SK280664B6 - Modified elastomeric polypropylenes, their use, and blends with their content - Google Patents

Abstract

Elastomeric polypropylenes and blends thereof with isotactic polypropylenes with essentially a stereoregular block arrangement in the chain structure are modified with graft monomers selected from the group containing ethylenically unsaturated aliphatic or aromatic carboxylic acids or derivatives thereof in the amount ranging from 0.1 to 30 wt.%. The use of modified polypropylenes as additives for improving compatibility by adding thereof into blends. Blends of polyolefins and nonolefinic thermoplastics containing such polypropylenes.

Description

Technical field

The invention relates to modified elastomeric polypropylenes, mixtures thereof with isotactic polypropylenes, modified inoculations, as well as their use as additives for improving compatibility or stickiness.

BACKGROUND OF THE INVENTION

For example, it is known from EP-A-280,454, EP-A-317,358, WO 91/5008, US 3,868,433, US 4,260,690, DE-A-41 31 908 that isotactic polypropylenes (IPPs) can be chemically modified by seeding monomers such as styrene, maleic anhydride (MSA), acrylic acid and derivatives thereof. These inoculation reactions produce inoculation copolymers of polypropylene, which have a higher polarity compared to the starting polypropylene. These products find use, for example, as additives for improving the adhesion of polyolefins, such as polyethylene, polypropylene PP and polypropylene copolymers, or as additives for improving compatibility in polyolefin-miscible polyolefins, such as polyamides, polyesters, polycarbonates, polystyrene, polystyrene, polystyrene, polystyrene, polystyrene polyacrylates and polyurethanes. In both fields of application, the additive to improve adhesion or compatibility is located in the interlayer between the polyolefin and the metal or the mixed partner, and by chemical and / or physical coupling (e.g., recrystallization) causes the adhesion of the materials. In the case of mixtures of PP with other thermoplastics, for example polyamide 6 (PA6), the phase boundary layer structure significantly determines mechanical properties such as impact strength, strength and stiffness (modulus of elasticity). For example, the PP / PA6 mixture, which contains an additive to improve compatibility based on sterol-ethylene / butylene-styrene triblock copolymers (SEBS), inoculated with MSA, has a relatively high toughness (impact toughness, Fallbolzentest). Mixtures of PP and PA6 have similar properties using ethylene propylene rubber (EPR) inoculated with MSA as an additive to improve compatibility. Said additives for improving compatibility, such as those of the SEBS type, however, have the disadvantage of a complex and expensive synthesis, since the copolymerization takes place in solution and subsequent seeding with functional monomers is required.

The grafted ethylene propylene rubber has the disadvantage of poor pourability, since the grafting in EPR is accompanied by a partial crosslinking of the ethylene moiety. The same applies to EPDM grafted ethylene propylene diene rubber. In particular, additives for improving compatibility or adhesion based on isotactic polypropylenes have the disadvantage that in many fields of application of thermoplastics, such as in the manufacture of cars, tools and instruments, the mechanical properties of the mixtures used, in particular toughness, are insufficient.

For these reasons, it has been necessary to find substances which act as additives for improving the compatibility or adhesion to polyolefins and which cause improved mechanical properties, in particular higher toughness or lower brittleness, especially in mixtures of polyolefins with neolefin thermoplastics.

SUMMARY OF THE INVENTION

According to the invention, the problem is solved by using grafted copolymers of elastomeric polypropylene (ELPP) or mixtures thereof with grafted polymers of isotactic polypropylenes (IPP) as additives to improve compatibility or adhesion.

Accordingly, the present invention provides elastomeric polypropylenes (ELPPs) modified with ethylenically unsaturated seed monomers, and mixtures thereof with isotactic polypropylenes (IPPs) with a stereoregulated block structure in the chain structure, modified with ethylenically unsaturated seed monomers.

