced d‐p orbital hybridization and charge interaction between Ni single‐atoms and iodine species effectively enhance the confinement of iodine species. Ni single‐atoms also accelerate the iodine conversion reactions with tailored bonding structure of I─I bonds and reduced energy barrier for the dual conversion of iodine species. Consequently, the high‐rate performance (180 mAh g −1 at 3 A g −1 ), cycling stability (capacity retention of 74% after 5900 cycles) and high energy efficiency (90% at 3 A g −1 ) are achieved. The work provides an effective strategy for the development of iodine hosts with high catalytic activity for Zn‐I2 batteries.