Compositions comprising alpha-glucan with alpha-1,3 glycosidic linkages

Abstract

Disclosed herein are various aqueous compositions, such as dispersions and emulsions, comprising at least water and alpha-glucan. At least about 50% of the glycosidic linkages of the alpha-glucan are alpha-1,3 glycosidic linkages. Emulsions with enhanced stability are disclosed as examples of such aqueous compositions. Methods are further disclosed for preparing and handling these compositions.

Description

[0001] COMPOSITIONS COMPRISING ALPHA-GLUCAN WITH ALPHA-1 ,3 GLYCOSIDIC LINKAGES

[0002] This application claims the benefit of U.S. Provisional Appl. No. 63 / 674,898 (filed July 24, 2024), which is incorporated herein by reference in its entirety.

[0003] FIELD

[0004] The present disclosure is in the field of polysaccharides. For example, the disclosure pertains to emulsions that comprise insoluble alpha-glucan having alpha-1 ,3 glycosidic linkages, and use of this material in various applications.

[0005] BACKGROUND

[0006] First observed in 1907, Pickering emulsions, based on a stabilization mechanism provided by colloidal particles in the nano- and micro- range, are continuing to gain attention owing to their superior stability at the oil-water interface compared to their traditional surfactant counterparts and their promise as environmentally more benign alternatives vs. typical fossil-based additives. The utilization of biopolymers, including polysaccharides, proteins, and oleosomes, as Pickering emulsion stabilizers has emerged as a promising alternative for emulsion stabilization. These biopolymers offer a range of advantageous properties such as being sourced from renewable feedstocks, biocompatibility, and a desired end-of-life profile typically avoiding the formation of microplastics, making them a viable substitute to traditional surfactants or emulsion control additives. However, using a Pickering emulsion approach has seen slow commercial adoption as typically formulated systems include various additives, contaminants, and other uncontrolled variables (e.g., pH, temperature) that have impacted the potential general applicability of this approach. Further, polysaccharides that have been employed as Pickering emulsion stabilizers are predominantly sourced from cellulose, starch, and chitosan, thereby limiting the ability to tailor materials to meet desired performance ranges.

[0007] Enzymatic polymerization using a glucosyltransferase (GTF) enzyme in isolated systems allows for the tailored connection of glucose monomers (forming glucan) through a range of different glycosidic linkages, and for the production of glucans with varying molecular masses and shapes. Characterized by its linearity, semi-crystalline nature, and water-insolubility, alpha-1 , 3-glucan meets biodegradability requirements, such as biodegradation in soil and marine environments. Even though alpha-1 , 3-glucan can be found as a structural component in cell walls of typical fungi systems, the interesting properties associated with alpha-1 , 3-glucan remain relatively unexplored in scientific research. As compared to other polysaccharides, a generally limited number of reports exist concerning its utilization in applications such as additives in coatings, fillers in co-polymer matrices, and aerogels for absorbents.

[0008] Further work to realize the full potential of using alpha-1 , 3-glucan in various applications is warranted, including its use to stabilize emulsions.

[0009] SUMMARY

[0010] In one embodiment, the present disclosure concerns an aqueous composition with a pH of 12.5 to 13.2 and comprising alpha-glucan, wherein a first fraction of the alpha-glucan is dissolved in the aqueous composition, and a second fraction of the alpha-glucan is not dissolved in the aqueous composition, wherein at least about 50% of the glycosidic linkages of the alpha-glucan are alpha-1 ,3 glycosidic linkages and typically the weight-average degree of polymerization (DPw) of the alpha-glucan is at least 15. In some embodiments, such an aqueous composition further comprises one or more hydrophobic additives.

[0011] In another embodiment, the present disclosure concerns an aqueous composition produced by reducing the pH of an aqueous composition as above that further comprises one or more hydrophobic additives (optionally, such an aqueous composition for pH reduction can be an emulsion), wherein this reduction of pH precipitates the alpha-glucan of the first fraction. In another embodiment, the present disclosure concerns this foregoing method / process of using pH reduction to provide a product.

[0012] BRIEF DESCRIPTION OF THE DRAWINGS

[0013] FIG. 1 : Shown is an overview of methodology for preparing an emulsion as presently disclosed.

[0014] FIG. 2: Solubility curve and DLS (dynamic light scattering) measurements of alpha-1 , 3-glucan. (a) Solubility curve at 1 wt% alpha-1 , 3-glucan loading with respect to pH (shaded area below line represents fraction of alpha-1 , 3-glucan in form of soluble chains). Photographs of glass vials containing alpha-1 , 3-glucan at various stages of preparation are shown as insets 1 , 2 and 3. (b) DLS measurements of 1 wt% alpha-1 , 3- glucan at pH 7.0, which is the preparation shown in Vial 1 . (c) DLS measurements of 1 wt% alpha-1 , 3-glucan at pH 12.9, which is the preparation shown in Vial 3.

[0015] FIG. 3: Dilution pathways through which pH was adjusted from initial value (13.4) to target values while maintaining constant final particle loading (1 wt%).

[0016] FIG. 4: Amplitude sweeps of 1 wt% alpha-1 , 3-glucan dispersions at pH 12.7, 12.9, or 13.1 , after 1 day.

[0017] FIG. 5: Amplitude sweeps of alpha-1 , 3-glucan-containing emulsions at pH 12.7, 12.9, or 13.1 , after 1 day. FIG. 6: Amplitude sweeps of alpha-1 , 3-glucan-containing emulsions at pH of 12.7 or 7.0 (pH neutralized from pH 12.7), or of “as received” alpha-1 , 3-glucan at pH 7.0 (no pH processing), after 1 day.

[0018] FIG. 7: A flow diagram regarding a process of producing highly crystalline alpha- 1 , 3-glucan. Refer to Auxiliary Example.

[0019] DETAILED DESCRIPTION

[0020] The disclosures of all cited patent and non-patent literature are incorporated herein by reference in their entirety.

[0021] The disclosures of all cited patent and non-patent literature are incorporated herein by reference in their entirety.

[0022] Unless otherwise disclosed, the terms “a” and “an” as used herein are intended to encompass one or more (i.e. , at least one) of a referenced feature.

[0023] Where present, all ranges are inclusive and combinable, except as otherwise noted. For example, when a range of “1 to 5” (i.e., 1-5) is recited, the recited range should be construed as including ranges “1 to 4”, “1 to 3”, “1-2”, “1-2 & 4-5”, “1-3 & 5”, and the like. The numerical values of the various ranges in the present disclosure, unless expressly indicated otherwise, are stated as approximations as though the minimum and maximum values within the stated ranges were both proceeded by the word “about”. In this manner, slight variations above and below the stated ranges can typically be used to achieve substantially the same results as values within the ranges. Also, the disclosure of these ranges is intended as a continuous range including each and every value between the minimum and maximum values.

[0024] It is intended that every maximum numerical limitation given throughout this specification includes every lower numerical limitation, as if such lower numerical limitations were expressly written herein. Every minimum numerical limitation given throughout this specification will include every higher numerical limitation, as if such higher numerical limitations were expressly written herein. Every numerical range given throughout this specification will include every narrower numerical range that falls within such broader numerical range, as if such narrower numerical ranges were all expressly written herein.

[0025] It is to be appreciated that certain features of the present disclosure, which are, for clarity, described above and below in the context of aspects / embodiments, may also be provided in combination in a single element. Conversely, various features of the disclosure that are, for brevity, described in the context of a single aspect / embodiment, can also be provided separately or in any sub-combination; i.e., the aspects / embodiments disclosed herein relate, where applicable, to all other aspects / embodiments of the disclosure, even if such applicability is not separately disclosed herein.

[0026] A “glucan” herein is a type of polysaccharide that is a polymer of glucose (polyglucose). A glucan can be comprised of, for example, about, or at least about, 90%, 91%, 92%, 93%, 94%, 95%, 96%, 97%, 98%, 99%, or 100% by weight glucose monomeric units. An example of a glucan herein is alpha-glucan.

[0027] The terms “alpha-glucan”, “alpha-glucan polymer” and the like are used interchangeably herein. An alpha-glucan is a polymer comprising glucose monomeric units linked together by alpha-glycosidic linkages. In typical aspects, the glycosidic linkages of an alpha-glucan herein are about, or at least about, 80%, 81%, 82%, 83%, 84%, 85%, 86%, 87%, 88%, 89%, 90%, 91%, 92%, 93%, 94%, 95%, 96%, 97%, 98%, 99%, or 100% alpha-glycosidic linkages. An example of an alpha-glucan polymer herein is alpha-1 , 3-glucan.

[0028] The term “saccharide” and other like terms herein refer to monosaccharides and / or disaccharides / oligosaccharides, unless otherwise noted. A “disaccharide” herein refers to a carbohydrate having two monosaccharides joined by a glycosidic linkage. An “oligosaccharide” herein can refer to a carbohydrate having 3 to 15 monosaccharides, for example, joined by glycosidic linkages. An oligosaccharide can also be referred to as an “oligomer”. Monosaccharides (e.g., glucose and / or fructose) comprised within disaccharides / oligosaccharides can be referred to as “monomeric units”, “monosaccharide units”, or other like terms.

[0029] The terms “alpha-1 , 3-glucan”, “poly alpha-1 , 3-glucan”, “alpha-1 , 3-glucan polymer” and the like are used interchangeably herein. Alpha-1 , 3-glucan is an alphaglucan comprising glucose monomeric units linked together by glycosidic linkages, wherein at least about 50% of the glycosidic linkages are alpha-1 ,3. Alpha-1 , 3-glucan in some aspects comprises about, or at least about, 90%, 95%, or 100% alpha-1 ,3 glycosidic linkages. Most or all of the other linkages, if present, in alpha-1 , 3-glucan herein typically are alpha-1 ,6, though some linkages may also be alpha-1 ,2 and / or alpha-1 ,4. Alpha-1 , 3-glucan herein is typically water-insoluble (i.e., alpha-1 , 3-glucan is insoluble under aqueous conditions of neutral pH such as pH 7.0).

[0030] The terms “linkage”, “glycosidic linkage”, “glycosidic bond” and the like refer to the covalent bonds connecting the sugar monomers within a saccharide compound (oligosaccharides and / or polysaccharides). Examples of glycosidic linkages include 1 ,6- alpha-D-glycosidic linkages (herein also referred to as “alpha-1 ,6” linkages), 1 ,3-alpha- D-glycosidic linkages (herein also referred to as “alpha-1 ,3” linkages), 1 ,4-alpha-D- glycosidic linkages (herein also referred to as “alpha-1 ,4” linkages), and 1 ,2-alpha-D- glycosidic linkages (herein also referred to as “alpha-1 ,2” linkages). The glycosidic linkages of a glucan polymer herein can also be referred to as “glucosidic linkages”. Herein, “alpha-D-glucose” is referred to as “glucose”.

[0031] The glycosidic linkage profile of an alpha-glucan can be determined using any method known in the art. For example, a linkage profile can be determined using methods using nuclear magnetic resonance (NMR) spectroscopy (e.g.,13C NMR and / or1H NMR). These and other methods that can be used are disclosed in, for example, Food Carbohydrates: Chemistry, Physical Properties, and Applications (S. W. Cui, Ed., Chapter 3, S. W. Cui, Structural Analysis of Polysaccharides, Taylor & Francis Group LLC, Boca Raton, FL, 2005), which is incorporated herein by reference.

[0032] The “molecular weight” of an alpha-glucan herein can be represented as weightaverage molecular weight (Mw) or number-average molecular weight (Mn), the units of which are in Daltons (Da) or grams / mole. In some aspects, molecular weight can be represented as DPw (weight average degree of polymerization) or DPn (number average degree of polymerization). DPw and DPn are calculated from the corresponding Mw or Mn, respectively, by dividing by the molar mass of one monomer unit Mi. In the case of glucan polymer, Mi = 162.14. In some aspects (e.g., oligosaccharides), molecular weight can sometimes be provided as “DP” (degree of polymerization), which simply refers to the number of glucoses comprised within the alpha-glucan on an individual molecule basis. Various means are known in the art for calculating these various molecular weight measurements such as with high-pressure liquid chromatography (HPLC), size exclusion chromatography (SEC), or gel permeation chromatography (GPC).

[0033] As used herein, Mw can be calculated as Mw = ZNiMi21 ZNiMi; where Mi is the molecular weight of an individual chain i and Ni is the number of chains of that molecular weight. Besides SEC, the Mw of a polymer can be determined by other techniques such as static light scattering, mass spectrometry, MALDI-TOF (matrix-assisted laser desorption / ionization time-of-flight), small angle X-ray or neutron scattering, or ultracentrifugation. As used herein, Mn can be calculated as Mn = ZNiMi I ZNi where Mi is the molecular weight of a chain i and Ni is the number of chains of that molecular weight. Besides SEC, the Mn of a polymer can be determined by various colligative property methods such as vapor pressure osmometry, end-group determination by spectroscopic methods such as proton NMR, proton FTIR, or UV-Vis. The terms “particle”, “particulate” and like terms are interchangeably used herein, and refers to the smallest identifiable unit in a particulate system. The term “particulated” and like terms can be used to characterize particles of insoluble alphaglucan herein; particulated insoluble alpha-glucan in typical aspects of the present disclosure is as this material exists when dispersed under aqueous conditions. Particle size in some aspects can refer to particle diameter and / or the length of the longest particle dimension. The average size can be based on the average of diameters and / or longest particle dimensions of at least 50, 100, 500, 1000, 2500, 5000, or 10000 or more particles, for example. Particle size herein can be measured by a process comprising light scattering or electrical impedance change (e.g., using a Coulter Counter), for example, such as described in any of U.S. Patent Nos. 6091492, 6741350, or 9297737 (each incorporated herein by reference). Particle size and / or distributions can be as measured for particles comprised in an aqueous dispersion or emulsion, for example. Particle size herein can optionally be expressed by a “D ”, “D5o”, “D90”, etc. value; for example, a D5o value is the diameter for which 50% by weight of the particles in a composition (e.g., dispersion or emulsion) have a diameter under that diameter, and 50% by weight of the particles have a diameter greater than that diameter.

[0034] A composition herein that is “dry” or “dried” typically has less than 6, 5, 4, 3, 2, 1 , 0.5, or 0.1 wt% water comprised therein.

[0035] The terms “aqueous liquid”, “aqueous fluid”, “aqueous conditions”, “aqueous setting”, “aqueous system” and the like as used herein can refer to water or an aqueous solution. An “aqueous solution” herein can comprise one or more dissolved salts, where the maximal total salt concentration can be about 3.5 wt% in some aspects. Although aqueous liquids herein typically comprise water as the only solvent in the liquid, an aqueous liquid can optionally comprise one or more other solvents (e.g., polar organic solvent) that are miscible in water. Thus, an aqueous solution can comprise a solvent having at least about 10 wt% water.

