CN105713732B - Extraction method of star anise oil - Google Patents

Abstract

The invention provides an extraction method of star anise oil. The invention adopts the process of firstly using the steam distillation method and then using the ethanol extraction method for operation, the method leads the anise oil remained in the aniseed after the steam distillation to be extracted by the ethanol extraction method, and realizes the secondary extraction and utilization of the effective components of the aniseed; meanwhile, the water vapor distillation can effectively remove impurities in the aniseed, so that the purity of the aniseed oil obtained by ethanol extraction at the later stage is improved, and the inherent defect of organic solvent extraction is overcome. The method can obviously improve the yield of the star anise oil, obtain the star anise oil with better quality, and is low in cost, convenient to implement and suitable for industrial mass production.

Description

Extraction method of star anise oil

Technical Field

The invention belongs to the technical field of natural product extraction, and particularly relates to an extraction method of star anise oil.

Background

In the compendium of materia medica, the star anise is dry mature fruit of the magnolia plant star anise, has the efficacies of dispelling wind and regulating qi, harmonizing stomach and regulating middle warmer, warming yang and dispelling cold, and regulating qi to alleviate pain, and is commonly used in traditional Chinese medicine for stomach cold vomiting, lumbago due to kidney deficiency, cold hernia and abdominal pain, and the like. The oleum Anisi Stellati can be extracted from dried fruits, branches and leaves, and the most important effective component in oleum Anisi Stellati is trans-anethole, also called anethole, with molecular formula C₁₀H₁₂And O is colorless transparent or light yellow liquid, has fennel-like aroma and sweet taste, is widely applied to the field of food production and processing such as candies, beverages, wine essences and the like, and scientific research shows that the product also has spectral antibacterial activity, can effectively remove DPPH-free radicals, and also has medicinal values of promoting gastrointestinal peristalsis, relieving cough caused by tracheitis and the like.

At present, the extraction method of the star anise oil is various, the traditional extraction method comprises a steam distillation method, a simultaneous distillation extraction method, an organic solvent extraction method and the like, and the newly developed new methods comprise a microwave extraction method and a supercritical CO extraction method₂Extraction methods, and the like. But in summary, the steam distillation method is still the most widely used extraction method at present due to good stability, low extraction cost and simple extraction method, but the yield of the method is relatively low; meanwhile, the distillation extraction method is a new volatile oil extraction technology developed in the sixties of the 20 th century, and is characterized in that two steps of steam distillation and solvent extraction of fractions of a sample are combined into one, the extraction steps are few, but special equipment with a special design and a complex structure is required in the method; although the organic solvent extraction method can improve the yield of the star anise oil to a certain extent, the obtained extract has more impurities and is not easy to separate and purify. Microwave extraction and supercritical CO emerging in recent years₂The extraction rule is important for the equipmentThe method has high yield and purity of the star anise oil, but the equipment is expensive and is not suitable for large-scale industrial production. Therefore, how to find an extraction process which has low cost, convenient implementation and higher anisic oil yield and purity becomes a difficult problem for the majority of researchers. The process comprehensively compares various extraction methods, improves and combines the process flow to a certain extent, adopts the process of firstly carrying out steam distillation and then carrying out ethanol extraction, and explores the optimal process conditions, although the price of 95 percent ethanol is relatively high, the ethanol can be recycled and recycled, and the production components can not be increased, so the process is a process which is convenient to implement, can obviously improve the extraction efficiency, and can fully utilize various active components in the aniseed.

Disclosure of Invention

Aiming at the defects of the prior art, the invention provides a method for extracting fennel oil by combining steam distillation and organic solvent extraction. The method can obviously improve the yield of the star anise oil, obtain the star anise oil with better quality, and meanwhile, the extraction method has low cost and convenient implementation and is suitable for industrial mass production.

In order to achieve the purpose, the invention adopts the following technical scheme:

a method for extracting star anise oil comprises the following steps:

(1) baking and drying the aniseed until the water content is 2% -7%, and then crushing the aniseed into powder of 60-70 meshes;

(2) adding water into the aniseed powder obtained in the step (1) and uniformly mixing, wherein the mass ratio of the added water to the aniseed powder is 8-12: 1;

(3) distilling the aniseed powder water mixed liquor obtained in the step (2) by adopting a steam distillation method, wherein the distillation temperature is 80-120 ℃, and the distillation time is 2-5, removing distilled impurities, and collecting distillate;

(4) adding analytically pure sodium chloride into the distillate obtained in the step (3) until white sodium chloride solid appears in the distillate, promoting oil-water stratification, and collecting an upper oil layer to obtain the fennel essential oil;

(5) collecting the aniseed powder extracted by steam distillation in the step (3), drying again, and performing Soxhlet extraction by using ethanol as a solvent at the extraction temperature of 60-90 ℃ for 4-6 hours to obtain an extract;

(6) and (5) recovering the ethanol in the extract to obtain the fennel extract oil.

