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WO2025211819A1 - Polymer-based adhesive composition comprising graphene-based material and preparation method therefor - Google Patents

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

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Publication number
WO2025211819A1
WO2025211819A1 PCT/KR2025/004479 KR2025004479W WO2025211819A1 WO 2025211819 A1 WO2025211819 A1 WO 2025211819A1 KR 2025004479 W KR2025004479 W KR 2025004479W WO 2025211819 A1 WO2025211819 A1 WO 2025211819A1
Authority
WO
WIPO (PCT)
Prior art keywords
polymer
graphene
group
adhesive composition
paragraph
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
PCT/KR2025/004479
Other languages
French (fr)
Korean (ko)
Inventor
박종보
이현택
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Graphene Square Chemical Inc
Original Assignee
Graphene Square Chemical Inc
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority claimed from KR1020250042958A external-priority patent/KR20250147302A/en
Application filed by Graphene Square Chemical Inc filed Critical Graphene Square Chemical Inc
Publication of WO2025211819A1 publication Critical patent/WO2025211819A1/en
Pending legal-status Critical Current
Anticipated expiration legal-status Critical

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/02—Elements
    • C08K3/04—Carbon
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02—Non-macromolecular additives
    • C09J11/04—Non-macromolecular additives inorganic
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J201/00—Adhesives based on unspecified macromolecular compounds
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J5/00—Adhesive processes in general; Adhesive processes not provided for elsewhere, e.g. relating to primers
    • C09J5/06—Adhesive processes in general; Adhesive processes not provided for elsewhere, e.g. relating to primers involving heating of the applied adhesive
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J7/00—Adhesives in the form of films or foils
    • C09J7/30—Adhesives in the form of films or foils characterised by the adhesive composition
    • C09J7/35—Heat-activated

Definitions

  • the present invention relates to a polymer-based adhesive composition comprising a graphene-based material and a method for producing the same.
  • 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.
  • 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.
  • conventional adhesives often suffer from uneven heat transfer across the thickness of the component during curing, increasing the defect rate.
  • repeated heat treatments to bond multiple layers of components can lead to product deformation and damage.
  • 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.
  • Figure 1b is a drawing showing the results of confirming the change in internal temperature over time by applying infrared heating to a graphene-containing polymer adhesive according to one embodiment of the present invention.
  • 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.
  • 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.
  • 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.
  • 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.
  • 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.
  • 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).
  • 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).
  • EVA ethylene vinyl acetate
  • TPU thermoplastic polyurethane
  • the present invention relates to a polymer-based adhesive composition comprising a graphene-based material
  • 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.
  • 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.
  • 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.
  • 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.
  • PE polyethylene
  • PP polypropylene
  • PVC polyvinyl chloride
  • PS polystyrene
  • acrylic resin nylon
  • PC polycarbonate
  • POM polyoxymethylene
  • thermoplastic polyester polyphenylene ether
  • PPS polyphenylene ether
  • PPS polyphenylene ether
  • PPS polysulfone
  • LCP liquid crystal polymer
  • 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.
  • 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 ⁇ m to 1 mm, 10 ⁇ m to 1 mm, 50 ⁇ m to 1 mm, 100 ⁇ m to 1 mm, 500 ⁇ m to 1 mm, 1 nm to 500 ⁇ m, 1 nm to 100 ⁇ m, 1 nm to 50 ⁇ m, 1 nm to 10 ⁇ m, 1 nm to 1 ⁇ m, 1 nm to 500 nm, 1 nm to 100 nm, 1 nm to 50 nm, 1 nm to 10 nm, 1 ⁇ m to 500 nm, 1 nm to 100 nm, 1 nm to 50 nm, 1 nm to 10 nm, 1
  • 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
  • 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.
  • 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.
  • the above hardener may be one or more selected from the group consisting of isocyanate (NCO), polyamine, and moisture, but is not limited thereto.
  • 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.
  • DOP dioctyl phthalate
  • DBP dibutyl phthalate
  • adipic acid esters but is not limited thereto.
  • 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.
  • the above promoter or catalyst may be an amine or organotin material, but is not limited thereto.
  • Siloxane or fluorine-based surfactants may be used as the above wetting agent or surfactant, but are not limited thereto.
  • the above stabilizer may include, but is not limited to, a UV stabilizer or an antioxidant (BHT, phenols).
  • the adhesive composition can be used for the manufacture of adhesives, sealants, coatings, embedding compounds or moldings, but is not limited thereto.
  • 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
  • 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.
  • the adhesive composition can exhibit high adhesive strength when bonding polyurethane and rubber, but is not limited thereto.
  • 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.
  • 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.
  • the heating is 40 to 90 °C, 40 to 85 °C, 40 to 80 °C, 40 to 75 °C, 40 to 70 °C, 40 to 65.5 °C, 40 to 60 °C, 40 to 55 °C, 40 to 50 °C, 40 to 45 °C, 45 to 90 °C, 45 to 85 °C, 45 to 80 °C, 45 to 75 °C, 45 to 70 °C, 45 to 65.5 °C, 45 to 60 °C, 45 to 55 °C, 45 to 50 °C, 50 to 90 °C, 50 to 85 °C, 50 to 80 °C, 50 to 75 °C, 50 to 70 °C, 50 to 65.5 °C, 50 to 60 °C, 50 to 55 °C, 55 to 90 °C, 55 to 85 °C, 55 to 80 °C, 55 to 75 °C, 55 to 70 °C, 55 to 60 °C, 60 to 90 °C, 55 to 85 °C, 55 to 80
  • 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.
  • 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.
  • 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,
  • 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.
  • 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.
  • 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 °C, or 24 to 25 °C, but is not limited thereto.
  • the present invention relates to an adhesive use of a polymer-based adhesive composition comprising a graphene-based material,
  • the present invention is for use in the manufacture of a formulation for bonding a polymer-based adhesive composition comprising a graphene-based material,
  • 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.
  • Example 1 Preparation of a polymer adhesive comprising a graphene-based material.
  • 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.
  • LOCTITE AQUACE ARF-50 isocyanate
  • LOCTITE AQUACE W-90S polyol
  • Example 2 Confirmation of internal temperature change under infrared heating (IR heating) of an adhesive containing a graphene-based material.
  • 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.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Inorganic Chemistry (AREA)
  • Adhesives Or Adhesive Processes (AREA)

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

그래핀 기반 물질을 포함하는 고분자 기반 접착제 조성물 및 이의 제조 방법 Polymer-based adhesive composition containing graphene-based material and method for producing the same

본 발명은 그래핀 기반 물질을 포함하는 고분자 기반 접착제 조성물 및 이의 제조 방법에 관한 것이다.The present invention relates to a polymer-based adhesive composition comprising a graphene-based material and a method for producing the same.

본 출원은 2024년 04월 03일에 출원된 한국특허출원 제10-2024-0045327호 및 2025년 04월 02일에 출원된 한국특허출원 제10-2025-0042958호에 기초한 우선권을 주장하며, 해당 출원의 명세서 및 도면에 개시된 모든 내용은 본 출원에 원용된다.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.

