Interfacial Engineering of Porous Poly(p‐Aminoazobenzene) toward Stable Zn Anodes

Aqueous zinc‐ion batteries (AZIBs) have recently emerged as a promising candidate for large‐scale energy storage applications, primarily due to their nonflammable nature, low production costs, and satisfactory specific energy. Nevertheless, their cycle stability is significantly limited by the inevitable formation of Zn dendrites and undesirable water‐induced parasitic reactions. To tackle these challenges, a porous poly(p‐aminoazobenzene) (PPAAB) interfacial protective layer is developed for regulating the transport and deposition behavior of Zn 2+ ions. The engineered PPAAB coating, functionalized with polar moieties (NH and N), exhibits strong hydrophilic characteristics that enable controlled Zn 2+ ion flux and deposition behavior via a selective ion‐confinement mechanism. Consequently, the Zn@PPAAB anode exhibits improved interfacial dynamics and a low nucleation overpotential, demonstrating stable plating/stripping behavior. When paired with a NaV 3 O 8 (NVO) cathode, the NVO||PPAAB@Zn cell showcases impressive capacity retention, maintaining 84% of its capacity after 1100 cycles at 1.0 A g −1 . This study not only advances accessible interface engineering but also provides deeper mechanistic insights into Zn anode behavior, paving the way for enhanced AZIBs.