Structured protein particles in the form of fibers or sheets that form oleogels and macrocolloids to serve as alternatives to fats and thickeners in foods and cosmetics.

Abstract

This disclosure provides protein-dried particles having a specified microstructure with beneficial properties. When combined with an aqueous solution, these dried particles form a macrocolloid with improved thickening and stabilizing properties. When combined with an oil, these dried particles form an oleogel with intrinsic oil-structuring and release properties. The microstructure is in the form of fibrils, sheets, or other particles that are substantially uninterconnected and have a high aspect ratio. These dried particles can be produced by denaturing a protein in an aqueous liquid and organizing the protein by freeze channel formation. The oleogel can be produced by gradually and gently adding a suitable oil so as not to pulverize the microstructure. When heated, the oleogel releases some, but not all, of the oil and forms an emulsion that is spreadable in an aqueous liquid and stable for at least 6 weeks. The oleogel can be used as a substitute for animal fats and tropical vegetable oils in food, cosmetics, and pharmaceuticals. TIFF2026509516000009.tif58170

Description

Technical Field

[0001] Field of Invention This patent disclosure generally relates to reducing environmental impact by using plant-based ingredients as alternatives to animal fats, tropical vegetable oils, and artificial thickeners. Compositions with excellent performance characteristics for use in food and personal care products are provided.

[0002] Related applications This PCT application claims priority to U.S. Patent Application No. 63 / 451,645, filed Mar. 13, 2023; U.S. Patent Application No. 18 / 199,974, filed May 22, 2023; U.S. Patent Application No. 18 / 473,245, filed Sep. 25, 2023; and U.S. Patent Application No. 63 / 552,668, filed Feb. 13, 2024. This application is a partial continuation of U.S. Patent Application No. 18 / 199,974, filed May 22, 2023, and issued as U.S. Patent No. 11,896,687 on Feb. 13, 2024.

[0003] The patents and patent applications listed above are hereby incorporated by reference in their entirety for all purposes.

Background Art

[0004] background Food security, i.e., the reliable access to nutritious food at a safe and affordable price, is closely linked to a predictable climate and a healthy ecosystem. Extreme weather, droughts, fires, and diseases caused by climate change already threaten food production worldwide. Unless we take decisive action, these problems will worsen, and the poorest and most vulnerable people in the international community will suffer disproportionately.

[0005] According to the United Nations Foundation in 2021, global yields of wheat, maize, and other crops have been declining for years due to heat waves and droughts. Some estimates suggest that global agricultural yields could fall by as much as 30% by 2050 unless climate change reverses. Despite decades of efforts to improve global food supply, hunger continues to spread at an alarming rate. A 2019 report found that approximately 750 million people worldwide are undernourished or food insecure, and that number continues to grow.

[0006] Livestock consume a lot of energy, produce enormous amounts of greenhouse gases, and contribute to climate change. Furthermore, the use of solid tropical vegetable oils (such as coconut oil and palm oil) in food negatively impacts the environment by causing deforestation of tropical forests and damaging biodiversity.

[0007] The environmental impact of society can be mitigated in part by reducing the world's reliance on animal fats and tropical vegetable oils in the production of food and other products. Innovators in the food industry are focusing on developing plant-based foods that mimic traditional foods such as meat, fish, eggs, and dairy products. Similarly, the cosmetics industry is taking steps to reduce the content of animal-derived ingredients in cosmetics.

[0008] The texture, flavor, and mouthfeel of meat and dairy substitutes, as well as the moisturizing and cosmetic effects of cosmetics, all function in part due to the thickeners and fats they contain. The improved ingredients provided in this disclosure may be useful in the development of climate-friendly food and personal care products. [Overview of the project]

[0009] overview This disclosure provides protein-dried particles having a specified structure and beneficial properties. When combined with an aqueous solution, these particles form a macrocolloid with improved thickening properties. When combined with an oil, these particles form an oleogel with unique oil-retaining and releasing properties. This product is configured to be used as a substitute for artificial ingredients, oils, structured fats, and tropical vegetable oils in food, food ingredients, cosmetics, and personal care products.

[0010] Dry particles can be produced by a process that involves denaturing proteins in water and performing freeze channel formation to create dispersible microlayers. They exist in high aspect ratio fibrils, sheets, and other forms, which are substantially uninterconnected and therefore free-flowing. Dry particles physically capture and structure the liquid in which they are suspended.

[0011] The oleogels of this disclosure are solid, self-supporting, and possess fat-like properties, thereby releasing oil under shear or heating, similar to traditional animal-derived structured fats. As illustrated below, the oleogels exhibit excellent performance in food systems and cosmetic care products. Oil is released during cooking and chewing, thereby providing the juiciness expected of fat-containing foods. The oleogels are spreadable and, in aqueous liquids, form emulsions that are stable for at least 6 weeks without signs of creaming.

[0012] Technological aspects This disclosure provides proteinaceous dry particles that primarily consist of proteins that are dispersed in either liquid oil or water and form a structuring agent. The proteins may be denatured proteins, typically protein isolates, or mixtures. Some dry particles have a solid microstructure that gives the product special properties. Typically, the microstructure contains fine particles with a median size of one or two dimensions of at least 10 μm. In the dry particles, the fine particles are clustered together in fairly close proximity, but when suspended and diluted in vegetable oil, they are free-flowing and substantially unconnected.

[0013] Therefore, dry particles have two structural aspects: one as fine particles with specific shapes and dimensions that together constitute a microstructure, and another as loosely bound, dispersible aggregates or collections of fine particles that constitute a macrostructure.

[0014] When the macrostructure is gently suspended and diluted in liquid oil or water, it generally disperses, but the individual particles remain substantially intact. In aqueous liquids, dispersed particles generally form macrocolloids, which can cause the liquid to thicken or increase in viscosity. When suspended in high-density liquid oil, the particles may stick together, but when diluted, the particles generally separate and can be characterized separately from one another.

[0015] In aggregate form, the microparticles obtained according to this disclosure are typically overlapping. In this context, “overlapping” means that the microparticles can come together such that each microparticle is positioned beyond the midpoint of the microparticles to its side or above it, thereby forming alternating, intertwined, coplanar, or parallel arrangements. Rounded or pebble-like microparticles cannot do this. The amount of overlap of densely aggregated spheres is approximately 26% of the diameter of each sphere. Overlapping is made possible by the elongated or irregular shape of the microparticles. Each microparticle can be quantified by its aspect ratio. “Aspect ratio” is the ratio of the longest dimension to the shortest dimension of the microparticle. The aspect ratio of a sphere is 1. Microparticles in dry particles or oleogels of this disclosure may have aspect ratios of at least 2, 3, 5, or higher. High aspect ratio microparticles may exist in the form of fibers, sheets, more irregular structures, or combinations thereof.

[0016] The particulate matter according to this disclosure does not need to be substantially interconnected in aggregated or dispersed form. When aggregated, the particulate matter may be in contact with each other and loosely interconnected with material chains. However, such interconnections (if any) are readily broken when the particulate matter is dispersed in water or dispersed and diluted in liquid oil.

[0017] This disclosure provides oleogels and macrocolloids containing such fine particles, which are typically, but not necessarily, obtained by dispersing dry particles in liquid oil or water. The oleogels of this disclosure may be independently characterized by their structural and physicochemical properties, by the method of their manufacture, by their properties when stored, or by their properties when used in the preparation of emulsions, foods, personal care products, pharmaceuticals, and other industrial products.

[0018] This disclosure provides foods, food ingredients, cosmetics, personal care products, pharmaceutical fillers and encapsulating means, as well as other industrial products, that contain or are made using the dried particles, macrocolloids and oleogels mentioned above.

[0019] This disclosure provides several procedures for producing dry particles, macrocolloids, or protein oleogels. In one approach, the production process involves hydrating and solubilizing a mixed isolate of plant proteins in an aqueous solvent, typically forming a gel. The proteins (if water-soluble or reactive) may be denatured by any preferred means, such as a low (acidic) pH and / or heat. A typical subsequent step is to perform freeze channel formation on the proteins to form a protein powder containing a matrix having a solid microstructure. Freeze channel formation can be performed, for example, by flash freezing and removing water by vacuum. Freeze channel formation is thought to facilitate the arrangement of denatured proteins and the formation of a desired microstructure.

[0020] To prepare an oleogel, the process is continued by gently adding oil or an oil mixture (optionally containing some water and other components) to the dry protein in a manner that disperses the fine particles without substantially grinding, destroying, or otherwise damaging them, until the desired protein-to-oil ratio is reached. The procedure described above can be used to prepare the dry particles, macrocolloids, and oleogels detailed above, or for any other suitable purpose.

[0021] The present disclosure also provides methods for using the dry particles, macrocolloids, and oleogels of the present disclosure for specific purposes. For example, the dry particles can be used for thickening, stabilizing, or modifying the mouthfeel of foods or ingredients. Protein oleogels can be used to modify the perceived firmness, juiciness, greasiness, and / or flavor of foods or ingredients, or to increase the creaminess of personal care products and improve therapeutic and cosmetic functions.

[0022] Advancements that surpass previous technologies The technologies presented in the present disclosure have important new properties. The high aspect ratio of the microparticles in both the dry particles and the oleogels of the present disclosure contributes to their excellent behavior when used in food products and other industrial products. The owner of the technology hypothesizes that due to the high aspect ratio of the microparticles, the microparticles can be suspended close to each other in liquid oil and constitute an effective structuring agent, but are not substantially interconnected, so the microparticles may slide past each other, thus imparting lubricity or a creamy feel to the oleogel and excellent oil retention and release properties.

[0023] As described below, the microstructures of previous protein oleogels do not have these properties. The prior art microstructures are either large solid blocks and honeycombs or microparticles like small rounded pebbles. This is an important difference from what is described herein. Solid microstructures impart a gritty viscosity to foods, while rounded microparticles readily release oil during storage or early in the cooking process.

[0024] Unit of invention The dry particles and oleogels of the present disclosure are separately claimed, but share common inventive qualities related to the solid microstructure, such as the ability of the microparticles to overlap when grouped together, the microparticles having a high aspect ratio, and the quality that the microparticles are not substantially interconnected and / or are free-flowing. These qualities impart special properties to products when used in foodstuffs and other products, as presented below and as described in the appended claims.

[0025] The products of the present disclosure are not bound by a particular manufacturing method, but the processes of the present disclosure provide a suitable and convenient method for obtaining dry particle preparations and oleogels with special properties. The freeze channel formation and other methodologies presented in the present disclosure facilitate the formation of the solid microstructure in dry particles and oleogels.

[0026] Terms, scope, and patent terminology The protein particles or dry particles of the present disclosure are preparations of solid proteinaceous particles that are dispersible in an aqueous liquid to form a macrocolloid and / or in a liquid oil to form an oleogel. The preparation of the proteinaceous particles mainly comprises a protein that is denatured or otherwise configured such that it forms at least partially a dispersion (not a solution) in the liquid in which it is suspended.

[0027] A "macrocolloid" is mainly composed of particles typically in the range of 0.1 to 100 μm in diameter, suspended in water or an aqueous liquid. The macrocolloid may have a distinguishable structure such as a gel network, a foam structure, or an emulsion droplet. The particles in the macrocolloid may be aggregated or dispersed in a continuous medium. This structure may stabilize the protein in the liquid, thereby making the particles less likely to sediment. The macrocolloid exhibits macroscopic properties such as viscosity, elasticity, and flow behavior due to the interaction between large particles. Examples include gels, emulsions, foams, and suspensions used as food additives, skin care products, and drug delivery systems.

[0028] As used in this disclosure, the term “oleogel” has its usual meaning. It generally refers to a semi-solid or solid-like material formed by a solid network of self-assembling molecules or oleogelating agents, such as proteins or other polymers, which can immobilize liquid oils within their structure, resulting in a semi-solid or gel-like viscosity. Semi-solid materials are flexible, viscous, and spreadable, but do not flow into narrow streams. The network provides structural stability to the liquid oil phase, allowing it to maintain its form and texture at room temperature. When cooked, the network typically remains, and the oleogel softens and / or releases some of the oil contained therein. Protein oleogels may be characterized as structured proteins dispersed, distributed, or spreading in a liquid oil phase, or as compositions or colloidal systems in which oil or an oil mixture is dispersed within a protein and / or the oil or oil mixture is structured by the protein. These descriptions have similar meanings and are generally interchangeable (depending on the context).

[0029] The oil-protein compositions of this disclosure can be characterized or defined by any of the following: (1) by the microstructure of the proteins contained therein; (2) by the method of manufacture; or (3) by the performance characteristics of the composition once prepared. The compositions can also be characterized by any two of these criteria, namely, by microstructure and manufacture, by microstructure and performance, or by microstructure and performance, or by all three criteria in combination. Similarly, the methods of this disclosure can be characterized or defined by the steps performed, and / or by the characteristics of the oleogel produced thereby, for example, by the microstructure of the oleogel immediately after production and / or immediately after incorporation into a food or cosmetic product, and / or by the performance of the oleogel.

[0030] In this disclosure, the term “protein oleogel” means a composition in which protein is dispersed in a liquid oil phase, or oil dispersed and permeated within a protein framework. Protein oleogels provided in this disclosure often have a total protein or oleogelating agent protein to oil ratio of at least 2:98 and up to 40:60 by weight. More typically, protein oleogels have a protein to oil ratio of 2% to 40%, up to 20% to 80%, 5% to 95%, up to 15% to 85%, or an average of 5% to 95% by weight. An oleogel may be characterized as a protein oleogel if at least 30%, 50%, 70%, or 90% of the non-oil composition is protein, and / or if the oleogel is manufactured using a protein isolate as the main component.

