Traditional Chinese medicine subcritical pure water extraction method and application thereof

Abstract

This invention relates to the field of traditional Chinese medicine (TCM) extraction technology, and discloses a subcritical pure water extraction method for TCM and its application. The subcritical pure water extraction method provided by this invention uses water as the sole extraction medium, deeply integrating subcritical extraction technology with pure water extraction processes. By optimizing key steps such as material pretreatment, core subcritical extraction parameters, and subsequent separation and purification, a systematic subcritical pure water extraction system is formed, achieving efficient enrichment of the effective components of TCM. This process is highly safe, effectively eliminating the generation of organic pollutants at the source, significantly improving the extraction rate and purity of effective components, and greatly shortening the extraction time.

Description

Technical Field

[0001] This invention relates to the field of traditional Chinese medicine extraction technology, specifically to a subcritical pure water extraction method for traditional Chinese medicine and its application. Background Technology

[0002] Extraction of active ingredients from traditional Chinese medicine (TCM) is a core and crucial step in the industrial production of TCM preparations. Currently, the industry mainly uses organic solvent extraction, commonly employing alcohols, alkanes, and esters as extraction media. Some processes also incorporate subcritical extraction technology, but organic solvents remain the core extraction medium. However, organic solvents are volatile and toxic, easily generating harmful waste gases and highly polluting organic waste liquids during production. This necessitates complex solvent recovery and deep waste liquid treatment equipment, significantly increasing energy consumption, equipment investment, and operating costs, and also causing environmental pollution. Furthermore, organic solvents readily react irreversibly with active ingredients such as polyphenols, saponins, and alkaloids in TCM, disrupting the natural structure and proportions of the active ingredients and affecting efficacy. Organic solvent residues are also prone to remain in the product, posing risks to medication safety and product quality stability. In addition, subcritical organic solvent extraction processes require extremely high equipment sealing, resulting in poor process controllability and making standardized, large-scale continuous production difficult.

[0003] Although traditional water extraction processes use water as the extraction medium, thus avoiding the aforementioned drawbacks of organic solvents, they are limited by conditions such as extraction temperature and pressure. Conventional water extraction processes are mostly carried out at normal pressure and below 100°C, resulting in low extraction efficiency, low dissolution rate of target active ingredients, and long-term extraction can easily cause the inactivation of heat-sensitive active ingredients, which cannot meet the needs of high-quality, industrialized production of traditional Chinese medicine preparations. Summary of the Invention

[0004] In view of this, the present invention provides a subcritical pure water extraction method for traditional Chinese medicine and its application, in order to solve the problems of serious pollution and solvent residue risk in organic solvent extraction processes or low extraction efficiency in water extraction processes in related technologies.

[0005] In a first aspect, the present invention provides a subcritical pure water extraction method for traditional Chinese medicine, comprising the following steps:

[0006] The Chinese herbal raw materials to be extracted are placed in purified water to moisten them, and the moistened Chinese herbal raw materials are obtained. The soaked Chinese herbal raw materials are subjected to subcritical extraction to obtain the extract product; The extracted product is separated and / or purified; The conditions for subcritical extraction include: The extraction solvent was purified water, the solid-liquid ratio was 1:(10~30) g / mL, the extraction temperature was 120~180 ℃, the extraction pressure was 0.5~2.0 MPa, the extraction time was 30~60 min, and the stirring rate was 0~8000 r / min.

[0007] In one optional embodiment, separating and / or purifying the extracted product includes: After the extracted product is cooled and depressurized, the residue in the extracted product is removed, and then at least one of the following operations is performed: solid-liquid separation, concentration, drying, resin adsorption, and alcohol precipitation purification.

[0008] In one optional embodiment, when performing the soaking process, the amount of purified water used is 20-40% of the raw Chinese medicine to be extracted, and the soaking time is 1-2 hours.

[0009] In one optional embodiment, before placing the Chinese herbal medicine raw material to be extracted in purified water for moistening, the step further includes a pretreatment step of the Chinese herbal medicine raw material to be extracted, wherein the pretreatment includes at least one of washing, drying, crushing or cutting.

[0010] In one optional embodiment, the traditional Chinese medicine raw material includes at least one of the following: Salvia miltiorrhiza, Taxus chinensis, Clove, Star anise, Sword bean, Fennel, Thistle, Dioscorea opposita, Hawthorn, Purslane, Black-striped snake, Dried plum, Papaya, Canna indica, Bitter orange blossom, Polygonatum odoratum, Licorice, Angelica dahurica, Ginkgo biloba, White hyacinth bean, White hyacinth bean flower, Longan pulp, Cassia seed, Lily bulb, Nutmeg, Cinnamon, Phyllanthus emblica, Buddha's hand, Almond (sweet, bitter), Sea buckthorn, Oyster shell, Euryale ferox, Sichuan pepper, Red adzuki bean, Donkey-hide gelatin, Chicken gizzard lining, Malt, Kelp, Jujube (jujube, sour jujube, black jujube), Monk fruit, Prunus japonica seed, Honeysuckle, Terminalia chebula, Houttuynia cordata, Ginger (fresh ginger, dried ginger), Japanese raisin tree fruit, Lycium barbarum, Gardenia jasminoides, Amomum villosum, Sterculia lychnophora, Poria cocos, Citronella foenum-graecum , Mosla chinensis, peach kernel, mulberry leaf, mulberry fruit, tangerine peel, platycodon root, alpinia oxyphylla, lotus leaf, radish seed, lotus seed, galangal, bamboo leaf, fermented soybean, chrysanthemum, chicory, yellow mustard seed, polygonatum, perilla, perilla seed, kudzu root, black sesame, black pepper, sophora japonica flower, dandelion, honey, torreya nut, jujube seed, fresh imperata root, fresh reed root, viper, tangerine peel, mint, coix seed, allium macrostemon, raspberry, patchouli, angelica sinensis, galangal, saffron, cardamom, turmeric, long pepper, codonopsis, desert cistanche, dendrobium officinale, American ginseng, astragalus, ganoderma lucidum, cornus officinalis, gastrodia elata, eucommia ulmoides leaf, rehmannia glutinosa, ophiopogon japonicus, asparagus cochinchinensis, tangerine peel.

