Multipurpose adhesive composition comprising polymer coacervate formed by polyphenol action

Abstract

The present invention relates to a multipurpose adhesive composition comprising a polymer coacervate formed by polyphenol action, the composition having excellent adhesion to cuticles and skin, being easily removable with water without irritation, and being easy for users to handle. The present invention provides the multipurpose adhesive composition comprising: a polyvinyl alcohol compound; a water-soluble polyphenol compound; and a solvent.

Description

A multipurpose adhesive composition comprising a polymer coacervate formed by polyphenol action.

[0001] The present invention relates to a multipurpose adhesive composition comprising a polymer coacervate formed by a polyphenol action, and more particularly, to a multipurpose adhesive composition comprising a polymer coacervate formed by a polyphenol action, which has excellent adhesiveness to cuticles and skin, can be easily removed with water without irritation, and is also easy for a user to handle.

[0002] With the recent rise of artificial eyelashes in the beauty industry, demand for cosmetic adhesives for attaching them has skyrocketed. These adhesives are widely used due to their ability to effectively bond false eyelashes of various lengths and shapes. Depending on the application and method, they can be used not only on eyelashes but also on skin, such as the eyelids. They are also widely used to attach additional cosmetic adornments, such as glitter powder or rhinestones, to the skin during special occasions or events like music festivals.

[0003] However, typical commercially available eyelash adhesives contain various chemicals, such as acrylates, formaldehyde, and latex, which can cause allergic reactions or irritation when used around the eyes and other sensitive skin areas. Therefore, allergic reactions and skin irritation caused by these adhesive chemicals are important safety considerations for multi-purpose cosmetic adhesives. One way to minimize these side effects is to reduce the content of harmful chemicals in the adhesive, and in particular, to exclude hazardous ingredients such as acrylates, formaldehyde, and latex from some adhesive formulations.

[0004] Furthermore, the physical irritation that occurs during the adhesive removal process can cause various side effects, including eyelash damage and removal, redness, and mild pain. Additional physical irritation to skin already irritated by chemical compounds can further exacerbate the inflammatory response. Therefore, minimizing the physical irritation associated with adhesive removal is also an important consideration.

[0005] Accordingly, the present invention provides a hypoallergenic composition derived from polyphenol coacervate that does not use irritating compositions such as acrylate, formaldehyde, and latex, and provides an adhesive composition that has excellent adhesiveness to cuticles and skin and is easily removed with water without irritation.

[0006] In order to solve the above-mentioned problems, the present invention seeks to provide a multipurpose adhesive composition comprising a polymer coacervate formed by a polyphenol action, which has excellent adhesiveness to cuticles and skin, can be easily removed with water without irritation, and is also easy for a user to handle.

[0007] To solve the above-described problem, the present invention provides a multipurpose adhesive composition comprising a polyvinyl alcohol compound; a water-soluble polyphenol compound; and a solvent.

[0008] In one embodiment, the polyvinyl alcohol compound and the water-soluble polyphenol compound may form a coacervate.

[0009] In one embodiment, the polyvinyl alcohol compound and the water-soluble polyphenol compound may form a coacervate through hydrogen bonding.

[0010] In one embodiment, the polyvinyl alcohol compound may be a random copolymer.

[0011] In one embodiment, the polyvinyl alcohol compound may have a structure represented by the following chemical formula 1.

[0012] [Chemical Formula 1]

[0013]

[0014] (In the above chemical formula 1, m and n are natural numbers, and n:m is 99.9:0.1~90:10)

[0015] In one embodiment, the polyvinyl alcohol compound may have a molecular weight of 13,000 to 23,000 Da.

[0016] In one embodiment, the polyvinyl alcohol compound comprises a hydroxyl group (OH), an amine group (NH2), a succinimidyl succinate, a succinic acid, a thiol group (SH), an acrylate, an epoxide group, a maleimide, a nitrophenyl carbonate, an orthopyridyl disulfide, a tosylate group, an azide, a phosphate group, an oligoamine group ([-CH2-CH2-NH-]n), a catechol, a catecholamine, an isothiocyanate, a vinylsulfone, an aldehyde, a glyoxal, a hydrazine, an acrylamide, It may contain at least one functional group selected from the group consisting of methacrylate, styrene, vinylpyridine, vinyl acetate, ethylene, propylene, and vinyl chloride.

[0017] In one embodiment, the water-soluble polyphenol compound is a Hydroxybenzoic acid compound, a Hydroxycinnamic acid compound, a Flavonoid compound, a Stilbenes compound, Caffeic acid, Chlorogenic acid, Anthocyanin, Pyrogallol, Ellagic acid, Gallic acid, Catechin, Hydrolyzable Tannin, Condensed Tannin, Theaflavin-3-gallate, Quercetin, Luteolin, Hesperidin, Resveratrol, Fisetin, Naringin, Pycnogenol, Curcumin, It may include at least one selected from the group consisting of gingerol, aloe-emodin, saponin, terpenes, lignans, lignin, curcuminoids, alkaloids, glucosinolates, and phytosterols.

[0018] In one embodiment, the water-soluble polyphenol compound may include at least one selected from the group consisting of tannic acid, gallotannins, ellagitannins, pentagalloyl glucose, casuarictin, grandin, tellimagrandin, chebulinic acid, terchebin, proanthocyanidin, prodelpinidin, catechins, epicatechins, fisetindiol, and robinetinidol.

[0019] In one embodiment, the multipurpose adhesive composition may include 0.1 to 20 parts by weight of the polyvinyl alcohol compound and 0.01 to 4 parts by weight of the water-soluble polyphenol compound.

[0020] In one embodiment, the polyvinyl alcohol compound and the water-soluble polyphenol compound may be mixed in a weight ratio of 1:1 to 10:1.

[0021] In one embodiment, the multipurpose adhesive composition may be used for bonding body hair or artificial body hair.

[0022] The present invention also provides a method for producing a multipurpose adhesive composition, comprising the steps of: dissolving a polyvinyl alcohol compound and a water-soluble polyphenol compound in a solvent to produce a coacervate solution; and separating the coacervate solution according to specific gravity and obtaining a supernatant.

[0023] In one embodiment, the step of preparing the coacervate solution may include the steps of: preparing a polyvinyl alcohol solution by dissolving a polyvinyl alcohol compound in a solvent; preparing a polyphenol aqueous solution by dissolving a water-soluble polyphenol compound in a solvent; and preparing a coacervate aqueous solution by mixing the polyvinyl alcohol aqueous solution and the polyphenol aqueous solution.

