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WO2005014716A1 - Article moule monocouche ou multicouche contenant une composition de resine copolymere polyethylene/alcool vinylique (evoh), contenant, et procede de production d'un article moule par recuperation/reutilisation - Google Patents

Article moule monocouche ou multicouche contenant une composition de resine copolymere polyethylene/alcool vinylique (evoh), contenant, et procede de production d'un article moule par recuperation/reutilisation Download PDF

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Publication number
WO2005014716A1
WO2005014716A1 PCT/JP2004/011655 JP2004011655W WO2005014716A1 WO 2005014716 A1 WO2005014716 A1 WO 2005014716A1 JP 2004011655 W JP2004011655 W JP 2004011655W WO 2005014716 A1 WO2005014716 A1 WO 2005014716A1
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WIPO (PCT)
Prior art keywords
resin
layer
vitamin
multilayer
molded article
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
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PCT/JP2004/011655
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English (en)
Japanese (ja)
Inventor
Kenichi Fujiwara
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Idemitsu Unitech Co Ltd
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Idemitsu Unitech Co Ltd
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Publication date
Application filed by Idemitsu Unitech Co Ltd filed Critical Idemitsu Unitech Co Ltd
Priority to JP2005513024A priority Critical patent/JP4916172B2/ja
Publication of WO2005014716A1 publication Critical patent/WO2005014716A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J11/00—Recovery or working-up of waste materials
    • C08J11/04—Recovery or working-up of waste materials of polymers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B17/00—Recovery of plastics or other constituents of waste material containing plastics
    • B29B17/0026—Recovery of plastics or other constituents of waste material containing plastics by agglomeration or compacting
    • B29B17/0042—Recovery of plastics or other constituents of waste material containing plastics by agglomeration or compacting for shaping parts, e.g. multilayered parts with at least one layer containing regenerated plastic
    • 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
    • B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B27/08—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00—Use of organic ingredients
    • C08K5/0008—Organic ingredients according to more than one of the "one dot" groups of C08K5/01 - C08K5/59
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29K—INDEXING SCHEME ASSOCIATED WITH SUBCLASSES B29B, B29C OR B29D, RELATING TO MOULDING MATERIALS OR TO MATERIALS FOR MOULDS, REINFORCEMENTS, FILLERS OR PREFORMED PARTS, e.g. INSERTS
    • B29K2029/00—Use of polyvinylalcohols, polyvinylethers, polyvinylaldehydes, polyvinylketones or polyvinylketals or derivatives thereof as moulding material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29K—INDEXING SCHEME ASSOCIATED WITH SUBCLASSES B29B, B29C OR B29D, RELATING TO MOULDING MATERIALS OR TO MATERIALS FOR MOULDS, REINFORCEMENTS, FILLERS OR PREFORMED PARTS, e.g. INSERTS
    • B29K2105/00—Condition, form or state of moulded material or of the material to be shaped
    • B29K2105/0005—Condition, form or state of moulded material or of the material to be shaped containing compounding ingredients
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2323/00—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers
    • C08J2323/02—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers not modified by chemical after treatment
    • C08J2323/04—Homopolymers or copolymers of ethene
    • C08J2323/08—Copolymers of ethene
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/141—Feedstock
    • Y02P20/143—Feedstock the feedstock being recycled material, e.g. plastics
    • 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 molded article, a container, and a method for producing a molded article by recovery and reuse using a stabilization technique for suppressing a thermal degradation reaction of an ethylene-vinyl alcohol copolymer (hereinafter, referred to as EVOH) resin. It is.
  • EVOH ethylene-vinyl alcohol copolymer
  • EVOH resins have the characteristic of extremely low permeability to gases such as oxygen, and are therefore used in various applications in addition to food packaging materials.
  • molded products of EVOH resin are used as a single-layer film and a film obtained by laminating the film with an adhesive, or as at least one layer of an extrusion-molded product such as a multilayer blown or multilayer film or a multilayer injection-molded product. It is used in forms such as films.
