Polypropylene compositions for interior automotive applications

By optimizing the ratio of heterophasic propylene copolymer and inorganic filler in the polypropylene-based composition, the problem of insufficient mechanical and impact properties of recycled polyolefin materials in automotive interior applications was solved, and excellent mechanical properties and thermal stability were achieved, making it suitable for injection molding.

CN117460774BActive Publication Date: 2025-09-12BOREALIS AG
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Patent Information

Application Number
CN202280040676.6
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Priority Date
2021-06-09
Filing Date
2022-06-07
Publication Date
2025-09-12
Estimated Expiration
2042-06-07

AI Technical Summary

Technical Problem

Existing recycled polyolefin materials in the automotive industry have deficiencies in mechanical properties, impact performance and odor emissions, making it difficult to meet the requirements of interior applications, especially due to cross-contamination of polymers in the recycled stream and limited mechanical properties.

Method used

By precisely selecting the ratio of heterophasic propylene copolymer and inorganic filler in the polypropylene-based composition, a composition comprising 15-50% mixed plastic polypropylene blend, 10-60% heterophasic propylene copolymer and 5-25% inorganic filler is formed, optimizing the intrinsic viscosity of the crystalline fraction and the soluble fraction, and improving the mechanical and impact properties.

Benefits of technology

It achieves an excellent balance of mechanical properties, thermal stability and impact performance for automotive interior applications and is suitable for injection molding to replace complex heterophasic polypropylene copolymers.

✦ Generated by Eureka AI based on patent content.

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Abstract

A composition suitable for automotive applications obtainable by blending at least components (A), (B) and (C): (A) 15 to 50 wt%, preferably 17 to 47 wt%, more preferably 18 to 45 wt% of a mixed plastic polypropylene blend; (B) 10 to 60 wt%, preferably 15 to 55 wt%, more preferably 17 to 52 wt% of a first heterophasic propylene copolymer; and (C) 5 to 25 wt%, preferably 7 to 22 wt%, more preferably 8 to 20 wt% of an inorganic filler.
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Description

Technical Field

[0001] The present invention relates to a polypropylene composition particularly suitable for automotive interior applications, the polypropylene composition comprising a mixed plastic polypropylene-based blend and an inorganic filler. Background Art

[0002] Compositions suitable for use in the automotive industry typically comprise one or more heterophasic polypropylene copolymers and / or random heterophasic copolymers, and conventionally some inorganic fillers.

[0003] A fundamental problem in the polymer industry is recycling. Currently, the market for recyclates, especially those from household waste, often referred to as PCR ("post-consumer resin"), is somewhat limited. Starting from household waste, the sorting and separation processes employed will not produce pure polymers, i.e. there will always be some contaminants, or these processes may even result in a blend of different polymers. When it comes to polyolefins, which constitute the vast majority of the polymer fraction of collected household waste, it is almost impossible to perfectly separate polypropylene and polyethylene. Recycled polyolefin materials, especially post-consumer resins, are often cross-contaminated with non-polyolefin materials, such as polyethylene terephthalate, polyamide, polystyrene or non-polymeric substances such as wood, paper, glass or aluminum. To make matters worse, these post-consumer recycled polyolefin materials are easily available on a multi-ton scale, but unfortunately, these post-consumer recycled polyolefin materials have limited mechanical properties and often suffer from severe odor and / or emission problems.

[0004] A major requirement of the automotive industry for interior applications is that the material exhibit good flow properties, high mechanical and stiffness-impact properties, and exhibit excellent surface appearance. Recently, market demand has expanded towards the use of recycled polyolefins in blends with virgin polymers to meet these specific requirements.

[0005] Unpublished patent application EP 20 190 814.2 relates to polypropylene compositions for automotive applications comprising mixed plastic polypropylene-based blends derived from post-consumer recycled polyolefin streams and inorganic fillers such as talc. These compositions exhibit beneficial VOC and tiger stripe properties (MSE) and can therefore replace complex heterophasic polypropylene copolymers in automotive applications. However, these compositions still exhibit deficiencies in impact properties.

[0006] The present invention is based on the surprising finding that by careful selection of the original components based on heterophasic propylene copolymers in a polypropylene based composition comprising a mixed plastic polypropylene based blend derived from post-consumer recycled polyolefin streams and an inorganic filler such as talc, the polypropylene based composition has an excellent balance of mechanical properties, thermal stability and especially impact properties such as in instrumented puncture tests. Thus, the inventive composition comprising a mixed plastic polypropylene based blend derived from post-consumer recycled polyolefin streams is suitable for injection molding applications, especially in the automotive sector, such as interior automotive applications, and can replace complex heterophasic polypropylene copolymers. Summary of the Invention

[0007] The present invention relates to a composition suitable for automotive applications, which composition can be obtained by blending at least components (A), (B) and (C)

[0008] (A) 15 to 50 wt. %, preferably 17 to 47 wt. %, more preferably 18 to 45 wt. % of a mixed plastic polypropylene blend;

[0009] (B) 10 to 60 wt.-%, preferably 15 to 55 wt.-%, more preferably 17 to 52 wt.-% of a heterophasic propylene copolymer; and

[0010] (C) 5 to 25 wt %, preferably 7 to 22 wt %, more preferably 8 to 20 wt % of an inorganic filler;

[0011] wherein all percentages refer to the total composition, and wherein

[0012] Mixed plastic polypropylene blend (A) has

[0013] - a crystalline fraction (CF) content determined according to CRYSTEXQC analysis in the range of 85.0 to 96.0 wt.-%, preferably in the range of 86.5 to 95.5 wt.-%, and

[0014] - a soluble fraction (SF) content determined according to CRYSTEXQC analysis in the range of 4.0 to 15.0 wt.-%, preferably in the range of 4.5 to 13.5 wt.-%, wherein

[0015] - the crystalline fraction (CF) has a content in the range of 1.0 to 10.0 wt. %, preferably in the range of 1.5 to 9.5 wt. % by quantitative 13 Ethylene content (C2(CF)) determined by FT-IR spectroscopy calibrated with C-NMR spectroscopy; and

[0016] - the soluble fraction (SF) has an intrinsic viscosity (iV(SF)) determined in decalin at 135° C. according to DIN ISO 1628 / 1 in the range of 0.9 to 2.1 dl / g, preferably in the range of 1.0 to 2.0 dl / g, more preferably in the range of 1.1 to 1.9 dl / g;

[0017] The heterophasic propylene copolymer (B) comprises a matrix phase and an elastomeric phase dispersed therein and has

[0018] - a melt flow rate MFR2 (230°C, 2.16 kg, ISO 1133) of 85 to 250 g / 10 min, preferably 90 to 150 g / 10 min, more preferably 95 to 125 g / 10 min;

[0019] - a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of greater than 20.0% to 30.0% by weight, and

[0020] - an intrinsic viscosity (iV(SF)) of the soluble fraction measured in decalin at 135° C. according to DIN ISO 1628 / 1 of 2.0 to 4.5 dl / g, preferably 2.4 to 3.8 dl / g, more preferably 2.5 to 3.7 dl / g;

[0021] The composition has

[0022] - a melt flow rate MFR2 (230°C, 2.16 kg, ISO 1133) of 20 to 60 g / 10 min, preferably 21 to 50 g / 10 min, more preferably 22 to 45 g / 10 min.

[0023] Furthermore, the present invention relates to an article, preferably a molded article, more preferably a molded automotive article, comprising the composition as described above or below.

[0024] Furthermore, the present invention relates to the use of a composition as described above or below for the injection molding of an article, preferably an automotive article, more preferably an automotive interior article.

[0025] definition

[0026] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which the invention belongs. Although any methods and materials similar or equivalent to those described herein can be used in practice to test the present invention, preferred materials and methods are described herein. In describing and claiming the present invention, the following terminology will be used in accordance with the definitions set out below. Unless expressly indicated otherwise, the use of the terms "a," "an," etc., refers to one or more.

[0027] Mixed plastics are defined as the presence of small amounts of compounds not normally found in virgin polypropylene blends, such as polystyrene, polyamide, polyester, wood, paper, limonene, aldehydes, ketones, fatty acids, metals and / or long-term degradation products of stabilizers. Virgin polypropylene blends are blends derived directly from the production process without intermediate uses.

[0028] By definition, "mixed plastics" may be equated to detectable amounts of polystyrene and / or polyamide-6 and / or limonene and / or fatty acids.

