JP2001031799A - Resin composition and profile extrusion produt - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain a profile extrusion product excellent in surface appearance by compounding a composition comprising a polyolefin resin and a cellulosic filler in a specified ratio with polytetrafluoroethylene, each in a specified amount. SOLUTION: The resin composition contains 100 pts.wt. composition comprising 30 to 80 wt.% polyolefin resin and 20 to 70 wt.% cellulosic filler (e.g. a chaff powder or a wood meal pulverized so as to pass through a 10-mesh metal net), 0.01 to 10 pts.wt. fibril-like polytetrafluoroethylene having an average diameter of 5 μm or lower, 0.01 to 10 pts.wt. polar-group-containing polymer (e.g. a polymer of an acrylate monomer), etc. Examples of the pololefin resin are preferably a high-density polyethylene and a propylene-α-olefin block or random copolymer, a copolymer comprising 90 to 99.9 wt.% propylene units and 0.1 to 10 wt.% ethylene or 1-butene units.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

The present invention relates to a resin composition containing a cellulosic filler, and a profile-extruded product comprising the resin composition. More specifically, the present invention relates to a resin composition which uses a polyolefin-based resin, has good moldability, and can provide a molded article having a good surface appearance, and a profile extrusion molded article using the same.

[0002]

2. Description of the Related Art Conventionally, attempts have been made to provide a resin composition in which a polyolefin resin is blended with a cellulosic filler such as wood flour to various molding materials in order to give the resin a woody feel or enable nailing. Many have been made.

However, a resin composition comprising a polyolefin resin and a large amount of a cellulosic filler such as wood flour has a remarkably reduced fluidity at the time of melting, impairs workability, and has poor surface appearance of a molded article. Molding defects are likely to occur. Further, since there is no affinity between the polyolefin and the cellulosic filler, the dispersibility of the compounded cellulosic filler is poor, which not only causes poor surface appearance and molding failure of the molded article, but also causes the molded article to have a poor shape. There is a problem that the mechanical strength is reduced.

In order to improve the fluidity of a polyolefin resin containing a cellulose filler, a method of blending an organic peroxide has been proposed (Japanese Patent Publication No. 62-1987).
No. 5186, Japanese Patent Publication No. Hei 1-222297, etc.).

[0005] However, in the resin composition obtained by these methods, although the injection moldability and the appearance of the molded product obtained by the method are improved to some extent,
Extrusion molding, in particular, profile extrusion molding, has rather problems such as impairing the surface appearance and increasing the drawdown during extrusion, making the molding process itself difficult.

As a proposal focusing on improving the affinity between a polyolefin resin and a cellulose-based filler, a part or all of the polyolefin resin is graft-polymerized with a monomer having a polar group such as maleic acid. Affinity is improved by using a modified so-called acid-modified polyolefin (for example, JP-A-55-131031, JP-A-61-155436, JP-A-57-4).
No. 2751, JP-A-59-115335, etc.)
Has also been proposed. In these methods, by improving the affinity between the polyolefin-based resin and the cellulosic filler, the uniform mixing properties of the two can be improved to some extent, the mechanical strength can be improved, and the appearance of the molded article in injection molding can be improved. However, it was still difficult to say that the composition was suitable for extrusion molding.

That is, these means improve the resin raw material in which the cellulosic filler is blended, and improve the fluidity and affinity, so that the transferability to a mold in injection molding is improved, and Is based on the technical idea of improving the surface appearance of the above. However, in the profile extrusion molding, with the raw material having improved fluidity as described above, the melt viscosity and the melt tension are extremely reduced, so that the profile extrusion molding becomes difficult.

Therefore, in the profile extrusion, a raw material in which wood powder is blended with a vinyl chloride resin having a high melt tension has been generally used, and in the field of building materials, it has been used as a building member for interior and exterior of houses. It was.

However, vinyl chloride resins may emit plasticizers at the time of use, generate toxic hydrogen chloride gas at the time of fire, and may generate harmful substances at the time of incineration and disposal due to environmental awareness in recent years. There is an increasing demand for converting vinyl chloride resins into polyolefins, and there has been a demand for the development of new raw materials comprising a polyolefin-based resin and a cellulose-based filler and having excellent deformability.

