CN1193937A - Bind enhancer for linear polyolefins - Google Patents
Bind enhancer for linear polyolefins Download PDFInfo
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- CN1193937A CN1193937A CN96196579A CN96196579A CN1193937A CN 1193937 A CN1193937 A CN 1193937A CN 96196579 A CN96196579 A CN 96196579A CN 96196579 A CN96196579 A CN 96196579A CN 1193937 A CN1193937 A CN 1193937A
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- ethene
- multipolymer
- copolymer
- laminate
- polar group
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Abstract
The invention is a laminate. The laminate comprises a) a first substrate of a first basic linear olefin copolymer; b) adhesion promoter which is piled up on the first substrate; the adhesion promoter comprises graft copolymer of a second basic linear olefin copolymer; c) adhesive resin which is mixed with the adhesion promoter or the adhesive which is piled up on or mixed with the adhesion promoter; and d) a second substrate which is adhered to the first substrate. The invention is also an adhesion promoter. The adhesion promoter comprises the copolymer which is derived from the C2- C20 olefin and the alkenyl unsaturated amide or anhydride, and the basic linear olefin copolymer which is functionalized by polar group or the mixture of the ethylene which is functionalized by polar group and the copolymer of C3-C20 Alpha- olefin. The functionalized ethylene is provided with narrow molecular weight distribution; the copolymerized monomer unit is randomly distributed along the main chain of the polymer; and the evenness index is at least 75. Both the laminate and the adhesion promoter of the invention can be used for various final purpose, such as the bathroom gasket, the shoe sole, the carpet pad and the windshield of automobile.
Description
The present invention relates to a kind of bind enhancer that is used for laminate, this laminate comprises it being the polyolefin elastomer of line style basically.
The laminar structure that comprises many polymer layers is well-known in the art.In United States Patent (USP) 4,058,647; 4,198,327; 4,332,858; 4,341,837 and 4,588,648; And among european patent application 0 322 045 A2 this class formation is disclosed.
For the laminate that makes polymkeric substance is successfully used, each polymer layer bonding must be split in use avoiding.United States Patent (USP) 4,058,647 disclose: can and comprise that the polymer composition with unmodified polyolefine and rubber components of modification is laminated together with ethylene-vinyl alcohol copolymer.United States Patent (USP) 4,198,327 disclose: can with polycarbonate and ethylene-vinyl alcohol copolymer with comprise carboxylation polyolefine and the composition bond of hydrocarbon elastomer be in the same place.United States Patent (USP) 4,332,858 and 4,341,837 disclose: adopt for example segmented copolymer of the maleinization of vinylbenzene and divinyl of unhydrided segmented copolymer, can be with homopolymer and the multipolymer and the polycarbonate adhesive of alkene.United States Patent (USP) 4,588,648 disclose: adopt to comprise the graft copolymer of alkene and maleic anhydride and the polyacrylic binder layer of grafted not, polypropylene and evoh layer can be forced together.European patent application 0322045A2 discloses: for example adopt comprise carboxylic acid-or the polyolefine of acid anhydrides-modification for example maleinization polypropylene and have mainly comprise hydrogenation conjugated diene block selective hydration for example saturated styrene butadiene of segmented copolymer or the binder composition of styrene isoprene segmented copolymer, can polycarbonate and ethylene-vinyl alcohol is laminated together.At United States Patent (USP) 4,954, disclose in 573 and 4,966,947: adopt the acidated polyolefine of chlorination, carboxylic of modification to have the first coating of promoting as generation with base material agglutinating polymkeric substance.
Do not propose in the reference cited above as United States Patent (USP) 5,272,236 and 5,278, being used to described in 272 comprises the suitable bind enhancer of laminate of the olefin copolymer that is line style basically.Find that suitable bind enhancer that this analog copolymer of a kind of confession uses should be a progress in this area.
