Sealant resin composition and use thereof

Abstract

The purpose of the present invention is to obtain a sealant resin composition having excellent whitening resistance during stretching, good heat seal strength, and good heat seal strength after heat treatment. The present invention pertains to a sealant resin composition (X) which contains (A) a 1-butene-ethylene copolymer that satisfies specific requirements and (B) a propylene polymer, and which satisfies the following requirements (X1) and requirements (2 of X1). Requirement (X1): The Shore hardness D measured in accordance with ASTM D2240 is within the range of 44-80. Requirement (X1 2): The melt flow rate (MFR) measured at 230 DEG C under a load of 2.16 kg in accordance with ASTM D1238 is in the range of 0.1 to 100 g / 10 minutes.

Description

Technical Field

[0001] The present invention relates to a sealant resin composition comprising a 1-butene·ethylene copolymer and a propylene-based polymer and use thereof. Background Art

[0002] 1-Butene polymers are excellent in creep properties at high temperatures, wear resistance, flexibility, and compatibility with polypropylene, and are therefore used in the modification of water and hot water pipes, skin material sheets, polypropylene resins, hot melt adhesives, and the like.

[0003] Patent Document 1 proposes, as a 1-butene-based polymer having a good balance among fluidity, tensile elastic modulus and elongation, and secondary processability, a resin modifier formed from a high-fluidity 1-butene-based polymer having an intrinsic viscosity [η] measured at 135° C. in a tetralin solvent in the range of 0.01 to 0.5 dl / g, a melting point measured using a differential scanning calorimeter (DSC) in the range of 0 to 100° C., and a stereoregularity index {(mmmm) / (mmrr+rmmr)} of 30 or less, and a hot-melt adhesive containing the 1-butene-based polymer.

[0004] In addition, Patent Document 2 proposes a hot melt adhesive comprising a 1-butene copolymer having high melt fluidity, the 1-butene copolymer comprising 2 to 6 wt % of units derived from ethylene and having a melt flow rate (MFR) of 200 to 1500 when measured in accordance with ISO 1133 (190° C., 2.16 kg).

[0005] However, when a resin composition containing a 1-butene copolymer is used as a sealant, there are problems such as insufficient whitening resistance during stretching in secondary processing such as deep drawing and insufficient heat seal strength after heat treatment.

[0006] Prior art literature

[0007] Patent Literature

[0008] Patent Document 1: International Publication No. 03 / 070788 Pamphlet

[0009] Patent Document 2: Japanese Patent Application No. 2017-504667 Summary of the invention

[0010] Problems to be solved by the invention

[0011] An object of the present invention is to obtain a sealant resin composition having excellent whitening resistance during stretching, good heat seal strength, and good heat seal strength after heat treatment.

[0012] Means for solving problems

[0013] The first invention relates to a sealant resin composition (X), characterized in that it is a resin composition containing a 1-butene-ethylene copolymer (A) and a propylene-based polymer (B), and the resin composition satisfies the following requirement (X1).

[0014] Requirement (X1): The Shore D hardness measured in accordance with ASTM D2240 is within the range of 44 to 80.

[0015] The second invention relates to a sealant resin composition (X), characterized in that it is a resin composition containing a 1-butene-ethylene copolymer (A) satisfying the following requirements (A1), (A2) and (A5), and a propylene-based polymer (B), and the resin composition satisfies the following requirements (X1) and (2 of X1).

[0016] Requirement (A1): The content of the structural unit (i) derived from 1-butene is in the range of 70 to 99.9 mol %, and the content of the structural unit (ii) derived from ethylene is in the range of 0.1 to 30 mol % (wherein the total of the structural unit (i) and the structural unit (ii) is 100 mol %);

[0017] Requirement (A2): Use 13 The isotactic pentad fraction (mmmm) calculated by C-NMR is in the range of 80 to 99.9%;

[0018] Requirement (A5): Using a differential scanning calorimeter (DSC), the temperature is temporarily cooled from 30°C to -70°C at a cooling rate of 20°C / min (first cooling), then maintained at -70°C for 5 minutes, and then heated from -70°C to 200°C at a heating rate of 20°C / min (first heating), and then maintained at 200°C for 10 minutes. Then, the temperature is cooled at a cooling rate of 20°C / min to -70°C (second cooling), and then maintained at -70°C for 1 minute. Then, the temperature is again heated from -70°C to 200°C at a heating rate of 20°C / min (second heating), and no melting peak is observed during the second heating.

[0019] Requirement (X1): The Shore D hardness measured in accordance with ASTM D2240 is within the range of 44 to 80;

[0020] Requirement (2 of X1): The melt flow rate (MFR) measured at 230° C. and a load of 2.16 kg in accordance with ASTM D1238 is within the range of 0.1 to 100 g / 10 minutes.

[0021] The third invention relates to an electrical storage device comprising the sealant resin composition (X).

[0022] The sealant resin composition (X) contains a 1-butene·ethylene copolymer (A) and a propylene-based polymer (B), and satisfies the following requirement (X1).

[0023] Requirement (X1): The Shore D hardness measured in accordance with ASTM D2240 is within the range of 44 to 80.

[0024] Effects of the Invention

[0025] The single-layer or multi-layer film including a layer formed from the resin composition of the present invention has excellent whitening resistance during stretching, good heat seal strength, and good heat seal strength after heat treatment, and can therefore be suitably used as a packaging body for, for example, daily necessities, foods, liquids, medicines, electronic components, and lithium ion batteries. DETAILED DESCRIPTION

[0026] <1-Butene·ethylene copolymer (A)>

[0027] The 1-butene·ethylene copolymer (A) as one of the components of the sealant resin composition (X) of the present invention is preferably a 1-butene·ethylene copolymer (A) that satisfies the following requirements (A1) to (A5). Here, the 1-butene·ethylene copolymer (A) may satisfy only one of the following requirements (A1) to (A5), or may satisfy two or more of them, or may satisfy all of them. In one of the preferred and exemplary embodiments of the present invention, the 1-butene·ethylene copolymer (A) satisfies the following requirements (A1), (A2) and (A5). In this embodiment, the aforementioned 1-butene·ethylene copolymer (A) may also satisfy one or more requirements selected from the group consisting of the following requirements (A3), requirement (A4), and the following requirements (2 of A5) to (A8) described later.

[0028] The monomers (1-butene and ethylene) contained in the 1-butene·ethylene copolymer (A) may be monomers derived from fossil fuels or monomers derived from biomass, or a combination of monomers derived from fossil fuels and monomers derived from biomass may be used.

[0029] 〈Requirements (A1)〉

[0030] The content of the structural unit (i) derived from 1-butene is in the range of 70 to 99.9 mol %, and the content of the structural unit (ii) derived from ethylene is in the range of 0.1 to 30 mol % (wherein the total of the structural unit (i) and the structural unit (ii) is 100 mol %).

[0031] In the 1-butene·ethylene copolymer (A) of the present invention, the lower limit of the amount of the structural unit derived from 1-butene is 70 mol%. The lower limit of the structural unit is preferably 75 mol%, more preferably 80 mol%, and particularly preferably 85 mol%.

[0032] On the other hand, the upper limit of the amount of the structural unit derived from 1-butene is 99.9 mol %, preferably 98 mol %, more preferably 96 mol %, further preferably 95 mol %, and particularly preferably 94.5 mol %.

[0033] In the 1-butene·ethylene copolymer (A) according to the present invention, the upper limit of the amount of the structural unit (ii) derived from ethylene is 30 mol%. The upper limit of the structural unit is preferably 25 mol%, more preferably 20 mol%, and particularly preferably 15 mol%. When the 1-butene·ethylene copolymer (A) contains the structural unit (ii) derived from ethylene in an amount below a certain level, the obtained sealant resin composition (X) tends to easily provide a sealant film or laminate having sufficient whitening resistance and excellent surface properties.

[0034] On the other hand, the lower limit of the amount of the structural unit (ii) derived from ethylene is 0.1 mol%, preferably 2 mol%, more preferably 4 mol%, further preferably 5 mol%, and particularly preferably 5.5 mol%. If the 1-butene·ethylene copolymer (A) contains a certain amount or more of the structural unit (ii) derived from ethylene, the obtained sealant resin composition (X) tends to easily provide a sealant film or laminate having sufficient whitening resistance and high mechanical strength.

[0035] In the 1-butene·ethylene copolymer (A) according to the present invention, by making the amount of the structural unit (ii) derived from ethylene within the above range, good compatibility with the propylene-based polymer (B) described later can be obtained. If the amount of the structural unit derived from ethylene is below the upper limit, when used as a sealant, the whitening resistance during stretching in secondary processing such as deep drawing is improved, and the heat seal strength and the heat seal strength after heat treatment are excellent, which is preferred.

[0036] The content (mol %) of each structural unit constituting the 1-butene·ethylene copolymer (A) is calculated using 13 C-NMR measurement. The details of the measurement method are as described in the examples described later.

[0037] 〈Requirements (A2)〉

[0038] use 13 The isotactic pentad fraction (mmmm) calculated by C-NMR was within the range of 80 to 99.9%.

[0039] The lower limit of the isotactic pentad fraction (mmmm) of the 1-butene·ethylene copolymer (A) of the present invention is preferably 85%, more preferably 90%. In addition, the upper limit of the isotactic pentad fraction (mmmm) is preferably 99.5%, more preferably 99.0%. By making the isotactic pentad fraction (mmmm) within the above range, even when ethylene is copolymerized to control the compatibility with the propylene polymer (B) described later, it is possible to design appropriate mechanical strength and flexibility.

[0040] In addition, the details of the method for measuring the isotactic pentad fraction (mmmm) are as described in the later-mentioned Examples.

[0041] 〈Requirements (A3)〉

[0042] The intrinsic viscosity [η] in decalin solvent at 135°C is within the range of 0.7 to 4.0 dl / g.

[0043] The intrinsic viscosity [η] of the 1-butene·ethylene copolymer (A) of the present invention is more preferably 0.8 to 3.0 dl / g, further preferably 0.9 to 2.5 dl / g, and particularly preferably 1.0 to 2.2 dl / g. The 1-butene·ethylene copolymer (A) having an intrinsic viscosity [η] within the above range has an excellent balance between fluidity and the mechanical strength of the resulting sealant.

[0044] The details of the method for measuring the intrinsic viscosity [η] are as described in the examples described later.

[0045] 〈Requirements(A4)〉

[0046] The melt flow rate (MFR) measured in accordance with ASTM D1238 at 190°C and a load of 2.16 kg is in the range of 0.1 to 100 g / 10 minutes, preferably in the range of 0.5 to 50 g / 10 minutes, more preferably in the range of 1.0 to 30 g / 10 minutes, further preferably in the range of 1.1 to 20 g / 10 minutes, further preferably in the range of 1.1 to 5 g / 10 minutes, and particularly preferably in the range of 1.1 to 3.5 g / 10 minutes.

[0047] When the MFR is within the above range, the fluidity is good, and the mechanical properties of the obtained sealant are good. For example, for the sealant resin composition (X) containing 1-butene·ethylene copolymer (A), when high fluidity is required, the melt flow rate (MFR) measured at 230°C and 2.16 kg load according to ASTM D1238 is particularly preferably in the range of 3 to 80 g / 10 minutes. In addition, a sealant with excellent mechanical properties can be easily obtained. In addition, considering the balance between fluidity and mechanical properties suitable for a film forming machine, it is particularly preferably 15 g / 10 minutes or less.

[0048] When the MFR is above the lower limit, the drawdown during film molding is good and the film forming property is suitable for high speed. When the MFR is below the upper limit, the mechanical properties of the 1-butene·ethylene copolymer (A) are excellent, and the sealant resin composition (X) containing the 1-butene·ethylene copolymer (A) is excellent in heat sealing strength, whitening resistance, and durability, so it is preferred.

[0049] 〈Requirements(A5)〉

[0050] In the calorimetry using a differential scanning calorimeter (DSC), no melting peak was observed at the second temperature increase.

[0051] The calorimetric measurement using a differential scanning calorimeter (DSC) in the present invention is performed as follows: about 6 to 10 mg of a sample is accurately weighed, sealed in an aluminum pan, temporarily cooled (first cooling) to -70°C, then heated from -70°C to 200°C at a heating rate of 20°C / min (first heating), and a DSC curve is measured. After holding at 200°C for 10 minutes, the temperature is then cooled to -70°C at a cooling rate of 20°C / min (second cooling), and a DSC curve is measured. After holding at -70°C for 1 minute, the temperature is again increased from -70°C to 200°C at a heating rate of 20°C / min (second heating), and a DSC curve is measured. In an exemplary embodiment of the present invention, the first cooling performed before the first heating is performed by temporarily cooling from 30°C to -70°C at a cooling rate of 20°C / min, and after the first cooling, the temperature is held at -70°C for 5 minutes, and then the first heating is performed.

