CN114555692A

CN114555692A - Polypropylene composition for extrusion as a laminated film for automotive interior articles

Info

Publication number: CN114555692A
Application number: CN201980100676.9A
Authority: CN
Inventors: 周信; 张怡; 赵品麟
Original assignee: Borouge Compounding Shanghai Co ltd
Current assignee: Borouge Compounding Shanghai Co ltd
Priority date: 2019-09-30
Filing date: 2019-09-30
Publication date: 2022-05-27
Also published as: WO2021062620A1

Abstract

The present invention relates to a polypropylene composition comprising a propylene random copolymer and an elastomeric ethylene random copolymer, a film comprising said polypropylene composition and an injection moulded polypropylene article laminated from said film.

Description

Polypropylene composition for extrusion as a laminated film for automotive interior articles

Technical Field

Background

Polypropylene is one of the main polymeric materials used in the manufacture of automotive parts due to its good mechanical properties, including a balance of stiffness and impact strength. Due to the high degree of complexity available on a large scale, these automotive parts are typically obtained by injection molding. While polypropylene is the polymer of choice for automotive exterior and interior parts, the properties of most polypropylene grades need to be improved for injection molded interior articles, since the surface properties and appearance of these articles are critical. Because of the rheological properties of polypropylene, unstable flow during injection molding can lead to surface appearance defects such as tiger stripes, gloss variation, and gate blush.

While overcoming these disadvantages has long been the goal of the polypropylene development art, it is difficult to properly adjust the rheological properties without adversely affecting the mechanical properties of the article.

Disclosure of Invention

The discovery of the present invention is that polypropylene compositions can be used to produce films for injection-molded polypropylene articles, avoiding undesirable aesthetic defects without affecting the critical mechanical properties of the article.

The present invention therefore relates to a Polypropylene Composition (PC) comprising:

a)60 to 90 wt% of a propylene random copolymer (R-PP) having propylene monomer units and one or more comonomer units selected from ethylene and/or an alpha-olefin having 4 to 12 carbon atoms, wherein

i) Melt flow Rate MFR₂(230 ℃, 2.16kg, ISO 1133) is in the range of 0.1 to 15.0g/10min, and

ii) Vicat softening temperature, method A in the range from 110 to 140 ℃ (ISO306),

b)5 to 35 wt% of an elastomeric ethylene random copolymer (E) having ethylene monomer units and one or more comonomer units selected from alpha-olefins having 4 to 12 carbon atoms,

wherein the melting temperature (ISO 11357) is at least 75 ℃,

c)0 to 5% by weight of an additive (A),

wherein the weight% given for each component is relative to the total weight of the polypropylene composition and the melt flow rate MFR of the polypropylene composition₂(230 ℃, 2.16kg, ISO 1133) is in the range of 1.0 to 5.0g/10 min.

In a preferred embodiment, the propylene random copolymer (R-PP) has a free radical weight in the range of from 2 to 5% by weight¹³A content of comonomer units selected from ethylene and/or alpha-olefins having from 4 to 12 carbon atoms, as determined by C-NMR spectroscopy.

In a preferred embodiment, the elastomeric ethylene random copolymer (E) has a free-running weight in the range of from 30 to 50% by weight¹³A content of comonomer units selected from alpha-olefins having from 4 to 12 carbon atoms, as determined by C-NMR spectroscopy.

In a preferred embodiment the combined content of (R-PP), (E) and (a) in the Propylene Composition (PC) is at least 90 wt%, preferably at least 95 wt%, most preferably the Propylene Composition (PC) consists of (R-PP), (E) and (a).

In a preferred embodiment, the ratio of the content of propylene random copolymer (R-PP) to the content of elastomeric ethylene random copolymer (E) in the Polypropylene Composition (PC) (R-PP)/(E) is in the range of 2 to 5.

In another preferred embodiment the Polypropylene Composition (PC) has a melting temperature (ISO 11357) in the range of 110 to 125 ℃, more preferably in the range of 112 to 120 ℃.

In another preferred embodiment the Polypropylene Composition (PC) has a vicat softening temperature, method a (ISO306), in the range of 85 to 105 ℃.

In another preferred embodiment, the propylene random copolymer (R-PP) consists of propylene monomer units and ethylene comonomer units.

In another preferred embodiment, the propylene random copolymer (R-PP) has a flexural modulus (ISO 527) of at least 800 MPa.

In another preferred embodiment, the elastomeric ethylene random copolymer (E) has a melt flow rate MFR in the range of from 0.1 to 2.0g/10min₂(190℃，2.16kg，ISO 1133)。

In another preferred embodiment, the elastomeric ethylene random copolymer (E) consists of ethylene monomer units and 1-octene comonomer units.

In another preferred embodiment, the additive (a) is selected from the group consisting of antioxidants, uv stabilizers, anti-scrapers, mold release agents, acid scavengers, lubricants, antistatic agents and mixtures thereof.

In another preferred embodiment, the Polypropylene Composition (PC) is free of talc, preferably free of any inorganic filler.

In another aspect, the present invention relates to an article comprising, preferably consisting of, a Polypropylene Composition (PC).

In a preferred embodiment, the article is a film, preferably a cast film.

In another preferred embodiment, the film is a laminate film for a polypropylene article, preferably a polypropylene automotive article, most preferably a polypropylene automotive interior article.

In another aspect, the present invention relates to an automotive interior article comprising an injection moulded polypropylene which has been laminated with a film of the present invention, the film comprising, preferably consisting of, a Polypropylene Composition (PC).

In a further aspect, the present invention relates to the use of the film of the present invention for laminating polypropylene articles, preferably for laminating polypropylene automotive articles, most preferably for laminating polypropylene automotive interior articles.

The present invention will now be described in more detail.

Detailed Description

Propylene random copolymer (R-PP)

The main component of the Polypropylene Composition (PC) of the present invention is a propylene random copolymer (R-PP).

In the context of the present invention, the term propylene random copolymer is understood to exclude heterophasic propylene copolymers. That is, the propylene random copolymer (R-PP) of the present invention is a single-phase propylene random copolymer.

The propylene random copolymer (R-PP) of the present invention comprises propylene monomer units and one or more comonomer units selected from ethylene and/or alpha-olefins having from 4 to 12 carbon atoms, the one or more comonomer unitsQuantitative analysis of body unit¹³The amount determined by C-NMR spectroscopy is preferably in the range of 2 to 5 wt.%, more preferably in the range of 2.0 to 5.0 wt.%, still more preferably in the range of 3.0 to 4.5 wt.%, most preferably in the range of 3.5 to 4.5 wt.%.

Preferably, the propylene random copolymer (R-PP) of the present invention comprises propylene monomer units and ethylene comonomer units, the ethylene comonomer units being quantitatively determined¹³The amount determined by C-NMR spectroscopy is in the range of 2 to 5 wt.%, preferably in the range of 2.0 to 5.0 wt.%, more preferably in the range of 3.0 to 4.5 wt.%, most preferably in the range of 3.5 to 4.5 wt.%.