The present invention is a kind of laminate, and this product comprises:
A) comprise that first kind is first base material of the olefin copolymer of line style basically;
B) be superimposed upon bind enhancer on this first base material, this bind enhancer comprise polar group functionalized second kind be the olefin copolymer of line style basically;
C) with this bind enhancer blended tackifying resin, or be superimposed upon on this bind enhancer or with its blended tackiness agent; With
D) glued second base material on this first base material; Wherein this first kind and second kind is that the olefin copolymer of line style is characterised in that to have basically:
I) M
w/ M
nLess than 3.5;
Ii) I
10/ I
2Be not less than 6; With
Critical shear speed ratio when iii) surperficial melt fracture begins has about same melt exponential sum M
w/ M
nThe surperficial melt fracture of the polymer of linear olefin critical shear speed big at least 50% when beginning; Every kind is that the olefin copolymer of line style is ethene and C basically
3-C
20The multipolymer of alpha-olefin.
On the other hand, the present invention is a kind of bind enhancer, and this bind enhancer comprises the mixture of following component:
A) by C
2-C
20Alkene and ethylenically unsaturated carboxylic acids or acid anhydrides deutero-multipolymer and
What b) polar group was functionalized is the olefin copolymer of line style basically, and this multipolymer has:
I) M
w/ M
nLess than 3.5;
Ii) I
10/ I
2Be not less than 6; With
Critical shear speed ratio when iii) surperficial melt fracture begins has about same melt exponential sum M
w/ M
nThe surperficial melt fracture of the polymer of linear olefin critical shear speed big at least 50% when beginning; The feature of every kind of olefin polymer also is to be ethene and C
3-C
20The multipolymer of alpha-olefin; Or
C) polar group is functionalized ethene and C
3-C
20The multipolymer of alpha-olefin, this multipolymer have narrow molecular weight distributions, comonomer unit along this main polymer chain stochastic distribution, and evenness index is at least 75.
First base material of laminate of the present invention comprises that first kind is the olefin copolymer of line style basically.Be superimposed upon on this first base material be comprise second kind be basically the polar group of olefin copolymer of line style functionalized the bind enhancer of polymkeric substance.
Perhaps, this bind enhancer can comprise polar group functionalized ethene and C
3-C
20The multipolymer of alpha-olefin, this multipolymer have narrow molecular weight distributions, comonomer unit along this main polymer chain stochastic distribution, and evenness index is at least 75.Elston is at United States Patent (USP) 3,645, in 992 and Welborn at United States Patent (USP) 5,324, this base polymer (hereinafter being called ' 992 polymkeric substance) is described in 800, this base polymer comprises can be by trade(brand)name TAFMER
TM(trade mark of Mitsui Petrochemical) and EXACT
TMThose polymkeric substance that (trade mark of Exxon Chemical) bought.
First kind and second kind is that the olefin copolymer (hereinafter being called the substantial linear olefin copolymer) of line style is characterised in that to have 1 basically) high melt elasticity; 2) high workability; 3) less than 3.5 polydispersity index; With 4) basically with the irrelevant melt flow index of polydispersity index.Critical shear speed ratio when the feature of this class substantial linear olefin copolymer is also that the surperficial melt fracture that has begins has about same melt exponential sum M
w/ M
nThe surperficial melt fracture of the polymer of linear olefin critical shear speed big at least 50% when beginning.
This class substantial linear olefin copolymer is ethene and at least a C
3-C
20Alpha-olefin and optional a kind of C
2-C
20Acetylene series unsaturated monomer or a kind of C
4-C
18Diolefinic is 5-ethylidene-2-norbornene or a kind ofly comprise 1,5-hexadiene, 1,7-octadiene and 1, the α of 9-decadiene, the multipolymer of ω-diene for example.Preferred this substantial linear olefin copolymer is ethene and C
4-C
10Alpha-olefin, be more preferably the multipolymer of ethene and 1-butylene, 1-hexene, 4-methyl-1-pentene or 1-octene.This substantial linear olefin copolymer multipolymer that is ethene and 1-octene most preferably.
Preferred this substantial linear olefin copolymer along this main polymer chain in per 1000 carbon atoms, have 0.01 to 3, more preferably 0.3 to 1 long-chain branch.In this article, long-chain branch is defined as chain length and is at least about 6 carbon atoms, and when being higher than this value, this chain length can not adopt the technology identification of carbon NMR spectrum.This long-chain branch can reach the only about half of of this main polymer chain length.