현재 자동차 내장재, 의류, 신발 등의 부품의 조립, 접합을 위해 사용되는 고분자 기반 접착제는 열을 이용하여 일정 온도까지 온도를 올린 후 프레싱, 냉각을 통해 결합하는 원리이다. 그러나 이 때 고분자 경화를 위한 작업온도가 너무 높은 경우 부품의 변형 또는 분해가 발생하여 품질 저하가 발행하며, 너무 낮은 온도로 작업하는 경우 작업속도가 오래 걸리고 요구되는 접착력에 미치지 못한다. 또한 기존 방식의 접착제는 경화를 위해 열을 가할 때, 부품의 두께에 따라 열이 균일하게 전달되지 않아 마찬가지로 불량률이 증가하게 된다. 아울러, 여러 층의 부품을 결합하기 위해 반복적으로 열처리를 하는 경우 제품의 변형 및 손상이 발행할 수 있다.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.

유기용매 기반 고분자 접착체의 경우 독성 및 환경오염의 문제가 발생되어 최근 친수성 기반의 폴리머 접착체 개발이 이루어지고 있으나, 유기용매 기반 접착체에 비해 접착성능이 낮고 불량률이 높은 것이 문제가 되고 있다.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.

한편, 일반적으로 그래핀 기반 물질은 여러 우수한 특성들을 가지기 때문에 기술적으로 매우 중요하게 고려되고 있다. 특히, 그래핀은 탄소 6개가 육각형의 형태로 연결된 2차원 형태의 물질로서 종래의 다른 어떤 물질들보다도 우수한 전기 전도성을 나타내고, 다이아몬드보다 더 큰 열 전도성을 가지며, 6분의 1의 무게로도 강철보다 200배 이상 더 큰 물리적 강도를 가진다. 또한, 그래핀은 투명도(Transparency), 전기적 특성(Electrical property), 기체/수분 베리어 특성(Gas/Moisture barrier property) 뿐만 아니라 플렉서블(Flexible) 디바이스에서 요구되는 연성(flexibility)과 물리적 강도(Mechanical strength)도 제공할 수 있기 때문에, 최근 각광받는 유기 발광 다이오드(OLED) 디스플레이나 플렉서블 디스플레이 디바이스에서도 유용하게 사용되는 등 학계 및 산학계에서 많은 관심을 받고 있는 물질이다. 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.

이에, 본 발명자들은 그래핀 기반 물질을 이용하여 기존의 고분자 기반 접착제에 비해 경화 시간이 단축되고 접착력이 향상된 접착제를 개발하고자 하였다.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.

본 발명자들은 기존의 고분자 기반 접착제에 그래핀 기반 물질을 첨가한 경우 기존 고분자 기반 접착제에 비해 내부 온도가 더 빨리 증가하여 경화 시간이 단축되고 인장강도가 증가하여 접착력이 향상된 것을 확인하였는 바, 이에 기초하여 본 발명을 완성하였다.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.

이에, 본 발명의 목적은 그래핀 기반 물질을 포함하는 고분자 기반 접착제 조성물을 제공하는 것이다.Accordingly, an object of the present invention is to provide a polymer-based adhesive composition comprising a graphene-based material.

본 발명의 다른 목적은 고분자 기반 접착제에 그래핀 기반 물질을 첨가하는 단계를 포함하는, 본 발명에 따른 접착제 조성물의 제조 방법을 제공하는 것이다.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.

그러나, 본 발명이 이루고자 하는 기술적 과제는 이상에서 언급한 과제에 제한되지 않으며, 언급되지 않은 또 다른 과제들은 아래의 기재로부터 본 발명이 속하는 기술 분야의 통상의 지식을 가진 자에게 명확하게 이해될 수 있을 것이다.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.

상기와 같은 목적을 달성하기 위해 본 발명은 그래핀 기반 물질을 포함하는 고분자 기반 접착제 조성물로서,In order to achieve the above purpose, the present invention provides a polymer-based adhesive composition comprising a graphene-based material,

상기 고분자는 천연 고분자, 열경화성 고분자, 및 열가소성 고분자로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 접착제 조성물을 제공한다.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.

본 발명의 일 구현예로서, 상기 천연 고분자는 전분(Starch), 셀룰로오스(Cellulose), 탄닌(Tannin), 아라비아 고무(Gum Arabic), 및 알긴산 나트륨(Sodium Alginate)으로 이루어진 군으로부터 선택된 하나 이상의 식물성 고분자 또는 뼈 아교(Bone Glue), 생선 젤라틴(Fish Gelatin), 혈액 단백질(Blood Protein), 카제인(Casein), 및 셸락(Shellac)으로 이루어진 군으로부터 선택된 하나 이상의 동물성 고분자일 수 있으나, 이에 제한되지 않는다.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.

본 발명의 다른 구현예로서, 상기 열경화성 고분자는 에폭시(Epoxy), 페놀 수지(Phenol Formaldehyde Resin), 불포화 폴리에스터(Unsaturated Polyester), 폴리우레탄(Polyurethane, PU), 실리콘(Silicone), 폴리이미드(Polyimide), 비스말레이미드(Bismaleimide), 알릴 수지(Allyl Resin), 푸란 수지(Furan Resin), 아미노 수지(Amino Resin), 및 알키드 수지(Alkyd Resin)로 이루어진 군으로부터 선택된 하나 이상일 수 있으나, 이에 제한되지 않는다.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.

본 발명의 또 다른 구현예로서, 상기 열가소성 고분자는 폴리에틸렌(Polyethylene, PE), 폴리프로필렌(Polypropylene, PP), 폴리염화비닐(Polyvinyl Chloride, PVC), 폴리스티렌(Polystyrene, PS), 아크릴 수지(Acrylic Resin), 나일론(Nylon), 폴리카보네이트(Polycarbonate, PC), 폴리옥시메틸렌(Polyoxymethylene, POM), 열가소성 폴리에스터(Thermoplastic Polyester), 폴리페닐렌 에테르(Polyphenylene Ether, PPE), 불소수지(Fluoropolymer), 폴리페닐렌 설파이드(Polyphenylene Sulfide, PPS), 폴리설폰(Polysulfone, PSU), 폴리케톤(Polyketone), 폴리페닐 에스테르(Polyphenyl Ester), 및 액정 폴리머(Liquid Crystal Polymer, LCP)로 이루어진 군으로부터 선택된 하나 이상일 수 있으나, 이에 제한되지 않는다.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.

본 발명의 일 구현예로서, 상기 그래핀 기반 물질은 그래핀, 그래파이트, 나노/마이크로 그래파이트, 산화그래핀, 환원된 산화그래핀, 그래핀양자점, 환원된 그래핀 양자점, 탄소나노튜브, 카본블랙, 및 카본 닷으로 이루어진 군으로부터 선택된 하나 이상일 수 있으나, 이에 제한되지 않는다.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.

