Dispersant for blend resin, and laminate and recycled plastic using the same

Abstract

To provide a material capable of recycling a laminate using two or more kinds of thermoplastic resins incompatible with each other, and to provide a laminate and a recycled plastic using the same.SOLUTION: A dispersant for a blend resin used for a blend resin of two or more kinds of thermoplastic resins that are incompatible with each other, the dispersant for a blend resin being composed of an olefin-based resin modified with an acid, an acid anhydride, and / or vinyl acetate; a first substrate film, a second substrate film, and a resin layer A disposed between the first substrate film and the second substrate film, the first substrate film contains an olefin-based resin as a main component, the second substrate film contains a thermoplastic resin incompatible with the olefin-based resin as a main component, and the resin layer A is provided so as to be in contact with the second substrate film.SELECTED DRAWING: None

Description

[Technical Field]

[0001] The present invention relates to a dispersant for blended resins that enables the recycling of laminates containing two or more thermoplastic resins that are poorly miscible with each other, and to a laminate and recycled plastic that use the same. [Background technology]

[0002] Conventionally, packaging materials used for packaging food and daily necessities have evolved by laminating films of different resins to meet the demand for a single packaging material that not only serves the purpose of packaging but also has various high functions such as barrier properties, moisture resistance, and retort resistance (see, for example, Patent Document 1). However, in recent years, there have been complaints that these laminated films of different resins degrade the quality of recycled plastics, and there is a demand for packaging materials that are not only highly functional but also recyclable. As a recyclable packaging material, laminated films made of the same resin type (monomaterial) have been proposed, but it is still difficult to achieve the high functionality that is originally required with monomaterial laminated films.

[0003] One reason why laminated films of different resins reduce the quality of recycled plastics is that different resins, such as polyester resin and polyolefin resin, nylon resin and polyolefin resin, etc., are not easily miscible with each other (also known as poor compatibility or incompatibility). Recycled plastics are obtained by crushing recovered waste plastics after cleaning them, melting and kneading the crushed pieces, and then solidifying them. However, since resins that are not compatible with each other do not mix even when kneaded, the resulting recycled plastics are brittle and difficult to stretch. Therefore, there is a demand for a highly functional laminate film made of different resins that is recyclable and does not degrade the quality of the recycled plastic obtained.

[0004] Generally, when various molded products are produced using two or more incompatible synthetic resins, a dispersant that makes the two or more synthetic resins compatible is used to melt and knead the two or more mutually incompatible synthetic resins as uniformly as possible (see, for example, Patent Document 2). However, because these dispersants are added during melt kneading, it is not practical to select a dispersant suitable for the recovered waste plastics at a recycling site and add it during melt kneading. [Prior art documents] [Patent documents]

[0005] [Patent Document 1] Japanese Patent Application Laid-Open No. 2014-004799 [Patent Document 2] Japanese Patent Application Publication No. 1-292015 Summary of the Invention [Problem to be solved by the invention]

[0006] The object of the present invention is to provide a material that enables a laminate containing two or more mutually incompatible thermoplastic resins to be recycled, and to provide a laminate and a recycled plastic that use the same. [Means for solving the problem]

[0007] The present inventors have found that the object of the present invention can be achieved by a dispersant for blended resins, which is used for blended resins of two or more mutually incompatible thermoplastic resins, and which is characterized by comprising an olefin-based resin modified with an acid, an acid anhydride, and / or vinyl acetate.

[0008] A dispersant for blended resins, consisting of an olefin-based resin modified with acid, acid anhydride, and / or vinyl acetate, is used by directly adhering it to at least one of two or more mutually incompatible thermoplastic resins. The easiest way to obtain a laminate by adhering it is to use it as an adhesive for bonding different resin films. Because it can be used as an adhesive for bonding different resin films, it can be added to the laminate in advance. The recycled plastic obtained by directly crushing and kneading the laminate has excellent elongation and toughness because the different resins exhibit a finely dispersed structure.

[0009] That is, the present invention provides a dispersant for blended resins to be used for blended resins of two or more mutually incompatible thermoplastic resins, the dispersant for blended resins comprising an olefin-based resin modified with an acid, an acid anhydride, and / or vinyl acetate.

[0010] The present invention also provides a method for using the above-described dispersant for a blended resin, which comprises a step of directly adhering two or more mutually incompatible thermoplastic resins to at least one resin.

[0011] The present invention also provides a laminate that is the dispersant for blended resins according to claim 1 or 2, comprising a first base film, a second base film, and a resin layer A disposed between the first base film and the second base film, wherein the first base film contains an olefin-based resin as a main component, and the second base film contains a thermoplastic resin that is incompatible with the olefin-based resin as a main component, and the resin layer A is provided so as to be in contact with the second base film.

[0012] The present invention also provides a recycled plastic made from the laminate described above.

[0013] The present invention also provides a method for producing recycled plastic using the above-described laminate as a raw material, which includes the steps of crushing the laminate described in claim 4, melting and kneading the crushed pieces, and pelletizing the melted and kneaded mixture. [Effects of the Invention]

[0014] The present invention can provide a material that makes it possible to recycle a laminate that uses two or more thermoplastic resins that are incompatible with each other, and can also provide a laminate and recycled plastic that use the material. DETAILED DESCRIPTION OF THE INVENTION

[0015] (Dispersant for blended resins) The dispersant for a resin blend of the present invention is characterized by comprising an olefin resin modified with an acid, an acid anhydride, and / or vinyl acetate. Here, an acid-modified olefin resin that is a copolymer of an olefin monomer and an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride is referred to as "acid-modified olefin resin (A-1)," an acid-modified olefin resin that is a resin in which a polyolefin is graft-modified with an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride is referred to as "acid-modified olefin resin (A-2)," and an olefin resin modified with vinyl acetate is referred to as "olefin resin with vinyl acetate (A-3)."

[0016] (Acid-modified olefin resin (A-1), Acid-modified olefin resin (A-2)) Examples of the olefin resin having an acid group and / or an acid anhydride group include an acid-modified olefin resin (A-1) which is a copolymer of an olefin monomer and an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride, and an acid-modified olefin resin (A-2) which is a resin in which a polyolefin is graft-modified with an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride.

[0017] Examples of olefinic monomers used in preparing the acid-modified olefinic resin (A-1) include olefins having 2 to 8 carbon atoms, such as ethylene, propylene, isobutylene, 1-butene, 4-methyl-1-pentene, hexene, vinylcyclohexane, etc. Among these, olefins having 2 to 8 carbon atoms are preferred because they provide particularly good adhesive strength, and ethylene, propylene, and 1-butene are more preferred, and their combined use is particularly preferred.

[0018] Examples of the ethylenically unsaturated carboxylic acid or ethylenically unsaturated carboxylic acid anhydride used in copolymerization with an olefin-based monomer include acrylic acid, methacrylic acid, maleic acid, itaconic acid, citraconic acid, mesaconic acid, maleic anhydride, 4-methylcyclohex-4-ene-1,2-dicarboxylic anhydride, bicyclo[2.2.2]oct-5-ene-2,3-dicarboxylic anhydride, 1,2,3,4,5,8,9,10-octahydronaphthalene Examples of suitable maleic anhydrides include methyl-bicyclo[2.2.1]hept-5-ene-2,3-dicarboxylic anhydride, 2-octa-1,3-diketospiro[4.4]non-7-ene, bicyclo[2.2.1]hept-5-ene-2,3-dicarboxylic anhydride, maleopimaric acid, tetrahydrophthalic anhydride, methyl-bicyclo[2.2.1]hept-5-ene-2,3-dicarboxylic anhydride, methyl-norbornene-5-ene-2,3-dicarboxylic anhydride, and norborn-5-ene-2,3-dicarboxylic anhydride. Among these, maleic anhydride is particularly preferred due to its excellent reactivity with olefinic monomers, the reactivity of the resulting anhydride after copolymerization, and the low molecular weight of the compound itself, resulting in a high functional group concentration when copolymerized. These may be used alone or in combination of two or more.

[0019] In preparing the acid-modified olefin resin (A-1), in addition to the olefin monomer, ethylenically unsaturated carboxylic acid or ethylenically unsaturated carboxylic acid anhydride, other compounds having ethylenically unsaturated groups, such as styrene, butadiene, and isoprene, may be used in combination.

