WO2018168720A1 - 熱可塑性樹脂シート、積層シート及び成形体 - Google Patents
熱可塑性樹脂シート、積層シート及び成形体 Download PDFInfo
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- WO2018168720A1 WO2018168720A1 PCT/JP2018/009342 JP2018009342W WO2018168720A1 WO 2018168720 A1 WO2018168720 A1 WO 2018168720A1 JP 2018009342 W JP2018009342 W JP 2018009342W WO 2018168720 A1 WO2018168720 A1 WO 2018168720A1
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- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J2451/00—Characterised by the use of graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Derivatives of such polymers
- C08J2451/04—Characterised by the use of graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Derivatives of such polymers grafted on to rubbers
-
- 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
- C08J2477/00—Characterised by the use of polyamides obtained by reactions forming a carboxylic amide link in the main chain; Derivatives of such polymers
- C08J2477/02—Polyamides derived from omega-amino carboxylic acids or from lactams thereof
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
Definitions
- the present invention relates to a thermoplastic resin sheet, a laminated sheet, and a molded body. More specifically, the present invention relates to a thermoplastic resin sheet containing a polyolefin resin and a polyamide resin, and a laminated sheet and a molded body using the thermoplastic resin sheet.
- Patent Document 1 discloses that a modified elastomer can be used as a compatibilizing agent in a resin mixture containing a polyamide resin and a polyolefin resin.
- Patent Document 2 discloses that a plant-derived polyamide resin can be used in a resin mixture containing a polyamide resin and a polyolefin resin.
- Patent Document 3 discloses that a resin mixture containing a polyamide resin and a polyolefin resin can exhibit a phase structure having a continuous phase, a dispersed phase, and a finely dispersed phase.
- Patent Document 4 discloses that after a polyamide resin and a compatibilizer are melt-mixed, a resin mixture having excellent impact resistance can be obtained by further melt-mixing the obtained resin mixture and a polyolefin resin. Is disclosed. However, Patent Documents 1-4 do not discuss the use of these resin mixtures as sheets. Patent Document 5 discloses a thermoplastic resin film that includes a polyamide resin and a polyolefin resin and exhibits a sea-island phase structure. However, studies on films having excellent mechanical strength and further studies on followability during molding have not been made.
- the present invention has been made in view of the above circumstances, and uses a thermoplastic resin sheet excellent in mechanical strength, a laminated sheet using such a thermoplastic resin sheet, and such a thermoplastic resin sheet. It aims at providing a molded object.
- a thermoplastic resin sheet having excellent mechanical strength and excellent followability during molding, a laminated sheet using such a thermoplastic resin sheet, and a molded body using such a thermoplastic resin sheet are provided. The purpose is to do.
- thermoplastic resin sheet according to claim 1 comprising a polyolefin resin, a polyamide resin, and a compatibilizing agent
- the compatibilizing agent comprises a thermoplastic resin which is a modified elastomer having a reactive group for the polyamide resin.
- the thermoplastic resin sheet according to claim 2 is the thermoplastic resin sheet according to claim 1, A continuous phase (A) containing the polyolefin resin;
- the dispersed phase (B) is a continuous phase (B 1 ) containing the polyamide resin, And a finely dispersed phase (B 2 ) containing the modified elastomer dispersed in the continuous phase (B 1 ).
- the thermoplastic resin sheet according to claim 4 is the thermoplastic resin sheet according to any one of claims 1 to 3, wherein the polyamide resin and the melted kneaded product of the modified elastomer, and the polyolefin resin. The gist is that it is a melt-kneaded product.
- the thermoplastic resin sheet according to claim 5 is the thermoplastic resin sheet according to any one of claims 1 to 4, wherein the polyamide resin is sandwiched between adjacent amide bonds in the main chain.
- the gist is that the hydrocarbon group has a structure having 6 or more linear carbon atoms.
- the thermoplastic resin sheet according to claim 6 is the thermoplastic resin sheet according to any one of claims 1 to 5, wherein the modified elastomer includes ethylene or propylene and an ⁇ -olefin having 3 to 8 carbon atoms.
- the gist of the present invention is an olefinic thermoplastic elastomer having a copolymer as a skeleton or a styrene thermoplastic elastomer having a styrene skeleton.
- the thermoplastic resin sheet according to claim 7 is the thermoplastic resin sheet according to any one of claims 1 to 6, wherein the elongation at break at 140 ° C is S 140 (%), and the break at 120 ° C is performed. When the elongation is S 120 (%), the gist is that S 140 is 1.2 times or more of S 120 .
- the molded body according to claim 10 is the molded body according to claim 9, wherein the base includes reinforcing fibers and a binder that binds the reinforcing fibers to each other.
- the gist is that the binder is the polyolefin resin.
- thermoplastic resin sheet a sheet having excellent mechanical strength can be provided. Moreover, according to this thermoplastic resin sheet, it can join to a molded object surface with sufficient followability, and the mechanical strength which this thermoplastic resin sheet has to a molded object can be provided. According to this laminated sheet, it can be joined to the surface of the base layer with good followability, and the mechanical strength of the thermoplastic resin sheet is imparted to the laminated sheet. Further, the present laminated sheet can be used by being attached to the surface of a molding substrate. In that case, this laminated sheet can be joined to the surface of the obtained molded body with good followability, and the mechanical strength of the thermoplastic resin sheet can be imparted to the molded body.
- the thermoplastic resin sheet is bonded to the one surface with good followability, and the mechanical strength of the thermoplastic resin sheet is imparted to the molded body. For this reason, the mechanical strength which is further excellent as the whole molded object can be exhibited rather than the mechanical strength which only a base has.
- thermoplastic resin composition which comprises the thermoplastic resin sheet of this invention.
- phase structure (3) of the thermoplastic resin composition which comprises the thermoplastic resin sheet of this invention.
- lamination sheet of this invention It is explanatory drawing explaining the molded object of this invention.
- manufacturing method of the molded object of this invention It is a graph which shows the correlation with test temperature and breaking elongation.
- thermoplastic resin sheet (1) of the present invention comprises a polyolefin resin, a polyamide resin, and a compatibilizing agent, and the compatibilizing agent has a reactive group with respect to the polyamide resin. It consists of a thermoplastic resin which is an elastomer.
- polyolefin resin constituting the thermoplastic resin sheet
- an olefin homopolymer and / or an olefin copolymer can be used as the polyolefin resin constituting the thermoplastic resin sheet.
- the olefin is not particularly limited, and examples thereof include ethylene, propylene, and ⁇ -olefin having 4 to 8 carbon atoms.
- Examples of the ⁇ -olefin having 4 to 8 carbon atoms include 1-butene, 3-methyl-1-butene, 1-pentene, 3-methyl-1-pentene, 4-methyl-1-pentene, 1-hexene, 1-hexene, Examples include octene. These may use only 1 type and may use 2 or more types together.
- examples of the polyolefin resin include polyethylene resin, polypropylene resin, poly 1-butene, poly 1-hexene, poly 4-methyl-1-pentene, and the like. These polymers may be used alone or in combination of two or more. That is, the polyolefin resin may be a mixture of the above polymers.
- polyethylene resin examples include ethylene homopolymers and copolymers of ethylene and other olefins (other olefins do not contain ethylene).
- examples of the latter include ethylene / 1-butene copolymer, ethylene / 1-hexene copolymer, ethylene / 1-octene copolymer, ethylene / 4-methyl-1-pentene copolymer, etc. 50% or more of the total number of structural units is a unit derived from ethylene).
- polypropylene resin examples include propylene homopolymers and copolymers of propylene and other olefins (other olefins do not contain propylene). Examples of the latter include propylene / ethylene copolymers and propylene / 1-butene copolymers (provided that 50% or more of all structural units are units derived from propylene). Further, the copolymer of propylene and other olefins may be a random copolymer or a block copolymer. Among these, a block copolymer is preferable from the viewpoint of obtaining a thermoplastic resin sheet having a larger S 140 / S 120 value to be described later.
- a propylene / ethylene block copolymer in which the other olefin is ethylene is preferable.
- This propylene / ethylene block copolymer is also referred to as, for example, an impact copolymer, a polypropylene impact copolymer, a heterophasic polypropylene, a heterophasic block polypropylene, or the like.
- the weight average molecular weight (standard polystyrene conversion) by the gel permeation chromatography (GPC) of polyolefin resin is also not specifically limited, For example, it can be 10,000 or more and 500,000 or less, and is 100,000 or more and 450,000 or less. Preferably, 200,000 or more and 400,000 or less are more preferable.
- the polyolefin resin is a polyolefin that does not have an affinity for a polyamide resin, which will be described later, and does not have a reactive group that can react with the polyamide resin. In this respect, it differs from the olefinic component as the modified elastomer described later.
- the polyamide resin constituting the thermoplastic resin sheet is a polymer obtained by polymerizing a plurality of monomers via an amide bond (—NH—CO—).
- Monomers constituting the polyamide resin include amino acids such as 6-aminocaproic acid, 11-aminoundecanoic acid, 12-aminododecanoic acid, paraaminomethylbenzoic acid, and lactams such as ⁇ -caprolactam, undecane lactam, and ⁇ -lauryllactam. Etc. These may use only 1 type and may use 2 or more types together.
- the polyamide resin can also be obtained by copolymerization of a diamine and a dicarboxylic acid.
- the diamine as a monomer includes ethylenediamine, 1,3-diaminopropane, 1,4-diaminobutane, 1,6-diaminohexane, 1,7-diaminoheptane, 1,8-diaminooctane, , 9-diaminononane, 1,10-diaminodecane, 1,11-diaminoundecane, 1,12-diaminododecane, 1,13-diaminotridecane, 1,14-diaminotetradecane, 1,15-diaminopentadecane, 1, 16-diaminohexadecane, 1,17-diaminoheptadecane, 1,18-diaminooctadecane, 1,19-dia
- dicarboxylic acids as monomers include oxalic acid, malonic acid, succinic acid, glutaric acid, adipic acid, pimelic acid, suberic acid, azelaic acid, sebacic acid, undecanedioic acid, dodecanedioic acid, brassic acid, Aliphatic dicarboxylic acids such as tetradecanedioic acid, pentadecanedioic acid, octadecanedioic acid, alicyclic dicarboxylic acids such as cyclohexanedicarboxylic acid, aromatic dicarboxylic acids such as phthalic acid, terephthalic acid, isophthalic acid, naphthalenedicarboxylic acid Etc. These may use only 1 type and may use 2 or more types together.
- polyamide resin polyamide 6, polyamide 66, polyamide 11, polyamide 610, polyamide 612, polyamide 614, polyamide 12, polyamide 6T, polyamide 6I, polyamide 9T, polyamide M5T, polyamide 1010, polyamide 1012, polyamide 10T, polyamide MXD6, polyamide 6T / 66, polyamide 6T / 6I, polyamide 6T / 6I / 66, polyamide 6T / 2M-5T, polyamide 9T / 2M-8T, and the like.
