FI80212B - Storable camomile extracts, rich in active substances, used as cosmetic agents - Google Patents

Description

1 80212 Chamomile extracts, preservatives, rich in active substances, used as cosmetics This application is separated from application 85 3562 by division.

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The present invention relates to preservative-rich chamomile extracts for use as cosmetics.

Liquid chamomile extracts can be obtained in various ways, for example by soaking, percolation, repeat percolation or serial percolation. Common to all methods is the use of chamomile, i.e. dried flower bunches, as a starting material. In addition to the bisabolol content, the content of essential oil, camazulene and flavones is a decisive factor in the quality assessment of chamomile flowers and chamomile extracts.

In the drying process, chamomile flowers lose 75 to 85% of their weight. At the same time, however, the amount of active ingredients is also lost from the flowers, depending on the method of drying. When drying bisabolol-type fresh chamomile under production conditions, it must be assumed that, for example, even at relatively low drying temperatures, 47% of essential oils or 48% of camazulene and 48% of (-) - α-bisabolol are lost, respectively.

25 Additional active ingredient losses occur during storage of chamomile herb. Thus, for example, after one year of storage, the essential oil content of chamomile herb was found to have decreased by 43.8%, with a relatively further decrease in the camazulene content of the essential oil of 68.4%.

In addition, the active ingredients of chamomile are difficult to extract from chamomile herb. Thus, for example, when preparing liquid extracts with 45% alcohol, only about half of the essential oil in the herb goes to 35 extracts.

2 80212

Extraction of fresh chamomile (i.e., freshly picked flower mycelium) has not been performed to date because the newly harvested plants or plant parts undergo numerous enzymatically controlled or microbial-induced processes that result in changes in the substances contained in the plant. Only the removal of water during drying inactivates or correspondingly denatures the enzymes in the plant. Only in Arch. Pharm. 280 (1942), pp. 437-438 describes the case where fresh chamomile-10 millas are extracted with 86% alcohol, however, the extraction is followed by heating at boiling temperature for 20 minutes to destroy the enzymes. However, the azulene yield was only 18.4% at that time, and after five months virtually all of the azulene had disappeared. In the known chamomile extracts, the active ingredients also have only a limited shelf life. In particular, the content of camatsulene decreases rapidly, which cannot be prevented by alkaline additions.

It has now surprisingly been found that the 20 fresh chamomile extractions described have advantages over the known chamomile herb extraction. In particular, it makes it possible to improve the yield of the active ingredient and the shelf life of the active ingredients.

Contrary to expectations, it is not necessary to stabilize the fresh plant extract by heating. Despite the remaining enzyme activity, heating of the fresh chamomile extract must even be avoided to ensure the described benefits.

The chamomile extract according to the invention is characterized in that it is obtained by extracting fresh or frozen chamomile flowers with aqueous C 1 -C 4 alkanols having an alkanol content in the range of 40 to 100%.

Extraction of fresh chamomile flowers is performed with saturated aliphatic alcohols having 1 to 4 carbon atoms. Suitable alcohols are, for example, methanol, ethanol, propan-1-ol, propan-2-ol, in particular ethanol and isopropanol. Pure alcohols (100%) or aqueous mixtures of these alcohols with an alcohol content of between 40 and 100% by weight, in particular from 50 to 90% by weight, preferably from 55 to 85% by weight, can be used. The extraction 5 can be carried out, for example, in a temperature range of 10 to 60 ° C, preferably 10 to 40 ° C.