[0031] The oleogelating proteins that give structure to the oleogel are typically, but not necessarily, protein mixtures or isolates. Alternatively, the proteins used to structure the oleogel may essentially consist of, or contain, single or multiple proteins produced by recombinant expression. A suitable mixture isolate contains a median protein molecular weight of 5–75 kDa or about 10–50 kDa and optionally has an acidic isoelectric point (pH ≤ 5). An example is a protein isolate from potato containing patatin and / or protease inhibitors, such as fractions of Solanic® 200 or Solanic® 300 produced by Avebe (Veendam, Netherlands). See International Publication No. 2018 / 183770.

[0032] The oil may be any oil or oil mixture that is liquid at room temperature or when heated. It may contain fatty acids or other fatty structures in unsaturated or saturated forms. Examples are provided in later sections of this disclosure. The oleogel composition may contain other solid components or solutes, such as crystalline carbohydrates, maltodextrins, or polysaccharide derivatives, that contribute to the oleogel by, for example, helping to form or stabilize the microstructure of proteins. The composition is typically produced and / or stored in a form that is substantially free of water or aqueous solvent, i.e., less than 3% (wt / wt), preferably less than 1%. This may then be combined with aqueous solvents, oils, solids, other components, and combinations thereof for analytical purposes or in the process of manufacturing industrial products therefrom.

[0033] The proteins in the dry particles, macrocolloids, or oleogels of this disclosure are often plant proteins, but are not necessarily so. Alternatively, the proteins may be animal-derived proteins or proteins naturally produced by microorganisms. The proteins are typically denatured. This means, at a minimum, that the proteins, when combined with a liquid, form some suspension, macrocolloid, dispersion, or other heterogeneous phase rather than a solution. This typically means that the proteins no longer possess the quaternary, tertiary, and / or secondary structures present in their native state. As a result, the proteins generally lose enzymatic activity or other inherent function. Denaturation may be achieved by the application of some external stress or compound, such as strong acids or bases, concentrated inorganic salts, organic solvents such as alcohols, stirring, radiation, heat, or a combination thereof. Proteins in oleogels can be denatured during isolation from plants prior to oleogel production and / or during the oleogel production process (e.g., by lowering the pH and heating the solubilized protein isolate). Denatured proteins tend to have reduced solubility in aqueous solvents and liquid oils, and are more likely to form stable microstructures in oleogels.

[0034] At least a portion of the proteins in dry particles or oleogels, at room temperature, form or exist as microstructures that tend to decrease the viscosity and / or increase the hardness of the oil in which they are dispersed. At least 10%, 20%, 30%, 50%, 70%, or 90% (wt / wt) of the protein content in macrocolloids or oleogels may be part of the microstructures. The contents of the protein microstructures (wt / wt) are at least 30%, 50%, 70%, or 90% protein, with the majority of the remainder typically being other components of the protein isolate used in the production of oleogels.

[0035] The microstructure has dimensions and properties that impart beneficial thickening or oil retention and release properties to the macrocolloid or oleogel, as described in the following and subsequent sections. For example, oleogels are solid at room temperature but have a flexible or spreadable texture. They can retain oil when stored at 4°C or room temperature. The term "spreadable" means that at room temperature, they can be spread freely and fairly uniformly onto a normal slice of bread using a normal butter knife, without excessive effort and without substantially deforming the slice of bread. When heated, oleogels gradually become fluid and / or release some, but not all, of the oil (typically 20%–30% and 60%–80%) when cooked. This is in contrast to saturated fats and hydrogenated fats, which are solid at room temperature but rapidly melt when heated to their transition point.

[0036] The oil-retaining capacity of oleogels at different temperatures can be evaluated by determining their melting curves, as shown in Figure 4. Depending on their intended use, the melting curves of oleogels have a downward slope that is not as steep as that of coconut oil. The melting curves of oleogels can demonstrate that when heated to typical cooking temperatures (e.g., 160-200°C or 300-425°F), oleogels retain some, but not all, of the oil, which is indicated by a curve that bottoms out at these temperatures or a curve that continues with only a gentle downward slope. The residual oil may be 20-80%, 10 or 30-60%, 25-75%, or 40-80% of the oil in the oleogel composition before heating.

[0037] Typically, the microstructure contains particles of a size where one or two dimensions, or all three dimensions, are at least 5, 10, or 20 μm. When suspended and diluted in vegetable oil, the fine particles are not substantially interconnected or irreversibly entangled. This means that microstructure fragments larger than 50 μm or 200 μm in any dimension are rare and constitute less than 10% or 2% by weight of the microstructure. In this configuration, the particles can freely pass or slide next to and between each other. The oleogel (including its suspended microstructure) flows freely when sufficiently diluted. The properties and morphology of the microstructure and its constituent particles can be evaluated, for example, by diluting the oleogel 5, 10, 20, 50, or 100 times in vegetable oil using the dilution protocols described later in this disclosure, and then observing the microstructure by optical microscopy, scanning electron microscopy, or another suitable visualization technique.

[0038] For example, many microstructures contain fibrils having a median size of at least 10, 20, or 30 μm in length and a diameter typically at least 0.5 μm but less than 2, 3, or 4 μm. The term "fibril" refers to any long, thin shape, which may or may not be rod-shaped, ribbon-shaped, hollow, or fibrous. Fibrils may be free-standing, branched, and / or clustered or entangled to form aggregates. In the case of branched structures, length is defined as the longest straight-line length of the structure's three dimensions.

[0039] Alternatively, the microstructure may contain sheets. The sheets may have a median size with a length and width of at least 10 or 20 μm and a thickness typically of at least 0.2 or 0.5 μm but less than 2, 3, or 4 μm. They may be folded, wavy, or compressed together. Alternatively, the microstructure may have rounded, faceted, or amorphous particles. Such particles may originate from protein isolates used to prepare the oleogel, may arise during the production of the oleogel, or may be formed by grinding, sonicating, or otherwise dispersing larger, less malleable, or more rigid or interconnected microstructures initially generated during production. To provide desirable oil retention and release properties, the particles are often designed to flow passing each other by having a high median aspect ratio (diagonal length to thickness) of at least 2, 3, 5, 7, 10, or 15.

[0040] Oleogels having the above composition, oleogels manufactured as described below, or oleogels having the desirable properties presented throughout this disclosure can be used in the preparation of food or ingredients, or cosmetic or personal care products. This can reduce the reliance of such products on animal fats and other refined products, thereby mitigating at least some of the impacts of climate change.

[0041] The descriptive terms used as guidelines for the proportions of components or preparations are as follows: “part” means at least 10% or 20%, “majority” means more than 50%, and “substantially all” means at least 90%, where the remaining components making up 10% or less do not substantially affect the performance characteristics of the mixture or product. Unless otherwise specified, proportions are given in units of (wt / wt).

[0042] Specific aspects, aspects, properties, and characteristics of the dried particles and oleogels of this disclosure, as well as their manufacture and use, are described and illustrated in subsequent sections.

[0043] trademark Oleogels having the characteristics described herein and / or oleogels manufactured by the processes presented herein may be referred to in this disclosure and elsewhere as OleoPro®, a trademark of Shiru Inc. of Alameda, California. [Brief explanation of the drawing]

[0044] [Figure 1]Figure 1 shows optical micrographs of two different oleogel preparations having plant protein microstructures according to this disclosure. The scale bar at the bottom of each panel represents a length of 20 μm. Panel (A) shows a preparation prepared by flash-freezing a 1% (wt / wt) solution of denatured plant protein, then drying it, and combining it with high-oleic sunflower seed oil. Fibrils, branched fibrils, and fibril clusters or entanglements are shown in this field of view. Panel (B) shows another preparation prepared in substantially the same manner, except that the denatured protein solution was flash-freezed at a concentration of 5% (wt / wt). This field of view includes a protein sheet. Lines sloping upwards indicate sheet folds and embedded fibrils. The images were obtained by diluting one of each of the two oleogel preparations with 10% vegetable oil. The microstructures of both types contain one or two particles that are at least 10 μm in size but are substantially uninterconnected and free-flowing. This contributes to the oil structuring and retention properties that make these oleogels suitable as substitutes for animal-derived fats and oils. [Figure 2A] Figures 2A and 2B are SEM images of dried particle preparations prepared using potato protein and whey, respectively. Each row in Figure 2A represents a different preparation. The left and right images in each row are at magnification levels of 200x and 1000x. The images show wavy or ridged plates and discontinuous fibril characteristics with little interconnection. The two rows in Figure 2B are two internal regions of the same particle aggregate at magnification levels of 200x and 1000x. There are loosely connected plates with fibril characteristics and a high aspect ratio. [Figure 2B] Refer to the explanation in Figure 2A. [Figure 3-1]Figure 3 is a compilation of fitted micrographs from publications reporting previous protein oleogels. Images from references (A), (C), and (D) show mesh and honeycomb-type microstructures. Images from references (B), (E), and (F) show pebble-like solids and circular or elliptical microaggregates, or aggregates thereof, and therefore have an aspect ratio (length to thickness) of 2 or less. None of the previous protein oleogels have any fibrils or sheets like those shown in Figure 1, and as a result have poor oil retention and release properties. [Figure 3-2] Refer to the explanation in Figure 3-1. [Figure 4A] Figure 4A is a flowchart that provides an overview of the procedural steps that can be used to optimize the production of oleogels according to this disclosure. [Figure 4B] Figure 4B is a flowchart showing one possible method for producing an oleogel having the microstructure shown in Figure 1. The starting protein isolate is hydrated and solubilized, then acidified and heated to denature the protein. A clear, chain-like gel is formed. This is blended, flash-frozen, and dried to form a powder. To preserve the original microstructure and form an oleogel, oil is gradually added to the prepared powder. [Figure 4C] Figure 4C shows melting curves comparing two determined values ​​for each of the two different protein oleogel preparations according to this disclosure, prepared using coconut oil. The curves obtained for some of the oleogel preparations show a gentle downward slope, indicating that a considerable proportion of the oil is gradually released as the preparation is heated to cooking temperatures. The curves do not drop completely to zero because not all of the oil is released. After heating, some oil remained in the protein structure. [Figure 5-1]Figure 5 shows the quantitative analysis of the oleogel microstructure shown in Figure 1. Detail areas A1, A2, A3, and A4 are representative fibrils or ribbons measured by comparing the detail areas of the images with a 20 μm scale bar. The total length (including branching) from end to end ranged from 12 to 35 μm. The diameter ranged from 1.7 to 3.0 μm. The aspect ratio (length to diameter) ranged from 9 to 21. Detail areas B1, B2, B3, and B4 are representative plates of different shapes. The length or height ranged from 19 to 88 μm, and the width ranged from 18 to 42 μm. For a thickness of 2 μm, the aspect ratio (length to thickness) ranged from 10 to 44. [Figure 5-2] See the explanation in Figure 5-1. [Figure 5-3] See the explanation in Figure 5-1. [Figure 6A] Figure 6A shows a five-point scale for subjectively evaluating gel characteristics. Protein oleogels prepared using the method described were scored as follows: hardness = 2, lubricity = 4.5, smoothness = 5, and adhesion = 1. Figure 6B presents the subjective data for these criteria as a spider plot. The solid line labeled "Shiru Oleogel 1" was prepared using the manufacturing process outlined above. High values ​​for lubricity and smoothness are prominent. [Figure 6B] Refer to the explanation in Figure 6A. [Figure 7] Figure 7 is a suitable flowchart for iteratively and empirically optimizing process control variables (right column) by measuring perceived properties using internal standards (left column) and material properties (center column). [Figure 8] Figures 8A and 8B show the properties of burger patties prepared using protein oleogel. Figure 8(A) shows weight loss during cooking and mechanically measured hardness. Figure 8(B) shows perceived firmness, juiciness, and greasiness as assessed by a group of trained volunteers. [Figure 9] Figure 9 shows the scale used to evaluate the putty based on perceptual criteria. [Figure 10]Figure 10 is an image showing the spreadable texture of a protein oleogel prepared according to this disclosure. [Figure 11] Figure 11 provides two photographic images comparing test patties made with coconut oil and protein oleogel when heated to cooking temperature. Oil seeped out and bubbles formed in the coconut oil patty (left), but this did not occur in the protein oleogel patty (right). [Figure 12] Figure 12 shows the protein oleogel according to this disclosure, incorporated as a discontinuous layer in a plant-based alternative product for bacon. [Figure 13] Figure 13 shows the visual appearance of three spreadable olive oil preparations. This product is an oleogel containing only pure virgin olive oil, potato protein as an oleogelling agent, and trace components to adjust flavor and color. [Figure 14] Figure 14 shows the visual appearance of the chocolate nut spread. On the right, 1% protein-free particles are included, preventing the oil separation observed in the control sample on the left. [Figure 15] Figure 15 shows the effect of including other elements in the oleogel preparation on its browning properties. [Figure 16] Figure 16 shows the temperature-dependent rheology of the macrocolloids of this disclosure in comparison to methylcellulose and a pure recombinant gelling protein named P44548. [Figure 17] Figure 17 demonstrates the viscosity-enhancing effect of combining protein dry particles with an aqueous liquid to form a macrocolloid. The addition of salt increases viscosity. [Figure 18] Figure 18 shows the appearance of a dried particle-structured emulsion prepared by adding liquid oil to a macrocolloid. [Figure 19]Figure 19 shows the appearance of uncooked plant-based meat dough prepared using methylcellulose (left) or dried particles (right) as a cryogenic binder. These exhibited a more uniform and smoother surface and a relatively lighter color compared to meatballs without a cryogenic binder (center). [Figure 20] Figure 20 shows images of a cosmetic cream containing 48% water, 47% oleogel, 4% olive oil, plus other trace ingredients. From left to right, the images show the freshly prepared cream, the preparation stored at ambient temperature for 10 days, and the cream stored at 50°C for 10 days. All preparations were thick, unseparated, and retained an indistinguishable appearance and texture. [Modes for carrying out the invention]

[0045] Detailed explanation The following sections describe preparations of dry particles, macrocolloids, and oleogels having microstructures that impart beneficial properties.

