Method for preparing high-SOD oral liquid by fermenting high-SOD rice with probiotics

Abstract

The invention provides a method for preparing high-SOD oral liquid by fermenting high-SOD rice with probiotics, which solves the technical problems of large SOD activity loss and poor product stability in the prior art through a process of combining directional expanding culture of composite strains and anaerobic fermentation with dynamic stability regulation and control. The SOD activity of the prepared high-SOD oral liquid is larger than or equal to 180 U / mL, the shelf life reaches 2 years, and the SOD content is increased by 12 times compared with that of a traditional method.

Description

Technical Field

[0001] The present invention relates to the technical field of food processing, and in particular to a method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice. Background Art

[0002] Superoxide dismutase (SOD) is a key antioxidant enzyme widely present in living organisms. It can effectively scavenge superoxide free radicals and delay cell damage caused by oxidative stress, and has important application value in the fields of functional foods and health products. In recent years, SOD-rich foods and beverages have attracted much attention due to their antioxidant and anti-aging effects. However, there are some significant defects in the existing technologies. For example, the retention rate of SOD activity is low. In traditional fermentation processes, high-temperature sterilization or long-time fermentation easily leads to heat-sensitive inactivation of SOD, resulting in generally low SOD activity in the final products.

[0003] Most of the existing fermentation technologies rely on single strains, resulting in limited types of metabolites and easy attenuation of viable cell counts. In addition, single strains have poor adaptability to complex substrates, low fermentation efficiency, and it is difficult to maintain the activity of probiotics in the final product. Liquid preparations are also prone to problems such as stratification, oxidation, and rapid decline of viable cell counts during storage. Conventional stability regulation relies on chemical preservatives, which may affect the natural properties of the product, and the packaging cannot effectively block light, leading to oxidative inactivation of SOD and shortening the shelf life of the product.

[0004] In view of these problems, there is an urgent need for an innovative method that can balance high SOD activity retention, improved stability, and industrial feasibility. Summary of the Invention

[0005] The present invention provides a method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice, so as to solve the technical defects of low SOD activity retention and poor stability of SOD oral liquid in the existing technologies.

[0006] On the one hand, the present invention provides a method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice, comprising the following steps: (1) Soak the SOD rice, with the soaking liquid completely covering the rice grains, and then break it to a particle size ≤ 200 mesh through a pulper or a grinder to obtain rice slurry; (2) Compound probiotics into a composite strain in a ratio of 1:1:1, and obtain an active bacterial liquid through two-stage expansion culture; (3) Put the rice slurry, activated bacterial liquid, honey, and water into a 2-ton fermentation tank according to a mass ratio of 100:10:10:1000, and carry out anaerobic fermentation. Stir for 0.5 hours every 12 hours during the process to obtain a fermentation broth; (4) Add 0.05 - 0.15% salt, 0.3 - 0.7% blended oil, and 3 - 7% cyclodextrin to the fermentation broth. After two rapid homogenizations, stir and ripen at 75 - 85°C at a rotation speed of 30 rpm for 30 minutes, and then perform rapid homogenization again to obtain a ripened liquid. (5) Mix the ripened liquid with water at a ratio of 1:1, add 6 - 7% fructose syrup to adjust the sweetness, and sterilize by ultra-high temperature instantaneous sterilization. (6) Seal with a light-proof bottle with a light transmittance ≤ 5% to obtain a high-SOD oral liquid. The SOD rice is superoxide dismutase (SOD) rice that is naturally generated during the planting process and has an SOD activity of 210 - 250 U / g, and its quality meets the first-class high-quality rice standard of GB / T 1354. The soaking time is 5 - 7 hours. The probiotics are any three of Lactobacillus acidophilus, Lactobacillus plantarum, Lactobacillus rhamnosus, Lactobacillus casei, and Lactobacillus pentosus. The activity of the activated bacterial liquid is 0.8×10 9 ~ 1.2×10 9 CFU / mL. The temperature of the anaerobic fermentation is 28 - 37°C, the time of the anaerobic fermentation is 48 - 96 hours, and the rotation speed of the stirring is 50 rpm. The time of the rapid homogenization is 1 - 3 minutes, and the pressure is 18 - 22 MPa. The temperature of the ultra-high temperature instantaneous sterilization is 30 - 140°C, and the time is 3 - 7 seconds.

