WO1996010611A1

WO1996010611A1 - Surface-treated filler and composition containing said filler

Info

Publication number: WO1996010611A1
Application number: PCT/JP1995/001973
Authority: WO
Inventors: Yuji Koushima; Hajime Tanisho; Teiji Kohara
Original assignee: Nippon Zeon Co., Ltd.
Priority date: 1994-09-30
Filing date: 1995-09-28
Publication date: 1996-04-11

Abstract

A composition comprising a thermoplastic norbornene resin and, dispersed therein, particles of an inorganic filler coated with a silane compound comprising a silicon atom and, bonded thereto, four groups consisting of one or more alkyl groups and one or more hydrolyzable groups, such as trimethoxy-p-propylphenylsilane. The composition is excellent in tensile properties and impact resistance, has such a low coefficient of linear expansion as to be excellent in dimensional accuracy resistant to temperatue changes, and is excellent in moldability to give moldings having excellent surface accuracy.

Description

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TECHNICAL FIELD Surface treatment filler and composition containing the filler

The present invention relates to an inorganic filler coated on the surface, and a thermoplastic norbornene-based resin composition containing the filler.More specifically, the surface is coated with a silane compound to improve wettability with the thermoplastic norbornene-based resin. The present invention relates to an improved inorganic filler, and a thermoplastic norbornene-based resin composition having improved mechanical strength by containing the filler.

Background art

For polyolefin-based resins such as polyethylene and polypropylene, it is widely used to improve the mechanical strength of resins by dispersing inorganic fillers in applications where mechanical strength is required. However, the general inorganic filler and the polyolefin resin have poor wettability, so that cracks are easily generated from the interface between the filler and the resin, and the resin becomes brittle. Therefore, usually, an inorganic filler in which the surface of the filler is coated with a silane compound having a vinyl group-containing hydrocarbon group is dispersed in a resin to improve the mechanical strength.

Recently, a thermoplastic norbornene resin, one of the polyolefin resins, has become more resistant to heat, transparency, low moisture absorption, low water absorption, chemical resistance, moisture resistance, water resistance, transparency, and low birefringence. It is widely used as resin for optical materials, medical materials, electrical insulation materials, and automotive parts materials. However, depending on the application, mechanical strength such as elastic modulus and dimensional stability were insufficient. Therefore, even in the case of thermoplastic norbornene-based resins, the modification of dispersing inorganic fillers in the resin has been carried out in order to improve the odor resistance, dimensional stability, flame retardancy, thermal conductivity, and abrasion resistance. There is a problem that it becomes brittle like the polyolefin-based resin.

Therefore, the present inventors have studied the use of an inorganic filler coated with vinylsilane as in the case of other polyolefin-based resins in order to increase the modifying effect.c However, the adhesion between the resin and the inorganic filler was considered. Not enough, dispersed inorganic filler Even thermoplastic norbornene resins are brittle, have low tensile elongation, and have a problem that the surface accuracy of the molded product is insufficient because the filler tends to agglomerate.

Disclosure of the invention

The present inventors have conducted intensive studies with the aim of improving the mechanical strength of thermoplastic norbornene-based resin, and as a result, the inorganic filler coated on the surface with a specific silane compound has improved wettability and adhesion with thermoplastic norbornene-based resin. The thermoplastic norbornene resin in which the filler is dispersed has a small decrease in tensile elongation, improves impact resistance, disperses the filler without agglomeration, and has excellent surface precision of the molded product. And completed the present invention.

BEST MODE FOR CARRYING OUT THE INVENTION

Thus, according to the present invention, general formula 1

R I O 丄 X l X 2 3 \

General formula 2

R ₂ R ₃ S i Χ Χ ₅ and

General formula 3

4 5 6 1 6

(Formula 1-3 in R, to R ₆ represents an alkyl group, X, to X ₆ represents a hydrolyzable group) were coated surface with a layer of at least one silane compound represented by inorganic And a composition comprising the inorganic filler and a thermoplastic norbornene-based resin.

