Five-grain highland barley beer and preparation method thereof

Abstract

The invention belongs to the technical field of beer brewing, and particularly relates to five-grain highland barley beer and a preparation method thereof. In order to overcome the defects that highland barley beer is single in flavor, turbid in wine body and high in wort viscosity, 70-75% of barley malt flour, 7.5-10% of highland barley flour and 17.5-20% of five-grain flour are used as beer raw materials, highland barley and five grains are gelatinized and then mixed with barley malt for protein resting, saccharification and dextrinization, and wort is obtained; and finally, filtering the wort, spraying grains, forming mixed wort by the grain spraying water and the filtered wort, boiling, cooling, adding yeast for fermentation, and preparing the five-grain highland barley beer after the fermentation is completed. Compared with highland barley beer without five grains, the five-grain highland barley beer is more harmonious in flavor and mouth feel and better in soaking holding property and mouth feel, has the malt fragrance and the hops fragrance, also has unique flower and fruit fragrance, is relatively low in fusel oil content, and is not easy to drink when people drink the five-grain highland barley beer.

Description

TECHNICAL FIELD

[0001] The present application belongs to the technical field of beer brewing, and particularly relates to a five-grain highland barley beer and a preparation method thereof. BACKGROUND

[0002] Highland barley is comprehensive and unique in nutritional composition, and has the nutritional and health care characteristics of "three highs and two lows", i.e., high protein, high fiber and high vitamins, and low fat and low sugar, and has extremely high nutritional and health care values. In addition, the mass fraction of β-glucan in highland barley is 7.68%, and the mass fraction of total flavones is 6.38%, both of which are higher than those in hulless barley. A large number of experiments have proved that β-glucan has the effects of clearing the intestines, reducing cholesterol, regulating blood sugar, improving immunity, reducing blood lipid abnormalities and preventing cardiovascular diseases, and also has an extremely important role in anti-cancer. Flavonoids have the effects of reducing blood sugar, reducing blood lipids, reducing blood pressure, resisting tumors, resisting oxidation, eliminating free radicals in the body, enhancing immunity and protecting the cardiovascular system, and have extremely high nutritional and health care values. Therefore, compared with hulless barley, the nutritional value of beer brewed by using highland barley as raw material is more abundant.

[0003] The existing literatures such as patents CN1556182A and CN104673566A all use highland barley to prepare craft beer, although the health care effects of highland barley are introduced, but because a high proportion of highland barley is used, the beer body of highland barley craft beer is turbid, the wort viscosity is large, the wort filtration is not conducive in production, and the aroma of highland barley beer is relatively single.

[0004] Five-grain liquor uses five kinds of grains, i.e., 36% of sorghum, 22% of rice, 18% of waxy rice, 16% of wheat and 8% of corn, as raw materials for liquor brewing, and the ratio is obtained through numerous scientific adjustments, so that the characteristics of each kind of grain are fully played, and are complementary and integrated with each other, so that the unique flavor of five-grain liquor is formed. Sorghum produces wine aroma, rice produces wine purity, waxy rice produces wine softness, wheat produces wine long-lasting and sweet corn produces wine, the flavors of the five kinds of grains are interwoven and integrated with each other, and the five-grain liquor has the unique taste of long-lasting aroma, mellow taste, sweet entrance, pure throat, harmonious taste and just right. The five kinds of grains themselves are rich in various nutritional ingredients such as vitamins, minerals and amino acids. However, there is still little report on the use of five-grain and highland barley as beer raw materials to prepare beer. SUMMARY

[0005] In order to overcome the defects of single flavor, turbid beer body and large wort viscosity of highland barley beer, the five grains of five-grain liquor and highland barley are used as beer raw materials to prepare a five-grain highland barley beer, the flavor and taste of which are coordinated, the foam retention and taste are good, and in addition to malt aroma and hop aroma, the beer also has unique fruit aroma. The content of fusel oil is relatively low, and the beer is less likely to be drunk.

