Method for obtaining effective components of citrus combined medicinal material by integrating supercritical CO2 extraction and microcapsule technology

Abstract

The invention relates to a method for integrating supercritical CO2 extraction (SCE) and a microcapsule technology to be applied to citrus combined medicinal materials, the effective component is essential oil, three factors including pressure (P), temperature (T) and time (t) are optimized, and then microencapsulation is carried out. The extracted essential oil contains a plurality of pharmacological active ingredients and has a unique fragrant smell. According to the essential oil extraction optimization process of the combined medicinal material, a fitted equation with a very high correlation coefficient is obtained through optimization fitting of a total extraction rate equation, and the essential oil extraction optimization process of the combined medicinal material has a great promotion effect on essential oil extraction of the citrus combined medicinal material in a Chinese patent medicine or health-care product preparation process. The extracted essential oil of the citrus combined medicinal material can be wrapped in a multi-layer structure through a microencapsulation process, and component volatilization and oxidation are prevented.

Description

Technical Field

[0001] The present invention belongs to the field of preparation technology of Chinese patent medicine or health care products, and specifically, relates to a method for obtaining effective ingredients of citrus combination medicinal materials by integrating supercritical CO2 extraction and microencapsulation technology. Background Art

[0002] Chinese herbal compound is the main means of clinical drug treatment in traditional Chinese medicine. It is established according to the theory of "principle, method, prescription and medicine" of traditional Chinese medicine, and is composed according to the structure of "monarch, minister, assistant and envoy". In form, it is a combination of medicinal flavors. Its basic unit "drug pair" is a combination of two medicinal materials, which can affect the efficacy by synergizing, antagonizing or regulating the drug metabolism process. At present, some citrus medicinal materials are often used in combination in various Chinese herbal prescriptions to improve people's health level, such as "Chenpi-Zhiqi" drug pair. In addition, many other citrus medicinal materials are also added to Chinese herbal prescriptions for other reasons to exert synergistic or antagonistic effects, such as Zhishi and Qingpi. These citrus medicinal materials have multiple pharmacological activities and present a unique citrus fragrance. Therefore, in the preparation process of Chinese patent medicine, how to extract the effective components of two or more mixed citrus medicinal materials to the greatest extent and retain their fragrance characteristics is a scientific issue worthy of in-depth study. This will inevitably involve multiple preparation process links of citrus medicinal materials.

[0003] At present, maceration, decoction, reflux extraction and steam extraction are the traditional methods for extracting the components of citrus combination medicinal materials such as "Chenpi-Zhiqi", which have the disadvantages of long production cycle and easy thermal damage of components. Supercritical CO2 extraction (SCE) is a new environmentally friendly extraction method. Low temperature is conducive to retaining the unique aroma components, heat-sensitive substances and easily oxidized components in the combination of citrus medicinal materials. There are many factors that affect SCE, including pressure (P), temperature (T) and time (t). In order to explore the influence of the interaction effect between various factors on the extraction rate, it is necessary to design and model multi-factor multi-level schemes through response surface methodology (RSM), and chemometric methods are needed to optimize experimental parameters. Through RSM analysis, the influence of a single factor on a certain extraction index can be obtained, and the interaction between different factors can also be obtained. At present, process research often takes a certain citrus medicinal material (food) as the object, but less related methodological exploration is carried out on common drug pairs or more drug mixtures in traditional Chinese medicine compound. Yang et al. have conducted SCE extraction studies on Pueraria root, Pinus massoniana needles, citrus peels and their mixture "Compound Songkudzu Uric Acid Lowering Powder". It is worth mentioning that RSM should be further explored around the total extraction rate index to obtain the optimal parameters for SCE extraction of multiple components of citrus combined medicinal materials.

