JP2006204192A - Coffee beverage composition - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a coffee beverage composition having excellent hypotension function. <P>SOLUTION: The coffee beverage composition contains the following components (A) and (B): (A) 0.01-1 mass% of chlorogenic acid, and (B) less than 0.1 mass% of hydroxy hydroquinone chlorogenic acid. <P>COPYRIGHT: (C)2006,JPO&NCIPI

Description

  The present invention relates to a coffee beverage composition having a blood pressure lowering effect.

  Antihypertensive drugs include various neuroleptic agents that act on the regulatory system of neural factors, ACE inhibitors that act on the regulatory system of humoral factors, AT receptor antagonists, and regulatory systems of vascular endothelium-derived substances Drugs such as Ca antagonists and antihypertensive diuretics related to the body fluid regulation system in the kidney can be mentioned, and these are mainly used in medical institutions for patients with severe hypertension. However, drugs currently used for the purpose of antihypertensive disease are satisfactory in terms of effectiveness, but the burden on patients is large due to the side effects that are present.

  Moreover, general therapies based on lifestyle improvements such as diet therapy, exercise therapy, and restrictions on drinking and smoking are widely applied to those with normal hypertension including those with mild to severe hypertension. With the increasing awareness of the importance of general therapy, it has been said that improving dietary habits is particularly important. Many foods having a blood pressure lowering action have been extensively searched for food-derived antihypertensive materials, and many active ingredients have been separated and identified.

Among these, it has been reported that chlorogenic acid, caffeic acid, ferulic acid and the like contained in foods such as coffee show excellent blood pressure lowering action (Patent Documents 1 to 3). However, coffee beverages known to contain a large amount of chlorogenic acids do not have a clear blood pressure lowering effect, and there is a report that blood pressure is increased (Non-patent Document 1).
JP 2002-363075 A JP 2002-22062 A JP 2002-53464 A Eur. J. Clin. Nutr., 53 (11), 831 (1999)

  An object of the present invention is to provide a food or drink that has an excellent action for improving hypertension and can be usually taken.

  Therefore, the present inventor has paid attention to the fact that coffee beverages do not show sufficient blood pressure lowering action despite containing chlorogenic acid, and as a result of various studies on the relationship between blood pressure lowering action and coffee beverage ingredients, It has been found that hydroxyhydroquinone contained in beverages inhibits the blood pressure lowering action of chlorogenic acids. And as a result of further investigation, if the amount of chlorogenic acids in the coffee beverage is kept within a certain range and the hydroxyhydroquinone content is lowered below a certain amount sufficiently smaller than the amount normally contained, the coffee beverage having an excellent blood pressure lowering effect It was found that a composition was obtained.

That is, the present invention includes the following components (A) and (B),
(A) Chlorogenic acids 0.01-1% by mass,
(B) Hydroxyquinone A coffee beverage composition containing less than 0.1% by mass of the amount of chlorogenic acids is provided.

The present invention also includes the following components (A) and (B),
(A) Chlorogenic acids 0.1 to 10% by mass,
(B) Hydroxyquinone A soluble coffee composition containing less than 0.1% by mass of the amount of chlorogenic acids is provided.

The present invention also includes the following components (A) and (B),
(A) Chlorogenic acids 0.01-1% by mass,
(B) Hydroxyquinone A container-packed beverage filled with a coffee beverage composition containing less than 0.1% by mass of chlorogenic acids is provided.
The present invention also relates to a coffee beverage composition containing 0.01 to 1% by mass of chlorogenic acids, which is based on gallic acid when gallic acid (gallic acid) is used as a standard substance in analysis by high performance liquid chromatography. It is intended to provide a coffee beverage composition characterized by having substantially no peak in a time region of a relative holding time of 0.54 to 0.61, and a packaged beverage filled with the coffee beverage composition.
The present invention also relates to a soluble coffee composition containing 0.1 to 10% by mass of chlorogenic acids, and the relative retention time for gallic acid when gallic acid is used as a standard substance in the analysis by high performance liquid chromatography. The present invention provides a soluble coffee composition characterized by having substantially no peak in the time range of 0.54 to 0.61.

  The coffee beverage composition of the present invention has an excellent antihypertensive effect, that is, an antihypertensive effect or an antihypertensive effect, and can be taken for a long time. Therefore, the coffee beverage composition of the present invention is a food indicated as being used as a medicament for improving hypertension, for lowering blood pressure, for suppressing blood pressure increase, or for higher blood pressure. Useful as.

The coffee beverage composition of the present invention contains 0.01 to 1% by mass of (A) chlorogenic acids, preferably 0.05 to 1% by mass in terms of blood pressure lowering effect, blood pressure increase inhibiting effect, and taste. More preferably, the content is 0.1 to 1% by mass. Moreover, although the soluble coffee composition of this invention contains 0.1-10 mass% of chlorogenic acids, Preferably it is 0.5-10 mass%, More preferably, it contains 1-10 mass%. (A) The chlorogenic acids include (A ¹ ) monocaffeoylquinic acid, (A ² ) ferulaquinic acid, and (A ³ ) dicaffeoylquinic acid. Here, (A ¹ ) monocaffeoylquinic acid includes at least one selected from 3-caffeoylquinic acid, 4-caffeoylquinic acid and 5-caffeoylquinic acid. Examples of (A ² ) ferulquinic acid include one or more selected from 3-ferlaquinic acid, 4-ferlaquinic acid and 5-ferlaquinic acid. (A ³ ) Examples of dicaffeoylquinic acid include one or more selected from 3,4-dicaffeoylquinic acid, 3,5-dicaffeoylquinic acid, and 4,5-dicaffeoylquinic acid. The content of the chlorogenic acids can be measured by high performance liquid chromatography (HPLC). As a detection means in HPLC, UV detection is generally used, but it can also be detected with higher sensitivity by CL (chemiluminescence) detection, EC (electrochemical) detection, LC-Mass detection, or the like.