  • the process of obtaining these molded articles of EVOH resin, like other thermoplastic resins, is generally carried out using a screw-type extruder or the like in a heat-plasticized state.
  • the EVOH resin must be heated at least twice before the resin pellet manufacturing stage and the bottle / film molding process. As a result, thermal degradation and thermal degradation reactions such as thermal decomposition and oxidation of EVOH resin occur to a non-negligible degree.
  • EVOH resin finally produces decomposed products such as acetoaldehyde, crotonaldehyde, pentanal, and acetone, which are contained in the molded product in a small amount. .
  • a composition comprising an EVOH resin and an alkali metal acetate (see, for example,
  • JP-A-293848 and a composition of an EVOH resin and acetic acid and a metal acetate (for example, JP-A-11-106592).
  • Antioxidants such as compounds having a hindered phenol group and compounds having a hindered amine group, carboxylic acids such as acetic acid, lactic acid and oxalic acid, phosphoric acid, phosphorous acid and phosphoric acid 2
  • carboxylic acids such as acetic acid, lactic acid and oxalic acid
  • phosphoric acid phosphorous acid and phosphoric acid 2
  • a composition to which a boron compound such as a phosphate compound such as sodium hydrogen, boric acids, borate esters, borates, and borohydrides is added (for example, see JP-A-2001-
  • JP-A-201-3547779 there is a case where a thermal degradation reaction may occur when EVOH resin is melt-pelleted at an extrusion temperature of 200 ° C. or higher, which is usually used. He pointed out that this is the case, and proposed a method for producing an EVOH resin composition that can be melt-kneaded at a low temperature.
  • thermoplastic resin such as polyolefin generates an odor due to an oxidative deterioration reaction.
  • an antioxidant is added to reduce the polyolefin. Stabilization has been attempted.
  • vitamin E As an antioxidant for polyolefin and the like, vitamin E and the like are also known (for example, Japanese Patent Application Laid-Open No. 2002-53166 and Japanese Patent Application Laid-Open No. 2003-181595).
  • a food consisting of an EVOH resin layer and a polyolefin resin layer Laminating packaging materials ⁇ Even if an antioxidant such as vitamin E was added only to the polyolefin resin layer of the container, sufficient odor control for retort foods could not be achieved.
  • the thermal degradation reaction of polyolefins includes oxidation reactions such as abstraction of hydrogen atoms from hydrocarbon-based polymer chains by oxygen, generation and decomposition of peroxides, cleavage of carbon-carbon bonds, isomerization reactions, and the like. It proceeds by a chain reaction called autoxidation with a crosslinking reaction.
  • phosphorus compounds which are effective for stabilizing peroxides, and compounds with hindered phenol groups, which are effective as radical scavengers, are used as antioxidants to suppress this degradation reaction. It is added to polyolefin in a complex manner and used as a polyolefin resin composition.
  • antioxidants may decompose due to degradation reactions such as thermal decomposition and hydrolysis of the antioxidants themselves, causing problems such as generation of offensive odor and yellowing (for example, Kenji Kimura, "New Stabilization Technology for Resin Processing", Polymer Digest, February 2002, p. 97).
  • the common object of the present invention is to increase the thermal stability of the EVOH resin in the heat-melted state, in particular, to the thermal stability during the molding process involving shearing due to the heat-melting and screw rotation, and as a result, the off-odor has been reduced.
  • the present inventor has paid attention to the fact that there is no effective antioxidant as described above, despite the fact that the thermal degradation reaction mechanism of EVOH resin is basically an oxidation reaction, and diligently studied to find out the reason. Was performed.
  • the thermal degradation reaction mechanism of EVOH resin is based on a series of degradation reactions that start with the oxidation of EVOH resin, resulting in the decomposition of EVOH resin chains and the isomerization reaction, resulting in the formation of aldehydes. Suggests to generate. Therefore, the following items can be inferred.
