Photoluminescent Natural Pigments - Manufacturing Process, Composition, and Cosmetic Applications

By integrating natural dyes into bentonite or kaolin clay substrates via spray-drying, the composition stabilizes color and reduces odor, addressing the instability of anthocyanins and enhancing cosmetic performance.

JP2026500980APending Publication Date: 2026-01-09SENSIENT TECH ASIA PACIFIC PTE LTD
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Patent Information

Application Number
JP2025540964
Authority / Receiving Office
JP · JP
Patent Type
Applications
Current Assignee / Owner
Priority Date
2023-01-13
Filing Date
2024-01-12
Publication Date
2026-01-09

AI Technical Summary

Technical Problem

Natural dyes, particularly anthocyanins, are unstable and prone to irreversible color changes due to light, temperature, and pH variations, leading to reduced performance and shelf life in cosmetic applications, and there is a need for stable, low-odor, non-hygroscopic natural colorants suitable for cosmetics.

Method used

A composition comprising natural dyes integrated into the cationic interlayer of bentonite or kaolin clay substrates through spray-drying, maintaining color stability and luminosity by encapsulating the dyes within the clay matrix, which includes adjusting pH and using optional surface treatment agents.

Benefits of technology

The composition achieves color stability of at least 50-90% over 30 days under high humidity and temperature conditions, reducing odor and moisture absorption, and enhancing luminosity and uniformity in cosmetic applications.

✦ Generated by Eureka AI based on patent content.

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Abstract

Disclosed is a composition comprising a natural dye, a bentonite clay substrate, maltodextrin, and an optional pH adjuster. The composition maintains color stability after 30 days of storage at 28°C and 68% relative humidity. Color stability includes maintaining one or more of the L*, a*, or b* values ​​as measured by reflectance-visible spectroscopy at one or more wavelengths between 400 nm and 800 nm.
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Description

[Technical Field]

[0001] CROSS-REFERENCE TO RELATED APPLICATIONS This application is related to, and is incorporated by reference for all purposes, and claims priority to, U.S. Patent Application No. 63 / 438,990, filed January 13, 2023.

[0002] Statement Regarding Federally Sponsored Research Not applicable.

[0003] Sequence Listing Reference Not applicable.

[0004] The technology of the present disclosure relates generally to compositions comprising natural dyes. More specifically, the technology relates to compositions comprising natural dyes for cosmetic applications. [Background technology]

[0005] Color is one of the key aspects of marketing cosmetics. The ability to capture consumer attention through brilliant, striking, and vibrant hues is a contributing factor to the success of marketing campaigns. Consumers around the world are increasingly concerned about the safety of products they apply to their bodies. Therefore, the demand for natural colorants derived from non-synthetic sources is rapidly growing. Natural dyes can have a wide range of hues and can be very brilliant, but they are often prone to instability, for example, to light, temperature, and pH. For example, anthocyanins can exhibit a variety of brilliant colors ranging from yellow to purple. However, anthocyanins are notoriously unstable, and changes in their molecular structure can result in undesirable, irreversible changes in color, such as degradation to undesirable brown pigments. Therefore, there is a desire to stabilize these natural colorants and develop them in a wider variety of hues suitable for the food, cosmetic, and pharmaceutical industries.

[0006] Therefore, there is a desire to stabilize natural dyes so that the desired color is maintained over an extended period of time, and any product containing natural dyes will therefore have a longer lifespan.

[0007] Existing natural substrates generally have a dull physical appearance, an unpleasant odor, and often absorb moisture, reducing the performance and shelf life of cosmetic products. Furthermore, the supply of these natural substrates remains limited, increasing the difficulty of deploying them for use in applications. Today, synthetic or mineral substrates are generally preferred for use in cosmetic products applied to the body. To meet the growing consumer demand for low-odor, radiant, stable, and non-hygroscopic natural cosmetics, there remains a need for natural colorant and natural substrate compositions that are stable over a wide range of conditions while retaining their original color for extended periods of time. Summary of the Invention

[0008] In one embodiment, disclosed herein is a composition comprising a natural dye in an amount of about 5% to about 35% by weight, a bentonite clay substrate in an amount of about 45% to about 60% by weight, maltodextrin in an amount of about 10% to about 45% by weight, and an optional pH adjuster, wherein the natural dye is at least partially integrated into the cationic interlayer of the bentonite clay substrate by a spray-drying process. The composition maintains color stability after 30 days of storage at 28°C and 68% relative humidity, where the color stability includes maintaining at least about 50%, at least about 60%, at least about 70%, at least about 80%, or at least about 90% of one or more of the L*, a*, or b* values ​​as measured by reflectance-visible spectroscopy at one or more wavelengths between 400 nm and 800 nm. More than about 50%, more than about 60%, more than about 70%, more than about 80%, or more than about 90% of the cations in the cationic interlayer are sodium cations (Na +), and the bentonite clay matrix has a brightness of at least about 50% before the natural dye is at least partially incorporated into the cationic interlayer. Before the natural dye is at least partially incorporated into the cationic interlayer, the bentonite clay matrix has an initial cation exchange capacity of at least about 75 meq / 100 g.

[0009] In another aspect, disclosed herein is a composition comprising a natural dye in an amount of about 20% to about 35% by weight, a kaolin clay substrate in an amount of about 55% to about 70% by weight, an optional pH adjuster, and an optional surface treatment agent, wherein the composition maintains color stability after 30 days of storage at 28° C. and 68% relative humidity. The color stability of the composition includes maintaining at least about 50%, at least about 60%, at least about 70%, at least about 80%, or at least about 90% of one or more of the L*, a*, or b* values ​​as measured by reflectance-visible spectroscopy at one or more wavelengths between 400 nm and 800 nm, and the kaolin clay substrate has a reflectance brightness of at least about 85% as measured by visible reflectance spectroscopy prior to contact with the natural dye.

[0010] In a further aspect, a method of making a powder composition is disclosed, the method comprising: a) homogenizing a natural dye with either i) a bentonite clay having a brightness of at least about 50% and a cation exchange capacity (CEC) of at least about 75 meq / 100 g, or ii) a kaolin clay having a reflectance optical brightness of at least about 85%; b) optionally adjusting the pH of the slurry by adding a pH adjuster; and c) spray drying the slurry at an outlet temperature of about 60° C. to about 120° C. to form a powder.

[0011] In another aspect, a natural pigment composition is disclosed, the composition comprising: a natural dye in an amount of about 3% to about 40% by weight; a clay substrate in an amount of about 20% to about 75% by weight; an optional co-substrate in an amount of about 0% to about 45% by weight; an optional pH adjuster; and an optional surface treatment agent in an amount of about 1% to about 15% by weight, wherein the natural pigment composition is in powder form.

