TW201249910A - A complex composition including an inorganic oxide particle and a silicone resin, and a transparent composite - Google Patents

Abstract

A complex composition including an inorganic oxide particle and a silicone resin of the present invention is a complex composition including (i) an inorganic oxide particle with an average dispersed particle size of from 1 nm to 20 nm, a surface of which is modified by binding to a polydimethylsiloxane skeleton polymer having one functional group at one terminal, (ii) a silicone resin and (iii) a reaction catalyst. The silicone resin includes a vinyl-modified silicone and a hydrogen-modified silicone, and the reaction catalyst includes a hydrosilylation catalyst.

Description

201249910 VI. Description of the Invention: [Technical Field of the Invention] The present invention relates to a composite composition of an inorganic oxide particle and a polycrystalline silicon resin and a transparent composite. The present application claims priority based on Japanese Patent Application No. 2011-128302, filed on Jun. ', [Prior Art] In the past, an attempt was made to combine an inorganic oxide such as a cerium oxide as a filler with a sapphire, thereby improving the mechanical properties of the resin. The method of mixing the filler with a resin is generally a method in which an inorganic oxide is dispersed in a solution containing either or both of water and an organic solvent to prepare a dispersion, and the dispersion is mixed with the resin. . By mixing the dispersion liquid and the resin by various methods, an inorganic oxide particle composite plastic in which inorganic oxide particles are used as the second phase can be produced (for example, see Patent Document). In addition, it has been proposed to adjust a coating composition or a coating film suitable for optical properties such as mechanical properties, refractive index, or transparency by coating a polymer on the surface of the inorganic oxide particles (see, for example, Patent Document 2). Among the polymer materials, since the polysulfide resin is excellent in weather resistance such as heat resistance and stagnation resistance, and is excellent in electrical properties and low toxicity, it can be widely used from cosmetic materials or medical materials to electrical and electronic materials. In recent years, the use of the ground has also focused on its transparency, and it has also been used in components requiring transparency such as a transparent sealing material for a light-emitting diode. The properties required for such a use are as follows: transparency, optical properties such as 324010 4 201249910, mechanical properties such as hardness, thermal stability such as heat resistance, and gas which inhibits the penetration of water vapor or various gases. Barrier. Conventionally, it has been proposed that a combination of a poly 7 oxygen resin and an inorganic material such as an inorganic oxide to improve optical properties or thermal stability has been proposed as follows: the oxide filament is contained in the presence of a chelating agent. A composition obtained by combining a polysiloxane (polysilxane) with a base (Patent Document 3); a composition for coating a light-emitting element obtained by combining a oxidized silk with a polyfunctional poly-Wei-Bake (Patent Document 4) A filler for a light-emitting element (Patent Document 5) obtained by coating an inorganic nanoparticle with an organic compound and then mixing σ into a phenyl group-containing cyanoxene (si ncone). [PRIOR ART DOCUMENT] Patent Document 1: Japanese Patent Laid-Open Publication No. JP-A-2005-292826 (Patent Document No. JP-A-2003-292826) Patent Document 3: JP-A-2006-316264 [Problems to be Solved by the Invention] However, conventionally, when inorganic oxide particles are to be compounded with a hydrophobic resin, the inorganic oxidation is due to the inorganic oxidation. Since the surface of the particles is hydrophilic, in particular, between the polyhydrazine resin having high hydrophobicity and the inorganic oxide particles, the polyoxyl resin and the inorganic oxide particles are separated, and there is a problem that it is difficult to recombine. In this case, the general solution is to hydrophobize the surface of the inorganic oxide particles of 324010 5 201249910, while the surface of the inorganic oxidation record disperses the surface-depleting agent, and the compatibility of the money with the = improve. However, it is difficult to sufficiently hydrophobize the surface of the inorganic oxide particles to be compatible with the money tree material, which is problematic. It is difficult to complain that the particle size of inorganic oxide particles is 2 〇nm or more, the brightness will decrease, depending on the situation, there will even be a loss of money (4). For example, in high-viscosity poly-stone resin, Even if used. The water-based molecular dispersant is still difficult to be compatible with the inorganic oxide particles: the surface of the inorganic oxide particles can be sufficiently hydrophobized, and /ρ is more a problem of the transparent dispersion of the inorganic oxide particles. ,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,, There is a problem in the resulting composite that there is a difference between a hole (P〇re) or a crack. On the other hand, when using polyfunctional polyglycol oxidization, there are restrictions on the blending of particles and poly-smoke, especially when the amount of particles is large, the occurrence of voids or chipping becomes significant. Multi-formal silk material, unreacted functional wire* Residue: The characteristics of the composite after cross-linking are prone to change over time, and the problem of poor durability is caused. ^ ' Further, when the sounding agent is used to melt the inorganic oxide particles and the polyelectrolyte, the coloring is exhibited due to temporal change or thermal deterioration: the 曰 phase is also proposed in the high refractive index filling material for the light-emitting element. In 324010 .201249910 A transparent dispersion of nano particles dispersed in methyl stupid polysiloxane which easily interacts with various organic molecules, but still cannot be transparent in low polarity dimethyl polyoxo resin Dispersed and hardened. Further, when an addition reaction type diterpene-based polysulfide is used, it is transparently dispersed in the polyfluorene oxygen before curing, but in the hardening step, phase separation occurs and whitening occurs. On the other hand, although the method of treating the surface of metal oxyhydroxide particles with modified money has been proposed, it is generally impossible to treat inorganic oxides because the modified polyglycol is polyfunctional. On the surface of the child, there is a problem that the unreacted modification will have a bad influence on the dissolution of the 4-mesh of the poly-resin. Then, in order to solve this problem, it is improved by three or three times of surface treatment (table, modification), etc., but there are problems such as steps. This month's issue is to solve the above problem. Its purpose: for: Γ: the composite composition of oxide particles and poly-stone resin and the first month of the moon, and the body of the sputum, in which the Tk is raised in refractive index, mechanical properties, and gas = Γ Inorganic gasification that maintains transparency: the sub-dispersion is in (4) bismuth, the dispersibility of the material is south, and the phase separation/whitening at the time of soil hardening is prevented. [Means for Solving the Problem] In order to solve the above-mentioned problems, the inventors of the present invention have found that the average fraction of (4) lnmwnm or less is a polydimethylsil_e backbone polymerization having an energy band at the end of the material. The material is used by the surface engineer to further combine the m-cut oxygen resin with the reaction catalyst, and the dispersion of the inorganic oxide particles of the 324010 7 201249910 to the inorganic oxide particles can greatly increase the aggregation. The present invention has been completed by maintaining the heat and the purity of the epoxy resin and maintaining the body. (4) Transparent composite of refractive index, that is, the inorganic oxide particle composition of the present invention is characterized in that it contains at least an inorganic oxide == ===: " a product; wherein the inorganic oxide is The edge material has a W functional group poly-di-polymer and is surface-modified, and at the same time, an inorganic oxide particle having an average particle diameter of 4 lnm ^ dry 2 〇 nm or less is dispersed; the poly-coin resin contains a modified poly-stone oxygen and hydrogen The (4) oxygen is modified; the reaction catalyst contains a hydrosilylation reaction catalyst. The polydidecyl oxynphthene backbone polymer is monoglycidyl ether terminal polyfluorene-based oxygen. The alkane and / bis- acetophenone terminal polydimethyl methoxy oxane are preferred. 3 The aforementioned vinyl modified poly fluorene is selected from the group consisting of ethylene dimercapto fluorene at both ends, and two terminal vinyl benzene. --dimethyl polyfluorene, terminal ethylene-phenyl fluorenyl polyoxo, two-terminal ethyl fluorene-dimethyl urethane, side chain vinyl-dimercapto fluorene, vinyl fluorene矽2 in the group of polyoxyl, fluorenyloxypolyoxyl, vinyl resin dispersion The above is preferred. 2 The hydrogen-modified polyfluorene oxygen system is selected from the group consisting of hydrogen-dimethyl polyoxalate, mercapto nitrogen-difluorenyl polyfluorene, mercapto hydrogen polyoxyl, ethyl hydrogen Polyoxygen #methylhydrogen-phenylmercaptopolyoxyl, hydride resin (hydride r*esin;)~ 324010 201249910 One or more of the groups are preferred. The aforementioned argon-modified polyfluorene: Polyoxyl oxide contains a side chain gas modified R3 下述 as shown by the following formula (丨): only 4 —Si — 0—Si—〇—Si—〇

