JP2008131932A - Method for producing tea extracted solution - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a method for producing a tea extracted solution which has a high rate of content of catechin even with a batch extraction method, and low thermal isomerization of catechin. <P>SOLUTION: This method for producing the tea extracted solution comprises extracting tea leaves in 55-80°C hot water so as to obtain an extracted solution (A) and used tea leaves B (first extraction process), and extracting the used tea leaves B in hot water of a temperature higher than that of the hot water used in the first extraction process, and in an extraction time period less than an extraction time period in the first extraction process so as to obtain an extracted solution C and used tea leaves D (second extraction process), and mixing the extracted solution (A) with the extracted solution C. <P>COPYRIGHT: (C)2008,JPO&INPIT

Description

本発明は、茶抽出液の製造方法、具体的には、濃縮液或いは乾燥エキスに調製して食品添加物として利用することができる、又は、そのまま或いは希釈して飲料として利用することができる茶抽出液の製造方法に関する。   The present invention relates to a method for producing a tea extract, specifically, a tea that can be used as a food additive prepared as a concentrated liquid or a dry extract, or used as a beverage as it is or after dilution. The present invention relates to a method for producing an extract.

茶抽出液や茶抽出エキスは、水可溶性成分としてタンニン（主にカテキン）、アミノ酸類、カフェイン、糖類、サポニンなどを含んでおり、茶特有の風味を添加するための食品添加物としてばかりか、薬理成分などとしても利用されている。   Tea extract and tea extract contains tannin (mainly catechin), amino acids, caffeine, sugars, saponins, etc. as water-soluble components, and is not only a food additive for adding tea-specific flavors. It is also used as a pharmacological component.

例えば、茶葉中に多く含まれるカテキン類には、抗酸化作用、抗菌作用、消臭作用、血中コレステロール抑制作用、α−アミラーゼ活性阻害作用、抗う蝕及び抗歯周病作用、下痢症ウイルス感染阻害作用、インフルエンザウイルス感染予防作用、マイコプラズマ感染予防作用、抗動脈硬化作用、解毒作用、活性酸素発生抑制作用、ガストリン分泌抑制作用などの様々な薬理作用が報告されている。   For example, catechins abundantly contained in tea leaves have antioxidant, antibacterial, deodorant, blood cholesterol inhibitory, α-amylase activity inhibitory, anti-cariogenic and anti-periodontal disease, diarrhea virus infection Various pharmacological actions such as an inhibitory action, an influenza virus infection preventive action, a mycoplasma infection preventive action, an anti-arteriosclerotic action, a detoxification action, an active oxygen generation inhibitory action, and a gastrin secretion inhibitory action have been reported.

カテキン類を高濃度で含有する茶エキス乃至茶抽出液を得るための方法として、有機溶媒を用いた液液抽出法やクロマト分離法などを利用する技術が知られている。   As a method for obtaining a tea extract or tea extract containing catechins at a high concentration, techniques using a liquid-liquid extraction method using an organic solvent, a chromatographic separation method, or the like are known.

例えば特許文献１には、クロロホルムでカフェインを除去し、酢酸エチルにより茶タンニン類を抽出することで、天然抗酸化剤を工業的に製造する方法が開示されている。
特許文献２や特許文献３には、クロマト分離を用いて茶カテキン類を選択的に充填剤に吸着させ、吸着成分を親水性有機溶媒により溶出させて茶カテキン類を精製する方法が開示されている。
特許文献４には、陽イオン交換樹脂に茶抽出物を接触させてカフェインを除去した後、エタノールを添加して沈殿物を生じさせ、該沈殿物を濾別除去することで、茶葉タンニン類を精製する方法が開示されている。 For example, Patent Document 1 discloses a method for industrially producing a natural antioxidant by removing caffeine with chloroform and extracting tea tannins with ethyl acetate.
Patent Document 2 and Patent Document 3 disclose a method for purifying tea catechins by selectively adsorbing tea catechins to a filler using chromatographic separation and eluting the adsorbed component with a hydrophilic organic solvent. Yes.
In Patent Document 4, tea extract is contacted with a cation exchange resin to remove caffeine, ethanol is added to form a precipitate, and the precipitate is removed by filtration to remove tea leaf tannins. A method for purifying is disclosed.

また、茶葉から高濃度のカテキン類を抽出する方法として、次のような方法が知られている。   Moreover, the following methods are known as a method of extracting high concentration catechins from tea leaves.

特許文献５には、香気成分保持を目的として、茶原料を、水を加えた後に密封できる柔軟性のある容器に封入し、これに対して低温で超高圧抽出を行い、第１の抽出液とする一方、この抽出残渣を高温で再抽出して高温抽出液を調製し、これを第２の抽出液として、第１抽出液と第２抽出液とを混合して加工する方法が開示されている。   In Patent Document 5, a tea raw material is enclosed in a flexible container that can be sealed after adding water for the purpose of retaining aroma components. On the other hand, a method is disclosed in which the extraction residue is re-extracted at a high temperature to prepare a high-temperature extract, and this is used as a second extract to mix and process the first extract and the second extract. ing.

特許文献６には、高濃度のカテキンを含有し、異臭の発生や雑味を低減させた緑茶飲料を提供することを目的として、緑茶葉を１０℃未満の水で抽出し(第１工程)、第１工程の抽出残渣を５０℃以上の温水で抽出し(第２工程)、第１工程で得られた抽出液（Ａ）と第２工程で得られた抽出液（Ｂ）を混合し、次いで殺菌処理を施す緑茶飲料の製造方法が開示されている。   In Patent Document 6, green tea leaves are extracted with water of less than 10 ° C. for the purpose of providing a green tea beverage that contains a high concentration of catechin and has reduced off-flavor generation and miscellaneous taste (first step). The extraction residue of the first step is extracted with warm water of 50 ° C. or more (second step), and the extract (A) obtained in the first step and the extract (B) obtained in the second step are mixed. Then, a method for producing a green tea beverage that is then sterilized is disclosed.

特許文献７には、紅茶や烏龍茶の香りが強く、雑味が低減され、後味が改良された発酵茶飲料又は半発酵茶飲料の提供することを目的として、発酵茶葉又は半発酵茶葉を１０℃未満の水で抽出し(第１工程)、第１工程の抽出残渣を５０℃以上の温水で抽出し(第２工程)、第１工程で得られた抽出液（Ａ）と第２工程で得られた抽出液（Ｂ）を混合し、次いで殺菌処理を施す茶飲料の製造方法が開示されている。   In Patent Document 7, fermented tea leaves or semi-fermented tea leaves are added at 10 ° C. for the purpose of providing a fermented tea drink or semi-fermented tea drink with strong aroma of black tea or oolong tea, reduced miscellaneous taste, and improved aftertaste. Extract with less than water (first step), extract the extraction residue of the first step with warm water of 50 ° C. or more (second step), and extract liquid (A) obtained in the first step and the second step A method for producing a tea beverage in which the obtained extract (B) is mixed and then sterilized is disclosed.

特許１５６１０４３号公報Japanese Patent No. 1561043 特許２７０３２４１号公報Japanese Patent No. 2703241 特許３０５２１７５号公報Japanese Patent No.3052175 特開平１１−２２８５６５号公報JP-A-11-228565 特開平６−３０７０３号公報JP-A-6-30703 特開２００３−２１９７９９号公報JP 2003-219799 A 特開２００３−２３０３５８号公報JP 2003-230358 A

カテキン類としては、（−）エピガロカテキンガレ−ト（ＥＧＣｇ）、（−）エピカテキンガレ−ト（ＥＣｇ）、（−）エピガロカテキン（ＥＧＣ）、（−）エピカテキン（ＥＣ）、（−）ガロカテキンガレ−ト（ＧＣｇ）、（−）カテキンガレ−ト（Ｃｇ）、（−）ガロカテキン（ＧＣ）及び（−）カテキン（Ｃ）の８種が知られているが、天然物である茶葉中に多く含まれている茶カテキン類は、これらのうちの（−）ＥＧＣｇ、（−）ＥＣｇ、（−）ＥＧＣ、（−）ＥＣの４種類であり、残りの４種、すなわち（−）ＧＣｇ、Ｃｇ、（−）ＧＣ及び（−）カテキン（Ｃ）は、前記４種類のカテキンのエピマー、すなわち一つの不斉炭素原子が反転した立体配置を持つジアステレオマー（鏡像異性体以外のすべての立体異性体）であり、これらは前記４種類のカテキンの熱異性体であることが知られている。   The catechins include (−) epigallocatechin gallate (EGCg), (−) epicatechin gallate (ECg), (−) epigallocatechin (EGC), (−) epicatechin (EC), ( Eight types of-) gallocatechin gallate (GCg), (-) catechin gallate (Cg), (-) gallocatechin (GC) and (-) catechin (C) are known, but are natural products. Tea catechins contained in a large amount in tea leaves are (−) EGCg, (−) ECg, (−) EGC, (−) EC, and the remaining 4 types, that is, (− GCg, Cg, (−) GC and (−) catechin (C) are epimers of the above four types of catechins, that is, diastereomers having a configuration in which one asymmetric carbon atom is inverted (other than enantiomers). All stereoisomers), These are known to be heat-isomer of the 4 types of catechins.

茶葉から得られるカテキン類の中でも、（−）ＥＧＣｇは、特に薬理効果に優れており、しかも茶特有の苦渋味の主体でもあるため、この（−）ＥＧＣｇを高濃度で含有する茶抽出液（エキス含む）が多くの分野で望まれている。   Among the catechins obtained from tea leaves, (−) EGCg is particularly excellent in pharmacological effect, and also has a bitter and astringent taste peculiar to tea. Therefore, a tea extract containing this (−) EGCg in a high concentration ( Extract) is desired in many fields.

ところが、バッチ抽出法によって茶葉を高温で抽出すると、カテキン類の収率は高まるが、熱異性化が進んで（−）ＥＧＣｇが（−）ＧＣｇに変化するため（−）ＥＧＣｇの含有濃度が低下してしまう。逆に、熱異性化を生じない低温で抽出したのではカテキン類の収率を高めることができないことが明らかになってきた。   However, when tea leaves are extracted at a high temperature by the batch extraction method, the yield of catechins increases, but thermal isomerization proceeds and (-) EGCg changes to (-) GCg, so the concentration of (-) EGCg decreases. Resulting in. On the contrary, it has become clear that the yield of catechins cannot be increased by extraction at a low temperature that does not cause thermal isomerization.

他方、カラム抽出法によれば、カテキン類の抽出効率を高めつつ、カテキン類の熱異性化を抑えることは可能であるものの、この抽出法によると抽出液量が大きくなり過ぎてしまうため、経済的に実用的な方法ではない。   On the other hand, according to the column extraction method, it is possible to suppress the thermal isomerization of catechins while increasing the extraction efficiency of catechins. Is not practical.

そこで本発明は、バッチ抽出法を採用した場合であっても、カテキン類の抽出効率の向上とカテキン類の熱異性化の抑制との両立を図ることができ、カテキン含有率が高く、且つカテキン類の熱異性化率が低い特徴を備えた茶抽出液を製造し得る茶抽出液の製造方法を提供せんとするものである。   Therefore, the present invention can achieve both improvement in the extraction efficiency of catechins and suppression of thermal isomerization of catechins even when a batch extraction method is adopted, a high catechin content, and catechins. It is intended to provide a method for producing a tea extract that can produce a tea extract having a low thermal isomerization rate.