[0029] Mixed plastics can therefore be derived from post-consumer and industrial waste rather than virgin polymers. Post-consumer waste refers to items that have completed at least their first use cycle (or life cycle), meaning they have been used for their first purpose. In contrast, industrial waste refers to manufacturing or conversion waste that does not typically reach consumers.

[0030] Those skilled in the art will appreciate that a soluble fraction (SF) obtained by CRYSTEX QC analysis having an intrinsic viscosity (iV(SF)) in the range of 0.9 to less than 2.2 dl / g is typically found in material from recycle streams. In a preferred aspect of the invention, the soluble fraction (SF) obtained by CRYSTEX QC analysis has an intrinsic viscosity (iV(SF)) in the range of 0.9 to 2.1 dl / g.

[0031] Polymer blend is a mixture of two or more polymer components. Generally, blend can be prepared by mixing two or more polymer components. Suitable mixing procedures known in the art are post-polymerization blending. Post-polymerization blending can be a dry blending of polymer components (such as polymer powder and / or compounded polymer pellets), or a melt blending of the polymer components by melt mixing.

[0032] "Polypropylene-polyethylene blend" refers to a composition containing both polypropylene and polyethylene, and also includes polypropylene copolymers and polyethylene copolymers. Since direct determination of the polypropylene and polyethylene contents is not possible, the weight ratio of polypropylene (A-1) to polyethylene (A-2) of 19:1 to 7:3 represents an equivalent ratio determined by calibration with iPP and HDPE and measured by IR spectroscopy.

[0033] Polypropylene refers to a polymer consisting of units derived from propylene in an amount of more than 50 mol%.

[0034] Polyethylene refers to a polymer consisting of units derived from ethylene in an amount greater than 50 mol%.

[0035] The term "elastomer" refers to a natural or synthetic polymer that possesses elastic properties. The term "plastomer" refers to a natural or synthetic polymer that combines the characteristics of elastomers and plastics, such as rubber-like properties and the processing capabilities of plastics. Ethylene-based plastomers are plastomers composed of units derived from ethylene in an amount greater than 50 mol%.

[0036] The presence of multiphase properties can be readily determined by the number of glass transition points, such as in dynamic mechanical analysis (DMA) and / or high-resolution microscopy, such as scanning electron microscopy (SEM), transmission electron microscopy (TEM) or atomic force microscopy (AFM).

[0037] The term "XCS" refers to the xylene cold soluble fraction (XCS weight %) measured at 25°C according to ISO 16152. The term "XCI" refers to the xylene cold insoluble fraction (XCI weight %) measured at 25°C according to ISO 16152.

[0038] Reactor blends are blends produced in two or more reactors coupled in series or in a reactor with two or more reaction chambers. Alternatively, reactor blends can be produced by blending in solution. Reactor blends are contrasted with compounds produced by melt extrusion.

[0039] If not stated otherwise, "%" refers to weight % (wt.-%). DETAILED DESCRIPTION

[0040] Composition

[0041] In a first aspect, the present invention relates to a composition suitable for automotive applications, obtainable by blending at least components (A), (B) and (C)

[0042] (A) 15 to 50 wt. %, preferably 17 to 47 wt. %, more preferably 18 to 45 wt. % of a mixed plastic polypropylene blend;

[0043] (B) 10 to 60 wt.-%, preferably 15 to 55 wt.-%, more preferably 17 to 52 wt.-% of a heterophasic propylene copolymer; and

[0044] (C) 5 to 25 wt %, preferably 7 to 22 wt %, more preferably 8 to 20 wt % of an inorganic filler;

[0045] wherein all percentages refer to the total composition, and wherein

[0046] Mixed plastic polypropylene blend (A) has

[0047] - a crystalline fraction (CF) content determined according to CRYSTEXQC analysis in the range of 85.0 to 96.0 wt.-%, preferably in the range of 86.5 to 95.5 wt.-%, and

[0048] - a soluble fraction (SF) content determined according to CRYSTEXQC analysis in the range of 4.0 to 15.0 wt.-%, preferably in the range of 4.5 to 13.5 wt.-%, wherein

[0049] - the crystalline fraction (CF) has a content in the range of 1.0 to 10.0 wt. %, preferably in the range of 1.5 to 9.5 wt. % by weight 13 Ethylene content (C2(CF)) determined by FT-IR spectroscopy calibrated with C-NMR spectroscopy; and

[0050] the soluble fraction (SF) has an intrinsic viscosity (iV(SF)) determined in decalin at 135° C. according to DIN ISO 1628 / 1 in the range of 0.9 to 2.1 dl / g, preferably in the range of 1.0 to 2.0 dl / g, more preferably in the range of 1.1 to 1.9 dl / g;

[0051] The heterophasic propylene copolymer (B) comprises a matrix phase and an elastomeric phase dispersed therein and has

[0052] - a melt flow rate MFR2 (230°C, 2.16 kg, ISO 1133) of 85 to 250 g / 10 min, preferably 90 to 150 g / 10 min, more preferably 95 to 125 g / 10 min;

[0053] - a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of greater than 20.0% to 30.0% by weight, and

[0054] - an intrinsic viscosity of the soluble fraction (iV(SF)) measured in decalin at 135° C. in accordance with DIN ISO 1628 / 1 of 2.0 to 4.5 dl / g, preferably 2.4 to 3.8 dl / g, more preferably 2.5 to 3.7 dl / g; and

[0055] The composition has

[0056] - a melt flow rate MFR2 (230°C, 2.16 kg, ISO 1133) of 20 to 60 g / 10 min, preferably 21 to 50 g / 10 min, more preferably 22 to 45 g / 10 min.

[0057] The compositions according to the invention suitable for automotive applications are particularly suitable for the injection molding of articles for vehicle interiors.

[0058] Compositions suitable for automotive applications according to the present invention have one or more of the following characteristics:

[0059] The composition has a melt flow rate MFR2 (230° C., 2.16 kg, ISO 1133) of 20 to 60 g / 10 min, preferably 21 to 50 g / 10 min, more preferably 22 to 45 g / 10 min.

[0060] The composition can be characterized by CRYSTEX QC analysis.In the CRYSTEX QC analysis, a crystalline fraction (CF) and a soluble fraction (SF) are obtained which can be quantified and analyzed according to the monomer and comonomer content and the intrinsic viscosity (IV).

[0061] Preferably, the composition exhibits one or all of the following properties in the CRYSTEX QC analysis:

[0062] - a crystalline fraction (CF) content determined according to CRYSTEXQC analysis in the range of 60.0 to 90.0 wt.-%, preferably in the range of 65.0 to 88.0 wt.-%, and

[0063] - a soluble fraction (SF) content determined according to CRYSTEXQC analysis in the range of 10.0 to 40.0 wt.-%, preferably in the range of 12.0 to 35.0 wt.-%.

[0064] Preferably, the crystalline fraction (CF) has one or more of the following properties, preferably all of the following properties:

[0065] - in the range of 4.0 to 15.0 wt. %, preferably in the range of 4.5 to 14.5 wt. % by quantitative 13 Ethylene content (C2(CF)) determined by FT-IR spectroscopy calibrated with C-NMR spectroscopy; and / or

[0066] An intrinsic viscosity (iV(CF)) of less than 1.8 dl / g, preferably from 0.8 to 1.7 dl / g, determined in decalin at 135° C. to DIN ISO 1628 / 1.

[0067] Preferably, the soluble fraction (SF) has one or more of the following properties, preferably all of the following properties:

[0068] - in the range of 28.0 to 65.0 wt. %, preferably in the range of 30.0 to 60.0 wt. % by quantitative 13 Ethylene content (C2(SF)) determined by FT-IR spectroscopy calibrated with C-NMR spectroscopy; and / or

[0069] An intrinsic viscosity (iV(SF)) of greater than 1.7 dl / g, preferably from 1.8 to 2.6 dl / g, determined in decalin at 135° C. to DIN ISO 1628 / 1.

[0070] Preferably, the composition comprises units derived from ethylene in an amount of from 10.0 to 30.0 wt%, more preferably from 12.5 to 27.5 wt%, still more preferably from 15.0 to 25.0 wt%.

[0071] Preferably, the composition according to the invention exhibits an excellent balance of properties in terms of mechanical properties, thermal stability and especially impact properties, such as in instrumented puncture tests.

[0072] Preferably, the composition has a flexural modulus of from 1500 MPa to 2200 MPa, more preferably from 1600 MPa to 2000 MPa.

[0073] Furthermore, preferably, the composition has a 2 Up to 50.0kJ / m 2 , more preferably 5.5 to 45.0 kJ / m 2 The Charpy notched impact strength at 23°C (CNIS at 23°C) is 2.5 % by weight.

