Mineral filled moldable thermoplastic composition

This invention is directed to an improved thermoplastic molding composition having an admixture of thermoplastic polymer or blends thereof and a particular mineral additive having needle like particles and a high aspect ratio of length to diameter. The composition when molded with the final article has improved surface characteristics, even a Class A surface, a lower coefficient of thermal expansion, as well as other improved properties, particularly impact as determined by Dynatup testing. The mineral additive can range from 5 to 70 weight percent. The polymer portion can be a copolyetherimide ester, a copolyether ester, an aromatic polycarbonate, a rubber modified homopolymer, or copolymer of a vinyl aromatic monomer, a polyphenylene ether, a polyamide, and blends thereof or blends with other polymers. The preferred mineral additive is calcium meta silicate, also known as wollastonite.

FIELD OF THE INVENTION 
The present invention is directed to an improved moldable thermoplastic 
composition having in admixture a particular polymer or blends of 
particular polymers and a particulate mineral additive. The particulate 
mineral additive of this invention has needle like particles of a 
relatively small diameter and having a high aspect ratio of length to 
diameter. A molded article employing the composition of this invention can 
have a lower coefficient of thermal expansion (CTE) and/or a high 
distinctness of image (DOI), which results in a molded article that can 
have a Class A surface, or an improved surface, as well as other improved 
properties, particularly impact when compared to other mineral additives. 
A Class A surface has been defined in many different ways with no universal 
definition. One accepted definition is a glossy, smooth and polished 
surface which should be as smooth as that of a current automobile exterior 
part made from sheet metal. Another definition is that the visible surface 
of the article in the finished state is free of exposed glass fibers, 
flash, sharp edges, visible parting lines, crazing, porosity, hair line 
cracks, blisters, and obvious repairs. In the present invention, another 
way of determining a Class A surface is based on the distinctiveness of 
image (DOI), which is a determination or measurement of reflective light 
waves. 
The compositions of the present invention are useful in many applications, 
but particularly in automotive exterior body panel applications such as 
fascia and side cladding parts, and can even find use in such parts as 
fenders, hoods, panels, trunk lids, door panels, etc. Due to the bake oven 
temperatures employed during painting of the automobile, as low a 
coefficient of thermal (CTE) expansion is wanted so as to obtain as close 
tolerances as possible between molded thermoplastic parts or between 
plastic and metal parts but still retain all other valuable properties of 
the thermoplastic parts being used. In other words, the parts would have 
predictable finished dimensions. In addition, the parts made with the 
compositions of this invention can have a Class A surface as measured by 
distinctness of image (DOI), which is a measure of reflective light waves. 
DESCRIPTION OF RELATIVE ART 
U.S. Pat. No. 5,091,461 discloses and claims an amorphous polymer matrix 
and an organic filler having improved properties of reduced coefficient of 
thermal expansion, high falling dart impact resistance and good resistance 
to heat under load. The composition consists of an aromatic polycarbonate, 
a rubber modified homopolymer or copolymer, such as 
acryonitrile-butadiene-styrene (ABS) and an inorganic filler having a 
particle size of a diameter of less than 44 microns (.mu.m) and a diameter 
to thickness ratio of 4 to 24. The inorganic fillers disclosed, however, 
are clays and talcs. The patent also discloses that the filler's large 
dimension is the diameter and the thickness is the small dimension showing 
that the filler is more of a plate shape particle or a flake shaped 
particle. 
With the ever increasing use of plastics in automotive application, 
particularly external parts thereof, there is a need for plastic parts 
that have a low coefficient of thermal expansion and stability under the 
high heat of the baking ovens. This is to avoid excessive expansion of the 
plastic parts under heat which would result in buckling or misfit such as, 
for example, a fender or a door of an automobile. Also important is impact 
resistance, particularly in such parts as fascia and side cladding, which 
is a plastic strip running along the lower part of the outside of the 
automobile, as well as in other exterior automotive body parts. It is also 
important that such molded parts have a Class A surface. 
When using such fillers as glass fibers, mica, glass flake, clay, or talc 
fillers not having the particular particle size of this invention in 
thermoplastic compositions, one or more of the desired properties is 
affected, such as DOI is lowered (which is a measure of the surface 
smoothness), brittleness occurs, poor resistance to impact, little or no 
CTE reduction, etc. 
Therefore, it is an object of this invention to provide an improved 
thermoplastic molding composition having a lower coefficient of thermal 
expansion. 
Another object of this invention is to provide an improved thermoplastic 
molding composition which when molded can result in a Class A surface as 
determined by distinctness of image. 
Yet another object of this invention is to provide an improved 
thermoplastic molding composition which when molded has improved surface 
characteristics. 
Still another object of this invention is to provide an improved 
thermoplastic molding composition which when molded has improved impact 
resistance. 
