DE2530726A1 - Polyolefins grafted with polar monomers as hot melt adhesives - for bonding polar or non polar surfaces - Google Patents

Abstract

The use is claimed of olefin copolymers comprising a graft copolymer contg. >0.1 and 100 wt.% (on satd. hydrocarbon chain) of grafted polar monomers, as hot melt adhesives. The polymers have good adhesion to a wide range of polar and non-polar substrates, have good hot and cold adhesive strength, and low cold flow. The adhesives can be used for packaging, in the prodn. of composite laminated foils of (e.g.) metal foil, paper, polyolefin film, corrugated paper etc.; for sealing cartons; for applying edging strips to chipboard panels; for making air- and petrol filters and for applying road markings. In an example, aluminium sheet was coated with low pressure polyethylene film using a hot melt adhesive comprising a low press. polyethylene grafted with 0.6% acrylic acid.

Description

The invention relates to the use of grafted olefin copolymers as hot-melt adhesive compositions.

Hot melt adhesives based on olefin copolymers, preferably those based on ethylene-vinyl acetate and Ethylene-acrylate copolymers have been known for a long time. These copolymers are predominantly true copolymers with a statistical arrangement of the monomeric reactants in the chain molecules formed. Furthermore are Graft copolymers based on ethylene and vinyl acetate have become known, based on the monomer mixtures of vinyl esters Carboxylic acids, esters νοηΛ-, ß- unsaturated carboxylic acids with Alcohols and other olefinically unsaturated copolymerizable monomers are grafted on. Such graft copolymers are described in DT-OS 2 253 245 and are used exclusively as pressure-sensitive adhesives for self-adhesive labels, signs, tapes and foils recommended. You therefore only have a limited area of application.

Atactic polypropylene is also used for some specific applications (AP?) Used as a hot melt adhesive base.

Hot melt adhesives on the basis described above, but also on other bases, such as polyester resins, polyamides a number of disadvantages, so that their use in various areas of application is often still problematic in terms of adhesive technology. In many cases, the adhesive properties of these hot melt adhesives are not sufficient on many substrates to create solid adhesive bonds but also to achieve satisfactory heat and cold strengths.

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The "cold flow" is also one of these hot melt adhesives very negative appearance.

The biggest problem in the adhesive technology of hot melt adhesives is that with them non-polar surfaces can not be glued to one another or to other substrates, if not beforehand the non-polar surfaces through very complex and costly process manipulations, e.g. through corona discharges, "to be activated. Non-"activated" or non-pretreated non-polar surfaces, e.g. polyethylene, polypropylene, deliver more or less only a very weak "contact adhesion" with hot melt adhesives, which can be done without the use of force can be solved by hand.

Furthermore, hotmelt adhesives based on such copolymers are not always absolutely resistant to grease or alcohol and not boil-proof or sterilization-proof. For this reason, hot-melt adhesives, for example, are still used today in the packaging sector has not yet found its way, although it is precisely this adhesive technology with hot melt adhesives that is widely used in this sector of economic and technical advantages.

But the economic side also plays an important role when using such hot melt adhesives. This is because the copolymers described at the outset are relatively expensive and as the comonomer content of vinyl acetate or acrylate increases, so do the purchase prices. In the case of the grafted ethylene-vinyl acetate copolymers, relatively laborious and costly manufacturing manipulations are necessary, which makes the products more expensive.

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It has now surprisingly been found that, in order to achieve high-quality bonds and adhesive bonds, by means of hot-melt adhesive masses Much simpler means, i.e. more economical base copolymers, are also sufficient to achieve the above and other known disadvantages.

The object of the invention is now to provide new grafted olefin copolymers, alone or in combination with other arbitrary olefin copolymers, adhesive resins, waxes, plasticizers and / or fillers can be used as hot melt adhesive masses. According to the current status and according to the knowledge in adhesive chemistry was not to be expected that such grafted olefin copolymers, which consist of an olefinic main molecular chain and Grafted polar side chains exist, alone or in mixtures with other additives as a hot melt adhesive masses can be used. These new grafted olefin copolymers can be used, among other things, by methods as described in DT-OS 1 932 739 and DT-OS 1 932 797, produce in a very economical way with specific comonomer contents. On the manufacture of such grafted No protection is claimed for olefin copolymers.

