Polymer-based adhesive composition comprising graphene-based material and preparation method therefor

Abstract

The present invention relates to a polymer-based adhesive composition comprising a graphene-based material, and a preparation method therefor. The polymer-based adhesive composition according to the present invention is obtained by adding a graphene-based material to a conventional polymer-based adhesive. Compared to conventional adhesives, the polymer-based adhesive composition offers the advantages of faster internal temperature increase, resulting in reduced curing time, improved tensile strength, and enhanced adhesive force. In addition, the present invention can increase the quality of products by reducing the heat treatment time and the number of heat treatment cycles compared to conventional adhesives, and is environmentally friendly by reducing the amount of adhesive used. Furthermore, the present invention enables the bonding of multiple layers at once using a microwave oven or the like, reduces defect rates due to high heat generated at the internal bonding interface, and allows for much easier debonding compared to general adhesives, thereby being advantageous for recycling.

Description

Polymer-based adhesive composition containing graphene-based material and method for producing the same

[0001] The present invention relates to a polymer-based adhesive composition comprising a graphene-based material and a method for producing the same.

[0002] This application claims priority to Korean Patent Application No. 10-2024-0045327, filed April 3, 2024, and Korean Patent Application No. 10-2025-0042958, filed April 2, 2025, the entire contents of which are incorporated herein by reference.

[0003]

[0004] Polymer-based adhesives currently used for assembling and bonding components such as automotive interiors, clothing, and shoes work by heating to a predetermined temperature, then pressing and cooling to bond. However, if the polymer curing temperature is too high, the components may deform or decompose, resulting in poor quality. Working at too low a temperature can take longer and fail to achieve the required bonding strength. Furthermore, conventional adhesives often suffer from uneven heat transfer across the thickness of the component during curing, increasing the defect rate. Furthermore, repeated heat treatments to bond multiple layers of components can lead to product deformation and damage.

[0005] In the case of organic solvent-based polymer adhesives, problems of toxicity and environmental pollution have arisen, so recently, hydrophilic polymer adhesives have been developed. However, compared to organic solvent-based adhesives, low adhesive performance and high defect rate are problems.

[0006] Meanwhile, graphene-based materials are generally considered very important from a technological perspective due to their various excellent properties. In particular, graphene is a two-dimensional material in which six carbon atoms are connected in a hexagonal shape, and it exhibits electrical conductivity superior to any other conventional material, thermal conductivity greater than diamond, and physical strength more than 200 times greater than steel at one-sixth the weight. Furthermore, graphene can provide not only transparency, electrical properties, and gas / moisture barrier properties, but also flexibility and mechanical strength required for flexible devices. Therefore, it is a material that is receiving much attention from both academia and industry, such as its useful use in organic light-emitting diode (OLED) displays and flexible display devices, which are recently in the spotlight.

[0007] Accordingly, the inventors of the present invention sought to develop an adhesive having a shorter curing time and improved adhesive strength compared to conventional polymer-based adhesives using graphene-based materials.

[0008]

[0009] The inventors of the present invention confirmed that when a graphene-based material is added to an existing polymer-based adhesive, the internal temperature increases more quickly compared to the existing polymer-based adhesive, shortening the curing time and increasing the tensile strength, thereby improving the adhesive strength. Based on this, the present invention was completed.

[0010] Accordingly, an object of the present invention is to provide a polymer-based adhesive composition comprising a graphene-based material.

[0011] Another object of the present invention is to provide a method for preparing an adhesive composition according to the present invention, comprising the step of adding a graphene-based material to a polymer-based adhesive.

[0012]

[0013] However, the technical problems to be solved by the present invention are not limited to the problems mentioned above, and other problems not mentioned can be clearly understood by a person having ordinary skill in the technical field to which the present invention belongs from the description below.

[0014]

[0015] In order to achieve the above purpose, the present invention provides a polymer-based adhesive composition comprising a graphene-based material,

[0016] An adhesive composition is provided, characterized in that the polymer is at least one selected from the group consisting of natural polymers, thermosetting polymers, and thermoplastic polymers.

[0017] In one embodiment of the present invention, the natural polymer may be, but is not limited to, one or more plant-based polymers selected from the group consisting of starch, cellulose, tannin, gum arabic, and sodium alginate, or one or more animal-based polymers selected from the group consisting of bone glue, fish gelatin, blood protein, casein, and shellac.

