Diffusion of Alkaline Metals in Two-Dimensional β1-ScSi2N4 and β2-ScSi2N4 Materials: A First-Principles Investigation

Abstract

The MA₂Z₄ family represents a class of two-dimensional materials renowned for their outstanding mechanical properties and excellent environmental stability. By means of elemental substitution, we designed two novel phases of ScSi₂N₄, namely β₁ and β₂. Their dynamical, thermal, and mechanical stabilities were thoroughly verified through phonon dispersion analysis, ab initio molecular dynamics (AIMD) simulations, and calculations of mechanical parameters such as Young’s modulus and Poisson’s ratio. Electronic structure analysis using both PBE and HSE06 methods further revealed that both the β₁ and β₂ phases exhibit metallic behavior, highlighting their potential for battery-related applications. Based on these outstanding properties, the climbing image nudged elastic band (CI-NEB) method was employed to investigate the diffusion behavior of Li, Na, and K ions on the material surfaces. Both structures demonstrate extremely low diffusion energy barriers (Li: 0.38 eV, Na: 0.22 eV, K: 0.12 eV), indicating rapid ion migration—especially for K—and excellent rate performance. The lowest barrier for K ions (0.12 eV) suggests the fastest diffusion kinetics, making it particularly suitable for high-power potassium-ion batteries. The significantly lower barrier for Na ions (0.22 eV) compared with Li (0.38 eV) implies that both β₁ and β₂ phases may be more favorable for fast-charging/discharging sodium-ion battery applications. First-principles calculations were applied to determine the open-circuit voltage (OCV) of the battery materials. The β₂ phase exhibits a higher OCV in Li/Na systems, while the β₁ phase shows more prominent voltage for K. The results demonstrate that both phases possess high theoretical capacities and suitable OCVs.