Rs

V

Hi

Ri

Re

Si—R7 IRe mn (except that 匕 to Rs are arbitrary organic groups independently of each other (except H), melon is an integer of 1 or more, and η is a positive integer containing ruthenium) in the aforementioned side chain hydrogen-modified polychlorite, The ratio (m/(m+n)) is preferably 1 or more. The transparent composite of the present invention is characterized in that the inorganic oxide particles passing through the surface are bonded to the surface of the inorganic oxide particles by a combination of a polyfunctional group having one functional group at the unilateral terminal, and the average dispersed particle diameter is 纟lnm or more and 2〇. The method of dispersing in the form of the coffee is dispersed in the polyoxo oxy-resin, and at the same time, the polyester contains a ruthenium hydrogenation catalyst. The transparent composite of the present invention is characterized in that the composite composition of the inorganic oxide particles of the present invention and the polyoxyloxy resin is formed into a predetermined shape or formed by curing the composite composition. . The invention of the composite composition of the inorganic oxide particles and the oxygen-containing resin of the invention has the following steps: the step of: forming the inorganic oxide particles to have a functional group at the unilateral end The base-wei-burning bone-drying polycondensate is used to obtain a surface-modified average particle size of 1 nm to 324010 9 201249910 and the steps of modifying the inorganic oxide particles; and the aforementioned surface particles, ^ The effect of the mixing step L of the dispersed particle size of 1 nm or more and 2GnraJ" under the inorganic oxidation of the cerium oxide resin mixed with the reaction catalyst], the composite composition of the inorganic oxide particles and the polyphenol resin of the present invention> Oxidation age, material oxygenation and reaction catalyst; can 'the inorganic oxidized age is a combination of unilateral ends with i-poly-methyl-Xi Oxygen backbone polymer and surface-modified, while flat 2 Inorganic oxide particles of 1 nm or more and 2 Gnm or less in the grain county; the poly resin contains ethylene-like (tetra) oxygen and hydrogen-modified material oxygen; and the reaction touches 3 with a hydrogenation reaction catalyst. Thereby, the dispersibility of the aggregated inorganic oxide particles can be greatly enhanced. In the case of using the composite composition, when the inorganic oxide particles are combined with the polyoxynoxy resin, the dispersibility is high, and phase separation/whitening at the time of curing can be prevented, so that transparency can be maintained. A transparent composite that has heat resistance and light resistance and controls refractive index. According to the transparent composite of the present invention, the surface-modified inorganic oxide particles are bonded to each other by a polydimethyl fluorene-based oxygen polymer having a singularity at the unilateral end, and the average dispersed particle diameter is 1 ηηη or more. The polyfluorene resin is dispersed in a manner of not more than 2 nm, and at the same time, a wonderful hydrogenation reaction catalyst is contained in the polyfluorene oxide resin. Thereby, a transparent composite of the inorganic oxide particles and the polyoxygen resin which maintain the transparency, the heat resistance and the light resistance and which suppress the refractive index can be easily obtained. The transparent composite according to the present invention is obtained by molding and solidifying the composite composition of the inorganic oxide 201249910: granule: f oxiran resin of the present invention, and curing the composition into a predetermined form. Thereby, "steep, heat resistance and light resistance and suppressing the refractive index of the organic oxide particles and the transparent composite of the oxygen resin. [Embodiment] Compound == Composite resin of inorganic oxide particles and poly-gel The filler material is compatible with the dispersion of the inorganic oxide particles suitable for maintaining transparency as a guide, when dispersed in the H resin; and can prevent phase separation during hardening/white = oxide particles and polylith a composite composition of an oxygen resin; and a transparent composite obtained by molding and solidifying L and a compound. X. The inorganic oxide particles of the present invention and (4) an oxygen resin, a composition, and a transparent composite The present invention is not limited to the scope of the invention, and is not intended to limit the scope of the invention, and may be added or omitted without departing from the scope of the invention. Replacement and other changes. [Composite composition of inorganic oxide particles and polyoxyloxy resin] The composite composition of the inorganic oxide particles and the material oxygen resin of the present embodiment (hereinafter also referred to simply as The "composite composition" is a composite composition obtained by dispersing an inorganic oxide particle knife into a polyoxo oxy-resin, and is a composite composition containing at least inorganic oxide particles, a polyfluorene oxide resin, and a reaction catalyst. Wherein, the inorganic oxide particles are surface-modified by combining a polydi-f-decyloxane backbone polymer having a functional group at the unilateral end, and an average of 3,240,010 11 201249910 has a dispersed particle diameter of 1 nm or more and 20 nm or less. Inorganic oxide particles. Here, the "composite composition" does not have a specific shape, but has an irreversible deformability that does not return to its original shape upon temporary deformation, and is a raw material of a transparent composite to be described later. The state of the composite composition is, for example, a liquid state showing a liquid state or a thixotropic property. The inorganic oxide which is a component of the inorganic oxide particles is not particularly limited, and examples thereof include oxides of non-metal elements such as Shi Xi (Si); junctions (zr), titanium (Ti), aluminum (A1), and iron ( Fe), copper (Cu), zinc (Zn), gamma (γ), sharp (Nb), molybdenum (Mo), indium (In), tin (Sn), surface (Ta), crane (W), wrong ( An oxide of a metal element such as Pb), silver (Bi), garnish (Ce), ruthenium (Sb), or (Ge). Examples of such an inorganic oxide include, for example, oxidization (Zr〇2), titanium oxide (Ti〇2), oxidized stone (Si〇2), alumina (Al2〇3), and iron oxide (Fe2〇3, FeO, Fe3〇4), copper oxide (CuO, CU2O), zinc oxide (zn〇), oxidized (Y2〇3), oxidized sharp (Nb2〇5), molybdenum oxide (M〇〇3), indium oxide ( In2〇3, ImO), tin oxide (Sn〇2), oxidation group (Ta2〇s), tungsten oxide (w〇3, w2〇5), oxidation error (Pb〇, Pb〇〇, yttrium oxide (Bi2〇) 3), yttrium oxide (Ce〇2, Ce2〇3), yttrium oxide (Sb2〇3, Sb2〇5), yttrium oxide (Ge〇2, yttrium), etc. β is also included in such inorganic oxides. A composite oxide such as indium tin oxide (ΙΤ0: IndiumTinOxide) and yttria (γδΖ: Yttria Stabilized Zirconia) which is stabilized by yttria is added. Such an inorganic oxide may be used alone or in combination of two or more. In particular, when the composite composition with the polyoxin resin is subjected to a high refractive index of 324010 12 201249910, the immortal has a high refractive index and is colorless and transparent to visible light, and It is suitable for the oxidative error (Zr〇2) or titanium oxide (Ti〇2) of the yttrium. In addition, when the composite composition with the polyoxin resin is reduced in refractive index, for example, hollow two is used. Oxide particles or multiple particles in the particle (4) are available _ so that the particle bribe becomes a low-profile ^ oxide particle is better. The average dispersion of the inorganic oxide particles in the composite composition is It is preferable that Imn is not more than 20 nm, and the average dispersed particle diameter is more preferably _: 10 nm or less. Here, the reason why the average dispersed particle diameter of the inorganic oxide particles is limited to _ or more and 20 or less is as follows. When the average dispersed particle diameter is less than 1 nm, the primary particle diameter of the particles constituting the particles is not less than 1 nm, and is extremely small. Therefore, the crystallinity of the inorganic oxide particles is lacking, and it is difficult to exhibit particle characteristics such as refractive index. On the other hand, when the average dispersed particle diameter exceeds 2 () nm, the influence of Rayleigh scattering of the inorganic oxide particles becomes large, so the transparency of the composite composition may decrease, or the composite may be compounded. The composition obtained by forming/curing The transparency of the composite is lowered by 0. Since the inorganic oxide particles are nanoparticles having a size of nanometers, the composite composition obtained by dispersing the inorganic oxide particles in the polyoxynoxide resin or In the transparent composite formed by molding/curing of the composite composition, the light scattering is small, and the transparency of the composite composition or the transparent composite can be maintained. The content of the inorganic oxide particles in the composite composition is 1 324010 13 201249910 = above and 90% by mass or less is better 'better is 5 or more and 9 〇 straight /. Hereinafter, it is more preferably 10% by mass or more and 85% by mass or less. Against pi this. The content of the inorganic oxide particles is limited to 1% by mass or more. t(10) is determined by (4). The content rate is not too high. "The amount of particles will be too small. When the inorganic oxide particles are combined with the yoke oxygen, it is difficult to present the optical properties or the machine of the oxygen resin: the result is that the inorganic oxide particles can not be compounded. When the content of the surface is more than 90% by mass, the dispersibility of the machine oxide particles or the decrease in the composition of the composite composition deteriorates the formability, which is not preferable. Secondly, for the surface of the inorganic oxide particles, it is repaired by one side = one. The surface modifier composed of the oxygen compound backbone polymer has a polydimethyl bond having a poly bond and a straight bond, especially in the surface. The main one has two == combined with the shape of the inorganic oxide particles (away from the shape of the inorganic oxygen-conducting m-drying special _ to the outer surface of the particle). High, and the affinity of the dry part and the poly-stone The surface composed of the compatibility of the oxygen resin;::::: The dimethyl backbone polymer is uniformly dispersed in the inorganic oxide particles of the polyoxo tree β, and the oxygen can be formed into a good t' Composite composition. 324010 201249910 A two-linear poly 2 Silicon oxide backbone alkoxy group "is a complex in - methyl: unbranched backbone bet on (differences) means. τ is --- a branch in the polydimethyl (tetra) burnt bone (differential $ 疋 belongs to the polar group of the functional group is located in the difference) or the heart knife will be easy to face the inorganic oxide particles, the surface of the particle parallel When the amount is 2, 朝向, the compatibility between the outer side of the inorganic oxide and the inorganic oxide oxide particles氧 氧 烧 骨 彼此 或 或 或 或 或 或 或 或 或 彼此 彼此 彼此 彼此 彼此 彼此 ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ ^ In the combination, the base, Bu will not have the same function as the two: == functional unreacted residual, and the raw "/ Lu Yue 4 Shi Xi milk burning, due to, for example, white clouding; The compatibility of the polyoxin oxy-resin is 4复合' can be a stable composite composition. Such a surface modifier is a diterpene base and/or a monoterpene: the early end of the cluster is from your field. It is better to dip the U-methane oxime-methyl oxane. The amount of glycerin in the middle of the month is preferably 500 to 10,000. : The end of the knives of the stalks of the stagnation of the stalks of the scorpion (4) Wei, the singularity of the singularity of the sulphuric acid in the molecule (4) is preferably from 500 to 10,000. Among the end groups of these surface modifiers, the monoglycidyl mystery 324010 15 201249910 The end is bonded to the hydroxyl group on the surface of the inorganic oxide particle by ring-opening the epoxy group which is part of the glycidyl group, and the monohydroxy ether end is made by the terminal hydroxyl group and the inorganic group. The surface of the oxide particles is dehydrated and condensed and combined. The surface modification of the mono-glycidyl fine-end polydimethyl oxalate is not contained in the original, and the mono-cluster polydimethyl Oxygen will only have a radical in the functional group bonded to the inorganic oxide particles. Therefore, in the any-surface modifier, after binding to the surface of the inorganic oxide particles, there will be no radical or a radical. The vicinity of the surface of the inorganic oxide particles does not hinder the state of being compatible with the oxygen-containing resin. Further, the surface is modified by the surface modifier: the composite of the inorganic oxide particles and the polyoxy 7 resin The transparent composite obtained by the product has a small shrinkage ratio, whereby pores or chipping in the transparent composite do not occur, and the polycondensation of the inorganic oxide particles in the oxygen resin is also ensured. ...good's to obtain a defect-free transparent composite. The official inorganic oxide particles have a unilateral end with 1 聚 夕 氧 oxygen tree π η μ. The city surface is modified, so the tree is known, its phase It is excellent in solubility or dispersibility. Therefore, there is no special limitation on the fat itself. 1 矽 Oxygen tree is used without any problem. 〃 ^(4) (4) The gas tree is difficult, and it can be used at room temperature (25t) or higher. And the use of the hardened material 矽 hydrogenation reaction 150〇c Tejia's such a poly-resin resin is suitable for the poly-xyloxy group of the sulphonic acid. The poly-xylene and gas-modified 324010 16 201249910 The polyoxyl oxyhydroxide may be exemplified by two terminal vinyl groups, dimethyl mercapto oxygen, two terminal ethylene diphenyl dimethyl poly oxalate oxygen, two terminal phenyl methyl poly fluorene, and two Terminal vinyl-diethyl polyoxo, side bond ethyl thiol-dimethyl polyoxyl, vinyl Poly silicon oxide group, a vinyl group ▼ stone Xi = oxygen, vinyl resin dispersions and the like. These vinyl modified polysiloxanes may be used in combination of one or two types, and may be used in combination of two or more. & Hydrogen-modified polyfluorene can be exemplified by hydrogen-dimethyl polyfluorene at the two ends, methyl hydrogen-dimercaptopolyoxyl, sulfhydryl hydrogen polyfluorene, ethyl hydrogen polyfluorene, methyl^ - Phenylmethyl polysulfide, hydrazine resin, etc., may be used in combination with two or more types of hydrogen-modified polysulfide. In the hydrogen-modified poly-wei, it is preferred to contain a side chain chlorine-modified polyoxane represented by the following formula (1):