- These polyamides may be used alone or in combination of two or more.
- a structure in which the hydrocarbon group sandwiched between adjacent amide bonds in the main chain is 6 or more (usually 16 or less) (the present invention)
- a polyamide resin having a simple “long chain structure” can be used. That is, it is a polyamide resin having a long chain structure.
- a long chain structure it is preferable to have 50% or more of the long chain structure among all the structural units of the polyamide resin, and may be 100%.
- Specific examples include polyamide 11, polyamide 610, polyamide 612, polyamide 614, polyamide 12, polyamide 6T, polyamide 6I, polyamide 9T, polyamide 1010, polyamide 1012, polyamide 10T, polyamide 9T / 2M-8T. These polyamides may be used alone or in combination of two or more.
- plant-derived polyamide resin can be used among the above-mentioned various polyamide resins.
- the plant-derived polyamide resin is a resin that uses a monomer obtained from a plant-derived component such as vegetable oil, and is therefore desirable from the viewpoint of environmental protection (particularly from the viewpoint of carbon neutral).
- Examples of plant-derived polyamide resins include polyamide 11 (hereinafter also simply referred to as “PA11”), polyamide 610 (hereinafter also simply referred to as “PA610”), polyamide 612 (hereinafter also simply referred to as “PA612”), polyamide 614 (hereinafter referred to as “PA612”).
- PA614 Polyamide 1010
- PA1012 polyamide 1012
- PA10T polyamide 10T
- PA11 is superior to other plant-derived polyamide resins in terms of low water absorption, low specific gravity, and high degree of planting.
- Polyamide 610 is inferior to PA 11 in terms of water absorption, chemical resistance, and impact strength, but is excellent in terms of heat resistance (melting point) and strength.
- Polyamide 1010 is superior to PA11 in terms of heat resistance and strength.
- the degree of planting is equivalent to PA11, and it can be used for parts that require more durability. Since polyamide 10T includes an aromatic ring in the molecular skeleton, it has a higher melting point and higher strength than polyamide 1010. Therefore, it can be used in more severe environments.
- the weight average molecular weight (standard polystyrene conversion) by the gel permeation chromatography (GPC) of a polyamide resin is not specifically limited, For example, it can be 5,000 or more and 100,000 or less, and is 7,500 or more and 50,000 or less. Preferably, it is 10,000 or more and 50,000 or less.
- the modified elastomer constituting the thermoplastic resin sheet is an elastomer having a reactive group for the polyamide resin.
- This modified elastomer is preferably a component having affinity for the polyolefin resin. That is, it is preferably a component having a compatibilizing effect on the polyamide resin and the polyolefin resin. In other words, it is preferably a compatibilizer between a polyamide resin and a polyolefin resin.
- the reactive group includes an acid anhydride group (—CO—O—OC—), a carboxyl group (—COOH), and an epoxy group ⁇ —C 2 O (a three-membered ring comprising two carbon atoms and one oxygen atom). Structure) ⁇ , an oxazoline group (—C 3 H 4 NO), an isocyanate group (—NCO), and the like. These may use only 1 type and may use 2 or more types together.
- the amount of modification of the modified elastomer is not limited, and the modified elastomer may have one or more reactive groups in one molecule. Further, the modified elastomer preferably has 1 or more and 50 or less reactive groups in one molecule, more preferably 3 or more and 30 or less, and particularly preferably 5 or more and 20 or less.
- modified elastomers polymers using various monomers capable of introducing reactive groups (modified elastomers obtained by polymerization using monomers capable of introducing reactive groups), and oxidative degradation products of various polymers (oxidation)
- Modified elastomers in which reactive groups have been formed by decomposition) and graft polymers of organic acids to various polymers Modified elastomers in which reactive groups have been introduced by graft polymerization of organic acids.
- These may use only 1 type and may use 2 or more types together. These may use only 1 type and may use 2 or more types together.
- Examples of the monomer capable of introducing a reactive group include a monomer having a polymerizable unsaturated bond and an acid anhydride group, a monomer having a polymerizable unsaturated bond and a carboxyl group, and a polymerizable unsaturated bond.
- Examples thereof include monomers having an epoxy group.
- acid anhydrides such as maleic anhydride, itaconic anhydride, succinic anhydride, glutaric anhydride, adipic anhydride, citraconic anhydride, tetrahydrophthalic anhydride, butenyl succinic anhydride, and maleic acid, itaconic acid And carboxylic acids such as fumaric acid, acrylic acid and methacrylic acid. These may be used alone or in combination of two or more. Of these compounds, acid anhydrides are preferred, maleic anhydride and itaconic anhydride are more preferred, and maleic anhydride is particularly preferred.
- skeleton resin the type of resin constituting the skeleton of the modified elastomer
- various thermoplastic resins can be used.
- this skeleton resin one kind or two or more kinds of various resins exemplified above as the polyolefin resin can be used.
- an olefin-based thermoplastic elastomer and a styrene-based thermoplastic elastomer can be used as the skeleton resin. These may use only 1 type and may use 2 or more types together.
- the olefin-based thermoplastic elastomer examples include a copolymer obtained by copolymerizing two or more olefins.
- the olefin one or more of the various olefins exemplified above as the olefin constituting the polyolefin resin can be used.
- the olefin-based thermoplastic elastomer a copolymer of ethylene and an ⁇ -olefin having 3 to 8 carbon atoms and a copolymer of propylene and an ⁇ -olefin having 4 to 8 carbon atoms are preferable.
- copolymers of ethylene and ⁇ -olefin having 3 to 8 carbon atoms include ethylene / propylene copolymer (EPR), ethylene / 1-butene copolymer (EBR), ethylene / 1-pentene copolymer. And ethylene / 1-octene copolymer (EOR).
- EPR ethylene / propylene copolymer
- EBR ethylene / 1-butene copolymer
- EOR ethylene / 1-octene copolymer
- Examples of the copolymer of propylene and ⁇ -olefin having 4 to 8 carbon atoms include propylene / 1-butene copolymer (PBR), propylene / 1-pentene copolymer, propylene / 1-octene copolymer. (POR). These may use only 1 type and may use 2 or more types together.
- examples of the styrenic thermoplastic elastomer include a block copolymer of a styrene compound and a conjugated diene compound, and a hydrogenated product thereof.
- examples of the styrene compound include styrene, ⁇ -methyl styrene, p-methyl styrene, alkyl styrene such as pt-butyl styrene, p-methoxy styrene, vinyl naphthalene, and the like. These may use only 1 type and may use 2 or more types together.
- conjugated diene compound examples include butadiene, isoprene, piperylene, methylpentadiene, phenylbutadiene, 3,4-dimethyl-1,3-hexadiene, 4,5-diethyl-1,3-octadiene, and the like. These may use only 1 type and may use 2 or more types together.
- styrene-based thermoplastic elastomers include styrene-butadiene-styrene copolymer (SBS), styrene-isoprene-styrene copolymer (SIS), styrene-ethylene / butylene-styrene copolymer (SEBS), styrene- And ethylene / propylene-styrene copolymer (SEPS). These may use only 1 type and may use 2 or more types together. Of these, SEBS is preferred.
- the weight average molecular weight (standard polystyrene conversion) by the gel permeation chromatography (GPC) of a modified elastomer is not specifically limited, For example, it can be 10,000 or more and 500,000 or less, for example, 35,000 or more and 500,000 or less. Preferably, 35,000 or more and 300,000 or less are more preferable.
- thermoplastic resin sheet In addition to polyolefin resin, polyamide resin, and modified elastomer, other components can be blended in the thermoplastic resin sheet.
- Other components include fillers (reinforcing fillers), nucleating agents, antioxidants, heat stabilizers, weathering agents, light stabilizers, plasticizers, UV absorbers, antistatic agents, flame retardants, and flame retardant aids. , Slip agent, anti-blocking agent, anti-fogging agent, lubricant, antibacterial agent, colorant (pigment, dye), dispersant, copper damage inhibitor, neutralizer, anti-bubble agent, weld strength improver, natural oil, synthetic An oil, a wax, etc. are mentioned. These may use only 1 type and may use 2 or more types together.
- thermoplastic resins examples include polyester resins (polybutylene terephthalate, polyethylene terephthalate, polycarbonate, polybutylene succinate, polyethylene succinate, polylactic acid) and the like. These may use only 1 type and may use 2 or more types together.
- Fillers include glass components (glass fibers, glass beads, glass flakes, etc.), silica, inorganic fibers (glass fibers, alumina fibers, carbon fibers), graphite, silicate compounds (calcium silicate, aluminum silicate, montmorillonite, kaolin, talc) , Clay, etc.), metal oxides (iron oxide, titanium oxide, zinc oxide, antimony oxide, alumina, etc.), carbonates and sulfates of metals such as lithium, calcium, magnesium, zinc, metals (aluminum, iron, silver, Copper, etc.), hydroxides (aluminum hydroxide, magnesium hydroxide, etc.), sulfides (barium sulfate, etc.), carbides (charcoal, bamboo charcoal, etc.), titanates (potassium titanate, barium titanate, etc.), organic fibers ( Aromatic polyester fiber, aromatic polyamide fiber, fluororesin fiber, polyimide fiber, vegetable fiber, etc. , Celluloses (cellulose microfibril
- Phase structure The phase structure exhibited by the thermoplastic resin sheet is not limited, but may have the following phase structures (1) to (3).
- Phase structure (1) Phase structure having a continuous phase (A) containing a polyolefin resin and a dispersed phase (B) containing a polyamide resin and a modified elastomer dispersed in the continuous phase (A) (FIG. 1). However, other phase structures having a continuous phase containing a polyamide resin and a dispersed phase dispersed in the continuous phase do not coexist.
- Phase structure (2) A phase structure having a continuous phase containing a polyamide resin and a dispersed phase containing a polyolefin resin dispersed in the continuous phase.
- Phase structure (3) a continuous phase (A 1 ) containing a polyolefin resin, a dispersed phase (B A1 ) containing a polyamide resin and a modified elastomer dispersed in the continuous phase (A 1 ), and a polyamide resin phase structure having the inclusive continuous phase (a 2), dispersed in a continuous phase (a 2), the dispersed phase containing the modified elastomer and (B A2), (see Figure 2).
- the phase structure (1) or the phase structure (3) is preferable, and the phase structure (1) is more preferable.
- the dispersed phase (B) in the phase structure (1) is a continuous phase in the dispersed phase (B), and a continuous phase (B 1 ) containing a polyamide resin, A finely dispersed phase dispersed in the continuous phase (B 1 ) and containing a modified elastomer (B 2 ) (see FIG. 1).
- the phase structure (1) exhibits a multiphase structure having a finely dispersed phase (B 1 ) in the dispersed phase (B).
- the modified elastomer may be an unreacted modified elastomer, a reaction product with a polyamide resin, or a mixture thereof.
