The main aim of this work was to study the effect of surface modification on the characteristics of local Pine cone flour (PCF) and on the interfacial adhesion in polypropylene/poly(lactic acid)/Pine cone (PP/PLA/PCF) blend composites. For this purpose, alkali, silane, and a combination of both treatments were applied to impart a hydrophobic character to the PCF flour. Treated and untreated flour samples were subjected to several investigations, such as Fourier transform infrared spectroscopy (FTIR), X-rays diffraction (XRD), thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). The results revealed a reduction in the contents of hemicellulose, lignin, and wax upon treatments, as evidenced by the disappearance or reduction in the intensity of some characteristic bands, such as that related to the carbonyl groups (C = O) at 1730 cm−1. Also, the treatments were seen to enhance the surface roughness, thermal stability, and crystallinity of the flour, as a result of greater exposure to cellulose. The dynamic mechanical analysis (DMA) showed that the storage modulus of blend composites with modified flour is higher than that of the unfilled blend. In this sense, the Alkali-GPTMS 5%-PCF composite exhibited a higher value by 20, 9, and 16% compared to Untreated-, Alkali-, and GPTMS-PCF composites, respectively. Surface treatments increased the interfacial adhesion, as it was perceived from the decrease in the height of tan δ peak owing to PP/PLA/PCF blend composites. Finally, the combination of both silane and alkali treatments was found to provide composites with a more cohesive microstructure owing to the improved compatibility.
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