KR101687447B1 - Method for isolating and removing chlorophyll from natural material - Google Patents

Abstract

The present invention relates to a method for extracting and removing chlorophyll from a natural extract without any change in the structure or content of a useful component and separating and removing the chlorophyll according to the method of the present invention. And can improve the efficacy and efficacy of the active ingredient. Thus, it can be used for the raw material industry of natural cosmetics, the beverage industry utilizing natural products, the bio-energy industry, and the like.

Description

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for separating chlorophyll from a natural product,

The present invention relates to a method for separating chlorophyll from natural products and a method for producing natural extract from which chlorophyll has been removed from natural products.

Natural plants contain large amounts of chlorophyll. This chlorophyll is an organ in the leaves of a green plant and produces energy through photosynthesis. When isolating the active ingredient of a plant with a solvent (for example, a spirit), a large amount of chlorophyll is contained and extracted together.

These chloroplasts reduce the efficacy of the active ingredients present in natural products, and are also responsible for skin pigmentation and skin troubles. In addition, when natural materials are added to foods or cosmetics, there is a limit in that they can not be added in large amounts due to the color of the natural product itself. The method of extracting the active ingredient of natural product with hot water is not affected by the effect of the ingredient extracted by ethanol because the main physiologically active ingredient is destroyed by heat. Therefore, chlorophyll removal technology is needed to extract chlorophyll from natural extracts with ethanol as a solvent by physical method without any change of core raw materials.

Various methods have been studied for removing pigment components from natural extracts. Korean Patent No. 10-1256222 discloses a method for removing a pigment of a red beet extract using radiation, and a method for removing a pigment of a red beet extract by irradiating the red beet extract with radiation, without complicated pigment preparation, is disclosed However, because of the use of radiation, a large amount of energy is consumed, the use thereof is limited, and there is a limit that the chemical structure and the content of the useful ingredient in the extract can be changed.

Korean Patent No. 10-1288303 discloses a method for producing a ginseng liquid containing ginsenoside from which a coloring matter and a fragrance component are removed. However, the method includes a step of using diatomaceous earth as a filtration method, Other active ingredients are also removed.

Accordingly, the present inventors have developed a manufacturing technique capable of removing chlorophyll, a pigment of a natural extract, without changing the active ingredient.

It is an object of the present invention to provide a method for producing a natural extract from which chlorophyll has been removed from a natural product without changing the structure and content of a useful component in the natural product using physical methods.

It is another object of the present invention to provide a natural extract from which chlorophyll has been removed from natural products produced by the above method.

It is still another object of the present invention to provide a cosmetic raw material, a food raw material, a health functional food raw material, a pharmaceutical raw material, etc., from which chlorophyll has been removed from natural products produced by the above method.

In order to achieve the above object, the present invention provides a method for producing a natural extract from which a chlorophyll has been removed from a natural product without changing the structure and content of a useful component contained in the natural product, using a physical method.

More particularly, the present invention provides a natural extract from which chlorophyll has been removed from a natural product produced by the above method.

The present invention also provides a cosmetic raw material, a food raw material, a health functional food raw material, a pharmaceutical raw material and a quasi-raw material, from which the chlorophyll has been removed from the natural product produced by the above method.

The chlorophyll-free natural product produced by the method according to the present invention can save a lot of time and cost because it does not undergo a complicated treatment process, and when a natural substance is added to foods or cosmetics, It is possible to overcome the limit that can not be added in a large amount.

The chlorophyll-free natural product produced by the present invention can be usefully used in the raw material industry of natural cosmetics, the beverage industry utilizing natural products, and the bio-energy industry.

In addition, it is possible to reduce a cost wasted in manufacturing a cosmetic container and to prevent contamination,

The chlorophyll-free natural product prepared according to the present invention can have a variety of concentration choices and minimizes the structural destruction and the content change of the useful component in the chlorophyll removal process, thereby improving the efficacy of various useful components .

