WO2004073828A1

WO2004073828A1 - Method for extracting chlorophyll from silkworm excrements and composition produced thereby

Info

Publication number: WO2004073828A1
Application number: PCT/KR2004/000348
Authority: WO
Inventors: Chang-Ho Jeon
Original assignee: Individual
Current assignee: Individual
Priority date: 2003-02-20
Filing date: 2004-02-19
Publication date: 2004-09-02
Anticipated expiration: 2005-08-20
Also published as: KR20030032983A

Abstract

The present invention relates to a method for extracting chlorophyll from silkworm excrements, which comprises the steps of: adding a first extraction solvent to the excrements of fifth-instar silkworms, stirring the mixture and centrifuging the stirred mixture; adding methylene chloride to a residue, stirring the residue-containing mixture and centrifuging the stirred residue-containing mixture, the methylene chloride being volatilized in the centrifugation process; concentrating the chlorophyll extract obtained from the first and second extraction processes, under vacuum, to produce a chlorophyll concentrate; adding corn oil, polyoxyethylene sorbitol fatty acid ether and polyoxyethylene glycerin fatty acid ester to the chlorophyll concentrate, and stirring the chlorophyll concentrate-containing mixture to emulsify the mixture; and mixing the emulsified chlorophyll concentrate and colloidal silver-ion water, and stirring the silver ion-containing mixture to produce a liquid chlorophyll composition containing chlorophyll.

Description

METHOD FOR EXTRACTING CHLOROPHYLL FROM SILKWORM EXCREMENTS AND COMPOSITION PRODUCED THEREBY

Technical Field

The present invention relates to a chlorophyll extraction method and a composition produced thereby, and more particularly, to extracting chlorophyll concentrate from fine powders of silkworm excrements by the addition of extraction solvent, and producing liquid and powdery chlorophyll compositions from the chlorophyll concentrate.

Background Art

Chlorophyll is generally present in a chloroplast, and it is most abundantly distributed in leaves and sometimes also in green parts of other tissues, such as stems and roots. The chlorophyll absorbs sunlight and converts the light energy into chemical energy by a photosynthesis process. In the photosynthesis process, the converted energy transforms carbon dioxide (C0₂) and water into carbohydrates, such as glucose or starch, to supply nutrition to plants. Thus, the chlorophyll plays an important role to provide the foundation of food chain.

In a chlorophyll extraction method according to the prior art, leaves or silkworm excrements in extraction solvent ethyl alcohol (ethanol) is stirred with a stirrer, passed through an ultrasonic system, a centrifuge and a vacuum concentrator to extract concentrate, and emulsified with the ultrasonic system.

However, this prior extraction method has the following problems when examining the chemical structure and components of chlorophyll as shown in FIG. 1.

When carefully examining the chemical structure and components of chlorophyll, the chlorophyll is a wax-like, blue and red fine crystal with about 5 μm size, and is a chelate form with magnesium (Mg) . The chlorophyll emits fluorescence when exposed to ultraviolet rays in a dark place, and chlorophyll-a and chlorophyll-b are generally found in higher plants at a ratio of 3:1-3:2. Since the chlorophyll extract according to the present invention contains tocopherol (vitamin E) , fatty acid (e.g., linoleic acid), carbohydrate, vegetable fat and carbon powder, the chlorophyll is difficult to store at room temperature and easily decomposed at room temperature, and thus should be freeze-stored. Thus, it has problems in terms of storage and distribution.

Also, in extracting and emulsifying the chlorophyll with an ultrasonic system (ultrasonic generator 2.5 KW, ultrasonic transducer 15 KHz, there is a problem in that a long time of total 18 hours (each 6-9 hours) is required, and thus productivity is significantly reduced. Another problem is that heat is generated in the ultrasonic system to break the active ingredients of the chlorophyll such that the complete extraction of the chlorophyll is difficult. Furthermore, high equipment cost is required so that production cost is increased.

Disclosure of Invention

Accordingly, the present invention has been made to solve the problems occurring in the chlorophyll extraction method according to the prior art, and an object of the present invention is to provide a chlorophyll extraction method in which the excrements of fifth-instar silkworms is dried, washed, sterilized and pulverized into fine powders, the fine powders are added only with extraction solvent and then stirred, the stirred solution is passed through a centrifuge and a vacuum concentrator without using an ultrasonic system, to extract chlorophyll concentrate, the extracted chlorophyll concentrate is emulsified without using the ultrasonic system, and from the emulsified chlorophyll concentrate, a liquid or powdery composition is produced, and also to provide liquid or powdery compositions produced by the above method.