本発明は、茶葉を５５℃〜８０℃の温水で抽出して抽出液Ａと茶殻Ｂとを得(第１抽出工程)、茶殻Ｂを、第１抽出工程で用いた温水の温度以上の温水で、且つ第１抽出工程での抽出時間以下の抽出時間で抽出して抽出液Ｃと茶殻Ｄを得(第２抽出工程)、抽出液Ａと抽出液Ｃを混合することを特徴とする茶抽出液の製造方法を提案する。   In the present invention, tea leaves are extracted with warm water of 55 ° C. to 80 ° C. to obtain an extract A and tea husk B (first extraction step), and the tea husk B is warm water at or above the temperature of the hot water used in the first extraction step. In addition, the extraction liquid C and the tea husk D are obtained by extraction with an extraction time equal to or less than the extraction time in the first extraction process (second extraction process), and the extraction liquid A and the extraction liquid C are mixed. A method for producing the extract is proposed.

本発明はまた、茶葉を５５℃〜８０℃の温水で抽出して抽出液Ａと茶殻Ｂを得(第１抽出工程)、茶殻Ｂを、第１抽出工程で用いた温水の温度以上の温水で、且つ第１抽出工程での抽出時間以下の抽出時間で抽出して抽出液Ｃと茶殻Ｄを得(第２抽出工程)、茶殻Ｄを、第１抽出工程で用いた温水の温度以上の温水で、且つ第１抽出工程での抽出時間以下の抽出時間で抽出して抽出液Ｅを得(第３抽出工程)、抽出液Ａ、抽出液Ｃ及び抽出液Ｅを混合することを特徴とする茶抽出液の製造方法を提案する。   In the present invention, the tea leaves are extracted with hot water of 55 ° C. to 80 ° C. to obtain an extract A and a tea husk B (first extraction step), and the tea husk B is warm water at or above the temperature of the hot water used in the first extraction step. In addition, extraction liquid C and tea husk D are obtained by extraction with an extraction time equal to or shorter than the extraction time in the first extraction step (second extraction step), and the tea husk D is higher than the temperature of the hot water used in the first extraction step. Extracted with warm water and with an extraction time not longer than the extraction time in the first extraction step to obtain an extract E (third extraction step), and the extract A, the extract C and the extract E are mixed. We propose a method for producing tea extract.

茶葉を熱異性化の生じ難い５５℃〜８０℃の温水で抽出した後、抽出残渣である茶殻を高温且つ短時間で抽出することにより、カテキン類の熱異性化を抑制しつつカテキン類の抽出率を高めることができる。よって、本発明によれば、従来のように有機溶媒を用いた液液抽出やクロマト分離を行なうことなく、カテキン類の含有率が高く、且つ、カテキン類の熱異性化が抑えられた茶抽出液を得ることができ、カテキン類、特にＥＧＣｇを高濃度で含む茶抽出液を提供することができる。   Extraction of tea catechins while suppressing thermal isomerization of catechins by extracting tea leaves, which are extraction residues, at high temperature and in a short time after extracting tea leaves with hot water at 55 ° C to 80 ° C where heat isomerization hardly occurs The rate can be increased. Therefore, according to the present invention, tea extraction with a high content of catechins and reduced thermal isomerization of catechins without performing liquid-liquid extraction or chromatographic separation using an organic solvent as in the prior art. And a tea extract containing a high concentration of catechins, particularly EGCg, can be provided.

なお、本発明において「カテキン類」とは、（−）−エピガロカテキン（ＥＧＣ）、（−）−エピガロカテキンガレート（ＥＧＣｇ）、（−）−エピカテキン（ＥＣ）、（−）−エピカテキンガレート（ＥＣｇ）、（−）−ガロカテキン（ＧＣ）、（−）−ガロカテキンガレート（ＧＣｇ）、（−）−カテキン（Ｃ）、（−）−カテキンガレート（Ｃｇ）のいずれか（これら８種類をまとめて「総カテキン」ともいう）、或いはこれらのうちの二種類以上の組み合わせからなる混合物を包含する意である。
但し、「カテキン類の熱異性化」と表現する場合の「カテキン類」は、「熱異性化カテキン類」ではないカテキン類、すなわち（−）−エピガロカテキン（ＥＧＣ）、（−）−エピガロカテキンガレート（ＥＧＣｇ）、（−）−エピカテキン（ＥＣ）、（−）−エピカテキンガレート（ＥＣｇ）のいずれか、或いはこれらのうちの二種類以上の組み合わせからなる混合物を包含する意である。
「熱異性化カテキン類」とは、（−）−ガロカテキン（ＧＣ）、（−）−ガロカテキンガレート（ＧＣｇ）、（−）−カテキン（Ｃ）、（−）−カテキンガレート（Ｃｇ）のいずれか、或いはこれらのうちの二種類以上の組み合わせからなる混合物を包含する意である。 In the present invention, “catechins” means (−)-epigallocatechin (EGC), (−)-epigallocatechin gallate (EGCg), (−)-epicatechin (EC), (−)-epi. Catechin gallate (ECg), (−)-gallocatechin (GC), (−)-gallocatechin gallate (GCg), (−)-catechin (C), or (−)-catechin gallate (Cg) (these 8) The types are collectively referred to as “total catechins”), or a mixture of two or more of these.
However, “catechins” when expressed as “thermal isomerization of catechins” means catechins that are not “thermal isomerized catechins”, that is, (−)-epigallocatechin (EGC), (−)-epi. Gallocatechin gallate (EGCg), (−)-epicatechin (EC), (−)-epicatechin gallate (ECg), or a mixture of two or more of these is meant to be included. .
“Thermal isomerized catechins” means any of (−)-gallocatechin (GC), (−)-gallocatechin gallate (GCg), (−)-catechin (C), and (−)-catechin gallate (Cg). Or a mixture of two or more of these.

また、本発明において、「Ｘ〜Ｙ」（Ｘ，Ｙは任意の数字）と表現した場合、特にことわらない限り「Ｘ以上Ｙ以下」の意を示し、同時に「好ましくはＸより大きく、Ｙより小さい」の意を包含する。   In the present invention, when expressed as “X to Y” (X and Y are arbitrary numbers), it means “X or more and Y or less” unless otherwise specified, and at the same time, “preferably larger than X, Y It means “smaller”.

発明を実施するための形態BEST MODE FOR CARRYING OUT THE INVENTION

以下、本発明を実施するための実施形態について説明するが、本発明が以下の実施形態に限定されるものではない。   Hereinafter, although the embodiment for carrying out the present invention is described, the present invention is not limited to the following embodiment.

本発明の実施形態に係る茶抽出液の製造方法は、茶葉を温水で抽出して抽出液Ａと茶殻Ｂとを得(第１抽出工程)、茶殻Ｂを、第１抽出工程での温水温度以上の温度の温水で、且つ第１抽出工程での抽出時間以下の抽出時間で抽出して抽出液Ｃと茶殻Ｄを得(第２抽出工程)、抽出液Ａと抽出液Ｃを混合するというものであり、好ましくは、さらに茶殻Ｄを、第１抽出工程での温水温度以上の温度の温水で、且つ第１抽出工程での抽出時間以下の抽出時間で抽出して抽出液Ｅを得(第３抽出工程)、抽出液Ａ、抽出液Ｃ及び抽出液Ｅを混合する製法である。以下、詳述する。   In the method for producing a tea extract according to an embodiment of the present invention, tea leaves are extracted with warm water to obtain an extract A and a tea husk B (first extraction step), and the tea husk B is subjected to a hot water temperature in the first extraction step. Extraction is performed with hot water at the above temperature and with an extraction time equal to or less than the extraction time in the first extraction step to obtain the extract C and the tea leaves D (second extraction step), and the extract A and the extract C are mixed. Preferably, the tea husk D is further extracted with hot water having a temperature equal to or higher than the hot water temperature in the first extraction step and with an extraction time equal to or less than the extraction time in the first extraction step to obtain an extract E ( (3rd extraction process), it is the manufacturing method which mixes the extract A, the extract C, and the extract E. Details will be described below.

（茶葉）
原料とする茶葉としては、茶樹（学名：Camellia sinensis）から摘採した葉や茎であれば、その品種、産地、摘採時期、摘採方法、栽培方法などに限られず、どのような茶も使用することができる。例えば、煎茶、釜炒り茶、かぶせ茶、玉露、てん茶、抹茶、番茶、焙じ茶、蒸製玉緑茶、釜炒製玉緑茶などのいずれか、或いはこれらの二種以上の組み合わせからなる混合物を原料として用いることができる。また、上記の茶に現在公知の仕上加工を施して得られる仕上茶も原料として用いることができる。
さらに、緑茶以外に、烏龍茶などの半発酵茶、紅茶などの発酵茶も原料として用いることができる。 (tea leaf)
The tea leaves used as raw materials are not limited to their cultivar, origin, picking time, picking method, cultivation method, etc., as long as they are leaves and stems picked from tea trees (scientific name: Camellia sinensis). Can do. For example, sencha, pot roasted tea, kabusecha, gyokuro, tencha, matcha, bancha, roasted tea, steamed ball green tea, kettle roasted ball green tea, or a mixture of two or more of these as raw materials Can be used. Also, a finished tea obtained by subjecting the above tea to a currently known finishing process can be used as a raw material.
In addition to green tea, semi-fermented tea such as oolong tea and fermented tea such as black tea can also be used as raw materials.

（第１抽出工程における抽出条件）
第１抽出工程において、抽出に用いる温水（以下「抽出温水」という）の温度は、５５〜８０℃であるのが好ましく、特に６０〜８０℃、中でも特に７０〜８０℃であるのが好ましい。５５〜８０℃で抽出することにより、カテキン類の熱異性化を抑えることができる。なお、９０℃で抽出すると、８０℃で抽出した場合に比べてＧＣｇの生成率が２倍以上になる場合があることが確認されている。
抽出温水のｐＨは、特に限定するものではない。例えばｐＨ４〜７、特にｐＨ５〜６の抽出温水を好ましく用いることができる。例えばｐＨ４以下であれば、抽出温度に関係なくカテキン類の熱異性化を抑制することができるが、ｐＨ調整剤を後工程で除去する必要があるため、前記ｐＨ領域が好ましい。
抽出温水の量は、原料茶葉の１０〜３０倍量（質量割合）であるのが好ましく、特に１０〜２５倍量、中でも特に１０〜２０倍量であるのが好ましい。
抽出時間は、５分〜６０分間とするのが好ましく、特に１５分〜６０分間、中でも特に１５分〜２０分間とするのが好ましい。 (Extraction conditions in the first extraction step)
In the first extraction step, the temperature of warm water used for extraction (hereinafter referred to as “extracted warm water”) is preferably 55 to 80 ° C., particularly 60 to 80 ° C., and particularly preferably 70 to 80 ° C. By extracting at 55-80 degreeC, the thermal isomerization of catechins can be suppressed. In addition, when extracting at 90 degreeC, compared with the case where it extracts at 80 degreeC, it has been confirmed that the production rate of GCg may become 2 times or more.
The pH of the hot extraction water is not particularly limited. For example, extraction hot water having a pH of 4 to 7, particularly a pH of 5 to 6 can be preferably used. For example, if the pH is 4 or less, the thermal isomerization of catechins can be suppressed regardless of the extraction temperature, but the pH region is preferable because the pH adjuster needs to be removed in a subsequent step.
The amount of the extracted hot water is preferably 10 to 30 times (mass ratio) of the raw tea leaves, more preferably 10 to 25 times, and particularly preferably 10 to 20 times.
The extraction time is preferably 5 minutes to 60 minutes, particularly 15 minutes to 60 minutes, and particularly preferably 15 minutes to 20 minutes.