- the phase structure (3) can exhibit a co-continuous phase structure in which two continuous phases of the continuous phase (A 1 ) and the continuous phase (A 2 ) coexist.
- the dispersed phase in the continuous phase (A 1) (B A1) is a continuous phase within the dispersed phase (B A1), the continuous phase comprising a polyamide resin and (B A11), the continuous phase (B A11 ) and a finely dispersed phase (B A12 ) containing a modified elastomer.
- the phase structure (3) exhibits a multiphase structure having a finely dispersed phase (B A12 ) in the dispersed phase (B A1 ).
- the modified elastomer may be an unreacted modified elastomer, a reaction product with a polyamide resin, or a mixture thereof.
- the continuous phase (A) contains a polyolefin resin.
- the polyolefin resin is a main component of the continuous phase (A) (generally 70% by mass or more and may be 100% by mass with respect to the entire continuous phase A).
- the dispersed phase (B) contains a polyamide resin and a modified elastomer.
- the polyamide resin (when the dispersed phase (B) contains a modified elastomer, the polyamide resin and the modified elastomer) is the main component of the dispersed phase (B) (generally 70% by mass or more with respect to the entire dispersed phase B, and 100% by mass). %).
- the continuous phase (B 1 ) contains a polyamide resin.
- the polyamide resin is a main component of the continuous phase (B 1 ) (typically 70% by mass or more and may be 100% by mass with respect to the entire continuous phase B 1 ).
- the finely dispersed phase (B 2 ) contains a modified elastomer.
- the modified elastomer is a main component of the finely dispersed phase (B 2 ) (typically 70% by mass or more and may be 100% by mass with respect to the entire finely dispersed phase B 2 ).
- the continuous phase (A 1 ) contains a polyolefin resin.
- the polyolefin resin is a main component of the continuous phase (A 1 ) (typically 70% by mass or more and may be 100% by mass with respect to the entire continuous phase A 1 ).
- the dispersed phase (B A1 ) contains a polyamide resin and a modified elastomer.
- the polyamide resin and the modified elastomer are the main components of the dispersed phase (B A1 ) (generally 70% by mass or more and may be 100% by mass with respect to the entire dispersed phase B A1 ).
- the continuous phase (B A11 ) contains a polyamide resin.
- the polyamide resin is the main component of the continuous phase (B A11 ) (typically 70% by mass or more and may be 100% by mass with respect to the entire continuous phase B A11 ).
- the finely dispersed phase (B A12 ) contains a modified elastomer.
- the modified elastomer is a main component of the finely dispersed phase (B A12 ) (generally 70% by mass or more and may be 100% by mass with respect to the entire finely dispersed phase B A12 ).
- the continuous phase (A 2 ) includes a polyamide resin.
- the polyamide resin is a main component of the continuous phase (A 2 ) (typically 70% by mass or more and may be 100% by mass with respect to the entire continuous phase A 2 ).
- the dispersed phase (B A2 ) with respect to the continuous phase (A 2 ) contains a modified elastomer.
- the modified elastomer is a main component of the dispersed phase (B A2 ) (typically 70% by mass or more and may be 100% by mass with respect to the entire dispersed phase B A2 ).
- thermoplastic resin sheet having a larger value of S 140 / S 120 described later can be obtained.
- these phase structures can be more reliably obtained by melt-kneading a melt-kneaded product of a polyamide resin and a modified elastomer and a polyolefin resin.
- the reactive group of the modified elastomer can be a reaction product obtained by reacting with the polyamide resin.
- the reactant is, for example, an interface between the continuous phase (A) and the dispersed phase (B) and / or a continuous phase (B 1 ) and a finely dispersed phase (B 2 ). Can exist at the interface.
- the phase structure (3) for example, the interface between the continuous phase (A 1 ) and the continuous phase (A 2 ), the interface between the continuous phase (A 1 ) and the dispersed phase (B A1 ), the continuous phase (B A11 ) and the finely dispersed phase (B A12 ), etc.
- phase structures can be observed with a field emission scanning electron microscope (FE-SEM) after the oxygen plasma etching treatment and further on the treated surface of the osmium-coated test piece (thermoplastic resin sheet test piece).
- FE-SEM field emission scanning electron microscope
- the dispersed phase and the finely dispersed phase can be observed by an image magnified 1000 times or more (usually 10,000 times or less) in this method.
- the components constituting each phase can be specified by performing energy dispersive X-ray analysis (EDS) during observation using a field emission scanning electron microscope (FE-SEM).
- the size of the dispersed phase (dispersed phase B in FIG. 1, dispersed phase B A1 in FIG. 2) of the thermoplastic resin sheet is not particularly limited, but the dispersed diameter (average dispersed diameter) is preferably 10,000 nm or less. More preferably, they are 50 nm or more and 8000 nm or less, More preferably, they are 100 nm or more and 4000 nm or less.
- the dispersion diameter of the dispersed phase can be measured in an enlarged image of 1000 times or more obtained using an electron microscope. That is, the longest diameter of each of the 20 dispersed phases randomly selected from a predetermined region in the image is measured, and the average value of the longest diameters obtained is set as the first average value. And the further average value of the 1st average value measured in five different area
- the finely dispersed phase (the finely dispersed phase B 2 in FIG. 1 and the finely dispersed phase B A12 in FIG. 2) contained in the dispersed phase (dispersed phase B in FIG. 1, dispersed phase B A1 in FIG. 2) of the thermoplastic resin sheet. )
- the dispersion diameter is preferably 5 nm to 1000 nm, more preferably 5 nm to 600 nm, still more preferably 10 nm to 400 nm, and particularly preferably 15 nm. It is 350 nm or less.
- the dispersion diameter of the finely dispersed phase can be measured in an enlarged image of 1000 times or more obtained using an electron microscope.
- the longest diameter of each of the 20 finely dispersed phases randomly selected from a predetermined region in the image is measured, and the average value of the obtained longest diameters is set as the first average value.
- regions in an image is the average dispersion diameter (major axis average dispersion diameter) of a fine dispersion phase.
- the ratio of the polyolefin resin may be 2% by mass or more and 90% by mass or less. It can. This proportion is preferably 5% by mass to 85% by mass, more preferably 10% by mass to 83% by mass, further preferably 15% by mass to 80% by mass, and further preferably 20% by mass to 78% by mass. Furthermore, 25 mass% or more and 75 mass% or less are preferable, 30 mass% or more and 73 mass% or less are more preferable, and 35 mass% or more and 70 mass% or less are more preferable. In the above range, it is possible that the value of S 140 / S 120 to obtain a greater thermoplastic resin sheet.
- the ratio of the polyamide resin and the modified elastomer (some or all of these may be reacted with each other) Can be 10 mass% or more and 98 mass% or less. This ratio is preferably 15% by mass to 95% by mass, more preferably 17% by mass to 90% by mass, further preferably 20% by mass to 85% by mass, and further preferably 22% by mass to 80% by mass. Furthermore, 25 mass% or more and 75 mass% or less are preferable, 27 mass% or more and 70 mass% or less are more preferable, and 30 mass% or more and 65 mass% or less are more preferable. In the above range, it is possible that the value of S 140 / S 120 to obtain a greater thermoplastic resin sheet.
- the ratio of the polyamide resin can be 1% by mass to 75% by mass. This proportion is preferably 2% by mass or more and 70% by mass or less, more preferably 4% by mass or more and 65% by mass or less, further preferably 6% by mass or more and 60% by mass or less, and further preferably 8% by mass or more and 55% by mass or less. Furthermore, 10 mass% or more and 50 mass% or less are preferable, 12 mass% or more and 45 mass% or less are more preferable, and 15 mass% or more and 40 mass% or less are more preferable. In the above range, it is possible that the value of S 140 / S 120 to obtain a greater thermoplastic resin sheet.
- the ratio of the modified elastomer can be 1% by mass or more and 60% by mass or less. This proportion is preferably 2% to 55% by mass, more preferably 4% to 45% by mass, further preferably 6% to 40% by mass, and further preferably 8% to 38% by mass. Furthermore, 10 mass% or more and 37 mass% or less are preferable, 12 mass% or more and 36 mass% or less are preferable, and 15 mass% or more and 35 mass% or less are more preferable. In the above range, it is possible that the value of S 140 / S 120 to obtain a greater thermoplastic resin sheet.
- the ratio of the polyamide resin can be 1.5% by mass or more and 88% by mass or less. This ratio is preferably 3% by mass or more and 75% by mass or less, more preferably 5% by mass or more and 70% by mass or less, further preferably 10% by mass or more and 65% by mass or less, and further preferably 15% by mass or more and 60% by mass or less. Furthermore, 18 mass% or more and 55 mass% or less are preferable, 20 mass% or more and 50 mass% or less are more preferable, and 25 mass% or more and 45 mass% or less are more preferable. In the above range, it is possible that the value of S 140 / S 120 to obtain a greater thermoplastic resin sheet.
- the ratio of the modified elastomer can be 20% by mass or more and 90% by mass or less. This ratio is preferably 22% by mass or more and 88% by mass or less, more preferably 25% by mass or more and 86% by mass or less, further preferably 27% by mass or more and 75% by mass or less, and preferably 29% by mass or more and 70% by mass or less. Furthermore, 32 mass% or more and 66 mass% or less are preferable, and also 36 mass% or more and 60 mass% or less are preferable. In the above range, it is possible that the value of S 140 / S 120 to obtain a greater thermoplastic resin sheet.
- the proportion of the polyolefin resin when the total of the above-mentioned polyolefin resin, polyamide resin and modified elastomer is 100% by mass is usually the whole phase. Is equal to the proportion of the continuous phase (A) in the case of 100 mass%.
- the phase structure (3) it is usually equal to the ratio of the continuous phase (A 1 ) when the entire phase is 100% by mass.
- the ratio here is a volume ratio, but is usually equal to an area ratio in which the volume ratio is reflected (the same applies hereinafter).
- the ratio of the polyamide resin and the modified elastomer when the total of the polyolefin resin, the polyamide resin and the modified elastomer is 100% by mass is usually It is equal to the proportion of the dispersed phase (B) when the total phase is 100% by mass.
- the phase structure (3) in the case of the phase structure (3) (see FIG. 2), normally, the dispersed phase (B A1 ), the continuous phase (A 2 ), and the dispersed phase (B A2 ) when the entire phase is 100 mass%. And equal to the total percentage.
- the ratio of the polyamide resin when the total of the above-mentioned polyolefin resin, polyamide resin and modified elastomer is 100% by mass is usually 100 for the entire phase. It is equal to the ratio of the continuous phase (B 1 ) in the case of mass%.
- the phase structure (3) in the case of the phase structure (3) (see FIG. 2), usually, the total ratio of the continuous phase (A 2 ) and the continuous phase in the dispersed phase (B A11 ) when the entire phase is 100% by mass. be equivalent to.