The elastic polypropylenes used for the inoculation reactions are in particular those described in US 4,335,225, US 4,522,982 and US 5,188,768. This includes both homopolymers and copolymers. They have a substantially stereospecific block arrangement of the structural chain and consist, for example, of blocks of isotactic and atactic propylene sequences that are alternately arranged on the polymer chain. It is also possible to insert additional comonomers into the polymer chain. The copolymers may contain other olefin units, such as ethylene, butene, pentene or hexene units, in addition to the propylene units in the molecule. They are prepared, for example, according to US 4,335,225 by polymerization with special catalysts which are prepared by reacting or mixing organic compounds Ti, Zr or Hf with a metal oxide, such as AtyO3, T1O2, S1O2 or MgO. In addition, elastic polyropylenes used for degradation can also be prepared analogously to US 4,522,982 using metallocene catalysts in combination with aluminoxanes or analogously US 5,118,768 to catalysts based on magnesium alkoxides and titanium tetrachloride in special electron donor environments.

According to the invention, the elastic polypropylenes (ELPPs) can be inoculated alone or in admixture with other, particularly isotactic polymers (IPPs). All other known polypropylene homopolymers or copolymers with other olefins can be used as other polypropylenes. However, it is also possible to separately inoculate ELPP and IPP and mix the modified polypropylenes. The mixtures preferably consist of elastic polypropylenes containing up to 80% by weight, particularly preferably 0.5 to 50% by weight, in particular isotactic polypropylenes.

The grafted polypropylenes of the invention are polypropylenes which have one or more chemically bonded (grafted) functional groups and / or polymer chains of monomodules having one or more functional groups along the polymer chain. ELPPs and / or IPPs can therefore be vaccinated with unsaturated mono- and / or dicarboxylic acids, their anhydrides, their esters with aliphatic alcohols and dialcohols containing 1 to 10 carbon atoms, and the glycidethers, vinyl alcohol esters as well as the vinyl aromatics or mixtures of these monomers, such as also mixtures of these monomers and olefins containing 2 to 10 carbon atoms.

Particularly preferred in this connection are seed monomers of the group of ethylenically unsaturated aliphatic or aromatic carboxylic acids or derivatives thereof, of the maleic, acrylic or methacrylic acid group or derivatives thereof and of the group of vinyl aromatics. Possible derivatives are, for example, esters, anhydrides, acid halides, amides, imides or oxazolines.

Thus, for example, ELPP, IPP or mixtures of ELPP and IPP in solution or melt can be reacted by a process of free-radical graft copolymerization with acrylic acid or its derivatives such as methyl methacrylate, butyl acrylate, tert-butyl acrylate, glycidylacrylate, glycidyl methacrylate, 2-hydroxyethyl ester with acrylic acid. maleic acid and its derivatives, such as maleic anhydride (MSA), mono- and diesters of maleic acid with methanol, ethanol, butanol and hexanol to produce ELPP and / or IPP modified with acid, acid ester, hydroxyester and glycidyl ether. Preparation of graft copolymers of ELPP and IPP and derivatives of vinyl alcohols, especially esters with aliphatic carboxylic acids, such as vinyl acetate, is likewise possible. Another group consists of inoculated products with vinylaromates, for example styrene. Furthermore, the reaction of ELPP or IPP with mixtures of seed monomers of any composition, such as mixtures of different acrylic acid derivatives, mixtures of acrylic acid and maleic acid derivatives, mixtures of acrylic acid derivatives with vinyl alcohol derivatives, mixtures of both acrylic acid and maleic acid derivatives, , and / or vinyl alcohol derivatives as well as vinylaromates such as styrene and / or alpha-olefins containing 2 to 10 carbon atoms to form grafted ELPP copolymers or mixtures of grafted ELPP / IPP copolymers.

The degree of seeding, i.e. the content of seeding monomers in the grafted polypropylenes, is preferably at about 0.1 to 30 wt%, more preferably at about 0.5 to 10 wt%. and most preferably at 0.5 to 5 wt.%.

The preparation of graft copolymers according to the invention ELPP, optionally ELPP / IPP, can be carried out according to the methods of radical graft copolymerization, as described for example for IPP in EP-A-280.454, EP-A-317.358, WO 91/5008, US 3,868,433, US 4,260,690, DE -A-41 31 908, seeding ELPP or a mixture of ELPP and IPP with ethylenically unsaturated seeding polymers. The seeding reaction takes place, for example, in solution, preferably in aromatic hydrocarbons at a temperature range of from 50 to 200 ° C, preferably from 80 to 150 ° C, or in a melt, preferably in an extruder, at a temperature range of from 170 to 300 ° C, preferably from 200 to 200 ° C. 250 ° C. It is advantageous here to initiate the formation of polymers by radical initiators, such as peroxides or azo compounds and / or high energy radiation, such as gamma radiation and electron radiation.

