Reconfiguring graphene for high-performance metal-ion battery anodes

Abstract Reconfiguring structures in materials is one of the most important building approaches in new material design. The atomically precise control of reconfiguration of two-dimensional (2D) carbon-based materials reshapes their properties for engineering applications. Herein, by employing density functional theory and tight-binding modeling, we reconfigured atomically precise structure in graphene and proposed a new 2D carbon allotrope Θ-graphene. The reconfiguring procedure adopted was realized in experiments using an electron beam. It exhibits semiconductor features with a bandgap of 0.58 eV, and is extendable to semimetal or metal. Mechanically-induced directional-dependent topological node line states are formed and their origin is the breaking of the geometrical symmetry. The reconfiguring procedure reshapes the adsorption and diffusion properties of Θ-graphene, promoting its storage capacities for metal ions (876.65/1275.12/956.34 mA h/g for Li/Na/K- ion batteries) and lowing its metal ion-diffusion energy barriers (≤ 0.48 eV) and lowing its average open circuit voltages (≤ 0.60 V). The transition from semiconductor to metal with metal ions introduced improves its high electronic conductivity, which could be beneficial to the fast charge/discharge rates. Our results show that the reconfigured structure in graphene reshapes its properties, bringing it numerous promising engineering applications such as in metal-ion batteries and in nanoelectronic devices and in energy storage. This work provides a new channel for materials design and innovation by combining the reconfiguring strategy and the structure-property-application relationship, and opens up a new strategy to extend the applications of low-dimensional materials such as graphene and to promote their application performance.