[0046] The oleogels of this disclosure are stable and possess excellent mechanical properties, making them ideal for use in products requiring semi-solid or solid but meltable viscosity. The dry particles and oleogels are suitable for large-scale production and possess excellent properties for inclusion in processed foods, cosmetics, and personal care products.

[0047] Interrelationship between microstructure, manufacturing method, and functional properties The protein-dried particles and oleogels of this disclosure can be characterized by any one of the following three types of properties, either alone or in combination with one or both of the other properties: (1) the microstructure of the protein, (2) the method of preparation or production, and (3) the physical and sensory properties of the food and other products made therefrom.

[0048] These properties may be characterized separately, but they are practically interrelated. The properties of the macrocolloids and oleogels of this disclosure are properties of the structure of the dried particle preparations, which are a function of, or influenced by, the methodology used in their manufacture.

[0049] Previous oleogels and their use Organogels are a type of gel consisting of a liquid organic phase within a structured network. Oleogels are organogels that have oil as their organic phase. Oleogels are lipophilic liquid-solid mixtures in which a solid lipid material (oleogelating agent) (<10 wt%) encapsulates and solidifies bulk liquid oil (typically a mixture of edible fatty acids) through a network of oleogelating agents in the bulk oil.

[0050] The most commonly used structuring agent for oleogels is ethylcellulose, a polysaccharide produced from wood pulp. This is a semi-crystalline derivative of cellulose and can be directly dispersed into edible oils. Its gel-forming ability stems from its hydrophobic properties and semi-crystalline characteristics. To induce gelation, ethylcellulose is heated to 130°C (above its glass transition temperature). Subsequent cooling creates strong intermolecular interactions linked by hydrogen bonds, transforming the one-dimensional polymer chains into a three-dimensional entangled network that traps the oil. (F. Manzoor et al., Food Hydrocolloids for Health, Vol 2: Dec. 2022).

[0051] EI Du Pont De Nemours and Company makes the following promising statement about ethylcellulose: Ethocel® polymers are water-insoluble thermoplastic polymers and can therefore be used in a variety of roles. They are used for rheological modification, film formation, bonding, water barriers, and sustained release agents. Also, because Ethocel® exhibits clean burning, it can be effectively used as a sacrificial binder.

[0052] Oleogels are internally structured and can be used as a substitute for structured oils, particularly animal fats, commonly used in processed foods. The field of oleogel research has been very active in recent years, producing products with desirable properties such as heat resistance, texture, and structural stability. Depending on the underlying matrix of the oleogel, it has been shown that foods can develop a texture similar to products conventionally made with hard stock fats, affect nutritional quality, demonstrate high physical and oxidative stability, and exhibit high oil-binding capacity.

[0053] An excellent review by C. Park and F. Maleky (Front. Sustain. Food Syst. 4:139, 2020) provides an overview of oleogels incorporated into various types of foods. Such foods are listed in Table 1 below. Readers should refer to Park's paper for cited publications listing the products listed in the table and the types of oleogels they contain.

[0054] (Table 1) Examples of oleogel application in food formulation TIFF2026509516000002.tif201170

[0055] None of the oleogels listed in Table 1 were prepared using proteins as oleogelating agents. The owners and inventors of the technologies presented herein have developed protein oleogels with superior properties that can serve as substitutes for animal fats and other components in food and cosmetic products.

[0056] The unique microstructure of the oleogel of this disclosure The oleogels according to this disclosure can be characterized as having a microstructure with specific observable properties.

[0057] Figure 1 shows a pair of optical micrographs of oleogel preparations produced by optimized freeze-channel formation, drying, and oil dispersion. The scale bar at the bottom of each panel is 20 μm long. Panel (A) shows the preparation diluted to 1% in oil. Fibrils and fibril clusters or entanglements are visible in this field of view. Fibrils are 30–50 μm long and 1–3 μm in diameter. Fibrils can be solid (rod-like) or hollow tubes with varying degrees of branching. Individual branches, or unbranched structures, are generally 10–50 μm long.

[0058] In addition to fibrils, microstructures in the form of square or irregular sheets can also be observed. Panel (B) shows preparations obtained by flash-freezing and lyophilizing a 5% w / v protein solution, followed by dilution to 1% in oil. Typical sheet structures exhibit a wide range of estimated planar dimensions, from 10 μm × 10 μm (length × width) to over 10 μm × 100 μm. Sheet thicknesses may be less than 2 μm, less than 1 μm, or less than 0.5 μm. Often, as shown in Panel (B), the sheets appear to have a texture embedded with wavy or ridged features.

[0059] Typically, microstructures account for more than 50% of the oleogelating protein or total protein in the composition. Water-insoluble microstructures typically make up about 50% of the lyophilized protein material before oil addition. This can be determined by dispersing the treated protein powder in water, centrifuging at 14 × g for 30 minutes at 24°C, and measuring the soluble protein content in the supernatant using a bicinchoninic acid assay (Thermo Fisher Scientific). When the proteins in the composition are dispersed in oil, they largely associate with microstructures.

[0060] Differences between the microstructures shown herein and the microstructures of previous protein oleogels. The microstructures described herein are novel for protein oleogels. They differ in important respects from the microstructures observed in oleogels previously prepared using proteins as oleogelating agents.

[0061] Figure 3 summarizes the optical images, confocal micrographs, and SEM micrographs adapted from the following previous publications. TIFF2026509516000003.tif91149

[0062] The image in Figure 3 is described in the references listed above as follows: (A) SEM images of whey protein isolate (WPI) at two different magnifications. (B) SEM images of WPI particles at two different magnifications. (C) Optical microscope images of freeze-dried WPI aggregates (top panel) compared with aggregates produced using supercritical drying (bottom panel). (D) SEM micrograph showing serial WPI aerogel produced by freeze-drying (upper panel) or supercritical drying (lower panel). (E) Confocal microscopy observation of aqueous microgel pellets with WPI (upper panel) and the corresponding oleogel prepared with WPI (lower panel). (F) Confocal laser scanning microscope (CLSM) observation of protein aggregates after homogenization using a stator-rotor dispenser (upper panel) or ball mill (lower panel).

[0063] Table 2 compares each reference (column 1) based on the oil structuring mechanism, the starting protein, the colloidal morphology of the protein after heating, and the morphology of the respective microstructures observed in oil (column 5).

[0064] (Table 2) Microstructures of previously published protein oleogels TIFF2026509516000004.tif153169

[0065] As is evident in Figure 3, previous efforts to create mesh-type microstructures (A), (C), and (D), as well as pebble-type microstructures (B), (E), and (F), differ from the fibrils and sheets for the oleogels of this disclosure shown in Figure 1. Without any intention to limit the invention as described herein and claimed, the producers of this invention believe that differences in preparation are the cause of differences in protein microstructure. The oleogels of this disclosure benefit from optimized freeze channel formation, drying, and oil dispersion. For example, in reference (A), water is removed by solvent exchange to avoid aggregation. Excessive aggregation can result in microstructures that are continuously interconnected as solid clumps, or rigid honeycomb-shaped microstructures.

[0066] Microstructure is thought to influence the functional properties of the microgels containing it. Without any limitation to the invention described and claimed in this patent application, oleogels with a pebble-type basic microstructure tend to be semi-soft at room temperature and completely melt when heated. On the other hand, oleogels with a basic microstructure in the form of a large solid mesh or honeycomb tend to be solid at room temperature and remain solid when heated. The data presented in this disclosure demonstrate that the Goldilocks optimal condition is a microstructuring agent primarily consisting of fibrils, sheets, and similar structures with high aspect ratios. These are substantially flat, with one or two dimensions being considerably large but lacking extensive interconnections. Protein oleogels with these microstructures are flexible and solid at room temperature, or spreadable and viscous, and gradually release some, though not all, of their oil content during cooking. The melting curves of protein oleogels with this type of microstructure are discussed in a later section of this disclosure.

[0067] The relationship between microstructure and functional properties can be theoretically detailed as follows: The high surface area provided by the high aspect ratio of the dry particle protein structure can serve as a seed for nucleation of fat crystals, or otherwise contribute to the alignment of aliphatic chains of unsaturated fatty acids, thus increasing intermolecular forces in the oil and resulting in semi-solid material properties. Oleogels produced by directly adding oil to the initial protein isolate without denaturation or drying produce a suspension with poor oil retention and a non-self-supporting (non-solid) structure. In addition to the size and shape of the dry particle protein and microgel, the stiffness of the particles can also affect the mouthfeel due to their tribological (frictional) properties.

[0068] Overview of the manufacturing process for producing protein-dried particles With a few exceptions, mixtures of protein isolates themselves are poorly soluble in water or aqueous solvents. Oleogels containing proteins as oleogelating agents are typically prepared by a multi-step process.

[0069] Previously, some protein oleogels were prepared using an emulsion template approach. High internal-phase Pickering emulsions (HIPE) are formed by first preparing an emulsion using a protein as an emulsifier, and then removing the aqueous phase. Alternatively, protein oleogels were prepared by solvent exchange. First, hydrophilic proteins are dispersed in water, and then the hydrogel is prepared by heat treatment to expose the hydrophobic groups of the spherical proteins. This establishes hydrophobic interactions, resulting in strong physical and covalent interactions that link proteins via disulfide crosslinking. After the network is formed, water is removed stepwise using an organic solvent with moderate polarity to avoid the collapse of the protein network due to any aggregation. After completely replacing the water with the solvent, oil is introduced into the system to obtain an oleogel with less than 1% water. F. Manzoor et al., Food Hydrocolloids for Health, Vol 2: Dec. 2022.

[0070] The owners and manufacturers of this disclosure have developed specific strategies and methodologies for preparing dried particles with beneficial properties. This procedure, when empirically optimized, facilitates the formation of effective oleogel microstructures from which beneficial properties are obtained. The following sequence of steps is recommended for the reader. (1) Hydrate and solubilize the starting protein isolate in purified water; (2) Make the dissolved protein moderately acidic (pH 2-4); (3) Denaturing proteins at a temperature below boiling point for a moderate amount of time (e.g., 30 minutes) that can form a transparent, chain-like gel; (4) Blend the denatured proteins using a high-shear mixer such as an immersion blender or overhead stirrer; (5) Instantaneous freezing (e.g., by spraying onto liquid N2); (6) The frozen protein is dried in a manner that does not disturb the resulting microstructure (for example, by freeze-drying) to form a powder.

[0071] When dry particles are used to prepare protein oleogels, the next part of the procedure is to gradually and gently add oil to the prepared powder in a manner that maintains the preferred microstructure of the particles, including high aspect ratios.

[0072] Figure 4A is a flowchart providing a scheme for evaluating and adjusting the phases of this procedure. The following modifications to the preparation process may be beneficial for forming an oleogel having the perceptual and performance characteristics of this disclosure. Selection of starting protein isolate. Isolates that have some initial microstructure and / or begin to form a microstructure early in the process, for example, those that form a clear, chain-like gel as mentioned in step (3) above, are beneficial. Optimized conditions for gel formation from denatured proteins. The presence of fine, chain-like nanostructures can affect the morphology and associated physical properties of the microstructure during the drying process. Adjusting the pH to 2–4 is helpful. Other factors influencing structure formation that can be empirically optimized include salt concentration, temperature cycling, timing, and other details of this part of the process. ● Optimized freeze channel formation. Instantaneous freezing of gels made from denatured proteins helps minimize ice crystal size. Drying the frozen preparation in a vacuum forms microchannels that serve as passages for water removal. These events promote the formation and solidification of microstructures and preserve any microstructures that have already begun to form. Spraying denatured proteins into liquid nitrogen and freeze-drying at low pressure is effective. In some cases, pellet freezers such as GEA brand nitrogen freezers may be used for scale-up. Another option is microwave-assisted freeze-drying, which reduces drying time and production costs compared to standard vacuum freeze-drying. ● Gradually incorporate oil into dry powder with optimized shear force. The oleogel imaged in Figure 1 was obtained by adding oil dropwise to the powder. Possible alternatives for scale-up include adding oil to the powder by spraying, dropwise, or other means, and then kneading or tumble mixing using a paddle mixer. The oil is added to the microstructure with a calibrated (empirically optimized) shear force.

[0073] Manufacturing process for obtaining dried structured dry particles The particles obtained after drying can be manufactured and distributed as a dried food additive without further processing. The dried product can be added by consumers to oil, suspended in water, or added directly to food (e.g., as a thickener) during manufacturing or cooking. When dried particles are added to water or an aqueous liquid, they generally become macrocolloids with substantially smooth emulsion-like sensory properties. The term "sensory properties" refers to the perceptual characteristics or features of a substance that can be perceived by senses, particularly taste, smell, appearance, texture, and / or mouthfeel.

[0074] Characteristics and Use of Dry Particles in Commercial Products The dried particle preparations of this disclosure contain non-water-soluble proteins. As a result, when added to an aqueous liquid, they form dispersions, suspensions, or macrocolloids that can alter and improve the properties of the product.

[0075] In typical protein suspensions, solid protein particles are dispersed in a liquid medium. However, they typically do not form a stable network and settle from the suspension over time due to gravity. Protein macrocolloids are colloidal systems in which larger, more stable structures are formed by protein aggregates dispersed in a liquid medium. Protein aggregates are more uniformly distributed in the medium and less prone to settling. Protein molecules in macrocolloids interact with each other to form stable networks or aggregates, which contribute to the macroscopic properties of the system, such as viscosity, texture, and stability.