The polydispersity index of this substantial linear olefin copolymer (be molecular weight distribution, or the ratio (M of weight-average molecular weight and number-average molecular weight
w/ M
n)) less than 3.5, preferred 1.5-2.5.Melt flow index is than (promptly pressing the I that ASTMD-1238 measures
10/ I
2) be at least 5.63, preferably be at least 6, more preferably be at least 7, and irrelevant with polydispersity index basically, this conventional polyolefine relevant with its polydispersity index with melt flow index is different.This specific character is described in Fig. 2 of above-mentioned United States Patent (USP) 5,272,236.The preparation of substantial linear olefin copolymer has detailed description in ' 236 patents.
The density of substantial linear olefin copolymer is generally 0.85-0.96, and is preferably 0.85-0.89, more preferably 0.86-0.88g/mL.
This first base material can be chosen wantonly and contain other conventional additives for example thermo-stabilizer, Weather-stable agent, static inhibitor, nucleator, filler, pigment, dyestuff, fire retardant and release agent.This first base material also can comprise having similarly or remarkable different weight average (or number average, the mixtures of some substantial linear olefin polymers of molecular weight thus).Therefore, though the substantial linear olefin copolymer has the polydispersity index less than 3.5, the polydispersity index of first base material (and bind enhancer) is not so limited.
Be superimposed upon bind enhancer on first base material comprise polar group functionalized second kind of substantial linear olefin copolymer or polar group functionalized ethene and the multipolymer of ' 992 polymkeric substance.The polar group that preferably this its content is enough to promote binder performance with any suitable method comprise methods known in the art graft to preformed second kind of substantial linear polyolefine or ' 992 polymkeric substance on.Also can introduce this polar group by the suitable monomer copolymerization that will contain required polar group.The example of suitable polar group comprises halogen particularly chlorine and bromine, hydroxyl, carboxyl, carbonyl, phosphono, acid anhydrides, amino, epoxy group(ing), sulfydryl, sulfuric ester, sulphonate, amide group and ester group.Wherein, carboxyl and the anhydride group that is grafted on the preformed polyolefine is preferred.Can connect skill on preformed polymkeric substance unsaturated carboxylic acid and the example of anhydride compound comprise toxilic acid, fumaric acid, methylene-succinic acid, vinylformic acid, methacrylic acid, Ba Dousuan, maleic anhydride and itaconic anhydride.For second kind of substantial linear olefin copolymer, maleic anhydride is the compound that preferably plays the grafting effect.
Preferably polar group is grafted on be in its preliminary shaping state and do not have basically polar group second kind of substantial linear olefin copolymer or ' 992 polymkeric substance on.Term used herein " do not have basically " to refer to such substantial linear olefin copolymer or ' 992 polymkeric substance: in the weight of preformed polymkeric substance contain less than 10% (weight), preferably less than 5% (weight), be more preferably less than 1% (weight), most preferably less than the polar group of 0.1% (weight).First kind of substantial linear olefin copolymer preferably also is the multipolymer that does not have polar group basically.
Second kind of substantial linear olefin copolymer or ' bonding that the content of grafted functional group in 992 polymkeric substance is enough to promote first base material, and in second kind of substantial linear olefin copolymer or ' weight of 992 polymkeric substance, be preferably 0.05-15%, more preferably 0.5-10%, most preferably be 1-5% (weight).
This bind enhancer preferably include grafting second kind of substantial linear olefin copolymer or grafting ' 992 polymkeric substance and a kind of mixture by following component deutero-multipolymer: a) C
2-C
20Alkene, preferred C
2-C
4Alkene, more preferably ethene; And b) unsaturated carboxylic acid or acid anhydrides, preferred toxilic acid, fumaric acid, methylene-succinic acid, vinylformic acid, methacrylic acid, Ba Dousuan, maleic anhydride or itaconic anhydride, more preferably acrylic or methacrylic acid.
Preferably with grafting second kind of substantial linear olefin copolymer or grafting ' 992 polymkeric substance and by C
2-C
20Total restatement of alkene and unsaturated carboxylic acid or acid anhydrides deutero-multipolymer, grafting second kind of substantial linear olefin copolymer comprise the 10-90% (weight) of this bind enhancer, more preferably 20-80% (weight), 40-60% (weight) most preferably.
This laminate can be processed (promptly this bind enhancer can promote bonding) under the temperature that is lower than the first base material fusing point.Preferred this laminate 20 ℃-100 ℃, more preferably 20 ℃-60 ℃, most preferably under 20 ℃-40 ℃ temperature, process.
