EA043072B1 - POLYMER COMPOSITION WITH IMPROVED PAINT ADHESION - Google Patents

Description

The invention relates to a polypropylene composition (C), a product containing a polypropylene composition (C) and the use of a polypropylene composition (C) to enhance the adhesion of the paint coating of the product.

In the automotive industry, polylefins such as polypropylenes are the preferred material because they can be customized for specific purposes. For example, heterophasic polypropylenes are widely used in the automotive industry, such as bumpers, because they combine good stiffness with sufficient impact resistance. However, the surface of cast products obtained from a heterophase polypropylene composition is quite smooth with low polarity, which as a result creates unfavorable conditions for interaction with the coating material. Therefore, high-demand applications such as automotive parts typically require pre-treatment along with adhesion promoters (called primers) to ensure proper paint adhesion. For environmental and economic reasons, it is desirable to reduce the use of primers to a minimum, preferably avoiding the use of primers entirely.

Accordingly, it is an object of the present invention to provide a material that allows one skilled in the art to which the present invention relates to produce castings with good stiffness, a good balance of impact strength and high paint adhesion, without the need for the use of adhesion promoters such as primers.

The invention of the present invention is to provide a polypropylene composition (C) containing a specific heterophasic propylene copolymer (HECO), a specific plastomer (PL) and a specific inorganic filler (F).

In a first aspect, the present invention relates to a polypropylene composition (C) containing:

(a) from 50 to 90 parts by weight. heterophasic propylene copolymer (HECO);

(b) from 2 to 25 parts by weight. plastomer (PL); and (c) from 8 to 25 parts by weight. inorganic filler (F) from the total parts by weight of compounds (a), (b) ^and (c);

wherein the polypropylene composition (C) has a xylene cold soluble fraction (XCS) content of at least 22% by weight of the total weight of the polypropylene composition (C); and wherein the intrinsic viscosity (IV) of the xylene cold soluble (XCS) fraction of the polypropylene composition (C) is no more than 3.4 dl/g.

In another aspect, the present invention relates to a polypropylene (C) composition comprising:

(a) from 70 to 80 parts by weight. heterophasic propylene copolymer (HECO), which contains:

i) a polypropylene matrix (M), which is a homopolymer or copolymer of propylene containing units derived from propylene and ethylene and/or C ₄ -C ₂₀ α-olefins; and ii) an elastomeric copolymer (E) containing units derived from propylene and ethylene and/or C4-C20 α-olefins;

(b) from 7 to 12 parts by weight. plastomer (PL), which is an elastomeric ethylene copolymer (EC) containing units derived from ethylene and at least one C ₄ -C ₂₀ α-olefin; and (c) from 13 to 18 parts by weight. inorganic filler (F) from the total parts by weight of compounds (a), (b) ^and (c);

wherein the polypropylene composition (C) has a xylene cold soluble fraction (XCS) content of at least 22% by weight, based on the total weight of the polypropylene composition (C); and wherein the intrinsic viscosity (IV) of the xylene cold soluble (XCS) fraction of the polypropylene composition (C) is no more than 3.3 dl/g.

The polypropylene composition (C) has a tensile modulus, as measured according to ISO 527-2, of at least 800 MPa, such as in the range from 800 to 2000 MPa;

elongation at break, as measured according to ISO 527-2, not more than 70%, such as in the range from 10 to 70%;

Charly cut strength (NIS+23), as measured according to ISO 179 1eA:2000 at +23°C, of at least 10 kJ/m ² , such as in the range from 10 to 80 kJ/m ² .

Heterophasic propylene copolymer (HECO) may contain:

(a) from 5 to 49 parts by weight. the first heterophasic propylene copolymer (HECO1), and (b) from 51 to 95 parts by weight. a second heterophasic propylene copolymer (HECO2) from the common parts by weight of a heterophasic propylene copolymer (HECO1) and a heterophasic propylene copolymer (HECO2);

wherein the first heterophasic propylene copolymer (HECO1) differs from the second heterophasic propylene copolymer (HECO2) by melt flow rate MFR2 (230°C, 2.16 kg) as measured according to ISO 1133.

A heterophasic propylene copolymer (HECO2) and a heterophasic propylene copolymer (HECO1) together satisfy inequality (I):

- 1 043072

MFR [HECO2] /MFR [HECO1] > 1.0 (I);

Where MFR [HECO2] is the melt flow rate of MFR ₂ (230°C, 2.16 kg), as measured according to ISO 1133, of heterophasic propylene copolymer (HECO2)

MFR [HECO1] is the melt flow rate of MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of heterophasic propylene copolymer (HECO1).

The melt flow rate of MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of heterophasic propylene copolymer (HECO1) may be no more than 40 g/10 min, such as in the range from 5 to 40 g/10 min , and/or the melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, heterophasic propylene copolymer (HECO2) may be at least 6 g/10 min, such as in the range from 6 to 50 g/10 min.

The polypropylene composition (C) may include a heterophasic propylene copolymer (HECO1) and a heterophasic propylene copolymer (HECO2), wherein (a1) the heterophasic propylene copolymer (HECO1) may contain: a cold xylene soluble fraction ranging from 10 to 55 wt.% from the total mass of heterophasic propylene copolymer (HECO1);

(a2) the xylene cold soluble (XCS) fraction of the heterophasic propylene copolymer (HECO1) may contain comonomer units derived from C ₂ and/or C ₄ -C ₁₂ α-olefin ranging from 30 to 65 mol.%; and (a3) the xylene cold soluble (XCS) fraction of the heterophasic propylene copolymer (HECO1) may have an intrinsic viscosity (IV) of no more than 4.0 dl/g; and/or (b1) the heterophasic propylene copolymer (HECO2) may contain a cold xylene soluble fraction ranging from 10 to 55 wt.% of the total weight of the heterophasic propylene copolymer (HECO2);

(b2) the xylene cold soluble (XCS) fraction of the heterophasic propylene copolymer (HECO2) may contain comonomer units derived from C ₂ and/or C 4 -C ₁₂ α-olefin, ranging from 30 to 65 mol.%; and (b3) the xylene cold soluble (XCS) fraction of the heterophasic propylene copolymer (HECO2) may have an intrinsic viscosity (IV) of no more than 3.5 dl/g.

The plastomer (PL) may be an elastomeric ethylene copolymer (EC) containing units derived from ethylene and at least one C4- _C20 α-olefin.

The plastomer (PL) may be an elastomeric ethylene copolymer (EC) consisting of units derived from ethylene and 1-octene, having a melt flow rate MFR (190°C) as measured according to ASTM D1238, ranging from 0.1 to 5.0 g/10 min;

The plastomer (PL) may be an elastomeric ethylene copolymer (EC) consisting of units derived from ethylene and 1-octene, having a density ranging from 830 to 890 kg/m ³ .

The plastomer (PL) may be an elastomeric ethylene copolymer (EC) consisting of units derived from ethylene and 1-octene, having an ethylene content ranging from 70 to 99 mol%.

The inorganic filler (F) may be a mineral filler.

The inorganic filler (F) may be talc with a median particle size (D50) of no more than 5.0 μm.

The inorganic filler (F) may be talc with a particle size limit (D95) of no more than 8.0 microns.

The polypropylene composition (C) cannot contain polymers other than heterophasic copolymer of propylene (HECO) and plastomer (PL) in an amount exceeding 2.5 wt.% of the total weight of the polypropylene composition (C).

Heterophasic propylene copolymer (HECO) and plastomer (PL) may be the only polymers present in the polypropylene composition (C).

In a second aspect, the present invention relates to the above-mentioned article containing polypropylene (C).

In a third aspect, the present invention relates to the use of the above polypropylene composition (C) for enhancing the adhesion of a paint coating of the above molded product.

Next, the polypropylene composition (C) and the product containing the polypropylene composition (C) will be described in more detail:

Polypropylene composition (C)

The polypropylene composition (C) contains a heterophasic propylene copolymer (HECO), a plastomer (PL) and an inorganic filler (F).

It should be understood that the polypropylene composition (C) contains heterophasic propylene copolymer (HECO) in an amount of from 50 to 90 parts by weight, preferably from 65 to 85 parts by weight, more preferably from 70 to 80 parts by weight. from the total parts by weight of heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F).

It should be understood that the polypropylene composition (C) contains plastomer (PL) in an amount of 2

- 2 043072 to 25 parts by weight, preferably from 5 to 15 parts by weight, more preferably from 7 to 12 parts by weight. from the total parts by weight of heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F).

It should be understood that the polypropylene composition (C) contains an inorganic filler (F) in an amount of from 8 to 25 parts by weight, preferably from 10 to 20 parts by weight, more preferably from 13 to 18 parts by weight. from the total parts by weight of heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F).

In one embodiment of the present invention, the polypropylene composition (C) contains from 50 to 90 parts by weight. heterophasic propylene copolymer (HECO), from 2 to 25 parts by weight. plastomer (PL) and 8 to 25 parts by weight. inorganic filler (F) from the total parts by weight of heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F).

In one embodiment of the present invention, the polypropylene composition (C) contains from 65 to 85 parts by weight. heterophasic propylene copolymer (HECO), from 5 to 15 parts by weight. plastomer (PL) and from 10 to 20 parts by weight. inorganic filler (F) from the total parts by weight of heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F).

In one embodiment of the present invention, the polypropylene composition (C) contains from 70 to 80 parts by weight. heterophasic propylene copolymer (HECO), from 7 to 12 parts by weight. plastomer (PL) and from 13 to 18 parts by weight. inorganic filler (F) from the total parts by weight of heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F).

In one embodiment of the present invention, the polypropylene composition (C) contains heterophasic propylene copolymer (HECO) ranging from 50 to 90 wt.%, plastomer (PL) ranging from 2 to 25 wt.% and inorganic filler (F) ranging from 8 to 25 wt.% of the total weight of the polypropylene composition (C).

In one embodiment of the present invention, the polypropylene composition (C) contains heterophasic propylene copolymer (HECO) ranging from 65 to 85 wt.%, plastomer (PL) ranging from 5 to 15 wt.%, and inorganic filler (F) ranging from from 10 to 20 wt.% of the total weight of the polypropylene composition (C).

In one embodiment of the present invention, the polypropylene composition (C) contains heterophasic propylene copolymer (HECO) ranging from 70 to 80 wt.%, plastomer (PL) ranging from 7 to 12 wt.%, and inorganic filler (F) ranging from from 13 to 18 wt.% of the total weight of the polypropylene composition (C).

With respect to the method for producing the polypropylene composition, in particular, if the polypropylene composition is used to produce a molded product such as an injection molded product, the polypropylene composition must exhibit sufficient melt flow rate.

Therefore, it will be understood that the polypropylene composition (C) has a melt flow rate MFR ₂ (230°C, 2.16 kg), as measured according to ISO 1133, of at least 5 g/10 min, preferably at least 8 g/ 10 min, even more preferably at least 11 g/10 min; such as in the range from 5 to 50 g/10 min, preferably in the range from 8 to 25 g/10 min, even more preferably in the range from 11 to 15.

The finding of the present invention is that the paint adhesion of a polypropylene composition containing a heterophasic propylene copolymer, a plastomer and an inorganic filler can be improved by providing a heterophasic propylene copolymer with a specific cold xylene soluble fraction content and a specific intrinsic viscosity.

Therefore, it is understood that the polypropylene composition (C) has a xylene cold soluble fraction (XCS) content of at least 22% by weight, preferably at least 25% by weight, more preferably at least 30% by weight; such as in the range from 22 to 45 wt.%, preferably in the range from 25 to 40 wt.%, more preferably in the range from 30 to 35 wt.%, based on the total weight of the polypropylene composition (C).

Additionally, it is understood that the intrinsic viscosity (IV) of the xylene cold soluble (XCS) fraction of the polypropylene composition (C) is no more than 3.4 dl/g, preferably no more than 3.3 dl/g, more preferably no more than 3.2 dl/g; such as in the range of 2.0 to 3.4 dl/g, preferably in the range of 2.5 to 3.3 dl/g, more preferably in the range of 2.5 to 3.2 dl/g.

In one embodiment of the present invention, the polypropylene composition (C) has a xylene cold soluble fraction (XCS) content ranging from 22 to 45 wt.% of the total weight of the polypropylene composition (C), where the intrinsic viscosity (IV) of the fraction, xylene cold soluble (XCS) ranges from 2.5 to 3.3 dl/g.