DETAILED DESCRIPTION OF THE INVENTION 
In accordance with the present invention, there is provided an improved 
thermoplastic molding composition having, in the molded state, a lower 
coefficient of thermal expansion (CTE) and a higher distinctness of image 
(DOI) comprising in intimate admixture of (1) a thermoplastic polymer 
which may be either a copolyetherimide ester, a polyalkylene 
terephthalate, an aromatic polycarbonate, a rubber modified homopolymer or 
copolymer of a vinyl aromatic monomer, a polyphenylene ether, a polyamide, 
blends thereof, or blends thereof with other polymers, and (2) a fine 
needle like particulate mineral additive wherein the needle like particles 
have a mean number average length of about 1.0 .mu.m to about 50 .mu.m and 
a mean number average diameter of about 0.1 .mu.m to about 10 .mu.m. The 
thermoplastic polymer portion of the intimate admixture of this invention 
is preferable at least about 30 to about 95 weight percent and more 
particularly at least about 50 to about 95 weight percent. The mineral 
additive portion of the intimate admixture is preferably about 70 to about 
5 weight and more particularly about 50 to about 5 weight percent the 
weight percents being based on the total weight of the thermoplastic 
molding composition disclosed herein. 
The copolyetherimide esters that may be employed in this invention consist 
of a multiplicity of recurring long chain ester units and short chain 
ester units that can be joined through imido-ester linkages. The hard 
segments of these elastomers consist essentially of multiple short chain 
ester units represented by the formula: 
##STR1## 
wherein R is a divalent radical remaining after removal of carboxyl groups 
from an aromatic dicarboxylic acid having a molecular weight less than 
about 300, and D is a divalent radical remaining after removal of hydroxyl 
groups from a diol having a molecular weight less than about 250; provided 
said short chain ester units amount to about 20-85 percent by weight of 
said copolyetherimide ester. 
The soft segments of these polymers are derived from poly(oxyalkylene 
diimide) diacid which can be characterized by the following formula: 
##STR2## 
Wherein, each R" is independently a trivalent organic radical, preferably 
a C.sub.2 to C.sub.20 aliphatic, aromatic or cycloaliphatic trivalent 
organic radical; R' is independently hydrogen or a monovalent organic 
radical preferably selected from the group consisting of C.sub.1 to 
C.sub.6 aliphatic and cycloaliphatic radicals and C.sub.6 to C.sub.12 
aromatic radicals, e.g., benzyl, much preferably hydrogen; and G' is the 
radical remaining after the removal of the terminal (or as nearly terminal 
as possible) amino groups of a long chain ether diamine having an average 
molecular weight of from about 600 to about 12,000, preferable from about 
900 to about 4,000, and a carbon-to-oxygen ratio of from 1.8 to about 4.3. 
These long chain ether glycols from which the polyoxyalkylene diamine is 
prepared include poly (ethylene ether) gylcol; poly(propylene ether) 
glycol; poly(tetramethylene ether) gylcol; random or block copolymers of 
ethylene oxide and propylene oxide, including propylene oxide terminated 
poly (ethylene ether) gylcol; and random or block copolymers of 
tetrahydrofuran with minor amounts of a second monomer such as methyl 
tetrahydrofuran. Especially preferred poly(alkylene ether) gylcols are 
poly(propylene ether) gylcol and poly(ethylene ether) gylcol end capped 
with poly(propylene ether) gylcol and/or propylene oxide. 
The tricarboxylic component is a carboxylic acid anhydride containing an 
additional carboxylic group or the corresponding acid thereof containing 
two imide forming vicinal carboxyl groups in lieu of the anhydride group. 
Mixtures thereof are also suitable. The additional carboxylic group must 
be esterified and preferably and substantially nonimidizable. 
Further, while trimellitic anhydride is preferred as the tricarboxylic 
component, any of a number of suitable tricarboxylic acid constituents 
will occur to those skilled in the art. 
Generally, the thermoplastic elastomers comprise the reaction product of 
dimethyltherephthalate, preferably with up to about 40 mole percent of 
another dicarboxylic acid; 1,4-butanediol, generally, with up to about 40 
mole percent of another saturated or unsaturated aliphatic and/or 
cycloaliphatic diol, and a polyoxyalkylene diamide diacid prepared from a 
polyoxyalkalene diamine of molecular weight, about 600 to about 12,000, 
preferable from about 900 to about 4,000, and trumellitic anhydride. 
Mixtures of two different diols can be employed, such as 1,4-butanediol 
and 1,4-butene-diol. 
The polyetherimide esters described herein and the procedures for their 
preparation are more fully described in U.S. Pat. Nos. 3,123,192, 
3,763,109; 3,651,014; 3,663,655; and 3,801,547 incorporated herein by 
reference. 
The preparation of the copolyetherimide ester is more fully described in 
U.S. Pat. No. 4,556,705, also incorporated herein by reference. 
