U.S. patent application number 13/279407 was filed with the patent office on 2012-02-16 for package drink.
This patent application is currently assigned to KAO CORPORATION. Invention is credited to Kojirou Hashizume, Eiichi Hoshino, Naoki Hosoya, Masaki Iwasaki, Yoshikazu Ogura, Jun Saito, Norihiko Satake, Masami Shimizu, Yukiteru Sugiyama, Shinichiro TAKASHIMA, Hitoshi Takaya, Shinji Yamamoto.
Application Number | 20120040075 13/279407 |
Document ID | / |
Family ID | 34658069 |
Filed Date | 2012-02-16 |
United States Patent
Application |
20120040075 |
Kind Code |
A1 |
TAKASHIMA; Shinichiro ; et
al. |
February 16, 2012 |
PACKAGE DRINK
Abstract
To provide a packaged high-catechin beverage in which a
low-caffeine green tea extract is added. A packaged beverage
containing from 0.03 to 1.0 wt % of non-polymer catechins, in which
a low-caffeine green tea extract obtained by a method of brining a
green tea extract into contact with a 91/9 to 97/3 by weight
mixture of an organic solvent and water, activated carbon, and acid
clay or activated clay is added.
Inventors: |
TAKASHIMA; Shinichiro;
(Tokyo, JP) ; Iwasaki; Masaki; (Tokyo, JP)
; Hashizume; Kojirou; (Haga-gun, JP) ; Hosoya;
Naoki; (Tokyo, JP) ; Yamamoto; Shinji; (Tokyo,
JP) ; Ogura; Yoshikazu; (Tokyo, JP) ; Saito;
Jun; (Kamisu-shi, JP) ; Takaya; Hitoshi;
(Kamisu-shi, JP) ; Shimizu; Masami; (Tokyo,
JP) ; Satake; Norihiko; (Tokyo, JP) ; Hoshino;
Eiichi; (Tokyo, JP) ; Sugiyama; Yukiteru;
(Tokyo, JP) |
Assignee: |
KAO CORPORATION
Tokyo
JP
|
Family ID: |
34658069 |
Appl. No.: |
13/279407 |
Filed: |
October 24, 2011 |
Related U.S. Patent Documents
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Application
Number |
Filing Date |
Patent Number |
|
|
10581200 |
Jun 1, 2006 |
8088429 |
|
|
PCT/JP04/17875 |
Dec 1, 2004 |
|
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13279407 |
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Current U.S.
Class: |
426/597 ;
426/490 |
Current CPC
Class: |
A23F 3/385 20130101;
C07D 311/62 20130101; A61K 31/353 20130101; A23F 3/163
20130101 |
Class at
Publication: |
426/597 ;
426/490 |
International
Class: |
A23F 3/38 20060101
A23F003/38; A23F 3/20 20060101 A23F003/20; A23F 3/16 20060101
A23F003/16 |
Foreign Application Data
Date |
Code |
Application Number |
Dec 2, 2003 |
JP |
2003-402533 |
Dec 22, 2003 |
JP |
2003-424557 |
Feb 26, 2004 |
JP |
2004-050719 |
Oct 29, 2004 |
JP |
2004-316760 |
Claims
1. A low-caffeine green tea extract comprising from 40 to 90 wt %
of non-polymer catechins based on a solid content of said
low-caffeine green tea extract, and the weight ratio of the
non-polymer catechins to caffeine is from 25 to 200, and wherein
the weight ratio of said non-polymer catechins to (free amino
acids+proteins) is from 15 to 25.
2. The low-caffeine green tea extract according to claim 1, wherein
the weight ratio of said non-polymer catechins to (free amino
acids+proteins) is from 15 to 20.
3. The low-caffeine green tea extract according to claim 1, wherein
the content of gallates in the low-caffeine green tea extract is
from 45 to 98 wt % of said non-polymer catechins.
4. The low-caffeine green tea extract according to claim 2, wherein
the content of gallates in the low-caffeine green tea extract is
from 45 to 98 wt % of said non-polymer catechins.
5. A packaged beverage comprising the low-caffeine green tea
extract according to claim 1, wherein non-polymer catechins
dissolved in water are contained in an amount of from 0.03 to 1.0
wt %.
6. A packaged beverage comprising the low-caffeine green tea
extract according to claim 2, wherein non-polymer catechins
dissolved in water are contained in an amount of from 0.03 to 1.0
wt %.
7. A packaged beverage comprising the low-caffeine green tea
extract according to claim 3, wherein non-polymer catechins
dissolved in water are contained in an amount of from 0.03 to 1.0
wt %.
8. A packaged beverage comprising the low-caffeine green tea
extract according to claim 4, wherein non-polymer catechins
dissolved in water are contained in an amount of from 0.03 to 1.0
wt %.
9. The packaged beverage according to claim 5, which has a pH of
from 2 to 6.
10. The packaged beverage according to claim 6, which has a pH of
from 2 to 6.
11. The packaged beverage according to claim 7, which has a pH of
from 2 to 6.
12. The packaged beverage according to claim 8, which has a pH of
from 2 to 6.
13. The packaged beverage according to claim 9, further comprising
from 0.0001 to 20 wt % of a sweetener.
14. The packaged beverage according to claim 10, further comprising
from 0.0001 to 20 wt % of a sweetener.
15. The packaged beverage according to claim 11, further comprising
from 0.0001 to 20 wt % of a sweetener.
16. The packaged beverage according to claim 12, further comprising
from 0.0001 to 20 wt % of a sweetener.
17. The low-caffeine green tea extract according to claim 1, which
has been produced by a process comprising bringing a green tea
extract, a mixture comprising ethanol and water in a weight ratio
of ethanol/water of 91/9 to 97/3, activated carbon, and 2.5 to 25
weight parts of acid clay or activated clay based on 100 weight
parts of said mixture of ethanol and water into contact with one
another, wherein a weight ratio of activated carbon to acid clay or
activated clay is from 1 to 10 parts of acid clay or activated clay
to 1 part of activated carbon.
18. The low-caffeine green tea extract according to claim 3, which
has been produced by a process comprising bringing a green tea
extract, a mixture comprising ethanol and water in a weight ratio
of ethanol/water of 91/9 to 97/3, activated carbon, and 2.5 to 25
weight parts of acid clay or activated clay based on 100 weight
parts of said mixture of ethanol and water into contact with one
another, wherein a weight ratio of activated carbon to acid clay or
activated clay is from 1 to 10 parts of acid clay or activated clay
to 1 part of activated carbon.
19. A packaged beverage comprising the low-caffeine green tea
extract according to claim 17, wherein non-polymer catechins
dissolved in water are contained in an amount of from 0.03 to 1.0
wt %.
20. A packaged beverage comprising the low-caffeine green tea
extract according to claim 18, wherein non-polymer catechins
dissolved in water are contained in an amount of from 0.03 to 1.0
wt %.
Description
[0001] This is a divisional application of U.S. application Ser.
No. 10/581,200, filed Jun. 1, 2006, which is a 371 of
PCT/JP04/017875 filed on Dec. 1, 2004.
FIELD OF THE INVENTION
[0002] This invention relates to a packaged beverage in which a
low-caffeine green tea extract is added, and also to a process for
production of the low-caffeine green tea extract.
BACKGROUND OF THE INVENTION
[0003] Catechins are known to have a suppressing effect on increase
in cholesterol level and an inhibitory effect on .alpha.-amylase
activity (Patent Documents 1 to 2). To develop such physiological
effects of catechins, it is necessary for an adult to drink 4 to 5
cups of tea per day. Accordingly, there is a desire for technology
that permits addition of catechins at a high concentration to
beverages to facilitate ingestion of a large amount of catechins.
As one of the methods, catechins are added in a dissolved form to a
beverage by using a concentrate of green tea extract (Patent
Document 3) or the like.
[0004] As processes for extracting catechins with a stable taste
from green tea or semi-fermented or fermented tea leaves, there are
known a two-step extraction process in which extraction is
conducted with slightly warm water, and subsequent to heating,
extraction is conducted again and an extraction process under
strongly acidic conditions (Patent Documents 4-6). However, these
extraction processes are limited to the extraction of catechins
from tea leaves, and are intended to achieve only stabilization of
a taste of a purified product and maintenance of a good taste.
[0005] Further, catechins are generally known to be sparingly
soluble in organic solvents. It is also known that the extraction
of catechins can be promoted in a weakly acidic range. A high
proportion of an organic solvent, however, involves such a problem
that the efficiency of extraction of catechins is substantially
lowered (Patent Document 7).
[0006] In tea leaves, however, caffeine component is also contained
generally at from 2 to 4 wt % although catechins are contained in
an amount as much as about 15 wt %. As caffeine exhibits a central
stimulant effect, it is used for the suppression of sleepiness. On
the other hand, its excessive ingestion is considered to bring
about adverse effects such as nervosity, nausea and hyposomnia.
Investigations have, therefore, been made for processes that
selectively remove only caffeine from caffeine-containing
compositions.
[0007] Proposed is, for example, a process in which caffeine is
selectively removed by bringing a caffeine-containing, aqueous
solution into contact with activated clay or acid clay (Patent
Document 8). However, this process is accompanied by such a problem
that the color may be deteriorated in some instances, although
caffeine can be selectively removed by simply using activated clay
or acid clay.
[0008] [Patent Document 1] JP-A-60-156614
[0009] [Patent Document 2] JP-A-03-133928
[0010] [Patent Document 3] JP-A-59-219384
[0011] [Patent Document 4] JP-A-2003-219799
[0012] [Patent Document 5] JP-A-2003-219800
[0013] [Patent Document 6] JP-A-2003-225053
[0014] [Patent Document 7] JP-A-2004-147508
[0015] [Patent Document 8] JP-A-06-142405
[0016] The present invention provides a packaged beverage
containing from 0.03 to 1.0 wt % of non-polymer catechins, wherein
the packaged beverage contains a low-caffeine green tea extract
obtained by a method of bringing a green tea extract into contact
with a 91/9 to 97/3 by weight mixture of an organic solvent and
water (i.e. a mixture of an organic solvent and water at a weight
ratio of 91/9 to 97/3), activated carbon, and acid clay or
activated clay.
[0017] The present invention also provides a process for producing
a low-caffeine green tea extract containing from 25 to 90 wt % of
non-polymer catechins based on a dry weight of the extract, which
comprises bringing a green tea extract into contact with a 91/9 to
97/3 by weight mixture of an organic solvent and water, activated
carbon, and acid clay or activated clay.