Therefore, in recent years, it has been considered that obtaining a polyolefin-based resin composition capable of being profile-extruded is an important issue, and various studies have been made. As one example, a method of paying attention to a mixing means of a polyolefin-based resin and a woody material, performing uniform mixing by performing melt-kneading within a certain energy range, and preventing thermal deterioration of the woody material (Japanese Patent Laid-Open No. No. 10-273538), and an attempt to partially deform a polyolefin resin to increase the melt tension to enable profile extrusion (Japanese Patent Laid-Open No. 10-330624).

In these methods, although the profile extrusion moldability is improved to some extent, there is still room for improvement in the sufficient moldability and appearance of the molded product, particularly in the smoothness of the surface.

[0012]

SUMMARY OF THE INVENTION Accordingly, an object of the present invention is to solve the above problems,
Using a polyolefin-based resin, a resin composition containing a cellulosic filler capable of stably molding a profile-extruded product having a good surface appearance with good moldability, and a profile extrusion molding comprising the composition To provide goods.

[0013]

Means for Solving the Problems The present inventors have intensively studied a polyolefin resin composition containing a cellulosic filler in order to solve these problems. As a result, surprisingly, by adding polytetrafluoroethylene to a composition comprising a polyolefin resin and a cellulosic filler, the profile extrusion moldability is dramatically improved, and the surface appearance is extremely excellent. The present inventors have found that an irregular shaped article can be obtained stably, and have completed the present invention.

That is, the present invention comprises 0.01 to 10 parts by weight of polytetrafluoroethylene per 100 parts by weight of a composition comprising 30 to 80% by weight of a polyolefin resin and 20 to 70% by weight of a cellulosic filler. And a profile extruded product comprising the resin composition.

In the present invention, in particular, polytetrafluoroethylene is used in a matrix of a polyolefin and a cellulosic filler so that extremely fine fibers having an average diameter of 5 μm or less, particularly 0.01 to 0.1 μm, are formed into fibrils. In the case where it is present, a particularly excellent effect is exhibited. Therefore, a preferred embodiment of the present invention is a polytetrafluoroethylene is a polyolefin 30-80 wt%,
The invention also includes the invention of a resin composition characterized by being dispersed as a fibrous material having an average diameter of 5 μm or less in 100 parts by weight of a matrix composed of 20 to 70% by weight of a cellulosic filler.

Furthermore, in the present invention, by forming a polymer containing a polar group-containing polymer in a proportion of 0.01 to 10 parts by weight in each of the above-mentioned compositions, the moldability such as profile extrusion can be improved. A further improved composition is also provided.

The present invention also provides a profile-extruded product using each of the above compositions.

[0018]

DESCRIPTION OF THE PREFERRED EMBODIMENTS As the polyolefin resin used in the present invention, known polyolefin resins can be used without any limitation. That is, a homopolymer of an α-olefin such as ethylene, propylene, or butene-1, a copolymer of ethylene and an α-olefin, a copolymer between α-olefins, and further mainly ethylene or an α-olefin. As the component, a copolymer with another monomer copolymerizable therewith, for example, styrene, methyl acrylate, methyl methacrylate and the like is included. Among these, preferred polyolefin-based resins are high-density polyethylene, linear low-density polyethylene, propylene homopolymer, propylene as a main component, and a block or random copolymer thereof with an α-olefin other than ethylene or propylene. It is. Examples of such α-olefins include 1-butene, 1-pentene, 1-hexene, 1-heptene, 1-
Octene, 3-methyl-1-butene, 4-methyl-1-
Penten and the like can be mentioned. A particularly suitable polyolefin resin is a copolymer containing propylene as a main component and ethylene or an α-olefin other than propylene. The amount of the ethylene or α-olefin to be copolymerized with propylene is not particularly limited, but is generally preferably about 0.1 to 10% by weight.

In the present invention, the most recommended polyolefin resin is a copolymer of 90 to 99.9% by weight of propylene and 0.1 to 10% by weight of ethylene or 1-butene.

