CN111718799A - Method for extracting pepper leaf essential oil by eutectic solvent method and ultrasonic-assisted distillation - Google Patents
Method for extracting pepper leaf essential oil by eutectic solvent method and ultrasonic-assisted distillation Download PDFInfo
- Publication number
- CN111718799A CN111718799A CN202010623162.6A CN202010623162A CN111718799A CN 111718799 A CN111718799 A CN 111718799A CN 202010623162 A CN202010623162 A CN 202010623162A CN 111718799 A CN111718799 A CN 111718799A
- Authority
- CN
- China
- Prior art keywords
- essential oil
- eutectic solvent
- ultrasonic
- extracting
- pepper
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11B—PRODUCING, e.g. BY PRESSING RAW MATERIALS OR BY EXTRACTION FROM WASTE MATERIALS, REFINING OR PRESERVING FATS, FATTY SUBSTANCES, e.g. LANOLIN, FATTY OILS OR WAXES; ESSENTIAL OILS; PERFUMES
- C11B9/00—Essential oils; Perfumes
- C11B9/02—Recovery or refining of essential oils from raw materials
- C11B9/025—Recovery by solvent extraction
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11B—PRODUCING, e.g. BY PRESSING RAW MATERIALS OR BY EXTRACTION FROM WASTE MATERIALS, REFINING OR PRESERVING FATS, FATTY SUBSTANCES, e.g. LANOLIN, FATTY OILS OR WAXES; ESSENTIAL OILS; PERFUMES
- C11B9/00—Essential oils; Perfumes
- C11B9/02—Recovery or refining of essential oils from raw materials
- C11B9/027—Recovery of volatiles by distillation or stripping
Abstract
The invention discloses a method for extracting pepper leaf essential oil by an ultrasonic-assisted distillation method through a eutectic solvent method, wherein a hydrogen bond acceptor HBA and a hydrogen bond donor HBD in a certain molar ratio form a eutectic solvent DES, and the eutectic solvent DES is used for extracting the essential oil in pepper leaves by the ultrasonic-assisted distillation method; the method mainly comprises the following steps: cleaning, drying and crushing fresh pepper leaves; preparing a eutectic solvent DES; thirdly, carrying out ultrasonic auxiliary treatment on the eutectic solvent DES and pepper leaf powder; and fourthly, extracting the pepper leaf essential oil. The invention has the beneficial effects that: the optimal extraction process conditions for response surface optimization of the method are as follows: the choline chloride-urea eutectic solvent is used as an optimal extracting agent, the liquid-material ratio is 14:1(mL/g), the ultrasonic power is 300W, and the distillation time is 53 min. The extraction method is simple, and improves yield of pepper leaf essential oil; the essential oil components are analyzed by adopting a gas chromatography-mass spectrometry method, a new thought is provided for an essential oil extraction method, and the application range of DES is expanded.
Description
Technical Field
The invention relates to a method for extracting plant essential oil, in particular to a method for extracting pepper leaf essential oil by a eutectic solvent method and ultrasonic-assisted distillation.
Background
Pepper (pepper nigrum L.) is a perennial evergreen flowering vine of the genus Piper of the family piperiaceae, a characteristic agricultural product of Hainan, and accounts for more than 90% of the total pepper yield in China. In the traditional medical field, pepper is a very widely used drug. Local people in thailand can purchase pepper leaves and stems on the market, indicating that pepper leaves can be used to treat certain diseases. The essential oil has antioxidant and antibacterial activities, and can be used for food preservation and in cosmetic industry. In addition, the essential oil has abundant chemical components and certain health care effects, such as anti-inflammation, blood circulation promotion and blood stasis removal.
At present, the research on the pepper essential oil is mainly focused on pepper leaves and pepper fruits, and some organizations and people research and test the extraction of the essential oil from the pepper leaves. The current methods which are relatively common mainly comprise: firstly, the pepper leaf essential oil is extracted by adopting a steam distillation method, and the yield of the essential oil is 1.25 percent; secondly, extracting the essential oil of the piper nigrum leaves by adopting a solvent extraction method, wherein the yield of the essential oil is 0.405%; thirdly, supercritical CO is adopted2Extracting black pepper essential oil, wherein the yield of the essential oil is 7.02%; fourthly, the white pepper essential oil is extracted by adopting an ultrasonic microwave synergistic technology, and the yield of the white pepper fruit essential oil is relatively higher than 3.80 percent. However, steam distillation, solvent extraction, supercritical CO2The traditional methods such as the extraction method and the like have high processing cost and overlong extraction time, so that the search for an extraction method which has low cost, short extraction time and environmental protection is necessary.
Abbott et al discovered a novel, green and low melting ionic solvent consisting of a molar ratio of Hydrogen Bond Acceptors (HBAs), such as quaternary ammonium salts, to Hydrogen Bond Donors (HBDs), such as carboxylic acids, polyols. The eutectic solvent (DES) has good thermal stability and low volatility, and especially has the advantages of easy degradability, simple preparation, low cost and the like.
Disclosure of Invention
The invention provides a method for extracting pepper leaf essential oil by ultrasonic-assisted distillation through a eutectic solvent method, which is designed for solving the technical problems.
