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CN110655872B - Halogen-free flame-retardant UV (ultraviolet) curing acrylate pressure-sensitive adhesive, pressure-sensitive adhesive tape and preparation method thereof - Google Patents

Halogen-free flame-retardant UV (ultraviolet) curing acrylate pressure-sensitive adhesive, pressure-sensitive adhesive tape and preparation method thereof Download PDF

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CN110655872B
CN110655872B CN201910931992.2A CN201910931992A CN110655872B CN 110655872 B CN110655872 B CN 110655872B CN 201910931992 A CN201910931992 A CN 201910931992A CN 110655872 B CN110655872 B CN 110655872B
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sensitive adhesive
pressure
halogen
retardant
acrylate
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CN110655872A (en
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刘星
林晓丹
廖平湘
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Hunan Province And New Material Co ltd
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    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J4/00Adhesives based on organic non-macromolecular compounds having at least one polymerisable carbon-to-carbon unsaturated bond ; adhesives, based on monomers of macromolecular compounds of groups C09J183/00 - C09J183/16
    • C09J4/06Organic non-macromolecular compounds having at least one polymerisable carbon-to-carbon unsaturated bond in combination with a macromolecular compound other than an unsaturated polymer of groups C09J159/00 - C09J187/00
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02Non-macromolecular additives
    • C09J11/04Non-macromolecular additives inorganic
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02Non-macromolecular additives
    • C09J11/06Non-macromolecular additives organic
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/08Macromolecular additives
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J7/00Adhesives in the form of films or foils
    • C09J7/20Adhesives in the form of films or foils characterised by their carriers
    • C09J7/22Plastics; Metallised plastics
    • C09J7/25Plastics; Metallised plastics based on macromolecular compounds obtained otherwise than by reactions involving only carbon-to-carbon unsaturated bonds
    • C09J7/255Polyesters
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J7/00Adhesives in the form of films or foils
    • C09J7/30Adhesives in the form of films or foils characterised by the adhesive composition
    • C09J7/38Pressure-sensitive adhesives [PSA]
    • C09J7/381Pressure-sensitive adhesives [PSA] based on macromolecular compounds obtained by reactions involving only carbon-to-carbon unsaturated bonds
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2301/00Additional features of adhesives in the form of films or foils
    • C09J2301/10Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive tape or sheet
    • C09J2301/12Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive tape or sheet by the arrangement of layers
    • C09J2301/122Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive tape or sheet by the arrangement of layers the adhesive layer being present only on one side of the carrier, e.g. single-sided adhesive tape
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2467/00Presence of polyester
    • C09J2467/006Presence of polyester in the substrate

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Inorganic Chemistry (AREA)
  • Adhesive Tapes (AREA)
  • Adhesives Or Adhesive Processes (AREA)

Abstract

The invention discloses a halogen-free flame-retardant UV (ultraviolet) curing acrylate pressure-sensitive adhesive, a pressure-sensitive adhesive tape and a preparation method thereof, wherein the halogen-free flame-retardant UV curing acrylate pressure-sensitive adhesive comprises the following raw materials in parts by weight: 100 parts of an acrylate prepolymer; 15-20 parts of dimethyl methylphosphonate; 0.8-2 parts of silicon dioxide; 0.2-0.25 part of cross-linking agent; 2.5-3.35 parts of tackifying resin; 0.5-1 part of second photoinitiator. The pressure-sensitive adhesive tape formed by the halogen-free flame-retardant UV-cured acrylate pressure-sensitive adhesive has the advantages of good flame-retardant effect, excellent pressure-sensitive adhesive performance and wide application range.

Description

Halogen-free flame-retardant UV (ultraviolet) curing acrylate pressure-sensitive adhesive, pressure-sensitive adhesive tape and preparation method thereof
Technical Field
The invention relates to the technical field of ultraviolet curing pressure-sensitive adhesives, in particular to a halogen-free flame-retardant UV curing acrylate pressure-sensitive adhesive, a pressure-sensitive adhesive tape and a preparation method thereof.
