Formation of small-granule starch oleogels based on capillary force: Impact of starch surface lipids on lubrication performance.

Starch granule oleogels were prepared and their rheological properties were precisely tuned using the capillary bridging phenomenon. The addition of a small amount of water to an oily suspension of starch granules can lead to starch granule bridging and network formation, transitioning it from a fluid-like to a gel-like state. Small-granule starches with high specific surface area and interfacial area exhibited a greater number of liquid bridges and stronger starch granules interactions, making them more prone to forming structurally stable oleogel systems. By increasing the content of water and starch granule, the starch oleogels exhibited three distinct structural states: pendular state (water ≤ 3.28 %, starch ≤ 17.85 %), pendular bridging network (water: 4.92 %, starch: 24.59 %), and capillary aggregates (water ≥ 6.56 %, starch > 24.59 %). Furthermore, the influence of starch granule surface lipids on the lubrication performance of the oleogel system was investigated. Surface roughness increased after extraction of surface lipids, and the friction coefficient also showed a significant increase. Overall, capillary suspension system can potentially be used to design novel fat food products, and our findings have established the correlation between starch granule surface properties and sensory perception in food, providing valuable insights for adjusting the oral processing characteristics of food.

Confining the Growth of AgNPs onto Epigallocatechin Gallate-Decorated Zein Nanoparticles for Constructing Potent Protein-Based Antibacterial Nanocomposites.

Sliver nanoparticles (AgNPs) have attracted tremendous interest as an alternative to commercially available antibiotics due to their low microbial resistance and broad-spectrum antimicrobial activity. However, AgNPs are highly reactive and unstable and are susceptible to fast oxidation. Synthesizing stable and efficient AgNPs using green chemistry principles remains a major challenge. To address this issue, we establish a facile route to form AgNP-doped zein nanoparticle core-satellite superstructures with ultralow minimum bactericidal concentration (MBC). In brief, polyphenol surface-functionalization of zein nanoparticles was performed, and the epigallocatechin gallate (EGCG) layer on zein nanoparticles served as a reducing-cum-stabilizing agent. We used EGCG-decorated zein nanoparticles (ZE) as a template to direct the nucleation and growth of AgNPs to develop metallized hybrid nanoparticles (ZE-Ag). The highly monodispersed core-satellite nanoparticles (∼150 nm) decorated with ∼4.9 nm AgNPs were synthesized successfully. The spatial restriction of EGCG by zein nanoparticles confined the nucleation and growth of AgNPs only on the surface of the particles, which prevented the formation of entangled clusters of polyphenols and AgNPs and concomitantly inhibited the coalescence and oxidation of AgNPs. Thus, this strategy improved the effective specific surface area of AgNPs, and as a result, ZE-Ag efficiently killed the indicator bacteria, Escherichia coli (E. coli) and Methicillin-resistant Staphylococcus aureus(MRSA) after 20 min of incubation, with MBCs of 2 and 4 µg/mL, respectively. This situation indicated that as-prepared core-satellite nanoparticles possessed potent short-term sterilization capability. Moreover, the simulated wound infection model also confirmed the promising application of ZE-Ag as an efficient antimicrobial composite. This work provides new insights into the synthesis and emerging application of AgNPs in food preservation, packaging, biomedicine, and catalysis.

One-Step Generation of O/W/O Double Pickering Emulsions Utilizing Biocompatible Gliadin/Ethyl Cellulose Complex Particles as the Exclusive Stabilizer.

Double emulsions hold great potential for various applications due to their compartmentalized internal structures. However, achieving their long-term physical stability remains a challenging task. Here, we present a simple one-step method for producing stable oil-in-water-in-oil (O/W/O) double emulsions using biocompatible gliadin/ethyl cellulose complex particles as the sole stabilizer. The resulting O/W/O systems serve as effective platforms for encapsulating enzymes and as templates for synthesizing porous microspheres. We investigated the impact of particle concentration and water fraction on the properties of Pickering O/W/O emulsions. Our results demonstrate that the number and volume of inner oil droplets increased proportionally with both the water fraction and particle concentration after a 60-day storage period. Moreover, the catalytic reaction rate of the encapsulated lipase within the double emulsion exhibited a significant acceleration, achieving a substrate conversion of 80.9% within 15 min. Remarkably, the encapsulated enzyme showed excellent recyclability, enabling up to 10 cycles of reuse. Additionally, by utilizing the O/W/O systems as templates, we successfully obtained porous microspheres whose size can be controlled by the outer water droplet. These findings have significant implications for the future design of Pickering complex emulsion-based systems, opening avenues for extensive applications in pharmaceuticals, food, cosmetics, material synthesis, and (bio)catalysis.