[0036] An “aqueous composition” herein has a liquid component that comprises about, or at least about, 10, 20, 30, 40, 50, 60, 70, 80, 90, 95, 99, or 100 wt% water, for example. Examples of aqueous compositions include mixtures, solutions, dispersions (e.g., colloidal dispersions), suspensions and emulsions, for example.

[0037] As used herein, the term “colloidal dispersion” refers to a heterogeneous system having a dispersed phase and a dispersion medium, i.e. , microscopically dispersed insoluble particles are suspended throughout another substance (e.g., an aqueous composition such as water or aqueous solution). An example of a colloidal dispersion herein is a hydrocolloid. All, or a portion of, the particles of a colloidal dispersion such as a hydrocolloid can comprise insoluble alpha-glucan as presently disclosed. The terms “dispersant” and “dispersion agent” are used interchangeably herein to refer to a material that promotes the formation and / or stabilization of a dispersion. “Dispersing” herein refers to the act of preparing a dispersion of a material in an aqueous liquid. As used herein, the term “latex” (and like terms) refers to a dispersion of one or more types of polymer particles in water or aqueous solution; typically, at least particles herein are in a latex composition as a dispersed polymer component. In some aspects, a latex is an emulsion that comprises a dispersion of at least particles herein.

[0038] An “emulsion” herein is a dispersion of minute droplets of one liquid in another liquid in which the droplets are not soluble or miscible (e.g., a non-polar substance such as oil or other organic liquid such as an alkane, in a polar liquid such as water or aqueous solution). An emulsion further comprises dispersed alpha-glucan herein, for example, which optionally can stabilize the emulsion. A “Pickering emulsion” comprises solid particles (e.g., insoluble alpha-glucan herein) on the interface between two liquid phases (e.g., water and hydrophobic additive such as oil) serving as a stabilizing agent. In some aspects, however, an emulsion herein can be a “dry emulsion”. A dry emulsion is typically produced by removing all or most (e.g. >95%, >99%, or >99.5%) of the water of a liquid emulsion, such as by freeze-drying or spray-drying.

[0039] Compositions of the present disclosure can provide stability to a dispersion or emulsion, for example. The “stability” (or the quality of being “stable”) of a dispersion or emulsion herein is, for example, the ability of dispersed particles of a dispersion, or liquid droplets dispersed in another liquid (emulsion), to remain dispersed (e.g., about, or at least about, 70, 75, 80, 85, 90, 95, 96, 97, 98, 99, or 100 wt% of the particles of the dispersion or liquid droplets of the emulsion are in a dispersed state) for a period of about, or at least about, 1 , 2, 4, 6, 9, 12, 18, 24, 30, or 36 months following initial preparation of the dispersion or emulsion. A stable dispersion or emulsion in some aspects can resist total sedimentation, flocculation, creaming, and / or coalescence of dispersed / emulsified material.

[0040] The term “viscosity” as used herein refers to the measure of the extent to which a fluid (aqueous or non-aqueous) resists a force tending to cause it to flow. Various units of viscosity that can be used herein include centipoise (cP, cps) and Pascal-second (Pa s), for example. A centipoise is one one-hundredth of a poise; one poise is equal to 0.100 kg m-1s-1. Viscosity can be reported as “intrinsic viscosity” (IV, r|, units of dL / g) in some aspects; this term refers to a measure of the contribution of a glucan polymer to the viscosity of a liquid (e.g., solution) comprising the glucan polymer. IV measurements herein can be obtained, for example, using any suitable method such as disclosed in U.S. Pat. Appl. Publ. Nos. 2017 / 0002335, 2017 / 0002336, or 2018 / 0340199, or Weaver et al. (J. Appl. Polym. Sci. 35:1631-1637) or Chun and Park (Macromol. Chem. Phys. 195:701-711), which are all incorporated herein by reference. IV can be measured, in part, by dissolving glucan polymer (optionally dissolved at about 100 °C for at least 2, 4, or 8 hours) in DMSO with about 0.9 to 2.5 wt% (e.g., 1 , 2, 1-2 wt%) LiCI, for example. IV herein can optionally be used as a relative measure of molecular weight.

[0041] An additive that “does not chemically react” (and like terminology) with an alphaglucan does not alter the chemical (covalent) structure of the alpha-glucan. For example, the presence of an additive in typical aspects does not lead to substitution of one or more hydrogens (of glucose monomer hydroxyl groups) with a group (e.g., an ether or ester group) originating from the additive. The presence of an additive in typical aspects does not lead to hydrolysis (or other breakage) of one or more (i) glycosidic linkages and / or (ii) intra-glucose monomer carbon-carbon bonds.

[0042] The term “hydrophobic” herein refers to a molecule / compound (e.g., additive herein) that is nonpolar and has little or no affinity to water, and tends to repel water. The term “hydrophilic” herein refers to a molecule / compound (e.g., additive herein) that is polar and has affinity to interact with polar solvents (e.g., water) and / or with other polar groups. A hydrophilic molecule tends to attract water.

[0043] The term “oil” as used herein typically refers to a lipid that is liquid at 25 °C and that is hydrophobic and soluble in organic solvents. Oil is typically composed primarily of triacylglycerols, but may also contain other neutral lipids, as well as phospholipids and free fatty acids. An oil can be from a plant, animal, or mineral source, for example.

[0044] A “wax” herein typically refers to an ester of a single fatty acid with a single long- chain alcohol. Generally, a wax is solid at temperatures below 45 or 50 °C, and / or is aqueous insoluble under both caustic and non-caustic conditions.

[0045] The terms “sequence identity”, “identity” and the like as used herein with respect to a polypeptide amino acid sequence (e.g., that of a glucosyltransferase) can be as defined and determined in U.S. Patent Appl. Publ. No. 2017 / 0002336, which is incorporated herein by reference.

[0046] Various polypeptide amino acid sequences are disclosed herein as features of certain embodiments. Variants of these sequences that are at least about 70-85%, 85- 90%, or 90%-95% identical to the sequences disclosed herein can be used or referenced. Alternatively, a variant amino acid sequence can have at least 70%, 71 %, 72%, 73%, 74%, 75%, 76%, 77%, 78%, 79%, 80%, 81%, 82%, 83%, 84%, 85%, 86%, 87%, 88%, 89%, 90%, 91 %, 92%, 93%, 94%, 95%, 96%, 97%, 98%, 99%, or 99.5% identity with a sequence disclosed herein. The variant amino acid sequence has the same function / activity of the disclosed sequence, or at least about 80%, 81 %, 82%, 83%, 84%, 85%, 86%, 87%, 88%, 89%, 90%, 91 %, 92%, 93%, 94%, 95%, 96%, 97%, 98%, or 99% of the function / activity of the disclosed sequence.

[0047] The terms “household care product”, “home care product”, and like terms typically refer to products, goods and services relating to the treatment, cleaning, caring, and / or conditioning of a home and its contents. The foregoing includes, for example, chemicals, compositions, products, or combinations thereof having application in such care.

[0048] A “fabric care composition”, “laundry care composition”, and like terms refer to any composition suitable for treating fabric, non-wovens, and / or any similar material in some manner. Examples of such a composition include laundry detergents and fabric softeners.

[0049] A “detergent composition” herein typically comprises at least a surfactant (detergent compound) and / or a builder. A “surfactant” herein refers to a substance that tends to reduce the surface tension of a liquid in which the substance is dissolved. A surfactant may act as a detergent, wetting agent, emulsifier, foaming agent, and / or dispersant, for example. In some aspects, an emulsion herein has at least one surfactant that interfaces between water and hydrophobic additive phases of the emulsion; this presence of a surfactant can optionally be in addition to the presence of insoluble alpha-glucan herein at the emulsion phase interface.

[0050] The term “personal care product” and like terms typically refer to products, goods and services relating to the treatment, cleaning, cleansing, caring or conditioning of a person. The foregoing include, for example, chemicals, compositions, products, or combinations thereof having application in such care.

[0051] The term “medical product” and like terms typically refer to products, goods and services relating to the diagnosis, treatment, and / or care of patients.

[0052] The term “industrial product” and like terms typically refer to products, goods and services used in industrial or institutional settings, but typically not by individual consumers.

[0053] The terms “ingestible product”, “ingestible composition” and the like refer to any substance that, either alone or together with another substance, may be taken orally (i.e. , by mouth), whether intended for consumption or not. Thus, an ingestible product includes food / beverage products. “Food / beverage products" refer to any edible product intended for consumption (e.g., for nutritional purposes) by humans or animals, including solids, semi-solids, or liquids. A “food” herein can optionally be referred to as a “foodstuff”, “food product”, or other like term, for example. “Non-edible products” (“nonedible compositions”) refer to any composition that can be taken by the mouth for purposes other than food or beverage consumption. Examples of non-edible products herein include supplements, nutraceuticals, functional food products, pharmaceutical products, oral care products (e.g., dentifrices, mouthwashes), and cosmetic products such as sweetened lip balms.

[0054] A “pharmaceutical product”, “medicine”, “medication”, “drug” or like term herein refers to a composition used to treat disease or injury, and can be administered enterally or parenterally.

[0055] The terms “percent by volume”, “volume percent”, “vol %”, “v / v %” and the like are used interchangeably herein. The percent by volume of a solute in a solution can be determined using the formula: [(volume of solute) / (volume of solution)] x 100%.

[0056] The terms “percent by weight”, “weight percentage (wt%)”, “weight-weight percentage (% w / w)” and the like are used interchangeably herein. Percent by weight refers to the percentage of a material on a mass basis as it is comprised in a composition, mixture, or solution.

[0057] The terms “weight / volume percent”, “w / v%” and the like are used interchangeably herein. Weight / volume percent can be calculated as: ((mass [g] of material) / (total volume [mL] of the material plus the liquid in which the material is placed)) x 100%. The material can be insoluble in the liquid (i.e. , be a solid phase in a liquid phase, such as with a dispersion), or soluble in the liquid (i.e., be a solute dissolved in the liquid).

[0058] The term “isolated” means a substance (or process) in a form or environment that does not occur in nature. A non-limiting example of an isolated substance includes any aqueous alpha-glucan composition disclosed herein (e.g., dispersion or emulsion). It is believed that the embodiments disclosed herein are synthetic / man-made (could not have been made or practiced except for human intervention / involvement), and / or have properties that are not naturally occurring.

[0059] The term “increased” as used herein can refer to a quantity or activity that is at least about 1 %, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 11 %, 12%, 13%, 14%, 15%, 16%, 17%, 18%, 19%, 20%, 50%, 100%, or 200% more than the quantity or activity for which the increased quantity or activity is being compared. The terms “increased”, “elevated”, “enhanced”, “greater than”, “improved” and the like are used interchangeably herein.

[0060] In some aspects, alpha-glucan comprises about, or at least about, 50%, 60%, 70%, 80%, 85%, 86%, 87%, 88%, 89%, 90%, 91 %, 92%, 93%, 94%, 95%, 96%, 97%, 98%, 99%, 99.5%, or 100% alpha-1 ,3 glycosidic linkages (i.e., the alpha-glucan is an alpha-1 , 3-glucan). In some aspects, accordingly, an insoluble alpha-glucan has about, or less than about, 50%, 40%, 30%, 20%, 15%, 10%, 9%, 8%, 7%, 6%, 5%, 4%, 3%, 2%, 1%, 0.5%, or 0% glycosidic linkages that are not alpha-1 ,3. Typically, the glycosidic linkages that are not alpha-1 ,3 are mostly or entirely alpha-1 ,6. In some aspects, an insoluble alpha-glucan has no branch points or less than about 5%, 4%, 3%, 2%, or 1 % branch points as a percent of the glycosidic linkages in the alpha-glucan.

[0061] The DPw, DPn, or DP of alpha-glucan in some aspects can be about, at least about, or less than about, 10, 15, 25, 50, 75, 100, 150, 200, 300, 400, 500, 600, 700, 800, 900, 1000, 1100, 1200, 1300, 1400, 1500, 1600, 1700, 1800, 1900, 2000, 2500, 3000, 3500, or 4000. DPw, DPn, or DP can optionally be expressed as a range between any two of these values. Merely as examples, the DPw, DPn, or DP can be about 50-1600, 100-1600, 200-1600, 300-1600, 400-1600, 500-1600, 600-1600, 700- 1600, 700-900, 50-1250, 100-1250, 200-1250, 300-1250, 400-1250, 500-1250, 600- 1250, 700-1250, 50-1000, 100-1000, 200-1000, 300-1000, 400-1000, 500-1000, 600- 1000, 700-1000, 50-900, 100-900, 200-900, 300-900, 400-900, 500-900, 600-900, 700- 900, 600-800, 600-750, 1500-1800, or 1500-1700, 1600-1800. Merely as further examples, the DPw, DPn, or DP can be about 15-100, 25-100, 35-100, 15-80, 25-80, 35-80, 15-60, 25-60, 35-60, 15-55, 25-55, 35-55, 15-50, 25-50, 35-50, 35-45, 35-40, 40- 100, 40-80, 40-60, 40-55, 40-50, 45-60, 45-55, 45-50, 15-35, 20-35, 15-30, or 20-30. Merely as further examples, the DPw, DPn, or DP can be about 100-600, 100-500, 100- 400, 100-300, 200-600, 200-500, 200-400, or 200-300. In some aspects, alpha-glucan can have a high molecular weight as reflected by high intrinsic viscosity (IV); e.g., IV can be about, or at least about, 6, 7, 8, 9, 10, 11 , 12, 13, 14, 15, 16, 17, 18, 19, 20, 21 , 22, 6- 8, 6-7, 6-22, 6-20, 6-17, 6-15, 6-12, 10-22, 10-20, 10-17, 10-15, 10-12, 12-22, 12-20, 12- 17, or 12-15 dL / g (for comparison purposes, note that the IV of alpha-glucan with at least 90% (e.g., about 99% or 100%) alpha-1 ,3 linkages and a DPw of about 800 has an IV of about 2-2.5 dL / g). IV herein can be as measured with alpha-glucan polymer dissolved in DMSO with about 0.9 to 2.5 wt% (e.g., 1 , 2, 1-2 wt%) LiCI, for example. Alpha-glucan herein can be as disclosed (e.g., molecular weight, linkage profile, and / or production method), for example, in U.S. Patent Nos. 7000000, 8871474, 10301604, or 10260053, or U.S. Patent Appl. Publ. Nos. 2019 / 0112456, 2019 / 0078062, 2019 / 0078063, 2018 / 0340199, 2018 / 0021238, 2018 / 0273731 , 2017 / 0002335, 2015 / 0232819, 2015 / 0064748, 2020 / 0165360, 2020 / 0131281 , 2019 / 0276806, or 2019 / 0185893, which are each incorporated herein by reference. Alpha-glucan can be produced, for example, by an enzymatic reaction comprising at least water, sucrose and a glucosyltransferase enzyme that synthesizes the alpha-glucan. Glucosyltransferases, reaction conditions, and / or processes contemplated to be useful for producing alphaglucan can be as disclosed in any of the foregoing references.

