Classifications

• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B27/00—Layered products comprising a layer of synthetic resin
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B27/00—Layered products comprising a layer of synthetic resin
  • B32B27/32—Layered products comprising a layer of synthetic resin comprising polyolefins
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B65—CONVEYING; PACKING; STORING; HANDLING THIN OR FILAMENTARY MATERIAL
  • B65D—CONTAINERS FOR STORAGE OR TRANSPORT OF ARTICLES OR MATERIALS, e.g. BAGS, BARRELS, BOTTLES, BOXES, CANS, CARTONS, CRATES, DRUMS, JARS, TANKS, HOPPERS, FORWARDING CONTAINERS; ACCESSORIES, CLOSURES, OR FITTINGS THEREFOR; PACKAGING ELEMENTS; PACKAGES
  • B65D65/00—Wrappers or flexible covers; Packaging materials of special type or form
  • B65D65/38—Packaging materials of special type or form
  • B65D65/40—Applications of laminates for particular packaging purposes
• • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
  • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
  • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
  • Y02W30/00—Technologies for solid waste management
  • Y02W30/50—Reuse, recycling or recovery technologies
  • Y02W30/62—Plastics recycling; Rubber recycling

Definitions

• the present invention relates to a laminated film with excellent recyclability and a packaging material obtained using the laminated film.
• Laminated films which are conventionally manufactured by the lamination method using adhesives, are not only intended for packaging, but also provide various high-performance functions such as barrier properties, moisture resistance, and retort resistance with a single packaging material. It has been developed and evolved to laminate films of different resin types in order to meet the demands. (See Patent Document 1, for example) However, in recent years, there have been voices that these different resin types of laminated films deteriorate the quality of recycled plastics.
• Laminated films of the same resin type are expected as recyclable packaging materials.
• a packaging material composed only of an olefin resin also called a monomaterial or the like
• these are coextrusion methods in which all of the constituent films are melted and laminated in a desired order in a molten state by a method such as the coextrusion multilayer die method or the feed block method, and then formed into a film shape. In many cases, it requires large-scale manufacturing equipment, and there are cases where there is a limit to interlayer adhesion strength, etc., compared to laminates that use adhesives.
• An object of the present invention is to provide a laminated film that does not degrade the quality of recycled plastic, is easy to manufacture, and maintains functionality such as interlayer adhesive strength.
• the present invention includes a first substrate, a second substrate, and an adhesive layer disposed between the first substrate and the second substrate, wherein the first and the A laminate in which the second substrate is made of a thermoplastic resin whose main component is an olefin resin, and the adhesive layer is made of an adhesive whose main component is an olefin resin (A) modified with an acid and/or hydroxyl group. provide the film.
• the present invention also provides a packaging material comprising the laminated film described above.
• An object of the present invention is to provide a laminated film that does not degrade the quality of recycled plastics, is easy to manufacture, and maintains functionality such as interlayer adhesive strength.
• the first substrate used in the present invention is a film made of a thermoplastic resin containing an olefin resin as a main component (sometimes referred to as a sheet, but is referred to as a film in the present invention.
• the first substrate may be referred to as film (1)) can be used without particular limitation.
• olefin-based resins include polyethylenes such as low-density polyethylene, medium-density polyethylene, high-density polyethylene, linear low-density polyethylene, polypropylene, ethylene-propylene copolymers, and ⁇ -olefin polymers.
• ethylene-vinyl acetate copolymer ethylene-vinyl alcohol copolymer, ethylene-acrylic acid copolymer, ethylene-methyl methacrylate copolymer, ethylene-ethyl acrylate copolymer, cyclic olefin resin, ionomer resin, poly olefin resins such as methylpentene; and modified olefin resins obtained by modifying olefin resins with acrylic acid, methacrylic acid, maleic anhydride, fumaric acid and other unsaturated carboxylic acids.
• Biomass films are sold by various companies, and for example, sheets listed in the list of certified biomass products described by the Japan Organic Resources Association can be used.
• biomass-derived ethylene glycol is produced from biomass-derived ethanol (biomass ethanol).
• biomass-derived ethylene glycol can be obtained by a method in which biomass ethanol is converted into ethylene glycol via ethylene oxide by a conventionally known method.
• commercially available biomass ethylene glycol may be used, and for example, biomass ethylene glycol commercially available from India Glycol can be preferably used.
• Radiocarbon 14C exists in the atmosphere at a rate of 1 in 1012, and this rate does not change even with carbon dioxide in the atmosphere. Therefore, the carbon of the plant-derived resin contains radioactive carbon 14C. In contrast, the carbon of the fossil fuel-derived resin contains almost no radioactive carbon 14C. Therefore, by measuring the concentration of radioactive carbon 14C in the resin with an accelerator mass spectrometer, the content ratio of the plant-derived resin in the resin, that is, the degree of biomass plasticity can be obtained.
• plant-derived low-density polyethylene which is a biomass plastic having a biomass plastic degree of 80% or more, preferably 90% or more, as defined by ISO 16620 or ASTM D6866
• plant-derived low-density polyethylene which is a biomass plastic having a biomass plastic degree of 80% or more, preferably 90% or more, as defined by ISO 16620 or ASTM D6866
• Examples of plant-derived low-density polyethylene, which is a biomass plastic having a biomass plastic degree of 80% or more, preferably 90% or more, as defined by ISO 16620 or ASTM D6866 include, for example, Braskem's product names "SBC818" and "SPB608". "SBF0323HC”, “STN7006”, “SEB853", “SPB681” and the like can be mentioned, and films using these as raw materials can be preferably used.
• biomass polyolefin films such as biomass polyethylene films containing polyethylene resins made from biomass-derived ethylene glycol and biomass polyethylene-polypropylene films are also available.
• the polyethylene-based resin is not particularly limited except that the biomass-derived ethylene glycol is used as a part of the raw material.
• ethylene- ⁇ -olefin copolymer containing 90% by mass or more of units can be used alone or in combination of two or more.
• the ⁇ -olefin constituting the copolymer of ethylene and ⁇ -olefin is not particularly limited, and may be 1-butene, 4-methyl-1-pentene, 1-hexene, 1-octene, or the like having 4 to 10 carbon atoms. 8 ⁇ -olefins.
• Known polyethylene resins such as low density polyethylene resins, medium density polyethylene resins and linear low density polyethylene resins can be used.
