Patent Description:
Polyolefins, in particular polyethylene and polypropylene are increasingly consumed in large amounts in a wide range of applications, including packaging for food and other goods, fibres, automotive components, and a great variety of manufactured articles. The reason for this is not only a favourable price/performance ratio, but also the high versatility of these materials and a very broad range of possible modifications, which allows tailoring of end-use properties in a wide range of applications. Chemical modifications, copolymerisation, blending, drawing, thermal treatment and a combination of these techniques can convert common-grade polyolefins into valuable products with desirable properties. This has led to huge amounts of polyolefin materials being produced for consumer applications.

During the last decade, concern about plastics and the environmental sustainability of their use in current quantities has arisen. This has led to new legislation on disposal, collection and recycling of polyolefins. There have, in addition, been efforts in a number of countries to increase the percentage of plastic materials, which are recycled instead of being sent to landfill.

One major trend in the field of polyolefins is the use of recycled materials, which are derived from a wide variety of sources. Mechanical recycling of polymer waste from various collection systems is the main target of present developments in the field. The recycled plastics typically comprise several types of polymers. For recyclates of polyolefins, mixture of polypropylene (PP) and polyethylene (PE) are commonly seen and the content of PP/PE depends on not only the feedstock, but also on the recycling process. Furthermore, other polar polymers, e.g., ethylene vinylacetate (EVA), polyamide (PA), polyethylene terephthalare (PET), etc. may not be fully removed during sorting and stay in the pellet of polyolefine recyclate. As such, the mechanical performance of the mechanically recycled polyolefines is inferior to the virgin PP or PE. However, there is a strong need for recyclates having good mechanical properties. The prior art describes ways for improving the mechanical properties of recyclates.

<CIT> discloses polymer compositions comprising (A) <NUM>-<NUM> wt% polymer blend comprising (a1) polypropylene and (a2) polyethylene and polymer blend (A) is a recycled material; and (B) <NUM>-<NUM> wt% virgin random polypropylene copolymer.

<CIT> relates to a regenerated plastic particle. The regenerated plastic particle comprises the following components: modified recycled plastic, intumescent flame retardant, barium sulfate, graphene, antioxidant, brightener and plasticizer. The recycled plastic is modified by in-process compatilizer, toughener and chain extender.

<CIT> relates to the recycling of polyamide and polyolefin wastes and fiber reinforced plastic wastes. Particularly, to polymer blends and homogenous polymer agglomerates containing polyamide and polyolefin wastes or co- -extruded film wastes and glass fiber reinforced plastic wastes, and to a single-stage continuous process for the preparation of said agglomerate.

<CIT> relates to film compositions and articles including recycled elastomer. The compositions comprise one or more virgin polymers. Optionally, the films may also include one or more compatibilizers having compatibility with the polymers and a thermoplastic elastomer (TPE) such as a block copolymer with a hard block and a soft block. Multi- or mono-layer films are possible. The films are useful for packaging films or component films for consumer products.

<CIT> relates to a preparation method of waste plastic regenerated granules. The method includes the steps of: performing melting mixing to raw materials at <NUM> to <NUM>, the raw materials including, by weight, <NUM> to <NUM> parts of waste plastic, <NUM> to <NUM> parts of a thermal stabilizer, <NUM> to <NUM> parts of a composite flexibilizer, and <NUM> to <NUM> parts of a thermal dispersant; and successively performing extrusion, wire drawing, cooling and granule cutting.

The known polymer compositions comprising recycled materials still show some disadvantages. There is a great need for recyclate-based polymer compositions with improved mechanical properties, in particular improved Charpy Notch Impact Strength and Tensile strain at break.

It was the objective of the present invention to overcome the disadvantages of the polymer compositions according to the prior art. In particular, it was one object of the present invention to provide polymer compositions having a high toughness, expressed by the Charpy Notched Impact Strength and Tensile strain at break.

This objective has been solved by the polymer composition according to claim <NUM> of the present invention comprising at least the following components.

with the proviso that the weight proportions of components A) and B) add up to <NUM> wt.

Advantageous embodiments of the polymer composition in accordance with the present invention are specified in the dependent claims <NUM> to <NUM>.

Claim <NUM> of the present invention relates to a process for manufacturing a polymer composition according to any one of claims <NUM> to <NUM>, comprising the following steps:.

Claims <NUM> and <NUM> specify preferred embodiments of the process according to the present invention.

Claim <NUM> relates to the use of a virgin ethylene alkyl (meth)acrylate B) having the following properties.

Claim <NUM> refers to an article comprising the polymer composition according to the present invention.

The polymer compositions in accordance with the present invention comprise the components A) and B) and optionally additives. The requirement applies here that the components A) and B) and if present the additives add up to <NUM> wt. The fixed ranges of the indications of quantity for the individual components A) and B) and optionally the additives are to be understood such that an arbitrary quantity for each of the individual components can be selected within the specified ranges provided that the strict provision is satisfied that the sum of all the components A), B) and optionally the additives add up to <NUM> wt.

For the purposes of the present description and of the subsequent claims, the term "recycled" is used to indicate that the material is recovered from post-consumer waste and/or industrial waste. Namely, 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 and been through the hands of a consumer; while industrial waste refers to the manufacturing scrap which does normally not reach a consumer. In the gist of the present invention "recycled polymers" may also comprise up to <NUM> wt. -%, preferably up to <NUM> wt. -%, more preferably up to <NUM> wt. -% and even more preferably up to <NUM> wt. -% based on the overall weight of the recycled polymer of other components originating from the first use. Type and amount of these components influence the physical properties of the recycled polymer. The physical properties given below refer to the main component of the recycled polymer.

Typical other components originating from the first use are thermoplastic polymers, like polystyrene and PA <NUM>, talc, chalk, ink, wood, paper, limonene and fatty acids. The content of polystyrene (PS) and polyamide <NUM> (PA <NUM>) in recycled polymers can be determined by Fourier Transform Infrared Spectroscopy (FTIR) and the content of talc, chalk, wood and paper may be measured by Thermogravimetric Analysis (TGA).