[0018] In another embodiment of the present invention, the thermosetting polymer may be at least one selected from the group consisting of epoxy, phenol formaldehyde resin, unsaturated polyester, polyurethane (PU), silicone, polyimide, bismaleimide, allyl resin, furan resin, amino resin, and alkyd resin, but is not limited thereto.

[0019] In another embodiment of the present invention, the thermoplastic polymer may be at least one selected from the group consisting of polyethylene (PE), polypropylene (PP), polyvinyl chloride (PVC), polystyrene (PS), acrylic resin, nylon, polycarbonate (PC), polyoxymethylene (POM), thermoplastic polyester, polyphenylene ether (PPE), fluoropolymer, polyphenylene sulfide (PPS), polysulfone (PSU), polyketone, polyphenyl ester, and liquid crystal polymer (LCP), but is not limited thereto.

[0020] As one embodiment of the present invention, the graphene-based material may be at least one selected from the group consisting of graphene, graphite, nano / micro graphite, graphene oxide, reduced graphene oxide, graphene quantum dots, reduced graphene quantum dots, carbon nanotubes, carbon black, and carbon dots, but is not limited thereto.

[0021] As another embodiment of the present invention, the graphene-based material may be graphene or graphite and have a particle size of 1 nm to 1 mm, but is not limited thereto.

[0022] As another embodiment of the present invention, the adhesive composition is a polymer-based adhesive in which a graphene-based material is added, and the graphene-based material may be included in an amount of 0.1 to 5% (w / w) relative to the polymer-based adhesive, but is not limited thereto.

[0023] In another embodiment of the present invention, the adhesive composition comprises at least one natural polymer selected from the group consisting of cotton, linen, silk, wool, and fur;

[0024] One or more synthetic polymers selected from the group consisting of polyester, nylon, rayon, acrylic, polyurethane (PU), rubber, ethylene vinyl acetate (EVA), and thermoplastic polyurethane (TPU); and

[0025] One or more selected from the group consisting of one or more plastics selected from the group consisting of polyethylene (PE), polypropylene (PP), polystyrene (PS), acrylonitrile butadiene styrene (ABS), polyvinyl chloride (PVC), polyoxymethylene (POM), polytetrafluoroethylene (PTFE), phenol formaldehyde resin (PF), and epoxy resin (EP) can be bonded, but is not limited thereto.

[0026] As another embodiment of the present invention, the formulation of the adhesive composition may be at least one selected from the group consisting of liquid, paste, film, solid, and gel, but is not limited thereto.

[0027] As another embodiment of the present invention, the adhesive composition may be heated or cured by one or more external energies selected from the group consisting of infrared light, microwave, and radio frequency, but is not limited thereto.

[0028] As another embodiment of the present invention, the graphene-based material can absorb one or more external energies selected from the group consisting of infrared light, microwaves, and radio frequencies and emit them as heat energy, but is not limited thereto.

[0029] In addition, the present invention provides a method for preparing the adhesive composition, comprising the step of adding a graphene-based material to a polymer-based adhesive,

[0030] A manufacturing method is provided, characterized in that the polymer is at least one selected from the group consisting of natural polymers, thermosetting polymers, and thermoplastic polymers.

[0031]

[0032] The polymer-based adhesive composition according to the present invention adds a graphene-based material to a conventional polymer-based adhesive, and has the effect of improving adhesive strength by reducing the curing time and increasing the tensile strength by increasing the internal temperature more quickly than conventional polymer-based adhesives. In addition, it can improve product quality by reducing the heat treatment time and the number of heat treatment repetitions compared to conventional adhesives, and is environmentally friendly by reducing the amount of adhesive used. In addition, it can bond multiple layers simultaneously using a microwave oven, etc., and the high heat generated at the internal bonding surface can reduce the defect rate. In addition, it has the advantage of being much easier to debond than conventional adhesives, making it useful for recycling.

[0033]

[0034] FIG. 1a is a photograph showing an experiment in which infrared heating is applied to a graphene-containing polymer adhesive according to one embodiment of the present invention to measure the change in internal temperature over time.