It is a further object of the invention to use ELPPs modified according to the invention, or mixtures thereof with modified IPPs, as additives to improve the compactness and tackiness of olefins, especially in mixtures with polyolefins with non-olefin thermoplastics, or as additives to improve tackiness on polyolefin-metal joints. The grafted ELPP and / or ELPP / PP copolymers of the invention can be used as additives to improve compatibility, especially in mixtures consisting of both polyethylene, IPP or its copolymers with ethylene and other alpha-olefins as well as neolefin thermoplastics, e.g. polyamides, polyesters, polycarbonates, polystyrenes, polyacrylates and polyurethanes.

A further object of the invention are mixtures of polyolefins and neolefin thermoplastics, which contain grafted ELPP and / or ELPP / IPP copolymers as additives to improve compatibility. The compositions of the invention exhibit better mechanical properties, for example higher toughness values (Doppel-V impact, Fallbolzentest) and lower toughness values than mixtures of the same composition with inoculated IPP as an additive to improve compatibility. The compositions of the invention may further comprise conventional additives such as technological and long-term stabilizers, nucleating agents, reinforcing agents and fillers such as talc, chalk or kaolin. Thus, for example, the advantages of the compositions according to the invention comprise 2 to 50% by weight, preferably 10 to 40% by weight. % talc or 1-40 wt. reinforcing fibers such as glass fibers or carbon fibers.

The compositions of the invention contain about 0.1 to 30 wt. additives to improve compatibility. Preference is given to using 1 to 15% by weight, particularly preferably 2 to 10% by weight. additives to improve compatibility. The mixing ratio of the polyolefin to the neolefin thermoplastics extends over the total possible blend range and is about 5 to 95 wt%, preferably 30 to 80 wt%. % polyolefin and 5 to 95 wt.%, preferably 20 to 70 wt. of a neolefin thermoplastic. The mixtures are used, for example, in extrusion or compression molding to produce films or moldings.

DETAILED DESCRIPTION OF THE INVENTION

In the following, particularly advantageous combinations of additives according to the invention for improving compatibility for special mixtures are exemplified:

(a) ELPP, inoculated with MSA, ELPP, inoculated with MSA-styrene, and ELPP, inoculated with acrylic acid, for mixtures of IPP and its copolymers with polyamides, for example PA 6, PA 6,6 and their copolymers with aromatic modules such as phthalic acid , terephthalic acid, isophthalic acid, p-, o- and m-phenylenediamine, aromatic carboxylic amino acids such as ρ-, o-, and m-aminobenzoic acid and other aromatic dicarboxylic acids, diamines and aminocarboxylic acids containing more than 1 aromatic ring,

b) ELPP, inoculated with MSA, for mixtures of IPP and its copolymers with polyesters, for example polyalkylene terephthalate such as polyethylene terephthalate (PET) or polybutylene terephthalate (PBT) and their copolymers with other comonomers such as p-hydroxybenzoic acid, isophthalic acid and / or other aliphatic diols and diphenols, as well as mixtures with fully aromatic esters,

(c) ELPP, inoculated with MSA for mixtures of IPP and its copolymers with thermoplastic polyurethanes;

(d) ELPP, inoculated with glycidyl methacrylate and glycidyl acrylate, for mixtures of IPP and its copolymers with polyesters, for example polyalkylene terephthalate (PET, PBT) and its copolymers with other comonomers, such as in point b, as well as mixtures with fully aromatic polyesters;

(e) other grafted ELPP copolymers with acrylic acid derivatives such as methyl methacrylate, butyl acrylate, hydroxyester of acrylic acid, acrylic acid, oxazoline or acrylic and methacrylic acid derivatives for mixtures of IPP and its copolymers with polyesters, for example polyalkylene terephthalates, (PET, PBT) and copolymers thereof with other comonomers, such as in point b, as well as mixtures with fully aromatic polyesters,

(f) ELPP, inoculated with vinyl acetate, for mixtures of IPP and its copolymers with polyesters, for example polyalkylene terephthalate (PET, PBT) and their copolymers with other comonomers, such as in point b, as well as mixtures with fully aromatic polyesters;

(g) ELPP, vaccinated with glycidyl methacrylate and glycidyl acrylate, for mixtures of IPP and its copolymers with polycarbonates;

