CN102805755A - Preparation method of high-quality ginkgo flavone - Google Patents
Preparation method of high-quality ginkgo flavone Download PDFInfo
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- CN102805755A CN102805755A CN2011101529466A CN201110152946A CN102805755A CN 102805755 A CN102805755 A CN 102805755A CN 2011101529466 A CN2011101529466 A CN 2011101529466A CN 201110152946 A CN201110152946 A CN 201110152946A CN 102805755 A CN102805755 A CN 102805755A
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Abstract
The invention relates to a preparation method for extracting high-quality ginkgo flavone from ginkgo leaves. The method comprises the following steps of: extracting a crude extracting solution from ginkgo leaves by using deionized water, filtering, depositing in alcohol for removing impurities, removing impurities by using a clarifying agent, enriching ginkgo flavone and lactone, and initially separating by using polar and weakly polar macroporous resins; and removing ginkgoic acid with a resin to finally obtain a ginkgo extract product. The preparation method has the technical advantages: (1) macroporous resins of difference performances are used in a combined way for enriching ginkgo flavone and lactone and removing ginkgoic acid, so that the product quality is enhanced remarkably, and a product is ensured; (b) a production process is simplified, the production period is shortened, and the production cost is reduced; and (c) a nontoxic and harmless organic solvent and a natural clarifying agent are used, so that the residual quantity of toxic and harmful substances in the product is lowered greatly, and the quality of the product is enhanced.
Description
Technical field
The present invention relates to a kind of from from Folium Ginkgo, extracting the method for preparing of high-quality ginkgetin.
Background technology
Ginkgetin mainly is present in the dry stem and leaf of Ginkgoaceae plant Ginkgo biloba Ginkgo biloba L. Semen Ginkgo; Folium Ginkgo is through the plant extract of technical process preparations such as solvent lixiviate separation, purification; The content of ginkgetin can reach 2%-5% in the dried leaves; The effective ingredient of Folium Ginkgo comprises: ginkegetin, different ginkegetin, bilobetin, Quercetin, kaempferol etc., bitter principle is ginkgoic acid A, B, C, M, J etc.
Ginkgo total flavones (FG); At the sixties in 20th century of its extension vessel activity after deliberation; And Preliminary Applications is in clinical acquisition curative effect preferably; After expert's years of researches and exploitation, FG not only has vasodilative effect but also effects such as antiinflammatory, analgesia, free radical resisting, blood fat reducing, antitumor and leukemia is arranged, and has been widely used in every field such as pharmacy, health product, article of everyday use, cosmetics.
All mainly be that raw material extracts ginkgetin at present inside and outside China with the Folium Ginkgo.The method of separation and purification ginkgetin is a lot; Comprise solvent extraction method, supercritical methanol technology, supercritical ultrasonics technology, microwave-assisted lifting manipulation, microwave method, high-speed counter-current method, macroreticular resin absorbing method method, polyamide column chromatography method and enzyme process etc.; Wherein the most ripe and the most frequently used extraction process is a solvent extraction method
(application number: 200610038797), it is characterized in that it is made up of the following step basically: the ethanol mass fraction that step 1. is dissolved in 200 parts of quality with the Folium Ginkgo extract of 1 part of quality is in ethanol-water of 60% to a kind of method of refining ginkgetin; Step 2. is carried out the ultrafiltration first time with the GBE solution in the step 1 under 0.05～0.3MPa pressure and 10～50 ℃ of temperature, ultrafilter membrane is that molecular cut off is 5000,10000 or the ultrafilter membrane of 30000dalton, collects permeate; Step 3. is dissolved in the residue behind the evaporate to dryness of 1 part of quality the dehydrated alcohol of 50 parts of quality again with the permeate concentrating under reduced pressure of step 2 collection; Step 4. adds beta-schardinger dextrin-or modification beta-schardinger dextrin-in the solution of step 3 gained; Make that the ratio of ginkgetin and the amount of substance of beta-schardinger dextrin-or modification beta-schardinger dextrin-is 1: 9～1: 1 in the solution; Earlier in 20～90 ℃ of water-baths, react 15min～5h, react 30min～24h more at normal temperatures; Step 5. is carried out the ultrafiltration second time with reacted product in the step 4 under 0.05～0.3MPa pressure and 10～50 ℃ of temperature; Ultrafilter membrane is that molecular cut off is 5000; 10000 or the ultrafilter membrane of 30000dalton; The liquid that collection is held back after concentrating promptly obtains purified ginkgetin alcoholic solution.