[0035] Figure 1b is a drawing showing the results of confirming the internal temperature change over time by applying infrared heating to a graphene-containing polymer adhesive according to one embodiment of the present invention.

[0036] FIG. 2a is a drawing showing a photograph of a film formed through infrared heating to confirm the tensile strength of a graphene-containing polymer adhesive film according to one embodiment of the present invention.

[0037] Figure 2b is a drawing showing the results of confirming the change in tensile strength according to the graphene content in a graphene-containing polymer adhesive film according to one embodiment of the present invention.

[0038] FIG. 3a is a drawing showing a photograph of a peeling test for confirming the adhesive strength between various materials using a graphene-containing polymer adhesive according to one embodiment of the present invention.

[0039] Figure 3b is a drawing showing the results of confirming the adhesive strength between various materials using a graphene-containing polymer adhesive according to one embodiment of the present invention.

[0040]

[0041] The polymer-based adhesive composition according to the present invention comprises a graphene-based material, and based on the property of graphene absorbing external energy of various wavelengths and releasing it as heat energy, the adhesive performance of the adhesive can be improved, and the cost-effectiveness can be improved through process improvement, thereby reducing the defect rate.

[0042] In one embodiment of the present invention, infrared heating was applied to a general polyurethane (PU) adhesive not containing graphene flakes and a PU adhesive containing graphene flakes to check the internal temperature change over time. As a result, it was confirmed that the temperature increase occurred more quickly in the PU adhesive containing graphene flakes than in the general PU adhesive (see Example 2).

[0043] In another embodiment of the present invention, the change in tensile strength of a PU adhesive film according to the graphene flake content was confirmed, and as a result, it was confirmed that as the graphene content in the PU solution increases, more external infrared energy is absorbed and released as heat energy, so that more moisture inside is evaporated, and the curing of the adhesive is more effective, and the tensile strength of the film increases (see Example 3).

[0044] In another embodiment of the present invention, the adhesive strength between various materials was confirmed using an adhesive containing a graphene-based material, and when PU and rubber, ethylene vinyl acetate (EVA) and thermoplastic polyurethane (TPU), and EVA and rubber were bonded, it was confirmed that the adhesive strength of the PU adhesive containing graphene flakes was superior to that of a general PU adhesive (see Example 4).

[0045]

[0046] Hereinafter, the present invention will be described in detail.

[0047]

[0048] The present invention relates to a polymer-based adhesive composition comprising a graphene-based material,

[0049] An adhesive composition is provided, characterized in that the polymer is at least one selected from the group consisting of natural polymers, thermosetting polymers, and thermoplastic polymers.

[0050] In the present invention, “polymer” refers to a long chain compound formed by repeated chemical bonding of small molecules (monomers), and generally refers to a large molecule having a molecular weight ranging from several thousand to several million.

[0051] In the present invention, the natural polymer may be, but is not limited to, one or more plant-based polymers selected from the group consisting of starch, cellulose, tannin, gum arabic, and sodium alginate, or one or more animal-based polymers selected from the group consisting of bone glue, fish gelatin, blood protein, casein, and shellac.

[0052] In the present invention, the thermosetting polymer may be at least one selected from the group consisting of epoxy, phenolic resin, unsaturated polyester, polyurethane (PU), silicone, polyimide, bismaleimide, allyl resin, furan resin, amino resin, and alkyd resin, but is not limited thereto.

[0053] In the present invention, the thermoplastic polymer may be at least one selected from the group consisting of polyethylene (PE), polypropylene (PP), polyvinyl chloride (PVC), polystyrene (PS), acrylic resin, nylon, polycarbonate (PC), polyoxymethylene (POM), thermoplastic polyester, polyphenylene ether (PPE), fluoropolymer, polyphenylene sulfide (PPS), polysulfone (PSU), polyketone, polyphenyl ester, and liquid crystal polymer (LCP), but is not limited thereto.

[0054] According to one embodiment of the present invention, the polymer may be polyurethane, and the polyurethane may be prepared by mixing a polyol and an isocyanate, but is not limited thereto.

[0055] In the present invention, “graphene-based materials” means various types of materials that are functionalized or modified while having graphene as the basic structure, and the graphene-based materials may be at least one selected from the group consisting of graphene, graphite, nano / micro graphite, graphene oxide, reduced graphene oxide, graphene quantum dots, reduced graphene quantum dots, carbon nanotubes, carbon black, and carbon dots, but are not limited thereto.