• linear low-density polyethylene resin (a copolymer of ethylene and 1-hexene, or ethylene and 1-octene) are preferred, and linear low density polyethylene resins having a density of 0.910 to 0.925 g/cm3 are more preferred.
• the biomass film may be a laminate obtained by laminating a plurality of biomass films, or may be a laminate of a conventional petroleum-based film and a biomass film.
• the film (1) may be subjected to any surface treatment, such as corona discharge treatment, ozone treatment, low-temperature plasma treatment using oxygen gas or nitrogen gas, glow discharge treatment, flame treatment, physical treatment, or chemical treatment. Chemical treatment such as oxidation treatment using , or other treatment may be applied.
• surface treatment such as corona discharge treatment, ozone treatment, low-temperature plasma treatment using oxygen gas or nitrogen gas, glow discharge treatment, flame treatment, physical treatment, or chemical treatment.
• Chemical treatment such as oxidation treatment using , or other treatment may be applied.
• the film (1) can be produced from the above-described resin by a conventionally known film-forming method such as an extrusion method, a cast molding method, a T-die method, a cutting method, and an inflation method. It may be an unstretched film, or it may be stretched uniaxially or biaxially using a tenter method, a tubular method, or the like, from the viewpoint of the strength, dimensional stability, and heat resistance of the film (1). may
• the film (1) may contain additives as necessary. Specifically, it improves workability, heat resistance, weather resistance, mechanical properties, dimensional stability, antioxidant properties, slip properties, releasability, flame resistance, mold resistance, electrical properties, strength, etc.
• plastic compounds and additives such as elastomers, lubricants, cross-linking agents, antioxidants, ultraviolet absorbers, light stabilizers, fillers, reinforcing agents, antistatic agents, and pigments can be added. can. The amount of additive added is adjusted within a range that does not affect other performances and recyclability.
• the film thickness of the film (1) is not particularly limited, and may be appropriately selected within the range of 0.1 to 300 ⁇ m from the viewpoint of moldability and transparency. It is preferably in the range of 0.3 to 100 ⁇ m. If it is less than 0.1 ⁇ m, the strength will be insufficient, and if it exceeds 300 ⁇ m, the rigidity will be too high, which may make processing difficult.
• the film (1) may be provided with a barrier layer for the purpose of providing barrier properties against water vapor, oxygen, alcohol, inert gases, volatile organic substances (fragrance), and the like.
• a coating layer such as a polyvinylidene chloride coat (K-coat), a metal deposition layer such as aluminum, and an inorganic deposition layer such as silica or alumina can be used.
• the film (1) may be provided with a coating layer for the purpose of improving ink receptivity when providing a printing layer, which will be described later.
• the second substrate used in the present invention is a film (sometimes referred to as a sheet) made of a thermoplastic resin containing an olefin resin as a main component, similar to the first substrate (film (1)). However, in the present invention, it is referred to as a film, and the second substrate may be referred to as a film (2).
• the type of olefinic resin that is the raw material of the film (2), the method for producing the film (2), the type of additives, the film thickness, etc., may be the same as those for the first base material.
• the first substrate, i.e. film (1), and the second substrate, i.e. film (2), may be a combination of completely the same films or may be a combination of different films within the above range. .
• the adhesive layer used in the present invention is characterized by comprising an adhesive containing an olefinic resin (A) having an acid group, an acid anhydride group and/or a hydroxyl group as a main component.
• an acid-modified olefin resin that is a copolymer of an olefin-based monomer and an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride is referred to as an "acid-modified olefin resin (A-1)".
• An acid-modified olefin resin obtained by graft-modifying an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride to an acid-modified olefin resin is referred to as "acid-modified olefin resin (A-2)", and an olefin resin having a hydroxyl group is referred to as "hydroxyl group Olefin resin (A-3) having
• an acid-modified olefin resin (A-1), acid-modified olefin resin (A-2) As the olefin resin having an acid group and/or an acid anhydride group, an acid-modified olefin resin (A -1) and an acid-modified olefin resin (A-2), which is a resin obtained by graft-modifying an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride to a polyolefin.
• Olefin monomers used for preparing the acid-modified olefin resin (A-1) include olefins having 2 to 8 carbon atoms, such as ethylene, propylene, isobutylene, 1-butene, 4-methyl-1-pentene, Examples include hexene and vinylcyclohexane. Among these, olefins having 2 to 8 carbon atoms are preferred, and ethylene, propylene, and 1-butene are more preferred, and their combined use is particularly preferred, since they provide particularly good adhesive strength.
• ethylenically unsaturated carboxylic acids or ethylenically unsaturated carboxylic anhydrides used for copolymerization with olefinic monomers include acrylic acid, methacrylic acid, maleic acid, itaconic acid, citraconic acid, mesaconic acid, and maleic anhydride.
• the reactivity with olefin-based monomers and the reactivity of acid anhydride after copolymerization are particularly excellent, and the molecular weight of the compound itself is small and the functional group concentration is high when it is made into a copolymer.
• the acid-modified olefin resin (A-1) in addition to the olefinic monomer, ethylenically unsaturated carboxylic acid or ethylenically unsaturated carboxylic acid anhydride, other compounds having ethylenically unsaturated groups such as styrene, Butadiene, isoprene, etc. may be used in combination.
• Polyolefins used for preparing the acid-modified olefin resin (A-2) include homopolymers and copolymers of olefins having 2 to 8 carbon atoms, and copolymers of olefins having 2 to 8 carbon atoms and other monomers.
• Examples include polymers, and specific examples include polyethylene such as high-density polyethylene (HDPE), low-density polyethylene (LDPE), linear low-density polyethylene resin, polypropylene, polyisobutylene, poly(1-butene), Poly(4-methyl-1-pentene), polyvinylcyclohexane, ethylene/propylene block copolymer, ethylene/propylene random copolymer, ethylene/1-butene copolymer, ethylene/4-methyl-1-pentene copolymer ⁇ -olefin copolymers such as coalescence, ethylene/hexene copolymers, ethylene/vinyl acetate copolymers, ethylene/methyl methacrylate copolymers, ethylene/vinyl acetate/methyl methacrylate copolymers, propylene/1-butene Examples include copolymers, ethylene/propylene/1-butene copolymers, and the like.
• polyethylene such as high
• homopolymers of olefins having 2 to 8 carbon atoms and copolymers of two or more kinds of olefins having 2 to 8 carbon atoms are preferred from the viewpoint of particularly good adhesive strength.