[0006] To achieve the above application purposes, the technical scheme adopted by the present application is as follows: In a first aspect, the present application provides a method for making five-grain highland barley beer, comprising the following steps: (1) highland barley-five-grain gelatinization: after highland barley powder and five-grain powder are uniformly mixed, water and amylase are added, the temperature is raised to the amylase hydrolysis temperature for gelatinization, and a highland barley-five-grain gelatinization mash is obtained; (2) malt saccharification: after malt is crushed, it is soaked in water, and at the end of the soaking, the highland barley-five-grain gelatinization mash in step (1) is added, mixed, and then subjected to protein rest, saccharification, and dextrinization, to obtain wort; (3) boiling, cooling, and fermentation: after the wort is filtered, it is subjected to wort dripping, the wort dripping water and the filtered wort are mixed to form mixed wort, which is boiled, cooled, and then fermented with yeast, and the fermentation is completed; wherein the mass content of malt, highland barley powder, and five-grain powder in the beer raw materials is 70-75%, 7.5-10%, and 17.5-20%, respectively.

[0007] In step (1), the highland barley powder is obtained by crushing highland barley and passing it through a 20-mesh sieve.

[0008] In step (1), the five-grain powder has ≤20% of fine powder that can pass through a 20-mesh sieve.

[0009] In step (1), the five-grain powder is composed of 36% sorghum, 22% rice, 18% glutinous rice, 16% wheat, and 8% corn.

[0010] In step (1), the addition amount of amylase is 0.04% of the total of highland barley powder and five-grain powder.

[0011] In step (1), the water to highland barley and five-grain mixture is (3-4):1 (L / kg).

[0012] In step (1), saccharification is carried out at 90-95°C until the starch iodine test does not change blue.

[0013] In step (2), the crushed malt is soaked in water at 35°C.

[0014] In step (2), the ratio of the amount of soaking water to the amount of malt is (3-4):1 (L / kg).

[0015] In step (2), the protein rest temperature is 50-55°C, and the protein rest time is 50 min.

[0016] In step (2), after protein rest, the saccharification temperature is 60-65°C, and the saccharification time is 70 min.

[0017] In step (2), the dextrinization temperature is 75-80℃, and the dextrinization time is 10 min.

[0018] In step (2), the temperature rising rate from the end of the immersion to the protein rest, saccharification and dextrinization stages is 1℃ / min.

[0019] In step (3), the ratio of the water used for the sparging to the beer raw material is 1.5-2:1 (L / kg).

[0020] In step (3), the sparging water temperature is 78℃.

[0021] In step (3), the boiling intensity is 10%, the boiling time is 1 h, and hops are added during the boiling.

[0022] In step (3), the hops addition amount is 1.0-1.2 g / L of the wort raw material.

[0023] Preferably, the hops are added in the following manner: 60% of the Saaz hops are added when the heat degradation to the wort surface foam disappears, and the remaining 40% of the Saaz hops are added 5 min before the end of the boiling.

[0024] In step (3), after the wort is cooled, the lager dry yeast W34 / 70 is added, and the addition amount is 1.0-1.3 g / L of the cooled wort.

[0025] In step (3), after the yeast is inoculated, the fermentation is carried out at an environment of 13℃, the wort sugar degree is reduced to 3.8-4.2 °P when the canning is sealed, the diacetyl reduction is carried out for 6 days, the reduction temperature is 15℃, the temperature is reduced by 6-7℃ per day, the post-ripening is carried out for 7-14 days when the temperature is reduced to 1℃, and the process is completed.

[0026] In a second aspect, the present application provides the five-grain highland barley beer prepared by the above preparation method.

[0027] Beneficial effects: The present application uses the five-grain powder, highland barley and malt of the five-grain liquor as raw materials, and adopts the lager dry yeast W34 / 70 for fermentation, so that the five-grain highland barley craft beer with coordinated flavor and taste, good head retention and taste, and unique floral and fruity aroma in addition to malt aroma and hop aroma is prepared. Experimental results show that, compared with the conventional highland barley beer, the specific proportion of the five-grain powder is added in the beer raw material of the present application, the five-grain powder, highland barley powder and malt powder are coordinated, the content of esters, terpenoids and aromatic compounds in the prepared five-grain highland barley beer is higher than that of the conventional highland barley beer, so that more floral and fruity aroma and herbal aroma are provided for the liquor body. Moreover, the content of fusel oil in the five-grain highland barley beer of the present application is relatively low, and the head is less likely to be formed when it is drunk. BRIEF DESCRIPTION OF DRAWINGS

[0028] Figure 1 The flavor substance comparison chart of the five-grain highland barley beer prepared in the embodiment of the present application and the conventional highland barley beer; "p1" is the five-grain highland barley beer of the present application, "p2" is the conventional highland barley beer, and the red color represents higher content of flavor substance. DETAILED DESCRIPTION

[0029] In order to make the technical problems, technical solutions and beneficial effects to be solved in the present application more clear and explicit, the present application will be further described in detail below in combination with the embodiments. Unless otherwise defined, all the technical terms used in the present application have the same meanings as understood by those skilled in the art.

