Method and system for extracting and separating high-purity guaiacol from natural plants

Abstract

The invention relates to the technical field of extraction of effective components from natural plants, and discloses a method and a system for extracting and separating high-purity guaiacol from natural plants. The method comprises the following steps: adding a plant raw material containing guaiacol and an extraction solvent into an extraction system for dissolving and extracting to extract guaiacol in plants, so as to obtain a guaiacol extracting solution; mixing the guaiacol extracting solutions, and concentrating to obtain an initial extract of guaiacol; extracting and distilling the initial extract to obtain a guaiacol hydrocarbon crude product; purifying the crude guaiacol product by using chromatography to obtain a concentrated guaiacol extract; and decolorizing the concentrated guaiacol extract, and crystallizing to obtain a high-purity guaiacol product. The invention provides a method and a system for extracting and separating high-content guaiacol from natural plants, and a guaiacol product with higher purity is obtained.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of extracting effective components from natural plants, in particular to a method and system for extracting and separating high-purity guaiazulenum from natural plants. BACKGROUND

[0002] Guaiazulenum is also known as guaiazulenum, guaiac or guaiac, and its English name is Guaiazulenum. It is a blue liquid at room temperature and a blue crystal at low temperature. It changes from dark blue to green and finally to yellow when exposed to light, and is easily soluble in liquid paraffin. Its chemical name is dimethyl isopropyl, and its molecular formula is C 15 H 18 . Guaiazulenum is a widely used external medicine with anti-allergic and anti-inflammatory effects. It is commonly used in daily life to treat burns, frostbite, radiation heat injury and promote wound healing. Because of its certain efficacy and low price, guaiazulenum as a wound treatment drug has potential development prospects and application value. Guaiazulenum is often enriched in plants such as chamomile leaves, stems and other parts; it also exists in lemon balm essential oil. However, most of the existing guaiazulenum is artificially synthesized, and the technology for extracting pure natural guaiazulenum from plants is just starting, and the purity of the extracted guaiazulenum is not high. SUMMARY

[0003] Therefore, according to one aspect of the present application, a method for extracting and separating high-purity guaiazulenum from natural plants is provided, which comprises:

[0004] S1, adding plant raw materials containing guaiazulenum and an extraction solvent into an extraction system for dissolution and extraction, extracting guaiazulenum in the plant to obtain a guaiazulenum extract;

[0005] S2, combining and concentrating the guaiazulenum extract to obtain an initial extract of guaiazulenum;

[0006] S3, extracting and distilling the initial extract to obtain a guaiazulenum crude product;

[0007] S4, purifying the guaiazulenum crude product using chromatography to obtain a concentrated guaiazulenum extract;

[0008] S5, decolorizing and crystallizing the concentrated guaiazulenum extract to obtain a high-purity guaiazulenum product.

[0009] Preferably, in the extraction process:

[0010] The mass ratio of the raw material to the extraction solvent is 1:5-15;

[0011] The extraction temperature is 35-75°.

[0012] Preferably, the extraction solvent is any one of polar organic solvent or inorganic solvent;

[0013] The polar organic solvent is 30%-75% ethanol;

[0014] The inorganic solvent is water.

[0015] Preferably, the merging and extraction process is:

[0016] First, the membrane guaicol extract is filtered to remove impurities;

[0017] Then, low-temperature vacuum concentration is used to obtain the initial extract with a concentration liquid specific gravity of 1.05-1.1, wherein the concentration temperature is controlled within 40-50°, and the concentration pressure is 10-760mmHg.

[0018] Preferably, the extraction and distillation process of the initial extract is:

[0019] (1) equal volume of organic solvent is added to the concentrated liquid in the upper part of the initial extract for extraction, after stirring, it is left for 8 hours, and after complete layering, the concentrated liquid phase is discharged to realize the first impurity removal;

[0020] (2) ethyl acetate or chloroform is added to the discharged concentrated liquid phase, until no organic solvent is generated in the combined concentrated liquid phase, to obtain completely concentrated concentrated liquid, which is ready for use, to realize the second impurity removal;

[0021] (3) distillation, the upper extract of the completely concentrated concentrated liquid is added to the reaction kettle, 5-50% pure water is added to the upper extract, the temperature is raised to 110° for distillation, and the third impurity removal is performed;

[0022] (4) cooling water is passed to cool and reduce to room temperature, to obtain the distilled extract, i.e. guaicol crude product.

[0023] Preferably, the chromatography gradient silica gel chromatography process is:

[0024] First, 5 times of n-hexane is added to the guaicol crude product to fully dissolve, to obtain a dissolved liquid;

[0025] Secondly, 0.1%-1% sodium hydroxide aqueous solution is added to the dissolved liquid in an equal volume of n-hexane, it is washed for 3 times, the sodium hydroxide aqueous solution is discharged, and then pure water is added for washing until neutral, the n-hexane phase is dehydrated by adding anhydrous sodium sulfate, and then concentrated to a specific gravity of 1.1;

[0026] Finally, 1.5 times of silica gel is added to the guaicol crude product for stirring, and then dried in a vacuum drying oven, to obtain the sample for chromatography use.

[0027] Preferably, the decoloring and crystallization process is as follows:

[0028] First, add an organic solvent to the concentrated guaicol extract for dissolution;

[0029] Second, add 1-5% of needle activated carbon to the concentrated guaicol extract for decoloring when heated to 40-75°;

[0030] Finally, freeze crystallization to obtain high purity guaicol product.

[0031] Preferably, the organic solvent system used is any one of n-hexane-ethyl acetate, n-hexane-trichloromethane;

[0032] The amount of silica gel used is between 5-10 times the amount of silica gel sample, and thin layer chromatography and gas chromatography are used for tracking detection during the chromatography process, the guaicol section is collected, and the concentrated guaicol extract is obtained by combining.

[0033] According to another aspect of the present application, a system for extracting and separating high purity guaicol from natural plants is provided, the system comprising, in sequence:

[0034] An extraction system for extracting guaicol from natural plant materials containing guaicol, comprising a monitoring device, a control system, and first, second, and third extraction devices arranged in sequence, wherein the first, second, and third extraction devices are respectively provided with a solvent input port, a feed port, an extract output port, and a discharge port, and the first and second extraction devices are respectively provided with first and second communication ports;

[0035] The monitoring device comprises a concentration monitor and a flow meter, which are respectively arranged at the solvent input port, the feed port, the extract output port, and the discharge port;

[0036] The control system comprises a controller and a plurality of solenoid valves, and the plurality of solenoid valves are respectively arranged at the solvent input port, the feed port, the extract output port, the discharge port, and the communication ports, and the controller is respectively electrically connected to the solenoid valves, the concentration monitor, and the flow meter;

[0037] A reaction kettle, wherein the input end of the reaction kettle is provided with a filter membrane, and the input end of the reaction kettle is respectively connected to the extract output ports of the first, second, and third extraction devices;

[0038] An extractive distillation machine, wherein the input end of the extractive distillation machine is connected to the output end of the reaction kettle;

[0039] A silica gel chromatography column, wherein the input end of the silica gel chromatography column is connected to the extractive distillation machine.