- the ratio of the modified elastomer when the total of the above-mentioned polyolefin resin, polyamide resin and modified elastomer is 100% by mass is usually 100 for the entire phase. It is equal to the proportion of the finely dispersed phase (B 2 ) in the case of mass%.
- the phase structure (3) in the case of the phase structure (3) (see FIG. 2), it is usually equal to the total ratio of the finely dispersed phase (B A12 ) and the dispersed phase (B A2 ) when the total phase is 100% by mass. .
- thermoplastic resin sheet when the elongation at break at 140 ° C. is S 140 (%) and the elongation at break at 120 ° C. is S 120 (%), S 140 is S 120. 1.2 times or more. That is, S 140 / S 120 ⁇ 1.2.
- This “S 140 / S 120 ” is usually 3.5 or less.
- “S 140 / S 120 ” may exceed 3.5, but if it is excessively large, it may be difficult to control the elongation in a temperature range suitable for processing. Therefore, “S 140 / S 120 ” is preferably 1.2 ⁇ S 140 / S 120 ⁇ 3.5. Further, the ratio is more preferably 1.3 ⁇ S 140 / S 120 ⁇ 3.0, more preferably 1.4 ⁇ S 140 / S 120 ⁇ 2.5, and 1.5 ⁇ S 140 / S 120 ⁇ 2.0 is particularly preferred.
- the above-mentioned breaking elongation (%) is measured and calculated by the following method. That is, a test piece in which a thermoplastic resin sheet having a basis weight of 300 g / m 2 is formed into a 6 mm ⁇ 35 mm strip is prepared. Next, the above test piece is set in a tensile tester having a distance between chucks of 20 mm (initial value T 0 ), held at a temperature for measurement for 2 minutes, and then a tensile test until the test piece breaks at the same temperature. I do. The distance between the chucks at the breaking point is T (mm), and the value calculated by “T (mm) / 20 (mm) ⁇ 100” is “breaking elongation (%)”.
- polyolefin resins are widely used in industrial products.
- its high fluidity is easy to use and convenient.
- pressure molding for example, cold pressing after heating
- the polyolefin resin tends to be too soft at the molding temperature and may be difficult to process.
- auxiliary sheet is used to assist the polyolefin in a heated state.
- this auxiliary sheet for example, a laminated film in which a nylon film is sandwiched between two layers of polyolefin film and integrated is used.
- the auxiliary sheet Insufficient elongation may be a problem. That is, it is difficult for the conventionally known auxiliary sheet to obtain an appropriate elongation at the processing temperature of the polyolefin.
- polyolefin and nylon are materials that are difficult to join, and there is a problem that the cost of integrating the three layers is required together with the cost of the three-layer raw material film, leading to an increase in the cost of the auxiliary sheet itself.
- thermoplastic resin sheet can exhibit suitable characteristics. That is, as described above, this thermoplastic resin sheet has S 140 / S 120 ⁇ 1.2, has a large change in elongation in the optimum processing temperature range for the polyolefin resin, and is harder than the polyolefin resin. Characteristics can be maintained. Therefore, this thermoplastic resin sheet can be suitably used as an auxiliary sheet at the time of pressure molding of a molded body containing the polyolefin resin as described above.
- thermoplastic resin sheet contains a polyolefin resin as its component, it has excellent affinity with the polyolefin resin, and when the polyolefin resin is molded, the thermoplastic resin sheet used as an auxiliary sheet is integrated, It can remain on the surface of the polyolefin resin (see FIG. 4). That is, after being used as an auxiliary sheet, the thermoplastic resin sheet can be directly heat-sealed to the surface of a molded body containing a polyolefin resin to form a part of the molded body (see FIG. 4).
- thermoplastic resin constituting the thermoplastic resin sheet can exhibit extremely excellent impact resistance (as shown in the aforementioned Patent Documents 1 to 4), it remains on the surface of the molded body containing the polyolefin resin. By making it, the outstanding impact resistance can also be provided to this molded object. That is, high impact resistance can be imparted, and the molded body can be imparted with a property that is difficult to break.
- the thickness of the thermoplastic resin sheet is not particularly limited, and may be an appropriate thickness as required.
- This thermoplastic resin sheet can also be called a thermoplastic resin film.
- As a specific thickness for example, a range of 0.01 ⁇ m or more and 5000 ⁇ m or less can be used.
- the thermoplastic resin sheet is used alone (for example, when the thermoplastic resin sheet itself is shaped and used as a base material, when used as a translucent film, etc.), it is 50 ⁇ m or more. It is preferably 4800 ⁇ m or less, more preferably 100 ⁇ m or more and 4500 ⁇ m or less, and particularly preferably 500 ⁇ m or more and 4200 ⁇ m or less.
- the thickness is preferably from 0.1 ⁇ m to 2500 ⁇ m, more preferably from 1 ⁇ m to 1000 ⁇ m, and particularly preferably from 10 ⁇ m to 500 ⁇ m.
- the basis weight of the thermoplastic resin sheet is not particularly limited, and may be an appropriate basis weight as necessary.
- the basis weight may be 1 g / m 2 or more and 1000 g / m 2 or less.
- it is preferably 25 g / m 2 or more and 800 g / m 2 or less.
- thermoplastic resin sheet The method for producing the thermoplastic resin sheet is not limited, and can be produced by a conventionally known method.
- a sheet forming method such as an extrusion method, a coating method, a casting method, a pressing method, an injection molding method or an inflation method can be used.
- this thermoplastic resin sheet may be extended
- thermoplastic resin composition constituting the thermoplastic resin sheet is not limited, but it can be obtained more reliably by, for example, melt-kneading a melt-kneaded product of a polyamide resin and a modified elastomer and a polyolefin resin. be able to.
- any melt-kneading apparatus may be used for the preparation of the above-mentioned melt-kneaded product and the melt-kneading of the melt-kneaded product and the polyolefin resin.
- an extruder single screw extruder, twin screw kneading extruder, etc.
- a kneader a mixer (high-speed flow mixer, paddle mixer, ribbon mixer, etc.), etc.
- the melt kneading temperature of the polyamide resin and the modified elastomer is not limited, but can be, for example, 190 ° C. or higher and 350 ° C. or lower, preferably 200 ° C. or higher and 330 ° C. or lower, and more preferably 205 ° C. or higher and 310 ° C. or lower.
- the melt kneading temperature of the obtained melt-kneaded product and the polyolefin resin is not limited, but can be, for example, 190 ° C or higher and 350 ° C or lower, preferably 200 ° C or higher and 300 ° C or lower, and 205 ° C or higher and 260 ° C or lower. Is more preferable.
- the laminated sheet (3) of the present invention comprises a base layer (31) containing a polyolefin resin, And the thermoplastic resin sheet (1) of the present invention joined to one surface of the base layer (31) (see FIG. 3).
- the base layer 31 and the thermoplastic resin sheet 1 are usually joined.
- the joining method at this time is not limited, and may be joined via an adhesive or may be heat-sealed.
- the base layer 31 containing polyolefin resin means containing polyolefin resin as the constituent material.
- the amount of the polyolefin resin contained in the base layer 31 is not limited. Usually, when the entire base layer 31 is 100% by mass, the polyolefin resin is contained by 50% by mass or more.
- the polyolefin resin may be contained uniformly in the base layer 31 or may be contained non-uniformly.
- the base layer 31 may be comprised only from polyolefin resin.
- the entire base layer 31 is 100% by mass, 100% by mass of the polyolefin resin may be included.
- the description regarding the polyolefin resin which comprises this thermoplastic resin sheet 1 is applicable as it is.
- the polyolefin resin constituting the base layer 31 and the polyolefin resin constituting the thermoplastic resin sheet 1 may be different, but are preferably the same type. By being the same kind, higher affinity can be obtained, and the base layer 31 and the thermoplastic resin sheet 1 can be easily joined without using an adhesive, which is preferable.
- the same type includes, for example, the case where 50% or more (preferably 70% or more, more preferably 90% or more) of the structural units of the polymer constituting the polyolefin resin are the same.
- the polyolefin resin constituting the base layer 31 and the polyolefin resin constituting the thermoplastic resin sheet 1 include different structural units, the upper limit of the same structural unit is less than 100%, and different structural units are included. When not included, the proportion of the same structural unit is 100%.
- the laminated sheet 3 may be composed of only the base layer 31 and the thermoplastic resin sheet 1, but can have another layer 32.
- the thermoplastic resin sheet 1 can be sandwiched between the base layer 31 and the other layer 32.
- the other layer 32 may be another layer containing the same polyolefin resin as the base layer 31.
- the laminated sheet 3 includes a form in which the base layer 31 is a polypropylene sheet, and the thermoplastic resin sheet 1 includes polypropylene as a polyolefin resin (FIGS. 3A and 3B). reference).
- the thermoplastic resin sheet 1 includes polypropylene as a polyolefin resin, and the other layer 32 has a layer made of a polyamide resin (see FIG. 3 (b)).
- the thickness of the base layer 31 is not particularly limited, and may be an appropriate thickness as necessary.
- the thickness is preferably in the range of 1 ⁇ m to 5000 ⁇ m.
- the basis weight of the base layer 31 is not particularly limited, and may be an appropriate basis weight according to need.
- the basis weight may be 1 g / m 2 or more and 1000 g / m 2 or less.
- it is preferably 25 g / m 2 or more and 800 g / m 2 or less.
- the laminated sheet 3 includes the thermoplastic resin sheet 1 as described above, the laminated sheet 3 can be suitably used as a shaping auxiliary sheet when pressure-molding a molded body containing a polyolefin resin. That is, since the thermoplastic resin sheet 1 has a characteristic of S 140 / S 120 ⁇ 1.2, it is harder than the base layer 31 at the same temperature in the laminated sheet 3, but maintains the property of being easily stretched. it can. Furthermore, the laminated sheet used as an auxiliary sheet at the time of molding a molded body made of polyolefin resin or a molded body containing polyolefin resin is integrated into the molded body as it is and remains on the surface of the molded body (see FIG. 4). be able to.
- the laminated sheet 3 can be heat-sealed to the surface of the base 51 as it is to form a part of the molded body 5 (see FIG. 4).
- the molded body 5 thus obtained can exhibit extremely excellent impact resistance.
- the molded body (5) of the present invention comprises a substrate (51) containing a polyolefin resin, The thermoplastic resin sheet (1) of the present invention or the laminated sheet (3) of the present invention bonded to one surface of the base (51) (see FIG. 4).
- thermoplastic resin sheet 1 and the laminated sheet 3 are as described above.
- the substrate 51 include a molded body made only of a polyolefin resin and a fiber reinforced molded body containing a polyolefin resin as a binder. That is, the fiber-reinforced molded body is a molded body that includes a reinforcing fiber and a binder that binds the reinforcing fibers, and a polyolefin resin is used as the binder.
