Investigation of the temperature effect on the lithium-based energy storage system {LiBF₄ + γ-butyrolactone} using the molecular dynamics approach and the DFT method

The growing consumer interest in electric vehicles and portable electronic devices powered by renewable and sustainable energy sources underscores the urgent need to address the global energy crisis and the associated environmental challenges. Rechargeable batteries, as essential components of electrochemical energy storage systems, are at the forefront of intensive design efforts aimed at enhancing performance while reducing both environmental impact and production costs. In this study, we employed two complementary molecular simulation approaches. The first is a classical molecular dynamics (MD) method, utilizing advanced numerical techniques to integrate the equations of motion with the OPLS-AA force field. The second is a quantum mechanical approach based on density functional theory (DFT), with calculations carried out using the ORCA software package. These calculations employed the B3LYP-D3 functional in conjunction with various basis sets, including def2-TZVP, 6-31G(d), and 6-311++G(d,p). Solvent effects were modeled using the conductor-like polarizable continuum model (CPCM). The resulting computational framework enabled a comprehensive investigation of the thermodynamic, electronic, structural, dynamic, and dielectric properties of the {LiBF₄ - GBL} energy system over a broad temperature range (298.15–373.15 K). The insights gained from the MD and DFT simulations contribute significantly to the development of next-generation lithium-based batteries and advance the progress of sustainable energy storage technologies.