The polyolefin resin used in the present invention preferably has a melt flow rate measured in accordance with JIS K7210 in a range of 0.1 to 20 g / 10 minutes, more preferably 0.2 to 10 g / min. It is preferably 10 minutes, particularly preferably 0.3 to 5 g / 10 minutes. When the melt flow rate of the polypropylene resin is less than 0.1 g / min, the productivity at the time of profile extrusion molding of the obtained resin composition tends to decrease, and when the melt flow rate exceeds 20 g / min. , The shape of the extruded molded product tends to be poor due to drawdown or the like.

The method for producing the polyolefin resin is not particularly limited, and it can be obtained according to a known polymerization method.

Examples of the cellulosic filler used in the present invention include wood, chaff, bamboo, starch, paper, pulp, pulverized materials such as waste paper and corrugated cardboard, and the like. These may be used alone or in combination of two or more. Can be used.
The shape and size of the cellulosic material are not particularly limited, but in the case of a heteromorphic product, considering the surface appearance,
The size is preferably reduced to a size that passes through a 10-mesh wire net, more preferably a size of 50 mesh passes or less, and still more preferably a size of 100 mesh passes or less.

The type of the above-mentioned cellulosic material may be arbitrarily selected in accordance with the performance required of the molded article. For example, considering that the resulting hetero-formed article is given a high woody feeling, rice husk powder Wood flour is particularly preferred.

The above-mentioned cellulosic material is generally hygroscopic. For example, if the cellulosic material has a water content of more than 10% by weight, foaming at the time of molding becomes severe, and the extrudability of the profile tends to be remarkably reduced. For this reason, it is preferable to dry and use it before mixing with the polyolefin resin of the present invention. Although the drying method is not particularly limited, a method in which the cellulosic material is dried in an oven or the like in advance or a method in which the cellulosic material is dried by heating and stirring in a mixer can be preferably employed. It is particularly preferable to use them.

The type of polytetrafluoroethylene used in the present invention is not particularly limited, and commercially available polytetrafluoroethylene can be used without any limitation. In particular, when preparing the resin composition of the present invention, for example, polytetrafluoroethylene that fibrillates into a fibrous shape by shearing force applied to the resin composition during mixing or granulation can be preferably used. Conversely, polytetrafluoroethylene in the form of wax cannot be used due to its low molecular weight like oligomers.

In the present invention, the content of polytetrafluoroethylene is 0.1 to 100 parts by weight of the composition of the present invention comprising a polyolefin resin and a cellulosic material.
0.01 to 10 parts by weight, preferably 0.05
To 5 parts by weight, more preferably 0.1 to 3 parts by weight.
If the content is less than 0.01 part by weight, the effect of improving the moldability of the obtained resin composition is not sufficient, and the surface appearance of the obtained hetero-formed product is unfavorable. If the content exceeds 10 parts by weight, the fluidity during the profile extrusion molding is lowered, and the cost is increased, which is not preferable.

The polytetrafluoroethylene contained in the resin composition of the present invention is in the form of a fibril having an average diameter of 5 μm or less, particularly 0.01 to 0.1 μm.
It is particularly preferable that there are many fine fibers of about m, for example, 50% or more, in order to further improve the moldability of the obtained resin composition and the surface appearance of the obtained profile-extruded product. By dispersing polytetrafluoroethylene at the above average diameter in the resin composition of the present invention, the melt tension of the resin composition is particularly improved. Therefore, when the resin composition is deformed by extrusion, the molten resin composition may be cut between the deformed die and the sizing mold, or the edge of the molded product may be partially cut, resulting in a poor surface condition. The effect of improvement is increased, the heteromorphic property is further improved, and a heteromorphic article excellent in surface appearance is easily obtained. In consideration of further improving the morphogenesis, the average diameter of the polytetrafluoroethylene of the present invention is preferably 3 μm or less, more preferably 1 μm or less, and particularly preferably 0.5 μm or less. Things are preferred.

The fiber length of the polytetrafluoroethylene of the present invention is not particularly limited, but is usually preferably at least 3 times the fiber diameter, more preferably at least 5 times, especially at least 10 times. Is preferred.

