CN104770629A - Supercritical CO2 extraction method for high flavone content propolis - Google Patents
Supercritical CO2 extraction method for high flavone content propolis Download PDFInfo
- Publication number
- CN104770629A CN104770629A CN201510129680.1A CN201510129680A CN104770629A CN 104770629 A CN104770629 A CN 104770629A CN 201510129680 A CN201510129680 A CN 201510129680A CN 104770629 A CN104770629 A CN 104770629A
- Authority
- CN
- China
- Prior art keywords
- propolis
- extraction
- supercritical
- raw material
- flavone content
- 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.)
- Granted
Links
- 238000000605 extraction Methods 0.000 title claims abstract description 40
- 241000241413 Propolis Species 0.000 title claims abstract description 39
- 229940069949 propolis Drugs 0.000 title claims abstract description 39
- 229930003944 flavone Natural products 0.000 title claims abstract description 28
- 235000011949 flavones Nutrition 0.000 title claims abstract description 28
- GAMYVSCDDLXAQW-AOIWZFSPSA-N Thermopsosid Natural products O(C)c1c(O)ccc(C=2Oc3c(c(O)cc(O[C@H]4[C@H](O)[C@@H](O)[C@H](O)[C@H](CO)O4)c3)C(=O)C=2)c1 GAMYVSCDDLXAQW-AOIWZFSPSA-N 0.000 title claims abstract description 10
- VHBFFQKBGNRLFZ-UHFFFAOYSA-N vitamin p Natural products O1C2=CC=CC=C2C(=O)C=C1C1=CC=CC=C1 VHBFFQKBGNRLFZ-UHFFFAOYSA-N 0.000 title claims abstract description 10
- 150000002212 flavone derivatives Chemical class 0.000 title claims abstract 8
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims abstract description 27
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 26
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 20
- 238000000034 method Methods 0.000 claims abstract description 17
- 239000000284 extract Substances 0.000 claims abstract description 14
- 238000000926 separation method Methods 0.000 claims abstract description 10
- 238000009736 wetting Methods 0.000 claims abstract description 5
- 239000000463 material Substances 0.000 claims abstract description 3
- 239000012670 alkaline solution Substances 0.000 claims abstract 3
- 239000002994 raw material Substances 0.000 claims description 19
- 150000002213 flavones Chemical class 0.000 claims description 18
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 claims description 12
- 239000003292 glue Substances 0.000 claims description 9
- 229920000168 Microcrystalline cellulose Polymers 0.000 claims description 7
- 239000012530 fluid Substances 0.000 claims description 7
- 235000019813 microcrystalline cellulose Nutrition 0.000 claims description 7
- 239000008108 microcrystalline cellulose Substances 0.000 claims description 7
- 229940016286 microcrystalline cellulose Drugs 0.000 claims description 7
- 230000000694 effects Effects 0.000 claims description 6
- 238000002156 mixing Methods 0.000 claims description 6
- 229910000029 sodium carbonate Inorganic materials 0.000 claims description 6
- 239000000126 substance Substances 0.000 claims description 6
- 239000004480 active ingredient Substances 0.000 claims description 5
- HEMHJVSKTPXQMS-UHFFFAOYSA-M sodium hydroxide Substances [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 5
- 239000003513 alkali Substances 0.000 claims description 4
- 229930003935 flavonoid Natural products 0.000 claims description 4
- 150000002215 flavonoids Chemical class 0.000 claims description 4
- 235000017173 flavonoids Nutrition 0.000 claims description 4
- 239000011259 mixed solution Substances 0.000 claims description 4
- 230000008569 process Effects 0.000 claims description 4
- 238000010298 pulverizing process Methods 0.000 claims description 4
- 230000010261 cell growth Effects 0.000 claims 1
- 238000000194 supercritical-fluid extraction Methods 0.000 abstract description 2
- 241000256844 Apis mellifera Species 0.000 description 5
- 239000000203 mixture Substances 0.000 description 5
- 238000005516 engineering process Methods 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- -1 flavone compound Chemical class 0.000 description 2
- 210000004907 gland Anatomy 0.000 description 2
- 230000036541 health Effects 0.000 description 2
- 229910001385 heavy metal Inorganic materials 0.000 description 2
- 241000256837 Apidae Species 0.000 description 1
- 230000000844 anti-bacterial effect Effects 0.000 description 1
- 230000003110 anti-inflammatory effect Effects 0.000 description 1
- 230000001139 anti-pruritic effect Effects 0.000 description 1
- 230000000259 anti-tumor effect Effects 0.000 description 1
- 239000003963 antioxidant agent Substances 0.000 description 1
- 230000003078 antioxidant effect Effects 0.000 description 1
- 235000006708 antioxidants Nutrition 0.000 description 1
- 239000003908 antipruritic agent Substances 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 239000008280 blood Substances 0.000 description 1
