Propylene α-olefin copolymer, resin composition, molded body, and power storage device

Abstract

A propylene α-olefin copolymer according to an embodiment has a constitutional unit (i) derived from propylene and a constitutional unit (ii) derived from C5-20 α-olefin, and satisfies the following requirements (A1) and (A2): (A1) the content of the constitutional unit (i) is 70-99 mol% and the content of the constitutional unit (ii) is 1-30 mol%, with the total content of the constitutional unit (i) and the constitutional unit (ii) being 100 mol%; and (A2) the melting point (Tm) as measured by differential scanning calorimetry (DSC) is less than 130°C or is not observable.

Description

Propylene-α-olefin copolymer, resin composition, molded article and electricity storage device CROSS-REFERENCE TO RELATED APPLICATIONS

[0001] This application claims priority based on Japanese Patent Application No. 2023-213227 filed on December 18, 2023, and Japanese Patent Application No. 2024-021910 filed on February 16, 2024, the entire disclosures of which are incorporated herein by reference.

[0002] The present disclosure relates to a propylene-α-olefin copolymer, a resin composition, a molded article, and an electricity storage device.

[0003] In recent years, propylene-α-olefin copolymers containing structural units derived from propylene as a main component, and resin compositions containing propylene-α-olefin copolymers have become known as soft materials made of polyolefins that are excellent in flexibility, heat resistance, and transparency, as well as environmental friendliness and hygienic properties (see, for example, Patent Documents 1, 2, and 3).

[0004] JP 2013-049863 A JP 11-193309 A JP 2000-7731 A

[0005] While the applications of propylene-based copolymers are expanding, the performance of currently used propylene-α-olefin copolymers or resin compositions containing propylene-α-olefin copolymers has sometimes been insufficient, for example, in terms of the balance between flexibility and tensile strength.

[0006] The present disclosure aims to provide a propylene-α-olefin copolymer having an excellent balance between flexibility and tensile strength, a resin composition containing the copolymer, a molded article having an excellent balance between flexibility and tensile strength, and an electricity storage device including the molded article.

[0007] The present disclosure relates to, for example, the following items [1] to

[21] . [1] A propylene-α-olefin copolymer (A) having a structural unit (i) derived from propylene and a structural unit (ii) derived from an α-olefin having 5 to 20 carbon atoms, and satisfying the following requirements (A1) and (A2): (A1) When the total content of the structural unit (i) and the structural unit (ii) is taken as 100 mol %, the content of the structural unit (i) is 70 to 99 mol %, and the content of the structural unit (ii) is 1 to 30 mol %; (A2) The melting point (Tm) measured by differential scanning calorimetry (DSC) is less than 130°C or is not observed. [2] The propylene-α-olefin copolymer (A) according to item [1] above, wherein the α-olefin having 5 to 20 carbon atoms is 4-methyl-1-pentene. [3] Density measured at 25 ° C. in accordance with ASTM D1505 is 855 to 875 kg / m 3 [4] The propylene / α-olefin copolymer (A) according to any one of [1] to [3] above, having a glass transition temperature (Tg) of -12 to -3°C. [5] The propylene / α-olefin copolymer (A) according to any one of [1] to [4] above, having a melting point (Tm) of less than 110°C or not observed at all. [6] The propylene / α-olefin copolymer (A) according to any one of [1] to [5] above, having an intrinsic viscosity [η] in decalin solvent at 135°C of 1.8 to 2.5 dl / g. [7] The propylene-α-olefin copolymer (A) according to any one of [1] to [6], wherein the ratio (Mw / Mn) of the weight average molecular weight (Mw) and the number average molecular weight (Mn) calculated in terms of polystyrene, as measured by gel permeation chromatography (GPC), is 1.7 to 2.5.

[0008] [8] A resin composition containing the propylene / α-olefin copolymer (A) according to any one of [1] to [7] above, and a propylene-based polymer (B) satisfying the following requirements (B1) and (B2): (B1) the MFR measured in accordance with ASTM D1238E at 230°C under a load of 2.16 kg is 0.1 to 500 g / 10 min; (B2) the melting point (Tm) measured by differential scanning calorimetry (DSC) is 110°C to 170°C. [9] The resin composition according to [8] above, wherein the α-olefin having 5 to 20 carbon atoms in the propylene / α-olefin copolymer (A) is 4-methyl-1-pentene.

[10] The resin composition according to [8] or [9], wherein the content of the copolymer (A) is 8 to 90% by mass and the content of the polymer (B) is 10 to 92% by mass, where the total content of the copolymer (A) and the polymer (B) is 100% by mass.

[11] The resin composition according to any one of [8] to

[10] , wherein the propylene-based polymer (B) comprises a random polypropylene or a block polypropylene.

[12] The resin composition according to any one of [8] to

[11] , further comprising an ethylene-based polymer (C).

[13] The resin composition according to any one of

[10] to

[12] , wherein the α-olefin having 5 to 20 carbon atoms in the propylene-α-olefin copolymer (A) is 4-methyl-1-pentene.

[14] The resin composition according to

[12] or

[13] , wherein the propylene-based polymer (B) comprises a random polypropylene or a block polypropylene.

[15] The resin composition according to any one of the above items

[12] to

[14] , wherein the ethylene polymer (C) comprises a high-pressure low-density polyethylene (c1) or an ethylene-α-olefin copolymer (c2).

[16] The high-pressure low-density polyethylene (c1) has a density of 900 to 925 kg / m 3The resin composition according to any one of

[12] to

[16] , wherein the ethylene / α-olefin copolymer (c2) has at least structural units derived from ethylene and structural units derived from an α-olefin having 3 to 20 carbon atoms, the content of the structural units derived from ethylene is 80 to 99 mol %, and the content of the structural units derived from the α-olefin having 3 to 20 carbon atoms is 1 to 20 mol %.

[17] The resin composition according to any one of

[12] to

[16] , wherein, when the total content of the copolymer (A), the polymer (B), and the polymer (C) is 100 mass %, the content of the copolymer (A) is 15 to 45 mass %, the content of the polymer (B) is 50 to 80 mass %, and the content of the polymer (C) is 5 to 15 mass %.

[0009]

[18] A molded article comprising the propylene / α-olefin copolymer (A) according to any one of the above [1] to [7], or the resin composition according to any one of the above [8] to

[17] .

[19] The molded article according to the above

[18] , which is a film.

[20] The molded article according to the above

[18] or

[19] , which is a battery packaging material.

[21] An electricity storage device comprising the molded article according to any one of the above

[18] to

[20] .

[0010] The propylene-α-olefin copolymer and resin composition containing the copolymer according to the present disclosure have an excellent balance between flexibility and tensile strength. The molded article according to the present disclosure has an excellent balance between flexibility and tensile strength. The electricity storage device according to the present disclosure includes the molded article.

[0011] In this specification, a numerical range expressed using "to" means a range that includes the numerical values ​​written before and after "to" as the lower and upper limits. A numerical range "A to B" indicates A or more and B or less. In this specification, when the units of the numerical values ​​written before and after "to" that indicate a numerical range are the same, the unit of the numerical value written before "to" may be omitted. For example, "851 kg / m 3 ~900 kg / m 3 " to "851 to 900 kg / m 3". In this specification, when referring to the amount of each component in a composition, if the composition contains multiple substances corresponding to each component, it means the total amount of multiple substances present in the composition, unless otherwise specified. In this specification, a combination of two or more preferred embodiments is a more preferred embodiment. In this specification, unless otherwise specified, each component in the composition or each structural unit in the polymer (resin) may be contained in one type or in two or more types. In this specification, room temperature means 23°C.

[0012] [Propylene / α-olefin copolymer (A)] The propylene / α-olefin copolymer (A) (hereinafter also referred to as "copolymer (A)") of the present disclosure has a structural unit (i) derived from propylene and a structural unit (ii) derived from an α-olefin having 5 to 20 carbon atoms.

[0013] Copolymer (A) satisfies the following requirements (A1) and (A2): (A1) When the total content of structural unit (i) and structural unit (ii) is taken as 100 mol %, the content of structural unit (i) is 70 to 99 mol %, and the content of structural unit (ii) is 1 to 30 mol %. (A2) The melting point (Tm) measured by differential scanning calorimetry (DSC) is less than 130°C or is not observed.

[0014] The copolymer (A) is, for example, a copolymer obtained by using at least propylene and one or more α-olefins having 5 to 20 carbon atoms. The copolymer (A) is preferably a random copolymer.

[0015] The content of the structural unit (i) is 70 to 99 mol%, preferably 75 to 93 mol%, more preferably 80 to 93 mol%, even more preferably 83 to 93 mol%, and particularly preferably 89 to 93 mol%. The content of the structural unit (ii) is 1 to 30 mol%, preferably 7 to 25 mol%, more preferably 7 to 20 mol%, even more preferably 7 to 17 mol%, and particularly preferably 7 to 11 mol%. The contents of the structural unit (i) and the structural unit (ii) are calculated based on the total content of the structural unit (i) and the structural unit (ii) being 100 mol%. The contents of the structural unit (i) and the structural unit (ii) are 13 It can be measured by C-NMR, specifically by the method described in the Examples section.

[0016] Copolymer (A) having the content of the structural unit (i) and the structural unit (ii) in the above range tends to have an excellent balance between flexibility and mechanical strength, and particularly tends to have an excellent balance between flexibility and tensile strength. By using copolymer (A) having the content of the structural unit (i) and the structural unit (ii) in the above range, a resin composition having an excellent balance between heat resistance, tensile strength, and whitening resistance can be obtained.

[0017] Examples of α-olefins having 5 to 20 carbon atoms include 1-pentene, 3-methyl-1-butene, 1-hexene, 4-methyl-1-pentene, 1-heptene, 1-octene, 1-nonene, 1-decene, 1-undecene, 1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene, 1-nonadecene, and 1-eicosene. Among these, 1-hexene, 4-methyl-1-pentene, 1-octene, 1-decene, and 1-dodecene are preferred because they can produce a crystalline structure with many tie molecules and result in a copolymer with a better balance between flexibility and tensile strength, and 4-methyl-1-pentene is more preferred because it results in a copolymer with better tensile strength.

[0018] In producing copolymer (A), at least one α-olefin having 5 to 20 carbon atoms is used, and two or more types may be used, but preferably one α-olefin is used. Copolymer (A) has at least one structural unit (ii) derived from an α-olefin having 5 to 20 carbon atoms, and may have two or more types, but preferably has one structural unit (ii).

[0019] The copolymer (A) may further contain other structural units in addition to the structural unit (i) and the structural unit (ii). Examples of polymerizable monomers that derive other structural units include ethylene, 1-butene, vinyl compounds, vinyl esters, conjugated dienes, and non-conjugated polyenes. The total content of the structural units (i) and (ii) in the copolymer (A) is preferably 80% by mass or more, more preferably 85% by mass or more, even more preferably 90% by mass or more, still more preferably 95% by mass or more, and particularly preferably 98% by mass or more, based on the mass of the copolymer (A).

[0020] The copolymer (A) may have at least one structural unit derived from a biomass-derived monomer. Examples of the biomass-derived monomer include biomass-derived propylene and biomass-derived α-olefins having 5 to 20 carbon atoms. The same type of monomer constituting the copolymer may be only biomass-derived monomers, only fossil fuel-derived monomers, or both biomass-derived monomers and fossil fuel-derived monomers.

[0021] In one embodiment, the density of the copolymer (A) is preferably 851 to 900 kg / m 3 , more preferably 851 to 890 kg / m 3 , more preferably 851 to 880 kg / m 3 , and even more preferably 855 to 875 kg / m 3 , particularly preferably 860 to 875 kg / m 3 The copolymer (A) having a density in the above range has excellent flexibility. In one embodiment, the density of the copolymer (A) is preferably 830 to 900 kg / m 3 , more preferably 840 to 890 kg / m3 , more preferably 850 to 880 kg / m 3 , and even more preferably 855 to 875 kg / m 3 , particularly preferably 860 to 875 kg / m 3 By using the copolymer (A) having a density within the above range, a resin composition having excellent flexibility and excellent whitening resistance can be obtained. The density is measured at 25°C in accordance with ASTM D1505. The density of the copolymer (A) can be adjusted, for example, by the contents of the structural units (i) and (ii).

[0022] In one embodiment, the intrinsic viscosity [η] of the copolymer (A) is preferably 1.6 to 5.0 dl / g, more preferably 1.6 to 4.0 dl / g, and even more preferably 1.8 to 2.5 dl / g. In one embodiment, the intrinsic viscosity [η] of the copolymer (A) is preferably 0.5 to 5.0 dl / g, more preferably 1.0 to 4.0 dl / g, and even more preferably 1.5 to 2.5 dl / g. A copolymer (A) having an intrinsic viscosity [η] within the above range exhibits excellent moldability, mechanical strength, and low stickiness. The intrinsic viscosity [η] is measured at 135°C in decalin solvent.

[0023] The melting point (Tm) of copolymer (A) is less than 130°C or is not observed. Preferably, a melting point is observed. If a melting point is observed, the melting point is preferably 110°C or less, more preferably 90°C or less, and even more preferably 85°C or less. The lower limit is not particularly limited, but it may be 50°C or higher, or even 55°C or higher. If a melting point is observed, the melting point is preferably 50°C or higher but less than 130°C, more preferably 50 to 110°C, even more preferably 50 to 90°C, and particularly preferably 55 to 85°C. Copolymer (A) having a melting point within the above range or no observed melting point has excellent flexibility. By using copolymer (A) having a melting point within the above range or no observed melting point, a resin composition with excellent flexibility and excellent whitening resistance can be obtained. The melting point (Tm) of copolymer (A) can be adjusted, for example, by the content of structural units (i) and (ii).

[0024] The melting point is measured by DSC, specifically by the method described in the Examples section. The melting point refers to the temperature at the apex of the melting peak. "No melting point observed in DSC measurement" means that no melting peak is observed in DSC measurement. "No melting peak observed" means that no crystalline melting peak with a heat of crystalline fusion (ΔH) of 1 J / g or more is observed in the range of -70 to 200°C. When two or more melting peaks are observed, the highest temperature among the apex temperatures of these peaks is the melting point.

[0025] When a melting peak is observed, the heat of fusion (ΔH), which is the integrated value of the melting peak, is preferably 1 to 50 J / g, more preferably 5 to 45 J / g, even more preferably 5 to 40 J / g, still more preferably 10 to 40 J / g, and particularly preferably 10 to 30 J / g. A copolymer (A) having a ΔH in the above range has an excellent balance between flexibility and low stickiness.

[0026] The weight average molecular weight (Mw) of the copolymer (A) is preferably 100,000 to 550,000, more preferably 200,000 to 525,000, and even more preferably 300,000 to 500,000. Copolymer (A) with an Mw in the above range exhibits excellent moldability, mechanical strength, and low stickiness. Mw is a value measured by gel permeation chromatography (GPC) and converted into polystyrene equivalent. Details of the measurement conditions are described in the Examples section.

[0027] The ratio (Mw / Mn) of the weight-average molecular weight (Mw) to the number-average molecular weight (Mn) of the copolymer (A) is preferably 1.0 to 3.5, more preferably 1.4 to 3.0, and even more preferably 1.7 to 2.5. Copolymer (A) having an Mw / Mn in the above range exhibits an excellent balance of mechanical strength, impact resistance, and low stickiness. Mw / Mn is an index indicating molecular weight distribution. Mw and Mn are values ​​measured by gel permeation chromatography (GPC) and converted into polystyrene equivalents. Details of the measurement conditions are described in the Examples section.

[0028] The MFR of the copolymer (A) is preferably 0.1 to 30 g / 10 min, more preferably 0.2 to 15 g / 10 min, and even more preferably 1 to 10 g / 10 min. The copolymer (A) having an MFR in the above range has an excellent balance of moldability, mechanical strength, and low stickiness. The MFR of the copolymer (A) is measured in accordance with ASTM D1238E under conditions of 230°C and a load of 2.16 kg.