본 발명의 다른 구현예로서, 상기 그래핀 기반 물질은 그래핀 또는 그래파이트이고, 1 nm 내지 1 mm의 입자 크기를 가지는 것일 수 있으나, 이에 제한되지 않는다.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.

본 발명의 또 다른 구현예로서, 상기 접착제 조성물은 고분자 기반 접착제에 그래핀 기반 물질이 추가된 것으로서, 상기 그래핀 기반 물질은 고분자 기반 접착제 대비 0.1 내지 5 %(w/w)로 포함될 수 있으나, 이에 제한되지 않는다.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.

본 발명의 또 다른 구현예로서, 상기 접착제 조성물은 면, 린넨, 실크, 울, 및 모피로 이루어진 군으로부터 선택된 하나 이상의 천연 고분자;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;

폴리에스터(Polyester), 나일론(Nylon), 레이온(Rayon), 아크릴(Acrylic), 폴리우레탄(Polyurethane, PU), 고무(rubber), 에틸렌 비닐 아세테이트(Ethylene vinyl acetate, EVA), 및 열가소성 폴리우레탄(Thermoplastic polyurethane, TPU)으로 이루어진 군으로부터 선택된 하나 이상의 합성 고분자; 및One 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

폴리에틸렌(Polyethylene, PE), 폴리프로필렌(Polypropylene, PP), 폴리스티렌(Polystyrene, PS), ABS 수지(Acrylonitrile Butadiene Styrene, ABS), 폴리염화비닐(Polyvinyl Chloride, PVC), 폴리아세탈(Polyoxymethylene, POM), 폴리테트라플루오로에틸렌(Polytetrafluoroethylene, PTFE), 페놀 수지(Phenol Formaldehyde Resin, PF), 및 에폭시 수지(Epoxy Resin, EP)로 이루어진 군으로부터 선택된 하나 이상의 플라스틱으로 이루어진 군으로부터 선택된 하나 이상을 접착시킬 수 있으나, 이에 제한되지 않는다.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.

본 발명의 또 다른 구현예로서, 상기 접착제 조성물의 제형은 액상(liquid), 페이스트(paste), 필름(film), 고체(solid), 및 겔(gel)로 이루어진 군으로부터 선택된 하나 이상일 수 있으나, 이에 제한되지 않는다.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.

본 발명의 또 다른 구현예로서, 상기 접착제 조성물은 적외선(Infrared light), 마이크로파(microwave), 및 무선 주파수(radio frequency)로 이루어진 군으로부터 선택된 하나 이상의 외부에너지로 가열 또는 경화되는 것일 수 있으나, 이에 제한되지 않는다.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.

본 발명의 또 다른 구현예로서, 상기 그래핀 기반 물질은 적외선(Infrared light), 마이크로파(microwave), 및 무선 주파수(radio frequency)로 이루어진 군으로부터 선택된 하나 이상의 외부에너지를 흡수하여 열에너지로 방출할 수 있으나, 이에 제한되지 않는다.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.

또한, 본 발명은 고분자 기반 접착제에 그래핀 기반 물질을 첨가하는 단계를 포함하는, 상기 접착제 조성물의 제조 방법으로서,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,

상기 고분자는 천연 고분자, 열경화성 고분자, 및 열가소성 고분자로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 제조 방법을 제공한다.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.

본 발명에 따른 고분자 기반 접착제 조성물은 기존의 고분자 기반 접착제에 그래핀 기반 물질을 첨가한 것으로서, 기존 고분자 기반 접착제에 비해 내부 온도가 더 빨리 증가하여 경화 시간이 단축되고 인장강도가 증가하여 접착력이 향상되는 효과가 있다. 또한 기존 접착제 대비 열처리 시간 및 열처리 반복횟수를 줄임으로써 제품의 품질을 높일 수 있고, 접착제 사용량을 줄임으로써 친환경적이다. 이에 더하여, 마이크로 오븐 등을 이용하여 여러 층을 한 번에 접착 가능하고, 내부 접착면에서 발생되는 높은 열로 불량률을 줄일 수 있으며, 일반적인 접착제와 비교하여 훨씬 더 손쉽게 디본딩(debonding)이 가능하여 재활용이 유용한 장점이 있다.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.

도 1a는 본 발명의 일 구현예에 따른 그래핀 함유 고분자 접착제에 적외선 가열을 가하여 시간에 따른 내부 온도 변화를 측정하는 실험에 대한 사진을 나타낸 도면이다.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.

도 1b는 본 발명의 일 구현예에 따른 그래핀 함유 고분자 접착제에 적외선 가열을 가하여 시간에 따른 내부 온도 변화를 확인한 결과를 나타낸 도면이다.Figure 1b is a drawing showing the results of confirming the change in internal temperature over time by applying infrared heating to a graphene-containing polymer adhesive according to one embodiment of the present invention.

도 2a는 본 발명의 일 구현예에 따른 그래핀 함유 고분자 접착제 필름의 인장강도를 확인하기 위해 적외선 가열을 통해 성형한 필름 사진을 나타낸 도면이다.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.

도 2b는 본 발명의 일 구현예에 따른 그래핀 함유 고분자 접착제 필름에서 그래핀 함유량에 따른 인장강도 변화를 확인한 결과를 나타낸 도면이다.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.

도 3a는 본 발명의 일 구현예에 따른 그래핀 함유 고분자 접착제를 이용한 다양한 물질 간의 접착력을 확인하기 위한 필링 테스트에 대한 사진을 나타낸 도면이다.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.

도 3b는 본 발명의 일 구현예에 따른 그래핀 함유 고분자 접착제를 이용한 다양한 물질 간의 접착력을 확인한 결과를 나타낸 도면이다.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.

본 발명에 따른 고분자 기반 접착제 조성물은 그래핀 기반 물질을 포함하는 것으로서, 그래핀이 다양한 파장의 외부에너지를 흡수하여 열에너지로 방출하는 특성을 기반으로 하여, 접착제의 접착 성능을 향상시키고 공정 개선을 통한 경제성을 향상시켜 불량률을 감소시킬 수 있다. 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.

본 발명의 일 실시예에서는 그래핀 플레이크를 함유하지 않는 일반적인 폴리우레탄(PU) 접착제 및 그래핀 플레이크를 함유하는 PU 접착제에 적외선 가열을 가하여 시간에 따른 내부 온도 변화를 확인한 결과, 그래핀 플레이크를 함유하는 PU 접착제에서 일반적인 PU 접착제에 비해 더 빠르게 온도 증가가 일어남을 확인하였다(실시예 2 참조).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).

본 발명의 다른 실시예에서는 그래핀 플레이크 함유량에 따른 PU 접착제 필름의 인장강도 변화를 확인한 결과, PU 용액 내에 그래핀 함량이 증가할수록 외부 적외선 에너지를 더 많이 흡수하여 이를 열에너지로 방출함으로써 내부의 수분이 더 많이 증발되어 접착제의 경화가 더 효과적으로 이루어지며 필름의 인장강도가 증가하는 것을 확인하였다(실시예 3 참조).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).