(Inorganic filler)

The inorganic filler used in the present invention is not particularly limited. Commonly used, e.g., silica, glass, clay, carion, wollastonite, tanolek, myriki, alumina, aluminum hydroxide, iron, iron oxide, titanium oxide, zinc oxide, magnesium hydroxide, calcium carbonate Inorganic fillers are exemplified. Among them, silica, glass, quartz, alumina and the like are preferable in terms of hardness and the like.

The shape and size of the inorganic filler are not particularly limited, and may be in the form of particles or fibers, depending on the purpose.Particles are preferred from the viewpoint of moldability and surface accuracy of the molded article, and the corners are preferably selected. Particles having no particles are more preferable, and true spherical particles are particularly preferable. The further away from the true sphere, the higher the melt viscosity, the worse the moldability, and the lower the surface accuracy of the molded product. The true spherical particles preferably have an average particle diameter of at least 0.01 m, more preferably at least 0.05 μm, particularly preferably at least 0.1 m. Further, those having an average particle size of 50 / zm or less are preferable, those having an average particle size of 10 m or less are more preferable, and those having a mean particle size of 5 / m or less are particularly preferable. If the particle size of the filler is too small, the melt flowability of the composition will be poor, the fillers will easily aggregate, and the surface accuracy of the molded article will be reduced. If the particle size of the filler is too large, the dimensional accuracy with respect to the temperature change of the molded product is deteriorated, and the surface accuracy of the molded product is deteriorated. Further, it is preferable that the particle size distribution is small from the viewpoint of uniform surface accuracy and physical properties, and particles in the range of 1 to 10 times the average particle size should be 70% by weight or more of all particles. Is preferably 80% by weight or more, more preferably 90% by weight or more.

(Silane compound)

The silane compound used in the present invention has the general formula 1

1 \. I S 1 Λ I A.2 A 3,

General formula 2

R ₂ R ₃ S i X, X ₅ and

General formula 3

R 4 R 5 R 6 S 1 X 6

(To R ₆ of general formula 1-3 represents an alkyl group, X, to X ₆ represents a hydrolyzable group) are those selected from. The silane compound of the general formula 1 is preferred from the viewpoint of excellent wettability and adhesion between the inorganic filler surface and the silane compound. Further, as these silane compounds, R, to R ₆ are represented by the general formula 4 because of their good wettability and adhesion to the thermoplastic norbornene resin. C a H 2 a ^

-General formula 5

Good. ,-C _b H _{2 b-} ,

General formula 6

C c H _{2 c} .,-(〇〉-,

—General formula 7

C d H 2 d + I ~ ku U〉 — C e H 2 e

General formula 8

H)-C, H

General formula 9

C _K H _{2 g + I-} (i)-and

General formula 1 0

(In general formulas 4 to 10, a, b, d, e, f, h, and i represent natural numbers, and are preferably selected from groups represented by (:, g represents 0 or a natural number.) More preferably, a to i are 3 to 5. Further, from the viewpoint of quickly adhering to the surface of the inorganic filler, X to X _{6 are} strong, and an alkoxy group such as a methoxy group or an ethoxyquin group: an acetoxy group; Halogens such as chlorine, bromine and iodine are preferred; alkoxy groups are more preferred; methoxy groups are particularly preferred.

Specific examples of the silane compound used in the present invention include trimethoxy η-hexyl silane, trimethoxy η-propyl silane, trimethoxy ρ-propylphenyl silane, trimethoxy phenyl propyl silane, and trimethoxy silane. Examples thereof include monophenylsilane, trimethoxy-1-ρ-provylcyclohexylsilane, trimethoxy-cyclohexylpropylsilane, and trimethoxycyclohexylsilane.

