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The use of lignocellulose-rich biowaste as reinforcing filler in biodegradable polymers represents a sustainable option to obtain cost-effective bio-based materials to be used for several applications. In addition, the scarce polymer-biofiller interaction can be improved by reactive functionalization of the matrix. However, the obtained biocomposites might show high thermal deformability and possibly a slow biodegradation rate. In this work, polylactic acid (PLA) was first chemically modified with itaconic anhydride, and then biocomposites containing 50 wt.% of pecan ( Carya illinoinensis ) nutshell (PNS) biowaste were prepared and characterized. Their physical and morphological properties were determined, along with their biodegradation behavior in soil. Moreover, the effects of two environmentally friendly physical treatments, namely ball-milling of the filler and thermal annealing on biocomposites, were assessed. Grafting increased PLA thermal-oxidative stability and crystallinity. The latter was further enhanced by the presence of PNS, achieving a 30% overall increase compared to the plain matrix. Accordingly, the biocomposites displayed mechanical properties comparable to those of the plain matrix. Thermal annealing dramatically increased the mechanical and thermomechanical properties of all materials, and the heat deflection temperature of the biocomposites dramatically increased up to 60 °C with respect to the non-annealed samples. Finally, PNS promoted PLA biodegradation, triggering the swelling of the composites under soil burial, and accelerating the removal of the polymer amorphous phase. These results highlight the potential of combining natural fillers and environmentally benign physicochemical treatments to tailor the properties of PLA biocomposites. The high biofiller content used in this work, in conjunction with the chemical and physico-mechanical treatments applied, increased the thermal, mechanical, and thermomechanical performance of PLA biocomposites while improving their biodegradation behavior. These outcomes allow for widening the application field of PLA biocomposites in those areas requiring a stiff and lightweight material with low deformability and faster biodegradability.

Biodegradable polymer composites reinforced with agri-food lignocellulosic biowaste represent cost-effective and sustainable materials potentially able to replace traditional composites for structural, household, and packaging applications. Herein, the preparation of polylactic acid (PLA)/pecan (Carya illinoinensis) nutshell (PNS) biocomposites at high filler loading (50 wt%) is reported, alongside the effect of two environmentally friendly physical treatments, namely ball-milling of the filler and thermal annealing on biocomposites. PNS enhanced the thermal stability, the viscoelastic response, and the crystallinity of the polymer. Furthermore, filler ball-milling also increased the melt fluidity of the biocomposites, potentially improving melt processing. Finally, the presence of PNS remarkably enhanced the effect of thermal annealing in the compounds. In particular, heat deflection temperature of the biocomposites dramatically increased, up to 60 °C with respect to the non-annealed samples. Overall, these results emphasize the potential of combining natural fillers and environmentally benign physical treatments to tailor the properties of PLA biocomposites, especially for those applications which require a stiff and lightweight material with low deformability., (Copyright © 2022 Elsevier B.V. All rights reserved.)