The term "virgin" denotes the newly produced materials and/or objects prior to first use and not being recycled. In case that the origin of the polymer is not explicitly mentioned the polymer is a "virgin" polymer.

Where the term "comprising" is used in the present description and claims, it does not exclude other non-specified elements of major or minor functional importance. For the purposes of the present invention, the term "consisting of' is considered to be a preferred embodiment of the term "comprising of". If hereinafter a group is defined to comprise at least a certain number of embodiments, this is also to be understood to disclose a group, which preferably consists only of these embodiments.

The polymer composition in accordance with the present invention comprises as component A) <NUM> to <NUM> wt. -% based on the overall weight of the polymer composition of a polymer blend, comprising a1) polypropylene; a2) polyethylene; wherein the weight ratio of a1) to a2) is from <NUM>:<NUM> to <NUM>:<NUM>; and wherein the polymer blend A) is a recycled material.

Preferred embodiments of component A) will be discussed in the following.

According to one preferred embodiment in accordance with the present invention component A) comprises <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% and more preferably <NUM> to <NUM> based on the overall weight of component A) of polypropylene a1) and polyethylene a2).

Still another preferred embodiment of the present invention stipulates that component A) comprises less than <NUM> wt. -%, preferably less than <NUM> wt. -% and more preferably from <NUM> to <NUM> wt. -% based on the overall weight of component A) of thermoplastic polymers different from a1) and a2), preferably less than <NUM> wt. -% PA <NUM> and less than <NUM> wt. -% polystyrene, more preferably component A) comprises <NUM> to <NUM> wt. -% polystyrene.

In another preferred embodiment according to the present invention component A) comprises less than <NUM> wt. -%, preferably less than <NUM> wt. -% and more preferably from <NUM> to <NUM> wt. -% based on the overall weight of component A) of talc.

According to another preferred embodiment in accordance with the present invention component A) comprises less than <NUM> wt. -%, preferably less than <NUM> wt. -% and more preferably from <NUM> to <NUM> wt. -% based on the overall weight of component A) of chalk.

A further preferred embodiment in accordance with the present invention stipulates that component A) comprises less than <NUM> wt. -%, preferably less than <NUM> wt. -% and more preferably from <NUM> to <NUM> wt. -% based on the overall weight of component A) of paper.

In a further preferred embodiment of the present invention component A) comprises less than <NUM> wt. -%, preferably less than <NUM> wt. -% and more preferably from <NUM> to <NUM> wt. -% based on the overall weight of component A) of wood.

According to another preferred embodiment in accordance with the present invention component A) comprises less than <NUM> wt. -%, preferably less than <NUM> wt. -% and more preferably from <NUM> to <NUM> wt. -% based on the overall weight of component A) of metal.

In a further preferred embodiment according to the present invention component A) comprises less than <NUM> ppm, preferably from <NUM> to <NUM> ppm based on the overall weight of component A) of limonene.

Still another preferred embodiment in accordance with the present invention stipulates that component A) comprises less than <NUM> ppm, preferably from <NUM> to <NUM> ppm based on the overall weight of component A) of fatty acids.

In another preferred embodiment according to the present invention component A) is a recycled material, which is recovered from waste plastic material derived from post-consumer and/or post-industrial waste.

In a further preferred embodiment of the present invention the MFR<NUM> (<NUM>, <NUM>) determined according to ISO <NUM> of component A) is in the range of <NUM> to <NUM>/<NUM>, preferably in the range of <NUM> to <NUM>/<NUM> and more preferably in the range from <NUM> to <NUM>/<NUM>.

Still another preferred embodiment according to the present stipulates that the content of component A) in the polymer composition is in the range from <NUM> to <NUM> wt. -%, preferably in the range from <NUM> to <NUM> wt. -% or in the range from <NUM> to <NUM> wt. -% based on the overall weight of the polymer composition.

According to another preferred embodiment in accordance with the present invention the content of polypropylene a1) in component A) is in the range from <NUM> up to <NUM> wt. -%, preferably from <NUM> to <NUM> wt. -%, more preferably in the range from <NUM> to <NUM> wt. -%, still more preferably in the range from <NUM> to <NUM> wt. -% and most preferably in the range from <NUM> to <NUM> wt. -% based on the overall weight of component A), or the content of polypropylene a1) in component A) is in the range from <NUM> to <NUM> wt. -%, preferably in the range from <NUM> to <NUM> wt. -%, more preferably in the range from <NUM> to <NUM> wt. -% and most preferably in the range from <NUM> to <NUM> wt. -% based on the overall weight of component A), even more preferably component a1) comprises more than <NUM> wt. -%, still more preferably from <NUM> to <NUM> wt. -% isotactic polypropylene and most preferably consists of isotactic polypropylene.

In another preferred embodiment according to the present invention the content of polypropylene a2) in component A) is in the range from <NUM> to <NUM> wt. -%, preferably in the range from <NUM> to <NUM> wt. -%, more preferably in the range from <NUM> to <NUM> wt. -% and most preferably in the range from <NUM> to <NUM> wt. -% based on the overall weight of component A); or the content of polypropylene a2) in component A) is in the range from <NUM> to <NUM> wt. -%, preferably in the range from <NUM> to <NUM> wt. -%, more preferably in the range from <NUM> to <NUM> wt. -% and most preferably in the range from <NUM> to <NUM> wt. -% based on the overall weight of component A).

In a further preferred embodiment the polypropylene a1) comprises one or more polymer materials selected from the following:.

A further preferred embodiment of the present invention stipulates that component a1) has a density in the range of <NUM> to <NUM>/cm<NUM>, preferably in the range of <NUM> to <NUM>/cm<NUM> as determined in accordance with ISO <NUM>.

