A natural plant source-containing essence-nourishing and body-strengthening composition and a preparation method thereof

Abstract

The present application belongs to the technical field of natural product extraction, and particularly relates to a natural plant source-containing essence benefiting and body consolidating composition and a preparation method thereof. In view of the technical contradiction that when medium-polarity active ingredients are extracted by supercritical CO2, ethanol entrainer leads to excessive solvent residue and degradation of heat-sensitive components, and when there is no entrainer, the extraction rate suddenly decreases, the present application provides a solution: mixing a natural plant raw material extract with an entrainer composed of natural phosphatidylcholine and modified phytosterol ester, treating under the condition of supercritical CO2 at 25-40 MPa and 45-65 DEG C, and then collecting the precipitate after multi-stage pressure reduction to normal pressure. The solution utilizes the characteristics of the entrainer, i.e., solubilization under high pressure and spontaneous dissociation after pressure reduction, to realize the unity of high extraction rate and zero residue. The examples show that the extraction yield of target components is greater than or equal to 88%, the ethanol residue is less than 1 ppm, and the retention rate of heat-sensitive components is greater than or equal to 94%. The present application has the advantages of high efficiency, greenness and safety, and has good industrial application prospect.

Description

Technical Field

[0001] This invention belongs to the field of natural product extraction technology, specifically relating to a composition for nourishing essence and strengthening the body containing natural plant sources and its preparation method. In particular, it relates to a method for preparing a composition containing active ingredients from natural plant sources using supercritical fluid technology. Background Technology

[0002] Supercritical carbon dioxide extraction technology has been widely used in the extraction and separation of active ingredients from natural products due to its advantages such as low operating temperature, no organic solvent residue, and environmental friendliness. However, supercritical carbon dioxide itself is a non-polar solvent, and its solubility for moderately polar components such as polysaccharides and glycosides is extremely limited, making it difficult to achieve effective extraction.

[0003] To address the aforementioned issues, the art typically employs the method of adding entrainers to supercritical carbon dioxide systems. Entrainers can alter the solubility of supercritical fluids, thereby improving the extraction efficiency of moderately polar components. Organic solvents such as ethanol, methanol, and acetone are commonly used entrainers, and studies have shown that adding even small amounts of entrainers can significantly enhance the solubility of the target components.

[0004] However, the aforementioned organic entrainers have inherent drawbacks in practical applications. During the separation stage after extraction, the entrainers cannot separate from the extract on their own and must be removed through heating, vacuuming, or other methods. This removal process not only increases the complexity of the process, but more importantly, high temperatures may cause degradation of heat-sensitive active ingredients, and the risk of residual organic solvents always exists, limiting the product's application in fields such as health foods. On the other hand, without the use of any entrainers, the extraction efficiency of moderately polar components by supercritical carbon dioxide decreases significantly.

[0005] Therefore, existing supercritical carbon dioxide extraction technology still faces the challenge of balancing extraction efficiency and product safety when processing moderately polar natural active ingredients. Summary of the Invention

[0006] The purpose of this invention is to overcome the dilemma in existing technologies for supercritical CO2 extraction of moderately polar active ingredients: while adding organic entrainers can improve the extraction rate, it also poses risks of solvent residue and degradation of heat-sensitive components; conversely, without entrainers, the extraction efficiency drops significantly. This invention provides a beneficial and nourishing composition containing natural plant sources and its preparation method. The natural plant extract is mixed with an entrainer composed of natural phosphatidylcholine and modified phytosterol esters. After supercritical CO2 treatment, the pressure is gradually reduced, causing the entrainer to spontaneously dissociate and the target component to be released. Complete separation of the entrainer and product can be achieved without high-temperature solvent removal. Examples show that this method achieves an extraction yield of 94.2%, solvent residue below the detection limit, and a heat-sensitive component retention rate of 96.8%, thus simultaneously achieving high extraction efficiency, zero solvent residue, and high activity retention.

[0007] A first aspect of the present invention provides a method for preparing a tonic composition containing natural plant sources, comprising the following steps: (1) Mix 40-65 parts by weight of natural plant raw material extract with 15-30 parts by weight of entrainer to form a premix; the entrainer is a compound of natural phosphatidylcholine and modified phytosterol ester in a weight ratio of 1:1.5-1:3. (2) Supercritical treatment was carried out in supercritical carbon dioxide fluid at 25-40 MPa and 45-65℃. (3) The effluent from step (2) is gradually depressurized to atmospheric pressure, the precipitate is collected and dried to obtain the composition.

