JP2002177703A - Separation method using multicomponent solution, and separation liquid - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a specific solution system and a separation method, by which a substance being dissolved, mixed or dispersed in various kinds of solutions can easily be separated. SOLUTION: In the separation method and the solution system, the substance to be extracted is separated by relatively or kinetically changing the mixing ratios of a mixed solution comprising at least three kinds of solutions. The three kinds of solutions satisfy at least following relations: 1. A liquid A and a liquid B mutually dissolve, mix or disperse at an arbitrary ratio. 2. The liquid A and a liquid C mutually dissolve, mix or disperse at an arbitrary ratio. 3. Either of the liquid B and the liquid C dissolves, mixes or disperses in the other liquid in an amount of <10%. The substance to be extracted can be more efficiently separated under following conditions: 4. The substance D to be extracted is able to dissolve, mix or disperse in the liquids A and B in an amount of <5%. 5. The substance D dissolves in the liquid C. The stability of the mixed solution can be improved by using a surfactant.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

TECHNICAL FIELD The present invention relates to a special solution system for separating a substance dissolved, mixed or dispersed in various solutions.

[0002]

2. Description of the Related Art Methods for separating substances dissolved in a solvent include a method using an emulsion and a method using a difference in boiling points. As a separation method using an emulsion, there is a method called an emulsification type liquid membrane extraction method represented by US Pat. No. 3,410,794. This method is a method of (1) preparing a W / O or O / W emulsion with a surfactant, oil and water, and (2) directly contacting the emulsion with a liquid containing a substance to be extracted.
(3) The phenomenon used in the extraction is the dissolution or diffusion of the substance to be extracted into the oily or aqueous layer or each layer in the surfactant. In other words, if the substance to be extracted is W / O
In the case of (1), the phenomenon of entering the W layer in the case of O / W is utilized. The difference in the diffusion rate between the extraction target substance and the solvent is used for separation. As a further characteristic, when the liquid containing the substance to be extracted is an oil layer, that is, an oily solvent, an O / W emulsion is added to the solvent, and when the liquid is an aqueous layer, that is, an aqueous solvent, a W / O emulsion is added to the solvent. That is, the oil solvent containing the substance to be extracted is mixed with W (aqueous layer) of the emulsion or the aqueous solvent of the emulsion containing the substance to be extracted with the O (oil layer) so as to come into contact with each other. These characteristics are also the same in Japanese Patent Application Laid-Open No. Hei 10-231240 “Method for solubilization and extraction using reverse micelles” filed with the Japan Patent Office. These methods have the following problems. (1) Strict temporal operation is required for separation by diffusion rate. (2) A liquid containing an object to be extracted and an emulsion as an extraction liquid are mixed and allowed to stand to separate into two layers. become. Therefore, it is necessary to separate the layer containing the target substance and further perform the operations of demilking and separating. Next, let's look at an example of recycling polystyrene waste with regard to methods that use the difference in boiling points. Limonene and other organic solvents may be used for the regeneration of discarded Styrofoam. Its purpose is to dissolve and extract the plastic. A typical separation method is (1) a method in which a solvent, that is, limonene is evaporated by heating using a difference in boiling points (Japanese Patent No. 2518493).
And (2) gelation using a surfactant (Japanese Patent Application No. 5-92656). First, (1) the method of heating may increase the size of the apparatus or cause deterioration of the solvent or polystyrene due to overheating. In addition, the method of gelation and separation in (2) has a problem that handling is inconvenient because the gelled polystyrene appears in the middle layer of the liquid divided into three layers. In order to solve these problems, the applicant has developed a method of bringing a multilayer emulsified emulsion into contact with an object to be extracted (see Patent No. 32).
No. 18031). However, this method includes a complicated step of having to prepare a multilayer emulsion, and a simpler method has been demanded especially in the field of resource recovery where cost is a problem. In light of these things,
The present invention provides a method for easily separating substances dissolved in various solvents, as a method for separating an object to be extracted by relatively or dynamically changing the mixing ratio of a mixed solution of at least three kinds of solutions. And a separation solution. In addition, by adjusting the composition of the separation liquid, precise separation can be performed. That is, Example 4 described later. As mentioned above, in a single separation operation, not only polystyrene was separated from limonene, but also impurities such as dyes in waste polystyrene were successfully separated. Such separation was not possible when using a multilayer emulsion. This is because the emulsion system was too complex to control easily. The present invention means that not only recycling but also bioindustry costs can be greatly reduced. Further, the present invention enables separation without using a surfactant, and has great significance in the case of purification in a subsequent step. This is because there is great difficulty in removing the surfactant.