Biocompatible gliadin-sericin complex colloidal particles used for topical delivery of the antioxidant phloretin.

Oxidative stress caused by environmental exposures results in numerous skin diseases. Phloretin (PHL) is often used to relieve various skin symptoms, however, precipitation or crystallization of PHL in aqueous systems limits its ability to diffuse through the stratum corneum, making it difficult to exert effect at the target. To address this challenge, we herein report a method for the generation of core-shell nanostructure (G-LSS) via the growth of sericin crust around gliadin nanoparticle as a topical nanocarrier of PHL to improve its cutaneous bioavailability. Physicochemical performance, morphology, stability, and antioxidant activity of the nanoparticles were characterized. G-LSS-PHL exhibited uniformed spherical nanostructures with the robust encapsulation on PHL (∼90 %). This strategy protected PHL from UV-induced degradation, facilitating to inhibit erythrocyte hemolysis and quench free radicals in a dose-dependent manner. Transdermal delivery experiments and porcine skin fluorescence imaging indicated that G-LSS facilitated the penetration of PHL across the epidermis layer of skin to reach deep-seated sites, and promoted cumulative turnover of PHL with a 2.0-fold increase. Cell cytotoxicity and uptake assay confirmed that as-prepared nanostructure was nontoxic to HSFs, and promoted cellular absorption of PHL. Therefore, this work opened up new promising avenues for developing robust antioxidant nanostructure for topical applications.

CO2-responsive Pickering emulsions stabilized by soft protein particles for interfacial biocatalysis.

Pickering emulsions are emulsions stabilized by colloidal particles and serve as an excellent platform for biphasic enzymatic catalysis. However, developing simple and green strategies to avoid enzyme denaturation, facilitate product separation, and achieve the recovery of enzyme and colloidal particle stabilizers is still a challenge. This study aimed to report an efficient and sustainable biocatalysis system via a robust CO2/N2-responsive Pickering oil-in-water (o/w) emulsion stabilized solely by pure sodium caseinate (NaCas), which was made naturally in a scalable manner. The NaCas-stabilized emulsion displayed a much higher reaction efficiency compared with conventional CO2/N2-responsive Pickering emulsions stabilized by solid particles with functional groups from polymers or surfactants introduced to tailor responsiveness, reflected by the fact that most enzymes were transferred and enriched at the oil-water interface. More importantly, the demulsification, product separation, and recycling of the NaCas emulsifier as well as the enzyme could be facilely achieved by alternatively bubbling CO2/N2 more than 30 times. Moreover, the recycled enzyme still maintained its catalytic activity, with a conversion yield of more than 90% after each cycle, which was not found in any of the previously reported CO2-responsive systems. This responsive system worked well for many different types of oils and was the first to report on a protein-based CO2/N2-responsive emulsion, holding great promise for the development of more sustainable, green chemical conversion processes for the food, pharmaceutical, and biomedical industries.

Pickering Emulsions Simultaneously Stabilized by Starch Nanocrystals and Zein Nanoparticles: Fabrication, Characterization, and Application.

Using two types of colloidal particles having natural origins to synergistically stabilize Pickering emulsions is essential for food, cosmetics, and pharmaceutics, especially when neither particle can stabilize the Pickering emulsions alone. The use of two natural stabilizers avoids the complicated surface treatments of particles and the introduction of poisonous or harmful chemicals. In this work, we report an all-natural Pickering emulsion stabilized synergistically by starch nanocrystals and zein protein nanoparticles. Our result shows that the electrostatic interaction between the two types of particles greatly affects their assembled structure at the oil/water interface, which is closely related to the emulsion stability. Specifically, particle bilayers could form with oppositely charged particles at the interface to endow the emulsion with improved stability. As a demonstration, the resultant Pickering emulsions effectively carry ß-carotene and have high stability against high temperatures and ultraviolet radiation. This type of all-natural Pickering emulsion is a promising tool to protect and deliver liposoluble bioactive components.

Growth of Au nanoparticles on phosphorylated zein protein particles for use as biomimetic catalysts for cascade reactions at the oil-water interface.

