Atomic-Scale Modulation of Lithium Metal Electrode Interfaces by Monolayer Graphene: A Molecular Dynamics Study

Graphene, owing to its exceptional mechanical properties and interfacial modulation capability, is considered an ideal material for enhancing the interfacial strength and damage resistance during the fabrication of ultra-thin lithium foils. Although previous studies have demonstrated the reinforcing effects of graphene on lithium metal interfaces, most analyses have been restricted to single-temperature or idealized substrate conditions, lacking systematic investigations under practical, multi-temperature environments. Consequently, the influence of graphene coatings on lithium-ion conductivity and mechanical stability under real thermal conditions remains unclear. To address this gap, we employ LAMMPS-based molecular dynamics simulations to construct atomic-scale models of pristine lithium and graphene-coated lithium (C/Li) interfaces at three representative temperatures. Through comprehensive analyses of dislocation evolution, root-mean-square displacement, frictional response, and lithium-ion diffusion, we find that graphene coatings synergistically alleviate interfacial stress, suppress crack initiation, reduce friction, and enhance ionic conductivity, with these effects being particularly pronounced at elevated temperatures. These findings reveal the coupled mechanical and electrochemical regulation imparted by graphene, providing a theoretical basis for optimizing the structure of next-generation high-performance lithium metal anodes and laying the foundation for advanced interfacial engineering in battery technologies.