[0024] In one embodiment, the step of preparing the coacervate aqueous solution may include a step of mixing the polyvinyl alcohol aqueous solution and the polyphenol aqueous solution at a weight ratio of 1:1 to 10:1.

[0025] In the low-viscosity adhesive composition according to the present invention, the hydroxyl group of polyvinyl alcohol physically bonds with the galol group of tannic acid through hydrogen bonding.

[0026] In particular, by using polyvinyl alcohol, there is an advantage in that it is possible to implement a non-toxic and non-irritating adhesive by preventing the slight toxicity problem that may occur when using tannic acid alone.

[0027] Additionally, tannic acid rich in gallic acid can effectively attach eyelashes and various cosmetic accessories through physical bonding with keratin fibers, specifically hair proteins, and skin through hydrophobic interactions.

[0028] In addition, the low-viscosity adhesive composition according to the present invention has the advantage of being able to bond without damaging the skin, preventing allergic reactions, and significantly shortening the drying time of the adhesive to within 10 minutes, since it substantially does not contain irritating compositions such as acrylate, formaldehyde, and latex.

[0029] In particular, the low-viscosity adhesive composition according to the present invention has the advantage of being able to be easily removed using water without irritation because it contains abundant hydroxyl groups, and artificial eyelashes or cosmetic decorations with adhesive on them can be rinsed with water and reused.

[0030] Figure 1 shows a PVA / TA solution according to one embodiment of the present invention. (a) is a photograph showing two states of a supernatant (l-VATA) and a subjacent solution (VATA). (b) shows a schematic structure of a PVA / TA complex (coacervate) on the supernatant (l-VATA).

[0031] FIG. 2 is a graph showing (a) a GPC chromatogram in combination with an RI detector (left; TA (pink, top), PVA (gray, middle), l-VATA (black, bottom)) and a UV detector (right; TA (top), PVA (middle), l-VATA (bottom)) according to one embodiment of the present invention, (b) a graph showing the results of an S1 experiment, and (c) a graph showing the results of an S2 experiment.

[0032] FIG. 3 illustrates the composition ratio of PVA (Initial), supernatant (l-VATA), and lower layer (VATA) for the initial PVA and TA solutions before mixing according to one embodiment of the present invention.

[0033] Figure 4 is a photograph showing an adhesive composition according to the pH value of a PVA solution according to one embodiment of the present invention. The pink arrow indicates the lower layer (VATA) attached to the wall while resisting centrifugal force.

[0034] Figure 5 shows (a) a graph of the S1 results according to one embodiment of the present invention, (b) the hydrodynamic diameter of PVA (left) and the supernatant (l-VATA) corrected from the GPC results, and (c) a schematic representation of TA decorated along the PVA chains, respectively. (n = 4, *p < 0.05)

[0035] Figure 6 shows (a) DLS results (n = 5) showing that the hydrodynamic diameter of l-VATA increases when a shear force is applied according to one embodiment of the present invention, (b) AFM images of l-VATA before (V0) and after (V5) the application of a shear force, and (c) the determination of particle volume obtained from the AFM results in (b) (n = 4, *p < 0.05).

[0036] Figure 7 shows the adhesive strength (n = 6, *p < 0.05) of the supernatant (l-VATA) before and after application of shear force (V0) according to one embodiment of the present invention (V5).

[0037] Figure 8 shows the experimental results on the viscosity and rheological behavior of the supernatant (l-VATA) according to one embodiment of the present invention, (a) viscosity measurement results of 14 wt% PVA (gray) and supernatant (l-VATA) solution (black) according to shear rate, (b) changes in storage modulus (G') and loss modulus (G'') of PVA (G' = filled gray, G'' = empty gray) and supernatant (l-VATA, G' = filled black, G'' = empty black). (c) A schematic explanation of the shear-dependent response shown in (b) is shown, respectively.

[0038] FIG. 9 shows the experimental results on the cytotoxicity of supernatant (l-VATA), PVA, and TA in L929 cells according to one embodiment of the present invention, showing (a) LIVE / DEAD staining (green: live cells, red: dead cells) and (b) quantitative cell viability (%) (n = 3) based on cell counting kit-8 (CCK-8) analysis using undiluted supernatant (l-VATA, black), PVA (gray), TA (pink), and phosphate buffered saline (PBS) (light gray).

[0039] FIG. 10 is a photograph showing the high viscosity and difficult-to-handle characteristics of a high-density sub-layer (VATA) according to one embodiment of the present invention, in which a bent cable tie (left, red box) can be straightened after being immersed and reshaped (right).

[0040] FIG. 11 is a schematic illustration of a method for hair-to-hair bonding using a needle template using (a) a supernatant (l-VATA) according to one embodiment of the present invention, and (b) a photograph demonstrating weight lifting using a fiber composed of 10 hair strands.

[0041] FIG. 12 shows (a) a photograph of human hair to pig skin adhesion and adhesion confirmation using tweezers movement according to one embodiment of the present invention, and (b) an evaluation result of adhesion strength in the presence of water.

[0042] Hereinafter, preferred embodiments of the present invention will be described in detail. In describing the present invention, if a detailed description of related known technology is judged to obscure the gist of the present invention, the detailed description thereof will be omitted. Throughout the specification, singular expressions should be understood to include plural expressions unless the context clearly indicates otherwise, and terms such as “comprise” or “have” should be understood to indicate the presence of described features, numbers, steps, operations, components, parts, or combinations thereof, but not to exclude in advance the possibility of the presence or addition of one or more other features, numbers, steps, operations, components, parts, or combinations thereof. In addition, in performing a method or a manufacturing method, each step constituting the method may occur in a different order from the stated order, unless the context clearly indicates a specific order. That is, each step may occur in the same order as the stated order, may be performed substantially simultaneously, or may be performed in the reverse order.

[0043] The technology disclosed in this specification is not limited to the implementation examples described herein and may be embodied in other forms. However, the implementation examples introduced herein are provided to ensure that the disclosed content is thorough and complete and to ensure that the technical spirit of the present technology can be sufficiently conveyed to those skilled in the art. In the drawings, the dimensions of each device component, such as width and thickness, are somewhat enlarged to clearly represent the components. Overall, the drawings are described from the observer's perspective, and when an element is mentioned as being positioned above another element, this includes the meaning that the element is positioned directly above the other element or that additional elements may be interposed between the elements. Furthermore, those skilled in the art will be able to implement the spirit of the present invention in various other forms without departing from the technical spirit of the present invention. In addition, the same reference numerals in multiple drawings indicate substantially the same elements.

