Regulating Zn ²⁺ Diffusion Dynamics in Aqueous  Zn‐Ion Batteries by Tweaking Coordination Sites in Organic–Inorganic Hybrid Cathode

Functional quinone units with π‐conjugated frameworks are promising organic cathode materials for aqueous zinc‐ion batteries (AZIBs). The critical drawbacks of quinone unit–containing electrodes are poor electronic conductivity and dissolution during electrochemical cycling, which poses a limitation in their practical deployment. Herein, we report a rational strategy of constructing organic–inorganic hybrid cathode that synergistically overcomes the intrinsic drawbacks including dissolution, limited conductivity, and sluggish electrochemical kinetics. In situ grown C─S─C enriched copolymer of quinone unit and thiophene (Pbz‐Th) on nitrogen‐doped siliconoxycarbide (g‐(C/N)SiO) is explored as a cathode material in AZIB. Mechanistic investigations led by spectroscopic analysis reveal that oxygen and sulfur moieties in the copolymer participate in Zn 2+ coordination, enabling reversible Zn 2+ storage and enhanced reaction kinetics, whereas g‐(C/N)SiO exhibits a fast and reversible pseudocapacitive charge‐storage process. Notably, the C─S units within the copolymer and the auxiliary active sites of g‐(C/N)SiO contribute to reversible surface redox processes, leading to enhanced capacitance and improved cycling stability. The resulting Pbz‐Th@g‐(C/N)SiO cell delivers a maximum discharge capacity of 181 mAhg −1 at 0.05 Ag −1 with 97% Coulombic efficiency and capacity retention of 90% over 500 cycles at 1 Ag −1 . Integrating redox‐active organic motifs with a conductive g‐(C/N)SiO scaffold addresses dissolution, enhances electronic transport, and improves interfacial kinetics.