A method for comprehensive extraction of eucommia ulmoides gum and eucommia ulmoides chlorogenic acid from eucommia ulmoides leaves

Abstract

The application discloses a method for comprehensively extracting eucommia ulmoides gum and eucommia ulmoides chlorogenic acid from eucommia ulmoides leaves, and relates to the technical field of natural plant extraction, and has the technical points that the eucommia ulmoides gum is effectively extracted without destroying the eucommia ulmoides chlorogenic acid by using the eucommia ulmoides leaves, eucommia ulmoides bark and eucommia ulmoides fruits through a subcritical ultrasonic extraction technology, and the eucommia ulmoides chlorogenic acid, which is a heat-sensitive component, is effectively extracted by using a continuous countercurrent ultrasonic extraction technology, so that the comprehensive extraction technology has the outstanding advantages of simple operation, safety, low comprehensive cost of raw materials for extracting the eucommia ulmoides gum and the eucommia ulmoides chlorogenic acid, no environmental pollution in the production process and industrialized large-scale production.

Description

Technical Field

[0001] This invention relates to the field of natural plant extraction technology, specifically to a method for the comprehensive extraction of Eucommia gum and Eucommia chlorogenic acid from Eucommia leaves. Background Technology

[0002] Eucommia ulmoides Oliv., a plant belonging to the genus Eucommia in the family Eucommiaceae, is a relict tree species endemic to my country and a national second-class protected species. In my country, Eucommia has been used for disease treatment and health maintenance for over 2000 years, as recorded in ancient pharmacopoeias such as the *Shennong Bencao Jing* and *Compendium of Materia Medica*. As a traditional Chinese medicine, Eucommia is characterized by its lack of toxic side effects. Eucommia contains abundant lignans, chlorogenic acid, and flavonoids, which can regulate immunity, have antioxidant, anti-aging, and anti-senile effects, and can also calm the nerves, relieve pain, and have cosmetic and pregnancy-supporting effects. Eucommia contains pinoresinol diglucoside, a recognized precious natural antihypertensive drug with a "bidirectional regulatory" effect, possessing a special efficacy in adjusting low blood pressure. Eucommia also contains flavonoids and cyclic ether terpenes, which have vasodilatory, blood sugar-lowering, and blood lipid-lowering effects, and are beneficial for the prevention and treatment of cardiovascular and cerebrovascular diseases. Eucommia ulmoides is an effective medicine for treating various diseases. It contains geniposide, aucubin, and various trace elements such as potassium, which have a laxative and diuretic effect. Eucommia ulmoides also helps eliminate neutral fats in the body, promotes collagen metabolism, and achieves weight loss. The alkaloids in Eucommia ulmoides have an important function: tonifying the liver and kidneys, strengthening muscles and bones, and relieving fatigue. Eucommia ulmoides is rich in eugenol, diquinone glycosides, α-linolenic acid, and many other active ingredients, which have anti-cancer, anti-AIDS, antibacterial, and harmful cell growth-inhibiting functions. Of the 27 functions of health foods published by the State Food and Drug Administration, Eucommia ulmoides possesses more than half. The multifaceted health benefits of Eucommia ulmoides are unique among traditional Chinese medicines. Compared with precious medicinal materials such as Cordyceps sinensis, Dendrobium, and ginseng, aside from not being a "scarce" resource, it is the most superior health food raw material in terms of function, lack of toxic side effects, utilization rate, cost-effectiveness, palatability, and authenticity. In my country's functional health food market, compound products focusing on boosting immunity, combating fatigue, lowering blood lipids, lowering blood pressure, lowering blood sugar, increasing bone density, protecting the liver, and providing antioxidant benefits are the most prevalent. Eucommia ulmoides, a single ingredient, can comprehensively cover these functions. Its multifunctionality and high utilization value will enable it to play a significant role in the future health industry and market economy.

[0003] Eucommia ulmoides leaves, bark, and fruit are rich in eucommia gum. my country has over 700,000 hectares of Eucommia ulmoides plantations, making it a new source of renewable natural rubber. Eucommia gum is extracted from plants such as Eucommia ulmoides, and its main component is trans-1,4-polyisoprene (TPI). TPI possesses many unique characteristics: it is a hard plastic with a fixed shape at room temperature; above 60°C, it exhibits rubbery properties, capable of various deformations, making it an excellent shape memory functional material; when the degree of cross-linking reaches a certain level, it transforms into a complete rubber elastomer, suitable for tires and various rubber products. Therefore, eucommia gum has a very broad application prospect in medical materials, rubber products, and other fields.

