The Critical Role of Ca²⁺ in Improving the Transparency and Strength of High-Filler-Content Nanocellulose/Montmorillonite Nanocomposite Films

Strong and transparent nanocellulose/montmorillonite (MMT) nanocomposite films with high filler content (≥50 wt %) are emerging as versatile materials for advanced applications due to their excellent optical, barrier, mechanical, and thermal properties, and environmental friendliness. Nonetheless, these films undergo a notable decline in optical and mechanical properties at high MMT loadings. This study first demonstrates that calcium-ion-induced tactoids are the key factor causing disordered structures in nanocomposite films, leading to the degradation of optical and mechanical properties. We then address this issue by employing a Ca 2+ removal strategy─dialysis. Through removing 43% of free Ca 2+, simultaneous improvements in both properties are observed. For example, in a nanocomposite film with 70 wt % MMT, light transmittance increases from 75.9 to 91.6%, and the tensile strength rises from 100.4 to 139.4 MPa. This work offers insights into developing strong and transparent nanocomposite films with high MMT contents.