[0008] This application provides a method for preparing a composition containing natural plant sources that benefits essence and strengthens the body. The method involves mixing natural plant extracts with an entrainer composed of natural phosphatidylcholine and modified phytosterol esters in a specific ratio, treating the mixture under supercritical CO2 conditions of 25-40 MPa and 45-65℃, collecting the precipitates by gradually reducing the pressure, and drying the mixture to obtain the final composition. Phosphatidylcholine has an amphiphilic molecular structure. Its polar head can capture moderately polar active ingredients through intermolecular interactions such as hydrogen bonds, while its nonpolar tail has good compatibility with supercritical CO2. Modified phytosterol esters are embedded in the hydrophobic region of phospholipid molecules and bind to the nonpolar tail of phospholipids through hydrophobic interactions and van der Waals forces, enhancing the stability of the associated structure. In a high-pressure supercritical CO2 environment, the two work together to form a ternary transient complex structure with phospholipids as the shell, sterol esters as the backbone, and the target ingredient as the core. This effectively shields the polar repulsion between the target ingredient and CO2, allowing it to be carried into the fluid phase. During depressurization, the decrease in CO2 density weakens the solubilization ability, and the associated structure spontaneously dissociates. The target ingredient precipitates in the solid state, while the entrainer component is automatically separated and removed due to differences in density and polarity. Complete separation can be achieved without high-temperature desolvation. The overall extraction yield can reach 94.2% after adopting the technical solution of this application, the ethanol residue is lower than the detection limit (<1 ppm), and the retention rate of heat-sensitive active ingredients reaches 96.8%, successfully achieving high extraction efficiency, zero solvent residue and high activity retention at the same time.

[0009] Furthermore, in the entrainer, the weight ratio of natural phosphatidylcholine to modified phytosterol ester is 1:1.8-1:2.5. Studies have found that the mass ratio of the two raw materials in the entrainer is a key factor affecting the solubilization effect. Reasonably controlling the weight ratio of the two components can better achieve the optimal balance between polar and nonpolarity in the system, allowing the entrainer to more effectively form a stable intermolecular association structure with the target component, thereby obtaining the optimal extraction efficiency.

[0010] Furthermore, the natural plant extracts mentioned in step (1) are selected from one or more of the following: ginsenoside enrichment, polygonatum oligosaccharide, icariin extract, maca extract, cistanche extract, and yam extract.

[0011] Furthermore, the premix described in step (1) also contains 5-12 parts by weight of a natural antioxidant stabilizer and 3-8 parts by weight of a pH buffer regulator.

[0012] Furthermore, the natural antioxidant stabilizer is a compound of vitamin E acetate and tea polyphenols in a weight ratio of 2:1 to 4:1; the pH buffer regulator is a mixture of sodium citrate and dipotassium hydrogen phosphate in a weight ratio of 1:1 to 2:1.

[0013] Antioxidant stabilizers: Vitamin E acetate is a fat-soluble antioxidant, and tea polyphenols are water-soluble antioxidants. The combination of these two forms a synergistic antioxidant network at the water-supercritical CO2 interface, effectively inhibiting the oxidative degradation of active ingredients during supercritical processing. pH buffering agents: The sodium citrate-dipotassium hydrogen phosphate buffer pair maintains the extraction system in a weakly acidic to neutral environment (pH 5.0-7.0), preventing extreme pH levels from causing hydrolysis or structural transformation of active ingredients. By introducing natural antioxidant stabilizers and pH buffering agents into the premix, the stability of heat-sensitive active ingredients during processing is effectively protected, extending the product's shelf life.

[0014] Furthermore, before step (1), the following steps are also included: crushing the natural plant raw materials to 40-80 mesh and vacuum drying them at 45-60℃ to a moisture content of 5%-8%.

[0015] Furthermore, in step (1), the mixing operation is carried out by stirring and melting at 50-70℃ under nitrogen protection for 0.5-1.5 hours, with the stirring speed controlled at 200-400 rpm.

[0016] Furthermore, in step (2), the carbon dioxide flow rate is 15-30 kg / h and the treatment time is 1.5-3.0 hours.

[0017] Crushing the material to 40-80 mesh ensures sufficient contact area between the raw material particles and supercritical CO2. A moisture content of 5%-8% can form a weak polar liquid film on the surface of the raw material, which helps the entrainer to wet and penetrate.

[0018] The premix is ​​melted at 50-70℃ under nitrogen protection, which ensures the full melting and mixing of phospholipids and sterol esters while avoiding high-temperature oxidation.

[0019] The coordinated control of CO2 flow rate and processing time ensures a balance between mass transfer efficiency and processing cost.

[0020] Furthermore, in step (3), the pressure is first reduced to 10-15 MPa for primary separation, and then reduced to 0.1 MPa for secondary separation. 10-15 MPa is the golden transition pressure range selected by this application through a large number of experiments: below 10 MPa, the entrainer dissociates too early, and the target component precipitates prematurely in the primary separation, resulting in a decrease in yield; above 15 MPa, impurities are not fully precipitated, affecting the purity of the product. Specifically, at a pressure of 10-15 MPa, the density and solubility of supercritical CO2 are in an intermediate state: large molecular impurities precipitate due to insufficient solubility, while the association structure of the entrainer-target component has not been completely dissociated, and the target component is retained in the fluid phase to enter the secondary separation. When the pressure is further reduced to 0.1 MPa (atmospheric pressure), CO2 completely loses its solubility, the association structure is completely dissociated, and the target component is concentrated and precipitated. Multi-stage pressure reduction is the core process means for this application to achieve spontaneous dissociation and gentle separation. By precisely controlling the pressure nodes of the primary and secondary separation, a gradient separation effect is achieved, in which impurities precipitate first, entrainers prepare for dissociation, and the target components are concentrated and precipitated last. This ensures both the extraction yield and the protection of the heat-sensitive active ingredients.