[0062] In some aspects, a glucosyltransferase enzyme for producing alpha-glucan herein can comprise an amino acid sequence that is 100% identical to, or at least 90%, 91 %, 92%, 93%, 94%, 95%, 96%, 97%, 98%, 98.5%, 99%, or 99.5% identical to, SEQ ID NO:2, 4, 6, 8, 10, 12, 14, 16, 18, 20, 26, 28, 30, 34, or 59, or amino acid residues 55- 960 of SEQ ID NO:4, residues 54-957 of SEQ ID NO:65, residues 55-960 of SEQ ID NO:30, residues 55-960 of SEQ ID NO:28, or residues 55-960 of SEQ ID NO:20, and have glucosyltransferase activity; these amino acid sequences are disclosed in U.S. Patent Appl. Publ. No. 2019 / 0078063, which is incorporated herein by reference. It is noted that a glucosyltransferase enzyme comprising SEQ ID NO:2, 4, 8, 10, 14, 20, 26, 28, 30, 34, or amino acid residues 55-960 of SEQ ID NO:4, residues 54-957 of SEQ ID NO:65, residues 55-960 of SEQ ID NO:30, residues 55-960 of SEQ ID NO:28, or residues 55-960 of SEQ ID NO:20, can synthesize alpha-glucan comprising at least about 90% (-100%) alpha-1 ,3 linkages.

[0063] Alpha-glucan herein typically does not have any chemical derivatization (e.g., etherification, esterification, phosphorylation, sulfation, oxidation, carbamation) (e.g., no substitution of hydrogens of glucan hydroxyl groups with a non-sugar chemical group). However, in some aspects, alpha-glucan can be a charged (e.g., cationic or anionic) derivative of an alpha-glucan as disclosed herein. The DoS of such a derivative typically is less than about 0.3, 0.25, 0.2, 0.15, 0.1 , or 0.05. The type of derivative can be any of the foregoing derivatives (e.g., ether, ester). Typically, alpha-glucan herein is enzymatically derived in an inert vessel (typically under cell-free conditions) and is not derived from a cell wall (e.g., fungal cell wall).

[0064] In some aspects, at least about 65% by weight of alpha-glucan particles (e.g., as partially precipitated at pH 12.5-13.2 or any other relevant pH disclosed herein, in a dispersion and / or an emulsion herein) have a diameter of less than 2.0, 1 .5, or 1.0 micron. Yet, in some aspects, about, or at least about, 65%, 70%, 75%, 80%, 85%, 90%, 95%, 65-95%, 70-95%, 75-95%, 80-95%, 85-95%, 65-90%, 70-90%, 75-90%, 80- 90%, 85-90%, 65-85%, 70-85%, 75-85%, or 80-85% by weight of alpha-glucan particles have a diameter of less than about 2.0, 1.5, or 1 .0 micron. It can additionally or alternatively be characterized, in some aspects, that alpha-glucan particles have an average diameter of about, or less than about, 1.0, 0.8, 0.7, 0.6, 0.5, 0.4, 0.3, 0.3-0.8, 0.3-0.7, 0.3-0.6, 0.4-0.8, 0.4-0.7, or 0.4-0.6 micron particles (e.g., as partially precipitated at pH 12.5-13.2 or any other relevant pH disclosed herein, in a dispersion and / or an emulsion herein). The foregoing particle size and / or distributions for particles can be as measured for particles comprised in an aqueous dispersion, emulsion, and / or as measured using a light scatter technique, for example.

[0065] In some aspects, an aqueous composition of the present disclosure (e.g., a dispersion of undissolved alpha-glucan in the presence of dissolved alpha-glucan, typically at pH 12.5-13.2 or any other relevant pH disclosed herein; the aqueous composition can further be an emulsion in some aspects) comprises about, at least about, or less than about, 0.25%, 0.3%, 0.5%, 0.75%, 1%, 1.5%, 2%, 2.5%, 3%, 4%, 5%, 0.25-5%, 0.25-3%, 0.25-2.5%, 0.25-2%, 0.25-1.5%, 0.25-1.25%, 0.25-1%, 0.25- 0.75%, 0.25-0.5%, 0.5-5%, 0.5-3%, 0.5-2.5%, 0.5-2%, 0.5-1.5%, 0.5-1.25%, 0.5-1 %, 0.5-0.75%, 0.75-5%, 0.75-3%, 0.75-2.5%, 0.75-2%, 0.75-1.5%, 0.75-1.25%, 0.75-1%, 1- 5%, 1-3%, 1-2.5%, 1-2%, or 1-1.5% by weight of alpha-glucan herein (e.g., weight based on total of the undissolved alpha-glucan and dissolved alpha-glucan in the aqueous composition, in dispersion and / or emulsion aspects at pH 12.5-13.2 or any other relevant pH disclosed herein) (e.g., weight based on total of the undissolved alphaglucan in the aqueous composition at a neutral pH, such as an emulsion herein).

[0066] In some aspects, an aqueous composition (e.g., dispersion and / or emulsion) of the present disclosure comprises about, or at least about, 30%, 40%, 50%, 60%, 70%, 80%, 90%, 92.5%, 95%, 96%, 97%, 98%, 99%, 30-70%, 30-60%, 40-70%, 40-60%, or 45-55% by weight (or by volume) water. In some aspects in which the aqueous composition is an emulsion as presently disclosed, the water content can be on a vol% basis, and typically the vol% is any of the foregoing values / ranges between 30-70%).

[0067] In some aspects, an aqueous composition (e.g., emulsion) of the present disclosure comprises about, or at least about, 30%, 40%, 50%, 60%, 70%, 30-70%, 30- 60%, 40-70%, 40-60%, or 45-55% by weight (or by volume) of one or more hydrophobic additives. A hydrophobic additive herein can be a liquid (in the form of a liquid), for example, or in any other form such as a malleable form (e.g., wax). Examples of hydrophobic additives herein include oil such as mineral oil, silicone oil (e.g., dimethicone / polydimethylsiloxane, hexamethyldisiloxane), paraffin oil, or plant / vegetable oil (e.g., linseed oil, soybean oil, palm oil, coconut oil, canola oil, com oil, sunflower oil, grape seed oil, cocoa butter, olive oil, rice bran oil, rapeseed oil, peanut oil, sesame oil, cottonseed oil, palm kernel oil); shortening (e.g., vegetable shortening); lipid; fat (e.g., lard, tallow, animal fat); glyceride (e.g., tri-, di- and / or mono-glyceride; e.g., caprylic / capric triglyceride); glycerol (glycerin) (or other polyol such as low molecular weight polyol); fatty acid; fatty aldehyde, fatty alcohol, fatty acid ester (e.g., sorbitan oleate); fatty acid amide; wax (e.g., paraffin wax, carnauba wax); phospholipid; sterol; alkane; alkene / olefin; petrolatum (i.e., petroleum jelly); or grease.

[0068] Emulsion droplet (e.g., of liquid hydrophobic additive such as an oil) size in some aspects can be about, or less than about, 22, 20, 17.5, 15, 12.5, 10, 7.5, 5, 5-20, 5-15, 5-10, 10-20, 10-15, 15-20, or 6-9 microns in diameter), for example. This size can be uniform (e.g., standard deviation under 2 or 3 microns), for example.

[0069] Typically, one or more additional components / ingredients can be present in an aqueous composition herein. Examples of other components can be any as disclosed herein, such as one or more of a salt, buffer, oil, organic solvent, enzyme, enzyme byproduct (e.g., glucosyltransferase byproduct such as leucrose, glucose, or glucooligosaccharide; e.g., fructose coproduct or unreacted sucrose, both of which are not byproducts per se), surfactant, preservative, personal care product ingredient, household care product ingredient, industrial product ingredient, ingestible product (e.g., food product) ingredient, medical product ingredient, or pharmaceutical product ingredient. Yet, in some aspects, an aqueous composition can consist of, or essentially consist of (e.g., further have one or more salts or buffers), (i) water, (ii) insoluble alphaglucan, and (iii) one or more hydrophobic additives; such a composition can optionally be stored and used for later formulation preparation (i.e., addition of one or more other ingredients / additives herein).

[0070] An aqueous composition of the disclosure in some aspects has no (detectable) dissolved sugars, or about 0.1-1.5, 0.1-1.25, 0.1-1.0, 0.1-.75, 0.1-0.5, 0.2-0.6, 0.3-0.5, 0.2, 0.3, 0.4, 0.5, or 0.6 wt% dissolved sugars. Such dissolved sugars can include sucrose, fructose, glucose, leucrose, and / or soluble gluco-oligosaccharides, for example. A composition in some aspects can have one or more salts / buffers (e.g., Na+, Ch, NaCI, phosphate, tris, citrate) (e.g., < 0.1 , 0.5, 1.0, 2.0, or 3.0 wt%), and / or a pH of 12.5 to 13.2 (e.g., pH 12.6 to 13.1 , pH 12.7 to 13.1 , pH 12.7, pH 12.8, pH 12.9, pH 13.0, pH 13.1) or about 5.0, 5.5, 6.0, 6.5, 7.0, 7.5, 8.0, 8.5, 9.0, 4.0-9.0, 4.0-8.0, 5.0-9.0, 5.0- 8.5, 5.0-8.0 6.0-9.0, or 6.0-8.0, or a suitable neutral pH, for example.

[0071] The temperature of an aqueous composition herein can be about, at least about, or less than about, 10, 15, 20, 25, 30, 35, 37, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 100, 105, 110, 115, 120, 125, 130, 10-30, 10-25, 15-50, 15-30, 15-25, 20-40, 20-35, 20-30, 20-25, 25-30, 30-50, 30-45, 30-40, 30-35, 35-40, 35-50, 40-45, 50-60, 110-130, 110-125, 110-120, 115-130, or 115-125 °C, for example. Such a temperature can optionally characterize the conditions used to prepare an aqueous composition in some aspects.

[0072] The liquid component of an aqueous composition can be an aqueous fluid such as water or aqueous solution, for instance. The solvent of an aqueous solution typically is water, or can comprise about, or at least about, 80, 90, 95, 98, or 99 wt% water, for example.

[0073] An aqueous composition herein can have a viscosity of about, at least about, or less than about, 1 , 5, 10, 100, 200, 300, 400, 500, 600, 700, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 15000, 20000, 25000, 1-300, 10-300, 25-300, 50- 300, 1-250, 10-250, 25-250, 50-250, 1-200, 10-200, 25-200, 50-200, 1-150, 10-150, 25- 150, 50-150, 1-100, 10-100, 25-100, or 50-100 centipoise (cps, cP), for example. Viscosity can be as measured with an aqueous composition herein at any temperature between about 3 °C to about 80 °C, for example (e.g., 4-30 °C, 15-30 °C, 15-25 °C), ), or any particular temperature disclosed herein for an aqueous composition.. Viscosity typically is as measured at atmospheric pressure (about 760 torr) or a pressure that is ±10% thereof. Viscosity can be measured using a viscometer or rheometer, for example, and can optionally be as measured at a shear rate (rotational shear rate) of about 0.1 , 0.3, 0.5, 1.0, 3, 5, 10, 50, 100, 500, 1000, 0.1-500, 0.1-100, 1.0-500, 1.0- 1000, or 1.0-100 S’1(1 / s), or about 5, 10, 20, 25, 50, 100, 200, or 250 rpm (revolutions per minute), for example.

[0074] In some aspects, insoluble particles of an aqueous composition herein are dispersed through about, or at least about, 30%, 40%, 50%, 60%, 70%, 80%, 85%, 90%, 95%, 98%, 99%, or 100% of the volume of the aqueous composition. In some aspects, such a level of dispersion is contemplated to be for a time (typically beginning from initial preparation of the dispersion) of about, at least about, or up to about, 0.5, 1 , 2, 4, 6, 8, 10, 20, 30, 60, 90, 120, 150, 180, 210, 240, 270, 300, 330, or 360 days, or 1 , 2, or 3 years. In some aspects, an aqueous composition is a stable emulsion; any of the above dispersal-volume percentages and / or times of such stability can likewise characterize dispersed / emulsified oil droplets. In some aspects, stability can additionally or alternatively characterize an emulsion in which the average emulsion droplet size is relatively small (e.g., about, or less than about, 22, 20, 17.5, 15, 12.5, 10, 7.5, 5, 5-20, 5- 15, 5-10, 10-20, 10-15, 15-20, or 6-9 microns in diameter) and typically uniform in size. A small average droplet size equates to an elevated total droplet surface area. In some aspects, stability can additionally or alternatively characterize an emulsion having an average storage modulus (Avg. G’) (also referred to as elastic modulus) of about, or at least about, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 1000- 10000, 1000-9000, 1000-8000, 5000-10000, 5000-9000, 5000-8000, 7000-10000, 7000- 9000, or 7000-8000 Pascals, such as measured with a shear strain (y) of about 10’2, 10’1, 10°, or 101. The storage modulus of an emulsion herein can be measured according to the below Examples, or as disclosed in Varanasi et al. (2018, Frontiers Chem. 6:1-9, Article 409, incorporated herein by reference), for example. Based on the foregoing dispersion and / or emulsion stability features of an aqueous composition, it is contemplated that an aqueous composition is suitable for use in an application / product in which dispersion or emulsion stabilization improves the performance of the application / product. Examples of such applications / products can be as disclosed herein, such as milk / dairy products (e.g., yogurt, ice cream, cream), mayonnaise, salad dressings, beverages / tonics as carriers for delivering non-polar bioactive ingredients, cosmetic or pharmaceutical lotions / creams / foams / serums, waterborne / latex paints, defoaming formulations, rolling oils for metal working, mining explosives, agrochemical formulations, downhole fluids such as for enhanced oil recovery operations, or pharmaceutical carrier or encapsulation systems.