In one embodiment of the present invention, the polypropylene composition (C) has a xylene cold soluble fraction (XCS) content ranging from 25 to 40% by weight of the total weight of the polypropylene composition (C), wherein the intrinsic viscosity (IV) of the fraction is, xylene cold soluble (XCS) ranges from 2.5 to 3.2 dl/g.

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Additionally, the polypropylene composition (C) must exhibit mechanical properties sufficient for the intended application. In particular, the polypropylene composition (C) must exhibit sufficient rigidity and impact resistance.

It will be understood that the polypropylene composition (C) has a tensile modulus, as measured according to ISO 527-2, of at least 800 MPa, preferably at least 1000 MPa, more preferably at least 1300 MPa; such as in the range of 800 to 2000 MPa, preferably in the range of 1000 to 1800 MPa, more preferably in the range of 1300 to 1650 MPa.

It will be understood that the polypropylene composition (C) has a tensile yield strength, as measured according to ISO 527-2, of at least 5 MPa, preferably at least 10 MPa, more preferably at least 15 MPa; such as in the range of 5 to 50 MPa, preferably in the range of 10 to 30 MPa, more preferably in the range of 15 to 25 MPa.

It will be understood that the polypropylene composition (C) has a tensile failure stress, as measured according to ISO 527-2, of at least 5 MPa, preferably at least 8 MPa, more preferably at least 10 MPa; such as in the range of 5 to 50 MPa, preferably in the range of 8 to 20 MPa, more preferably in the range of 10 to 15 MPa.

It will be understood that the polypropylene composition (C) has an elongation at break, as measured according to ISO 527-2, of no more than 70%, preferably no more than 60%, more preferably no more than 50%; such as in the range of 10 to 70%, preferably in the range of 20 to 60%, more preferably in the range of 30 to 50%.

It will be understood that the polypropylene composition (C) has a Charlie cut strength (NIS+23), as measured according to ISO 179-1eA:2000 at +23°C, of at least 10 kJ/m ² , preferably at least 15 kJ/m ² , more preferably at least 25 kJ/m ² ; such as in the range from 10 to 80 kJ/m ² , preferably in the range from 15 to 60 kJ/m ² , more preferably in the range from 25 to 55 kJ/m ² .

It will be understood that the polypropylene composition (C) has a Charly cut strength (NIS 20), as measured according to ISO 179-1eA:2000 at -20°C, of at least 2 kJ/m ² , preferably at least 5 kJ /m ² , more preferably at least 7 kJ/m ² ; such as in the range from 2 to 20 kJ/m ² , preferably in the range from 5 to 15 kJ/m ² , more preferably in the range from 7 to 12 kJ/m ² .

In one embodiment of the present invention, the polypropylene composition (C) has a tensile modulus, as measured according to ISO 527-2, ranging from 800 to 2000 MPa, a tensile failure stress, as measured according to ISO 527-2, ranging from 5 up to 50 MPa, elongation at break, as measured according to ISO 527-2, ranging from 10 to 70%, tensile strength at yield strength, as measured according to ISO 527-2, ranging from 5 to 50 MPa, strength Charly cut strength (NIS+23) as measured according to ISO 179-1eA:2000 at +23°C, ranging from 10 to 80 kJ/ ^m2 and Charly cut strength (NIS-20) as measured according to ISO 179-1eA:2000 at -20°C, ranging from 2 to 20 kJ/ ^m2 .

In one embodiment of the present invention, the polypropylene composition (C) has a tensile modulus, as measured according to ISO 527-2, ranging from 1000 to 1800 MPa, a tensile failure stress, as measured according to ISO 527-2, ranging from 8 up to 20 MPa, elongation at break, as measured according to ISO 527-2, ranging from 20 to 60%, tensile strength at yield strength, as measured according to ISO 527-2, ranging from 10 to 30 MPa, strength Charly cut strength (NIS+23) as measured according to ISO 179-1eA:2000 at +23°C, ranging from 15 to 60 kJ/ ^m2 and Charly cut strength (NIS-20) as measured according to ISO 179-1eA:2000 at -20°C, ranging from 5 to 15 kJ/ ^m2 .

In one embodiment of the present invention, the polypropylene composition (C) has a tensile modulus, as measured according to ISO 527-2, ranging from 1300 to 1650 MPa, a tensile failure stress, as measured according to ISO 527-2, ranging from 10 up to 15 MPa, elongation at break, as measured according to ISO 527-2, ranging from 30 to 50%, tensile strength at yield strength, as measured according to ISO 527-2, ranging from 15 to 25 MPa, strength Charly cut strength (NIS+23) as measured according to ISO 179-1eA:2000 at +23°C, ranging from 25 to 55 kJ/ ^m2 and Charly cut strength (NIS-20) as measured according to ISO 179-1eA:2000 at -20°C, ranging from 7 to 12 kJ/ ^m2 .

The polypropylene composition (C) may not contain polymers other than heterophasic propylene copolymer (HECO) and plastomer (PL) in an amount exceeding 10 wt.%, preferably in an amount exceeding 5 wt.%, more preferably in an amount exceeding 2.5 wt.%, even more preferably in an amount exceeding 0.8 wt.% based on the total weight of the polypropylene composition (C).

In one embodiment of the present invention, the polypropylene composition (C) does not contain polymers other than heterophasic propylene copolymer (HECO) and plastomer (PL) in an amount greater than 10 wt.%, preferably in an amount greater than 5 wt.%, more than

- 4 043072 preferably in an amount greater than 2.5% by weight, even more preferably in an amount greater than 0.8% by weight, based on the total weight of the polypropylene composition (C).

In one embodiment of the present invention, heterophasic propylene copolymer (HECO) and plastomer (PL) are the only polymers present in the polypropylene composition (C).

In one embodiment of the present invention, the polypropylene composition (C) consists of a heterophasic propylene copolymer (HECO), a plastomer (PL) and an inorganic filler (F).

Heterophasic propylene copolymer (HECO).

The polypropylene composition necessarily contains heterophasic propylene copolymer (HECO).

As used herein, the term heterophasic means that at least one elastomeric propylene copolymer is (finely) dispersed in a matrix. In other words, at least one elastomer forms inclusions in the matrix. Therefore, the matrix contains (finely) dispersed inclusions that are not part of the matrix, and said inclusions contain at least one elastomeric copolymer. As used herein, the term inclusion preferably indicates that the matrix and inclusions form distinct phases in the heterophasic propylene copolymer; said inclusions are, for example, visible using high-resolution microscopy, such as electron microscopy, or scanning atomic force microscopy.

As described in the specification of the present patent application, the heterophasic propylene copolymer contains, as polymer components, only a polypropylene matrix and an elastomeric copolymer dispersed in said polypropylene matrix.

Therefore, it should be understood that the heterophasic propylene copolymer (HECO) contains, preferably consists of:

(a) a polypropylene matrix (M) and (b) an elastomeric copolymer (E) containing units derived from: propylene and ethylene and/or C ₄ -C ₂₀ α-olefins, preferably from ethylene and/or C ₄ -Csh α -olefins, more preferably only ethylene.

The polypropylene matrix (M) may be a random propylene copolymer (RPP) or a propylene homopolymer (HPP), the latter being substantially preferred.

In one embodiment of the present invention, the polypropylene matrix (M) is a propylene homopolymer (HPP).

As used herein, the term propylene homopolymer refers to polypropylene which consists essentially, i.e., more than 99.7% by weight, even more preferably at least 99.8% by weight, of propylene units based on the total weight of the homopolymer. propylene (HPP). In a preferred embodiment of the present invention, only propylene units (PRU) are detected in the propylene homopolymer.

In the case where the polypropylene matrix (M) is a propylene homopolymer (HPP), the comonomer content of the polypropylene matrix (M) may be equal to or less than 1.0 mass%, preferably equal to or less than 0.8 mass%, more preferably equal to or less than 0.5 wt.%, even more preferably equal to or less than 0.2 wt.% of the total weight of the polypropylene matrix (M).

In the case where the polypropylene matrix (M) is a random propylene copolymer (RPP), it is understood that the random propylene copolymer (RPP) contains, preferably consists of propylene derived units and ethylene and/or C ₄ -derived units C ₂₀ α-olefins, preferably propylene-derived units and ethylene-derived units and/or C ₄ -C ₁₀ α-olefins, more preferably propylene-derived units and ethylene-derived units and/or C ₄ , C ₆ and/or C ₈ α-olefins.

It will be understood that the random propylene copolymer (RPP) contains, preferably consists of, units derived from propylene and units derived from ethylene, 1-butene and/or 1-hexene. In particular, it should be understood that random propylene copolymer (RPP) contains, in addition to propylene, only units derived from ethylene, 1-butene and/or 1-hexene.

In one embodiment of the present invention, the random propylene copolymer (RPP) consists of propylene-derived units and ethylene-derived units.

The second component of the heterophasic propylene copolymer (HECO) is an elastomeric copolymer (E).

The elastomeric copolymer (E) may contain propylene derived units and ethylene derived units and/or C ₄ -C ₂₀ α-olefins, preferably propylene derived units and ethylene and/or C ₄ - derived units C ₁₀ α-olefins, more preferably units derived from propylene and units derived from ethylene and/or C ₄ , C ₆ and/or C ₈ α-olefins.

The elastomeric copolymer (E) may further contain units derived from conjugated dienes, such as butadiene, or non-conjugated dienes. Suitable non-conjugated dienes (dienes without conjugated double bonds), if used, include straight and

- 5 043072 branched acyclic dienes, such as 1,4-hexadiene, 1,5-hexadiene, 1,6-octadiene, 5-methyl-1,4hexadiene, 3,7-dimethyl-1,6-octadiene, 3,7 -dimethyl-1,7-octadiene and mixtures of dihydromyrcene and dihydroocymene isomers, and single-ring acyclic dienes such as 1,4-cyclohexadiene, 1,5cyclooctadiene, 1,5-cyclododecadiene, 4-vinylcyclohexene, 1-allyl-4 -isopropylidene cyclohexane, 3-allyl cyclopentene, 4-cyclohexene and 1-isopropenyl-4-(4-butenyl) cyclohexane.

However, preferably the elastomeric copolymer (E) consists of units derived from propylene and units derived from ethylene and/or C ₄ -C ₂₀ α-olefins, preferably units derived from propylene and units derived from ethylene and/or C ₄ -C1 ₀ α-olefins, more preferably units derived from propylene and units derived from ethylene and/or C ₄ , C ₆ and/or C ₈ α-olefins.

As stated above, the polypropylene composition (C) may contain heterophasic propylene copolymer (HECO) in an amount of 50 to 90 parts by weight, preferably 65 to 85 parts by weight, more preferably 70 to 80 parts by weight. from the total parts by weight of heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F).

In one embodiment of the present invention, the polypropylene composition (C) contains heterophasic propylene copolymer (HECO) in the range of 50 to 90 wt.%, preferably in the range of from 65 to 85 wt.%, more preferably in the range of 70 to 80 wt.% from the total weight of the polypropylene composition (C).

The heterophasic propylene copolymer (HECO) may contain at least one α-nucleating agent. Additionally, preferably the heterophasic propylene copolymer (HECO) does not contain any β-nucleating agents.

The α-nucleating agent is preferably selected from the group consisting of:

(i) salts of monocarboxylic acids and polycarboxylic acids, for example sodium benzoate or aluminum tert-butyl benzoate and (ii) dibenzylidene sorbitol (for example, 1,3:2,4 dibenzylidene sorbitol) and C ₁ -C ₈ -alkyl-substituted dibenzylidene sorbitol derivatives, such as methyl dibenzylidene sorbitol, ethyl dibenzylidene sorbitol or dimethyldibenzylidene sorbitol (for example, 1,3:2,4 di(methylbenzylidene) sorbitol), or nonitol-substituted derivatives such as 1,2,3,-trideoxy-4,6:5,7-bis-O-[( 4-propylphenyl)methylene]-nonite, and (iii) salts of phosphoric acid diesters, for example sodium 2,2'-methylenebis-(4,6-di-tert-butylphenyl)phosphate or aluminum-hydroxy-bis-[2,2' -methylene-bis-(4,6-di-t-butylphenyl)phosphate], and (iv) vinylcycloalkane polymer and vinylalkane polymer (as described in more detail below) and (v) mixtures thereof.