본 발명의 또 다른 실시예에서는 그래핀 기반 물질을 포함하는 접착제를 이용하여 다양한 물질 간 접착력을 확인한 결과, PU와 고무, 에틸렌 비닐 아세테이트(EVA)와 열가소성 폴리우레탄(TPU), EVA와 고무를 접착시킨 경우 그래핀 플레이크 함유 PU 접착제의 접착력이 일반 PU 접착제에 비해 우수한 것을 확인하였다(실시예 4 참조).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).

이하, 본 발명을 상세히 설명한다.Hereinafter, the present invention will be described in detail.

본 발명은 그래핀 기반 물질을 포함하는 고분자 기반 접착제 조성물로서,The present invention relates to a polymer-based adhesive composition comprising a graphene-based material,

상기 고분자는 천연 고분자, 열경화성 고분자, 및 열가소성 고분자로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 접착제 조성물을 제공한다.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.

본 발명에 있어서, “고분자(polymer)”는 작은 분자(단량체, Monomer)들이 반복적으로 화학 결합하여 형성된 긴 사슬형 화합물이며, 일반적으로 분자량이 수천~수백만에 이르는 거대 분자를 의미한다.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.

본 발명에 있어서, 상기 천연 고분자는 전분(Starch), 셀룰로오스(Cellulose), 탄닌(Tannin), 아라비아 고무(Gum Arabic), 및 알긴산 나트륨(Sodium Alginate)으로 이루어진 군으로부터 선택된 하나 이상의 식물성 고분자 또는 뼈 아교(Bone Glue), 생선 젤라틴(Fish Gelatin), 혈액 단백질(Blood Protein), 카제인(Casein), 및 셸락(Shellac)으로 이루어진 군으로부터 선택된 하나 이상의 동물성 고분자일 수 있으나, 이에 제한되지 않는다.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.

본 발명에 있어서, 상기 열경화성 고분자는 에폭시(Epoxy), 페놀 수지(Phenolic Resin), 불포화 폴리에스터(Unsaturated Polyester), 폴리우레탄(Polyurethane, PU), 실리콘(Silicone), 폴리이미드(Polyimide), 비스말레이미드(Bismaleimide), 알릴 수지(Allyl Resin), 푸란 수지(Furan Resin), 아미노 수지(Amino Resin), 및 알키드 수지(Alkyd Resin)로 이루어진 군으로부터 선택된 하나 이상일 수 있으나, 이에 제한되지 않는다.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.

본 발명에 있어서, 상기 열가소성 고분자는 폴리에틸렌(Polyethylene, PE), 폴리프로필렌(Polypropylene, PP), 폴리염화비닐(Polyvinyl Chloride, PVC), 폴리스티렌(Polystyrene, PS), 아크릴 수지(Acrylic Resin), 나일론(Nylon), 폴리카보네이트(Polycarbonate, PC), 폴리옥시메틸렌(Polyoxymethylene, POM), 열가소성 폴리에스터(Thermoplastic Polyester), 폴리페닐렌 에테르(Polyphenylene Ether, PPE), 불소수지(Fluoropolymer), 폴리페닐렌 설파이드(Polyphenylene Sulfide, PPS), 폴리설폰(Polysulfone, PSU), 폴리케톤(Polyketone), 폴리페닐 에스테르(Polyphenyl Ester), 및 액정 폴리머(Liquid Crystal Polymer, LCP)로 이루어진 군으로부터 선택된 하나 이상일 수 있으나, 이에 제한되지 않는다.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.

본 발명의 일 실시예에 따르면, 상기 고분자는 폴리우레탄일 수 있으며, 상기 폴리우레탄은 폴리올 및 아이소시아네이트를 혼합하여 제조된 것일 수 있으나, 이에 제한되지 않는다.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.

본 발명에 있어서, “그래핀 기반 물질(Graphene-based materials)”은 그래핀(graphene)을 기본 구조로 하면서 기능화되거나 변형된 다양한 형태의 재료를 의미하며, 상기 그래핀 기반 물질은 그래핀, 그래파이트, 나노/마이크로 그래파이트, 산화그래핀, 환원된 산화그래핀, 그래핀양자점, 환원된 그래핀 양자점, 탄소나노튜브, 카본블랙, 및 카본 닷으로 이루어진 군으로부터 선택된 하나 이상일 수 있으나, 이에 제한되지 않는다.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.

또한, 그래핀 기반 물질은 넓은 범위의 전자기장을 흡수하여 외부에 열 또는 형광으로 방출하는 특성이 있으며, 특히 마이크로 또는 나노 크기의 그래핀 입자의 경우 마이크로파(microwave) 또는 근적외선(Near-Infrared, NIR) 등 넓은 영역에서 외부 에너지를 흡수하여 열을 방출하는 특성을 갖는다.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.

본 발명에 있어서, 상기 그래핀 기반 물질은 그래핀 또는 그래파이트일 수 있으며, 상기 그래핀 또는 그래파이트는 1 nm 내지 1 mm, 10 nm 내지 1 mm, 50 nm 내지 1 mm, 100 nm 내지 1 mm, 500 nm 내지 1 mm, 1 μm 내지 1 mm, 10 μm 내지 1 mm, 50 μm 내지 1 mm, 100 μm 내지 1 mm, 500 μm 내지 1 mm, 1 nm 내지 500 μm, 1 nm 내지 100 μm, 1 nm 내지 50 μm, 1 nm 내지 10 μm, 1 nm 내지 1 μm, 1 nm 내지 500 nm, 1 nm 내지 100 nm, 1 nm 내지 50 nm, 1 nm 내지 10 nm, 1 μm 내지 500 μm, 1 μm 내지 100 μm, 1 μm 내지 50 μm, 1 μm 내지 10 μm, 1 μm 내지 8 μm, 1 μm 내지 6 μm, 1 μm 내지 4 μm, 2 μm 내지 10 μm, 2 μm 내지 8 μm, 2 μm 내지 6 μm, 2 μm 내지 4 μm, 3 μm 내지 10 μm, 3 μm 내지 8 μm, 3 μm 내지 6 μm, 3 μm 내지 4 μm, 4 μm 내지 10 μm, 4 μm 내지 8 μm, 또는 4 μm 내지 6 μm의 입자 크기를 가지는 그래핀 플레이크일 수 있으나, 이에 제한되지 않는다.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.

본 발명의 일 실시예에 따르면, 상기 그래핀 플레이크는 4 μm 내지 6 μm의 균일한 입자 크기를 가짐으로써 다른 그래파이트 또는 탄소나노튜브와 비교하여 접착제 용액에서 상대적으로 매우 균일하게 섞여서 분포하여, 우수한 열적 특성을 낼 수 있다. 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.

본 발명에 있어서, “그래핀(grapheme)”은 복수개의 탄소 원자들이 서로 공유결합으로 연결되어 폴리시클릭 방향족 분자를 형성한 것을 의미하는 것으로서, 상기 공유 결합으로 연결된 탄소 원자들은 기본 반복 단위로서 6 원환을 형성하나, 5원환 및/또는 7 원환을 더 포함하는 것도 가능하다.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.

