JPH06122601A - Encapsulant - Google Patents

Abstract

PURPOSE:To provide an encapsulant ready to encapsulate, exhibiting a high gelling speed, suitable for observation and administration of an encapsulated material and capable of readily taking out the encapsulated material again. CONSTITUTION:An encapsulant composed of a composition containing an amine compound of formula I [R1 to R3 are each H or a hydrocarbon group; R4 is H, a hydrocarbon group or O; The hydrocarbon group is 1 to 28C and the total number of C contained in R1 to R4 is 4 to 50; X<-> is an inorganic or organic acid residue; (n) is 0 in the case of R4=O<-> and 1 in other cases] and water, performing a reversible phase transition from a transparent liquid to a get state when the temperature is changed and capable of performing a phase transition from a liquid of <=200cP viscosity to a solid gel within a range of 3min by a change in temperature within a range of 3 deg.C from the phase transition temperature. As the compound of formula I, a quaternary ammonium salt of formula II (R1 to R4 are each an alkyl, an alkylene or an alkanol), an alkylamine of formula III (Y<->-R4 is sulfonic acid ion, sulfonate ion, phosphonate ion, nitrate ion, etc.) or an amine oxide of formula IV is preferably used.

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an encapsulating agent for enclosing and storing specimens, samples, products, etc. in cells, display cases, etc. The encapsulant is easy and has a high gelation speed, and is suitable for observing and appreciating the encapsulated product. Particularly, the encapsulant has a feature that the encapsulated product can be easily taken out again.

[0002]

2. Description of the Related Art Conventionally, gelatin has been used as an encapsulating agent.
High-concentration solution gels such as agar and polyoxyalkylene glycol are used, and polymer compounds such as curable acrylic resins, unsaturated polyester resins, and silicone resins are used.

Among these, high-concentration solution gels of gelatin, agar, polyoxyalkylene glycol, etc. can be returned to a liquid state by heating, but it takes time to prepare the gel and a high-temperature solution is also very high. It was difficult to prepare a viscous, difficult to handle and transparent gel.

Further, a high molecular compound such as a curable acrylic resin, an unsaturated polyester resin or a silicone resin is a highly transparent encapsulant, but it is a very viscous liquid even in a solution state and contains a curing agent. It is not easy to take out the encapsulated article because the handling method such as required is complicated, and once cured, it does not return to a liquid state easily.

Further, the phase change depending on the temperature of a high-concentration aqueous solution of a surfactant has been described in the following documents for a long time. For example, Shigeru Kuroiwa: “Oil Chemistry” Vol.34, 377, (1
985), Hironobu Kunieda: “Nikka”, 1977, (10), p.1428, Hironobu Kunieda: “Nikka”, 1977, (2), p, 151, Shigetaka Kuroiwa, Matsuda: “Nikka”, 1976 , (7), p.1040, Satoshi Tomomasa, Harusawa: "Oil Chemistry" Vo
l.36, 938, (1987), Shoji Fukushima, Michihiro Yamaguchi: "Oil Chemistry"
Vol.29,106, (1980), Hisao Tang: "Oil Chemistry" Vol.37,96
5, (1988), T. Hisao: “Nika”, 1981, (11), p.1691, Keizo Hagino: “Engineering” Vol.64,1021, T. Hisa, Ishida: “Oil Chemistry” Vol.33, 270, (1984), Shoji Fukushima, Michihiro Yamaguchi: “Oil Chemistry” Vol.29, 106, (1980), Takenori Maruyama, Shintani: “Oil Chemistry”
Vol. 27, 214, (1978), etc. However, the solutions of these surfactants have many drawbacks such as slow phase change speed, often colored and poor transparency due to turbidity, making it difficult to use as an encapsulant. Is.

[0006]

DISCLOSURE OF THE INVENTION The present invention improves the physical defects of the encapsulants conventionally used as described above, so that the encapsulating operation is easy and the gelling rate of the encapsulant is high. The purpose of the present invention is to provide a new encapsulant that is suitable for observing and appreciating encapsulated products and is easy to take out again.

[0007]

Means for Solving the Problems The inventors of the present invention have conducted various studies on the phase change of a highly concentrated aqueous solution of a surfactant, and as a result, an aqueous solution of a group of compounds containing an amine bond is reversible by a slight temperature change. In addition, it was found that the phase changes rapidly between a transparent liquid and a gel state. Therefore, when used as an encapsulant when storing specimens / samples in cells, etc., it is easy to enclose and remove the sample, and the biological tissue of the sample does not change. Got Furthermore,
Based on this, the range of compounds having such physical properties and the method of controlling the gelation temperature were examined, and the present invention was reached.

That is, the composition is composed of an amine compound represented by the chemical formula 5 and water, and reversibly undergoes a phase change between a transparent liquid and a gel state by a temperature change.
The encapsulant is characterized in that the viscosity changes from 200 centipoise or less to a solid gel within 3 minutes by a temperature change within ℃.

[0009]

[Chemical 5]

Here, R ₁ , R ₂ and R ₃ are hydrogen or a hydrocarbon group, R ₄ is a hydrogen or hydrocarbon group or O ⁻ , and the hydrocarbon group has _{1 to} 28 carbon atoms and R _{1 to} R ₄ Has a total carbon number of 4 to 50. X ⁻ is an inorganic or organic acid residue, n is R ₄ is O
^- In case of 0, the other is 1.

Alternatively, a phase change temperature controlling agent may be added to the above composition, wherein the content of the amine compound is 15 to 80%, and the content of the phase changing temperature controlling agent is the sum of water and the phase change temperature controlling agent. More preferably, it has a composition of 0 to 80%.

Here, the solid gel has a diameter of 6.
10 cm when a steel ball with a weight of 4 mm and a load of 1.0 g is placed and dropped
Indicates the state of gel in which the time required to fall is 1 minute or more. The present invention will be described in detail below.

The composition of the present invention must contain the amine compound represented by Chemical Formula 5. Among these, for example, the quaternary ammonium salt represented by the chemical formula 6, the alkylamine represented by the chemical formula 7, and the amine oxide represented by the chemical formula 8 are preferable as components of the composition of the present invention.

[0014]

[Chemical 6]

[0015]

[Chemical 7]

[0016]

[Chemical 8]

Here, R ₁ , R ₂ , R ₃ and R ₄ are hydrogen or a single or mixed alkyl group having 1 to 28 carbon atoms, an alkylene group, an alkanol group, and in the chain and / or side chain. May contain one or more hetero atoms, unsaturated groups, amide bonds, and aromatic rings, and the total number of carbon atoms of R _{1 to} R ₄ is ₄ to 50.

X ⁻ is a halogen group, a residue of a dialkyl sulfate, a residue of a trialkyl phosphate ester, a sulfonate ion, a sulfonate ion, a phosphonate ion, a phosphonate ion, a nitrate ion or an eruvate ion. Is a residue of an inorganic acid or an organic acid containing. Y ⁻ −R ₄ is a residue of an inorganic or organic acid containing a sulfonate ion, a sulfonate ion, a phosphonate ion, a phosphonate ion, a nitrate ion, and a carboxylate ion.

Examples of the single or mixed alkyl group having 1 to 28 carbon atoms include the following groups.