Such additives and nucleating agents are generally commercially available and are described, for example, in the Plastic Additives Handbook, ^5th edition, 2001 of Hans Zweifel.

Preferably, the α-nucleating agent is part of a heterophasic propylene copolymer (HECO) and therefore a polypropylene composition (C). The content of the α-nucleating agent in the heterophasic propylene copolymer (HECO) is preferably up to 5.0 wt.% of the total weight of the heterophasic propylene copolymer (HECO).

It should be understood that the heterophasic propylene copolymer (HECO) contains no more than 3000 ppm of α-nucleating agent, preferably no more than 2000 ppm.

In one embodiment of the present invention, the heterophasic propylene copolymer (HECO), and hence the polypropylene composition (C), contains a vinylcycloalkane, such as vinylcyclohexane (VCH) polymer and/or a vinylalkane polymer as an α-nucleating agent.

It should be understood that the vinylcycloalkane, such as vinylcyclohexane (VCH) polymer, and/or the vinylalkane polymer are contained in the heterophasic propylene copolymer (HECO) in an amount of not more than 500 ppm, preferably in an amount of not more than 200 ppm; such as in the range from 1 to 200 ppm, preferably in the range from 5 to 100 ppm, based on the total weight of the heterophasic propylene copolymer (HECO).

Accordingly, it should be understood that the polypropylene composition (C) contains vinylcycloalkane; such as a vinylcyclohexane (VCH) polymer, and/or a vinyl alkane polymer in an amount of not more than 500 ppm, preferably in an amount of not more than 200 ppm, such as in the range of 1 to 200 ppm, preferably in the range of 5 to 100 ppm of the total weight of the polypropylene composition (C).

Preferably, the vinylcycloalkane polymer that is introduced into the heterophasic propylene copolymer (HECO) and therefore into the polypropylene composition (C) is a vinylcyclohexane (VCH) polymer introduced using BNT technology.

Regarding BNT technology, reference is made to international patent applications WO 99/24478, WO 99/24479 and in particular WO 00/68315. According to this technology, the catalyst system, preferably a Ziegler-Natta procatalyst, can be modified by polymerization with a vinyl compound in the presence of a catalyst system containing, in particular, a specific Ziegler-Natta procatalyst, an external donor and a cocatalyst, wherein the vinyl compound has the formula:

- 6 043072

CH2=CH-CHR ³ R ⁴ where R ³ and R ⁴ together form a 5- or 6-membered saturated, unsaturated or aromatic ring, or independently represent an alkyl group of 1 to 4 carbon atoms. The modified catalyst is used to produce heterophasic, that is, heterophasic propylene copolymer (HECO). A polymerized vinyl compound can be used as an α-nucleating agent. The weight ratio of vinyl compound to solid catalyst component in the catalyst modification step is preferably up to 5 (5:1), more preferably up to 3 (3:1), such as in the range of 0.5 (1:2) to 2 ( 2:1). The most preferred vinyl compound is vinylcyclohexane (VCH).

The nucleating agent can be introduced in the form of a masterbatch. In this case, the masterbatch contains a nucleating agent, which is preferably a polymeric nucleating agent, more preferably an alpha nucleating agent, most preferably a vinylcycloalkane such as a vinylcyclohexane (VCH) polymer and/or a vinylalkane polymer, preferably a vinylcyclohexane (VCH) polymer, as above or lower, in an amount of not more than 500 ppm, more preferably from 1 to 200 ppm and even more preferably from 5 to 100 ppm, based on the total weight of the masterbatch.

The heterophasic propylene copolymer (HECO) of the present invention is preferably produced by using a sequential polymerization process, that is, a multi-step process known in the art to which the present invention relates, wherein the corresponding matrix, that is, a polypropylene matrix (M), is prepared by using at least at least one slurry reactor and optionally at least one gas-phase reactor, preferably one slurry reactor and one gas-phase reactor, after which the elastomeric copolymer (E) is obtained using at least one gas-phase reactor, preferably two gas-phase reactors. Namely, a heterophasic propylene copolymer (HECO) is produced by producing a polypropylene matrix (M) using at least one reactor system, said system comprising at least one reactor, by moving said polypropylene matrix (M) to a subsequent reactor system, said system containing at least one reactor where, in the presence of a polypropylene matrix (M), an elastomeric propylene copolymer (E) is produced.

However, it is also possible that heterophasic propylene copolymer (HECO) along with its individual components (matrix and elastomeric copolymer) can be obtained by mixing polymers of different types, that is, polymers that differ from each other in the units from which they can be obtained, and /or polymers that differ from each other in molecular weight, comonomer content, cold xylene soluble fraction (XCS), comonomer content in cold xylene soluble (XCS) fraction, and/or intrinsic viscosity (IV) fraction , xylene cold soluble (XCS).

In a preferred embodiment of the present invention, the propylene copolymer (HECO) is produced by blending different types of polymers, preferably by melt blending the different types of polymers in an extruder.

The heterophasic propylene copolymer (HECO) may be multimodal, in particular the matrix (M) and/or the elastomeric copolymer (E) of the heterophasic propylene copolymer (HECO) may be multimodal.

As used herein, the terms multimodal or bimodal or trimodal refer to the modality of the polymer, that is, the shape of the molecular weight distribution curve, which is a graph of the molecular weight of a fraction as a function of its molecular weight, and/or the shape of the comonomer content distribution curve, which represents a graph of comonomer content as a function of the molecular weight of polymer fractions, where the distribution curve shows at least two distinct peaks.

In one embodiment of the present invention, the heterophasic propylene copolymer (HECO) is multimodal in terms of its molecular weight and/or comonomer content.

In one embodiment of the present invention, the heterophasic propylene copolymer (HECO) is multimodal, both in terms of its molecular weight and comonomer content.

In the case where the heterophasic propylene copolymer (HECO) is multimodal in terms of its molecular weight and/or in terms of comonomer content, preferably at least the matrix (M) is multimodal in terms of its molecular weight.

In one embodiment of the present invention, the heterophasic propylene copolymer (HECO) is multimodal, where the matrix (M) is multimodal in terms of its molecular weight.

The heterophasic propylene copolymer (HECO) may comprise a first heterophasic propylene copolymer (HECO1) comprising a first polypropylene matrix (M1) and a first elastomeric

- 7 043072 copolymer (E1) dispersed in a first polypropylene matrix (M1), and a second heterophasic propylene copolymer (HECO2) containing a second polypropylene matrix (M2), and a second elastomeric copolymer (E2) dispersed in a second polypropylene matrix (M2) .

In one embodiment of the present invention, the heterophasic propylene copolymer (HECO) comprises a first heterophasic propylene copolymer (HECO1) comprising a first polypropylene matrix (M1) and a first elastomeric copolymer (E1) dispersed in the first polypropylene matrix (M1), and a second heterophasic propylene copolymer (HECO2) containing a second polypropylene matrix (M2) and a second elastomeric copolymer (E2) dispersed in the second polypropylene matrix (M2), wherein the heterophasic propylene copolymer (HECO1) and the heterophasic propylene copolymer (HECO2) differ from each other in molecular weight.

In this case, it should be understood that the heterophasic propylene copolymer (HECO2) and the heterophasic propylene copolymer (HECO1) together satisfy inequality (I), preferably inequality (Ib), more preferably inequality (Ic):

MFR [HECO2] /MFR [HECO1] > 1.0 (I);

> MFR [HECO2]/MFR [HECO1] >1.0 (Ib);

2.5 > MFR [HECO2] /MFR [HECO1] >1.5 (Ic), where MFR [HECO2] is the melt flow rate of MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of heterophasic propylene copolymer (HECO2) ;

MFR [HECO1] is the melt flow rate of MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of heterophasic propylene copolymer (HECO1).

In one embodiment of the present invention, the heterophasic propylene copolymer (HECO) comprises a first heterophasic propylene copolymer (HECO1) comprising a first polypropylene matrix (M1) and a first elastomeric copolymer (E1) dispersed in the first polypropylene matrix (M1), and a second heterophasic propylene copolymer (HECO2) comprising a second polypropylene matrix (M2) and a second elastomeric copolymer (E2) dispersed in the second polypropylene matrix (M2), wherein the first polypropylene matrix (M1) and the second polypropylene matrix (M2) differ from each other in molecular weight.

In this case, it should be understood that the matrix phase (M2) of the heterophasic propylene copolymer (HECO2) and the matrix phase (M1) of the heterophasic propylene copolymer (HECO1) together satisfy inequality (II), preferably inequality (IIb), more preferably inequality (IIc):

MFR [M2]/MFR [Ml] >1.0 (II);

> MFR [M2] /MFR [Ml] >1.0 (lib);

2.5 > MFR [M2]/MFR [Ml] > 1.5 (IIc), where MFR [M2] is the flow rate of the melt MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of the matrix phase (M2) heterophasic propylene copolymer (HECO2)

MFR [M1] is the melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of the matrix phase (M1) of heterophasic propylene copolymer (HECO1)

In other words, it should be understood that both polypropylene matrices, and (M1) heterophasic propylene copolymer (HECO1), and polypropylene matrix (M2) heterophasic propylene copolymer (HECO2), forming the polypropylene matrix (M) heterophasic propylene copolymer (HECO), differ from each other from each other by molecular weight.

The heterophasic propylene copolymer (HECO) cannot contain polymers other than heterophasic propylene copolymer (HECO1) and heterophasic propylene copolymer (HECO2) in an amount exceeding 10 wt.%, preferably in an amount exceeding 5 wt.%, more preferably in an amount exceeding 2.5% by weight, even more preferably in an amount greater than 0.8% by weight based on the total weight of the heterophasic propylene copolymer (HECO).

In one embodiment of the present invention, the heterophasic propylene copolymer (HECO) does not contain polymers other than heterophasic propylene copolymer (HECO1) and heterophasic propylene copolymer (HECO2) in an amount exceeding 10 wt.%, preferably in an amount exceeding 5 wt.%, more preferably in an amount greater than 2.5% by weight, even more preferably in an amount greater than 0.8% by weight based on the total weight of the heterophasic propylene copolymer (HECO).

In one embodiment of the present invention, heterophasic propylene copolymer (HECO1) and heterophasic propylene copolymer (HECO2) are the only polymers present in heterophasic propylene copolymer (HECO).

In one embodiment of the present invention, the heterophasic propylene copolymer (HECO) consists of a heterophasic propylene copolymer (HECO1) and a heterophasic propylene copolymer (HECO2).

Heterophasic propylene copolymer (HECO1).

It should be understood that heterophasic propylene copolymer (HECO) contains heterophasic propylene copolymer (HECO1) in an amount of not more than 49 wt.%, preferably in an amount of not more than

- 8 043072 than 35 wt.%, more preferably in an amount of not more than 30 wt.%; such as in the range from 5 to 49 wt.%, preferably in the range from 10 to 35 wt.%, more preferably in the range from 20 to 30 wt.% based on the total weight of the heterophasic propylene copolymer (HECO).

As stated above, it should be understood that the heterophasic propylene copolymer (HECO1) contains, preferably consists of:

(a) a polypropylene matrix (M1) and (b) an elastomeric copolymer (E1) containing units derived from propylene and ethylene and/or C ₄ -C ₂₀ α-olefins, preferably from ethylene and/or C ₄ -C ₁₀ α -olefins, more preferably only ethylene.

The polypropylene matrix (M1) may be a random propylene copolymer (RPP1) or a propylene homopolymer (HPP1), the latter being substantially preferred.

In one embodiment of the present invention, the polypropylene matrix (M1) is a propylene homopolymer (HPP1).

In the case where the polypropylene matrix (M1) is a propylene homopolymer (HPP1), the comonomer content of the polypropylene matrix (M1) may be equal to or less than 1.0 mass%, preferably equal to or less than 0.8 mass%, more preferably equal to or less than 0.5 wt.%, even more preferably equal to or less than 0.2 wt.% of the total weight of the polypropylene matrix (M1)

In the case where the polypropylene matrix (M1) is a random propylene copolymer (RPP1), it is understood that the random propylene copolymer (RPP1) contains, preferably consists of units derived from propylene and units derived from ethylene and/or C ₄ - C ₂₀ α-olefins, preferably propylene-derived units and ethylene-derived units and/or C ₄ -C ₁₀ α-olefins, more preferably propylene-derived units and ethylene-derived units and/or C ₄ , C ₆ and/or C ₈ α-olefins.