[0012] Non-limiting embodiments of the present disclosure are illustratively described with reference to the accompanying drawings, which are schematic and not intended to be drawn to scale. In the drawings, each identical or nearly identical component illustrated is typically represented by a single numeral. For clarity, not every component is explicitly shown in every drawing, nor are every component of each embodiment of the present invention shown, where illustration is not necessary for those skilled in the art to understand the invention. [Brief explanation of the drawings]

[0013] [Figure 1] The effect of pH on anthocyanin color is shown. Form (A) is red and occurs under acidic, low pH conditions. Form (B) is purple and occurs under nearly neutral conditions, about pH 6-7. Form (C) is blue-green and occurs under basic conditions, or at pH > 7. [Figure 2] 1 is an illustration of the tetrahedron-octahedron-tetrahedron layers of bentonite. [Figure 3] CIELAB space for color measurement. CIELAB or CIE L*a*b* is a device-independent 3D color space that allows the accurate measurement and comparison of all perceptible colors using three color values. [Figure 3a] 1 shows the components of the lipstick formulation used in the test examples. [Figure 4] 1 is a table showing the colorimetric values ​​and corresponding physical appearance of powdered pigment composites using bentonite / montmorillonite as the primary substrate. [Figure 5] 1 is a table showing colorimetric values ​​and corresponding physical appearance of powdered pigment composites using kaolin as the primary substrate. [Figure 6] Photographs showing observation of water sorption on various substrate-pigment composites after 30 days at 28° C. and 68% relative humidity. [Figure 7]1 shows the colorimetric values ​​of red radish compositions measured on day 1 (fresh) and day 6 using Kunipia-F ("Kunipia" is a registered trademark) and ImerCare® Opaque. [Figure 8] 8 shows the corresponding physical color of the pigment composition of FIG. 7 measured on day 1 (fresh) and day 6 as measured by an X-rite spectrophotometer. [Figure 9] 1 is a table of colorimetric values ​​measured by a spectrophotometer on a composite of raw material and purple sweet potato (PSP) pigment. [Figure 10] For the PSP pigment composite in Figure 9, the physical appearance of the powder and lipstick after application to the skin is shown. [Figure 11] 1 shows the physical appearance of powder and lipstick after application to skin for the GB composite material. DETAILED DESCRIPTION OF THE INVENTION

[0014] In consideration of the instability of natural dyes, the present disclosure provides a pigment composition for achieving brilliant shades of natural dyes encapsulated within a natural matrix, enhancing stability over time and in high temperature and humidity conditions. This pigment composition provides improved color stability over a longer period of time compared to other commercially available products, and when used in cosmetic applications, can also provide at least one of high luminosity, reduced odor, reduced moisture adsorption, and better coverage and uniformity. According to one aspect of the present disclosure, the pigment composition includes a natural dye, such as anthocyanin, and a natural matrix comprising bentonite or kaolin.

[0015] natural dyes The pigment compositions disclosed herein include natural dyes. Natural dyes are colored substances obtained from natural sources. Natural dyes can have colors in the visible wavelength range of 400 nm to 800 nm. These colors can be red, orange, yellow, green, blue, purple, and blends of these colors.

[0016] The source of natural dyes can be plant extracts. Plant extracts can be isolated from any part of a plant, such as roots, leaves, flowers, or stems. Additionally and alternatively, the source of natural dyes can include fruit extracts or vegetable extracts. Natural dyes can be derived from biotechnology, such as biosynthesis, bioengineering, or biotechnology-derived color molecules.

[0017] Natural dyes can be soluble in water.Water-soluble natural dyes include anthocyanins.Anthocyanins can be extracted from many kinds of plants, including red radish, wild carrot, purple sweet potato, or butterfly pea.More specifically, anthocyanins can include pelagonidin, peonidin, cyanidin, malvidin, delphinidin, and petunidin, which can be harvested from red radish (Raphanus sativus L.), red sweet potato (Ipomoea batatas L.), wild carrot (Daucus carota L.), red cabbage (Brassica oleracea), grape (Vitis vinifera), elderberry (Sambucus nigra), and strawberry (Fragaroa ananassa). Further examples of water-soluble natural dyes include betaine from beet root extract, norbixin from annatto seed, and genipin complex produced from gardenia jasminoides or Genipa americana fruit extract.

[0018] Natural oil-soluble dyes can include, for example, beta-carotene extracted from algae or fungal extracts, paprika oleoresin extracted from chili peppers, bixin extracted from annatto seeds, and azulene extracted from chamomile flowers.Natural dyes can be in solid form, such as powders, or in liquid form, such as oils.

[0019] Many natural dyes change color with pH. For example, the color of some anthocyanins changes from red (acidic) to purple (neutral) to blue-green (basic). Figure 1 shows that as pH increases, anthocyanins transition from red to green. Form (A) is red and occurs under acidic, low pH conditions. Form (B) is purple and occurs under nearly neutral conditions, about pH 6-7. Form (C) is blue-green and occurs under basic conditions, or at pH > 7.

[0020] substrate The pigment composition can include a natural substrate. In certain embodiments, the substrate can be clay, such as bentonite clay, montmorillonite, or kaolin. Bentonite has a layered structure and ion-exchange properties, making it ideal for use in cosmetic applications. Bentonite clay has the general formula Al2O3·4(SiO2)·H2O and is a layered aluminum phyllosilicate mineral. At the molecular level, bentonite clay is structurally arranged such that one layer contains an aluminum octahedron sheet sandwiched between two tetrahedron silica sheets, known as a tetrahedron-octahedron-tetrahedron (TOT) structure. The TOT layers are slightly negatively charged and balanced by exchangeable interlayer cations. The interlayer cations are sodium (Na + ), calcium (Ca 2+ ), or a mixture of these ions. It may contain other ions such as alkali metal ions, alkaline earth metal ions, or transition metal ions.

[0021] Bentonite layers can shrink or expand depending on the level of hydration. Each monolayer is roughly 1 nm thick. When dry, the layers can stack up to several hundred nanometers thick with interlayer cations. During hydration, the volume of bentonite increases significantly. This swelling phenomenon is due to osmotic swelling. Exchangeable cations can diffuse from regions of high concentration, such as between the layers of the bulk solution, to regions of low concentration. When exchangeable cations diffuse out of the lattice, the negatively charged layers experience electrostatic repulsion, resulting in volume expansion. This layered molecular structure, including the interlayer cations, provides the matrix with a cation exchange capacity (CEC), or the total capacity of the material to retain exchangeable cations. In one example, the CEC of a bentonite matrix can be at least 75 meq / 100 g, optionally at least 80 meq / 100 g, or optionally at least 85 meq / 100 g.

