KR101311743B1 - Green Tea of Tablet Type and the Method for Preparing Thereof - Google Patents

Abstract

The present invention relates to a tablet-type green tea and a method for manufacturing the same, and more particularly, after grinding green tea, while fluidizing the green tea powder in a fluidized bed granulator, 0.01 to 1 times purified water or 0.01 to 1 times purified water and Spray the binder, granulate and dry, form granules 1 to 10 times the size of the original green tea powder, make it flowable for tableting, and then mold to the appropriate size It relates to a tablet-type green tea produced by the same and a method for producing the same. Tablet-type green tea according to the present invention can provide a portable portability and a single intake quantitatively, and makes it possible to consume green tea regardless of preference.

Green Tea * Green Tea Powder * Tablets * Tablets * Granulated Green Tea Powder

Description

Green Tea of Tablet Type and the Method for Preparing Thereof}

Figure 1 is a graph showing the price and catechin content of green tea production time.

Figure 2 is a schematic diagram showing a manufacturing method of green tea tablets.

Figure 3 is a schematic diagram showing the tablet molding capacity of granulated green tea powder.

The present invention relates to a tablet-type green tea and a method for manufacturing the same, and more particularly, after grinding green tea, while fluidizing the green tea powder in a fluidized bed granulator, 0.01 to 1 times purified water or 0.01 to 1 times purified water and Spraying the binder, granulating and drying, forming granules 1 to 10 times the size of the original green tea powder, making it flowable for tableting, and then molding it to a size suitable for one serving It relates to a tablet-type green tea produced by the same and a method for producing the same.

Green tea is produced by activating the oxidase present in the shoots or leaves of Camellia sinensis of Camellia family. Green tea has not only been consumed as a symbol tea since its origin, but its value is now being recognized as the pharmacological mechanism of various ingredients in green tea is gradually revealed, and catechins, amino acids, vitamin C, beta-carotene and It is known to have excellent effects on fatigue, skin care, diabetes, constipation improvement, hangover and nicotine detoxification because it contains a large amount of active ingredients such as dietary fiber.

Recently, the effects of antioxidant, anti-aging, anti-cancer, blood cholesterol lowering, heavy metal detoxification, caries prevention and bad breath removal by the catechins, which are the most contained in green tea, have been attracting much attention. In particular, when drinking green tea in water, drink only the water-soluble ingredients contained in green tea, and discard the rest. In the case of green tea powder, all the ingredients of green tea, such as tocopherol, vitamin A and fiber, are ingested. There is an advantage to this. In addition, green tea powder is not only consumed as tea, but is also added to milk, yogurt, and ice cream, and used in various fields such as baking, bakery, and confectionery. .

Such green tea powder is obtained by grinding green tea with a grinding device. The crusher can be largely classified into a crusher and a grinder. The crusher is a device for crushing a large lump of solid to a size of 6 to 250mm, examples of the device is a jaw crusher and a gyratory crusher. A powder mill is a device that produces a powder of 1 to 500 μm from the first milled powder in a crusher, or prepares fine powder without first milling. A hammer mill, a roller mill, a ball mill ), Attrition mills and air-flow type mills. In the case of producing green tea powder by grinding green tea, the above-mentioned grinding device, in particular, an electric mill, a ball mill, a hammer mill, and the like are used.

Powdered green tea is a common ingestion method to drink in drinking water and is sometimes added to food and ingested. However, green tea in powder form is not easy to drink because it is entangled when it is soaked in water and there is less heat contact during secondary processing to maintain green color. 1 is a graph comparing the production time and catechin content of green tea. In general, green tea powder is rich in taste when drinking it in water, and there is a pottery powder tea (the pottery of FIG. 1) obtained by milling crushed young leaves shaded with shade, but this is very limited in quantity and expensive. Green tea harvested in summer and autumn (abundance of FIG. 1) is abundant in quantity, but it is very difficult to satisfy consumers when compared with the aroma in terms of taste. Summer and autumn green tea is higher in the content of functional ingredients such as catechins by receiving more sunlight than green tea harvested in spring. Therefore, green tea powder, which is crushed green tea harvested in summer and autumn, which is low in price, high in production, and rich in green tea ingredients, is not good for drinking in drinking water. .

