JP2003096203A - Thermoplastic elastomer composition and its manufacturing method - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a method of manufacturing a thermoplastic elastomer composition which is excellent in the shape of a calender bank and roller separability during calendaring and capable of affording a calendered article with good appearance and to provide the thermoplastic elastomer composition. SOLUTION: In this method a mixture comprising the following components (A) 35-95 wt.%, (B) 5-65 wt.% (wherein, (A)+(B)=100 wt.%) and (C) 0.005-20 pts.wt. (wherein, (A)+(B)=100 pts.wt.) is dynamically heat treated in the presence of a crosslinking agent: (A) an oil-extended rubber of an olefin copolymer having a Mooney viscosity of 20-350 composed of 100 pts.wt. of an olefin copolymer rubber and 20-150 pts.wt. of a mineral oil-based softener, (B) a crystalline polyolefin and (C) a hydrogenated copolymer of an aromatic vinyl compound and a conjugated diene.

Description

Detailed Description of the Invention

[0001]

TECHNICAL FIELD The present invention relates to a method for producing a thermoplastic elastomer composition for calendering and a composition obtained by the method. More specifically, it relates to a method for producing a thermoplastic elastomer composition which is excellent in a bank shape and a roll-releasing property at the time of calender molding, and which gives a calender molded article having a good appearance, and for calender molding obtained by the manufacturing method. The present invention relates to a thermoplastic elastomer composition.

[0002]

2. Description of the Related Art In recent years, from the viewpoint of environmental problems such as recycling and hygiene, a soft vinyl chloride resin material has been used,
The use of olefin-based thermoplastic elastomer materials has been investigated, and particularly in the fields of films and sheets, calender-moldable materials having excellent thickness accuracy and high-speed productivity are required. However, since the olefinic thermoplastic elastomer adheres to a calender roll during calender molding and the surface of the molded sheet becomes rough,
Molding was difficult. As a method for solving such a problem, for example, in Japanese Patent Publication No. 2-37942, adding a higher fatty acid amide is disclosed in JP-A-7-2607.
Japanese Patent Publication 7 discloses adding metal soap. Further, JP-A No. 7-166012 discloses the use of an oil-extended olefin copolymer rubber.

[0003]

However, in the above method, although the effect of improving the calendering workability is recognized,
It wasn't quite satisfactory. Under such circumstances,
The problem to be solved by the present invention is to provide a method for producing a thermoplastic elastomer composition capable of obtaining a calendered article having a bank shape during calendering, an excellent roll-releasing property, and a good appearance. It is to provide a plastic elastomer composition.

[0004]

That is, the first aspect of the present invention is to provide the following components (a) 35 to 95% by weight and (b) 5 to 65%.
% By weight (however, (a) + (b) = 100% by weight) and (c) 0.005 to 20 parts by weight (however,
(A) + (B) is 100 parts by weight. The present invention relates to a method for producing a thermoplastic elastomer composition for calender molding, which comprises subjecting a mixture of the above) to a dynamic heat treatment in the presence of a crosslinking agent. (A): An oil-extended olefin copolymer rubber comprising 100 parts by weight of an olefin copolymer rubber and 20 to 150 parts by weight of a mineral oil-based softener, and having a Mooney viscosity (ML _{1 + 4} 100 ° C.) of 20 to 350. (B): Crystalline polyolefin. (C): Hydrogenated product of copolymer of vinyl aromatic compound and conjugated diene. A second aspect of the present invention relates to a calender molding thermoplastic elastomer composition obtained by the above-mentioned production method.