[0020] Examples of polyolefins used in 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 with other monomers. Specific examples include polyethylenes such as high-density polyethylene (HDPE), low-density polyethylene (LDPE), and linear low-density polyethylene resins; polypropylene; polyisobutylene; poly(1-butene); poly(4-methyl-1-pentene); polyvinylcyclohexane; α-olefin copolymers such as ethylene-propylene block copolymers, ethylene-propylene random copolymers, ethylene-1-butene copolymers, ethylene-4-methyl-1-pentene copolymers, and ethylene-hexene copolymers; ethylene-vinyl acetate copolymers; ethylene-methyl methacrylate copolymers; ethylene-vinyl acetate-methyl methacrylate copolymers; propylene-1-butene copolymers; and ethylene-propylene-1-butene copolymers. Among these, homopolymers of olefins having 2 to 8 carbon atoms and copolymers of two or more olefins having 2 to 8 carbon atoms are preferred because they provide particularly good adhesive strength, and polyethylene, polypropylene, or ethylene-propylene copolymers are particularly preferred.

[0021] The ethylenically unsaturated carboxylic acid or ethylenically unsaturated carboxylic acid anhydride used for graft-modification with polyolefin can be the same as that used for copolymerization with olefinic monomers in the preparation of the acid-modified olefinic resin (A-1) described above. Maleic anhydride is preferred because it has high reactivity of functional groups after graft-modification and a high functional group concentration in the graft-modified polyolefin. These can be used alone or in combination of two or more.

[0022] Specific examples of methods for reacting an ethylenically unsaturated carboxylic acid or an ethylenically unsaturated carboxylic acid anhydride with a polyolefin by graft modification include a method in which the polyolefin is melted and the ethylenically unsaturated carboxylic acid or the ethylenically unsaturated carboxylic acid anhydride (graft monomer) is added thereto to carry out a graft reaction; a method in which the polyolefin is dissolved in a solvent to form a solution and the ethylenically unsaturated carboxylic acid or the ethylenically unsaturated carboxylic acid anhydride is added thereto to carry out a graft reaction; and a method in which the polyolefin dissolved in an organic solvent is mixed with the ethylenically unsaturated carboxylic acid or the ethylenically unsaturated carboxylic acid anhydride and heated at a temperature equal to or higher than the softening temperature or melting point of the polyolefin to simultaneously carry out radical polymerization and hydrogen abstraction reaction in the molten state.

[0023] In either case, in order to efficiently graft copolymerize the graft monomer, it is preferable to carry out the graft reaction in the presence of a radical initiator. The graft reaction is usually carried out under conditions of 60 to 350°C. The proportion of the radical initiator used is usually in the range of 0.001 to 1 part by weight per 100 parts by weight of the polyolefin before modification.

[0024] As the radical initiator, organic peroxides are preferred, such as benzoyl peroxide, dichlorobenzoyl peroxide, dicumyl peroxide, di-tert-butyl peroxide, 2,5-dimethyl-2,5-di(peroxidebenzoate)hexyne-3, 1,4-bis(tert-butylperoxyisopropyl)benzene, lauroyl peroxide, tert-butyl peracetate, 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne-3, 2,5-dimethyl-2,5-di(tert-butylperoxy)hexane, tert-butyl perbenzoate, tert-butyl perphenyl acetate, tert-butyl perisobutyrate, tert-butyl per-sec-octoate, tert-butyl perpivalate, cumyl perpivalate, and tert-butyl perdiethyl acetate. Other azo compounds such as azobisisobutyronitrile and dimethylazoisobutyrate can also be used.

[0025] The radical initiator may be selected optimally depending on the grafting reaction process, but typically, dialkyl peroxides such as dicumyl peroxide, di-tert-butyl peroxide, 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne-3, 2,5-dimethyl-2,5-di(tert-butylperoxy)hexane, and 1,4-bis(tert-butylperoxyisopropyl)benzene are preferably used.

[0026] When an acid-modified olefin resin (A-1) or an acid-modified olefin resin (A-2) is used as the olefin resin (A), it is preferable to use one having an acid value of 1 to 200 mgKOH / g.

[0027] (Olefin Resin (A-3) Containing Vinyl Acetate) Examples of the vinyl acetate-containing olefin resin (A-3) include copolymers of polyolefins and vinyl acetate. The polyolefins used in the preparation of the olefin resin (A-2) can be used. The modification method can be the same as that used in the preparation of the acid-modified olefin resin (A-1). The polyolefins used are particularly preferably polyethylene, polypropylene, or ethylene-propylene copolymers.

[0028] When an olefin resin (A-3) having a hydroxyl group is used as the olefin resin (A), it is preferable to use one containing 5 to 20 mol % of vinyl acetate.

[0029] As the olefin resin (A), the polyolefin used in preparing the acid-modified olefin resin (A-2) or the vinyl acetate-containing olefin resin (A-3) may be used as is without modification.

[0030] To ensure good adhesiveness, the weight-average molecular weight of the olefin resin (A) is preferably 40,000 or more, and to ensure appropriate fluidity, the weight-average molecular weight of the olefin resin (A) is preferably 300,000 or less.

[0031] In the present invention, the weight average molecular weight (Mw) and number average molecular weight (Mn) are values ​​measured by gel permeation chromatography (GPC) under the following conditions.

[0032] Measuring device: Tosoh Corporation HLC-8320GPC Column: Tosoh Corporation TSKgel 4000HXL, TSKgel 3000HXL, TSKgel 2000HXL, TSKgel 1000HXL Detector: RI (differential refractometer) Data processing: Tosoh Corporation Multistation GPC-8020modelII Measurement conditions: Column temperature 40°C Solvent: Tetrahydrofuran Flow rate 0.35ml / min Standard: Monodisperse polystyrene Sample: 100 μl of tetrahydrofuran solution containing 0.2% by mass of resin solids filtered through a microfilter

[0033] The melting point of the olefin resin (A) is preferably 40° C. or higher, more preferably 50° C. or higher, and even 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.

[0034] The melting point of olefin resins is measured by DSC (differential scanning calorimetry). Specifically, the temperature is raised at 10°C / min from the final cooling temperature to the final heating temperature, then cooled at 10°C / min to the final cooling temperature to remove the thermal history, and then heated again at 10°C / min to the final heating point. The peak temperature at the second heating is taken as the melting point. The final cooling temperature is set to a temperature at least 50°C lower than the crystallization temperature, and the final heating temperature is set to a temperature at least 30°C higher than the melting point. The final cooling temperature and heating temperature are determined by trial measurements.

[0035] Among them, (1) It is preferable that the olefin resin (A) is a polypropylene resin modified with maleic anhydride, the polypropylene content is 70 to 99 mol %, and the modification rate of the maleic anhydride is 0.1 mol % or more. Also, (2) it is preferable that the olefin resin (A) is a polyethylene resin modified with maleic anhydride, the polyethylene content is 70 to 99 mol %, and the modification rate of the maleic anhydride is 0.1 mol % or more. Also, (3) it is preferable that the olefin resin (A) is a polyethylene resin modified with vinyl acetate, and the modification rate of the vinyl acetate is 5 to 20 mol % or more.

[0036] (metal compound) The dispersant for blended resins used in the present invention may be used in combination with a metal compound, etc. By using the dispersant in combination with a metal compound, it is possible to further strengthen the adhesion when used as an adhesive for bonding different types of resin films, which is the easiest method for obtaining a laminate by bonding films together, as described below.

[0037] The metal compound can be any compound that forms an ionic crosslink with the olefin resin (A). Specifically, it is a compound containing a metal ion, such as a metal oxide, hydroxide, carbonate, bicarbonate, acetate, formate, methoxide, or ethoxide. Examples of the metal ion include monovalent ions such as Li+, Na+, K+, Ag+, and Cu+, and divalent ions such as Cu2+, Ba2+, Zn2+, and Fe2+. Two or more of these metal ions can be mixed together as needed.

[0038] Other usable compounds include aziridine group-containing compounds, oxazolines, amino resins, etc. Examples of aziridine group-containing compounds include N,N'-hexamethylene-1,6-bis(1-aziridinecarboxamide), N,N'-diphenylmethane-4,4'-bis(1-aziridinecarboxamide), trimethylolpropane-tri-β-aziridinylpropionate), N,N'-toluene-2,4-bis(1-aziridinecarboxamide), triethylenemelamine, trimethylolpropane-tri-β(2-methylaziridine)propionate, bisisophthaloyl-1-2-methylaziridine, tri-1-aziridinylphosphine oxide, and tris-1-2-methylaziridinephosphine oxide.