より具体的には、原料茶葉の１０〜３０倍量の６０〜８０℃の抽出温水で５分〜６０分間抽出するのが好ましく、特に原料茶葉の１０〜２５倍量の６０〜８０℃の抽出温水で１５分〜６０分間抽出するのがより好ましく、中でも特に原料茶葉の１０〜２０倍量の７０〜８０℃の抽出温水で１５分〜２０分間抽出するのがさらに好ましい。   More specifically, it is preferable to extract for 5 to 60 minutes with 60 to 80 ° C. extraction hot water of 10 to 30 times the amount of the raw tea leaves, and particularly 60 to 80 ° C. extraction for 10 to 25 times the amount of the raw tea leaves. It is more preferable to extract with warm water for 15 minutes to 60 minutes, and it is particularly preferable to extract with warm water extracted at 70 to 80 ° C., which is 10 to 20 times the amount of raw tea leaves.

得られた抽出液はすぐに３０℃以下に冷却し、３０℃以下の環境下で保管するのが好ましい。３０℃以下に冷却し保管することで、酸化防止を図ることができるばかりか、難溶性成分を析出させることができるため、遠心分離等により難溶性成分を分離除去することができる。   The obtained extract is immediately cooled to 30 ° C. or lower and stored in an environment of 30 ° C. or lower. By cooling and storing at 30 ° C. or lower, not only can the oxidation be prevented, but also a hardly soluble component can be precipitated, so that the hardly soluble component can be separated and removed by centrifugation or the like.

（第２抽出工程・第３抽出工程）
第１抽出工程終了後は、より速やかに第２抽出工程を開始するのが好ましい。具体的には、処理する茶葉量にもよるが、目安としては、第１抽出工程の固液分離開始から第２抽出工程の熱水投入までの時間を３０秒〜５分以内とするのが好ましい。このように第１抽出工程終了後、より速やかに第２抽出工程を開始するようにすれば、茶殻の温度が冷めないように維持することができ、カテキン類の抽出率向上並びにカテキン類の熱異性化抑制に貢献することができる。第２抽出工程終了後の第３抽出工程の開始においても同様である。 (Second extraction process / Third extraction process)
It is preferable to start the second extraction step more promptly after the first extraction step. Specifically, although it depends on the amount of tea leaves to be processed, as a guide, the time from the start of solid-liquid separation in the first extraction process to the addition of hot water in the second extraction process should be within 30 seconds to 5 minutes. preferable. Thus, if the 2nd extraction process is started more promptly after the completion of the 1st extraction process, the temperature of the tea husk can be maintained so as not to cool, and the extraction rate of catechins can be improved and the heat of catechins can be increased. It can contribute to suppression of isomerization. The same applies to the start of the third extraction step after the end of the second extraction step.

第２乃至第３抽出工程で用いる抽出温水の温度は、第１抽出工程で用いた抽出温水の温度と同じか或いはそれより高温であるのが好ましく、第１抽出工程で用いた抽出温水に比べて５〜２０℃高温であるのが好ましい。特に７５〜１００℃、中でも特に７５〜９５℃の抽出温水で抽出するのが好ましい。
この際、抽出温水のｐＨは、特に限定するものではない。例えばｐＨ４〜７、特にｐＨ５〜６の抽出温水を好ましく用いることができる。例えばｐＨ４以下であれば、抽出温度に関係なくカテキン類の熱異性化を抑制することができるが、ｐＨ調整剤を後工程で除去する必要があるため、前記ｐＨ領域が好ましい。 The temperature of the extraction hot water used in the second to third extraction steps is preferably the same as or higher than the temperature of the extraction hot water used in the first extraction step, compared to the extraction hot water used in the first extraction step. The temperature is preferably 5 to 20 ° C. It is particularly preferable to extract with extraction hot water of 75 to 100 ° C, particularly 75 to 95 ° C.
At this time, the pH of the extracted hot water is not particularly limited. For example, extraction hot water having a pH of 4 to 7, particularly a pH of 5 to 6 can be preferably used. For example, if the pH is 4 or less, the thermal isomerization of catechins can be suppressed regardless of the extraction temperature, but the pH region is preferable because the pH adjuster needs to be removed in a subsequent step.

第２乃至第３抽出工程で用いる抽出温水の量は、第１抽出工程で用いた抽出温水と同じか或いは少ない量であるのが好ましく、第１抽出工程で用いた抽出温水に比べて２〜５倍量（抽出前の茶葉に対する質量割合）だけ少ない量で、且つ５倍量以上であるのが好ましく、特に原料茶葉の５〜２５倍量（質量割合）、中でも特に５〜２０倍量であるのがさらに好ましい。   The amount of hot extraction water used in the second to third extraction steps is preferably the same or less than the hot extraction water used in the first extraction step, and is 2 to 2 compared to the extraction hot water used in the first extraction step. 5 times the amount (mass ratio with respect to the tea leaves before extraction) is preferably as small as 5 times the amount, especially 5 to 25 times the amount (mass ratio) of the raw tea leaves, especially 5 to 20 times the amount. More preferably.

第２乃至第３抽出工程における抽出時間は、第１抽出工程と同じか或いはより短時間とするのが好ましく、第１抽出工程に比べて３分〜１０分短くするのが好ましい。特に１分〜１５分間、中でも特に５分〜１５分間とするのが好ましい。   The extraction time in the second to third extraction steps is preferably the same as or shorter than that of the first extraction step, and is preferably 3 to 10 minutes shorter than that of the first extraction step. It is particularly preferably 1 minute to 15 minutes, and particularly preferably 5 minutes to 15 minutes.

ここで、第２乃至第３抽出工程における好ましい抽出条件としては、第１抽出工程で用いた抽出温水より少ない量で、且つ、第１抽出工程で用いた抽出温水より高温の抽出温水にて、第１抽出工程より短い抽出時間で抽出を行なうのが好ましく、特に原料茶葉の５〜２５倍量の７５〜１００℃の抽出温水で１分〜１５分間抽出するのが好ましく、中でも特に原料茶葉の５〜２０倍量の７５〜９５℃の抽出温水で５分〜１５分間抽出するのがさらに好ましい。
このような第２乃至第３抽出工程を実施すれば、第１抽出工程では、６０〜８５℃で抽出することにより、カテキン類の熱異性化を抑えることができるが、それではカテキン抽出率が十分ではないため、茶殻に高温の抽出温水を追加し、１回目の抽出より短時間で抽出を行い、第２及び第３抽出工程で得られた抽出液を混合することにより、カテキン類の熱異性化を抑えつつカテキン抽出率を高めることができる。 Here, as a preferable extraction condition in the second to third extraction steps, the extraction hot water is smaller in amount than the extraction hot water used in the first extraction step, and the extraction hot water is higher in temperature than the extraction hot water used in the first extraction step. Extraction is preferably performed with an extraction time shorter than that of the first extraction step, and in particular, extraction is preferably performed for 1 to 15 minutes with 75 to 100 ° C. hot water of 5 to 25 times the amount of the raw tea leaves. It is more preferable to extract for 5 to 15 minutes with 5 to 20 times the extraction warm water of 75 to 95 ° C.
If such 2nd thru | or 3rd extraction process is implemented, in a 1st extraction process, it can suppress the thermal isomerization of catechins by extracting at 60-85 degreeC, However, The catechin extraction rate is enough in that Therefore, by adding hot extraction hot water to the tea husk, extracting in a shorter time than the first extraction, and mixing the extract obtained in the second and third extraction steps, the thermal isomerism of catechins The catechin extraction rate can be increased while suppressing crystallization.

（抽出方式）
第１抽出工程から第３抽出工程のいずれにおいても、抽出方式を特に限定するものではないが、バッチ方式を選択するのがより好ましい。カラム抽出法によれば、抽出液量が大きくなるため経済的に実用的な方法ではない。また、本発明は、バッチ抽出法であっても、カテキン類の抽出効率の向上とカテキン類の熱異性化の抑制とを両立することができる点に特徴があるからである。
なお、バッチ方式或いはバッチ抽出法とは、抽出槽内へ原料と抽出溶媒とを投入し、抽出後に溶媒（抽出液）を充分に排出させた後、当該抽出槽内に前記とは別の抽出溶媒を投入する。この操作を１〜３回繰り返し行なう抽出方式（抽出方法）の意である。 (Extraction method)
In any of the first extraction process to the third extraction process, the extraction method is not particularly limited, but it is more preferable to select the batch method. The column extraction method is not an economically practical method because the amount of the extract becomes large. Moreover, even if it is a batch extraction method, this invention is because the improvement in extraction efficiency of catechins and the suppression of thermal isomerization of catechins can be made compatible.
The batch method or batch extraction method is a method in which a raw material and an extraction solvent are introduced into an extraction tank, and after extraction, the solvent (extract liquid) is sufficiently discharged, and then the extraction tank is subjected to another extraction. Add solvent. This means an extraction method (extraction method) in which this operation is repeated 1 to 3 times.

また、第１抽出工程から第３抽出工程のいずれにおいても、抽出に用いる装置の種類を特に限定するものではないが、複数の抽出釜とバスケットとを備えた装置を使用するのが好ましい。第２抽出工程以降の抽出工程において、茶殻をバスケットごと別の抽出釜に速やかに移すことができ、茶殻の冷却を抑えることができるからである。   In any of the first extraction process to the third extraction process, the type of apparatus used for extraction is not particularly limited, but it is preferable to use an apparatus including a plurality of extraction kettles and baskets. This is because, in the extraction process after the second extraction process, the tea husk can be quickly transferred to another extraction kettle together with the basket, and cooling of the tea husk can be suppressed.

本実施形態の製造方法は、第１抽出工程の後、第２抽出工程、好ましくはさらに第３抽出工程を行い、各工程で得られた抽出液を混合するというものである。この際、第３抽出工程以後、第２若しくは第３抽出工程と同様の抽出工程を繰り返すことも可能である。但し、第３抽出工程以後に抽出を繰り返してもカテキン類の抽出率は顕著に向上せず、抽出液量の増加を考慮すると、かえってカテキン類濃度が低下する可能性があるから、第３抽出工程までに留めるのが好ましい。   The manufacturing method of this embodiment performs a 2nd extraction process after the 1st extraction process, Preferably a 3rd extraction process is performed, and the extract obtained at each process is mixed. At this time, after the third extraction step, it is also possible to repeat the same extraction step as the second or third extraction step. However, even if the extraction is repeated after the third extraction step, the extraction rate of catechins is not significantly improved, and considering the increase in the amount of the extract, the concentration of catechins may be lowered. It is preferable to stop by the process.

第２若しくは第３抽出工程以後、必要に応じて、不溶性物除去或いは清澄性を高めるために、遠心分離、珪藻土濾過などの濾過処理を行ってもよい。   After the second or third extraction step, if necessary, filtration treatment such as centrifugation or diatomaceous earth filtration may be performed in order to remove insoluble matters or improve the clarification.

（茶抽出液の利用）
得られた茶抽出液は、例えば必要に応じて精製した後に濃縮乃至乾燥させて濃縮液或いは乾燥エキスに調製して飲食品添加物、薬理成分などとして利用することができる。また、茶抽出液をそのまま或いは希釈して飲料として利用することもできる。 (Use of tea extract)
The obtained tea extract can be used as a food / drink additive, a pharmacological component, etc., for example, after refine | purifying as needed, concentrating thru | or drying, preparing to a concentrate or a dry extract. The tea extract can be used as a beverage as it is or after dilution.