• Propylene copolymers, ethylene/1-butene copolymers, propylene/1-butene copolymers, and ethylene/propylene/1-butene copolymers are preferred.
• ethylenically unsaturated carboxylic acid or ethylenically unsaturated carboxylic acid anhydride used for graft modification with the polyolefin those used for copolymerization with the olefinic monomer in the preparation of the above-mentioned acid-modified olefin resin (A-1) can be used.
• Maleic anhydride is preferable because the reactivity of the functional group after graft modification is high and the functional group concentration of the graft-modified polyolefin is high. These can be used alone or in combination of two or more.
• an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride with a polyolefin by graft modification specifically, the polyolefin is melted, and the ethylenically unsaturated carboxylic acid or ethylenically unsaturated carboxylic acid is added thereto.
• a method of adding an acid anhydride (grafting monomer) for a graft reaction dissolving a polyolefin in a solvent to form a solution, adding an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride to the solution and allowing the graft reaction to occur.
• Polyolefin dissolved in an organic solvent is mixed with ethylenically unsaturated carboxylic acid or ethylenically unsaturated carboxylic acid anhydride, heated at a temperature above the softening temperature or melting point of polyolefin, and radically polymerized and hydrogenated in a molten state.
• a method of carrying out an abstraction reaction at the same time and the like can be mentioned.
• the graft reaction in the presence of a radical initiator in order to efficiently graft-copolymerize the graft monomer.
• the graft reaction is usually carried out at 60-350°C.
• the ratio of the radical initiator to be used is usually in the range of 0.001 to 1 part by weight per 100 parts by weight of polyolefin before modification.
• organic peroxides are preferred, such as benzoyl peroxide, dichlorobenzoyl peroxide, dicumyl peroxide, di-tert-butyl peroxide, 2,5-dimethyl-2,5-di(peroxidobenzoate)hexyne-3, 1,4-bis(tert-butylperoxyisopropyl)benzene, lauroyl peroxide, tert-butylperacetate, 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne-3,2,5-dimethyl- 2,5-di(tert-butylperoxy)hexane, tert-butyl perbenzoate, tert-butyl perphenylacetate, tert-butyl perisobutyrate, tert-butyl per-sec-octoate, tert-butyl perpivalate, chloro Examples include mil perpivalate
• the most suitable radical initiator may be selected according to the grafting reaction process, but usually dicumyl peroxide, di-tert-butyl peroxide, 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne Dialkyl peroxides such as -3,2,5-dimethyl-2,5-di(tert-butylperoxy)hexane and 1,4-bis(tert-butylperoxyisopropyl)benzene are preferably used.
• the acid-modified olefin resin (A-1) or the acid-modified olefin resin (A-2) as the olefin resin (A) it is preferable to use one having an acid value of 1 to 200 mgKOH/g.
• Olefin resins (A-3) having hydroxyl groups include copolymers of polyolefin with hydroxyl group-containing (meth)acrylic acid esters or hydroxyl group-containing vinyl ethers, and polyolefins grafted with hydroxyl group-containing (meth)acrylic acid esters or hydroxyl group-containing vinyl ethers. Examples include modified resins. Polyolefins similar to those used for preparing the olefin resin (A-2) can be used. As a modification method, a method similar to the method for preparing the acid-modified olefin resins (A-1) and (A-2) can be used.
• Hydroxyl group-containing (meth)acrylic acid esters used for modification include hydroxyethyl (meth)acrylate, hydroxypropyl (meth)acrylate, glycerol (meth)acrylate, lactone-modified hydroxyethyl (meth)acrylate, and polyethylene glycol mono(meth)acrylate. , polypropylene glycol mono(meth)acrylate and the like.
• hydroxyl group-containing vinyl ethers include 2-hydroxyethyl vinyl ether, diethylene glycol monovinyl ether, 4-hydroxybutyl vinyl ether and the like.
• the olefin resin (A-3) having hydroxyl groups is used as the olefin resin (A), it is preferable to use one having a hydroxyl value of 1 to 200 mgKOH/g.
• the polyolefin used for preparing the acid-modified olefin resin (A-2) or the olefin resin (A-3) having a hydroxyl group may be used as it is without modification.
• the weight average molecular weight of the olefin resin (A) is preferably 40,000 or more in order to improve adhesion. Moreover, the weight-average molecular weight of the olefin resin (A) is preferably 250,000 or less in order to ensure appropriate fluidity.
• the weight average molecular weight (Mw) and number average molecular weight (Mn) are values measured by gel permeation chromatography (GPC) under the following conditions.
• HLC-8320GPC manufactured by Tosoh Corporation Column
• TSKgel 4000HXL TSKgel 3000HXL
• TSKgel 2000HXL TSKgel 1000HXL manufactured by Tosoh Corporation Detector
• RI differential refractometer
• Multi-station GPC-8020modelII manufactured by Tosoh Corporation Measurement conditions
• Monodisperse polystyrene Sample 0.2 mass% tetrahydrofuran solution in terms of resin solid content filtered through a microfilter (100 ⁇ l)
• the melting point of the olefin resin (A) is preferably 40°C or higher, more preferably 50°C or higher, and more preferably 60°C or higher.
• the melting point of the olefin resin (A) is preferably 120°C or lower, more preferably 90°C or lower, and even more preferably 85°C or lower.
• the melting point of the olefin resin is measured by DSC (differential scanning calorimetry). Specifically, after the temperature is raised from the temperature drop target temperature to the temperature rise target temperature at 10 ° C./min, after cooling to the temperature drop target temperature at 10 ° C./min to remove the heat history, the temperature is raised again at 10 ° C./min. The temperature rises to a point. Let the peak temperature at the time of heating up for the second time be a melting point. Further, the temperature to be lowered is set to a temperature lower than the crystallization temperature by 50° C. or more, and the temperature to be raised is set to a temperature higher than the melting temperature by about 30° C. or more. The temperature to be lowered and the temperature to be raised are determined by trial measurement.
• DSC differential scanning calorimetry
• the curing agent (B) used in the present invention is not particularly limited, and is a curing agent capable of cross-linking acid groups, acid anhydride groups and/or hydroxyl groups, i.e., capable of cross-linking acid groups, acid anhydride groups and/or hydroxyl groups.
• Any curing agent (B) having a reactive group can be used without particular limitation. Specifically, it is preferably at least one compound selected from the group consisting of isocyanate compounds, epoxy compounds, carbodiimide compounds, silane coupling agents, and metal compounds.
• polyfunctional isocyanate compounds are preferable from the viewpoint of curability.