[0052] Furthermore, in the aforementioned DSC curve, when an endothermic peak (melting peak) due to melting is observed during the aforementioned first temperature increase, the temperature at which the melting peak (hereinafter, referred to as "melting peak P1") is observed is set to Tm1. When a melting peak is observed during the aforementioned second temperature increase, the temperature at which the melting peak (hereinafter, referred to as "melting peak P2") is observed is set to Tm2.

[0053] In the present invention, “no melting peak is observed during the second temperature increase” means that the melting peak P2, that is, Tm2, ​​is not observed during the second temperature increase.

[0054] In this specification, the melting peak is measured by the determination method recorded in the previous text, and the melting point refers to the temperature at which the melting peak is observed, specifically the temperature at the peak top of the melting peak, and the so-called failure to observe the melting peak refers to the failure to observe the crystal melting peak with a crystal melting enthalpy of 1 J / g or more. It should be noted that, when more than two melting peaks are observed, the highest temperature among the temperatures at the peak tops of these peaks is the melting point.

[0055] 〈Requirements (A5 2)〉

[0056] In addition to the above requirements (A1) to (A5), the 1-butene·ethylene copolymer (A) according to the present invention preferably has a melting point (Tm) of 70°C or less, more preferably 66°C or less, as measured at the first temperature rise of a differential scanning calorimeter (DSC). On the other hand, the melting point (Tm) is preferably 40°C or more, more preferably 44°C or more. For example, the melting point (Tm) is preferably 40 to 70°C, more preferably 44 to 66°C.

[0057] When the melting point (Tm) is below the upper limit, the crystallinity is low and the flexibility is excellent. When the melting point is above the lower limit, the mechanical properties are excellent and the heat seal strength is improved. When the melting point (Tm) is within the above range, the flexibility and low tackiness are well balanced.

[0058] Here, the "melting point (Tm) measured at the first temperature rise of a differential scanning calorimeter (DSC)" can be measured by the "calorimetric measurement using a differential scanning calorimeter (DSC)" stated in the aforementioned "Requirement (A5)". In this case, the temperature Tm1 of the melting peak P1 observed at the first temperature rise is set as Tm.

[0059] 〈Requirements (A5 3)〉

[0060] With respect to the 1-butene·ethylene copolymer (A) of the present invention, in addition to the above-mentioned requirements (A1) to (A5) (or, the above-mentioned requirements (A1) to (2 of A5)), the melting enthalpy measured in the first temperature rise of the differential scanning calorimeter (DSC) is preferably 1 to 60 J / g, and more preferably 2 to 50 J / g. The melting enthalpy is an indicator of crystallinity. When the melting enthalpy is below the upper limit, the crystallinity is low and the flexibility is excellent. When the melting enthalpy is above the lower limit, the mechanical properties are excellent and the heat sealing strength is improved. When the melting enthalpy is within the above-mentioned range, the flexibility and low tackiness are well balanced and excellent.

[0061] Here, the “melting enthalpy measured in the first temperature rise of a differential scanning calorimeter (DSC)” can be measured by the “calorimetric measurement using a differential scanning calorimeter (DSC)” stated in the aforementioned “requirement (A5)”, and the melting enthalpy obtained for the aforementioned melting peak P1 is taken as the “melting enthalpy measured in the first temperature rise of a differential scanning calorimeter (DSC)”.

[0062] The fact that a melting peak was observed at the first temperature increase, but no melting peak was observed at the second temperature increase despite the presence of crystallinity, indicates that the crystallization rate of the 1-butene·ethylene copolymer (A) is extremely slow.

[0063] 〈Requirements(A6)〉

[0064] The 1-butene-ethylene copolymer (A) according to the present invention preferably satisfies, in addition to the above requirements (A1) to (A5) (or the above requirements (A1) to (3) of A5),

[0065] (A6): The weight average molecular weight (Mw) is 100,000 to 550,000.

[0066] When fluidity is required, the weight average molecular weight (Mw) of the 1-butene·ethylene copolymer (A) is more preferably 100,000 to 520,000, further preferably 100,000 to 500,000, and particularly preferably 100,000 to 490,000. When the weight average molecular weight (Mw) is within the aforementioned range, the sealant resin composition containing the 1-butene·ethylene copolymer (A) is suitable for high-speed moldability. However, the weight average molecular weight (Mw) of the 1-butene·ethylene copolymer (A) may sometimes exceed 550,000. For example, when the mechanical strength of the sealant is required, the weight average molecular weight (Mw) is more preferably 150,000 to 600,000, further preferably 200,000 to 600,000, and particularly preferably 202,000 to 600,000. When the weight average molecular weight (Mw) is within the aforementioned range, a sealant with excellent mechanical properties can be easily obtained.

[0067] 〈Requirements (A6 2)〉

[0068] Furthermore, the molecular weight distribution (Mw / Mn) of the 1-butene·ethylene copolymer (A) of the present invention is preferably 1.5 to 3.0, and more preferably 1.6 to 2.8. Mw / Mn is a value measured by the GPC method and converted to polystyrene. The 1-butene·ethylene copolymer (A) having Mw / Mn within the above range is preferred because it contains less low molecular weight components that reduce mechanical strength and less high molecular weight components that deteriorate fluidity.

[0069] <Requirements (A7) and (A8)>

[0070] The 1-butene-ethylene copolymer (A) according to the present invention preferably satisfies, in addition to the above requirements (A1) to (A5) (or 2 of the above requirements (A1) to (A6)),

[0071] Requirement (A7): The maximum value of Shore A hardness (according to ASTM D2244) is 70 to 99, or

[0072] Requirement (A8): The maximum value of Shore D hardness (according to ASTM D2244) is 20 to 70.

[0073] A more preferred range of Shore hardness A is 75 to 98. A more preferred range of Shore hardness D is 25 to 65. Shore hardness A or Shore hardness D is an index of crystallinity. When Shore hardness A or Shore hardness D is below the upper limit, a sealant having low crystallinity, excellent flexibility, and excellent whitening resistance during stretching can be easily obtained. When Shore hardness A or Shore hardness D is above the lower limit, a sealant having excellent mechanical properties can be easily obtained.

[0074] The 1-butene·ethylene copolymer (A) may satisfy only one of the requirements (A7) and (A8), or may satisfy both the requirements (A7) and (A8).

[0075] <Method for producing 1-butene / ethylene copolymer (A)>

[0076] The 1-butene·ethylene copolymer (A) of the present invention can be prepared by polymerizing the monomers by a known polymerization method such as a gas phase method, a bulk method, or a slurry method in the presence of a catalyst such as a Ziegler-Natta catalyst or a metallocene catalyst. Among them, from the viewpoint of obtaining a sealant resin composition having a narrow molecular weight distribution and a composition distribution of the polymer and excellent balance between mechanical strength and flexibility, and obtaining good compatibility when combined with the propylene polymer (B) described later, it is preferred to use a metallocene catalyst capable of uniformly controlling the reaction, and it is particularly preferred to use a metallocene compound represented by the following general formula (1) or (2) for polymerization.

[0077] [Chemical formula 1]

[0078]

[0079] [Chemical formula 2]

[0080]

[0081] R in the above general formula (1) or (2) 1 , R 2 , R 3 , R 4, R 5 , R 6 , R 7 , R 8 , R 9 , R 10 , R 11 , R 12 It is selected from hydrogen, a hydrocarbon group, and a silicon-containing hydrocarbon group, and each of them may be the same or different.

[0082] The hydrocarbon group is preferably an alkyl group having 1 to 20 carbon atoms, an arylalkyl group having 7 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, or an alkylaryl group having 7 to 20 carbon atoms, and may contain one or more ring structures. Specific examples thereof include methyl, ethyl, n-propyl, isopropyl, 2-methylpropyl, 1,1-dimethylpropyl, 2,2-dimethylpropyl, 1,1-diethylpropyl, 1-ethyl-1-methylpropyl, 1,1,2,2-tetramethylpropyl, sec-butyl, tert-butyl, and the like.

[0083] The silicon-containing hydrocarbon group is preferably an alkylsilyl group or arylsilyl group having 1 to 4 silicon atoms and 3 to 20 carbon atoms, and specific examples thereof include a trimethylsilyl group, a tert-butyldimethylsilyl group, and a triphenylsilyl group.

[0084] It should be noted that R 2 Preferably, it is a hydrocarbon group that is bulky on the steric level, a silicon-containing hydrocarbon group, that is, a secondary or tertiary substituent, and more preferably a substituent having 4 or more carbon atoms. Specific examples of hydrocarbon groups include isopropyl, 1,1-dimethylpropyl, 1,1-diethylpropyl, 1-ethyl-1-methylpropyl, 1,1,2,2-tetramethylpropyl, sec-butyl, tert-butyl, 1,1-dimethylbutyl, etc. Tert-butyl is particularly preferred. Examples of silicon-containing hydrocarbon groups include compounds in which a portion or all of the carbon in the above compounds is replaced by silicon.

[0085] R on the fluorene ring 5 To R 12 Adjacent substituents may be bonded to each other to form a ring. Examples of such substituted fluorenyl groups include benzofluorenyl and dibenzofluorenyl. 5 To R 12 The substituents are preferably bilaterally symmetrical, that is, R 5 =R 12 , R 6 =R 11 , R 7 =R 10 , R 8 =R 9, more preferably unsubstituted fluorene, 3,6-disubstituted fluorene, 2,7-disubstituted fluorene or 2,3,6,7-tetrasubstituted fluorene. Here, the 3-position, 6-position, 2-position and 7-position on the fluorene ring correspond to R 7 , R 10 , R 6 , R 11 .

[0086] R in the above general formula (1) 3 and R 4 are selected from hydrogen and hydrocarbon groups, and each may be the same or different. Specific examples of preferred hydrocarbon groups include the same groups as above. Y is carbon or silicon. In the case of general formula (1), R 3 and R 4 It is bonded to Y to form a substituted methylene group or a substituted silylene group as a crosslinking portion. Preferred specific examples include methylene, dimethylmethylene, diisopropylmethylene, methyl-tert-butylmethylene, dicyclohexylmethylene, methylcyclohexylmethylene, methylphenylmethylene, diphenylmethylene, dimethylsilylene, and diisopropylsilylene. More preferably, Y is carbon.

[0087] R in the general formula (1) or (2) 2 When it is tert-butyl, R 1 It is preferably a methyl group or an ethyl group, and more preferably a methyl group. 3 , R 4 is methyl or phenyl, preferably methyl. 3 , R 4 Preferably, they are the same as each other. 2 is tert-butyl, R 1 When it is methyl, R 5 ~R 12 It may be hydrogen.

[0088] In addition, R in the above general formula (1) 2 is tert-butyl, R 1 When it is ethyl, it is preferred to use R 5 , R 7 , R 8 , R 9 , R 10 , R 12 is hydrogen, R 6 , R 11 It is a tert-butyl compound.

[0089] In the case of general formula (2), Y is bonded to a divalent hydrocarbon group A having 2 to 20 carbon atoms which may contain an unsaturated bond and / or an aromatic ring, to form a cycloalkylene group or a cyclomethylenesilylene group. Preferred specific examples include cyclopropylene, cyclobutylene, cyclopentylene, and cyclohexylene.

[0090] M in the general formula (1) and (2) is a metal selected from Group 4 of the periodic table, and examples of M include titanium, zirconium, and hafnium. Q can be selected from halogens, hydrocarbon groups having 1 to 20 carbon atoms, anionic ligands, or neutral ligands that can coordinate with lone pairs of electrons in the same or different combinations. Specific examples of halogens include fluorine, chlorine, bromine, and iodine, and specific examples of hydrocarbon groups include the same hydrocarbon groups as mentioned above. Specific examples of anionic ligands include alkoxy groups such as methoxy, tert-butoxy, and phenoxy, carboxylate groups such as acetate, benzoate, and sulfonate groups such as mesylate and tosylate. Specific examples of neutral ligands that can coordinate with lone pairs of electrons include organic phosphorus compounds such as trimethylphosphine, triethylphosphine, triphenylphosphine, and diphenylmethylphosphine, or ethers such as tetrahydrofuran, diethyl ether, dioxane, and 1,2-dimethoxyethane. Among these, Q may be the same or may be a combination of different ones, but it is preferred that at least one of them is a halogen or an alkyl group.