[0075] An aqueous composition herein can optionally contain one or more enzymes (active enzymes). Examples of suitable enzymes include proteases, cellulases, hemicellulases, peroxidases, lipolytic enzymes (e.g., metallolipolytic enzymes), xylanases, lipases, phospholipases, esterases (e.g., arylesterase, polyesterase), perhydrolases, cutinases, pectinases, pectate lyases, mannanases, keratinases, reductases, oxidases (e.g., choline oxidase), phenoloxidases, lipoxygenases, ligninases, pullulanases, tannases, pentosanases, malanases, beta-glucanases, arabinosidases, hyaluronidases, chondroitinases, laccases, metalloproteinases, amadoriases, glucoamylases, arabinofuranosidases, phytases, isomerases, transferases, nucleases, and amylases. If an enzyme(s) is included, it may be comprised in a composition herein at about 0.0001-0.1 wt% (e.g., 0.01-0.03 wt%) active enzyme (e.g., calculated as pure enzyme protein), for example. In fabric care or automatic dishwashing applications, an enzyme herein (e.g., any of the above such as cellulase, protease, amylase, and / or lipase) can be present in an aqueous composition in which a fabric or dish is treated (e.g., wash liquor, grey water) at a concentration that is minimally about 0.01-0.1 ppm total enzyme protein, or about 0.1-10 ppb total enzyme protein (e.g., less than 1 ppm), to maximally about 100, 200, 500, 1000, 2000, 3000, 4000, or 5000 ppm total enzyme protein, for example.

[0076] An aqueous composition herein can optionally contain one or more organic solvents such as a polar organic solvent. A polar organic solvent in some aspects can be protic. Examples of protic polar organic solvents herein include an alcohol (e.g., methanol, ethanol, isopropanol, 1 -propanol, tert-butyl alcohol, n-butanol, iso-butanol), methyl formamide and formamide. Additional examples of protic polar organic solvents herein include n-butanol, ethylene glycol, polyethylene glycol, propylene glycol, dipropylene glycol, tripropyleneglycol, polypropylene glycol, 2-methoxyethanol, 1- methoxy-2-propanol, glycerol, 1 ,2-propanediol, and 1 ,3-propanetriol. A polar organic solvent in some aspects can be aprotic. Examples of aprotic polar organic solvents herein include acetonitrile, dimethyl sulfoxide, acetone, N,N-dimethylformamide, N,N- dimethylacetamide, tetrahydrofuran, propylene carbonate, and sulfolane. Additional examples of aprotic polar organic solvents herein include hexamethylphosphoramide, dimethylimidazolidinone (1 ,3-dimethyl-2-imidazolidinone), dioxane, nitromethane, and butanone. In general, ester, ketone and aldehyde solvents having no acidic hydrogen atom are other examples of aprotic polar organic solvents herein. Organic solvent(s) can constitute about, or up to about, 10% or 20% by weight or volume of the solvent (balance is water), for example, of an aqueous composition.

[0077] An aqueous composition herein can optionally contain one or more preservatives. Examples of preservatives herein include phenoxyethanol, caprylyl glycol, ethylhexylglycerin, benzoate (e.g., sodium benzoate), diazolidinyl urea, iodopropynyl butylcarbamate, 2-methyl-4-isothiazolin-3-one, 5-chloro-2-methyl-4-isothiazolin-3-one, methylcholoroisothiasolinone, methylisothiasolinone, sorbate, benzisothiazolinone, paraben (e.g., methylparaben, ethylparaben, propylparaben, butylparaben, isobutylparaben), nitrate (e.g., sodium nitrate), propionate (e.g., sodium propionate), levulinic acid, anisic acid, formaldehyde, DMDM hydantoin, imadozolidinyl urea, diazolidinyl urea, German® II, and Germaben® II.

[0078] An aqueous composition as presently disclosed can be in the form of, or comprised in (e.g., as an ingredient / component of), a household care product, personal care product, industrial product, ingestible product (e.g., food product), medical product, or pharmaceutical product, for example, such as described in any of U.S. Patent Appl. Publ. Nos. 2018 / 0022834, 2018 / 0237816, 2018 / 0230241 , 20180079832, 2016 / 0311935, 2016 / 0304629, 2015 / 0232785, 2015 / 0368594, 2015 / 0368595, 2016 / 0122445, 2019 / 0202942, or 2019 / 0309096, or International Patent Appl. Publ. No.

[0079] WO201 6 / 133734, which are all incorporated herein by reference. In some aspects, an aqueous composition can comprise at least one component / ingredient of a household care product, personal care product, industrial product, pharmaceutical product, medical product, or ingestible product (e.g., food product) as disclosed in any of the foregoing publications and / or as presently disclosed.

[0080] An aqueous composition in some aspects is believed to be useful for providing one or more of the following physical properties to a personal care product, pharmaceutical product, household product, industrial product, or ingestible product (e.g., food product): thickening, freeze / thaw stability, lubricity, moisture retention and release, texture, consistency, shape retention, emulsification, binding, suspension, dispersion, gelation, for example.

[0081] Personal care products herein are not particularly limited and include, for example, skin care compositions, cosmetic compositions, antifungal compositions, and antibacterial compositions. Personal care products herein may be in the form of, for example, lotions, creams, foams, pastes, balms, ointments, pomades, gels, liquids, serums, combinations of these and the like. The personal care products disclosed herein can include at least one active ingredient, if desired. An active ingredient is generally recognized as an ingredient that causes an intended pharmacological effect.

[0082] A personal care product in some aspects can be a skin care product. A skin care product can be used on, and / or be designed for, general body application or targeted application (e.g., to hands or feet), for example. A skin care product in some aspects can be used on hair and / or nails (or exclusively for nails) in some aspects. In some aspects, a skin care product can be applied to skin for addressing skin damage related to a lack of moisture. A skin care product may also be used to address the visual appearance of skin (e.g., reduce the appearance of flaky, cracked, and / or red skin) and / or the tactile feel of the skin (e.g., reduce roughness and / or dryness of the skin while improved the softness and subtleness of the skin). A skin care product typically may include at least one active ingredient for the treatment or prevention of skin ailments, providing a cosmetic effect, or for providing a moisturizing benefit to skin, such as zinc oxide, petrolatum, white petrolatum, mineral oil, cod liver oil, lanolin, dimethicone, hard fat, vitamin A, allantoin, calamine, kaolin, glycerin, or colloidal oatmeal, and combinations of these. A skin care product may include one or more natural moisturizing factors such as ceramides, hyaluronic acid, glycerin, squalane, amino acids, cholesterol, fatty acids, triglycerides, phospholipids, glycosphingolipids, urea, linoleic acid, glycosaminoglycans, mucopolysaccharide, sodium lactate, or sodium pyrrolidone carboxylate, for example. Other ingredients that may be included in a skin care product include, without limitation, glycerides, apricot kernel oil, canola oil, squalane, squalene, coconut oil, com oil, jojoba oil, jojoba wax, lecithin, olive oil, safflower oil, sesame oil, shea butter, soybean oil, sweet almond oil, sunflower oil, tea tree oil, shea butter, palm oil, cholesterol, cholesterol esters, wax esters, fatty acids, and orange oil. A skin care product can be an ointment, lotion, or sanitizer (e.g., hand sanitizer) in some aspects. A skin care product / formulation that can be adapted to be an aqueous composition herein can be as disclosed in, for example, US20100189669, US20200093799, US20080014162, US20050002889, US20020039565, US20080213323, US20040022822, US20070166249, US20080152606, US20080008668, US20140256830, US20030206932, US20030114323, US20110152335, US20150202139, US20040180026, US4595586, US4268526, US4272519, US4285967, US4368189, US4372944, US4699780, US4816271 , US4839164, US4464362, US5552135, US5693255, US5976555, US5607921 , US5618523, US5798108, US5356627, US5811083, US5939085, US6280714, US8465973, US9867774, US11110049, US10546658, US11033480, EP0321929, or WO201 3092872, all of which are incorporated herein by reference. A skin care product can comprise one or more ingredients / additives as disclosed in any of the foregoing references, for example.

[0083] A personal care product herein can also be in the form of makeup, lipstick, mascara, rouge, foundation, blush, eyeliner, lip liner, lip gloss, other cosmetics, sunscreen, sun block, nail polish, nail conditioner, bath gel, shower gel, body wash, face wash, lip balm, skin conditioner, cream, foam, cold cream, moisturizer, body spray, soap, body scrub, exfoliant, astringent, scruffing lotion, depilatory, permanent waving solution, antidandruff formulation, antiperspirant composition, deodorant, shaving product, preshaving product, after-shaving product, cleanser, skin gel, serum (skin serum), rinse, dentifrice composition, toothpaste, or mouthwash, for example. An example of a personal care product (e.g., a cleanser, soap, scrub, cosmetic) comprises a carrier or exfoliation agent (e.g., jojoba beads [jojoba ester beads]) (e.g., about 1-10, 3-7, 4-6, or 5 wt%); such an agent may optionally be dispersed within the product. A personal care product in some aspects can be a hair care product. Examples of hair care products herein include shampoo, hair conditioner (leave-in or rinse-out), cream rinse, hair dye, hair coloring product, hair shine product, hair serum, hair anti-frizz product, hair split-end repair product, mousse, hair spray, and styling gel. A hair care product can be in the form of a liquid, paste, gel, cream, foam, solid, or powder in some embodiments. A hair care product as presently disclosed typically comprises one or more of the following ingredients, which are generally used to formulate hair care products: anionic surfactants such as polyoxyethylenelauryl ether sodium sulfate; cationic surfactants such as stearyltrimethylammonium chloride and / or distearyltrimethylammonium chloride; nonionic surfactants such as glyceryl monostearate, sorbitan monopalmitate and / or polyoxyethylenecetyl ether; wetting agents such as propylene glycol, 1 ,3-butylene glycol, glycerin, sorbitol, pyroglutamic acid salts, amino acids and / or trimethylglycine; hydrocarbons such as liquid paraffins, petrolatum, solid paraffins, squalane and / or olefin oligomers; higher alcohols such as stearyl alcohol and / or cetyl alcohol; superfatting agents; antidandruff agents; disinfectants; anti-inflammatory agents; crude drugs; water-soluble polymers such as methyl cellulose, hydroxycellulose and / or partially deacetylated chitin; antiseptics such as paraben; ultra-violet light absorbers; pearling agents; pH adjustors; perfumes; and pigments.

[0084] An personal care product in some aspects can be a hair care composition such as a hair styling or hair setting composition (e.g., hair gel or lotion, hair mousse / foam, hair serum) (e.g., foam, creme, paste, non-runny gel, mousse, pomade, lacquer, hair wax). A hair styling / setting composition / formulation that can be adapted to be an aqueous composition herein can be as disclosed in, for example, US20090074697, WO1999048462, US20130068849, JPH0454116A, US5304368, AU667246B2, US5413775, US5441728, US5939058, JP2001302458A, US6346234, US20020085988, US7169380, US20090060858, US20090326151, US20160008257, W02020164769, or US20110217256, all of which are incorporated herein by reference. A hair care composition such as a hair styling / setting composition can comprise one or more ingredients / additives as disclosed in any of the foregoing references, and / or one or more of a fragrance / perfume, aroma therapy essence, herb, infusion, antimicrobial, stimulant (e.g., caffeine), essential oil, hair coloring, dying or tinting agent, anti-gray agent, antifoam agent, sunscreen / UV-blocker (e.g., benzophenone-4), vitamin, antioxidant, surfactant or other wetting agent, mica, silica, metal flakes or other glitter-effect material, conditioning agent (e.g., a volatile or non-volatile silicone fluid), anti-static agent, opacifier, detackifying agent, penetrant, preservative (e.g., phenoxyethanol, ethylhexylglycerin, benzoate, diazolidinyl urea, iodopropynyl butylcarbamate), emollient (e.g., panthenol, isopropyl myristate), rheology-modifying or thickening polymer (e.g., acrylates / methacrylamide copolymer, polyacrylic acid [e.g., CARBOMER]), emulsified oil phase, petrolatum, fatty alcohols, diols and polyols, emulsifier (e.g., PEG-40 hydrogenated castor oil, Oleth-20), humectant (e.g., glycerin, caprylyl glycol), silicone derivative, protein, amino acid (e.g., isoleucine), conditioner, chelant (e.g., EDTA), solvent (e.g., see below), monosaccharide (e.g., dextrose), disaccharide, oligosaccharide, pH-stabilizing compound (e.g., aminomethyl propanol), film former (e.g., acrylates / hydroxyester acrylate copolymer, polyvinylpyrrolidone / vinyl acetate copolymer, triethyl acetate), and / or any other suitable material herein. Optional hair fixing / styling agents herein include PVP (polyvinylpyrrolidone), octylacrylamide / acrylates / butylaminoethyl methacrylate copolymer, vinyl caprolactam / PVP / dimethylaminoethyl methacrylate copolymer, AMPHOMER, or any film former such as listed above.

[0085] A hair styling / setting composition can comprise a solvent comprising water and optionally a water-miscible (typically polar) organic compound (e.g., liquid or gas) such as an alcohol (e.g., ethanol, propanol, isopropanol, n-butanol, iso-butanol, tert-butanol), an alkylene glycol alkyl ether, and / or a monoalkyl or dialkyl ether (e.g., dimethyl ether), for example. If an organic compound is included, it can constitute about 10%, 20%, 30%, 40%, 50%, or 60% by weight or volume of the solvent (balance is water), for example. The amount of solvent in a hair styling / setting composition herein can be about 50-90, 60-90, 70-90, 80-90, 50-95, 60-95, 70-95, 80-95, or 90-95 wt%, for example.

[0086] A pharmaceutical product herein can be in the form of an emulsion, liquid, elixir, gel, suspension, solution, cream, foam, serum, or ointment, for example. Also, a pharmaceutical product herein can be in the form of any of the personal care products disclosed herein, such as an antibacterial or antifungal composition. A pharmaceutical product can further comprise one or more pharmaceutically acceptable carriers, diluents, and / or pharmaceutically acceptable salts. A composition herein can also be used in capsules, encapsulants, tablets, tablet coatings, and as an excipients for medicaments and drugs.

[0087] A household care and / or industrial product herein can be in the form of drywall tape-joint compounds; mortars; grouts; cement plasters; spray plasters; cement stucco; adhesives; pastes; wall / ceiling texturizers; binders and processing aids for tape casting, extrusion forming, injection molding and ceramics; spray adherents and suspending / dispersing aids for pesticides, herbicides, and fertilizers; fabric care products such as fabric softeners and laundry detergents; hard surface cleaners; air fresheners; polymer emulsions; latex; gels such as water-based gels; surfactant solutions; paints such as water-based paints; protective coatings; adhesives; sealants and caulks; inks such as water-based ink; metal-working fluids; films or coatings; or emulsion-based metal cleaning fluids used in electroplating, phosphatizing, galvanizing and / or general metal cleaning operations, for example. In some aspects, a composition herein is comprised in a fluid as a viscosity modifier and / or friction reducer; such uses include downhole operations / fluids (e.g., in hydraulic fracturing and enhanced oil recovery).

[0088] Examples of ingestible products herein include a food, beverage, animal feed, an animal health and / or nutrition product, and / or pharmaceutical product. The intended use of a composition as presently disclosed in an ingestible product can be to provide texture, add volume, and / or thicken, for example.