Ra Η R4— Si — 〇 — Si Ο R5

Ri m ISi-I Ri 0 n

ReI Si-I Re R7 (1) is (only, 匕 to r8 are arbitrary organic groups independently of each other (except H), m is an integer on i, and η is a positive integer containing 0). Here, the reason why the side chain hydrogen-modified polychlorite is preferred is that when the vinyl group is polymerized and hardened by a hydroxylation reaction or the like, and (4) oxygen tree filament is formed, Compared with the oxygen (4) oxygen, the reactivity is higher, and the progress is further improved. Because the amount of hydrogen modified polyoxane which belongs to the reactive group can be more, the crosslinking density becomes higher, and the result can be obtained. Ju Shi Xi 3240011 17 201249910 Characteristics of oxygen resin polymer. Further, in the side chain hydrogen-modified polyfluorene oxygen represented by the above formula (1), the ratio of m to n (ra/(m+n)) hX G.25 or more and 1 or less is preferable. The ratio (in / (m + n)) is preferably 30 30 or more and 〇 · 7 〇 or less. Here, the reason why the ratio of m to η (m/(m+n)) P is 〇. 25 or more and 1 or less is as follows. First, when q 25 is not used, since the crosslink density at the time of hardening is too small, the aggregation/phase separation speed of the inorganic oxide particles becomes faster than that of the polyoxyl resin, and as a result, it hardens with the polyoxyl resin. It loses transparency. The ratio of 'm to n' (m/(m+n)) is the upper limit of 1, but the larger the ratio of m to η (m/(m+n)), the following formula (2) The content of the hydrogen-containing unit will become higher: Η

I (2)