[0022] Cation exchange capacity is the rate at which the replacement ion, Na, is released while the substrate is in solution. + and / or Ca 2+ The positively charged natural dye can exchange with the exchangeable cations and become encapsulated between the layers when the substrate is dried. For example, when a dry substrate is exposed to a bulk solution of a positively charged natural dye, as shown in FIG. 1A, the layers move apart and at least some of the cations migrate from between the layers. At this point, the positively charged natural dye can replace the exchangeable cations and migrate between the layers. The presence of the positively charged natural dye between the layers stabilizes the negatively charged layer. When the substrate is dry, the positively charged natural dye can be trapped between the layers. Thus, the natural dye can be at least partially integrated or intercalated within the layers of the substrate.

[0023] As a natural substrate, bentonite is available from commercial sources in various forms. As a natural substrate, the present disclosure specifically includes the use of Kunipia-F from Kunimine Industries Co., Ltd. Kunipia is a high-purity sodium montmorillonite and can have the properties shown in Table 1 below. Table 1: Exemplary properties of Kunipia-F [Table 1] Viscosity: 4% dispersion solution, BM type viscometer, 60 rpm, 25℃ Whiteness; brightness by Hunter

[0024] Another natural substrate that can be used in the pigment compositions disclosed herein is kaolin, which has the formula Al2Si2O5(OH)4. Kaolin has stacked tetrahedron-octahedron (TO) layers, with the T and O layers composed of silicon and aluminum, as previously described for bentonite. Kaolin has two sheets in each layer, strongly bonded together through shared oxygen ions. The layers are bonded to each other through hydrogen bonds between oxygen on the outer surface of the T sheet of one layer and hydroxyl groups (-OH) on the outer surface of the O sheet of the next layer. Because the kaolin layers have no net charge, there are no cations (such as calcium, sodium, or potassium) between the layers, as in bentonite. Therefore, kaolin has a low ion exchange capacity. The hydrogen bonds between the layers also prevent water molecules from penetrating between the layers, explaining the lack of swelling behavior observed with kaolin.

[0025] When wet, the water molecules loosely bond to the kaolin platelets in a way that allows the platelets to slide past each other when the clay is manipulated, but allows the kaolin clay to retain its molded shape. When the kaolin is dry, the plates hydrogen bond directly to each other.

[0026] Examples of natural substrates include, but are not limited to, Kunipia-F (Kunimine Industries Co., Ltd.), ImerCare® Opaque (Imerys SA), Moistonite-S ("Moistonite" is a registered trademark of Kunimine Industries Co., Ltd.), Moistonite-U (Kunimine Industries Co., Ltd.), Caolin G30M (Veneta Mineraria SPA), Cosmetico, AV-Beige, AV-Red, AV-Grey, etc. Additionally, alternatively, the substrate may be tricalcium citrate, tricalcium phosphate, palm kernel powder, silica, polyhydroxybutyrate, or diatomaceous earth.

[0027] As a natural substrate, kaolin is available from commercial sources in a variety of forms. The present disclosure specifically includes the use of kaolin in the form of ImerCare® Opaque from Imerys SA to achieve the desired performance.

[0028] Whiteness and Luminance Reflectance The whiteness and luminance reflectance of a substrate are important for cosmetic applications and can be measured using spectrophotometric measurements. Luminance reflectance measures visible reflectance of light at a wavelength of, for example, 457 nm, while whiteness measures reflectance at all wavelengths. The pigment composition according to the presently disclosed embodiments can include a substrate with a whiteness of at least 50%, or at least 60%, or at least 70%. Kunipia, a sodium bentonite, can have a whiteness of, for example, at least 50%, or at least 60%, or at least 70%. The pigment composition can also include kaolin with a high luminance reflectance, for example, at least 85%, or at least 90%, or at least 95%.

[0029] Auxiliary substrate The auxiliary substrate can be used to add additional cosmetic application properties, such as increasing the slip effect. The auxiliary substrate can include polysaccharides, such as maltodextrin, chitosan, gum arabic, cellulose, pullulan, etc. The auxiliary substrate can include fillers, such as mica, talc, silica, calcium carbonate, etc. The auxiliary substrate can include mineral pigments, such as boron nitride or clay, as well as combinations of polysaccharides, fillers, and mineral pigments.

[0030] pH adjustment The color of natural dyes can be adjusted to a desired hue by changing the pH of the natural dye solution or the slurry of the natural dye mixed with the substrate. The pH can be adjusted with acids or bases commonly used in the chemical field to obtain the appropriate hue or increase the solubility of the natural dye. According to one embodiment disclosed herein, citric acid and sodium hydroxide are preferably used. Additionally or alternatively, acids such as ascorbic acid, hydroxy acids, beta-hydroxy acids, volatile acids, or fatty acids, or combinations thereof, can be used. The base used to adjust the pH can include amines such as organic amines, ammonium hydroxide, sodium hydroxide, potassium hydroxide, or combinations thereof. The pH adjuster can be present in an amount of 8% to 15%, 9% to 14%, 12% to 15%, or 10% to 12% by weight.

[0031] Method for Making a Pigment Composition A method of making the pigment composition can include (i) homogenizing a natural dye and a substrate in a solvent to form a slurry, including pH adjustment as needed to achieve a desired hue or solubility of the natural dye; and (ii) spray drying the slurry at an outlet temperature of about 60°C to about 120°C, or 90°C to 120°C, 70°C to 100°C, or 60°C to 90°C.

[0032] The solvent can be water, or a volatile organic solvent, such as ethanol, or a blend thereof. The solvent can be an emulsion base, such as an oil-in-water emulsion base. The choice of solvent depends on the nature of the natural dye. Water is preferably used for water-soluble natural dyes, while volatile organic solvents or emulsion-based pigment compositions can be used for natural oil-soluble dyes.

[0033] The hue and / or solubility of natural dyes can be adjusted by adjusting the pH of the solution. As shown in Figure 1, the molecular structure of natural dyes can change according to the pH, which in turn corresponds to a change in the color and / or solubility of the natural dye. The pH can be adjusted using an acid or base, as previously described. The pH of the natural dye solution can be adjusted before the addition of the substrate. The pH of the substrate and natural dye mixture can be adjusted after the natural dye and substrate are combined with the solvent to form a homogeneous suspension or slurry.