It will be understood that the random propylene copolymer (RPP1) contains, preferably consists of units derived from propylene and units derived from ethylene, 1-butene and/or 1hexene. In particular, it should be understood that the random propylene copolymer (RPP1) contains, in addition to propylene, only units derived from ethylene, 1-butene and/or 1-hexene.

In one embodiment of the present invention, the random propylene copolymer (RPP1) consists of propylene-derived units and ethylene-derived units.

The second component of the heterophasic propylene copolymer (HECO1) is an elastomeric copolymer (E1).

The elastomeric copolymer (E1) may contain propylene derived units and ethylene derived units and/or C ₄ -C ₂₀ α-olefins, preferably propylene derived units and ethylene and/or C _{4 -} derived units C ₁₀ α-olefins, more preferably units derived from propylene and units derived from ethylene and/or C ₄ , C ₆ and/or C ₈ α-olefins. The elastomeric copolymer (E1) may further contain units derived from conjugated dienes; such as butadiene, or non-conjugated dienes. Suitable non-conjugated dienes (dienes without conjugated double bonds), when used, include straight and branched acyclic dienes such as 1,4-hexadiene, 1,5-hexadiene, 1,6-octadiene, 5-methyl-1,4- hexadiene, 3,7-dimethyl1,6-octadiene, 3,7-dimethyl-1,7-octadiene, and mixtures of dihydromyrcene and dihydroocymene isomers, and single ring acyclic dienes such as 1,4-cyclohexadiene, 1,5- cyclooctadiene, 1,5cyclododecadiene, 4-vinyl cyclohexene, 1-allyl-4-isopropylidene cyclohexane, 3-allyl cyclopentene, 4-cyclohexene and 1-isopropenyl-4-(4-butenyl) cyclohexane.

However, preferably the elastomeric copolymer (E1) consists of units derived from propylene and units derived from ethylene and/or C ₄ -C ₂₀ α-olefins, preferably units derived from propylene and units derived from ethylene and/or C ₄ -C ₁₀ α-olefins, more preferably units derived from propylene and units derived from ethylene and/or C ₄ , C ₆ and/or C ₈ α-olefins.

In one embodiment of the present invention, the elastomeric copolymer (E1) consists of units derived from propylene and ethylene.

The heterophasic propylene copolymer (HECO1) may contain at least one α-nucleating agent. Additionally, preferably the heterophasic propylene copolymer (HECO1) does not contain any β-nucleating agents.

It will be appreciated that the information provided regarding suitable and preferred α-nucleating agents for heterophasic propylene copolymer (HECO) also applies to α-nucleating agents that may be contained in heterophasic propylene copolymer (HECO1) and is specifically indicated in this part.

Heterophasic propylene copolymer (HECO1), along with its individual components (matrix phase and elastomeric phase), can be obtained by mixing different types of polymers.

However, it should be understood that heterophasic propylene copolymer (HECO1) is obtained using a sequential polymerization process, that is, a multi-step method known in the art to which the present invention relates, wherein the polypropylene matrix (M1)

- 9 043072 is produced using at least one slurry reactor and optionally at least one gas-phase reactor, and then the elastomeric copolymer (E1) is produced using at least one gas-phase reactor, preferably two gas-phase reactors. Specifically, heterophasic propylene copolymer (HECO1) is produced by producing a polypropylene matrix (M1) using at least one reactor system including at least one reactor, transferring the polypropylene matrix (M1) to a subsequent reactor system including at least one reactor, in which an elastomeric propylene copolymer (E1) is obtained in the presence of a polypropylene matrix (M1).

In one embodiment of the present invention, a heterophasic propylene copolymer (HECO1) is produced using a sequential polymerization process wherein a polypropylene matrix (M1) is produced in a first reactor system including a slurry reactor (SL) and a first gas phase reactor (GPR1). Next, the polypropylene matrix (M1) is transferred to a second reactor system comprising a second gas phase reactor (GPR2) and a third gas phase reactor (GPR3), where the elastomeric copolymer (E1) is produced in the presence of the polypropylene matrix (M1).

A preferred multi-stage process is a gas-cycle process such as that developed by Borealis A/S, Denmark (known as BORSTAR® technology), described for example in patent documents such as EP 0887379, WO 92/12182, WO 2004/000899, WO 2004/111095, WO 99/24478, WO 99/24479 or WO 00/68315. An additional suitable gas-phase suspension process is the Spheripol® Basell process.

Heterophasic propylene copolymer (HECO1) is obtained in the presence of a catalytic system. Suitable catalyst systems are known to one skilled in the art and are selected according to need and need, however, it will be understood that the Ziegler-Natta catalyst system is used. Suitable Ziegler-natta catalyst systems are described, for example, in WO 2014/023603, EP 591224, WO 2012/007430, EP 2610271, EP 261027 and EP2610272.

The heterophasic propylene copolymer (HECO1) contains a polypropylene matrix (M1) and an elastomeric copolymer (E1) dispersed in a polypropylene matrix (M1). As stated above, the heterophasic propylene copolymer (HECO1) contains a polypropylene matrix (M1) and an elastomeric copolymer (E1) dispersed in the polypropylene matrix (M1).

It should be understood that the heterophasic propylene copolymer (HECO1) contains a polypropylene matrix (M1) ranging from 55 to 80 wt.%, preferably in the range from 60 to 70 wt.%, of the total weight of the heterophasic propylene copolymer (HECO1).

Additionally, it should be understood that the heterophasic propylene copolymer (HECO1) contains the elastomeric copolymer (E1) in the range of 20 to 45 wt.%, preferably in the range of 30 to 40 wt.% of the total weight of the heterophasic propylene copolymer (HECO1).

As stated above, the melt flow rate of the polypropylene matrix (M1) is a very important factor determining the properties of the polypropylene composition (C). It should be understood that the polypropylene matrix (M1) has a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of no more than 100 g/10 min, preferably no more than 80 g/10 min, more preferably no more than 70 g/10 min, even more preferably no more than 60 g/10 min; such as in the range from 5.0 to 100 g/10 min, preferably in the range from 10 to 80 g/10 min, more preferably in the range from 20 to 70 g/10 min, even more preferably in the range from 45 to 65 g /10 min.

In one embodiment of the present invention, the polypropylene matrix (M1) is a propylene homopolymer (HPP1).

In one embodiment of the present invention, the polypropylene matrix (M1) has a melt flow rate MFR ₂ (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 20 to 70 g/10 min.

In a preferred embodiment of the present invention, the polypropylene matrix (M1) is a propylene homopolymer (HPP1) with a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 20 to 70 g/10 min.

The heterophasic polypropylene copolymer (HECO1) may have a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of no more than 40 g/10 min, preferably no more than 25 g/10 min, more preferably no more than 15 g/10 min; such as in the range of 1 to 40 g/10 min, preferably in the range of 5 to 25 g/10 min, more preferably in the range of 8 to 15 g/10 min.

The heterophasic polypropylene copolymer (HECO1) may have a total comonomer content of no more than 40 mol%, preferably no more than 30 mol%, more preferably no more than 25 mol%; such as in the range of 5.0 to 40 mol%, preferably in the range of 10 to 30 mol%, more preferably in the range of 15 to 25 mol%.

The heterophasic polypropylene (HECO1) may have a xylene cold soluble fraction (XCS) content of no more than 55 wt.%, preferably no more than 45 wt.%, more preferably

- 10 043072 no more than 38 wt.%; such as in the range from 10 to 55 wt.%, preferably in the range from 20 to 45 wt.%, more preferably in the range from 25 to 38 wt.% of the total weight of heterophasic polypropylene (HECO1).

The heterophasic polypropylene (HECO1) may have an intrinsic viscosity (IV) of the xylene cold soluble fraction (XCS) of no more than 4.0 dl/g, preferably no more than 3.8 dl/g, more preferably no more than 3. 6 dl/g, even more preferably not more than 3.5 dl/g; such as in the range from 2.0 to 4.0 dl/g, preferably in the range from 25 to 3.8 dl/g, more preferably in the range from 3.0 to 3.6 dl/g, even more preferably in the range from 3.2 to 3.5 dl/g.

The heterophasic polypropylene (HECO1) may have a xylene cold soluble fraction (XCS) comonomer content of no more than 65 mol%, preferably no more than 60 mol%, more preferably no more than 50 mol%; such as in the range from 30 to 65 mol.%, preferably in the range from 35 to 60 wt.%, more preferably in the range from 45 to 52 mol.%.

In one embodiment of the present invention, heterophasic polypropylene (HECO1) has a melt flow rate MFR ₂ (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 1.0 to 50 g/10 min, total comonomer content ranging from 5.0 to 40 mol.%, content of the fraction soluble in cold xylene (XCS), ranging from 10 to 55 wt.% of the total mass of heterophasic polypropylene (HECO1), characteristic viscosity (IV) of the fraction soluble in cold xylene (XCS), ranging from 2.0 to 3.5 dl/g, and the comonomer content of the cold xylene soluble fraction (XCS), ranging from 30 to 65 mol.%.

In one embodiment of the present invention, heterophasic polypropylene (HECO1) has a melt flow rate MFR ₂ (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 5.0 to 25 g/10 min, total comonomer content in the range from 10 to 30 mol.%, the content of the fraction soluble in cold xylene (XCS), in the range from 20 to 45 wt.% of the total mass of heterophasic polypropylene (HECO1), intrinsic viscosity (IV) of the fraction soluble in cold xylene (XCS), ranging from 25 to 3.4 dl/g, and the content of the comonomer fraction, soluble in cold xylene (XCS), ranging from 35 to 60 mol.%.

In one embodiment of the present invention, heterophasic polypropylene (HECO1) has a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 8.0 to 15 g/10 min, total comonomer content in ranging from 10 to 30 mol.%, the content of the fraction soluble in cold xylene (XCS), ranging from 20 to 45 wt.% of the total mass of heterophasic polypropylene (HECO1), characteristic viscosity (IV) of the fraction soluble in cold xylene ( XCS), ranging from 2.9 to 3.2 dl/g, and the content of the comonomer fraction, soluble in cold xylene (XCS), ranging from 35 to 60 mol.%.

Heterophase copolymer of propylene (HECO2).

It should be understood that the heterophasic propylene copolymer (HECO) contains heterophasic propylene copolymer (HECO2) in an amount of at least 51 wt.%, preferably at least 65 wt.%, more preferably at least 70 wt.%; like in the range from 51 to 95 wt.%, preferably in the range from 65 to 90 wt.%, more preferably in the range from 70 to 80 wt.% of the total weight of the heterophasic propylene copolymer (HECO).

As stated above, it should be understood that the heterophasic propylene copolymer (HECO2) contains, preferably consists of:

(a) a polypropylene matrix (M2) and (b) an elastomeric copolymer (E2) containing units derived from propylene and ethylene and/or C4-C20 α-olefins, preferably from ethylene and/or C ₄ -C ₁₀ α-olefins , more preferably only ethylene.

The polypropylene matrix (M2) may be a random propylene copolymer (RPP2) or a propylene homopolymer (HPP2), the latter being substantially preferred.

In one embodiment of the present invention, the polypropylene matrix (M2) is a propylene homopolymer (HPP2).

In the case where the polypropylene matrix (M2) is a propylene homopolymer (HPP2), the comonomer content of the polypropylene matrix (M2) may be equal to or less than 1.0 mass%, preferably equal to or less than 0.8 mass%, more preferably equal to or less than 0.5 wt.%, even more preferably equal to or less than 0.2 wt.% of the total weight of the polypropylene matrix (M2).

In the case where the polypropylene matrix (M2) is a random propylene copolymer (RPP2), it is understood that the random propylene copolymer (RPP2) contains, preferably consists of propylene derived units and ethylene and/or C ₄ -derived units C ₂₀ α-olefins, preferably propylene-derived units and ethylene-derived units and/or C ₄ -C ₁₀ α-olefins, more preferably propylene-derived units and ethylene-derived units and/or C ₄ , C ₆ and/or C ₈ α-olefins.