[0091] Component (C) is composed of at least one compound (C-3) selected from the group consisting of an organoaluminum oxy-compound (C-1), a compound (C-2) that reacts with the metallocene compound (A) to form an ion pair, and an organoaluminum compound, and optionally, a particulate support (D).

[0092] As the organoaluminum oxy-compound (C-1) which can be used, a conventionally known aluminoxane can be used as it is.

[0093] As the compound (C-2) that reacts with the metallocene compound (A) to form an ion pair (hereinafter, sometimes referred to as "ionic compound"), Lewis acids, ionic compounds, borane compounds and carborane compounds described in Japanese Unexamined Patent Publication No. 1-501950 and Japanese Unexamined Patent Publication No. 2004-51676 can be mentioned. In addition, heteropoly compounds and isopoly compounds can also be mentioned.

[0094] Specifically, examples include triphenylboron, tri(o-tolyl)boron, tri(p-tolyl)boron, tri(3,5-dimethylphenyl)boron, trimethylboron, triisobutylboron; compounds having a fluorine-containing aromatic group such as tri(4-fluorophenyl)boron, tri(3,5-difluorophenyl)boron, tri(4-fluoromethylphenyl)boron, tri(pentafluorophenyl)boron; and compounds having a halogen-containing aromatic group; boron trifluoride.

[0095] Examples of the organoaluminum compound (C-3) as a polymerization catalyst for olefin formation include organoaluminum compounds represented by the following general formula (3).

[0096] Ra m Al(ORb) n H p Qq ···the organoaluminum compound represented by (3)

[0097] (In the formula, Ra and Rb may be the same or different from each other, and represent a hydrocarbon group having 1 to 15 carbon atoms, preferably 1 to 4 carbon atoms, Q represents a halogen atom, m is a number of 0 < m ≤ 3, n is a number of 0 ≤ n < 3, p is a number of 0 ≤ p < 3, q is a number of 0 ≤ q < 3, and m + n + p + q = 3.).

[0098] Specific examples of such compounds include trialkylaluminums such as trimethylaluminum, triethylaluminum, tri-n-butylaluminum, and triisobutylaluminum; dialkylaluminum hydrides such as diisopropylaluminum hydride and diisobutylaluminum hydride; and alkylalkoxyaluminums such as isobutylaluminum methoxide and isobutylaluminum ethoxide, etc.

[0099] As the organoaluminum compound (C-3), tri-n-alkylaluminums such as trimethylaluminum, triethylaluminum, and trioctylaluminum, and tri-branched alkylaluminums such as triisobutylaluminum are preferred, and trimethylaluminum and triisobutylaluminum are particularly preferably used.

[0100] In the present invention, the polymerization of the 1-butene·ethylene copolymer (A) can be carried out by any method among solution polymerization, suspension polymerization and other liquid phase polymerization methods or gas phase polymerization methods. In the liquid phase polymerization method, an inert hydrocarbon solvent can be used. Specifically, aliphatic hydrocarbons such as propane, butane, pentane, hexane, heptane, octane, and decane; cycloaliphatic hydrocarbons such as cyclopentane, cyclohexane, and methylcyclopentane; aromatic hydrocarbons such as benzene, toluene, and xylene, or mixtures thereof, etc. can be cited. In addition, bulk polymerization in which the olefin itself containing 1-butene is used as a solvent can also be carried out.

[0101] When carrying out the polymerization, component (A) is usually 10 -8 to 10 -2 moles, preferably 10 -7 to 10 -3 moles in terms of the Group 4 metal atom of the periodic table per 1 liter of the reaction volume. Component (C-1) is used in such an amount that the molar ratio [(C-1) / M] of component (C-1) to the transition metal atom (M) in component (A) is usually 0.01 to 5000, preferably 0.05 to 2000. Component (C-2) is used in such an amount that the molar ratio [(C-2) / M] of component (C-2) to the transition metal atom (M) in component (A) is usually 1 to 10, preferably 1 to 5. Component (C-3) is used in such an amount that the molar ratio [(C-2) / M] of component (C-3) to the transition metal atom (M) in component (A) is usually 10 to 5000, preferably 20 to 2000.

[0102] The polymerization temperature is usually in the range of -50 to 200° C., preferably 0 to 100° C., more preferably 20 to 100° C. If the polymerization temperature is too low, it tends to be industrially disadvantageous in terms of polymerization activity per unit catalyst, heat recovery efficiency, and the like.

[0103] The polymerization pressure is usually normal pressure to 10 MPa gauge pressure, preferably normal pressure to 5 MPa gauge pressure, and the polymerization reaction can be carried out in any of batch, semi-continuous, and continuous methods. In addition, the polymerization can be carried out in two or more steps under different reaction conditions.

[0104] Hydrogen may be added for the purpose of controlling the molecular weight and polymerization activity of the 1-butene·ethylene copolymer (A) produced during polymerization. The appropriate amount of hydrogen is about 0.001 to 100 NL per 1 kg of the 1-butene·ethylene copolymer (A).

[0105] <Propylene polymer (B)>

[0106] The propylene-based polymer (B) as one of the components contained in the sealant resin composition (X) of the present invention is preferably a propylene-based polymer (B-1) satisfying the following requirements (B1) and (B2).

[0107] 〈Requirements (B1)〉

[0108] The melting point measured by a differential scanning calorimeter is in the range of 100 to 170°C, more preferably 130 to 170°C, and further preferably 132 to 150°C.

[0109] The sealant resin composition containing the propylene-based polymer (B) having a melting point within the above range exhibits excellent heat resistance, has good transparency, and has a moderately slow crystallization rate.

[0110] 〈Requirements (B2)〉

[0111] The isotactic pentad fraction (mmmm) is in the range of 80 to 99.9%, more preferably 85 to 99.9%, further preferably 90 to 99.9%.

[0112] The sealant resin composition (X) containing the propylene polymer (B) having an isotactic pentad fraction (mmmm) satisfying the above range has good heat seal strength.

[0113] The propylene polymer (B) according to the present invention preferably satisfies at least one of the following requirements (B3) and (B4) in addition to the above requirements (B1) and (B2), and more preferably satisfies both (B3) and (B4).

[0114] 〈Requirements (B3)〉

[0115] The crystallization temperature is in the range of 40 to 120°C, preferably 60 to 120°C, more preferably 80 to 120°C.

[0116] When the crystallization temperature of the propylene polymer (B) according to the present invention is within the above range, the heat seal strength of the sealant resin composition (X) containing the propylene polymer (B) is good, which is preferred from the viewpoint of heat resistance.

[0117] Regarding the crystallization temperature of the propylene polymer (B) according to the present invention, the temperature of the peak observed in the second temperature drop process of the differential scanning calorimeter (DSC) is taken as the crystallization temperature. Here, the measurement of the propylene polymer (B) by the differential scanning calorimeter (DSC) can be carried out in the same manner as the "calorimetric measurement by the differential scanning calorimeter (DSC)" stated in the aforementioned "requirement (A5)", and when an exothermic peak due to crystallization is observed during the temperature drop (second temperature drop) between the aforementioned first temperature rise and the aforementioned second temperature rise, the temperature at which the exothermic peak is observed is taken as the aforementioned crystallization temperature.

[0118] 〈Requirements(B4)〉

[0119] The melt flow rate (MFR) measured under the conditions of a temperature of 230°C and a load of 2.16 kg is preferably in the range of 0.1 to 150 g / 10 minutes, more preferably in the range of 0.5 to 100 g / 10 minutes, further preferably in the range of 1 to 50 g / 10 minutes, and particularly preferably in the range of 2 to 25 g / 10 minutes.

[0120] When the MFR is within the above range, the obtained sealant resin composition (X) has good moldability and is excellent in heat seal strength.

[0121] The propylene polymer (B) of the present invention may be a propylene homopolymer or a copolymer of propylene and at least one α-olefin having 2 to 20 carbon atoms other than propylene. Here, examples of the α-olefin having 2 to 20 carbon atoms other than propylene include ethylene, 1-butene, 1-pentene, 1-hexene, 4-methyl-1-pentene, 1-octene, 1-decene, 1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene, 1-eicosene, etc., and ethylene or an α-olefin having 4 to 10 carbon atoms is preferred.

[0122] The copolymer of propylene and these α-olefins may be a random copolymer (random polypropylene) or a block copolymer (block polypropylene). The copolymer of α-olefin and propylene may contain structural units derived from these α-olefins in a ratio of 35 mol % or less, preferably 30 mol % or less.

[0123] The propylene polymer (B) preferably contains one or more selected from the group consisting of random copolymers and block copolymers. Such a propylene polymer (B) is preferably a random copolymer, a block copolymer, or a combination of a random copolymer and a block copolymer, and more preferably a random copolymer.

[0124] In addition, the aforementioned propylene-based polymer (B) may be a single type or a combination of two or more types. For example, it may be composed only of a propylene-based polymer (B-1) satisfying the aforementioned requirements (B1) and (B2), or it may be a combination of the propylene-based polymer (B-1) and a propylene-based polymer (B-2) that does not satisfy either or both of the aforementioned requirements (B1) and (B2).

[0125] The monomers contained in the propylene-based polymer (B) (propylene and α-olefins having 2 to 20 carbon atoms other than propylene) may be monomers derived from fossil fuels or monomers derived from biomass, or a combination of monomers derived from fossil fuels and monomers derived from biomass may be used.

[0126] The method for producing the propylene polymer (B) according to the present invention is not particularly limited, and examples thereof include known methods using known catalysts such as Ziegler-Natta catalysts and metallocene catalysts.

[0127] <Ethylene polymer (C)>

[0128] The sealant resin composition (X) of the present invention may further contain an ethylene polymer (C). The ethylene polymer (C) contains 60 to 100 mol% of structural units derived from ethylene. Specific examples of the ethylene polymer (C) of the present invention include high pressure low density polyethylene (C1) and ethylene α-olefin copolymer (C2).

[0129] By using the ethylene polymer (C), the obtained sealant resin composition (X) can easily provide an excellent sealant having particularly good balance between impact resistance and transparency.

[0130] The monomers (ethylene and α-olefins having 3 to 20 carbon atoms) contained in the ethylene-based polymer (C) may be monomers derived from fossil fuels or monomers derived from biomass, or a combination of monomers derived from fossil fuels and monomers derived from biomass may be used.

[0131] <<High Pressure Low Density Polyethylene (C1)>>

[0132] As the high pressure low density polyethylene (C1), known high pressure low density polyethylene can be used without limitation. The so-called high pressure low density polyethylene is generally polyethylene obtained by subjecting ethylene to free radical polymerization under high temperature and pressure. There are no particular limitations on its production method, and examples thereof include free radical polymerization methods in which free radical polymerization is carried out under conditions of 500 to 2000 atmospheres and 150 to 300° C., and here, as the polymerization initiator, for example, organic peroxides can be cited.

[0133] The density of the high pressure low density polyethylene (C1) measured in accordance with ASTM D1505 is preferably 900 to 925 kg / m 3 The range of is more preferably 910 to 925 kg / m 3 .

[0134] When the density is not less than the lower limit, the adhesive resistance is excellent, and when it is not more than the upper limit, the flexibility is excellent.

[0135] The melt flow rate (MFR) of the high-pressure low-density polyethylene (C1) measured at 190°C and 2.16 kg load in accordance with ASTM D1238 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, preferably 50 g / 10 min or less, more preferably 30 g / 10 min or less, particularly preferably 20 g / 10 min or less.

[0136] When the MFR is at least the lower limit value, the film-forming property is excellent, and when it is at most the upper limit value, the heat resistance is excellent.

[0137] The melting point of the high pressure low density polyethylene (C1) measured by a differential scanning calorimeter (DSC) is preferably 104 to 130°C, more preferably 105 to 125°C, and further preferably 106 to 120°C.

[0138] When the melting point is at least the lower limit value, the resistance to tackiness and heat resistance are excellent, and when it is at most the upper limit value, the flexibility is excellent.

[0139] <<Ethylene·α-olefin copolymer (C2)>>

[0140] The ethylene·α-olefin copolymer (C2) contains at least a structural unit derived from ethylene and a structural unit derived from an α-olefin having 3 to 20 carbon atoms.

[0141] The content of the structural unit derived from ethylene in the ethylene / α-olefin copolymer (C2) is 60 to 99 mol%, preferably 65 to 99 mol%, more preferably 70 to 99 mol%, particularly preferably 80 to 99 mol%.

[0142] When the ethylene content is at least the lower limit value, the adhesiveness resistance and heat resistance are excellent, and when it is at most the upper limit value, the flexibility is excellent.