According to still a further embodiment of the present invention the melt flow rate (MFR) of component a1) is in the range of <NUM> to <NUM>/<NUM>, preferably in the range of <NUM> to <NUM>/<NUM> and alternatively in the range of <NUM> to <NUM>/<NUM> as determined in accordance with ISO <NUM> (at <NUM>; <NUM> load).

In another preferred embodiment of the present invention the melting temperature of component a1) is within the range of <NUM> to <NUM>, preferably in the range of <NUM> to <NUM> and more preferably in the range of <NUM> to <NUM>. In case it is a propylene homopolymer like item (I) above it will have a melting temperature in the range of <NUM> to <NUM>, preferably in the range from <NUM> to <NUM> and more preferably in the range of <NUM> to <NUM> as determined by differential scanning calorimetry (DSC) according to ISO <NUM>-<NUM>. In case it is a random copolymer of propylene like item (II) above it will have a melting temperature in the range of <NUM> to <NUM>, preferably in the range of <NUM> to <NUM> and more preferably in the range of <NUM> to <NUM> as determined by DSC according to ISO <NUM>-<NUM>.

The polyethylene a2) is preferably a high density polyethylene (HDPE) or a linear low density polyethylene (LLDPE) or a long-chain branched low density polyethylene (LDPE). The comonomer content of component a2) is usually below <NUM> wt. -% preferably below <NUM> wt. -% and most preferably below <NUM> wt.

Herein a HDPE suitable for use as component a2) has a density as determined according to ISO <NUM> of equal to or greater than <NUM>/cm<NUM>, preferably in the range of <NUM> to <NUM>/cm<NUM> and more preferably in the range of <NUM> to <NUM>/cm<NUM>.

According to another preferred embodiment, the HDPE is an ethylene homopolymer. A HDPE suitable for use as component a2) in this disclosure generally has a MFR determined by ISO <NUM> (at <NUM>; <NUM> load), in the range of <NUM>/<NUM> to <NUM>/<NUM>, preferably in the range of <NUM> to <NUM>/<NUM>, like in the range of <NUM> to <NUM>/<NUM>.

The HDPE may also be a copolymer, for example a copolymer of ethylene with one or more alpha-olefin monomers such as propylene, butene, hexene, etc..

A LLDPE suitable for use as component a2) in this disclosure generally has a density as determined with ISO <NUM>, in the range of <NUM> to <NUM>/cm<NUM>, or in the range of <NUM> to <NUM>/cm<NUM>, or in the range of <NUM> to <NUM>/cm<NUM> and an MFR determined by ISO <NUM> (at <NUM>; <NUM> load), in the range of <NUM> to <NUM>/min, or in the range of <NUM> to <NUM>/<NUM>, like in the range of <NUM> to <NUM>/<NUM>. The LLDPE is a copolymer, for example a copolymer of ethylene with one or more alpha-olefin monomers such as propylene, butene, hexene, etc..

A LDPE suitable for use as component a2) in this disclosure generally has a density as determined with ISO <NUM>, in the range of <NUM> to <NUM>/cm<NUM>, and an MFR determined by ISO <NUM> (<NUM>; <NUM>), in the range of <NUM> to <NUM>/min. The LDPE is an ethylene homopolymer.

According to a further preferred embodiment the melting temperature of component a2) is in the range from <NUM> to <NUM> and preferably in the range from <NUM> to <NUM>.

Such post-consumer and/or post-industrial waste can be derived from inter alia waste electrical and electronic equipment (WEEE) or end-of-life vehicles (ELV) or from differentiated waste collection schemes like the German DSD system, the Austrian ARA system and the Austrian ASZ system (especially for Purpolen materials) or the Italian "Raccolta Differenziata" system.

Recycled materials are commercially available, e.g. from Corpela (Italian Consortium for the collection, recovery, recycling of packaging plastic wastes), Resource Plastics Corp. (Brampton, ON), Kruschitz GmbH, Plastics and Recycling (AT), Ecoplast (AT), Vogt Plastik GmbH (DE), mtm plastics GmbH (DE) etc..

A preferred recycled polymer blend is Purpolen PP, being a recycled polymer mixture comprising polyethylene and polypropylene obtained from mtm plastics GmbH, Niedergebra, Germany. Another preferred recycled polymer blend is Dipolen, being a recycled polymer mixture comprising polyethylene and polypropylene obtained from mtm plastics GmbH, Niedergebra, Germany.

The polymer composition in accordance with the present invention comprises as component B) <NUM> to <NUM> wt. -% based on the overall weight of the polymer composition of a virgin ethylene alkyl (meth)acrylate having the following properties: MFR<NUM> (<NUM>, <NUM>) determined according to ISO <NUM> in the range from <NUM> to <NUM>/<NUM>; and an alkyl (meth)acrylate content based on the total weight of component B) in the range from <NUM> to <NUM> wt.

Preferred embodiments of component B) will be discussed in the following.

According to one preferred embodiment in accordance with the present invention component B) is an ethylene alkyl acrylate, preferably an ethylene methyl acrylate and/or an ethylene butyl acrylate.

Still another preferred embodiment in accordance with the present invention stipulates that component B) is an ethylene methyl acrylate having a MFR<NUM> (<NUM>, <NUM>) determined according to ISO <NUM> in the range from <NUM> to <NUM>/<NUM>, preferably from in the range from <NUM> to <NUM>/<NUM> and more preferably in the range from <NUM> to <NUM>/<NUM>; and/or an methyl acrylate content based on the total weight of component B) in the range from <NUM> to <NUM> wt. -%; preferably in the range from <NUM> to <NUM> wt. -% and more preferably in the range from <NUM> to <NUM> wt.

In still another preferred embodiment in accordance with the present invention component B) is an ethylene butyl acrylate having a MFR<NUM> (<NUM>, <NUM>) determined according to ISO <NUM> in the range from <NUM> to <NUM>/<NUM>, preferably from in the range from <NUM> to <NUM>/<NUM> and more preferably in the range from <NUM> to <NUM>/<NUM>; and/or an butyl acrylate content based on the total weight of component B) in the range from <NUM> to <NUM> wt. -%; preferably in the range from <NUM> to <NUM> wt. -% and more preferably in the range from <NUM> to <NUM> wt.