[0074] Still more preferably, the composition has very good impact strength in an instrumented puncture test, especially at low temperatures:

[0075] Preferably, the composition has a puncture energy measured at 23°C of from 12 to 65 J, more preferably from 14 to 60 J.

[0076] Preferably, the composition has an energy at maximum force measured at 23°C of 10 to 60 J, more preferably 12 to 55 J.

[0077] Furthermore, preferably, the composition has a puncture energy measured at 0°C of 3 to 50 J, more preferably of 5 to 45 J.

[0078] Preferably, the composition has an Energy at Maximum Force measured at 0°C of 3 to 50 J, more preferably 5 to 45 J.

[0079] Furthermore, preferably, the composition has a puncture energy measured at -30°C of 3 to 50 J, more preferably 5 to 45 J.

[0080] Preferably, the composition has an Energy at Maximum Force measured at -30°C of 3 to 50 J, more preferably 5 to 45 J.

[0081] Furthermore, preferably, the composition has a heat distortion temperature (ISO 75B) of at least 95°C, more preferably from 96°C to 110°C.

[0082] Furthermore, preferably, the composition has a coefficient of linear thermal expansion (CLTE) of 60 to 125 μm / mK, more preferably 70 to 105 μm / mK.

[0083] The composition of the invention compulsorily comprises components (A), (B) and (C) as described above or below in the amounts described accordingly.

[0084] The composition may optionally comprise additional polymer components, such that the composition may be obtained by blending components (A), (B), (C) and one or more of the following components:

[0085] (D) 0 to 25 wt.%, preferably 0 to 23 wt.%, more preferably 0 to 20 wt.% of a second heterophasic propylene copolymer;

[0086] (E) 0 to 10 wt %, preferably 0 to 9 wt %, more preferably 0 to 8 wt % of high density polyethylene;

[0087] (F) 0 to 20 wt%, preferably 0 to 18 wt%, more preferably 0 to 16 wt% of an ethylene-based plastomer;

[0088] wherein all percentages refer to the total composition, and wherein

[0089] The second heterophasic propylene copolymer (D) comprises a matrix phase and an elastomeric phase dispersed therein and has

[0090] - a melt flow rate MFR2 (230°C, 2.16 kg, ISO 1133) of 8 to 25 g / 10 min, preferably 10 to 24 g / 10 min, more preferably 12 to 23 g / 10 min;

[0091] - a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of 12.5 to 30.0 wt.-%, preferably in the range of 14.0 to 27.0 wt.-%, more preferably in the range of 15.0 to 25.0 wt.-%; and

[0092] - an intrinsic viscosity iV(SF) of the soluble fraction measured in decalin at 135° C. according to DIN ISO 1628 / 1 in the range of 2.3 to 6.0 dl / g, preferably in the range of 2.5 to 5.5 dl / g, more preferably in the range of 2.6 to 4.5 dl / g;

[0093] High-density polyethylene (E) has

[0094] - a melt flow rate MFR2 (190°C, 2.16 kg, ISO 1133) of 0.5 to 30.0 g / 10 min; and

[0095] -945 to 965 kg / m 3 density; and

[0096] The ethylene-based plastomer is a copolymer of ethylene and a comonomer unit selected from an α-olefin having 3 to 12 carbon atoms, preferably an α-olefin having 4 to 10 carbon atoms, most preferably 1-octene, the ethylene-based plastomer having

[0097] - a melt flow rate MFR2 (190° C., 2.16 kg, ISO 1133) of 0.2 to 2.5 g / 10 min, preferably 0.3 to 2.0 g / 10 min; and

[0098] -850 to 870 kg / m 3 , preferably 855 to 865 kg / m 3 density.

[0099] In one embodiment, the composition is obtainable by blending components (A), (B), (C) and (F), in the absence of (D) and (E),

[0100] (A) 15 to 35 wt. %, preferably 17 to 32 wt. %, more preferably 18 to 30 wt. % of a mixed plastic polypropylene blend;

[0101] (B) 30 to 60 wt.-%, preferably 35 to 55 wt.-%, more preferably 40 to 52 wt.-% of the first heterophasic propylene copolymer;

[0102] (C) 5 to 25 wt %, preferably 7 to 22 wt %, more preferably 8 to 20 wt % of an inorganic filler; and

[0103] (F) 5 to 20 wt%, preferably 7 to 18 wt%, more preferably 8 to 16 wt% of an ethylene-based plastomer;

[0104] All percentages therein refer to the total composition.

[0105] In another embodiment, the composition is obtainable by blending components (A), (B), (C), (E) and (F), in the absence of (D),

[0106] (A) 25 to 50 wt. %, preferably 27 to 47 wt. %, more preferably 30 to 45 wt. % of a mixed plastic polypropylene blend;

[0107] (B) 20 to 50 wt.-%, preferably 25 to 45 wt.-%, more preferably 30 to 42 wt.-% of the first heterophasic propylene copolymer;

[0108] (C) 5 to 25 wt %, preferably 7 to 22 wt %, more preferably 8 to 20 wt % of an inorganic filler;

[0109] (E) 2 to 10 wt %, preferably 3 to 9 wt %, more preferably 5 to 8 wt % high density polyethylene; and

[0110] (F) 2 to 20 wt%, preferably 3 to 18 wt%, more preferably 4 to 16 wt% of an ethylene-based plastomer;

[0111] All percentages therein refer to the total composition.

[0112] In yet another embodiment, the composition is obtainable by blending components (A), (B), (C), (D), and (E), in the absence of (F),

[0113] (A) 25 to 50 wt. %, preferably 27 to 47 wt. %, more preferably 30 to 45 wt. % of a mixed plastic polypropylene blend;

[0114] (B) 15 to 30 wt.-%, preferably 17 to 27 wt.-%, more preferably 18 to 25 wt.-% of the first heterophasic propylene copolymer;

[0115] (C) 5 to 25 wt %, preferably 7 to 22 wt %, more preferably 8 to 20 wt % of an inorganic filler;

[0116] (D) 5 to 25 wt.%, preferably 8 to 23 wt.%, more preferably 10 to 20 wt.% of a second heterophasic propylene copolymer; and

[0117] (E) 2 to 10 wt %, preferably 3 to 9 wt %, more preferably 5 to 8 wt % high density polyethylene;

[0118] All percentages therein refer to the total composition.

[0119] Mixed plastic polypropylene blend (A)

[0120] The mixed plastic polypropylene blend (A) is suitable for characterization by CRYSTEX QC analysis. In the CRYSTEX QC analysis, a crystalline fraction (CF) and a soluble fraction (SF) are obtained which can be quantified and analyzed according to the monomer and comonomer content and the intrinsic viscosity (iV).

[0121] In the CRYSTEX QC analysis, the mixed plastic polypropylene blend (A) showed the following properties:

[0122] - a crystalline fraction (CF) content determined according to CRYSTEX QC analysis in the range of 85.0 to 96.0 wt.-%, preferably in the range of 86.5 to 95.5 wt.-%, more preferably in the range of 88.0 to 95.0 wt.-%; and

[0123] - a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of 4.0 to 15.0 wt.-%, preferably in the range of 4.5 to 13.5 wt.-%, more preferably in the range of 5.0 to 12.0 wt.-%.

[0124] The crystalline fraction (CF) has one or more of the following properties, preferably all of the following properties:

[0125] - in the range of 1.0 to 10.0 wt. %, preferably in the range of 1.5 to 9.5 wt. %, more preferably in the range of 2.0 to 9.0 wt. % by quantitative 13 Ethylene content (C2(CF)) determined by FT-IR spectroscopy calibrated with C-NMR spectroscopy; and / or

[0126] - an intrinsic viscosity (iV(CF)) measured in decalin at 135° C. according to DIN ISO 1628 / 1, preferably in the range of 1.0 to 2.6 dl / g, more preferably in the range of 1.2 to 2.5 dl / g, still more preferably in the range of 1.3 to 2.4 dl / g.

[0127] The soluble fraction (SF) has one or more of the following properties, preferably all of the following properties:

[0128] - preferably in the range of 20.0 to 55.0 wt. %, preferably in the range of 22.0 to 50.0 wt. %, more preferably in the range of 24.0 to 48.0 wt. % by quantitative 13 Ethylene content (C2(SF)) determined by FT-IR spectroscopy calibrated with C-NMR spectroscopy; and / or

[0129] - an intrinsic viscosity (iV(SF)) measured in decalin at 135° C. according to DIN ISO 1628 / 1 in the range of 0.9 to 2.1 dl / g, preferably in the range of 1.0 to 2.0 dl / g, more preferably in the range of 1.1 to 1.9 dl / g.