[0089] Further examples of using a composition of the present disclosure for ingestible products include use as: a bulking, binding and / or coating ingredient; a carrier for coloring agents, flavors / fragrances, and / or high intensity sweeteners; a spray drying adjunct; a bulking, bodying, dispersing and / or emulsification agent; and an ingredient for promoting moisture retention (humectant). Illustrative examples of products that can be prepared having a composition herein include food products, beverage products, pharmaceutical products, nutritional products, and sports products. Examples of beverage products herein include concentrated beverage mixes, carbonated beverages, non-carbonated beverages, fruit-flavored beverages, fruit juices, teas, coffee, milk nectars, powdered drinks, liquid concentrates, milk drinks, ready-to-drink (RTD) products, smoothies, alcoholic beverages, flavored waters and combinations thereof. Examples of food products herein include baked goods (e.g., breads), confectioneries, frozen dairy products, meats, artificial / synthetic / cultured meat, cereal products (e.g., breakfast cereals), dairy products (e.g., yogurt), condiments (e.g., mustard, ketchup, mayonnaise), snack bars, soups, dressings, mixes, prepared foods, baby foods, diet preparations, peanut butter, syrups, sweeteners, food coatings, pet food, animal feed, animal health and nutrition products, dried fruit, sauces, gravies, jams / jellies, dessert products, spreads, batters, breadings, spice mixes, frostings and the like. In some aspects, a composition herein can provide or enhance the foaming of beverages such as dairy beverages, non-dairy alternative beverages (e.g., “vegan” milk such as soy milk, almond milk, or coconut milk), dairy creamers, and / or non-dairy creamers (e.g., for a hot beverage such as coffee [e.g., cappuccino], tea [e.g., chai tea]).

[0090] An aqueous composition as presently disclosed can be in the form of, or comprised in (e.g., as an ingredient / component of), a latex composition, for example. Examples of latex compositions herein include paint (e.g., primer, finishing / decorative), adhesives, films, coatings, and binders. Formulations and / or components (in addition to alpha-glucan particles herein) of a latex composition herein can be as described in, for example, U.S. Patent Nos. 6881782, 3440199, 3294709, 5312863, 4069186, or 6297296, or U.S. Patent Appl. Publ. No. 2020 / 0263026, which are all incorporated herein by reference.

[0091] Alpha-glucan as presently disclosed can be present in a latex composition in any useful amount, such as at about, or at least about, 0.01%, 0.02%, 0.03%, 0.04%, 0.05%, 0.06%, 0.07%, 0.08%, 0.09%, 0.1%, 0.2%, 0.3%, 0.4%, 0.5%, 0.6%, 0.7%, 0.8%, 0.9%, 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 15%, 20%, 25%, 30%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 0.01%-75% 0.01 %-5%, 5%-20%, 20%-50%, or 50%-75% based on the weight of all the dispersed polymer solids of the latex.

[0092] A latex composition in some aspects can comprise a polymer polymerized from at least one ethylenically unsaturated monomer (e.g., monoethylenically unsaturated monomer); polyurethane; epoxy, and / or a rubber elastomer. Examples of monoethylenically unsaturated monomers herein include vinyl monomers, acrylic monomers, allylic monomers, acrylamide monomers, monocarboxylic unsaturated acids and dicarboxylic unsaturated acids.

[0093] Examples of suitable vinyl monomers of a polymer in a latex composition herein include any compounds having vinyl functionality (i.e. , ethylenic unsaturation) such as vinyl esters (e.g., vinyl acetate, vinyl propionate, vinyl laurate, vinyl pivalate, vinyl nonanoate, vinyl decanoate, vinyl neodecanoate, vinyl butyrates, vinyl benzoates, vinyl isopropyl acetates), vinyl aromatic hydrocarbons (e.g., styrene, methyl styrenes and similar lower alkyl styrenes, chlorostyrene, vinyl toluene, vinyl naphthalene, divinyl benzene), vinyl aliphatic hydrocarbons (e.g., vinyl chloride; vinylidene chloride; alpha olefins such as ethylene, propylene and isobutylene; conjugated dienes such as 1 ,3- butadiene, methyl-2-butadiene, 1 ,3-piperylene, 2,3-dimethyl butadiene, isoprene, cyclohexene, cyclopentadiene, and dicyclopentadiene) and vinyl alkyl ethers (e.g., methyl vinyl ether, isopropyl vinyl ether, n-butyl vinyl ether, isobutyl vinyl ether), but excluding compounds having acrylic functionality (e.g., acrylic acid, methacrylic acid, esters of such acids, acrylonitrile, acrylamides). In some aspects, a latex composition herein comprises a vinyl acetate-ethylene copolymer, carboxylated vinyl acetateethylene copolymer, and / or or polyvinyl acetate.

[0094] Examples of suitable acrylic monomers of a polymer in a latex composition herein include alkyl acrylates, alkyl methacrylates, acrylate acids, methacrylate acids, aromatic derivatives of acrylic and methacrylic acid, acrylamides, and acrylonitrile. Typically, alkyl acrylate and methacrylic monomers (also referred to as alkyl esters of acrylic or methacrylic acid) have an alkyl ester portion containing from 1 to about 18 carbon atoms per molecule, or from 1 to about 8 carbon atoms per molecule. Suitable acrylic monomers include, for example, methyl acrylate and methacrylate, ethyl acrylate and methacrylate, butyl acrylate and methacrylate, propyl acrylate and methacrylate, 2-ethyl hexyl acrylate and methacrylate, cyclohexyl acrylate and methacrylate, decyl acrylate and methacrylate, isodecyl acrylate and methacrylate, benzyl acrylate and methacrylate, isobornyl acrylate and methacrylate, neopentyl acrylate and methacrylate, and 1- adamantyl methacrylate . If acid functionality is desired, acids such as acrylic acid or methacrylic acid can also be used.

[0095] A latex composition in some aspects comprises a polyurethane polymer. Examples of suitable polyurethane polymers are those comprising polysaccharides as disclosed in U.S. Patent Appl. Publ. No. 2019 / 0225737, which is incorporated herein by reference. A latex comprising a polyurethane can be prepared, for example, as disclosed in U.S. Patent Appl. Publ. No. 2016 / 0347978, which is incorporated herein by reference, and / or comprise the reaction product of one or more polyisocyanates with one or more polyols. Useful polyols include polycarbonate polyols, polyester polyols and polyether polyols, for example. Polycarbonate polyurethane herein can be formed as the reaction product of a polyol such as 1 ,3-propanediol, 1 ,4-butanediol, 1 ,6-hexanediol, diethylene glycol, or tetraethylene glycol, with a diaryl carbonate such as diphenyl carbonate or phosgene. At least one polyisocyanate herein can be an aliphatic polyisocyanate, aromatic polyisocyanate, or polyisocyanate that has both aromatic and aliphatic groups. Examples of polyisocyanates include 1 ,6-hexamethylene diisocyanate, isophorone diisocyanate, 2,4-toluene diisocyanate, 2,6-toluene diisocyanate, mixtures of 2,4- and 2,6-toluene diisocyanate, bis(4-isocyanatocyclohexyl) methane, 1 ,3-bis(1- isocyanato-1 -methylethyl)benzene, bis(4-isocyanatophenyl)methane, 2,4'- diphenylmethane diisocyanate, 2,2'-diphenylmethane diisocyanate, 2,4- diisocyanatotoluene, bis(3-isocyanatophenyl)methane, 1 ,4-diisocyanatobenzene, 1 ,3- diisocyanato-o-xylene, 1 ,3-diisocyanato-p-xylene, 1 ,3-diisocyanato-m-xylene, 2,4- diisocyanato-1 -chlorobenzene, 2,4-diisocyanato-1 -nitrobenzene, 2,5-diisocyanato-1 - nitrobenzene, m-phenylene diisocyanate, hexahydrotoluene diisocyanate, 1 ,5- naphthalene diisocyanate, 1-methoxy-2,4-phenylene diisocyanate, 4,4'-biphenylmethane diisocyanate, 4,4'-biphenylene diisocyanate, 3,3'-dimethyl-4,4'-diphenylmethane, diisocyanate, 3,3'-4,4'-diphenylmethane diisocyanate, and 3,3'- dimethyldiphenylmethane-4,4'-diisocyanate. Also useful herein are polyisocyanate homopolymers comprising allophanate, biuret, isocyanurate, iminooxadiazinedione, or carbodiimide groups, for example. A polyol herein can be any polyol comprising two or more hydroxyl groups, for example, a C2 to C12 alkane diol, ethylene glycol, 1 ,2- propylene glycol, 1 ,3-propylene glycol, isomers of butane diol, pentane diol, hexane diol, heptane diol, octane diol, nonane diol, decane diol, undecane diol, dodecane diol, 2- methyl-1 ,3-propane diol, 2,2-dimethyl-1 ,3-propane diol (neopentyl glycol), 1 ,4- bis(hydroxymethyl)cyclohexane, 1 ,2,3-propane triol (glycerol), 2-hydroxymethyl-2- methyl-1 ,3-propanol (trimethylolethane), 2-ethyl-2-hydroxymethyl-1 ,3-propanediol (trimethylolpropane), 2,2-bis(hydroxymethyl)-1 ,3-propane diol (pentaerythritol); 1 ,4,6- octanetriol; chloropentanediol; glycerol monoalkyl ether; glycerol monoethyl ether; diethylene glycol; 1 ,3,6-hexanetriol; 2-methylpropanediol; 2,2,4-trimethyl-1 ,3- pentanediol, cyclohexanedimethanol, polymeric polyols, for example, polyether polyols or polyester polyols. In some aspects, a polyol herein can be poly(oxytetramethylene) glycol, polyethylene glycol, or poly 1 ,3-propane diol. A polyol in some aspects can be polyester polyol, such as one produced by transesterification of aliphatic diacids with aliphatic diols. Suitable aliphatic diacids include, for example, C3 to C10 diacids, malonic acid, succinic acid, glutaric acid, adipic acid, pimelic acid, suberic acid, azelic acid, sebacic acid. In some aspects, aromatic and / or unsaturated diacids can be used to form a polyester polyol.

[0096] A latex composition in some aspects comprises an epoxy polymer / resin (polyepoxide), such as bisphenol A epoxy resin, bisphenol F epoxy resin, Novolac epoxy resin, aliphatic epoxy resin, or glycidylamine epoxy resin.

[0097] A latex composition in some aspects comprises a rubber elastomer. In some aspects, a rubber elastomer can include one or more diene-based sulfur-vulcanizable elastomers having a glass transition temperature (Tg) below -30 °C, as determined, for example, by dynamic mechanical analysis. In further examples, a rubber elastomer herein includes natural rubber, synthetic polyisoprene, polybutadiene rubber, styrene / butadiene copolymer rubber, ethylene propylene diene monomer rubber, hydrogenated nitrile butadiene rubber, neoprene, styrene / isoprene / butadiene terpolymer rubber, butadiene / acrylonitrile rubber, polyisoprene rubber, isoprene / butadiene copolymer rubber, nitrile rubber, ethylene-acrylic rubber, butyl and halobutyl rubber, chlorosulfonated polyethylene, fluoroelastomer, hydrocarbon rubber, polybutadiene, and silicone rubber.

[0098] A latex composition herein comprises alpha-glucan particles dispersed in a dispersion (other polymers such as above can optionally be dispersed along with the alpha-glucan particles) or emulsion, where the liquid component of the latex can be water or an aqueous solution. An aqueous solution of a latex in some aspects can comprise an organic solvent that is either miscible or immiscible with water. Suitable organic solvents herein include acetone, methyl ethyl ketone, butyl acetate, tetrahydrofuran, methanol, ethanol, isopropanol, diethyl ether, glycerol ethers, hexane, toluene, dimethyl acetamide, dimethylformamide, and dimethyl sulfoxide.

[0099] A latex composition herein can further comprise one or more additives in some aspects. Examples of additives herein include dispersants, rheological aids, antifoams, foaming agents, adhesion promoters, flame retardants, bactericides, fungicides, preservatives, optical brighteners, fillers, anti-settling agents, coalescing agents, humectants, buffers, pigments / colorants (e.g., metallic oxides, synthetic organic pigments, carbon black), viscosity modifiers, antifreeze, surfactants, binders, crosslinking agents, anticorrosion agents, hardeners, pH regulators, salts, thickeners, plasticizers, stabilizers, extenders, and matting agents. Examples of pigments herein include titanium dioxide (TiCh), calcium carbonate, diatomaceous earth, mica, hydrated aluminum oxide, barium sulfate, calcium silicate, clay, silica, talc, zinc oxide, aluminum silicate, nepheline syenite, and mixtures thereof. In some aspects, a latex composition is essentially free from (e.g., less than 1 , 0.5, 0.1 , or 0.01 wt% of component) starch, starch derivative (e.g., hydroxyalkyl starch), cellulose, and / or cellulose derivative (e.g., carboxymethyl cellulose).

[0100] A latex composition in the form of a paint or other coloring agent herein can have a pigment volume concentration (PVC) of about 3% to about 80% in some aspects. As examples, a flat paint can have a PVC in the range of about 55-80%, a primer or undercoat can have a PVC in the range of about 30-50%, and / or a gloss colored paint can have a PVC in the range of about 3-20%. A paint or other coloring agent in some aspects can have a PVC of about 55%, 60%, 65%, 70%, 75%, 80%, 55-80%, 55-75%, 55-70%, 60-80%, 60-75%, 60-70%, 63-67%, 64-66%, 65-80%, 65-75%, or 65-70%. A PVC value herein can be that of a particular pigment (or mix of pigments) such as those disclosed above (e.g., titanium dioxide), for instance. It is notable that insoluble alpha- glucan particles of the present disclosure can act as a pigment extender (see below Examples). For example, insoluble alpha-glucan particles can be used to replace a portion the amount of pigment in a paint (e.g., reduce pigment by about, or at least about, 1 %, 2.5%, 5%, 7.5%, 10%, 12.5%, 15%, 17.5%, 20%, 22.5%, 25%, 27.5%, 30%, 5-15%, 5-20%, 5-25%, 5-30%, 10-15%, 10-20%, 10-25%, 10-30%, 15-20%, 15-25%, 15-30%), while optionally simultaneously increasing the opacity of the paint (despite there being less pigment) by about, or at least about, 1 %, 1.25%, 1.5%, 1.75%, 2, 2.25%, 1-2.25%, 1-2%, or 1-1.75%. Replacement of pigment with insoluble alphaglucan particles herein can be on a basis of about 0.9-1.1 (e.g., 1.0) parts pigment to about 0.5-0.7 (e.g., 0.6 parts) insoluble alpha-glucan particles, for example. Aside from these advantages (opacity, less pigment needed), insoluble alpha-glucan particles of the present disclosure are believed to provide one or more other physical properties to a latex composition (e.g., for use as a paint or other coloring agent): increased hardness, reduced tackiness, decreased gloss (i.e. , providing a matte effect), increased shear strength, better abrasion resistance, improved dry time, improved fade resistance, lower blistering, and / or improved hand (a less tacky feel), for example, as compared to a latex composition that only differs by not comprising the insoluble alpha-glucan particles.