[0040] Preferably, the first extraction device comprises a first outer shell, and a first extraction part and a first separation part arranged in the first outer shell in a top-to-bottom manner, the first extraction part is arranged in a gap with the outer shell, a cable is wound outside the first extraction part, and two ends of the cable are connected with an alternating current generator;

[0041] First feed ports (natural plant feed ports) and first solvent input ports are arranged on both sides of the top of the first extraction part, and a first communication port is arranged at the bottom of the first extraction part and communicates with the first separation part;

[0042] The first separation part is arranged in a gap with the first outer shell and forms a first filter cavity with the first outer shell, the top of the first separation part is connected with the first communication port, the side wall of the first separation part is uniformly provided with a plurality of first filter holes, the bottom of the first separation part is rotationally connected with the first outer shell, and the bottom of the first separation part is provided with a first discharge port;

[0043] The outer side of the bottom of the first filter cavity is provided with a first extraction liquid output port;

[0044] The first feed ports, the first solvent input ports, the first communication port, the first discharge port, and the first extraction liquid output port are respectively provided with first electromagnetic valves, and the first discharge port and the first extraction liquid output port are respectively provided with first concentration monitors and first flow meters;

[0045] The second extraction device comprises an inner rotating body, an outer rotating body and a second outer shell arranged in sequence from inside to outside, the inner rotating body and the outer rotating body are arranged in a gap, the inner rotating body and the outer rotating body are controlled separately, the directions of rotation of the inner rotating body and the outer rotating body are opposite, the rotation speed of the inner rotating body is greater than that of the outer rotating body, and an annular second filter cavity is arranged between the inner rotating body and the outer rotating body;

[0046] The top surface of the inner rotating body is a conical surface with a taper less than 15°, and the bottom of the inner rotating body is rotationally connected with the second outer shell;

[0047] The outer rotating body is arranged in a gap with the second outer shell and is rotationally connected with the second outer shell, the outer rotating body is higher than the inner rotating body, the top of the outer rotating body is provided with a first feed port, the circumferential side of the outer rotating body is uniformly provided with two circles of second solvent input ports, and one side of the bottom of the outer rotating body is provided with a second discharge port;

[0048] The two circles of second solvent input ports are respectively lower than the highest part of the conical surface and higher than the lowest part of the conical surface;

[0049] The inner and outer sides of the second filtering cavity are connected with the inner rotating body and the outer rotating body respectively, the top of the second filtering cavity is provided with a second communication port, the top plate of the annular second filtering cavity is uniformly provided with a plurality of second filtering holes, and the bottom plate of the annular second filtering cavity is provided with a second extraction liquid output port.

[0050] The second solvent input port, the second extraction liquid output port, the second discharge port and the second communication port are respectively provided with a second electromagnetic valve, and the second extraction liquid output port and the second discharge port are respectively provided with a second concentration monitor and a second flow meter.

[0051] The third extraction device comprises an extraction tank, a buffer tank and a metering tank, the top of the extraction tank is provided with a third feed port, one side of the top of the extraction tank is provided with a third solvent input port, and the bottom of the extraction tank is provided with a third extraction liquid output port.

[0052] The input port of the buffer tank is connected with the third extraction liquid output port, and the output port of the buffer tank is connected with a reaction kettle and the extraction tank.

[0053] The output port of the metering tank is connected with the third solvent input port.

[0054] The third solvent input port, the third feed port and the third extraction liquid output port are respectively provided with a third electromagnetic valve, a third concentration monitor and a third flow meter.

[0055] The AC power generator, the first electromagnetic valve, the first flow meter, the first concentration monitor, the second electromagnetic valve, the second flow meter, the second concentration monitor, the third electromagnetic valve, the third flow meter and the third concentration monitor are connected with the controller.

[0056] Compared with the prior art, the application has the beneficial effects that:

[0057] In the application, natural plants containing guaiazulene are placed in an extraction system, and corresponding solvents are added for dissolution, and after three extractions, an extraction liquid containing guaiazulene is obtained; the extraction liquids are combined and concentrated to obtain an initial extract; the initial extract is repeatedly extracted with an organic solvent and an acid and alkali aqueous solution to remove impurities, and a guaiazulene crude product is obtained; the guaiazulene crude product is chromatographed by using a n-hexane ethyl acetate system gradient silica gel to obtain a guaiazulene high-content product (i.e., a concentrated guaiazulene extract); finally, the guaiazulene high-content product is subjected to decolorization and ethanol crystallization to obtain a guaiazulene fine product (i.e., a high-purity guaiazulene product), and the content can reach more than 99% after detection.

[0058] In the present application, the natural plants containing guaiazulene are extracted three times by the first extraction device, the second extraction device and the third extraction device in the extraction system, which guarantees the complete extraction of guaiazulene from the natural plants containing guaiazulene; the controller in the extraction system calculates the theoretical extraction liquid amount and concentration of the first extraction device, the second extraction device and the third extraction device according to the total amount of the natural plants containing guaiazulene initially input into the extraction system and the total amount of the theoretical guaiazulene components that can be extracted when the plants are completely extracted, and calculates the corresponding extraction time, the addition amount of the theoretical solvent and the concentration of the solvent of the first extraction device, the second extraction device and the third extraction device, thereby guaranteeing that the total extraction amount reaches the total amount of the theoretical guaiazulene components; in the whole extraction system, the control system calculates the extraction amount of guaiazulene after the first extraction according to the concentration and flow rate of the first extraction liquid obtained by the monitoring module in real time, compares the extraction amount with the theoretical extraction amount after the first extraction, and correspondingly adjusts the related parameters (such as the concentration of the added solvent, the total amount of the solvent, the extraction time and the extraction temperature) of the second extraction and the third extraction for the dynamic adjustment of the extraction between the three extractions, so that the actual extraction total amount after the three extractions is consistent with the theoretical extraction total amount. BRIEF DESCRIPTION OF DRAWINGS

[0059] Figure 1 The structure diagram of the extraction system in the system for extracting and separating high-purity guaiazulene from natural plants in the present application;

[0060] Figure 2 The structure diagram of the third extraction device in the system for extracting and separating high-purity guaiazulene from natural plants in the present application;

[0061] Figure 3 The guaiazulene spectrum in chamomile in the embodiment of the present application;

[0062] Figure 4 The guaiazulene extract spectrum after silica gel chromatography in the embodiment of the present application;

[0063] Figure 5 The guaiazulene fine product spectrum prepared in the present application;

[0064] SEQUENCE LISTING

[0065] 1, first housing; 2, first feed inlet; 3, first extraction part; 4, cable; 5, first separation part; 6, first extraction liquid outlet; 7, first solvent inlet; 8, first communication port; 9, first discharge port; 10, second filter cavity; 11, second filter hole; 12, first circle second solvent inlet; 13, second circle second solvent inlet; 14, second extraction liquid outlet; 15, extraction tank; 16, metering tank; 17, buffer tank. DETAILED DESCRIPTION

[0066] The technical solutions in the embodiments of the present application will be clearly and completely described below with reference to the drawings in the embodiments of the present application. Obviously, the described embodiments are only part of the embodiments of the present application, rather than all the embodiments. Based on the embodiments in the present application, all other embodiments obtained by those skilled in the art without creative labor fall within the scope of protection of the present application.