A preferred ethylene methyl acrylate is commercially available under the tradename Elvaloy AC1125 from Dow/DuPont.

A preferred ethylene butyl acrylate is commercially available under the tradenames Ebantix E1704 or Ebantix E2770 from Repsol.

The polymer composition according to the present invention may also comprise additives.

Preferably these additives are selected from the group consisting of slip agents, UV-stabilisers, pigments, anti-acids, antioxidants, antiblocking agents, antistatic agents, additive carriers, nucleating agents and mixtures thereof, more preferably the at least one additive are antioxidants, whereby these additives preferably are present in <NUM> to <NUM> wt. -%, more preferably in <NUM> to <NUM> wt. -% and most preferably in the range of <NUM> to <NUM> wt. -% based on the overall weight of the polymer composition.

Examples of antioxidants which may be used, are sterically hindered phenols (such as <NPL>, also sold as Irganox <NUM> FF™ by BASF), phosphorous based antioxidants (such as <NPL>, also sold as Hostanox PAR <NUM> (FF)™ by Clariant, or Irgafos <NUM> (FF)TM by BASF), sulphur based antioxidants (such as <NPL>, sold as Irganox PS-<NUM> FL™ by BASF), nitrogen-based antioxidants (such as <NUM>,<NUM>'- bis(<NUM>,<NUM>'-dimethylbenzyl)diphenylamine), or antioxidant blends.

Examples for anti-acids which may be used in the polymer compositions according to the present invention are calcium stearates, sodium stearates, zinc stearates, magnesium and zinc oxides, synthetic hydrotalcite (e.g. SHT, <NPL>), lactates and lactylates, as well as calcium stearate (<NPL>) and zinc stearate (<NPL>).

Antiblocking agents that may be used in the polymer compositions according to the present invention are natural silica such as diatomaceous earth (such as <NPL> (SuperfFloss™), <NPL> (SuperFloss E™), or <NPL> (Celite <NUM>™)), synthetic silica (such as <NPL>, <NPL>, <NPL>, <NPL>, <NPL>, <NPL>, <NPL>, <NPL>, or <NPL>), silicates (such as aluminium silicate (Kaolin) <NPL>, sodium aluminum silicate CAS-No. <NUM>-<NUM>-<NUM>, calcined kaolin <NPL>, aluminum silicate <NPL>, or calcium silicate <NPL>), synthetic zeolites (such as sodium calcium aluminosilicate hydrate <NPL>, <NPL>, or sodium calcium aluminosilicate, hydrate <NPL>).

UV-stabilisers which might be used in the polymer compositions according to the present invention are, for example, Bis-(<NUM>,<NUM>,<NUM>,<NUM>-tetramethyl-<NUM>-piperidyl)-sebacate (<NPL>, Tinuvin <NUM>); <NUM>-hydroxy-<NUM>-n-°Ctoxy-benzophenone (<NPL>, Chimassorb <NUM>).

Nucleating agents that can be used in the polymer compositions according to the present invention are for example sodium benzoate (<NPL>) or <NUM>,<NUM>:<NUM>,<NUM>-bis(<NUM>,<NUM>-dimethylbenzylidene)sorbitol (<NPL>, Millad <NUM>).

Suitable antistatic agents are, for example, glycerol esters (<NPL>) or ethoxylated amines (<NPL> or <NPL>) or ethoxylated amides (<NPL>).

Below preferred embodiments of the polymer composition according to the present invention will be discussed.

According to one preferred embodiment in according with the present invention the polymer composition has a MFR<NUM> (<NUM>, <NUM>) determined according to ISO <NUM> in the range of <NUM> to <NUM>/<NUM>, preferably in the range of <NUM> to <NUM>/<NUM> or <NUM> to <NUM>/<NUM> and more preferably in the range of <NUM> to <NUM>/<NUM> or <NUM> to <NUM>/<NUM>.

Still another preferred embodiment in accordance with the present invention stipulates that the polymer composition has a Tensile Strain at Break measured according to ISO527-<NUM> in the range of <NUM> to <NUM> %, preferably in the range of <NUM> to <NUM> % or <NUM> to <NUM> % and more preferably in the range of <NUM> to <NUM> % or <NUM> to <NUM> %.

In another preferred embodiment in accordance with the present invention the polymer composition has a Charpy Notched Impact Strength measured according to ISO <NUM>-1eA at <NUM> of more than <NUM> kJ/m<NUM>, preferably in the range of <NUM> to <NUM> kJ/m<NUM>, more preferably in the range of <NUM> to <NUM> kJ/m<NUM> or <NUM> to <NUM> kJ/m<NUM>.

According to a further preferred embodiment in accordance with the present invention the content of component A) in the polymer composition is in the range from <NUM> to <NUM> wt. -%, preferably in the range from <NUM> to <NUM> wt. -% or in the range from <NUM> to <NUM> wt. -% based on the overall weight of the polymer composition.

Still another preferred embodiment in accordance with the present invention stipulates that the content of component B) in the polymer composition is in the range from <NUM> to <NUM> wt. -% and preferably in the range from <NUM> to <NUM> wt. -% or in the range from <NUM> to <NUM> wt. -% based on the overall weight of the polymer composition.

According to a further preferred embodiment in accordance with the present invention the content of polypropylene a1) in component A) is in the range from <NUM> up to <NUM> wt. -%, preferably from <NUM> to <NUM> wt. -%, more preferably in the range from <NUM> to <NUM> wt. -%, still more preferably in the range from <NUM> to <NUM> wt. -% and most preferably in the range from <NUM> to <NUM> wt. -% based on the overall weight of component A), or the content of polypropylene a1) in component A) is in the range from <NUM> to <NUM> wt. -%, preferably in the range from <NUM> to <NUM> wt. -%, more preferably in the range from <NUM> to <NUM> wt. -% and most preferably in the range from <NUM> to <NUM> wt. -% based on the overall weight of component A), even more preferably component a1) comprises more than <NUM> wt. -%, still more preferably from <NUM> to <NUM> wt. -% isotactic polypropylene and most preferably consists of isotactic polypropylene.