[0004] Through the above RSM modeling and optimization, SCE high-yield products of citrus combination medicinal materials such as "Chenpi-Zhiqi" can be obtained. These SCE extracts generally contain fatty acids, sterols and active ingredients, and also contain terpenoids (monoterpenes, sesquiterpenes, etc.) that can release unique fragrances. It is worth mentioning that these components are often volatile and easily oxidized, which is an important factor in the preparation process of traditional Chinese medicine. At present, there are a large number of literatures involving the microencapsulation of plant essential oils to achieve the purpose of component protection or slow release of fragrance. In addition, the microencapsulation of fat-soluble flavonoids and other multi-components of SCE products is of great significance to the modernization of traditional Chinese medicine. In short, the microencapsulation process can protect the core material from the influence of the surrounding environment and achieve long-lasting release performance. At present, β-cyclodextrin (β-CD) is commonly used in industry as a wall material, and microcapsule samples of plant essential oils are prepared by saturated aqueous solution method. Gao et al. suggested the preparation of consumer-friendly essential oil microcapsules with a viscous core structure to achieve ultra-long-term release performance. Hashim et al. observed that the stability, antioxidant and antibacterial properties of cinnamon essential oil core materials were significantly enhanced by encapsulation with various wall materials. Therefore, SCE products of citrus combination medicinal materials such as "Chenpi-Zhiqi" should also use various types of microencapsulation processes to protect active ingredients and be used in the preparation process of traditional Chinese medicine or health products. Summary of the invention

[0005] The purpose of the present invention is to overcome the shortcomings of the existing Chinese medicine preparation process and provide a method for extracting the effective ingredients in the citrus combination medicinal materials with supercritical CO2 fluid and preparing microcapsule preparations. The present invention can retain the aroma and active ingredients in the citrus combination medicinal materials to the greatest extent by adopting the process.

[0006] In a first aspect, the present invention provides a method for obtaining effective ingredients of citrus medicinal materials by supercritical CO2 extraction (SCE):

[0007] The composition of SCE extracted medicinal materials is:

[0008] ① “Chenpi-Zhiqi”; or

[0009] ② Add other citrus herbs to the above ①; or

[0010] ③ A combination of various other citrus medicinal materials;

[0011] The preparation process is as follows:

[0012] (1) Material preparation: crushing, sieving and mixing the raw material components;

[0013] (2) Extraction: Using supercritical extraction equipment, the mixed medicinal powder is placed in a high-pressure extraction kettle, and liquid CO2 is used to extract the essential oil, which is the extract.

[0014] Preferably, the weight ratio of ① "tangerine peel-citrus aurantium" is 1:2-2:1, and more preferably 4:3 or 1:1.

[0015] Preferably, the (1) material preparation is as follows: drying the raw material components in a 40° C. air dryer for 5 hours, crushing and sieving, taking the sieved material, and mixing the particles according to the required proportion.

[0016] Preferably, the (2) extraction: using a supercritical extraction device, the mixed medicinal powder is loaded into a high-pressure extraction kettle, and the essential oil is extracted with liquid CO2, the extraction temperature is: 40-60°C, the extraction pressure is: 200-500bar, the extraction time is 1-2 hours, the extract enters the separator for decompression separation, and is completely separated from the gaseous CO2, and the essential oil flowing out of the separator is collected, which is the extract.

[0017] In a second aspect, the present invention provides a product prepared by the above method, wherein the extract contains components such as fat-soluble flavonoids, fatty acids and sterols.

[0018] The present invention provides a product prepared by the above method in a third aspect, wherein the extract contains aromatic terpenoid components.

[0019] In a fourth aspect, the present invention provides a method for obtaining effective components of a citrus medicinal material by integrating supercritical CO2 extraction (SCE) and microencapsulation technology. The composition of the SCE extracted medicinal material is:

[0020] ① “Chenpi-Zhiqi”; or

[0021] ② Add other citrus herbs to the above ①; or

[0022] ③ A combination of various other citrus medicinal materials;

[0023] The core composition of the microcapsule is:

[0024] ① SCE extract of a combination of citrus herbs; or

[0025] ② The above ①, adding other medicinal extracts in Chinese patent medicine products;

[0026] The preparation process is as follows:

[0027] (1) Material preparation: crushing, sieving and mixing the raw material components;

[0028] (2) Extraction: Using a supercritical extraction device, the mixed medicinal material powder is placed in a high-pressure extraction kettle and the essential oil is extracted using liquid CO2;

[0029] (3) Microcapsules: Microencapsulation is carried out by complex coacervation, saturated aqueous solution, spray drying or other methods.

[0030] Preferably, the weight ratio of ① "tangerine peel-citrus aurantium" is 1:2-2:1, and more preferably 4:3 or 1:1.

[0031] Preferably, the (1) material preparation is as follows: drying the raw material components in a 40° C. air dryer for 5 hours, crushing and sieving, taking the sieved material, and mixing the particles according to the required proportion.