ここで、カテキン高含有組成物に調製する場合の具体的な処理方法を説明すると、例えば、合成樹脂吸着剤や親水性ビニルポリマーなどを充填したカラムに抽出液を通液し、水でカラムを洗浄した後、含水有機溶媒（アルコール類など）を通液して吸着剤に吸着しているカテキン類やカフェインを回収し、カテキン高含有組成物或いはカフェイン高含有組成物を得ることができる。また、強酸性の陽イオン交換樹脂を充填したカラムに抽出液を通液し、カフェインの低減された通過液を得、これよりカテキン高含有組成物を得ることもできる。
さらに、これらの工程の後、さらにクロマト分離を行い、個々のカテキン類を分離してもよい。 Here, a specific processing method when preparing a high catechin-containing composition will be described. For example, the extract is passed through a column filled with a synthetic resin adsorbent or a hydrophilic vinyl polymer, and the column is filled with water. After washing, a water-containing organic solvent (alcohol or the like) is passed through to collect catechins and caffeine adsorbed on the adsorbent, thereby obtaining a catechin-rich composition or a caffeine-rich composition. . Alternatively, the extract can be passed through a column packed with a strongly acidic cation exchange resin to obtain a passing liquid with reduced caffeine, and thus a catechin-rich composition can be obtained.
Furthermore, after these steps, further chromatographic separation may be performed to separate individual catechins.

以下、本発明を実施例に基づいて説明するが、本発明は実施例に限定されるものではない。
先ず、実施例及び比較例の評価方法について説明する。 EXAMPLES Hereinafter, although this invention is demonstrated based on an Example, this invention is not limited to an Example.
First, the evaluation method of an Example and a comparative example is demonstrated.

＜カテキン類の定量方法＞
実施例及び比較例で得られた茶抽出液のカテキン類の定量はＨＰＬＣ法により行い、その定量条件は「Journal of Food Composition and Analysis、Vol.17、p.675〜685、2004年」に従った。詳しくは以下のとおりである。 <Method for quantifying catechins>
The catechins in the tea extracts obtained in the examples and comparative examples were quantified by HPLC, and the quantification conditions were in accordance with `` Journal of Food Composition and Analysis, Vol. 17, p.675-685, 2004 ''. It was. Details are as follows.

（ＨＰＬＣ条件）
ＨＰＬＣ装置：島津ＬＣ−１０ＡＤ二液高圧グラジエントシステム
カラム：Ｗａｋｏｓｉｌ−ＩＩ ５Ｃ１８ＨＧ（３．０ｍｍ Ｉ．Ｄ．×１５０ｍｍ）
カラム温度：４０℃
移動相Ａ：水−メタノール−りん酸（８５：１５：０．１）
移動相Ｂ：水−メタノール−酢酸エチル−りん酸（８５：１５：１：０．１）
検出：ＵＶ ２８０ｎｍ
試料注入量：５μＬ
グラジエントプログラム：移動相Ａを１００％、流速を０．３ｍＬ／分で分析開始から１２分まで流し、その後１分間で流速を０．４５ｍＬ／分にリニアに上昇させた。以降１９分まで流速を保持し、その後１分間で流速を１．０ｍＬ／分に、移動相Ｂを０％から１００％にリニアに上昇させた。以降４０分まで流速を保持した。 (HPLC conditions)
HPLC apparatus: Shimadzu LC-10AD two-component high pressure gradient system Column: Wakosil-II 5C18HG (3.0 mm ID × 150 mm)
Column temperature: 40 ° C
Mobile phase A: water-methanol-phosphoric acid (85: 15: 0.1)
Mobile phase B: water-methanol-ethyl acetate-phosphoric acid (85: 15: 1: 0.1)
Detection: UV 280nm
Sample injection volume: 5 μL
Gradient program: 100% mobile phase A and a flow rate of 0.3 mL / min were allowed to flow for 12 minutes from the start of the analysis, and then the flow rate was linearly increased to 0.45 mL / min in 1 minute. Thereafter, the flow rate was maintained until 19 minutes, and thereafter, the flow rate was increased linearly from 0% to 100% and the flow rate was increased to 1.0 mL / min in 1 minute. Thereafter, the flow rate was maintained until 40 minutes.

（標準液の調製）
ＥＧＣ，ＥＧＣｇ，ＥＣ，ＥＣｇ，ＧＣ，ＧＣｇ，Ｃ及びＣｇの各１０ｍｇを１００ｍＬのメスフラスコに秤取し、０．５％アスコルビン酸−０．０１％ＥＤＴＡ二ナトリウム水溶液に溶解し、定容した。この溶液を２倍または５倍に希釈した。分析前に０．４５μＬバーサポアフィルタを通過させた。 (Preparation of standard solution)
10 mg each of EGC, EGCg, EC, ECg, GC, GCg, C and Cg was weighed into a 100 mL volumetric flask, dissolved in 0.5% ascorbic acid-0.01% disodium EDTA aqueous solution, and the volume was adjusted. . This solution was diluted 2 or 5 times. Passed through a 0.45 μL Versapore filter prior to analysis.

（分析試料の調製）
実施例及び比較例で得られた茶抽出液を水で１Ｌに定容した後に１０倍に希釈し、各溶液を０．４５μＬバーサポアフィルタを通過させて分析試料とした。
但し、比較例６で得られた茶抽出液は水で２Ｌに定容した後に５倍に希釈した。また、実施例５の茶抽出物は、水に溶解して５００ｐｐｍに調整した。 (Preparation of analysis sample)
The tea extracts obtained in Examples and Comparative Examples were made up to 1 L with water and then diluted 10 times, and each solution was passed through a 0.45 μL Versapore filter to make an analytical sample.
However, the tea extract obtained in Comparative Example 6 was diluted to 5 times after being made up to 2 L with water. Moreover, the tea extract of Example 5 was dissolved in water and adjusted to 500 ppm.

（測定方法）
未希釈、２倍希釈、５倍希釈の標準液を用いてＨＰＬＣ分析を行い、得られたクロマトグラムの各成分のピーク面積と成分濃度で検量線を作成し、その検量線を用いて分析試料用液中の各成分の濃度を求めた。 (Measuring method)
Perform HPLC analysis using undiluted, 2-fold diluted, and 5-fold diluted standard solutions, create a calibration curve with the peak area and component concentration of each component in the resulting chromatogram, and use the calibration curve for analysis samples The concentration of each component in the working solution was determined.

なお、「総カテキン含有量」は、（−）ＥＧＣ、（−）ＥＧＣｇ、（−）ＥＣ、（−）ＥＣｇ、（−）ＧＣ、（−）ＧＣｇ、（−）Ｃ、（−）Ｃｇの８種の合計含有量として求めた。
また、「熱異性化カテキン含有量」は、（−）ＧＣ、（−）ＧＣｇ、（−）Ｃ、（−）Ｃｇの４種類の合計含有量として求めた。
「熱異性化率」は、総カテキン含有量における熱異性化カテキン含有量の割合の意であり、以下の式（Ａ）により求めた。 In addition, "total catechin content" is (-) EGC, (-) EGCg, (-) EC, (-) ECg, (-) GC, (-) GCg, (-) C, (-) Cg. It calculated | required as total content of 8 types.
The “thermal isomerized catechin content” was determined as the total content of four types of (−) GC, (−) GCg, (−) C, and (−) Cg.
“Thermal isomerization rate” means the ratio of the heat isomerized catechin content to the total catechin content, and was determined by the following formula (A).

（熱異性化カテキン含有量）÷（総カテキン含有量）×１００（％）・・・（Ａ）   (Thermal isomerization catechin content) ÷ (total catechin content) × 100 (%) (A)

「抽出率」は、茶葉に含まれているカテキン類が抽出により回収される割合の意であり、以下の式（Ｂ）により求めた。   “Extraction rate” means the ratio of catechins contained in tea leaves recovered by extraction, and was determined by the following formula (B).

（（抽出液質量或いは容量）×（抽出液の成分濃度（ｐｐｍ））÷１０００）÷（（抽出に使用した茶葉質量）×（茶葉の成分含有量（％））÷１００）×１００ ・・・・・・・・・・（Ｂ）   ((Extract liquid mass or volume) × (Extract liquid component concentration (ppm)) ÷ 1000) ÷ ((tea leaf mass used for extraction) × (tea leaf component content (%)) ÷ 100) × 100 ... (B)

なお、茶葉の成分含量（表１）は以下の方法により測定した。
茶葉はミルで粉砕し、目開き５００μｍの篩を通過させた。粉砕した茶葉１００ｍｇを１００ｍＬのメスフラスコへ秤量し、８０℃の温水を約８０ｍＬ注いで、８０℃の湯浴中で３０分間抽出した。抽出後冷水で冷却を行い、水で１００ｍＬに定容し、濾紙（ＪＩＳ Ｎｏ．２）で濾過して、濾液を０．４５μＬバーサポアフィルタに通過させ、ＨＰＬＣで定量分析を行った。 The component content of tea leaves (Table 1) was measured by the following method.
The tea leaves were pulverized by a mill and passed through a sieve having an opening of 500 μm. 100 mg of crushed tea leaves were weighed into a 100 mL volumetric flask, about 80 mL of 80 ° C. warm water was poured, and the mixture was extracted in an 80 ° C. hot water bath for 30 minutes. After extraction, the mixture was cooled with cold water, adjusted to 100 mL with water, filtered through a filter paper (JIS No. 2), the filtrate was passed through a 0.45 μL Versapore filter, and quantitative analysis was performed by HPLC.

（実施例１）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れた後、温水３００ｍＬを入れて７０℃に加温した。次いで、前記籠の中に中国産緑茶葉３０ｇを入れ、７０℃の湯浴上で適宜攪拌しながら１０分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管した。
前記抽出の固液分離の開始から２分以内に、７０℃の温水３００ｍＬを入れた１Ｌ容量のガラスビーカーに、茶殻の入った籠を入れて沈め、７０℃の湯浴上で適宜攪拌しながら１０分間の再抽出を行なった。再抽出後、１回目と同様に固液分離及びろ過を行い、得られた抽出液を３０℃以下に冷却した後、先に得られた抽出液と混合し、合計４８２ｇの抽出液（ｐＨ５．５）を得た。 (Example 1)
A cylindrical stainless steel bottle (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L capacity glass beaker (inner diameter 105 mm, depth 150 mm), and then 300 mL of hot water was added and heated to 70 ° C. Next, 30 g of Chinese green tea leaves were put into the koji, and extraction was performed for 10 minutes with appropriate stirring on a 70 ° C. hot water bath. After extraction, the koji containing the tea husk was pulled up from the beaker and subjected to solid-liquid separation. The extract was filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the extraction, put the straw containing the tea husk into a 1 L glass beaker containing 300 mL of hot water at 70 ° C., and stir appropriately in a 70 ° C. hot water bath. Re-extraction for 10 minutes was performed. After re-extraction, solid-liquid separation and filtration were performed in the same manner as in the first time, and the obtained extract was cooled to 30 ° C. or lower and then mixed with the previously obtained extract to give a total of 482 g of extract (pH 5. 5) was obtained.

なお、抽出に用いた温水は、全てイオン交換水（ｐＨ６．５）であり、以下の実施例及び比較例においても同様である。   In addition, all the warm water used for extraction is ion-exchange water (pH 6.5), and it is the same also in the following Examples and Comparative Examples.

