Recyclate-containing polyethylene multilayer films

Abstract

A multilayer film (F), comprising, in the given order, the following layers: (A) a skin layer, comprising at least 70 wt.-% of a polyethylene or mixture of polyethylenes, (B) a core layer, comprising the following components: i) 1.0 to 60.0 wt.-% of a multimodal polymer (B1) of ethylene, 1-butene and optionally one or more further comonomers selected from the group consisting of propylene and C5-C8 alpha olefins, wherein the multimodal polymer (B1) has a density in the range from 910 to 945 kg / m3, and ii) 40.0 to 99.0 wt.-% of a polyethylene-based post-consumer recyclate (B2) having a density in the range from 930 to 1050 kg / m3; wherein the combined amounts of the multimodal polymer (B1) and the polyethylene-based post-consumer recyclate (B2) add up to at least 90 wt.-%, and (C) a sealing layer, comprising at least 75 wt.-% of a polyethylene or mixture of polyethylenes.

Description

[0001] Recyclate-containing polyethylene multilayer films

[0002] Field of the Invention

[0003] The present invention relates to a multilayer film (F) comprising a skin layer, a core layer and a sealing layer, wherein the core layer comprises a multimodal polymer of ethylene, 1- butene and optionally one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins, and a polyethylene-based post-consumer recyclate.

[0004] Background to the Invention

[0005] Plastic packaging is widely used in daily life due to a favorable cost / performance ratio. Polyolefins are easy and economical to produce with good properties and are widely used in plastic packaging.

[0006] Conflicting properties are often required in the packing industry. For example, high stiffness and toughness as well as excellent sealing behavior and good optical properties are required in parallel for plastic films. Different types of polyolefin, for example polypropylene and polyethylene, are routinely combined in blends and / or used in different layers of multilayer films to achieve desired properties. However, use of more than one polymer type, such as combinations of polyethylene terephthalate) (PET) or polyamide(s) with polyolefins, complicates the task of recycling the resulting plastic packaging.

[0007] One approach to enabling recycling is a ‘single material solution’, where only one type of polymer material is used. This simplifies recycling of both post-consumer waste and manufacturing waste but limits the range of properties that are available. As such, there is still a need for plastic packaging that may be formed from a single polymer type though comprising various different polymer grades within that polymer type, optimizing the mechanical, optical and sealing properties required for packaging materials, whilst also being straightforward to mechanically recycle with the resultant recyclate also having a good balance of properties.

[0008] The demands on multilayer films especially those used for courier bags, are high, thus it is not possible to compromise on the mechanical properties of such multilayer films. The inclusion of recycled polyolefins, especially recycled polyethylene and / or polyethylene into many applications, including injection moulding and films is known; however, in the context of the present multilayer films, it is generally understood to be difficult to achieve good mechanical properties when the content of recycled material is high. As such, it is the object of the present invention to achieve good mechanical properties, despite the presence of high amounts of recycled material.

[0009] Summary of the Invention

[0010] The finding of the present invention is that multilayer films having a core layer that contains both a higher density polyethylene recyclate and a lower density multimodal polyethylene exhibit improved mechanical properties.

[0011] As such, the present invention is directed to a multilayer film (F), comprising, in the given order, the following layers:

[0012] (A) a skin layer, comprising at least 70 wt.-%, based on the total weight of the skin layer, of a polyethylene or mixture of polyethylenes,

[0013] (B) a core layer, comprising the following components: i) from 1.0 to 60.0 wt.-%, relative to the total weight of the core layer, of a multimodal polymer (Bl) of ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins, wherein the multimodal polymer (Bl) has a density, determined according to ISO 1183, in the range from 910 to 945 kg / m3, and ii) from 40.0 to 99.0 wt.-%, relative to the total weight of the core layer, of a polyethylene-based post-consumer recyclate (B2) having a density, determined according to ISO 1183, in the range from 930 to 1050 kg / m3; wherein the combined amounts of the multimodal polymer (Bl) and the polyethylenebased post-consumer recyclate (B2) add up to at least 90 wt.-%, relative to the total weight of the core layer, and

[0014] (C) a sealing layer, comprising at least 75 wt.-%, based on the total weight of the sealing layer, of a polyethylene or mixture of polyethylenes. Definitions

[0015] Unless defined otherwise, 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 pertains. Although, any methods and materials similar or equivalent to those described herein can be used in practice fortesting of the present invention, the 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.

[0016] Unless clearly indicated otherwise, use of the terms “a,” “an,” and the like refers to one or more.

[0017] In the following, amounts are given in % by weight (wt.-%) unless it is stated otherwise.

[0018] An ethylene homopolymer is a polymer that essentially consists of ethylene monomer units. Due to impurities especially during commercial polymerization processes, an ethylene homopolymer can comprise up to 0.1 mol-% comonomer units, preferably up to 0.05 mol-% comonomer units and most preferably up to 0.01 mol-% comonomer units.

[0019] An ethylene copolymer is a copolymer of ethylene monomer units and comonomer units in an amount of at least 0.1 mol-%, preferably selected from Cs-Cs alpha-olefins. Ethylene copolymers can comprise comonomer units from one or more comonomers different in their amounts of carbon atoms.

[0020] In the context of the present invention, a “copolymer of ethylene and 1 -butene” (for example) is a copolymer that consists essentially of only ethylene monomers and 1 -butene comonomers.

[0021] The term “multimodal” means that a polymer contains two or more fractions that differ in one or more properties, for example molecular weight or comonomer content. In the context of multimodal ethylene copolymers, fractions that differ in molecular weight will generally have differing melt flow rates and fractions that differ in comonomer content will generally have differing densities. A polyethylene that comprises two or more polyethylene fractions that have been produced under different polymerization conditions resulting in different (weight average) molecular weights and / or molecular weight distributions will be termed “multimodal”. In certain embodiments, a multimodal polymer will contain two differing fractions and will thus be termed “bimodal”. Bimodal polymers are a subset of multimodal polymers. For a multimodal polymer, e.g. a multimodal polyethylene, the form of the molecular weight distribution curve, i.e. the appearance of the graph of the polymer weight fraction as a function of its molecular weight, will exhibit two or more maxima or at least be distinctly broadened in comparison with the curves for the individual fractions.

[0022] In multimodal polyethylenes that are multimodal in molecular weight, there is by definition a lower molecular weight component (LMW) and a higher molecular weight component (HMW). The LMW component has a lower molecular weight than the higher molecular weight component, preferably at least 5000 g / mol lower. Any copolymer of ethylene may be multimodal in regard to the comonomer content, the comonomer distribution, the comonomer type, and the density of the constituent fractions.

[0023] For the purposes of the present description and of the subsequent claims, the term “recycled waste” is used to indicate a material recovered from both post-consumer waste and industrial waste, as opposed to virgin polymers. Post-consumer waste refers to objects having completed at least a first use cycle (or life cycle), i.e. having already served their first purpose; while industrial waste refers to manufacturing scrap, which does not normally reach a consumer.

[0024] The term “virgin” denotes the newly produced materials and / or objects prior to their first use, which have not already been recycled.

[0025] The term “recycled material” such as used herein denotes materials reprocessed from “recycled waste”.

[0026] Linear low-density polyethylenes (LLDPE) are substantially linear polymers containing a significant number of short chain branches, typically resulting from the incorporation of alpha-olefin comonomers. Linear low-low density polyethylenes (LLDPE) differ from low- density polyethylenes (LDPE) by being substantially free from long -chain branching. Linear low-density polyethylenes (LLDPE) are produced by the copolymerization of ethylene with alpha-olefin comonomers using a metallic / organometallic catalyst, such as a Ziegler Natta catalyst or a single site catalyst, e.g. a metallocene catalyst.

[0027] Low-density polyethylenes (LDPE) are produced in a high-pressure free-radical process in the absence of a metallic / organometallic catalyst. In contrast to polyethylenes produced using a metallic / organometallic catalyst (e.g. HDPE, MDPE, LLDPE etc.), low-density polyethylenes typically have higher levels of long chain branching due to the radical mechanism of the polymerization reaction.

[0028] The present invention will now be described in more detail.

[0029] Detailed Description

[0030] The present invention is directed to a multilayer film (L), comprising, in the given order, the following layers:

[0031] (A) a skin layer;

[0032] (B) a core layer; and

[0033] (C) a sealing layer.

[0034] Core layer

[0035] The core layer (B) of the present invention comprises: i) from 1.0 to 60.0 wt.-%, relative to the total weight of the core layer, of a multimodal polymer (Bl) of ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins, wherein the multimodal polymer (Bl) has a density, determined according to ISO 1183, in the range from 910 to 945 kg / m3, and ii) from 40.0 to 99.0 wt.-%, relative to the total weight of the core layer, of a polyethylene-based post-consumer recyclate (B2) having a density, determined according to ISO 1183, in the range from 930 to 1050 kg / m3; wherein the combined amounts of the multimodal polymer (Bl) and the polyethylene-based post-consumer recyclate (B2) add up to at least 90 wt.-%, relative to the total weight of the core layer.

[0036] The core layer (B) comprises: i) from 1.0 to 60.0 wt.-%, more preferably from 5.0 to 50.0 wt.-%, most preferably from 10.0 to 40.0 wt.-%, relative to the total weight of the core layer, of the multimodal polymer (Bl), and ii) from 40.0 to 99.0 wt.-%, more preferably from 50.0 to 95.0 wt.-%, most preferably from 60.0 to 90.0 wt.-%, relative to the total weight of the core layer, of the polyethylene-based post-consumer recyclate (B2).

[0037] The combined amounts of the multimodal polymer (Bl) and the polyethylene-based postconsumer recyclate (B2) add up to at least 90 wt.-%, more preferably at least 93 wt.-%, most preferably at least 95 wt.-%, relative to the total weight of the core layer.

[0038] If components other than the multimodal polymer (Bl) and the polyethylene-based postconsumer recyclate (B2) are present in the core layer (B), then it is preferred that these further components are one or more additives.

[0039] The skilled practitioner would be able to select suitable additives that are well known in the art.

[0040] The additives are preferably selected from pigments, antioxidants, UV-stabilizers, nucleating agents, mold release agents, acid scavengers, lubricants, anti-static agents, and mixtures thereof. It is understood that the content of additives includes any carrier polymers used to introduce the additives to the core layer, i.e. masterbatch carrier polymers. An example of such a carrier polymer would be a polyethylene in the form of powder.

[0041] If present, it is preferred that the total content of additives is in the range from 0.0 to 5.0 wt.- 0 / / o.

[0042] The core layer (B) preferably comprises, more preferably consists of: i) from 1.0 to 60.0 wt.-%, more preferably from 5.0 to 50.0 wt.-%, most preferably from 10.0 to 40.0 wt.-%, relative to the total weight of the core layer, of the multimodal polymer (Bl), ii) from 40.0 to 99.0 wt.-%, more preferably from 50.0 to 95.0 wt.-%, most preferably from 60.0 to 90.0 wt.-%, relative to the total weight of the core layer, of the polyethylene-based post-consumer recyclate (B2), and iii) optionally from 0.0 to 5.0 wt.-%, relative to the total weight of the core layer, of one or more additives.

[0043] The individual components will now be described in more detail.

[0044] The multimodal polymer (Bl)

[0045] One essential component of the core layer (B) is the multimodal polymer (Bl).

[0046] The multimodal polymer (Bl) is a multimodal polymer of ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins.

[0047] The multimodal polymer (Bl) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.10 to 3.0 g / 10 min, more preferably in the range from 0.12 to 2.0 g / 10 min, most preferably in the range from 0.15 to 1.6 g / 10 min. The multimodal polymer (Bl) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 6.0 g / 10 min, more preferably in the range from 0.45 to 5.0 g / 10 min, most preferably in the range from 0.50 to 4.5 g / 10 min.