본 발명에 있어서, “그래파이트(Graphite)”는 여러 개의 그래핀(Graphene) 층이 쌓인 3차원 물질로서, 층과 층 사이가 반데르발스 힘으로 약하게 결합되어 있고, 연필심, 윤활제, 전극 등에 사용된다. 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.

본 발명에 있어서, “그래핀 플레이크”는 얇고 조각난 형태의 그래핀 시트로서, 그래핀 또는 그래파이트를 미세한 조각(flake) 형태로 만든 것을 의미한다.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.

본 발명에 있어서, 상기 접착제 조성물은 고분자 기반 접착제에 그래핀 기반 물질이 추가된 것으로서, 상기 그래핀 기반 물질은 고분자 기반 접착제 대비 0.1 내지 5 %(w/w), 0.1 내지 4.5 %(w/w), 0.1 내지 4 %(w/w), 0.1 내지 3.5 %(w/w), 0.1 내지 3 %(w/w), 0.1 내지 2.5 %(w/w), 0.1 내지 2 %(w/w), 0.1 내지 1.5 %(w/w), 0.1 내지 1 %(w/w), 0.2 내지 5 %(w/w), 0.2 내지 4.5 %(w/w), 0.2 내지 4 %(w/w), 0.2 내지 3.5 %(w/w), 0.2 내지 3 %(w/w), 0.2 내지 2.5 %(w/w), 0.2 내지 2 %(w/w), 0.2 내지 1.5 %(w/w), 0.2 내지 1 %(w/w), 0.5 내지 5 %(w/w), 0.5 내지 4.5 %(w/w), 0.5 내지 4 %(w/w), 0.5 내지 3.5 %(w/w), 0.5 내지 3 %(w/w), 0.5 내지 2.5 %(w/w), 0.5 내지 2 %(w/w), 0.5 내지 1.5 %(w/w), 0.5 내지 1 %(w/w), 0.7 내지 5 %(w/w), 0.7 내지 4.5 %(w/w), 0.7 내지 4 %(w/w), 0.7 내지 3.5 %(w/w), 0.7 내지 3 %(w/w), 0.7 내지 2.5 %(w/w), 0.7 내지 2 %(w/w), 0.7 내지 1.5 %(w/w), 0.7 내지 1 %(w/w), 또는 1 %(w/w)로 포함될 수 있으나, 이에 제한되지 않는다.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.

본 발명에 있어서, 상기 접착제 조성물의 제형은 액상(liquid), 페이스트(paste), 필름(film), 고체(solid), 및 겔(gel)로 이루어진 군으로부터 선택된 하나 이상일 수 있으나, 이에 제한되지 않는다.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.

본 발명에 있어서, 상기 고분자 기반 접착제 조성물은 그래핀 기반 물질 및 접착 성분인 고분자 외에 통상적으로 접착제에 포함되는 것으로 알려진 성분들을 추가로 포함할 수 있으나, 이에 제한되지 않는다. 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.

예를 들어, 상기 접착제 조성물은 용제, 경화제, 가소제, 충전제, 촉진제, 촉매, 습윤제, 계면활성제, 및 안정제로 이루어진 군으로부터 선택된 하나 이상을 더 포함할 수 있으나, 이에 제한되지 않는다.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.

상기 용제로는 자일렌, 시클로헥사논, 에틸아세테이트, 메틸에틸케톤, 톨루엔, 이소프로필알콜, 메틸이소부틸케톤, 아세톤, 부틸아세테이트 및 셀로솔브아세테이트로 이루어진 군에서 선택된 하나 이상을 사용할 수 있으나, 이에 제한되지 않는다.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.

상기 경화제로는 이소시아네이트계(NCO), 폴리아민(Polyamine), 및 수분(Moisture)으로 이루어진 군으로부터 선택된 하나 이상을 사용할 수 있으나, 이에 제한되지 않는다.The above hardener may be one or more selected from the group consisting of isocyanate (NCO), polyamine, and moisture, but is not limited thereto.

상기 가소제로는 디옥틸프탈레이트(DOP), 디부틸프탈레이트(DBP), 및 아디픽산 에스터류로 이루어진 군으로부터 선택된 하나 이상을 사용할 수 있으나, 이에 제한되지 않는다.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.

상기 충전제로는 탄산칼슘(CaCO₃), 실리카(SiO₂), 및 산화티타늄(TiO₂)으로 이루어진 군으로부터 선택된 하나 이상을 사용할 수 있으나, 이에 제한되지 않는다.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.

상기 촉진제 또는 촉매로는 아민계(Amines) 또는 유기주석계(Organotin) 물질을 사용할 수 있으나, 이에 제한되지 않는다.The above promoter or catalyst may be an amine or organotin material, but is not limited thereto.

상기 습윤제 또는 계면활성제로는 실록산계(Siloxane) 또는 불소계 계면활성제를 사용할 수 있으나, 이에 제한되지 않는다.Siloxane or fluorine-based surfactants may be used as the above wetting agent or surfactant, but are not limited thereto.

상기 안정제로는 UV 안정제 또는 항산화제(BHT, 페놀류)를 사용할 수 있으나, 이에 제한되지 않는다.The above stabilizer may include, but is not limited to, a UV stabilizer or an antioxidant (BHT, phenols).

본 발명에 있어서, 상기 접착제 조성물은 접착제, 밀봉제, 코팅, 매립 화합물(embedding compounds) 또는 몰딩의 제조를 위해 사용될 수 있으나, 이에 제한되지 않는다.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.

본 발명에 있어서, 상기 접착제 조성물은 면, 린넨, 실크, 울, 및 모피로 이루어진 군으로부터 선택된 하나 이상의 천연 고분자;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;

폴리에스터(Polyester), 나일론(Nylon), 레이온(Rayon), 아크릴(Acrylic), 폴리우레탄(Polyurethane, PU), 고무(rubber), 에틸렌 비닐 아세테이트(Ethylene vinyl acetate, EVA), 및 열가소성 폴리우레탄(Thermoplastic polyurethane, TPU)으로 이루어진 군으로부터 선택된 하나 이상의 합성 고분자; 및One 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

폴리에틸렌(Polyethylene, PE), 폴리프로필렌(Polypropylene, PP), 폴리스티렌(Polystyrene, PS), ABS 수지(Acrylonitrile Butadiene Styrene, ABS), 폴리염화비닐(Polyvinyl Chloride, PVC), 폴리아세탈(Polyoxymethylene, POM), 폴리테트라플루오로에틸렌(Polytetrafluoroethylene, PTFE), 페놀 수지(Phenol Formaldehyde Resin, PF), 및 에폭시 수지(Epoxy Resin, EP)로 이루어진 군으로부터 선택된 하나 이상의 플라스틱으로 이루어진 군으로부터 선택된 하나 이상을 접착시킬 수 있으나, 이에 제한되지 않는다. 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.