Si-Ο

I 13⁄4 The ratio of units unreacted with vinyl modified polyoxyl is also considered to increase after the formation of the transparent composite. However, this unreacted hydrogen-containing unit hardly affects the properties of the transparent composite. Therefore, in the side chain hydrogen-modified polyfluorene oxide, the ratio of m to n (m/(m+n)) may have a maximum value of 1. In the above formula, 匕 to R8 are any organic groups independently of each other (except H), and some or all of them are the same. Here, "a part of the same" 疋 means that not only 匕 and % are the same as R4 and Re, but 匕 and 尺 2 and Rs and R7 and Ra are different from each other, and only part of them are the same kind. 324010 18 201249910 Further, for example, 1^ is the same as R3 and R4, and R2 and 仏 are the same as R7 and Re, and R, and R2 and Re are mutually different combinations of the same. In addition, the "organic group" is an all-group including an organic group, a functional group, a substituent, and the like, and includes, for example, an alkyl group or an alkoxy group. In the polyoxyxene resin, the properties of the composite composition which is mixed with the inorganic oxide particles or the like are irreversible deformability which does not return to the original shape upon deformation, as long as it does not have a specific shape. The raw material to be a transparent composite to be described later may be, for example, a liquid or a thixotropic gel, and the degree of polymerization is not particularly limited. In other words, the composite composition may be any of a monomer, an oligomer (a polymer of about 2 to several hundreds), and a polymer (a polymer of several hundreds or more) as long as it has the above characteristics. In order to combine these, the degree of polymerization has a wide range. Further, in the polyoxyxylene resin, an antioxidant, a release agent, a coupling agent, an inorganic filler, or the like may be added to the extent that the properties are not impaired. The composite composition of the present embodiment contains a reaction catalyst. The reaction catalyst is preferably a catalyst containing a hydrazine hydrogenation reaction. The hydrogenation reaction catalyst may be a noble metal catalyst, and a powder of a noble metal, a metal salt, a noble metal complex or the like may be appropriately selected. The noble metal-based catalyst is preferably a platinum-based catalyst. Examples thereof include a platinum-based catalyst, a ruthenium-based catalyst, and a palladium-based catalyst, and particularly a platinum-based catalyst. The platinum-based catalyst may be, for example, a platinum micropowder, a chlorinated acid, a sulphuric acid, a sulphuric acid, or a sulphuric acid compound. These may be used alone or in combination of two or more. 324010 19 201249910 The composite composition of the present embodiment may contain an organic solvent. Here, the advantages of the composite composition containing an organic solvent are discussed. Further, the first advantage is proposed, and for example, it is possible to control the adhesion of the composite composition. When the mixture of the inorganic oxide particles and the (IV) oxygen resin is as high as 'the fluidity is deteriorated' and the formability of the transparent composite described later occurs, the problem of the ease of the treatment is lowered. Here, the solution is lowered or In this case, the problem can be lowered to the desired viscosity by adding an organic solvent to the mixture. Inorganic oxide particles = point of matter The viscosity of the mixture of fats is at 0. 05Pa· 3 to the eve of the tree is better.  IPa · s to l〇OPa.  s. a · s is preferable, and the second advantage is, for example, inorganic oxide particles modified by an easy-mixing/dispersing surface modifier, and the surface-mixed polyoxo-oxygen resin is an organic solvent having high compatibility =/, It is preferable to use the sub-dispersion and the inorganic oxide particles to make the inorganic oxide particles, since the inorganic oxide particles are very oriented for the two. = The solvent is preferably a hydrophobic solvent. The reason for this is that the dispersibility of the surface-modified inorganic oxide is a solvent having high compatibility with the polyoxymethylene resin. Such a hydrophobic solution (IV) can be suitably used, for example, as stupid, toluene, or two: two basic isobaric hydrocarbons; methylene chloride, gas, carbon tetrachloride, etc., so that ^ #solvering can be used alone or Two or more kinds of 324010 20 201249910 are mixed, and the content of the organic solvent is not particularly limited as long as it is obtained by the above-mentioned solvent addition and the effect, but usually with respect to the surface-treated inorganic oxide particles and polystones The total amount of the epoxy resin is preferably 4% by mass or less. The content of the organic solvent is preferably at most 1% by mass. The reason for this is that if the organic solvent is excessively present, when the composite composition is used to form a transparent composite described later, the viscosity is too low, and it is difficult to form moldability, or it takes time to remove the organic solvent, which is not preferable. [Manufacturing Method of Composite Composition] The method for producing a composite composition of the present embodiment is the following method: First, the surface of the inorganic oxide particles has a polydimethyl siloxane skeleton having a base at one end The polymer is modified to form an inorganic oxide particle having a surface-modified average particle diameter of Inm or more and 2 〇 nm or less. Next, the surface-modified average particle diameter of the inorganic oxide is 1 ηηη or more and 20 nm or less. Particles, polyoxin, and a method of mixing with a reaction catalyst. The method of modifying the surface of the inorganic oxide particles by a poly-methyloxo-calcined polymer having one S-th b-group at the unilateral end can be exemplified by the following methods. In other words, a method in which a specific dispersing agent is previously bonded to the surface of the inorganic oxide particles to disperse the hydrophobic solvent (organic solvent dispersibility) is described. The particles are dispersed in a hydrophobic solvent to obtain a dispersion liquid. Next, in the obtained Kawasaki liquid, a surface modifying agent composed of a poly-dry polymer having a functional group at the unilateral end is added thereto, and a hydrophobic hydrazine is added thereto. In the agent, a specific component of the surface of the inorganic oxide particles is bound to 324,010, 201249910, and a surface modification consisting of a backbone polymer having a unilateral end: a dibasic group: a poly-methyl group, The surface of the method is such that the specific dispersant is first bound to the inorganic oxide particles, and the dispersibility to the hydrophobic solvent is obtained. The inorganic oxide particles of the Shuyongding dispersant are easily dispersed in the above-mentioned table, at: a polydimethyl oxy-combustible bone granule having one functional group at the end of the inorganic oxygen-dry hydrazine combined with the specific dispersing agent; = a surface modifying agent constituting the coexistence of the above-mentioned inorganic For the specific dispersant to be combined with the specific dispersant, the organic acid compound or the organic base compound can be exemplified. The β-acid compound can be exemplified by hydrazine, acid, lysine, etc. Known, phosphazene base, etc. 〇 In these dispersants, 'the carboxylic acid or amine is suitable because the function of the dispersant which disperses the inorganic oxide particles is exhibited by The surface modifier can be well detached in the reaction. For the carboxylic acid, 'as long as the saturated fat is used from formic acid, acetic acid, butyric acid, pentamidine, caproic acid, heptanoic acid, caprylic acid, citric acid, lauric acid, stearic acid, etc. And one or more of the unsaturated fatty acids such as oleic acid may be selected. Further, for the guanamine, for example, pyridine, bipyridine or the like, diethylamine, diethylamine, and monoethyl byanide may be selected and used. One or two or more kinds of aliphatic amines such as a base amine and a butylamine may be selected. Next, the inorganic oxide particles 324〇1〇22 201249910 having a specific dispersing agent bonded to the surface thereof are dispersed in a hydrophobic solvent. Hydrophobic dissolution In addition, as long as the inorganic oxide particles in which the surface is bonded with a specific dispersing agent can be stably dispersed, it is suitable to use aromatic fumes such as benzene, toluene, dimethyl benzene, ethyl benzene, etc. a gas-containing solvent such as a second imitation or a four-gasified carbon. In these solvents, two kinds of ruthenium species can be used, and the inorganic particles in which the surface is combined with a specific dispersant are dispersed, and the former is coated. a functionalized polydimethyl-stone-oxygenated backbone polymer: a modifier that replaces the surface modifier with an inorganic oxide surface-dispersing agent. It is modified by a surface modifying agent composed of one functional group at the unilateral end. The dry poly U is a surface modifier composed of a functional dimer at the unilateral end. None: The oxygen ratio is relative to the total mass of the money oxidation record, which is ^ = and the mass % or less is preferably '10% by mass or less, preferably more than 20% by mass, and more preferably 20% by mass or more (4). Sister, the mass ratio of the surface modifier is limited to 5% by mass or more and 2曰00 is less than or equal to % _ _ surface repair _ quality 篁 ° /. When the amount of the surface modifier is too small, the surface of the proton is 5, so that the inorganic oxide particles in this table are difficult to be compatible with the poly-wei resin, and the inorganic oxide particles in the fish are clear TM. == Loss of translating when compounding <Quality ratio exceeds 2〇〇% by mass, 324010 23 201249910 The ratio of surface finishing agent in the composite composition will increase to the benefit of the law = lower = 虞 will greatly affect the compound Characteristics of the composition: ^ = "Use a surface modifier consisting of a polydactile = dry polymer with one functional group at the unilateral end, : Energy base (polarly selective to inorganic oxide particles == On the other hand, the other end side is in the shape of the hydrophobic solvent port = the outer side of the compound particle. Therefore, these two: ', the S 旎 group portion is bonded to the inorganic oxide particles, and the other is the inorganic oxide particles * In the shape of a radial shape, relative to the above, it is possible to obtain an inorganic oxide having a functional dimethyl group at the end of the county and a bone-drying polymer, and an average dispersed particle 2 of 1 nm or more and 20 nm or less. Particles. Secondly, this surface-modified flat When the inorganic oxide particles having a dispersed particle diameter of atm or more and (10) or less and the polywei resin are mixed with the reaction catalyst, an organic solvent may be added as needed. Here, the polysiloxane resin itself is not particularly limited. As long as it is a combination of a hardened ethylene group and a hydrogen-modified gas by a hydrogenation reaction, it can be used without any problem. 324〇1〇~ In the case of dilute-based modified poly-stones, it can be obtained from the two ends of the ethylene group, the fluorenyl group, the two ends, the vinyl diphenyl-dimethyl polyoxynium, and the two ends, the ethyl group, the phenyl group. Based on the dream oxygen, the two ends of the county _ diethyl poly sulphate ~, side chain vinyl - dimethyl polyoxyn, vinyl methyl polyoxyl, ethylene 24 201249910 on the dispersion of the use of a single exhaust丨 、, A 甲: 气_改甲:=言' can be obtained from both ends of hydrogen-dimethyl condensate mi-methyl polyfluorene, methyl hydrogen polymethyl hydrazine methyl phenyl-polymethyl meth Oxygen, vaporized resin, etc.: Either species or a combination of two or more. The hydrogen-reducing system is characterized by containing a side chain represented by the above formula (1). For better reasons, it is polymerized and hardened by the hydrogenation of the blood group, and the formation of polysulfide is the same as that of the hydrogen-modified (tetra) oxygen. Higher, more advanced, can make the hydrogen belonging to the reactive group change more than the polyoxygenation, so the crosslink density becomes higher, and as a result, the characteristics of the oxygen tree of the family can be improved. In the side chain hydrogen-modified polyfluorene oxygen represented by the above formula (2), the ratio ηn/(m+n) of the signal to η is 〇. 25 or more and 丨 below is preferred. The ratio (m+n) is 0. 30 or more and 〇. 7〇 or less is preferred. Here, the reason for limiting the ratio of ra to η (m/(m+n)) to 〇 25 or more is as follows. First, when the ratio of 'm to η (m/(m+n)) is less than 逹〇25, since the crosslink density at the time of hardening is too small, the aggregation/phase separation speed of the inorganic oxide particles is also higher than that of the polyoxyl resin. The hardening speed is faster, resulting in loss of transparency when hardened with the polyoxymethylene resin. Next, the ratio of m to η (m/(m+n)) is an upper limit of 1, but the larger the ratio of m to η (m/(m+n)), the one represented by the above formula (2) The hydrogen unit contains 324010 25 201249910. The higher the rate becomes, the ratio of mono-oxime which is not reacted with the vinyl modified polysulfide after the formation of the transparent complex is also considered to increase. However, this unreacted unit contains The ram complex is made with #秘秘. Therefore, in the side bond nitrogen modification, the maximum value of &quot;1 and ktt(m/(m+n)) in oxygen can be 1 〇, which will be the surface of the inorganic a mixture of oxide particles and (iv) oxygen resin. 