[0101] A latex composition herein can be applied to the substrate of an article (above) using any method known in the art. Typically, after application of the latex composition, at least a portion of the aqueous solution is removed, for example by drying, to provide an adhesive, film, coating, or binder comprising the latex composition in a dry or semidry form. Suitable application methods include air knife coating, rod coating, bar coating, wire bar coating, spray coating, brush coating, cast coating, flexible blade coating, gravure coating, jet applicator coating, short dwell coating, slide hopper coating, curtain coating, flexographic coating, size-press coating, reverse roll coating, and transfer roll coating. A latex composition can be applied on at least a portion of a substrate, and can be in one or more coats / applications, for example.

[0102] Some aspects herein are drawn to a pigment-comprising composition. Examples of a pigment-comprising composition herein include any of such compositions disclosed elsewhere herein (e.g., paint, primer, stain), ink, dye (e.g., food-coloring dye, fabriccoloring dye), resin, sunscreen, and cosmetics (e.g., mascara, blush, nail varnish / polish, lipstick, gloss, eyeliner, foundation, eye shadow, skin decoration composition). A pigment in a pigment-comprising composition can be any pigment herein, for example. Examples of a pigment for these and / or other aspects herein include oxides of titanium (e.g., titanium dioxide), zinc, iron, zirconium, cerium, and chromium; manganese violet; ultramarine blue; chromium hydrate; Prussian Blue; zinc sulfide; nitroso, nitro, azo, xanthene, quinoline, anthraquinone and / or phthalocyanine compounds; metal complex compounds; and isoindolinone, isoindoline, quinacridone, perinone, perylene, diketopyrrolopyrrole, thioindigo, dioxazine, triphenylmethane and / or quinophthalone compounds. Further pigment examples useful herein are disclosed in U.S. Patent. Appl. Publ. No. 2006 / 0085924, which is incorporated herein by reference.

[0103] Some aspects herein regard a method / process of producing an aqueous composition as presently disclosed. Such a method can comprise: (a) providing an aqueous composition herein (e.g., an aqueous composition with a pH of 12.5 to 13.2 and comprising alpha-glucan herein, wherein a first fraction of the alpha-glucan is dissolved in the aqueous composition, and a second fraction of the alpha-glucan is not dissolved in the aqueous composition; any feature thereof can be as disclosed herein, for example) that further comprises at least one hydrophobic additive (that is not chemically [covalently] linked to the alpha-glucan) (the hydrophobic additive is aqueous- insoluble under non-caustic conditions [e.g., water-insoluble] and caustic conditions), (b) reducing the pH (e.g., pH neutralization, reducing pH to ~5.5 to ~8.5, or to ~6.0 to ~8.0) of the aqueous composition of step (a), thereby precipitating the alpha-glucan of the first fraction (e.g., thus now, typically, none of the alpha-glucan of aqueous composition is dissolved in the aqueous composition). In some aspects, the aqueous composition provided in step (a) is an emulsion, and an emulsion is produced with step (b). Any of the features of such methodology can be as disclosed herein, as suitable / appropriate, for example.

[0104] Step (b) follows step (a) in typical aspects of producing an emulsion using this methodology. Thus, in such aspects, providing the emulsion in step (a) does not comprise pH neutralization before or during any mixing, such as homogenization, used to provide the emulsion in step (a).

[0105] Reducing the pH in step (b) can comprise adding one or more acids to the aqueous composition of step (a), for example. Examples of suitable acids herein include weak acids (e.g., citric acid, acetic acid) or strong acids (e.g., sulfuric acid). In some aspects, the amount of acid added would result in an acid concentration of about 0.008, 0.010, 0.012, 0.0125, 0.013, 0.014, 0.015, 0.020, 0.025, 0.030, 0.040, 0.050, 0.075, 0.10, 0.25, 0.50, 1 , 2.5, 5, 0.008-0.020, 0.008-0.015, 0.010-0.020, 0.010-0.015, or 0.01- 0.014 wt% (where such wt% would occur if the acid was not consumed during the ensuing neutralization). In some aspects, the amount of acid added is a suitable amount that can result in neutralizing the pH of the aqueous composition provided in step (a), such as to a pH of -5.5 to ~8.5, ~6.0 to ~8.0, ~6.5 to -7.5, or -7.0.

[0106] In some aspects, a method of producing an aqueous composition can be performed as disclosed in the below Examples, but with conditions / parameters (e.g., temperatures, pH values, mixing speeds, time periods, and / or concentrations) that are within 5%, 10%, 15%, and / or 20% of the disclosed conditions / parameters.

[0107] Non-limiting examples of compositions and methods disclosed herein include:

[0108] 1. An aqueous composition with a pH of 12.5 to 13.2 (e.g., pH 12.6 to 13.1 , pH 12.7 to 13.1 , pH 12.7, pH 12.8, pH 12.9, pH 13.0, or pH 13.1) and comprising alpha-glucan, wherein a first fraction of the alpha-glucan is dissolved in the aqueous composition, and a second fraction of the alpha-glucan is not dissolved in the aqueous composition (i.e., the alpha-glucan is partially dissolved in the aqueous composition), wherein at least about 50% of the glycosidic linkages of the alpha-glucan are alpha-1 ,3 glycosidic linkages and typically the weight-average degree of polymerization (DPw) of the alpha-glucan is at least 15 (the alpha-glucan typically is water-insoluble - i.e., the alpha-glucan is insoluble under aqueous conditions of neutral pH such as pH 7.0) (e.g., the aqueous composition comprises a dispersion of the undissolved alpha-glucan of the second fraction).

[0109] 2. The aqueous composition of embodiment 1 , wherein at least about 90% (e.g., > -95%, or about 100%) of the glycosidic linkages of the alpha-glucan are alpha-1 ,3 glycosidic linkages.

[0110] 3. The aqueous composition of embodiment 1 or 2, wherein the DPw of the alphaglucan is at least about 400 (e.g., DPw is about, or at least about, 600, 700, 800, or 700- 900; e.g., DPw is about, or at least about, 1400, 1500, 1600, 1500-1700, or 1600-1800).

[0111] 4. The aqueous composition of embodiment 1 , 2, or 3, further comprising at least one hydrophobic additive (that is not chemically [covalently] linked to the alpha-glucan) (the hydrophobic additive is aqueous-insoluble under non-caustic conditions [e.g., waterinsoluble] and caustic conditions).

[0112] 5. The aqueous composition of embodiment 4, which comprises an emulsion (i.e., the hydrophobic additive is dispersed in the aqueous phase of the aqueous composition, typically by having performed a mixing process on the aqueous composition such as homogenization).

[0113] 6. The aqueous composition of embodiment 4 or 5, wherein said at least one hydrophobic additive comprises an oil (and / or a wax). 7. The aqueous composition of embodiment 1 , 2, 3, 4, 5, or 6, which comprises about 0.5 to 3.0 percent by weight (e.g., about 0.5-2.5, 0.5-2.0, 0.5-1 .5, 1 .0-3.0, 1 .0-2.5, 1.0-2.0, or 1.0-1 .5 wt%) of said alpha-glucan (based on total of both said first and second fractions).

[0114] 8. The aqueous composition of embodiment 4, 5, 6, or 7, which comprises about 30 to 70 percent by volume (e.g., about 40-60, 45-55, or 50 vol%) of said at least one hydrophobic additive.

[0115] 9. The aqueous composition of embodiment 8, which comprises about 0.25 to 1 .5 percent by weight (e.g., about 0.25-1.25, 0.25-1.0, 0.25-0.75, 0.5-1.5, 0.5-1.25, 0.5-1.0, or 0.5-0.75 wt%) of said alpha-glucan (based on total of both said first and second fractions).

[0116] 10. The aqueous composition of embodiment 1 , 2, 3, 4, 5, 6, 7, 8, or 9, wherein the pH is 12.6 to 13.1 (e.g., pH 12.7 to 13.1 , pH 12.7, pH 12.8, pH 12.9, pH 13.0, or pH 13.1).

[0117] 11. An aqueous composition produced by reducing the pH (e.g., pH neutralization, reducing pH to about 5.5-8.5, 6.0-8.0, or 7.0) of the aqueous composition of embodiment 4, 5, 6, 7, 8, 9, or 10, wherein said reducing the pH precipitates the alpha-glucan of the first fraction (now, typically, none of the alpha-glucan of aqueous composition is dissolved in the aqueous composition).

[0118] 12. An aqueous composition produced by reducing the pH (e.g., pH neutralization, reducing pH to about 5.5-8.5, 6.0-8.0, or 7.0) of the aqueous composition of embodiment 4, 5, 6, 7, 8, 9, or 10, wherein said reducing the pH precipitates the alpha-glucan of the first fraction (now, typically, none of the alpha-glucan of aqueous composition is dissolved in the aqueous composition), wherein the aqueous composition comprises an emulsion (i.e., the hydrophobic additive is dispersed in the aqueous phase of the aqueous composition) (e.g., the hydrophobic additive is an oil, and the emulsion is an oil-in-water -type emulsion) (i.e., the emulsion that was previously of an elevated pH with both the first and second alpha-glucan fractions has now been pH-reduced to form a more neutral pH emulsion having mainly, or only, undissolved alpha-glucan [with respect to the alpha-glucan component of the emulsion]).

[0119] 13. The aqueous composition of embodiment 12, wherein the emulsion is a Pickering emulsion (e.g., the hydrophobic additive is an oil, and the Pickering emulsion is an oil-in- water -type emulsion).

[0120] 14. The aqueous composition of embodiment 11 , 12, or 13, wherein the aqueous composition is in the form of, or comprised in, a household care product, personal care product, industrial product, ingestible product (e.g., food product), or pharmaceutical product (i.e. , the aqueous composition can be in the form of, or comprised in, an aqueous product).

[0121] 15. The aqueous composition of embodiment 14 wherein the aqueous composition is in the form of, or comprised in, a lotion or serum.

[0122] 16. The aqueous composition of embodiment 15, wherein the lotion or serum is a skin care product (which typically is of a personal care product or pharmaceutical product).

[0123] 17. The aqueous composition of embodiment 11 , 12, 13, 14, 15, or 16, wherein the aqueous composition has enhanced stability (e.g., stable emulsion).

[0124] 18. The aqueous composition of embodiment 11 , 12, 13, 14, 15, 16, or 17, wherein the aqueous composition has enhanced viscosity.

[0125] 19. A method (process) of producing an aqueous composition (e.g., according to any of embodiments 11 , 12, 13, 14, 15, 16, 17, or 18), said method comprising:

[0126] (a) providing an aqueous composition according to embodiment 4, 5, 6, 7, 8, 9, or 10, and

[0127] (b) reducing the pH (e.g., pH neutralization, reducing pH to ~5.5 to ~8.5, or to ~6.0 to ~8.0) of the aqueous composition of step (a), thereby precipitating the alpha-glucan of the first fraction (e.g., now, typically, none of the alpha-glucan of aqueous composition is dissolved in the aqueous composition).

[0128] 20. The method of embodiment 19, wherein the aqueous composition provided in step (a) is according to embodiment 5, 6, 7, 8, 9, or 10 (i.e., comprises an emulsion, typically wherein such emulsion has already been subjected to a suitable emulsification mixing procedure such as homogenization to provide the emulsion), wherein the aqueous composition resulting from step (b) is an emulsion (e.g., the hydrophobic additive is an oil, and the emulsion is an oil-in-water -type emulsion) (i.e., the emulsion that was previously of an elevated pH with both the first and second alpha-glucan fractions has now been pH-reduced to form a more neutral pH emulsion having mainly, or only, undissolved alpha-glucan [with respect to the alpha-glucan component of the emulsion resulting from step (b)]).

[0129] 21 . The method of embodiment 20, wherein step (b) follows step (a) (i.e., providing the emulsion in step [a] does not comprise pH neutralization before or during any mixing, such as homogenization, used to provide the emulsion in step [a]). 22. The method of embodiment 19, 20, or 21 , wherein said reducing the pH comprises adding a suitable acid (in a suitable amount) to the aqueous composition of step (a).

[0130] 23. An aqueous composition produced according to the method of embodiment 19, 20, 21 , or 22 (e.g., an aqueous product in the form of, or comprising, the aqueous composition).

[0131] EXAMPLES

[0132] The present disclosure is further exemplified in the following Examples. It should be understood that these Examples, while indicating certain aspects herein, are given by way of illustration only. From the above discussion and these Examples, one skilled in the art can ascertain the essential characteristics of the disclosed embodiments, and without departing from the spirit and scope thereof, can make various changes and modifications to adapt the disclosed embodiments to various uses and conditions.

[0133] Preparing Stable Oil-in-Water Emulsions Using Water-Insoluble Alpha-Glucan Having a High Content of Alpha-1 ,3 Glycosidic Linkages Overview

[0134] Polysaccharide-based particles are valued for their low toxicity, biodegradability, and their environmentally friendly production that aligns with green chemistry principles. Yet, their potential in stabilizing Pickering emulsions has not been fully realized. Herein, we introduced a new emulsion design strategy that leverages a solubility window of alpha-1 , 3-glucan in an alkaline aqueous environment. By adjusting the pH to dissolve and subsequently precipitate alpha-1 , 3-glucan in a controlled manner, we introduced a new route for tuning microstructure and rheological properties of emulsions. We demonstrated herein that optimal conditions generally occur at a pH level where solubilized alpha-1 , 3-glucan chains coexist with their precipitated counterparts in a specific ratio. While not intending to be held to any particular theory, we propose that the solubilized chains adsorb onto the still-precipitated agglomerates, imparting steric hindrance to further aggregation, while the remaining fraction in solution serves as depletants between the precipitates, thereby inducing entropic repulsion. This dual role is utilized to control the precipitated alpha-1 , 3-glucan particle size, dispersion extent of the precipitates, and the network formed between them. The enhanced particle surface area induced by the increased particle dispersion facilitates the stabilization of a significantly larger interface compared to emulsions formed with alpha-1 , 3-glucan (“as received” alpha-1 , 3-glucan, FIG. 1) that had not undergone a solubilization / precipitation process as presently disclosed. The subsequent neutralization of the emulsion from alkaline pH precipitated the remaining soluble alpha-1 , 3-glucan fraction and strengthened the particle network between oil droplets, resulting in improved stability of the emulsion.