[0021] Furthermore, in step (3), the drying operation is vacuum belt drying at 35-50℃ for 1-2 hours.

[0022] A second aspect of the present invention provides a preservative-strengthening composition containing natural plant sources, prepared by the method described above.

[0023] The essence-enhancing and tonic composition containing natural plant sources disclosed in this application is directly obtained by the above-described preparation method. Since the preparation process does not require high-temperature solvent removal, degradation of heat-sensitive active ingredients is avoided, and the retention rate of active ingredients in the product can reach over 94%. Simultaneously, because the entrainer spontaneously dissociates and automatically separates during the separation stage, there are no organic solvent residues in the product (ethanol residue <1 ppm), meeting compliance standards in fields with high safety requirements such as health foods. Furthermore, experimental studies show that the overall extraction yield of this composition can reach 87.2%-94.2%, and the product exhibits excellent batch-to-batch stability.

[0024] Furthermore, the overall extraction yield of the target active ingredient in the composition is ≥88%, the residual ethanol content is <1ppm, and the retention rate of the heat-sensitive active ingredient is ≥94%.

[0025] The composition of this invention exhibits a regular granular structure with a uniform particle size distribution (D50 of 15-25 μm). This morphological characteristic stems from the uniform mixing of the entrainer and the target component at the molecular level during supercritical processing. After spontaneous dissociation through multi-stage depressurization, the target component is uniformly precipitated in the form of fine particles, ensuring the consistency and stability of the product.

[0026] Compared with the prior art, the beneficial effects of the present invention are as follows: 1. This invention uses a combination of natural phosphatidylcholine and modified phytosterol esters as an entrainer to form a reversible association structure with the target component in a supercritical CO2 environment, which significantly improves the solubility of moderately polar active ingredients and achieves an extraction yield of 94.2%, which is a significant improvement over the process without an entrainer.

[0027] 2. This invention utilizes the spontaneous dissociation property of the discovered entrainer under progressively decreasing pressure conditions, which can achieve complete separation of the entrainer from the product without high-temperature desolventizing, so that the residual ethanol in the product is below the detection limit (<1 ppm), eliminating the risk of organic solvent residue and meeting the compliance standards of fields with high safety requirements such as health food.

[0028] 3. This invention employs medium-low pressure and medium-low temperature supercritical processing conditions of 25-40 MPa and 45-65℃, combined with a multi-stage depressurization separation process that does not require heating. This avoids the damage of heat-sensitive active ingredients to high temperatures, resulting in a heat-sensitive ingredient retention rate of 96.8%, which is significantly better than traditional ethanol entrainment processes and high-temperature and high-pressure processes.

[0029] 4. This invention uses natural plant-derived components as entrainers, and the entire process does not involve volatile organic solvents. The entrainers can be automatically removed in layers after separation, without the need for additional solvent recovery processes. The process is green and environmentally friendly, has low energy consumption, and is easy to operate, and has good prospects for industrial application. Detailed Implementation

[0030] The present invention will now be described in further detail with reference to specific embodiments. However, this should not be construed as limiting the scope of the present invention to the following embodiments; all technologies implemented based on the content of the present invention fall within the scope of the present invention.

[0031] It should be noted that the terms "first" and "second" are used for descriptive purposes only and should not be construed as indicating or implying relative importance or implicitly specifying the number of indicated technical features. Therefore, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature. Furthermore, in the description of this invention, unless otherwise stated, "a plurality of" means two or more. The endpoints and any values ​​of the ranges disclosed herein are not limited to the precise ranges or values, and these ranges or values ​​should be understood to include values ​​close to these ranges or values. For numerical ranges, the endpoint values ​​of the various ranges, the endpoint values ​​of the various ranges and individual point values, and individual point values ​​can be combined with each other to obtain one or more new numerical ranges, which should be considered as specifically disclosed herein. To facilitate understanding of the invention, certain technical and scientific terms are specifically defined below. Unless otherwise expressly defined elsewhere in this document, all other technical and scientific terms used herein have the meanings commonly understood by one of ordinary skill in the art to which this invention pertains. In this document, the terms “comprising” or “including” are open-ended expressions, meaning that they include the contents specified in this invention, but do not exclude other aspects. In this document, the terms “optionally,” “optionally,” or “optionally” generally refer to an event or condition that may, but may not, occur, and the description includes both cases in which the event or condition occurs and cases in which the event or condition does not occur. To better understand the technical solutions of the above embodiments, the following more detailed experimental examples are provided for further explanation. Those skilled in the art will understand that the following examples are for illustrative purposes only and should not be considered as limiting the scope of this disclosure. Where specific techniques or conditions are not specified in the examples, they are performed according to the techniques or conditions described in the literature in the art or according to the product instructions. Reagents or instruments used, unless otherwise specified, are all commercially available conventional products.