In another preferred embodiment in accordance with the present invention the content of polyethylene a2) in component A) is in the range from <NUM> to <NUM> wt. -%, preferably in the range from <NUM> to <NUM> wt. -%, more preferably in the range from <NUM> to <NUM> wt. -% and most preferably in the range from <NUM> to <NUM> wt. -% based on the overall weight of component A); or the content of polyethylene a2) in component A) is in the range from <NUM> to <NUM> wt. -%, preferably in the range from <NUM> to <NUM> wt. -%, more preferably in the range from <NUM> to <NUM> wt. -% and most preferably in the range from <NUM> to <NUM> wt. -% based on the overall weight of component A).

A further preferred embodiment of the present invention stipulates that component B) is an ethylene methyl acrylate and the polymer composition has a Tensile Strain at Break measured according to ISO527-<NUM> being at least <NUM> % higher, preferably in the range of <NUM> to <NUM> % higher, more preferably <NUM> to <NUM> % higher and most preferably <NUM> to <NUM> % higher than for the same polymer composition without component B).

According to still a further preferred embodiment according to the present invention component B) is an ethylene methyl acrylate and the polymer composition has a Charpy Notched Impact Strength measured according to ISO <NUM>-1eA at <NUM> being at least <NUM> % higher, preferably in the range of <NUM> to <NUM> % higher, more preferably <NUM> to <NUM> % higher and most preferably <NUM> to <NUM> % higher than for the same polymer composition without component B).

A further preferred embodiment of the present invention stipulates that component B) is an ethylene butyl acrylate and the polymer composition has a Tensile Strain at Break measured according to ISO527-<NUM> being at least <NUM> % higher, preferably in the range of <NUM> to <NUM> % higher, more preferably <NUM> to <NUM> % higher and most preferably <NUM> to <NUM> % higher than for the same polymer composition without component B).

According to still a further preferred embodiment according to the present invention component B) is an ethylene butyl acrylate and the polymer composition has a Charpy Notched Impact Strength measured according to ISO <NUM>-1eA at <NUM> being at least <NUM> % higher, preferably in the range of <NUM> to <NUM> % higher, more preferably <NUM> to <NUM> % higher and most preferably <NUM> to <NUM> % higher than for the same polymer composition without component B).

A preferred polymer composition in accordance with the present invention comprises at least the following components and preferably consists of these components:.

The process for manufacturing a polymer composition according to the present invention comprises the following steps:.

A preferred embodiment in accordance with the present invention stipulates that component B) is an ethylene methyl acrylate having a MFR<NUM> (<NUM>, <NUM>) determined according to ISO <NUM> in the range from <NUM> to <NUM>/<NUM>, preferably from in the range from <NUM> to <NUM>/<NUM> and more preferably in the range from <NUM> to <NUM>/<NUM>.

Still another preferred embodiment in accordance with the present invention stipulates that component B) has a methyl acrylate content based on the total weight of component B) in the range from <NUM> to <NUM> wt. -%; preferably in the range from <NUM> to <NUM> wt. -% and more preferably in the range from <NUM> to <NUM> wt.

According to a further preferred embodiment in accordance with the present invention component B) is an ethylene butyl acrylate having a MFR<NUM> (<NUM>, <NUM>) determined according to ISO <NUM> in the range from <NUM> to <NUM>/<NUM>, preferably from in the range from <NUM> to <NUM>/<NUM> and more preferably in the range from <NUM> to <NUM>/<NUM>.

Still another preferred embodiment in accordance with the present invention stipulates that component B) has a butyl acrylate content based on the total weight of component B) in the range from <NUM> to <NUM> wt. -%; preferably in the range from <NUM> to <NUM> wt. -% and more preferably in the range from <NUM> to <NUM> wt.

All preferred aspects and embodiments as described above shall also hold for the process according to the present invention.

The present invention also relates to the use of a virgin ethylene alkyl (meth)acrylate B) having the following properties: MFR<NUM> (<NUM>, <NUM>) determined according to ISO <NUM> in the range from <NUM> to <NUM>/<NUM>; and an alkyl (meth)acrylate content based on the total weight of component B) in the range from <NUM> to <NUM> wt. -%; for increasing the Tensile Strain at Break measured according to ISO527-<NUM>; and/or the Charpy Notched Impact Strength measured according to ISO <NUM>-1eA at <NUM> of a polymer blend A) of a recycled material comprising a1) polypropylene and a2) polyethylene in a weight ratio of a1) to a2) from <NUM>:<NUM> to <NUM>:<NUM>; whereby the virgin ethylene alkyl (meth)acrylate B) is present in amount of <NUM> to <NUM> wt. -% based on the overall weight of components A) and B).

All preferred aspects and embodiments as described above shall also hold for the use according to the present invention.

The present invention also relates to an article comprising the polymer composition according to the invention, preferably said article is selected from selected from the group consisting of consumer goods or houseware, preferably caps, closures and packaging containers.

MFR was measured according to ISO <NUM> at a load of <NUM> (MFR<NUM>), at <NUM> for polypropylene and MFR was measured according to ISO <NUM> at a load of <NUM> (MFR<NUM>) at <NUM> for polyethylene. For compounds comprising a mixture of both polypropylene and polyethylene, MFR was measured both at a load of <NUM> (MFR<NUM>), at <NUM> and at a load of <NUM> (MFR<NUM>) at <NUM>.