[0056] Additionally, graphene-based materials have the property of absorbing a wide range of electromagnetic fields and emitting them as heat or fluorescence to the outside, and in particular, in the case of micro- or nano-sized graphene particles, they have the property of absorbing external energy in a wide range such as microwaves or near-infrared (NIR) and emitting heat.

[0057] In the present invention, the graphene-based material may be graphene or graphite, and the graphene or graphite may have a thickness of 1 nm to 1 mm, 10 nm to 1 mm, 50 nm to 1 mm, 100 nm to 1 mm, 500 nm to 1 mm, 1 μm to 1 mm, 10 μm to 1 mm, 50 μm to 1 mm, 100 μm to 1 mm, 500 μm to 1 mm, 1 nm to 500 μm, 1 nm to 100 μm, 1 nm to 50 μm, 1 nm to 10 μm, 1 nm to 1 μm, 1 nm to 500 nm, 1 nm to 100 nm, 1 nm to 50 nm, 1 nm to 10 nm, 1 μm to 500 μm, 1 μm to 100 μm, 1 μm to The graphene flakes may have a particle size of, but is not limited to, 50 μm, 1 μm to 10 μm, 1 μm to 8 μm, 1 μm to 6 μm, 1 μm to 4 μm, 2 μm to 10 μm, 2 μm to 8 μm, 2 μm to 6 μm, 2 μm to 4 μm, 3 μm to 10 μm, 3 μm to 8 μm, 3 μm to 6 μm, 3 μm to 4 μm, 4 μm to 10 μm, 4 μm to 8 μm, or 4 μm to 6 μm.

[0058] According to one embodiment of the present invention, the graphene flakes have a uniform particle size of 4 μm to 6 μm, and thus are relatively very uniformly mixed and distributed in an adhesive solution compared to other graphite or carbon nanotubes, thereby exhibiting excellent thermal properties.

[0059] In the present invention, “graphene” means a polycyclic aromatic molecule formed by a plurality of carbon atoms covalently bonded to each other, wherein the carbon atoms connected by the covalent bonds form a 6-membered ring as a basic repeating unit, but may also include a 5-membered ring and / or a 7-membered ring.

[0060] In the present invention, “graphite” is a three-dimensional material in which multiple graphene layers are stacked, with the layers weakly bonded by van der Waals forces, and is used in pencil leads, lubricants, electrodes, etc.

[0061] In the present invention, “graphene flake” means a thin, fragmented graphene sheet, which is made of graphene or graphite in the form of fine flakes.

[0062] In the present invention, the adhesive composition is a polymer-based adhesive with a graphene-based material added thereto, wherein the graphene-based material is added in an amount of 0.1 to 5% (w / w), 0.1 to 4.5% (w / w), 0.1 to 4% (w / w), 0.1 to 3.5% (w / w), 0.1 to 3% (w / w), 0.1 to 2.5% (w / w), 0.1 to 2% (w / w), 0.1 to 1.5% (w / w), 0.1 to 1% (w / w), 0.2 to 5% (w / w), 0.2 to 4.5% (w / w), 0.2 to 4% (w / w), 0.2 to 3.5% (w / w), 0.2 to 3% (w / w), 0.2 to 2.5% (w / w), 0.2 to 2 %(w / w), 0.2 to 1.5 %(w / w), 0.2 to 1 %(w / w), 0.5 to 5 %(w / w), 0.5 to 4.5 %(w / w), 0.5 to 4 %(w / w), 0.5 to 3.5 %(w / w), 0.5 to 3 %(w / w), 0.5 to 2.5 %(w / w), 0.5 to 2 %(w / w), 0.5 to 1.5 %(w / w), 0.5 to 1 %(w / w), 0.7 to 5 %(w / w), 0.7 to 4.5 %(w / w), 0.7 to 4 %(w / w), 0.7 to 3.5 %(w / w), 0.7 to 3 %(w / w), 0.7 to 2.5 %(w / w), 0.7 to 2 %(w / w), 0.7 to 1.5 %(w / w), 0.7 to 1 %(w / w), or 1 %(w / w), but is not limited thereto.