It is further preferred that the propylene random copolymer (R-PP) of the present invention consists of propylene monomer units and ethylene comonomer units, the ethylene comonomer units being quantitatively determined¹³The amount determined by C-NMR spectroscopy is in the range of 2 to 5 wt.%, preferably in the range of 2.0 to 5.0 wt.%, more preferably in the range of 3.0 to 4.5 wt.%, most preferably in the range of 3.5 to 4.5 wt.%.

Melt flow Rate MFR of the propylene random copolymer (R-PP) of the present invention₂(230 ℃, 2.16kg, ISO 1133) is in the range of 0.1 to 15.0g/10min, preferably in the range of 0.5 to 10.0g/10min, more preferably in the range of 0.8 to 5.0g/10min, most preferably in the range of 1.0 to 3.0g/10 min.

The vicat softening temperature of the propylene random copolymer (R-PP) of the present invention, method a (ISO306), is in the range of 110 to 140 ℃, preferably in the range of 112 to 135 ℃, more preferably in the range of 114 to 130 ℃, most preferably in the range of 115 to 125 ℃.

Preferably, the propylene random copolymer (R-PP) of the present invention has a flexural modulus (ISO 527) of at least 800MPa, preferably at least 825MPa, more preferably at least 850MPa, most preferably at least 875 MPa.

The flexural modulus is generally not more than 1400 MPa.

It is therefore preferred that the propylene random copolymer (R-PP) of the present invention has a flexural modulus (ISO 527) in the range of 800 to 1400MPa, preferably in the range of 825 to 1300MPa, more preferably in the range of 850 to 1200MPa, most preferably in the range of 875 to 1100 MPa.

Preferably, the polypropylene random copolymer (R-PP) has a xylene cold soluble content (XCS) measured according to ISO 16152(25 ℃) in the range of 2 to 15 wt. -%, preferably in the range of 3 to 10 wt. -%.

The propylene random copolymer (R-PP) of the present invention may be synthesized or selected from commercially available propylene random copolymers.

Elastomeric ethylene random copolymer (E)

As a further essential component, the Polypropylene Composition (PC) comprises an elastomeric ethylene random copolymer (E).

The elastomeric ethylene random copolymer (E) of the present invention comprises ethylene monomer units and one or more comonomer units in an amount in the range of from 30 to 50 wt%, wherein the one or more comonomer units are selected from alpha-olefins having from 4 to 12 carbon atoms, more preferably from 1-hexene and 1-octene, most preferably 1-octene.

It is preferred that the elastomeric ethylene random copolymer (E) of the present invention consists of ethylene monomer units and 1-octene comonomer units.

The comonomer units of the elastomeric ethylene random copolymer (E) are preferably present in the range of from 30 to 50% by weight, more preferably in the range of from 35 to 45% by weight, of¹³C-NMR spectroscopy.

The elastomeric ethylene random copolymer (E) of the present invention has a melting temperature (ISO 11357) of at least 75 ℃, preferably at least 90 ℃, more preferably at least 100 ℃, most preferably at least 110 ℃.

The elastomeric ethylene random copolymer (E) of the present invention preferably has a molecular weight of 860 to 890kg/m³In the range of 862 to 880kg/m, more preferably³In the range of 865 to 875kg/m, most preferably³Density within the range.

The elastomeric ethylene random copolymer (E) of the present invention preferably has a melt flow rate MFR in the range of from 0.1 to 2.0g/10min, more preferably in the range of from 0.2 to 1.5g/10min, most preferably in the range of from 0.3 to 1.0g/10min₂(190℃，2.16kg，ISO 1133)。

The elastomeric ethylene random copolymer (E) of the present invention may be selected from commercially available elastomeric ethylene random copolymers or synthesized directly, preferably the elastomeric ethylene random copolymer (E) is a commercially available elastomeric ethylene random copolymer.

In a particularly preferred embodiment, the elastomeric ethylene random copolymer (E) is the commercial product Engage available from the Dow Chemical Company (USA)^TM XLT 8677。

Additive (A)

The Polypropylene Composition (PC) of the present invention may contain the additive (a) in an amount of 0 to 5.0 wt%. The skilled practitioner is able to select suitable additives known in the art.

The additive (a) is preferably selected from the group consisting of antioxidants, uv stabilizers, anti-scratch agents, mold release agents, acid scavengers, lubricants, antistatic agents and mixtures thereof.

The skilled practitioner will recognize that talc may be used in similar compositions as a nucleating agent or as an inorganic filler. If talc is present in the Polypropylene Composition (PC) of the invention, the talc must only be present in an amount suitable for its use as nucleating agent, suitably less than 1.0 wt%, more preferably less than 0.5 wt%, most preferably less than 0.3 wt%.

It is preferred that the Polypropylene Composition (PC) is free of talc, more preferably free of any type of inorganic filler.

It is understood that the content of additive (a) given with respect to the total weight of the Polypropylene Composition (PC) includes any carrier polymer used for introducing additives into said Polypropylene Composition (PC), i.e. a masterbatch carrier polymer. An example of such a carrier polymer may be a polypropylene homopolymer in powder form.

Polypropylene Composition (PC)

It is desirable that the polypropylene composition of the present invention has properties suitable for use as a laminate film for injection molded polypropylene articles. Important properties are those required for extrusion into a film (melt flow rate and softness) and for lamination (melt temperature).

Thus, the Polypropylene Composition (PC) of the present invention has a melt flow rate MFR in the range of 1.0 to 5.0g/10min, preferably in the range of 1.1 to 4.0g/10min, more preferably in the range of 1.2 to 3.0g/10min, most preferably in the range of 1.3 to 2.0g/10min₂(230℃，2.16kg，ISO 1133)。

The Polypropylene Composition (PC) of the present invention preferably has a melting temperature (ISO 11357) in the range of 110 to 125 ℃, more preferably in the range of 111 to 122 ℃, most preferably in the range of 112 to 120 ℃.

The Polypropylene Composition (PC) of the present invention preferably has a vicat softening temperature, method a (ISO306), in the range of 85 to 105 ℃, more preferably in the range of 88 to 102 ℃, most preferably in the range of 90 to 100 ℃.

The Polypropylene Composition (PC) of the present invention comprises several essential components including a propylene random copolymer (R-PP), an elastomeric ethylene random copolymer (E) and optionally additives (a). Thus, the Polypropylene Composition (PC) comprises:

ii) Vicat softening temperature, method A (ISO306) in the range from 110 to 140 ℃,

wherein the melting temperature (ISO 11357) is at least 75 ℃,

c)0 to 5% by weight of additive (A).

The propylene random copolymer (R-PP) preferably has a free-running weight in the range from 2 to 5% by weight¹³The content of comonomer units selected from the group consisting of comonomer units as determined by C-NMR spectroscopyEthylene and/or an alpha-olefin having from 4 to 12 carbon atoms.

The elastomeric ethylene random copolymer (E) preferably has a free-running weight in the range from 30 to 50% by weight¹³A content of comonomer units selected from alpha-olefins having from 4 to 12 carbon atoms as determined by C-NMR spectroscopy.