The technical scheme adopted by the invention for solving the technical problems is as follows:
a method for extracting pepper leaf essential oil by ultrasonic-assisted distillation with a eutectic solvent method comprises the steps of forming a eutectic solvent DES by a hydrogen bond acceptor HBA and a hydrogen bond donor HBD according to a certain molar ratio, and extracting the essential oil in pepper leaves by ultrasonic-assisted distillation with the eutectic solvent DES; the method mainly comprises the following steps:
cleaning fresh pepper leaves, drying in an electric heating air blast drying oven at 40-80 ℃ to constant weight, crushing and sieving into pepper leaf powder of 30-80 meshes, and drying in a dryer for later use;
secondly, preparing a eutectic solvent DES, mixing, heating and stirring the hydrogen bond acceptor HBA and the hydrogen bond donor HBD in a constant warm water bath kettle at 70-90 ℃ for 30-120 minutes until a uniform colorless transparent liquid eutectic solvent DES is formed;
mixing the eutectic solvent DES and the pepper leaf powder according to a ratio of liquid-material ratio in a range of 5:1 to 25:1(mL/g), adding distilled water, and treating in an ultrasonic cleaning machine to make the mixture subjected to ultrasonic radiation;
and fourthly, extracting the pepper leaf essential oil from the mixture subjected to ultrasonic auxiliary treatment in the eutectic solvent DES through steam distillation, separating the liquid, and then adding anhydrous sodium sulfate for drying to obtain the pepper leaf essential oil.
According to the method for extracting the pepper leaf essential oil by the deep eutectic solvent method and ultrasonic-assisted distillation, the hydrogen bond receptor HBA is choline chloride.
The method for extracting the pepper leaf essential oil by the ultrasonic-assisted distillation through the eutectic solvent method is characterized in that the hydrogen bond donor HBD is one of quaternary ammonium salts of glycerol, glycol, lactic acid, urea or glucose.
The method for extracting the pepper leaf essential oil by ultrasonic-assisted distillation through the eutectic solvent method is characterized in that the eutectic solvent DES is one of the following mixtures in molar ratio:
a mixture of choline chloride and glycerol in a molar ratio of 1: 2;
a mixture of choline chloride and ethylene glycol in a molar ratio of 1: 4;
a mixture of choline chloride and lactic acid in a molar ratio of 1: 2;
a mixture of choline chloride and urea in a molar ratio of 1: 2;
a mixture of choline chloride and glucose in a molar ratio of 2: 1.
The method for extracting the pepper leaf essential oil by the ultrasonic-assisted distillation through the eutectic solvent method comprises the following steps of drying in an electric heating air blowing drying oven at the temperature of 60 ℃, crushing pepper leaf powder and sieving the crushed pepper leaf powder into 50 meshes.
In the second step, the hydrogen bond acceptor HBA and the hydrogen bond donor HBD are mixed, heated and stirred in a water bath kettle at the constant temperature of 80 ℃ for 30-120 minutes until a uniform, colorless and transparent liquid eutectic solvent DES is formed.
In the third step, the mixture is mixed according to a ratio of the eutectic solvent DES to pepper leaf powder within a range of 10:1 to 15:1 (mL/g).
In the step III, the power intensity of the ultrasonic wave is 100-500W; in the step IV, the distillation time for extracting the pepper leaf essential oil by steam distillation is 30-70 minutes.
In the third step, the power intensity of the ultrasonic wave is 300W; in the step IV, the distillation time for extracting the pepper leaf essential oil by steam distillation is 50-55 minutes.
In the third step, the eutectic solvent DES is a mixture of choline chloride and urea in a molar ratio of 1:2, the eutectic solvent DES and pepper leaf powder are mixed according to a liquid-material ratio of 14.36:1(mL/g), and the power intensity of the ultrasonic wave is 300W; in the step IV, the distillation time for extracting the pepper leaf essential oil by steam distillation is 53 minutes.
The invention has the beneficial effects that: an eutectic solvent is used as an extracting agent, pepper leaf essential oil is extracted by adopting an ultrasonic-assisted steam distillation method, three factors, namely liquid-material ratio, ultrasonic power and distillation time, which have great influence on the extraction process of the pepper leaf essential oil are optimized by applying a response method, and the optimal extraction condition is obtained. The essential oil components are analyzed by adopting a gas chromatography-mass spectrometry method, a new thought is provided for an essential oil extraction method, and the application range of DES is expanded.
Drawings
FIG. 1 is a graph showing the effect of different types of DES on the yield of essential oil; note that different letters a-d represent significant differences (p < 0.05).
FIG. 2 is a graph showing the influence of liquid-material ratio on the yield of essential oil;
FIG. 3 is a graph showing the influence of ultrasonic power on the yield of essential oil;
FIG. 4 is a graph showing the effect of distillation time on the yield of essential oil;
FIG. 5 is a response surface diagram of the interaction effect of liquid-to-material ratio and ultrasonic power on the yield of pepper leaf essential oil;
FIG. 6 is a response surface graph showing the interaction between the liquid-to-material ratio and the distillation time on the yield of the pepper leaf essential oil;
FIG. 7 is a graph of the response surface of the interaction of ultrasonic power and distillation time on the yield of pepper leaf essential oil.
Detailed Description
The invention is further illustrated with reference to the following figures and examples.