[0048] The multimodal polymer (Bl) has a density, determined according to ISO 1183, in the range from in the range from 910 to 945 kg / m3, more preferably in the range from 912 to 935 kg / m3, yet more preferably in the range from 913 to 930 kg / m3, most preferably in the range from 913 to 927 kg / m3.

[0049] The multimodal polymer (B 1) preferably has a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.0 to 6.0 mol- %, more preferably in the range from 2.5 to 5.5 mol-%, most preferably in the range from 3.0 to 5.0 mol-%.

[0050] It is preferred that the multimodal polymer (Bl) does not contain any fractions being ethylene homopolymers.

[0051] In some embodiments, the multimodal polymer (Bl) is a multimodal ethylene- 1 -butene copolymer, i.e. the optional one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins are not present.

[0052] Such multimodal ethylene- 1 -butene copolymers preferably consists of a first polyolefin fraction being an ethylene- 1 -butene copolymer and a second polyolefin fraction being an ethylene- 1 -butene copolymer.

[0053] The first polyolefin fraction may differ from the second polyolefin fraction in density and / or melt flow rate.

[0054] In a first embodiment, the multimodal polymer (Bl) is a first multimodal ethylene- 1 -butene copolymer (Bia). The first multimodal ethylene- 1 -butene copolymer (Bia) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0.50 to 3.0 g / 10 min, more preferably in the range from 0.60 to 2.0 g / 10 min, most preferably in the range from 0.70 to 1.6 g / 10 min.

[0055] The first multimodal ethylene- 1 -butene copolymer (Bia) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 1.5 to 6.0 g / 10 min, more preferably in the range from 2.0 to 5.0 g / 10 min, most preferably in the range from 2.5 to 4.5 g / 10 min.

[0056] The first multimodal ethylene- 1 -butene copolymer (Bia) preferably has a density, determined according to ISO 1183, in the range from 910 to 920 kg / m3, more preferably in the range from 912 to 918 kg / m3, most preferably in the range from 913 to 917 kg / m3.

[0057] The first multimodal ethylene- 1 -butene copolymer (Bia) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.5 to 6.0 mol-%, more preferably in the range from 3.0 to 5.5 mol-%, most preferably in the range from 3.5 to 5.0 mol-%.

[0058] The first multimodal ethylene- 1 -butene copolymer (Bia) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 2.0 to 8.0, more preferably in the range from 3.0 to 7.0 most preferably in the range from 4.0 to 6.0.

[0059] It is preferred that the first multimodal ethylene- 1 -butene copolymer (Bia) has been prepared in the presence of a single site catalyst, more preferably a metallocene catalyst.

[0060] In a second embodiment, the multimodal polymer (Bl) is a second multimodal ethylene- 1- butene copolymer (Bib).

[0061] The second multimodal ethylene- 1 -butene copolymer (Bib) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0.10 to 1.00 g / 10 min, more preferably in the range from 0.12 to 0.50 g / 10 min, most preferably in the range from 0.15 to 0.30 g / 10 min.

[0062] The second multimodal ethylene- 1 -butene copolymer (Bib) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 2.0 g / 10 min, more preferably in the range from 0.50 to 1.5 g / 10 min, most preferably in the range from 0.60 to 1.2 g / 10 min.

[0063] The second multimodal ethylene- 1 -butene copolymer (Bib) preferably has a density, determined according to ISO 1183, in the range from 918 to 945 kg / m3, more preferably in the range from 920 to 935 kg / m3, most preferably in the range from 921 to 925 kg / m3.

[0064] The second multimodal ethylene- 1 -butene copolymer (Bib) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.5 to 6.0 mol-%, more preferably in the range from 3.0 to 5.5 mol-%, most preferably in the range from 3.5 to 5.0 mol-%.

[0065] The second multimodal ethylene- 1 -butene copolymer (Bib) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 8.0 to 30.0, more preferably in the range from 9.0 to 27.0 most preferably in the range from 10.0 to 24.0.

[0066] It is preferred that the second multimodal ethylene- 1 -butene copolymer (B lb) has been prepared in the presence of a Ziegler Natta catalyst.

[0067] In some embodiments, the multimodal polymer (Bl) a comprises a further comonomer selected from selected from the group consisting of propylene and Cs-Cs alpha olefins.

[0068] In a third embodiment, the multimodal polymer (Bl) is a multimodal ethylene- 1 -butene- 1- hexene terpolymer (Bic). The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0. 10 to 1.00 g / 10 min, more preferably in the range from 0. 11 to 0.50 g / 10 min, most preferably in the range from 0. 12 to 0.30 g / 10 min.

[0069] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 2.0 g / 10 min, more preferably in the range from 0.45 to 1.5 g / 10 min, most preferably in the range from 0.50 to 1.0 g / 10 min.

[0070] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) preferably has a density, determined according to ISO 1183, in the range from 918 to 945 kg / m3, more preferably in the range from 920 to 935 kg / m3, most preferably in the range from 921 to 925 kg / m3.

[0071] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) preferably has a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.0 to 6.0 mol-%, more preferably in the range from 2.5 to 5.0 mol-%, most preferably in the range from 3.0 to 4.8 mol-%.

[0072] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 8.0 to 30.0, more preferably in the range from 9.0 to 27.0 most preferably in the range from 10.0 to 24.0.

[0073] It is preferred that the multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) has been prepared in the presence of a Ziegler Natta catalyst.

[0074] It is preferred that the multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) consists of a first polyolefin fraction that is an ethylene- 1 -butene copolymer and a second polyolefin fraction that is an ethylene- 1 -butene- 1 -hexene terpolymer. Alternatively, the multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) may consist of a first polyolefin fraction that is an ethylene homopolymer and a second polyolefin fraction that is an ethylene- 1 -butene- 1 -hexene terpolymer.

[0075] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 1.0 to 4.0 mol-%, more preferably in the range from 1.3 to 3.0 mol-%, most preferably in the range from 1.5 to 2.5 mol-%.

[0076] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) preferably has a 1 -hexene (C6) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 0.5 to 2.0 mol-%, more preferably in the range from 0.8 to 1.9 mol-%, most preferably in the range from 1.0 to 1.8 mol-%.

[0077] The polyethylene-based post-consumer recyclate (B2)

[0078] Another essential component of the core layer is the polyethylene-based post-consumer recyclate (B2).

[0079] The polyethylene-based post-consumer recyclate (B2) is a polyethylene rich recycled material, meaning that it comprises significantly more polyethylene than polypropylene (and other contaminants). Recycled waste streams, which are high in polyethylene can be obtained for example from the recycling of courier bags, heavy duty shipping sacks, or general -purpose films.

[0080] Preferably, the polyethylene rich recycled material is obtained from recycled waste, more preferably wherein the recycled waste is at least partially derived from courier bags, by means of plastic recycling processes known in the art. Such recyclates may be commercially available, e.g. from Shanghai Tianqiang Environmental Protection Technology Co. Ltd, Changzhou Jinyong Technology materials Co. Ltd, Borouge Sales & Marketing (Shanghai) Co., Ltd. etc. Non-exhaustive examples of polyethylene rich recycled materials include: rLLD471, rLLD461 (Borouge Sales & Marketing Shanghai Co., Ltd), r-PE158, r-PE668 or r-PE778 (Shanghai Tianqiang Environmental Protection Technology Co. Ltd).

[0081] During recycling, any reasonable measure will usually be taken for any components other than polyethylene to be reduced / removed as far as the final application or use suggests such measures; however, other components are often present in small amounts.

[0082] Other such components include polypropylene (PP), polystyrene (PS), polyamides (PA), polyethylene terephthalate (PET), which are all present in as low an amount as possible, preferably below the detection limit.

[0083] The polyethylene-based post-consumer recyclate (B2) has a density, determined according to ISO 1183, in the range from 930 to 1050 kg / m3, more preferably in the range from 935 to 1020 kg / m3, yet more preferably in the range from 940 to 1000 kg / m3, even more preferably in the range from 945 to 1000 kg / m3, most preferably in the range from 950 to 1000 kg / m3.

[0084] The polyethylene-based post-consumer recyclate (B2) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.20 to 10.0 g / 10 min, more preferably in the range from 0.30 to 5.0 g / 10 min, most preferably in the range from 0.40 to 3.0 g / 10 min.

[0085] The polyethylene-based post-consumer recyclate (B2) preferably has a flexural modulus, determined according to ISO 178 using 80x 10x4 mm3test bars compression-moulded in line with ISO 294-1, in the range from 150 to 600 MPa, more preferably in the range from 160 to 550 MPa, most preferably in the range from 175 to 500 MPa.

[0086] The polyethylene-based post-consumer recyclate (B2) preferably has a tensile modulus, determined according to ISO 527-2:2012, on a specimen of Tensile type 1A, in the range from 150 to 600 MPa, more preferably in the range from 160 to 500 MPa, most preferably in the range from 175 to 400 MPa. The polyethylene-based post-consumer recyclate (B2) preferably has a tensile stress at yield, determined according to ISO 527-2:2012, on a specimen of Tensile type 1A, in the range from 4 to 30 MPa, more preferably in the range from 6 to 20 MPa, most preferably in the range from 8 to 15 MPa.

[0087] The polyethylene-based post-consumer recyclate (B2) preferably has a tensile strain at yield, determined according to ISO 527-2:2012, on a specimen of Tensile type 1A, in the range from 5 to 50%, more preferably in the range from 8 to 35%, most preferably in the range from 10 to 20%.

[0088] The polyethylene-based post-consumer recyclate (B2) preferably has a tensile stress at break, determined according to ISO 527-2:2012, on a specimen of Tensile type 1A, in the range from 10 to 50 MPa, more preferably in the range from 12 to 40 MPa, most preferably in the range from 14 to 30 MPa.

[0089] The polyethylene-based post-consumer recyclate (B2) preferably has an elongation at break, determined according to ISO 527-2:2012, on a specimen of Tensile type 1A, in the range from 300 to 1200%, more preferably in the range from 325 to 1100%, most preferably in the range from 350 to 1050%.

[0090] The polyethylene-based post-consumer recyclate (B2) preferably has a Charpy Notched impact strength at 23 °C, determined according to ISO 179 using 80x 10x4 mm3test bars compression-moulded in line with ISO 294-1, in the range from 25 to 100 kJ / m2, more preferably in the range from 30 to 90 kJ / m2, most preferably in the range from 35 to 80 kJ / m2.

[0091] The polyethylene-based post-consumer recyclate (B2) preferably has an ash content, determined according to the method given in the determination methods, in the range from 1.0 to 12.0 wt.-%, more preferably in the range from 1.5 to 11.0 wt.-%, most preferably in the range from 2.0 to 10.0 wt.-%. Skin layer

[0092] The skin layer (A) of the present invention, comprises at least 70 wt.-%, more preferably at least 75 wt.-%, based on the total weight of the skin layer, of a polyethylene or mixture of polyethylenes.

[0093] It is preferred that the skin layer (A) comprises: a) from 20.0 to 70.0 wt.-%, relative to the total weight of the skin layer, of an ethylene copolymer (Al) containing ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins and having a density, determined according to ISO 1183, in the range from 910 to 945 kg / m3; b) from 5.0 to 30.0 wt.-%, relative to the total weight of the skin layer, of one or more inorganic pigments (A2), wherein the one or more inorganic pigments are preferably white inorganic pigments; c) from 10.0 to 50.0 wt.-%, relative to the total weight of the skin layer, of one or more further polyethylenes (A3) that are different to the ethylene copolymer (Al); and d) optionally, from 0.0 to 5.0 wt.-%, relative to the total weight of the skin layer, of one or more further additives (A4) other than inorganic pigments.

