Rheology of Cellulosic Microfiber Suspensions Under Oscillatory and Rotational Shear for Biocomposite Applications

Abstract

This study investigates the rheological behavior of cellulose microfiber suspensions derived from kahili ginger stems (Hedychium gardnerianum), an invasive species, in two adhesive matrices: a commercial water-based adhesive (Coplaseal®) and a casein-based adhesive made from non-food-grade milk, referred to as K and S samples, respectively. Rheological analyses were performed using oscillatory and rotational shear tests conducted at 25 °C, 50 °C, and 75 °C to assess the materials’ viscoelastic properties more comprehensively. Oscillatory tests across a frequency range of 1–100 rad/s assessed the storage modulus (G′) and loss modulus (G″), while rotational shear tests evaluated apparent viscosity and shear stress across shear rates from 0.1 to 1000 s−1. Fiber-free samples consistently showed lower moduli than fiber-containing samples at all frequencies. The incorporation of fibers increased the dynamic moduli in both K and S samples, with a quasi-plateau observed at lower frequencies, suggesting solid-like behavior. This trend was consistent in all tested temperatures. As frequencies increased, the fiber network was disrupted, transitioning the samples to fluid-like behavior, with a marked increase in G′ and G″. This transition was more pronounced in K samples, especially above 10 rad/s at 25 °C and 50 °C, but less evident at 75 °C. This shift from solid-like to fluid-like behavior reflects the transition from percolation effects at low frequencies to matrix-dominated responses at high frequencies. In contrast, S samples displayed a wider frequency range for the quasi-plateau, with less pronounced moduli changes at higher frequencies. At 75 °C, the moduli of fiber-containing and fiber-free S samples nearly converged at higher frequencies, indicating similar effects of the fiber and matrix components. Both fiber-reinforced and non-reinforced suspensions exhibited pseudoplastic (shear-thinning) behavior. Fiber-containing samples exhibited higher initial viscosity, with K samples displaying greater differences between fiber-reinforced and non-reinforced systems compared to S samples, where the gap was narrower. Interestingly, S samples exhibited overall higher viscosity than K samples, implying a reduced influence of fibers on the viscosity in the S matrix. This preliminary study highlights the complex interactions between cellulosic fiber networks, adhesive matrices, and rheological conditions. The findings provide a foundation for optimizing the development of sustainable biocomposites, particularly in applications requiring precise tuning of rheological properties.