CN1451658A - Method for extracting seabuckthorn fruit total flavonoids by three-solvent system - Google Patents

Method for extracting seabuckthorn fruit total flavonoids by three-solvent system Download PDF

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Publication number
CN1451658A
CN1451658A CN 03108045 CN03108045A CN1451658A CN 1451658 A CN1451658 A CN 1451658A CN 03108045 CN03108045 CN 03108045 CN 03108045 A CN03108045 A CN 03108045A CN 1451658 A CN1451658 A CN 1451658A
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fructus hippophae
solvent
water
extraction
flavones
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CN1176083C (en
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傅建熙
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LIAONING DONGNING PHARMACEUTIC
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Abstract

The invention discloses a method for extracting total flavonoids from seabuckthorn fruits (namely hippophae rhamnoides fruits), which comprises the following steps: the method comprises extracting total flavone from fructus Hippophae with three-solvent system as solvent, removing liposoluble substances such as oleum Hippophae by static separation technology, and removing impurities with high polarity by washing with water. The extraction method shortens the extraction time and the production period, and improves the extraction rate and the purity of the total flavonoids in the seabuckthorn fruits. In the whole production process, flammable and explosive organic solvents such as normal hexane or petroleum ether and toxic and harmful organic solvents such as chloroform are eliminated, the production cost is reduced, and the production safety and environmental protection requirements are ensured.