（実施例２）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れた後、温水３００ｍＬを入れて７０℃に加温した。次いで、前記籠の中に中国産緑茶葉３０ｇを入れ、７０℃の湯浴上で適宜攪拌しながら１０分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管した。
前記抽出の固液分離の開始から２分以内に、９０℃の温水３００ｍＬを入れた１Ｌ容量のガラスビーカーに、茶殻の入った籠を入れて沈め、９０℃の湯浴上で適宜攪拌しながら１０分間の再抽出を行なった。再抽出後、１回目と同様に固液分離及びろ過を行い、得られた抽出液を３０℃以下に冷却した後、先に得られた抽出液と混合し、合計４９８ｇの抽出液（ｐＨ５．５）を得た。 (Example 2)
A cylindrical stainless steel bottle (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L capacity glass beaker (inner diameter 105 mm, depth 150 mm), and then 300 mL of hot water was added and heated to 70 ° C. Next, 30 g of Chinese green tea leaves were put into the koji, and extraction was performed for 10 minutes with appropriate stirring on a 70 ° C. hot water bath. After extraction, the koji containing the tea husk was pulled up from the beaker and subjected to solid-liquid separation. The extract was filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the extraction, put the straw containing the tea husk into a 1 L glass beaker containing 300 mL of hot water at 90 ° C., and appropriately stir in a 90 ° C. hot water bath. Re-extraction for 10 minutes was performed. After re-extraction, solid-liquid separation and filtration were performed in the same manner as in the first time, and the obtained extract was cooled to 30 ° C. or lower and then mixed with the previously obtained extract to give a total of 498 g of extract (pH 5. 5) was obtained.

（実施例３）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れた後、温水３００ｍＬを入れて７０℃に加温した。次いで、籠の中に中国産緑茶葉３０ｇを入れ、７０℃の湯浴上で適宜攪拌しながら１５分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管した。
前記抽出の固液分離の開始から２分以内に、９０℃の温水３００ｍＬを入れた１Ｌ容量のガラスビーカーに、茶殻の入った籠を入れて沈め、９０℃の湯浴上で適宜攪拌しながら５分間の再抽出を行なった。再抽出後、１回目と同様に固液分離及びろ過を行い、得られた抽出液を３０℃以下に冷却した後、先に得られた抽出液と混合し、合計４８５ｇの抽出液（ｐＨ５．５）を得た。 (Example 3)
A cylindrical stainless steel bottle (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L capacity glass beaker (inner diameter 105 mm, depth 150 mm), and then 300 mL of hot water was added and heated to 70 ° C. Next, 30 g of Chinese green tea leaves were put into the koji, and extraction was performed for 15 minutes with appropriate stirring on a 70 ° C. hot water bath. After extraction, the koji containing the tea husk was pulled up from the beaker and subjected to solid-liquid separation. The extract was filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the extraction, put the straw containing the tea husk into a 1 L glass beaker containing 300 mL of hot water at 90 ° C., and appropriately stir in a 90 ° C. hot water bath. Re-extraction for 5 minutes was performed. After the re-extraction, solid-liquid separation and filtration were performed in the same manner as in the first time, and the obtained extract was cooled to 30 ° C. or lower and then mixed with the previously obtained extract to obtain a total of 485 g of extract (pH 5. 5) was obtained.

（実施例４）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れた後、温水３００ｍＬを入れて７０℃に加温した。次いで、籠の中に中国産緑茶葉３０ｇを入れ、７０℃の湯浴上で適宜攪拌しながら１０分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管した。
前記抽出の固液分離の開始から２分以内に、９０℃の温水３００ｍＬを入れた１Ｌ容量のガラスビーカーに、茶殻の入った籠を入れて沈め、９０℃の湯浴上で適宜攪拌しながら５分間の再抽出を行なった。再抽出後、１回目と同様に固液分離及びろ過を行い、得られた抽出液を３０℃以下に冷却し保管した。
前記再抽出の固液分離の開始から２分以内に、９０℃の温水２００ｍＬを入れた１Ｌ容量のガラスビーカーに、前工程の抽出残渣である茶殻の入った籠を入れて沈め、９０℃の湯浴上で適宜攪拌しながら５分間の再々抽出を行なった。再々抽出後、１回目と同様に固液分離及びろ過を行い、得られた抽出液を３０℃以下に冷却し、以上３回の抽出液を混合し、６８６ｇの抽出液（ｐＨ５．５）を得た。 Example 4
A cylindrical stainless steel bottle (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L capacity glass beaker (inner diameter 105 mm, depth 150 mm), and then 300 mL of hot water was added and heated to 70 ° C. Next, 30 g of Chinese green tea leaves were placed in the koji, and extraction was performed for 10 minutes with appropriate stirring on a 70 ° C. hot water bath. After extraction, the koji containing the tea husk was pulled up from the beaker and subjected to solid-liquid separation. The extract was filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the extraction, put the straw containing the tea husk into a 1 L glass beaker containing 300 mL of hot water at 90 ° C., and appropriately stir in a 90 ° C. hot water bath. Re-extraction for 5 minutes was performed. After re-extraction, solid-liquid separation and filtration were performed as in the first time, and the obtained extract was cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the re-extraction, put the straw filled with tea leaves, which is the extraction residue of the previous step, into a 1 L glass beaker containing 200 mL of hot water at 90 ° C. Extraction was performed again for 5 minutes with appropriate stirring on a hot water bath. After re-extraction, solid-liquid separation and filtration were performed in the same manner as in the first time, and the obtained extract was cooled to 30 ° C. or lower, and the extract was mixed three times to obtain 686 g of extract (pH 5.5). Obtained.

（比較例１）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れた後、温水６００ｍＬを入れて７０℃に加温した。次いで、籠の中に中国産緑茶葉３０ｇを入れ、７０℃の湯浴上で適宜攪拌しながら２０分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管し、４７９ｇの抽出液（ｐＨ５．５）を得た。 (Comparative Example 1)
A cylindrical stainless steel bowl (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L capacity glass beaker (inner diameter 105 mm, depth 150 mm), and then 600 mL of hot water was added and heated to 70 ° C. Next, 30 g of Chinese green tea leaves were placed in the koji, and extraction was performed for 20 minutes with appropriate stirring on a 70 ° C. hot water bath. After extraction, the cocoon containing the tea husk is pulled up from the beaker and separated into solid and liquid, and the extract is filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or less and stored, and 479 g of extract (pH 5. 5) was obtained.

（比較例２）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れた後、温水３００ｍＬを入れて５０℃に加温した。次いで、籠の中に中国産緑茶葉３０ｇを入れ、５０℃の湯浴上で適宜攪拌しながら１０分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管した。
前記抽出の固液分離の開始から２分以内に、５０℃の温水３００ｍＬを入れた１Ｌ容量のガラスビーカーに、茶殻の入った籠を入れて沈め、５０℃の湯浴上で適宜攪拌しながら１０分間の再抽出を行なった。再抽出後、１回目と同様に固液分離及びろ過を行い、得られた抽出液を３０℃以下に冷却した後、先に得られた抽出液と混合し、合計４８６ｇの抽出液（ｐＨ５．５）を得た。 (Comparative Example 2)
A cylindrical stainless steel bottle (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L capacity glass beaker (inner diameter 105 mm, depth 150 mm), and then 300 mL of hot water was added and heated to 50 ° C. Next, 30 g of Chinese green tea leaves were placed in the koji, and extraction was performed for 10 minutes with appropriate stirring in a 50 ° C. hot water bath. After extraction, the koji containing the tea husk was pulled up from the beaker and subjected to solid-liquid separation. The extract was filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the extraction, put the straw containing the tea husk into a 1 L glass beaker containing 300 mL of hot water at 50 ° C., and stir appropriately in a 50 ° C. hot water bath. Re-extraction for 10 minutes was performed. After re-extraction, solid-liquid separation and filtration were performed in the same manner as in the first time, and the obtained extract was cooled to 30 ° C. or lower, and then mixed with the previously obtained extract to obtain a total of 486 g of extract (pH 5. 5) was obtained.

（比較例３）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れた後、温水６００ｍＬを入れて９０℃に加温した。次いで、籠の中に中国産緑茶葉３０ｇを入れ、９０℃の湯浴上で適宜攪拌しながら２０分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管し、４６９ｇの抽出液（ｐＨ５．５）を得た。 (Comparative Example 3)
A cylindrical stainless steel bottle (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L capacity glass beaker (inner diameter 105 mm, depth 150 mm), and then 600 mL of hot water was added and heated to 90 ° C. Next, 30 g of Chinese green tea leaves were placed in the bowl, and extraction was performed for 20 minutes with appropriate stirring in a 90 ° C. water bath. After extraction, the cocoon containing the tea husk is pulled up from the beaker and separated into solid and liquid. The extract is filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or lower and stored, and 469 g of extract (pH 5. 5) was obtained.

（比較例４）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れた後、温水３００ｍＬを入れて９０℃に加温した。次いで、籠の中に中国産緑茶葉３０ｇを入れ、９０℃の湯浴上で適宜攪拌しながら１０分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管した。
前記抽出の固液分離の開始から２分以内に、９０℃の温水３００ｍＬを入れた１Ｌ容量のガラスビーカーに、茶殻の入った籠を入れて沈め、９０℃の湯浴上で１０分間の再抽出を行なった。抽出後、１回目と同様に固液分離及びろ過を行い、得られた抽出液を３０℃以下に冷却した後、先に得られた抽出液と混合し、合計４５３ｇの抽出液（ｐＨ５．５）を得た。 (Comparative Example 4)
A cylindrical stainless steel bottle (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L glass beaker (inner diameter 105 mm, depth 150 mm), and then 300 mL of hot water was added and heated to 90 ° C. Next, 30 g of Chinese green tea leaves were placed in the koji, and extraction was performed for 10 minutes with appropriate stirring in a 90 ° C. water bath. After extraction, the koji containing the tea husk was pulled up from the beaker and subjected to solid-liquid separation. The extract was filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the extraction, put the straw containing the tea leaves in a 1 L glass beaker containing 300 mL of hot water at 90 ° C., and re-stain for 10 minutes on a 90 ° C. water bath. Extraction was performed. After extraction, solid-liquid separation and filtration were performed in the same manner as in the first time, and the obtained extract was cooled to 30 ° C. or lower and then mixed with the previously obtained extract to obtain a total of 453 g of extract (pH 5.5). )

（比較例５）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れ、ガラスビーカーに温水３００ｍＬを入れて９０℃に加温した。次いで、籠の中に中国産緑茶葉３０ｇを入れ、９０℃の湯浴上で適宜攪拌しながら１０分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管した。
前記抽出の固液分離の開始から２分以内に、７０℃の温水３００ｍＬを入れた１Ｌ容量のガラスビーカーに、茶殻の入った籠を入れて沈め、７０℃の湯浴上で適宜攪拌しながら１０分間の再抽出を行なった。再抽出後、１回目と同様に固液分離及びろ過を行い、得られた抽出液を３０℃以下に冷却した後、先に得られた抽出液と混合し、合計４７８ｇの抽出液（ｐＨ５．５）を得た。 (Comparative Example 5)
A cylindrical stainless steel bottle (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L capacity glass beaker (inner diameter 105 mm, depth 150 mm), and 300 mL of warm water was added to the glass beaker and heated to 90 ° C. . Next, 30 g of Chinese green tea leaves were placed in the koji, and extraction was performed for 10 minutes with appropriate stirring in a 90 ° C. water bath. After extraction, the koji containing the tea husk was pulled up from the beaker and subjected to solid-liquid separation. The extract was filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the extraction, put the straw containing the tea husk into a 1 L glass beaker containing 300 mL of hot water at 70 ° C., and stir appropriately in a 70 ° C. hot water bath. Re-extraction for 10 minutes was performed. After re-extraction, solid-liquid separation and filtration were performed in the same manner as in the first time, and the obtained extract was cooled to 30 ° C. or lower, and then mixed with the previously obtained extract to give a total of 478 g of extract (pH 5. 5) was obtained.