Another thermoplastic resin that may be employed in the practice of this 
invention are the copolyether esters which also consist of a multiplicity 
of recurring long chain ester units and short chain ester units, joined 
head-to-tail through ester linkages. The long chain ester units are 
represented by the formula: 
##STR3## 
and the said short chain ester units are represented by the formula: 
##STR4## 
wherein G is a divalent radical remaining after the removal of terminal 
hydroxyl groups from a poly(alkyleneoxide) glycol having a number average 
molecular weight of about 400 to about 6,000 and a carbon to oxygen atomic 
ratio of about 2.0-4.3; R is a divalent radical remaining after removal of 
carboxyl groups from an aromatic dicarboxylic acid having a molecular 
weight of less than about 300 and D is a divalent radical remaining after 
removal of hydroxyl groups from a diol having a molecular weight less than 
about 250; provided said short chain ester units amount to about 25-70 
percent by weight of said copolyetherester. 
A more detailed description of suitable copolyether esters and procedures 
for their preparation are further described in U.S. Pat. Nos. 3,023,192; 
3,651,014; 3,763,109; 3,766,146; and 4,355,155, which are incorporated 
herein by reference. 
The high molecular weight polyalkylene terephthalates are another 
thermoplastic resin that may be employed in the practice of the present 
invention, and they are polyesters derived from an aliphatic or 
cycloaliphatic diol or mixtures thereof, containing 2 or more carbon atoms 
and at least one aromatic dicarboxylic acid. The polyester which are 
utilized herein are available commercially or can be prepared by known 
techniques, such as by the alcoholysis of esters of the phthalic acid or 
combination of phthalic acids with an aliphatic diol and subsequent 
polymerization, by heating the diol with the free acids or with halide 
derivatives thereof, and similar processes. These are described in U.S. 
Pat. Nos. 2,465,319 and 3,047,539, and elsewhere. 
One class of preferred polyesters employed in the practice of this 
invention will be of the family consisting of high molecular weight, 
polymeric aliphatic terephthalates and/or isophthalates having repeating 
units of the general formula: 
##STR5## 
wherein n is a whole number of from two to four, and mixtures of such 
esters, including copolyesters of terephthalic and isophthalic acids of up 
to about 30 mole percent of isophthalic units. 
Especially preferred polyesters are poly(ethylene terephthalate) and 
poly(1,4-butylene terephthalate), although poly(propylene terephthalate) 
may also be employed herein. 
Illustratively, high molecular weight polyesters will have an intrinsic 
viscosity of at least about 0.4 deciliters/gram and, preferably, at least 
about 0.7 deciliters/gram as measured in a 60:40 phenol tetrachloroethane 
mixture at 30.degree. C. At intrinsic viscosities of at least about 1.1 
deciliters/gram, there is a further enhancement in toughness of the 
present compositions. 
Also included within the scope of the present invention with respect to the 
high molecular weight linear polyesters are combinations of polybutylene 
terephthalates and polyethylene terephthalates. The combinations may be 
blends thereof, or blends of copolymers of polybutylene terephthalate and 
polyethylene terephthalate with homopolymers of polybutylene 
terephthalate, or copolymers of the two polyesters. The preferred 
combination is a blend of polybutylene terephthalate and polyethylene 
terephthalate. Although during extrusion of the blend of the two 
polyesters, some copolymer may be formed, probably in about the 5 weight 
percent range. Normally, a phosphorous stabilizer is added, particularly a 
phosphite, in order to inhibit the formation of the copolymer of the 
polybutylene terephthalate and the polyethylene terephthalate. In the 
blends thereof, the composition will generally consist essentially of 
about 30 to 70 and preferably 40 to 60 parts by weight of the polybutylene 
terephthalate and correspondingly about 70 to 30 parts and preferably 
about 60 to 40 parts by weight of the polyethylene terephthalate, the 
parts by weight being based on the total weight of the polybutylene 
terephthalate and polyethylene terephthalate. 
Also contemplated herein are the above polyesters with minor amounts, e.g., 
from 0.5 to about 2 percent by weight, of units derived from aliphatic 
acids and/or aliphatic polyols, to form copolyesters. The aliphatic 
polyols include glycols such as poly(ethylene glycol). These can be made 
following the teachings of, for example, U.S. Pat. Nos. 2,465,319 and 
3,047,539. 
Among the units which can be present in the copolyesters are those derived 
from aliphatic dicarboxylic acids, e.g., of up to and above about 50 
carbon atoms, including cycloaliphatic straight and branched chain acids, 
such as adipic acid, cyclohexanediacetic acid, dimerized C.sub.16 
-C.sub.18 unsaturated acids (which have 32 to 36 carbon atoms), trimerized 
acids, and the like. 
Another preferred class of polyesters employed in the present invention are 
derived from a cycloaliphatic diol and an aromatic dicarboxylic acid 
prepared by condensing either the cis- or trans-isomer (or mixtures 
thereof) of, for example, 1,4-cyclohexanedimethanol with the aromatic 
dicarboxylic acid so as to produce a polyester having recurring units 
having the following formula: 
##STR6## 
wherein the 1,4-cyclohexane dimethanol is selected from the cis- and 
trans-isomers thereof and R.sub.10 represents an aryl radical containing 6 
to 20 carbon atoms and which is the decarboxylated residue derived from an 
aromatic dicarboxylic acid. 