  • Hindered phenol group among antioxidants considered to be ineffective A compound having an amide bond and having an amide bond (see Japanese Patent Application Laid-Open No. 2001-354579) can provide relatively good results only because the compound forms a hydrogen bond with EVOH resin and reacts. It is considered that the probability of collision between the sites has been increased, and the result must support the above 1.
  • Antioxidants contained in trace amounts in living organisms and plants can be expected to have an order of magnitude higher reaction rate than ordinary antioxidants that are artificially synthesized and commercially available (Burton et al. J. Am. Chem. Soc., 107
  • the present inventor has made earnest efforts to reduce the generation of aldehydes that also cause odor during molding of EVOH resin and the molded article itself, and contained them in living organisms and plants.
  • the present inventors have found that antioxidant substances are extremely effective, and have completed the present invention.
  • EVOH resin an ethylene-butyl alcohol copolymer resin
  • antioxidant substances selected from vitamin E, vitamin C, flavonoid and carotenoid.
  • thermoplastic resin molded article in which a multilayer thermoplastic resin article containing at least one EVOH resin-containing layer is recovered and reused in at least one layer of a single-layer or multilayer thermoplastic resin article, A method for producing a multilayer thermoplastic resin molded article in which the reused layer of the recovered molded article contains an antioxidant selected from vitamin E, vitamin C, flavonoid and carotenoid;
  • a food or beverage container or medical container obtained by thermoforming the single-layer or multi-layer resin molded product described in 1 above.
  • a single-layer or multi-layer resin molded article having at least one layer of the composition according to 2 or 10 above,
  • the antioxidant used in the present invention is selected from one or more of vitamin E, vitamin C, flavonoid and carotenoid.
  • Vitamin E in the present invention means tocopherol, tocotrienol and derivatives thereof.
  • Tocopherol and tocotrienol have ⁇ -, ⁇ -, 7- and ⁇ -forms, respectively, and naturally contain at least eight types of vitamin ⁇ .
  • Vitamin ⁇ has different biological properties (efficacy), and it is said that one tocopherol has the strongest biological activity.
  • vitamin ⁇ refers to a-tocopherol, but in the present invention, Contains vitamin E.
  • Natural vitamin E is mainly extracted from oil residues such as soybeans, rapeseed and cottonseed, but may be derivatives with acetic acid and the like.
  • artificially synthesized vitamin E may be used.
  • Vitamin C in the present invention means ascorbic acid.
  • Braponoid in the present invention does not mean a single substance, but is a generic term for a group of compounds such as polifenols, anthocyanidins, quercetin, catechins, and disoflavones.
  • the carotenoid in the present invention is basically a tetraterpenoid composed of eight isoprenoid units, and is a general term for a group of compounds of carotenes and xanthophylls.
  • the antioxidant used in the present invention is preferably vitamin E, and among vitamin E, ⁇ -tocopherol is more preferred.
  • the addition amount of the antioxidant is preferably from 0:! To 500 x 100 to 6 parts by mass, more preferably from 10 to 100 parts by mass of the total of the thermoplastic resin and the EVOH resin. : a looo xl 0- 6 parts by weight. When it is 0. 1 x 1 0- 6 parts by mass or more, to suppress the thermal degradation reactions, it can be effectively reduced the formation of substances causing offensive odors, such as aldehyde compounds.
  • the EVOH resin used in the present invention is generally produced through a saponification reaction of an ethylene-vinyl acetate copolymer (hereinafter referred to as EVA) resin.
  • EVA ethylene-vinyl acetate copolymer
  • Ethylene unit content of the EVOH resin in the present invention is not particularly limited, preferably 3-9 7 mole 0/0, more preferably 20 to 50 mole 0/0.
  • the saponification degree of the EVOH resin in the present invention is not particularly limited, preferably 70: A L 00 mole 0/0.
  • one kind of the EVOH resin may be used, or two or more kinds having different ethylene unit content and / or saponification degree may be used in combination.
  • the method of adding an antioxidant to EVOH is not particularly limited, and examples thereof include the following methods.