[0018] The present invention further provides a low-caffeine green
tea extract, wherein the low-caffeine green tea extract contains
from 40 to 90 wt % of non-polymer catechins based on a solid
content of the low-caffeine green tea extract, and a weight ratio
of the non-polymer catechins to caffeine is from 25 to 200.
[0019] The present invention still further provides a process for
selectively removing caffeine from a caffeine-containing catechin
composition, which comprises dispersing a green tea extract in a
91/9 to 97/3 by weight mixture of an organic solvent and water and
bringing the resulting dispersion into contact with activated
carbon and acid clay or activated clay.
EMBODIMENTS OF THE INVENTION
[0020] The present invention relates to a method for selectively
removing caffeine from a green tea extract without significantly
changing the composition of catechins and moreover, without
deteriorating the color, and also to a low-caffeine green tea
extract produced by the method and a packaged beverage, especially
a packaged non-tea beverage in which the low-caffeine green tea
extract is added.
[0021] The present invention further relates to a process for
selectively removing caffeine from a green tea extract without
significantly changing the composition of catechins and moreover,
without deteriorating the color.
[0022] The present inventors have found that a low-caffeine green
tea extract can be obtained as a purified green tea extract, in
which caffeine has been selectively removed without significantly
changing the composition of catechins, and moreover, without
deteriorating the color, by bringing a green tea extract into
contact with a 91/9 to 97/3 by weight mixture of ethanol and water,
activated carbon, and acid clay or activated clay, and also that
the low-caffeine green tea extract provides high-catechin
beverages, especially packaged high-catechin non-tea beverages with
a good taste.
[0023] According to the present invention, it is possible to
selectively remove caffeine from a green tea extract without
significantly changing the compositions of catechins, and moreover,
without changing the color, and to efficiently extract non-polymer
catechins. In addition, the addition of the resulting low-caffeine
green tea extract enables obtention of a packaged beverage which is
low in caffeine content, contains catechins at a high
concentration, and is good in color and taste.
[0024] The green tea extract for use in the present invention
contains one or more non-polymer catechins. The term "non-polymer
catechins" as used herein is a generic term which collectively
encompasses non-epicatechins such as catechin, gallocatechin,
catechin gallate and gallocatechin gallate, and epicatechins such
as epicatechin, epigallocatechin, epicatechin gallate and
epigallocatechin gallate. On the other hand, the term "gallates" is
a generic term which collectively embraces catechin gallate,
gallocatechin gallate, epicatechin gallate and epigallocatechin
gallate among the above-described non-polymer catechins. Further,
the term "gallocatechins" is a generic term which collectively
encompasses gallocatechin, gallocatechin gallate, epigallocatechin
and epigallocatechin gallate among the above-described non-polymer
catechins. The term "gallocatechins percentage" means the weight
percentage of the gallocatechins in these non-polymer
catechins.
[0025] As green tea extracts usable in the present invention,
extracts obtained from tea leaves such as green tea, black tea and
oolong tea can be mentioned. In addition, mixtures of caffeine
derived from other caffeine-containing plants such as coffee with
tea extracts are also usable. Among such green tea extracts
containing non-polymer catechins, preferred are those obtained by
drying or concentrating extracts from green tea leaves.
[0026] Tea leaves for use in the present invention include, more
specifically tea leaves manufactured from tea leaves of the Genus
Camellia, for example, C. sinensis and C. assamica, and the
Yabukita variety or their hybrids. Such manufactured tea leaves
include green teas such as sencha (middle-grade green tea), bancha
(coarse green tea), gyokuro (shaded green tea), tencha (powdered
tea) and kamairicha (roasted tea).
[0027] A tea leaf extract can be obtained by a method such as
stirring extraction. An organic acid or organic acid salt such as
sodium ascorbate can be added beforehand to water upon extraction.
It is also possible to make combined use of boiling deaeration or
an extraction method which is conducted while flowing an inert gas
such as nitrogen gas to eliminate dissolved oxygen, that is, under
a so-called non-oxidizing atmosphere.
[0028] The extract obtained as described above is dried to provide
the green tea extract for use in the present invention. Forms of
the green tea extract include liquid, slurry, semi-solid and solid
forms. From the viewpoint of dispersibility in ethanol, a slurry,
semi-solid or solid form is preferred.
[0029] Instead of employing, as a green tea extract for use in the
present invention, a dried tea leaf extract, it is also possible to
employ a concentrate of a tea extract in a form dissolved in or
diluted with water or to employ an extract from tea leaves and a
concentrate of a tea extract in combination.
[0030] The term "the concentrate of a tea extract" as used herein
means a concentrate of an extract obtained from tea leaves with hot
water or a water-soluble organic solvent, and includes, for
example, those prepared by the processes disclosed in
JP-A-59-219384, JP-A-04-20589, JP-A-05-260907, JP-A-05-306279 and
the like.
[0031] As the green tea extract, it is possible to use specifically
a commercially-available crude solid catechin preparation such as
"Polyphenon" (product of Tokyo Food Techno Co., Ltd.), "TEAFURAN"
(product of ITO EN, LTD.) or "SUNPHENON" (product of Taiyo Kagaku
Co., Ltd.).
[0032] As the green tea extract, it is also possible to use an
extract obtained from tea leaves belonging to the Genus Camellia
and subjected beforehand to a treatment of contacting with carbon
dioxide in a supercritical state. The tea leaves for use in
supercritical extraction can be either raw tea leaves or
manufactured tea leaves insofar as they belong to the Genus
Camellia. As the manufactured tea leaves, non-fermented tea is more
preferred. Preferred examples of steamed tea leaves include sencha
(middle-grade green tea), fukamushicha (deep-steamed green tea),
gyokuro (shaded green tea), kabusecha (partially shaded green tea),
mushi-tamaryokucha (steamed, rounded, beads-shaped green tea),
andbancha (coarse green tea). Preferred examples of roasted tea
leaves, on the other hand, include kamairi-tamaryokucha (roasted,
rounded, beads-shaped green tea) and Chinese green tea. As
manufactured tea leaves, steamed tea leaves or dipped tea leaves
are preferred from the standpoint of avoiding generation of an
additional flavor and taste derived from tea leaves during
roasting.
[0033] In this method, an extract containing non-polymer catechins
is obtained from tea leaves available as a residue in the
supercritical extraction. There have conventionally been several
techniques for obtaining flavor components from tea leaves by
supercritical extraction (JP-A-2001-293076, JP-A-10-77496,
JP-A-06-133726, and JP-A-06-184591). Any of these techniques uses a
supercritical extract of tea leaves, however, and there is no
description as to a technique that makes use of residual tea leaves
after supercritical extraction or as to the components that remain
in the residual tea leaves.
[0034] A process for production of a tea extract from tea leaves,
which belong to the Genus Camillia and have been subjected to a
treatment to contact with carbon dioxide in its supercritical
state, includes specifically (A) a step of moistening green tea
leaves, (B) a step of treating the green tea leaves with carbon
dioxide in its supercritical state, and (C) a step of extracting a
green tea extract from the tea leaves. Each of these steps will
hereinafter be described.
[0035] In the step (A), from 0.2 to 0.4 weight part of a 75:25 to
99.5:0.5 mixture of ethanol and water is at first added to 1 weight
part of the green tea leaves to moisten the green tea leaves.
Without this moistening step of the green tea leaves with the 75:25
to 99.5:0.5 mixture of ethanol and water, elimination of a green
tea flavor in the step (B) cannot be achieved sufficiently. In view
of the effect of elimination of the green tea flavor and the
efficiency of extraction, it is preferred to add from 0.2 to 0.4
weight part of the 75:25 to 99.5:0.5 mixture of ethanol and water
to 1 weight part of the green tea leaves.
[0036] The ratio of ethanol to water in the mixture is preferably
from 75:25 to 99.5:0.5, more preferably from 80:20 to 99.5:0.5,
still more preferably from 80:20 to 90:10. The mixture of ethanol
and water is added in an amount of from 0.2 to 0.4 weight part,
preferably from 0.3 to 0.4 weight part.
[0037] The green tea leaves to which the above-described
predetermined amount of the mixture of ethanol and water has been
added is preferably left to stand at from 0 to 100.degree. C. for
0.5 hour or longer to have the green tea leaves moistened
sufficiently.
[0038] In the step (B), carbon dioxide in a supercritical state in
which a 75:25 to 99.5:0.5 mixture of ethanol and water has been
added is preferably brought into contact with the moistened green
tea leaves. According to the step (B), the water content of the
green tea leaves can be retained constant so that the green tea
flavor in the green tea leaves can be efficiently eliminated. On
the other hand, the catechins in the green tea remain substantially
completely in the green tea leaves, and are not impaired by the
above operation.
[0039] The ratio of ethanol to water in the mixture to be used is
preferably from 75:25 to 99.5:0.5, more preferably from 75:25 to
95:5, still more preferably from 80:20 to 90:10. The mixture of
ethanol and water is added in an amount of from 0.02 to 0.04 weight
part, preferably from 0.03 to 0.04 weight part per weight parts of
carbon dioxide.
[0040] As to the carbon dioxide to be used, elimination of green
tea flavor components can be efficiently achieved insofar as carbon
dioxide is in a supercritical state (pressure: 7 MPa or higher,
temperature: 31.degree. C. or higher). From the standpoints of the
efficiency of elimination of bitter components and green tea
flavor, however, carbon dioxide at from 20 to 50 MPa and at 35 to
100.degree. C., particularly at from 30 to 40 MPa and at 60 to
80.degree. C. is preferred. Carbon dioxide can be used in a
proportion of preferably 20 weight parts or more, more preferably
from 20 to 250 weight parts, still more preferably from 50 to 150
weight parts per weight part of the green tea leaves.
[0041] Ethanol and/or water and supercritical carbon dioxide is
brought into contact with the green tea leaves preferably at the
same time. For example, an aqueous ethanol solution and
supercritical carbon dioxide may be brought into contact with the
tea leaves at the same time, or an aqueous ethanol solution and
supercritical carbon dioxide maybe mixed together in advance, and
may then be brought into contact with the green tea leaves. To
bring ethanol and/or water and supercritical carbon dioxide into
contact with the green tea leaves, use of an ordinary supercritical
extraction apparatus is preferred. In general, the above-described
contact may be effected preferably at a feed rate of from 10 to 25
weight parts/hour of supercritical carbon dioxide per weight part
of green tea leaves to retain the water content of the green tea
leaves although the feed rate may vary depending on the capacity of
the apparatus.
