Efficient Electron Injection into Graphullerene Enables Reversible NaC₂ Sodium Storage

Abstract

Sodium-ion batteries are emerging as promising alternatives to conventional lithium-based technology, offering solutions to challenges in large-scale grid storage. However, the capacity of conventional graphite-based anodes for storing Na-ions is inherently limited by suboptimal thermodynamic interactions and irreversible structural changes that occur in the anode during charge−discharge cycles. Herein, we present a computational design that explores the potential of graphullerene, a twodimensional framework with interconnected fullerene moieties, for the reversible storage of Na-ions. A unique aspect of this design is the electron injection capacity into the graphullerene anode, reaching 15 electrons per fullerene moiety, which is the highest limit to date. This advancement enables large-scale Na-ion storage up to the stoichiometry of NaC 2 , exhibiting specific capacity of 551 mAhg −1 and averaged open circuit voltage of 0.18 V vs Na/Na + . In addition, the multilayered arrangement of stored Na-ions enhances the Na-ion diffusivity on the graphullerene surface, leading to rapid insertion and extraction kinetics. Thus, raising the electron injection limit offers a promising strategy to transform carbon-based anodes into suitable candidates for reversible Na-ion storage, without relying on artificial defect introduction or doping.