Background
The acrylate pressure-sensitive adhesive is a material with viscoelastic property, has good wettability to the surfaces of various base materials, does not contain unsaturated double bonds, and has excellent aging resistance. And after the adhesive tape is stripped, no adhesive residue is left on the surface of the base material. The composite material is widely used in the industries of packaging, automobiles, electronic communication, medicine, construction, personal care and the like. As a third generation acrylate pressure-sensitive adhesive, the UV curing acrylate pressure-sensitive adhesive has the unique characteristics that: no solvent, low energy consumption, little pollution, easy reaction control, simple equipment and the like, and is rapidly developed under the advocation of energy conservation and environmental protection in recent years.
With the expansion of the application range, the requirements on the acrylate pressure-sensitive adhesive are gradually increased. The acrylate pressure-sensitive adhesive is a flammable polymer consisting of three elements of carbon, hydrogen and oxygen, and is greatly limited in application in the fields of automobiles, aerospace and the like. And the flame-retardant acrylate pressure-sensitive adhesive sold on the market at present mainly adopts a halogen flame retardant, so that the flame-retardant acrylate pressure-sensitive adhesive is difficult to be used in the fields of electronic communication and the like.
Patent document CN108003818A discloses a heat-conducting low-halogen flame-retardant pressure-sensitive adhesive and a preparation method thereof. Acrylic monomers, acrylate monomers and organic peroxide initiators are heated, mixed and polymerized to obtain the polyacrylate adhesive, and then the polyacrylate adhesive is stirred and mixed with heat-conducting fillers and flame-retardant substances to obtain the pressure-sensitive adhesive which has good heat-conducting capacity and excellent flame-retardant performance. But the use of organic solvent causes pollution to the environment; the addition amount of the heat-conducting filler and the flame retardant substance is too much, and the light transmittance, initial adhesion, peeling strength and coating performance of the pressure-sensitive adhesive are seriously reduced.
Patent document CN101805567A discloses a preparation method of a phosphorus-combined flame-retardant acrylate pressure-sensitive adhesive. Mixing acrylate monomers and phosphorus-containing monomers, adding an initiator for heating reaction to obtain the combined phosphorus-type flame-retardant pressure-sensitive adhesive, and then adding the flame-retardant slurry for uniform mixing to improve the flame-retardant property of the adhesive. Although the pressure-sensitive adhesive has good base material adhesion, good flame retardant dispersibility and high light transmittance, the pressure-sensitive adhesive has common flame retardant performance due to low phosphorus content, and has low initial adhesion and permanent adhesion, and the pressure-sensitive adhesive contains a small amount of solvent which is difficult to volatilize.
Patent document CN103275657A discloses a peelable type flame retardant acrylate pressure sensitive adhesive. The flame retardant is prepared by uniformly mixing acrylate monomers, modified epoxy resin, a flame retardant, an initiator and a curing agent and heating for reaction, wherein the flame retardant is prepared by reacting hexachlorocyclotriphosphazene with 2-allylphenol. The adhesive has the advantages of wide raw material source, low price, easy obtainment, simple synthesis process and high reuse rate, but the acetone is used as a solvent, so the problem of environmental pollution exists, and the flame retardant has more rigid groups, so the initial adhesion is reduced.
Patent document CN102719206A discloses a preparation method of halogen-free environment-friendly flame-retardant acrylate pressure-sensitive adhesive. The method comprises the steps of firstly reacting hexachlorocyclotriphosphazene with an alcohol monomer to prepare a phosphorus-containing flame retardant, and then mixing and reacting the phosphorus-containing flame retardant with a soft monomer, a hard monomer, an initiator and a crosslinking agent in a certain proportion to finally obtain the target pressure-sensitive adhesive. The initial decomposition temperature after curing is increased from 150 ℃ in the prior art to 200 ℃, the carbon residue rate at 600 ℃ is increased from 0% in the prior art to about 21%, and the thermal stability and the carbon forming effect are good. But the compatibility of the flame retardant and the pressure-sensitive adhesive is poor, and the rigid group of the flame retardant is too large, so that the permanent adhesion and the initial adhesion of the pressure-sensitive adhesive are small. And harmful solvents may remain in the system.