（比較例６）
中国産緑茶葉３０ｇを、内径５０ｍｍ、高さ３５０ｍｍの７０℃に保温したガラスカラムに充填し、７０℃の温水を上方から下方に１００ｍＬ／分の速度で通液して抽出液を得た。得られた抽出液は速やかに３０℃以下に冷却し、抽出液が１２００ｍＬになった段階で回収を終了した。 (Comparative Example 6)
30 g of green tea leaves from China were packed into a glass column kept at 70 ° C. having an inner diameter of 50 mm and a height of 350 mm, and 70 ° C. warm water was passed from above to below at a rate of 100 mL / min to obtain an extract. The obtained extract was quickly cooled to 30 ° C. or less, and the recovery was completed when the extract reached 1200 mL.

（実施例５）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に円筒形のステンレス製の籠（内径９３ｍｍ、深さ７７ｍｍ、目開き１ｍｍ）を入れた後、温水３００ｍＬを入れて７５℃に加温した。次いで、前記籠の中に中国産緑茶葉３０ｇを入れ、７５℃の湯浴上で適宜攪拌しながら１５分間抽出を行った。抽出後、茶殻の入った籠をビーカーから引き上げて固液分離し、抽出液を目開き１８０μｍの金属メッシュでろ過した後、速やかに３０℃以下に冷却し保管した。
前記抽出の固液分離の開始から２分以内に、８０℃の温水３００ｍＬを入れた１Ｌ容量のガラスビーカーに、茶殻の入った籠を入れて沈め、８０℃の湯浴上で適宜攪拌しながら１０分間の再抽出を行なった。再抽出後、１回目と同様に固液分離・濾過を行い、得られた抽出液を３０℃以下に冷却した後、先に得られた抽出液と混合し、合計４８０ｇの抽出液（ｐＨ５．５）を得た。この抽出液を、３０００ｒｐｍ×１０分で遠心分離し、得られた上清を減圧濃縮し、次いで凍結乾燥を行い、茶抽出物７．１ｇを得た。 (Example 5)
A cylindrical stainless steel bottle (inner diameter 93 mm, depth 77 mm, opening 1 mm) was placed in a 1 L capacity glass beaker (inner diameter 105 mm, depth 150 mm), and then 300 mL of hot water was added and heated to 75 ° C. Next, 30 g of Chinese green tea leaves were placed in the koji, and extracted for 15 minutes with appropriate stirring in a 75 ° C. hot water bath. After extraction, the koji containing the tea husk was pulled up from the beaker and subjected to solid-liquid separation. The extract was filtered through a metal mesh having an opening of 180 μm, and then quickly cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the extraction, put the straw filled with tea husk into a 1 L glass beaker containing 300 mL of hot water at 80 ° C., and stir appropriately in a hot water bath at 80 ° C. Re-extraction for 10 minutes was performed. After re-extraction, solid-liquid separation and filtration were performed in the same manner as in the first time, and the obtained extract was cooled to 30 ° C. or lower and then mixed with the previously obtained extract to obtain a total of 480 g of extract (pH 5. 5) was obtained. This extract was centrifuged at 3000 rpm × 10 minutes, and the resulting supernatant was concentrated under reduced pressure, followed by lyophilization to obtain 7.1 g of a tea extract.

（実施例６）
中国産緑茶葉１０ｇを７５℃の温水１００ｍＬに浸漬し、７５℃の湯浴上で適宜攪拌しながら１５分間の抽出を行った。抽出後、目開き１８０μｍの金属メッシュで固液分離を行い、得られた抽出液を３０℃以下に冷却し保管した。
前記抽出の固液分離の開始から２分以内に、前記抽出後の茶殻を８０℃の温水８０ｍＬ中に投入し、８０℃の湯浴上で適宜攪拌しながら１０分間の再抽出を行った。
再抽出後、１回目と同様に固液分離を行い、得られた抽出液を３０℃以下に冷却した後、１回目の抽出液と混合して抽出液を得た。この抽出液を、３０００ｒｐｍ×１０分で遠心分離し、得られた上清を水でＢｒｉｘ０．３となるように希釈してＰＥＴボトルに充填してＰＥＴボトル詰茶飲料を得た。 (Example 6)
10 g of green tea leaves from China were immersed in 100 mL of 75 ° C. hot water, and extracted for 15 minutes in a 75 ° C. hot water bath with appropriate stirring. After extraction, solid-liquid separation was performed with a metal mesh having an opening of 180 μm, and the resulting extract was cooled to 30 ° C. or lower and stored.
Within 2 minutes from the start of the solid-liquid separation of the extraction, the extracted tea husk was put into 80 mL of hot water at 80 ° C., and re-extraction was carried out for 10 minutes while appropriately stirring in an 80 ° C. hot water bath.
After re-extraction, solid-liquid separation was performed in the same manner as in the first time, and the resulting extract was cooled to 30 ° C. or lower and then mixed with the first time to obtain an extract. This extract was centrifuged at 3000 rpm × 10 minutes, and the resulting supernatant was diluted with water to a Brix of 0.3 and filled into a PET bottle to obtain a PET bottled tea beverage.

以上の実施例及び比較例の結果をまとめて表５に示した。これより、次の点が明らかとなった。
・実施例１と比較例１は同じ温度で、総加水量と総抽出時間が等しい条件での抽出であるが、カテキン類の抽出率は１０％以上の差が見られた。
・実施例１と比較例２では、温度以外の条件は同じであるが、比較例２ではカテキン抽出率が低く、特にＥＧＣｇの抽出率に約１０％の差が見られた。
・比較例３及び４では９０℃で抽出を行い、特に比較例３では高いカテキン回収率が得られたが、カテキン類の熱異性化率が１０％以上と高くなっていた。実施例２及び３では二段階目を９０℃で抽出しているが、カテキン類の熱異性化率は実施例１とほとんど変わっていなかった。
・比較例５では、実施例１と二段階の抽出での温度を逆にしたが、カテキン類の熱異性化率が高く、一段階目を低温で抽出することが重要であることが示された。
・比較例６は、カラム抽出法であり、カテキン類の熱異性化率は低いが、高いカテキン抽出率を得ようとすると、得られる抽出液のカテキン濃度が低下することが見て取れる。
・実施例４の三段階抽出は比較例６よりもカテキン抽出率と得られる抽出液のカテキン濃度の面で効率的といえる。
・実施例５では、７５℃と８０℃の二段階抽出を行い、凍結乾燥により粉末エキスを製造した。得られた粉末エキスは、カテキンの異性化率が６．２％であり、原料茶葉の異性化率と大差ないものであった。
・実施例６では、実施例５と同様の抽出液をＢｒｉｘ０．３に調製してＰＥＴ詰茶飲料を製造した。得られた飲料は、一般的な茶飲料よりも高濃度のカテキンを含有しており、カテキンの異性化率が低く、ＥＧＣｇ含量が高いものであった。 The results of the above Examples and Comparative Examples are summarized in Table 5. From this, the following points became clear.
-Although Example 1 and Comparative Example 1 were extraction on the conditions with the same temperature and total water content and total extraction time, the extraction rate of catechins showed the difference of 10% or more.
In Example 1 and Comparative Example 2, the conditions other than the temperature were the same, but in Comparative Example 2, the catechin extraction rate was low, and in particular, a difference of about 10% was found in the EGCg extraction rate.
In Comparative Examples 3 and 4, extraction was performed at 90 ° C., and in particular, high catechin recovery was obtained in Comparative Example 3, but the thermal isomerization rate of catechins was as high as 10% or more. In Examples 2 and 3, the second stage was extracted at 90 ° C., but the thermal isomerization rate of catechins was almost the same as in Example 1.
In Comparative Example 5, the temperature in the two-stage extraction was reversed from that in Example 1, but it was shown that the thermal isomerization rate of catechins is high and it is important to extract the first stage at a low temperature. It was.
Comparative Example 6 is a column extraction method, and although the thermal isomerization rate of catechins is low, it can be seen that the catechin concentration of the resulting extract decreases when trying to obtain a high catechin extraction rate.
The three-stage extraction of Example 4 is more efficient than Comparative Example 6 in terms of the catechin extraction rate and the catechin concentration of the resulting extract.
In Example 5, two-stage extraction at 75 ° C. and 80 ° C. was performed, and a powder extract was produced by lyophilization. The obtained powder extract had an isomerization rate of catechin of 6.2% and was not significantly different from the isomerization rate of the raw tea leaves.
-In Example 6, the same extract as in Example 5 was prepared in Brix 0.3 to produce a PET-stuffed tea beverage. The obtained beverage contained a higher concentration of catechin than a general tea beverage, had a low catechin isomerization rate and a high EGCg content.

（試験例１〜８）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に温水４００ｍＬを入れて指定水温I＋５℃に調整した後、中国産緑茶葉４０ｇを投入し、指定水温Iの湯浴上で１５分間の１回目の抽出を行なった。抽出後、ビーカー内容物を目開き１０６μｍの金属メッシュでろ過し、濾液（抽出液）は速やかに３０℃以下に冷却した。
茶殻は、固液分離後速やかにビーカーに戻し、指定水温II＋５℃の温水３２０ｍＬを注ぎ、指定水温IIの湯浴上で１０分間の２回目の抽出を行ない、抽出後、１回目と同様に固液分離および濾過を行い、得られた抽出液を３０℃以下に冷却した。
そして、２回目の抽出で得られた抽出液を１回目の抽出で得られた抽出液に混合して混合抽出液（表７の抽出液回収量）を得た。なお、指定水温IIは指定水温I＋１０℃に設定した。
得られた混合抽出液のＥＧＣｇ濃度、総カテキン濃度、異性化率、ＥＧＣｇ抽出率、総カテキン抽出率を測定し、各項目について各基準に基づいて（表８の備考参照）判定を行なうとともに総合的な判定も行ない、結果を表８に示した。
なお、カテキン類の定量方法は、前述の実施例と同様に行なった（後述する試験例でも同様である）。 (Test Examples 1-8)
A 1-liter glass beaker (inner diameter: 105 mm, depth: 150 mm) is charged with 400 mL of hot water and adjusted to the specified water temperature I + 5 ° C. Then, 40 g of green tea leaves from China are introduced, and the first time for 15 minutes on the water bath with the specified water temperature I. Was extracted. After extraction, the contents of the beaker were filtered through a metal mesh having an opening of 106 μm, and the filtrate (extract) was quickly cooled to 30 ° C. or lower.
The tea husk is immediately returned to the beaker after solid-liquid separation, poured with 320 mL of hot water at the specified water temperature II + 5 ° C, extracted for the second time for 10 minutes in a hot water bath at the specified water temperature II, and after extraction, the tea cake is hardened as in the first time. Liquid separation and filtration were performed, and the obtained extract was cooled to 30 ° C. or lower.
And the extract obtained by the 2nd extraction was mixed with the extract obtained by the 1st extraction, and the mixed extract (the extract collection amount of Table 7) was obtained. The designated water temperature II was set to the designated water temperature I + 10 ° C.
The EGCg concentration, total catechin concentration, isomerization rate, EGCg extraction rate, and total catechin extraction rate of the obtained mixed extract are measured, and each item is determined based on each criterion (see the remarks in Table 8) and comprehensively determined. Judgment was also made and the results are shown in Table 8.
The method for quantifying catechins was carried out in the same manner as in the previous examples (the same applies to test examples described later).