Preferably, the anise is baked and dried in the step (1) until the water content is 3% -5%.

Preferably, the mass ratio of the water and the anise powder added in the step (2) is 9-11: 1.

Preferably, the distillation temperature in the step (3) is 90-110 ℃, and the distillation time is 3-4 hours.

Preferably, the extraction temperature in step (5) is 70-80 ℃ and the extraction time is 3-5 hours.

Preferably, the ethanol concentration in the step (5) is 75-95%.

Preferably, the method for extracting the star anise oil comprises the following steps:

(1) baking and drying the star anise until the water content is 4%, and then crushing the star anise into powder of 60 meshes;

(2) adding water into the aniseed powder obtained in the step (1) and uniformly mixing, wherein the mass ratio of the added water to the aniseed powder is 10: 1;

(3) distilling the aniseed powder water mixed liquor obtained in the step (2) by adopting a steam distillation method, wherein the distillation temperature is 105 ℃, the distillation time is 4 hours, removing distilled impurities, and collecting distillate;

(4) adding analytically pure sodium chloride into the distillate obtained in the step (3) until white sodium chloride solid appears in the distillate, promoting oil-water stratification, and collecting an upper oil layer to obtain the fennel essential oil;

(5) collecting the aniseed powder extracted by steam distillation in the step (3), drying again, and performing Soxhlet extraction by using 95% ethanol as a solvent, wherein the extraction temperature is 78 ℃, and the extraction time is 4.5 hours, so as to obtain an extract;

(6) and (5) recovering the ethanol in the extract to obtain the fennel extract oil.

Compared with the prior art, the invention has the remarkable advantages that:

(1) the invention adopts the process of firstly carrying out the steam distillation method and then carrying out the ethanol extraction method, has simple process, is convenient to implement and does not need expensive equipment.

(2) Compared with the traditional extraction method, the yield is obviously improved, the anise oil remaining in the aniseed after steam distillation is extracted by an ethanol extraction method, and the secondary extraction and utilization of the effective components of the aniseed are realized; meanwhile, the impurities in the aniseed can be effectively removed by steam distillation, so that the purity of the aniseed oil obtained by ethanol extraction at the later stage is obviously improved.

(3) The method does not add any toxic and harmful solvent, prevents chemical residues harmful to human bodies and environmental pollution in the processing process, can recycle and reuse the ethanol used in the ethanol extraction method, saves resources, effectively reduces the production cost, and is suitable for industrial large-scale production and application.

Drawings

FIG. 1 is a gas chromatogram of anise essential oil obtained by steam distillation in example 1;

FIG. 2 is a gas chromatogram of an oil extract of Illicium verum obtained by Soxhlet extraction in example 1;

FIG. 3 is a gas chromatogram of anise essential oil obtained by steam distillation in comparative example 1;

FIG. 4 is a gas chromatogram of an extract oil of Illicium verum obtained by Soxhlet extraction in comparative example 2;

FIG. 5 is a gas chromatogram of an extract oil of Illicium verum obtained by Soxhlet extraction in comparative example 3;

FIG. 6 is a gas chromatogram of anise essential oil obtained by steam distillation in comparative example 3;

FIG. 7 is a gas chromatogram of anise oil obtained in comparative example 4 by simultaneous distillation and extraction.

Detailed Description

The present invention will be further described with reference to examples, but the following description is only for the purpose of explaining the present invention and does not limit the contents thereof.

Example 1

Baking and drying fructus Anisi Stellati until the water content is 2%, pulverizing with a pulverizer, sieving with a 60-mesh sieve, weighing 100g fructus Anisi Stellati powder with an electronic scale, adding 1200mL water, mixing, placing in a steam receiving bottle of a steam distillation device, distilling at 80 deg.C for 5 hr, removing distilled impurities, collecting distillate, adding analytically pure sodium chloride until white sodium chloride solid appears in the water phase, allowing oil and water to separate into layers, absorbing upper oil layer to obtain 5.74g fructus Anisi Stellati essential oil, placing in a brown bottle, keeping the yield of 5.74%, discarding the water phase in the steam receiving bottle of the steam distillation device, collecting lower residue, directly pouring into a tray, oven drying to obtain 71g residue, placing in an extraction tube of a Soxhlet extractor, adding 70% ethanol, extracting until the residue does not pass through a siphon tube, extracting at 60 deg.C for 6h, collecting distillate, and recovering the ethanol to obtain 13g of anise extract oil, and placing the anise extract oil in a brown bottle for storage and later use, wherein the yield is 18.31 percent. Detecting the components of fructus Anisi Stellati essential oil and fructus Anisi Stellati extract oil by gas chromatography, wherein the detection results are shown in fig. 1 and 2, the essential oil contains anethole 82.7%, and the extract oil contains anethole 31.2%.