• Polyfunctional isocyanate compounds include 2,4-tolylene diisocyanate, 2,6-tolylene diisocyanate, xylylene diisocyanate, diphenylmethane diisocyanate, isophorone diisocyanate, 1,5-naphthalene diisocyanate, hexamethylene diisocyanate, bis(4-isocyanatocyclohexyl )
• Diisocyanates such as methane or hydrogenated diphenylmethane diisocyanate, and compounds derived from these, i.e., isocyanurate forms, adduct forms, biuret forms, uretdione forms, allophanate forms, prepolymers having an isocyanate residue (diisocyanate and a low polymer obtained from a polyol), a compound in which a part of the isocyan
• a compound obtained by reacting a part of the isocyanate groups of the polyfunctional isocyanate compound as described above with a compound reactive with the isocyanate groups may be used as the curing agent.
• Compounds reactive with isocyanate groups include compounds containing amino groups such as butylamine, hexylamine, octylamine, 2-ethylhexylamine, dibutylamine, ethylenediamine, benzylamine, and aniline: methanol, ethanol, propanol, isopropanol.
• the epoxy compound is not particularly limited as long as it is a compound having an epoxy group in the molecule.
• Polyglycidyl ether type epoxy resins of aliphatic polyols such as glycerin, sorbitol, spiroglycol or hydrogenated bisphenol A; bisphenol type epoxy resins such as bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, bisphenol AD type epoxy resin; Aromatic epoxy resins such as novolac-type epoxy resins, which are glycidyl ales of phenolic novolak resins and cresol novolac resins; Polyglycidyl ethers of polyols which are ethylene oxide or propylene oxide adducts of aromatic polyhydroxy compounds such as bisphenol A, bisphenol F, bisphenol S and bisphenol AD; Polyglycidyl ether type epoxy resin of polyether polyol such as polyethylene glycol, polypropylene glycol or polytetramethylene glycol; bis(3,4-ep
• the epoxy compound used in the present invention preferably has two or more epoxy groups and one or more hydroxyl groups in one molecule and has a weight average molecular weight of 3000 or less.
• Carbodiimide compounds include N,N'-di-o-toluylcarbodiimide, N,N'-diphenylcarbodiimide, N,N'-di-2,6-dimethylphenylcarbodiimide, N,N'-bis(2,6 -diisopropylphenyl)carbodiimide, N,N'-dioctyldecylcarbodiimide, N-triyl-N'-cyclohexylcarbodiimide, N,N'-di-2,2-tert.
• silane coupling agent examples include ⁇ -aminopropyltriethoxysilane, ⁇ -aminopropyltrimethoxysilane, N- ⁇ (aminoethyl)- ⁇ -aminopropyltrimethoxysilane, N- ⁇ (aminoethyl)- ⁇ - aminosilanes such as aminopropyltrimethyldimethoxysilane and N-phenyl- ⁇ -aminopropyltrimethoxysilane; ⁇ -(3,4-epoxycyclohexyl)ethyltrimethoxysilane, ⁇ -glycidoxypropyltrimethoxysilane, ⁇ -glycides Epoxysilanes such as xypropyltriethoxysilane; Vinylsilanes such as vinyltris( ⁇ -methoxyethoxy)silane, vinyltriethoxysilane, vinyltrimethoxysilane,
• the metal compound can be used without particular limitation as long as it forms an ionic cross-linking bond with the olefin resin (A).
• it is a compound containing a metal ion, and examples thereof include metal oxides, hydroxides, carbonates, bicarbonates, acetates, formates, methoxides, ethoxides, and the like.
• metal ions include monovalent ions such as Li + , Na + , K + , Ag + , and Cu + , and divalent ions such as Cu 2+ , Ba 2+ , Zn 2+ , and Fe 2+ . Two or more kinds of these metal ions can be mixed and included as needed.
• aziridine group-containing compounds examples include N,N'-hexamethylene-1,6-bis(1-aziridinecarboxamide) and N,N'-diphenylmethane-4,4'-bis(1-aziridinecarboxamide).
• trimethylolpropane-tri- ⁇ -aziridinylpropionate trimethylolpropane-tri- ⁇ -aziridinylpropionate
• N,N′-toluene-2,4-bis(1-aziridinecarboxamide) triethylene melamine
• trimethylolpropane-tri- ⁇ (2 -methylaziridine)propionate bisisophthaloyl-1-2-methylaziridine, tri-1-aziridinylphosphine oxide, tris-1-2-methylaziridinephosphine oxide and the like.
• Oxazolines include monooxazoline compounds such as 2-oxazoline, 2-methyl-2-oxazoline, 2-phenyl-2-oxazoline, 2,5-dimethyl-2-oxazoline and 2,4-diphenyl-2-oxazoline; ,2′-(1,3-phenylene)-bis(2-oxazoline), 2,2′-(1,2-ethylene)-bis(2-oxazoline), 2,2′-(1,4butylene) -bis(2-oxazoline), 2,2'-(1,4-phenylene)-bis(2-oxazoline) and the like.
• monooxazoline compounds such as 2-oxazoline, 2-methyl-2-oxazoline, 2-phenyl-2-oxazoline, 2,5-dimethyl-2-oxazoline and 2,4-diphenyl-2-oxazoline
• ,2′-(1,3-phenylene)-bis(2-oxazoline) 2,2′-(1,2-ethylene)-bis(2-oxazoline
• Amino resins include melamine resins, benzoguanamine resins, and urea resins.
• the amount of the curing agent (B) compounded is preferably 0.01 parts by mass or more, more preferably 0.1 parts by mass or more, and 0.5 parts by mass with respect to 100 parts by mass of the olefin resin (A). More preferably, it is at least 1 part by mass.
• the amount of the curing agent (B) compounded is preferably 50 parts by mass or less, more preferably 35 parts by mass or less, and 25 parts by mass or less with respect to 100 parts by mass of the olefin resin (A). is more preferred. Thereby, excellent adhesiveness can be exhibited.
• the adhesive used in the present invention can secure fluidity and develop appropriate coatability by blending an organic solvent.
• an organic solvent is not particularly limited as long as it can be volatilized and removed by heating in the drying process during adhesive coating.
