Synergistic behavior of epoxidized natural rubber grafted di(ethylene glycol) methyl ether methacrylate-based solid polymer electrolytes: Experimental and density functional theory (DFT) study
Journal of Industrial and Engineering Chemistry, vol.158, pp.626-646, 2026 (SCI-Expanded, Scopus)
- Publication Type: Article / Article
- Volume: 158
- Publication Date: 2026
- Doi Number: 10.1016/j.jiec.2025.11.038
- Journal Name: Journal of Industrial and Engineering Chemistry
- Journal Indexes: Science Citation Index Expanded (SCI-EXPANDED), Scopus, Chemical Abstracts Core, Compendex, INSPEC
- Page Numbers: pp.626-646
- Keywords: Density functional theory, Epoxidized natural rubber, In situ UV curing, Ion transport, Molecular structure, Solid polymer electrolytes
- Erciyes University Affiliated: No
Abstract
Epoxidized natural rubber (ENR) is a sustainable, cost-effective host for polymer electrolytes due to its environmental compatibility and film-forming ability. In this work, solid polymer electrolytes (SPEs) were prepared by grafting di(ethylene glycol) methyl ether methacrylate (DEGMEM) onto ENR (ENR- g -DEGMEM) and incorporating LiTFSI via UV curing. Structural analysis confirmed efficient grafting (∼61 %), enhancing thermal stability and ionic conductivity. The optimized ENR- g -DEGMEM SPE with 25 wt% LiTFSI achieved a room-temperature ionic conductivity of 1.4 × 10−6 S cm−1 several orders of magnitude higher than neat ENR (10−11 S cm−1). Ion transport followed Arrhenius-type behavior, indicating efficient mobility, while the lithium-ion transference number remained low (∼3%) due to ion pairing. Complementary density functional theory (DFT) calculations provided molecular-level insights into structural, vibrational, and electronic features of ENR- g -DEGMEM and its LiTFSI complexes. Natural Bond Orbital (NBO)-derived donor–acceptor interactions and moderate stabilization energies (∼10.6 kcal/mol) revealed limited Li+ coordination and linked polymer rigidity and orbital distribution to the observed ionic transport and electrochemical stability, coherently explaining FTIR and conductivity trends. These results demonstrate the potential of ENR- g -DEGMEM as a sustainable, high-performance SPE platform and highlight the value of combining experimental and theoretical approaches to guide the rational design of next-generation lithium-ion battery (LIB) materials.