Example (b):
the invention relates to a method for extracting pepper leaf essential oil by ultrasonic-assisted distillation through a eutectic solvent method, which is characterized in that a hydrogen bond acceptor HBA and a hydrogen bond donor HBD in a certain molar ratio form a eutectic solvent DES, and the eutectic solvent DES is used for extracting the essential oil in pepper leaves by ultrasonic-assisted distillation; the method mainly comprises the following steps:
cleaning fresh pepper leaves, drying in an electric heating air blast drying oven at 40-80 ℃ to constant weight, crushing and sieving into pepper leaf powder of 30-80 meshes, and drying in a dryer for later use;
secondly, preparing a eutectic solvent DES, mixing, heating and stirring the hydrogen bond acceptor HBA and the hydrogen bond donor HBD in a constant warm water bath kettle at 70-90 ℃ for 30-120 minutes until a uniform colorless transparent liquid eutectic solvent DES is formed;
mixing the eutectic solvent DES and the pepper leaf powder according to a ratio of liquid-material ratio in a range of 5:1 to 25:1(mL/g), adding distilled water, and treating in an ultrasonic cleaning machine to make the mixture subjected to ultrasonic radiation;
and fourthly, extracting the pepper leaf essential oil from the mixture subjected to ultrasonic auxiliary treatment in the eutectic solvent DES through steam distillation, separating the liquid, and then adding anhydrous sodium sulfate for drying to obtain the pepper leaf essential oil.
According to the method for extracting the pepper leaf essential oil by the deep eutectic solvent method and ultrasonic-assisted distillation, the hydrogen bond receptor HBA is choline chloride.
The method for extracting the pepper leaf essential oil by the ultrasonic-assisted distillation through the eutectic solvent method is characterized in that the hydrogen bond donor HBD is one of quaternary ammonium salts of glycerol, glycol, lactic acid, urea or glucose.
The method for extracting the pepper leaf essential oil by ultrasonic-assisted distillation through the eutectic solvent method is characterized in that the eutectic solvent DES is one of the following mixtures in molar ratio:
a mixture of choline chloride and glycerol in a molar ratio of 1: 2;
a mixture of choline chloride and ethylene glycol in a molar ratio of 1: 4;
a mixture of choline chloride and lactic acid in a molar ratio of 1: 2;
a mixture of choline chloride and urea in a molar ratio of 1: 2;
a mixture of choline chloride and glucose in a molar ratio of 2: 1.
The method for extracting the pepper leaf essential oil by the ultrasonic-assisted distillation through the eutectic solvent method comprises the following steps of drying in an electric heating air blowing drying oven at the temperature of 60 ℃, crushing pepper leaf powder and sieving the crushed pepper leaf powder into 50 meshes.
In the second step, the hydrogen bond acceptor HBA and the hydrogen bond donor HBD are mixed, heated and stirred in a water bath kettle at the constant temperature of 80 ℃ for 30-120 minutes until a uniform, colorless and transparent liquid eutectic solvent DES is formed.
In the third step, the mixture is mixed according to a ratio of the eutectic solvent DES to pepper leaf powder within a range of 10:1 to 15:1 (mL/g).
In the step III, the power intensity of the ultrasonic wave is 100-500W; in the step IV, the distillation time for extracting the pepper leaf essential oil by steam distillation is 30-70 minutes.
In the third step, the power intensity of the ultrasonic wave is 300W; in the step IV, the distillation time for extracting the pepper leaf essential oil by steam distillation is 50-55 minutes.
In the third step, the eutectic solvent DES is a mixture of choline chloride and urea in a molar ratio of 1:2, the eutectic solvent DES and pepper leaf powder are mixed according to a liquid-material ratio of 14.36:1(mL/g), and the power intensity of the ultrasonic wave is 300W; in the step IV, the distillation time for extracting the pepper leaf essential oil by steam distillation is 53 minutes.
Experimental procedures and data analysis
1 materials and methods
1.1 materials and apparatus
The material is pepper leaf of yellow bamboo town of Ding' an county, Hainan province;
the equipment comprises: a numerical control ultrasonic cleaner, a pulverizer, a constant temperature air-blast drying box, an analytical balance, a JB volatile oil determinator and an AMD10 gas chromatography-mass spectrometer.
1.2 Experimental methods
1.2.1 sample pretreatment
Cleaning fresh pepper leaves, drying in an electrothermal blowing dry box at 60 ℃ to a constant weight, crushing, sieving (50 meshes), and drying in a dryer for later use. Preparing DES, mixing HBA (choline chloride) and HBD in 80 deg.C water bath, heating and stirring for 0.5-2 hr until uniform colorless transparent liquid is formed. Different types of DES were prepared according to table 1.
Table 1: DES of different types
| Numbering | HBA | HBD | Molar ratio of |
| DES-1 | Choline chloride | Glycerol | 1:2 |
| DES-2 | Choline chloride | Ethylene glycol | 1:4 |
| DES-3 | Choline chloride | Lactic acid | 1:2 |
| DES-4 | Choline chloride | Urea | 1:2 |
| DES-5 | Choline chloride | Glucose | 2:1 |
1.2.2 extraction of essential oil from pepper leaves
Accurately weighing 30g of pepper leaf powder, adding a certain amount of DES (data encryption standard) into a 500mL round-bottom flask, adding distilled water according to the liquid-material ratio for ultrasonic auxiliary treatment, then performing steam distillation to extract pepper leaf essential oil, adding anhydrous sodium sulfate for drying after liquid separation, weighing and calculating the yield of the pepper leaf essential oil.
