Silica-containing resin composition and method for producing same, and molded article produced from silica-containing resin composition

Patent metadata

Field	Value
Publication number	US-9777141-B2
Application number	US-201414896070-A
Country	US
Kind code	B2
Filing date	Jun 5, 2014
Priority date	Jun 10, 2013
Publication date	Oct 3, 2017
Grant date	Oct 3, 2017

Abstract

A silica-containing resin composition, characterized by containing a resin and silica particles in an amount of 5 to 300 parts by mass, with respect to 100 parts by mass of the resin, wherein the silica particles satisfy the following requirements (a) to (c): (a) the silica particles have a specific surface area, as determined through a nitrogen absorption method, of 20 to 500 m 2 /g; (b) the silica particles have a percent moisture absorption of 5.0 mass % or less at a relative humidity of 50%; and (c) the silica particles contain substantially no metallic impurity or halogen.

First claim

The invention claimed is:

1. A silica-containing resin composition, comprising a resin and surface-treated silica particles in an amount of 5 to 300 parts by mass, with respect to 100 parts by mass of the resin, wherein
(a) the silica particles have a specific surface area, as determined through a nitrogen absorption method, of 20 to 500 m 2 /g,
(b) the silica particles have a percent moisture absorption of 5.0 mass % or less at 23° C. and a relative humidity of 50%,
(c) the silica particles contain substantially no metallic impurity or halogen,
(d) the silica particles have a moisture absorption amount per surface area thereof of 0.5 mg/m 2 or less at 23° C. and a relative humidity of 50%,
(e) the silica particles have a ratio (D2/D1) of mean particle size (D2) measured through dynamic light scattering to mean particle size (D1) measured through the BET method of 1.6 or lower, and
(f) the surface-treated silica particles are produced, without firing of the silica particles, by a method that comprises:
hydrolyzing a silicon alkoxide in water and an optional hydrophilic organic solvent as a reaction medium in the presence of a hydrolysis catalyst, with the temperature of the reaction medium being 60° C. or higher and the ratio by mole of water to silicon (H 2 O/Si) being maintained at 25 or higher, to obtain the silica particles, wherein the hydrolysis catalyst is at least one member selected from the group consisting of ammonia, primary to tertiary amines, and a quaternary ammonium; and
modifying surfaces of the silica particles with hydrolysis products and/or hydrolysis condensation products of an organic silane compound in water and/or a hydrophilic organic solvent.

2. The silica-containing resin composition according to claim 1 , wherein the surface-treated silica particles have undergone organophilization with the organic silane compound at ≧0.5 molecules per 1 nm 2 surface thereof.

3. The silica-containing resin composition according to claim 2 , wherein the organic silane compound is at least one compound selected from the group consisting of alkoxysilane, silazane, siloxane, acetoxysilane, and silylurea.

4. The silica-containing resin composition according to claim 2 , wherein the surface-modified silica particles have a percent moisture absorption of 3.0 mass % or less at 23° C. and a relative humidity of 50%.

5. A molded article formed of the silica-containing resin composition according to claim 1 .

6. A method for producing a silica-containing resin composition, the method comprising:
forming surface-treated silica particles without firing of the silica particles; and
incorporating the silica particles into a resin in an amount of 5 to 300 parts by mass, with respect to 100 parts by mass of the resin, wherein forming the surface-treated silica particles includes:
hydrolyzing a silicon alkoxide in water and an optional hydrophilic organic solvent as a reaction medium in the presence of a hydrolysis catalyst, with the temperature of the reaction medium being 60° C. or higher and the ratio by mole of water to silicon (H 2 O/Si) being maintained at 25 or higher, to obtain the silica particles, wherein the hydrolysis catalyst is at least one member selected from the group consisting of ammonia, primary to tertiary amines, and a quaternary ammonium; and
modifying surfaces of the silica particles with hydrolysis products and/or hydrolysis condensation products of an organic silane compound in water and/or a hydrophilic organic solvent; and
wherein the silica particles have
a moisture absorption amount per surface area thereof of 0.5 mg/m 2 or less at 23° C. and a relative humidity of 50%,
a specific surface area, as determined through a nitrogen absorption method, of 20 to 500 m 2 /g, and
a ratio (D2/D1) of mean particle size (D2) measured through dynamic light scattering to mean particle size (D1) measured through the BET method of 1.6 or lower.

7. The method according to claim 6 , wherein the organic silane compound is present at ≧0.5 molecules per 1 nm 2 surface of the silica particles.

8. A molded article formed of the silica-containing resin composition according to claim 2 .

9. A molded article formed of the silica-containing resin composition according to claim 3 .

10. A molded article formed of the silica-containing resin composition according to claim 4 .

11. A method for producing a silica-containing resin composition, the method comprising:
forming surface-treated silica particles; and
incorporating the silica particles into a resin in an amount of 5 to 300 parts by mass, with respect to 100 parts by mass of the resin, wherein forming the surface-treated silica particles consists essentially of:
hydrolyzing a silicon alkoxide in water and an optional hydrophilic organic solvent as a reaction medium in the presence of a hydrolysis catalyst, with the temperature of the reaction medium being 60° C. or higher and the ratio by mole of water to silicon (H 2 O/Si) being maintained at 25 or higher, to obtain the silica particles, wherein the hydrolysis catalyst is at least one member selected from the group consisting of ammonia, primary to tertiary amines, and a quaternary ammonium; and
modifying surfaces of the silica particles with hydrolysis products and/or hydrolysis condensation products of an organic silane compound in water and/or a hydrophilic organic solvent; and
wherein the silica particles have
a moisture absorption amount per surface area thereof of 0.5 mg/m 2 or less at 23° C. and a relative humidity of 50%,
a specific surface area, as determined through a nitrogen absorption method, of 20 to 500 m 2 /g, and
a ratio (D2/D1) of mean particle size (D2) measured through dynamic light scattering to mean particle size (D1) measured through the BET method of 1.6 or lower.

Assignees

• Nissan Chemical Ind Ltd

Inventors

• Yoshitake Keiko
• Kikunaga Ichitaro
• Miyamoto Ai
• Shimada Megumi

Classifications

• C01B33/148

  Concentration; Drying; Dehydration; Stabilisation; Purification {(C01B33/1465 takes precedence)} · CPC title

• C01P2006/12

  Surface area · CPC title

• C08K3/36

  Silica · CPC title

• C08L101/00

  Compositions of unspecified macromolecular compounds · CPC title

• C09C1/3081

  Treatment with organo-silicon compounds · CPC title