The starting materials for obtaining such grafted olefin copolymers polyolefins can be of any type. These polyolefins can be produced by various processes, such as high pressure processes, coordination catalysis, radical polymerization in solution, etc.

Examples of polyolefins include:

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High pressure polyethylene

Low pressure polyethylene according to ZIEGLER

isotactic low-pressure polypropylene according to NATTA - ZIEGLER

isotactic polybutene-1 stereoregular poly-4-methyl-pentene-1

The polymerizable monomers that can be used for grafting are unsaturated organic compounds that contain a double bond that can be activated by free radicals. These monomers can belong to a wide variety of chemical substance classes. These include, for example, carboxylic and sulfonic acids, esters, Amides, aromatic compounds, halides, amines, nitriles, ethers, thioethers, ketones etc.

The unsaturated carboxylic acids include, for example, mono- and dicarboxylic acids, such as acrylic acid, methacrylic acid, 1,2-dichloroachrylic acid, Undecylenic acid, maleic acid, itaconic acid, and the like.

Unsaturated esters include the esters of the above acids, in particular the alkyl esters of acrylic and methacrylic acid, such as polyalkylene glycol acrylates, e.g. tetraethylene glycol dimethacrylate, Dimethylaminoethyl methacrylate, 2-hydroxyethyl methacrylate, glycidyl methacrylate, are suitable. Another group of esters includes unsaturated esters in which the double bonds are on the esterifying group, e.g. Vinyl acetate, vinyl benzoate.

Examples of the unsaturated amides are amides of unsaturated ones Carboxylic acids such as acrylamides, methacrylamides, N-phenylacetamides.

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The aromatic compounds include those that contain a vinyl group that is linked to a carbocyclic, mono- or polycyclic or heterocyclic group is connected, which can also be substituted. Examples are styrene, p-chlorostyrene, p-dimethylaminostyrene, vinylpyridines, 2-vinylcarbazole, Vinyl pyrrolidone.

Monomers that belong to the other classes of substances not yet mentioned can include the following:

unsaturated amines such as N-alkyl-N-aryl amines, e.g. N-phenyl-vinylamine,

N, N-dialkyl-vinylamine, e.g. N, N-diethylvinylamine,

Alkyl vinyl or aryl vinyl ethers or thioethers, e.g. Benzyl vinyl ether, ethyl vinyl thioether,

Vinyl or vinylidene halides, e.g. vinyl chloride, vinylidene chloride,

Vinyl nitriles, e.g. acrylonitrile, vinyl sulfonic acids,

organically unsaturated derivatives of silicon such as vinyl silanes, e.g. vinyl trialkyl and vinyl trialkoxysilanes.

The amount of reacting monomers depends on many factors, in particular on the physical form of the polyolefin « This amount can, for example, between 0.1 to 100 percent by weight, based on the polyolefin, vary. However, it is preferably between 0.1 and 50 percent by weight.

In the case of polyolefins, according to the invention, low and medium molecular weight Polyethylene and polypropylene are used, but high molecular weight olefins can also be used.

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For use as a hot melt adhesive mass or in modified hot melt adhesives, those according to the invention are grafted Olefin copolymers in particular those which have grafted side chains with polar acid or ester functions own. Preferred polar monomers are acrylic acid and methacrylic acid and their mono-, bi- and polyfunctional esters and other derivatives. These include mono- and polyvalent acrylic acid esters, e.g. methyl methacrylate, ethyl methacrylate, n-butyl methacrylate, isobutyl methacrylate, allyl methacrylate, tetrahydrofurfuryl methacrylate, 2-hydroxyethyl acrylate, tert-butylaminoethyl methacrylate, 1,4-butanediol dimethacrylate, trimethylolpropane trimethacrylate, Pentaerythritol triacrylate. But vinyl acetate, N-vinylpyrrolidone, allylamine, among others, are also special suitable monomers.

The organic unsaturated derivatives of silicon, such as vinylsilanes and acrylicsilanes, occupy a certain special position. These include vinyltrichlorosilane, vinyltriethoxysilane, vinyltris- (beta-methoxyethoxy) -silane, vinyltriacetoxysilane, gamma-methacryloxypropyltrimethoxysilane.