Example 2

Baking and drying fructus Anisi Stellati until the water content is 5%, pulverizing with a pulverizer, sieving with a 60-mesh sieve, weighing 200g fructus Anisi Stellati powder with an electronic scale, adding 2200mL water, mixing, placing in a steam receiving bottle of a steam distillation device, distilling at 90 deg.C for 3 hr, removing distilled impurities, collecting distillate, adding analytically pure sodium chloride until white sodium chloride solid appears in the water phase, allowing oil and water to separate into layers, absorbing upper oil layer to obtain 11.62g fructus Anisi Stellati essential oil, placing in a brown bottle, keeping the yield of 5.81%, discarding the water phase in the steam receiving bottle of the steam distillation device, collecting lower residue, directly pouring into a tray, oven drying to obtain 141g residue, placing in an extraction tube of a Soxhlet extractor, adding 80% ethanol, extracting until the residue does not pass through a siphon tube, extracting at 70 deg.C for 5 hr, collecting distillate, 26.4g of anise oil is obtained after the ethanol is recycled, and the anise oil is placed in a brown bottle for storage and standby, wherein the yield is 18.72%. Detecting the material components of the essential oil of the star anise and the extracted oil of the star anise by using gas chromatography, wherein the essential oil contains 81.3 percent of anethole and the extracted oil contains 30.7 percent of anethole.

Example 3

Baking and drying fructus Anisi Stellati until the water content is 4%, pulverizing with a pulverizer, sieving with a 60-mesh sieve, weighing 150g fructus Anisi Stellati powder with an electronic scale, adding 1500mL water, mixing, placing in a steam receiving bottle of a steam distillation device, distilling at 105 deg.C for 4 hr, removing distilled impurities, collecting distillate, adding analytically pure sodium chloride until white sodium chloride solid appears in water phase, allowing oil and water to separate into layers, absorbing upper oil layer to obtain 8.83g fructus Anisi Stellati essential oil, placing in a brown bottle, keeping the yield of 5.89%, discarding water phase in the steam receiving bottle of the steam distillation device, collecting lower residue, directly pouring into a tray, oven drying, collecting dried residue to obtain 108g, placing in an extraction tube of a Soxhlet extractor, adding 95% ethanol, extracting without siphon tube, extracting at 78 deg.C for 4.5 hr, collecting effluent, and recovering the ethanol to obtain 20.48g of anise extract oil, and placing the anise extract oil in a brown bottle for storage for later use, wherein the yield is 18.96%. Detecting the material components of the essential oil of the star anise and the extracted oil of the star anise by using gas chromatography, wherein the essential oil contains 82.9 percent of anethole and the extracted oil contains 30.6 percent of anethole.

Example 4

Baking and drying fructus Anisi Stellati until the water content is 3%, pulverizing with a pulverizer, sieving with a 70 mesh sieve, weighing 100g fructus Anisi Stellati powder with an electronic scale, adding 900mL water, mixing, placing in a steam receiving bottle of a steam distillation device, distilling at 120 deg.C for 2 hr, removing distilled impurities, collecting distillate, adding analytically pure sodium chloride until white sodium chloride solid appears in the water phase, allowing oil and water to separate into layers, absorbing upper oil layer to obtain 5.92g fructus Anisi Stellati essential oil, placing in a brown bottle, keeping the yield of 5.92%, discarding the water phase in the steam receiving bottle of the steam distillation device, collecting lower residue, directly pouring into a tray, oven drying, collecting dried residue to obtain 72g, placing in an extraction pipe of a Soxhlet extractor, adding 75% ethanol, extracting until the residue does not pass through a siphon, extracting at 80 deg.C for 5 hr, collecting distillate, and recovering the ethanol to obtain 13.62g of anise extract oil, and placing the anise extract oil in a brown bottle for storage for later use, wherein the yield is 18.92%. Detecting the material components of the essential oil of the star anise and the extracted oil of the star anise by using gas chromatography, wherein the essential oil contains 82.9 percent of anethole and the extracted oil contains 30.9 percent of anethole.