[0143] The ethylene / α-olefin copolymer (C2) is characterized in that it has fewer long-chain branch structures than the high-pressure low-density polyethylene (C1), and is sometimes generally referred to as linear low-density polyethylene (LLDPE).

[0144] The content of the structural unit derived from α-olefin having 3 to 20 carbon atoms in the ethylene·α-olefin copolymer (C2) is 1 to 40 mol %, preferably 1 to 35 mol %, more preferably 1 to 30 mol %, particularly preferably 1 to 20 mol %.

[0145] When the content of the α-olefin having 3 to 20 carbon atoms is at least the lower limit, the flexibility and impact resistance are excellent, and when it is at most the upper limit, the stickiness resistance and heat resistance are excellent.

[0146] The contents thereof are amounts relative to 100 mol% of the total of structural units derived from ethylene and α-olefins having 3 to 20 carbon atoms.

[0147] When the content of the structural unit is within the above range, a sealant having excellent impact resistance and flexibility with a good balance can be easily obtained.

[0148] Examples of the α-olefin 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-olefin having 3 to 10 carbon atoms is preferred, α-olefin having 3 to 8 carbon atoms is more preferred, propylene, 1-butene, and 1-octene are further preferred, and propylene is particularly preferred.

[0149] The aforementioned α-olefins having 3 to 20 carbon atoms may be used alone or in combination of two or more.

[0150] The ethylene / α-olefin copolymer (C2) may contain, in addition to the aforementioned structural units, one or two or more structural units derived from other polymerizable monomers within a range not impairing the purpose of the present invention.

[0151] Examples of such other polymerizable monomers include vinyl compounds such as styrene, vinylcyclopentene, vinylcyclohexane, and vinyl norbornene; vinyl esters such as vinyl acetate; unsaturated organic acids such as maleic anhydride or their derivatives; and non-conjugated polyenes such as dicyclopentadiene, cyclohexadiene, and 5-ethylidene-2-norbornene.

[0152] Specific examples of the ethylene α-olefin copolymer (C2) include ethylene propylene copolymers, ethylene 1-butene copolymers, ethylene propylene 1-butene copolymers, ethylene propylene ethylidene norbornene copolymers, ethylene 1-butene 1-octene copolymers, ethylene 4-methyl-1-pentene copolymers, ethylene 1-hexene copolymers, and ethylene 1-octene copolymers. Among these, for example, ethylene propylene copolymers and ethylene 1-butene copolymers are preferred.

[0153] The density of the ethylene·α-olefin copolymer (C2) is preferably 840 kg / m 3 More preferably 850kg / m 3 Above, particularly preferably 855 kg / m 3 Above, preferably 940kg / m 3 Below, more preferably 899kg / m 3 Below, more preferably 890kg / m 3 Below, particularly preferably 885kg / m 3 the following.

[0154] When the density is within the above range, a sealant resin composition having excellent impact resistance, rigidity, and transparency in a well-balanced manner can be easily obtained.

[0155] The density can be measured using the density gradient tube method.

[0156] The MFR (measured in accordance with ASTM D1238 at 190°C and a load of 2.16 kg) 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, preferably 40 g / 10 min or less, more preferably 20 g / 10 min or less, particularly preferably 10 g / 10 min or less.

[0157] When the MFR is within the above range, a sealant resin composition having excellent impact resistance, rigidity, and transparency in a well-balanced manner can be easily obtained.

[0158] The MFR of the ethylene·α-olefin copolymer (C2) measured in accordance with ASTM D1238 at 190°C and a load of 10 kg is 10 , and the ratio of MFR2 measured at 190°C and load 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.

[0159] MFR 10When / MFR2 is within the above range, a sealant resin composition having excellent transparency and impact resistance well-balanced can be easily obtained.

[0160] The ethylene·α-olefin copolymer (C2) can be produced by a conventionally known method using a vanadium-based catalyst, a titanium-based catalyst or a metallocene-based catalyst, etc. It is preferably produced using a metallocene-based catalyst, which can obtain a copolymer with a narrow molecular weight distribution and composition distribution, which is more preferred from the perspectives of mechanical properties, transparency and impact resistance.

[0161] The melting point of the ethylene / α-olefin copolymer (C2) measured by a differential scanning calorimeter (DSC) is preferably 30 to 100°C, more preferably 31 to 90°C, and further preferably 32 to 80°C.

[0162] When the melting point is within the above range, a sealant resin composition having excellent well-balanced transparency and impact resistance can be easily obtained.

[0163] <Sealing agent resin composition (X)>

[0164] The sealant resin composition (X) of the present invention is a resin composition comprising the above-mentioned 1-butene·ethylene copolymer (A) and a propylene-based polymer (B), and the composition satisfies the following requirements (X1) and (2 of X1).

[0165] 〈Requirements (X1)〉

[0166] The Shore D hardness measured according to ASTM D2240 is in the range of 44-80, preferably in the range of 44-71.

[0167] The sealant resin composition having a Shore hardness D satisfying the above range becomes a sealant that is soft and has excellent mechanical properties.

[0168] 〈Requirements (X1 of 2)〉

[0169] The melt flow rate (MFR) of the sealant resin composition (X) of the present invention measured at 230°C and under a load of 2.16 kg in accordance with ASTM D1238 is not particularly limited, but is, for example, in the range of 0.1 to 100 g / 10 minutes, more preferably in the range of 1 to 30 g / 10 minutes.

[0170] When the MFR of the sealant resin composition (X) of the present invention measured at 230° C. and under a load of 2.16 kg is within the above range, the sealant has good moldability and good mechanical properties.

[0171] In particular, when fluidity is required, the MFR is preferably 20 to 100 g / 10 min, more preferably 20 to 50 g / 10 min. However, even when high fluidity is required, the MFR may preferably be 3 to 80 g / 10 min.

[0172] When excellent mechanical strength is required, the MFR is preferably 1 g / 10 minutes or more and less than 20 g / 10 minutes.

[0173] The sealant resin composition (X) of the present invention may further contain the ethylene polymer (C) as required in addition to the 1-butene·ethylene copolymer (A) and the propylene polymer (B).

[0174] Examples of the sealant resin composition (X) of the present invention include: a composition comprising a 1-butene·ethylene copolymer (A) and a propylene-based polymer (B); a composition comprising a 1-butene·ethylene copolymer (A), a propylene-based polymer (B), and a high-pressure low-density polyethylene (C1); a composition comprising a 1-butene·ethylene copolymer (A), a propylene-based polymer (B), and an ethylene·α-olefin copolymer (C2); and a composition comprising a 1-butene·ethylene copolymer (A), a propylene-based polymer (B), a high-pressure low-density polyethylene (C1), and an ethylene·α-olefin copolymer (C2).

[0175] The sealant resin composition (X) of the present invention preferably satisfies any one or two or more of the following (X2), (X3) and (X4) in addition to the above (X1) and (2) of (X1).

[0176] 〈Requirements (X2)〉

[0177] Using a differential scanning calorimeter (DSC), the temperature is temporarily lowered (first temperature reduction) to -70°C, then the temperature is increased from -70°C to 200°C at a heating rate of 20°C / min (first temperature increase), and after being maintained at 200°C for 10 minutes, the temperature is then lowered to -70°C at a cooling rate of 20°C / min (second temperature reduction), and after being maintained at -70°C for 1 minute, the temperature is again increased from -70°C to 200°C at a heating rate of 20°C / min (second temperature increase), and the melting enthalpy ΔHfus generated at this time is in the range of 20 to 100 J / g. In an exemplary embodiment of the present invention, the aforementioned first temperature reduction performed before the first temperature increase is performed by temporarily cooling from 30°C to -70°C at a cooling rate of 20°C / min, and after the first temperature reduction, it is maintained at -70°C for 5 minutes, and then the aforementioned first temperature increase is performed.

[0178] 〈Requirements (X3)〉

[0179] The content of the 1-butene·ethylene copolymer (A) is in the range of 1 to 50% by mass, the content of the propylene polymer (B) is in the range of 30 to 99% by mass, and the content of the ethylene polymer (C) is in the range of 0 to 20% by mass (wherein the total of the 1-butene·ethylene copolymer (A), the propylene polymer (B), and the ethylene polymer (C) is set to 100% by mass).

[0180] 〈Requirements (X4)〉

[0181] The Young's modulus (YM) measured in accordance with ASTM D638 is 1100 MPa or less, preferably 10 to 1100 MPa, more preferably 100 to 1050 MPa, and further preferably 200 to 1000 MPa. The Young's modulus is also called tensile elastic modulus.

[0182] When the Young's modulus is equal to or less than the upper limit, a sealing agent having excellent flexibility and excellent whitening resistance during stretching can be easily obtained. When the Young's modulus is equal to or more than the lower limit, a sealing agent having excellent mechanical properties and heat resistance can be easily obtained.

[0183] In addition, in the sealant resin composition (X) of the present invention, the 1-butene-ethylene copolymer (A) contained in the sealant resin composition (X) may satisfy any one of the above requirements (A1), the above requirements (A2), the above requirements (A3), and the above requirements (A4), or two or more thereof.

[0184] The sealant resin composition (X) of the present invention preferably has a melting enthalpy ΔHfus measured at the second temperature rise of a differential scanning calorimeter (DSC) in the range of 20 to 100 J / g, preferably in the range of 20 to 90 J / g, more preferably in the range of 30 to 85 J / g, and further preferably in the range of 35 to 80 J / g.

[0185] The melting enthalpy is an index of crystallinity. When the melting enthalpy is below the upper limit, a sealant with low crystallinity, excellent flexibility, and excellent resistance to whitening during stretching can be easily obtained. When the melting enthalpy is above the lower limit, a sealant with excellent mechanical properties and heat resistance can be easily obtained.

[0186] The sealant resin composition (X) of the present invention may contain at least one additive selected from the group consisting of conventionally known flow modifiers, crystal nucleating agents, antioxidants, heat stabilizers, weathering stabilizers such as ultraviolet absorbers and light stabilizers, hydrochloric acid absorbers, pigments, dyes, antibacterial agents, antifungal agents, antistatic agents, lubricants, slip agents, antiblocking agents, anticorona agents, foaming agents, foaming aids, plasticizers such as mineral oils, and fillers, as needed, within a range not impairing the purpose of the present invention.

[0187] [Method for producing sealant resin composition (X)]

[0188] The method for producing the sealant resin composition (X) of the present invention is not particularly limited, and can be prepared, for example, by mixing the above-mentioned 1-butene·ethylene copolymer (A) and the propylene polymer (B), and the ethylene polymer (C) added as required, and other optional components added as required in the above-mentioned mixing ratio using, for example, a Henschel mixer, a V-type mixer, a ribbon mixer, a drum mixer, a kneading extruder, etc., or by melt-kneading after or without mixing using a single-screw extruder, a twin-screw extruder, a kneader, a Banbury mixer, etc. In addition, granulation, pulverization, etc. can be performed as required.

[0189] When mixing and kneading these, the components to be formulated may be added all at once or in stages.

[0190] The method of melt kneading 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 portion kneaded by the melt kneading device is usually 170 to 250° C., preferably 190 to 230° C. The kneading time is usually 0.5 to 30 minutes, particularly preferably 0.5 to 5 minutes.

[0191] <Sealing agent film>

[0192] The sealant film of the present invention is a single-layer or multi-layer sealant film including at least one layer containing the sealant resin composition (X) of the present invention.

[0193] In order to obtain a sealant film using the sealant resin composition (X), it is possible to produce it using a conventionally known single-layer or multi-layer film-forming machine.

[0194] The sealant resin composition (X) of the present invention can be used as a sealant film even in the form of a single-layer film, and can be used as a sealant film even in the form of a multi-layer film laminated with a substrate film composed of a polyolefin resin or the like. That is, the sealant film of the present invention may be a single-layer or multi-layer film comprising only a layer composed of the sealant resin composition (X) of the present invention, or may be a laminate comprising a layer composed of the sealant resin composition (X) of the present invention and a layer composed of a substrate film.

[0195] Examples of the substrate film formed of the polyolefin resin include single-layer or multi-layer films of polyolefin resins (e.g., polyethylene, polypropylene), polyester resins, polycarbonate resins, polyarylate resins, acrylic resins, polyphenylene sulfide resins, polystyrene resins, vinyl resins, vinyl chloride resins, polyimide resins, epoxy resins, etc. In a preferred and exemplary embodiment of the present invention, the substrate film is at least one selected from the group consisting of polyolefin films, polystyrene films, polyester films, polyamide films, laminated films of polyolefins and gas barrier resin films, metal foils such as aluminum foil, paper, and vapor-deposited films.