[0032] The sources and specifications of the raw materials used in the following examples and comparative examples are as follows: Natural plant extracts (ginsenoside enrichment, Polygonatum oligosaccharides, and icariin extract) were purchased from Xi'an Tianyi Biotechnology Co., Ltd. The Polygonatum oligosaccharides refer to oligosaccharide products obtained by degradation treatment of Polygonatum polysaccharides, with a molecular weight lower than that of untreated crude Polygonatum polysaccharides.

[0033] Natural phosphatidylcholine (brand name SPC-70), purchased from Lipoid GmbH.

[0034] The modified phytosterol ester (brand name Plantanol D MAX) was purchased from BASF SE. The modified phytosterol ester is an esterification product obtained by esterification of phytosterols with fatty acids, with an esterification rate ≥95%.

[0035] Vitamin E acetate, purchased from DSM Nutritional Products.

[0036] Tea polyphenols were purchased from Hunan Tianxiakang Biotechnology Co., Ltd.

[0037] Sodium citrate and dipotassium hydrogen phosphate were purchased from Sinopharm Chemical Reagent Co., Ltd.

[0038] Example 1 Formula composition (by weight): Natural plant extracts (25 parts ginsenoside concentrate, 15 parts polygonatum oligosaccharide, 10 parts icariin extract): 50 parts; Entrainer (a mixture of natural phosphatidylcholine and modified phytosterol esters in a weight ratio of 1:2): 22 parts; Natural antioxidant stabilizer (a blend of vitamin E acetate and tea polyphenols in a 3:1 weight ratio): 8 parts; pH buffer (sodium citrate and dipotassium hydrogen phosphate mixed in a 1:1 weight ratio): 5 parts.

[0039] Preparation method: S1 (Pretreatment): The above natural plant raw material extracts are pulverized to 60 mesh, mixed evenly, and placed in a vacuum drying oven. They are dried at 55°C for 3 hours to control the moisture content of the material to 6.5%.

[0040] S2 (Premix Preparation): Add 22 parts of entrainer and 8 parts of natural antioxidant stabilizer to a melting tank equipped with a nitrogen protection device. Purge the air in the tank with high-purity nitrogen, heat to 60°C, turn on the stirrer, and stir at 300 rpm for 1.0 hour to form a homogeneous and transparent liquid premix. Then add 5 parts of pH buffer adjuster and continue stirring for 15 minutes to disperse it evenly.

[0041] S3 (Supercritical Treatment): The raw material treated in S1 is loaded into a supercritical extraction vessel. The liquid premix obtained in S2 is injected into the top spray system of the extraction vessel by a high-pressure pump to uniformly wet the material. The supercritical carbon dioxide generator is started, and the pressure is controlled at 32 MPa, the temperature at 55℃, the carbon dioxide flow rate at 22 kg / h, and the dynamic treatment time is 2.0 hours.

[0042] S4 (Multi-stage pressure reduction and collection): The effluent enters the multi-stage separation system. First, it is depressurized to 12MPa by the first-stage pressure reducing valve for primary separation, and then depressurized to 0.1MPa (atmospheric pressure) by the second-stage pressure reducing valve for secondary separation. The target component precipitates at the bottom of the separation vessel, and the precipitate is collected.

[0043] S5 (drying): The collected precipitate is transferred to a vacuum belt dryer and dried at 42°C for 1.5 hours to obtain the final product of the Yijing Guben composition.

[0044] The total extraction yield was 94.2%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 96.8%.

[0045] Example 2 Based on Example 1, only the weight ratio of natural phosphatidylcholine to modified phytosterol ester in the entrainer was adjusted to 1:1.2, 1:1.5, 1:1.8, 1:2.0, 1:2.2, 1:2.5, 1:3.0, and 1:4.0, respectively. The rest of the formulation and preparation method were exactly the same as in Example 1.

[0046] The test results are shown in Table 1.

[0047] Table 1. Effect of different entrainer ratios on extraction efficiency Example 3 Formula composition: Natural plant extracts (20 parts ginsenoside concentrate, 12 parts polygonatum oligosaccharide, 8 parts icariin extract): 40 parts; Entrainer (a mixture of natural phosphatidylcholine and modified phytosterol esters in a weight ratio of 1:2): 18 parts; Natural antioxidant stabilizer (a blend of vitamin E acetate and tea polyphenols in a 3:1 weight ratio): 8 parts; pH buffer (sodium citrate and dipotassium hydrogen phosphate mixed in a 1:1 weight ratio): 5 parts.

[0048] Preparation method: S1 (Pretreatment): The above natural plant raw material extracts are pulverized to 40 mesh, mixed evenly, and placed in a vacuum drying oven. They are dried at 45°C for 4 hours, and the moisture content of the material is controlled to be reduced to 5.0%.