However, the powdered green tea produced by the ordinary grinding device does not combine into the desired shape when it is compressed as it is due to the fibrous characteristics of the particles. In addition, there is a problem in productivity, such as difficult to produce a uniform weight or a lot of troubles during production due to poor flowability when put into a tablet press. Most green tea powder is manufactured and sold in powder form, and high-quality raw materials must be used for the color of the green tea powder, and the powder is ground as finely as possible to reduce the gritty feeling when drinking in drinking water. If the green tea powder is prepared in tablet form, this excessive cost can be reduced.

Korean Patent No. 10-0516911 discloses a method for producing green tea rings, which facilitates the production using raw materials other than green tea as a binder to make green tea powder into tablet form. However, the green tea ring is helpful when ingesting other ingredients at the same time, but the amount of green tea intake per serving is reduced, and even if the user does not necessarily need other ingredients, the ingested ingredients are ingested together and are manufactured as a complex preparation. There is a cost. In addition, there is no process to maintain the color of green tea, so color cannot be guaranteed. Sugar, starch, etc. are placed and inherently formed with their own health raw materials, and additional processes such as drying and coating are added. The longer the drying process, the more functional ingredients contained in the green tea are gradually lost. It also does not mention the easy-to-take dose per product.

Korean Patent Registration No. 10-0500438 discloses a method of manufacturing a ring, but in order to make a ring shape, it has to go through many steps of dough-janghwan-seed-jeonghwan-drying, There is no mention. In general, the process of making a ring is formed when the two plates face each other and the contents are rotated at a constant pressure while the rotation is different. In such a process, it is difficult to obtain a product of 1g or less. In addition, when the tea extract is mixed with water, but when excessive moisture is mixed into the tea powder, the oxidation of the functional components of the tea is promoted after the manufacture, and the hot-air drying after all processes causes the appearance color of the product not to turn green. Therefore, it is not considered the visual sensory of the intake.

U.S. Patent Publication No. 2003-0044505 discloses a method of preparing a tablet for tableting in water using tea extract mainly, but it uses a rather expensive extract and can also consume nutritional ingredients as it is. Not the proper way.

Therefore, the inventors of the conventional green tea powder has a bad tableting suitability due to the fine particle size, while many of the functional ingredients, taste, aroma and taste when drinking, deterioration of ease of use, maintaining visual sensory preferences, simple manufacturing method, ingestion We studied the convenient size and capacity and how to easily consume all the ingredients of green tea, and by controlling the particle size of green tea powder to be suitable for processing tablets, and instantaneously granulating the green tea powder with water in a special fluidized bed granulator, The present invention has been accomplished by finding that it is possible to prepare a tableting green tea powder and to secure the flowability that can be compressed.

Accordingly, it is an object of the present invention to provide a tablet-type green tea and a method for preparing the same, which can ingest all the components of green tea and can be ingested regardless of the preference of drinking.

Other objects than the above objects and features of the present invention will become apparent to those skilled in the art from the configuration of the following invention.

In order to achieve the above object, in the present invention, the tablet-type green tea that is not limited to the form and size of the package because it is processed into a tablet (tablet) form by applying a certain pressure after granulation while retaining the ingredients of the green tea as it is and It provides a manufacturing method.

In addition, the tablet-type green tea according to the present invention can ingest all the ingredients of green tea at the time of ingestion, the density is higher than the powder form is easy to carry and can be consumed without drinking in drinking water, the intake is also easy to select and know by the user. When a specific ingredient of green tea is fortified, it is often not acceptable to drink it in drinking water, but when applied to the present invention, a functional ingredient can be appropriately added without such a barrier. In addition, since the spraying and drying are uniform in the fluidizing granulator, it can be manufactured without a large amount of thermal process at a target moisture content that is stable in distribution and is excellent for other products because it can maintain the color of green tea.

A method for producing a tablet-type green tea according to the present invention is shown in FIG. 2 and includes the following processes:

1) first step of obtaining green tea powder by putting green tea leaves in a grinder and crushing them;

2) a second step of obtaining granulated green tea powder by adding purified water to the green tea powder or by adding purified water and a binder;

3) a third step of drying the granulated green tea powder obtained in the second step with dry air to obtain granulated green tea powder; And

4) a fourth step of producing the tablet-type green tea in the tableting machine or capsule machine granulated green tea powder.