Examples of aromatic dicarboxylic acids indicated by R.sub.10 in the 
formula above include isophthalic or terephthalic acid, 
1,2-di(p-carboxyphenyl)ethane, 4,4'dicarboxydiphenyl ether, etc., and 
mixtures of these. All of these acids contain at least one aromatic 
nucleus. Fused rings can also be present such as in 1,4 or 1,5 
naphthalene-dicarboxylic acids. The preferred dicarboxylic acid is 
terephthalic acid or mixtures of terephthalic and isophthalic acid. 
A preferred polyester may be derived from the reaction of either the cis- 
or trans-isomer (or a mixture thereof) of 1,4-cyclohexanedimethanol with a 
mixture of iso- and terephthalic acids. These polyesters have repeating 
units of the formula: 
##STR7## 
Another preferred polyester is a copolyester derived from a 
cyclohexanedimethanol, an alkylene glycol and an aromatic dicarboxylic 
acid. These copolyesters are prepared by condensing either the cis- or 
trans-isomer (or mixtures thereof) of, for example, 
1,4-cyclohexanedimethanol and an alkylene glycol with an aromatic 
dicarboxylic acid so as to produce a copolyester having repeating units of 
the following formula: 
##STR8## 
wherein the 1,4-cyclohexanedimethanol is selected from the cis- and 
trans-isomers thereof, R.sub.10 is a previously defined, .sub.n is an 
integer of 2 to 4, the c units comprise from about 10 to about 90 percent 
by weight, and the d units comprise from about 10 to about 90 percent by 
weight. 
The preferred copolyesters may be derived from the reaction of either the 
cis- or trans-isomer (or mixtures thereof) of 1,4-cyclohexanedimethanol 
and ethylene glycol with terephthalic acid in, for example, a molar ratio 
of 1:2:3. These copolyesters have repeating units of the following 
formula: 
##STR9## 
wherein c and d are as previously defined. 
The polyesters are described herein are either commercially available or 
can be produced by methods well known in the art such as those set forth 
in, for example, U.S. Pat. No. 2,901,466. 
The preferred cycloaliphatic polyesters are poly(1,4-cyclohexanedimethanol 
tere/iso-phthalate) and a copolyester of 1,4-cyclohexanedimethanol, 
ethylene glycol and terephthalic acid and poly(ethylene terephthalate) as 
previously described. 
The polyesters used herein have an intrinsic viscosity of at least about 
0.4 and may be as high as about 2.0 dl/g. measured in a 60:40 
phenol/tetrachloroethane mixture of similar solvent at 
23.degree.-30.degree. C. 
The aromatic polycarbonates employed in the instant invention are well 
known polymers and are disclosed in many U.S. patents such as U.S. Pat. 
Nos. 2,999,835, 3,038,365, 3,334,154, and 4,131,575, all of which are 
incorporated herein by reference. Such aromatic polycarbonates are 
prepared from dihydroxy phenols and carbonate precursors. The 
polycarbonates suitable for use in the instant invention generally have a 
number average molecular weight of from about 8,000 to about 80,000 and 
preferably from about 10,000 to about 50,000 and an intrinsic viscosity 
(I.V.) of about 0.35 to about 1.0 deciliters per gram (dl/g) as measured 
in methylene chloride at 25.degree. C. 
Suitable dihydroxy phenols employed in the preparation of the 
polycarbonates include for example 2,2-bis(4-hydroxyphenyl)propane, 
bis(4-hydroxyphenyl) methane, 2,2-bis(4-hydroxy-3-methylphenyl) propane, 
4,4-bis(4-hydroxyphenyl)heptane, 
2,2,-(3,5,3',5'-tetrachloro-4,4'-dihydroxyphenyl)propane, 
2,2-(3,5,3',5'tetrabromo-4,4'-dihydroxyphenyl)propane, and 
3,3'-dichloro-4,4'-dihydroxydiphenyl)methane. Other dihydroxy phenols 
which are also suitable for use in the preparation of the above 
polycarbonates are also disclosed in the above references which have been 
incorporated herein by reference. 
It is of course possible to employ two or more different dihydroxy phenols 
in preparing the polycarbonates of the invention. In addition, branched 
polycarbonates such as those described in U.S. Pat. No. 4,001,184 can also 
be utilized in the practice of the instant invention, as well as blends of 
a linear aromatic polycarbonate and a branched aromatic polycarbonate. The 
branched polycarbonate resins may be prepared by reacting (i) at least one 
dihydroxy phenol of the type described herein, (ii) a carbonate precursor, 
and (iii) a minor amount of a polyfunctional organic compound. The 
polyfunctional organic compounds used in making the branched 
polycarbonates are well known in the art and are disclosed, for example, 
in the U.S. Pat. Nos. 3,525,712; 3,541,049; 3,544,514; 3,635,895; 
3,816,373; 4,001,184; 4,294,953, and 4,204,047, all of which are hereby 
incorporated herein by reference. These polyfunctional organic compounds 
are generally aromatic in nature and contain at least three functional 
groups which may be, for example, hydroxyl, carboxyl, carboxylic 
anhydride, haloformyl, and the like. Some illustrative non-limiting 
examples of these polyfunctional compounds include trimellitic anhydride, 
trimellitic acid, trimellityl trichloride, 4-chloroformyl phthalic 
anhydride, pyomellitic dianhydride, mellitic acid, mellitic anhydride, 
trimesic acid, benzophenonetetracarboxylic acid, 
benzophenonetetracarboxylic acid, benzophenone-tetracarboxylic anhydride, 
and 4,6-dimethyl-2,4,6-tri-(4-hydroxyphenyl) heptene-2. The amount of this 
polyfunctional organic compound or branching agent used is in the range of 
from about 0.05 to about 2 mole percent based on the amount of dihydric 
phenol employed, and preferable from about 0.1 to about 1 mole percent. 