[0044] As used herein, the term "and / or" includes a combination of multiple listed items or any one of multiple listed items. As used herein, "A or B" may include "A," "B," or "both A and B."

[0045] The present invention relates to a multipurpose adhesive composition comprising a polyvinyl alcohol compound; a water-soluble polyphenol compound; and a solvent.

[0046] The above polyvinyl alcohol compound and the water-soluble polyphenol compound may form a coacervate.

[0047] The above coacervate is a process in which a homogeneous aqueous solution of a polymer undergoes liquid-liquid phase separation, forming a dense phase rich in polymers at the bottom and a dilute phase of polymers remaining at the top. At this time, the dense phase is called a coacervate, and the molecules inside the coacervate show relatively slow exchange with molecules in the external environment. Due to the polymer-rich phase, the coacervate is inherently very viscous, and if it contains an adhesive substance such as polyphenol, it exhibits adhesive properties. Such adhesive coacervates can be used as medical welding adhesives that can replace surgical sutures or hemostatic agents. The coacervate refers to a colloid formed by nucleic acids, sugars, proteins, or polymers and dispersed in a solvent. Since its first recognition in 1929, the various physicochemical properties of coacervates generated from liquid-to-liquid phase separation have received much attention. In a biological context, it functions as a membraneless compartment within the cell and can provide a spatiotemporal platform for various biochemical reactions.

[0048] On the other hand, synthetic polyelectrolyte coacervates have been reported to have diverse applications beyond the realm of biology. Their unique physicochemical properties have been utilized to synthesize nanomaterials, improve drug delivery systems, enhance cosmetic formulations, and enhance food processing.

[0049] Almost all coacervate research focuses on the subsurface. Therefore, our study focused on the functional significance of the coacervate supernatant, highlighting its unique functions and diverse applications. This supernatant, characterized by low polymer concentration and viscosity, retains the inherent properties of a dense coacervate subsurface. In particular, the low viscosity of the supernatant offers unique advantages over the adhesive of the dense subsurface, enabling easy application and the formation of a thin, uniform layer on biological surfaces (see Figure 1).

[0050] The above polyvinyl alcohol compound and the water-soluble polyphenol compound may form a coacervate through hydrogen bonding.

[0051] In general, coacervates are dynamic systems governed primarily by chemical equilibrium. The formation of complex coacervates from synthetic polymers relies heavily on interactions between cationic and anionic polymers, namely electrostatic interactions. Examples include the formation of coacervates between poly(allylamine hydrochloride) (PAH) / poly(acrylic acid) (PAA), polyethyleneimine (PEI) / PAA, and poly(diallyldimethylammonium chloride) (PDADMAC) / poly(styrenesulfonate) (PSS).

[0052] Recently, neutral polyphenol coacervates have been used. Polyphenol coacervates are formed through hydrogen bonding, and these polyphenol coacervates exhibit adhesive properties similar to the molecular mechanism of mussel adhesion. Therefore, the present invention can utilize coacervates formed through hydrogen bonding.

[0053] The above polyvinyl alcohol compound may be a random copolymer.

[0054] The above random copolymer refers to a polymer formed by two or more monomers having a random arrangement. If the probability of finding a residue of a specific monomer at a specific point of a polymer is equal to the molar fraction of the specific monomer, it can be called a random copolymer. Such a random copolymer can generally be formed when an olefin-type monomer copolymerizes through a process in which it has a free radical form, and the properties of such a random copolymer may be different from those of the polymers of each monomer.

[0055] In the present invention, the polyvinyl alcohol compound may have a structure represented by the following chemical formula 1.

[0056] [Chemical Formula 1]

[0057]

[0058] (In the above chemical formula 1, m and n are natural numbers, and n:m is 99.9:0.1 to 90:10, preferably 98:2)

[0059] As described above, the polyvinyl alcohol may be a random copolymer. In particular, the polyvinyl alcohol of the present invention may be a random copolymer of a vinyl alcohol monomer and a vinyl acetate monomer, as represented by the above chemical formula 1.

[0060] A closer look reveals that vinyl alcohol (CH2CHOH) typically reversibly transforms into aldehyde and alcohol in the air. Therefore, when vinyl alcohol is directly polymerized, only a copolymer of vinyl alcohol and vinylaldehyde is obtained.

[0061] Therefore, to solve this problem, vinyl acetate (CH3COOCHCH2) can be polymerized, and then produced by hydrolyzing it or adding alcohol. At this time, the acetic acid portion of the polyvinyl acetate can be removed through the hydrolysis or alcohol addition process, and this removal process is performed randomly. Therefore, after the polyvinyl acetate is converted to the polyvinyl alcohol, a random copolymer can be formed.

[0062] In particular, in this process, it is possible to control the ratio of n:m by controlling the amount of hydrolysis or alcohol addition, and in the case of the present invention, n:m can have a ratio of 99.9:0.1 to 90:10, preferably 98:2. Within the above range, the adhesive composition according to the present invention can be formed normally, but when it is less than 90:10, the adhesiveness may be reduced, and when the ratio exceeds 99.9:0.1, it may be difficult to manufacture in terms of chemical equilibrium.

[0063] The polyvinyl alcohol compound manufactured as described above exhibits water solubility, thereby facilitating the formation of a coacervate, as described below. Furthermore, the polyvinyl alcohol contains a large number of hydroxyl groups (OH groups) capable of hydrogen bonding, facilitating the formation of a water-soluble polyphenol, as described below.

[0064] The polyvinyl alcohol compound may have a molecular weight of 13,000 to 23,000 Da. The polyvinyl alcohol preferably forms a coacervate, as described below. In this case, if the molecular weight is less than 13,000 Da, formation of a coacervate may be difficult due to the small molecular weight, and if it exceeds 23,000 Da, the amount of coacervate included in the supernatant may decrease, resulting in poor adhesiveness.

[0065] The above polyvinyl alcohol compound comprises a hydroxyl group (OH), an amine group (NH2), a succinimidyl succinate, a succinic acid, a thiol group (SH), an acrylate, an epoxide group, a maleimide, a nitrophenyl carbonate, an orthopyridyl disulfide, a tosylate group, an azide, a phosphate group, an oligoamine group ([-CH2-CH2-NH-]n), a catechol, a catecholamine, an isothiocyanate, a vinylsulfone, an aldehyde, a glyoxal, a hydrazine, an acrylamide, It may contain at least one functional group selected from the group consisting of methacrylate, styrene, vinylpyridine, vinyl acetate, ethylene, propylene, and vinyl chloride.

