2D Mesoporous Naphthalene‐Based Conductive Heteroarchitectures toward Long‐Life, High‐Capacity Zinc‐Iodine Batteries

Abstract Nowadays, rechargeable aqueous zinc‐iodine batteries have attracted extensive attention due to their low cost, high safety, and high theoretical capacity. However, the poor electrical conductivity of iodine and the shuttling effect of soluble polyiodide ions impose an insurmountable constraint on their performance. Here, a facile soft‐hard‐templated co‐assembly strategy is proposed to fabricate naphthalene‐based heteroarchitectured conductive nanosheets with ordered mesopore arrays (≈10 nm), uniform thickness (24.5 nm), high specific surface area (221.5 m 2 g −1 ), and good electronic conductivity (3.9 × 10 −3 S cm −1 ). Density function theory calculation and systematic experimental results show that the complementary combination of the 2D polar semiconducting polymer chains and conductive carbon framework enables the highly efficient immobilization of iodine and then constrains their shuttling effect through strong physicochemical interactions. Accordingly, the resultant zinc‐iodine batteries deliver a high specific capacity of 271.4 mAh g −1 , excellent rate capability, and impressive long‐term cycling stability (35 000 cycles at a high current density of 10 A g −1 ), superior to most of the previous reports. This study opens new venues for rationally constructing heteroarchitectured porous materials for energy storage applications.