This study reports the effect of pH (2, 7, 10) and heat treatment (80 °C for 30 min) on the oil–water (o/w) interfacial behavior of hemp seed protein isolate (HPI) aqueous dispersions. The physicochemical, interfacial adsorption, rheology, and emulsifying properties of protein dispersions were evaluated. HPI dispersions at pH 10 exhibited the highest water solubility (60%), the greatest net charge (−27 mV), and the lowest hydrophobicity (~5 a.u.), promoting o/w interfacial pressure (π) and interfacial viscoelasticity. Strong interfacial viscoelastic protein layers (E^* = 25 mN/m) were also observed under acidic conditions (pH 2), where proteins exhibited high solubility (40%), a high positive net charge (21 mV), and increased hydrophobicity (46 a.u.). HPI dispersions in their neutral state (pH 7) were not able to form stable o/w emulsions due to their poor physicochemical properties such as low solubility (18%), low surface charge (−18 mV), and hydrophobicity (~5 a.u.). Heat treatment significantly increased the charge and hydrophobicity of both neutral and alkaline proteins (~30 mV and ~10 a.u., respectively), increasing their particle size distribution and ultimately reducing their interfacial protein layer elasticity (E^* = 20 and 13 nM/m, respectively). While particles at acidic conditions showed high thermal resistance, heat treatment improved the emulsifying stability in alkaline conditions while further reducing it in the neutral state. Overall, HPI dispersions demonstrated the ability to form stable emulsions at both alkaline and acid pHs, with those formed at pH 2 exhibiting a lower droplet size and superior stability.

This study reports on the design and characterisation of thermo-reversible gelatine hydrogels incorporating beeswax-structured oil-in-water emulsions as novel 3D-printable food inks. Beeswax oil-in-gel emulsions (BOGEs) were prepared by varying the sunflower oil to beeswax (SFO:BW) mass fraction (1:0, 3:1, 1:1, 1:3 and 0:1) at a fixed lipid loading (10% wt.) within a 4% wt. gelatine matrix. The BOGEs were evaluated in terms of microstructure, thermophysical properties, small and large amplitude oscillatory shear rheological behaviour, instrumental hardness, and 3D printability. CLSM images revealed a progressive transition from an emulsion-filled to a bigel-like microstructure with increasing beeswax content, driven by partial crystallisation and percolation of lipid droplets. Differential scanning calorimetry confirmed that beeswax incorporation progressively suppressed the gelatine hydrogel fusion enthalpy, indicating that wax crystal lattices govern the supramolecular organisation of the gelatine network. SAOS tests showed that BW enhanced the elastic modulus, with a critical solid fat content threshold (Φc = 0.294) above which lipid droplet percolation provided an additional structural reinforcement. LAOS characterisation revealed a type III nonlinear viscoelastic response, with delayed yielding and enhanced structural integrity at higher BW fractions. Instrumental hardness measurements confirmed the active filler role of BW at mass fractions ≥0.5. 3D printing assessment demonstrated that intermediate SFO:BW ratios (3:1 and 1:1) afforded the highest printing fidelity, combining favourable extrusion flow with adequate post-deposition shape retention. Overall, the results demonstrate that beeswax-structured emulsions can effectively tailor the structure–function properties of gelatine hydrogels, enabling the development of clean-label, multiphase food inks suitable for extrusion-based 3D printing applications.

Nanocelluloses are versatile, bio-based materials capable of forming stable colloidal systems via Pickering stabilization. The combination of deep eutectic solvent (DES) pretreatment with ultra-high-pressure homogenization (UHPH) represents a promising green strategy to produce functional nanocellulose particles with tunable properties. In the present work, choline chloride-based DESs with glycerol (Ch_G), urea (Ch_U), or malic acid (Ch_MA) were used to pretreat microcrystalline cellulose prior to UHPH processing, yielding nanocelluloses with distinct morphologies and surface characteristics. Pickering oil-in-water emulsions were prepared, and their microstructure, rheological behavior, and colloidal stability were evaluated under varying temperature, pH, and ionic strength conditions. Ch_G and Ch_U treated nanocellulose exhibited long, flexible fibrils that stabilized the o/w emulsions primarily through network-mediated steric hindrance and lipid droplet immobilization. In contrast, Ch_MA treated nanocellulose featured shorter, highly charged particles that enhanced droplet dispersion via electrostatic repulsion though showing higher sensitivity to pH and ionic strength. Overall, the Pickering o/w emulsions demonstrated high stability over a broad range of temperatures (25-50 °C), pH values (4.5-10), and ionic strengths (≤ 200 mM NaCl), highlighting the effectiveness of DES-UHPH processing for tuning nanocellulose-based Pickering stabilization mechanisms in food-relevant emulsion systems.