[0011] In one optional embodiment, the traditional Chinese medicine raw material includes Astragalus membranaceus or Salvia miltiorrhiza, and the subcritical pure water extraction method for the traditional Chinese medicine includes: After washing and drying, the raw materials of Chinese medicine to be extracted are moistened with purified water at 20-40% of the weight of the raw materials of Astragalus membranaceus for 1-2 hours to obtain the moistened raw materials of Chinese medicine. The soaked Chinese herbal raw materials are put into a subcritical extraction vessel, purified water is added, and subcritical extraction is carried out to obtain the Chinese herbal extract product; wherein, the material-to-liquid ratio is 1:(15-25)g / mL, the extraction temperature is 120-160 ℃, the extraction pressure is 0.7-1.1 MPa, the extraction time is 30-60 min, and the stirring rate is 20-8000 r / min; The herbal extract was subjected to solid-liquid separation. The resulting liquid fraction was centrifuged at 5500–8000 r / min for 10–20 min, and the supernatant was collected to obtain the herbal extract.

[0012] In the above-mentioned subcritical pure water extraction method for Astragalus membranaceus or Salvia miltiorrhiza, after the raw materials are washed and dried, they can be directly used for moistening, or the raw materials can be crushed into granules of 20-40 mesh before moistening.

[0013] In one optional embodiment, the traditional Chinese medicine raw material includes Asparagus cochinchinensis, and the subcritical pure water extraction method for the traditional Chinese medicine includes: After washing and drying, the asparagus raw material to be extracted is moistened with 20-40% of the weight of the asparagus raw material in purified water for 1-2 hours to obtain the moistened asparagus raw material. The asparagus raw material after being moistened was put into a subcritical extraction vessel, purified water was added, and subcritical extraction was carried out to obtain the asparagus extract product; wherein, the material-to-liquid ratio was 1:(20-30)g / mL, the extraction temperature was 120-150℃, the extraction pressure was 0.7-0.9 MPa, the extraction time was 30-60 min, and the stirring rate was 20-8000 r / min; The asparagus extract is subjected to solid-liquid separation, and the resulting liquid portion is concentrated to 20%–50% of its original volume to obtain the asparagus extract.

[0014] In the above-mentioned subcritical pure water extraction method for Asparagus, after the Asparagus raw material is washed and dried, it can be directly used as a medicinal decoction piece for moistening, or the raw medicinal decoction piece can be peeled, cut into small pieces or slices and then moistened.

[0015] In one optional embodiment, the traditional Chinese medicine raw material includes licorice, and the subcritical pure water extraction method for the traditional Chinese medicine includes: After washing and drying, the licorice raw material to be extracted is moistened with 20-40% of the weight of the licorice raw material in purified water for 1-2 hours to obtain the moistened licorice raw material. The licorice raw material after being moistened was put into a subcritical extraction vessel, purified water was added, and subcritical extraction was carried out to obtain licorice extract; wherein, the material-to-liquid ratio was 1:(10-25)g / mL, the extraction temperature was 120-160 ℃, the extraction pressure was 0.7-1.1 MPa, the extraction time was 30-60 min, and the stirring rate was 40-50 r / min; The licorice extract was subjected to solid-liquid separation. The resulting liquid fraction was centrifuged at 5500–6500 r / min for 15–20 min, and the supernatant was collected to obtain the danshen extract.

[0016] In the above-mentioned subcritical pure water extraction method for licorice, after the licorice raw material is washed and dried, it can be directly used for moistening the medicine with the raw medicinal material slices, or the raw medicinal material slices can be crushed into granules of 20-40 mesh before moistening the medicine.

[0017] In one optional embodiment, the traditional Chinese medicine raw material includes yew, and the subcritical pure water extraction method for the traditional Chinese medicine includes: After washing and drying, the yew raw material to be extracted is moistened with 20-40% of purified water by weight for 1-2 hours to obtain moistened yew raw material. The moistened yew raw material was put into a subcritical extraction apparatus, purified water was added, and subcritical extraction was carried out to obtain yew extract; wherein, the material-to-liquid ratio was 1:(15-30) g / mL, the extraction temperature was 150-160 ℃, the extraction pressure was 1.0-2.0 MPa, the extraction time was 30-60 min, and the stirring rate was 40-50 r / min; The yew extract was subjected to solid-liquid separation, and the resulting liquid portion was concentrated under reduced pressure to a relative density of 1:(1.3-1.4) to obtain the yew extract.

[0018] In the above-mentioned subcritical pure water extraction method for Taxus chinensis, after washing and drying, the raw Taxus chinensis can be directly used as a medicinal decoction piece for moistening, or the raw medicinal decoction piece can be crushed into granules of 20-40 mesh before moistening.

[0019] The above-mentioned subcritical pure water extraction method for traditional Chinese medicine can effectively extract astragaloside A from Astragalus membranaceus, tanshinone IIA and salvianolic acid B from Salvia miltiorrhiza, polysaccharides and saponins from Asparagus cochinchinensis, glycyrrhizic acid from Glycyrrhiza uralensis, and paclitaxel from Taxus chinensis. The entire extraction process involves the absence of any organic solvents or chemical auxiliaries. Ethanol is used only as a non-extraction aid in the separation and purification steps of some medicinal materials, but no ethanol residue remains in the final extract.