[0196] The laminate comprising a layer formed by the sealant resin composition (X) of the present invention and a layer formed by a substrate film can also be manufactured using a conventionally known single-layer or multi-layer film forming machine. For example, it can be manufactured in the following manner: using any one of the group consisting of melt extrusion lamination, heat lamination, and dry lamination, the layer of the sealant film is bonded to the substrate film. In a typical and exemplary embodiment of the present invention, the laminate can be obtained by a manufacturing method including the following steps, wherein the steps are: using any one of the group consisting of melt extrusion lamination, heat lamination, and dry lamination, a single-layer or multi-layer film containing only a layer formed by the sealant resin composition (X) of the present invention is bonded to the substrate film.

[0197] The sealant film containing the sealant resin composition (X) of the present invention may be either a stretched film or an unstretched film, and is preferably an unstretched film.

[0198] As long as the unstretched film is an unstretched film, there is no particular restriction, and the shape, size (thickness), etc. can be appropriately selected according to the desired use. In addition, the unstretched film can be a single layer or a multilayer. In the case of a multilayer, at least one layer thereof is a film comprising the sealant resin composition (X) of the present invention. That is, the unstretched film can be a single layer or a multilayer film comprising only a layer formed by the sealant resin composition (X) of the present invention, or a laminate comprising a layer formed by the sealant resin composition (X) of the present invention and a layer formed by a substrate.

[0199] The method for producing the unstretched film is not particularly limited as long as it does not impair the purpose of the present invention, and the unstretched film includes: a film obtained by a co-extrusion method using a known multi-layer film forming method such as a T-die film forming method and an inflation film forming method; a film obtained by further laminating a layer containing the sealant resin composition (X) of the present invention on a pre-formed substrate. For example, the unstretched film may be a film obtained by a production method including the following steps: a single-layer or multi-layer sealant film (for example, a single-layer or multi-layer film containing only a layer formed by the sealant resin composition (X) of the present invention) containing at least one layer containing the sealant resin composition (X) is bonded to a substrate using any one of the methods selected from the group consisting of a melt extrusion lamination method, a heat lamination method, and a dry lamination method.

[0200] The substrate is not particularly limited, and may be a metal such as aluminum foil, steel foil, stainless steel foil, or a thermoplastic resin. The substrate is in the form of a substrate film in most cases, and may be, for example, a substrate film exemplified as the above-mentioned "substrate film formed of a polyolefin resin, etc.", or may be a metal foil such as aluminum foil. It should be noted that, when the unstretched film is multilayer, "unstretched" means that all layers thereof are not stretched.

[0201] The thickness of the unstretched film (in the case of multiple layers, the total thickness) is preferably 5 μm or more, more preferably 10 μm or more, further preferably 20 μm or more, and is preferably 150 μm or less, more preferably 130 μm or less, further preferably 100 μm or less.

[0202] It should be noted that in this specification, there is no particular distinction between a film and a sheet. Generally, a film refers to a film-like body having a thickness of less than 250 μm, and a sheet refers to a thin plate-like body having a thickness of 250 μm or more.

[0203] Specific uses of the unstretched film include, for example, packaging films for packaging food, liquids, medicines, electronic parts, and the like, and packaging materials obtained therefrom.

[0204] <Application of sealant film>

[0205] The sealant film of the present invention and the laminated body formed by laminating the sealant film and the substrate film (for example, a single-layer or multi-layer sealant film containing only a layer formed by the above-mentioned sealant resin composition (X), and a laminated body containing a layer formed by the above-mentioned sealant resin composition (X) and a layer formed by a substrate film) can be used as a packaging body for all articles represented by daily necessities, food (food packaging materials), liquids, medicines, electronic components, and building materials. In addition, the aforementioned sealant film and the aforementioned laminated body can be included in power storage devices such as lithium ion batteries and lithium ion capacitors, for example, and can be used as a packaging body for lithium ion batteries. If the view is changed, it can also be said that the present invention provides a power storage device containing the above-mentioned sealant resin composition (X). As an example of such a power storage device, a power storage device containing the aforementioned sealant film or the aforementioned laminated body can be cited, and as a specific example thereof, a packaging body for lithium ion batteries containing the aforementioned sealant film or the aforementioned laminated body can be cited.

[0206] Lithium-ion batteries usually contain a positive electrode, a negative electrode, a separator between the positive electrode and the negative electrode, and a non-aqueous electrolyte. The positive electrode usually contains: a positive electrode collector formed of a metal material or a carbon material; and a positive electrode material that can absorb and release lithium, such as a composite oxide formed of lithium and a transition metal as a positive electrode active material. The negative electrode usually contains: a negative electrode collector formed of a carbon material, etc.; and a negative electrode material that can absorb and release lithium ions, such as metallic lithium, a lithium-containing alloy, a metal or alloy that can be alloyed with lithium, etc. as a negative electrode active material. The non-aqueous electrolyte contains a lithium salt as an electrolyte and a non-aqueous solvent. In addition, in a lithium-ion battery, the non-aqueous electrolyte is impregnated in the positive electrode, the negative electrode, and the separator. It should be noted that the details of the non-aqueous solvent are described in the "non-aqueous solvent" section below.

[0207] Furthermore, the lithium-ion battery often has a packaging body (lithium-ion battery packaging body) at its peripheral portion, and the positive electrode, the negative electrode, the separator, and the non-aqueous electrolyte are sealed inside the packaging body. Here, in general, a positive terminal and a negative terminal are connected to the positive electrode and the negative electrode, respectively, and a portion of the positive terminal and a portion of the negative terminal are exposed outside the packaging body.

[0208] When the sealant film or laminate of the present invention is used as the aforementioned packaging body, the aforementioned positive electrode and the aforementioned negative electrode are sandwiched by a pair of sealant films or a pair of laminates, and the peripheral portions of the pair of sealant films or the pair of laminates are heat-fused in a manner that a portion of the positive terminal and a portion of the negative terminal are exposed outside the pair of sealant films or the pair of laminates, thereby obtaining a lithium ion battery. Here, when the laminate of the present invention is used as the aforementioned packaging body, the aforementioned laminate may include a substrate formed of a metal such as aluminum foil.

[0209] Lithium-ion batteries using the lithium-ion battery package can be used in, for example, portable electronic devices, personal computers, robots, drones, automobiles, aircraft, wearable devices, and power storage systems (ESS) for household use or renewable energy generation.

[0210] <Non-aqueous solvent>

[0211] Non-aqueous electrolytes for lithium-ion batteries generally contain a non-aqueous solvent.

[0212] As the nonaqueous solvent, various known nonaqueous solvents can be appropriately selected, and it is preferable to use at least one selected from the group consisting of cyclic aprotic solvents and chain aprotic solvents.

[0213] When it is desired to increase 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.

[0214] (Cyclic aprotic solvent)

[0215] As the cyclic aprotic solvent, cyclic carbonate, cyclic carboxylic acid ester, cyclic sulfone, and cyclic ether can be used.

[0216] The cyclic aprotic solvent can be used alone or in combination. The mixing ratio of the cyclic aprotic solvent in the non-aqueous solvent is 10% to 100% by mass, more preferably 20% to 90% by mass, and particularly preferably 30% to 80% by mass. By setting such a ratio, the conductivity of the electrolyte solution related to the charge and discharge characteristics of the battery can be improved.

[0217] As an example of cyclic carbonate, specifically, ethylene carbonate, propylene carbonate, 1,2-butylene carbonate, 2,3-butylene carbonate, 1,2-pentylene carbonate, 2,3-pentylene carbonate, etc. can be cited. Among these, ethylene carbonate and propylene carbonate with high dielectric constant are preferably used. In the case of a battery using graphite in the negative electrode active material, ethylene carbonate is more preferred. In addition, these cyclic carbonates can be used in combination of two or more.

[0218] Specific examples of the cyclic carboxylic acid ester include γ-butyrolactone, δ-valerolactone, or alkyl-substituted products such as methyl-γ-butyrolactone, ethyl-γ-butyrolactone, and ethyl-δ-valerolactone.

[0219] Cyclic carboxylic acid esters have low vapor pressure, low viscosity, and high dielectric constant, and can reduce the viscosity of the electrolyte without reducing the flash point of the electrolyte and the degree of dissociation of the electrolyte. Therefore, it has the characteristic of being able to improve the conductivity of the electrolyte, which is an indicator related to the charge and discharge characteristics of the battery, without increasing the flammability of the electrolyte. Therefore, when it is desired to increase the flash point of the solvent, it is preferred to use a cyclic carboxylic acid ester as the aforementioned cyclic aprotic solvent. γ-butyrolactone is most preferred.

[0220] In addition, the cyclic carboxylic acid ester is preferably used in a mixture with other cyclic aprotic solvents. For example, a mixture of a cyclic carboxylic acid ester and a cyclic carbonate and / or a chain carbonate can be mentioned.

[0221] Examples of combinations of cyclic carboxylates and cyclic carbonates and / or chain carbonates include, specifically, γ-butyrolactone and ethylene carbonate, γ-butyrolactone and ethylene carbonate and dimethyl carbonate, γ-butyrolactone and ethylene carbonate and ethyl methyl carbonate, γ-butyrolactone and ethylene carbonate and diethyl carbonate, γ-butyrolactone and propylene carbonate, γ-butyrolactone and propylene carbonate and dimethyl carbonate, γ-butyrolactone and propylene carbonate and ethyl methyl carbonate, γ-butyrolactone and propylene carbonate and diethyl carbonate, γ-butyrolactone and ethylene carbonate and propylene carbonate, γ-butyrolactone and ethylene carbonate and propylene carbonate and dimethyl carbonate, γ-butyrolactone and ethylene carbonate and propylene carbonate and ethyl methyl carbonate, γ-butyrolactone and ethylene carbonate and propylene carbonate and diethyl carbonate, γ-butyrolactone and ethylene carbonate and dimethyl carbonate and ethyl methyl carbonate, γ-butyrolactone and ethylene carbonate and propylene carbonate and diethyl carbonate. -Butyrolactone with ethylene carbonate and dimethyl carbonate and diethyl carbonate, γ-butyrolactone with ethylene carbonate and ethyl methyl carbonate and diethyl carbonate, γ-butyrolactone with ethylene carbonate and dimethyl carbonate and ethyl methyl carbonate and diethyl carbonate, γ-butyrolactone with ethylene carbonate and propylene carbonate and dimethyl carbonate and ethyl methyl carbonate, γ-butyrolactone with ethylene carbonate and propylene carbonate and dimethyl carbonate and diethyl carbonate, γ-butyrolactone With ethylene carbonate and propylene carbonate and ethyl methyl carbonate and diethyl carbonate, γ-butyrolactone with ethylene carbonate and propylene carbonate and dimethyl carbonate and ethyl methyl carbonate and diethyl carbonate, γ-butyrolactone with sulfolane, γ-butyrolactone with ethylene carbonate and sulfolane, γ-butyrolactone with propylene carbonate and sulfolane, γ-butyrolactone with ethylene carbonate and propylene carbonate and sulfolane, γ-butyrolactone with sulfolane and dimethyl carbonate, etc.

[0222] Examples of the cyclic sulfone include sulfolane, 2-methylsulfolane, 3-methylsulfolane, dimethyl sulfone, diethyl sulfone, dipropyl sulfone, methylethyl sulfone, and methylpropyl sulfone.

[0223] Examples of cyclic ethers include dioxolane.

[0224] (chain aprotic solvent)

[0225] As the chain aprotic solvent, chain carbonate, chain carboxylic acid ester, chain ether, chain phosphate ester and the like can be used.

[0226] The mixing ratio of the chain aprotic solvent in the nonaqueous solvent is 10% by mass to 100% by mass, more preferably 20% by mass to 90% by mass, and particularly preferably 30% by mass to 80% by mass.

[0227] As the linear carbonate, specifically, dimethyl carbonate, ethyl methyl carbonate, diethyl carbonate, methyl propyl carbonate, methyl isopropyl carbonate, ethyl propyl carbonate, dipropyl carbonate, methyl butyl carbonate, ethyl butyl carbonate, dibutyl carbonate, methyl amyl carbonate, ethyl amyl carbonate, diamyl 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, methyl trifluoroethyl carbonate etc. can be enumerated.These linear carbonates can be used in combination of two or more.

[0228] Specific examples of the chain carboxylic acid ester include methyl pivalate and the like.

[0229] Specific examples of the chain ether include dimethoxyethane and the like.

[0230] Specific examples of the chain phosphoric acid ester include trimethyl phosphate and the like.

[0231] (Combination of solvents)

[0232] The nonaqueous solvent contained in the nonaqueous electrolyte may be only one kind or two or more kinds.