The melting temperature was determined with a TA Instrument Q2000 differential scanning calorimetry (DSC) on <NUM> to <NUM> samples. DSC is run according to ISO <NUM> / part <NUM> / method C2 in a heat / cool /heat cycle with a scan rate of <NUM>/min in the temperature range of -<NUM> to +<NUM>. Crystallization temperature (Tc) is determined from the cooling step, while melting temperature (Tm) and melting enthalpy (Hm) are determined from the second heating step. For calculating the melting enthalpy <NUM> is used as lower integration limit. Melting and crystallization temperatures were taken as the peaks of endotherms and exotherms.

The measurements were conducted after <NUM> conditioning time (at <NUM> at <NUM> % relative humidity) of the test specimen.

Tensile Modulus was measured according to ISO <NUM>-<NUM> (cross head speed = <NUM>/min; <NUM>) using injection moulded specimens as described in EN ISO <NUM>-<NUM> (dog bone shape, <NUM> thickness).

Tensile Strain at Break was measured according to ISO <NUM>-<NUM> (cross head speed = <NUM>/min; <NUM>) using injection moulded specimens as described in EN ISO <NUM>-<NUM> (dog bone shape, <NUM> thickness).

Charpy Notched impact strength was determined (after <NUM> hours of conditioning at <NUM> and <NUM>% relative humidity) according to ISO <NUM>1eA at <NUM> using <NUM>×<NUM>×<NUM><NUM> test bars injection moulded in line with EN ISO <NUM>-<NUM>.

Density of the materials was measured according to ISO <NUM>-<NUM>.

Below is exemplified the determination of the polar comonomer content of ethylene butyl acrylate and ethylene methyl acrylate. The weight-% can be converted to mol-% by calculation and is well documented in the literature.

Film samples of the polymers were prepared for the FTIR measurement: <NUM> to <NUM> thickness was used for ethylene butyl acrylate ><NUM> wt. -% butylacrylate content and <NUM> to <NUM> thickness was used for ethylene butyl acrylate <<NUM> wt. -% butylacrylate content.

After the FT-IR analysis the maximum absorbance for the peak for the butyl acrylate ><NUM> wt. -% at <NUM>-<NUM> was subtracted with the absorbance value for the base line at <NUM>-<NUM> (Abutylacrylate - A<NUM>). Then the maximum absorbance peak for the polyethylene peak at <NUM>-<NUM> was subtracted with the absorbance value for the base line at <NUM>-<NUM> (A<NUM> -A<NUM>). The ratio between (Abutylacrylate-A<NUM>) and (A<NUM>-A<NUM>) was then calculated in the conventional manner, which is well documented in the literature.

The maximum absorbance for the peak for the comonomer butylacrylate <<NUM> wt. -% at <NUM>-<NUM> was subtracted with the absorbance value for the base line at <NUM>-<NUM> (Abutyl acrylate - A<NUM>). Then the maximum absorbance peak for polyethylene peak at <NUM>-<NUM> was subtracted with the absorbance value for the base line at <NUM>-<NUM> (A<NUM> - A<NUM>). The ratio between (Abutylacrylate-A<NUM>) and (A<NUM>-A<NUM>) was then calculated.

Film samples of the polymers were prepared for the FTIR measurement: <NUM> thickness was used for ethylene methyl acrylate ><NUM> wt. -% methyl acrylate content and <NUM> thickness was used for ethylene methyl acrylate <<NUM> wt. -% methyl acrylate content.

After the analysis the maximum absorbance for the peak for the methyl acrylate ><NUM> wt. -% at <NUM>-<NUM> was subtracted with the absorbance value for the base line at <NUM>-<NUM> (Amethylacrylate - A<NUM>). Then the maximum absorbance peak for the polyethylene peak at <NUM>-<NUM> was subtracted with the absorbance value for the base line at <NUM>-<NUM> (A<NUM> -A<NUM>). The ratio between (Amethylacrylate-A<NUM>) and (A<NUM>-A<NUM>) was then calculated in the conventional manner, which is well documented in the literature.

The maximum absorbance for the peak for the comonomer methyl acrylate <<NUM> wt. -% at <NUM>-<NUM> was subtracted with the absorbance value for the base line at <NUM>-<NUM> (Amethyl acrylate - A<NUM>). Then the maximum absorbance peak for polyethylene peak at <NUM>-<NUM> was subtracted with the absorbance value for the base line at <NUM>-<NUM> (A<NUM> - A<NUM>). The ratio between (Amethyl acrylate-A<NUM>) and (A<NUM>-A<NUM>) was then calculated.

All calibration samples and samples to be analyzed were prepared in similar way, on molten pressed plates. Around <NUM> to <NUM> of the compounds to be analyzed were molten at <NUM>. Subsequently, for <NUM> seconds <NUM> to <NUM> bar pressure was applied in a hydraulic heating press. Next, the samples are cooled down to room temperature in <NUM> seconds in a cold press under the same pressure, in order to control the morphology of the compound. The thickness of the plates was controlled by metallic calibrated frame plates <NUM> by <NUM>, <NUM> to <NUM> thick (depending MFR from the sample); two plates were produced in parallel at the same moment and in the same conditions. The thickness of each plate was measured before any FTIR measurements; all plates were between <NUM> to <NUM> thick.

To control the plate surface and to avoid any interference during the measurement, all plates were pressed between two double-sided silicone release papers.

In case of powder samples or heterogeneous compounds, the pressing process was repeated three times to increase homogeneity by pressed and cutting the sample in the same conditions as described before.

Standard transmission FTIR spectroscope such as Bruker Vertex <NUM> FTIR spectrometer was used with the following set-up:.

Spectrum were recorded and analysed in Bruker Opus software.

As FTIR is a secondary method, several calibration standards were compounded to cover the targeted analysis range, typically from:.

The following commercial materials were used for the compounds: Borealis HC600TF as iPP, Borealis FB3450 as HDPE and for the targeted polymers such RAMAPET N1S (Indorama Polymer) for PET, Ultramid® B36LN (BASF) for Polyamide <NUM>, Styrolution PS 486N (Ineos) for High Impact Polystyrene (HIPS), and for PVC Inovyn PVC 263B (under powder form).