It should be understood that the random propylene copolymer (RPP2) contains, preferably consists of units derived from propylene and units derived from ethylene, 1-butene and/or 1

- 11 043072 hexenes. In particular, it should be understood that random propylene copolymer (RPP2) contains, in addition to propylene, only units derived from ethylene, 1-butene and/or 1-hexene.

In one embodiment of the present invention, the random propylene copolymer (RPP2) consists of propylene-derived units and ethylene-derived units.

The second component of the heterophasic propylene copolymer (HECO2) is an elastomeric copolymer (E2).

The elastomeric copolymer (E2) may contain propylene derived units and ethylene derived units and/or C ₄ -C ₂₀ α-olefins, preferably propylene derived units and ethylene and/or C _{4 -} derived units C ₁₀ α-olefins, more preferably units derived from propylene and units derived from ethylene and/or C ₄ , C ₆ and/or C ₈ α-olefins.

The elastomeric copolymer (E2) may further comprise units derived from conjugated dienes; such as butadiene, or non-conjugated dienes. Suitable non-conjugated dienes (dienes without conjugated double bonds), when used, include straight and branched acyclic dienes such as 1,4-hexadiene, 1,5-hexadiene, 1,6-octadiene, 5-methyl-1,4hexadiene, 3,7-dimethyl-1,6-octadiene, 3,7-dimethyl-1,7-octadiene, and mixtures of dihydromyrcene and dihydroocymene isomers, and single ring acyclic dienes such as 1,4-cyclohexadiene, 1,5cyclooctadiene, 1,5-cyclododecadiene, 4-vinyl cyclohexene, 1-allyl-4-isopropylidene cyclohexane, 3-allyl cyclopentene, 4-cyclohexene and 1-isopropenyl-4-(4-butenyl) cyclohexane.

However, preferably the elastomeric copolymer (E2) consists of units derived from propylene and units derived from ethylene and/or C ₄ -C ₂₀ α-olefins, preferably units derived from propylene and units derived from ethylene and/or C ₄ -C ₁₀ α-olefins, more preferably units derived from propylene and units derived from ethylene and/or C ₄ , C ₆ and/or C ₈ α-olefins.

In one embodiment of the present invention, the elastomeric copolymer (E2) consists of units derived from propylene and ethylene.

The heterophasic propylene copolymer (HECO2) may contain at least one α-nucleating agent. Additionally, preferably the heterophasic propylene copolymer (HECO2) does not contain any β-nucleating agents.

It will be appreciated that the information provided regarding suitable and preferred α-nucleating agents for heterophasic propylene copolymer (HECO) also applies to α-nucleating agents that may be contained in heterophasic propylene copolymer (HECO2) and is specifically indicated herein.

Heterophasic propylene copolymer (HECO2), along with its individual components (matrix phase and elastomeric phase), can be obtained by mixing different types of polymers.

However, it should be understood that heterophasic propylene copolymer (HECO2) is obtained using a sequential polymerization process, that is, a multi-stage method known in the field of technology to which the present invention relates, wherein a polypropylene matrix (M2) is obtained using at least one suspension reactor and optionally at least one gas-phase reactor, and further the elastomeric copolymer (E2) is produced using at least one gas-phase reactor, preferably two gas-phase reactors. Specifically, heterophasic propylene copolymer (HECO2) is produced by producing a polypropylene matrix (M2) using at least one reactor system including at least one reactor, transferring the polypropylene matrix (M2) to a subsequent reactor system including at least one reactor, where an elastomeric propylene copolymer (E2) is obtained in the presence of a polypropylene matrix (M2).

In one embodiment of the present invention, a heterophasic propylene copolymer (HECO2) is produced using a sequential polymerization process wherein a polypropylene matrix (M2) is produced in a first reactor system including a slurry reactor (SL) and a first gas phase reactor (GPR1). Next, the polypropylene matrix (M2) is transferred to a second reactor system comprising a second gas phase reactor (GPR2) and a third gas phase reactor (GPR3), where the elastomeric copolymer (E2) is produced in the presence of the polypropylene matrix (M2).

A preferred multi-stage process is a gas-cycle process such as that developed by Borealis A/S, Denmark (known as BORSTAR® technology), described for example in patent documents such as EP 0887379, WO 92/12182, WO 2004/000899, WO 2004/111095, WO 99/24478, WO 99/24479 or WO 00/68315. An additional suitable gas-phase suspension process is the Spheripol® Basell process.

Heterophasic propylene copolymer (HECO2) is obtained in the presence of a catalytic system. Suitable catalyst systems are known to one skilled in the art and are selected according to need and need, however, it will be understood that the Ziegler-Natta catalyst system is used. Suitable Ziegler-natta catalyst systems are described, for example, in WO 2014/023603, EP 591224, WO 2012/007430, EP 2610271, EP 261027 and EP2610272.

- 12 043072

As stated above, heterophasic propylene copolymer (HECO2) contains a polypropylene matrix (M2) and an elastomeric copolymer (E2) dispersed in a polypropylene matrix (M2).

It should be understood that the heterophasic propylene copolymer (HECO2) contains a polypropylene matrix (M2) ranging from 55 to 80 wt.%, preferably in the range from 60 to 70 wt.% of the total weight of the heterophasic propylene copolymer (HECO2).

Additionally, it should be understood that the heterophasic propylene copolymer (HECO2) contains elastomeric copolymer (E2) in the range of 20 to 45 wt.%, preferably in the range of 20 to 40 wt.% of the total weight of the heterophasic propylene copolymer (HECO2).

As stated above, the melt flow rate of the polypropylene matrix (M2) is a very important factor determining the properties of the polypropylene composition (C). It will be understood that the polypropylene matrix (M2) has a melt flow rate MFR ₂ (230°C, 2.16 kg), as measured according to ISO 1133, of at least 70 g/10 min, preferably at least 80, more preferably according to at least 90 g/10 min, even more preferably at least 100 g/10 min; such as in the range from 70 to 180 g/10 min, preferably in the range from 80 to 160 g/10 min, more preferably in the range from 90 to 150 g/10 min, even more preferably in the range from 100 to 125 g/10 min.

In one embodiment of the present invention, the polypropylene matrix (M2) is a propylene homopolymer (HPP2).

In one embodiment of the present invention, the polypropylene matrix (M2) has a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 90 to 150 g/10 min.

In a preferred embodiment of the present invention, the polypropylene matrix (M2) is a propylene homopolymer (HPP2) with a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 90 to 150 g/10 min.

The heterophasic polypropylene copolymer (HECO2) may have a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of at least 6 g/10 min, preferably at least 16 g/10 min, more preferably at least 21 g/10 min; such as in the range of 6 to 50 g/10 min, preferably in the range of 16 to 40 g/10 min, more preferably in the range of 21 to 30 g/10 min.

The heterophasic polypropylene copolymer (HECO2) may have a total comonomer content of no more than 40 mol%, preferably no more than 30 mol%, even more preferably no more than 25 mol%; such as in the range of 5 to 40 mol%, preferably in the range of 10 to 30 mol%, more preferably in the range of 15 to 25 mol%.

The heterophasic polypropylene (HECO2) may have a xylene cold soluble fraction (XCS) content of no more than 55 wt%, preferably no more than 45 wt%, more preferably no more than 40 wt%; such as in the range from 10 to 55 wt.%, preferably in the range from 20 to 45 wt.%, more preferably in the range from 25 to 40 wt.% of the total weight of heterophasic polypropylene (HECO2).

The heterophasic polypropylene (HECO2) may have an intrinsic viscosity (IV) of the xylene cold soluble fraction (XCS) of no more than 3.5 dl/g, preferably no more than 3.4 dl/g, more preferably no more than 3. 3 dl/g, even more preferably not more than 3.2 dl/g; such as in the range of 2.0 to 3.5 dl/g, preferably in the range of 2.5 to 3.4 dl/g, more preferably in the range of 2.5 to 3.3 dl/g, even more preferably ranging from 2.9 to 3.2 dl/g.

The heterophasic polypropylene (HECO2) may have a xylene cold soluble (XCS) comonomer content of no more than 65 mol%, preferably no more than 60 mol%, more preferably no more than 50 mol%; such as in the range from 30 to 65 mol.%, preferably in the range from 35 to 60 wt.%, more preferably in the range from 45 to 55 mol.%.

In one embodiment of the present invention, heterophasic polypropylene (HECO2) has a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 6 to 50 g/10 min, total comonomer content ranging from 5 to 40 mol.%, content of the cold xylene soluble fraction (XCS), ranging from 10 to 55 wt.% of the total mass of heterophasic polypropylene (HECO2), intrinsic viscosity (IV) of the cold xylene soluble fraction (XCS) , ranging from 2.0 to 3.5 dl/g, and the content of the comonomer fraction, soluble in cold xylene (XCS), ranging from 30 to 65 mol.%.

In one embodiment of the present invention, heterophasic polypropylene (HECO2) has a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 16 to 40 g/10 min, total comonomer content ranging from 10 to 30 mol.%, content of the cold xylene soluble fraction (XCS), ranging from 25 to 45 wt.% of the total mass of heterophasic polypropylene (HECO2), intrinsic viscosity (IV) of the cold xylene soluble fraction (XCS) , ranging from 2.5 to 3.4 dl/g, and the content of the comonomer fraction, soluble in cold xylene (XCS), ranging from 35 to 60 mol.%.

In one embodiment of the present invention, heterophasic polypropylene (HECO2) has a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, ranging from 21 to 30 g/10 min, total comonomer content ranging from 15 to 25 mol.%, fraction content,

- 13 043072 cold soluble in xylene (XCS), ranging from 20 to 45 wt.% of the total mass of heterophasic polypropylene (HECO2), intrinsic viscosity (IV) of the fraction soluble in cold xylene (XCS), ranging from 2.9 up to 3.2 dl/g, and the content of the comonomer fraction, soluble in cold xylene (XCS), ranging from 35 to 60 mol.%.

Plastomer (PL).

The plastomer (PL) can be any elastomeric polyolefin, provided that it is chemically different from the elastomeric propylene copolymer (E), heterophasic propylene copolymer (HECO), along with the elastomeric propylene copolymer (E1), heterophasic propylene copolymer (HECO1), and the elastomeric propylene copolymer (HECO1). E2) heterophasic propylene copolymer (HECO2).

It will be understood that the plastomer (PL) is a low density polyolefin, even more preferably a low density polyolefin polymerized using metal single site catalysis.

The plastomer (PL) may be an elastomeric ethylene copolymer (EC) containing, preferably consisting of units derived from ethylene and at least another C ₄ -C ₂₀ α-olefin.

It should be understood that a plastomer (PL) is an elastomeric copolymer of ethylene (EC) containing, preferably consisting of units derived from ethylene and at least another C ₄ -C ₁₀ α-olefin.

In particular, it is to be understood that a plastomer (PL) is an elastomeric copolymer of ethylene (EC) containing, preferably consisting of units derived from ethylene and at least another α-olefin selected from the group consisting of 1-butene, 1-pentene , 1-hexene, 1-heptene and 1-octene, more preferably the elastomeric ethylene copolymer (EC) contains, preferably consists of units derived from ethylene and (ii) at least another α-olefin selected from the group consisting of 1-butene and 1-octene, even more preferably the elastomeric ethylene copolymer (EC) contains, preferably consists of units derived from ethylene and 1-octene.

In one embodiment of the present invention, the plastomer (PL) is an elastomeric ethylene copolymer (EC) containing, preferably consisting of units derived from ethylene and at least another α-olefin selected from the group consisting of 1-butene, 1-pentene, 1-hexene and 1-octene.

In a preferred embodiment of the present invention, the plastomer (PL) is an elastomeric ethylene copolymer (EC) consisting of units derived from ethylene and 1-octene.

It should be understood that the plastomer (PL) has a melt flow rate MFR2 (190°C, 2.16 kg), as measured according to ISO 1133, not more than 5.0 g/10 min, preferably not more than 2.5 g/ 10 min, more preferably not more than 1.5 g/10 min; such as in the range of 0.1 to 5.0 g/10 min, preferably in the range of 0.3 to 2.5 g/10 min, more preferably in the range of 0.5 to 1.5 g/10 min.