FIG. 1 is a diagram illustrating a process of removing chlorophyll from a concentrated natural extract.
Figure 2 is an illustration of an example of a process for removing chlorophyll from a concentrated natural extract.
FIG. 3 is a diagram illustrating a process of removing chlorophyll from a lyophilized natural extract.
Figure 4 is an illustration of an example of the process of removing chlorophyll from a lyophilized natural extract.
Fig. 5 is a photograph showing natural products extracted without removing chlorophyll.
A: Camellia sinensis leaf extract
B: Freeze-dried extract of camellia leaves
C: Hojangun freeze-dried extract
6 is a photograph showing the cosmetic raw materials produced by other companies and the cosmetic raw materials produced by the present inventors.
A: Cosmetic raw materials produced by treating activated carbon, activated clay and diatomaceous earth filters in cosmetic raw materials (biorand)
B: Camellia sinensis leaf extract without chlorophyll removed by treatment with 10 mg / mℓ
FIG. 7 is a photograph showing the chlorophyll-free extract prepared through the concentrated natural extract extraction process. FIG.
A: Chlorophyll removed from lyophilized Camellia sinensis leaf extract (Control group: 12 ㎎ / ㎖, w / v)
B: High concentration of Camellia sinensis leaf extract (0.2 ml / ml v / v)
C: Camellia sinensis leaf extract (0.16 ml / ml, v / v) from which chlorophyll was removed,
D: Camellia crassifolia leaf extract (0.1 ml / ml, v / v)
E: Camellia sinensis leaf extract (0.06 ml / ml, v / v) from which chlorophyll was removed,
F: Camellia sinensis leaf extract with clear chlorophyll removed (0.04 ml / ml, v / v)
G: Camellia crassifolia leaf extract (0.02 ml / ml, v / v)
H: Camellia crassifolia leaf extract (0.015 ml / ml, v / v) from which chlorophyll was removed,
I: Camellia crassifolia leaf extract (0.01 ml / ml, v / v) from which chlorophyll was removed,
J: Camellia sinensis leaf extract (0.005 ml / ml, v / v) from which chlorophyll was removed,
FIG. 8 is a photograph showing the extract prepared from chlorophyll prepared through the lyophilized natural extract extraction process.
A: Camellia sinensis leaf extract with no chlorophyll separated at (10 ㎎ / ㎖, w / v)
B: Camphor leaf extract with chlorophyll removed at a concentration of 5 ㎎ / ㎖ (w / v)
C: High concentration of roots root extract with chlorophyll removed at a concentration of 5 ㎎ / ㎖ (w / v)
D: Extract of chlorophyll from 5 mg / ml (w / v)
E: Chlorophyll-free extract from 10 mg / ml (w / v)
F: Camphor leaf extract with chlorophyll removed at a concentration of 10 mg / ml (w / v)
9 is a photograph showing the process of removing chlorophyll from a concentrated natural extract (green tea).
A: green tea extract immersed in a mixed alcohol and feral water
B: Green tea extract with chlorophyll completely separated
C: Chlorophyll was removed using a filter paper, and then concentrated green tea extract

The present invention relates to a method for separating chlorophyll from a natural product and a method for producing a chlorophyll-free natural extract.

Hereinafter, the present invention will be described in detail.

The present invention relates to a process for producing a natural product, comprising the steps of: a) crushing the natural product to obtain a crushed natural product; b) immersing the obtained natural material crumbs in a mixed solvent of alcohol and feral water and heating or setting them at room temperature; c) filtering and concentrating the solution obtained in step b); d) adding alcohol and a mixed solvent of a mixture of a foaming water and a solvent to the concentrate obtained in the step c) and stirring the mixture; e) centrifuging the solution obtained in step d) to remove the lower layer solution containing chlorophyll; f) adding an alcohol and a mixed solvent of a mixture of a water and a water to the supernatant obtained in the step e), concentrating and centrifuging to remove the supernatant containing the residual solvent; g) obtaining a lower layer from which the chlorophyll obtained in step f) has been removed, wherein the alcohol and furoral water mixed solvent used in steps b), d), f) : 0.4 to 100, by weight, based on the total weight of the extract.