In the present invention, the method for making the average diameter of polytetrafluoroethylene into the fine fibrils as described above is not particularly limited, and any method may be used as long as it is a production method having the above average diameter in the resin composition. For example, a polyolefin-based resin and tetrafluoroethylene, or, a polyolefin-based resin and tetrafluoroethylene and a cellulose-based filler, in a super mixer or a gelation mixer, a method of stirring and mixing under high shear,
A method of melt-kneading using a single-screw or twin-screw extruder or the like can be used. Furthermore, polytetrafluoroethylene and another polymer, for example, a polyolefin, a polar group-containing polymer, or the like, are previously prepared by the above-described means so that fibrillation easily proceeds even under a relatively low shearing force under mixing conditions. Polytetrafluoroethylene-containing material that has been mixed and adjusted to a group with high shear force, and an aqueous dispersion of polytetrafluoroethylene particles and an aqueous dispersion of polar group-containing polymer particles are mixed and coagulated, or spray-dried. A method using the obtained polytetrafluoroethylene-containing mixed powder (for example, trade name Metablen A-3000 manufactured by Mitsubishi Rayon Co., Ltd.) can also be preferably employed.

The resin composition of the present invention may contain a polar group-containing polymer for the purpose of improving the compatibility between the polyolefin resin and the cellulosic material and further improving the surface appearance of the obtained molded article. Is more preferable.

The polar group-containing polymer of the present invention includes, for example,
A carbonyl group, a carboxyl group, or an anhydride group, an amino group, a cyano group, an epoxy group, a hydroxyl group, a polymer containing an ionic, hydrogen-bonding functional group or element such as a halogen, and the type of the polymer and The content of the polar group is not particularly limited. In the present invention, a polar group-containing polymer that can be particularly preferably used is, for example, a homopolymer of an acid-modified polyolefin such as maleated polypropylene, an acrylate-based monomer such as methyl (meth) acrylate or ethyl (meth) acrylate, or the above-mentioned monomer. Or a homopolymer of a vinyl cyanide monomer such as acrylonitrile or methacrylonitrile, or a homopolymer of a vinyl carboxylate monomer such as vinyl acetate. Alternatively, a copolymer containing the above-mentioned monomer as a main component, a polyvinyl chloride resin, or the like may be used, and these may be used alone or in combination of two or more. Among them, polymers of acrylate monomers are preferable, and the above-mentioned methabrene A-3000 is a mixture of polytetrafluoroethylene and a polymer having a polar group, and is particularly preferable.

The content of the polar group-containing polymer is preferably from 0.01 to 10 parts by weight based on 100 parts by weight of the composition of the present invention comprising a polyolefin resin and a cellulose filler. More preferably, it is 0.1 to 5 parts by weight. When the content of the polar group-containing polymer of the present invention is less than 0.01 part by weight, the effect of improving the surface appearance of the resulting shaped article is small, and when the content exceeds 10 parts by weight, The moldability of the obtained resin composition tends to decrease or the cost tends to increase.

In the resin composition of the present invention, if necessary, in addition to the above-mentioned components, other additives such as a heat stabilizer, a neutralizing agent for acidic substances contained in the cellulose-based filler, an antistatic agent, An ultraviolet absorber, a lubricant, a crystal nucleating agent, an inorganic filler, a foaming agent, a pigment and the like may be blended.

The resin composition of the present invention obtained from the above is
It can be suitably used as various molded body materials by various known molding methods, for example, injection molding, extrusion molding, press molding, etc., and above all, it can be used as a material suitable for profile extrusion molding.

The form of supply of raw materials when the resin composition of the present invention is subjected to profile extrusion molding is not particularly limited, as long as each component is contained in a required ratio. For example, a method of mixing powdery polyolefin-based resin, cellulose-based filler, polytetrafluoroethylene, and raw material components of a polar group-containing polymer as needed, and supplying the raw material to a molding machine in powder form,
A method in which all necessary components are mixed in advance by a mixer that generates high shearing force such as a super mixer or a gelation mixer, then granulated into pellets by an extruder or the like, and then supplied to a molding machine. Examples of the method include a method in which a system filler and polytetrafluoroethylene are each used as a master batch of a polyolefin-based resin, dry-blended with polyolefin-based resin pellets, and supplied to a molding machine.

In a preferred embodiment, polytetrafluoroethylene and a polymer containing a polar group and / or a polyolefin are previously mixed by applying a strong shearing force, and then mixed with other components. It is recommended because it is easy to convert.