[0029] The glass transition temperature (Tg) of the copolymer (A) is preferably −20 to 5° C., more preferably −15 to 0° C., even more preferably −12 to −3° C., and particularly preferably −12 to −7° C. The copolymer (A) having a Tg in the above range has excellent shape conformability. Tg is measured by DSC, specifically by the method described in the Examples section.

[0030] In one embodiment of the copolymer (A), when the total content of the structural unit (i) and the structural unit (ii) is taken as 100 mol %, the content of the structural unit (i) is 75 to 93 mol %, the content of the structural unit (ii) is 7 to 25 mol %, and the density is 851 to 900 kg / m 3 The intrinsic viscosity [η] is 1.6 to 5.0 dl / g, and the melting point (Tm) is less than 110° C. or is not observed.

[0031] In one embodiment of the copolymer (A), when the total content of the structural unit (i) and the structural unit (ii) is taken as 100 mol %, the content of the structural unit (i) is 75 to 93 mol %, the content of the structural unit (ii) is 7 to 25 mol %, and the density is 855 to 875 kg / m 3 the intrinsic viscosity [η] is 1.8 to 2.5 dl / g, the melting point (Tm) is less than 110°C or is not observed, and the glass transition temperature (Tg) is -12 to -3°C.

[0032] The copolymer (A) has a breaking stress of preferably 10 to 40 MPa, more preferably 13 to 37 MPa, and even more preferably 15 to 35 MPa. The copolymer (A) has a tensile modulus of preferably 1 to 250 MPa, more preferably 3 to 230 MPa, and even more preferably 5 to 200 MPa.

[0033] The stress at break and tensile modulus of copolymer (A) are measured using dumbbell test pieces prepared as follows: Copolymer (A) is heated for 5 minutes using a hydraulic hot press set at 190°C, molded for 2 minutes under a pressure of 7.5 MPa, and then cooled at 20°C under a pressure of 7.5 MPa for 5 minutes to produce a 2 mm-thick sheet. After 7 days or more have passed at room temperature since molding, ASTM No. 4 dumbbells are prepared from the sheet in accordance with ASTM D638, and the tensile modulus and stress at break are measured for the dumbbells at 23°C and a pulling rate of 50 mm / min.

[0034] The Shore A hardness (instantaneous value) of the copolymer (A) is preferably 20 to 99, more preferably 25 to 99, even more preferably 28 to 98, still more preferably 30 to 98, particularly preferably 40 to 98, particularly preferably 50 to 98, and particularly preferably 60 to 97. When it is difficult to measure the Shore A hardness, a similar evaluation can be performed using the Shore D hardness instead, and the Shore D hardness (instantaneous value) of the copolymer (A) is preferably 12 to 62, more preferably 16 to 60.

[0035] The Shore A hardness and Shore D hardness of copolymer (A) are values ​​measured on a test piece prepared as follows. Using a hydraulic hot press molding machine set at 190°C, copolymer (A) is heated for 5 minutes, molded under a pressure of 7.5 MPa for 2 minutes, and then cooled at 20°C under a pressure of 7.5 MPa for 5 minutes to prepare a sheet with a thickness of 2 mm. Three sheets are stacked to prepare a test piece. After 7 days or more have passed at room temperature since the molding, a durometer (type A or type D) is used in accordance with ASTM D2240, and the scale is read immediately after the indenter is brought into contact with the test piece. In this way, the Shore A hardness and Shore D hardness are obtained.

[0036] <Method for Producing Copolymer (A)> The copolymer (A) can be suitably produced by a method including a step of polymerizing propylene and at least one olefin selected from α-olefins having 5 to 20 carbon atoms in the presence of an olefin polymerization catalyst described below. By using such an olefin polymerization catalyst and appropriately setting the polymerization conditions within the ranges described below, the copolymer (A) satisfying the above-mentioned requirements can be easily produced.

[0037] The olefin polymerization catalyst is preferably a catalyst containing a bridged metallocene compound (a) and at least one compound (b) selected from the following (b-1) to (b-3): (b-1) an organoaluminum oxy compound, (b-2) an ionic compound that reacts with the bridged metallocene compound (a) to form an ion pair, and (b-3) an organoaluminum compound.

[0038] <Bridged Metallocene Compound (a)> The bridged metallocene compound (a) is preferably a bridged metallocene compound represented by the following formula [a1], and more preferably a bridged metallocene compound represented by the following formula [a2]. One or more bridged metallocene compounds (a) may be used.

[0039]

[0040] The meanings of the symbols in formula [a1] are as follows: M is a Group 4 transition metal, such as a titanium atom, a zirconium atom, or a hafnium atom; j is an integer of 1 to 4; Q is selected from a halogen atom, a hydrocarbon group, a neutral conjugated or non-conjugated diene having 10 or less carbon atoms, an anionic ligand, and a neutral ligand capable of coordinating with a lone electron pair; when j is an integer of 2 to 4, multiple Qs may be the same or different; R A and R B may be the same or different and are mononuclear or polynuclear hydrocarbon residues capable of forming a sandwich structure with M. Y is a carbon atom or a silicon atom. R C and R D may be the same or different and are selected from a hydrogen atom, a hydrocarbon group, a silicon-containing group, a halogen atom and a halogen-containing hydrocarbon group, and may be bonded to each other to form a ring.

[0041]

[0042] The meanings of the symbols in formula [a2] are as follows: 1 is a hydrocarbon group, a silicon-containing group, or a halogen-containing hydrocarbon group. 2 ~R 10 are selected from a hydrogen atom, a hydrocarbon group, a silicon-containing group, a halogen atom, and a halogen-containing hydrocarbon group, and may be the same or different, and the respective substituents may be bonded to each other to form a ring. M is a Group 4 transition metal. j is an integer of 1 to 4. Q is selected from a halogen atom, a hydrocarbon group, a neutral conjugated or non-conjugated diene having 10 or less carbon atoms, an anionic ligand, and a neutral ligand capable of coordinating with a lone electron pair. When j is an integer of 2 to 4, multiple Qs may be the same or different.

[0043] Among the bridged metallocene compounds represented by formula [a2], a bridged metallocene compound represented by the following formula [a3] is particularly preferred in terms of polymerization properties, availability, and the ease with which a propylene / α-olefin copolymer satisfying the above requirements can be obtained.

[0044]

[0045] The meanings of the symbols in formula [a3] are as follows: 1b is a hydrocarbon group, a silicon-containing group, or a halogen-containing hydrocarbon group. 2b ~R 12b are selected from a hydrogen atom, a hydrocarbon group, a silicon-containing group, a halogen atom, and a halogen-containing hydrocarbon group, and may be the same or different, and the respective substituents may be bonded to each other to form a ring. M is a Group 4 transition metal. n is an integer of 1 to 3. j is an integer of 1 to 4. Q is selected from a halogen atom, a hydrocarbon group, a neutral conjugated or non-conjugated diene having 10 or less carbon atoms, an anionic ligand, and a neutral ligand capable of coordinating with a lone electron pair. When j is an integer of 2 to 4, multiple Qs may be the same or different.

[0046] R 1 From R 10 and R 1bFrom R 12b Examples of the hydrocarbon group in include a linear hydrocarbon group, a branched hydrocarbon group, a cyclic saturated hydrocarbon group, a cyclic unsaturated hydrocarbon group, and a group in which one or more hydrogen atoms of a saturated hydrocarbon group are substituted with a cyclic unsaturated hydrocarbon group. The number of carbon atoms in the hydrocarbon group is preferably 1 to 20, more preferably 1 to 15, and even more preferably 1 to 10.

[0047] Examples of the linear hydrocarbon group include linear alkyl groups such as a methyl group, an ethyl group, an n-propyl group, an n-butyl group, an n-pentyl group, an n-hexyl group, an n-heptyl group, an n-octyl group, an n-nonyl group, and an n-decanyl group; and linear alkenyl groups such as an allyl group.

[0048] Examples of branched hydrocarbon groups include branched alkyl groups such as an isopropyl group, a tert-butyl group, a tert-amyl group, a 3-methylpentyl group, a 1,1-diethylpropyl group, a 1,1-dimethylbutyl group, a 1-methyl-1-propylbutyl group, a 1,1-propylbutyl group, a 1,1-dimethyl-2-methylpropyl group, and a 1-methyl-1-isopropyl-2-methylpropyl group.

[0049] Examples of the cyclic saturated hydrocarbon group include cycloalkyl groups such as a cyclopentyl group, a cyclohexyl group, a cycloheptyl group, a cyclooctyl group, and a methylcyclohexyl group; and polycyclic groups such as a norbornyl group, an adamantyl group, and a methyladamantyl group.

[0050] Examples of the cyclic unsaturated hydrocarbon group include aryl groups such as a phenyl group, a tolyl group, a naphthyl group, a biphenyl group, a phenanthryl group, and an anthracenyl group; cycloalkenyl groups such as a cyclohexenyl group; and polycyclic unsaturated alicyclic groups such as a 5-bicyclo[2.2.1]hept-2-enyl group.

[0051] Examples of the group in which one or more hydrogen atoms of a saturated hydrocarbon group are substituted with a cyclic unsaturated hydrocarbon group include groups in which one or more hydrogen atoms of an alkyl group are substituted with an aryl group, such as a benzyl group, a cumyl group, a 1,1-diphenylethyl group, and a triphenylmethyl group.

[0052] R 1 From R 10 and R 1b From R 12b Examples of the silicon-containing group in the formula include groups represented by the formula -SiR3 (wherein the multiple Rs are each independently an alkyl group or a phenyl group having 1 to 15 carbon atoms), such as a trimethylsilyl group, a triethylsilyl group, a dimethylphenylsilyl group, a diphenylmethylsilyl group, and a triphenylsilyl group.

[0053] R 1 From R 10 and R 1b From R 12b Examples of the halogen-containing hydrocarbon group in the above formula include groups in which one or more hydrogen atoms of the hydrocarbon group are substituted with halogen atoms, such as a trifluoromethyl group.

[0054] R 2 From R 10 and R 2b From R 12b Examples of the halogen atom in include a fluorine atom, a chlorine atom, a bromine atom, and an iodine atom.

[0055] R 2 From R 10 and R 2b From R 12b Among the substituents up to 2 and R 3 , R 3 and R 4 , R 5 and R 6 , R 6 and R 7 , R 8 and R 9 , R 9 and R 10 , R 2b and R3b , R 3b and R 4b , R 5b and R 6b , R 6b and R 7b , R 8b and R 9b , R 9b and R 10b , R 10b and R 11b , R 11b and R 12b ) may be bonded to each other to form a ring, and the ring formation may occur at two or more positions in the molecule.

[0056] In this specification, examples of rings formed by bonding two substituents together (spiro rings, additional rings) include alicyclic rings and aromatic rings. Specific examples include a cyclohexane ring, a benzene ring, a hydrogenated benzene ring, and a cyclopentene ring, with a cyclohexane ring, a benzene ring, and a hydrogenated benzene ring being preferred. Furthermore, such ring structures may further have a substituent such as an alkyl group on the ring.

[0057] R 1 and R 1b is preferably a hydrocarbon group, more preferably a hydrocarbon group having 1 to 20 carbon atoms, still more preferably not an aryl group, particularly preferably a linear hydrocarbon group, a branched hydrocarbon group, or a cyclic saturated hydrocarbon group, and particularly preferably a group in which the carbon having a free valence (the carbon bonded to the cyclopentadienyl ring) is a tertiary carbon.

[0058] R 1 and R 1b Specific examples of R include a methyl group, an ethyl group, an isopropyl group, a tert-butyl group, a tert-pentyl group, a tert-amyl group, a 1-methylcyclohexyl group, and a 1-adamantyl group. 1 and R 1bis more preferably a substituent in which the carbon having a free valence is a tertiary carbon, such as a tert-butyl group, a tert-pentyl group, a 1-methylcyclohexyl group, or a 1-adamantyl group, and particularly preferably a tert-butyl group or a 1-adamantyl group.

[0059] R 8 In one embodiment, R is preferably a hydrocarbon group, more preferably a hydrocarbon group having 1 to 20 carbon atoms, and even more preferably an ethyl group. 8 is R 9 may be bonded to form a ring.

[0060] In the formula [a2] and the formula [a3], the fluorene ring portion is not particularly limited as long as it has a structure obtained from a known fluorene or fluorene derivative. 4 and R 5 is preferably a hydrogen atom from the viewpoint of stereoregularity and molecular weight. 4b and R 5b is preferably a hydrogen atom from the viewpoints of stereoregularity and molecular weight.

[0061] R 2 , R 3 , R 6 and R 7 are preferably hydrogen atoms or hydrocarbon groups, more preferably at least two of them are hydrocarbon groups, and even more preferably at least two of them are hydrocarbon groups having 1 to 20 carbon atoms. 2 and R 3 are bonded to each other to form a ring, and R 6 and R 7 may be bonded to each other to form a ring.

[0062] R 2b , R 3b , R 6b and R 7b are preferably hydrogen atoms or hydrocarbon groups, more preferably at least two of them are hydrocarbon groups, and even more preferably at least two of them are hydrocarbon groups having 1 to 20 carbon atoms. 2b and R 3bare bonded to each other to form a ring, and R 6b and R 7b may be bonded to each other to form a ring.

[0063] Examples of such substituted fluorenyl groups include a benzofluorenyl group, a dibenzofluorenyl group, an octahydrodibenzofluorenyl group, a 1,1,4,4,7,7,10,10-octamethyl-2,3,4,7,8,9,10,12-octahydro-1H-dibenzo[b,h]fluorenyl group, a 1,1,3,3,6,6,8,8-octamethyl-2,3,6,7,8,10 1,1,4,4,7,7,10,10-octamethyl-2,3,4,7,8,9,10,12-octahydro-1H-dibenzo[b,h]fluorenyl group, and 1',1',3',6',8',8'-hexamethyl-1'H,8'H-dicyclopenta[b,h]fluorenyl group are particularly preferred.

[0064] R 9 and R 10 In one embodiment, R is preferably a hydrocarbon group, and particularly preferably an aryl group. 9 is R 8 may be bonded to form a ring, in which case R 10 is preferably a hydrocarbon group, and particularly preferably an alkyl group.

[0065] R 8b is preferably a hydrogen atom or a hydrocarbon group, more preferably a hydrogen atom or a hydrocarbon group having 1 to 20 carbon atoms, and even more preferably a hydrogen atom or a methyl group.

[0066] R 9b is more preferably a hydrocarbon group, further preferably an alkyl group having one or more carbon atoms such as a linear alkyl group or a branched alkyl group, a cycloalkyl group or a cycloalkenyl group, and particularly preferably an alkyl group having one or more carbon atoms.

[0067] From a synthetic point of view, R 10b and R 11bis also preferably a hydrogen atom. Or, when n=1, R 9b and R 10b are more preferably bonded to each other to form a ring, and the ring is particularly preferably a six-membered ring such as a cyclohexane ring. 11b is preferably a hydrogen atom. 12b is preferably a hydrocarbon group, and particularly preferably an alkyl group.

[0068] M is a Group 4 transition metal, for example, Ti, Zr or Hf, preferably Zr or Hf, and particularly preferably Zr.

[0069] Q represents a halogen atom, a hydrocarbon group, a neutral conjugated or non-conjugated diene having 10 or less carbon atoms, an anionic ligand, or a neutral ligand capable of coordinating with a lone electron pair. Examples of the halogen atom in Q include fluorine, chlorine, bromine, and iodine.

[0070] The hydrocarbon group for Q is preferably an alkyl group having 1 to 10 carbon atoms, or a cycloalkyl group having 3 to 10 carbon atoms. Examples of the alkyl group having 1 to 10 carbon atoms include a methyl group, an ethyl group, an n-propyl group, an isopropyl group, a 2-methylpropyl group, a 1,1-dimethylpropyl group, a 2,2-dimethylpropyl group, a 1,1-diethylpropyl group, a 1-ethyl-1-methylpropyl group, a 1,1,2,2-tetramethylpropyl group, a sec-butyl group, a tert-butyl group, a 1,1-dimethylbutyl group, a 1,1,3-trimethylbutyl group, and a neopentyl group. Examples of the cycloalkyl group having 3 to 10 carbon atoms include a cyclohexylmethyl group, a cyclohexyl group, and a 1-methyl-1-cyclohexyl group. It is more preferable that the hydrocarbon group have 5 or fewer carbon atoms.