In conclusion, the existing flame-retardant acrylate pressure-sensitive adhesive has the following main problems: although the pressure-sensitive adhesive containing the halogen flame retardant has high flame retardant grade, the application range of the pressure-sensitive adhesive is greatly limited; the halogen-free additive flame retardant has poor compatibility with the pressure-sensitive adhesive, and can damage the cohesive force, initial adhesion and peel strength of the pressure-sensitive adhesive; although the halogen-free reaction type flame retardant can participate in the polymerization reaction of the monomers to form a copolymer, the content of phosphorus and nitrogen elements is low, and the flame retardant effect is poor.
Therefore, there is a need to develop a halogen-free flame retardant UV curable acrylate pressure-sensitive adhesive with excellent comprehensive properties while having both flame retardant effect and pressure-sensitive adhesion.
Disclosure of Invention
The invention mainly aims to provide a halogen-free flame-retardant UV-cured acrylate pressure-sensitive adhesive, a pressure-sensitive adhesive tape and a preparation method thereof.
In order to achieve the above object, according to one aspect of the present invention, there is provided a halogen-free flame retardant UV curable acrylate pressure-sensitive adhesive, which comprises the following raw materials in parts by weight:
Figure BDA0002220477390000021
according to the invention, 15-20 parts by weight of dimethyl methylphosphonate and 0.8-2 parts by weight of silicon dioxide are adopted, and the flame retardant effect of the UV curing acrylate pressure-sensitive adhesive is effectively improved under the condition of using a lower dosage of flame retardant through the synergistic flame retardant effect of the dimethyl methylphosphonate and the silicon dioxide in a specific ratio; and the crosslinking agent and the tackifying resin in a specific ratio are combined, so that the UV-cured acrylate pressure-sensitive adhesive has good flame retardance and excellent adhesive property.
The synergistic flame retardant principle is as follows: in the combustion process, phosphorus-containing groups in dimethyl methylphosphonate are firstly degraded into acidic phosphate ester or phosphite ester and the like, pressure-sensitive adhesive is promoted to dehydrate into carbon to form a carbon layer rich in phosphorus elements, and silicon dioxide is used as a protective layer of the phosphorus-rich carbon layer to prevent oxygen from invading at high temperature and maintain the stability of the carbon layer; the flame retardant property of the UV curing acrylate pressure-sensitive adhesive is greatly improved through the synergistic promotion of the two components.
Furthermore, the soft monomer in the acrylate prepolymer is 85-90 parts by weight of isooctyl acrylate, the hard monomer and the functional monomer are any one or combination of more of acrylic acid, hydroxyethyl acrylate and isobornyl acrylate in 10-15 parts by weight, the acrylate prepolymer is formed by polymerizing the soft monomer, the hard monomer and the functional monomer under the action of a first photoinitiator through ultraviolet light irradiation, and the adding amount of the first photoinitiator is 0.01-0.05 part by weight. According to the invention, the pressure-sensitive adhesive has higher curing speed and good bonding performance by adopting the acrylate prepolymer with a specific proportion and a specific type and acting with the first photoinitiator with a specific amount.
Further, the first photoinitiator and the second photoinitiator are both TPO. By comparing various photoinitiators, 184 photoinitiators are not easy to dissolve in the prepolymer and need to be slightly heated; the liquid 1173 photoinitiator has a relatively low initiation efficiency, while other photoinitiators are not as efficient and do not initiate as TPO, and do not initiate as quickly as TPO, and thus, TPO is preferred for use as the first and second photoinitiators in the present invention.