[0039] Examples of 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, as well as 2,2'-(1,3-phenylene)-bis(2-oxazoline), 2,2'-(1,2-ethylene)-bis(2-oxazoline), 2,2'-(1,4butylene)-bis(2-oxazoline), and 2,2'-(1,4-phenylene)-bis(2-oxazoline).

[0040] Examples of the amino resin include melamine resin, benzoguanamine resin, and urea resin.

[0041] The blending amount of the metal compound is preferably 0.01 parts by mass or more, more preferably 0.1 parts by mass or more, and even more preferably 0.5 parts by mass or more, per 100 parts by mass of the olefin-based resin (A). The blending amount of the metal compound is preferably 50 parts by mass or less, more preferably 35 parts by mass or less, and even more preferably 25 parts by mass or less, per 100 parts by mass of the olefin-based resin (A). This allows for excellent adhesive properties to be achieved.

[0042] (additives) The dispersant for blend resins of the present invention can contain various additives as needed, such as a silane coupling agent, a tackifier, a plasticizer, a thermoplastic elastomer, a reactive elastomer, a phosphoric acid compound, a silane coupling agent, an adhesion promoter, a metal catalyst, an amine catalyst, an aliphatic cyclic amide compound, a titanium chelate complex, an esterification catalyst, etc. The content of these additives may be adjusted appropriately within a range that does not impair the function of the adhesive of the present invention.

[0043] (Silane coupling agent) Examples of silane coupling agents include aminosilanes such as γ-aminopropyltriethoxysilane, γ-aminopropyltrimethoxysilane, N-β(aminoethyl)-γ-aminopropyltrimethoxysilane, N-β(aminoethyl)-γ-aminopropyltrimethyldimethoxysilane, and N-phenyl-γ-aminopropyltrimethoxysilane; epoxysilanes such as β-(3,4-epoxycyclohexyl)ethyltrimethoxysilane, γ-glycidoxypropyltrimethoxysilane, and γ-glycidoxypropyltriethoxysilane; vinylsilanes such as vinyltris(β-methoxyethoxy)silane, vinyltriethoxysilane, vinyltrimethoxysilane, and γ-methacryloxypropyltrimethoxysilane; hexamethyldisilazane, γ-mercaptopropyltrimethoxysilane, and the like.

[0044] Examples of tackifiers include rosin-based or rosin ester-based tackifiers, terpene-based or terpene phenol-based tackifiers, saturated hydrocarbon resins, coumarone-based tackifiers, coumarone-indene-based tackifiers, styrene resin-based tackifiers, xylene resin-based tackifiers, phenol resin-based tackifiers, petroleum resin-based tackifiers, etc. These may be used alone or in combination of two or more.

[0045] Plasticizers include polyisoprene, polybutene, and procell oil. Thermoplastic elastomers include styrene-butadiene copolymer (SBS), hydrogenated styrene-butadiene copolymer (SEBS), SBBS, hydrogenated styrene-isoprene copolymer (SEPS), styrene block copolymer (TPS), and olefin elastomer (TPO). Reactive elastomers include acid-modified versions of these elastomers.

[0046] Examples of 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; Examples of the mono- and diesters of di-2-ethylhexyl orthophosphate, diphenyl orthophosphate, dimethyl phosphite, diethyl phosphite, dipropyl phosphite, dibutyl phosphite, di-2-ethylhexyl phosphite, diphenyl phosphite, and the like; mono- and diesters of condensed phosphoric acid and alcohols; products obtained by adding an epoxy compound such as ethylene oxide or propylene oxide to the above-mentioned phosphoric acids; and epoxy phosphoric acid esters obtained by adding the above-mentioned phosphoric acids to aliphatic or aromatic diglycidyl ethers.

[0047] Examples of adhesion promoters include imidazole compounds such as 2-methylimidazole, 1,2-dimethylimidazole, 2-phenyl-4-methylimidazole, 2-ethyl-4-methylimidazole, 1-benzyl-2-methylimidazole, and 1-cyanoethyl-2-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, and 6-dibutylamino-1,8-diazabicyclo[5.4.0]undecene (DBU). Examples of suitable amine compounds include tertiary amines such as cyclo[5.4.0]undecene, compounds obtained by converting these tertiary amines into amine salts with phenol, octylic acid, quaternized tetraphenylborate salts, etc., cationic catalysts such as triallylsulfonium hexafluoroantimonate and diaryliodonium hexafluoroantimonate, and organic phosphine compounds such as tributylphosphine, methyldiphenylphosphine, triphenylphosphine, tris(4-methylphenyl)phosphine, tris(4-butylphenyl)phosphine, diphenylphosphine, and phenylphosphine. These compounds may be used alone or in combination of two or more.

[0048] Examples of metal catalysts include metal complex catalysts, inorganic metal catalysts, and organic metal catalysts. Examples of metal complex catalysts include acetylacetonate salts of metals selected from the group consisting of Fe (iron), Mn (manganese), Cu (copper), Zr (zirconium), Th (thorium), Ti (titanium), Al (aluminum), and Co (cobalt), such as iron acetylacetonate, manganese acetylacetonate, copper acetylacetonate, and zirconia acetylacetonate. From the viewpoints of toxicity and catalytic activity, iron acetylacetonate (Fe(acac)3) or manganese acetylacetonate (Mn(acac)2) is preferred. These may be used alone or in combination of two or more.

[0049] Examples of inorganic metal catalysts include those selected from Sn, Fe, Mn, Cu, Zr, Th, Ti, Al, Co, etc. These may be used alone or in combination of two or more.

[0050] Examples of organometallic catalysts include organic zinc compounds such as zinc octylate, zinc neodecanoate, and zinc naphthenate, organic tin compounds such as stannous diacetate, stannous dioctoate, stannous dioleate, stannous dilaurate, dibutyltin diacetate, dibutyltin dilaurate, dioctyltin dilaurate, dibutyltin oxide, and dibutyltin dichloride, organic nickel compounds such as nickel octylate and nickel naphthenate, organic cobalt compounds such as cobalt octylate and cobalt naphthenate, organic bismuth compounds such as bismuth octylate, bismuth neodecanoate, and bismuth naphthenate, and titanium compounds such as tetraisopropyloxytitanate, dibutyltitanium dichloride, tetrabutyltitanium, and butoxytitanium trichloride. These may be used alone or in combination of two or more.

[0051] Examples of amine catalysts include triethylenediamine, 2-methyltriethylenediamine, quinuclidine, 2-methylquinuclidine, N,N,N',N'-tetramethylethylenediamine, N,N,N',N'-tetramethylpropylenediamine, 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-N'-(2-hydroxyethyl)propanediamine, bis(dimethylaminopropyl)amine, bis(dimethylaminopropyl)isopropanolamine, Propanolamine, 3-quinuclidinol, N,N,N',N'-tetramethylguanidine, 1,3,5-tris(N,N-dimethylaminopropyl)hexahydro-S-triazine, 1,8-diazabicyclo[5.4.0]undecene-7, N-methyl-N'-(2-dimethylaminoethyl)piperazine, N,N'-dimethylpiperazine, dimethylcyclohexylamine, N-methylmorpholine, N-ethylmorpholine, 1-methylimidazole, 1 ,2-dimethylimidazole, 1-isobutyl-2-methylimidazole, 1-dimethylaminopropylimidazole, N,N-dimethylhexanolamine, N-methyl-N'-(2-hydroxyethyl)piperazine, 1-(2-hydroxyethyl)imidazole, 1-(2-hydroxypropyl)imidazole, 1-(2-hydroxyethyl)-2-methylimidazole, 1-(2-hydroxypropyl)-2-methylimidazole, etc. These may be used alone or in combination of two or more.

[0052] Examples of aliphatic cyclic amide compounds include δ-valerolactam, ε-caprolactam, ω-enantholactam, η-capryllactam, and β-propiolactam. Among these, ε-caprolactam is more effective in promoting curing. These compounds may be used alone or in combination of two or more.

[0053] Titanium chelate complexes are compounds whose catalytic activity is enhanced by ultraviolet irradiation, and titanium chelate complexes having an aliphatic or aromatic diketone as a ligand are preferred because of their excellent curing-accelerating effect. Furthermore, in the present invention, those having an alcohol having 2 to 10 carbon atoms as a ligand in addition to an aromatic or aliphatic diketone are preferred because the effects of the present invention are more pronounced. These may be used alone or in combination of two or more.

