RU2818757C1 - Automotive composition - Google Patents

Abstract

FIELD: chemistry.

SUBSTANCE: present invention relates to a composition for automotive products obtained by mixing: (A) from 18.0 to 60.0 wt.%, based on total amount of composition, heterophase composition (HECO); (B) from 7.0 to 55.0 wt.%, based on the total amount of the composition, of the recovered polypropylene-polyethylene mixture (B); (C) from 0.0 to 12.0 wt.%, based on the total amount of the composition, high-density polyethylene (HDPE); (D) from 2.0 to 12.0 wt.%, based on the total amount of the composition, plastomer (P), and (E) from 7.0 to 25.0 wt.%, based on the total amount of the composition, talc (T), where said composition contains a total amount of 5.0 to 15.0 wt.% of polyethylene, which is the sum of said high-density polyethylene (HDPE) and polyethylene contained in said reclaimed polypropylene-polyethylene mixture (B); wherein heterophase composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together make at least 90 wt. % of the total amount of the composition; where also the heterophase composition (HECO) contains: (a) a propylene homopolymer as a matrix and (b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has (i) a melting point Tm, measured by DSC in accordance with ISO 11357-3 (heating and cooling rate of 10 °C/min), from 150 to 159 °C; (ii) melt flow index MFR₂ (230 °C, 2.16 kg), measured in accordance with ISO 1133, from 20.0 to 120 g/10 min; (iii) a crystalline fraction (CF) determined in accordance with the CRYSTEX QC ISO 6427 Appendix B method, present in amount of 79.0 to 91.0 wt.%, in terms of total weight of heterophasic propylene copolymer (HECO); (iv) a soluble fraction (SF), determined in accordance with the CRYSTEX QC ISO 6427 Appendix B method, present in amount of 9.0 to 21.0 wt.%, based on the total weight of the heterophase propylene copolymer (HECO); and (v) total content of ethylene, measured by Fourier transform infrared spectroscopy (FTIR) during CRYSTEX analysis, from 1.5 to 6.5 mol.%, wherein ethylene is the only comonomer in the heterophase composition (HECO); regenerated polypropylene-polyethylene mixture (B) contains: B-1) at least 85.0 wt.%, based on the total weight of the regenerated polypropylene-polyethylene mixture (B), polypropylene, B-2) is not more than 15.0 wt.%, in terms of total weight of regenerated polypropylene-polyethylene mixture (B), polyethylene, wherein the regenerated polypropylene-polyethylene mixture (B) has: i) melt flow index MFR₂ (230 °C, 2.16 kg), measured in accordance with ISO 1133, from 5.0 to 75 g/10 min; and ii) residual ash content, measured by thermogravimetric analysis according to ISO 11358-1, from 0.1 to 3.0 wt.%; and one or more of the following properties: iii) content of limonene, determined by solid phase micro-extraction (HS-SPME-GC-MS) from 0.1 ppm to 100 ppm; iv) content of fatty acid or acids, determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 to 100 ppm; v) content of polyamide or polyamides, determined by NMR, up to 1.5 wt.% and above detection limit; vi) content of polystyrene or polystyrenes, determined by NMR, from 0.05 to 3.0 wt.%; wherein the plastomer is a copolymer of ethylene and 1-octene or a copolymer of ethylene and 1-butene, having a density measured in accordance with ISO 1183-1 of 850 to 900 kg/m³.

EFFECT: reducing the amount of VOC contaminants release measured by VDA278 to less than 100 mcg per gram of the composition without detriment to mechanical characteristics.

15 cl, 1 dwg, 3 tbl

Description

The invention relates to a new composition suitable for automotive products, especially automotive interior trim products, comprising a low ethylene heterophasic propylene copolymer produced using a metallocene catalyst, a regenerated polypropylene-polyethylene blend, a plastomer and talc. The invention also relates to automotive products containing the specified composition.

It is well known that heterophasic propylene copolymers are used in the automotive industry mainly due to their low specific gravity and good performance. In some specific applications, such as automotive interior applications, low emission of pollutants is an important requirement. A significant drawback of existing technical solutions is that they have a fairly high level of emission of pollutants, mainly caused by polypropylene components. Typically, heterophasic propylene copolymers are characterized by a fairly large number of oligomers, which are mainly responsible for fairly high emissions of carbon compounds, for example high emissions of volatile organic compounds (VOCs) or emissions of fats, oils and greases (FOL). These values can be reduced to some extent due to washing stages, however, such stages complicate the production process and are environmentally unsafe. Some heterophasic propylene copolymers are already known to have fairly low pollutant release values, although they have a low melting point and/or low hardness.

Thus, one object of the present invention is to provide a heterophasic propylene copolymer composition that is useful for reducing the amount of pollutant emission of compositions applicable to automotive products, especially automotive interior products, without sacrificing mechanical properties, especially rigidity and impact resistance.

One of the fundamental problems in the polymer industry is recycling. Currently, the market for reclaimed materials, especially reclaimed materials from post-consumer waste, commonly referred to as PPP (post-consumer polymers), is somewhat limited. Starting with household waste, the sorting and separation processes used will not produce pure polymers, meaning there will always be some contaminants present, or the processes may even result in different polymers being mixed. When it comes to polyolefins, which make up the vast majority of the polymer fraction of collected municipal waste, perfect separation of polypropylene and polyethylene is almost impossible. Reclaimed polyolefin materials, especially post-consumer polymers, are traditionally cross-contaminated with non-polyolefin materials such as polyethylene terephthalate, polyamide, polystyrene, or non-polymer substances such as wood, paper, glass or aluminum. To make matters worse, these post-consumer reclaimed polyolefin materials are readily available on a multi-ton scale, but unfortunately have limited mechanical properties and often severe odor and/or contaminant release problems.

In addition to stringent requirements for the mechanical properties of their components, the automotive industry also has stringent requirements regarding odor and pollutant emissions, and the requirements are likely to become more stringent in the future. This severely limits the use of reclaimed materials in automotive applications.

However, there is a deeply felt need to allow post-consumer polyolefin reclaimed materials to be repurposed and reused in finished products without health and safety hazards.

This invention is based on the unexpected discovery that complex heterophasic polypropylene copolymers can be at least partially replaced by polypropylene-polyethylene blends derived from post-consumer reclaimed polyolefin streams.

SUMMARY OF THE INVENTION The discovery of this invention is to provide a composition comprising a heterophasic propylene copolymer prepared with a metallocene catalyst and having a low total ethylene content, a regenerated polypropylene-polyethylene blend, a plastomer, talc and optionally high density polyethylene (HDPE).

Accordingly, the present invention provides a composition containing

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 0.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) in this case from 5.0 to 15.0 wt. %, based on the total amount of the composition, is polyethylene, which is the sum of said high-density polyethylene (HDPE) and the polyethylene contained in said polypropylene-polyethylene mixture (B);

(E) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P); And

(F) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T);

and

heterophasic composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together make up at least 90 wt. % of the total amount of the composition;

where also

- heterophase composition (HECO) contains

(a) propylene homopolymer as matrix, and

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined in accordance with the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined in accordance with the CRYSTEX QC ISO 6427 Annex B method, present in an amount of 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO); And

(v) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) during the CRYSTEX analysis, from 1.5 to 6.5 mol. %, while ethylene is the only comonomer in the heterophasic composition (HECO);

- polypropylene-polyethylene mixture (B) contains:

B-1) at least 85.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polypropylene,

B-2) no more than 15.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polyethylene,

in this case, the polypropylene-polyethylene mixture (B) has:

i) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 5.0 to 75 g/10 min; And

ii) residual ash content, measured by thermogravimetric analysis, from 0.1 to 3.0 mass. %; and one or more of the following:

iii) limonene content determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 ppm to 100 ppm;

iv) fatty acid(s) content determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 to 100 ppm;

v) polyamide(s) content, determined by NMR, from 0 to 1.5 wt. %;

vi) polystyrene(s) content, determined by NMR, from 0.05 to 3.0 wt. %;

- wherein the plastomer is a copolymer of ethylene and 1-octene or a copolymer of ethylene and 1-butene having a density, measured in accordance with ISO 1183-1, from 850 to 900 kg/m ³ .

Alternatively, the invention relates to a composition containing

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 0.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) in this case from 5.0 to 15.0 wt. %, based on the total amount of the composition, is polyethylene, which is the sum of said high-density polyethylene (HDPE) and the polyethylene contained in said polypropylene-polyethylene mixture (B);

(E) from 2.0 to 12.0 wt. %, based on the total amount of composition, plastomer

(R); And

(F) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T);

and

heterophasic composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together make up at least 90 wt. % of the total amount of the composition;

where also

- heterophase composition (HECO) contains

(a) a propylene homopolymer as a matrix, wherein the propylene homopolymer has a 2,1-regiodefect content, determined by ¹³ C-NMR, from 0.05 to 0.90%, and

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 20.0 to 120 g/10 min;

(ii) crystalline fraction (CF), determined in accordance with the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iii) soluble fraction (SF), determined in accordance with the CRYSTEX QC ISO 6427 Annex B method, present in an amount of 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO); And

(iv) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) during the CRYSTEX analysis, from 1.5 to 6.5 mol. %, while ethylene is the only comonomer in the heterophasic composition (HECO);

- polypropylene-polyethylene mixture (B) contains:

B-1) at least 85.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polypropylene,

B-2) no more than 15.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polyethylene,

in this case, the polypropylene-polyethylene mixture (B) has:

i) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 5.0 to 75 g/10 min; And

ii) residual ash content, measured by thermogravimetric analysis, from 0.1 to 3.0 mass. %; and one or more of the following:

iii) limonene content determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 ppm to 100 ppm;

iv) fatty acid(s) content determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 to 100 ppm;

v) polyamide(s) content, determined by NMR, from 0 to 1.5 wt. %;

vi) polystyrene(s) content, determined by NMR, from 0.05 to 3.0 wt. %;

- wherein the plastomer is a copolymer of ethylene and 1-octene or a copolymer of ethylene and 1-butene having a density, measured in accordance with ISO 1183-1, from 850 to 900 kg/m ³ .

Accordingly, the invention particularly relates to a composition containing

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 0.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) in this case from 5.0 to 15.0 wt. %, based on the total amount of the composition, is polyethylene, which is the sum of said high-density polyethylene (HDPE) and the polyethylene contained in said polypropylene-polyethylene mixture (B);

(E) from 2.0 to 12.0 wt. %, based on the total amount of composition, plastomer

(R); And

(F) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T);

and

heterophasic composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together make up at least 90 wt. % of the total amount of the composition;

where also

- heterophase composition (HECO) contains

(a) a propylene homopolymer as a matrix, wherein the propylene homopolymer has a 2,1-regiodefect content, determined by ¹³ C-NMR, from 0.05 to 0.90%, and

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined in accordance with the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined in accordance with the CRYSTEX QC ISO 6427 Annex B method, present in an amount of 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO); And

(v) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) during the CRYSTEX analysis, from 1.5 to 6.5 mol. %, while ethylene is the only comonomer in the heterophasic composition (HECO);

- polypropylene-polyethylene mixture (B) contains:

B-1) at least 85.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polypropylene,

B-2) no more than 15.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polyethylene,

in this case, the polypropylene-polyethylene mixture (B) has:

i) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 5.0 to 75 g/10 min; And

ii) residual ash content, measured by thermogravimetric analysis, from 0.1 to 3.0 mass. %; and one or more of the following:

iii) limonene content determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 ppm to 100 ppm;

iv) fatty acid(s) content determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 to 100 ppm;

v) polyamide(s) content, determined by NMR, from 0 to 1.5 wt. %;

vi) polystyrene(s) content, determined by NMR, from 0.05 to 3.0 wt. %;

- wherein the plastomer is a copolymer of ethylene and 1-octene or a copolymer of ethylene and 1-butene having a density, measured in accordance with ISO 1183-1, from 850 to 900 kg/m ³ .