Further, the tackifying resin is any one of or a combination of two of a C5 resin and a hydrogenated rosin resin. The C5 resin has a soft and smooth structure and good fluidity, and can improve the wettability of the main material, thereby improving the bonding strength of the main material to the base material; the rosin resin has a hydrogen bond network structure, and can reduce the viscoelasticity of the pressure-sensitive adhesive after being added into the acrylate prepolymer, so that the wettability between the pressure-sensitive adhesive and an adherend is improved, and the initial adhesion, the quick-drying speed and the peel strength of the pressure-sensitive adhesive are improved; in addition, the C5 resin, the hydrogenated rosin resin and the acrylate prepolymer have good compatibility. The tackifying resin is added into the acrylate prepolymer according to a certain proportion, so that the bonding performance of the acrylate pressure-sensitive adhesive to a base material can be effectively improved.
Further, the cross-linking agent is any one or the combination of two of trimethylolpropane triacrylate and polyethylene glycol 400 diacrylate. By adopting the specific type and ratio of the cross-linking agent, and combining the cross-linking agent with the specific ratio of the acrylate prepolymer, the dimethyl methyl phosphonate, the silicon dioxide and the tackifying resin, the flame retardant property of the pressure-sensitive adhesive is improved, and meanwhile, the bonding property of the pressure-sensitive adhesive is ensured, so that the halogen-free flame retardant UV curing acrylate pressure-sensitive adhesive has excellent comprehensive properties.
Further, the viscosity of the acrylate prepolymer is 450mPa.s-600 mPa.s.
Further, the particle size of the silica is 1.5 μm to 2.5. mu.m. By adopting the silicon dioxide with the particle size range, the synergistic flame retardant effect between the silicon dioxide and dimethyl methylphosphonate is better.
According to another aspect of the invention, a preparation method of the halogen-free flame retardant UV-cured acrylate pressure-sensitive adhesive is provided, and the preparation method comprises the following steps:
(1) uniformly mixing the soft monomer, the first photoinitiator, the hard monomer and the functional monomer according to the proportion, initiating polymerization by UV illumination in a nitrogen atmosphere, and introducing oxygen to terminate the reaction when the viscosity of the system reaches 450-600 mPa.s to obtain an acrylate prepolymer;
(2) and (2) adding dimethyl methyl phosphonate and silicon dioxide into the acrylate prepolymer obtained in the step (1) according to the proportion, stirring and dissolving until the mixture is transparent, then adding a second photoinitiator, tackifying resin and a cross-linking agent, stirring and dissolving to obtain the acrylate pressure-sensitive adhesive.
The preparation method has the advantages of simple operation, low energy consumption, low cost and little environmental pollution.
According to still another aspect of the present invention, there is provided a halogen-free flame retardant UV curable acrylate pressure sensitive adhesive tape, which is obtained by coating the above halogen-free flame retardant UV curable acrylate pressure sensitive adhesive or the acrylate pressure sensitive adhesive obtained by the above preparation method on a polyester film, then covering with a release film to exclude oxygen, and curing under a UV lamp.
Furthermore, the halogen-free flame-retardant UV-cured acrylate pressure-sensitive adhesive tape has the flame retardant grade reaching V-0, the peel strength being more than 8.6N/25mm, good flame retardant property and excellent adhesive property.
Compared with the prior art, the invention has the beneficial effects that: adopts flame retardants of dimethyl methylphosphonate (DMMP) and SiO2Matched with each other by dimethyl methylphosphonate and SiO under the condition of specific proportioning dosage2The synergistic effect between the two components obviously improves the flame retardant grade of the acrylate pressure-sensitive adhesive; by adopting the specific cross-linking agent and the tackifying resin and adjusting the dosage of the cross-linking agent and the tackifying resin, the pressure-sensitive adhesive has excellent adhesive property and controllable mechanical property; the halogen-free flame-retardant UV curing pressure-sensitive adhesive has near zero volatile components and small environmental pollution; the preparation method has the advantages of simple operation, low energy consumption and low cost.
Detailed Description
In order to facilitate an understanding of the present invention, the present invention will be described more fully and in detail with reference to the preferred embodiments, but the scope of the present invention is not limited to the specific embodiments described below.
