Hierarchical Heterostructure Engineering of Layered Double Hydroxides on Nickel Sulfides Heteronanowire Arrays as Efficient Cathode for Alkaline Aqueous Zinc Batteries

Abstract Aqueous alkaline rechargeable nickel‐zinc (Ni–Zn) batteries possess great potential for large‐scale energy storage systems because of their high output voltage, cheap cost, and intrinsic safety. However, the practical applicability of Ni–Zn batteries has been limited by traditional Ni‐based cathodes with low capacity and poor cycle stability. Rational design of electrode structure and composition is highly desired but still significantly challenging. Herein, uniform self‐supported hierarchical heterostructure composites interacting NiCo‐layered double hydroxide with 1D nickel sulfides heteronanowire rooted on Ni foam (NF\Ni 3 S 2 /NiS@NiCo‐LDH) are successfully developed by a hydrothermal sulfurization‐electrodeposition process. The self‐supported 3D hierarchical heterostructured composites nanoarray provides abundant reactive sites, rapid ion diffusion channels, and fast electron transfer routes, as well as strong structural stability. More significantly, the strong interfacial charge transfer between Ni 3 S 2 /NiS heteronanowire and NiCo‐LDH effectively modifies the electronic structure of the composites and thereby improving the reaction kinetics. Consequently, the NF\Ni 3 S 2 /NiS@NiCo‐LDH electrode presents a superior capacity of 434.5 mAh g −1 (1.73 mAh cm −2 ) at 3 mA cm −2 . In addition, the fabricated NF\Ni 3 S 2 /NiS@NiCo‐LDH//Zn battery can offer a maximal energy density and power density as large as 556.3 Wh kg −1 and 26.3 kW kg −1 , respectively, as well as an exceptional cycling performance.