１回目の抽出の温度は抽出効率に影響することを確認した。試験例１（５０℃）は、試験例２〜８と比較して明確に抽出率が低下することが確認された。
また、１回目の抽出の温度が高いと、抽出効率の向上が見られる一方で、カテキンの異性化が進み易いことを確認した。特に試験例８の９０℃では異性化率が６．０％を超え、試験例１〜７と明確な差が確認された。
このことより、１回目の抽出の抽出温度は５５〜８０℃が好ましく、６０〜８０℃が特に好ましいと考えられる。 It was confirmed that the temperature of the first extraction affects the extraction efficiency. In Test Example 1 (50 ° C.), it was confirmed that the extraction rate was clearly reduced as compared with Test Examples 2-8.
Moreover, when the temperature of the 1st extraction was high, while improving the extraction efficiency was seen, it confirmed that the isomerization of catechin progressed easily. In particular, at 90 ° C. in Test Example 8, the isomerization rate exceeded 6.0%, and a clear difference from Test Examples 1 to 7 was confirmed.
From this, it is considered that the extraction temperature of the first extraction is preferably 55 to 80 ° C, and particularly preferably 60 to 80 ° C.

（試験例９〜１４）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に温水４００ｍＬを入れて８０℃に調整した後、中国産緑茶葉４０ｇを投入し、７５℃の湯浴上で１５分間の１回目の抽出を行なった。抽出後、ビーカー内容物を目開き１０６μｍの金属メッシュでろ過し、濾液（抽出液）は速やかに３０℃以下に冷却した。
茶殻は、固液分離後速やかにビーカーに戻し、指定水温III＋５℃の温水３２０ｍＬを注ぎ、指定水温IIIの湯浴上で１０分間の２回目の抽出を行ない、抽出後、１回目と同様に固液分離および濾過を行い、得られた抽出液を３０℃以下に冷却した。
そして、２回目の抽出で得られた抽出液を１回目の抽出で得られた抽出液に混合して混合抽出液（表９の抽出液回収量）を得た。
得られた混合抽出液のＥＧＣｇ濃度、総カテキン濃度、異性化率、ＥＧＣｇ抽出率、総カテキン抽出率を測定し、各項目について各基準に基づいて（表１０の備考参照）判定を行なうとともに総合的な判定も行ない、結果を表１０に示した。 (Test Examples 9 to 14)
In a 1 L glass beaker (inner diameter 105 mm, depth 150 mm), add 400 mL of warm water to 80 ° C., and then add 40 g of Chinese green tea leaves and extract for the first time in a 75 ° C. water bath for 15 minutes. I did it. After extraction, the contents of the beaker were filtered through a metal mesh having an opening of 106 μm, and the filtrate (extract) was quickly cooled to 30 ° C. or lower.
After the solid-liquid separation, the tea husk is immediately returned to the beaker, poured with 320 mL of hot water at the specified water temperature III + 5 ° C, extracted for the second time for 10 minutes in the hot water bath at the specified water temperature III, and after extraction, the tea cake is hardened in the same way as the first time. Liquid separation and filtration were performed, and the obtained extract was cooled to 30 ° C. or lower.
And the extract obtained by the 2nd extraction was mixed with the extract obtained by the 1st extraction, and the mixed extract (the extract collection amount of Table 9) was obtained.
Measure the EGCg concentration, total catechin concentration, isomerization rate, EGCg extraction rate, total catechin extraction rate of the resulting mixed extract, and make a judgment based on each criterion (see the remarks in Table 10) for each item. The results are shown in Table 10.

２回目の抽出の水温（抽出温度）も、１回目の抽出と同じく抽出率に影響するが、一度抽出が行なわれた後であるため、高温で抽出した場合のカテキン異性化率への影響は少ないことが確認された。１回目の抽出と同じ温度である試験例９では十分な抽出が行なわれており、加えて試験例１０〜１４でも抽出率は十分に高く、且つ異性化率は６．０％未満であることから、２回目の抽出の抽出温度は、１回目の抽出の抽出温度以上であるのが好ましいことが確認された。   The water temperature (extraction temperature) of the second extraction also affects the extraction rate as in the first extraction, but since it is once extracted, the effect on the catechin isomerization rate when extracted at a high temperature is It was confirmed that there were few. In Test Example 9 at the same temperature as the first extraction, sufficient extraction was performed, and in addition, in Test Examples 10 to 14, the extraction rate was sufficiently high and the isomerization rate was less than 6.0%. From the results, it was confirmed that the extraction temperature of the second extraction is preferably equal to or higher than the extraction temperature of the first extraction.

（試験例１５〜１９）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に温水４００ｍＬを入れて８０℃に調整した後、中国産緑茶葉４０ｇを投入し、７５℃の湯浴上で１５分間の１回目の抽出を行なった。抽出後、ビーカー内容物を目開き１０６μｍの金属メッシュでろ過し、濾液（抽出液）は速やかに３０℃以下に冷却した。
茶殻は、固液分離後速やかにビーカーに戻し、９５℃の熱水３２０ｍＬを注ぎ、９０℃の湯浴上で指定時間Iの２回目の抽出を行ない、抽出後、１回目と同様に固液分離および濾過を行い、得られた抽出液を３０℃以下に冷却した。
そして、２回目の抽出で得られた抽出液を１回目の抽出で得られた抽出液に混合して混合抽出液（表１１の抽出液回収量）を得た。
得られた混合抽出液のＥＧＣｇ濃度、総カテキン濃度、異性化率、ＥＧＣｇ抽出率、総カテキン抽出率を測定し、各項目について各基準に基づいて（表１２の備考参照）判定を行なうとともに総合的な判定も行ない、結果を表１２に示した。 (Test Examples 15 to 19)
In a 1 L glass beaker (inner diameter 105 mm, depth 150 mm), add 400 mL of warm water to 80 ° C., and then add 40 g of Chinese green tea leaves and extract for the first time in a 75 ° C. water bath for 15 minutes. I did it. After extraction, the contents of the beaker were filtered through a metal mesh having an opening of 106 μm, and the filtrate (extract) was quickly cooled to 30 ° C. or lower.
The tea husk is immediately returned to the beaker after solid-liquid separation, poured with 320 mL of hot water at 95 ° C., extracted for the second time at the specified time I on a 90 ° C. hot water bath, and after extraction, the solid and liquid are the same as in the first time. Separation and filtration were performed, and the resulting extract was cooled to 30 ° C. or lower.
And the extract obtained by the 2nd extraction was mixed with the extract obtained by the 1st extraction, and the mixed extract (the extract collection amount of Table 11) was obtained.
The EGCg concentration, total catechin concentration, isomerization rate, EGCg extraction rate, and total catechin extraction rate of the obtained mixed extract are measured, and each item is determined based on each criterion (see the remarks in Table 12) and comprehensively determined. Judgment was also made and the results are shown in Table 12.

２回目の抽出の抽出時間は、短時間、具体的には１分以下でもカテキンを充分に抽出できる。その一方、長時間になるとカテキンの異性化等に影響を及ぼすことが確認された。特に２回目の抽出を３０分行なった試験例１９ではカテキンの異性化率が顕著に上昇した。このことより、２回目の抽出の抽出時間は、１回目の抽出の抽出時間以下であるのが好ましく、１回目の抽出の抽出時間が１５分以上である場合でも、２回目の抽出の抽出時間は１５分以内とするのが好ましく、カテキンの抽出率と異性化率の両方を考慮すると５分〜１５分が特に好ましいと考えられる。   The catechin can be sufficiently extracted even if the extraction time of the second extraction is short, specifically, 1 minute or less. On the other hand, it was confirmed that the catechin isomerization and the like were affected over a long period of time. In particular, in Test Example 19 in which the second extraction was performed for 30 minutes, the isomerization rate of catechin was significantly increased. Accordingly, the extraction time of the second extraction is preferably equal to or shorter than the extraction time of the first extraction, and even if the extraction time of the first extraction is 15 minutes or more, the extraction time of the second extraction Is preferably within 15 minutes, and in consideration of both the extraction rate of catechin and the isomerization rate, 5 to 15 minutes is considered to be particularly preferable.

（試験例２０〜２６）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に温水４００ｍＬを入れて８０℃に調整した後、中国産緑茶葉４０ｇを投入し、７５℃の湯浴上で指定時間IIの１回目の抽出を行なった。抽出後、ビーカー内容物を目開き１０６μｍの金属メッシュでろ過し、濾液（抽出液）は速やかに３０℃以下に冷却した。
茶殻は、固液分離後速やかにビーカーに戻し、８５℃の温水３２０ｍＬを注ぎ、８０℃の湯浴上で指定時間IIIの２回目の抽出を行ない、抽出後、１回目と同様に固液分離および濾過を行い、得られた抽出液を３０℃以下に冷却した。
そして、２回目の抽出で得られた抽出液を１回目の抽出で得られた抽出液に混合して混合抽出液（表１３の抽出液回収量）を得た。
得られた混合抽出液のＥＧＣｇ濃度、総カテキン濃度、異性化率、ＥＧＣｇ抽出率、総カテキン抽出率を測定し、各項目について各基準に基づいて（表１４の備考参照）判定を行なうとともに総合的な判定も行ない、結果を表１４に示した。 (Test Examples 20 to 26)
In a 1 L glass beaker (inner diameter 105 mm, depth 150 mm), add 400 mL of warm water to 80 ° C., then add 40 g of Chinese green tea leaves, and extract for the first time specified time II on a 75 ° C. water bath. Was done. After extraction, the contents of the beaker were filtered through a metal mesh having an opening of 106 μm, and the filtrate (extract) was quickly cooled to 30 ° C. or lower.
The tea husk is returned to the beaker immediately after solid-liquid separation, poured with 320 mL of 85 ° C hot water, and extracted for the second time at the specified time III on an 80 ° C hot water bath. After extraction, the solid-liquid separation is performed in the same manner as the first time. And filtration was performed, and the obtained extract was cooled to 30 ° C. or lower.
And the extract obtained by the 2nd extraction was mixed with the extract obtained by the 1st extraction, and the mixed extract (the extract collection amount of Table 13) was obtained.
The EGCg concentration, total catechin concentration, isomerization rate, EGCg extraction rate, and total catechin extraction rate of the obtained mixed extract are measured, and each item is determined based on each criterion (see the remarks in Table 14) and comprehensively determined. Judgment was also made and the results are shown in Table 14.

１回目の抽出の抽出時間に依存してカテキンの抽出率が向上する一方、カテキンの異性化率も向上することが確認された。１回目の抽出を２分間行なった試験例２０ではカテキン抽出率が４０％以下と低い一方、９０分間行なった試験例２６ではカテキンの異性化率が６．０％以上と高かった。この結果より、１回目の抽出の抽出時間は５分〜６０分が好ましく、１５分〜６０分がより好ましく、中でも１５分〜２０分がさらに好ましいと考えられる。   It was confirmed that the extraction rate of catechin was improved depending on the extraction time of the first extraction, while the isomerization rate of catechin was also improved. In Test Example 20 in which the first extraction was performed for 2 minutes, the catechin extraction rate was as low as 40% or less, whereas in Test Example 26 in which the extraction was performed for 90 minutes, the catechin isomerization rate was as high as 6.0% or more. From this result, the extraction time of the first extraction is preferably 5 to 60 minutes, more preferably 15 to 60 minutes, and more preferably 15 to 20 minutes.