[0007] According to a method for preparing a high-SOD oral liquid by fermenting high-SOD rice with probiotics provided by the present invention, the two-stage expansion culture described in step (2) includes: The first stage: culture in MRS medium at 37°C for 24 hours. The second stage: use rice slurry as a nutrient matrix and expand the culture at 30°C for 12 hours.

[0008] According to a method for preparing a high-SOD oral liquid by fermenting high-SOD rice with probiotics provided by the present invention, the dissolved oxygen content of the anaerobic fermentation described in step (3) is ≤ 0.5 mg / L.

[0009] According to a method for preparing a high-SOD oral liquid by fermenting high-SOD rice with probiotics provided by the present invention, the cyclodextrin described in step (4) is hydroxypropyl-β-cyclodextrin, and its addition amount is dynamically adjusted to 3 - 7% according to the consistency.

[0010] According to a method for preparing a high-SOD oral liquid by fermenting high-SOD rice with probiotics provided by the present invention, the light-proof bottle mouth in step (6) is filled and sealed with nitrogen.

[0011] According to a method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by the present invention, in step (6), the SOD activity of the high-SOD oral liquid is ≥180 U / mL, and the viable count of lactic acid bacteria is ≥1×10 8 CFU / mL.

[0012] According to a method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by the present invention, in step (1), the pH value of the soaking solution is 6.5 - 7.0, and the water content of the rice after soaking is 40 - 45%.

[0013] According to a method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by the present invention, in step (3), the honey is sophora flower honey.

[0014] According to a method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by the present invention, in step (4), the blended oil is high-oleic sunflower oil, and its peroxide value is ≤5 meq / kg.

[0015] On the other hand, the present invention provides a high-SOD oral liquid prepared by a method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice.

[0016] The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by the present invention has the following advantages compared with the prior art: (1) The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by the present invention combines the co-fermentation of composite strains with an anaerobic environment to achieve a technical effect that the SOD activity retention rate is ≥85% and the SOD activity of the high-SOD oral liquid is ≥180 U / mL, significantly improving the retention of SOD activity. Compared with the traditional preparation method, the SOD content in the oral liquid prepared in this application is increased by 12 times.

[0017] (2) The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by the present invention dynamically regulates the consistency of the liquid preparation through hydroxypropyl-β-cyclodextrin and combines nitrogen sealing to improve the stability of the high-SOD oral liquid, solving the problems of stratification and oxidation of the SOD oral liquid.

[0018] (3) The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by the present invention reduces the loss of heat-sensitive components while killing microorganisms through ultra-high temperature instantaneous sterilization. After ultra-high temperature instantaneous sterilization, the oral liquid meets the requirements of GB7101-2022 "National Food Safety Standard Beverages" for microbial indicators, and the shelf life is extended by more than 50% compared with the traditional process. Description of the Drawings

[0019] To more clearly illustrate the technical solutions in the present invention or the prior art, the following briefly introduces the drawings required for the description of the embodiments or the prior art. Obviously, the drawings in the following description are some embodiments of the present invention. For those of ordinary skill in the art, without creative efforts, other drawings can also be obtained based on these drawings.

[0020] Figure 1 It is a process flow chart of the method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by an embodiment of the present invention; Figure 2 It is a comparison chart of the SOD activity changes before and after fermentation of the method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice provided by an embodiment of the present invention. Detailed implementation manners

[0021] To make the objectives, technical solutions and advantages of the present invention clearer, the following clearly and completely describes the technical solutions in the present invention with reference to the drawings in the present invention. Obviously, the described embodiments are some, but not all, of the embodiments of the present invention. All other embodiments obtained by those of ordinary skill in the art without creative efforts based on the embodiments in the present invention belong to the scope protected by the present invention.