[0076] The types of colloidal structures are as follows: Sol: Colloidal protein particles are dispersed in a continuous liquid medium. The colloidal particles are small enough to remain suspended and do not settle over time. The size of sol particles is typically on the order of nanometers to micrometers. Gel: A gel is a colloidal system in which a three-dimensional network of interconnected colloidal particles is formed in a liquid medium. This network structure gives gels a semi-solid or jelly-like viscosity. Gels are formed by the aggregation, crosslinking, and entanglement of colloidal particles. Emulsions: Protein macrocolloids possess emulsifying properties that allow for the stabilization of emulsion droplets by reducing the interfacial tension between immiscible phases; Foam: A foam is a colloidal system consisting of bubbles dispersed in a liquid or solid medium. The colloidal structure of a foam involves the arrangement of bubbles within a continuous phase, which can be stabilized by surfactants or proteins.

[0077] Macrocolloids prepared using the dried particles of this disclosure can be used as a substitute for thickeners currently used in processed foods, cosmetics, and other products, particularly animal-sourced ingredients, allergens, and artificial ingredients, such as methylcellulose derivatives. Some of the commercially valuable properties of macrocolloids in processed foods include: Texture Improvement: Macrocolloids contribute to the desired texture of food, providing properties such as creaminess, richness, and smoothness that improve mouthfeel and the overall sensory experience; Viscosity control: Macrocolloids influence the viscosity of food products, providing thickening or reducing effects by controlling the flow behavior and viscosity of the product; Stabilization: Helps prevent phase separation, precipitation, or syneresis in food preparations; Moisture retention: Helps prevent drying, extends shelf life, and improves the juiciness and moisture content of the product; Structural support: Helps maintain the shape, volume, and integrity of food during processing and handling; Flavor containment: Protects flavors, aromas, and volatile compounds in food from degradation and dispersion, thereby improving stability.

[0078] Macrocolloidal sheets can contribute to the texture of food by forming layers or coatings. They can act as barriers against moisture, gases, and flavors, helping to maintain freshness and extend shelf life. The sheet-like structure of macrocolloids can stabilize emulsions by forming an interfacial layer between the oil and aqueous phases. Macrocolloids can act as scaffolds or frameworks, holding other components in place. In baked foods, macrocolloidal sheets can contribute to the formation of flaky layers or skins during baking, and in fried foods, they can influence the crispness and texture of the outer coating.

[0079] Macrocolloidal fibers can form networks or matrices that contribute to the thickening and gelling of food preparations, helping to create a smooth, creamy texture and improve mouthfeel. In baked foods, the fibers can contribute to the formation of a fibrous crumb structure, and in meat products, they can influence the texture and mouthfeel of the final product during cooking. Macrocolloidal fibers can also act as fillers or binders in food preparations, helping to improve the texture, viscosity, and yield of processed foods. They impart bulk and volume to products such as meatballs, sausages, and meat substitutes, improving their perceived properties and nutritional profile.

[0080] In cosmetics, macrocolloids can improve texture, enhance stability, retain moisture, control viscosity, induce thickening, gelling, or film formation, and improve the sensory experience.

[0081] A method of combining oil with protein to create an oleogel. Generally speaking, the mixing of oil into protein preparations is carried out in a manner that suspends and separates solid protein particles in a suspension, gently breaking down loosely associated but structurally non-interconnected microparticles. The objective is to minimize pulverization or substantial damage to individual microparticles that have optimal size and aspect ratio.

[0082] The method of adding oil to protein powder may be continuous or discontinuous. In the case of gentle manual or automatic paddle mixing, partial oil addition is carried out in multiple steps, each step involving the addition of a portion of the oil and mixing that portion into the protein before further addition. For example, the combination may be mixed for 1 to 5 minutes between each addition, and complete oil incorporation may be achieved over a total of at least 10 or 20 minutes, up to 30 or 60 minutes, or longer. Alternatively, the oil may be continuously dripped, sprayed, or poured into the powder while mixing, for example, for at least 10 or 20 minutes, up to 30 or 60 minutes, or longer.

[0083] When using a stirring device, the blade shape and flexibility are selected to optimize the maintenance of the microstructure. For stirring and mixing around a vertical axis, hydrofoil blades can provide the gentlest stirring with the least shear force. The blade profile creates a nearly uniform flow with minimal rpm and power input, making it particularly effective for materials that may be damaged by high shear forces. For example, a large-diameter hydrofoil, one-third the vessel diameter, driven at low rpm, is suitable. Marine propellers and axial-flow turbine impellers can also be used as alternatives. The selected mixing speed (in rpm) should be slow and gentle, which will increase the time required to complete the procedure but minimizes the impact on individual particles in the microstructure.

[0084] Alternatively, when using a tumble mixer, select a chamber size that matches the lot size of the preparation to reduce the drop distance and impact in the descending part of the rotating section. In this case as well, the mixing speed (in rpm) should be slow and gentle, which will increase the time required to complete the procedure but minimize the impact on individual particles of the microstructure.

[0085] Depending on the situation (depending on the protein source and desired outcome), protein powder can be added to the oil (rather than the other way around). However, in this case, the buoyancy of the dry protein in the oil must be overcome, which often means more vigorous mixing and greater shear forces. A third alternative is to combine the entire amount of oil and protein at once. After this, gentle mixing at a low turn or slow flow is continued for a mixing time of, for example, 10 or 20 minutes or longer, which helps preserve the microstructure.

[0086] The mixing method is selected from these alternatives and empirically developed to apply an optimized amount of shear force, thereby creating an oleogel containing protein particles dispersed in oil with a microstructure having a high aspect ratio. If the shear force on the proteins during oil incorporation is too high, the particles are unnecessarily crushed or ground to a smaller median size and a rounder shape, resulting in a lower ability to structure the oleogel to have the desired oil-releasing properties. Shear force is a function of shear stress and the time the shear force is applied. The shear stress depends on the method of mixing the powder with oil and the equipment used.

[0087] If the dry protein preparation already contains microstructures that are mostly in the form of high-aspect-ratio fibrils, sheets, or other particles, the amount of shear force is calibrated to minimize the effect on individual particles and break up loose interconnections between particles, but without reducing the median particle size or median aspect ratio of particles to less than half. If the dry protein instead contains microstructures that are mostly in the form of larger solid, mesh-like, or honeycomb-like blocks, the amount of shear force is calibrated differently. In this case, the goal is to break up the protein blocks to result in and maintain particles with median size and median aspect ratio that structure the oleogel to have the desired oil-releasing properties.

[0088] Detailed protocol for preparing dry particles and oleogels Figure 4B is a flowchart of the method currently used at Shiru to prepare oleogels with desired features and properties. When replaced with the Betty Crocker® recipe, the procedure is as follows:

[0089] component: (1) Protein isolate (e.g., potato protein fraction Solanic® 300 from Royal Avebe (Veendam, Netherlands)) (2) Baking soda (3) Vacuum bag (4) Filtered water (5) Food-safe liquid nitrogen (6) Edible vegetable oil (e.g., high-oleic sunflower seed oil).

[0090] procedure: Hydration and Solubilization: Weigh 190 g of potato protein isolate powder into one or two large containers. Add 2.8 L of filtered water to the protein. Stir at 600 rpm on a magnetic stirring plate with a large magnetic stirring rod for at least 20 minutes, or until the solution is no longer opaque and no clumps of protein powder are visible. The resulting suspension is clear and brownish.

[0091] Preparation of protein aggregates: Prepare sous vide (vacuum-packed) of hydrated protein as follows, for example, using an apparatus at Annova (Lewis, Delaware): Cover the sous vide container with a jacket to reduce heat loss during temperature rise and gelation cycles. Fill the sous vide container with 9-10 quarts of liquid. Set the temperature to 92°C and begin preheating.

[0092] While monitoring with a calibrated pH probe, adjust the pH of the hydrated protein to 4 by adding sodium bicarbonate. Add the sodium bicarbonate in small amounts (<0.5g) and allow approximately 2 minutes between each addition to allow pH equilibrium. Once the pH is adjusted and stabilized, place the acidified protein mixture into a souvet vacuum bag and seal it using a vacuum sealer. Typically, this will result in five bags, each containing approximately 500 mL.

[0093] Place the bag into the heated liquid in the souvit container. Start timing when the liquid returns to 92°C (gelling temperature). Maintain this temperature for 30 minutes. Then, remove the souvit bag from the heat and immerse it in ice water for 10-20 minutes. A clear, chain-like gel will form.

[0094] Preparation of high-shear mixture: Combine the clear gel from the soubit bag in a Cambro (or other large food-safe plastic container). Add 500 mL of filtered water to the gel mass. Begin shearing with a high-shear mixer or immersion blender (such as a Breville Control Grip Immersion Blender, combined with an overhead stirrer such as an IKA Microstart, set to at least 10,000 rpm). The resulting solution should be homogeneous throughout. It may appear opaque due to air being incorporated during mixing. If bubbles form on top, allow time for them to settle.

[0095] Flash freezing in liquid nitrogen (LN2): Clean and rinse a Mister sprayer (such as a food-grade Mister of the HeritageQ® brand) with food-safe disinfectant and water. Fill the cryogenic container with liquid nitrogen. Spray the high-shear protein mixture directly into the liquid nitrogen, simultaneously crushing any dry ice particles that may form using a strainer. Once the container is full, collect the frozen beads using a mesh and pour the beads into a labeled container. Repeat spraying and collection as needed. The frozen beads may be stored at this point or placed directly into a freeze-drying tray.

[0096] Freeze-drying / lyophilization: Pack the frozen material from the previous process into trays and place them in a freeze-drying apparatus (such as a Harvest Right freeze-dryer). Start the drying cycle. Once the sample reaches room temperature and the pressure is below 200 MT, remove the dried protein from the freeze-dryer. Disperse into powder as needed. The moisture content at this stage should typically be about 5% or less.

[0097] Oil Incorporation: Carefully place the freeze-dried protein into a large beaker or Cambro container. Gradually begin adding the oil, stirring with a paddle or rubber spatula between additions. The oil should be added to the powder in multiple batches or cycles, with mixing between each addition to combine them. For example, add approximately 25% of the oil at a time, using smaller amounts towards the final addition. Alternatively, the oil can be gradually added to the protein by dropwise or spraying while continuing to mix. To produce the oleogel with the microstructure shown in Figures 1A and 1B, the oil was added discontinuously, with mixing for 1–5 minutes between additions, for a total time of 10–30 minutes until the combination was complete.

[0098] The final mixture is kneaded (for example, by hand or with a rubber spatula) until the mass is homogeneous. This forms an oleogel dough with no visible unevenness in dryness or oil content.

[0099] Properties of proteins used in the preparation of dry particles or oleogels The mixed protein preparations for producing dried particles and oleogels according to this disclosure may have one or more of the following properties. High solubility (well above 5% (wt / vol)) in low ionic strength aqueous buffers or pure water. Isolated compounds with lower median molecular weights or those that have undergone hydrolysis tend to be more soluble; Consistent (lot-to-lot) higher-order protein structures for robust, reproducible hot-onset aggregation and gelation; An appropriate isoelectric point (pI) that allows the protein to remain soluble during the low-pH denaturation process; When heated, proteins form a transparent, fine, chain-like, relatively homogeneous hydrogel network.

[0100] The high water solubility under the relevant processing conditions promotes the formation of a relatively homogeneous transparent gel intermediate, which can then yield an oleogel with a relatively homogeneous protein structure and excellent texture and oil retention characteristics.

[0101] Mixed protein preparations exhibiting high solubility or dispersibility in low ionic strength solutions (aqueous solvents, organic solvents, or binary solvent mixtures) are generally suitable for freeze-structuring, particularly protein dispersions that lack the dense amorphous aggregates on a micron or multimicron scale common to many conventional dried plant protein components. Such proteins may be prepared from plant sources by microfiltration and / or dried by methods intended to maximize dispersibility in solution (e.g., optimized spray drying and / or dry milling or sieving). Protein inputs in solution (protein solutions that have not been dried prior to the freeze-structuring process) may also be suitable.

[0102] Suitable proteins for testing the production of oleogels or structured particles according to this disclosure include: Potato protein isolates in concentrated solution form, shipped and received directly as solutions from manufacturers of commercially available potato isolates: for example, Solanic® 300, commercially available from Royal A``vebe in the Netherlands; Soy protein isolate, available in both microfiltered and highly dispersible powder and liquid solution forms; A highly soluble, chemically modified pea protein isolate, commercially available as a powder for dairy substitute and viscosity enhancer applications; A highly soluble hydrolyzed pea protein isolate with gelling properties; A highly soluble canola protein isolate with gelling properties; Plant proteins, either single proteins or mixtures, produced by heterologous expression and microfermentation.

[0103] Other possible candidates include Rubisco, which is processed from plant leaves as a dry powder or liquid flow and has high solubility and robust gelling properties, and zein, gluten, or other prolamins used in organic solvents or binary solvents.

[0104] Non-plant proteins can be used to produce morphologically similar (but not identical) macrostructures through rapid freezing channel formation. For example, as follows: Whey protein isolates and concentrates can be optionally modified by altering the ratio of major protein components (β-lactoglobulin, α-lactalbumin, bovine serum albumin) and fine-tuning the chemical (disulfide) bonding between proteins, intermediate aggregate / gel density, and long-distance dry particle structure to achieve a wide range of texture outcomes; Dry particulate whey protein with high dispersibility in solution; Other highly soluble / dispersible egg proteins or dairy proteins; Hydrolyzable proteins with high solubility and gelling properties; Non-plant proteins, either single proteins or mixtures, produced by heterologous expression and microfermentation.

[0105] Some aspects of this disclosure may be carried out using recombinantly expressed proteins or mixtures thereof as the primary protein source or additive, as an alternative to mixed protein isolates. U.S. Patent No. 11,439,159 (Hume et al., Shiru Inc.) provides information on how to select individual proteins with the desired function and how to express and test the selected proteins. Specific recombinant gelling proteins are described in PCT / US2023 / 075601.