  The coffee beverage composition or soluble coffee composition of the present invention contains less than 0.1% by mass of hydroxyhydroquinone (B) with respect to the amount of chlorogenic acids. If the amount of hydroxyhydroquinone is less than 0.1% by mass relative to the amount of chlorogenic acids, the blood pressure lowering action of chlorogenic acids is sufficiently exhibited. More preferably, it is 0.03 mass% or less, Most preferably, it is 0.01 mass% or less. If the amount of hydroxyhydroquinone is 0.01% by mass or less with respect to the amount of chlorogenic acids, the blood pressure lowering action of chlorogenic acid is not suppressed at all. Here, the hydroxyhydroquinone content in the composition of the present invention may be zero.

  The hydroxyhydroquinone content can be measured by high performance liquid chromatography (HPLC). As a detection means in HPLC, UV detection is generally used, but it can also be detected with higher sensitivity by CL (chemiluminescence) detection, EC (electrochemical) detection, LC-Mass detection, or the like. In addition, in measuring the hydroxyhydroquinone content by HPLC, it can also measure after concentrating a coffee drink.

  Furthermore, the hydroxyhydroquinone content can be directly measured by HPLC, but from the coffee beverage composition or soluble coffee beverage composition, hydroxyhydroquinone is concentrated by various chromatographies, and the amount of the concentrated fraction is measured. Can also be quantified. In the measurement of the amount of chlorogenic acids and the amount of hydroxyhydroquinone, in the case of a packaged beverage, immediately after opening, hydrochloric acid is added so as to become, for example, 0.1 N (normative), or 0.1 N hydrochloric acid / water. It is preferable to measure in a sodium oxide buffer system.

  The coffee beverage composition and soluble coffee composition of the present invention preferably contain ordinary coffee components as they are, except for reducing the hydroxyhydroquinone content.

The coffee beverage composition of the present invention preferably contains 30 to 300 mg / 100 g, further 40 to 250 mg / 100 g, particularly 50 to 200 mg / 100 g of potassium, based on 100 g of the coffee beverage composition. In addition, the soluble coffee composition of the present invention contains potassium in an amount of 20 to 200 mg / 1 g, further 30 to 180 mg / 1 g, particularly 40 to 150 mg / 1 g based on 1 g of the soluble coffee composition. Is preferable. In order to make potassium content into the said range, it is preferable not to perform operation, such as removing potassium positively in the manufacture process of a coffee drink composition.
The coffee beverage composition of the present invention has an ash content of 280 mg or less, more preferably 250 mg or less, even more preferably 220 mg or less, particularly 200 mg or less, based on 100 g of the coffee beverage composition. It is preferable in terms of the flavor. Ash content is measured according to the method described in the 4th Japanese Food Standard Composition Table (published in 1982, edited by the Science and Technology Agency Resource Research Committee, page 28), and heated at 550 ° C until there is no residual carbon and a constant weight is obtained. It can be measured using the ashing method. In order to make the amount of ash within the above range, in the process of producing a coffee beverage composition, an operation that increases the amount of ash is not performed, such as treatment with strong alkali and then returning to the neutral region using acid. Is preferred.

The coffee beverage composition of the present invention preferably has a H ₂ O ₂ (hydrogen peroxide) content of 1 ppm or less, more preferably 0.1 ppm or less, particularly 0.01 ppm or less from the viewpoint of the original flavor of coffee. The measurement of hydrogen peroxide can be performed using a commonly used hydrogen peroxide meter. For example, a high-sensitivity hydrogen peroxide meter Super Orientor Model 5 (SUPER ORITECTOR MODEL 5) manufactured by Central Science Co., Ltd. can be used. .

  Although the kind of coffee bean used for the coffee drink composition of this invention is not specifically limited, For example, Brazil, Colombia, Tanzania, mocha etc. are mentioned. Examples of coffee types include Arabica and Robusta. One kind of coffee beans may be used, or a plurality of kinds may be blended. There are no particular restrictions on the roasting method of roasted coffee beans, and there are no restrictions on the roasting temperature and roasting environment, and ordinary methods can be employed. Furthermore, there is no restriction | limiting also about the extraction method from the bean, For example, the method of extracting from a roasted coffee bean or its ground material using water-hot water (0-100 degreeC) for 10 second-30 minutes is mentioned. Examples of the extraction method include a boiling type, an espresso type, a siphon type, and a drip type (paper, flannel, etc.).

  The coffee beverage composition of the present invention refers to one using 1 g or more of coffee beans per 100 g in terms of green beans. Preferably, 2.5 g or more of coffee beans are used. More preferably, 5 g or more of coffee beans are used. When making the coffee drink composition of this invention into a container-packed drink, it is preferable that it is a single strength. Here, “single strength” means that after opening a packaged beverage, it can be taken as it is without being diluted.