[0063] In the present invention, the formulation of the adhesive composition may be at least one selected from the group consisting of liquid, paste, film, solid, and gel, but is not limited thereto.

[0064] In the present invention, the polymer-based adhesive composition may additionally include components known to be commonly included in adhesives in addition to the graphene-based material and the polymer as an adhesive component, but is not limited thereto.

[0065] For example, the adhesive composition may further include, but is not limited to, one or more selected from the group consisting of a solvent, a curing agent, a plasticizer, a filler, an accelerator, a catalyst, a wetting agent, a surfactant, and a stabilizer.

[0066] The above solvent may be at least one selected from the group consisting of xylene, cyclohexanone, ethyl acetate, methyl ethyl ketone, toluene, isopropyl alcohol, methyl isobutyl ketone, acetone, butyl acetate, and cellosolve acetate, but is not limited thereto.

[0067] The above hardener may be one or more selected from the group consisting of isocyanate (NCO), polyamine, and moisture, but is not limited thereto.

[0068] The above plasticizer may be one or more selected from the group consisting of dioctyl phthalate (DOP), dibutyl phthalate (DBP), and adipic acid esters, but is not limited thereto.

[0069] The above filler may be one or more selected from the group consisting of calcium carbonate (CaCO₃), silica (SiO₂), and titanium oxide (TiO₂), but is not limited thereto.

[0070] The above promoter or catalyst may be an amine or organotin material, but is not limited thereto.

[0071] Siloxane or fluorine-based surfactants may be used as the above wetting agent or surfactant, but are not limited thereto.

[0072] The above stabilizer may include, but is not limited to, a UV stabilizer or an antioxidant (BHT, phenols).

[0073] In the present invention, the adhesive composition can be used for the manufacture of adhesives, sealants, coatings, embedding compounds or moldings, but is not limited thereto.

[0074] In the present invention, the adhesive composition comprises at least one natural polymer selected from the group consisting of cotton, linen, silk, wool, and fur;

[0075] One or more synthetic polymers selected from the group consisting of polyester, nylon, rayon, acrylic, polyurethane (PU), rubber, ethylene vinyl acetate (EVA), and thermoplastic polyurethane (TPU); and

[0076] One or more selected from the group consisting of one or more plastics selected from the group consisting of polyethylene (PE), polypropylene (PP), polystyrene (PS), acrylonitrile butadiene styrene (ABS), polyvinyl chloride (PVC), polyoxymethylene (POM), polytetrafluoroethylene (PTFE), phenol formaldehyde resin (PF), and epoxy resin (EP) can be bonded, but is not limited thereto.

[0077] According to one embodiment of the present invention, the adhesive composition can exhibit high adhesive strength when bonding polyurethane and rubber, but is not limited thereto.

[0078] In the present invention, the adhesive composition may be heated or cured by one or more external energies selected from the group consisting of infrared light, microwaves, and radio frequencies, but is not limited thereto. In this case, when the adhesive composition is treated with infrared light, microwaves, or radio frequencies, the curing time of the polymer-based adhesive can be shortened and the adhesive strength can be increased by utilizing the principle of absorbing external energy and releasing heat.

[0079] In the present invention, the heating is 40 to 90 ℃, 40 to 85 ℃, 40 to 80 ℃, 40 to 75 ℃, 40 to 70 ℃, 40 to 65.5 ℃, 40 to 60 ℃, 40 to 55 ℃, 40 to 50 ℃, 40 to 45 ℃, 45 to 90 ℃, 45 to 85 ℃, 45 to 80 ℃, 45 to 75 ℃, 45 to 70 ℃, 45 to 65.5 ℃, 45 to 60 ℃, 45 to 55 ℃, 45 to 50 ℃, 50 to 90 ℃, 50 to 85 ℃, 50 to 80 ℃, 50 to 75 ℃, 50 to 70 ℃, 50 to 65.5 ℃, 50 to 60 ℃, 50 to 55 ℃, 55 to 90 ℃, 55 to 85 ℃, 55 to 80 ℃, 55 to 75 ℃, 55 to 70 ℃, 55 to 65.5 ℃, 55 to 60 ℃, 60 to 90 ℃, 60 to 85 ℃, 60 to 80 ℃, 60 to 75 ℃, 60 to 70 ℃, 60 to 65.5 ℃, 63 to 90 ℃, 63 to 85 ℃, 63 to 80 ℃, 63 to 75 ℃, 63 to 70 ℃, 63 to 69 ℃, 63 to 68 ℃, It can be performed at a temperature of, but is not limited to, 63 to 67°C, 63 to 66°C, 63 to 65.5°C, or 65.5°C.

