Articles and methods made from recycled materials containing solvent-based binders

Abstract

The present disclosure provides a method. In one embodiment, the method includes providing pellets of recycled non-native material. The recycled non-native material is formed from a multilayer structure consisting of at least (i) a layer consisting of an olefin-based polymer, and (ii) an adhesive layer. The adhesive layer is composed of a solvent-based adhesive composition. The method includes blending the pellets with an olefin-based polymer blend component to form a blended material, and forming the blended material into an article.

Description

BACKGROUND OF THE INVENTION

[0001] The harm caused by plastic waste to the environment is well known. Large-scale social efforts are devoted to recycling and reusing plastic materials, which are referred to herein as recycled non-native materials. The efforts to reprocess and reintegrate recycled non-native materials into usable consumer products continue to expand.

[0002] However, when articles are made from recycled non-native materials, it has been found that the articles can have reduced physical properties. In particular, film-based articles formed from recycled non-native materials lack sufficient tear strength, tensile strength, and / or dart impact strength. Recycled non-native materials made from packaging (laminates and / or coated articles) containing adhesives are particularly difficult to recycle because the adhesives have an adverse effect on the physical properties of the recycled articles. To date, efforts to form recycled non-native materials containing solvent-based polyurethane adhesives into film-based articles with suitable physical properties have been insufficient.

[0003] The art recognizes a need for polymer compositions containing solvent-based adhesive compositions (and in particular solvent-based polyurethane adhesive compositions) that, when recycled, can produce recycled articles having suitable physical properties compared to recycled articles produced from olefin-based polymer materials not containing solvent-based polyurethane adhesives. There is also a need for polymer films / laminates containing a solvent-based polyurethane adhesive layer or a polyester coating that, when recycled, can produce film-based articles having suitable tear strength, tensile strength, and / or dart impact strength. SUMMARY OF THE INVENTION

[0004] The present disclosure provides a method. The method includes providing pellets of recycled non-native materials. The recycled non-native materials are formed from a multi-layer structure that consists of at least: (i) a layer composed of an olefin-based polymer, and (ii) an adhesive layer. The adhesive layer is composed of a solvent-based adhesive composition. The method includes blending the pellets with an olefin-based polymer blend component to form a blend material, and forming the blend material into an article.

[0005] The present disclosure also provides an article. The article contains an olefin-based polymer blend component and recycled non-native materials. The recycled non-native materials are formed from a multi-layer structure that consists of at least: (i) a layer composed of an olefin-based polymer, and (ii) an adhesive layer. The adhesive layer is composed of a solvent-based adhesive composition.

[0006] Definition

[0007] Any reference to the Periodic Table is to the Periodic Table as published by CRC Press, Inc. in 1990 - 1991. A group of elements in the table is referred to by a new notation for numbering the groups.

[0008] For the purposes of U.S. patent practice, any patent, patent application, or publication mentioned is incorporated by reference in its entirety (or its equivalent U.S. version is so incorporated by reference), particularly for disclosures of definitions in the art (to the extent not inconsistent with any definitions specifically provided in this disclosure) and common general knowledge.

[0009] The numerical ranges disclosed herein include all values from the lower value to the upper value, including the lower and upper values. For ranges that contain definite values (e.g., 1 or 2 or 3 to 5 or 6 or 7), any sub - range between any two definite values is included (e.g., the above range 1 - 7 includes sub - ranges 1 to 2; 2 to 6; 5 to 7; 3 to 7; 5 to 6; etc.).

[0010] Unless stated to the contrary, implied by the context, or customary in the art, all parts and percentages are by weight, and all test methods are current as of the filing date of this disclosure.

[0011] The term "adhesive" or "adhesive composition" is a composition that adheres to at least one substrate. The adhesive composition can be used as a coating on a substrate or as an adhesive layer between two or more substrates in a laminate.

[0012] As used herein, the term "blend" or "polymer blend" is a blend of two or more polymers. This blend may or may not be miscible (not phase - separated at the molecular level). Such blends may or may not be phase - separated. Such blends may or may not contain one or more domain configurations, as determined by transmission electron spectroscopy, light scattering, x - ray scattering, and other methods known in the art.

[0013] The term "coating" or "coating composition" is an adhesive composition that adheres to a single surface of a substrate or film. The coating is the outermost layer on the substrate or film. A coated article (such as a coated film) has a coating that is the outermost (or innermost) layer containing the adhesive composition; the coated article is different from a laminate in which the adhesive composition is disposed between the film / substrate layers or otherwise sandwiched between the film / substrate layers.

[0014] The term "composition" refers to a mixture of materials that comprise the composition, as well as reaction products and decomposition products formed from the materials of the composition.

[0015] The terms "comprising", "including", "having" and their derivatives are not intended to exclude the presence of any additional components, steps or procedures, whether or not specifically disclosed. For the avoidance of any doubt, unless stated to the contrary, all compositions claimed by use of the term "comprising" may include any additional additives, adjuvants or compounds, whether in polymeric form or otherwise. In contrast, the term "consisting essentially of" excludes from the scope of any subsequent recitation any other components, steps or procedures (except those that are not essential to the operability) and the term "consisting of" excludes any component, step or procedure not specifically recited or listed. Unless otherwise stated, the term "or" refers to the listed members individually as well as in any combination. The use of the singular includes the use of the plural and vice versa.

[0016] "Ethylene-based polymer" is a polymer containing more than 50 weight percent (wt%) of polymerized ethylene monomer (based on the total amount of polymerizable monomers) and optionally may contain at least one comonomer. Ethylene-based polymers include ethylene homopolymers and ethylene copolymers (meaning units derived from ethylene and one or more comonomers). The terms "ethylene-based polymer" and "polyethylene" may be used interchangeably. Non-limiting examples of ethylene-based polymers (polyethylenes) include low density polyethylene (LDPE) and linear polyethylene. Non-limiting examples of linear polyethylene include linear low density polyethylene (LLDPE), ultra low density polyethylene (ULDPE), very low density polyethylene (VLDPE), multi-component ethylene-based copolymers (EPE), ethylene / α-olefin multi-block copolymers (also known as olefin block copolymers (OBC)), substantially linear or linear plastomers / elastomers and high density polyethylene (HDPE). Generally, polyethylene can be produced using heterogeneous catalyst systems (such as Ziegler-Natta catalysts), homogeneous catalyst systems containing Group 4 transition metals and ligand structures (such as metallocenes, non-metallocene metal centers, heteroaryls, heteroaryloxy ethers, phosphinimines, etc.) in gas phase fluidized bed reactors, liquid phase slurry reactors or liquid phase solution reactors. Combinations of heterogeneous and / or homogeneous catalysts can also be used in single reactor or dual reactor configurations.

