TW201533167A - Curable organopolysiloxane composition, member for transducers - Google Patents

Abstract

To provide a curable organopolysiloxane composition having excellent mechanical characteristics and/or electrical characteristics, and particularly one capable of producing a silicone elastomer cured product capable of being used as a member for transducers. A curable organopolysiloxane composition comprising an organopolysiloxane and at least one type of inorganic microparticles having an average primary particle diameter of not less than 50 nm, wherein the mass fraction of monovalent aromatic hydrocarbon groups having from 6 to 10 carbons (Z) in the total of organopolysiloxanes is not less than 0.2% by mass and not greater than 50% by mass, and the mass fraction of straight-chain organopolysiloxanes having a certain chain length range and a group capable of a curing reaction (W) in the total of organopolysiloxanes is not less than 50% by mass.

Description

Curable organopolyoxane composition, component of converter

The present invention relates to organopolyoxane compositions which can be advantageously used in electrical and/or electronic applications, in particular in which the converter is curable. In particular, the present invention provides a curable organopolyoxane composition which can be advantageously used as an electroactive polyoxyxene elastomer material by curing the formed organopolyoxane cured product, which material can be used as The dielectric layer or electrode layer of the converter. The invention relates in particular to a curable organopolyoxane composition having an organopolyoxyalkylene cured product having electrical properties suitable for use as a dielectric material and more particularly as a dielectric layer for a converter. And mechanical properties. The invention further relates to a method of producing an electroactive polymer material formed using a curable organopolyoxane composition and a member of a converter comprising the electroactive polymer material. The present application claims priority to Japanese Patent Application No. 2013-272971, filed on Dec. 27, 2013, which is hereby incorporated by reference.

AGBenjanariu et al. indicate that dielectric polymers are potential materials for artificial muscles (AGBenjanariu et al., "New elastomeric silicone based networks applicable as electroactive systems," Proc. of SPIE SPIE No. 7976 Volume 79762V-1 to 79762V- 8 (2011)). Here, it shows the physical properties of a material having a unimodal or bimodal network formed using an addition curable polyoxyxene rubber. To form the polyoxyxene rubber, a short-chain organic hydroquinone having 4 hydrazine-bonded hydrogen atoms is used as a crosslinking agent. To crosslink a linear poly(dimethyloxane) (PDMS) polymer having a vinyl group. In addition, an actuator is mentioned in B. Kussmaul et al., Actuator 2012, 13th International Conference on New Actuators, Bremen, Germany, June 18-20, 2012, pages 374-378. The chemically modified organic polydimethyl methoxy hydride is sandwiched between the electrodes as a dielectric elastomer by using a crosslinking agent as a group of an electric dipole bonded to a polydimethyl siloxane. Actuator material.

However, the specific composition of the curable organopolyoxane composition is not disclosed in any of the above references, and additionally, in practice, the physical properties of the curable organopolyoxane composition are used in the industry. Insufficient materials for various types of converters in the application. Accordingly, there is a need in the art to achieve electroactive polymer materials that are capable of meeting the mechanical and electrical properties of the practical application of materials for various types of converters. In particular, there is a great need in the art for a curable organopolyoxane composition that cures and provides an electroactive polymer material having excellent physical properties.

On the other hand, it has been known to incorporate inorganic microparticles (e.g., thermally conductive fillers, fluorescent fillers, and reinforcing fillers) into curable organopolyoxane compositions for electrical and/or electronic applications. For example, Patent Documents 1 to 3 disclose an addition curable organopolyoxyalkylene having a phenyloxysiloxane and it is stated that inorganic fine particles can be added.

However, the addition-curable organopolysiloxanes lack a rubber-elastic sealant, and do not clarify a curable organopolyoxane composition for providing an elastomer having a tensile elongation at break of not less than 200%. Any content. Additionally, these documents do not address or suggest providing rubber elasticity or the addition of inorganic particulates, especially dielectric inorganic particulates, to a curable oxyalkylene having a predetermined high aromatic content.

Citation list Patent literature

Patent Document 1: Japanese Unexamined Patent Application Publication No. 2013-159670A.

Patent Document 2: Japanese Unexamined Patent Application Publication No. 2010-084118A.

Patent Document 3: Japanese Unexamined Patent Publication Application (Translation of PCT Publication) No. 2012-507582A

Non-patent literature

Non-Patent Document 1: "New elastomeric silicone based networks applicable as electroactive systems", Proc. of SPIE No. 7976 Volume 79762V-1 to 79762V-8 (2011)

Non-Patent Document 2: Actuator 2012, 13th International Conference on New Actuators, Bremen, Germany, June 18-20, 2012, pp. 374-378

The present invention solves the problems of conventional curable polyorganosiloxane compositions and aims to provide polyoxyxene elastomers having excellent mechanical and/or electrical properties and, in particular, capable of producing components that can be used as converters. A curable organopolyoxane composition of the cured product.

Another object of the present invention is to provide a curable organopolyoxane composition capable of providing high specific dielectric constant, high dielectric breakdown strength and low by providing excellent mechanical and/or electrical properties. Young's modulus to achieve high energy density; ability to achieve durability due to excellent mechanical strength (ie tensile strength, tear strength, elongation, and the like) when used as a dielectric layer for a converter And the actual amount of displacement; and it is possible to manufacture a cured product which can be used as a material for a converter. In addition, various types of fillers (including fillers that have been surface treated) can be blended with the curable organopolyoxane compositions of the present invention to achieve desired electrical properties, and the curable organic polyfluorenes of the present invention The oxyalkylene composition may include a release additive to prevent breakage upon molding into a sheet, and may also include an additive for improving dielectric breakdown characteristics.

Another object of the present invention is to provide a process for the production of a curable organopolyoxane composition, which provides a curable polyoxoelastic which can be used as an electroactive polymer material for a converter. The bulk material provides a method of producing the curable polyoxyxene elastomer material and provides various types of converters using the curable polyoxyxide elastomer material.

The object of the present invention is attained by a curable organopolyoxane composition comprising an organopolyoxane represented by the following formula (I): R ^a _a R ^b _b SiO _{(4-ab)/ 2} (I)

(wherein R ^a is a monovalent aromatic hydrocarbon group having 6 to 10 carbons, and R ^b is at least one type of monovalent functional group (however, R ^b is in addition to a monovalent aromatic hydrocarbon group having 6 to 10 carbons) a group), wherein at least a portion of R ^{b is a} group capable of undergoing a curing reaction, and 0 < a, 0 < b, 1.9 < a + b < 2.1, and one or more types of inorganic fine particles having a diameter of not less than An average primary particle diameter of 50 nm, wherein the mass fraction (Z) of the monovalent aromatic hydrocarbon group having 6 to 10 carbons in all the organopolysiloxanes is not less than 0.2% by mass and not more than 50% by mass, and all of the organic polymerization The mass fraction (W) of the linear organopolyoxane represented by the following formula (II) in the oxane is not less than 50% by mass: R ¹ R ² ₂ Si(OSiR ³ R ⁴ ) _n (OsiR ³ R ¹ ) _m OsiR ¹ R ² ₂ (II)

(wherein R ¹ is a group capable of undergoing a curing reaction, and R ² , R ³ and R ⁴ each independently, identically or differently represent a hydrogen atom, a monovalent aliphatic hydrocarbon group having 1 to 10 carbons, and have 6 to 10 The monovalent aromatic hydrocarbon group of carbon; the n and m systems respectively satisfy the values of the conditions 200 < n and 0 = < m = < (n / 20).

Here, the mass fraction (Z) of the monovalent aromatic hydrocarbon group is preferably not less than 0.5% by mass and not more than 30% by mass. In addition, the mass fraction (W) of the linear organopolyoxane is preferably Not less than 75.0% by mass and not more than 99.9% by mass. Further, the curable organopolyoxane composition preferably has such preferred embodiments of "Z" and "W" at the same time. Further, the monovalent aromatic hydrocarbon group having 6 to 10 carbons is preferably a phenyl group. Further, one or more types of inorganic fine particles having an average primary particle diameter of not less than 50 nm preferably comprise dielectric inorganic fine particles having a specific dielectric constant of not less than 10 at 1 kHz and at room temperature, and more preferably by one or more Each type of surface treatment agent performs a surface treatment on some or all of the inorganic particles.

The curing mechanism of the curable organopolyoxane composition of the present invention is not particularly limited, but the group capable of performing the curing reaction may be a curing reaction capable of undergoing a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction reaction. The group, and preferably, is capable of undergoing an addition curing reaction group represented by a hydrogenation reaction (particularly, a hydrazine-bonded unsaturated hydrocarbon group (for example, an alkenyl group) or a hydrazine atom-bonded hydrogen atom). Other constituent features that are advantageous for achieving better mechanical and/or electrical properties are set forth below.

By the present invention, a polyoxyxene elastomer cured product having excellent mechanical and/or electrical properties and particularly capable of being used as a member of a converter can be produced.

In addition, the present invention can provide a curable organopolyoxane composition which, when used as a dielectric layer of a converter, can have excellent mechanical properties and/or electrical properties (especially due to high specific dielectric constant, High dielectric breakdown strength and low energy density achieved by low Young's modulus) and excellent mechanical strength (specifically, tensile strength, tear strength, elongation, and the like) to achieve durability and actual displacement; The curable organopolyoxane composition produces a cured product that can be used as a material for the converter.

The invention can also provide a method for producing a curable organopolyoxane composition; a curable polyoxyxene elastomer material capable of being used as an electroactive polymer material for a converter; the curable polyoxyxene elastomer material a method of producing; and various types of converters using a curable polyoxyxene elastomer material.

1‧‧‧Actuator

2‧‧‧Actuator

3‧‧‧Sensor

4‧‧‧Power generation components

10a‧‧‧ dielectric layer

10b‧‧‧ dielectric layer

11a‧‧‧electrode layer (conducting layer)

11b‧‧‧electrode layer (conducting layer)

12‧‧‧ wire

13‧‧‧Power supply

20a‧‧‧ dielectric layer

20b‧‧‧ dielectric layer

20c‧‧‧ dielectric layer

21a‧‧‧Electrode layer (conducting layer)

21b‧‧‧Electrode layer (conductive layer)

21c‧‧‧electrode layer (conducting layer)

21d‧‧‧electrode layer (conductive layer)

22‧‧‧Wire

23‧‧‧Power supply

30‧‧‧Dielectric layer

31a‧‧‧Upper electrode layer

31b‧‧‧Upper electrode layer

31c‧‧‧ upper electrode layer

32a‧‧‧lower electrode layer

32b‧‧‧lower electrode layer

32c‧‧‧lower electrode layer

40a‧‧‧ dielectric layer

40b‧‧‧ dielectric layer

41a‧‧‧electrode layer

41b‧‧‧electrode layer

[Fig. 1] Fig. 1 illustrates a cross-sectional view of an actuator 1 of the present invention in which a dielectric layer is stacked.

2] Fig. 2 illustrates a cross-sectional view of an actuator 2 of the present invention in which a dielectric layer and an electrode layer are stacked.

Fig. 3 illustrates the configuration of the sensor 3 of the present invention.

Fig. 4 shows a cross-sectional view of a power generating element 4 of the present invention in which a dielectric layer is stacked.

By diligently exploring, the inventors have found that a curable organopolysiloxane cured product having excellent mechanical properties and/or electrical properties is obtained by a curable organopolyoxane composition. The oxyalkylene composition comprises: an organopolyoxane represented by the following formula (I): R ^a _a R ^b _b SiO _(4-ab)/2 (I)

Wherein R ^a is a monovalent aromatic hydrocarbon group having 6 to 10 carbons, and R ^b is at least one type of monovalent functional group (however, R ^b is in addition to a monovalent aromatic hydrocarbon group having 6 to 10 carbons) a group), wherein at least a portion of R ^{b is a} group capable of undergoing a curing reaction, and 0 < a, 0 < b, 1.9 < a + b <2.1; and one or more types of inorganic fine particles having a diameter of not less than An average primary particle diameter of 50 nm, wherein the mass fraction (Z) of the monovalent aromatic hydrocarbon group having 6 to 10 carbons in all the organopolysiloxanes is not less than 0.2% by mass and not more than 50% by mass, and all of the organic polyfluorene The mass fraction (W) of the linear organopolyoxane represented by the following formula (II) in the oxane is not less than 50% by mass: R ¹ R ² ₂ Si(OSiR ³ R ⁴ ) _n (OSiR ³ R ¹ ) _m OSiR ¹ R ² ₂ (II)

Wherein R ¹ is a group capable of undergoing a curing reaction, and R ² , R ³ and R ⁴ each independently represent, independently or differently represent a hydrogen atom, a monovalent aliphatic hydrocarbon group having 1 to 10 carbons, and have 6 to 10 The monovalent aromatic hydrocarbon group of carbon; the n and m systems respectively satisfy the values of the conditions 200 < n and 0 = < m = < (n / 20). Accordingly, the inventors have completed the present invention.