[0066] As described above, it is preferable to have a hydroxyl group to form a hydrogen bond with water-soluble polyphenols. However, in addition to the hydroxyl group, various functional groups may be present, through which the hydrogen bond can be formed and various physical properties can be added to the adhesive. For example, by adding a different type of functional group instead of the hydroxyl group, the adhesive's adhesive strength can be controlled, and its solubility in water can be controlled or it can be made hydrophilic or hydrophobic after bonding (see Figure 1).

[0067] The water-soluble polyphenol compound contains a large amount of gallic acid groups, which enable it to have a material binding effect through hydrophobic interaction with proteins such as keratin in body hair and skin. However, since such water-soluble polyphenol compound has a low toxicity, in the present invention, by combining it with polyvinyl alcohol, it can prevent absorption into the skin and exhibit only an adhesive effect on the skin surface (see Fig. 12).

[0068] The water-soluble polyphenols that can be used at this time can be used without limitation as long as they can have the above effects, but hydroxybenzoic acid compounds, hydroxycinnamic acid compounds, flavonoid compounds, stilbene compounds, caffeic acid, chlorogenic acid, anthocyanin, pyrogallol, ellagic acid, gallic acid, catechin, hydrolyzable tannin, condensed tannin, theaflavin-3-gallate, quercetin, luteolin, hesperidin, resveratrol, It may include at least one selected from the group consisting of Fisetin, Naringin, Pycnogenol, Curcumin, Gingerol, Aloe-emodin, Saponin, Terpenes, Lignans, Lignin, Curcuminoids, Alkaloids, Glucosinolates and Phytosterols.

[0069] Among the water-soluble polyphenols, hydrolyzed tannins or condensed tannins may be preferably used. As an example of the hydrolyzed tannins, the water-soluble polyphenol compounds may include at least one selected from the group consisting of tannic acid, gallotannins, ellagitannins, pentagalloyl glucose, casuarictin, grandin, tellimagrandin, chebulinic acid, and terchebin. As an example of the condensed tannins, the water-soluble polyphenol compounds may include at least one selected from the group consisting of proanthocyanidin, prodelpinidin, catechins, epicatechins, fisetindiol, and It may include at least one selected from the group consisting of Robinetinidol.

[0070] The above multipurpose adhesive composition may contain 0.1 to 20 parts by weight of the polyvinyl alcohol compound and 0.01 to 4 parts by weight of the water-soluble polyphenol compound.

[0071] If the polyvinyl alcohol compound is less than 0.1 parts by weight, coacervate formation may be difficult, and if it exceeds 20 parts by weight, the yield of the supernatant may decrease in the manufacturing step described later. In addition, if the water-soluble polyphenol compound is included in an amount of less than 0.01 parts by weight, the adhesiveness of the adhesive manufactured by the present invention may decrease, and if it exceeds 20 parts by weight, unreacted water-soluble polyphenol compound may be present, which may irritate the skin.

[0072] In addition, it is preferable that the multipurpose adhesive composition contains less than 99.8 wt% of water. If the water content exceeds 99.8 wt%, the adhesive strength may be reduced.

[0073] The above polyvinyl alcohol compound and the water-soluble polyphenol compound may be mixed in a weight ratio of 1:1 to 10:1, preferably 5:1.

[0074] If the above weight ratio is less than 10:1, the content of water-soluble polyphenol may decrease, which may result in poor adhesive strength, and if it exceeds 1:1, unreacted water-soluble polyphenol may cause skin irritation.

[0075] The above multipurpose adhesive composition may be used for bonding body hair or artificial body hair. As described above, in the case of water-soluble polyphenol, it can perform hydrophobic interaction with keratin and skin of body hair or artificial body hair. Through this, the water-soluble polyphenol can adhere to the body hair and skin, respectively. In particular, in the case of the present invention, since the water-soluble polyphenol is combined with the polyvinyl alcohol to form a coacervate, absorption into the skin is hardly performed, and thus skin irritation caused by the water-soluble polyphenol can be minimized. The body hair used in this case may include hair, eyebrows, eyelashes, a beard, and pubic hair, and the artificial body hair may be used without limitation as long as it is artificial body hair that can adhere to the water-soluble polyphenol, as well as artificial body hair containing keratin.

[0076] Hereinafter, the present invention will be described in detail according to a method for manufacturing a multipurpose adhesive composition.

[0077] The present invention also relates to a method for producing a multipurpose adhesive composition, comprising the steps of: dissolving a polyvinyl alcohol compound and a water-soluble polyphenol compound in a solvent to produce a coacervate solution; and separating the coacervate solution according to specific gravity and obtaining a supernatant.

[0078] Descriptions of polyvinyl alcohol compounds, water-soluble polyphenol compounds, and coacervates are omitted as they are as described above.

[0079] The step of preparing the above coacervate solution may include a step of preparing a polyvinyl alcohol solution by dissolving a polyvinyl alcohol compound in a solvent; a step of preparing a polyphenol aqueous solution by dissolving a water-soluble polyphenol compound in a solvent; and a step of preparing a coacervate aqueous solution by mixing the polyvinyl alcohol aqueous solution and the polyphenol aqueous solution.

[0080] As described above, the polyvinyl alcohol is water-soluble and can be easily dissolved in polar solvents, particularly water. However, when the water-soluble polyphenol is added to the polyvinyl alcohol solution mixed with the solvent, the polyvinyl alcohol solution has a high viscosity, making it difficult to mix the water-soluble polyphenol. To prevent this, if an excessive amount of solvent is used, it may be difficult for the polyvinyl alcohol solution to form a coacervate. Therefore, as described above, by dissolving polyvinyl alcohol and water-soluble polyphenol in each solvent and then mixing them, it is possible to form a coacervate having an appropriate concentration.

[0081] In addition, at this time, the mixing ratio of the polyvinyl alcohol aqueous solution and the polyphenol aqueous solution may be 1:1 to 10:1 by weight, preferably 5:1. Within the above range, it is possible to manufacture an appropriate adhesive, but if it is outside the above range, the adhesive strength may decrease or it may irritate the skin.

[0082] The solvent used in the above mixing process may be a polar solvent, but water is preferred. As described above, the present invention can be used to bond body hair or artificial body hair. Therefore, solvents harmful to the human body cannot be used, and water is most preferably used as the solvent.