Brief Description of Drawings

FIG. 1 shows the chemical structure of chlorophyll to be produced according to the present invention;

FIG. 2 is a flow diagram showing the extraction and emulsification processes of chlorophyll according to the present invention;

FIG. 3 is a flow diagram showing a process for producing a liquid chlorophyll composition according to the present invention; and FIG. 4 is a flow diagram showing a process for producing a powdery chlorophyll composition according to the present invention.

Best Mode for Carrying Out the Invention Hereinafter, a method for extracting chlorophyll from silkworm excrements according to the present invention, and a composition produced by the method, will be described in detail with reference to the accompanying drawing. In the present invention, the excrements of fifth- instar silkworms are dried in a shaded place, which is not sunny and is well ventilated. The dried excrements are collected.

The collected excrements are washed clean with water in a spraying manner, and sterilized with ultraviolet rays and ozone (O₃) , and then pulverized into fine powders.

Starch raw materials, such as corns, sweet potatoes and potatoes, are fermented in the pulverized excrements, and a distilled and purified ethyl alcohol having a 95% alcohol concentration is added to the fermented product at the amount of 50-70% by weight relative to the excrements. The mixture is introduced into a stainless container which is not oxidized by strong acid and strong alkaline. The introduced material is stirred at high speed, and separated into a first chlorophyll extract and a residue by a centrifuge.

To the residue separated by the centrifuge, methylene chloride (dichloromethane; CHCI₂) with excellent extraction and volatilization properties are added at the amount of 40- 70% by weight relative to the residue, and the mixture is stirred in a stainless container at high speed, and then separated into a second chlorophyll extract and a residue.

The first and second chlorophyll extracts are stirred while volatilizing the extraction solvent. The remaining chlorophyll extract is vacuum-concentrated to produce chlorophyll concentrate.

The chlorophyll concentrate produced is emulsified in the following manner.

The chlorophyll concentrate is stirred in a stainless container which is not oxidized by strong acid and strong alkaline. During the stirring step, the chlorophyll concentrate is emulsified with fatty acid, hydrogenated oil from animals and plants, and fatty acid ester.

Namely, as the emulsifiers, corn oil, polyoxyethylene sorbitol fatty acid ether and polyoxyethylene glycerin fatty acid ester are used to emulsify the chlorophyll concentrate (see FIG. 2) .

From the chlorophyll concentrate emulsified with such emulsifiers, a liquid or powdery chlorophyll composition is produced.

In order to produce the liquid chlorophyll composition from the chlorophyll concentrate, the following preparation and process are performed (see FIG. 3) .

Namely, water containing no minerals is prepared from tap water by a reverse osmosis system. The prepared water has a pH below 7. Using the prepared water, silver-ion water is made by a colloidal silver ion water-making system.

It is known that silver in the silver-ion water has excellent bactericidal ability against various bacteria, such as E . coli and virus, and has the ability to sterilize about 650 kinds of bacteria within at least 6 minutes.

The silver-ion water-making system, which is used in the present invention, is a colloidal silver-ion preparation system, in which silver microparticles with a purity of

99.99% and a size of 0.005-0.015 microns are dissolved in 800 cc of distilled pure water at a concentration of 3-5 ppm. added to the colloidal silver-ion water prepared by the silver-ion water-making system, and stirred in a glass or plastic container at high speed, thereby producing a liquid chlorophyll composition. The liquid chlorophyll composition produced as described above does not to be stored in a refrigerator during its distribution, because the silver contained in the liquid chlorophyll composition continuously sterilizes bacteria and inhibits the production of bacteria. In the sterilization principle of the colloidal silver, the results of experiments conducted till the recent time showed that the colloidal silver was a natural bactericidal (antibiotic) agent sterilizing substantially all single-cell pathogenic organisms found on the ground. It is the most powerful theory that the silver inactivates special enzymes with metabolic actions (digestion and breathing) in the single-cell pathogenic organisms, thereby sterilizing the organisms .

Furthermore, in order to produce the powdery chlorophyll composition from the emulsified chlorophyll concentrate, the following process is performed (see FIG. 4).

Namely, to 10 g of the emulsified chlorophyll concentrate, 60 g of starches (potato, corn and sweet potato starches) are added, and the mixture is stirred in a stainless container at high speed, and dried by spraying into air. Organic and inorganic minerals (e.g., organic zinc, organic germanium and calcium, etc.) are added to the dried material to produce a powdery mineral chlorophyll composition.

Hereinafter, the method of producing the liquid and powdery chlorophyll compositions by various processes, including extraction from the excrements of fifth-instar silkworms, emulsification and stirring, according to the present invention, will be described in detail with reference to the following examples.

