JPH04227982A - Hot melt adhesive based on ethylene terpolymer and method of bonding by using the same - Google Patents

Abstract

PURPOSE:To obtain a heat-stable hot melt adhesive which can be used for bonding various adherends by mixing a specified ethylene terpolymer with a tackifier. CONSTITUTION:A hot melt adhesive composition which is a molten liquid at a service temperature and comprises an ethylene terpolymer comprising about 40-87wt.% ethylene, about 5-50wt.% second monomer selected between an alkyl acrylate and an alkyl vinyl ether (wherein the alkyl has 1-8C atoms) and about 3-30wt.% third monomer selected between carbon monoxide and sulfur dioxide (based on the weight of the terpolymer), about 5-80wt.% compatible tackifier (based on the total weight of the terpolymer and the tackifier) and 0-30wt. % compatible plasticizer (about 4wt.% or below when the second monomer is present in an amount of 10wt.% or below).

Description

Description: FIELD OF THE INVENTION The present invention relates to hot melt adhesives, and more particularly to hot melt adhesives made from terpolymers of ethylene, alkyl acrylates or alkyl vinyl ethers, and carbon monoxide or sulfur dioxide. The present invention relates to hot melt adhesives that are prepared. TECHNICAL BACKGROUND OF THE INVENTION Various copolymers of ethylene are known for use in hot melt adhesives. The most widely known and used of these are ethylene copolymers with vinyl acetate having various viscosities and vinyl acetate contents. Ethylene vinyl acetate methacrylic acid copolymers have also been disclosed for adhesive applications. Other ethylene copolymers are also known for this use, such as ethylene and acrylic acid and ethylene and maleic anhydride copolymers. Ethylene-vinyl acetate copolymer has a temperature of 350°F (17
It is not very thermally stable at application temperatures above 7°C. More stable ethylene copolymer adhesives are disclosed. Ethylene butyl acrylate copolymer is Bardy
No. 4,816,306, issued to et. ” is shown. The better melt stability and low temperature properties of these polymers
ive Age', November 1989, which states that ethylene/n-butyl acrylate adhesive formulations retain their fluidity better at 350°F (177°C). It was also possible to process at temperatures over 100°F. Carbon monoxide is polymerized with ethylene and vinyl acetate or alkyl acrylate to form ethylene vinyl acetate carbon monoxide terpolymers and ethylene alkyl acrylate carbon monoxide terpolymers. Such polymers are described in US Pat. No. 3,780,140 to Hammer et al. as plasticizers in polymer blends with PVC. US Pat. No. 4, issued to Brugel et al.
, 434,261, 200-350°F (
Hot-melt adhesive sheets are described that are self-supporting at application temperatures of 94-177° C.), which sheets can be cut on their own and shaped to the shape of the adherend. These sheets are distinguished from "conventional hot melt adhesives which must be applied in molten form as pre-melted hot fluids". The self-supporting nature of this sheet is characterized by a filler content of 20-80% (most preferably 50%).