[0083] As described above, the coacervate aqueous solution prepared by mixing the polyvinyl alcohol aqueous solution and the polyphenol aqueous solution can be separated into a supernatant and a lower layer. This separation process can be performed by centrifugation or allowing to stand for a certain period of time.

[0084] When separating the supernatant and the lower layer through the above centrifugation, it is preferable that the rotation speed of the centrifuge be 1000 to 5000 rpm, preferably 300 rpm. If the speed of the centrifuge is less than 100 rpm, the separation takes a long time, which is uneconomical. If it exceeds 5000 rpm, the coacervate of the supernatant may move to the lower layer, reducing the adhesiveness of the supernatant. In addition, the centrifugation can be performed for 10 to 30 minutes, preferably 20 minutes.

[0085] When separating the supernatant and substratum by static separation, the coacervate solution is poured into a container and stored at room temperature for 12 to 36 hours, preferably 24 hours. If stored for less than 12 hours, the supernatant yield may decrease, and if stored for more than 36 hours, it is no longer effective and is therefore uneconomical.

[0086] In the present invention, the supernatant can be recovered and used. While the lower layer contains a large amount of the coacervate, it has a high viscosity and excessive adhesiveness, making it difficult to apply directly to the human body. Furthermore, the supernatant is typically separated and discarded. However, in the present invention, by using the supernatant, it can have an appropriate viscosity and adhesiveness, allowing it to be applied directly to the human body. Furthermore, by recycling the discarded supernatant, manufacturing costs can be significantly reduced.

[0087] The separation of the above supernatant can be achieved by using the same separation method used in the production of coacervate, or by simply separating manually using a pipette or the like, or by mechanically separating using the difference in viscosity.

[0088] The multipurpose adhesive composition manufactured by the above method can be used by applying the multipurpose adhesive composition to hair or skin and leaving it for 1 to 10 minutes. That is, the multipurpose adhesive composition according to the present invention can attach hair to skin without additional joining or energy supply. In addition, since water, the solvent used in the multipurpose adhesive composition, can be easily removed by evaporating into the air or being absorbed into the skin, sufficient adhesive strength can be exhibited with only a drying time of 1 to 10 minutes.

[0089] In addition, the adhesive composition attached as described above can be easily separated simply by re-supplying water as a solvent. As described above, the adhesive composition of the present invention binds to the keratin of body hair or skin through hydrophobic bonds, and the coacervate having an adhesive effect can be easily dissolved in a solvent. Therefore, after bonding is complete, it is possible to easily remove the adhesive composition simply by re-supplying water. In particular, since a water-soluble adhesive is used, the body hair or artificial body hair as the bonding target can be washed with water and reused after being removed from the skin as described above.

[0090]

[0091] Hereinafter, preferred embodiments of the present invention will be described with reference to the accompanying drawings so that those skilled in the art can easily implement them. Furthermore, when describing the present invention, detailed descriptions of related, known functions or configurations will be omitted if they are deemed to unnecessarily obscure the gist of the present invention. Furthermore, certain features presented in the drawings may be enlarged, reduced, or simplified for ease of explanation, and the drawings and their components are not necessarily drawn to scale. However, those skilled in the art will readily understand these details.

[0092]

[0093] Example 1

[0094] Polyvinyl alcohol (PVA, Sigma-Aldrich) and tannic acid (TA, Sigma-Aldrich) were dissolved in double-distilled water (DDW), respectively. PVA was dissolved by stirring at 85°C for 24 h, and TA was dissolved by stirring at room temperature for 24 h. The final concentration of TA was 4 wt%, and that of PVA was 20 wt%.

[0095] After mixing the PVA (5 mL) and TA (5 mL) solutions prepared as described above, the mixture was vigorously stirred for 10 seconds. At this stage, aqueous-to-aqueous phase separation could be observed (Fig. 1a).

[0096] The PVA / TA mixture prepared as described above was left at room temperature for 24 hours to separate the supernatant and the lower layer.

[0097]

[0098] Experimental Example 1

[0099] Presence or absence of binding of PVA and TA in the supernatant

[0100] Since coacervates are generally in a state of thermodynamic equilibrium, the components of the precipitated, dense lower layer and the supernatant are closely similar. Therefore, it was predicted that PVA and TA would also be present in the supernatant. To confirm this, gel permeation chromatography (GPC) experiments were performed using the supernatant and lower layers prepared in Example 1.

[0101] Before mixing, each component, PVA and TA, is water-soluble, so the formation of coacervate (a in Figure 1) is the result of the binding of the two molecules. However, it is necessary to confirm whether PVA and TA exist separately or are bound to each other in the supernatant. However, due to the adhesive properties of TA, it can be predicted that PVA and TA are also physically bound (b in Figure 1). If PVA and TA are bound, they can be detected by a refractive index (RI) detector and a UV detector in a gel permeation chromatography (GPC) system. PVA (13 to 23 kDa), a high molecular weight polymer, can be detected by a refractive index detector, and TA (1700 Da), a small molecule, can be detected by a UV detector. Therefore, if PVA and TA are bound, despite the low molecular weight of TA, the absorption of TA will appear in the elution time range of PVA due to the high molecular weight retention time of PVA.

[0102] Figure 2a shows that the elution time of PVA is 14.05 minutes, which was detected by the RI detector (Figure 2a, left chromatogram, second row) but not by the UV detector. For TA, the elution time was 19.19 minutes, which was detected by the UV detector but not by the RI detector (Figure 2a, right chromatogram, first row). For the PVA / TA mixture, there was a notable change in the UV detector profile, with the elution peak shifting upward to 10.27 minutes and 13.95 minutes. This change is in good agreement with the PVA profile results from the RI detector and appears in the high molecular weight range.

[0103] That is, as a result similar to the above, it can be confirmed that PVA and TA are combined to form coacervate in the supernatant.

[0104]

[0105] Experimental Example 2

[0106] Composition ratio of PVA and TA in the supernatant

[0107] An experiment was conducted to determine the specific composition ratio of PVA and TA in the supernatant.

[0108] For PVA quantification, the standard equation was derived from the GPC chromatogram, and the peak integration values ​​were obtained and calculated from samples with various PVA concentrations (y = 6.49 - (-0.39) * ln(x - 0.09); where y represents the area under the curve and x represents the molecular weight) (Fig. 2b).

[0109] For TA quantification, TA solutions of different concentrations were prepared to create a standard curve, and then the absorbance (280 nm) was measured using a UV-Vis spectrophotometer (y = -0.22+18.88x; where y represents absorbance and x represents concentration) (Fig. 2c).