<Organic polyoxane>

The organopolyoxane represented by the general formula (I): R ^a _a R ^b _b SiO _(4-ab)/2 used in the present invention contains one or more kinds of organopolysiloxanes, and the whole has curability. And containing a monovalent aromatic hydrocarbon having 6 to 10 carbons (the mass fraction (Z) is not less than 0.2% by mass and not more than 50% by mass relative to all of the organopolysiloxane), and relative to all the organic polyfluorene The mass fraction (W) of the linear organopolyoxane represented by the above formula (II) is not less than 50% by mass. In addition, since the monovalent aromatic hydrocarbon Ra is ^a mandatory substituent, a>0, and more specifically, the a value must be a monovalent aromatic hydrocarbon having 6 to 10 carbons relative to the total organopolysiloxane. The mass fraction (Z) is not less than 0.2% by mass and not more than 50% by mass. Here, the organopolyoxane containing a monovalent aromatic hydrocarbon having 6 to 10 carbons may be the same as or different from the linear organopolyoxane represented by the above formula (II), but is given by the above formula (I) The organic polyoxoxane represented preferably contains a plurality of curable organopolyoxyalkylenes, in which case the mass fraction (Z) of the monovalent aromatic hydrocarbons satisfies the above range relative to the total organopolyoxane. And the mass fraction (W) of the linear organopolyoxane represented by the above formula (II) with respect to all the organopolyoxyalkylene is not less than 50% by mass. Assuming that the mass fraction (Z) of the monovalent aromatic hydrocarbon in all of the organopolysiloxanes satisfies the above range, the monovalent aromatic hydrocarbon having 6 to 10 carbons may be contained in any of the organic polyoxanes which may be cured or not. Cured in organic polyoxane.

First, a monovalent aromatic hydrocarbon group R ^a having 6 to 10 carbons is illustrated. The monovalent aromatic hydrocarbon group is exemplified by a phenyl group, a naphthyl group, a substituted phenyl group, and a substituted naphthyl group, and specific examples include a phenyl group, a naphthyl group, an o-tolyl group, a m-tolyl group, a p-tolyl group, a xylyl group, Ethyl phenyl and the like. On the other hand, although the aliphatic hydrocarbon group substituted by the aromatic hydrocarbon group (i.e., arylalkyl group) is not strictly an aromatic hydrocarbon group, it is also considered to be a monovalent aromatic hydrocarbon group in the present invention. Such groups are exemplified by benzyl, phenethyl and the like. Among these groups, phenyl is preferred from the viewpoint of economics and industrial productivity.

The content of the monovalent aromatic hydrocarbon group (relative to the mass fraction of all the organic decane components in the curable organopolyoxane composition: Z) is not less than 0.2% by mass and not more than 50% by mass. If Z is less than 0.2% by mass, the dielectric breakdown strength improving effect cannot be sufficiently exhibited in the obtained cured product, and on the other hand, if it exceeds 50% by mass, the obtained cured product has an excessively high modulus of elasticity and molded. The product is not brittle due to being too brittle. A preferred range of Z is not less than 0.5% by mass and not more than 30% by mass, and more preferably not less than 0.5% by mass and not more than 10% by mass.

The monovalent aromatic hydrocarbon groups are contained in an organopolyoxane containing a monovalent aromatic hydrocarbon group constituting part or all of the organic decane component. The organopolyoxyalkylene group containing a monovalent aromatic hydrocarbon group is exemplified by a dimethyl methoxy oxyalkylene/methyl phenyl siloxane copolymer terminated with a dimethylvinyl methoxy group at two molecular terminals. a dimethyl methoxy alkane/methylvinyl fluorene/methyl phenyl siloxane copolymer terminated with dimethylvinyl methoxy at the end of two molecules, at the end of two molecules via dimethyl a vinyl methoxy-terminated polymethylphenyl siloxane, a dimethyl methoxy oxane/diphenyl siloxane copolymer terminated with a dimethylvinyl methoxy group at the end of two molecules a dimethyl methoxy oxane/methylphenyl decane copolymer terminated with dimethylhydroquinone at the end of two molecules, terminated with dimethylhydroquinone at the end of two molecules Polymethylphenyl sulfoxane, a dimethyl methoxy oxane/diphenyl decane copolymer terminated with dimethylhydroquinone at the end of two molecules, and a trimethyl group at the end of two molecules a nonyloxy-terminated diphenyloxane/methylvinylaluminoxane copolymer, a diphenylphosphonium/methylhydroquinone terminated by a trimethylmethoxy group at two molecular ends Alkane copolymerization a methylphenyl siloxane/methylvinyl decane copolymer terminated with a trimethyl methoxy group at the end of two molecules, and a terminal terminated by a trimethyl methoxy group at two molecular ends a phenyl phenyl oxane/methylhydroquinoxane copolymer, a polymethylphenyl siloxane having a methyl phenylvinyloxy group terminated at the end of two molecules, at the end of two molecules Phenyl phenyl vinyl oxy-terminated polydiphenyl siloxane and the like.

The organopolyoxane represented by the general formula (I): R ^a _a R ^b _b SiO _(4-ab)/2 used in the present invention has curability as a whole, and in the formula (I), the R ^b system At least one type of monovalent functional group (however, R ^b is a group other than a monovalent aromatic hydrocarbon group having 6 to 10 carbons), and at least a portion of R ^b has a group capable of undergoing a curing reaction. Here, the substituents R ^b may be one type or two or more types of functional group, provided at least a part of the system-based substituent group capable of curing reaction and is not a substituent R ^b R ^a, and a substituted A part of the group R ^b is preferably a reactive group capable of undergoing a curing reaction by a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction.

Further, a part of the substituent R ^b is particularly preferably a non-reactive functional group. Further, the reactive group capable of undergoing a curing reaction as a part of the substituent R ^b may be one type or two or more types of reactive groups (for example, an addition reactive functional group and a photoreactive functional group) Combination).

Specific examples of the substituent R ^b as a non-reactive group are an alkyl group such as a methyl group, an ethyl group, a propyl group, a butyl group, a hexyl group, and the like. From the perspective of economics, the methyl group is preferred.

The substituent R ^b as a reactive group is a reactive group capable of undergoing a curing reaction by a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction. More preferably, a portion of R ^b is a reactive group capable of being cured by an addition reaction. Examples of reactive groups capable of undergoing an addition reaction include: a styryl group, a (meth)acrylic group, a vinyl ether group, and the like, which are addition polymerizable functional groups; organic groups containing thiol groups a group (which is a thiol-ene reactive group) and a combination of alkenyl groups; a BH group-containing organic group (which is a hydroboration reactive group) and a combination of alkenyl groups; a combination of an organic group of an atom (which is a hydrogenation-reactive group) and an alkenyl group; an organic group containing a diene group (which is a Diels-Alder reaction active group) And combinations of alkenyl groups; and the like. When combining the two types of reactive groups, it is especially preferred to use a compound having only one type of reactive group and a compound having another type of reactive group.

Other reactive groups capable of undergoing a curing reaction are exemplified by a hydroxyl group and an alkoxy group having 1 to 4 carbons, specifically, a methoxy group, an ethoxy group, a propoxy group, and the like, but are not limited thereto.

The organopolyoxane represented by the general formula (I): R ^a _a R ^b _b SiO _(4-ab)/2 used in the present invention is preferably an organic polyoxyalkylene which is curable by an addition reaction. Further, the group capable of undergoing the curing reaction is preferably a group capable of undergoing an addition reaction. The group capable of undergoing the addition reaction is as described above.

In particular, R ^b in formula (I) is selected from the group consisting of: optionally substituted monovalent hydrocarbon groups having from 1 to 10 carbons (however, R ^b is in addition to from 6 to 10 a group other than the monovalent aromatic hydrocarbon group of carbon), a hydrogen atom, an alkenyl group having 2 to 8 carbons, an alkoxy group having 1 to 4 carbons, and a hydroxyl group, and at least a part of R ^b is preferably capable of proceeding The addition reaction is selected from the group consisting of a hydrogen atom and an alkenyl group having 2 to 8 carbons.

In such groups, in view of the high reaction rate and low side reactions, at least a portion of R ^b is preferably a hydrogenation reactive group, that is, a halogen atom bonded to a hydrogen atom and an alkenyl group. Here, from the viewpoint of economics, a vinyl group is preferred as an alkenyl group.

In the organopolyoxane represented by the general formula (I): R ^a _a R ^b _b SiO _(4-ab)/2 , as used in the present invention, the ratio of the substituent on the ruthenium atom as a whole (矽 atom) The total number of substituents relative to the mass fraction of the ruthenium atom; a + b) is in the range of 1.9 < a + b < 2.1. If the ratio of the substituent is outside this range, the mechanical properties (especially tensile elongation at break and modulus of elasticity) of the obtained polyoxyxene elastomer of the cured product are insufficient and are not appropriate. Further, since 1.9 < a + b < 2.1, it is meant that the organopolysiloxane used in the present invention as a whole contains a plurality of chain polyoxyalkylene structures having diorganosiloxane units.

The organopolyoxane represented by the formula (I): R ^a _a R ^b _b SiO _(4-ab)/2 used in the present invention is also represented by the following formula (II) in an amount of not less than 50% by mass. Straight chain organic polyoxane. The content of the linear organopolyoxane is not less than 50% by mass. If the content is outside this range, the mechanical properties (especially the elongation at break) of the polyoxyxene elastomer as a cured product cannot reach a satisfactory range. The tensile elongation at break is preferably not less than 200%, as measured according to JIS K 6249, and the preferred content of the linear organopolyoxane for achieving this property is not less than 70% by mass. And not more than 99.9 mass%.

R ¹ R ² ₂ Si(OSiR ³ R ⁴ ) _n (OSiR ³ R ¹ ) _m OSiR ¹ R ² ₂ (II)

(In the formula, R ¹ is a group capable of undergoing a curing reaction, and R ² , R ³ and R ⁴ each independently, identically or differently represent a monovalent aliphatic hydrocarbon group having 1 to 10 carbons and have 6 to A monovalent aromatic hydrocarbon group of 10 carbons; n and m systems satisfy the values of the conditions 200 < n and 0 = < m = < (n / 20).

In the formula (II), R ¹ is a group capable of undergoing a curing reaction, and may be the same group as the reactive group of R ^b , but for the above reasons, a reactive group capable of undergoing an addition reaction Preferably. In particular, it is preferably a hydrogenation reactive group, that is, a ruthenium atom-bonded hydrogen atom or a vinyl group. R ² , R ³ and R ⁴ are each independently, identically or differently a monovalent aliphatic hydrocarbon group having 1 to 10 carbons and a monovalent aromatic hydrocarbon group having 6 to 10 carbons, and are exemplified as methyl group and B group. Base, propyl, butyl, hexyl, phenyl, naphthyl, substituted phenyl, substituted naphthyl, benzyl, phenethyl and the like, but from the economic point of view, methyl and phenyl are preferred . Further, it is needless to say that the monovalent aromatic hydrocarbon group in the linear organopolyoxane represented by the formula (II) is also included in the organic poly group represented by the formula (I) by the mass fraction (Z) of the monovalent aromatic hydrocarbon group. In the oxime.

In formula (II), n is a value exceeding 200. If it is not more than 200, the mechanical properties (especially elongation at break) of the obtained cured product are low, and thus are not suitable for use in the present invention. A value of not more than 20,000 is preferable in view of molding processability. On the other hand, there is no upper limit to the value of m, but similarly to the above, considering the elongation at break of the obtained cured product, it must be not more than (n/20). Additionally, this condition is closely related to the advantageous improvement of the present invention due to the fact that all of the decane components of the curable organopolyoxane composition described below satisfy the specified compositional characteristics.