[0017] "High density polyethylene" (or "HDPE") is an ethylene homopolymer or copolymer with at least one C4-C 10An ethylene / α-olefin copolymer of an α-olefin comonomer or a C4-C8 α-olefin comonomer, and having a density of 0.940 g / cc, or 0.945 g / cc, or 0.950 g / cc, or from 0.953 g / cc to 0.955 g / cc, or 0.960 g / cc, or 0.965 g / cc, or 0.970 g / cc, or 0.975 g / cc, or 0.980 g / cc. The HDPE can be a single-peak copolymer or a multi-peak copolymer. A "single-peak ethylene copolymer" is an ethylene / C4-C 10 α-olefin copolymer having one distinct peak in gel permeation chromatography (GPC) showing the molecular weight distribution. A "multi-peak ethylene copolymer" is an ethylene / C4-C 10 α-olefin copolymer having at least two distinct peaks in GPC showing the molecular weight distribution. The multi-peak includes copolymers having two peaks (bimodal) and copolymers having more than two peaks. Non-limiting examples of HDPE include ELITE TM 5960G1 high density polyethylene (HDPE) resin (available from Dow Chemical Company), DOW TM high density polyethylene (HDPE) resin (available from Dow Chemical Company), CONTINUUM TM bimodal polyethylene resin (available from Dow Chemical Company), LUPOLEN TM (available from LyondellBasell), and HDPE products from Borealis, Ineos, and ExxonMobil.

[0018] "Low density polyethylene" (or "LDPE") consists of an ethylene homopolymer or an ethylene / α-olefin copolymer containing at least one C3-C having a density of 0.915 g / cc to less than 0.940 g / cc 10 α-olefin, and contains long chain branches having a wide MWD. LDPE is typically produced by high pressure free radical polymerization (tubular reactor or autoclave with a free radical initiator). Non-limiting examples of LDPE include AGILITY TM 1021 low density polyethylene (LDPE) resin (available from Dow Chemical Company), MarFlex TM (Chevron Phillips), LUPOLEN TM (LyondellBasell), and LDPE products from Borealis, Ineos, ExxonMobil, and others.

[0019] "Linear low density polyethylene" (or "LLDPE") is a linear ethylene / α-olefin copolymer containing a heterogeneous short chain branch distribution, which contains units derived from ethylene and units derived from at least one C3-C 10 α-olefin comonomer. LLDPE is characterized by very little long chain branching (if any) compared to conventional LDPE. LLDPE has a density of 0.910 g / cc to less than 0.940 g / cc. Non-limiting examples of LLDPE include ELITE TM 5400G linear low density polyethylene resin (available from The Dow Chemical Company), TUFLIN TM linear low density polyethylene resin (available from The Dow Chemical Company), DOWLEX TM polyethylene resin (available from The Dow Chemical Company), FINGERPRINT TM polyethylene resin (available from The Dow Chemical Company) and MARLEX TM polyethylene (available from Chevron Phillips).

[0020] "Olefin-based polymer" or "polyolefin" is a polymer containing a majority or greater than 50 weight% of polymerized olefin monomers (such as ethylene or propylene) (by weight of the polymer) and optionally containing at least one comonomer. Non-limiting examples of olefin-based polymers are ethylene-based polymers and propylene-based polymers.

[0021] "Plastic" is a polymeric material that can generally be molded or shaped when subjected to heat and / or pressure. Non-limiting examples of olefin-based polymers include ethylene-based polymers and propylene-based polymers. Plastics do not include glass, metal, and / or wood or other cellulose-based materials (i.e., paper-based materials).

[0022] "Polymer" is a polymeric compound prepared by polymerizing monomers (whether of the same type or different types). Thus, the general term polymer encompasses the term homopolymer (used to refer to a polymer prepared from only one type of monomer, where it should be understood that trace impurities may be incorporated into the polymer structure) and the term "interpolymer". Trace impurities (e.g., catalyst residues) may be incorporated into and / or within the polymer. It also encompasses all forms of copolymers, such as random copolymers, block copolymers, etc. The terms "ethylene / α-olefin polymer" and "propylene / α-olefin polymer" denote copolymers prepared as described above by polymerizing ethylene or propylene and one or more additional polymerizable α-olefin monomers, respectively. It should be noted that although polymers are commonly referred to as "made from", "based on", "containing" a specified monomer or monomers, etc., in this context, the term "monomer" should be understood to refer to the polymerized residue of the specified monomer rather than the unpolymerized material. Generally, polymers herein are referred to as being based on "units" that are the polymerized form of the corresponding monomer.

[0023] "Polyurethane" is a polymer having urethane bonds derived from the chemical reaction between isocyanate groups and polyols. Chemical entities having isocyanate groups and polyols can have many different compositions. For example, one or more isocyanate-terminated polymers can react with small molecule polyols, such as ethylene glycol, propylene glycol, butylene glycol, neopentyl glycol, 1,6-hexanediol, and combinations thereof, to provide a polyurethane polymer. Alternatively, one or more hydroxyl-terminated polymers can react with small molecule isocyanates, such as toluene diisocyanate (TDI), 4,4'-methylenebis(phenyl isocyanate) (MDI), hexamethylene diisocyanate (HMDI), isophorone diisocyanate (IPDI), 4,4'-methylenebis(cyclohexyl isocyanate), 1,5-naphthalene diisocyanate, 1,3-bis(isocyanatomethyl)benzene, dimers and trimers of these isocyanates, and combinations thereof, to produce a polyurethane polymer. Still alternatively, one or more hydroxyl-terminated polymers can react with one or more isocyanate-terminated polymers to provide a polyurethane polymer. Common backbones for the hydroxyl-terminated polymers and isocyanate-terminated polymers used in the synthesis of polyurethanes include polyesters, polyethers, polycarbonates, poly(meth)acrylates, polyamides, nylons, and silicones. Polyurethanes can be linear or crosslinked.

[0024] "Propylene-based polymer" is a polymer containing more than 50 wt% of polymerized propylene monomer (based on the total amount of polymerizable monomers) and optionally may contain at least one comonomer. The terms "propylene-based polymer" and "polypropylene" may be used interchangeably.

[0025] As used herein, the terms "recyclability" or "mechanical recyclability" with respect to a first material or article having an adhesive or coating mean mechanically recyclable or recyclable; and mean that the first material or article having an adhesive or coating can be mechanically reprocessed to produce a second material or article having a desired range of physical properties, where the second article has a mechanical or physical property change of at least less than or equal to 33% relative to the properties of a control material or article that has no adhesive or coating and is reprocessed in the same manner as the second article. Examples (but not limited to) of test methods and guidelines for determining the recyclability of plastic articles can be found in the publication "Critical Guidance Protocol for PE Film and Flexible Packaging" of the Association of Plastic Recyclers (APR), Document No. FPE-CG-01, Revision Date - August 2, 2022.