~60%) and plasticizer 2-30% (most preferably 12-30%)
18%) to any of various ethylene copolymers. Ethylene/vinyl acetate is exemplified as a polymer component. Among the many other ethylene copolymers disclosed but not exemplified in this patent are terpolymers with vinyl acetate or alkyl acrylates and carbon monoxide or sulfur dioxide. These sheets are cloth-like structures,
In particular, it is described that it can be laminated to polyester nonwoven fabrics and polypropylene nonwoven fabrics. US Pat. No. 4,600,614 to Lancaster et al. describes multilayer microwave packaging in which two layers of the same "radiation-sealable material" are in sealable contact with each other. The electromagnetic radiation sealable material can be any of a number of copolymers and terpolymers, which should contain from 0.01 to 50% by weight carbon monoxide. Carbon monoxide allows the polymer to be heated by high frequency electromagnetic radiation (microwave energy). If a ternary monomer is present, this may be vinyl acetate, acrylic acid, methacrylic acid, esters or salts thereof. US Pat. No. 4,601,948 to Lancaster et al. discloses new terpolymers that can be used as hot melt adhesives. These terpolymers are terpolymers of ethylene, carbon monoxide and acrylic or methacrylic acid, with each of the last two components ranging from 1 to 40% by weight. Acids are in the free acid form, not esters of acids. It is well known that ethylene/methacrylic acid copolymers are used in hot melt adhesives. [0007] Japanese Patent Publication No. 2-73 transferred to Mitsui DuPont
Publication No. 828 (published on March 13, 1990) states that
A high performance adhesive of nylon grafted ethylene butyl acrylate carbon monoxide terpolymer is disclosed. This publication describes the use of a terpolymer alone in a comparative example with insufficient high temperature adhesion performance. There remains a need for hot melt adhesives with good thermal stability that have wide applicability with respect to adherend type, ie, end use, and that can be applied in commonly available commercially available low shear hot melt application equipment. There is. SUMMARY OF THE INVENTION The present invention can be used to bond a wide variety of adherends, such as metals, polar and non-polar plastics, and wood and paper products, and can be used to bond conventional low shear hot The above needs are met by providing a heat stable adhesive composition that can be applied in an economical manner using melt adhesive application equipment. That is, the adhesive composition takes the form of a molten liquid when heated for application as a hot melt adhesive, which is too fluid to be extrudable or self-supporting, but It can be ideally applied to hot melt applications. Accordingly, one embodiment of the present invention provides about 40-87% by weight of ethylene and about 5-50% by weight of the second monomer alkyl acrylate or alkyl vinyl ether.
Weight % and carbon monoxide or sulfur dioxide about 3-30
Ethylene terpolymer containing wt% (wt% above)
(based on the weight of the terpolymer) and about 5 to 80% by weight of a compatible tackifier (based on the weight of the terpolymer plus the tackifier). , provides a thermally stable hot melt adhesive composition that is liquid at the application temperature. However, if the second monomer is present at between about 5 and 10 weight percent, then at least about 4 weight percent plasticizer is always present. A compatible wax may optionally be present in the composition. Another aspect of the invention is to apply the adhesive composition of the invention to metals, polar and non-polar plastics, wood and paper products at elevated temperatures such that the composition converts to a molten liquid. and applying the applied composition to a second adherend while the composition applied to the adherend is in the form of a molten liquid. In this method, the composite structure is brought into contact with each other, and then the resulting composite structure is cooled. DETAILED DESCRIPTION OF THE INVENTION The terpolymer component of the adhesive composition of the present invention provides cohesive strength, adhesive strength and thermal stability to the composition. The alkyl acrylate or alkyl vinyl ether can be considered the second monomer of the terpolymer. Examples of alkyl acrylates are those in which the alkyl group has 1 to 8 carbon atoms. Such examples include alkyl acrylates and methacrylates such as methyl acrylate, ethyl acrylate, isobutyl acrylate, n-butyl acrylate, 2-ethylhexyl acrylate and the corresponding methacrylates. The second monomer that lowers the glass transition temperature of the terpolymer tends to lower the viscosity of the terpolymer for a given molecular weight and makes it tougher at room temperature and moderately low temperatures. Guarantees high strength polymers. n-Butyl acrylate is particularly useful in this regard and is therefore a preferred second monomer. When using lower alkyl acrylates, such as methyl acrylate, it is advantageous to add suitable plasticizers. [0015] In order for the adhesive composition to provide strong adhesion, at least about 5% by weight of the terpolymer should consist of alkyl acrylate. The maximum amount of acrylate monomer is generally governed by the maximum amount that can be copolymerized with ethylene and the third monomer. Generally this maximum amount is about 50% by weight. Alkyl vinyl ethers as second monomers, preferably having 1 to 8 carbon atoms in the alkyl group, can be used in place of alkyl acrylate comonomers and provide the same properties as alkyl acrylates in adhesive compositions. give something to something. Examples of alkyl vinyl ethers include methyl vinyl ether, ethyl vinyl ether,
