Performance and multi-scale investigation on the phase miscibility of poly(lactic acid)/amided silica nanocomposites

In this work, amino-functionalized nano-SiO₂ (m@g-SiO₂) was synthesized through coupling reaction on the surface of nano-SiO₂. Moreover, the optimum preparation conditions of m@g-SiO₂ were selected via orthogonal experiments as follows: reaction temperature of 80 °C, reaction time of 8 h, the mass ratio of stearic acid, N,N'‑carbonyldiimidazole, imidazole hydrochloride and g-SiO₂ of 0.5:0.7:0.7:1. Fourier transform infrared spectroscopy, static angle measurement and X-ray photoelectron spectroscopy unanimously confirmed the formation of m@g-SiO₂. Furthermore, poly(lactic acid)(PLA)/m@g-SiO₂ nanocomposites was prepared with m@g-SiO₂ as fillers to improve the comprehensive performance of PLA. Then, the mechanical properties and crystallization behavior of PLA/m@g-SiO₂ nanocomposites were studied, which showed that the impact strength and elongation-at-break of PLA/m@g-SiO₂ (0.3 wt%) nanocomposites were increased by 78.05% and 1148%, respectively, and its crystallinity was increased by 26.46%. Simultaneously, thermal gravimetric analysis indicated that the thermal stability of PLA/m@g-SiO₂ nanocomposites was improved. Eventually, the multi-scale investigation on the phase miscibility of PLA/m@g-SiO₂ nanocomposites was probed by rheological behaviors analysis and the molecular dynamics simulations, which confirmed that surface modification of SiO₂ greatly enhanced the interaction energy and miscibility between the filler and PLA bulk.