본 발명의 일 실시예에 따르면, 상기 접착제 조성물은 폴리우레탄 및 고무를 접착시킬 경우 높은 접착력을 나타낼 수 있으나, 이에 제한되지 않는다.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.

본 발명에 있어서, 상기 접착제 조성물은 적외선(Infrared light), 마이크로파(microwave), 및 무선 주파수(radio frequency)로 이루어진 군으로부터 선택된 하나 이상의 외부에너지로 가열 또는 경화되는 것일 수 있으나, 이에 제한되지 않는다. 이때, 상기 접착제 조성물에 적외선, 마이크로파, 또는 무선 주파수 등을 처리할 경우 외부에너지를 흡수하여 열을 방출하는 원리를 이용하여 고분자 기반 접착제의 경화시간을 단축시키고 접착력을 증가시킬 수 있다.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.

본 발명에 있어서, 상기 가열은 40 내지 90 ℃, 40 내지 85 ℃, 40 내지 80 ℃, 40 내지 75 ℃, 40 내지 70 ℃, 40 내지 65.5 ℃, 40 내지 60 ℃, 40 내지 55 ℃, 40 내지 50 ℃, 40 내지 45 ℃, 45 내지 90 ℃, 45 내지 85 ℃, 45 내지 80 ℃, 45 내지 75 ℃, 45 내지 70 ℃, 45 내지 65.5 ℃, 45 내지 60 ℃, 45 내지 55 ℃, 45 내지 50 ℃, 50 내지 90 ℃, 50 내지 85 ℃, 50 내지 80 ℃, 50 내지 75 ℃, 50 내지 70 ℃, 50 내지 65.5 ℃, 50 내지 60 ℃, 50 내지 55 ℃, 55 내지 90 ℃, 55 내지 85 ℃, 55 내지 80 ℃, 55 내지 75 ℃, 55 내지 70 ℃, 55 내지 65.5 ℃, 55 내지 60 ℃, 60 내지 90 ℃, 60 내지 85 ℃, 60 내지 80 ℃, 60 내지 75 ℃, 60 내지 70 ℃, 60 내지 65.5 ℃, 63 내지 90 ℃, 63 내지 85 ℃, 63 내지 80 ℃, 63 내지 75 ℃, 63 내지 70 ℃, 63 내지 69 ℃, 63 내지 68 ℃, 63 내지 67 ℃, 63 내지 66 ℃, 63 내지 65.5 ℃, 또는 65.5 ℃의 온도에서 이루어질 수 있으나, 이에 제한되지 않는다.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.

본 발명에 있어서, 상기 경화는 건조를 포함하며, 이때 건조는 상기 가열 온도에서 5 내지 30분, 5 내지 25분, 5 내지 20분, 10 내지 30분, 10 내지 25분, 10 내지 20분, 15 내지 30분, 15 내지 25분, 15 내지 20분, 20 내지 30분, 20 내지 25분, 또는 20분 동안 건조하는 것일 수 있다. 또한, 상기 외부에너지로 건조 후 12 내지 36시간, 12 내지 32시간, 12 내지 28시간, 12 내지 24시간, 16 내지 36시간, 16 내지 32시간, 16 내지 28시간, 16 내지 24시간, 20 내지 36시간, 20 내지 32시간, 20 내지 28시간, 20 내지 24시간, 24 내지 36시간, 24 내지 32시간, 24 내지 28시간, 또는 24시간 동안 자연건조할 수 있으나, 이에 제한되지 않는다. 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.

또한, 본 발명은 고분자 기반 접착제에 그래핀 기반 물질을 첨가하는 단계를 포함하는, 상기 접착제 조성물의 제조 방법으로서,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,

상기 고분자는 천연 고분자, 열경화성 고분자, 및 열가소성 고분자로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 제조 방법을 제공한다.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.

본 발명에 있어서, 상기 방법은 고분자 기반 접착제에 그래핀 기반 물질을 넣고 100 내지 2000 rpm, 100 내지 1500 rpm, 100 내지 1000 rpm, 500 내지 2000 rpm, 500 내지 1500 rpm, 500 내지 1000 rpm, 1000 내지 2000 rpm, 1000 내지 1500 rpm, 또는 1000 rpm으로 1 내지 30분, 1 내지 25분, 1 내지 20분, 1 내지 15분, 1 내지 10분, 5 내지 30분, 5 내지 25분, 5 내지 20분, 5 내지 15분, 5 내지 10분, 10 내지 30분, 10 내지 25분, 10 내지 20분, 10 내지 15분, 또는 10분 동안 교반하는 단계를 포함할 수 있다.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.

본 발명에 있어서, 상기 교반 시 온도는 상온일 수 있으며, 예컨대 20 내지 30 ℃, 20 내지 29 ℃, 20 내지 28 ℃, 20 내지 27 ℃, 20 내지 26 ℃, 20 내지 25 ℃, 20 내지 24 ℃, 20 내지 23 ℃, 20 내지 22 ℃, 20 내지 21 ℃, 22 내지 30 ℃, 22 내지 29 ℃, 22 내지 28 ℃, 22 내지 27 ℃, 22 내지 26 ℃, 22 내지 25 ℃, 22 내지 24 ℃, 22 내지 23 ℃, 24 내지 30 ℃, 24 내지 29 ℃, 24 내지 28 ℃, 24 내지 27 ℃, 24 내지 26 ℃, 또는 24 내지 25 ℃일 수 있으나, 이에 제한되지 않는다.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.

또한, 본 발명은 그래핀 기반 물질을 포함하는 고분자 기반 접착제 조성물의 접착 용도로서, In addition, the present invention relates to an adhesive use of a polymer-based adhesive composition comprising a graphene-based material,

상기 고분자는 천연 고분자, 열경화성 고분자, 및 열가소성 고분자로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 용도를 제공한다.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.

또한, 본 발명은 그래핀 기반 물질을 포함하는 고분자 기반 접착제 조성물의 접착을 위한 제제의 제조를 위한 용도로서,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,

상기 고분자는 천연 고분자, 열경화성 고분자, 및 열가소성 고분자로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 용도를 제공한다.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.

이하, 본 발명의 이해를 돕기 위하여 바람직한 실시예를 제시한다. 그러나 하기의 실시예는 본 발명을 보다 쉽게 이해하기 위하여 제공되는 것일 뿐, 하기 실시예에 의해 본 발명의 내용이 한정되는 것은 아니다.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.

[실시예][Example]

실시예 1. 그래핀 기반 물질을 포함하는 고분자 접착제의 제조Example 1. Preparation of a polymer adhesive comprising a graphene-based material.

폴리우레탄(PU) 접착 용액은 수성 접착제 성분인 폴리올(LOCTITE AQUACE W-90S)에 경화제로서 아이소시아네이트(LOCTITE AQUACE ARF-50)를 100:5(폴리올:아이소시아네이트)의 부피비(v/v) 비율로 넣고 교반기를 이용하여 1,000 rpm으로 10분 동안 상온에서 교반을 진행함으로써 제조하였다.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.