Examples of a single alkyl group include methyl, ethyl, n-propyl, iso-propyl, n-butyl, is
o-butyl, sec-butyl, ter-butyl, n-amyl (pentyl), iso-amyl (pentyl), sec-amyl, ter-amyl (pentyl), n-hexyl, n-heptyl, n-octyl, iso -Octyl, sec-octyl, 2-ethylhexyl,
n-nonyl, iso-nonyl, n-decyl, n-undecyl, n-dodecyl (lauryl), n-tridecyl, iso-tridecyl,
n-tetradecyl (myristyl), n-pentadecyl, n-hexadecyl, n-heptadecyl (palmityl), n-octadecyl (stearyl), n-octadecenyl (oleyl)
, Iso-octadecyl (isostearyl), n-nonadecyl, n-eicosyl, n-docosyl, n-tricosyl, n-tetracosyl, n-pentacosyl, n-hexacosyl, n-heptacosyl, n-octacosyl, n-heptacosyl, n -Octacosyl group and the like.

The mixed alkyl groups include coconut alkyl, coconut alkyl, beef tallow alkyl, hardened beef tallow alkyl, soybean alkyl, octyl / lauryl mixture, lauryl / myristyl mixture, lauryl / palmityl mixture, myristyl / palmityl mixture, palmityl / stearyl mixture, Stearyl / oleyl mixed groups and the like.

Examples of the alkylene group having 1 to 28 carbon atoms, which may be used alone or in combination, include the following groups.

Examples of the aliphatic alkylene group include methylene, ethylene, propylene, butylene, hexylene, heptylene, octylene, nonylene, decylene, undecylene, dodecylene, tridecylene, tetradecylene, heptadecylene, hexadecylene, octadecylene, octadecylene, nonadecylene, eicosylene, hen. Eicosylene, docosylene, tricosylene, tetracosylene, pentacosylene, hexacosylene, heptacosylene, octacosylene group and the like.

The alkylene group containing an aromatic ring includes benzyl, cyclohexyl, mono- or polystyrylbenzyl group and the like.

Examples of the monooxyalkylene group include monooxyethylene, monooxypropylene, monooxybutylene, monooxypentylene, monooxyhexylene,
Examples include monooxyheptylene and monooxyoctylene groups.

As the polyoxyalkylene group, dioxyethylene, dioxypropylene, dioxybutylene,
Dioxypentylene, dioxyhexylene, dioxyheptylene, dioxyoctylene, trioxyethylene,
Trioxypropylene, trioxybutylene, trioxypentylene, trioxyhexylene, trioxyheptylene, trioxyoctylene, polyoxyethylene,
Examples thereof include polyoxypropylene, polyoxybutylene, polyoxypentylene, polyoxyhexylene, polyoxyheptylene, and polyoxyoctylene groups.

As the monohydroxyalkylene group, monohydroxyethylene, monohydroxypropylene, monohydroxybutylene, monohydroxypentylene, monohydroxyhexylene, monohydroxyheptylene,
A monohydroxyoctylene group and the like.

Examples of the polyhydroxyalkylene group include dihydroxyethylene, dihydroxypropylene, dihydroxybutylene, dihydroxypentylene, dihydroxyhexylene, dihydroxyheptylene, polyhydroxyethylene, polyhydroxypropylene, polyhydroxybutylene, polyhydroxypentylene, and polyhydroxypentylene. Examples thereof include hydroxyhexylene, polyhydroxyheptylene, polyhydroxyoctylene groups and the like.

Examples of the alkanol group having 1 to 28 carbon atoms, which may be used alone or in combination, include the following groups.

Examples of monoalkanol groups include methanol, ethanol, propanol, pentanol, hexanol, heptanol, and octanol groups.

Examples of the monooxyalkanol group include monooxyethyl ethanol, monooxypropyl propanol, monooxybutyl butanol groups and the like.

Examples of the polyoxyalkanol group include dioxyethyl ethanol, dioxypropyl propanol, dioxybutyl butanol, dioxypentyl pentanol, dioxyhexyl hexanol, trioxyethyl ethanol, trioxypropyl propanol and trioxypropyl propanol. Oxybutyl butanol, trioxypentyl pentanol, trioxyhexyl hexanol, polyoxyethyl ethanol, polyoxypropyl propanol, polyoxybutyl butanol, polyoxypentyl pentanol, polyoxyhexyl hexanol groups, etc. Is.

As the monohydroxyhectanol group,
Examples thereof include monohydroxyethanol, monohydroxypropanol, monohydroxybutanol, monohydroxyhexanol, monohydroxyheptanol and monohydroxyoctanol groups.

Further, monohydroxyethyl ethanol, monohydroxypropyl propanol, monohydroxybutyl butanol, dihydroxyethyl ethanol, dihydroxypropyl propanol, dihydroxy disibutyl butanol, trihydroxyethyl ethanol, trihydroxypropyl propanol. , Trihydroxybutyl, butanol and the like.

Furthermore, polyhydroxyalkanol groups such as polyhydroxyethyl ethanol, polyhydroxypropyl propanol and polyhydroxybutyl butanol are also included.

R ₁ also includes an alkylamine having at least one or more long-chain alkyl groups and having an amide bond, and an alkylamine containing a polyamine and a long-chain alkyl group, represented by Chemical Formula 9.

[0037]

[Chemical 9]

Where R ₅ is independent or mixed C ₆ -C ₂₈
, R ₆ and R ₇ are independently or simultaneously hydrogen, independently or mixed C ₁ -C ₂₈ alkyl group, alkylene group, alkanol group. Independent or mixed C _6- C
The alkyl group of ₂₈ is a group having C ₆ or more among the alkyl groups described in the chemical formula 6. In addition, C _{1 to} C ₂₈ alkyl groups, alkylene groups, and alkanol groups also have the chemical formula 6
Refers to the group described above. In addition, m is an integer of 1 to 10, n is an integer of 0 to 10, and z is an integer of 0 to 10.

The halogen group is chlorine, bromine, fluoro group or the like. Further, the residue of dialkylsulfate refers to a residue of dimethylsulfate, a residue of diethylsulfate, a residue of monomethylmonoethyl / sulfate, a residue of dipropylsulfate, a residue of dibutylsulfate and the like.

The residue of trialkyl phosphate ester means a residue of trimethyl phosphate ester, a residue of triethyl phosphate ester, a residue of tripropyl phosphate ester, a residue of tributyl phosphate ester and the like.

Sulfonate ion, sulfonate ion, phosphonate ion, phosphonate ion,
The residue of an inorganic acid or an organic acid containing a nitrate ion or a carboxylate ion means, for example, the residue of the following acid.

Inorganic acids such as sulfuric acid, sulfurous acid, hyposulfuric acid, orthophosphoric acid, pyrophosphoric acid, tripolyphosphoric acid, polyphosphoric acid and nitric acid, and formic acid, acetic acid, propionic acid, butyric acid, valeric acid, capric acid, caproic acid, octyl acid, Nonanoic acid, decanoic acid,
Undecanoic acid, lauric acid, palmitic acid, stearic acid, oleic acid, linoleic acid, aliphatic monocarboxylic acids such as linolenic acid, and adipic acid, sebacic acid, azelaic acid and other aliphatic dicarboxylic acids, lactic acid, glycolic acid, DL
-Malilic acid, L (+)-tartaric acid, maleic acid, succinic acid, itaconic acid, citric acid, gluconic acid, ricinoleic acid, and other aliphatic monocarboxylic acids or aliphatic polycarboxylic acids containing hydroxyl groups, double bonds, etc. Etc.