- the form of the base body 51 is not limited, for example, it can have a plate shape having a substantially uniform thickness as a whole. Moreover, it can have the uneven
- the molded body 5 is suitable when the base 51 has a deep-drawn portion 55 that is shaped by being greatly drawn as shown in FIGS. 4 (a) and 4 (b).
- suitable shaping can be performed by using this thermoplastic resin sheet 1 or this lamination sheet 3 as an auxiliary sheet. That is, for example, it is possible to prevent a situation in which the base 51 is not sufficiently drawn, or excessive thinning.
- thermoplastic resin sheet or the present laminated sheet on the surface of the molded body 5, it is difficult to break while using the base 51 in which the reinforcing fibers are bound with a resin binder, or It can be made into a molded body that does not break.
- Such a base 51 can be obtained, for example, by heating and compressing a mixed fiber (a mixture of fibers) of reinforcing fibers and fibers (resin fibers) formed from a polyolefin resin. More specifically, for example, after obtaining a fiber reinforced board obtained by heating and compressing a mixture of reinforcing fibers and polyolefin resin fibers, necessary processing is performed, and the polyolefin resin (resin fibers) is heated and softened again ( If necessary, the substrate 51 can be obtained by shaping while providing a concavo-convex shape (see PR2 in FIG. 5).
- the type of reinforcing fiber is not limited, and inorganic fiber (glass fiber or the like) or organic fiber (natural fiber such as plant fiber or animal fiber) can be used. These may use only 1 type and may use 2 or more types together. Of these, organic fibers are preferable, natural fibers are more preferable, and plant fibers are particularly preferable.
- Plant fiber is a fiber derived from a plant, and includes a fiber taken out from a plant and a fiber obtained by processing the fiber. Plant fibers include leaf vein plant fibers, bast plant fibers, woody plant fibers, and other plant fibers. These may use only 1 type and may use 2 or more types together. Specific examples include abaca, sisal, agave, flux, jute, hemp, kenaf, ramie, coconut shell fiber, oil palm empty fruit bunch fiber, rice straw fiber, wheat straw fiber, bamboo fiber, and cotton.
- the fiber length of the reinforcing fiber is not limited, the average fiber length can be 10 to 200 mm (further 20 to 170 mm, particularly 30 to 150 mm). This average fiber length is based on JIS L1015. Single fibers are randomly picked up one by one by the direct method, stretched straight without stretching, and the fiber length is measured on a measuring scale. It is the average value of the measured values.
- the polyolefin resin described in the thermoplastic resin sheet and the laminated sheet can be applied as it is.
- the polyolefin resin as a binder can further contain a modified polyolefin resin (excluding a modified elastomer) modified by introducing a polar group.
- polar groups include carboxylic anhydride groups (—CO—O—OC—), carboxylic acid groups (—COOH), carbonyl groups (—CO—), hydroxyl groups (—OH), amino groups (—NH 2 ), Examples thereof include a nitro group (—NO 2 ) and a nitrile group (—CN). These may use only 1 type and may use 2 or more types together.
- the molded body 5 can have a skin 52 (see FIG. 4B).
- the skin 52 is, for example, a layer laminated on one surface side of the base 51, and the outer surface thereof is a layer that becomes the design surface of the molded body 5. That is, the skin 52 usually constitutes the design surface of the molded body 5.
- the molded body 5 has a concavo-convex shape, it is laminated (further bonded) to the surface of the substrate 51 following the concavo-convex shape.
- the configuration of the skin layer 12 is not limited, and may be composed of only one layer or may be composed of two or more layers. In the case of two or more layers, for example, a laminate comprising a surface layer having a design surface (for example, synthetic leather or woven fabric) and a cushion layer (arranged on the non-design surface side of the skin 52), can do.
- the manufacturing method of the molded object 5 is not limited, For example, when using the base
- the heating step (PR1) is a step of heating the fiber reinforced board 51 to soften the polyolefin resin contained in the fiber reinforced board 51.
- the fiber reinforced board 51 used in this step is a precursor that becomes the base 51 in the molded body 5.
- the fiber reinforced board 51 is a compressed plate-like body containing reinforcing fibers and a polyolefin resin, and usually has a flat plate shape.
- the thickness of the fiber reinforced board 51 can be set to 1 mm or more and 10 mm or less, for example.
- the fiber reinforcing board 51 may be heated in any way, but it is preferable to heat the fiber reinforcing board 51 while applying pressure so that the compression is not excessively released. From such a viewpoint, it is preferable to use a hot press machine 91 (see FIG. 5). Although heating conditions etc. are not limited, For example, it is preferable to heat to 70 degreeC or more (temperature inside the fiber reinforced board 51).
- the heating temperature is preferably 80 ° C. or higher and 150 ° C. or lower, more preferably 85 ° C. or higher and 130 ° C. or lower, and particularly preferably 90 ° C. or higher and 120 ° C. or lower.
- the shaping step (PR2) is a step of shaping the fiber reinforced board 51 in which the polyolefin resin is softened. This step can be performed using a cold press 92 (see FIG. 5).
- the molding conditions at the time of cold press molding are not particularly limited, for example, the mold temperature at the time of molding can be 20 ° C. or more and 60 ° C. or less.
- the mold clamping time can be 30 seconds or more and 60 seconds or less.
- the skin 52 and the thermoplastic resin sheet 1 or the laminated sheet 3 are laminated and pressed together with the base 51 to form the fiber reinforced board 51 at the same time as the skin 52 and
- the main molded body 5 in which the thermoplastic resin sheet 1 or the laminated sheet 3 is bonded to one surface of the fiber reinforced board 55 can be obtained (see FIG. 5).
- thermoplastic resin sheet and the laminated sheet are not particularly limited.
- the thermoplastic resin sheet and the laminated sheet are used as sheets constituting exterior materials, interior materials, structural materials, impact absorption auxiliary materials, etc. for automobiles, railway vehicles, ships and airplanes. Can do.
- size, and thickness of this molded object 5 are not specifically limited.
- the use is also not specifically limited.
- it can be used as exterior materials, interior materials, structural materials, impact absorbing auxiliary materials, etc. for automobiles, railway vehicles, ships and airplanes.
- examples of the automobile article include an automotive exterior material, an automotive interior material, an automotive structural material, an automotive shock absorber, and an engine room component.
- Energy absorber such as body shell components such as a front-end module and the like.
- thermoplastic resin sheet 1 and the laminated sheet 3 can be used as sheets constituting interior materials such as buildings and furniture, exterior materials, and structural materials, for example.
- size, and thickness of this molded object 5, are not specifically limited, The use is also not specifically limited. Examples thereof include interior materials such as buildings and furniture, exterior materials, and structural materials. That is, it can be used as a door covering material and a structural material, and a covering material and a structural material of various furniture (desk, chair, shelf, bag, etc.). In addition, it can be used as a package, a container (such as a tray), a protective member, a partition member, and the like.
- a housing and a structure of a home appliance a thin TV, a refrigerator, a washing machine, a vacuum cleaner, a mobile phone, a portable game machine, a notebook computer, etc.
- a home appliance a thin TV, a refrigerator, a washing machine, a vacuum cleaner, a mobile phone, a portable game machine, a notebook computer, etc.
- it can be suitably used as electronic / electrical equipment, medical equipment, civil engineering and building materials, food-related materials, office equipment parts, and the like.
- Thermoplastic Resin Sheet of Experimental Example 1 Thermoplastic Resin Sheet of Experimental Example 1 The following polyamide resin pellets and the following modified elastomer pellets are dry blended, then charged into a biaxial melt kneading extruder and kneaded. Melt-kneading was performed at a temperature of 210 ° C., and pellets made of a melt-kneaded product of polyamide resin and modified elastomer were obtained via a pelletizer.
- pellets made of a melt-kneaded product of polyamide resin and modified elastomer are put into a biaxial melt-kneading extruder and melt-kneaded at a kneading temperature of 210 ° C.
- a sheet made of a thermoplastic resin composition having a basis weight of 300 g / m 2 was obtained via a T-die extruder.
- the blending ratio of the polyolefin resin, the polyamide resin, and the modified elastomer was 55:25:20 by mass ratio.
- thermoplastic resin composition having this mass ratio exhibits a phase structure (1) (see FIG. 1).
- Polyolefin resin Polypropylene resin, homopolymer, manufactured by Nippon Polypro Co., Ltd., product name “Novatech MA1B”, weight average molecular weight 312,000, melting point 165 ° C.
- Polyamide resin Nylon 11 resin, manufactured by Arkema Co., Ltd., product name “Rilsan BMN O”, weight average molecular weight 18,000, melting point 190 ° C.
- Modified elastomer maleic anhydride modified ethylene / butene copolymer (modified EBR), manufactured by Mitsui Chemicals, Inc., product name “Toughmer MH7020”
- thermoplastic resin sheet of Experimental Example 2 The same as (1) above, except that the mixing ratio of the polyolefin resin, the polyamide resin, and the modified elastomer was 32.5: 42.5: 25 by mass ratio.
- a sheet made of a thermoplastic resin composition having a basis weight of 300 g / m 2 (Experimental Example 2) was obtained.
- the thermoplastic resin composition having this mass ratio exhibits a phase structure (3) (see FIG. 2).
- Thermoplastic resin sheet of Experimental Example 3 Using a T-die extruder, the following polyolefin resin was formed into a sheet having a basis weight of 300 g / m 2 .
- Polyolefin resin Polypropylene resin, block polymer, manufactured by Prime Polymer Co., Ltd., product name “J-452HP”, melting point 165 ° C.
- Thermoplastic resin sheet of Experimental Example 4 Using a T-die extruder, the following polyamide resin was formed into a sheet having a basis weight of 300 g / m 2 .
- Polyamide resin Nylon 6 resin, manufactured by Toray Industries, Inc., product name “Amilan CM1021FS”, melting point 225 ° C.
- thermoplastic resin sheet of Experimental Examples 1 to 4 obtained in [1] above was cut into 6 mm ⁇ 35 mm strips to obtain test pieces for evaluation.
- the test piece was set in a tensile tester (Instron type) with a distance between chucks of 20 mm (initial value T 0 ) and held at a temperature of 80 ° C. for 2 minutes.
- a tensile test was performed at a pulling speed of 50 mm / min until breaking. Then, the distance between chucks at the breaking point was defined as T (mm), and the value calculated by T (mm) / 20 (mm) ⁇ 100 was defined as elongation at break (%).