In the present invention, the following fifth step may be further included as necessary:

5) A fifth step of coating the tablet surface of the tablet with a sugar solution or film formulation in a coating machine.

The present description will be described in more detail below.

In the first step, the green tea leaves are put in a grinder, pulverized and classified into a diameter of 20 mm to 500 mm to obtain green tea powder. Green tea for use in the present invention is a steamed tea produced by the process of tea leaf leaves harvesting, steaming, crude oil, keeping in mind, heavy oil, essential oil and drying; Green tea produced by the process of harvesting, cutting, keeping in mind and drying; Or a dencha manufactured by heating, cooling, drying, sorting and redrying the tea leaves having increased greenness by shielding general tea leaves; It is preferable to use such as, but is not limited thereto.

In the second step, granulated green tea powder is obtained by spraying green tea powder prepared in the first step by adding 0.01-1 times purified water or 0.01-1 times multiple purified water and a binder to the green tea powder. The binder used in the second step of the present invention is preferably a paste selected from the group consisting of guar gum, xanthan gum, gum arabic, agar, carrageenan, konjac, tara gum, gellan gum and locust bean gum.

The additional or single binder used in the second step is preferably a tea extract selected from the group consisting of green tea extract powder, concentrated green tea extract, extract, catechin and tea polyphenol compound.

In addition, when it is desired to construct a product that requires sweetness, a sugar alcohol selected from the group consisting of xylitol, isomalt, maltitol, sorbitol, erythritol, mannitol, lactitol and manatol as an additional or sole binder in the second process It is preferred to use Sugarless).

In addition, to prepare a product requiring sweetness, maltodextrin, cyclodextrin, sugar, isomerized sugar, glucose, fructose, lactose, xylose, maltose, fructooligosaccharide, malto oligosaccharide, iso Preference is given to using general sugars selected from the group consisting of maltooligosaccharides, galactooligosaccharides, soy oligosaccharides, coupling sugars and paratinoses.

The binder of the second step is preferably 0.1 to 10% of the total weight of the purified water. If the binder content is less than 0.1% by weight relative to the total weight of the purified water, the binding force is insufficient and if it is 10% by weight or more, spraying to the fluidized bed granulator is difficult due to the strong viscosity of the binder solution.

In addition, the binder of the second step is preferably 1.0 to 10.0% by weight based on the total weight of the green tea powder. If the content of the binder is less than 1.0% by weight relative to the total weight of the green tea powder, the binding force is insufficient and if the content is more than 10% by weight, the binding force is excessive and the dispersion of powder particles is difficult and easily precipitated when suspended in water.

In addition, in the second step, a solvent such as ethyl alcohol may be mixed with purified water in addition to purified water. At this time, the ethyl alcohol is preferably 10 to 30% of the total weight of the purified water. If the content of ethyl alcohol is less than 10% by weight based on the total weight of purified water, the mixing effect of ethyl alcohol is weak and more than 30% by weight, it is difficult to spray green tea powder evenly in the liquid phase because of the strong volatility.

On the other hand, in the step of adding purified water or purified water and the binder of the second step may further contain a sweetener. The sweetener further contained is preferably one or more compounds selected from the group of synthetic sweeteners consisting of sucralose, acesulfamekei, cyclamate, steviosides, aspartame, altam, glycyricin and somate.

The sweetener content is preferably 0.001 to 1.0% of the total weight of the purified water. If the content of the sweetener is less than 0.001% by weight, the sweetening effect is insignificant, and if it is more than 1.0% by weight, the sweetness is excessive and the product composition becomes difficult. The sweetener is sprayed by dissolving in purified water or a mixture of purified water and ethyl alcohol as a trace, without mixing into powder.

In the third step, the granulated green tea powder prepared in the second step is dried with dry air of 40 ° C. or less for 30 minutes to 1 hour to obtain granulated green tea powder having a moisture content of 5% or less of the total weight of the granular green tea powder.

In the third step of the present invention, the green tea or other flavor (Flavor) may be sprayed and mixed in the liquid or powder at the end of the drying process. At this time, the fragrance added is preferably 0.1 to 5.0% of the total weight of the granulated green tea powder. If the content of the flavor is less than 0.1% by weight relative to the total weight of the green tea powder is insufficient flavoring and if more than 5% by weight the strength of the flavor is too strong to lose the inherent flavor of green tea.