[0042] In the step (C), it is preferred to conduct the extraction
from the green tea leaves which have been brought into contact with
the supercritical carbon dioxide by using from 10 to 150 weight
parts of water per weight part of the green tea leaves. To maximize
the efficiency of extraction of water-soluble components such as
catechins, water may be used preferably in an amount of from 20 to
100 weight parts, more preferably in an amount of from 20 to 50
weight parts.
[0043] The extraction in the step (C) can be conducted under usual
extraction conditions. Upon conducting the extraction from the
green tea leaves, the temperature can be changed as needed
depending on the kind of the tea leaves. The temperature is
preferably, for example, from 60 to 90.degree. C. in the case of
sencha (middle-grade green tea) or gyokurocha (shaded green tea),
or from 50 to 60.degree. C. in the case of gyokuro (shaded green
tea) or kabusecha (partially shaded green tea). In the case of
bancha (coarse tea), on the other hand, a temperature in a range of
from 90.degree. C. to boiling water can be used. The time of
extraction from the green tea leaves is preferably from 1 to 60
minutes, more preferably from 1 to 40 minutes, still more
preferably from 1 to 30 minutes. In the case of a process for
production of an extract from middle-grade sencha leaves, for
example, an extract can be obtained by adding the tea leaves into
ion-exchanged water heated at 65.degree. C., stirring them for 2
minutes or so, leaving them to stand for 2 minutes or so, filtering
out the green tea leaves, and then filtering out fragmented tea
leaves with a flannel filter cloth.
[0044] As the green tea extract for use in the present invention, a
green tea extract containing preferably from 25 to 90 wt %, more
preferably from 25 to 70 wt %, still more preferably from 40 to 70
wt % of non-polymer catechins on a dry weight basis can be used
preferably, because taste components other than the non-polymer
catechins still remain in the green tea extract.
[0045] By the method of bringing the resulting green tea extract
into contact with the 91/7 to 97/3 by weight mixture of the organic
solvent and water, activated carbon, and acid clay or activated
clay, the green tea extract is purified to give a low-caffeine
green tea extract.
[0046] As the organic solvent for use in the production of the
low-caffeine green tea extract in the present invention, ethanol,
methanol, acetone, ethyl acetate or the like can be mentioned.
Among these, a hydrophilic organic solvent such as methanol,
ethanol or acetone is preferred, with ethanol being more preferred
in view of the use of the low-caffeine green tea extract in
foods.
[0047] Concerning the organic solvent and water to be used in the
production of the low-caffeine green tea extract in the present
invention, it is preferred to adjust their weight ratio to a range
of preferably from 91/9 to 97/3, more preferably to from 92/8 to
96/4, still more preferably from 92/8 to 95/5. The above-mentioned
range is preferred from the standpoints of the extraction
efficiency of catechins, the purification and long-term
drinkability of the green tea extract, fractionation conditions for
the recovered organic solvent and the like.
[0048] In the present invention, it is preferred to conduct the
processing by adding from 10 to 40 weight parts, more preferably
from 10 to 30 weight parts, particularly preferably from 15 to 30
weight parts of the green tea extract (on a dry weight basis) to
100 weight parts of the mixture of the organic solvent and water
because the green tea extract can be processed efficiently.
[0049] No particular limitation is imposed on the activated carbon
to be used in the present invention insofar as it is generally used
on an industrial level. Usable examples include
commercially-available products such as "ZN-50" (product of
Hokuetsu Carbon Industry Co., Ltd.), "KURARAY COAL GLC", "KURARAY
COAL PK-D" and "KURARAY COAL PW-D" (products of Kuraray Chemical K.
K.), and "SHIROWASHI AW50", "SHIROWASHI A", "SHIROWASHI M" and
"SHIROWASHI C" (products of Takeda Pharmaceutical Company
Limited).
[0050] The pore volume of the activated carbon is preferably from
0.01 to 0.8 mL/g, more preferably from 0.1 to 0.7 mL/gm. The
activated carbon having a specific surface area in a range of from
800 to 1,300 m.sup.2/g, particularly from 900 to 1,200 m.sup.2/g is
preferred. It is to be noted that these physical values are those
determined by the nitrogen adsorption method.
[0051] The activated carbon can be added preferably in a proportion
of from 0.5 to 5 weight parts, particularly in a proportion of from
0.5 to 3 weight parts to 100 weight parts of the mixture of the
organic solvent and water, because such a proportion results in
high decaffeination efficiency and low cake resistance in the
filtration step.
[0052] Acid clay and activated clay for use in the present
invention both contain, as general chemical components, SiO.sub.2,
Al.sub.2O.sub.3, Fe.sub.2O.sub.3, CaO, MgO, etc., and those having
a SiO.sub.2/Al.sub.2O.sub.3 ratio of from 3 to 12, particularly
from 4 to 9 are preferred. Also preferred are those which contain
from 2 to 5 wt % of Fe.sub.2O.sub.3, from 0 to 1.5 wt % of CaO and
from 1 to 7 wt % of MgO.
[0053] Activated clay is obtained by treating a naturally-occurring
acid clay (montmorillonite clay) with a mineral acid such as
sulfuric acid, and is a compound having a porous structure of large
specific surface area and adsorbability. Further treatment of acid
clay with an acid is known to change its specific surface area so
that its decoloring ability is improved and its physical properties
are modified.
[0054] The specific surface area of acid clay or activated clay is
preferably from 50 to 350 m.sup.2/g although it varies depending on
the degree of the acid treatment or the like, and its pH (5 wt %
suspension) is preferably from 2.5 to 8, particularly from 3.6 to
7. Usable examples of acid clay include commercially-available
products such as "MIZUKA ACE #600" (product of Mizusawa Chemical
Industries, Ltd.).
[0055] The weight ratio of activated carbon to acid clay or
activated clay is appropriately from 1 to 10 of acid clay or
activated clay to 1 activated carbon, with the weight ratio of
activated carbon: acid clay or activated clay=1:1 to 1:6 being
preferred.
[0056] The process of the present invention for the production of
the low-caffeine green tea extract is preferably (a) a process in
which the green tea extract is dissolved in the mixture of the
organic solvent and water and is then brought into contact with
activated carbon and acid clay or activated clay, or (b) a process
in which a dispersion of activated carbon and acid clay or
activated clay in a mixture of the organic solvent and water, as
well as the green tea extract are subjected to a treatment for
contacting them with each other. It is to be noted that as the feed
green tea extract, one obtained by the above-described
supercritical extraction may also be used.
[0057] No particular limitation is imposed on the order of contact
among the green tea extract, activated carbon, and acid clay or
activated clay. Activated clay and acid clay or activated clay may
be brought into contact with each other at the same time, or the
green tea extract and acid clay or activated clay may first be
brought into contact with each other, followed by contact with
activated carbon.
[0058] For obtaining a purified green tea extract with non-polymer
catechins efficiently extracted therein, it is preferred to effect
the contact between the green tea extract and acid clay or
activated clay by adjusting the pH to a range of from 4 to 6. Upon
effecting the contact, an organic acid such as citric acid, lactic
acid, tartaric acid, succinic acid or malic acid is preferably
added at a weight ratio of the organic acid to the non-polymer
catechins (organic acid/non/polymer catechins) in a range of from
0.02 to 0.20.
[0059] When producing the low-caffeine green tea extract by
dispersing the green tea extract in the mixture of the organic acid
and water and then subjecting the resulting dispersion to a
treatment to contact it with activated carbon and acid clay or
activated clay, no particular limitation is imposed on the manner
of dissolution of the green tea extract in the mixture of the
organic solvent and water insofar as the weight ratio of the
organic solvent to water upon final treatment of the
caffeine-containing catechin composition is in the range of from
91/9 to 97/3. For example, the weight ratio of the organic solvent
to water may be brought into the range of from 91/9 to 97/3 by
gradually adding the organic solvent after dissolving the green tea
extract in water, or water may be gradually added to give a similar
ratio after suspending the green tea extract in the organic
solvent. From the standpoint of extraction efficiency, however, it
is preferred to gradually add the organic solvent subsequent to the
dissolution in water.
[0060] As to the time over which a required amount of water or the
organic solvent is added, it is preferred to slowly add dropwise
water or the organic solvent over a time of from approximately 10
to 30 minutes. To improve the efficiency of extraction of
catechins, it is also preferred to effect the dropwise addition
under stirring. It is more preferred to include an aging time of
from 10 to 120 minutes or so after the completion of the dropwise
addition of water.
[0061] These processing can be conducted at from 10 to 60.degree.
C., preferably from 10 to 50.degree. C., more preferably from 10 to
40.degree. C.
[0062] Acid clay or activated clay can be added preferably in a
proportion of from 2.5 to 25 weight parts, particularly in a
proportion of from 2.5 to 15 weight parts to 100 weight parts of
the mixture of the organic solvent and water. The addition of acid
clay or activated clay in an unduly small proportion leads to
deterioration in decaffeination efficiency, while the addition of
acid clay or activated clay in an excessively large proportion
leads to increase in the cake resistance in the filtration step. It
is, therefore, not preferred to add acid clay or activated clay in
a proportion outside the above-described range.
[0063] When mixing the green tea extract in contact with the
dispersion of acid clay or activated clay in the mixture of the
organic solvent and water in the present invention, the mixing
weight ratio of the acid clay or activated clay to the green tea
extract is preferably from 0.9 to 5.0, more preferably from 1.5 to
3.0 in terms of the acid clay or activated clay/non-polymer
catechins value. The addition of acid clay or activated clay in an
unduly small proportion leads to deterioration in decaffeination
efficiency, while the addition of acid clay or activated clay in an
excessively large proportion leads to increase in the cake
resistance in the filtration step. It is, therefore, not preferred
to add acid clay or activated clay at a ratio outside the
above-described range.
[0064] As to the temperature at which the dispersion is brought
into contact with the green tea extract, it is preferred at first
to set the temperature at from 10 to 30.degree. C. and then to
raise the temperature to from 40 to 60.degree. C. because
dissolution of the green tea extract can be promoted and the
efficiency of extraction of catechins into the dispersion can be
also promoted.