In one embodiment of the present invention, floral water refers to a water-soluble substance obtained by distillation extraction of essential oil with high-temperature steam, and in the present invention refers to a plant extract extracted using an essential oil extractor. Furoal water is a byproduct produced during the process of making essential oil (essential oil), which is a water-soluble substance containing aromatic substances to some extent without containing lipophilic substances. In recent years, furoral water itself is also used as a raw material for lotion or toner.

In an embodiment according to the invention, the alcohol used in steps b), d), f) is ethanol and the furoral water may be a water extract of the plant.

In an embodiment of the present invention, instead of purified water, furoral water is used, and if purified water is used, there is a high possibility that the chlorophyll is not properly separated.

In an embodiment according to the present invention, the plant used to make said fuller's water may be, but is not limited to, a plant selected from the group consisting of large leaves, bud leaf and camellia leaves.

In an embodiment according to the present invention, when heating in step b), the temperature may be from 40 to 55 캜, in particular from 45 to 52 캜, and more particularly about 50 캜.

In one embodiment according to the invention, in step c), it may be filtered with a filter of less than 0.5 μm, and in particular may be filtered with a filter of less than 0.45 μm.

In one embodiment according to the present invention, in step e), centrifugation can be performed at 3,000 to 4,000 rpm for at least 5 minutes, specifically at 3,500 rpm for 15 minutes.

In one embodiment according to the invention, in the step f), the concentrate can be concentrated using a reduced pressure evaporator.

In one embodiment according to the invention, the concentrate is centrifuged in step f) and separated into an upper layer and a lower layer which have not been removed during the concentration process. At this time, most of the active ingredient is present in the lower layer.

In one embodiment according to the invention, in step f) it is possible to centrifuge at 3,000 to 4,000 rpm for at least 5 minutes, in particular at 3,500 rpm for 35 minutes.

In one embodiment according to the present invention, after step g), drying step; Adding a mixed solvent of alcohol and feral water, stirring, and centrifuging to remove the supernatant.

More specifically, the chlorophyll-free lower layer obtained in step g) is lyophilized, and then mixed with an alcohol and a mixed solvent of a furoral water, wherein the alcohol and the mixed solvent of the furoral water are alcohol and furoral water in a weight ratio of 1: 0.4 to 100 Is added and dissolved by stirring at 50 to 55 ° C for 30 minutes to 3 hours so that the active ingredient can be separated. After centrifugation at 3,000 ~ 4,000 rpm for 5 minutes or more, specifically at 3,500 rpm for 15 minutes, the supernatant is separated into supernatant and supernatant, and supernatant is removed. Thereafter, the lower layer liquid is washed with furoral water and centrifuged for 2 minutes or more, specifically 5 minutes. The supernatant is then removed. Thereafter, the remaining solvent may be removed by using a vacuum pump or the like. When the above process is further carried out, a liquid raw material in which chlorophyll has been completely removed can be obtained.

In one embodiment of the present invention, the natural extract from which chlorophyll has been removed can be obtained by using purified water. More specifically, the extract extracted from purified water is immersed in a mixed solvent of alcohol and feral water at 21 ° C to 50 ° C for 12 hours to 24 hours to decompose the extract and then concentrated using a vacuum concentrator for 2 to 3 times do. Thereafter, the concentrate is removed with a filter paper to remove chlorophyll, and the extract is concentrated using a vacuum concentrator to obtain a chlorophyll-free raw material.

In one embodiment of the present invention, the natural extract from which chlorophyll has been removed can be prepared by the above method.

In an embodiment of the present invention, a cosmetic composition containing a natural extract from which chlorophyll has been removed may be prepared by the above method.

In one embodiment of the present invention, a composition for quasi-drug containing the natural extract from which chlorophyll has been removed may be prepared by the above method.

In one embodiment of the present invention, a pharmaceutical composition containing the natural extract from which chlorophyll has been removed can be prepared by the above method.

In one embodiment of the present invention, when the concentration of the extracting raw material of the cosmetic composition is 5%, the diluting concentration of the concentrated raw material may be 0.01 to 0.1 ml / ml.