Other preferred embodiments of the composition according to the invention are defined in the dependent claims.

In addition, this invention relates to an automobile product, especially an automobile product containing at least 95 wt. %, preferably consisting of a composition containing

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 0.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P); And

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T);

and

heterophasic composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together make up at least 90 wt. % of the total amount of the composition;

where also

- heterophase composition (HECO) contains

(a) a propylene homopolymer as a matrix, wherein the propylene homopolymer has a 2,1-regiodefect content, determined by ¹³ C-NMR, from 0.05 to 0.90%, and

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined in accordance with the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined in accordance with the CRYSTEX QC ISO 6427 Annex B method, present in an amount of 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO); And

(v) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) during the CRYSTEX analysis, from 1.5 to 6.5 mol. %, while ethylene is the only comonomer in the heterophasic composition (HECO);

- polypropylene-polyethylene mixture (B) contains:

B-1) at least 85.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polypropylene,

B-2) no more than 15.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polyethylene,

in this case, the polypropylene-polyethylene mixture (B) has:

i) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 5.0 to 75 g/10 min; And

ii) residual ash content, measured by thermogravimetric analysis, from 0.1 to 3.0 mass. %;

- wherein the plastomer is a copolymer of ethylene and 1-octene or a copolymer of ethylene and 1-butene having a density, measured in accordance with ISO 1183-1, from 850 to 900 kg/m ³ .

The invention is described in more detail below.

Definitions

Unless otherwise defined, all technical and scientific terms used in this description have the same meaning as commonly understood by one skilled in the art to which the invention pertains.

Although any methods and materials similar or equivalent to those described herein may be practiced to test the invention, preferred materials and methods are described herein. The specification and claims use the following terminology as defined below. Unless expressly stated otherwise, use of a characteristic in the singular refers to one or more such characteristics.

For the purposes of this description, the term "recovered waste" or "reclaimed material" is used to refer to material recovered from both post-consumer waste and industrial waste, as opposed to virgin polymers. Post-consumer waste refers to objects that have completed at least their first use cycle (or life cycle), that is, they have already served their first purpose. In contrast, industrial waste refers to production scrap, or conversion scrap, which usually does not reach the consumer.

The term “virgin” refers to newly produced materials and/or items prior to their first use that have not yet been regenerated. Virgin and post-consumer materials can be easily distinguished based on the absence or presence of contaminants such as limonene and/or fatty acids and/or paper and/or wood. Polypropylene-polyethylene mixtures can also be distinguished regarding their origin by the presence of polystyrene and/or polyamide. Residual content refers to content exceeding the detection limit.

A polymer blend is a mixture of two or more polymer components. In general, a mixture can be prepared by mixing two or more polymer components. A suitable mixing procedure known in the art is post-polymerization mixing. Post-polymerization mixing may be dry mixing of polymer components, such as polymer powders and/or compounded polymer granules, or melt mixing by melt mixing the polymer components.

Many different types of polyethylene or polypropylene may be present in the "reclaimed material".

A random propylene copolymer is a copolymer of propylene monomer units and comonomer units, in which the comonomer units are randomly distributed along the polypropylene chain. “Polypropylene-polyethylene blend” refers to a composition containing both polypropylene and polyethylene, including also propylene copolymers as well as ethylene copolymers. Since direct determination of each of these components is not possible, the content of polypropylene and polyethylene, as defined in this invention, is determined by the content of C2 and C3, determined by calibration using isotactic PP (iPP) and HDPE.

The term "plastomer" refers to a natural or synthetic polymer that has both elastic and plastic properties.

The term "XCS" refers to the xylene cold soluble content (XCS wt.%) determined at 25°C in accordance with ISO 16152.

The term "CSG" refers to the xylene cold insoluble content (XCI wt.%) determined at 25°C in accordance with ISO 16152.

Unless otherwise stated, "%" refers to mass. %.

A heterophasic propylene copolymer, having a propylene homopolymer as a matrix and obtained in the presence of a metallocene catalyst, is characterized by a melting point below 160°C, but above 150°C. In addition, a heterophasic propylene copolymer having a propylene homopolymer as a matrix and obtained in the presence of a metallocene catalyst contains 2,1-regiodefects in the matrix phase. In contrast, heterophasic propylene copolymers, having a propylene homopolymer as a matrix and obtained in the presence of a Ziegler-Natta catalyst, have a significantly higher melting point, i.e. above 160°C, and do not exhibit 2,1-regiodefects.

The presence of heterophase nature can be easily determined by the number of glass transition points. A reactor mixture is a mixture resulting from production in two or more reactors connected in series, or in a reactor having two or more reaction compartments. The reactor mixture can alternatively be prepared by mixing in solution. The reactor mixture is different from the combination obtained by melt extrusion.

Detailed description

Composition

As stated above, the composition according to the invention must contain a heterophasic composition (HECO), a polypropylene-polyethylene mixture (B), a plastomer (P), talc (T) and optionally high-density polyethylene (HDPE). It is especially preferable that the inventive composition consists of the above components and possibly additional additives. However, the composition according to the invention should preferably not contain additional polymers.

Accordingly, the composition according to the invention preferably contains

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 0.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P); And

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T);

and

heterophasic composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together make up at least 90 wt. %, preferably at least 90.0 wt. %, of the total amount of the composition;

and from 5.0 to 15.0 wt. %, based on the total amount of the composition, is polyethylene, which is the sum of said high-density polyethylene (HDPE) and the polyethylene contained in said polypropylene-polyethylene mixture (B).

Accordingly, particularly preferably, the composition according to the invention contains

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 2.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P); And

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T);

where the specified composition contains a total amount of from 5.0 to 15.0 wt. %, polyethylene, representing the sum of the specified high-density polyethylene (HDPE) and the polyethylene contained in the specified polypropylene-polyethylene mixture (B);

and

heterophasic composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together make up at least 90 wt. %, preferably at least 90.0 wt. %, of the total amount of the composition.

Even more preferably, the composition according to the invention consists of

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 0.0 to 12.0 wt. %, based on the total amount of composition, high-density polyethylene (HDPE); F

(D) from 2.0 to 12.0 wt. %, based on the total amount of composition, plastomer

(R);

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T); And

(F) from 1.0 to 10.0 wt. %, preferably from 1.0 to 5.0 wt.% based on the total amount of the composition, additives (A),

where the specified composition contains a total amount of from 5.0 to 15.0 wt. %, polyethylene, being the sum of said high-density polyethylene (HDPE) and the polyethylene contained in said polypropylene-polyethylene mixture (B).

Even more preferably, the composition according to the invention consists of

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 2.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D)from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P);

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T); And

(F) from 1.0 to 10.0 wt. %, preferably from 1.0 to 5.0 wt.%, based on the total amount of the composition, additives (A),

where the specified composition contains a total amount of from 5.0 to 15.0 wt. %, polyethylene, representing the sum of the specified high-density polyethylene (HDPE) and the polyethylene contained in the specified polypropylene-polyethylene mixture (B)/

Preferably, the composition according to the invention has a melt flow index MTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 10.0 to 30.0 g/10 min.

It is therefore preferred that the composition according to the invention has a melt flow index MFR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 10.0 to 30.0 g/10 min and contains

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 0.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P); And

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T);

where the specified composition contains a total amount of from 5.0 to 15.0 wt. %, polyethylene, representing the sum of the specified high-density polyethylene (HDPE) and the polyethylene contained in the specified polypropylene-polyethylene mixture (B);

and

- heterophasic composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together make up at least 90 mass. % of the total composition

And

- optionally, the weight ratio between the first heterophasic composition (HECO) and the polypropylene-polyethylene mixture (B) [(HECO)/(B)] is from 0.2 to 8.0, preferably from 0.3 to 6.0.

Even more preferably, the composition according to the invention has a melt flow index MTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 10.0 to 30.0 g/10 min and consists of

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 2.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P);

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T); And

(F) from 1.0 to 10.0 wt. %, preferably from 1.0 to 5.0 wt.% based on the total amount of the composition, additives (A);

where the specified composition contains a total amount of from 5.0 to 15.0 wt. %, polyethylene, representing the sum of the specified high-density polyethylene (HDPE) and the polyethylene contained in the specified polypropylene-polyethylene mixture (B);

and, possibly, the mass ratio between the heterophase composition

(HECO) and polypropylene-polyethylene mixture (B) [(HECO)/(B)] is from 0.2 to 8.0, preferably from 0.3 to 6.0.

Even more preferably, the composition according to the invention contains

(A) from 16.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 0.0 to 12.0 wt. %, preferably from 2 to 12 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P); And

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T);

where the specified composition contains a total amount of from 5.0 to 15.0 wt. %, polyethylene, representing the sum of the specified high-density polyethylene (HDPE) and the polyethylene contained in the specified polypropylene-polyethylene mixture (B);

and

- heterophase composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together make up at least 90 mass. % of the total amount of the composition,

And

- the mass ratio between the heterophasic composition (HECO) and the polypropylene-polyethylene mixture (B) [(HECO)/(B)] is from 0.2 to 8.0, preferably from 0.3 to 6.0,

Moreover, the composition also has

- melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 10.0 to 30.0 g/10 min;

- flexural modulus of elasticity, measured in accordance with ISO 178, from 1600 to 2400 MPa;

- Charpy impact strength of a notched sample (UVSHN), measured in accordance with ISO 179 1 eA at +23°C, from 4.5 to 45.0 kJ/m ² , preferably from 5.0 to 40.0 kJ/ m ² ; And

- Charpy impact strength of a notched sample (UVSHN), measured in accordance with ISO 179 1 eA at -20°C, from 1.8 to 8.0 kJ/m ² , preferably from 2.0 to 7.0 kJ/ m ² .

In particular, it is preferable when the composition according to the invention consists of

(A) from 16.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 2.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P);

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T); And

(F) from 1.0 to 10.0 wt. %, preferably from 1.0 to 5.0 wt.% based on the total amount of the composition, additives (A);

where the specified composition contains a total amount of from 5.0 to 15.0 wt. %, polyethylene, representing the sum of the specified high-density polyethylene (HDPE) and the polyethylene contained in the specified polypropylene-polyethylene mixture (B);

wherein the weight ratio between the heterophasic composition (HECO) and the polypropylene-polyethylene mixture (B) [(HECO)/(B)] is from 0.2 to 8.0, preferably from 0.3 to 6.0,

Moreover, the composition also has

- melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 10.0 to 30.0 g/10 min;

- flexural modulus of elasticity, measured in accordance with ISO 178, from 1600 to 2400 MPa;

- Charpy impact strength of a notched sample (UVSHN), measured in accordance with ISO 179 1 eA at +23°C, from 4.5 to 45.0 kJ/m ² , preferably from 5.0 to 40.0 kJ/ m ² ; And

- Charpy impact strength of a notched sample (UVSHN), measured in accordance with ISO 179 1 eA at -20°C, from 1.8 to 8.0 kJ/m ² , preferably from 2.0 to 7.0 kJ/ m ² .