The processes for preparing the polycarbonate employed in the instant 
invention are well known in the art. There are many patents fully 
describing the preparation of the polycarbonates including those recited 
previously herein, and as well as U.S. Pat. No. 4,937,130 and U.S. Pat. 
No. 4,513,037, both of which are incorporated herein by references. 
As described in the prior art, a carbonate precursor is employed to prepare 
the polycarbonates such as a carbonyl halide, a carbonate ester or a 
haloformate. Typically, the well known carbonate precursor is a carbonyl 
chloride. A typical carbonate ester is diphenyl carbonate. A typical 
haloformate is a bishaloformate of a dihydroxyphenol such as the 
bishaloformate of ethylene glycol. The above carbonate precursors are 
merely typical or those that can be employed and are not intended to be 
limiting. Such carbonate precursors are also well known in the art and are 
listed in the prior art cited previously herein. 
The polycarbonate employed herein may also be a copolyestercarbonate as 
described in U.S Pat. No. 4,430,484 and in the other references cited in 
U.S. Pat. No. 4,430,484, which is incorporated herein by reference. 
Preferred polyestercarbonates are those derived from the dihydroxyphenols 
and carbonate precursors described above and aromatic dicarboxylic acids 
or their relative derivatives thereof, such as the acid dihalides, e.g. 
dichlorides. In addition, a mixture of dicarboxylic acids can be employed 
such as terephthalic acid and isophthalic acid. Further, their respective 
acid chlorides can also be used. Thus, a useful class of aromatic 
polyestercarbonates are those prepared from bisphenol-A, terephthalic acid 
or isophthalic acid or a mixture thereof and a carbonyl chloride also 
known as phosgene. These copolyestercarbonates are also commonly known as 
polyphthalate carbonates and are also described in U.S. Pat. No. 
4,465,820, incorporated herein by reference. 
Rubber modified homopolymers and copolymers of vinyl aromatic monomers that 
can be employed in the present invention include the rubber modified 
homopolymers and copolymers of styrene or a-methylstyrene with a 
copolymerizable comonomer. Preferred comonomers include acrylonitrile 
which may be employed alone or in combination with other comonomers, 
particularly methylmethacrylate, methacrylonitrile, fumaronitrile and/or 
an N-arylmaleimide such as N-phenylmaleimide. Highly preferred copolymers 
contain from about 70 to about 80 percent styrene monomer and 30 to 20 
percent acrylonitrile monomer. 
Suitable rubbers include the well known homopolymers and copolymers of 
conjugated dienes, particularly butadiene, as well as other rubbery 
polymers such as olefin polymers, particularly copolymers of ethylene, 
propylene and optionally a nonconjugated diene, or acrylate rubbers, 
particularly homopolymers and copolymers of alkyl acrylates having from 4 
to 6 carbons in the alkyl group. In addition, mixtures of the foregoing 
rubbery polymers may be employed if desired. Preferred rubbers are 
homopolymers of butadiene and copolymers thereof with up to about 30 
percent by weight styrene. Such copolymers may be random or block 
copolymers, and, in addition, may be hydrogenated to remove residual 
unsaturation. 
The rubber modified copolymers are preferably prepared by a graft 
generating process such as by a bulk or solution polymerization or by 
emulsion polymerization of the copolymer in the presence of the rubbery 
polymer. In the emulsion polymerization to form graft copolymers of 
rubbery substrates, it is previously known in the art to employ 
agglomeration technology to prepare large and small rubber particles 
containing the copolymer grafted thereto. In the process, various amounts 
of an ungrafted matrix of the copolymer are also formed. In the solution 
or built polymerization of a rubber modified copolymer of a vinyl aromatic 
monomer, a matrix copolymer is formed. The matrix further contains rubber 
particles having copolymer grafted thereto occluded therein. 
A particularly desirable product comprises rubber modified copolymer blend 
comprising both the mass or solution polymerized rubber modified copolymer 
and additional quantities of an emulsion polymerized and preferably 
agglomerated rubber modified copolymer containing a bimodal particle-sized 
distribution. A most preferred rubber modified copolymer comprises a 
butadiene rubber modified copolymer. Butadiene rubber modified copolymers 
of styrene and acrylonitrile are referred to in the art as ABS resins. 