(Silane compound coated inorganic filler) The silane compound-coated inorganic filler of the present invention is obtained by coating the above-mentioned inorganic filler with the above-mentioned silane compound. From the viewpoint of good wettability with the thermoplastic norbornene-based resin, it is preferable that the entire surface of the inorganic filler is coated with the silane compound. The coating method is not particularly limited, and may be a commonly used method such as an aqueous solution method, an organic solvent method, a spray method, or the like. It is preferable that the filler be immersed and taken out and dried to remove the solvent. The thickness of the coating is not particularly limited.

(Thermoplastic norbornene resin)

The thermoplastic norbornene-based resin used in the present invention is disclosed in JP-A-51-800, JP-A-S60-260, and JP-A-11-16887. JP, JP-A-1-190772, JP-A-3-148882, JP-A-3-122, 739, JP-A-316380 And the like. Specific examples thereof include a ring-opening polymer of a norbornene-based monomer, a hydrogenated product thereof, an addition polymer of a norbornene-based monomer, and a norbornene-based monomer. And addition-type copolymers of olefins.

Norbornene-based monomers are also known monomers described in the above publications {Japanese Patent Application Laid-Open Nos. 2-222744 and 2-2-276842, for example, norbornene, Alkyl, alkylidene, aromatic substituted derivatives thereof and substituted or unsubstituted polar olefins such as halogens, hydroxyl groups, ester groups, alkoxy groups, cyano groups, amide groups, imide groups, and silyl groups; For example, 2-norbornene, 5-methyl-2-norbornene, 5,5-dimethyl-12-norbornene, 5_ethyl- 2-norbornene, 5-butyl-12-norbornene, 5-ethylidene-12-norbornene, 5- Methoxycarbonyl 2-norbornene, 5-cyano 2-norbornene, 5-methyl-5-methoxy-2-norbornene, 5-phenyl-2-norbornene, 5-phenyl-1-5-methyl-2-norbornene, 5-hexyl-12-norboernene, 5-octyl-12-norbornene, 5-octadecyl-12-norbornene, etc .; more than 1 ^^ cyclopentagen in norbornene Is a monomer to which is added, or a derivative or a substitute thereof similar to the above, for example, dimethano-1,2,3,4,4a, 5,8,8a-2,3- Cyclopentadi Enoctahi dronaphlene, 6-methyl-1,4,5,8-dimethanone 1,4,4a, 5,6,7,8,8a-octahidronaphthalene, 1,4: 5,10: 6 1,9,1 Trimethanoe 1,2,3,4,4a, 5,5a, 6,9,9a, 10,10a—dodekahi draw 2,3-cyclopentadienoanthracene, etc .; Monomers having a polycyclic structure multiplied by the Diels-Alder reaction, derivatives and substituents similar to the above, for example, dicyclopentadiene, 2,3-dihydrofuran dicyclopentadiene, etc .; Adducts with trahydrodroindene and the like, and derivatives and substitutes thereof as described above, for example, 1,4-methanol 1,4,4a, 4b, 5,8,8a, 9a-octahydrofluorene; 5,8-methano 1,2,3,4,4a, 5,8,8a-octahydro-1,2,3-cyclopentadienonaphthalene, etc. Etc. The.

The norbornene-based monomer may be polymerized by a known method, and if necessary, may be copolymerized with another copolymerizable monomer or may be hydrogenated to form a thermoplastic saturated norbornene-based resin. It can be a hydrogenated norbornene polymer. Further, the polymer or the polymer hydrogenated product can be obtained by a method known in, for example, JP-A-3-92553, such as —unsaturated carboxylic acid and / or its derivative, styrene-based hydrocarbon, and olefin-unsaturated. It may be modified with an organic gay compound having a bondable and hydrolyzable group or an unsaturated epoxy monomer. In order to obtain a material having excellent moisture resistance and chemical resistance, a thermoplastic norbornene resin containing no polar group is preferable.

