A highly effective and deodorizing snake oil Pickering emulsion and its preparation process and application

Abstract

The present invention relates to the technical field of snake oil deodorization and emulsion preparation, and more particularly to a highly effective deodorizing snake oil Pickering emulsion, its preparation process, and its application. The present invention utilizes β-molecular sieves to deodorize snake oil, and utilizes octenyl succinate starch ester (OSAS) / sodium caseinate (SC) complex particles to construct a stable snake oil-loaded Pickering single emulsion. The Pickering emulsion exhibits excellent performance in terms of pH, ionic strength, thermal stability, and centrifugal stability, providing a new carrier for the delivery of fat-soluble functional ingredients. The snake oil deodorization technology is highly practical and has broad application prospects. The implementation of the project is expected to increase the diversified application of snake oil in the fields of food, medicine, and cosmetics.

Description

Technical Field

[0001] The invention relates to the technical field of deodorizing snake oil and preparing emulsions, in particular to a highly efficient deodorizing snake oil Pickering emulsion and a preparation process and application thereof. Background Art

[0002] Snake oil's primary components are fatty acids, with a high content of unsaturated fatty acids. In particular, eicosatetraenoic acid (EA), which is significantly higher than in warm-blooded animals and higher than the 7%-9% found in fish and amphibians, is highly compatible and complementary to the physiological growth characteristics of human skin. It has strong affinity and permeability for the skin and mucous membranes, making it easily absorbed by the skin, making it suitable for use in cosmetics for beauty and skincare. However, snake oil's high oxidability, poor storage, high viscosity, and strong fishy odor limit its application. Furthermore, commercially available snake oil creams contain low levels of EA and often use fragrances to mask the odor, further weakening its effectiveness and increasing its cost.

[0003] Pickering emulsions, also known as Pickering emulsions, are a novel emulsification system that uses solid particles instead of surfactants or amphiphilic polymers to stabilize the oil-water interface. Their stabilization mechanism is that the solid particles form a stable interfacial film on the surface of the dispersed phase droplets. This steric hindrance at the oil-water interface effectively prevents coalescence of the droplets. Compared to emulsions formed using traditional surfactants as stabilizers, Pickering emulsions require lower emulsifier dosages, have high biocompatibility, and are essentially non-irritating and non-toxic. Furthermore, the interfacial stabilization effect of Pickering emulsions effectively inhibits lipid oxidation, reducing the contact of unsaturated lipids with pro-oxidants and free radicals in the aqueous phase, thereby weakening the oxidation reaction. Pickering emulsions offer numerous advantages, such as encapsulating and transporting flavors and active ingredients, slowing their degradation. Encapsulating flavors in Pickering emulsions can effectively mask unpleasant odors and improve the sensory properties of food, offering significant potential for application in the cosmetics, food, and pharmaceutical industries.

[0004] Starch is one of the most commonly used polysaccharides for stabilizing Pickering emulsions. It is biocompatible and biodegradable, inexpensive, edible, non-irritating, and nontoxic. Among a range of starch derivatives, octenyl succinate starch (OSAS) has gained increasing attention due to its strong emulsifying ability. OSAS is the product of the esterification reaction between hydroxyl groups in starch molecules and octenyl succinic anhydride (OSA). The introduced hydrophobic octenyl groups and hydrophilic carboxyl groups impart amphiphilic properties to OSAS. The multi-branched polymer structure and high molar mass of OSAS also facilitate its adsorption at the oil-water interface, forming a steric barrier. However, because the esterification reaction primarily occurs on the particle surface, the internal hydrophobic chains are less likely to reach the oil phase during stabilization, reducing OSAS's emulsification efficiency. The strong rigidity and large size of OSAS also limit its sustained adsorption at the interface, hindering the long-term stability of the emulsion.

[0005] Therefore, if what Efficiently removing the fishy smell of snake oil and constructing a stable Pickering emulsion are still technical problems that need to be solved urgently in this field. Summary of the Invention

[0006] The technical problem to be solved by the present invention is how to develop an efficient process for removing the odor of snake oil and construct a stable snake oil system based on a Pickering emulsion. This approach aims to overcome the bottleneck in the application of snake oil in the medical and healthcare fields and expand its diverse application scenarios in food, medicine, and cosmetics. Therefore, the present invention provides a Pickering emulsion for efficiently removing the odor of snake oil, as well as its preparation process and application.

[0007] The present invention solves the above technical problems through the following technical solutions:

[0008] The invention provides a preparation process of a highly effective fishy-free snake oil Pickering emulsion. The process comprises the following steps: using a β-molecular sieve to remove the fishy smell of the snake oil; and utilizing octenyl succinate starch ester (OSAS) / sodium caseinate (SC) complex particles to construct a stable snake oil-loaded Pickering single emulsion.

[0009] The present invention utilizes β-molecular sieves to remove the odor of snake oil, thereby achieving efficient odor removal of snake oil. A stable Pickering single emulsion loaded with snake oil is constructed through OSAS / SC composite particles. By embedding the snake oil in the Pickering emulsion, lipid oxidation can be effectively reduced.

[0010] As one of the preferred embodiments of the present invention, the snake oil is selected from any one of the snake oils of Bungarus nigripes, Agkistrodon rubripes, Agkistrodon acutus, Cobra, and Elaphe, more preferably Bungarus nigripes oil.

[0011] As one of the preferred embodiments of the present invention, in the step of removing the fishy smell of snake oil using β-molecular sieve, the mass ratio of snake oil to β-molecular sieve is 15:1-5:1, more preferably 10:1.

[0012] As one of the preferred embodiments of the present invention, in the step of removing the fishy smell of snake oil using β-molecular sieve, the snake oil and β-molecular sieve are stirred and reacted at 30-50° C. for 0.5-5 h; more preferably, the reaction is stirred and reacted at 35° C. for 1 h.

[0013] As one of the preferred embodiments of the present invention, the optimal performance indicators of the deodorized snake oil are as follows: acid value 0.84±0.067 mg / g, peroxide value 0.080±0.004 g / 100g, conjugated diene value 2.613±0.006 gL / 100g, and conjugated triene value 0.8843±0.001 gL / 100g. The sample deodorized with β-molecular sieve has a volatile alcohol content of 0.21 mg / kg, a content of other substances of 0.36 mg / kg, a content of ketones, acids, and esters of no more than 0.05 mg / kg, and a hydrocarbon content similar to that of the original snake oil, reaching 1.11 mg / kg.