[0094] The skin layer (A) comprises: a) from 20.0 to 70.0 wt.-%, more preferably from 30.0 to 60.0 wt.-%, most preferably from 40.0 to 50.0 wt.-%, relative to the total weight of the skin layer, of the ethylene copolymer (Al); b) from 5.0 to 30.0 wt.-%, more preferably from 10.0 to 27.0 wt.-%, most preferably from 15.0 to 24.0 wt.-%, relative to the total weight of the skin layer, of the one or more inorganic pigments (A2); c) from 10.0 to 50.0 wt.-%, more preferably from 20.0 to 45.0 wt.-%, most preferably from 30.0 to 40.0 wt.-%, relative to the total weight of the skin layer, of the one or more further polyethylenes (A3) that are different to the ethylene copolymer (Al); and d) optionally, from 0.0 to 5.0 wt.-%, relative to the total weight of the skin layer, of the one or more further additives (A4) other than inorganic pigments. The total weight of the ethylene copolymer (Al), the one or more inorganic pigments (A2), the one or more further polyethylenes (A3), and the optional one or more further additives (A4) add up to at least 90 wt.-%, more preferably at least 95 wt.-%, yet more preferably at least 98 wt.-%, relative to the total weight of the skin layer, most preferably the skin layer consists of the ethylene copolymer (Al), the one or more inorganic pigments (A2), the one or more further polyethylenes (A3), and the optional one or more further additives (A4).

[0095] The skilled practitioner would be able to select suitable additives that are well known in the art.

[0096] The additives are preferably selected from antioxidants, UV-stabilizers, nucleating agents, mold release agents, acid scavengers, lubricants, anti-static agents, and mixtures thereof.

[0097] In the context of the present invention, any carrier polymers used to introduce the one or more inorganic pigments (A2) and / or optional one or more further additives (A4) to the skin layer, i.e. masterbatch carrier polymers, are assigned to the one or more further polyethylenes (A3) if they are polyethylenes, or to the content of the optional one or more further additives (A4) if they are not polyethylenes. An example of such a carrier polymer would be a polyethylene in the form of powder.

[0098] The individual components will now be described in more detail.

[0099] Ethylene copolymer (Al)

[0100] One essential component of the preferred skin layer (A) is the ethylene copolymer (Al).

[0101] The ethylene copolymer (Al) is a polymer of ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins. The ethylene copolymer (Al) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.10 to 3.0 g / 10 min, more preferably in the range from 0.12 to 2.0 g / 10 min, most preferably in the range from 0.15 to 1.6 g / 10 min.

[0102] The ethylene copolymer (Al) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 6.0 g / 10 min, more preferably in the range from 0.45 to 5.0 g / 10 min, most preferably in the range from 0.50 to 4.5 g / 10 min.

[0103] The ethylene copolymer (Al) has a density, determined according to ISO 1183, in the range from in the range from 910 to 945 kg / m3, more preferably in the range from 912 to 935 kg / m3, yet more preferably in the range from 913 to 930 kg / m3, most preferably in the range from 913 to 927 kg / m3.

[0104] The ethylene copolymer (Al) preferably has a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.0 to 6.0 mol- %, more preferably in the range from 2.5 to 5.5 mol-%, most preferably in the range from 3.0 to 5.0 mol-%.

[0105] It is preferred that the ethylene copolymer (Al) does not contain any fractions being ethylene homopolymers.

[0106] It is particularly preferred that the ethylene copolymer (Al) is a multimodal ethylene copolymer.

[0107] In some embodiments, the ethylene copolymer (Al) is an ethylene- 1 -butene copolymer, i.e. the optional one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins are not present. More preferably, the ethylene- 1 -butene copolymer is a multimodal ethylene- 1 -butene copolymer. Such multimodal ethylene- 1 -butene copolymers preferably consists of a first polyolefin fraction being an ethylene- 1 -butene copolymer and a second polyolefin fraction being an ethylene- 1 -butene copolymer.

[0108] The first polyolefin fraction may differ from the second polyolefin fraction in density and / or melt flow rate.

[0109] In a first embodiment, the ethylene copolymer (Al) is a first multimodal ethylene- 1 -butene copolymer (Ala).

[0110] The first multimodal ethylene- 1 -butene copolymer (Ala) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0.50 to 3.0 g / 10 min, more preferably in the range from 0.60 to 2.0 g / 10 min, most preferably in the range from 0.70 to 1.6 g / 10 min.

[0111] The first multimodal ethylene- 1 -butene copolymer (Ala) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 1.5 to 6.0 g / 10 min, more preferably in the range from 2.0 to 5.0 g / 10 min, most preferably in the range from 2.5 to 4.5 g / 10 min.

[0112] The first multimodal ethylene- 1 -butene copolymer (Ala) preferably has a density, determined according to ISO 1183, in the range from 910 to 920 kg / m3, more preferably in the range from 912 to 918 kg / m3, most preferably in the range from 913 to 917 kg / m3.

[0113] The first multimodal ethylene- 1 -butene copolymer (Ala) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.5 to 6.0 mol-%, more preferably in the range from 3.0 to 5.5 mol-%, most preferably in the range from 3.5 to 5.0 mol-%.

[0114] The first multimodal ethylene- 1 -butene copolymer (Ala) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 2.0 to 8.0, more preferably in the range from 3.0 to 7.0 most preferably in the range from 4.0 to 6.0.

[0115] It is preferred that the first multimodal ethylene- 1 -butene copolymer (Ala) has been prepared in the presence of a single site catalyst, more preferably a metallocene catalyst.

[0116] In a second embodiment, the ethylene copolymer (Al) is a second multimodal ethylene- 1- butene copolymer (Alb).

[0117] The second multimodal ethylene- 1 -butene copolymer (Alb) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0. 10 to 1.00 g / 10 min, more preferably in the range from 0. 12 to 0.50 g / 10 min, most preferably in the range from 0. 15 to 0.30 g / 10 min.

[0118] The second multimodal ethylene- 1 -butene copolymer (Alb) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 2.0 g / 10 min, more preferably in the range from 0.50 to 1.5 g / 10 min, most preferably in the range from 0.60 to 1.2 g / 10 min.

[0119] The second multimodal ethylene- 1 -butene copolymer (Alb) preferably has a density, determined according to ISO 1183, in the range from 918 to 945 kg / m3, more preferably in the range from 920 to 935 kg / m3, most preferably in the range from 921 to 925 kg / m3.

[0120] The second multimodal ethylene- 1 -butene copolymer (Alb) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.5 to 6.0 mol-%, more preferably in the range from 3.0 to 5.5 mol-%, most preferably in the range from 3.5 to 5.0 mol-%.

[0121] The second multimodal ethylene- 1 -butene copolymer (Alb) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 8.0 to 30.0, more preferably in the range from 9.0 to 27.0 most preferably in the range from 10.0 to 24.0. It is preferred that the second multimodal ethylene- 1 -butene copolymer (Alb) has been prepared in the presence of a Ziegler Natta catalyst.

[0122] In some embodiments, the ethylene copolymer (Al) a comprises a further comonomer selected from selected from the group consisting of propylene and Cs-Cs alpha olefins.

[0123] In a third embodiment, the ethylene copolymer (Al) is a multimodal ethylene- 1 -butene- 1 - hexene terpolymer (Ale).

[0124] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0.10 to 1.00 g / 10 min, more preferably in the range from 0.11 to 0.50 g / 10 min, most preferably in the range from 0. 12 to 0.30 g / 10 min.

[0125] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 2.0 g / 10 min, more preferably in the range from 0.45 to 1.5 g / 10 min, most preferably in the range from 0.50 to 1.0 g / 10 min.

[0126] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) preferably has a density, determined according to ISO 1183, in the range from 918 to 945 kg / m3, more preferably in the range from 920 to 935 kg / m3, most preferably in the range from 921 to 925 kg / m3.

[0127] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) preferably has a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.0 to 6.0 mol-%, more preferably in the range from 2.5 to 5.0 mol-%, most preferably in the range from 3.0 to 4.8 mol-%.

[0128] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 8.0 to 30.0, more preferably in the range from 9.0 to 27.0 most preferably in the range from 10.0 to 24.0.

[0129] It is preferred that the multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) has been prepared in the presence of a Ziegler Natta catalyst.

[0130] It is preferred that the multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) consists of a first polyolefin fraction that is an ethylene- 1 -butene copolymer and a second polyolefin fraction that is an ethylene- 1 -butene- 1 -hexene terpolymer.

[0131] Alternatively, the multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) may consist of a first polyolefin fraction that is an ethylene homopolymer and a second polyolefin fraction that is an ethylene- 1 -butene- 1 -hexene terpolymer.

[0132] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 1.0 to 4.0 mol-%, more preferably in the range from 1.3 to 3.0 mol-%, most preferably in the range from 1.5 to 2.5 mol-%.

[0133] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Ale) preferably has a 1 -hexene (C6) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 0.5 to 2.0 mol-%, more preferably in the range from 0.8 to 1.9 mol-%, most preferably in the range from 1.0 to 1.8 mol-%.

[0134] One or more inorganic pigments (A2)

[0135] Another essential component of the preferred skin layer is one or more inorganic pigments.

[0136] In the broadest sense, the one or more inorganic pigments may be any inorganic pigments known in the art. It is, however, preferred that the one or more pigments are white inorganic pigments. Even more preferably, at least one of the one or more inorganic pigments is titanium dioxide.

[0137] It is particularly preferred that only one white pigment is present, wherein this white pigment is titanium dioxide.

[0138] The titanium dioxide is preferably in a form of rutile. Rutile is a mineral that is primarily based on titanium dioxide and has a tetragonal unit cell structure as well known in the art.

[0139] One or more further polyethylenes (A3)

[0140] Another essential component of the preferred skin layer is the one or more further polyethylenes (A3) that are different to the ethylene copolymer (Al).

[0141] In the broadest sense, these polyethylenes may be any suitable polyethylenes.

[0142] In a first embodiment, it is preferred that at least one of the one or more further polyethylenes (A3) is a low-density polyethylene (A3a).

[0143] The low-density polyethylene (A3a) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.5 to 4.0 g / 10 min, more preferably in the range from 1.0 to 3.0 g / 10 min, most preferably in the range from 1.5 to 2.5 g / 10 min.

[0144] The low-density polyethylene (A3a) preferably has a density, determined according to ISO 1183, in the range from 910 to 935 kg / m3, more preferably 915 to 930 kg / m3, most preferably in the range from 920 to 925 kg / m3.

[0145] The low-density polyethylene (A3a) preferably has a molecular weight distribution (Mw / Mn), determined according to the viscosity GPC method given in the determination methods, in the range from 3.0 to 12.0, more preferably in the range from 4.0 to 10.0, most preferably in the range from 5.0 to 9.0. If present, the low-density polyethylene (A3a) is preferably present in an amount in the range from 10.0 to 50.0 wt.-%, more preferably in the range from 20.0 to 40.0 wt.-%, most preferably in the range from 25.0 to 35.0 wt.-%, relative to the total weight of the skin layer.

[0146] In a second embodiment, it is preferred that at least one of the one or more further polyethylenes (A3) is a linear low-density polyethylene (A3b).

[0147] The linear low-density polyethylene (A3b) contains ethylene and one or more comonomers selected from the group consisting of Cs-Cs alpha olefins.

[0148] The linear low-density polyethylene (A3b) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.3 to 3.0 g / 10 min, more preferably in the range from 0.5 to 2.5 g / 10 min, most preferably in the range from 0.7 to 2.0 g / 10 min.

[0149] The linear low-density polyethylene (A3b) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 1.0 to 8.0 g / 10 min, more preferably in the range from 1.5 to 7.0 g / 10 min, most preferably in the range from 2.0 to 6.0 g / 10 min.

[0150] The linear low-density polyethylene (A3b) preferably has a density, determined according to ISO 1183, in the range from 909 to 923 kg / m3, more preferably in the range from 911 to 921 kg / m3, most preferably in the range from 913 to 919 kg / m3.

[0151] The linear low-density polyethylene (A3b) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 2.0 to 7.0, more preferably in the range from 2.5 to 6.0, most preferably in the range from 3.0 to 5.0.