[0004] Currently, extraction methods for Eucommia gum production include alkaline extraction, solvent extraction, and enzymatic hydrolysis. These methods mostly utilize Eucommia leaves, fruits, and bark directly, resulting in high costs due to single-use of raw materials, large consumption of organic solvents, significant flammability and explosiveness hazards, low extraction rates, and severe environmental pollution. Similarly, extraction methods for Eucommia chlorogenic acid production include organic solvent extraction, water extraction, and enzymatic hydrolysis. These methods also mostly utilize Eucommia leaves, fruits, and bark directly, leading to high costs due to single-use of raw materials, large water consumption, low extraction rates, and low content. Consequently, my country's unique Eucommia resources are not effectively developed and utilized, hindering the widespread application of high-performance Eucommia gum and health-promoting Eucommia chlorogenic acid.

[0005] Therefore, the present invention aims to provide a method for the comprehensive extraction of eucommia gum and eucommia chlorogenic acid from Eucommia ulmoides leaves, in order to solve the above-mentioned problems. Summary of the Invention

[0006] The purpose of this invention is to solve the above-mentioned problems and provide a method for the comprehensive extraction of Eucommia ulmoides gum and Eucommia chlorogenic acid from Eucommia ulmoides leaves. This invention uses subcritical ultrasonic extraction technology to effectively extract Eucommia ulmoides gum from Eucommia ulmoides leaves, bark, and fruit without destroying Eucommia chlorogenic acid. The residue is then subjected to continuous countercurrent ultrasonic extraction technology to effectively extract the heat-sensitive component Eucommia chlorogenic acid. The comprehensive extraction technology has outstanding advantages such as simple and safe operation, low overall cost of extracting both Eucommia ulmoides gum and Eucommia chlorogenic acid from raw materials, no environmental pollution during the production process, and suitability for large-scale industrial production.

[0007] To achieve the above objectives, the technical solution of the present invention is as follows:

[0008] This invention provides a method for the comprehensive extraction of eucommia gum and eucommia chlorogenic acid from Eucommia ulmoides leaves, the method comprising the following steps:

[0009] S1. Take dried Eucommia ulmoides leaves, bark, and pericarp, crush and press them into raw material granules, and send them into a subcritical ultrasonic extractor. Use R134a mixed solvent at an extraction pressure of 0.4MPa-2.0MPa and a temperature of 10℃-50℃ for subcritical ultrasonic countercurrent extraction for 40min-60min to obtain the extract.

[0010] S2. The extract is then filtered through a filter, and the resulting filtrate is pumped into an analytical tank. By adjusting the temperature to 10℃-50℃ and the pressure to 5×105pa-1×104pa, R134a in the R134a mixed solvent is converted from liquid to gaseous state, separating it from the extract, and obtaining Eucommia ulmoides crude gum paste.

[0011] S3. The crude eucommia gum viscous paste is fed into an integrated crystallization-purification-drying tank, and after being dissolved in petroleum ether organic solvent, impurities are removed, crystallization occurs, purification is performed, concentration is achieved, and drying is carried out to finally obtain refined eucommia gum.

[0012] S4. The residue after extracting the crude gum viscous extract of Eucommia ulmoides is extracted using a continuous countercurrent ultrasonic extraction device with a material-to-water ratio of 1:6 at 30-50℃ for 60 minutes. The filtrate is clarified and impurities are removed using a 1+1 clarifying agent or chitosan clarifying agent, followed by membrane separation and concentration, and vacuum low-temperature drying to obtain Eucommia ulmoides pure powder with light color, high purity, and good solubility.

[0013] Using dried Eucommia ulmoides leaves, bark, and pericarp as raw materials for extracting Eucommia gum, crushing and pressing the raw materials into granules facilitates subcritical fluid extraction and increases the feed rate. Subcritical ultrasonic extraction equipment is used with colorless, non-toxic, odorless, and non-flammable / explosive R134a subcritical fluid for subcritical extraction. Subcritical ultrasonic extraction greatly increases the extraction capacity. The choice of R134a subcritical fluid avoids the drawbacks of conventional methods using petroleum ether extraction, which is flammable, explosive, and extremely dangerous. The extract is naturally recovered (concentrated) by controlling temperature and pressure to obtain a crude Eucommia gum paste. The crude Eucommia gum paste is then processed in an integrated crystallization-purification-drying tank to obtain refined Eucommia gum, i.e., the purification process of crystallization, decolorization, and re-crystallization is completed in the integrated tank. Subcritical ultrasonic extraction equipment has outstanding advantages such as large processing capacity, high extraction rate, no damage to the heat-sensitive components of raw materials, fire and explosion prevention, and small footprint. The residue after gum extraction is extracted with water using a continuous countercurrent ultrasonic extraction device, clarified and impurities removed with a clarifying agent, concentrated by membrane separation, and vacuum low-temperature drying to obtain pure Eucommia ulmoides powder with light color, high purity, and good solubility.