[0054] 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 such a metal. Polymerization catalysts comprising such metals or metal compounds include metals such as Ti, Sn, Zn, Al, Zr, Mg, Hf, and Ge, and compounds of these metals, more specifically titanium tetraisopropoxide, titanium tetrabutoxide, titanium oxyacetylacetonate, tin octoate, 2-ethylhexanetin, zinc acetylacetonate, zirconium tetrachloride, zirconium tetrachloride tetrahydrofuran complex, hafnium tetrachloride, hafnium tetrachloride tetrahydrofuran complex, germanium oxide, and tetraethoxygermanium. These may be used alone or in combination of two or more.

[0055] (Other additives) In addition to the above-mentioned components, the dispersant for a blend resin of the present invention may contain a leveling agent, inorganic fine particles such as colloidal silica or alumina sol, polymethyl methacrylate-based organic fine particles, an antifoaming agent, an anti-sagging agent, a wetting and dispersing agent, a viscosity adjuster, an ultraviolet absorber, a metal deactivator, a peroxide decomposer, a flame retardant, a reinforcing agent, a plasticizer, a lubricant, a rust inhibitor, a fluorescent brightening agent, an inorganic heat ray absorber, a flame retardant, an antistatic agent, a dehydrating agent, and the like.

[0056] (How to use dispersants for blended resins) The dispersant for blend resins of the present invention can be used in a manner that includes a step of directly adhering it to at least one of two or more mutually incompatible thermoplastic resins. Specifically, when the target thermoplastic resin is in the form of a sheet or film, the step of directly adhering it to at least one thermoplastic resin can be achieved by directly applying (coating) the dispersant for blend resins of the present invention onto the sheet or film, or by laminating a molten resin containing the dispersant for blend resins of the present invention by melt extrusion lamination or sand lamination. Furthermore, for example, when the target thermoplastic resin is in the form of pellets or other granules, the pellets and the dispersant for blend resins of the present invention can be mixed by stirring or otherwise treating the pellets with the dispersant for blend resins of the present invention to coat the pellet surfaces with the dispersant for blend resins, thereby enabling direct adhesion.

[0057] To facilitate the coating, the dispersant for blended resins of the present invention can be blended with an organic solvent to achieve appropriate coatability. Such organic solvents are not particularly limited as long as they can be removed by evaporation by heating in the drying step during coating. Examples of such organic solvents include aromatic organic solvents such as toluene and xylene; aliphatic organic solvents such as n-hexane and n-heptane; alicyclic organic solvents such as cyclohexane and methylcyclohexane; halogenated organic solvents such as trichloroethylene, 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; ethanol, methanol, n-propanol, 2-propanol (isopropyl alcohol), and the like. ether solvents such as diisopropyl ether, butyl cellosolve, tetrahydrofuran, dioxane, butyl carbitol; glycol ether solvents such as diethylene glycol monomethyl ether, triethylene glycol monomethyl ether, propylene glycol monomethyl ether; glycol ester solvents such as ethylene glycol monomethyl ether acetate, propylene glycol monomethyl ether acetate, diethylene glycol monoethyl ether acetate, and the like. These may be used alone or in combination of two or more.

[0058] Even when an olefin resin having an acid group or an acid anhydride group or an olefin resin having vinyl acetate is used as the olefin resin (A), it is preferable to use a mixed solvent of an alicyclic organic solvent and an ester solvent because of its excellent solubility. In particular, when an olefin resin having an acid group, an acid anhydride group, and / or vinyl acetate is used, it is preferable to use a mixed solvent of methylcyclohexane, ethyl acetate, and 2-propanol because of its excellent solubility.

[0059] The amount of the organic solvent used is preferably such that the proportion of the olefin resin (A) relative to the total mass of the olefin resin (A) and the organic solvent is 5 to 20 mass %.

[0060] The dispersant for blend resins of the present invention can be prepared by mixing the above-mentioned components. In this case, the components may be mixed simultaneously to form an adhesive, or the components other than the metal compound may be mixed in advance to prepare a premixture, and the metal compound may be mixed when the dispersant for blend resins is to be used.

[0061] (Blend resin of two or more thermoplastic resins that are incompatible with each other) By using the dispersant for a blend resin of the present invention, a compatible blend resin can be obtained even when two or more thermoplastic resins that are incompatible with each other are used. In the present invention, "incompatible" does not only mean complete incompatibility, but also includes a state in which compatibility is difficult. Examples of combinations of two or more mutually incompatible thermoplastic resins include a combination of polyester resin and an olefin resin, a combination of nylon resin and an olefin resin, a combination of PVA (polyvinyl alcohol)-coated olefin resin (e.g., A-OP) and an olefin resin, a combination of an ethylene-vinyl alcohol copolymer resin and an olefin resin, a combination of nylon resin, polyester resin and an olefin resin, and a combination of nylon resin, ethylene-vinyl alcohol copolymer resin and an olefin resin. There are no particular limitations on the shape of these thermoplastic resins, and if the purpose is packaging materials, thermoplastic resins in the shape of sheets or films (hereinafter in this invention, sheets and films may be collectively referred to as "films") can be used. Much of the collected waste plastic that has become a problem in recent years is packaging material for food, household goods, etc., and in these cases, the thermoplastic resin is almost always in the form of film.

[0062] In some cases, a coating agent is applied to the thermoplastic resin film to impart functionality. Examples of combinations of films and coating agents that are incompatible with each other include a combination of a PVDC (polyvinylidene chloride)-coated olefin resin (e.g., KOP) and an olefin resin, a PVDC (polyvinylidene chloride)-coated polyester resin (e.g., KET) and an olefin resin, a PVDC (polyvinylidene chloride)-coated nylon resin (e.g., KON) and an olefin resin, and a PVDC (polyvinylidene chloride)-coated cellophane resin and an olefin resin.

[0063] (olefin resin) Specific examples of olefin-based resins include polyethylenes such as low-density polyethylene, medium-density polyethylene, high-density polyethylene, and linear low-density polyethylene, polypropylene, ethylene-propylene copolymers, α-olefin polymers, ethylene-vinyl acetate copolymers, ethylene-vinyl alcohol copolymers, ethylene-acrylic acid copolymers, ethylene-methyl methacrylate copolymers, ethylene-ethyl acrylate copolymers, cyclic olefin-based resins, ionomer resins, and polymethylpentene; and modified olefin-based resins obtained by modifying olefin-based resins with acrylic acid, methacrylic acid, maleic anhydride, fumaric acid, or other unsaturated carboxylic acids.

[0064] The polyethylene may also be made from biomass-derived ethylene glycol. Biomass-derived ethylene glycol is made from ethanol (biomass ethanol) produced from biomass as a raw material. For example, biomass-derived ethylene glycol can be obtained by converting biomass ethanol into ethylene oxide by a conventionally known method to produce ethylene glycol. Commercially available biomass ethylene glycol may also be used, and for example, biomass ethylene glycol commercially available from India Glycoal Limited can be suitably used.

[0065] Alternatively, products made from biomass materials are also available, classified by their biomass plastic content as specified by ISO 16620 or ASTM D6866. Radioactive carbon-14C exists in the atmosphere at a rate of 1 in 1012 particles, and this rate remains the same for atmospheric carbon dioxide, so this rate remains the same even in plants that fix this carbon dioxide through photosynthesis. Therefore, the carbon in plant-derived resins contains radioactive carbon-14C. In contrast, the carbon in fossil fuel-derived resins contains almost no radioactive carbon-14C. Therefore, by measuring the concentration of radioactive carbon-14C in the resin using an accelerator mass spectrometer, the plant-derived resin content, or biomass plastic content, can be determined. Examples of plant-derived low-density polyethylene that is a biomass plastic having a biomass plastic content of 80% or more, preferably 90% or more as specified by ISO 16620 or ASTM D6866, include products manufactured by Braskem under the trade names "SBC818," "SPB608," "SBF0323HC," "STN7006," "SEB853," and "SPB681."

[0066] Many of the above olefinic resins function as heat seal layers when the desired application is packaging materials.