[0005]

BEST MODE FOR CARRYING OUT THE INVENTION The oil-extended olefin copolymer rubber (a) of the present invention contains an olefin copolymer rubber and a mineral oil-based softening agent. The olefin copolymer rubber is a repeating unit derived from one or more olefins having 2 to 10 carbon atoms such as ethylene, propylene, 1-butene, 1-pentene, 1-hexene, and 1-octene. A polymer containing, according to JIS K
A polymer having an A hardness of −6301 (1975) of 98 or less. The olefin copolymer rubber may contain a repeating unit derived from a monomer other than olefin,
Examples of the other monomer include 1,3-butadiene,
2-methyl-1,3-butadiene (isoprene), 1,
C4-C8 conjugated dienes such as 3-pentadiene and 2,3-dimethyl-1,3-butadiene; dicyclopentadiene, 5-ethylidene-2-norbornene, 1,4-
Hexadiene, 1,5-dicyclooctadiene, 7-methyl-1,6-octadiene, 5-vinyl-2-norbornene and other non-conjugated dienes having 5 to 15 carbon atoms; vinyl ester compounds such as vinyl acetate; acryl Unsaturated carboxylic acid esters such as methyl acrylate, ethyl acrylate, butyl acrylate, methyl methacrylate, ethyl methacrylate; unsaturated carboxylic acids such as acrylic acid and methacrylic acid, and one or more of them are used. To be The olefin copolymer rubber may be used alone or in combination of two or more.

Examples of the olefin copolymer rubber include polypropylene, poly-1-butene, ethylene-propylene copolymer, ethylene-1-butene copolymer, ethylene-1-hexene copolymer and ethylene-1-octene. Copolymer, propylene-1-butene copolymer, propylene-1-hexene copolymer, propylene-1-octene copolymer, ethylene-propylene-5-ethylidene-2
-Norbornene copolymer, ethylene-propylene-1-
Examples thereof include butene copolymer, ethylene-propylene-1-hexene copolymer, and ethylene-propylene-1-octene copolymer, and these can be produced by a known method.

Among the olefin copolymer rubbers, ethylene-α-olefin copolymers and ethylene-α-olefin-non-conjugated diene copolymers are preferable. Here, the α-olefin is an olefin having 3 to 10 carbon atoms. From the viewpoint of easy availability, the α-olefin is preferably propylene or 1-butene, more preferably propylene, and the non-conjugated diene is 5-ethylidene-.
2-norbornene. Weight ratio of the content of repeating units derived from ethylene and the content of repeating units derived from α-olefin of the olefin copolymer rubber (ethylene unit content / α-olefin unit content)
Is preferably 90/10 to 30/7 from the viewpoint of flexibility.
It is 0, more preferably 85/15 to 45/55, and further preferably 80/20 to 60/40. The content of the non-conjugated diene unit in the olefin copolymer rubber is preferably 1 to 30% by weight, more preferably 3 to 20%.
% By weight. If the content of the non-conjugated diene unit is too small, the mechanical strength may decrease, and if it is too large, the motor load of the extruder may increase.

As the mineral oil-based softening agent contained in the oil-extended olefin copolymer rubber (a), an extension oil usually used for adjusting oil-extended rubber can be used. For example, paraffin-based mineral oil, High-boiling fractions of petroleum such as naphthenic mineral oils and aromatic mineral oils (average molecular weight of 300 to 150)
0, and the pour point is 0 ° C. or lower).

The blending amount of the mineral oil-based softening agent is 20 to 1 of the mineral oil-based softening agent per 100 parts by weight of the olefin copolymer rubber.
It is 50 parts by weight. If the amount of the mineral oil-based softening agent is too small, the bank shape and the sheet appearance may deteriorate, and if the amount of the mineral oil-based softening agent is too large, roll fouling may occur. The amount is preferably 25 to 130 parts by weight, more preferably 30 to 120 parts by weight.

The Mooney viscosity (ML _{1 + 4} 100 ° C.) of the oil-extended olefin copolymer rubber (a) is 20 to 350. If the Mooney viscosity is too low, mechanical strength may decrease, and if the Mooney viscosity is too high, moldability may decrease. It is preferably 30 to 150,
More preferably, it is 40-100.