Highly effective abstraction method for preparation of high-purity ginko flavonoid (application number: 200610068733), it is characterized in that may further comprise the steps: A, the Folium Ginkgo when employing leaf in autumn is yellow, preserve the oven dry back; B. Folium Ginkgo is pulverized, subsequent use; C, extract with ethanol; D, extracting solution concentrating under reduced pressure reclaim ethanol; E, with concentrated solution dilution, cooling-sedimentation; F, clear liquid advance the styrene type macroporous resin adsorption column and adsorb; G, use the alcohol solution eluting; H, eluent concentrating under reduced pressure, vacuum drying, crushing packing.
Summary of the invention
So the objective of the invention is for the high-quality ginkgetin preparation technology of preparation from Folium Ginkgo, so that solve existing problem in the technology of producing this product in the market, so that obtain high-recovery and high-quality ginkgetin product.
The object of the invention is mainly realized through following technical process:
Concrete steps are following:
1) from Folium Ginkgo, extracts ginkgetin: the Semen Ginkgo leaf was pulverized 10 orders; Add the deionized water heating and refluxing extraction three times that its weight 5-8 doubly measures, extracted 1.5 hours at every turn, filter extracting solution; Extract slag with deionized water wash; Merge extractive liquid, and cleaning mixture are evaporated to certain proportion, just obtain the crude extract of ginkgetin;
2) crude extract that obtains precipitate with ethanol remove impurity: with process 1) adds anhydrous organic solvent (I) after filtering, and organic solvent content fully stirs, leaves standstill to 30-80% in the adjusting liquid, and settle precipitates is filtered, and the stillness of night is concentrated to does not have alcohol, for use; Organic solvent in the said process (I) comprising: methanol, ethanol, acetone;
3) concentrated solution for use clarifier remove impurity: with 2) is heated to 30 ℃ of addings through pretreated clarifiers (II), fully stirs, and sedimentation 12H whenever stirs once at a distance from 2H, after the sedimentation fully, filters, and the stillness of night is for use; Clarifier in the said process (II) comprising: chitosan, chitin, ZTC1+1;
4) enriching ginkgetin and lactone: utilize the macroporous resin of polarity, low pole to carry out just separating.Place ethanol to soak 24 hours polarity, the low pole macro-reticular adsorbing resin of nonionic, wash resin successively with ethanol, deionized water then; To pass through the resin of said process activation, adorn post with settling methods; With 3) in stillness of night of obtaining; Be splined on the chromatographic column of handling well, filling, adopting water-containing organic solvent (III) that macroporous resin is carried out eluting, Fractional Collections; Concentrating under reduced pressure is collected contains ginkgetin and lactone part, obtains being rich in the concentrated solution of ginkgetin and lactone; The content of organic solvent is 10-90v% in the above-mentioned water-containing organic solvent (III); Organic solvent in the above-mentioned water-containing organic solvent (III) comprises: methanol, ethanol, acetone, n-butyl alcohol.
5) resin removes ginkgoic acid: utilize the macroporous resin of polarity or low pole to carry out just separating.Place ethanol to soak 24 hours the polarity or the low pole macro-reticular adsorbing resin of nonionic, wash resin successively with ethanol, deionized water then; To pass through the resin of said process activation, adorn post with settling methods; With 4) in the concentrated solution that obtains, be splined on the chromatographic column of handling well, filling, collect effluent, concentrating under reduced pressure, drying is waited until final Semen Ginkgo extrac product;
Clarifier used in the said step 3) is pretreated through the code requirement process.
Said step 4), 5) used macro-reticular adsorbing resin comprises and gathers third vinyl, polystyrene resin, polymethacrylate resin, acrylamide and styrene copolymer resin in.
A kind of technical advantage that from Folium Ginkgo, prepares high-quality ginkgetin that this invention is stated is:
A) unite the macroporous resin that uses different performance and come enriching ginkgetin and lactone, deviate from ginkgoic acid, product quality is obviously improved, guaranteed product.
