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Abstract

Azo-dye polymers, characterized by reversible –N=N– redox units, have recently emerged as promising organic cathode materials for aqueous zinc-ion batteries (ZIBs) owing to their structural tunability, environmental compatibility, and multi-electron storage capability. This review provides a critical and mechanism-oriented analysis of recent progress in azo-polymer cathodes, with particular emphasis on molecular design strategies, structure-property-performance relationships, and Zn2+ storage mechanisms. The influence of polymer architecture (linear, conjugated, and cross-linked), functional group engineering, and hybrid composite formation on electrochemical metrics, including capacity, voltage window, rate capability, and cycling stability are systematically compared. Beyond summarizing reported performances, this review identifies key structure-driven limitations-such as solubility, conductivity, and voltage constraints and evaluates the effectiveness of current material-engineering approaches to overcome them. Finally, forward-looking perspectives on the rational design of next-generation azo-polymer cathodes, highlighting opportunities in conjugated networks, multifunctional redox systems, and sustainable synthesis routes, have been explored, thereby providing new insights to guide future development of high-performance organic ZIBs.

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