As a method for blending the olefin copolymer rubber and the mineral oil-based softening agent for producing the oil-extended olefin copolymer rubber (a), a known method is used, for example, a roll, a Banbury mixer, an extrusion. Examples thereof include a method of melt-kneading using a machine and the like, a method of adding a mineral oil-based softening agent to an olefin copolymer rubber solution, and then a method of desolventizing by a method such as steam strip. Preferably, a mineral oil softener is added to the olefin copolymer rubber solution,
Then, a method of removing the solvent by a method such as steam strip is preferable.

The crystalline polyolefin (b) is derived from one or more olefins having 2 to 10 carbon atoms such as ethylene, propylene, 1-butene, 1-pentene, 1-hexene and 1-octene. Which is a polymer having an A hardness of 98 according to JIS K-6301 (1975).
It is a polymer exceeding. The crystalline polyolefin (b) may contain a repeating unit derived from a monomer other than an olefin, and other monomers include, for example,
Dicyclopentadiene, 5-ethylidene-2-norbornene, 1,4-hexadiene, 1,5-dicyclooctadiene, 7-methyl-1,6-octadiene, 5-vinyl-2-norbornene and the like having 5 carbon atoms. 15 to 15 non-conjugated diene; vinyl ester compound such as vinyl acetate; unsaturated carboxylic acid ester such as methyl acrylate, ethyl acrylate, butyl acrylate, methyl methacrylate, ethyl methacrylate; Examples thereof include saturated carboxylic acids, and these may be used alone or in combination of two or more. Further, the crystalline polyolefin (II) may be used alone or in combination of two or more kinds.

Examples of the crystalline polyolefin (B) include polyethylene, polypropylene, poly 1-butene, ethylene-propylene copolymer, ethylene-1-butene copolymer, ethylene-1-hexene copolymer, ethylene- 1-octene copolymer, propylene-1-butene copolymer, propylene-1-hexene copolymer, propylene-1-octene copolymer, ethylene-propylene-
5-ethylidene-2-norbornene copolymer, ethylene-propylene-1-butene copolymer, ethylene-propylene-1-hexene copolymer, ethylene-propylene-
1-octene copolymers are mentioned, and these can be produced by a known method.

Among the crystalline polyolefins (b), from the viewpoint of heat resistance, a propylene polymer having a content of repeating units derived from propylene of 80% by weight or more is preferable. The content of repeating units derived from propylene in the propylene polymer is more preferably 90% by weight or more, and further preferably 95% by weight or more.

The hydrogenated product (c) of a copolymer of a vinyl aromatic compound and a conjugated diene is a repeating unit derived from a vinyl aromatic compound having 8 to 12 carbon atoms and a conjugated diene having 4 to 8 carbon atoms. It is a copolymer obtained by hydrogenating the contained copolymer.

Examples of the vinyl aromatic compound having 8 to 12 carbon atoms in the hydrogenated product (c) of the copolymer of vinyl aromatic compound and conjugated diene include styrene, p-methylstyrene and α-methylstyrene. These may be used alone or in combination of two or more. Examples of the conjugated diene having 4 to 8 carbon atoms include 1,3-butadiene and 2-
Methyl-1,3-butadiene (isoprene), 1,3-
Examples include pentadiene and 2,3-dimethyl-1,3-butadiene, and these may be used alone or in combination of two or more.
Further, the hydrogenated product (c) of the copolymer of vinyl aromatic compound and conjugated diene may contain a repeating unit derived from a monomer other than the vinyl aromatic compound and conjugated diene. Examples of the monomer include dicyclopentadiene, 5-ethylidene-2-norbornene, 1,4
-Hexadiene, 1,5-dicyclooctadiene, 7-
Non-conjugated dienes having 5 to 15 carbon atoms such as methyl-1,6-octadiene and 5-vinyl-2-norbornene; vinyl ester compounds such as vinyl acetate; methyl acrylate, ethyl acrylate, butyl acrylate, methacrylic acid Unsaturated carboxylic acid esters such as methyl, ethyl methacrylate, glycidyl acrylate, glycidyl methacrylate, hydroxyethyl acrylate, dimethylaminoethyl methacrylate; unsaturated carboxylic acids such as acrylic acid, methacrylic acid, maleic acid; maleic anhydride, etc. Acid anhydrides; vinyl compounds containing epoxy groups such as allyl glycidyl ether; vinyl compounds containing isocyanate groups such as isopropenyl isocyanate; vinyl nitrile compounds such as acrylonitrile and methacrylonitrile.