Yield (%) of pepper leaf essential oil (weight of extracted essential oil/weight of dry pepper leaf powder) × 100
1.2.3 Effect of different types of DES on essential oil yield
According to the table 1, pepper leaf powder is extracted by 5 DES of different types, the extraction effect of 5 DES on essential oil is analyzed according to the yield of pepper leaf essential oil, and the DES with the best extraction effect is selected for subsequent single-factor experiment
1.2.4 Single factor experiment
Extracting the pepper leaf essential oil by a method of 1.2.2 under the following extraction conditions: keeping the factors of ultrasonic power 300W and distillation time 50min unchanged, and comparing the influence of different liquid-material ratios (5:1, 10:1, 15:1, 20:1 and 25:1) on the yield of the pepper leaf essential oil; keeping the liquid-material ratio of 10:1(mL/g) and the distillation time of 50min unchanged, and comparing the influences of different ultrasonic powers (100, 200, 300, 400 and 500W) on the yield of the pepper leaf essential oil; keeping the liquid-material ratio of 10:1(mL/g) and the ultrasonic power of 300W constant, and comparing the influence of different distillation times (30, 40, 50, 60 and 70min) on the yield of the pepper leaf essential oil. According to a single-factor experiment, the influence of various factor variables on the yield of the pepper leaf essential oil is researched.
1.2.5BBD optimization of extraction conditions of pepper leaf essential oil
According to the results of 1.2.4 single-factor experiments, the liquid-material ratio (A), the ultrasonic power (B) and the distillation time (C) are used as independent variables, the yield (Y) of the pepper leaf essential oil is used as a response value, and a three-factor three-level response surface is designed for analysis experiments and statistical analysis according to BBD design experiment principles. The experimental design factors and levels are shown in table 2.
TABLE 2 response surface design experiment factors and levels
1.2.6GC-MS analysis of essential oil composition of pepper leaves
GC conditions were as follows: BR-5ms capillary columns (30 m.times.0.25 mm. times.0.25 μm); temperature rising procedure: the initial temperature is 60 ℃, the temperature is increased to 185 ℃ at the speed of 1.5 ℃/min, the temperature is maintained for 1min, and then the temperature is increased to 275 ℃ at the speed of 9 ℃/min, the temperature is maintained for 2 min; the sample injection amount is 0.5 mu L; the pressure is 2.4kPa, the carrier gas is He, the flow rate is 1mL/min, and the split ratio is 40: 1.
MS conditions: EI ionization source, energy 70 eV; the ion source temperature is 230 ℃, the quadrupole rod temperature is 150 ℃, the interface temperature is 250 ℃, and the mass scanning range m/z is 35-500.
1.3 data processing
All experiments were repeated 3 times. SPSS16.0 statistical software is used for carrying out single-factor variance statistical analysis and significance test on single-factor experimental data, Design-Expert response surface software is used for carrying out analysis and response surface optimization on relevant factor data extracted from the pepper leaf essential oil, and origin8.5 software is used as a response surface map.
2 results and analysis
2.1 screening for DES types
According to the figure 1, in the influence of the 5 eutectic solvents on the yield of the essential oil, the DES-4 (choline chloride-urea) has the best effect on the extraction of the essential oil of the pepper leaves, and the yield of the essential oil is 1.312 +/-0.018%. Kumar et al have shown that some DES can solubilize cellulose and that pretreatment of plant tissue can enhance the release of intracellular compounds. According to the experimental result, the extraction yield of the hydrogen bond donor which is the eutectic solvent of amides (DES-4) to the essential oil is better than that of the hydrogen bond donor which is the eutectic solvent of polyols (DES-1, DES-2) and carboxylic acids (DES-3, DES-5). The dissolving mechanism of the quaternary ammonium salt (choline chloride) eutectic solvent for cellulose is that quaternary ammonium salt cations react with oxygen atoms on cellulose hydroxyl groups to form new hydrogen bonds, which accords with the mechanism of electron acceptance and supply participated by hydrogen and oxygen atoms on the cellulose hydroxyl groups, the action of acetate anions and caprolactam can provide more active sites for dissolving hemicellulose, and the hydrogen bond structure between the quaternary ammonium salt and amide substances enables the cellulose to be changed from a compact ordered structure to a rough disordered structure, so that the quaternary ammonium salt (choline chloride) eutectic solvent has stronger dissolving capacity for lignin. Therefore, a choline chloride-urea (DES-4) eutectic solvent is selected for subsequent experiments.
2.2 Single factor experiment
2.2.1 Effect of liquid ratio on essential oil yield
According to fig. 2, it can be analyzed that the yield of the pepper leaf essential oil is increased with the increase of the liquid-to-material ratio before the liquid-to-material ratio is 10:1(mL/g), the yield of the pepper leaf essential oil reaches the maximum value with the liquid-to-material ratio being 10:1(mL/g), and then the yield of the pepper leaf essential oil is gradually decreased with the increase of the liquid-to-material ratio. The reason is that when the liquid material ratio is too small, namely the distilled water in the pepper leaf powder is too little, the distilled water cannot fully permeate into the pepper leaf powder, so that the essential oil is difficult to overflow, and the yield of the pepper leaf essential oil is reduced because the pepper leaf powder is locally heated due to too little distilled water; when the liquid-material ratio is too large, namely the distilled water in the pepper leaf powder is too much, the yield is reduced because a small part of pepper leaf essential oil is dissolved in the water, and the time cost and the energy consumption are considered at the same time. Therefore, the liquid-to-feed ratio is preferably controlled to about 10:1 (mL/g).