The coffee beverage composition or soluble coffee composition of the present invention can be obtained by reducing the hydroxyhydroquinone content by treating the roasted coffee bean extract with an adsorbent. Examples of the adsorbent include activated carbon and reverse phase carrier. More specifically, after adding an adsorbent to an aqueous solution of a roasted coffee bean extract or a dried product of the roasted coffee bean extract and stirring at 0 to 100 ° C. for 10 minutes to 5 hours, the adsorbent is removed. Good. Here, the adsorbent is preferably used in an amount of 0.02 to 1.0 times in the case of activated carbon and 2 to 100 times in the case of a reverse phase carrier with respect to the weight of roasted coffee beans. As the activated carbon, the average pore radius in the micropore region is preferably 5 angstroms (Å) or less, more preferably in the range of 2 to 5 angstroms, and particularly preferably in the range of 3 to 5 angstroms. The average pore diameter in the micropore region in the present invention is the MP method described in the literature (Colloid and Interface Sc., 26, 46 (1968)) (a method adopted at Sumika Chemical Analysis Center, Toray Research Center) Can be measured. Moreover, as a kind of activated carbon, coconut shell activated carbon is preferable, and also water vapor activated coconut shell activated carbon is preferable. As a commercial product of activated carbon, Shirakaba WH ₂ c (Nippon Enviro Chemicals), Taiko CW (Nikamura Chemical), Kuraray Coal GW (Kuraray Chemical) and the like can be used. Examples of the reverse phase carrier include YMC • ODS-A (YMC) and C18 (GL Science).
Among these adsorbent treatment methods, the adsorbent treatment method using activated carbon can not only selectively reduce the hydroxyhydroquinone content without lowering the amount of chlorogenic acids, but is also industrially advantageous. It is also preferable from the viewpoint of not reducing the potassium content (maintaining 1/5 or more, particularly 1/2 or more in mass ratio).

  The amount of hydroxyhydroquinone in the coffee beverage composition or soluble coffee composition of the present invention is such that the relative retention time for gallic acid is 0.54 to 0.61 when gallic acid is used as a standard substance by high performance liquid chromatography. It can be detected as a peak in the time domain. Therefore, the coffee beverage composition of the present invention is a coffee beverage composition containing 0.01 to 1% by mass of chlorogenic acids, and gallic acid when gallic acid is used as a standard substance in analysis by high performance liquid chromatography. It can be defined as a coffee beverage composition characterized by having substantially no peak in the time range of 0.54 to 0.61 relative retention time. The soluble coffee composition of the present invention is a soluble coffee composition containing 0.1 to 10% by mass of chlorogenic acids, and in the analysis by high performance liquid chromatography, gallic acid when gallic acid is used as a standard substance. It can be defined as a soluble coffee composition characterized by having substantially no peak in the time range of 0.54 to 0.61 relative retention time. Incidentally, the analysis conditions of the high performance liquid chromatography in this rule are based on the analysis conditions B described later.

  The coffee composition of the present invention has substantially no peak in the time region where the relative retention time with respect to gallic acid is 0.54 to 0.61 when gallic acid is used as a standard substance in the analysis by high performance liquid chromatography. In order to confirm this, general HPLC can be used, for example, using a gradient of 0.05 M acetic acid aqueous solution and 0.05 M acetic acid 100% acetonitrile solution as an eluent, and using an ODS column, UV absorption spectrophotometry This can be confirmed by detecting with a meter or the like.

  In the present invention, the fact that the relative retention time with respect to gallic acid does not substantially have a peak in the time range of 0.54 to 0.61 means that the area value at the time of analysis of a 1 ppm solution of gallic acid is S1, and coffee under the same conditions. When the sum of the peak areas derived from the components eluted in the specific region when the beverage composition is analyzed is S2, it means that S2 / S1 <0.01.

  If desired, sugar composition such as sucrose, glucose, fructose, xylose, fructose glucose solution, sugar alcohol, milk components, antioxidant, pH adjuster, emulsifier, fragrance, etc. are added to the coffee beverage composition of the present invention. be able to. Examples of the milk component include raw milk, cow milk, whole milk powder, skim milk powder, fresh cream, concentrated milk, skim milk, partially skimmed milk, and milk. The pH of the coffee beverage composition of the present invention is preferably 3 to 7.5, more preferably 4 to 7, and particularly preferably 5 to 7 in terms of beverage stability.

  The soluble coffee composition is a powdered food such as powdered instant coffee powder. Instant coffee powder can be manufactured according to a conventional method. For example, spraying coffee extract from a nozzle and dropping it into hot air at about 210 to 310 ° C. to form a porous, water-soluble coffee powder (spray drying); or the coffee extract in liquid nitrogen or freezer It is possible to obtain a dry powder by freeze drying (freeze drying) or the like by freezing with, etc., pulverizing, sieving and then sublimating the moisture in a vacuum to bring the moisture to 3% or less.