(h) styrene-grafted ELPP for mixtures of IPP and its copolymers with polystyrene and its copolymers;

(i) styrene grafted ELPP for mixtures of IPP and its copolymers with polycarbonates and copolymers;

(j) ELPP, grafted with glycidyl methacrylate and glycidyl acrylate, and other grafted ELPP copolymers with acrylic acid derivatives such as methyl methacrylate, butyl acrylate, hydroxyester of acrylic acid, acrylic acid, for mixtures of IPP and its copolymers with polyacrylates and polymethyl methacrylate,

k) a mixture of 50 to 99.5 wt. % Of ELPP grafted with MSA and 0.5 to 50 wt. vaccinated IPP, for mixtures of IPP and its copolymers with polyamides.

I. A method for producing elastomeric polypropylene

Example A:

1.1. Production of catalyst

44.22 g of tetraneolphyl zirconium (TNZ; Tm = 66 ° C, Du Pont) of gray brown were dissolved in an atmosphere of pure nitrogen in 620 ml of oxygen-free n-hexane on a copper catalyst (BASF R 3-11 catalyst at 70 ° C) and free of water and polar impurities at 20 ° C in a reaction vessel under a shielding gas atmosphere on molecular sieves 4A and 10A, respectively. The resulting suspension was filtered after 15 minutes after settling the bulk of the insoluble residue on the glass frit in a glass reaction vessel under an inert gas atmosphere, equipped with a stirrer, cooled to -40 ° C (heated above 150 ° C and purged with pure nitrogen (containing O2 max.) 2ppm)). The contents of the reaction vessel were further stirred after completion of the filtration (which lasted approximately 140 minutes) for a further 15 minutes at 40 ° C so that the TNZ would be as quantitative as possible. After the TNZ had settled, the residual solution was filtered on a filter plug under nitrogen pressure to another cooled reaction vessel under an inert gas atmosphere. The remaining TNZ was dissolved in an additional volume of 350 mL of N-hexane at about 5-10 ° C for 15 minutes and re-precipitated upon cooling to -34 ° C.

After the TNZ precipitate had settled, the solution was re-filtered with nitrogen over a glass filter candle into a first mother liquor reaction vessel, then the TNZ was dried using a vacuum pump (below 1 Pa) with cold precipitation by liquid nitrogen cooling. The purified TNZ had a melting point of 68 ° C and was white to cream. The combined mother liquors were concentrated to approximately 200 ml and TNZ, which was still in solution, precipitated in the cold at -40 ° C. After further pressure filtration through a filter plug, TNZ was redissolved in 100 mL hexane, reprecipitated at -40 ° C, filtered and dried under vacuum as described. The overall yield of this purification process was 82.2%. All processes were performed under pure nitrogen.

Conditioned (Alumina C, DEGUSSA product, conditioned at approximately 800 to 1000 ° C under a stream of nitrogen and after 16 hours storage at 50% relative humidity and 23 ° C relative humidity, was weighed into a 6-liter four-necked reaction vessel. repeated drying at 400 ° C under a stream of nitrogen to achieve an optimal surface hydroxyl concentration of approximately 1 mmol / g Alumina C) and supplemented with 5035 ml of n-hexane, purified on BASF R 3-11 catalyst and molecular sieves 4A and 10A, respectively. The suspension was stirred for about 1 hour at 400 rpm. Thereafter, 33.23 g of said TNZ (without mother liquor product) were dissolved in 465 ml of n-hexane (purified according to the above procedure) at 20 ° C, and this TNZ solution was added dropwise to the Al 2 O 3 slurry with stirring for 50 minutes. addition of a small amount of TNZ solution resulted in a significant decrease in the viscosity of the suspension. After addition of the TNZ solution, the number of revolutions was reduced to approximately 120 rpm. and stirring was continued for 12.5 hours in the absence of light. To speed up the filtration, the solid catalyst obtained was allowed to settle for 1 hour and finally the solution was filtered by pressure filtration through a sintered glass (3 hours). Finally, the solid catalyst was dried under vacuum at a value below 1 Pa (a diffusion oil pump with two interconnected freezing chambers, cooled with liquid nitrogen) with stirring until a constant weight of 292 g. All operations were performed in a pure nitrogen atmosphere. The obtained TNZ / Al 2 O 3 catalyst was an easily filterable beige to light brown powder, which tended to form tiny spheres of approximately 1 mm diameter. The Zr content was 1.66% by weight.