[0067] A method for extracting and separating high-purity guaiazulene from natural plants, in the present application, natural plants containing guaiazulene are taken as raw materials, such as chamomile, eucalyptus oil, and rosmarinus officinalis:

[0068] S1, the natural plants are extracted, and the extraction is performed for 3 times, and the extraction temperature of each time is controlled within 35-75°, and the specific extraction process is as follows:

[0069] The first extraction process is that the natural plant raw material is crushed into 10-20 mesh coarse particles, and the coarse particle natural plant raw material is loaded into the first extraction device, 5-15 times water or 30%-75% ethanol of the mass of the raw material is added as the extraction solvent, after soaking for 2 hours, heating extraction is started, the extraction temperature is controlled at 35-75°, then the first separation is performed, the first extraction liquid after the first extraction is introduced into the combination and concentration device, and the first mixture of the first solvent and the plant raw material after filtration is input into the second extraction device from the first discharge port;

[0070] The second extraction process is that the actual first extraction amount is calculated according to the total amount and the concentration of the first extraction liquid, and the concentration, the addition amount, the extraction time and the extraction temperature of the second solvent in the second extraction process are set according to the concentration and the total amount of the first mixture entering the second extraction device, so that the extraction amount after the first extraction and the second extraction matches the theoretical first extraction amount and the second extraction amount; after the second extraction is completed, the second separation is performed, the second extraction liquid is introduced into the combination and concentration device, the second mixture of the first solvent, the second solvent and the plant raw material is input into the third extraction device from the second discharge port, and the third extraction is performed;

[0071] The third extraction process is set according to the comprehensive calculation of the first and second extraction amounts, the total amount and concentration of the second mixture entering the third extraction device, and the concentration, addition amount, extraction time and extraction temperature of the third solvent in the third extraction process, so as to ensure that the actual extraction amount is the theoretical extraction amount. After the third extraction is completed, the third extraction liquid is introduced into the extraction and combination device;

[0072] The first solvent, the second solvent and the third solvent are the same solvent, and the concentration is adjusted to keep the same difference with the concentration coefficient of the extract.

[0073] S2, after the first extraction liquid, the second extraction liquid and the third extraction liquid are combined in the extraction and combination device, the filtered liquid is obtained by membrane filtration, and then the filtered liquid is concentrated at low temperature and reduced pressure to obtain the initial extract of guaicol, wherein the concentration temperature is controlled within 50°, and the pressure is 10-760mmHg. The specific gravity of the obtained initial extract is between 1.05 and 1.1.

[0074] S3, the initial extract is extracted, distilled, and the specific process is as follows: the initial extract is added into equal volume of organic solvents such as ethyl acetate and chloroform, stirred and then placed for 8 hours. After the complete separation of layers, the concentrated liquid phase is discharged to realize the first impurity removal. The free alkaloids, organic acids, flavones, coumarin aglycone and other medium-polar compounds are removed. Ethyl acetate or chloroform is added to the discharged concentrated liquid phase until no organic solvent is generated in the combined concentrated liquid phase to obtain completely concentrated concentrated liquid for use, realizing the second impurity removal and removing the organic impurities in the initial extract. Distillation is carried out by adding 5-50% pure water to the upper extract of the completely concentrated concentrated liquid, increasing the temperature to 110° for distillation, and removing the impurities such as amino acids, sugars and inorganic salts for the third time. Part of the impurities is distilled out with water vapor. After 2 hours, cooling water is passed to cool and reduce the temperature to room temperature to obtain viscous extract.

[0075] S4, the concentrated guaicol extract is obtained by using chromatography to purify the guaicol crude product, and the specific process is as follows:

[0076] (1) washing, the viscous extract obtained after distillation is added with 5 times volume of n-hexane for complete dissolution, then equal volume of 0.1%-1% sodium hydroxide aqueous solution is added, and the mixture is washed for 3 times. The sodium hydroxide aqueous solution is discharged, and then pure water is added for washing until neutral. Anhydrous sodium sulfate is added to the n-hexane phase for dehydration, and then the mixture is concentrated to a specific gravity of 1.1. 1.5 times of silica gel is added to the distilled extract for stirring, and then the mixture is placed in a vacuum drying oven for drying to obtain a sample for chromatography.

[0077] (2) Chromatography, silica gel sample preparation using silica gel column chromatography, using organic solvent system is n-hexane-ethyl acetate; n-hexane-trichloromethane; and not limited to the next several solvent systems, the amount of silica gel used between 5-10 times the silica gel sample, the process using thin layer chromatography and gas chromatography tracking detection, collection of guaiac blue oil hydrocarbon segment combined and concentrated into guaiac blue oil hydrocarbon extract.

[0078] S5, crystallization, column chromatography collected extract using ethanol, acetone, ethyl acetate and other organic solvents, heated to 40-75 °, add blue oil hydrocarbon extract weight of 1%-5% needle with activated carbon decolorization, then freeze crystallization, get the final guaiac blue oil hydrocarbon product (i.e., high purity guaiac blue oil hydrocarbon product).

[0079] The application is further explained by the following examples.

[0080] Example 1

[0081] Step one: take the golden chamomile 300 kg, the raw material is crushed into 20 mesh particles, put into a 3000 liter multifunctional extraction tank, add 75% ethanol about 2500 liters, adjust the temperature to 70 °, extract 2.5 hours * 3 times, the process constantly heat cycle, improve the yield, three times of extraction liquid using low temperature concentrator combined and concentrated to specific gravity 1.05, get the extraction concentrate 299.5 kg;

[0082] Step two: step one extraction concentrate 299.5 kg, loaded into the extraction tank, then add 299.5 liters of ethyl acetate extraction, placed after 24 hours, put out the ethyl acetate phase, then add 299.5 liters of ethyl acetate extraction again, combined twice extraction liquid low temperature concentration to specific gravity 1.1, get the extraction extract 48.5 kg;

[0083] Step three: take step two extraction extract 48.5 kg, add to 200 liters of reaction kettle, add 9 liters of pure water, gradually heated to 110 °, heated to reflux for 2 hours, then slowly cool to room temperature, get the distillation extract 42.7 kg;

[0084] Step four: step three distillation extract 42.7 kg, add 85.4 liters of n-hexane solution, after stirring evenly add 85.4 liters of 0.5% sodium hydroxide aqueous solution extraction three times, then washed with pure water three times, and then use anhydrous sodium sulfate to remove water from n-hexane, concentrated to get the extraction extract 24.2 kg;

[0085] Step five: the upper n-hexane extraction extract 24.2 kg, add 24.2 liters of ethanol heated to dissolve, then add 24.2 kg of 200 mesh silica gel, mix evenly and then put into a vacuum drying oven for low temperature drying, get silica gel dry powder 36.2 kg;

[0086] Step six: take 36.2 kg of upper silica gel dry powder, load into the chromatography column, and load 120 kg of 200 mesh silica gel into the lower part of the column. Gradient chromatography is used with n-hexane: ethyl acetate, the ratio gradually increases from 10:1 to 1:1. According to the TLC spots, the guaicol part is collected and concentrated at low temperature to obtain 2.5 kg of blue oily extract;

[0087] Step seven: 2.5 kg of guaicol crude product is dissolved in 25 liters of 10 times the amount of anhydrous ethanol by heating, then 250 grams of 757 needle activated carbon is added, heated and stirred at 70° for 30 minutes, filtered the activated carbon, and the ethanol solution is concentrated at low temperature to the alcohol-free state, obtaining 1960 grams of blue semi-crystalline product, and the guaicol content is more than 99%;

[0088] Example 2

[0089] Step one: take 400 kg of golden chamomile, crush the raw material into 20 mesh particles, and put it into a 3000 liter multifunctional extraction tank. Add about 3300 liters of 90% ethanol, adjust the temperature to 75°, and extract for 2.5 hours*3 times. Heat circulation is continuously improved during the process to improve yield. The three extraction liquids are combined and concentrated to a specific gravity of 1.05 using a low-temperature concentrator, obtaining 380 kg of extraction concentrate;

[0090] Step two: 380 kg of extraction concentrate from step one is loaded into the extraction tank, then 380 liters of ethyl acetate is added for extraction. After 24 hours, the ethyl acetate phase is discharged, then 380 liters of ethyl acetate is added again for extraction. The two extraction liquids are combined and concentrated at low temperature to a specific gravity of 1.1, obtaining 62 kg of extraction extract;

[0091] Step three: take 62 kg of extraction extract from step two, add to a 200 liter reaction kettle, add 18 liters of pure water, gradually heat to 120°, heat reflux for 2 hours, then slowly cool to room temperature, obtaining 53.1 kg of distillation extract;