The coffee beverage composition or soluble coffee of the present invention can be packed into containers such as PET bottles, cans (aluminum, steel), paper, retort pouches, bottles (glass) and the like to form a container-packed beverage. In this case, the coffee beverage composition of the present invention can be packed as it is into a 50 to 2500 mL container-packed beverage. The pH of the packaged beverage is preferably 5 to 7.5, and particularly preferably 5.4 to 7. As a constituent ratio of monocaffeoylquinic acid in the packaged beverage, a mass ratio of 4-caffeoylquinic acid / 3-caffeoylquinic acid is 0.6 to 1.2, and 5-caffeoylquinic acid / 3. -It is preferable that the mass ratio of caffeoylquinic acid is 0.01 to 3. The container is preferably an oxygen-impermeable container from the viewpoint of preventing changes in the ingredients in the coffee. For example, aluminum or steel cans, glass bottles, or the like may be used. In the case of cans and bottles, resealable ones that can be recapped are also included. Here, the oxygen non-permeability means that the oxygen permeability (cc · mm / m ² · day · atm) measured in an environment of 20 ° C. and 50% relative humidity is 5 or less, and further 3 or less. In particular, 1 or less is more preferable.
Moreover, the soluble coffee of the present invention can be taken by dissolving in 25 to 500 mL of water or hot water per 1 g.

  When a beverage is packaged, it is normally sterilized, but if the sterilization can be heat sterilized after filling the container like a metal can, it is performed under the sterilization conditions stipulated in the Food Sanitation Law. . For items such as PET bottles and paper containers that cannot be sterilized by retort, sterilization conditions equivalent to those stipulated in the Food Sanitation Law in advance, such as high-temperature and short-time sterilization using a plate heat exchanger, are cooled to a certain temperature. A method such as filling the container is adopted. In addition, after sterilization under heat, the pH may be returned to neutral under aseptic conditions, or after sterilization under heat under neutral conditions, the pH may be returned to acidity under aseptic conditions.

  The coffee beverage composition and soluble coffee beverage composition of the present invention contain an effective amount of chlorogenic acids having an antihypertensive effect, and the amount of hydroxyhydroquinone that inhibits the antihypertensive effect of chlorogenic acids is reduced. Therefore, it is useful as a blood pressure lowering or blood pressure increase suppressing pharmaceutical composition, a blood pressure lowering beverage, and a blood pressure increase suppressing beverage. It is also useful as a beverage with a display indicating that it is used to lower blood pressure or to suppress an increase in blood pressure, or a beverage with a higher blood pressure.

Example 1
(A) The coffee beverage composition of the present invention was produced as follows. 2.5 g of instant coffee (Nescafe caffeine-less) was applied to a column packed with 500 g of ODS filler (octadecylsilylated silica gel) (YMC GEL ODS-A pore size 6 nm, particle size 150 μm), and 0.5 L of acetic acid 6 L Then, the fraction containing hydroxyhydroquinone was eluted, and the fraction containing chlorogenic acids and other components was eluted with 6 L of methanol. Fraction A containing chlorogenic acids and other components was completely free of methanol by lyophilization. 0.933 g of fraction A was obtained from 2.5 g of instant coffee.

(B) The analysis method of chlorogenic acids and hydroxyhydroquinone in the coffee beverage composition is as follows. The following analysis conditions are set as analysis condition A. The analytical instrument used was HPLC (Shimadzu Corporation). The model numbers of the unit units are as follows. Detector: SPD-M10A, Oven: CTO-10AC, Pump: LC-10AD, Autosampler: SIL-10AD, Column: Inertsil OD
S-2 Inner diameter 4.6 mm × length 250 mm.
The analysis conditions are as follows. Sample injection volume: 10 μL, flow rate: 1.0 mL / min, ultraviolet absorption photometer detection wavelength: 325 nm (chlorogenic acids), 290 nm (hydroxyhydroquinone), eluent A: 0.05 M acetic acid 3% acetonitrile solution, eluent B: 0.05M acetic acid 100% acetonitrile solution

Concentration gradient condition Time Eluent A Eluent B
0 minutes 100% 0%
20 minutes 80% 20%
35 minutes 80% 20%
45 minutes 0% 100%
60 minutes 0% 100%
70 minutes 100% 0%
120 minutes 100% 0%

Retention time of chlorogenic acids (unit: minutes) (A ¹ ) Monocaffeoylquinic acid: 17.9, 20.4, 22.0, 3 points in total (A ² ) Ferlaquinic acid: 22.8, 25.8, 27.0 total 3 points (A ³ ) dicaffeoylquinic acid: 32.3, 33.0, 35.8 total 3 points From the area determined here, 5-caffeoylquinic acid is the standard substance, and the mass %.
Hydroxyquinone retention time: 5.5 minutes. From the area determined here, hydroxyhydroquinone was used as a standard substance, and mass% was determined.

  Further, hydroxyhydroquinone in the coffee composition can be measured by the following analytical method. The following analysis conditions are set as analysis condition B. The analytical instrument was HPLC (Hitachi, Ltd.). The model numbers of the unit units are as follows. Detector: L-7455, Oven: L-7300, Pump: L-7100, Autosampler: L-7200, Column: Inertsil ODS-2 Inner diameter 4.6 mm × Length 250 mm.

  The analysis conditions are as follows. Sample injection volume: 10 μL, flow rate: 1.0 mL / min, ultraviolet absorption photometer detection wavelength: 258 or 288 nm, eluent A: 0.05 M acetic acid aqueous solution, eluent B: 0.05 M acetic acid 100% acetonitrile solution

Concentration gradient condition Time Eluent A Eluent B
0 minutes 100% 0%
15 minutes 100% 0%
15.1 min 0% 100%
25 minutes 0% 100%
25.1 minutes 100% 0%
30 minutes 100% 0%

  Retention time of hydroxyhydroquinone: 6.8 minutes. From the area determined here, mass% was determined using hydroxyhydroquinone as a standard substance. The retention time of gallic acid measured in the same manner was 11.5 minutes.