(b) Polymerization:

20-liter double-shell reactor, with paddle stirrer with polished surface, thermostat shell, temperature, speed and torque measurement, heated at 160 ° C and 10 Pa after three vacuum rinses with propene were charged with 7.3 kg of propene at 25 ° C. C. After increasing the number of revolutions to 400 rpm. 10.02 g of catalyst prepared according to 1.1 were flushed with 300 ml of liquid propene (approximately 20 ° C) and after two minutes the speed was reduced to 260 rpm. Over the next 10 minutes, the temperature of the propene was raised up to 60 ° C and maintained at that temperature for 120 minutes. from the addition of the catalyst. Then the speed was reduced to 200 rpm. and 1880 g of acetone preheated to 50 [deg.] C. were introduced into the reactor under nitrogen over 3 minutes. After increasing the number of revolutions to 400 rpm. to about 2 minutes followed by a reduction to 100 rpm. In the course of 20 minutes, unused propene was withdrawn at 60-46 ° C. The remaining acetone slurry of the ELPP elastomeric polypropylene was miscible and could be discharged through an opening at the bottom of the reactor.

After filtering the ELPP and drying under a stream of nitrogen at 50 ° C, 1.88 kg of a granular, non-sticky ELPP and a melting point (Tm) of 148.1 ° C (measured on a Du Pont 910/20 differential scanning calorimeter (Thermal Analyst 2100)) were obtained. ELPP had an ITT (melt flow index according to ISO 1133 / DIN 53735 at 230 ° C / 2.16 kg) of less than 0.01 g / 10 min, according to the calculated Zr 89 ppm and Al 2 O 3 content 0.49 wt%. ..

Example B:

The elastic polypropylene prepared according to Example A was ground on a crusher after cooling below 0 ° C to a grain size of less than 3 mm. 0.2 wt. bis with (2 (1,1 dimethylethyl) peroxoisopropyl) benzol (Perkadox 14SFI, Akzo), calculated on the amount of polypropylene, the mixture was melted at 190 ° C on an 18 mm Brabender single screw extruder and extruded at 1kg / h through a round nozzle for 3 mm diameter skein. The residence time in the extruder was about 1 minute. The skein was granulated after solidification in a water bath. The elastic polypropylene was degraded up to an ITT of 25 g / 10 min. The ITT was measured according to ISO 1133 / DIN 53735 at 230 ° C / 2.16 kg.

II. Method of making the additive to improve compatibility: Example 1:

In a 2 liter, oil bath, reflux condenser, nitrogen inlet, hermetically sealed stirrer and dropping funnel, 50 g of the elastomeric PP of Example A (ITT: 25) was dissolved in 1250 mL of xylol (isomer mixture) under nitrogen atmosphere. stirring at 120 ° C, and then 60 g of maleic anhydride (MSA) was added. 40 g of benzoyl peroxide dissolved in 100 ml of xylene was added dropwise at 130 ° C over 60 minutes. The solution was stirred for an additional 60 minutes and after cooling to 80 ° C was added to 2.5 L of acetone. The precipitated graft copolymer was aspirated, washed in 2.5 L of acetone, aspirated again and dried under vacuum at 80 ° C for 8 hours.

The MSA seeding degree, determined by infrared spectroscopy, was 1.2 wt%, calculated on the total.

Comparative example V1:

An additive to improve compatibility was prepared analogously to Example 1, but instead of ELPP, 100 g of isotactic PP (IPP, Daplen B-Pulver, reaction product, PCD polymers, ITT: small 0.001) in 1250 ml xylene with 60 g MSA were used for the reaction. and 40 g of benzoyl peroxide. The degree of seeding as determined by IR spectroscopy was 1.3% by weight, calculated on the total amount.

Example 2:

In analogy to the procedure described in Example 1, 100 g of elastomeric polypropylene (ELPP) according to Example B with ITT: 25, dissolved in 650 ml of xylene, 40 g of MSA and 20 g of benzoyl peroxide were used for the reaction. The MSA seeding degree was 2.9% by weight, calculated on the total amount.