In the present invention, the number-average molecular weight of the thermoplastic norbornene-based resin is 100,000 or more, preferably 15 to 15, in terms of polystyrene measured by GPC (gel 'permeation' chromatography) using a toluene solvent. , 0000 or more, more preferably 20 000 or more, 200 000 or less, preferably 100 000 or less, more preferably 50 000 or less. is there. When the thermoplastic norbornene-based resin has an unsaturated bond in the main chain structure, it can be converted into a thermoplastic saturated norbornene-based resin by hydrogenation. In the case of hydrogenation, the hydrogenation rate is 90% or more, preferably 95% or more, more preferably 99% or more from the viewpoint of heat deterioration resistance and light deterioration resistance. 11 ₇ P / JP95 / 01973

When used for medical applications, it is preferable to prevent the transition metal derived from the polymerization catalyst from remaining in the resin to elute. Pore volume 0. 5 cm ³ or less on, preferably 0. 7 cm ³ / g or more, preferably adsorbent on the specific surface area 2 5 0 cm ² or more, for example adsorbents such as alumina, hydrogenation such as nickel The polymer is hydrogenated using a heterogeneous catalyst carrying a catalytic metal, the resin solution is treated with such an adsorbent to adsorb metal atoms, and the resin solution is treated with acidic water and pure water. It is possible to reduce the amount of transition metal atoms derived from the polymerization catalyst in the resin to 1 ppm or less by repeatedly washing the resin, etc., and such a resin is safe for medical use. Further, the thermoplastic norbornene-based resin used in the present invention preferably has a higher glass transition temperature, and when used in medical applications, it is preferably at least 105 ° C, more preferably at least 120 ° C, Particularly preferably, the temperature is 130 ° C. or higher. Some sterilization methods do not require heating such as y-ray irradiation, but the simplest sterilization methods include methods that require heating, especially boiling methods and steam sterilization. For sterilization by boiling, there is no problem if the glass transition temperature is 105 ° C or more, but for steam sterilization, the required heat resistance depends on the temperature setting during sterilization. The most common method of steam sterilization is to use autoclave at 121 ° C. In this case, those having a glass transition temperature of 130 ° C. or more are preferable. In general, the more monomers having a large number of rings, the higher the glass transition temperature of the resin.For example, a hydrogenated product of a ring-opened polymer consisting of only four or more monomers usually has a temperature of 130 ° C or more. Glass transition temperature. In addition, in the case of the addition type polymer, even the addition type polymer of norbornene has a glass transition temperature of 300 or more. However, if the glass transition temperature is too high, there are adverse effects such as difficulty in injection molding.Therefore, select a monomer, comonomer, polymerization method, etc. to obtain a thermoplastic norbornene resin having a glass transition temperature according to the purpose. It may be manufactured.

Further, various additives may be added to the thermoplastic norbornene-based resin as long as the object of the present invention is not impaired. For example, in the case of a thermoplastic norbornene resin, an anti-aging agent such as a phenol X-based resin; a thermal degradation inhibitor such as a phenol X-based resin; an ultraviolet stabilizer such as a benzofudinone-based resin; Lubricants such as esters of aliphatic alcohols, partial esters of polyhydric alcohols and partial ethers; and other resins, rubbers, and the like. Can You. It may be added before the resin composition of the present invention is prepared, added at the time of preparation, or added after the preparation.

(Resin composition)

The thermoplastic norbornene-based resin composition of the present invention is obtained by dispersing a silane compound-coated inorganic filler in a thermoplastic norbornene-based resin.

The amount ratio of both is 0.1 part by weight or more, preferably 0.5 part by weight or more, more preferably 1 part by weight, based on 100 parts by weight of the thermoplastic norbornene resin. Parts by weight, particularly preferably at least 10 parts by weight, at most 250 parts by weight, preferably at most 150 parts by weight, more preferably at most 100 parts by weight. The thermoplastic norbornene-based resin composition is too brittle when the amount of the silane compound-coated inorganic filler is too small, so that the mechanical strength, for example, the elastic modulus, is not improved. In addition, the surface accuracy of the molded product deteriorates.

