3D nitrogen-doped carbon frameworks with hierarchical pores and graphitic carbon channels for high-performance hybrid energy storages

Abstract

In principle, hybrid energy storages can utilize the advantages of capacitor-type cathodes and battery-type anodes, but their cathode and anode materials still cannot realize a high energy density, fast rechargeable capability, and long-cycle stability. Herein, we report a strategy to synthesize cathode and anode materials as a solution to overcome this challenge. Firstly, 3D nitrogen-doped hierarchical porous graphitic carbon (NHPGC) frameworks were synthesized as cathode materials using Co–Zn mixed metal–organic frameworks (MOFs). A high capacity is achieved due to the abundant nitrogen and micropores produced by the MOF nanocages and evaporation of Zn. Also, fast ion/electron transport channels were derived through the Co-catalyzed hierarchical porosity control and graphitization. Moreover, tin oxide precursors were introduced in NHPGC to form the SnO₂@NHPGC anode. Operando X-ray diffraction revealed that the rescaled subnanoparticles as anodic units facilitated the high capacity during ion insertion-induced rescaling. Besides, the Sn–N bonds endowed the anode with a cycling stability. Furthermore, the NHPGC cathode and SnO₂@NHPGC achieved an ultrahigh energy density (up to 244.5 W h kg⁻¹ for Li and 146.1 W h kg⁻¹ for Na), fast rechargeable capability (up to 93C-rate for Li and 147C-rate for Na) as exhibited by photovoltaic recharge within a minute and a long-cycle stability with ∼100% coulombic efficiency over 10 000 cycles.