[0032] Preferably, the (2) extraction: using a supercritical extraction device, the mixed medicinal powder is loaded into a high-pressure extraction kettle, and the essential oil is extracted with liquid CO2, the extraction temperature is: 40-60°C, the extraction pressure is: 200-500bar, the extraction time is 1-2 hours, the extract enters the separator for decompression separation, and is completely separated from the gaseous CO2, and the essential oil flowing out of the separator is collected, which is the extract.

[0033] In a fifth aspect, the present invention provides a product prepared by the above-mentioned method of integrating supercritical CO2 extraction and microencapsulation technology to obtain the effective ingredients of citrus combination medicinal materials.

[0034] Preferably, the product is essential oil microcapsule.

[0035] In a sixth aspect, the present invention provides the use of a product prepared by the above-mentioned method of integrating supercritical CO2 extraction and microencapsulation technology to obtain effective ingredients of citrus combination medicinal materials, which is used for Chinese patent medicines or health care products.

[0036] Beneficial effects of the present invention:

[0037] Compared with the prior art, the optimal process for obtaining the citrus combined medicinal material components provided by the present invention has the following beneficial effects:

[0038] First, using citrus combination medicinal materials such as "tangerine peel-citrus aurantium" as raw materials, active ingredients such as fat-soluble flavonoids, fatty acids and sterols can be obtained under the extraction process conditions provided by the present invention, and the highest total extraction rate can be obtained.

[0039] Second, the extracted essential oils of citrus medicinal materials such as "tangerine peel-citrus aurantium" have volatile terpene components and a unique fragrance. The whole process is simple, easy to operate, and non-toxic to the human body.

[0040] Third, the extracted essential oil components of citrus medicinal materials such as "tangerine peel-citrus aurantium" can be encapsulated in a multi-layer structure through microencapsulation technology to prevent the volatilization and oxidation of the components. BRIEF DESCRIPTION OF THE DRAWINGS

[0041] Figure 1 Analysis of supercritical CO2 extraction parameters of dried tangerine peel and bitter orange peel based on the total extraction rate: (a) single factor analysis; (b) multi-factor interaction.

[0042] Figure 2 Optimization was performed to determine the optimal supercritical CO2 extraction parameters using PSO, GWO and ACGWO.

[0043] Figure 3 Components of the supercritical CO2 extraction product from "Chenpi-Zhiqi": (a) terpenes, which contribute to the aroma characteristics; (b) lipophilic flavonoids with potential health benefits; (c) fatty acids; (d) sterol components with various functions.

[0044] Figure 4 Aromatic characteristics of the supercritical CO2 extraction products of "Chenpi-Zhiqi": (a) quantitative descriptive analysis results; (b) electronic nose data showing different odor characteristics.

[0045] Figure 5 The complex coacervation microencapsulation process of the supercritical CO2 extraction product of "Chenpi-Zhiqi": (a) flow chart; (b) microscope observation at different magnifications; (c) UV spectrum analysis and particle size test of microcapsules.

[0046] Figure 6 The Fourier transform infrared characteristic spectra of the microcapsules formed by spray drying of the compound Chinese herbal volatile oil containing "Chenpi-Zhiqi" supercritical CO2 extract: (a) spray drying of a mixture of gum arabic and maltodextrin; (b) compound Chinese herbal essential oil; (c) spray drying of a mixture of gum arabic, maltodextrin and compound Chinese herbal essential oil.

[0047] Figure 7 Electron micrograph of microcapsules formed after spray drying of the compound Chinese herbal volatile oil containing supercritical CO2 extract of "Chenpi-Zhiqi". DETAILED DESCRIPTION

[0048] The present invention will be further described below in conjunction with specific examples. It should be understood that these examples are only used to illustrate the present invention and are not intended to limit the scope of the present invention. The experimental methods in the following examples without specifying specific conditions are usually based on conventional conditions or the conditions recommended by the manufacturer. Unless otherwise stated, all percentages, ratios, proportions or parts are by weight.

[0049] Unless otherwise defined, all professional and scientific terms used herein have the same meanings as those familiar to those skilled in the art. In addition, any methods and materials similar or equivalent to those described herein can be applied to the methods of the present invention. The preferred implementation methods and materials described herein are for demonstration purposes only.

