Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Mixing of two or more solid polymers; mixing of solid...
Reexamination Certificate
2000-05-17
2004-01-06
Woodward, Ana (Department: 1711)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Mixing of two or more solid polymers; mixing of solid...
C525S390000, C525S436000
Reexamination Certificate
active
06673872
ABSTRACT:
BACKGROUND OF THE INVENTION
High performance thermoplastic polymers such as poly(etherimide)s have been used to fabricate parts for numerous applications. Each application requires particular tensile and flexural properties, impact strength, heat distortion temperature (HDT), and resistance to warp. For example, U.S. Pat. No. 4,455,410 provides a poly(etherimide)-poly(phenylene sulfide) blend having good flexural strength characteristics. U.S. Pat. No. 3,983,093 provides poly(etherimide) compositions that have improved solvent resistance and are suitable for use in preparing films, molding compounds, coatings, and the like.
These thermoplastic polymers are characterized by a high glass transition temperature, usually above about 180° C., which makes them suitable for use in applications that require exposure to high temperatures. A drawback of these materials is that they exhibit poor melt flow properties, which makes processing difficult. Injection molding of thermoplastic polymers, for instance, is more easily performed with a thermoplastic resin that has a higher melt volume rate (MVR). Good melt flow properties are necessary to achieve fast molding cycles and to permit molding of complex parts. At the same time, mechanical properties such as impact strength and ductility must be maintained in order to pass product specifications.
U.S. Pat. No. 4,431,779 to White et al. discloses blends of polyetherimide and polyphenylene ether which exhibit good impact strength as well as good mechanical properties. White et al. focus on the comparability of polyphenylene ethers with polyetherimide, teaching that homogenous blends and non-uniform products may result. However, if amorphous polymers are employed, they are compatible and transparent films may be cast. The compatibility of the polyphenylene ethers to polyetherimide lessens as the quantity of aliphatic groups in the polymer increases. Although White et al. discuss polypheneylene ether polymers, they fail to teach the effects of such polymers and polymer blends on melt flow characteristics.
There accordingly remains a need in the art for thermoplastic polymers with improved melt flow properties, without the consequent loss of other desirable characteristics in the finished product.
BRIEF SUMMARY OF THE INVENTION
The above-described needs are met by a high performance, thermoplastic polymer composition having improved melt flow properties, comprising a high Tg, thermoplastic polymer resin and a poly(arylene ether) having a low intrinsic viscosity, preferably less than about 0.25 deciliters per gram (dl/g). Addition of low intrinsic viscosity poly(arylene ether)s generally have no or minimal detrimental effects on other physical properties of the thermoplastic polymer compositions.
DETAILED DESCRIPTION OF THE INVENTION
Addition of a poly(arylene ether) having a low intrinsic viscosity (IV) to high performance, high Tg, amorphous thermoplastic polymers provides highly improved melt flow properties to such polymers, without causing degradation of important mechanical properties such as impact strength and ductility. Other optional additives may also be used in the compositions to obtain other desired polymer properties.
Suitable high performance, high Tg thermoplastic polymer resins are known in the art, and typically have glass transition temperatures (Tg) of about 170° C. or greater, with about 200° C. or greater preferred. Exemplary resins include poly(imide), poly(sulfone), poly(ether sulfone), and other polymers.