Specific examples of the reactive organopolyoxyalkylene constituting the curable organopolyoxane composition used in the present invention include polydimethyl hydrazine terminated at two molecular terminals via dimethylvinyl hydroxy group. Oxyalkane, a dimethyl methoxy alkane/methylvinyl decane copolymer terminated with a dimethylvinyl methoxy group at the end of two molecules, and a dimethyl vinyl oxime at the end of two molecules a dimethyl methoxy oxane/methylphenyl decane copolymer at the base end, dimethyl methoxy oxane/methyl vinyl fluorene terminated by a dimethylvinyl methoxy group at two molecular terminals An alkane/methylphenyl decane copolymer, a polymethylphenyl decane terminated by a dimethylvinyl methoxy group at two molecular ends, and a dimethyl vinyl group at the end of two molecules a methoxy-terminated dimethyl methoxy oxane/diphenyl decane copolymer, a polydimethyl methoxy alkane terminated by a dimethyl hydroquinone at two molecular ends, in two molecules a dimethyl methoxy oxane/methylhydroioxane copolymer terminated with a dimethylhydroquinoneoxy group and a dimethyl hydroxy group at the end of two molecules a quinone oxo/methylphenyl decane copolymer, a polymethylphenyl siloxane having a dimethylhydroquinone-terminated at two molecular ends, and a dimethyl hydrogen at the ends of two molecules a methoxy-terminated dimethyl methoxy oxane/diphenyl decane copolymer, dimethyl methoxy oxane/methylhydroxyloxy terminated with dimethylhydroquinone at the end of two molecules An alkane/methylphenyl decane copolymer, a polymethylvinyl siloxane having a trimethyl methoxy group terminated at two molecular ends, and a trimethyl methoxy group at the end of two molecules a polymethylhydroquinone, a dimethyl methoxy alkane/methylvinyl decane copolymer terminated with a trimethyl methoxy group at the end of two molecules, and a trimethyl group at the end of two molecules a methoxy-terminated dimethyl methoxy oxane/methylhydroquinoxane copolymer, a diphenyl oxirane/methyl vinyl oxime terminated at the end of two molecules via a trimethyl methoxy group An alkane copolymer, a diphenyl methoxy oxane/methylhydroquinoxane copolymer terminated with a trimethyl methoxy group at two molecular ends, terminated by a trimethyl methoxy group at two molecular ends Methylphenyl decane / Vinyl vinyl alkane copolymer, methyl phenyl siloxane/methyl hydrazine copolymer terminated with trimethyl methoxy group at the end of two molecules, trimethyl group at the end of two molecules a methoxy-terminated dimethyl methoxy oxane/methylvinyl fluorene/methyl phenyl decane copolymer, a dimethyl hydrazine terminated by a trimethyl methoxy group at two molecular ends Oxylkane/methylhydroquinone/methylphenyl decane copolymer, dimethyl hydrogen functional MQ resin, dimethylvinyl functional MQ resin, diphenyl vinyl oxime at the ends of two molecules a polycapped dimethyl oxoxane, a polymethylphenyl siloxane having a diphenylvinyloxy group terminated at two molecular ends, and a diphenylvinyl fluorene at the end of two molecules. Oxy-terminated polydiphenyl fluorene oxide, polydimethyl methoxy oxane terminated by methyl phenyl vinyl methoxy group at two molecular ends, methyl phenyl ethylene at the ends of two molecules a oxy-terminated polymethylphenyl sulfoxane, a polydiphenyl fluorene terminated with a methylphenylvinyl methoxy group at the end of two molecules, containing dimethylvinyl fluorene Group _{((CH 3) 2 (CH} 2 = CH) SiO 1/2) and phenyl silicon group (C ₆ H ₅ SiO _3/2) the copolymer containing silicon dimethylhydrogensiloxy group ((CH ₃ a copolymer of ₂ HSiO _1/2 ) and phenyl decyloxy (C ₆ H ₅ SiO _3/2 ) containing dimethylvinyl decyloxy ((CH ₃ ) ₂ (CH ₂ =CH)SiO _{1 /2} ), a copolymer of dimethyl decyloxy ((CH ₃ ) ₂ SiO _2/2 ) and phenyl decyloxy (C ₆ H ₅ SiO _3/2 ), containing dimethylhydroquinoneoxy ( a copolymer of (CH ₃ ) ₂ HSiO _1/2 ), dimethyl decyloxy ((CH ₃ ) ₂ SiO _2/2 ) and phenyl decyloxy (C ₆ H ₅ SiO _3/2 ), containing a a copolymer of a vinyl methoxy group ((CH ₃ )(CH ₂ =CH)SiO _2/2 ) and a phenyl fluorenyloxy group (C ₆ H ₅ SiO _3/2 ), containing a methylhydroquinoneoxy group ( a copolymer of (CH ₃ )HSiO _2/2 ) and a phenyldecyloxy group (C ₆ H ₅ SiO _3/2 ) and the like. In these examples, it is particularly preferred to use an organic polysiloxane having a hydrogen atom bonded to a ruthenium atom and an organopolysiloxane having a ruthenium atom-bonded unsaturated hydrocarbon group as the organic polyoxane of the present invention. An alkane or a component constituting an organopolyoxyalkylene.

The number average molecular weight (Mw) of the reactive organopolyoxane is preferably in the range of from 250 to 100,000. In addition, there is no particular limitation on the viscosity of the reactive organopolyoxane measured at a shear rate of 10 (l/s) at 25 ° C using a rheometer equipped with a 20 mm diameter cone plate, but this The viscosity is preferably in the range of 1 mPa s to 50,000 mPa s, and particularly preferably in the range of 5 mPa s to 10,000 mPa s.

Further, the oxirane component of the curable organopolyoxane composition of the present invention can be constituted by appropriately combining the above various reactive organopolysiloxanes, thereby mass fraction of the monovalent aromatic hydrocarbon group (Z) And a linear chain having a reactive group at both ends of the molecular chain The mass fraction (W) of the organopolyoxane is within the specified range.

<Inorganic fine particles having an average primary particle diameter of not less than 50 nm>

Further, the curable organopolyoxane composition of the present invention is characterized in that the composition contains an organopolysiloxane having the above characteristics and at least one type of inorganic fine particles having an average primary particle diameter of not less than 50 nm. Therefore, a polyoxyxene elastomer cured product having excellent mechanical properties and/or electrical properties which are difficult to obtain using a conventional curable organopolyoxane composition can be obtained.

The average primary particle diameter of the particles is not less than 50 nm. The microparticles can be a mixture of microparticles of different particle diameters. The average particle diameter can be measured by a measurement method commonly used in the industry. For example, if the average particle diameter is not less than 50 nm and not more than about 500 nm, it can be observed by microscopy by averaging (using a transmission electron microscope (TEM), a field emission type transmission electron microscope (FE-TEM), The average primary particle diameter is measured by a scanning electron microscope (SEM), a field emission type scanning electron microscope (FE-SEM) or the like to measure the particle diameter. On the other hand, if the average particle diameter is not less than about 500 nm, the average primary particle diameter value can be directly measured by a laser diffraction-scattering type particle size distribution measuring device or the like.

The function and type of the inorganic fine particles are not particularly limited, but examples include conductive inorganic fine particles, insulating inorganic fine particles, thermally conductive inorganic fine particles, and dielectric inorganic fine particles. Preferably, one or more types selected from the group of particles are used in the compositions of the invention. In particular, it is preferred to use dielectric inorganic fine particles, and particularly preferably, the dielectric inorganic fine particles are dielectric inorganic fine particles in which at least one of the average primary particle diameter is not less than 50 nm or at least a part of a plurality of types of inorganic fine particles is at 1 kHz. And a specific dielectric constant of not less than 10 at room temperature. Further, the upper limit of the preferable size (average primary particle diameter) of the inorganic fine particles is 20,000 nm (20 μm), but 10,000 nm (10 μm) is more preferable in view of the rationality of the film used for the converter described below.

<Dielectric inorganic particles (C)>

Advantageously, the dielectric inorganic fine particles (C) are dielectric inorganic fine particles (C1) having a specific dielectric constant of not less than 10 at 1 kHz and room temperature. By carrying dielectric inorganic particles in a cured product comprising a curable organopolyoxyalkylene, the physical and electrical properties required for the converter are met.

For example, the dielectric inorganic fine particles may be selected from a metal oxide represented by the following formula (C2) (hereinafter also referred to as "metal oxide (C2)"): M ^a _na M ^b _nb O _nc (C2)

(In the formula, the second metal element M ^a system of the Periodic Table; Group 4 metal element M ^b of the Periodic Table of the system; of Na-based value between 0.9 to 1.1; Nb-based range of 0.9 to 1.1 The value between; and the nc is between 2.8 and 3.2)

Preferred examples of the Group 2 metal element M ^a of the periodic table in the metal oxide (C2) include beryllium (Be), magnesium (Mg), calcium (Ca), strontium (Sr) and barium (Ba). Titanium (Ti) is cited as a preferred example of the Group 4 metal element M ^b of the periodic table. In the particles of the metal oxide represented by the formula (C2), each of M ^a and M ^b may be a single element or may be two or more elements.

Specific examples of the metal oxide (C2) include barium titanate, calcium titanate, and barium titanate.

For example, the dielectric inorganic fine particles may be selected from a metal oxide represented by the following formula (C3) (hereinafter also referred to as "metal oxide (C3)"): M ^a _na M ^b' _nb' O _nc (C3)

(In the formula, Ma is ^a Group 2 metal element of the periodic table; M ^{b '} is the fifth periodic metal element of the periodic table; na is a value between 0.9 and 1.1; nb' is between 0.9 and The value between 1.1; and the nc is between 2.8 and 3.2)

Preferred examples of the Group 2 metal element M ^a of the periodic table in the metal oxide (C3) include beryllium (Be), magnesium (Mg), calcium (Ca), strontium (Sr) and barium (Ba). Preferred examples of the metal element M ^{b '} of the fifth period of the periodic table include tin (Sn), bismuth (Sb), zirconium (Zr), and indium (In). In the particles of the metal oxide represented by the formula (C3), each of M ^a and M ^{b '} may be a single type of element or may be two or more elements.

Specific examples of the metal oxide (C3) include magnesium stannate, calcium stannate, barium stannate, barium stannate, magnesium citrate, calcium citrate, barium strontium citrate, barium strontium citrate, magnesium zirconate, calcium zirconate, Barium zirconate, barium zirconate, magnesium indium, calcium indium, barium indiumate and barium indium.

In addition, in combination with such metal oxide particles, particles of other metal oxides may be permitted, such as lead zirconate titanate, zinc titanate, lead titanate, titanium oxide or the like (especially in addition to those previously listed) Their other titanium oxide composite oxides). In addition, a solid solution including other metal elements may be used as the dielectric inorganic fine particles (C). In this case, other metal elements are exemplified as La (镧), Bi (铋), Nd (钕), Pr (鐠), and the like.

Among the inorganic fine particles, preferred examples of the dielectric inorganic fine particles (C) include one or more types of inorganic fine particles selected from the group consisting of titanium oxide, barium titanate, barium titanate, lead zirconate titanate, And a composite metal oxide in which barium titanate and titanium are partially replaced by an alkaline earth metal such as calcium or barium, zirconium or a rare earth metal such as lanthanum, cerium, lanthanum or cerium. Titanium oxide, barium titanate, barium zirconate titanate and barium titanate are more preferred, and titanium oxide and barium titanate are preferred.

The form of the dielectric inorganic fine particles (C) may be in any form such as a spherical shape, a flat shape, a needle shape, a fibrous shape or the like. The average primary particle diameter is not less than 50 nm, but in view of mold handling property, particularly film formability, of the curable organopolyoxane composition, a range of 50 nm to 5,000 nm is preferred. If the inorganic fine particles are in the form of flat, needle-like, fibrous or the like, the aspect ratio is usually not less than 5 although the aspect ratio of the fine particles is not limited.

The specific limitation is not imposed on the particle size distribution of the dielectric inorganic fine particles (C), and the dielectric inorganic fine particles may be monodisperse fine particles, or alternatively, the void fraction between the fine particles may be reduced by filling at a higher density. A particle diameter distribution is produced to improve mechanical strength. As a measure of the particle size distribution, with the particle diameter at the cumulative particle size distribution curve by the method of laser light diffraction in the amount of 90% cumulative area (D ₉₀₎ to (D ₁₀₎ of the ratio of the particle diameter at 10% cumulative area (D ₉₀ /D ₁₀ ) is preferably not less than 2. In addition, no limitation is imposed on the shape of the particle size distribution (the relationship between the particle diameter and the particle concentration). There may be a so-called flat top distribution or a multimodal (i.e., bimodal (i.e., having two mountain distributions), three peaks, or the like) particle size distribution.

In order to obtain a particle size distribution of dielectric inorganic particles (C) similar to those of the above particle size distribution, various methods may be employed, for example, combining two or more types of particles having different average diameters or particle size distributions, and blending Particles of various particle diameter fractions obtained by sieving or the like to produce a desired particle size distribution, or the like.

Further, the dielectric inorganic fine particles (C) can be treated using various types of surface treating agents as described below.

In view of the mechanical properties and dielectric properties of the obtained cured product, the blending amount (filling ratio) of the electro-organic inorganic fine particles (C) of the curable organopolysiloxane composition of the present invention is relative to the total volume of the composition. It may be not less than 10%, preferably not less than 15%, and further preferably not less than 20%. Further, the blending amount with respect to the total volume of the composition is preferably not more than 70% and further preferably not more than 60%.

In the curable organopolyoxane composition of the present invention, one or more types of inorganic fine particles having an average primary particle diameter of not less than 50 nm are preferably dielectric inorganic fine particles (C), but they may also contain the following conductive materials. Inorganic fine particles, insulating inorganic fine particles, and thermally conductive inorganic fine particles.

The conductive inorganic fine particles usable herein are not particularly limited as long as they impart conductivity to the cured product of the organopolyoxane composition. Specific examples of the conductive inorganic fine particles include: conductive carbon such as conductive carbon black, graphite, vapor grown carbon (VGCF) or the like; and metal powder such as platinum, gold, silver, copper, nickel, tin, zinc, iron, Aluminum or the like; and coated pigments such as antimony doped tin oxide, phosphorus doped tin oxide, a needle-shaped titanium oxide surface-treated with tin oxide/niobium oxide, tin oxide, indium oxide, antimony oxide or zinc antimonate, and graphite or carbon whisker such as surface-treated with tin oxide or the like; and at least one type of conductive metal oxide ( It is selected from pigments coated with tin-doped indium oxide (ITO), fluorine-doped tin oxide (FTO), and phosphorus-doped tin oxide and phosphorus-doped nickel oxide; conductive and in the surface of titanium dioxide particles Pigments containing tin oxide and phosphorus; the conductive inorganic particles are surface treated as appropriate using various types of surface treatment agents as set forth below. The conductive inorganic fine particles may be used in one type or in a combination of two or more types.