[0020] Secondly, this invention provides the application of the above-mentioned subcritical pure water extraction method for traditional Chinese medicine in the production of traditional Chinese medicine preparations. The extract of effective components obtained by the above-mentioned subcritical pure water extraction method can be directly used to prepare traditional Chinese medicine preparations such as decoctions, granules, capsules, pills, tablets, medicated wines, oral liquids, or extracts.

[0021] Based on the above technical solution, the present invention has at least the following advantages: This invention addresses the core shortcomings of existing traditional Chinese medicine (TCM) extraction processes by providing a subcritical pure water extraction process. This process uses water as the sole extraction medium, deeply integrating subcritical extraction technology with pure water extraction. By optimizing key steps such as material pretreatment, core subcritical extraction parameters, and subsequent separation and purification, a systematic subcritical pure water extraction system is formed, achieving highly efficient enrichment of the effective components of TCM. This process is highly safe, eliminating the generation of organic pollutants at the source, significantly improving the extraction rate and purity of effective components, and greatly shortening the extraction time.

[0022] Specifically, compared with the prior art, the present invention has at least the following significant beneficial effects: (1) Green and environmentally friendly, achieving zero-pollution clean production from the source: This invention uses natural, non-toxic, and renewable water as the only extraction medium and applies subcritical extraction technology to the pure water extraction system. No organic solvents or chemical additives are added throughout the process, eliminating the generation of organic waste gas, solvent-based waste liquid, and solid chemical waste from the source. The small amount of waste liquid generated during the production process is a water-soluble system, which can be recycled or discharged in compliance with standards after simple physical and chemical treatment. There is no need to match complex solvent recovery and waste liquid deep treatment equipment, which greatly reduces the environmental burden of production.

[0023] (2) Integrating technological advantages to significantly improve extraction efficiency and component retention rate: This invention combines the low boiling point and high permeability of subcritical extraction with the mildness of pure water extraction. By precisely controlling the core parameters such as extraction temperature (120-180℃) and extraction pressure (0.5-2.0MPa) of pure water under subcritical conditions, the permeability of pure water to the cell walls of Chinese herbal raw materials and the solubility of effective components are enhanced. Compared with the traditional atmospheric pressure pure water extraction process, the extraction rate of target effective components is increased by 33%-65%, solving the technical problems of "low extraction efficiency and insufficient dissolution of effective components" in the traditional pure water extraction process. At the same time, within the parameter range of material-liquid ratio 1: (10-30) and extraction time 30-60min, the extraction conditions are mild and controllable, which can effectively avoid the inactivation and destruction of heat-sensitive and easily oxidized active components, and completely preserve the natural structure and ratio of each effective component in Chinese herbal medicine, which is more in line with the medicinal essence of Chinese herbal medicine.

[0024] (3) Improve product safety and eliminate quality risks: This process completes the extraction in a subcritical pure water system at 120-180℃ and 0.5-2.0MPa, which completely avoids the irreversible reaction between organic solvents and active ingredients of traditional Chinese medicine. At the same time, it completely eliminates the quality and safety risks of solvent residue and chemical auxiliary agent residue. The purity of the extracted product is 1.5%-3.5% higher than that of the organic solvent extraction process. Moreover, the pure water medium is consistent with the traditional processing and decoction theory of traditional Chinese medicine, and the pharmaceutical compatibility of the extracted product is better. It can be directly used in the production of various traditional Chinese medicine preparations, which greatly reduces the difficulty of quality control in subsequent preparation processes.

[0025] (4) Simplify the production process and reduce the overall production cost: The subcritical pure water extraction system of the present invention can be realized using conventional subcritical equipment without the need for complex equipment such as organic solvent recovery and deep treatment of waste liquid, which greatly reduces equipment investment and maintenance costs; at the same time, a fixed operation process is formed by standardized parameters, the production process is simple and highly controllable, and continuous and large-scale industrial production can be realized. The energy consumption per unit product is reduced by more than 40% compared with the organic solvent extraction process, and the extraction time is shortened by more than 70% compared with the traditional water extraction process, which reduces production energy consumption and labor operation costs; and the extracted residue is a natural material without chemical pollution, which can be further utilized as a resource (such as feed, organic fertilizer, etc.), which improves the comprehensive utilization rate of raw materials and further reduces the overall production cost.

[0026] (5) Wide process adaptability and broad industrial application prospects: The subcritical pure water extraction process of the present invention can be adapted to different medicinal parts such as roots, stems, leaves, flowers, fruits and seeds of Chinese medicine, as well as the extraction of effective components of single Chinese medicine and Chinese medicine compound prescriptions by finely adjusting the extraction temperature and pressure parameters. The material-liquid ratio can be flexibly adjusted according to the characteristics of the raw materials. The extracted products can be directly adapted to the production needs of various Chinese medicine preparations such as decoctions, granules, capsules, pills, tablets, wines, oral liquids and extracts. The process parameters are easy to adjust and simple to operate, with strong adaptability and practicality, and can be widely used in the field of Chinese medicine extraction. Detailed Implementation

[0027] The following embodiments are provided to better understand the present invention and are not limited to the preferred embodiments described. They do not constitute a limitation on the content and scope of protection of the present invention. Any product that is the same as or similar to the present invention, derived by any person under the guidance of the present invention or by combining the features of the present invention with other prior art, falls within the protection scope of the present invention.