Hereinafter, the present invention will be described in more detail through Production Examples and Examples. However, these preparation examples and examples are presented for illustrating the present invention, and the scope of the present invention is not limited by the following embodiments.

Production Example 1. Preparation of Dilute Solution from Natural Products

Leaf, broadleaf and camellia leaves with high activity were selected as natural materials.

In order to produce floral water extracted from the mung bean sprout leaves, the leaves of mung bean sprout (20 kg), which is grown in large quantities at Suwol - gil 32, Gogdal - myeon,

Large leaves (20 kg) were harvested from Hwasun Daesan Farm (Deokgok-myeon, Hwasun-gun, Jeonnam, Korea) to produce larval leaf feral water.

Camellia leaves were selected for the most active season, and camellia leaves (20 kg) were obtained from the camellia community at 176-12 Mansei, Doam-myeon, Gangjin-gun.

Each of the Furoraru water is supplied with the essential oil extractor of Chosun University, which is a research institute of the neighboring research institute, 20 kg, 20 kg, 20 kg, and 20 kg, . Extracted furoral water is extracted from gall bladder leaves or large leaves or camellia leaves and shows strong activity.

≪ Production method of concentrated raw material from which chlorophyll is removed from natural extract >

The camellia leaves which have been pulverized for ethanol extraction are immersed in a 10-fold 30-70% high-grade alcohol (70-30% of gall bladder leaves or large leaves or camphor leaf feral water instead of purified water) and heated at 50 ° C for 4-12 hours After filtration through a Whatman filter to pass particles of 100 μm or less through the primary filtration. The filtrate is passed through a 0.45 μm filter. After 70% concentration with a vacuum evaporator, 70% high-grade alcohol (30-70% alcohol and 50-50% of foliar or camellia leaf furoral water) was added and stirred for 30 minutes to 3 hours Centrifuge at 3,500 rpm for 15 minutes at room temperature to remove precipitated sublayer. A supernatant from which the black layer is removed can be obtained. To the supernatant, a high-grade alcohol (30-70% alcohol and 35-70% of a leaf or a leaf or camellia leaf) is added to the supernatant, and the mixture is concentrated using a vacuum evaporator and centrifuged to separate the supernatant and the supernatant . The supernatant is completely removed by centrifugation, and the supernatant can be diluted to a portion where most of the concentrated active ingredient is present.

≪ Method for freeze-drying concentrated raw material from which chlorophyll has been removed >

The extract is prepared by removing chlorophyll from the concentrated natural extract, followed by lyophilization. The camellia leaves were pulverized for ethanol extraction and were immersed in 10% 70% high-grade alcohol (70-30% of gall bladder leaves or large leaves or camellia leaf furoral water instead of purified water), heated at 50 ° C for 4 to 12 hours, Filter through a Whatman filter to pass particles below 100 μm. The filtrate is passed through a 0.45 μm filter. After 30-70% of high-grade alcohol (30-70% of alcohol and 70-30% of foliar or broad-leaved leaf or camellia leaf furoral water) was added, the mixture was concentrated for about 30 minutes to 3 hours And then centrifuged at 3,500 rpm for 15 minutes at room temperature to remove the precipitated sublayer. The lower layer of black color is removed by chlorophyll and the chlorophyll-free supernatant is obtained. To the supernatant, a high-grade alcohol (30-70% alcohol and 35-70% of a leaf or a leaf or camellia leaf) is added to the supernatant, and the mixture is concentrated using a vacuum evaporator and centrifuged to separate the supernatant and the supernatant . The supernatant is completely removed by centrifugation with the remaining solvent, and the supernatant is dried through a freeze dryer in which the concentrated active ingredient is mostly present.