[0110] Through this analysis, it was confirmed that the PVA / TA solution manufactured in Example 1 of the present invention was composed of 1.62 wt% TA and 10.15 wt% PVA. A concentration of about 10 wt% of PVA indicates that the PVA chains are entangled. As observed in Fig. 2d, from about 6 wt% of PVA, PVA exists as a cyclic polymer due to hydrogen bonding between the internal PVA chains. Therefore, according to the results, TA molecules are bound to the entangled PVA chains, which is shown in the configuration diagram in Fig. 1b.

[0111] Quantitative analysis showed that the supernatant had a PVA:TA ratio of 6.29:1, while the lower phase had a PVA:TA ratio of 4.12:1 (Fig. 3). This ratio is very similar to the initial 5:1 PVA:TA ratio used to generate the coacervate, confirming the existence of an equilibrium state of the liquid-to-liquid phase separation (LLPS) system between the supernatant and lower phases.

[0112]

[0113] Experimental Example 3

[0114] To investigate the effect of pH on the formation of PVA / TA solutions, the pH of the PVA solution was adjusted before mixing with the TA solution. The pH of the TA solution was kept constant to maintain the integrity of the hydrolyzable ester bonds. The pH of the PVA / TA solution was found to be 5.1. When the pH of the PVA solution was adjusted to 8.0, no significant change was observed in the morphology of the resulting coacervate, as shown in Figure 4. However, when the pH of the PVA solution was changed to an acidic level—specifically, to pH 3.5 and 2.0—the adhesive ability of the coacervate significantly increased. Typically, coacervates formed without pH adjustment precipitated to the bottom of the tube upon centrifugation. On the other hand, at acidic pH, the coacervate had difficulty precipitating and exhibited adhesive residue on the wall, indicating improved adhesive properties. This solution behavior is illustrated in the first two images of Figure 4. The coacervate indicated by the pink arrow remained floating or attached to the wall even after centrifugation at 3,000 rpm for 20 minutes.

[0115]

[0116] Experimental Example 4

[0117] Measurement of the change in hydrodynamic diameter of PVA / TA composites

[0118] A simple vortex experiment was conducted to measure changes in the hydrodynamic dimensions of a PVA / TA solution. 2 mL of the 1 / 100 diluted supernatant of Example 1 was vortexed (rotationally mixed) for 10 seconds, allowed to stabilize at room temperature for 5 minutes, and then this process was repeated five times.

[0119] At the end of each cycle, we measured the hydrodynamic size using dynamic light scattering (DLS). The size indeed started at 45.02 (V0) nm and gradually increased to 63.1 (V1), 76.1 (V2), 84.1 (V3), 87.6 (V4), and 93.1 (V5) nm after each cycle (Fig. 6a). This trend confirmed that the hydrodynamic size increased when an external shear force was applied through the vortex.

[0120] Measurement of the change in hydrodynamic size of PVA / TA composites

[0121] Using atomic force microscopy (AFM), we examined the bonding state of the supernatant PVA / TA before the application of a shear force (V0) and after the fifth vortex cycle (V5). As shown in Fig. 6b, the particle height and lateral dimensions of the V5 sample exceeded those of the V0 sample. When we converted the volume of each particle to the equivalent spherical volume, the V0 sample measured an average of 1.9 x 10^6 nm³ (n = 4) and the V5 sample measured 3.8 x 10^6 nm³ (n = 4), reflecting a clear increase (Fig. 6c). This evidence allowed us to confirm that the bonding between PVA chains by the external shear force increased the concentration of the supernatant.

[0122] Measurement of the change in adhesive strength of supernatant PVA / TA composites due to external shear force

[0123] Furthermore, we investigated the effect of the molecular-level hydrodynamic size increase due to the application of external shear on the adhesion strength. To measure this effect, we performed adhesion stress tests using the supernatants before (V0) and after (V5) vortexing. 200 μL of each supernatant was applied to an area of ​​3.8 cm² at both ends of two wooden rods, bonded, and then the excess was removed. After drying at room temperature for 3 hours, the adhesion strength was evaluated using a universal testing machine (UTM), applying a force of 500 N at a speed of 300 mm / min. The results, shown in Figure 7, show a 71% increase in adhesion strength, from 0.61 MPa for the V0 sample to 0.86 MPa after five vortexing cycles. Therefore, we confirmed that the adhesion strength of the supernatants increased due to the expansion of the polymer complex promoted by TA when an external shear force was applied.

[0124]

[0125] Experimental Example 5

[0126] Analysis of the bonding behavior between PVA / TA composites under external shear force

[0127] In the present invention, one of the key features of the coacervate supernatant is its remarkably low viscosity. Considering the results of Experimental Example 3, the polyphenol coacervate exhibited a unique increase in hydrodynamic volume and adhesive strength through shear-induced interactions between TA and PVA chains. Therefore, we measured the change in viscosity of the solution using a rheometer.

[0128] As the shear rate was gradually increased from 10 s-1 to 1,000 s-1, the viscosity of the supernatant continuously increased, reaching a peak at approximately 43.3 s-1. After this point, the viscosity decreased rapidly (Fig. 8a, black). This viscosity behavior was weakly observed for PVA alone (14 wt%). The viscosity increased up to 43.3 s-1, then stabilized until 280 s-1, and slightly decreased after 280 s-1 (Fig. 8a, gray).

[0129] It was predicted that unique rheological behavior would appear in response to changes in shear strain (%) as well as shear rate. To investigate this, the shear strain was varied from 10% to 6,000% while maintaining the shear rate at 1 rad / s. The values ​​of the storage modulus (G') and loss modulus (G'') were monitored during this process. As a result, it was observed that G' and G'' initially increased and then decreased sequentially. G' and G'' increased up to approximately 198% shear strain and then decreased thereafter (Fig. 8b, black). When PVA alone was tested, no such change in the shear strain-dependent behavior was detected (Fig. 8b, gray). Therefore, considering the results of Experimental Examples 4 and 5, it was confirmed that the PVA / TA composite units present in the supernatant were associated with each other. This association was promoted by the TA molecules decorated on the surface of the composite in response to vortexing or shear force. This process leads to an improvement in overall solution properties, including properties such as viscosity, storage modulus, and loss modulus. However, when extreme shear rates or shear strains are introduced, the bonding between PVA and TA exhibits reversible characteristics, resulting in the dissociation of the PVA / TA composite, resulting in a decrease in overall viscosity and rheological properties (Figure 8c).

