Thermoplastic composition

 

(57) Abstract:

Use: in the manufacture of thermoplastic compositions. The inventive composition comprising 20-50 wt.%. the grafted copolymer of ethylene-propylene-diene rubber and 50 to 80 wt.%. the grafted copolymer polypropylene, the ethylene-propylene-diene rubber grafted 13-40% wt. a mixture of styrene and Acrylonitrile or styrene and/or methyl methacrylate, and a copolymer of polypropylene containing grafted mixture of styrene and Acrylonitrile or styrene and/or methyl methacrylate in the amount of 45-46% wt. table 4.

The present invention relates to compositions comprising a graft copolymer of propylene polymer material with a graft-copolymer of olefinic rubber material, where the grafted monomers are (I) aromatic vinyl compounds, (II) acrylic compound, (III) a mixture of compounds (I) and (II) or (IV) other monomers, copolymerizate at least one compound (I) at least one compound (II) or mixtures of at least one compound (I) and at least one compound (II).

Typically, the graft copolymers of olefinic polymeric materials modified with the aim of increasing the impact strength of the ethylene-example, in the description to the us patent N 3314904 suggested getting a "rubber plastic by first obtaining the graft-copolymer by grafting of styrene on polyethylene or polypropylene, in particular graft-copolymer of styrene, Acrylonitrile, and polyethylene or polypropylene, with subsequent mixing of this graft-copolymer with certain selected compatible rubber chemicals-like materials. The content of grafted styrene or styrene/Acrylonitrile component in the graft-copolymer is 75-95% preferably 85-95%, more preferably 90-95% Thus, the graft-copolymer is a predominantly linked styrene or linked styrene/Acrylonitrile in the graft-copolymers derived from polypropylene, the polypropylene component is only a minor component and is present as dispersed phase. Thus, dominated by the properties of the bound styrene or styrene/Acrylonitrile. The graft-copolymer get subjecting the polyolefin ionization irradiation of high energy followed by the introduction of irradiated polyolefin in contact with styrene or styrene and Acrylonitrile.

In the description to the us patent N 4537933 offers a mixture of the polyolefin glimmer is a copolymer of styrene with Acrylonitrile (CAH), modified acrylate polymer, chlorinated polyethylene or polymer-modified olefin-diolefin, in particular ethylene-profilepoliticians polymer. The content of the styrene/Acrylonitrile component in AsA polymer, a modified olefin-ioleinplaceframe polymer is 60-95% Properties CAH-component dominates, because the rubber is contained as only a minor component and is present in the dispersed phase. In addition, the matrix phase polymer components must have qualities.

The closest analogue of the present invention is U.S. patent N 4916186, C 08 L 51/04, 10.04.90, which describes thermoplastic mixture, which consists of two graft-copolymer constituting the copolymers of styrene and Acrylonitrile grafted to the ethylene/propylene rubber ERDM and polybutadiene rubber.

It was found that by functionalization of olefinic rubber materials and mixing the specified functionalized olefinic rubber graft copolymer of propylene polymer material, where the links of the polymerizable (co)monomers used for functionalization of rubber and its grafting on polypropylene by what about the seam, impact resistance and rigidity while maintaining the balance of other independent engineering plastics for injection molding products and the manufacture of extruded profiled materials.

In accordance with this invention features a thermoplastic composition comprising the graft copolymer of vinyl-based monomer, characterized in that the graft-copolymer ethylene-propylene-diene rubber contains ethylene-propylene-diene rubber grafted 13-40% wt. a mixture of styrene and Acrylonitrile or styrene and/or methyl methacrylate, as well as graft-copolymer of vinyl-based monomer contains polypropylene, grafted 45-46% wt. a mixture of styrene and Acrylonitrile or styrene and/or methyl methacrylate in the following ratio, wt;

grafted ethylene-propylene-diene rubber 20-50

grafted polypropylene 50-80

The material of the propylene polymer base can be either (I) a homopolymer of propylene, (II) statistical copolymer of propylene and olefin selected from the class of ethylene and alpha-olefins of C4-C10provided that when the olefin is ethylene, the maximum content of polymerized ethylene comp/SUB>-C10the maximum content of the polymerized component is approximately 20% preferably about 16%, or (III) statistical ternary copolymer of propylene with two alpha-olefins selected from a class which includes ethylene and alpha-olefins, C4-C8provided that the maximum content of polymerized alpha-olefin (C4-C8component is approximately 20% preferably about 16% and in that case, when ethylene is one of these alpha-olefins, the maximum content of polymerized ethylene component is approximately 5% preferably about 4% Class of alpha-olefins of C4-C10covers linear and branched alpha-olefins, C4-C10in particular 1-butene,1-penten, 4-methylpentene-1,3-methyl-1-butene, 1-hexene, 3,4-dimethyl-1-butene, 1-hepten, 3-methyl-1-hexene, and the like.

