New insights into food O/W emulsion gels: Strategies of reinforcing mechanical properties and outlook of being applied to food 3D printing.

3D printing technology has been widely used in food processing with its advantages of customized food design, personalized nutrition design, and simplified food supply chain. Food emulsion gels have application value and prospects in food 3D printing due to their promising properties, including biodegradability, biocompatibility, as well as dual characteristics of emulsions and biopolymer gels. Food emulsion gels with appropriate mechanical properties, as a new type of food inks, expand the types and functions of the inks. However, food emulsion gels without adequate reinforced mechanical properties may suffer from defects in shape, texture, mouthfeel, and functionality during 3D printing and subsequent applications. Therefore, it is necessary to summarize the strategies to improve the mechanical properties of food emulsion gels. According to the methods of characterizing the mechanical properties of emulsion gels, this article summarizes four strategies for improving the mechanical properties of emulsion gels through two ways: inside-out (reinforcement of interface and reinforcement of cross-linking) and outside-in (physical approaches and environmental regulations), as well as their basic mechanisms. The application status and future research trends of emulsion gels in food 3D printing are finally discussed.

Gel Property of Soy Protein Emulsion Gel: Impact of Combined Microwave Pretreatment and Covalent Binding of Polyphenols by Alkaline Method.

This study investigated the effects of microwave modification, alkali polyphenol (ferulic acid) covalently combined modification, and microwave-alkali polyphenol covalently combined modification on the gel properties of soy protein emulsions. The results showed that the properties of soy protein emulsions were improved significantly by the three modification methods. After three kinds of modification, the viscoelasticity of soy protein emulsion gel increased, and a gel system with stronger elasticity was formed. The texture, water-holding, and hydration properties of the emulsion gel increased significantly. The SEM and ClSM results showed that the modified soy protein emulsion gel had a more compact and uniform porous structure, and the oil droplets could be better embedded in the network structure of the gel. Among the three modification methods, the microwave-alkali method polyphenol covalently combining the compound modification effect was best, and the microwave modification effect was least effective compared to the other two methods. Our obtained results suggested that for gel property modification of soy protein emulsion gels, microwave pretreatment combined with the covalent binding of polyphenols by an alkaline method is an effective method.

Ultra-Sensitive and Ultra-Stretchable Strain Sensors Based on Emulsion Gels with Broad Operating Temperature.

Hydrogels with mechanical elasticity and conductivity are ideal materials in wearable devices. However, traditional hydrogels are fragile upon mechanical loading and lose functions in climate change because the internal water undergoes freeze and dehydration. Herein, we synthesize stable emulsions at high and low temperatures by introducing glycerol into the W/W emulsions. Then the high-stable emulsions are used as templates to produce the freestanding emulsion gels with enhanced mechanical strength and conductivity. The introduction of glycerol endows emulsions and emulsion gels with high and low temperature resistance (-20 to 90 °C). The fabricated strain sensors based on emulsion gels show high sensitivity (gauge factor=6.240), high stretchability (1081 %), fatigue resistance, self-healing and adhesion properties, realizing the repeatable and accurate detection of various human motions. These high-performance and eco-friendly emulsion gels can be promising candidates for next-generation artificial skin and human-machine interface.

Fabrication and characterization of Pickering emulsion gels stabilized by zein/pullulan complex colloidal particles.

BACKGROUND: Zein particles are unsuitable as stabilizers of Pickering emulsions because of their high hydrophobicity. However, few studies have reported on the use of a strong hydrophilic neutral polysaccharide to regulate its wettability. In this work, zein/pullulan complex particles (ZPPs) were formulated by an anti-solvent method to fabricate Pickering emulsions. RESULTS: The presence of pullulan increased the size, decreased the zeta, and provided excellent resistance to the gravitational separation of zein. Scanning electron microscopy (SEM) revealed that the shape of zein particles changed from spherical as they became aggregated ZPP nanoparticles. Fourier transform infrared (FTIR) spectroscopy indicated that the flocculation phenomenon of ZPPs was related to the hydrogen bond between zein and pullulan. Moreover, the hydrophobicity of zein was modified by hydrophilic pullulan to endow the ZPPs with nearly neutral wettability when the mass ratio was 15:1, allowing for the preparation of stable Pickering emulsions. In contrast to zein, the ZPPs contributed to building a compact interface layer around the droplets and smaller emulsion droplets. Under a certain ZPP concentration, the size and viscosity of emulsion increased with an increase in the oil volume fraction, indicating that the Pickering emulsions stabilized by ZPPs showed better stability against coalescence. Confocal laser scanning microscopy (CLSM) revealed that the ZPPs constructed a dense filling layer on the surface of oil droplets, thus further emphasizing that ZPPs can potentially be used in fabricating Pickering emulsion gels. CONCLUSION: Zein/pullulan complex particles are an excellent Pickering emulsion gel stabilizer that can be used in the delivery system of bioactive substances in food formulations. © 2020 Society of Chemical Industry.