The composition of the invention can be prepared by compounding the components in suitable melt mixing devices to produce polymer compositions, including in particular extruders such as single screw extruders as well as co-rotating or counter-rotating twin screw extruders. Other suitable melt mixing devices include planetary extruders and single screw mixers. Particularly preferred are co-rotating twin screw extruders incorporating high intensity mixing and mixing sections. Suitable melt temperatures for preparing the compositions are from 170 to 300°C, preferably from 200 to 260°C.

The composition according to the invention, in particular the composition described in the previous embodiments, preferably has a low VOC pollution emission value, measured according to VDA278, of less than 100 μg per gram of composition, more preferably from 10 to 90 μg per gram of composition, most preferably from 15 to 75 mcg per gram of composition.

The composition according to the invention, in particular the composition described in the previous embodiments, is further preferably characterized by a low FOG measured according to VDA278 of less than 320 μg per gram of composition, more preferably from 25 to 300 μg per gram of composition, most preferably from 30 to 280 mcg per gram of composition.

Below, the components present in the composition according to the invention are described in more detail.

Heterophasic propylene copolymer (HECO)

Heterophasic propylene copolymer (HECO) is a heterophasic system understood by one skilled in the art. That is, heterophasic propylene copolymer (HECO) contains a matrix that is a propylene homopolymer in which ethylene-propylene rubber is dispersed. In other words, the expression "heterophasic" indicates that the ethylene-propylene rubber is (finely) dispersed in the matrix. In other words, EPDM forms inclusions in the matrix. Thus, the matrix contains (finely) dispersed inclusions that are not part of the matrix, and said inclusions are ethylene-propylene rubber. The term "inclusion" according to this invention preferably indicates that the matrix and inclusion form different phases within the heterophasic propylene copolymer, said inclusions being, for example, visible by high resolution microscopy such as electron microscopy or scanning force microscopy.

The heterophasic propylene copolymer (HECO) of the invention is prepared using a metallocene catalyst, especially a metallocene catalyst as defined in more detail below. Accordingly, the heterophasic propylene copolymer (HECO) according to the present invention has a melting point Tm, measured by DSC according to ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C, preferably from 153 to 158°C, and/or the content of 2,1-regiodefects in the matrix, that is, in the propylene homopolymer, from 0.05 to 0.90%, preferably from 0.25 to 0.85, determined by ¹³ C-NMR.

In addition, the heterophasic propylene copolymer (HECO) according to the present invention is characterized by a rather low ethylene content. Ethylene is the only comonomer in heterophasic propylene copolymer (HECO). Accordingly, the total ethylene content of the heterophasic propylene copolymer (HECO) measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis ranges from 1.5 to 6.5 mol. %, more preferably from 1.7 to 6.0 mol. %, for example from 1.9 to 5.8 mol. %, with ethylene being the only comonomer in the heterophasic composition (HECO).

In addition, the heterophasic propylene copolymer (HECO) of the present invention is further characterized by a relatively low amount of ethylene-propylene rubber, which is reflected in the relatively low amount of soluble fraction (SF) measured by the CRYSTEX analysis. That is, the heterophasic propylene copolymer (HECO) according to this invention has

(a) the crystalline fraction (CF), determined by the CRYSTEX QC ISO 6427 Annex B method, present in an amount between 79.0 and 91.0 mass. %, preferably from 80.5 to 90.5 wt. %, for example from 81.0 to 90.0 wt. %, based on the total amount of heterophasic propylene copolymer (HECO), and

(b) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount of from 9.0 to 21.0 mass. %, preferably from 9.5 to 19.5 wt. %, for example from 10.0 to 19.0 wt. %, based on the total amount of heterophasic propylene copolymer (HECO).

The crystalline fraction (CF) is dominated by the matrix, i.e. heterophasic propylene homopolymer (HECO), while the soluble fraction (SF) is dominated by the rubber component, i.e. heterophasic ethylene propylene rubber (HECO). Accordingly, preferably, the heterophasic composition (HECO) contains

(a) from 79.0 to 91.0 wt. %, more preferably from 80.5 to 90.5 wt. %, based on the total amount of heterophasic composition (HECO), propylene homopolymer; And

(b) from 9.0 to 21.0 wt. %, more preferably from 9.5 to 19.5 wt. %, based on the total amount of heterophasic composition (HECO), ethylene-propylene rubber.

In addition, the heterophasic composition (HECO) has a melt flow index MFR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 20.0 to 120 g/10 min.

It is also preferable that the ethylene content in the soluble fraction (C2(SF)) of the heterophasic composition (HECO), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, is from 22.0 to 39.0 mol. %, more preferably from 25.0 to 35.0 mol. %.

In addition, the ethylene content in the crystalline fraction (C2(CF)) of the heterophasic composition (HECO), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, ranges from 0.0 to 0.7 mol. %, more preferably from 0.0 to 0.5 mol. %.

In addition, it is preferable that the matrix and rubber, that is, the crystalline fraction (CF) and the soluble fraction (SF), have a specific molecular weight. Accordingly, it is preferable when

(i) the intrinsic viscosity of the soluble fraction (IV(SF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), is from 1.80 to 3.20 dl/g, more preferably from 2.00 to 3.00 dl/g, for example 2.20 to 2.80 dl/g;

(ii) the intrinsic viscosity of the crystalline fraction (IV(CF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), is from 0.80 to 1.80 dl/g, more preferably from 1.00 to 1.60 dl/g, and

(iii) the ratio of the intrinsic viscosity of the soluble fraction (SF) to the intrinsic viscosity of the crystalline fraction (CF) [IV(SF)/IV(CF)] of the heterophasic composition (HECO) is from 1.50 to 2.80, more preferably from 1, 60 to 2.70, for example, from 1.70 to less than 2.60.

Accordingly, the heterophasic composition (HECO) contains

(a) propylene homopolymer as matrix, and

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined according to the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount from 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO), and

(v) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 1.5 to 6.5 mol. %.

In a preferred embodiment, the heterophasic composition (HECO) contains

(a) propylene homopolymer as matrix, and

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined according to the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount from 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(v) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 1.5 to 6.5 mol. %;

(vi) ethylene content in the soluble fraction (C2(SF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 22.0 to 39.0 mol. %, and, perhaps,

(vii) ethylene content in the crystalline fraction (C2(CF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 0.0 to 0.7 mol. %.

In a more preferred embodiment, the heterophasic composition (HECO) contains

(a) a propylene homopolymer as a matrix, in which the propylene homopolymer has 2,1-regiodefects, determined by ¹³ C-NMR, from 0.05 to 0.90%, and

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined according to the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount from 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(v) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 1.5 to 6.5 mol. %;

(viii) ethylene content in the soluble fraction (C2(SF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 22.0 to 39.0 mol. %, and, perhaps,

(ix) ethylene content in the crystalline fraction (C2(CF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 0.0 to 0.7 mol. %.

In an even more preferred embodiment, the heterophasic composition (HECO) contains

(a) propylene homopolymer as matrix

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133 from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined according to the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount from 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(v) intrinsic viscosity of the soluble fraction (IV(SF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 1.80 to 3.20 dl/g;

(vi) intrinsic viscosity of the crystalline fraction (IV(CF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 0.80 to 1.80 dl/g;

(vii) the ratio of the intrinsic viscosity of the soluble fraction (SF) to the intrinsic viscosity of the crystalline fraction (CF) [IV(SF)/IV(CF)] of the heterophasic composition (HECO) from 1.50 to 2.80;

(viii) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 1.5 to 6.5 mol. %;

(ix) ethylene content in the soluble fraction (C2(SF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis from 22.0 to 39.0 mol. %, and, perhaps,

(x) ethylene content in the crystalline fraction (C2(CF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 0.0 to 0.7 mol. %.

In an even more preferred embodiment, the heterophasic composition (HECO) contains

(a) a propylene homopolymer as a matrix, in which the propylene homopolymer has 2,1-regiodefects, determined by ¹³ C-NMR, from 0.05 to 0.90%, and

(b) ethylene-propylene rubber dispersed in said matrix,

in this case, heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined according to the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount from 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(v) intrinsic viscosity of the soluble fraction (IV(SF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 1.80 to 3.20 dl/g;

(vi) intrinsic viscosity of the crystalline fraction (IV(CF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 0.80 to 1.80 dl/g;

(vii) the ratio of the intrinsic viscosity of the soluble fraction (SF) to the intrinsic viscosity of the crystalline fraction (CF) [IV(SF)/IV(CF)] of the heterophasic composition (HECO) from 1.50 to 2.80;

(viii) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 1.5 to 6.5 mol. %;

(ix) ethylene content in the soluble fraction (C2(SF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 22.0 to 39.0 mol. %, and, perhaps,

(x) ethylene content in the crystalline fraction (C2(CF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 0.0 to 0.7 mol. %.

In a specific embodiment, the heterophasic composition (HECO) contains

(a) a propylene homopolymer as a matrix, in which the propylene homopolymer has 2,1-regiodefects, determined by ¹³ C-NMR, from 0.05 to 0.90%, and

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined according to the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount from 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(v) intrinsic viscosity of the soluble fraction (IV(SF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 1.80 to 3.20 dl/g;

(vi) intrinsic viscosity of the crystalline fraction (IV(CF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 0.80 to 1.80

dl/g;

(vii) the ratio of the intrinsic viscosity of the soluble fraction (SF) to the intrinsic viscosity of the crystalline fraction (CF) [IV(SF)/IV(CF)] of the heterophasic composition (HECO) from 1.50 to 2.80;

(viii) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 1.5 to 6.5 mol. %;

(ix) ethylene content in the soluble fraction (C2(SF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 22.0 to 39.0 mol. %, and, perhaps,

(x) ethylene content in the crystalline fraction (C2(CF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 0.0 to 0.7 mol. %.

In a very special embodiment, the heterophasic composition (HECO) contains

(a) a propylene homopolymer as a matrix, in which the propylene homopolymer has 2,1-regiodefects, determined by ¹³ C-NMR, from 0.05 to 0.90%, and

(b) ethylene-propylene rubber dispersed in said matrix,

in this case, heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 153 to 158°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined according to the CRYSTEX QC method ISO 6427 Annex B, present in an amount of from 80.5 to 90.5 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount of from 9.5 to 19.5 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(v) intrinsic viscosity of the soluble fraction (IV(SF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 2.30 to 2.80 dl/g;

(vi) intrinsic viscosity of the crystalline fraction (IV(CF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 1.00 to 1.40 dl/g;

(vii) the ratio of the intrinsic viscosity of the soluble fraction (SF) to the intrinsic viscosity of the crystalline fraction (CF) [IV(SF)/IV(CF)] of the heterophasic composition (HECO) from 1.65 to 2.65;

(viii) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 1.7 to 4.5 mol. %;

(ix) ethylene content in the soluble fraction (C2(SF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 25.0 to 35.0 mol. %, and, perhaps,

(x) ethylene content in the crystalline fraction (C2(CF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 0.0 to 0.5 mol. %.