[0049] S2 (Premix Preparation): Add 18 parts of entrainer and 8 parts of natural antioxidant stabilizer to a melting tank equipped with a nitrogen protection device. Purge the air in the tank with high-purity nitrogen, heat to 50°C, turn on the stirrer, and stir at 200 rpm for 1.5 hours to form a homogeneous and transparent liquid premix. Then add 5 parts of pH buffer adjuster and continue stirring for 20 minutes to ensure uniform dispersion.

[0050] S3 (Supercritical Treatment): The raw material treated in S1 is loaded into a supercritical extraction vessel. The liquid premix obtained in S2 is injected into the top spray system of the extraction vessel by a high-pressure pump to uniformly wet the material. The supercritical carbon dioxide generator is started, and the pressure is controlled at 25 MPa, the temperature at 45℃, the carbon dioxide flow rate at 15 kg / h, and the dynamic treatment time is 3.0 hours.

[0051] S4 (Multi-stage pressure reduction and collection): The effluent enters the multi-stage separation system. First, it is depressurized to 10MPa by the first-stage pressure reducing valve for primary separation, and then depressurized to 0.1MPa (atmospheric pressure) by the second-stage pressure reducing valve for secondary separation. The target component precipitates at the bottom of the separation vessel, and the precipitate is collected.

[0052] S5 (drying): The collected precipitate is transferred to a vacuum belt dryer and dried at 35°C for 2 hours to obtain the final product of the Yijing Guben composition.

[0053] The total extraction yield was 87.2%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 97.8%.

[0054] Example 4 Formula composition: Natural plant extracts (33 parts of ginsenoside enrichment, 19 parts of polygonatum oligosaccharide, and 13 parts of icariin extract): 65 parts; Entrainer (a mixture of natural phosphatidylcholine and modified phytosterol esters in a weight ratio of 1:2): 28 parts; Natural antioxidant stabilizer (a blend of vitamin E acetate and tea polyphenols in a 3:1 weight ratio): 8 parts; pH buffer (sodium citrate and dipotassium hydrogen phosphate mixed in a 1:1 weight ratio): 5 parts.

[0055] Preparation method: S1 (Pretreatment): The above natural plant raw material extracts are pulverized to 80 mesh, mixed evenly, and placed in a vacuum drying oven. They are dried at 60°C for 2 hours to control the moisture content of the material to drop to 8.0%.

[0056] S2 (Premix Preparation): Add 28 parts of entrainer and 8 parts of natural antioxidant stabilizer to a melting tank equipped with a nitrogen protection device. Purge the air in the tank with high-purity nitrogen, heat to 70°C, turn on the stirring device, and stir at 400 rpm for 0.5 hours to form a homogeneous and transparent liquid premix. Then add 5 parts of pH buffer adjuster and continue stirring for 10 minutes to disperse it evenly.

[0057] S3 (Supercritical Treatment): The raw material treated in S1 is loaded into a supercritical extraction vessel. The liquid premix obtained in S2 is injected into the top spray system of the extraction vessel by a high-pressure pump to uniformly wet the material. The supercritical carbon dioxide generator is started, and the pressure is controlled at 40 MPa, the temperature at 65℃, the carbon dioxide flow rate at 30 kg / h, and the dynamic treatment time is 1.5 hours.

[0058] S4 (Multi-stage pressure reduction and collection): The effluent enters the multi-stage separation system. First, it is depressurized to 15MPa by the first-stage pressure reducing valve for primary separation, and then depressurized to 0.1MPa (atmospheric pressure) by the second-stage pressure reducing valve for secondary separation. The target component precipitates at the bottom of the separation vessel, and the precipitate is collected.

[0059] S5 (drying): The collected precipitate is transferred to a vacuum belt dryer and dried at 50°C for 1 hour to obtain the final product of the Yijing Guben composition.

[0060] The total extraction yield was 93.8%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 93.5%.

[0061] Example 5 Based on Example 1, only the weight ratio of vitamin E acetate to tea polyphenols in the natural antioxidant stabilizer was adjusted to 2:1, while the total amount remained unchanged at 8 parts. The rest of the formulation and preparation method were exactly the same as in Example 1.

[0062] Tests showed that the total extraction yield was 91.5%, ethanol residue was <1 ppm, heat-sensitive component retention rate was 95.8%, and POV increase after accelerated aging was 1.3 meq / kg.

[0063] Example 6 Based on Example 1, only the weight ratio of vitamin E acetate to tea polyphenols in the natural antioxidant stabilizer was adjusted to 4:1, while the total amount remained unchanged at 8 parts. The rest of the formulation and preparation method were exactly the same as in Example 1.

[0064] The test results showed that the total extraction yield was 90.8%, the ethanol residue was <1 ppm, the heat-sensitive component retention rate was 96.5%, and the POV increase after accelerated aging was 1.1 meq / kg.