[0065] After the contact of the green tea extract with the
dispersion, the resulting mixture is further brought into contact
with activated carbon. Preferably, the green tea extract and the
dispersion is first mixed together to bring them into contact with
each other, and subsequent to filtration, the filtrate is then
subjected to a treatment to contact it with activated carbon.
[0066] The treatment of the green tea extract to contact it with
activated carbon and acid clay or activated clay can be conducted
by any method such as a batchwise treatment method or a continuous
treatment method making use of a column. As to a method for
bringing the green tea extract into contact with activated carbon,
the contact may be effected preferably by a continuous treatment
through a column packed with activated carbon. Adopted in general
is a method in which powdery activated carbon or the like is added,
the resulting mixture is stirred to selectively adsorb caffeine,
and subsequent to selective adsorption of caffeine by a filtering
operation, filtration is conducted to obtain a decaffeinated
filtrate, or a method in which caffeine is selectively adsorbed by
a continuous treatment using a column packed with granular
activated carbon or the like.
[0067] After the contact of the green tea extract with activated
carbon and acid clay or activated clay, distillation such as
reduced-pressure distillation is conducted to remove the organic
solvent such as ethanol from the mixture of the organic solvent and
water. The treated green tea extract can be either in a liquid form
or in a solid form. To prepare it into a solid form, it may be
formed into powder by a method such as freeze drying or spray
drying.
[0068] The purified green tea extract (low-caffeine green tea
extract), which has been subjected to the decaffeination treatment
according to the present invention, may preferably remain
substantially unchanged in the composition of the non-polymer
catechins containing therein compared with the composition before
the treatment. The yield of the non-polymer catechins in the
mixture of the organic solvent and water before and after the
treatment is preferably 60 wt % or more, more preferably 65 wt % or
more, still more preferably 70 wt % or more, particularly
preferably 80 wt % or more.
[0069] Further, the content of the gallates consisting of catechin
gallate, epicatechin gallate, gallocatechin gallate and
epigallocatechin gallate in the low-caffeine green tea extract is
preferably from 45 to 100 wt %, more preferably from 50 to 98 wt %
of the whole non-polymer catechins from the standpoint of the
effectiveness of physiological effects of the non-polymer
catechins.
[0070] The concentration of caffeine in the low-caffeine green tea
extract is preferably from 25 to 200, more preferably from 30 to
150, still more preferably from 30 to 100, particularly preferably
from 30 to 60 relative to the non-polymer catechins, that is, in
terms of the non-polymer catechins/caffeine.
[0071] In the solid content of the low-caffeine green tea extract,
the non-polymer catechins amount to preferably from 25 to 90 wt %,
more preferably from 30 to 90 wt %, still more preferably from 35
to 90 wt %.
[0072] In the solid content of the low-caffeine green tea extract,
free amino acids and proteins may also amount preferably to from 0
to 5.0 wt % in total. The weight ratio of the non-polymer catechins
to the total amount of the free acids and proteins (the non-polymer
catechins/ (the free amino acids+proteins) is preferably from 15 to
25.
[0073] The resulting low-caffeine green tea extract, despite its
low caffeine concentration, still contains non-polymer catechins at
a high concentration, has a good color, and further, is
substantially free of the flavor of green tea. Therefore, packaged
beverages in which the low-caffeine green tea extract is
incorporated are useful particularly as non-tea beverages such as
sports drinks and isotonic drinks.
[0074] The packaged beverage according to the present invention
contains non-polymer catechins (A) dissolved in water in an amount
of from 0.03 to 1.0 wt %, preferably from 0.04 to 0.5 wt %, more
preferably from 0.06 to 0.4 wt %, still more preferably from 0.07
to 0.4 wt %, particularly preferably from 0.08 to 0.3 wt %, even
more preferably from 0.09 to 0.3 wt %, still even more preferably
from 0.1 to 0.3 wt %. Insofar as the content of non-polymer
catechins falls within the above-described range, a great deal of
non-polymer catechins can be taken with ease, and from the
standpoint of the color tone of the beverage shortly after its
preparation, this content range is also preferred. The
concentration of the non-polymer catechins can be adjusted by the
amount of the green tea extract to be incorporated.
[0075] Further, the daily intake of green tea required for an adult
to exhibit the effects of the promotion of accumulated fat burning,
the promotion of dietary fat burning and the promotion of
.beta.-oxidation gene expression in the liver is preferably 300 mg
or more, more preferably 450 mg or more, still more preferably 500
mg or more in terms of non-polymer catechins. Specifically, it has
been confirmed that an anti-puffiness effect and/or visceral fat
reducing effect can be brought about by ingesting a beverage which
contains 483 mg, 555 mg or 900 mg of non-polymer catechins per
package (JP-A-2002-326932).
[0076] Therefore, the daily intake of the packaged beverage
according to the present invention for an adult can also be
preferably 300 mg or more, more preferably 450 mg or more, still
more preferably 500 mg or more in terms of non-polymer catechins.
From the standpoint of assuring the required daily intake amount,
the non-polymer catechins is contained in an amount of preferably
300 mg or more, more preferably 450 mg or more, still more
preferably 500 mg or more in the packaged beverage according to the
present invention.
[0077] The weight ratio of the non-polymer catechins to caffeine
contained in the packaged beverage according to the present
invention is preferably from 25 to 200, more preferably from 30 to
200, still more preferably from 30 to 150, particularly preferably
from 30 to 100.
[0078] The packaged beverage according to the present invention may
also contain sodium ions and/or potassium ions. Beverages of the
present invention containing such ions are useful in the form of
drinks such as sports drinks and isotonic drinks. The term "sports
drink" is generally defined to mean a drink that can promptly
replenish water and minerals lost in the form of sweat during
physical exercise.
[0079] Sodium and potassium can be mentioned as primary
physiological electrolytes. These ion ingredients can be
incorporated in their corresponding water-soluble ingredients or
inorganic salts. They are also found in fruit juices and tea
extracts. The amount of an electrolyte or ion ingredient in the
packaged beverage according to the present invention is its content
in the final packaged beverage ready for drinking. The
concentration of an electrolyte is expressed in terms of "ion
concentration". In the beverage according to the present invention,
a potassium ion ingredient can be added in the form of a salt such
as potassium chloride, potassium carbonate, potassium sulfate,
potassium acetate, potassium hydrogencarbonate, potassium citrate,
potassium phosphate, potassium hydrogenphosphate, potassium
tartrate, potassium sorbate or a mixture thereof or as a component
of an added fruit juice or tea. In the packaged beverage according
to the present invention, potassium ions can be contained in an
amount of preferably from 0.001 to 0.2 wt %, more preferably from
0.002 to 0.15 wt %, even more preferably from 0.003 to 0.12 wt %.
Similarly, a sodium ion ingredient can also be added as a
readily-available sodium salt such as sodium chloride, sodium
carbonate, sodium hydrogencarbonate, sodium citrate, sodium
phosphate, sodium hydrogenphosphate, sodium tartrate, sodium
benzoate or a mixture thereof or as a component of an added fruit
juice or tea. A lower sodium ion concentration is desired from the
standpoint of facilitating the absorption of water owing to osmotic
pressure. Preferably, however, the sodium ion concentration should
be such a level as to avoid suction of water into the intestine
from the body by osmotic pressure. The sodium ion concentration
required to achieve such level can preferably be lower than the
sodium ion concentration in the plasma. In the packaged beverage
according to the present invention, sodium ions can be contained at
a concentration of preferably from 0.001 to 0.5 wt %, more
preferably from 0.002 to 0.4 wt %, most preferably from 0.003 to
0.2 wt %. In addition to potassium ions and sodium ions, from 0.001
to 0.5 wt %, preferably from 0.002 to 0.4 wt %, still more
preferably from 0.003 to 0.3 wt % of chloride ions can also be
incorporated in the packaged beverage according to the present
invention. A chloride ion ingredient can be added in the form of a
salt such as sodium chloride or potassium chloride. Further, trace
ions such as calcium, magnesium, zinc and/or iron ions can also be
added. These ions can also be added in the form of salt or salts.
The total amount of ions existing in the beverage includes not only
an amount of ions added but also an amount of ions naturally
existing in the beverage. When sodium chloride is added, for
example, the amounts of sodium ions and chloride ions in the added
sodium chloride are included in the total amount of ions in the
beverage.
[0080] Depending upon the situation of drinking, an excessively low
concentration of sodium ions and potassium ions may fail to provide
a fulfilled feeling in taste and to achieve an effective
replenishment of minerals, and therefore, may not be preferred. An
unduly high concentration of sodium ions and potassium ions, on the
other hand, leads to strong tastes of the salts themselves and is
not preferred for long-term drinking.
[0081] In the packaged beverage according to the present invention,
a sweetener may also be used to improve the taste. As the
sweetener, an artificial sweetener, carbohydrate or glycerol (for
example, glycerin) can be used. The content of such a sweetener in
the packaged beverage according to the present invention is
preferably from 0.0001 to 20 wt %, more preferably from 0.001 to 15
wt %, even more preferably from 0.001 to 10 wt % from the
standpoints of the balance among sweetness, sourness and saltiness,
avoidance of excessive sweetness and a reduction in the feeling of
being caught in the throat and an improvement in the feeling as the
beverage passes down the throat.
[0082] As the sweeteners usable in the packaged beverage according
to the present invention, use of an artificial sweetener is
preferred. Example of the artificial sweeteners usable in the
present invention include high-sweetness sweeteners such as
saccharin, saccharin sodium, aspartame, acesulfame-K, sucralose and
neotame; and sugar alcohols such as sorbitol, erythritol and
xylitol. As commercial products, "SLIM-UP SUGAR" composed of
aspartame, "LAKANTO-S" containing erythritol, and "PALSWEET"
composed of erythritol and aspartame can be used.
[0083] When the aimed packaged beverage is intended to replenish
energy, it is preferred to use a carbohydrate sweetener.
[0084] As the carbohydrate sweeteners usable in the present
invention, soluble carbohydrates can be employed. A soluble
carbohydrate serves not only as a sweetener but also as an energy
source. Upon choosing a carbohydrate for use in the beverage
according to the present invention, it is preferred to take a
sufficient gastric excretion rate and intestinal absorption rate
into consideration.