Can be at high temperature, preferably under 100 ℃-160 ℃, mix with this bind enhancer and tackifying resin, so that between first kind and second base material, form the hot melt glued layer.This tackifying resin is compatible with bind enhancer, and normally aliphatic resin, polyterpene resin, hydrogenation resin or blended aliphatic series aromatic resin.The example of tackifying resin comprise those can by trade(brand)name ESCOREZ (ExxonChemical Co.), PICCOTAC, PICCOVAR, PICCOLYTE (Hercules, Inc.), the resin bought of WINGTAC (Goodyear) and ZONARES (Arizona).
Perhaps, laminate of the present invention can comprise any suitable be superimposed upon on this bind enhancer or with its blended tackiness agent.This tackiness agent can be for example purified or solvent based, or single part or double.The example of suitable tackiness agent includes but not limited to Resins, epoxy, urethane, latex, acrylate, elastomerics-molten stick, natural gum and organosilicon polymer.
Can with a kind of be dissolved in The suitable solvent for example the polyisocyanate compounds or the prepolymer of mono chloro benzene or ethyl acetate be used for promoting solvent based bonding, this polyisocyanate compounds or prepolymer be preferred two-or triisocyanate compound or prepolymer for example three (4-isocyanato-phenyl) thiophosphatephosphorothioate, tolylene diisocyanate, methylene radical two-to phenylene isocyanic ester or its polyether polyols with reduced unsaturation.For example, this polyisocyanate compounds can be coated on the bind enhancer layer; Prepare with this bind enhancer, be coated to then on first base material; Or prepare with solvent-based adhesive, be coated to then on the bind enhancer layer.
The consumption of this polyisocyanate compounds or prepolymer is enough to promote the bonding between solvent-based adhesive and the bind enhancer, and preferably its consumption accounts for the 0.1-25% of bind enhancer weight, more preferably 0.5-10%, and 1-5% (weight) most preferably.
The example of commercially available polyisocyanate compounds or prepolymer comprises DESMODUR
TMRF-E (trade mark of Miles Inc.), PAPI
TMPolymeric MDI (trade mark of The Dow ChemicalCompany) and UPACO 3570 (Worthen Industries, UPACO Division produces).
It also is favourable that isocyanate compound or precursor use in the presence of catalyzer.Suitable catalyzer comprises divalence or tetravalence organotin catalysts for example two lauric acid tin methides, dicarboxylic acid tin methide, two mercaptan tin methide and stannous octoates; Or amines catalyst.
Laminate of the present invention also comprises glued second base material on first base material.This second base material can be for example leather, metal, plastics, rubber, glass, timber or a concrete of any suitable material.
Laminate of the present invention can be used for various end-uses, comprises the windshield glass of bathroom squamous pad (scale), sole, carpet backing and automobile.
Following examples only are never to mean for explanation to limit the scope of the present invention.The preparation of embodiment 1-polyolefin elastomer/leather laminated product and T-tear strength
By 50 grams being had melt flow index is that 0.3 gram/10 minutes and density are the maleic anhydride grafted ethene-1-octene copolymer and the PICCOVAR of 0.87 grams per milliliter
AP-10 tackifying resin (50 grams, Hercules, the trade mark of Inc.) is mixed together under 150 ℃ until uniform preparation hot melt adhesive agent formulation.With ESCOREZ
5300 tackifying resins (75 gram, the trade mark of Exxon Chemical Company) under agitation add in this mixture till evenly.This hot melt adhesive agent formulation is coated in ENGAGE
Being with of 8200 polyolefin elastomers (trade mark of The Dow Chemical Company).Adopt 7.6 centimetres overlap joint and 760 microns bonding thickness, the sole mixture is overlapped preheating (150 ℃) snag the leather band on, preparation is used for the laminate that T-tears test.This sole band is of a size of 15.2cm * 2.5cm * 0.32cm, and the leather band is 10cm * 2.5cm * 0.095cm.Tackiness agent was solidified 30 minutes.Excess binder around the tack coat is removed, before the test each bonding piece is adapted to 2 hours under probe temperature.According to ASTM methodD1876-72,, adopt INSTRON with the lateral velocity of 25.4 cm per minute
Tensile 4204Testing System measures, and recording the T-tear strength is 34pli.Embodiment 2-is used for the room-temperature curing epoxy type tackiness agent of the metal laminate product that ethene-1-octene copolymer/E-applied
With toluene (30.0 gram), tetrachloroethylene (6.0 gram), the trimethyl carbinol (6.0 gram), to have melt flow index be that 0.3 gram/10 minutes and density are the maleic anhydride grafted ethene-1-octene copolymer (0.34 gram) and the PRIMACOR of 0.87 grams per milliliter
3460 mixed polymers (0.5 gram, the trade mark of The DowChemical Company) mix and are heated to 80 ℃ till forming uniform solution in beaker.This bind enhancer mixture is cooled to 25 ℃, then, with it at ENGAGE
TMApply thin film on 8200 ethene-1-octene copolymer band, and be allowed to condition at 25 ℃ of following dryings 24 hours.With 12.5 gram D.E.R.