The alcohol content of the extraction solvent depends on the herbal equivalent of chamomile, i.e. the dry weight of chamomile in the resulting extract. The herbal equivalent of fresh chamomile is the amount by weight of chamomile herb obtained from this fresh chamomile by conventional drying, i.e. as drying is done in the usual way for chamomile herbs, for example by drying thin layers protected from direct sunlight at 40-60 ° C. Such a herb generally still contains up to 10% by weight of water. The dry weight of chamomile, on the other hand, is the weight of a virtually anhydrous herb. For example, if the ratio of fresh chamomile to extraction solvent is high, then the alcohol content of the extraction solvent must be higher. However, one part by weight of the dry weight of the fresh chamomile (determined by drying the sample for three hours at 105 ° C in an oven) must correspond to at least 4 parts by weight, preferably 4 to 8 parts by weight, especially 5 to 6 parts by weight of extract, of the extraction solvent alcohol. -25 must be dimensioned in such a way that the alcohol content of the extract is not less than 20% by weight. In general, the alcohol content of the extract must be from 20 to 50% by weight, preferably from 20 to 40% by weight, in particular from 20 to 35% by weight. 100 g of fresh chamomile usually corresponds to a dry weight of 20 to 30 g. Depending on the alcoholic strength of the extract, the following amounts of alcohol per 100 g of fresh chamomile, depending on the alcoholic strength (for example, 24.6 g dry weight of fresh chamomile, corresponding to a moisture content of 73.6% by weight): 57 g ethanol (96% vol. %) per such batch of 100 g of fresh chamomile-35 gives, for example, an alcohol content of the extract of 4 80212 40% by weight.

The active ingredient yield depends on the alcohol content of the extraction solvent as well as on the herbal extraction. The water (= moisture) bound by its fresh chamomile together with the added alcohol forms an extraction solvent. The addition of alcohol must therefore be chosen taking into account the moisture content of the fresh chamomile so as to obtain the alcoholic strength of the extract which was the target.

Fresh chamomile flowers (fresh chamomile) 10 means chamomile flowers which are extracted within 24 hours of picking or which are frozen during this time. In this case, during these 24 hours, only moderate drying takes place, ie not more than 10% (calculated on the water content of fresh chamomile flowers), which amount 15 depends on the ambient climatic conditions (temperature, humidity).

Usually chamomile flowers are extracted within the first 24 hours after picking. If extraction cannot be performed within this time, chamomile 20 can therefore be frozen until extracted.

Frozen chamomile flowers may also be used in the method described herein if fresh chamomile flowers (as defined above) are used for freezing. For example, fresh chamomile flowers can be frozen as follows: Fresh chamomile is cooled, for example, by cold air at -10 to -50 ° C, especially at -30 to -50 ° C and preferably at -35 to -45 ° C or with liquid gases. as a batch process or continuously and stored in a temperature range of, for example, -10 to -50 ° C. Continuous freezing with liquid gases can be performed with, for example, carbon dioxide, nitrogen or phrygene, preferably liquid nitrogen, in a tunnel cooler. Store at the above temperatures. In the extraction, the frozen chamomile flowers can be used directly or they can be gently thawed in whole or in part (for example, by pouring an extraction solvent having a temperature of 30 to 60 ° C on them).

When fresh chamomile is used in the extraction instead of chamomile herb, the active ingredient yield is improved. Thus, for 5 of the same dry weight and the same herbal equivalent (1 part dry weight = 5 parts extract) and an ethanol content of the extract of about 33%, the following active ingredient yields were obtained based on fresh chamomile (= 100%) content and dry weight: 10 Fresh chamomile extract

Essential oil 54.6% 39.5%

Camatsulene 100.0% 24.1% (-) - α-bisabolol 58.8% 26.7% For this comparison, fresh chamomile was dried under mild conditions. However, these mild conditions are not fully reproducible on a production scale. Therefore, in a comparative experiment carried out using an herb obtained according to a conventional production procedure, the method according to the invention would give an even better active ingredient ratio of 20.

Thus, in addition to the loss of active ingredient in the drying of the chamomile flowers, the extraction of fresh chamomile also has the advantage that the extraction yield, in particular the yield of camazulene and (-) - o-bisabolol, is improved. 25 In addition, the higher active ingredient yield allows the use of chamomile, which contains more green parts of the plant. In this case, it is no longer necessary to screen out the green parts that may come along when picking flowers.

The only advantage of extracting fresh chamomile 30 is that the use of costly dryers becomes unnecessary. The significant energy costs associated with their use are also eliminated. The cost of preparing the extract is thus clearly reduced.