The Polypropylene Composition (PC) of the present invention may comprise further components in addition to the essential components as defined above. However, it is preferred that the respective contents of the propylene random copolymer (R-PP), the elastomeric ethylene random copolymer (E) and the additive (a) sum up to at least 90 wt. -%, more preferably to at least 95 wt. -%, based on the total weight of the Polypropylene Composition (PC). Most preferably the Polypropylene Composition (PC) consists of (R-PP), (E) and (A) only.

As mentioned above, it is preferred that the Polypropylene Composition (PC) is free of talc, more preferably free of any type of inorganic filler.

The Polypropylene Composition (PC) comprises:

a)60 to 90% by weight of a propylene random copolymer (R-PP)

b)5 to 35% by weight of an elastomeric ethylene random copolymer (E)

c)0 to 5% by weight of additive (A).

The content of the propylene random copolymer (R-PP) in the Polypropylene Composition (PC) is 60 to 90 wt. -%, more preferably 63 to 85 wt. -%, most preferably 65 to 80 wt. -%.

The elastomeric ethylene random copolymer (E) is present in the Polypropylene Composition (PC) in an amount of from 5 to 35 wt%, more preferably from 10 to 33 wt%, most preferably from 15 to 30 wt%.

Thus, it is preferred that the Polypropylene Composition (PC) comprises:

a)63 to 85% by weight of a propylene random copolymer (R-PP)

b)10 to 33% by weight of an elastomeric ethylene random copolymer (E)

c)0 to 5% by weight of additive (A).

It is further preferred that the Polypropylene Composition (PC) comprises:

a)65 to 80% by weight of a propylene random copolymer (R-PP)

b)15 to 30 wt% of an elastomeric ethylene random copolymer (E)

c)0 to 5% by weight of additive (A).

Preferably, the ratio of the content of propylene random copolymer (R-PP) to the content of elastomeric ethylene random copolymer (E), (R-PP)/(E), is in the range of 2 to 5, more preferably in the range of 2.0 to 5.0, most preferably in the range of 2.0 to 4.0.

The preparation and further processing of the Polypropylene Composition (PC) comprises mixing the individual components of the Polypropylene Composition (PC), for example by using conventional compounding or blending equipment, such as a Banbury mixer, a two-roll rubber mill, a Buss-co-kneader (Buss-co-kneader) or a twin-screw extruder, followed by granulation. Typical extrusion temperatures are in the range of 160 to 210 ℃ or more preferably in the range of 180 to 200 ℃. From the pellets of the Polypropylene Composition (PC) films, preferably cast films, multilayer or monolayer films, can be prepared.

Preparation process for propylene random copolymer (R-PP)

The polymerization system for the preparation of the propylene random copolymer (R-PP) may comprise one or more conventional stirred slurry reactors and/or one or more gas phase reactors. Preferably, the reactor used is selected from the group of loop and gas phase reactors, and in particular, the process uses at least one loop reactor. It is also possible to use a plurality of reactors of each type, for example one loop reactor and two or three gas phase reactors in series, or two loop reactors and one or two gas phase reactors in series.

Preferably, the process further comprises a prepolymerization with a selected catalyst system comprising a ziegler-natta procatalyst, an external donor and a cocatalyst as described in detail below.

In a preferred embodiment, the prepolymerization is carried out as a bulk slurry polymerization in liquid propylene, i.e. the liquid phase comprises mainly propylene in which minor amounts of other reactants and optionally inert components are dissolved.

The prepolymerization is generally carried out at a temperature of from 0 to 50 ℃, preferably from 10 to 45 ℃, and more preferably from 15 to 40 ℃.

The pressure in the prepolymerization reactor is not critical but must be high enough to maintain the reaction mixture in the liquid phase. Thus, the pressure may be 20 to 100 bar, for example 30 to 70 bar.

The catalyst components are preferably introduced entirely into the prepolymerization step. However, in case the solid catalyst component (i) and the cocatalyst (ii) may be fed separately, only a part of the cocatalyst may be introduced into the prepolymerization stage and the remaining part into the subsequent polymerization stage. Also, in this case, it is necessary to introduce a large amount of co-catalyst in the prepolymerization stage to obtain sufficient polymerization therein.

Other components may also be added during the prepolymerization stage. Thus, hydrogen may be added during the prepolymerization stage to control the molecular weight of the prepolymer, as is known in the art. In addition, antistatic additives may be used to prevent particles from adhering to each other or to the reactor walls.

Precise control of the prepolymerization conditions and the reaction parameters is within the skill of the art.

Slurry reactor refers to any reactor operating in bulk or slurry and in which the polymer is formed in particulate form, such as a continuous or simple batch stirred tank reactor or a loop reactor. "bulk" refers to polymerization in a reaction medium comprising at least 60 weight percent monomer. According to a preferred embodiment, the slurry reactor comprises a bulk loop reactor.

By "gas phase reactor" is meant any mechanically mixed or fluidized bed reactor. Preferably, the gas phase reactor comprises a mechanically stirred fluidized bed reactor with a gas velocity of at least 0.2 m/s.

A preferred multistage process is a slurry-gas phase process, such as developed by Borealis and referred to as

The technology is provided. In this respect, reference is made to EP 0887379A 1, WO 92/12182, WO 2004/000899, WO 2004/111095, WO 99/24478, WO 99/24479 and WO 00/68315. Which are incorporated herein by reference.

Other suitable slurry-gas phase processes are Basell

And (5) processing.

Preferably, the propylene random copolymer (R-PP) according to the invention is preferably in

Or at

-PP process by using a specific Ziegler-Natta procatalyst in combination with a specific external donor, as described in detail below.

Thus, a preferred multi-stage process may comprise the steps of:

-producing a propylene random copolymer (R-PP) in a first slurry reactor and optionally in a second slurry reactor in the presence of a selected catalyst system comprising a specific Ziegler-Natta procatalyst (i), an external donor (iii) and a cocatalyst (ii), as for example described in detail below, both slurry reactors using the same polymerization conditions,

optionally transferring the slurry reactor product into at least one first gas phase reactor, such as one gas phase reactor or a first gas phase reactor and a second gas phase reactor connected in series,

-recovering the polymer product for further processing.

With respect to the preferred slurry or slurry-gas phase processes described above, the following general information regarding the process conditions can be provided.

The temperature is preferably from 40 to 110 ℃, preferably between 50 and 100 ℃, in particular between 60 and 90 ℃, and the pressure is in the range from 20 to 80 bar, preferably in the range from 30 to 60 bar, hydrogen being optionally added in order to control the molecular weight in a manner known per se.

The reaction product of the slurry polymerization, preferably carried out in a loop reactor, is optionally transferred to a subsequent gas phase reactor or reactors, wherein the temperature is preferably in the range of from 50 to 130 ℃, more preferably in the range of from 60 ℃ to 100 ℃ and the pressure is in the range of from 5 to 50 bar, preferably in the range of from 8 to 35 bar, optionally also with the addition of hydrogen in order to control the molecular weight in a manner known per se.

The average residence time in the above reactor zones may vary. In one embodiment, the average residence time in the slurry reactor (e.g. loop reactor) is in the range of 0.5 to 5 hours, e.g. in the range of 0.5 to 2 hours, while the average residence time in the gas phase reactor is typically 1 to 8 hours.