Further, 1-hydroxyethylidene-1,
1-diphosphonic acid, amino tris (ethylene phosphonic acid, paratoluene sulfonic acid, benzoic acid, sulphonic acid ions such as salicylic acid, phosphonic acid ions, residues of organic acids containing aromatic rings, etc. are also included. .

An aqueous solution of the amine compound represented by the chemical formula 5 is an essential component of the composition of the present invention, and water is the most preferable solvent for the amine compound of the present invention.

The composition of the present invention may further contain a phase change temperature controlling agent. In the composition of the present invention, the content of the amine compound represented by Chemical Formula 1 is 15 to 80%, and the content of the phase change temperature controlling agent is 0 relative to the total amount of water and the phase change temperature controlling agent.
The range of up to 80% is preferred. Amine compound content is 15%
If the water content is less than or equal to 85%, the gelling temperature lowers and the gel may change phase during storage to become a solution, which is not preferable.

As the phase change temperature controlling agent, monohydric or polyhydric alcohols, dihydric alcohol alkyl ethers,
Organic acid esters of dihydric alcohol alkyl ethers are preferred.

Examples of monohydric or polyhydric alcohols include monohydric alcohols such as methanol, ethanol, propanol, butanol, amyl alcohol, hexyl alcohol, heptyl alcohol and octyl alcohol.
Monoalkylene glycols such as ethylene glycol, propylene glycol, butylene glycol, and octylene glycol. Polyethylene glycol such as diethylene glycol, triethylene glycol, tetraethylene glycol, polyethylene glycol, dipropylene glycol, tripropylene glycol, tetrapropylene glycol, polypropylene glycol, dibutylene glycol, tributylene glycol, tetrabutylene glycol, polyethylene butylene glycol, etc. is there.

Further, mono- or polyglycerin such as glycerin, diglycerin, triglycerin, tetraglycerin, polyglycerin and the like, and polyalkylolalkyl such as trimethylolmethane, trimethylolethane, trimethylolpropane, trimethylolbutane and the like.

The following compounds can be used as the alkyl ether of dihydric alcohol. For example, ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, ethylene glycol monopropyl ether, ethylene glycol monobutyl ether, propylene glycol monomethyl ether, propylene glycol monoethyl ether, propylene glycol monopropyl ether, propylene glycol monobutyl ether, and other monoalkylene glycols. It is an alkyl ether.

Further, diethylene glycol monomethyl ether, diethylene glycol monoethyl ether, diethylene glycol monopropyl ether, diethylene glycol monobutyl ether, dipropylene glycol monomethyl ether, dipropylene glycol monoethyl ether, dipropylene glycol monopropyl ether, dipropylene glycol monobutyl ether, etc. It is a monoalkylene glycol alkyl ether.

Further, it is an alkyl ether of mono- or polyhydroxyl alkylene alcohol such as isopropylene glycol, solfit (3-methyl-3-methoxybutanol) and hexylene glycol.

As the organic acid ester of alkyl ether of dihydric alcohol, solfit acetate is used.
Organic acid esters of mono- or polyhydroxyl alkylene alcohols such as (3-methyl-3methoxy-butanol-acetate) can be used.

To prepare the composition of the present invention, the starting amine compound is dispersed in heated water, and a quaternizing agent for preparing the amine compound represented by Chemical Formula 5, an inorganic acid or an organic acid is added dropwise. The composition of the present invention can be prepared by a conventional method. If necessary, a composition having a property of phase change in a predetermined temperature range is prepared by adding a phase change temperature controlling agent before or after addition of the quaternizing agent or the like.

The composition prepared as described above, that is, the encapsulant of the present invention is transparent and mainly reversibly changes the temperature of the liquid on the high temperature side and the temperature on the low temperature side by a slight temperature change within the temperature range of 20 to 70 ° C. It has the characteristic of changing phase with gel.

To enclose a specimen, sample, etc. using the encapsulant of the present invention, the composition is placed in a warm water bath or a constant temperature bath,
A uniform transparent low-viscosity liquid is prepared by heating to a temperature 5 to 10 ° C. higher than the phase change temperature. On the other hand, the sample is placed in a container for enclosing the sample, the sample, etc., preheated and kept at a temperature 5 to 10 ° C. higher than the phase change temperature, the aqueous solution of the composition is injected, and the mixture is left at room temperature. Upon cooling, a sample is obtained which is encapsulated in a transparent, elastic gel.

Further, the sample enclosed in the gel is placed in a warm water bath or a constant temperature bath together with the container at a temperature of 5 ° C or below the phase change temperature.
Heat up to ~ 10 ° C higher to return to a clear, low-viscosity liquid,
The sample can be removed again.

[0057]

EXAMPLES The present invention will be described in more detail with reference to the following examples. The parts and% described in the examples are parts by weight and% by weight. The methods for measuring viscosity, transparency and gel hardness are as follows.

[Viscosity measuring method] Using a BL-type viscometer manufactured by Tokyo Keiki Co., Ltd., 400 g of the sample was put into a cylindrical glass container having an inner diameter of 70 mm and a height of 110 mm, and at 70 ° C. for 2 hours or more. After keeping the temperature, it was measured while gradually cooling at a rate of 2 ° C./min. The unit of viscosity is expressed in centipoise.

[Transparency Measuring Method] manufactured by Hitachi, Ltd.
Using a 100-10 type spectrophotometer, heat the sample to be measured above the phase change temperature into a 10 mm glass cell, leave it in a thermostatic chamber at 20 ° C for 30 minutes or longer, and then use a tungsten lamp as a light source. The transmittance was measured at a wavelength of 470 nm. The unit of transparency is
Display in% transmittance.

[Method for Measuring Gel Hardness] A measurement sample is heated to a temperature not lower than the phase change temperature to make it liquid, and then put into a colorimetric tube having an inner diameter of 20 mm. While gradually cooling the colorimetric tube at a rate of 2 ° C / minute, the colorimetric tube is allowed to stand for 30 minutes or more at a temperature 3 ° C lower than the center of the phase change temperature.

A diameter of 6.4 mm and a load of 1.0 g on the surface of the measurement sample
The steel ball of No. 1 was placed on it, and the time it took to fall at a distance of 10 cm was measured. When the drop time measured by this method was 1 minute or more, it was indicated as a firm gel.

Example 1 Dimethyllaurylamine 65.7
Part (0.300 mol) is dispersed in 40.0 parts of warm water heated to 80 ° C., and 47.3 parts (0.315 mol) of L (+) tartaric acid (natural type) is added.
What was melt | dissolved in 35.0 parts of warm water heated at 80 degreeC is dripped slowly. During the dropping, a soft gel is mixed in the transparent liquid. After the dropping is completed, the mixture is slowly stirred while maintaining the temperature at 80 to 90 ° C., and reacted until the whole becomes a uniform liquid, and then cooled to room temperature.