[0071] Examples of neutral conjugated or non-conjugated dienes having 10 or less carbon atoms include s-cis- or s-trans-η 4 -1,3-butadiene, s-cis- or s-trans-η 4 -1,4-diphenyl-1,3-butadiene, s-cis- or s-trans-η 4-3-methyl-1,3-pentadiene, s-cis- or s-trans-η 4 -1,4-dibenzyl-1,3-butadiene, s-cis- or s-trans-η 4 -2,4-hexadiene, s-cis- or s-trans-η 4 -1,3-pentadiene, s-cis- or s-trans-η 4 -1,4-ditolyl-1,3-butadiene, s-cis- or s-trans-η 4 and 1,4-bis(trimethylsilyl)-1,3-butadiene.

[0072] Examples of anionic ligands include alkoxy groups such as methoxy and tert-butoxy; aryloxy groups such as phenoxy; carboxylate groups such as acetate and benzoate; and sulfonate groups such as mesylate and tosylate.

[0073] Examples of neutral ligands capable of coordinating with lone electron pairs include organic phosphorus compounds such as trimethylphosphine, triethylphosphine, triphenylphosphine, and diphenylmethylphosphine; and ethers such as tetrahydrofuran (THF), diethyl ether, dioxane, and 1,2-dimethoxyethane.

[0074] A preferred embodiment of Q is a halogen atom or an alkyl group having 1 to 5 carbon atoms.

[0075] n is an integer of 1 to 3, preferably 1 or 2, and more preferably 1. When n is within the above range, the propylene / α-olefin copolymer can be efficiently obtained, which is preferable. j is an integer of 1 to 4, and preferably 2.

[0076] The above describes the structure of the bridged metallocene compound represented by formula [a2] or formula [a3], i.e., R 1 ~R 10 , R 1b ~R 12bPreferred embodiments of M, n, Q, and j have been described above. Any combination of the preferred embodiments of the bridged metallocene compound (a) is also a preferred embodiment. Such a bridged metallocene compound can be suitably used to obtain the copolymer (A) having the above-described physical properties.

[0077] An example of the bridged metallocene compound represented by the formula [a2] is diphenylmethylene(3-tert-butyl-5-ethylcyclopentadienyl)(2,7-di-tert-butylfluorenyl)zirconium dichloride.

[0078] Examples of the bridged metallocene compound represented by formula [a3] include (8-octamethylfluoren-12'-yl-(2-(adamantan-1-yl)-8-methyl-3,3b,4,5,6,7,7a,8-octahydrocyclopenta[a]indene))zirconium dichloride and catalyst (b) described in Japanese Patent No. 6568082. Here, the octamethylfluorene refers to 1,1,4,4,7,7,10,10-octamethyl-2,3,4,7,8,9,10,12-octahydro-1H-dibenzo[b,h]fluorene.

[0079] Other examples of the bridged metallocene compound represented by the formula [a1] include R A and R B may be the same or different, are a substituted indenyl group, and Y is a silicon atom. Examples of the substituent in the substituted indenyl group include a halogen atom, a hydrocarbon group, a silicon-containing group, and a halogen-containing hydrocarbon group. Specific examples of these include R in the formula [a2] and formula [a3]. 1 and R 2 and the like. C , R D and MQ j The R moiety is as described in the formula [a2] and formula [a3] sections. 9 , R 10 and MQ jExamples of such bridged metallocene compounds include dimethylsilylene-bis{1-(2-n-propyl-4-phenanthryl indenyl)}zirconium dichloride and dimethylsilylene-bis{1-(2-n-propyl-4-phenanthryl indenyl)}hafnium dichloride.

[0080] <Compound (b)> The compound (b) is at least one compound selected from an organoaluminum oxy-compound (b-1), an ionic compound (b-2) that reacts with the bridged metallocene compound (a) to form an ion pair, and an organoaluminum compound (b-3).

[0081] (Organoaluminum oxy compound (b-1)) Examples of the organoaluminum oxy compound (b-1) include conventionally known aluminoxanes such as compounds represented by the following formula [b1] and compounds represented by the following formula [b2], modified methylaluminoxanes having a structure represented by the following formula [b3], and boron-containing organoaluminum oxy compounds represented by the following formula [b4]. One or more types of organoaluminum oxy compound (b-1) may be used.

[0082]

[0083] In formula [b1] and formula [b2], R is a hydrocarbon group having 1 to 10 carbon atoms, preferably a methyl group, and multiple Rs may be the same or different, and n is an integer of 2 or greater, preferably 3 or greater, and more preferably 10 or greater. In formula [b1] and formula [b2], methylaluminoxane in which R is a methyl group is preferably used.

[0084]

[0085] In formula [b3], Me is a methyl group, R is a hydrocarbon group having 2 to 10 carbon atoms, and m and n are each independently an integer of 2 or greater. Multiple Rs may be the same or different. Modified methylaluminoxane [b3] can be prepared using trimethylaluminum and an alkylaluminum other than trimethylaluminum. Such modified methylaluminoxane [b3] is generally called MMAO (modified methyl aluminoxane). MMAO can be prepared, for example, by the methods described in U.S. Pat. Nos. 4,960,878 and 5,041,584.

[0086] Modified methylaluminoxanes prepared using trimethylaluminum and triisobutylaluminum (i.e., R is an isobutyl group in formula [b3]) are commercially produced by Tosoh Finechem Corporation and other companies under the trade names MMAO and TMAO.

[0087] MMAO is an aluminoxane with improved solubility in various solvents and improved storage stability. Specifically, unlike compounds that are insoluble or poorly soluble in benzene, such as the compounds represented by formula [b1] or [b2], MMAO is soluble in aliphatic hydrocarbons, alicyclic hydrocarbons, aromatic hydrocarbons, and the like.

[0088]

[0089] In formula [b4], R c is a hydrocarbon group having 1 to 10 carbon atoms, and there are multiple R d are each independently a hydrogen atom, a halogen atom, or a hydrocarbon group having 1 to 10 carbon atoms. In a production method using an olefin polymerization catalyst, a propylene-α-olefin copolymer can be produced even at high temperatures as described below. Therefore, organoaluminum oxy compounds that are insoluble or slightly soluble in benzene, such as those exemplified in JP-A No. 2-78687, can also be used. Organoaluminum oxy compounds described in JP-A No. 2-167305 and aluminoxanes having two or more alkyl groups, such as those described in JP-A No. 3-103407, can also be suitably used.

[0090] The "benzene-insoluble or sparingly soluble" organoaluminum oxy-compound refers to an organoaluminum oxy-compound that is insoluble or sparingly soluble in benzene, and in which the amount of the compound that dissolves in benzene at 60°C is usually 10% by mass or less, preferably 5% by mass or less, and particularly preferably 2% by mass or less, calculated as Al atoms.

[0091] (Ionic Compound (b-2)) Examples of the compound (b-2) (hereinafter also referred to as "ionic compound (b-2)") that reacts with the bridged metallocene compound (a) to form an ion pair include Lewis acids, ionic compounds, borane compounds, and carborane compounds described in, for example, JP-T-1-501950, JP-T-1-502036, JP-A-3-179005, JP-A-3-179006, JP-A-3-207703, JP-A-3-207704, JP-A-2004-51676, and U.S. Pat. No. 5,321,106. Further examples of the ionic compound (b-2) include heteropoly compounds and isopoly compounds. Among these, compounds represented by the following formula [b5] are preferred. The ionic compound (b-2) may be used alone or in combination of two or more.

[0092]

[0093] In formula [b5], R e+ For example, H + , oxonium cation, carbenium cation, ammonium cation, phosphonium cation, cycloheptyltrienyl cation, and ferrocenium cation with a transition metal. f , R g , R h and R i each independently represents an organic group, preferably an aryl group or a halogen-substituted aryl group.

[0094] Examples of carbenium cations include trisubstituted carbenium cations such as triphenylcarbenium cation, tris(methylphenyl)carbenium cation, and tris(dimethylphenyl)carbenium cation.

[0095] Examples of ammonium cations include trialkylammonium cations such as trimethylammonium cation, triethylammonium cation, tri(n-propyl)ammonium cation, triisopropylammonium cation, tri(n-butyl)ammonium cation, and triisobutylammonium cation; N,N-dialkylanilinium cations such as N,N-dimethylanilinium cation, N,N-diethylanilinium cation, and N,N,2,4,6-pentamethylanilinium cation; and dialkylammonium cations such as diisopropylammonium cation and dicyclohexylammonium cation.

[0096] Examples of the phosphonium cation include triarylphosphonium cations such as triphenylphosphonium cation, tris(methylphenyl)phosphonium cation, and tris(dimethylphenyl)phosphonium cation.

[0097] R e+ Among the above examples, carbenium cations and ammonium cations are preferred, and triphenylcarbenium cation, N,N-dimethylanilinium cation, and N,N-diethylanilinium cation are particularly preferred.

[0098] ・R e+ is a carbenium cation (carbenium salt): Examples of the carbenium salt include triphenylcarbenium tetraphenylborate, triphenylcarbenium tetrakis(pentafluorophenyl)borate, triphenylcarbenium tetrakis(3,5-ditrifluoromethylphenyl)borate, tris(4-methylphenyl)carbenium tetrakis(pentafluorophenyl)borate, and tris(3,5-dimethylphenyl)carbenium tetrakis(pentafluorophenyl)borate.

[0099] ・R e+When is an ammonium cation (ammonium salt): Examples of the ammonium salt include trialkylammonium salts, N,N-dialkylanilinium salts, and dialkylammonium salts.

[0100] Specific examples of the trialkylammonium salt include triethylammonium tetraphenylborate, tripropylammonium tetraphenylborate, tri(n-butyl)ammonium tetraphenylborate, trimethylammonium tetrakis(p-tolyl)borate, trimethylammonium tetrakis(o-tolyl)borate, tri(n-butyl)ammonium tetrakis(pentafluorophenyl)borate, triethylammonium tetrakis(pentafluorophenyl)borate, tripropylammonium tetrakis(pentafluorophenyl)borate, tripropylammonium tetrakis(2,4-dimethylphenyl)borate, tri(n-butyl)ammonium tetrakis(3,5-dimethylphenyl)borate, tri(n-butyl)ammonium tetrakis(4-trifluoromethylphenyl)borate, and tri(n- tri(n-butyl)ammonium tetrakis(o-tolyl)borate, dioctadecylmethylammonium tetraphenylborate, dioctadecylmethylammonium tetrakis(p-tolyl)borate, dioctadecylmethylammonium tetrakis(o-tolyl)borate, dioctadecylmethylammonium tetrakis(pentafluorophenyl)borate, dioctadecylmethylammonium tetrakis(2,4-dimethylphenyl)borate, dioctadecylmethylammonium tetrakis(3,5-dimethylphenyl)borate, dioctadecylmethylammonium tetrakis(4-trifluoromethylphenyl)borate, and dioctadecylmethylammonium tetrakis(3,5-ditrifluoromethylphenyl)borate.

[0101] Specific examples of N,N-dialkylanilinium salts include N,N-dimethylanilinium tetraphenylborate, N,N-dimethylanilinium tetrakis(pentafluorophenyl)borate, N,N-dimethylanilinium tetrakis(3,5-ditrifluoromethylphenyl)borate, N,N-diethylanilinium tetraphenylborate, N,N-diethylanilinium tetrakis(pentafluorophenyl)borate, N,N-diethylanilinium tetrakis(3,5-ditrifluoromethylphenyl)borate, N,N,2,4,6-pentamethylanilinium tetraphenylborate, and N,N,2,4,6-pentamethylanilinium tetrakis(pentafluorophenyl)borate.

[0102] Specific examples of dialkylammonium salts include diisopropylammonium tetrakis(pentafluorophenyl)borate and dicyclohexylammonium tetraphenylborate.

[0103] (Organoaluminum Compound (b-3)) Examples of the organoaluminum compound (b-3) include an organoaluminum compound represented by the following formula [b6] and an alkylated complex of a metal of Group 1 of the periodic table with aluminum represented by the following formula [b7]. One or more types of organoaluminum compound (b-3) may be used.

[0104] R a m Al (OR b ) n H p X q ...[b6] In formula [b6], R a and R b are each independently a hydrocarbon group having 1 to 15 carbon atoms, preferably 1 to 4 carbon atoms, X is a halogen atom, m is a number that satisfies 0<m≦3, n is a number that satisfies 0≦n<3, p is a number that satisfies 0≦p<3, q is a number that satisfies 0≦q<3, and m+n+p+q=3.

[0105] M 2 AlR a 4 ... [b7] In formula [b7], M 2is Li, Na or K, and there are multiple R a are each independently a hydrocarbon group having 1 to 15 carbon atoms, preferably 1 to 4 carbon atoms.

[0106] Examples of the organoaluminum compound [b6] include tri-n-alkylaluminums such as trimethylaluminum, triethylaluminum, tri-n-butylaluminum, trihexylaluminum, and trioctylaluminum; tri-branched alkylaluminums such as triisopropylaluminum, triisobutylaluminum, trisec-butylaluminum, tritert-butylaluminum, tri-2-methylbutylaluminum, tri-3-methylhexylaluminum, and tri-2-ethylhexylaluminum; tricycloalkylaluminums such as tricyclohexylaluminum and tricyclooctylaluminum; triarylaluminums such as triphenylaluminum and tritolylaluminum; and compounds of the formula (i-CH) x Al y (C5H 10 ) z (wherein x, y, and z are positive numbers, and z≦2x); alkylaluminum alkoxides such as isobutylaluminum methoxide and isobutylaluminum ethoxide; dialkylaluminum alkoxides such as dimethylaluminum methoxide, diethylaluminum ethoxide, and dibutylaluminum butoxide; alkylaluminum sesquialkoxides such as ethylaluminum sesquiethoxide and butylaluminum sesquibutoxide; a 2.5 Al (OR b ) 0.5 (In the formula, R a and R b is R in formula [b6] a and R bpartially alkoxylated alkylaluminums having an average composition represented by the formula (I); alkylaluminum aryloxides such as diethylaluminum phenoxide and diethylaluminum (2,6-ditert-butyl-4-methylphenoxide); dialkylaluminum halides such as dimethylaluminum chloride, diethylaluminum chloride, dibutylaluminum chloride, diethylaluminum bromide, and diisobutylaluminum chloride; alkylaluminum sesquihalides such as ethylaluminum sesquichloride, butylaluminum sesquichloride, and ethylaluminum sesquibromide; ethylaluminum dichloride; partially halogenated alkylaluminums such as alkylaluminum dihalides such as aluminum hydride; dialkylaluminum hydrides such as diethylaluminum hydride, dibutylaluminum hydride, diisopropylaluminum hydride, and diisobutylaluminum hydride; partially hydrogenated alkylaluminums such as alkylaluminum dihydrides such as ethylaluminum dihydride and propylaluminum dihydride; and partially alkoxylated and halogenated alkylaluminums such as ethylaluminum ethoxychloride, butylaluminum butoxychloride, and ethylaluminum ethoxybromide.

[0107] Examples of the alkylated complex [b7] include LiAl(C2H5)4 and LiAl(C7H 15 ) 4. Compounds similar to the alkylated complex [b7] can also be used, specifically organoaluminum compounds in which two or more aluminum compounds are bonded via nitrogen atoms. Examples of such compounds include (C2H5)2AlN(C2H5)Al(C2H5)2.

[0108] As the organoaluminum compound (b-3), trimethylaluminum and triisobutylaluminum are preferred because they are readily available.