  • the method of adding and kneading the antioxidant substance is not particularly limited.
  • a continuous system using a quantity feeder can be employed.
  • the antioxidant substance in a liquid state may be directly added to the EVOH resin and kneaded.
  • the EVOH resin composition can be obtained as described above, and the resin composition may optionally contain various additives such as other thermoplastics, as long as the object of the present invention is not impaired. Resins, other antioxidants, ultraviolet absorbers, light stabilizers, antistatic agents, plasticizers, crosslinking agents, fillers, coloring agents, and the like can be appropriately compounded.
  • thermoplastic resins include, for example, various polyolefins (polyethylene, polypropylene, poly (l-butene), poly (4-methylenol-1-ene), ethylene-propylene copolymer, ethylene and ⁇ -carbon having 4 or more carbon atoms.
  • antioxidants conventionally known hindered phenol-based antioxidants, phosphorus-based antioxidants, sulfur-based antioxidants and the like can be used.
  • UV absorbers include conventionally known benzotriazoles, benzophenones, and salicylic acids
  • light stabilizers include conventionally known hindered An amine compound is used. .
  • the single-layer or multi-layer molded product in the present invention is, for example, a single-layer or multilayer film, sheet, container, or the like.
  • a multilayer molded product can be produced by various molding methods such as an injection molding method, a professional method, an injection / blowing method, a T-die method, and a tumbler method. These single- or multi-layer molded products are further processed to produce secondary processed products.
  • the molded article is formed into a laminated film with other materials such as a polyethylene terephthalate resin and a nylon resin using an adhesive, or is subjected to a thermoforming process, so that a beverage packaging material and a beverage container, a food packaging material, And it can be used as food containers, medical packaging materials and medical containers.
  • the single-layer or multi-layer molded product of the present invention can be optimally used as a container or packaging material for retort foods accompanied by reheating. It is most suitable as a container that contains side dishes, pilaf, fried rice, etc.
  • other resins used for layers other than the layer composed of the resin composition of the present invention include linear low-density polyethylene, low-density polyethylene, medium-density polyethylene, and high-density polyethylene.
  • olefin such as ethylene-butyl acetate copolymer, ethylene-propylene copolymer, polypropylene, propylene monoolefin copolymer ( ⁇ -olefin having 4 to 20 carbon atoms), polybutene, polypentene, etc.
  • polyesters such as polyethylene terephthalate, polyester elastomers, polyamide-6, nylon-6, nylon-6,6, etc., polyamide resins, polystyrene, polychlorinated vinyl, polyvinylidene chloride, acrylic resins, vinylesters Resin, polyurethane elastomer, polycarbonate, salt Examples include polished polyethylene and chlorinated polypropylene.
  • polyesters such as polyethylene terephthalate, polyester elastomers, polyamide-6, nylon-6, nylon-6,6, etc., polyamide resins, polystyrene, polychlorinated vinyl, polyvinylidene chloride, acrylic resins, vinylesters Resin, polyurethane elastomer, polycarbonate, salt Examples include polished polyethylene and chlorinated polypropylene.
  • thermoplastic resin composition of the present invention will be described in detail below.
  • EVOH resin and antioxidant may be the same as (A)-(1) and (2) above.
  • thermoplastic resin is not particularly limited as long as it forms a composition with the EVOH resin.
  • EVOH resin As described in the above (A) to (5), “In a single-layer or multilayer molded article, Other resins used in layers other than the layer composed of the resin composition in the present invention '' can be appropriately selected.
  • polypropylene is used as a food container or medical container heated by retort or sterilization. It is also preferable because it can be used and is inexpensive.
  • thermoplastic resin composition of the present invention may be mainly used for at least one layer of a multilayer molded product or a secondary processed product thereof, such as a multilayer sheet, a thermoformed product thereof, and a multilayer blow molded product. Many.