By grafting such unsaturated silanes onto polyolefins, graft copolymers are obtained which have a high specific wetting ability on various substrate surfaces wrap. If they are used alone as a hot-melt adhesive mass, a content of 0.5-5 percent by weight of grafted is preferred Comonomers, based on the polyolefin, required. On the other hand, it is used as a modifier in other hot melt adhesives used, the content of grafted silanes can be up to 50 percent by weight in the polyolefin graft copolymer.

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According to the invention, the grafted-on silanes give the hotmelt adhesive mass a high resistance to moisture, wetness, steam, without sacrificing the other good properties, such as e.g. heat stability.

The new grafted olefin copolymers according to the invention can now be used alone or in a mixture with one another as a hot melt adhesive use mass. You can also use other additives, such as with another random copolymer, such as Ethylene-vinyl acetate or ethylene-acrylate copolymer, polypropylene, Adhesive resins, waxes, thinners, plasticizers and / or fillers are modified. To protect them from thermal Stabilizers and antioxidants can also be added to protect against degradation and discoloration.

Furthermore, the hot-melt adhesive compositions according to the invention can also be mixed with coloring agents, such as titanium dioxide, earth colors and the like be colored. For special applications, these hot melt adhesives can also be mixed with bitumen, tars, Modify asphaltene, pitch and the like. The olefin graft copolymers according to the invention already contribute low contents of polar groups in the side chain good adhesive properties, with the preferred, grafted Monomers that include acrylic acid or one of its derivatives, vinyl pyrrolidone, and vinyl silane.

Furthermore, it has surprisingly been found that the olefin graft copolymers according to the invention ali hotmelt adhesive compositions can be used to bond or bond mainly non-polar surfaces, such as those of polyethylene, polypropylene and the like, without surface pretreatment thereof.

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For example, polyolefin graft copolymers with low comonomer contents, in particular those with 0.5 to 10 percent by weight, based on the polyolefin, when melt bonding non-pretreated, non-polar polyolefin substances with a metal surface, in particular aluminum, has such high adhesive strengths that a peel strength test results in a clear cohesive break occurs in the polyolefin substrate.

Since olefin graft copolymers according to the invention whose melt viscosity is too high or whose melt index is too low or other specific adhesive properties are required must be used for many areas of application
they have to be modified with other additives.

To reduce the melt viscosity or to increase the melt index and / or to modify adhesion or cohesion properties, the olefinic graft copolymers according to the invention can contain diluents in amounts of up to
200 percent by weight, based on the total weight of the 01efinpfropfpolymeren, are added. Diluents include liquid polybutene or polypropylene with molecular weights between 600 and 1,500; Petroleum waxes, for example paraffins and microcrystalline waxes; Polyethylene oils with
a molecular weight <1000; Mineral oil and synthetic waxes, such as Fischer-Tropsch wax, hydrogenated animal and vegetable fats.

Particularly suitable additives and modifiers for the olefinic According to the invention, graft copolymers are also so-called tackifying substances and plasticizers,

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on the one hand to change the adhesion properties but also on the other hand as a "diluent" to reduce the Serve melt viscosity. Such additives can also make the hot melt adhesive masses soft and pliable and give them give specific tack. Such additives and modifiers can be added to the polyolefin graft copolymers according to the invention in amounts up to 70 percent by weight, based on the total weight of the hot melt adhesive mass. For this include for example:

1. Aliphatic hydrocarbon resins with a ball and ring softening point (according to ASTM E 28-58T) of about 60-150 C. These resins are obtained, among other things, during the polymerization of monomers consisting predominantly of olefins, diolefins and other dienes with 5-7 carbon atoms. Such hydrocarbon resins are particularly suitable for modification because of their relationship to the polyolefinic chains of the polyolefin graft copolymer. They are compatible with the graft copolymers according to the invention in all proportions. Among other things, they have a "plasticizing ¹¹ effect on the olefin graft copolymers and at the same time lower the melt viscosity or increase the melt index.

2. Coumarone-indene resins with a ball and ring softening point of about 10-160 C.

3. Polyterpene resins with a softening point (according to ASTM E 28-58T) of about 10 to 150 C, which are used in the polymerization of Bicyclic pinene obtained in the presence of Friedel-Crafts catalysts.

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4. Phenol-modified terpene resins, such as those obtained, for example, in the condensation of a bicyclic terpene and a phenol in an acidic medium. They generally have a ball and ring softening point of about 80 to 160 ^° C.