[0003]

A problem to be solved is to provide a method and a separation solution for easily separating a substance dissolved in various solvents.

[0004]

Means for Solving the Problems The present invention provides a method for separating an object to be extracted by changing the mixing ratio of a mixed solution of at least three types of solutions relatively or dynamically, and a special solution system. It is a separated liquid, and the most main feature is that the relationship between the three types of solutions satisfies at least all of the following. That is, 1. Solution A and Solution B dissolve, mix or disperse in a free ratio. Solution A and Solution C dissolve, mix or disperse in a free ratio. 3. Liquid B and liquid C dissolve, mix or disperse in less than 10% of the other. Solution C dissolves, mixes, or disperses the separation target, but Solution A and B dissolves, mixes, or disperses less than 5%. Such a solution has a specific mixing ratio and is a mixture of each component constituting the mixed solution. Along with the dynamic change of the composition ratio, a part of the constituent solution is associated and precipitated, and the object to be extracted or the molecular assembly containing the object to be extracted can be taken into the deposited liquid. Further, with the dynamic change of the composition ratio of each component constituting the mixed solution, a part of the constituent solution is associated precipitation,
By incorporating the extraction target or a molecular assembly containing the extraction target into the precipitation liquid, and further changing the composition ratio of each component constituting the mixed solution to a dynamic change, one of the constituent solutions once associated and precipitated is extracted. It is possible to take the part again into the mixed solution. As a more special case, a molecular aggregate is formed in the course of solution mixing, and the molecular aggregate encloses the extraction target according to the dynamic change of the composition ratio of each component constituting the mixed solution to which the molecular aggregate belongs. In some cases, a complex molecular assembly may be formed.

(Definition) In this specification, the following terms include the following: "Molecular assembly" refers to a state in which two or more molecules are gathered, and at least an emulsion,
It shall include all sub-concepts such as microemulsions, micelles, reverse micelles, multilayer emulsions, liposomes, vesicles and clusters. “Associative precipitation” includes the aggregation or association of molecules dispersed in a solution to form a molecular aggregate. When the temperature is changed, particularly as the temperature is lowered, the molecular assembly that has been associated and precipitated starts to separate. Therefore, even if the two layers are not separated at the temperature at the time of mixing, it can be confirmed whether or not association precipitation has occurred due to a change in temperature. Also, even if the temperature is higher than the temperature at which it separates into two layers,
The effects of the present invention can be obtained.

[0006]

DESCRIPTION OF THE PREFERRED EMBODIMENTS The present invention relates to a method for easily separating substances dissolved in various solvents and a separation liquid for generating a special system. In Example 1, polystyrene dissolved in limonene is extracted as a liquid precipitate with limonene, ethanol, and water without using a surfactant. In Example 2, with this solution system, a part of the constituent solution was associated and precipitated with the change of the constituent ratio of each of the constituent solutions, and as the constituent ratio was further changed, the solution that was associated and precipitated again This indicates that it is recovered in the entire mixture. Example 3
Shows that a similar precipitate can be obtained using glycerin instead of water. It is also shown that by changing the mixing ratio of water and glycerin, the polystyrene in limonene can be separated from the transparent polystyrene portion and impurities such as dyes in a single operation. In Example 4, even if glycerin was used instead of water, this solution system caused a part of the constituent solution to associate and precipitate with the change of the constituent ratio of each constituent solution, and further changed the constituent ratio. This indicates that part of the solution that has been associated and precipitated is recovered again in the entire mixture. Example 5 shows the use of a surfactant to improve the solution stability against temperature changes. The embodiment is not limited to the following example.

[0007]

Embodiment 1 The polystyrene dissolved in limonene without using a surfactant is limonene,
An example of taking out as a liquid precipitate with ethanol and water will be described.

