Intercatenation weaves MOFs with conductive networks as iodine hosts for zinc-iodine batteries

With large specific surface area, structural diversity and porosity, metal–organic frameworks (MOFs) have emerged as a highly attractive candidate in energy storage field, yet the limited electrical conductivity hinders their further application. Herein, we developed an intercatenation approach to weave MOFs materials with conductive networks by transforming the reactive functional groups ([sbnd]NH₂) into interpenetrated polypyrrole chains. The interlocked conductive network opened a new charge transport pathway through the MOFs, and thus endowed them with excellent conductivity and electrochemical activity. Moreover, during the oxidative polymerization of MIL-68-Py, not only are numerous pores formed within the In-MOF structure, but cracks with specific orientations are also induced. The derived MIL-68-PPy served as an iodine carrier demonstrated a capacity of 209 mAh g⁻¹ at a current density of 0.5 A/g in aqueous zinc-iodine batteries, and after 1000 cycles, its specific capacity remains 1.12 times that of MIL-68-NH₂. This work not only provides new insights for MOFs conductivity, but also lays the groundwork for enhancing the performance of MOFs materials towards practical applications.