B) simplify production technology, shorten the production cycle, production cost is decreased.
C) use nontoxic organic solvent and natural clarifying agent, greatly reduced the residual quantity of poisonous and harmful substance in the product, improved the quality of product.
Instantiation
Instance 1
1) extract: with the 200g flavonoid of ginkgo biloba is that 2.0% Folium Ginkgo raw material process is pulverized, and puts into the 2000ml triangular flask, adds the hot reflux of 1000ml deionized water and extracts; Extract three times, one time 1.5H/ time, merge three times extracting solution; Be evaporated to d=1.05 (proportion), about 400ml detects through UV; The concentration of ginkgetin is 9.8mg/ml in the concentrated solution, and the effective ingredient response rate is 98%.
2) the concentrated solution 400ml that obtains precipitate with ethanol: with process 1) adds dehydrated alcohol, and ethanol content reaches 50% in the adjusting liquid; Fully stir, leave standstill, settle precipitates is filtered; The stillness of night is concentrated to does not have alcohol, obtains precipitate with ethanol concentrated solution 380ml, detects through UV; The concentration of ginkgetin is 10.1mg/ml in the precipitate with ethanol concentrated solution, and the effective ingredient response rate is 95%.
3) precipitate with ethanol concentrated solution 380ml for use clarifier remove impurity: with 2), be heated to 30 ℃ after, add amount of liquid 0.5% through pretreated clarifier ZTC1+1; Fully stir, sedimentation 12H, every separated 2H stirs once; After the sedimentation fully, it is for use that filtration obtains the 360ml stillness of night, detects through UV; The concentration of ginkgetin is 10.6mg/ml in the stillness of night, and the effective ingredient response rate is 95%.
4) enriching ginkgetin and lactone: with 3) in stillness of night of obtaining, be splined on the LS-46D chromatographic column of handling well, filling, adopting aquiferous ethanol that macroporous resin is carried out eluting; Collect the 40-70% ethanol elution; Concentrating under reduced pressure is collected contains ginkgetin and lactone part, obtains being rich in the concentrated solution 280ml of ginkgetin and lactone, detects through UV; The concentration of ginkgetin is 12.9mg/ml in the concentrated solution, and the effective ingredient response rate is 90%.
5) resin is deviate from ginkgoic acid: with 4) in the concentrated solution that obtains, be splined on the HPD-5000 chromatographic column of handling well, filling, collect effluent; Concentrating under reduced pressure, drying is waited until final Semen Ginkgo extrac product 12.3g; Detect through UV, the content of ginkgetin reaches 26.3% in the final products, and HPLC detects bilobalide content greater than 6%; Ginkgoic acid content is less than 0.005ppm, and the effective ingredient response rate is 80%.
Instance 2
1) extract: with the 200g flavonoid of ginkgo biloba is that 2.0% Folium Ginkgo raw material process is pulverized, and puts into the 2000ml triangular flask, adds the hot reflux of 1000ml deionized water and extracts; Extract three times, one time 1.5H/ time, merge three times extracting solution; Be evaporated to d=1.08 (proportion), about 375ml detects through UV; The concentration of ginkgetin is 10.45mg/ml in the concentrated solution, and the effective ingredient response rate is 98%.
2) the concentrated solution 375ml that obtains precipitate with ethanol: with process 1) adds dehydrated alcohol, and ethanol content reaches 65% in the adjusting liquid; Fully stir, leave standstill, settle precipitates is filtered; The stillness of night is concentrated to does not have alcohol, obtains precipitate with ethanol concentrated solution 500ml, detects through UV; The concentration of ginkgetin is 7.7mg/ml in the precipitate with ethanol concentrated solution, and the effective ingredient response rate is 96.3%.
3) precipitate with ethanol concentrated solution 500ml for use clarifier remove impurity: with 2), be heated to 30 ℃ after, add amount of liquid 0.3% through pretreated clarifier ZTC1+1; Fully stir, sedimentation 12H, every separated 2H stirs once; After the sedimentation fully, it is for use that filtration obtains the 485ml stillness of night, detects through UV; The concentration of ginkgetin is 7.92mg/ml in the stillness of night, and the effective ingredient response rate is 96%.