If desired, the polymerization can be carried out under supercritical conditions in a known manner in a slurry reactor, preferably a loop reactor, and/or in condensed mode in a gas phase reactor.

According to the present invention, the random propylene copolymer (R-PP) is obtained by a polymerization process as described above in the presence of a catalyst system comprising as component (i) a ziegler-natta procatalyst comprising the transesterification reaction product of a lower alcohol and a phthalate.

The procatalyst used according to the invention is prepared by the following process

a) Making MgCl₂And C₁-C₂Spray-or emulsion-solidified adducts of alcohols with TiCl₄Reaction of

b) At the C₁To C₂Reacting the product of stage a) with a dialkyl phthalate of formula (I) under conditions such that a transesterification reaction between an alcohol and the dialkyl phthalate of formula (I) takes place to form an internal donor,

wherein R is^1’And R^2’Independently at least C₅An alkyl group, a carboxyl group,

c) washing the product of stage b), or

d) Optionally reacting withThe product of step c) is reacted with additional TiCl₄And (4) reacting.

The procatalyst is produced as defined, for example, in patent applications WO 87/07620, WO 92/19653, WO 92/19658 and EP 0491566. The contents of these documents are incorporated herein by reference.

First forming MgCl₂And C₁-C₂Adducts of alcohols of the formula MgCl₂nROH, wherein R is methyl or ethyl and n is 1 to 6. Ethanol is preferably used as the alcohol.

The adduct, which is first melted and then spray crystallized or emulsion solidified, is used as a catalyst support.

In the next step, MgCl₂Spray-or emulsion-solidified adducts of nROH (wherein R is methyl or ethyl, preferably ethyl, and n is 1 to 6) with TiCl₄Contacting to form a titanized support, followed by the steps of:

adding to the titanized support the following compounds to form a first product,

(i) a dialkyl phthalate of the formula (I) wherein R^1’And R^2’Independently is at least C₅Alkyl radicals, e.g. at least C₈-an alkyl group,

or preferably

(ii) A dialkyl phthalate of the formula (I) wherein R^1’And R^2’Are identical and are at least C₅Alkyl radicals, e.g. at least C₈-an alkyl group,

or more preferably

(iii) A dialkyl phthalate of formula (I) selected from the group consisting of propylhexyl phthalate (PrHP), dioctyl phthalate (DOP), diisodecyl phthalate (DIDP) and tricosyl phthalate (DTDP), still more preferably the dialkyl phthalate of formula (I) is dioctyl phthalate (DOP), such as diisooctyl phthalate or diethylhexyl phthalate, in particular diethylhexyl phthalate,

subjecting the first product to suitable transesterification reaction conditions, i.e. to a temperature above 100 ℃, preferably between 100 and 150 ℃, more preferably between 130 and 150 ℃, such that the methanol or ethanol transesterifies with the ester groups of the dialkyl phthalate of formula (I) to form preferably at least 80 mole%, more preferably 90 mole%, most preferably 95 mole% of dialkyl phthalate of formula (II)

Wherein R is¹And R²Is a methyl or ethyl group, preferably an ethyl group,

a dialkyl phthalate of the formula (II) as internal donor, and

recovering the transesterification reaction product as the main catalyst component (i)).

In a preferred embodiment, the compound of formula MgCl₂The adduct of nROH (where R is methyl or ethyl and n is 1 to 6) is melted and the melt is then preferably injected by gas into a cooled solvent or cooled gas to crystallize the adduct into a morphologically advantageous form as described for example in WO 87/07620. The crystalline adduct is preferably used as a catalyst support and reacted to a procatalyst useful in the present invention as described in WO 92/19658 and WO 92/19653.

When the catalyst residue is removed by extraction, an adduct of the titanized support and the internal donor is obtained in which the group originating from the ester alcohol is changed.

If sufficient titanium remains on the support, it will act as the active element of the procatalyst.

Otherwise, the titanation is repeated after the above treatment to ensure a sufficient titanium concentration to ensure activity.

Preferably, the procatalyst used according to the invention comprises at most 2.5 wt%, preferably at most 2.2 wt% and more preferably at most 2.0 wt% titanium. Its donor content is preferably between 4 and 12% by weight, and more preferably between 6 and 10% by weight.

More preferably, the procatalyst used according to the present invention has been prepared by using ethanol as alcohol and dioctyl phthalate (DOP) as dialkyl phthalate of formula (I), yielding diethyl phthalate (DEP) as internal donor compound.

In a preferred embodiment, the procatalyst is obtained by emulsion technology developed by Borealis. Reference is made in this respect to WO 2009/040201. Thus, preferably, the procatalyst is obtained by a process comprising the steps of:

a) preparing a solution of a complex of a metal of group 2 and an electron donor by reacting a compound of said metal with said electron donor or a precursor thereof in an organic liquid reaction medium;

b) adding the solution of the complex to at least one compound of a transition metal of any one of groups 4 to 6 to produce an emulsion whose dispersed phase contains more than 50 mole% of the group 2 metal in the complex;

c) optionally agitating the emulsion in the presence of an emulsion stabilizer to maintain droplets of the dispersed phase in a mean particle size range of suitably 5 to 200 μm, preferably 10 to 100 μm, even more preferably 20 to 50 μm;

d) solidifying the droplets of the dispersed phase; and

e) recovering the solidified particles of the obtained olefin polymerization catalyst.

