Mechanical Characteristics of Tara Gum/Orange Peel Films Influenced by the Synergistic Effect on the Rheological Properties of the Film-Forming Solutions

Film-forming solutions were prepared using Tara gum (TG), with glycerol (GL) as a plasticizer and orange peel powder (OP) as a filler. A TG stock solution (10 g/L) was initially prepared to facilitate homogenization, from which appropriate dilutions were made to obtain final concentrations of 0.6%, 0.8%, and 1.0% (w/v). GL (30% and 50%) and OP (0%, 20%, and 50%) were incorporated based on the dry weight of TG, meaning their amounts were calculated relative to TG content to ensure consistent formulation ratios. Rheological parameters, including the flow behavior index, consistency coefficient, storage modulus (G′), and loss modulus (G″), were characterized via steady shear and oscillatory rheometry. Mechanical properties, such as the Young’s modulus, tensile strength, and elongation at break, were also evaluated. A strong positive correlation (R2 = 0.840) was observed between G′ and the Young’s modulus, indicating that solutions with higher internal network strength yield films with greater stiffness. The synergistic interaction between TG and OP was critical: TG primarily enhanced stiffness and mechanical reinforcement, whereas OP improved structural cohesion and stability. GL functioned as a plasticizer, increasing film flexibility while reducing stiffness. These interactions led to a reduction in film solubility by up to 62.43%, particularly in formulations without orange peel powder. In contrast, mechanical strength increased by up to 50.21% in films containing orange peel powder, as those without it exhibited significantly lower tensile strength. Flexibility, expressed as elongation at break, was enhanced by up to 78.86% in formulations with higher glycerol content. Barrier properties were also improved, demonstrated by decreased water vapor permeability and increased hydrophobicity, attributed to the TG–OP synergy. A regression model (R2 = 0.928) substantiated the contributions of TG to stiffness, OP to matrix reinforcement, and GL to flexibility modulation. This study underscores the pivotal role of rheological behavior in defining film performance and presents a novel analytical framework applicable to the design of sustainable, high-performance biopolymeric materials.