[0028] For experiments not specifically described in the examples, the procedures or conditions should be followed according to the conventional experimental procedures described in the literature in this field. Reagents or instruments whose manufacturers are not specified are all commercially available conventional reagent products.

[0029] The present invention will be further described in detail below with reference to specific embodiments, which should not be construed as limiting the scope of protection claimed by the present invention.

[0030] All medicinal materials used in the embodiments and comparative examples of this invention belong to the same batch and specification. The detection of effective components was conducted using the standard testing methods specified in the Pharmacopoeia of the People's Republic of China (2025 edition). The testing equipment and operating environment were kept consistent to ensure the objectivity and accuracy of the data comparison. The source and batch number of each medicinal material are as follows: Astragalus: Sichuan Chunsheng Pharmaceutical Group Co., Ltd., batch number 230601; Danshen: Sichuan Chunsheng Pharmaceutical Group Co., Ltd., batch number 230901; Asparagus: Sichuan Chunsheng Pharmaceutical Group Co., Ltd., batch number 230901; Licorice: Sichuan Chunsheng Pharmaceutical Group Co., Ltd., batch number 230901; Taxus: Sichuan Chunsheng Pharmaceutical Group Co., Ltd., batch number 230601.

[0031] Example 1 Subcritical pure water extraction of Astragalus membranaceus was performed using the following method: (1) Raw material pretreatment: Select dried Astragalus membranaceus without mold or impurities, wash and dry it, then crush it into 20 mesh particles. After sieving, take 100g of Astragalus membranaceus particles and moisten them with purified water at 40% of the raw material mass for 2 hours to obtain moistened Astragalus membranaceus particles for later use.

[0032] (2) Subcritical pure water extraction: After moistening the Astragalus granules, put them into a subcritical extraction vessel and add 1500 mL of purified water at a material-to-liquid ratio of 1:15 (g / mL). After sealing the extraction vessel, start the equipment, raise the temperature to 140℃, adjust the pressure to 0.9 MPa, and maintain the subcritical state for constant temperature and pressure extraction for 50 min. During the extraction process, stir at a rate of 50 r / min to promote the dissolution of effective components and obtain Astragalus extract.

[0033] (3) Separation and purification: After extraction, turn off the heating device. After the temperature in the extraction vessel drops to room temperature and the pressure drops to normal pressure, open the discharge valve and filter the Astragalus extract through a 200-mesh bag filter to remove the dregs and obtain the crude Astragalus extract. Place the crude Astragalus extract in a centrifuge and centrifuge at 8000 r / min for 15 min. Take the supernatant, which is the Astragalus extract.

[0034] Test results: The Astragalus extract prepared above was tested by high performance liquid chromatography (HPLC). The results showed that the extraction rate of astragaloside A was 0.085%, there was no organic solvent residue in the extract, and the purity of astragaloside A reached 92.3%.

[0035] Comparative Example 1 Astragalus membranaceus was extracted with pure water under normal pressure using the following method: (1) Raw material pretreatment: Same as step (1) in Example 1.

[0036] (2) Normal pressure water extraction: After moistening the medicine, the Astragalus granules were put into the extraction tank, and 1500mL of purified water was added at a material-to-liquid ratio of 1:15 (g / mL). The mixture was boiled and refluxed for 2 hours under normal pressure. The extraction was carried out once, and the stirring rate was 50r / min.

[0037] (3) Separation and purification: Same as step (3) in Example 1.

[0038] Test results: The Astragalus extract prepared above was tested by high performance liquid chromatography (HPLC). The results showed that the extraction rate of astragaloside A was 0.052%, with no organic solvent residue and a purity of 88.5%.

[0039] Comparative Example 2 Astragalus alcohol extraction was performed using the following method: (1) Raw material pretreatment: Same as step (1) in Example 1.

[0040] (2) Ethanol extraction: After moistening the Astragalus granules, put them into the extraction tank and add 1500mL of 70% ethanol solution at a material-to-liquid ratio of 1:15 (g / mL). Boil and reflux for 1 hour under normal pressure. Extract twice and combine the two extracts.

[0041] (3) Separation and purification: After filtration and centrifugation, the ethanol was removed by vacuum concentration to obtain Astragalus extract.

[0042] Test results: The Astragalus extract prepared above was tested by high performance liquid chromatography (HPLC). The results showed that the extraction rate of astragaloside A was 0.078%, trace amounts of ethanol residue were detected in the extract (residual amount 0.03%), and the purity of astragaloside A was 90.2%.

[0043] Example 2 The subcritical pure water extraction of Salvia miltiorrhiza was performed using the following method: (1) Raw material pretreatment: Select high-quality dried Salvia miltiorrhiza, remove fibrous roots and impurities, wash and dry, then crush into 20 mesh particles. Take 100g of Salvia miltiorrhiza particles and moisten them with purified water at 40% of the raw material mass for 2 hours to obtain moistened Salvia miltiorrhiza particles for later use.

[0044] (2) Subcritical pure water extraction: After moistening the danshen granules, add them to the subcritical extraction vessel, add 1800mL of purified water at a material-to-liquid ratio of 1:18 (g / mL), seal the vessel, start the equipment, heat to 160℃, adjust the pressure to 1.1MPa, and extract at constant temperature and pressure for 60min. During the extraction process, maintain a low stirring speed of 70r / min to avoid raw material clumping, and obtain the danshen extract.

[0045] (3) Separation and purification: After extraction, the temperature is naturally reduced to below 50℃ and the pressure is reduced to normal pressure. The extract of Salvia miltiorrhiza is filtered through a 200-mesh bag filter, the filtrate is collected, and then centrifuged at 6000r / min for 20min. The supernatant is taken to obtain the Salvia miltiorrhiza extract.