The group 2 metal used in the preparation of the procatalyst according to the emulsion technique is preferably magnesium and the liquid organic medium used for reacting the group 2 metal compound preferably comprises C₆-C₁₀Aromatic hydrocarbons, preferably including toluene. The electron donor compound which is reacted with the group 2 metal compound is preferably a mono-or diester of an aromatic carboxylic acid or diacid, the latter being capable of forming a complex resembling a chelate structure. The aromatic carboxylic acid ester or diester may be prepared by reacting an aromatic carboxylic acid chloride or diacid chloride with C₂-C₁₆The reaction of the alkanol and/or diol is formed in situ and is preferably dioctyl phthalate or bis- (2-ethylhexyl) phthalate. The reaction for preparing the group 2 metal complex is generally carried out at a temperature of 20 to 80 ℃ andin the case where the group 2 metal is magnesium, the preparation of the magnesium complex may advantageously be carried out at a temperature of from 50 to 70 ℃. The compound of a group 4 to 6 metal is preferably a compound of a group 4 metal. The group 4 metal is preferably titanium, and the compound with which the complex of the group 2 metal reacts is preferably a halide. In still further embodiments of the present invention, the compound of a group 4 to 6 metal may also be selected from group 5 metals and group 6 metals, such as Cu, Fe, Co, Ni and/or Pd compounds. In a preferred embodiment of the process for the production of the catalyst, a Turbulence Minimizing Agent (TMA) is added to the reaction mixture before solidifying said particles of the dispersed phase, the TMA being inert and soluble in the reaction mixture under the reaction conditions. The Turbulence Minimizing Agent (TMA) or mixture thereof is preferably a polymer with a linear aliphatic carbon backbone, which may be branched with only short side chains to provide uniform flow conditions upon stirring. The TMA is particularly preferably selected from those having a molecular weight of about 1 to 40X 10⁶High molecular weight M of_wAn alpha-olefin polymer or a mixture thereof (as measured by gel permeation chromatography). Especially preferred are polymers of alpha-olefin monomers having from 6 to 20 carbon atoms, and more preferred are polyoctenamer, polynonanene, polydecene, polyundecene or polydodecene or mixtures thereof, having a molecular weight and a general backbone structure as defined before, and most preferred TMA is polydecene. In general, the turbulence minimizing agent may be added at any process step prior to the start of particle formation, i.e. at the latest before solidification of the emulsion, and is added to the emulsion in an amount of from 1 to 1000ppm, preferably from 5 to 100ppm and more preferably from 5 to 50ppm, based on the total weight of the reaction mixture. In a preferred embodiment of the invention, the procatalyst is obtained by the steps of: by including C₆-C₁₀Aromatic hydrocarbons or C₆-C₁₀Aromatic hydrocarbons and C₅-C₉C of a mixture of aliphatic hydrocarbons₆-C₁₀Reacting a magnesium alkoxide compound and an electron donor or a precursor thereof in an aromatic liquid reaction medium to prepare a solution of a magnesium complex; reacting the magnesium complex with at least one compound of a tetravalent group 4 metal at a temperature higher than 10 ℃ and lower than 60 ℃ toGenerating a higher density of TiCl-insoluble material having a group 4 metal/Mg molar ratio of 0.1 to 10 in an oil dispersed phase having a group 4 metal/Mg molar ratio of 10 to 100₄An emulsion of a dispersed oil phase of toluene; maintaining the droplets of the dispersed phase in the size range of 5 to 200 μm by stirring in the presence of an emulsion stabilizer while heating the emulsion to solidify the droplets and adding a turbulence minimizing agent to the reaction mixture prior to solidifying the droplets of the dispersed phase, the turbulence minimizing agent being inert and soluble in the reaction mixture under reaction conditions; and solidifying the particles of the dispersed phase by heating and recovering the obtained catalyst particles. Thus, the dispersed phase and the dispersed phase differ from each other in that the denser oil will not dissolve in the toluene solution of titanium tetrachloride if contacted therewith. Suitable TiCl for establishing the standard₄The toluene solution is TiCl₄A solution having a/toluene molar ratio of 0.1 to 0.3. The dispersed and dispersed phases are also distinguished in that the Mg provided for reaction with the group 4 metal compound (as a complex) is present in the dispersed phase in a large proportion, as can be seen by comparing the corresponding group 4 metal/Mg molar ratios. Thus, in practice, the reaction product of the Mg complex with the group 4 metal, which is the precursor of the final catalyst, becomes almost entirely in the dispersed phase and, through further processing steps, in the final dry particulate form. The dispersed phase, still containing an effective amount of a group 4 metal, can be reprocessed to recover the metal. The formation of a two-phase reaction product, rather than a single-phase reaction product, is promoted by carrying out the reaction of the Mg complex/group 4 metal compound at low temperatures, particularly at temperatures above 10 ℃ but below 60 ℃, preferably between 20 ℃ and 50 ℃. Since the two phases naturally tend to separate into a lower, denser phase and a lighter supernatant phase, it is necessary to maintain the reaction product as an emulsion by stirring, preferably in the presence of an emulsion stabilizer. The resulting particles from the dispersed phase of the emulsion have a certain size, shape (spherical) and homogeneity, which makes the final catalyst very effective in olefin polymerization. This morphology is retained during the heat curing of the particles, of course during the final washIs also retained during the washing and drying steps. In contrast, it is difficult or even impossible to achieve this morphology by precipitation due to the substantial uncontrollable nature of nucleation and growth and the large number of variables that affect these events. The electron donor is preferably an aromatic carboxylic acid ester, particularly preferred esters being dioctyl phthalate and bis- (2-ethylhexyl) phthalate. By reacting aromatic carboxylic acid chloride precursors with C₂-C₁₆The reaction of the alkanol and/or diol may conveniently form the donor in situ. The liquid reaction medium preferably comprises toluene. In addition, emulsifiers/emulsion stabilizers may additionally be used in a manner known in the art to facilitate the formation and/or stability of the emulsion. For the above purpose, for example, a surfactant, such as a type based on an acrylic polymer or a methacrylic polymer, may be used. Preferably, the emulsion stabilizer is an acrylic polymer or a methacrylic polymer, particularly those having medium-sized ester side chains with greater than 10, preferably greater than 12, and preferably less than 30, and preferably 12 to 20 carbon atoms. Particular preference is given to unbranched C₁₂-C₂₀Acrylates, such as poly (hexadecyl) -methacrylate and poly (octadecyl) -methacrylate. It has been found that the best results are obtained when the denser oil has a group 4 metal/Mg molar ratio of from 1 to 5, preferably from 2 to 4, and the dispersed phase oil has a group 4 metal/Mg molar ratio of from 55 to 65. Typically, the ratio of the group 4 metal/Mg molar ratio in the dispersed phase oil to the group 4 metal/Mg molar ratio of the denser oil is at least 10. The solidification of the droplets of the dispersed phase by heating is suitably carried out at a temperature of from 70 to 150 c, typically from 90 to 110 c.

The finally obtained procatalyst is desirably in the form of particles having an average particle size in the range of 5 to 200. mu.m, preferably 10 to 100. mu.m, more preferably 20 to 50 μm. The reagents may be added to the aromatic reaction medium in any order. However, it is preferred that in the first step the magnesium alkoxide compound is reacted with a carboxylic acid halide precursor of the electron donor to form an intermediate; and in a second step, the product obtained is further reacted with a group 4 metal. Each alkoxy group of the magnesium compound preferably contains 1 to 20 carbon atoms and the carboxylic acid should contain at least 8 carbon atoms. The reaction of the magnesium compound, the carboxylic acid halide and the alcohol is satisfactorily carried out at a temperature in the range of 20 to 80 c, preferably in the range of 50 to 70 c. The product of this reaction, the "magnesium complex", reacts with the group 4 metal compound at relatively low temperatures to form a two-phase oil-in-oil product. The reaction medium used as solvent may be an aromatic or a mixture of aromatic and aliphatic hydrocarbons, the latter preferably containing from 5 to 9 carbon atoms, more preferably from 5 to 7 carbon atoms, or a mixture thereof. Preferably, the liquid reaction medium used as solvent in the reaction is aromatic and more preferably selected from hydrocarbons such as substituted and unsubstituted benzene, preferably from alkylated benzenes, even more preferably from toluene and xylene, and most preferably toluene. The molar ratio of the aromatic medium to magnesium is preferably less than 10, for example from 4 to 10, preferably from 5 to 9. The alkoxy magnesium compound group is preferably selected from the group consisting of dialkoxy magnesium, a complex of magnesium dihalide and alcohol, and a complex of magnesium dihalide and dialkoxy magnesium. It may be the reaction product of an alcohol and a magnesium compound selected from the group consisting of dialkylmagnesium, alkylalkoxymagnesium, alkylmagnesium halide and magnesium dihalide.