[0022] The present invention provides a method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice, including the following steps: (1) Soak the SOD rice, with the soaking liquid completely covering the rice grains, and then crush it to a particle size ≤ 200 mesh through a beater or a grinder to obtain rice slurry; (2) Compound probiotics into a composite strain in a ratio of 1:1:1, and obtain an active bacterial liquid through two-stage expansion culture; (3) Put the rice slurry, activated bacterial liquid, honey and water into a 2-ton fermentation tank according to a mass ratio of 100:10:10:1000, and carry out anaerobic fermentation. Stir for 0.5 hours every 12 hours during the period to obtain a fermentation broth; (4) Add 0.05 - 0.15% salt, 0.3 - 0.7% blended oil and 3 - 7% cyclodextrin to the fermentation broth. After two rapid homogenizations, stir and ripen at 75 - 85 °C at a speed of 30 rpm for 30 minutes, and then carry out rapid homogenization again to obtain a ripened liquid; (5) Mix the ripened liquid with water in a ratio of 1:1, add 6 - 7% fructose syrup to adjust the sweetness, and perform ultra-high temperature instantaneous sterilization; (6) Seal it with a light-proof bottle with a light transmittance ≤ 5% to obtain high-SOD oral liquid; The SOD rice is superoxide dismutase (SOD) rice that is naturally generated during the planting process and has an SOD activity of 210-250 U / g, and its quality meets the first-class high-quality rice standard of GB / T1354, preferably 220-240 U / g, and more preferably 225-235 U / g; The soaking time is 5-7 hours, preferably 5.5-6.5 hours; The probiotics are any three of Lactobacillus acidophilus, Lactobacillus plantarum, Lactobacillus rhamnosus, Lactobacillus casei, and Lactobacillus pentosus, preferably Lactobacillus acidophilus, Lactobacillus rhamnosus, and Lactobacillus casei; The activity of the activated bacterial liquid is 0.8×10 9 ~1.2×10 9 CFU / mL, preferably 0.9×10 9 ~1.1×10 9 CFU / mL; The temperature of the anaerobic fermentation is 28-37°C, preferably 30-35°C; the time of the anaerobic fermentation is 48-96 hours, preferably 60-84 hours; the rotation speed of the stirring is 50 rpm; The time of the rapid homogenization is 1-3 minutes, and the pressure is 18-22 MPa, preferably 19-21 MPa; The temperature of the ultra-high temperature instantaneous sterilization is 130-140°C, preferably 133-137°C, and the time is 3-7 seconds, preferably 4-6 seconds.

[0023] In the present invention, the two-stage amplification culture described in step (2) includes: The first stage: Culturing at 37°C for 24 hours in MRS medium; The second stage: Using rice slurry as the nutrient matrix and amplifying the culture at 30°C for 12 hours.

[0024] In the present invention, the dissolved oxygen content of the anaerobic fermentation described in step (3) is ≤0.5 mg / L.

[0025] In the present invention, the cyclodextrin described in step (4) is hydroxypropyl-β-cyclodextrin, and its addition amount is dynamically adjusted to 3-7% according to the consistency.

[0026] In the present invention, the mouth of the light-proof bottle in step (6) is filled and sealed with nitrogen.

[0027] In the present invention, the SOD activity of the high-SOD oral liquid in step (6) is ≥180 U / mL, and the viable count of lactic acid bacteria is ≥1×10 8 CFU / mL.

[0028] In the present invention, the pH value of the soaking solution in step (1) is 6.5 - 7.0, and the water content of the rice after soaking is 40 - 45%.

[0029] In the present invention, the honey mentioned in step (3) is sophora flower honey.

[0030] In the present invention, the blending oil mentioned in step (4) is high-oleic sunflower oil, and its peroxide value ≤ 5 meq / kg.

[0031] The present invention also provides a high-SOD oral liquid prepared by a method for preparing a high-SOD oral liquid by fermenting high-SOD rice with probiotics.

