A superheated water rapid extraction method of volatile oil in agastache rugosa mixture

Abstract

The application discloses a superheated water rapid extraction method of volatile oil in an agillae herba mixture, and belongs to the technical field of effective component extraction of traditional Chinese medicines. The method comprises the following steps: mixing pachysandra terminalis, perilla leaves and radix anemarrhena asperae, mechanically crushing and sieving the mixture to prepare powder; adding the powder and purified water into a pressure-resistant extraction tank, stirring and heating the mixture to 105 DEG C to 130 DEG C, increasing the pressure in the tank to 0.05 to 0.20 MPa, and extracting the mixture at constant temperature and pressure for 10 to 40 minutes; stopping heating after the extraction is completed, slightly opening an exhaust valve to perform differential pressure flash evaporation, guiding out a water vapor mixture, and cooling and collecting the upper layer volatile oil after layering; cooling the remaining material in the tank to below 60 DEG C, filtering and removing residues, and collecting water phase extraction liquid; and using the extraction liquid and the obtained volatile oil as raw materials for preparing the agillae herba mixture. The application accelerates the dissolution of volatile oil in the mixed powder of pachysandra terminalis, perilla leaves and radix anemarrhena asperae, and the extraction process can be completed in ten to forty minutes, so that the extraction time is greatly shortened.

Description

Technical Field

[0001] This invention relates to the field of extraction of effective components from traditional Chinese medicine, specifically a method for rapid extraction of volatile oil from Huoxiang Zhengqi Compound using hot water. Background Technology

[0002] The volatile oil extracted from a mixture of patchouli, perilla leaves, and angelica is a medicinal raw material rich in active ingredients such as patchouli alcohol, and has a core application in the formulation of Huoxiang Zhengqi compound. The volatile oil of this mixture of herbs has specific pharmacological activities and can be efficiently released under closed pressurized superheated water conditions. Moreover, the aqueous phase after extraction still contains effective substances such as soluble glycosides and flavonoids. Therefore, the extraction of volatile oil is a recognized key step in the preparation of compound preparations. However, from the perspective of conventional atmospheric pressure or long-time extraction processes, there are still many shortcomings in the use of it as a raw material extraction method for high-quality preparations. To address the problems of low polar solubility, insufficient cell wall disruption and release, easy oxidation of marker components, and high overall energy consumption in conventional extraction, process improvement is one of the most effective methods to overcome extraction defects. Extraction process improvement mainly involves two methods: optimization of extraction parameters and upgrading of the separation system. Optimization of extraction parameters utilizes superheated water in a closed system to increase the solubility of weakly polar components in the solvent, reduce the resistance to the migration of internal components, and thus ensure more complete release. Upgrading the separation system often involves differential pressure flash evaporation and aqueous phase reuse. This method offers continuous operation, significant extraction efficiency, and reduced waste liquid, making it the primary method for obtaining this volatile oil. Currently, commonly used and efficient methods for preparing such formulation raw materials include closed pressurized superheated water extraction, differential pressure flash evaporation, and aqueous phase extract collection and preparation methods. Summary of the Invention

[0003] The purpose of this invention is to provide a rapid hot water extraction method for volatile oils in Huoxiang Zhengqi Compound, so as to solve the problems mentioned in the background art.

[0004] The technical solution of the present invention includes: Step 1, pretreatment of medicinal materials: mixing patchouli, perilla leaves and angelica dahurica, mechanically pulverizing and sieving to obtain mixed medicinal material powder; Step 2, closed pressurized superheated water extraction: The mixed medicinal powder obtained in Step 1 is put into a pressure-resistant extraction tank and purified water is added; the pressure-resistant extraction tank is sealed, stirring is turned on, and the temperature is raised to 105℃~130℃, so that the internal pressure of the pressure-resistant extraction tank is raised to 0.05MPa~0.20MPa. Under this superheated water condition, the extraction is carried out at constant temperature and pressure for 10~40 minutes. Step 3, differential pressure flash evaporation and volatile oil collection: After the extraction in step 2 is completed, heating is stopped, and the exhaust valve at the top of the pressure-resistant extraction tank is slightly opened to perform differential pressure flash evaporation. The water vapor mixture generated by differential pressure flash evaporation is discharged and cooled to obtain a gas-liquid mixture. The gas-liquid mixture is allowed to stand and separate into layers, and the upper oily substance is collected to obtain the volatile oil for Huoxiang Zhengqi Compound. Step 4, Extract Collection and Compound Preparation: The remaining material in the pressure-resistant extraction tank after the pressure difference flash evaporation and depressurization in Step 3 is cooled to below 60°C, the dregs are removed by filtration, and the aqueous extract is collected; the aqueous extract and the volatile oil collected in Step 3 are used together as raw materials for Huoxiang Zhengqi Compound.