4) enriching ginkgetin and lactone: with 3) in stillness of night of obtaining, be splined on the LS-46D chromatographic column of handling well, filling, adopting aquiferous ethanol that macroporous resin is carried out eluting; Collect the 40-70% ethanol elution; Concentrating under reduced pressure is collected contains ginkgetin and lactone part, obtains being rich in the concentrated solution 350ml of ginkgetin and lactone, detects through UV; The concentration of ginkgetin is 9.9mg/ml in the concentrated solution, and the effective ingredient response rate is 94%.
5) resin is deviate from ginkgoic acid: with 4) in the concentrated solution that obtains, be splined on the HPD-5000 chromatographic column of handling well, filling, collect effluent; Concentrating under reduced pressure, drying is waited until final Semen Ginkgo extrac product 12.76g; Detect through UV, the content of ginkgetin reaches 29.3% in the final products, and HPLC detects bilobalide content greater than 6%; Ginkgoic acid content is less than 0.005ppm, and the effective ingredient response rate is 93.5%.
Instance 3
1) extract: with the 200g flavonoid of ginkgo biloba is that 2.0% Folium Ginkgo raw material process is pulverized, and puts into the 2000ml triangular flask, adds the hot reflux of 1000ml deionized water and extracts; Extract three times, one time 1.5H/ time, merge three times extracting solution; Be evaporated to d=1.08 (proportion), about 375ml detects through UV; The concentration of ginkgetin is 10.45mg/ml in the concentrated solution, and the effective ingredient response rate is 98%.
2) the concentrated solution 375ml that obtains precipitate with ethanol: with process 1) adds dehydrated alcohol, and ethanol content reaches 80% in the adjusting liquid; Fully stir, leave standstill, settle precipitates is filtered; The stillness of night is concentrated to does not have alcohol, obtains precipitate with ethanol concentrated solution 355ml, detects through UV; The concentration of ginkgetin is 10.8mg/ml in the precipitate with ethanol concentrated solution, and the effective ingredient response rate is 95.4%.
3) precipitate with ethanol concentrated solution 355ml for use clarifier remove impurity: with 2), be heated to 30 ℃ after, add amount of liquid 0.5% through pretreated clarifier ZTC1+1; Fully stir, sedimentation 12H, every separated 2H stirs once; After the sedimentation fully, it is for use that filtration obtains the 342ml stillness of night, detects through UV; The concentration of ginkgetin is 11.06mg/ml in the stillness of night, and the effective ingredient response rate is 94.6%.
4) enriching ginkgetin and lactone: with 3) in stillness of night of obtaining, be splined on the LS-46D chromatographic column of handling well, filling, adopting aquiferous ethanol that macroporous resin is carried out eluting; Collect the 40-70% ethanol elution; Concentrating under reduced pressure is collected contains ginkgetin and lactone part, obtains being rich in the concentrated solution 273ml of ginkgetin and lactone, detects through UV; The concentration of ginkgetin is 13.3mg/ml in the concentrated solution, and the effective ingredient response rate is 90.8%.
5) resin is deviate from ginkgoic acid: with 4) in the concentrated solution that obtains, be splined on the HPD-5000 chromatographic column of handling well, filling, collect effluent; Concentrating under reduced pressure, drying is waited until final Semen Ginkgo extrac product 11.99g; Detect through UV, the content of ginkgetin reaches 28.5% in the final products, and HPLC detects bilobalide content greater than 6%; Ginkgoic acid content is less than 0.005ppm, and the effective ingredient response rate is 85.7%.