Example 5

Baking and drying fructus Anisi Stellati until the water content is 7%, pulverizing with a pulverizer, sieving with a 70-mesh sieve, weighing 200g fructus Anisi Stellati powder with an electronic scale, adding 1600mL water, mixing, placing in a steam receiving bottle of a steam distillation device, distilling at 100 deg.C for 3.5 hr, removing distilled impurities, collecting distillate, adding analytically pure sodium chloride until white sodium chloride solid appears in water phase, layering oil and water, absorbing upper oil layer to obtain 11.52g oleum Anisi Stellati, placing in a brown bottle, keeping for use, with yield of 5.76%, discarding water phase in the steam receiving bottle of the steam distillation device, collecting lower residue, directly pouring into a tray, oven drying, collecting residue to obtain 143g, placing in an extraction tube of a Soxhlet extractor, adding 70% ethanol, extracting until the residue is submerged in a siphon tube, extracting at 90 deg.C for 4 hr, collecting distillate, 26.75g of anise oil is obtained after the ethanol is recycled, and the anise oil is placed in a brown bottle for storage and standby, and the yield is 18.75 percent. Detecting the material components of the essential oil of the star anise and the extracted oil of the star anise by using gas chromatography, wherein the essential oil contains 82.4 percent of anethole and the extracted oil contains 31.3 percent of anethole.

Comparative example 1

Baking and drying the star anise fruits until the water content is 2%, crushing the star anise fruits by a crusher, sieving the star anise fruits by a 60-mesh sieve, weighing 100g of star anise powder by an electronic scale, adding 1200mL of water into the star anise powder, uniformly mixing the star anise powder and the water, placing the mixture into a steam receiving bottle in a steam distillation device to start distillation at the distillation temperature of 80 ℃ for 5h, removing distilled impurities, collecting distillate, adding analytically pure sodium chloride until white sodium chloride solid appears in a water phase, layering oil and water, absorbing an upper oil layer to obtain 5.72g of star anise essential oil, placing the star anise essential oil in a brown bottle for storage, wherein the yield is 5.72%, detecting the material components of the star anise essential oil by using a gas chromatography, and detecting the result is shown in figure 3, and the essential oil.

However, in comparison with example 1, comparative example 1, which uses only steam distillation, cannot extract the anise oil remaining in the aniseed, and the total yield is not high.

Comparative example 2

Baking and drying the aniseed fruits until the water content is 2%, crushing the aniseed fruits by a crusher, sieving the crushed aniseed fruits by a 60-mesh sieve, weighing 100g of aniseed powder by an electronic scale, placing the aniseed powder into an extraction tube of a Soxhlet extractor, adding 70% ethanol for extraction until the powder does not pass through a siphon, extracting the powder for 6 hours at 60 ℃, collecting distillate, recovering the ethanol to obtain 21.5g of aniseed extraction oil, and placing the aniseed extraction oil into a brown bottle for storage for later use, wherein the yield is 21.5%. The extract oil of fructus Anisi Stellati contains anethole 36.7% as shown in FIG. 4.

Compared with the example 1, the comparative example 2 only uses ethanol as a solvent to carry out Soxhlet extraction, the yield and the anisic acid brain component contained in the extracted oil are slightly improved, but the total yield is still not as good as the example 1, and the gas chromatography detection analysis is used, so that the components in the extracted oil are very complex, and a large amount of unidentifiable substances exist, which means that the impurity types are many, the content is high, and the further separation and purification of the effective component of the anise oil are not favorably realized.

Comparative example 3

Baking and drying the aniseed fruits until the water content is 2%, crushing the aniseed fruits by a crusher, sieving the crushed aniseed fruits by a 60-mesh sieve, weighing 100g of aniseed powder by an electronic scale, placing the aniseed powder into an extraction tube of a Soxhlet extractor, adding 70% ethanol for extraction until the powder does not pass through a siphon, extracting the powder for 6 hours at 60 ℃, collecting distillate, recovering the ethanol to obtain 22.3g of aniseed extraction oil, and placing the aniseed extraction oil into a brown bottle for storage for later use, wherein the yield is 22.3%. The extract oil of fructus Anisi Stellati contains anethole 36.2% as shown in FIG. 5. Collecting fructus Anisi Stellati residue, directly pouring into tray, oven drying, collecting dried residue 59g, adding 708mL of water, mixing the two, placing in steam receiving bottle of steam distillation device, distilling at 80 deg.C for 5 hr, removing distilled impurities, collecting distillate, adding analytically pure sodium chloride until white sodium chloride solid appears in water phase, allowing oil and water to separate, absorbing upper oil layer to obtain fructus Anisi Stellati essential oil 1.03g, placing in brown bottle, storing, with yield of 1.74%, detecting substance components of fructus Anisi Stellati essential oil with gas chromatography, and detecting result shown in FIG. 6, wherein the essential oil contains fructus Anisi Stellati brain 72.8%.

