Reinforcement of peanut oil bodies by nanocellulose to prepare oleogels as fat substitutes: Molecular entanglement and lipid droplet embedding

• Reinforcement of peanut oil bodies (POB) with nanocellulose to form oleogels. • Cross-links of POB and nanocellulose to form oleogel verified by Cryo-SEM. • CNF-POB leads to thick and viscoelastic layers, but a loose interfacial network. • Nanocellulose binds to POB through hydrogen bonding and hydrophobic interactions. • Texture, rheological, and thermal properties of oleogels suited as fat substitutes. To address the health risks of traditional animal fats and meet the demand for solid fat substitutes, oleogels were fabricated by reinforcing the peanut oil body (POB) interface with three modified nanocelluloses: cellulose nanofibers (CNF), carboxymethyl cellulose (CMC), and cellulose nanocrystals (CNC). CNF-POB exhibited the highest oil binding capacity (OBC, 98.69 ± 2.21%), and CNF-POB formed a robust fibrous three-dimensional network, leading to the highest storage modulus and hardness. QCM-D revealed the adsorption process of the gel on hydrophobic surfaces. Combined with fitting using the Voigt model, it was found that films formed by different nanocelluloses at the POB interface have varying thicknesses and densities. FTIR and SERS confirmed interfacial interactions, primarily involving hydrogen bonding and hydrophobic interactions between nanocelluloses and POB. Sensory evaluation and principal component analysis demonstrated that the introduction of nanocellulose regulates the release of volatile components such as aldehydes, ketones, and hydrocarbons in POB. Mechanistically, nanocelluloses adsorbed on the POB interface to reduce aggregation, and their molecular entanglement formed a matrix for lipid droplet embedding. Collectively, this study provides a theoretical and practical basis for developing natural, high-performance fat substitutes using nanocellulose-reinforced oleogels.