[0026] "Ultra-low density polyethylene" (or "ULDPE") and "very-low density polyethylene" (or "VLDPE") are each linear ethylene / α-olefin copolymers containing a heterogeneous short-chain branch distribution, which contain units derived from ethylene and units derived from at least one C3-C 10 α-olefin comonomer. ULDPE and VLDPE each have a density of 0.885 g / cc to 0.915 g / cc. Non-limiting examples of ULDPE and VLDPE include AFFINITY TM PL 1850G ultra linear low density polyethylene resin (available from The Dow Chemical Company), ATTANE TM ultra-low density polyethylene resin (available from The Dow Chemical Company) and FLEXOMER TM very-low density polyethylene resin (available from The Dow Chemical Company).

[0027] Test method

[0028] Density is measured according to ASTM D792 Method B. Results are reported in grams per cubic centimeter (g / cc).

[0029] Differential scanning calorimetry (DSC) can be used to measure the melting, crystallization, and glass transition behavior of polymers over a wide temperature range. For example, this analysis is performed using a TA Instruments Q1000 DSC equipped with a refrigerated cooling system (RCS) and an autosampler. During testing, a nitrogen purge gas flow of 50 ml / min is used. Each sample is melt-pressed into a film at approximately 175 °C; then the melted sample is air-cooled to room temperature (approximately 25 °C). A 3 mg to 10 mg 6 mm diameter specimen is taken from the cooled polymer, weighed, placed in a light aluminum pan (approximately 50 mg), and crimped shut. Then the analysis is performed to determine its thermal properties.

[0030] The melting point Tm is determined from the DSC heating curve by first drawing a baseline between the start and end of the melting transition. Then a tangent is drawn to the data on the low-temperature side of the melting peak. The point where this tangent intersects the baseline is the extrapolated onset point of melting (Tm). This is as described in Bernhard Wunderlich, The Basis of Thermal Analysis, in Thermal Characterization of Polymeric Materials 92, 277 - 278 (edited by Edith A. Turi, 2nd edition, 1997).

[0031] The crystallization temperature Tc is determined from the DSC cooling curve as above, except that a tangent is drawn to the data on the high-temperature side of the crystallization peak. The point where this tangent intersects the baseline is the extrapolated onset temperature of crystallization (Tc).

[0032] The glass transition temperature Tg is determined from the DSC heating curve where the heat capacity of half of the sample has become liquid, as described in Bernhard Wunderlich, The Basis of Thermal Analysis, in Thermal Characterization of Polymeric Materials 92, 278 - 279 (edited by Edith A. Turi, 2nd edition, 1997). The baseline is drawn below and above the glass transition region and extrapolated through the Tg region. The temperature at the midpoint of the heat capacity of the sample between these baselines is Tg.

[0033] The melt index (MI) (I2) is measured according to ASTM D1238 (190 °C / 2.16 kg), where the results are reported in grams per 10 minutes (g / 10 min) or decigrams per minute (dg / min). The melt index (I10) is measured according to ASTM D1238 (190 °C / 10 kg), where the results are reported in grams per 10 minutes. The melt index ratio (I10 / I2) is measured according to ASTM D1238 at a temperature of 190 °C using the ratio of the values obtained at 10 kg and 2.16 kg.

[0034] The tear strain is measured according to ASTM D1922, where the results are reported in grams force (gf).

[0035] The tensile strength is measured according to ASTM D882, where the results are reported in kilopounds per square inch (ksi).

[0036] The tensile elongation is measured according to ASTM D882, where the results are reported as a percentage (%).

[0037] The dart impact is measured according to ASTM D1709 A, where the results are reported in newtons (N) as force or joules (J) as energy.

[0038] The film haze is measured according to ASTM D1709 A, where the results are reported as a percentage (%). Detailed Description

[0039] The present disclosure provides a method. In one embodiment, the method includes providing pellets of recycled non-native material. The recycled non-native material is formed from a multi-layer structure. The multi-layer structure includes (i) a layer composed of an olefin-based polymer, and (ii) an adhesive layer. The adhesive layer contains a solvent-based polyurethane adhesive composition (or a solvent-based polyester adhesive composition). The method includes blending the pellets of the recycled non-native material with an olefin-based polymer blend component to form a blend material, and forming the blend material into an article.

[0040] The method includes providing pellets of recycled non - virgin materials. As used herein, the term "recycled non - virgin materials" includes particles of polymer materials recycled from consumer plastics and / or industrial plastics, which are referred to as post - consumer recycled polymer materials ("PCR") and post - industrial recycled polymer materials ("PIR"). Non - limiting examples of such PCR / PIR articles include polymer materials that have been previously used in the context of single - layer films, multi - layer films, laminates, and are used as plastic consumer goods and / or plastic industrial products, such as plastic packaging, tubing, fibers, industrial waste, or molded products in consumer or industrial applications. In other words, recycled non - virgin materials are formed from waste plastics and may include traces of paper (from labels), inks, etc. The recycled non - virgin materials are re - processed plastic materials collected after the plastic materials have completed their first use; that is, plastic products that have been used for their first purpose. Recycled non - virgin materials are typically collected from recycling programs and / or recycling plants. Recycled non - virgin materials generally require additional cleaning and processing before they can be re - introduced into the production line.

[0041] The method includes providing pellets of recycled non - virgin materials. The recycled non - virgin materials are formed from a multi - layer structure. As used herein, a "multi - layer structure" has (i) a layer composed of an olefin - based polymer, (ii) an adhesive layer composed of a solvent - based polyurethane adhesive composition (or a solvent - based polyester adhesive composition), and (iii) an optional additional layer. The multi - layer structure can be a laminate article that includes at least one olefin - based polymer layer and at least one adhesive layer that adheres the layer having the olefin - based polymer to another layer. Alternatively, the multi - layer structure can be a coated article that includes at least one adhesive layer applied as a coating (or a coating layer) on the surface of an olefin - based polymer substrate.

[0042] In one embodiment, the multi - layer structure forming the recycled non - virgin materials is a multi - layer film, such as a waste film used for consumer food packaging. The multi - layer film has a layer composed of an olefin - based polymer. The olefin - based polymer can be an ethylene - based polymer or a propylene - based polymer. In additional embodiments, the olefin - based polymer used for the layer is one or more ethylene - based polymers. Non - limiting examples of suitable ethylene - based polymers include ethylene homopolymers or ethylene / α - olefin copolymers. The ethylene - based copolymer is an ethylene / C3 - C 12 α - olefin copolymer or an ethylene / C4 - C8α - olefin copolymer. Non - limiting examples of suitable comonomers for the ethylene / α - olefin copolymer include propylene, butene, hexene, and octene. Ethylene / C3 - C 12The α-olefin copolymer (or ethylene / C4-C8 α-olefin copolymer) can be MDPE, LDPE, LLDPE, ULDPE, VLDPE, HDPE, and combinations thereof. The layer having an olefin-based polymer can include one or more additives, including but not limited to slip agents, anti-blocking agents, and combinations thereof. The multilayer film can be a laminated article or a coated article as previously discussed herein.