[0080] In the present invention, the curing includes drying, and at this time, the drying may be drying at the heating temperature for 5 to 30 minutes, 5 to 25 minutes, 5 to 20 minutes, 10 to 30 minutes, 10 to 25 minutes, 10 to 20 minutes, 15 to 30 minutes, 15 to 25 minutes, 15 to 20 minutes, 20 to 30 minutes, 20 to 25 minutes, or 20 minutes. In addition, after drying with the external energy, natural drying may be performed for 12 to 36 hours, 12 to 32 hours, 12 to 28 hours, 12 to 24 hours, 16 to 36 hours, 16 to 32 hours, 16 to 28 hours, 16 to 24 hours, 20 to 36 hours, 20 to 32 hours, 20 to 28 hours, 20 to 24 hours, 24 to 36 hours, 24 to 32 hours, 24 to 28 hours, or 24 hours, but is not limited thereto.

[0081]

[0082] In addition, the present invention provides a method for preparing the adhesive composition, comprising the step of adding a graphene-based material to a polymer-based adhesive,

[0083] A manufacturing method is provided, characterized in that the polymer is at least one selected from the group consisting of natural polymers, thermosetting polymers, and thermoplastic polymers.

[0084] In the present invention, the method comprises adding a graphene-based material to a polymer-based adhesive and bonding the graphene-based material at 100 to 2000 rpm, 100 to 1500 rpm, 100 to 1000 rpm, 500 to 2000 rpm, 500 to 1500 rpm, 500 to 1000 rpm, 1000 to 2000 rpm, 1000 to 1500 rpm, or 1000 rpm for 1 to 30 minutes, 1 to 25 minutes, 1 to 20 minutes, 1 to 15 minutes, 1 to 10 minutes, 5 to 30 minutes, 5 to 25 minutes, 5 to 20 minutes, 5 to 15 minutes, 5 to 10 minutes, 10 to 30 minutes, 10 to 25 minutes, 10 to 20 minutes, 10 to It may include a step of stirring for 15 minutes, or 10 minutes.

[0085] In the present invention, the temperature during the stirring may be room temperature, for example, 20 to 30°C, 20 to 29°C, 20 to 28°C, 20 to 27°C, 20 to 26°C, 20 to 25°C, 20 to 24°C, 20 to 23°C, 20 to 22°C, 20 to 21°C, 22 to 30°C, 22 to 29°C, 22 to 28°C, 22 to 27°C, 22 to 26°C, 22 to 25°C, 22 to 24°C, 22 to 23°C, 24 to 30°C, 24 to 29°C, 24 to 28°C, 24 to 27°C, 24 to 26 ℃, or 24 to 25 ℃, but is not limited thereto.

[0086] In addition, the present invention relates to an adhesive use of a polymer-based adhesive composition comprising a graphene-based material,

[0087] The invention provides a use characterized in that the polymer is at least one selected from the group consisting of natural polymers, thermosetting polymers, and thermoplastic polymers.

[0088] In addition, the present invention is for use in the manufacture of a formulation for bonding a polymer-based adhesive composition comprising a graphene-based material,

[0089] The invention provides a use characterized in that the polymer is at least one selected from the group consisting of natural polymers, thermosetting polymers, and thermoplastic polymers.

[0090]

[0091] Hereinafter, preferred examples are presented to aid in understanding the present invention. However, the following examples are provided solely to facilitate a better understanding of the present invention, and the scope of the present invention is not limited by the following examples.

[0092]

[0093] [Example]

[0094] Example 1. Preparation of a polymer adhesive comprising a graphene-based material.

[0095] A polyurethane (PU) adhesive solution was prepared by adding an isocyanate (LOCTITE AQUACE ARF-50) as a hardener to a polyol (LOCTITE AQUACE W-90S), a water-based adhesive component, at a volume ratio (v / v) of 100:5 (polyol:isocyanate) and stirring the mixture at 1,000 rpm for 10 minutes at room temperature using a stirrer.

