Synthesis and characterization of linseed oil-derived polyurethane composites via epoxidation and ring-opening pathway: Structure–property relationships and DFT insights
摘要
The environmental toll of petroleum-based plastics, with tensile strengths of 10–20 MPa, includes pollution, greenhouse gas emissions, and crude oil depletion, driving the need for sustainable alternatives. This study established linseed oil (LO), a renewable source rich in polyunsaturated fatty acids, as an exceptional feedstock for polyurethane (PU) biomaterials, surpassing traditional materials. An optimized synthesis route involving epoxidation, ring-opening, and polyaddition with a suitable linker is the conventional route for PU materials. In the current work, hexamethylene diisocyanate (HDI) as a linker and cellulose nanofibers (CNF) as a sustainable filler material were used at an optimized ratio to produce LO-derived polyurethane (LPU) and CNF-reinforced LPU (LPU-CNF) composite sheets. These achieved a tensile strength of 18.95 MPa and a glass transition temperature (Tg) of 220–240°C, outperforming many fossils fuel-derived PUs (Tg 150–200°C). Spectroscopic (FTIR, XPS) and crystallographic (XRD) analyses confirmed their molecular structure and enhanced crystallinity. The high unsaturation of LO enabled robust crosslinking, while CNF reinforcement boosted mechanical and thermal properties, validated by tensile testing, TGA, and DSC. Computational density functional theory (DFT) studies underscored the thermodynamic favorability of the synthesis, reinforcing the stability of LPU-CNF. These biomaterials hold potential for packaging, foams, coatings, adhesives, and biocomposites, supporting the transition to eco-friendly, high-performance alternatives to petroleum-based plastics.