Importance of Viscosity Control for Recyclable Reinforced Thermoplastic Composites

Abstract

Thermoplastic composites consisting of a liquid crystalline polymer (LCP) and poly(lactide) (PLA) have the potential to combine good mechanical performance with recyclability and are therefore interesting as strong and sustainable composite materials. The viscoelastic behavior of both the LCP and the PLA is of great importance for the performance of these composites, as they determine the LCP morphology in the composite and play a crucial role in preventing the loss of mechanical performance upon recycling. Though the effect of the matrix viscosity is well-documented in literature, well-controlled systems where the LCP viscosity is tailored are not reported. Therefore, four LCPs, with the same chemical backbone but different molecular weights, are used to produce reinforced LCP-PLA composites. The differences in viscosity of the LCPs and viscosity ratio between the dispersed phase and the matrix of the blends are evident in the resultant composite morphology: in all cases fibrils are formed; however, the diameter increases considerably as the viscosity ratio increases for the higher molar mass LCPs. The fibril diameter ranges from several hundred nanometer to a few micrometer. A typical layered structure in the injection molded composites is observed, where the layer-thickness is influenced by the LCP viscosity. The LCPs are found to effectively reinforce the PLLA matrix, increasing the Young’s modulus by 60% and the maximum stress by 40% for the composite containing 30 wt % of the most viscous LCP. Remarkably, this did not result in an increase in brittleness, effectively increasing the toughness of the composite compared to pure PLLA. The feasible reprocessability of this composite is confirmed, by subjecting it to three reprocessing cycles. The relaxation of the LCPs orientation upon heating is measured via in situ WAXD. We compare the relaxation in an amorphous PLA matrix and in a semicrystalline PLLA matrix with that of the pure LCPs. The matrix viscosity is found to strongly influence the relaxation. For example, in a low viscous amorphous matrix relaxation of the LCP fibrils into droplets dominates the process, whereas a semicrystalline matrix helps in maintaining the fibril morphology and intermolecular orientation of the LCP. In the latter case, the LCPs relax via contraction and coalescence of the polydomain texture and maintains a significant degree of orientation until the PLLA crystals melt and the matrix viscosity decreases. The insights gained in this study on the role of the LCP viscosity on the morphology and performance of thermoplastic composites, as well as the relaxation of LCPs in a matrix, will aid progression toward sustainable and reprocessable LCP reinforced thermoplastic composites.

Highly Tough and Thermally Stable Polylactide Blends Compatibilized with Glycidyl Methacrylate‐Grafted Polypropylene

“…To overcome the shortcomings of PLA, various organic and inorganic fillers have been introduced as reinforcing materials to develop PLA‐dominant blends and composites. [ 5,11–23 ] The stereocomplexation ability of PLA isomers has been also proposed as an effective method for enhancing the thermal and mechanical properties. [ 24,25 ] Some researchers have explored the potential of blending PLA with conventional polymers to improve performance and lower prices by investigating the blends in terms of miscibility, morphology, thermal, and mechanical properties.…”

A integração do conhecimento científico e a produção sustentável de termoplásticos vulcanizados a partir de resíduos de pneus

“…Essas observações são consistentes com estudos anteriores (Ghahramani et al, 2020). A literatura reporta a influência da massa molar na viscosidade de polímeros termoplásticos, sendo observado o aumento da viscosidade com o aumento da massa molar (Kort et al, 2020;Khunprasert et al, 2009;Stadler et al, 2009). O comportamento de fluxo de polímeros com diferentes massas molares e de baixa massa molar exibem comportamento newtoniano, enquanto polímeros de alta massa molar apresentam comportamento pseudoplástico (Agrawal et al, 2022).…”

Strong, transparent composites based on glass‐fiber textile and a polycarbonate–polycaprolactone blend with matching refractive indices

“…Unfortunately, thermosets typically take more than 5 min to cure and resulting products are impossible to recycle (convert into other products) by remelting, limiting their suitability for mass production. In contrast, thermoplastics are promising polymer matrices for transparent composites because they can be produced by injection molding within 1 min and resulting products can be remolded into other objects by remelting 19–22 …”

“…In contrast, thermoplastics are promising polymer matrices for transparent composites because they can be produced by injection molding within 1 min and resulting products can be remolded into other objects by remelting. [19][20][21][22] A refractive index-adjustable thermoplastic matrix can be prepared using a polymer blend and a simple, melt-mixing process; its optical properties are tailored by adjusting its composition. In polymer-blend composites, transparency is reduced by phase separation, crystallization, and the mismatch of the refractive indices of the fibers (fillers) and matrices.…”