The third product obtained by the above reaction and having a solid content of 60%
An aqueous solution of an organic acid salt of a primary amine is a homogeneous and transparent low-viscosity liquid at a temperature of 38 ° C or higher, and changes to a colorless and transparent elastic gel at a temperature of 36 ° C or lower. When gelled at 36 ° C or lower, if it is heated again to a temperature of 38 ° C or higher, it returns to a low viscosity liquid. This change from a low-viscosity liquid to an elastic solid occurs rapidly, completely and reversibly with a temperature change of about 2 ° C from 38 ° C to 36 ° C.

The above reaction product has a viscosity of 110 centipoise at 40 ° C., which is 3 ° C. higher than the center of the phase change temperature, and the gel at 34 ° C. which is 3 ° C. lower than the center of the phase change temperature has a sedimentation time of 5 minutes. That was all and it was solid. The transparency was 99.5%.

The aqueous solution of the organic acid salt of the tertiary amine was heated in a warm water bath to obtain a uniform transparent low viscosity liquid. A cutter knife made of preheated transparent styrene resin with a width of 10 cm, a depth of 10 cm, and a height of 5 cm, and a lid with a lid. What was incised by the median line was immersed in a commercially available 2% aqueous solution of aluminum sulfate for 1 hour in advance, and the solution of the present composition which had been preheated was injected and gelled to prepare a sample. This specimen has petals, stamens, pistils,
The shape and color of the sepals, flowers, and floral patterns were clearly discernible with the naked eye, and it was the best teaching material for science education.

This sample can be stored in multiple layers in a room at room temperature by simply sealing the lid of a square case with cellophane tape, and it can be discolored or deformed even after storage for one month. No alteration was observed.

Example 2 Dimethyllaurylamine 29.9
Parts (0.1404 mol) were dispersed in a mixture of 40.0 parts of warm water heated to 80 ° C. and 10.0 parts of propylene glycol to give 80 to 90 parts.
20.1 parts of trimethyl phosphate (0.14
(35 mol) is slowly added dropwise. After completion of dropping, the reaction product was dissolved in 1% of the apparent pH of ion-exchanged water to obtain a PH solution.
However, after continuing the reaction until it becomes 5.0 ± 0.5, cool to room temperature.

The fourth product obtained by the above reaction and having a solid content of 50%
The aqueous solution of the primary ammonium salt is a uniform and transparent low-viscosity liquid at a temperature of 39 ° C or higher, and changes to a colorless and transparent elastic gel at 37 ° C or lower. When the gelled substance at 37 ° C or lower is heated again to a temperature of 39 ° C or higher, it becomes a low-viscosity liquid.

This change from a low-viscosity liquid to an elastic gel occurs promptly, completely and reversibly with a temperature change of about 2 ° C. from 39 ° C. to 37 ° C.

The above-mentioned reaction product has a viscosity of 90 centipoise at 41 ° C. which is 3 ° C. higher than the center of the phase change temperature, and the gel at 35 ° C. which is 3 ° C. lower than the center of the phase change temperature has a settling time of 10
It was more than a minute and hard enough. The transparency is 99.5%.
Met.

The above aqueous solution of quaternary ammonium salt having a solid content of 50% was heated to 45 ° C. in a warm water bath to obtain a uniform transparent low viscosity liquid, and then heated to 40 ° C. in advance. Pour onto a commercially available goldfish (wakin) with a body length of 3 cm placed in a wide-mouthed specimen bottle, leave it at room temperature, and allow it to cool. Gelation started within 1 to 2 minutes, and a preservation sample of a goldfish (wakin) enclosed in a colorless and transparent elastic gel was obtained.
The goldfish (wakin) storage sample enclosed in the glass wide-mouthed sample bottle did not break even when moved or transported.

The above goldfish (wakin) storage sample enclosed in the glass wide-mouthed sample bottle remained a colorless and transparent elastic gel even after storage for one year at room temperature. After one year of storage, the goldfish (wakin) storage sample enclosed in a glass wide-mouthed sample bottle was heated to 40 ° C in a warm water bath to return it to a uniform transparent low-viscosity liquid, and then An aqueous solution of a quaternary ammonium salt type cationic surfactant was poured into the bottle of No. 1 and washed briefly with water, and then the goldfish (wakin) was taken out.

Example 3 Dimethyllaurylamine 65.7
Parts (0.300 mol) are dispersed in 118.4 parts of warm water heated to 80 ° C., and 39.9 parts (0.315 mol) of glycolic acid having a solid content of 60% are slowly added dropwise.

During the dropping, a soft jelly was added to the transparent liquid.
Although a substance is formed, it becomes a uniform and transparent low-viscosity liquid at the end of the dropping. Continue stirring slowly for 30 minutes while maintaining the temperature at 80-90 ℃, then cool to room temperature.

A third 40% solids product obtained from the above reaction.
An aqueous solution of an organic acid salt of a primary amine is a homogeneous and transparent low-viscosity liquid at a temperature of 38 ° C or higher, and changes to a colorless and transparent elastic gel at a temperature of 36 ° C or lower. If the gelled substance at 38 ° C or lower is heated again to a temperature of 36 ° C or higher, it becomes a low-viscosity liquid.

This change from a low-viscosity liquid to an elastic gel occurs rapidly, completely and reversibly with a temperature change of about 2 ° C. from 38 ° C. to 36 ° C.

The viscosity of the above reaction product at 40 ° C., which is 3 ° C. higher than the center of the phase change temperature, is 98 centipoise, and the gel at 34 ° C., which is 3 ° C. lower than the center of the phase change temperature, has a sedimentation time of 5
It was more than a minute. This product was colored slightly pale yellow, but the transparency was 93.5%.

Example 4 Dimethyllaurylamine 70.1
Part (0.320 mol) is dispersed in 72.3 parts of warm water heated to 80 ° C, and 22.5 parts (0.168 mol) of DL-malic acid dissolved in 30.0 parts of warm water heated to 80 ° C is slowly added dropwise. .
During the dropping, a soft gel is mixed in the transparent liquid. After the completion of dropping, the mixture is slowly stirred while maintaining the temperature at 80 to 90 ° C., reacting until the whole becomes a uniform liquid, and then cooled to room temperature.

The aqueous solution of an organic acid salt of a tertiary amine having a solid content of 47.5% obtained by the above reaction is a uniform and transparent low-viscosity liquid at a temperature of 41 ° C. or higher, and a colorless and transparent liquid at 39 ° C. or lower. Turns into a resilient solid. When gelled at 39 ° C or lower, if it is heated again to a temperature of 41 ° C or higher, it returns to a low-viscosity liquid. This change from a low viscosity liquid to an elastic gel occurs rapidly, completely and reversibly with a temperature change of about 2 ° C from 41 ° C to 39 ° C. The viscosity of the above reaction product at 43 ° C, which is 3 ° C higher than the center of the phase change temperature, is 130 centipoise, and is 37 ° C, 3 ° C lower than the center of the phase change temperature.
The gel set forth above had a settling time of 10 minutes or more and was sufficiently firm.
The transparency was 93.5%.