[0043] The multilayer structure (from which the recycled non-virgin material is formed) further includes at least one adhesive layer. The adhesive layer is composed of a solvent-based polyurethane adhesive composition (or a solvent-based polyester composition). The adhesive can be the adhesive layer in the laminate or can be a coating on the film or substrate. The solvent-based polyurethane adhesive composition (or the solvent-based polyester composition) can optionally contain one or more ingredients such as fillers, dyes and pigments, tackifiers, plasticizers, rheology modifiers, polymers (including, for example, thermoplastic resins other than those discussed above), dehydrating agents (including, for example, silanes), benzoyl chloride, other polyols (including, for example, fatty polyols), UV indicators, solvents, etc.

[0044] Without being bound by a particular theory, the recyclability of a multilayer structure of a layer containing an olefin-based polymer (ethylene-based polymer) and an adhesive layer of a solventless polyurethane adhesive composition can be determined by comparing the Hansen solubility parameter (HSP) and the aliphatic carbon ratio (ACR) of the solventless polyurethane adhesive composition with the corresponding thresholds of HSP and ACR. As used herein, the "Hansen solubility parameter" (or "HSP") is a set of physicochemical parameters of a substance that can be used to estimate the types of intermolecular forces responsible for the compatibility between the substance and other materials. The basis of HSP is that the cohesive energy of two substances can be approximated by the sum of London dispersion forces, molecular dipole interactions, and hydrogen bond interactions. HSP values can be obtained from the book "Properties of Polymers", 4th Edition, Completely Revised Edition, by D.W. van Krevelen, available from Elsevier: Amsterdam, 2009, e-book ISBN: 9780080915104. As used herein, the term "aliphatic carbon ratio" (or "ACR") is defined as the ratio of the total number of moles of aliphatic carbon (carbon in methyl (CH3), methylene (CH2), methine (CH), quaternary carbon (C), and olefinic carbon (C═C) groups) in a substance or mixture of substances to the number of moles of the substance or mixture of substances. Generally, the higher the ACR, the higher the chemical similarity of the adhesive or coating composition to hydrocarbons, and the greater the likelihood that the composition is mechanically recyclable in polyolefin polymers. By way of non-limiting example, for 0.034 moles of 2-phenylethanol (C6H5CH2CH2OH), there are 0.068 moles of aliphatic carbon (two CH2 functional groups within one molecule). Thus, the ACR of the compound is 0.068 / 0.034 = 2. Applying the same calculation to " 102E / coc-reactant CT" with a mixing weight ratio of 100:5.2 and obtaining an ACR of 2.48.

[0045] In the context of a solvent-based adhesive composition (solvent-based polyurethane adhesive composition), a multi-layer structure comprising the solvent-based adhesive composition is more likely to be recyclable (or will be recyclable) when both (i) the HSP of the solvent-based adhesive composition is less than or equal to 22.7 and (ii) the ACR of the solvent-based adhesive composition is greater than or equal to 6.9. More specifically, in the context of a solvent-based adhesive composition (solvent-based polyurethane adhesive composition) having both an HSP value less than or equal to 22.7 and an ACR value greater than or equal to 6.9, a recycled non-virgin material formed from a multi-layer structure having a layer of an olefin-based polymer (ethylene-based polymer) and an adhesive or coating composed of the solvent-based adhesive composition (solvent-based polyurethane adhesive composition) will be recyclable into a film-based article with suitable physical properties with a greater than 75% probability (or 100% probability). In contrast, in the context of a solvent-based adhesive composition (solvent-based polyurethane adhesive composition), a multi-layer structure having a layer of an olefin-based polymer (ethylene-based polymer) and an adhesive layer composed of a solvent-based adhesive composition that only meets one of the following two conditions (or does not meet both of the following two conditions): (i) an HSP value less than or equal to 22.7 or (ii) an ACR value greater than or equal to 6.9, provides a recycled non-virgin material having the solvent-based adhesive composition (solvent-based polyurethane adhesive composition) that will be recyclable into a film-based article with suitable physical properties with a less than 50% probability (or 0% probability). The method of modeling the chemical compatibility of chemical species with polyethylene (Method of Modeling Chemical Compatibility of Chemical Species with Polyethylene) (Attorney Docket No. 84969-US-PSP) filed on January 30, 2023 as U.S. Patent Application No. 63 / 482,099 describes the selection of a solvent-based adhesive composition in a recycled non-virgin material to increase the likelihood of recyclability; the entire content of this application is incorporated herein by reference.

[0046] In one embodiment, the method includes selecting a solvent-based adhesive composition (solvent-based polyurethane adhesive composition) for the adhesive or coating (for the multi-layer structure) having an aliphatic carbon ratio (ACR) greater than or equal to 6.9 and a Hansen solubility parameter (HSP) value less than or equal to 22.7. When forming the multi-layer film structure, a solvent-based adhesive composition (solvent-based polyurethane adhesive composition) having the ACR value and the HSP value is selected.

[0047] In one embodiment, the solvent-based adhesive composition for recycled non-native materials is a solvent-based polyurethane adhesive composition having a polyol component and an isocyanate curable component. The polyol component is a blend of a polyether polyol and a polyester polyol. Non-limiting examples of such polyol components are ADCOTE TM 536B (available from The Dow Chemical Company). A non-limiting example of such an isocyanate curable component is ADCOTE TM 536A (available from The Dow Chemical Company). The solvent-based adhesive composition consisting of ADCOTE TM 536B and ADCOTE TM 536A (and optional additives) exhibits an HSP value less than or equal to 22.7 and an ACR value greater than or equal to 6.9. More specifically, the solvent-based adhesive consisting of ADCOTE TM 536B and ADCOTE TM 536A (and optional additives) exhibits an HSP value less than or equal to 22.6 and an ACR value greater than or equal to 7.0. Thus, the solvent-based adhesive composed of ADCOTE TM 536B and ADCOTE TM 536A (and optional additives) provides a greater than 75% probability (or 100% probability) that the recycled non-native materials formed from a multi-layer structure of a layer having an olefin-based polymer (ethylene-based polymer) and an adhesive layer composed of ADCOTE TM 536B and ADCOTE TM 536A (and optional additives) will be successfully recycled into a film-based article having suitable physical properties.

[0048] In one embodiment, the solvent-based adhesive composition for recycled non-native materials is a solvent-based adhesive composition applied in the presence of a solvent. Non-limiting examples of such solvents include aromatic petroleum distillates such as toluene; aliphatic solvents such as naphtha; ketone solvents such as acetone, methyl ethyl ketone, methyl isobutyl ketone, and methyl amyl ketone; alcohols such as ethanol, propanol, and diacetone alcohol; mono- and dialkyl ethers of ethylene glycol and diethylene glycol such as ethylene glycol monoethyl ether, ethylene glycol monobutyl ether, ethylene glycol monoethyl ether acetate, diethylene glycol monobutyl ether, and diethylene glycol diethyl ether; methyl acetate, ethyl acetate, propyl acetate, butyl acetate, or similar esters of propionic acid and butyric acid; dioxolane, dioxane, furan, and combinations thereof.