[0050] Example 1 Integrating supercritical CO2 extraction and microencapsulation technology to obtain the active ingredients of "Chenpi-Fructus Aurantii Immaturus"

[0051] (1) Optimization experimental design of supercritical CO2 extraction of active ingredients from dried tangerine peel and fructus aurantii based on total extraction rate

[0052] The response surface methodology was used to analyze the effects of three factors (extraction pressure, extraction temperature and particle size) on the total extraction yield (Y), while other variables were fixed values, such as carbon dioxide flow rate and medicinal powder weight. In order to reduce the number of experiments and reduce costs, this experiment used the small facet central composite design (SFCCD) to design the experimental scheme. As shown in Table 1, the experiment was carried out according to the 15 groups of operating parameters recommended by SFCCD, and the respective total extraction rates were obtained. The experimental results used the analysis of variance (AOV) method to analyze the mutual influence of the three independent variables and EY, and the F-value test method and P-value were used to analyze the statistical significance of each coefficient on the response value. The nonlinear fitting method was used to establish a quadratic polynomial regression fitting equation, and this statistical model was used to predict the highest yield.

[0053] Table 1 Pressure, temperature, extraction time and total extraction rate in each experimental extraction kettle

[0054]

[0055] (2) Single factor analysis of supercritical CO2 extraction of dried tangerine peel and fructus aurantii

[0056] exist Figure 1 In (a), we can see the impact of the three factors T, P and t on different scenarios:

[0057] ① As P increases, Y also increases, indicating that high pressure is conducive to the improvement of Y.

[0058] ② As T increases, Y increases first, but when it reaches a certain temperature, Y no longer increases. The above shows that setting the temperature too high or too low is not conducive to extraction.

[0059] ③With the increase of t, Y first increases rapidly and reaches the highest at 95 minutes. If t is further increased, Y will no longer increase and may even decrease, indicating that the optimal extraction time is 95 minutes.

[0060] (3) Analysis of the interaction between two factors in supercritical CO2 extraction of dried tangerine peel and fructus aurantii

[0061] The response surface and contour plots of RSM can analyze the interaction between multiple factors. The steeper the response surface, the more significant the impact of the interaction between the two factors on the response value, and the more irregular or dense the contour lines, the more significant the interaction between the two factors.

[0062] from Figure 1b(i) shows that: on the one hand, the surface of P is steeper than that of T, indicating that P has a more significant effect on Y, and the response surface generated by the two factors is steeper overall, indicating that the interaction between the two factors is strong. On the other hand, the contour map is denser, indicating that the interaction between P and T is strong and has a greater impact on Y, and the contour lines along the P direction are denser than the contour lines along the T direction, indicating that the effect of P on Y is more significant than that of T.

[0063] from Figure 1 b(ii) shows that: on the one hand, the surface of P is not as steep as that of t, indicating that t has a more significant effect on Y, and the response surface generated by the two factors is relatively flat, indicating that the interaction between the two factors is weak. On the other hand, the contour map is sparse, indicating that the interaction between P and t is weak and the impact on Y is not too large, and the contour lines along the t direction are denser than the contour lines along the P direction, indicating that the impact of t on Y is more significant than that of P.

[0064] from Figure 1 b(iii) shows that: on the one hand, the surface of T is not steeper than that of t, indicating that t has a more significant effect on Y, and the response surface generated by the two factors is very steep, indicating that the interaction between the two factors is very strong. On the other hand, the contour map is very dense, indicating that t and T interact strongly and have a significant effect on Y, and the contour lines along the t direction are denser than the contour lines along the P direction, indicating that the effect of t on Y is more significant than that of T.

[0065] In summary, the significance of the interaction among the three factors is BC>AB>AC.

[0066] (4) Optimization results of supercritical CO2 extraction model of “Chenpi-Fructus Aurantii Immaturus”

[0067] After establishing the SCE response surface model, the optimal experimental conditions were obtained through the model optimization program: A = 400 bar (P), B = 48.3 ° C (T), C = 87.4 min (t), and the extraction yield response value was Y = 2.14%. The researchers also selected particle swarm optimization (PSO), gray wolf optimization algorithm (GWO), and improved gray wolf optimization algorithm (ACGWO) from other optimization algorithms to obtain the optimal value. Figure 2It can be observed that the maximum yield of the optimized PSO algorithm is 2.04%, while the best values ​​of GWO and ACGWO are both 2.14%. The results of the PSO algorithm are not ideal, which is due to the small size of the group and less collaborative search. The GWO and ACGWO algorithms are more flexible, and the group size has fewer restrictions on them, so their optimization effect is good. It can also be seen that ACGWO has a faster reaction speed than GWO, and can approach prey faster and capture it. Compared with Design-Expert, the above two algorithms have higher accuracy, and the final optimal value is 2.14%, and the corresponding operating parameters are 400bar (P), 48.0℃ (T) and 87.0min (t).