The method for mixing the two is not particularly limited, and a usual method such as a method using a twin-screw kneader may be used. Alternatively, a composition having a high concentration of the silane compound-coated inorganic filler may be prepared in advance, and a thermoplastic norbornene-based resin and the composition may be mixed to prepare a composition having a predetermined concentration.

(Molding method)

The method for molding the resin composition of the present invention is not particularly limited, and molding methods used for ordinary thermoplastic resins, for example, injection molding, extrusion molding, pressure molding, vacuum molding, hot press molding, and the like are used.

(Molding)

The molded article made of the resin composition of the present invention has a large tensile strength, a large tensile elongation, a high tensile elasticity, a high impact resistance, excellent dimensional stability, and a small decrease in the tensile elongation. Excellent surface accuracy. The resin composition of the present invention, tensile strength is preferably 5 ² 0 kg / cm 2 or more, more preferably 5 3 0 kg / cm ² or more, a tensile elongation of preferably 5%, more preferably at least 6% , tensile elastic modulus preferably 2 0 0 0 0 kg / cm 2 or more, more preferably ² 5 0 0 O k gZcm 2 or more, notched IZ 0 D衝擊value of preferably 3 · 0 kg / cm ² or more, More preferably 3.5 kg / cm ² or more, and a coefficient of linear expansion is preferred. Properly it is ^{6. 0 X 1 0 "5} deg ' or less, more preferably ^{5. O xi 0" 5 deg} ' is below. In addition, the protrusions formed by the filler on the surface are preferably 10 Zcm ² or less, more preferably 5 Zcm ² or less.

(Application)

The application of the resin composition of the present invention is not limited, and can be generally used for thermoplastic norbornene-based resins other than those requiring transparency.Specific examples include precision molded products (information disk substrates, mirror substrates, , Coating materials (for electric wires, cables, etc.), consumer / industrial electronic equipment enclosures (copiers, computers, printers, televisions, VCRs, video cameras, etc.), structural members (parabolic antenna structural members) , Flat antenna structural members, radar dome structural members, etc .; electrical insulating materials; general circuit boards (hard printed boards, flexible printed boards, multilayer printed wiring boards, etc.), high-frequency circuit boards (circuit boards for satellite communication equipment, etc.) ) Etc. Circuit board; transparent conductive film (liquid crystal board, optical memory, surface heating element, etc.) Base materials; semiconductor encapsulation materials (transistor encapsulation materials, IC encapsulation materials, LSI encapsulation materials, etc.), electric and electronic parts encapsulation materials (motor encapsulation materials, capacitor encapsulation materials, switch encapsulation materials) , Sealing materials for sensors, etc.); interior materials for automobiles such as rearview mirrors and meter covers; exterior materials for automobiles such as door mirrors, fender mirrors, beam lenses, light covers, etc .;

Example

Hereinafter, the present invention will be described specifically with reference to Examples and Comparative Examples. The measurement of tensile strength, tensile elongation, tensile elastic modulus, etc. was performed at a tensile speed of 5 mmZmiη according to JIS K7113. Measurement of I Z O D impact value

The measurement was performed according to JIS K 7110.

(Manufacture of inorganic filler)

Example 1

Spherical silica beads (Admatech, Admafine S0-C2, average particle size 0 m, particle size 0 m) were added to a mixture of 5 g of trimethoxine chlorohexylsilane and 995 g of water with sufficient stirring. (0.2 to 2 m particles are 95% by weight or more), and stirred for 1 hour. Afterwards, the particles are filtered off and placed in a 130 ° C environment. After leaving it for a while to dry the water, an inorganic filler of the present invention coated with about 0.3 g of the silane compound per 1 cn of the surface area was obtained.

Example 2

But using trimethyl butoxy hexyl silane to single cycloalkyl instead of Kishirushiran to trimethyl Tokishi n- in the same manner as in Example 1, inorganic invention coated with a silane compound of about 0. 4 U g per surface area 1 cm ² A filler was obtained.