Unless otherwise defined, all terms of art used hereinafter have the same meaning as commonly understood by one of ordinary skill in the art. The terminology used herein is for the purpose of describing particular embodiments only and is not intended to limit the scope of the present invention.
Unless otherwise specifically stated, various raw materials, reagents, instruments, equipment and the like used in the present invention are commercially available or can be prepared by existing methods.
Example 1:
the preparation method of the halogen-free flame-retardant UV-cured acrylate pressure-sensitive adhesive and the pressure-sensitive adhesive tape comprises the following steps:
(1) preparation of acrylate prepolymer
Uniformly mixing 85 parts by weight of isooctyl acrylate, 5 parts by weight of acrylic acid, 10 parts by weight of isobornyl acrylate and 0.05 part by weight of a first photoinitiator (TPO, 2,4, 6-trimethylbenzoyl-diphenyl phosphine oxide), performing polymerization reaction under the condition of UV illumination in a nitrogen atmosphere, and introducing oxygen to terminate the reaction when the viscosity of a system reaches 450-600 mPa.s to obtain an acrylate prepolymer;
(2) preparation of pressure-sensitive adhesive liquid
Adding 15 parts by weight of dimethyl methyl phosphonate (DMMP) serving as a flame retardant and 2 parts by weight of silicon dioxide into the prepared acrylate prepolymer, fully stirring until the dimethyl methyl phosphonate and the silicon dioxide are completely dissolved, and then adding 1 part by weight of a second photoinitiator (TPO), 3.35 parts by weight of hydrogenated rosin resin and 0.25 part by weight of a cross-linking agent TMPTA (trimethylolpropane triacrylate) into the obtained solution, continuously stirring and dissolving to obtain viscous and light yellow acrylate pressure-sensitive adhesive liquid, and standing for later use;
(3) coating film
Coating the acrylate pressure-sensitive adhesive solution obtained in the step (2) on a polyester film, wherein the coating thickness is 100 mu m, then covering a release film to isolate oxygen, and curing for 360s under a UV lamp (the illumination energy is 100 mJ/cm)2-150 mJ/cm2) And obtaining the halogen-free flame-retardant UV curing acrylate pressure sensitive adhesive tape.
Performance testing
The pressure-sensitive adhesive tape sample obtained after the coating in the embodiment is cured is cut and stored, the 180-degree peel strength of the adhesive tape is tested on an electronic tensile machine according to the GB/T2792-2014 standard, and the flame retardant grade of the adhesive tape is tested on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Example 2:
this example was prepared in much the same manner as example 1 except that dimethyl methylphosphonate and silica were used in different amounts than in example 1. In this example, dimethyl methylphosphonate was used in an amount of 20 parts by weight and silica was used in an amount of 1 part by weight.
The pressure-sensitive adhesive tape sample obtained after the coating in the embodiment is cured is cut and stored, the 180-degree peel strength of the adhesive tape is tested on an electronic tensile machine according to the GB/T2792-2014 standard, and the flame retardant grade of the adhesive tape is tested on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Example 3:
the preparation process of this example is essentially the same as that of example 1, with the main difference that 20 parts by weight of dimethyl methylphosphonate and 0.8 part by weight of silica are used as flame retardant.