Further, the conductive inorganic fine particles may be fibers such as glass fibers, cerium oxide alumina fibers, alumina fibers, carbon fibers or the like; or acicular reinforcing materials such as aluminum borate whiskers, potassium titanate whiskers or the like; or inorganic A filler material such as glass beads, talc, mica, graphite, apatite, dolomite or the like, the surfaces of which are coated with a conductive substance such as a metal or the like.

The specific dielectric constant of the organopolyoxyalkylene cured product can be increased by blending conductive inorganic particles into the composition. Regarding the application of the conductive inorganic fine particles, the blending amount thereof relative to the curable organopolyoxane composition is preferably in the range of 0.01% by mass to 10% by mass, and more preferably 0.05% by mass to Within 5 mass%. When the blending amount of the conductive inorganic fine particles deviates from the above preferred range, the blending effect cannot be obtained, or the dielectric collapse strength of the cured product can be lowered.

The insulating inorganic fine particles usable in the present invention are not particularly limited, provided that they are generally known as insulating inorganic fine particles, that is, inorganic material particles having a volume resistivity of 10 ¹⁰ ohm cm to 10 ¹⁸ ohm cm, and may be particles or flakes. And any of the fibers (including whiskers) used. Preferred specific examples include spherical particles, flat particles and ceramic fibers, metal silicate particles (for example, alumina), iron oxide, copper oxide, mica and talc, and particles such as quartz, amorphous ceria, and glass. Further, the insulating inorganic fine particles may be subjected to surface treatment using various types of surface treating agents as described below. The electrically insulating inorganic fine particles may be used in one type or in a combination of two or more types.

The mechanical strength and dielectric breakdown strength of the organopolyoxyalkylene cured product can be increased by blending the insulating inorganic fine particles into the composition, and sometimes the specific dielectric constant is observed to increase. Regarding the application of the insulating inorganic particles, the blending amount thereof relative to the curable organopolyoxane composition is preferably in the range of 0.1% by mass to 20% by mass, and more preferably 0.1% by mass to Within 5 mass%. When the blending amount of the insulating inorganic particles deviates from the above preferred range, the blending effect cannot be obtained, or the mechanical strength of the cured product can be lowered.

Examples of the thermally conductive inorganic fine particles usable in the present invention are metal oxide particles such as magnesium oxide, zinc oxide, nickel oxide, vanadium oxide, copper oxide, iron oxide, silver oxide, and the like; and inorganic compound particles such as aluminum nitride. , boron nitride, tantalum carbide, tantalum nitride, boron carbide, titanium carbide, diamond, diamond-like carbon, and the like. Zinc oxide, boron nitride, tantalum carbide and tantalum nitride are preferred. By incorporating one or more types of such thermally conductive inorganic particles into the composition, the thermal conductivity of the organopolyoxyalkylene cured product can be increased. In view of the application of the thermally conductive inorganic fine particles, the blending amount with respect to the curable organopolyoxane composition is preferably in the range of 0.1% by mass to 30% by mass.

The curable organopolyoxane composition of the present invention contains an organic polyoxoxane and at least one type of inorganic fine particles having an average primary particle diameter of not less than 50 nm, but more advantageously, an organic polyoxane combination is preferred. The material satisfies the composition characteristics of items [1], [2] and [3] below.

[1] The curable organopolyoxane composition is not less than 0.1% by mass and not more than 10% by mass relative to all of the organopolyoxane component in the curable organopolyoxane composition. Containing an organopolyoxane represented by the formula: M _a M ^R _b D _c D ^R _d T _e T ^R _f Q _g , wherein (a+c)/(b+d+e+f+g) Less than 3. Here, in the above formula, M is a triorganosyloxy unit; a D is a diorganomethoxy unit; a T is a _{monoorganomethoxy} unit; and a Q is a _decyl unit represented by SiO _4/2 . And the substituent R on each of the methoxy units is a group capable of undergoing a curing reaction by a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction.

[2] The curable organopolyoxane composition contains the amount in an amount of not less than 75% by mass and not more than 99.9% by mass, based on the entire oxyalkylene component in the curable organopolyoxane composition. A reactive organopolyoxyalkylene having a group capable of undergoing a curing reaction by a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction at two molecular terminals.

[3] The curable organopolyoxane composition contains at least: (S) reactivity having at least two groups capable of undergoing a curing reaction by a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction in a molecule An organic polyoxyalkylene oxide having a mean molecular weight of less than 10,000 between two groups capable of undergoing a curing reaction; and (L) having at least two capable of undergoing a condensation reaction in the molecule a reactive organopolyoxane which is a group which undergoes a reaction, a peroxidation reaction or a photoreaction to carry out a curing reaction, and the reactive organopolyoxane L has a molecular weight of not less than 10,000 and not more than 150,000 between the two groups; And the blending ratio of the component (S) and the component (L) is 1:99 to 20:80.

The above features [1] to [3] are explained in further detail below. More preferably, the organopolyoxane of the present invention satisfies all of these conditions.

With respect to the feature [1], with respect to all of the oxane component in the curable organopolyoxane composition of the present invention, by M _a M ^R _b D _c D ^R _d T _e T ^R _f Q _g (wherein the value of (a+c)/(b+d+e+f+g) is less than 3) represents that the mass fraction of the reactive organopolyoxane is preferably not less than 0.1% by mass and not more than 10% by mass. And particularly preferably not less than 0.1% by mass and not more than 5% by mass. When the ratio is less than 0.1% by mass, the number of crosslinking points in the polyoxyalkylene component is too low, and thus there is a risk that mechanical strength and dielectric breakdown strength are insufficient after the curing reaction. On the contrary, a ratio of more than 10% by mass is not preferable because the number of crosslinking points is excessive, and thus the modulus of elasticity after curing is high and the elongation at break is low.

With respect to the feature [2], reactive organic polymerization having a group capable of undergoing a curing reaction at only two molecular terminals with respect to all of the organopolyoxane components in the curable organopolyoxane composition The weight fraction of the oxane is preferably not less than 75% by mass and not more than 99.9 mass%. If the ratio is outside the above range, it is not preferable because the high elongation at break of the polysiloxane elastomer as a cured product cannot be achieved or the dielectric collapse strength is insufficient. Here, as the group capable of undergoing a curing reaction, a group capable of undergoing a condensation reaction, an addition reaction, a peroxidation reaction, or a photoreaction can be used. However, for reasons similar to those set forth above, this group is preferably capable of undergoing an addition reaction. In such groups capable of undergoing an addition reaction, the group is preferably active in a hydrogenation reaction, that is, the group contains a group in which a halogen atom is bonded to a hydrogen atom or contains an aliphatic unsaturated bond. a group (for example, an alkenyl group having 2 to 20 carbons or the like). Specific examples thereof include polydimethyl methoxy oxane terminated with dimethylhydroquinone at the end of two molecules and polydimethyl hydrazine terminated by dimethylvinyl hydroxy groups at the ends of two molecules. Oxytomane. To further suit the material properties of such polymers (eg, mechanical, dielectric, heat resistant, or the like), a portion of the methyl groups of the polymers may be substituted with ethyl, propyl, butyl, hexyl or phenyl groups. .

The number average molecular weight (Mw) of the reactive organopolyoxane having only a group capable of undergoing a curing reaction at the end of two molecular chains is in the range of 250 to 100,000. In addition, there is no particular limitation on the viscosity of the reactive organopolyoxane measured at a shear rate of 10 (l/s) at 25 ° C using a rheometer equipped with a 20 mm diameter cone plate, but this The viscosity is preferably in the range of from 1 mPa s to 100,000 mPa s, and more preferably in the range of from 5 mPa s to 10,000 mPa s.

In the case of the feature [3], in the present invention, it is preferred to use a reactive organopolyoxane (S) which is a reactive organopolyoxy group having at least two groups capable of undergoing a curing reaction in the molecule. An alkane having an average molecular weight of less than 10,000 between two groups capable of undergoing a curing reaction) and a reactive organopolyoxane (L) having at least two groups capable of undergoing a curing reaction in the molecule The reactive organopolyoxane has a molecular weight of not less than 10,000 and not more than 150,000 between two groups capable of undergoing a curing reaction. The reactive organopolyoxanes are contained in the molecule as a short chain non-reactive polymer portion and a long chain non-reactive polymer portion, respectively. Here, there is an inverse at only the two ends of the molecular chain In the case of a functional organofunctional chain polyorganosiloxane, the molecular weight between the two groups capable of undergoing a crosslinking reaction is defined as a non-reactive polyoxane moiety (excluding both ends) The molecular weight of the oxy unit). In the case of a molecular weight between a plurality of groups capable of undergoing a crosslinking reaction, this molecular weight is the molecular weight of the longest portion.

When the component (S) and the component (L) are used together as the raw material for the curable organopolyoxane in the above blending ratio, the polyoxyxene elastomer obtained by the curing reaction may be formed. Part of the chain length is introduced into the polyoxyxene chain component. In this way, the permanent strain of the obtained polyoxyxene elastomer can be reduced, and the mechanical energy conversion loss can be reduced. In particular, when the polyxene oxide elastomer of the present invention is used in a dielectric layer of a converter, the combined use of component (S) and component (L) has the practical advantage of improving energy conversion efficiency.

As mentioned previously, a group capable of undergoing a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction may be used as a group capable of undergoing a curing reaction of the components. However, for reasons similar to those set forth above, this is preferably a group capable of undergoing an addition reaction. In the group capable of undergoing an addition reaction, the group is preferably a hydrogenation-reactive group, that is, the group contains a hydrogen atom bonded to a halogen atom or a group containing an aliphatic unsaturated bond (for example, 2 to 20 carbon alkenyl groups or the like). Specific examples of the reactive organopolyoxyalkylenes (S) and (L) are cited as examples of reactive organopolyoxyalkylene represented by M _a M ^R _b D _c D ^R _d T _e T ^R _f Q _g And an example of a reactive organopolyoxyalkylene which is cited as having only a group capable of undergoing a curing reaction at the end of two molecular chains. To further suit the mechanical and thermal properties after curing, a portion of the methyl group may be substituted with ethyl, propyl, butyl, hexyl or phenyl.

The preferred range of the blending ratio (mass ratio) S:L of the component (S) and the following component (L) is from 1:99 to 40:60. If the blend ratio value is outside this range, the cured product obtained by curing the curable organopolyoxane composition of the present invention cannot satisfy at least one property (including high elongation at break, high mechanical strength, high dielectric Electrical collapse strength and low elastic modulus).

<SiH/Vi ratio>

The curable organopolyoxane composition is advantageously cured by a hydrazine hydrogenation reaction, and the hydrazine-bonded hydrogen atom (H) in the organopolysiloxane of the invention is bonded to an unsaturated hydrocarbon group (Vi) The blend ratio (molar ratio) is preferably in the range of 0.5 to 3.0. When the value is outside the above range, the residual functional group after curing by the hydrazine hydrogenation reaction may adversely affect the material physical properties of the cured product.

The curable organopolyoxane composition of the present invention preferably contains a curing catalyst (B) for curing the organopolyoxane component.

The component (B) used in the present invention is preferably a compound which is generally referred to as a hydrazine hydrogenation reaction catalyst, and is not particularly limited, provided that it is a substance capable of promoting a hydrogenation reaction of hydrazine. Examples include platinum-based catalysts, ruthenium-based catalysts, and palladium-based catalysts. Among these catalysts, since the catalytic activity is high, a platinum group element catalyst and a platinum group element compound catalyst are particularly cited as the component (B). Without limitation, the platinum-based catalyst is exemplified by platinum fine powder, platinum black, chloroplatinic acid, alcohol modified chloroplatinic acid, chloroplatinic acid-diolefin complex, olefin-platinum complex; platinum-carbonyl a complex such as bis(acetonitrile) platinum, bis(ethylmercaptopyruvate) platinum or the like; a chloroplatinic acid-alkenyl alkoxylate complex such as chloroplatinic acid-divinyltetramethyl a oxane complex, a chloroplatinic acid-tetravinyltetramethylcyclotetraoxane complex or the like; a platinum-alkenyl alkane complex, such as platinum-divinyltetramethyldifluorene An oxane complex, a platinum-tetravinyltetramethylcyclotetraoxane complex or the like; and a complex between chloroplatinic acid and acetylene alcohol. The preferred example of component (B) is a platinum-alkenyl alkane complex, especially platinum 1,3-divinyl-1.1,3,3, due to the higher catalytic activity of the hydrogenation reaction. - Tetramethyldioxane complex.

Further, in order to further improve the stability of the platinum-alkenyl alkane complex, the platinum-alkenyl alkoxylate complex may be dissolved in an organic oxane oligomer such as: 1,3 -divinyl-1,1,3,3-tetramethyldioxane, 1,3-diallyl-1,1,3,3-tetramethyldioxane, 1,3- Divinyl-1,3-dimethyl-1,3-diphenyldioxane, 1,3-divinyl-1,1,3,3-tetraphenyldioxane, 1, 3,5,7-tetramethyl-1,3,5,7-tetravinylcyclotetraoxane Or an alkenyl alkoxy olefin oligomer such as; or a dimethyl methoxy olefin oligomer; or the like. In particular, a platinum-alkenyl alkoxylate complex dissolved in an alkenyloxyalkane oligomer is preferably used.