[0067] (polyester resin) The polyester resin is a polyester resin produced by polycondensation of a polycarboxylic acid and a polyhydric alcohol. Examples of polycarboxylic acids include aromatic polycarboxylic acids such as phthalic acid, phthalic anhydride, terephthalic acid, isophthalic acid, orthophthalic acid, naphthalenedicarboxylic acid, and trimellitic acid; aliphatic polycarboxylic acids such as succinic acid, adipic acid, azelaic acid, sebacic acid, decanoic acid, undecanedioic acid, dodecanedioic acid, tridecanedioic acid, tetradecanedioic acid, heptadecanedioic acid, hexadecanedioic acid, heptadecanedioic acid, octadecanedioic acid, dimer acid, and cyclohexanedicarboxylic acid; and other polycarboxylic acids such as malonic acid, glutaric acid, pimelic acid, suberic acid, hexahydrophthalic acid, 1,4-cyclohexanedicarboxylic acid, malonic acid, glutaric acid, pimelic acid, suberic acid, hexahydrophthalic acid, 1,4-cyclohexanedicarboxylic acid, malonic acid, glutaric acid, pimelic acid, hexahydrophthalic acid, 1,4-cyclohexanedicarboxylic acid, malonic acid, glutaric ... Examples of the carboxylic acid include leic acid, maleic anhydride, citraconic acid, dimethylmaleic acid, cyclopentene-1,2-dicarboxylic acid, 1-cyclohexene-1,2-dicarboxylic acid, 4-cyclohexene-1,2-dicarboxylic acid, fumaric acid, mesaconic acid, itaconic acid, glutaconic acid, phthalic acid, phthalic anhydride, terephthalic acid, isophthalic acid, orthophthalic acid, 1,2,5-hexanetricarboxylic acid, 1,2,4-cyclohexanetricarboxylic acid, trimellitic acid, trimellitic anhydride, 1,2,5-benzenetricarboxylic acid, 2,5,7-naphthalenetricarboxylic acid, pyromellitic acid, and pyromellitic anhydride. These may be used alone or in combination of two or more. Furthermore, if necessary, monocarboxylic acids such as methanoic acid, ethanoic acid, propanoic acid, butanoic acid, pentanoic acid, hexanoic acid, heptanoic acid, octanoic acid, nonanoic acid, decanoic acid, dodecanoic acid, tetradecanoic acid, hexadecanoic acid, heptadecanoic acid, and octadecanoic acid may be used as raw material components.

[0068] Examples of polyhydric alcohols include ethylene glycol, diethylene glycol, propylene glycol, 2-methyl-1,3-propanediol, 2,2-dimethyltrimethylene glycol, 1,4-butanediol, 1,5-pentanediol, 3-methylpentanediol, 1,6-hexanediol, 1,7-heptanediol, 1,8-octanediol, 1,9-nonanediol, 1,10-decanediol, 1,12-dodecanediol, 1,16-hexadecanediol, 1,18-octadecanediol, 1,20-icosanediol, 1,4-cyclohexanedimethanol, polyethylene glycol, polypropylene glycol, polytetramethylene glycol, neopentyl glycol, pentaethylene glycol, and trimethylolpropane.

[0069] The polycarboxylic acid and the polyhydric alcohol may be used in any combination. Specific examples include terephthalic acid / ethylene glycol copolymer (polyethylene terephthalate, also known as PET resin), terephthalic acid / 1,4-butanediol copolymer, terephthalic acid / 1,4-butanediol / adipic acid copolymer, terephthalic acid / polytetramethylene ether glycol / 1,4-butanediol copolymer, terephthalic acid / isophthalic acid / 1,4-butanediol / polytetramethylene ether glycol copolymer, terephthalic acid / isophthalic acid / 1,4-butanediol copolymer, terephthalic acid / ethylene glycol / neopentyl glycol copolymer, terephthalic acid / ethylene glycol / 1,4-cyclohexanedimethanol / isosorbide copolymer, terephthalic acid / isophthalic acid / ethylene glycol copolymer, terephthalic acid / ethylene glycol / 1,4-cyclohexanedimethanol copolymer, and terephthalic acid / 1,4-cyclohexanedimethanol / 2,2,4,4-tetramethyl-1,3-cyclobutanediol copolymer.

[0070] Many of the polyester resins described above function as surface layers or intermediate materials when the desired application is packaging materials.

[0071] (nylon resin) Examples of nylon resins (polyamide resins) that can be used include aliphatic polyamide resins (nylon resins) such as nylon 6, nylon 66, nylon 46, nylon 11, nylon 12, nylon 610, nylon 612, nylon 6 / 66 copolymer, nylon 6 / 66 / 610 copolymer, nylon MXD6, nylon 6T, and nylon 6 / 6T copolymer.

[0072] Many of the nylon resins described above function as surface layers or intermediate materials when the desired application is packaging materials.

[0073] (ethylene-vinyl alcohol copolymer resin) Ethylene-vinyl alcohol copolymer (EVOH) can be obtained, for example, by copolymerizing ethylene with a vinyl ester monomer and then saponifying the copolymer. The copolymerization of ethylene with a vinyl ester monomer can be carried out by any known polymerization method, such as solution polymerization, suspension polymerization, or emulsion polymerization.

[0074] Many of the ethylene-vinyl alcohol copolymers function as surface layers or intermediate materials when the desired application is packaging materials.

[0075] (cellophane resin) Cellophane resin is made from pulp and is a biomass material, so it can be used where biomass is desired.

[0076] (Filmization of thermoplastic resin) The thermoplastic resin can be produced by a conventionally known film-forming method, such as extrusion, cast molding, T-die molding, cutting, or inflation. The film may be an unstretched film, or may be stretched uniaxially or biaxially using a tenter system, tubular system, or the like, from the viewpoint of the strength, dimensional stability, and heat resistance of the resulting film. The film may also be subjected to some kind of surface treatment, such as a physical treatment such as corona discharge treatment, ozone treatment, low-temperature plasma treatment using oxygen gas or nitrogen gas, glow discharge treatment, or flame treatment, or a chemical treatment such as oxidation treatment using chemicals, or other treatment.

[0077] Furthermore, when forming a thermoplastic resin into a film, additives may be added as necessary. Specifically, plastic compounding agents and additives such as elastomers, lubricants, crosslinking agents, antioxidants, UV absorbers, light stabilizers, fillers, reinforcing agents, antistatic agents, and pigments may be added for the purpose of improving or modifying processability, heat resistance, weather resistance, mechanical properties, dimensional stability, antioxidant properties, slipperiness, mold releasability, flame retardancy, mildew resistance, electrical properties, strength, etc. The amount of additive added is adjusted within a range that does not affect other properties or recyclability.

[0078] The thickness of the thermoplastic resin film is not particularly limited and is appropriately selected depending on the desired application. For example, in the case of a packaging material, the thickness is appropriately selected in the range of 0.1 to 300 μm from the viewpoints of formability and transparency.

[0079] As described above, when the target thermoplastic resin is a film, the blend resin dispersant of the present invention maximizes its effects by directly applying (coating) the blend resin dispersant of the present invention to the film and directly adhering to it. Adhesion here refers to adhesion to a portion of the target thermoplastic resin. For example, if the target thermoplastic resin film has a printed layer and the blend resin dispersant of the present invention is laminated on top of the printed layer, the blend resin dispersant of the present invention will adhere to the target thermoplastic resin film through the gaps in the ink or halftone dots that form the printed layer.

[0080] The blend resin dispersant of the present invention has good adhesion to various thermoplastic resins and can therefore be used as an adhesive for bonding films of different types of resins that are incompatible with each other. When using the blend resin dispersant of the present invention as an adhesive, the blend resin dispersant of the present invention can be directly applied (coated) to a target thermoplastic resin film, and then another thermoplastic film of a different type can be laminated and adhered to the target thermoplastic resin film. In this case, a laminate can be obtained in which films of different types of thermoplastic resins are bonded together with the blend resin dispersant of the present invention.

[0081] The blend resin dispersant of the present invention is characterized by including a step of directly adhering it to at least one thermoplastic resin, as described above, but it does not have to be in direct contact with another thermoplastic resin. That is, it may be a laminate obtained by directly applying (coating) the blend resin dispersant of the present invention to the target thermoplastic resin film, and then laminating and adhering a laminate film containing another thermoplastic film of a different type.