[0152] The linear low-density polyethylene (A3b) preferably has a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 1.5 to 5.6 mol-%, more preferably in the range from 2.1 to 5.0 mol-%, most preferably in the range from 2.7 to 4.5 mol-%.

[0153] It is preferred that the linear low-density polyethylene (A3b) contains ethylene, 1 -butene and 1 -hexene.

[0154] The linear low-density polyethylene (A3b) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 0.05 to 1.00 mol-%, more preferably in the range from 0. 10 to 0.90 mol-%, most preferably in the range 0.20 to 0.80 mol-%.

[0155] The linear low-density polyethylene (A3b) preferably has a 1 -hexene (C6) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 1.5 to 4.8 mol-%, more preferably in the range from 2.0 to 4.3 mol-%, most preferably in the range from 2.5 to 3.5 mol-%

[0156] The linear low-density polyethylene (A3b) is preferably multimodal.

[0157] The linear low-density polyethylene (A3b) preferably has a bimodal structure wherein the linear low-density polyethylene (LLDPE) consists of a first polymer fraction that is a copolymer of ethylene and a first C4-C8 alpha olefin and a second polymer fraction that is a copolymer of ethylene and a second C4-C8 alpha olefin, wherein the first C4-C8 alpha olefin is different to the second C4-C8 alpha olefin. Preferably the first C4-C8 alpha olefin is 1 - butene and the second C4-C8 alpha olefin is 1 -hexene.

[0158] If present, the linear low-density polyethylene (A3b) is preferably present in an amount in the range from 10.0 to 50.0 wt.-%, more preferably in the range from 20.0 to 40.0 wt.-%, most preferably in the range from 25.0 to 35.0 wt.-%, relative to the total weight of the skin layer. Sealing layer

[0159] The sealing layer (C) of the present invention, comprises at least 75 wt.-%, more preferably at least 85 wt.-%, most preferably at least 95 wt.-%, based on the total weight of the sealing layer, of a polyethylene or mixture of polyethylenes.

[0160] It is preferred that the sealing layer (C) comprises: a) from 30.0 to 89.9 wt.-%, relative to the total weight of the sealing layer, of an ethylene copolymer (Cl) containing ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins and having a density, determined according to ISO 1183, in the range from 910 to 945 kg / m3; b) from 0.1 to 5.0 wt.-%, relative to the total weight of the sealing layer, of one or more pigments (C2), wherein the one or more inorganic pigments are preferably black pigments; c) from 10.0 to 69.9 wt.-%, relative to the total weight of the sealing layer, of one or more further polyethylenes (C3) that are different to the ethylene copolymer (Cl); and d) optionally, from 0.0 to 5.0 wt.-%, relative to the total weight of the sealing layer, of one or more further additives (C4) other than inorganic pigments.

[0161] The sealing layer (C) comprises: a) from 30.0 to 89.9 wt.-%, more preferably from 40.0 to 79.8 wt.-%, most preferably from 45.0 to 69.7 wt.-%, relative to the total weight of the sealing layer, of the ethylene copolymer (Cl); b) from 0.1 to 5.0 wt.-%, more preferably from 0.2 to 3.0 wt.-%, most preferably from 0.3 to 2.0 wt.-%, relative to the total weight of the sealing layer, of the one or more pigments (C2); c) from 10.0 to 69.9 wt.-%, more preferably from 20.0 to 59.8 wt.-%, most preferably from 35.0 to 54.7 wt.-%, relative to the total weight of the sealing layer, of the one or more further polyethylenes (C3) that are different to the ethylene copolymer (Cl); and d) optionally, from 0.0 to 5.0 wt.-%, relative to the total weight of the sealing layer, of the one or more further additives (C4) other than inorganic pigments. The total weight of the ethylene copolymer (Cl), the one or more pigments (C2), the one or more further polyethylenes (C3), and the optional one or more further additives (C4) add up to at least 90 wt.-%, more preferably at least 95 wt.-%, yet more preferably at least 98 wt.-%, relative to the total weight of the sealing layer, most preferably the sealing layer consists of the ethylene copolymer (Cl), the one or more pigments (C2), the one or more further polyethylenes (C3), and the optional one or more further additives (C4).

[0162] The skilled practitioner would be able to select suitable additives that are well known in the art.

[0163] The additives are preferably selected from antioxidants, UV-stabilizers, nucleating agents, mold release agents, acid scavengers, lubricants, anti-static agents, and mixtures thereof.

[0164] In the context of the present invention, any carrier polymers used to introduce the one or more pigments (C2) and / or optional one or more further additives (C4) to the sealing layer, i.e. masterbatch carrier polymers, are assigned to the one or more further polyethylenes (C3) if they are polyethylenes, or to the content of the optional one or more further additives (C4) if they are not polyethylenes. An example of such a carrier polymer would be a polyethylene in the form of powder.

[0165] The individual components will now be described in more detail.

[0166] Ethylene copolymer (Cl)

[0167] One essential component of the preferred sealing layer (C) is the ethylene copolymer (Cl).

[0168] The ethylene copolymer (Cl) is a polymer of ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins. The ethylene copolymer (Cl) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.10 to 3.0 g / 10 min, more preferably in the range from 0.12 to 2.0 g / 10 min, most preferably in the range from 0.15 to 1.6 g / 10 min.

[0169] The ethylene copolymer (Cl) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 6.0 g / 10 min, more preferably in the range from 0.45 to 5.0 g / 10 min, most preferably in the range from 0.50 to 4.5 g / 10 min.

[0170] The ethylene copolymer (Cl) has a density, determined according to ISO 1183, in the range from in the range from 910 to 945 kg / m3, more preferably in the range from 912 to 935 kg / m3, yet more preferably in the range from 913 to 930 kg / m3, most preferably in the range from 913 to 927 kg / m3.

[0171] The ethylene copolymer (Cl) preferably has a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.0 to 6.0 mol- %, more preferably in the range from 2.5 to 5.5 mol-%, most preferably in the range from 3.0 to 5.0 mol-%.

[0172] It is particularly preferred that the ethylene copolymer (Cl) is a multimodal ethylene copolymer.

[0173] It is preferred that the ethylene copolymer (Cl) does not contain any fractions being ethylene homopolymers.

[0174] In some embodiments, the ethylene copolymer (Cl) is an ethylene- 1 -butene copolymer, i.e. the optional one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins are not present. More preferably, the ethylene- 1 -butene copolymer is a multimodal ethylene- 1 -butene copolymer. Such multimodal ethylene- 1 -butene copolymers preferably consists of a first polyolefin fraction being an ethylene- 1 -butene copolymer and a second polyolefin fraction being an ethylene- 1 -butene copolymer.

[0175] The first polyolefin fraction may differ from the second polyolefin fraction in density and / or melt flow rate.

[0176] In a first embodiment, the ethylene copolymer (Cl) is a first multimodal ethylene- 1 -butene copolymer (Cl a).

[0177] The first multimodal ethylene- 1 -butene copolymer (Cl a) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0.50 to 3.0 g / 10 min, more preferably in the range from 0.60 to 2.0 g / 10 min, most preferably in the range from 0.70 to 1.6 g / 10 min.

[0178] The first multimodal ethylene- 1 -butene copolymer (Cl a) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 1.5 to 6.0 g / 10 min, more preferably in the range from 2.0 to 5.0 g / 10 min, most preferably in the range from 2.5 to 4.5 g / 10 min.

[0179] The first multimodal ethylene- 1 -butene copolymer (Cl a) preferably has a density, determined according to ISO 1183, in the range from 910 to 920 kg / m3, more preferably in the range from 912 to 918 kg / m3, most preferably in the range from 913 to 917 kg / m3.

[0180] The first multimodal ethylene- 1 -butene copolymer (Cl a) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.5 to 6.0 mol-%, more preferably in the range from 3.0 to 5.5 mol-%, most preferably in the range from 3.5 to 5.0 mol-%.

[0181] The first multimodal ethylene- 1 -butene copolymer (Cl a) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 2.0 to 8.0, more preferably in the range from 3.0 to 7.0 most preferably in the range from 4.0 to 6.0.

[0182] It is preferred that the first multimodal ethylene- 1 -butene copolymer (Cl a) has been prepared in the presence of a single site catalyst, more preferably a metallocene catalyst.

[0183] In a second embodiment, the ethylene copolymer (Cl) is a second multimodal ethylene- 1- butene copolymer (Clb).

[0184] The second multimodal ethylene- 1 -butene copolymer (Clb) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0. 10 to 1.00 g / 10 min, more preferably in the range from 0. 12 to 0.50 g / 10 min, most preferably in the range from 0. 15 to 0.30 g / 10 min.

[0185] The second multimodal ethylene- 1 -butene copolymer (Clb) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 2.0 g / 10 min, more preferably in the range from 0.50 to 1.5 g / 10 min, most preferably in the range from 0.60 to 1.2 g / 10 min.

[0186] The second multimodal ethylene- 1 -butene copolymer (Clb) preferably has a density, determined according to ISO 1183, in the range from 918 to 945 kg / m3, more preferably in the range from 920 to 935 kg / m3, most preferably in the range from 921 to 925 kg / m3.

[0187] The second multimodal ethylene- 1 -butene copolymer (Clb) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.5 to 6.0 mol-%, more preferably in the range from 3.0 to 5.5 mol-%, most preferably in the range from 3.5 to 5.0 mol-%.

[0188] The second multimodal ethylene- 1 -butene copolymer (Clb) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 8.0 to 30.0, more preferably in the range from 9.0 to 27.0 most preferably in the range from 10.0 to 24.0. It is preferred that the second multimodal ethylene- 1 -butene copolymer (Clb) has been prepared in the presence of a Ziegler Natta catalyst.

[0189] In some embodiments, the ethylene copolymer (Cl) a comprises a further comonomer selected from selected from the group consisting of propylene and Cs-Cs alpha olefins.

[0190] In a third embodiment, the ethylene copolymer (Cl) is a multimodal ethylene- 1 -butene- 1 - hexene terpolymer (Clc).

[0191] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0.10 to 1.00 g / 10 min, more preferably in the range from 0.11 to 0.50 g / 10 min, most preferably in the range from 0. 12 to 0.30 g / 10 min.

[0192] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 2.0 g / 10 min, more preferably in the range from 0.45 to 1.5 g / 10 min, most preferably in the range from 0.50 to 1.0 g / 10 min.

[0193] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) preferably has a density, determined according to ISO 1183, in the range from 918 to 945 kg / m3, more preferably in the range from 920 to 935 kg / m3, most preferably in the range from 921 to 925 kg / m3.

[0194] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) preferably has a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.0 to 6.0 mol-%, more preferably in the range from 2.5 to 5.0 mol-%, most preferably in the range from 3.0 to 4.8 mol-%.

[0195] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 8.0 to 30.0, more preferably in the range from 9.0 to 27.0 most preferably in the range from 10.0 to 24.0.

[0196] It is preferred that the multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) has been prepared in the presence of a Ziegler Natta catalyst.

[0197] It is preferred that the multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) consists of a first polyolefin fraction that is an ethylene- 1 -butene copolymer and a second polyolefin fraction that is an ethylene- 1 -butene- 1 -hexene terpolymer.

[0198] Alternatively, the multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) may consist of a first polyolefin fraction that is an ethylene homopolymer and a second polyolefin fraction that is an ethylene- 1 -butene- 1 -hexene terpolymer.

[0199] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 1.0 to 4.0 mol-%, more preferably in the range from 1.8 to 3.0 mol-%, most preferably in the range from 1.5 to 2.5 mol-%.

[0200] The multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Clc) preferably has a 1 -hexene (C6) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 0.5 to 2.0 mol-%, more preferably in the range from 0.8 to 1.9 mol-%, most preferably in the range from 1.0 to 1.8 mol-%.

[0201] One or more pigments (C2)

[0202] Another essential component of the preferred sealing layer is the one or more pigments.