Included are isobutyl vinyl ether, n-butyl vinyl ether, and 2-ethylhexyl vinyl ether. [0017] Compared to vinyl acetate, alkyl acrylate and alkyl vinyl ether monomers provide greater thermal stability to the composition. The adhesive composition of the invention, and therefore the polymer used therein, must first of all have sufficient thermal stability at temperatures at which the polymer is sufficiently liquid to carry out applications such as coating using hot-melt equipment. It is necessary to have Stability requirements are generally more stringent than those required for extrudable or preformed adhesives, as they are often accompanied by extended holding times at application temperatures. Carbon monoxide or sulfur dioxide can be considered the third monomer of the terpolymer. This comonomer increases the adhesive flexibility of the terpolymer and thus the composition so that it can adhere to a wide variety of adherends. At least about 3% by weight of the terpolymer is
It should be carbon monoxide or sulfur dioxide to provide this versatile effect. These termonomers are polar and impart this polarity to the terpolymer, allowing the adhesive compositions of the present invention to adhere to polar as well as non-polar plastic adherends. More than about 30 weight percent of these termonomers in the terpolymer can adversely affect the thermal stability of the terpolymer. The third monomer used here destroys the thermal stability of ethylene vinyl acetate terpolymers containing CO or SO2, even in the presence of antioxidants. Surprisingly, the terpolymers of the present invention have much better thermal stability, so that hot-melt adhesive compositions in which these terpolymers are applied as adhesives in the molten liquid state Advantageous utility can be achieved in One feature of thermal stability is the composition's resistance to oxidation while remaining in the liquid state at the application temperature. Preferred adhesive compositions of the present invention contain about 45-80% by weight ethylene, about 10-80% by weight alkyl acrylate.
40% by weight of a terpolymer containing about 3-20% by weight of carbon monoxide (amounts above are based on the weight of the terpolymer), and about 30-80% by weight of a tackifier (amounts above are based on the weight of the terpolymer). (based on the combined weight of copolymer and tackifier). The polymeric components of the present invention are disclosed in US Pat. No. 3,78
No. 0,140, which is incorporated herein. The tackifier component of the present invention can be selected from a wide variety of materials, including: a) Wood rosin acid, gum rosin acid and tall oil rosin acid. These may be hydrogenated, disproportionated or lightly polymerized. b) Esters of various grades of the above rosin acids. Alcohols suitable for preparing these esters include mono- and polyethylene glycols, glycerol, pentaerythritol and related products. c) Terpene resin. d) dicyclopentadiene-aromatic hydrocarbon resins, such as Hercules
Inc. No. 3,023,200, which includes 'Piccovar' resin manufactured by US Pat. No. 3,023,200. e) Low molecular weight resins based on styrene and/or substituted styrenes. The tackifier is selected to be compatible with the terpolymer component. This compatibility is
It is obtained by a terpolymer and a tackifier that are miscible with each other in the melt. Composition compatibility within the composition is observed by the composition being both clear in appearance and soft in appearance when cooled to room temperature. The proportion and type of tackifier, mixed with the terpolymer, generally ranges from about 250 to 400°F (121°F).
-204°C) to produce the desired flow properties at hot melt application temperatures. The flow properties of the adhesive compositions of the present invention are defined herein as 350°F (1
Brookfield viscosity at 77°C). The low viscosity required for the adhesive compositions of the present invention is achieved by starting from a relatively high viscosity terpolymer and by incorporating significant amounts of tackifier and compatible plasticizer (if used). and/or use waxes to reduce the viscosity to the required level, or start with even lower viscosity terpolymers and use lower amounts of tackifiers, plasticizers and/or waxes. This can be achieved either by: The viscosity of a terpolymer can be described as the melt index. The melt index of the terpolymer component is 190
It may be 1 to 3000 g/10 min, measured at °C. The viscosity of the hot melt adhesives of the present invention should be at least about 1000 cps at 177°C, and generally 5 cps at 177°C.