Description

Three solvent systems extract the method for Fructus Hippophae total flavones
One, affiliated technical field
The invention belongs to the extraction and separation technology of Fructus Hippophae total flavones, relate to a kind of Fructus Hippophae total flavone extracting method.
Two, background technology
Fructus Hippophae (being fructus hippophae) total flavones is the Flavonoid substances based on glycosides million that extracts Cong the fruit of Hu Decadent scarabaeidae Hippophne (Hippophae L.) plant.Because the Fructus Hippophae total flavones has multiple biological activity, particularly aspect the treatment diseases of cardiovascular and cerebrovascular systems, as resist myocardial ischemia, aspect such as stenocardia, blood fat reducing and anti-arrhythmia, all has good curative effect, have bigger pharmaceutical use, therefore many investigators have proposed to extract the method for total flavones from Fructus Hippophae.
Up to now, the existing method of extraction Fructus Hippophae total flavones is concluded and is mainly contained following five kinds:
First method is that people such as Wang Chang profit in 1994 write proposition in " Chinese patent medicine ".Its method is as follows: with 75% extraction using alcohol sea-buckthorn dry powder, after extraction concentrates, with the saturated limewater dissolving, remove fruit wet goods lipid-soluble substance with ethyl acetate, use recrystallizing methanol at last, promptly get Fructus Hippophae total flavones, productive rate is 0.94%.
Second method is to propose in 1997 " Sichuan Province's drug standard ".Its method is as follows: get sea-buckthorn 1000g and be ground into meal, oil expression divides heating and refluxing extraction three times with 85% ethanol 9000ml, each 2h filters filtrate recycling ethanol, be condensed into dried cream, oil expression again with ethanol 200ml heating and refluxing extraction, is reclaimed ethanol, be condensed into dried cream, water 100ml washing, drying promptly gets Fructus Hippophae total flavones.
The third method is that the bright people of grade of high brocade in 1997 proposes in " sea-buckthorn " magazine.Its method is as follows: get 1kg seabuckthorn fruit peel slag, with industrial normal hexane degreasing, filter residue extracts 3 times with 70% industrial spirit heat about 70 ℃.Extracting solution is condensed into medicinal extract, adds water and stir, tell macroporous resin column on the water suspension, wash the solubility impurity that anhydrates with water, use 80% industrial spirit wash-out again, shorten elutriant into medicinal extract, vacuum-drying promptly gets Fructus Hippophae total flavones.
The 4th kind of patent of invention " safe extraction technology of general flavone from whole sea-buckthorn fruit " patent No.: the ZL 97 1 08475.0 that method is Cheng Peilin.Its method is as follows: get sea-buchthorn fresh fruit 1000kg, isolate about 400kg of Normal juice and pericarp 200kg through the squeezing machine squeezing, the former obtains the Fructus Hippophae total flavones intermediate through separating press filtration and hybrid extraction at Normal juice.Latter's pericarp obtains the Fructus Hippophae total flavones intermediate through the pre-treatment of vibration letter sorting sieve, separation and hybrid extraction.Then the Fructus Hippophae total flavones intermediate is carried out the degreasing of non-ethers solvent, promptly with adding total flavones intermediate and medical grade chloroform in the dynamic degreasing tank, both part by weight are 1: 2, keep 45 ℃~55 ℃ of temperature, stir degreasing through 1h and obtain the Fructus Hippophae total flavones wet-milling.Add water again and stir, filter in water washing tank, water elution desolvates, and puts into the vacuum drying box oven drying at low temperature, and temperature is 56 ℃~65 ℃.Insulation 3h~4h takes out and obtains Fructus Hippophae flavone dry powder, its total recovery rate 1.4%.
The 5th kind of method is general common method.Promptly elder generation extracts 2h~4h with 95% ethanol of 3~5 times of seabuckthorn fruit powder weight with it, filters.Filter residue repeats to extract 2~3 times by top-operation again.Merging filtrate is condensed into medicinal extract.Then medicinal extract is suspended in the warm water, extracts and isolate Oleum Hippophae impurity such as (comprising vegetable wax, pigment) with 60 ℃~90 ℃ sherwood oils or with other fat-soluble solvent.Filter then, separate water outlet, precipitation is dry, promptly gets Fructus Hippophae (being fructus hippophae) total flavones.
Mainly there is the shortcoming of following three aspects in above-mentioned method of the prior art:
(1) because the flavones in the Fructus Hippophae (being fructus hippophae) mainly exists with glucoside n-ary form ns such as Isorhamnetol, Quercetin, kaempferols, their solubleness in intensive polar solvents such as methyl alcohol, second alcohol and water is all very little.Above-mentioned first method is done solvent extraction with 75% ethanol, second method is done solvent extraction with 85% ethanol, the third method is done solvent extraction with 70% ethanol all very big shortcoming, because the Fructus Hippophae glycosides million is 70%, solubleness is all very little in 75% and 85% the ethanol, with 70% (or 75% of three times of material quantities, or 85%) extraction using alcohol is 3 times, flavones is basic to be extracted endless, product yield is very low, for example, the flavones productive rate only has 0.94% in first method, solvent recuperation in the extracting solution is difficulty also, all is worthless so make solvent with the ethanol of these concentration.Also adopt the saturated limewater dissolving in the first method, remove fruit wet goods lipid-soluble substance, use recrystallizing methanol at last with ethyl acetate, not only production process is many, be not suitable for industrial production, and Fructus Hippophae glycosides million solubleness in saturated limewater is also very little, is difficult for extracting.In addition, the oil length of Fructus Hippophae has only about 8%, so the oil in the Fructus Hippophae is impossible squeeze out with the method for oil expression, so the technology that second method proposed is actually and can not realizes.The third method will go up macroporous resin column, and production cost height, operation are loaded down with trivial details, are not suitable for industrialized mass production.The 4th kind of method only said " hybrid extraction ", do not indicate solvent for use, is difficult to estimate the quality of extracting method, but from the result as can be seen, the recovery rate of Fructus Hippophae total flavones is 1.4% of a sea-buchthorn fresh fruit, is impossible.Moreover with the chloroform grease removal no matter on safety, in the environmental protection, or from operating procedure, all have very big defective.The 5th kind of method adopts 95% ethanol to make solvent, and be all better than preceding four kinds of methods, but also have following shortcoming: a. ethanol consumption is big, and is uneconomical; B. extraction time is many, and the production cycle is long; C. the concentrated extracting solution workload is big, and it is many to expend solvent.
(2) make separated from solvent sea-buckthorn wet goods lipid-soluble substance have following shortcoming a: a. they are volatile, easily catch fire with normal hexane or sherwood oil, dangerous; B. the concentration of normal hexane or sherwood oil can be blasted when 1~6% (by volume calculating) in the air; C. they are very little even insoluble to the big organic compound solubleness of polarity, so the flavones purity that obtains is not high.
(3) in the 4th kind of method, substitute sherwood oil separation sea-buckthorn wet goods lipid-soluble substance with chloroform and have following shortcoming: a. chloroform proportion is 1.489, and is more much bigger than the proportion of water.So when Fructus Hippophae medicinal extract was suspended in the water, sea-buckthorn wet goods lipid-soluble substance was on the upper strata, the centre is a water layer, and chloroform is in lower floor.Though add stirring, upper strata sea-buckthorn wet goods lipid-soluble substance also is difficult to fully contact with lower floor's chloroform, so extraction efficiency is not high; B. chloroform has certain solubleness to Fructus Hippophae total flavones; C. chloroform is a narcotic, is not suitable for use in industrial solvent; D. chloroform is easy to be decomposed by oxygen in air, generates the phosgene of severe toxicity, so both do not met the safety in production requirement with the chloroform give industrial solvent, does not also meet environmental requirement.
Three, summary of the invention
At defective that exists in the above-mentioned prior art or deficiency, the invention provides a kind of employing three solvent systems and from Fructus Hippophae, extract the method for Fructus Hippophae total flavones, and Fructus Hippophae total flavones extraction yield and purity thereof all are significantly increased.
The technical scheme that realizes foregoing invention is as follows:
1) adopt three solvent systems, press water: ethyl acetate: ethanol=preparation in 1: 6: 13 substitutes in the prior art with 95% ethanol or other single solvent; 2) extracting solution is concentrated to degree Beaume 30Be °~35Be ° after, adopt static partition method to remove sea-buckthorn wet goods lipid-soluble substance, substitute in the prior art with inflammable, explosive organic solvent such as normal hexane or sherwood oil or with poisonous, deleterious organic solvents such as chloroforms; 3) adopt repeatedly washing, till PH=7, remove tart, water miscible and impurity that polarity is bigger; 4) the wet flavones that will extract is pulverized 60 ℃ of vacuum-dryings, promptly gets Fructus Hippophae total flavones powder.
Fructus Hippophae total flavone extracting method of the present invention, technology is simple, easy to operate, extracting total flavones from Fructus Hippophae (being fructus hippophae) only need extract twice, the extraction yield of Fructus Hippophae total flavones can reach more than 99%, not only improved extraction yield, and reduced the consumption and the extraction time of solvent, and having shortened extraction time and production cycle, the purity of Fructus Hippophae total flavones can reach more than 80%.
Four, embodiment
The present invention is described in further detail below in conjunction with specific embodiment that the contriver provides.
Embodiment:
Take by weighing 100kg Fructus Hippophae dry powder, (water: ethyl acetate: 300kg ethanol=1: 6: 13), at 50 ℃~60 ℃ stirring extraction 1h, cooling is filtered to add three solvent system solvents.Filter residue repeats to extract 1 time by top-operation again.Merging filtrate is concentrated to degree Beaume 30Be °~35Be °, the static sea-buckthorn wet goods lipid-soluble substance phase of isolating with filtrate.Wash the flavones phase then with water, till PH=7, to remove tart, water miscible and impurity that polarity is bigger.Filter.To be deposited in 60 ℃ of vacuum-dryings, pulverize, promptly get Fructus Hippophae (being fructus hippophae) total flavones powder.
The present invention is compared with existing technology, and has following advantage:
1. adopt three dicyandiamide solutions to make solvent and only need extract twice from fructus hippophae (being fructus hippophae) extraction general flavone, Each 1h, the recovery rate of total seabuckthorn flavone can reach more than 99%, has not only improved recovery rate, and reduces Consumption and the extraction time of solvent, shortened extraction time and production cycle.
2. calculate with 100kg fructus hippophae dry powder, do solvent extraction twice with three dicyandiamide solutions, need solvent 600kg (putting aside recovery); If do solvent extraction three times with 95% ethanol, need ethanol 1500kg (temporarily Do not consider to reclaim). The former has saved production cost.
3. under same appointed condition, make solvent extraction fructus hippophae flavones with three dicyandiamide solutions, 4 workmans, Production cycle is 6h; Do solvent extraction with ethanol, 4 workmans, production cycles are at least 10h.
4. compared with prior art, except sea-buckthorn wet goods liposoluble substance, reduced production with static isolation technics Operation has been avoided with an organic solvent having reduced production cost. Producing 1kg fructus hippophae flavones can save at least Take more than 500 yuan the cost-saving.
5. help safety in production without inflammable, explosive organic solvents such as normal hexane or sherwood oils; Without chloroform etc. poisonous, the deleterious organic solvent of health is helped safety in production and environmental requirement.
6. can reduce the input of equipment (as storage tank, grease removal jar etc.).
7. the purity of Fructus Hippophae total flavones can reach more than 80% and (calculate with Isorhamnetol).
8. technology of the present invention is simple, easy to operate.