[0135] The work disclosed in this Example of exploring pH-controlled alpha-1 , 3-glucan particle solubility and precipitation now provides for further enhancing stabilization of the oil / water interface in emulsion systems with alpha-1 , 3-glucan. As illustrated in FIG. 1 , leveraging the unique solubility window of alpha-1 , 3-glucan, we strategically first solubilized alpha-1 , 3-glucan at elevated pH, and subsequently neutralized this system to reach an equilibrium in which both water-soluble alpha-1 , 3-glucan chains and the already precipitated, water-insoluble alpha-1 , 3-glucan particles coexist. We showed that a small difference in pH ranging from 13.4 to 12.7 significantly affects the ratio between soluble chains and the already precipitated portion. We demonstrated significant differences in both microstructure and rheological performance of the prepared emulsions as a function of this ratio. The subsequent neutralization of the emulsion, achieved through addition of acid in a single step, resulted in the complete precipitation of alpha-1 , 3-glucan. Through the transition from a partially dissolved alpha-1 , 3-glucan system in the emulsion formed at elevated pH to a fully precipitated one, we demonstrated that oil droplets serve as a barrier against the formation of large alpha- 1 , 3-glucan aggregates, while the alpha-1 , 3-glucan network formed in aqueous channels between oil droplets contributes significantly to the rheological properties and overall observed emulsion stabilization.

[0136] Materials and Methods

[0137] The alpha-1 , 3-glucan used in this work was initially in powder form having a purity of >99%, an average particle size of 3 pm and zeta potential of almost zero over a wide pH range. Sodium hydroxide (reagent grade, >97%), citric acid monohydrate (reagent grade, >99%), dodecane (anhydrous, >99%), and perylene (sublimed grade, >99.5%) were purchased from Sigma Aldrich and used as received. Purified water collected from a MILLI-Q system was used.

[0138] Representative Preparation of Alpha-1 , 3-Glucan: Alpha-1 , 3-glucan with -100% alpha-1 ,3 glycosidic linkages can be synthesized, for example, following the procedures disclosed in U.S. Appl. Publ. No. 2014 / 0179913 (see Example 12 therein, for example), which is incorporated herein by reference.

[0139] As another example, a slurry of alpha-1 , 3-glucan with -100% alpha-1 ,3 glycosidic linkages was prepared from an aqueous solution (0.5 L) containing Streptococcus salivarius GtfJ enzyme (100 unit / L) as described in U.S. Patent Appl. Publ. No. 2013 / 0244288 (incorporated herein by reference), sucrose (100 g / L), potassium phosphate buffer (10 mM), and FermaSure® antimicrobial agent (100 ppm) adjusted to pH 5.5. The resulting enzyme reaction was maintained at 20-25 °C for 24 hours. A slurry was formed since the alpha-1 , 3-glucan synthesized in the reaction was aqueous- insoluble. The alpha-1 , 3-glucan solids were then collected using a Buchner funnel fitted with a 325-mesh screen over 40-micrometer filter paper.

[0140] The weight average degree of polymerization (DPw) of alpha-1 , 3-glucan used in this study was about 800, and about 100% of the glycosidic linkages of the alpha-1 , 3- glucan were alpha-1 ,3 glycosidic linkages.

[0141] Preparation of Alpha-1 , 3-Glucan Stock Solution: Alpha-1 , 3-glucan powder was dissolved in NaOH (8 M). Briefly, stock solutions at 3, 4 and 6 wt% of alpha-1 , 3-glucan were prepared by dispersing the required weight of glucan powder in purified water (16.6 g) and stirring for 5 minutes. Next, NaOH solution (2.2 g, 8 M) was added to the dispersion and stirred for 40 minutes to dissolve the material at pH > 13.4. Next, the stock solutions were diluted in one step with a precise amount of purified water and stirred for 2 minutes using magnetic stirrer at 300 rpm to prepare alpha-1 , 3-glucan dispersions (partially dissolved system) having an alpha-1 , 3-glucan loading of 1 wt% or 1.5 wt% with the pH ranging from pH 13.1 to 12.7.

[0142] Preparation of Alpha-1 , 3-Glucan Emulsions: Alpha-1 , 3-glucan dispersions at pH ranging from 12.7 to 13.1 and at 1 wt% or 1 .5 wt% loading were used to prepare emulsions at a 50 / 50 oil (dodecane) / water ratio. Each emulsion was prepared using a rotor-stator homogenizer (Pro Scientific PRO 250) and mixing for 2 minutes. These emulsions were neutralized to pH 7.0 by adding citric acid (CA, 1 M) after the emulsification step. The emulsion prepared from the “as-received” alpha-1 , 3-glucan powder only dispersed in purified water without subsequent pH modulation (dissolution and precipitation steps) was used as the control sample. To help study the continuous phase of the emulsions, dispersions made from the above pH modulation procedure, but without any added oil (referred to as “alpha-1 , 3-glucan dispersions” herein below), were characterized as well.

[0143] Solubility Measurements of Alpha-1 , 3-Glucan System Dissolved In NaOH: Alpha- 1 , 3-glucan powder was added to different vials and dispersed in purified water (1 wt% glucan). Next, varying amounts of an 8 M NaOH solution (to produce solutions with different pH) were added to the vials (the total weight of each solution was maintained at 30 g by balancing water and NaOH amount), and pH readings were taken after mixing for 40 minutes. The resulting solutions were then centrifuged at 3200 rpm for 10 minutes to separate non-dissolved alpha-1 , 3-glucan particles in the sediment from the solubilized portion in the supernatant. The supernatant was separated via decantation. The sediment was then redispersed in purified water and washed thoroughly in a vacuum filtration system. These steps were repeated until an alpha-1 , 3-glucan powder with neutral pH was collected ensuring that NaOH was removed completely. The dispersion was dried overnight in an oven at 70 °C, and the relative solubility at different pHs was calculated using this equation: S=(w0-wi) / w0, where S is the relative solubility, wo is the initial weight of alpha-1 , 3-glucan powder, and wi is the weight of the insoluble fraction in the sediment.

[0144] Contact Angle: A 1 .5 wt% dispersion of alpha-1 , 3-glucan at pH 12.9 was casted onto microscope slides and left to air dry overnight followed by oven-drying at 70 °C for 1 hour prior to measurement. The measurement was conducted using a sessile drop test with MILLI-Q water on a DataPhysics contact angle meter.

[0145] Dynamic Light Scattering: Particle size was measured using a disposable cell on a Malvern ZETASIZER PRO at room temperature. Measurements were conducted immediately after sample preparation to minimize effects of particle aggregation and repeated at least two times.

[0146] Confocal Laser Scanning Microscopy (CLSM): The samples were imaged using a Leica SP8 inverted CLSM at excitation wavelengths of 405 nm and 640 nm. Dodecane was tagged with perylene (0.01 mg / mL) and imaged at 405 nm (appears green). Alpha-1 , 3-glucan particles were imaged in the reflectance mode at 640 nm (appears red). Images were obtained using a water immersion objective at 25X magnification and 0.95 numerical aperture. The images have a resolution of 252 nm / pixel. Consequently, the images obtained by the CLSM can either resolve “as received” alpha-1 , 3-glucan particles or reflect the average particle concentration within the emulsion when they are precipitated at elevated pH. The intensity at a given point in the image represented the average local number concentration of particles, with brighter areas indicating higher concentrations at the local level. Droplet size analysis was performed on emulsions using Amira Avizo 3D software.

[0147] Scanning Electron Microscopy: Emulsion microstructure was imaged using cryogenic scanning electron microscopy (FEI Quanta FEG 250 SEM). Briefly, samples were loaded onto a slotted aluminum stub and placed on the sample carrier. The assembly was then submerged into nitrogen slush to freeze the sample. The sample was then transferred into the Gatan ALTO 2500 cryogen prep chamber, where it was held at -150 °C and fractured under vacuum. After fracturing, the temperature in the prep chamber was set to -95 °C for 10 minutes to sublime the top layer of ice. The temperature was then cooled to -150 °C and a thin layer of AuPd alloy was sputtered onto the surface. The sample was transferred under high vacuum onto a Gatan cryostage installed in the specimen chamber of the SEM, where images were collected at 10 kV beam energy in both SE and BSE modes. The fracture typically passed through, over or under oil droplets, resulting in protruding, concave, and dissected regions with irregular shaped droplets in some cases.

[0148] Rheology: A stress-controlled rotational rheometer (Anton Paar MCR-302) with a parallel plate geometry and a gap size of 1 mm was used to perform oscillatory strain sweep measurements on emulsions and dispersions. Amplitude sweeps were performed at a frequency of 1 Hz. The measurements were performed after one day of aging and repeated at least two times. Results and Discussion

[0149] Leveraging Alpha-1 , 3-Glucan Solubility to Increase Particle Surface Area: Since alpha-1 , 3-glucan herein isolated as a dry powder from a bioprocess generally does not show any charge (essentially zero zeta potential), it exists naturally as aggregates with a size of -3 pm (FIG. 2b), and dispersion of these aggregates is not colloidally stable (FIG. 2a, Vial 1). FIG. 2a depicts the solubility curve of alpha-1 , 3-glucan as a function of pH, detailing the proportion of soluble alpha-1 , 3-glucan chains at various pH levels for a 1 wt% loading dispersion. At pH of > 13.4, the alpha-1 , 3-glucan powder is completely dissolved in NaOH (FIG. 2a, Vial 2). However, the solubility of alpha-1 , 3-glucan is a complex system depending on factors such as concentration in the solution which shifts the pH of the solubility window.

[0150] By subsequently reducing the pH of the solution from 13.4 to 12.9 via dilution with water (FIG. 2a), the concentration of alpha-1 , 3-glucan and the strength of basic environment diminished, weakening the interaction between R-O_(glucan) and Na+. This, in turn, restored much of the inter- and intra-molecular hydrogen bonding between hydroxyl groups of the alpha-1 , 3-glucan polymer and produced a partially soluble system where soluble chains and precipitates coexist. This process resulted in the reduction of the original, “as received” alpha-1 , 3-glucan particle average size from -3 pm (FIG. 2b) to ~0.6 pm (FIG. 2c). Forming emulsions by introducing an additional oil phase at this stage (FIG. 2a) was favourable due to the larger surface area and improved dispersion of the alpha-1 , 3-glucan particles provided by the reduced average particle size, allowing the particles to stabilize a larger oil / water interface. When the pH was shifted from 13.4 to 12.9 by using citric acid (1 M), the resulting dispersion started to yield large alpha-1 ,3-glucan aggregates. This outcome was driven by the local supersaturation induced by the acid addition into the viscous solution at pH 13.4; essentially as the alpha-1 , 3-glucan polyanion was being neutralized, intermolecular hydrogen bonding was enabled again to start forming larger structures that cross the solubility threshold, and it was assumed that the generated sodium citrate only loosely interacted with the polysaccharide at this point. In such an environment, the solute molecules diffused at a markedly slower rate, leading to a localized decrease in pH and consequently large local supersaturation. This scenario resulted in uncontrolled nucleation of particles in close proximity to each other, leading to their coagulation, as seen by the DLS analysis (data not shown). Additionally, adjusting pH directly from 7.0 to 12.9 (FIG. 2a) by adding NaOH dissolved an equivalent fraction of alpha-1 , 3-glucan particles. However, this alteration had little impact on reducing the size of pre-existing aggregates, since only the chains at the edge of the aggregates were dissolved, as confirmed by the DLS (data not shown).

[0151] Solubility-Dependent Dispersion of Alpha-1 , 3-Glucan Particles, Emulsion Microstructure and Rheological Signature: To elucidate the influence of dissolved alpha- 1 , 3-glucan chains on their ability to aid dispersion stabilization of the already precipitated alpha-1 , 3-glucan particles as well as assess their impact on gelation kinetics and emulsion formation, we prepared dispersions with 1 wt% loading at pH 12.7, 12.9 and 13.1 by diluting stock solutions of 3, 4 and 6 wt% respectively, using dilution factors of 3, 4 and 6 times in each case. The dilution pathways can be seen in FIG. 3 along with a schematic representation of the dispersion microstructure at different pH as insets.

[0152] We conducted non-invasive CLSM imaging of these dispersions within 1 hour and after 1 day of preparation. CLSM imaging captured within 1 hour revealed the highest extent of aggregation at pH 12.7 dispersion, at which -17% of the alpha-1 , 3- glucan existed in a dissolved state (see FIG. 3). However, the CLSM imaging of pH 12.9 and 13.1 dispersions, corresponding to systems with -20% and -33% of alpha-1 ,3- glucan in a dissolved state, respectively, showed no significant reflectance signal. While the fraction of precipitated alpha-1 ,3-glucan in these systems was substantial, their size was below the resolution limit at these imaging conditions, accounting for their absence in the images (data not shown). This agreed with DLS measurements, which revealed that although all three systems contain precipitates, their respective sizes differed, with the precipitates (from largest to smallest) existing at pH 12.7 (average diameter 0.78 p.m), pH 12.9 (average diameter 0.57 .m) and pH 13.1 (average diameter 0.3 .m). CLSM imaging after 1 day of preparation showed a relatively unchanged network for 1 wt% dispersion at pH 13.1 (data not shown). In contrast, at pH 12.7, the imaging revealed a particle network predominantly composed of large and disconnected aggregates, and weak gel formation. At pH 12.9, imaging revealed that the particle network provided a relatively uniform reflectance signal, indicating the greatest extent of dispersion of the precipitates and reduction in inter-particle distance among the precipitates over the gelation period resulting in a stronger network. Conversely, at pH 13.1 , with -33% of soluble chains, the inter-particle distance between precipitates became excessively large due to the presence of a significant number of soluble chains. This prevented effective interactions and formation of a robust network, which result corresponded to the dark reflectance signal in the confocal image (data not shown).

[0153] Rheological characteristics were probed using amplitude sweep measurements. Plots of G' (storage modulus) and G" (loss modulus) versus shear strain revealed the disruption of microstructure with increasing strain where storage modulus signifies energy stored within the elastic structure of the emulsion and loss modulus signifies the energy dissipated by the system under stress. Amplitude sweeps conducted on these dispersions after 1 day (FIG. 4) were consistent with the extent of particle networks in the CLSM images: the largest G' and G" corresponded to the pH 12.9 dispersion. While the pH 13.1 dispersion exhibited the weakest G' and G", its crossover strain (the strain at which G' and G" intersect) is the largest, signifying a transition from predominantly elastic to predominantly viscous behavior occurring at the largest strains. This agreed with the acquired confocal imaging that revealed absence of a particle network (data not shown). In contrast, the pH 12.7 dispersion indicated the most brittle network induced by the most pronounced particle aggregation extent as evidenced by the smallest crossover strain. These results indicate an importance of striking a delicate balance among the ratio of solubilized to precipitated alpha-1 , 3-glucan, which influences the size of precipitated alpha-1 , 3-glucan particles, the number of soluble chains, and the interparticle distance favorable for strong network formation.