[0130] Preferably, the mixed plastic polypropylene blend (A) comprises polypropylene and polyethylene.

[0131] Preferably, the weight ratio of polypropylene to polyethylene is from 19:1 to 7:3.

[0132] Preferably the mixed plastic polypropylene blend (A) comprises propylene-derived units in an amount of more than 50 mol%.

[0133] Preferably the mixed plastic polypropylene blend (A) comprises units derived from ethylene in an amount of 2.5 to 15.0 wt%, more preferably 4.0 to 12.5 wt%, still more preferably 5.0 to 10.0 wt%.

[0134] Furthermore, preferably, the mixed plastic polypropylene blend (A) has one or more, preferably all, of the following properties:

[0135] - a melt flow rate MFR2 (230°C, 2.16 kg, ISO 1133) of 8.0 to 40 g / 10 min, preferably 9.0 to 35 g / 10 min, more preferably 10.0 to 30 g / 10 min; and / or

[0136] - Limonene content determined by using solid phase microextraction (HS-SPME-GC-MS): 0.1 ppm to 50 ppm; and / or

[0137] - a tensile modulus of 1000 MPa to 1500 MPa, preferably 1100 MPa to 1400 MPa; and / or

[0138] -3.0 to 7.5 kJ / m 2 , preferably 4.0 to 7.0 kJ / m 2 The Charpy notched impact strength at 23°C (CNIS at 23°C) is 1.23°C.

[0139] The mixed plastic polypropylene blend according to the present invention is preferably in the form of pellets. Pelletization contributes to low amounts of volatile matter.

[0140] Heterophasic propylene copolymer (B)

[0141] The heterophasic polypropylene copolymer (B) comprises a matrix phase and an elastomeric phase dispersed therein.

[0142] The heterophasic propylene copolymer (B) is characterized in that

[0143] - a melt flow rate MFR2 (230°C, 2.16 kg, ISO 1133) of 85 to 250 g / 10 min, preferably 90 to 150 g / 10 min, more preferably 95 to 125 g / 10 min;

[0144] - a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of 20.0 to 30.0 wt.-%, preferably in the range of 20.5 to 28.0 wt.-%, more preferably in the range of 21.0 to 26.0 wt.-%; and

[0145] - an intrinsic viscosity iV(SF) of the soluble fraction measured in decalin at 135° C. according to DIN ISO 1628 / 1 of 2.0 to 4.5 dl / g, preferably 2.4 to 3.8 dl / g, more preferably 2.5 to 3.7 dl / g.

[0146] Preferably, the heterophasic propylene copolymer (B) has one or more, preferably all, of the following properties:

[0147] - a content of units derivable from ethylene (C2) in the soluble fraction (SF) of 30 to 45% by weight, preferably of 32 to 40% by weight, more preferably of 33 to 38% by weight; and / or

[0148] - a content of units derived from ethylene (C2) in the crystalline fraction (CF) of from 0.1 to 5.0% by weight, preferably from 0.2 to 4.0% by weight, more preferably from 0.5 to 3.0% by weight; and / or

[0149] - a total content of units derived from ethylene (C2) of 5.0 to 15.0% by weight, preferably 6.0 to 12.0% by weight, more preferably 7.0 to 10.0% by weight; and / or

[0150] - intrinsic viscosity of the crystalline fraction iV(CF), determined according to CRYSTEX QC analysis and measured in decalin at 135° C. according to DIN ISO 1628 / 1, of from 0.8 to 2.0 dl / g, preferably from 0.9 to 1.8 dl / g; and / or

[0151] - a melting temperature Tm of 155 to 175°C, preferably 157 to 172°C, more preferably 160 to 170°C; and / or

[0152] - a crystallization temperature Tc of 120 to 140°C, preferably 122 to 137°C, more preferably 125 to 135°C; and / or

[0153] - a tensile modulus of 1250 MPa to 1800 MPa, preferably 1300 MPa to 1750 MPa, more preferably 1350 to 1700 MPa; and / or

[0154] -4.0 to 8.5 kJ / m 2 , preferably 5.0 to 7.0 kJ / m 2The Charpy notched impact strength at 23°C (CNIS at 23°C) is 1.23°C.

[0155] Preferably, the heterophasic propylene copolymer (B) consists of propylene units and ethylene units.

[0156] Although not measured, the content of units derived from propylene (C3) in the soluble fraction (SF) and the content of units derived from ethylene (C2) in the soluble fraction (SF) preferably total 100% by weight.

[0157] Preferably, the content of units derived from propylene (C3) in the soluble fraction (SF) is in the range of 55 to 70 wt.-%, more preferably in the range of 60 to 68 wt.-%, still more preferably in the range of 62 to 67 wt.-%.

[0158] Although not measured, the content of units derived from propylene (C3) in the crystalline fraction (CF) and the content of units derived from ethylene (C2) in the crystalline fraction (CF) preferably total 100% by weight.

[0159] Preferably, the content of units derived from propylene (C3) in the crystalline fraction (CF) is from 95.0 to 99.9 wt%, more preferably from 96.0 to 99.8 wt%, still more preferably from 97.0 to 99.5 wt%.

[0160] Preferably, the total content of units derived from propylene (C3) in the heterophasic propylene copolymer (B) is from 85.0 to 95.0 wt.-%, more preferably from 88.0 to 94.0 wt.-%, yet more preferably from 90.0 to 93.0 wt.-%.

[0161] These heterophasic propylene copolymers are commercially available.

[0162] Inorganic filler (C)

[0163] Preferably, the inorganic filler (C) is talc.

[0164] Preferably, the inorganic filler (preferably talc) (C) has a median particle size d before compounding of 0.3 to 30.0 microns, more preferably 1.5 to 15.0 microns. 50 .

[0165] Furthermore, preferably, the inorganic filler (preferably talc) (C) has a top cut particle size d before compounding of 1.0 to 50.0 μm, preferably 5.0 to 35.0 μm. 95 .

[0166] These inorganic fillers are commercially available.

[0167] additive

[0168] Additives are typically used in the composition according to the present invention. Preferably, the additive is selected from one or more of an antioxidant, a UV stabilizer, a slip agent, a nucleating agent, a pigment, a lubricant, a masterbatch polymer and / or an anti-fog agent.

[0169] The additive is generally present in the composition in an amount of 0.01 to 4.0 wt. %, preferably 0.05 to 3.0 wt. %, based on the total composition.

[0170] Second heterophasic propylene copolymer (D)

[0171] The optional heterophasic polypropylene copolymer (D) comprises a matrix phase and an elastomeric phase dispersed therein.

[0172] In case a second heterophasic propylene copolymer (D) is present in the composition, preferably this second heterophasic propylene copolymer (D) has a melt flow rate which is lower than the melt flow rate of the heterophasic propylene copolymer (B).

[0173] The optional second heterophasic propylene copolymer (D) has a melt flow rate MFR2 (230°C, 2.16 kg, ISO 1133) of 8 to 25 g / 10 min, preferably 10 to 24 g / 10 min, more preferably 12 to 23 g / 10 min.

[0174] Furthermore, the optional second heterophasic propylene copolymer (D) has a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of 12.5 to 30.0 wt.-%, preferably in the range of 14.0 to 27.0 wt.-%, more preferably in the range of 15.0 to 25.0 wt.-%.

[0175] Preferably, the soluble fraction has an intrinsic viscosity iV(SF) measured in decalin at 135° C. according to DIN ISO 1628 / 1 of 2.3 to 6.0 dl / g, preferably 2.5 to 5.5 dl / g, more preferably 2.6 to 4.5 dl / g.

[0176] Preferably, the optional second heterophasic propylene copolymer (D) has a crystalline fraction (CF) content determined according to CRYSTEX QC analysis in the range of 70.0 to 87.5 wt.-%, preferably in the range of 73.0 to 86.0 wt.-%, more preferably in the range of 75.0 to 85.0 wt.-%.