[0046] Test results: The tanshinone IIA extract prepared above was tested by HPLC. The results showed that the extraction rate of tanshinone IIA was 0.028%, the extraction rate of salvianolic acid B was 3.25%, there was no organic solvent residue, and the total purity of the two components was 91.7%.

[0047] Comparative Example 3 The following method was used for the atmospheric pressure pure water extraction of Salvia miltiorrhiza: (1) Raw material pretreatment: Same as step (1) in Example 2.

[0048] (2) Normal pressure water extraction: After moistening the danshen granules, put them into the extraction tank, add 1800mL of purified water at a material-to-liquid ratio of 1:18 (g / mL), boil and reflux for 2.5h at normal pressure, and extract once.

[0049] (3) Separation and purification: Same as step (3) in Example 2.

[0050] Test results: The tanshinone IIA extract prepared above was tested by HPLC. The results showed that the extraction rate of tanshinone IIA was 0.015%, the extraction rate of salvianolic acid B was 1.86%, there was no organic solvent residue, and the total purity of the two components was 87.3%.

[0051] Comparative Example 4 The alcohol extraction of Tanshinone was carried out using the following method: (1) Raw material pretreatment: Same as step (1) in Example 2.

[0052] (2) Ethanol extraction: After moistening the danshen granules, put them into the extraction tank and add 1800mL of 95% ethanol solution at a material-to-liquid ratio of 1:18 (g / mL). Boil and reflux for 1.5h under normal pressure. Extract twice and combine the extracts.

[0053] (3) Separation and purification: After filtration and centrifugation, the ethanol was removed by vacuum concentration to obtain the tanshinone extract.

[0054] Test results: The tanshinone IIA extract prepared above was tested by HPLC. The results showed that the extraction rate of tanshinone IIA was 0.025%, the extraction rate of salvianolic acid B was 2.13%, trace amounts of ethanol residue (0.04%) were detected, and the total purity was 89.5%.

[0055] Example 3 Subcritical pure water extraction of asparagus was performed using the following method: (1) Raw material pretreatment: Select plump and rot-free dried asparagus medicinal material, remove the outer skin and impurities, wash and dry, cut into small pieces of 0.5cm×0.5cm, take 100g of asparagus pieces, moisten with purified water of 40% of the raw material mass for 2 hours to obtain moistened asparagus pieces.

[0056] (2) Subcritical pure water extraction: After moistening the asparagus, put the asparagus block into the subcritical extraction vessel, add 2000mL of purified water at a material-to-liquid ratio of 1:20 (g / mL), seal the equipment, raise the temperature to 130℃, adjust the pressure to 0.7MPa, and extract at constant temperature and pressure for 45min. The stirring rate during the extraction process is 50 r / min to obtain the asparagus extract.

[0057] (3) Separation and purification: After extraction, the temperature is rapidly reduced to room temperature and the pressure is reduced to normal pressure. The extract is filtered to remove the asparagus residue. The filtrate is concentrated to 1 / 5 of its original volume to obtain the asparagus extract.

[0058] Test results: The polysaccharides in the above asparagus extract were detected by the phenol-sulfuric acid method, and the saponins were detected by the vanillin-glacial acetic acid method. The results showed that the polysaccharide extraction rate was 12.8%, the saponin extraction rate was 2.35%, there was no organic solvent residue, and the total purity of polysaccharides and saponins was 89.5%.

[0059] Comparative Example 5 Asparagus was extracted with pure water under normal pressure using the following method: (1) Raw material pretreatment: Same as step (1) in Example 3.

[0060] (2) Normal pressure water extraction: After moistening the asparagus, put the asparagus blocks into the extraction tank, add 2000mL of purified water at a material-to-liquid ratio of 1:20 (g / mL), boil and reflux for 3 hours under normal pressure, and extract once.

[0061] (3) Separation and purification: Same as step (3) in Example 3.

[0062] Test results: The polysaccharides in the above asparagus extract were detected by the phenol-sulfuric acid method, and the saponins were detected by the vanillin-glacial acetic acid method. The results showed that the polysaccharide extraction rate was 8.3%, the saponin extraction rate was 1.42%, there was no organic solvent residue, and the total purity was 85.2%.

[0063] Comparative Example 6 Aspartic alcohol extraction was performed using the following method: (1) Raw material pretreatment: Same as step (1) in Example 3.

[0064] (2) Ethanol extraction: After soaking the asparagus, put the asparagus pieces into the extraction tank, add 2000mL of 80% ethanol solution at a material-to-liquid ratio of 1:20 (g / mL), reflux extract at normal pressure for 2 hours, extract twice, and combine the extracts.

[0065] (3) Separation and purification: After filtration, the alcohol is removed by vacuum concentration, and then 3 times the volume of anhydrous ethanol is added. After stirring evenly, the mixture is allowed to stand for 12 hours. The precipitate is collected by centrifugation, and the precipitate is reconstituted with purified water to obtain the asparagus extract.

[0066] Test results: The polysaccharides in the above asparagus extract were detected by the phenol-sulfuric acid method, and the saponins were detected by the vanillin-glacial acetic acid method. The results showed that the polysaccharide extraction rate was 10.5%, the saponin extraction rate was 1.98%, trace amounts of ethanol residue (0.02%) were detected, and the total purity was 87.8%.

[0067] Example 4 The subcritical pure water extraction of licorice was performed using the following method: (1) Raw material pretreatment: Select dried licorice materials that are free from insects and deterioration, wash and dry them, and then crush them into 20-mesh particles. Take 100g of licorice particles and moisten them with purified water at 40% of the raw material mass for 2 hours to obtain moistened licorice particles for later use.