Example 1 : Production of liquid chlorophyll composition Chlorophyll concentrate is extracted from the excrements of fifth-instar silkworms using extraction solvent.

Namely, in a first extraction, an extraction solvent with 95% alcohol concentration is added to 160 kg of silkworm excrements at the amount of 50-70% by weight relative to the silkworm excrements, stirred at high speed and centrifuged to produce a first chlorophyll extract.

In a second extraction process, to a residue remaining after the first extraction process, methylene chloride

(dichloromethane) is added at the amount of 40-70% by weight, and the solution is stirred at high speed and centrifuged to produce a second chlorophyll extract.

In the centrifugation process, the extraction solvent is volatilized.

6 kg of the chlorophyll extract obtained from the first and second extraction processes is added with 1-3% by weight of corn oil, 10-15% by weight of polyoxyethylene sorbitol fatty acid ether and 2-5% by weight of polyoxyethylene glycerin fatty acid ester, and emulsified by high-speed stirring . In order to produce a liquid chlorophyll composition from the emulsified chlorophyll concentrate, 6 kg of the emulsified chlorophyll concentrate is mixed with 600 liters of colloidal silver-ion water, and stirred at high speed to produce a liquid chlorophyll composition containing chlorophyll.

Example 2: Production of powdery chlorophyll composition

Chlorophyll concentrate is extracted from the excrements of fifth-instar silkworms using extraction solvent. Namely, in a first extraction process, an extraction solvent with 95% alcohol concentration is added to 160 kg of silkworm excrements at the amount of 50-70% by weight relative to the silkworm excrements, and the solution is stirred at high speed and centrifuged to produce a first chlorophyll extract. In a second extraction process, to a residue remaining after the first extraction process, methylene chloride (dichloromethane) is added at the amount of 40-70% by weight, and the mixture is stirred at high speed and centrifuged to produce a second chlorophyll extract. In the centrifugation process, the extraction solvent is volatilized.

6 kg of the chlorophyll extract obtained from the first and second extraction processes is added with 1-3% by weight of corn oil, 10-15% by weight of polyoxyethylene sorbitol fatty acid ether and 2-5% by weight of polyoxyethylene glycerin fatty acid ester, and emulsified by high-speed stirring.

In order to produce a powdery chlorophyll composition from the emulsified chlorophyll concentrate, 10 g of the emulsified chlorophyll concentrate is mixed with 60 g of starch, 3 g of calcium (Ca) , 3 g of organic zinc and 1 g of organic germanium (Ge) is dried by spraying into the air, thereby producing a powdery chlorophyll composition containing chlorophyll. The chlorophyll concentrate produced in Examples 1 and 2 was analyzed for their components, and the results showed that it was composed of the following components:

1. chlorophyll-b: 12.4 mg/lOOg chlorophyll-a: 30.9 mg/lOOg

2. linoleic acid: 22 mg/lOOg 3. tocopherol (vitamin E) : 1.6 mg/lOOg

4. carbon powder: 0.1 g/lOOg.

5. carbohydrate: 0.3 g/lOOg

6. lipid: 0.3 g /100g

7. protein: 0.2 g/lOOg 8. water: 98.7 g/lOOg.

Also, it was found that the concentrate had a viable bacterial cell count of 5.0 x 10 and was positive to E . coli .

In a liquid chlorophyll composition produced from this concentrate, the general viable bacteria were completely sterilized and E. coli was found to be negative, as a result of examination conducted by the Japan food and environment association on January 21, 2003.

Industrial Applicability

As described above in detail, according to the inventive method for extracting chlorophyll from silkworm excrements and the composition produced thereby, various problems in the prior process of extracting the chlorophyll using ultrasonic waves can be completely solved. Namely, problems, such as an increase in production cost caused by high equipment cost, the breakdown of the active ingredients of chlorophyll, and a reduction in productivity, can be solved. Also, according to the present invention, the colloidal silver-ion water is used to produce the chlorophyll composition so that the chlorophyll composition can be distributed without a need for freeze-storage .

In addition, the present invention has many effects in that it reduces production cost and increases productivity, and bacteria are not produced even when the composition is distributed at room temperature.