331 Resins, epoxy (trade mark of The Dow Chemical Company), 25.0 gram ANCAREZ
TM2364X properties-correcting agent (Air Products and Chemicals, the trade mark of Inc.) and 10.0 gram ANCAMINE
TMThe uniform mixture of 2384X solidifying agent (Air Products and Chemicals, the trade mark of Inc.) is coated to being with of this existing first coating, then the 0.75-mL diameter glass beads is sprayed at this and is with control thickness.The metal that then E-has been applied and ethene-1-octene copolymer be by the overlap joint amalgamation of 7.6-cm, and with this tackiness agent 25 ℃ of following solidify overnight.The T-tear strength is 40pli.Embodiment 3-is used for the room-temperature curing epoxy type tackiness agent of the metal laminate product that ethene-1-octene copolymer/E-applied
Except this bind enhancer is to be blended in the gram of 0.67 in toluene/tetrachloroethylene/t-butanol solvent mixture maleic anhydride grafted ethene-1-octene copolymer and 0.17 gram PRIMACOR
Beyond 3460 mixed polymers, repeat the step of embodiment 2.The T-tear strength is 32pil.Embodiment 4-is used for the room-temperature curing epoxy type tackiness agent of the metal laminate product that ethene-1-octene copolymer/E-applied
Except this bind enhancer is to be blended in the gram of 0.17 in toluene/tetrachloroethylene/t-butanol solvent mixture maleic anhydride grafted ethene-1-octene copolymer and 0.67 gram PRIMACOR
Beyond 3460 mixed polymers, repeat the step of embodiment 2.The T-tear strength is 38pli.
Claims (10)
1. laminate, this product comprises:
A) comprise first base material of first kind of substantial linear olefin copolymer;
B) be superimposed upon bind enhancer on this first base material, this bind enhancer comprise polar group functionalized second kind of substantial linear olefin copolymer;
C) with this bind enhancer blended tackifying resin, or be superimposed upon on this bind enhancer or with its blended tackiness agent; With
D) glued second base material on this first base material; Wherein this first kind and second kind of elastic olefin polymer are characterised in that to have:
I) weight-average molecular weight and the ratio of number-average molecular weight are less than 3.5;
Ii) I
10/ I
2Be not less than 6; With
Critical shear speed ratio when iii) surperficial melt fracture begins has about same melt exponential sum M
w/ M
nThe surperficial melt fracture of the polymer of linear olefin critical shear speed big at least 50% when beginning; The feature of every kind of olefin polymer also is to be ethene and C
3-C
20The multipolymer of alpha-olefin.
2. the laminate of claim 1, wherein this bind enhancer also comprises by C
2-C
20Alkene and ethylenically unsaturated carboxylic acids or acid anhydrides deutero-multipolymer.
3. the laminate of claim 2, wherein the multipolymer of this alkene and ethylenically unsaturated carboxylic acids is the multipolymer of ethene and vinylformic acid or ethene and methacrylic acid.
4. each laminate among the claim 1-3, wherein every kind of multipolymer that the substantial linear olefin copolymer independently is ethene and 1-butylene, 4-methyl-1-pentene, 1-hexene or 1-octene.
5. each laminate among the claim 1-4, wherein every kind of substantial linear olefin copolymer is to have the ethene that density is 0.86-0.88g/mL and the multipolymer of 1-octene.