The component (B) may be utilized in any amount which is capable of promoting the addition reaction of the organopolyoxane component of the composition of the present invention, without particular limitation. The concentration of the platinum group metal atom (for example, platinum atom) contained in the component (B) is usually in the range of 0.01 ppm to 500 ppm, preferably in the range of 0.1 ppm to 100 ppm, based on the total mass of the organopolyoxane component. Internal, and particularly preferably in the range of 0.1 ppm to 50 ppm.

An example of a preferred embodiment of the curable organopolyoxane composition of the present invention is a composition comprising the following optional ingredients: at least one type of reaction having at least two ruthenium atoms bonded to a hydrogen atom in the molecule The organoorganohydropolysiloxane (A1) having a hydrogen atom weight fraction of 0.01% by weight to 2.0% by weight; at least one type of reactive organic polymer having a repeating unit number of more than 200 and having an alkenyl group at two molecular terminals a siloxane (A2); a weight fraction of an alkenyl group of 0.05% by weight to 5.0% by weight; a hydrogenation reaction catalyst (B); and a dielectric inorganic fine particle (C1); which has not less than 10 at 1 kHz and room temperature. The specific dielectric constant.

Here, a preferred example of (A1) is a polydimethyl methoxy alkane terminated with a dimethylhydroquinone group at the end of two molecules, and terminated with a trimethyl methoxy group at the end of two molecules. a dimethyl methoxy oxane/methylhydroquinoxane copolymer and a dimethyl methoxy oxane/methylhydroquinoxane copolymer terminated by a dimethylhydroquinone group at two molecular ends. On the other hand, an example of (A2) is a polydimethylsiloxane having a terminal end of two molecular groups terminated by dimethylvinyloxyl group, and a dimethylvinyl alkoxy group at the end of two molecules. a polymethylphenyl sulfoxane, a dimethyl methoxy oxane/methylvinyl decane copolymer terminated with a dimethylvinyl methoxy group at the end of two molecules, and at the end of two molecules a dimethyl methoxy oxane/methyl phenyl siloxane copolymer terminated with dimethylvinyl methoxy. To further optimize material properties (such as mechanical properties, dielectric properties, heat resistance, and the like), ethyl, propyl, butyl, and hexyl can be used. The base or phenyl group is substituted for a part of the methyl group of the polymer.

The molecular weight of (A1) and (A2) is not particularly limited as long as the weight fraction of the hydrogen atom and the weight fraction of the alkenyl group are within the above range. However, the number of units of the oxane is preferably from 5 to 1,500.

The curable organopolyoxane composition of the present invention can be further provided with the following characteristics.

The curable organopolyoxane composition of the present invention may also contain at least one type of inorganic particulate having an average primary particle diameter of less than 50 nm.

The function of at least one type of inorganic fine particles having an average primary particle diameter of less than 50 nm and the like are not particularly limited, provided that the average primary particle diameter is less than 50 nm, and even so-called nanocarbon materials (for example, single layer, double layer, and multilayer) may be used. Carbon nanotubes, fullerenes, metal-encapsulated fullerenes, single-layer and multi-layer graphene, carbon nanofibers and the like are used as dielectric inorganic particles.

Preferred examples of at least one type of inorganic fine particles having an average primary particle diameter of less than 50 nm are reinforcing inorganic fine particles, which are exemplified by fumed cerium oxide, wet cerium oxide, ground cerium oxide, calcium carbonate, diatomaceous earth, fine Grinding quartz, various types of metal oxide powders other than alumina-zinc oxide, glass fibers, carbon fibers, and the like. Additionally, it can be used after treatment with various types of surface treatment agents as set forth below. Among them, cerium oxide is especially recommended.

From the viewpoint of mechanical strength improvement, preferred examples are partially concentrated fumed cerium oxide having an average primary particle diameter of not more than 10 nm and a specific surface area of not less than 50 m ² /g and not more than 300 m ² /g. Further, from the viewpoint of improvement in dispersibility, fumed cerium oxide treated with the following decane coupling agent is preferred. However, if the curable organopolyoxane (A) is additive curable, the cerium-doped surface treated fumed cerium oxide is not used as the reinforcing inorganic particles. The reinforcing inorganic particles may be used in a single type or may be used in combination of two or more types.

By blending the reinforcing inorganic particles into the composition, the mechanical strength and dielectric collapse strength of the organopolyoxyalkylene cured product can be increased. The blending amount of the reinforcing inorganic fine particles with respect to the curable organopolyoxane composition is preferably in the range of 0.1% by mass to 30% by mass, and more preferably in the range of 0.1% by mass to 10% by mass. When the blending amount deviates from the above preferred range, the effect of not incorporating the inorganic fine particles or the moldable processability of the curable organopolyoxane composition can be lowered.

One or more types of surface treatment agents may be used to surface treat some or all of the inorganic particulates (regardless of particle diameter, function, or the like) used in the curable organopolyoxyalkylene composition of the present invention. The type of the surface treatment may be a hydrophilic treatment or a hydrophobization treatment and is not particularly limited, but a hydrophobizing treatment is preferred. When the inorganic fine particles subjected to the hydrophobization treatment are used, the inorganic fine particles can be dispersed into the organopolyoxane composition at a high filling ratio. In addition, the viscosity increase of the composition is suppressed, and the mold processability is improved.

The surface treatment can be carried out by treating (or coating) the inorganic fine particles with a surface treating agent. The surface treatment agent for hydrophobization is exemplified by at least one type of surface treatment agent selected from the group consisting of an organotitanium compound, an organic cerium compound, an organozirconium compound, an organoaluminum compound, and an organophosphorus compound. The surface treatment agents may be used singly or in combination of two or more types.

The organotitanium compound is exemplified by a coupling agent such as titanium alkoxide, titanium chelate, titanium acrylate or the like. Preferred coupling agents in such compounds are exemplified by titanium alkoxide compounds such as tetraisopropyl titanate or the like; and titanium chelates such as tetraisopropylbis(dioctyl phosphate) titanate or And so on.

The organic ruthenium compound is exemplified as a low molecular weight organic ruthenium compound such as decane, decane, decane or the like; and an organic ruthenium polymer or oligomer such as polyoxyalkylene, polycarbazane or the like. Preferred decanes are exemplified by the so-called decane coupling agents. Representative examples of such decane coupling agents include alkyl trialkoxy decanes (e.g., methyltrimethoxy fluorene). Alkane, vinyltrimethoxynonane, hexyltrimethoxydecane, octyltrimethoxydecane or the like), alkoxy decane containing an organofunctional group (for example, glycidoxypropyltrimethoxydecane, epoxy) Cyclohexylethyltrimethoxydecane, methacryloxypropyltrimethoxydecane, aminopropyltrimethoxydecane or the like). Preferably, the decane and the polyoxyalkylene comprise hexamethyldioxane, 1,3-dihexyl-tetramethyldioxane, and a polyalkylene terminated by a trialkoxyalkylene group at one terminal. a methyloxane, a polydimethyloxane terminated with a trialkoxyalkylene group at one molecule and terminated with a dimethylvinyl group at the other end of the molecule, and a trialkoxy group at the end of one molecule. a polydimethyl methoxy alkane terminated by an alkyl group and terminated with an organic functional group at the other molecular end, and a polydimethyl methoxy alkane terminated by a trialkoxy fluorenyl group at the end of two molecules, Two polydimethylsiloxanes terminated at the end of the molecule via an organofunctional group or the like. The number n of the oxane bonds in this case is preferably from 2 to 150. Preferred examples of the decane alkane include hexamethyldioxane, 1,3-dihexyl-tetramethyldiazepine, and the like. Preferred polycarbomethoxyanes are exemplified as polymers having Si-C-C-Si-O linkages in the polymer backbone.

The organic zirconium compound is exemplified by an alkoxy zirconium compound (e.g., tetraisopropoxy zirconium or the like) and a zirconium chelate.

The organoaluminum compound is exemplified by aluminum alkoxide and aluminum chelate.

The organophosphorus compound is exemplified by a phosphite, a phosphate, and a phosphoric acid chelate.

Among these surface treatment agents, an organic ruthenium compound is preferred. Among these organic ruthenium compounds, decane, decane and polyoxane are preferred. As explained previously, it is preferred to use an alkyltrialkoxydecane and a polydimethyloxane which are terminated at the molecular end with a trialkoxyalkylene group.

The ratio of the surface treating agent to the total amount of the inorganic fine particles is preferably not less than 0.1% by mass and not more than 10% by mass, and more preferably not less than 0.3% by mass and not more than 5% by mass. Further, the treatment concentration is the ratio of the supplied inorganic particles to the supplied surface treatment agent, and preferably the excess surface treatment agent is removed after the treatment.

The curable organopolyoxane composition of the present invention may further comprise an additive for improving mold release or dielectric breakdown characteristics. An electroactive polysiloxane elastomer sheet obtained by curing the organopolyoxane composition into a sheet can be advantageously used as an electroactive film (dielectric layer or electrode layer) constituting the converter. However, when the release property of the polyoxyxene elastomer sheet during film molding is poor, and particularly when a dielectric film is produced at a high speed, the dielectric film may be damaged by demolding. However, the curable organopolyoxane composition of the present invention has excellent mold release property, and thus the curable organopolyoxane composition is advantageous in that it does not damage the film. The rate at which the film is produced is improved. This additive further improves these characteristics of the curable organopolyoxane composition of the present invention, and the additive may be used singly or in combination of two or more types. On the other hand, according to the name of the additive, an additive which improves dielectric breakdown characteristics is used to improve the dielectric breakdown strength of the polyoxyxene elastomer sheet obtained by curing.

The mold release improving additive (that is, the release agent) which can be used is exemplified as a carboxylic acid-based release agent, an ester-based release agent, an ether-based release agent, a ketone-based release agent, and an alcohol-based release agent. Agent, fluorine-based release agent and the like. These release agents may be used singly in a single type or in combination of two or more types. Further, although the releasing agent does not contain a halogen atom, a releasing agent containing a halogen atom may be used, or a mixture of the releasing agents may be used.

The release agent containing no halogen atoms may be selected, for example, from the group consisting of saturated or unsaturated aliphatic carboxylic acids such as palmitic acid, stearic acid or the like; alkali metal salts of such aliphatic carboxylic acids ( For example, sodium stearate, magnesium stearate, calcium stearate or the like; esters of aliphatic carboxylic acids with alcohols (eg 2-ethylhexyl stearate, glyceryl tristearate, neopentyl alcohol) Monostearate or the like), an aliphatic hydrocarbon (liquid paraffin, paraffin or the like), an ether (distearyl ether or the like), a ketone (distearyl ketone or the like), a high carbon number alcohol (2- Cetylstearyl alcohol or the like and mixtures of such compounds.

The release agent containing a ruthenium atom is preferably a polyfluorene-based non-curable release agent. The Specific examples of polyoxo-based release agents include non-organic modified polyoxyxides such as polydimethylsiloxane, polymethylphenyloxane, poly(dimethyloxane-methyl) Phenyl phenyl oxyalkylene) copolymer, poly(dimethyl methoxy oxane-methyl (3,3,3-trifluoropropyl) decane copolymer or the like; and modified polyoxyl oil, for example Amine-based modified polyfluorene oxide, amino polyether modified polyfluorene oxide, epoxy modified polyoxynium, carboxyl modified polyoxyn, polyoxyalkylene modified polyoxyl or the like. The polyoxon release agent may have any structure such as a linear, partially branched linear or cyclic structure. Further, the viscosity of the polyoxygenated oil at 25 ° C is not subject to specific restrictions. The viscosity is preferably in the range of 10 mPa s to 100,000 mPa s, and particularly preferably in the range of 50 mPa s to 10,000 mPa s.

Although no particular limitation is imposed on the blending amount of the demolding improving additive, the amount is preferably not less than 0.1% by mass and not more than 30% by mass based on the total amount of the curable organopolyoxane composition.

On the other hand, the dielectric breakdown property improver is preferably an electrical insulation improver. The dielectric breakdown property improver is exemplified by aluminum or magnesium hydroxide or a salt, clay mineral, and a mixture of such materials. Specifically, the dielectric breakdown property modifier may be selected from the group consisting of aluminum citrate, aluminum sulfate, aluminum hydroxide, magnesium hydroxide, calcined clay, montmorillonite, hydrotalcite, talc, and mixtures thereof. . In addition, the insulation modifier may be surface treated by a surface treatment method as may be required.

Although no particular limitation is imposed on the blending amount of the insulating modified additive, the amount is preferably not less than 0.1% by mass and not more than 30% by mass based on the total amount of the curable organopolyoxane composition.

The curable organopolyoxane composition of the present invention may comprise other organopolyoxane having a different high dielectric functional group than the reactive organopolyoxane.

In the same manner, the curable organopolyoxane composition of the present invention may further comprise including a high dielectric functional group in the molecule and at least one capable of undergoing a condensation curing reaction, an addition curing reaction, a peroxidation curing reaction or light. Curing reaction Compound. This high dielectric functional group is introduced into the obtained cured product (i.e., electroactive polysiloxane elastomer) by a curing reaction.

For the curable organopolyoxane composition of the present invention, part or all of the reactive organopolyoxane may be a reactive organopolyoxane further having a high dielectric functional group.