It will be understood that the plastomer (PL) has a density, as measured according to ISO 1183 187, of no more than 890 kg/m ³ , preferably no more than 880 kg/m ³ , more preferably no more than 860 kg/m ³ ; such as in the range from 830 to 890 kg/m ³ , preferably in the range from 840 to 880 kg/m ³ , more preferably in the range from 850 to 860 kg/m ³ .

In the case where the plastomer (PL) is an elastomeric ethylene copolymer (EC) consisting of units derived from ethylene and 1-octene, it is understood that the ethylene content of the elastomeric ethylene copolymer (EC) is at least 70 mol.%, preferably at least 80 mol.%; such as in the range of 70 to 99 mol%, preferably in the range of 80 to 90 mol%, more preferably 82 to 88 mol%.

Plastomer (PL) is known from the prior art and is commercially available. Suitable examples are Engage® 8842 from The Dow Chemical Company.

Filler (F).

As stated above, the finding of the present invention is that the paint adhesion of a polypropylene composition can be improved while maintaining sufficient stiffness and impact resistance by providing a specific heterophasic propylene copolymer in combination with a specific inorganic filler.

Therefore, the polypropylene composition (C) necessarily contains an inorganic filler (F).

Inorganic filler (F) is not included within the scope of the term additive, as described in more detail below.

It should be understood that the inorganic filler (F) is a mineral filler, in particular the mineral filler is selected from the group consisting of mica, wollastonite, kaolinite, montmorillonite, talc and mixtures thereof, preferably is a mineral filler selected from the group consisting of mica, wollastonite , talc and mixtures thereof, is even more preferably mica and/or talc.

In one embodiment of the present invention, the inorganic filler (F) - mineral filler is selected from the group consisting of mica, talc and mixtures thereof.

- 14 043072

In one embodiment of the present invention, the inorganic filler (F) is talc.

It will be understood that the inorganic filler (F) has a median particle size (D50) of no more than 5.0 µm, preferably no more than 3.0 µm, more preferably no more than 1.5 µm; such as in the range from 0.1 to 5.0 μm, preferably in the range from 0.3 to 3.0 μm, more preferably in the range from 0.5 to 1.5 μm.

It will be understood that the inorganic filler (F) has particle size limits (D95) of no more than 8.0 µm, preferably no more than 5.0 µm, more preferably no more than 4.0 µm; such as in the range from 0.5 to 8.0 µm, preferably in the range from 1.0 to 5.0 µm, more preferably in the range from 2.0 to 4.0 µm.

In one embodiment of the present invention, the inorganic filler (F) is a mineral filler selected from the group consisting of mica, wollastonite, talc and mixtures thereof, with a median particle size (D50) ranging from 0.1 to 5.0 μm and with particle size limits (D95) ranging from 0.5 to 8.0 microns.

In one embodiment of the present invention, the inorganic filler (F) is a mineral filler selected from the group consisting of mica, wollastonite, talc and mixtures thereof, with a median particle size (D50) ranging from 0.5 to 1.5 μm and with particle size limits (D95) ranging from 2.0 to 4.0 µm.

In one embodiment of the present invention, the inorganic filler (F) is talc with a median particle size (D50) ranging from 0.3 to 3.0 μm and a particle size range (D95) ranging from 1.0 to 5.0 μm .

In one embodiment of the present invention, the inorganic filler (F) is talc with a median particle size (D50) ranging from 0.5 to 1.5 μm and a particle size range (D95) ranging from 2.0 to 4.0 μm .

The inorganic filler (F) may have a BET specific surface area, as measured according to DIN 66131/2, of no more than 30 m ² /g, preferably no more than 20 m ² /g, more preferably no more than 18 m ² /g; such as in the range from 1.0 to 30.0 m ² /g, preferably in the range from 5.0 to 20.0 m ² /g, more preferably in the range from 10.0 to 18.0 m ² /g.

The inorganic filler (F) is known from the prior art and is commercially available. A suitable example is Jetfine®3CA of Imerys LLC.

Additives (AD).

In addition to heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F), the polypropylene composition (C) may contain additives (AD).

Typical additives include acid scavengers, antioxidants, colorants, light stabilizers, plasticizers, slip agents, scratch resistant agents, dispersants, processing aids, lubricants, pigments, antistatic agents, and the like.

Such additives are commercially available and are described, for example, in Plastic Additives Handbook, 6 ^th edition 2009 of Hans Zweifel (pages 1141 - 1190).

As stated above, as used in the specification of this patent application, the term additives (AD) does not include within the scope of the concept an inorganic filler (F), in particular a mineral filler (F) selected from the group consisting of mica, wollastonite, kaolinite, montmorillonite, talc and mixtures of them. In other words, the inorganic filler (F), in particular the mineral filler (F), selected from the group consisting of mica, wollastonite, kaolinite, montmorillonite, talc and mixtures thereof, is not considered as an additive.

However, as used herein, the term additives (AD) may also include carrier materials, in particular polymeric carrier materials (PCMs).

The polypropylene composition (C) may contain additives (AD) in an amount of not more than 10.0% by weight, preferably in an amount of not more than 5.0% by weight, more preferably in an amount of not more than 3.0% by weight, even more preferably in an amount of not more than 2.0% by weight; such as in the range from 0.1 to 10.0 wt.%, preferably in the range from 0.1 to 5.0 wt.%, more preferably in the range from 0.1 to 3.0 wt.%, even more preferably in the range from 0.1 to 2.0 wt.%, based on the total weight of the polypropylene composition (C).

The polypropylene composition (C) may contain additives selected from the group consisting of antioxidants, acid scavengers, anti-scratch agents, release agents, lubricants, UV stabilizers, and mixtures thereof.

Additives (AD) can be included in the polypropylene composition (C) as a separate ingredient. Alternatively, additives (AD) may be included in the polypropylene composition (C) along with at least one other component. For example, additives (AD) can be added to the polymer composition (C) together with heterophasic propylene copolymer (HECO), plastomer (PL) and/or inorganic filler (F), preferably in the form of a masterbatch (MB). Therefore, as used herein, the terms heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F) may refer to a composition including additives (AD).

- 15 043072

Additives (other than polymeric carrier materials (PCMs)) are typically added to the polypropylene composition (C) along with a carrier material, such as a polymeric carrier material (PCM), in the form of a masterbatch (MB).

Therefore, the polypropylene composition (C), consisting of heterophasic propylene copolymer (HECO), plastomer (PL) and inorganic filler (F), may additionally contain additives (AD).

Polymer carrier material (PCM).

As stated above, the polypropylene composition (C) cannot contain polymers other than heterophasic propylene copolymer (HECO) and plastomer (PL) in an amount exceeding 10 wt.%, preferably in an amount exceeding 5 wt.%, more preferably in an amount exceeding 2.5 wt.%, even more preferably in an amount exceeding 0.8 wt.% based on the total weight of the polypropylene composition (C).

In one embodiment of the present invention, the polypropylene composition (C) does not contain polymers other than heterophasic propylene copolymer (HECO) and plastomer (PL) in an amount greater than 0.8 wt.% of the total weight of the polypropylene composition (C).

In the case where an additional polymer is present, the polymer is typically a polymeric carrier material (PCM).

Polymeric carrier material (PCM) provides a polymeric carrier for other additives to ensure uniform distribution into the polypropylene composition (C). The polymer carrier material (PCM) is not limited to a specific polymer. The polymeric carrier material (PCM) may be an ethylene homopolymer, an ethylene copolymer such as an ethylene copolymer containing units derived from ethylene and units derived from C ₃ -C ₈ α-olefins, a propylene homopolymer, a propylene copolymer such as a copolymer propylene containing units derived from propylene and units derived from ethylene and/or C ₄ -C ₈ α-olefins and mixtures thereof.

Typically, the polymeric carrier material (PCM), as such, does not contribute to achieving the improved properties of the polypropylene composition (C).

It should be understood that the polymeric carrier material (PCM) is present in the polypropylene composition (C) in an amount of no more than 10 wt.%, preferably in an amount of no more than 5 wt.%, more preferably in an amount of no more than 2.5 wt. .%, even more preferably in an amount of not more than 0.8 wt.% of the total weight of the polypropylene composition (C).

In one embodiment of the present invention, the polymeric carrier material (PCM) is present in the polypropylene composition (C) in an amount of no more than 5 wt.% of the total weight of the polypropylene composition (C).

In a preferred embodiment of the present invention, the polymeric carrier material (PCM) is present in the polypropylene composition (C) in an amount of not more than 0.8 wt.% of the total weight of the polypropylene composition (C).

Product.

Additionally, the present invention relates to an article containing a polypropylene composition (C).

The article may comprise a polypropylene composition (C) in an amount of at least 80% by weight, preferably in an amount of at least 90% by weight, more preferably in an amount of at least 95% by weight; such as in the range from 80 to 99.9 wt.%, preferably in the range from 90 to 99.9 wt.%, more preferably in the range from 95 to 99.9 wt.%, based on the total weight of the polypropylene composition (C).

The product may be a cast product or an extruded product, preferably the product is a molded product such as an injection molded product or a compression molded product.

In one embodiment of the present invention, the product is an automotive product, in particular an automotive interior or exterior product such as instrument carriers, housings, structural carriers, bumpers, trim panels, running boards , body panels, spoilers, instrument panels, interior trim parts and the like.

Application.

Additionally, the present invention relates to the use of the above-mentioned polypropylene composition (C) for enhancing the adhesion of the paint coating of the above-mentioned product.

Examples

Definitions/measurement methods.

For the above description of the present invention, unless clearly stated otherwise, the following definitions of terms and methods of measurement apply in addition to the following examples.

Quantitative analysis of polymer microstructure using NMR spectroscopy.

Quantitative nuclear magnetic resonance (NMR) spectroscopy is used to evaluate the isotacticity and regioregularity of polypropylene homopolymers.

- 16 043072

Quantitative analysis ^{of the 13} C{1H} NMR spectrum was recorded in solution using a Bruker Advance III 400 NMR spectrometer operating at frequencies ranging from 400.15 to 100.62 MHz for 1H and ¹³ C, respectively. The entire spectrum is recorded using a ¹³ C optimized 10 mm linear sensor over an extended temperature range at 125° C using nitrogen gas throughout the pneumatics.

For propylene homopolymers, about 200 mg of material was dissolved in 3 ml of 1,2-tetrachloroethane-d ₂ (TCE-d ₂ ). To ensure homogeneity of the solution, after obtaining the initial sample in the thermoblock, the ampoule for NMR spectroscopy was additionally heated in an oven with a circular rotating hearth for at least 1 hour. When installed in the magnet, the ampoule was exposed to 10 Hz. This design was chosen primarily because of the need for high resolution quantitative analysis to accurately quantify the regularity of molecular structure (Busico, V., Cipullo, R., Prog. Polym. Sci. 26 (2001) 443; Busico, V. ; Cipullo, R., Monaco, G., Vacatello, M., Segre, A.L., Macromolecules 30 (1997) 6251). Created a standard single-pulse excitation without NOE at an optimized tilt angle with a 1-second cycle delay and a two-level WALTZ 16 decoupling circuit (Zhou, Z., Kuemmerle, R., Qiu, X., Redwine, D., Cong, R., Taha, A., Baugh, D. Winniford, V., J. Mag. Reson. 187 (2007) 225; Busico, V., Carbonniere, P., Cipullo, R., Pellecchia, R., Severn, J. , Talarico, G., Macromol. Rapid Commun. 2007, 28, 11289). A total of 8192 (8k) pulses were required for the spectrum.

A quantitative analysis was carried out based on ^{the 13} C{1H} NMR spectrum with a certain average value and the corresponding quantitative values were determined using the integral using special computer programs.

For propylene homopolymers, all chemical shifts essentially point to the methyl isotactic pentad (mmmm) at 21.85 ppm.

Signals corresponding to regiodefects or comonomers have been observed (Resconi, L., Cavallo, L., Fait, A., Piemontesi, F., Chem. Rev. 2000, 100, 1253; Wang, W-J., Zhu, S., Macromolecules 33 (2000), 1157; Cheng, H. N., Macromolecules 17 (1984), 1950).

The regularity of the distribution of molecular structure is quantified through the integration of the methyl region in the range of 23.6-19.7 ppm, corrected for any regions not associated with the stereosequence of interest (Busico, V., Cipullo, R., Prog. Polym. Sci 26 (2001) 443; Busico, V., Cipullo, R., Monaco, G., Vacatello, M., Segre, A. L., Macromolecules 30 (1997) 6251).