[0014] Compared with existing technologies, the beneficial effects of this solution are:

[0015] 1. This invention utilizes subcritical ultrasonic extraction technology and uses R134a solvent as the extraction solvent, which solves the production difficulties caused by the need to use flammable and explosive organic solvents (petroleum ether or n-hexane) in solvent extraction.

[0016] 2. This invention utilizes subcritical ultrasonic extraction technology. The pressure of subcritical ultrasonic extraction equipment is much lower than that of supercritical extraction equipment, and the equipment volume is greatly increased, making large-scale production a reality. This solves the problem that supercritical CO2 extraction requires high pressure, resulting in strict equipment manufacturing requirements and small extraction volume, which seriously affects large-scale production.

[0017] 3. This invention adopts a purification process of dissolving, crystallizing, decolorizing, and re-crystallizing Eucommia ulmoides crude gum in an integrated crystallization-purification-drying tank, which solves the production difficulties caused by the use of flammable and explosive organic solvents (petroleum ether or n-hexane) and multiple tank conversions in the purification process of Eucommia ulmoides crude gum.

[0018] 4. In this invention, after subcritical extraction of Eucommia gum, chlorogenic acid in the Eucommia raw material is preserved, and then chlorogenic acid is extracted using a continuous countercurrent ultrasonic extraction device, so that the product activity is maintained while maintaining a high yield.

[0019] 5. This invention effectively combines subcritical ultrasonic extraction technology with continuous countercurrent ultrasonic extraction technology, making full use of Eucommia ulmoides leaves and doubling production efficiency. Attached Figure Description

[0020] Figure 1 This is a flowchart of the method in an embodiment of the present invention. Detailed Implementation

[0021] To enable those skilled in the art to better understand the present invention, the technical solution of the present invention will be described in further detail below with reference to the embodiments and accompanying drawings. Obviously, the described embodiments are merely some, not all, of the embodiments of the present invention. All other embodiments obtained by those skilled in the art based on the embodiments of the present invention without creative effort should fall within the scope of protection of the present invention.

[0022] It should be noted that, unless otherwise specified, the embodiments and features described in the present invention can be combined with each other. The present invention will now be described in detail with reference to the embodiments.

[0023] Example:

[0024] The present invention provides a method for the comprehensive extraction of eucommia gum and eucommia chlorogenic acid from Eucommia ulmoides leaves, as described above. The method includes the following steps:

[0025] S1. Take dried Eucommia ulmoides leaves, bark, and pericarp, crush and press them into raw material granules, and send them into a subcritical ultrasonic extractor. Use R134a mixed solvent at an extraction pressure of 0.4MPa-2.0MPa and a temperature of 10℃-50℃ for subcritical ultrasonic countercurrent extraction for 40min-60min to obtain the extract.

[0026] S2. The extract is then filtered through a filter, and the resulting filtrate is pumped into an analytical tank. By adjusting the temperature to 10℃-50℃ and the pressure to 5×105pa-1×104pa, R134a in the R134a mixed solvent is converted from liquid to gaseous state, separating it from the extract, and obtaining Eucommia ulmoides crude gum paste.

[0027] S3. The crude eucommia gum viscous paste is fed into an integrated crystallization-purification-drying tank, and after being dissolved in petroleum ether organic solvent, impurities are removed, crystallization occurs, purification is performed, concentration is achieved, and drying is carried out to finally obtain refined eucommia gum.

[0028] S4. The residue after extracting the crude gum viscous extract of Eucommia ulmoides is extracted using a continuous countercurrent ultrasonic extraction device with a material-to-water ratio of 1:6 at 30-50℃ for 60 minutes. The filtrate is clarified and impurities are removed using a 1+1 clarifying agent or chitosan clarifying agent, followed by membrane separation and concentration, and vacuum low-temperature drying to obtain Eucommia ulmoides pure powder with light color, high purity, and good solubility.

[0029] Using dried Eucommia ulmoides leaves, bark, and pericarp as raw materials for extracting Eucommia gum, crushing and pressing the raw materials into granules facilitates subcritical fluid extraction and increases the feed rate. Subcritical ultrasonic extraction equipment is used with colorless, non-toxic, odorless, and non-flammable / explosive R134a subcritical fluid for subcritical extraction. Subcritical ultrasonic extraction greatly increases the extraction capacity. The choice of R134a subcritical fluid avoids the drawbacks of conventional methods using petroleum ether extraction, which is flammable, explosive, and extremely dangerous. The extract is naturally recovered (concentrated) by controlling temperature and pressure to obtain a crude Eucommia gum paste. The crude Eucommia gum paste is then processed in an integrated crystallization-purification-drying tank to obtain refined Eucommia gum, i.e., the purification process of crystallization, decolorization, and re-crystallization is completed in the integrated tank. Subcritical ultrasonic extraction equipment has outstanding advantages such as large processing capacity, high extraction rate, no damage to the heat-sensitive components of raw materials, fire and explosion prevention, and small footprint. The residue after gum extraction is extracted with water using a continuous countercurrent ultrasonic extraction device, clarified and impurities removed with a clarifying agent, concentrated by membrane separation, and vacuum low-temperature drying to obtain pure Eucommia ulmoides powder with light color, high purity, and good solubility.