If a polyoxyxene elastomer obtained by curing the curable organopolyoxane composition of the present invention is used for a dielectric layer, the dielectric constant of the dielectric layer is preferably higher and can be introduced high. Dielectric functional groups to improve the specific dielectric constant of the elastomer.

Specifically, the dielectric properties of the curable polyoxyxene elastomer obtained by curing the curable organopolyoxane composition and the cured curable organopolyoxane composition can be increased by, for example, the following method: A component imparting high dielectric properties is added to the cured organopolyoxane composition, and a group imparting high dielectric properties is introduced into the organopolyoxane component constituting the curable organopolyoxane composition. , or a combination of these methods. These specific examples and the high dielectric functional groups that can be introduced are explained below.

In a first embodiment, the curable organopolyoxane composition comprises a curable organopolyoxane composition comprising an organic cerium compound having a high dielectric group. In the curable composition, a part or all of the reactive organopolyoxyalkylene contained in the curable composition further has a high dielectric functional reactive organopolysiloxane, and the polymer obtained by curing The specific dielectric constant of the cerium oxide elastomer is increased.

In the second embodiment, by adding an organic germanium compound having a high dielectric group to the curable organopolyoxane composition, the specific dielectric constant of the polyoxyxene elastomer obtained by curing has Increased. An organic cerium compound having a high dielectric group can be added separately from the component for curing in the curable composition.

In a third embodiment, an organic compound having a high dielectric group and a functional group reactive with a reactive organic polyoxyalkylene contained in the curable composition is added to the curable organopolyoxane composition Thereby increasing the ratio of the polysiloxane elastomer obtained by curing Dielectric constant. Due to the functional group of the organic compound reacting with the reactive organopolyoxane in the curable composition, a bond is formed between the organic compound and the organopolyoxane, thereby introducing a high dielectric group In the polyoxynene elastomer obtained by curing.

In a fourth embodiment of the present invention, an organic compound which is miscible with the curable organopolyoxane composition and has a high dielectric group is added to the curable organopolyoxane composition. The specific dielectric constant of the polyoxyxene elastomer obtained by curing is increased. Due to the miscibility between the organic compound and the organopolyoxane in the curable composition, the organic compound having the high dielectric groups is incorporated into the matrix of the polysiloxane elastomer obtained by curing.

There is no particular limitation on the high dielectric group in the present invention, and the high dielectric group can increase the curable organic polycondensation by curing the present invention as compared with the dielectric property when the group is not contained. Any group of dielectric properties of the cured product obtained obtained from the oxyalkylene composition. Examples of high dielectric groups used in the present invention are listed below without limitation.

a) a halogen atom and a group containing a halogen atom

The halogen atom is not particularly limited, and the halogen atom is exemplified by a fluorine atom and a chlorine atom. A group containing a halogen atom may be selected as an organic group having one or more types of atoms selected from a fluorine atom and a chlorine atom, such as an alkyl group substituted by a halogen, an aryl group substituted with a halogen, and An arylalkyl group substituted with a halogen. Specific examples of the organic group containing a halogen include, but are not limited to, a chloromethyl group, a 3-chloropropyl group, a 3,3,3-trifluoropropyl group, and a perfluoroalkyl group. By introducing such groups, it is also contemplated to improve the release properties of the compositions of the invention and the cured products obtained from the compositions.

b) a group containing a nitrogen atom

The group containing a nitrogen atom is exemplified by a nitro group, a cyano group (for example, a cyanopropyl group and a cyanoethyl group), a decylamino group, an imido group, a urea group, a thiourea group, and an isocyanate group.

c) a group containing an oxygen atom

The group containing an oxygen atom is exemplified by an ether group, a carbonyl group, and an ester group.

d) heterocyclic groups

The heterocyclic group is exemplified by an imidazole group, a pyridyl group, a furan group, a pyran group, a thiophene group, an anthraquinone group, and a complex of such groups.

e) boron-containing groups

Boron-containing groups are exemplified as borate groups and borate groups.

f) phosphorus-containing groups

Phosphorus-containing groups are exemplified by phosphine groups, phosphine oxide groups, phosphonate groups, phosphite groups, and phosphate groups.

g) sulfur-containing groups

Sulfur-containing groups are exemplified by thiol groups, thioether groups, anthracene groups, anthracene groups, thioketone groups, sulfonate groups, and sulfonamide groups.

The curable organopolyoxane composition of the present invention may comprise an additive typically incorporated into an organopolyoxane composition. Any additive such as a curing retarder (curing inhibitor), a flame retardant, a heat resistance improver, a colorant, a solvent or may be blended as long as the object of the curable organopolyoxane composition of the present invention is not impaired. And so on. If the curable organopolyoxane composition is an addition reaction curable organopolyoxane composition, the curing retarder (curing inhibitor) is exemplified by, but not limited to, an alkyne alcohol, for example, 2 -methyl-3-butyn-2-ol, 3,5-dimethyl-1-hexyn-3-ol, 2-phenyl-3-butyn-2-ol or the like; an enyne compound, For example, 3-methyl-3-penten-1-yne, 3,5-dimethyl-3-hexene-1-yne or the like; and benzotriazole. The concentration of the curing retarder (curing inhibitor) is preferably in the range of 1 ppm to 50,000 ppm with respect to the total composition (by mass).

Hybridization can be carried out by combining the curable organopolyoxane composition for a converter of the present invention with a polymer other than the organopolyoxane, as long as the object of the present invention is not impaired. By intermingling the organopolyoxane with a polymer having a higher dielectric constant than the organopolyoxane, the dielectric constant of the composition of the present invention and the cured product obtained from the composition can be increased. Hybrids encompass so-called polymer blending of organic polyoxyalkylenes with non-organic polyoxyalkylene polymers and fusion polymers formed by bonding organopolysiloxanes to other polymers (also known as so-called fusion polymers) Copolymer).

The curing type of the curable organopolyoxane composition of the present invention may be condensation curing, addition curing, peroxidation curing or photocuring, however, the addition curable organopolyoxane composition is preferred. In this curable system, an acrylic group, a methacrylic group, an epoxy group or a thiol group can be introduced into the curable organopolyoxane composition according to the method of introducing the above-mentioned dielectric functional group. The organic polyoxane is in the molecular chain. In addition to the addition curing reaction, a photocuring reaction or an electron beam curing reaction may also be used by using the photocurable portion or the electron beam curable portion. When such a combination reaction is used, a compound called a monomer and/or an oligomer (for example, a (meth) acrylate and a polyfunctional (meth) acrylate compound) which can be cured by light or electron beam can be used. Further added to the curable composition. In addition, a so-called photosensitizer can be added.

When a dielectric polyoxyxene elastomer as a member of a converter obtained by at least partially curing the curable organopolyoxane composition of the present invention is hot molded into a 2.0 mm thick sheet, it has the following columns It is shown as a mechanical property measured based on JIS K 6249.

(1) The Young's modulus (MPa) at room temperature can be set in the range of 0.1 MPa to 10 MPa, and particularly preferably in the range of 0.1 MPa to 2.5 MPa.

(2) The tear strength (N/mm) at room temperature may be set to not less than 1 N/mm and particularly preferably not less than 2 N/mm.

(3) The tear strength (MPa) at room temperature may be set to not less than 1 MPa and particularly preferably not less than 2 MPa.

(4) The elongation at break (%) may be set to not less than 200%, and is particularly preferably in the range of 200% to 1,000% from the viewpoint of the displacement amount of the converter.

The dielectric polyoxyxene elastomer as a member of the converter obtained by curing the curable organopolyoxane composition of the present invention has the dielectric properties listed below.

(1) When the curable organopolyoxane composition is thermoformed into a 0.07 mm thick sheet, the dielectric collapse strength (V/micron) can be set to not less than 20 V/micron. Although the preferred dielectric breakdown strength will vary depending on the application of the converter, the dielectric breakdown strength is particularly preferably in the range of not less than 30 V/micron.

(2) When the curable organopolyoxane composition is hot-molded into a 1 mm-thick sheet, the specific dielectric constant measured at a measurement frequency of 1 MHz and a measurement temperature of 23 ° C can be set to not less than 3.0. . Although the preferred specific dielectric constant will vary depending on the desired form of the dielectric layer and the type of converter, a preferred range of specific dielectric constants under the above-described measurement conditions is not less than 5.0.

The curable organopolyoxane composition of the present invention can be produced by an extruder or a kneader (more specifically, at least one type of mechanical component selected from the group consisting of: twin screw In the extruder, twin-screw kneader and single-leaf extruder, the organic polyoxane component, the curing catalyst, and the dielectric constant of dielectric constant of not less than 10 at 1 kHz and room temperature are kneaded. Particles and optionally at least one type of inorganic particulates and other additives. Specifically, in the present invention, it is possible to knead a reactive organopolyoxane component, a dielectric inorganic fine particle, and a surface treatment agent by using a twin-screw extruder having a free volume of at least 5,000 (L/h). The curable organopolyoxane composition is preferably produced by forming a polyoxyxylene rubber compound (masterbatch) comprising a high concentration (for example, at least 80% by mass) of inorganic fine particles and then adding and kneading Other reactive organopolyoxyalkylene components, curing catalysts, and other components form a curable organopolyoxane composition.

The inorganic fine particles are sufficiently dispersed at a high concentration in the curable organopolyoxane composition obtained by the above production method, and thereby a member of a converter having good electrical characteristics and mechanical characteristics can be produced. In addition, a uniform film-like cured product can be obtained during the generation of the member of the converter, the obtained film-like cured product is excellent in electrical characteristics and mechanical properties, and excellent in handling ability for lamination or the like.

In the above kneading process, a polysulfide rubber compound (masterbatch) containing no curing catalyst The temperature during formation does not impose a specific limit. However, this temperature is set in the range of 40 ° C to 200 ° C and can be set in the range of 100 ° C to 180 ° C. In a continuous process using a twin-screw extruder or the like, the residence time during the treatment can be set to about 30 seconds to 5 minutes.

Owing to the dielectric properties and mechanical properties of the electroactive polyoxosiloxane obtained by curing or semi-curing the curable organopolyoxane composition of the invention, it can be used particularly advantageously as being selected from the group consisting of The components of the group converter: artificial muscles, actuators, sensors and power generation components. In particular, after molding the curable organopolyoxane composition into a sheet or film-like shape, the member can typically be cured by heating, by high energy beam irradiation, or the like. Although no particular limitation is imposed on the method for molding the curable organopolyoxane composition into a film-like shape, the method is exemplified as a method of curing by using a conventional coating method known in the art. The organopolyoxane composition is applied to the substrate to form a coating film, which is molded by passing the curable organopolyoxane composition through an extruder equipped with a slit of a desired shape, or the like.

The thickness of the film-curable organopolyoxane composition of this type can be set, for example, in the range of from 0.1 micron to 5,000 microns. Depending on the coating method and the presence or absence of a volatile solvent, the thickness of the cured product obtained can be made thinner than when the composition is applied.

After the film-form curable organopolyoxane composition is produced by the above method, the curable organopolyoxane composition can be subjected to thermal curing, room temperature curing or high energy beam irradiation curing, and simultaneously The electric or magnetic field is applied to the target orientation direction of the electro-chemical particles, or after the filler is oriented by applying a magnetic field or an electric field for a fixed period of time. Although no particular limitation is imposed on the conditions during each curing operation or each curing operation, if the curable organopolyoxane composition is added to the curable organopolyoxane composition, curing is preferred. It is carried out in the temperature range of 90 ° C to 180 ° C by staying in this temperature range for 30 seconds to 30 minutes.

No specific limitation is imposed on the thickness of the polyoxynene elastomer used for the converter, and is thick The degree can be, for example, from 1 micron to 2,000 microns. The polyoxyxene elastomers for converters of the present invention may be stacked in one or two or more layers. In addition, an electrode layer may be provided at both tips of the dielectric elastomer layer, and a configuration in which the converter itself is composed of a plurality of stacked electrode layers and a dielectric elastomer layer may be used. The thickness of the polyoxyxene elastomer for the converter of each of the single layers may be from 0.1 micron to 1,000 microns. If the layers are stacked in at least 2 layers, each single layer may have a thickness of from 0.2 micron to 2,000 microns.

Although no particular limitation is imposed on the formation method of the two or more types of the polyoxysiloxane elastomer-cured layer, any of the following methods may be used: (1) by coating a curable organic layer on a substrate. After the polyoxyalkylene composition is cured and cured to obtain a cured layer of the polyoxyxene elastomer, a curable organopolyoxane composition is applied on the same cured layer to repeat coating and curing, thereby stacking the layers; (2) Stacking the curable organopolyoxane composition on the substrate in an uncured or semi-cured state, and curing all of the various curable organopolyoxane compositions coated in a stacked manner; or (3) A method of combining the methods of (1) and (2).

For example, in the present invention, it can be produced by coating a curable organopolyoxane composition on a substrate by die coating, curing to form two or more stacked polyoxynitrides. The elastomer cures the layer and then the resulting cured layer of the polyoxyxene elastomer is adhered to the electrode. For this configuration, the two or more stacked polyoxyxene elastomer cured layers are preferably dielectric layers, and the electrodes are preferably electrically conductive layers.

High speed coating can be carried out by slit coating, and this coating method has a high yield. After coating a monolayer comprising an organopolyoxane composition, the converter of the present invention having a multilayer configuration can be produced by coating a layer comprising a different organopolyoxane composition. Alternatively, it can be produced by simultaneously coating a plurality of layers containing each organopolyoxane composition.