All compounds were made at small scale in a Haake kneader at a temperature below <NUM> and less than <NUM> minutes to avoid degradation. Additional antioxidant such as Irgafos <NUM> (<NUM> ppm) was added to minimise the degradation.

The FTIR calibration principal was the same for all the components: the intensity of a specific FTIR band divided by the plate thickness was correlated to the amount of component determined by <NUM>H or <NUM>C solution state NMR on the same plate.

Each specific FTIR absorption band was chosen due to its intensity increase with the amount of the component concentration and due to its isolation from the rest of the peaks, whatever the composition of the calibration standard and real samples.

This methodology was described in the publication from <NPL>.

The wavelength for each calibration band was:.

For each polymer component i, a linear calibration (based on linearity of Beer-Lambert law) was constructed. A typical linear correlation used for such calibrations is given below: <MAT> where xi is the fraction amount of the polymer component i (in wt%).

No specific isolated band can be found for C2 rich fraction and as a consequence the C2 rich fraction is estimated indirectly, <MAT>.

The EVA, Chalk and Talc contents are estimated "semi-quantitatively". Hence, this renders the C2 rich content "semi-quantitative".

For each calibration standard, wherever available, the amount of each component is determined by either <NUM>H or <NUM>C solution state NMR, as primary method (except for PA). The NMR measurements were performed on the exact same FTIR plates used for the construction of the FTIR calibration curves.

Calibration standards were prepared by blending iPP and HDPE to create a calibration curve. The thickness of the films of the calibration standards were <NUM>. For the quantification of the iPP, PS and PA <NUM> content in the samples quantitative IR spectra were recorded in the solid-state using a Bruker Vertex <NUM> FTIR spectrometer. Spectra were recorded on 25x25 mm square films of <NUM> to <NUM> thickness prepared by compression moulding at <NUM> and <NUM> to <NUM> mPa. Standard transmission FTIR spectroscopy was employed using a spectral range of <NUM> to <NUM>-<NUM>, an aperture of <NUM>, a spectral resolution of <NUM>-<NUM>, <NUM> background scans, <NUM> spectrum scans, an interferogram zero filling factor of <NUM> and Norton Beer strong apodisation.

The absorption of the band at <NUM>-<NUM> in iPP was measured and the iPP content was quantified according to a calibration curve (absorption/thickness in cm versus iPP content in wt.

The absorption of the band at <NUM>-<NUM> (PS) and <NUM>-<NUM> (PA6) were measured and the PS- and PA6 content quantified according to the calibration curve (absorption/thickness in cm versus PS and PA content in wt. The content of ethylene was obtained by subtracting the content of iPP, PS and PA6 from <NUM>. The analysis was performed as double determination.

The amount of talc and chalk were measured by Thermogravimetric Analysis (TGA); experiments were performed with a Perkin Elmer TGA <NUM>. Approximately <NUM> to <NUM> of material was placed in a platinum pan. The temperature was equilibrated at <NUM> for <NUM> minutes, and afterwards raised to <NUM> under nitrogen at a heating rate of <NUM>/min. The weight loss between ca. <NUM> and <NUM> (WCO2) was assigned to CO<NUM> evolving from CaCOs, and therefore the chalk content was evaluated as: <MAT>.

Afterwards the temperature was lowered to <NUM> at a cooling rate of <NUM>/min. Then the gas was switched to oxygen, and the temperature was raised again to <NUM>. The weight loss in this step was assigned to carbon black (Wcb). Knowing the content of carbon black and chalk, the ash content excluding chalk and carbon black was calculated as: <MAT>.

Where Ash residue is the wt. -% measured at <NUM> in the first step conducted under nitrogen. The ash content is estimated to be the same as the talc content for the investigated recyclates.

Paper and wood is determined by conventional laboratory methods including milling, floatation, microscopy and Thermogravimetric Analysis (TGA).

The amount of metals is determined by x ray fluorescence (XRF).

The amount of limonene is determined by solid phase microextraction (HS-SPME-GC-MS).

The amount of total fatty acids is determined by solid phase microextraction (HS-SPME-GC-MS).

Purpolen PP is a recycled polymer mixture comprising polyethylene and polypropylene obtained from mtm plastics GmbH, Niedergebra, Germany. Table <NUM> below shows the composition of the batch used in the Working Examples.

The content of components a1) and a2) in Purpolen PP adds up with PS (<NUM> wt. -%), talc (<NUM> wt. -%), chalk PA <NUM> (<NUM> wt. -%) (content also determined by FTIR) and other substances in minor amounts to <NUM> wt. -% (MFR<NUM> (<NUM>) of the used Purpolen PP was <NUM> /<NUM>).

Dipolen S is a recycled polymer mixture comprising polyethylene and polypropylene obtained from mtm plastics GmbH, Niedergebra, Germany. Table <NUM> below shows the composition of the batch used in the Working Examples.

The content of components a1) and a2) adds up with PS (<NUM> wt. -%), PA <NUM> (<NUM> wt. -%), talc (<NUM> wt. -%), chalk (<NUM> wt. -%) and other substances in minor amounts to <NUM> wt. -% (MFR<NUM> (<NUM>) of the used Dipolen S was <NUM> /<NUM>, MFR<NUM> (<NUM>) was <NUM> /<NUM>).

EMA is an ethylene methyl acrylate (MFR<NUM> <NUM> = <NUM>/<NUM>, MA content = <NUM> wt. -% based on the total weight of the polymer), commercially available under the tradename Elvaloy AC1125 from Dow/DuPont.

EBA1 is an ethylene butyl acrylate (MFR<NUM> <NUM> = <NUM>/<NUM>, BA content = <NUM> wt. -% based on the total weight of the polymer) which was produced as follows.

