Two-Dimensional Biphenylene-Based Carbon Allotrope Family with High Potassium Storage Ability

The development of new carbon materials with novel properties and excellent applications is essential and urgent in many fields, such as potassium-ion batteries (PIBs). In this study, a family of 30 two-dimensional biphenylene carbon allotropes (2D-BCAs) have been systematically extended in theory. The energies of these allotropes are slightly higher than that of graphene, which can be well described by a quantitative energy equation. The 2D-BCAs show high synthesizability consistent with the experimental biphenylene network via “HF-zipping” reactions. The 2D-BCAs are metallic or semimetallic. Six representative 2D-BCAs exhibit good lattice dynamical and thermal stability, excellent anisotropic mechanical properties, and ORR catalytic activity. Moreover, the selected 2D-BCAs demonstrate ultrahigh theoretical potassium-storage capacities of 1116–1489 mAh·g^–1, low migration barriers of 0.03–0.22 eV, and low open-circuit voltages of 1.10–0.02 V. The remarkable properties render 2D-BCAs as promising anode materials in PIBs, electrocatalysts, and conductors in electronics and iontronics.