[0109] <<Carrier (c)>> A carrier (c) may be used as a component of the olefin polymerization catalyst. The carrier (c) is preferably an inorganic or organic compound that is a granular or particulate solid. One type of carrier (c) may be used, or two or more types may be used.

[0110] (Inorganic Compound) Examples of inorganic compounds include porous oxides, inorganic halides, clay minerals, clays (usually composed mainly of clay minerals), and ion-exchange layered compounds (most clay minerals are ion-exchange layered compounds).

[0111] Examples of porous oxides include SiO2, Al2O3, MgO, ZrO, TiO2, BO3, CaO, ZnO, BaO, and ThO2, as well as composites or mixtures containing these oxides. Examples of composites or mixtures include natural or synthetic zeolites, SiO2-MgO, SiO2-Al2O3, SiO2-TiO2, SiO2-VO5, SiO2-Cr2O3, and SiO2-TiO2-MgO. Among these, porous oxides containing either or both of SiO2 and Al2O3 as the main components are preferred.

[0112] The properties of the porous oxide vary depending on the type and manufacturing method, but the particle size is preferably in the range of 10 to 300 μm, more preferably 20 to 200 μm; the specific surface area is preferably 50 to 1000 m 2 / g, more preferably 100 to 700 m 2 / g; the pore volume is preferably in the range of 0.3 to 3.0 cm 3 Such porous oxides are calcined, if necessary, at a temperature of, for example, 100 to 1000°C, preferably 150 to 700°C before use.

[0113] Examples of inorganic halides include MgCl, MgBr, MnCl, and MnBr. The inorganic halides may be used as they are, or may be used after being pulverized using a ball mill, a vibration mill, or the like. It is also possible to dissolve the inorganic halide in a solvent such as alcohol, and then precipitate the resulting component in the form of fine particles using a precipitating agent.

[0114] Clays, clay minerals, and ion-exchangeable layered compounds are not limited to natural products, but may also be synthetically produced. Note that ion-exchangeable layered compounds are compounds having a crystalline structure in which planes formed by ionic bonds or the like are stacked in parallel with each other with weak bonding forces, and the ions contained therein are exchangeable.

[0115] Specific examples of clays and clay minerals include kaolin, bentonite, kibushi clay, gairome clay, allophane, hisingerite, pyrophyllite, synthetic mica and other mica group, montmorillonite group, vermiculite, ryokudeite group, palygorskite, kaolinite, nacrite, dickite, hectorite, taeniolite, and halloysite.

[0116] It is also preferable to subject clay and clay minerals to chemical treatment. Examples of chemical treatments that can be used include surface treatments to remove impurities adhering to the surface and treatments that affect the crystalline structure of the clay. Examples of chemical treatments include acid treatment, alkali treatment, salt treatment, and organic treatment.

[0117] Examples of ion-exchangeable layered compounds include ionic crystalline compounds having a layered crystal structure such as hexagonal close-packed type, antimony type, CdCl2 type, CdI2 type, etc. Specific examples of ion-exchangeable layered compounds include crystalline acid salts of polyvalent metals such as α-Zr(HAsO4)2.H2O, α-Zr(HPO4), α-Zr(KPO4), 3H2O, α-Ti(HPO4), α-Ti(HAsO4)2.H2O, α-Sn(HPO4), H2O, γ-Zr(HPO4), γ-Ti(HPO4), and γ-Ti(NH4PO4)2.H2O.

[0118] Ion-exchangeable layered compounds may be converted into layered compounds with expanded interlayer spacing by utilizing their ion-exchange properties and exchanging the interlayer exchangeable ions with other large, bulky ions. Such bulky ions act as supports supporting the layered structure and are commonly called pillars. For example, oxide supports (pillars) can be formed between layers by intercalating the following metal hydroxide ions between the layers of a layered compound and then dehydrating them by heating. The introduction of another substance between the layers of a layered compound in this manner is called intercalation.

[0119] Examples of the guest compound to be intercalated include cationic inorganic compounds such as TiCl4 and ZrCl4; metal alkoxides such as Ti(OR)4, Zr(OR)4, PO(OR)3, and B(OR)3 (where R is a hydrocarbon group, etc.); 13 O4 (OH) 24 ] 7+ , [Zr(OH) 14 ] 2+ , and [Fe3O(OCOCH3)] + These guest compounds may be used alone or in combination of two or more.

[0120] When intercalating a guest compound, a polymer obtained by hydrolysis and polycondensation of metal alkoxides (R is a hydrocarbon group, etc.) such as Si(OR)4, Al(OR)3, and Ge(OR)4, or a colloidal inorganic compound such as SiO2 may also be present.

[0121] Among the inorganic compounds, clay minerals and clays are preferred, with the montmorillonite group, vermiculite, hectorite, taeniolite and synthetic mica being particularly preferred.

[0122] (Organic Compound) Examples of the organic compound include granular or fine particle solids having a particle size in the range of 10 to 300 μm. Specific examples of the organic compound include polymers synthesized using ethylene and an α-olefin having 3 to 20 carbon atoms as the main components; polymers synthesized using vinylcyclohexane or styrene as the main component; and modified products of these polymers.

[0123] <Organic Compound Component (d)> An organic compound component (d) may be used as a component of the olefin polymerization catalyst. The organic compound component (d) is used, as necessary, for purposes such as improving the polymerization performance in the α-olefin polymerization reaction and the physical properties of the resulting copolymer. Examples of the organic compound component (d) include alcohols, phenolic compounds, carboxylic acids, phosphorus compounds, and sulfonates. One type of organic compound component (d) may be used, or two or more types may be used.

[0124] <<Constitution of Olefin Polymerization Catalyst>> When polymerizing olefins using an olefin polymerization catalyst, the amounts of each component that can constitute the olefin polymerization catalyst are preferably as follows, or are preferably set as follows:

[0125] (1) When olefin polymerization is carried out using an olefin polymerization catalyst, the bridged metallocene compound (a) is used in an amount of usually 10 -9 ~10 -1 moles, preferably 10 -8 ~10 -2 It is used in molar amounts.

[0126] (2) When the organoaluminum oxy compound (b-1) is used as a component of the olefin polymerization catalyst, the compound (b-1) is used in such an amount that the molar ratio [Al / M] of the aluminum atom (Al) in the compound (b-1) to the total transition metal atoms (M) in the bridged metallocene compound (a) is preferably 0.01 to 5,000, more preferably 0.05 to 2,000.

[0127] (3) When the ionic compound (b-2) is used as a component of the olefin polymerization catalyst, the compound (b-2) is used in such an amount that the molar ratio of the compound (b-2) to the total transition metal atoms (M) in the bridged metallocene compound (a), [(b-2) / M], is preferably 1 to 10, more preferably 1 to 5.

[0128] (4) When the organoaluminum compound (b-3) is used as a component of the olefin polymerization catalyst, the compound (b-3) is used in such an amount that the molar ratio of the compound (b-3) to the total transition metal atoms (M) in the bridged metallocene compound (a), [(b-3) / M], is preferably 10 to 5,000, more preferably 20 to 2,000.

[0129] (5) When an organic compound component (d) is used as a component of an olefin polymerization catalyst, when compound (b) is an organoaluminum oxy compound (b-1), the organic compound component (d) is used in an amount such that the molar ratio of the organic compound component (d) to the compound (b-1) [(d) / (b-1)] is preferably 0.01 to 10, more preferably 0.1 to 5; when compound (b) is an ionic compound (b-2), the organic compound component (d) is used in an amount such that the molar ratio of the organic compound component (d) to the compound (b-2) [(d) / (b-2)] is preferably 0.01 to 10, more preferably 0.1 to 5; and when compound (b) is an organoaluminum compound (b-3), the organic compound component (d) is used in an amount such that the molar ratio of the organic compound component (d) to the compound (b-3) [(d) / (b-3)] is preferably 0.01 to 2, more preferably 0.005 to 1.

[0130] <Polymerization Method> In producing the copolymer (A), the polymerization can be carried out by either a liquid phase polymerization method such as solution polymerization or suspension polymerization, or a gas phase polymerization method.

[0131] In the liquid phase polymerization method, it is preferable to use an inert hydrocarbon medium. Examples of the inert hydrocarbon medium include aliphatic hydrocarbons such as propane, butane, pentane, hexane, heptane, octane, decane, dodecane, and kerosene; alicyclic hydrocarbons such as cyclopentane, cyclohexane, and methylcyclopentane; aromatic hydrocarbons such as benzene, toluene, and xylene; and halogenated hydrocarbons such as ethylene chloride, chlorobenzene, and dichloromethane. One or more inert hydrocarbon mediums may be used. A so-called bulk polymerization method can also be used, in which the liquefied olefin to be supplied to the polymerization itself is used as a solvent.

[0132] The polymerization temperature is preferably −50 to +200° C., more preferably 0 to +180° C. The polymerization pressure is preferably normal pressure to 10 MPa gauge pressure, more preferably normal pressure to 5 MPa gauge pressure.

[0133] The polymerization reaction can be carried out in any of batch, semi-continuous, and continuous modes. The polymerization can also be carried out in two or more stages with different reaction conditions. The molecular weight of the resulting copolymer (A) can be adjusted by adding hydrogen or the like to the polymerization system, changing the polymerization temperature, or by adjusting the amount of compound (b) used.

[0134] When producing the copolymer (A), it is possible to produce a copolymer (A) having high stereoregularity while maintaining high catalytic activity even under high-temperature conditions that are advantageous in industrial production. Such high-temperature conditions include conditions in which the polymerization temperature is preferably 40°C or higher, more preferably 40 to 200°C, even more preferably 45 to 150°C, and particularly preferably 50 to 150°C (in other words, a temperature that can be industrially implemented is particularly preferred).

[0135] When producing the copolymer (A), the use of hydrogen in particular is preferable because it can improve the polymerization activity of the catalyst and increase or decrease the molecular weight of the resulting polymer. When hydrogen is added to the polymerization system, the amount of hydrogen is preferably about 0.00001 to 100 NL per mole of olefin. The hydrogen concentration in the polymerization system can be adjusted not only by adjusting the amount of hydrogen supplied, but also by carrying out a reaction that produces or consumes hydrogen within the polymerization system, by separating hydrogen using a membrane, or by releasing a portion of the hydrogen-containing gas outside the system.

[0136] When producing the copolymer (A), after synthesis by the above method, known post-treatment steps such as a catalyst deactivation step, a catalyst residue removal step, and a drying step may be carried out, if necessary.

[0137] [Resin composition] The resin composition of the present disclosure (hereinafter also referred to as "the composition") contains the copolymer (A) of the present disclosure described above. The copolymer (A) contained in the composition may be one type or two or more types. It is preferable that the composition further contains a propylene-based polymer (B) (hereinafter also referred to as "polymer (B)") that satisfies the following requirements (B1) and (B2).

[0138] <Propylene Polymer (B)> The propylene polymer (B) is a polymer other than the copolymer (A), and is not particularly limited as long as it satisfies the following requirements (B1) and (B2): (B1) the melt flow rate (MFR) measured in accordance with ASTM D1238E at 230°C under a load of 2.16 kg is 0.1 to 500 g / 10 min; (B2) the melting point (Tm) measured by differential scanning calorimetry (DSC) is 110°C to 170°C. When the composition contains polymer (B), the polymer (B) may be one type or two or more types.

[0139] The polymer (B) may be, for example, a homopolymer of propylene (homopolypropylene), or a copolymer of propylene and an α-olefin other than propylene having 2 to 20 carbon atoms. The copolymer may be, for example, a random copolymer (random polypropylene) or a block copolymer (block polypropylene). In one embodiment, the polymer (B) is preferably a homopolypropylene or a random polypropylene. In one embodiment, the polymer (B) is preferably a random polypropylene or a block polypropylene. The random polypropylene is, for example, a random copolymer of propylene and an α-olefin other than propylene having 2 to 20 carbon atoms.

[0140] Polymer (B) may have at least one structural unit derived from a biomass-derived monomer. Examples of biomass-derived monomers include biomass-derived ethylene, biomass-derived propylene, and biomass-derived α-olefins having 4 to 20 carbon atoms. The same type of monomers constituting the polymer may be only biomass-derived monomers, only fossil fuel-derived monomers, or both biomass-derived monomers and fossil fuel-derived monomers.

[0141] As the polymer (B), a homopolypropylene is preferred in view of the ease with which a molded article having excellent heat resistance can be obtained, etc. As the polymer (B), a random copolymer is preferred in view of the ease with which a molded article having excellent transparency or impact properties, or a molded article having excellent whitening resistance and impact properties can be obtained, etc.

[0142] As the random copolymer, a copolymer of propylene and an α-olefin having 2 to 10 carbon atoms other than propylene is preferred, and specifically, a copolymer of propylene and ethylene, or a copolymer of propylene, ethylene and an α-olefin having 4 to 10 carbon atoms is preferred.

[0143] The content of structural units derived from propylene in the random copolymer is preferably 90 mol% or more, more preferably 92 mol% or more, even more preferably 92.5 mol% or more, and preferably 99.9 mol% or less, more preferably 99.8 mol% or less, based on 100 mol% of the total of structural units derived from propylene and structural units derived from α-olefins other than propylene having 2 to 20 carbon atoms. The content of structural units derived from α-olefins other than propylene having 2 to 20 carbon atoms in the random copolymer is preferably 10 mol% or less, more preferably 8 mol% or less, even more preferably 7.5 mol% or less, based on 100 mol% of the total of structural units derived from propylene and structural units derived from α-olefins other than propylene having 2 to 20 carbon atoms, and is preferably 0.1 mol% or more, more preferably 0.2 mol% or more. The content of the above structural units is 13 It can be measured by C-NMR.

[0144] Examples of the α-olefins having 2 to 20 carbon atoms other than propylene include ethylene, 1-butene, 1-pentene, 3-methyl-1-butene, 1-hexene, 4-methyl-1-pentene, 1-heptene, 1-octene, 1-nonene, 1-decene, 1-undecene, 1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene, 1-nonadecene, and 1-eicosene. One or more of the α-olefins having 2 to 20 carbon atoms other than propylene may be used.

[0145] The random copolymer may further contain other structural units in addition to the structural units derived from propylene and the structural units derived from an α-olefin having 2 to 20 carbon atoms other than propylene. Examples of polymerizable monomers from which other structural units are derived include vinyl compounds, vinyl esters, conjugated dienes, and non-conjugated polyenes. The total content of the structural units derived from propylene and the structural units derived from an α-olefin having 2 to 20 carbon atoms other than propylene in the random copolymer is preferably 80% by mass or more, more preferably 85% by mass or more, even more preferably 90% by mass or more, still more preferably 95% by mass or more, and particularly preferably 98% by mass or more, based on the mass of the random copolymer.

[0146] The melt flow rate (MFR) of the polymer (B) is 0.1 to 500 g / 10 min, preferably 0.5 g / 10 min or more, more preferably 1 g / 10 min or more, and preferably 300 g / 10 min or less, more preferably 200 g / 10 min or less, even more preferably 100 g / 10 min or less, particularly preferably 90 g / 10 min or less, 50 g / 10 min or less, 30 g / 10 min or less, or 10 g / 10 min or less. That is, the MFR is preferably 0.5 to 300 g / 10 min, more preferably 0.5 to 200 g / 10 min, even more preferably 0.5 to 100 g / 10 min, and particularly preferably 0.5 to 90 g / 10 min. When the MFR is within the above range, a composition having excellent moldability can be easily obtained, and a composition or molded article having excellent dispersibility between the polymer (B) and the copolymer (A) and excellent mechanical strength such as tensile strength can be easily obtained.

[0147] In one embodiment, the melting point (Tm) of the polymer (B) measured by DSC is 110 to 170° C., preferably 120 to 170° C., more preferably 125 to 168° C., even more preferably 130 to 168° C., still more preferably 133 to 168° C., and particularly preferably 135 to 165° C. When the melting point is in the above range, the balance of moldability, heat resistance, and transparency is excellent, and the properties as a crystalline polypropylene are good, which is preferable.