[0049] The multilayer structure (from which the recycled non-native material is formed) may include one, two, three, four, five, six, seven or more additional layers, each of these additional layers being composed of an olefin-based polymer (i.e., an ethylene-based polymer). The ethylene / C3-C 12 α-olefin copolymer (or ethylene / C4-C8 α-olefin copolymer) can be any ethylene / C3-C 12 α-olefin copolymer (or ethylene / C4-C8 α-olefin copolymer) as previously disclosed herein. It should be understood that the multilayer structure may also include one, two, three, four, five, six, seven or more additional adhesive layers of the solvent-based polyurethane adhesive layer composition.

[0050] In one embodiment, the recycled non-native material formed from the multilayer structure contains 99.5 wt% to 80 wt%, or 99.5 wt%, or 99 wt%, or 98 wt%, or 97 wt%, or 96 wt%, or 95 wt%, or 94 wt%, or 93 wt%, or 92 wt%, or 91 wt%, or 90 wt%, 90 wt%, or 89 wt%, or 88 wt%, or 87 wt%, or 86 wt%, or 85 wt% to 84 wt%, or 83 wt%, or 82 wt%, or 81 wt%, or 80 wt% of the ethylene-based polymer (native ethylene-based polymer and non-native ethylene-based polymer) and 0.5 wt% to 20 wt%, or 0.5 wt%, or 1 wt%, or 2 wt%, or 3 wt%, or 4 wt%, or 5 wt% or 6 wt% to 7 wt%, or 8 wt%, or 9 wt%, or 10 wt%, or 11 wt%, or 12 wt%, 13 wt%, or 14 wt%, or 15 wt%, or 16 wt%, or 17 wt%, or 18 wt%, or 19 wt%, or 20 wt% of a supplementary amount of the solvent-based polyurethane adhesive composition (to obtain 100 wt% of the recycled non-native material). The weight percentages are based on the total weight of the recycled non-native material.

[0051] In one embodiment, the solvent-based polyurethane adhesive composition can be the inner layer in the laminate. The adhesive layer can improve the interlayer adhesion between the functional layers of the olefin-based polymer and prevent delamination of the layers of the multilayer structure. In another embodiment, the solvent-based polyurethane adhesive composition can be included in the outer layer of the coated article, such as in a coating. The coating can provide mechanical support and protection for the other layers of the coated article. In addition, the outer layer of the solvent-based polyurethane adhesive composition in the coated article can be particularly suitable for protection, scribing, and / or printing.

[0052] In one embodiment, the method includes granulating a multilayer structure to form granules of recycled non-native material. The multilayer structure is a consumer and / or industrial article that has been subjected to a molding process and has completed its initial purpose as previously disclosed. The multilayer structure, i.e., a multilayer film having a layer of an olefin-based polymer (ethylene-based polymer) and an adhesive layer having a solvent-based polyurethane adhesive composition (where ACR ≥ 6.9 and HSR ≤ 22.7), is ground, flaked, or otherwise shredded and granulated to form recycled non-native material. Granulating may include grinding or exfoliating the multilayer structure to form flakes. The method may further include densifying the flakes to form granules of recycled non-native material. In one embodiment, a multilayer structure having at least (i) an olefin-based polymer (ethylene-based polymer) and (ii) an adhesive layer comprising a solvent-based polyurethane adhesive composition is subjected to a granulator unit that is capable of converting the multilayer structure into granules of recycled non-native material.

[0053] The method includes blending the granules of recycled non-native material with an olefin-based polymer blend component to form a blend material. The olefin-based polymer blend component may be in the form of granules, flakes, and combinations thereof.

[0054] The olefin-based polymer blend component is (i) a recycled olefin-based polymer multilayer film, (ii) a virgin ethylene-based polymer, and (iii) combinations thereof. The olefin-based polymer blend component differs from the granules of recycled non-native material in that the material / structure forming the olefin-based polymer blend component does not include an adhesive layer or does not contain an adhesive therein. In particular, the olefin-based polymer blend component does not contain or otherwise exclude a solvent-based polyurethane adhesive composition.

[0055] In one embodiment, the olefin-based polymer blend component is a recycled olefin-based multilayer film. The recycled olefin-based multilayer film used for the olefin-based polymer blend component may be the same multilayer film as the multilayer structure, except that the recycled olefin-based multilayer film used for the olefin-based polymer blend component does not include an adhesive layer or otherwise does not contain an adhesive. In additional embodiments, the recycled olefin-based multilayer film is a recycled ethylene-based multilayer film, where each layer in the recycled olefin-based multilayer film contains only a recycled ethylene-based polymer (and optional additives) (or consists only thereof).

[0056] In one embodiment, the olefin-based polymer is a virgin olefin-based polymer. As used herein, a "virgin olefin-based polymer" is one or more olefin-based polymers that do not contain PCR and / or do not contain PIR. The virgin olefin-based polymer has not undergone a molding process to form an article for first use (except for the initial pellet formation after polymerization).

[0057] In a further embodiment, the virgin olefin-based polymer is a virgin ethylene-based polymer. The virgin ethylene-based polymer differs from a non-virgin ethylene-based polymer in that the virgin ethylene-based polymer does not include resin particles recovered from post-consumer articles or post-industrial articles. For example, the virgin ethylene-based polymer is not a reprocessed material collected after the material has completed its first use; i.e., a PCR multilayer film that has already served its first purpose.

[0058] In one embodiment, the blend material contains from 1 wt% to 99 wt%, or from 1 wt% to 75 wt%, or 1 wt%, or 2.5 wt%, or 5 wt%, or 10 wt%, or 15 wt% to 20 wt% or 30 wt%, or 40 wt%, or 50 wt%, or 60 wt%, or 70 wt%, or 75 wt% of recycled non-virgin material and a complementary amount (to obtain 1OO wt% blend material) of olefin-based polymer blend components, or from 99 wt% to 1 wt%, or from 99 wt% to 25 wt%, or 99 wt%, or 97.5 wt%, or 95 wt%, or 90 wt%, or 85 wt% to 80 wt% or 70 wt%, or 60 wt%, or 50 wt%, or 4O wt%, or 30 wt%, or 25 wt%. The weight percentages are based on the total weight of the blend material.

[0059] In one embodiment, the blend material contains 50 wt% of pellets formed from recycled non-virgin material and 50 wt% of pellets of olefin-based polymer blend components. The weight percentages are based on the total weight of the blend material.