• aromatic organic solvents such as toluene and xylene; n-hexane; Aliphatic organic solvents such as n-heptane; Alicyclic organic solvents such as cyclohexane and methylcyclohexane; Halogen organic solvents such as trichlorethylene, dichloroethylene, chlorobenzene and chloroform; Ketone solvents such as methyl ethyl ketone, methyl isobutyl ketone and cyclohexanone Ester solvents such as ethyl acetate and butyl acetate; Alcohol solvents such as ethanol, methanol, n-propanol, 2-propanol (isopropyl alcohol), butanol and hexan
• Ether-based solvents such as diethylene glycol monomethyl ether, triethylene glycol monomethyl ether, and propylene glycol monomethyl ether
• Glycol ester-based solvents such as ethylene glycol monomethyl ether acetate, propylene glycol monomethyl ether acetate, and diethylene glycol monoethyl ether acetate Examples include solvents and the like, and these may be used alone or in combination of two or more.
• the solubility is excellent. It is preferable to use a mixed solvent of an organic solvent and an ester solvent. In particular, when an olefin resin having an acid group, an acid anhydride group and/or a hydroxyl group is used, it is preferable to use a mixed solvent of methylcyclohexane and ethyl acetate because of its excellent solubility.
• the amount of the organic solvent used is preferably such that the ratio of the olefin resin (A) to the total weight of the olefin resin (A) and the organic solvent is 10 to 30% by mass. As a result, the adhesive can be excellent in coatability and wettability to the substrate.
• Adhesives used in the present invention may optionally include tackifiers, plasticizers, thermoplastic elastomers, reactive elastomers, phosphoric compounds, silane coupling agents, adhesion promoters, metal catalysts, amine catalysts, fatty
• additives such as group cyclic amide compounds, titanium chelate complexes, and esterification catalysts can be used. The content of these additives may be appropriately adjusted within a range that does not impair the functions of the adhesive of the present invention.
• Tackifiers that can be used here include, for example, rosin-based or rosin-ester-based tackifiers, terpene-based or terpene-phenol-based tackifiers, saturated hydrocarbon resins, coumarone-based tackifiers, and coumarone-indene-based tackifiers.
• tackifier, styrene resin-based tackifier, xylene resin-based tackifier, phenol resin-based tackifier, and petroleum resin-based tackifier Each of these may be used alone, or two or more of them may be used in combination.
• plasticizers include polyisoprene, polybutene, and process oil.
• thermoplastic elastomers include styrene/butadiene copolymer (SBS), hydrogenated styrene/butadiene copolymer (SEBS), SBBS, and styrene/isoprene. Hydrogenated copolymers (SEPS), styrene block copolymers (TPS), olefinic elastomers (TPO), etc., and reactive elastomers obtained by acid-modifying these elastomers can be mentioned.
• phosphoric acid compounds include phosphoric acids such as hypophosphorous acid, phosphorous acid, orthophosphoric acid and hypophosphoric acid; condensed phosphoric acids such as metaphosphoric acid, pyrophosphoric acid, tripolyphosphoric acid, polyphosphoric acid and ultraphosphoric acid; monomethyl orthophosphate, monoethyl orthophosphate, monopropyl orthophosphate, monobutyl orthophosphate, mono-2-ethylhexyl orthophosphate, monophenyl orthophosphate, monomethyl phosphite, monoethyl phosphite, monopropyl phosphite, monobutyl phosphite , mono-2-ethylhexyl phosphite, monophenyl phosphite, di-2-ethylhexyl orthophosphate, diphenyl orthophosphate dimethyl phosphite, diethyl phosphite, dipropyl phosphite, dibuty
• Adhesion promoters include 2-methylimidazole, 1,2-dimethylimidazole, 2-phenyl-4-methylimidazole, 2-ethyl-4-methylimidazole, 1-benzyl-2-methylimidazole, 1-cyanoethyl-2 - imidazole compounds such as ethyl-4-methylimidazole, triethylamine, triethylenediamine, N'-methyl-N-(2-dimethylaminoethyl)piperazine, 1,8-diazabicyclo[5.4.0]undecene (DBU) , 1,5-diazabicyclo[4.3.0]-nonene, 6-dibutylamino-1,8-diazabicyclo[5.4.0]undecene and other tertiary amines and these tertiary amines in phenol, octyl Acids, amine salts with quaternized tetraphenylborate salts, etc.
• Metal-based catalysts include metal complex-based, inorganic metal-based, and organic metal-based catalysts.
• the metal complex catalyst a group consisting of Fe (iron), Mn (manganese), Cu (copper), Zr (zirconium), Th (thorium), Ti (titanium), Al (aluminum), Co (cobalt)
• acetylacetonate salts of metals selected from the above such as iron acetylacetonate, manganese acetylacetonate, copper acetylacetonate, zirconia acetylacetonate and the like.
• iron acetylacetonate Fe(acac)3
• manganese acetylacetonate Mn(acac)2
• inorganic metal-based catalysts examples include those selected from Sn, Fe, Mn, Cu, Zr, Th, Ti, Al, Co, and the like. These may be used alone or in combination of two or more.
• Organometallic catalysts include organozinc compounds such as zinc octylate, zinc neodecanoate, and zinc naphthenate; , dioctyltin dilaurate, dibutyltin oxide, dibutyltin dichloride and other organic tin compounds, nickel octylate, nickel naphthenate and other organic nickel compounds, cobalt octylate, cobalt naphthenate and other organic cobalt compounds, bismuth octylate, neodecanoic acid
• organic bismuth compounds such as bismuth and bismuth naphthenate
• titanium compounds such as tetraisopropyloxytitanate, dibutyltitanium dichloride, tetrabutyltitanate and butoxytitanium trichloride. These may be used alone or in combination of two or more.
• Amine catalysts include triethylenediamine, 2-methyltriethylenediamine, quinuclidine, 2-methylquinuclidine, N,N,N',N'-tetramethylethylenediamine, N,N,N',N'-tetramethyl Propylenediamine, N,N,N',N',N''-pentamethyldiethylenetriamine, N,N,N',N'',N'-pentamethyl-(3-aminopropyl)ethylenediamine, N,N,N', N′′,N′′-pentamethyldipropylenetriamine, N,N,N′,N′-tetramethylhexamethylenediamine, bis(2-dimethylaminoethyl)ether, dimethylethanolamine, dimethylisopropanolamine, dimethylaminoethoxyethanol , N,N-dimethyl-N'-(2-hydroxyethyl)ethylenediamine, N,N-dimethyl
• Aliphatic cyclic amide compounds include, for example, ⁇ -valerolactam, ⁇ -caprolactam, ⁇ -enanthollactam, ⁇ -capryllactam, ⁇ -propiolactam and the like.