[0148] The melting point of polymer (B) is the melting point (the temperature at the apex of the melting peak) observed using a DSC measurement device when the polymer is heated from room temperature to 200°C at a heating rate of 10°C / min, held at 200°C for 10 minutes, cooled to -20°C at a heating rate of 10°C / min, held at -20°C for 1 minute, and then heated again to 200°C at a heating rate of 10°C / min. The heat of fusion (ΔH), which is the integrated value of the melting peak, is preferably 50 to 120 J / g. When two or more melting peaks are observed, the highest temperature among the apex temperatures of these peaks is taken as the melting point.

[0149] The polymer (B) can be produced by various known methods using a catalyst such as a Ziegler-Natta catalyst or a metallocene catalyst.

[0150] Hereinafter, a resin composition containing copolymer (A) and polymer (B) will be described. In this composition, when the total content of copolymer (A) and polymer (B) is taken as 100% by mass, the content of copolymer (A) is preferably 1 to 99% by mass, more preferably 5 to 95% by mass, even more preferably 6 to 93% by mass, even more preferably 8 to 90% by mass, and particularly preferably 12 to 70% by mass; and the content of polymer (B) is preferably 1 to 99% by mass, more preferably 5 to 95% by mass, even more preferably 7 to 94% by mass, even more preferably 10 to 92% by mass, and particularly preferably 30 to 88% by mass. When the contents of copolymer (A) and polymer (B) are within the above ranges, a composition or molded article having an excellent balance between flexibility and mechanical strength, such as tensile strength, can be easily obtained.

[0151] The total content of copolymer (A) and polymer (B) in the present composition can be appropriately set according to its application and is not particularly limited.The total content of copolymer (A) and polymer (B) in the present composition can be, for example, 50 mass% or more, 60 mass% or more, 70 mass% or more, 80 mass% or more, 90 mass% or more, or 95 mass% or more, based on the mass of the present composition.

[0152] <Ethylene-Based Polymer (C)> From the viewpoint of improving whitening resistance during stretching in secondary processing such as deep drawing, the present composition preferably further contains an ethylene-based polymer (C) (hereinafter also referred to as “polymer (C)”).

[0153] One embodiment of the present composition contains a copolymer (A), a propylene-based polymer (B), and an ethylene-based polymer (C). The present composition containing the ethylene-based polymer (C) in addition to the copolymer (A) and the propylene-based polymer (B) can easily provide a sealant film that is particularly excellent in balance between impact resistance and transparency.

[0154] The ethylene polymer (C) is a polymer having preferably 60 to 100 mol % of structural units derived from ethylene, based on 100 mol % of the total amount of structural units derived from polymerizable monomers.

[0155] The ethylene polymer (C) may have at least one structural unit derived from a biomass-derived monomer. Examples of biomass-derived monomers include biomass-derived ethylene and biomass-derived α-olefins having 3 to 20 carbon atoms. The same type of monomer constituting the polymer may be only biomass-derived monomers, only fossil fuel-derived monomers, or may contain both biomass-derived monomers and fossil fuel-derived monomers. When the present composition contains a polymer (C), the polymer (C) may be one type or two or more types.

[0156] Examples of the ethylene polymer (C) include high-pressure low-density polyethylene (c1) and ethylene / α-olefin copolymer (c2). The ethylene polymer (C) preferably contains high-pressure low-density polyethylene (c1) or ethylene / α-olefin copolymer (c2). These polymers are described below.

[0157] <High-pressure low-density polyethylene (c1)> Any known high-pressure low-density polyethylene can be used as the high-pressure low-density polyethylene (c1) without any restrictions. High-pressure low-density polyethylene is generally polyethylene obtained by radical polymerization of ethylene under high temperature and high pressure. The method for producing high-pressure low-density polyethylene is not particularly limited, but examples thereof include a radical polymerization method in which ethylene is radically polymerized under conditions of 500 to 2000 atmospheres and 150 to 300°C. Examples of the polymerization initiator include organic peroxides.

[0158] The density of the high-pressure low-density polyethylene (c1) is preferably 900 to 925 kg / m 3 , more preferably 910 to 925 kg / m 3 The high-pressure low-density polyethylene (c1) having a density in the above range is excellent in, for example, stickiness resistance and flexibility. The density is measured at 25°C in accordance with ASTM D1505.

[0159] The melt flow rate (MFR) of the high-pressure low-density polyethylene (c1) is preferably 0.1 g / 10 min or more, more preferably 0.5 g / 10 min or more, particularly preferably 1.0 g / 10 min or more, and is preferably 50 g / 10 min or less, more preferably 30 g / 10 min or less, particularly preferably 20 g / 10 min or less, for example, 0.1 to 50 g / 10 min. High-pressure low-density polyethylene (c1) having an MFR in the above range has, for example, excellent moldability and heat resistance. The MFR is measured in accordance with ASTM D1238E under conditions of 190°C and a load of 2.16 kg.

[0160] The melting point (Tm) of the high-pressure low-density polyethylene (c1) measured by DSC is preferably 104 to 130° C., more preferably 105 to 125° C., and even more preferably 106 to 120° C. The high-pressure low-density polyethylene (c1) having a melting point within the above range is excellent in, for example, stickiness resistance, heat resistance, and flexibility.

[0161] The melting point of the high-pressure low-density polyethylene (c1) is the melting point (the temperature at the apex of the melting peak) observed using a DSC when the sample is heated from room temperature to 200°C at a heating rate of 10°C / min, held at 200°C for 10 minutes, cooled to -20°C at a heating rate of 10°C / min, held at -20°C for 1 minute, and then heated again to 200°C at a heating rate of 10°C / min. When two or more melting peaks are observed, the highest temperature among the temperatures at the apex of these peaks is taken as the melting point.

[0162] The high-pressure low-density polyethylene (c1) is preferably a polymer having 100 mol % of structural units derived from ethylene, relative to a total of 100 mol % of structural units derived from polymerizable monomers.

[0163] <Ethylene / α-olefin copolymer (c2)> The ethylene / α-olefin copolymer (c2) has at least structural units derived from ethylene and structural units derived from an α-olefin having 3 to 20 carbon atoms. The content of structural units derived from ethylene in the ethylene / α-olefin copolymer (c2) is preferably 60 to 99 mol%, more preferably 65 to 99 mol%, even more preferably 70 to 99 mol%, and particularly preferably 80 to 99 mol%. Ethylene / α-olefin copolymers (c2) having a content of structural units derived from ethylene within the above ranges are excellent in, for example, stickiness resistance, heat resistance, and flexibility.

[0164] The ethylene / α-olefin copolymer (c2) is characterized by having fewer long-chain branched structures than the high-pressure low-density polyethylene (c1), and is generally sometimes referred to as linear low-density polyethylene (LLDPE).

[0165] The content of structural units derived from an α-olefin having 3 to 20 carbon atoms in the ethylene / α-olefin copolymer (c2) is preferably 1 to 40 mol%, more preferably 1 to 35 mol%, even more preferably 1 to 30 mol%, and particularly preferably 1 to 20 mol%. Ethylene / α-olefin copolymer (c2) having a content of structural units derived from an α-olefin having 3 to 20 carbon atoms in the above range exhibits, for example, excellent stickiness resistance, heat resistance, and flexibility.

[0166] In the ethylene / α-olefin copolymer (c2), the content of each of the structural units is the amount relative to 100 mol % of the total of the structural units derived from ethylene and the structural units derived from an α-olefin having 3 to 20 carbon atoms. When the content of each of the structural units is within the above range, for example, a sealant film having an excellent balance between impact resistance and flexibility can be easily obtained.

[0167] Examples of α-olefins having 3 to 20 carbon atoms include propylene, 1-butene, 1-pentene, 3-methyl-1-butene, 1-hexene, 4-methyl-1-pentene, 1-heptene, 1-octene, 1-nonene, 1-decene, 1-undecene, 1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene, 1-nonadecene, and 1-eicosene. Among these, α-olefins having 3 to 10 carbon atoms are preferred, α-olefins having 3 to 8 carbon atoms are more preferred, and α-olefins having 3 to 6 carbon atoms are even more preferred. Specifically, propylene, 1-butene, and 1-octene are preferred, propylene and 1-butene are more preferred, and propylene is even more preferred.

[0168] In producing the ethylene / α-olefin copolymer (c2), one type or two or more types of α-olefins having 3 to 20 carbon atoms may be used. The ethylene / α-olefin copolymer (c2) has at least one type of structural unit derived from an α-olefin having 3 to 20 carbon atoms, and may have two or more types.

[0169] In addition to the above structural units, the ethylene / α-olefin copolymer (c2) may contain one or more structural units derived from other polymerizable monomers, provided that the objectives of the present disclosure are not impaired. Examples of such other polymerizable monomers include vinyl compounds such as styrene, vinylcyclopentene, vinylcyclohexane, and vinylnorbornane; vinyl esters such as vinyl acetate; unsaturated organic acids or derivatives thereof such as maleic anhydride; and non-conjugated polyenes such as dicyclopentadiene, cyclohexadiene, and 5-ethylidene-2-norbornene.

[0170] The total content of structural units derived from ethylene and structural units derived from an α-olefin having 3 to 20 carbon atoms in the ethylene / α-olefin copolymer (c2) is preferably 80% by mass or more, more preferably 85% by mass or more, even more preferably 90% by mass or more, still more preferably 95% by mass or more, and particularly preferably 98% by mass or more, based on the mass of the copolymer (c2).

[0171] Examples of the ethylene-α-olefin copolymer (c2) include an ethylene-propylene copolymer, an ethylene-1-butene copolymer, an ethylene-propylene-1-butene copolymer, an ethylene-propylene-ethylidenenorbornene copolymer, an ethylene-1-butene-1-octene copolymer, an ethylene-4-methyl-1-pentene copolymer, an ethylene-1-hexene copolymer, and an ethylene-1-octene copolymer. Among these, for example, an ethylene-propylene copolymer and an ethylene-1-butene copolymer are preferred.

[0172] The density of the ethylene / α-olefin copolymer (c2) is preferably 840 kg / m 3 More preferably, 850 kg / m 3 More preferably, 855 kg / m 3 or more, preferably 940 kg / m 3 or less, more preferably 899 kg / m 3 More preferably, 890 kg / m or less 3 Particularly preferably 885 kg / m or less 3 or less, for example, 840 to 940 kg / m 3 The present composition containing the copolymer (c2) having a density within the above range has, for example, an excellent balance of impact resistance, rigidity, and transparency. The density is measured at 25°C in accordance with ASTM D1505.

[0173] The melt flow rate (MFR) of the ethylene / α-olefin copolymer (c2) is preferably 0.01 g / 10 min or more, more preferably 0.1 g / 10 min or more, and preferably 40 g / 10 min or less, more preferably 20 g / 10 min or less, particularly preferably 10 g / 10 min or less, for example, 0.01 to 40 g / 10 min. The composition containing the copolymer (c2) having an MFR in the above range has, for example, an excellent balance of impact resistance, rigidity, and transparency. The MFR is measured in accordance with ASTM D1238E under conditions of 190°C and a load of 2.16 kg.

[0174] The ethylene / α-olefin copolymer (c2) had an MFR measured under conditions of 190°C and a load of 10 kg in accordance with ASTM D1238E. 10 and the ratio of MFR2 measured under the conditions of 190°C and a load of 2.16 kg (MFR 10 / MFR2) is preferably 4.0 or more, more preferably 5.0 or more, and is preferably 8.0 or less, more preferably 7.0 or less, for example, 4.0 to 8.0. 10 The present composition containing the copolymer (c2) having a / MFR2 in the above range has, for example, an excellent balance between transparency and impact resistance.

[0175] The melting point (Tm) of the ethylene / α-olefin copolymer (c2) measured by DSC is preferably 30 to 100°C, more preferably 31 to 90°C, and even more preferably 32 to 80°C. The composition containing the copolymer (c2) having a melting point within the above range has, for example, an excellent balance between transparency and impact resistance. Details of the conditions for measuring the melting point are as described in the section for the high-pressure low-density polyethylene (c1).

[0176] The ethylene / α-olefin copolymer (c2) can be produced by a conventional method using, for example, a vanadium catalyst, a titanium catalyst, or a metallocene catalyst. Preferably, a metallocene catalyst is used to obtain an ethylene / α-olefin copolymer (c2) having a narrow molecular weight distribution and composition distribution. Such a copolymer (c2) is more suitable in terms of, for example, mechanical properties, transparency, and impact resistance.

[0177] Hereinafter, a resin composition containing copolymer (A), propylene-based polymer (B), and ethylene-based polymer (C) will be described. When the total content of copolymer (A), polymer (B), and polymer (C) is taken as 100% by mass, it is preferable that the content of copolymer (A) is 1 to 98% by mass, the content of polymer (B) is 1 to 98% by mass, and the content of polymer (C) is 1 to 20% by mass.

[0178] The content of copolymer (A) is preferably 1 to 98 mass%, more preferably 5 to 78 mass%, even more preferably 10 to 57 mass%, and particularly preferably 15 to 45 mass%, relative to 100 mass% of the total content of copolymer (A), polymer (B), and polymer (C). A resin composition having a content of copolymer (A) within the above range tends to have an excellent balance of heat resistance, tensile strength, and whitening resistance.

[0179] The content of the propylene polymer (B) is preferably 1 to 98 mass%, more preferably 20 to 93 mass%, still more preferably 40 to 87 mass%, and particularly preferably 50 to 80 mass%, relative to 100 mass% of the total content of the copolymer (A), the polymer (B), and the polymer (C). A resin composition having a content of the polymer (B) within the above range tends to have an excellent balance of heat resistance, tensile strength, and whitening resistance.

[0180] The content of the ethylene polymer (C) is preferably 1 to 20 mass%, more preferably 2 to 19 mass%, even more preferably 3 to 18 mass%, and particularly preferably 5 to 15 mass%, relative to 100 mass% of the total content of the copolymer (A), the polymer (B), and the polymer (C). A resin composition having a content of the polymer (C) within the above range tends to have an excellent balance of heat resistance, tensile strength, and whitening resistance.

[0181] The total content of the copolymer (A), propylene polymer (B), and ethylene polymer (C) in the composition is not particularly limited and can be appropriately set depending on the application. The total content of the copolymer (A), propylene polymer (B), and ethylene polymer (C) in the composition may be, for example, 50% by mass or more, 60% by mass or more, 70% by mass or more, 80% by mass or more, 90% by mass or more, or 95% by mass or more, based on the mass of the composition.

[0182] One embodiment of the composition contains a copolymer (A), a propylene-based polymer (B), and an ethylene-based polymer (C). The resin composition of the above embodiment can form a layer or film that has an excellent balance of heat resistance, tensile strength, and whitening resistance during stretching in secondary processing such as deep drawing. A single-layer or multilayer film having a layer formed from the resin composition of the above embodiment has excellent whitening resistance during stretching and good heat resistance and tensile strength, and is therefore suitable for use as packaging for daily necessities, food, liquids, pharmaceuticals, electronic components, building materials, and lithium-ion batteries, for example.

[0183] <Additives> The composition may further contain additives as long as the objectives of the present disclosure are not impaired. Examples of additives include polyolefins other than the copolymer (A), the propylene polymer (B), and the ethylene polymer (C), or modified polyolefins thereof, weathering stabilizers such as ultraviolet absorbers and light stabilizers, heat stabilizers, antioxidants, antiaging agents, antistatic agents, antislip agents, antiblocking agents, antifogging agents, nucleating agents (crystal nucleating agents), lubricants, pigments, dyes, flowability modifiers, plasticizers such as mineral oil, foaming agents, foaming assistants, hydrochloric acid absorbers, antibacterial agents, antifungal agents, and fillers. The composition may contain one or more additives. One or more of each additive may be used.