A film-like polyoxyxene elastomer as a component of the converter can be obtained by applying a curable organopolyoxane composition to a substrate and then heating or lending at room temperature The assembly is cured by irradiation with a high energy beam, such as ultraviolet radiation or the like. In addition, when stacking a film-like dielectric polyoxynene elastomer, uncured The cured organopolyoxane composition is applied to the cured layer and then sequentially cured, or the uncured curable organopolyoxane composition can be stacked into layers and the layers can then be cured simultaneously.

Film-like polyoxyxides are especially useful as dielectric layers for converters. The converter can be formed by arranging electrode layers on both ends of the film-like polyoxynastomer. Further, the electrode layer function can be imparted by blending the conductive inorganic particles into the curable organopolyoxane composition of the present invention. Further, in the specification of the present invention, the "electrode layer" may be simply referred to as "electrode".

One embodiment of the components of the converter is a film and is a sheet or film. The film thickness is usually from 1 micrometer to 2,000 micrometers, and the film may have a single layer, two or more layers or a larger number of stacked layer structures. In addition, the stacked electroactive polyoxyxene elastomer layers may be used as a film thickness of 5 micrometers to 10,000 micrometers when used as a dielectric layer, or may be stacked to obtain a greater thickness, as may be required.

The film-like polyoxyxene elastomer layer can be formed as a member of the converter by stacking the same film-like polyoxynene elastomer, or stacking two or more types having different physical properties or pre-curing compositions. Film-like polyoxynene elastomer. In addition, the thin film-like polyoxyxide elastomer layer can function as a dielectric layer or an electrode layer. In particular, in a preferred converter member, the thickness of the dielectric layer is from 1 micron to 1,000 microns, and the thickness of the electrode layer is from 0.05 microns to 100 microns.

The converter of the present invention is characterized by having such a member of a converter produced by curing the curable organopolyoxane composition of the present invention, and the converter of the present invention may have a layer structure including, in particular, a highly stacked layer (i. The structure of two or more dielectric layers). The converter of the present invention may further have a structure including three or more dielectric layers. A converter having this type of highly stacked structure can generate more force by including multiple layers. In addition, by stacking a plurality of layers, a displacement greater than that obtained by using a single layer can be obtained.

Electrodes may be included at both ends of the dielectric layer used in the converter of the present invention. Electricity used The polar material is exemplified by metals and metal alloys such as gold, platinum, silver, palladium, copper, nickel, aluminum, titanium, zinc, zirconium, iron, cobalt, tin, lead, indium, chromium, molybdenum, manganese or the like; For example, indium-tin compound oxide (ITO), bismuth-tin compound oxide (ATO), cerium oxide, titanium oxide, zinc oxide, tin oxide, and the like; carbon materials such as carbon nanotubes, carbon nanohorns , carbon nanosheet, carbon fiber, carbon black or the like; and a conductive resin such as poly(extended ethyl-3,4-dioxythiophene) (PEDOT), polyaniline, polypyrrole or the like. A conductive elastomer and a conductive resin having a conductive filler dispersed in the resin can be used.

The electrode may include only one of the conductive materials, or may include two or more of the conductive materials. If the electrode includes two or more types of conductive materials, at least one type of conductive material can be used as the active material, and can be used as a conductive material for lowering the electrical resistance of the other electrode.

The total thickness of the dielectric layer used in the converter of the present invention can be set in the range of 10 micrometers to 2,000 micrometers (2 mm), but the total thickness can be set to a value of not less than 200 micrometers. Specifically, the thickness of each of the single layers of the dielectric polyoxyxide elastomer layer forming the dielectric layer is preferably 0.1 μm to 500 μm, and the thickness is particularly preferably 0.1 μm to 200 μm. Characteristics such as dielectric breakdown voltage, dielectric constant, and displacement amount can be improved by stacking two or more layers of the thin layers of the polyoxysiloxane elastomers as compared with the use of a single layer.

The term "converter" as used in the present invention means an element, machine or device for converting a certain type of energy into a different type of energy. The converter is exemplified as an artificial muscle and an actuator for converting electrical energy into mechanical energy; a sensor and a power generating element for converting mechanical energy into electrical energy; a speaker for converting electrical energy into sound energy, a microphone and a headphone; a fuel cell for converting chemical energy into electrical energy; and a light emitting diode for converting electrical energy into light energy.

The converter of the present invention is particularly useful as an artificial muscle, actuator, sensor or power generating component due to the dielectric and mechanical properties of the converter of the present invention. Artificial muscles are expected to be used, for example In applications such as robots, nursing equipment, rehabilitation equipment or the like. Embodiments as actuators will be explained below in the form of examples of the invention.

1 shows a cross-sectional view of an actuator 1 of an embodiment of the present invention in which a dielectric layer is stacked. In this embodiment, the dielectric layer is composed of, for example, two dielectric layers. The actuator 1 is provided with dielectric layers 10a and 10b, electrode layers 11a and 11b, wires 12, and a power source 13. The electrode layers 11a and 11b cover respective contact surfaces of the dielectric layer, and the electrode layers are coupled to the power source 13 via respective wires 12.

The actuator 1 can be driven by applying a voltage between the electrode layer 11a and the electrode layer 11b. By applying a voltage, the dielectric layers 10a and 10b are thinned by dielectric properties, and are elongated parallel to the faces of the electrode layers 11a and 11b. That is, electrical energy can be converted into force or mechanical energy for movement or displacement.

2 shows a cross-sectional view of an actuator 2 of an embodiment of the present invention in which a dielectric layer and an electrode layer are stacked. For example, according to an embodiment of the invention, the dielectric layer is composed of three layers, and the electrode layer is composed of four layers. The actuator 2 is provided with dielectric layers 20a, 20b, and 20c, electrode layers 21a, 21b, 21c, and 21d, a wire 22, and a power source 23. The electrode layers 21a, 21b, 21c, and 21d each cover respective contact surfaces of the dielectric layer, and the electrode layers are connected to the power source 23 via respective wires 22. The electrode layers are alternately connected to different voltage sides, and the electrode layers 21a and 21c are connected to the side different from the electrode layers 21b and 21d.

The actuator 2 can be driven by applying a voltage between the electrode layer 21a and the electrode layer 21b, applying a voltage between the electrode layer 21b and the electrode layer 21c, and applying a voltage between the electrode layer 21c and the electrode layer 21d. By applying a voltage, the dielectric layers 20a, 20b, and 20c are thinned by dielectric properties, and are elongated parallel to the faces of the electrode layers 21a, 21b, 21c, and 21d. That is, electrical energy can be converted into force or mechanical energy for movement or displacement.

Although the embodiment of the actuator is illustrated as an example of the converter of the present invention, when mechanical energy (e.g., pressure or the like) is applied from the outside to the converter of the present invention, a potential difference form can be formed between mutually insulated electrode layers. Electrical energy. That is, it can be used as a machine for A sensor that can be converted into electrical energy. This embodiment of the sensor will be explained below.

Figure 3 shows the structure of a sensor 3 in accordance with an embodiment of the present invention. The sensor 3 has a structure in which the dielectric layer 30 is disposed between the upper electrode layers 31a, 31b, and 31c and the lower electrode layers 32a, 32b, and 32c in a matrix-like mode. According to an embodiment of the present invention, for example, the electrode layers are arranged in a matrix mode having three columns in the vertical direction and the horizontal direction, respectively. The surface of each electrode layer that does not contact the dielectric layer 30 can be protected by an insulating layer. Additionally, dielectric layer 30 can include two or more layers of the same dielectric layer containing an organopolyoxane.

When an external force is applied to the surface of the sensor 3, the thickness of the dielectric layer 30 interposed between the upper electrode layer and the lower electrode layer changes at the application position, and the static capacitance between the electrode layers thus varies. Variety. The external force can be detected by measuring the potential difference between the electrode layers caused by the change in the static capacitance between the electrode layers. That is, this embodiment can be used as a sensor for converting mechanical energy into electrical energy.

In addition, although three pairs of opposite electrode layers sandwiching the dielectric layer are formed in the sensor 3 of the embodiment of the present invention, the number, size, layout, or the like of the electrode layers may be appropriately selected depending on the application.

A power generation component is a converter for converting mechanical energy into electrical energy. This power generating element can be applied to a power generating device, which starts with power generation by natural energy (for example, wave force, water power, water power, or the like) and power generation due to vibration, impact, pressure change, or the like. Embodiments of this power generating component will be described below.

4 shows a cross-sectional view of a power generating component 4 of an embodiment of the present invention in which a dielectric layer is stacked. In this embodiment, the dielectric layer is composed of, for example, two dielectric layers. The power generating element 4 is composed of dielectric layers 40a and 40b and electrode layers 41a and 41b. The electrode layers 41a and 41b are configured to cover one face of the respective dielectric layers that are in contact.

The electrode layers 41a and 41b are electrically connected to a load not illustrated. This power generating element 4 can change the static capacitance by changing the distance between the electrode layers 41a and 41b, thereby generating electric energy. That is, since the electrostatic field is formed by the dielectric layers 40a and 40b, the electrostatic charge sensing state is caused. The shape of the element between the electrode layers 41a and 41b changes, so that the charge distribution shifts, and the static capacitance between the electrode layers changes due to the offset, and a potential difference is generated between the electrode layers.

In the embodiment of the present invention, since the state in which the compressive force is applied in the direction parallel to the faces of the electrode layers 41a and 41b of the power generating element 4 shown in Fig. 4 (upper panel) becomes uncompressed as shown in the same figure. In the state (below), a potential difference is generated between the electrode layers 41a and 41b, and the function of the power generating element can be realized by outputting this potential difference change in the form of electric power. That is, mechanical energy can be converted into electrical energy. In addition, a plurality of components may be disposed on the substrate, and a power generating device that generates a larger amount of electricity may be constructed by connecting the plurality of components in series or in parallel.

The converter of the present invention can be operated in air, water, vacuum or an organic solvent. Further, the converter of the present invention can be appropriately sealed according to the use environment of the converter. No particular limitation is imposed on the sealing method, and this sealing method is exemplified by using a resin material or the like.

[Industrial Applicability]

The curable organopolyoxane composition of the present invention can be advantageously used in applications requiring an elastomer having excellent mechanical and electrical properties (e.g., producing a converter). The curable organopolyoxane composition of the present invention may comprise a so-called B-stage material rather than only an uncured curable composition which is partially reacted and not fully cured in a reactive organopolyoxane. State. The B-stage material of the present invention is exemplified as a material which is in a gel-like state or in a fluid state. Accordingly, embodiments of the present invention also include members in which the curing reaction of the curable organopolyoxane composition has been carried out in part, and wherein the members of the converter are in a gel-like or fluid state. Further, the member of the converter in the semi-cured state type may be composed of a single layer or a stacked layer of a film-like polyoxynene elastomer.

[Example]

The present invention will be described by way of example, and practical examples will now be given. However, it should be understood that such practices are The examples do not limit the scope of the invention. In addition, "%" below represents the mass percentage.

Practice example 1

85.35% was added to 14.22% of dimethyl methoxide (A ₂₁ ) (vinyl content of 0.23%) having a viscosity of 2,000 mPa s at 25 ° C and dimethylvinyl methoxy group terminated at both ends. Spherical barium titanate (produced by Fuji Titanium Industry Co., Ltd., HPBT-1B) having an average particle diameter of 1.0 μm, 0.356% terminated with trimethoxydecyl group at one molecule end and dimethylethylene at the other molecule end Base-terminated polyoxyalkylene (average degree of polymerization = 25) and 0.071% 1,1,3-trimethyl-3,3-diphenyl-1-carboxyindenyldioxane. After uniformly mixing using a Ross mixer, the mixture was further heated and mixed at 150 ° C for 30 minutes to obtain a polyoxyxene elastomer matrix.

To the polyoxymethylene rubber matrix, polydimethyl methoxyoxane (A ₁₁ ; SiH content: 0.015%) terminated with dimethylhydroquinone at the end of two molecules and containing dimethylhydroquinone oxygen was added. a copolymer of (CH ₃ ) ₂ HSiO _1/2 ) and phenyl decyloxy (C ₆ H ₅ SiO _3/2 ) (A ₁₆ ; SiH content: 0.66%), containing 0.67% (based on platinum) 1 , a solution of 3-divinyl-1,1,3,3-tetramethyldioxanane platinum complex dimethyl methoxide having dimethylvinyloxime at both ends And tetramethyltetravinylcyclotetraoxane was used as a reaction control agent to obtain the blend ratios shown in Table 1. The mixture was mixed until homogeneous (about 10 minutes) to obtain a polyoxyxene elastomer composition. Here, the molar ratio of all SiH functional groups to all vinyl groups (SiH groups/vinyl groups) in this polyoxyxene elastomer composition is 1.3.