Examples of hydrogenated products (c) of copolymers of vinyl aromatic compounds and conjugated dienes include styrene-
Hydrogenated product of 1,3-butadiene copolymer, styrene-
Examples thereof include hydrogenated products of isoprene copolymers, which can be produced by known methods.

The content of the repeating unit derived from the vinyl aromatic compound in the hydrogenated product (c) of the copolymer of vinyl aromatic compound and conjugated diene is preferably 1 to 7.
It is 0% by weight, more preferably 5 to 50% by weight, still more preferably 7 to 35% by weight. If the content of the vinyl aromatic compound unit is too small, the sheet appearance may be deteriorated, and if the content of the vinyl aromatic compound unit is too large, flexibility and low temperature impact resistance may be deteriorated.

The hydrogenated product (c) of the copolymer of vinyl aromatic compound and conjugated diene may have one block structure or two or more different block structures. As the structure consisting of one block, a hydrogenated product of a copolymer having a structure in which a vinyl aromatic compound and a conjugated diene or an olefin are randomly arranged, for example, a copolymer of a structure in which styrene and butadiene are randomly arranged. Examples thereof include hydrogenated products of polymers. Examples of the block composed of two or more blocks having different structures include a hydrogenated product of a copolymer composed of a styrene homopolymer block-butadiene homopolymer block-styrene homopolymer block, and a styrene homopolymer. Block-Styrene-Butadiene Copolymer Block-
An example is a hydrogenated product of a copolymer composed of styrene homopolymer blocks. In the hydrogenated product of such a copolymer, the styrene-butadiene copolymer block is a block having a structure in which styrene and butadiene are randomly copolymerized. Or a block having a tapered structure in which the content of styrene units gradually decreases.

The hydrogenated product (c) of a copolymer of a vinyl aromatic compound and a conjugated diene can be prepared by a known hydrogenation method.
It is obtained by saturating a double bond of a repeating unit derived from a conjugated diene of a copolymer of a vinyl aromatic compound and a conjugated diene, and the saturated amount is 100% of the conjugated diene unit.
%, Usually 80 mol% or more, preferably 9
It is 0 mol% or more, and more preferably 95 mol% or more. If the saturation amount is too small, the thermal stability may be poor.

Regarding the blending amount of the oil-extended olefin copolymer rubber (a), the crystalline polyolefin (b) and the hydrogenated product (c) of the copolymer of vinyl aromatic compound and conjugated diene, the oil-extended olefin copolymer Oil-extended olefin copolymer rubber (ii) / crystalline polyolefin (ii) based on 100% by weight of the total amount of rubber (ii) and crystalline polyolefin (ii)
Is 35 to 95/5 to 65% by weight, preferably 4
5 to 90/10 to 60% by weight, more preferably 5
5 to 85/15 to 55, and the total amount of the oil-extended olefin copolymer rubber (a) and the crystalline polyolefin (b) is 1
The blending amount of the hydrogenated product (c) of the copolymer of vinyl aromatic compound and conjugated diene is 0.005 to 100 parts by weight.
It is 20 parts by weight, preferably 0.01 to 15 parts by weight, and more preferably 0.05 to 10 parts by weight. If the oil-extended olefin copolymer rubber (a) is too small, the flexibility of the molded product may be poor, and if it is too large, the processability may be poor. If the amount of the crystalline polyolefin (b) is too small, the processability may be poor, and if it is too large, the flexibility of the molded product may be poor. If the hydrogenated product (c) of the copolymer of vinyl aromatic compound and conjugated diene is too small, the sheet appearance and the bank shape may be inferior, and if it is too large, flexibility and low temperature impact resistance may be deteriorated.

