LAUSR

Abstract Three-dimensional porous carbon materials play a significant role in gas separation and energy storage. However, their low performances in energy storage hamper their applications. Herein, we propose a new possible category of carbon honeycomb (CHC), i.e. CHCs with asymmetrical channels (denoted as asymmetrical CHCs), to increase their performance. As an example, by cross-linking graphene sheet with sp3–hybridized carbon chains, we prepare a new 3D porous asymmetrical CHC, i.e. bco-C24. It is dynamically, thermally, and mechanically stable. Our first-principles calculations and tight binding results demonstrate that it possesses a significant electronic band structure of Dirac nodal lines, which are ascribed to the px and py orbitals of α carbon atoms in the graphene ribbons that have both α and β carbon atoms. It provides high carrier mobility between 7.98 × 105 and 9.99 × 105 m/s. It has high theoretical capacities (743.8/495.9/991.8/743.8 mA h/g), low diffusion barriers (0.077/0.032/0.117/0.169 eV), low average voltages, and negligible volume changes for Na/K/Ca/Li-ion batteries. This study not only constructs a new concept of asymmetrical CHCs and provides a strategy of cross-linking graphene sheets to create its sample structures, but also suggests new carriers for ion storage in the superior next generation metal-ion battery anodes.