6. each laminate among the claim 1-5, second kind of substantial linear olefin copolymer that wherein polar group is functionalized comprises anhydride group or the hydroxy-acid group that is grafted on the ethene-1-octene copolymer that is in its preliminary shaping state and does not have polar group basically, the polymkeric substance that wherein this polar group is functionalized is in the weight of preformed ethene-1-octene copolymer, comprise the maleic anhydride on the preformed ethene of being grafted on of 0.05-10% (weight)-1-octene copolymer, and wherein the maleic anhydride grafting the ratio of ethene-1-octene copolymer and the multipolymer of ethene and vinylformic acid or ethene and methacrylic acid be 20: 80 to 80: 20.
7. each laminate among the claim 1-6, wherein the solvent-based adhesive preparation is superimposed upon on this bind enhancer or with it and mixes, and wherein this bind enhancer or solvent-based adhesive also comprise isocyanate compound or isocyanate prepolymer.
8. each laminate among the claim 1-9, wherein second base material comprises metal, glass, timber, cement, plastics, rubber or leather.
9. bind enhancer, this bind enhancer comprises the mixture of following component:
A) by C
2-C
20Alkene and ethylenically unsaturated carboxylic acids or acid anhydrides deutero-multipolymer and
B) the substantial linear olefin copolymer that polar group is functionalized, this multipolymer has:
I) M
w/ M
nLess than 3.5;
Ii) I
10/ I
2Be not less than 6; With
Critical shear speed ratio when iii) surperficial melt fracture begins has about same melt exponential sum M
w/ M
nThe surperficial melt fracture of the polymer of linear olefin critical shear speed big at least 50% when beginning; The feature of every kind of olefin polymer also is to be ethene and C
3-C
20The multipolymer of alpha-olefin; Or
C) olefin copolymer that polar group is functionalized, this multipolymer has narrow molecular weight distributions; Comonomer unit is along this main polymer chain stochastic distribution, and evenness index is at least 75.
10. bind enhancer, this bind enhancer comprises the mixture of following component:
A) a kind of C
2-C
20The multipolymer of alkene and ethylenically unsaturated carboxylic acids or acid anhydrides and
B) the substantial linear olefin copolymer that polar group is functionalized, this multipolymer has:
I) M
w/ M
nLess than 3.5;
Ii) I
10/ I
2Be not less than 6; With
Critical shear speed ratio when iii) surperficial melt fracture begins has about same melt exponential sum M
w/ M
nThe surperficial melt fracture of the polymer of linear olefin critical shear speed big at least 50% when beginning; The feature of every kind of olefin polymer also is to be ethene and C
3-C
20The multipolymer of alpha-olefin, wherein C
2-C
20The multipolymer of alkene and ethylenically unsaturated carboxylic acids comprises the multipolymer of ethene and acrylic or methacrylic acid, and the substantial linear olefin copolymer that polar group is functionalized comprises being grafted on and is in its preliminary shaping state, do not have a polar group and have maleic anhydride on the ethene that density is 0.86-0.88g/mL-1-octene copolymer basically, and wherein the maleic anhydride grafting the ratio of ethene-1-octene copolymer and the multipolymer of ethene and vinylformic acid or ethene and methacrylic acid be 20: 80 to 80: 20.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN96196579A CN1193937A (en) | 1995-08-28 | 1996-07-26 | Bind enhancer for linear polyolefins |
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US08/510,149 | 1995-08-28 | ||
| CN96196579A CN1193937A (en) | 1995-08-28 | 1996-07-26 | Bind enhancer for linear polyolefins |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN1193937A true CN1193937A (en) | 1998-09-23 |
Family
ID=5129108
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN96196579A Pending CN1193937A (en) | 1995-08-28 | 1996-07-26 | Bind enhancer for linear polyolefins |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN1193937A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101932438A (en) * | 2007-09-03 | 2010-12-29 | 陶氏环球技术公司 | The method that contains the substrate and the described substrate of preparation of polymeric layer |
-
1996
- 1996-07-26 CN CN96196579A patent/CN1193937A/en active Pending
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101932438A (en) * | 2007-09-03 | 2010-12-29 | 陶氏环球技术公司 | The method that contains the substrate and the described substrate of preparation of polymeric layer |
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