[0092] Step four: add 106.2 liters of n-hexane to 53.1 kg of distillation extract from step three, stir evenly, then add 106.2 liters of 1% sodium hydroxide solution for extraction three times, then wash with pure water three times, then use anhydrous sodium sulfate to remove water from n-hexane, and concentrate to obtain 30.8 kg of extraction extract;

[0093] Step five: add 30.8 liters of ethanol to 30.8 kg of n-hexane extraction extract, heat to dissolve, then add 30.8 kg of 200 mesh silica gel, mix evenly, then put into a vacuum drying oven for low-temperature drying, obtaining 44.7 kg of silica gel dry powder;

[0094] Step six: take the upper silica gel dry powder 44.7 kg, loaded into the chromatography column, the lower chromatography silica gel loaded into 147 kg of 200 mesh silica gel, using n-hexane: ethyl acetate gradient chromatography, ratio from 10:1 gradually increased to 1:1, according to the thin layer spot collection guaicol part, combined low temperature concentration of blue oil extract 3.3 kg;

[0095] Step seven: the upper guaicol crude product 3.3 kg with 10 times the amount of anhydrous ethanol 33 liters heated to dissolve, then add 400 grams of 757 needle activated carbon, 70 ° heating stirring 30 minutes, filter activated carbon, ethanol solution low temperature concentration to no alcohol state, get 2650 grams of blue semi crystalline product, detection guaicol content of more than 99%.

[0096] Example 3

[0097] Step one: take the golden yellow chamomile 400 kg, the raw material is crushed into 20 mesh particles, put into the 3000 liters of multifunctional extraction tank, add 50% ethanol about 3600 liters, adjust the temperature to 80 °, extraction 2.5 hours * 3 times, the process of constant heat cycle, improve the yield, three times extraction liquid using low temperature concentrator combined concentration to specific gravity 1.05, get the extraction concentrate 425 kg;

[0098] Step two: step one extraction concentrate 425 kg, loaded into the extraction tank, then add 425 liters of ethyl acetate extraction, after 24 hours, put out the ethyl acetate phase, then add 425 liters of ethyl acetate extraction again, combined two times extraction liquid low temperature concentration to specific gravity 1.1, get the extraction extract 65.6 kg;

[0099] Step three: take the extraction extract 65.6 kg in step two, add to 200 liters of reaction kettle, add pure water 20 liters, gradually heated to 120 °, heating reflux 2 hours, then slowly cool to room temperature, get the distillation extract 54.3 kg;

[0100] Step four: step three distillation extract 54.3 kg, add 108.6 liters of n-hexane solution, stirring uniformity after adding 108.6 liters of 1% sodium hydroxide aqueous solution extraction three times, then washed with pure water three times, and then use anhydrous sodium sulfate to remove water from n-hexane, concentrated to get the extraction extract 31.6 kg;

[0101] Step five: the upper n-hexane extraction extract 31.6 kg, add 31.6 liters of ethanol heated to dissolve, then add 31.6 kg of 200 mesh silica gel, mix well and then put into the vacuum drying oven low temperature drying, get silica gel dry powder 46.8 kg;

[0102] Step six: take the upper silica gel dry powder 46.8 kg, loaded into the chromatographic column, the lower chromatographic silica gel loaded into 152 kg of 200 mesh silica gel, using n-hexane: ethyl acetate gradient chromatography, ratio from 10:1 gradually increased to 1:1, according to the thin layer spot collection guaiazulene part, combined low temperature concentration of blue oil extract 3.2 kg;

[0103] Step seven: the upper guaiazulene crude product 3.2 kg with 10 times the amount of anhydrous ethanol 33 liters heated to dissolve, then add 400 grams of 757 needle activated carbon, 70 ° heating stirring 30 minutes, filter activated carbon, ethanol solution low temperature concentration to no alcohol state, get 2570 grams of blue semi crystalline product, detection guaiazulene content of more than 99%.

[0104] Example 4

[0105] Step one: take the geranium raw material 400 kg, the raw material is crushed into 20 mesh particles, put into the 3000 liters of multifunctional extraction tank, add 75% ethanol about 3500 liters, adjust the temperature to 75 °, extraction 2.5 hours * 3 times, the process of constant heat cycle, improve the yield, three times extraction liquid using low temperature concentrator combined concentration to specific gravity 1.05, get the extraction concentrate 355 kg;

[0106] Step two: step one extraction concentrate 355 kg, loaded into the extraction tank, then add 355 liters of ethyl acetate extraction, after 24 hours, put out the ethyl acetate phase, then add 355 liters of ethyl acetate extraction again, combined two times extraction liquid low temperature concentration to specific gravity 1.1, get the extraction extract 52.4 kg;

[0107] Step three: take step two extraction extract 52.4 kg, add to 200 liters of reaction kettle, add pure water 20 liters, gradually heated to 120 °, heating reflux 2 hours, then slowly cool to room temperature, get the distillation extract 38.7 kg;

[0108] Step four: step three distillation extract 38.7 kg, add 77.4 liters of n-hexane solution, stirring uniformity after adding 77.4 liters of 1% sodium hydroxide aqueous solution extraction three times, then washed with pure water three times, and then use anhydrous sodium sulfate to remove water from n-hexane, concentrated to get the extraction extract 22.6 kg;

[0109] Step five: the upper n-hexane extraction extract 22.6 kg, add 22.6 liters of ethanol heated to dissolve, then add 22.6 kg of 200 mesh silica gel, mix well after putting into the vacuum drying oven low temperature drying, get silica gel dry powder 32.8 kg;

[0110] Step six: take 32.8 kg of the upper dry silica gel powder and load into a chromatographic column, and load 150 kg of 200 mesh silica gel into the lower part of the column. Gradient chromatography is performed using n-hexane: ethyl acetate with the ratio gradually increasing from 10:1 to 1:1. The guaicol part is collected according to the thin layer spots, and the blue oily extract 1.8 kg is obtained by low temperature concentration.

[0111] Step seven: 1.8 kg of the guaicol crude product is dissolved by heating with 10 times the amount of anhydrous ethanol 18 liters, and then 360 grams of 757 needle activated carbon is added. The mixture is heated and stirred at 70° for 30 minutes. The activated carbon is filtered, and the ethanol solution is concentrated at low temperature to the anhydrous state to obtain 1420 grams of blue semi-crystalline product. The guaicol content is detected to be more than 99%.

[0112] The guaicol products prepared in the above examples 1-4 are identified and determined.

[0113] Guaicol product standards:

[0114] Appearance: The product is dark blue liquid or crystal.

[0115] Melting point: The melting point of the product should be 30.5°-32.5°.

[0116] Freezing point: The freezing point of the product should be ≤30°.

[0117] Moisture: The moisture of the product should be ≤0.5%.

[0118] Ignition residue: The ignition residue of the product should be ≤0.1%.

[0119] Total bacterial count: The total bacterial count of the product should be 1000 CFU / g.

[0120] Heavy metals: According to general rule 2321, the lead content of the product should be ≤2 PPM; the arsenic content should be ≤1 PPM; the cadmium content should be ≤1 PPM; and the mercury content should be ≤0.1 PPM.

[0121] Solvent residue: According to general rule 0861 third method, the ethanol content of the product should be ≤0.5%; the ethyl acetate content should be ≤0.1%; and the n-hexane content should be ≤0.1%.

[0122] Related substances: The peak area of a single impurity of the product should not be greater than 0.1% of the main peak area of the control solution; the total impurity peak area should not be greater than 5 times the main peak area of the control solution (0.5%); and the peaks in the chromatogram of the test solution that are less than 0.5 times the main peak area of the control solution can be ignored (0.05%).