[0005] Furthermore, in step 1, the weight ratio of patchouli, perilla leaf and angelica is 5:3:2; the sieving is done through a 20-40 mesh sieve.

[0006] Furthermore, in step 2, the amount of purified water added is 8 to 15 times the weight of the mixed medicinal powder.

[0007] Furthermore, in step 2, the stirring speed is set to 60~120 r / min.

[0008] Furthermore, in step 3, the cooling temperature is controlled at 20℃~30℃; the settling time is 5~10 minutes.

[0009] Furthermore, in step 2, the temperature is raised to 115°C, so that the internal pressure of the pressure-resistant extraction tank is raised to 0.10 MPa, and the extraction is carried out at constant temperature and pressure for 20 minutes.

[0010] Further, in step 2, the temperature is raised to 130°C, so that the internal pressure of the pressure-resistant extraction tank is raised to 0.20 MPa, and the extraction is carried out at constant temperature and pressure for 10 minutes.

[0011] This invention provides a rapid hot water extraction method for volatile oils from Huoxiang Zhengqi Compound, which has the following improvements and advantages compared with the prior art: 1. This method involves adding purified water to a pressure-resistant extraction tank and sealing it for heating, using a closed pressurized superheated water environment for constant temperature and pressure extraction. The superheated water environment at specific temperature and pressure greatly accelerates the dissolution of volatile oils in the mixed herbal powder of patchouli, perilla leaf and angelica, and the extraction process can be completed in only ten to forty minutes, significantly shortening the extraction time. 2. This method utilizes differential pressure flash evaporation technology. After the superheated water extraction is completed, the pressure is released by slightly opening the exhaust valve, allowing the volatile oil to be quickly extracted with the water vapor mixture. Combined with subsequent cooling treatment and short-time settling and stratification operation, oil-water separation can be quickly achieved and the upper oily substance can be collected, thus improving the extraction speed of volatile oil. 3. After the flash separation of volatile oil is completed, the remaining material in the pressure-resistant extraction tank is cooled and filtered to remove the residue, and the aqueous extract is collected. The volatile oil and the aqueous extract are used together as raw materials for Huoxiang Zhengqi Compound. The preparation of two key raw materials is completed continuously in the same extraction tank, avoiding multiple transfers and cumbersome steps, and simplifying the overall compound preparation process. 4. This method involves mechanically pulverizing and sieving the pretreatment of patchouli, perilla leaves, and angelica dahurica. With the addition of appropriate purified water and continuous stirring during the extraction process, sufficient contact and mixing of the herbal powder and purified water solvent are ensured. This uniform mass transfer environment ensures the stability of hot water extraction, making the quality of the final volatile oil and aqueous extract more reliable and controllable. Detailed Implementation

[0012] To make the objectives, technical solutions, and advantages of this invention clearer, the invention will be further described in detail below with reference to specific embodiments. Example 1:

[0013] This embodiment provides a method for rapid hot water extraction of volatile oil for preparing Huoxiang Zhengqi Compound, the specific steps of which are as follows; S1 Pretreatment of medicinal materials: Weigh 500g of patchouli, 300g of perilla leaves and 200g of angelica dahurica. Mix the patchouli, perilla leaves and angelica dahurica, mechanically pulverize and pass through a 20-mesh sieve to obtain mixed medicinal material powder. This mixed medicinal material powder is used as the raw material for subsequent hot water extraction, which can increase the contact area between the medicinal material and the solvent and improve the extraction efficiency of volatile oil and active ingredients. S2 Closed-loop pressurized superheated water extraction: The mixed medicinal powder obtained in step 1 is put into a 20L pressure-resistant extraction tank, and 10kg of purified water is added, with a material-to-liquid mass ratio of 1:10; the pressure-resistant extraction tank is sealed, and the stirring is turned on, with the mechanical stirring speed set to 80r / min; the temperature is raised to 115℃, so that the internal pressure of the pressure-resistant extraction tank is raised to 0.10MPa, and the extraction is carried out under constant temperature and pressure for 20 minutes under this superheated water condition to obtain the extracted mixture. S3 Differential Pressure Flash Evaporation and Volatile Oil Separation: After the extraction in step 2 is completed, heating is stopped, and the exhaust valve at the top of the pressure-resistant extraction tank is slightly opened to perform differential pressure flash evaporation. The water vapor mixture generated by differential pressure flash evaporation is discharged and cooled, and flows through the condenser to control the condensation temperature at 25°C to obtain a gas-liquid mixture. The gas-liquid mixture is allowed to stand and separate into layers, and then left to stand in an oil-water separator for 8 minutes. The upper oily substance is collected to obtain the volatile oil for Huoxiang Zhengqi Mixture. S4 Extract Collection and Compound Preparation: After pressure difference flash evaporation and depressurization in step 3, the remaining material in the pressure-resistant extraction tank is cooled to 50°C, filtered to remove the dregs, and the aqueous extract is collected; the aqueous extract and the volatile oil collected in step 3 are used as raw materials for Huoxiang Zhengqi Compound. Example 2:

[0014] The process steps in this embodiment are the same as those in Embodiment 1, except that the parameter settings are as follows; In S1, 500g of patchouli, 300g of perilla leaves, and 200g of angelica dahurica are weighed out respectively. The patchouli, perilla leaves, and angelica dahurica are mixed, mechanically pulverized, and passed through a 40-mesh sieve to obtain mixed medicinal powder. This mixed medicinal powder can increase the contact area between the medicinal materials and the solvent, and improve the subsequent extraction efficiency. In step S2, the mixed medicinal powder obtained in step 1 is put into a pressure-resistant extraction tank, and 8 kg of purified water is added, with a material-to-liquid ratio of 1:8. The pressure-resistant extraction tank is sealed, and the stirring is turned on at a speed of 60 r / min. The temperature is raised to 105℃, and the internal pressure of the pressure-resistant extraction tank is raised to 0.05 MPa. The mixture is extracted under these superheated water conditions at constant temperature and pressure for 40 minutes to obtain the extracted mixture. In S3, after the extraction in step 2 is completed, heating is stopped, and the exhaust valve at the top of the pressure-resistant extraction tank is slightly opened to perform differential flash evaporation. The water vapor mixture generated by differential flash evaporation is discharged and cooled. The condensation temperature is controlled at 30°C to obtain a gas-liquid mixture. The gas-liquid mixture is allowed to stand and separate into layers. After standing for 10 minutes, the upper oily substance is collected to obtain the volatile oil for Huoxiang Zhengqi Mixture. In step S4, the remaining material in the pressure-resistant extraction tank after pressure difference flash evaporation in step 3 is cooled to 55°C, the dregs are removed by filtration, and the aqueous extract is collected. The aqueous extract and the volatile oil collected in step 3 are used together as raw materials for Huoxiang Zhengqi Compound. Example 3:

[0015] The process steps in this embodiment are the same as those in Embodiment 1, except that the parameter settings are as follows; In S1, patchouli, perilla leaves and angelica are mixed. 500g of patchouli, 300g of perilla leaves and 200g of angelica are weighed and mechanically pulverized and passed through a 30-mesh sieve to obtain mixed medicinal powder. This mixed medicinal powder can increase the contact area between the medicinal materials and the solvent and improve the subsequent extraction efficiency. In step S2, the mixed medicinal powder obtained in step 1 is put into a pressure-resistant extraction tank, and 12 kg of purified water is added, with a material-to-liquid ratio of 1:12. The pressure-resistant extraction tank is sealed, and the stirring is turned on at a speed of 100 r / min. The temperature is raised to 120°C, and the internal pressure of the pressure-resistant extraction tank is raised to 0.15 MPa. The mixture is extracted under these superheated water conditions for 15 minutes at constant temperature and pressure to obtain the extracted mixture. In S3, after the extraction in step 2 is completed, heating is stopped, and the exhaust valve at the top of the pressure-resistant extraction tank is slightly opened to perform differential flash evaporation. The water vapor mixture generated by differential flash evaporation is discharged and cooled. The condensation temperature is controlled at 22°C to obtain a gas-liquid mixture. The gas-liquid mixture is allowed to stand and separate into layers. After standing for 6 minutes, the upper oily substance is collected to obtain the volatile oil for Huoxiang Zhengqi Mixture. In step S4, the remaining material in the pressure-resistant extraction tank after pressure difference flash evaporation in step 3 is cooled to 45°C, filtered to remove the dregs, and the aqueous extract is collected. The aqueous extract and the volatile oil collected in step 3 are used together as raw materials for Huoxiang Zhengqi Compound. Example 4:

[0016] The process steps in this embodiment are the same as those in Embodiment 1, except that the parameter settings are as follows; In S1, weigh out 5 kg of patchouli, 3 kg of perilla leaves and 2 kg of angelica dahurica, mix and grind them, and then pass them through a 40-mesh sieve. In S2, the mixed medicinal materials are put into a pressure-resistant extraction tank, and 15 times the amount of purified water is added. The stirring speed is set to 120 r / min. The mixture is heated to 130℃, the gauge pressure is 0.20 MPa, and the extraction is carried out at a constant temperature for 10 min. In S3, the condensation temperature is controlled at 20℃, and the oil-water separation is allowed to stand for 5 minutes. In S4, the mixture is cooled to 58°C and filtered to collect the aqueous extract, which is then used together with the volatile oil in the subsequent preparation of the compound.

[0017] Comparative Example 1: The difference between this comparative example and Example 1 is that the particle size of the medicinal materials in S1 is changed from a 20-mesh sieve to a 10-mesh sieve, while the other operating steps and process parameters are exactly the same as in Example 1.

[0018] Comparative Example 2: The difference between this comparative example and Example 1 is that the amount of purified water added in S2 is changed from 10 times the weight of the medicinal materials to 5 times. Other operating steps and process parameters are exactly the same as in Example 1.

[0019] Comparative Example 3: The difference between this comparative example and Example 1 is that the extraction conditions in S2 are changed from 115℃, 0.10MPa, 20min to 100℃, atmospheric pressure, 20min. The other operating steps and process parameters are exactly the same as in Example 1.

[0020] Comparative Example 4: The difference between this comparative example and Example 1 is that the extraction time in S2 is changed from 20 min to 60 min, while the other operating steps and process parameters are exactly the same as in Example 1.

[0021] Comparative Example 5: The difference between this comparative example and Example 1 is that the condensation temperature in S3 is changed from 25°C to 40°C, while the other operating steps and process parameters are exactly the same as in Example 1.

[0022] Comparative Example 6: The difference between this comparative example and Example 1 is that the operation of using the aqueous extract and volatile oil together as raw materials for Huoxiang Zhengqi Compound in S4 is omitted, and only the volatile oil is retained for subsequent preparation. Other operation steps and process parameters are exactly the same as in Example 1.