  The total chlorogenic acid amount and hydroxyhydroquinone amount of instant coffee and fraction A produced in Example 1 (a) are shown in Table 1.

  In addition, when the amount of hydrogen peroxide in the coffee beverage composition of the present invention was measured using a highly sensitive hydrogen peroxide meter, the amount of hydrogen peroxide was below the detection limit and was not detected. The analysis method of hydrogen peroxide is as follows. The measurement was performed with a high-sensitivity hydrogen peroxide meter SUPER ORITECTOR MODEL 5 (Central Science Co., Ltd.). 2 mL of the sample was precisely weighed with a whole pipette and injected into the reaction cell of the apparatus main body. After sealing the reaction cell, the measurement range was selected and the measurement switch was pushed to start the measurement. After confirming the beep sound informing that measurement preparation was complete, 20 μL of the catalase for the protector was quickly injected with a microsyringe, and the output value was read.

The apparatus was calibrated with hydrogen peroxide standard solutions of 0.1, 1, and 5 mg / L.
The hydrogen peroxide standard solution was prepared by diluting hydrogen peroxide (30% aqueous solution, special grade, Wako Pure Chemical Industries, Ltd.) with ion-exchanged water to 1,000 mg / L as a stock solution. The stock solution was diluted with an extraction solution to prepare a hydrogen peroxide standard solution of 5 mg / L. Further, a 5 mg / L hydrogen peroxide standard solution was diluted with an extraction solution to prepare 1 mg / L and 0.1 mg / L.

  Extraction solution (0.2M phosphate buffer containing 0.5% potassium bromate, pH 7.0) is 11.0 g of potassium dihydrogen phosphate (special grade), disodium hydrogen phosphate dodecahydrate (special grade) 44.8 g and potassium bromate (special grade) 5.0 g were dissolved in ion-exchanged water, and the volume was adjusted to 1 L. At the time of use, nitrogen gas was aerated for 1 hour or more in advance under ice cooling.

Example 2
Blood pressure lowering evaluation i) Experimental materials and methods (a) A non-invasive blood pressure measuring device for rats (manufactured by Softron Co., Ltd.) commercially available for 12 consecutive weeks on male spontaneously hypertensive rats (SHR) for 5 weeks. The blood pressure measurement was used to make the rat sufficiently accustomed to blood pressure manipulation, and then the evaluation test was measured. All rats were housed under conditions of 25 ± 1 ° C., 55 ± 10% relative humidity, and 12 hours of illumination (7 am to 7 pm) (rat room breeding room).

(B) Administration method and dose: In the test group, fraction A obtained by removing hydroxyhydroquinone from instant coffee was used as the administration material. The control group used instant coffee. Fraction A instant coffees were each dissolved in physiological saline to prepare a total chlorogenic acid amount of 200 mg / kg. The administration method was oral administration using an oral sonde. The dose was 5 mL / animal.

(C) Test method: 3-6 SHRs were used per group. The systolic blood pressure of the tail vein before and 12 hours after oral administration was measured, and the blood pressure change rate after 12 hours was calculated from the blood pressure before administration.

(D) Statistical processing method: The measurement results obtained were subjected to Student's t-test representing the mean value and standard error, and the significance level was 5%.

ii) Results As can be seen from Table 2, by taking the coffee beverage composition of the present invention, a significant decrease in blood pressure was recognized as compared with the case of taking ordinary instant coffee.

Example 3
Blood pressure drop evaluation i) Experimental materials and methods (a) 12 weeks old male spontaneously hypertensive rats (SHR) were preliminarily raised in the same manner as in Example 2.

(B) Administration method and dose: In the control group, physiological saline was orally administered. In the comparative group, a green coffee bean extract (flavor holder FH1041: manufactured by Hasegawa Fragrance Co., Ltd.) containing chlorogenic acid as a main component was used. The dose was prepared so that the total amount of chlorogenic acid was 300 mg / kg. In test group 1, FH1041 was prepared so that the total amount of chlorogenic acid was 300 mg / kg, and hydroxyhydroquinone was 0.03 mg / kg (0.01% with respect to the total chlorogenic acid amount). In test group 2, FH1041 is 300 mg / kg as the total amount of chlorogenic acid, hydroxyhydroquinone is 0.3 mg / kg (0.1% with respect to the total chlorogenic acid amount), and in test group 3, FH1041 is the total amount of chlorogenic acid. As a dose of 300 mg / kg and hydroxyhydroquinone of 3 mg / kg (1% with respect to the total amount of chlorogenic acid). The administration method was oral administration using an oral sonde. The dose was 5 mL / animal.

(C) Test method: Three SHRs were used per group. The systolic blood pressure of the tail vein before and 12 hours after oral administration was measured, and the blood pressure change rate after 12 hours was calculated from the blood pressure before administration.

(D) Statistical processing method; the obtained measurement results were expressed as an average value and standard error, and subjected to a multigroup test (Scheffe), and the significance level was set to 5%.
ii) Results As can be seen from Table 3, the addition of hydroxyhydroquinone to chlorogenic acid inhibited the blood pressure drop of chlorogenic acid.

Example 4
(Production of canned coffee using fraction A obtained in Example 1)
Fraction A 0.75g was melt | dissolved in 140 mL water, and after filling and winding up a can, retort sterilization (at 121 degreeC for 10 minutes) was performed, and canned coffee was obtained.