• ⁇ -caprolactam is more effective in accelerating hardening. These may be used alone or in combination of two or more.
• a titanium chelate complex is a compound whose catalytic activity is enhanced by ultraviolet irradiation, and a titanium chelate complex having an aliphatic or aromatic diketone as a ligand is preferable from the viewpoint of excellent curing acceleration effect.
• a titanium chelate complex having an aliphatic or aromatic diketone as a ligand is preferable from the viewpoint of excellent curing acceleration effect.
• those having alcohols having 210 carbon atoms as ligands are preferred from the viewpoint that the effects of the present invention are more pronounced. These may be used alone or in combination of two or more.
• the esterification catalyst is preferably a polymerization catalyst comprising at least one metal selected from the group consisting of Groups 2, 4, 12, 13, 14 and 15 of the Periodic Table, or a compound of the metal.
• Polymerization catalysts composed of such metals or metal compounds thereof include metals such as Ti, Sn, Zn, Al, Zr, Mg, Hf and Ge, compounds of these metals, more specifically titanium tetraisopropoxide, titanium Tetrabutoxide, titanium oxyacetylacetonate, tin octoate, 2-ethylhexane tin, zinc acetylacetonate, zirconium tetrachloride, zirconium tetrachloride tetrahydrofuran complex, hafnium tetrachloride, hafnium tetrachloride tetrahydrofuran complex, germanium oxide, tetraethoxygermanium etc. These may be used alone or in combination of two or
• the adhesive used in the present invention includes a leveling agent, inorganic fine particles such as colloidal silica and alumina sol, polymethyl methacrylate-based organic fine particles, antifoaming agents, anti-sagging agents, wetting and dispersing agents, viscosity Regulators, UV absorbers, metal deactivators, peroxide decomposers, flame retardants, reinforcing agents, plasticizers, lubricants, rust inhibitors, fluorescent brighteners, inorganic heat absorbers, flame retardants , an antistatic agent, a dehydrating agent, and the like.
• the content of these additives may be appropriately adjusted within a range that does not impair the functions of the adhesive of the present invention.
• the adhesive used in the present invention can be adjusted by mixing the components described above. At this time, each component may be mixed at the same time to form an adhesive, but the premixture is adjusted by mixing components other than the curing agent (B) in advance, and the curing agent (B) is mixed when the adhesive is used. It is preferable to use a two-liquid type adhesive that is used because the adhesive is excellent in stability and workability.
• a laminated film of the present invention comprises a first substrate, a second substrate, and an adhesive layer disposed between the first substrate and the second substrate, and the second base material is made of a thermoplastic resin containing an olefin resin as a main component, and the adhesive layer is made of an adhesive containing an olefin resin (A) modified with an acid and/or hydroxyl group as a main component.
• the layer structure be as simple as possible, but from the viewpoint of distribution of the packaging material, it is often necessary to print to indicate the contents of the packaging material and the description and name of the product.
• Liquid inks such as gravure printing inks and flexographic printing inks are often used as printing inks for this purpose.
• the printed layer is a layer on which characters, figures, symbols, and other desired patterns are printed using liquid ink or the like.
• the position where the laminate is provided is arbitrary.
• Liquid ink as used herein is a general term for solvent-based inks used in gravure printing or flexographic printing. It may contain a resin, a colorant, and a solvent as essential components, or it may be a so-called clear ink that contains a resin and a solvent but does not substantially contain a colorant.
• Resins used in liquid inks are not particularly limited, and examples include acrylic resins, polyester resins, styrene resins, styrene-maleic acid resins, maleic acid resins, polyamide resins, polyurethane resins, vinyl chloride-vinyl acetate copolymer resins, Vinyl chloride-acrylic copolymer resin, ethylene-vinyl acetate copolymer resin, vinyl acetate resin, polyvinyl chloride resin, chlorinated polypropylene resin, cellulose-based resin, epoxy resin, alkyd resin, rosin-based resin, rosin-modified maleic acid resin , ketone resins, cyclized rubbers, chlorinated rubbers, butyrals, petroleum resins, etc., and may be used alone or in combination of two or more. At least one, or two or more selected from polyurethane resins, vinyl chloride-vinyl acetate copolymer resins, and cellulose resins are preferred.
• Colorants used in liquid inks include inorganic pigments such as titanium oxide, red iron oxide, antimony red, cadmium red, cadmium yellow, cobalt blue, Prussian blue, ultramarine blue, carbon black, graphite, soluble azo pigments, insoluble azo pigments, and azo lakes.
• Extender pigments such as pigments, condensed azo pigments, copper phthalocyanine pigments, organic pigments such as condensed polycyclic pigments, calcium carbonate, kaolin clay, barium sulfate, aluminum hydroxide and talc.
• the organic solvent used for liquid ink preferably does not contain an aromatic hydrocarbon-based organic solvent. More specifically, alcohol-based organic solvents such as methanol, ethanol, n-propanol, isopropanol and butanol, ketone-based organic solvents such as acetone, methyl ethyl ketone and methyl isobutyl ketone, methyl acetate, ethyl acetate, propyl acetate and butyl acetate.
• alcohol-based organic solvents such as methanol, ethanol, n-propanol, isopropanol and butanol
• ketone-based organic solvents such as acetone, methyl ethyl ketone and methyl isobutyl ketone, methyl acetate, ethyl acetate, propyl acetate and butyl acetate.
• ester-based organic solvents n-hexane, n-heptane, n-octane and other aliphatic hydrocarbon-based organic solvents, cyclohexane, methylcyclohexane, ethylcyclohexane, cycloheptane, cyclooctane and other alicyclic hydrocarbon-based organic solvents etc., and can be used alone or in combination of two or more.
• the laminated film of the present invention includes a first substrate, a second substrate, and an adhesive layer disposed between the first substrate and the second substrate. Although it is a laminated film, it may be further laminated with another base material other than the first base material and the second base material.
• it may be a laminated film having a structure in which a plurality of substrates are laminated.
• the raw material of the other base material is a thermoplastic resin containing an olefin resin as a main component because of its excellent recyclability.
• the kind of olefinic resin used as the raw material, the method for producing the film, the kind of additives, the film thickness, etc. may be the same as those of the first base material and the second base material.
• the laminated film of the present invention and other substrates are laminated together, it is preferable to use the above-mentioned adhesive because of its excellent recyclability and adhesiveness.