11. Two methods can be used, such as a mixer, various grinders Ornll, plus ultrasonic waves. The inorganic oxide particles which are surface-modified by a surface modifying agent are mixed with a cardioic resin. However, in order to make the ==! decoration of the inorganic oxide particles, it is preferred to use the solvent dispersion and the cardio-oxidation oxide particles for the use of the (10)^ filter. , the inorganic oxide particles:: _ resin in the _,: machine = = viscous polyoxyn oxy-resin in the dip - ..., machine oxide particles in the dispersion, the system: and anti-recording (four) The inorganic oxide particles in the bulk of the knife are further made of inorganic oxide particles. The step of the Lie is also a big (four) force. "When the inorganic oxide particles dispersed in the resin are temporarily dispersed in the organic solvent of the second solvent, the organic 324010 oxide particles (4) are uniformly dispersed in the organic solvent. 26 201249910 In the solvent of the machine, the inorganic oxide particle dispersion liquid having a low viscosity is formed. Here, if the dispersion liquid in which the inorganic oxide particles are uniformly dispersed is mixed with the polyoxin resin, since the liquids are mixed with each other, Even if the polyoxyxene resin has a certain viscosity, it can be uniformly mixed with the dispersion having a low viscosity, and as a result, the inorganic oxide particles are easily and uniformly dispersed in the polyoxin resin. Further, the low viscosity The step of mixing the inorganic oxide particle dispersion with the low-viscosity polyoxynoxy resin itself does not require much labor because it is a mixing step between the solutions. · If the mixture of inorganic oxide particles and polyoxygen resin which does not return U is high viscosity, the fluidity of the mixture may deteriorate, and the formability of the transparent composite described later may be lowered or the ease of handling may be improved. Falling two questions. The tree problem is that the viscosity of the obtained mixture is first lowered in the case where the mixed inorganic oxide particles and the polyoxo oxide == the dispersibility of the compound particles are high and the organic solvent of the (iv) oxy resin is used. It is preferable to use a hydrophobic solvent, for example, a content ratio of an aromatic solvent of the U-based ethyl ester to a =2, as long as it is an inorganic oxidation (4) which is obtained by adding the above solvent. The surface modification is preferably as follows. There is;; the concentration of 400% by mass of organic solvent is better than 27 201249910. The reason for this is that when the bitter organic solvent forms a transparent composite described later, it is not preferable to use the composite grade, or to require a flower to be too thin and to form a shame. Specific examples include, for example, a method in which the inorganic particles are redispersed in an organic solvent in which the particles are mixed with the polyoxo wax, and (2) the inorganic oxide particles are mixed in the liquid. A suitable organic solvent is added to the mixing mixture, and after mixing, the viscosity is adjusted by mixing, and the 劁A B+ 专 is mixed with a mixer/method of a mixture of W females and the like. The method of adding an organic solvent can also be carried out by means of an organic solvent. When the viscosity of the material becomes low, the viscosity of the line is adjusted (high viscosity). The knives are removed by volatilization or the like, and the complex S composition of the present embodiment and the [transparent composite] '" can be obtained as described above. The transparent composite of the present embodiment has a functional polydimethyl group. Shixi Oxygen is formed by combining inorganic oxide particles with unilateral ends in an average dispersion = polymer surface repairing method in a polyoxin resin: 1 nm or more and 20 servings of resin containing Shi Xi In the case of U, in the case of U, the polycene gas does not contain an organic solvent, especially a hydrophobic solution; the "transparent complex" has a p content and is extremely small. The predetermined shape "S" refers to the shape of the transparent composite ^, but this has irreversible deformability, and is used in conjunction with the shape of a liquid, a gel, or the like. Can = hold ~ difficult to hang dead without deformation of the solid, 324010 28 . 201249910 In addition, the rubbery shape and other elastic deformation properties themselves are not shown as specific shapes. ^ (Shape-recovery), in the form of a transparent composite, by increasing the degree of polymerization or cross-linking of the upper, &gt; oxyresin, or the sputum of the compound in the composite The degree of polymerization between the oxane backbones bites six to separate the shape of the resin and the surface to shape the shape. Therefore, by constituting this transparency, it is possible to obtain a polydimethyloxane backbone having a surface modifier which is preliminarily composed of a component having one bureaucratic body at the unilateral end, that is, a polymer. The inorganic oxide particles of the surface of the 3 decorative materials of the polyoxin and the reaction catalyst are the same. The knives are compatible with the above-mentioned composite composition of the yam-yellow complex, and the inorganic oxidized front-end complex of the ruthenium is modified to have the compatibility and affinity of the dispersive cup tree in the polyoxyl resin. The burden and the poly-resin resin do not occur in the phase VIII = two, thus the phenomenon of agglomeration of the inorganic oxide particles. Therefore, the inorganic oxide optical extremes do not occur in the second or second, and there is no such thing as the pre-characteristics, mechanical properties, and properties. ..., the deterioration of the literary specialty, can maintain a good time, as described above 'make this polyoxyl resin hardened by the reaction catalyst / '4 oxygen resin hardening degree, agglomeration of inorganic oxide particles No ^ fast and fast. (4) Among the transparent composites produced, the composite chemical particles do not aggregate, and the transparency is also high. Further, a composite composition which is a transparent material, which is a material which is colored in a transparent composite because it does not use a chelating agent. The average of the inorganic oxide particles contained in the 1 transparent composite is 324010 29 201249910 20 nm or less. Therefore, it is possible to suppress the occurrence of shadowing if the level exceeds 20 nm, and the transparency of the transparent blunder scattering (Rayleigh SCatteri) = the transparency of the transparent composite does not decrease. In this inorganic-inorganic gasification teacher is a nanometer-sized particle, so in the inorganic vaporized particle octagonal or transparent composite into a poly-stone resin or a composite group or The transparency of the transparent composite. The light scattering is also small, 'the composite composition can be maintained, and the transparent particle size is dispersed. The average particle size of the inorganic oxide particles in the crossbody is not the same; the above, so the inorganic oxidation The range of the particle 1 (10). As a result, the maintenance of this nature has declined. ..., the gasification particles of the machine can maintain good crystallinity === sub-crystallinity, so characteristics such as inorganic oxygenity do not deteriorate. Therefore, 'that is, the effect of the refractive index or the hardness, the heat-resistant composite, and the transparent compound 2 machine oxide particles and the poly-stone tree _:f: the effect of the resin. Oxygen resin t is about, so if the polyfluorene oxide is compounded, the refractive index of the 5 refractive index oxide particles is higher than that of the polysulfide resin alone. The letter shape can make the transparent composite especially the refractive index 2 or more high spells 324,010 refractive index inorganic oxide particles, 30 . 201249910 For example with tetragonal zirconia (refractive index: 2.  15) or titanium oxide (refractive index: about 26) composite system is effective 'by using such high refractive index inorganic oxide particles, the refractive index of the transparent composite can be increased to be higher than that of the polyoxyl resin alone 0.  1 to 0, 2 or so, can be increased to 1.  5 to L 65 or so. With regard to the transparency of the transparent composite, as described above, by setting the average dispersed particle diameter of the inorganic oxide particles to 2 〇 nm or less, the light scattering can be sufficiently suppressed. Therefore, in the transparent composite, transparency can be sufficiently maintained. Further, by having voids in the particles like hollow cerium oxide particles or porous cerium oxide particles, the particles as a whole become inorganic oxide particles having a lower refractive index than the polyoxyn oxyresin, and are compounded with polyoxyn oxyresin. Further, the refractive index of the transparent composite can be further lowered as compared with the case where the polyoxyxylene resin is used alone. ‘‘、、[Mechanical Properties] The mechanical properties of the transparent composite may be such that the hardness is further improved as compared with the case of the resin alone. In general, the inorganic oxide particles are harder than the polyoxynoxy resin by combining the inorganic oxide particles with the polyoxynoxy resin, and can be transparent compared to the case where the polyoxin alone is used. The surface hardness of the composite is further improved. Thereby, the scratch resistance of the transparent composite can be improved, and the dimensional accuracy of the transparent composite itself can be improved. In particular, cerium oxide is also high in hardness in the oxide-based ceramics, so that it can exhibit a high effect in terms of surface hardness improvement by compositing. [Thermal stability and chemical stability] 324〇i〇31 201249910 *Juxixi Oxygen Resin has heat resistance or quality compared with the resin of the pass because it contains Si Xi (Si) in the backbone. Excellent thermal stability and chemical stability. On the other hand, minus (10) her son wins in terms of heat resistance = oxygen resin. Therefore, the thermal stability or chemical stability of the obtained transparent composite can be obtained by combining the inorganic oxide particles having high chemical stability and the inorganic oxide particles having high chemical stability with the polyoxo resin. It is more improved than the case of Juqin resin alone. Here, the (IV) oxygen resin has high compatibility with a hydrophobic solvent, and is hydrophobic (water repellency), but it is rich in visibility, and the barrier property is lower than that of other resins. In the transparent composite of the embodiment, the inorganic particles having excellent gas barrier properties are scattered in the transparent composite compound = the combination of the chemical particles and the poly-resin is high, so that the gas of the money alone is Resist the secret, the remaining 1 is expected to be an oxygen resin in the early days, but can be improved to a higher state. ^Through the Japanese and the United States is suitable for the optical penetration of the inspection ^The reason: According to the = month] complex] by the high refractive index of inorganic oxide particles,! When the human is compounded with the oxy-resin, the refractive index of the obtained fluoroform can be obtained, for example, from the case of the poly-resin alone, and the hardness is due to the hardness of the oxy-resin alone. It is also possible to improve the dimensional accuracy. Thus, the degree of freedom in designing the optical element is raised. As a result, for example, it is possible to reduce the size, thickness, and integration of the collecting light 324010 32 as compared with the case where the polycrystalline stone is used alone in the optical lens. 201249910 Efficiency, reducing the dependence of the refractive index wavelength, etc. Therefore, it is possible to improve the characteristics such as high resolution or high sensitivity of a mechanical CCD or CMOS camera using such a light-emitting element. Further, this transparent composite can be suitably used as a [rib seal material belonging to a light-emitting element. The reason for this is that the transparent composite has a high refractive index as compared with the individual oxime resin. Therefore, when used as an A sealing material belonging to a light-emitting element, the illuminant covered with the sealing material can be raised or formed with = The refractive index of the semiconductor material having a high refractive index such as a substrate of the illuminant (which belongs to LE) is = 2. At about 5, the refractive index of the transparent substrate of the semiconductor material is about L76. The refractive index is integrated into this, and is internally reflected during the emission from the illuminator of the LED to the outside. In other words, by using the transparent composite of the present embodiment for the sealing material of the LED, the light extraction efficiency of