Creating Mesopores in Two-Dimensional Conductive Metal–Organic Frameworks for Enhanced Electrochemical Capacitive Performance

Abstract Two-dimensional conductive metal–organic frameworks (2D c-MOFs), such as Ni3(2,3,6,7,10,11-hexaiminotriphenylene)2 (Ni3(HITP)2), are promising active materials for electrochemical energy storage due to their intrinsic conductivity and well-defined porous structures. However, their predominantly microporous nature limits ionic transport, leading to poor performance at fast charging rates. Herein, we report a soft-template strategy using a symmetric triblock copolymer to introduce mesoporosity into Ni3(HITP)2. The resulting materials exhibit preserved crystallinity and hierarchical pore structures, with mesopores of 3–5 nm confirmed by both nitrogen sorption and transmission electron microscopy. This work demonstrates the creation of mesopores in 2D c-MOFs via a soft-template approach. The mesopores of Ni3(HITP)2 facilitate the mass transfer of ions and thus enhance the rate capability for the application in supercapacitors, highlighting soft-template engineering as an effective strategy for tuning pore structure and electrochemical performance.