2.2.2 Effect of ultrasonic Power on essential oil yield
According to fig. 3, it can be analyzed that the yield of the pepper leaf essential oil is increased along with the increase of the ultrasonic power before the ultrasonic power is 300W, because when the ultrasonic power is too low, the cavitation is weak, so that the local tensile stress in the liquid is insufficient, the essential oil is not easy to overflow, and when the ultrasonic power is increased, the cavitation is enhanced along with the increase of the ultrasonic power, the molecular diffusion speed is increased, the essential oil is easy to overflow, and thus the yield of the essential oil is increased; the yield of the pepper leaf essential oil is reduced along with the increase of the ultrasonic power after the ultrasonic power is 300W, because the cavitation effect is greatly enhanced when the ultrasonic power is too high, the time of the material staying in an ultrasonic field is reduced, and the probability of water permeating into plant tissues is reduced, which is similar to the research result of the ultrasonic-assisted extraction of the perilla essential oil from the plum snow. Therefore, the ultrasonic power should be reasonably controlled to be about 300W.
2.2.3 Effect of distillation time on essential oil yield
According to the analysis of fig. 4, the yield of the pepper leaf essential oil is improved along with the increase of the distillation time before the distillation time reaches 50min, because the distillation time is short and the overflow of the essential oil is not thorough, the yield of the essential oil is not high; the yield of essential oil reaches a maximum at a distillation time of 50 min. However, after the distillation time exceeds 50min, the yield of the pepper leaf essential oil is rather reduced, and probably due to the volatilization loss of part of the essential oil, similar findings are found in the almond essential oil extraction process researched by mallow and the like, and the distillation time is controlled to be about 50min in consideration of time cost and energy consumption.
2.3 response surface method for optimizing the extraction conditions of pepper leaf essential oil test results
2.3.1 response surface optimization experiment design results and analysis of variance
According to the results of the single-factor test, the liquid-material ratio (A), the ultrasonic power (B) and the distillation time (C) are used as optimization parameters, the yield (Y) of the pepper leaf essential oil is used as a response value, and the response surface analysis is carried out according to the BBD design principle, and the results are shown in Table 3.
TABLE 3 response surface experimental design and results
And performing regression analysis and variance analysis on the obtained data by using Design-Expert software, so as to obtain a quadratic regression equation of Y (essential oil yield), liquid-material ratio (A), ultrasonic power (B) and distillation time (C), wherein the quadratic regression equation comprises the following components:
Y＝1.32+0.082A+0.13B+0.034C+0.012AB+0.044AC+0.036BC－0.07A2－0.17B2－0.12C2
as can be seen from Table 4, the regression model determines the coefficient R20.9973, correction decision coefficient R2 Adj＝0.9938, regression equation model is extremely significant (P)<0.0001), indicating that the model is consistent with the reality and has reliability. And the mismatch term is not significant (P is 0.068)>0.05), which shows that non-experimental factors have little influence on the yield of the pepper leaf essential oil and have little abnormal error. The influence of the single-factor liquid-material ratio (A), the ultrasonic power (B) and the distillation time (C) is extremely obvious (P)<0.01), the interaction effect of the liquid-material ratio and the distillation time interaction term (AC) and the interaction term (BC) of the ultrasonic power and the distillation time is extremely obvious (P <0.05), and the interaction effect of the liquid-material ratio and the ultrasonic power interaction term (AB) is not obvious (P)>0.05). According to the judgment of the F value, the influence of each factor on the yield of the essential oil is B>A>C, i.e. ultrasonic power>Liquid to feed ratio>And (4) distilling time.
TABLE 4 regression model and analysis of variance
Note: p <0.01 was very significant.
2.3.2 response surface map analysis
Response surface variance analysis and regression equation model establishment are carried out on the pepper leaf essential oil through the Designenxpert software, and then a corresponding response surface graph is made by utilizing the origin8.0 software, as shown in FIGS. 5-7.
The influence of each factor on the rate of the pepper leaf essential oil and the interaction among the factors can be analyzed from the graphs of 5 to 7, and the interaction between the other two factors and the influence on the yield of the pepper leaf essential oil are kept at a zero level for any one of the factors of the liquid-material ratio (A), the ultrasonic power (B) and the distillation time (C). From the results of fig. 5-7, it can be seen that the curved surfaces of fig. 6-7 have steep trends in view of the trend and slope of the response surface, which shows that the interaction effect between the liquid-material ratio and the distillation time, and the ultrasonic power and the distillation time is significant, and is consistent with the analysis result of variance. From the shape and the density degree of the contour lines, the contour lines of fig. 6-7 are elliptical and have dense curves, which shows that the interaction effect between the liquid-material ratio and the distillation time, the ultrasonic power and the distillation time is strong, and the interaction effect has obvious influence on the response value.
2.4 optimal conditions and validation experiments
Analyzing by Design expert software to obtain a regression equation, wherein the optimal optimization conditions for predicting and extracting the pepper leaf essential oil by a regression model are as follows: the liquid-material ratio is 13.63:1(mL/g), the ultrasonic power is 344.11W, the distillation time is 53.39min, and the maximum yield of the essential oil reaches 1.387 percent. In view of the operability and convenience of the process flow, the modified process parameters for extracting the pepper leaf essential oil are as follows: the liquid-material ratio is 14:1(mL/g), the ultrasonic power is 300W, and the extraction time is 53 min. And (3) repeating the experiment to verify the yield of the essential oil extracted from the pepper leaves according to the corrected process parameters, so that the actual yield of the pepper leaf essential oil is 1.380% +/-0.018%, the error relative to the theoretical value of the response surface model is about 0.50% (the error is within an allowable range), and the fitting between the actual situation and the prediction situation of the regression model is better. The optimized process for extracting the pepper leaf essential oil by ultrasonic assisted steam distillation based on DES by using a response surface method has accurate and reliable result.