[0106] In some contexts, the methodologies provided herein can be used to produce oleogels or particles made from non-protein materials. This category of oleogelating agents includes functionalized celluloses such as methylcellulose; food-grade gums such as gellan, carrageenan, and agar; and other food-grade fibers or polysaccharides such as citrus fiber, maltodextrin, pectin, β-glucan, konjac starch, arginate, and chitosan.

[0107] Properties of oils used in the preparation of oleogels The oil phase of an oleogel can be any type of oil or blend of oils suitable for the intended purpose. For use in food, cosmetics, and pharmaceuticals, oils are suitable for human consumption. In this context, oils are typically mixtures of fatty acids and / or fatty acid esters, where the lipids are primarily saturated, monounsaturated, polyunsaturated, or a combination thereof, and are typically unhydrogenated. Examples of suitable oils include canola oil, soybean oil, sunflower oil, olive oil, palm oil, and coconut oil. Suitable oils for personal care products may or may not be characterized as edible, as long as they are safe for frequent ingestion or topical application. Different oils may be filled in different ways, which may affect the properties of the oleogel product.

[0108] The physical and / or sensory properties of the oleogels of this disclosure can be empirically modified and optimized by testing and selecting from various starting protein isolates, by testing and selecting oils, by adjusting the protein-to-oil ratio, and by adjusting the preparation method. In principle, oleogels can be formulated to have a range of desired properties and viscosity, from soft and smooth viscosity (e.g., for use in spreadable foods and cosmetics) to hard viscosity (e.g., for use in plant-based meat substitutes) that releases oil when cooked or remains solid.

[0109] Any protein component or additive to promote microstructure formation The detailed protocol described above facilitates the formation of high aspect ratio (HAR) microstructures through rapid freezing and subsequent freeze channel formation for water removal. To form an oleogel from the dried protein, oil is gently added to preserve structural characteristics.

[0110] Other methods can also be used, such as drying the denatured protein and adding oil. Certain additives promote the formation of HAR microstructures that give the oleogel a desired oil release profile.

[0111] For example, solubilized or suspended proteins may be treated to promote crosslinking between smaller particles before flash freezing and drying of the solution or suspension. Suitable agents include transglutaminases, enzymes that catalyze protein crosslinking between glutamyl and lysyl residues in the protein, and certain oxidases. Other potentially suitable enzymes include laccases, tyrosinases, and peroxidases. M. Motoki et al., Trends Food Sci Technol 9(5):204-210, 1998, NS Sulaiman et al., Int Food Res J 29(4):723-739, 2022. The amount of crosslinking agent and reaction time are set so that the proteins in the preparation can form loose associations of appropriately sized particles and then be optimally dispersed in the subsequent oil incorporation stage.

[0112] The formation of fibrils and related structures can also be promoted by adding additional components to the protein preparation at appropriate times during the procedure. To create complex polysaccharides in the form of fibers, for example, maltodextrin or other polysaccharides can be used by optionally applying a physical process such as needleless ultraspinning. M Gibis et al., Appl. Sci. 2021, 11:7896-7909.

[0113] As an alternative to or addition to freeze-structuring, other upstream pathways for protein microstructuring include alternative solvent evaporation processes and bulk spinning or film casting methods. Y. Shen et al., ACS Nano 2021 15 (4), 5819-5837; DOI: 10.1021 / acsnano.0c08510.

[0114] Other potential additives to be included in the preparation of suitably structured dried protein particles include the following:

[0115] Solubility modifiers (in the thermal gelation process): Low molecular weight molecules (small amounts of salt, sugar, or other osmolites) known to improve protein solubility can facilitate fine-tuning of the gel network structure and subtly influence the oil retention and shear sensitivity of the final dry particle structure. These types of molecules may be naturally present in the components of the particular input or may be intentionally added / optimized to achieve the desired properties.

[0116] Colloidal stability modifiers (for homogenized microgel mixtures): Desirable charge shielding or surface interactions with low molecular weight or other biomacromolecules (proteins or polysaccharides) can reduce undesirable aggregation before freezing. This can reduce the content of low aspect ratio aggregates, which disrupt high aspect ratio structures that form freeze channels, leading to suboptimal shear sensitivity or oil retention properties.

[0117] Colloidal Structure Modifiers (Enzymes, etc.): Chemical or enzymatic modification of homogenized colloidal microgel particles can be used to reduce or enhance specific intermolecular interactions within and between colloidal protein particles. This can be used to adjust the properties of the solution immediately before freezing (e.g., viscosity), as well as to fine-tune the surface properties and porosity or density of the dried particle structure. Partial enzymatic hydrolysis can be used to reduce viscosity or to reduce the overall degree of covalent bonding and / or steric entanglement between particles before freezing. Enzymatic crosslinking can be used to increase viscosity and the overall degree of covalent bonding. In addition to fine-tuning the properties of process intermediates and dried particle structures, this can also affect the texture properties of the final oil-incorporated system.

[0118] Alternatively, the microstructure in the dried particles or oleogel can be enhanced by using oleogel-forming agent components that already have a layered structure. Homogeneous cellular macromolecules are often constructed from repeating units containing high aspect ratio (HAR) particles. For example, fungal mycelium (macroscopic aerogel) contains fungal hyphae (typically 1–10 μm or larger in diameter). After cultivation by liquid or solid fermentation, the fungal mycelium is dried, preserving a porous network of loosely associated HAR hyphae fibrils in a dry state. To produce an oleogel, dried mycelial particles or dried mycelial cubes, each containing a porous network of HAR microparticles, may be immersed in oil, followed by shear dispersion and homogenization.

[0119] Microstructure fine-tuning characteristics Once high aspect ratio (HAR) fibrils or sheets have formed, oil may be added slowly to preserve the structure as much as possible. However, if the user wishes to work with smaller HAR particles, the microstructure particles can be broken down to any desired degree (e.g., by mixing before or after oil addition with greater shear force, or by subjecting the particles to a short grinding and / or sieving process), which will break down the fibrils and sheets and reduce their longest dimensions. Alternatively, dry particles can be broken down by jet, blade, or ball milling, or aggregated oleogels by milling or homogenization.

[0120] Other properties of the microstructure can be modified by adjusting the protein sources and / or additives in the mixture prepared for drying. When used to produce aggregate and dried particle forms, the protein preparations may be functionalized by bioconjugation, enzymatically modified (partially hydrolyzed), or further fractionated to alter the solubility and adjust the surface chemistry of the preparations. For example, adjusting the number of reactive thiols in the protein mixture can alter the long-range (covalent) bonds between proteins in the microstructure, further affecting the density / morphology and shear sensitivity of the final dried particles.

[0121] Another means of modifying the properties of the microstructure is to alter the drying process, for example, by altering the freezing rate and / or packing density of the protein solid. The freezing rate determines the size and morphology of the ice crystal inclusions, which play a role in forcing the protein into a highly interconnected parent structure containing high aspect ratio sheets and fibrils. Modification of the freezing rate can be done by: (1) changing the solute / solvent system that significantly alters the freezing temperature or freezing rate of the solution (e.g., alternative solvent, antifreeze compound, or antifreeze protein); (2) changing the physical droplet size, supply rate, and supply temperature of the solution delivered to the cryogenic bath / surface; (3) altering the cryogenic liquid (alternative liquid cryogenic substance, or stirring / agitation of the cryogenic bath); or (4) replacing the liquid bath with a cryogenic cooling metal surface with high thermal conductivity.

[0122] Image analysis for characterizing microstructures The dried particles and oleogel preparations according to this disclosure can be visually characterized by optical microscopy, confocal microscopy, scanning electron microscopy (SEM), or other techniques for visualizing microparticles in the micron range. Particle aggregates in the dried particles can be imaged as a whole. Individual microparticles can be characterized by imaging them separately and then determining their shape and dimensional measurements.

[0123] The optical microscope images shown in Figure 1 were obtained from protein oleogels prepared according to the protocol provided below. The oleogels were dispersed in a substantially water-free liquid vegetable oil: 0.1 grams of oleogel were mixed with the liquid oil for 1 minute at the highest setting using a benchtop vortexer (Vortex® Genie 2). The resulting suspension was directly imaged with an optical microscope using an oil immersion 100x objective lens.

[0124] Figures 2A and 2B are scanning electron microscopy (SEM) images of dried particle preparations made using potato protein and whey, respectively. To access the interior of the particles, individual dried particle aggregates were gently cross-sectionalized using a razor blade. The samples were mounted on a double-sided copper tape on the SEM stub / stage and sputter-coated with 15 nm platinum. Imaging was performed in low vacuum mode using an FEI Scios dual-beam scanning electron microscope.

[0125] Each row in Figure 2A represents separate preparations of dried particles made from potato protein. The left and right images of each row are at magnification levels of 200x and 1000x. The first row was obtained from a standard benchtop preparation, obtained by flash-freezing and drying a 5% (wt / vol) homogenized gel slurry. The images include plates with discontinuous fibril characteristics and wavy or ridged plates. Interconnection is minimal. The long axes of these structures are generally >100 μm, and the plate thickness is on the order of 1 μm. The second and third rows were obtained from larger preparations, obtained by flash-freezing and drying a 5% (wt / vol) homogenized gel slurry using pilot-scale manufacturing equipment. Loosely connected, high aspect ratio structures are shown. While there are some less aligned fibrils, there are still loosely connected, irregular structures with lengths <100 μm.

[0126] The image in Figure 2B was obtained from particles prepared with whey protein instead of potato protein. Solubilized whey protein isolate (6% wt / vol) was adjusted to pH 6.5, then subjected to thermal denaturation and gelation to produce an optically clear gel intermediate, which was then freeze-dried. The first and second rows are two internal regions of the same particle aggregate at magnifications of 200x and 1000x. There are loosely connected plates with fibril characteristics and a high aspect ratio. The ciliary structures may constitute rare interconnections between the plates.

[0127] The disclosure hypothesizes that the plates and fibrils appearing in the protein oleogel of this disclosure are obtained by dispersing the larger structures shown in the SEM images so that the individual plates and fibrils are separated. When dry particles are gently combined with liquid oil with minimal shear force, the slight interconnections between the microparticles are almost completely broken down, while the sheets and fibrils remain almost intact.

[0128] The dilution protocol used to obtain Figure 1 constitutes an assay for evaluating the characteristics and median aspect ratio of microparticles, either in an oleogel or in dry particles. To prepare particles for analysis, a protein suspension is prepared by gently adding and incorporating liquid oil, taking care not to over-grind or crush the individual microparticles. The oleogel or protein suspension may then be diluted with liquid oil (such as vegetable oil) to sufficiently separate the microparticles, allowing them to be individually characterized and measured. The required amount of dilution is determined empirically, depending on the protein-to-oil ratio in the oleogel or protein suspension and the particle size. Dilutions of the oleogel may be appropriate to 1:2, 1:5, 1:10, 1:20, 1:50, or 1:100, or within those ranges (oleogel to final suspension, in wt / vol). Dry particle preparations may be appropriately suspended and diluted to ratios of 1:50, 1:100, 1:200, 1:500, or 1:1,000, or within those ranges (particles versus final diluted suspension, in wt / vol).

[0129] Image analysis of Figure 1 The superior oil retention and release properties of the oleogels of this disclosure are thought to be due to the function of the microstructure embedded in the oil. Some solid microstructures of previous protein oleogels result in oleogels that are hard, difficult to spread, and do not release oil well when heated or sheared. Some pebble-like or granular microstructures of previous protein oleogels result in oleogels that liquefy at low temperatures and become unstable during storage or when emulsified in water. Oleogels with larger particle microstructures are often gritty and have an unsatisfactory mouthfeel.

[0130] Figure 5 quantifies some of the characteristics observed in the micrographs shown in Figure 1. The fibrils shown in insets A1, A2, A3, and A4 (left) were characterized by outlining the resolved edges of the structure (center) and representing its features with line drawings (right). Measurements were derived from an embedded 20 μm scale bar and performed using pixel-to-micron conversion. The selected structures are micron-scale protein tubes, fibers, or ribbons, with characteristic diameters or thicknesses (T) defining their thinnest dimensions ranging from 0.5 to 5, typically 1 to 3 microns.

[0131] Some of the fibrils in this preparation constituted a single linear segment with a specified length (L). Other fibrils had more complex structures, containing several linear segments of length (L) joined at branching points (indicated by circles in the line drawing). The maximum length (ML) of each branched structure was calculated as the sum of the lengths of the most parallel linear segments, ranging from 10 to 100 μm, longer than 10 microns. The aspect ratio (AR) of each microstructure was calculated by dividing the maximum length (ML) by the diameter or thickness (T). High aspect ratios of 10 to 100 were frequently observed.

[0132] The sheet-like structures shown in insets B1, B2, B3, and B4 were irregular plates with characteristic widths (W) and heights (H) determined as the longest apparent axis of an ideal two-dimensional polygonal structure. In this preparation, W and H ranged from 10 to 100 microns. The plate thickness (T) is assumed not to be greater than the thickness of the fibrils observed in the same preparation or micrograph. In this example, it is approximately 1 to 3 (average 2) microns. The plates may or may not have one or more associated or embedded fiber, tube, or ribbon-like features. Such features are suggested by their simultaneous termination at the edges of a larger continuous structure. Interconnections between plates ("ridges") and between plates and fibrils ("seams") often extended along the width or height of the plates. These extending interconnections are shown by dotted lines in insets B1, B2, B3, and B4. Each plate may be flat, folded, or folded.

[0133] A high aspect ratio (due to the thinness of the fibril or sheet) helps maximize the effective oil absorption capacity (oil-to-protein ratio) of the microstructurer while maintaining a semi-solid lubrication system, which lacks the roughness associated with dispersing low-aspect-ratio protein particles in oil.