  • Non-product parts such as shank parts generated during the production of molded products, non-standard products with dimensional accuracy, or container parts that are products after thermoforming ⁇ Losses generated during the production of secondary processed products such as skeletons generated by punching And then granulated into a suitable shape as a raw material resin for melt molding by pulverization (hereinafter referred to as “pulverized products, etc.”), and then to vitamin E, vitamin C, flavonoids and carotenoids.
  • pulverized products, etc.” When recovered and reused after returning to the base layer or intermediate layer of a multilayer resin molded product such as a multilayer sheet containing at least one or more antioxidants selected from The generation of objects and odors can be suppressed.
  • thermoplastic resin other than the EVOH resin contained in the recovery layer also has a longer residence time in the molten state for recovery and reuse, resulting in thermal degradation such as oxidation reactions.
  • thermal degradation reaction of the thermoplastic resin itself is suppressed, and the influence of the interaction with the degradation reaction of the EVOH resin in the oxidation degradation reaction is also considered to be reduced.
  • the base layer is a main layer that generally occupies the largest layer ratio in a multilayer molded product, and is a layer that retains strength and heat resistance.
  • the intermediate layer is a layer inside the multilayer molded product. This means that it can be intentionally provided as a collection layer for the purpose of collection and reuse.
  • base layer thermoplastic resin such as polypropylene
  • adhesive layer / layer containing EVOH / adhesive layer base layer
  • intermediate layer Adhesive resin layer Layer containing ZEVOH resin Z Adhesive resin layer Z Base layer ”.
  • each essential component is as follows: 99.9 to 60% by mass of thermoplastic resin, 0.1% to 40% by mass of EVOH resin, preferably thermoplastic resin. 99.8 to 80% by mass, and £ 011 resin is 0.2 to 20% by mass.
  • the EVOH resin content is less than 0.1% by mass, the recovery / reuse ratio is too low, and there is no point in collecting and reusing. If it exceeds 40% by mass, the strength and heat resistance of the thermoplastic resin composition are reduced. In some cases, making it difficult to use, especially for containers to be heated.
  • Antioxidant is, when the sum of thermoplastic resin and EVOH ⁇ 1 0 0 parts by weight, if included 0. 1 X 1 0_ 6 parts by mass or more, express the present effect , But preferably,
  • the total amount of the thermoplastic resin and the EVOH resin is more than 5000 ⁇ 10 16 parts by mass, the decomposition of the antioxidant itself may proceed, which is economically inferior.
  • Vitamin E is preferred as the antioxidant.
  • thermoplastic resin composition is the same as (A) to (5) above.
  • EVOH resin and antioxidant may be the same as (A)-(1) and (2) above.
  • a multi-layered thermoplastic resin molded article containing at least one EVOH resin-containing layer of the present invention is collected into at least one layer of a single-layered or multi-layered thermoplastic resin molded article.
  • the layer in which the collected molded article is reused contains an antioxidant selected from vitamin E, vitamin C, flavonoids and carotenoids, gels and burns will occur when collected and reused. ⁇ Generation of aggregates and odor can be suppressed.
  • the antioxidant substance will be added to the sum of the thermoplastic resin and EVOH resin in the above-mentioned ground product.
  • the addition should be melt-kneaded with the addition so that 0. 1 ⁇ 5 0 0 0 X 1 0- 6 parts by weight, the addition during melt kneading, when recovery and reuse, gel burnt-aggregates and odor Can be suppressed.
  • Vitamin E is preferred as the antioxidant.
  • the ground product is not particularly limited as long as it can be used as a raw material system for the extrusion process.
  • the pulverized product or the like is not particularly limited as long as it is a molded product containing an EVOH resin, but is usually a multilayer molded product itself having at least one layer of the EVOH resin or a composition containing the resin, or the multilayer molded product itself. Crushed products and the like generated during the production of the product can be used.
  • the generation of agglomerates can be suppressed even if the product is formed again.
  • the parzine resin used for the base material layer includes linear low-density polyethylene, low-density polyethylene, medium-density polyethylene, high-density polyethylene, ethylene-vinyl acetate copolymer, ethylene-propylene copolymer, and polypropylene.