[0203] In the broadest sense, these pigments may be any suitable pigments. It is, however, preferred that the one or more pigments are black pigments

[0204] Even more preferably, at least one of the one or more pigments is carbon black. It is particularly preferred that only one black pigment is present, wherein this black pigment is carbon black.

[0205] One or more further polyethylenes (C3)

[0206] Another essential component of the preferred sealing layer is the one or more further polyethylenes (C3) that are different to the ethylene copolymer (Cl).

[0207] In the broadest sense, these polyethylenes may be any suitable polyethylenes.

[0208] In a first embodiment, it is preferred that at least one of the one or more further polyethylenes (C3) is a low-density polyethylene (C3a).

[0209] The low-density polyethylene (C3a) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.5 to 4.0 g / 10 min, more preferably in the range from 1.0 to 3.0 g / 10 min, most preferably in the range from 1.5 to 2.5 g / 10 min.

[0210] The low-density polyethylene (C3a) preferably has a density, determined according to ISO 1183, in the range from 910 to 935 kg / m3, more preferably 915 to 930 kg / m3, most preferably in the range from 920 to 925 kg / m3.

[0211] The low-density polyethylene (C3a) preferably has a molecular weight distribution (Mw / Mn), determined according to the viscosity GPC method given in the determination methods, in the range from 3.0 to 12.0, more preferably in the range from 4.0 to 10.0, most preferably in the range from 5.0 to 9.0.

[0212] If present, the low-density polyethylene (C3a) is preferably present in an amount in the range from 10.0 to 50.0 wt.-%, more preferably in the range from 15.0 to 40.0 wt.-%, most preferably in the range from 18.0 to 33.0 wt.-%, relative to the total weight of the sealing layer. In a second embodiment, it is preferred that at least one of the one or more further polyethylenes (C3) is a linear low-density polyethylene (C3b).

[0213] The linear low-density polyethylene (C3b) contains ethylene and one or more comonomers selected from the group consisting of Cs-Cs alpha olefins.

[0214] The linear low-density polyethylene (C3b) preferably has a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.3 to 3.0 g / 10 min, more preferably in the range from 0.5 to 2.5 g / 10 min, most preferably in the range from 0.7 to 2.0 g / 10 min.

[0215] The linear low-density polyethylene (C3b) preferably has a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 1.0 to 8.0 g / 10 min, more preferably in the range from 1.5 to 7.0 g / 10 min, most preferably in the range from 2.0 to 6.0 g / 10 min.

[0216] The linear low-density polyethylene (C3b) preferably has a density, determined according to ISO 1183, in the range from 909 to 923 kg / m3, more preferably in the range from 911 to 921 kg / m3, most preferably in the range from 913 to 919 kg / m3.

[0217] The linear low-density polyethylene (C3b) preferably has a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 2.0 to 7.0, more preferably in the range from 2.5 to 6.0, most preferably in the range from 3.0 to 5.0.

[0218] The linear low-density polyethylene (C3b) preferably has a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 1.5 to 5.6 mol-%, more preferably in the range from 2.1 to 5.0 mol-%, most preferably in the range from 2.7 to 4.5 mol-%. It is preferred that the linear low-density polyethylene (C3b) contains ethylene, 1 -butene and 1 -hexene.

[0219] The linear low-density polyethylene (C3b) preferably has a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 0.05 to 1.00 mol-%, more preferably in the range from 0. 10 to 0.90 mol-%, most preferably in the range 0.20 to 0.80 mol-%.

[0220] The linear low-density polyethylene (C3b) preferably has a 1 -hexene (C6) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 1.5 to 4.8 mol-%, more preferably in the range from 2.0 to 4.3 mol-%, most preferably in the range from 2.5 to 3.5 mol-%

[0221] The linear low-density polyethylene (C3b) is preferably multimodal.

[0222] The linear low-density polyethylene (C3b) preferably has a bimodal structure wherein the linear low-density polyethylene (LLDPE) consists of a first polymer fraction that is a copolymer of ethylene and a first C4-C8 alpha olefin and a second polymer fraction that is a copolymer of ethylene and a second C4-C8 alpha olefin, wherein the first C4-C8 alpha olefin is different to the second C4-C8 alpha olefin. Preferably the first C4-C8 alpha olefin is 1 - butene and the second C4-C8 alpha olefin is 1 -hexene.

[0223] If present, the linear low-density polyethylene (C3b) is preferably present in an amount in the range from 10.0 to 50.0 wt.-%, more preferably in the range from 20.0 to 40.0 wt.-%, most preferably in the range from 25.0 to 35.0 wt.-%, relative to the total weight of the sealing layer.

[0224] Multilayer film (F)

[0225] As described above, the multilayer film (F) comprises, in the given order, the following layers:

[0226] (A) a skin layer; (B) a core layer; and

[0227] (C) a sealing layer.

[0228] Although other layers may be present, it is preferred that any further layers, if present, are between the skin layer (A) and the core layer (B) or between the core layer (B) and between the sealing layer (C), most preferably between the skin layer (A) and the core layer (B).

[0229] If a further layer is between the skin layer (A) and the core layer (B), it may be termed a subouter skin layer (AB) and if a further layer is between the core layer (C) and the sealing layer (C), it may be termed a sub-inner sealing layer (BC). In some embodiments, the film may comprise more than one instance of any one of layers (A), (AB), (B), (BC) or (C).

[0230] It is preferred that the multilayer film (F) consists of from 3 to 7 layers, more preferably from 3 to 5 layers.

[0231] It is particularly preferred that no further layers are present, i.e. that the multilayer film (F) is a 3 -layer film, consisting of layers (A), (B) and (C).

[0232] It is preferred that the multilayer film (F) has a thickness in the range from 15 to 100 pm, more preferably in the range from 20 to 95 pm, most preferably in the range from 25 to 90 pm.

[0233] It is preferred that: a) the skin (A) layer has a thickness in the range from 5 to 40% of the total thickness of the multilayer film (F); b) the core layer (B) has a thickness in the range from 20 to 90% of the total thickness of the multilayer film (F); and c) the sealing layer (C) has a thickness in the range from 5 to 40% of the total thickness of the multilayer film (F).

[0234] It is further preferred that: a) the skin layer (A) has a thickness in the range from 10 to 35% of the total thickness of the multilayer film (F); b) the core layer (B) has a thickness in the range from 30 to 80% of the total thickness of the multilayer film (F); and c) the sealing layer (C) has a thickness in the range from 10 to 35% of the total thickness of the multilayer film (F).

[0235] It is particularly preferred that: a) the skin layer (A) has a thickness in the range from 15 to 30% of the total thickness of the multilayer film (F); b) the core layer (B) has a thickness in the range from 40 to 70% of the total thickness of the multilayer film (F); and c) the sealing layer (C) has a thickness in the range from 15 to 30% of the total thickness of the multilayer film (F).

[0236] It is preferred that the polyethylene-based post consumer recyclate (B2) is present in an amount in the range from 20.0 to 80.0 wt.-%, more preferably in the range from 25.0 to 65 wt.-%, most preferably in the range from 30.0 to 60 wt.-%, relative to the total weight of the multilayer film (F).

[0237] It is preferred that the multilayer film (F) has a tensile modulus in the machine direction (TM-MD), measured according to ASTM D882, in the range from 125 to 500 MPa, more preferably in the range from 150 to 400 MPa, most preferably in the range from 175 to 300 MPa.

[0238] It is preferred that the multilayer film (F) has a tensile strength in the machine direction (TS- MD), measured according to ISO 527-3, in the range from 30 to 75 MPa, more preferably in the range from 32 to 70 MPa, most preferably in the range from 35 to 60 MPa.

[0239] It is preferred that the multilayer film (F) has an elongation at break in the machine direction (EB-MD), measured according to ISO 527-3, in the range from 350 to 1000%, more preferably in the range from 400 to 800%, most preferably in the range from 450 to 700%. It is preferred that the multilayer film (F) has an elongation at break in the transverse direction (EB-TD), measured according to ISO 527-3, in the range from 400 to 1000%, more preferably in the range from 550 to 900%, most preferably in the range from 700 to 800%.

[0240] It is preferred that the multilayer film (F) has a dart drop impact strength (DDI), determined according to ASTM D1709 method A, in the range from 2.0 to 6.0 g / pm, more preferably in the range from 2.2 to 5.5 g / pm, most preferably in the range from 2.7 to 5.0 g / pm.

[0241] It is preferred that the multilayer film (F) has a dart drop impact strength (DDI), determined according to ASTM DI 709 method A, in the range from 100 to 500 g, more preferably in the range from 125 to 400 g, most preferably in the range from 150 to 300 g.

[0242] It is preferred that the multilayer film (F) has a puncture force at break, determined according to ASTM D5748, in the range from 30 to 100 N, more preferably in the range from 40 to 90 N, most preferably in the range from 44 to 80 N.

[0243] It is preferred that the multilayer film (F) has a tear resistance in the transverse direction, determined according to ASTM D1922, in the range from 8.0 to 50.0 N, more preferably in the range from 9.0 to 40.0 N, most preferably in the range from 10.0 to 30.0 N.

[0244] It is preferred that the multilayer film (F) has a sealing strength, determined according to ASTM F2029 and ASTM F88, in the range from 15 to 50 N, more preferably in the range from 16 to 40 N, most preferably in the range from 17 to 30 N.

[0245] It is preferred that the multilayer film (F) has a whiteness index, determined according to ASTM E313, in the range from 60.0 to 100.0, more preferably in the range from 70.0 to 95.0.

[0246] It is preferred that the multilayer film (F) has a total light transmittance value, determined according to ASTM D1003, in the range from 0.0 to 5.0%, more preferably in the range from 0.0 to 3.0%, most preferably in the range from 0.0 to 2.5%. E X A M P L E S

[0247] 1. Determination Methods

[0248] The following definitions of terms and determination methods apply for the above general description of the invention as well as to the below examples unless otherwise defined.

[0249] Melt flow rate

[0250] The melt flow rate (MFR) was determined according to ISO 1133 and is indicated in g / 10 min. The MFR is an indication of the flowability, and hence the processability, of the polymer. The higher the melt flow rate, the lower the viscosity of the polymer. The MFR5 of polyethylene was measured at a temperature of 190 °C and a load of 5 kg and the MFR2 of polyethylene at a temperature of 190 °C and a load of 2. 16 kg.

[0251] Density

[0252] Density of the polymer was measured according to ISO 1183-1:2004 Method A on compression moulded specimen prepared according to EN ISO 1872-2 (Feb 2007) and is given in kg / m3.

[0253] Comonomer content

[0254] Quantitative nuclear-magnetic resonance (NMR) spectroscopy was used to quantify the comonomer content of the polymers.

[0255] Quantitative13C {1H} NMR spectra recorded in the molten-state using a Bruker Advance III 500 NMR spectrometer operating at 500. 13 and 125.76 MHz for 'H and13C respectively. All spectra were recorded using a13C optimised 7 mm magic-angle spinning (MAS) probehead at 150 °C using nitrogen gas for all pneumatics. Approximately 200 mg of material was packed into a 7 mm outer diameter zirconia MAS rotor and spun at 4 kHz. This setup was chosen primarily for the high sensitivity needed for rapid identification and accurate quantification. {klimke06, parkinson07, castignolles09} Standard single-pulse excitation was employed utilising the NOE at short recycle delays {pollard04, klimke06} and the RS-HEPT decoupling scheme {fillipO5,griffmO7}. A total of 1024 (Ik) transients were acquired per spectra. Quantitative13C{1H} NMR spectra were processed, integrated and relevant quantitative properties determined from the integrals. All chemical shifts are internally referenced to the bulk methylene signal (5+) at 30.00 ppm.