Example 5
(Production of powdered coffee using fraction A obtained in Example 1)
Fraction A was pulverized to obtain a powdered coffee.

Example 6
The coffee beverage composition of the present invention was also produced by the following method.
Production of activated carbon-treated coffee After dissolving 20 g of commercial instant coffee (Nescafe Gold Blend Red Label) in 1400 mL of distilled water (this coffee is referred to as coffee P), activated carbon white rice WH ₂ c 28/42 (average pore size 4.2 angstrom) , Nippon Envirochemicals) was added and stirred for 1 hour, followed by filtration using a membrane filter (0.45 μm) to obtain a filtrate (this coffee is referred to as coffee Q). The obtained filtrate was freeze-dried to obtain 15.8 g of a brown powder. This brown powder was dissolved in distilled water, and chlorogenic acid and HHQ were quantified by HPLC analysis in the same manner as in Example 1. As a result, 4.12% by mass of chlorogenic acid was contained, and HHQ was below the detection limit (analysis). (Condition B). Moreover, when the potassium content was measured by ICP emission spectroscopic analysis, both the raw instant coffee and the activated carbon-treated coffee were about 4.2% by mass. When the coffee P, coffee Q, and gallic acid were analyzed using HPLC, the charts shown in FIGS. 1 and 2 were obtained. In coffee Q, the peak at a retention time of about 6.8 minutes disappears, and substantially no peak is present. In FIG. 1, a is a coffee P chart, b is a coffee Q chart, and c is a garlic acid chart. In FIG. 2, b is a chart of coffee P, c is a chart of coffee Q, and a is a chart of garlic acid.
The amount of hydroxyhydroquinone (HHQ) in the coffee beverage composition of the present invention was also measured by the following method.

Measurement of Hydroxyhydroquinone The analysis method of hydroxyhydroquinone in the coffee beverage composition is as follows. The analytical instrument used was a Couloarray system (model 5600A, development / manufacturing: ESA, USA, import / sales: MC Medical Co., Ltd.) which is an HPLC-electrochemical detector (coulometric type). The names and model numbers of the constituent units of the apparatus are as follows.
Analytical Cell: Model 5010, Couloarray Organizer, Couloarray Electronics Module / Software: Model 5600A, Solvent Delivery Module: Model 582, Gradient Mixer, Autosampler: Model 542, Pulse Damper, Degasser: Degasys Ultimate DU3003, Column Oven : 505. Column: CAPCELL PAK C18 AQ inner diameter 4.6 mm × length 250 mm Particle diameter 5 μm (Shiseido Co., Ltd.).
The analysis conditions are as follows.
Sample injection volume: 10 μL, flow rate: 1.0 mL / min, applied voltage of electrochemical detector: 0 mV, column oven set temperature: 40 ° C., eluent A: 0.1 (W / V)% phosphoric acid, 0. 1 mM 1-hydroxyethane-1,1-diphosphonic acid, 5 (V / V)% methanol solution, eluent B: 0.1 (W / V)% phosphoric acid, 0.1 mM 1-hydroxyethane-1,1 -Diphosphonic acid, 50 (V / V)% methanol solution.

  Eluents A and B were prepared by using distilled water for high performance liquid chromatography (Kanto Chemical Co., Ltd.), methanol for high performance liquid chromatography (Kanto Chemical Co., Ltd.), phosphoric acid (special grade, Wako Pure Chemical Industries, Ltd.) )), 1-hydroxyethane-1,1-diphosphonic acid (60% aqueous solution, Tokyo Chemical Industry Co., Ltd.).

Concentration gradient condition Time Eluent A Eluent B
0.0 minutes 100% 0%
10.0 minutes 100% 0%
10.1 min 0% 100%
20.0 minutes 0% 100%
20.1 minutes 100% 0%
50.0 minutes 100% 0%

  The analytical sample was prepared by accurately weighing 2 g of the sample, measuring up to 10 mL with Eluent A, and membrane filter (HLC-DISK25 solvent system, pore size 0.45 μm, for high performance liquid chromatography, Kanto Chemical Co., Inc.) And filtered. About 2.5 mL of the obtained filtrate was passed through Bond Elut SCX (solid phase filling amount: 500 mg, reservoir volume: 3 mL, GL Sciences Inc.), and the first passing solution was removed from about 0.5 mL. Were immediately subjected to analysis.

In the analysis under the above conditions, the retention time of hydroxyhydroquinone was 6.38 minutes. From the obtained peak area value, mass% was determined using hydroxyhydroquinone (Wako Pure Chemical Industries, Ltd.) as a standard substance.
In addition, when the amount of hydrogen peroxide in the coffee beverage composition of the present invention was measured using a highly sensitive hydrogen peroxide meter, the amount of hydrogen peroxide was below the detection limit and was not detected. Moreover, when the ash content of coffee P was measured by the above-described measurement method, it was 186 mg / 100 g in terms of the amount per 100 g of coffee drink, and the ash content of coffee Q was 176 mg / 100 g.