Chemo-enzymatic cascade processes are invaluable due to their ability to rapidly construct high-value products from available feedstock chemicals in a one-pot relay manner. However, they have proven to be challenging because of the mutual inactivation of both catalysts. A conceptually novel strategy based on Pickering interfacial catalysis (PIC) is proposed here to address this challenge. This study aimed to construct a protein-stabilized Pickering system for biphasic cascade catalysis, enabled by phosphorylated zein nanoparticles (ZCPOPs) immobilized in gold nanoparticles (Au NCs). Ultra-small Au NCs, 1-2 nm in diameter, were integrated into ZCPOPs at room temperature. Then, the as-synthesized ZCPOPs-Au NCs were used to stabilize the oil-in-water (o/w) Pickering emulsion. Besides their excellent catalytic activity and recycling ability in a variety of oil phases, ZCPOPs-Au NCs possess unpredictable catalytic activity and exhibit mimicking properties of horseradish peroxidase. Particularly, the cascade reaction is well achieved using a metal catalyst and a biocatalyst at the oil-water interface. The result showed that such a combination of chemo- and biocatalysis improved the catalytic yield more than two times compared with that of sole metal catalysis. This study opened a new avenue to design nanomaterials using the combination of chemo- and biocatalysis in a Pickering emulsion system for multistep syntheses.

Bioavailability of quercetin in zein-based colloidal particles-stabilized Pickering emulsions investigated by the in vitro digestion coupled with Caco-2 cell monolayer model.

Protein-based Pickering emulsions have received considerable attention as nutraceutical vehicles. However, the oral bioavailability of nutraceuticals encapsulated in Pickering emulsions was not well established. In this work, a simulated gastrointestinal tract/Caco-2 cell culture model was applied to investigate the oral bioavailability of quercetin encapsulated in zein-based Pickering emulsions with quercetin in zein particles as the control. Pickering emulsions with shell (ZCP-QE) and core quercetin (ZCPE-Q) were constructed, and quercetin bioaccessibility, cell uptake and secretion, and the overall bioavailability were evaluated and compared. The overall oral bioavailability of quercetin was increased from 2.71% (bulk oil) to 38.18% (ZCPs-Q) and 18.97% (ZCPE-Q), particularly reached 41.22% for ZCP-QE. This work took new insights into the contributions of bioaccessibility and absorption (cell uptake plus secretion) to the overall oral bioavailability of quercetin. A schematic representation is proposed to relate the types of colloidal nanostructures in the digesta to the uptake, cell absorption, and overall oral bioavailability of quercetin. This study provided an attractive basis for identifying effective strategies to improve the oral bioavailability of hydrophobic nutraceuticals.

Hofmeister Effect-Assistant Fabrication of All-Natural Protein-based Porous Materials Templated from Pickering Emulsions.

Porous materials derived from natural and biodegradable polymers have received growing interest. We demonstrate here an attractive method for the preparation of protein-based porous materials using emulsions stabilized by gliadin-chitosan hybrid particles (GCHPs) as the template, with the addition of gelatin and kosmotropic ions to improve the mechanical strength. The microstructure, mechanical properties, cytotoxicity, and fluid absorption behavior of porous materials were systematically investigated. This strategy facilitated the formation of porous materials with highly open and interconnected pore structure, which can be manipulated by altering the mass ratio of hexane or gelatin in the matrix. The Hofmeister effect resulted from kosmotropic ions greatly enhanced the Young's modulus and the compressive stress at 40% strain of porous materials from 0.56 to 6.84 MPa and 0.26 to 1.11 MPa, respectively. The developed all-natural porous materials were nontoxic to HaCaT cells; they also had excellent liquid (i.e., simulated body fluid and rabbit blood) absorption performance and advantages in resisting stress and maintaining geometry shape. The effects of different concentration amounts and type of salts in the Hofmeister series on the formation and performance of porous materials were also explored. Mechanical strength of porous materials was gradually enhanced when the (NH4)2SO4 concentration increased from 0 to 35 wt %, and the other four kosmotropic salts, including Na2S2O3, Na2CO3, NaH2PO4, and Na2SO4, also showed positive effects. This work opens a simple and feasible way to produce nontoxic and biodegradable porous materials with favorable mechanical strength and controllable pore structure. These materials have broad potential application in many fields involving biomedical and material science, such as cell culture, (bio)catalysis, and wound or bone defect healing.

Inverse Pickering Emulsion Stabilized by Binary Particles with Contrasting Characteristics and Functionality for Interfacial Biocatalysis.