[0068] (2) Subcritical pure water extraction: After moistening the licorice granules, put them into a subcritical extraction vessel, add 1200mL of purified water at a material-to-liquid ratio of 1:12 (g / mL), seal the vessel, start the equipment, heat to 150℃, adjust the pressure to 1.0MPa, and extract at constant temperature and pressure for 55min. Stir at a rate of 40r / min during the extraction process to enhance the mass transfer effect and obtain the licorice extract.

[0069] (3) Separation and purification: After extraction, cool down to below 40℃, filter the above licorice extract, remove the licorice residue, centrifuge the filtrate at 6000r / min for 20min, take the supernatant, and obtain the licorice extract.

[0070] Test results: The glycyrrhizic acid content of the licorice extract prepared above was detected by HPLC. The results showed that the glycyrrhizic acid extraction rate was 2.86%, there was no organic solvent residue, and the glycyrrhizic acid purity reached 93.1%.

[0071] Comparative Example 7 Licorice was extracted with pure water at normal pressure using the following method: (1) Raw material pretreatment: Same as step (1) in Example 4.

[0072] (2) Normal pressure water extraction: After moistening the licorice granules, put them into the extraction tank, add 1200mL of purified water at a material-to-liquid ratio of 1:12 (g / mL), boil and reflux for 2 hours at normal pressure, extract once, and stir at a speed of 40r / min.

[0073] (3) Separation and purification: Same as step (3) in Example 4.

[0074] Test results: The licorice extract prepared above was tested by high performance liquid chromatography (HPLC). The results showed that the glycyrrhizic acid extraction rate was 1.72%, there was no organic solvent residue, and the glycyrrhizic acid purity was 88.9%.

[0075] Comparative Example 8 Licorice alcohol extraction was performed using the following method: (1) Raw material pretreatment: Same as step (1) in Example 4.

[0076] (2) Ethanol extraction: After moistening the licorice granules, put them into the extraction tank and add 1200mL of 75% ethanol solution at a material-to-liquid ratio of 1:12 (g / mL). Reflux the solution under normal pressure for 1 hour and extract twice. Combine the extracts.

[0077] (3) Separation and purification: After filtering the extract obtained in step (2), the alcohol is removed by vacuum concentration. The concentrate is passed through a macroporous resin adsorption column (D101 type), impurities are washed off with purified water, and glycyrrhizic acid is eluted with 50% ethanol solution (the eluent is only used for separation and is not the extraction medium). The eluent is collected and concentrated until there is no alcohol taste to obtain licorice extract.

[0078] Test results: The licorice extract prepared above was tested by high performance liquid chromatography (HPLC). The results showed that the glycyrrhizic acid extraction rate was 2.53%, trace amounts of ethanol residue (0.03%) were detected, and the purity of glycyrrhizic acid was 90.6%.

[0079] Example 5 Subcritical pure water extraction of Taxus chinensis was performed using the following method: (1) Raw material pretreatment: Select dry yew medicinal materials that are free from insects and deterioration, wash and dry them, and then crush them into 20 mesh particles. Take 100g of yew particles and moisten them with purified water at 40% of the raw material mass for 2 hours to obtain moistened yew particles for later use.

[0080] (2) Subcritical pure water extraction: After moistening the yew granules, put them into a subcritical extraction vessel, add 1500 mL of purified water at a material-to-liquid ratio of 1:15 (g / mL), seal the vessel, start the equipment, heat to 160℃, adjust the pressure to 1.9 MPa, and extract at constant temperature and pressure for 55 min. Stir at a rate of 40 r / min during the extraction process to enhance the mass transfer effect and obtain the yew extract.

[0081] (3) Separation and purification: After extraction, the temperature and pressure are reduced to normal temperature and pressure. The yew extract is filtered through a 1250-mesh bag filter to remove the yew residue. The filtrate is collected and concentrated under reduced pressure to a relative density of 1:1.3 to obtain the yew extract.

[0082] Test results: The paclitaxel content of the paclitaxel extract prepared above was detected by HPLC. The results showed that the paclitaxel extraction rate was 0.04%, there was no organic solvent residue, and the paclitaxel purity reached 99.1%.

[0083] Example 6 The subcritical pure water extraction of yew was carried out according to the method of Example 5. The difference is that in step (2) of this example, the material-to-liquid ratio is 1:30 (g / mL), the extraction temperature is 150 ℃, the extraction pressure is 1.0 MPa, the extraction time is 30 min, and the stirring rate is 50 r / min.

[0084] Test results: The paclitaxel content of the paclitaxel extract prepared above was detected by HPLC. The results showed that the paclitaxel extraction rate was 0.03%, there was no organic solvent residue, and the purity of paclitaxel reached 98.8%.

[0085] Comparative Example 9 Taxus chinensis was extracted with pure water at atmospheric pressure using the following method: (1) Raw material pretreatment: Same as step (1) in Example 5.

[0086] (2) Normal pressure water extraction: Put the moistened yew granules into the extraction tank, add 1500mL of purified water at a material-to-liquid ratio of 1:15 (g / mL), boil and reflux for 2 hours at normal pressure, extract once, and stir at a stirring rate of 40r / min.

[0087] (3) Separation and purification: Same as step (3) in Example 5.

[0088] Test results: The paclitaxel content of the paclitaxel extract prepared above was detected by HPLC. The results showed that the paclitaxel extraction rate was 0.001%, there was no organic solvent residue, and the paclitaxel purity was 85.6%.