[0082] (Laminate) As described above, the laminate of the present invention is a laminate in which the blend resin dispersant of the present invention is directly applied (coated) onto a target thermoplastic resin film, and then a laminate film containing another thermoplastic film of a different type is laminated and adhered to the target thermoplastic resin film. The blend resin dispersant of the present invention only needs to be directly adhered to at least one thermoplastic resin, and does not need to be in direct contact with the other thermoplastic resin. In other words, the laminate may be a laminate in which the blend resin dispersant of the present invention is directly applied (coated) onto the target thermoplastic resin film, and then a laminate film containing another thermoplastic film of a different type is laminated and adhered to the target thermoplastic resin film.

[0083] When the thermoplastic resin film to which the dispersant for blend resin of the present invention is directly adhered is designated as the second film and another thermoplastic resin film is designated as the first film, the laminate of the present invention is characterized by comprising the first film, the second film, and a resin layer A disposed between the first film and the second film, the resin layer A being the dispersant for blend resin provided so as to be in contact with the second film. In particular, it is preferable that the first film contains an olefin-based resin as a main component and the second film contains a thermoplastic resin that is incompatible with the olefin-based resin as a main component.

[0084] An example of a specific embodiment of the laminate of the present invention is shown below, but the present invention is not limited to this, and it is sufficient for the laminate to be one in which the dispersant for blended resins of the present invention is directly adhered to at least one thermoplastic resin of two or more mutually incompatible thermoplastic resins. Furthermore, as described above, even when a printed layer is present between the target thermoplastic resin layer and the blend resin dispersant layer, the blend resin dispersant directly adheres to the thermoplastic resin layer through the gaps between the dots that make up the printed layer, so the effects of the present invention can be achieved. The first film and the second film are films whose main components are two or more thermoplastic resins that are incompatible with each other.

[0085] Second film / dispersant layer for blended resin / first film Second film / blend resin dispersion layer / curable adhesive layer / first film Second film / printing layer / blend resin dispersant layer / first film Second film / blend resin dispersant layer / printed layer / blend resin dispersant layer / first film Second film / printing layer / blend resin dispersion layer / curable adhesive layer / first film Second film / dispersant layer for blended resin / printing layer / curable adhesive layer / first film Second film / blend resin dispersant layer / printing layer / blend resin dispersant layer / curable adhesive layer / first film Second film / dispersant layer for blended resin / functional layer / first film Second film / printing layer / dispersant layer for blended resin / functional layer / first film Second film / blend resin dispersant layer / printing layer / blend resin dispersant layer / functional layer / first film Second film / printing layer / dispersing agent layer for blended resin / curable adhesive layer / functional layer / first film Second film / Blend resin dispersant layer / Printing layer / Blend resin dispersant layer / Curable adhesive layer / Functional layer / First film Second film / curable adhesive layer / blend resin dispersant layer / first film Second film / printing layer / curable adhesive layer / blend resin dispersant layer / first film Second film / blend resin dispersant layer / printing layer / curable adhesive layer / blend resin dispersant layer / first film Second film / blend resin dispersion layer / film having vapor-deposited layer / blend resin dispersion layer / first film Second film / blend resin dispersion layer / curable adhesive layer / film having vapor deposition layer / blend resin dispersion layer / curable adhesive layer / first film Second film / printed layer / blend resin dispersant layer / film having vapor deposition layer / blend resin dispersant layer / first film Second film / printed layer / blend resin dispersant layer / curable adhesive layer / film having vapor deposition layer / blend resin dispersant layer / curable adhesive layer / first film Second film / blend resin dispersant layer / film having metal layer / blend resin dispersant layer / first film Second film / blend resin dispersant layer / curable adhesive layer / film having a metal layer / blend resin dispersant layer / curable adhesive layer / first film Second film / printed layer / blend resin dispersant layer / film having metal layer / blend resin dispersant layer / first film Second film / printed layer / blend resin dispersant layer / curable adhesive layer / film having metal layer / blend resin dispersant layer / curable adhesive layer / first film

[0086] Films having a vapor-deposited layer include, for example, films on which a metal or an inorganic compound is vapor-deposited. The vapor-deposited layer may be obtained by vapor-depositing a metal such as aluminum, or a metal compound such as aluminum oxide (AlOx), silicon oxide (SiOx), silicon oxide (SiOx), zinc oxide, magnesium oxide, calcium oxide, manganese oxide, iron oxide, cobalt oxide, nickel oxide, or copper oxide. These metals or inorganic compounds may be used alone or in combination of two or more.

[0087] The film having a metal layer is a film having a metal foil, such as aluminum foil.

[0088] (Printing layer) The printing layer is a layer on which letters, figures, symbols, and other desired designs are printed. There are no particular limitations on the printing method or printing ink, and any known printing method or printing ink can be used. Printing inks using methods such as gravure printing, flexographic printing, lithographic offset printing, and inkjet recording printing are often used for the films used as the substrate. Printing inks that combine these printing methods with methods of curing using active energy rays such as ultraviolet (UV), LED, and electron beam (EB), or methods of curing using heat, are also used. Depending on the solvent used, inks may be referred to as water-based inks or organic solvent-based inks.

[0089] Specific examples include gravure printing ink and flexographic printing ink (in some industries, gravure printing ink and flexographic printing ink are sometimes referred to as liquid printing ink), ultraviolet-curable ink for lithographic offset printing, electron-beam-curable ink for lithographic offset printing, ultraviolet-curable ink for inkjet recording and printing, and electron-beam-curable ink for inkjet recording and printing.

[0090] (Manufacturing method for recycled plastics) The recycled plastic of the present invention can be obtained by a known processing method for recycling waste plastics using the laminate of the present invention. An example of the processing method is shown below. Of course, the present invention is not limited to this, and various known recycled plastic processing methods can be applied.

[0091] An example of the processing method is a method for producing recycled plastics, which includes the steps of crushing the laminate of the present invention, melting and kneading the crushed pieces, and pelletizing the melted and kneaded mixture. The crusher used in the step of crushing the laminate of the present invention is not particularly limited, and any known crusher may be used. The crushed film pieces are physically blended using methods such as melt mixing, solvent cast blending, latex blending, and polymer complexing. Melt mixing is particularly common. Examples of mixing devices include tumblers, Henschel mixers, rotary mixers, super mixers, ribbon tumblers, and V-blenders. The film pieces are melt-mixed using these mixers and then pelletized. Single- or multi-screw extruders are typically used for melt mixing and pelletization. The film pieces may be fed directly into the extruder or may be compressed with or without heating before being added. In addition to these extruders, Banbury mixers, roller mixers, Ko-kneaders, blast mills, and Prabender Bloutographs can also be used, operated batchwise or continuously. Alternatively, the film pieces may be used as molding resins without melt mixing and then melt-kneaded in the heating barrel of a molding machine.

[0092] The pellets of the present invention, which are made primarily from recycled plastic, can be recycled into non-oriented polyolefin films or molded products made by injection molding or the like, thereby maximizing their effectiveness. The method for recycling the unstretched polyolefin film is not particularly limited and can be achieved by known film production methods. For example, melt-kneading methods using common mixers such as single-screw extruders, twin-screw extruders, and multi-screw extruders, or methods in which the components are dissolved or dispersed and mixed and then the solvent is removed by heating, can be used. Considering workability, the use of a single-screw extruder or twin-screw extruder is particularly preferred. When using a single-screw extruder, full-flight screws, screws with mixing elements, barrier-flight screws, fluted screws, and the like can be used without particular limitations. Twin-screw kneading devices include co-rotating twin-screw extruders and counter-rotating twin-screw extruders, and the screw shapes are not particularly limited, including full-flight screws and kneading disk types. Alternatively, a method in which the material is melted in a single-screw extruder or twin-screw extruder, etc., and then passed through a feed block or multi-manifold and then subjected to film formation using a T-die can also be used. Furthermore, if necessary, the recycled film can be subjected to a surface modification treatment to appropriately improve its suitability for subsequent processes. For example, to improve printability when used as a standalone film or lamination suitability when used in a laminated structure, a surface modification treatment can be performed on the surface that comes into contact with other substrates. Suitable surface modification treatments include corona discharge treatment, plasma treatment, flame treatment, and other methods that oxidize the film surface to develop functional groups, as well as wet process methods such as coating with an easy-adhesion layer.

[0093] In addition, in the same manner as with pellets made primarily from virgin plastics, the plastic may be molded into a molded article by a conventional molding method other than the above-mentioned film formation, such as injection molding, extrusion molding, vacuum molding, pressure molding, blow molding, or the like, and used for various purposes. For example, it can be used as daily necessities, stationery, toys, sporting goods, home appliances, and automobile parts used in ordinary households, as well as films, sheets, and fibers. If there are no hygiene issues, it can also be used in medical devices, food containers, and food packaging materials. [Example]

[0094] The present invention will be described in more detail below with reference to specific examples, but the present invention is not limited to these examples. In the following examples, "parts" and "%" represent "parts by mass" and "% by mass", respectively, unless otherwise specified.