Water-in-oil (w/o) Pickering emulsions have received considerable attention in biphasic enzymatic catalysis for their advantages of good stability, large interfacial area, and ease of product separation. However, enzymes are commonly encapsulated in the interior of aqueous droplets, which inevitably increases the diffusional resistance to catalysis. Alternatively, enzymes are immobilized or trapped into Pickering stabilizers. Often, however, these approaches suffer from leaching and a decrease of enzyme activity during the chemical treatments. We report here a new Pickering interfacial biocatalysis platform with efficient enzyme encapsulation, binary particle composition, and high catalytic performance. Our approach is based on w/o Pickering emulsions stabilized by binary particles consisting of hard silica and soft, pH-responsive microgel particles. We demonstrate that pH-responsive microgels can simultaneously stabilize a w/o Pickering emulsion, encapsulate enzymes, and catalyze reactions at the water/oil interface. In addition, we show that the coordination with rigid silica nanoparticles as additional stabilizers markedly improves the emulsion structure and will provide a new avenue for the preparation of w/o Pickering emulsion and concept of biphasic catalysis.

Sodium caseinate as a particulate emulsifier for making indefinitely recycled pH-responsive emulsions.

pH-responsive emulsions are one of the simplest and most readily implementable stimuli-responsive systems. However, their practical uses have been greatly hindered by cyclability. Here, we report a robust pH-responsive emulsion prepared by utilizing pure sodium caseinate (NaCas) as the sole emulsifier. We demonstrate that the emulsification/demulsification of the obtained NaCas-stabilized emulsion can be triggered by simply changing the pH value over 100 cycles, which has never been observed in any protein-stabilized emulsion system. The NaCas-stabilized emulsion maintains its pH-responsive properties even in a saturated salt solution (NaCl ∼ 6.1 M) or seawater. We illustrate how NaCas functions in pH-responsive emulsions and show that when conventional nanoparticles such as zein protein or bare SiO2 particles were coated with a layer of NaCas, the resulting formulated emulsions could be switched on and off over 10 cycles. The unique properties of NaCas thus enable the engineering of conventional Pickering emulsions to pH-responsive Pickering emulsions. Finally, we have integrated catalytically active gold (Au) nanoclusters (NCs) into the NaCas protein and then utilized them to produce emulsions. Remarkably, these NaCas-Au NCs assembled at the oil-water interface exhibited excellent catalytic activity and cyclability, not only in aqueous solution, but also in complicated seawater environments.

Protein-Based Pickering High Internal Phase Emulsions as Nutraceutical Vehicles of and the Template for Advanced Materials: A Perspective Paper.

Pickering high internal phase emulsions (HIPEs) are normally highly concentrated emulsions stabilized by colloidal particles with a minimum internal phase volume fraction of 0.74. They have received considerable attention in many fields, including pharmaceuticals, tissue engineering, foods, and personal care products. The aim of this perspective is to update the current knowledge on the field of protein-based Pickering HIPEs, emphasizing those aspects that need to be explored and clarified. Research progress in constructing HIPEs by protein-type colloid particles and promising research trends in basic research and potential applications were highlighted. Promising studies in this field include (1) clarifying bioavailability and evolution of activity of active ingredients in Pickering HIPEs by oral administration, (2) constructing a Pickering interfacial catalysis platform using protein colloidal particles, and (3) expanding the emerging applications of Pickering HIPEs in fields, such as partially hydrogenated oil replacers, probiotic encapsulation, and the template for porous materials.

Lactobacillus reuteri improves gut barrier function and affects diurnal variation of the gut microbiota in mice fed a high-fat diet.

Lactobacillus reuteri FN041 is a secretory IgA-targeted Lactobacillus strain from human breast milk that has probiotic potential. The aim of this study was to test whether FN041 can alleviate dyslipidaemia and mucosal-barrier damage caused by a high-fat diet (HFD) and whether it can affect diurnal variation of the intestinal microbiota. C57BL/6 mice were fed either a normal chow diet or high-fat diet (HFD) for 7 weeks and were treated with either PBS as a control or L. reuteri FN041 for 4 weeks. Our results showed that FN041 treatment significantly attenuated HFD-induced weight gain (P < 0.01), accumulation of testicular fat, an increase in locomotor activity during the active phase (P < 0.01), triglyceridaemia, hypercholesterolaemia (P < 0.05), liver Fas overexpression, and Srebp1c mRNA expression inhibition. Moreover, FN041 treatment improved intestinal epithelial barrier function and induced a daily oscillation-dependent change in short-chain fatty acid production by the gut microbiota. A deeper understanding of the molecular pathways participating in intestinal barrier and microbiota modifications, and changes to lipid metabolism under the influence of FN041, will have important implications by potentially opening new horizons for the development of relevant foods to prevent metabolic disorders and unrelated intestinal diseases.