Compared with the example 1, the ethanol is used as the solvent for the soxhlet extraction, and then the steam distillation is carried out, so that the yield and the purity of the fennel oil by the later steam distillation method are both obviously reduced, and the direct soxhlet extraction is not carried out in the earlier stage, so that the extracted volatile oil has various impurity types and high content, and the further separation and purification of the effective components of the fennel oil are not facilitated as compared with the comparative example 2.

Comparative example 4

Baking and drying fructus Anisi Stellati to water content of 2%, pulverizing with pulverizer, sieving with 60 mesh sieve, weighing fructus Anisi Stellati powder 100g with electronic scale, adding water 1200mL, distilling and extracting one end of the apparatus, adding 70% ethanol into the other end of the apparatus, distilling and extracting for 10 hr, recovering ethanol solvent to obtain oleum Anisi Stellati 6.72g, detecting the components with gas chromatography, and determining that oleum Anisi Stellati contains 82.5% of anethole

Compared with the embodiment 1, the total yield of the anise oil extracted by distillation is not high, and the purity is not obviously increased. In fact, the essence of the simultaneous distillation and extraction method is that a sample is only subjected to steam distillation all the time, and the volatilized fraction is dissolved in the extracting agent, specifically, in the comparative example, the star anise is subjected to steam distillation all the time, volatile components such as the fennel oil are distilled out and then volatilized to a condensation pipe to be dissolved in ethanol to complete the extraction process, and the star anise as a raw material does not directly contact with the ethanol, which is fundamentally different from the application.

Although the specific embodiments of the present invention have been described with reference to the examples, the scope of the present invention is not limited thereto, and those skilled in the art will appreciate that various modifications and variations can be made without inventive effort by those skilled in the art based on the technical solution of the present invention.

Claims (4)

1. The extraction method of star anise oil is characterized by comprising the following steps:

(1) baking and drying the aniseed until the water content is 3% -5%, and then crushing the aniseed into powder of 60-70 meshes;

(2) adding water into the aniseed powder obtained in the step (1) and uniformly mixing, wherein the mass ratio of the added water to the aniseed powder is 8-12: 1;

(3) distilling the aniseed powder water mixed liquor obtained in the step (2) by adopting a steam distillation method, wherein the distillation temperature is 80-120 ℃, the distillation time is 2-5 hours, removing distilled impurities, and collecting distillate;

(4) adding analytically pure sodium chloride into the distillate obtained in the step (3) until white sodium chloride solid appears in the distillate, promoting oil-water stratification, and collecting an upper oil layer to obtain the fennel essential oil;

(5) collecting the aniseed powder extracted by steam distillation in the step (3), drying again, and performing Soxhlet extraction by using ethanol as a solvent at the extraction temperature of 70-80 ℃ for 3-5 hours to obtain an extract; the concentration of the ethanol is 75-95%;

(6) and (5) recovering the ethanol in the extract to obtain the fennel extract oil.

2. The method for extracting star anise oil according to claim 1, wherein the mass ratio of the water and star anise powder added in the step (2) is 9-11: 1.

3. the method for extracting star anise oil according to claim 1, wherein the distillation temperature in the step (3) is 90 to 110 ℃ and the distillation time is 3 to 4 hours.

4. The method for extracting star anise oil as claimed in claim 1, wherein the method for extracting star anise oil comprises the following steps:

(1) baking and drying the star anise until the water content is 4%, and then crushing the star anise into powder of 60 meshes;

(2) adding water into the aniseed powder obtained in the step (1) and uniformly mixing, wherein the mass ratio of the added water to the aniseed powder is 10: 1;

(3) distilling the aniseed powder water mixed liquor obtained in the step (2) by adopting a steam distillation method, wherein the distillation temperature is 105 ℃, the distillation time is 4 hours, removing distilled impurities, and collecting distillate;

(4) adding analytically pure sodium chloride into the distillate obtained in the step (3) until white sodium chloride solid appears in the distillate, promoting oil-water stratification, and collecting an upper oil layer to obtain the fennel essential oil;

(5) collecting the aniseed powder extracted by steam distillation in the step (3), drying again, and performing Soxhlet extraction by using 95% ethanol as a solvent, wherein the extraction temperature is 78 ℃, and the extraction time is 4.5 hours, so as to obtain an extract;

(6) and (5) recovering the ethanol in the extract to obtain the fennel extract oil.

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