the LED can be improved by about 1% to 15%, and as a result, the brightness of the LED can be improved. Further, since the transparent composite has high gas barrier property against water vapor, it is possible to suppress moisture infiltrating from the outside and to suppress deterioration of the light-emitting region. Therefore, it is possible to extend the life of the light-emitting element. Further, this transparent composite can also be suitably used as a sealing material for an organic EL element. The reason for this is that when the transparent composite is used as a sealing material for an organic EL element, since the gas barrier property against water vapor is high, moisture permeating from the outside can be suppressed, and deterioration of the pure domain can be suppressed. Further, since the inorganic oxide particles in the transparent composite can effectively suppress the penetration of oxygen, the deterioration of the light-emitting region can be suppressed similarly. Therefore, when the transparent composite of the embodiment 324010 33 201249910 is used as a sealing material for an organic EL device, the life of the light-emitting device in the organic EL device can be extended. [Method for Producing Transparent Composite] The transparent composite system of the present embodiment can be obtained by the following process: forming and curing the composite composition of the present embodiment into a predetermined shape, or curing the composite composition It is then shaped into a predetermined shape. In the production method of the present embodiment, the "method of molding and solidifying into a predetermined shape" is as follows. First, the composite composition of the present embodiment is formed by using a mold or a mold, or is filled in a mold or a frame-shaped container, whereby a molded body or a filler which is shaped into a desired shape can be obtained. In this case, when the viscosity of the composite composition to be used is high, it is preferred to first add an organic solvent or the like and stir or mix to lower the viscosity, and first adjust the viscosity suitable for forming or filling. On the other hand, the composite composition used. When the viscosity is low, it is preferred to polymerize or crosslink the polyoxynoxy resins or the polyoxyxylene resin and the surface modifier in the following manner, or when the composite composition contains an organic solvent. Some or all of the solvent is removed by volatilization or the like to increase the viscosity' and is first adjusted to a viscosity suitable for forming or filling. Next, the shaped body or the filling is directly heated at a room temperature (about 25 ° C) or to a predetermined temperature (room temperature to 15 ICC, more preferably 80 Ϊ to 15 〇. (:;) and allowed to stand for a predetermined time. A polymerization reaction or crosslinking reaction of the polyoxyxylene resin or the surface modifier in the composite composition via a reaction catalyst to increase the combination of the polyoxo resin or the polyoxo resin and the surface modifier. Degree 324010 34 201249910 (degree of polymerization). Further, the organic solvent is left in the molded body or the filler. The organic solvent is left, and the volatilization is removed, and the molded body or the filler is removed from the mold or the container. By applying an external force to it, it is also possible to maintain a shape-shaped shape energy. From the above, it is possible to obtain a composite having no defects, excellent properties, high thermal stability or chemical stability, and mechanical special migration. In the manufacturing method of the present embodiment, the method of "inspecting, forming, and molding a predetermined shape" is as follows. After the second product is cured, ☆ first, the composite composition of the present embodiment is cured. Get: the solid of the object Compound (unformed transparent composite). For curing method: s 'As long as the composite composition is directly at room temperature (about 25t) or added to the field, the temperature is set (room temperature to navigation, preferably 8吒 to 15rc) And static; 疋 time, for the composite composition of the material of the oxygen resin or surface = by the reaction (four) money to polymerize money and reaction to increase the polyglycolation month g or each of the dream milk sap and the surface modifier In addition, in the case of residual organic solvent, the organic solvent is removed by volatilization, and the cured product can maintain a certain shape even after application of an external force, and the cured product is cut or The mechanical processing of the mold is performed, such as mold release, and the opening is a necessary shape. The poly-stone oxide resin of the present embodiment is also easily cured after being cured by 324010 35 201249910. The fats are mutually processed or the polyoxynium tree. 'You can also improve the polyoxo tree or::r: machine two == 'upper valley, you can get the defect-free, optically-acceptable, learning stability':::, the fit is suitable for no See transparency as a problem area, to ensure transparency' It is not necessary to use the average fraction of the particles to be used, and to apply the m, the lower oxide, for example, to increase the surface hardness of the composite containing the inorganic oxide particles and the polyoxo oxygen as the target (4). Further, a particle larger than 2 mm, for example, a particle of the inorganic oxide particles of the (10) particle can be produced in a composite composition by applying the method for producing the composite composition of the present embodiment even in such a case. The inorganic particles have high dispersibility, and a composite composition of a molded article or a filler having good physical properties can be produced. EXAMPLES Hereinafter, the present invention will be specifically described based on examples and comparative examples, but the present invention is not limited thereto. The additions, omissions, substitutions, and other modifications of the structure may be made without departing from the spirit and scope of the invention. Example 1 In a zirconium salt solution obtained by dissolving 2615 g of zirconium oxychloride 8 hydrate salt in 40 L (liter) of pure water, '34 red red 324010 36 201249910 28% ammonia water was dissolved in 20 L of pure water. The diluted aqueous ammonia is added while mixing, and the oxidized precursor slurry is prepared. Next, in this poly-liquid, a sodium sulfate aqueous solution obtained by dissolving 3 g of sodium sulfate in 5 L of pure water is added while stirring, and the amount of sodium sulfate added at this time is relative to the zirconium salt solution. The converted value of the oxidation of the recorded ions was 30% by mass. Next, this mixture was dried in the atmosphere using a drier. Dry under the arm for 24 hours to obtain a solid. Next, this solid matter was pulverized using an automatic mortar, and then fired in the air at 500 ° C for 1 hour in an electric furnace. Then, the fired product was poured into pure water, stirred to form a slurry, and then washed with a centrifugal separator. The sodium sulfate added was sufficiently removed, and then dried in a desiccator to obtain oxidized particles. Next, 85 g of toluene and hexanoic acid 5 were added to and mixed with the oxidized hammer particles 100 g. The surface of the zirconia particles was modified by the hexanoic acid of the genus (d). Thereafter, a dispersion treatment is performed to modulate the oxygen storage and correction dispersion. In the case of the oxidized oxidized dispersion·g + , a monoglycidyl-terminated polydimer having a polydimethyl 7 oxy-oxide dry polymer having one functional end at one end is added. Silk oxide 6 (pDMS_G: number SOOOUldrich) 10 g, dilauric = surface modification under reflux. Ji Xixi. 〇 lg, after the reaction is terminated, the solvent is removed by washing and washing and centrifuging, while the argon (10) particles m should be monoglycidyl _ dimethyl benzo: 324010 37 201249910 That is to say, the surface of the oxidized silk fabric is the result of the measurement of the surface-treated oxidation record, 2·6 to 3 5dmi attached to the evening whistle m, Li Yuhuai) # 00 .  , the result of glycidyl group-induced terminal polydimethyl ketone _ terminal f - formazan, this result can be judged that 'monoglycidyl-methyl ketone-burning ring-opening and After oxidizing the wrong particles, 15 g of the surface-modified oxidized silk was redispersed to toluene, and then a side chain of the vinyl modified polyfluorene, W-131 (manufactured by GeleSt Co., Ltd.), 14 lg, was added as a gas f'-methyl group. Shi Xi oxygen .  ^ ; g gas modified poly-stone oxygen methyl ^ dimethyl _ oxygen hall - 151 (Gelest company) Q. 9g, further: into the surface of the room temperature hardening as a reaction catalyst::!IP6830-3(Gel--^&gt;-^^^u;^ 乜 轧 rolling zirconium particles-polyoxyl resin composite composition Next, the surface-modified cerium oxide particles are polycondensed, dissolved, and then poured into a mold 2 which is assembled into a glass plate to remove the money (4), and subjected to a hardening reaction to obtain a transparent composite having a thickness of 1 mm. The content of the zirconia particles of the transparent composite is Torr%. The surface of the transparent composite of the example i found is observed by a field emission electron microscope, Sheng 2 vine (manufactured by Sakamoto Electronics Co., Ltd.), and measured = The particle size of (10) particles is selected by the machine, and the average particle size of the oxidized erroneous particles which are transparently composited is averaged. The average result is 324,010 38 201249910 散 疋 7 ηηη. The conclusion is as follows: the average residual diameter of the emulsification such as the sub-composition in the composite composition of Example 1 is also ? nm or below the pot. The result of the analysis is that the transparent composite of Example 1 obtained is elemental. The score of the film is the same as the amount added as the reaction catalyst. Therefore, the transparent composites invented by the county were confirmed. Example 2 In addition to changing the cerium oxide particles from 1 Gg (25 mass%) to 14 valences and 5 mass%, respectively, it will be modified as a compound in the county. The side chain vinyl-dimethyl polyfluorene VDT-131 from 14.  Lg (47% by mass) is changed to 8.4% by mass), which will be used as a gas-modified (tetra) oxygen methyl hydrogen-dimercapto (tetra)oxy__ΐ5ΐ from 〇.  9 g (3 mass%) was changed to 〇·6 g (2 mass%), and the other was subjected to the operation of Example i to obtain the surface-modified oxidized silk _ poly 7 oxy-resin composite composition of Example 2 and the end degree was 1 ππιπ Transparent complex. The content of the cerium oxide particles in the transparent composite was 35% by mass. The particle diameter of the cerium oxide particles in the obtained transparent composite of Example 2 was measured in the same manner as in Example 1. As a result, the average dispersed particle diameter was 8 nm. From the results, it was concluded that the average dispersed particle diameter of the oxidized oxide particles in the composite composition of Example 2 was also 8 ηηη or less. Further, as a result of elemental analysis of the obtained transparent composite of Example 2, the platinum component of the same amount as that added as the reaction catalyst was detected, and thus the transparent composite of the present invention was confirmed. Example 3 324010 39 201249910 In addition to changing the cerium oxide particles from l〇g (25 mass%) to 16 g (4 畺%), respectively, and modifying the side chain ethylene group as a vinyl group _ Diterpene polyoxyl VDT-131 from 14.  Lg (47 quality « changed to 5.  7 g (19% by mass), which is a hydrogen-modified polyfluorene-based fluorenyl hydrogen-dimercaptopolyoxyl HMS-151 from 〇·_% by mass) to G. 3g (1% by mass), which will act as the surface of the reaction catalyst. Divinyltetradecyldioxane SIP683〇 3 is changed from 6rag(〇 〇2质量〇/〇) to 3mg (0.  Other than 01% by mass. The remainder was subjected to the operation of Example i to obtain a surface-modified oxidized silk-oxygen composite composition of Example 3 and a transparent composite having a thickness of 1 mm. The content of the oxidized silk of the transparent composite was 4 (% by mass). / The granules of the oxidized oxide particles in the obtained transparent composite of Example 3 were rubbed in the same manner as in the examples, and as a result, the average dispersion was 10 nm. As a result, it was concluded that the average dispersed particle diameter of the oxidized silk in the composite composition of Example 3 was 4 Q nm or less. Further, in the obtained transparent composite of Example 3, the elemental component was found to be detectable in the same manner as the amount added as the reaction catalyst, and it was confirmed that the transparent complex Example 4 of the present invention was obtained. As a vinyl modified poly-stone oxygen-based ruthenium poly-stone oxygen-131 from 14.  Lg (47 mass%) vinyl-amount, and will be modified as hydrogen, ? g (39 quality (5).. 9 (10) quality (four) changed to methyl ώ Ί $ 〇 3. 3δ (11 mass (4)), according to the example! 324010 40 201249910 operation, the surface modified oxidized composition of Example 4 and a transparent composite having a thickness of 1 mm were obtained. ^子' Juqian resin complexed with the transparent composite The oxidized erroneous particles contained 25% by mass of the obtained transparent composite of Example 4, and 丨, / were also obtained by dry oxidized particles.

