Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – At least one aryl ring which is part of a fused or bridged...
Reexamination Certificate
1998-05-21
2001-04-24
Seidleck, James J. (Department: 1711)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
At least one aryl ring which is part of a fused or bridged...
C524S492000, C524S493000, C523S200000
Reexamination Certificate
active
06221951
ABSTRACT:
FIELD OF THE INVENTION
This invention relates to a polymer composition comprising of a ketone polymer of carbon monoxide and one or more olefins. For some formulations or applications, such polymer formulation must be reinforced. Well-known reinforcing materials are fibers, particularly glass fibers, which may be in the form of thin fibers. The compositions of this invention employ fibers treated with a particular composition, which particular composition comprises an acrylic functionality moiety. The ketone polymer composition has improved impact strength. Polymers based on carbon monoxide and one or more olefins have excellent chemical resistance and can be semicrystalline with a melting point of up to 255° C. Such a class of polymers of carbon monoxide and olefins has been known for some time. U.S. Pat. No. 2,495,286 (Brubaker) disclosed such polymers of relatively low carbon monoxide content In the presence of free radical initiators, e.g., peroxy compounds. Great Britain Patent 1,081,304 discloses similar polymers of higher carbon monoxide content In the presence of alkylphosphine complexes of palladium compounds as catalyst. U.S. Pat. 3,694,412 (Nozaki) extended the reactions to produce linear alternating polymers in the presence of arylphosphine complexes of palladium moieties and certain inert solvents.
More recently, the class of linear alternating polymers of carbon monoxide and at least one ethylenically unsaturated hydrocarbon, now known as polyketones or ketone polymers, has become of greater interest. U.S. Pat. No. 4,880,903 (VanBroekhoven, et al.) discloses a linear alternating ketone terpolymer of carbon monoxide, ethylene, and other olefinically unsaturated hydrocarbons, such as propylene. Processes for production of the polyketones typically involve the use of a catalyst composition formed from a compound of a Group VIII metal selected from palladium, cobalt or nickel, the anion of a strong non-hydrohalogenic acid and a bidentate ligand of phosphorus, arsenic or antimony. U.S. Pat. No. 4,843,144 (VanBroekhoven, et al.) discloses a process for preparing a polymer of carbon monoxide and at least one ethylenically unsaturated hydrocarbon using the preferred catalyst comprising a compound of palladium, the anion of a non-hydrohalogenic acid having a pKa of below about 6 and a bidentate ligand of phosphorus. U.S. Pat. No. 4,880,903 and U.S. Pat. No. 4,843,144 are hereby incorporated by reference.
The resulting polymers are relatively high molecular weight materials having established utility as premium thermoplastics in the production of shaped articles, such as containers for food and drink and parts for the automotive industry, which are produced by processing the ketone polymer according to well known methods.
This family of polymers is called polyketones. The polyketone is, generally, semi-crystalline with a melting point in the range of about 170 to about 250° C.; depending on the polyketone olefinic monomer ratio. In the melt, the polyketone exhibits rheological behavior typical for a linear entangled flexible chain. Therefore, these polyketones are suitable for use in a broad range of processes and equipment, which have been developed for conventional thermoplastics.
The prior art reference EP Patent 0,322,959 describes reinforcement of a polyketone with an inorganic fiber. The reference discloses glass fibers coated with polyketone from a solution in m-cresol and that the glass fibers must have specific (polar) coating, which Is compatible with the polyketone.
U.S. Pat. No. 5,034,431 discloses reinforcement of polyketone with glass fibers having a specific sizing composition. The blending of polyketone and glass fibers is achieved by melt blending. The sizing composition has aminosilane and polyurethane. The sizing composition disclosed in U.S. Pat. No. 5,034,431 may also contain an epoxy functionality.
SUMMARY OF THIS INVENTION
The present invention is directed to ketone polymer compositions comprising (a) a ketone polymer of an alternating or random type, which polymer comprises carbon monoxide and at least one unsaturated compound and (b) fibers which fibers have been treated with a composition comprising an acrylic functionality. Preferably, the fibers are glass fibers coated on the surface with a composition comprising an acrylic functionality. The blend of ketone polymer and glass fibers can be prepared by blending and heating the ketone polymer and glass fibers Into a homogenous, melt processable blend. The blended composition can then be formed into finished articles by such processes as extrusion, injection molding, compression molding and extrusion blow molding.
The composition of this invention employed to treat the reinforcing fibers is comprised of a material having an acrylic functionality moiety. The acrylic functionality composition may be comprised of homopolymers, copolymers, and/or mixtures thereof, having acrylic functionality or mixtures thereof, with other materials.
DESCRIPTION OF THE INVENTION
The ketone polymers (hereinafter referred to polyketones) of this invention preferably comprise an alternating structure which contain substantially one molecule of carbon monoxide for each molecule of unsaturated compound. Suitable unsaturated compounds for use as precursors of the ketone polymers are hydrocarbons having up to 20 carbon atoms inclusive, preferably up to 10 carbon atoms, and are aliphatic such as ethylene and other &agr;-olefins including propylene, 1-butene, isobutylene, 1-octene and 1-dodecene, or are arylaliphatic, cycloaliphatic or olefinic compounds with other functional groups such as unsaturated compounds containing an aryl substituent or containing acrylic, acetate and the like. Illustrative of this latter class of unsaturated compounds are styrene, p-methylstyrene, p-ethylstyrene or m-isopropylstyrene, acrylonitrile, methyl methacrylate and the like. The preferred ketone polymers are copolymers of carbon monoxide and ethylene or terpolymers of carbon monoxide, ethylene and a second ethylenically unsaturated hydrocarbon of at least 3 carbon atoms, particularly an a-olefin such as propylene.
Of particular interest are the polyketones of number average molecular weight from about 1000 to about 200,000, particularly those of number average molecular weight from about 20,000 to about 90,000 as determined by gel permeation chromatography. The physical properties of the polymer will depend in part upon the molecular weight, whether the polymer is a copolymer or a terpolymer and, in the case of the terpolymers, the nature and the proportion of the second unsaturated compound present Typical melting points for the polymers are from about 175° C. to about 280° C., more typically form about 180° C. to about 260° C. The polymers have a limiting viscosity number (LVN), measured in m-cresol at 60° C. in a standard capillary viscosity measuring device, from about 0.3 dl/g to about 10 dl/g, more frequently from about 0.5 dl/g to about 2 dl/g.
A method for the production of the polyketones is illustrated by U.S. Patent No. 4,843,144 (VanBroekhoven, et al.) which has been incorporated herein by reference.
The polyketones compositions of the invention comprise an intimate blend of a polyketone and a fibrous component which fibrous component has in combination therewith a composition having acrylic functionality. The blend may be prepared by mixing the components under heat and/or pressure.
The reinforcing agent is a filamentous fiber treated with a composition comprising an acrylic functionality moiety. The acrylic functionality fiber treating material may be admixed with the polyketone and fibers, but is preferably coated on the surface of the fibers before blending with the polyketone. Preferably, the filamentous fibers are glass fibers. For compositions ultimately to be employed for electrical uses, it is preferred to use fibrous glass filaments comprised of lime-aluminum borosilicate glass that is relatively sodium free. This is known as “E” glass. However, other glass compositions are useful as well. All such glasses are contempla
de Wit Gerrit
Gosens Johannes
Lohmeijer Johannes
General Electric Company
Rajguru U. K
Seidleck James J.
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