It may also be selected from the group consisting of magnesium dialkoxides, diaryloxy magnesium, alkoxy magnesium halides, aryloxy magnesium halides, alkyl alkoxy magnesium, aryl alkoxy magnesium, and alkyl aryloxy magnesium. The magnesium dialkoxide may be the reaction product of a magnesium dihalide (such as magnesium dichloride) or a magnesium dialkyl of the formula R 'xR "yMg, where x + y ═ 2 and x and y are in the range of 0.3 to 1.7 and each of R' and R" is similar or different C₁-C₂₀Alkyl, preferably similar or different C₄-C₁₀An alkyl group. Typical alkyl magnesium are ethylbutyl magnesium, dibutyl magnesium, dipropyl magnesium, propylbutyl magnesium, diamyl magnesium, butylpentylgagnesium, butyloctyl magnesium and dioctylmagnesium. Preferably, R' is butyl and R "is octyl, i.e. the dialkylmagnesium compound is butyloctylmagnesium, most preferably the dialkylmagnesium compound is Mg [ (Bu)_1.5(Oct)_0.5]。

Magnesium dialkyl, alkyl alkoxy or dihalideMagnesium may be reacted with a polyol R (OH)_m(wherein m is in the range of 2 to 4) or a monohydric alcohol ROH or a mixture thereof. Typical C₂To C₆The polyols may be linear or branched and include ethylene glycol, propylene glycol (also known as 1, 3-propanediol), 1, 2-butanediol, 1, 3-butanediol, 1, 4-butanediol, 2, 3-butanediol, 1, 5-pentanediol, 1, 6-hexanediol, 1, 8-octanediol, pinacol, diethylene glycol, triethylene glycol, and triols such as glycerol, hydroxymethylpropane, and pentaerythritol. The aromatic reaction medium may also comprise a monohydric alcohol, which may be linear or branched. Typical C₁-C₅The monohydric alcohol is methanol, ethanol, n-propanol, isopropanol, n-butanol, isobutanol, sec-butanol, tert-butanol, n-pentanol, isopentanol, sec-pentanol, tert-pentanol, diethylmethanol, 2-methyl-1-butanol, sec-isoamyl alcohol, tert-butylmethanol. Typical C₆-C₁₀The monohydric alcohols are hexanol, 2-ethyl-1-butanol, 4-methyl-2-pentanol, 1-heptanol, 2-heptanol, 4-heptanol, 2, 4-dimethyl-3-pentanol, 1-octanol, 2-ethyl-1-hexanol, 1-nonanol, 5-nonanol, diisobutylcarbinol, 1-decanol and 2, 7-dimethyl-2-octanol. Typically, a>C₁₀The monohydric alcohol is n-1-undecanol, n-1-dodecanol, n-1-tridecanol, n-1-tetradecanol, n-1-pentadecanol, 1-hexadecanol, n-1-heptadecanol and n-1-octadecanol. The monoalcohols may be unsaturated, provided that they do not act as catalyst poisons. Preferred monoalcohols are those of the formula ROH, wherein R is C₂-C₁₆Alkyl, most preferably C₄-C₁₂Alkyl radicals, in particular 2-ethyl-1-hexanol or 1-octanol.

Preferably, substantially all of the aromatic carboxylic acid ester is the reaction product of a carboxylic acid halide, preferably a dicarboxylic acid dihalide, more preferably an unsaturated dicarboxylic acid dihalide, and most preferably phthaloyl chloride, with a monohydric alcohol.

The compound of a tetravalent group 4 metal containing a halogen is preferably a titanium tetrahalide. Equivalent to the titanium tetrahalide is a combination of an alkoxy titanium halide and a halogenating agent which is capable of forming the titanium tetrahalide in situ. The most preferred halide is chloride.

All of the peopleIt is known that the addition of at least one halogenated hydrocarbon during the main catalyst preparation process can further increase the catalytic activity. The reactive halogenated hydrocarbons are preferably of the formula R '"X')"_nWherein R' is C₁-C₂₀Hydrocarbyl, especially C₁-C₁₀An aliphatic hydrocarbon group, X' "is halogen, preferably chlorine, and n is an integer from 1 to 4.

Such chlorinated hydrocarbons include monochloromethane, dichloromethane, trichloromethane (chloroform), tetrachloromethane, monochloroethane, (1,1) -dichloroethane, (1,2) -dichloroethane, (1,1,1) -trichloroethane, (1,1,2) -tetrachloroethane, (1,1,2,2) -tetrachloroethane, pentachloroethane, hexachloroethane, 1-chloropropane, 2-chloropropane, (1,2) -dichloropropane, (1,3) -dichloropropane, (1,2,3) trichloropropane, 1-chlorobutane, 2-chlorobutane, isobutyl chloride, tert-butyl chloride, (1,4) -dichlorobutane, 1-chloropentane and (1,5) -dichloropentane. The chlorinated hydrocarbons may also be unsaturated, provided that the unsaturation does not act as a catalyst poison in the final catalyst.

In the above formula, R' ″ is preferably C₁-C₁₀Alkyl, X' "is preferably chlorine, and n is preferably 1 or 2. Preferred compounds include butyl chloride (BuCl), dichloroalkanes such as (1,4) -dichlorobutane, and tert-butyl chloride.

The catalyst preparation as described herein may be carried out batchwise, semi-continuously or continuously. In such a semi-continuous or continuous process, a solution of a complex of a group 2 metal and the electron donor, prepared by reacting a compound of the metal with the electron donor in an organic liquid reaction medium, is mixed with at least one transition metal compound, which may be dissolved in the same or a different organic liquid reaction medium. The solution thus obtained may then be stirred in the presence of an emulsion stabilizer and the stirred emulsion is then fed to a temperature gradient reactor in which the emulsion is subjected to a temperature gradient, resulting in solidification of the droplets of the dispersed phase of the emulsion. TMA is preferably contained in a solution of the complex or added to the solution prior to feeding the stirred solution to the temperature gradient reactor.

When the stirred emulsion is fed to a temperature gradient reactor, an inert solvent in which the droplets are insoluble may additionally be fed to the gradient reactor to improve the formation of droplets, resulting in a uniform particle size of the catalyst particles formed in the temperature gradient reactor when passing through the conduit. This additional solvent may be the same as the organic liquid reaction medium used to prepare the solution of the complex of the group 2 metal as explained in more detail above.

The solidified particles of catalyst can then be recovered by an in-stream filter unit and preferably washed to remove unreacted starting components.

The recovered particulate product is washed at least once, preferably at least twice, most preferably at least three times, with a hydrocarbon, preferably selected from aromatic and aliphatic hydrocarbons, preferably with toluene, in particular with hot (e.g. 90 ℃) toluene, which may comprise a small amount (preferably about 0.01 to 10 vol.%) of TiCl₄Or an alkyl aluminum chloride such as diethyl aluminum chloride (DEAC). Advantageously, the further washing step is carried out with heptane, most preferably with hot (e.g. 90 ℃) heptane, and the further washing step is carried out with pentane. The washing step typically comprises several sub-steps. For example, the preferred washing sequence is one washing step with 90 ℃ toluene, two washing steps with 90 ℃ heptane and one or two washing steps with pentane at room temperature.