  • Propylene- ⁇ -olefin copolymers ( ⁇ -olefins having 4 to 20 carbon atoms), homo- or copolymers of olefins such as polybutene and polypentene, polyesters such as polyethylene terephthalate, polyester elastomers, and nylon-6 And polyamide resins such as nylon 1.6 and 6, polystyrene, polyvinyl chloride, polyvinylidene chloride, acrylic resin, vinyl ester resin, polyurethane elastomer, polycarbonate, chlorinated polyethylene and chlorinated polypropylene. No.
  • Preferred virgin resins include polypropylene, polystyrene and the like.
  • the adhesive resin layer with the EVOH resin layer is made of maleic anhydride-modified polypropylene in the case of polypropylene, and styrene-hydrogenated butadiene-styrene copolymer, styrene-water in the case of polystyrene.
  • An added isoprene-styrene copolymer or the like is used.
  • these adhesive resins are also contained in the recovery layer. Further, it may contain a coloring agent such as titanium oxide or an additive generally used for molding.
  • a compatibilizing agent for a commonly used resin and EVOH resin can be added to the recovery layer.
  • E VOH resin containing ethylene units 3 2 mol% [Nippon Synthetic Chemical E Industry Co., Soanoru BS 3 203, saponification degree 10 10 mol 0/0 or more], vitamin E [Ciba ' IRGANOX E 201, manufactured by Specialty Chemical Co., Ltd .; 2,5,7,8-tetramethyl-12 (4,, 8,1,12'-trimethyltridecyl) chroman-1-6-ol 1% by mass of low-density polyethylene (MFR 9 gZlO content, 190 ° C) -based masterbatch containing 1% by mass of [IRGANOX MB202] (made of Ciba Specialty Chemicals) After performing dry blending, a single-screw extruder (Braco
  • vitamin E masterbatch 0 kg vitamin E masterbatch was added 2 parts by weight of (1) dry blending , 3.5 m A full-flight type die-equipped extruder with three ⁇ openings 4 ⁇ ⁇ Melt extrusion at 230 ° C using a rod extruder, a rod-shaped molded product made of a composition such as polypropylene, EVOH resin, and vitamin E Got.
  • the titanium oxide master batch low-density polyethylene [Higashisoichi Co., Petrocene 20 5] 3 1 wt%, titanium oxide [manufactured by Ishihara Sangyo Kaisha Ltd. R- 6 8 0] 6 0 mass 0/0, high Dorotarusai preparative [Kyowa chemical Co., Ltd., consisting of DHT-4 A] 7. 5 weight 0/0 and calcium stearate 1.5 mass 0/0.
  • This rod-shaped molded product was pulverized and melt-kneaded at a resin temperature of 230 ° C. with a single screw extruder to obtain a rod-shaped molded product having two passes of the extruder.
  • Table 1 shows the measurement results.
  • the area value is the area of each component on the ion chromatogram.
  • the olfactory threshold in Table 1 is the minimum amount of a substance that causes olfactory sensation.
  • a composition consisting of polypropylene, titanium oxide, modified polypropylene, and E VOH resin (hereinafter abbreviated as PP ZE VOH composition) that has passed through the extruder five times in (2) above is equipped with a flat die.
  • a full-foil 40 ⁇ extruder was used to produce a 3 Om film at a molding temperature of 230 ° C.
  • A4 size sample was cut out from this film, and the number of aggregates was visually observed. As a result, eight aggregates were confirmed.
  • Example 11 After processing this extruded sheet in the same manner as in Example 11- (3), the components in the produced gas were measured using GC-MS. The results are shown in Table 1. (2) Example 11 (1) The EVOH resin used in (1) was combined with the above-mentioned (1) hindered phenolic antioxidant (Chipa 'Specialty' Chemicals,
  • Example 1 I RGANOX TM 1 0 9 8) 100 00 x 10 0-The same operation as in Example 1 (2) was performed except that a resin composition consisting of 6 parts by mass was used. 0 3 mg.