[0184] <Method for Producing the Composition> The method for producing the composition is not particularly limited. The composition can be produced, for example, by mixing the propylene-α-olefin copolymer (A), optionally the propylene polymer (B), optionally the ethylene polymer (C), and optionally other optional components such as additives using, for example, a Henschel mixer, a V-blender, a ribbon blender, a tumbler blender, a kneader-ruder, or the like, or by melt-kneading the components after mixing or without mixing using a single-screw extruder, a twin-screw extruder, a kneader, a Banbury mixer, or the like. Furthermore, granulation or pulverization may be carried out as necessary. When mixing or kneading these components, the components to be blended may be added all at once or in stages.

[0185] The melt-kneading method is not particularly limited, and can be carried out using a melt-kneading device such as a commercially available extruder. For example, the temperature of the part of the melt-kneading device where the kneading is carried out may be 170 to 250° C. or 190 to 230° C. The kneading time may be 0.5 to 30 minutes or 0.5 to 5 minutes.

[0186] <Coating Agent> An example of an application of the copolymer (A) or the present composition is a coating agent. The coating agent is not particularly limited, and examples thereof include coating agents prepared by dissolving or dispersing the copolymer (A) or the present composition in an organic solvent. The coating agent contains the copolymer (A) or the present composition. In this case, the present composition is preferably a resin composition containing the propylene-α-olefin copolymer (A) and the propylene-based polymer (B).

[0187] Examples of organic solvents include aromatic hydrocarbons such as benzene, toluene, and xylene; aliphatic hydrocarbons such as hexane, heptane, octane, and decane; alicyclic hydrocarbons such as cyclohexane, cyclohexene, methylcyclohexane, ethylcyclohexane, and decahydronaphthalene; alcohols such as methanol, ethanol, isopropyl alcohol, butanol, pentanol, hexanol, and propanediol; ketone solvents such as acetone, methyl isobutyl ketone, methyl ethyl ketone, pentanone, hexanone, isophorone, and acetophenone; cellosolves such as methyl cellosolve and ethyl cellosolve; esters such as methyl acetate, ethyl acetate, butyl acetate, methyl propionate, and butyl formate; and halogenated hydrocarbons such as trichloroethylene, dichloroethylene, and chlorobenzene. One or more organic solvents may be used.

[0188] The content of the organic solvent in the coating agent is not particularly limited, but may be, for example, 30% by mass or more, 40% by mass or more, 90% by mass or less, or 80% by mass or less.

[0189] The coating agent can be used, for example, as an adhesive or heat sealing agent between metals, between polyolefins, between metals and polyolefins, or as an adhesive for PTP (press through pack) packaging, a laminating adhesive, a paint raw material, or a primer raw material. It is particularly suitable when at least one of the adherends is a plastic material, and among plastic materials, it is preferable when the adherend is a polyolefin material, particularly a polybutene-based material or a polypropylene-based material.

[0190] [Molded Article] The molded article of the present disclosure contains the copolymer (A) or the present composition. The molded article can be produced by molding the copolymer (A) or the present composition using a conventionally known molding method. Examples of molding methods include sheet (film) molding, blow molding, injection molding, press molding, extrusion molding, inflation molding, extrusion blow molding, injection blow molding, vacuum molding, calendar molding, and melt T-die casting.

[0191] The molded article is not particularly limited, but since the copolymer (A) or the present composition exhibits the above-mentioned effects, it is preferable that the molded article is one that can more effectively exhibit the above-mentioned effects.Specific examples of the molded article include films, sheets, injection molded articles, and blow molded articles.More specifically, the molded article includes civil engineering and building material parts such as multi-layer hoses, pipes, tubes, decorative sheets, and flooring mats; covering materials for electric wires and cables (e.g., insulating layers, sheath layers), nonwoven fabrics, stretch films, food packaging films, packaging sheets, food packaging trays and beverage cups (thermoformed from sheets), and plastic containers (folded from sheets).

[0192] The molded article can be suitably used as a battery packaging body, such as a lithium-ion battery packaging body. That is, the present disclosure also provides an electricity storage device including the molded article. Examples of electricity storage devices include lithium-ion batteries and lithium-ion capacitors.

[0193] <Pellets> The molded article of the present disclosure may be pellets. In this specification, pellets are obtained by cutting the copolymer (A) or the present composition while extruding it, and are therefore included in the molded article. The shape, size, etc. of the pellets are not particularly limited and may be appropriately selected depending on the desired application. The pellets can be produced by melting the copolymer (A) or the present composition in a kneader and granulating it. Examples of kneaders include a Banbury mixer, a roll, and an extruder.

[0194] <Film> The molded article of the present disclosure may be, for example, a film. The film is not particularly limited, and the shape, size, thickness, etc. may be appropriately selected depending on the desired application. The film may be a stretched film or a non-stretched film. The film may be a single-layer film or a multilayer film. When the film is a multilayer film, at least one layer thereof may contain the copolymer (A) or the present composition.

[0195] The thickness of the film (total thickness in the case of a multilayer film) is preferably 5 to 150 μm, more preferably 10 to 100 μm. In this specification, no particular distinction is made between film and sheet, but a film generally refers to a membranous body with a thickness of less than 250 μm, and a sheet generally refers to a thin plate-like body with a thickness of 250 μm or more.

[0196] Specific applications of the film include, for example, packaging films for packaging food, liquids, medicines, and the like.

[0197] <Sheet> The molded article of the present disclosure may be, for example, a sheet. The sheet is not particularly limited, and the shape, size, thickness, etc. may be appropriately selected depending on the desired application. The sheet may be a single-layer sheet or a multi-layer sheet. When the sheet is a multi-layer sheet, at least one layer thereof may be a layer containing the copolymer (A) or the present composition.

[0198] The thickness of the sheet (total thickness in the case of a multi-layer sheet) is preferably 250 to 2000 μm, more preferably 250 to 1500 μm.

[0199] Specific uses of the sheet include, for example, packaging sheets for packaging food, liquids, medicines, etc., and containers formed from the sheet (e.g., trays or cups obtained by thermoforming the sheet, and containers obtained by folding the sheet).

[0200] <Injection Molded Article and Blow Molded Article> The molded article of the present disclosure may be, for example, an injection molded article. The injection molded article is not particularly limited, and examples of the injection molded article include a molded article produced by injection molding into a desired shape using a conventionally known injection molding device under known conditions. The injection molded article can be widely used, for example, for trim materials for automobile interiors, exterior parts for automobiles, housings for home appliances, containers, tubes, or pipes.

[0201] The molded article of the present disclosure may be, for example, a blow-molded article. The blow-molded article is not particularly limited, and examples of blow-molded articles include those produced by blow molding into a desired shape using a conventionally known blow molding apparatus under known conditions. The blow-molded article may be, for example, a multilayer molded article. In this case, at least one layer of the multilayer molded article contains copolymer (A) or the present composition. Specific applications of injection-molded articles and blow-molded articles include, for example, food containers, beverage containers, caps, pharmaceutical containers, various other containers, daily necessities, housings for home appliances, automobile parts, tubes, and pipes. Daily necessities include, for example, clothing cases, buckets, washbasins, stationery such as writing implements, containers, toys, cooking utensils, and various other cases. <Sealant Film> An example of the molded article is a sealant film. The sealant film has at least one layer (hereinafter also referred to as "layer (X)") formed from the present composition. The sealant film may be a single layer or a multilayer of two or more layers. In this case, the present composition is preferably a resin composition containing a propylene-α-olefin copolymer (A) and a propylene-based polymer (B), or a resin composition containing a propylene-α-olefin copolymer (A), a propylene-based polymer (B), and an ethylene-based polymer (C).

[0202] The sealant film may have two or more layers (X). The sealant film may have the layer (X) and a layer (another layer) other than the layer (X). The sealant film may have two or more of the other layers.

[0203] In this specification, no particular distinction is made between a film and a sheet, but a film generally refers to a membranous body having a thickness of less than 250 μm, and a sheet generally refers to a thin plate-like body having a thickness of 250 μm or more.

[0204] The shape, size, thickness, etc. of the sealant film may be appropriately selected depending on the desired application. The sealant film may be either a stretched film or a non-stretched film, but is preferably a non-stretched film. When the non-stretched film is a multilayer film, "non-stretched" means that none of the layers are stretched.

[0205] The non-stretched film is not particularly limited as long as it is a film that has not been stretched, and the shape, size, thickness, etc. may be appropriately selected depending on the desired application. The non-stretched film may be a single layer or a multilayer film having two or more layers. When the non-stretched film is a multilayer film, at least one of the layers may be layer (X). That is, the non-stretched film may be a single layer or multilayer film consisting of only layer (X), or may be a laminate having layer (X) and a substrate. Specific examples of the substrate will be described later.

[0206] The thickness of the sealant film or unstretched film (the total thickness of each layer if the film is multilayered) is preferably 5 μm or more, more preferably 10 μm or more, even more preferably 20 μm or more, and is preferably 150 μm or less, more preferably 130 μm or less, even more preferably 100 μm or less, for example, 5 to 150 μm.

[0207] Specific applications of the sealant film or non-stretched film include, for example, packaging films for packaging food, liquids, medicines, electronic components, etc., and packaging materials obtained therefrom.

[0208] The sealant film or unstretched film can be produced, for example, using at least the present composition using a conventionally known monolayer or multilayer film molding machine. The method for producing the unstretched film is not particularly limited as long as it does not impair the objectives of the present disclosure. Examples of unstretched films include films obtained by coextrusion using known multilayer film molding methods such as T-die film molding and inflation film molding, and films obtained by laminating layer (X) onto a preformed substrate. The unstretched film may be obtained, for example, by a production method including a step of bonding a monolayer or multilayer film containing at least one layer (X) (e.g., a monolayer or multilayer film consisting only of layer (X)) to a substrate by any method selected from the group consisting of melt extrusion lamination, thermal lamination, and dry lamination.

[0209] <Laminate> An example of the molded article is a laminate. The laminate has a substrate and a layer (layer (X)) formed from the present composition. In this case, the present composition is preferably a resin composition containing a propylene-α-olefin copolymer (A) and a propylene-based polymer (B), or a resin composition containing a propylene-α-olefin copolymer (A), a propylene-based polymer (B), and an ethylene-based polymer (C). In one embodiment, the laminate has a substrate and the sealant film. In the laminate, for example, a substrate and a sealant film are laminated together.

[0210] Examples of the substrate include resin films, metal foils, paper, and vapor-deposited films. Examples of the resin constituting the resin film include thermoplastic resins, specifically polyolefin resins (e.g., polyethylene, polypropylene), polystyrene resins, polyester resins (e.g., polyethylene terephthalate (PET)), polyamide resins, polyimide resins, polycarbonate resins, polyarylate resins, acrylic resins, polyphenylene sulfide resins, vinyl resins, vinyl chloride resins, and epoxy resins. The resin film may be a single layer or a multilayer of two or more layers. The resin film may be a stretched film or a non-stretched film. Examples of the metal foil include aluminum foil, steel foil, and stainless steel foil, with aluminum foil being preferred.

[0211] The substrate is preferably at least one selected from the group consisting of polyolefin film, polystyrene film, polyester film, polyamide film, laminated film of polyolefin film and gas barrier resin film, metal foil such as aluminum foil, paper, and vapor-deposited film.

[0212] The laminate can be produced, for example, using a conventionally known single-layer or multi-layer film molding machine. The laminate can be produced, for example, by a production method including a step of bonding a substrate and the sealant film by any one selected from the group consisting of melt extrusion lamination, thermal lamination, and dry lamination. The laminate can be produced, for example, by a production method including a step of bonding a substrate and a single-layer or multi-layer film consisting of only layer (X) by any one selected from the group consisting of melt extrusion lamination, thermal lamination, and dry lamination.

[0213] The laminate itself may be used as a sealant film. In this case, the substrate is preferably a resin film, more preferably a non-stretched film. That is, the sealant film may be a single-layer or multi-layer film consisting of only the layer (X), or may be a laminate having the layer (X) and the substrate.

[0214] The sealant film and the laminate have excellent resistance to whitening when stretched, and good heat resistance and tensile strength. Therefore, by taking advantage of the properties of the sealant film, they can be suitably used as packaging for a variety of items, such as daily necessities, food (food packaging materials), liquids, pharmaceuticals, electronic components, and construction materials.

[0215] The sealant film or the laminate may be included in an electricity storage device such as a lithium ion battery or a lithium ion capacitor. The sealant film or the laminate can be suitably used, for example, as a packaging material for a lithium ion battery. From another perspective, the present disclosure can also be said to provide an electricity storage device including the composition. Examples of such electricity storage devices include electricity storage devices including the sealant film or the laminate, and specific examples thereof include packaging materials for lithium ion batteries including the sealant film or the laminate.

[0216] A lithium-ion battery typically includes a positive electrode, a negative electrode, a separator between the positive and negative electrodes, and a nonaqueous electrolyte. The positive electrode typically includes a positive electrode current collector made of a metal or carbon material, and a positive electrode active material capable of absorbing and releasing lithium, such as a composite oxide of lithium and a transition metal. The negative electrode typically includes a negative electrode current collector made of a carbon material, and a negative electrode active material capable of absorbing and releasing lithium ions, such as metallic lithium, a lithium-containing alloy, or a metal or alloy capable of alloying with lithium. The nonaqueous electrolyte includes a lithium salt as an electrolyte and a nonaqueous solvent. In a lithium-ion battery, the positive electrode, negative electrode, and separator are impregnated with the nonaqueous electrolyte. Details of the nonaqueous solvent will be described later in the section "Nonaqueous Solvent."

[0217] Lithium-ion batteries often have a packaging body (lithium-ion battery packaging body) around their periphery. A positive electrode, a negative electrode, a separator, and a nonaqueous electrolyte are enclosed inside the packaging body. Typically, a positive electrode terminal and a negative electrode terminal are connected to the positive electrode and the negative electrode, respectively. A portion of the positive electrode terminal and a portion of the negative electrode terminal are exposed to the outside of the packaging body.

[0218] The case where the sealant film or the laminate is used as a package will be described below. A lithium ion battery is obtained by sandwiching a positive electrode, a negative electrode, or the like between a pair of sealant films or a pair of laminates, and heat-sealing the peripheral edges of the pair of sealant films or the pair of laminates in a manner such that a portion of the positive electrode terminal and a portion of the negative electrode terminal are exposed to the outside of the pair of sealant films or the pair of laminates. When the laminate is used as a package, the laminate may have a substrate made of a metal such as aluminum foil.

[0219] Lithium ion batteries using the lithium ion battery packaging can be used in, for example, portable electronic devices, personal computers, robots, drones, automobiles, aircraft, wearable devices, and energy storage systems (ESS) for home use or renewable energy power generation.

[0220] <Non-aqueous solvent> A non-aqueous electrolyte for a lithium ion battery generally contains a non-aqueous solvent. Various known non-aqueous solvents can be appropriately selected as the non-aqueous solvent. As the non-aqueous solvent, it is preferable to use at least one selected from the group consisting of cyclic aprotic solvents and chain aprotic solvents. When aiming to improve the flash point of the solvent in order to improve the safety of the battery, it is preferable to use a cyclic aprotic solvent as the non-aqueous solvent.

[0221] (Cyclic Aprotic Solvent) Examples of cyclic aprotic solvents include cyclic carbonates, cyclic carboxylic acid esters, cyclic sulfones, and cyclic ethers.

[0222] The cyclic aprotic solvent may be used alone or in combination of two or more. The content of the cyclic aprotic solvent in the nonaqueous solvent is preferably 10 to 100% by mass, more preferably 20 to 90% by mass, and even more preferably 30 to 80% by mass. By adjusting the content to such a ratio, for example, the conductivity of the electrolyte, which is related to the charge / discharge characteristics of the battery, can be increased.

[0223] Examples of cyclic carbonates include ethylene carbonate, propylene carbonate, 1,2-butylene carbonate, 2,3-butylene carbonate, 1,2-pentylene carbonate, and 2,3-pentylene carbonate. Among these, ethylene carbonate and propylene carbonate, which have high dielectric constants, are preferred. In the case of batteries using graphite as the negative electrode active material, ethylene carbonate is more preferred. Two or more cyclic carbonates may be used in combination.