[0065] Example 7 Based on Example 1, only the weight ratio of sodium citrate to dipotassium hydrogen phosphate in the pH buffer was adjusted to 2:1, while the total amount remained unchanged at 5 parts. All other formulations and preparation methods were exactly the same as in Example 1.

[0066] The total extraction yield was 91.2%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 96.0%.

[0067] Example 8 Based on Example 1, only the moisture content of the S1 pretreatment was strictly controlled to be reduced to 3%, and the CO2 flow rate in S3 was increased to 26 kg / h to compensate for the change in mass transfer resistance that may be caused by low moisture content. The rest of the formulation and preparation method are exactly the same as in Example 1.

[0068] The total extraction yield was 89.7%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 95.2%.

[0069] Example 9 Based on Example 1, only the natural plant extract was replaced with 50 parts of ginsenoside enrichment (excluding Polygonatum oligosaccharide and icariin extract), and the rest of the formula and preparation method were exactly the same as in Example 1.

[0070] Tests showed that the ginsenoside extraction yield was 91.0%, the ethanol residue was <1 ppm, and the heat-sensitive component retention rate was 96.2%.

[0071] Example 10 Based on Example 1, only the natural plant extract was replaced with 50 parts of Polygonatum oligosaccharide (excluding ginsenoside enrichment and icariin extract), and the rest of the formula and preparation method were exactly the same as in Example 1.

[0072] Tests showed that the polysaccharide extraction yield of Polygonatum was 90.2%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 95.8%.

[0073] Example 11 Based on Example 1, only the natural plant material extract was replaced with 50 parts of icariin extract (excluding ginsenoside enrichment and polygonatum oligosaccharide), and the rest of the formula and preparation method were exactly the same as in Example 1.

[0074] Tests showed that the icariin extract yield was 89.5%, the ethanol residue was <1 ppm, and the heat-sensitive component retention rate was 95.5%.

[0075] Comparative Example 1 Formula composition: Natural plant extracts (25 parts ginsenoside concentrate, 15 parts polygonatum oligosaccharide, 10 parts icariin extract): 50 parts; Anhydrous ethanol (alternative entrainer): 22 parts; Natural antioxidant stabilizer (a blend of vitamin E acetate and tea polyphenols in a 3:1 weight ratio): 8 parts; pH buffer (sodium citrate and dipotassium hydrogen phosphate mixed in a 1:1 weight ratio): 5 parts.

[0076] Preparation method: S1 (Pretreatment): The above natural plant raw material extracts are pulverized to 60 mesh, mixed evenly, and placed in a vacuum drying oven. They are dried at 55°C for 3 hours to control the moisture content of the material to 6.5%.

[0077] S2 (Premix Preparation): Add 22 parts anhydrous ethanol and 8 parts natural antioxidant stabilizer to a melting tank equipped with a nitrogen protection device. Purge the air in the tank with high-purity nitrogen, heat to 60°C, turn on the stirrer, and stir at 300 rpm for 1.0 hour to form a liquid premix. Then add 5 parts pH buffer adjuster and continue stirring for 15 minutes to disperse it evenly.

[0078] S3 (Supercritical Treatment): The raw material treated in S1 is loaded into a supercritical extraction vessel. The liquid premix obtained in S2 is injected into the top spray system of the extraction vessel by a high-pressure pump to uniformly wet the material. The supercritical carbon dioxide generator is started, and the pressure is controlled at 32 MPa, the temperature at 55℃, the carbon dioxide flow rate at 22 kg / h, and the dynamic treatment time is 2.0 hours.

[0079] S4 (Desolventizing and Collection): Since ethanol cannot spontaneously dissociate, after the effluent enters the separation system, the temperature of the separation vessel needs to be raised to 75°C, and the ethanol needs to be forcibly evaporated and removed under a vacuum of -0.09 MPa for 2 hours before the product can be collected.

[0080] S5 (drying): Transfer the collected product to a vacuum belt dryer and dry at 42°C for 1.5 hours.

[0081] The total extraction yield was 91.3%, the ethanol residue was 2450 ppm, and the retention rate of heat-sensitive components was 86.2%.

[0082] Comparative Example 2 Formula composition: Natural plant extracts (25 parts ginsenoside concentrate, 15 parts polygonatum oligosaccharide, 10 parts icariin extract): 50 parts; No entrainers, antioxidant stabilizers, or pH buffers are added.

[0083] Preparation method: S1 (Pretreatment): The above natural plant raw material extracts are pulverized to 60 mesh, mixed evenly, and placed in a vacuum drying oven. They are dried at 55°C for 3 hours to control the moisture content of the material to 6.5%.

[0084] S2 (Premix Preparation): This step is not performed.

[0085] S3 (Supercritical Treatment): The raw material treated in S1 is loaded into a supercritical extraction vessel, and only supercritical carbon dioxide fluid is introduced. No liquid premix is ​​injected. The pressure is controlled at 32 MPa, the temperature at 55℃, the carbon dioxide flow rate at 22 kg / h, and the dynamic treatment time is 2.0 hours.