In particular, the effect of regiodefects and comonomer on the quantitative analysis of the regularity of the molecular structure distribution is corrected by subtracting the integrals of the representative regiodefect and comonomer from the specific region of the stereosequence integral.

Isotacticity was determined by the level of pentads and indicated as the percentage of isotactic pentad sequences (mmm) from the sequences of all pentads:

[mmmm] % = 100 * (mmmm / sum of all pentads).

The presence of 2.1 erythro regiodefects is indicated by the presence of two methyl areas at 17.7 and 17.2 ppm and is confirmed by other characteristic areas. No characteristic signals corresponding to other types of regiodefects were observed (Resconi, L., Cavallo, L., Fait, A., Piemontesi, F., Chem. Rev. 2000, 100, 1253).

Quantitative analysis of 2.1 erythroregiodefects was carried out using the average integral of two characteristic methyl sites of 17.7 and 17.2 ppm:

Р21е = (1е6 + 1е8) / 2

Quantitative analysis of 1,2 primary insertion propene is performed based on the methyl region, correcting for regions included in this region that are not associated with the primary insertion, and regions of the primary insertion excluded from this region:

Р12 = 1сНЗ + Р12е

The total amount of propene is quantified as the sum of the initially inserted propene and all other regional defects present:

Рtotal = Р12 + ?21е where total is total/total.

The molar percentage of 2.1 erythrioregiodefects is quantified from the total propene content:

[21e] mol.% = 100 * (P ₂ i _e / Ptotal).

The characteristic signals corresponding to the introduction of ethylene were observed (as reported in Cheng, H.N., Macromolecules 1984, 17, 1950), and the comonomer fraction was calculated as the fraction of ethylene in the polymer relative to all monomers in the polymer.

The comonomer fraction was quantified using the method of W.-J. Wang and S. Zhu, Macromolecules 2000, 33 1157 by integrating multiple signals from the entire spectral region of the ¹³ C{1H} spectrum. This method was chosen for its accuracy, reliability and ability to explain the presence of regional defects, if necessary. The integral regions were slightly adjusted to improve applicability to a wide range of comonomer contents.

- 17 043072

The molar percentage of introduced comonomer was calculated from the molar fraction.

The mass percentage of introduced comonomer was calculated from the molar fraction.

Melt flow rate MFR2 (230°C) is measured at 230°C with a load of 2.16 kg according to ISO 1133.

Melt flow rate MFR2 (190°C) is measured at 190°C with a load of 2.16 kg according to ASTM D1238.

The xylene cold soluble fraction (XCS) content was determined at 25°C according to ISO 16152; first edition 2005-07-01.

The intrinsic viscosity was measured according to DIN ISO 1628/1, October 1999 (in decalin at 135°C).

Tensile modulus of elasticity; Tensile failure stress was measured according to ISO 527-2 (ram speed=1 mm/min; 23°C) using injection molded specimens as described in EN ISO 1873-2 (dog bone shape, 4 mm thickness).

Relative elongation at the moment of rupture; Tensile yield strength is measured according to ISO 527-2 (ram speed=50 mm/min; 23°C) using injection molded specimens as described in EN ISO 1873-2 (dog bone shape, thickness 4 mm).

The Charly notched impact strength at +23°C (NIS+23) is determined according to ISO 1791eA:2000 using an injection molded test piece measuring 80x10x4 mm ³ produced in accordance with EN ISO 1873-2.

The Charly notched impact strength at -20°C (NIS-20) is determined according to ISO 1791eA:2000 using an injection molded test piece measuring 80x10x4 mm ³ produced in accordance with EN ISO 1873-2.

Particle size limits D95 (Sedimentation) are calculated from the particle size distribution [wt%] as determined using gravimetric liquid sedimentation ISO 13317-3 (Sedigraph).

Median particle size D50 (Sedimentation) is calculated from the particle size distribution [wt%] as determined using gravimetric liquid sedimentation ISO 13317-3 (Sedigraph).

The specific surface area of BET is measured according to DIN 66131/2 using nitrogen (N2).

Adhesion is characterized as the stability of a commercially produced scratch standard using a pressurized water jet according to DIN 55662 (Method C).

Injection-molded samples in the form of plates (150 mm x 80 mm x 2 mm) were washed using Zeller Gmelin Divinol® 1262. The surface was then activated by flaming using a burner with a speed of 670 mm/s with a mixture of propane (9 l/min) and air (180 l/min ) in a ratio of 1:20 on a polymer substrate. The polymer substrate was then coated with 2 layers, i.e. a base coat (Iridium Silver Metallic 117367) and a top coat (Carbon Creations® 107062). The flambéing stage was repeated twice.

A sprayed stream of hot water with a temperature T was directed over a time t to a distance d at an angle α to the surface of the test panel. The pressure of the water jet is a result of the speed of the water flow and is determined by the type of nozzle installed at the end of the water pipe.

The following parameters were used:

T (water) = 60°C;

t=60 s;

d=130 mm, α=90°, water flow rate 11.3 l/min, Nozzle type=MREO 2506.

Adhesion was assessed by quantifying the areas of damaged or peeling paint on the test line. For each example, 5 panels (size 80 mm x 150 mm x 2 mm) were tested. The panels were produced by injection molding at a melting temperature of 240°C and a mold temperature of 50°C. The frontal flow velocity was 100 mm/s and 400 mm/s, respectively.

Specific lines [ ^mm2 ] were used to assess paint damage on each panel. For this purpose, an image of the test point was obtained before and after exposure to the steam jet. Next, using image processing software, the area of detachment was calculated. The average area of damaged staining of 5 test lines with 5 test samples (ie, the overall average of 25 test points) was reported as the median area of damaged staining.

SD is the standard deviation, which is determined according to the following formula:

- *) ²

Sample Standard Deviation = -------J (η-υ

Sample Standard Deviation - Standard deviation of the sample where x - measured values;

F - average measured values and

- 18 043072 n - number of measurements.

Preparation of heterophasic propylene copolymer (HECO1).

Preparation of the catalyst.

First, 0.1 mol MgCl ₂ x3EtOH was suspended under inert conditions in 250 ml of decalin in a reactor at atmospheric pressure. The solution was cooled to a temperature of -15°C and 300 ml of cold TiCl ₄ was added with stirring, maintaining the temperature at the specified level. The temperature of the suspension was then slowly increased to 20°C. At this temperature, 0.02 mol of dioctyl phthalate (DOP) was added to the suspension. After adding the phthalate, the temperature was increased to 135°C for 90 minutes and the suspension was allowed to settle for 60 minutes. Then another 300 ml of TiCl ₄ was added and the temperature was maintained at 135°C for 120 minutes. After this, the catalyst was filtered from the liquid and washed six times with 300 ml of heptane at a temperature of 80°C. The solid catalyst component was then filtered and dried.

The catalyst and the general concept for its preparation are described, for example, in WO 87/07620, WO 92/19653, WO 92/19658 and EP 0 491 566, EP 591224 and EP 586390.

VCH modification.

To a 125 mL stainless steel reactor, 35 mL of mineral oil (Paraffinum Liquidum PL68) was added, followed by the addition of 0.82 g of triethylaluminum (TEAL) and 0.33 g of dicyclopentyldimethoxysilane (donor D) under inert conditions at room temperature. After 10 minutes, 5.0 g of the catalyst obtained in 1a (Ti content 1.4 wt.%) was added and after an additional 20 minutes, 5.0 g of vinylcyclohexane (VCH) was added. The temperature was raised to 60°C over 30 minutes and maintained for 20 hours. Finally, the temperature was lowered to 20°C and the concentration of unreacted VCH in the oil/catalyst mixture was analyzed and found to be 200 ppm by weight. Di(cyclopentyl) dimethoxysilane (donor D) was used as an external donor.

Preparation of polymer:

Heterophasic propylene copolymer (HECO1) is produced in a slurry reactor (SL) and a plurality of gas phase reactors connected in series (1st GPR, 2nd GPR and 3rd GPR). The applied conditions and properties of the resulting products are given in table. 1.

Table 1

Preparation of heterophasic propylene copolymer (HECO1)

HECO1 Pre-polymerization TEAL/Ti [mol/mol] 220 TEAL/Do [mol/mol] 7.3 Temperature [°C] thirty Stay time M 0.08 Circulating Temperature [°C] 72 Stream division (split) [%] 25 H2/C3 [mol/kmol] 15 C2/C3 [mol/kmol] 0 MFR2 [g/10 minutes] 55 XCS [mass%] 2.0 C2 [mol%] 0 1st GPR Temperature [°C] 80 Pressure [kPa] 2231 Stream division (split) [%] 40 H2/C3 [mol/kmol] 150 C2/C3 [mol/kmol] 0 MFR2 [g/10 minutes] 55 XCS [mass%] 2.0 C2 [mol%] 0 2nd GPR Temperature [°C] 70 Pressure [kPa] 2291 Stream division (split) [%] 20 C2/C3 [mol/kmol] 584 H2/C2 [mol/kmol] 117

- 19 043072

MFR ₂ [g/10 minutes] 20 XCS [mass%] 20 IV (XCS) [dl/g] But. C ₂ (XCS) [mol%] But. from ₂ [mol%] 18 3rd GPR Temperature [°C] 85 Pressure bar 1421 Stream division (split) [%1 15 С ₂ /Сз [mol/kmol] 585 n ₂ /s ₂ [mol/kmol] 93 mfr ₂ [g/10 minutes] eleven XCS [mass%] thirty IV (XCS) [dl/g] 3.5 C ₂ (XCS) [mol%] 50 from ₂ [mol%] 19 C ₂ - ethylene content H ₂ /C3 - hydrogen/propylene ratio C ₂ /C3 - ethylene/propylene ratio H ₂ / _C2 - hydrogen/ethylene ratio 1st 2nd 3rd GPR - 1st 2nd 3rd gas-phase reactor Circulation - circulation reactor TEAL/Ti - TEAL/Ti ratio TEAL/Do - TEAL / Donor ratio MFR ₂ - melt flow rate XCS - fraction soluble in cold xylene C ₂ (XCS) - ethylene content of the fraction soluble in cold xylene IV (XCS) - characteristic viscosity of the fraction soluble in cold

xylene

But. - not determined

Naturally, the properties of products obtained in individual reactors are determined not from homogenized material, but from samples from the reactor (local samples). The properties of the final polymer are determined from the homogenized material.

Preparation of heterophasic propylene copolymer (HECO2).

Preparation of the catalyst.

The catalyst used to produce heterophasic propylene copolymer (HECO2) is the same catalyst used to produce heterophasic propylene copolymer (HECO1).

Preparation of polymer.

Heterophase propylene copolymer (HECO2) is produced in a slurry reactor and a variety of gas phase reactors connected in series. The applied conditions and properties of the resulting products are given in table. 2.

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Table 2 Preparation of heterophasic propylene copolymer (HECO2)

HECO2 Circulating Temperature [°C] 72 Stream division (split) [%] 29 H2/C3 [mol/kmol] 21 C2/C3 [mol/kmol] 0 MFR2 [g/10 minutes] 115 XCS [mass%] But. C2 [mol%] 0 1st GPR Temperature [°C] 75 Pressure [kPa] 2000 Stream division (split) [%] 36 H2/C3 [mol/kmol] 204 C2/C3 [mol/kmol] 0 mfr ₂ [g/10 minutes] 115 XCS [mass%] But. C2 [mol%] 0 2nd GPR Temperature [°C] 85 Pressure [kPa] 2500 Stream division (split) [%] 22 C2/C3 [mol/kmol] 701 H2/C2 [mol/kmol] 85 mfr ₂ [g/10 minutes] 40 XCS [mass%] 20 IV (XCS) [dl/g] ZD C ₂ (XCS) [mol%] 50 c ₂ [mol%] 12 3rd GPR Temperature [°C] 85 Pressure bar 1400 Stream division (split) [%] 13 C2/C3 [mol/kmol] 699 H ₂ / C ₂ [mol/kmol] 129 MFR ₂ [g/10 minutes] 23 XCS [mass%] 29 IV (XCS) [dl/g] ZD C ₂ (XCS) [mol%] 50 c ₂ [mol%] 19

C2 - ethylene content

H2/C3 - hydrogen/propylene ratio

C2/C3 - ethylene/propylene ratio

H ₂ /C ₂ hydrogen/ethylene ratio

1st 2nd 3rd GPR - 1st 2nd 3rd gas phase reactor

Circulation - circulation reactor

TEAL/Ti - TEAL/Ti ratio

TEAL/Do - TEAL/Donor ratio

MFR2 - melt flow rate

XCS - fraction soluble in cold xylene

C2 (XCS) - content of ethylene fraction soluble in cold xylene

IV (XCS) - characteristic viscosity of the fraction soluble in cold xylene

But. - not determined

Naturally, the properties of products obtained in individual reactors are determined not from homogenized material, but from samples from the reactor (local samples). The properties of the final polymer are determined from the homogenized material.

