ABSTRACT The practical application of zinc metal batteries remains severely impeded by dendritic growth at the electrolyte/electrode interface. A self‐amplifying vicious cycle involving ion depletion and localized electric‐field distortion exacerbates interfacial charge accumulation, leading to the formation of dendrites. This work designs a Lewis acid polymer electrolyte to rectify Zn 2+ transport for disrupting this detrimental cycle. Within this framework, the unsaturated Ti (Lewis acidic) sites on Ti 3 C 2 T x ‐NH 2 ‐O v anchor anions, effectively sieving ions for unrestricted Zn 2+ conduction. Meanwhile, Ti 3 C 2 T x ‐NH 2 ‐O v nanosheets restrict the conformational freedom of the polymer chains (carboxymethyl cellulose and poly (ethylene glycol) diacrylate), while amino functionalization establishes balanced coordination sites within the polymer matrix, collectively constructing well‐aligned Zn 2+ transport channels. This synergistic regulation rectifies Zn 2+ flux, enabling the electrolyte to achieve an ultrahigh Zn 2+ transference number of 0.88 and high ionic conductivity of 6.8 mS cm −1 , even under ultralow liquid content (0.1 µL mg −1 ). The continuous and directional supply of Zn 2+ alleviates local charge accumulation. Zn//Zn cells demonstrate remarkably stable cycling for over 5000 h. Furthermore, full batteries coupled with high mass loading vanadium‐ and iodine‐based cathodes exhibit superior cycling durability. This work provides a novel pathway toward dendrite‐free metal batteries by tailoring ion‐transport features to resolve interfacial failure.
Wang et al. (Mon,) studied this question.