Triple Redox–Enabled High‐Entropy Metal–Organic Coordination Driving High‐Performance Aqueous Zinc–Ion Batteries

Abstract High entropy (HE) nanomaterials offer a promising strategy for advancing aqueous zinc–ion batteries (AZIBs). In this study, 1,4‐dihydroxyanthraquinone (1,4‐DHAQ) is employed as an organic ligand to coordinate with multiple metal ions, forming a series of binary to quinary high‐entropy (HE) nanomaterials. All synthesized materials exhibit a layered flower cluster structure. Among them, MnCoNiFeCu‐1,4‐DHAQ (denoted as HE‐1,4‐DHAQ) demonstrates the largest specific surface area and pore volume, along with superior electronic conductivity. HE‐1,4‐DHAQ delivers outstanding electrochemical performance, maintaining a high specific capacity of 222.6 mAh·g −1 after 150 cycles at a current density of 0.3 A·g −1 . A combination of in situ powder X‐ray diffraction, ultraviolet and visible spectrophotometry, and Fourier transform infrared, together with ex situ X‐ray photoelectron spectroscopy and elemental mapping, is employed to comprehensively elucidate the structural evolution and reaction mechanisms during cycling. The results reveal that HE‐1,4‐DHAQ exhibits excellent structural stability and a highly reversible Zn 2+ insertion/extraction mechanism. Moreover, the involvement of three active centers, namely the ─OH groups on the ligand, Mn, and Cu, is confirmed. Notably, HE‐1,4‐DHAQ has been applied as a cathode in soft‐pack batteries, gel electrolyte, and screen‐printed devices, demonstrating strong potential for energy storage and flexible electronics.