The polymerization to obtain a heterophasic composition (HECO) is described in detail below.

The heterophasic composition (HECO) according to this invention can be produced in a reactor cascade of two or more reactors, preferably three reactors. Polymerization methods suitable for preparing the heterophasic composition (HECO) according to the invention are known in the art. They involve at least two polymerization steps, in which the polymerization is typically carried out in solution, suspension, bulk or gas phase. Typically, the polymerization process includes additional polymerization steps or reactors. In one particularly preferred embodiment, the polymerization process includes at least one volumetric reactor and at least two gas phase reactors arranged in this order. The process may further include pre- and post-reactors. Pre-reactors typically include pre-polymerization reactors. In this type of process, it is preferable to use higher polymerization temperatures to achieve specific polymer properties. Typical temperatures in these processes are 65°C or higher, preferably 75°C or higher. Higher polymerization temperatures, as mentioned previously, can be used in some or all of the reactors of the reactor cascade, preferably in the first gas phase reactor.

The preferred multi-stage process is a "loop reactor gas phase reactor" process such as developed by Borealis (known as BORSTAR® technology), described for example in patent literature such as EP 0887379, WO 92/12182, WO 2004/000899, WO 2004/ 111095, WO 99/24478, WO 99/24479 or WO 00/68315. Another suitable slurry gas phase process is the Spheripol® process from Basell.

As noted above, the heterophasic composition (HECO) according to this invention is specifically prepared by a polymerization process using a metallocene catalyst having formula (I)

where each of the R ¹ , which are independently the same or may be different, represents hydrogen or a linear or branched C ₁ -C ₆ alkyl group, and at least one R ¹ per phenyl group is not hydrogen,

R' represents a C ₁ -C ₁₀ hydrocarbyl group, preferably a C ₁ -C ₄ hydrocarbyl group and more preferably a methyl group and

X independently represents a hydrogen atom, a halogen atom, a C ₁ -C ₆ alkoxy group, a C ₁ -C _b alkyl group, a phenyl or a benzyl group.

Most preferably X represents chlorine, benzyl or methyl group. Preferably both X groups were the same. The most preferred options are two chlorides, two methyl or two benzyl groups, especially two chlorides.

Specific preferred metallocene catalysts according to the invention include:

rac-anti-dimethylsilanediyl[2-methyl-4,8-bis-(4'-tert-butylphenyl)-1,5,6,7-tetrahydro-s-indacen-1-yl][2-methyl-4] dichloride -(3',5'-dimethylphenyl)-5-methoxy-6-tert-butylinden-1-yl]zirconium

rac-anti-dimethylsilanediyl[2-methyl-4,8-bis-(3',5'-dimethylphenyl)-1,5,6,7-tetrahydro-s-indacen-1-yl][2-methyl- 4-(3',5'-dimethylphenyl)-5-methoxy-6-tert-butylinden-1-yl]zirconium

rac-anti-dimethylsilanediyl[2-methyl-4,8-bis-(3',5'-dimethylphenyl)-1,5,6,7-tetrahydro-s-indacen-1-yl][2-methyl- 4-(3',5'-di-tert-butylphenyl)-5-methoxy-6-tert-butylinden-1-yl]zirconium

or corresponding analogues of dimethyl zirconium compounds.

The most preferred catalyst is rac-anti-dimethylsilanediyl[2-methyl-4,8-bis-(3',5'-dimethylphenyl)-1,5,6,7-tetrahydro-s-indacen-1-yl][ 2-methyl-4-(3',5'-dimethylphenyl)-5-methoxy-6-tert-butylinden-1-yl]zirconium

The ligands required to form the complexes and hence the catalysts of the invention can be synthesized by any method, and a skilled organic chemist will be able to develop various synthetic protocols for the preparation of the required ligand materials. For example, WO2007/116034 discloses the required chemistry. Synthesis protocols can also generally be found in WO 2002/02576, WO 2011/135004, WO 2012/084961, WO 2012/001052, WO 2011/076780, WO 2015/158790 and WO 2018/122134. Of particular note is WO 2019/179959, which describes the most preferred catalyst of the present invention. The examples section also provides sufficient guidance to one skilled in the art.

Cocatalyst

To form active catalytic molecules it is generally necessary to use a cocatalyst, as is well known in the art.

According to the present invention, a cocatalyst system comprising a boron cocatalyst and/or an alumoxane cocatalyst is used in combination with the metallocene catalyst complex defined above.

The alumoxane sotalizer may be one of the compounds of formula (III):

where n is typically between 6 and 20, and R has the meaning given below.

Alumoxanes are formed by partial hydrolysis of organoaluminum compounds, for example compounds of the formula AlR3, AlR ₂ Y and Al ₂ R ₃ Y ₃ , where R can be, for example, C ₁ -C ₁₀ alkyl, preferably C ₁ -C ₅ alkyl, or C _{3 -10} cycloalkyl, C ₇ -C ₁₂ arylalkyl or alkylaryl and/or phenyl or naphthyl, and where Y may be hydrogen, halogen, preferably chlorine or bromine, or C ₁ -C ₁₀ alkoxy, preferably methoxy or ethoxy. The resulting oxygen-containing alumoxanes are generally not pure compounds, but mixtures of oligomers of formula (III).

A preferred alumoxane is methylaluminoxane (MAO). Since the alumoxanes used according to the invention as co-catalysts are not, due to the method of their preparation, pure compounds, the indication of the molarity of the alumoxane solutions is further based on their aluminum content.

According to the invention, instead of an alumoxane co-catalyst, a boron-containing co-catalyst can also be used, or an aluminoxane co-catalyst can be used in combination with a boron-containing co-catalyst.

One skilled in the art will appreciate that when boron-based cocatalysts are used, it is common to pre-alkylate the complex by reacting it with an alkylaluminum compound such as triisobutylaluminum (TIBA). This procedure is well known and any suitable aluminum alkyl can be used, for example Al(C ₁ -C ₆ -alkyl) ₃ . Preferred alkylaluminum compounds are triethylaluminum, triisobutylaluminum, triisohexylaluminum, tri-n-octylaluminum and triisooctylaluminum.

Alternatively, when using a borate cocatalyst, the metallocene catalyst complex is present in its alkylated version, that is, for example, a dimethyl or dibenzyl metallocene catalyst complex can be used.

Boron-based cocatalysts of interest include cocatalysts of formula (IV)

BY ₃ (IV)

wherein Y, the same or different, represents a hydrogen atom, an alkyl group of 1 to about 20 carbon atoms, an aryl group of 6 to about 15 carbon atoms, an alkylaryl, arylalkyl, haloalkyl, or haloaryl, each having from 1 to 10 carbon atoms in an alkyl radical and from 6 to 20 carbon atoms in an aryl radical, or fluorine, chlorine, bromine or iodine. Preferred examples of Y are methyl, propyl, isopropyl, isobutyl or trifluoromethyl, unsaturated groups such as aryl or haloaryl, for example phenyl, tolyl, benzyl groups, p-fluorophenyl, 3,5-difluorophenyl, pentachlorophenyl, pentafluorophenyl, 3,4, 5-trifluorophenyl and 3,5-di(trifluoromethyl)phenyl. Preferred options are trifluoroborane, triphenylborane, tris(4-fluorophenyl)borane, tris(3,5-difluorophenyl)borane, tris(4-fluoromethylphenyl)borane, tris(2,4,6-trifluorophenyl)borane, tris(pentafluorophenyl)borane , tris(tolyl)borane, tris(3,5-dimethylphenyl)borane, tris(3,5-difluorophenyl)borane and/or tris(3,4,5-trifluorophenyl)borane.

Particular preference is given to tris(pentafluorophenyl)borane.

However, it is preferable to use borates, that is, compounds containing the 3+ borate ion. Such ionic cocatalysts preferably contain a non-coordinating anion such as tetrakis(pentafluorophenyl) borate and tetraphenyl borate. Suitable counterions are protonated amine or aniline derivatives such as methylammonium, anilinium, dimethylammonium, diethylammonium, N-methyl anilinium, diphenylammonium, N,N-dimethylanilinium, trimethylammonium, triethylammonium, tri-n-butylammonium, methyldiphenylammonium, pyridinium, p-bromo-N,N-dimethylanilinium or p-nitro-N,N-dimethylanilinium.

Preferred ionic compounds that can be used according to the invention include:

triethyl ammonium tetra(phenyl)borate,

tributylammonium tetra(phenyl)borate,

trimethylammonium tetra(tolyl)borate,

tributylammonium tetra(tolyl)borate,

tributylammonium tetra(pentafluorophenyl)borate,

tripropyl ammonium tetra(dimethylphenyl) borate,

tributylammonium tetra(trifluoromethylphenyl)borate,

tributylammonium tetra(4-fluorophenyl)borate,

N,N-dimethylcyclohexylammonium tetrakis(pentafluorophenyl)borate,

N,N-dimethylbenzylammonium tetrakis(pentafluorophenyl)borate,

N,N-dimethylanilinium tetra(phenyl)borate,

N,N-diethylanilinium tetra(phenyl)borate,

N,N-dimethylanilinium tetrakis(pentafluorophenyl)borate,

N,N-di(propyl)ammonium tetrakis(pentafluorophenyl)borate,

di(cyclohexyl)ammonium tetrakis(pentafluorophenyl)borate,

triphenylphosphonium tetrakis(phenyl)borate,

triethylphosphonium tetrakis(phenyl)borate,

diphenylphosphonium tetrakis(phenyl)borate,

tri(methylphenyl)phosphonium tetrakis(phenyl)borate,

tri(dimethylphenyl)phosphonium tetrakis(phenyl)borate,

triphenylcarbenium tetrakis(pentafluorophenyl)borate,

or ferrocenium tetrakis(pentafluorophenyl)borate.

Preference is given to triphenylcarbenium tetrakis(pentafluorophenyl)borate,

N,N-dimethylcyclohexylammonium tetrakis(pentafluorophenyl)borate or

N,N-dimethylbenzylammonium tetrakis(pentafluorophenyl)borate.

It has surprisingly been discovered that certain boron cocatalysts are particularly preferred. Thus, preferred borates used in the invention contain trityl ion. Thus, it is therefore particularly preferred to use N,N-dimethylammonium tetrakispentafluorophenylborate and Ph ₃ CB(PhF ₅ ) ₄ and analogs thereof.

According to the invention, preferred cocatalysts are alumoxanes, more preferably methylaluminoxanes, combinations of alumoxanes with Al-alkyl, boron or borate cocatalysts, and combinations of alumoxanes with boron-based cocatalysts.

Suitable amounts of cocatalyst are well known to those skilled in the art.