Fabrication and Characterization of Novel Water-Insoluble Protein Porous Materials Derived from Pickering High Internal-Phase Emulsions Stabilized by Gliadin-Chitosan-Complex Particles.

Pickering high internal-phase emulsions (HIPEs) and porous materials derived from the Pickering HIPEs have received increased attention in various research fields. Nevertheless, nondegradable inorganic and synthetic stabilizers present toxicity risks, thus greatly limiting their wider applications. In this work, we successfully developed nontoxic porous materials through the Pickering HIPE-templating process without chemical reactions. The obtained porous materials exhibited appreciable absorption capacity to corn oil and reached the state of saturated absorption within 3 min. The Pickering HIPE templates were stabilized by gliadin-chitosan complex particles (GCCPs), in which the volume fraction of the dispersed phase (90%) was the highest of all reported food-grade-particle-stabilized Pickering HIPEs so far, further contributing to the interconnected pore structure and high porosity (>90%) of porous materials. The interfacial particle barrier (Pickering mechanism) and three-dimensional network formed by the GCCPs in the continuous phase play crucial roles in stabilization of HIPEs with viscoelastic and self-supporting attributes and also facilitate the development of porous materials with designed pore structure. These materials, with favorable biocompatibility and biodegradability, possess excellent application prospects in foods, pharmaceuticals, materials, environmental applications, and so on.

Cellular Uptake and Intracellular Antioxidant Activity of Zein/Chitosan Nanoparticles Incorporated with Quercetin.

In this work, zein/chitosan nanoparticles (ZCPs-Q) were developed for encapsulating quercetin to overcome its lower water solubility and instability, and to concomitantly enhance its cellular uptake and intracellular antioxidant activity. This strategy enhanced quercetin solubility 753.6 and 9.95 times in water and PBS (7.4), respectively, and quercetin encapsulated in ZCPs remained stable after UV irradiation and heat treatment. ZCPs-Q could significantly attenuate AAPH induced erythrocyte hemolysis through the inhibition of ROS generation. It restored intracellular antioxidant enzyme (SOD and GSH-Px) activities to normal levels and inhibited intracellular malondialdehyde (MDA) formation. Simultaneously, ZCPs-Q showed a strong antioxidant activity in HepG2 cells with an EC50 value of 31.18 µg/mL, which was lower than free quercetin's 41.02 µg/mL. ZCPs enhanced the uptake efficiency of quercetin in Caco-2 cells, which contributed to the improvement of cellular antioxidant activities (CAA) evaluated with the CAA assay and AAPH-induced erythrocyte hemolysis assay. The designed route is particularly suitable for the encapsulation of water-insoluble nutraceuticals and for enhancing cell uptake and CAA.

Fabrication of Zein/Pectin Hybrid Particle-Stabilized Pickering High Internal Phase Emulsions with Robust and Ordered Interface Architecture.

Diets containing partially hydrogenated oils (PHOs) expose the human body to trans fatty acids, thus endangering cardiovascular health. Pickering high internal phase emulsions (HIPEs) is a promising alternative of PHOs. This work attempted to construct stable Pickering HIPEs by engineering interface architecture through manipulating the interfacial, self-assembly, and packing behavior of zein particles using the interaction between protein and pectin. Partially wettable zein/pectin hybrid particles (ZPHPs) with three-phase contact angles ranging from 84° to 87° were developed successfully. ZPHPs were irreversibly anchored at the oil-water interface, resulting in robust and ordered interfacial structure, evidenced by the combination of LB-SEM and CLSM. This situation helped to hold a percolating 3D oil droplet network, which facilitated the formation of Pickering HIPEs with viscoelasticity, excellent thixotropy (>91.0%), and storage stability. Curcumin in HIPEs was well protected from UV-induced degradation and endowed HIPEs with ideal oxidant stability. Fabricated Pickering HIPEs possess a charming application prospect in foods and the pharmaceutical industry.