As for the method for producing the profile-extruded article of the present invention, known methods can be employed without any limitation.
It is generally performed by a manufacturing apparatus including an extruder equipped with a deformed die, a sizing mold, a cooling device, a take-off device, and a cutting machine.

In the present invention, if a suitable method for producing a profile-extruded product is shown, for example, it is preferable to mold the resin composition at a temperature of 180 to 220 ° C. at the time of molding. The temperature is
If the temperature is lower than 180 ° C., the surface appearance of the obtained molded article tends to be poor, and if it is higher than 220 ° C., burning of the cellulosic filler occurs and the obtained molded article tends to be colored. Become. Further, a method of spraying air or mist-like water onto the resin composition in a molten state between the deformed die and the sizing mold to solidify the surface layer of the resin composition and improve shape retention can also be preferably employed.

Further, for the purpose of improving the dimensional stability of the resulting extruded molded product, a method of performing a heat treatment can be suitably employed. Although the heat treatment temperature is not particularly limited, it is generally 50 to 200 ° C., and the heat treatment may be performed in-line or in a batch system. The heat treatment time is not particularly limited, and may be set as needed.

As described above, the application field of the obtained profile-extruded product of the present invention is not particularly limited, and it can be used in many fields where a resin composition has been conventionally used.
Further, in the present invention, the extruded molded product obtained by molding a resin composition using rice husk powder, wood flour in a cellulose-based filler, has an excellent surface appearance and a high woody feel, and is a building component for housing, for example, It can be particularly suitably used as various materials such as baseboards, handrails, and peripheral edges.

[0041]

As will be understood from the above description, the resin composition of the present invention can be used not only as a material for various moldings, but also particularly as a material for profile extrusion molding. Further, the molded product obtained by the profile extrusion molding has an excellent surface appearance, and provides an effective molded product in various fields including the building material field.

Further, high filling of the cellulosic filler in the resin composition is possible, and in the case of incineration disposal, the caloric combustion is low, and the generation of harmful gases such as chlorine gas is small.
At the time of disposal, it has excellent environmental characteristics, such as collapse in the soil.

[0043]

EXAMPLES The present invention will be described below with reference to examples and comparative examples, but the present invention is not limited to these examples.

The evaluation method used in the examples will be described below. (1) Deformed extrusion moldability A deformed die (colored portion is a resin discharge portion) having a cross-sectional shape shown in FIG. 1 was attached to a 50 mmφ single screw extruder (L / D = 30) manufactured by GM Engineering Co., Ltd. The profile extrusion was performed at a cylinder temperature of 200 ° C. and a die temperature of 200 ° C., and subsequently, 1.0 and 2.5 m in a vacuum sizing mold (degree of vacuum: 40 mg / Hg) set to 25 ° C.
The solidified product was cooled and solidified while being picked up at a rate of / min to produce a shaped article. With respect to the above profile extrusion molding, the moldability was evaluated according to the following criteria.

：: Extrusion molding is easy.

Δ: Partial cuts occur at the edge of the molded product, resulting in poor molding stability.

×: Unable to mold (the molten resin composition is torn between the die and the sizing). (2) Surface appearance of molded article The surface state of the molded article obtained by the above-mentioned profile extrusion molding was visually observed, and the surface state was evaluated based on the following criteria.

：: Molded product surface is smooth.

Δ: Roughness and cracks are observed at the edge of the molded product.

×: The whole surface of the molded article is rough and cracks are observed.

-: Unable to evaluate because no molded product was obtained.

