Computational tools for studying the atomic and molecular structures of complex systems are very useful. This work uses the first principle method to investigate the structural and optoelectronic properties of a polyethylene oxide (PEO)-based solid polymer electrolyte including lithium salt (LiFSI) as an ion-conducting species. Density functional theory (DFT) has been used for the analysis of electrolyte conducting properties. The band gap of the polymer electrolyte (PEO)₈-LiFSI system has been quantitatively examined by the HOMO–LUMO concept. It is verified that (PEO)₈ exhibits insulator properties with a wide band gap of 6.27 eV, whereas the bandgap of (PEO)₈-LiFSI slightly drops to 6.00 eV. These findings suggest that the current polymer electrolyte system (PEO)₈-LiFSI could be a viable option for the electrolyte in next-generation energy storage devices. The low electronic conductivity, confirmed through electronic analysis, is essential in maintaining high safety standards by preventing electronic leakage, which could lead to short circuits in solid-state batteries. Raman and IR spectra reveal crucial interactions between the Li⁺ ions and the PEO matrix, specifically the coordination of Li⁺ with the ether oxygen of PEO and the FSI⁻ anion. These interactions significantly affect the ionic conductivity by influencing ion transport mechanisms in the electrolyte. NMR analysis provides detailed insights about the (PEO)₈ and (PEO)₈-LiFSI structures that in turn help to estimate the mobility and dynamics of lithium ions within the polymer matrix. The UV–vis-nir analysis offers insights into the optical and electronic properties. This is important for understanding the lifetime and reliability of the electrolyte in solid-state battery applications. Therefore, the results collectively provide a comprehensive understanding of the (PEO)₈-LiFSI system, for using it as a solid polymer electrolyte for next-generation solid-state batteries.

用于研究复杂系统的原子和分子结构的计算工具非常有用。这项工作使用第一原理方法研究了基于聚环氧乙烷 （PEO） 的固体聚合物电解质（包括锂盐 （LiFSI） 作为离子导电物质）的结构和光电性质。密度泛函理论 （DFT） 已用于分析电解质导电特性。聚合物电解质 （PEO）8-LiFSI 系统的带隙已通过 HOMO-LUMO 概念进行了定量检查。经验证，（PEO）₈ 表现出 6.27 eV 宽禁带的绝缘体特性，而 （PEO）8-LiFSI 的带隙略微下降至 6.00 eV。这些发现表明，当前的聚合物电解质系统 （PEO）8-LiFSI 可能是下一代储能设备中电解质的可行选择。通过电子分析证实的低电子电导率对于通过防止电子泄漏来保持高安全标准至关重要，电子泄漏可能导致固态电池短路。拉曼光谱和红外光谱揭示了 Li⁺ 离子和 PEO 基体之间的关键相互作用，特别是 Li⁺ 与 PEO 的醚氧和 FSI⁻ 阴离子的配位。这些相互作用通过影响电解质中的离子传输机制来显着影响离子电导率。NMR 分析提供了有关 （PEO）₈ 和 （PEO）8-LiFSI 结构的详细见解，这反过来又有助于估计聚合物基质中锂离子的迁移率和动力学。UV-vis-nir 分析提供了对光学和电子特性的见解。 这对于了解固态电池应用中电解质的寿命和可靠性非常重要。因此，这些结果共同提供了对 （PEO）8-LiFSI 系统的全面理解，以将其用作下一代固态电池的固体聚合物电解质。