[0233] In addition, only one or more cyclic aprotic solvents may be used, only one or more chain aprotic solvents may be used, or a cyclic aprotic solvent and a chain protic solvent may be mixed and used. In particular, when it is desired to improve the load characteristics and low temperature characteristics of the battery, it is preferred to use a cyclic aprotic solvent and a chain aprotic solvent in combination as the nonaqueous solvent.

[0234] In addition, consider from the electrochemical stability aspect of electrolyte, in the cyclic aprotic solvent, most preferably use cyclic carbonate, in the chain aprotic solvent, most preferably use linear carbonate.In addition, by the combination of cyclic carboxylic acid ester and cyclic carbonate and / or linear carbonate, also can improve the conductivity of the electrolyte relevant with the charge-discharge characteristic of battery.

[0235] Specific examples of the combination of cyclic carbonate and linear carbonate include ethylene carbonate and dimethyl carbonate, ethylene carbonate and ethyl methyl carbonate, ethylene carbonate and diethyl carbonate, propylene carbonate and dimethyl carbonate, propylene carbonate and ethyl methyl carbonate, propylene carbonate and diethyl carbonate, ethylene carbonate and propylene carbonate and ethyl methyl carbonate, ethylene carbonate and propylene carbonate and diethyl carbonate, ethylene carbonate and dimethyl carbonate and ethyl methyl carbonate, ethylene carbonate and Dimethyl carbonate and diethyl carbonate, ethylene carbonate with ethyl methyl carbonate and diethyl carbonate, ethylene carbonate with dimethyl carbonate, ethyl methyl carbonate and diethyl carbonate, ethylene carbonate and propylene carbonate with dimethyl carbonate and ethyl methyl carbonate, ethylene carbonate and propylene carbonate with dimethyl carbonate and diethyl carbonate, ethylene carbonate and propylene carbonate with ethyl methyl carbonate and diethyl carbonate, ethylene carbonate and propylene carbonate with dimethyl carbonate, ethyl methyl carbonate and diethyl carbonate, etc.

[0236] The mixing ratio of cyclic carbonate and linear carbonate is expressed by mass ratio, and cyclic carbonate: linear carbonate is 5:95~80:20, and more preferably 10:90~70:30. By setting such a ratio, the viscosity rise of the electrolyte can be suppressed, and the dissociation degree of the electrolyte can be improved, so the conductivity of the electrolyte related to the charge and discharge characteristics of the battery can be improved. In addition, the solubility of the electrolyte can be further improved. Therefore, an electrolyte with excellent conductivity at room temperature or low temperature can be formed, so the load characteristics of the battery at room temperature to low temperature can be improved.

[0237] The lithium ion battery contains a non-aqueous electrolyte containing the above-mentioned non-aqueous solvent in its interior. Thus, the package (lithium ion battery package) constituting the lithium ion battery needs to be less likely to dissolve into the above-mentioned non-aqueous solvent and swell due to the above-mentioned non-aqueous solvent, and needs to be able to maintain a certain mechanical strength even when exposed to contact with the above-mentioned non-aqueous solvent. The sealant film and laminate of the present invention containing the above-mentioned sealant resin composition (X) have excellent whitening resistance, and are less likely to dissolve into the above-mentioned non-aqueous solvent and swell due to the above-mentioned non-aqueous solvent. Even if exposed to contact with the above-mentioned non-aqueous solvent, they can maintain a certain mechanical strength, and can therefore be appropriately used as a lithium ion battery package.

[0238] Example

[0239] Hereinafter, the present invention will be described in more detail based on Examples, but the present invention is not limited to these Examples at all.

[0240] The polymers and the like used in Examples and Comparative Examples are shown below.

[0241] [1-Butene·ethylene copolymer (A)]

[0242] 1-Butene·ethylene copolymers (A-1) to (A-6) obtained in the Production Examples described below were used.

[0243] (A-1): 1-butene·ethylene copolymer (ethylene content: 14.6 mol %, MFR (190° C., 2.16 kg load): 3.0 g / 10 min, intrinsic viscosity [η]: 1.72 dl / g, mmmm fraction: 95.9%)

[0244] (A-2): 1-butene·ethylene copolymer (ethylene content: 14.3 mol %, MFR (190° C., 2.16 kg load): 1.1 g / 10 min, intrinsic viscosity [η]: 2.14 dl / g, mmmm fraction: 96.2%)

[0245] (A-3): 1-butene·ethylene copolymer (ethylene content: 12.2 mol %, MFR (190° C., 2.16 kg load): 3.3 g / 10 min, intrinsic viscosity [η]: 1.68 dl / g, mmmm fraction: 94.6%)

[0246] (A-4): 1-butene·ethylene copolymer (ethylene content: 10.1 mol %, MFR (190°C, 2.16 kg load): 3.0 g / 10 min, intrinsic viscosity [η]: 1.68 dl / g, mmmm fraction: 93.6%)

[0247] (A-5): 1-butene·ethylene copolymer (ethylene content: 8.1 mol %, MFR (190°C, 2.16 kg load): 3.1 g / 10 min, intrinsic viscosity [η]: 1.65 dl / g, mmmm fraction: 92.8%)

[0248] (A-6): 1-butene·ethylene copolymer (ethylene content: 5.7 mol %, MFR (190°C, 2.16 kg load): 3.0 g / 10 min, intrinsic viscosity [η]: 1.66 dl / g, mmmm fraction: 92.3%)

[0249] [Propylene polymer (B)]

[0250] As the propylene-based polymer (B), random polypropylene (produced by Prime Polymer Co., Ltd., trade name PrimePolypro F327, MFR (230°C, 2.16 kg load): 7 g / 10 min, melting point: 140°C, crystallization temperature: 93°C, mmmm: 95.3%) was used (B-1).

[0251] [Ethylene polymer (C)]

[0252] As the ethylene polymer (C),

[0253] High-pressure low-density polyethylene (manufactured by Dow-Mitsui Polychemicals CO., LTD., trade name MIRASON11P, MFR (190°C, 2.16 kg load) 7.2 g / 10 min, density: 0.917 g / cm 3 (917kg / m 3 ), melting point: 108°C) (C-1); or,

[0254] Ethylene-propylene copolymer (MFR (190°C, 2.16 kg load): 0.6 g / 10 min, density: 0.869 g / cm 3 (869kg / m 3 ), propylene content: 19 mol%, melting point: 40°C) (C-2).

[0255] [Other ingredients]

[0256] As other components, a propylene-ethylene copolymer (ethylene content: 20.6 mol %, MFR (190° C., 2.16 kg load): 1.4 g / 10 min., melting point: 44° C.) (PER) was used.

[0257] 《Production Example of 1-butene·ethylene copolymer (A)》

[0258] [Production Example 1]

[0259] To one supply port of a continuous polymerization vessel having a volume of 300 liters, n-hexane was supplied at a rate of 14.2 L / h, and from another supply port, a mixed hexane solution of isopropylidene (3-tert-butyl-5-methylcyclopentadienyl-fluorenyl) zirconium dichloride (main catalyst 1) and modified methylaluminoxane and triisobutylaluminum (the zirconium conversion concentration of the main catalyst 1 was 0.5 mmol / liter, the aluminum conversion concentration of the modified methylaluminoxane was 4 mmol / L, and the aluminum conversion concentration of the triisobutylaluminum was 100 mmol / L) was continuously supplied at a rate of 0.22 L / h (total hexane 10 L / h). At the same time, from another supply port of the polymerization vessel, 1-butene was continuously supplied at a rate of 27 kg / h, ethylene at a rate of 1.0 kg / h, and hydrogen at a rate of 0.6 NL / h, and continuous solution polymerization was carried out under the conditions of a polymerization temperature of 60°C, a polymerization pressure of 0.8 MPaG, and a residence time of 1.5 hours to obtain a 1-butene·ethylene copolymer (A-1).

[0260] [Production Example 2]

[0261] A 1-butene·ethylene copolymer (A-2) was produced in the same manner as in Production Example 1 except that 1-butene was adjusted to 27 kg / h, ethylene was adjusted to 0.9 kg / h, and hydrogen was adjusted to 0.1 NL / h.

[0262] [Production Example 3]

[0263] 1-Butene·ethylene copolymer (A-3) was produced in the same manner as in Production Example 1 except that 1-butene was adjusted to 27 kg / h, ethylene was adjusted to 0.8 kg / h, and hydrogen was adjusted to 0.6 NL / h.

[0264] [Production Example 4]

[0265] A 1-butene·ethylene copolymer (A-4) was produced in the same manner as in Production Example 1 except that 1-butene was adjusted to 27 kg / h, ethylene was adjusted to 0.7 kg / h, and hydrogen was adjusted to 0.7 NL / h.

[0266] [Production Example 5]

[0267] 1-Butene·ethylene copolymer (A-5) was produced in the same manner as in Production Example 1 except that 1-butene was adjusted to 27 kg / h, ethylene was adjusted to 0.6 kg / h, hydrogen was adjusted to 0.7 NL / h, and the polymerization pressure was adjusted to 0.7 MPaG.

[0268] [Production Example 6]

[0269] 1-Butene·ethylene copolymer (A-6) was produced in the same manner as in Production Example 1 except that 1-butene was adjusted to 27 kg / h, ethylene was adjusted to 0.4 kg / h, hydrogen was adjusted to 0.6 NL / h, and the polymerization pressure was adjusted to 0.6 MPaG.

[0270] The physical properties of the 1-butene·ethylene copolymer (A) obtained in the production example were measured by the following methods.

[0271] [Table 1]

[0272] Table 1

[0273]

[0274] [1-Butene and ethylene contents in 1-butene / ethylene copolymer (A)]

[0275] The quantification of 1-butene and ethylene content was performed using a Bruker BioSpin AVANCE cryo-500 nuclear magnetic resonance apparatus as follows. The solvent was a mixed solvent of o-dichlorobenzene / deuterated benzene (volume ratio: 80 / 20), the sample concentration was 20 mg / 0.6 mL, the measurement temperature was 120° C., and the observation nucleus was 13 C (125MHz), the sequence is single pulse proton broadband decoupling, the pulse width is 4.7 microseconds (45° pulse), the repetition time is 5.5 seconds, the accumulation number is 128 times, and the chemical shift reference value is 27.50ppm for the carbon signal of the methylene group of the butene side chain. 13 C-NMR spectroscopy was used to quantify the compositions of 1-butene (C4 content; mol %) and ethylene (C2 content; mol %).

[0276] [MFR of 1-butene·ethylene copolymer (A)]

[0277] The MFR at 190°C and a load of 2.16 kg was measured in accordance with ASTM D1238.

[0278] [Determination of isotactic pentad fraction (mmmm)]

[0279] The pentad isotacticity (mmmm) of the 1-butene·ethylene copolymer (A) was calculated by the following formula: the peak area S with 27.5 ppm as the peak top and the total area S' of the peaks appearing in the range of 27.3 ppm to 26.3 ppm were determined, assuming that the chemical shift of the peak top belonging to the pentad represented by mmmm was 27.5 ppm. (Detection limit: 0.01%)

[0280] (mmmm) = S / (S+S') × 100 (%)

[0281] Here, the main peak appearing in the range of 27.3 ppm to 26.3 ppm is a peak attributable to mmmr (27.3 ppm), mmrr and rmmr (27.2 ppm), and mrrm (26.3 ppm).

[0282] [Intrinsic viscosity [η] (dl / g)]

[0283] The intrinsic viscosity [η] of the 1-butene·ethylene copolymer (A) is a value measured at 135° C. in a decalin solvent using an Ubbelohde viscometer. About 20 mg of polymer powder, pellets or resin blocks are collected and dissolved in 15 mL of decalin, and the specific viscosity ηsp is measured in an oil bath heated to 135° C. After adding 5 mL of decalin solvent to the decalin solution to dilute it, the specific viscosity ηsp is measured in the same manner. This dilution operation is further repeated twice, and the value of ηsp / C when the concentration (C) is extrapolated to zero is calculated as the intrinsic viscosity [η].

[0284] [η] = lim(ηsp / C)(C→0)

[0285] [Weight average molecular weight (Mw) and molecular weight distribution (Mw / Mn)]

[0286] As a GPC apparatus, a gel permeation chromatograph Alliance GPC-2000 manufactured by Waters Corporation was used, and Mw and Mn in terms of polystyrene were measured under the following conditions, and Mw / Mn was calculated.