[0030] In an embodiment of the present application, a preparation method of five-grain highland barley beer is provided, comprising the following steps: (1) highland barley-five-grain gelatinization: after the highland barley powder and the five-grain powder are uniformly mixed, water and amylase are added, and the temperature is raised to the optimum hydrolysis temperature of the amylase for gelatinization, to obtain highland barley-five-grain gelatinized mash; (2) malt saccharification: after the barley malt is crushed and soaked in water, the highland barley-five-grain gelatinized mash in step (1) is added at the end of the soaking, and then the mixture is uniformly mixed and subjected to the protein rest, saccharification and dextrinization stages, to obtain wort; (3) boiling, cooling and fermentation: after the wort is filtered, it is subjected to wort dripping, and the wort dripping water and the filtered wort are mixed to form mixed wort, which is subjected to boiling, cooling and then yeast fermentation, and the fermentation is completed; wherein the mass content of the barley malt, the highland barley powder and the five-grain powder is 70-75%, 7.5-10% and 17.5-20%, respectively.

[0031] The advantage of controlling the mass content of the barley malt, the highland barley powder and the five-grain powder to be 70-75%, 7.5-10% and 17.5-20%, respectively, in the present application is that the barley malt can ensure sufficient enzyme system and malt aroma, the highland barley in this range can prevent the β-glucan content from being too high to cause filtration difficulty and affect the sugar content of the wort, and the five-grain powder in this range can bring rich fruit aroma to the beer, and a too high range can cause the grain flavor to be too strong.

[0032] In some specific embodiments of the present application, in step (1), the highland barley powder is prepared by crushing the highland barley and passing the crushed highland barley through a 20-mesh sieve.

[0033] In some specific embodiments of the present application, in step (1), the five-grain powder can pass through a 20-mesh sieve with ≤20% of fine powder. Among them, the crushing degree of sorghum, rice, glutinous rice and wheat is 4, 6, 6 and 8 petals, respectively, and no whole grains are mixed in, and the corn is crushed to a size comparable to the first four, and no more than 1 / 4 grain is mixed in.

[0034] The raw materials in the present application are all crushed in order to fully hydrolyze the starch in the raw materials.

[0035] The size of the crushed corn particles should be basically the same as the crushing effect of the previous four kinds of grains, that is, through crushing treatment, form a "petal-like" particle (not fine powder or whole grain), the overall roughness is equivalent to the 4-8 petal state of the previous four kinds of grains such as sorghum, to ensure consistent physical properties (such as water absorption speed, gelatinization degree, etc.), and avoid unbalanced process effect due to particle differences. No more than 1 / 4 grain means: in the crushed corn particles, the "maximum coarse particle" allowed to exist cannot exceed 1 / 4 of the size of the original whole corn kernel; more colloquially, it means that no larger than "1 / 4 grain corn" particles can be mixed in.

[0036] In some embodiments of the present application, in step (1), the five-grain flour is composed of 36% sorghum, 22% rice, 18% glutinous rice, 16% wheat and 8% corn.

[0037] In some embodiments of the present application, in step (1), the amount of amylase added is 0.04% of the total of highland barley powder and five-grain flour. At this ratio, the starch can be rapidly hydrolyzed, and the cost can be saved.

[0038] In some embodiments of the present application, in step (1), the water: highland barley and five-grain mixture = (3-4): 1 (L / kg). At this ratio, the highland barley powder and five-grain flour can be fully hydrated.

[0039] In some embodiments of the present application, in step (1), the temperature is slowly raised to 90°C during the program temperature gelatinization, and stirring is continuously performed during this period, which is to prevent the bottom of the pot from being burnt, and the saccharification is carried out at 90-95°C, which is to reach the optimal hydrolysis temperature range of amylase, until the starch iodine test does not change blue and stops.