Compared with the traditional method, the DES is used for extracting the pepper leaf essential oil, the appearance of the essential oil such as color and luster, properties and the like is not obviously different, and the essential oil is light blue transparent oily liquid at normal temperature and is accompanied with thick pepper leaf smell. As can be seen from Table 5, compared with the steam distillation method and the ultrasonic assisted water distillation method, the yield of the pepper leaf essential oil is respectively improved by 14.33% and 5.18%. The results are similar to the results of the main research institution for researching the chemical component analysis of the pepper fruit and pepper leaf essential oil, and the experimental results are in line with expectations.
Table 5: effect of different extraction methods on essential oil yield
| Extraction method | Yield of essential oil (%) |
| Water vaporGas distillation | 1.207±0.020 |
| Ultrasonic assisted steam distillation | 1.312±0.022 |
| DES-based ultrasonic assisted steam distillation | 1.380±0.018 |
2.5 GC-MS analysis of the essential oil of Piper nigrum leaves
34 volatile chemical components are separated and detected from the pepper leaf essential oil, mass spectrum information and a standard library NIST08 are used for respectively carrying out preliminary search and relevant literature reference characterization on each spectrum peak, the name of the volatile substance is confirmed, and the analysis result is shown in Table 6. As can be seen from table 6, the main components of 18 olefins, 11 alcohols, 1 aldehyde, 1 phenol, 1 ester and 2 other compounds include: -elemene (19.75%), alpha-cubebene (9.17%), caryophyllene (8.97%), alpha-guyucene (6.12%), beta-elemene (5.13%), wherein the content of olefin compounds is the most abundant, accounting for 73.0% of essential oil components. Elemene in the pepper leaf essential oil extracted in the experiment is relatively high, and is known to have an obvious anti-tumor effect according to related literature records, wherein beta-elemene belongs to a national class II non-cytotoxic tumor medicament, so that the pepper leaf has high development and utilization values.
Table 6: chemical composition of pepper leaf essential oil
3 conclusion
The research utilizes a novel eutectic solvent to extract the pepper leaf essential oil, optimizes the process conditions for extracting the pepper leaf essential oil through a single-factor experiment and a response surface analysis method, takes the liquid-material ratio, the ultrasonic power and the distillation time as self-factors, takes the yield of the pepper leaf essential oil as a response value to carry out regression model analysis on the response surface of the pepper leaf essential oil, and is carried out after the process optimization conditions for extracting the pepper leaf essential oil are corrected: the liquid-material ratio is 14:1(mL/g), the ultrasonic power is 300W, the extraction time is 53min, the actual yield of the pepper leaf essential oil is 1.380% +/-0.018%, the predicted value and the actual value of the regression model are better matched, and the reliability of the model is further verified. Through the DES-based ultrasonic-assisted steam distillation process of the pepper leaf essential oil, the yield of the essential oil is improved by 14.33% compared with that of the steam distillation essential oil, and is improved by 5.18% compared with that of the ultrasonic-assisted steam distillation essential oil. Thus, it is demonstrated that a method for extracting the essential oil of pepper leaves using choline chloride-urea as a eutectic solvent is feasible. GC-MS analysis identifies 34 compounds, the main components of which are-elemene (19.75%), alpha-cubebene (9.17%), caryophyllene (8.97%), alpha-guyucene (6.12%) and beta-elemene (5.13%), wherein the-elemene has good research value. The invention provides a new extraction method for the development and utilization of pepper leaf essential oil, and widens the DES application field. The comprehensive utilization of the pepper leaves is also beneficial to the popularization of the pepper leaf essential oil in the industries of food, medicine and cosmetics.
The present invention is not limited to the above-mentioned preferred embodiments, and any other products similar or identical to the present invention, which can be obtained by anyone based on the teaching of the present invention, fall within the protection scope of the present invention.
Claims (10)
1. A method for extracting pepper leaf essential oil by ultrasonic-assisted distillation through a eutectic solvent method is characterized by comprising the following steps: a hydrogen bond acceptor HBA and a hydrogen bond donor HBD in a certain molar ratio form a eutectic solvent DES, and the eutectic solvent DES is used for extracting essential oil from the pepper leaves by ultrasonic-assisted distillation; the method mainly comprises the following steps:
cleaning fresh pepper leaves, drying in an electric heating air blast drying oven at 40-80 ℃ to constant weight, crushing and sieving into pepper leaf powder of 30-80 meshes, and drying in a dryer for later use;
secondly, preparing a eutectic solvent DES, mixing, heating and stirring the hydrogen bond acceptor HBA and the hydrogen bond donor HBD in a constant warm water bath kettle at 70-90 ℃ for 30-120 minutes until a uniform colorless transparent liquid eutectic solvent DES is formed;
mixing the eutectic solvent DES and the pepper leaf powder according to a ratio of liquid-material ratio in a range of 5:1 to 25:1(mL/g), adding distilled water, and treating in an ultrasonic cleaning machine to make the mixture subjected to ultrasonic radiation;
and fourthly, extracting the pepper leaf essential oil from the mixture subjected to ultrasonic auxiliary treatment in the eutectic solvent DES through steam distillation, separating the liquid, and then adding anhydrous sodium sulfate for drying to obtain the pepper leaf essential oil.