Comparative example V2:

Analogously to Example 1, 100 g of isotactic polypropylene (Daplen RT 551, PCD polymers) with ITT: 28, dissolved in 650 ml of xylene, with 60 g of MSA and 40 g of benzoyl peroxide were used for the reaction. The MSA vaccination grade was 2.7% by weight, calculated on the total amount.

Example 3

Analogous to the procedure described in Example 1, 100 g of the elastomeric polypropylene of Example B with ITT: 25 dissolved in 650 ml of xylene, 40 g of glycidyl methacrylate (GMA, Fluka Chemie) and 20 g of benzoyl peroxide were used for the reaction. The GMA seeding degree, determined by IR spectroscopy, was 1.9% by weight, calculated on the total amount.

Comparative example V3:

In analogy to the procedure described in Example 1, 100 g of isotactic PP (IPP, Daplen RT 551, PCD polymers, ΙΓΓ: 28) in 750 ml of xylene, with 40 g of GMA and 20 g of benzoyl peroxide were used for the reaction. The GMA seeding degree, determined by IR spectroscopy, was 2.0% by weight, calculated on the total.

Example 4:

Analogously to the procedure described in Example 1, 100 g of the elastomeric polypropylene of Example B with ITT: 25, dissolved in 650 ml of xylene, with 40 g of styrene and 20 g of benzoyl peroxide, were used for the reaction. The styrene grafting degree, determined gravimetrically, was 10.4% by weight, calculated on the total.

Comparative example V4:

Analogously to Example 1, 100 g of isotactic polypropylene (Daplen RT 551, PCD polymers) with ΙΤΓ: 28 dissolved in 650 ml of xylene, 50 g of styrene and 20 g of benzoyl peroxide were used for the reaction. The styrene grafting degree, determined gravimetrically, was 9.8% by weight, calculated on the total amount.

III. Preparation of mixtures:

Example 5:

Polypropylene / polyamide 6 blend together with the grafted ELPP copolymers of Example 1 as an additive to improve compatibility (VM), IPP / PA6 / BM composition = 60/35/5% by weight.

Mixture of 3000 g IPP (Daplen BE 50, PCD polymers, ITT: 0.3), 1750 g polyamide 6 (SH3, by Leuna Werke AG, viscosity to DIN 53727: 140 cc / g in 96 percent sulfuric acid) and 250 g vaccinated The ELPP copolymer of Example 1 was extruded at a mass temperature of 255 ° C in a Berstorff ZE 25 twin screw extruder (L / D = 49.5) at a mass flow of 5 kg / h, cured in a water bath and granulated. After drying under vacuum at 80 ° C (8 hours), the granulate of the mixture was injected at a bulk temperature of 260 ° C and a compression temperature of 40 ° C onto 150x80x2 mm plates. The samples milled from these plates were then conditioned for 10 days at 70 ° C and 60% relative humidity. The following mechanical tests were performed: determination of the E modulus in bending according to DIN 53 457 (1987) on 50x10x2mm samples at 23 ° C; determination of Doppel-V bending strength according to DIN 53 753 (1981) on 50x6x2mm samples at 23 ° C; Determination of the Schadigungsarbeit (Wmax) and Durchstossarbeit (Wges.) in the breakdown test according to DIN 53 443/2. part (1984) on plates 150x80x2mm at 23 ° C. The mechanical properties are summarized in Table L

Comparative example V5:

In analogy to the conditions and blend ratios given in Example 5, an IPP / PA 6 mixture was prepared together with an IPP inoculated with MSA not according to the invention described in Comparative Example VI: 3000 g IPP (60 wt%), 1750 g PA 6 (35 wt%) and 250 g of IPP inoculated with MSA (according to Comparative Example VI; 5 wt%). The mechanical test values are given in Table 1.

Example 6:

Analogous to the conditions of Example 5, a mixture of IPP / PA 6 in a mixing ratio (IPP / PA 6 / VM) of 75/20/5 wt. together with the inoculated MSA ELPP described in Example 1 as an additive to improve compatibility: 3750 g (75 wt%) IPP, 1000 g (20 wt%) polyamide 6, and 2050 g (5 wt%) of the grafted ELPP copolymer according to Example L

The results of the mechanical tests of the mixture are shown in Table L

Comparative Example V6;

In analogy to the conditions of Example 6, an IPP / PA 6 mixture was prepared according to a mixing ratio (IPP / PA 6 / VM) of 75/20/5 wt. together with IPA grafted with MSA described in Comparative Example VI as an additive to improve compatibility: 3750 g (75 wt%) IPP, 1000 g (20 wt%) polyamide 6, and 250 g (5 wt%) graft copolymer IPP from Comparative Example VI.