Example 5 216.8 parts of an aqueous solution of dihydroxyethyllaurylamine oxide having a solid content of 40% was depressurized with a vacuum pump while heating to 80 ° C. to dehydrate 59.2 parts of water, and then to normal pressure. Return and cool to room temperature.

The aqueous solution of amine oxide having a solid content of 55% obtained by the above reaction is a uniform transparent low viscosity liquid at a temperature of 45 ° C. or higher, and a pale yellow transparent elastic solid at 43 ° C. or lower. Changes to. When a substance that has gelled at 43 ° C or lower is heated again to a temperature of 45 ° C or higher, it returns to a low-viscosity liquid.

This change from a low-viscosity liquid to an elastic gel occurs rapidly, completely and reversibly with a temperature change of about 2 ° C. from 45 ° C. to 43 ° C.

The above-mentioned reaction product has a viscosity of 98 centipoise at 47 ° C. which is 3 ° C. higher than the center of the phase change temperature, and the gel settling time at 41 ° C. which is 3 ° C. lower than the center of the phase change temperature is 3 minutes or less. It was tough. The transparency was 92%.

Using this reaction product, the same procedure as in Example 1 was carried out.
cha (Mont.) Sacc.] was used to create archival specimens.
The archival sample was a pale yellow, transparent, elastic solid.

After storage for one year, the regenerated sample in the original state could be taken out in the same manner as in Example 1.

(Example 6) 401.1 parts (1.050 mol) of stearic acid diethylaminoethylamide having a total amine value of 146.9 and 3-methyl-3-methoxybutanol [Co., Ltd.]
Kuraray's Solfit] A mixture of 64.1 parts and 100 parts of water is heated to 80 ° C and dispersed. To this, 75.0 parts (0.500 mol) of L (+) tartaric acid (natural type) was added to warm water at 80 ° C 92.3
What was melt | dissolved in the part was slowly dripped, and it stirred until it became a uniform transparent solution.

The third product obtained by the above reaction and having a solid content of 65% was used.
74.0 parts (1.00 mol) of glycidyl was slowly added dropwise over 1 hour while maintaining the aqueous solution of the organic acid salt of primary amine at 80 ° C.

After completion of the dropping, stirring was continued slowly while maintaining the temperature at 80 to 90 ° C. for about 2 hours, and the pH of the solution prepared by dissolving the reaction product in 1% of apparent ion-exchanged water was 5.0 ± 0.5.
Continue the reaction until it becomes, then add 233.7 parts of water and cool to room temperature.

The fourth product obtained by the above reaction and having a solid content of 60%
The aqueous solution of the primary ammonium salt is a uniform and transparent low-viscosity liquid at a temperature of 54 ° C or higher, and changes to a colorless and transparent elastic gel at a temperature of 52 ° C or lower. When the gelled substance at 52 ° C or lower is heated again to a temperature of 54 ° C or higher, it becomes a low-viscosity liquid.

The change from the low-viscosity liquid to the elastic gel occurs rapidly, completely and reversibly with a temperature change of about 2 ° C. from 54 ° C. to 52 ° C.

The above-mentioned reaction product has a viscosity of 120 centipoise at 56 ° C., which is 3 ° C. higher than the center of the phase change temperature, and the gel at 50 ° C. which is 3 ° C. lower than the center of the phase change temperature has a settling time.
It was 10 minutes or more and was sufficiently hard. The transparency was 93%.

Petunia petals with white and red petals were placed in a glass wide-mouth specimen bottle in the same manner as in Example 2.
Stems and leaves were soaked in a commercially available 2% aqueous solution of magnesium chloride for 1 hour in advance, and then preserved specimens were prepared.

Example 7 Stearic acid diethylaminoethylamide having a total amine value of 146.9 76.4 parts (0.200 mol)
Is dispersed in 70.0 parts of warm water heated to 80 ° C., 43.7 parts (0.300 mol) of adipic acid is made into a slurry with 50.2 parts of warm water heated to 80 ° C., and slowly added.

During the dropping, a soft gel is mixed in the transparent liquid. After the completion of dropping, the mixture is slowly stirred while maintaining the temperature at 80 to 90 ° C., reacting until the whole becomes a uniform liquid, and then cooled to room temperature.

An aqueous solution of an organic hydrochloric acid of a tertiary amine containing an amide bond having a solid content of 50% obtained in the above reaction was 42 ° C.
It is a uniform transparent low viscosity liquid at the above temperature, and changes to a colorless and transparent elastic gel at 40 ° C or lower. When gelled at 40 ° C or lower, if it is heated again to a temperature of 42 ° C or higher, it returns to a low-viscosity liquid.

The change from the low-viscosity liquid to the elastic gel occurs rapidly, completely and reversibly with a temperature change of about 2 ° C. from 42 ° C. to 40 ° C.

The above-mentioned reaction product has a viscosity of 75 centipoise at 44 ° C. which is 3 ° C. higher than the center of the phase change temperature, and the gel at 38 ° C. which is 3 ° C. lower than the center of the phase change temperature has a settling time of 5
It was more than a minute and hard. The transparency was 90.5%.

(Example 8) In the same manner as in Example 2, the solid content of the L (+) tartaric acid (natural type) salt of dimethyllaurylamine was from 65% to 57.5%, and 4 points in 2.5% increments. Created. In the same manner as in Example 3, five dimethyllaurylamine glycolate solids having a solid content of 47.5 to 37.5% were prepared in increments of 2.5%.

In the same manner as in Example 4, the solid content of dimethyllaurylamine DL-malate was 52.5% to 4%.
Four points up to 5.0% were made in increments of 2.5%.

Table 1 shows the characteristics of these products during the phase change from liquid to gel and the properties of the gel phase.

[0101]

[Table 1]

The properties of these compositions of the present invention during the phase change from liquid to gel and the properties of the gel phase could be adjusted within a certain range by changing the solution concentration of the compound.

(Example 9) In the same manner as in Example 3 and Example 8, part of the warm water of the dimethyllaurylamine glycolate was replaced with glycerin, propylene glycol, ethylene glycol monomethyl ether or the like. hand,
A compound was prepared by changing the mixing ratio of various compounds.

Table 2 shows the characteristics of these products at the time of phase change from liquid to gel and the properties of the gel phase.

[0105]

[Table 2]

The properties of these products of the present invention during the phase change from liquid to gel and the properties of the gel phase can be adjusted within a certain range by changing the mixing ratio of the compounds.

(Example 10) The same procedure as in Examples 2 and 8 and 9 was carried out using warm water of a quaternary ammonium salt type cationic surfactant formed by trimethylphosphoric acid ester of dimethyllaurylamine. Part of it is replaced with ethylene glycol, propylene glycol, dipropylene glycol, dipropylene glycol monomethyl ether, glycerin, diglycerin, ethylene glycol monomethyl ether, solfit and solfit acetate, which are phase change temperature regulators, and various A compound was prepared by changing the mixing ratio of the compound.

Table 3 shows the characteristics of these products during the phase change from liquid to gel and the properties of the gel phase.

[0109]

[Table 3]

The properties of these products of the present invention during the phase change from liquid to gel and the properties of the gel phase can be adjusted within the range of 20 to 70 ° C. by changing the mixing ratio of the compounds.