Development of Pickering Emulsions Stabilized by Gliadin/Proanthocyanidins Hybrid Particles (GPHPs) and the Fate of Lipid Oxidation and Digestion.

This work attempted to engineer emulsions' interface using the special affinity between proline-rich gliadin and proanthocyanidins (PA), to develop surfactant-free antioxidant Pickering emulsions with digestive-resistant properties. This binding interaction between gliadin and PA benefited the interfacial adsorption of the particles to corn oil droplets. Pickering droplets as building units assembled into an interconnected three-dimensional network structure, giving the emulsions viscoelasticity and ultrastability. Oxidative markers in Pickering emulsions were periodically monitored under thermally accelerated storage. Lipid digestion and oxidation fates were characterized using in vitro gastrointestinal (GI) models. The interfacial membrane constructed by antioxidant particles served as a valid barrier against lipid oxidation and digestion, in a PA dose-dependent manner. Briefly, lipid oxidation under storage and simulated GI tract was retarded. Free fatty acid (FFA) fraction released decreased by 55% from 87.9% (bulk oil) to 39.5% (Pickering emulsion), implying engineering interfacial architecture potentially benefited to fight obesity. This study opens a facile strategy to tune lipid oxidation and digestion profiles through the cooperation of the Pickering principle and the interfacial delivery of antioxidants.

Development and characterization of novel antimicrobial bilayer films based on Polylactic acid (PLA)/Pickering emulsions.

Biodegradable food packaging is sustainable and has a great application prospect. PLA is a promising alternative for petroleum-derived polymers. However, PLA packaging suffers from poor barrier properties compared with petroleum-derived ones. To address this issue, we designed bilayer films based on PLA and Pickering emulsions. The formed bilayer films were compact and uniform and double layers were combined firmly. This strategy enhanced mechanical resistance, ductility and moisture barrier of Pickering emulsion films, and concomitantly enhanced the oxygen barrier for PLA films. Thymol loadings in Pickering emulsion layer endowed them with antimicrobial and antioxidant activity. The release profile of thymol was well fitted with Fick's second law. The antimicrobial activity of the films depended on film types, and Pickering emulsion layer presented larger inhibition zone than PLA layer, hinting that the films possessed directional releasing role. This study opens a promising route to fabricate bilayer architecture creating synergism of each layer.

Development of antioxidant Pickering high internal phase emulsions (HIPEs) stabilized by protein/polysaccharide hybrid particles as potential alternative for PHOs.

We report for the first time the usage of mono-dispersed gliadin/chitosan hybrid particles as a particulate emulsifier for Pickering high internal phase emulsions (HIPEs) development. The hybrid particles with partial wettability were fabricated at pH 5.0 using a facile anti-solvent route. Stable Pickering HIPEs with internal phases of up to 83% can be prepared with low particle concentrations (0.5-2%). The hybrid latexes were effectively adsorbed and anchored at the oil-water interface to exert steric hindrance against coalescence. Concomitantly, the compressed droplets in Pickering HIPEs to form a percolating 3D-network framework endowed the emulsions viscoelastic and self-standing features. The protective effect of Pickering HIPEs on curcumin was confirmed, and the content of primary oxidation products in HIPEs was slightly lower than that in bulk oil. This work opens an attractive strategy to convert liquid oils to viscoelastic soft solids without artificial trans fats, as a potential alternative for PHOs.

Responsive Emulsion Gels with Tunable Properties Formed by Self-Assembled Nanofibrils of Natural Saponin Glycyrrhizic Acid for Oil Structuring.

Saponin nanofibrils assembled from natural glycyrrhizic acid (GA) have been recently shown to be an effective structurant for edible oil structuring. This work showed that the microstructure and mechanical properties of the novel emulsion gels formed by GA fibrils could be well tuned by oil phase polarity. For more polar oils (algal oil), the GA fibrils had a higher affinity to the oil-water interface, showing a faster adsorption kinetics, thus leading to the formation of fine multilayer emulsion droplets with smaller droplet size. Accordingly, the emulsion gels had a denser network microstructure and higher mechanical strength, which should be attributed to the fact that the smaller emulsion droplets could be packed more tightly within the continuous network, providing stronger interdroplet interactions, and thereby contribute to reinforcing the gel matrix. In addition, all emulsion gels had interesting thermoresponsive behavior, independent of oil phase, which is probably due to the thermoreversibility of the hydrogen-bond fibrillar network in the continuous phase.