The present invention relates to a method for separating an object to be extracted by changing the mixing ratio of a mixed solution of at least three types of solutions relatively or dynamically, and a separation solution as a special solution system. The most important feature is that the relationship between the three types of solutions satisfies at least all of the following. That is, 1. Solution A and Solution B dissolve, mix or disperse in a free ratio. Solution A and Solution C dissolve, mix or disperse in a free ratio. Either solution B or solution C dissolves, mixes or disperses only in less than 10% of the other. The extraction target can be separated more efficiently under the following conditions. 4. 4. Extraction target D is dissolved, mixed or dispersed in liquid A and liquid B at less than 5%. The extraction target D is dissolved in the liquid C. Each of the above solutions does not need to be composed of a single component. Further, as described later, by further finely controlling the composition of each solution, it becomes possible to selectively extract substances. FIG. 1 shows the relationship between the solutions. In the figure, the solid line shows the relationship of dissolving, mixing or dispersing at a free ratio, and the broken line shows less than 10% (5% for D).
) Indicates that they are only dissolved, mixed or dispersed.

Here, water is used for solution A, ethanol is used for solution B,
Use limonene for solution C. The temperature is preferably 15 ° C
To 34 ° C, most preferably 21 ° C to 30 ° C, and in the examples 25 ° C. (1) A liquid mixture is prepared using liquid A water and liquid B ethanol. The concentration of water is preferably 1% to 15%, most preferably 4.
From 8% to 6.25%, 5% in the examples. As the ethanol, ethanol having a purity of 99.5% manufactured by Showa Chemical Industry Co., Ltd. was used, but exactly the same result was obtained with denatured alcohol for industrial use and anhydrous alcohol for disinfection. (2) The above (1) and limonene (manufactured by Wako Pure Chemical Industries, Ltd.
(R)-(+)-limonene, purity 95.0%, the same applies hereinafter). The mixing ratio was such that the ratio of the volume of limonene to the whole liquid mixture was desirably 5% to 45%, most desirably 10% to 25%, and in the examples, 20%. This solution (hereinafter referred to as a separated solution) is subjected to an optical microscope at a magnification of 60
When observed at 0 magnification, vacuolar particles were observed and the size was about 2 microns. Therefore, it was confirmed that some kind of molecular assembly was formed. (3) Dissolve the waste styrofoam for packaging in limonene as a liquid containing the extraction target. In the examples, 16.2 cubic centimeters were dissolved in 4 ml of limonene. (4) When 2 ml of the liquid of (2) was added to 4 ml of the liquid of (3), a fluid precipitate was formed. Here, the volume ratio of limonene was 20% before mixing, but was 66.67% of the total solution after mixing after mixing. From the viewpoint of the separated liquid, the composition ratio of limonene has changed from the region A to the region B in FIG. 2 described below. Here, when the amount of the liquid containing the substance to be separated, i.e., limonene in which polystyrene is dissolved in this example, is small, limonene is added, and separation can be performed by changing the composition ratio of the entire solution. . Such a dynamic change is difficult in the case of an emulsion, but can be easily achieved in the present invention. Further, not only the change from B to A in FIG. 2 but also the change in the x-axis direction in FIG.
Even if the composition ratio is changed in the y-axis direction (the composition ratio of water or ethanol) so as to pass through the area surrounded by,
Separation is possible. When the precipitate was observed with an optical microscope at a magnification of 600 times, vacuolar particles were observed and the size was about 25 microns. This vacuole has been observed to be covered by at least one layer of membrane. That is, some kind of molecular assembly is produced.

[0010] The ability to separate without using a surfactant has great significance when purifying in a subsequent step. This is because there is great difficulty in removing the surfactant.

A very significant feature of this solution system is that a part of the solution constituting the solution system is associated and precipitated with a change in the composition ratio in the solution, and is recovered again in the mixed solution. Embodiment 2. FIG. It will be described as.