그런 다음, 상기 폴리올과 아이소시아네이트가 100:5 비율로 담긴 PU 접착제에 그래파이트를 평균 4~6 μm 크기로 조각낸 그래핀 플레이크(GPX10)를 0.1 %(w/w) 또는 1 %(w/w) 넣고 교반기를 이용하여 1,000 rpm으로 10분 동안 상온에서 교반을 진행함으로써 그래핀 플레이크를 포함하는 PU 접착제를 제조하였다.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.

실시예 2. 그래핀 기반 물질을 포함하는 접착제의 적외선 가열(IR heating) 하에서의 내부 온도 변화 확인Example 2. Confirmation of internal temperature change under infrared heating (IR heating) of an adhesive containing a graphene-based material.

폴리우레탄(Polyurethane, PU) 접착제 및 1 %(w/w) 그래핀 플레이크가 함유된 PU 접착제에 적외선 가열을 가하여 시간에 따른 내부 온도 변화를 도 1a에 나타낸 바와 같이 확인하였다. 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.

그 결과, 도 1b에 나타낸 바와 같이 그래핀 플레이크를 함유하지 않는 일반적인 PU 접착제(PU)에 비해 그래핀 플레이크가 함유된 접착제(PU/G_1.0) 용액에서 더 빠르게 온도 증가가 일어남을 확인하였다. 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.

이로부터, 그래핀 플레이크 함유 접착제가 적외선 에너지를 효과적으로 흡수하고 내부 온도를 더 빨리 증가시키는 것을 알 수 있었다.From this, it was found that the graphene flake-containing adhesive effectively absorbs infrared energy and increases the internal temperature more quickly.

실시예 3. 그래핀 플레이크 함유량에 따른 PU 접착제 필름의 인장강도 변화 확인Example 3. Confirmation of changes in tensile strength of PU adhesive film according to graphene flake content.

PU 용액에 각각 0.1 %, 1.0 % 그래핀 플레이크를 혼합한 후 일정 시간 동안 적외선 히터를 이용하여 65.5 ℃ 내에서 도 2a에 나타낸 바와 같이 필름을 성형하였다. 그런 다음 각각의 필름을 대상으로 만능재료 시험기(Z010 TN)를 이용하여 인장강도를 측정한 후 평균값을 계산하였다. 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.

그 결과, PU 용액 내에 그래핀 함량이 증가할수록 외부 적외선 에너지를 더 많이 흡수하여 이를 열에너지로 방출함으로써 이 열에 의해 PU 용액 내부의 수분이 더 많이 증발되어 접착제의 경화가 더 효과적으로 이루어지며, 도 2b에 나타낸 바와 같이 그래핀 함량이 증가할수록 PU 접착제 필름의 인장강도가 증가하는 것을 확인하였다.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.

실시예 4. 그래핀 기반 물질을 포함하는 접착제를 이용한 다양한 물질 간의 접착력 확인(필링 테스트)Example 4. Confirmation of adhesion between various materials using an adhesive containing graphene-based materials (peeling test)

폴리우레탄(PU)과 고무(rubber)(PU_Rubber), 에틸렌 비닐 아세테이트(Ethylene vinyl acetate, EVA)와 열가소성 폴리우레탄(Thermoplastic polyurethane, TPU)(EVA_TPU), EVA와 고무(EVA_Rubber)를 접착시키기 위해, 이들의 표면에 각각 일반적인 PU기반 접착제(PU)와 그래핀 플레이크가 1 %(w/w) 함유된 PU 접착제(PU/G_1.0)를 브러쉬를 통해 골고루 펴 바른 후, 접착제가 접착될 수 있도록 2 kg 무게를 갖는 추를 이용해 1분간 압력을 가하였다. 그런 다음, IR 오븐(Toshiba Speedy Convection)의 열원 위쪽으로 65.5 ℃의 온도로 20분 건조 후 자연 건조를 24시간 진행하였다. 그리고 나서 도 3a에 나타낸 바와 같이 필링 테스트를 수행하여 평균값을 계산하였다. 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.

그 결과, 도 3b에 나타낸 바와 같이 그래핀 플레이크가 함유된 접착제의 접착력이 일반적인 PU 기반 접착제에 비해 우수한 것을 확인하였다.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.

　　

전술한 본 발명의 설명은 예시를 위한 것이며, 본 발명이 속하는 기술분야의 통상의 지식을 가진 자는 본 발명의 기술적 사상이나 필수적인 특징을 변경하지 않고서 다른 구체적인 형태로 쉽게 변형이 가능하다는 것을 이해할 수 있을 것이다. 그러므로 이상에서 기술한 실시예들은 모든 면에서 예시적인 것이며 한정적이 아닌 것으로 이해해야 한다.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.

본 발명에 따른 고분자 기반 접착제 조성물은 기존 고분자 기반 접착제에 비해 내부 온도가 더 빨리 증가하여 경화 시간이 단축되고 인장강도가 증가하여 접착력이 향상되는 효과를 가져 기존 고분자 기반 접착제에 비해 효율적으로 사용이 가능한 바, 산업상 이용가능성이 있다. 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 (16)