[0287] Separation columns: 2 TSKgel GNH6-HT manufactured by Tosoh Corporation, and 2 TSKgel GNH6-HTL manufactured by Tosoh Corporation (column dimensions: 7.5 mm in diameter, 300 mm in length)

[0288] Column temperature: 140°C

[0289] Mobile phase: o-dichlorobenzene (manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.) containing 0.025 wt% of BHT (manufactured by Takeda Pharmaceutical Co., Ltd.) as an antioxidant

[0290] Moving speed: 1.0mL / min

[0291] Sample concentration: 15mg / 10mL

[0292] Sample injection volume: 400μL

[0293] Detector: Differential refractometer

[0294] Standard polystyrene: in the molecular weight range of Mw<1000 and Mw>4×10 6 In the case of , standard polystyrene manufactured by Tosoh Corporation was used, and the molecular weight was 1000≤Mw≤4×10 6 In the case of , standard polystyrene manufactured by Pressure Chemical Company was used.

[0295] [Pressure molding conditions]

[0296] The pressurized sheets prepared under the following conditions and stored at room temperature for 10 days or more were used for the test. In the following tests, unless otherwise specified, the pressurized sheets stored at room temperature for 10 days or more were used as test pieces or mechanical property test pieces.

[0297] Pressing machine: Made by KANSAI ROLL Co., Ltd. (Model: PEWE-70 / 50 35)

[0298] Residual heat time: 4min

[0299] Residual heat and pressurization temperature: 120℃

[0300] Pressure: 10MPa

[0301] Pressurization time: 3min

[0302] Cooling rate: 40°C / min (pressurized at 10 MPa for 4 minutes using another press set at 20°C, and cooled to room temperature)

[0303] [Melting point and melting enthalpy]

[0304] The melting point and the melting enthalpy ΔHfus (1st, 2nd) were measured by the measurement method described above (ie, the measurement method described in the above “Requirement (A5)”).

[0305] That is, the calorimetric measurement of a polymer such as the 1-butene·ethylene copolymer (A) by a differential scanning calorimeter (DSC) is performed as follows: about 6 to 10 mg of a sample is accurately weighed, sealed in an aluminum pan, and temporarily cooled to -70°C (first cooling), then heated from -70°C to 200°C at a heating rate of 20°C / min (first heating), and a DSC curve is measured. After holding at 200°C for 10 minutes, the temperature is then cooled to -70°C at a cooling rate of 20°C / min (second cooling), and a DSC curve is measured. After holding at -70°C for 1 minute, the temperature is again heated from -70°C to 200°C at a heating rate of 20°C / min (second heating), and a DSC curve is measured. Here, the first cooling performed before the first heating is performed by temporarily cooling from 30°C to -70°C at a cooling rate of 20°C / min, and after the first cooling, the temperature is held at -70°C for 5 minutes, and then the first heating is performed.

[0306] Here, the DSC measurement of polymers such as the 1-butene·ethylene copolymer (A) is performed using X-DSC7000 (differential scanning calorimeter, manufactured by Hitachi High-Tech Science Corporation).

[0307] Moreover, in the aforementioned DSC curve, when an endothermic peak (melting peak) caused by melting is observed during the aforementioned first temperature increase, the temperature at which the melting peak (hereinafter, referred to as "melting peak P1") is observed, specifically, the temperature of the peak top of the "melting peak P1" is set to Tm1 or "melting point (1st)". When a melting peak is observed during the aforementioned second temperature increase, the temperature at which the melting peak (hereinafter, referred to as "melting peak P2") is observed, specifically, the temperature of the peak top of the "melting peak P2" is set to Tm2 or "melting point (2nd)". Here, for each of the "melting peak P1" and the "melting peak P2", when two or more melting peaks are observed, the highest temperature among the temperatures of the peak tops of these peaks is set to the melting point.

[0308] In addition, in the above-mentioned DSC curve, when the above-mentioned "melting peak P1" exists, the melting enthalpy obtained for the melting peak P1 is set to ΔHfus(1st) or "melting enthalpy(1st)". Similarly, when the above-mentioned "melting peak P2" exists, the melting enthalpy obtained for the melting peak P2 is set to ΔHfus(2nd) or "melting enthalpy(2nd)".

[0309] When a crystal melting peak having a crystal melting enthalpy of 1 J / g or more is not observed as the “melting peak P1” or “melting peak P2”, it is judged as “melting peak not observed” or “na”.

[0310] [Mechanical properties (normal temperature)]

[0311] The yield stress, breaking strength (TS), breaking elongation (between chucks, EL), and Young's modulus (YM) were measured for the mechanical property test pieces according to JIS K 6251 (measurement temperature: 23° C., tensile speed: 200 mm / min, maximum strain: 800%). In addition, in the case where no breakage occurs under the condition of strain = 800%, the stress at that time is defined as TS.

[0312] [Shore hardness A (instantaneous value) and Shore hardness D]

[0313] Use a type A tester to read the scale immediately after the indenter contacts the test piece, and set it as Shore A hardness (according to ASTM D2240).

[0314] Use a D-type tester to read the maximum value after the indenter contacts the test piece, and set it as Shore hardness D. (According to ASTM D2240).

[0315] In addition, during the press molding, a 100 μm thick release PET film (manufactured by Toray, trade name Lumirror) was used as a release film.

[0316] The physical properties of the sealant resin compositions obtained in Examples and Comparative Examples were measured by the following methods. The results are shown in Tables 2-1 and 2-2.

[0317] [Melting point and melting enthalpy (sealant resin composition)]

[0318] The melting point and the enthalpy of fusion ΔHfus(2nd) are measured by the measurement method described above (ie, the measurement method described in the above “Requirement (X2)”).

[0319] That is, the melting point and melting enthalpy of the sealant resin composition (X) are measured by DSC measurement. The DSC measurement is performed using X-DSC7000 (differential scanning calorimeter, manufactured by Hitachi High-Tech Science Corporation) in the same manner as described in the above "Melting point and melting enthalpy". Then, based on the DSC curve obtained by the above DSC measurement, the "melting point (2nd)" and "melting enthalpy (2nd)" are obtained by the same method as described in the above "Melting point and melting enthalpy".

[0320] In addition, in the comparative example which used the single polymer instead of the sealant resin composition (X), the same DSC measurement was performed on this polymer.

[0321] [Tensile elastic modulus (sealant resin composition)]

[0322] use A single screw extruder (single shaft extruder) is used to melt-knead various polymers in the proportions (parts by mass) listed in Tables 2-1 and 2-2 at a melting temperature of 210°C and a rotation speed of 40 to 50 rpm to prepare pellets. A hydraulic hot press molding machine set at 190°C is used to heat the sealant resin composition (X) obtained in the form of the above-mentioned pellets for 5 minutes, and then molded under a pressure of 10 MPa for 2 minutes, and then cooled at 20°C and a pressure of 10 MPa for 4 minutes to prepare a 2 mm thick sheet (test piece). Here, in the comparative example in which a single polymer is used instead of the sealant resin composition (X), the preparation of pellets and the preparation of sheets (test pieces) are similarly performed for the polymer.

[0323] After molding, the test piece was stored at room temperature for more than 7 days, and then a dumbbell-shaped test piece (Type ASTM-4) specified in ASTM D638 was made from the piece. A tensile test was performed on the dumbbell-shaped test piece in accordance with ASTM D638 (measuring temperature 23°C, tensile speed = 50 mm / min), and the tensile elastic modulus (Young's modulus (YM)) was calculated based on the obtained stress / strain curve.

[0324] [Shore hardness D (sealant resin composition)]

[0325] use A single screw extruder (single shaft extruder) is used to melt-knead various polymers in the proportions (parts by mass) listed in Tables 2-1 and 2-2 at a melting temperature of 210°C and a rotation speed of 40 to 50 rpm to prepare pellets. A hydraulic hot press molding machine set at 190°C is used to heat the sealant resin composition (X) obtained in the form of the above-mentioned pellets for 5 minutes, and then molded under a pressure of 10 MPa for 2 minutes, and then cooled at 20°C and a pressure of 10 MPa for 4 minutes to prepare a 2 mm thick sheet (test piece). Here, in the comparative example in which a single polymer is used instead of the sealant resin composition (X), the preparation of pellets and the preparation of sheets (test pieces) are similarly performed for the polymer.

[0326] After molding, the test piece was stored at room temperature for 7 days or more, and then the Shore D hardness was measured.

[0327] [MFR (sealant resin composition)]

[0328] The MFR at 230° C. and a load of 2.16 kg was measured in accordance with ASTM D1238.

[0329] [Whitening resistance test]

[0330] use A single screw extruder (single shaft extruder) was used to melt-knead various polymers in the proportions (parts by mass) listed in Tables 2-1, 2-2 and 3 at a melting temperature of 210°C and a rotation speed of 40 to 50 rpm to prepare pellets. A hydraulic hot press molding machine set at 190°C was used to heat the sealant resin composition (X) obtained in the form of the above-mentioned pellets for 5 minutes, and then molded under a pressure of 10 MPa for 2 minutes, and then cooled at 20°C and a pressure of 10 MPa for 4 minutes to prepare a 0.5 mm thick sheet (test piece). Here, in the comparative example in which a single polymer was used instead of the sealant resin composition (X), the preparation of pellets and the preparation of sheets (test pieces) were similarly performed for the polymer.

[0331] The obtained sheet (test piece) was stored at room temperature for 7 days or more after molding.

[0332] A No. 2 dumbbell (dumbbell-shaped No. 2 dumbbell test piece) specified in JIS K 6251 was made from the sheet, and the hue before stretching (L value (before stretching)) and the hue when stretched by 15 mm at a stretching speed of 50 mm / min (L value (after stretching)) were measured using a spectrophotometer (manufactured by Konica Minolta, Inc., CM-3700d), and the hue change (ΔL) was calculated based on the following formula.

[0333] Furthermore, using the obtained sheet after heat treatment at 85° C. for 5 days, the color change (ΔL) was calculated in the same manner.

[0334] The smaller the ΔL value, the better the whitening resistance.

[0335] Evaluation criteria for whitening resistance

[0336] ΔL = L value (after stretching) - L value (before stretching)

[0337] ○: ΔL≤15

[0338] ×: ΔL≥16

[0339] [Heat seal strength]

[0340] The polymers listed in Tables 2-1 and 2-2 were extruded at the ratios (parts by mass) listed in Tables 2-1 and 2-2. The obtained pellets were kneaded and extruded at 230°C using a cast film forming machine to produce a 100 μm thick single-layer unstretched film. Next, a stretched PET film (manufactured by Toray) having a thickness of 25 μm was laminated on the substrate layer of the obtained unstretched film via an adhesive layer using a dry lamination method to produce a laminate (hereinafter, in this item, sometimes referred to as a "laminated film"). That is, the laminate has a layer composed of a sealant resin composition such as a sealant resin composition (X), an adhesive layer, and a substrate layer composed of a stretched PET film in sequence, and the aforementioned adhesive layer is directly in contact with the layer composed of the aforementioned sealant resin composition and the substrate layer composed of the stretched PET film. The laminate was used for the following evaluation.

[0341] 〈Heat seal (HS) strength (before heat treatment)〉

[0342] A test body was prepared by sequentially stacking a 50 μm thick Teflon (registered trademark) sheet, two obtained laminated films, and a 50 μm thick Teflon (registered trademark) sheet. The two laminated films were stacked so that the surfaces having the layer composed of the sealant resin composition faced each other.

[0343] The heat sealing rod of the heat sealing tester (made by TESTER SANGYO CO,.LTD, TB-701B model) is set to a width of 15mm × a length of 300mm, the temperature of the lower side of the sealing rod is set to 70°C, the temperature of the upper side of the sealing rod is set to 190°C, the aforementioned test body is clamped with the sealing rod, and heat-sealed for 1.0 seconds at a pressure of 0.2MPa. Then, two Teflon (registered trademark) sheets are removed to obtain a laminated film, which is placed at 23°C for 1 day. A slit of 15mm width is formed on the laminated film in a manner including the heat-sealed portion, and the unheat-sealed portion is clamped in a tensile testing machine (made by INTESCO Co., Ltd., IM-20ST). The maximum load when the heat-sealed portion is peeled off in a direction of 180° at a speed of 300mm / min is measured. This measurement is performed 5 times, and the average value of the maximum load is taken as the heat seal strength.

[0344] 〈Heat seal (HS) strength (after heat treatment)〉

[0345] In the HS strength (before heat treatment) test, the heat seal strength after heat treatment was measured in the same manner as in the HS strength (before heat treatment) test, except that a film obtained by heat treating the single-layer unstretched film obtained above at 85°C for 5 days was used instead of the single-layer unstretched film.

[0346] Evaluation criteria for HS strength (after heat treatment)

[0347] ○: HS strength is 35 N / 15 mm or more.

[0348] ×: HS strength is less than 35N / 15mm.