Comparative Example 1

An inorganic filler coated with about 0.4 tz g of a silane compound per 1 cm ^{2 of} surface area was obtained in the same manner as in Example 1 except that trimethoxyvinylsilane was used instead of trimethoxycyclohexane silane. This is not the silane compound-coated inorganic filler of the present invention.

(Production of resin composition)

Example 3

Thermoplastic norbornene resin (ZEONEX 280, manufactured by Nippon Zeon Co., Ltd., hydrogenated norbornene monomer ring-opening polymer, molecular weight about 28,000, glass transition temperature 140 ° C, hydrogenation rate 9 9.7% or more) To 90 parts by weight, 10 parts by weight of the silane compound-coated inorganic filler of the present invention obtained in Example 1 was added, and at a resin temperature of 250, a twin screw extruder (manufactured by Toshiba Machine Co., Ltd.) And TEM35 B) to obtain a resin composition of the present invention. The resin composition was pelletized by a pelletizer.

A dumbbell was prepared by injection molding using this pellet and its tensile properties were measured. The tensile strength was 560 kg / cm ² , the tensile elongation was 7%, and the yield point was recognized. The tensile modulus was 2800 kg / cm ² . Further, the linear expansion coefficient of ^{4. 0 X 1 0- 5 deg '} , I ZOD impact value Notched 3. 9 kg - was CmZcm. When the molded product was broken and the cross section was observed with a scanning electron microscope, no formation of a gap between the filler and the resin was observed. Furthermore, the surface of the molded product was smooth, and when observed with an atomic force microscope, no protrusion with a height of 0.5 m or more was observed.

Example 4

The silane obtained in Example 2 was used in place of the silane compound-coated inorganic filler obtained in Example 1. A resin composition of the present invention was obtained and pelletized in the same manner as in Example 3 except that an inorganic compound-coated inorganic filler was used, and a dumbbell was produced. When the tensile properties were measured, the tensile strength was 540 kg / cm ² , the tensile elongation was 9%, the tensile elastic modulus was 270 kg / cm ² , and the yield point was recognized. No gap was formed between the filler and the resin. The linear expansion coefficient was 3.9 X 10 " ⁵ deg" ^{1. The} notched I ZOD impact value was 3.7 kg-cmZcm. Furthermore, the surface of the molded product was smooth, and no protrusions with a height of 0.5 mm or more were observed.

Comparative Example 2

A resin composition was obtained in the same manner as in Example 3 except that the silane compound-coated inorganic filler obtained in Comparative Example 1 was used instead of the silane compound-coated inorganic filler obtained in Example 1, and a dumbbell was prepared. . When the tensile properties were measured, the tensile strength 5 ² 0 k gZcm 2, a tensile elongation of 3%, the tensile modulus was 2 9 0 0 0 kg / cm 2. No yield point was observed. Further, the linear expansion coefficient of ^{4. 2 X 1 0- 5 deg '} , I ZOD impact value Notched 2. 5 k - was cm / cm. Gaps were observed between some silane compound-coated inorganic fillers and thermoplastic norbornene resin. In addition, about 7 protrusions with a height of 0.5 m or more are formed on the molded product surface.

C ΠΊ ² recognized

Comparative Example 3

A resin composition was obtained and pelletized in the same manner as in Example 3 except that an uncoated inorganic filler (Admafine S0-C2) was used instead of the silane compound-coated inorganic filler obtained in Example 1. A dumbbell was made. When the tensile properties were measured, the tensile strength was 500 kg / cm ² , the tensile elongation was 2%, and the tensile modulus was 2800 kgZ cm ² . No yield point was observed. The coefficient of linear expansion was 3.9 X 1 (T ⁵ deg, notched I ZOD impact value was 1.6 kg · cmZ cm. The formation of a large number of gaps was observed more than in the sample No. 5. Further, about 15 protrusions having a height of 0. 0 or more were observed on the surface of the molded article at about Zcm ² .