[0014] As one of the preferred embodiments of the present invention, the OSAS / SC complex particles are prepared by mixing equal volumes of an OSAS solution and a SC solution at a constant speed to obtain a complex solution, and then centrifuging and freeze-drying the complex solution to obtain the OSAS / SC complex particles.

[0015] More preferably, in the composite solution, the composite ratio of OSAS to SC is 1:1-15:1, more preferably 1:1;

[0016] and / or, in the composite solution, the concentration of OSAS is 6% (w / v);

[0017] and / or, the degree of substitution of OSA starch is 0.024, 0.03, 0.037, more preferably 0.037;

[0018] And / or, the pH of the composite solution is 4-5.

[0019] More preferably, during the preparation of the OSAS / SC composite particles, the constant mixing speed is 20-40 rpm;

[0020] and / or, centrifugation conditions were 3,000 g, 5 min;

[0021] And / or, the freeze-drying conditions are -40°C, 0.9 Pa.

[0022] As one of the preferred embodiments of the present invention, the particle size of the OSAS / SC composite particles is 107.07±3.10 nm, the PDI is 0.52±0.03, and the potential is -10.17±1.80 mV.

[0023] As one of the preferred embodiments of the present invention, an aqueous solution of OSAS / SC composite particles is used as the aqueous phase, and deodorized snake oil is used as the oil phase. After the aqueous phase and the oil phase are mixed, a primary emulsion is prepared by shear stirring at a certain temperature, and then a snake oil Pickering emulsion is obtained by ultrasonication.

[0024] More preferably, the concentration of the OSAS / SC composite particles in the aqueous phase is 2.0 wt%-10.0 wt%, more preferably 8.0 wt%;

[0025] and / or, the pH of the aqueous phase is 4-5, more preferably 4;

[0026] and / or, the volume fraction of the oil phase is 50.0-85.0%, more preferably 75%;

[0027] and / or, a temperature of 10-25°C;

[0028] and / or, the shear stirring condition parameter is 12000 r / min-15000 r / min;

[0029] And / or, the ultrasonic power is 200-300 W, more preferably 250 W; the ultrasonic conditions are ultrasonication for 6 seconds and rest for 3 seconds, for a total of 5 minutes.

[0030] As one of the preferred embodiments of the present invention, the snake oil Pickering emulsion has the following optimal performance indicators: emulsion particle size of 22.18 ± 2.47 μm, Zeta potential of 10.40 ± 0.61 mV, centrifugal water retention of ≥ 60%, and tolerance to pH (2-8), ionic strength (0-200 mmoL / L NaCl) and high temperature (90°C) environments.

[0031] The present invention also provides a highly effective and fishy-free snake oil Pickering emulsion prepared by any of the above preparation methods.

[0032] The present invention also provides an application of the highly effective and fishy-free snake oil Pickering emulsion prepared by any of the above preparation methods in the fields of cosmetics, food, medicine and health care products.

[0033] In this invention, sodium caseinate (SC) is a salt of casein. Casein is a safe and harmless thickener and emulsion stabilizer with good viscosity and protein-specific foaming and gas retention properties. However, in practical applications, sodium caseinate typically requires the use of multiple traditional emulsifiers to maintain emulsion stability. This invention successfully improves the stability of snake oil emulsions by combining SC with OSAS and then adding them to deodorized snake oil to prepare a Pickering emulsion.

[0034] This invention offers the following advantages over existing snake oil deodorization technologies: Using OSA starch / sodium caseinate composite particles as a stabilizer, it successfully constructs a stable snake oil-loaded Pickering emulsion. By optimizing the oil phase volume fraction and particle concentration, an emulsion with a small particle size and uniform microstructure is obtained. This emulsion exhibits excellent properties in terms of pH, ionic strength, thermal stability, and centrifugal stability, and has broad application prospects. It provides a new vehicle for delivering the fat-soluble functional components of snake oil Pickering emulsions, while also expanding the diverse application scenarios of snake oil in the food, pharmaceutical, and cosmetic sectors. BRIEF DESCRIPTION OF THE DRAWINGS

[0035] Figure 1 These are the XPS characterization results of the β-molecular sieve before and after deodorization in Example 1.

[0036] Figure 2 1 is the XRD spectrum of the β-molecular sieve before and after deodorization in Example 1.

[0037] Figure 3 This is the FT-IR graph of the β-molecular sieve before and after deodorization in Example 1.

[0038] Figure 4 Schematic diagram of the wettability of OSAS / SC composite solutions at different composite ratios / pH values / substitution degrees in Example 2.

[0039] Figure 5 The stabilization ability of different composite particles as emulsifiers for Pickering emulsions with snake oil as the oil phase in Example 3 is used as an indicator, and the particle size potential diagrams of the emulsions obtained under the preparation conditions of 30% and 75% oil phase volume are selected respectively.

[0040] Figure 6 The stabilization ability of different composite particles as emulsifiers for Pickering emulsions with snake oil as the oil phase in Example 3 is used as an indicator, and the appearance of the emulsions obtained under the preparation conditions of 30% and 75% oil phase volume are selected respectively.

[0041] Figure 7Schematic diagram showing the selection of the OSAS DS=0.037, compounding ratio 1:1, and pH value 4 as the preparation conditions for the composite in Example 4, and the characterization of the composite prepared under these conditions.

[0042] Figure 8 Schematic diagram of the appearance of Pickering emulsions stabilized by OSAS / SC complexes at different oil phase volume fractions at different storage times in Example 5.

[0043] Figure 9 3 is a particle size potential diagram of the Pickering emulsion stabilized by the OSAS / SC complex at different oil phase volumes in Example 5.

[0044] Figure 10 Graph showing the rheological properties of the Pickering emulsion stabilized by the OSAS / SC composite at different oil phase volume fractions in Example 5.

[0045] Figure 11 Schematic diagram of the appearance of Pickering emulsions stabilized by OSAS / SC complexes at different particle concentrations at different storage times in Example 6.

[0046] Figure 12 Graph showing the rheological properties of the Pickering emulsion stabilized by the OSAS / SC complex at different particle concentrations in Example 6.

[0047] Figure 13 Schematic diagram of the optical microscope showing the dispersion behavior of the Pickering emulsion stabilized by the OSAS / SC complex in Example 7 in different dissociation agents.