[0012] Water is used for solution A, ethanol is used for solution B, and limonene is used for solution C. The temperature is preferably between 15 ° C and 34
° C, most preferably from 21 ° C to 30 ° C, and in the examples 25 ° C. (1) A liquid mixture is prepared using liquid A water and liquid B ethanol. The concentration of water is preferably 1% to 15%, most preferably 4.
From 8% to 6.25%, 5% in the examples. As the ethanol, ethanol having a purity of 99.5% manufactured by Showa Chemical Industry Co., Ltd. was used, but exactly the same result was obtained with denatured alcohol for industrial use and anhydrous alcohol for disinfection. (2) Limonene is gradually added to the solution of (1) as solution C. When the volume of limonene with respect to the whole solution reaches 10%, it starts to become cloudy, and when it reaches 34%, a part of the constituent liquid starts to separate and separate downward. This precipitation is greatest when the volume of limonene relative to the whole solution is 40% and disappears at 44%. That is, it is collected in the entire solution. It is cloudy up to 48%, but becomes clearer when the volume of limonene is further increased, and at 68% the entire solution separates into two layers. When the volume of limonene is 40% and the temperature is raised to 30 ° C.,
This separation layer disappears.

FIG. 2 shows a phase diagram of the solution. The left side of the line connected by ● is one layer of liquid, and the right side is separated into two layers. The region surrounded by ▲ is a range where a part of the constituent solution is associated and precipitated and separated. The vertical axis indicates the volume (%) of water in ethanol, and the horizontal axis indicates the concentration (%) of limonene in the whole solution. It has been confirmed that the precipitation of Example 1 occurs when the volume composition ratio is changed from region A to region B to pass through the precipitation region.

Embodiment 3 Shows that a similar precipitate can be obtained using glycerin instead of water. A
Glycerin (manufactured by Showa Chemical Co., Ltd., glycerin, purity 95%, the same applies hereinafter) is used as the liquid, ethanol is used as the liquid B, and limonene is used as the liquid C. The temperature is preferably between 17 ° C and 34 ° C.
° C, most preferably from 21 ° C to 30 ° C, and in the examples 25 ° C. (1) A mixed solution is prepared with solution A glycerin and solution B ethanol. The concentration of glycerin is desirably 1% to 60%,
Most preferably, it was 4% to 40%, and in the example, 10%. As the ethanol, ethanol having a purity of 99.5% manufactured by Showa Chemical Industry Co., Ltd. was used, but exactly the same result was obtained with denatured alcohol for industrial use and anhydrous alcohol for disinfection. (2) The above (1) and limonene are mixed. The mixing ratio was such that the ratio of the volume of limonene to the whole liquid mixture was desirably 5% to 45%, most desirably 10% to 25%, and in the examples, 20%. When this solution (hereinafter, referred to as a separated solution) was observed with an optical microscope at a magnification of 600 times, vacuolar particles were observed and the size was about 2 μm. Therefore, it was confirmed that some kind of molecular assembly was formed. (3) Dissolve the waste styrofoam for packaging in limonene as a liquid containing the extraction target. In the examples, 16.2 cubic centimeters were dissolved in 4 ml of limonene. (4) When 2 ml of the liquid of (2) was added to 4 ml of the liquid of (3), a fluid precipitate was formed. In this case, the volume ratio of limonene was 20% before mixing, but was 66.67% of the total solution after mixing after mixing. When viewed from the separated solution, the composition ratio of limonene has changed to a region corresponding to the region from A to B in the phase diagram corresponding to FIG. 2 in the case of glycerin. Here, similarly to Embodiment 1, when the amount of the liquid containing the separation target is small,
Separation can be achieved by adding limonene and changing the composition ratio of the whole solution. Such a dynamic change is difficult in the case of an emulsion, but can be easily achieved in the present invention. Further, in the phase diagram corresponding to FIG. 2 in the case of glycerin, not only the change from B to the region corresponding to A, but also the change in the x-axis direction in FIG. In this case, the separation can be performed by changing in the y-axis direction (the composition ratio of glycerin or ethanol) so as to pass through the region corresponding to the region enclosed by the triangle in the phase diagram corresponding to FIG. . When the precipitate was observed under an optical microscope at a magnification of 600 times, vacuolar particles were observed and the size was about 25 microns. This vacuole has been observed to be covered by at least one layer of membrane. That is, some kind of molecular assembly is produced.

Further, when 0.5% water is added to glycerin, the precipitated portion is separated into a colorless and transparent polystyrene portion and impurities such as dyes, and centrifuged.
Impurities can be removed. Therefore, it can be seen that selective separation becomes possible by controlling the mixing ratio of the solution. Such separation was not possible when using a multilayer emulsion. This is because the emulsion system was too complex to control easily.