5. natural and modified types of rosin, e.g. Wooden rosin, tall oil rosin, tap rosin,

. distilled rosin, hydrogenated rosin, dimerized Rosin, disproportionated and polymerized rosin.

6. Esters of natural or modified rosin, e.g. glycerine, methyl, triethylene glycol and pentaerythritol esters of natural or modified rosin, hydrogenated rosin glycerol esters, hydrogenated rosin triethylene glycol esters, the methyl ester of rosin and the penterythritol ester of polymerized rosin.

7. Polystyrene and styrene copolymers in combination with at least one unsaturated aromatic compound, for example vinyl toluene or C-- methyl styrene. These homo- and Mischpoly merisate have a ball and Ring softening point of about 50 to 125 ⁰ C.

8. Chlorinated terphenyl and diphenyl resins with a chlorine content of 40 to 70 percent by weight.

9. Alkyl phthalic acid esters, e.g., dibutyl and dioctyl phthalate;

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Glycol esters of phthalic acid, e.g. butyl phthalyl butyl glycolate, Methyl and ethyl phthalyl ethyl glycolate.

10. Acrylic phosphoric acid, e.g., tricresyl phosphate.

Π. Aryl sulfonamide derivatives, e.g. p-toluene sulfonamide, N-ethyl -p-toluene-sulfonate.

To achieve certain properties, the hot melt adhesive masses other olefinic polymers and copolymers can also be incorporated according to the invention. This is suitable including ethylene-vinyl acetate, ethylene-acrylate copolymers, with about 4 to 16 moles of ethylene per mole of vinyl acetate or acrylate, Polyvinyl acetate and copolymers. Particularly interesting in this context are those ethylene vinyl acetate and ethylene / Acid copolymers with which additionally a strong melt viscosity reduction is achieved. Typical representatives of such copolymers are the "AC-COPOLYMERS" from ALLIED CHEMICAL COP., In particular the commercial products A-C 540, 430, 580 and 760. For specific areas of application in which the brown to dark color does not play an essential role, the olefin graft copolymers according to the invention can also be used with bitumina, Asphaltene, tar, tar and the like can be modified. Such hot-melt adhesive compositions contain, in particular, blown ones Bituminous, which have a ring and ball softening point of around 50-130 ° C.

Furthermore, fillers, preferably those of mineral origin, such as talc, light spar, barite, chalk, asbestos, quartz flour, Neuburg silica

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earth and the like are added.

To protect the new hot melt adhesive masses against thermal degradation and discoloration, stabilizers and anti-oxidants, e.g. butylated hydroxytoluene, high molecular weight, sterically hindered phenols and substituted phosphates are used will.

The new hot-melt adhesive compositions can be produced by various processes if the inventive Olefin graft copolymers must be modified. Mixing vessels with agitators that are equipped with are equipped with a jacket for steam or oil heating. But also heatable kneading machines with 2 kneading arms, single-screw extruders and heatable roller mills can be used for this. The homogeneous mixed hot melt adhesive mass can then be converted into pellets, small pieces, granules and the like on known devices.

The new hot-melt adhesive compositions according to the invention can be used in many areas of application. Are particularly suitable they are used for a wide variety of packaging and lamination processes, e.g. for the production of composite films from polar and non-polar Substrates with each other and with each other. These include in particular polyolefin films, metal foils, paper, coated paper, corrugated cardboard, Cardboard lids and cellophane films.

However, these new hot melt adhesive masses can also be used to coat packaging films without surface pretreatment to reduce or prevent the water vapor and aroma permeability, the hotmelt adhesive layer being a very

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retains good heat sealability, even with respect to untreated, non-polar substrate surfaces. But they can also be used to close cardboard boxes and the like. Leave in the bookbindery they are involved in gluing the spine of the book.

The new hot-melt adhesive masses are ideal for the production of laminates completely new aspects, because the sole use of the graft copolymers according to the invention or With a high proportion in mixtures, there is often no surface pretreatment, apart from a possibly necessary degreasing, is required for a large number of material surfaces. This is especially true for polyolefins and aluminum Laminates are used today, among other things, as ski coverings.

Other areas of application are in the woodworking industry for gluing edges and laminate boards on chipboard and the like given.