The polyphenylene esters employed in the practice of this invention are a 
well known class of compounds sometimes referred to as polyphenylene 
oxides. Examples of suitable polyphenylene ethers and processes for their 
preparation can be found in U.S. Pat. Nos. 3,3086,874; 3,3086,875; 
3,257,357; and 3,257,358 which are incorporated by reference. Compositions 
of the present invention will encompass homopolymers, copolymers and graft 
copolymers obtained by the oxidative coupling of phenolic compounds. The 
preferred polyphenylene ethers used as base resins in compositions of the 
present invention will be comprised of units derived from 3,6-dimethyl 
phenol. Also contemplated are PPE copolymers comprised of units derived 
from 2,6-dimethyl phenol and 2,3,6-trimethyl phenol. 
A particularly useful polyphenylene ether would be 
poly(2,6-dimethyl-1,4-phenylene ether) having an intrinsic viscosity 
(I.V.) greater than, approximately 0.10 dl/g as measured in chloroform at 
25.degree. C. The I.V. will typically be between 0.30 and 0.60 dl/g. 
The polyamide resins useful in the practice of the present invention are 
known as nylons, and are characterized by the presence of an amide group 
(--CONH--). Nylon-6 and nylon 6,6 are the generally preferred polyamides 
and are available from a variety of commercial sources. The polyamides may 
be either amorphous or crystalline polyamides. 
Typical examples of the polyamides or nylons, as these are often called, 
include for example polyamides 6, 6/6, 11, 12, 6/3, 6/4, 6/10, and 6/12, 
as well as polyamides resulting from terephthalic acid and/or isophthalic 
acid and trimethyl hexamethylene diamine, polyamides resulting from adipic 
acid and meta xylylenediamines, polyamides resulting from adipic acid, and 
metaxylylenediamines, polyamides resulting from adipic acid, azelaic acid 
and 2,2-bis-(p-aminocyclohexyl)propane and polyamides resulting from 
terephthalic acid and 4,4'-diamino-dicyclohexylmethane. Mixtures and/or 
copolymers of two or more of the foregoing polyamides or prepolymers 
thereof, respectively, are also within the scope of the present invention. 
Preferred polyamides are the polyamides 6, 6/6, 11, and 12, most 
preferably polyamide 6/6. 
It is also to be understood that the use of the term "polyamides" herein 
and in the appended claims is intended to include the toughened or super 
tough polyamides. Super tough polyamides, or super tough nylons, as they 
are more commonly known, are available commercially, e.g. from E. I. 
duPont under the tradename Zytel ST, or may be prepared in accordance with 
a number of U.S. Patents, including, among others, Epstein U.S. Pat. No. 
4,174,358; Novak U.S. Pat. No. 4,474,927; Roura U.S. Pat. No. 4,346,194; 
and Joffrion U.S. Pat. No. 4,251,644, all of which are herein incorporated 
by reference. These super tough nylons are prepared by blending one or 
more polyamides with one or more polymeric or copolymeric elastomeric 
toughening agents. Suitable toughening agents are disclosed in the 
above-identified U.S. Pat. Nos., as well as in Caywood, Jr. U.S. Pat. No. 
3,884,882 and Swiger U.S. Pat. No. 4,147,740 and Gallucci et al., 
"Preparation and Reactions of Epoxy-Modified Polyethylene", J. APPL. POLY. 
SCI. V. 27, pp. 425-437 91982) all incorporated herein by reference. 
Typically, these elastomeric polymers and copolymers may be straight chain 
or branched, as well as graft polymers and copolymers, including 
core-shell graft copolymers, and are characterized as having incorporated 
therein either by copolymerization or by grafting on the preformed 
polymer, a monomer having functional and/or active or highly polar 
groupings capable of interacting with or adhering to the polyamide matrix 
so as to enhance the toughness of the polyamide polymer. 
As stated previously, the thermoplastic composition of this invention may 
also comprise blends of the above polymers. An example of such blends may 
be blends of an aromatic polycarbonate and an ABS in a range of about 30 
to about 70 weight percent of polycarbonate and about 70 to about 30 
weight percent of ABS based on the weight of the polymers employed. In 
another system, a blend of the polycarbonate and a polyalkylene 
terephthalate (polybutylene terephthalate) may also be employed herein. 
Still another blend that may be employed in the practice of this invention 
is a blend of a polyphenylene ether and a polyamide. Yet another blend may 
be that of copolyetherimide ester or a copolyether ester and a 
polyalkylene terephthalate (PBT), or a blend of a polycarbonate, a 
polybutylene terephthalate (PBT) and ABS. The above blends are merely some 
of the typical blends that may be employed in the practice of this 
invention and other blends will become obvious to those skilled in the art 
in view of the disclosure herein. 
In addition, as stated previously, blends of the above polymers with other 
polymers are also included within the scope of the present invention. For 
example, blends of polyphenylene ether and a styrene polymer may be 
employed, such as NORYL.RTM. resin sold by General Electric Company. 