Comparative Example 4

Injection molding using thermoplastic norbornene resin (ZEONEX 280) More dumbbells were made. The tensile strength was 720 kgZcm ² , the tensile elongation was 11%, and the tensile modulus was 17000 kg / cm. No yield point was found. Further, the linear expansion coefficient of ^{7. 0 X 1 0_ 5 deg '} , I ZOD impact pricing Notsuchi is 3. Atsuta at 0 kg · cm / cm. Furthermore, there was no force on the surface of the molded product.

The thermoplastic norbornene-based resin composition containing the silane compound-coated inorganic filler of the present invention is excellent in tensile properties and impact resistance, and has a small coefficient of linear expansion, so that it has excellent dimensional accuracy with respect to temperature change, moldability, and molding. Excellent surface accuracy of products.

Claims

The scope of the claims

1. General formula 1

R I 1 I λ 2 X 3

General formula 2

R ₂ R ₃ S i X, Χ ₅ and

General formula 3

(R in the general formula 1 to 3, to R ₆ represents an alkyl group, X, to X ₆ represents a hydrolyzable group) were coated surface with a layer of at least one silane compound represented by inorganic Huila one.

2. The inorganic filler according to claim 1, wherein the silane compound is represented by the general formula 1.

3. R, up to R ₆ is the general formula 4

General formula 5

, 〇〉 — C _b H _2b ―,

General formula 6

Cc H _{2c +} .- ^ O)-,

General formula 7

General formula 8

<H> -C, H _{2 (} —,

General formula 9

C, Η _{2Ί + ι-} (H> — and

General formula 10

C _h H _2l , -.- (i) -C, H ₂ , (Where a, b, d, e, f, h, and i in the general formulas 4 to 10 represent natural numbers, and c and g each represent 0 or a natural number). The inorganic filler described in 1.

4. The inorganic filler according to claim 3, wherein a to i are 3 to 5.

5. X> to X ₆ Chikaraku, alkoxy group, Asetokishi group, inorganic FILLER one of claims 3-4, wherein a member selected from halogen.

6. The inorganic filler according to claim 1, which is silica, glass, quartz, or alumina.

7. The inorganic filler according to claim 1, which is in the form of particles having an average particle diameter of 0.01 to 50 / m or less.

8. The inorganic filler according to claim 1, wherein particles in a range of 1/10 to 10 times the average particle diameter are 70% by weight or more.

9. A composition comprising the inorganic filler according to claim 1 and a thermoplastic norbornene-based resin.

10. The composition according to claim 9, wherein the amount of the silane compound-coated inorganic filler is 0.1 to 250 parts by weight based on 100 parts by weight of the thermoplastic norbornene resin.

11. Tensile strength 5 ² 0 kg / cm 2 or more at which claims 9-1 0 composition.

12. The composition according to claims 9 to 11, which has a tensile elongation of 5% or more.

13. Tensile claim 9-1 2 composition according modulus is 2 0 0 0 0 kg / cm 2 or more.

14. The composition according to any one of claims 9 to 13, wherein the notched I ZOD impact value is 3. O kg / cm ² or more.

15. linear expansion coefficient of 6 is 0 X 1 0 ⁵ deg 'subclaims 9-1 4 set composition as described.

16. protrudes formed by FILLER one expressed on the surface of 1 0 / cm ² or less der Ru claim 9-1 5 composition.

17. The number average molecular weight of the thermoplastic norbornene-based resin is calculated by gel permeation using a toluene solvent. The composition according to claim 9, wherein the composition has a molecular weight of 0.0000 to 200,000.

18. The composition according to claim 9, wherein the thermoplastic norbornene resin has a metal content of 1 ppm or less.

19. The composition according to any one of claims 6 to 18, wherein the thermoplastic norbornene resin has a glass transition temperature of 105 ° C or more.