[0034] A solution or slurry of natural dyes combined with a substrate can be spray-dried. An atomizer or spray nozzle disperses the liquid or slurry into a spray of controlled droplet size. A heated drying gas, such as air, oxygen, nitrogen, or other inert gas, can be passed in the same direction as the atomized liquid. Alternatively, the gas can flow countercurrently to the liquid flow, with the hot air flowing against the flow from the atomizer. After spray drying, the moisture content is about 0% to about 10% by weight, 1% to 9%, 2% to 5%, and preferably about 0% to about 5% by weight. This drying procedure effectively reduces the moisture content of the pigment composition. The dried pigment composition can be stabilized against absorption of atmospheric humidity.

[0035] Spray drying of a slurry of the natural dye combined with the substrate results in particles of relatively uniform size. The method can further include an optional step of (iii) particle size reduction to prepare a powdered product. Particle size reduction and homogenization can be achieved by grinding, pulverizing, or micronizing using a grinder or jet mill. The particle size of the pigment composition in powder form can be about 1 μm to about 20 μm, preferably about 2 μm to about 10 μm, as measured by laser diffraction. The particle size can also be 1 μm to 20 μm, 2 μm to 20 μm, 1 μm to 5 μm, 5 μm to 20 μm, 10 μm to 15 μm, or 5 μm to 15 μm.

[0036] Surface treatment agents The method can further include the optional step of (iv) adding a surface treatment agent. The surface treatment agent can additionally be used in a later process according to an embodiment of the present disclosure. For example, synthetic or natural surface treatment agents such as oils, butters, or waxes can be used to make the natural pigment more hydrophobic and / or lipophilic, improving the dispersion of the natural pigment in oil or silicone media. Surface treatment agents can include stearates, such as polyglyceryl-10-pentaisostearate or polyglyceryl-10 nonaisostearate, waxes, such as meadowfoam wax, oils or butters, such as moringa oil or butter, or aloe oil or butter, and combinations thereof.

[0037] The pigment composition obtained in powder form according to the embodiments of the present disclosure can be used in cosmetic applications. The pigment composition can be used in powder form, such as a compact powder. The pigment composition can be used in dispersions, such as lipstick, or in liquids, such as liquid foundation. In these cases, the pigment composition is generally dispersed in an oil, wax, or silicone medium. The pigment composition can be dispersed in an oil, wax, or silicone emulsion, preferably in water in cosmetic formulations. The pigment composition can be dispersed in a liquid (such as oil or silicone) or a solid (such as butter or wax). The pigment composition disclosed herein can increase the luminosity of the cosmetic pigment composition and the luminosity of the body (skin, lips, hair, eyelashes) after application.

[0038] Cosmetic applications in the present invention can include, for example, lipsticks, lip glosses, face makeup products, hair color products, sunscreen products, mascara, and foundations. The cosmetic formulations can be in powder form, single-phase or two-phase lotions, water-in-oil or oil-in-water emulsions, gels, or creams.

[0039] In certain embodiments, the pigment composition can include the natural dye in an amount of about 3% to about 40%, about 5% to about 30%, about 5% to about 35%, or about 10% to about 25% by weight. In certain embodiments, the pigment composition can include the bentonite clay substrate in an amount of about 25% to about 75%, about 50% to about 70%, about 45% to about 50%, about 50% to about 65%, or about 45% to about 60% by weight. In certain embodiments, the pigment composition can include the kaolin clay substrate in an amount of about 45% to about 80%, about 50% to about 75%, about 45% to about 50%, about 50% to about 65%, or about 55% to about 70% by weight. In certain embodiments, the pigment composition can include a co-substrate such as maltodextrin in an amount of about 1% to about 70%, about 5% to about 60%, about 10% to about 30%, about 20% to about 40%, or about 10% to about 45% by weight.

[0040] In certain embodiments, the pigment composition maintains color stability after 30 days of storage at 28° C. and 68% relative humidity, where color stability includes maintaining at least about 50%, at least about 60%, at least about 70%, at least about 80%, or at least about 90% of one or more of the L*, a*, or b* values ​​as measured by reflectance-visible spectroscopy at one or more wavelengths between 400 nm and 800 nm.

[0041] As illustrated in the examples below, pigment compositions containing either Kunipia-F or ImerCare® Opaque and prepared according to the methods disclosed herein demonstrate exceptional color stability over time when stored at 28° C. and 68% relative humidity. Factors contributing to this exceptional performance and stability of compositions having Kunipia-F or ImerCare Opaque materials include purity, composition, and ion exchange capacity (in the case of Kunipia-F), as well as the spray drying method for encapsulating natural dyes.

[0042] others Unless otherwise specified or indicated by context, the terms "a," "an," and "the" mean "one or more." For example, "a molecule" should be interpreted as meaning "one or more molecules."

[0043] As used herein, "about," "generally," "substantially," and "significantly" will be understood by those of ordinary skill in the art and will vary to some extent depending on the context in which they are used. If there are uses of a term that are not clear to those of ordinary skill in the art in a given context, "about" and "generally" mean within plus or minus 10% of the particular term, and "substantially" and "significantly" mean plus or minus more than 10% of the particular term.

[0044] As used herein, the terms "include" and "including" have the same meaning as the terms "comprise" and "comprising." The terms "comprise" and "comprising" should be interpreted as "open-ended" transitional terms that allow for the inclusion of additional elements beyond those elements recited in a claim. The terms "consist" and "consisting of" should be interpreted as "closed" transitional terms that do not allow for the inclusion of additional elements other than those recited in a claim. The term "consisting essentially of" should be interpreted as partially closed, allowing for the inclusion of only additional elements that do not fundamentally alter the nature of the claimed subject matter.

[0045] All methods described herein can be performed in any suitable order unless otherwise indicated herein or clearly contradicted by context. Any and all examples provided herein, or the use of exemplary language (e.g., "etc."), are intended merely to better illustrate the invention and do not pose a limitation on the scope of the invention unless otherwise claimed. No language in the specification should be construed as indicating any non-claimed element as essential to the practice of the invention.

[0046] All references, including publications, patent applications, and patents, cited in this specification are herein incorporated by reference to the same extent as if each reference was individually and specifically indicated to be incorporated by reference and was set forth in its entirety herein. [Example]

[0047] method Physical evaluation Physical evaluation of the example pigment compositions was performed by humans using the senses of touch, sight, and smell, observed by those skilled in the cosmetic arts, and included physical observation of odor, uniformity or coverage, and brilliance after application of the pigment compositions to the skin.

[0048] Humidity Rating Higher moisture absorption over time causes natural pigments to darken and harden over time. Bentonite, montmorillonite, and kaolin pigment composites were further subjected to moisture sorption studies using high humidity conditions of 28°C and 68% relative humidity for 30 days. These conditions were set to mimic the high humidity atmospheres found in Asian countries while also illustrating the moisture absorption properties of the pigment composites.