When the curve drawn by ● in FIG. 2 is changed from the left side to the right side, the separation target can be separated, but the whole solution after mixing is separated. It is desirable to mix so that the composition ratio is on the right side of the curve drawn with ●.

Even if glycerin is used instead of water,
A part of the solution constituting this solution is associated and precipitated with the change of the composition ratio in the solution, and is recovered again in the mixed solution. Embodiment 4. FIG. It will be described as.

Glycerin in solution A, ethanol in solution B,
Use limonene for solution C. The temperature is desirably 17 ° C
To 34 ° C, most preferably 21 ° C to 30 ° C, and in the examples 25 ° C. (1) A mixed solution is prepared with solution A glycerin and solution B ethanol. The concentration of glycerin is desirably 1% to 60%,
Most preferably, it was 4% to 40%, and in the example, 10%. As the ethanol, ethanol having a purity of 99.5% manufactured by Showa Chemical Industry Co., Ltd. was used, but exactly the same result was obtained with denatured alcohol for industrial use and anhydrous alcohol for disinfection. (2) Limonene is added little by little to the solution of (1) as solution C, and the volume of limonene relative to the total solution is 5%.
%, 40%, 70%. 13 ° C
When cooled, glycerin precipitates and separates by only 40% below.

Next, the use of a surfactant in Example 5 shows an improvement in solution stability against temperature changes. Embodiment 1 FIG. In the same manner as described above, the volume ratio of limonene is 3
Make a 0% mixture. In addition, a mixed solution using a surfactant is prepared in the following procedure. Use water for solution A, ethanol for solution B, and limonene for solution C. (1) A liquid mixture is prepared using liquid A water and liquid B ethanol. The concentration of water is preferably 1% to 15%, most preferably 4.
From 8% to 6.25%, 5% in the examples. (2) HLB 19 and 13 sucrose fatty acid esters (Daiichi Pharmaceutical Co., Ltd.) and HB
A mixture of L11 polyglycerin fatty acid esters (manufactured by Sakamoto Yakuhin Kogyo Co., Ltd.) in equal volumes is added and dissolved in 0.1% of the mixed solution. (3) Limonene to glycerin fatty acid ester (food additive grade, manufactured by NOF Corporation), HLB6 and HLB6
And 1 of sucrose fatty acid ester (manufactured by Daiichi Pharmaceutical Co., Ltd.) and HBL2 polyglycerin fatty acid ester (manufactured by Sakamoto Yakuhin Kogyo Co., Ltd.) were mixed at the same volume.
Add 0.1% of the mixed solution and dissolve. (4) The above (2) and (3) are replaced with (3)
Mix to 0%. Looking at the effect of the temperature change, the mixed solution without using the surfactant starts to precipitate a solution at 27.8 ° C., whereas the mixed solution using the surfactant uses 15 ° C.
No solution was precipitated until. Further, the type of the surfactant is X. One with only sucrose fatty acid ester HLB19,
Y. Comparing only the HLB5, X. Is 27.3
° C. Did not precipitate up to 18 ° C. Therefore, it was confirmed that the presence of the surfactant contributed to the stability of the mixed solution with respect to the temperature. In addition, in Example 1. And 3.
It has also been confirmed that a precipitate of polystyrene is formed by the procedure described above.

In the solutions A, B and C described above, at least the following are effective. 1. 1. alcohols having 1 to 20 carbon atoms 2. ethylene glycol, glycerin, propylene glycol, sorbit 3. Aromatic hydrocarbons having 6 to 60 carbon atoms 4. Cyclic hydrocarbons having 3 to 60 carbon atoms Water 6. Ethers represented by R1-O-R2, wherein R1 and R2 have 1 to 60 carbon atoms each. 7. 7. A hydrocarbon containing an aldehyde group or a carboxyl group and having 60 or less carbon atoms. Fatty acids, fats and oils 9. It is a hydrocarbon containing an ester bond and has 10 carbon atoms.
0 or less 10. As the liquefied nitrogen, oxygen, carbon dioxide and surfactant, at least the following are effective. 1. Nonionic surfactant 2. 2. Anionic surfactant 3. Cationic surfactant Alcohols and glycols, having 1 to 1 carbon atoms
6. More specifically, at least the following are effective. 1. 1. The following fatty acid esters: glycerin, sucrose, pentaerythritol, sorbitol 2. Alkyl ether of alcohol having 2 or more carbon atoms 3. Polyethylene glycol type surfactant, alkyl ether of polyhydric alcohol 4. Amino acid type and betaine type amphoteric surfactants 5. The following sulfonates or sulfates: alkylbenzenes, alcohols having 6 or more carbon atoms Ammonium salt type and amine salt type cationic surfactants