[0032] Example 1 Select 100 kg of SOD rice with an SOD activity of 230 U / g, soak it in water for 6 hours, during which the water completely covers the rice grains, and then grind it into a slurry with a particle size of 180 mesh through a grinder to obtain a rice slurry; Take Lactobacillus acidophilus, Lactobacillus rhamnosus and Lactobacillus casei in a ratio of 1:1:1 as a composite strain, first culture it in MRS medium at 37 °C for 24 hours, and then use the rice slurry as a nutrient matrix to expand the culture at 30 °C for 12 hours to obtain an active bacterial liquid; after detection, the activity of the active bacterial liquid is 1.0×10 9 CFU / mL; Put the rice slurry, activated bacterial liquid, sophora flower honey and water into a 2-ton fermentation tank according to a mass ratio of 100:10:10:1000 for anaerobic fermentation, control the dissolved oxygen content to 0.3 mg / L, ferment at 35 °C for 72 hours, and stir at a speed of 50 rpm for 0.5 hours every 12 hours during this period to obtain a fermentation liquid; after detection, the SOD activity of the fermentation liquid is 200 U / mL; Add 56 kg of hydroxypropyl-β-cyclodextrin, 5.8 kg of high-oleic sunflower oil with a peroxide value of 3 meq / kg, and 1.16 kg of table salt to the fermentation liquid, carry out two rapid homogenizations for 2 minutes each under the condition of 20 MPa, and then stir and ripen at 80 °C at a speed of 30 rpm for 30 minutes, and carry out rapid homogenization for 2 minutes again under the condition of 20 MPa to obtain a ripened liquid; Mix the ripened liquid with water at a ratio of 1:1, add 73 kg of fructose syrup to adjust the sweetness, and carry out ultra-high temperature instantaneous sterilization at 135 °C for 5 seconds; Use a light-proof bottle with a light transmittance ≤ 5%, and fill and seal the bottle mouth with nitrogen to obtain a high-SOD oral liquid.

[0033] After storing at room temperature for 24 months, there is no layering or oxidation phenomenon.

[0034] Example 2 Select 100 kg of SOD rice with an SOD activity of 210 U / g, soak it in water for 5 hours, with the water completely covering the rice grains during this period, and then grind it into a slurry with a particle size of 200 mesh through a grinder to obtain rice slurry; Use Lactobacillus acidophilus, Lactobacillus rhamnosus, and Lactobacillus casei in a ratio of 1:1:1 as a composite strain. First, culture it in MRS medium at 37 °C for 24 hours, and then use the rice slurry as a nutrient substrate and expand the culture at 30 °C for 12 hours to obtain an active bacterial liquid; after testing, the activity of the active bacterial liquid is 0.8×10 9 CFU / mL; Put the rice slurry, activated bacterial liquid, sophora flower honey, and water into a 2-ton fermentation tank for anaerobic fermentation according to a mass ratio of 100:10:10:1000, control the dissolved oxygen content to 0.5 mg / L, and ferment at 28 °C for 96 hours. During this period, stir at a speed of 50 rpm for 0.5 hours every 12 hours to obtain a fermentation liquid; after testing, the SOD activity of the fermentation liquid is 180 U / mL; Add 34 kg of hydroxypropyl-β-cyclodextrin, 5.8 kg of high-oleic sunflower oil with a peroxide value of 3 meq / kg, and 1.16 kg of table salt to the fermentation liquid, perform two rapid homogenizations for 3 minutes each under the condition of 18 MPa, and then stir and ripen at 75 °C at a speed of 30 rpm for 30 minutes, and perform rapid homogenization for 2 minutes again under the condition of 20 MPa to obtain a ripened liquid; Mix the ripened liquid with water at a ratio of 1:1, add 73 kg of fructose syrup to adjust the sweetness, and perform ultra-high temperature instantaneous sterilization at 135 °C for 7 seconds; Use a light-proof bottle with a light transmittance ≤ 5%, and fill and seal the bottle mouth with nitrogen to obtain a high-SOD oral liquid.