Finally, the washed catalyst is dried, for example by evaporation or flushing with nitrogen.

The catalyst system used according to the invention also comprises a cocatalyst, preferably an alkylaluminum compound, as defined in detail below. In the case of the production of the procatalyst by emulsion technology, the cocatalyst is added in pure form or in solution shortly before the start of the formation of the emulsion until it is added to the wash liquor (e.g. toluene) in an amount such that the final Al content of the particles is from 0.05 to 1 wt%, preferably from 0.1 to 0.8 wt%, and most preferably from 0.2 to 0.7 wt% of the final catalyst particles. The most preferable Al content may vary depending on the type of Al compound and the addition step. For example, in some cases, the most preferred amount may be 0.1 to 0.4 weight percent.

In a further embodiment, the ziegler-natta procatalyst may be modified by polymerizing a vinyl compound in the presence of a catalyst system comprising the specific ziegler-natta procatalyst, an external donor and a cocatalyst, the vinyl compound having the formula:

CH₂＝CH-CHR³R⁴

wherein R is³And R⁴Together form a 5-or 6-membered saturated, unsaturated or aromatic ring or independently represent an alkyl group comprising 1 to 4 carbon atoms, and the modified catalyst is used for the preparation of the propylene random copolymer (R-PP) according to the present invention. The polymerized vinyl compound may act as an alpha-nucleating agent.

With regard to the modification of the catalyst, reference is made to international applications WO 99/24478, WO 99/24479, in particular WO 00/68315, which are incorporated herein by reference with regard to the reaction conditions involved in the modification of the catalyst and with regard to the polymerization reaction.

As mentioned above, for the production of the propylene random copolymer (R-PP) according to the present invention, the catalyst system used preferably comprises, as component (ii), in addition to the specific Ziegler-Natta procatalyst, an organometallic cocatalyst.

Thus, it is preferred to select the cocatalyst from the group consisting of trialkylaluminums, such as Triethylaluminum (TEA), dialkylaluminum chlorides and alkylaluminum sesquichlorides.

Component (III) of the catalyst system used is an external donor represented by formula (III)

Si(OCH₃)₂R₂ ⁵ (III)

Wherein R is⁵Represents a branched alkyl group having 3 to 12 carbon atoms, preferably a branched alkyl group having 3 to 6 carbon atoms, or a cycloalkyl group having 4 to 12 carbon atoms, preferably a cycloalkyl group having 5 to 8 carbon atoms.

It is particularly preferred that R⁵Selected from isopropyl, isobutyl, isoamyl, tert-butyl, tert-amyl, neopentylCyclopentyl, cyclohexyl, methylcyclopentyl and cycloheptyl.

More specific examples of hydrocarbyloxysilane compounds which can be used as external electron donor in the present invention are diphenyldimethoxysilane, dicyclopentyldimethoxysilane (D-donor), dicyclopentyldiethoxysilane, cyclopentylmethyldimethoxysilane, cyclopentylmethyldiethoxysilane, dicyclohexyldimethoxysilane, dicyclohexyldiethoxysilane, cyclohexylmethyldimethoxysilane (C-donor), cyclohexylmethyldiethoxysilane, methylphenyldimethoxysilane, diphenyldiethoxysilane, cyclopentyltrimethoxysilane, phenyltrimethoxysilane, cyclopentyltriethoxysilane, phenyltriethoxysilane. Most preferably, the organosilane compound is diethylamino-triethoxy-silane (U-donor), cyclohexylmethyldimethoxysilane (C-donor) or dicyclopentyldimethoxysilane (D-donor), the latter being particularly preferred.

Comprising ethylene and/or C produced by the process outlined above₄To C₁₂The properties of the propylene random copolymer of alpha-olefins (R-PP) can be adjusted and controlled using process conditions known to the person skilled in the art, for example by one or more of the following process parameters: temperature, hydrogen feed, comonomer feed, propylene feed, catalyst, type and amount of external donor, split ratio (split) between two or more components of the multimodal polymer.

Preparation of Polypropylene Composition (PC)

For mixing the individual components of the polypropylene composition of the present invention, conventional compounding or blending equipment may be used, such as a Banbury mixer, a two-roll rubber mill, a Brookfield co-kneader or a twin-screw extruder. Preferably, the mixing is accomplished in a co-rotating twin screw extruder. The polymeric material recovered from the extruder is typically in the form of pellets. These pellets are then preferably further processed, for example by compression moulding, to produce articles and products of the Polypropylene Composition (PC) of the invention.

Film(s)

The invention also relates to a film comprising the Polypropylene Composition (PC) of the invention.

Preferably, the film of the invention comprises at least 90 wt. -%, more preferably at least 95 wt. -%, yet more preferably at least 97 wt. -%, even more preferably at least 99 wt. -% of the Polypropylene Composition (PC) of the invention relative to the total weight of the film.

It is particularly preferred that the film of the invention consists of the Propylene Composition (PC) of the invention.

Preferably, the film of the present invention is a cast film.

It is particularly preferred that the film of the present invention is a laminate film for a polypropylene article, preferably a polypropylene automotive article, most preferably a polypropylene automotive interior article.

The term interior trim denotes that the article is not part of the exterior of an automobile, but part of the interior of an automobile. Preferred automotive interior articles include door modules, seat structures, armrests, pedals, dashboards, and interior trim.

The invention therefore also relates to an automotive interior article comprising injection-moulded polypropylene which has been laminated with a film according to the invention, the film comprising, preferably consisting of, a Polypropylene Composition (PC).

The laminated automotive interior trim article according to the present invention will be free of typical aesthetic defects typically associated with injection molding processes, such as tiger stripes, gloss differential, and the like.

Another aspect of the invention is the use of a film according to the invention for laminating a polypropylene article, preferably for laminating a polypropylene automotive article, most preferably for laminating a polypropylene automotive interior article.

Preferably, the films of the present invention are used for laminating injection molded polypropylene articles, more preferably injection molded polypropylene automotive articles, most preferably injection molded polypropylene automotive interior articles.

The use of the films of the present invention in the lamination of injection molded articles helps to avoid the adverse aesthetic defects typically associated with injection molding processes, such as tiger stripes, gloss differences, and the like.

The present invention will now be described in more detail by way of the examples provided below. It will be clear to the skilled practitioner that the following examples are illustrative only and do not pose any further limitations to the invention described above.

Examples

1. Defining/measuring method

The following definitions of terms and assay methods apply, unless otherwise defined, to the above general description of the invention as well as to the examples below.

The density was measured according to ISO 1183-187. Sample preparation was done by compression molding according to ISO 1872-2: 2007.

Melting temperature T_mMeasured according to ISO 11357-3.

MFR₂Measured according to ISO 1133(230 ℃, 2.16kg load).

Quantification of comonomer content by FTIR spectroscopy

Comonomer content is determined by quantitative determination in a manner well known in the art¹³C Nuclear Magnetic Resonance (NMR) spectroscopy quantitative fourier transform infrared spectroscopy (FTIR) measurements were performed after basic partition calibration. The film was pressed to a thickness between 100 and 500 μm and the spectrum was recorded in transmission mode.