In the fourth step, the granulated green tea powder prepared in the third step is press-molded in the form of tablets or capsules of 0.1 g to 10 g in a tableting or capsule machine of a single and single shot to produce a tablet-type green tea. If the weight of the granular green tea powder is less than 0.1g, the amount thereof is insufficient for press molding as a single dose, and if it exceeds 10g, it is difficult to consume a large amount as a single dose.

In addition, when the green tea powder is molded and packaged in the form of tablets and capsules, the product can be easily packaged in a small packaging container, can guarantee the content of the active ingredient of green tea, and can reduce changes in distribution.

In the fifth step, the tablet-type green tea prepared in the fourth step is coated in the coating machine with the sugar solution or film formulation. The sugar solution used as the coating agent in the present invention is a sugar alcohol selected from the group consisting of xylitol, isomalt, maltitol, sorbitol, erythritol, mannitol, lactitol and manatol (cavities caries, sugar-free (Sugarless)); And maltodextrin, cyclodextrin, sugar, isosaccharide, glucose, fructose, lactose, xylose, maltose, fructooligosaccharide, maltooligosaccharide, isomaltoligosaccharide, galactooligosaccharide, soy oligosaccharide, coupling sugar and paratinose. It is preferable to use at least one compound selected from the group of common sugars selected from the group. The film preparation used in the present invention includes hydroxypropylmethyl cellulose, methyl cellulose, methylethyl cellulose, carboxymethyl starch, paraffin, beeswax, At least one selected from the group consisting of carnauba wax and shellac may be used.

In the fifth step of the present invention, the tablet-type green tea product is packaged in a rectangular bulk form of 0.1 g to 100 g.

Hereinafter, although an Example and a comparative example demonstrate this invention further in detail, this invention is not limited only to these examples.

Example 1 Preparation of Tablet Type Green Tea

Air current type using a grinder after grinding green tea leaves, including stems average 20kg was passed through a classification particle size (indicated by the D4,3) manufactures 40~50mm the green tea powder, green tea powder, 800g of the prepared Glatt fluid bed granulator's Into a fluidized solution and then sprayed with 0.3 times the weight of purified water. The dry air supplied in this fluidization and spraying step was 25-50% RH, 70 ° C, and the temperature of the fluidized green tea powder was 30-35 ° C. After the spraying was terminated, the same dry air was supplied at 40 ° C., dried to 5% or less of moisture, and separated into 30 meshes to prepare granulated green tea powder. The granulated green tea powder thus prepared was made into tablets of 0.5 g by a tablet press (ERWEKA EKO-single tablet press, Germany). The hardness of the tablets is 1-25 kp.

Example 2 Preparation of Tablet Type Green Tea

20kg of green tea leaves including stems were pulverized using an air flow grinder, and then passed through a classifier to produce green tea powder having a D4,3 of 40 to 50 mm. 0.5 times purified water was sprayed. Guar gum was added as binder at 2% by weight of purified water. The dry air supplied in this fluidization and spraying step is 25-50% RH, 70 ° C, and the temperature of the fluidized green tea powder is 30-35 ° C. After the spraying was terminated, the same dry air was supplied to 40 ° C., dried to 5% or less of moisture, and then separated into 30 mesh to prepare granulated green tea powder. The granulated green tea powder thus prepared was made into tablets of 0.5 g by a tablet press (ERWEKA EKO-single tablet press, Germany). The hardness of the tablets is 1-25 kp.

Example 3 Preparation of Tablet Type Green Tea

20kg of green tea leaves including stems were pulverized using an air flow grinder, and then passed through a classifier to prepare green tea powder having 40 to 50 mm of D4,3, and the obtained green tea powder was put into a fluidized bed granulator and fluidized. 0.5 times purified water was sprayed. As a binder, green tea extract powder was added at 1 to 20% by weight of purified water. The dry air supplied in this fluidization and spraying step is 25-50% RH, 70 ° C, and the temperature of the fluidized green tea powder is 30-35 ° C. After the spraying was terminated, the same dry air was supplied to 40 ° C., dried to 5% or less of moisture, and then separated into 30 mesh to prepare granulated green tea powder. The granulated green tea powder thus prepared was made into tablets of 0.5 g by a tablet press (ERWEKA EKO-single tablet press, Germany). The hardness of the tablets is 1-25 kp.