[0111]

INDUSTRIAL APPLICABILITY The encapsulant of the present invention is easy to enclose, has a high gelation rate of the encapsulant, is suitable for observing and appreciating the encapsulated product, and is easy to take out the sample again. Various flora and fauna,
It can be applied to many applications such as tissue samples, various samples, and product sample displays, and can enhance the product value.

[Procedure amendment]

[Submission date] July 23, 1992

[Procedure Amendment 1]

[Document name to be amended] Statement

[Name of item to be corrected] Claim 4

[Correction method] Change

[Correction content]

[Chemical 3] R ₁ , R ₂ and R ₃ are the same as in Chemical Formula 2. The Y ^- -R ₄ is the residue of an inorganic or organic acid containing sulfonium <br/> phosphate ion or sulfonate ion, phosphonic acid ion, phosphonate ion, nitrate ion, a carboxylate ion.

[Procedure Amendment 2]

[Document name to be amended] Statement

[Correction target item name] 0004

[Correction method] Change

[Correction content]

Further, a high molecular compound such as a curable acrylic resin, an unsaturated polyester resin or a silicone resin is a highly transparent encapsulant, but it is a very viscous liquid even in a solution state and contains a curing agent. The handling method is complicated, such as required, and once cured, it does not return to a liquid state easily, so the encapsulated article can not be taken out .

[Procedure 3]

[Document name to be amended] Statement

[Correction target item name] 0013

[Correction method] Change

[Correction content]

The composition of the present invention must contain the amine compound represented by Chemical Formula 5. Among them for example, quaternary ammonium salt shown in Chemical Formula 6 or alkylamine salt shown in Chemical Formula 7, amine oxides shown in Formula 8 is preferred as a component of a composition of the present invention.

[Procedure amendment 4]

[Document name to be amended] Statement

[Correction target item name] 0018

[Correction method] Change

[Correction content]

[0018] X ^- a halogen group, or the residue of a dialkyl sulfate, residues of trialkyl phosphate or sulfonate ion, sulfonate ion, phosphonic acid ion, phosphonate ion, nitrate ion, Ca Le < It is a residue of an inorganic acid or an organic acid containing a borate ion. The Y ^- -R ₄ is the residue of an inorganic or organic acid include sulfonium phosphate ion or sulfonate ion, phosphonic acid ion, phosphonate ion, nitrate ion, a carboxylate ion.

[Procedure Amendment 5]

[Document name to be amended] Statement

[Correction target item name] 0020

[Correction method] Change

[Correction content]

Examples of a single alkyl group include methyl, ethyl, n-propyl, iso-propyl, n-butyl, is
o-butyl, sec-butyl, te rt -butyl, n-amyl (pentyl), iso-amyl (pentyl), sec-amyl (pliers )
) , Te rt -amyl (pentyl), n-hexyl, n-heptyl, n-octyl, iso-octyl, sec-octyl, 2-ethylhexyl, n-nonyl, iso-nonyl, n-decyl, n-undecyl , N-dodecyl (lauryl), n-tridecyl, is
o-Tridecyl, n-tetradecyl (myristyl), n-pentadecyl, n-hexadecyl (palmityl) , n-heptadecyl, n-octadecyl (stearyl), n-octadecenyl (oleyl), iso-octadecyl (isostearyl)
, N -nonadecyl, n-eicosyl, n-heneicosyl, n
-Docosyl, n-tricosyl, n-tetracosyl, n-pentacosyl, n-hexacosyl, n-heptacosyl, n-octacosyl group and the like.

[Procedure correction 6]

[Document name to be amended] Statement

[Name of item to be corrected] 0023

[Correction method] Change

[Correction content]

[0023] In the aliphatic alkylene group such as methylene, ethylene, propylene, butylene, hexylene,
Heptylene, octylene, nonylene, decylene, undecylene, dodecylene, tridecylene, tetradecylene,
Hexadecylene, heptadecylene, octadecylene, octadecenylene, nonadecylene, eicosylene, heneicosylene, docosylene, tricosylene, tetracosylene, pentacosylene, hexacosylene, heptacosylene, octacosylene group and the like.

[Procedure Amendment 7]

[Document name to be amended] Statement

[Correction target item name] 0033

[Correction method] Change

[Correction content]

[0033] as mono-hydroxy alkanols group,
Examples thereof include monohydroxyethanol, monohydroxypropanol, monohydroxybutanol, monohydroxyhexanol, monohydroxyheptanol and monohydroxyoctanol groups.

[Procedure Amendment 8]

[Document name to be amended] Statement

[Correction target item name] 0034

[Correction method] Change

[Correction content]

Further, monohydroxyethyl ethanol, monohydroxypropyl propanol, monohydroxybutyl butanol, dihydroxyethyl ethanol, dihydroxypropyl propanol, dihydroxybutyl butanol, trihydroxyethyl ethanol, trihydroxypropyl propanol, Examples include trihydroxybutyl and butanol.

[Procedure Amendment 9]

[Document name to be amended] Statement

[Name of item to be corrected] 0037

[Correction method] Change

[Correction content]

[0037]

[Chemical 9]

[Procedure Amendment 10]

[Document name to be amended] Statement

[Correction target item name] 0038

[Correction method] Change

[Correction content]

Where R ₅ is independent or mixed C ₆ -C ₂₈
, R ₆ and R ₇ are independently or simultaneously hydrogen, independently or mixed C ₁ -C ₂₈ alkyl group, alkylene group, alkanol group. Independent or mixed C _6- C
The alkyl group of ₂₈ is a group having C ₆ or more among the alkyl groups described in the chemical formula 6. In addition, C _{1 to} C ₂₈ alkyl groups, alkylene groups, and alkanol groups also have the chemical formula 6
Refers to the group described above. Incidentally, m is an integer of from 1 to 10, n represents 1 to 10 integer, z is an integer of 0.

[Procedure Amendment 11]

[Document name to be amended] Statement

[Correction target item name] 0041

[Correction method] Change

[Correction content]

The sulfonium phosphate ion, sulfonate ion, phosphonic acid ion, phosphonate ion,
The residue of an inorganic acid or an organic acid containing a nitrate ion or a carboxylate ion means, for example, the residue of the following acid.

[Procedure Amendment 12]

[Document name to be amended] Statement

[Correction target item name] 0042

[Correction method] Change

[Correction content]

Inorganic acids such as sulfuric acid, sulfurous acid, hyposulfuric acid, orthophosphoric acid, pyrophosphoric acid, tripolyphosphoric acid, polyphosphoric acid, nitric acid, nitrous acid and carbonic acid, and formic acid, acetic acid, propionic acid, butyric acid, valeric acid, Capric acid, caproic acid, octylic acid, nonanoic acid, decanoic acid, undecanoic acid, lauric acid, palmitic acid, stearic acid, oleic acid, linoleic acid, aliphatic monocarboxylic acids such as linolenic acid, and adipic acid, sebacic acid, Aliphatic dicarboxylic acids such as azelaic acid, lactic acid, glycolic acid, DL-malic acid, L (+)-tartaric acid, maleic acid, succinic acid, itaconic acid, citric acid, gluconic acid, ricinoleic acid, etc. An aliphatic monocarboxylic acid or an aliphatic polycarboxylic acid containing a bond or the like.