[0095] (Preparation of dispersant for blended resin) (Dispersant for blended resins 1) Auroren S-5601S (registered trademark) (olefin resin having an acid group and an acid anhydride group, manufactured by Nippon Paper Industries Co., Ltd.) was used as dispersant 1 for blended resins. Dispersant 1 for blended resins was adjusted to a nonvolatile content of 12 mass % with a mixed solution of methylcyclohexane, ethyl acetate, and isopropanol.

[0096] (Dispersant for blended resins 2) Auroren S-5631S (registered trademark) (olefin resin having an acid group and an acid anhydride group, manufactured by Nippon Paper Industries Co., Ltd.) was used as dispersant 2 for blended resins. Dispersant 2 for blended resins was adjusted to a nonvolatile content of 12 mass % with a mixed solution of methylcyclohexane, ethyl acetate, and isopropanol.

[0097] (Dispersant for blended resins 3) Ultrathene (registered trademark) 13B53D (olefin resin modified with vinyl acetate groups, manufactured by Tosoh Corporation) was used as dispersant 3 for blended resins. Dispersant 3 for blended resins was prepared using a mixed solution of methylcyclohexane, ethyl acetate, and isopropanol to have a nonvolatile content of 12% by mass.

[0098] (Dispersant for blended resins 4) Evaflex (registered trademark) EV-45X (olefin resin modified with vinyl acetate groups, manufactured by Dow Mitsui Polychemicals Co., Ltd.) was used as a dispersant 4 for the blend resin. Dispersant 4 for blended resins was adjusted to a nonvolatile content of 12 mass % with a mixed solution of methylcyclohexane, ethyl acetate, and isopropanol.

[0099] (Dispersant for blended resins 5) 85% by mass of Auroren S-5601S (registered trademark) (olefin resin having acid groups and acid anhydride groups, manufactured by Nippon Paper Industries Co., Ltd.) and 15% by mass of Ultrathene (registered trademark) 13B53D (olefin resin modified with vinyl acetate groups, manufactured by Tosoh Corporation) were used as dispersant 5 for the blended resin. Dispersant 5 for blended resins was adjusted to a nonvolatile content of 12% by mass with a mixed solution of methylcyclohexane, ethyl acetate, and isopropanol.

[0100] (General-purpose adhesive U) A general-purpose adhesive U was prepared by blending polyurethane polyol and polyisocyanate in a ratio of 10% by mass to 1% by mass and diluting the mixture with ethyl acetate to a solid content of 30% by mass.

[0101] Example 1 The second substrate film was a biaxially stretched polyethylene terephthalate (PET) film (Toyobo Ester (registered trademark) Film E5102, 12 μm, manufactured by Toyobo Co., Ltd.) coated with a blend resin dispersant 1 prepared with a solvent to a solid content weight of approximately 1.8 g / m 2 After the solvent was evaporated, a non-oriented linear low-density polyethylene (L-LDPE) film (TUX manufactured by RM Tohcello Co., Ltd.) was applied as the first substrate film using a tabletop calendar roll. TM HC, 60 μm) to prepare a laminate A-1.

[0102] Example 2 A laminate A-2 was produced in the same manner as in Example 1, except that dispersant 2 for blend resins was used as the dispersant for blend resins.

[0103] Example 3 A laminate A-3 was produced in the same manner as in Example 1, except that dispersant 3 for blend resins was used as the dispersant for blend resins.

[0104] Example 4 A laminate A-4 was produced in the same manner as in Example 1, except that blend resin dispersant 4 was used as the blend resin dispersant.

[0105] Example 5 A laminate A-5 was produced in the same manner as in Example 1, except that blend resin dispersant 5 was used as the blend resin dispersant.

[0106] Example 6 The second substrate film was a biaxially oriented nylon (OPA) film (manufactured by Unitika Ltd., Emblem (registered trademark) ON, 15 μm) to which the blend resin dispersant 1 was added so that the solid content weight was approximately 1.8 g / m 2 After the solvent was evaporated, a non-oriented linear low-density polyethylene (L-LDPE) film (TUX manufactured by RM Tohcello Co., Ltd.) was applied as the first substrate film using a tabletop calendar roll. TM HC, 60 μm) to prepare a laminate B-1.

[0107] Example 7 A laminate B-2 was produced in the same manner as in Example 6, except that blend resin dispersant 2 was used as the blend resin dispersant.

[0108] Example 8 A biaxially stretched polyethylene terephthalate (PET) film (manufactured by Toyobo Co., Ltd., Toyobo Ester (registered trademark) Film E5102, 12 μm) was used as a second substrate film, and a dispersant 3 for blended resin was added to the film to a solid content weight of about 1.8 g / m 2 The solution was applied using a bar coater so that the thickness became equal to that of the coated film, and the solvent was evaporated. After that, a desktop calendar roll was used to bond the coated film to a non-oriented polypropylene (CPP) film (manufactured by Toyobo Co., Ltd., Pylen (registered trademark) Film-CT P1128, 60 μm) as a first base film to produce laminate C-1.

[0109] Example 9 A laminate C-2 was produced in the same manner as in Example 8, except that blend resin dispersant 4 was used as the blend resin dispersant.

[0110] Example 10 A biaxially stretched polyethylene terephthalate (PET) film (manufactured by Toyobo Co., Ltd., Toyobo Ester (registered trademark) Film E5102, 12 μm) was used as a second substrate film, and dispersant 1 for blended resin was added to the film to a solid content weight of about 1.0 g / m 2 After the solvent was evaporated, general-purpose adhesive U was applied on top of it so that the solid content was approximately 1.5 g / m. 2 After the solvent was evaporated, a non-oriented linear low-density polyethylene (L-LDPE) film (TUX manufactured by RM Tohcello Co., Ltd.) was applied as the first substrate film using a tabletop calendar roll. TM HC, 60 μm) and subjected to predetermined aging to prepare a laminate D-1.

[0111] Example 11 A laminate D-2 was produced in the same manner as in Example 10, except that blend resin dispersant 2 was used as the blend resin dispersant.

[0112] Example 12 The first base film was a non-oriented linear low-density polyethylene (L-LDPE) film (TUX, manufactured by RM Tocello Co., Ltd.). TM HC, 60 μm) and blend resin dispersant 2 at a solids weight of approximately 1.0 g / m 2 After the solvent was evaporated, general-purpose adhesive U was applied on top of it so that the solid content was approximately 1.5 g / m. 2 The solution was applied using a bar coater so that the thickness became equal to the thickness of the laminate, and the solvent was evaporated. After that, a biaxially oriented polyethylene terephthalate (PET) film (manufactured by Toyobo Co., Ltd., Toyobo Ester (registered trademark) film E5102, 12 μm) was laminated as a second substrate film using a desktop calendar roll, and the laminate was subjected to a predetermined aging process to produce laminate D-3.

[0113] Example 13 A laminate D-4 was produced in the same manner as in Example 12, except that blend resin dispersant 4 was used as the blend resin dispersant.

[0114] Example 14 A biaxially oriented nylon (OPA) film (manufactured by Unitika Ltd., Emblem (registered trademark) ON, 15 μm) was used as a second substrate film, and dispersant 1 for blended resin was added to the film so that the solid content weight was approximately 1.0 g / m 2 After the solvent was evaporated, general-purpose adhesive U was applied on top of it so that the solid content was approximately 1.5 g / m. 2 After the solvent was evaporated, a non-oriented linear low-density polyethylene (L-LDPE) film (TUX manufactured by RM Tohcello Co., Ltd.) was applied as the first substrate film using a tabletop calendar roll. TM HC, 60 μm) to prepare a laminate D-5.

[0115] Example 15 The first base film was a non-oriented linear low-density polyethylene (L-LDPE) film (TUX, manufactured by RM Tocello Co., Ltd.). TM HC, 60 μm) and blend resin dispersant 1 at a solids weight of approximately 1.0 g / m 2 After the solvent was evaporated, general-purpose adhesive U was applied on top of it so that the solid content was approximately 1.5 g / m. 2 The solution was applied using a bar coater so that the thickness became equal to that of the coated film, and the solvent was evaporated. After that, a biaxially oriented nylon (OPA) film (manufactured by Unitika Ltd., Emblem (registered trademark) ON, 15 μm) was laminated to the coated film as a second substrate film using a desktop calendar roll to prepare a laminate D-6.