Enzymatically Crosslinked Emulsion Gels Using Star-Polymer Stabilizers.

A novel type of emulsion gel based on star-polymer-stabilized emulsions is highlighted, which contains discrete hydrophobic oil and hydrophilic aqueous solution domains. Well-defined phenol-functionalized core-crosslinked star polymers are synthesized via reversible addition-fragmentation chain transfer (RAFT)-mediated dispersion polymerization and are used as stabilizers for oil-in-water emulsions. Horseradish-peroxidase-catalyzed polymerization of the phenol moieties in the presence of H2 O2 enables rapid formation of crosslinked emulsion gels under mild conditions. The crosslinked emulsion gels exhibit enhanced mechanical strength, as well as widely tunable composition.

Enhanced probiotic viability in innovative double-network emulsion gels: Synergistic effects of the whey protein concentrate-xanthan gum complex and κ-carrageenan.

In this study, the whey protein concentrate and xanthan gum complex obtained by specific pH treatment, along with κ-carrageenan (KC), were used to encapsulate Lactobacillus acidophilus JYLA-191 in an emulsion gel system. The effects of crosslinking and KC concentration on the visual characteristics, stability, mechanical properties, and formation mechanism of emulsion gels were investigated. The results of optical imaging, particle size distribution, and rheology exhibited that with the addition of crosslinking agents, denser and more homogeneous emulsion gels were formed, along with a relative decrease in the droplet size and a gradual increase in viscosity. Especially when the concentration of citric acid (CA) was 0.09 wt%, KC was 0.8 wt%, and K+ was present in the system, the double-network emulsion gel was stable at high temperatures and in freezing environments, and the swelling ratio was the lowest (9.41%). Gastrointestinal tract digestive treatments and pasteurization revealed that the probiotics encapsulated in the double-network emulsion gel had a higher survival rate, which was attributed to the synergistic cross-linking of CA and K+ biopolymers to construct the emulsion gels. Overall, this study highlights the potential of emulsion gels to maintain probiotic vitality and provides valuable insights for developing inventive functional foods.

Development of pea protein nanoparticle/hydrolyzed rice glutelin fibril emulsion gels for encapsulation of curcumin.

The potential of using emulsion gels stabilized by binary plant protein nanoparticle mixtures for the encapsulation and delivery of lipophilic nutraceuticals was evaluated. The particle characteristics, physical stability, water diffusivity, microrheology, large amplitude oscillating shear (LAOS) properties, and in vitro digestion of emulsion gels prepared by different ratios of hydrolyzed rice glutelin fibrils (HRGFs) and pea protein nanoparticle (PNP) were characterized. The emulsion gel with P/H = 2:1 (0.84 µm) exhibited the best storage stability and freeze-thaw stability, as seen by the smaller oil droplet size (1.02 and 1.42 µm, respectively). Low-field pulsed NMR indicated that the majority of water in samples was highly mobile. All the samples were predominantly elastic-like materials. The P/H 2:1 emulsion gel had the lowest FI value (6.21 × 10-4 Hz), the highest MVI value (5.57 s/nm2), G'/ G″ values and enclosed area, showing that it had denser 3D network structures, higher stiffness values, and a high sensitivity to changes in strain. Additionally, P/H 2:1 emulsion gel had a relatively high lipid digestibility (96.1 %), curcumin bioaccessibility (58.9 %), and curcumin stability (94.2 %). This study showed that emulsion gels stabilized by binary protein nanoparticle mixtures (PNP/HRGF) have potential as edible delivery systems for lipophilic nutraceuticals.