[0085] The carbohydrate can be a mixture of glucose and fructose,
or a carbohydrate hydrolyzable into glucose and fructose or capable
of forming glucose and fructose in the digestive tract. The term
"carbohydrate" as used herein includes monosaccharides,
disaccharides, oligosaccharides, conjugated polysaccharides, and
mixtures thereof.
[0086] Monosaccharides usable in the present invention include
tetroses, pentoses, hexoses and ketohexoses. Examples of the
hexoses are aldohexoses such as glucose known as grape sugar. The
content of glucose in the packaged beverage can be preferably from
0.0001 to 20 wt %, more preferably from 0.001 to 15 wt %, still
more preferably from 0.001 to 10 wt %. Fructose known as fruit
sugar is a ketohexose. The content of fructose in the packaged
beverage according to the present invention can be preferably from
0.0001 to 20 wt %, more preferably from 0.001 to 15 wt %,
particularly preferably from 0.001 to 10 wt %.
[0087] Preferred in the beverage according to the present invention
is a single artificial sweetener system or a combination of an
artificial sweetener and a glucose compound or a combination of an
artificial sweetener and a fructose compound.
[0088] As a carbohydrate sweetener for use in the present
invention, a soluble carbohydrate can be employed. As an
oligosaccharide, a carbohydrate which produces these two kinds of
monosaccharides in vivo (specifically, sucrose, maltodextrin, corn
syrup, and fructose-rich corn syrup) can be mentioned. It is a
disaccharide that is an important type of the saccharide. An
illustrative disaccharide is sucrose known as cane sugar or beet
sugar. The content of sucrose in the packaged beverage according to
the present invention can be preferably from 0.001 to 20 wt %, more
preferably from 0.001 to 15 wt %, particularly preferably from
0.001 to 10 wt %.
[0089] The pH of the packaged beverage according to the present
invention can be preferably from 2 to 6, more preferably from 2 to
5, still more preferably from 3 to 4.5 from the standpoint of the
stability of catechins. An excessively low pH provides the beverage
with a stronger sour taste and pungent smell. An unduly high pH, on
the other hand, fails to achieve a harmony in flavor and leads to
reduction in taste. Such an excessively low pH or unduly high pH
is, therefore, not preferred.
[0090] Addition of a bitterness suppressor to the packaged beverage
according to the present invention facilitates its drinking, and
therefore, is preferred. Although no particular limitation is
imposed on the bitterness suppressor to be used, a cyclodextrin is
preferred. As the cyclodextrin, an .alpha.-,
.beta.-ory-cyclodextrin or a branched .alpha.-,
.beta.-ory-cyclodextrin can be used. In the beverage, a
cyclodextrin may be contained preferably in an amount of from 0.005
to 0.5 wt %, more preferably from 0.01 to 0.3 wt %. To the packaged
beverage according to the present invention, it is possible to add,
either singly or in combination, additives such as antioxidants,
flavorings, various esters, organic acids, organic acid salts,
inorganic acids, inorganic acid salts, inorganic salts, dyes,
emulsifiers, preservatives, seasoning agents, sweeteners, sour
seasonings, gums, emulsifiers, oils, vitamins, amino acids, fruit
extracts, vegetable extracts, flower honey extracts, pH regulators
and quality stabilizers.
[0091] To the beverage according to the present invention, one or
more of flavorings and fruit juices may preferably be added to
improve the taste. In general, the juice of a fruit is called
"fruit juice" and a flavoring is called "flavor". Natural or
synthetic flavorings and fruit juices can be used in the present
invention. They can be selected from fruit juices, fruit flavors,
plant flavors, and mixtures thereof. For example, a combination of
a fruit juice with a tea flavor, preferably a green tea or black
tea flavor provides attractive taste. Preferred fruit juices
include apple, pear, lemon, lime, mandarin, grapefruit, cranberry,
orange, strawberry, grape, kiwi, pineapple, passion fruit, mango,
guava, raspberry and cherry juices. More preferred are citrus
juices (preferably, grapefruit, orange, lemon, lime and mandarin
juices), mango juice, passion fruit juice, guava juice, and
mixtures thereof. Preferred natural flavors include jasmine,
chamomile, rose, peppermint, Crataegus cuneata, chrysanthemum,
water caltrop, sugarcane, bracket fungus of the genus Fomes (Fomes
japonicus), bamboo shoot, and the like. Such a juice can be
contained preferably in an amount of from 0.001 to 20 wt %, more
preferably from 0.002 to 10 wt % in the beverage according to the
present invention. Fruit flavors, plant flavors, tea flavors and
mixtures thereof can also be used as fruit juices. Particularly
preferred flavorings are citrus flavors including orange flavor,
lemon flavor, lime flavor and grapefruit flavor. In addition to
such citrus flavors, various other fruit flavors such as apple
flavor, grape flavor, raspberry flavor, cranberry flavor, cherry
flavor and pineapple flavor are also usable. These flavorings can
be derived from natural sources such as fruit juices and balms, or
can be synthesized. The term "flavoring" as used herein can also
include blends of various flavors, for example, a blend of lemon
and lime flavors and blends of citrus flavors and selected spices.
Such a flavoring can be added preferably in an amount of from
0.0001 to 5 wt %, more preferably from 0.001 to 3 wt % to the
beverage according to the present invention.
[0092] The beverage according to the present invention may also
contain a sour seasoning as needed. As the sour seasoning, edible
acids such as malic acid, citric acid, tartaric acid, and fumaric
acid can be mentioned. A sour seasoning may be used to adjust the
pH of the beverage according to the present invention. The pH of
the beverage according to the present invention is preferably from
2 to 7. As a pH adjuster, an organic or inorganic edible acid can
be used. The acid can be used either in a non-dissociated form or
in the form of its salt, for example, potassium hydrogenphosphate,
sodium hydrogenphosphate, potassium dihydrogenphosphate, or sodium
dihydrogenphosphate. Preferred acids can be edible organic acids
including citric acid, malic acid, fumaric acid, adipic acid,
phosphoric acid, gluconic acid, tartaric acid, ascorbic acid,
acetic acid, phosphoric acid, and mixtures thereof. Most preferred
acids are citric acid and malic acid. A sour seasoning is useful
also as an antioxidant which stabilizes the ingredients in the
beverage. Examples of commonly employed antioxidants include
ascorbic acid, EDTA (ethylenediaminetetraacetic acid) and salts
thereof, and plant extracts.
[0093] In the beverage according to the present invention, one or
more vitamins can be incorporated further. Preferably, vitamin A,
vitamin C, and vitamin E can be added. Other vitamins such as
vitamin D and vitamin B may also be added. Minerals can also be
used in the beverage according to the present invention. Preferred
minerals include calcium, chromium, copper, fluorine, iodine, iron,
magnesium, manganese, phosphorus, selenium, silicon, molybdenum,
and zinc. Particularly preferred minerals are magnesium,
phosphorus, and iron.
[0094] As in general beverages, a package used for the packaged
beverage according to the present invention can be provided in a
conventional form such as a molded package made essentially of
polyethylene terephthalate (a so-called PET bottle), a metal can, a
paper container combined with metal foils or plastic films, a
bottle or the like. The term "packaged beverage" as used herein
means a beverage that can be taken without dilution.
[0095] The packaged beverage according to the present invention can
be produced, for example, by filling the beverage in a package such
as a metal can and, when heat sterilization is feasible, conducting
heat sterilization under sterilization conditions as prescribed in
the Food Sanitation Act. For packages which cannot be subjected to
retort sterilization such as PET bottles or paper packages, adopted
is a process in which the beverage is sterilized beforehand at a
high temperature for a short time under similar sterilization
conditions as those described above, for example, by a plate-type
heat exchanger or the like, is cooled to a predetermined
temperature, and is then filled in a package. Under aseptic
conditions, additional ingredients may be added to and filled in a
beverage-filled package. It is also possible to conduct such an
operation that subsequent to heat sterilization under acidic
conditions, the pH of the beverage is brought back to neutral under
aseptic conditions or that subsequent to heat sterilization under
neutral conditions, the pH of the beverage is brought back to
acidic under aseptic conditions.
EXAMPLES
Measurement of Catechins
[0096] A high-performance liquid chromatograph (model: "SCL-10Avp")
manufactured by Shimadzu Corporation was fitted with a liquid
chromatograph column packed with octadecyl-introduced silica gel,
"L-Column, TM ODS" (4.6 mm in diameter.times.250 mm; product of
Chemicals Evaluation and Research Institute, Japan). A non-polymer
catechin composition was diluted with distilled water, filtered
through a filter (0.8 .mu.m), and then subjected to chromatography
at a column temperature of 35.degree. C. by the gradient elution
method making use of a solution A and a solution B. The solution A,
mobile phase, was a solution containing 0.1 mol/L of acetic acid in
distilled water, while the solution B was a solution containing 0.1
mol/L of acetic acid in acetonitrile. The measurement was conducted
under the conditions of 20 .mu.L sample injection volume and 280 nm
UV detector wavelength.
Measurement of Caffeine
(Analyzer)
[0097] A HPLC system (manufactured by Hitachi, Ltd.) was used.
[0098] Plotter: "D-2500", Detector: "L-4200", Pump: "L-7100",
[0099] Autosampler: "L-7200", Column: "INTERSIL ODS-2" (2.1 mm in
inner diameter.times.250 mm in length).
(Analytical Conditions)
[0099] [0100] Sample injection volume: 10 .mu.L [0101] Flow rate:
1.0 mL/min. [0102] Detection wavelength of UV spectrophotometer:
280 nm [0103] Eluent A: A 0.1 mol/L solution of acetic acid in
water [0104] Eluent B: A 0.1 mol/L solution of acetic acid in
acetonitrile
TABLE-US-00001 [0104] Concentration gradient conditions (vol. %)
Time (min) Eluent A Eluent B 0 97 3 5 97 3 37 80 20 43 80 20 43.5 0
100 48.5 0 100 49 97 3 62 97 3
[0105] (Retention Time of Caffeine) [0106] Caffeine: 27.2 min
[0107] From each area % determined here, the corresponding wt % was
determined based on the standard substance.
Assessment of Color
(Analyzer)
[0108] "UV MINI1240" (manufactured by Shimadzu Corporation)
analyzer was used.
[0109] An absorbance value at 450 nm was measured by a
spectrophotometer. In the measurement, each purified green tea
extract was diluted with ion-exchanged water such that the
concentration of catechins was lowered to 100 mg %. Using the
sample, the absorbance was measured, and was employed as an index
of color.