[0060] Then the olefin-based polymer blend components are transferred to the feed zone of an extruder. The extruder is designed to densify and melt the pellets of both the recycled non-native material and the olefin-based polymer blend components to form a melt pool of the polymer. This polymer pool is pressurized and pushed out of the extruder through a die, where the polymer can be converted into solid pellets. The term "extruding" or "extrusion" is a process in which a polymer is introduced into an extruder and continuously advanced along a screw through zones of high temperature and pressure, where the polymer is melted and compacted and finally forced through a die. The extruder can be a single-screw extruder, a multi-screw extruder, a disk extruder, or a ram extruder. The method can include extruding pellets of the blend material to form an extrudate.

[0061] The method includes forming the extrudate (of the blend material) into a product. Since the product contains recycled non-native material, the product is a recycled product. The method includes forming the extrudate (of the blend material) into a recycled product, which is (a recycled) pellet, (a recycled) single-layer film, (a recycled) multi-layer film, (a recycled) laminate, (a recycled) plastic packaging, (a recycled) pipe, (a recycled) fiber, (a recycled) molded product, and any combination thereof.

[0062] In one embodiment, the forming step includes molding the extrudate (of the blend material) into a molded product. As used herein, the term "molding" or "moulding" is a process in which a polymer is melted and an extrudate is formed, and then the extrudate is introduced into a mold, which is opposite to the desired shape, to form a product (or part) of the desired shape and size. Molding can be low-pressure or pressure-assisted.

[0063] In one embodiment, the method includes injection molding the extrudate (formed from the molten pellets of the blend material) and forming an injection molded product. As used herein, the term "injection molding" is a process by which a polymer material is melted and injected into a mold at high pressure, which is opposite to the desired shape, to form a product of the desired shape and size. The mold can be made of metals such as steel and aluminum.

[0064] In one embodiment, the method includes blow molding the extrudate (formed from the molten pellets of the blend material) and forming a blow molded product. As used herein, the term "blow molding" is a process that includes placing the extrudate in the center of a mold, inflating the polymer onto the mold wall with a blow pin, and curing the product by cooling. Blow molding can be used to make hollow plastic containers.

[0065] In one embodiment, the method includes manufacturing a film from an extrudate (of a blend material), including positioning a gear pump downstream of an extruder, the gear pump providing a high and stable pressure to push the extrudate through a blown film die to form the film.

[0066] In one embodiment, the method includes forming a recycled film from a blend material, the recycled film exhibiting a performance change of less than 33% in physical properties as compared to the performance of the same physical properties in a film formed from a 100 wt% olefin-based polymer blend component (which lacks an adhesive, and specifically, lacks a solvent-based polyurethane composition). The physical film properties compared between the recycled film and the 100 wt% olefin-based polymer blend component film include tear strength, tensile strength, dart impact strength, and combinations thereof. As an example, if the 100 wt% olefin-based polymer blend component film has a dart impact strength of 100 g, the recycled film (formed from the blend material) will have a dart impact strength of less than 33% of 100 g or a dart impact strength of 67 g to 133 g.

[0067] In one embodiment, the method includes blending 1 wt% to 99 wt%, or 1 wt% to 75 wt%, or 50 wt% of pellets of recycled non-virgin material with 99 wt% to 1 wt%, or 99 wt% to 25 wt%, or 50 wt% of an olefin-based polymer blend component to form a blend material, the olefin-based polymer blend component being a recycled olefin-based polymer film (the same film as the multilayer film in a multilayer structure but without an adhesive composition). The recycled non-virgin material comprises 88 wt% to 99.5 wt% of an ethylene-based polymer and 12 wt% to 0.5 wt% (based on the total weight of the recycled non-virgin material) of a solvent-based polyurethane adhesive composition, the solvent-based polyurethane adhesive composition having an aliphatic carbon ratio (ACR) value greater than or equal to 6.9 and a Hansen solubility parameter (HSP) value less than or equal to 22.7. The method includes extruding the blend material to form a recycled film. The recycled film exhibits a performance change of less than 33% in physical properties as compared to the performance of the same physical properties in a film composed of a recycled olefin-based polymer multilayer film of the olefin-based polymer blend component. The physical properties are selected from one, some, or all of the following properties: tear strength, tensile strength, and / or dart impact strength.

[0068] The present disclosure provides an article. In one embodiment, the article is a recycled article and is formed from a blend of an olefin-based polymer blend component and recycled non-native materials. The recycled non-native materials are formed from a multi-layer structure having at least two of the following: (i) a layer composed of an olefin-based polymer, and (ii) an adhesive layer composed of a solvent-based polyurethane adhesive composition that exhibits an aliphatic carbon ratio (ACR) value of greater than or equal to 6.9 and a Hansen solubility parameter (HSP) value of less than or equal to 22.7. Alternatively, the adhesive layer can be composed of a solvent-based polyester adhesive composition.

[0069] The olefin-based polymer blend component is selected from virgin olefin-based polymers, recycled olefin-based polymer multi-layer films, and combinations thereof.

[0070] Based on the total weight of the (recycled) article, the (recycled) article contains 1 wt% to 99 wt%, or 1 wt% to 75 wt%, or 50 wt% of recycled non-native materials and 99 wt% to 1 wt%, or 99 wt% to 25 wt%, or 50 wt% of the olefin-based polymer blend component. Based on the total weight of the (recycled) article, the (recycled) article contains 88 wt% to 99.5 wt%, or 90 wt% to 99.0 wt%, or 95 wt% to 99.0 wt%, or 97 wt% to 99 wt% of ethylene-based polymers (virgin ethylene-based polymers and non-virgin ethylene-based polymers) and 0.5 wt% to 12 wt%, or 1 wt% to 10 wt%, or 1 wt% to 5 wt%, or 1 wt% to 3 wt% of the solvent-based polyurethane adhesive composition.

[0071] In one embodiment, the article is a recycled article, which is (recycled) pellets, (recycled) single-layer films, (recycled) multi-layer films, (recycled) laminates, (recycled) plastic packaging, (recycled) pipes, (recycled) fibers, (recycled) molded products, and any combination thereof.

[0072] In one embodiment, the (recycled) article is a recycled film. Based on the total weight of the (recycled) article, the recycled film contains 1 wt% to 75 wt% or 50 wt% of recycled non-virgin material and 99 wt% to 25 wt% or 50 wt% of an olefin-based polymer blend component. Based on the total weight of the (recycled) article, the (recycled) article contains 88 wt% to 99.5 wt%, or 90 wt% to 99.0 wt%, or 95 wt% to 99.0 wt%, or 97 wt% to 99 wt% of an ethylene-based polymer and 0.5 wt% to 12 wt%, or 1 wt% to 10 wt%, or 1 wt% to 5 wt%, or 1 wt% to 3 wt% of a solvent-based polyurethane adhesive composition. The solvent-based polyurethane adhesive composition has an aliphatic carbon ratio (ACR) value greater than or equal to 6.9 and a Hansen solubility parameter (HSP) value less than or equal to 22.7. The olefin-based polymer blend component is a recycled ethylene-based polymer multilayer film. The recycled film exhibits a performance change in physical properties of less than 33% compared to the performance of the same physical properties in a film (recycled ethylene-based polymer multilayer film) consisting of only 100 wt% of the olefin-based blend component. The film physical properties are one, some, or all of the following: tear strength, tensile strength, and / or dart impact strength.