[0023] Performance Tests and Data Sheets: The total yield of volatile oil was calculated as a percentage of the mass of volatile oil to the total mass of the raw medicinal materials; the relative content of patchouli alcohol was determined by GC-MS and calculated using the normalization method of total ion chromatogram area; the availability of aqueous phase was calculated based on the proportion of the obtained aqueous extract actually incorporated into the compound preparation. The overall energy consumption (E) is evaluated using the converted values ​​of steam and electricity consumption per unit of feed mass. The calculation formula is as follows: Where ms is the steam consumption during the extraction process (kg), Hs is the steam enthalpy conversion factor (2.8 MJ / kg), We is the equipment power consumption (kWh), He is the electrical energy conversion factor (3.6 MJ / kWh), and M is the total mass of the medicinal materials fed (kg); the evaluation criteria are set as follows: MJ / kg is set as low; MJ / kg MJ / kg is set as medium to low; MJ / kg MJ / kg is set as medium; MJ / kg is set as high; Comparing the test results of Example 1 and Comparative Example 1 in the table, it can be seen that after changing the particle size of the medicinal material from 20 mesh to 10 mesh, the total yield of volatile oil decreased from 0.82% to 0.71%, and the relative content of patchouli alcohol decreased from 28.5% to 24.8%. The underlying reason is that when the particle size is too coarse, the surface area of ​​the medicinal material decreases, the path of hot water entering the plant tissue becomes longer, the cell wall softens due to heat and the release of cell contents is insufficient, resulting in increased resistance to the migration of volatile oil from the inside of the tissue to the outside. At the same time, components such as patchouli alcohol remain in the inside of the tissue, and the proportion carried out with flash evaporation decreases, thus reducing both the yield and the content of marker components. Comparing the test results of Example 1 and Comparative Example 2 in the table, it can be seen that after changing the material-liquid ratio from 1:10 to 1:5, the total yield of volatile oil decreased from 0.82% to 0.69%, and the relative content of patchouli alcohol decreased from 28.5% to 25.4%. The underlying reason is that when the liquid volume is insufficient, the degree of wetting of the medicinal materials in the tank decreases, the heat transfer in local areas is uneven, the effective contact area between the hot water and the medicinal powder decreases, and the dissolution and carrying efficiency of volatile oil decreases. At the same time, the viscosity of the system increases, the macroscopic convection formed by stirring weakens, resulting in a decrease in the mass transfer rate, thus the extraction result deteriorates. Comparing the test results of Example 1 and Comparative Example 3 in the table, it can be seen that after changing the extraction conditions from 115℃ and 0.10MPa to 100℃ and atmospheric pressure, the total yield of volatile oil decreased from 0.82% to 0.63%, and the relative content of patchouli alcohol decreased from 28.5% to 23.2%. The underlying reason is that the solubility of weakly polar volatile components in liquid water at atmospheric pressure (100℃) is lower than that in superheated water, and the turgor pressure formed inside the medicinal cell is also significantly weakened, resulting in insufficient opening of the cell structure and incomplete release of volatile oil. In addition, the amount of residual air in the system is higher under atmospheric pressure, and components such as patchouli alcohol are more prone to oxidation and loss, thus the yield and the content of marker components both decrease significantly. Comparing the test results of Example 1 and Comparative Example 4 in the table, it can be seen that extending the extraction time from 20 min to 60 min only reduced the total yield of volatile oil from 0.82% to 0.79%, but the relative content of patchouli alcohol decreased from 28.5% to 24.6%, and the overall energy consumption increased from low to high. The underlying reason is that extending the holding time did not significantly increase the total amount of extractable volatile oil, indicating that the main volatile oils were basically released at 20 min. Continued heating will cause some heat-sensitive terpenes and alcohols to undergo hydrolysis, isomerization, or oxidation, resulting in a decrease in the relative content of patchouli alcohol. At the same time, the increase in holding time leads to an increase in steam and stirring energy consumption, thus worsening the overall performance. Comparing the test results of Example 1 and Comparative Example 5 in the table, it can be seen that after increasing the condensation temperature from 25℃ to 40℃, the total yield of volatile oil decreased from 0.82% to 0.74%, and the relative content of patchouli alcohol decreased from 28.5% to 27.1%. The underlying reason is that when the condensation temperature is too high, the volatile components are not completely condensed, and some low-boiling-point aroma components cannot be fully liquefied and enter the oil-water separator, resulting in a decrease in the recovery of volatile oil. At the same time, the stratification rate at the oil-water interface slows down, and a small amount of volatile oil remains in the aqueous phase, thus reducing the yield. A comparison of the test results of Example 1 and Comparative Example 6 in the table shows that after omitting the aqueous extract and adding it to the mixture, the total yield of volatile oil and the relative content of patchouli alcohol remained basically unchanged, but the availability of the aqueous phase decreased from 100% to 0%. The aqueous phase obtained from S4 still contains soluble glycosides, flavonoids, and some dissolved aromatic components. These substances do not affect the volatile oil separation results, but they are directly related to the material utilization level and the composition of raw materials for subsequent formulations. Omitting this step will result in the loss of effective components in the aqueous phase, reduce the raw material utilization rate, and increase the burden of waste liquid treatment. Based on the data from various embodiments and comparative examples, it can be seen that closed superheated water extraction for 20 min at 20 mesh sieve, a material-to-liquid ratio of 1:10, 115℃ and 0.10 MPa, combined with 25℃ condensation and reuse of the aqueous extract, showed a relatively balanced performance in terms of volatile oil yield, patchouli alcohol retention and process resource utilization. Other embodiments within the range of 105℃ to 130℃, 0.05MPa to 0.20MPa, and 10 min to 40 min also achieved high yields and high content of marker components.