[0177] Preferably, the optional second heterophasic propylene copolymer (D) has one or more, preferably all, of the following properties:

[0178] - a content of units derived from ethylene in the soluble fraction (SF) of 30 to 45% by weight, preferably of 32 to 40% by weight, more preferably of 33 to 38% by weight; and / or

[0179] - a content of units derived from ethylene in the crystalline fraction (CF) of 0.5 to 7.5% by weight, preferably of 1.0 to 5.0% by weight, more preferably of 1.5 to 4.0% by weight; and / or

[0180] - a total content of units derived from ethylene of from 5.0 to 15.0% by weight, preferably from 6.0 to 12.0% by weight, more preferably from 6.5 to 10.0% by weight; and / or

[0181] - intrinsic viscosity iV(CF) of the crystalline fraction determined according to CRYSTEX QC analysis and measured in decalin at 135° C. according to DIN ISO 1628 / 1 in the range of 1.0 to 2.0 dl / g, preferably in the range of 1.1 to 1.9 dl / g; and / or

[0182] - a melting temperature Tm of 155 to 175°C, preferably 157 to 172°C, more preferably 160 to 170°C; and / or

[0183] - a crystallization temperature Tc of 120 to 140°C, preferably 122 to 137°C, more preferably 125 to 135°C.

[0184] It is preferred that the optional heterophasic propylene copolymer (D) consists of propylene units and ethylene units.

[0185] Although not measured, the content of units derived from propylene (C3) in the soluble fraction (SF) and the content of units derived from ethylene (C2) in the soluble fraction (SF) preferably total 100% by weight.

[0186] Preferably, the content of units derived from propylene (C3) in the soluble fraction (SF) is from 55 to 70 wt%, more preferably from 60 to 68 wt%, still more preferably from 62 to 67 wt%.

[0187] Although not measured, the content of units derived from propylene (C3) in the crystalline fraction (CF) and the content of units derived from ethylene (C2) in the crystalline fraction (CF) preferably total 100% by weight.

[0188] Preferably, the content of units derived from propylene (C3) in the crystalline fraction (CF) is from 92.5 to 99.5 wt.-%, more preferably from 95.0 to 99.0 wt.-%, still more preferably from 96.0 to 98.5 wt.-%.

[0189] Preferably, the total content of units derived from propylene (C3) in the heterophasic propylene copolymer (B) is from 85.0 to 95.0 wt.-%, more preferably from 88.0 to 94.0 wt.-%, more preferably from 90.0 to 93.5 wt.-%.

[0190] The optional second heterophasic polypropylene copolymer (D) is preferably nucleated, more preferably nucleated with poly(vinylcyclohexane) such as described in EP 2 960 279 B1.

[0191] These heterophasic propylene copolymers are commercially available.

[0192] High-density polyethylene (E)

[0193] High-density polyethylene (E), in particular virgin high-density polyethylene (E), can be added to the composition according to the invention.

[0194] The high density polyethylene (E) contributes to the scratch resistance of the final composition. Due to the presence of high density polyethylene in the blend (A), the amount of high density polyethylene (E) for the targeted scratch resistance can be reduced or can be omitted entirely.

[0195] The optional high density polyethylene (E) preferably has one or more, preferably all of the following properties:

[0196] - a melt flow rate MFR2 (190°C, 2.16 kg, ISO 1133) of 0.5 to 30.0 g / 10 min; and / or

[0197] -945 to 965 kg / m 3 density.

[0198] These high-density polyethylenes are commercially available.

[0199] Ethylene-based plastomers (F)

[0200] Preferably, the optional ethylene-based plastomer (F) is a copolymer of ethylene and comonomer units selected from α-olefins having 3 to 12 carbon atoms, preferably α-olefins having 4 to 10 carbon atoms, most preferably 1-octene.

[0201] Ethylene-based plastomers are often added to further improve the impact properties of the composition.

[0202] Preferably, the optional ethylene-based plastomer (F) has one or more, preferably all, of the following properties:

[0203] - a melt flow rate MFR2 (190° C., 2.16 kg, ISO 1133) of 0.2 to 2.5 g / 10 min, preferably 0.3 to 2.0 g / 10 min; and

[0204] -850 to 870 kg / m 3 , preferably 855 to 865 kg / m 3 density.

[0205] These ethylene-based plastomers are commercially available under the trade names Engage, Exact, Queo, Tafmer, and the like.

[0206] Products

[0207] In another aspect, the present invention relates to an article, preferably a molded article, more preferably a molded automotive article, comprising a composition as described above or below.

[0208] Preferably, the article is used in a vehicle interior.

[0209] Preferably, the article exhibits good surface quality.

[0210] It is preferred that the article has a surface quality of MSE below 15, preferably below 14.

[0211] use

[0212] In another aspect, the present invention relates to the use of a composition as described above or below for injection molding of an article, preferably an automotive article, more preferably an automotive interior article.

[0213] Experimental part

[0214] The following examples are included to illustrate certain aspects and embodiments of the present invention as described in the claims. However, it should be understood by those skilled in the art that the following description is illustrative only and should not be regarded as limiting the present invention in any way.

[0215] Test Method

[0216] a) CRYSTEX

[0217] Crystalline and soluble fractions and determination of their respective properties (IV and ethylene content)

[0218] The crystalline fraction (CF) and soluble fraction (SF) of the polypropylene composition, as well as the comonomer content and intrinsic viscosity of each fraction, were analyzed using a CRYSTEX instrument, Polymer Char (Valencia, Spain). Details of this technology and method can be found in the literature (Ljiljana Jeremic, Andreas Albrecht, Martina Sandholzer & Markus Gahleitner (2020) Rapid characterization of high-impact ethylene-propylene copolymer composition by crystallization extraction separation: comparability to standard separation methods, International Journal of Polymer Analysis and Characterization, 25: 8, pp. 581-596).

[0219] The crystalline and amorphous fractions were separated by temperature cycling with dissolution at 160°C, crystallization at 40°C, and redissolution in 1,2,4-trichlorobenzene at 160°C. Quantification of SF and CF as well as determination of the ethylene content (C2) were achieved by an integrated infrared detector (IR4), and the intrinsic viscosity (iV) was determined using an online 2-capillary viscometer.

[0220] The IR4 detector is based on two different wavelengths (CH3 stretching vibration (centered at about 2960 cm -1 ) and CH stretching vibration (2700 to 3000 cm -1 The IR4 detector is calibrated with a series of eight EP copolymers having known ethylene contents (measured by the IR absorbance at the two different wavelength bands) ranging from 2 wt% to 69 wt%. 13 C-NMR spectroscopy), and each EP copolymer used for calibration had multiple concentrations between 2 and 13 mg / ml. In order to simultaneously experience two characteristics of the polymer at various concentrations during the Crystex analysis, concentration and ethylene content, the following calibration equation was applied:

[0221] Concentration = a + b * absorbance (CH) + c * (absorbance (CH)) 2 +d*absorbance(CH3)+e*absorbance(CH3) 2+f*Absorbance(CH)*Absorbance(CH3) (Equation 1)

[0222] CH3 / 1000C=a+b*absorbance(CH3)+c*absorbance(CH3)+d*(absorbance(CH3) / absorbance(CH3))+e*(absorbance(CH3) / absorbance(CH3)) 2 (Equation 2)

[0223] Constants a to e of Equation 1 and constants a to f of Equation 2 are determined by using least squares regression analysis.

[0224] The following relationship is used to convert CH3 / 1000C to ethylene content in weight %:

[0225] Weight % (ethylene in EP copolymer) = 100 - CH3 / 1000TC*0.3 (Equation 3)

[0226] The amounts of the soluble fraction (SF) and the crystalline fraction (CF) are related by means of an XS calibration to the amount of "xylene cold solubles" (XCS) and the xylene cold insolubles (XCI) fraction, respectively, determined according to the standard gravimetric method according to ISO 16152. The XS calibration was achieved by testing various EP copolymers with an XS content in the range of 2 to 31 wt%. The determined XS calibration is linear:

[0227] wt%XS=1.01*wt%SF (Equation 4)

[0228] The intrinsic viscosity (iV) of the parent EP copolymer and its soluble fraction and crystalline fraction was determined using an online 2-capillary viscometer and correlated with the corresponding iV determined by the standard method in decalin according to ISO 1628-3. Calibration was achieved using various EP PP copolymers with iV = 2 to 4 dl / g. The calibration curve determined was linear:

[0229] iV(dL / g)=a*Vsp / c (Equation 5)

[0230] The sample to be analyzed was weighed out at a concentration of 10 mg / ml to 20 mg / ml. To avoid injecting gels and / or polymers that are insoluble in TCB at 160°C, such as PET and PA, the weighed sample was squeezed through a stainless steel mesh MW 0.077 / D 0.05 mm.

[0231] After automatically filling the vial with 1,2,4-TCB containing 250 mg / l 2,6-tert-butyl-4-methylphenol (BHT) as an antioxidant, the sample was dissolved at 160°C until completely dissolved, typically for 60 minutes, with continuous stirring at 400 rpm. To avoid sample degradation, the polymer solution was covered with a N2 atmosphere during the dissolution process.

