Composite of silicon oxide nanoparticles and silsesquioxane polymer, method for producing same, and composite material produced using composite thereof
An object of the present invention is to provide a composite of silicon oxide nanoparticles and a silsesquioxane polymer, from which a cured film having a low refractive index can be formed inexpensively. Provided are a method of producing a composite of silicon oxide nanoparticles and a silsesquioxane polymer, the method comprising reacting a silsesquioxane polymer having a silanol group at a terminal or a silane monomer with silicon oxide nanoparticles having a hydroxyl group or an alkoxy group on the surface in a mixed solvent of an aqueous solvent and an organic solvent in the presence of a phase transfer catalyst, and a composite produced by the method.
1. A composite consisting of silicon oxide nanoparticles, a silsesquioxane polymer, a phase transfer catalyst and one or more optional components selected from the group consisting of surfactants, organic spacers, lubricants and viscosity modifiers, wherein such that said composite has a transmittance of >95% at a wavelength of 400 nm, wherein the transmittance is obtained by curing the coating film at a temperature of 150° C. or higher for 5 min or longer, and wherein said composite is obtained by reacting said silsesquioxane polymer having a silanol group at a terminal with silicon oxide nanoparticles having a hydroxyl group or an alkoxy group on a surface of the silicon oxide nanoparticles in a mixed solvent of an aqueous solvent and an organic solvent in the presence of said phase transfer catalyst, said phase transfer catalyst is present in an amount of 2 to 50% by mol based on the total amount of said composite, and wherein said silsesquioxane polymer comprises a repeating unit selected from the group consisting of [R 1 SiO 1.5 ], wherein R 1 is selected from the group consisting of hydrogen, an alkyl group, an aryl group and an alkenyl group, and [SiO 2 ].
2. The composite according to claim 1 , wherein said silsesquioxane polymer has a weight-average molecular weight of 500 to 20,000.
3. The composite according to claim 1 , wherein said silicon oxide nanoparticles have an average particle size of 5 to 200 nm.
4. The composite according to claim 1 , wherein said aqueous solvent is water or a mixed solvent of water and an alcohol.
5. The composite according to claim 1 , comprising said silicon oxide nanoparticles in an amount of 5 to 90% by weight based on the a total amount of said composite.
6. The composite according to claim 1 , wherein silicon atoms of said silsesquioxane polymer are bound with the surface of said silicon oxide nanoparticles via oxygen atoms.
7. The composite according to claim 1 , obtained by heat-curing the composite according to claim 1 in the air or in an inert atmosphere.
8. The silicon oxide-containing composite material according to claim 7 , which is a porous material comprising pores formed therein.
9. An electron device, comprising the silicon oxide-containing composite material according to claim 7 as an interlayer film, a refractive index control film, an anti-reflection film or a protective film.
10. A method of producing the composite of claim 1 wherein said method comprises reacting said silsesquioxane polymer having a silanol group at a terminal with silicon oxide nanoparticles having a hydroxyl group or an alkoxy group on the surface of the silicon oxide nanoparticles in a mixed solvent of an aqueous solvent and an organic solvent in the presence of a phase transfer catalyst in an amount of 2 to 50% by mol based on the total amount of said composite.