[0089] Comparative Example 10 Paclitaxel extraction was performed using the following method: (1) Raw material pretreatment: Same as step (1) in Example 5.

[0090] (2) Ethanol extraction: After moistening the paclitaxel granules, put them into the extraction tank and add 1500mL of 75% ethanol solution at a material-to-liquid ratio of 1:15 (g / mL). Reflux the solution under normal pressure for 1 hour and extract twice. Combine the extracts to obtain the paclitaxel extract.

[0091] (3) Separation and purification: After filtering the paclitaxel extract, concentrate it under reduced pressure to remove alcohol, then pass it through a silica gel column, and then elute the paclitaxel with 50% ethanol solution (the eluent is only used for separation and is not the extraction medium). Collect the eluent and concentrate it until there is no alcohol odor to obtain the paclitaxel extract.

[0092] Test results: The paclitaxel content of the paclitaxel extract prepared above was detected by HPLC. The results showed that the paclitaxel extraction rate was 0.02%, trace amounts of ethanol residue (0.03%) were detected, and the paclitaxel purity was 98.2%.

[0093] Comparative Example 11 The subcritical pure water extraction of yew was carried out according to the method of Example 5. The difference is that in step (2) of this comparative example, the material-to-liquid ratio was 1:35 (g / mL), the extraction temperature was 190 ℃, the extraction pressure was 2.5 MPa, the extraction time was 20 min, and the stirring rate was 40 r / min.

[0094] Test results: The paclitaxel content of the paclitaxel extract prepared above was detected by HPLC. The results showed that the paclitaxel extraction rate was 0.035%, with no organic solvent residue and a paclitaxel purity of 81.3%.

[0095] Comparative Example 12 The subcritical pure water extraction of yew was carried out according to the method of Example 5. The difference is that in step (2) of this comparative example, the material-to-liquid ratio was 1:8 (g / mL), the extraction temperature was 110 ℃, the extraction pressure was 0.3 MPa, the extraction time was 80 min, and the stirring rate was 40 r / min.

[0096] Test results: The paclitaxel content of the paclitaxel extract prepared above was detected by HPLC. The results showed that the paclitaxel extraction rate was 0.008%, with no organic solvent residue and a paclitaxel purity of 98.5%.

[0097] Therefore, the subcritical pure water extraction process for traditional Chinese medicine of this invention, compared with the traditional atmospheric pressure water extraction process, increases the extraction rate of target components by 33%-65%, reduces extraction time by more than 70%, and increases purity by 3%-5%. Compared with the traditional alcohol extraction process, the extraction rate is even higher (3.5%-42%), with no organic solvent residue, and the purity is increased by 1.5%-3.5%. Moreover, a single extraction can achieve the effect of two alcohol extractions, significantly reducing production time. Furthermore, this invention uses water as the sole extraction medium throughout the entire process, eliminating the generation of organic pollutants at the source. Subsequent wastewater treatment is simple, equipment modification costs are low, and it combines high efficiency, safety, and environmental friendliness, perfectly meeting the green, standardized, and industrialized development needs of the traditional Chinese medicine industry.

[0098] Obviously, the above embodiments are merely illustrative examples for clear explanation and are not intended to limit the implementation. Those skilled in the art will recognize that other variations or modifications can be made based on the above description. It is neither necessary nor possible to exhaustively list all possible implementations here. However, obvious variations or modifications derived therefrom are still within the scope of protection of this invention.

Claims

1. A subcritical pure water extraction method for traditional Chinese medicine, characterized in that, Includes the following steps: The Chinese herbal raw materials to be extracted are placed in purified water to moisten them, and the moistened Chinese herbal raw materials are obtained. The soaked Chinese herbal raw materials are subjected to subcritical extraction to obtain the extract product; The extracted product is separated and / or purified; The conditions for subcritical extraction include: The extraction solvent was purified water, the solid-liquid ratio was 1:(10~30) g / mL, the extraction temperature was 120~180 ℃, the extraction pressure was 0.5~2.0 MPa, the extraction time was 30~60 min, and the stirring rate was 0~8000 r / min.

2. The subcritical pure water extraction method for traditional Chinese medicine according to claim 1, characterized in that, The separation and / or purification of the extracted product includes: After the extracted product is cooled and depressurized, the residue in the extracted product is removed, and then at least one of the following operations is performed: solid-liquid separation, concentration, drying, resin adsorption, and alcohol precipitation purification.

3. The subcritical pure water extraction method for traditional Chinese medicine according to claim 1, characterized in that, When performing the soaking process, the amount of purified water used is 20% to 40% of the raw Chinese medicine to be extracted, and the soaking time is 1 to 2 hours.

4. The subcritical pure water extraction method for traditional Chinese medicine according to claim 1, characterized in that, Before placing the Chinese herbal raw material to be extracted in purified water for moistening, the process also includes a pretreatment step of the Chinese herbal raw material to be extracted, which includes at least one of washing, drying, crushing or cutting.