Visual Assessment of Stability
[0110] Each purified green tea extract was diluted with
ion-exchanged water such that the concentration of catechins was
lowered to 100 mg %. An assessment sample filled in a 50-mL vial
was observed for the state of its contents on an illuminator, and
the state of the contents was visually ranked.
Measurement of Proteins and Free Amino Acids
[0111] Calculation formula for (the amount of proteins and free
amino acids):
[0111] (Total nitrogen in purified green tea extract-caffeine-form
nitrogen).times.conversion index
[0112] Quantitation Method for Total Nitrogen
[0113] Determined by a nitrogen quantitation conversion method
(modified macro-Kjeldahl method) developed following the analytical
methods for nutritional components in the Nutrition Labeling
Standards (the methods listed in Column 3 of Table 1 attached to
the Nutrition Labeling Standards) (Notification No. 146 of the
Ministry of Health and Welfare, May 1996).
[0114] Caffeine-Form Nitrogen
[0115] Determined by converting each caffeine amount, which has
been obtained by the above-described measurement of the caffeine
amount, into the molecular weight of nitrogen (Mw=54) in the
molecular weight of caffeine (Mw=194).
[0116] Conversion Index
[0117] A conversion index (6.25) is used following the analytical
methods for nutritional components in the Nutrition Labeling
Standards (the methods listed in Column 3 of Table 1 attached to
the Nutrition Labeling Standards) (Notification No. 146 of the
Ministry of Health and Welfare, May 1996).
Example 1
Low-Caffeine Green Tea Extract A
[0118] A green tea extract ("POLYPHENON HG", product of Tokyo Food
Techno Co., Ltd.; 200 g) was dispersed in a 95% aqueous ethanol
solution (800 g) at room temperature under stirring at 250 r/min.
After addition of acid clay "MIZUKA ACE #600" (product of Mizusawa
Chemical Industries, Ltd.; 100 g), stirring was continued for about
10 minutes. Subsequently, filtration was conducted through No. 2
filter paper. Activated carbon (20 g) was then added, followed by
filtration through No. 2 filter paper again. Re-filtration was then
conducted through a 0.2-.mu.m membrane filter. Finally,
ion-exchanged water (200 g) was added to the filtrate, ethanol was
distilled away at 40.degree. C. and 0.0272 kg/cm.sup.2, and the
concentration of catechins was adjusted with ion-exchanged water to
obtain a product.
[0119] Content of non-polymer catechins [0120] after the treatment:
22 wt %.
[0121] Non-polymer catechins/caffeine weight [0122] ratio after the
treatment: 33.0
[0123] Gallates percentage after the treatment: 51 wt %.
Example 2
Low-Caffeine Green Tea Extract B
[0124] A green tea extract ("POLYPHENON HG", product of Tokyo Food
Techno Co., Ltd.; 100 g) was dispersed in a 70% aqueous ethanol
solution (100 g) at room temperature under stirring at 250 r/min.
After addition of activated carbon "KURARAY COAL GLC" (product of
Kuraray Chemical K.K.; 25 g) and acid clay "MIZUKAACE #600"
(product of Mizusawa Chemical Industries, Ltd.; 30 g), stirring was
continued for about 10 minutes. After a 95% aqueous ethanol
solution (800 g) was added dropwise over 30 minutes, stirring was
continued for 30 minutes at room temperature. Subsequently,
filtration was conducted again through No. 2 filter paper.
Re-filtration was then conducted through a 0.2-.mu.m membrane
filter. Finally, ion-exchanged water (200 g) was added to the
filtrate, ethanol was distilled away at 40.degree. C. and 0. 0272
kg/cm.sup.2, and the water content was adjusted to obtain a desired
product.
[0125] Content of non-polymer catechins [0126] after the treatment:
22 wt %.
[0127] Non-polymer catechins/caffeine weight [0128] ratio after the
treatment: 59.5
[0129] Gallates percentage after the treatment: 51.2 wt %.
Comparative Example 1
[0130] "POLYPHENON HG" (product of Tokyo Food Techno Co., Ltd.; 100
g) was dispersed as a green tea extract in water (900 g) at room
temperature under stirring at 250 r/min. After the addition of acid
clay "MIZUKA ACE #600" (product of Mizusawa Chemical Industries,
Ltd.; 100 g), stirring was continued for about 20 minutes.
Subsequently, stirring was continued for about 30 minutes at room
temperature. After filtration was conducted through No. 2 filter
paper, re-filtration was conducted through a 0.2-.mu.m membrane
filter. Finally, water was gradually evaporated by a drying
apparatus until the concentration of non-polymer catechins became
equivalent to that in Example 1 to obtain a product.
[0131] Content of non-polymer catechins [0132] after the treatment:
22 wt %.
[0133] Non-polymer catechins/caffeine weight [0134] ratio after the
treatment: 23.6
[0135] Gallates percentage after the treatment: 49.6 wt %.
Comparative Example 2
[0136] "POLYPHENONHG" (product of Tokyo Food Techno Co., Ltd.; 100
g) was dispersed as a green tea extract in water (900 g) at room
temperature under stirring at 250 r/min. After the addition of
activated carbon "KURARAY COAL GLC" (product of Kuraray Chemical
K.K.; 20 g) and acid clay "MIZUKA ACE #600" (product of Mizusawa
Chemical Industries, Ltd.; 100 g), stirring was continued for about
20 minutes. Stirring was then continued for about 30 minutes at
room temperature. After filtration was conducted through No. 2
filter paper, re-filtration was conducted through a 0. 2-.mu.m
membrane filter. Finally, water was gradually evaporated by a
drying apparatus until the concentration of non-polymer catechins
became equivalent to that in Example 1 to obtain a product.
[0137] Content of non-polymer catechins [0138] after the treatment:
22 wt %.
[0139] Non-polymer catechins/caffeine weight [0140] ratio after the
treatment: 42.6
[0141] Gallates percentage after the treatment: 47.6 wt %.
[0142] As shown in Table 1, the combined use of activated carbon
and acid clay while employing an aqueous solution, which contains
an organic solvent at a very high concentration, enables production
of a purified green tea extract having good color and stability in
which caffeine content is lowered without changing the gallates
percentage and gallocatechins percentage of its non-polymer
catechins.
TABLE-US-00002 TABLE 1 Present invention Comparison Example 1
Example 2 Comp. Ex. 1 Comp. Ex. 2 Solid green tea extract
(g).sup.1) 200 100 100 100 Ethanol (g) 760 830 0 0 Water (g) 40 70
900 900 Activated carbon (g).sup.2) 20 25 0 20 Acid clay (g).sup.3)
100 30 100 100 Organic solvent/water (weight 95/5 92/8 0/100 0/100
ratio) Non-polymer catechins after treatment (wt %).sup.4) GC 6.26
6.25 6.75 7.42 EGC 29.71 29.72 31.75 34.72 C 2.00 1.92 2.22 2.02 EC
9.92 10.01 9.64 8.24 EGCg 37.65 37.65 35.93 35.86 GCg 1.26 1.23
1.39 1.47 ECg 12.14 12.19 11.34 9.61 C 1.08 1.02 0.94 0.66
Non-polymer catechins/caffeine 33.0 59.5 23.6 42.6 after treatment
(weight ratio) Gallates percentage of non-polymer 51.0 51.2 49.6
47.6 catechins after treatment (wt %) Gallocatechins percentage of
74.9 73.5 75.8 79.5 non-polymer catechins after treatment (wt %)
Concentration of non-polymer 66 64 34 34 catechins in solids after
treatment (wt %) Absorbance (--) 0.038 0.031 0.535 0.270 Assessment
of purified products Caffeine Caffeine Color Color content was
content was deteriorated, deteriorated, lowered, color lowered,
color and and was good, and was good, and precipitation
precipitation stability was stability was occurred. occurred.
visually good. visually good.
[0143] (Note) 1) "POLYPHENON HG", product of Tokyo Food Techno Co.,
Ltd. [0144] 2) "KURARAY COAL GLC" , product of Kuraray Chemical
K.K. [0145] 3) "MIZUKA ACE #600", product of Mizusawa Chemical
Industries, Ltd. [0146] 4) Composition of non-polymer catechins in
the "POLYPHENON HG" preparation: [0147] GC (gallocatechin) 6.39 wt
%, EGC (epigallocatechin) 29.42 wt %, C (catechin) 2.16 wt %, EC
(epicatechin) 10.3 wt %, EGCg (epigallocatechingallate) 37.13 wt %,
GCg (gallocatechin gallate) 1.93 wt %, ECg (epicatechin gallate)
11.89 wt %, Cg (catechin gallate) 0.79 wt %, gallates percentage
51.73 wt %, gallocatechins percentage 74.88 wt %
Example 3
Packaged Beverages
[0148] Formulated solutions were prepared by adding the respective
green tea extracts shown in Table 1, adding the ingredients
described in Table 2, and then bringing the total amounts to 100
with ion-exchanged water, respectively. The formulated solutions
were subjected to a sterilization step according to the Food
Sanitation Act and hot-pack filling to obtain packaged
beverages.
[0149] The green tea extract C had the following composition:
[0150] Green Tea Extract C [0151] Caffeine-containing catechin
composition ("POLYPHENON HG", product of Tokyo Food Techno Co.,
Ltd). [0152] Content of non-polymer catechins 33.70 wt %, caffeine
content 5.5 wt %, non-polymer catechins/caffeine: 6.1, gallates
percentage 51 wt %.
[0153] Five trained male assessors were used. Those assessors
ingested 350 mL of each beverage, and assessed the beverages by
giving ranking scores to their mouth refreshment shortly after
drinking in accordance with the following standards.
[0154] 5: Very good mouth refreshment
[0155] 4: Good mouth refreshment
[0156] 3: Slightly good mouth refreshment
[0157] 2: Slightly poor mouth refreshment
[0158] 1: Poor mouth refreshment
TABLE-US-00003 TABLE 2 Comparative Invention products product
Formulations 1 2 1 Low-caffeine green tea extract A 1.00 -- --
Low-caffeine green tea extract B -- 1.00 -- Green tea extract C --
-- 0.65 Antioxidant 0.03 0.03 0.03 Sour seasoning 0.30 0.30 0.30
Sweetener 5.00 5.00 5.00 Fruit juice 0.05 0.05 0.05 Ion-exchanged
water Balance Balance Balance Total amount 100 100 100 PH of
beverage 3.5 3.5 3.6 Non-polymer catechins (wt %) 0.22 0.22 0.22
Non-polymer catechins/caffeine ratio 33 59.5 6.1 Mouth refreshment
shortly after 4 5 1 drinking
[0159] As evident from the results of Table 2, a packaged beverage
with outstanding mouth refreshment shortly after its drinking can
be obtained by using a low-caffeine green tea extract in which,
while maintaining the composition of catechins, caffeine has been
selectively removed by treating a green tea extract in accordance
with the present invention.