Seven sour substances enhancing characteristics and stability of whey protein isolate emulsion and its heat-induced emulsion gel under the non-acid condition.

Protein emulsion gels, as potential novel application ingredients in the food industry, are very unstable in their formation. However, the incorporation of sour substances (phosphoric acid, lactic acid, acetic acid, malic acid, glutamic acid, tartaric acid and citric acid) would potentially contribute to the stable formation of whey protein isolate (WPI) emulsion as well as its gel. Thus, in this work, physical stability of seven acid-treated WPI emulsions, and microstructures, rheological properties, water distribution of its emulsion gels were characterized and compared. Initially, the absolute zeta-potential, interfacial protein adsorption, and emulsifying characteristics of acid-induced WPI emulsions were higher in contrast to acid-untreated WPI emulsions. Moreover, acid-induced WPI emulsions were thermally induced (95 ℃, 30 min) to form its emulsion gel networks via disulfide bonds as the main force (acid-untreated WPI emulsions were unable to form gels). High-resolution microscopic observation revealed that acid-induced WPI in emulsion gel network showed the morphology of aggregates. Dynamic oscillatory rheology results indicated that acid-induced emulsion gel exhibited highly elastic behavior and its viscoelasticity was associated with the generation of protein gel networks and aggregates. In addition, PCA and heatmap results further illustrated that malic acid-induced WPI emulsion gels had the best water holding capacity and gel characteristics. Therefore, this study could provide an effective way for the foodstuffs industry to open up new texture and healthy emulsion gels as fat replaces and loading systems of bioactive substances.

Salmon protein gel enhancement for dysphagia diets: Konjac glucomannan and composite emulsions as texture modifiers.

The growing prevalence of dysphagia among the aging population presents a significant challenge. Many highly nutritious foods, like salmon, are often unsuitable for the elderly due to their firm texture when heated. To address this concern, a combination of salmon myofibrillar protein (SMP), Konjac glucomannan (KGM), and different emulsion fillers-such as oil droplets, octenyl succinic anhydride (OSA)-modified potato starch emulsion, and high methoxylated pectin (HMP) emulsions-was selected to enhance the network of salmon protein gels with the aims to create potential applications as dysphagia-friendly foods. The International Dysphagia Dietary Standardization Initiative (IDDSI) test indicated that all gel samples were classified as level 5. The OSA-SMP-KGM gel exhibited notably higher cohesiveness (P < 0.05), reduced adhesion, and enhanced mouthfeel. The OSA-SMP-KGM gel exhibited a smooth surface and excellent water retention (92.4 %), rendering it suitable for individuals with swallowing difficulties, particularly those prone to experiencing dry mouth. The yield stress of OSA-SMP-KGM gel was 594.14 Pa and stable structure was maintained during chewing and swallowing (γe/γv = 62.5). This study serves as a valuable reference for developing salmon-based products that are not only highly nutritious but also fulfill the criteria for a desirable swallowing texture.

Survivability of probiotics in Pickering emulsion gels stabilized by salmon by-product protein / sodium alginate soluble complexes at neutral pH.

Adequate amounts of live probiotics reaching the gut are necessary to maintain host health. However, the harsh environment during processing, the low pH of human gastric acid, and the high concentration of bile salts in the gut can significantly reduce survivability of probiotics. In this work, we propose a simple Pickering emulsion gels strategy to encapsulate Lactobacillus plantarum Lp90 into oil droplets filled in calcium alginate gels to improve its viability under pasteurization and gastrointestinal conditions. The emulsion gels were stabilized by the soluble complexes of salmon by-product protein (SP) and sodium alginate (ALG), and the aqueous phase was solidified by the addition of calcium. The interaction between SP and ALG and the effect of ALG concentration on emulsifying ability and emulsion stability were studied. The results from optical imaging, nuclear magnetic resonance, and rheological properties showed that the stability and viscosity of the emulsions gradually increased with the increased ALG concentration, while the droplet size of the emulsions and the content of free water in the system decreased significantly. Especially when the concentration of ALG was 1 %, the emulsion system was stable under the environment of high temperature and high ionic strength, and the water holding capacity was the highest. Through pasteurization and gastrointestinal digestion experiments, it was found that the survival rate of probiotics encapsulated in emulsion gels was significantly higher than that encapsulated in emulsions or hydrogels, which benefited from the dual action of oil droplets and calcium alginate gels network. These results provide a new strategy for the processing of probiotics and the high-value utilization of marine fish by-products.