The results of the mechanical tests of the mixture are shown in Table 1.

Example 7:

IPP / polyamide 6 mixture together with the grafted ELPP copolymers of Example 2 as additives to improve compatibility, composition of the mixture (IPP / PA 6 / VM) 45/50/5.

A mixture of 18 g (45% by weight) IPP (Daplen BE 50, PCD polymers, ITT: 0.3) was charged to a Brabender-Plasticorder with an electrically heatable 50 ml plasticization chamber. 20 g (50% by weight) of polyamide 6 (SH3, from Leuna-Werke, viscosity according to DIN 53 727: 150 cc / g in 96% sulfuric acid) and 2 g (5% by weight) of the grafted ELPP copolymer from Example 2 at a chamber temperature of 260 ° C with plasticizers switched on (60 rpm), plasticized for 5 minutes, and then removed from the plasticizer chamber. The mixture was processed at 260 ° C into a 200x80x2 mm plate from which 50x10x2 mm test specimens were milled to determine the modulus E in bending. Module E in bend is shown in Table 1.

Comparative example V7:

Analogously to the conditions of Example 7, an IPP / polyamide 6 mixture was prepared together with the grafted IPP copolymer from Comparative Example V2 as an additive to improve compatibility. Composition of the mixture (IPP / PA 6 / VN) 45/50/5: 18 g (45 wt%) IPP (ITT: 0.3), 20 g (50 wt%) polyamide 6 and 2 g (5 wt%) .) of the grafted IPP copolymer from Comparative Example V2. The modulus E in strength is shown in Table 1.

Example 8:

IPP / polyethylene terephthalate (PET) blend together with the grafted ELPP copolymer of Example 3 as an additive to improve compatibility.

Analogously to Example 7, a mixture of 18 g (45 wt%) of IPP, 20 g (50 wt%) of PET (Polyclear F, from Hoechst, MW: 60,000) and 2 g (5 wt%) of the grafted ELPP copolymer was prepared. from Example 3. Module E in bend is shown in Table L

Comparative example V8:

Analogously to the conditions set forth in Example 8, an IPP / polyethylene terephthalate mixture was prepared together with the grafted IPP copolymer from Comparative Example V3 as an additive to improve compatibility.

Mixture composition (IPP / PET / VM) 45/50/5: 18 g (45 wt%) IPP (ITT: 0.3), 20 g (50 wt%) PET and 2 g (5 wt%) the grafted IPP copolymer of Comparative Example V3.

Module E in bend is shown in Table 1.

Example 9:

Process for preparing the IPP / polycarbonate (PC) mixture together with the grafted ELPP copolymer of Example 3 as an additive to improve compatibility.

Analogously to Example 7, a mixture of 18 g (45 wt%) IPP, 20 g (50 wt%) PC (Lexan PK 1340, from General Electric, MVR (melt volume flow rate according to ISO 1133, 300 ° C)) was prepared. 1.2 kg): 6 ml / 10 minutes) and 2 g (5 wt.%) Of the grafted ELPP copolymer of Example 3. Module E in bend is shown in Table L

Comparative example V9:

Analogously to the conditions of Example 9, an IPP / polycarbonate mixture was prepared together with the grafted IPP copolymer from Comparative Example V3 as an additive to improve compatibility.

Mixture composition (IPP / PC / VM) 45/50/5: 18 g (45 wt%) IPP (ITT: 0.3), 20 g (50 wt%) PC and 2 g (5 wt%) the grafted IPP copolymer of Comparative Example V3.

Module E in bend is shown in Table 1.

Example 10:

Process for the preparation of the IPP / Polystyrene (PS) mixture together with the grafted ELPP copolymer of Example 4 as an additive to improve compatibility.

Analogously to Example 7, a mixture of 18 g (45 wt%) IPP, 20 g (50 wt%) PS (PSH 165, BASF, viscosity according to ISO 1628/1 (1984) 119 ml / g) and 2 was prepared. g (5 wt%) of the grafted ELPP copolymer of Example 4.