[0134] In the microstructure, the proportion of total protein or denatured protein in the preparation is typically between 20% and 100%, with higher proportions (40%, 60%, or more) indicating more efficient use of the protein content for oil structuring and stabilization. Additional proteins, carbohydrates, or other components may be included, for example, to catalyze or promote microstructure formation, to stabilize or preserve the oleogel during storage, as pharmaceutical ingredients, and / or to enhance nutritional value.

[0135] The protein-to-oil ratio in protein oleogel preparations is typically 2:98–40:60 (wt / wt). Ratios of 25:75 or higher generally result in less creaminess and are therefore less desirable in many situations. Lower ratios (5:95, or 3:97–10:90) generally result in more efficient use of protein and are therefore more cost-effective in food production. Lower ratios are also suitable for use with highly saturated oils such as coconut oil and palm oil used in baking, and mango butter used in cosmetics. Saturated oils are generally solid or semi-solid at room temperature but benefit from their incorporation into oleogels to improve their melting and / or oil-retention properties.

[0136] Evaluation of the physical properties of protein oleogels In addition to microstructure, protein oleogels can be evaluated by physical criteria. This allows users to compare oleogels produced by modified procedures, iteratively refine the process, and re-evaluate the resulting oleogels.

[0137] Figure 4C shows melting curves comparing the behavior of coconut oil and two types of protein oleogel preparations (each measured twice). Traditional (non-protein) oleogels can generally retain oil but do not release it, resulting in a waxy or plastic-like viscous material. This is shown as a nearly horizontal line near the top in this type of plot. Protein oleogels with rigid mesh or honeycomb structures are expected to show similar horizontal melting curves. In contrast, unstructured coconut oil melts completely at low temperatures, showing a steep downward curve towards zero. Protein oleogels with mesh structures consisting mainly of pebbles or other small particles are also expected to show similar melting curves.

[0138] The oleogels of this disclosure achieve a satisfactory compromise. They are flexible solids or spreadable at room temperature and release oil upon heating and / or shearing. The curves of some oleogel preparations in Figure 4C show a downward slope, indicating that a significant proportion of the oil they contain is released at typical cooking temperatures. Not all oil is released, so the curve does not drop to zero. After heating to cooking temperatures (160°C ≡ 320°F), some protein material remained.

[0139] The texture of oleogels can be objectively measured using analytical instruments such as the AMETEK® Brookfield CTX Texture Analyzer. Texture profile analysis (TPA) is performed by a double compression test using a 5 kg load cell, deforming it by 50% at 0.5 mm per second. The reading is the peak force during the first compression, reported in Newtons (N). Total work (mJ), chewiness (N), rubberiness (N), elasticity, cohesiveness, and adhesion (mJ) can also be determined. Hardness tends to be the most differentiating measurement. Oleogels can also be characterized by their viscosity at room temperature or when heated.

[0140] Evaluation of the emulsification properties of protein oleogels The emulsifying properties were determined at several stages of the oleogel formation process. The relative proportions of oil, water, and protein were maintained in all samples. The solution of natural potato protein foamed but did not form a stable emulsion and separated quickly. The gelled potato protein solution showed some emulsifying ability, but a considerable portion of the free oil remained, and the mixture separated into two phases. However, the dried particulate protein obtained after denaturation and freeze-drying produced a firm, stable, bright white emulsion.

[0141] The protein oleogels of this disclosure produce stable emulsions without the need for additional stabilizers. The oleogels can be combined with water using medium to high shear forces at a total utilization rate of 40-60%. The oil-in-water emulsion formed thereby is stable at ambient temperature for at least 4 or 8 weeks without any signs of phase separation.

[0142] Emulsions can be destabilized by one of four different mechanisms: creaming or precipitation, cottony precipitation, coalescence, and Ostwald maturation. Creaming occurs when the emulsion separates due to density differences, with lighter oil droplets rising to the surface. Precipitation follows the same mechanism, but typically occurs in water-in-oil emulsions, where denser water droplets accumulate at the bottom of the emulsion. Creaming or precipitation can be prevented by having a highly viscous continuous phase. Cottony precipitation occurs when droplets of the emulsion aggregate to form larger units. Coalescence occurs when smaller droplets combine to form larger droplets. This is due to droplets coming into contact with each other, breaking the interfacial film and causing phase separation. Ostwald maturation occurs when smaller droplets first dissolve into the continuous phase and then coalesce into larger droplets to reach a thermodynamically more stable state. The oleogels of this disclosure are resistant to all forms of such destabilization.

[0143] Evaluation of the perceptual properties of oleogel The sensory properties of oleogels, despite being essentially compositions of proteins and oils, can be systematically evaluated. Standardized methods for evaluating lubricity, smoothness, hardness, and adhesion are described below. These measurements are performed by human volunteers using their thumbs and index fingers. Table 3 outlines the protocol.

[0144] (Table 3) Subjective tests on the sensory properties of fats, oils, and oleogels TIFF2026509516000005.tif81164

[0145] Figure 6A shows a 5-point scale for each of the four evaluations. Each scale is standardized using lard, butter, shortening, coconut oil, and animal fat, as shown. For the protein oleogel preparations prepared according to the protocol described above, the values ​​were as follows: hardness = 2, lubricity = 4.5, smoothness = 5, and adhesion = 1. These values ​​are particularly suitable for food preparation. The oleogel preparations tested here are neither hard nor sticky, but smooth and lubricating.

[0146] Figure 6B presents the test data as a spider plot. The solid line labeled "Shiru Oleogel 1" represents the product prepared using the optimization process outlined above. High values ​​for lubricity and smoothness are prominent. The dashed line labeled "Shiru Oleogel 2" represents an earlier product prepared using a different process that did not involve pH adjustment, modification, or immersion blending.

[0147] Figure 7 is a flowchart for iteratively and empirically optimizing process control variables (right column) by measuring perceived properties using internal standards (left column) and material properties (center column).

[0148] Characterization of food prepared with protein oleogels The sensory properties of oleogels can be systematically determined even when combined with other ingredients in food preparations. Products made using different oleogel preparations can be compared with each other, as well as with products made using fats and oils of more traditional structures.

[0149] Protein oleogels prepared according to the protocol described above were incorporated into cooked patties. The ingredients are listed in Table 4. In this type of study, the use of flavorings is optional. Flavorings were not used here so that volunteers could focus on texture and other subjective characteristics.

[0150] (Table 4) Components of the test putty TIFF2026509516000006.tif60128

[0151] The procedure for preparing the pâté was as follows: Soak the TVP in the first part of water and salt for 30 minutes. Disperse the methylcellulose and soy protein in the melted coconut oil and add additional water to form an emulsion. Add the cornstarch and emulsion to the soaked TVP and mix until incorporated. Cool at 40°F for 2 hours. Shape into 25g pâté and bake at 375°F for 14 minutes.

[0152] Two controls were prepared using oil instead of oleogel. The positive control was 15% coconut oil. The negative control was 5% coconut oil, which was baked for an additional 8 minutes.

[0153] Figure 8A shows graphs of cooking loss (percentage of weight loss after baking) and hardness. Hardness was evaluated using a Brookfield CTX texture analyzer at 40% compression and an internal temperature of 50–70°C. The oleogel patties were compared to two controls: a patty made with 15% coconut oil instead (positive control) and a patty made with only 5% coconut oil and baked for an additional 8 minutes (negative control). Compared to the positive control, the oleogel reduced cooking loss from an average of 17% to 13.6%. The hardness of the oleogel patties (5.5N) was comparable to that of the coconut oil patties (6.3N).

[0154] Figure 9 shows the scale used to evaluate patties based on perceptual criteria. Qualitative Descriptive Analysis (QDA) was performed by a group of 24 trained volunteers to evaluate burger patties for firmness, juiciness, and greasiness. The study was blinded, so the group members did not know which patties were made with oleogel or coconut oil. For each criterion, a standard was established using other products. Standard patties were made with oleogel or with low (5%, Shiru B), medium (15%, Shiru A), and high (20%, Shiru C) levels of coconut oil.

[0155] The results are shown in Figure 8B. The firmness, juiciness, and greasiness scores of the pâté prepared with oleogel ("Shiru alt fat") were rated by the group as being similar to those of the positive control. There was a significant difference compared to the negative control, demonstrating sensitivity to the reaction.

[0156] Figure 10 shows the spreadable texture of a protein oleogel preparation prepared according to this disclosure. This is an anhydrous oleogel. It looks more creamy but is not wet. When mixed with water, the oleogel forms an emulsion which is glossier and has softer edges.

[0157] Figure 11 compares the cooking of test patties made with coconut oil and protein oleogel. The coconut oil patty melted and foamed (left). In contrast, the oil in the oleogel patty remained almost entirely within the patty (right).

[0158] Lipids and oils in commonly used foods that can be replaced with oleogels The oleogels of this disclosure can be used with necessary modifications to serve as a substitute for structured fats and tropical vegetable oils, in particular those that are solid, semi-solid, or spreadable at room temperature but transition to a liquid or softer state when heated, such as beef tallow, pork back fat, lard, other refined meat fats and extracts, coconut oil, palm oil, hydrogenated oils, margarine, other types of shortening, and butter.

[0159] Foods that incorporate protein oleogels The oleogels of this disclosure can now be used in any food that has a substantial oil and / or fat content. Protein oleogels may be used as a partial or complete substitute for animal fats, fats that are considered nutritionally unsatisfactory, or fats that are difficult or expensive to produce. Alternatively, users may want to use the oleogels of this disclosure in food simply because they possess superior properties. Any of the foods listed in Table 1 above can be prepared using the oleogels of this disclosure instead of the oleogels specified in the referenced literature.

[0160] The method of incorporating or generating oleogels into food products may be optimized empirically by the user. As a guideline, the user may wish to start by adapting a known recipe or manufacturing process for a particular processed food, which would involve replacing one or more oils, fats, or oily structures in that recipe or process entirely or partially with oleogels of approximately equal or equivalent mass. For food products such as marbled beef or bacon, this may involve sowing the areas where meat-like proteins and meat-like fats would be incorporated into a scaffold structure to visually and texturally mimic animal products.

[0161] Users may incorporate oleogels into food products in a mass ratio suitable for the desired optimal texture. This depends on other ingredients in the product, whether the product is heated, and the specific protein oleogel used.

[0162] Generally, any concentration between 1% and 90% (wt / wt) of the dry food component may be suitable. The range of 3% or 5% to 80% is more typical. Typical usage ranges for various types of food are as follows: ● Plant-based ground meat substitute: 4-25% (wt / wt) of the product formulation; ● Vegan cake: 10-25% (wt / wt); ●Dairy products: 2-50%; ●Whipped cream topping: 15-45%.

[0163] The protein oleogel preparations of this disclosure can be used to create plant-based alternative foods for meat products, dairy products, and baked foods that are typically made with animal fats or tropical vegetable oils. Protein oleogels can also be used in foods traditionally made with unsaturated vegetable oils for the purpose of improving structure, oil-release properties, or palatability.

[0164] Detailed recipes for using protein oleogel to make plant-based beef-like products, sausages, plant-based chicken nuggets, vegan vanilla cakes, cookies, and plant-based ice cream are provided in U.S. Patent No. 11,896,687, which this disclosure claims as priority.

[0165] Spreadable olive oil prepared as an oleogel The technology of this disclosure can be used to produce spreadable olive oil. Currently available "olive oil spreads" are made by combining oil mixtures, such as olive oil mixed with palm oil, canola oil, and flaxseed oil, with water and emulsifiers such as lecithin. In one embodiment of the technology described herein, a superior product can be produced containing only pure olive oil, a protein structuring agent, and a trace amount of flavor enhancer. The spreadable olive oil of this disclosure has excellent flavor and mouthfeel.

[0166] Table 5 shows the preparation of spreadable olive oil produced at Shiru Food Research Institute.

[0167] (Table 5) Preparation of spreadable olive oil TIFF2026509516000007.tif189131

[0168] The procedure was as follows: Batch A dried particles were produced from a 5% (wt / vol) homogenized potato protein isolate gel slurry using commercially available pilot-scale equipment. Batch B dried particles were produced from a 1% (wt / vol) homogenized potato protein isolate gel slurry using a bench-scale method. Extra virgin olive oil was used. The spread was prepared by gradually adding the oil to the dried protein particles while gently mixing and stirring. After 24 hours, sodium bicarbonate and powdered salt were added as flavor enhancers.

[0169] Both batches produced high-quality olive oil spread products. All preparations from batch B had acceptable outcomes. Preparations from batch A contained more dry particles. Additional structuring was achieved by adding saturated fat in the form of 10% mango butter (A2). Preparations C1, C2, and C3 were prepared using the dry particles from batch A and flavored extra virgin olive oil. The distinctive colors and flavors obtained using truffle-infused and chili-infused oils demonstrate that low molecular weight molecules with desirable sensory properties can be readily incorporated.

[0170] Figure 13 shows the visual appearance of preparations B1, B3, and C2. Higher dry particle content (B3) increases spread firmness and shape formation. The use of truffle infused oil darkens the color. Further improvements to the ingredients and procedures can be made to enhance desirable properties such as a smooth texture, a rich mouthfeel, and product versatility.

[0171] Other spreadable foods Peanut oil spreads containing 5-10% dry protein particles, 1-2% baking soda, up to 1% powdered salt, 65-93% peanut oil, and up to 30% saturated fat (mango butter, cocoa butter, or coconut oil) were prepared at the Shiru Laboratory. The procedure was as follows: Oils and fats were gradually added to the dry particles, with gentle stirring until all oils and fats were incorporated. This combination was left to stand for 24 hours to allow the oils to be incorporated, after which baking soda and powdered salt were added.