[0086] S4 (Collection): Process the effluent into the separation system, reduce the pressure to atmospheric pressure, and collect the precipitate.

[0087] S5 (drying): Transfer the collected precipitate to a vacuum belt dryer and dry at 42°C for 1.5 hours.

[0088] The total extraction yield was 50.5%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 92.0%.

[0089] Comparative Example 3 Based on Example 1, only the entrainer was replaced with 22 parts of natural phosphatidylcholine (without modified phytosterol esters), and the rest of the formulation and preparation method were exactly the same as in Example 1.

[0090] The total extraction yield was 75.8%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 89.5%.

[0091] Comparative Example 4 Formula composition: Same as Example 1.

[0092] Preparation method: S1 (Preprocessing): Same as Example 1.

[0093] S2 (Premix preparation): Same as Example 1.

[0094] S3 (Supercritical Treatment): Controlled pressure 48 MPa, temperature 80℃, carbon dioxide flow rate 22 kg / h, dynamic treatment time 2.0 hours.

[0095] S4 (Rapid Depressurization Collection): The effluent is not subjected to multi-stage depressurization; instead, it is rapidly depressurized directly from the extraction pressure (48 MPa) to atmospheric pressure (0.1 MPa) to collect the precipitate. After collection, the product is vacuum dried at 60°C for 3 hours to remove any adsorbed additives.

[0096] S5 (drying): The collected precipitate is vacuum dried at 60°C for 3 hours.

[0097] The total extraction yield was 83.9%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 78.4%.

[0098] Comparative Example 5 Based on Example 1, only the entrainer was replaced with 22 parts of polysorbate-80 (Tween-80), and a water washing step was added in S4 to remove surfactant residue. The rest of the formulation and preparation method were exactly the same as in Example 1.

[0099] The total extraction yield was 87.3%, Tween-80 residue was 45 ppm, n-hexane residue was 135 ppm, and the retention rate of heat-sensitive components was 84.5%.

[0100] Comparative Example 6 Based on Example 1, only the entrainer was replaced with 22 parts of soybean lecithin and modified phytosterol ester in a weight ratio of 1:2 (excluding natural phosphatidylcholine). The rest of the formulation and preparation method were exactly the same as in Example 1.

[0101] The total extraction yield was 72.3%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 87.2%.

[0102] Comparative Example 7 Based on Example 1, only the entrainer was replaced with a mixture of natural phosphatidylcholine and free phytosterols in a weight ratio of 1:2 (excluding modified phytosterol esters). The rest of the formulation and preparation method were exactly the same as in Example 1.

[0103] The total extraction yield was 73.8%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 86.5%.

[0104] Comparative Example 8 Based on Example 1, only the entrainer was replaced with 22 parts of modified phytosterol ester (without natural phosphatidylcholine), and the rest of the formulation and preparation method were exactly the same as in Example 1.

[0105] The total extraction yield was 67.8%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 88.1%.

[0106] Comparative Example 9 Based on Example 1, only S4 was changed to directly and rapidly depressurize from the extraction pressure (32 MPa) to atmospheric pressure (0.1 MPa) without multi-stage depressurization. The rest of the formulation and preparation method were exactly the same as in Example 1.

[0107] The total extraction yield was 84.6%, the ethanol residue was <1 ppm, and the retention rate of heat-sensitive components was 89.7%.

[0108] Performance testing Test 1: Determination of Extraction Yield and Solvent Residue Experimental methods: (1) Sample pretreatment: Accurately weigh 1.0 g of the finished product of each example and comparative example, place it in a 50 mL volumetric flask, add methanol-water (70:30, v / v) solution and ultrasonically extract for 30 minutes, then filter through a 0.22 μm filter membrane after adjusting the volume, and wait for testing.

[0109] (2) Determination of extraction yield: High performance liquid chromatography (HPLC) was used. The chromatographic column was a C18 column (250 mm × 4.6 mm, 5 μm), the mobile phase was acetonitrile-water gradient elution, the flow rate was 1.0 mL / min, and the detection wavelength was 203 nm. The contents of ginsenosides (total of Rg1, Re, and Rb1), Polygonatum oligosaccharides, and icariin were calculated by external standard method, and the extraction yield (%) was calculated in combination with the initial contents of the raw materials.

[0110] (3) Solvent residue determination: Headspace gas chromatography (HS-GC) was used, with a headspace heating temperature of 80℃, an equilibration time of 20 minutes, a DB-624 capillary column, and an FID detector. The residual amounts of ethanol and other volatile organic compounds (ppm) were calculated.

[0111] The test data for the embodiments and comparative examples are shown in Table 2.

[0112] Table 2 Note: ND indicates not detected, and the detection limit is 1 ppm.