그래핀 기반 물질을 포함하는 고분자 기반 접착제 조성물로서,A polymer-based adhesive composition comprising a graphene-based material, 상기 고분자는 천연 고분자, 열경화성 고분자, 및 열가소성 고분자로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 접착제 조성물.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. 제1항에 있어서,In the first paragraph, 상기 천연 고분자는 전분(Starch), 셀룰로오스(Cellulose), 탄닌(Tannin), 아라비아 고무(Gum Arabic), 및 알긴산 나트륨(Sodium Alginate)으로 이루어진 군으로부터 선택된 하나 이상의 식물성 고분자 또는 뼈 아교(Bone Glue), 생선 젤라틴(Fish Gelatin), 혈액 단백질(Blood Protein), 카제인(Casein), 및 셸락(Shellac)으로 이루어진 군으로부터 선택된 하나 이상의 동물성 고분자인 것을 특징으로 하는, 접착제 조성물.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. 제1항에 있어서,In the first paragraph, 상기 열경화성 고분자는 에폭시(Epoxy), 페놀 수지(Phenol Formaldehyde Resin), 불포화 폴리에스터(Unsaturated Polyester), 폴리우레탄(Polyurethane, PU), 실리콘(Silicone), 폴리이미드(Polyimide), 비스말레이미드(Bismaleimide), 알릴 수지(Allyl Resin), 푸란 수지(Furan Resin), 아미노 수지(Amino Resin), 및 알키드 수지(Alkyd Resin)로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 접착제 조성물.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. 제1항에 있어서,In the first paragraph, 상기 열가소성 고분자는 폴리에틸렌(Polyethylene, PE), 폴리프로필렌(Polypropylene, PP), 폴리염화비닐(Polyvinyl Chloride, PVC), 폴리스티렌(Polystyrene, PS), 아크릴 수지(Acrylic Resin), 나일론(Nylon), 폴리카보네이트(Polycarbonate, PC), 폴리옥시메틸렌(Polyoxymethylene, POM), 열가소성 폴리에스터(Thermoplastic Polyester), 폴리페닐렌 에테르(Polyphenylene Ether, PPE), 불소수지(Fluoropolymer), 폴리페닐렌 설파이드(Polyphenylene Sulfide, PPS), 폴리설폰(Polysulfone, PSU), 폴리케톤(Polyketone), 폴리페닐 에스테르(Polyphenyl Ester), 및 액정 폴리머(Liquid Crystal Polymer, LCP)로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 접착제 조성물.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). 제1항에 있어서,In the first paragraph, 상기 그래핀 기반 물질은 그래핀, 그래파이트, 나노/마이크로 그래파이트, 산화그래핀, 환원된 산화그래핀, 그래핀양자점, 환원된 그래핀 양자점, 탄소나노튜브, 카본블랙, 및 카본 닷으로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 접착제 조성물.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. 제5항에 있어서,In paragraph 5, 상기 그래핀 기반 물질은 그래핀 또는 그래파이트이고, 1 nm 내지 1 mm의 입자 크기를 가지는 것을 특징으로 하는, 접착제 조성물.An adhesive composition, wherein the graphene-based material is graphene or graphite and has a particle size of 1 nm to 1 mm. 제1항에 있어서,In the first paragraph, 상기 접착제 조성물은 고분자 기반 접착제에 그래핀 기반 물질이 추가된 것으로서, 상기 그래핀 기반 물질은 고분자 기반 접착제 대비 0.1 내지 5 %(w/w)로 포함되는 것을 특징으로 하는, 접착제 조성물.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. 제1항에 있어서,In the first paragraph, 상기 접착제 조성물은 면, 린넨, 실크, 울, 및 모피로 이루어진 군으로부터 선택된 하나 이상의 천연 고분자;The adhesive composition comprises at least one natural polymer selected from the group consisting of cotton, linen, silk, wool, and fur; 폴리에스터(Polyester), 나일론(Nylon), 레이온(Rayon), 아크릴(Acrylic), 폴리우레탄(Polyurethane, PU), 고무(rubber), 에틸렌 비닐 아세테이트(Ethylene vinyl acetate, EVA), 및 열가소성 폴리우레탄(Thermoplastic polyurethane, TPU)으로 이루어진 군으로부터 선택된 하나 이상의 합성 고분자; 및One 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 폴리에틸렌(Polyethylene, PE), 폴리프로필렌(Polypropylene, PP), 폴리스티렌(Polystyrene, PS), ABS 수지(Acrylonitrile Butadiene Styrene, ABS), 폴리염화비닐(Polyvinyl Chloride, PVC), 폴리아세탈(Polyoxymethylene, POM), 폴리테트라플루오로에틸렌(Polytetrafluoroethylene, PTFE), 페놀 수지(Phenol Formaldehyde Resin, PF), 및 에폭시 수지(Epoxy Resin, EP)로 이루어진 군으로부터 선택된 하나 이상의 플라스틱으로 이루어진 군으로부터 선택된 하나 이상을 접착시키는 것을 특징으로 하는, 접착제 조성물.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). 제1항에 있어서,In the first paragraph, 상기 접착제 조성물의 제형은 액상(liquid), 페이스트(paste), 필름(film), 고체(solid), 및 겔(gel)로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 접착제 조성물.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. 제1항에 있어서,In the first paragraph, 상기 접착제 조성물은 적외선(Infrared light), 마이크로파(microwave), 및 무선 주파수(radio frequency)로 이루어진 군으로부터 선택된 하나 이상의 외부에너지로 가열 또는 경화되는 것을 특징으로 하는, 접착제 조성물.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. 제1항에 있어서,In the first paragraph, 상기 그래핀 기반 물질은 적외선(Infrared light), 마이크로파(microwave), 및 무선 주파수(radio frequency)로 이루어진 군으로부터 선택된 하나 이상의 외부에너지를 흡수하여 열에너지로 방출하는 것을 특징으로 하는, 접착제 조성물.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. 고분자 기반 접착제에 그래핀 기반 물질을 첨가하는 단계를 포함하는, 제1항 내지 제11항 중 어느 한 항의 접착제 조성물의 제조 방법으로서,A method for preparing 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, 상기 고분자는 천연 고분자, 열경화성 고분자, 및 열가소성 고분자로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 제조 방법.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. 제12항에 있어서,In paragraph 12, 상기 천연 고분자는 전분(Starch), 셀룰로오스(Cellulose), 탄닌(Tannin), 아라비아 고무(Gum Arabic), 및 알긴산 나트륨(Sodium Alginate)으로 이루어진 군으로부터 선택된 하나 이상의 식물성 고분자 또는 뼈 아교(Bone Glue), 생선 젤라틴(Fish Gelatin), 혈액 단백질(Blood Protein), 카제인(Casein), 및 셸락(Shellac)으로 이루어진 군으로부터 선택된 하나 이상의 동물성 고분자인 것을 특징으로 하는, 제조 방법.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. 제12항에 있어서,In paragraph 12, 상기 열경화성 고분자는 에폭시(Epoxy), 페놀 수지(Phenol Formaldehyde Resin), 불포화 폴리에스터(Unsaturated Polyester), 폴리우레탄(Polyurethane, PU), 실리콘(Silicone), 폴리이미드(Polyimide), 비스말레이미드(Bismaleimide), 알릴 수지(Allyl Resin), 푸란 수지(Furan Resin), 아미노 수지(Amino Resin), 및 알키드 수지(Alkyd Resin)로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 제조 방법.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. 제12항에 있어서,In paragraph 12, 상기 열가소성 고분자는 폴리에틸렌(Polyethylene, PE), 폴리프로필렌(Polypropylene, PP), 폴리염화비닐(Polyvinyl Chloride, PVC), 폴리스티렌(Polystyrene, PS), 아크릴 수지(Acrylic Resin), 나일론(Nylon), 폴리카보네이트(Polycarbonate, PC), 폴리옥시메틸렌(Polyoxymethylene, POM), 열가소성 폴리에스터(Thermoplastic Polyester), 폴리페닐렌 에테르(Polyphenylene Ether, PPE), 불소수지(Fluoropolymer), 폴리페닐렌 설파이드(Polyphenylene Sulfide, PPS), 폴리설폰(Polysulfone, PSU), 폴리케톤(Polyketone), 폴리페닐 에스테르(Polyphenyl Ester), 및 액정 폴리머(Liquid Crystal Polymer, LCP)로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 제조 방법.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). 제12항에 있어서,In paragraph 12, 상기 그래핀 기반 물질은 그래핀, 그래파이트, 나노/마이크로 그래파이트, 산화그래핀, 환원된 산화그래핀, 그래핀양자점, 환원된 그래핀 양자점, 탄소나노튜브, 카본블랙, 및 카본 닷으로 이루어진 군으로부터 선택된 하나 이상인 것을 특징으로 하는, 제조 방법.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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