[0256] The amount of ethylene was quantified using the integral of the methylene (5+) sites at 30.00 ppm accounting for the number of reporting sites per monomer:

[0257] E= I5+ / 2 the presence of isolated comonomer units is corrected for based on the number of isolated comonomer units present:

[0258] Etotal = E + (3*B + 2*H) / 2 where B and H are defined for their respective comonomers. Correction for consecutive and non-consecutive commoner incorporation, when present, is undertaken in a similar way. Characteristic signals corresponding to the incorporation of 1 -butene were observed and the comonomer fraction calculated as the fraction of 1 -butene in the polymer with respect to all monomer in the polymer: fBtotal = (Btotal / (Etotal + Btotal + Htotal))

[0259] The amount isolated 1 -butene incorporated in EEBEE sequences was quantified using the integral of the *B2 sites at 38.3 ppm accounting for the number of reporting sites per comonomer:

[0260] B = I„B2

[0261] If no other signals indicative of other comonomer sequences, i.e. consecutive comonomer incorporation, were observed, the total 1 -butene comonomer content was calculated based solely on the amount of isolated 1 -butene sequences:

[0262] Btotal = B

[0263] The amount consecutively incorporated 1 -butene in EEBBEE sequences was quantified using the integral of the aaB2B2 site at 39.4 ppm accounting for the number of reporting sites per comonomer:

[0264] BB = 2 * IaaB2B2

[0265] The amount non consecutively incorporated 1 -butene in EEBEBEE sequences was quantified using the integral of the PPB2B2 site at 24.7 ppm accounting for the number of reporting sites per comonomer:

[0266] BEB = 2 * IPPB2B2 Due to the overlap of the *B2 and *PB2B2 sites of isolated (EEBEE) and non-consecutivly incorporated (EEBEBEE) 1 -butene respectively the total amount of isolated 1 -butene incorporation is corrected based on the amount of non-consecutive 1 -butene present: B = I„B2 - 2 * IppB2B2

[0267] The total 1 -butene content was calculated based on the sum of isolated, consecutive and non consecutively incorporated 1 -butene:

[0268] Btotal = B + BB + BEB

[0269] The total mole fraction of 1 -butene in the polymer was then calculated as: fB = (Btotal / ( Etotal + Btotal + Htotal)

[0270] Characteristic signals corresponding to the incorporation of 1 -hexene were observed and the comonomer fraction calculated as the fraction of 1 -hexene in the polymer with respect to all monomer in the polymer: fHtotal = (Htotal / (Etotal + Btotal + Htotal)

[0271] The amount isolated 1 -hexene incorporated in EEHEE sequences was quantified using the integral of the *B4 sites at 39.9 ppm accounting for the number of reporting sites per comonomer:

[0272] H = I.B4

[0273] The amount consecutively incorporated 1 -hexene in EEHHEE sequences was quantified using the integral of the aaB4B4 site at 40.5 ppm accounting for the number of reporting sites per comonomer:

[0274] HH = 2 * IaaB4B4

[0275] The amount non consecutively incorporated 1 -hexene in EEHEHEE sequences was quantified using the integral of the PPB4B4 site at 24.7 ppm accounting for the number of reporting sites per comonomer:

[0276] HEH = 2 * IPPB4B4

[0277] The total mole fraction of 1 -hexene in the polymer was then calculated as: fH = (Htotal / (Etotal + Btotal + Htotal)

[0278] The amount of ethylene was quantified using the integral of the bulk methylene (5+) sites at 30.00 ppm. This integral included the y site as well as the 3B4 sites from 1- hexene. The total ethylene content was calculated based on the bulk integral and compensating for the observed 1 -butene and 1 -hexene sequences and end-groups:

[0279] E= I5+ / 2 Characteristic signals resulting from saturated end-groups were observed. The content of such saturated end-groups was quantified using the average of the integral of the signals at 22.8 and 32.2 ppm assigned to the 2s and 3s sites respectively:

[0280] S = (1 / 2)*(I2S+ I3S)

[0281] The presence of isolated comonomer units is corrected for based on the number of comonomer units and saturated end-groups present:

[0282] Etotal = E + (§ / 2)*B + (2 / 2)*H + (1 / 4)*HH + (3 / 4)*HEH + (3 / 2)*S

[0283] The mole percent comonomer incorporation is calculated from the mole fraction:

[0284] B [mol%] = 100 * fB

[0285] H [mol%] = 100 * fH

[0286] The weight percent comonomer incorporation is calculated from the mole fraction:

[0287] B [wt%] = 100 * (fB * 56.11) / ((fB * 56.11) + (fH * 84.16) + ((l-(fB + fH)) * 28.05))

[0288] H [wt%] = 100 * (fH * 84.16) / ((fB * 56.11) + (fH * 84.16) + ((l-(fB + fH)) * 28.05))

[0289] References: klimke06

[0290] Klimke, K., Parkinson, M., Piel, C., Kaminsky, W., Spiess, H.W., Wilhelm, M., Macromol. Chem. Phys. 2006;207:382. parkinson07

[0291] Parkinson, M., Klimke, K., Spiess, H.W., Wilhelm, M., Macromol. Chem. Phys. 2007;208:2128. pollard04

[0292] Pollard, M., Klimke, K., Graf, R., Spiess, H.W., Wilhelm, M., Sperber, O., Piel, C., Kaminsky, W., Macromolecules 2004;37:813. filip05

[0293] Filip, X., Tripon, C„ Filip, C„ J. Mag. Resn. 2005, 176, 239 griffin07

[0294] Griffin, J.M., Tripon, C., Samoson, A., Filip, C., and Brown, S.P., Mag. Res. in Chem. 2007 45, SI, S198 castignolles09

[0295] Castignolles, P., Graf, R., Parkinson, M., Wilhelm, M., Gaborieau, M., Polymer 50 (2009) 2373 busicoOl

[0296] Busico, V., Cipullo, R., Prog. Polym. Sci. 26 (2001) 443 busico97

[0297] Busico, V., Cipullo, R., Monaco, G., Vacatello, M., Segre, A.L., Macromoleucles 30 (1997) 6251 zhou07

[0298] Zhou, Z., Kuemmerle, R., Qiu, X., Redwine, D., Cong, R., Taha, A., Baugh, D. Winniford, B„ J. Mag. Reson. 187 (2007) 225 busico07

[0299] Busico, V., Carbonniere, P., Cipullo, R., Pellecchia, R., Severn, J., Talarico, G., Macromol.

[0300] Rapid Commun. 2007, 28, 1128 resconiOO

[0301] Resconi, L., Cavallo, L., Fait, A., Piemontesi, F., Chem. Rev. 2000, 100, 1253

[0302] Molecular Weight

[0303] (1) GPC conventional method (all PE other than LDPE)

[0304] Unless otherwise indicated, the GPC conventional method was used for the measurement of ethylene polymers - except for LDPE.

[0305] Molecular weight averages (Mz, Mwand Mn), molecular weight distribution (MWD) and its broadness, described by polydispersity index, PDI= Mw / Mn(wherein Mnis the number average molecular weight and Mwis the weight average molecular weight) were generally determined by Gel Permeation Chromatography (GPC) according to ISO 16014-4:2003 and ASTM D 6474-12 using the following formulas:

[0306] For a constant elution volume interval AVi, where A and Mi are the chromatographic peak slice area and polyolefin molecular weight (MW), respectively associated with the elution volume, Vi, where N is equal to the number of data points obtained from the chromatogram between the integration limits. A high temperature GPC instrument, equipped with either infrared (IR) detector (IR4 or IR5 from PolymerChar (Valencia, Spain)) or differential refractometer ((RI) from Agilent Technologies, equipped with 3 x Agilent-PLgel Olexis and lx Agilent-PLgel Olexis Guard columns) was used. As mobile phase 1,2,4-trichlorobenzene (TCB) stabilized with 250 mg / L 2,6-Di tert-butyl-4-methyl-phenol) was used. The chromatographic system was operated at column temperature of 160 °C and detector at 160 °C and at a constant flow rate of 1 mL / min. 200 pL of sample solution was injected per analysis. Data collection was performed using either Agilent Cirrus software version 3.3 or PolymerChar GPC-IR control software. The column set was calibrated using 19 narrow MWD polystyrene (PS) standards in the range of from 0.5 kg / mol to 11 500 kg / mol. The PS standards were dissolved at room temperature over several hours. The conversion of the polystyrene peak molecular weight to polyolefin molecular weights is accomplished by using the Mark-Houwink equation and the following Mark-Houwink constants:

[0307] KPS = 19 x 103mL / g, aPS= 0.655

[0308] KPE = 39 x 10"3mL / g, «PE = 0.725

[0309] A third order polynomial fit was used to fit the calibration data.

[0310] All samples were prepared in the concentration range of around 1 mg / ml and dissolved at 160 °C for 3 (three) hours for PE in fresh distilled TCB stabilized with 250 ppm BHT (butylated hydroxytoluene) under continuous gentle shaking with N2 gas purging.

[0311] (2) GPC viscosity method (LDPE)

[0312] Molecular weight averages (Mz, Mwand Mn), molecular weight distribution (MWD) of LDPE were measured by GPC-viscosity method using universal calibration. Molecular weight averages (Mw, Mn), Molecular weight distribution (MWD) and its broadness, described by polydispersity index, PDI= Mw / Mn(wherein Mnis the number average molecular weight and Mwis the weight average molecular weight) were determined by Gel Permeation Chromatography (GPC) according to ISO 16014-4 2019. A PL 220 (Polymer Laboratories) GPC equipped with an IR4 infrared detector, an online four capillary bridge viscometer (PL-BV 400-HT) was used. 3x Olexis and lx Olexis Guard columns from Polymer Laboratories as stationary phase and 1,2,4-trichlorobenzene (TCB, stabilized with 250 mg / L 2,6-Di tert butyl-4-methyl-phenol) as mobile phase at 160 °C and at a constant flow rate of 1 mL / min was applied. 200 pL of sample solution were injected per analysis. The corresponding detector constant of the viscometer as well as the inter-detector delay volumes were determined with a narrow PS standard (MWD = 1.01) with a molar mass of 132900 g / mol and an intrinsic viscosity of 0.4789 dl / g. The detector constant of the IR4 detector was determined using NIST1475a with dn / dc of 0.094 cm3 / g.

[0313] The column set was calibrated using universal calibration (according to ISO 16014-2:2019) with at least 15 narrow MWD polystyrene (PS) standards in the range of 0.5 kg / mol to 11600 kg / mol. The corresponded intrinsic viscosities of the PS standards were calculated from their corresponding concentration (IR4), online viscometer signals, and determined detector constants for polystyrene. For low molecular weight PS with a molar mass below 3000 g / mol the initial weight out concentration is used, due to end group effects in the IR detector.

[0314] The molecular weight of the sample (M2) at each chromatographic slice using the universal calibration approach can be calculated by following correlation: logMi[r|i] = VR = logM2[r|2] with: Mi Molar mass of PS r| 1 intrinsic viscosity of the PS

[0315] M2Molar mass of sample r|2 intrinsic viscosity of sample

[0316] VR Retention volume

[0317] All data processing and calculation was performed using the Cirrus Multi-Offline SEC- Software Version 3.2 (Polymer Laboratories a Varian inc. Company).

[0318] All samples were prepared by dissolving 5.0 - 9.0 mg of polymer in 8 m (at 160 °C) of stabilized TCB (same as mobile phase) 3 hours for PE at max. 160 °C under continuous gentle shaking.

[0319] Optical properties

[0320] The optical properties were determined on the multilayer film produced in the experimental section.

[0321] 1. Total Light Transmittance

[0322] Total light transmittance of plastics film was determined according to ASTM D 1003 and ISO 14782. Total transmittance is the ratio of transmitted light to the incident light, measured using hazemeter. This property is influenced by the absorption and reflection properties. The total transmitted light consists of the directly transmitted and the diffused components. 2 Whiteness Index

[0323] Whiteness index (WI) of fdm was determined according to ASTM E 313. The whiteness index is expressed as a single-number scale that was computed from colorimetric data, that indicates the degree of departure of an object color from that of a preferred white. It correlates with visual ratings of whiteness of white and near white specimen, viewed in daylight by an observer with normal color vision.