[0130]

[0131] Experimental Example 6

[0132] Cytotoxicity analysis of supernatant

[0133] Cytotoxicity analysis of the supernatant was performed considering its water-like composition and strong adhesive properties. Equivalent concentrations of PVA (10.15 wt%) and TA (1.62 wt%) were added to the medium for comparison. The concentrations were verified by GPC for PVA and UV-Vis spectrophotometry for TA (Figs. 2b and 2c). Phosphate-buffered saline (PBS) solution served as a negative control. After 24 h of incubation, LIVE / DEAD assay and CCK-8 quantification were performed.

[0134] The number of dead cells (indicated in red) did not show a significant decrease up to 1.5 μL, and the cells did not change into a round shape (Fig. 9a). Consequently, it was observed that the cytotoxicity of TA alone was effectively alleviated when combined with PVA. The cell viability data showed that the supernatant of the present invention showed a higher viable cell ratio than TA alone at various concentrations (Fig. 9b). Specifically, the supernatant was 115 ± 13%, TA was 93 ± 4% (0.25 μL); the supernatant was 103 ± 2%, TA was 92 ± 4% (0.5 μL); the supernatant was 88 ± 9%, TA was 73 ± 10% (1 μL); the supernatant was 57 ± 10%, TA was 41 ± 30% (1.5 μL).

[0135]

[0136] Experimental Example 7

[0137] Adhesion evaluation

[0138] The dense lower layer of polyphenol coacervate is difficult to spread evenly on a surface (Figure 10). Conversely, the chemical composition of the supernatant is similar to that of the dense lower layer, but its low viscosity makes it easy to handle when used as an adhesive. This characteristic allows the supernatant to be easily applied to materials with fine curvature, such as human hair.

[0139] Hair-to-hair adhesion test using supernatant

[0140] Hair-to-hair strand adhesion was tested using human hair strands thinly coated with the supernatant.

[0141] Because individual hair strands are very thin and flexible, handling them individually is difficult. Therefore, a 30G needle was used to support the exposed hair, leaving approximately 3 cm of hair exposed. The supernatant was loaded onto a larger 18G needle, and the exposed hair was immersed in the 18G needle for 1 minute (Figure 11a). This process of attaching individual hair strands was repeated, creating a total of 10 strands.

[0142] These were then overlapped to form thicker hair fibers and threaded between the handles of a binder clip to allow lifting of a weighted object at the center (Fig. 11b). Weights of 50, 100, 200, 500, and 700 grams could be easily lifted, but the hair strands could not support a weight of 1,200 grams (Fig. 11b). Examining the magnified image of the point where the hair broke, it is clear that the failure occurred in the normal hair region, not at the hair-to-hair attachment point indicated by the dotted red box (Fig. 11b, right image). Therefore, the supernatant demonstrated its ability as an effective low-viscosity adhesive. It can be spread thinly and evenly over localized areas, such as hair, resulting in significant bond strength.

[0143] Hair-to-skin adhesion test using supernatant

[0144] The supernatant was used to test the adhesion between hair and skin. To mimic human skin conditions, pig skin was used as a substrate and heated in a 37°C warm water bath. Several human hair tips were immersed in the supernatant and then attached to pig skin. After drying the adhesive at room temperature for 5 minutes, the hair strands were successfully attached to the skin (Fig. 12a, left image). To evaluate the bond strength, the hair strands were moved back and forth using tweezers (Fig. 12a, center and right images). Although the hair strands bent due to mechanical stress, the bonded root portion maintained remarkable stability.

[0145] Test for loss of adhesion of supernatant due to moisture

[0146] A test was conducted to determine whether the supernatant's adhesive strength was lost due to moisture. As shown in Figure 12b, after applying water to the hair bonded to the pig skin, the supernatant's adhesive strength on the pig skin decreased after the fourth tweezers movement cycle. This demonstrates the easily washable nature of the supernatant, which easily loses its adhesive strength with water alone when used as a cosmetic adhesive.

[0147]

[0148] Examples 2-7

[0149] Experiments were conducted to determine the applicability of various water-soluble polyphenol compounds.

[0150] Instead of TA in Example 1, gallotannin (Example 2), ellagitannin (Example 3), proanthocyanidin (Example 4), catechin (Example 5), caffeic acid (Example 6), and chlorogenic acid (Example 7) were used, and the rest was performed in the same manner as in Example 1.

[0151]

[0152] Experimental Example 8

[0153] The supernatants of Examples 1 to 7 were collected using the same method, and then the applicability to hair was measured. At this time, 100 hairs were arranged at 0.5 mm intervals, and the supernatant was sufficiently absorbed by a 5 mm diameter brush, which was applied once back and forth to the upper part of the hair. After the application was completed, the degree to which the hair surface was coated was visually confirmed to determine the number of uncoated hairs.

[0154] In addition, the same adhesion evaluation, hair-to-skin adhesion test, and moisture-induced adhesion loss test as in Experimental Example 7 were each performed using 100 hairs. The hair used in this experiment was from a 35-year-old male, and in order to increase the objectivity of the experiment, hairs collected from each part of the head were randomly mixed and then used. For the adhesion evaluation, the maximum weight supported by each hair was measured using 100 hairs, and the average of 90 hairs after excluding the five highest and five lowest points was calculated. The hair-to-skin adhesion test was performed in the same manner as in Experimental Example 7, but the number of hairs that fell off after attachment was measured using tweezers. The moisture-induced adhesion loss test was performed by washing the hairs three times with water and then measuring the number of hairs remaining on the pig skin.

[0155] Application (ea) Adhesion evaluation (g) Adhesion test (ea) Adhesion loss test (ea) Example 12 1200 12 Example 28 1200 32 Example 34 1100 56 Example 46 1200 52 Example 57 1200 34 Example 65 1200 25 Example 73 1100 24

[0156] In the case of the adhesive strength evaluation in Table 1 above, as shown in Example 7 above, when it exceeds 1200, it is the hair itself, not the bonded portion, that breaks, and it was found that most examples satisfy 1200g.

[0157] In addition, as shown in Table 1, Example 1 of the present invention was confirmed to have excellent applicability, high adhesive strength, and to be easily removed with water. It was also confirmed that similar results to Example 1 of the present invention were obtained when other types of water-soluble polyphenol compounds were used.

[0158]

[0159] Examples 8-17

[0160] Experiments were conducted according to the amount of various polyvinyl alcohol compounds and water-soluble polyphenol compounds used.

