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Polycarbonate Resin Blends Containing Titanium Dioxide

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Polycarbonate Resin Blends Containing Titanium Dioxide (19) & (11) EP 1 123 350 B1 (12) EUROPEAN PATENT SPECIFICATION (45) Date of publication and mention (51) Int Cl.: of the grant of the patent: C08L 69/00 (2006.01) C08K 9/00 (2006.01) 07.10.2009 Bulletin 2009/41 C08K 3/22 (2006.01) (21) Application number: 99941997.1 (86) International application number: PCT/US1999/017567 (22) Date of filing: 03.08.1999 (87) International publication number: WO 2000/024828 (04.05.2000 Gazette 2000/18) (54) POLYCARBONATE RESIN BLENDS CONTAINING TITANIUM DIOXIDE TITANDIOXID ENTHALTENDE POLYCARBONATMISCHUNGEN MELANGES DE RESINES DE POLYCARBONATES RENFERMANT DU DIOXYDE DE TITANE (84) Designated Contracting States: • DATABASE WPI Section Ch, Week 199443 DE ES FR GB NL Derwent Publications Ltd., London, GB; Class A13, AN 1994-347250 XP002125382 & JP 06 (30) Priority: 23.10.1998 US 177946 271728 A (MITSUBISHI GAS CHEM CO INC), 27 September 1994 (1994-09-27) (43) Date of publication of application: • CHEMICAL ABSTRACTS, vol. 124, no. 20, 13 May 16.08.2001 Bulletin 2001/33 1996 (1996-05-13) Columbus, Ohio, US; abstract no. 262612, XP002125378 & JP 08 012869 A (60) Divisional application: (SUMITOMO DOW KK) 16 January 1996 07121738.4 (1996-01-16) • CHEMICAL ABSTRACTS, vol. 124, no. 4, 22 (73) Proprietor: SABIC Innovative Plastics IP B.V. January 1996 (1996-01-22) Columbus, Ohio, US; 4612 PX Bergen op Zoom (NL) abstract no. 31193, XP002125379 & JP 07 216181 A (JAPAN SYNTHETIC RUBBER CO. LTD.) 15 (72) Inventors: August 1995 (1995-08-15) • Barren, James Paul • CHEMICAL ABSTRACTS, vol. 126, no. 18, 5 May Scotia, NY 12302 (US) 1997 (1997-05-05) Columbus, Ohio, US; abstract • Osborn, Arthur J. no. 239235, XP002125380 & JP 09 048911 A Catskill, NY 12414 (US) (SUMIKA EI BII ESU RATETSUKUSU) 18 February • Chen, Fuh-Sheng Fred 1997 (1997-02-18) Evansville, IN 47712 (US) • DATABASE WPI Section Ch, Week 199808 Derwent Publications Ltd., London, GB; Class (74) Representative: Modiano, Micaela Nadia et al A23, AN 1998-082834 XP002125383 & JP 09 Modiano Josif Pisanty & Staub Ltd 316315 A (DAITO KASEI KOGYO KK; TEIJIN Thierschstrasse 11 KASEI LTD.), 9 December 1997 (1997-12-09) 80538 München (DE) • CHEMICAL ABSTRACTS, vol. 127, no. 12, 22 September 1997 (1997-09-22) Columbus, Ohio, (56) References cited: US; abstract no. 162602, XP002125381 & JP 09 EP-A- 0 065 777 EP-A- 0 739 914 176471 A (NIHON GE PLASTICS, LTD.) 8 July 1997 EP-A- 0 771 852 WO-A-80/00708 (1997-07-08) DE-A- 2 019 325 DE-A- 19 530 200 • DATABASE WPI Section Ch, Week 199329 DE-A- 19 630 063 Derwent Publications Ltd., London, GB; Class A18, AN 1993-232499 XP002125384 & JP 05 156102 A (MITSUI TOATSU CHEM INC), 22 June 1993 (1993-06-22) Note: Within nine months of the publication of the mention of the grant of the European patent in the European Patent Bulletin, any person may give notice to the European Patent Office of opposition to that patent, in accordance with the Implementing Regulations. Notice of opposition shall not be deemed to have been filed until the opposition fee has been paid. (Art. 99(1) European Patent Convention). EP 1 123 350 B1 Printed by Jouve, 75001 PARIS (FR) EP 1 123 350 B1 Description FIELD OF THE INVENTION 5 [0001] This invention relates to a method for making streak resistant, injection moldable polycarbonate resin blends which contain titanium dioxide. BRIEF DESCRIPTION OF THE RELATED ART 10 [0002] Flame retardant thermoplastic resin compositions that contain an aromatic polycarbonate resin, an ABS graft copolymer, a fluoropolymer and an organophosphate flame retardant are known and have been found to exhibit good flame retardency and good heat resistance, see, for example, coassigned U.S. Patent Number 5,204,394. [0003] It is also known that it is desirable to incorporate titanium dioxide into various thermoplastic resin blends. Titanium dioxide is incorporated into resin blends as a coloring agent to obtain desirable appearance. 15 [0004] The prior art specifically relating to polycarbonate resins indicate that a preferred titanium dioxide for use in such resins consists of plural coatings, usually two or three coatings which may comprise a first polysiloxane or polyol coating, a second silicone type coating, and/or a third branched polyorganosiloxane with silanol functionality. See, for example, Kronos Titanium Dioxide in Plastics Issue 1993, commercial brochure; and Plastics Compounding, November/ December 1993, pages 44-46. Such prior art indicates that titanium dioxide with such coatings provides polycarbonate 20 resins with good color and physical properties. [0005] Polycarbonate resin blend compositions that incorporate titanium dioxide to impart improved aesthetic appear- ance, particularly improved resistance to streaking, are