The volume composition ratio of the mixed solution as the separation liquid is as follows:
Desirably, solution A is 1% to 60% and solution B is 99% to 4%.
0%, solution C ranges from 1% to 80%. But 3
As long as there are kinds of liquids, the composition ratio can be changed by adding them later.
If the B and C liquids are not 0%, they can perform their final function.

[0022]

As described above, according to the separation method and the separation solution of the present invention, the object to be extracted is separated by changing the mixing ratio of the mixed solution of at least three kinds of solutions relatively or dynamically. It is a method and a separation solution as a special solution system, and the most important feature is that the relationship among the three types of solutions satisfies at least all of the following. That is, 1. Solution A and Solution B dissolve, mix or disperse in a free ratio. Solution A and Solution C dissolve, mix or disperse in a free ratio. Either solution B or solution C dissolves, mixes or disperses only in less than 10% of the other. The extraction target can be separated more efficiently under the following conditions. 4. 4. Extraction target D is dissolved, mixed or dispersed in liquid A and liquid B at less than 5%. The extraction target D is dissolved in the liquid C. Thereby, the extraction target can be precipitated without using a surfactant. In such a solution, at a specific mixing ratio, with the dynamic change of the composition ratio of each component constituting the mixed solution, a part of the constituent solution is associated and precipitated, and the extraction target or the extraction target It is possible to incorporate a molecular assembly that contains a substance. Further, with the dynamic change of the composition ratio of each component constituting the mixed solution, a part of the constituent solution is associated and precipitated, and the extracted liquid or the molecular assembly containing the extracted substance is incorporated into the deposited liquid. Further, by changing the composition ratio of each component constituting the mixed solution to a dynamic change, a part of the constituent solution once separated and separated can be taken into the mixed solution again. As a more special case, molecular aggregates are formed during the solution mixing process,
The molecular assembly may form a new molecular assembly including the object to be extracted in accordance with the dynamic change of the composition ratio of each component constituting the mixed solution to which the molecular assembly belongs. Then, by adjusting the composition of each constituent solution, selective separation becomes possible.

【The invention's effect】 [Brief description of the drawings]

FIG. 1 is a relationship diagram relating to the solubility of a constituent solution.

FIG. 2 is a phase diagram based on a volume ratio of ethanol, water, and limonene.

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[Procedure amendment]

[Submission date] August 22, 2001 (2001.8.2)
2)

[Procedure amendment 1]

[Document name to be amended] Statement

[Correction target item name] Claim 5

[Correction method] Change

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[Procedure amendment 2]

[Document name to be amended] Statement

[Correction target item name] Claim 13

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[Correction target item name] 0020

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In the solutions A, B and C described above, at least the following are effective. 1. 1. alcohols having 1 to 20 carbon atoms 2. ethylene glycol, glycerin, propylene glycol, sorbit 3. Aromatic hydrocarbons having 6 to 60 carbon atoms 4. Hydrocarbons having 3 to 60 carbon atoms Water 6. Ethers represented by R1-O-R2, wherein R1 and R2 have 1 to 60 carbon atoms each. 7. 7. A hydrocarbon containing an aldehyde group or a carboxyl group and having 60 or less carbon atoms. Fatty acids, fats and oils 9. It is a hydrocarbon containing an ester bond and has 10 carbon atoms.
0 or less 10. As the liquefied nitrogen, oxygen, carbon dioxide and surfactant, at least the following are effective. 1. Nonionic surfactant 2. 2. Anionic surfactant 3. Cationic surfactant Alcohols and glycols, having 1 to 1 carbon atoms
6. More specifically, at least the following are effective. 1. 1. The following fatty acid esters: glycerin, sucrose, pentaerythritol, sorbitol 2. Alkyl ether of alcohol having 2 or more carbon atoms 3. Polyethylene glycol type surfactant, alkyl ether of polyhydric alcohol 4. Amino acid type and betaine type amphoteric surfactants 5. The following sulfonates or sulfates: alkylbenzenes, alcohols having 6 or more carbon atoms Ammonium salt type and amine salt type cationic surfactants ────────────────────────────────────── ───────────────