Claims (1)

1. three solvent systems extract the method for Fructus Hippophae total flavones, may further comprise the steps:
1) water intaking, ethyl acetate, ethanol three solvents, and by water: ethyl acetate: ethanol=1: 6: 13 is mixed and made into the extraction solvent;
2) take by weighing Fructus Hippophae dry powder, add the said extracted solvent, extract at 50 ℃~60 ℃, time 1h, after the filtration, filter residue extracts once again;
3) merge extracted twice filtrate, and degree Beaume 30Be °~35Be °, the static sea-buckthorn wet goods lipid-soluble substance phase of isolating are cooled off, filtered, are concentrated to filtrate;
4) repeatedly wash the flavones phase with water, till PH=7, remove tart, water miscible and impurity that polarity is bigger;
5) the wet flavones that will extract is pulverized 60 ℃ of vacuum-dryings, promptly gets Fructus Hippophae total flavones powder.
CNB031080456A 2003-05-20 2003-05-20 Method for extracting seabuckthorn fruit total flavonoids by three-solvent system Expired - Lifetime CN1176083C (en)

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN100451028C (en) * 2005-08-18 2009-01-14 学校法人日本大学 Antiinflammation compound
CN102533431A (en) * 2011-10-08 2012-07-04 上海友信生物科技有限公司 Method for continuously extracting and separating sea buckthorn oil and isorhamnetin from sea buckthorn pulps
CN104490956A (en) * 2014-12-25 2015-04-08 上海交通大学 Technology for purifying total flavones of hippophae

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN100451028C (en) * 2005-08-18 2009-01-14 学校法人日本大学 Antiinflammation compound
CN102533431A (en) * 2011-10-08 2012-07-04 上海友信生物科技有限公司 Method for continuously extracting and separating sea buckthorn oil and isorhamnetin from sea buckthorn pulps
CN104490956A (en) * 2014-12-25 2015-04-08 上海交通大学 Technology for purifying total flavones of hippophae
CN104490956B (en) * 2014-12-25 2017-12-29 上海交通大学 A kind of total seabuckthorn flavone purifying technique

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