The cross-linking agent cross-links a composition comprising an oil-extended olefin copolymer rubber (a), a crystalline polyolefin (b) and a hydrogenated product (c) of a copolymer of a vinyl aromatic compound and a conjugated diene. And organic oxides. Examples of organic oxides include dicumyl peroxide, di-t-butyl peroxide, and 2,5.
-Dimethyl-2,5-di- (t-butylperoxy) hexane, 2,5-dimethyl-2,5-di (t-butylperoxy) hexyne-3,1,3-bis (t-butylperoxyisopropyl) Benzene, 1,1-bis (t-
Butylperoxy) -3,3,5-trimethylcyclohexane, n-butyl-4,4-bis (t-butylperoxy) valerate, benzoyl peroxide, p-chlorobenzoyl peroxide, 2,4-dichlorobenzoyl peroxide, t-butyl Peroxybenzoate,
Examples thereof include t-butylperoxyisopropyl carbonate, diacetyl peroxide, lauroyl peroxide, and t-butylcumyl peroxide, which usually have a half-life of 1
A temperature of 150 to 280 ° C. is used.
You may use these 1 type or in combination of 2 or more types.

The amount of the cross-linking agent to be added is a hydrogenated product (c) of a copolymer of oil-extended olefin copolymer rubber (a), crystalline polyolefin (b), vinyl aromatic compound and conjugated diene.
The total amount is preferably 0.001 with respect to 100 parts by weight.
~ 5 parts by weight. If the blending amount is too small, the mechanical strength of the molded product may decrease. If the blending amount is too large, the motor load of the extruder may increase. The amount is more preferably 0.005 to 3 parts by weight, and further preferably 0.01 to 1 part by weight.

Improve the uniformity of cross-linking of a composition comprising an oil-extended olefin copolymer rubber (a), a crystalline polyolefin (b), and a hydrogenated product (c) of a copolymer of a vinyl aromatic compound and a conjugated diene. For this purpose, a crosslinking aid may be added. Processing aids include divinylbenzene, ethylene glycol dimethacrylate, polyethylene glycol dimethacrylate, 1,3-butylene glycol dimethacrylate, trimethylolpropane trimethacrylate, pentaerythritol triacrylate, neopentyl glycol diacrylate, allyl methacrylate, diallyl phthalate. , Diallyl terephthalate, triallyl cyanurate, triallyl isocyanurate,
Polyfunctional vinyl monomers such as tetraaryloxyethane; N, N'-m-phenylene bismaleimide, N,
N'-p-phenylene bismaleimide, bismaleimide compounds such as N, N'-ethylene bismaleimide; p-
Examples thereof include peroxide crosslinking aids such as quinone oxime and p, p'-dibenzoylquinone dioxime.

The amount of the crosslinking aid compounded is the total amount of the hydrogenated product (c) of the copolymer of oil-extended olefin copolymer rubber (a), crystalline polyolefin (b), vinyl aromatic compound and conjugated diene. To 100 parts by weight, preferably 0.
001-5 parts by weight, more preferably 0.01-3
Parts by weight, and more preferably 0.05 to 2 parts by weight. If the blending amount is too small, the effect of uniformity of crosslinking may be small, and if the blending amount is too large, the motor load of the extruder may be increased.

The dynamic heat treatment for obtaining the thermoplastic elastomer composition of the present invention means oil-extended olefin copolymer rubber (a), crystalline polyolefin (b), a copolymer of a vinyl aromatic compound and a conjugated diene. Melting and kneading a mixture of hydrogenated products (C) in the presence of a crosslinking agent. As the dynamic heat treatment device, known devices such as an open type mixing roll, a non-open type Banbury mixer, a kneader and an extruder can be used. Further, in the melt-kneading of the dynamic heat treatment, all the components to be kneaded may be melt-kneaded together, or some of the components may be kneaded and then unselected components may be added and melt-kneaded. May be performed once or more than once. From the viewpoint of uniformity of cross-linking, preferably,
It is preferable to melt-knead all the components to be kneaded together.