Example 4
[0160] In a similar manner as in Example 3, packaged beverages were
produced by mixing the ingredients shown in Table 3 and conducting
predetermined post-treatments.
[0161] It is to be noted that the green tea extract D was produced
in accordance with the following process.
[0162] Green Tea Extract D
[0163] A caffeine-containing catechin composition ("POLYPHENON HG",
product of Tokyo Food Techno Co., Ltd.; 100 g) was dispersed in a
95% aqueous ethanol solution (490.9 g) at room temperature under
stirring at 250 r/min. After addition of activated carbon "KURARAY
COAL GLC" (product of Kuraray Chemical K.K; 25 g) and acid clay
"MIZUKA ACE #600" (product of Mizusawa Chemical Industries, Ltd.;
30 g), stirring was continued for about 10 minutes. After a 40%
aqueous ethanol solution (409.1 g) was added dropwise over 10
minutes, stirring was continued for about 30 minutes at room
temperature. Subsequently, the activated carbon and precipitates
were filtered out by No. 2 filter paper, and re-filtration was
conducted through a 0.2-.mu.m membrane filter. Finally,
ion-exchanged water (200 g) was added to the filtrate, ethanol was
distilled away at 40.degree. C. and 0.0272 kg/cm.sup.2, and the
water content was adjusted to obtain the desired product.
[0164] Content of non-polymer catechins [0165] after the treatment:
22 wt %.
[0166] Non-polymer catechins/caffeine weight [0167] ratio after the
treatment: 20.0
[0168] Gallates percentage after the treatment: 51 wt %.
[0169] An assessment was performed to determine whether or not the
beverages according to the present invention are suited for
long-term drinking. Using ten trained assessors, drinking of 500 mL
per day was continued for 21 days to give a ranking score in
accordance with the following standards.
[0170] A: Suited
[0171] B: Somewhat suited
[0172] C: A little hard to continue drinking
[0173] D: Not suited for long-term drinking
[0174] Ten trained male assessors were used. Those assessors
ingested 500 mL of each beverage, and assessed the beverages by
giving ranking scores to their mouth refreshment shortly after
drinking in accordance with the following standards.
[0175] A: Good mouth refreshment
[0176] B: Slightly good mouth refreshment
[0177] C: Slightly poor mouth refreshment
[0178] D: Poor mouth refreshment
[0179] The assessment results are shown in Table 3.
TABLE-US-00004 TABLE 3 Invention products Comparative products
Formulations 3 4 5 2 3 4 5 Low-caffeine green tea extract A 1.00
2.00 0.50 5.00 0.1 -- -- Green tea extract C -- -- -- -- -- -- 0.65
Green tea extract D -- -- -- -- -- 1.00 -- Antioxidant 0.03 0.03
0.03 0.03 0.03 0.03 0.03 Sour seasoning 0.30 0.30 -- 0.30 0.30 0.30
0.30 pH adjuster -- -- -- -- -- -- -- Sweetener 5.00 5.00 -- 5.00
5.00 5.00 5.00 Mineral salts (Na, K) 0.07 0.07 -- 0.07 0.07 0.07
0.07 Fruit juice 0.05 0.05 -- 0.05 0.05 0.05 0.05 Black tea flavor
-- -- 0.1 -- -- -- -- Ion-exchanged water Balance Balance Balance
Balance Balance Balance Balance Total amount 100 100 100 100 100
100 100 pH of beverage 3.5 3.5 6.0 3.6 3.5 3.6 3.6 Non-polymer
catechins (wt %) 0.22 0.44 0.11 1.10 0.02 0.2 0.22 Non-polymer
catechins/caffeine 33 33 33 33 33 22 6.1 ratio Long-term
drinkability A A B D A C D Mouth refreshment shortly after A A A C
A C D drinking
[0180] As evident from the results of Table 3, a packaged beverage
suited for long-term drinking and capable of providing outstanding
mouth refreshment shortly after its drinking can be obtained by
using a low-caffeine green tea extract in which, while maintaining
the composition of catechins, caffeine has been selectively removed
by treating a green tea extract in accordance with the present
invention.
Example 5
Purified Green Tea Extract E
[0181] Acid clay "MIZUKAACE #600" (product of Mizusawa Chemical
Industries, Ltd.; 100 g) was dispersed in a 92.4 wt % aqueous
ethanol solution (800 g) at room temperature under stirring at 400
r/min, and the dispersion was stirred for about 10 minutes. A green
tea extract ("POLYPHENON HG", product of Tokyo Food Techno Co.,
Ltd.; 200 g) was added thereto, and stirring was continued for
about 3 hours at room temperature.
[0182] Filtration was then conducted through No. 2 filter paper.
The filtrate was brought into contact with activated carbon
"KURARAY COAL GLC" (product of Kuraray Chemical K.K.; 20 g), and
re-filtration was then conducted through a 0.2-.mu.m membrane
filter. Finally, ion-exchanged water (200 g) was added to the
filtrate, ethanol was distilled away at 40.degree. C. and 0.0272
kg/cm.sup.2, and the water content was adjusted to obtain a
product.
[0183] Acid clay/non-polymer catechins weight ratio: 1.5
[0184] Post-treatment: non-polymer [0185] catechins/(free
acids+proteins): 17
Example 6
Purified Green Tea Extract F
[0186] Acid clay "MIZUKAACE #600" (product of Mizusawa Chemical
Industries, Ltd.; 100 g) and citric acid (6.0 g) were dispersed in
a 92.4 wt % aqueous ethanol solution (800 g) at room temperature
under stirring at 400 r/min, and the dispersion was stirred for
about 10 minutes. A green tea extract ("POLYPHENON HG", product of
Tokyo Food Techno Co., Ltd.; 200 g) was added thereto, and stirring
was continued for about 3 hours at room temperature.
[0187] Filtration was then conducted through No. 2 filter paper.
The filtrate was brought into contact with activated carbon
"KURARAY COAL GLC" (product of Kuraray Chemical K.K.; 20 g), and
re-filtration was then conducted through a 0.2-.mu.m membrane
filter. Finally, ion-exchanged water (200 g) was added to the
filtrate, ethanol was distilled away at 40.degree. C. and 0.0272
kg/cm.sup.2, and the water content was adjusted to obtain a
product.
[0188] Citric acid/non-polymer catechins weight ratio: 0.08
[0189] Post-treatment: non-polymer [0190] catechins/(free
acids+proteins): 18
Example 7
Purified Green Tea Extract G
[0191] Acid clay "MIZUKAACE #600" (product of Mizusawa Chemical
Industries, Ltd.; 100 g) was dispersed in a 92.4 wt % aqueous
ethanol solution (800 g) at room temperature under stirring at 400
r/min, and the dispersion was stirred for about 10 minutes. A green
tea extract ("POLYPHENON HG", product of Tokyo Food Techno Co.,
Ltd.; 200 g) was added thereto, and stirring was continued for
about 3 hours at room temperature. After the temperature was raised
to 40.degree. C., stirring was continued for about 3 hours.
[0192] While maintaining the temperature at 40.degree. C.,
filtration was conducted through No. 2 filter paper. The filtrate
was then brought into contact at room temperature with activated
carbon "KURARAY COAL GLC" (product of Kuraray Chemical K.K.; 20 g),
and re-filtration was conducted through a 0.2-.mu.m membrane
filter. Finally, ion-exchanged water (200 g) was added to the
filtrate, ethanol was distilled away at 40.degree. C. and 0.0272
kg/cm.sup.2, and the water content was adjusted to obtain a
product.
[0193] Post-treatment: non-polymer [0194] catechins/(free
acids+proteins): 20
Example 8
Purified Green Tea Extract H
[0195] Acid clay "MIZUKAACE #600" (product of Mizusawa Chemical
Industries, Ltd.; 100 g) and citric acid (6.0 g) were dispersed in
a 92.4 wt % aqueous ethanol solution (800 g) at room temperature
under stirring at 400 r/min, and the dispersion was stirred for
about 10 minutes. A green tea extract ("POLYPHENON HG", product of
Tokyo Food Techno Co., Ltd.; 200 g) was added thereto, and stirring
was continued for about 3 hours at room temperature. After the
temperature was raised to 40.degree. C., stirring was continued for
about 3 hours.
[0196] While maintaining the temperature at 40.degree. C.,
filtration was conducted through No. 2 filter paper. The filtrate
was then brought into contact at room temperature with activated
carbon "KURARAY COAL GLC" (product of Kuraray Chemical K.K.; 20 g),
and re-filtration was conducted through a 0.2-.mu.m membrane
filter. Finally, ion-exchanged water (200 g) was added to the
filtrate, ethanol was distilled away at 40.degree. C. and 0.0272
kg/cm.sup.2, and the water content was adjusted to obtain a
product.
[0197] Post-treatment: non-polymer [0198] catechins/(free
acids+proteins): 19
Comparative Example 3
[0199] A green tea extract ("POLYPHENON HG", product of Tokyo Food
Techno Co., Ltd.; 200 g) was dispersed in water (900 g) at room
temperature under stirring at 250 r/min. After addition of
activated carbon "KURARAY COAL GLC" (product of Kuraray Chemical
K.K.; 40 g) and acid clay "MIZUKA ACE #600" (product of Mizusawa
Chemical Industries, Ltd.; 200 g), stirring was continued for about
20 minutes. Subsequently, stirring was continued for 30 minutes at
room temperature. After filtration was conducted through No. 2
filter paper, re-filtration was conducted through a 0.2-.mu.m
membrane filter. Finally, water was gradually evaporated by a
drying apparatus until the concentration of non-polymer catechins
became equivalent to that in Example 1 to obtain a product.
[0200] The production conditions and the analysis results of the
obtained green tea extracts in Examples 5 to 8 and Comparative
Example 3 are shown in Table 4.