[0096] Then, 0.1% (w / w) or 1% (w / w) of graphene flakes (GPX10), which are graphite fragments with an average size of 4 to 6 μm, were added to the PU adhesive containing the polyol and isocyanate in a ratio of 100:5, and stirred at room temperature for 10 minutes at 1,000 rpm using a stirrer to manufacture a PU adhesive including graphene flakes.

[0097]

[0098] Example 2. Confirmation of internal temperature change under infrared heating (IR heating) of an adhesive containing a graphene-based material.

[0099] Infrared heating was applied to polyurethane (PU) adhesive and PU adhesive containing 1% (w / w) graphene flakes, and the internal temperature change over time was confirmed as shown in Fig. 1a.

[0100] As a result, it was confirmed that the temperature increase occurred more rapidly in the adhesive solution containing graphene flakes (PU / G_1.0) than in the general PU adhesive (PU) not containing graphene flakes, as shown in Fig. 1b.

[0101] From this, it was found that the graphene flake-containing adhesive effectively absorbs infrared energy and increases the internal temperature more quickly.

[0102]

[0103] Example 3. Confirmation of changes in tensile strength of PU adhesive film according to graphene flake content.

[0104] After mixing 0.1% and 1.0% graphene flakes into the PU solution, films were formed using an infrared heater at 65.5°C for a certain period of time, as shown in Fig. 2a. Then, the tensile strength of each film was measured using a universal material testing machine (Z010 TN), and the average value was calculated.

[0105] As a result, as the graphene content in the PU solution increases, more external infrared energy is absorbed and released as heat energy, so that more moisture inside the PU solution is evaporated by this heat, and the curing of the adhesive is more effective. As shown in Fig. 2b, it was confirmed that the tensile strength of the PU adhesive film increases as the graphene content increases.

[0106]

[0107] Example 4. Confirmation of adhesion between various materials using an adhesive containing graphene-based materials (peeling test)

[0108] In order to bond polyurethane (PU) and rubber (PU_Rubber), ethylene vinyl acetate (EVA) and thermoplastic polyurethane (TPU) (EVA_TPU), and EVA and rubber (EVA_Rubber), a general PU-based adhesive (PU) and a PU adhesive containing 1% (w / w) of graphene flakes (PU / G_1.0) were evenly applied to their surfaces using a brush, and then a 2 kg weight was used to apply pressure for 1 minute so that the adhesives could adhere. Then, they were dried at 65.5 ℃ for 20 minutes above the heat source in an IR oven (Toshiba Speedy Convection) and naturally dried for 24 hours. Then, a peeling test was performed as shown in Fig. 3a, and the average value was calculated.

[0109] As a result, as shown in Fig. 3b, it was confirmed that the adhesive strength of the adhesive containing graphene flakes was superior to that of a general PU-based adhesive.

[0110]

[0111] The foregoing description of the present invention is provided for illustrative purposes only. Those skilled in the art will readily appreciate that the present invention can be readily modified into other specific forms without altering the technical spirit or essential characteristics of the present invention. Therefore, the embodiments described above should be understood as illustrative in all respects and not restrictive.

[0112]

[0113] The polymer-based adhesive composition according to the present invention has the effect of increasing the internal temperature more quickly than existing polymer-based adhesives, shortening the curing time and increasing the tensile strength, thereby improving the adhesive strength, and thus can be used more efficiently than existing polymer-based adhesives, and thus has industrial applicability.​

Claims

1. A polymer-based adhesive composition comprising a graphene-based material, An adhesive composition, characterized in that the polymer is at least one selected from the group consisting of natural polymers, thermosetting polymers, and thermoplastic polymers.

2. In paragraph 1, An adhesive composition characterized in that the natural polymer is at least one plant-based polymer selected from the group consisting of starch, cellulose, tannin, gum arabic, and sodium alginate, or at least one animal-based polymer selected from the group consisting of bone glue, fish gelatin, blood protein, casein, and shellac.

3. In paragraph 1, An adhesive composition characterized in that the thermosetting polymer is at least one selected from the group consisting of epoxy, phenol formaldehyde resin, unsaturated polyester, polyurethane (PU), silicone, polyimide, bismaleimide, allyl resin, furan resin, amino resin, and alkyd resin.