[0224] Examples of cyclic carboxylic acid esters include γ-butyrolactone, δ-valerolactone, and alkyl-substituted derivatives such as methyl-γ-butyrolactone, ethyl-γ-butyrolactone, and ethyl-δ-valerolactone.

[0225] Cyclic carboxylic acid esters have low vapor pressure, low viscosity, and high dielectric constant, and can reduce the viscosity of the electrolyte without lowering the flash point and the degree of dissociation of the electrolyte. Therefore, cyclic carboxylic acid esters have the characteristic of being able to increase the conductivity of the electrolyte, which is an indicator of the charge / discharge characteristics of the battery, without increasing the flammability of the electrolyte. Therefore, when aiming to increase the flash point of the solvent, it is preferable to use a cyclic carboxylic acid ester as the cyclic aprotic solvent. γ-Butyrolactone is most preferable.

[0226] The cyclic carboxylic acid ester is preferably used in combination with other cyclic aprotic solvents and / or chain aprotic solvents, for example, a mixture (combination) of a cyclic carboxylic acid ester with a cyclic carbonate and / or a chain carbonate.

[0227] Examples of combinations of cyclic carboxylic acid esters and cyclic carbonates and / or chain carbonates include γ-butyrolactone and ethylene carbonate, γ-butyrolactone, ethylene carbonate and dimethyl carbonate, γ-butyrolactone, ethylene carbonate and methyl ethyl carbonate, γ-butyrolactone, ethylene carbonate and diethyl carbonate, γ-butyrolactone and propylene carbonate, γ-butyrolactone, propylene carbonate and dimethyl carbonate, γ-butyrolactone, propylene carbonate and Methyl ethyl carbonate, γ-butyrolactone, propylene carbonate, and diethyl carbonate, γ-butyrolactone, ethylene carbonate, and propylene carbonate, γ-butyrolactone, ethylene carbonate, propylene carbonate, and dimethyl carbonate, γ-butyrolactone, ethylene carbonate, propylene carbonate, and methyl ethyl carbonate, γ-butyrolactone, ethylene carbonate, propylene carbonate, and diethyl carbonate, γ-butyrolactone, ethylene carbonate, dimethyl carbonate, and methyl ethyl ethyl carbonate, γ-butyrolactone, ethylene carbonate, dimethyl carbonate, and diethyl carbonate, γ-butyrolactone, ethylene carbonate, methyl ethyl carbonate, and diethyl carbonate, γ-butyrolactone, ethylene carbonate, dimethyl carbonate, methyl ethyl carbonate, and diethyl carbonate, γ-butyrolactone, ethylene carbonate, propylene carbonate, dimethyl carbonate, and methyl ethyl carbonate, γ-butyrolactone, ethylene carbonate, propylene carbonate, and dimethyl carbonate ester and diethyl carbonate, γ-butyrolactone, ethylene carbonate, propylene carbonate, methyl ethyl carbonate, and diethyl carbonate, γ-butyrolactone, ethylene carbonate, propylene carbonate, dimethyl carbonate, methyl ethyl carbonate, and diethyl carbonate, γ-butyrolactone and sulfolane, γ-butyrolactone, ethylene carbonate, and sulfolane, γ-butyrolactone, propylene carbonate, and sulfolane, γ-butyrolactone, ethylene carbonate, propylene carbonate, and sulfolane,Examples include γ-butyrolactone, sulfolane, and dimethyl carbonate.

[0228] Examples of cyclic sulfones include sulfolane, 2-methylsulfolane, 3-methylsulfolane, dimethylsulfone, diethylsulfone, dipropylsulfone, methylethylsulfone, and methylpropylsulfone. Examples of cyclic ethers include dioxolane.

[0229] (Chain Aprotic Solvent) Examples of chain aprotic solvents include chain carbonates, chain carboxylic acid esters, chain ethers, and chain phosphate esters.

[0230] The chain aprotic solvent may be used alone or in combination of two or more. The content of the chain aprotic solvent in the non-aqueous solvent is preferably 10 to 100% by mass, more preferably 20 to 90% by mass, and even more preferably 30 to 80% by mass.

[0231] Examples of chain carbonate include dimethyl carbonate, methyl ethyl carbonate, diethyl carbonate, methyl propyl carbonate, methyl isopropyl carbonate, ethyl propyl carbonate, dipropyl carbonate, methyl butyl carbonate, ethyl butyl carbonate, dibutyl carbonate, methyl pentyl carbonate, ethyl pentyl carbonate, dipentyl carbonate, methyl heptyl carbonate, ethyl heptyl carbonate, diheptyl carbonate, methyl hexyl carbonate, ethyl hexyl carbonate, dihexyl carbonate, methyl octyl carbonate, ethyl octyl carbonate, dioctyl carbonate and methyl trifluoroethyl carbonate.Two or more chain carbonates can be mixed and used.

[0232] Examples of the chain carboxylic acid ester include methyl pivalate, examples of the chain ether include dimethoxyethane, and examples of the chain phosphate ester include trimethyl phosphate.

[0233] (Solvent Combination) The nonaqueous solvent contained in the nonaqueous electrolyte may be one type or two or more types. One or more cyclic aprotic solvents may be used alone, one or more chain aprotic solvents may be used alone, or a mixture of a cyclic aprotic solvent and a chain aprotic solvent may be used. When it is particularly intended to improve the load characteristics and low-temperature characteristics of the battery, it is preferable to use a combination of a cyclic aprotic solvent and a chain aprotic solvent as the nonaqueous solvent.

[0234] From the viewpoint of electrochemical stability of the electrolyte, it is most preferable to use a cyclic carbonate as the cyclic aprotic solvent and a chain carbonate as the chain aprotic solvent. The combination of a cyclic carboxylic acid ester with a cyclic carbonate and / or a chain carbonate can also increase the conductivity of the electrolyte, which is related to the charge / discharge characteristics of the battery.

[0235] Examples of combinations of cyclic carbonates and chain carbonates include ethylene carbonate and dimethyl carbonate, ethylene carbonate and methyl ethyl carbonate, ethylene carbonate and diethyl carbonate, propylene carbonate and dimethyl carbonate, propylene carbonate and methyl ethyl carbonate, propylene carbonate and diethyl carbonate, ethylene carbonate, propylene carbonate and methyl ethyl carbonate, ethylene carbonate, propylene carbonate and diethyl carbonate, ethylene carbonate, dimethyl carbonate and methyl ethyl carbonate, and ethylene carbonate and dimethyl carbonate. Examples of suitable carbonates include ethylene carbonate and diethyl carbonate, ethylene carbonate, methyl ethyl carbonate and diethyl carbonate, ethylene carbonate, dimethyl carbonate, methyl ethyl carbonate and diethyl carbonate, ethylene carbonate, propylene carbonate, dimethyl carbonate and methyl ethyl carbonate, ethylene carbonate, propylene carbonate, dimethyl carbonate and diethyl carbonate, ethylene carbonate, propylene carbonate, methyl ethyl carbonate and diethyl carbonate, and ethylene carbonate, propylene carbonate, dimethyl carbonate, methyl ethyl carbonate and diethyl carbonate.

[0236] The mixing ratio of the cyclic carbonate to the chain carbonate (cyclic carbonate:chain carbonate), expressed as a mass ratio, is preferably 5:95 to 80:20, more preferably 10:90 to 70:30. By using such a mixing ratio, an increase in the viscosity of the electrolyte can be suppressed and the degree of dissociation of the electrolyte can be increased, thereby increasing the conductivity of the electrolyte, which is related to the charge / discharge characteristics of the battery, and further increasing the solubility of the electrolyte. Therefore, an electrolyte with excellent electrical conductivity at room temperature or low temperatures can be obtained, thereby improving the load characteristics of the battery at room temperature to low temperatures.

[0237] The lithium ion battery contains a non-aqueous electrolyte solution containing the non-aqueous solvent. Therefore, it is preferable that the packaging (lithium ion battery packaging) constituting the lithium ion battery is resistant to leaching in the non-aqueous solvent and swelling caused by the non-aqueous solvent, and is also able to maintain a certain level of mechanical strength even when exposed to contact with the non-aqueous solvent. The sealant film and the laminate having a layer formed from this composition have excellent whitening resistance and, for example, are resistant to leaching in the non-aqueous solvent and swelling caused by the non-aqueous solvent, and are able to maintain a certain level of mechanical strength even when exposed to contact with the non-aqueous solvent. Therefore, the sealant film and the laminate can be suitably used as a packaging for a lithium ion battery.

[0238] The propylene / α-olefin copolymer and resin composition of the present disclosure will be described below with reference to examples, but the propylene / α-olefin copolymer and resin composition of the present disclosure are not limited to these examples in any way.

[0239] Example 1A Production of Propylene / α-Olefin Copolymer (A-1) n-Hexane was continuously supplied from one supply port to a 300-liter continuous polymerization reactor at a rate of 20.9 L / h, and a mixed hexane solution of diphenylmethylene(3-tert-butyl-5-ethylcyclopentadienyl)(2,7-di-tert-butylfluorenyl)zirconium dichloride (catalyst type a), modified methylaluminoxane, and triisobutylaluminum (zirconium-equivalent concentration: 0.6 mmol / L, modified methylaluminoxane aluminum-equivalent concentration: 154 mmol / L, triisobutylaluminum aluminum-equivalent concentration: 62 mmol / L) was continuously supplied from another supply port at a rate of 0.057 L / h. At the same time, propylene was continuously fed to the continuous polymerization reactor through separate feed ports at a rate of 13 kg / h, 4-methyl-1-pentene (4MP-1) at a rate of 3.1 kg / h, and hydrogen at a rate of 0.5 NL / h. Continuous solution polymerization was carried out under conditions of a polymerization temperature of 60°C, a polymerization pressure of 1.0 MPaG, and a residence time of 1.5 hours, to obtain a propylene / 4-methyl-1-pentene copolymer (A-1).

[0240] Example 2A Production of Propylene / α-Olefin Copolymer (A-2) A propylene / 4-methyl-1-pentene copolymer (A-2) was produced in the same manner as in Example 1A, except that propylene was continuously supplied at 8.8 kg / h, 4-methyl-1-pentene at 3.5 kg / h, and hydrogen at 0.2 NL / h.

[0241] Example 3A Production of Propylene / α-Olefin Copolymer (A-3) A propylene / 4-methyl-1-pentene copolymer (A-3) was produced in the same manner as in Example 1A, except that propylene was continuously supplied at 16 kg / h, 4-methyl-1-pentene at 10 kg / h, and hydrogen at 2 NL / h.

[0242] Example 4A Production of Propylene / α-Olefin Copolymer (A-4) To a 300-liter continuous polymerization reactor, n-hexane was continuously supplied at a rate of 41.7 L / h through one supply port, and a mixed hexane solution of (8-octamethylfluoren-12′-yl-(2-(adamantan-1-yl)-8-methyl-3,3b,4,5,6,7,7a,8-octahydrocyclopenta[a]indene))zirconium dichloride (catalyst type b) and modified methylaluminoxane (zirconium-equivalent concentration 0.2 mmol / L, modified methylaluminoxane aluminum-equivalent concentration 61 mmol / L) was continuously supplied at a rate of 0.17 L / h, and a hexane solution of triisobutylaluminum (aluminum-equivalent concentration 5.0 mmol / L) was continuously supplied at a rate of 0.30 L / h through another supply port. At the same time, propylene was continuously fed to the continuous polymerization reactor through another feed port at a rate of 9.8 kg / h, 4-methyl-1-pentene at a rate of 2.8 kg / h, and hydrogen at a rate of 4 NL / h. Continuous solution polymerization was carried out under conditions of a polymerization temperature of 70°C, a polymerization pressure of 0.7 MPaG, and a residence time of 1.5 hours, to obtain a propylene / 4-methyl-1-pentene copolymer (A-4).

[0243] Comparative Example 1A As Comparative Example 1A, a commercially available propylene-ethylene copolymer (hereinafter also referred to as "PER-1") (MFR (230°C, 2.16 kg load) = 8 g / 10 min) was used.

[0244] Comparative Example 2A: For Comparative Example 2A, a commercially available propylene-ethylene copolymer (hereinafter also referred to as "PER-2") (MFR (230°C, 2.16 kg load) = 7 g / 10 min) was used.

[0245] [Physical Properties of Propylene-α-olefin Copolymers, etc.] The physical properties of the propylene-α-olefin copolymers obtained in the examples and the propylene-α-olefin copolymers used in the comparative examples were measured by the following methods. The results are shown in Table 1.

[0246] <Propylene content and α-olefin content> The propylene content and comonomer (α-olefin) content in a propylene-α-olefin copolymer were determined under the following conditions: 13 C-NMR measurement was performed, and the obtained 13 It was calculated by analyzing the C-NMR spectrum. In this specification, the content of structural units derived from propylene is also referred to as the "propylene content", and the content of structural units derived from the comonomer α-olefin (other than propylene) is also referred to as the "comonomer content". For polymers other than the above copolymers, the content of each structural unit was calculated in accordance with the above measurement method. Apparatus: AVANCE III Cryo-500 Nuclear Magnetic Resonance Apparatus manufactured by Bruker Biospin Measurement Nuclei: 13 C (125 MHz) Measurement mode: Single pulse proton broadband decoupling Pulse width: 45° (5.00 μsec) Number of points: 64k Measurement range: 250 ppm (-55 to 195 ppm) Repetition time: 5.5 seconds Number of accumulations: 128 Measurement solvent: orthodichlorobenzene / benzene-d6 (4 / 1 [v / v]) Sample concentration: ca. 60 mg / 0.6 mL Measurement temperature: 120°C Window function: exponential (BF: 1.0 Hz) Chemical shift reference: benzene-d6: 128 ppm

[0247] <Density> The density of the propylene-α-olefin copolymer and the ethylene polymer was measured at 25° C. in accordance with ASTM D1505.

[0248] <Intrinsic Viscosity [η]> The intrinsic viscosity [η] of the propylene-α-olefin copolymer was measured in decalin solvent at 135°C using an Ubbelohde viscometer. Approximately 20 mg of the propylene-α-olefin copolymer was dissolved in 15 mL of decalin, and the specific viscosity ηsp was measured in an oil bath heated to 135°C. After diluting this decalin solution with an additional 5 mL of decalin solvent, the specific viscosity ηsp was measured in the same manner. This dilution procedure was repeated two more times, and the value of ηsp / C when the concentration (C) was extrapolated to zero was calculated as the intrinsic viscosity [η] (see the formula below). [η] = lim(ηsp / C) (C → 0)

[0249] <Melting Point (Tm), Heat of Fusion (ΔH), and Glass Transition Temperature (Tg)> The melting points (Tm), heats of fusion (ΔH), and glass transition temperatures (Tg) of the copolymers (A-1) to (A-4) in the above examples and the PER-1 and PER-2 in the above comparative examples were measured by the following method. The melting points (Tm) of the polymers used as the propylene polymer (B-1) and the ethylene polymers (C-1) and (C-2) described below were measured by the same methods as those used to measure the melting points of the polymers (B) and (C), respectively. Using a hydraulic hot press molding machine set at 190°C, the propylene-α-olefin copolymer was heated for 5 minutes, molded under a pressure of 7.5 MPa for 2 minutes, and then cooled at 20°C under a pressure of 7.5 MPa for 5 minutes to produce a sheet having a thickness of 500 μm. After 7 days or more had passed at room temperature after molding, a test piece of approximately 10 mg was punched out from the sheet and cooled from room temperature to -40 ° C at a temperature drop rate of 10 ° C / min under a nitrogen atmosphere and held at that temperature for 5 minutes. Next, the temperature was increased to 200 ° C at a temperature increase rate of 10 ° C / min and held at that temperature for 10 minutes. Next, the temperature was decreased to -70 ° C at a temperature drop rate of 10 ° C / min and held at that temperature for 1 minute. Next, the temperature was increased to 200 ° C at a temperature increase rate of 10 ° C / min. The heat of fusion (ΔH) was calculated from the integrated value of the crystalline melting peak when heated for the second time. The melting point (Tm) was taken as the temperature at the apex of the crystalline melting peak when heated for the second time. The glass transition temperature (Tg) was taken as the temperature at which a baseline shift occurred when heated for the second time. When two or more melting peaks were observed, the highest temperature among the peak apex temperatures of these peaks was taken as the melting point. When the heat of fusion (ΔH) and melting point (Tm) were not observed, the result was indicated as "ND."