[0123] Content: The C15H18 content of the product should be 98.0%-102%.

[0124] Guaiacwood detection method

[0125] 1. Appearance: The product is dark blue liquid or crystal

[0126] Observe whether it is consistent with the standard description. Take 0.05 g of the product, place it in a 100 ml volumetric flask, and dilute to the mark with benzene, and shake well. Measure by UV-visible spectrophotometry (General Rule 0401), and there is a maximum absorption at 604-608 nm.

[0127] 2. Melting point: The melting point of the product should be 30.5°-32.5°

[0128] The melting point of the product is detected by capillary melting point detection method, and the melting point meets the standard requirements.

[0129] 3. Solidification point: The solidification point of the product should be ≤30°

[0130] Take 15 ml of the sample in the inner tube of the solidification point determination device, and then place the inner tube in a water bath higher than the solidification point by 10°C, so that only a very small amount of the condensate is not melted. Then place the inner tube together with the sleeve in a water bath with a temperature lower than the solidification point by 5°C, and continuously stir the sample with a stirrer, observe the temperature every 30 seconds, until the liquid begins to condense, stop stirring and observe the temperature every 5-10 seconds, until the mercury column of the thermometer stays at one point for about 1 minute, or rises to the highest temperature and stays for about 1 minute, record the temperature. Take 4 consecutive readings, and the range of each reading should be less than 0.2°C, and the average of the readings is taken as the solidification point of the sample.

[0131] 4. Moisture: The moisture of the product should be ≤0.5%

[0132] Take 3.0 g of the product, measure by moisture determination method (General Rule 0832, first method 1), and when titrating the Karl Fischer reagent, titrate 3 times in parallel, and the relative standard deviation should not be greater than 1.0%, the moisture content of the sample should not exceed 0.5%, and 3 parallel measurements are made.

[0133] 5. Ignition residue: The ignition residue of the product should be ≤0.1%

[0134] After the crucible constant weight, the sample was accurately weighed about 2.0 g, and laid in the crucible, the total weight of the crucible and sample was accurately weighed W1. In the electricOn the stove, open the lid, slowly incinerate to complete carbonization, and cool to room temperature. Add 1 ml of concentrated sulfuric acid to completely wet the carbonized material, and heat at low temperature until the sulfuric acid vapor is completely removed and the white smoke disappears (this operation is carried out in a fume hood). Put the crucible into the muffle furnace, cover the crucible with the lid at an angle, and incinerate at 600±50°C to completely ash. Cover the crucible lid, cool for a moment, and then put it into a silica gel desiccator and cool to room temperature. Repeat the above operation after precise weighing until the difference between two consecutive weighing results is less than 0.3 mg (the incineration time is 30 minutes from the second time). The initial weight is g, the second weighing is g, the third weighing is g, …, and the final constant weight is W2. Calculate the result according to the constant weight.

[0135] 6. Total number of colonies: The total number of colonies of the product should be 1000 CFU / g.

[0136] According to GB 4789.2-94, "Determination of Total Number of Colonies in Food Hygiene Microbiological Examination" of the National Standards of the People's Republic of China

[0137] 7. Heavy metals: According to Pharmacopoeia General 2321, the product requires Pb ≤ 2 PPM; As ≤ 1 PPM; Cd ≤ 1 PPM; Hg ≤ 0.1 PPM 8. Pesticide residues: According to Pharmacopoeia General 2341, 33 kinds of banned pesticides should not be detected (not more than the quantitative limit).

[0138] 9. Solvent residue: According to Pharmacopoeia General 0861, the third method, the product is determined to be ≤0.5% ethanol; ≤0.1% ethyl acetate; ≤0.1% n-hexane.

[0139] Control solution: Precisely weigh 50 mg of ethanol or ethyl acetate, n-hexane into a 100 ml volumetric flask, dilute to the mark with N, N-dimethylformamide, and shake well.

[0140] Sample solution: Accurately weigh 1.0 g of sample into a 10 ml volumetric flask, dissolve and dilute to the mark with N, N-dimethylformamide, and shake well. Two sample solutions are prepared in parallel.

[0141] Determination method: Precisely take 1 ul of the control solution and the sample solution, respectively, and inject them into the gas chromatograph, and record the chromatogram.

[0142] 10. Related substances: The area of a single impurity peak in the product should not be greater than 0.1% of the main peak area of the control solution (0.1%), and the total impurity peak area should not be greater than 5 times the main peak area of the control solution (0.5%), and peaks less than 0.5 times the main peak area of the control solution in the chromatogram of the test sample solution can be ignored (0.05%).

[0143] Detection method: see content detection

[0144] 11. Content: The content of C15H18 in the product should be 98.0%-102%.

[0145]

[0146] Test solution: Take the product, accurately weigh, dissolve in methanol and dilute to make a solution of about 0.02 mg guaiacwood blue oil per 1 ml.

[0147] Reference solution: Take guaiacwood blue oil reference, accurately weigh, dissolve in methanol and dilute to make a solution of about 0.02 mg guaiacwood blue oil per 1 ml.

[0148] 5.9.2. Calculation formula:

[0149] Wherein: A 样 : Test solution main peak area; M 对 : Reference weight, mg; W: guaiacwood blue oil reference content; A 对 : Reference solution main peak area; M 样 : Sample weight, mg.

[0150] Figure 3 The guaiacwood blue oil spectrum in chamomile, the specific values are shown in Table 1, which can be seen that in Figure 3 No. 20 peak is guaiacwood blue oil, and the peak height percentage is 2.19%.

[0151] Table 1

[0152]

[0153]

[0154] Figure 4 The guaiacwood blue oil extract spectrum after silica gel chromatography in this application, the specific data are shown in Table 2, in Figure 4 No. 35 peak is guaiacwood blue oil, and the peak height percentage is 83.37%.

[0155] Table 2

[0156]

[0157]

[0158] Figure 5 The guaiacwood blue oil fine spectrum of the final product in this application, the specific data are shown in Table 3, in Figure 5 No. 3 peak is guaiacwood blue oil, and the peak height percentage is 99.81%.

[0159] Table 3

[0160] Serial number Retention time Peak area Peak height Peak separation Peak height percentage Area percentage 1 6.9664 2.6399 0.5410 0.0000 0.1140％ 0.0490％ 2 9.5036 0.7269 0.1005 16.2530 0.0212％ 0.0135％ 3 11.1148 5384.6960 473.9057 6.5356 99.8199％ 99.9026％ 4 12.1842 0.2848 0.0321 3.9120 0.0068％ 0.0053％ 5 12.6751 1.1242 0.1374 2.1719 0.0289％ 0.0209％ 6 15.2873 0.4724 0.440 10.4467 0.0093％ 0.0088& Total 5389.9440 474.7607 100& 100％

[0161] Combining Figure 3-5 and Table 1-3 can be obtained that the peak height percentage of guaiazulene extracted from chamomile by the method described in the present application is 99.81%. That is, according to the above results, the purity of guaiazulene extracted from chamomile by the method described in the present application can reach 99.81, which indicates that the present application not only provides a method for extracting pure natural guaiazulene from natural plants, but also solves the problem of how to separate guaiazulene with high purity from chamomile in the prior art.

[0162] The purity of guaiazulene extracted from chamomile by the method described in the present application can reach 99.81, which indicates that the present application not only provides a method for extracting pure natural guaiazulene from natural plants, but also solves the problem of how to separate guaiazulene with high purity from chamomile in the prior art.