[0154] Based on the evolving microstructure over a 1-day period and rheological signature of dispersions, we propose the dual role of soluble alpha-1 , 3-glucan chains. We anticipate that, in the process of reaching equilibrium between nucleation and growth of alpha-1 , 3-glucan precipitates, a fraction of soluble chains adsorbs onto the surface of the precipitates owing to the hydrogen bonding sites present. Since the overall particle charge does not change when soluble chains are adsorbed on it, they impart steric hindrance, preventing the aggregation of precipitates. Simultaneously, the remaining fraction of soluble chains in solution act as depletants, establishing a depletion layer that induces depletion stabilization among the precipitates based on their concentration. The dual functionality of soluble chains was evident by the absence of large aggregates and lack of network formation in the pH 13.1 (-33% soluble chains) dispersion, as compared to the pH 12.7 dispersion which showed significant aggregation and network formation (data not shown). These observations also underscore the importance of achieving the optimal ratio between the soluble and precipitated fractions. An excess of soluble alpha- 1 ,3-glucan chains can result in large inter-particle distances, while an insufficient concentration of solubilized alpha-1 ,3-glucan chains fails to supress the aggregation of precipitates. It is important to note that depletion stabilization offers a kinetic stability, and over time, as particles equilibrate, particle networks can still be formed.

[0155] CLSM imaging was conducted on emulsions prepared from the 1 wt% alpha-1 , 3- glucan dispersions at pH of 12.7, 12.9 and 13.1 (see Materials and Methods). While only the dispersion at pH 12.9 could sustain its weight, the emulsions across the entire range of pH levels tested exhibited the ability to support their own weight upon vial inversion. This observation suggests the impact of an additional oil / water interface formed during the emulsification process on the rheological properties of these systems. The CLSM imaging indicated that particles remained largely in water phase, indicating a lack of specific affinity to the oil and water interface (data not shown). Although particles at the oil / water interface were not apparent at pH 12.7 and 12.9, it is important to note that the high curvature of small droplets (average diameters: 12.6 m ±3.9 pm for the pH 12.7 emulsion, 8.0 pm ±4.0 pm for the pH 12.9 emulsion) might have affected the CLSM reflectance signal. Conversely, interfacial localization was evident in the larger droplets of the pH 13.1 emulsion (18.0 pm ±10.9 pm), suggesting the presence of particles at the interface in the other two emulsions as well.

[0156] However, the adsorption of an alpha-1 ,3-glucan particle at the oil / water interface was not due to the particle’s affinity for it, as alpha-1 , 3-glucan displayed hydrophilic behavior with a water contact angle of 37°. Instead, it is attributed to the fact that the particles localized there during the process of preventing droplet-droplet coalescence by establishing a particle network in the aqueous phase. Additionally, once adsorbed, their anisotropic shape resulted in higher desorption energy which further enhances the stability of the emulsion. This observed emulsion microstructure was consistent with the microstructure and rheological characteristics of the corresponding dispersions. Given that these particles primarily stabilized droplets by forming an inter-particle network within the aqueous phase and impeded droplet coalescence through steric hindrance, the effectiveness in stabilizing the interfacial area depends on the strength and brittleness of the network they form.

[0157] At pH 12.9, the strongest emulsion network existed, resulting in the smallest droplet diameters as imaged by CLSM (data not shown). At pH 12.7, particle aggregation was more pronounced, but still effective in stabilizing a large oil / water interface. On the other hand, the emulsion generated at pH 13.1 exhibited the largest droplet diameters, consistent with the presence of numerous soluble chains, a large inter-particle distance (as viewed by CLSM imaging, indicated by extensive dark regions in the aqueous phase [data not shown]), and a weak particle network unable to prevent droplet coalescence. The rheological characteristics of these emulsions (FIG. 5) revealed elevated G' and G" values when compared to their dispersion counterparts (FIG. 4), signifying the contribution from an elastic oil / water interface in each case. As expected from the above data, the emulsion at pH 12.9 exhibited the highest G' and G" values, with similar crossover strains observed across all the other systems.

[0158] Neutralization Preserves Emulsion Microstructure and Strengthens Particle Network: To assess the effectiveness of higher alpha-1 , 3-glucan particle loading, we prepared emulsions at the optimal pH of 12.9 using a corresponding 1.5 wt% alpha-1 , 3- glucan dispersion (see Materials and Methods). Subsequently, we examined the impact of neutralizing these emulsions to form emulsions at pH 7.0, comparing them to emulsions generated from “as-received” alpha-1 , 3-glucan that was not subjected to the above dissolution and in-situ precipitation process. CLSM imaging of the emulsion (pH 7.0) from “as-received” alpha-1 , 3-glucan powder revealed large aggregates in the aqueous phase (data not shown), consistent with previous observations (Kedzior et al., 2020, Carbohydrate Polymers 251 : Article no. 117112). These aggregates, with lower surface area, resulted in a weak particle network, which was evident by the existence of isolated aggregates of alpha-1 , 3-glucan (data not shown). Consequently, the resulting emulsion exhibited distinct creaming due to the formation of larger, less stable oil droplets.

[0159] Emulsions prepared at pH 12.9 or neutralized from pH 12.9 to pH 7.0 showed a more uniform emulsion microstructure under CLSM imaging (data not shown). The average droplet diameters were significantly smaller, and there were no visible large aggregates in the aqueous phase. While the emulsion of “as-received” alpha-1 , 3-glucan at pH 7.0 had oil droplets of about 43.5 m (±36.3 pm), the emulsion at pH 12.9 (diluted from pH 13.4) had oil droplets of about 7.0 pm (±3.7 pm), and the emulsion at pH 7.0 (neutralized from pH 12.9) had oil droplets of about 7.3 pm (±4.0 pm). Comparison of pH 12.9 emulsions generated from the initial 1 wt% or 1.5 wt% alpha-1 , 3-glucan pH 12.9 dispersions indicated that there were smaller oil droplet diameters for the emulsion prepared from the 1 .5 wt% dispersion.

[0160] Emulsions at neutral pH are desired for many practical applications. However, neutralization either before or during homogenization resulted in aggregation of alpha- 1 , 3-glucan particles, nullifying the benefit of enhanced particle surface area at pH 12.9 (data not shown). To overcome this, we performed neutralization post-emulsification, which neutralization effectively reinstated inter- and intra-molecular alpha-1 , 3-glucan hydrogen bonding resulting in formation of aggregates. But importantly, due to the presence of emulsion droplets during this neutralization, the aggregates congregated within the confined aqueous channels, ultimately leading to the development of a three- dimensional particle network. This effectively retained the microstructure of the high-pH emulsion (as observed by CLSM, data not shown), resulting in a neutral pH emulsion with a strong particle network.

[0161] Cryo-SEM images of emulsions prepared with “as-received” alpha-1 , 3-glucan particles or alpha-1 , 3-glucan processed at high pH (dissolved and undissolved fractions) or neutral pH (undissolved particles) agreed with CLSM imaging (data not shown). The high aggregation state of neutrally charged “as-received” a-1 , 3-glucan particles was evident at the interface and in the aqueous phase, resulting in lower surface area available for emulsion stabilization. However, in the pH 12.9 emulsion, the network of precipitates in the aqueous phase and at the interface stabilized a larger oil / water interface. The soluble chains present in the pH 12.9 emulsion precipitated during cryogenic freezing. However, due to the speed of the freezing process, the now- precipitated solubilized chains likely remained “frozen” in their positions. Cryo-SEM imaging showed the presence of a web-like structure of particles at the interface and between the droplets, strengthening our hypothesis of the dual function of soluble chains. Upon neutralization to pH 7.0, the emulsion exhibited bridged-droplets combined with a particle network that formed between droplets owing to the in-situ precipitation of remaining soluble chains. This result strengthens our hypothesis that the oil droplets confined alpha-1 , 3-glucan aggregation within narrow aqueous channels and preserved droplet microstructure.

[0162] The amplitude sweeps shown in FIG. 6 show the benefit of the controlled process disclosed herein of alpha-1 , 3-glucan dissolution followed by precipitation in emulsion design. Using the highly aggregated “as received” alpha-1 , 3-glucan particles in a neutral pH aqueous phase - without any intervening dissolution-then-precipitation steps - resulted in a significantly weaker emulsion. Comparison of the G' and G" values of the emulsion formed and kept at pH 12.9 versus the emulsion that is further neutralized from pH 12.9 to pH 7.0 indicates almost an order of magnitude difference due to the strong particle network imparted (to the latter emulsion) by the precipitation of the soluble chains and restoration of inter- and intra-molecular hydrogen bonding between the precipitates. This was evidenced by the formation of a bridged droplet and particle network in CryoSEM imaging (data not shown). The critical strain (cross-over point in FIG. 6) also occurs at a higher level for neutralized emulsion as a result of an enhanced interparticle network, coupled with a uniform particle network distribution.

[0163] Conclusion: In the present disclosure, we presented a novel approach for emulsion stabilization that takes advantage of the pH path-dependent solubilization of alpha-1 , 3-glucan. Unlike naturally occurring polysaccharides, alpha-1 , 3-glucan can be completely dissolved at high pH. Reducing the pH after solubilization (but while still maintaining an elevated pH) precipitates some of the dissolved alpha-1 , 3-glucan, with two consequences: a fraction of the dissolved alpha-1 , 3-glucan chains start to precipitate and adsorb onto each other, while the fraction remaining in solution acts as depletants between those precipitates. This dual role allows for precise control over the size and dispersion of precipitated alpha-1 , 3-glucan particles and the network formed between them. The fraction of precipitated particles is determined by the final pH.

[0164] We found that an optimal ratio of dissolved alpha-1 , 3-glucan to precipitated alpha-1 , 3-glucan at which aggregation is prevented, while enabling formation strong interparticle networks between precipitates. The latter were effective for stabilization of an oil / water emulsion despite the low affinity of the particles for the oil / water interface. Emulsions generated at near-optimal pH were then neutralized with citric acid, which regenerated inter- and intra-molecular hydrogen bonding between hydroxyl groups of glucan polymer chains. Confocal microscopy and amplitude sweep measurements performed on dispersions and emulsions verified the formation of stable gel-like emulsions with small droplet sizes and enhanced rheological performance when the ratio of soluble chains to precipitates was tuned. Cryo-SEM imaging also confirmed the presence of a three-dimensional network at neutral pH that stabilized the emulsion strongly by forming bridged droplet microstructures. This innovative method in emulsion engineering, utilizing alpha-1 , 3-glucan particles with a biocompatible and low hazard profile, offers opportunities for customizing structure and rheology for a range of applications, including cosmetics, food, and beyond. AUXILIARY EXAMPLE

[0165] A process for producing highly crystalline alpha-1 , 3-glucan as disclosed in U.S. Patent Appl. Publ. No. 2021 / 0130504 (incorporated herein by reference) is described in this auxiliary Example. Herein, highly crystalline alpha-1 , 3-glucan is referred to as microcrystalline glucan (MCG).

[0166] The MCG-production process consisted of an acid hydrolysis using 20% methane sulfonic acid (MSA) with alpha-1 , 3-glucan (e.g., DPw -800 or -1600-1800, either molecular weight species having about 100% alpha-1 ,3 glycosidic linkages) performed in a highly mixed reactor for 2-4 hours, followed by raising pH to -3.5-4 using 20% sodium hydroxide, and downstream purification and concentration of the MCG product. To stabilize MCG and provide contamination protection, the MCG was “neutralized” to a pH of 3.5-4 when the reaction was complete. The MCG purification step currently is envisioned to use a membrane filtration step to first remove both salts and sugars and then concentrate the MCG with a target of >10% total suspended glucan solids. The finished product is an MCG slurry solution at greater than 10% total suspended solids with negligible salt (<350 milliSiemens / cm conductivity) and sugar impurities (non- detectable) with a suitable preservative. A flow diagram of this process is presented in FIG. 7.

Claims

CLAIMSWhat is claimed is:

1. An aqueous composition with a pH of 12.5 to 13.2 and comprising alpha-glucan, wherein a first fraction of the alpha-glucan is dissolved in the aqueous composition, and a second fraction of the alpha-glucan is not dissolved in the aqueous composition, wherein at least about 50% of the glycosidic linkages of the alpha-glucan are alpha-1 ,3 glycosidic linkages and the weight-average degree of polymerization (DPw) of the alpha-glucan is at least 15.

2. The aqueous composition of claim 1 , wherein at least about 90% of the glycosidic linkages of the alpha-glucan are alpha-1 ,3 glycosidic linkages.

3. The aqueous composition of claim 1 , wherein the DPw of the alpha-glucan is at least about 400.

4. The aqueous composition of claim 1 , further comprising at least one hydrophobic additive.

5. The aqueous composition of claim 4, which comprises an emulsion.

6. The aqueous composition of claim 4, wherein said at least one hydrophobic additive comprises an oil.

7. The aqueous composition of claim 1 , which comprises about 0.5 to 3.0 percent by weight of said alpha-glucan.

8. The aqueous composition of claim 4, which comprises about 30 to 70 percent by volume of said at least one hydrophobic additive.

9. The aqueous composition of claim 8, which comprises about 0.25 to 1 .5 percent by weight of said alpha-glucan.

10. The aqueous composition of claim 1 , wherein the pH is 12.6 to 13.1.

11. An aqueous composition produced by reducing the pH of the aqueous composition of claim 4, wherein said reducing the pH precipitates the alphaglucan of the first fraction.

12. An aqueous composition produced by reducing the pH of the aqueous composition of claim 5, wherein said reducing the pH precipitates the alphaglucan of the first fraction, wherein the aqueous composition comprises an emulsion.

13. The aqueous composition of claim 12, wherein the emulsion is a Pickering emulsion.

14. The aqueous composition of claim 11 , wherein the aqueous composition is in the form of, or comprised in, a household care product, personal care product, industrial product, ingestible product, or pharmaceutical product.

15. The aqueous composition of claim 14, wherein the aqueous composition is in the form of, or comprised in, a lotion or serum.

16. The aqueous composition of claim 15, wherein the lotion or serum is a skin care product.

17. The aqueous composition of claim 11 , wherein the aqueous composition has enhanced stability.

18. The aqueous composition of claim 11 , wherein the aqueous composition has enhanced viscosity.

19. A method of producing an aqueous composition, said method comprising:(a) providing an aqueous composition according to claim 4, and(b) reducing the pH of the aqueous composition of step (a), thereby precipitating the alpha-glucan of the first fraction.

20. The method of claim 19, wherein the aqueous composition provided in step (a) is according to claim 5, wherein the aqueous composition resulting from step (b) is an emulsion. 21 . The method of claim 20, wherein step (b) follows step (a).

22. The method of claim 19, wherein said reducing the pH comprises adding a suitable acid to the aqueous composition of step (a).

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