Example 4 Preparation of Tablet Type Green Tea

20kg of green tea leaves including stems were pulverized using an air flow grinder, and then passed through a classifier to prepare green tea powder having 40 to 50 mm of D4,3, and the obtained green tea powder was put into a fluidized bed granulator and fluidized. 0.5 times purified water was sprayed. Dextrin was added as a binder in 1-20% by weight of purified water. The dry air supplied in this fluidization and spraying step is 25-50% RH, 70 ° C, and the temperature of the fluidized green tea powder is 30-35 ° C. After the spraying was terminated, the same dry air was supplied to 40 ° C., dried to 5% or less of moisture, and then separated into 30 mesh to prepare granulated green tea powder. The granulated green tea powder thus prepared was made into tablets of 0.5 g by a tablet press (ERWEKA EKO-single tablet press, Germany). The hardness of the tablets is 1-25 kp.

Comparative Example 1 Tablet-type Green Tea Manufactured with Green Tea Powder of 500 mm to 1000 mm or Less

20 kg of green tea leaves including stems were pulverized using an air flow grinder, and then passed through a classifier to prepare green tea powder having a 600 to 650 mm D4,3, and dextrin was mixed homogeneously by adding 1 to 10% by weight of the green tea powder. . The green tea mixed powder thus prepared was made into tablets of 0.5 g by a tablet press (ERWEKA EKO-single tablet press, Germany). The hardness of the tablets is 0.1-5 kp.

[Comparative Example 2] Tablet type green tea prepared with 1000mm or more green tea powder

Air current type using a grinder was passed through an after grinding green tea leaves, including stems 20kg classification D4, to thereby prepare a green tea powder 3 1500~1600mm. Dextrin was added 1 to 10% by weight of green tea powder and mixed homogeneously. The green tea mixed powder thus prepared was made into tablets of 0.5 g by a tablet press (ERWEKA EKO-single tablet press, Germany). The hardness of the tablets is 0.1-5 kp.

Test Example 1 Hardness Comparison

Ten tablet-type green teas of Examples 1 to 4 and Comparative Examples 1 to 2 were each prepared at the same sample weight and at the same sample weight, and then hardness thereof was measured by a disintegration tester (Lab Fine). Table 1 shows.

division Hardness (kPa) Example 1 5.1 Example 2 8.8 Example 3 6.4 Example 4 6.9 Comparative Example 1 3.0 Comparative Example 2 1.2

As can be seen from the results of Table 1, the tablet-type green tea prepared in Examples 1 to 4 has a higher hardness than the tablet-type green tea prepared in Comparative Examples 1 and 2, which is suitable for preparing tablets.

Test Example 2 Comparison of Friability

Five tablet-type green teas of Examples 1 to 4 and Comparative Examples 1 and 2 were put into a prabilator, respectively, rotated for 5 minutes, and passed through a width of 100 mm. The ratio was recorded and the results are shown in Table 2 below.

division weight% Example 1 55 Example 2 75 Example 3 60 Example 4 63 Comparative Example 1 25 Comparative Example 2 17

In the results of Table 2, the tablet-type green tea prepared in Examples 1 to 4 has better friability than the tablet-type green tea prepared in Comparative Examples 1 and 2, and thus, during tablet manufacturing and distribution It was found that the damage resistance is more suitable for the manufacture of tablets.

Test Example 3 Flowability (Processability) Comparison

300 g each of the tablet-type green tea prepared in Example 1 and Comparative Example 1 were each manufactured in a continuous state (20 rpm) in a tablet press (ERWEKA EKO-single tablet press, Germany) to measure shape defects of the finished product, and the results are shown in Table 3 below. And FIG. 3 (n = 100).

(n = 100) Shape occurrence frequency compatibility Example 1 8 8% ○ Comparative Example 1 26 26% ×

As shown in the results of Table 3 and Figure 3, the tablet-type green tea prepared in Example 1 was excellent in flowability compared to Comparative Example 1 was suitable for the tablet production equipment, it was found that the defective rate of the product is more suitable.

As described above, in the present invention, by forming granules of purified water or purified water and a binder in a fluidized bed granulator on green tea powder pulverized to 20 mm to 500 mm or less, the flowability and dispersibility are improved by using granulated green tea powder, which is improved compared to general green tea powder. The tablet type green tea which was good in ignition property was able to be manufactured.