In particular, use is made of a mixture of 720 to 722 and 730 to 733cm^-1The baseline corrected peak area of the quantitative band found at (a) was used to determine the ethylene content of the polypropylene-co-ethylene copolymer. Quantitative results were obtained on the basis of the reference film thickness.

Xylene solubles (XCS, wt%): the content of Xylene Cold Soluble (XCS) is according to ISO 16152; a first edition; 2005-07-01 was measured at 25 ℃.

Vicat softening temperature: the Vicat softening temperature is determined according to ISO306, method A.

2. Examples of the embodiments

2.1 Synthesis of propylene random copolymer (R-PP)

The catalyst used for the preparation of R-PP is a self-supported Ziegler-Natta catalyst described in WO 2004/029112; triethylaluminum (TEAL) was used as cocatalyst and dicyclopentyldimethoxysilane as donor. R-PP is polymerized in a sequential reactor process as described in table 1:

table 1: preparation of propylene random copolymer (R-PP) by sequential polymerization:

2.2 compounding of examples

The propylene compositions of inventive examples IE1 to IE3 and comparative example CE1 were prepared by compounding in a co-rotating twin-screw extruder under the conditions described in table 3 based on the formulations shown in table 2.

Table 2: formulations used in inventive and comparative examples and their properties.

Components	Unit of	CE1	IE1	IE2	IE3
						HomoPP	By weight%	98
R-PP	By weight%		78	73	68
						Engage^TM XLT 8677	By weight%		20	25	30
PP-H,GD,225	By weight%	1.0	1.0	1.0	1.0
						Irgafos 168	By weight%	0.2	0.2	0.2	0.2
Irganox 1076	By weight%	0.2	0.2	0.2	0.2
						CaSt	By weight%	0.3	0.3	0.3	0.3
Rikemal AS-105	By weight%	0.3	0.3	0.3	0.3
						General assembly	By weight%	100	100	100	100
Physical Properties of the PP composition Compound of the invention obtained
						MFR₂(230℃)	g/10min	25	1.5	1.4	1.3
Melting temperature	℃	168	118	116	114
						Vicat softening temperature, method A	℃	145	100	95	90

HomopP propylene homopolymer, available under the trade designation "HG 385 MO", is commercially available from Borough Pte Co

Engage^TMXLT 8677 ethylene/1-octene elastomer having a density of 870kg/m³Melt flow Rate MFR₂(190 ℃, 2.16kg) was 0.50g/10min and the melting temperature was 118 ℃. Engage^TMXLT 8677 is commercially available from the Dow Chemical Company (US)

A propylene homopolymer carrier in the form of a PP-H, GD 225 powder, having a melting temperature of 160 ℃;

tris (2, 4-di-tert-butylphenyl) phosphite from Irgafos 168 BASF SE (CAS number 31570-04-4) having a melting temperature of 182 ℃

Irganox 1076 BASF SE octadecyl 3- (3, 5-di-tert-butyl-4-hydroxyphenyl) propionate (CAS number 2082-79-3), having a melting temperature of 50 ℃;

CaSt calcium stearate, CAS No. 1592-23-0, commercially available from Faci

Rikemal AS-105 glyceryl monostearate, CAS number 31566-31-1, commercially available from Riken Vitamin

Table 3: conditions for compounding the propylene compositions of the present invention

As can be seen from the examples, the polypropylene compositions according to the invention have very excellent properties for forming laminated films, wherein the Vicat A temperature and the melt flow rate are much lower and the melting temperature is much higher than room temperature in the range required for film extrusion, suitable for laminating automotive interiors. Lamination using such films for injection molded automotive interior articles is expected to reduce the occurrence of aesthetic defects typically associated with injection molded articles.

Claims

1. A Polypropylene Composition (PC) comprising

wherein the melting temperature (ISO 11357) is at least 75 ℃,

c)0 to 5% by weight of an additive (A),

2. According to the rightThe Polypropylene Composition (PC) of claim 1, wherein the propylene random copolymer (R-PP) has a basis weight in the range of 2 to 5 wt. -%¹³A content of comonomer units selected from ethylene and/or alpha-olefins having from 4 to 12 carbon atoms, as determined by C-NMR spectroscopy.

3. The Polypropylene Composition (PC) according to claim 1 or 2, wherein the elastomeric ethylene random copolymer (E) has a basis weight in the range of from 30 to 50 wt. -%¹³A content of comonomer units selected from alpha-olefins having from 4 to 12 carbon atoms as determined by C-NMR spectroscopy.

4. Polypropylene Composition (PC) according to any one of the preceding claims, wherein the combined content of (R-PP), (E) and (a) is at least 90 wt%, preferably at least 95 wt%, most preferably the Propylene Composition (PC) consists of (R-PP), (E) and (a).

5. Polypropylene Composition (PC) according to anyone of the preceding claims, wherein the ratio of the content of the propylene random copolymer (R-PP) to the content of the elastomeric ethylene random copolymer (E) (R-PP)/(E) is in the range of 2 to 5.

6. Polypropylene Composition (PC) according to any of the preceding claims having a melting temperature (ISO 11357) in the range of 110 to 125 ℃, more preferably in the range of 112 to 120 ℃.

7. Polypropylene Composition (PC) according to any of the preceding claims having a vicat softening temperature, method a (ISO306), in the range of from 85 to 105 ℃.

8. Polypropylene Composition (PC) according to any of the preceding claims, wherein the propylene random copolymer (R-PP) consists of propylene monomer units and ethylene comonomer units.

9. Polypropylene Composition (PC) according to any of the preceding claims, wherein the propylene random copolymer (R-PP) has a flexural modulus (ISO 527) of at least 800 MPa.

10. The Polypropylene Composition (PC) according to any one of the preceding claims, wherein the elastomeric ethylene random copolymer (E) has a melt flow rate MFR in the range of from 0.1 to 2.0g/10min₂(190℃，2.16kg，ISO1133)。

11. The Polypropylene Composition (PC) according to any one of the preceding claims, wherein the elastomeric ethylene random copolymer (E) consists of ethylene monomer units and 1-octene comonomer units.

12. Polypropylene Composition (PC) according to any of the preceding claims, wherein the additive (a) is selected from antioxidants, uv stabilizers, anti-scratch agents, mold release agents, lubricants, antistatic agents, acid scavengers and mixtures thereof.

13. Polypropylene Composition (PC) according to any of the preceding claims, which is free of talc, preferably free of any inorganic filler.

14. A film comprising, preferably consisting of, preferably being a cast film, a Polypropylene Composition (PC) according to any of the preceding claims.

15. The film according to claim 14, wherein the film is a laminate film for a polypropylene article, preferably a polypropylene automotive article, most preferably a polypropylene automotive interior article.

16. Automotive interior article comprising an injection moulded polypropylene article which has been laminated with a film according to claims 14 to 15, said film comprising, preferably consisting of, a Polypropylene Composition (PC) according to claims 1 to 13.

17. Use of a film according to claims 14 to 15 for laminating a polypropylene article, preferably for laminating a polypropylene automotive article, most preferably for laminating a polypropylene automotive interior article.