Antioxidant-Enhanced Alginate Beads for Stabilizing Rapeseed Oil: Utilizing Extracts from Post-Distillation Waste Residues of Rosemary.

An eco-friendly extraction process of polyphenols from conventional dried rosemary tissues and post-distillation waste residues was applied using ß-cyclodextrin as a co-solvent. The aqueous extracts were characterized by measuring the total phenolic content, and their phenolic compounds were identified and quantified by LC-MS. Sodium alginate solutions (2% w/w) with/without incorporation of rosemary aqueous extracts were prepared and used for the preparation of O/W emulsions containing 20% rapeseed oil and an 80% water phase. Hydrogel beads were then stored at 20 °C for 28 days. The quality of encapsulated oil during storage was evaluated by measurements of the peroxide value, p-anisidine value, free fatty acids, total oxidation value, and fatty acid composition, whilst the aqueous phase of the beads was analyzed for its total extractable phenolic content (TEPC). The experimental findings indicate that the incorporation of aqueous extracts from post-distillation rosemary residues in emulsion-filled hydrogel beads resulted in the lowest level of oxidation products in the encapsulated rapeseed oil (PV = 10.61 ± 0.02 meq/Kg oil, p-AnV = 4.41 ± 0.09, and FFA = 0.14 ± 0.00, expressed as % oleic acid content), indicating an acceptable oil quality until the end of the storage period.

Emulsion gels prepared from Longzhua mushroom polysaccharides with self-gelling properties as ß-carotene carriers: Stability and in vitro digestibility of ß-carotene.

ß-Carotene is widely used in food systems because of its biological activity; however, ß-carotene has poor chemical stability and low bioavailability. Thus, researchers use encapsulated delivery systems to overcome these disadvantages. In this study, we prepared emulsion gels to encapsulate ß-carotene, using Longzhua mushroom polysaccharide (LMP), which can autonomously form weak gels. The LMP emulsion gel (LEG) exhibited a high water-holding capacity of up to 95.06 %. All samples showed adequate storage stability for 28 days. Increasing the polysaccharide content in the emulsion gel enhanced the encapsulation efficiency of ß-carotene (96.76 %-98.27 %), the release of free fatty acids (68.21 %-81.44 %), and the photostability (80.65 %-91.27 %), thermal stability (73.84 %-97.08 %), and bioaccessibility (18.28 %-30.26 %) of ß-carotene. In conclusion, LEG is a promising fat-soluble material that can be used for food-grade encapsulated delivery systems.

Advances of protein-based emulsion gels as fat analogues: Systematic classification, formation mechanism, and food application.

Fat plays a pivotal role in the appearance, flavor, texture, and palatability of food. However, excessive fat consumption poses a significant risk for chronic ailments such as obesity, hypercholesterolemia, and cardiovascular disease. Therefore, the development of green, healthy, and stable protein-based emulsion gel as an alternative to traditional fats represents a novel approach to designing low-fat food. This paper reviews the emulsification behavior of proteins from different sources to gain a comprehensive understanding of their potential in the development of emulsion gels with fat-analog properties. It further investigates the emulsifying potential of protein combined with diverse substances. Then, the mechanisms of protein-stabilized emulsion gels with fat-analog properties are discussed, mainly involving single proteins, proteins-polysaccharides, as well as proteins-polyphenols. Moreover, the potential applications of protein emulsion gels as fat analogues in the food industry are also encompassed. By combining natural proteins with other components such as polysaccharides, polyphenols, or biopolymers, it is possible to enhance the stability of the emulsion gels and improve its fat-analog texture properties. In addition to their advantages in protecting oil oxidation, limiting hydrogenated oil intake, and delivering bioactive substances, protein-based emulsion gels have potential in food 3D printing and the development of specialty fats for plant-based meat.