The molar ratio of boron to metallocene metal ion may be from 0.5:1 to 10:1 mol/mol, preferably from 1:1 to 10:1, especially from 1:1 to 5:1 mol/mol.

The molar ratio of Al in the alumoxane to metallocene metal ion may be from 1:1 to 2000:1 mol/mol, preferably from 10:1 to 1000:1, and more preferably from 50:1 to 500:1 mol/mol.

The catalyst can be used in supported or unsupported form, preferably in supported form. The particulate support material used is preferably an organic or inorganic material such as silica, alumina or zirconium oxide, or a mixed oxide such as an aluminosilicate, in particular silica, alumina or aluminosilicate. Preferably, the carrier is silica. One skilled in the art will know the procedures required to apply the metallocene catalyst.

Particularly preferably, the support is a porous material so that the complex can be loaded into the pores of the support, for example, using a process similar to that described in WO 94/14856 (Mobil), WO 95/12622 (Borealis) and WO 2006/097497.

The average particle size of the silica carrier can generally be from 10 to 100 μm. However, it has turned out that particular advantages can be obtained if the carrier has an average particle size of from 15 to 80 μm, preferably from 18 to 50 μm.

The average pore size of the silica carrier can be from 10 to 100 nm, and the pore volume can be from 1 to 3 ml/g.

Examples of suitable support materials are, for example, ES757 manufactured and sold by PQ Corporation, Sylopol 948 manufactured and sold by Grace, or SUNSPERA DM-L-303 silica manufactured by AGC Si-Tech Co. The supports can be further calcined before use in catalyst preparation to achieve optimal silanol group content.

The use of these media is common in the art.

Polypropylene-polyethylene mixture (B)

The polypropylene-polyethylene mixture (B) according to the invention contains

B-1) at least 85.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polypropylene,

B-2) no more than 15.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B,) polyethylene

At the same time, the polypropylene-polyethylene mixture (B) has

- melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 5.0 to 75 g/10 min, preferably from 7.0 to 50 g/10 min, more preferably from 9.0 to 30 g/10 min; And

- residual ash content from 0.1 to 3.0 mass. %, preferably from 0.5 to 2.7 wt. %, more preferably from 0.7 to 2.5 wt. %.

The polypropylene-polyethylene mixture (B) according to the invention is preferably a reclaimed material. It is particularly preferred that the polypropylene-polyethylene mixture (B) according to the invention occurs in an amount of at least 90 wt. % from post-consumer and/or industrial waste, more preferably from post-consumer waste.

The polypropylene-polyethylene mixture (B) according to the invention may have one or more of the following properties

a) limonene content, determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 parts per million (ppm) to 100 ppm, preferably from 0.1 ppm to 50 ppm, more preferably 0.1 ppm to 20 ppm, most preferably 0.1 ppm to 5 ppm;

b) fatty acid(s) content determined by solid phase microextraction (HS-SPME-GC-MS) from 0.1 to 100 ppm;

c) polyamide(s) content, determined by NMR, from 0 to 1.5 wt. %;

d) polystyrene(s) content, determined by NMR, from 0.05 to 3.0 wt. %;

e) residual ash content as stated above.

It should be understood that the polypropylene-polyethylene blend (B) can vary widely in composition, that is, it can include propylene homopolymers, propylene copolymers, ethylene homopolymers, and ethylene copolymers. Since direct determination of each of these components is not possible, the content of polypropylene and polyethylene, as defined in this invention, is determined by the content of C2 and C3, determined by calibration using iPP and HDPE.

Typically, the polypropylene-polyethylene mixture (B) according to the invention may also have one or more of the following properties:

- residual PET content, determined as described in the experimental part;

- residual content of talc and chalk, as described in the experimental part;

- residual metal content (determined by X-ray fluorescence (XRF))

- residual amount of paper, as described in the experimental part

- residual amount of wood, as described in the experimental part.

The polypropylene-polyethylene mixture (B) according to the invention is preferably obtained through washing and/or aeration steps, as is known in the art.

Plastomer

The composition according to the invention further contains a plastomer, which is a copolymer of ethylene and 1-octene or a copolymer of ethylene and 1-butene, having a density, measured according to ISO 1183-1, from 850 to 900 kg/m ³ , preferably from 860 to 890 kg/m ³ .

Preferably the plastomer has a melt flow index MTR ₂ (190°C, 2.16 kg), measured according to ISO 1133, from 1.5 to 15.0 g/10 min, preferably from 2.0 to 10.0 g/10 min .

Particularly preferably, the plastomer is an ethylene-1-octene copolymer having a density measured according to ISO 1183-1 of 850 to 900 kg/m ³ and a melt flow index MFR ₂ (190° C., 2.16 kg) measured according to ISO 1133, from 1.5 to 15.0 g/10 min.

According to one embodiment, the plastomer is a copolymer of ethylene and 1-octene having a density, measured according to ISO 1183-1, from 860 to 890 kg/m ³ and a melt flow index MFR ₂ (190 ° C, 2.16 kg), measured according to ISO 1133, from 2.0 to 10.0 g/10 min.

In one preferred embodiment, the plastomer is prepared with at least one metallocene catalyst. The plastomer may also be formulated with more than one metallocene catalyst or may be a mixture of several elastomers formulated with different metallocene catalysts. In some embodiments, the plastomer is a substantially linear ethylene polymer (SLEP). SLEP plastomers and other plastomers prepared with metallocene catalysts are known in the art, for example from US 5272236. These polymers are also commercially available, for example, Queo™ plastomers available from Borealis AG (Austria), ENGAGE™ plastomer resins available from Dow Chemical Co. (USA) or EXACT™ polymers from ExxonMobil (USA) or TAFMER™ polymers from Mitsui (Japan).

High Density Polyethylene (HDPE)

According to a preferred embodiment of the present invention, the composition further comprises high density polyethylene (HDPE).

High density polyethylene (HDPE) preferably has a density, measured in accordance with ISO 1183-1, from 940 to 970 kg/m ³ .

In addition, preferably high density polyethylene (HDPE) has a fairly low melt flow rate. Accordingly, the melt flow index of PTR ₂ (190°C, 2.16 kg), measured in accordance with ISO 1133, of high density polyethylene (HDPE) is preferably from 1.0 to 30.0 g/10 min, more preferably from 2 .0 to 20.0 g/10 min.

Preferably, the high density polyethylene (HDPE) of the invention is a high density polyethylene known in the art. In particular, it is preferable if the high density polyethylene (HDPE) is a commercial ethylene homopolymer "HE9621-PH" from Borealis AG.

Talc

Another essential component of this invention is talc (T). Preferably, talc (T) has a mean median particle size ( _d50 ) of 0.3 to 3.0 μm and a top particle size ( _d95 ) of 0.5 to 10.0 μm, measured in accordance with ISO 13317-3.

According to one embodiment, talc (T) has an average median particle size (d ₅₀ ) from 0.5 to 2.5 μm and a top particle size (d ₉₅ ) from 1.0 to 8.0 μm, measured according to ISO 13317-3 .

According to the invention, talc (T) does not belong to the class of alpha-nucleating agents and additives (A).

Talc (T) is a product known in the art and produced in industry.

Additives (A)

The composition according to the invention may additionally contain additives (A). Typical additives are acid scavengers, nucleating agents, antioxidants, dyes, light stabilizers, glidants, anti-scratch agents, dispersants, processing aids, lubricants, pigments, carbon black masterbatches, etc.

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

Supplements are usually supplied in the form of a masterbatch. A masterbatch is a composition in which an additive or mixture of additives is dispersed in a sufficiently large amount in a polymer. Accordingly, the term "additive" according to the invention also includes carrier materials, in particular polymeric carrier materials in which the "active additive" or "mixture of active additives" is dispersed.

Automotive product

The invention also relates to an automobile product containing at least 90 wt. %, preferably at least 95 wt. %, compositions according to the invention. The invention particularly relates to a product for the interior decoration of a car containing at least 90 wt. %, preferably at least 95 wt. %, compositions according to the invention. Even more preferably, the invention relates to a product for the interior decoration of an automobile consisting of a composition according to the invention. Examples of such automotive interior trim products include dashboards, center consoles, door trims and pillar trims.

Particularly preferred embodiments The invention particularly relates to a composition having a melt flow index MFR ₂ (230° C., 2.16 kg), measured in accordance with ISO 1133, from 10.0 to 30.0 g/10 min and containing

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 2.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P);

(E) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T); And

(F) from 1.0 to 5.0 wt. %, based on the total amount of composition, additives (A); wherein the weight ratio between the heterophasic composition (HECO) and the polypropylene-polyethylene mixture (B) [(HECO)/(B)] is from 0.2 to 8.0, preferably from 0.3 to 6.0;

where also

- heterophase composition (HECO) contains

(a) propylene homopolymer as matrix, and

(b) ethylene-propylene rubber dispersed in said matrix,

in this case, heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 153 to 158°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined according to the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount from 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO); And

(v) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 1.5 to 6.5 mol. %, where ethylene is the only comonomer in the heterophasic composition (HECO);

- polypropylene-polyethylene mixture (B) contains:

B-1) at least 85.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polypropylene,

B-2) no more than 15.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polyethylene,

in this case, the polypropylene-polyethylene mixture (B) has:

i) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 5.0 to 75 g/10 min; And

ii) residual ash content, measured by thermogravimetric analysis, from 0.1 to 3.0 wt. %,

- the plastomer is a copolymer of ethylene and 1-octene or a copolymer of ethylene and 1-butene, having a density, measured according to ISO 1183-1, from 850 to 900 kg/m ³ .

The invention relates in particular to a composition having a melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 10.0 to 30.0 g/10 min and consisting of

(A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO);

(B) from 7.0 to 55.0 wt. %, based on the total amount of the composition, polypropylene-polyethylene mixture (B);

(C) from 2.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE);

(D) and from 5.0 to 15.0 wt. %, based on the total amount of the composition, is polyethylene, which is the sum of said high-density polyethylene (HDPE) and the polyethylene contained in said polypropylene-polyethylene mixture (B);

(E) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P);

(F) from 7.0 to 25.0 wt. %, based on the total amount of the composition, talc (T); And

(G) from 1.0 to 5.0 wt. %, based on the total amount of composition, additives (A); wherein the mass ratio between the heterophasic composition (HECO) and

polypropylene-polyethylene mixture (B) [(HECO)/(B)] is from 0.2 to 8.0, preferably from 0.3 to 6.0,

at the same time also

- heterophase composition (HECO) contains

(a) a propylene homopolymer as a matrix, in which the propylene homopolymer has 2,1-regiodefects, determined by ¹³ C-NMR, from 0.05 to 0.90%, and

(b) ethylene-propylene rubber dispersed in said matrix, wherein the heterophasic propylene copolymer (HECO) has

(i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 153 to 158°C;

(ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133 from 20.0 to 120 g/10 min;

(iii) crystalline fraction (CF), determined according to the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(iv) soluble fraction (SF), determined according to the CRYSTEX QC ISO 6427 Annex B method, present in an amount from 9.0 to 21.0 mass. %, based on the total weight of heterophasic propylene copolymer (HECO);

(v) intrinsic viscosity of the soluble fraction (IV(SF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 2.00 to 3.00 dl/g;