As experiments have shown, extraction of fresh chamomile-35 can also produce chamomile extracts rich in active ingredients with a lower alcohol content (e.g. those with an alcohol content of 25%) than the 45% recommended in the literature. Surprisingly, even fresh chamomile extracts with an alcohol content of 25% did not show any enzymatic conversion of the active ingredients. By reducing the alcohol content to 25%, an extract is obtained in which the total content of extractives (water-soluble and water-insoluble) is about 20% higher than that of the chamomile herb extract with an alcohol content of 45%.

Finally, it has completely unexpectedly been found that the shelf life of the active ingredients in fresh chamomile extracts is considerably better than the shelf life of the active ingredients in chamomile herbal extracts. Thus, for example, extracts made from fresh chamomile with an ethanol content of 26% or 40% showed no reduction in matrixin or camazulene, respectively, after the extracts were stored at room temperature for nine months. This was all the less predictable because the extraction method could be expected to better cause more robust degradation through enzyme activity. It is known from the literature that especially in the form of chamomile, which is present in the chamomile itself and in the chamomile extracts as a precursor as a matrix, rapid decomposition occurs during storage. To date, no method has been known to ensure the permanent stability of matrix in chamomile extracts.

table 1

Active substance content in chamomile extracts after nine months (initial value = 100) 30 Herbal extraction Fresh chamomile extraction

Alcohol content of the extract 40% 40% 25%

Essential oil 86% 91% 86%

Camatsulene 27% 130% 109% 35 (-) - α-bisabolol 98% 102% 83% 7 80212

As shown in Table 1, the azulene content in the chamomile herb extract decreases sharply as expected over a nine-month storage period, while the essential oil and bisabolol content 5 remains relatively stable. In fresh chamomile extracts, the change in essential oil and bisabol content is comparable to herbal extract. The concentration of camatsulene, on the other hand, has remained surprisingly stable, even slightly increasing from baseline.

In the fresh chamomile extraction, the known extraction method can be used. However, since fresh chamomile takes up more space than chamomile herb, it is expedient to use a soaking procedure or a mixed soaking procedure, for example the method described in DE patent 1,093,951.

The method described here is very generally applicable, i.e. it is suitable for use with all the chamomile meals present. The method is particularly suitable for use with the chamomile variety Degumill (DDR-Sorten-20 schutzrecht Degumill; DE patent 2,402,802; IT patent 1,035,096), the chamomile variety Manzana (DE application 3 423 207) and the DE patent application P 3 446 216.3 kamomilloihin.

Thus, for example, the fresh chamomile extracts of Degumill chamomile flowers of the invention of the invention contain at least 19 mg% (-) - bisabolol and less than 9 mg% other bisaboloids (such as bisabolol oxides).

When using chamomile flowers of the variety Manzana or flowers of variety 30 according to DE patent application P 3 446 216.3, the chamomile extracts according to the invention contain, for example, at least 24 mg% of (-) - α-bisabolol and less than 12 mg% of other bisaboloids.

Since fresh chamomile flowers generally still have all or part of their side flowers left, the extracts according to the invention also have a higher flavone content. The extracts according to the invention also have a higher flavone content than the extracts made from hitherto dried flowers. Of course, it is also possible to add fresh kamo-5 Milla side flowers, frozen chamomile side flowers or also dried kamo Milla side flowers in the preparation of the extract according to the invention, by means of which the flavone content can be further increased. Chamomile side flowers have a high content of flavones (such as apigenin and its glycosides).

Example 1 A batch of fresh chamomile equivalent to a batch of 200 g of chamomile herb (758 g, water content 73.6%, essential oil 876 mg%, azulene 57 mg%, bisabolol 151 mg% is extracted with 510 g of ethanol (84% by weight) in a mixing tank stirred at 15 rpm at 65 rpm, after 30 minutes the extract mixture is compressed and the extract is filtered The active ingredient content of the extract is determined in a known manner: azulene 14.7 mg-% essential oil 105.7 mg-% 20 bisabolol 20.4 mg-% apigenin and apigenin glucosides 73 , 1 mg-% (calculated as apigenin) extractants 5.9 mg-% ethanol 39.6% by weight 25 Comparative example (known method) 200 g of chamomile flowers used as described above, but now dried under the protection of direct sunlight in a thin layer below At 40 ° C, essential oil 598 mg%; azulene 22.7 30 mg%; bisabolol 150 mg%; water content 9%) is extracted with 1,050 g of ethanol (40% by weight) in a stirred tank. n at 65 rpm. After 30 minutes, the extraction mixture is compressed and the extract is filtered. The active substance content of the extract is determined in a known manner: 8021 2 9 azulene 4.7 mg-% essential oil 87.0 mg-% bisabolol 12.9 mg-% apigenin and apigenin glucosides 59.9 mg-% 5 (calculated as apigenin) extractants 5.3 mg-% ethanol 37.9% by weight