[0172] Spread formulations can also be produced by combining protein-dried particles with an oil-rich mixture consisting of natural fats, oils, proteins, carbohydrates, and other components of a ground nut preparation. This helps stabilize the product and prevents separation and oil loss. Using 0.5% dried particles, stabilized almond butter was prepared at Shiru Laboratory as follows: Smooth almond butter was heated to 200°F and mixed with dried particles until homogeneous. A 32g sample of almond butter was stored in a conical flask at 40°C for 6 days, with and without dried particles. The almond butter itself lost 2.0g of oil, while the preparation stabilized with dried particles lost only 1.3g.

[0173] Chocolate nut spread was prepared at the Shiru Laboratory using 61% hazelnut spread, 17% powdered sugar, 8.5% Ghirardelli cocoa powder, 1% vanilla, and 12% sunflower oil. Up to 1% of protein-free particles were added by heating the nut butter to 200°F. Oil separation was determined using the same method as for almond butter.

[0174] The results are shown in Figure 14. The control sample without dry particles (left) had a 2-5 μm layer of separated oil. The sample containing dry particles (right) did not separate.

[0175] Meat substitutes containing oleogel When using protein oleogels as a fat substitute in meat substitute products, it is often appropriate to adjust the texture, flavor, and cooking outcomes to match those of natural meat products.

[0176] Figure 15 shows the browning of oleogel preparations containing various additives. The oleogel was a 95% fat mixture (high-oleic sunflower oil and mango butter) with 5% protein oleogelating agent (wt / vol). Row 1: Oleogel alone, oleogel + glycerin, oleogel + monodiglyceride, oleogel + lecithin, and oleogel + arginine. Row 2: Oleogel emulsion (1% water) + trisodium phosphate, emulsion + citrus fiber, emulsion + xanthan gum, oleogel containing sodium bicarbonate, and emulsion alone. The outcomes were as follows: Moderate browning (samples of sodium bicarbonate, xanthan gum, and citrus fiber), Severe browning (samples of glycerin, diglycerides, lecithin, and sodium phosphate), and Changes in structure / texture (lecithin and trisodium phosphate).

[0177] Shiru Labs created a plant-based alternative bacon by layering a protein meat base with oleogel. The meat base was made with 74% extremely firm tofu (Azamaya), 15% soy protein (FarBest), 7% potato starch (Bob's Red Mill), 1.4% vegetarian pork (Givaudan), 1% κ-carrageenan, plus natural flavor and coloring ingredients. The ingredients were blended until smooth and placed in a -20°C freezer for 1 hour. This was then sliced ​​lengthwise into 1cm sheets, forming layers with sheets of oleogel. The combined product was frozen and sliced.

[0178] Figure 12 (right side) shows the composite product after freezing and slicing into thin bacon slices. The left side shows the product after frying in a pan until browned.

[0179] Other food products produced at the Shiru Institute included: Base sausage or frankfurter: 16-20% textured vegetable protein, 14-20% oleogel, approximately 38% water, 5% lava bean protein, flavors, and colorings in vegetarian casein. Plant-based foie gras: foie gras flavored nut or tofu preparation (appropriately flavored with 50-70% cashew or silky protein base) combined with 30-50% oleogel.

[0180] Preparation and storage of dried particle preparations The dried particle preparations according to this disclosure can be used not only as structuring agents in oleogels, but also as thickeners or stabilizers, added directly to food preparations in their dry form.

[0181] Dry particle preparations for use as dry components or for preparing macrocolloids are prepared in substantially the same manner as dry particles used to prepare oleogels. Dry particles are typically aggregates of fine particles that have come together into larger particles, beads, or aggregates. These constitute the macrostructure of the preparation and, when dispersed in an oil or aqueous liquid, separate into individual high-aspect-ratio fine particles as shown in Figure 1.

[0182] The bulk material can essentially consist of porous, irregular, hemispherical, dry bead-like macrostructures and / or flake aggregates with diameters of approximately 0.1 mm to 10 mm, as determined by mesh sieve analysis. The solid volume of each particle may be reduced by the presence of pores. The macrostructures (both bulk and individual particle-based) absorb both polar liquids (water) and non-polar liquids (oil) when passively immersed.

[0183] The physical structure of dried particles at the macroscopic aggregation level can be tuned by altering the incorporation of air before freezing channel formation. Typically, a certain amount of air is incorporated into the viscous, homogenized protein hydrogel slurry before freezing by physical operations such as mixing, heating, cooling, and spraying. Bubbles remaining in the protein slurry at freezing can create small, spherical adsorption portions in the dried macrostructure. For example, the air content can be intentionally increased by stirring with a high-speed or immersion blender, or by sparging (passing air or gas into a solution). High levels of aeration (e.g., 5% vol / vol) of the protein slurry used to prepare the dried particles can be used to produce stable bubbles that are freeze-dryable. The presence of air content can also act at the microstructural level to promote the formation of high aspect ratio microparticles.

[0184] The dry particle preparation does not need to be immediately solubilized or compounded. It can be stored for long-term use by sealing under a gentle vacuum. For small bench-scale preparations, this can be done using a benchtop vacuum bag sealer (Weston Pro-2600 or equivalent). For larger quantities of material, rigid vacuum containers or drums can be used. The moisture content may be determined by heating a small amount (<2g) of powder sample to 160°C in a halogen-heated gravimetric moisture meter. Generally, a moisture content of 2-9% is useful for extending the storage period and ensuring stable dispersibility in oil or water. When creating a vacuum, care must be taken not to apply excessive force that could disrupt the particle structure.

[0185] Evaluation of the physical properties of protein-free particles and macrocolloids A notable property of the macrocolloids of this disclosure is that their viscosity tends to increase, particularly at high salt concentrations.

[0186] Figure 17 demonstrates this effect. Dried particles made from potato protein were combined with deionized water in a 2 mL microcentrifuge tube. The dried particles were gently dispersed by repeated inversion on a tube rotating device (30-60 minutes). The pH of the resulting solution was 4. The 1.25% dried particle solution (Panel A, left tube) appeared substantially clear, while the 2.5% dried particle solution (Panel A, right tube) appeared homogeneous but slightly turbid. The turbidity is due to the presence of protein particles remaining dispersed in the solution.

[0187] Panel B demonstrates the effect of adding salt (sodium phosphate) up to a final concentration of 20 mM. The aqueous solution (left), which was previously free-flowing and low-viscosity, forms a relatively high-viscosity gel-like slurry (coacervate), as can be seen from the lack of flow in the inverted tube (right). There was also a substantial change in opacity, which indicates the formation of larger dry particle aggregates or networks. When this solution was vigorously stirred for a long time, it became free-flowing again (shear-induced viscosity reduction behavior). This suggests that the association between proteins in the dry particle network is relatively weak and reversible.

[0188] Dry particle coacervates can be prepared by adding a portion of a 5-fold concentrated salt solution (20-100 mM sodium phosphate and / or 50-300 mM NaCl). The same effect can be achieved by adding powdered or crystalline salt. The dynamic salt-dependent gel-like network formation in macrocolloids may be used in food or cosmetic formulations.

[0189] Figure 16 shows the temperature-dependent rheology of the macrocolloids of this disclosure in comparison to methylcellulose and a pure recombinant gelling protein named P44548. Small-amplitude vibrational shear (SAOS) rheology was determined over heating (25°C to 75°C) and cooling (75°C to 50°C). This mimics heating to a typical internal temperature of a cooked burger (75°C) and the temperature at which it is "hot bite" (50°C) following a cooling period, as indicated by the "endpoint".

[0190] A 2% dry particle solution exhibited an initial storage modulus (G') comparable to that of a 2% methylcellulose solution. However, in contrast to methylcellulose, the storage modulus decreased with increasing temperature, dropping to approximately 0 Pa for the remainder of the temperature cycle (cooling data not shown). Upon addition of a thermoinitiated gelling protein (2% P44588) to the solution, the dry particles demonstrated a high initial G' (40 Pa) due to thermoinitiated gelling behavior (G' increases as a function of temperature increase). The two-component system more closely replicated the rheometric profile of methylcellulose than either the dry particles or P44588 alone. The meltback of 2% methylcellulose (decrease in G' during cooling from 75°C to 50°C) is not generally observed in the cooling behavior of most protein gels.

[0191] Foods that incorporate dried protein particles Macrocolloids prepared from dried particles in water can be used to prepare oil-in-water emulsions. Methylcellulose is commonly incorporated as an emulsion into plant-based meat doughs and butters. Macrocolloid-stabilized emulsions can be used instead.

[0192] Figure 18 shows an image of a typical dry particle structured emulsion. It was prepared as follows: 1-10% dry particles were mixed in water for 30 minutes, with occasional gentle stirring (e.g., with a spoon) to hydrate them. The aqueous dispersion was further homogenized using an immersion mixer under moderate shear force. Oil was added and the moderate shear mixing was repeated.

[0193] Figure 19 shows the appearance of uncooked meat mixtures prepared using dry particles as a cryogenic binder. Plant-based meatballs were prepared in a similar manner to the test patties in Figure 11. Meatballs hand-formed using 2% dry particles (right) exhibited a uniform, smooth surface and a relatively light color. This appeared similar to meatballs formed using methylcellulose (left). Meatballs without a cryogenic binder (center) were looser in form, exhibited a coarser texture, and had a darker surface.

[0194] Regulatory approval for dried particles and oleogels as ingredients in processed foods. After confirming that a particular dry particle or oleogel formulation is to be further developed as a food ingredient, the user will ensure that all regulatory requirements are met before commencing commercial distribution. For example, new food additives and their products may be subject to premarket approval by the Food and Drug Administration (FDA) for distribution in the United States. A new additive may be "generally recognized as safe" (GRAS) if there is commonly available and recognized scientific data, information, or methods demonstrating its safety, or if this is supported by voluntary, unpublished scientific data. The notification submitted to the FDA's Office of Food Additive Safety for approval includes a brief description of the substance (chemical, toxicological, and microbiological characteristics), applicable conditions of use, and the basis for determining GRAS. The FDA then evaluates whether the submitted notification provides sufficient grounds for determining GRAS.

[0195] Use of dry particles and oleogels in cosmetics and beauty products The dried particles and oleogels of this disclosure can be tested as substitutes for one or more of the various thickeners, lubricants, emulsifiers, emollients, and other oily and creamy components commonly used as components of cosmetics and personal care products.

[0196] Cosmetics typically contain a combination of main ingredients such as water, emulsifiers, preservatives, thickeners, emollients, colorants, fragrances, and pH stabilizers. Purified water forms the base of almost all types of cosmetics.

[0197] Emulsifiers prevent the separation of hydrophilic and hydrophobic components in a preparation. Many cosmetics are based on emulsions (droplets of oil dispersed in water, or droplets of water dispersed in oil). Emulsifiers are added to alter the surface tension between water and oil, resulting in a homogeneous, well-mixed product with a uniform texture. Common emulsifiers used in cosmetics include polysorbate, laureth-4, and potassium cetyl sulfate. Preservatives are added to cosmetics to extend their shelf life and to prevent the growth of microorganisms such as bacteria and fungi that can degrade the product and, in some cases, harm the user.

[0198] Thickeners are used to give products an attractive viscosity and facilitate their use. Lipid thickeners work by imparting their natural richness to formulations. Examples include cetyl alcohol, stearic acid, and carnauba wax. So-called naturally derived thickeners are polymers that absorb water and swell, increasing the viscosity of products. Examples include hydroxyethylcellulose, guar gum, xanthan gum, and gelatin. Mineral thickeners absorb water and oil to increase viscosity, but the final emulsion will have a different result than gum. Popular mineral thickeners include aluminum magnesium silicate, silica, and bentonite.

[0199] Emulsifiers soften the user's skin by preventing moisture loss. They are used in a wide range of lipsticks, lotions, and cosmetics. A wide variety of natural and synthetic chemicals that act as emollients include beeswax, olive oil, coconut oil, and lanolin, as well as petrolatum (petroleum jelly), mineral oil, glycerin, zinc oxide, butyl stearate, and diglycol laurate. Colorants and pigments are used in many cosmetics to enhance or alter a person's natural skin tone. Mineral components may include iron oxide, mica flakes, manganese, chromium oxide, and coal tar. Natural pigments may be derived from plants, such as beet powder, or from animals, such as carmine, which is often used in red lipsticks. The two most common organic pigments are lake and toner. Fragrances are often added to liquid and cream cosmetics to enhance their appeal.

[0200] Fat is an animal-derived product with a long history of use to soothe and moisturize the skin. It is often an ingredient in cosmetics, personal care products, and soaps. Fat is a refined form of beef or sheep fat and is primarily made from triglycerides containing a combination of saturated, monounsaturated, and polyunsaturated fatty acids. Compositional changes in cosmetics to remove animal-derived materials may involve replacing one or more components, such as tallow, lanolin, squalene, and / or other oils and oil-related chemicals and materials, in any combination.

[0201] The fine particles or oleogels will typically be present in cosmetic or personal care products at concentrations of 0.5% to 80%, 1% to 60%, or 2% to 20% of the weight of the final product, depending on the nature of the product and the desired properties. This includes, but is not limited to, personal care products such as creams, lotions, and balms.

[0202] Body butter and mineral sunscreen having the formulations shown in Table 6 are intended.

[0203] (Table 6) Formulation of Cosmetics TIFF2026509516000008.tif44128

[0204] Potential performance benefits of body butter include reduced moisture loss, increased barrier function, absorption and activation of active proteins, and anti-aging effects on appearance. Potential performance benefits of sunscreen include activity stabilization, increased water resistance to UV irradiation, and extended bioactivity. The selection and amount of specific ingredients may be adjusted by the user to produce a product with the desired texture, scent, color, stability, washability, moisturizing ability, and other factors.

[0205] For example, mango butter is light, non-greasy, and non-comedogenic (does not clog pores). It has antibacterial properties, nourishes acne-prone skin, and reduces sebum production. Mango butter and shea butter can be adapted for cosmetic use by incorporating them into the oleogels of this disclosure as part of an oil mixture in a low protein-to-oil ratio of 2:98 to 5:95 (wt / wt).