The temperature of the dynamic heat treatment is usually such that when the organic oxide is used as the crosslinking agent, the half-life of the organic peroxide is 1.
It is a temperature of not more than minutes, preferably 150 to 280
C., more preferably 180 to 260.degree. The time for the dynamic heat treatment is usually the half life of the organic peroxide or more, preferably 1 to 30 minutes, more preferably 3 to 20 minutes. If the temperature is too low or the time is too short, the mechanical strength of the molded product may decrease, and if the temperature is too high or the time is too long, the motor load of the extruder may increase.

The thermoplastic elastomer composition of the present invention comprises
Melt flow rate is preferably 0.1 to 100 g /
It is 10 minutes, more preferably 0.5 to 80 g / 10 minutes, still more preferably 1 to 60 g / 10 minutes. If the melt flow rate is too low, the motor load of the extruder may increase, and if the melt flow rate is too high, the mechanical strength of the molded product may decrease. Here, the melt flow rate is JIS K-7210 (1
976) at a temperature of 230 ° C and a load of 98.07N.

The thermoplastic elastomer composition of the present invention comprises
If necessary, antioxidant, weather resistance stabilizer, antistatic agent,
You may mix | blend additives, such as a mold release agent, a flame retardant, a metal soap, wax, an antifungal agent, an antibacterial agent, a filler, a foaming agent.
These additives may be blended before the dynamic heat treatment or after the dynamic heat treatment.

The thermoplastic elastomer composition of the present invention comprises
It can be used as a material suitable for calendar molding,
The calender molded article is used for, for example, automobile interior parts such as instrument panels and door trims, footwear such as shoe soles and sandals, leisure sheets, gaskets, waterproof sheets, bags, belts and covers.

[0031]

EXAMPLES The present invention will be described below with reference to examples.

[1] Evaluation Method (1) Mooney Viscosity (ML _{1 + 4} 100 ° C.) It was measured at 100 ° C. according to ASTM D-927-57T. (2) Melt flow rate According to JIS K-7210 (1976), temperature 23
It was measured at 0 ° C. and a load of 98.07N. (3) Calender processability Roll temperature of 170 ° C., guide width of 30 cm, roll gap adjusted to 0.6 mm, using two rolls (Kansai Roll's 8-inch roll), melt-kneading 150 g of pellets,
The sheet was molded. The shape of the bank during melt-kneading and the adhesion to the heating roll were evaluated as follows. <Bank shape> ○: A uniform bank shape without disturbance. Δ: Disturbance sometimes occurs. ×: Always disturbed, no normal bank can be formed. <Roll Adhesiveness> Good: Almost no resistance when the sheet is manually peeled from the roll surface. Δ: There is some peel resistance when the sheet is manually peeled from the roll surface. X: There is a large peel resistance when the sheet is manually peeled from the roll surface. (4) Appearance of Sheet The appearance of the formed sheet was visually determined as follows. ○: Almost no roughness on the sheet surface. Δ: Some slight roughness is seen on the surface of the sheet. X: Large roughness is seen on the sheet surface.

[2] Raw material oil-extended olefin copolymer rubber Esprane EPDM E673 manufactured by Sumitomo Chemical Co., Ltd.
(Composition of 100 parts by weight of ethylene-propylene-5-ethylidene-2-norbornene copolymer and Idemitsu Kosan, Diana Process Oil PW-380: 40 parts by weight, ML
_{1 + 4} 100 ° C. = 78) Crystalline polyolefin Sumitomo Chemical Co., Ltd. Noblene AH161C (ethylene-propylene copolymer) Hydrogenated product of copolymer of vinyl aromatic compound and conjugated diene JSR Corporation Dynaron 1320P, 1321P Organic peroxide chemical agent Akzo Co., Ltd. 2,5-dimethyl-2,5-di (t-butylperoxy) hexane crosslinking aid Seiko Chemical Co., Ltd. High Cross MP (Trimethylolpropane trimethacrylate) Antioxidant Agent Ciba Specialty Chemicals Irganox 1010 Weather Stabilizer Sumitomo Chemical Co., Ltd. Sumisorb 300 Wax Kao KAO-WAX 230-2