[Procedure Amendment 13]

[Document name to be amended] Statement

[Correction target item name] 0043

[Correction method] Change

[Correction content]

Furthermore, 1-hydroxyethylidene-1 ,
1-diphosphonic acid, amino tris (ethylene phosphonic acid ) , paratoluene sulfonic acid, benzoic acid,
Sulfonate ions such as salicylic acid, phosphonate ions, residues of organic acids containing aromatic rings, etc. are also included.

[Procedure Amendment 14]

[Document name to be amended] Statement

[Correction target item name] 0047

[Correction method] Change

[Correction content]

Examples of monohydric or polyhydric alcohols include monohydric alcohols such as methanol, ethanol, propanol, butanol, amyl alcohol, hexyl alcohol, heptyl alcohol and octyl alcohol.
Monoalkylene glycols such as ethylene glycol, propylene glycol, butylene glycol, and octylene glycol. Polyethylene glycol such as diethylene glycol, triethylene glycol, tetraethylene glycol, polyethylene glycol, dipropylene glycol, tripropylene glycol, tetrapropylene glycol, polypropylene glycol, dibutylene glycol, tributylene glycol, tetrabutylene glycol, polybutylene glycol, etc. is there.

[Procedure Amendment 15]

[Document name to be amended] Statement

[Correction target item name] 0050

[Correction method] Change

[Correction content]

Further, diethylene glycol monomethyl ether, diethylene glycol monoethyl ether, diethylene glycol monopropyl ether, diethylene glycol monobutyl ether, dipropylene glycol monomethyl ether, dipropylene glycol monoethyl ether, dipropylene glycol monopropyl ether, dipropylene glycol monobutyl ether, etc. It is a polyalkylene glycol alkyl ether.

[Procedure Amendment 16]

[Document name to be amended] Statement

[Name of item to be corrected] 0057

[Correction method] Change

[Correction content]

[0057]

EXAMPLES The present invention will be described in more detail with reference to the following examples. The parts and% described in the examples are parts by weight and% by weight. The methods for measuring viscosity, transparency and gel hardness are as follows.

[Procedure Amendment 17]

[Document name to be amended] Statement

[Correction target item name] 0060

[Correction method] Change

[Correction content]

[Method for Measuring Gel Hardness] A measurement sample is heated to a temperature not lower than the phase change temperature to make it liquid, and then put into a colorimetric tube having an inner diameter of 20 mm. While gradually cooling the colorimetric tube at a rate of 2 ° C / minute, the colorimetric tube is allowed to stand for 30 minutes or more at a temperature 3 ° C lower than the center of the phase change temperature.

[Procedure 18]

[Document name to be amended] Statement

[Correction target item name] 0061

[Correction method] Change

[Correction content]

A diameter of 6.4 mm and a load of 1.0 g on the surface of the measurement sample
The steel ball of No. 1 was placed on it, and the time it took to fall at a distance of 10 cm was measured. When the drop time measured by this method was 1 minute or more, it was indicated as a hard gel.

[Procedure Amendment 19]

[Document name to be amended] Statement

[Correction target item name] 0063

[Correction method] Change

[Correction content]

The third product obtained by the above reaction and having a solid content of 60%
An aqueous solution of an organic acid salt of a primary amine is a homogeneous and transparent low-viscosity liquid at a temperature of 38 ° C or higher, and changes to a colorless and transparent elastic gel at a temperature of 36 ° C or lower. When gelled at 36 ° C or lower, if it is heated again to a temperature of 38 ° C or higher, it returns to a low viscosity liquid. This change from a low viscosity liquid to an elastic gel occurs rapidly, completely and reversibly with a temperature change of about 2 ° C from 38 ° C to 36 ° C.

[Procedure amendment 20]

[Document name to be amended] Statement

[Correction target item name] 0064

[Correction method] Change

[Correction content]

The above reaction product has a viscosity of 110 centipoise at 40 ° C. which is 3 ° C. higher than the center of the phase change temperature, and the gel at 34 ° C. which is 3 ° C. lower than the center of the phase change temperature has a falling time of 5
It was more than a minute and hard . The transparency was 99.5%.

[Procedure correction 21]

[Document name to be amended] Statement

[Name of item to be corrected] 0070

[Correction method] Change

[Correction content]

The above reaction product has a viscosity of 90 centipoise at 41 ° C., which is 3 ° C. higher than the center of the phase change temperature, and the gel at 35 ° C. which is 3 ° C. lower than the center of the phase change temperature has a falling time of 10 minutes or more. It was hard enough. The transparency was 99.5%.

[Procedure correction 22]

[Document name to be amended] Statement

[Name of item to be corrected] 0072

[Correction method] Change

[Correction content]

The above goldfish (wakin) storage sample enclosed in the glass wide-mouthed sample bottle remained a colorless and transparent elastic gel even after storage for one year at room temperature. After one year of storage, the goldfish (wakin) storage sample enclosed in a glass wide-mouthed sample bottle was heated to 40 ° C in a warm water bath to return it to a uniform transparent low-viscosity liquid, and then No. 4 in the bottle
An aqueous solution of a high-grade ammonium salt was poured out, washed briefly with water, and then a goldfish (wakin) was taken out.

[Procedure amendment 23]

[Document name to be amended] Statement

[Correction target item name] 0075

[Correction method] Change

[Correction content]

A third 40% solids product obtained from the above reaction.
An aqueous solution of an organic acid salt of a primary amine is a homogeneous and transparent low-viscosity liquid at a temperature of 38 ° C or higher, and changes to a colorless and transparent elastic gel at a temperature of 36 ° C or lower. When gelled at 36 ° C or lower, it is returned to a low-viscosity liquid when heated again to a temperature of 38 ° C or higher.

[Procedure correction 24]

[Document name to be amended] Statement

[Correction target item name] 0077

[Correction method] Change

[Correction content]

The above reaction product has a viscosity of 98 centipoise at 40 ° C. which is 3 ° C. higher than the center of the phase change temperature, and the gel at 34 ° C. which is 3 ° C. lower than the center of the phase change temperature has a falling time of 5 minutes or more. Met. This product was colored slightly pale yellow, but the transparency was 93.5%.

[Procedure correction 25]

[Document name to be amended] Statement

[Correction target item name] 0079

[Correction method] Change

[Correction content]

The aqueous solution of an organic acid salt of a tertiary amine having a solid content of 47.5% obtained by the above reaction is a uniform and transparent low-viscosity liquid at a temperature of 41 ° C. or higher, and a colorless and transparent liquid at 39 ° C. or lower. Turns into an elastic gel . When gelled at 39 ° C or lower, if it is heated again to a temperature of 41 ° C or higher, it returns to a low-viscosity liquid. This change from a low viscosity liquid to an elastic gel occurs rapidly, completely and reversibly with a temperature change of about 2 ° C from 41 ° C to 39 ° C. The viscosity of the above reaction product at the temperature of 43 ° C., which is 3 ° C. higher than the center of the phase change temperature, is 130 centipoise, and at 37 ° C., which is 3 ° C. lower than the center of the phase change temperature, the dropping time is 10 minutes or more. It was hard . The transparency was 93.5%.