desired. We have discovered that the titanium dioxides preferred by the prior art, having plural coatings, result in streaking when molding polycarbonate resin blends. [0006] Derwent Abstract AN 1996-262612 (JP-A-08012869) discloses a polycarbonate resin composition comprising 25 (A) a polycarbonate resin, (B) a composition prepared by kneading a styrene resin with titanium dioxide treated with hydrous alumina and/or silica, and (C) a rubber reinforcing material. The compositions have good impact resistance, heat resistance and light reflecting properties for the preparation of reflectors for liquid crystal displays. [0007] Derwent Abstract AN 1998-082834 (JP-A-9316315) discloses an aromatic polycarbonate resin composition consisting of (A) 99.95-60 parts by weight of a thermoplastic resin in which an aromatic polycarbonate resin is not less 30 than 50 wt% of 100 wt% resin components, and (B) 0.05-40 parts by weight titanium dioxide whose surface is treated at 150-300°C with polysiloxane. The compositions have good mechanical properties, heat stability, no decrease in whiteness or reflection, and high impact strength. [0008] Derwent Abstract AN 1997-246641. (JP-A-09048911) discloses a polycarbonate resin composition containing (A) 100 parts by weight polycarbonate resin, (B) 0.01-5 parts by weight of a light diffusing filler, and (C) 0.0001-5 parts 35 by weight titanium dioxide composition containing polyhydric alcohol. The composition has good transparency, mechan- ical strength, and light diffusivity realized by the addition of a light diffusing filler. [0009] EP-A-0 771 852 discloses flame retardant thermoplastic compositions containing an aromatic polycarbonate resin, a vinyl aromatic-unsaturated nitrile rigid resin, a vinyl aromatic-unsaturated nitrile-rubber graft copolymer containing a C30-C108 polyacid, a phosphate flame retardant, and a tetrafluoroethylene polymer. The compositions have reduced 40 levels of viscosity without a reduction in Izod impact properties. [0010] Plastics Compounding, November/December 1993, pages 44-46 discloses that the high temperature and pres- sure processing conditions required by engineering thermoplastics can accelerate adverse chemical reactions that lead to degradation, especially with a resin-pigment combination such as polycarbonate and titanium dioxide. One titanium dioxide tested is treated with 0.3% aluminum oxide and 1% of a proprietary polysiloxane. Results show the importance 45 of titanium dioxide grade to properties of polycarbonate The properties mentioned are melt flow index, mechanical properties, surface defects and color. [0011] WO 80/00708 discloses pigmented polycarbonate compositions having improved color stability and melt flow stability which are obtained by admixing a high molecular weight aromatic polycarbonate resin containing a pigment such as titanium dioxide with a methyl hydrogen silicone fluid (MHSF). The pigment can be coated with the methyl 50 hydrogen silicone fluid and the thusly coated pigment can then be admixed with the aromatic polycarbonate resin. Improved results measured by a streak test were seen when the concentration of the MHSF-coated titanium dioxide was increased. [0012] WO 99/51671, which is prior art under the terms of Article 54(3) and (4) EPC, discloses a thermoplastic resin composition exhibiting improved thermal stability containing (a) an aromatic polycarbonate resin, (b) a rubber modified 55 graft copolymer that contains a discontinuous elastomeric phase dispersed in a continuous rigid thermoplastic phase, wherein at least a portion of the rigid thermoplastic phase is chemically grafted to the elastomeric phase, (c) a sterically hindered phenol stabilizer compound, (d) a thioester stabilizer compound, and (e) a phosphate stabilizer compound. The composition may also contain a fluoropolymer additive. In addition, the composition may contain a surface-modified 2 EP 1 123 350 B1 titanium dioxide that is coated with one or more layers of one or more organopolysiloxane polymers selected from linear organosiloxane polymers, branched organosiloxane polymers and mixtures thereof. Preferably, the coating contains an organopolysiloxane polymer having Si-H bonds as disclosed in U.S. Patent No. 5,389,714. Composition are exemplified which contain 0.9 parts by weight colorants, including a coated titanium dioxide. 5 [0013] EP-A-0 924 248, which is prior art under the terms of Article 54(3) and (4) EPC, discloses compositions stabilized against the adverse effects of heat and light which comprise (a) a blend of polycarbonate and a second polymer selected from the group consisting of polyesters, styrenic copolymers, rubbers and vinyl chloride polymers or copolymers, and (b) an effective stabilizer amount of a mixture of a non-basic hindered amine containing the 3,3,5,5-tetramethyl-2-oxo- 1-piperazinyl moiety
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