[0068] (5) Analysis of ingredients in the SCE product “Chenpi-Zhiqi”

[0069] The SCE products of citrus combination medicinal materials such as "Chenpi-Zhiqi" are very complex samples, containing components such as volatile terpenes, fat-soluble flavonoids and fatty acids. First, after mass spectrometry similarity search and retention index matching, the GC-MS fingerprint peaks were annotated as volatile components such as D-Limonene, γ-Terpinene, o-Cymene, α-Terpineol and Terpinolene. Secondly, after non-targeted LC-MS analysis, the sample mainly contained fat-soluble components such as Nobiletin, Tangeretin and Isomeranzin. Thirdly, the sample was methylated and analyzed by GC-MS, and it was confirmed that it contained oil components such as 16:0, 18:2 and 18:3. In addition, the sample also contains β-sitosterol, which has a wide range of biological activities. Such as Figure 3 As shown in the figure, these complex components together constitute the material system of the "Chenpi-Zhiqi" SCE product, each of which exerts different material properties or pharmacological activities. Among them, Nobiletin has anti-hemagglutination, anti-thrombosis, anti-cancer, anti-fungal, anti-inflammatory, anti-allergic, anti-cholinesterase and anti-epileptic effects. β-Sitosterol has the effects of lowering cholesterol, relieving cough, removing phlegm, inhibiting tumors and repairing tissues.

[0070] (6) Description of the aroma characteristics of the supercritical CO2 extract of “Chenpi-Zhiqi”

[0071] Seven professional perfumers described the aroma characteristics of supercritical CO2 extracts. Figure 4As shown in (a), fruity aroma (7.1), green aroma (3.6), spicy aroma (2.7), sweet aroma (2.9), fresh aroma (2.6) and floral aroma (0.7) occupy the main body of the olfactory style characteristics. The SCE product of "Chenpi-Zhiqi" was also tested by the SmartNose electronic nose, and compared with the separate SCE products of the two medicinal materials. The SmartNose electronic nose uses a gas chromatography injection method, an external air compression pump and a three-stage filtration system to provide clean cleaning gas; the built-in electronically controlled six-way valve and quantitative loop ensure the quantitative delivery of the sample gas. In the signal spectrum, the 14 odor sensors of the electronic nose all responded well to the three SPE extracts. Then, the researchers extracted the eigenvalues ​​from the original response signal for the next PCA analysis. Component 1 (PC1) contains the most information provided by the original variables, and component 2 (PC2) explains most of the information provided by the original variables not explained by PC1. As shown Figure 4 As shown in (b), each point represents each parallel experiment of the SPE extract of this category, and the clusters formed by different points represent a type of sample; the distance in the figure represents the difference in the overall odor quality of the SPE extract. It can be seen from the figure that the DI value (88.29) is large, and there is a large odor difference among the three samples, and the differentiation effect is ideal. In short, the SCE product of "Chenpi-Zhiqi" has a unique odor fragrance.

[0072] (7) Complex coacervation microencapsulation of “Chenpi-Fructus Aurantii Immaturus” SCE product

[0073] like Figure 5 As shown in the complex coagulation flow chart (a), the SCE product of "Chenpi-Zhiqi" has been subjected to emulsification, coagulation, cross-linking, filtration and drying, and the obtained microcapsules can protect the volatile or oxidizable components. Figure 5 In (b1), the researchers used a Motic microscope to observe the emulsion and its diluted solution. The droplets are usually round or oval; the droplets have clear edges and regular shapes; the droplets vary in size, generally in the micrometer range; the droplets are evenly distributed and do not merge with each other. Figure 5 (b2) shows that the microcapsule product (×250) usually presents a regular spherical or nearly spherical shape, with a smooth surface and clear edges; the microcapsules are relatively evenly distributed in the aqueous phase, with different sizes but regular shapes. The shell structure is visible at a larger magnification (×1000), and the structure is uniform and continuous, without obvious defects or cracks. In addition, the shell and the core have different refractive indices, resulting in different colors or brightness under microscopy. The microcapsule can be divided into three layers: the inner layer is the oily capsule core; the middle layer is the shell layer condensed by chitosan and sodium alginate; the outer layer is further hardened and stabilized by glutaraldehyde cross-linking. In summary, the stability of the emulsion and the multilayer structure of the SCE product microcapsules were verified by microscopic observation and analysis at different magnifications.