[Procedure Amendment 26]

[Document name to be amended] Statement

[Correction target item name] 0081

[Correction method] Change

[Correction content]

The aqueous solution of amine oxide having a solid content of 55% obtained by the above reaction is a uniform transparent low-viscosity liquid at a temperature of 45 ° C. or higher, and a pale yellow transparent elastic gel at a temperature of 43 ° C. or lower. Changes to. When a substance that has gelled at 43 ° C or lower is heated again to a temperature of 45 ° C or higher, it returns to a low-viscosity liquid.

[Procedure Amendment 27]

[Document name to be amended] Statement

[Name of item to be corrected] 0083

[Correction method] Change

[Correction content]

The viscosity of the above reaction product at 47 ° C., which is 3 ° C. higher than the center of the phase change temperature, is 98 centipoise, and the gel drop time at 41 ° C., which is 3 ° C. lower than the center of the phase change temperature, is 3 minutes or less. It was solid . The transparency was 92%.

[Procedure correction 28]

[Document name to be amended] Statement

[Correction target item name] 0084

[Correction method] Change

[Correction content]

Using this reaction product, the same procedure as in Example 1 was carried out.
cha (Mont.) Sacc.] was used to create archival specimens.
The archival sample was a pale yellow, transparent, elastic gel .

[Procedure correction 29]

[Document name to be amended] Statement

[Correction target item name] 0085

[Correction method] Change

[Correction content]

After storing for one year, the regenerated specimen in the original state could be taken out in the same manner as in Example 2 .

[Procedure amendment 30]

[Document name to be amended] Statement

[Correction target item name] 0091

[Correction method] Change

[Correction content]

The above reaction product has a viscosity of 120 centipoise at 56 ° C., which is 3 ° C. higher than the center of the phase change temperature, and a gel at 50 ° C. which is 3 ° C. lower than the center of the phase change temperature has a falling time of 10 times.
It was more than a minute and hard enough. The transparency was 93%.

[Procedure correction 31]

[Document name to be amended] Statement

[Correction target item name] 0097

[Correction method] Change

[Correction content]

The above reaction product has a viscosity of 75 centipoise at 44 ° C., which is 3 ° C. higher than the center of the phase change temperature, and the gel at 38 ° C. which is 3 ° C. lower than the center of the phase change temperature has a dropping time of 5 minutes or more. It was hard. The transparency was 90.5%.

[Procedure correction 32]

[Document name to be amended] Statement

[Correction target item name] 0098

[Correction method] Change

[Correction content]

(Example 8) In the same manner as in Example 1 , the solid content of the L (+)-tartaric acid (natural type) salt of dimethyllaurylamine was from 65% to 57.5%, and 4 points in 2.5% increments. Created. In the same manner as in Example 3, five points of dimethyllaurylamine glycolate having a solid content of 47.5 % to 37.5% were prepared in 2.5% increments.

[Procedure amendment 33]

[Document name to be amended] Statement

[Correction target item name] 0101

[Correction method] Change

[Correction content]

[0101]

[Table 1]

[Procedure amendment 34]

[Document name to be amended] Statement

[Correction target item name] 0103

[Correction method] Change

[Correction content]

(Example 9) In the same manner as in Example 3 and Example 8, part of the warm water of the dimethyllaurylamine glycolate was replaced with glycerin, propylene glycol, ethylene glycol monomethyl ether or the like. hand,
A composition to which a phase change temperature adjusting agent was added was prepared.

[Procedure amendment 35]

[Document name to be amended] Statement

[Correction target item name] 0107

[Correction method] Change

[Correction content]

(Example 10) In the same manner as in Examples 2 and 8 and 9, the warm water of the quaternary ammonium salt of trimethyl laurylamine trimethyl phosphate was used, and a part thereof was added. A composition was prepared by substituting ethylene glycol, propylene glycol, dipropylene glycol, dipropylene glycol monomethyl ether, glycerin, diglycerin, ethylene glycol monomethyl ether, solfit and solfit acetate, which are temperature-changing agents.

[Procedure correction 36]

[Document name to be amended] Statement

[Correction target item name] 0110

[Correction method] Change

[Correction content]

[0110] The solution of these characteristics and properties of the gel phase during the phase change from liquid to gel products, various compounds of the present invention
Concentration and phase change The type and amount of temperature regulator can be changed.
The temperature can be adjusted within the range of 20-70 ℃ by and.

Claims (6)

[Claims] 1. A composition comprising an amine compound represented by Chemical Formula 1 and water, which undergoes a reversible phase change between a transparent liquid and a gel state upon temperature change, and a temperature change within 3 ° C. from the phase change temperature. An encapsulant characterized in that the viscosity changes from 200 centipoise or less to a solid gel within 3 minutes. [Chemical 1] R ₁ , R ₂ and R ₃ are hydrogen or a hydrocarbon group, R ₄ is a hydrogen or hydrocarbon group or O ⁻ , and the hydrocarbon group has 1 to 2 carbon atoms.
8, the total carbon number of R _{1 to} R ₄ is _{4 to} 50. X ⁻ is an inorganic or organic acid residue, n is 0 when R ₄ is O ⁻ , and 1 otherwise. 2. A composition comprising an amine compound represented by Chemical Formula 1, water and a phase change temperature controlling agent, wherein the content of the amine compound is 15 to 80%, and the content of the phase change temperature controlling agent is phase with water. 0 to 80% of the total of the temperature change agent,
In the temperature range of 〜70 ℃, the phase changes reversibly between the transparent liquid and gel state by the temperature change, and the temperature changes within 3 ℃ from the phase change temperature, the viscosity changes from 200 centipoise or less to the solid gel within 3 minutes. An encapsulant characterized by changing. 3. The encapsulating agent according to claim 1, wherein the amine compound represented by the chemical formula 1 is a compound represented by the chemical formula 2. [Chemical 2] R ₁ , R ₂ , R ₃ , and R ₄ are hydrogen or an alkyl group or alkylene group having 1 to 28 carbon atoms, an alkanol group, and a hetero atom, an unsaturated group, an amide bond, an aromatic group in the chain and / or the side chain. It may contain one or more rings, and the total carbon number of R _{1 to} R ₄ is _{4 to} 50.
Is. X ^- is a residue of an inorganic or organic acid. 4. The encapsulant according to claim 1, wherein the amine compound represented by the chemical formula 1 is a compound represented by the chemical formula 3. [Chemical 3] R ₁ , R ₂ and R ₃ are the same as in Chemical Formula 2. Y ⁻ −R ₄ is a residue of an inorganic or organic acid containing a sulfonate ion, a sulfonate ion, a phosphonate ion, a phosphonate ion, a nitrate ion, and a carboxylate ion. 5. The encapsulant according to claim 1, wherein the amine compound represented by the chemical formula 1 is a compound represented by the chemical formula 4. [Chemical 4] R ₁ , R ₂ and R ₃ are the same as in Chemical Formula 2. 6. The encapsulant according to claim 2, wherein the phase change temperature controlling agent is a monohydric or polyhydric alcohol, an alkyl ether of a dihydric alcohol, or an organic acid ester of a dihydric alcohol alkyl ether.