[0232] A defined volume of sample solution is injected into a column filled with an inert support, where crystallization of the sample and separation of the soluble fraction from the crystalline portion occur. This process is repeated twice. During the first injection, the entire sample is measured at high temperature, and the IV (dl / g) and C2 (wt%) of the PP composition are determined. During the second injection, the soluble fraction (at low temperature) and the crystalline fraction (CF) (at high temperature) are measured during the crystallization cycle (wt% SF, wt% C2, IV).

[0233] b) Xylene cold soluble fraction (XCS, weight %)

[0234] The xylene cold soluble fraction (XCS) is determined according to ISO 16152; 1st edition; 2005-07-01 at 25° C. The portion that remains insoluble is the xylene cold insoluble (XCI) fraction.

[0235] c) Intrinsic viscosity

[0236] The intrinsic viscosity is measured in accordance with DIN ISO 1628 / 1, October 1999 (in decalin at 135° C.).

[0237] d) Simply supported beam notched impact strength

[0238] According to ISO 1791eA at +23 ° C and -20 ° C on 80 × 10 × 4 mm prepared according to EN ISO 1873-2 3 The measurement is carried out after a conditioning time of 96 hours at 23° C. on the test specimens.

[0239] e) Flexural modulus

[0240] Flexural modulus according to ISO 178 at a test speed of 2 mm / min and a force of 100 N on a specimen prepared by injection molding according to EN ISO 1873-2 with dimensions of 80×10×4 mm 3 The test specimens were measured with a length of 64 mm (length x width x thickness) where the span between the supports was 64 mm.

[0241] f) Tensile modulus

[0242] Measured according to ISO 527-2 (crosshead speed = 1 mm / min; test speed at 23° C. is 50 mm / min) using injection molded test specimens 1B (dog bone shape, 4 mm thick) prepared as described in EN ISO 1873-2. The measurement is carried out after a conditioning time of 96 hours at 23° C.

[0243] g) Instrumented puncture test

[0244] The instrumented puncture test was carried out according to ISO 6603-2:2000 at 23°C, 0°C and -30°C on a 60×60×3 mm 3 The measurements were carried out after a conditioning time of 96 hours at 23°C on the samples.

[0245] h) Comonomer content

[0246] Poly(propylene-co-ethylene)-ethylene content-IR spectroscopy

[0247] Quantitative infrared (IR) spectroscopy was used to quantify the ethylene content of poly(ethylene-co-propylene) copolymers by calibration to the primary method. 13 Calibration was facilitated by in-house, non-commercial calibration standards of known ethylene content, determined by solution-state nuclear magnetic resonance (NMR) spectroscopy. The calibration procedure was performed in a conventional manner well documented in the literature. The calibration set consisted of 38 calibration standards with ethylene contents ranging from 0.2 to 75.0 wt%, produced under various conditions at pilot or full scale. The calibration set was selected to reflect the typical types of copolymers encountered by the final quantitative IR spectroscopy method.

[0248] Solid-state quantitative IR spectra were recorded using a Bruker Vertex 70 FTIR spectrometer. Spectra were recorded at 180 to 210° C. and 4 to 6 MPa on 25×25 mm square films 300 μm thick prepared by compression molding. For samples with very high ethylene content (>50 mol %), 100 μm thick films were used. Standard transmission FTIR spectrometer was used with a 5000–500 cm -1 spectral range, 6mm aperture, 2cm -1 spectral resolution, 16 background scans, 16 spectral scans, an interferogram zero filling factor of 64, and the Blackmann-Harris 3-term apodization method. >2 The structural unit is at 730 and 720 cm -1 (A Q ) total area of ​​CH2 rocking deformation at 762 and 694 cm (integration method G, -1 The quantitative analysis was performed using the limit value. The quantitative band was normalized to the band corresponding to the CH structural unit at 4323 cm -1 (A R ) (integration method G, limit 4650, 4007 cm -1 ). Then a quadratic calibration curve was used to calculate the normalized absorbance (A Q / A R) to predict the ethylene content in weight percent. This calibration curve has been previously constructed by ordinary least squares (OLS) regression of the normalized absorbance measured on the calibration set and the main comonomer content.

[0249] Poly(propylene-co-ethylene)-ethylene content- 13 CNMR spectroscopy

[0250] Use for 1 H and 13 Quantitative measurements were recorded in solution on a Bruker Avance III 400 NMR spectrometer operating at 400.15 and 100.62 MHz, respectively. 13 C{ 1 H} NMR spectroscopy. Nitrogen was used for all pneumatics and all spectra were 13 The C-optimized 10 mm extended temperature probe was recorded at 125° C. About 200 mg of the material was dissolved in 3 ml of 1,2-tetrachloroethane-d2 (TCE-d2) along with chromium(III) acetylacetonate (Cr(acac)3) to give a 65 mM solution of the relaxation agent in the solvent (Singh, G., Kothari, A., Gupta, V., Polymer Testing 28 5 (2009), 475).

[0251] To ensure a homogeneous solution, the NMR tube was further heated in a rotary oven for at least 1 hour after initial sample preparation in a heating block. After insertion of the magnet, the tube was rotated at 10 Hz. This setup was chosen primarily for high resolution and accurate quantification of ethylene content, which was quantitatively required. A standard single pulse excitation without NOEs was employed, using an optimized top cone angle, a recycle delay of 1 s, and a two-stage WALTZ16 decoupling scheme (Zhou, Z. et al., J. Mag. Reson. 187 (2007) 225, and Busico, V. et al., Macromol. Rapid Commun. 2007, 28, 1128). A total of 6144 (6k) transients were collected for each spectrum. For quantitative 13 C{ 1H} NMR spectra are processed, integrated and the relevant quantitative properties are determined from the integration. All chemical shifts are indirectly referenced to the central methylene group of the ethylene block (EEE) at 30.00 ppm using the chemical shift of the solvent. This method allows for comparable references even if this structural unit is not present. Characteristic signals corresponding to the incorporation of ethylene are observed (Cheng, HN, Macromolecules 17 (1984), 1950), and the comonomer fraction is calculated as the fraction of ethylene in the polymer relative to all monomers in the polymer: fE=(E / (P+E). Using the method of Wang et al. (Wang, WJ., Zhu, S., Macromolecules 33 (2000), 1157), by 13 C{ 1 The integration of multiple signals over the entire spectral region in the H} spectrum quantifies the comonomer fraction. This method was chosen for its robustness and ability to account for the presence of regional defects when required. The integration region was slightly adjusted to improve applicability over the entire range of comonomer contents encountered. For systems where only isolated ethylene with very low ethylene content in the PPEPP sequence was observed, the method of Wang et al. was modified to reduce the influence of the integration of sites that are no longer present. This method reduces the overestimation of ethylene content in such systems and is achieved by reducing the number of sites used to determine the absolute ethylene content to the following: E ​​= 0.5(Sββ + Sβγ + Sβδ + 0.5(Sαβ + Sαγ)). By using this set of sites, the corresponding integration equation becomes: E = 0.5(I H +I G +0.5(I C +I D )). The same symbols used in the article by Wang et al. (Wang, WJ., Zhu, S., Macromolecules 33 (2000), 1157) are used. The equations for absolute propylene content are not modified. The mole percent comonomer incorporation is calculated from the mole fraction: E [mol %] = 100 * fE. The weight percent comonomer incorporation is calculated from the mole fraction: E [weight %] = 100 * (fE * 28.06) / ((fE * 28.06) + ((1 - fE) * 42.08)).

[0252] i) Comonomer content

[0253] Using the film thickness method, the content is determined using the strength of the quantitative tape I(q) and the thickness of the pressed film T using the following relationship: [I(q) / T]m+c=C, where m and c are obtained from 13 The coefficients were determined from the calibration curve constructed using C-NMR spectroscopy to determine the comonomer content.

[0254] Comonomer content was determined using a Nicolet Magna 550 IR spectrometer and Nicolet Omnic FTIR software based on 13 Fourier transform infrared spectroscopy (FTIR) calibrated with C-NMR was measured in a known manner. Films with a thickness of approximately 250 μm were compression molded from the samples. Similar films were made from calibration samples with known comonomer content. The comonomer content was determined by the wavelength range of 1430 to 1100 cm -1 The absorbance is measured as the peak height by selecting the so-called short baseline, the long baseline, or both. The short baseline is drawn through the lowest point at approximately 1410 to 1320 cm -1 , and the long baseline is drawn at about 1410 and 1220 cm -1 A specific calibration is required for each baseline type. In addition, the comonomer content of the unknown samples is within the comonomer content range of the calibration samples.