- 210000004369 blood Anatomy 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000012159 carrier gas Substances 0.000 description 1
- 210000004027 cell Anatomy 0.000 description 1
- 210000002421 cell wall Anatomy 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000000084 colloidal system Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000007598 dipping method Methods 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 230000002218 hypoglycaemic effect Effects 0.000 description 1
- 238000002955 isolation Methods 0.000 description 1
- 150000002632 lipids Chemical class 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 230000028327 secretion Effects 0.000 description 1
- 239000000080 wetting agent Substances 0.000 description 1
Landscapes
- Jellies, Jams, And Syrups (AREA)
- Medicines Containing Material From Animals Or Micro-Organisms (AREA)
Abstract
The invention relates to a supercritical CO2 extraction method for high flavone content propolis. The specific method includes: crushing coarse propolis, performing wetting with an alkaline solution, conduct microwave wall-breaking, then putting the product into a supercritical CO2 extraction kettle with three-stage separation, and taking hydrous ethanol and ethyl acetate in certain proportion as a mixed carrying agent to perform supercritical extraction, thus obtaining the high flavone content propolis. According to the invention, firstly the coarse propolis wetted by the weak alkaline solution is subjected to microwave treatment, then the hydrous ethanol and ethyl acetate in certain proportion are taken as the carrying agent to form an extraction medium with wide polarity range together with CO2, and the extraction medium can effectively extract different polarity active components in the coarse propolis. In addition, three-stage separation is also carried out on the extracted material by a multi-gradient temperature and pressure adjustment system to obtain low flavone content supercritical propolis and high flavone content supercritical propolis respectively. The method provided by the invention solves the problem of super low flavone content of supercritically extracted propolis.
Description
Technical field
The present invention is the extractive technique in the fields such as food, health products and medicine, be a kind of with propolis hair glue for raw material, use supercritical CO
2the method of bee glue extracting.
Background technology
Propolis is the resinous matter that honeybee gathers from the newborn twig of glue source plant, is mixed into the colloid substance of its mandibular gland, wax gland secretion reprocessabilty through honeybee.Propolis resource is more precious, and every 50,000 honeybees can only collect the propolis of about 100 g for 1 year, and containing the flavone compound of more than 70 kinds in propolis.Research proves, enriching and the bioactivator of uniqueness contained by propolis, make it have antibacterial, anti-inflammatory, antipruritic, anti-oxidant, strengthen immune, hypoglycemic, reducing blood lipid, the several functions such as antitumor, medical treatment, health-care effect is widely had to human body, now become the focus of various countries' scientific research, and become emerging and extremely praise highly
health products.
At present, the method for extracting propolis of main flow mainly ethonal extraction and gradually prosperous get up supercritical CO
2abstraction technique.Supercritical CO
2abstraction technique is the CO utilized under supercriticality
2fluid has gas and liquid double grading simultaneously, then substance dissolves is out reduced pressure or the raised temperature of carrier gas from matrix, supercritical CO
2solubility reduce, thus reach the object of extraction and isolation.
The problem having lead element to exceed standard in the propolis that ethonal extraction method is extracted, must carry out de-splicer's sequence, and the production process of supercritical carbon dioxide extracting propolis is pollution-free, effectively can remove heavy metal.But, common supercritical CO
2also there is following point in bee glue extracting technique:
1) due to common supercritical CO
2due to CO in extraction process
2polarity more weak, it only can extract propolis nonpolar state composition and the less composition of polarity, and the extracts active ingredients poor effect relatively large to polarity, although solve the problem of the heavy metal in propolis, also causes Flavonoids in Propolis content very low.2) propolis caking property is very strong, is easy to lump in extraction kettle, makes CO
2fluid and carry agent by extraction axe difficulty strengthen, affect the extraction efficiency of active ingredient.3) one-level or two-stage separation kettle is generally only had at separating end, can not effectively to target component and carry agent and be separated.