≪ Production method from freeze-dried raw material from which chlorophyll has been removed to liquid raw material >

Camellia sinensis leaf extract (5 mg / ml) and powdered callus root extract (5 mg / ml) were added to a liquid solution containing 30-70% alcohol and 70-30% furoral water at 50 ° C for 30 minutes to 3 Time Chlorophyll and active ingredient are mixed separately after dissolving. After confirming that the chlorophyll has been separated, centrifuge at 3,500 rpm for 15 minutes at room temperature. The supernatant is removed and the precipitate is mixed with 30-70% alcohol containing furoral water and centrifuged at 3,500 rpm for 5 minutes. The supernatant is again removed and the vial is completely removed from the harvest with a vacuum pump. To prepare the liquid raw material, a liquid raw material is prepared by mixing, in place of purified water, crops, furoral water of a highly active cucumber leaf, camellia leaf furor water or large leaf furor water.

Example 1.1. Removal of chlorophyll from natural extracts

The camellia leaves which had been pulverized for ethanol extraction were immersed in 10 times 70% high-grade alcohol (a solvent formulated with 70:30 of high-grade alcohol and mushroom fullerate), heated at 50 ° C for 6 hours, (Whatman filter). The filtrate was passed through a 0.45 μm filter. The mixture was concentrated to about 70% with a vacuum evaporator, and further, a 70% high-grade alcohol (a solvent mixed with 70:30 of high-grade alcoholic beverages and mushroom furocal water) was added and stirred for about 1 hour. And centrifuged at 3,500 rpm for 15 minutes at room temperature. Remove the lower layer with chlorophyll. To the supernatant was added a 70% high-grade alcohol (a mixture of high-grade alcohol and fructose-containing furoral water in a ratio of 70:30), and then concentrated under reduced pressure in an evaporator. The concentrate was then centrifuged and separated into supernatant and sub- Can be diluted to a portion where most of the concentrated active ingredient is present, and the lower layer having chlorophyll removed can be obtained.

Example 1.2. Removal of chlorophyll from natural extracts

Except that 30% high-grade alcohol (solvent blended with high-grade alcoholic beverages and municipal furrow water 30:70) was used in place of the 70% high-grade alcohol (solvent in which 70% of high-grade alcohol and myrrh Was performed under the same conditions as in Example 1.1. Thus, a chlorophyll-free supernatant was obtained.

Example 1.3. Removal of chlorophyll from natural extracts

Except that 70% high grade alcohol (solvent blended with high grade alcohol and 70.0% fresh water) instead of 70% high grade alcohol (solvent blended with high-grade alcoholic beverages and municipal furrow water 70:30) was used as the immersion solvent The same procedure as in Example 1.1. Was carried out to obtain a lower layer having chlorophyll removed.

Example 1.4. Removal of chlorophyll from natural extracts

Except that 30% high grade alcohol (a solvent formulated with high-grade alcohol and 30:70 of fresh water) was used as the immersion solvent in place of the 70% high-grade alcohol (the solvent in which the high-grade alcoholic beverages and municipal waste water were mixed at 70:30) The same procedure as in Example 1.1. Was carried out to obtain a lower layer having chlorophyll removed.

Example 1.5. Removal of chlorophyll from natural extracts

Except that 70% high-grade alcohol (a solvent formulated with 70:30 high-grade alcohol and camellia leaf furoral water) was used as the immersion solvent in place of the 70% high-grade alcohol (the solvent in which the high-grade alcoholic beverages and the municipal furrow water were mixed at 70:30) And under the same conditions as in Example 1.1., A chlorophyll-undersubstrate was obtained.

Example 1.6. Removal of chlorophyll from natural extracts

Except that 30% high-grade alcohol (a solvent formulated with 30:70 of high-grade alcohol and camphor leaf feral water) was used as the immersion solvent in place of the 70% high-grade alcohol (a solvent in which 70% And under the same conditions as in Example 1.1., A chlorophyll-undersubstrate was obtained.