Fresh ethylene and recycled ethylene and comonomer butyl acrylate was compressed to reach an initial reactor pressure of <NUM> bars in two parallel streams to supply the front and the side of a split feed <NUM> zone reactor with a varying L/D between around <NUM> to <NUM>. Comonomer was added in amounts to reach <NUM> wt. -% in the final polymer. An MFR<NUM> of the final polymer of <NUM>/<NUM> was maintained. After compression, the front stream was heated to <NUM> in a preheating section before entering the front zone of the reactor and the side stream was cooled and entered at the side of the reactor. Mixtures of commercially available peroxide radical initiators dissolved in an essentially inert hydrocarbon solvent were injected after the preheating section and at one more position along the reactor in amounts sufficient for the exothermal polymerisation reaction to reach peak temperatures of <NUM>, and <NUM> respectively, with cooling in-between to <NUM>. The reaction mixture was depressurised by a pressure control valve, cooled and the polymer was separated from unreacted gas.

EBA2 is an ethylene butyl acrylate (EBA, MFR<NUM> <NUM> = <NUM>/<NUM>, BA content = <NUM> wt. -% based on the total weight of the polymer) which was produced as follows.

Fresh ethylene and recyclsed ethylene and comonomer butyl acrylate was compressed to reach an initial reactor pressure of <NUM> bars in two parallel streams to supply the front and the side of a split feed <NUM> zone reactor with a varying L/D between around <NUM> to <NUM>. Comonomer was added in amounts to reach <NUM> wt. -% in the final polymer. An MFR<NUM> of the final polymer of <NUM>/<NUM> was maintained. After compression, the front stream was heated to <NUM> in a preheating section before entering the front zone of the reactor and the side stream was cooled and entered at the side of the reactor. Mixtures of commercially available peroxide radical initiators dissolved in an essentially inert hydrocarbon solvent were injected after the preheating section and at one more position along the reactor in amounts sufficient for the exothermal polymerisation reaction to reach peak temperatures of <NUM>, and <NUM> respectively, with cooling in-between to <NUM>. The reaction mixture was depressurised by a pressure control valve, cooled and the polymer was separated from unreacted gas.

AO is a blend of commercially available antioxidants mainly containing Irganox B <NUM> (FF) commercially available from BASF (CH).

The polymer compositions according to the inventive examples (IE1 to IE15) and the comparative examples (CE1 to CE4) were prepared on a Coperion ZSK24, L/D ratio <NUM>. A compounding temperature of <NUM> to <NUM> was used during mixing, solidifying the melt strands in a water bath followed by strand pelletization. The amounts of the different components in the polymer compositions and the properties of the polymer compositions according to the inventive examples and the comparative examples can be gathered from below Tables <NUM> to <NUM>.

The polymer compositions shown in Table <NUM> above do all contain the same type of recyclate (Purpolen PP). The polymer composition according to CE1 consists of this recyclate and an antioxidant mixture. IE1 contains in addition <NUM> wt. -% of EMA and the EMA content is increased to <NUM> and <NUM> wt. -% for IE2 and IE3 respectively. As can be gathered from Table <NUM>, with increasing content of EMA the toughness, expressed by the Charpy Notched Impact Strength and the Tensile strain at break at <NUM>, of the polymer compositions increases. A small increase for the Charpy Notch Impact Strength and a significant increase for the Tensile Strain are already observed after addition of <NUM> wt. -% EMA, the use of higher amounts allows to obtain recyclate-based polymer compositions having significantly increased Charpy Notch Impact Strength and Tensile strain at break.

The polymer compositions shown in Table <NUM> above do all contain the same type of recyclate (Dipolen S). The polymer composition according to CE2 consists of this recyclate and an antioxidant mixture. IE4 contains in addition <NUM> wt. -% of EMA and the EMA content is increased to <NUM> and <NUM> wt. -% for IE5 and IE6 respectively. As can be gathered from Table <NUM>, with increasing content of EMA the toughness, expressed by the Charpy Notched Impact Strength and the Tensile Strain at <NUM>, of the polymer compositions increases. Already after addition of <NUM> wt. -% EMA a significant increase for the Charpy Notch Impact Strength and the Tensile Strength is observed, the addition of higher amounts allows to obtain recyclate-based polymer compositions having excellent Charpy Notch Impact Strength and Tensile Strain.

The polymer compositions shown in Table <NUM> above do all contain the same type of recyclate (Purpolen PP). The polymer composition according to CE3 consists of this recyclate and an antioxidant mixture. IE7 contains in addition <NUM> wt. -% of EBA and the EBA content is increased to <NUM> and <NUM> wt. -% for IE8 and IE9 respectively. As can be gathered from Table <NUM>, with increasing content of EBA the toughness, expressed by the Charpy Notched Impact Strength and the Tensile Strain at <NUM>, of the polymer compositions increases. A small increase for the Charpy Notch Impact Strength and a significant increase for the tensile strain at break are already observed after addition of <NUM> wt. -% EBA, the use of higher amounts allows to obtain recyclate-based polymer compositions having significantly increased Charpy Notch Impact Strength and Tensile strain at break.

Claim 1:
A polymer composition comprising at least the following components
A) <NUM> to <NUM> wt.-% based on the overall weight of the polymer composition of a polymer blend, comprising
a1) polypropylene;
a2) polyethylene;
wherein the weight ratio of a1) to a2) is from <NUM>:<NUM> to <NUM>:<NUM>; and
wherein the polymer blend A) is a recycled material;
B) <NUM> to <NUM> wt.-% based on the overall weight of the polymer composition of a virgin ethylene alkyl (meth)acrylate having the following properties
• MFR<NUM> (<NUM>, <NUM>) determined according to ISO <NUM> in the range from <NUM> to <NUM>/<NUM>; and
• an alkyl (meth)acrylate content based on the total weight of component B) in the range from <NUM> to <NUM> wt.-%;
with the proviso that the weight proportions of components A) and B) add up to <NUM> wt.-%.