[3] Preparation of Thermoplastic Elastomer Compositions Examples 1 to 3 and Comparative Example 1 Oil-extended olefin copolymer rubber, crystalline polyolefin, vinyl aromatic compound and conjugated diene in the compounding amounts shown in Table 1 were prepared. A hydrogenated product of a copolymer, a crosslinking aid, an antioxidant, a weather resistance stabilizer and a wax are mixed with a Banbury mixer at 170-
The mixture was kneaded at 200 ° C. for 7 minutes, and an undynamically heat-treated resin composition pellet was produced using an extruder. Next, the undynamically heat-treated resin composition pellets having the compounding amounts shown in Table 1 and the organic peroxide were blended for 10 minutes using a Henschel mixer. This blend is heated at 230 ° C ± 2 with a twin-screw kneading extruder.
Dynamic heat treatment was performed at 0 ° C. for 60 seconds to obtain a dynamically heat-treated thermoplastic elastomer composition. The evaluation results are shown in Table 1.

[0035]

[Table 1]

[0036]

According to the present invention, an oil-extended olefin copolymer rubber, a crystalline polyolefin, a hydrogenated product of a copolymer of a vinyl aromatic compound and a conjugated diene, and a crosslinking agent, which are excellent in calender moldability, are subjected to a dynamic heat treatment. The thermoplastic elastomer composition thus obtained could be provided. The thermoplastic elastomer composition calender molded article has excellent appearance and mechanical strength, for example, automobile interior parts such as instrument panels and door trims, footwear such as shoe soles and sandals, leisure sheets, gaskets, waterproof sheets, Used for bags, belts, covers, etc.

   ─────────────────────────────────────────────────── ─── Continued front page    (72) Inventor Hiroshi Oyama             Sumitomo Chemical Co., Ltd. 1-5 Anezaki Kaigan, Ichihara City, Chiba Prefecture             Business F-term (reference) 4F070 AA06 AA12 AA13 AA15 AA16                       AA18 AA63 AC56 AC94 AE02                       AE08 GA05 GA07 GB07 GC02                 4J002 AC08Z AC11Z AE04X AE05X                       BB02Y BB09W BB11W BB11Y                       BB14W BB14Y BB15W BB17Y                       BB18W BC05Z EK036 EK046                       EK056 EK066 FD146 GG00                       GL00

Claims (4)

[Claims] 1. The following components (a) 35 to 95% by weight, (b)
5 to 65% by weight (however, (a) + (b) = 100% by weight) and (c) 0.005 to 20 parts by weight (however, (a) + (b) is 100 parts by weight) A method for producing a thermoplastic elastomer composition for calender molding, which comprises subjecting a mixture of the composition (1) and (2) to a dynamic heat treatment in the presence of a crosslinking agent. (A): An oil-extended olefin copolymer rubber comprising 100 parts by weight of an olefin copolymer rubber and 20 to 150 parts by weight of a mineral oil-based softener, and having a Mooney viscosity (ML _{1 + 4} 100 ° C.) of 20 to 350. (B): Crystalline polyolefin. (C): Hydrogenated product of copolymer of vinyl aromatic compound and conjugated diene. 2. The method for producing a thermoplastic elastomer composition for calendar molding according to claim 1, wherein the crystalline polyolefin is a propylene polymer. 3. A thermoplastic elastomer composition for calender molding obtained by the method according to claim 1. 4. A thermoplastic elastomer composition for calender molding obtained by the method according to claim 1 or 2, which has a melt flow rate of 0.1 to 100.