[0049] Colorimetric evaluation Colorimetric analysis was performed using an X-rite VS450 spectrophotometer equipped with the Color iQC program. The primary objective of this colorimetric study was to identify the pigment composite that yielded the warmest, most radiant shade of red exhibiting the highest L*, a*, and b* values. Figure 2 shows the CIELAB color sphere to illustrate and help select the best pigment composite. The study used commercially available NATPURE XFINE RADISH RR319 (INC1: Raphanus Sativus Extract) as a standard for comparison purposes.

[0050] lipstick formulation The pigment compositions were tested in some examples as lipsticks, and the formulations of the pigment compositions as lipsticks are shown in the table in FIG.

[0051] Examples 1-5 use a natural water-soluble dye anthocyanin from a radish species (Raphanus sativus) called Red Radish (RR). Example 6 uses another source of anthocyanin from a sweet potato species (Ipomoea batatas) called Purple Sweet Potato (PSP). Example 7 uses genipin-hydrolyzed gardenia called Gardenia Blue (GB). Typical compositions include the natural dye (1-70% by weight), substrate (30-99% by weight), optional co-substrate (0-60% by weight), optional pH adjuster, and optional surface treatment agent (1-15% by weight).

[0052] Example 1: Selection of natural substrates Radish seed extract powder as a source of anthocyanins was obtained from Sensient Beauty as "NATPURE XFINE RADISH RR319 (INCl: Raphanus sativus L extract)".

[0053] The composition of the natural pigment is as follows: natural dye: 3 to 40% by weight, natural substrate: 20 to 75% by weight, optional 1 - auxiliary substrate: 0 to 40% by weight, optional 2 - pH adjustment depending on the natural dye with an acid or base such as citric acid or sodium hydroxide, optional 3 - surface treatment agent: 1 to 15% by weight.

[0054] New substrates were selected for their opaque appearance: (1) tricalcium citrate, (2) tricalcium phosphate, (3) kaolin, (4) palm kernel powder, (5) montmorillonite, (6) silica, (7) polyhydroxybutyrate, (8) bentonite, and (9) diatomaceous earth.

[0055] The freshly spray-dried pigment composites were evaluated for the following five factors, the results of which are summarized in Table 2: (A) brilliance in powder form, (B) odor in powder form, (C) moisture content of the powder, (D) uniformity / coverage in lipstick, and (E) brilliance after application to skin.

[0056] The scale is 0 to 10, with a value of 0 corresponding to a natural pigment that is not radiant, has a strong odor, has a high water content, does not provide even coverage during lipstick application, and is not radiant after application to the skin. A value of 10 corresponds to a natural pigment that is very radiant, has no odor, no water content, provides even coverage during lipstick application, and is very radiant after application to the skin.

[0057] The results shown in Table 2 indicate that only kaolin and bentonite provide brilliant natural pigments, have low moisture content, little or no odor, are homogeneous, and provide good coverage upon application. [Table 2]

[0058] Example 2: Red radish extract encapsulated in clay: bentonite vs. montmorillonite Seven different grades of clay, four bentonites (Kunipia-F, Moistnite-S, Moistnite-U ("Moistnite" is a registered trademark), and COSMETICO), and three montmorillonites (gray, beige, and red) are used for comparison in lipstick applications.

[0059] These natural pigments contain approximately 20% to 35% by weight of Xfine Radish RR319, approximately 45% to 60% by weight of bentonite or montmorillonite, approximately 10% to 25% by weight of maltodextrin, and approximately 8% to 15% by weight of citric acid. The citric acid is added to adjust the pH to a range of 2.9 to 3.4, preferably 3.0. Commercially available natural clays were obtained: bentonite clay (Kunipia-F, Moistnite-U, and Moistnite-S) from Kunimine Kogyo Co., Ltd.; bentonite clay (Cosmotico) from SwellWell MineChem Pvt. Ltd.; and montmorillonite clay (ArgileVerte Grey / Beige / Red) from Argiles Du Bassin Mediterraneen ABM.

[0060] Figure 4 presents the L*, a*, b*, C*, and h results for the powdered pigment composite of the composition of Example 2. The spray-dried ingredients were then subjected to lipstick application testing. Images of the lab-scale lipsticks and their corresponding skin applications were recorded and are also tabulated in Figure 4.

[0061] As summarized in Figure 4, the results demonstrate that the Kunipa-F-red radish composite notably exhibited the highest L*, a*, and C* values, indicating the most radiant and reddest of the selected bentonite and montmorillonite. It is also noteworthy that Kunipa-F provided the warmest shade of red and the highest b* value. The analytically analyzed values ​​also correspond to the most radiant physical appearance observed as a lipstick and when applied to the skin.

[0062] Example 3: Red radish extract encapsulated on kaolin Three different grades of kaolin were used for comparison in lipstick applications. Radish seed (Raphanus sativus L) extract powder as a source of anthocyanins was obtained from Sensient Beauty as "Raphanus sativus extract (INCl)."

[0063] The pigment composite contains about 20% to about 35% by weight of red radish extract, about 55% to about 70% by weight of kaolin, and about 8% to about 15% by weight of citric acid. The natural clay kaolin (Caolin G30M) was obtained from Veneta Mineraria SPA, and the kaolin (ImerCare Opaque) was obtained from Imerys SA. The composition in this example is surface-treated with about 1% to about 6% by weight of polyglyceryl-10 pentaisostearate. The surface treatment agent is not limited to polyglyceryl-10 pentaisostearate, but can also be extended to other agents such as meadowfoam wax, polyglyceryl-10 nonaisostearate, moringa oil / moringa butter, and aloe oil or butter.

[0064] For this embodiment with kaolin as the primary substrate, the analyzed colorimetric values ​​were recorded and tabulated in Figure 5. The colorimetric results indicate that the ImerCare Opaque-RedRadish composite may be another effective candidate for improving the luminosity and saturation of pigments. Comparing Figures 4 and 5, the difference between the ImerCare Opaque and Kunipia-F pigmented composites is the b* value, with the pigmented bentonite composition exhibiting the highest b* value, imparting a warmer (yellower) hue, and the pigmented kaolin composition imparting a cooler (bluer) hue.

[0065] Example 4: Moisture absorption evaluation The bentonite, montmorillonite, and kaolin pigment composites were further subjected to a moisture absorption study for 30 days using high humidity conditions at 28°C and 68% relative humidity. These conditions were set to mimic the high humidity atmospheres found in Asian countries while also illustrating the moisture absorption properties of the pigment composites. These pigment composites were compared with the benchmark Xfine RR319, and the results are shown in Figure 6.