Furthermore, the new hot melt adhesive compositions for the production of composite film webs that are used in construction, packaging and as tarpaulins.

In the automotive industry, however, they can be used for many purposes, e.g. for gluing in air and gasoline filters in engine construction can also be used for vehicle interiors.

Another area of application as a new hot melt adhesive mass is the bonding of road marking nails or their use as road marking compounds.

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The following examples are intended to illustrate the use of the new grafted olefin copolymers as hot melt adhesive mass will.

example 1

The olefin graft copolymer used was produced from a low-pressure polyethylene with a melt index (MFi 190/2) of 5.2 by grafting on acrylic acid. The acrylic acid content of the graft copolymer was 0.6 and the melt index 5.3. It was stabilized with 0.45% butylated hydroxytoluene.

This olefin graft copolymer powder was used to bond aluminum to low-pressure polyethylene. For this purpose, aluminum sheets were used and low pressure polyethylene tapes measuring 200 χ 10 χ 0.3 cm degreased with a chlorinated hydrocarbon and about 5 g of the olefin graft copolymer powder on each aluminum surface scattered. The low-pressure polyethylene was applied and this test specimen was subjected to a pressure of approx. 5-6 atU at 130.degree pressed for about 10-15 minutes. After the test specimens had cooled, the adhesive bond was subjected to a peel strength test. The bending angle was 180 and the feed rate 100 mm / minute. The bond strengths were so excellent that a cohesive failure could be determined in all 5 test pieces in the low-pressure polyethylene tape.

Example 2

A customary aluminum packaging film was extrusion-coated on the matte surface side with an olefin graft copolymer of low-pressure polyethylene with a melt index of 3.7 and an acrylic acid content of 0.7% and on "one

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heated roller (180 C), with additional use of one Hot air stream, a non-pretreated low-pressure polyethylene film was laminated to a thickness of about 100 nm. The subsequent peel strength test on 5 test specimens yielded values between 3-5 kp / cm.

Example 3

The following hot melt adhesive compound was produced:

50.0 parts by weight of olefin graft copolymer

2)

50.0 parts by weight aliphatic hydrocarbon

0.4 parts by weight of stabilizer BHT ³ ^

'MFi Ί90 / 2 = 5.3, acrylic acid content: 0.6 % Basis: low-pressure polyethylene

Ring and ball softening point: 100 C Acid number: max. I.

3)

Butylated hydroxytoluene

The products were melted together homogeneously at 240 C and daruas glue cartridges poured for the hot melt glue gun. The finished hot melt adhesive mass had a melt index (MFi 190/2) from 62. This was used to apply hot-melt adhesive diamonds at 220 to 230 ° C using a hot-melt glue gun Polyethylene coated cardboard is applied and glued together. When the adhesive or. Verbundprüfung separated the Polyethylene layer from the cardboard substrate, while the hot-melt adhesive bond was completely perfect.

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Example 4

20 parts by weight of olefin graft copolymer 20 parts by weight of ethylene-vinyl acetate copolymer with

approx. 18 % vinyl acetate

10 parts by weight of aliphatic hydrocarbon resin 15 parts by weight of the glycerol ester of rosin

(Softening point 65 C)

5 parts by weight of coumarone-indene resin

(Softening point 105 C)

20 parts by weight of light spar 10 parts by weight of heavy spar 0.5 parts by weight of stabilizer BHT

Basis: high pressure polyethylene

Melt index (MFi 190/2): 10.1 Acrylic acid content: 15 %

Melamine resin edging was applied with this hot melt adhesive mass Chipboard glued at 220 C. When the glue joint was pierced, not only an 80-year-old was torn out, but also one good heat resistance (+ 80 ° C) and cold resistance (-10 ° C) achieved.

Example 5

25 parts by weight of olefin graft copolymer 25 parts by weight of aliphatic HC resin

(Softening point 110 C)

5 parts by weight of pentaerythritol ester of rosin 15 parts by weight of polybutene, molecular weight approx 10 parts by weight of polyterpene resin

(Softening point 100 C)

10 parts by weight of chlorinated diphenyl resin with a chlorine content

from approx. 50/2

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5 parts by weight of styrene / ^ - methyl styrene copolymer /

75 ⁰ C

5 parts by weight of A-C- COPOLYMER 760 0.5 parts by weight of stabilizer BHT

Basis: high pressure polyethylene

Melt index (MFi 190/2 = 15.3) Vinyl acetate content: approx. 10 %

This hot melt adhesive mass was used to produce a commercially available Aluminum foil glued to a cardboard box. In the peel test, 100 # paper tear and a peel strength of 2-3 kp / cm achieved.