[0040] In some embodiments of the present application, in step (2), the crushed malt is soaked in water at 35°C. The barley malt needs to be crushed, which is to reduce the particle size of the raw material, increase the specific surface area, and be beneficial to the action of enzymes, the leaching of soluble substances, and the separation of spent grain and wort.

[0041] In some embodiments of the present application, in step (2), the ratio of water amount to malt amount is (3-4): 1 (L / kg). This amount of water is beneficial to the leaching of enzymes and the decomposition of β-glucan.

[0042] In some embodiments of the present application, in step (2), the protein rest temperature is 50-55°C. The protein rest time is 50 min. This stage is to decompose the high molecular protein existing in the malt to meet the needs of yeast for medium and low molecular nitrogen content in the beer brewing process.

[0043] In some embodiments of the present application, in step (2), the protein rest saccharification temperature is 60-65℃. The saccharification time is 70 min. This stage is to allow the malt amylase to act, so as to increase the content of fermentable sugar.

[0044] In preferred embodiments of the present application, the saccharification time at 65℃ is 70 min. Since β-glucan inhibits starch hydrolysis, the saccharification time is appropriately extended, which is conducive to obtaining wort with higher sugar content and improving yield, etc.

[0045] In some embodiments of the present application, in step (2), the dextrinization temperature after saccharification is 75-80℃, and the dextrinization time is 10 min. At this temperature, the α-amylase still acts, and the residual starch can be further decomposed, while other enzymes are inhibited or inactivated.

[0046] In some embodiments of the present application, in step (2), the temperature rising rate from the end of the steeping to the protein rest, saccharification and dextrinization stages is 1℃ / min.

[0047] In some embodiments of the present application, in step (3), the ratio of the amount of water used for wort leaching to the wort raw material is 1.5-2:1 (L / kg).

[0048] In some embodiments of the present application, in step (3), the leaching water temperature is 78℃.

[0049] In some embodiments of the present application, in step (3), the boiling intensity is 10%, the boiling time is 1 h, and hops are added during boiling.

[0050] In some embodiments of the present application, in step (3), the amount of hops added is 1.0-1.2 g / L of wort raw material.

[0051] In some preferred embodiments of the present application, the hops are added in the following manner: 60% of the Saaz hops are added when the foam on the surface of the wort disappears due to heat degradation, and the remaining 40% of the Saaz hops are added 5 min before the end of boiling.

[0052] In some embodiments of the present application, in step (3), after the wort is cooled, lager dry yeast W34 / 70 is added, and the amount of addition is 1.0-1.3 g / L of the cooled wort. The lager dry yeast W34 / 70 is selected in the present application, which has high fermentation efficiency, good sedimentation, good flavor, moderate alcohol tolerance, and high microbial purity.

[0053] In some embodiments of the present application, in step (3), after inoculation of the yeast, fermentation is carried out at 13°C, the wort sugar content is reduced to 3.8-4.2 °P, the can is sealed, the diacetyl is reduced for 6 days, the reduction temperature is 15°C, the temperature is reduced by 6-7°C per day, the temperature is reduced to 1°C, and post-ripening is carried out for 7-14 days, and then the process is completed.

[0054] The following specific examples will be listed to explain the scheme of the present application. Those skilled in the art will understand that the following examples are only used to illustrate the present application, and should not be regarded as limiting the scope of the present application. If the specific technology or condition is not indicated in the examples, it is carried out according to the technology or condition described in the literature in the art or according to the product instruction. If the reagent or instrument is not indicated by the manufacturer, it is a conventional product that can be obtained by purchase.

[0055] Five grain powder: 36% sorghum + 22% rice + 18% waxy rice + 16% wheat + 8% corn. The fineness of sorghum, rice, waxy rice and wheat is 4, 6, 6 and 8 petals respectively, without whole grain mixed in. The size of corn powder is similar to the first four kinds, without more than 1 / 4 grain mixed in. The fine powder passing through a 20 mesh sieve is not more than 20% of the five kinds of mixed grain powder.