[0066] As moisture absorption increases over time, natural pigments become darker and harder over time. Based on the observations shown in Figure 6, the benchmark Xfine RR319 went from a maroon powder state to a black solid state. This observed phenomenon is expected due to the hygroscopic nature of maltodextrin and natural fruit juice extracts. The addition of bentonite, montmorillonite, or kaolin when forming new pigment composites reduces the moisture absorption process. However, the delay in moisture absorption is limited to five days, as hardening and darkening are observed in the pigment composites AV-Beige-RR, AV-Red-RR, and G30M-RR. The hardening and darkening in appearance clearly indicates that moisture absorption has occurred. Observations continue until the eighth day, when Moistnite-S-RR, Moistnite-U-RR, Cosmetico-RR, and AV-Grey-RR again show hardening and darkening in appearance. The moisture sorption study was completed on day 30, and Kunipia-F-RR and ImerCare Opaque-RR (indicated by arrows) showed no hardening or darkening.

[0067] Overall, colorimetric and humidity evaluation of radishes with various auxiliary substrates indicates that the pigment composite containing Kunipia-F exhibited the highest L*, a*, and C* values, indicating brilliance and reddest color. The pigment composite ImerCare Opaque-RR was included for further evaluation due to the best performance shown in the humidity test.

[0068] Example 5: Evaluation of color change in lipstick The commercially available Natpure Xfine RR319 has been reported to exhibit color shifts when formulated into lipstick applications. A blue shift in color on Xfine RR319 was observed 6 hours after application to the skin. Because of the variability in pH on the skin, investigations into the color evolution of new pigment composites were performed using a neutral pH paper substrate instead.

[0069] The pigment composites Kunipia-F-RR and ImerCare Opaque-RR were applied to paper, and the L*, a*, b*, C*, and h values ​​were immediately measured using an X-rite spectrophotometer and then designated as day 1. The final measurements were taken after 6 days and recorded in the table shown in Figure 7, and the corresponding measured colors are shown in Figure 8.

[0070] Natural red radish extract is known to experience a blue shift in color due to the influence of pH-dependent anthocyanins. Based on the results shown in Figures 7 and 8, the Kunipia-F-RR and ImerCare opaque-RR pigment composites in lipsticks were physically more radiant and redder than the Xfine RR319 lipstick. In terms of performance, when applied to neutral pH paper, the freshly applied Kunipia-F-RR pigment composite exhibited the best results, exhibiting the most radiant and reddest (orange tint) physical color on neutral pH paper. As the observations progressed toward day 6, it was noted that the red tint of both Xfine RR319 and ImerCare opaque-RR turned purple at the end of day 1, while the red tint of Kunipia-F-RR remained stable. By the end of day 6, only Kunipia-F-RR maintained its red hue with the highest a* and b* values, while the other two shifted to purple and pink, respectively.

[0071] The Kunipia-F-RR pigment composite exhibited good stability on bentonite with pH-dependent anthocyanins beyond day 1 and maintained its stability well into day 6. This behavior is attributed to the physicochemical properties of bentonite, which has an attractive electrostatic interaction with the anthocyanins in the extract.

[0072] In the completed study of radish species, sodium bentonite (Kunipia-F) from Kunimine Industries Co., Ltd. and kaolin (ImerCare opaque) from Imerys Co., Ltd. were deployed in the remainder of the case studies of various vegetable / fruit extracts.

[0073] Example 6: Another source of anthocyanins from sweet potato species (Ipomoea batatas, purple sweet potato). A second case study of the present invention provides a bluish-red to pink hue using sweet potato seed (Ipomoea batatas) extract powder as a source of anthocyanins. The source of sweet potato seed extract powder was obtained from a commercially available product: Sensient Beauty "Purple Sweet Potato (PSP) Extract."

[0074] In this preferred embodiment, the pigment composite comprises about 5% to about 30% by weight of purple sweet potato extract, about 25% to about 40% by weight of bentonite (Kunipia-F), about 30% to about 45% by weight of maltodextrin, and about 8% to about 15% by weight of citric acid, which is added to function as a pH adjuster in the range of 2.9 to 3.4, preferably 3.0.

[0075] Natpure Xfine Potato SP313 is used as an example for illustrative purposes, but was not included in the colorimetric analysis due to its low color intensity and poor coverage in lipstick applications. Figure 9 records the colorimetric values ​​measured by the spectrophotometer, and Figure 10 shows the physical appearance of the powder and lipstick after application to the skin.

[0076] Based on the investigations conducted in the first case study, the color evolution and evaluation of this new Kunipia-F-PSP vs. raw PSP study are measured on days 1 and 6. Figures 9 and 10 clearly demonstrate and demonstrate that bentonite (Kunipia-F) can stabilize and maintain the anthocyanins in purple sweet potato extract. The electronic data shown in Figure 9 demonstrate that a slight blue shift occurs in the Kunipia-F-PSP pigment composite, but its optical brightness and red color changes are minimal. Raw PSP is chosen as a benchmark to highlight the stabilizing effect of bentonite on anthocyanins.

[0077] The investigation of sweet potato seeds (Ipomoea batatas L.) further supported the conclusions stated in the first case study using radish seed extract. This study demonstrated that the application of bentonite (as Kunipia-F) can be extended to other natural extracts containing anthocyanins, regardless of which type of anthocyanin predominates in the extract.

[0078] Example 7: Non-anthocyanin source as a natural dye - Genipin hydrolyzed gardenia [Gardenia Blue] This case study of the present disclosure provides a blue hue derived from a non-anthocyanin extract, such as gardenia extract. The source of gardenia extract powder was obtained from a commercially available product: Sensient Beauty's "Natpure Xfine Gardenia GB618."

[0079] In this preferred embodiment, the pigment composite comprises about 1% to about 15% by weight of Xfine Gardenia GB618 powder, about 25% to about 40% by weight of bentonite (Kunipia-F), and about 60% to about 75% by weight of maltodextrin.

[0080] In another preferred embodiment, the pigment composite comprises about 1% to about 15% by weight of Xfine Gardenia GB618 powder, about 40% to about 55% by weight of kaolin (ImerCare Opaque), and about 40% to about 55% by weight of maltodextrin.

[0081] Based on the physical observations shown in Figure 11, investigation of this non-anthocyanin case study clearly demonstrates that bentonite (Kunipia-F) imparts warmer shades (yellowish hues) of the pigment composite, while kaolin (ImerCare Opaque) produces cooler shades (bluish hues). This study demonstrates that bentonite (Kunipia-F) can generally provide more radiant shades (yellowish hues) with natural extracts containing anthocyanins, but can also be extended to other natural extracts containing genipin-amino acid complex pigments (Gardenia Blue or Jagua Blue). The same behavior was observed with kaolin (ImerCare Opaque) as a co-substrate, providing more radiant shades (bluish hues) with an underlying high photoluminescence reflectance index, regardless of whether the natural extract contained anthocyanin or amino acid complex extracts.