[Procedure amendment]

[Submission date] August 27, 2001 (2001.8.2
7)

[Procedure amendment 1]

[Document name to be amended] Statement

[Correction target item name] Claim 14

[Correction method] Change

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[Procedure amendment 2]

[Document name to be amended] Statement

[Correction target item name] Claim 16

[Correction method] Change

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[Procedure amendment 3]

[Document name to be amended] Statement

[Correction target item name] Claim 18

[Correction method] Change

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18. A process for further separating a separated product by adding a substance which dissolves, mixes or disperses with the liquids to a part or all of the liquids A to C constituting the liquid mixture. The separation method according to any one of claims 1 to 8, and the mixed solution according to (9) to (17), which comprises a step of separating the mixture.

[Procedure amendment]

[Date of submission] February 18, 2002 (2002.2.1
8)

[Procedure amendment 1]

[Document name to be amended] Drawing

[Correction target item name] Figure 2

[Correction method] Change

[Correction contents]

FIG. 2

Claims (18)

[Claims] 1. A method for separating an object to be extracted by changing the mixing ratio of a mixed solution of at least three types of solutions relatively or dynamically, wherein the relationship between the three types of solutions is at least all of the following: What satisfies. 1. Solution A and Solution B dissolve, mix or disperse in a free ratio. Solution A and Solution C dissolve, mix or disperse in a free ratio. 3. Liquid B and liquid C dissolve, mix or disperse in less than 10% of the other. Solution C dissolves, mixes, or disperses the separation target, but Solution A and B dissolves, mixes, or disperses less than 5%. 2. A part of the constituent solution is associated and precipitated with the dynamic change of the composition ratio of each component constituting the mixed solution, and the object to be extracted or the molecular assembly including the object to be extracted is included in the separated liquid. 2. The separation method according to claim 1, further comprising the step of: 3. A part of the constituent solution is associated and precipitated with the dynamic change of the composition ratio of each component constituting the mixed solution, and the object to be extracted or the molecular assembly including the object to be extracted is included in the deposited liquid. 3. The method according to claim 1, further comprising a step of incorporating a part of the component solution once deposited into the mixed solution by changing the composition ratio of each component constituting the mixed solution into a dynamic change. . 4. A molecular assembly is formed in the course of solution mixing,
4. The separation method according to claim 1, wherein the molecular assembly includes a step of forming a new molecular assembly including an object to be extracted according to a dynamic change in the composition ratio of each component constituting the mixed solution to which the molecular assembly belongs. . 5. The separation method according to claim 1, wherein said solution A, solution B and solution C are each selected from one or more of the following. 1. 1. alcohols having 1 to 20 carbon atoms 2. ethylene glycol, glycerin, propylene glycol, sorbit 3. Aromatic hydrocarbons having 6 to 60 carbon atoms 4. Cyclic hydrocarbons having 3 to 60 carbon atoms Water 6. Ethers represented by R1-O-R2, wherein R1 and R2 have 1 to 60 carbon atoms each. 7. 7. A hydrocarbon containing an aldehyde group or a carboxyl group and having 60 or less carbon atoms. Fatty acids, fats and oils 9. It is a hydrocarbon containing an ester bond and has 10 carbon atoms.
0 or less 10. Liquefied nitrogen, oxygen, carbon dioxide, 6. The separation method according to claim 1, wherein a surfactant is used. 7. The separation method according to claim 6, wherein one or more surfactants are selected from the following. 1. Nonionic surfactant 2. 2. Anionic surfactant 3. Cationic surfactant Amphoteric surfactant5. Alcohols and glycols, having 1 to 1 carbon atoms