Copolymers of styrene and methyl-methacrylate may also be used herein with 
any of the polymers described above. Polyethylene and polycarbonate is 
another blend that may be employed herein. Again, these blends are merely 
representative of some of the blends that may be employed herein and other 
such blends will be obvious to those skilled in the art in view of the 
teachings disclosed herein. 
The mineral additive employed in the practice of this invention has needle 
like particles. While any such mineral additive may be employed herein, 
the particles should have the particle size distribution as disclosed 
herein. Preferably, the mineral filler consists essentially of calcium 
meta silicate, which is also referred to as calcium silicate, and more 
commonly as wollastonite. However, since the mineral is mined, other 
ingredients may also be present in wollastonite, such as trace amounts of 
aluminum oxide, magnesium oxide and/or iron oxide. Although wollastonite 
is identified as calcium meta silicate, there may be some free silicon 
dioxide present therein as well. The mineral filler of this invention 
consists essentially of needle like particles having a mean number average 
length of about 1.0 .mu.m to about 50 .mu.m and and a mean number average 
diameter of about 0.1 .mu.m to about 10 .mu.m. Preferably, at least 80 
percent of the needle like particles of the mineral additive have a length 
of about 5 .mu.m to about 40 .mu.m, and more specifically at least 50 
percent of the needle like particles have a length of about 5 .mu.m to 
about 25 .mu.m. This results in a number average aspect ratio of length to 
diameter of up to about 6 and preferably ranging from less than about 1.0 
to about 10. 
The preferred mineral additive employed in the present invention is 
wollastonite or also known as calcium meta silicate, having the particular 
particle morphology disclosed previously. Wollastonites are well known 
minerals and are used as fillers in thermoplastics. However, the known and 
previously employed wollastonites have a mean number average length of 
about 90 .mu.m, and a mean average diameter of about 15 .mu.m or greater. 
Also, at least 50 percent of the particles have a length ranging from 
about 15 .mu.m to over 50 .mu.m, with at least 80 percent of the particles 
ranging from 15 to about 150 .mu.m. 
It has also been found that when the composition of this invention is 
injection molded, the mineral additive particles may undergo a breaking or 
shearing, which may result in a decrease of the aspect ratio. Even though 
this shearing may occur, the mean average aspect ratio would probably 
still be within the range of less than about 1 to about 10. 
The object of this invention is to provide an improved thermoplastic 
molding composition as described previously having the advantage of 
providing molded articles having a lower CTE and a high or improved DOI. 
It has also been found that certain compositions of this invention are 
ductile compared to previously commonly employed wollastonites, as 
demonstrated in the Examples. It has further been unexpectedly discovered 
that the use of the particular wollastonite of this invention may also 
result in a higher DOI, as compared in previously employed wollastonites 
or other fillers. For example, as shown in the Examples, the use of the 
wollastonite of this invention greatly increased the DOI of the molded 
article over previously known fillers. In addition, the mineral filler 
herein disclosed also provides greater impact strength as determined by 
the Dynatup impact test, even though brittle breaks may occur. This is 
demonstrated in the Examples, wherein higher energy is required to break 
or pierce the sample, again in comparison to previously known 
wollastonite. This represents that even though the break may be brittle, 
greater impact is necessary in order to achieve breakage. The results show 
that a substantial greater energy is required, both at room temperature 
and at subzero temperatures. It is surprising that the substantial 
unexpected property increases that are achieved with the particular 
mineral additives of this invention. Even when employed in combination 
with other fillers, which are described hereinafter, dramatic increases in 
properties can be achieved. 
The mineral additive of this invention may act as a filler or it may act as 
a reinforcing agent or it may act as a combination of both. The particular 
mineral additive may also preferably have a surface treatment on the 
particles such as with a silane surface treatment such as an alkoxy silane 
or other type of coupling agent such as a titinate or zirconate for 
example. However, the critical feature of the present invention is that by 
employing the particular mineral additive disclosed herein, the results 
achieved as shown in the Examples are not achieved with previously known 
fillers such as carbon fibers, mica, talc, glass fibers, and even 
previously known wollastonites, other than the wollastonite having the 
particle morphology disclosed in this invention. 
In addition, it has also been unexpectedly discovered that articles molded 
from the improved composition of this invention may have a Class A 
surface. The test procedure employed in this invention for determining 
Class A surface is the distinctness of image (DOI) test procedure (as 
later described herein), which is a determination of the percentage of 
reflective light waves that are reflected from the surface of the molded 
article. The higher the percentage, the smoother is the surface. In the 
present invention, articles molded with the composition herein disclosed 
can have a DOI of greater than 95% as compared to lower DOI's for the same 
composition employing previously known fillers or reinforcing agents when 
molded under the same conditions. As is understood by those skilled in the 
art, the composition itself is an important and critical factor in 
obtaining a Class A surface. However, properly prepared surfaces of the 
mold employed in injection molding or whatever mold is employed in molding 
are also a factor in achieving a Class A surface along with the factor of 
the composition. With a dull or slightly imperfect mold surface, one may 
still obtain a Class A surface with an article molded from the composition 
of this invention. On the other hand, a roughened mold surface may well 
not produce a Class A surface on an article molded from the composition of 
this invention, regardless of the composition. All things being equal, 
i.e. a properly polished mold surface, molded articles molded from the 
composition of this invention can have a Class A surface as determined by 
the DOI. 