Module E in bend is shown in Table 1. Comparative Example V10:

Analogously to the conditions set forth in Example 10, an IPP / polystyrene mixture was prepared together with the grafted IPP copolymer from Comparative Example V4 as an additive to improve compatibility.

Mixture composition (IPP / PS / VM) 45/50/5: 18 g (45 wt%) IPP (ITT: 0.3), 20 g (50 wt%) PS and 2 g (5 wt%) of the grafted IPP copolymer of Comparative Example V4.

Module E in bending is shown in Table L

From the measured values shown in Table 1, it can be seen that the compositions in which the additives used to improve the compatibility according to the invention were used have a much lower stiffness (lower modulus E) and much better toughness (Fallbolzentest and Doppel V impact strength). known additives to improve compatibility.

Table 1: Properties of mixtures

Ex. mixture VMZ E modul FB DV Ex. (MPa) (D (kJ / m ² ) i q Wmax. WGES. i q 5 PP / PA 1 985 1010 6 9 44,6 9 V5 PP / PA VI 1405 1289 5.3 7.8 22.7 2.4 6 PP / PA 1 1134 1082 22 23 48.1 52 V6 PP / PA VI 1298 1276 2.2 3.6 32.8 4.7 7 PP / PA 2 1552 V7 PP / PA V2 2061 8 PP / PET 3 1795 V8 PP / PET V3 2277 9 PP / PC 3 1442 V9 PP / PC V3 1580 10 PP / PS 4 1683 V10 PP / PS V4 1953

E modul modulus of bending elasticity according to DIN 53 457 (1987) FB Fallbolzentest according to DIN 53 443 (1984), Part 2 (23 ° C) Wmax. work at maximum strength WGES total work DV notch impact strength Doppel-V according to DIN 53753 (1981) (1) test in the processing direction (Q) transversal test for processing direction PP polypropylene PA polyamide PET polyethylene terephthalate PC polycarbonate PS polystyrene IN M additive to improve compatibility

PATENT CLAIMS

Claims (10)

Modified elastomeric polypropylenes and mixtures thereof with modified isotactic polypropylenes, with a stereoregulated block arrangement in the chain structure, characterized in that the elastomeric polypropylenes are modified with ethylenically unsaturated seeding monomers and mixtures thereof with isotactic polypropylenes which are modified with ethylenically unsaturated monomers. Modified elastomeric polypropylenes and mixtures thereof according to claim 1, characterized in that the seeding monomers belong to the group of ethylenically unsaturated aliphatic or aromatic carboxylic acids or derivatives thereof. Modified elastomeric polypropylenes and mixtures thereof according to claim 1 or 2, characterized in that the seeding monomers belong to the group of maleic acid or its derivatives, acrylic acid or its derivatives, methacrylic acid or its derivatives. Modified elastomeric polypropylenes and mixtures thereof according to claim 1, characterized in that the seeding monomers belong to the group of vinyl aromatics or vinyl alcohol esters. Modified elastomeric polypropylenes and mixtures thereof according to one of claims 1 to 4, characterized in that the content of seeding monomers is 0.1 to 30% by weight, more preferably 0.5 to 10% by weight, particularly preferably 0, 5 to 5 wt. Modified elastomeric polypropylenes and mixtures thereof according to one of claims 1 to 5, characterized in that they contain up to 80% by weight, more preferably 0.5 to 50% by weight. modified isotactic polypropylenes. 7. A process for the modification of elastomeric polypropylenes with a stereoregulated block arrangement in the chain structure or mixtures thereof with isotactic polypropylenes, characterized in that ethylenically unsaturated grafting monomers are used for grafting elastomeric polypropylenes or a mixture of elastomeric polypropylenes and isotactic polypropylenes. Use of modified elastomeric polypropylenes and / or mixtures thereof with modified isotactic polypropylenes according to one of claims 1 to 7 as an additive to improve compatibility in mixtures of polyolefins with neolefin thermoplastics. Use of modified elastomeric polypropylenes and / or mixtures thereof with modified isotactic polypropylenes according to one of claims 1 to 7 as an additive for improving adhesion in polyolefin and metal laminates or laminates. A mixture of polyolefins and neolefin thermoplastics, characterized in that it contains modified elastomeric polypropylenes and / or mixtures thereof with modified isotactic polypropylenes according to one of Claims 1 to 6 as a compatibility additive.