[0349] 〈Heat seal (HS) strength retention rate〉

[0350] The HS strength retention rate was calculated from the HS strength before and after the heat treatment using the following formula. It can be said that the larger the value, the better the heat resistance. In addition, based on the HS strength retention rate, the HS strength retention was evaluated according to the following criteria.

[0351] HS strength retention rate (%) = 100 × HS strength (after heat treatment) / HS strength (before heat treatment)

[0352] Evaluation criteria for HS strength retention

[0353] ○: HS strength retention rate is 80% or more.

[0354] ×: HS strength retention rate is less than 80%.

[0355] The single-layer unstretched film was heat-treated at 85°C for 5 days, and the presence or absence of changes in the appearance of the film surface before and after the heat treatment was evaluated.

[0356] ○: No appearance change

[0357] △: Bleeding components are generated on a part of the surface (a part of the surface is sticky).

[0358] ×: Bleeding components are generated on the entire surface (the entire surface is sticky).

[0359] [Resistance to non-aqueous solvents]

[0360] In order to evaluate the resistance to non-aqueous solvents, the sealant resin composition was evaluated as described below. Here, in the following evaluation, it is assumed that the sealant resin composition is used in a lithium ion battery package and the package is in contact with the electrolyte, and a mixed solvent of ethylene carbonate (EC) and diethyl carbonate (DEC) is used as the non-aqueous solvent.

[0361] It should be noted that the density of ethylene carbonate (EC) and diethyl carbonate (DEC) is 1.32 g / cm 3 and 0.975g / cm 3 Therefore, the mass ratio of EC to DEC in a 1:1 (v / v) mixed solvent of EC and DEC is approximately 58:42.

[0362] 〈Weight change rate after immersion in non-aqueous solvent〉

[0363] use A single screw extruder (single shaft extruder) was used to melt-knead various polymers in the proportions (parts by mass) listed in Table 3 at a melting temperature of 210°C and a rotation speed of 40 to 50 rpm to prepare pellets. The sealant resin composition (X) obtained in the form of the above-mentioned pellets was heated for 5 minutes using a hydraulic hot press molding machine set at 190°C, and then molded for 2 minutes under a pressure of 10 MPa, and then cooled for 4 minutes at 20°C and a pressure of 10 MPa to prepare a 0.3 mm thick sheet (test piece). Here, in the comparative example in which a single polymer was used instead of the sealant resin composition (X), the preparation of pellets and the preparation of sheets (test pieces) were similarly performed for the polymer.

[0364] A dumbbell No. ASTM638-4 was made from the 0.3 mm thick sheet obtained by the above-mentioned press molding, and after being immersed in ethylene carbonate (EC) / diethyl carbonate (DEC) = 1 / 1 (v / v%, manufactured by Kishida Chemical Co., Ltd., trade name "EC:DEC (1:1 v / v%)") at 80°C for 24 hours, the weight change rate was measured using the following formula.

[0365] Weight change rate (%) = 100 × (weight after immersion - weight before immersion) / weight before immersion

[0366] When the value of the weight change rate is negative, it means that the resin composition is dissolved in EC / DEC, and when the value is positive, it means that the resin composition is swollen by EC / DEC.

[0367] Evaluation criteria for weight change rate

[0368] ○: Weight change rate is -4.5% or more and 4.5% or less.

[0369] ×: The weight change rate is less than -4.5% or greater than 4.5%.

[0370] 〈Mechanical properties after EC / DEC immersion〉

[0371] ASTM-4 dumbbells were prepared from a 0.3 mm thick sheet obtained by press molding as described in the above “Weight change rate after immersion in a non-aqueous solvent”, and immersed in EC / DEC=1 / 1 (v / v%, manufactured by Kishida Chemical Co., Ltd.) at 80°C for 24 hours. The yield stress, breaking strength (TS), breaking elongation (between chucks, EL), and Young's modulus (YM) were measured for the test pieces before and after the immersion in accordance with ASTM D638 (measurement temperature: 23°C, tensile speed: 50 mm / min).

[0372] The Young's modulus (YM) maintenance rate and the breaking strength (TS) maintenance rate were measured by the following formula.

[0373] YM maintenance rate (%) = 100 × Young's modulus after immersion / Young's modulus before immersion

[0374] TS maintenance rate (%) = 100 × breaking point strength after immersion / breaking point strength before immersion

[0375] Evaluation criteria for YM maintenance rate and TS maintenance rate

[0376] ○: YM maintenance rate and TS maintenance rate are more than 81%.

[0377] ×: YM maintenance rate and TS maintenance rate are less than 81%.

[0378] [Physical properties and heat-sealing characteristics of sealant resin composition]

[0379] [Example A1]

[0380] As the 1-butene·ethylene copolymer (A), 10 parts by mass of the 1-butene·ethylene copolymer (A-1) described above was used, and as the propylene-based polymer (B), 90 parts by mass of the (B-1) described above was used, and a sealant resin composition was obtained by the method described above, and then the physical properties of the sealant resin composition were measured by the method described above. The obtained physical properties are shown in Table 2-1.

[0381] [Examples A2 to A9]

[0382] The same operation as in Example A1 was performed except that the polymers shown in Table 1 and Table 2-1 were used instead of the polymer constituting the sealant resin composition used in Example 1 to obtain a sealant resin composition. The physical properties of the obtained sealant resin composition were measured by the above-described methods. The obtained physical properties are shown in Table 2-1.

[0383] [Comparative Examples a1 to a4]

[0384] The same operation as in Example A1 was performed except that the polymers shown in Table 1 and Table 2-2 were used instead of the polymer constituting the sealant resin composition used in Example 1 to obtain a sealant resin composition. However, in Comparative Example a1, the random polypropylene (B-1) was used as it was. The physical properties of the obtained sealant resin composition or polymer were measured by the method described above. The obtained physical properties are shown in Table 2-2.

[0385] [Table 2-1]

[0386] Table 2-1

[0387]

[0388] [Table 2-2]

[0389] Table 2-2

[0390]

[0391] [Physical properties of the sealant resin composition after immersion in a non-aqueous solvent]

[0392] [Examples B1, B10-B11 and B8-B9, and Comparative Examples b1-b4]

[0393] In Examples B1 and B8 to B9, Comparative Example b1, and Comparative Examples b2 to b4, the weight change rate of the sealant resin composition obtained in the above-mentioned Examples A1 and A8 to A9, the polymer used in the above-mentioned Comparative Example a1, and the sealant resin composition obtained in the above-mentioned Comparative Examples a2 to a4 were each measured based on the method described in the above-mentioned "Weight change rate after non-aqueous solvent immersion" and measured based on the method described in the above-mentioned "Mechanical properties after EC / DEC immersion".

[0394] On the other hand, in Examples B10 to B11, the same operation as in Example A1 was performed except that the polymers shown in Tables 1 and 3 were used instead of the polymer constituting the sealant resin composition used in Example A1 to obtain a sealant resin composition. For each of the obtained sealant resin compositions, a whitening resistance test according to the method described in the above "whitening resistance test", a weight change rate measurement according to the method described in the above "weight change rate after non-aqueous solvent immersion", and a measurement according to the method described in the above "mechanical properties after EC / DEC immersion" were performed.

[0395] The obtained physical properties are shown in Table 3. For reference, Table 3 also shows the data on the whitening resistance described in Table 2-1 and Table 2-2 for the sealant resin compositions obtained in Examples A1 and A8 to A9, the polymer used in Comparative Example a1, and the sealant resin compositions obtained in Comparative Examples a2 to a4.

[0396] [Table 3]

[0397] Table 3

[0398]

[0399] From the comparison results of Examples B10 and B11 with Comparative Example b2, and the comparison results of Example B9 with Comparative Example b4 shown in Table 3, it can be seen that the sealant resin composition of the present invention has a smaller weight change rate after non-aqueous solvent immersion, a smaller decrease in Young's modulus after EC / DEC immersion, and high whitening resistance than the composition containing propylene·ethylene copolymer instead of 1-butene·ethylene copolymer (A). From the comparison results of Example B1 with Comparative Example b1, it can be seen that when only random polypropylene is used instead of the sealant resin composition of the present invention, the physical properties after non-aqueous solvent immersion are good, but the whitening resistance is insufficient.

Claims

1. A sealant resin composition (X), comprising a 1-butene-ethylene copolymer (A) satisfying the following requirements (A1), (A2) and (A5), and a propylene polymer (B), wherein the resin composition satisfies the following requirements (X1) and (2 of X1), Requirement (A1): The content of the structural unit (i) derived from 1-butene is in the range of 70 to 99.9 mol %, and the content of the structural unit (ii) derived from ethylene is in the range of 0.1 to 30 mol %, wherein: The total amount of structural unit (i) and structural unit (ii) is set to 100 mol %; Requirement (A2): Use 13 The isotactic pentad fraction (mmmm) calculated by C-NMR is in the range of 80 to 99.9%; Requirement (A5): Using a differential scanning calorimeter (DSC), the temperature is temporarily cooled from 30°C to -70°C at a cooling rate of 20°C / min (first cooling), then maintained at -70°C for 5 minutes, and then heated from -70°C to 200°C at a heating rate of 20°C / min (first heating), and then maintained at 200°C for 10 minutes. Then, the temperature is cooled to -70°C at a cooling rate of 20°C / min (second cooling), and then maintained at -70°C for 1 minute. Then, the temperature is again heated from -70°C to 200°C at a heating rate of 20°C / min (second heating), and no melting peak is observed during the second heating. Requirement (X1): The Shore D hardness measured in accordance with ASTM D2240 is within the range of 44 to 80; Requirement (2 of X1): The melt flow rate (MFR) measured at 230° C. and a load of 2.16 kg in accordance with ASTM D1238 is within the range of 0.1 to 100 g / 10 minutes.

2. The sealant resin composition (X) according to claim 1, which satisfies the following requirement (X2): Requirement (X2): Using a differential scanning calorimeter (DSC), temporarily cool from 30°C to -70°C at a cooling rate of 20°C / min (first cooling), then hold at -70°C for 5 minutes, increase the temperature from -70°C to 200°C at a heating rate of 20°C / min (first heating), hold at 200°C for 10 minutes, then cool to -70°C at a cooling rate of 20°C / min (second cooling), hold at -70°C for 1 minute, and then increase the temperature from -70°C to 200°C at a heating rate of 20°C / min (second heating). The melting enthalpy ΔHfus at this time is in the range of 20 to 100 J / g. 3 . The sealant resin composition (X) according to claim 1 , comprising a vinyl polymer (C).

4. The sealant resin composition (X) according to claim 1, which satisfies the following requirement (X3): Requirement (X3): The content of the 1-butene-ethylene copolymer (A) is in the range of 1 to 50% by mass, the content of the propylene polymer (B) is in the range of 30 to 99% by mass, and the content of the ethylene polymer (C) is in the range of 0 to 20% by mass, wherein: The total amount of the 1-butene / ethylene copolymer (A), the propylene polymer (B), and the ethylene polymer (C) is 100% by mass.

5. The sealant resin composition (X) according to claim 1, wherein The 1-butene-ethylene copolymer (A) satisfies the following requirement (A3), Requirement (A3): The intrinsic viscosity [η] in a decalin solvent at 135° C. is within a range of 0.7 to 4.0 dl / g.

6. The sealant resin composition (X) according to claim 1, wherein The propylene-based polymer (B) includes one or more selected from the group consisting of random copolymers and block copolymers.

7. A single-layer or multi-layer sealant film comprising at least one layer comprising the sealant resin composition (X) according to claim 1.

8. A laminated body comprising at least one substrate film selected from the group consisting of polyolefin films, polystyrene films, polyester films, polyamide films, laminated films of polyolefin and gas barrier resin films, metal foils, paper, and vapor-deposited films laminated on the sealant film layer according to claim 7.

9. The laminate according to claim 8, wherein: The sealant film layer and the base film are bonded together by any one of melt extrusion lamination, heat lamination, and dry lamination.

10. The laminate according to claim 8, wherein The substrate film is aluminum foil.

11. A packaging body comprising the laminate according to claim 9 or 10. 12 . An electric storage device comprising the laminate according to claim 9 . 13 . A lithium ion battery package comprising the laminate according to claim 9 or 10.

14. An electrical storage device comprising a sealant resin composition (X), The sealant resin composition (X) contains a 1-butene-ethylene copolymer (A) and a propylene-based polymer (B), and satisfies the following requirement (X1): Requirement (X1): The Shore D hardness measured in accordance with ASTM D2240 is within the range of 44 to 80.

15. The power storage device according to claim 14, which is a lithium ion battery.

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