What is 6 8. The separation method according to claim 6, wherein one or more surfactants are selected from the following. 1. 1. The following fatty acid esters: glycerin, sucrose, pentaerythritol, sorbitol 2. Alkyl ether of alcohol 3. Polyethylene glycol type surfactant, alkyl ether of polyhydric alcohol 4. Amino acid type and betaine type amphoteric surfactants 5. The following sulfonates or sulfates: alkylbenzenes, alcohols having 6 or more carbon atoms Ammonium salt type and amine salt type cationic surfactants 9. A mixed solution for separating an object to be extracted by changing the mixing ratio of a mixed solution of at least three types of solutions relatively or dynamically, wherein the relationship between the three types of solutions is at least: What satisfies all. 1. 1. Liquid A and liquid B are mixed or dispersed in a free ratio. 2. Liquid A and liquid C are mixed or dispersed in a free ratio. 3. Liquid B and liquid C are mixed or dispersed only in less than 10% of the other. Solution C dissolves, mixes, or disperses the separation target, but Solution A and B dissolves, mixes, or disperses less than 5%. 10. A dynamic change in the composition ratio of each component constituting the mixed solution causes a part of the constituent solution to associate and precipitate, and the extracted liquid or a molecular assembly including the extracted liquid in the deposited liquid. 10. The mixed solution according to claim 9, wherein 11. A part of the constituent solution is associated and precipitated with the dynamic change of the composition ratio of each component constituting the mixed solution, and the object to be extracted or the molecular assembly including the object to be extracted is included in the deposited liquid. 11. The mixed solution according to claim 9, wherein a part of the constituent solution once precipitated is again taken into the mixed solution by changing the composition ratio of each component constituting the mixed solution into a dynamic change. 12. A molecular assembly is formed in the course of solution mixing, and the molecular assembly includes a new molecule containing an object to be extracted according to a dynamic change in the composition ratio of each component constituting the mixed solution to which the molecular assembly belongs. The mixed solution according to any one of claims 9 to 11, which forms an aggregate. 13. The mixed solution according to claim 9, wherein said solution A, solution B and solution C are each selected from one or more of the following. 1. 1. alcohols having 1 to 20 carbon atoms 2. ethylene glycol, glycerin, propylene glycol, sorbit 3. Aromatic hydrocarbons having 6 to 60 carbon atoms 4. Cyclic hydrocarbons having 3 to 60 carbon atoms Water 6. Ethers represented by R1-O-R2, wherein R1 and R2 have 1 to 60 carbon atoms each. 7. 7. A hydrocarbon containing an aldehyde group or a carboxyl group and having 60 or less carbon atoms. Fatty acids, fats and oils 9. It is a hydrocarbon containing an ester bond and has 10 carbon atoms.
0 or less 10. Liquefied nitrogen, oxygen, carbon dioxide, 14. The method according to claim 9, wherein a surfactant is used.
Mixed solution. 15. The mixed solution according to claim 14, wherein one or more surfactants are selected from the following. 1. Nonionic surfactant 2. 2. Anionic surfactant 3. Cationic surfactant Amphoteric surfactant5. Alcohols and glycols, having 1 to 1 carbon atoms
What is 6 16. The mixed solution according to claim 8, wherein one or more surfactants are selected from the following. 1. 1. The following fatty acid esters: glycerin, sucrose, pentaerythritol, sorbitol 2. Alkyl ether of alcohol 3. Polyethylene glycol type surfactant, alkyl ether of polyhydric alcohol 4. Amino acid type and betaine type amphoteric surfactants 5. The following sulfonates or sulfates: alkylbenzenes, alcohols having 6 or more carbon atoms Ammonium salt type and amine salt type cationic surfactants 17. A mixed solution of at least three types of solutions, wherein the relationship between the three types of solutions satisfies at least all of the following. 1. Solution A and Solution B dissolve, mix or disperse in a free ratio. Solution A and Solution C dissolve, mix or disperse in a free ratio. 3. Liquid B and liquid C dissolve, mix or disperse in less than 10% of the other. 4. Solution C dissolves, mixes or disperses the object to be separated, but solution A and B dissolves, mixes or disperses less than 5%. When the volume composition ratio of each solution constituting the mixed solution is changed, a part of the solution is associated and precipitated, and when further changed, a part or all of the precipitated solution is recovered in the mixed solution. 18. A process for further separating a separated product by adding a substance which dissolves, mixes or disperses with the liquids to a part or all of the liquids A to C constituting the liquid mixture. 9. The separation method according to claim 1, further comprising the step of separating into pieces.