[0113] Test 2: Retention rate and oxidative stability of heat-sensitive active ingredients Experimental methods: (1) Determination of retention rate of thermosensitive components: The enthalpy change value of characteristic endothermic peaks in each sample is analyzed by differential scanning calorimetry (DSC). The DSC thermograms of raw materials and finished products are overlaid and compared. The retention rate is calculated by the sum of the enthalpy changes of all characteristic endothermic peaks, i.e., retention rate = (sum of enthalpy changes of all characteristic endothermic peaks in the DSC thermogram of finished product / sum of enthalpy changes of all characteristic endothermic peaks in the DSC thermogram of raw materials) × 100%.

[0114] (2) Accelerated oxidation stability test: Each sample was placed in a constant temperature and humidity test chamber, with a temperature of 45±1℃ and a relative humidity of 75±5%, and placed continuously for 30 days.

[0115] (3) Peroxide value and color determination: Before and after accelerated aging, the peroxide value (POV) was determined according to the first method of GB 5009.227, and the change of L*a*b* color value was determined. The increase in POV and color difference ΔE were calculated.

[0116] The test data for the embodiments and comparative examples are shown in Table 3.

[0117] Table 3 This invention provides a nourishing and strengthening composition containing natural plant sources and its preparation method. Addressing the technical contradiction of excessive solvent residue and degradation of heat-sensitive components caused by ethanol entrainers during supercritical CO2 extraction of moderately polar active ingredients, and the sharp drop in extraction rate without entrainers, this invention provides a solution: The natural plant extract is mixed with an entrainer composed of natural phosphatidylcholine and modified phytosterol esters, and treated under supercritical CO2 conditions of 25-40 MPa and 45-65℃, followed by multi-stage depressurization to atmospheric pressure to collect the precipitate. This method utilizes the solubilization properties of the entrainer under high pressure and its spontaneous dissociation after depressurization, achieving a balance between high extraction rate and zero residue. Examples show that the target component extraction yield is ≥88%, ethanol residue is <1 ppm, and the retention rate of heat-sensitive components is ≥94%. This invention combines high efficiency, greenness, and safety, and has promising prospects for industrial application.

[0118] In some embodiments, the natural plant extracts mentioned in step (1) are selected from one or more of ginsenoside enrichment, polygonatum oligosaccharide, icariin extract, maca extract, cistanche extract, and yam extract.

[0119] The composition prepared by the method of this invention can be used as an active ingredient in health foods, functional foods, or dietary supplements. The composition features high content of active ingredients, no organic solvent residue, and complete retention of heat-sensitive components, making it particularly suitable for the preparation of oral health products with high requirements for product purity and safety.

[0120] The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention. Any modifications, equivalent substitutions, and improvements made within the spirit and principles of the present invention should be included within the protection scope of the present invention.

Claims

1. A method for preparing a composition containing natural plant sources that benefits essence and strengthens the body, characterized in that, Includes the following steps: (1) Mix 40-65 parts by weight of natural plant raw material extract with 15-30 parts by weight of entrainer to form a premix; the entrainer is a compound of natural phosphatidylcholine and modified phytosterol ester in a weight ratio of 1:1.5-1:

3. (2) Supercritical treatment was carried out in supercritical carbon dioxide fluid at 25-40 MPa and 45-65℃. (3) The effluent from step (2) is gradually depressurized to atmospheric pressure, the precipitate is collected and dried to obtain the composition.

2. The preparation method according to claim 1, characterized in that, In the entrainer, the weight ratio of natural phosphatidylcholine to modified phytosterol ester is 1:1.8-1:2.

5.

3. The preparation method according to claim 1, characterized in that, The natural plant extracts mentioned in step (1) are selected from one or more of the following: ginsenoside enrichment, polygonatum oligosaccharide, icariin extract, maca extract, cistanche extract, and yam extract.

4. The preparation method according to claim 1, characterized in that, The premix described in step (1) also contains 5-12 parts by weight of a natural antioxidant stabilizer and 3-8 parts by weight of a pH buffer regulator.

5. The preparation method according to claim 4, characterized in that, The natural antioxidant stabilizer is a compound of vitamin E acetate and tea polyphenols in a weight ratio of 2:1-4:1; the pH buffer adjuster is a mixture of sodium citrate and dipotassium hydrogen phosphate in a weight ratio of 1:1-2:

1.

6. The preparation method according to claim 1, characterized in that, Before step (1), the process also includes: crushing the natural plant material to 40-80 mesh and vacuum drying it at 45-60℃ to a moisture content of 5%-8%.

7. The preparation method according to claim 1, characterized in that, In step (1), the mixing operation is to stir and melt at 50-70℃ under nitrogen protection for 0.5-1.5 hours, and the stirring speed is controlled at 200-400 rpm.

8. The preparation method according to claim 1, characterized in that, In step (2), the carbon dioxide flow rate is 15-30 kg / h and the treatment time is 1.5-3.0 hours.

9. The preparation method according to claim 1, characterized in that, In step (3), the pressure is first reduced to 10-15 MPa for primary separation, and then reduced to 0.1 MPa for secondary separation.

10. A composition containing natural plant extracts for strengthening essence and consolidating the body, characterized in that, Prepared by the method described in any one of claims 1-9.

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