[0056] Example 1 Preparation of five-grain highland barley beer Take 45 kg of raw materials as an example, including 70% Pilsen malt, 20% five-grain powder and 10% highland barley to produce beer with original wort concentration of 12 °P, the specific steps are as follows: (1) High-land barley-five-grain gelatinization: After crushing, 4.5 kg of highland barley powder is obtained by passing through a 20 mesh sieve. According to the weight ratio of five-grain powder and highland barley powder 2:1, 9 kg of five-grain powder is mixed uniformly, then 54 L of water and 0.04% of raw material powder of amylase 5.4 g are added, the temperature is raised to 90°C, and the stirring is continuously carried out during the process, finally the sugarization is controlled at 92°C, when the starch iodine test does not change blue, the gelatinization is stopped, and the highland barley-five-grain gelatinization mash is obtained.

[0057] (2) Malt saccharification: 31.5 kg of Pilsen malt is crushed and soaked in 35°C water for 10 min, the water to material ratio is 4:1 (L / kg), after soaking, the highland barley-five-grain gelatinization mash in step (1) is added, the temperature is raised to 50°C for protein rest and maintained for 50 min, then the temperature is raised to 65°C for 70 min of saccharification, and finally the temperature is raised to 76°C for 10 min of dextrinization to obtain malt wort; the temperature raising rate is 1°C / min.

[0058] (3) Boiling, cooling and fermentation: the wort after saccharification was filtered and then 1:2 water was added at 78°C, the wort and water were mixed to form a mixed wort, the mixed wort was boiled for 1 h at a boiling intensity of 10%, during the boiling process, the following method was used to add Saaz hops: hot degradation to the disappearance of the foam on the surface of the wort, 60% of the Saaz hops were added, 5 min before the end of boiling, the remaining 40% of the Saaz hops were added, the total amount of hops added was 1.2 g / L based on the amount of wort obtained after filtration; after boiling, cooling was performed, then 1 g / L of lager dry yeast W34 / 70 was added to the cooled wort, and fermentation was performed at 13°C, when the wort sugar content decreased to 4.2 °P, the beer was canned, and the diacetyl was reduced for 6 days, then the temperature was reduced to 15°C, and the temperature was reduced by 7°C per day, when the temperature was reduced to 1°C, the beer was aged for 7-14 days, and then the five-grain highland barley beer was obtained.

[0059] Preparation of highland barley beer in Comparative Example 1 The difference from Example 1 is that 70% Pilsen malt and 30% highland barley are used. The other production processes are the same.

[0060] The flavor substances of the beers produced in Example 1 and Comparative Example 1 were compared and analyzed by GC-MS, and the results are shown in Table 1. Figure 1

[0061] The GC-MS detection steps are as follows: 1 ml of sample was taken in a headspace bottle, and then the bottle cap was tightly closed. Agilent 7890A gas chromatograph and Agilent 5977B inert mass spectrometer (running in electron ionization (EI) mode) were used to analyze volatile compounds. The volatile components were extracted by a 50 / 30 micron DVB / CAR / PDMS extraction head (Supelco, Bellefonte, PA). Before extraction, the sample was equilibrated at 50°C for 15 minutes, and then extracted at 50°C for 45 minutes.

[0062] The extraction head was then thermally desorbed in the GC injection port (230°C) for 3 minutes. The compounds were separated by a DB-WAXUI chromatographic column (60 m x 0.25 mm, 0.25 μm film thickness), the carrier gas was helium (constant flow rate 1 mL / min), and the programmed temperature conditions were as follows: initial 40°C for 2 minutes, increased to 230°C at 4°C / min, and finally kept at 5 minutes. The mass spectrometry detection used an electron impact ionization source (70 eV), the ion source temperature was 230°C, and the full scan range was 35-350 amu.

[0063] ​Qualitative and quantitative: the compounds were identified by NIST library matching (matching degree ≥ 85), by Kovats method to calculate the retention index (RI) of the compounds and by comparison with the RI reported in the literature, the difference of RI is less than 50. Semi-quantitative analysis was carried out according to the relative peak area of each volatile component and 4-octanol as internal standard.