[0035] After storing at room temperature for 18 months, it is slightly oxidized but does not layer.

[0036] Example 3 Select 100 kg of SOD rice with an SOD activity of 240 U / g, soak it in water for 7 hours, with the water completely covering the rice grains during this period, and then grind it into a slurry with a particle size of 150 mesh through a grinder to obtain rice slurry; Use Lactobacillus acidophilus, Lactobacillus rhamnosus, and Lactobacillus casei in a ratio of 1:1:1 as a composite strain. First, culture it in MRS medium at 37 °C for 24 hours, and then use the rice slurry as a nutrient substrate and expand the culture at 30 °C for 12 hours to obtain an active bacterial liquid; after testing, the activity of the active bacterial liquid is 1.2×10 9 CFU / mL; Put rice slurry, activated bacterial liquid, sophora flower honey and water into a 2-ton fermentation tank according to the mass ratio of 100:10:10:1000 for anaerobic fermentation. Control the dissolved oxygen content at 0.2 mg / L and ferment at 37°C for 48 hours. During this period, stir at a speed of 50 rpm for 0.5 hours every 12 hours to obtain a fermentation broth. After testing, the SOD activity of the fermentation broth is 210 U / mL; Add 78 kg of hydroxypropyl-β-cyclodextrin, 5.8 kg of high-oleic sunflower oil with a peroxide value of 3 meq / kg, and 1.16 kg of table salt to the fermentation broth. After performing two rapid homogenizations for 1 minute each under the condition of 22 MPa, stir and ripen at 85°C at a speed of 30 rpm for 30 minutes, and then perform rapid homogenization again for 2 minutes under the condition of 20 MPa to obtain a ripened liquid; Mix the ripened liquid with water at a ratio of 1:1, add 73 kg of fructose syrup to adjust the sweetness, and perform ultra-high temperature instantaneous sterilization at 140°C for 3 seconds; Use a light-proof bottle with a light transmittance ≤ 5%, and fill and seal the bottle mouth with nitrogen to obtain a high-SOD oral liquid.

[0037] After storing at room temperature for 24 months, the stability is good.

[0038] Comparative Example 1 Select 100 kg of ordinary rice with an SOD activity of 15 U / g, soak it in water for 6 hours, during which the water completely covers the rice grains, and then grind it into a slurry with a particle size of 200 mesh through a grinder to obtain rice slurry; Culture Lactobacillus acidophilus in MRS medium at 37°C for 24 hours to obtain a bacterial liquid. After testing, the activity of the bacterial liquid is 1.2×10 9 CFU / mL; Put rice slurry, bacterial liquid, sophora flower honey and water into a 2-ton fermentation tank according to the mass ratio of 100:10:10:1000 for fermentation. Control the dissolved oxygen content at 1.0 mg / L and ferment at 35°C for 72 hours. During this period, stir at a speed of 50 rpm for 0.5 hours every 12 hours to obtain a fermentation broth. After testing, the SOD activity of the fermentation broth is 9 U / mL; Add 78 kg of hydroxypropyl-β-cyclodextrin, 5.8 kg of high-oleic sunflower oil with a peroxide value of 3 meq / kg, and 1.16 kg of table salt to the fermentation broth. After performing two rapid homogenizations for 1 minute each under the condition of 22 MPa, stir and ripen at 85°C at a speed of 30 rpm for 30 minutes, and then perform rapid homogenization again for 2 minutes under the condition of 20 MPa to obtain a ripened liquid; Mix the ripened liquid with water at a ratio of 1:1, add 73 kg of fructose syrup to adjust the sweetness, and perform pasteurization at 75°C for 30 minutes; Seal with a transparent bottle to obtain an oral liquid.

[0039] After 6 months of storage at room temperature, serious stratification occurred and the SOD activity loss reached 70%.