[0024] It should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and are not intended to limit it. Although the present invention has been described in detail with reference to preferred embodiments, those skilled in the art should understand that modifications or equivalent substitutions can be made to the technical solutions of the present invention without departing from the spirit and scope of the technical solutions of the present invention.

Claims

1. A rapid hot water extraction method for volatile oils from Huoxiang Zhengqi Compound, characterized in that, Includes the following steps: Step 1, Pre-treatment of medicinal materials: Mix patchouli, perilla leaves and angelica dahurica, mechanically pulverize and sieve to obtain mixed medicinal powder; Step 2, closed pressurized superheated water extraction: The mixed medicinal powder obtained in Step 1 is put into a pressure-resistant extraction tank and purified water is added; the pressure-resistant extraction tank is sealed, stirring is turned on, and the temperature is raised to 105℃~130℃, so that the internal pressure of the pressure-resistant extraction tank is raised to 0.05MPa~0.20MPa. Under this superheated water condition, the extraction is carried out at constant temperature and pressure for 10~40 minutes. Step 3, differential pressure flash evaporation and volatile oil collection: After the extraction in step 2 is completed, heating is stopped, and the exhaust valve at the top of the pressure-resistant extraction tank is slightly opened to perform differential pressure flash evaporation. The water vapor mixture generated by differential pressure flash evaporation is discharged and cooled to obtain a gas-liquid mixture. The gas-liquid mixture is allowed to stand and separate into layers, and the upper oily substance is collected to obtain the volatile oil for Huoxiang Zhengqi Compound. Step 4, Extract Collection and Compound Preparation: The remaining material in the pressure-resistant extraction tank after the pressure difference flash evaporation and depressurization in Step 3 is cooled to below 60°C, the dregs are removed by filtration, and the aqueous extract is collected; the aqueous extract and the volatile oil collected in Step 3 are used together as raw materials for Huoxiang Zhengqi Compound.

2. The method for rapid hot water extraction of volatile oil from Huoxiang Zhengqi Compound according to claim 1, characterized in that, In step 1, the weight ratio of patchouli, perilla leaf and angelica is 5:3:2; the sieving is done through a 20-40 mesh sieve.

3. The method for rapid hot water extraction of volatile oil from Huoxiang Zhengqi Compound according to claim 1, characterized in that, In step 2, the amount of purified water added is 8 to 15 times the weight of the mixed medicinal powder.

4. The method for rapid hot water extraction of volatile oil from Huoxiang Zhengqi Compound according to claim 1, characterized in that, In step 2, the stirring speed is set to 60~120 r / min.

5. The method for rapid hot water extraction of volatile oil from Huoxiang Zhengqi Compound according to claim 1, characterized in that, In step 3, the cooling temperature is controlled at 20℃~30℃; the settling time is 5~10 minutes.

6. The method for rapid hot water extraction of volatile oil from Huoxiang Zhengqi Compound according to claim 1, characterized in that, In step 2, the temperature is raised to 115°C, so that the internal pressure of the pressure-resistant extraction tank is raised to 0.10 MPa, and the extraction is carried out at constant temperature and pressure for 20 minutes.

7. The method for rapid hot water extraction of volatile oil from Huoxiang Zhengqi Compound according to claim 1, characterized in that, In step 2, the temperature is raised to 130°C, so that the internal pressure of the pressure-resistant extraction tank is raised to 0.20 MPa, and the extraction is carried out at constant temperature and pressure for 10 minutes.