Effect of Cellulose and Cellulose Nanocrystal Contents on the Biodegradation, under Composting Conditions, of Hierarchical PLA Biocomposites

In this work, the effect of microfibrillated cellulose (MFC) and cellulose nanocrystals (CNCs) on the biodegradation, under composting conditions, of hierarchical PLA biocomposites (HBCs) was studied using a full 2(2) factorial experimental design. The HBCs were prepared by extrusion processing and were composted for 180 days. At certain time intervals, the specimens were removed from the compost for their chemical, thermal and morphological characterizations. An ANOVA analysis was carried out at different composting times to study MFC and CNCs’ effects on biodegradation. The specimen’s mass loss and molecular weight loss were selected as independent variables. The results show that the presence of MFC enhances the PLA biodegradation, while with CNCs it decreases. However, when both cellulosic fibers are present, a synergistic effect was evident—i.e., in the presence of the MFC, the inclusion of the CNCs accelerates the HBCs biodegradation. Analysis of the ANOVA results confirms the relevance of the synergistic role between both cellulosic fibers over the HBC biodegradation under composting conditions. The results also suggest that during the first 90 days of incubation, the hydrolytic PLA degradation prevails, whereas, beyond that, the enzymatic microbial biodegradation dominates. The SEM results show MFC’s presence enhances the surface biodeterioration to a greater extent than the CNCs and that their simultaneous presence enhances PLA biodegradation. The SEM results also indicate that the biodegradation process begins from hydrophilic cellulosic fibers and promotes PLA biodegradation.