[0048] Figure 14 3 is a graph showing the particle size and zeta potential of the Pickering emulsion stabilized by the OSAS / SC complex at different pH values ​​and ionic strengths in Example 8.

[0049] Figure 15 Schematic diagram of the appearance of the Pickering emulsion stabilized by the OSAS / SC complex at different pH values / ion concentrations in Example 8.

[0050] Figure 16 Schematic diagram of the particle size and Zeta potential of the Pickering emulsion stabilized by the OSAS / SC complex at different temperatures in Example 9.

[0051] Figure 17 1 is an appearance diagram of the Pickering emulsion stabilized by the OSAS / SC complex at different temperatures in Example 9.

[0052] Figure 18 Schematic diagram of the centrifugation stability of the Pickering emulsion stabilized by the OSAS / SC complex at different particle concentrations in Example 10.

[0053] Figure 19 This is a graph showing the in vitro antioxidant properties of the Pickering emulsion in Example 11. DETAILED DESCRIPTION

[0054] In order to better clarify and understand the purpose, process scheme and advantages of the present invention, the technical scheme and implementation method of the present invention are further clearly, completely and in detail described below through specific examples and in conjunction with the accompanying drawings. It should be noted that the embodiments described in the present invention are implemented under the premise of the technical scheme of the present invention, and detailed implementation methods and specific operating processes are given, but they are only part of the embodiments of the present invention, not all of the embodiments. The specific implementation methods described are limited to illustrating and explaining the present invention and do not limit the present invention. Based on the embodiments in the present invention, all other implementation methods obtained by ordinary technicians in this field without making creative work are within the scope of protection of the present invention. Unless otherwise specified, the experimental methods and conditions used in the embodiments of the present invention are all conventional methods and conventional conditions. The materials, reagents or instruments and equipment used in the embodiments, unless otherwise specified, are all conventional substances or equipment known to those skilled in the art and can be obtained from commercial channels or prepared by conventional methods. The reaction conditions embodied in the summary of the invention of the present invention can all achieve the described reaction and obtain the product with the expected effect. Due to space limitations, some examples are listed below to further illustrate the advantages of the technical scheme of the present invention.

[0055] Example 1

[0056] This embodiment uses β-molecular sieve to remove the fishy smell of Bungarus serpentissima oil purchased and boiled from a snake farm.

[0057] Snake oil:β-molecular sieve = 10:1 (w / w), react at 35°C with stirring for 1 h, stop the reaction, and centrifuge.

[0058] Physical and Chemical Index Testing: Relative density was determined according to the Pharmacopoeia of the People's Republic of China (2020 edition), Part IV, General Rules, 0601, Determination of Relative Density; acid value and saponification value were determined according to the Pharmacopoeia of the People's Republic of China (2020 edition), Part IV, General Rules, 0713, Determination of Fats and Fatty Oils. Conjugated Diene Value (CD) and Conjugated Triene Value (CT) Determination: Accurately weigh 0.25 g of oil sample into a 25 mL volumetric flask, dilute and dissolve with isooctane, and calibrate to volume. Using isooctane as a blank, measure the absorbance A at 232 nm and 270 nm. Calculate using the following formula:

[0059]

[0060] Where: A is the absorbance of the sample at 232 nm and 270 nm; m is the mass of the sample / g; l is the optical diameter of the cuvette / cm.

[0061] Fatty acid composition analysis: Weigh 0.2 g of a homogenized sample (accurate to 0.1 mg, approximately 100-200 mg fat) into a 50 mL flat-bottom flask. Add 8 mL of 0.5 mol / L sodium hydroxide in methanol. Connect a reflux condenser and reflux in an 80°C ± 1°C water bath until the oil droplets disappear. Add 10 mL of 14% boron trifluoride in methanol from the top of the condenser. Continue reflux in an 80°C ± 1°C water bath for 2 minutes. Cool, then accurately add 8 mL of n-hexane. Continue reflux for 1 minute. Add 20 mL of saturated sodium chloride solution and allow to stand for separation. Pipette 5 mL of the upper n-hexane extract into a 25 mL test tube. Add 3-5 g of anhydrous sodium sulfate. Shake for 1 minute and allow to stand for 5 minutes. A 1 μL aliquot of the upper layer of the test solution was injected into a gas chromatograph. GC-MS conditions were as follows: GC column: HP-FFAP (30 m × 0.25 mm × 0.25 μm); temperature program: start at 70°C, hold for 2 min, then increase to 240°C at a rate of 4°C / min, hold for 24 min; injection port: 220°C; carrier gas: helium; gas flow rate: 1.0 mL / min. MS conditions: electron impact ionization (EI); ion source temperature: 250°C, interface temperature: 240°C; solvent delay: 4 min; full scan mode; mass spectrometry scan range: m / z 33-450. Chromatographic peaks were recorded, and the content of each fatty acid methyl ester was calculated by peak area normalization.

[0062] Volatile component analysis: 1 mL of 0.5 μg / mL 2-octanol was added to 4.5 g of sample as an internal standard and equilibrated at 80°C for 10 minutes. Extraction and adsorption were performed using a 65 μm DVB / PDMS solid phase microextraction head for 20 minutes and desorption for 2 minutes. Gas chromatography-mass spectrometry (GC-MS) conditions: GC column: DB-5MS (30 m×0.25 mm×0.25 μm), injection volume: 1 mL, split ratio: 20:1, injection port temperature: 250°C, temperature program: starting temperature: 35°C for 3 minutes, heating to 100°C at 10°C / min, holding for 0.5 minutes, heating to 250°C at 5°C / min, holding for 2 minutes. MS conditions: ion source: EI, electron energy: 70 eV, ion source temperature: 200°C; full scan mode; mass scan range: 30-650 m / z; Qualitative analysis method: First, remove silicon-containing substances that have been lost from the column, then select those with a match greater than 75 (maximum 100), refer to the NIST 2020 spectral library, and perform qualitative analysis in combination with the mass spectrum.

[0063] FT-IR: Characteristic groups of OSA starch, SC, and composite samples were determined by Fourier transform infrared spectroscopy (FT-IR). The dried samples were mixed with KBr at a ratio of 1:100 (w / w) in an agate mortar, ground, and pressed into pellets. A KBr blank was used as a control. The wavelength of the test was 4000-500 cm -1 , resolution 4 cm -1 , scan times 32 times.