It does not need to be greater than 0000 cps. These viscosities approximately correspond to melt indices of about 10,000 to 200 g/10 min. [0027] Reducing the molecular weight of the terpolymer component lowers its viscosity, but this is accompanied by a decrease in the strength of the terpolymer itself. However, this means that smaller amounts of low molecular weight viscosity diluents (tackifiers, plasticizers and/or waxes) may be required in the formulation. The strength of the final preparation is usually a compromise between the viscosity of the terpolymer components and the amount of tackifier and plasticizer (if used). Using significantly higher molecular weight terpolymers and formulating the viscosity with excessive amounts of compatible tackifiers and plasticizers or waxes can result in compositions with insufficient cohesive strength. be. At least about 20% by weight terpolymer is required for the composition to have sufficient strength properties. The compositions of the invention may also contain compatible plasticizers and/or waxes for the purpose of adjusting the flow properties of the composition at the application temperature as well as other properties in the adhesive and the application equipment used. can contain. Generally, tackifiers tend to be more glassy and can increase the tackiness of the formulation, whereas plasticizers tend to be low molecular weight liquids with low glass transition temperatures. Examples of plasticizers that can be used in the adhesive compositions of the invention include phthalates, azelates, adipates, tricresyl phosphates and polyesters such as those used to soften polyvinyl chloride, alkylated phenols, phenolic modified Included are low molecular weight resins made from coumaron indene, terpenes and synthetic terpenes and petroleum-derived process oils. Wax compatibility is generally considered important in preparing many hot melt adhesives. Waxes can provide an inexpensive means of reducing viscosity, contribute to some extent to improved heat resistance, and can reduce air drying time or the time the polymer is tacky after application. This then leads to quick application times. In addition, wax can promote wetting and prevent blocking. Paraffin waxes commonly used in hot melt adhesives have the desired flexibility in adhesive compositions of the present invention due to the polarity imparted to the terpolymer by the CO or SO2 comonomer. Generally not compatible. Other waxes such as carnauba wax can be used in the adhesive compositions of the present invention. To vary the application, the adhesive preparer chooses from a wide range of possible formulation ingredients, such as tackifiers and optionally waxes and/or plasticizers, and Their concentrations will also be selected. There are many guidelines available to assist the preparer in finding suitable compositions for a given application. An excellent description of how these variables interact was presented at the Adhesives Short Course at the Adhesives and Sealants Conference held in Cleveland, Ohio, September 1989, and in the accompanying Adhesives Paul P Pulett published in Short Course Notebook
Written by i “Hot Melts-Yesterday, To
day and tomorrow”.Therefore,
Those skilled in the art of adhesive preparation can arrive at suitable formulations that balance these variables and adjust the economic constraints imposed by the costs of the various components. In addition to the terpolymers used in the adhesive compositions of the invention, small amounts of copolymers such as ethylene/vinyl acetate or ethylene/alkyl acrylate or ethylene/methacrylic acid may be added to the ternary copolymers of the composition. Can be mixed with polymeric components. Antioxidants are commonly used in the formulation of ethylene copolymer hot melt adhesives, and it has been found that these are desirable for optimal performance of the formulations of this invention. Suitable antioxidants include typical hindered phenols such as butylated hydroxytoluene (BHT), 'Etyl'330, Ciba Geigy'
Included are Irganox'1010 or 1098, as well as phosphites, butyl cinnamate. The hindered phenol 'Irganox' 1010 has been found to be particularly advantageous. When antioxidants are used, they are used in amounts effective to provide the desired oxidative stability at or above the oxidative stability of the terpolymer. The adhesive compositions of this invention can be made by conventional melt compounding of the components to form a miscible melt. This melt can then be applied as a hot melt adhesive. When used by themselves, this adhesive differs from solvent-based adhesives by the absence of a solvent and the adhesion-aiding effect of a solvent. this is,