The pressure-sensitive adhesive tape sample obtained after the coating in the embodiment is cured is cut and stored, the 180-degree peel strength of the adhesive tape is tested on an electronic tensile machine according to the GB/T2792-2014 standard, and the flame retardant grade of the adhesive tape is tested on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 1:
the comparative example was prepared in substantially the same manner as in example 1, with the main difference that the flame retardant used only 20 parts by weight of dimethyl methylphosphonate and no silica was added.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 2:
the comparative example was prepared in substantially the same manner as example 1, with the main difference that the flame retardant used was only 15 parts by weight of dimethyl methylphosphonate, and no silica was added.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 3:
the comparative example was prepared in substantially the same manner as in example 1, with the main difference that the flame retardant used was only 21 parts by weight of dimethyl methylphosphonate, and no silica was added.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 4:
the comparative example was prepared in substantially the same manner as example 1, with the main difference that the flame retardant used only 17 parts by weight of dimethyl methylphosphonate and no silica was added.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 5:
the comparative example was prepared in substantially the same manner as in example 1, with the main difference that 10 parts by weight of dimethyl methylphosphonate and 2 parts by weight of silica were used as the flame retardant.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 6:
the comparative example was prepared in substantially the same manner as in example 1, with the main difference that 15 parts by weight of dimethyl methylphosphonate and 3 parts by weight of silica were used as the flame retardant.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 7:
the comparative example was prepared in substantially the same manner as example 1, with the main difference that 25 parts by weight of dimethyl methylphosphonate and 1 part by weight of silica were used as the flame retardant.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 8:
this comparative example was prepared in substantially the same manner as in example 1, except that 0.2 parts by weight of the crosslinking agent and 2.5 parts by weight of the hydrogenated rosin resin were used.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 9:
this comparative example was prepared in substantially the same manner as in example 1, except that 0.3 parts by weight of the crosslinking agent and 4.0 parts by weight of the hydrogenated rosin resin were used.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 10:
this comparative example was prepared in substantially the same manner as in example 2, except that 0.2 parts by weight of a crosslinking agent and 2.5 parts by weight of a hydrogenated rosin resin were used.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 11:
this comparative example was prepared in substantially the same manner as in example 2, except that 0.3 parts by weight of the crosslinking agent and 4.0 parts by weight of the hydrogenated rosin resin were used.
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 12:
the comparative example was prepared in substantially the same manner as example 1, with the main difference that the flame retardant was changed from dimethyl methylphosphonate to triphenyl phosphate (TPP).
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 13:
the comparative example was prepared in substantially the same manner as example 1, with the main difference that the flame retardant was replaced by dimethyl methylphosphonate to melamine polyphosphate (MPP).
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 14:
the comparative example was prepared in substantially the same manner as example 2, with the main difference that the flame retardant was changed from dimethyl methylphosphonate to triphenyl phosphate (TPP).
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
Comparative example 15:
the comparative example was prepared in substantially the same manner as example 2, with the main difference that the flame retardant was replaced by dimethyl methylphosphonate to melamine polyphosphate (MPP).
And (3) cutting and storing the pressure-sensitive adhesive tape sample obtained after the coating film is cured in the comparative example, testing the 180-degree peel strength of the adhesive tape on an electronic tensile machine according to the GB/T2792-2014 standard, and testing the flame retardant grade of the adhesive tape on a horizontal vertical combustion instrument according to the UL94-2006 standard. The test results are shown in table 1.
TABLE 1 formulation (wt%) and peel strength and flame retardant rating of halogen-free flame retardant UV-cured pressure sensitive adhesive for each example and comparative example
Figure BDA0002220477390000081
Figure BDA0002220477390000091
As can be seen from Table 1, SiO2The acrylate pressure-sensitive adhesive is added into a flame retardant DMMP for complex use, can generate a synergistic effect, and obviously improves the flame retardant grade of the acrylate pressure-sensitive adhesive; in addition, the crosslinking agent and the tackifying resin are added in an appropriate amount so that the pressure-sensitive adhesive can achieve the proper peel strength. And flame retardants TPP, MPP and SiO2No obvious synergistic effect exists, and even if the proportion of the two is changed, the flame-retardant acrylate pressure-sensitive adhesive cannot be prepared.
As is clear from examples 1 to 3, the peel strengths thereof all exceeded 8.6N/25mm, and the flame retardant ratings all reached V-0, and the practical use was satisfied.
From comparative examples 1 to 4, it can be seen that the flame retardant effect can be significantly improved by increasing the amount of the flame retardant DMMP under the condition that other factors are fixed and unchanged. However, at the same time, because the molecular weight of the DMMP is low and the DMMP has more methyl flexible groups, the DMMP has strong plasticizing effect on the pressure-sensitive adhesive, and the cohesive strength of the pressure-sensitive adhesive is damaged, so that the stripping performance of the pressure-sensitive adhesive is reduced, and the adhesive performance of the pressure-sensitive adhesive is reduced. And when the increase amount of DMMP is less than 17 parts by mass, no flame retarding effect will be produced.