[0064] XRD: The crystalline structure of the composite was determined by X-ray diffractometer (XRD). The crystal structure of the composite particles was determined by X-ray diffractometer with a scanning speed of 2° / min, a diffraction angle range set to 5°–40°, and a step size (Δ2θ) set to 0.02°.

[0065] XPS: XPS data were obtained using a focused monochromatic Al-K source as the incident radiation (hv = 1486 eV). The C1s binding energy (284.5 eV) was used as the standard energy, and the XPS data were fitted and analyzed using XPS Peak 4.1 software.

[0066] Table 1 shows the physical and chemical properties of snake oil before and after deodorization using β-molecular sieves. As can be seen, the acid value of the snake oil changed significantly after deodorization, indicating a significant reduction in free fatty acids. The peroxide value, conjugated diene value, and conjugated triene value of the deodorized snake oil also increased slightly, but the increase was small and had little impact on the quality of the snake oil.

[0067] Table 1 Physical and chemical indexes of snake oil before and after deodorization using β-molecular sieve

[0068]

[0069] Table 2 is the analysis table of fatty acid composition of snake oil before and after deodorization by β-molecular sieve. As can be seen from the table, the difference in fatty acid composition content after deodorization by β-molecular sieve is small.

[0070] Table 2 Analysis of fatty acid composition of snake oil before and after deodorization using β-molecular sieve

[0071]

[0072] Table 3 is a quantitative analysis of the volatile components of snake oil before and after deodorization with β-molecular sieve. It can be seen that the overall volatile content of the sample after β-molecular sieve treatment is significantly reduced, especially the content of aldehydes. The total relative internal standard mass fraction of volatile components detected in the untreated original snake oil sample is 22.70 mg / kg, of which the content of aldehydes can reach 8.10 mg / kg. The content of aldehydes in the sample treated with β-molecular sieve is significantly reduced to 0.45 mg / kg, the content of alcohols is 0.21 mg / kg, and the content of other substances is 0.36 mg / kg. The contents of ketones, acids, and esters are all less than 0.05 mg / kg.

[0073] Table 3 Quantitative analysis of volatile components of snake oil before and after deodorization using β-molecular sieve

[0074]

[0075] Figure 1 These are the XPS characterization results of the β-molecular sieve before and after deodorization in Example 1. Figure 1 The AC part in the middle is the XPS spectrum of β-molecular sieve before deodorization. Figure 1 The DF part in the middle is the XPS spectrum sample of the β-zeolite before deodorization. Comprehensive comparison shows that the surface may have adsorbed compounds containing functional groups such as amines, ketones, aldehydes and esters. Figure 2 1 is the XRD spectrum of the β-molecular sieve before and after the fishy smell removal in Example 1. The crystal structure of the β-molecular sieve remains intact and is not damaged before and after the fishy smell removal. Figure 3 This is the FT-IR graph of the β-molecular sieve before and after deodorization in Example 1. The infrared characteristic peaks of the samples before and after deodorization are similar, indicating that the crystal structure of the β-molecular sieve remains intact and is not damaged before and after deodorization. By characterizing the β-molecular sieve before and after deodorization using XRD, FT-IR, XPS and other means, it was found that the crystal structure of the β-molecular sieve remains intact and is not damaged before and after deodorization. The snake oil after deodorization by β-molecular sieve in this example is applied to subsequent examples.

[0076] Example 2

[0077] In this example, octenyl starch succinate (OSAS) and sodium caseinate (SC) were used to prepare OSAS / SC composite particles.

[0078] Quantities of OSA starch (degree of substitution DS = 0.024, 0.03, and 0.037) and sodium caseinate were dispersed in deionized water, stirred at 60 rpm for 2 h, and allowed to stand for full hydration to prepare solutions of the corresponding concentrations. For use, OSA starch was mixed with SC solutions of varying concentrations at equal volumes at a constant speed (20-40 rpm) to produce composite solutions with varying OSAS / SC ratios (r = 1:1, 3:1, 6:1, 9:1, 12:1, and 15:1, m / m). The OSA starch concentration in the composite solutions was fixed at 6% (w / v). The pH of the composite solutions (pH = 3-9) was adjusted using varying concentrations of HCl or NaOH (0.01 mol / L-2 mol / L) to minimize dilution. OSAS / SC complexes were prepared by centrifugation of the complex solution (3000 g, 10 min) and freeze-drying (-40°C, 0.9 Pa). The complex yield (%) was determined by calculating the ratio of the mass of the dried complex to the total mass of OSA starch and SC added to the initial complex solution. The freeze-dried particles of the OSAS / SC complex were used to prepare the Pickering emulsion described below.

[0079] Zeta potential and average particle size determination: The zeta potential, average particle size, and polydispersity index (PDI) of the complex solution were measured using a Malvern Zetasizer Nano ZS90 particle size analyzer. Prior to measurement, the complex solution was diluted with deionized water at a ratio of 1:100 (v / v) and vortexed to minimize multiple scattering. A 2 mL sample was aspirated and measured at 25°C. Each sample was measured in triplicate.

[0080] Determination of the three-phase contact angle of the composite particles: The three-phase contact angle of the composite was measured by a video optical contact angle meter ( θow ) for measurement and analysis. It was immersed in a glass cuvette filled with soybean oil. Using the sitting drop method, 5 μL of deionized water was slowly dropped onto the surface of the cylindrical sheet using a high-precision syringe. After balancing for 4 seconds, a high-speed camera was used to capture the droplet image. The Laplace-Young equation was fitted to obtain θow Each sample was measured three times in parallel.

[0081] Data analysis: All experiments were performed more than three times independently and the results are expressed as mean ± standard deviation.

[0082] The yield, particle size and Zeta potential of the OSAS / SC complex are shown in Table 4. The yields at different degrees of substitution are as follows: DS = 0.037 > DS = 0.024 > DS = 0.030. The yields at the six composite ratios are as follows: 15:1 > 6:1 > 9:1 > 12:1 > 1:1 > 3:1. The yields at the seven pH values ​​are as follows: pH 6 > pH 9 > pH 5 > pH 3 > pH 4 > pH 8 > pH 7.