Example 2 A batch of fresh 10 chamomile (952 g; water content 79%; essential oil 876 mg%; azulene 57 mg%; bisabolol 151 mg%) equivalent to a 200 g batch of chamomile herb is extracted with 540 g of ethanol (80% by weight). ) in a mixing tank at a stirrer speed of 65 rpm. After 30 minutes, the extraction mixture is compressed and the extract is filtered. The active substance content of the extract 15 is determined in a known manner: azulene 8.2 mg-% essential oil 75.5 mg-% bisabolol 9.1 mg-% apigenin and apigenin glucosides 62.2 mg-% 20 (calculated as apigenin) extractants 6.6 mg-% ethanol 26.5% by weight

Comparative example known method) 200 g of chamomile flowers, now dried as described above, dried as in Comparative Example 1; essential oil 598 mg%; azulene 22.7 mg%; bisabolol 150 mg%; water content 9 %) is extracted with 1,050 g of ethanol (25% by weight) in a stirred tank at a speed of 65 rpm. After 30 minutes 30, the extraction mixture is compressed and the extract is filtered. The active substance content of the extract is determined in a known manner: azulene 3.6 mg-% essential oil 66.0 mg-% bisabolol 6.5 mg-% 35 apigenin and apigenin glucosides 48.9 mg-% (calculated as apigenin) extractants 6.3 mg-% ethanol 25.4% by weight 10 8021 2

Example 3 A batch of 300 g of fresh chamomile equivalent to a batch of chamomile herb (1.154 g; water content 74%; essential oil 950 mg%; azulene 92 mg%; bisabolol oxide A 180 5 mg%) is extracted with 1,330 g of propan-2-ol ( 52% by weight) in a mixing tank at a stirrer speed of 65 rpm. After 90 minutes, the extraction mixture is compressed and the extract is filtered. The active substance content of the extract is determined in a known manner: 10 azulene 14.2 mg-% essential oil 101.5 mg-% bisabolol oxide A 26.0 mg-% apigenin and apigenin glucosides 57.0 mg-% (calculated as apigenin) 15 extractants 6.9 mg- % propan-2-ol 26.0% by weight

Comparative Example (known method) 300 g of chamomile flowers used as described above, but now dried (drying as in Comparative Example 1; essential oil 740 mg%; azulene 56 mg%; bisabolol oxide A 168 mg%; water content 9%) extract 2,100 g of 11-propan-2-ol (33% by weight) in a mixing tank at a stirrer speed of 65 rpm. After 90 minutes, the extract mixture is compressed and the extract is filtered.

The active substance content of the extract is determined in a known manner: azulene 6.7 mg-% essential oil 85.2 mg-% bisabolol oxide A 17.4 mg-% apigenin and apigenin glucosides 52.4 mg-% 30 (calculated as apigenin) extractants 6.6 mg- % propan-2-ol 28.5% by weight

Claims (3)

1. Preserved, high-active chamomile extracts for use as cosmetics, characterized in that they are obtained by extracting fresh or frozen chamomile flowers with aqueous -C4 alkanols having an alkanol content in the range of 40 to 100%. Chamomile extracts according to Claim 1, characterized in that they contain at least 18 mg% of (-) - α-bisabolol and less than 9 mg% of other bisaboloids. 3. Preservative, high-active cosmetic chamomile extracts with a higher flavone content, characterized in that they are obtained by extracting fresh or frozen chamomile flowers with aqueous Cx-C4 alkanols with an alkanol content in the range of 40 to 100%, with the addition of fresh , frozen or dried side flowers. 12 8021 2