[0206] Figure 20 shows an image of a cosmetic cream prepared under Shiru's instructions using an oleogel preparation of 90% sunflower oil and 10% oleogelating protein. This cream contained 48% water, 47% oleogel, 4% olive oil, plus trace amounts of preservatives, antioxidants, and chelating agents. The image shows the appearance of the freshly prepared cream (left), the cream stored at ambient temperature for 10 days (center), and the cream stored at 50°C for 10 days (right). Long-term product stability was confirmed. All creams remained thick, non-separated, and retained an indistinguishable appearance and texture.

[0207] Regulatory approval for dry particles and oleogels as ingredients in personal care products. In the context of this disclosure, the term “Personal Care Products” generally means any article intended to be rubbed, poured, sprinkled, sprayed, introduced, or otherwise applied to any surface or part of the human body for cleansing, beautifying, enhancing attractiveness, or altering appearance, and any thing intended to be used as a component thereof. In the context of this disclosure, “Oleogel” may be a component of a product or ingredient, which is a formulated liquid, cream, gel, emulsion, colloid, powder, or soluble solid, and may optionally be used in combination with a dispensing agent or personal care device.

[0208] Some personal care products and ingredients are regulated as cosmetics by the Food and Drug Administration. The Federal Food, Drug, and Cosmetic Act (FD&C Act) defines cosmetics as “articles intended to be rubbed, poured, sprinkled, sprayed, introduced, or otherwise applied to the human body to cleanse, beautify, enhance attractiveness, or alter appearance.” This definition includes products such as skin moisturizers, perfumes, lipsticks, fingernail polishes, eye and facial makeup preparations, shampoos, permanent wave products, hair dyes, toothpastes, and deodorants, as well as any material intended to be used as a component of cosmetics.

[0209] Some personal care products and ingredients meet both the FDA's definitions of cosmetics and drugs. This can happen when a product has two intended uses. For example, shampoo is a cosmetic because its intended use is to clean hair. Anti-dandruff treatments are drugs because their intended use is to treat dandruff. As a result, anti-dandruff shampoo is both a cosmetic and a drug because it is intended to clean hair and treat dandruff. Other cosmetic / drug combinations include fluoride toothpaste, deodorants that are also antiperspirants, and moisturizers and makeup products marketed as sunscreens. Such products must meet both cosmetic and drug requirements.

[0210] Use of dried particles and oleogels in pharmaceutical products The dried particles and oleogels of this disclosure can be used as part of a pharmaceutical or nutritional supplement by combining, for example, an effective amount of one or more pharmaceutically active substances or nutrients, any components such as a pharmaceutically compatible preservative, and a pharmaceutically or nutritionally compatible excipient, lubricant, diluent, or filler. For example, the product may be in the form of a capsule or a moderately semi-solid for oral administration, or a cream or ointment for topical administration. The oleogel is present in a concentration of 0.5% to 50% or 2% to 20% of the weight of the final product. Users may wish to adjust the salt and pH of the product to stabilize its role in the oleogel and the composition.

[0211] A drug or pharmaceutical product is a composition containing at least one active substance that requires regulatory approval and provides pharmacological activity or other direct effect in diagnosing, curing, reducing, treating, or preventing a disease, or that affects the structure or any function of the human or animal body. A dietary supplement is any substance or ingredient that is advertised as providing health benefits but is not regulated by the U.S. Food and Drug Administration.

[0212] For a drug to be approved by the FDA, its safety and efficacy must be tested in clinical trials or equivalent, and it must be reviewed by the FDA's Center for Drug Evaluation and Research (CDER). A drug is approved if it is determined to provide benefits that outweigh the known and potential risks to the intended population.

[0213] Use of dry particles and oleogels in other industrial products and processes The structured dried particles and oleogels of this disclosure can be used as substitutes for thickeners and other manufactured products, including solid, semi-solid, or structured oils and lubricants.

[0214] For example, oleogel can be used as a component of automotive fuels and lubricants; applied to metal printing plates in the printing industry to impart resistance to acid etching; as an additive to substrates used in polymer banknotes; in the manufacture of candles and other solid fuel sources for the production of heat or light; in the lubrication of steam-driven piston engines in locomotives and steamship engines (oleogel is resistant to emissions); in the steel rolling industry to provide the necessary lubrication when steel plates are compressed by steel rollers; in the lubrication of rifles and other cannons; as a flux for soldering; or in the manufacture and storage of textile products, for example, for strengthening and lubricating threads attached to looms, and for finishing textile products.

[0215] Prior Patent Publications CN 113261594 B (South China Ag. U.) - Rice bran protein oil gel. CN 114190443 A (South China Inst. Technol.) - Preparation of oleogels, comprising dispersing protein powder in oil using ball milling technology. EP 3011836 A1 (Sholten) (Abandoned) - Protein-stabilized oleogel prepared by solvent exchange. US 2022 / 0295811 A1 (Sholten) - Procedure for producing a protein oleogel by suspending a protein in oil and then very slowly adding water. US Patent No. 4,734,287 (N. Singer, John Labatt Ltd.) - Protein product-based. US Patent No. 8,940,354 (Marangoni, Mars Inc.) - Edible oleogel comprising oil, ethylcellulose, and surfactant. US Patent No. 9,655,376 (Ergun, Dow Chemical) - A continuous process for preparing oleogels from ethylcellulose and oily feedstocks. US Patent No. 10,874,115 (Perez Gallardo, Sigma Alimentos) - Edible oleogel comprising an oil or oil mixture, a grease or fat mixture, and a structured material of distilled monoglycerides of saturated fatty acids. WO 2022 / 031172 (Camilleri, BFLike BV) - Oleogel prepared by crosslinking oil and water hydrocolloids using proteins.

[0216] Inclusion by reference Any publications and patent documents referenced herein are incorporated herein by reference in whole for any purpose to the same extent that each such publication or document is specifically and individually indicated as being incorporated herein by reference.

[0217] Interpretation and implementation of this technology While the technologies described above are partially illustrated by certain concepts, procedures, information, and examples, the claimed invention is not limited by these, except with respect to features that are expressly mentioned or otherwise required. The theories presented in this disclosure concerning the formation and behavior of microstructures, and other underlying modes of manufacture, operation, and evaluation of various products and their components, are provided for the interest and potential enlightenment of the reader and are not intended to limit the practice of the claimed invention.

[0218] The dry particles and oleogels of this disclosure were developed by Shiru primarily for use in the manufacture of food and cosmetic products, but they may be used in other circumstances for any reason. The discussion of the microstructure of the dry particles, macrocolloids, and oleogels in this disclosure does not limit the implementation of the invention, the composition of the substances, or the methods claimed as appended, unless expressly stated or otherwise required. For example, an oleogel of the invention produced by the manufacturing process presented herein, or having the beneficial properties presented herein, may or may not have a particular microstructure. An oleogel of the invention containing a particular microstructure may or may not be produced by a particular process. Readers may use any aspect of the technology presented herein for any appropriate or desired purpose.

[0219] Although the present invention has been described above with reference to specific examples and diagrams, modifications can be made, and components can be replaced, to adapt the technology to specific circumstances or purposes of use, as is a matter of conventional development and optimization, and within the scope of the skill of those skilled in the art, thereby obtaining the benefits of the present invention without departing from the scope of the appended claims and their equivalents.

Claims

1. Protein-based dry particles mainly containing proteins that are dispersed in either liquid oil or water and form a structuring agent, The protein is a substantially denatured plant protein isolate or mixture. At least 20% of the dried particles have a solid microstructure, The microstructure is These fine particles, which are substantially overlapping in the dry particles but are free-flowing and substantially non-interconnected when suspended and diluted in vegetable oil, have a median size of at least 10 μm in one or more dimensions. including, Protein-based dried particles.

2. The proteinaceous dried particles according to claim 1, wherein the particles suspended in the oil phase form an oleogel having substantially smooth emulsion-like sensory stimulation characteristics.

3. The proteinaceous dried particles according to claim 1, wherein the hydrated particles form a macrocolloid having substantially smooth emulsion-like sensory stimulation characteristics.

4. A macrocolloidal preparation comprising the protein structuring agent described in claim 1, dispersed in an aqueous phase.

5. A protein oleogel containing a protein structuring agent dispersed in an oil phase, The oleogel has a protein-to-oil ratio of 2:98 to 20:80 (wt / wt), The protein is a substantially denatured plant protein isolate or mixture. At least 20% of the protein dispersed in the liquid oil phase has a solid microstructure. The microstructure is When together, these particles substantially overlap, but when diluted in vegetable oil, they are free-flowing and substantially unconnected, with one or two particles having a median size of at least 10 μm. including, Protein oleogel.

6. The aforementioned microstructure is in the oleogel, It is a solid or semi-solid substance at room temperature and releases some, but not all, of its oil when cooked. Grant and Therefore, the oleogel is deemed suitable as a substitute for animal fats and tropical vegetable oils in food. The oleogel according to claim 5.

7. The product according to any one of the claims, wherein the microstructure is mainly in the form of fine particles having a median aspect ratio (length to thickness) of at least 3 or at least 5.

8. The product according to any one of the claims, wherein the microstructure comprises at least 20% fibrils and / or sheets.

9. The aforementioned microstructure is A fibril having a median size of at least 20 μm in length but less than 4 μm in diameter. The product according to claim 8, including the product described in claim 8.

10. The aforementioned microstructure is A sheet having a median size of at least 10 μm in length and width, but less than 2 μm in thickness. The product according to claim 8, including the product described in claim 8.

11. The oleogel according to any one of claims 4 to 10, wherein the majority of the oil in the oleogel is a vegetable oil mainly containing monounsaturated fatty acids, polyunsaturated fatty acids, or mixtures thereof.

12. The oleogel according to any one of claims 4 to 10, wherein the contained oil is maintained at room temperature and releases 20% to 80% of the oil when heated to 160°C.

13. The oleogel according to any one of claims 4 to 10, wherein when combined in a 1:1 ratio with an aqueous liquid, it forms an emulsion, and the emulsion is stable at room temperature for at least 4 weeks without any signs of creaming or phase separation.

14. An oleogel according to any one of claims 4 to 10, having spreadable viscosity at room temperature.

15. The oleogel according to any one of claims 4 to 10, which is in the form of a storage oil or fat substitute that is substantially free of aqueous liquids.

16. The oleogel according to any one of claims 4 to 10, in the form of an oil or fat substitute constituting at least 5% (wt / wt) of the processed food.

17. The oleogel according to claim 16, wherein the processed food is a hamburger patty or other meat product or a plant-based substitute thereof.

18. The oleogel according to claim 16, wherein the processed food is a spreadable olive oil, nut butter, or chocolate spread.

19. An oleogel according to any one of claims 4 to 10, in the form of an oil or fat substitute constituting at least 5% (wt / wt) of a cosmetic or personal care product.

20. The oleogel according to claim 19, wherein the cosmetic or personal care product is in the form of a cream, ointment, or lotion.

21. A method for producing a protein oleogel according to any one of claims 4 to 10, (a) A step of hydrating and solubilizing a mixed isolate of plant proteins in an aqueous solvent, thereby forming a gel. (b) A step of denaturing the proteins in the gel by heating it to over 80°C at a pH of 4 or lower, and then cooling it. (c) A step of forming a protein powder containing a matrix of denatured proteins having a solid microstructure by performing freeze channel formation on the proteins from step (b), and (d) A step of gradually adding oil or an oil mixture to the powder with a calibrated shear force that disperses but does not pulverize the solid microstructure until a desired protein-to-oil ratio is reached. Includes, This generates a protein oleogel containing the oil dispersed in a protein microstructure, which includes particles having specified characteristics that are substantially not interconnected. The oleogel formed thereby is solid or semi-solid at room temperature and releases some, but not all, of the oil when heated to cooking temperature (160°C). method.

22. The method according to claim 21, wherein the denaturation and cooling in step (b) form a transparent chain-like gel.

23. The method according to claim 21, wherein the freeze channel formation in step (c) is carried out by immersing the protein in liquid nitrogen and drying it in a vacuum.

24. The method according to claim 21, wherein the oil is added to the protein powder of step (d) in at least four portions, with shear mixing in between.

25. The method according to claim 21, wherein the oil is added to the protein powder of step (d) by spraying or dropping the oil onto the protein powder and continuously mixing the oil with the powder for at least 10 minutes.

26. The method according to claim 21, wherein the oleogel produced thereby forms an emulsion when combined in a 1:1 ratio with an aqueous liquid, and the emulsion is stable at room temperature for at least 4 weeks without signs of creaming or phase separation.

27. The method according to claim 21, wherein the oleogel produced thereby has spreadable viscosity when at room temperature.

28. The method according to any one of claims 21, wherein the oleogel produced thereby retains the oil it contains at room temperature and releases 20% to 80% of the oil when heated to 160°C.

29. The method according to claim 21, further comprising the step of producing a food product using the oleogel instead of one or more types of animal-derived fats or oils.

30. The method according to claim 29, wherein the food is a hamburger patty or other meat product or a plant-based substitute thereof.

31. The method according to claim 29, wherein the food is a spreadable oil, chocolate spread, or baked product.

32. The method according to claim 21, further comprising the step of manufacturing a cosmetic using the oleogel instead of one or more types of animal-derived fats or oils.

33. The method according to claim 33, wherein the cosmetic or personal care product is in the form of a cream, ointment, or lotion.

34. A method for thickening, stabilizing, or altering the texture of a food or ingredient, comprising the step of preparing the food or ingredient to contain the protein-dried particles described in claim 2 or 3.

35. A method for altering the perceived firmness, juiciness, greasiness, or flavor of a food or ingredient, comprising the step of preparing the food or ingredient to contain a protein oleogel as described in any one of claims 4 to 10.

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