- thermoplastic resin sheet, 3 laminated sheet, 31; base layer (base layer containing polyolefin resin), 5; molding, 51; substrate (substrate containing polyolefin resin or precursor thereof), 52; skin, 55; deep drawn portion, 91; Hot press machine, 92; Cold press machine,
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Abstract
Description
上記特許文献2には、ポリアミド樹脂とポリオレフィン樹脂とを含んだ樹脂混合物において、植物由来ポリアミド樹脂を利用できることが開示されている。
上記特許文献3には、ポリアミド樹脂とポリオレフィン樹脂とを含んだ樹脂混合物において、連続相と分散相と微分散相とを有する相構造を呈し得ることが開示されている。
上記特許文献4には、ポリアミド樹脂と相容化剤とを溶融混合したのち、得られた樹脂混合物とポリオレフィン樹脂とを更に溶融混合することで、耐衝撃性に優れた樹脂混合物が得られることが開示されている。
しかしながら、上記特許文献1-4には、これらの樹脂混合物をシートとして利用することに関しては検討がない。
上記特許文献5には、ポリアミド樹脂とポリオレフィン樹脂とを含み、海島相構造を呈する熱可塑性樹脂フィルムが開示されている。しかしながら、機械強度に優れたフィルムについての検討、更には、成形時の追従性についての検討はなされていない。
請求項1に記載の熱可塑性樹脂シートは、ポリオレフィン樹脂と、ポリアミド樹脂と、相容化剤と、含み、
前記相容化剤が、前記ポリアミド樹脂に対する反応性基を有する変性エラストマーである熱可塑性樹脂からなることを要旨とする。
請求項2に記載の熱可塑性樹脂シートは、請求項1に記載の熱可塑性樹脂シートにおいて、
前記ポリオレフィン樹脂を含んだ連続相(A)と、
前記連続相(A)中に分散された分散相であって、前記ポリアミド樹脂及び前記変性エラストマーを含んだ分散相(B)と、を有する
請求項3に記載の熱可塑性樹脂シートは、請求項2に記載の熱可塑性樹脂シートにおいて、前記分散相(B)が、前記ポリアミド樹脂を含んだ連続相(B1)と、
前記連続相(B1)中に分散された前記変性エラストマーを含んだ微分散相(B2)と、を有することを要旨とする。
請求項4に記載の熱可塑性樹脂シートは、請求項1乃至3のうちのいずれかに記載の熱可塑性樹脂シートにおいて、前記ポリアミド樹脂及び前記変性エラストマーの溶融混練物と、前記ポリオレフィン樹脂と、の溶融混練物であることを要旨とする。
請求項5に記載の熱可塑性樹脂シートは、請求項1乃至4のうちのいずれかに記載の熱可塑性樹脂シートにおいて、前記ポリアミド樹脂が、主鎖中の隣り合ったアミド結合同士に挟まれた炭化水素基の直鎖炭素数が6以上である構造を有することを要旨とする。
請求項6に記載の熱可塑性樹脂シートは、請求項1乃至5のうちのいずれかに記載の熱可塑性樹脂シートにおいて、前記変性エラストマーは、エチレン若しくはプロピレンと炭素数3~8のα-オレフィンとの共重合体を骨格としたオレフィン系熱可塑性エラストマー、又は、スチレン骨格を有するスチレン系熱可塑性エラストマーであることを要旨とする。
請求項7に記載の熱可塑性樹脂シートは、請求項1乃至6のうちのいずれかに記載の熱可塑性樹脂シートにおいて、温度140℃における破断伸びをS140(%)とし、温度120℃における破断伸びをS120(%)とした場合に、S140がS120の1.2倍以上であることを要旨とする。
請求項8に記載の積層シートは、ポリオレフィン樹脂を含んだ基層と、
前記基層の一面に接合された請求項1乃至7のうちのいずれかに記載の熱可塑性樹脂シートと、を有することを要旨とする。
請求項9に記載の成形体は、ポリオレフィン樹脂を含んだ基体と、
前記基体の一面に接合された請求項1乃至7のうちのいずれかに記載の熱可塑性樹脂シート、又は、請求項8に記載の積層シートと、を有することを要旨とする。
請求項10に記載の成形体は、請求項9に記載の成形体において、前記基体は、補強繊維と、前記補強繊維同士を結着しているバインダと、を含み、
前記バインダは、前記ポリオレフィン樹脂であることを要旨とする。
本積層シートによれば、基層表面に追従性よく接合でき、積層シートに上記熱可塑性樹脂シートが有する機械強度が付与される。また、本積層シートは、成形用基体の表面に貼り付けて利用できる。その際には、得られる成形体表面に本積層シートを追従性よく接合でき、成形体に上記熱可塑性樹脂シートが有する機械強度を付与できる。
本成形体によれば、その一面に上記の熱可塑性樹脂シートが追従性よく接合され、この熱可塑性樹脂シートが有する機械強度が成形体に対して付与される。このため、基体のみが有する機械強度よりも、成形体全体として更に優れた機械強度を発揮できる。
本発明の熱可塑性樹脂シート(1)は、ポリオレフィン樹脂と、ポリアミド樹脂と、相容化剤と、含み、相容化剤が、ポリアミド樹脂に対する反応性基を有する変性エラストマーである熱可塑性樹脂からなることを特徴とする。
本熱可塑性樹脂シートを構成するポリオレフィン樹脂としては、オレフィンの単独重合体、及び/又は、オレフィンの共重合体を用いることができる。
上記オレフィンは特に限定されないが、エチレン、プロピレン及び炭素数4~8のα-オレフィン等が挙げられる。炭素数4~8のα-オレフィンとしては、1-ブテン、3-メチル-1-ブテン、1-ペンテン、3-メチル-1-ペンテン、4-メチル-1-ペンテン、1-ヘキセン、1-オクテン等が挙げられる。これらは1種のみを用いてもよく2種以上を併用してもよい。
具体的には、ポリオレフィン樹脂としては、ポリエチレン樹脂、ポリプロピレン樹脂、ポリ1-ブテン、ポリ1-ヘキセン、ポリ4-メチル-1-ペンテン等が挙げられる。これら重合体は1種のみで用いてもよく、2種以上を併用してもよい。即ち、ポリオレフィン樹脂は上記重合体の混合物であっても良い。
また、プロピレンと他のオレフィンとの共重合体は、ランダム共重合体であってもよく、ブロック共重合体であってもよい。これらのうちでは、後述するS140/S120の値がより大きい熱可塑性樹脂シートを得るという観点からブロック共重合体が好ましい。とりわけ、他のオレフィンがエチレンであるプロピレン・エチレンブロック共重合体であることが好ましい。このプロピレン・エチレンブロック共重合体は、例えば、インパクトコポリマー、ポリプロピレンインパクトコポリマー、ヘテロファジックポリプロピレン、ヘテロファジックブロックポリプロピレン等とも称される。
本熱可塑性樹脂シートを構成するポリアミド樹脂は、アミド結合(-NH-CO-)を介して複数の単量体が重合されてなる重合体である。
ポリアミド樹脂を構成する単量体としては、6-アミノカプロン酸、11-アミノウンデカン酸、12-アミノドデカン酸、パラアミノメチル安息香酸などのアミノ酸、ε-カプロラクタム、ウンデカンラクタム、ω-ラウリルラクタムなどのラクタムなどが挙げられる。これらは1種のみを用いてもよく2種以上を併用してもよい。
植物由来ポリアミド樹脂としては、ポリアミド11(以下、単に「PA11」ともいう)、ポリアミド610(以下、単に「PA610」ともいう)、ポリアミド612(以下、単に「PA612」ともいう)、ポリアミド614(以下、単に「PA614」ともいう)、ポリアミド1010(以下、単に「PA1010」ともいう)、ポリアミド1012(以下、単に「PA1012」ともいう)、ポリアミド10T(以下、単に「PA10T」ともいう)等が挙げられる。これらは1種のみを用いてもよく2種以上を併用してもよい。
本熱可塑性樹脂シートを構成する変性エラストマーは、ポリアミド樹脂に対する反応性基を有するエラストマーである。この変性エラストマーは、ポリオレフィン樹脂に対して親和性を有する成分であることが好ましい。即ち、ポリアミド樹脂とポリオレフィン樹脂とに対する相容化作用を有する成分であることが好ましい。更に換言すれば、ポリアミド樹脂とポリオレフィン樹脂との相容化剤であることが好ましい。
変性エラストマーの変性量は限定されず、変性エラストマーは1分子中に1以上の反応性基を有すればよい。更に、変性エラストマーは1分子中に1以上50以下の反応性基を有することが好ましく、3以上30以下がより好ましく、5以上20以下が特に好ましい。
具体的には、無水マレイン酸、無水イタコン酸、無水コハク酸、無水グルタル酸、無水アジピン酸、無水シトラコン酸、テトラヒドロ無水フタル酸、ブテニル無水コハク酸等の酸無水物、及びマレイン酸、イタコン酸、フマル酸、アクリル酸、メタクリル酸等のカルボン酸が挙げられる。これらは1種のみ用いてもよく2種以上を併用してもよい。これらの化合物のうちでは、酸無水物が好ましく、無水マレイン酸及び無水イタコン酸がより好ましく、無水マレイン酸が特に好ましい。
オレフィンとしては、ポリオレフィン樹脂を構成するオレフィンとして先に例示した各種のオレフィンの1種又は2種以上を用いることができる。このなかでも、オレフィン系熱可塑性エラストマーとしては、エチレンと炭素数3~8のα-オレフィンとの共重合体、及び、プロピレンと炭素数4~8のα-オレフィンとの共重合体が好ましい。
また、プロピレンと炭素数4~8のα-オレフィンとの共重合体としては、プロピレン・1-ブテン共重合体(PBR)、プロピレン・1-ペンテン共重合体、プロピレン・1-オクテン共重合体(POR)等が挙げられる。これらは1種のみを用いてもよく2種以上を併用してもよい。
上記スチレン系化合物としては、例えば、スチレン、α-メチルスチレン、p-メチルスチレン、p-t-ブチルスチレン等のアルキルスチレン、p-メトキシスチレン、ビニルナフタレン等が挙げられる。これらは1種のみを用いてもよく2種以上を併用してもよい。
上記共役ジエン化合物としては、ブタジエン、イソプレン、ピペリレン、メチルペンタジエン、フェニルブタジエン、3,4-ジメチル-1,3-ヘキサジエン、4,5-ジエチル-1,3-オクタジエン等が挙げられる。これらは1種のみを用いてもよく2種以上を併用してもよい。
本熱可塑性樹脂シートには、ポリオレフィン樹脂、ポリアミド樹脂及び変性エラストマー以外に、他の成分を配合できる。他の成分としては、充填剤(補強フィラー)、造核剤、酸化防止剤、熱安定剤、耐候剤、光安定剤、可塑剤、紫外線吸収剤、帯電防止剤、難燃剤、難燃助剤、スリップ剤、アンチブロッキング剤、防曇剤、滑剤、抗菌剤、着色剤(顔料、染料)、分散剤、銅害防止剤、中和剤、気泡防止剤、ウェルド強度改良剤、天然油、合成油、ワックス等が挙げられる。これらは1種のみを用いてもよく2種以上を併用してもよい。