This is because conventional hot melt adhesives are highly selective with respect to the substrates to which they are attached. [0036] Like conventional hot melt adhesives applied in the liquid state, the hot melt adhesives of the present invention face stringent requirements for thermal stability, including oxidative stability. The hot melt adhesive components can be melt compounded in a container and held in a heated molten state until applied as an adhesive. If the melt of the composition to be prepared is very viscous, known equipment such as, for example, a Banbury mixer or a Perkins Sigma blade mixer can be advantageously used for the melt compounding process. The time the resulting composition is held in the molten state may depend on the size of the container and the speed at which the composition is applied as an adhesive. During this time the composition will be exposed to the atmosphere and its oxidation. The adhesive compositions of the present invention are both oxidatively stable and thermally stable, or are sufficiently thermally stable that the use of an antioxidant in the composition can provide the desired additional oxidative stability. have sex. The adhesive compositions of the present invention also differ from the extrudable self-supporting sheets disclosed in US Pat. No. 4,434,261, which require heating only when applied as adhesives. and is therefore not exposed to the decomposition effects of heating for long periods of time, and is not exposed at all to heating to bring it to a liquid or molten state. Surprisingly, the compositions of the present invention have outstanding versatility as hot melt adhesives in terms of application to a wide variety of adherends, both polar and non-polar; A hot melt adhesive having sufficient thermal stability to be useful for the purpose is provided. The adhesive composition of the present invention is applied by conventional means for hot melt adhesives used in the liquid state. applying the adhesive composition in molten liquid form to an adherend; subsequently contacting the adhesive composition still in molten liquid state on the first adherend with a second adherend; The resulting composite structure is then cooled to form an adhesive layer. The adherends are typically at room temperature and the contacting step is typically conducted under sufficient pressure to obtain uniform distribution of the adhesive composition between the adherends. [0040] The adherends or substrates that can be adhered to each other by the adhesive compositions of the invention can be the same or different materials, such as metals, wood, paper, polar and non-polar plastics. Examples of plastics include polyethylene, polyesters including polycarbonates, polyacrylates including polymethyl methacrylate, polystyrene, polyvinyl chloride and ABS polymers. Examples of metals include aluminum and stainless steel. Effects of the Invention The hot melt adhesive composition of the present invention has the following properties:
It is in a molten liquid state at the application temperature and has excellent thermal and oxidative stability, allowing good adhesion to a wide range of adherends such as metals, wood, paper, polar and non-polar plastics. The hot melt adhesive compositions of the present invention can be applied with conventional hot melt adhesive applicators. EXAMPLES In these examples, the procedure for making the adhesive compositions tested was as follows. 350°F (1
A small amount of the adhesive formulation was made in a pint paint can placed in a block heated to 77°C. The tackifier, plasticizer (if used), and antioxidant were added first and, after melting, the terpolymer was added gradually. These mixtures were stirred using a commercially available three-blade propeller stirrer with an air-driven motor until the terpolymer was melted and completely dissolved. Adhesion tests in these Examples were conducted as follows. The substrate used was a panel with dimensions of 3 x 1 x 1/4 inches. Adhesion strength is measured using the so-called "button test"
It was tested using This was done as follows. Approximately 177
C. adhesive was applied to one substrate at room temperature, then a second substrate, also at room temperature, was placed on top of the adhesive and the two substrates were pressed together using finger pressure. The two substrates were laterally pressed together such that the total bonded area was about 1 square inch. After the adhesive has cooled and solidified, place the board in the Instro
Adhesion was tested by pulling apart at 0.5 inches/min with an n tester. The force required to break the bond was recorded. Thermal stability was measured using a Brookfield viscometer, model RVT, using 7 spindles. The viscosity was measured after various times in a viscometer. Oxidative stability was determined by leaving the adhesive composition in an open 2 inch diameter container in an air oven at about 177°C for the indicated time. Approximately 1/4 of the molten material is in this container.