Dual functionality of diacylglycerols in water-in-oil emulsion gel systems.

Distearin (DS) can be used as an emulsifier, due to its surface activity derived from the amphiphilic nature of the molecule, moreover, it can also crystallize and form a 3D crystal network that can induce oil gelation. The current research aimed to examine the ability to combine both emulsifying and oil gelation properties to structure and stabilize water-in-oil emulsion gel system. Different water contents and DS concentrations produce emulsion gels with different textural attributes while incorporating up to 30% of water in a 15% wt. DS-based oleogel resulted in stable white gels. Microscopy imaging confirmed the formation of a water-in-oleogel type emulsion gel characterized by DS crystallization in the continuous phase and at the interface through Pickering mechanism. A positive relation was observed between the G' and hardness values and water content, suggesting gel strengthening resulted from interactions between the DS crystals at the interface and the continuous phase, as suggested by the active filler theory. Thermal analysis revealed two broad melting events at the temperature range of 42.2-44.9 °C and 55.9-58.6 °C for emulsion gels with 10-30% water content, suggesting initial melting of ß' polymorph and transition to ß during melting, which was confirmed by XRD. The results showed that homogenization significantly improved the oil retention of the gels due to increased crystal surface area, while water addition slightly reduced it. Compared with traditional emulsions or oleogels, this water-in-oil gel system demonstrated prolonged stability and enhanced mechanical properties due to the dual functionality of DS at the water/oil interface and bulk.

Synergistic formulation approach for developing pea protein and guar gum enriched olive oil-in-water emulsion gels as solid fat substitutes: Formulation optimization, characterization, and molecular simulation.

This study aimed to optimize the formulation of olive oil-in-water (O/W) emulsion gels by incorporating Pea Protein (PP) and Guar Gum (GG) as alternative options for solid fats. The optimum rheological (consistency index, apparent viscosity, recovery) and texture (firmness) properties of the emulsion gels were obtained using a mixture of 2 % PP, 1 % GG, 60 % Olive Oil (OO), and 37 % Water (W). The blend of PP2/GG1 showed the highest results for recovery and firmness, 111.27 % and 33.89 g, respectively. PP/GG blend emulsion gels exhibited higher absolute ζ-potential values, ranging between -72.3 and -77.4 mV. The polydispersity index (PDI) ranged from 0.185 to 0.535, with the most uniform distributions found in the PP/GG blend emulsion gels. Strong phase separation resistance indicated strong stability of PP-GG complex emulsion gels. Higher PP concentrations decreased emulsion oxidation. FTIR and XRD research showed that PP and GG interact strongly, indicating good compatibility. The free binding energy of the most stable configuration of the molecules was -6.8 kcal mol-1, indicating a high affinity. PP interacted with GG through 9 amino acid residues, with notable residues being Asp 224, Thr 235, Ala 332, Ile 334, and Arg 336, and their respective interaction distances ranged between 2.69 Å and 3.87 Å.

Improved light and ultraviolet stability of curcumin encapsulated in emulsion gels prepared with corn starch, OSA-starch and whey protein isolate.

The objective of this study was to enhance the bioavailability and stability of curcumin (Cur) by encapsulating it in corn starch (CS)/octenylsuccinic acid modified (OSA)-starch-whey protein isolate (WPI) emulsion gels (EGs). As the volume fraction of the oil phase increased, the droplet size and ζ- potential of the EGs decreased. The encapsulation efficiency and bioavailability of Cur in CS/OSA-starch-WPI EGs with a 60% oil ratio were 96.0% and 67.3%, respectively. The release rate of free fatty acid and the bioavailability of Cur from the EGs after digestion were significantly higher compared to Cur dissolved in oil. EGs with an oil phase volume fraction of 75% and 80% demonstrated greater protection against light irradiation but were less effective against UV irradiation compared to EGs with a 60% oil phase volume fraction. Encapsulation in EGs proved to be an effective method for enhancing the bioavailability and stability of Cur.

Construction of emulsion gel based on the interaction of anionic polysaccharide and soy protein isolate: Focusing on structural, emulsification and functional properties.