充填剤としては、ガラス成分(ガラス繊維、ガラスビーズ、ガラスフレーク等)、シリカ、無機繊維(ガラス繊維、アルミナ繊維、カーボン繊維)、黒鉛、珪酸化合物(珪酸カルシウム、珪酸アルミニウム、モンモリロナイト、カオリン、タルク、クレー等)、金属酸化物(酸化鉄、酸化チタン、酸化亜鉛、酸化アンチモン、アルミナ等)、リチウム、カルシウム、マグネシウム、亜鉛等の金属の炭酸塩及び硫酸塩、金属(アルミニウム、鉄、銀、銅等)、水酸化物(水酸化アルミニウム、水酸化マグネシウム等)、硫化物(硫酸バリウム等)、炭化物(木炭、竹炭等)、チタン化物(チタン酸カリウム、チタン酸バリウム等)、有機繊維(芳香族ポリエステル繊維、芳香族ポリアミド繊維、フッ素樹脂繊維、ポリイミド繊維、植物性繊維等)、セルロース類(セルロースミクロフィブリル、酢酸セルロース等)などが挙げられる。これらは1種のみを用いてもよく2種以上を併用してもよい。これらは、造核剤としても利用できる。
本熱可塑性樹脂シートの呈する相構造は限定されないが、下記相構造(1)~(3)を取り得る。
相構造(1):ポリオレフィン樹脂を含んだ連続相(A)と、連続相(A)中に分散された、ポリアミド樹脂及び変性エラストマーを含んだ分散相(B)と、を有する相構造(図1参照)。但し、ポリアミド樹脂を含んだ連続相、及び、この連続相中に分散された分散相、を有する他の相構造は共存されない。
相構造(2):ポリアミド樹脂を含んだ連続相と、この連続相中に分散された、ポリオレフィン樹脂を含んだ分散相と、を有する相構造。但し、ポリオレフィン樹脂を含んだ連続相、及び、この連続相中に分散された分散相、を有する他の相構造は共存されない。
相構造(3):ポリオレフィン樹脂を含んだ連続相(A1)と、連続相(A1)中に分散された、ポリアミド樹脂及び変性エラストマーを含んだ分散相(BA1)と、ポリアミド樹脂を含んだ連続相(A2)と、連続相(A2)中に分散された、変性エラストマーを含んだ分散相(BA2)と、を有する相構造(図2参照)。
これらの相構造のなかでは、相構造(1)又は相構造(3)が好ましく、相構造(1)がより好ましい。
尚、相構造(1)において変性エラストマーは、未反応の変性エラストマーであってもよく、ポリアミド樹脂との反応物であってもよく、これらの混合物であってもよい。
尚、相構造(3)において変性エラストマーは、未反応の変性エラストマーであってもよく、ポリアミド樹脂との反応物であってもよく、これらの混合物であってもよい。
更に、相構造(1)において前述の多重相構造を呈する場合、連続相(B1)は、ポリアミド樹脂を含む。ポリアミド樹脂は連続相(B1)の主成分(連続相B1全体に対し、通常70質量%以上であり、100質量%であってもよい)である。また、微分散相(B2)は、変性エラストマーを含む。変性エラストマーは微分散相(B2)の主成分(微分散相B2全体に対し、通常70質量%以上であり、100質量%であってもよい)である。
更に、相構造(3)において前述の多重相構造を呈する場合、連続相(BA11)は、ポリアミド樹脂を含む。ポリアミド樹脂は連続相(BA11)の主成分(連続相BA11全体に対し、通常70質量%以上であり、100質量%であってもよい)である。また、微分散相(BA12)は、変性エラストマーを含む。変性エラストマーは微分散相(BA12)の主成分(微分散相BA12全体に対し、通常70質量%以上であり、100質量%であってもよい)である。
また、連続相(A2)は、ポリアミド樹脂を含む。ポリアミド樹脂は連続相(A2)の主成分(連続相A2全体に対し、通常70質量%以上であり、100質量%であってもよい)である。また、連続相(A2)に対する分散相(BA2)は、変性エラストマーを含む。変性エラストマーは分散相(BA2)の主成分(分散相BA2全体に対し、通常70質量%以上であり、100質量%であってもよい)である。
尚、前述のように、本熱可塑性樹脂シートでは、変性エラストマーが有する反応性基がポリアミド樹脂に対して反応された反応物となることができる。この場合、反応物は、相構造(1)では、例えば、連続相(A)と分散相(B)との界面、及び/又は、連続相(B1)と微分散相(B2)との界面、に存在できる。同様に、相構造(3)では、例えば、連続相(A1)と連続相(A2)との界面、連続相(A1)と分散相(BA1)との界面、連続相(BA11)と微分散相(BA12)との界面、等に存在できる。
この分散相の分散径は、電子顕微鏡を用いて得られる1000倍以上の拡大画像において測定できる。即ち、画像内の所定の領域内から無作為に選択された20個の分散相の各々の最長径を測定し、得られた最長径の平均値を第1平均値とする。そして、画像内の異なる5つの領域において測定された第1平均値の更なる平均値が、分散相の平均分散径(長軸平均分散径)である。
この微分散相の分散径は、電子顕微鏡を用いて得られる1000倍以上の拡大画像において測定できる。即ち、画像内の所定の領域内から無作為に選択された20個の微分散相の各々の最長径を測定し、得られた最長径の平均値を第1平均値とする。そして、画像内の異なる5つの領域において測定された第1平均値の更なる平均値が、微分散相の平均分散径(長軸平均分散径)である。
本熱可塑性樹脂シートにおいて、ポリオレフィン樹脂とポリアミド樹脂と変性エラストマーとの合計を100質量%とした場合に、ポリオレフィン樹脂の割合は、2質量%以上90質量%以下とすることができる。この割合は、5質量%以上85質量%以下が好ましく、更に10質量%以上83質量%以下が好ましく、更に15質量%以上80質量%以下が好ましく、更に20質量%以上78質量%以下が好ましく、更に25質量%以上75質量%以下が好ましく、更に30質量%以上73質量%以下が好ましく、更に35質量%以上70質量%以下が好ましい。上記範囲では、S140/S120の値がより大きな熱可塑性樹脂シートを得ることができる。
本熱可塑性樹脂シートによれば、温度140℃における破断伸びをS140(%)とし、温度120℃における破断伸びをS120(%)とした場合に、S140をS120の1.2倍以上にすることができる。即ち、S140/S120≧1.2とすることができる。この「S140/S120」は、通常、3.5以下である。「S140/S120」は3.5を超えてもよいが、過度に大きいと、加工に適した温度範囲での伸び率のコントロールが困難となってしまう場合がある。従って、「S140/S120」は、1.2≦S140/S120≦3.5が好ましい。更に、この比は、1.3≦S140/S120≦3.0がより好ましく、1.4≦S140/S120≦2.5が更に好ましく、1.5≦S140/S120≦2.0が特に好ましい。
この点、ポリオレフィン樹脂の重合度を大きくしたり、重合度の小さいポリオレフィン樹脂と重合度の大きいポリオレフィン樹脂とを混合したりすることで、加温時の硬さを増すことが可能である。しかしながら、重合度は製品性能を左右するために、成形のし易さを基準として、ポリオレフィンの重合度を選択できない場合も多い。このような問題から、ポリオレフィンを加圧成形する場合、加熱状態においてポリオレフィンを補助するために補助シートが利用される。従来、この補助シートとしては、例えば、2層のポリオレフィンフィルム間にナイロンフィルムを挟んで一体化させた積層フィルム等が利用される。しかしながら、ナイロンフィルムは、ポリオレフィンの加工温度では十分に軟化されないため、絞り加工(平板状の材料に凹凸形状を付与する深絞り等、図4及び図5参照)を施そうとすると、補助シートの伸びが不十分であることが問題となる場合がある。即ち、従来知られている補助シートでは、ポリオレフィンの加工温度で適度な伸びを得ることが困難である。また、ポリオレフィンとナイロンとは接合させ難い材料であり、3層の原料フィルム費とともに、3層を一体化させるコストが必要となり、補助シート自体のコスト増に繋がるという問題がある。
本熱可塑性樹脂シートの厚さは特に限定されず、必要に応じた適宜の厚さとすることができる。本熱可塑性樹脂シートは、熱可塑性樹脂フィルムと称することもできる。具体的な厚さとしては、例えば、0.01μm以上5000μm以下の範囲とすることができる。更に、本熱可塑性樹脂シートを単独で利用する場合(例えば、本熱可塑性樹脂シート自体を賦形して基材として利用する場合、透光性のフィルムとして利用する場合等)には、50μm以上4800μm以下が好ましく、100μm以上4500μm以下がより好ましく、500μm以上4200μm以下が特に好ましい。一方、本熱可塑性樹脂シートを成形体の賦形を補助する目的で利用する場合には、0.1μm以上2500μm以下が好ましく、1μm以上1000μm以下がより好ましく、10μm以上500μm以下が特に好ましい。
また、本熱可塑性樹脂シートの目付は特に限定されず、必要に応じた適宜の目付とすることができるが、例えば、1g/m2以上1000g/m2以下とすることができる。とりわけ、成形体の賦形を補助する目的で利用する場合、25g/m2以上800g/m2以下が好ましい。
本熱可塑性樹脂シートを製造する方法は限定されず、従来公知の方法で製造できる。例えば、押出法、コーティング法、キャスト法、プレス法、射出成形法又はインフレーション法等のシート成形方法を利用できる。また、本熱可塑性樹脂シートは、延伸されていてもよく、延伸されていなくてもよい。
尚、ポリアミド樹脂と変性エラストマーとの溶融混練温度は限定されないが、例えば、190℃以上350℃以下とすることができ、200℃以上330℃以下が好ましく、205℃以上310℃以下がより好ましい。また、得られた溶融混練物とポリオレフィン樹脂との溶融混練温度は限定されないが、例えば、190℃以上350℃以下とすることができ、200℃以上300℃以下が好ましく、205℃以上260℃以下がより好ましい。
本発明の積層シート(3)は、ポリオレフィン樹脂を含んだ基層(31)と、
基層(31)の一面に接合された本発明の熱可塑性樹脂シート(1)と、を有する(図3参照)。
また、ポリオレフィン樹脂を含んだ基層31は、その構成材料として、ポリオレフィン樹脂を含有することを意味する。基層31に含まれるポリオレフィン樹脂量は限定されないが、通常、基層31全体を100質量%とした場合に、ポリオレフィン樹脂は50質量%以上含まれる。尚、ポリオレフィン樹脂は、基層31内に均一に含有されてもよく、不均一に含有されてもよい。また、基層31は、ポリオレフィン樹脂のみから構成されてもよい。即ち、基層31全体を100質量%とした場合に、ポリオレフィン樹脂が100質量%含まれてもよい。基層31に含まれるポリオレフィン樹脂については、本熱可塑性樹脂シート1を構成するポリオレフィン樹脂に関する説明をそのまま適用できる。