Example 1 Homopolypropylene having an MFR of 1.0 g / 10 min as a polyolefin resin and rice hull powder (Golden Powder 120, trade name, manufactured by Central Japan) as a cellulose-based filler
M), as a polytetrafluoroethylene component, Metablen A-3000 manufactured by Mitsubishi Rayon Co. (based on in-house analysis results, a mixture of 26% by weight of polytetrafluoroethylene and 74% by weight of a polar group-containing polymer: Soxhlet extraction, solvent p-xylene , Extraction time of 10 hours) in a weight ratio described in Table 1 with a Henschel mixer with stirring and mixing.
Using an mφ single-screw extruder, the mixture was melt-kneaded at a cylinder temperature of 200 ° C. to prepare pellets of the resin composition. The obtained pellets were subjected to profile extrusion molding using a 50 mmφ extruder equipped with a profile die at a cylinder temperature of 200 ° C. and a die temperature of 200 ° C., and subsequently, a vacuum sizing mold (temperature of 40 mg / Hg) 1.0
Cooling and solidification were carried out while taking off at a speed of m / min and 2.5 m / min, to obtain a shaped article. Table 1 shows the evaluation results of the obtained heteroformed products. Further, a thin section obtained by cutting out the obtained abnormally shaped article was stained with ruthenium tetroxide and observed with a transmission electron microscope. Polytetrafluoroethylene was confirmed as a fibrous undyed material. Table 1 also shows the diameter of polytetrafluoroethylene in an arbitrary field of view.

Examples 2 and 3 Rice husk flour (Salon Filler Co., trade name, Salon Fiber A type) (Cellulose 100M, product of Casino Co., Ltd.) as cellulosic fillers
A resin composition and a profile-extruded product were obtained in the same manner as in Example 1 except that (Example 3) was used. The results are shown in Table 1.

Examples 4 to 6 A resin composition and a profile-extruded product were obtained in the same manner as in Example 1 except that the mixing ratio of the polyolefin resin and the cellulosic filler was changed as shown in Table 1. Was. The results are shown in Table 1.

Example 7 Ethylene-propylene random copolymer having an MFR of 0.5 g / 10 min (Tokuyama Polypro RB410), rice husk powder (manufactured by Central Japan, trade name: Golden Powder 120)
M), polytetrafluoroethylene (manufactured by Asahi ICI, trade name Fluonlubricant L-171J) was melt-mixed in a gelation mixer at a weight ratio shown in Table 1 until the temperature reached 170 ° C. due to shearing heat. 50
Using a mmφ single screw extruder, the mixture was melt-kneaded at a cylinder temperature of 200 ° C. to prepare resin composition pellets. The obtained pellets were subjected to profile extrusion in the same manner as in Example 1. Table 1 shows the evaluation results of the obtained heteroformed products.

Example 8 The same operation as in Example 7 was carried out except that maleated polypropylene (Tokuyama Polypro AD89G) was used in the amount shown in Table 1 as the polar group-containing polymer. The results are shown in Table 1.

Comparative Example 1 A resin composition and a profile-extruded product were obtained in the same manner as in Example 1, except that methabrene A-3000 was not used. The results are shown in Table 1.

Comparative Examples 2 and 3 The same procedures as in Example 1 were carried out except that methabrene A-3000 was not used and the mixing ratio of the polyolefin resin and the rice husk powder was changed as shown in Table 1. The same operation was performed. The results are shown in Table 1.

Comparative Examples 4 to 6 The same operation as in Example 8 was carried out except that polytetrafluoroethylene or a polymer containing a polar group (AD89G) was used in the amount shown in Table 1, or was not used. . The results are shown in Table 1.

[0060]

[Table 1]

[Brief description of the drawings]

FIG. 1 is a drawing showing a cross-sectional shape of a deformed die used in an embodiment of the present invention.

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Claims (5)

[Claims] 1. A polyolefin-based resin in an amount of 30 to 80% by weight,
Composition 1 comprising 20 to 70% by weight of cellulosic filler
With respect to 100 parts by weight of polytetrafluoroethylene, 0.1 part by weight.
A resin composition containing from 0.01 to 10 parts by weight. 2. The resin composition according to claim 1, wherein the polytetrafluoroethylene is dispersed as a fibrous material having an average diameter of 5 μm or less in a matrix composed of a polyolefin resin and a cellulose filler. 3. A polyolefin resin in an amount of 30 to 80% by weight,
Composition 1 comprising 20 to 70% by weight of cellulosic filler
With respect to 100 parts by weight of polytetrafluoroethylene, 0.1 part by weight.
01 to 10 parts by weight and a polar group-containing polymer 0.01 to 10
A resin composition containing parts by weight. 4. The resin composition according to claim 1, wherein the cellulosic filler is rice husk powder or wood powder. 5. A profile-extruded product comprising the resin composition according to claim 1, 2, 3, or 4.