4. In paragraph 1, An adhesive composition characterized in that the thermoplastic polymer is at least one selected from the group consisting of polyethylene (PE), polypropylene (PP), polyvinyl chloride (PVC), polystyrene (PS), acrylic resin, nylon, polycarbonate (PC), polyoxymethylene (POM), thermoplastic polyester, polyphenylene ether (PPE), fluoropolymer, polyphenylene sulfide (PPS), polysulfone (PSU), polyketone, polyphenyl ester, and liquid crystal polymer (LCP).

5. In paragraph 1, An adhesive composition, characterized in that the graphene-based material is at least one selected from the group consisting of graphene, graphite, nano / micro graphite, graphene oxide, reduced graphene oxide, graphene quantum dots, reduced graphene quantum dots, carbon nanotubes, carbon black, and carbon dots.

6. In paragraph 5, An adhesive composition, wherein the graphene-based material is graphene or graphite and has a particle size of 1 nm to 1 mm.

7. In paragraph 1, The adhesive composition is characterized in that the graphene-based material is added to a polymer-based adhesive, and the graphene-based material is included in an amount of 0.1 to 5% (w / w) relative to the polymer-based adhesive.

8. In paragraph 1, The adhesive composition comprises at least one natural polymer selected from the group consisting of cotton, linen, silk, wool, and fur; One or more synthetic polymers selected from the group consisting of polyester, nylon, rayon, acrylic, polyurethane (PU), rubber, ethylene vinyl acetate (EVA), and thermoplastic polyurethane (TPU); and An adhesive composition characterized in that it bonds at least one selected from the group consisting of at least one plastic selected from the group consisting of polyethylene (PE), polypropylene (PP), polystyrene (PS), acrylonitrile butadiene styrene (ABS), polyvinyl chloride (PVC), polyoxymethylene (POM), polytetrafluoroethylene (PTFE), phenol formaldehyde resin (PF), and epoxy resin (EP).

9. In paragraph 1, An adhesive composition, characterized in that the formulation of the adhesive composition is at least one selected from the group consisting of liquid, paste, film, solid, and gel.

10. In paragraph 1, An adhesive composition characterized in that the adhesive composition is heated or cured by one or more external energies selected from the group consisting of infrared light, microwave, and radio frequency.

11. In paragraph 1, An adhesive composition characterized in that the graphene-based material absorbs one or more external energies selected from the group consisting of infrared light, microwaves, and radio frequencies and releases them as heat energy.

12. A method for producing an adhesive composition according to any one of claims 1 to 11, comprising the step of adding a graphene-based material to a polymer-based adhesive, A manufacturing method, characterized in that the polymer is at least one selected from the group consisting of natural polymers, thermosetting polymers, and thermoplastic polymers.

13. In paragraph 12, A manufacturing method characterized in that the natural polymer is at least one plant-based polymer selected from the group consisting of starch, cellulose, tannin, gum arabic, and sodium alginate, or at least one animal-based polymer selected from the group consisting of bone glue, fish gelatin, blood protein, casein, and shellac.

14. In paragraph 12, A manufacturing method characterized in that the thermosetting polymer is at least one selected from the group consisting of epoxy, phenol formaldehyde resin, unsaturated polyester, polyurethane (PU), silicone, polyimide, bismaleimide, allyl resin, furan resin, amino resin, and alkyd resin.

15. In paragraph 12, A manufacturing method, characterized in that the thermoplastic polymer is at least one selected from the group consisting of polyethylene (PE), polypropylene (PP), polyvinyl chloride (PVC), polystyrene (PS), acrylic resin, nylon, polycarbonate (PC), polyoxymethylene (POM), thermoplastic polyester, polyphenylene ether (PPE), fluoropolymer, polyphenylene sulfide (PPS), polysulfone (PSU), polyketone, polyphenyl ester, and liquid crystal polymer (LCP).

16. In paragraph 12, A manufacturing method, characterized in that the graphene-based material is at least one selected from the group consisting of graphene, graphite, nano / micro graphite, graphene oxide, reduced graphene oxide, graphene quantum dots, reduced graphene quantum dots, carbon nanotubes, carbon black, and carbon dots.

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