In this study, the effects on the structures and emulsion gels of carrageenan (CA) and gum arabic (GA) with soybean protein isolate (SPI) were investigated. The results showed that CA and GA exposed hydrophobic groups to SPI, and formed complexes through non-covalent interactions to improve the stability of the complexes. Furthermore, the emulsion gels based on the emulsions exhibited that CA formed emulsion-filled gels with higher elasticity, stronger gel strength, and thermal reversibility, whereas GA formed emulsion-aggregated gels with higher viscosity, and a weak-gel network. The results of digestion showed that, CA was more helpful to slow down the release of free fatty acids and protect vitamin E during digestion. Compared with SPI-GA emulsion gel, SPI-CA emulsion gel had better physicochemical properties and stronger network structure. The results of this study may be useful in the development of anionic polysaccharides that interact with SPI, and they may provide new insights on the preparation of emulsion gels that slowly release fat-soluble nutrients.

Texture characterization of 3D printed fibrous whey protein-starch composite emulsion gels as dysphagia food: A comparative study on starch type.

Texture-modified, multi-nutrient composite foods are essential in clinical treatment for dysphagia individuals. Herein, fibrous whey protein-stabilized emulsion and different crystalline starches (wheat, corn, rice, potato, sweet potato, cassava, mung bean and pea) were used to structure composite emulsion gels (CEGs). These CEGs then underwent 3D printing to explore the feasibility of developing a dysphagia diet. The network of molded CEGs was mainly maintained by hydrophobic interactions and hydrogen bonds. Rice and cassava starches were better suited for structuring soft-textured CEGs. Compared with molded CEGs, 3D printing decreased hydrogen bonds and the compactness of the nano-aggregate structure within the gel system, forming a looser gel network and softening the CEGs. Interestingly, these effects were more pronounced for the CEGs with high initial hardness. This study provided new strategy to fabricate CEGs as dysphagia diet using fibrous whey protein and starch, and to design texture-modified foods for patients using 3D printing.

Enhancing Lactobacillus plantarum delivery: Impact of gluconolactone concentration on high-internal-phase emulsion gels and gastrointestinal viability.

In this study, the impact of Gluconolactone (GDL) concentration on the formation of high-internal-phase emulsion gels (HIPEGs) and the gastrointestinal digestive viability of Lactobacillus plantarum encapsulated within these HIPEGs were demonstrated. Increasing GDL concentrations led to cross-linking of particles at the oil-water interface, thereby stabilizing smaller oil droplets. The addition of GDL to HIPEs results in a significant increase in the secondary structure of SPI, specifically in ß-sheet and ß-turn formations, accompanied by a reduction in α-helix percentage. This alteration enhanced the binding effect of protein on water, leading to changes in intermolecular force. Notably, HIPEGs containing 3.0% GDL demonstrated superior encapsulation efficiency and delivery efficiency, reaching 99.0% and 84.5%, respectively. After 14 d of continuous zebrafishs feeding, the intestinal viable cells count of Lactobacillus plantarum reached 1.18 × 107 CFU/mL. This finding supports the potential use of HIPEGs as a probiotic delivery carrier, effectively enhancing the intestinal colonization rate.

Development and characterization of ultrastable emulsion gels based on synergistic interactions of xanthan and sodium stearoyl lactylate.

Emulsion gels with the mixtures of low-molecular-weight emulsifier (LME) and polymer have attracted much attention in food; however, the LME-polymer interactions in emulsion system are complex and unclear. Here, the interactions between SSL and xanthan in emulsions and the mechanisms of stabilizing emulsions were investigated by using tensiometry, zeta potential, Fourier transform infrared spectroscopy (FTIR), confocal laser scanning microscopy (CLSM), cryo-scanning electron microscopy (cryo-SEM) and rheology. SSL was more efficiently adsorbed on the oil-water interface than xanthan. Interestingly, the honeycomb structure was formed in emulsion gels, which firmly immobilized oil droplets. Furthermore, electrostatic repulsion and hydrophobic interactions between xanthan and SSL facilitated the efficient bonding at interface and in bulk. Both linear and nonlinear rheology strongly supported the fact that the interactions between xanthan and SSL enhanced gel-like viscoelastic structure of emulsion gels. This structure endows excellent stability of emulsion gels under high temperature storage, sealed conditions and pH change.