2. The method for extracting the essential oil of the pepper leaves by the ultrasonic-assisted distillation of the eutectic solvent method according to claim 1, which is characterized in that: the hydrogen bond receptor HBA is choline chloride.
3. The method for extracting the essential oil of the pepper leaves by the ultrasonic-assisted distillation of the eutectic solvent method according to claim 1, which is characterized in that: the hydrogen bond donor HBD is a quaternary ammonium salt of one of glycerol, ethylene glycol, lactic acid, urea or glucose.
4. The method for extracting the essential oil of the pepper leaves by the ultrasonic-assisted distillation of the eutectic solvent method according to claim 1, which is characterized in that: the eutectic solvent DES is one of the following mixtures in molar ratio:
a mixture of choline chloride and glycerol in a molar ratio of 1: 2;
a mixture of choline chloride and ethylene glycol in a molar ratio of 1: 4;
a mixture of choline chloride and lactic acid in a molar ratio of 1: 2;
a mixture of choline chloride and urea in a molar ratio of 1: 2;
a mixture of choline chloride and glucose in a molar ratio of 2: 1.
5. The method for extracting the essential oil of the pepper leaves by the ultrasonic-assisted distillation of the eutectic solvent method according to claim 1, which is characterized in that: in the step I, the temperature for drying in an electric heating forced air drying oven is 60 ℃, and the pepper leaf powder is crushed and sieved into 50 meshes.
6. The method for extracting the essential oil of the pepper leaves by the ultrasonic-assisted distillation of the eutectic solvent method according to claim 1, which is characterized in that: in the second step, the hydrogen bond acceptor HBA and the hydrogen bond donor HBD are mixed, heated and stirred in a water bath kettle at the constant temperature of 80 ℃ for 30-120 minutes until a uniform, colorless and transparent liquid eutectic solvent DES is formed.
7. The method for extracting the essential oil of the pepper leaves by the ultrasonic-assisted distillation of the eutectic solvent method according to claim 1, which is characterized in that: in the step (c), the eutectic solvent DES and the pepper leaf powder are mixed according to a ratio of liquid-material ratio in a range of 10:1 to 15:1 (mL/g).
8. The method for extracting the essential oil of the pepper leaves by the ultrasonic-assisted distillation of the eutectic solvent method according to claim 1, which is characterized in that: in the step III, the power intensity of the ultrasonic wave is 100-500W; in the step IV, the distillation time for extracting the pepper leaf essential oil by steam distillation is 30-70 minutes.
9. The method for extracting the essential oil of the pepper leaves by the ultrasonic-assisted distillation of the eutectic solvent method according to claim 1, which is characterized in that: in the third step, the power intensity of the ultrasonic wave is 300W; in the step IV, the distillation time for extracting the pepper leaf essential oil by steam distillation is 50-55 minutes.
10. The method for extracting the essential oil of the pepper leaves by the ultrasonic-assisted distillation of the eutectic solvent method according to claim 1, which is characterized in that: in the step III, the eutectic solvent DES is a mixture of choline chloride and urea in a molar ratio of 1:2, the eutectic solvent DES and pepper leaf powder are mixed according to a liquid-material ratio of 14.36:1(mL/g), and the power intensity of the ultrasonic wave is 300W; in the step IV, the distillation time for extracting the pepper leaf essential oil by steam distillation is 53 minutes.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202010623162.6A CN111718799A (en) | 2020-06-30 | 2020-06-30 | Method for extracting pepper leaf essential oil by eutectic solvent method and ultrasonic-assisted distillation |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202010623162.6A CN111718799A (en) | 2020-06-30 | 2020-06-30 | Method for extracting pepper leaf essential oil by eutectic solvent method and ultrasonic-assisted distillation |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN111718799A true CN111718799A (en) | 2020-09-29 |
Family
ID=72570976
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202010623162.6A Pending CN111718799A (en) | 2020-06-30 | 2020-06-30 | Method for extracting pepper leaf essential oil by eutectic solvent method and ultrasonic-assisted distillation |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN111718799A (en) |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112708506A (en) * | 2021-01-11 | 2021-04-27 | 上海应用技术大学 | Method for extracting plant hydrolat by combining eutectic solvent and distillation method |
| CN112779096A (en) * | 2021-01-11 | 2021-05-11 | 上海应用技术大学 | Method for extracting plant essential oil by using double auxiliary agents |
| CN112831376A (en) * | 2021-01-11 | 2021-05-25 | 上海应用技术大学 | Method for extracting plant essential oil by using eutectic solvent |
| CN112852549A (en) * | 2021-01-11 | 2021-05-28 | 上海应用技术大学 | Method for extracting plant hydrolat by using double auxiliary agents |
| CN113549497A (en) * | 2021-07-19 | 2021-10-26 | 上海应用技术大学 | Method for extracting perilla leaf essential oil by using ultrasonic-assisted natural deep eutectic solution and application of perilla leaf essential oil |