(vi) intrinsic viscosity of the crystalline fraction (IV(CF)) of the heterophasic composition (HECO), measured according to ISO 1628-1 (at 135°C in decalin), from 1.00 to 1.50 dl/g;

(vii) the ratio of the intrinsic viscosity of the soluble fraction (SF) to the intrinsic viscosity of the crystalline fraction (CF) [IV(SF)/IV(CF)] of the heterophasic composition (HECO) from 1.50 to 2.80;

(viii) ethylene content in the soluble fraction (C2(SF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 22.0 to 39.0 mol. %;

(ix) ethylene content in the crystalline fraction (C2(CF)), measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 0.0 to 0.7 mol. %, And

(x) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) in the CRYSTEX analysis, from 1.5 to 6.5 mol. %, with ethylene being the only comonomer in the heterophasic composition (HECO);

- polypropylene-polyethylene mixture (B) contains:

B-1) at least 85.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polypropylene,

B-2) no more than 15.0 mass. %, based on the total weight of the polypropylene-polyethylene mixture (B), polyethylene,

in this case, the polypropylene-polyethylene mixture (B) has:

i) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 5.0 to 75 g/10 min; And

ii) residual ash content, measured by thermogravimetric analysis, from 0.1 to 3.0 wt. %; and one or more of the following:

iii) limonene content determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 ppm to 100 ppm;

iv) fatty acid(s) content determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 to 100 ppm;

v) polyamide(s) content, determined by NMR, from 0 to 1.5 wt. %;

vi) polystyrene(s) content, determined by NMR, from 0.05 to 3.0 wt. %;

- plastomer is a copolymer of ethylene and 1-octene or a copolymer of ethylene and 1-butene, having a density, measured according to ISO 1183-1, from 850 to 900 kg/m ³ and a melt flow index PTR ₂ (190 ° C, 2.16 kg), measured according to ISO 1133, from 1.5 to 15.0 g/10 min;

- polyethylene (HDPE), having a density, measured according to ISO 1183-1, from 940 to 970 kg/m ³ and a melt flow index PTR ₂ (190 ° C, 2.16 kg), measured according to ISO 1133, from 1.0 up to 30.0 g/10 min;

- talc (T) has an average median particle size d ₅₀ , measured in accordance with ISO 13317-3, from 0.3 to 3.0 μm, and an upper particle size d ₉₅ , measured in accordance with ISO 13317-3, from 0 .5 to 10.0 µm.

The invention will be described below using examples.

Examples Melt Flow Index Melt flow index (MFR ₂ ) is determined according to ISO 1133 and is reported in g/10 minutes. The MFR ₂ of a heterophasic propylene copolymer is determined at a temperature of 230° C. and under a load of 2.16 kg, while the MFR ₂ of plastomer and HDPE is determined at a temperature of 190°C and a load of 2.16 kg.

Melting temperature T _pl and crystallization temperature T _cr

The melting point T _pl is determined by differential scanning calorimetry (DSC) in accordance with ISO 11357-3 using a TA-Instruments 2920 Dual-Cell with an RSC refrigeration unit and a data transfer station. A heating and cooling rate of 10°C/min is used in a heating/cooling/heating cycle between +23 and 210°C. The crystallization temperature ( _Tcr ) is determined in the cooling stage, while the melting temperature ( _Tmelt ) and enthalpy of fusion ( _Hmelt ) are determined in the second heating stage.

Crystex Analysis

Method of crystalline and soluble fractions

The crystalline fraction (CF) and soluble fraction (SF) of heterophasic propylene copolymers, the final comonomer content of heterophasic propylene copolymers, the comonomer content of the corresponding fractions, and the intrinsic viscosity of the corresponding fractions were analyzed using CRYSTEX QC, Polymer Char (Valencia, Spain) at based on ISO 6427 Appendix B: 1992 (E). A schematic representation of the CRYSTEX QC instrument is shown in Fig. 1a. Crystalline and amorphous fractions are separated by temperature cycling of dissolution in 1,2,4-trichlorobenzene (1,2,4-TCB) at 160°C, crystallization at 40°C and redissolution in 1,2,4-TCB at 160°C C, as shown in Fig. 1b.

Quantification of SF and CF and determination of ethylene content (C2) is carried out using an infrared detector (IR4), and an online 2-capillary viscometer is used to determine the intrinsic viscosity (iV). The IR4 detector is a multi-wavelength detector that measures IR absorption in two different ranges (CH ₃ stretching vibration (centered around 2960 cm ^-1 ) and CH _x stretching vibration (2700-3000 cm ^-1 ), which can be used for determining the concentration and content of ethylene in ethylene-propylene copolymers (EP copolymers). The IR4 detector is calibrated with a series of 8 ethylene-propylene copolymers with a known ethylene content from 2 wt.% to 69 wt.% (determined by ¹³ C-NMR). concentrations, from 2 to 13 mg/ml. To account for both features, concentration and ethylene content simultaneously for the various polymer concentrations expected in the Crystex assays, the following calibration equations were applied: Equation 1:

The constants a to e for Equation 1 and a to f for Equation 2 were determined using least squares regression analysis.

Equation 3:

CH ₃ /1000C is converted to ethylene content in mass. % using the following ratio:

wt. % (ethylene in EP copolymers) = 100 - CH ₃ /1000TC * 0.3

The amount of soluble fraction (SF) and crystalline fraction (CF) are correlated using the XS calibration with the Xylene Cold Soluble (XCS) fraction and the Xylene Cold bisoluble (XCI) fraction, respectively, determined according to the standard gravimetric method in accordance with IS016152. XS calibration is carried out by testing different EP copolymers with xylene cold solubles (XCS) contents ranging from 2 to 31 wt. %. The resulting XS calibration is linear (Equation 4):

wt. % XCS = 1.01* wt. %SF

The intrinsic viscosity (IV) of the original heterophasic propylene copolymer and its soluble fraction (SF) and crystalline fraction (CF) is determined using an on-line 2-capillary viscometer and correlated with the corresponding IV determined by the standard decalin method according to ISO 1628-3. Calibration is carried out with various EP copolymers with IV = 2 to 4 dl/g. The defined calibration curve between Vsp measured in CRYSTEX QC and normalized by concentration (c) and IV is linear (Equation 5):

with an angle of inclination a = 16.2. A sample of the heterophasic propylene copolymer to be analyzed is weighed in concentrations ranging from 10 mg/ml to 20 mg/ml. After automatically filling the vial with 1,2,4-TCB containing 250 mg/L 2,6-tert-butyl-4-methylphenol (BNT) as an antioxidant, the sample is dissolved at 160°C until complete dissolution is achieved, usually within 60 min, with constant stirring at 400 rpm. To avoid sample destruction, the polymer solution is protected under an N ₂ atmosphere during dissolution.

As shown in Fig. 1a and b, a certain volume of the sample solution is introduced into a column filled with an inert carrier, where the sample crystallizes and the soluble fraction is separated from the crystalline part. This process is repeated twice. During the first injection, the entire sample is measured at high temperature, determining IV[dl/g] and C2[wt. %] heterophasic propylene copolymer. During the second injection, the soluble fraction (SF) (at low temperature, 40°C) and the crystalline fraction (CF) (at high temperature, 160°C) are measured with a crystallization cycle (wt.% SF, wt.% C2 SF, IV SF).

Determination of C2 content for calibration standards based on ¹³ C NMR spectroscopy

Quantitative NMR spectra of ^13C { ^1H } were recorded in the dissolved state using a Bruker Avance III 400 NMR spectrometer operating at frequencies of 400.15 and 100.62 MHz for ^1H and ^13C , respectively. All spectra were recorded using a ¹³ C optimized 10 mm probe at 125 °C using nitrogen gas for the entire pneumatic system. Approximately 200 mg of material was dissolved in 3 ml of 1,2-tetrachloroethane-d ₂ (TCE-d ₂ ) along with chromium(III) acetylacetonate (Cr(acac) ₃ ), resulting in a 65 mM solution of the relaxant in solvent (Singh , G., Kothari, A., Gupta, V., Polymer Testing 28 5 (2009), 475). To ensure a homogeneous solution, after initial sample preparation in the heat block, the NMR ampoule was further heated in a rotary oven for at least 1 hour. After insertion into the magnet, the ampoule was rotated at a frequency of 10 Hz. This setup was chosen primarily for high resolution and is quantitatively required for accurate ethylene quantification. Standard single-pulse excitation was used without NOE, using optimized tip angle, 1 s recirculation delay, and WALTZ 16 two-level 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., Cipullo, R., Pellecchia, R., Severn, J., Talarico, G., Macromol. Rapid Commun. 2007, 28, 1128). A total of 6144 (6k) transitions were obtained in the spectrum. Quantitative ^13C { ^1H } NMR spectra were processed, integrated, and corresponding quantitative properties determined from integrals. All chemical shifts are internally assigned to the central methylene group of the ethylene block (EEE) at 30.00 ppm. using solvent chemical shift. This approach allowed for comparable assignments even when this structural link was missing. Characteristic signals corresponding to the incorporation of ethylene were observed (Cheng, HN, Macromolecules 17 (1984), 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 Wang et al. (Wang, W. J., Zhu, S., Macromolecules 33 (2000), 1157) by integrating multiple signals across the entire spectral region in the ¹³ C{ ¹ H} spectra. This method was chosen due to its robust nature and ability to take into account the presence of regional defects when necessary. The integration ranges have been slightly adjusted to improve applicability over the entire range of comonomer contents encountered. For systems with very low ethylene content, where only isolated ethylene was observed in the PPEPP sequences, the method of Wang et. al. has been modified to reduce the influence of non-zero patch integrals, which are known to be missing. This approach reduced the overestimation of ethylene content in such systems and was achieved by reducing the number of sites used to determine absolute ethylene content to

By using this set of plots, the corresponding integral equation becomes:

using the same notation used in the paper by Wang et al. (Wang, W-J., Zhu, S., Macromolecules 33 (2000), 1157). The equations used to determine the absolute propylene content have not been modified. The molar percentage of incorporated comonomer was calculated from the molar fraction:

The mass percentage of incorporated comonomer was calculated from the mole fraction:

Microstructure quantification using NMR spectroscopy

Quantitative nuclear magnetic resonance (NMR) spectroscopy was used to quantify the isotacticity and regioregularity of the heterophasic copolymer (HECO) matrix component on samples taken after the first gas-phase reactor (GPR1).

Quantitative NMR spectra of ^13C { ^1H } were recorded in the solution state using a Bruker Advance III 400 NMR spectrometer operating at frequencies of 400.15 and 100.62 MHz for ^1H and ^13C , respectively. All spectra were recorded using a ¹³ C optimized 10 mm extended temperature probe at 125° C using nitrogen gas for the entire pneumatic system.

For propylene homopolymers, approximately 200 mg of material was dissolved in 1,2-tetrachloroethane-d2 (TCE-d2). To ensure a homogeneous solution, after initial sample preparation in the heat block, the NMR ampoule was further heated in a rotary oven for at least 1 hour. After insertion into the magnet, the ampoule was rotated at a frequency of 10 Hz. This setup was chosen primarily for the high resolution needed to quantify the tacticity distribution (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). Standard single-pulse excitation was used using NOE and a WALTZ 16 two-level 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., Severn, J., Talarico, G., Macromol. 2007, 28, 11289). A total of 8192 (8k) transitions were obtained in the spectrum.