[0324] In this procedure, a 10° observer, D65 illuminant, and three degrees color parameters are used. The combination of measurement and calculation leading to indices of whiteness index is a psychophysical process - that is the procedures specified are designed to provide numbers correlating with visual estimates made under specified typical observation conditions.

[0325] Film tensile properties (Tensile Modulus, Tensile Strength, Elongation at Break)

[0326] Tensile properties of films were determined at 23°C according to ISO 527-3 with a specimen Type 2 using blown films. Tensile modulus in machine direction (MD) and tensile modulus in transverse direction (TD) were determined as 1 % secant modulus with 5 mm / min test speed and 50 mm gauge length according to ASTM D882.

[0327] Tensile stress at break or Elongation at break of films were determined according to ISO 527-3 specimen Type 2 with 50 mm gauge length and 500 mm / min test speed.

[0328] Recyclate tensile properties (Tensile Modulus, Tensile Strength, Elongation at Break) The tensile properties were determined according to ISO 527-2:2012, on a specimen of Tensile type 1A prepared in accordance with ISO 294-1 and ISO 17855-2 using a melt temperature of 190 °C and 10 bar specific back pressure during compression molding. Tensile modulus was determined according to ISO 527-2 / 1 A at 1 mm / min and 23°C. To determine tensile stress at yield, a speed of 50 mm / min was used.

[0329] Flexural modulus

[0330] The flexural modulus was determined in 3 -point-bending according to ISO 178 on molded specimens of 80 x 10 x 4 mm3prepared by compression molding in accordance with ISO 294-1 and ISO 17855-2 using a melt temperature of 190°C. Charpy impact strength (NIS)

[0331] The Charpy notched impact strength (NIS) was measured according to ISO 179 leA at +23 °C or -20 °C, using moulded bar test specimens of 80x 10x4 mm3prepared by compression molding in accordance with ISO 294-1 and ISO 17855-2 using a melt temperature of 190 °C.

[0332] Puncture Resistance

[0333] Protrusion Puncture Resistance testing was conducted according to ASTM D5748 on the multilayer fdms produced in the experimental section. This test method determines the resistance of a fdm sample to the penetration of a probe with specific size of 19mm diameter pear-shaped TFE fluorocarbon coated at a standard low rate, a single test velocity (250 mm / min). Performed at standard conditions, the test method imparts a biaxial stress loading. Cut the film specimens 150mmxl50mm to fit into the jig and conditioning done at 23±2°C at 50+5% relative humidity.

[0334] The Puncture Resistance Force (N) is the maximum force or highest force observed during the test and Puncture Resistance Energy (J) is the energy used until the probe breaks the test specimen, both were measured using the high accuracy 500N loadcell and crosshead position sensor.

[0335] DDI

[0336] Dart-drop impact was measured according to ASTM DI 709, method A on the multilayer films produced in the experimental section. A dart with a 38 mm diameter hemispherical head was dropped from a height of 0.66 m onto a film clamped over a hole. Successive sets of twenty specimens were tested. One weight was used for each set and the weight is increased (or decreased) from set to set by uniform increments. The weight resulting in failure of 50 % of the specimens was calculated and reported.

[0337] DDI per unit thickness (in g / micron) was calculated by dividing DDI (in gram) to the thickness of film (in micron).

[0338] Tear resistance

[0339] Elmendorf tear strength in machine direction (MD) and in transverse direction (TD) were measured on the multilayer film according to ASTM DI 922 and reported in Newton (N) or Gram -force (gf).

[0340] Gloss

[0341] Gloss was measured on films, prepared as described in the example section below according to ISO 2813 at an angle of 60°. Gloss values were recorded and reported as gloss units (GU).

[0342] Sealing strength

[0343] In principle, heat seal was formed by bonding two films (polymeric) in the way that surfaces are pressed together into a close contact while being at least in partially molten. This test method also covers the evaluation part after the heat seal process is performed. The force required to separate a test strip of film containing the seal is measured using UTM (also to identify the mode of specimen failure). Following the ASTM F 2029; ASTM F 88 standard, a tested specimen with a preferred film thickness of 50 microns where the sealed surfaces were selected. Samples were conditioned for at least 24hrs in the case of PE after sealing at 23±2°C and 50±5 % relative humidity. For testing, a minimum of five specimens were used for each seal temperature. The term “seal initiation temperature” (SIT) is specified as the “heat seal initiation temperature at 5N” and it refers to the temperature at which a seal is formed that will have a seal strength of 5N after cooling. The temperature at which a heat seal forms immediately after the sealing operation (sealing time 1.0 seconds, sealing pressure 3 bar for less than 65 micron film and sealing time 1.5 seconds for 65 micron and above thickness), the strength of the heat seal being measured at a specified time interval (at least 24 hrs after completion of the sealing cycle and after the seal had cooled to ambient temperature and reached maximum strength) were determined.

[0344] Ash content

[0345] The ash content of the recyclate was determined by combusting the material in a weighed platinum crucible. About 100 grams of polymer is weighed into the crucible. The crucible is then heated in a Bunsen burner flame so that the polymer slowly bums at 600 °C. After the polymer is completely burned the crucible is cooled, dried and weighed. The ash content is then the weight of the residue divided by the weight of the polymer sample. At least two measurements are made, and the average values were taken as final ash content. 2. Examples

[0346] 2.1 Materials used

[0347] PCR is a post-consumer recyclate derived from courier bag waste, commercially available from Shanghai Tianqiang Environmental Protection Technology Co. Ltd (CN) under the trade name r-PE158. r-PE158 has an MFR2 of 0.8 g / 10 min, a density of 970 kg / m3, a tensile stress@yield of 9.5 MPa, a tensile strain@yield of 12.8%, a tensile modulus of 240 MPa, a tensile stress@break of 19.2 MPa, an elongation@break of 550%, a flexural modulus of 260 MPa, a Charpy NIS @+23 °C of 53.5 kJ / m2, and an ash content of 3.8 wt.-%.

[0348] LDPE is a low-density polyethylene based on the tubular technology, commercially available from Abu Dhabi Polymers Co. Ltd (AE) under the trade name FT6236. FT6236 has an MFR2 of 2.0 g / 10 min, a density of 923 kg / m3and a Mw / Mn of approximately 7 (determined using the GPC viscosity method).

[0349] MB1 is a TiCE masterbatch composition containing 60 wt.-% of TiO? in a polyethylene carrier, commercially available from Astra PolyMers (SA) under the trade name A4000.

[0350] MB2 is a black-colour masterbatch in a polyethylene carrier containing about 40 wt.-% of carbon black, commercially available from Astra PolyMers (SA) under the trade name AS1458.

[0351] PEI is a unimodal C2C4 copolymer, commercially available from SABIC Global Technologies B.V (NL) under the trade name SABIC LLDPE 118W.

[0352] PE2 is a unimodal C2C6 copolymer, commercially available from ExxonMobil (US) under the trade name Enable 2703 MC.

[0353] PE3 corresponds to IE2 of WO 2021 / 013552, is a bimodal copolymer, comprising a C2C4 fraction and a C2C4 fraction. PE4 is a bimodal linear low density polyethylene comprising a C2C4 fraction and a C2C4 fraction, commercially available from Abu Dhabi Polymers Co. Ltd (Borouge) (AE) under the trade name Borstar® FB2230.

[0354] PE5 corresponds to CE1 ofWO 2024 / 028421 Al. PE4 is a bimodal copolymer, comprising a C2C4 fraction and a C2C6 fraction.

[0355] PE6 corresponds to IE2 of WO 2024 / 028421 Al. PE3 is a bimodal copolymer, comprising a C2C4 fraction and a C2C6 fraction.

[0356] The properties of PEI to PE6 are given in Table 1.

[0357] 2.2 Compounding of Inventive and Comparative Multilayer films

[0358] The compositions for each layer were pre-mixed as dry blends of pellets according to the recipes given in Table 2.

[0359] 3 -layer fdms were produced on a Polyrema (Reifeinhauser blown film line with internal bubble cooling system) having an output of 140 kg / h. The die diameters were 180 mm, the die gap was 1.8 mm, the blow up ratio (BUR) was 2.5: 1, bubble cooling was IBC and the cooling air temperature was 15 °C. For each layer, extruder zone 1 had a temperature of 160 °C, the heating zones had temperatures of 200 to 220 °C and the melt temperature was 210 to 220 °C. The resultant films had a thickness of 50 pm and layers A:B:C were in a 1 :2: 1 ratio for examples CE1 to CE3, IE1 and IE2 and a 1:3: 1 ratio for IE3. The performance properties of the inventive and comparative films are given in Table 3.

[0360] Table 2 Recipes for inventive and comparative examples Table 3 Performance of the inventive and comparative multilayer films

[0361] As can be seen from Table 3, the inventive multilayer films have markedly improved DDI, improved tensile strength, and improved puncture resistance, relative to the comparative multilayer films.

Claims

C L A I M S1. A multilayer film (F), comprising, in the given order, the following layers:(A) a skin layer, comprising at least 70 wt.-%, based on the total weight of the skin layer, of a polyethylene or mixture of polyethylenes,(B) a core layer, comprising the following components: i) from 1.0 to 60.0 wt.-%, relative to the total weight of the core layer, of a multimodal polymer (Bl) of ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and Cs-Cs alpha olefins, wherein the multimodal polymer (Bl) has a density, determined according to ISO 1183, in the range from 910 to 945 kg / m3, and ii) from 40.0 to 99.0 wt.-%, relative to the total weight of the core layer, of a polyethylene-based post-consumer recyclate (B2) having a density, determined according to ISO 1183, in the range from 930 to 1050 kg / m3; wherein the combined amounts of the multimodal polymer (Bl) and the polyethylene-based post-consumer recyclate (B2) add up to at least 90 wt.-%, relative to the total weight of the core layer, and(C) a sealing layer, comprising at least 75 wt.-%, based on the total weight of the sealing layer, of a polyethylene or mixture of polyethylenes.

2. The multilayer film (F) according to claim 1, wherein the polyethylene-based postconsumer recyclate (B2) has one or more, preferably all, of the following properties: a) a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.20 to 10.0 g / 10 min, more preferably in the range from 0.30 to 5.0 g / 10 min, most preferably in the range from 0.40 to 3.0 g / 10 min; b) a density, determined according to ISO 1183, in the range from 935 to 1020 kg / m3, most preferably in the range from 940 to 1000 kg / m3; and c) an ash content, determined according to the method given in the determination methods, in the range from 1.0 to 12.0 wt.-%, more preferably in the range from 1.5 to 11.0 wt.-%, most preferably in the range from 2.0 to 10.0 wt.-%.

3. The multilayer film (F) according to claim 1 or claim 2, wherein the multimodal polymer (Bl) has one or more, preferably all, of the following properties: a) a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.10 to 3.0 g / 10 min, more preferably in the range from 0.12 to 2.0 g / 10 min, most preferably in the range from 0.15 to 1.6 g / 10 min; b) a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 6.0 g / 10 min, more preferably in the range from 0.45 to 5.0 g / 10 min, most preferably in the range from 0.50 to 4.5 g / 10 min; c) a density, determined according to ISO 1183, in the range from 912 to 935 kg / m3, yet more preferably in the range from 913 to 930 kg / m3, most preferably in the range from 913 to 927 kg / m3; and d) a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.0 to 6.0 mol-%, more preferably in the range from 2.5 to 5.5 mol-%, most preferably in the range from 3.0 to 5.0 mol-%.