[0082] Preferred embodiments of this invention are described herein, including the best mode known to the inventors for carrying out the invention. Variations of those preferred embodiments may become apparent to those skilled in the art upon reading the foregoing description. The inventors expect that skilled artisans will employ such variations as they see fit, and the inventors intend the invention to be practiced otherwise than as specifically described herein. Accordingly, this invention includes all modifications and equivalents of the subject matter recited in the claims appended hereto as permitted by applicable law. Furthermore, any combination of the above-described elements in all possible variations thereof is encompassed by the invention unless otherwise indicated herein or otherwise clearly contradicted by context.

Claims

1. 1. A composition comprising: a natural dye in an amount of 5% to 35% by weight, optionally 5% to 30% by weight, or optionally 10% to 25% by weight; a bentonite clay substrate in an amount of 45% to 60% by weight, optionally 50% to 60% by weight, or optionally 45% to 55% by weight; maltodextrin in an amount of 10% to 45% by weight, optionally 20% to 40% by weight, or optionally 10% to 30% by weight; and an optional pH adjuster; the natural dye is at least partially integrated into the cationic interlayer of the bentonite clay matrix by a spray drying process; the composition maintains color stability after storage for 30 days at 28°C and 68% relative humidity; the color stability comprises maintaining at least 50%, at least 60%, at least 70%, at least 80%, or at least 90% of one or more of the L*, a*, or b* values ​​as measured by reflectance visible spectroscopy at one or more wavelengths from 400 nm to 800 nm; greater than 50%, greater than 60%, greater than 70%, greater than 80%, or greater than 90% of the cations in the cationic interlayer are sodium cations; prior to at least partially incorporating the natural dye into the cationic interlayer, the bentonite clay matrix has a whiteness of at least 50%, optionally at least 60%, or optionally at least 70%; The composition, wherein, prior to at least partially incorporating the natural dye into the cationic interlayer, the bentonite clay matrix has an initial cation exchange capacity of at least 75 meq / 100g, optionally at least 80 meq / 100g, or optionally at least 85 meq / 100g.

2. 1. A composition comprising: a natural dye in an amount of 20% to 35%, 20% to 30%, or 25% to 35% by weight; a kaolin clay substrate in an amount of 55% to 70%, 60% to 70%, or 55% to 65% by weight; an optional pH adjuster; and and an optional surface treatment agent; the composition maintains color stability after storage for 30 days at 28°C and 68% relative humidity; the color stability comprises maintaining at least 50%, at least 60%, at least 70%, at least 80%, or at least 90% of one or more of the L*, a*, or b* values ​​as measured by reflectance visible spectroscopy at one or more wavelengths from 400 nm to 800 nm; The composition, wherein the kaolin clay substrate, prior to contact with the natural dye, has a reflectance optical brightness of at least 85%, optionally at least 90%, or optionally at least 95%, as measured by visible reflectance spectroscopy.

3. 3. The composition of claim 2, wherein the composition comprises the surface treatment agent, and the surface treatment agent is selected from the group consisting of stearates, optionally polyglyceryl-10-pentaisostearate or polyglyceryl-10 nonaisostearate, waxes, optionally meadowfoam wax, oils or butters, optionally moringa oil or butter, optionally aloe oil or butter, silicones, and combinations thereof.

4. 4. The composition of claim 1, wherein the color of the natural dye changes with pH, ​​and the composition comprises a pH adjuster.

5. The composition of claim 4 , wherein the pH adjuster is citric acid.

6. 6. The composition of claim 4 or 5, wherein the pH adjuster is present in the composition in an amount of from 8% to 15% by weight, optionally from 9% to 14% by weight, optionally from 12% to 15% by weight, or optionally from 10% to 12% by weight.

7. 7. The composition of claim 1, further comprising a co-substrate, said co-substrate comprising a polysaccharide.

8. 8. A filled composition comprising the composition of any one of claims 1 to 7, further comprising at least one filler, said filler comprising mica, talc, silica, or calcium carbonate.

9. 9. The composition of claim 1, further comprising at least one mineral pigment, wherein the mineral pigment comprises boron nitride or clay.

10. 10. The composition of claim 1, wherein the natural dye is an anthocyanin, a genipin-amino acid complex, or a combination thereof.

11. 1. A method for preparing a powder composition, comprising: a) homogenizing a natural dye with a solvent to form a slurry with either i) a bentonite clay having a whiteness of at least 50%, optionally at least 60%, or optionally at least 70%, and a cation exchange capacity (CEC) of at least 75 meq / 100g, optionally at least 80 meq / 100g, or optionally at least 85 meq / 100g, or ii) a kaolin clay having a reflectance optical brightness of at least 85%, optionally at least 90%, optionally at least 95%; b) optionally adjusting the pH of the slurry by adding a pH adjuster; c) spray drying the slurry at an outlet temperature of from 60°C to 120°C, optionally from 90°C to 120°C, optionally from 70°C to 100°C, or optionally from 60°C to 90°C to form a powder.

12. 12. The method of claim 11, further comprising the step of: d) performing a particle size reduction process to reduce the particle size of said powder composition to between 1 μm and 20 μm, optionally between 1 μm and 5 μm, optionally between 5 μm and 20 μm, optionally between 10 μm and 15 μm, or optionally between 5 μm and 15 μm, wherein said particle size reduction process comprises milling, grinding, micronization, or a combination thereof.

13. 13. The method of claim 1, wherein the solvent is water, a volatile organic solvent, or an emulsion base.

14. 14. The method of any one of claims 1 to 13, wherein the particle size of the powder composition is from 2 μm to 10 μm, optionally from 2 μm to 5 μm, optionally from 5 μm to 10 μm, or optionally from 8 μm to 10 μm.

15. 15. The method of any one of claims 1 to 14, wherein the moisture content is from 0% to 10% by weight, from 1% to 9%, from 2% to 5%, or from 0% to 5% by weight.

16. 16. The method of any one of claims 1 to 15, further comprising the step (v) of combining particles of the powder composition with an additive, wherein the additive comprises an oil, butter, or wax.

17. 17. The method of any one of claims 1 to 16, wherein the additive comprises polyglyceryl-10 pentaisostearate, meadowfoam wax, polyglyceryl-10 nonaisostearate, moringa oil, moringa butter, aloe oil, aloe butter, and combinations thereof.