[0255] j)MFR

[0256] The melt flow rate (MFR2) is measured at 230°C (polypropylene-based materials) or 190°C (polyethylene-based materials) under a load of 2.16 kg. The melt flow rate is the amount of polymer in grams that can be extruded in 10 minutes at a temperature of 230°C (or 190°C) under a load of 2.16 kg using a test apparatus according to ISO 1133.

[0257] k) Density

[0258] Density was measured according to ISO 1183-187. Sample preparation was performed by compression molding according to ISO 1872-2:2007.

[0259] 1) Heat Deflection Temperature (HDT)

[0260] HDT was prepared in accordance with ISO 1873-2 in an 80×10×4 mm 3 The test results are determined on injection-molded test specimens of 100 nm and stored at +23°C for at least 96 hours before measurement. The test is carried out on horizontally supported specimens according to ISO 75, condition B with a nominal surface stress of 0.45 MPa.

[0261] m) Coefficient of linear thermal expansion (CLTE)

[0262] The coefficient of linear thermal expansion (CLTE) was determined according to ISO 11359-2: 1999 on 10 mm long pieces cut from the same injection molded specimens used for the tensile modulus determination. The measurements were carried out in the machine direction (MD) at a heating rate of 1°C / min in the temperature range of -30 to +80°C (or -30 to +85°C) and at a heating rate of 1°C / min in the temperature range of 23 to +80°C (or 23 to +85°C).

[0263] n) Tiger stripes (MSE) or flow marks

[0264] The trend of flow marks was examined using the method described below. This method is described in detail in WO 2010 / 149529, the entire contents of which are incorporated herein. Optical measurement systems were used to characterize surface quality, as described by Sybille Frank et al. in PPS 25 Intern. Conf. Polym. Proc. Soc 2009 or Proceedings of the SPIE, Vol. 6831, pp. 68130T-68130T-8 (2008).

[0265] This approach consists of two aspects:

[0266] 1. Image recording:

[0267] The basic principle of the measurement system is to illuminate the board with a defined light source (LED) in a closed environment and record the image with a CCD camera system.

[0268] 2. Image Analysis:

[0269] The specimen is flood-illuminated from one side, and the upwardly reflected portion of the light is deflected by two mirrors onto a CCD sensor. The grayscale image thus created is analyzed line by line. Based on the deviations in the recorded grayscale values, the mean square error (MSE) is calculated, thereby quantifying the surface quality. The larger the MSE value, the more pronounced the surface defects. Generally, for the same material, the tendency for flow marks increases as the injection speed increases.

[0270] For this evaluation, a die VW K50 of 440 × 148 × 2.8 mm was used. 3 The plates were gated with a 1.4 mm film gate and were produced with different fill times of 1.5, 3, and 6 seconds, respectively.

[0271] Other conditions:

[0272] Melting temperature: 240℃.

[0273] Mold temperature 30℃.

[0274] Dynamic pressure: 10 bar hydraulic

[0275] Within a certain filling time, the smaller the MSE value, the smaller the trend of the flow trace.

[0276] experiment

[0277] Catalyst system:

[0278] For the polymerization of HECO 2, the Ziegler-Natta catalyst used in the inventive examples of WO 2016 / 066446 A1 and described in detail therein was used. For the polymerization of HECO 1 and HECO 3, the same catalyst was used, but prepolymerized with vinylcyclohexane to achieve nucleation with poly(vinylcyclohexane).

[0279] Nucleation by prepolymerization with vinylcyclohexane is described in detail in EP 2 960 256 B1 and EP 2 960 279 B1. These documents are incorporated by reference. In all cases, triethylaluminum (TEAL) was used as a cocatalyst and dicyclopentadienyl-dimethoxysilane (donor D) was used as an external donor, the respective feed ratios being indicated in Table 1 below.

[0280] HECO 1, HECO 2 and HECO 3 were produced in a Borstar PP pilot plant with a prepolymerization / loop reactor / gas phase reactor 1 / gas phase reactor 2 / gas phase reactor 3 configuration followed by a pelletizing step.

[0281] Table 1: Preparation of HECO 1, HECO 2, and HECO 3

[0282]

[0283]

[0284] The heterophasic copolymers HECO 1, HECO 2, and HECO 3 were compounded in a co-rotating twin-screw extruder Coperion ZSK 47 at 220° C. with 0.15% by weight of an antioxidant (Irganox B215FF from BASF AG, Germany; a 1:2 mixture of pentaerythritol tetrakis(3-(3',5'-di-tert-butyl-4-hydroxyphenyl)propionate (CAS No. 6683-19-8) and tris(2,4-di-tert-butylphenyl)phosphite (CAS No. 31570-04-4)); and 0.05% by weight of calcium stearate (CAS No. 1592-23-0, commercially available from Faci, Italy). CRYSTEX QC analysis of the three copolymers gave the results listed in Table 2.

[0285] Table 2: CRYSTEX QC analysis of HECO 1, HECO 2, and HECO 3

[0286] HECO 1 HECO 2 HECO 3 CF weight% 78.0 83.0 83.1 C2(CF) weight% 1.1 1.8 2.2 iV(CF) dl / g 1.0 1.6 1.4 SF weight% 22.0 17.0 16.9 C2(SF) weight% 35.0 35.0 32.2 iV(SF) dl / g 3.4 2.7 3.3

[0287] The properties of the polypropylene / polyethylene blends (A) used for evaluation are shown in Table 3. Since these compositions are from a mechanical recycling process, the properties are indicated as ranges.

[0288] Table 3: Properties of polypropylene / polyethylene blends (blend A)

[0289]

[0290]

[0291] HDPE 1 is commercial grade MB5568 from Borealis AG, Austria, with a density of 955 kg / m 3 (ISO 1183), a density of 0.8 g / 10 min (2.16 kg, 190° C., ISO 1133), and a tensile modulus of 1000 MPa (ISO 527-2).

[0292] HDPE 2 is commercial grade MB7541 from Borealis AG, Austria, with a density of 954 kg / m 3 (ISO 1183), a density of 4 g / 10 min (2.16 kg, 190° C., ISO 1133), and a tensile modulus of 850 MPa (ISO 527-2).

[0293] Plastic body 1 is Engage 8842, with a density of 857 kg / m 3 and an ethylene-1-octene plastomer having an MFR2 (2.16 kg, 190° C., ISO 1133) of 1.0 g / 10 min, commercially available from The Dow Company, USA.

[0294] Plastic body 2 is Engage 8180, with a density of 863kg / m 3 and an ethylene-1-octene plastomer having an MFR2 (2.16 kg, 190° C., ISO 1133) of 0.5 g / 10 min, commercially available from The Dow Company, USA.

[0295] Talc 1 is Luzenac HAR T84, its d 50 2.0 μm, d 95 10.0 μm (sedimentography measurement), commercially available from IMERYS, France.

[0296] Talc 2 is Jetfine 3CA, its d 50 1.2 μm, d 953.3 μm (sedimentography measurement), commercially available from IMERYS, France.

[0297] The final compositions were compounded in a Coperion ZSK40 twin screw extruder at 220° C. using polymer and talc along with antioxidants, UV-stabilizers, slip agents, nucleating agents, carbon black masterbatch, calcium stearate, anti-fog agents.

[0298] Table 4: Composition of Examples

[0299]

[0300]

[0301] Table 5 shows the performance of the examples.