• the laminated film of the present invention is obtained by bonding the first base material and the second base material together with the adhesive. Moreover, even when other base materials are included in the composition, it is preferable to use the above-mentioned adhesive because of its excellent recyclability and adhesiveness.
• the adhesive is a solvent type
• the adhesive is applied to either the first base material or the second base material using a roll such as a gravure roll, and heated in an oven or the like to form an organic solvent. After evaporating the solvent, the other is laminated to obtain the laminated film of the present invention. It is preferable to perform an aging treatment after lamination.
• the aging temperature is preferably room temperature to 80° C.
• the aging time is preferably 12 to 240 hours.
• the adhesive When the adhesive is a non-solvent type, the adhesive previously heated to about 40° C. to 100° C. is applied to either the first base material or the second base material using a gravure roll or the like. After coating using a roll, the other is immediately laminated to obtain the laminated film of the present invention. It is preferable to perform an aging treatment after lamination.
• the aging temperature is preferably room temperature to 70° C., and the aging time is preferably 6 to 240 hours.
• the amount of the adhesive to be applied is appropriately adjusted.
• the solid content is adjusted to 0.1 g/m 2 or more and 10 g/m 2 or less, preferably 0.3 g/m 2 or more and 5 g/m 2 or less.
• the coating amount of the adhesive is, for example, 0.1 g/m 2 or more and 10 g/m 2 or less, preferably 0.3 g/m 2 or more and 5 g/m 2 or less.
• the laminated film of the present invention can be used as a multilayer packaging material for the purpose of protecting foods, pharmaceuticals, and the like.
• the layer structure may vary depending on the contents, usage environment, and usage pattern.
• the package of the present invention may be appropriately provided with an easy-opening treatment or a resealing means.
• the packaging material of the present invention is obtained by using the laminated film of the present invention, stacking the laminated films with their sealant film surfaces facing each other, and then heat-sealing the peripheral edges to form a bag.
• the laminated film of the present invention is folded or overlapped so that the inner layer surface (surface of the sealant film) faces each other, and the peripheral edge is sealed, for example, by side seal type, two side seal type, There are three-side seal type, four-side seal type, envelope seal type, palm-joint seal type, pleated seal type, flat-bottom seal type, square-bottom seal type, gusset type, and other heat-sealing methods. be done.
• the packaging material of the present invention can take various forms depending on the contents, environment of use, and form of use.
• a self-supporting packaging material (standing pouch) or the like is also possible.
• As a heat sealing method known methods such as bar sealing, rotary roll sealing, belt sealing, impulse sealing, high frequency sealing and ultrasonic sealing can be used.
• first base material and the second base material of the laminated film of the present invention do not function as a sealant layer that serves as a heat-sealed portion when forming the packaging material, a further sealant layer may be added.
• a further sealant layer may be added as the sealant layer.
• an additional substrate may be laminated with the adhesive of the present invention, or an adhesive layer made of the adhesive of the present invention may be used.
• the opening is heat-sealed to manufacture a product using the packaging material of the present invention.
• filling contents include foods such as rice confectionery, bean confectionery, nuts, biscuits and cookies, wafer confectionery, marshmallows, pies, half-baked cakes, candy, snacks, bread, snack noodles, and instant noodles.
• Non-food items include cigarettes, disposable body warmers, medicines such as infusion packs, liquid laundry detergents, liquid kitchen detergents, liquid bath detergents, liquid bath soaps, liquid shampoos, liquid conditioners, cosmetics such as lotions and milky lotions, and vacuum cleaners. It can also be used as various packaging materials such as heat insulators, batteries and the like.
• the laminated film of the present invention and the packaging material comprising the laminated film of the present invention are excellent in recyclability.
• an example of a processing method for making the laminated film into a recycled plastic is shown.
• the present invention is not limited to this, and various known recycled plastic processing methods can be applied.
• the laminated film is crushed with a crusher or the like.
• a known grinder may be used as the grinder, and there is no particular limitation.
• the crushed film pieces are physically blended by melt kneading, solvent cast blending, latex blending, polymer complexes, and the like.
• a melt-kneading method is particularly common. Apparatuses for kneading include a tumbler, a Henschel mixer, a rotary mixer, a super mixer, a ribbon tumbler, a V-blender and the like. After being melted and kneaded by such a kneading device, the mixture is pelletized.
• a single-screw extruder or a multi-screw extruder is generally used for melt-kneading and pelletizing, and the film pieces may be put in as they are or after compression volume reduction treatment with or without heating.
• Banbury mixers, rollers, co-kneaders, blast mills, Plabender brautographs, etc. can also be used, and these are operated batchwise or continuously.
• the resin may be used as a molding resin and melt-kneaded in a heating cylinder of a molding machine without melt-kneading.
• isocyanate compound 1 (Adjustment of isocyanate compound 1)
• Desmodur L-75 (an adduct-type polyisocyanate in which 3 mol of tolylene diisocyanate is added to 1 mol of trimethylolpropane, manufactured by Sumika Covestro Urethane Co., Ltd.) was adjusted to a non-volatile content of 75% by mass with an ethyl acetate solution.
• Epoxy compound 1 Denacol EX-321L (trimethylolpropane polyglycidyl ether, manufactured by Nagase ChemteX Corporation) was used.
• Olefin resin 1 Adjustment of olefin resin
• UNISTOL P-901 an olefin resin having a hydroxyl group, manufactured by Mitsui Chemicals, Inc., non-volatile content 22% by mass
• Olefin resin 2 Aurorene S-5419S (an olefin resin having an acid group and an acid anhydride group, manufactured by Nippon Paper Industries Co., Ltd.) was adjusted to have a non-volatile content of 15% by mass with a methylcyclohexane and ethyl acetate solution.
• Adhesive coating liquids 1 to 8 were prepared by blending at the weight ratios shown in Table 1 below. In addition, a blank indicates unblended.
• Adhesive coating liquid 1 was applied to a biaxially stretched polypropylene film (manufactured by Toyobo Co., Ltd., Pyrene film-OT P2161, 20 ⁇ m) as a base material 1 so that the solid content weight of the adhesive was about 3.0 g / m 2 . After coating using a bar coater and volatilizing the solvent, it was laminated with a non-stretched polypropylene film (manufactured by Toyobo Co., Ltd., pyrene film-CT P1128, 30 ⁇ m) as the base material 2 using a desk calendar roll, 25 ° C. Laminated film 1 was prepared by aging for 72 hours at .