Claims (18)

1) first step of obtaining green tea powder by putting green tea leaves in a grinder and crushing them; 2) a second step of obtaining granulated green tea powder by adding purified water to the green tea powder or by adding purified water and a binder; 3) a third step of drying the granulated green tea powder obtained in the second step with dry air to obtain granulated green tea powder; And 4) a fourth step of preparing the tablet-type green tea in the tableting machine or capsule machine granulated green tea powder; Tablet type green tea manufacturing method comprising a. The method of claim 1, 5) a fifth process of coating the tablet surface with a sugar solution or a film preparation in a tablet-type green tea; Method for producing a tablet-type green tea, characterized in that it further comprises. delete The method of claim 1, wherein the purified water of the second step is a tablet-type green tea production method, characterized in that the purified water of 0.01 to 1 times the total weight of the green tea powder. The method of claim 1, wherein the binder of the second process Flavors selected from the group consisting of guar gum, xanthan gum, gum arabic, agar, carrageenan, konjac, tara gum, gellan gum and locust bean gum; Tea extract selected from the group consisting of green tea extract powder, concentrated green tea extract, catechin and tea polyphenol compounds; Sugar alcohols selected from the group consisting of maltodextrin, xylitol, isomalt, maltitol, sorbitol, erythritol, mannitol, lactitol and manatol; And General sugars selected from the group consisting of sugar, isosaccharides, glucose, fructose, lactose, xylose, maltose, fructooligosaccharides, maltooligosaccharides, isomaltooligosaccharides, galactooligosaccharides, soy oligosaccharides, coupling sugars and paratinose; Method for producing a tablet-type green tea, characterized in that at least one compound selected from the group consisting of. The method for producing a tablet-type green tea according to claim 1, wherein a sweetener is added in the second step. The method of claim 6, wherein the sweetener is characterized in that at least one compound selected from the group of synthetic sweeteners consisting of sucralose, acesulfamekei, cyclamate, stevioside, aspartame, alitam, glycyricin, and somartin. Method for producing a tablet-type green tea. 7. The method of claim 6, wherein the sweetener is used at 0.001 to 1.0% of the total weight of the purified water. The method of claim 1, wherein the binder of the second step is used for producing a tablet-type green tea, characterized in that 0.1 to 10% of the total weight of the purified water. The method for producing a tablet-type green tea according to claim 1, further comprising mixing ethyl alcohol with purified water in the second step. The method for producing a tablet-type green tea according to claim 10, wherein the ethyl alcohol is used at 10 to 30% of the total weight of the purified water. The method of claim 1, wherein in the third step, the dry air is a tablet-type green tea manufacturing method, characterized in that the dry air of 40 ℃ or less. The method of claim 1, wherein the drying time in the third step is a tablet-type green tea production method, characterized in that 30 minutes to 1 hour. The method of claim 1, wherein the water content of the granular green tea powder in the third step is 5% or less of the total weight of the granular green tea powder. The tablet-type green tea according to claim 1, wherein in the third step, the green tea flavor (Flavor) is used in the liquid or powder form at 0.1 to 5.0% of the total weight of the granulated green tea powder. Manufacturing method. According to claim 2, wherein the sugar solution used as a coating in the fifth step Sugar alcohols selected from the group consisting of xylitol, isomalt, maltitol, sorbitol, erythritol, mannitol, lactitol and manatol; And Group consisting of maltodextrin, cyclodextrin, sugar, isosaccharide, glucose, fructose, lactose, xylose, maltose, fructooligosaccharide, maltooligosaccharide, isomaltooligosaccharide, galactooligosaccharide, soy oligosaccharide, coupling sugar and paratinose A method for producing a tablet-type green tea, characterized in that at least one compound selected from the group consisting of saccharides selected from. The method of claim 2, wherein the film used as the coating agent in the fifth step is hydroxypropylmethyl cellulose (Hydroxypropylmethyl cellulose), methyl cellulose (Methyl cellulose), methyl ethyl cellulose (methylethyl cellulose), carboxymethyl starch (Carboxymethyl starch), paraffin, beeswax, carnauba wax and shellac method for producing a tablet-type green tea, characterized in that at least one compound selected from the group consisting of. A tablet green tea prepared by the method according to any one of claims 1, 2 and 4 to 17.

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