Example 7
After dissolving 20 g of commercial instant coffee (Nescafe Gold Blend Red Label) in 1400 mL of distilled water (this coffee is called Coffee P), 10 g of activated carbon Kuraray Coal GW-H 48/100 (average pore diameter 3.9 angstrom) is added. After stirring for 1 hour, the mixture was filtered using a membrane filter (0.45 μm) to obtain a filtrate (this coffee is referred to as coffee Q). The obtained filtrate was freeze-dried to obtain 16.5 g of a brown powder. This brown powder was dissolved in distilled water, and chlorogenic acid and HHQ were quantified by HPLC analysis in the same manner as in Example 1. As a result, 4.31% by mass of chlorogenic acid was contained, and HHQ was below the detection limit (analysis). (Condition B). Moreover, when the potassium content was measured by ICP emission spectroscopic analysis, both the raw instant coffee and the activated carbon-treated coffee were about 4.2% by mass.

Example 8
Blood pressure drop evaluation of coffee beverage composition prepared in Example 6 Experimental materials and methods (a) 13-14 weeks old spontaneously hypertensive rats (SHR) preliminarily commercially available for 5 consecutive days for rats The blood pressure measurement was carried out by using a blood pressure measuring apparatus (manufactured by Softron Co., Ltd.) to sufficiently familiarize the rat with the blood pressure operation, and then the evaluation test was measured. All rats were housed under conditions of 25 ± 1 ° C., 55 ± 10% relative humidity, and 12 hours of illumination (7 am to 7 pm) (rat room breeding room).
(B) Administration method and dose: In the test group, the coffee beverage composition (activated carbon coffee) prepared in Example 6 was used. The control group used commercial instant coffee. Activated charcoal-treated coffee and instant coffee were each dissolved in physiological saline to prepare a total chlorogenic acid amount of 200 mg / kg. The administration method was oral administration using an oral sonde. The dose was 5 mL / kg.
(C) Test method: 4 to 6 SHRs were used per group. The systolic blood pressure of the tail vein before and 12 hours after oral administration was measured, and the blood pressure change rate after 12 hours was calculated from the blood pressure before administration.
(D) Statistical processing method: The measurement results obtained were subjected to Student's t-test representing the mean value and standard error, and the significance level was 5%.
Results: As is apparent from Table 4, when the coffee beverage composition of the present invention was ingested, a significant decrease in blood pressure was observed as compared with the case of ingesting ordinary instant coffee.

Blood pressure drop evaluation of the coffee beverage composition prepared in Example 6 (blood pressure rise inhibition evaluation in rats)
Experimental materials and methods (a) Animals used: 6-week-old male spontaneously hypertensive rats (SHR) were preliminarily used for 7 consecutive days using a commercially available non-invasive blood pressure measuring device for rats (manufactured by Softron). By making blood pressure measurement, the rat was fully accustomed to blood pressure measurement operation, and then the evaluation test was started. All rats were housed under the conditions of 25 ± 1 ° C., 55 ± 10% humidity, and 12 hours of illumination (7 am to 7 pm) (rat room breeding room).
(B) Administration method and dose: Test groups 1 and 2 and a control group were prepared. The administration method was oral administration, and it was forcibly administered using a metal gastric sonde. The dose was 10 mL / kg / day and was administered for 5 weeks a week for 4 weeks.
(C) Test method: Seven to nine-week-old SHR was used in a group of 6-9 animals, and the systolic blood pressure of the tail artery was measured every week before and 7 weeks after the start of the test.
(D) Statistical processing method: The obtained test results were expressed as an average value and standard error and subjected to Student's t-test, and the significance level was set to 5% or less.
Results: The graph shows systolic blood pressure (SBP) before and 7 weeks after the start of the test. As is clear from FIG. 3, test group 2 which is HHQ-removed coffee in the control group and compared with test group 1 significantly suppressed an increase in blood pressure.

A sample for blood pressure lowering evaluation was produced as follows and subjected to a blood pressure lowering test.
Placebo (P): After adding 400 g of medium roast (L = 22) and ground (medium ground) Decaf Colombia beans to a general extractor, add 95 ° C. hot water to obtain 3200 g of extract. Ion-exchanged water and sodium bicarbonate are added to the extract so that the pH is 6.3 to obtain a preparation liquid. The preparation liquid is filled in a 190 g metal can and sealed, and then subjected to retort sterilization at 118.1 ° C. for 10 minutes. A test drink for placebo was obtained. The pH after sterilization was 5.8.
Sample (S): After adding 400 g of medium roast (L = 22) and ground (meat ground) Decaf Colombia beans to a general extractor, add 95 ° C. hot water to obtain 3200 g of extract. 50% (w / w) of activated carbon WH ₂ c (manufactured by Nippon Enviro Chemical Co., Ltd.) is added to the solid content of the extract, stirred for 30 minutes, centrifuged to remove the activated carbon, and de-HHQ coffee extract Get. Ion exchange water and baking soda are added to the de-HHQ coffee extract so as to have a pH of 6.3 to obtain a mixed solution. The prepared solution was filled in a 190 g metal can and sealed, and then subjected to retort sterilization at 118.1 ° C. for 10 minutes to obtain a sample test beverage. The pH after sterilization was 5.8.
(Health blood pressure reduction test)
Test beverage (1 can 190mL)
(P) Placebo chlorogenic acid 433 mg / can caffeine 194 mg / can HHQ 3.0 ppm
(S) Sample Chlorogenic acid 448 mg / can Caffeine 142 mg / can HHQ 0.1 ppm or less Test method Evaluation of blood pressure lowering performance using HHQ-removed coffee drinks by 9 males aged 30 to 40 years by crossover test every 4 weeks did.
1) Two types of canned coffee beverages (S) from which HHQ was removed by activated carbon treatment and normal canned coffee (P) were prepared and confirmed to be equivalent in flavor. Keeping the blinds about the contents, 1 bottle (190 mL) every day under the condition of drinking when you like, (P) for 4 weeks, (S) for 4 weeks, drinking continuously for a total drinking period of 8 weeks did.
2) Blood pressure measurement An OMRON blood pressure monitor was used for blood pressure measurement. Blood pressure measurement was carried out after a 10-minute rest before blood pressure measurement at a regular time zone every week for 4 weeks after starting drinking and for 4 weeks after drinking. The average blood pressure value before the test was 138 mmHg (systole). During the test period, other coffee drinks were prohibited.
FIG. 4 shows the systolic blood pressure drop after drinking, and FIG. 5 shows the antihypertensive blood pressure drop. The HHQ-removed coffee beverage of the present invention showed a blood pressure lowering effect.