4. The multilayer film (F) according to any one of the preceding claims, wherein the multimodal polymer (Bl) is a first multimodal ethylene- 1 -butene copolymer (Bia) having one or more, preferably all, of the following properties: a) a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.50 to 3.0 g / 10 min, more preferably in the range from 0.60 to 2.0 g / 10 min, most preferably in the range from 0.70 to 1.6 g / 10 min; b) a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 1.5 to 6.0 g / 10 min, more preferably in the range from 2.0 to 5.0 g / 10 min, most preferably in the range from 2.5 to 4.5 g / 10 min;c) a density, determined according to ISO 1183, in the range from 910 to 920 kg / m3, more preferably in the range from 912 to 918 kg / m3, most preferably in the range from 913 to 917 kg / m3; d) a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 2.0 to 8.0, more preferably in the range from 3.0 to 7.0, most preferably in the range from 4.0 to 6.0; and e) a 1-butene content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.5 to 6.0 mol-%, more preferably in the range from 3.0 to 5.5 mol-%, most preferably in the range from 3.5 to 5.0 mol-%.

5. The multilayer fdm (F) according to any one of claims 1 to 3, wherein the multimodal polymer (Bl) is a second multimodal ethylene- 1-butene copolymer (B lb) having one or more, preferably all, of the following properties: a) a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.10 to 1.00 g / 10 min, more preferably in the range from 0.12 to 0.50 g / 10 min, most preferably in the range from 0.15 to 0.30 g / 10 min; b) a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 2.0 g / 10 min, more preferably in the range from 0.50 to 1.5 g / 10 min, most preferably in the range from 0.60 to 1.2 g / 10 min; c) a density, determined according to ISO 1183, in the range from 918 to 945 kg / m3, more preferably in the range from 920 to 935 kg / m3, most preferably in the range from 921 to 925 kg / m3; d) a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 8.0 to 30.0, more preferably in the range from 9.0 to 27.0, most preferably in the range from 10.0 to 24.0; and e) a 1-butene content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.5 to 6.0 mol-%, more preferably in the range from 3.0 to 5.5 mol-%, most preferably in the range from 3.5 to 5.0 mol-%.

6. The multilayer film (F) according to any one of the preceding claims, wherein the multimodal polymer (Bl) is a multimodal ethylene- 1 -butene- 1 -hexene terpolymer (Bic) having one or more, preferably all, of the following properties: a) a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.10 to 1.00 g / 10 min, more preferably in the range from 0.11 to 0.50 g / 10 min, most preferably in the range from 0.12 to 0.30 g / 10 min; b) a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 2.0 g / 10 min, more preferably in the range from 0.45 to 1.5 g / 10 min, most preferably in the range from 0.50 to 1.0 g / 10 min; c) a density, determined according to ISO 1183, in the range from 918 to 945 kg / m3, more preferably in the range from 920 to 935 kg / m3, most preferably in the range from 921 to 925 kg / m3; d) a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 8.0 to 30.0, more preferably in the range from 9.0 to 27.0, most preferably in the range from 10.0 to 24.0; e) a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.0 to 6.0 mol-%, more preferably in the range from 2.5 to 5.0 mol-%, most preferably in the range from 3.0 to 4.8 mol-%; f) a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 1.0 to 4.0 mol-%, more preferably in the range from 1.3 to 3.0 mol-%, most preferably in the range from 1.5 to 2.5 mol-%; and g) a 1 -hexene (C6) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 0.5 to 2.0 mol-%, more preferably in the range from 0.8 to 1.9 mol-%, most preferably in the range from 1.0 to 1.8 mol-%.

7. The multilayer film (F) according to any one of the preceding claims, wherein the skin layer comprises: a) from 20.0 to 70.0 wt.-%, relative to the total weight of the skin layer, of an ethylene copolymer (Al) containing ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and C5-C8alpha olefins and having a density, determined according to ISO 1183, in the range from 910 to 945 kg / m3; b) from 5.0 to 30.0 wt.-%, relative to the total weight of the skin layer, of one or more inorganic pigments (A2), wherein the one or more inorganic pigments are preferably white inorganic pigments; c) from 10.0 to 50.0 wt.-%, relative to the total weight of the skin layer, of one or more further polyethylenes (A3) that are different to the ethylene copolymer (Al); and d) optionally, from 0.0 to 5.0 wt.-%, relative to the total weight of the skin layer, of one or more further additives (A4) other than inorganic pigments, wherein the total weight of the ethylene copolymer (Al), the one or more inorganic pigments (A2), the one or more further polyethylenes (A3), and the optional one or more further additives (A4) add up to at least 90 wt.-%, more preferably at least 95 wt.-%, yet more preferably at least 98 wt.-%, relative to the total weight of the skin layer, most preferably the skin layer consists of the ethylene copolymer (Al), the one or more inorganic pigments (A2), the one or more further polyethylenes (A3), and the optional one or more further additives (A4).

8. The multilayer film (F) according to any one of the preceding claims, wherein the sealing layer comprises: a) from 30.0 to 89.9 wt.-%, relative to the total weight of the sealing layer, of an ethylene copolymer (Cl) containing ethylene, 1 -butene and optionally one or more further comonomers selected from the group consisting of propylene and C5-C8alpha olefins and having a density, determined according to ISO 1183, in the range from 910 to 945 kg / m3;b) from 0.1 to 5.0 wt.-%, relative to the total weight of the sealing layer, of one or more pigments (C2), wherein the one or more pigments are preferably black pigments; c) from 10.0 to 69.9 wt.-%, relative to the total weight of the sealing layer, of one or more further polyethylenes (C3) that are different to the ethylene copolymer (Cl); and d) optionally, from 0.0 to 5.0 wt.-%, relative to the total weight of the sealing layer, of one or more further additives (C4) other than pigments, wherein the total weight of the ethylene copolymer (Cl), the one or more pigments (C2), the one or more further polyethylenes (C3), and the optional one or more further additives (C4) add up to at least 90 wt.-%, more preferably at least 95 wt.-%, yet more preferably at least 98 wt.-%, relative to the total weight of the sealing layer, most preferably the sealing layer consists of the ethylene copolymer (Cl), the one or more pigments (C2), the one or more further polyethylenes (C3), and the optional one or more further additives (C4).

9. The multilayer fdm (F) according to any one of the preceding claims, wherein the ethylene copolymer (Al) and / or the ethylene copolymer (Cl) has / have one or more, preferably all, of the following properties: a) a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.10 to 3.0 g / 10 min, more preferably in the range from 0.12 to 2.0 g / 10 min, most preferably in the range from 0.15 to 1.6 g / 10 min; b) a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 0.40 to 6.0 g / 10 min, more preferably in the range from 0.45 to 5.0 g / 10 min, most preferably in the range from 0.50 to 4.5 g / 10 min; c) a density, determined according to ISO 1183, in the range from 910 to 945 kg / m3, more preferably in the range from 912 to 935 kg / m3, yet more preferably in the range from 913 to 930 kg / m3, most preferably in the range from 913 to 927 kg / m3; andd) a total comonomer content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 2.0 to 6.0 mol-%, more preferably in the range from 2.5 to 5.5 mol-%, most preferably in the range from 3.0 to 5.0 mol-%; and e) is a multimodal ethylene- 1 -butene copolymer.

10. The multilayer fdm (F) according to any one of the preceding claims, wherein at least one of the one or more further polyethylenes (A3) and / or at least one of the one or more further polyethylenes (C3), is a low-density polyethylene (LDPE) having one or more, preferably all, of the following properties: a) a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2.16 kg, in the range from 0.5 to 4.0 g / 10 min, more preferably in the range from 1.0 to 3.0 g / 10 min, most preferably in the range from 1.5 to 2.5 g / 10 min; b) a density, determined according to ISO 1183, in the range from 910 to 935 kg / m3, more preferably 915 to 930 kg / m3, most preferably in the range from 920 to 925 kg / m3; and c) a molecular weight distribution (Mw / Mn), determined according to the viscosity GPC method given in the determination methods, in the range from 3.0 to 12.0, more preferably in the range from 4.0 to 10.0, most preferably in the range from 5.0 to 9.0.

11. The multilayer fdm (F) according to any one of the preceding claims, wherein at least one of the one or more further polyethylenes (A3) and / or at least one of the one or more further polyethylenes (C3), is a linear low-density polyethylene (LLDPE) having one or more, preferably all, of the following properties: a) a melt flow rate MFR2, determined according to ISO 1133 at a temperature of 190 °C and a load of 2. 16 kg, in the range from 0.3 to 3.0 g / 10 min, more preferably in the range from 0.5 to 2.5 g / 10 min, most preferably in the range from 0.7 to 2.0 g / 10 min; b) a melt flow rate MFR5, determined according to ISO 1133 at a temperature of 190 °C and a load of 5.0 kg, in the range from 1.0 to 8.0 g / 10 min, morepreferably in the range from 1.5 to 7.0 g / 10 min, most preferably in the range from 2.0 to 6.0 g / 10 min; c) a density, determined according to ISO 1183, in the range from 909 to 923 kg / m3, more preferably in the range from 911 to 921 kg / m3, most preferably in the range from 913 to 919 kg / m3; d) a 1 -butene (C4) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 0.05 to 1.00 mol-%, more preferably in the range from 0.10 to 0.90 mol-%, most preferably in the range 0.20 to 0.80 mol-%; e) a 1 -hexene (C6) content, determined according to quantitative13C-NMR spectroscopic analysis, in the range from 1.5 to 4.8 mol-%, more preferably in the range from 2.0 to 4.3 mol-%, most preferably in the range from 2.5 to 3.5 mol-%; f) a molecular weight distribution (Mw / Mn), determined according to the conventional GPC method given in the determination methods, in the range from 2.0 to 7.0, more preferably in the range from 2.5 to 6.0, most preferably in the range from 3.0 to 5.0; g) a bimodal structure wherein the linear low-density polyethylene (LLDPE) consists of a first polymer fraction that is a copolymer of ethylene and a first C4- C8alpha olefin and a second polymer fraction that is a copolymer of ethylene and a second C4-C8 alpha olefin, wherein the first C4-C8 alpha olefin is different to the second C4-C8 alpha olefin.

12. The multilayer film (F) according to any one of the preceding claims, wherein the polyethylene-based post-consumer recyclate (B2) is present in an amount in the range from 20.0 to 80.0 wt.-%, more preferably in the range from 25.0 to 65 wt.-%, most preferably in the range from 30.0 to 60 wt.-%, relative to the total weight of the multilayer film (F), and / or wherein: a) the skin layer has a thickness in the range from 5 to 40% of the total thickness of the multilayer film (F);b) the core layer has a thickness in the range from 20 to 90% of the total thickness of the multilayer film (F); and c) the sealing layer has a thickness in the range from 5 to 40% of the total thickness of the multilayer film (F).

13. The multilayer film (F) according to any one of the preceding claims, having a thickness in the range from 15 to 100 pm, more preferably in the range from 20 to 95 pm, most preferably in the range from 25 to 90 pm.

14. The multilayer film (F) according to any one of the preceding claims, having one or more, preferably all, of the following properties: a) a dart drop impact strength (DDI), determined according to ASTM D1709 method A, in the range from 2.0 to 6.0 g / pm, more preferably in the range from 2.2 to 5.5 g / pm, most preferably in the range from 2.7 to 5.0 g / pm; b) a tensile strength in the machine direction, determined according to ISO 527-3, in the range from 30 to 75 MPa, more preferably in the range from 32 to 70 MPa, most preferably in the range from 35 to 60 MPa; c) a puncture force at break, determined according to ASTM D5748, in the range from 30 to 100 N, more preferably in the range from 40 to 90 N, most preferably in the range from 44 to 80 N; and d) a tear resistance in the transverse direction, determined according to ASTM D1922, in the range from 8.0 to 50.0 N, more preferably in the range from 9.0 to 40.0 N, most preferably in the range from 10.0 to 30.0 N.

15. The multilayer film (F) according to any one of the preceding claims, having one or more, preferably both, of the following properties: a) whiteness index, determined according to ASTM E313, in the range from 60.0 to 100.0, more preferably in the range from 70.0 to 95.0; and b) a total light transmittance value, determined according to ASTM DI 003, in the range from 0.0 to 5.0%, more preferably in the range from 0.0 to 3.0%, most preferably in the range from 0.0 to 2.5%.

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