Example 2 Freeze-drying a concentrated raw material from which a chlorophyll was removed from a natural extract

Lyophilization was carried out after the preparation by the method of Example 1.1. The camellia leaves which had been pulverized for ethanol extraction were immersed in 10 times 70% high-grade alcohol (a solvent formulated with 70:30 of high-grade alcohol and mushroom fullerate), heated at 50 ° C for 6 hours, (Whatman filter). The filtrate was passed through a 0.45 μm filter. The mixture was concentrated to about 70% with a vacuum evaporator, and then 70% of the high-grade alcohol (a solvent mixed with high-grade alcohol and high-boiling water and 70-50% of folyline fullerate) was stirred for about 1 hour and then the precipitated sub- And centrifuged at 3,500 rpm for 15 minutes at room temperature. The lower layer was removed with chlorophyll. The supernatant was separated into the supernatant and the supernatant by centrifugation of the supernatant, followed by concentrating the supernatant with a solvent containing 70:30 of high-grade alcohol and fructose, It can be diluted to the most existing part, and it is possible to obtain the lower layer liquid in which the upper layer liquid is completely removed and the chlorophyll is removed. The lower layer was dried through a freeze dryer with a liquid raw material in which most of the concentrated active ingredients were present.

Example 3 Preparation of a Chlorophyll-Freeze-Dried Raw Material as a Liquid Raw Material

Camellia sinensis leaf extract (5 mg / ml) and powdered carrageenan extract (5 mg / ml) were placed in a 70% high-grade alcohol (solvent formulated with 70:30 high-grade alcohol and mushroom furocal water) , And the chlorophyll and the active ingredient were separately stirred and dissolved for 1 hour. After confirming that chlorophyll was isolated, it was centrifuged at 3,500 rpm for 15 minutes at room temperature. The lower layer was removed with chlorophyll. The supernatant was separated into the supernatant and the supernatant by centrifugation of the supernatant, followed by concentrating the supernatant with a solvent containing 70:30 of high-grade alcohol and fructose, It can be diluted to the most existing part, and the supernatant is completely removed and the chlorophyll-free sublayer is harvested. The supernatant was mixed with 70% high grade alcohol (solvent blended with 70:30 high grade alcohol and myrrh) and centrifuged at 3,500 rpm for 5 minutes. The supernatant was again removed and the vial was completely removed from the harvest with a vacuum pump. For the preparation of the liquid raw material, the liquid raw material was prepared by mixing the fertile water with the feral water of the fungus leaf having a strong activity instead of the purified water.

Claims (12)

a) crushing camellia leaves, carrageenan or green tea to obtain a plant lysate;
b) immersing the obtained plant disruption in a mixed solvent of Fowler water and ethanol, which is a water extract extracted from any one group selected from the group consisting of Laeroux leaf, Leaf leaf, and Camellia sinensis leaf, heating or standing at room temperature;
c) filtering and concentrating the solution obtained in step b);
d) adding a mixed solvent of ethanol and a furoral water to the concentrate obtained in the step c) and stirring;
e) centrifuging the solution obtained in step d) at 3,000 to 4,000 rpm for 5 to 15 minutes to remove the lower layer solution containing chlorophyll;
f) concentrating the supernatant obtained in step e) with ethanol and a mixed aqueous solution of furocal water, and centrifuging at 3,000 to 4,000 rpm for 2 to 5 minutes to remove supernatant containing residual solvent;
g) obtaining a lower layer from which the chlorophyll obtained in step f) has been removed,
Wherein the ethanol and furoral water mixed solvent used in steps b), d) and f) is a solvent in which ethanol and furoral water are mixed in a weight ratio of 30 to 70: 70 to 30,
A method for producing a camellia leaf extract, a Japanese apricot kernel extract or a green tea extract from which chlorophyll has been removed from a camellia leaf, a Japanese apricot or a green tea.
delete delete The method according to claim 1,
And heating to a temperature of 40 to 55 DEG C when heating in step b).
The method according to claim 1,
Characterized in that in step c) filtration is carried out with a filter below 0.5 μm.
delete delete The method of claim 1, further comprising: after step g), drying; Adding a mixed solvent of alcohol and feral water to the mixture, stirring the mixture, and centrifuging to remove the supernatant.
The chlorophyll-removed camellia leaves, horsetail, or green tea extract prepared by the method of claim 1.
9. A cosmetic composition comprising a chlorophyll-free extract according to claim 9.

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