[0083] Table 4 Yield, particle size, PDI and Zeta potential (n=3) of OSAS / SC complexes at different complex ratios / substitution degrees / pH values

[0084]

[0085] OSA starch with different degrees of substitution θow They are 34.35°, 31.10°, and 30.35° respectively, and are extremely hydrophilic. After electrostatic complexation with SC, the composite θow Increase. Figure 4 This is a schematic diagram of the wettability of the OSAS / SC complex solution at different composite ratios / pH values / substitution degrees in Example 2. θow The influence is significant. When the composite ratio is 1:1, the maximum contact angle of the composite is 63.05°. The pH value has a significant effect on the composite. θow There is also a certain influence. When pH=3, which is lower than the isoelectric point of SC, SC flocculates, the SC content decreases, and the relative content of OSA increases. θow The results showed that the zeta potential of the OSA starch / SC composite solution decreased significantly at pH 5, and the particle size decreased significantly. As the pH increased further, both OSA starch and SC were negatively charged, which led to electrostatic repulsion, thus causing the particle size to increase. When the pH was below the isoelectric point (pI = 4.6), sodium caseinate carried a positive charge, and OSA starch was partially deprotonated at pH 4, resulting in a negative surface charge. The electrostatic attraction between the positive and negative charges of OSA starch and SC drove the two to form a complex. As the pH decreased, the charge strength weakened, the positive and negative charges in the solution became similar, and the electrostatic repulsion between SC and OSA starch decreased, resulting in flocculation and a decrease in yield. With the increase in OSA starch concentration, the zeta potential of the OSAS / SC composite solution showed a decreasing trend of varying magnitude. At the same time, the PDI of the OSAS / SC solution gradually increased, and the particle size distribution became more uneven. When the OSA starch:SC composite ratio reached 1:1, the particle size was minimized to 197.57±3.17 nm, and the absolute value of the zeta potential was maximized to -35.17±2.45 mV.

[0086] Combined with the particle size, potential, and contact angle results of the OSAS / SC composites at different composite ratios / pH values / degrees of substitution, the composite conditions of OSA starch DS = 0.037, composite ratio 1:1, and pH values ​​of 4 and 5 were selected as the preparation conditions for further screening of the composites.

[0087] Example 3

[0088] In this example, the method of Example 2 was used to prepare OSAS / SC complex particles (pH = 4 and 5). The preparation principle involved characterizing the particle size and potential of different complex particles (pH = 4 and 5) and using this potential as an indicator of their ability to stabilize Pickering emulsions containing snake oil as the oil phase. Preparation conditions were selected with oil phase volumes of 30% and 75%, respectively. The resulting emulsions were characterized by particle size, potential, and appearance, allowing for further screening of two complexes. Table 5 shows the yield, particle size, PDI, and zeta potential of the OSAS / SC complex (pH = 4 and 5). When the pH of the OSAS / SC complex was 4, the yield reached 33.13±4.23%, the minimum particle size reached 107.07±3.10 nm, the PDI was 0.52±0.03, and the zeta potential reached -10.17±1.80 mV.

[0089] Table 5 Yield, particle size, PDI and Zeta potential of OSAS / SC complex (pH = 4, 5) in Example 3

[0090]

[0091] Pickering emulsion particle size and potential results are as follows Figure 5 When pH=4 and Φ=75%, the emulsion particle size is the smallest; the absolute value of the Zeta potential of the two emulsions prepared using the composite particles OSAS / SC (pH=5) is significantly higher than that of the emulsion prepared using the composite particles OSAS / SC (pH=4), which is -28.6±0.3 mV. The results are related to the Zeta potential of the composite particle solution. Figure 6 The following images show the appearance of the four emulsions used in this experiment after standing for 24 hours: A-OSAS / SC composite (pH = 4) (Φ = 30%); B-OSAS / SC composite (pH = 4) (Φ = 75%); C-OSAS / SC composite (pH = 5) (Φ = 30%); and D-OSAS / SC composite (pH = 5) (Φ = 75%). It can be clearly seen that the two emulsions prepared using the composite particles OSAS / SC (pH = 5) exhibited stratification and oil phase precipitation, indicating poor emulsion stability. At pH = 4 and Φ = 75%, the emulsion particle size reached a minimum of 79.36 ± 1.97 μm, and the emulsion was relatively stable, with no stratification after standing at room temperature for 24 hours.

[0092] Combined with the above results, the composite conditions of OSA starch substitution degree of 0.037, composite ratio of 1:1, and pH value of 4 were finally selected as the preparation conditions of the composite, and the composite prepared under these conditions was used as an emulsifier to stabilize the Pickering emulsion with snake oil as the oil phase.

[0093] Example 4

[0094] In this example, OSAS / SC composite particles (substitution degree DS = 0.037, pH = 4, composite ratio 1:1) were used as the preparation conditions for the composite and characterized.

[0095] Characteristic groups and crystal structure of composite particles: The characteristic groups of OSA starch, SC, and composite samples were determined by Fourier transform infrared spectroscopy (FT-IR). The dried samples were mixed with KBr in an agate mortar at a ratio of 1:100 (w / w), ground, and pressed into pellets. A blank KBr was used as a control. The measurement wavelength was 4000-500 cm -1 , resolution 4 cm -1 The crystal structure of the composite was determined using an X-ray diffraction (XRD) instrument. The composite particle powder was equilibrated in a desiccator containing a saturated sodium chloride solution for one week. The crystal structure of the composite particles was determined using an X-ray diffractometer with a scan speed of 2° / min, a diffraction angle range of 5° to 40°, and a step size (Δ2θ) of 0.02°.

[0096] Observation of the micromorphology of the composite particles: The surface morphology of the composite was observed by scanning electron microscopy (SEM). The sample was fixed with conductive glue and a gold coating with a thickness of less than 10 nm was sprayed on its surface. The sample was then characterized and analyzed using a scanning electron microscope at a magnification of 2000.

[0097] The characteristic groups and crystal structure results of the complex are as follows Figure 7 As shown. Figure 7 Part A is the FT-IR image of the complex, and the results show that sodium caseinate and OSA starch interact to form a relatively stable OSAS / SC binary complex, rather than a simple physical mixture. Figure 7 Part B is the XRD spectrum of OSA, SC and OSAS / SC complex. It can be seen from the figure that OSA and SC in the complex form an amorphous complex with intermolecular interaction, which is consistent with the above FT-IR results.

[0098] Attachment Figure 7Parts CE (center) and (center) show SEM images of OSAS, SC, and an OSAS / SC composite. The morphological and structural characteristics of the samples were observed using SEM. In the SEM images of OSAS, SC, and the OSAS / SC composite, OSAS exhibits an uneven spherical shape with internal micropores; SC appears as irregular particles with pronounced surface wrinkles. Both OSAS / SC composite particles exhibit a lamellar network structure, with the lamellar layers connected by micropores, demonstrating interaction between OSAS and SC.