Above-mentioned reason, causes supercritical CO
2extraction energy consumption is high, and cost is high, extracted amount is relatively little, constrains the application of supercritical extraction technique in effective bee glue components extracts.The present invention is exactly a kind of extracting method of inventing for the problems referred to above.
Summary of the invention
The object of the invention is to invention one supercritical CO
2prepare the method for high flavones propolis.
Concrete technology step of the present invention:
(1) by propolis hair rubber pulverizing, add in certain proportion in mao glue with sodium carbonate liquor and mix, wetting (raw material A);
(2) by " raw material A " microwave treatment, microcrystalline cellulose is added, mixing (raw material B);
(3) " raw material B " is put into the supercritical COs with three grades of separation
2in extraction kettle, using ethyl acetate and hydrous ethanol mixed solution as carrying agent, and successively add in extraction process and carry agent and carry out supercritical extract;
(4) obtain the different propolis of flavones content from separating still I and separating still II, and carry agent mainly from separating still III releasing.
Know-why of the present invention:
1. common supercritical CO
2due to CO in extraction process
2polarity more weak, it only can extract nonpolar state composition and the less composition of polarity, but the extracts active ingredients poor effect relatively large to polarity.Flavones is the general name of a compounds, and polarity scope is very wide, need higher extraction conditions just can extract, and it is dissolved in the reagent such as alkali lye, ethanol and ethyl acetate, and flavones solubility can strengthen further under elevated pressure conditions.So by alkali lye as wetting agent, the ethyl acetate of certain proportioning and hydrous ethanol mixed solution are as carrying agent as carrying agent and CO
2form the fluid media (medium) that polarity scope is very wide, fluid media (medium) effectively can extract propolis and flavones in mao glue.
2. flavone compound is stored in raw cell inside, is carrying out microwave treatment, effectively can destroy raw material cell wall, flavones is effectively discharged with after dipping by lye.
3. microcrystalline cellulose is a kind of good anticaking agent, prevents raw material from luming in extraction process and affects permeability and the extraction effect of fluid, and " adopting the mode of successively adding and carrying agent " when also allowing the sticky materials such as propolis extract becomes possibility.It allows raw material be in always and carries in the extraction environment of agent, be conducive to extracting more Flavonoid substances.
Advantage of the present invention:
1. have employed the wall breaking technology that alkali lye soaks microwave treatment, be conducive to the release of active ingredient.
2. adopt microcrystalline cellulose as anticaking agent, prevent extraction axe Raw from luming and affecting circulation and the effect of extracting of fluid.
3. have employed the mode of successively adding and carrying agent, allow raw material be in always and carry in the extraction environment of agent, be conducive to extracting more Flavonoid substances.
4., by many gradient temperatures pressure regulating system, three grades of separation are carried out to extracting substance, obtains the propolis of high flavones content.
Detailed description of the invention
Embodiment 1:
By 7kg hair rubber pulverizing, add the wetting 10h of sodium carbonate liquor mixing of 0.9L 1mol/L; Then by its point 14 parts every part microwave 100s, add 560g microcrystalline cellulose, mixing evenly; Put into and there are three grades of supercritical COs be separated
2in extraction kettle, add continuously with the flow of 35 mL/min and carry agent and extract, carrying agent is ethyl acetate and 95% ethanol, and the two ratio is 1:10(V/V).Wherein extracting pressure is 35MPa, and extraction temperature is 55 DEG C, and extraction time is 4.0h.From separation axe I, obtain 1.55kg propolis, flavones content is 8.21%, lead content≤0.01mg/kg; From separation axe II, obtain 0.73kg propolis, flavones content is 18.31%, lead content≤0.01mg/kg.
Embodiment 2:
By 9kg hair rubber pulverizing, add the wetting 8h of sodium carbonate liquor mixing of 0.8L 0.8mol/L; Then by its point 18 parts every part microwave 70s, then add 410g microcrystalline cellulose, mixing evenly; Put into and there are three grades of supercritical COs be separated
2in extraction kettle, add continuously with the flow of 25mL/min and carry agent and extract, carrying agent is ethyl acetate and 95% ethanol, and the two ratio is 2:10(V/V).Wherein extracting pressure is 30MPa, and extraction temperature is 45 DEG C, and extraction time is 5.0h.From separation axe I, obtain 1.73kg propolis, flavones content is 6.53%, lead content≤0.01mg/kg; From separation axe II, obtain 0.87kg propolis, flavones content is 15.24%, lead content≤0.01mg/kg.