Here, the mass fraction (Z) of the monovalent aromatic hydrocarbon group having 6 to 10 carbons is 0.49% with respect to all of the oxane component in the curable polyoxyxene elastomer composition; The mass fraction (W) of the organopolyoxane having a reactive group at the molecular end and having more than 200 repeating units is 85.2%; relative to all the oxane component in the curable organopolyoxane composition Reactive organopolyfluorene represented by M _a M ^R _b D _c D ^R _d T _e T ^R _f Q _g (where (a+c)/(b+d+e+f+g) has a value less than 3) The mass fraction of oxyalkylene (X) is 1.6%; an organopolyoxane having a reactive group at the end of two molecules with respect to all of the oxane component in the curable organopolyoxane composition ( Y) has a mass fraction of 98.4%; a reactive organopolysiloxane (S) (having at least two groups capable of undergoing a curing reaction in the molecule and having less than 10,000 between two groups capable of undergoing a curing reaction) Average molecular weight) to a reactive organopolyoxane (L) having at least two groups capable of undergoing a curing reaction in the molecule and two groups capable of undergoing a curing reaction The blend ratio (mass ratio: S/L) having a molecular weight of not less than 10,000 and not more than 150,000 was 1.6/98.4.

The polyoxyxene elastomer composition was press cured at 150 ° C for 15 minutes and then post cured in an oven at 150 ° C for 60 minutes. The Young's modulus, tensile strength, elongation at break, and tear strength of the obtained cured product were measured based on JIS K 6249. To measure the mechanical strength, a 2 mm thick piece was produced. The hardness A hardness of a 6 mm thick piece was measured based on JIS K 6253.

Further, the polyoxyxene elastomer composition was press-cured at 150 ° C for 15 minutes to produce a 0.07 mm thick sheet, and a dielectric breakdown voltage oil tester (i.e., PORTATEST 100A-2 manufactured by Soken Electric Co., Ltd.) was used. ) Measuring dielectric breakdown strength. Similarly, the polyoxyxene elastomer composition was compression cured at 150 ° C for 15 minutes to produce a 1 mm thick sheet, and was measured at a measurement frequency ranging from 100 Hz to 30 MHz at a measurement temperature of 23 ° C using Wayne Kerr Electronics. The LCR meter 6530P/D2 measures the dielectric constant. Among the values, the values measured at 1 MHz were used in practical examples and comparative examples. These results are shown in Tables 4.1 and 4.2.

Practical Examples 2 to 16 and Comparative Examples 1 to 2

The same procedure as in Practical Example 1 was carried out except that the addition amount and chemical structure of the crosslinking agent and the polymer were changed, or the particles listed in Tables 1 to 3 were used as needed to obtain a polyoxyethylene rubber composition. The above Z, X, Y and S/L values were calculated in the same manner. The obtained composition was heated and cured in the same manner, and mechanical strength and electrical properties were evaluated. The results are shown in Tables 4.1, 4.2 and 5. Further, in the tables, the chemical structures of the crosslinking agent and the polymer not described above are as follows.

A ₂₂ : polydimethyl methoxy oxane terminated by dimethyl vinyl oxyl at the end of two molecules

A ₂₃ : polymethylphenyl sulfoxide terminated with dimethylvinyl oxyl at the end of two molecules

A ₂₄ : polymethylphenyl sulfoxide terminated with diphenylvinyl hydroxy groups at the ends of two molecules

A ₁₂ : dimethylmethylhydroquinone copolymer terminated by a trimethyldecyloxy group at the end of two molecules

A ₁₃ : polydimethyl methoxy oxane terminated by dimethyl hydroquinone at the end of two molecules

A ₁₄ : dimethyl methoxy oxane/methyl hydrazine oxyalkylene copolymer terminated at the end of two molecules via trimethyl decyl decyloxy

A ₁₅ : polydiphenyl fluorene terminated by dimethyl hydroquinone at the end of two molecules

Reaction control agent: tetramethyltetravinylcyclotetraoxane

Pt catalyst (hydrazine hydrogenation catalyst): 1,3-divinyl-1,1,3,3-tetramethyldioxane platinum complex

As explained in Tables 4.1, 4.2 and 5, having a constituent component: a curable organopolyoxane (containing an organopolyoxane having a reactive group at two molecular terminals and having more than 200 repeating units and A curable organopolyoxane composition containing a predetermined amount of a monovalent aromatic hydrocarbon group and inorganic fine particles (having an average primary particle diameter of not less than 50 nm) provides excellent mechanical properties (represented by elongation at break) and electrical properties (Polyoxime elastomer represented by dielectric breakdown strength). In addition, the use of dielectric inorganic fine particles as the inorganic fine particles makes it possible to reduce the elastic modulus of the cured product and increase its dielectric collapse strength, and enables design of a polyoxyxene elastomer which is advantageously used in converter applications.

On the other hand, as shown in Table 5, it is difficult to simultaneously achieve a reduction in the elastic modulus of the cured product as a whole by the curing of the polyoxyxene elastomer obtained by curing the substance other than the organopolysiloxane which is curable by the present invention. And the increase in dielectric breakdown strength, which has been achieved in practical examples.

1‧‧‧Actuator

10a‧‧‧ dielectric layer

10b‧‧‧ dielectric layer

11a‧‧‧electrode layer

11b‧‧‧electrode layer

12‧‧‧ wire

13‧‧‧Power supply

Claims (22)

A curable organopolyoxane composition comprising an organopolyoxane represented by the following formula (I): R ^a _a R ^b _b SiO _(4-ab)/2 (I) wherein R ^a has a monovalent aromatic hydrocarbon group of 6 to 10 carbons, and R ^b is at least one type of monovalent functional group, with the proviso that R ^b is a group other than a monovalent aromatic hydrocarbon group having 6 to 10 carbons, wherein At least a part of R ^b is a group capable of undergoing a curing reaction, and 0 < a, 0 < b, 1.9 < a + b <2.1; and at least one type of inorganic fine particles having an average primary particle diameter of not less than 50 nm; The mass fraction (Z) of the monovalent aromatic hydrocarbon group having 6 to 10 carbons in the polyoxyalkylene is not less than 0.2% by mass and not more than 50% by mass; and all of the organopolyoxane is represented by the following formula (II) The linear organic polyoxane represented by the mass fraction (W) is not less than 50% by mass: R ¹ R ² ₂ Si(OSiR ³ R ⁴ ) _n (OSiR ³ R ¹ ) _m OSiR ¹ R ² ₂ (II) Wherein R ¹ is a group capable of undergoing a curing reaction, and R ² , R ³ and R ⁴ are each independently, identically or differently a hydrogen atom, a monovalent aliphatic hydrocarbon group having 1 to 10 carbons, and having 6 to 10 Carbon monovalent aromatic Group; and n-m system satisfy the condition 200 <n and 0 = <m = <(n / 20) of values. The curable organopolyoxane composition of claim 1, wherein the mass fraction (Z) of the monovalent aromatic hydrocarbon groups is not less than 0.5% by mass and not more than 30% by mass. The curable organopolyoxane composition of claim 1 or 2, wherein the mass fraction (W) of the linear organopolysiloxanes is not less than 75.0% by mass and not more than 99.9% by mass. The curable organopolyoxane composition of claim 1 or 2, wherein the monovalent aromatic hydrocarbon group having 6 to 10 carbons is a phenyl group. The curable organopolyoxane composition according to claim 1 or 2, wherein the at least one type of inorganic fine particles having an average primary particle diameter of not less than 50 nm comprises a dielectric constant of not less than 10 at 1 kHz and room temperature. Electrical inorganic particles. The curable organopolyoxane composition of claim 1 or 2, wherein the group capable of undergoing a curing reaction is capable of undergoing a curing reaction by a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction reaction. The curable organopolyoxane composition of claim 1 or 2, which additionally satisfies all of the compositional features set forth in [1], [2] and [3] below: [1] relative to the curable The entire organopolyoxane component in the organopolyoxane composition, the curable organopolyoxane composition containing the formula: M in an amount of not less than 0.1% by mass and not more than 10% by mass _a M ^R _b D _c D ^R _d T _e T ^R _f Q _g represents an organopolyoxane wherein the value of (a+c)/(b+d+e+f+g) is less than 3; In the above formula, M is a triorganosyloxy unit; a D is a diorganomethoxy unit; a T is a _{monoorganomethoxy} unit; and a Q is a _decyl unit represented by SiO _4/2 ; and the oxime The substituent R on each of the oxy units is a group capable of undergoing a curing reaction by a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction; [2] relative to the curable organopolyoxane The curable organopolyoxane composition containing, in an amount of not less than 75% by mass and not more than 99.9% by mass in the composition, having only a condensation reaction at the end of two molecules, is added in an amount of not less than 75% by mass and not more than 99.9% by mass. a reactive organopolyoxane which reacts, peroxidizes or photoreacts a group which undergoes a curing reaction; [3] the curable organopolyoxane composition contains: (S) having at least two capable molecules in the molecule a reactive organopolyoxyalkylene group which undergoes a curing reaction by a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction, and the reactive organopolyoxyalkylene S is in the two groups capable of undergoing a curing reaction. a reactive organopolyoxyalkylene having an average molecular weight of less than 10,000 and (L) having at least two groups capable of undergoing a curing reaction by a condensation reaction, an addition reaction, a peroxidation reaction or a photoreaction in the molecule, The reactive organopolyoxane L has a molecular weight of not less than 10,000 and not more than 150,000 between the two groups capable of undergoing a curing reaction, and the blend ratio (mass) of the component (S) and the component (L) The ratio) is 1:99 to 20:80. The curable organopolyoxane composition of claim 7, wherein the total organopolyoxane component in the curable organopolyoxane composition is as described in [1] above The weight fraction of the reactive organopolysiloxanes represented by the formula M _a M ^R _b D _c D ^R _d T _e T ^R _f Q _{g is} not more than 5% by mass. The curable organopolyoxane composition according to claim 1 or 2, wherein the group capable of undergoing a curing reaction is a group capable of undergoing an addition reaction, and the R ^b in the formula (I) is selected from the group consisting of Group of groups: a monovalent hydrocarbon group substituted with 1 to 10 carbons as appropriate (with the limitation that R ^b is a group other than a monovalent aromatic hydrocarbon group having 6 to 10 carbons), a hydrogen atom An alkenyl group having 2 to 8 carbons, an alkoxy group having 1 to 4 carbons, and a hydroxyl group, and at least a part of R ^b is selected from a hydrogen atom and an alkene having 2 to 8 carbons capable of undergoing an addition reaction. Base group. The curable organopolyoxane composition according to claim 1 or 2, wherein the organopolysiloxane comprises an organopolysiloxane having a hydrazine-bonded hydrogen atom and an organopoly group having a hydrazine-bonded unsaturated hydrocarbon group. a siloxane having a blend ratio (molar ratio) of the hydrazine-bonded hydrogen atoms and the hydrazine-bonded unsaturated hydrocarbon groups in the organopolyoxane of from 0.5:1.0 to 3.0:1.0 (矽 bond Hydrogen atom: 矽-bonded unsaturated hydrocarbon group). The curable organopolyoxane composition of claim 1 or 2, comprising at least one type of reactive organohydrogenpolyoxane, wherein the organopolyoxyalkylene has at least two hydrazone linkages in the molecule The hydrogen atom and the hydrogen atom have a weight fraction of 0.01% by weight. Up to 2.0% by weight, and at least one type of reactive organopolyoxane, wherein the number of repeating units exceeds 200, which has an alkenyl group at both ends of the molecular chain, and the weight fraction of the alkenyl group is 0.05% by weight to 5.0% by weight The composition further comprises: a hydrazine hydrogenation reaction catalyst; and a dielectric inorganic fine particle having a dielectric constant of not less than 10 at 1 kHz and room temperature. The curable organopolyoxane composition of claim 1 or 2, wherein at least a portion of the organopolyoxyalkylene is an organopolyoxane having a high dielectric functional group. The curable organopolyoxane composition of claim 1 or 2, which further comprises a compound having a high dielectric functional group (except for the organopolyoxyalkylene participating in the curing reaction). The curable organopolyoxane composition of claim 1 or 2, further comprising at least one type of inorganic particulate having an average primary particle diameter of less than 50 nm. The curable organopolyoxane composition of claim 14, wherein the at least one inorganic fine particle having an average primary particle diameter of less than 50 nm further contains reinforcing inorganic fine particles. The curable organopolyoxane composition of claim 1 or 2, wherein some or all of the inorganic microparticles are surface treated by one or more types of surface treatment agents. The curable organopolyoxane composition of claim 1 or 2, further comprising an additive for improving release properties or dielectric breakdown characteristics. An organic polyoxane cured product having a tensile elongation at break according to JIS K 6249 of not less than 200%, the product being at least partially cured as claimed in any one of claims 1 to 17. The cured organopolyoxane composition is formed. A member of a converter formed by at least partially curing the curable organopolyoxane composition of any one of claims 1 to 17. A converter comprising an intermediate layer of a polyoxyxene elastomer disposed between at least one pair of electrodes, the intermediate layer of the polyoxyxene elastomer being curable by organic polymerization according to any one of claims 1 to 17. The curing reaction or partial curing reaction of the decane composition is formed. A converter according to claim 20, wherein at least two layers of polyoxyxene elastomer are stacked. A method of producing a curable organopolyoxane composition according to any one of claims 1 to 17, the method comprising the steps of: blending at least two of at least one mechanical component selected from the group consisting of The components of the curable organopolyoxane composition: a twin-screw extruder, a twin-screw kneader, and a single-screw blade type extruder.