[0073] By way of example and not limitation, some embodiments of the present disclosure will now be described in detail in the following examples.

[0074] Example

[0075] The following Table 1 provides a list of materials for Comparative Samples (CS) and Invention Examples (IE).

[0076] Table 1 - Materials

[0077]

[0078]

[0079] A. Multilayer film manufacturing

[0080] An olefin-based polymer multilayer film (alternatively referred to as a 7-layer film) is manufactured on a seven-layer blown film line available from Hosokawa-Alpin. The material composition of each of the seven layers is described in Table 2. The seven-layer blown film line utilizes seven 30 L / D extruders with a 50 millimeter (mm) diameter that feed a 250 mm diameter spiral mandrel die with a 2 mm die gap, which is 610 mm when laid flat and has a gauge of 2 mils (50 μm). The output rate is 148 kilograms per hour (kg / h) and the melt temperature is approximately 185 °C to 245 °C. A blow-up ratio of 2.5 is used when blowing the 7-layer film, and then the 7-layer film is cooled using a single-lip air ring and internal bubble cooling. The line speed is approximately 17 meters per minute (m / min), and the 7-layer film is corona treated to an average surface energy of > 38 dynes / cm.

[0081] Table 2 below provides the structure / composition of a 7-layer film with a thickness of 50 μm.

[0082] Table 2 - 7 - layer film

[0083]

[0084]

[0085] B. Multilayer structure

[0086] 1. Laminate

[0087] As described below, two 7-layer films are bonded together to form a laminate by applying a layer of a solvent-based polyurethane adhesive composition as listed in Table 3A on the surface of one 7-layer film and then contacting another 7-layer film with the adhesive layer.

[0088] 2. Coated film

[0089] A coated article (laminated film) is formed by applying a layer of a solvent-based polyurethane adhesive composition as listed in Table 3A on the surface of one 7-layer film as described below.

[0090] Table 3A below provides the composition and coating weight of the solvent-based polyurethane adhesive composition applied to the 7-layer film in forming the resulting multilayer structure (laminate). Table 3B below provides the composition and coating weight of the solvent-based polyester coating composition applied to the 7-layer film in forming the resulting multilayer structure (coated film).

[0091] Table 3A - Solvent - based polyurethane adhesive composition

[0092]

[0093] Table 3B - Solvent - based polyester adhesive composition (coating)

[0094] Polyester Solvent <![CDATA[Coating weight (g / m 2 )]]> HSP ACR PE C <![CDATA[ADCOTE TM 3840D]]> 1,3 - Dioxolane 1.8 29.6 2.1

[0095] As shown in Table 3A, the solvent-based polyurethane adhesive PU A formed by ADCOTE TM 536A / ADCOTE TM 536B exhibits an aliphatic carbon ratio (ACR) value greater than or equal to 6.9 (PU A 7) and a Hansen solubility parameter (HSP) value less than or equal to 22.7 (PU A 22.6). The solvent-based polyurethane adhesive PU B formed by ADCOTE TM 577 / CR87-124 fails to exhibit an ACR value greater than or equal to 6.9 (PU B 3.7), and also fails to exhibit an HSP value less than or equal to 22.7 (PU B 25.1). As shown in Table 3B, the solvent-based polyester coating PE C formed by ADCOTE TM 3840D fails to exhibit an ACR value greater than or equal to 6.9 (PU B 2.1), and also fails to exhibit an HSP value less than or equal to 22.7 (PU B 29.6).

[0096] Lamination of the multi-layer structure is applied using a commercial Labocombi 400 series laminator (available from Nordmecanica). The Labocombi 400 has a maximum film width of 406 mm and a minimum film width of 254 mm. The laminator includes a gravure deck for laminating solvent-based polyurethane adhesives. The laminator also contains a two-zone forced air dryer and a 7.5 kilowatt (KW) corona processor (available from Enercon Industries Corporation) for the primary and secondary films. The coated film is dried in the drying section of the laminator to evaporate the solvent to a residual solvent content of less than 10 mg / m 2 2. The maximum line speed of the laminator is 400 meters per minute (m / min) (or 1,312 feet per minute). All unwinding uses a 76 mm or 152 mm core, and rewinding uses a 76 mm core. When the lamination is completed, the laminate is fully cured at 20 ± 1 °C and 50% relative humidity for 7 days.

[0097] Table 3C below provides the structure / composition of laminate 1 and laminate 2. Each has a 7-layer film / PU adhesive layer / 7-layer film structure.

[0098] Table 3C: Laminated structure

[0099] Olefin - based polymer film one Adhesive layer Olefin - based polymer film two Laminate 1 7 - layer film <![CDATA[PU A(3.0g / m 2 )]]> 7 - layer film Laminate 2 7 - layer film <![CDATA[PU B(3.2g / m 2 )]]> 7 - layer film

[0100] Table 3D provides the structure / composition of Coating 1 having a 7-layer film / PU adhesive layer structure.

[0101] Table 3D - Coated film

[0102] Olefin - based polymer film one Adhesive layer Coated film 1 7 - layer film <![CDATA[PE C(1.8g / m 2 )]]>

[0103] C. Film shredding / granulation

[0104] Subsequently, each of the resulting multilayer structures (Laminate 1, Laminate 2, and Coated Film 1) is reprocessed by shredding each multilayer structure into particulate form and granulating the shredded multilayer structure to form recycled non-virgin material. Using a 605K granulator unit (available from EREMA North America, Inc., 23 Old Right Road - Unit #2, Ipswich, MA 01938, USA) to complete shredding and granulation. The cylinder zone of the granulator operates at 171 °C; and the granulator area operates at 176 °C. The pellets of the resulting recycled non-virgin material have an average size of 30 pellets per 1 gram.

[0105] Table 4 below provides the composition of the recycled non-virgin material.

[0106] Table 4 - Recycled non - virgin material composition

[0107]

[0108] wt%, based on the total weight of each recycled non-virgin material.

[0109] D. Compounding blend ratio

[0110] Once granulated, the pellets of the recycled non-virgin material (pellets of RNM 1, pellets of RNM 2, and pellets of RNM 3) are blended with pellets of an olefin-based polymer blend component at a ratio of approximately 50:50 wt%. The olefin-based polymer blend component, which may be referred to interchangeably herein as "control pellets", is a recycled olefin-based polymer multilayer film that is shredded and granulated 7-layer film (which may be referred to interchangeably herein as "recycled 7-layer film"). In addition, the recycled olefin-based polymer multilayer film differs from the pellets of the recycled non-virgin material in that the recycled olefin-based polymer multilayer film is not formed into a multilayer structure and thus lacks a solvent-based polyurethane adhesive and has not undergone lamination.

