ArXiv · 2026
In this work, we combine first-principles calculations, ab initio molecular dynamics (AIMD), and machine-learning-interatomic-potential molecular dynamics (MLIP-MD) to investigate lithium storage and transport in two-dimensional Cu₈B₁₄, including an experimentally identified line-defect configuration. Pristine Cu₈B₁₄ remains metallic upon lithiation and exhibits favourable Li adsorption, a single-surface theoretical capacity of 427 mAh g⁻¹, and an average open-circuit voltage of approximately 0.53 V. The lowest Li migration barrier on the pristine surface is 0.32 eV. The line-defected structure retains a capacity of approximately 400 mAh g⁻¹ while reducing the local migration barrier to 0.21 eV. To access Li dynamics beyond the picosecond time scale of AIMD, a pretrained MACE-MP-0 model was fine-tuned against system-specific DFT energies and forces and employed in nanosecond-scale simulations from 400 to 600 K. Both pristine and line-defected lithiated monolayers remain structurally stable over this temperature range. At 400 K, the line-defected system exhibits a higher in-plane Li tracer diffusivity (3.97×10⁻⁵~cm²~s⁻¹) than the pristine monolayer (2.50×10⁻⁵~cm²~s⁻¹), whereas the pristine system becomes more diffusive at 500 and 600 K. Arrhenius analysis yields effective activation energies of 0.147 and 0.225 eV for the line-defected and pristine systems, respectively. These results show that the line defect modifies the Li-transport landscape and its temperature dependence rather than uniformly enhancing long-range diffusion, while preserving competitive Li-storage capacity and structural stability.
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