Claims (6)
1. the supercritical CO of a high flavones content propolis
2extracting process, is characterized in that:
(1) by propolis hair rubber pulverizing, with the sodium carbonate liquor of 0.5-1.8mol/L with 0.5-2:10(sodium carbonate liquor/mL: ratio hair glue/g) is added in mao glue and mixed, wetting 4-12h(raw material A);
(2) by " raw material A " microwave 30-120s, 2-10% microcrystalline cellulose is added, mixing (raw material B);
(3) " raw material B " is put into the supercritical COs with three grades of separation
2in extraction kettle, with ethyl acetate and hydrous ethanol (1-3:10, V/V, concentration of alcohol 90-100%) mixed solution as carrying agent, and successively add in extraction process and carry agent and carry out supercritical extract, flow is 20-40
ML/min; Wherein extracting pressure is 25 ~ 40MPa, and extraction temperature is 35 ~ 65 DEG C, and extraction time is 2.5 ~ 5h;
(4) obtain the different propolis of flavones content from separating still I and separating still II, and carry agent mainly from separating still III releasing, the propolis flavone content wherein obtained in separating still I is 3-10%; The propolis flavone content obtained in separating still II is 12-20%.
2. method according to claim 1, is characterized in that: raw material A sodium carbonate liquor soaks, and flavones is soluble in alkaline solution on the one hand, is conducive to the extraction of flavones; After raw material absorbs alkali lye on the other hand, cell expansion easily breaks, and is conducive to follow-up microwave frequency measurment.
3. according to claim 1 and claim 2, it is characterized in that: raw material B carries out of short duration microwave frequency measurment process, be conducive to release and the extraction of active ingredient.
4. the supercritical CO of a kind of high flavones content propolis according to claim 1
2extracting process, is characterized in that: raw material with the addition of microcrystalline cellulose, prevents supercritical CO
2during extraction, because of material thickness, caking and cause extraction kettle to block, fluid is not smooth, and extraction effect is poor.
5. method according to claim 1, is characterized in that: use ethyl acetate and hydrous ethanol mixed solution as carrying agent, the CO under itself and supercriticality
2define polarity scope abundanter, wider carry agent, be conducive to the extraction of flavones.
6. according to claim 1,2,3,4, described in 5, in extraction process, adopt the mode of adding continuously and carrying agent, allow raw material be in have always and carry in the extraction environment of agent, thus more effectively extract the Flavonoid substances in raw material.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510129680.1A CN104770629B (en) | 2015-03-24 | 2015-03-24 | A kind of supercritical CO of high flavones content propolis2Extracting process |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510129680.1A CN104770629B (en) | 2015-03-24 | 2015-03-24 | A kind of supercritical CO of high flavones content propolis2Extracting process |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN104770629A true CN104770629A (en) | 2015-07-15 |
| CN104770629B CN104770629B (en) | 2018-02-09 |
Family
ID=53612652
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201510129680.1A Active CN104770629B (en) | 2015-03-24 | 2015-03-24 | A kind of supercritical CO of high flavones content propolis2Extracting process |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN104770629B (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106993789A (en) * | 2017-03-17 | 2017-08-01 | 江苏鸿祺生物科技有限公司 | A kind of method that subcritical multiple mixed solvent extracts high-quality propolis |
| CN114271462A (en) * | 2021-12-28 | 2022-04-05 | 南昌蜂芝缘健康科技有限公司 | A method for preparing propolis by supercritical carbon dioxide extraction |
| CN114588181A (en) * | 2022-04-01 | 2022-06-07 | 江苏蜂奥生物科技有限公司 | Propolis extract and production process thereof |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1389218A (en) * | 2002-07-12 | 2003-01-08 | 江苏大学 | Method for supercritical extraction and microwave-assisted extraction separation of effective components of propolis |
| CN102429140A (en) * | 2011-10-27 | 2012-05-02 | 喀左县春蕾特产品开发中心 | Supercritical CO2Method for extracting propolis with fluid |