Quantitative ¹³ C{1H} NMR spectra were processed, integrated, and the corresponding quantitative properties were determined from integrals using proprietary computer programs.

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

Characteristic signals corresponding to regiodefects were 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) or comonomer.

The tacticity distribution was quantified by integrating the region of methyl groups between 23.6-19.7 ppm. with correction for any regions not associated with the stereo sequences 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 influence of regiodefects and comonomer on the quantification of tacticity distribution is corrected by subtracting representative integrals related to regiodefects and comonomers from specific integration regions related to stereo sequences.

Isotacticity was determined at the pentad level and reported as the percentage of isotactic pentad sequences (mmmm) relative to all pentad sequences:

The presence of 2,1-erythro-regiodefects was shown by the presence of two methyl sites at 17.7 and 17.2 ppm. and 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).

The amount of 2,1-erythro-regiodefects was quantified using the average integral of two characteristic methyl sites at 17.7 and 17.2 ppm:

The amount of 1,2 primary intruded propene was quantified based on the methyl region with corrections made for sites included in this region not associated with primary intrusion and for primary intrusive sites excluded from this region:

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

The mole percentage of 2,1-erythro-regiodefects was quantified for all propenes:

Intrinsic viscosity

Intrinsic viscosity (iV) is measured in accordance with DIN ISO 1628/1, October 1999, in decalin at 135°C.

Density

Density is measured in accordance with ISO 1183-1. Sample preparation is carried out by direct compression in accordance with ISO 1872-2:2007.

Particle size distribution

The average median particle size d ₅₀ and the top particle size d ₉₅ are measured by gravitational liquid sedimentation in accordance with ISO 13317-3.

Flexural modulus

The flexural modulus was determined at 3-point bending at 23°C in accordance with ISO 178 on 80×10×4 mm ³ injection molded test rods in accordance with EN ISO 1873-2.

Impact Strength of Notched Specimens (NIS)

The Charpy impact strength of notched specimens (NIS) was measured in accordance with ISO 179 1 eA at -20°C and +23°C using injection molded 80 x 10 x 4 mm ³ test rod specimens prepared in accordance with ISO 294-1: 1996.

VOC values, LMS values

Preparation of samples

VOC values and LMC values were measured as described below after preparing injection molded plate samples in accordance with EN ISO 19069-2:2016. These records were packaged in aluminum composite foil immediately after production and the foil was sealed.

For thermal desorption analysis in accordance with VDA 278 (October 2011), samples were stored at room temperature (23°C max) for 7 days immediately before analysis.

The production date of the injection molded records, the time the sample arrived at the laboratory, and the date of analysis were recorded.

VOC and LMS in accordance with VDA278

The VOC value is determined in accordance with VDA 278, October 2011, on injection molded plates. VDA 278 October 2011, Thermal Desorption Analysis of Organic Emissions for the Characterization of Non-Metallic Materials for Automobiles (, VDA Verband der Automobilindustrie. According to VDA 278, October 2011, the VOC value is defined as “the total amount of highly volatile and moderately volatile substances. Calculated as toluene equivalent. The method described in this Recommendation allows the determination and analysis of substances in the boiling range/eluting range to n-pentacosane (C25).

The LMS value is determined in accordance with VDA 278, October 2011, on injection molded plates. According to VDA 278, October 2011, the LMS value is defined as “the total amount of low volatility substances that elute from the retention time of n-tetradecane (inclusive).” It is calculated as hexadecane equivalent. Substances in the boiling range from n-alkanes “C 14” to “C32” are determined and analyzed.

Special methods for regenerated products

Amount of iPP, polystyrene, polyethylene (and ethylene-containing copolymers), poly(ethylene terephthalate) and amount of polyamide-6

To establish different calibration curves, different standards were mixed, iPP and HDPE as well as iPP, PS and PA6. To quantify the content of foreign polymers, IR spectra were recorded in the solid state using a Bruker Vertex 70 FTIR spectrometer. Films were prepared using a molding device at 190°C with a pressing force of 4-6 MPa. The film thicknesses for the calibration standards for iPP and HDPE were 300 µm, while film thicknesses of 50–100 µm were used for the quantification of iPP, PS and PA6. Standard FT-IR transmittance spectroscopy is used using a spectral range of 4000-400 cm ^-1 , 6 mm aperture, spectral resolution 2 cm ^-1 , 16 background scans, 16 spectral scans, zero interferogram fill factor of 32, and strong Norton Beer apodization .

Measure the absorbance of the band at 1167 cm ^-1 in iPP and quantify the iPP content according to the calibration curve (absorbance/thickness in cm vs iPP content in wt%).

Measure the absorbance of the band at 1601 cm ^-1 (PS) and 3300 cm (PA6) and quantify the PS and PA6 content according to the calibration curve (absorbance/thickness in cm versus PS and PA content in wt%). The content of polyethylene and ethylene-containing copolymers is obtained by subtracting (iPP + PS + PA6) from 100, taking into account the content of non-polymer impurities, determined by the methods given below. The analysis is carried out in the form of a double determination.

Number of metals

Determined by X-ray fluorescence (XRF)

Amount of paper, wood

The amount of paper and wood was determined by conventional laboratory methods including milling, flotation, microscopy and thermogravimetric analysis (TGA).

Amount of talc and chalk

TGA was performed according to the following procedure:

Thermogravimetric analysis (TGA) experiments were performed using a Perkin Elmer TGA 8000 instrument. Approximately 10-20 mg of material was placed in a platinum crucible. The temperature was set at 50°C for 10 minutes and then raised to 950°C under nitrogen at a heating rate of 20°C/min. The loss of mass between about 550°C and 700°C (WCO ₂ ) was attributed to CO ₂ released from CaCO ₃ , and accordingly the chalk content was estimated as:

Chalk content = 100/44 × WCO ₂

After this, the temperature was lowered to 300°C at a cooling rate of 20°C/min. The gas was then switched to oxygen and the temperature was raised again to 900°C. The mass loss at this stage was attributed to carbon black (Web). Knowing the content of carbon black and chalk, the ash content excluding chalk and carbon black was calculated as:

Ash content = (Ash residue) - 56/44 × WCO ₂ - Web

where the bottom ash is % by weight measured at 900°C in the first stage carried out under a nitrogen atmosphere. The ash content is estimated to be the same as the talc content for the reclaims studied.

Ash content

Ash content is measured using thermogravimetric analysis (TGA) in accordance with ISO 11358-1 (20147).

Measurement of limonene content

Limonene content was quantified using solid phase microextraction (HS-SPME-GC-MS) by standard addition.

50 mg of ground samples were weighed into 20 mL vials and after adding limonene at different concentrations and a glass coated magnetic stirrer. The vial was closed with a magnetic cap lined with silicone/PTFE. Microcapillaries (10 pl) were used to add diluted limonene standards of known concentrations to the sample. Addition of 0, 2, 20 and 100 ng equals 0 mg/kg, 0.1 mg/kg, 1 mg/kg and 5 mg/kg limonene, and in addition standard amounts of 6.6 mg/kg, 11 mg/kg were used. kg and 16.5 mg/kg limonene in combination with some of the samples tested in this application. Ion 93 obtained in SIM mode was used for quantitative assessment. Enrichment of the volatile fraction was carried out by solid-phase microextraction with 2 cm of stably flexible 50/30 pm DVB/Carboxen/PDMS fiber at 60°C for 20 minutes. Desorption was carried out directly in the heated injection port of the GCMS system at 270°C.

GCMS parameters:

Column: 30 m HP 5 MS 0.25*0.25

Injector: Without flow splitting, lined with SPME 0.75 mm, 270°C

Temperature program: -10°C (1 min)

Carrier gas: helium 5.0, linear velocity 31 cm/s, constant flow

MS: Single quadrupole, direct interface, interface temperature 280°C

Receive: SIM scan mode

Scan parameter: 20-300 amu

SIM parameter: m/Z 93, waiting time 100 ms

Total free fatty acids Fatty acids were quantified using headspace solid phase microextraction (HS-SPME-GC-MS) by standard addition.

50 mg of crushed samples were weighed into a 20 mL vial and after adding limonene at various concentrations and a glass coated magnetic stirrer, the vial was sealed with a silicone/PTFE lined magnetic cap. 10 μL microcapillaries were used to add a dilute mixture of free fatty acid (acetic acid, propionic acid, butyric acid, pentanoic acid, hexanoic acid, and octanoic acid) standards of known concentrations to the sample at three different levels. Addition of 0, 50, 100 and 500 ng equals 0 mg/kg, 1 mg/kg, 2 mg/kg and 10 mg/kg of each individual acid. For quantification, ion 60 obtained in SIM mode was used; for all acids except propanoic acid, ion 74 was used here.

GCMS Parameter:

Column: 20m ZB Wax plus 0.25*0.25

Injector: 5:1 split glass lined, 250°C

Temperature program: from 40°C (1 min) at 6°C/min to 120°C, at 15°C to 245°C (5 min)

Carrier: helium 5.0, linear speed 40 cm/s, constant flow

MS: Single quadrupole, direct interface, interface temperature 220°C

Receive: SIM scan mode

Scan parameter: 46-250 amu 6.6 scans/s

SIM parameter: m/Z 60.74, 6.6 scans/s

1. Preparation of heterophasic propylene copolymer (HECO)

a) Preparation of a single-site catalyst system Catalytic complex The following metallocene complex was used as described in WO 2019/179959:

Preparation of MAO-silica carrier

A steel reactor equipped with a mechanical stirrer and a filter mesh was flushed with nitrogen, and the reactor temperature was set at 20°C. DM-L-303 silica from AGC Si-Tech Co, pre-calcined at 600°C (5.0 kg), was then added from the feed drum, followed by careful increase and decrease in nitrogen pressure using manual valves. Toluene (22 kg) was then added. The mixture was stirred for 15 minutes. Next 30 wt. A % solution of MAO in toluene (9.0 kg) from Lanxess was added through the feed line to the top of the reactor over 70 min. The reaction mixture was then heated to 90°C and stirred at 90°C for an additional two hours. The suspension was allowed to settle and the mother liquor was filtered. The catalyst was washed twice with toluene (22 kg) at 90°C, followed by precipitation and filtration. The reactor was cooled to 60°C and the solid was washed with heptane (22.2 kg). Finally, the MAO-treated SiO ₂ was dried at 60° under nitrogen flow for 2 hours and then for 5 hours in vacuum (-0.5 barg (-0.05 MPa g)) with stirring. The MAO-treated support was collected as a free-flowing white powder containing 12.2% Al by weight.

