Thiosalicylic‐Acid‐Mediated Coordination Structure of Nickel Center via Thermodynamic Modulation for Aqueous Ni–Zn Batteries

Abstract Uniquely functional nanocomplexes with rich coordination environments are critical in energy storage. However, the construction of structurally versatile nanocomplexes remains challenging. In this study, a nickel‐based complex with structural variations is designed via thermodynamic modulation using a dual‐ligand synthesis strategy. A nickel‐based nanomaterial (NiSA‐SSA‐160) with a large specific surface area is synthesized around the competing coordination of the host and guest molecules that differ in terms of the chemical properties of the O and S elements. Concurrently, the coordination environment of NiSA‐SSA‐160 is investigated via X‐ray absorption fine structure spectroscopy. The thiol functional groups synergistically induced an electron‐rich Ni structure, thus increasing the electron density of the central atom. The electrochemical performance of an assembled NiSA‐SSA‐160//Zn@CC battery is shown to improve significantly, with a maximum energy density of 0.54 mWh cm⁻² and a peak power density of 49.49 mW cm⁻². This study provides a new perspective regarding coordination transformations and offers an idea for the design of functionally rich nanomaterials.