Useful thermoplastic poly(imide) resins have the general formula (I):
wherein a is more than 1, typically about 10 to about 1,000 or more, and more preferably about 10 to about 500; and V is a tetravalent linker without limitation, as long as the linker does not impede synthesis or use of the polyimide. Suitable linkers include but are not limited to: (a) substituted or unsubstituted, saturated, unsaturated or aromatic monocyclic and polycyclic groups having about 5 to about 50 carbon atoms, (b) substituted or unsubstituted, linear or branched, saturated or unsaturated alkyl groups having 1 to about 30 carbon atoms; or combinations comprising at least one of the foregoing. Suitable substitutions and/or linkers include, but are not limited to, ethers, epoxides, amides, esters, and combinations comprising at least one of the foregoing. Preferred linkers include but are not limited to tetravalent aromatic radicals of formula (II), such as:
wherein W is a divalent moiety selected from the group consisting of —O—, —S—, —C(O)—, —SO
2
—, C
y
H
2y
—, C
y
H
2y-2
— (y being an integer from 1 to 10), and halogenated derivatives thereof, including perfluoroalkylene groups, or a group of the formula —O—Z—O— wherein the divalent bonds of the —O— or the —O—Z—O— group are in the 3,3′, 3,4′, 4,3′, or the 4,4′ positions, and wherein Z includes, but is not limited, to divalent radicals of formula (III):
R in formula (I) includes but is not limited to substituted or unsubstituted divalent organic radicals such as: (a) aromatic hydrocarbon radicals having about 6 to about 20 carbon atoms and halogenated derivatives thereof; (b) straight or branched chain alkylene radicals having about 2 to about 20 carbon atoms; (c) cycloalkylene radicals having about 3 to about 20 carbon atoms, or (d) divalent radicals of the general formula (IV):
wherein Q includes but is not limited to a divalent moiety selected from the group consisting of —O—, —S—, —C(O) —, —SO
2
—, C
y
H
2y
—, C
y
H
2y-2
— (y being an integer from 1 to 10), and halogenated derivatives thereof, including perfluoroalkylene groups.
Preferred classes of poly(imide) polymers include poly(amide imide) polymers and poly(etherimide) polymers, particularly those poly(etherimide) polymers known in the art which are melt processable, such as those whose preparation and properties are described in U.S. Pat. Nos. 3,803,085 and 3,905,942, each of which is incorporated herein by reference.
Preferred poly(etherimide) resins comprise more than 1, typically about 10 to about 1000 or more, and more preferably about 10 to about 500 structural units, of the formula (V):
wherein T is —O— or a group of the formula —O—Z—O— wherein the divalent bonds of the —O— or the —O—Z—O— group are in the 3,3′, 3,4′, 4,3′, or the 4,4′ positions, and wherein Z includes, but is not limited, to divalent radicals of formula (III) as defined above.
In one embodiment, the poly(etherimide) may be a copolymer which, in addition to the etherimide units described above, further contains poly(imide) structural units of the formula (VI):
wherein R is as previously defined for formula (I) and M includes, but is not limited to, radicals of formula (VII):
The poly(etherimide) can be prepared by any of the methods known to those skilled in the art, including the reaction of an aromatic bis(ether anhydride) of the formula (VIII):
with an organic diamine of the formula (IX):
H
2
N—R—NH
2
(IX)
wherein T and R are defined as described above in formulas (I) and (IV).
Examples of specific aromatic bis(ether anhydride)s and organic diamines are disclosed, for example, in U.S. Pat. Nos. 3,972,902 and 4,455,410, which are incorporated herein by reference. Illustrative examples of aromatic bis(ether anhydride)s of formula (VIII) include: 2,2-bis[4-(3,4-dicarboxyphenoxy)phenyl]propane dianhydride (i.e., the dianhydride of bisphenol-A); 4,4′-bis(3,4-dicarboxyphenoxy)diphenyl ether dianhydride; 4,4′-bis(3,4-dicarboxyphenoxy)diphenyl sulfide dianhydride; 4,4′-bis(3,4-dicarboxyphenoxy)benzophenone dianhydride; 4,4′-bis(3,4-dicarboxyphenoxy)diphenyl sulfone dianhydride; 2,2-bis[4-(2,3-dicarboxyphenoxy)phenyl]propane dianhydride; 4,4′-bis(2,3-dicarboxyphenoxy)diphenyl ether dianhydride; 4,4′-bis(2,3-dicarboxyphenoxy)diphenyl sulfide dianhydride; 4,4′-bis(2,3-dicarboxyphenoxy)benzophenone dianhydride; 4,4′-bis(2,3-dicarboxyphenoxy)diphenyl sulfone dianhydride; 4-(2,3-dicarboxyphenoxy)-4′-(3,4-dicarboxypheno
Merfeld Glen D.
Oshinski Alan
Puyenbroek Robert
van Beek Franciscus Johannes Maria
Zarnoch Kenneth Paul
General Electric Company
Woodward Ana
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