The ruthenium was determined in the same manner as in the case of Example 1, and was at 7 nm. ,,. The 'average dispersed particle diameter is oxidation =:=: also::= group - and 'the result of elemental separation of the obtained transparent composite of Example 4' is detectable and added as a reaction catalyst Since the amount of the platinum component in the same amount was obtained, it was confirmed that the transparent composite of the present invention was obtained. Example 5: In addition to the side-chain oxime dimethyl phthalocyanine VDT_131 as a vinyl modified polyoxo oxygen, 14. lg (47% by mass) was changed to side ς 〇 dimethyl phthalocyanine Alkyl VDT, a 73UGelest company, 4 8g (i6 quality &quot;%), and 0.9g (3 mass « changed to 甲基 as hydrogen hydrogen modified polyhydrogenated methyl hydrogen-difluorenyl polyoxyl HMS_ 151 The surface-modified cerium oxide particle-polyoxymethylene resin composite composition of Example 5 was obtained by the operation of Example 丨 except for the hydrazine of the hydrazine-hydrogen hms 〇3i, 2 g (34% by mass). And a transparent composite having a thickness of 1 mm. The content of the zirconia particles in the transparent composite is 25% by mass. ^ The particles of the oxidized oxidized particles in the obtained transparent composite of Example 5 are lightly In the same manner, as a result, the average dispersed particle diameter was 7 nm. 324010 41 201249910 From the results, it was concluded that the average dispersed particle diameter of the oxidized mision in the composite composition of Example 5 was also 7 nm or less. 'The elemental analysis of the obtained transparent composite of Example 5 was carried out." The transparent composite of the present invention was confirmed to be the same amount as the amount of the reaction catalyst added. Example 6 In addition to the side-chain vinyl fluorenyl group which is a vinyl modified polyfluorene oxygen; 14. lg (47% by mass) was changed to a two-terminal ethyl sulfanyl group, a fluorene-based DMS-V21 (manufactured by Gelest), 13.5 g (45 mass 〇) and used as a hydrogen-modified polyoxyl The methyl quinone dimercapto polyoxyl oxime. 9g (3 mass%) was changed to sulfhydryl hydrogen monodimethyl sulphate oxime hms_3〇i (GeleSt company made 5g (5 f%%) According to the embodiment, the surface-repaired and purified particles of the embodiment 6 were obtained, and the composite composition having a thickness of 1 mm was obtained. The content of the oxidized hammer particles of the transparent composite was 25 mass. The pellet of cerium oxide particles in the obtained transparent composite of Example 6 was measured in the same manner as in Example ,, and the average dispersed particle diameter of the yarn was the result of the following conclusion: Compound of Example 6 The average dispersed particle size of the group of oxidized particles is also advised or less. As a result of the analysis of the transparent composite of Example 6, since the same amount of the platinum component as the reaction catalyst was detected, it was confirmed that the transparent composite 4 of the present invention was obtained. Example 7 324010 42 201249910 Vinyl modified polyfluorene side chain vinyl-dimethyl methacrylate VlyM31 14 lg (47% by mass) changed to two-end vinyl _ monomethyl concentrating DMS-V22 (Gelest 14.7g (49 mass / 〇) and as a hydrogen modified polyoxyl hydrazino hydrogen-dimercaptopolyoxyl HMS_ 151 〇.9g (3 mass « changed to thiol hydrogen - dimercapto In addition to 0.3 g (1% by mass) of polyoxyl HMS-301, the remaining portion was subjected to the operation of Example 1, to obtain a surface-modified oxide particle-polyoxyresin composite composition and a transparent composite having a thickness of 1 mm. The content of the cerium oxide particles in the transparent composite was 25% by mass. The particles of the oxidized particles in the obtained transparent composite of Example 7 were measured in the same manner as in Example 1 and, as a result, the average dispersed particle diameter was 疋 l 〇 nm. As a result, it was concluded that the average dispersed particle diameter of the embodiment (10) was 10 nm or less in the composite composition or less. = The elemental component of the obtained transparent composite of Example 7 was found to have the same amount as that of the reaction catalyst: the platinum component was confirmed, and the transparent composite of the present invention was confirmed. Example 8 ', the knife was changed as a vinyl modified polyfluorene side chain vinyl _ two amount & polyoxy VDT-131 from 14. lg (47% by mass) to H. 4g (48 quality 151 and will be used as a hydrogen modified polyhydrogenated methyl hydrogen _ dimethyl polyoxan HMS - 0 6 〇 9g (3 quality set to methyl hydrogen monodimethyl phthalocyanine HMS_301 Example 8g In addition to (2% by mass), according to the operation of Example 1, a surface-modified cerium oxide particle-polyoxymethylene resin composite composition and a transparent composite having a thickness of 1 _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ The content of the oxidized particles was 25% by mass. The particle size of the cerium oxide particles in the obtained transparent composite of Example 8 was measured in the same manner as in Example 1, and as a result, the average dispersed particle diameter was 7 nm. From this result, it was concluded that the average dispersed particle diameter of the oxidized dipole in the composite composition of Example 8 was also 7 nm or less. Further, the elemental composition of the obtained transparent composite of Example 8 was subjected. As a result of the =, since the surface component equivalent to the amount added as the reaction catalyst can be detected, it is confirmed The transparent composite of the present invention. Example 9 In addition to the side change of 14. lg (47% by mass) of the side chain vinyl one-two-polyoxyl VDT-131 as a vinyl modified polyoxyl group, respectively Key B ^ ϊ Γ Γ Γ 731 - 731 u.4g (38 ft%) ' and will be used as hydrogen-based soil-based U-based oxygen HMS_151 of Mg (3 mass into methyl hydrazine - dimethyl poly Qianling Xie Zhi 3 The content of the oxidized H particles obtained by the operation of the surface-repairing complex oxygen resin composite composition of Example 9 and the transparent transparent coating of the thickness of the composite material of Example 9 was 25 mass. %. The obtained oxidized erroneous particles in the transparent composite of Example 9 was obtained in the same manner as in the case of carrying out W (IV), and as a result, the average dispersed particles were =324 〇i 〇, and the results were as follows: The average dispersed particle diameter of the 201249910 oxidation-degraded particles in the composite composition of 9 is also (10) or less. Analysis: Fruit pair: The obtained transparent composite of Example 9 was subjected to elemental concentration = two measured and reacted The surface of the same amount added by the catalyst was formed into a knife, and it was confirmed that the transparent composite of the present invention was obtained. Example 10 = respectively As a side of the county, the f (four) oxygen side chain ethylene base _ 21 土 甲 氧 oxygen VDT-131 14 lg (47% by mass) was changed into two ends of the gynecological group 曱 曱 矽 矽 D D DMS-V22 14 傲-〇/, 改(四) of U.7S (49 罝W, and will be used as hydrogen * i methyl hydrogen - dimethyl poly oxyhydrogen leg _i5i ο </ </ /> </ </ /> The quality of the base polysulfide hms-301 〇.3 ^ as anti-sense media money divinyl tetramethyl dioxine oxygen training _ changed to platinum 5 曱 vinyl 曱 矽 矽 SIP SIP 6832.2 (Gelest company gas Except for the rest of the operation according to Example i, the surface-modified oxidized silk-(tetra) oxy-resin composite composition of the example and the transparent composite having a thickness of - were obtained. The content of the cerium oxide particles of the 5 Å transparent composite was 25% by mass. The oxidized erroneous particles in the obtained transparent composite of Example 10 were rubbed in the same manner as in Example 1, and as a result, the average dispersed particle diameter was 9 nm. From the results, it was concluded that the average dispersed particle diameter of the oxidized particles in the composite composition of Example 10 was also 9 nm or less. Further, as a result of performing the elemental division of the obtained transparent composite of Example 10, since the platinum component equivalent to the amount added as the reaction catalyst was detected, it was confirmed that the transparent composite of the present invention was obtained. 324010 45 201249910 The comparative methyl group will be used as a vinyl-modified polyfluorene-terminated side chain vinyl-dicarboxylic polyglycol Amg (29% by mass), and will be changed to a polymethyl group. Shi Xi oxygen HMS-151 〇 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 A surface modification of 1. The content of the oxidized erroneous particles of the composite composition of the Μ' poly-stone composite resin and the thickness of 1 mm was 25% by mass. The compound of Zhao Zhongzhi oxidized the particles of the particle 35 coffee. As a result of the measurement in the same manner as in ours, the average dispersed particle size is the end of the comparative example 2 ι=Γ::=the side of the side chain of the oligo-oxygen-ethylene group, the two ends of the two-dimethyl ketones ms-V22 Ethyl group was formed into methyl argon-dimethyl poly-bis;:;; = gasification ^1 operation, and the surface modification of Comparative Example 2 was obtained. The content ratio of the oxidized erroneous particles of the composite composition of the ～子, the cut oxide resin, and the composite 324〇1〇 46 1 having a thickness of 1 mm was 25% by mass. 2 The particles of the cerium oxide particles in the obtained composite of Comparative Example 2 were measured in the same manner as in Example 1 and the average dispersed particle diameter was *42 nm. Comparative Example 3 In the same manner as in Example 1, In the ruthenium oxide particles produced in the same manner, 85 g of toluene and 5 g of hexanoic acid were added and mixed, and the surface of the oxidation cone particles was modified via hexanoic acid belonging to a ligand. Thereafter, dispersion treatment was carried out to prepare a transparent dispersion of zirconia. After the reaction was terminated, the solvent was removed by an evaporator, and acetone was washed and centrifuged repeatedly to remove oxidized # particles and unreacted hexanoic acid. The recovered zirconia particles which have been modified by the hexanoic acid belonging to the ligand are llg. In addition to using the hexanoic acid-modified oxidized particles (% by mass) as zirconia particles, and respectively, as a vinyl-modified polyfluorene-oxyethylene-dimethyl polyoxet VDT-131 from I4.ig ( The change of 47 mass%) to 18. 8g (63 mass%), which is a hydrogen-modified polyfluorene-based sulfhydryl hydrogen-dioxime polyoxyl HMS-151 from 0. 9g (3 mass « changed to h 2g ( /mass^, two as the reaction catalyst, platinum divinyltetramethyldioxane SIp683〇3 from 6mg (〇.〇2 mass « changed to 9mg (〇.〇3 mass%), Example 1 was operated to prepare a surface-modified oxidized silk fabric of Comparative Example 3 and a composite having a thickness of 1 mm. The content of the oxidized erroneous particles of the 6-mite composite was 25% by mass. The obtained oxidized silk particles in the composite of Comparative Example 3 were measured in the same manner as in Example 1 and the average dispersion range was [Evaluation] 324010 47 201249910 For each of the transparent composites of Examples 1 to 10 and The composites of Comparative Examples 1 to 3 were evaluated for transparency, refractive index, and durability by the following apparatus or method. (1) Transparency use The spectrophotometer (manufactured by JASCO Corporation) measures the transmittance of visible light. Here, the transmittance of visible light in the thickness direction (L = 1 mm) of the transparent composite (or composite) is measured, and the visible light is Those who have a penetration rate of 80% or more are treated as "〇", and those who do not exceed 80% are regarded as "X". (2) The refractive index is based on Japanese Industrial Standard JIS K 7132 "Method for Measuring Refractive Index of Plastics" The refractometer is used for the measurement. Here, the resin having no cerium oxide particles added is used as a reference, and the refractive index is increased to 0.03 or more, and the refractive index is increased only to The case of 0.03 is considered as "X". (3) Durability The transparent composite (or composite) is allowed to stand at a temperature of 150 ° C for 24 hours, and then taken out to visually observe the transparent composite (or The appearance of the composite) is regarded as "〇" in the absence of yellowing and as "X" in the yellowing. The composition of each composite composition of Examples 1 to 10 and Comparative Examples 1 to 2 and the transparent composite ( The results of the evaluation of the composites are shown in Table 1. 324010 48 201 249910 Durability 〇〇〇〇〇〇〇〇〇〇 Not evaluated X Refractive index 〇〇〇〇〇〇〇〇〇〇 Transparency 〇〇〇〇〇〇〇〇〇〇 XXX Reaction Catalyst Hardening with 0.02 Mass% 1 1 1 Room temperature hardening is determined by the peasant peasant desire to determine φ4φ!φ{φ!(φ1φ4φ&lt;1φ|ι^4 启桃无生"“““11 〇G&gt;OCD 0 000&lt;=&gt;0 To seek the second φ| 叙启龄 c&lt;j 〇v3 co ο ο ο ο ο ο Hydrogen modified polyoxygen side chain i 30 mol% 5 mass% 1 mass% 2 mass ft% 12 mass% 1 mass% 1 1 1 side chain 3 mass%; 2 mass% 1 mass%: 1 ! 4 mass S% side chain 3 mol% - ! 11 mass% 34 mass% 21 mass% 6 mass% Vinyl-modified polyoxyl, side chain 7 mol% 16 mass% 38 mass% 1 1 1 side chain l mol% 47 mass% 28 mass% 19 mass% 39 mass% 48 mass% 63 f ft% both ends 1 mass%; 45% by mass 29% by mass Both ends 0.45 mass% 49% by mass 49% by mass 44 Mass 3:3⁄4 1 - Surface modifier PDMS-G 25 mass 96 35 mass% 40 mass% 25 mass Amount % 25 mass% 25 mass% 25 mass% 25 mass% 25 mass%: 25 mass% 25 mass% 25 ft% one (氺) inorganic oxide particles cerium oxide. 25 mass% 35 mass% 40 mass% 25 mass% 25 mass% 25 mass% 25 mass% 25 mass% 25 mass% 25 mass% 25 mass% 25 25 mass% Example 1 Example 2 Example 3 Example 4 Example 5 Example 6 Example 7 Example 8 Implementation Example 9 Example 10 Comparative Example 1 Comparative Example 2 Comparative Example 3 sss-铋8 铋10:* 49 324010 201249910 From Table 1, it is understood that all of the transparent composites of Example 1 S 10 have transparency, refractive index and durability. The characteristics are excellent. The composite of Comparative Example 2 has a visible light transmittance of 0% to 20% and is extremely low. Further, the refractive index cannot be measured. It is speculated that the reason is that the agglomeration density of the inorganic oxide particles becomes smaller than that of the polyoxo oxy-resin due to the small cross-linking density of the hydrogen-modified poly-stone and the oxidized poly-stone. The hardening speed is also fast, and as a result, the transparency is lost when the inorganic oxide particles and the polyoxymethylene resin are hardened. * The composite of Comparative Example 3 has a visible light transmittance of 10% or less and is extremely low, and the refractive index cannot be measured. The reason for the basin is that the surface of the inorganic oxide particles is insufficiently repaired, so that the inorganic oxide particles aggregate in the composite composition of the inorganic oxide particles and the polyoxygen peroxide resin, and as a result, the transparency in the composite cannot be obtained. . Further, regarding the durability, after the air was left for 24 hours, the effect of discoloration caused by hexanoic acid was confirmed because the yellowing was observed. [Industrial Applicability] The present invention provides an inorganic oxide particle composite composition and a transparent composite, wherein the complex characteristics of the S. cerevisiae and the gas barrier property of the inorganic oxide particles are dispersed::: At 2 o'clock, the dispersibility is high, and the transparency is prevented in the hard J-polyoxynium tree. In the phase separation/whitening of the first embodiment, the inorganic oxide particle I of the present invention can be dispersed into a polycomposite composition, which contains inorganic oxide particles 324010 50 201249910 catalyst; The inorganic oxide particles are surface-modified by combining a polydifluorenyl fluorene oxide backbone polymer having one functional group at the unilateral terminal, and an inorganic oxide particle having an average dispersed particle diameter of 1 nm or more and 20 nm or less. Thereby, it is possible to obtain a transparent composite which maintains the transparency, heat resistance and light resistance of the composite obtained by combining the inorganic oxide particles and the polyoxynoxy resin, and also controls the refractive index. Therefore, it is of course possible to use the semiconductor. Light-emitting element (LED) sealing material, substrate for liquid crystal display device, substrate for organic EL display device, substrate for color filter, substrate for touch panel, substrate for solar cell, transparent sheet, optical lens, optical element In the optical waveguides, adhesives, and the like, it is also widely available in various industrial fields. [Simplified description of the drawings] None. [Main component symbol list description] No 0 324010 51