• Adhesive coating liquid 1 was applied to a biaxially stretched polypropylene film (manufactured by Toyobo Co., Ltd., Pyrene film-OT P2161, 20 ⁇ m) as a base material 1 so that the solid content weight of the adhesive was about 3.0 g / m 2 . After applying using a bar coater and volatilizing the solvent, it was laminated with a non-stretched polypropylene film (manufactured by Toyobo Co., Ltd., pyrene film-CT P1128, 30 ⁇ m) as the base material 2 using a desktop calender roll, 40 ° C. Laminated film 2 was prepared by aging for 72 hours at .
• Example 3 Laminated film 3 was prepared in the same manner as in Example 1, except that adhesive coating liquid 2 was used as the adhesive coating liquid.
• Example 4 Laminated film 4 was prepared in the same manner as in Example 2, except that adhesive coating liquid 2 was used as the adhesive coating liquid.
• Example 5 Laminated film 5 was prepared in the same manner as in Example 1, except that adhesive coating liquid 3 was used as the adhesive coating liquid.
• Example 6 A laminated film 6 was prepared in the same manner as in Example 2, except that the adhesive coating liquid 3 was used as the adhesive coating liquid.
• Example 7 Laminated film 7 was prepared in the same manner as in Example 2, except that adhesive coating liquid 4 was used as the adhesive coating liquid.
• Example 8 A laminate film 8 was prepared in the same manner as in Example 2, except that the adhesive coating liquid 5 was used as the adhesive coating liquid.
• Example 9 Laminated film 9 was prepared in the same manner as in Example 2, except that adhesive coating liquid 6 was used as the adhesive coating liquid.
• Example 10 A laminate film 10 was prepared in the same manner as in Example 2, except that the adhesive coating liquid 7 was used as the adhesive coating liquid.
• Example 11 A laminate film 11 was prepared in the same manner as in Example 2, except that the adhesive coating liquid 8 was used as the adhesive coating liquid.
• Example 12 A biaxially oriented polypropylene film (manufactured by Toyobo Co., Ltd., Pylen Film-OT P2161, 20 ⁇ m) as a base material 1 was coated with an adhesive coating liquid 2 so that the solid content weight of the adhesive was about 0.7 g / m 2 . After coating using a bar coater and volatilizing the solvent, a desktop calender roll was used as the base material 2.
• Laminated with unstretched polypropylene film manufactured by Toyobo Co., Ltd., pyrene film-CT P1128, 30 ⁇ m
• 50 Laminated film 12 was produced by aging at 0 C for 24 hours.
• Laminated film 13 was prepared in the same manner as in Example 12, except that a non-stretched polypropylene film vapor-deposited with aluminum (manufactured by Toray Advanced Film Co., Ltd., aluminum vapor-deposited barrier film VM-CPP 2703, 30 ⁇ m) was used as the base material 2. bottom.
• a non-stretched polypropylene film vapor-deposited with aluminum manufactured by Toray Advanced Film Co., Ltd., aluminum vapor-deposited barrier film VM-CPP 2703, 30 ⁇ m
• Laminated film 14 was prepared in the same manner as in Example 12 except that a biaxially stretched polypropylene film coated with polyvinyl alcohol (A-OP BH, 20 ⁇ m, manufactured by Mitsui Chemicals Tohcello Co., Ltd.) was used as the substrate 1.
• A-OP BH polyvinyl alcohol
• Adhesion strength measurement A sample of 150 mm ⁇ 15 mm was cut from the prepared laminated film and used as a specimen. Adhesion strength (unit: N/15 mm) was measured between a biaxially stretched polypropylene film and a non-stretched polypropylene film. The measurement was performed using a tensile tester (AGS-X manufactured by Shimadzu Corporation) at a peel rate of 300 mm/min by a 180° peel method and a T-type peel method. The ambient temperature during the measurement was set at 25°C. The results are shown in Tables 2, 3, 4 and 5.
• Heat seal strength measurement The heat seal strength of the laminated film obtained in Example 4 was measured. Cut a 200 mm ⁇ 100 mm piece from the laminated film, bend it to 100 mm ⁇ 100 mm so that the unstretched polypropylene film is on the inside, bend the bent part with a width of 10 mm, 1 atm, 160 ° C., 1 second under the conditions of a heat seal tester (Tester Sangyo (manufactured). A sample was cut from the heat-sealed laminated film so that the heat-sealed portion had a size of 10 mm ⁇ 15 mm and the non-heat-sealed portion had a size of 90 mm ⁇ 15 mm.
• the heat seal strength (unit: N/15 mm) was determined by attaching the non-heat-sealed portion to a tensile tester and measuring the value of the heat-sealed portion. The measurement was performed using a tensile tester (AGS-X manufactured by Shimadzu Corporation) at a peel speed of 300 mm/min by a T-type peel method. The ambient temperature during the measurement was set at 25°C. Table 6 shows the results.
• Laminated film 4 obtained in Example 4 and the unstretched polypropylene film of Comparative Example 2 were used. Each film is cut into strips with a width of 10 mm and a length of 300 mm, and is melted and kneaded at 240 ° C. and 100 rpm for 3 minutes using a twin-screw kneading extruder (manufactured by Technobell Co., Ltd., ULTnano 15TW). and immediately cooled with tap water to obtain a strand-shaped resin, which was cut to obtain a repellet sample.
• a twin-screw kneading extruder manufactured by Technobell Co., Ltd., ULTnano 15TW
• the repellet sample obtained from the laminated film 4 obtained in Example 4 is referred to as "A", and the repellet sample obtained from the unstretched polypropylene film of Comparative Example 2 is referred to as "Z".
• 9 g of the repellet sample was put into a stainless steel press picture frame mold (inner dimension 100 mm square, thickness 1 mm), sandwiched between stainless steel plates (thickness 2 mm), and compression molded at 210 ° C., 30 MPa, for 3 minutes, A plastic plate with a thickness of 1 mm was prepared, and a 1/3 size test piece of JIS K6251-5 was punched out using a Super Dumbbell Cutter SDK500 1/3 manufactured by Dumbbell Co., Ltd. and used for a tensile test. The tensile test was performed at 50 mm/min and the distance between chucks was 30 mm, and the tensile elongation was measured.
• the YI value (yellowness index) was measured according to ASTM E 313. Table 7 shows the results.
• the laminated films of the examples of the present application do not degrade the quality of recycled plastics, are easy to manufacture, and can maintain functionality such as interlayer adhesive strength.

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• 2022
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