[0099] Example 5

[0100] This example presents OSAS / SC composite particles (degree of substitution DS = 0.037, pH = 4, composite ratio 1:1). The method for stably loading snake oil therein is to screen the appearance and particle size of the snake oil Pickering emulsion by the oil phase volume fraction, and to explore the effect of the oil phase volume fraction on the formation of the Pickering emulsion.

[0101] Preparation of Pickering emulsions stabilized by OSA starch / SC composite particles: The OSA starch / SC complex was freeze-dried and diluted with deionized water to obtain an OSA starch / SC complex solution, with the pH adjusted to 4. The complex solution was mixed with snake oil and subjected to shear stirring at 12,000 rpm for 3 minutes at room temperature to prepare a primary emulsion. The primary emulsion was sonicated at 250 W for 5 minutes, with ultrasound on for 6 seconds and off for 3 seconds, to obtain a snake oil Pickering emulsion. To investigate the effect of the oil phase volume fraction (Φ = 5.0%-85.0%, v / v) on the emulsion, c was fixed at 3.0 wt%, and the total emulsion volume was set to 60 mL.

[0102] In the Pickering emulsion prepared in this study, during the emulsification process, the OSAS / SC complex was adsorbed from the aqueous phase to the surface of fat globules, preventing the aggregation of small fat globules and the formation of large fat globules, thereby maintaining the stability of the emulsion. Figure 9 Figure 5 is a particle size potential diagram of the Pickering emulsion stabilized by the OSAS / SC complex at different oil phase volumes in Example 5. [4,3] It has a greater impact. When Φ≥75%, the emulsion particle size is significantly reduced, which is related to the high oil phase ratio causing the emulsion to transform from O / W type to W / O type emulsion.

[0103] Attachment Figure 8This is the appearance diagram of the Pickering emulsion stabilized by OSA / SC composite at different oil phase volume fractions in this embodiment. In the figure, A is the appearance diagram of the Pickering emulsion stabilized by OSA / SC composite at different oil phase volume fractions (stored for 3 days); B is the appearance diagram of the Pickering emulsion stabilized by OSA / SC composite at different oil phase volume fractions (stored for 5 days); C is the appearance diagram of the Pickering emulsion stabilized by OSA / SC composite at different oil phase volume fractions (stored for 7 days); D is the appearance diagram of the Pickering emulsion stabilized by OSA / SC composite at different oil phase volume fractions (stored for 15 days). From the appearance diagrams of the Pickering emulsions stabilized by OSAS / SC composite at different storage times and different oil phase volume fractions, it can be found that when Φ = 75%, the emulsion remains stable and no cream separation phenomenon occurs after 2 weeks of storage. Figure 9 It is the particle size potential diagram of the Pickering emulsion stabilized by OSAS / SC composite at different oil phase volumes in Example 5. Different oil phase volumes have a greater impact on the average particle size D of the emulsion. [4,3] When Φ ≥ 75%, the particle size of the emulsion decreases significantly, which is related to the fact that a high oil phase ratio causes the emulsion to change from an O / W type to a W / O type emulsion. Figure 10 It is the rheological property diagram of the Pickering emulsion stabilized by OSAS / SC composite at different oil phase volume fractions in Example 5. Except for Φ = 75%, as the shear frequency increases, the emulsion gradually evolves from a weak elastic structure (G′ > G′′) to a viscous fluid (G′ < G′′), indicating that the internal gel structure of the emulsion is unstable. In summary, Φ = 75% is selected as the optimal oil phase volume.

[0104] Example 6

[0105] In this embodiment, the OSAS / SC composite particles (degree of substitution DS = 0.037, pH = 4, composite ratio 1:1) are used. The method for stably loading snake oil is to screen the appearance and particle size of the snake oil Pickering emulsion through the concentration of OSAS / SC composite particles. When investigating the influence of the composite particle concentration (c = 0.2% - 10.0%, wt%) on the emulsion, Φ is fixed at 40%, and the total volume of the emulsion is set to 60 mL.

[0106] Attachment Figure 11This is the appearance diagram of the Pickering emulsion stabilized by OSA / SC complex at different particle concentrations in this embodiment. In the figure, A - Appearance diagram of the Pickering emulsion stabilized by OSA / SC complex at different particle concentrations (stored for 3 days); B - Appearance diagram of the Pickering emulsion stabilized by OSA / SC complex at different particle concentrations (stored for 5 days); C - Appearance diagram of the Pickering emulsion stabilized by OSA / SC complex at different particle concentrations (stored for 7 days); D - Appearance diagram of the Pickering emulsion stabilized by OSA / SC complex at different particle concentrations (stored for 15 days). Table 6 shows the particle size and zeta potential results of the Pickering emulsion stabilized by OSAS / SC complex at different particle concentrations in Example 6.

[0107] Table 6 Particle size and zeta potential results of the Pickering emulsion stabilized by OSAS / SC complex at different particle concentrations

[0108]

[0109] The results show that with the increase of particle concentration, the emulsion stability increases. By investigating the particle size, Zeta-potential and appearance morphology of the Pickering emulsion stabilized by OSAS / SC complex at different particle concentrations, it is found that the particle size of the Pickering emulsion stabilized by 0.2% OSAS / SC complex is 32.67 ± 4.90 μm. When the particle concentration is further increased to 0.5 wt%, the droplet size of the emulsion decreases to 3.26 ± 0.08 μm. With the further increase of c, the oil droplet size further decreases. The rheological property results of the Pickering emulsion at different particle concentrations are shown in Figure 12 . All emulsions show similar shear-thinning behavior, and the apparent viscosity and viscoelastic moduli (G′ and G′′) are positively correlated with the complex particle concentration. However, the emulsions all show a viscous fluid structure (G′ < G′′), and the internal gel structure of the emulsion is unstable. Further research is carried out on the Pickering emulsion with an oil phase volume of 75% at different particle concentrations. When c = 8%, the G′ of the emulsion is much higher than its corresponding G′′, and the two moduli are hardly affected by the shear frequency, indicating that the emulsion forms a highly elastic gel network structure. Combining the rheological properties of the Pickering emulsion at different particle concentrations and the emulsion stability at different storage times, the particle concentration of c = 8% is finally selected as the optimal concentration for emulsion preparation.