[0074] like Figure 5 (c1), the researchers further conducted UV spectroscopy analysis on the microcapsule encapsulated components. Among them, i is the UV spectrum of SCE extract (anhydrous ethanol solution); ii is the UV spectrum of blank microcapsules (anhydrous ethanol solution); iii is the UV spectrum of emulsion (anhydrous ethanol solution); iv is the UV spectrum of extract microcapsule product (after washing the surface, ultrasonic crushing with anhydrous ethanol). The results show that compared with the blank microcapsules, SCE extract, SCE product emulsion and SCE product microcapsules all have strong characteristic peaks at 325nm. This phenomenon also indirectly shows that the SCE component of "Chenpi-Zhiqi" has been encapsulated inside the microcapsules.

[0075] like Figure 5 (c2), the researchers further used laser diffraction to test the particle size of the microcapsule product. From this figure, it can be inferred that the particle size of most microcapsules is concentrated in the range of 0.479um-138.038um, and the D50 (median particle size) is 34.346um. Through particle size analysis, the particle size of the microcapsules prepared by this complex coacervation method for SCE products meets the standard.

[0076] Example 2 Process for preparing a Chinese patent medicine preparation containing a combination of citrus medicinal materials by integrating supercritical CO2 extraction and microencapsulation technology

[0077] Take the compound prescription "Bupleurum Liver-Soothing Powder" as an example to explain:

[0078] (1) Extraction of active ingredients from dried orange peel and Citrus aurantium by supercritical CO2

[0079] As shown in Example 1, a supercritical CO2 extract of "Citrus Aurantium and Citrus aurantium" was prepared.

[0080] According to the composition of the compound medicinal materials, the next capsule core is composed of the supercritical CO2 extract of "tangerine peel-citrus aurantium" and other medicinal essential oils.

[0081] (2) Preparation of compound Chinese medicine essential oil microcapsules containing "Chenpi-Fructus Aurantii Immaturus" (spray drying method)

[0082] Weigh 20g of gum arabic and maltodextrin (1:1) and add them to a beaker, add 200ml of water at the same time, stir at 60℃ for 40min, put into a 4℃ refrigerator overnight to ensure complete hydration, add 4ml of essential oil mixture (including: supercritical CO2 extract of "Chenpi-Fructus Aurantii Immaturus", various schemes of extracting essential oils from other medicinal materials) and 2ml of Span 80 to the hydrated liquid, put into a high-speed homogenizer and stir for 10min at 10000rpm, put into an ultrasonic homogenizer and stir for 5 minutes at a frequency of 5s / 5s after stirring to obtain an emulsion (the two homogenizations are because the supercritical extraction of volatile oil has poor solubility), and put the emulsions into a spray dryer for drying, and the spray dryer conditions (air inlet temperature 160℃, air outlet temperature 80℃, creep speed 5%, wind speed 90%) to obtain a microcapsule product.

[0083] Figure 6 The following are Fourier infrared characteristic spectra. Curve a is the infrared curve of the mixture of gum arabic and maltodextrin after spray drying, curve b is the infrared curve of the volatile oil of common Chinese medicine compound ("Chenpi-Fructus Aurantii Immaturus" and "Chuanxiong-Cyperus Rhizoma"), and curve c is the infrared curve of the mixture of gum arabic, maltodextrin and compound Chinese patent medicine essential oil after spray drying. It can be seen from the figure that both curves b and c have 2342.7cm -1 Characteristic absorption peaks. In addition, a, b and c are at 2925.4cm -1 Both have CH asymmetric absorption peaks, but only b has 2851.3 cm -1 CH symmetrical absorption peak. Through the above infrared analysis, it can be seen that the infrared spectra of b and c are similar.

[0084] Figure 7 This is an electron microscope image. Through the electron microscope, it can be seen that the microcapsules are approximately spherical and unevenly distributed in size. Further zooming in, it can be found that there is an oily substance inside a single microcapsule, and the outer shell appears as a shadow under the microscope. Through the electron microscope, it can be intuitively seen that the combined volatile oil of the mixed medicinal materials is embedded in the microcapsule through spray drying.