Examples 1 to 3 and comparative examples 1 to 4 were carried outBy comparison, it was found that a small amount of SiO was added2Can improve the flame retardant grade of the pressure sensitive adhesive, and SiO2The flame-retardant adhesive has no flame-retardant effect, so that the flame-retardant adhesive and the DMMP generate a remarkable synergistic effect, in the combustion process, phosphorus-containing groups in the DMMP are firstly degraded into acidic phosphate ester or phosphite ester and the like, the pressure-sensitive adhesive is promoted to dehydrate into carbon to form a carbon layer rich in phosphorus elements, and the silicon dioxide is used as a protective layer of the phosphorus-rich carbon layer to prevent oxygen from invading at high temperature and maintain the stability of the carbon layer. Thereby the two are synergistically promoted, and the flame retardant property of the pressure-sensitive adhesive is improved.
Comparing examples 1 to 3 with comparative examples 5 to 7, it is understood that only when DMMP is used in an amount of 15 parts by mass, it is possible to compare with SiO2A synergistic effect is formed because a sufficient amount of phosphorus element is required for the synergistic effect to occur. When the phosphorus content is low, it is difficult to form a phosphorus catalytic carbon layer in a wide range, so that volatilization of combustible gas, heat transfer and oxygen invasion cannot be effectively prevented, and diffusion and aggravation of combustion are caused. And found SiO2The addition amount in the pressure-sensitive adhesive can not exceed 2 parts by mass, and although the flame retardant effect is still good, the peel strength is greatly reduced, so that the application value of the pressure-sensitive adhesive is lost. When SiO is present2When the dosage is slightly reduced, the flame retardant effect is not obviously reduced, and the peeling strength can be properly increased.
Comparing examples 1 to 3 with comparative examples 8 to 11, it was found that changing the addition amounts of the crosslinking agent and the hydrogenated rosin resin with a fixed amount of the flame retardant had an effect only on the peel strength of the pressure-sensitive adhesive. The cross-linking agent and the hydrogenated rosin resin are substances only containing three elements of carbon, hydrogen and oxygen, and even if the dosage of the cross-linking agent and the hydrogenated rosin resin in the pressure-sensitive adhesive is adjusted, the cross-linking agent and the hydrogenated rosin resin cannot generate a synergistic effect with DMMP, so that the flame retardant effect is influenced. It was found that the amount of the crosslinking agent and the hydrogenated rosin resin is present at a suitable value, and when deviating from this value, a different degree of reduction in the peel strength of the pressure-sensitive adhesive results.
Comparing examples 1 to 3 with comparative examples 12 to 15, it was found that, in the case where the flame retardant DMMP was changed to TPP or MPP, even though the flame retardant rating was changed, the peel strength was changed. Because the phosphorus contents of the flame retardant TPP and MPP are farThe phosphorus content is lower than that of DMMP, and the flame-retardant acrylate pressure-sensitive adhesive is difficult to prepare; even if SiO is added2And adjusting the flame retardant and SiO2The proportion of (a) does not produce an effective synergistic effect, cannot form a sufficient carbon layer structure, and cannot remarkably improve the flame retardant effect. However, TPP and MPP both have cyclic rigid groups, and can weaken the impact of plasticization on the cohesive strength of the pressure-sensitive adhesive, so that the peel strength of the pressure-sensitive adhesive is kept at a higher level.
In conclusion, the invention adds the specific high-efficiency flame retardant DMMP and the inorganic oxide SiO2And the proportion of the acrylic acid ester pressure-sensitive adhesive is adjusted, and the two can generate obvious synergistic effect to improve the flame retardant grade. Meanwhile, proper amounts of cross-linking agent and tackifying resin are added, so that the peel strength of the pressure-sensitive adhesive reaches a proper value.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (9)

1. The halogen-free flame-retardant UV-cured acrylate pressure-sensitive adhesive is characterized by comprising the following raw materials in parts by weight:
100 parts of an acrylate prepolymer;
15-20 parts of dimethyl methylphosphonate;
0.8-2 parts of silicon dioxide;
0.25 part of a crosslinking agent;
3.35 parts of tackifying resin;
0.5-1 part of a second photoinitiator;
the cross-linking agent is trimethylolpropane triacrylate.
