The changes of crosslink density of polyurethanes synthesised with using recycled component. Chemical structure and mechanical properties investigations

This paper aims at the utilisation of glycerolysate (Gly) obtained in polyurethane recycling process by means of crude glycerine, which has in its structure hydroxyl end groups that allow for further processing. Polyurethanes (PUs) were synthesised using prepolymer method with the mixture of neat polyol and glycerolysate, in different ratios, with 4,4-diphenylmethane diisocyanate (MIDI). The prepolymer was subsequently extended using 1,4-butanediol (BD). The incorporation of glycerolysate caused the crosslinking of obtained polyurethane materials. The crosslink density was calculated from swelling measurements by means of Flory and Reimer equation. The effect of recycled component content on the structure, thermal and mechanical properties were investigated by Fourier transform infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), dynamic mechanical analysis (DMA) and mechanical tests, respectively. Morphology was also analysed by atomic force microscopy (AFM). As the content of recycled component increased, the swelling ratio decreased and simultaneously crosslink density increased, resulting in the increase of glass transition and storage modulus at room temperature. Thermomechanical stability, tensile strength, elastic modulus and hardness of PUs also increased with the incorporation of glycerolysate. Although elongation at break decreased, the recoverable deformation increased with the content of glycerolysate. Morphology reveals the transition from a microphase-separated microstructure to an interconnected hard segments domain structure with the incorporation of glycerolysate. These materials can be applied as protective coatings.