[0111] A blend material having 50 wt% recycled 7-layer film and 50 wt% recycled non-virgin material is formed into a blown film. The blown film manufacturing conditions are shown in Table 5A below. For each of RNM 1, RNM 2, and RNM 3, the resulting film formed from a blend of 50 wt% olefin-based polymer blend component (i.e., recycled 7-layer film) and 50 wt% recycled non-virgin material is provided. A corresponding control film formed from 100 wt% recycled 7-layer film (formed under the manufacturing conditions in Table 5A) is also provided, as shown in Table 5B.

[0112] Table 5A.

[0113] Table 5A - Blown film manufacturing conditions

[0114] Condition Value Mold temperature 215℃ Die gap 2.0mm Film thickness 2 mils Die diameter 60mm Blow - up ratio (BUR) 2.5 Output 8.80 kg / hour Frost line height (FLH) 165mm

[0115] Table 5B - Recycled film

[0116]

[0117] Table 6 below provides the dart impact strength, tear strength, and tensile strength values for Examples IE 2 (which includes PU A from Table 3A), CS 3 (which includes PU B from Table 3A), and CS 4 (which includes PU C from Table 3A) of the present invention. Table 6 also includes the mechanical properties of control film CS1 - this film is formed from 100 wt% recycled 7-layer film. Table 6 also provides the percentage change in the values comparing (i) CS1 with IE 2, and (ii) CS1 with CS 3.

[0118] Table 6 - Film mechanical property values

[0119]

[0120]

[0121] * Film IE 4 is not extrudable and therefore does not exhibit mechanical properties.

[0122] Table 6 shows that compared to film IE3 composed of 50 wt% 7-layer film and 50 wt% RNM 2 (based on the total weight of film IE2), film IE2 (recycled film) formed from 50 wt% recycled 7-layer film and 50 wt% RNM 1 (based on the total weight of film IE2) exhibits improved dart impact strength, film haze, tear strength, and tensile strength values, where the recycled non-virgin material includes PU A and RNM 2 includes PU B.

[0123] Table 6 further shows that film IE2 exhibits less than 33% performance change in the physical properties of dart impact, tear strength, and tensile strength relative to film CS1 (CS1 consisting of 100 wt% olefin-based polymer blend components, which is a recycled 7-layer film). Thus, Table 6 shows the recyclability of a recycled non-virgin material comprising a layer of an olefin-based polymer (formed from a laminate of a 7-layer film having two ethylene-based polymers) and a layer of a solvent-based polyurethane adhesive composition having an ACR value greater than or equal to 6.9 and an HSP value less than or equal to 22.7.

[0124] In contrast, IE3 in Table 6 (with PU B) demonstrates the lack of recyclability of a recycled non-virgin material comprising a layer of an olefin polymer (formed from a laminate of a 7-layer film having two ethylene-based polymers) and a layer of a solvent-based polyurethane adhesive composition (PU B) that does not have an ACR value greater than or equal to 6.9 and an HSP value less than or equal to 22.7, as evidenced by a performance change of greater than 33% in the physical properties of dart impact strength, tear strength, and tensile strength relative to film CS1, which consists of 100 wt% olefin-based polymer blend components, i.e., a recycled 7-layer film.

[0125] It is particularly desirable that the present disclosure is not limited to the embodiments and descriptions contained herein, but includes modifications of those embodiments that include portions of the embodiments and combinations of elements of different embodiments that fall within the scope of the following claims.

Claims

1. A method, the method comprising: Providing pellets of recycled non - virgin material formed from a multi - layer structure, the multi - layer structure comprising at least (i) a layer composed of an olefin - based polymer, and (ii) an adhesive layer comprising a solvent - based adhesive composition; Blending the pellets with an olefin - based polymer blend component to form a blend material; And Forming the blend material into an article.

2. The method according to claim 1, the method further comprising selecting a solvent - based polyurethane adhesive composition having an aliphatic carbon ratio (ACR) value greater than or equal to 6.9 and a Hansen solubility parameter (HSP) value less than or equal to 22.7 before providing the solvent - based adhesive composition.

3. The method according to any one of claims 1 to 2, wherein the olefin - based polymer blend component is selected from the group consisting of virgin olefin - based polymers, recycled olefin - based polymer multi - layer films, and combinations thereof.

4. The method according to any one of claims 1 to 3, the method comprising providing the pellets of recycled non - virgin material, the pellets comprising 99.5 wt% to 88 wt% of an ethylene - based polymer, and 0.5 wt% to 12 wt% of a solvent - free adhesive composition.

5. The method according to any one of claims 1 to 4, the method comprising Blending 1 wt% to 99 wt% of the pellets of the recycled non - virgin material with 99 wt% to 1 wt% of the olefin - based polymer blend component to form the blend material; Wherein the olefin - based polymer blend component is a recycled olefin - based polymer multi - layer film.

6. The method according to any one of claims 1 to 5, wherein the multi - layer structure is selected from the group consisting of single - layer films, multi - layer films, laminates, plastic packaging, molded products, and combinations thereof.

7. The method according to any one of claims 1 to 6, the method comprising forming the blend material into an article selected from the group consisting of pellets, single - layer films, multi - layer films, multi - layer laminates, plastic packaging, pipes, fibers, and molded products.

8. The method according to claim 7, wherein the article is a film; and Compared with the performance of the same physical properties in a film composed only of the olefin - based polymer blend component, the film exhibits a performance change of less than 33% in physical properties.

9. The method according to claim 8, wherein the physical properties are selected from the group consisting of tear strength, tensile strength, dart impact, and combinations thereof.

10. An article, the article comprising: An olefin - based polymer blend component; and Recycled non - virgin material formed from a multi - layer structure, the multi - layer structure comprising at least (i) a layer comprising an olefin - based polymer, and (ii) an adhesive layer comprising a solvent - based adhesive composition.

11. The article according to claim 10, wherein the solvent-based adhesive composition is a solvent-based polyurethane composition having an aliphatic carbon ratio (ACR) value greater than or equal to 6.9 and a Hansen solubility parameter (HSP) value less than or equal to 22.

7.

12. The composition according to any one of claims 10 to 11, wherein the olefin-based polymer blend component is selected from the group consisting of: virgin olefin-based polymers, recycled olefin-based polymer multilayer films, and combinations thereof.

13. The article according to any one of claims 10 to 12, wherein the article comprises 99.5 wt% to 88 wt% of an ethylene-based polymer, and 0.5 wt% to 12 wt% of a solventless adhesive or coating composition.

14. The article according to any one of claims 10 to 13, wherein the article is selected from the group consisting of: pellets, single-layer films, multilayer films, multi-layer laminates, plastic packaging materials, pipes, fibers, and molded products.

15. The article according to claim 14, wherein the article is a film, and the film exhibits a performance change of less than 33% in physical properties compared to the performance of the film having the same physical properties in the film composed of the olefin-based blend component.

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