Melt-processing of cellulose nanofibril/polylactide bionanocomposites via a sustainable polyethylene glycol-based carrier system

Abstract

Considering the appealing need for an industrially viable approach, this works aims at demonstrating the rapid and easy melt processing of Polylactide (PLA) bio-composites reinforced with cellulose nanofibrils (CNF). For this purpose and against to their high propensity to self-aggregate on processing, an aqueous CNF-based suspension in the presence of polyethylene glycol (PEG) followed by a gentle drying way were performed to provide melt-processable CNF-based masterbatches. Morphological observations coupled with rheological analyses confirmed how the strategy of the PEG-based masterbatch approach facilitated the formation of a well-dispersed and strongly interacting CNF network within the polymeric matrix. At temperatures above Tg, thermo-mechanical characterization showed that the load-bearing capacity of the web-like CNF network was even more apparent and counteracted the PEG plasticizing effect. Thermogravimetric analysis evidenced that in the case of selective positioning at the PLA-PEG interface, CNF mitigated the negative impact of PEG addition on the PLA thermal stability. These results revealed the successfulness of our sustainable organic solvent-free approach to prepare melt-processable CNF masterbatches, which can be readily converted into conventional industrially scalable melt-processing techniques.