[0030] By utilizing subcritical ultrasonic extraction technology and employing R134a solvent as the extraction solvent, the production difficulties caused by the necessity of using flammable and explosive organic solvents (petroleum ether or n-hexane) in solvent extraction are resolved. Furthermore, using R134a solvent eliminates the need for distillation recovery during production, restoring the solvent to a high purity state and overcoming the difficulties associated with distillation and concentration of flammable and explosive organic solvents (petroleum ether or n-hexane) in solvent extraction. Moreover, the use of R134a solvent allows for finely ground raw materials without affecting production, overcoming the limitation of excessively finely ground raw materials that hinders extract flow due to operational constraints. Finally, the subcritical ultrasonic extraction equipment operates at a significantly lower pressure than supercritical extraction equipment, greatly increasing equipment volume and enabling large-scale production. This addresses the issue of the high pressure required for supercritical CO2 extraction, which necessitates stringent equipment manufacturing requirements and small extraction volumes, severely impacting large-scale production. The purification process of Eucommia ulmoides crude gum, including dissolution, crystallization, decolorization, and re-crystallization, is completed in an integrated crystallization-purification-drying tank. This solves the production difficulties caused by the use of flammable and explosive organic solvents (petroleum ether or n-hexane) and multiple tank switching during the purification process. After subcritical extraction of Eucommia ulmoides gum, while preserving the chlorogenic acid in the raw material, continuous countercurrent ultrasonic extraction is used to extract chlorogenic acid. This ensures high yield and maintains product activity, overcoming the damage to chlorogenic acid caused by high-temperature extraction in conventional equipment. The effective combination of subcritical ultrasonic extraction and continuous countercurrent ultrasonic extraction technologies fully utilizes Eucommia ulmoides leaves, significantly increasing production efficiency and solving the prominent problem of high production costs due to single extraction of Eucommia ulmoides raw materials.

[0031] The above specific embodiments are merely explanations of the present invention and are not intended to limit the present invention. After reading this specification, those skilled in the art can make modifications to these embodiments without contributing any inventive step, but as long as they are within the scope of the claims of the present invention, they are protected by patent law.

Claims

1. A method for the comprehensive extraction of eucommia gum and eucommia chlorogenic acid from Eucommia ulmoides leaves, characterized in that: The method includes the following steps: S1. Take dried Eucommia ulmoides leaves, bark, and pericarp, crush and press them into raw material granules, and feed them into an extractor. Use a mixed solvent at a temperature of 10℃-50℃, an extraction pressure of 0.4MPa-2.0MPa, and an extraction time of 40min-60min to obtain the extract. S2. The extract is then filtered through a filter, and the resulting filtrate is pumped into an analytical tank. By adjusting the temperature to 10℃-50℃ and the pressure to 5×105pa-1×104pa, R134a in the R134a mixed solvent is converted from liquid to gaseous state, separating it from the extract, and obtaining Eucommia ulmoides crude gum paste. S3. The crude eucommia gum viscous paste is fed into an integrated crystallization-purification-drying tank, and after being dissolved in petroleum ether organic solvent, impurities are removed, crystallization occurs, purification is performed, concentration is achieved, and drying is carried out to finally obtain refined eucommia gum. S4. The residue after extracting the crude gum viscous extract of Eucommia ulmoides is extracted using a continuous countercurrent ultrasonic extraction device with a material-to-water ratio of 1:6 at 30-50℃ for 60 minutes. The filtrate is clarified and impurities are removed using a 1+1 clarifying agent or chitosan clarifying agent, followed by membrane separation and concentration, and vacuum low-temperature drying to obtain Eucommia ulmoides pure powder with light color, high purity, and good solubility.

2. The method for comprehensively extracting eucommia gum and eucommia chlorogenic acid from Eucommia ulmoides leaves as described in claim 1, characterized in that: The extractor is a subcritical ultrasonic extractor, and the mixed solvent is R134a mixed solvent. S1 involves crushing and pressing dried Eucommia ulmoides leaves, bark, and pericarp into raw material particles, which are then fed into the subcritical ultrasonic extractor. The extract is obtained by subcritical ultrasonic countercurrent extraction at 0.4MPa-2.0MPa extraction pressure and 10℃-50℃ using R134a mixed solvent for 40min-60min to obtain the extract.

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