  • Example 1-1 (4) The same operation as in Example 1-1 (4) was carried out except that the PP / EVOH composition obtained in the above (2) and passed through the extruder five times was used, and the aggregates were counted. There were nine.
  • Example 11 In the same manner as in (1), only an E VOH resin containing 32 mol% of ethylene units [manufactured by Nippon Synthetic Chemical Industry Co., Ltd., Soanol BS 3203, saponification degree of at least 99 mol%] An extruded sheet consisting of
  • Example 1-1 (2) The same operation as in Example 1-1 (2) was performed except that no antioxidant was used, and the amount was determined to be 140 mg by eye.
  • Example 11- (4) The same operation as in Example 11- (4) was performed, except that the PP / E VOH composition obtained in (2) and passed through the extruder five times was used, and the aggregates were counted. There were 17 pieces.
  • Example 2 a model set consisting of polypropylene, EVOH resin, vitamin E, etc. From the results of the recovery and reuse tests, the extruder was passed five times through the extruder, and in Example 1, the amount of waste that was considered to be mainly due to the thermal degradation and decomposition of the EVOH resin was determined in Example 1. It was found that the amount can be suppressed as compared with Comparative Example 1 using the antioxidant. Table 2
  • an EVOH resin containing a specific antioxidant or a composition containing the resin is molded at 200 ° C. or higher, or a multilayer molded article having at least one layer containing an EVOH resin Even when recovered and reused, the thermal degradation reaction of EVOH resin is significantly suppressed.
  • aldehydes such as acetoaldehyde, crotonaldehyde and pentanal, which are decomposition products of EVOH resin, is extremely suppressed, so that products that have almost no odor even when used in multilayer molded products and containers. Goods can be obtained.

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  • Laminated Bodies (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Containers Having Bodies Formed In One Piece (AREA)
  • Manufacture Of Macromolecular Shaped Articles (AREA)

Abstract

L'invention concerne un article monocouche ou multicouche comprenant une composition de résine copolymère polyéthylène/alcool vinylique (résine EVOH), une composition contenant ladite résine, et un procédé de production d'un article moulé. Selon ledit procédé, un article moulé présentant une couche contenant une résine EVOH est récupéré et réutilisé pour la réalisation d'un moulage de résine thermoplastique, ladite couche de l'article moulé récupéré à réutiliser contenant un antioxydant.
PCT/JP2004/011655 2003-08-07 2004-08-06 Article moule monocouche ou multicouche contenant une composition de resine copolymere polyethylene/alcool vinylique (evoh), contenant, et procede de production d'un article moule par recuperation/reutilisation Ceased WO2005014716A1 (fr)

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JP2005513024A JP4916172B2 (ja) 2003-08-07 2004-08-06 エチレン−ビニルアルコール共重合体樹脂組成物からなる単層又は多層成形品、容器及び回収・再使用による成形品の製造方法

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JP2003-288961 2003-08-07
JP2003288961 2003-08-07

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WO2005014716A1 true WO2005014716A1 (fr) 2005-02-17

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PCT/JP2004/011655 Ceased WO2005014716A1 (fr) 2003-08-07 2004-08-06 Article moule monocouche ou multicouche contenant une composition de resine copolymere polyethylene/alcool vinylique (evoh), contenant, et procede de production d'un article moule par recuperation/reutilisation