Preferred bases propylene polymer material is polypropylene and ethylene-propylene statistical copolymer.

Olefinic rubber base can be either (I) ethylene-propylene copolymer rubber (EPA), the content of the ethylene component in which is from 30 to 70% (III) copolymer rubber, propylene and butene-1 (NBC), the content of the component butene-1 which comprises from 30 to 70% (IV) rubber of ethylene, propylene and a non-conjugate diene monomer (EPDM), ethylene content of the component which is 30 to 70% and the content of the diene from 1 to 10% (V) a propylene-butenova terpolymeric rubber (APBC), the content of the propylene component, which ranges from 1 to 10% and butenova component from 30 to 70%, or the content of the propylene component is from 30 to 70% and butenova component from 1 to 10% (VI) a homopolymer of propylene, modified to improve the impact resistance of 10-80% ethylene-propylene copolymer rubber, ethylene-butenova copolymer rubber, rubber of ethylene, propylene and a non-conjugate diene monomer and/or ethylene-propylene-butenova terpolymer rubber, (VII) statistical copolymer of propylene and olefin selected from the class of ethylene and alpha-olefins of C4-C10modified to improve the impact resistance of 10-80% of the product (I), (II), (III), (IV) and/or (V). The product (VI) and (VII) the content of the ethylene component is from 30 to 70% and diene component, if present, from 2 to 8% and in the case when the use of industrial safety examinations-terpolymer, the content of the propylene component is from 1 to 10% if ad% if the content butenova component is from 1 to 10% examples of non-conjugate dienes include 1,4-hexadiene, ethyldiethanolamine and Dicyclopentadiene. Class alpha-olefins comprises linear and branched alpha-olefins, C4-C10in particular 1-butene, 1-penten, 4-methylpentene-1,3-methyl-1-butene and 1-hexane. Preferred are rubber of ethylene, propylene and a non-conjugate diene monomer and ethylene-propylene rubber, modified to improve the impact resistance of polypropylene.

The monomer or monomers to be grafted on the main propylene polymer material and the primary olefin rubber component may represent (I) aromatic vinyl compounds selected from styrene, styrene with alkilany or alkoxysubstituted in the ring, where the alkyl or alkoxygroup represents a linear or branched alkyl or alkoxyalkyl C1C4their mixtures, where the styrene content with alkilany or alkoxysubstituted in the ring is from 5 to 95%, or mixtures of styrene containing ring alkyl or alkoxylation, with 5-40% of alpha-methylstyrene and alpha methylstyrene derived; (II) acrylic compound selected from methyl methacrylate, ethyl methacrylate, benzylmethylamine, fenilsalicilata or alkoxy-substituted (C1-C4) felinely or branched alkylacrylate, containing from 1 to 10 carbon atoms, acrylic acid, methacrylic acid, glycidylmethacrylate, glycidylmethacrylate, Acrylonitrile or Methacrylonitrile, together with at least one product (I) or at least one product (II) or mixtures of at least one product (I) and at least one product (II), where the content of the above other copolymerizes monomer is up to 50% preferably from 1 to 30%

Preferred grafted monomers are styrene, methyl methacrylate, styrene-Acrylonitrile, styrene-methyl methacrylate, methyl methacrylate-Acrylonitrile, methyl methacrylate-Methacrylonitrile, styrene-methyl-methacrylate-Methacrylonitrile and styrene-methyl methacrylate-Acrylonitrile.

To an acceptable bulk forms grafted propylene polymer material includes powder, flakes, granules, spheres, cubes, and the like. Preferred are materials in the form of spherical particles prepared from a propylene polymer material with a share of pore volume of at least approximately 0,07.

Most preferred for the preparation of grafted propylene polymer material is a propylene polymer material (the second least 0.1 square meters/g and (3) with volume fraction of pores of at least about 0.07 to, with a diameter of more than 40% of the pores in the particle must exceed 1 micron. Such propylene polymer materials are produced on an industrial scale company "Himont Italia S. R. L".

The grafted propylene polymer material and olefin rubber material of the present invention receive a free radical graft-polymerization of at least one monomer, which is defined above, in place of the free radical with propylene polymer material and olefin rubber material. Free radical sites can be created by irradiation or by using a material forming free radicals by chemical means, for example by reaction with an appropriate organic peroxide.