Example 9
2 g of the activated carbon-treated coffee obtained in Example 6 was dissolved in 140 mL of water, filled into cans and tightened, and then subjected to retort sterilization (at 121 ° C. for 10 minutes) to obtain canned coffee.

Example 10
The freeze-dried product obtained in Example 6 was directly used as powdered coffee.
Examples 11-13
Manufacture of coffee extract and manufacture of beverages and evaluation of drinking In a multi-stage extractor, 120 ° C hot water is added to roasted (medium roast, L = 22) and ground Guatemala coffee beans and cooled, then coffee extract (Extract) was obtained. 30% of solids were collected with respect to the amount of charged beans. 50% (w / w) of activated carbon WH ₂ c (manufactured by Nippon Enviro Chemical Co., Ltd.) is added to the solid content of the resulting extract, and after stirring for 30 minutes, the activated carbon is removed by centrifugal filtration to remove HHQ coffee. An extract was obtained. Next, ion-exchanged water and sodium bicarbonate are added to the extract so as to have a pH of 6.3 to obtain a preparation liquid. The preparation liquid is heated to 85 ° C. and then filled into a 190 g capacity metal can, and the head space is filled with N 2 gas. After the replacement, the product was wrapped and sealed, and the resulting sealed container was sterilized by retort at 118.1 ° C. for 10 minutes to obtain a packaged beverage. The pH after sterilization was 5.8. Table 5 shows the analytical values and evaluations of the obtained container-packed beverages.

It is a figure which shows the HPLC chart (detection wavelength 258nm) of Coffee Q. It is a figure which shows the HPLC chart (detection wavelength 288nm) of Coffee Q. It is a figure which shows the blood pressure lowering effect | action of the chlorogenic acid removal coffee drink composition (HHQ (-) C) by the continuous administration with respect to SHR. HHQ (+) C is a chlorogenic acid non-removed coffee administration group. It is a figure which shows the blood pressure lowering effect (systolic blood pressure) of the chlorogenic acid removal coffee drink composition (Sample) with respect to a human. It is a figure which shows the blood pressure lowering effect (diastolic blood pressure) of the chlorogenic acid removal coffee drink composition (Sample) with respect to a human.

Claims (17)

The following components (A) and (B),
(A) Chlorogenic acids 0.01-1% by mass,
(B) Hydroxyquinone A coffee beverage composition containing less than 0.1% by mass of the amount of chlorogenic acids.   A coffee beverage composition containing 0.01 to 1% by mass of chlorogenic acids and having a relative retention time of 0.54 to 0. 0 relative to gallic acid when gallic acid is used as a standard substance in analysis by high performance liquid chromatography. A coffee beverage composition characterized by having substantially no peak in the 61 time region.   The coffee beverage composition according to claim 1 or 2, which is a composition for improving hypertension.   3. The coffee beverage composition according to claim 1 or 2, characterized by having an effect of improving hypertension and labeled to be used for improving hypertension.   The coffee beverage composition according to claim 1 or 2, wherein the blood pressure is indicated as higher. The following components (A) and (B),
(A) Chlorogenic acids 0.1 to 10% by mass,
(B) Hydrohydroquinone A soluble coffee composition containing less than 0.1% by mass of the amount of chlorogenic acids.   It is a soluble coffee composition containing 0.1 to 10% by mass of chlorogenic acids, and the relative retention time with respect to gallic acid is 0.54 to 0. A soluble coffee composition characterized by having substantially no peak in the 61 time region.   The soluble coffee composition according to claim 6 or 7, which is a composition for improving hypertension.   The soluble coffee composition according to claim 6 or 7, characterized by having an effect of improving hypertension and labeled to be used for lowering blood pressure.   The soluble coffee composition according to claim 6 or 7, wherein the blood pressure is indicated as higher. The following components (A) and (B),
(A) Chlorogenic acids 0.01-1% by mass,
(B) Hydroxyquinone A packaged beverage filled with a coffee beverage composition containing less than 0.1% by mass of chlorogenic acids.   The container-packed drink according to claim 11, which is a composition for improving hypertension.   12. The packaged beverage according to claim 11, which has an effect of improving hypertension and is labeled as being for improving hypertension.   12. The packaged beverage according to claim 11, which is displayed as having a higher blood pressure.   A packaged beverage filled with the coffee beverage composition according to claim 2.   The packaged beverage according to any one of claims 11 to 15, which is a single strength.   The container-packed drink according to any one of claims 11 to 16, wherein the container is oxygen-impermeable.

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