TABLE-US-00005 TABLE 4 Present invention Comparison Example 5
Example 6 Example 7 Example 8 Comp. Ex. 3 Solid green tea extract
(g) 200 200 200 200 200 Ethanol (g) 739.2 739.2 739.2 739.2 0 Water
(g) 60.8 60.8 60.8 60.8 900 Activated carbon (g) 20 20 20 20 40
Acid clay (g) 100 100 100 100 200 Organic acid (g) 0 5.6 0 5.6 0
Organic solvent/water (weight 92/8 92/8 92/8 92/8 0/100 ratio)
Dissolution temperature (.degree. C.) 25 25 25.fwdarw.40
25.fwdarw.40 25 pH of the mixture 5.8 4.6 4.8 4.7 6.5 Non-polymer
catechins after treatment (wt %) GC 5.55 4.95 6.04 5.92 7.42 EGC
26.03 23.81 28.33 28.45 34.72 C 2.84 2.62 3.09 3.13 2.02 EC 8.49
7.45 9.24 8.90 8.24 EGCg 35.47 32.61 38.60 38.97 35.86 GCg 1.15
0.96 1.24 1.14 1.47 ECg 11.50 10.43 12.51 12.47 9.61 Cg 0.88 0.86
0.96 1.03 0.66 Non-polymer 29.6 30.4 32.2 36.4 42.6
catechins/caffeine(weight ratio) after treatment Gallates
percentage of 53.3 53.5 53.3 53.6 47.6 non-polymer catechins after
treatment (wt %) Gallocatechins percentage of 74.3 74.8 74.2 74.5
79.5 non-polymer catechins after treatment (wt %) Concentration of
non-polymer 68 62 63 61 34 catechins in solids after treatment (wt
%) Yield of non-polymer catechins 68 70 74 75 76 (wt %) Assessment
of purified products Caffeine Caffeine Caffeine Caffeine Color
deteri- content was content was content was content was orated, and
lowered, lowered, lowered, lowered, precipitation color was color
was color was color was occurred. good, and good, and good, and
rather good, stability stability was stability and stability was
visually visually was visually was visually good. good. good.
good.
[0201] Yield: Percentage of the amount of non-polymer catechins in
a purified green tea extract based on the amount of non-polymer
catechins in a green tea extract used as a feed material (wt %).
[0202] Composition of non-polymer catechins in the "POLYPHENON HG"
preparation: [0203] GC (gallocatechin) 6.39 wt %, EGC
(epigallocatechin) 29.42 wt %, C (catechin) 2.16 wt %, EC
(epicatechin) 10.3 wt %, EGCg (epigallocatechingallate) 37.13 wt %,
GCg (gallocatechin gallate) 1.93 wt %, ECg (epicatechin gallate)
11.89 wt %, Cg (catechin gallate) 0.79 wt %, gallates percentage
51.73 wt %, gallocatechins percentage 74.88 wt %
[0204] As shown in Table 4, use of acid clay and the contact
treatment in a particular pH range while employing an aqueous
solution which contains an organic solvent at a very high
concentration enables production of a purified green tea extract
having good color and stability in which caffeine content is
lowered without changing the gallates percentage and gallocatechins
percentage of the non-polymer catechins.
Example 9
[0205] Formulated solutions were prepared by adding the respective
purified green tea extracts shown in Table 4 and then bringing the
total amounts to 100 with ion-exchanged water, respectively. The
formulated solutions were subjected to a sterilization step
according to the Food Sanitation Act and hot-pack filling to obtain
packaged beverages.
[0206] Five trained male assessors were used. Those assessors
ingested 350 mL of each beverage, and assessed the beverages by
giving ranking scores to their mouth refreshment shortly after
drinking in accordance with the following standards.
[0207] 5: Very good mouth refreshment
[0208] 4: Good mouth refreshment
[0209] 3: Slightly good mouth refreshment
[0210] 2: Slightly poor mouth refreshment
[0211] 1: Poor mouth refreshment
TABLE-US-00006 TABLE 5 Comparative Invention products product
Formulations 6 7 8 9 6 Green tea extract (E) 1.00 Green tea extract
(F) 1.00 Green tea extract (G) 1.00 Green tea extract (H) 1.00
Extract of Comparative Example 3 1.00 Antioxidant 0.03 0.03 0.03
0.03 0.03 Sour seasoning 0.30 0.30 0.30 0.30 0.30 Sweetener 5.00
5.00 5.00 5.00 5.00 Fruit juice 0.05 0.05 0.05 0.05 0.05
Ion-exchanged water Balance Balance Balance Balance Balance Total
amount 100 100 100 100 100 pH of beverage 3.5 3.4 3.5 3.5 3.6
Non-polymer catechins (wt %) 0.22 0.22 0.22 0.22 0.22 Non-polymer
catechins/caffeine 29.6 30.4 32.2 36.4 42.6 Mouth refreshment
shortly after drinking 4 3 4 3 1
[0212] As evident from the results of Table 5, a packaged beverage
with outstanding mouth refreshment shortly after its drinking can
be obtained by using an invention product in which, while
maintaining the composition of catechins, caffeine has been
selectively removed by treating a green tea extract in accordance
with the present invention.
Example 10
Low-Caffeine Green Tea Extract I
[0213] Green tea leaves (steamed tea leaves from Sri Lanka; 100 g)
were evenly mixed with an 80% aqueous ethanol solution (36.5 g),
and were moistened at 5.degree. C. for 15 hours. The moistened
green tea leaves were charged in a semi-batch supercritical carbon
dioxide extraction apparatus, and were treated with carbon dioxide
which contained 2% of an 80% aqueous ethanol solution, at 30 MPa
and 70.degree. C. for 6 hours. The amount of carbon dioxide used
for the treatment was 14 kg. Subsequent to the treatment, the
extraction residue was dried under reduced pressure at 40.degree.
C. to obtain supercritical CO.sub.2-treated green tea leaves (92
g). The green tea leaves were extracted at 92.degree. C. for 1 hour
with ion-exchanged water (10 L), followed by filtration to obtain
an extract. The extract was lyophilized to obtain a green tea
extract (40 g). The contents of non-polymer catechins and caffeine
in the extract were 48 wt % and 2.2 wt %, respectively, and the
non-polymer catechins/caffeine weight ratio was 22.
[0214] The thus-obtained green tea extract (20 g) was suspended in
a 95% aqueous ethanol solution (98.18 g) at room temperature under
stirring at 250 r/min. After addition of activated carbon ("KURARAY
COAL GLC", product of Kuraray Chemical K.K.; 4 g) and acid clay
("MIZUKA ACE #600", product of Mizusawa Chemical Industries, Ltd.;
20 g), stirring was continued for about 10 minutes. After a 40%
aqueous ethanol solution (82 g) was added dropwise over 10 minutes,
stirring was continued for 40 minutes at room temperature. After
the activated carbon and precipitates were filtered out by No. 2
filter paper, re-filtration was conducted through a 0.2-.mu.m
membrane filter. Finally, ion-exchanged water (40 g) was added to
the filtrate, and ethanol was distilled away at 40.degree. C. and
3.4.times.10.sup.-3 MPa to obtain a product. The contents of
non-polymer catechins and caffeine in the product were 263 mg/100
mL and 4.3 mg/100 mL, respectively, and the non-polymer
catechins/caffeine weight ratio was 61.
TABLE-US-00007 TABLE 6 Example 10 Moistening Charged amount of
green 100 step of green tea leaves (g) tea leaves Moistening
solvent 80% aq. soln. of ethanol Amount of moistening 36.5 solvent
Supercritical Extraction pressure 30 carbon dioxide (MPa) treatment
step Extraction temperature 70 (.degree. C.) Extraction time (h) 6
Added solvent 80% aq. soln. of ethanol Amount of added solvent 2
(wt %) Amount of tea leaves 92 recovered after treatment (g)
Extraction Extraction solvent Ion-exchanged step for green water
tea extract Amount of extraction 10 solvent (L) Amount of extract
(g) 40
Example 11
[0215] Using the tea extract obtained in Example 10, the
citrus-flavored, packaged beverage described in Table 7 was
produced. The thus-obtained beverage was taken by eight trained
male assessors, and was assessed for the following five features.
The results are shown in Table 7.
Assessed Features
[0216] Tea flavor and taste (5-stage assessment): [0217] 1 Weak
[0218] 2 Slightly weak [0219] 3 Average [0220] 4 Slightly strong
[0221] 5 Strong
[0222] Citrus flavor and taste (5-stage assessment): [0223] 1 Weak
[0224] 2 Slightly weak [0225] 3 Average [0226] 4 Slightly strong
[0227] 5 Strong
[0228] Taste assessment (5-stage assessment): [0229] 1 Unpalatable
[0230] 2 Slightly unpalatable [0231] 3 Average [0232] 4 Slightly
tasty [0233] 5 Tasty
[0234] Changes in flavor and taste during high-temperature storage
(3-stage assessment): [0235] A Not changed [0236] B Slightly
changed [0237] C Changed
TABLE-US-00008 [0237] TABLE 7 Invention Added ingredients product
10 Beverage Supercritically treated product.sup.1) 460 formulation
Artificial sweetener.sup.2) 8 Sour seasoning 2.1 Ascorbic acid 0.3
NaCl 0.6 KCl 0.4 Dextrins 5 Citrus fruit juice.sup.3) 2 Citrus
flavor.sup.4) 5.5 Ion-exchanged water Balance Total 1000
Non-polymer catechins in beverage (wt %) 0.12 Non-polymer
catechins/caffeine ratio in 61 beverage (--) Assessment Tea flavor
and taste 1 results Citrus flavor and taste 5 Taste assessment 5
Changes in flavor and taste during high- A temperature storage
(product stored at 37.degree. C. for 3 months) .sup.1)Green tea
extract of Example 10 .sup.2)Sucralose .sup.3)Grape fruit
.sup.4)Grape fruit
[0238] It is appreciated from Table 7 that the packaged beverage
according to the present invention, which used the low-caffeine
green tea extract purified using the extract from the tea leaves as
the supercritical extraction residue, was extremely reduced in tea
flavor and taste, exhibited the flavor and taste of the added
citrus fruit juice and flavor, did not exhibit a green tea-derived
flavor and taste which would have been otherwise developed after
high-temperature storage, and was inhibited from flavor and taste
changes.
* * * * *