In accordance with the method of creating parcels of free radicals by irradiating the propylene polymer material, preferably in the form of particles, is subjected to irradiation at a temperature in the range from about 10 to 85oC using ionization radiation high energy, resulting in the propylene polymer material there are free sites. Then the irradiated propylene polymer material contained in virtually noncorrosive of Atmosfera time of at least about 3 minutes with about 5 to 80% specific grafted monomer or monomers, calculated on the total weight of propylene polymer material and grafted monomer or monomers. After exposure propylene polymer material in terms of the effects of the monomer during the selected period of time, simultaneously or sequentially (in any selected order) obtained grafted propylene polymer material is still almost non-oxidizing atmosphere is treated with the aim of decontamination of almost all the remaining free radicals, and then from the above-mentioned material remove all unreacted grafted monomer.

The deactivation of free radicals in the obtained graft-copolymer is preferable to carry out heating, although it can be done by using additives, such as methylmercaptan, which serves as a trap for free radicals. Usually the temperature of the decontamination must be at least 110oC, preferably at least 120oC. Typically, the extract at a temperature of decontamination for at least 20 minutes is sufficient.

Any unreacted grafted monomer is removed from the graphite-copolymer, either before or after decontamination radicals, or simultaneously with decontamination. In that case, when the delete operation performed before or simultaneously with decontamination,free radicals are created with the help of organic chemical compounds, it is an organic chemical compound, preferably an organic peroxide, is an initiator of free radical polymerization, the half-life is approximately from 1 to 240 minutes at a temperature, which is supported in the process. Class acceptable organic peroxides covers allperks, in particular benzoyl peroxide and Dibenzoyl; dialkyl - and aralkylamines, in particular di-tert. butylperoxide, dicumylperoxide, peroxide kanelbulle, 1,1-dicret, butyl peroxy-3,5,5-trimethylcyclohexane, 2,5-dimethyl-2,5-dicret, butylperoxide and bis-/alpha-tert. -butylperoxyisopropyl); peroxide esters, in particular tert.butyl peroxypivalate, tert. butylperbenzoate, 2.5-dimethylhexane-2,5-di-(perbenzoate), tert.butylphthalate, tert, butyl peroxy-2-ethylhexanoate; 1,1-dimethyl-3-hydroxy-butyl peroxy-2-ethylhexanoate; peroxocarbonate, in particular di(2-ethylhexyl) PEROXYDICARBONATE, di-(n-propyl)- PEROXYDICARBONATE di-/4-tert.butylcyclohexyl/-PEROXYDICARBONATE. These peroxides can be used in concentrated form or in the environment of diluent concentration activitiesthese substances from 0.1 to 6.0 hours/100 hours preferably from 0.2 to 3.0 hours/100 hours

In coemperor from about 60 to 125oC process the initiator of free radical polymerization, which is described above, in the amount of from 0.1 to 6.0 hours/100 hours Polymeric material is treated with from about 5 to 240 hours/100 hours grafted monomer at a speed of add, which does not exceed 4.5 hours/100h./min when the total amount of added substance is from 5 to 240 hours/100 hours monomer during the time period that coincides with or follows the processing time by the initiator. In other words, the monomer and initiator can be added to the heated propylene polymer material simultaneously or the monomer can be added: 1) when the operation is complete addition of the initiator; 2) after the start of addition of the initiator, but before the append operation has completed; 3) after a certain cooling-off period after the completion of addition of the initiator.

After inoculation on propylene polymer material, the resulting grafted propylene polymer material, which is still almost non-oxidizing atmosphere, is treated, preferably aged at a high temperature component of at least 120oC for at least 20 min, with the aim of destruction of all unreacted initiator and dehdasht from the specified material either before or after deactivation of radicals, either simultaneously with this decontamination.

The graft-copolymer of propylene polymer material is contained in an amount of from 40 to 90% preferably from 45 to 80%, the most preferably from 50 to 70% of the total amount of the composition. The grafted propylene polymer material contains from 5 to 70% monomer, graft or graft-polymerized with him, preferably from 25 to 55%

The graft-copolymer of olefinic rubber material is contained in an amount of from 10 to 60% preferably from 20 to 55% and most preferably from 30 to 50%, calculated on the total amount of the composition. Grafted olefinic material contains from 5 to 50% monomer, graft or graft-polymerized with him, preferably from 10 to 45%

Such a composition may include about 80 hours (in total) additives, including fillers, reinforcing agents and the like, for every 100 hours graft-copolymer and a rubber component. Additionally, this composition may contain from about 5 to 30 p.m. propylene polymer material for every 100 hours graft-copolymer and a rubber component, where appropriate propylene polymer materials presented in this description in the polymer.