Getting examples.

Examples of the present invention EE1, IE 2, IE3, IE4 and IE5 and comparative examples CE1, CE2 and CE3 are prepared by melt mixing using a twin screw extruder such as a Coperion STS-35 twin screw extruder from Coperion (Nanjing) Corporation, China. The average screw speed of two screw extruders was 400 rpm, the temperature profile of the zones was from 180 to 250°C.

Example of the present invention EE1, comparative examples CE1 and CE2 are based on the recipe, a brief description of which is given in table. 3.

- 21 043072

Table 3

Formulation for preparing the compositions of the present invention and comparative compositions

Example CE1 SE2 SEZ IE1 HECO1 [mass%]* 15.00 15.00 21.00 HECO2 [mass. %]* 50.15 50.15 54.15 54.15 NESOP [mass. %]* 10.00 10.00 21.00 Plastomer [mass. %]* 9.00 9.00 9.00 9.00 Filler! [mass. %]* 15.00 15.00 15.00 Filler 2 15.00

* The rest up to 100 wt.% are additives in their usual dosage, including polymeric carrier material, antioxidants, and UV stabilizers such as octadecyl 3-(3',5'di-tert-butyl-4-hydroxyphenyl)propionate in the form commercial antioxidant Irganox 1076 BASF, Germany, CAS-no. 2082-79-3, dyes such as Jet Black masterbatch Cabot Plasblak® PE1639 (40% Jet Black) from Cabot Corporation.

HECO3 is a commercial product ED007HP from Borealis AG, with a melt flow rate MFR2 (230°C, 2.16 kg) 7 g/10 min, content of the cold xylene soluble fraction (XCS) 27 wt.% of the total mass of the heterophasic propylene copolymer (HECO2), where the intrinsic viscosity (IV) of the xylene cold soluble fraction (XCS) is 6.3 dl/g.

Plastomer 1 is a commercial product from Engage® 8842 from The Dow Chemical Company, which is an ethylene/1-octene copolymer with a melt flow rate MFR2 (190°C, 2.16 kg) of 1.0 g/10 min and a density of 0.857 g/ cm ³ .

Filler 1 is a commercial product from Jetfme®TlCA from Imerys LLC, which is a talc with an average particle size (D50) of 1.0 µm, a particle size limit (D95) of 4.2 µm and a BET specific surface area of 14.5 m ² /g .

Filler2 is a commercial product Luzenac®HAR T84 from Imerys LLC, which is a talc with an average particle size (D50) of 11.5 microns and a specific surface area BET of 16.0 m ² /g.

Example of the present invention IE1, comparative examples CE1, CE2 and CE3 are based on the recipe, a brief description of which is given in table. 4.

Table 4

Formulation for obtaining compositions according to the present ____invention and comparative compositions____

Example MFR [g/10 minutes] CE1 10.8 SE2 9.8 SEZ 9.9 I.E. 12.1 XCS [mass%]* 30.9 30.9 30.0 31.5 IV (XCS) [dl/g] 3.4 3.4 3.7 3.1 tm [MPa] 1625 1786 1668 1586 Tensile Strength at Yield Strength (TS@Yield) [MPa] 18.2 18.8 19.0 17.1 Tensile Breaking Stress (TS@Break) [MPa] 12.6 12.2 13.5 12.3 Relative extension to moment of break (TE@Break) [%] 72 58 91 42 NIS+23 [kJ/ ^m2 ] 55.9 57.1 59.5 30.5 NIS-20 [kJ/ ^m2 ] 8.6 9.0 7.8 8.7

* Based on the total weight of the composition.

MFR-

Claims (20)

The adhesive properties of the example of the present invention EE1 and comparative examples CE1, CE2 and CE3 are shown in table. 5. Table 5 Adhesive properties of compositions of the present _______invention and comparative compositions_______ Example ICE, |CE2 SEZ 1 ^1E Paintability (100 mm/s Flow front) Average DA [mm ² ] 19 8 5 12 Median DA [mm ² ] 0 0 0 0 SD [mm ² ] 34 18 AND 24 Paintability (400 mm/s Flow front) Average DA [mm ² ] 70 95 87 41 Median DA [mm ² ] 64 92 79 29 SD [mm ² ] 59 37 53 42 Average DA - average area of detachment. Median DA - median area of detachment. SD - standard deviation. CLAIM 1. Polypropylene composition (C) containing: (a) from 70 to 80 parts by weight. heterophasic propylene copolymer (HECO), which contains: i) a polypropylene matrix (M), which is a homopolymer or copolymer of propylene containing units derived from propylene and ethylene and/or C ₄ -C ₂₀ α-olefins; and ii) an elastomeric copolymer (E) containing units derived from propylene and ethylene and/or C ₄ -C ₂₀ α-olefins; (b) from 7 to 12 parts by weight. plastomer (PL), which is an elastomeric ethylene copolymer (EC) containing units derived from ethylene and at least one C ₄ -C ₂₀ α-olefin; and (c) from 13 to 18 parts by weight. inorganic filler (F) from common parts by weight of compounds (a)-(c); wherein the polypropylene composition (C) has a cold xylene soluble fraction (XCS) content of at least 22% by weight of the total weight of the polypropylene composition (C) and an intrinsic viscosity (IV) of the cold xylene soluble fraction (XCS) of the composition polypropylene (C) is no more than 3.3 dl/g. 2. The polypropylene composition (C) according to claim 1, wherein the polypropylene composition (C) has a melt flow rate MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of at least 5 g/10 min, such as in the range from 5 to 50 g/10 min. 3. The polypropylene composition (C) according to claim 1 or 2, wherein the polypropylene composition (C) has a tensile modulus, as measured according to ISO 527-2, of at least 800 MPa, such as in the range from 800 to 2000 MPa. 4. The polypropylene composition (C) according to any one of claims 1 to 3, wherein the polypropylene composition (C) has an elongation at break, as measured according to ISO 527-2, of not more than 70%, such as in the range from 10 to 70%. 5. The polypropylene composition (C) according to any one of claims 1 to 4, wherein the polypropylene composition (C) has a Charlie cut strength (NIS+23), as measured according to ISO 179 1eA:2000 at +23°C, of at least at least 10 kJ/m ² , such as in the range from 10 to 80 kJ/m ² . 6. The polypropylene composition (C) according to any of the preceding claims 1-5, where the heterophasic propylene copolymer (HECO) contains: (a) from 5 to 49 parts by weight. the first heterophasic propylene copolymer (HECO1) and (b) from 51 to 95 parts by weight. a second heterophasic propylene copolymer (HECO2) from the common parts by weight of the heterophasic propylene copolymer (HECO1) and the heterophasic propylene copolymer (HECO2); wherein the first heterophasic propylene copolymer (HECO1) differs from the second heterophasic propylene copolymer (HECO2) in melt flow rate MFR ₂ (230°C, 2.16 kg), as measured according to ISO 1133. 7. The polypropylene composition (C) according to claim 6, where the heterophasic propylene copolymer (HECO2) and the heterophasic propylene copolymer (HECO1) together satisfy inequality (I) MFR [HECO2] /MFR [HECO1] > 1.0 (I); where MFR [HECO2] is the melt flow rate of MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of heterophasic propylene copolymer (HECO2); MFR [HECO1] is the melt flow rate of MFR2 (230°C, 2.16 kg), as measured according to ISO 1133, of heterophasic propylene copolymer (HECO1). - 23 043072 8. Polypropylene composition (C) according to claim 6 or 7, where: (a) the melt flow rate of MFR ₂ (230°C, 2.16 kg), as measured according to ISO 1133, of heterophasic propylene copolymer (HECO1) is not more than 40 g/10 min, such as in the range from 5 to 40 g /10 min; and/or (b) the melt flow rate of MFR ₂ (230°C, 2.16 kg), as measured according to ISO 1133, heterophasic propylene copolymer (HECO2) is at least 6 g/10 min, such as in the range of 6 up to 50 g/10 min. 9. Polypropylene composition (C) according to any of the preceding claims 6-8, where: (al) the heterophasic propylene copolymer (HECO1) contains a cold xylene soluble fraction ranging from 10 to 55% by weight of the total weight of the heterophasic propylene copolymer (HECO1); (a2) the xylene cold soluble (XCS) fraction of the heterophasic propylene copolymer (HECO1) contains comonomer units derived from C ₂ and/or C ₄ -Ci ₂ α-olefin, ranging from 30 to 65 mol.%; and (a3) the xylene cold soluble (XCS) fraction of the heterophasic propylene copolymer (HECO1) has an intrinsic viscosity (IV) of not more than 4.0 dl/g; and/or (N) the heterophasic propylene copolymer (HECO2) contains a fraction soluble in cold xylene, ranging from 10 to 55 wt.% of the total mass of the heterophasic propylene copolymer (HECO2); (b2) the xylene cold soluble (XCS) fraction of heterophasic propylene copolymer (HECO2) contains comonomer units derived from C ₂ and/or C ₄ -Ci ₂ α-olefin, ranging from 30 to 65 mol.% and ( b3) the xylene cold soluble (XCS) fraction of heterophasic propylene copolymer (HECO2) has an intrinsic viscosity (IV) of no more than 3.5 dl/g. 10. The polypropylene composition (C) according to any one of the preceding claims, wherein the plastomer (PL) is an elastomeric ethylene copolymer (EC) containing units derived from ethylene and at least one C ₄ -C ₂₀ a-olefin. 11. The polypropylene composition (C) according to any one of the preceding claims, wherein the plastomer (PL) is an elastomeric ethylene copolymer (EC) consisting of units derived from ethylene and 1-octene, having a melt flow rate MFR (190°C) as measured according to ASTM D1238, ranging from 0.1 to 5.0 g/10 min. 12. The polypropylene composition (C) according to any one of the preceding claims, wherein the plastomer (PL) is an elastomeric ethylene copolymer (EC) consisting of units derived from ethylene and 1-octene, having a density ranging from 830 to 890 kg/m ³ . 13. The polypropylene composition (C) according to any one of the preceding claims, wherein the plastomer (PL) is an elastomeric ethylene copolymer (EC) consisting of units derived from ethylene and 1-octene, having an ethylene content ranging from 70 to 99 mol.% . 14. The polypropylene composition (C) according to any of the preceding claims, wherein the inorganic filler (F) is a mineral filler. 15. The polypropylene composition (C) according to claim 14, wherein the inorganic filler (F) is talc with a median particle size (D50) of not more than 5.0 μm. 16. The polypropylene composition (C) according to claim 14 or 15, wherein the inorganic filler (F) is talc with a particle size limit (D95) of not more than 8.0 μm. 17. The polypropylene composition (C) according to any of the preceding paragraphs, where the polypropylene composition (C) does not contain polymers other than heterophasic copolymer of propylene (HECO) and plastomer (PL) in an amount exceeding 2.5 wt.% of the total weight of the polypropylene composition (WITH). 18. The polypropylene composition (C) according to any one of the preceding claims, wherein heterophasic propylene copolymer (HECO) and plastomer (PL) are the only polymers present in the polypropylene composition (C). 19. Product for the automotive industry containing the polypropylene composition (C) according to any of the preceding claims 1 to 18 in an amount of at least 80 wt.%. 20. The use of a polypropylene composition (C) according to any of the preceding claims 1 to 18 to enhance the adhesion of the paint coating of the product according to claim 19, where the product is a cast product. Eurasian Patent Organization, EAPO Russia, 109012, Moscow, Maly Cherkassky lane, 2