[0040] It can be seen from the statistics that through the co-fermentation of composite strains, dynamic stability regulation and ultra-high temperature instantaneous sterilization, the present invention significantly improves the activity retention rate and shelf life of SOD, which are comprehensively superior to the traditional process Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention, rather than to limit them; although the present invention has been described in detail with reference to the foregoing embodiments, those of ordinary skill in the art should understand that they can still modify the technical solutions recorded in the foregoing embodiments, or perform equivalent replacements on some of the technical features; and these modifications or replacements do not make the essence of the corresponding technical solutions deviate from the spirit and scope of the technical solutions of the embodiments of the present invention.

Claims

1. A method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice, characterized in that, It includes the following steps: (1) Soak the SOD rice, with the soaking liquid completely covering the rice grains, and then break it to a particle size of ≤200 mesh through a pulper or grinder to obtain rice slurry; (2) Compound probiotics into a composite strain in a ratio of 1:1:1, and obtain an active bacterial liquid through two-stage expansion culture; (3) Put the rice slurry, activated bacterial liquid, honey and water into a 2-ton fermentation tank according to a mass ratio of 100:10:10:1000, and carry out anaerobic fermentation. Stir for 0.5 hours every 12 hours during the period to obtain a fermentation liquid; (4) Add 0.05~0.15% table salt, 0.3~0.7% blending oil and 3~7% cyclodextrin to the fermentation liquid. After two rapid homogenizations, stir and ripen at 75~85°C at a speed of 30 rpm for 30 minutes, and then carry out rapid homogenization again to obtain a ripened liquid; (5) Mix the ripened liquid with water in a ratio of 1:1, add 6~7% fructose syrup to adjust the sweetness, and carry out ultra-high temperature instantaneous sterilization; (6) Seal it with a light-proof bottle with a light transmittance of ≤5% to obtain a high-SOD oral liquid; The SOD rice is superoxide dismutase (SOD) rice that is naturally generated during the planting process and has an SOD activity of 210~250 U / g, and its quality meets the first-class high-quality rice standard of GB / T1354; The soaking time is 5~7 hours; The probiotics are any three of Lactobacillus acidophilus, Lactobacillus plantarum, Lactobacillus rhamnosus, Lactobacillus casei and Lactobacillus pentosus; The activity of the activated bacterial liquid is 0.8×10 9 ~1.2×10 9 CFU / mL; The temperature of the anaerobic fermentation is 28~37°C, the time of the anaerobic fermentation is 48~96 hours, and the stirring speed is 50 rpm; The time of the rapid homogenization is 1~3 minutes, and the pressure is 18~22 MPa; The temperature of the ultra-high temperature instantaneous sterilization is 130~140°C, and the time is 3~7 seconds.

2. The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice according to claim 1, characterized in that, The two-stage expansion culture described in step (2) includes: The first stage: culture in MRS medium at 37°C for 24 hours; The second stage: use rice slurry as the nutrient matrix and expand culture at 30°C for 12 hours.

3. The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice according to claim 1, characterized in that The dissolved oxygen content of the anaerobic fermentation described in step (3) is ≤0.5 mg / L.

4. The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice according to claim 1, characterized in that, The cyclodextrin described in step (4) is hydroxypropyl-β-cyclodextrin, and its addition amount is dynamically adjusted to 3~7% according to the consistency.

5. The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice according to claim 1, characterized in that, The light-proof bottle mouth described in step (6) is filled and sealed with nitrogen.

6. The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice according to claim 1, characterized in that, In step (6), the SOD activity of the high-SOD oral liquid is ≥180 U / mL, and the viable count of lactic acid bacteria is ≥1×10 8 CFU / mL.

7. The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice according to claim 1, wherein The pH value of the soaking liquid described in step (1) is 6.5~7.0, and the water content of the rice after soaking is 40~45%.

8. The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice according to claim 1, characterized in that, The honey described in step (3) is sophora flower honey.

9. The method for preparing high-SOD oral liquid from probiotic-fermented high-SOD rice according to claim 1, wherein The blending oil described in step (4) is high-oleic sunflower oil, and its peroxide value is ≤5 meq / kg.

10. A high-SOD oral liquid prepared by the method according to any one of claims 1~9.

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