Nitrogen‐Doped Carbon Networks with Consecutive Conductive Pathways from a Facile Competitive Carbonization‐Etching Strategy for High‐Performance Energy Storage

Abstract Recently, new carbonization strategies for synthesizing structure‐controlled and high‐performance carbon electrode materials have attracted great attentions in the field of energy storage and conversion. Here a competitive carbonization‐etching strategy to prepare nitrogen‐doped carbon polyhedron@carbon nanosheet (NCP@CNS) hybrids derived from zeolitic imidazolate framework‐8 is presented. Consecutive conductive networks are constructed in the NCP@CNS hybrids during a unique carbonization‐etching pyrolysis, where a competition between the formation of NCPs and CNSs exists. When the NCP@CNS hybrids are employed as supercapacitor electrodes, their hierarchically porous NCPs serve as ion‐buffering reservoirs for offering fast ion transport channels, and the CNSs within hybrids not only link the NCPs together to build electron transfer pathways but also restrict the volume fluctuation of electrodes during charging and discharging process. As a result, the as‐fabricated NCP@CNS electrode displays excellent electrochemical performances including a superior specific capacitance of 320 F g⁻¹, a high energy density of 22.2 W h kg⁻¹ (5.6 W h kg⁻¹ for symmetric device), and a long cycle life with capacitance retention of ≈101.8% after 5000 cycles. This study opens an encouraging avenue toward the tailored synthesis of metal‐organic frameworks (MOFs)‐derived carbon electrodes for renewable energy storage applications and devices.