[0250] <Weight average molecular weight (Mw) and molecular weight distribution (Mw / Mn)> A GPC apparatus, GPC-IR6_MCT gel permeation chromatograph manufactured by Polymer Characterization, Inc., was used to measure Mw and Mn in terms of polystyrene under the following conditions, and Mw / Mn was calculated.

[0251] Separation columns: two TSKgel GNH6-HT columns manufactured by Tosoh Corporation, and two TSKgel GNH6-HTL columns manufactured by Tosoh Corporation (both column sizes: diameter 7.5 mm, length 300 mm) Column temperature: 140°C Mobile phase: o-dichlorobenzene (manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.) containing 0.025 wt% BHT (manufactured by Takeda Pharmaceutical Co., Ltd.) as an antioxidant Movement speed: 1.0 mL / min Sample concentration: 10 mg / 10 mL Sample injection volume: 400 μL Detector: IR6 type MCT infrared detector Column calibration: monodisperse polystyrene (manufactured by Tosoh Corporation) Molecular weight conversion: polystyrene conversion / standard calibration method

[0252] <MFR> The MFR of the propylene-α-olefin copolymer (A), the propylene polymer (B), PER-1, and PER-2 was measured at 230°C under a load of 2.16 kg in accordance with ASTM D1238E. The MFR of the ethylene polymer (C) was measured at 190°C under a load of 2.16 kg in accordance with ASTM D1238E.

[0253] <Tensile Modulus and Stress at Break> A 2 mm-thick sheet (test specimen) was prepared by heating a propylene-α-olefin copolymer for 5 minutes using a hydraulic heat press molding machine set at 190°C, molding it under a pressure of 7.5 MPa for 2 minutes, and then cooling it at 20°C under a pressure of 7.5 MPa for 5 minutes. Seven days or more after molding, ASTM No. 4 dumbbells were prepared from the above sheet in accordance with ASTM D638. The tensile modulus and stress at break were measured for the dumbbells at 23°C and a pulling rate of 50 mm / min. <Shore D Hardness (Instantaneous Value)> A 2 mm-thick sheet was prepared by heating a propylene-α-olefin copolymer for 5 minutes using a hydraulic heat press molding machine set at 190°C, molding it under a pressure of 7.5 MPa for 2 minutes, and then cooling it at 20°C under a pressure of 7.5 MPa for 5 minutes. Three of these sheets were stacked to prepare a test specimen. After 7 days or more had passed at room temperature from molding, a durometer hardness tester (D type) was used, and the indenter was brought into contact with the test piece, and the scale was immediately read (in accordance with ASTM D2240).

[0254] <Shore A hardness (instantaneous value)> A propylene-α-olefin copolymer was heated for 5 minutes using a hydraulic hot press molding machine set at 190°C, molded under a pressure of 7.5 MPa for 2 minutes, and then cooled at 20°C under a pressure of 7.5 MPa for 5 minutes to produce a sheet with a thickness of 2 mm. Three of these sheets were stacked to produce a test piece. After 7 days or more had passed at room temperature after molding, a durometer hardness tester (Type A) was used, and the indenter was brought into contact with the test piece, and the scale was read immediately (in accordance with ASTM D2240).

[0255] The propylene / α-olefin copolymers of Examples 1A to 4A have a higher breaking stress or a lower tensile modulus and are superior in balance between flexibility and strength compared to the propylene / α-olefin copolymers of Comparative Examples 1A to 2A. For example, when Examples and Comparative Examples with similar tensile modulus were compared, the Examples had a higher breaking stress and superior strength compared to the Comparative Examples.

[0256]

[0257] [Examples 1B to 5B and Comparative Examples 1B to 3B] In Examples 1B to 5B and Comparative Examples 1B to 2B, resin compositions were prepared by melt-kneading various polymers in the amounts (parts by mass) shown in Table 2 using a φ40 mm single-screw extruder (single-screw extruder) at a melt temperature of 210°C and a rotation speed of 40 to 50 rpm. In Comparative Example 3B, only propylene polymer (B-1) was used. The propylene polymer (B-1) used in the examples and comparative examples is as follows. Propylene polymer (B-1): Random polypropylene (Prime Polypro F327, manufactured by Prime Polymer Co., Ltd., MFR (230°C, 2.16 kg load): 7.0 g / 10 min, melting point: 140°C).

[0258] The tensile modulus and breaking stress were measured in the same manner as in <Tensile modulus and breaking stress> above, except that the obtained resin composition or the propylene-based polymer (B-1) was used. The results are shown in Table 2.

[0259] The resin compositions of Examples 1B to 5B have a higher breaking stress or a lower tensile modulus of elasticity than the resin compositions or propylene-based polymers of Comparative Examples 1B to 3B, and are excellent in the balance between flexibility and strength. For example, when Examples and Comparative Examples with similar breaking stresses are compared, the Examples have a lower tensile modulus of elasticity than the Comparative Examples, resulting in superior flexibility. Furthermore, when Examples and Comparative Examples with similar tensile modulus of elasticity are compared, the Examples have a higher breaking stress than the Comparative Examples, resulting in superior strength.

[0260] [Examples 1C to 7C and Comparative Examples 1C to 3C] In Examples 1C to 7C and Comparative Examples 1C to 3C, resin compositions were prepared by melt-kneading various polymers in the amounts (parts by mass) shown in Table 3 using a φ40 mm single-screw extruder (single-screw extruder) at a melt temperature of 210°C and a rotation speed of 40 to 50 rpm.

[0261] The propylene polymer (B-1), ethylene polymer (C-1), and ethylene polymer (C-2) used in the examples and comparative examples are as follows: Propylene polymer (B-1): Random polypropylene (Prime Polypro F327, manufactured by Prime Polymer Co., Ltd., MFR (230°C, 2.16 kg load): 7.0 g / 10 min, melting point: 140°C) Ethylene polymer (C-1): High-pressure low-density polyethylene (Mirason 11P, manufactured by Mitsui-Dow Polychemicals Co., Ltd., MFR (190°C, 2.16 kg load): 7.2 g / 10 min, density: 917 kg / m 3 , melting point: 108°C) Ethylene-based polymer (C-2): ethylene-propylene copolymer (MFR (190°C, 2.16 kg load): 0.6 g / 10 min, density: 869 kg / m 3 , propylene content: 19 mol%, melting point: 40°C)

[0262] <Tensile modulus and breaking stress (23°C)> The tensile modulus and breaking stress were measured in the same manner as in <Tensile modulus and breaking stress> above, except that the resin compositions obtained in the Examples and Comparative Examples were used instead of the propylene-α-olefin copolymer. The results are shown in Table 3.

[0263] <Heat Resistance (Breaking Stress (80°C))> The resin compositions obtained in the Examples or Comparative Examples were heated for 5 minutes using a hydraulic hot press molding machine set at 190°C, molded for 2 minutes under a pressure of 7.5 MPa, and then cooled at 20°C under a pressure of 7.5 MPa for 5 minutes to produce sheets (test pieces) with a thickness of 2 mm. After 7 days or more had passed at room temperature after molding, 5A-type dumbbells were produced from the sheets in accordance with JIS K7161-2, and the breaking stress of the dumbbells was measured under conditions of 80°C and a tensile speed of 500 mm / min. The obtained value was used as an index of heat resistance.

[0264] <Bleaching Resistance> The resin compositions obtained in the Examples or Comparative Examples were heated for 5 minutes using a hydraulic hot press molding machine set at 190°C, molded for 2 minutes under a pressure of 7.5 MPa, and then cooled at 20°C under a pressure of 7.5 MPa for 5 minutes to produce sheets (test pieces) with a thickness of 0.5 mm. After 7 days or more had passed at room temperature after molding, size 2 dumbbells as specified in JIS K6251 were produced from the sheets. The hue of the dumbbells before stretching (L value (before stretching)) and the hue after stretching the dumbbells by 15 mm at 23°C and a tensile speed of 50 mm / min (L value (after stretching)) were measured using a spectrophotometer (CM-3700d, manufactured by Konica Minolta, Inc.). The hue change (ΔL) was calculated based on the following formula. A smaller ΔL value indicates better blushing resistance of the resin composition. ΔL = L value (after stretching) - L value (before stretching)

[0265]

[0266] [Example 1D and Comparative Examples 1D to 2D] In Example 1D and Comparative Examples 1D to 2D, resin compositions were prepared by melt-kneading various polymers in the amounts (parts by mass) shown in Table 4 using a φ40 mm single-screw extruder (single-screw extruder) at a melt temperature of 210°C and a rotation speed of 40 to 50 rpm. Details of the various polymers used in the examples and comparative examples are as described above.

[0267] The obtained resin composition was extruded at 230 ° C. using a cast film molding machine to produce a 100 μm thick single-layer unstretched film. Next, a 25 μm thick stretched PET film (manufactured by Toray) was laminated to one surface of the obtained unstretched film by dry lamination via an adhesive layer (a polyurethane adhesive consisting of 90 parts by mass of Takelac A-525S (manufactured by Mitsui Chemicals) and 10 parts by mass of Takenate A-50 (manufactured by Mitsui Chemicals)) to produce a laminate. That is, this laminate has, in this order, a layer made of the resin composition described in Table 4, an adhesive layer, and a base layer made of a stretched PET film, with the adhesive layer being in direct contact with the layer made of the resin composition described in Table 4 and the base layer made of a stretched PET film. Using this laminate, the following evaluations were performed.

[0268] <Heat seal (HS) strength (before heat treatment)> A test specimen was prepared by stacking a 50 μm thick Teflon® sheet, two of the obtained laminates, and another 50 μm thick Teflon® sheet in this order. The two laminates were stacked such that the surfaces having the layers of the resin composition faced each other.

[0269] The heat seal bar of a heat seal tester (manufactured by Tester Sangyo Co., Ltd., TB-701B model) was adjusted to a width of 15 mm and a length of 300 mm. The temperature of the lower side of the seal bar was set to 70°C and the temperature of the upper side of the seal bar to 190°C. The test specimen was sandwiched between the seal bars and heat-sealed for 1.0 second at a pressure of 0.2 MPa. The two Teflon (registered trademark) sheets were then removed to obtain a test laminate, which was then left at 23°C for one day. A 15 mm-wide slit was made in the test laminate to include the heat-sealed portion, and the non-heat-sealed portion was chucked onto a tensile tester (manufactured by Intesco Co., Ltd., IM-20ST). The maximum load was measured when peeling the heat-sealed portion in a 180° direction at a speed of 300 mm / min. This measurement was performed five times, and the average of the maximum loads was taken as the heat-seal strength.

[0270] <Heat seal (HS) strength (after heat treatment)> The heat seal strength after heat treatment was measured in the same manner as in the test for HS strength (before heat treatment), except that in the test for HS strength (before heat treatment), a laminate obtained by heat-treating the above-mentioned monolayer unstretched film at 85°C for 5 days was used instead of the above-mentioned monolayer unstretched film.

[0271] <Heat seal (HS) strength retention> The HS strength retention was calculated from the HS strength before and after heat treatment using the following formula. The larger this value, the more excellent the heat resistance of the resin composition and its film. HS strength retention (%) = 100 × HS strength (after heat treatment) / HS strength (before heat treatment) The results are shown in Table 4.

[0272]

Claims

1. A propylene-α-olefin copolymer (A) having a structural unit (i) derived from propylene, and a structural unit (ii) derived from an α-olefin having 5 to 20 carbon atoms, which satisfies the following requirements (A1) and (A2): (A1) when the total content of the structural units (i) and (ii) is taken as 100 mol %, the content of the structural unit (i) is 70 to 99 mol %, and the content of the structural unit (ii) is 1 to 30 mol %; (A2) the melting point (Tm) measured by differential scanning calorimetry (DSC) is less than 130°C or is not observed.

2. The propylene / α-olefin copolymer (A) according to claim 1, wherein the α-olefin having 5 to 20 carbon atoms is 4-methyl-1-pentene.

3. Density, measured at 25°C in accordance with ASTM D1505, is 855-875 kg / m 3 The propylene / α-olefin copolymer (A) according to claim 2 , 4. The propylene / α-olefin copolymer (A) according to any one of claims 1 to 3, having a glass transition temperature (Tg) of -12 to -3°C.

5. The propylene / α-olefin copolymer (A) according to any one of claims 1 to 3, wherein the melting point (Tm) is less than 110°C or is not observed.

6. The propylene / α-olefin copolymer (A) according to any one of claims 1 to 3, having an intrinsic viscosity [η] in decalin solvent at 135°C of 1.8 to 2.5 dl / g.

7. The propylene / α-olefin copolymer (A) according to any one of claims 1 to 3, wherein the ratio (Mw / Mn) of the weight average molecular weight (Mw) and the number average molecular weight (Mn) calculated in terms of polystyrene, as measured by gel permeation chromatography (GPC), is 1.7 to 2.

5.

8. A resin composition comprising the propylene / α-olefin copolymer (A) according to claim 1, and a propylene-based polymer (B) satisfying the following requirements (B1) and (B2): (B1) the MFR measured in accordance with ASTM D1238E at 230°C under a load of 2.16 kg is 0.1 to 500 g / 10 min; (B2) the melting point (Tm) measured by a differential scanning calorimeter (DSC) is 110°C to 170°C.

9. The resin composition according to claim 8, wherein the α-olefin having 5 to 20 carbon atoms in the propylene / α-olefin copolymer (A) is 4-methyl-1-pentene.

10. The resin composition according to claim 8 or 9, wherein the content of said copolymer (A) is 8 to 90 mass%, and the content of said polymer (B) is 10 to 92 mass%, assuming that the total content of said copolymer (A) and said polymer (B) is 100 mass%.

11. The resin composition according to claim 8 or 9, wherein the propylene polymer (B) comprises a random polypropylene or a block polypropylene.

12. The resin composition according to claim 8, further comprising an ethylene polymer (C).

13. The resin composition according to claim 12, wherein the α-olefin having 5 to 20 carbon atoms in the propylene / α-olefin copolymer (A) is 4-methyl-1-pentene.

14. The resin composition according to claim 12 or 13, wherein the propylene polymer (B) comprises a random polypropylene or a block polypropylene.

15. The resin composition according to claim 12 or 13, wherein the ethylene polymer (C) comprises a high-pressure low-density polyethylene (c1) or an ethylene / α-olefin copolymer (c2).

16. The density of the high-pressure low-density polyethylene (c1) is 900 to 925 kg / m 3 The resin composition according to claim 15, wherein the ethylene / α-olefin copolymer (c2) has at least a structural unit derived from ethylene and a structural unit derived from an α-olefin having 3 to 20 carbon atoms, the content of the structural units derived from ethylene is 80 to 99 mol %, and the content of the structural units derived from the α-olefin having 3 to 20 carbon atoms is 1 to 20 mol %.

17. The resin composition according to claim 12 or 13, wherein, when the total content of the copolymer (A), the polymer (B) and the polymer (C) is taken as 100% by mass, the content of the copolymer (A) is 15 to 45% by mass, the content of the polymer (B) is 50 to 80% by mass, and the content of the polymer (C) is 5 to 15% by mass.

18. A molded article comprising the propylene / α-olefin copolymer (A) according to any one of claims 1 to 3, or the resin composition according to claim 8, 9, 12 or 13.

19. The molded article according to claim 18, which is a film.

20. The molded article according to claim 18, which is a packaging body for a battery.

21. An electricity storage device comprising the molded article according to claim 18.

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