[0085] (3) The compound Chinese medicine essential oil microcapsules prepared in (2) or by other methods are mixed with other compound medicinal material extracts to prepare a Chinese patent medicine preparation.

[0086] The above description is only a preferred embodiment of the present invention and is not intended to limit the scope of the substantial technical content of the present invention. The substantial technical content of the present invention is broadly defined in the scope of the claims of the application. Any technical entity or method completed by others, if it is exactly the same as that defined in the scope of the claims of the application or an equivalent variation, will be deemed to be included in the scope of the claims.

Claims

1. A method for obtaining effective ingredients from a combination of citrus medicinal materials by supercritical CO2 extraction (SCE), characterized in that: The composition of SCE extracted medicinal materials is: ① "Chenpi-Zhiqi"; or ② Add other citrus herbs to the above ①; or ③ A combination of various other citrus medicinal materials; The preparation process is as follows: (1) Material preparation: crushing, sieving and mixing the raw material components; (2) Extraction: Using supercritical extraction equipment, the mixed medicinal powder is placed in a high-pressure extraction kettle, and liquid CO2 is used to extract the essential oil, which is the extract.

2. The method according to claim 1, characterized in that: The weight ratio of ① "tangerine peel-citrus aurantium" is 1:2-2:1, preferably 4:3 or 1:

1.

3. The method according to claim 1, characterized in that: (1) Material preparation: drying the raw material components in a 40° C. air dryer for 5 hours, crushing and sieving, taking the sieved material, and mixing the particles according to the required proportion.

4. The method according to claim 1, characterized in that: The (2) extraction: using a supercritical extraction device, the mixed medicinal powder is loaded into a high-pressure extraction kettle, and the essential oil is extracted with liquid CO2, the extraction temperature is: 40-60°C, the extraction pressure is: 200-500bar, the extraction time is: 1-2 hours, the extract enters the separator and is decompressed and separated, and is completely separated from the gaseous CO2, and the essential oil flowing out of the separator is collected, which is the extract.

5. The product prepared by the method according to any one of claims 1 to 4, characterized in that: The extract contains medicinal ingredients such as fat-soluble flavonoids, fatty acids and sterols.

6. The product prepared by the method according to any one of claims 1 to 4, characterized in that: The extract contains aromatic terpenoid components.

7. A method for obtaining effective ingredients from a combination of citrus medicinal materials by integrating supercritical CO2 extraction (SCE) and microencapsulation technology, characterized in that: The composition of SCE extracted medicinal materials is: ① "Chenpi-Zhiqi"; or ② Add other citrus herbs to the above ①; or ③ A combination of various other citrus medicinal materials; The core composition of the microcapsule is: ① SCE extract of a combination of citrus herbs; or ② The above ①, adding other medicinal extracts in Chinese patent medicine products; The preparation process is as follows: (1) Material preparation: crushing, sieving and mixing the raw material components; (2) Extraction: Using a supercritical extraction device, the mixed medicinal material powder is placed in a high-pressure extraction kettle and the essential oil is extracted using liquid CO2; (3) Microcapsules: Microencapsulation is carried out by complex coacervation, saturated aqueous solution, spray drying or other methods.

8. The method according to claim 7, characterized in that: The weight ratio of ① "tangerine peel-citrus aurantium" is 1:2-2:1, preferably 4:3 or 1:

1.

9. The method according to claim 7, characterized in that: (1) Material preparation: drying the raw material components in a 40° C. air dryer for 5 hours, crushing and sieving, taking the sieved material, and mixing the particles according to the required proportion.

10. The method according to claim 7, characterized in that: The (2) extraction: using a supercritical extraction device, the mixed medicinal powder is loaded into a high-pressure extraction kettle, and the essential oil is extracted with liquid CO2, the extraction temperature is: 40-60°C, the extraction pressure is: 200-500bar, the extraction time is: 1-2 hours, the extract enters the separator and is decompressed and separated, and is completely separated from the gaseous CO2, and the essential oil flowing out of the separator is collected, which is the extract.

11. A product prepared according to the method for obtaining effective ingredients of citrus medicinal materials by integrating supercritical CO2 extraction and microencapsulation technology according to any one of claims 7 to 10.

12. The product according to claim 11, which is an essential oil microcapsule.

13. Use of a product prepared by the method for obtaining effective ingredients of citrus medicinal materials by integrating supercritical CO2 extraction and microencapsulation technology as described in any one of claims 7 to 11, which is used in Chinese patent medicines or health care products.

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