The geometry, electronic structure, and chemical reactivity of polycaprolactone (PCL), solid polymer electrolyte (SPE; PCL/LiTFSI), and polymer-in-salt/ionic liquid-based biodegradable gel polymer electrolyte, i.e., ionogel (IG; PCL/LiTFSI/[EMIMDCA]) have been discussed on the basis of quantum chemical density functional theory (DFT) calculations using B3LYP method and LANL2DZ basis set. The interaction of Li⁺-ion with PCL and ionic liquid (IL) has been calculated in terms of electronic structures of clusters of the mixtures of PCL and IL including a Li⁺-ion. The energy values of − 6.76, − 7.02, and − 5.29 eV and − 1.11, − 3.60, and − 3.35 eV were related to HOMO-LUMO orbitals of PCL, SPE, and IG, respectively. The energy gap (\({E}_{{\text{g}}}\)) of the molecular systems are found 5.65 (PCL), 3.41 (SPE), and 1.95 eV (IG), respectively. The migration of the LiTFSI (Li⁺-ion) cation is what causes the lowered band gap (\({E}_{{\text{g}}}\)) of SPE. Finally, the narrowed \({E}_{{\text{g}}}\) of IG demonstrates that IL improves the migration of the LiTFSI cation (Li⁺-ion) across the PCL oxygen atom. The HOMO-LUMO energy levels are used to calculate the global and local chemical descriptors and electrochemical stability windows (ESWs). Mulliken population analysis (MPA) and the surface of the molecular electrostatic potential (MEP) are used to study partial charge analysis.

聚己内酯（PCL）、固体聚合物电解质（SPE；PCL/LiTFSI）和基于盐/离子液体的聚合物可生物降解凝胶聚合物电解质（即离子凝胶（IG；PCL/使用 B3LYP 方法和 LANL2DZ 基组在量子化学密度泛函理论 (DFT) 计算的基础上讨论了 LiTFSI/[EMIMDCA])。已经根据包含Li ^{+离子的PCL和IL混合物的簇的电子结构计算了Li +}离子与PCL和离子液体(IL)的相互作用。- 6.76、- 7.02和- 5.29 eV以及- 1.11、- 3.60和- 3.35 eV的能量值分别与PCL、SPE和IG的HOMO-LUMO轨道相关。分子系统的能隙（\({E}_{{\text{g}}}\) ）分别为 5.65 (PCL)、3.41 (SPE) 和 1.95 eV (IG)。^{LiTFSI (Li +} -ion) 阳离子的迁移是导致SPE带隙 ( \({E}_{{\text{g}}}\)降低的原因。最后，IG 的缩小\({E}_{{\text{g}}}\)表明 IL 改善了 LiTFSI 阳离子（Li ⁺ -离子）穿过 PCL 氧原子的迁移。HOMO-LUMO 能级用于计算全局和局部化学描述符以及电化学稳定性窗口 (ESW)。马利肯布居分析（MPA）和表面分子静电势（MEP）用于研究部分电荷分析。