| CN115044412A (en) * | 2022-05-25 | 2022-09-13 | 湖南诺泽生物科技有限公司 | Dried orange peel essential oil and preparation method and application thereof |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109609270A (en) * | 2018-11-21 | 2019-04-12 | 浙江工业大学 | Method based on essential oil in the microwave-assisted steam extraction fragrance of natural eutectic solvent- |
| CN109966348A (en) * | 2019-04-09 | 2019-07-05 | 中国科学院昆明植物研究所 | Snippings Fructus Piperis extract and its pharmaceutical composition and its application |
| CN110623988A (en) * | 2019-07-31 | 2019-12-31 | 湖州耕香生物科技有限公司 | Method for extracting and preparing total flavonoids of cotton rose leaves |
-
2020
- 2020-06-30 CN CN202010623162.6A patent/CN111718799A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109609270A (en) * | 2018-11-21 | 2019-04-12 | 浙江工业大学 | Method based on essential oil in the microwave-assisted steam extraction fragrance of natural eutectic solvent- |
| CN109966348A (en) * | 2019-04-09 | 2019-07-05 | 中国科学院昆明植物研究所 | Snippings Fructus Piperis extract and its pharmaceutical composition and its application |
| CN110623988A (en) * | 2019-07-31 | 2019-12-31 | 湖州耕香生物科技有限公司 | Method for extracting and preparing total flavonoids of cotton rose leaves |
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112708506A (en) * | 2021-01-11 | 2021-04-27 | 上海应用技术大学 | Method for extracting plant hydrolat by combining eutectic solvent and distillation method |
| CN112779096A (en) * | 2021-01-11 | 2021-05-11 | 上海应用技术大学 | Method for extracting plant essential oil by using double auxiliary agents |
| CN112831376A (en) * | 2021-01-11 | 2021-05-25 | 上海应用技术大学 | Method for extracting plant essential oil by using eutectic solvent |
| CN112852549A (en) * | 2021-01-11 | 2021-05-28 | 上海应用技术大学 | Method for extracting plant hydrolat by using double auxiliary agents |
| US20220220413A1 (en) * | 2021-01-11 | 2022-07-14 | Shanghai Institute Of Technology | Method for extracting plant essential oil with dual auxiliaries |
| US11959043B2 (en) * | 2021-01-11 | 2024-04-16 | Shanghai Institute Of Technology | Method for extracting plant essential oil with dual auxiliaries |
| CN113549497A (en) * | 2021-07-19 | 2021-10-26 | 上海应用技术大学 | Method for extracting perilla leaf essential oil by using ultrasonic-assisted natural deep eutectic solution and application of perilla leaf essential oil |
| CN115044412A (en) * | 2022-05-25 | 2022-09-13 | 湖南诺泽生物科技有限公司 | Dried orange peel essential oil and preparation method and application thereof |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN111718799A (en) | Method for extracting pepper leaf essential oil by eutectic solvent method and ultrasonic-assisted distillation | |
| Ranitha et al. | A comparative study of lemongrass (Cymbopogon citratus) essential oil extracted by microwave-assisted hydrodistillation (MAHD) and conventional hydrodistillation (HD) method | |
| Ahangari et al. | Extraction of lipids from spent coffee grounds using organic solvents and supercritical carbon dioxide | |
| Wu et al. | Essential oil extracted from Cymbopogon citronella leaves by supercritical carbon dioxide: antioxidant and antimicrobial activities | |
| AU2017290107A1 (en) | Decarboxylated cannabis resins, uses thereof and methods of making same | |
| CN106924073A (en) | A kind of replenishing water and preserving moisture facial mask and preparation method thereof | |
| CN106387990A (en) | High-nicotine tobacco extract and application thereof | |
| CN107518101B (en) | Processing method of green tea | |
| CN104830537B (en) | A kind of preparation method and applications of agalloch eaglewood hydrosol | |
| CN106344429B (en) | A kind of needle mushroom Essence and preparation method thereof | |
| Zhao et al. | Variations in main flavor compounds of freshly distilled brandy during the second distillation | |
| CN106398859A (en) | Sesame oil production technology | |
| CN111718798A (en) | Method for extracting pepper leaf essential oil by microwave-assisted distillation through eutectic solvent method | |
| Radzi et al. | Effect of microwave pretreatment on gaharu essential oil using hydrodistillation method | |
| CN107119096B (en) | Preparation method and application of pholiota nameko active peptide | |
| CN108794651A (en) | The method that pectin is extracted in passion fruit pericarp | |
| CN106349020B (en) | A kind of extracting method of menthol | |
| CN110623886A (en) | Preparation method of cortex meliae extract | |
| KR20170056830A (en) | Manufacturing method and cosmetic compositions using Dendropanax morbifera Lev extraction fluid | |
| Murakonda et al. | Combined use of pulse ultrasound–assisted extraction with atmospheric cold plasma: extraction and characterization of bioactive compounds from wood apple shell (Limonia acidissima) | |
| Safin et al. | Water vacuum-oscillating extraction of chaga | |
| CN107412336A (en) | Fruit of Chinese magnoliavine lignanoid and preparation method and application with antioxidant and anti-aging activity | |
| CN105943467A (en) | Method for extracting natural humectant from abelmoschus manihot | |
| CN105779126A (en) | Chinese arborvitae twig and leaf absolute oil as well as preparation method and application thereof | |
| CN110151662A (en) | A kind of plant extract face-nourishing liquor and preparation method thereof |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| WD01 | Invention patent application deemed withdrawn after publication | ||
| WD01 | Invention patent application deemed withdrawn after publication |
Application publication date: 20200929 |