具体的には、本積層シート3としては、基層31をポリプロピレンシートとし、本熱可塑性樹脂シート1が、ポリオレフィン樹脂としてポリプロピレンを含んだ形態が挙げられる(図3(a)及び図3(b)参照)。
更に、本積層シート3としては、基層31をポリプロピレンシートとし、本熱可塑性樹脂シート1がポリオレフィン樹脂としてポリプロピレンを含み、更に、他層32として、ポリアミド樹脂からなる層を有する形態が挙げられる(図3(b)参照)。
また、基層31の目付は特に限定されず、必要に応じた適宜の目付とすることができるが、例えば、1g/m2以上1000g/m2以下とすることができる。とりわけ、成形体の賦形を補助する目的で利用する場合、25g/m2以上800g/m2以下が好ましい。
本発明の成形体(5)は、ポリオレフィン樹脂を含んだ基体(51)と、
基体(51)の一面に接合された本発明の熱可塑性樹脂シート(1)又は本発明の積層シート(3)と、を有する(図4参照)。
本熱可塑性樹脂シート1及び本積層シート3については、前述の通りである。一方、基体51としては、ポリオレフィン樹脂のみからなる成形体や、ポリオレフィン樹脂をバインダとして含んだ繊維補強成形体が挙げられる。即ち、繊維補強成形体は、補強繊維と、この補強繊維同士を結着しているバインダと、を含み、このバインダとしてポリオレフィン樹脂が利用された成形体である。
表皮層12の構成は限定されず、1層のみからなってもよく、2層以上からなってもよい。2層以上からなる場合、例えば、意匠面を有する表層(例えば、合成皮革や織物等)と、クッション層(表皮52の非意匠面側に配置)と、を備えた積層体を、表皮52とすることができる。
成形体5の製造方法は限定されないが、例えば、基体51として、補強繊維とこれを結着するバインダがポリオレフィン樹脂である基体を利用する場合には、下記方法で製造できる。即ち、補強繊維とポリオレフィン樹脂とを含んで圧縮された繊維補強ボード51を加熱し、ポリオレフィン樹脂を軟化させる加熱工程(PR1)と、ポリオレフィン樹脂が軟化された繊維補強ボード51を賦形する賦形工程(PR2)と、により製造できる。
また、表皮52を備える成形体5の場合には、賦形工程(PR2)とともに、又は、賦形工程(PR2)後に、繊維補強ボード51の一面側に表皮52を接合することができる。
[1]熱可塑性樹脂シートの作製
(1)実験例1の熱可塑性樹脂シート
下記ポリアミド樹脂のペレットと、下記変性エラストマーのペレットとをドライブレンドした後、二軸溶融混練押出機に投入し、混練温度210℃で溶融混練を行い、ペレタイザーを介して、ポリアミド樹脂及び変性エラストマーの溶融混練物からなるペレットを得た。更に、上記ペレット(ポリアミド樹脂及び変性エラストマーの溶融混練物からなるペレット)と、下記ポリオレフィン樹脂のペレットと、をドライブレンドした後、二軸溶融混練押出機に投入し、混練温度210℃で溶融混練を行い、Tダイ押出機を介して、目付300g/m2の熱可塑性樹脂組成物製のシート(実験例1)を得た。
尚、ポリオレフィン樹脂とポリアミド樹脂と変性エラストマーとの配合割合は、質量比で、55:25:20とした。この質量比の熱可塑性樹脂組成物は、相構造(1)(図1参照)を呈する。
・ポリオレフィン樹脂:ポリプロピレン樹脂、ホモポリマー、日本ポリプロ株式会社製、品名「ノバテック MA1B」、重量平均分子量312,000、融点165℃)
・ポリアミド樹脂:ナイロン11樹脂、アルケマ株式会社製、品名「Rilsan BMN O」、重量平均分子量18,000、融点190℃
・変性エラストマー:無水マレイン酸変性エチレン・ブテン共重合体(変性EBR)、三井化学株式会社製、品名「タフマー MH7020」
ポリオレフィン樹脂とポリアミド樹脂と変性エラストマーとの配合割合を、質量比で、32.5:42.5:25とした以外は、上記(1)と同様にして、目付300g/m2の熱可塑性樹脂組成物製のシート(実験例2)を得た。この質量比の熱可塑性樹脂組成物は、相構造(3)(図2参照)を呈する。
Tダイ押出機を用いて、下記ポリオレフィン樹脂を目付300g/m2のシートに成形した。
・ポリオレフィン樹脂:ポリプロピレン樹脂、ブロックポリマー、株式会社プライムポリマー製、品名「J-452HP」、融点165℃
Tダイ押出機を用いて、下記ポリアミド樹脂を目付300g/m2のシートに成形した。
・ポリアミド樹脂:ナイロン6樹脂、東レ株式会社製、品名「アミランCM1021FS」、融点225℃
上記[1]で得られた実験例1~4の各熱可塑性樹脂シートを6mm×35mmの短冊状に裁断して、評価用の試験片を得た。
次いで、チャック間距離を20mm(初期値T0)とした引張試験機(インストロン型)に、上記の試験片をセットし、温度80℃で2分間保持した後、温度80℃において試験片が破断するまで、引張速度50mm/分で引張試験を行った。そして、破断点におけるチャック間距離をT(mm)とし、T(mm)/20(mm)×100により算出される値を破断伸び(%)とした。同様にして、温度100℃、温度120℃、温度140℃において、各試験片の破断伸びを計測した。この結果を、表1に表として、図6にグラフ(横軸:試験温度/縦軸:破断伸び)として示した。尚、実験例3では、120℃及び140℃の測定において測定上限に達した。また、このことから実験例3のS140/S120は、実際には1を超えると考えられる。
図6の結果より、実験例4(PA6)は、温度120~140℃の間で、破断伸びがほとんど変化していない。即ち、実施例4の熱可塑性樹脂シートをポリプロピレン樹脂の加圧成形時に同時賦形しようとしても、実験例4のシートは、この間の温度域において伸びをコントロールすることができない。また、ポリプロピレンの加圧成形温度域では、ポリプロピレンの伸びに対して実験例4のシートの伸びが非常に小さいために、両者を同時賦形しつつ深絞りを行うことが困難であることが分かる。また、実験例2の熱可塑性樹脂シートは、全温度域にわたって実験例4のシートよりも高い破断伸びを示している。しかしながら、依然として、ポリプロピレンの加圧成形温度域では、ポリプロピレンの伸びに対して実験例2のシートの伸びが非常に小さいために、両者を同時賦形しつつ深絞りを行うことが困難であることが分かる。
これに対して、実験例1の熱可塑性樹脂シートは、温度120~140℃の間で、ポリプレピレン(実験例3)と同様に破断伸びが非常に大きく変化していることが分かる。具体的には、S140/S120=1.68である。しかしながら、実験例3のシートよりは、どの温度域においても、破断伸びが小さく収まっている。このため、実験例1のシートは、この間の温度域において伸びをコントロールし易いことが分かる。また、ポリプロピレンの加圧成形温度域で、ポリプロピレンの伸びに対して実験例1のシートの伸びが適度に小さいために、両者を同時賦形しつつ深絞りを行うことができることが分かる。
3;積層シート、31;基層(ポリオレフィン樹脂を含んだ基層)、
5;成形体、51;基体(ポリオレフィン樹脂を含んだ基体、又は、その前駆体)、52;表皮、55;深絞り部、
91;ホットプレス機、92;コールドプレス機、
A;連続相、
B;分散相、
B1;連続相(分散相B内の連続相)、
B2;微分散相(分散相B内の分散相)、
A1、A2;連続相、
BA1、BA2;分散相、
BA11;連続相(分散相BA1内の連続相)、
BA12;微分散相(分散相BA1内の分散相)、
PR1;加熱工程、PR2;賦形工程。
Claims (10)
- ポリオレフィン樹脂と、ポリアミド樹脂と、相容化剤と、含み、
前記相容化剤が、前記ポリアミド樹脂に対する反応性基を有する変性エラストマーである熱可塑性樹脂からなることを特徴とする熱可塑性樹脂シート。 - 前記ポリオレフィン樹脂を含んだ連続相(A)と、
前記連続相(A)中に分散された分散相であって、前記ポリアミド樹脂及び前記変性エラストマーを含んだ分散相(B)と、を有する請求項1に記載の熱可塑性樹脂シート。 - 前記分散相(B)が、前記ポリアミド樹脂を含んだ連続相(B1)と、
前記連続相(B1)中に分散された前記変性エラストマーを含んだ微分散相(B2)と、を有する請求項2に記載の熱可塑性樹脂シート。 - 前記ポリアミド樹脂及び前記変性エラストマーの溶融混練物と、前記ポリオレフィン樹脂と、の溶融混練物である請求項1乃至3のうちのいずれかに記載の熱可塑性樹脂シート。
- 前記ポリアミド樹脂が、主鎖中の隣り合ったアミド結合同士に挟まれた炭化水素基の直鎖炭素数が6以上である構造を有する請求項1乃至4のうちのいずれかに記載の熱可塑性樹脂シート。
- 前記変性エラストマーは、エチレン若しくはプロピレンと炭素数3~8のα-オレフィンとの共重合体を骨格としたオレフィン系熱可塑性エラストマー、又は、スチレン骨格を有するスチレン系熱可塑性エラストマーである請求項1乃至5のうちのいずれかに記載の熱可塑性樹脂シート。
- 温度140℃における破断伸びをS140(%)とし、温度120℃における破断伸びをS120(%)とした場合に、S140がS120の1.2倍以上である請求項1乃至6のうちのいずれかに記載の熱可塑性樹脂シート。
- ポリオレフィン樹脂を含んだ基層と、
前記基層の一面に接合された請求項1乃至7のうちのいずれかに記載の熱可塑性樹脂シートと、を有することを特徴とする積層シート。 - ポリオレフィン樹脂を含んだ基体と、
前記基体の一面に接合された請求項1乃至7のうちのいずれかに記載の熱可塑性樹脂シート、又は、請求項8に記載の積層シートと、を有することを特徴とする成形体。 - 前記基体は、補強繊維と、前記補強繊維同士を結着しているバインダと、を含み、
前記バインダは、前記ポリオレフィン樹脂である請求項9に記載の成形体。
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CN110392714B (zh) | 2021-03-12 |
CN110392714A (zh) | 2019-10-29 |
BR112019015862A2 (pt) | 2020-04-14 |
EP3597699A4 (en) | 2020-12-23 |
RU2742377C1 (ru) | 2021-02-05 |
JP6525122B2 (ja) | 2019-06-05 |
KR20190109557A (ko) | 2019-09-25 |
SG11201907705VA (en) | 2019-09-27 |
US11326031B2 (en) | 2022-05-10 |
EP3597699A1 (en) | 2020-01-22 |
JPWO2018168720A1 (ja) | 2019-06-27 |
US20200032018A1 (en) | 2020-01-30 |
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