Critical roles of gelator network structure and concentration modulation synergy in manipulating freeze-thaw stability of oleogel-based Pickering emulsions

Network architecture and gelator concentration impact oleogel emulsions (OGEs). • Critical gelator concentration (CGC) guides architecture-specific stability. • Crystalline/fibrillar gelator at CGC achieved optimal freeze-thaw (F-T) stability. • OGEs based on ethyl cellulose at supra-CGC exhibited enhanced F-T stability. • Network architecture guides concentration requirements for stable OGEs. A systematic understanding of how internal network architectures (crystalline, fibrillar, and polymeric forms) and gelator concentration relative to critical gelation concentration (CGC) govern freeze-thaw stability in oleogel-based Pickering emulsions (OGEs) remain scarce. This study elucidated these relationships by preparing OGEs utilizing soybean oil structured with beeswax (BW, crystalline), phytosterols (PS, fibrillar), or ethyl cellulose (EC, polymeric) at subcritical (0.5 × CGC), critical (1.0 × CGC), and supercritical (2.0 × CGC) concentrations. The oil-water interfaces were stabilized by protein fibril-polysaccharide nanoparticles. For crystalline/fibrillar systems, CGC yielded optimal stability: uniform droplets, maximal viscoelasticity, no storage separation, and > 97% oil-binding after five freeze-thaw cycles, whereas excessive gelator concentrations induced destabilization. Conversely, polymeric systems required higher gelator concentrations to form robust matrices, minimizing freeze-thaw-induced water separation and maintaining high oil-binding capacity (>96%). These findings support an architecture-dependent formulation strategy: CGC enables balanced functionality for crystalline/fibrillar networks, while polymeric systems require supra-CGC reinforcement for optimal freeze-thaw resistance. Download: Download high-res image (147KB) Download: Download full-size image