[0163] Example 5

[0164] Referring to Figure 1-2 The present embodiment provides a system for extracting and separating high-purity guaiazulene from natural plants, which comprises, in sequence:

[0165] Referring to Figure 1-2 The present embodiment provides a system for extracting and separating high-purity guaiazulene from natural plants, which comprises, in sequence:

[0166] The extraction system is used to extract guaiazulene from natural plant raw materials containing guaiazulene, and comprises a monitoring device,

[0167] a control system, and a first extraction device, a second extraction device, and a third extraction device arranged in sequence, wherein the first extraction device, the second extraction device, and the third extraction device are respectively provided with a solvent input port, a feed inlet, an extraction liquid output port, and a discharge outlet, and the first extraction device and the second extraction device are respectively provided with a first communication port and a second communication port;

[0168] The monitoring device comprises a concentration monitor and a flow meter, and the concentration monitor and the flow meter are respectively arranged at the solvent input port, the feed inlet, the extraction liquid output port, and the discharge outlet;

[0169] The control system comprises a controller and a plurality of solenoid valves, and the plurality of solenoid valves are respectively arranged at the solvent input port, the feed inlet, the extraction liquid output port, the discharge outlet, and the communication ports, and the controller is electrically connected to the solenoid valves, the concentration monitor, and the flow meter;

[0170] The reaction kettle is provided with a filter membrane at the input end, and the input end of the reaction kettle is connected to the extraction liquid output ports of the first extraction device, the second extraction device, and the third extraction device;

[0171] The input end of the extractive distillation machine is connected to the output end of the reaction kettle;

[0172] The input end of the silica gel chromatographic column is connected to the extractive distillation machine.

[0173] Further, the first extraction device comprises a first outer shell 1, and a first extraction part 3 and a first separation part 5 arranged in the first outer shell 1 in a top-to-bottom manner, the first extraction part 3 is arranged in a gap with the outer shell, a cable 4 is wound outside the first extraction part 3, and the two ends of the cable 4 are connected with an alternating current generator;

[0174] First feed port 2 (natural plant feed port) and first solvent input port 7 are arranged on both sides of the top of the first extraction part 3, and a first communication port is arranged at the bottom of the first extraction part 3 and communicated with the first separation part 5;

[0175] The first separation part 5 is arranged in a gap with the first outer shell 1 and forms a first filter cavity with the first outer shell 1, the top of the first separation part 5 is connected with the first communication port 8, the side wall of the first separation part 5 is uniformly provided with a plurality of first filter holes, the bottom of the first separation part 5 is rotatably connected with the first outer shell 1, and the bottom of the first separation part 5 is provided with a first discharge port 9;

[0176] The outer side of the bottom of the first filter cavity is provided with a first extraction liquid output port 6;

[0177] The first feed port, the first solvent input port, the first communication port, the first discharge port 9 and the first extraction liquid output port 6 are respectively provided with a first electromagnetic valve, and the first discharge port 9 and the first extraction liquid output port 6 are respectively provided with a first concentration monitor and a first flowmeter;

[0178] The second extraction device comprises an inner rotating body, an outer rotating body and a second outer shell arranged in sequence from inside to outside, the inner rotating body and the outer rotating body are arranged in a gap, the inner rotating body and the outer rotating body are controlled separately, the directions of rotation of the inner rotating body and the outer rotating body are opposite, the rotation speed of the inner rotating body is greater than that of the outer rotating body, and an annular second filter cavity 10 is arranged between the inner rotating body and the outer rotating body;

[0179] The top surface of the inner rotating body is a conical surface, and the taper is less than 15°, and the bottom of the inner rotating body is rotatably connected with the second outer shell;

[0180] The outer rotating body is arranged in a gap with the second outer shell and rotatably connected with the second outer shell, the outer rotating body is higher than the inner rotating body, the top of the outer rotating body is provided with a second feed port, the circumferential side of the outer rotating body is uniformly provided with two circles of second solvent input ports, and one side of the bottom of the outer rotating body is provided with a second discharge port;

[0181] The two circles of second solvent input ports are respectively lower than the highest part of the conical surface and higher than the lowest part of the conical surface;

[0182] The inner and outer sides of the second filter cavity 10 body are connected with the inner rotating body and the outer rotating body respectively, the top of the second filter cavity 10 body is provided with a second communication port, the bottom plate of the annular second filter cavity 10 body is provided with a second extract output port 14, and the top plate of the annular second filter cavity 10 body is uniformly provided with a plurality of second filter holes 11.

[0183] The second solvent input port, the second extract output port 14, the second discharge port and the second communication port are respectively provided with a second electromagnetic valve, and the second extract output port 14 and the second discharge port are respectively provided with a second concentration monitor and a second flow meter.

[0184] The third extraction device comprises an extraction tank 15, a buffer tank 17 and a metering tank 16, the top of the extraction tank 15 is provided with a third feed port, the top side of the extraction tank 15 is provided with a third solvent input port, and the bottom of the extraction tank 15 is provided with a third extract output port.

[0185] The input port of the buffer tank 17 is connected with the third extract output port, and the output port of the buffer tank 17 is connected with a reaction kettle and the extraction tank 15 respectively,

[0186] The output port of the metering tank 16 is connected with the third solvent input port.

[0187] The third solvent input port, the third feed port and the third extract output port are respectively provided with a third electromagnetic valve, a third concentration monitor and a third flow meter.

[0188] The AC generator, the first electromagnetic valve, the first flow meter, the first concentration monitor, the second electromagnetic valve, the second flow meter, the second concentration monitor, the third electromagnetic valve, the third flow meter and the third concentration monitor are connected with the controller respectively.

[0189] The first extraction device, the second extraction device and the third extraction device respectively perform first extraction, second extraction and third extraction of guaiazulene in natural plants containing guaiazulene, so as to obtain first extract, second extract and third extract containing guaiazulene.

[0190] It should be noted that:

[0191] In the present application, the first outer shell 1 and the second outer shell are respectively intelligent heatable shells.

[0192] In the present application, the merging and concentrating device is a reaction kettle, wherein the first extract, the second extract and the third extract enter the reaction kettle respectively and are merged and concentrated in the reaction kettle.

[0193] In the present application, the first extraction device comprises a first outer shell body 1 in a cylindrical structure, and an inner cavity provided in the first outer shell body 1, wherein the inner cavity comprises a first extraction part 3 and a first separation part 5 arranged in sequence from top to bottom;

[0194] The first extraction part 3 is in a barrel structure, and is installed in the outer shell body. Two sides of the top of the first extraction part 3 are respectively provided with a plant feeding port and a first solvent input port. Plant raw materials and the first solvent enter the first extraction cavity in a countercurrent manner through the plant feeding port and the first solvent input port. The outer side of the first extraction part 3 is spirally wound by a coil along an extension direction. Two ends of the coil are respectively connected to an alternating current generator. The alternating current generator is powered to make the mixed solution of the plant raw materials and the first solvent in the first extraction part 3 form a vortex. The plant raw materials and the first solvent in the first extraction part 3 are fully mixed to complete the first extraction. The bottom of the first extraction part 3 is provided with a first communication port in communication with the first separation part 5.

[0195] The bottom of the first separation part 5 is rotationally connected to the bottom of the first outer shell body 1 through a first driving motor and a first hollow rotating shaft. Specifically, the first driving motor is installed on the outside of the bottom of the first outer shell body 1. The two ends of the first hollow rotating shaft are respectively connected to the output end of the first driving motor and the center of the bottom of the first separation part 5. The first hollow rotating shaft is rotationally connected to the first outer shell body 1. The center of the bottom of the first separation part 5 is provided with a first discharge port 9, which is located on the inside of the first hollow rotating shaft.

[0196] The first electromagnetic valve, the first concentration monitor and the first flowmeter are respectively wirelessly connected to the control system.