[0064] The results are shown in Table 1. Figure 1 As shown in Table 1, 39 kinds of flavor compounds were detected in the five-grain highland barley beer of Example 1 and the highland barley beer of Comparative Example 1, including 17 kinds of esters, 8 kinds of alcohols, 6 kinds of terpenes, 5 kinds of acids and 3 kinds of aromatic compounds. The content of ester substances in the five-grain highland barley beer of the present application was higher than that of the highland barley beer of Comparative Example 1 except for ethyl acetate, thereby providing more fruit aroma to the wine body. The content of terpenes and aromatic compounds in the five-grain highland barley beer of the present application was higher than that of the highland barley beer, thereby providing fruit aroma, herbal aroma to the wine body. Among the alcohols, the content of 2-methyl-1-propanol, 3-methyl-1-butanol and 1-octanol in the five-grain highland barley beer of the present application was lower than that of the highland barley beer of Comparative Example 1, and the content of fusel oil was relatively low, so it was less likely to cause a headache when drinking. Moreover, the content of β-glucan in the five-grain highland barley beer of the present application was 48.24 mg / L.

Claims

1. A method for preparing Wuliang barley beer, characterized in that: The following steps are involved: (1) Highland barley-five-grain gelatinization: Highland barley flour and five-grain flour are mixed, water and amylase are added, and the temperature is raised to the amylase hydrolysis temperature for gelatinization to obtain highland barley-five-grain gelatinized mash; (2) Malt saccharification: After the barley malt is crushed, it is soaked in water. At the end of the soaking, the highland barley-five-grain gelatinized mash in step (1) is added, and after mixing, protein rest, saccharification and dextrinization are performed to obtain wort; (3) Boiling, cooling and fermenting: After the wort is filtered, the wort is rinsed with lees, and the lees water and the filtered wort are mixed to form a mixed wort. After boiling and cooling, yeast is added for fermentation until the fermentation is completed; wherein, in the beer raw materials, the mass contents of barley malt powder, highland barley powder and five-grain powder are 70-75%, 7.5-10% and 17.5-20% respectively.

2. The method for making Wuliang barley beer according to claim 1, wherein In step (1), at least one of the following conditions must be met: Highland barley flour is obtained by crushing highland barley and passing it through a 20-mesh sieve; The fine powder of five-grain flour that can pass through a 20-mesh sieve is ≤20%; Five-grain flour is composed of 36% sorghum, 22% rice, 18% glutinous rice, 16% wheat and 8% corn; The amount of amylase added is 0.04% of the total amount of highland barley flour and five-grain flour; Water: barley and five-grain mixture = (3-4): 1 (L / kg); Saccharify at 90-95°C until the starch does not turn blue when tested with iodine.

3. The method for making Wuliang barley beer according to claim 1 or 2, wherein: In step (2), at least one of the following conditions must be met: The crushed malt is soaked in 35°C water; The ratio of soaking water to malt is (3-4):1 (L / kg); The heating rate from the end of immersion to the protein rest, saccharification and dextrinization stages was 1°C / min.

4. The method for making Wuliang highland barley beer according to any one of claims 1 to 3, characterized in that: In step (2), the protein resting temperature is 50-55°C, and the protein resting time is 50 min.

5. The method for making Wuliang barley beer according to any one of claims 1 to 4, characterized in that: In step (2), the saccharification temperature after protein rest is 60-65°C, and the saccharification time is 70 min.

6. The method for making Wuliang barley beer according to any one of claims 1 to 5, characterized in that: In step (2), after saccharification, dextrinization is performed at a temperature of 75 to 80° C. and a dextrinization time of 10 min.

7. The method for making Wuliang barley beer according to any one of claims 1 to 6, characterized in that: In step (3), the ratio of the amount of water used for leaching the grains to the amount of beer raw materials is 1.5 to 2:1 (L / kg), and the temperature of the leaching water is 78°C.

8. The method for making Wuliang barley beer according to any one of claims 1 to 7, characterized in that: In step (3), at least one of the following conditions must be met: The boiling intensity is 10%, the boiling time is 1 h, and hops are added during the boiling process; The amount of hops added is 1.0-1.2 g / L of wort raw materials; After the wort is cooled, add lager dry yeast W34 / 70, and the addition amount is 1.0-1.3 g / L of the cooled wort.

9. The method for making Wuliang barley beer according to any one of claims 1 to 8, characterized in that: In step (3), after yeast inoculation, fermentation is carried out at 13°C. When the sugar content of the wort drops to 3.8-4.2 °P, the can is sealed. After 6 days of diacetyl reduction, the temperature is lowered. The reduction temperature is 15°C, and the temperature is lowered by 6-7°C every day. When the temperature drops to 1°C, the wort is ripened for 7-14 days.

10. Wuliang barley beer prepared by the method according to any one of claims 1 to 9.

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