[0110] Example 7

[0111] This example examined the effects of different dissociation agents on the dispersibility of Pickering emulsions stabilized by OSAS / SC complexes. The emulsions were mixed with different dissociation agents (deionized water, urea (6 mol / L), sodium chloride (100 mmol / L), and SDS (1%, w / v)) in a 1:9 (w / w) ratio. The emulsions were then allowed to stand at 25°C for 1 hour before being observed for dispersion. The emulsions were then vortexed at low speed for 20 seconds, and their microstructures were observed using an optical microscope.

[0112] Figure 13 Figure 7 shows an optical microscopic diagram of the dispersion behavior of the Pickering emulsion stabilized by the OSAS / SC complex in different dissociating agents. The results of investigating the interaction forces and flocculation structure between the Pickering emulsion droplets stabilized by the OSAS / SC complex using different dissociating agents show that the flocculation state of the emulsion droplets changes significantly after dilution with NaCl, indicating that the droplets interact to a high degree through electrostatic interactions on top of flocculation.

[0113] Example 8

[0114] This example is used to examine the effects of pH and ionic strength on Pickering emulsions stabilized by OSAS / SC complexes.

[0115] The effect of pH on the stability of Pickering emulsions was investigated. The pH of the Pickering emulsions was adjusted to 3.0, 4.0, 5.0, 6.0, 7.0, and 9.0, respectively, using 1 mol / L HCl solution or NaOH solution. After refrigeration at 4°C for 5 h, the appearance, droplet size, and zeta potential of the emulsions were recorded.

[0116] Figure 14 3 is a graph showing the particle size and zeta potential of the Pickering emulsion stabilized by the OSAS / SC complex at different pH values ​​and ionic strengths in Example 8. Figure 15Schematic diagram of the appearance of the Pickering emulsion stabilized by the OSAS / SC complex at different pH values ​​and ion concentrations in Example 8. The results demonstrate that the Pickering emulsion stabilized by the OSAS / SC complex exhibits a certain degree of responsiveness to changes in pH and possesses a certain degree of ionic stability. As the pH of the emulsion increases from 3.0 to 5.0, as the potential decreases from -1.2 mV to -21.67 mV, the repulsive force between the emulsion droplets increases, the stability of the emulsion increases, and the droplet size decreases significantly, from 390.67 μm to 1.38 μm. As the pH increases further, the Pickering emulsion droplet size increases significantly. At pH 5.0 and 6.0, the emulsion remains stable, exhibiting a uniform and stable appearance. At pH ≥ 7, both OSA starch and SC carry negative charges, and excessive electrostatic repulsion may lead to a loose structure of the complex and decreased emulsion stability. These results demonstrate that the Pickering emulsion stabilized by the OSAS / SC complex exhibits a certain degree of responsiveness to changes in pH.

[0117] The effect of ionic strength on the stability of Pickering emulsions was investigated. Different concentrations of NaCl (0 mmol / L, 30 mmol / L, 60 mmol / L, 90 mmol / L, 120 mmol / L, 150 mmol / L, and 200 mmol / L) were mixed with Pickering emulsions at a ratio of 1:1 (V / V). After refrigeration at 4°C for 24 h, the appearance, droplet size, and zeta potential of the emulsions were recorded. Figure 14 Part B shows the changes in emulsion particle size and potential at different ionic strengths. As the NaCl concentration increases from 0 mmol / L to 200 mmol / L, the emulsion particle size increases slowly. After reaching 120 mmol / L, the increase in ion concentration has little effect on the emulsion particle size and potential. This result is related to the shielding effect of salt ions on the surface potential of the complex and droplets. As the NaCl concentration increases, the potential of the emulsion droplets decreases, the electrostatic repulsion between the droplets weakens, and the emulsion droplets partially coalesce, increasing the droplet size. However, further increases in ion concentration have little effect on the emulsion particle size and potential.

[0118] Example 9

[0119] This example is used to test the effect of different temperatures on the Pickering emulsion stabilized by the OSAS / SC complex.

[0120] The effect of temperature on the stability of the Pickering emulsion of Example 5 (c = 8%, Φ = 75%) was investigated by storing the emulsion at different temperatures (-4°C, 25°C, 37°C, 60°C, and 90°C) for 30 min.

[0121] Figure 16 Schematic diagram of the particle size and Zeta potential of the Pickering emulsion stabilized by the OSAS / SC complex at different temperatures in Example 9. Figure 17 The following are images of the Pickering emulsions stabilized by the OSAS / SC complex at different temperatures in Example 9. The Pickering emulsions stored at different temperatures showed no significant changes in appearance, and no demulsification occurred. This result indicates that the Pickering emulsion stabilized by the OSAS / SC complex has good temperature flexibility.

[0122] Example 10

[0123] This example tested the centrifugal stability of Pickering emulsions stabilized by the OSAS / SC complexes described in Example 6 at various particle concentrations (c = 3-10%, Φ = 75%). 15 g of freshly prepared Pickering emulsion was placed in a 50 mL centrifuge tube and centrifuged at 4000 g for 15 minutes at 4°C. The emulsion's appearance after centrifugation was used as a guide for determining its centrifugal stability. The centrifugal stability was further analyzed in conjunction with the WHC. After centrifugation, the upper oil phase, lower aqueous phase, and intermediate emulsion were weighed. The WHC of the emulsion was calculated using the following formula:

[0124]

[0125] W in the formula T is the total mass of the sample, W F is the mass of water released after centrifugation.

[0126] Centrifugation accelerates the emulsion's creaming process, forcing the droplets to coalesce. After centrifugation, excess water is expelled from the emulsion, creating a tight encapsulation. Phase separation occurred in all emulsions after centrifugation, with the lower layer of the centrifuge tube containing water and the upper layer containing the emulsion after water separation. However, no demulsification leading to oil leakage was observed. Figure 18 Part A is a schematic diagram of the centrifugal stability of the Pickering emulsion stabilized by the OSAS / SC complex at different particle concentrations in Example 10. Figure 18 Part B is a graph showing the centrifugal water retention of Pickering emulsions stabilized by the OSAS / SC complex at different particle concentrations in Example 10. The water retention of all emulsions is above 60%, indicating that the stable structure of the emulsion can retain a large amount of water.