[0161] As shown in Table 2, the contents of PVA and TA were adjusted and used, and the remaining supernatant was obtained in the same manner as in Example 1.

[0162] PVA(wt%)TA(wt%)PVA / TAExample 110.151.626.27Example 80.841.620.52Example 95.451.623.36Example 1015.341.629.47Example 1122.461.6213.86Example 1210.150.8112.53Example 1310.151.119.14Example 1410.152.593.92Example 1510.154.212.41Example 163.153.560.88Example 1716.251.2812.69

[0163] Experimental Example 9

[0164] The same experiment as Experimental Example 8 was performed using Examples 8 to 17 above.

[0165] Application (unit) Adhesion evaluation (g) Adhesion test (unit) Adhesion loss test (unit) Example 12 1 2 0 0 1 2 Example 8 5 1 2 0 0 2 5 Example 9 3 1 2 0 0 2 4 Example 10 1 3 1 0 0 1 5 6 Example 11 2 5 8 0 0 2 6 Example 12 3 6 0 0 3 5 2 Example 13 5 9 0 0 1 3 4 Example 14 1 2 1 2 0 0 1 2 Example 15 1 5 1 2 0 0 2 2 Example 16 3 1 2 0 0 2 5 Example 17 1 2 5 0 0 3 2 4

[0166] As shown in Table 3, it was confirmed that the applicability changed depending on the PVA content, and it was confirmed that the adhesive strength changed depending on the TA content. In particular, in the case of Example 8 with a reduced amount of PVA and Example 15 with an excessive amount of TA, it was confirmed that the toxicity due to the excessive amount of TA increased in the same cytotoxicity evaluation as Experimental Example 6, and this was also observed in Example 16 with a low PVA / TA ratio.

[0167]

[0168] While specific aspects of the present invention have been described in detail above, it will be apparent to those skilled in the art that these specific descriptions merely represent preferred embodiments and are not intended to limit the scope of the present invention. Therefore, the substantial scope of the present invention is defined by the appended claims and their equivalents.

Claims

1. Polyvinyl alcohol compound; Water-soluble polyphenol compounds; and menstruum; A multipurpose adhesive composition comprising:

2. In paragraph 1, A multipurpose adhesive composition characterized in that the polyvinyl alcohol compound and the water-soluble polyphenol compound form a coacervate.

3. In paragraph 2, A multipurpose adhesive composition characterized in that the polyvinyl alcohol compound and the water-soluble polyphenol compound form a coacervate through hydrogen bonding.

4. In paragraph 1, A multipurpose adhesive composition characterized in that the above polyvinyl alcohol compound is a random copolymer.

5. In paragraph 4, A multipurpose adhesive composition characterized in that the polyvinyl alcohol compound has a structure represented by the following chemical formula 1. [Chemical Formula 1] (In the chemical formula 1 above, m and n are natural numbers, and n:m is 99.9:0.1~90:10) 6. In paragraph 4, A multipurpose adhesive composition, characterized in that the polyvinyl alcohol compound has a molecular weight of 13,000 to 23,000 Da.

7. In paragraph 4, The above polyvinyl alcohol compound comprises a hydroxyl group (OH), an amine group (NH2), a succinimidyl succinate, a succinic acid, a thiol group (SH), an acrylate, an epoxide group, a maleimide, a nitrophenyl carbonate, an orthopyridyl disulfide, a tosylate group, an azide, a phosphate group, an oligoamine group ([-CH2-CH2-NH-]n), a catechol, a catecholamine, an isothiocyanate, a vinylsulfone, an aldehyde, a glyoxal, a hydrazine, an acrylamide, A multipurpose adhesive composition characterized by containing at least one functional group selected from the group consisting of methacrylate, styrene, vinylpyridine, vinyl acetate, ethylene, propylene, and vinyl chloride.

8. In paragraph 1, The above water-soluble polyphenol compounds are Hydroxybenzoic acid compounds, Hydroxycinnamic acids compounds, Flavonoids compounds, Stilbenes compounds, Caffeic acid, Chlorogenic acid, Anthocyan, Pyrogallol, Ellagic acid, Gallic acid, Catechin, Hydrolyzable Tannin, Condensed Tannin, Theaflavin-3-gallate, Quercetin, Luteolin, Hesperidin, Resveratrol, Fisetin, Naringin, Pycnogenol, Curcumin, Gingerol, A multipurpose adhesive composition characterized by comprising at least one selected from the group consisting of aloe-emodin, saponins, terpenes, lignans, lignin, curcuminoids, alkaloids, glucosinolates and phytosterols.

9. In paragraph 8, A multipurpose adhesive composition characterized in that the water-soluble polyphenol compound comprises at least one selected from the group consisting of tannic acid, gallotannins, ellagitannins, pentagalloyl glucose, casuarictin, grandin, tellimagrandin, chebulinic acid, terchebin, proanthocyanidin, prodelpinidin, catechins, epicatechins, fisetindiol, and robinetinidol.

10. In paragraph 1, A multipurpose adhesive composition characterized in that the above multipurpose adhesive composition comprises 0.1 to 20 parts by weight of the polyvinyl alcohol compound and 0.01 to 4 parts by weight of the water-soluble polyphenol compound.

11. In paragraph 10, A multipurpose adhesive composition characterized in that the polyvinyl alcohol compound and the water-soluble polyphenol compound are mixed in a weight ratio of 1:1 to 10:

1.

12. In paragraph 1, The above multipurpose adhesive composition is characterized in that it is used for bonding body hair or artificial body hair.

13. A step of preparing a coacervate solution by dissolving a polyvinyl alcohol compound and a water-soluble polyphenol compound in a solvent; and A step of separating the above coacervate solution according to specific gravity and obtaining a supernatant; A method for producing a multipurpose adhesive composition comprising:

14. In paragraph 13, The step of preparing the above coacervate solution is: A step of preparing a polyvinyl alcohol solution by dissolving a polyvinyl alcohol compound in a solvent; A step of preparing a polyphenol aqueous solution by dissolving a water-soluble polyphenol compound in a solvent; and A step of preparing a coacervate aqueous solution by mixing the above polyvinyl alcohol aqueous solution and the above polyphenol aqueous solution; A method for producing a multipurpose adhesive composition, characterized by including:

15. In paragraph 14, A method for producing a multipurpose adhesive composition, characterized in that the step of producing the above coacervate aqueous solution includes the step of mixing the above polyvinyl alcohol aqueous solution and the above polyphenol aqueous solution at a weight ratio of 1:1 to 10:1.

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