[0197] The control system calculates the rated concentration of the first extraction liquid after the first extraction within a preset extraction time according to the amount of the plant raw materials and the first solvent put into the first extraction system within a period. The control system compares the feedback value of the first concentration monitor with the calculated rated concentration of the first extraction liquid after the first extraction to adjust the related values of the second extraction system, such as the extraction time, the extraction temperature, the corresponding concentration of the second solvent added into the second extraction system and the amount of the second solvent.

[0198] In the present application, the inner rotating body and the outer rotating body are separately controlled. The rotation directions of the inner rotating body and the outer rotating body are opposite, and the rotating speed of the outer rotating body is lower than that of the inner rotating body. The top surface of the inner rotating body is in a conical shape, and the taper is less than 10°. The first discharge port 9 is located directly above the center of the inner rotating body. The first mixture drops into the center of the inner rotating body. Due to the slow rotation of the inner rotating body, the first mixture dropped into the inner rotating body is uniformly coated on the top surface of the entire inner rotating body.

[0199] The outer rotating body is uniformly provided with two circles of second solvent input ports around the inner rotating body, and the two circles of second solvent input ports are arranged up and down, wherein the first circle of second solvent input ports 12 is flush with the highest part of the top surface of the inner rotating body; the second circle of second solvent input ports 13 is arranged obliquely, and the oblique degree is the same as the taper of the conical surface, and the lowest part is flush with the lowest part of the top surface of the inner rotating body.

[0200] The second solvent storage cavity is formed between the outer rotating body and the second shell body, the second shell body is provided with a second solvent input port, and the second shell body is installed at the top of the third extraction system.

[0201] The axial section of the bottom of the second shell body is in the shape of an isosceles trapezoid as a whole.

[0202] The bottom of the inner rotating body is a second extraction liquid output port 14, the rotation of the inner rotating body is realized through a second hollow rotating shaft and a second driving motor, the second driving motor is installed outside the end of the second shell body, the second extraction liquid output port 14 is located in the second hollow rotating shaft, one end of the second hollow rotating shaft extends into the second shell body and is connected with the center of the bottom of the inner rotating body, and the other end of the second hollow rotating shaft is connected with the output end of the second driving motor.

[0203] The rotation of the outer rotating body is realized through a third hollow rotating shaft, a third driving motor, a driving gear and a driven gear, the third driving motor is located outside the second shell body, the driving gear and the driven gear are vertically fitted and located in the shell body, wherein the driven gear is installed outside the third hollow rotating shaft, the driving gear is connected with the output end of the third driving motor; the third hollow rotating shaft is sleeved outside the second hollow rotating shaft, and the third hollow rotating shaft is rotationally connected with the center of the bottom of the second shell body.

[0204] The second solvent is sprayed to the top surface of the inner rotating body through the second solvent input port, due to the opposite rotation directions of the outer rotating body and the inner rotating body, the first plant mixed liquid is simultaneously subjected to the tangential force of the second solvent sprayed by the first circle of second solvent input ports 12 and the influence of the second solvent sprayed by the second circle of second solvent input ports 13 when the first mixture coats the entire top surface of the inner rotating body, and the second solvent and the first mixture are fully contacted for the second extraction under the action of the second solvent sprayed by the first circle of second solvent input ports 12 and the second circle of second solvent input ports 13, and the second extraction is completed in the whole process.

[0205] When the second extraction is completed, the control system controls the rotation speed of the inner rotating body to increase, so that the first mixture coating the top surface of the entire inner rotating body is rotated to fall on the top plate of the annular second filtering cavity 10, at this time the second electromagnetic valve at the second communication port is opened, the mixture of the first mixture and the second solvent enters the annular filtering cavity, since the annular second filtering cavity 10 is connected with the inner rotating body, it rotates synchronously with the inner rotating body, and the second separation is carried out through the top plate of the annular second filtering cavity 10, the second extraction liquid and the second mixture formed by mixing the natural plant with the first solvent and the second solvent are separated;

[0206] The second concentration monitor and the second flow meter arranged at the second extraction liquid output port 14 are used to monitor the concentration and flow of the second purification liquid; the content of guaicol extracted by the second extraction is calculated by the concentration and flow.

[0207] The control system compares the comprehensive value of the second purification liquid concentration value and the first purification liquid value with the rated comprehensive value of the calculated second purification liquid concentration value and the first purification liquid value, adjusts the related parameters of the third extraction system, if it is less than the rated value, the corresponding related parameters of the third purification system are increased, if it is greater, the corresponding related parameters are reduced.

[0208] The third purification system is an extraction tank 15, a buffer tank 17 and a metering tank 16, the input end of the extraction tank 15 is connected with the output port of the third mixture, the top side of the extraction tank 15 is provided with a third solvent input port, the bottom side of the extraction tank is provided with a third extraction liquid output port, and the third extraction liquid output port is connected with the input end of the buffer tank 17.

[0209] During the third extraction, the third mixture and the third solvent are added into the extraction tank 15, after a certain time of immersion, the leakage liquid is discharged at a certain flow rate, and at the same time, the control system controls the third electromagnetic valve arranged at the third solvent input port according to the real-time monitoring of the third flow meter to ensure that the concentration and liquid level of the third solvent in the extraction tank 15 meet the extraction requirements until the leakage is completed.

[0210] In the present application, the rated extraction amount of guaiazulene in the whole plant is calculated according to the total content of the plant added into the extraction system, then the theoretical extraction amount of each time of the three extraction systems is calculated according to the rated extraction amount, and the actual extraction amount of guaiazulene extracted by the first extraction system, the second extraction system and the third extraction system respectively is calculated through the total flow rate fed back by the concentration monitors (including the first concentration monitor, the second concentration monitor and the third concentration monitor) and the flow meters (including the first flow meter, the second flow meter and the third flow meter at the third extraction liquid outlet) in the process, and compared with the rated extraction amount to determine the complete extraction. Meanwhile, the parameter adjustment of the next extraction corresponding to the extraction amount of each time is carried out during the extraction process, so that the dynamic adjustment among the three extractions is carried out to ensure that the actual extraction total amount is the theoretical extraction amount.

[0211] In the present application, the first driving motor and the second driving motor are hollow motors, the first driving motor and the second driving motor are connected with the controller, and both are precision reduction motors.

Claims

1. A method for extracting and separating high-purity guaiac blue hydrocarbons from natural plants, characterized in that, The method includes: S1, plant raw materials containing guaiac blue hydrocarbon and extraction solvent are added to the extraction system for dissolution and extraction to extract guaiac blue hydrocarbon from the plant and obtain guaiac blue hydrocarbon extract. S2, the guaiac blue oil extract was combined and concentrated to obtain the initial extract of guaiac blue oil; S3, after extraction and distillation of the initial extract, yields crude guaiac blue hydrocarbon; S4. The crude guaiac blue hydrocarbon was purified by chromatography to obtain concentrated guaiac blue hydrocarbon extract. S5 is used to decolorize and crystallize concentrated guaiac blue extract to obtain high-purity guaiac blue product.

2. The method for extracting and separating high-purity guaiac blue hydrocarbon from natural plants according to claim 1, characterized in that, The extraction process is as follows: The mass ratio of raw materials to extraction solvent is 1:5-15; The extraction temperature is 35-75°C.

3. The method for extracting and separating high-purity guaiac blue hydrocarbon from natural plants according to claim 2, characterized in that, The extraction solvent is any one of a polar organic solvent or an inorganic solvent; The polar organic solvent is 30%-75% ethanol; The inorganic solvent is water.