[0116] (Comparative Example 1) Biaxially oriented polyethylene terephthalate (PET) film (Toyobo Ester (registered trademark) Film E5102, 12 μm, manufactured by Toyobo Co., Ltd.) and unoriented linear low-density polyethylene (L-LDPE) film (RM Tocello Co., Ltd., TUXTM HC, 60 μm) were alternately stacked to prepare a mixed plastic sample G-1. Comparative Example 1 was prepared by adding 2% by mass of dispersant 1 for blended resins to 98% by mass of laminate G-1 when preparing recycled pellets.

[0117] (Comparative Example 2) Biaxially oriented nylon (OPA) film (Emblem® ON, 15 μm, manufactured by Unitika Ltd.) and unstretched linear low-density polyethylene (L-LDPE) film (TUX, manufactured by RM Tocello Co., Ltd.) TM HC, 60 μm) were alternately stacked to prepare a mixed plastic sample G-2.

[0118] (Comparative Example 3) Comparative Example 9 (G-3) was prepared by adding 2% by mass of dispersant 1 for blended resins to 98% by mass of the laminate G-2 when preparing recycled pellets.

[0119] Comparative Example 4 Plastic sample G-4 was prepared by alternately stacking and mixing biaxially oriented polyethylene terephthalate (PET) film (Toyobo Ester (registered trademark) Film E5102, 12 μm, manufactured by Toyobo Co., Ltd.) and unstretched polypropylene (CPP) film (Toyobo Pylen (registered trademark) Film-CT P1128, 60 μm, manufactured by Toyobo Co., Ltd.).

[0120] (Comparative Example 5) Comparative Example 11 (G-5) was prepared by adding 2% by mass of dispersant 3 for blended resins to 98% by mass of the laminate G-4 when preparing recycled pellets.

[0121] (Comparative Example 6) Comparative Example 6 (G-6) was prepared by adding 2% by mass of dispersant 4 for blended resins to 98% by mass of the laminate G-4 when preparing recycled pellets.

[0122] (Comparative Example 7) The second substrate film was a biaxially stretched polyethylene terephthalate (PET) film (Toyobo Ester (registered trademark) Film E5102, 12 μm, manufactured by Toyobo Co., Ltd.) coated with a general-purpose adhesive U at a solid content weight of approximately 3.0 g / m 2 After the solvent was evaporated, a non-oriented linear low-density polyethylene (L-LDPE) film (TUX manufactured by RM Tohcello Co., Ltd.) was applied as the first substrate film using a tabletop calendar roll. TM This was subjected to predetermined aging to prepare a laminate E-1. This was designated Comparative Example 7.

[0123] (Comparative Example 8) Comparative Example 8 (E-2) was prepared by adding 2% by mass of dispersant 1 for blended resins to 98% by mass of the laminate E-1 when preparing recycled pellets.

[0124] (Comparative Example 9) Comparative Example 9 (E-3) was prepared by adding 2% by mass of dispersant 4 for blended resins to 98% by mass of the laminate E-1 when preparing recycled pellets.

[0125] (Comparative Example 10) The second substrate film was a biaxially oriented nylon (OPA) film (manufactured by Unitika Ltd., Emblem (registered trademark) ON, 15 μm) coated with a general-purpose adhesive U at a solid content weight of approximately 3.0 g / m 2 After the solvent was evaporated, a non-oriented linear low-density polyethylene (L-LDPE) film (TUX manufactured by RM Tohcello Co., Ltd.) was applied as the first substrate film using a tabletop calendar roll. TM HC, 60 μm) to prepare a laminate F-1. This was designated Comparative Example 10.

[0126] (Comparative Example 11) Comparative Example 8 (F-2) was prepared by adding 2% by mass of dispersant 1 for blended resins to 98% by mass of the laminate F-1 when preparing recycled pellets.

[0127] (Comparative Example 12) Comparative Example 8 (F-3) was prepared by adding 2% by mass of dispersant 2 for blended resins to 98% by mass of the laminate F-1 when preparing recycled pellets.

[0128] (Evaluation results) The laminated films obtained in Examples 1 to 15 and Comparative Examples 1 to 12 were evaluated as follows.

[0129] (Recyclability evaluation) (Production of recycled pellets) The laminated films obtained in the examples and the comparative examples were used. Each film was cut into strips 10 mm wide and 300 mm long, which were melt-mixed at 240°C, 100 rpm, and 3 minutes using a twin-screw kneading extrusion machine (ULTnano15TW, manufactured by Technovel Co., Ltd.), extruded from the nozzle, immediately cooled with tap water, and resin strands were obtained. These strands were then cut into pellet samples. In Comparative Examples 2, 3, 5, 6, 7, 9, 11, and 12, the specified strips were placed in the kneading machine, and then a specified blend resin dispersant was added to obtain recycled pellet samples.

[0130] (Tensile elongation of recycled pellet molded product) A 9g sample of recycled pellets was placed in a stainless steel press frame mold (inner dimensions 100mm square, 1mm thick), sandwiched between two stainless steel plates (2mm thick), and compression molded at 210°C, 30MPa, and 3 minutes to produce a 1mm thick plastic plate. A 1 / 3 size test piece conforming to JIS K6251-5 was punched out of the plate using a Super Dumbbell Cutter SDK500 1 / 3 manufactured by Dumbbell Co., Ltd. A tensile test was conducted on the punched test piece at 50mm / min with a chuck distance of 30mm to measure the tensile elongation. This tensile elongation was taken as the tensile elongation of the recycled plastic.

[0131] The results are shown in Tables 1 to 6.

[0132] [Table 1]

[0133] [Table 2]

[0134] [Table 3]

[0135] [Table 4]

[0136] [Table 5]

[0137] [Table 6]

[0138] In Tables 1 to 6, the abbreviations are as follows: PET: biaxially oriented polyethylene terephthalate OPA: Biaxially oriented nylon LLDPE: Unstretched linear low-density polyethylene CPP: Non-oriented polypropylene

[0139] Example 16 The laminate A-1 and the laminate E-1 were alternately stacked to prepare a mixed plastic sample.

[0140] Example 17 The laminate A-2 and the laminate E-1 were alternately stacked to prepare a mixed plastic sample.

[0141] Example 18 The laminate A-3 and the laminate E-1 were alternately stacked to prepare a mixed plastic sample.

[0142] Example 19 The laminate B-1 and the laminate F-1 were alternately stacked to prepare a mixed plastic sample.

[0143] Example 20 The laminate A-3 and the laminate B-1 were alternately stacked to prepare a mixed plastic sample.

[0144] Example 21 The laminate A-3, laminate B-1, laminate E-1, and laminate F-1 were alternately stacked to prepare a mixed plastic sample.

[0145] (Evaluation results) The laminated films obtained in Examples 16 to 21 were subjected to the above-mentioned evaluations. The results are shown in Table 7.

[0146] [Table 7]

Claims

1. A dispersant for blended resins to be used for blended resins of two or more mutually incompatible thermoplastic resins, the dispersant for blended resins being characterized by comprising an olefin-based resin modified with an acid, an acid anhydride, and / or vinyl acetate.

2. 2. The dispersant for blended resins according to claim 1, wherein the two or more mutually incompatible thermoplastic resins are a polyester resin and an olefin resin, or a nylon resin and an olefin resin.

3. 3. A method for using the dispersant for blended resins according to claim 1 or 2, comprising a step of directly adhering the dispersant to at least one of two or more mutually incompatible thermoplastic resins.

4. a first base film, a second base film, and a resin layer A disposed between the first base film and the second base film; the first substrate film is composed mainly of an olefin-based resin, the second substrate film is mainly composed of a thermoplastic resin that is incompatible with an olefin-based resin, 3. A laminate, comprising the dispersant for blended resins according to claim 1 or 2, wherein the resin layer A is provided so as to be in contact with the second substrate film.

5. A recycled plastic made from the laminate according to claim 4.

6. A method for producing recycled plastic using the laminate described in claim 4 as a raw material, comprising the steps of crushing the laminate described in claim 4, melting and kneading the crushed pieces, and pelletizing the melted and kneaded mixture.

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