Claims (1)

201249910 VII. Patent application scope: 1. A kind of inorganic oxide particles and silicin resin, containing six a person &amp; 丄, .&quot; * . 7 〇μ' a composite composition of the present invention, the composite composition comprising at least inorganic oxide particles, a composite composition of a polyoxyxylene resin and a reaction catalyst; wherein the inorganic oxide particles are combined by a single side a polydimethyl ketone (tetra) dry polymer having a functional group at the end and an inorganic oxide particle having a surface-modified average particle size of 1 nm or more and 2 〇 nm or less; Ethylene-based modified polychlorite and hydrogen modified polyoxo; the above reaction catalyst contains a hydrogenation reaction catalyst. 2. The inorganic oxide particles and polyfluorene composition according to Item 1, wherein 'the aforementioned polydimethyl-dicalcified bone dry (4) hydroglyceryl ether terminal polydimethyl oxalate and early hydroxy ether terminal poly 2 Methyl decane. The inorganic oxide particles according to Item 1 or 2 and the poly(4) oxydiphenyl-dimethyl odor poly(tetra) soil: methyl poly-coin, two-terminal vinyl oxygen, two end-heart benzene The group consists of oxygen, ethyl, and sulfonate grades, wherein the hydrogen-modified poly-324010 1 201249910 is selected from the hydrogen-dithiol group at both ends. One or two of a group consisting of hydrogen-dimethyl polyfluorene, methyl hydrogen polyoxynium, ethyl hydrogen polyoxynium oxide, mercaptohydrogen-phenylmethyl polyfluorene, and hydride resin the above. 5. The composite composition of the inorganic oxide particles and the polyoxyxylene resin according to any one of the first aspect of the present invention, wherein the hydrogen-modified polyfluorene oxygen contains the following formula (1). Side chain hydrogen-modified polyfluorene: r3 Η R2 Re (1) R4——Si—0—Si—Ο Si—Ο—Si—R7 R5 Ri Ri Re nm (However, 1 to R8 are mutual Independent of any organic group (except H), m is an integer of 1 or more, η is a positive integer containing 0); ratio of m to η in the aforementioned side chain hydrogen-modified polychlorite (m/(m+n) )) is 0.25 or more and 1 or less. 6. A transparent composite obtained by combining surface-modified inorganic oxide particles with a polydimethyl methoxy siloxane backbone polymer having one functional group at one end and having an average dispersed particle diameter of 1 nm or more Further, it is dispersed in a polyoxonium resin in a form of 20 nm or less, and a deuteration reaction catalyst is contained in the polyfluorene oxide resin. 7. A transparent composite which is formed and cured into a predetermined shape by the composite composition of the inorganic oxide particles and the polyoxin resin according to any one of claims 1 to 5, or It is formed by solidifying the composite composition. The method for producing a composite composition of an inorganic oxide particle and a polyoxyxylene resin according to any one of claims 1 to 5, which comprises the following steps: a surface modified by a polydidecyl fluorene oxide backbone polymer having one functional group at one end, to obtain a surface-modified inorganic oxide particle having an average dispersed particle diameter of 1 nm or more and 20 nm or less; The step of mixing the surface-modified average dispersed particle diameter of 1 nm or more and 20 nm or less of the inorganic oxide particles and the polyoxoxime resin with the reaction catalyst. 324010 3 201249910 IV. Designated representative map: (1) The representative representative of the case is: The case has no schema. (2) A brief description of the symbol of the representative figure: None. 5. If there is a chemical formula in this case, please disclose the chemical formula that best shows the characteristics of the invention: 4 R R—si—R o 5 IV ΗIsiIRl o i R2IsiIRl ο η R6Isi—R8 R7 324010 3