Filled with enough material to be an inch deep. The viscosity was then measured by transferring the cooled hot air Bacro material to a Brookfield viscometer at 177°C. In the following description of the examples of the invention, parts and percentages are by weight unless otherwise indicated. Examples 1-10 and Comparative Examples C1-C3 These examples illustrate the good thermal and oxidative stability of the compositions of the invention and comparative preparations. Antioxidants are commonly used in ethylene copolymer hot melt adhesives. 'Irganox' 1010 was used here. The thermal stability results are shown in Table 1, and the oxidative stability results are shown in Table 2. Better stability of the terpolymer means better thermal stability of the prepared adhesive, which gives better processing flexibility. Examples 1 to 4 show that preparations with various terpolymers of ethylene and acrylate and carbon monoxide or sulfur dioxide are unstable after 3 hours. It is shown to be more thermally stable than polymers. In other words, the termonomer copolymerized with EVA(C1) almost destroyed the thermal stability of this terpolymer, whereas the composition of the invention in which the terpolymer contains CO is extremely thermally stable. Met. The composition of Example 1 had a relatively high viscosity. This can be reduced by using a larger proportion of tackifier or a different tackifier that gives greater fluidity at the application temperature and/or by adding compatible plasticizers and/or waxes to the composition. I can do it. Examples 5 to 7 and Comparative Example C2 show that the ethylene n-butyl acrylate carbon monoxide terpolymer surprisingly
It is shown to be just as stable as an ethylene n-butyl acrylate polymer that does not contain carbon monoxide. Carbon monoxide does not impair thermal stability at this concentration and, as is known from later examples, carbon monoxide improves the quality of the adhesive. Examples 8-10 and Comparative Example C3 demonstrate the oxidative stability of the compositions of the invention. The presence of CO at the indicated concentrations does not significantly affect oxidative stability. The stability is good as in Comparative Example C3. [Table 1] Table 1 Thermal stability (preparation:
In Examples 1-4 and Comparative Example C1, 40 parts of polymer, 6
0 parts of Foral 105, 1 parts of 'Irganox
'1010. 35 in Examples 5 to 7 and Comparative Example C2
part polymer, 65 parts Foral 105, 0.2 parts 'Irganox' 1010) Example no.
Resin Viscosity at 176℃, centipoise x 10-2
(Weight%) Initial 3 hours 24 hours
48 hours 72 hours 96 hours──────────
──────────────────────────
── 1 E/iBA/CO
(54/37.4/8.6)
2000 2000 2920
2 E/MA/CO
(63.7/26.3/10) 105
102.5 190 3
E/EA/CO (51.6/31
．． 9/16.5) 160 160
230 4 E/nBA/SO
2 (61.4/29.3/9.3
) 95 93 90
C1 E/VAc/CO
(66/24/10)
157 1000 5 E/
nBA/CO (63/19
/12) 32.8
39.7 41.2 43.9 4
8 6 E/nBA/CO
(66/25/9)
38.6 42.6 5
0 68 7 E/n
BA/CO (71/25/
4) 44.6 5
6 59 58 65
C2 E/nBA
(80/20) 3
7.2 45.5 49.
1 53 55.5 [Table 2] Table 2 Oxidative stability (Preparation: 35 parts of polymer, 65 parts of Foral 105
, 0.2 parts of 'Irganox' 1010) Example No. Resin
Viscosity at 350°F
(Weight%) Initial 24 hours 48 hours
72 hours 96 hours────────────────
──────────────────────
8 E/nBA/CO
(69/19/12) 32.8
28.2 28.4 27.2
27.4 9 E/nBA/C
O (66/25/9)
38.6 29.8 26
26 27.7 10
E/nBA/CO
(71/25/4) 44.6 3
7.2 29.8 29.4 29
C3 E/nBA
(80/20) 37.2
43.2 49.5 62
67.5 'Irganox'1010, CAS
Registration 6683-19-8 [Examples 11-13 and Comparative Example C4] Examples 11-1
3 and Comparative Example C4 are E/nBA and E/nBA/CO
Compatibility with various ranges of tackifiers compared with In evaluating the usefulness of tackifiers, it is necessary that the final composition be compatible as well as non-brittle and flexible. The test results shown in Table 3 show that 25% by weight n
Two terpolymers containing BA and 26% by weight nB
Regarding copolymers containing A, although the CO concentration may be low (
4%), indicating substantially greater compatibility of the terpolymer (9%). Further variations in the terpolymer components as in Example 13 result in more compatible compositions compared to Comparative Example C4. Useful compatibility with a wide range of tackifiers makes the compositions versatile. Opacity is a sign of incompatibility. [Table 3] C=compatible, I=incompatible, F=flexible, B
= Brittle, O = Opaque (1) Hercules In
c. Rosin acid (2) manufactured by Hercules Inc.