Example 6

30 parts by weight of olefin graft copolymer 70 parts by weight of bitumen, softening point: 85 ° C

Basis: high pressure polyethylene

Melt index (MFi 190/2 = 2.4) Acrylate content: 15.2 %

Road marking nails were made with this hot melt adhesive mass glued to an asphalt substrate and exposed to normal driving for 50 days. Compared to another Hot melt adhesive based on ethylene vinyl acetate, showed the Hot melt adhesive mass with grafted olefin copolymers does not fail, while with the other adhesive approx Marker nails were removed.

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Claims (16)

PATENT CLAIMS 1. Use of olefin copolymers consisting of olefinic Graft copolymers with a content of grafted, polar monomers of more than 0.1 and less than 100 percent by weight, based on the saturated hydrocarbon chain, as a hot melt adhesive mass. 2. hot melt adhesive composition according to claim 1, characterized in that that the grafted monomer is an unsaturated carboxylic acid, especially acrylic acid, methacrylic acid, oC-chloroacrylic acid and / or maleic acid. 3. hot melt adhesive composition according to claim 1, characterized in that that the grafted-on monomer is one of the general formula CH ₀ = C - C ² I \. worxn R. = hydrogen, halogen or an alkyl group with 1-4 carbon atoms, X = - 0 - or -N-, and R ~ = H, or a C.-C "-alkyl group, which can be substituted with a hydroxyl group, R _n = hydrogen or an alkyl radical with 1 to 18 carbon atoms, it being possible for this radical to be substituted by an amino or hydroxyl group, is. 609883/1044 -19 - 45 4. hot melt adhesive composition according to claims 1 and 3, characterized characterized in that the grafted-on monomer is preferably an unsaturated ester, in particular a mono- or poly- is a functional ester of acrylic acid and its derivatives, 5. hot melt adhesive composition according to claim 1, characterized in that that the grafted monomer is an unsaturated ester from the class included in the esterifying group at least carry a double bond, in particular vinyl acetate, vinyl benzoate, is· 6. hot melt adhesive composition according to claim 1, characterized in that that the grafted-on monomer is an aryl vinyl compound, especially styrene 7. hot melt adhesive composition according to claim 1, characterized in that that the grafted-on monomer is a vinyl sulfonic acid, in particular ethene sulfonic acid, 8. Hot melt adhesive composition according to claim 1, characterized in that that the grafted-on monomer is a heterocyclic compound bearing vinyl groups, in particular vinylpyrrolidone. 9. hot melt adhesive composition according to claim 1, characterized in that that the grafted-on monomer is an organically unsaturated derivative of silicon, in particular a vinylsilane. 10. hot melt adhesive composition according to any one of claims 1 to 9, characterized characterized as being a blend of the grafted olefin copolymers. - 20 - 608883/1044 11. hot melt adhesives according to one of claims 1 to 10, characterized in that it is based on up to 200 percent by weight of a waxy or oily diluent on the total weight of the olefin graft polymer, contains 12. hot melt adhesive composition according to one of claims 1 to 11, characterized in that it contains up to 70 percent by weight of a tackifying substance, based on the total weight of the hot melt adhesive mass. 13. hot melt adhesive composition according to any one of claims 1 to 12, characterized in that it contains up to 70 percent by weight of a bitumen, a coal tar, asphalt, earth pitch or the like, based on the total weight the hot melt adhesive mass. 14. hot melt adhesive composition according to one of claims 1 to 13, characterized in that they also contain genuine copolymers with a random arrangement of the monomers Reactants, especially ethylene / vinyl acetate or ethylene / acrylate copolymers. 15. hot melt adhesive composition according to one of claims 1 to 14, characterized in that they contain up to 100 percent by weight of inert fillers, based on the total weight of the Olefin graft polymers. 16. Use of the hot melt adhesive composition according to any one of claims 1 to 15 for connecting and / or coating untreated, non-polar and polar surfaces under and with each other 609883/1 044