[0302] Table 5: Performance of the Examples

[0303] CE1 CE2 CE3 IE1 IE2 IE3 IE4 IE5 <![CDATA[MFR2,g / 10min]]> 22 18 14 23 23 26 24 26 C2(Comp), weight% 22.0 16.0 12.2 16.3 16.3 19.7 23.0 22.0 iV(Comp), dl / g 1.88 1.74 1.77 1.63 1.63 1.53 1.59 1.56 CF (CRYSTEX), weight % 79 84 79 84 85 79 67 67 C2(CF), wt% 14.2 13.0 13.8 13.5 13.5 13.8 4.8 5.25 iV(CF), dl / g 1.42 1.69 1.46 1.56 1.56 1.44 1.28 1.31 SF (CRYSTEX), weight % 21 16 21 16 15 21 33 33 C2(SF), weight % 39.8 36.0 33.5 32.6 32.6 43.5 59.0 57.0 iV(SF), dl / g 1.42 1.93 1.78 2.05 2.05 1.91 2.19 2.08 Flexural modulus, MPa 1891 1819 1706 1731 1884 1761 1868 1759 <![CDATA[Simply supported beam NIS, +23 °C, kJ / m 2 > 6.0 6.1 5.8 5.7 5.7 8.8 38.0 38.0 <![CDATA[Simply supported beam NIS, -20 °C, kJ / m 2 > 3.1 2.2 2.1 nm nm nm 4.8 5.0 IPT test: Maximum force energy, +23℃, J 9.2 7.5 4.9 20.0 24.0 25.0 21.0 21.0 Puncture energy, +23℃, J 11.0 9.0 7.8 20.0 26.0 38.0 38.0 37.0 Maximum force energy, 0℃, J nm nm nm 6.0 9.0 20.0 nm nm Puncture energy, 0℃, J nm nm nm 7.0 10.0 21.0 nm nm Maximum force energy, -30℃, J nm nm nm nm nm nm 25.0 13.0 Puncture energy, -30℃, J nm nm nm nm nm nm 27.0 15.0 HDT,℃ 103 98 51 98 104 102 103 99 CLTE, +23 / 80℃, μm / mK, MD nm nm nm 98* 93* 91* 74 75 Tiger stripes, MSE 18 15 22 8 10 5 8 13

[0304] *CLTE is evaluated at +23°C / 85°C. This data can be compared with data measured at +23°C / 80°C.

[0305] nm = not measured

[0306] As can be seen, the composition according to the invention exhibits improved impact performance in the instrumented puncture test, also at low temperatures, and has a good surface appearance with low tiger stripes. The composition of the invention is therefore suitable for automotive interior molded articles containing a mixed plastic polypropylene blend obtained from post-consumer waste in an amount of up to 40% by weight.

Claims

1. A composition suitable for automotive applications, The composition can be obtained by blending at least components (A), (B) and (C) (A) 15% to 50% by weight of a mixed plastic polypropylene blend; (B) 10 to 60 wt% of a heterophasic propylene copolymer; and (C) 5 to 25 wt% of an inorganic filler; wherein all percentages refer to the total composition, and wherein The mixed plastic polypropylene blend (A) has - a crystalline fraction (CF) content determined according to CRYSTEX QC analysis in the range of 85.0 to 96.0 wt.-%, and - a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of 4.0 to 15.0 wt.-%, wherein - the crystalline fraction (CF) has a content in the range of 1.0 to 10.0 wt.% by quantitative 13 Ethylene content (C2(CF)) determined by FT-IR spectroscopy calibrated with C-NMR spectroscopy; and - the soluble fraction (SF) has an intrinsic viscosity (iV(SF)) in the range of 0.9 to 2.1 dl / g; The heterophasic propylene copolymer (B) comprises a matrix phase and an elastomeric phase dispersed therein and has - a melt flow rate MFR2, measured in accordance with ISO 1133 at a temperature of 230° C. under a load of 2.16 kg, of 85 to 250 g / 10 min; - a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of greater than 20.0% to 30.0% by weight, and - an intrinsic viscosity (iV(SF)) of the soluble fraction, measured in decalin at 135° C. in accordance with DIN ISO 1628 / 1, of from 2.0 to 4.5 dl / g; The composition has - melt flow rate MFR2, measured to ISO 1133 at a temperature of 230° C. under a load of 2.16 kg, of 20 to 60 g / 10 min.

2. The composition according to claim 1, wherein the composition is obtainable by blending components (A), (B), (C) and one or more of the following components (D) 0 to 25 wt% of a second heterophasic propylene copolymer; (E) 0 to 10 wt% high density polyethylene; (F) 0 to 20 weight percent ethylene-based plastomer; wherein all percentages refer to the total composition, and wherein The second heterophasic propylene copolymer (D) comprises a matrix phase and an elastomeric phase dispersed therein and has - a melt flow rate MFR2, measured in accordance with ISO 1133 at a temperature of 230° C. under a load of 2.16 kg, of 8 to 25 g / 10 min; - a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of 12.5 to 30.0 wt.-%; and - an intrinsic viscosity iV(SF) of the soluble fraction, measured in decalin at 135° C. in accordance with DIN ISO 1628 / 1, in the range of 2.3 dl / g to 6.0 dl / g; The high-density polyethylene (E) has - a melt flow rate MFR2, measured according to ISO 1133 at a temperature of 190° C. under a load of 2.16 kg, of 0.5 to 30.0 g / 10 min; and -945 to 965 kg / m 3 density; and The ethylene-based plastomer is a copolymer of ethylene and a comonomer unit selected from α-olefins having 3 to 12 carbon atoms, and the ethylene-based plastomer has - a melt flow rate MFR2, measured according to ISO 1133 at a temperature of 190° C. under a load of 2.16 kg, of 0.2 to 2.5 g / 10 min; and -850 to 870 kg / m 3 density.

3. The composition according to claim 2, wherein the composition can be prepared by blending components (A), (B), (C) and (F) is obtained, (D) and (E) are not present, (A) 15% to 35% by weight of a mixed plastic polypropylene blend; (B) 30 to 60 wt% of a first heterophasic propylene copolymer; (C) 5 to 25 wt% of an inorganic filler; and (F) 5 to 20 weight percent of an ethylene-based plastomer; All percentages therein refer to the total composition.

4. The composition according to claim 2, wherein the composition can be prepared by blending components (A), (B), (C), (E) and (F) are obtained, (D) is not present, (A) 25% to 50% by weight of a mixed plastic polypropylene blend; (B) 20 to 50 wt% of a first heterophasic propylene copolymer; (C) 5 to 25 wt% of an inorganic filler; (E) 2 to 10 weight percent high-density polyethylene; and (F) 2 to 20 weight percent of an ethylene-based plastomer; All percentages therein refer to the total composition.

5. The composition according to claim 2, wherein the composition can be prepared by blending components (A), (B), (C), (D) and (E) are obtained, (F) is not present, (A) 25% to 50% by weight of a mixed plastic polypropylene blend; (B) 15 to 30 wt% of a first heterophasic propylene copolymer; (C) 5 to 25 wt% of an inorganic filler; (D) 5 to 25 wt% of a second heterophasic propylene copolymer; and (E) 2 to 10 weight percent high-density polyethylene; All percentages therein refer to the total composition.

6. The composition according to any one of claims 1 to 5, wherein the inorganic filler (C) is talc, having - Median particle size d before compounding of 0.3 to 30.0 microns 50 and / or - Top cut particle size d before compounding of 1.0 to 50.0 microns 95 .

7. The composition according to any one of claims 1 to 5, wherein the composition has - a crystalline fraction (CF) content, determined according to CRYSTEX QC analysis, in the range of 60.0 to 90.0 wt.-%, and - a soluble fraction (SF) content determined according to CRYSTEX QC analysis in the range of 10.0 to 40.0 wt.-%, wherein - the crystalline fraction (CF) has a content in the range of 4.0 to 15.0 wt.% by quantitative 13 Ethylene content (C2(CF)) determined by FT-IR spectroscopy calibrated with C-NMR spectroscopy; and / or - the crystalline fraction (CF) has an intrinsic viscosity (iV(CF)) of less than 1.8 dl / g; and / or - the soluble fraction (SF) has a content in the range of 28.0 to 65.0 wt. % by quantitative 13 Ethylene content (C2(SF)) determined by FT-IR spectroscopy calibrated with C-NMR spectroscopy; and - the soluble fraction (SF) has an intrinsic viscosity (iV(SF)) greater than 1.7 dl / g.

8. The composition of any one of claims 1 to 5, wherein the composition has a flexural modulus of 1500 MPa to 2200 MPa.

9. The composition according to any one of claims 1 to 5, wherein the composition has a 5.0 kJ / m 2 Up to 50.0kJ / m 2 Charpy notched impact strength at 23°C.

10. The composition according to any one of claims 1 to 5, wherein the composition has a heat distortion temperature of at least 95°C, measured according to ISO 75B, and / or a coefficient of linear thermal expansion (CLTE) of 60 to 125 μm / mK.

11. The composition according to any one of claims 1 to 5, wherein the composition has a puncture energy of 12 to 65 J and / or a maximum force energy of 10 to 60 J when measured in an instrumented drop weight test according to ISO 6603-2 at 23°C.

12. An article comprising the composition according to any one of claims 1 to 11.

13. The article of claim 12, wherein the composition has an MSE surface quality of less than 15.

14. Use of the composition according to any one of claims 1 to 11 for injection molding of articles.

Citation Information

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