[0127] Example 11

[0128] This example detects the in vitro antioxidant activity of the Pickering emulsion of Example 5 (c=8%, Φ=75%). The DPPH free radical scavenging ability kit was used to prepare the test solutions and working solutions according to the requirements of the test kit. The samples were diluted to 4 times with anhydrous ethanol. The control group was 400 μL of sample added to 600 μL of anhydrous ethanol; the assay group was 400 μL of sample added to 600 μL of DPPH working solution; the blank group was 400 μL of anhydrous ethanol added to 600 μL of DPPH working solution, and the mixture was mixed. The mixture was allowed to stand at room temperature at 25°C in the dark for 30 min, centrifuged at 4000 r / min for 5 min, the supernatant was taken, its OD value at 517 nm was determined, and the DPPH free radical scavenging rate (%) was calculated according to the following formula:

[0129]

[0130] Using a DPPH free radical scavenging assay kit, prepare the test solutions and working solution according to the kit's instructions. Samples were diluted 4-fold with anhydrous ethanol, and 20 μL of peroxidase working solution was added to each well. To the blank well, standard well, and assay well, add 10 μL of distilled water, 10 μL of standard solutions of varying concentrations, and the 4-fold diluted sample solution. Gently shake to mix. Add 170 μL of ABTS working solution to each well and shake to mix. Incubate at room temperature for 6 minutes. Measure the absorbance at 405 nm using a microplate reader. The total antioxidant capacity of the Pickering emulsion and deodorized Bungarus bungarus oil was calculated using the standard curve. Figure 19 Part A is the result diagram of the DPPH free radical scavenging ability of the Pickering emulsion in Example 11. Figure 19 Part B shows the total antioxidant capacity of the Pickering emulsion in Example 11. The results show that the Pickering emulsion has a higher antioxidant capacity than the original snake oil, with a total antioxidant capacity of 0.66 mM, equivalent to 0.66 mM Trolox. The original snake oil has a slightly lower total antioxidant capacity of 0.45 mM Trolox. In vitro antioxidant studies demonstrate that snake oil has a certain antioxidant capacity, and preparing it into a Pickering emulsion further enhances its antioxidant capacity.

[0131] The above experiments demonstrate that β-zeolite was used to remove the fishy smell of snake oil and to prepare OSAS / SC particles as stabilizing particles. Ultrasound-assisted Pickering emulsions were prepared. The effects of varying OSA / SSC concentrations and oil volume fractions on the particle size, appearance, and microstructure of the emulsions were investigated. The results showed that when the oil volume fraction remained constant, the particle size decreased to 22.18 ± 2.47 μm as the OSAS / SC concentration increased to 8.0%. At a constant OSAS / SC concentration, increasing the oil volume fraction resulted in larger particle sizes and thicker emulsion layers. As the oil volume fraction increased to 75%, the emulsion remained stable after 15 days of storage at room temperature, exhibiting no creaming, demulsification, or demixing. The microstructure of the Pickering emulsions stabilized by the composite particles was investigated using optical microscopy. The droplets were round and tightly connected, indicating that the OSAS / SC was firmly adsorbed to the oil-water interface. The pH, ionic strength, thermal, and centrifugal stability of a Pickering emulsion stabilized by composite particles were investigated. The results demonstrated good temperature flexibility, high stability to ionic strength, and a moderate responsiveness to pH changes. Centrifugal stability tests revealed that the emulsion's water retention capacity exceeded 60%, indicating that its stable structure was capable of retaining a significant amount of water.

Claims

1. A process for preparing a fishy-free snake oil Pickering emulsion, characterized in that: The process involves using β-molecular sieves to remove the odor of snake oil and using octenyl succinate starch ester (OSAS) / sodium caseinate (SC) complex particles to construct a Pickering single emulsion loaded with snake oil. The specific construction operation is as follows: using an aqueous solution of the OSAS / SC complex particles as the aqueous phase and the deodorized snake oil as the oil phase, the aqueous phase and the oil phase are mixed, and then sheared and stirred at a certain temperature to prepare a primary emulsion, and then subjected to ultrasound to obtain a snake oil Pickering emulsion.

2. The preparation process of a deodorized snake oil Pickering emulsion according to claim 1, wherein The snake oil is selected from any one of the snake oils of Bungarus bungarus, Agkistrodon wiryana, Agkistrodon acutus, Cobra or Elaphe.

3. The preparation process of a deodorized snake oil Pickering emulsion according to claim 1, wherein In the step of removing the smell of snake oil by using β-molecular sieve, the mass ratio of snake oil to β-molecular sieve is 10:0.1-10, and the snake oil and β-molecular sieve are stirred and reacted at 30-50° C. for 0.5-5 hours.

4. The preparation process of a deodorized snake oil Pickering emulsion according to claim 3, wherein: In the step of removing the fishy smell of snake oil by using β-molecular sieve, the mass ratio of snake oil to β-molecular sieve is 10:1, and the snake oil and β-molecular sieve are stirred and reacted at 35° C. for 1 hour.

5. The preparation process of a deodorized snake oil Pickering emulsion according to claim 1, wherein The preparation method of the OSAS / SC complex particles is as follows: equal volumes of OSAS solution and SC solution are mixed at a constant speed to obtain a complex solution, and the complex solution is centrifuged and freeze-dried to obtain the OSAS / SC complex particles.

6. The preparation process of a deodorized snake oil Pickering emulsion according to claim 5, wherein: In the composite solution, the composite ratio of OSAS and SC is 1-15:1; and / or, in the composite solution, the concentration of OSAS is 6% (w / v); and / or, the degree of substitution of OSA starch is 0.024, 0.03, or 0.037; And / or, the pH of the composite solution is 4-5.

7. The preparation process of a deodorized snake oil Pickering emulsion according to claim 1, characterized in that: In the aqueous phase, the concentration of OSAS / SC composite particles was 0.6 wt%-10.0 wt%; and / or, the pH of the aqueous phase is 4-5; and / or, the volume fraction of the oil phase is 50.0-85.0%; And / or, the ultrasonic power is 200-300W; the ultrasonic conditions are ultrasonication for 6 seconds and rest for 3 seconds, for a total of 5 minutes.

8. The process for preparing a deodorized snake oil Pickering emulsion according to claim 7, wherein: The ultrasonic power is 250W.

9. A deodorized snake oil Pickering emulsion prepared according to the preparation process according to any one of claims 1 to 8.

10. Use of the deodorized snake oil Pickering emulsion prepared according to the preparation process according to any one of claims 1 to 8 in the fields of cosmetics, food or medical health products.

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