4. The method for extracting and separating high-purity guaiac blue hydrocarbon from natural plants according to claim 1, characterized in that, The merging and extraction process is as follows: First, the guaiac blue oil extract was filtered through a filter membrane to remove impurities. Then, low-temperature vacuum concentration is used to obtain an initial extract with a specific gravity of 1.05-1.1, wherein the concentration temperature is controlled within 40-50°C and the concentration pressure is 10-760 mmHg.

5. The method for extracting and separating high-purity guaiac blue hydrocarbon from natural plants according to claim 4, characterized in that, The extraction and distillation process of the initial extract is as follows: (1) Add an equal volume of organic solvent to the concentrated liquid at the top of the initial extract for extraction. After stirring, let stand for 8 hours. After the layers are completely separated, release the concentrated liquid phase to achieve the first impurity removal. (2) Add ethyl acetate or chloroform to the released concentrated liquid phase until no organic solvent is produced in the combined concentrated liquid phase, and obtain a completely concentrated liquid for later use to achieve the second impurity removal. (3) Distillation: Add the upper part of the fully concentrated extract to the reaction vessel, add 5-50% of the mass of the upper extract of pure water, raise the temperature to 110°C for distillation, and carry out the third impurity removal. (4) Cool the mixture with cooling water to room temperature to obtain distilled extract, i.e. crude guaiac blue oil.

6. The method for extracting and separating high-purity guaiac blue hydrocarbons from natural plants according to claim 1, characterized in that, The sample preparation process for the gradient silica gel chromatography method described above is as follows: First, add 5 times the amount of n-hexane to the crude guaiac blue oil to dissolve it completely, and obtain a solution. Next, add an equal volume of 0.1%-1% sodium hydroxide aqueous solution to the solution, wash three times, release the sodium hydroxide aqueous solution, add pure water and wash until neutral, add anhydrous sodium sulfate to the hexane phase to dehydrate, and then concentrate to a specific gravity of 1.

1. Finally, add 1.5 times the amount of silica gel to the crude guaiac blue oil and stir well. Then, dry the mixture in a vacuum drying oven to obtain a sample suitable for chromatography.

7. The method for extracting and separating high-purity guaiac blue hydrocarbon from natural plants according to claim 1, characterized in that, The decolorization and crystallization process is as follows: First, an organic solvent is added to the concentrated guaiac blue oil extract to dissolve it; Secondly, when heated to 40-75°C, add 1%-5% by weight of concentrated guaiac blue oil extract and needle-grade activated carbon for decolorization; Finally, the product is freeze-crystallized to obtain a high-purity guaiacol product.

8. The method for extracting and separating high-purity guaiac blue hydrocarbon from natural plants according to claim 1, characterized in that, During the chromatography process, the organic solvent system used is either hexane-ethyl acetate or hexane-chloroform. The amount of silica gel used is 5-10 times that used for silica gel sample preparation. Thin-layer chromatography and gas chromatography are used for monitoring during the chromatography process to collect the guaiac blue oil hydrocarbon fragments and combine them to obtain concentrated guaiac blue oil hydrocarbon extract.

9. A system for extracting and separating high-purity guaiac blue hydrocarbons from natural plants, characterized in that, The system comprises the following components connected in sequence: An extraction system for extracting guaiac blue hydrocarbon from natural plant raw materials containing guaiac blue hydrocarbon includes a monitoring device, a control system, and a first extraction device, a second extraction device, and a third extraction device arranged in sequence. The first extraction device, the second extraction device, and the third extraction device are respectively provided with a solvent inlet, a feed inlet, an extract outlet, and a discharge outlet. The first extraction device and the second extraction device are respectively provided with a first connecting port and a second connecting port. The monitoring device includes a concentration monitor and a flow meter, which are respectively installed at the solvent inlet, feed inlet, extract outlet, and discharge outlet; The control system includes a controller and several solenoid valves. The solenoid valves are respectively located at the solvent inlet, feed inlet, extract outlet, discharge outlet and communication port. The controller is electrically connected to the solenoid valves, concentration monitor and flow meter respectively. The reactor has a filter membrane installed at its input end, and the input end of the reactor is connected to the extract outlets of the first extraction device, the second extraction device, and the third extraction device, respectively. An extraction distillation machine, with its input end connected to the output end of the reaction vessel; A silica gel chromatography column is connected at its input end to the extraction distillation machine.

10. The system for extracting and separating high-purity guaiac blue hydrocarbons from natural plants according to claim 9, characterized in that, The first extraction device includes a first outer shell, and a first extraction part and a first separation part disposed inside the first outer shell and arranged vertically. The first extraction part is separated from the outer shell, and a cable is wound around the outside of the first extraction part. Both ends of the cable are connected to an AC power generator. The top of the first extraction section has a first feed inlet and a first solvent input inlet on opposite sides, and the bottom of the first extraction section has a first communication port that communicates with the first separation section. The first separating part is spaced apart from the first outer shell and forms a first filter cavity with the first outer shell. The top of the first separating part is connected to the first communication port. A plurality of first filter holes are evenly arranged on the side wall of the first separating part. The bottom of the first separating part is rotatably connected to the first outer shell. A first discharge port is provided at the bottom of the first separating part. The bottom outer side of the first filter chamber is provided with a first extract outlet; The first feed inlet, the first solvent inlet, the first connecting port, the first discharge port, and the first extract outlet are each equipped with a first solenoid valve, and the first discharge port and the first extract outlet are each equipped with a first concentration monitor and a first flow meter. The second extraction device includes an inner rotating body, an outer rotating body, and a second outer shell arranged sequentially from the inside to the outside. The inner rotating body and the outer rotating body are spaced apart. The inner rotating body and the outer rotating body are controlled independently. The inner rotating body and the outer rotating body rotate in opposite directions, and the rotation speed of the inner rotating body is greater than that of the outer rotating body. An annular second filter chamber is provided between the inner rotating body and the outer rotating body. The top surface of the inner rotating body is conical with a taper of less than 15°, and the bottom of the inner rotating body is rotatably connected to the second outer shell. The outer rotating body and the second outer shell are separated by a gap and are rotatably connected. The outer rotating body is higher than the inner rotating body. The top of the outer rotating body is provided with a first feed port. Two rings of second solvent inlets are evenly arranged around the periphery of the outer rotating body. A second discharge port is provided on one side of the bottom of the outer rotating body. The two rings of second solvent inlets are respectively lower than the highest point of the cone surface and higher than the lowest point of the cone surface; The inner and outer rotating bodies are respectively connected to the inner and outer rotating bodies on the inner and outer sides of the second filter cavity. A second communication port is provided at the top of the second filter cavity. A plurality of second filter holes are evenly provided on the top plate of the annular second filter cavity. A second extract outlet is provided on the bottom plate of the annular second filter cavity. The second solvent inlet, the second extract outlet, the second discharge outlet, and the second connecting port are each equipped with a second solenoid valve, and the second extract outlet and the second discharge outlet are each equipped with a second concentration monitor and a second flow meter. The third extraction device includes an extraction tank, a buffer tank, and a metering tank. The top of the extraction tank is provided with a third feed inlet, one side of the top of the extraction tank is provided with a third solvent inlet, and the bottom of the extraction tank is provided with a third extract outlet. The inlet of the buffer tank is connected to the outlet of the third extract, and the outlet of the buffer tank is connected to both the reaction vessel and the extraction tank. The output port of the metering tank is connected to the third solvent input port; The third solvent inlet, the third feed inlet, and the third extract outlet are respectively equipped with a third solenoid valve, a third concentration monitor, and a third flow meter; The AC generator, the first solenoid valve, the first flow meter, the first concentration monitor, the second solenoid valve, the second flow meter, the second concentration monitor, and the third solenoid valve, the third flow meter, and the third concentration monitor are respectively connected to the controller.

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