Compositions of the present invention is prepared by mechanical mixing of the components in conventional mixing equipment, i.e. in a single screw or twin screw extruder, a Bunbury mixer, or any other conventional device for mixing in the melt. The order in which the mixed components of the composition, not decisive.

The essence of the present invention is illustrated in more detail with reference to examples of its implementation, which is shown below.

Examples 1-3, 5-7, 8-10 and 12-14.

Compositions of the present invention are prepared in accordance with the normal procedure, which provides for the mixing drum graft-copolymer of polypropylene and a graft-copolymer of olefinic rubber, as shown in table. 1, prior to the formation of a homogeneous mixture (for about 1 min). This mixture was loaded into a cold Bunbury mixer, were mixed to liquefy for about 3 to 5 min, and then were crushed. Powdered mixture was extrudible at a temperature of 520oF (271oC) with a rotation speed of 150 rpm./min in a twin-screw with protivovirusnym extruder preemptive actions with augers located in sawalani, and vacuum on the machine Battenfeld 1.5 oz (42.5 g) with a working pressure of 25 tons at a temperature of cylinder 450oF (232oC) and the temperature of the forming tool 140oF (60oC). Injection molding cycle for production of standard samples for testing tensile and bending strength included an injection time of 10 seconds, a cooling time of 20 seconds and time of opening of the form 2 seconds with a maximum speed of injection (setting 15) and setting the speed of rotation of the screw 2.

Compositions for experiments of comparative examples 4, 8, 11 and 15 were prepared similarly to the foregoing data for examples.

The physical properties shown in the tables were determined in accordance with the following methods.

The ultimate tensile strength ASTM d-638 (at speed through the guide head 2 inches/min (50.8 mm/min) without extensometer).

Elongation at break ASTM d 638

Wdline when the yield strength ASTM d-638

The modulus of elasticity in bending ASTM d-790 and D-618, procedure A (at speed through the guide cylinder, 0.5 inch/min (12.7 mm/min) and the Central section being formed T-shaped pattern)

Flexural strength ASTM d-638, procedure A (Central section of the T-shaped pattern)

Impact strength Izod specimen with notch ASTM d-256-87

The weld strength ASTM d-638

Composition, providentiality table. 1, except that in this case, instead of polypropylene grafted with styrene used a polypropylene grafted with methyl methacrylate, and instead of polypropylene modified with ethylene-propylene rubbers with graft-styrene used polypropylene, modified ethylene-propylene rubber grafted with methyl methacrylate.

Compositions are given in table. III, were prepared in accordance with the usual procedure, which was carried out in the preparation of compositions of table. 1, except that in this case, instead of polypropylene grafted with styrene and polypropylene modified with ethylene-propylene rubber grafted with styrene, used a polypropylene grafted styrene-Acrylonitrile component and polypropylene modified with ethylene-propylene rubber grafted with styrene-Acrylonitrile component.

The compositions listed in table IV were prepared in accordance with the usual procedure, which was carried out in the preparation of compositions of table. 1, except that in this case, instead of polypropylene modified with ethylene-propylene rubber grafted with styrene, used the product Royaltuf 160, ethylene-probita and variants of the embodiment of the present invention, which of the above, it is obvious for any person skilled in the art from the above description. In this regard, it should be stated that, although the specific variants of the embodiment of the present invention is described with many details on these options and their modifications you can make any changes without departing from the scope of the present invention, which is defined above description and the appended claims.

Thermoplastic composition comprising a grafted copolymer of ethylene-propylene-diene rubber grafted copolymer of vinyl-based monomer, characterized in that the grafted copolymer of ethylene-propylene-diene rubber, it contains ethylenepropylene rubber, grafted 13 40 wt. a mixture of styrene and Acrylonitrile or styrene and/or methyl methacrylate, as well as grafted copolymer of vinyl-based monomer contains polypropylene, grafted 45 46 wt. a mixture of styrene and Acrylonitrile or styrene and/or methyl methacrylate, in the following ratio, wt.

Grafted ethylenepropylene rubber 20 50

Grafted polypropylene 50 R

 

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< / BR>
where a 98,0-to 98.4 mol

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20 cl, 4 tbl, 4 ex

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15 cl, 2 tbl

FIELD: chemistry.

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13 cl, 2 tbl, 4 ex

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8 cl, 1 tbl, 4 ex

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12 cl, 8 tbl, 20 ex

FIELD: chemistry.

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16 cl, 4 tbl

FIELD: chemistry.

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13 cl, 4 tbl, 3 ex

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