5. The method for subcritical pure water extraction of traditional Chinese medicine according to any one of claims 1 to 4, characterized in that, The traditional Chinese medicine raw materials include at least one of the following: Salvia miltiorrhiza, Taxus chinensis, Clove, Star anise, Sword bean, Fennel, Thistle, Dioscorea opposita, Hawthorn, Purslane, Black-striped snake, Dried plum, Papaya, Canna indica, Bitter orange blossom, Polygonatum odoratum, Licorice, Angelica dahurica, Ginkgo biloba, White hyacinth bean, White hyacinth bean flower, Longan pulp, Cassia seed, Lily bulb, Nutmeg, Cinnamon, Phyllanthus emblica, Buddha's hand, Almond (sweet, bitter), Sea buckthorn, Oyster shell, Euryale ferox, Sichuan pepper, Red adzuki bean, Donkey-hide gelatin, Chicken gizzard lining, Malt, Kelp, Jujube (jujube, sour jujube, black jujube), Monk fruit, Prunus japonica seed, Honeysuckle, Terminalia chebula, Houttuynia cordata, Ginger (fresh ginger, dried ginger), Japanese raisin tree fruit, Lycium barbarum, Gardenia jasminoides, Amomum villosum, Sterculia lychnophora, Poria cocos, Citronella foenum-graecum , Mosla chinensis, peach kernel, mulberry leaf, mulberry fruit, tangerine peel, platycodon root, alpinia oxyphylla, lotus leaf, radish seed, lotus seed, galangal, bamboo leaf, fermented soybean, chrysanthemum, chicory, yellow mustard seed, polygonatum, perilla, perilla seed, kudzu root, black sesame, black pepper, sophora japonica flower, dandelion, honey, torreya nut, jujube seed, fresh imperata root, fresh reed root, viper, tangerine peel, mint, coix seed, allium macrostemon, raspberry, patchouli, angelica sinensis, galangal, saffron, cardamom, turmeric, long pepper, codonopsis, desert cistanche, dendrobium officinale, American ginseng, astragalus, ganoderma lucidum, cornus officinalis, gastrodia elata, eucommia ulmoides leaf, rehmannia glutinosa, ophiopogon japonicus, asparagus cochinchinensis, tangerine peel.

6. The method for subcritical pure water extraction of traditional Chinese medicine according to any one of claims 1 to 4, characterized in that, The herbal raw materials include Astragalus membranaceus or Salvia miltiorrhiza, and the subcritical pure water extraction method for the herbal raw materials includes: After washing and drying, the raw materials of traditional Chinese medicine to be extracted are moistened with purified water at 20-40% of the weight of the raw materials of Astragalus membranaceus for 1-2 hours to obtain the raw materials of traditional Chinese medicine after moistening. The soaked Chinese herbal raw materials are put into a subcritical extraction vessel, purified water is added, and subcritical extraction is carried out to obtain the Chinese herbal extract product; wherein, the material-to-liquid ratio is 1:(15-25)g / mL, the extraction temperature is 120-160 ℃, the extraction pressure is 0.7-1.1 MPa, the extraction time is 30-60 min, and the stirring rate is 20-8000 r / min; The herbal extract was subjected to solid-liquid separation. The resulting liquid fraction was centrifuged at 5500–8000 r / min for 10–20 min, and the supernatant was collected to obtain the herbal extract.

7. The method for subcritical pure water extraction of traditional Chinese medicine according to any one of claims 1 to 4, characterized in that, The herbal raw material includes Asparagus root, and the subcritical pure water extraction method for the herbal raw material includes: After washing and drying, the asparagus raw material to be extracted is moistened with 20-40% of the weight of the asparagus raw material in purified water for 1-2 hours to obtain the moistened asparagus raw material. The asparagus raw material after being moistened was put into a subcritical extraction vessel, purified water was added, and subcritical extraction was carried out to obtain the asparagus extract product; wherein, the material-to-liquid ratio was 1:(20-30)g / mL, the extraction temperature was 120-150℃, the extraction pressure was 0.7-0.9 MPa, the extraction time was 30-60 min, and the stirring rate was 20-8000 r / min; The asparagus extract is subjected to solid-liquid separation, and the resulting liquid portion is concentrated to 20%–50% of its original volume to obtain the asparagus extract.

8. The method for subcritical pure water extraction of traditional Chinese medicine according to any one of claims 1 to 4, characterized in that, The herbal raw material includes licorice, and the subcritical pure water extraction method for the herbal raw material includes: After washing and drying, the licorice raw material to be extracted is moistened with 20-40% of the weight of the licorice raw material in purified water for 1-2 hours to obtain the moistened licorice raw material. The licorice raw material after being moistened was put into a subcritical extraction vessel, purified water was added, and subcritical extraction was carried out to obtain licorice extract; wherein, the material-to-liquid ratio was 1:(10-25)g / mL, the extraction temperature was 120-160 ℃, the extraction pressure was 0.7-1.1 MPa, the extraction time was 30-60 min, and the stirring rate was 40-50 r / min; The licorice extract was subjected to solid-liquid separation. The resulting liquid fraction was centrifuged at 5500–6500 r / min for 15–20 min, and the supernatant was collected to obtain the licorice extract.

9. The method for subcritical pure water extraction of traditional Chinese medicine according to any one of claims 1 to 4, characterized in that, The medicinal material includes Taxus chinensis, and the subcritical pure water extraction method for the medicinal material includes: After washing and drying, the yew raw material to be extracted is moistened with 20-40% of the weight of the yew raw material in purified water for 1-2 hours to obtain the moistened yew raw material. The moistened yew raw material was put into a subcritical extraction apparatus, purified water was added, and subcritical extraction was carried out to obtain yew extract; wherein, the material-to-liquid ratio was 1:(15-30) g / mL, the extraction temperature was 150-160 ℃, the extraction pressure was 1.0-2.0 MPa, the extraction time was 30-60 min, and the stirring rate was 40-50 r / min; The yew extract was subjected to solid-liquid separation, and the resulting liquid portion was concentrated under reduced pressure to a relative density of 1:(1.3-1.4) to obtain the yew extract.

10. The application of the subcritical pure water extraction method for traditional Chinese medicine according to any one of claims 1 to 9 in the production of traditional Chinese medicine preparations.