Claims (3)
1. the method for preparing of a high-quality ginkgetin is characterized in that:
1) from Folium Ginkgo, extracts ginkgetin: the Semen Ginkgo leaf was pulverized 10 orders; Add the deionized water heating and refluxing extraction three times that its weight 5-8 doubly measures, extracted 1.5 hours at every turn, filter extracting solution; Extract slag with deionized water wash; Merge extractive liquid, and cleaning mixture are evaporated to certain proportion, just obtain the crude extract of ginkgetin;
2) crude extract that obtains precipitate with ethanol remove impurity: with process 1) adds anhydrous organic solvent (I) after filtering, and organic solvent content fully stirs, leaves standstill to 30-80% in the adjusting liquid, and settle precipitates is filtered, and the stillness of night is concentrated to does not have alcohol, for use; Organic solvent in the said process (I) comprising: methanol, ethanol, acetone;
3) concentrated solution for use clarifier remove impurity: with 2) is heated to 30 ℃ of addings through pretreated clarifiers (II), fully stirs, and sedimentation 12H whenever stirs once at a distance from 2H, after the sedimentation fully, filters, and the stillness of night is for use; Clarifier in the said process (II) comprising: chitosan, chitin, ZTC1+1;
4) enriching ginkgetin and lactone: utilize the macroporous resin of polarity, low pole to carry out just separating, polarity, the low pole macro-reticular adsorbing resin of nonionic placed ethanol immersion 24 hours, wash resin successively with ethanol, deionized water then; To pass through the resin of said process activation, adorn post with settling methods; With 3) in stillness of night of obtaining; Be splined on the chromatographic column of handling well, filling, adopting water-containing organic solvent (III) that macroporous resin is carried out eluting, Fractional Collections; Concentrating under reduced pressure is collected contains ginkgetin and lactone part, obtains being rich in the concentrated solution of ginkgetin and lactone; The content of organic solvent is 10-90v% in the above-mentioned water-containing organic solvent (III); Organic solvent in the above-mentioned water-containing organic solvent (III) comprises: methanol, ethanol, acetone, n-butyl alcohol.
5) resin removes ginkgoic acid: utilize the macroporous resin of polarity or low pole to carry out just separating, place ethanol to soak 24 hours the polarity or the low pole macro-reticular adsorbing resin of nonionic, wash resin successively with ethanol, deionized water then; To pass through the resin of said process activation, adorn post with settling methods; With 4) in the concentrated solution that obtains, be splined on the chromatographic column of handling well, filling, collect effluent, concentrating under reduced pressure, drying is waited until final Semen Ginkgo extrac product.
2. by the method for preparing of the described a kind of high-quality ginkgetin of claim 1, it is characterized in that: clarifier used in the said step 3) is pretreated through the code requirement process.
3. by the method for preparing of the described a kind of high-quality ginkgetin of claim 1, it is characterized in that: used macro-reticular adsorbing resin comprises and gathers third vinyl, polystyrene resin, polymethacrylate resin, acrylamide and styrene copolymer resin said step 4), 5).
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103110671A (en) * | 2013-01-29 | 2013-05-22 | 华中科技大学 | Method for removing ginkgolic acid and heavy metals in ginkgo biloba extract by using nanometer material |
| CN105380750A (en) * | 2015-10-22 | 2016-03-09 | 俞祖勋 | Making method for anti-bacterial non-woven fabric, anti-bacterial paper diaper and use method |
| CN107873932A (en) * | 2017-11-30 | 2018-04-06 | 胡江宇 | Crisp sugar of gingko and preparation method thereof |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1931199A (en) * | 2006-09-25 | 2007-03-21 | 辽宁大生药业有限公司 | Double resin process for preparing high quality active gingko leaf component extract |
| CN101703534A (en) * | 2009-09-29 | 2010-05-12 | 武征杰 | Natural ginkgo extract capsule and preparation method thereof |
-
2011
- 2011-06-02 CN CN2011101529466A patent/CN102805755A/en active Pending
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1931199A (en) * | 2006-09-25 | 2007-03-21 | 辽宁大生药业有限公司 | Double resin process for preparing high quality active gingko leaf component extract |
| CN101703534A (en) * | 2009-09-29 | 2010-05-12 | 武征杰 | Natural ginkgo extract capsule and preparation method thereof |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103110671A (en) * | 2013-01-29 | 2013-05-22 | 华中科技大学 | Method for removing ginkgolic acid and heavy metals in ginkgo biloba extract by using nanometer material |
| CN103110671B (en) * | 2013-01-29 | 2015-06-17 | 华中科技大学 | Method for removing ginkgolic acid and heavy metals in ginkgo biloba extract by using nanometer material |
| CN105380750A (en) * | 2015-10-22 | 2016-03-09 | 俞祖勋 | Making method for anti-bacterial non-woven fabric, anti-bacterial paper diaper and use method |
| CN107873932A (en) * | 2017-11-30 | 2018-04-06 | 胡江宇 | Crisp sugar of gingko and preparation method thereof |
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Application publication date: 20121205 |