2. The halogen-free flame-retardant UV-curable acrylate pressure-sensitive adhesive according to claim 1, wherein the soft monomer in the acrylate prepolymer is 85-90 parts by weight of isooctyl acrylate, the hard monomer and the functional monomer are 10-15 parts by weight of any one or a combination of acrylic acid, hydroxyethyl acrylate and isobornyl acrylate, the acrylate prepolymer is formed by polymerizing the soft monomer, the hard monomer and the functional monomer under the action of a first photoinitiator through ultraviolet light irradiation, and the addition amount of the first photoinitiator is 0.01-0.05 part by weight.
3. The halogen-free flame retardant UV-curable acrylate pressure-sensitive adhesive according to claim 2, wherein the first photoinitiator and the second photoinitiator are both TPO.
4. The halogen-free flame retardant UV-curable acrylate pressure-sensitive adhesive according to claim 1, wherein the tackifying resin is any one or a combination of two of C5 resin and hydrogenated rosin resin.
5. The halogen-free flame-retardant UV-curable acrylate pressure-sensitive adhesive according to claim 1, wherein the viscosity of the acrylate prepolymer is 450mPa.s-600 mPa.s.
6. The halogen-free flame retardant UV-curable acrylate pressure-sensitive adhesive according to claim 1, wherein the particle size of the silica is 1.5 μm to 2.5 μm.
7. The preparation method of the halogen-free flame retardant UV-cured acrylate pressure-sensitive adhesive according to any one of claims 2 to 6, characterized by comprising the following steps:
(1) uniformly mixing the soft monomer, the first photoinitiator, the hard monomer and the functional monomer according to the proportion, initiating polymerization by UV illumination in a nitrogen atmosphere, and introducing oxygen to terminate the reaction when the viscosity of the system reaches 450-600 mPa.s to obtain an acrylate prepolymer;
(2) and (2) adding dimethyl methyl phosphonate and silicon dioxide into the acrylate prepolymer obtained in the step (1) according to the proportion, stirring and dissolving until the mixture is transparent, then adding a second photoinitiator, tackifying resin and a cross-linking agent, stirring and dissolving to obtain the acrylate pressure-sensitive adhesive.
8. A halogen-free flame-retardant UV-curable acrylate pressure-sensitive adhesive tape is characterized in that the halogen-free flame-retardant UV-curable acrylate pressure-sensitive adhesive tape is prepared by coating the halogen-free flame-retardant UV-curable acrylate pressure-sensitive adhesive according to any one of claims 2 to 6 or the acrylate pressure-sensitive adhesive obtained by the preparation method according to claim 7 on a polyester film, covering the polyester film with a release film to isolate oxygen, and curing the polyester film under a UV lamp.
9. The halogen-free flame retardant UV-curable acrylate pressure sensitive adhesive tape according to claim 8, wherein the halogen-free flame retardant UV-curable acrylate pressure sensitive adhesive tape has a flame retardant rating of V-0 and a peel strength of more than 8.6N/25 mm.
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CN113528030B (en) * 2020-04-17 2022-04-22 华南理工大学 A kind of flame retardant UV light curing acrylate pressure sensitive adhesive and its preparation method and application
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CN114196369A (en) * 2021-12-27 2022-03-18 东莞市阿普帮新材料科技有限公司 Environment-friendly flame-retardant low-sensitization ultraviolet curing adhesive and preparation method thereof
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CN115260948B (en) * 2022-08-30 2023-11-07 东莞澳中新材料科技股份有限公司 Flame-retardant UV (ultraviolet) curing adhesive and preparation method and application thereof
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