18. 18. The method of any one of claims 1 to 17, wherein the pH adjuster is an acid, and the acid comprises citric acid, ascorbic acid, an alpha-hydroxy acid, a beta-hydroxy acid, a volatile acid, or a fatty acid, or a combination thereof.

19. 19. The method of any one of claims 1 to 18, wherein the pH adjuster is a base, and the base comprises an amine, an organic amine, ammonium hydroxide, sodium hydroxide, potassium hydroxide, or a combination thereof.

20. 20. The method of any one of claims 1 to 19, wherein the powder composition is used in a cosmetic application, the cosmetic application being in the form of a powder, a lotion, an emulsion, a gel, and / or a cream.

21. 1. A natural pigment composition comprising: a natural dye in an amount of 3% to 40% by weight; a clay substrate in an amount of 20% to 75% by weight; an optional co-substrate in an amount of 0% to 45% by weight; an optional pH adjuster; and an optional surface treatment agent in an amount of 1% to 15% by weight; 1. A natural pigment composition, wherein the natural pigment composition is in powder form.

22. 22. The natural pigment composition of claim 21, wherein the clay substrate is at least one of a bentonite clay substrate, a montmorillonite, or a kaolin clay substrate.

23. 23. The natural pigment composition of claim 21 or 22, wherein the natural dye is a plant extract, a fruit extract, a vegetable extract, or an anthocyanin.

24. 24. The natural pigment composition of claim 23, wherein the anthocyanin is at least one of pelagonidin, peonidin, cyanidin, malvidin, delphinidin, and petunidin, which can be harvested from red radish (Raphanus sativus), red sweet potato (Ipomoea batatas), wild carrot (Daucus carota), red cabbage (Brassica oleracea), grape (Vitis vinifera), elderberry (Sambucus nigra), or strawberry (Fragaroa ananassa).

25. 25. The natural pigment composition according to any one of claims 21 to 24, wherein the natural dye is water-soluble or oil-soluble.

26. 26. The natural pigment composition of claim 25, wherein the natural dye is oil-soluble and is at least one of beta-carotene extracted from algae or fungal extracts, paprika oleoresin extracted from chili peppers, bixin extracted from annatto seeds, or azulene extracted from chamomile flowers.

27. 27. The natural pigment composition of any one of claims 21 to 26, wherein the clay substrate comprises exchangeable interlayer cations comprising at least one of sodium cations, calcium cations, alkali metal ions, alkaline earth metal ions, or transition metal ions.

28. 28. The natural pigment composition according to any one of claims 21 to 27, wherein the clay substrate has a cation exchange capacity (CEC) of at least 75 meq / 100g, optionally at least 80 meq / 100g, or optionally at least 85 meq / 100g.

29. 29. The natural pigment composition of any one of claims 21 to 28, wherein the natural pigment composition comprises a brightness of at least 50%, optionally at least 60%, or optionally at least 70%.

30. 30. The natural pigment composition of any one of claims 21 to 29, wherein the natural pigment composition comprises a luminance reflectance of at least 85%, optionally at least 90%, or optionally at least 95%, as measured by visible reflectance spectroscopy.

31. 31. The natural pigment composition of any one of claims 21 to 30, further comprising a co-substrate, wherein the co-substrate comprises at least one of a polysaccharide, maltodextrin, chitosan, gum arabic, cellulose, pullulan, a filler, mica, talc, silica, calcium carbonate, a mineral pigment, boron nitride, or a clay.

32. 32. The natural pigment composition of any one of claims 21 to 31, further comprising a pH adjuster, wherein the pH adjuster comprises at least one of citric acid, sodium hydroxide, ascorbic acid, an alpha-hydroxy acid, a beta-hydroxy acid, a volatile acid, a fatty acid, an amine, an organic amine, ammonium hydroxide, sodium hydroxide, or potassium hydroxide.

33. A natural pigment composition according to any one of claims 21 to 32, wherein the natural dye is at least partially integrated into the cationic interlayers of the clay matrix by a spray drying process.

34. 34. The natural pigment composition of claim 33, wherein greater than 50%, greater than 60%, greater than 70%, greater than 80%, or greater than 90% of the cations in the cationic interlayer are sodium cations.

35. 35. The natural pigment composition of any one of claims 21 to 34, wherein the natural pigment composition maintains color stability after storage at 28°C and 68% relative humidity for 30 days.

36. 36. The natural pigment composition of claim 35, wherein the color stability comprises maintaining at least 50%, at least 60%, at least 70%, at least 80%, or at least 90% of one or more of the L*, a*, or b* values ​​as measured by reflectance visible spectroscopy at one or more wavelengths from 400 nm to 800 nm.

37. 37. The natural pigment composition of any one of claims 21 to 36, wherein the clay substrate has an initial cation exchange capacity of at least 75 meq / 100g, optionally at least 80 meq / 100g, or optionally at least 85 meq / 100g, prior to the natural dye being at least partially integrated into the cationic interlayer of the clay substrate.

38. 38. The natural pigment composition of any one of claims 21 to 37, wherein the clay substrate has a reflectance optical brightness of at least 85%, optionally at least 90%, optionally at least 95%, measured by visible reflectance spectroscopy, prior to contact with the natural dye.

39. 39. The natural pigment composition of any one of claims 21 to 38, wherein the surface treatment agent is selected from the group consisting of a stearate, such as polyglyceryl-10-pentaisostearate or polyglyceryl-10 nonaisostearate, a wax, such as meadowfoam wax, an oil or butter, such as moringa oil or butter, or aloe oil or butter, a silicone, and combinations thereof.

40. 40. The natural pigment composition of any one of claims 21 to 39, wherein the color of the natural dye changes with pH, ​​and the composition comprises the pH adjuster.

41. 41. The natural pigment composition of claim 40, wherein the pH adjuster is present in the composition in an amount from 8% to 15% by weight, optionally from 9% to 14% by weight, optionally from 12% to 15% by weight, or optionally from 10% to 12% by weight.

42. 42. The natural pigment composition of any one of claims 21 to 41, wherein the particle size of the natural pigment composition is from 2 μm to 10 μm, optionally from 2 μm to 5 μm, optionally from 5 μm to 10 μm, or optionally from 8 μm to 10 μm.

43. 43. The natural pigment composition of any one of claims 21 to 42, wherein the water content of the natural pigment composition is from 0% to 10% by weight, optionally from 1% to 9%, optionally from 2% to 5%, or optionally from 0% to 5% by weight.

44. The natural pigment composition according to any one of claims 21 to 43, wherein the natural pigment composition is used in cosmetic applications.