Rosin ester (3) manufactured by Hercules Inc.
Rosin Ester (4) Reinchhold Che
m. Terpene phenolic resin made by Hercules (5)
Inc. Pure monomer aromatic resin (6) Herc
ules Inc. Hydrocarbon resin (7) Nevil
le Chem. Aromatic hydrocarbons (8) Reich
hold Chem. Made of terpene phenolic resin (9
) Goodyear Tire and Rubber
Co. Synthetic polyterpene (10) Arizona
Chem. Rosin ester (11) manufactured by Hercule
s Inc. Polymerized α-pinene (12) manufactured by Hercu
les Inc. Examples 14-27 and Comparative Examples C5-C10 Examples 14-27 and Comparative Examples C5-C10 show various ternary compounds prepared using different types of tackifiers. The polymers exhibit adhesion to all of the various substrates, which is generally superior to ethylene vinyl acetate or ethylene butyl acrylate resin preparations. Despite the polar nature of the terpolymers, the adhesion even to non-polar resins such as polyethylene is even more markedly good. Ethylene vinyl acetate carbon monoxide terpolymer provides good adhesion but, as seen earlier, is thermally unstable. Examples 26 and 27 show that very low concentrations of the second monomer provide sufficient adhesion to a variety of substrates if a plasticizer is also present. Example 27 is the second
At this low concentration of monomer, we show that increasing the concentration of plasticizer improves the adhesive behavior. The results are shown in Table 4. Although viscosity was not measured in most cases, all preparations were liquid at the application temperature. [Table 4] [Table 5] NM Not measured NT Not tested T1=
Foral 105, T2=Kristolex 3
070P1=Plastal 550, C. P. Ha
ll, Company plasticizer 1. Aluminum 2. High density polyethylene 3. 'Lexan' polycarbonate resin4. 'Lucite' acrylic resin5. Polystyrene resin6. Hard polychlorinated resin7. Acrylonitrile butadiene styrene resin A value of 8.134 was the highest reading obtained. Because the invention can be made in many markedly different embodiments without departing from its spirit and scope, the invention is not intended to be limited to the particular embodiments thereof except as specified in the claims. It should be understood that there is no such thing.

Claims (8)

[Claims] 1. About 40-87% by weight of ethylene, about 5-50% by weight of a second monomer selected from the group consisting of alkyl acrylates and alkyl vinyl ethers, where alkyl has 1 to 8 carbon atoms. , an ethylene terpolymer containing from about 3 to 30% by weight of a third monomer selected from the group consisting of carbon monoxide and sulfur dioxide (the above amounts are based on the weight of the terpolymer); about 5-80% by weight of a soluble tackifier (based on the combined weight of terpolymer and tackifier), and 0-3% of a compatible plasticizer.
is a molten liquid at the application temperature consisting essentially of 0% by weight (but if the second monomer is present at 10% or less, the level of plasticizer is about 4% or more) Hot melt adhesive composition. 2. The composition of claim 1, wherein the molten liquid has a viscosity of about 50,000 cps or less at 177°C. 3. A composition according to claim 1, wherein the second monomer is present in an amount of 15 to 40% by weight and the third monomer is carbon monoxide. 4. A composition according to claim 3, wherein the tackifier is present in an amount of 30 to 70% by weight. [Claim 5] Claim 1 containing a compatible wax.
Compositions as described. [Claim 6] Claim 1 containing an effective amount of an antioxidant.
Compositions as described. 7. The adhesive composition according to claim 1, consisting of metal, wood, paper, cardboard, polar and non-polar plastic materials, at an elevated temperature such that the composition converts into a molten liquid. applying the composition to any adherend selected from the group, while the composition is in a molten liquid state, contacting the applied composition with a second adherend, and the resulting composite structure. Cooling bonding method. 8. The plastic material is polyethylene,
8. The adhesive method according to claim 7, wherein the adhesive is selected from the group consisting of polyester, polyacrylate, polystyrene, polyvinyl chloride, and acrylonitrile butadiene styrene copolymer.