Puffing Up Energetic Metal–Organic Frameworks to Large Carbon Networks with Hierarchical Porosity and Atomically Dispersed Metal Sites

Abstract Large carbon networks featuring hierarchical pores and atomically dispersed metal sites (ADMSs) are ideal materials for energy storage and conversion due to the spatially continuous conductive networks and highly active ADMSs. However, it is a challenge to synthesize such ADMS‐decorated carbon networks. Here, an innovative fusion‐foaming methodology is presented in which energetic metal–organic framework (EMOF) nanoparticles are puffed up to submillimeter‐scaled ADMS‐decorated carbon networks via a one‐step pyrolysis. Their extraordinary catalytic performance towards oxygen reduction reaction verifies the practicability of this synthetic approach. Moreover, this approach can be readily applicable to a wide range of unexplored EMOFs, expanding scopes for future materials design.