Claims

What Is Claimed Is:

1. A method for extracting chlorophyll from silkworm excrements, which comprises the steps of: adding a first extraction solvent having a 95% alcohol concentration to 160 kg of the excrements of fifth-instar silkworms at the amount of 50-70% by weight relative to the excrements, stirring the mixture at high speed and centrifuging the stirred mixture to produce a first chlorophyll extract; adding 40-70% by weight of methylene chloride to a residue remaining after the first extraction step, stirring the residue-containing mixture at high speed and centrifuging the stirred residue-containing mixture to produce a second chlorophyll extract, the methylene chloride being volatilized in the centrifugation process; concentrating the chlorophyll extract obtained from the first and second extraction processes, under vacuum, to produce a chlorophyll concentrate; adding 1-3% by weight of corn oil, 10-15% of polyoxyethylene sorbitol fatty acid ether and 2-5% by weight of polyoxyethylene glycerin fatty acid ester to 6 kg of the chlorophyll concentrate, and stirring the chlorophyll concentrate-containing mixture at high speed to emulsify the mixture; and mixing 6 kg of the emulsified chlorophyll concentrate and 600 liters of colloidal silver-ion water, and stirring the silver ion-containing mixture at high speed to produce a liquid chlorophyll composition containing chlorophyll.

2. A chlorophyll composition extracted from silkworm excrements, which is produced by a method comprising the steps : adding a first extraction solvent having a 95% alcohol concentration to 160 kg of the excrements of fifth-instar silkworms at the amount of 50-70% by weight relative to the excrements, stirring the mixture at high speed and centrifuging the stirred mixture to produce a first chlorophyll extract; adding 40-70% by weight of methylene chloride to a residue remaining after the first extraction step, stirring the residue-containing mixture at high speed and centrifuging the stirred residue-containing mixture to produce a second chlorophyll extract, the methylene chloride being volatilized in the centrifugation process; concentrating the chlorophyll extract obtained from the first and second extraction processes, under vacuum, to produce a chlorophyll concentrate; adding 1-3% by weight of corn oil, 10-15% of polyoxyethylene sorbitol fatty acid ether and 2-5% by weight of polyoxyethylene glycerin fatty acid ester to 6 kg of the chlorophyll concentrate, and stirring the chlorophyll concentrate-containing mixture at high speed to emulsify the mixture; and mixing 6 kg of the emulsified chlorophyll concentrate and 600 liters of colloidal silver-ion water, and stirring the silver ion-containing mixture at high speed to produce a liquid chlorophyll composition containing chlorophyll.

3. A method for extracting chlorophyll from silkworm excrements, which comprises the steps of: adding a first extraction solvent having a 95% alcohol concentration to 160 kg of the excrements of fifth-instar silkworms at 50-70% by weight relative to the excrements, stirring the mixture at high speed and centrifuging the stirred mixture to produce a first chlorophyll extract; adding 40-70% by weight of methylene chloride to a residue remaining after the first extraction step, stirring the residue-containing mixture at high speed and centrifuging the stirred residue-containing mixture to produce a second chlorophyll extract, the methylene chloride being volatilized in the centrifugation process; concentrating the chlorophyll extract obtained from the first and second extraction processes, under vacuum, to produce a chlorophyll concentrates- adding 1-3% by weight of corn oil, 10-15% of polyoxyethylene sorbitol fatty acid ether and 2-5% by weight of polyoxyethylene glycerin fatty acid ester to 6 kg of the chlorophyll concentrate, and stirring the concentrate- containing mixture at high speed to emulsify the mixture; and mixing 10 g of the emulsified chlorophyll concentrate, 60 g of starch, 3 g of calcium, 1 g of organic zinc and 1 g of germanium, stirring the mixture at high speed and drying the stirred mixture by spraying it into the air, to produce a powdery chlorophyll composition containing chlorophyll.

4. A chlorophyll composition extracted from silkworm excrements, which is produced by a method comprising the steps of: adding a first extraction solvent having a 95% alcohol concentration to 160 kg of the excrements of fifth-instar silkworms at 50-70% by weight relative to the excrements, stirring the mixture at high speed and centrifuging the stirred mixture to produce a first chlorophyll extract; adding 40-70% by weight of methylene chloride to a residue remaining after the first extraction step, stirring the residue-containing mixture at high speed and centrifuging the stirred residue-containing mixture to produce a second chlorophyll extract, the methylene chloride being volatilized in the centrifugation process; concentrating the chlorophyll extract obtained from the first and second extraction processes, under vacuum, to produce a chlorophyll concentrate; adding 1-3% by weight of corn oil, 10-15% of polyoxyethylene sorbitol fatty acid ether and 2-5% by weight of polyoxyethylene glycerin fatty acid ester to 6 kg of the chlorophyll concentrate, and stirring the concentrate- containing mixture at high speed to emulsify the mixture; and mixing 10 g of the emulsified chlorophyll concentrate,

60 g of starch, 3 g of calcium, 1 g of organic zinc and 1 g of germanium, stirring the mixture at high speed and drying the stirred mixture by spraying it into the air, to produce a powdery chlorophyll composition containing chlorophyll.