Preparation of a single-site catalytic system In a steel reactor under a nitrogen atmosphere, 30 wt. was added through a burette. % MAO in toluene (0.7 kg) at 20°C. Toluene (5.4 kg) was then added with stirring. The metallocene complex as described in section 2a) above (93 g) was added from a metal can followed by rinsing with 1 kg of toluene. The mixture was stirred for 60 minutes at 20°C. Trityltetrakis(pentafluorophenyl)borate (91 g) was then added from a metal can, followed by rinsing with 1 kg of toluene. The mixture was stirred for 1 hour at room temperature. The resulting solution was added to the stirred precipitate of MAO-silica support prepared as described above for 1 hour. The precipitate was left to stand for 12 hours, then dried in a stream of N2 at 60°C for 2 hours and an additional 5 hours in vacuum (-0.5 barog (-0.05 MPa excess)) with stirring.

The dried catalyst was collected as a pink free-flowing powder containing 13.9% Al and 0.11% Zr.

"HECO2" is a commercial heterophasic propylene copolymer "BJ400HP" from Borealis AG, Austria (see Table 2 for properties);

"HECO3" is a commercial heterophasic propylene copolymer of propylene "BE170CF" from Borealis AG, Austria (for properties see Table 2);

“Blend (B)” is an experimental reclaimed polypropylene-polyethylene blend of sorting, washing and compounding steps based on separately collected post-consumer plastic waste. It has a PP content of 91.2 wt. %, total ethylene content determined by FTIR, 7.0 wt. %, ash content 1.7 wt. % and limonene content greater than 0.1 ppm (see Table 3 for further properties).

“Plastomer” is a commercial copolymer of ethylene and 1-octene “Engage 8200” from Dow Chemical Company, USA, having a density of 870 kg/m ³ and a melt flow index PTR ₂ (190 ° C, 2.16 kg) 5.0 g /10 min;

“HDPE” is a commercial high-density polyethylene “HE9621-RN” from Borealis AG, Austria, having a density of 964 kg/m ³ and a melt flow rate PTR ₂ (190 ° C, 2.16 kg) 12.0 g/10 min ;

The talc is commercial talc "Jetfine 3 CA" from Imerys, UK, having an average median particle size d ₅₀ of 1.2 μm and a top particle size d ₉₅ of 3.3 μm;

“Additives” are a mixture of the following components:

- 15.5 mass. %, based on the total weight of the "additives", of commercial solid epoxy resin "NPES 902" medium molecular weight from Nan Ya Plastics Corp. (Republic of China),

- 8.9 mass. %, based on the total weight of the “additives,” of commercial erucamide “Finawax-E” from Fine Organics (United Kingdom);

- 7.8 mass. %, based on the total weight of “additives”, commercial nucleating agent “NA-21” from Adeka (France), a mixture of aluminum-hydroxy-bis[2,2'-methylene-bis(4,6-di-tert-butylphenyl )phosphate] and lithium myristate,

- 7.8 mass. %, based on the total mass of “additives”, light stabilizer Cyasorb UV-3808РР5 from Solvay - masterbatch with 25 wt. % n-hexadecyl-3,5-di-tert-butyl-4-hydroxybenzoate and 25 wt. % esters of 2,2,6,6-tetramethyl-4-piperidinol and higher fatty acids (mainly stearic acid), the latter commercially available as Cyasorb UV-3853 from Solvay, in PP homopolymer,

- 5.8 mass. %, based on the total weight of “additives”, commercial sterically hindered phenol - octadecyl-3-(3,5-di-tert-butyl-4-hydroxyphenyl) propionate “Songnox 1076” from Songwon (Republic of Korea),

- 3.9 mass. %, based on the total mass of “additives,” a commercial antioxidant based on phosphorus - tris(2,4-di-tert-butylphenyl)phosphite “Irgafos 168” from BASF SE (Germany),

- 50.3 mass. %, based on the total mass of “additives”, carbon black superconcentrate Plasblak 10 PPP6331 from Cabot Corporation (Germany).

As can be seen from the data in Table 3, HECO according to the invention can be replaced in various quantities by a regenerated polypropylene-polyethylene mixture without noticeable deterioration in the mechanical and odor properties of the final compositions (compare IE1 - IE3 with CE1). Stiffness remains nearly constant despite the addition of a lower stiffness component (see CE3 stiffness for reclaimed stiffness), while impact and odor properties are significantly better than would be expected from simple estimates based on reclaimed material properties. This allows reclaimed materials to be repurposed to replace potentially costly virgin HECO in automotive applications, while also helping to minimize plastic waste through recycling.

Claims (53)

1. Composition for automobile products obtained by mixing (A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO); (B) from 7.0 to 55.0 wt. %, based on the total amount of composition, regenerated polypropylene-polyethylene mixture (B); (C) from 0.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE); (D) from 2.0 to 12.0 wt. %, based on the total amount of composition, plastomer (P), and (E) from 7.0 to 25.0 wt. %, based on the total amount of composition, talc (T), where the specified composition contains a total amount of from 5.0 to 15.0 wt. % polyethylene, which is the sum of said high-density polyethylene (HDPE) and the polyethylene contained in said regenerated polypropylene-polyethylene mixture (B); wherein the heterophasic composition (HECO), polypropylene-polyethylene mixture (B), high-density polyethylene (HDPE), plastomer (P) and talc (T) together constitute at least 90 wt.% of the total amount of the composition; where also - heterophase composition (HECO) contains (a) a propylene homopolymer as a matrix, and (b) ethylene-propylene rubber dispersed in said matrix, in this case, heterophasic propylene copolymer (HECO) has (i) melting point Tm measured by DSC in accordance with ISO 11357-3 (heating and cooling rate 10°C/min), from 150 to 159°C; (ii) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 20.0 to 120 g/10 min; (iii) crystalline fraction (CF), determined in accordance with the CRYSTEX QC method ISO 6427 Annex B, present in an amount from 79.0 to 91.0 mass. %, based on the total mass of heterophasic propylene copolymer (HECO); (iv) soluble fraction (SF), determined in accordance with the CRYSTEX QC ISO 6427 Annex B method, present in an amount of 9.0 to 21.0 mass. %, based on the total mass of heterophasic propylene copolymer (HECO); And (v) total ethylene content, measured by Fourier transform infrared spectroscopy (FTIR) during the CRYSTEX analysis, from 1.5 to 6.5 mol. %, while ethylene is the only comonomer in the heterophasic composition (HECO); - regenerated polypropylene-polyethylene mixture (B) contains: B-1) at least 85.0 mass. %, based on the total weight of the regenerated polypropylene-polyethylene mixture (B), polypropylene, B-2) no more than 15.0 mass. %, based on the total weight of the regenerated polypropylene-polyethylene mixture (B), polyethylene, in this case, the regenerated polypropylene-polyethylene mixture (B) has: i) melt flow index PTR ₂ (230°C, 2.16 kg), measured in accordance with ISO 1133, from 5.0 to 75 g/10 min; And ii) residual ash content, measured by thermogravimetric analysis according to ISO 11358-1, from 0.1 to 3.0 mass. %; and one or more of the following properties: iii) limonene content determined by solid phase microextraction (HS-SPME-GC-MS) from 0.1 ppm to 100 ppm; iv) fatty acid or acids content determined by solid phase microextraction (HS-SPME-GC-MS), from 0.1 to 100 ppm; v) content of polyamide or polyamides, determined by NMR, up to 1.5 wt. % and above the detection limit; vi) content of polystyrene or polystyrenes, determined by NMR, from 0.05 to 3.0 mass. %; - wherein the plastomer is a copolymer of ethylene and 1-octene or a copolymer of ethylene and 1-butene having a density, measured in accordance with ISO 1183-1, from 850 to 900 kg/m ³ . 2. The composition according to claim 1, in which the heterophasic propylene copolymer (HECO) has a content of 2,1-regiodefects, determined by ¹³ C-NMR, from 0.05 to 0.90%, and/or a melting point Tm, measured by DSC according to ISO 11357-3 (heating and cooling rate 10°C/min), from 153 to 158°C. 3. The composition according to claim 1 or 2, in which the ethylene content in the soluble fraction (C2(SF)) of the heterophasic composition (HECO), measured by infrared spectroscopy in the CRYSTEX analysis, ranges from 22.0 to 39.0 mol. %. 4. The composition according to claim 1 or 2, in which the ethylene content of the crystalline fraction (C2(CF)) of the heterophasic composition (HECO), measured by infrared spectroscopy in the CRYSTEX analysis, ranges from 0.0 to 0.7 mol. %. 5. The composition according to claim 1 or 2, in which the heterophasic composition (HECO) has (i) intrinsic viscosity of the soluble fraction (IV(SF)) from 1.80 to 3.20 dl/g; (ii) an intrinsic viscosity of the crystalline fraction (IV(CF)) from 0.80 to 1.80 dl/g and (iii) the ratio between the intrinsic viscosity of the soluble fraction (SF) and the intrinsic viscosity of the crystalline fraction (CF) [IV(SF)/IV(CF)] from 1.50 to 2.80. 6. Composition according to claim 1 or 2, in which the regenerated polypropylene-polyethylene mixture (B) occurs in an amount of at least 90 wt. % from post-consumer waste. 7. Composition according to claim 1 or 2, in which the mass ratio between the heterophasic composition (HECO) and the regenerated polypropylene-polyethylene mixture (B) [(HECO)/(B)] is from 0.2 to 8.0, preferably from 0.3 to 6.0. 8. The composition according to claim 1 or 2, wherein the plastomer is a copolymer of ethylene and 1-octene having a melt flow index MFR ₂ (190°C, 2.16 kg), measured according to ISO 1133, from 2.0 to 10 .0 g/10 min and having a density, measured according to ISO 1183-1, from 860 to 890 kg/m ³ . 9. The composition according to claim 1 or 2, in which the high-density polyethylene (HDPE) has a density, measured according to ISO 1183-1, from 940 to 970 kg/m ³ and a melt flow index MFR ₂ (190 ° C, 2.16 kg), measured according to ISO 1133, from 2.0 to 20.0 g/10 min. 10. The composition according to claim 1 or 2, where the composition contains from 2 to 12 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE). 11. Composition according to claim 1 or 2, consisting of (A) from 18.0 to 60.0 wt. %, based on the total amount of the composition, heterophasic composition (HECO); (B) from 7.0 to 55.0 wt. %, based on the total amount of composition, regenerated polypropylene-polyethylene mixture (B); (C) from 2.0 to 12.0 wt. %, based on the total amount of the composition, high-density polyethylene (HDPE); (D) from 2.0 to 12.0 wt. %, based on the total amount of the composition, plastomer (P); (E) from 7.0 to 25.0 wt. %, based on the total amount of composition, talc (T) and additionally (F) from 1.0 to 10.0 wt. %, based on the total amount of composition, additives (A). 12. The composition according to claim 1 or 2, wherein the talc (T) has an average median particle size d ₅₀ measured according to ISO 13317-3, from 0.5 to 2.0 μm, and an upper maximum particle size d ₉₅ measured according to ISO 13317-3, from 1.0 to 8.0 µm. 13. Composition according to claim 1 or 2, having a melt flow index PTR ₂ (230°C, 2.16 kg), measured according to ISO 1133, from 10.0 to 30.0 g/10 min. 14. A composition according to claim 1 or 2, having a volatile organic compound (VOC) content, measured on material obtained directly from extrusion in accordance with the procedure described in VDA278, of less than 100 μg per gram of composition. 15. An automobile product made from the composition according to any of the preceding paragraphs.