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JP2008222817A (ja) * 2007-03-12 2008-09-25 Furukawa Electric Co Ltd:The 樹脂組成物およびそれを用いた成形物品
WO2013005807A1 (fr) * 2011-07-07 2013-01-10 株式会社クラレ Composition de résine de copolymère éthylène-alcool vinylique et son procédé de fabrication
WO2013146962A1 (fr) * 2012-03-28 2013-10-03 株式会社クラレ Conteneur moulé par soufflage, conteneur de carburant et procédé de fabrication d'un conteneur moulé par soufflage
JP2015054878A (ja) * 2013-09-10 2015-03-23 株式会社クラレ エチレン−ビニルアルコール共重合体含有樹脂組成物、フィルム、積層体、包装材料及びフィルムの製造方法
WO2015041258A1 (fr) * 2013-09-20 2015-03-26 株式会社クラレ Récipient moulé thermiquement et son procédé de fabrication
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WO2015050223A1 (fr) * 2013-10-02 2015-04-09 株式会社クラレ Composition de résine, feuille multicouches, matériau d'emballage et récipient
WO2015050222A1 (fr) * 2013-10-02 2015-04-09 株式会社クラレ Composition de résine, corps moulé en résine, et structure multicouche
WO2015050221A1 (fr) * 2013-10-02 2015-04-09 株式会社クラレ Récipient moulé par soufflage, récipient pour combustible, récipient pour bouteilles moulé par soufflage, et procédé de production de récipient moulé par soufflage
WO2015050211A1 (fr) * 2013-10-03 2015-04-09 株式会社クラレ Composition de résine, structure multicouche, et récipient thermoformé la contenant
WO2015050224A1 (fr) * 2013-10-02 2015-04-09 株式会社クラレ Composition de résine d'éthylène-alcool vinylique, structure multicouche, feuille multicouche, récipient et matériau d'emballage
JP2015071711A (ja) * 2013-10-03 2015-04-16 株式会社クラレ 樹脂組成物、多層構造体及びそれからなる熱成形容器
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JP2015071710A (ja) * 2013-10-03 2015-04-16 株式会社クラレ 樹脂組成物、多層構造体及びそれからなる熱成形容器
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JP2015071691A (ja) * 2013-10-02 2015-04-16 株式会社クラレ 樹脂組成物、樹脂成形体及び多層構造体
JP2015071694A (ja) * 2013-10-02 2015-04-16 株式会社クラレ 樹脂組成物、多層シート、包装材及び容器
JP2015071693A (ja) * 2013-10-02 2015-04-16 株式会社クラレ 樹脂組成物、多層シート、包装材及び容器
JP2015071689A (ja) * 2013-10-02 2015-04-16 株式会社クラレ ブロー成形容器及びブロー成形容器の製造方法
JP2015083377A (ja) * 2013-09-20 2015-04-30 株式会社クラレ 熱成形容器及びその製造方法
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US9096751B2 (en) 2010-03-22 2015-08-04 Borealis Ag Heterophasic polypropylene with excellent creep performance
US9163131B2 (en) 2012-03-28 2015-10-20 Kuraray Co., Ltd. Resin composition containing ethylene-vinyl alcohol copolymer
US10047204B2 (en) 2013-05-29 2018-08-14 Kuraray Co., Ltd. Ethylene-vinyl alcohol copolymer-containing resin composition, film, laminate, packaging material, vacuum thermal insulator, film production method, and laminate production method
JP2018141170A (ja) * 2018-05-25 2018-09-13 株式会社クラレ 樹脂組成物、多層構造体、熱成形容器及びその製造方法
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WO2023228970A1 (fr) * 2022-05-27 2023-11-30 三菱ケミカル株式会社 Composition de résine, structure multicouche, article moulé et procédé de production de composition de résine

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US9096751B2 (en) 2010-03-22 2015-08-04 Borealis Ag Heterophasic polypropylene with excellent creep performance
WO2013005807A1 (fr) * 2011-07-07 2013-01-10 株式会社クラレ Composition de résine de copolymère éthylène-alcool vinylique et son procédé de fabrication
US9951199B2 (en) 2011-07-07 2018-04-24 Kuraray Co., Ltd. Ethylene-vinyl alcohol copolymer resin composition and method for producing same
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EP2730614A4 (fr) * 2011-07-07 2015-03-04 Kuraray Co Composition de résine de copolymère éthylène-alcool vinylique et son procédé de fabrication
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