-
2015
- 2015-03-24 CN CN201510129680.1A patent/CN104770629B/en active Active
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1389218A (en) * | 2002-07-12 | 2003-01-08 | 江苏大学 | Method for supercritical extraction and microwave-assisted extraction separation of effective components of propolis |
| CN102429140A (en) * | 2011-10-27 | 2012-05-02 | 喀左县春蕾特产品开发中心 | Supercritical CO2Method for extracting propolis with fluid |
Non-Patent Citations (4)
| Title |
|---|
| 王震宇: "不同夹带剂条件下超临界CO2萃取蜂胶黄酮的研究", 《中国优秀硕士学位论文全文数据库 工程科技I辑》 * |
| 盛文胜: "蜂胶中黄酮的提取及应用研究", 《中国优秀硕士学位论文全文数据库 工程科技I辑》 * |
| 郭华等: "微波对蜂胶黄酮提取率影响的研究", 《江苏食品与发酵》 * |
| 高荫榆等: "蜂胶黄酮类化合物超临界萃取工艺研究", 《食品科学》 * |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106993789A (en) * | 2017-03-17 | 2017-08-01 | 江苏鸿祺生物科技有限公司 | A kind of method that subcritical multiple mixed solvent extracts high-quality propolis |
| CN114271462A (en) * | 2021-12-28 | 2022-04-05 | 南昌蜂芝缘健康科技有限公司 | A method for preparing propolis by supercritical carbon dioxide extraction |
| CN114271462B (en) * | 2021-12-28 | 2024-02-20 | 南昌蜂芝缘健康科技有限公司 | Preparation method of supercritical carbon dioxide extracted propolis |
| CN114588181A (en) * | 2022-04-01 | 2022-06-07 | 江苏蜂奥生物科技有限公司 | Propolis extract and production process thereof |
Also Published As
| Publication number | Publication date |
|---|---|
| CN104770629B (en) | 2018-02-09 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN104311688B (en) | Method for extracting and separating dendrobium nobile polysaccharide and total alkali | |
| CN102839053B (en) | Method for extracting aurantiamarin from orange peel | |
| CN107115251A (en) | A kind of original plant juice of oil control and acne removal and preparation method thereof | |
| CN101781606A (en) | Extraction method of rosa rugosa essential oil | |
| CN101513211A (en) | Complex biological preservative formula of citrus fruit chitosan oligosaccharide | |
| CN105434256A (en) | Natural emulsion, and preparation method and applications thereof | |
| CN110464682A (en) | A kind of peach gum composition, preparation method and application | |
| CN101439014B (en) | A kind of white fungus extract and preparation method thereof | |
| CN104770629A (en) | Supercritical CO2 extraction method for high flavone content propolis | |
| CN105440003A (en) | Method for efficiently extracting procyanidine in sea-buckthorn seeds at low temperature and with low energy consumption | |
| CN105801391B (en) | The method that purple perilla extracts perillaldehyde and anthocyanin | |
| CN109010504A (en) | A kind of extracting method of lycium ruthenicum general flavone | |
| CN112076129A (en) | An extract of natural plant material mixture and its extraction method | |
| CN107652337B (en) | Method for extracting and preparing anthocyanin such as black rice, black beans, purple potatoes, roses, peonies and the like | |
| CN103396891A (en) | Method for extracting essential oil by taking jackfruit peel as raw material | |
| CN108570031A (en) | A kind of extracting method of lycium ruthenicum anthocyanidin | |
| CN104921997B (en) | The whitening of a kind of peony ultrahigh-pressure extraction method and its preparation, anti-oxidant Essence | |
| CN106380458A (en) | Method for extracting anthocyanidin in blueberry | |
| CN104719895A (en) | Grape polyphenol microcapsule health care product and preparation method thereof | |
| CN103536622A (en) | Application of sargassum fusiforme sulphated polysaccharide in preparation of anti-aging drugs and healthcare products | |
| CN105769727A (en) | Whitening skin-care product containing sea cucumber decoction extract and preparation method of whitening skin-care product | |
| CN109082723A (en) | A kind of Leaves of Hippophae L cellulose fibre | |
| CN109287665A (en) | A kind of ginkgolic acid-avermectin compound insecticide and preparation method thereof | |
| CN111039841B (en) | Method for simultaneously extracting carotenoid and polyphenol from green leaf vegetables | |
| CN106108019A (en) | A kind of method of total flavones in microwave-assisted multiplex-enzyme extraction peel of Citrus sinensis Osbeck |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| C06 | Publication | ||
| PB01 | Publication | ||
| EXSB | Decision made by sipo to initiate substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| GR01 | Patent grant | ||
| GR01 | Patent grant |