（試験例２７〜３３）
試験例２７〜３０では１Ｌ容量のガラスビーカーに、試験例３１〜３３では２Ｌ容量のステンレスビーカーに、指定容量Iの温水を入れて８０℃に調整した後、中国産緑茶葉４０ｇを投入し、７５℃の湯浴上で１５分間の１回目の抽出を行なった。抽出後、ビーカー内容物を目開き１０６μｍの金属メッシュでろ過し、濾液（抽出液）は速やかに３０℃以下に冷却した。
茶殻は、固液分離後速やかにビーカーに戻し、指定容量IIの８５℃の温水を注ぎ、８０℃の湯浴上で１０分間の２回目の抽出を行ない、抽出後、１回目と同様に固液分離および濾過を行い、得られた抽出液を３０℃以下に冷却した。
そして、２回目の抽出で得られた抽出液を１回目の抽出で得られた抽出液に混合して混合抽出液（表１５の抽出液回収量）を得た。
得られた混合抽出液のＥＧＣｇ濃度、総カテキン濃度、異性化率、ＥＧＣｇ抽出率、総カテキン抽出率を測定し、各項目について各基準に基づいて（表１６の備考参照）判定を行なうとともに総合的な判定も行ない、結果を表１６に示した。 (Test Examples 27 to 33)
In Test Examples 27 to 30, a 1 L capacity glass beaker was added. In Test Examples 31 to 33, a 2 L capacity stainless beaker was charged with warm water of a specified capacity I and adjusted to 80 ° C., and then 40 g of Chinese green tea leaves were added. The first extraction for 15 minutes was performed on a 75 ° C. water bath. After extraction, the contents of the beaker were filtered through a metal mesh having an opening of 106 μm, and the filtrate (extract) was quickly cooled to 30 ° C. or lower.
The tea husk is immediately returned to the beaker after solid-liquid separation, poured with 85 ° C warm water of the specified volume II, and extracted for the second time for 10 minutes in a hot water bath at 80 ° C. Liquid separation and filtration were performed, and the obtained extract was cooled to 30 ° C. or lower.
And the extract obtained by the 2nd extraction was mixed with the extract obtained by the 1st extraction, and the mixed extract (the extract recovery amount of Table 15) was obtained.
The EGCg concentration, total catechin concentration, isomerization rate, EGCg extraction rate, and total catechin extraction rate of the obtained mixed extract are measured, and each item is determined based on each criterion (see the remarks in Table 16) and comprehensively determined. The results are shown in Table 16.

抽出時の加水倍率は、抽出槽内での茶葉の運動性に影響するために、多いほど抽出率が向上するが、得られる抽出液量が多くなることによるカテキン濃度の低下が同時に生じる。試験例２７の５倍水量では、液量が不十分であり、カテキン抽出率が４０％以下にとどまってしまっている。他方、試験例３３では、カテキン抽出率が変らずに液量だけが増えたことにより、カテキン濃度が低くなってしまっている。このことより、１回目の抽出の加水倍率は１０〜３０倍が好ましく、抽出効率とカテキン濃度とを考慮すると１０〜２５倍がより好ましく、特に１０〜２０倍がさらに好ましいと考えれる。   The ratio of water addition at the time of extraction affects the motility of tea leaves in the extraction tank, so that the extraction rate is improved as the amount is increased. However, the catechin concentration is lowered simultaneously with the increase in the amount of the extract to be obtained. With the five times the amount of water of Test Example 27, the amount of liquid is insufficient, and the catechin extraction rate remains at 40% or less. On the other hand, in Test Example 33, the catechin concentration was lowered because only the liquid amount increased without changing the catechin extraction rate. From this, the water extraction rate of the first extraction is preferably 10 to 30 times, more preferably 10 to 25 times, and even more preferably 10 to 20 times considering the extraction efficiency and the catechin concentration.

（試験例３４〜３７）
１Ｌ容量のガラスビーカー（内径１０５ｍｍ、深さ１５０ｍｍ）に温水４００ｍＬを入れて８０℃に調整した後、中国産緑茶葉４０ｇを投入し、７５℃の湯浴上で１５分間の１回目の抽出を行なった。抽出後、ビーカー内容物を目開き１０６μｍの金属メッシュでろ過し、濾液（抽出液）は速やかに３０℃以下に冷却した。
茶殻は、固液分離後速やかにビーカーに戻し、指定容量IIIの８５℃の温水を注ぎ、８０℃の湯浴上で１０分間の２回目の抽出を行ない、抽出後、１回目と同様に固液分離および濾過を行い、得られた抽出液を３０℃以下に冷却した。
そして、２回目の抽出で得られた抽出液を１回目の抽出で得られた抽出液に混合して混合抽出液（表１７の抽出液回収量）を得た。
得られた混合抽出液のＥＧＣｇ濃度、総カテキン濃度、異性化率、ＥＧＣｇ抽出率、総カテキン抽出率を測定し、各項目について各基準に基づいて（表１８の備考参照）判定を行なうとともに総合的な判定も行ない、結果を表１８に示した。 (Test Examples 34 to 37)
In a 1 L glass beaker (inner diameter 105 mm, depth 150 mm), add 400 mL of warm water to 80 ° C., and then add 40 g of Chinese green tea leaves and extract for the first time in a 75 ° C. water bath for 15 minutes. I did it. After extraction, the contents of the beaker were filtered through a metal mesh having an opening of 106 μm, and the filtrate (extract) was quickly cooled to 30 ° C. or lower.
The tea husk is immediately returned to the beaker after solid-liquid separation, poured with 85 ° C warm water of specified volume III, extracted for the second time for 10 minutes in a 80 ° C hot water bath, and after extraction, the tea cake is solidified in the same way as the first time. Liquid separation and filtration were performed, and the obtained extract was cooled to 30 ° C. or lower.
And the extract obtained by the 2nd extraction was mixed with the extract obtained by the 1st extraction, and the mixed extract (the extract collection amount of Table 17) was obtained.
The EGCg concentration, total catechin concentration, isomerization rate, EGCg extraction rate, total catechin extraction rate of the obtained mixed extract are measured, and each item is determined based on each criterion (see the remarks in Table 18) and comprehensively determined. The results are shown in Table 18.

２回目の抽出の加水倍率は、１回目の抽出と同様に、多いほど抽出率は向上するが、カテキン濃度の低下を生じる。２回目の抽出は、１回目の抽出の抽出不足を補うためのものであるため、２回目の抽出の加水倍率は少量でも構わないが、試験例３４の２倍量のように少ない場合は、抽出率が低めになってしまうことがあり、試験例３５のように少なくとも５倍量の加水倍率であることが好ましいといえる。試験例３４〜３７において、２回目の抽出の加水倍率の増加に伴い、混合抽出液のカテキン濃度が低下する傾向が見られていることから、２回目の抽出の加水倍率は、１回目の抽出の加水倍率以下に留める方が好ましいと予想される。
As with the first extraction, the extraction rate of the second extraction increases as the extraction rate increases, but the catechin concentration decreases. The second extraction is intended to compensate for the lack of extraction of the first extraction, so the amount of hydration of the second extraction may be small, but when it is as small as twice the amount of Test Example 34, An extraction rate may become low, and it can be said that it is preferable that it is at least 5 times the amount of hydrolysis like Test Example 35. In Test Examples 34 to 37, the catechin concentration of the mixed extract tends to decrease with the increase of the water extraction ratio of the second extraction, and therefore the water extraction ratio of the second extraction is the first extraction. It is expected that it is preferable to keep it below the hydrolysis ratio.

Claims (9)

茶葉を５５℃〜８０℃の温水で抽出して抽出液Ａと茶殻Ｂとを得(第１抽出工程)、茶殻Ｂを、第１抽出工程で用いた温水の温度以上の温水で、且つ第１抽出工程での抽出時間以下の抽出時間で抽出して抽出液Ｃと茶殻Ｄを得(第２抽出工程)、抽出液Ａと抽出液Ｃを混合することを特徴とする茶抽出液の製造方法。   The tea leaves are extracted with hot water of 55 ° C. to 80 ° C. to obtain an extract A and a tea husk B (first extraction step), and the tea husk B is heated with hot water equal to or higher than the temperature of the hot water used in the first extraction step. Extraction C and tea husk D are extracted with an extraction time equal to or less than the extraction time in one extraction process (second extraction process), and the extraction liquid A and the extraction liquid C are mixed to produce a tea extraction liquid Method. 茶葉を５５℃〜８０℃の温水で抽出して抽出液Ａと茶殻Ｂを得(第１抽出工程)、茶殻Ｂを、第１抽出工程で用いた温水の温度以上の温水で、且つ第１抽出工程での抽出時間以下の抽出時間で抽出して抽出液Ｃと茶殻Ｄを得(第２抽出工程)、茶殻Ｄを、第１抽出工程で用いた温水の温度以上の温水で、且つ第１抽出工程での抽出時間以下の抽出時間で抽出して抽出液Ｅを得(第３抽出工程)、抽出液Ａ、抽出液Ｃ及び抽出液Ｅを混合することを特徴とする茶抽出液の製造方法。   The tea leaves are extracted with warm water of 55 ° C. to 80 ° C. to obtain an extract A and tea husk B (first extraction step), and the tea husk B is warm water at or above the temperature of the hot water used in the first extraction step, and the first Extraction with an extraction time equal to or less than the extraction time in the extraction step yields extract C and tea husk D (second extraction step), and the tea husk D is warm water equal to or higher than the temperature of the hot water used in the first extraction step. Extraction liquid E is obtained by extraction with an extraction time equal to or less than the extraction time in one extraction step (third extraction step), and the extraction liquid A, extraction liquid C, and extraction liquid E are mixed. Production method. 第１抽出工程の抽出時間が５分〜６０分であり、抽出に用いる温水量が茶葉質量の１０〜３０倍であることを特徴とする請求項１又は２に記載の茶抽出液の製造方法。   The method for producing a tea extract according to claim 1 or 2, wherein the extraction time of the first extraction step is 5 to 60 minutes, and the amount of hot water used for extraction is 10 to 30 times the tea leaf mass. . 第２抽出工程で抽出に用いる温水量が、第１抽出工程で抽出に用いた温水量以下であることを特徴とする請求項１乃至３の何れかに記載の茶抽出液の製造方法。   The method for producing a tea extract according to any one of claims 1 to 3, wherein the amount of hot water used for extraction in the second extraction step is equal to or less than the amount of hot water used for extraction in the first extraction step. 第２抽出工程及び第３抽出工程の各工程で抽出に用いる温水量が、第１抽出工程で抽出に用いた温水量以下であることを特徴とする請求項２又は３に記載の茶抽出液の製造方法。   The tea extract according to claim 2 or 3, wherein the amount of hot water used for extraction in each of the second extraction step and the third extraction step is equal to or less than the amount of hot water used for extraction in the first extraction step. Manufacturing method. 第１抽出工程および第２抽出工程、或いはさらに第３抽出工程の抽出法が、バッチ式であることを特徴とする請求項１乃至５の何れかに記載の茶抽出液の製造方法。   The method for producing a tea extract according to any one of claims 1 to 5, wherein the extraction method of the first extraction step and the second extraction step, or further the third extraction step is a batch type. 請求項１乃至６の何れかに記載の製造方法によって得られる茶抽出液を乾燥することを特徴とする茶抽出物の製造方法。   A method for producing a tea extract, comprising drying the tea extract obtained by the production method according to claim 1. 請求項１乃至６の何れかに記載の製造方法によって得られる茶抽出液。   The tea extract obtained by the manufacturing method in any one of Claims 1 thru | or 6. 請求項８に記載の製造方法によって得られる茶抽出液を乾燥して得られる茶抽出物。

The tea extract obtained by drying the tea extract obtained by the manufacturing method of Claim 8.