In addition, the composition of this invention may include other additives 
such as impact modifiers, heat and light stabilizers, flame retardants and 
other additives well known to those skilled in the art. An impact modifier 
can be an important additive where increased or improved impact resistance 
is wanted. While many known impact modifiers may be employed herein 
providing that the impact modifier employed enhances the impact properties 
of the molded article substantially without affecting the other physical 
properties of the composition of this invention, particularly useful are 
the rubbery shell-core type of impact modifiers. One type of shell-core 
impact modifier is the all acrylic modifier, i.e. one having a 
polyacrylate core such as polybutyl acrylate with a shell of a methyl 
methacrylate such as styrene methyl methacrylate or an acrylonitrile 
methyl methacrylate shell. Another type of shell-core impact modifiers is 
one having a polybutadiene core that is preferably a cross-linked 
polybutadiene core with an acrylate shell such as the same types of 
acrylate shells disclosed above. Sometimes it is advantageous to use 
linking compounds or linking monomers during the polymerization of the 
impact modifiers in order to link or bind the shell to the core. Another 
type of rubbery impact modifier that may be employed herein is 
styrene-butadiene-tyrene triblock copolymers, or 
styrene-ethylene/butylene-styrene triblock copolymers or styrene 
ethylene/propylene-styrene diblock copolymers. These are available from 
Shell Chemical which is sold under the trademark Kraton. The amount of 
impact modifier that may be optionally employed herein is about 0.5 to 
about 25 parts by weight based on the weight of the polymer, the mineral 
additive and the impact modifier. Such impact modifiers as described above 
are available commercially from various polymer manufacturers. 
Also contemplated as part of this invention are blends of mineral additives 
such as blends of the mineral additive of this invention with other 
fillers such as mica, talc, carbon black, or other minerals not having the 
needle like morphology of the mineral additive of this invention Even the 
blend of minerals produces improvement in such properties as DOI and/or 
the CTE, i.e. by lowering the CTE. For example, a blend of the polymers of 
this invention with just mica demonstrates (not with the mineral filler of 
this invention) that a low DOI is obtained on molded parts. However, when 
adding wollastonite having the particle morphology disclosed in this 
invention to a blend of a polymer and mica, the DOI is dramatically 
improved, and the CTE is lowered. This can also occur with blends of the 
mineral additive of this invention and other mineral additives. The use of 
such blends can produce lower CTE and better or improved DOI, as 
demonstrated in the Examples. The amount of other mineral additive that 
can be blended with the mineral additive of this invention should be that 
amount that does not affect the increased properties of CTE, DOI, impact, 
etc. obtained with the mineral additive of the invention. In effect, one 
can use a lower cost mineral additive in place of part of the mineral 
additive of this invention without significantly affecting the increased 
properties afforded by the instant additive disclosed herein. Preferably, 
the amount of mineral additive of this invention should be about at least 
50 percent by weight of the additive, and, more particularly, about at 
least 70 percent by weight with the balance being such other mineral 
additive not of the needle like particles disclosed herein. 
Also included within the scope of this invention, is the use of a blend of 
needle like particles having the morphology of the mineral additive of 
this invention. 
DESCRIPTION OF THE PREFERRED EMBODIMENTS 
The following Examples are set forth to illustrate the present invention 
and are not to be construed as limiting the scope of this invention 
thereto. Unless otherwise indicated, all parts and percentages are on a 
weight basis.

EXAMPLES 1-4 
All ingredients were dry blended in a laboratory tumbler. The blend was 
then fed to a twin screw 58 mm. co-rotating intermeshing extruder. The 
temperature of the extruder was at about 480.degree. F. to about 
520.degree. F. flat temperature profile along the extruder barrel, 
depending on the polymer used, and one skilled in the art would well know 
the temperature to use. The die temperature through which the composition 
was extruded was about the same temperature as the extruder barrel 
temperature, namely about 480.degree. F. to about 500.degree. F. The 
extrudate was pelletized and dried at a temperature of about 230.degree. 
F. for 2 hours in a hot air circulating oven. The pelletized compositions 
were then molded into test specimens using an 80 ton Van Dorn injection 
molding machine. The temperature of the molding machine was at about 
480.degree. F. to a about 500.degree. F. with a mold temperature of about 
150.degree. F., again depending on the polymer employed and would well be 
within the knowledge of one skilled in the art. The size of the test 
specimens varied depending on the test to be run. For notched IZOD impact, 
the tests specimens were about 3" long by 1/2" wide by 1/8" thick and were 
tested in accordance with ASTM D630A. For Dynatup impact testing and paint 
testing, the test specimens molded were about 4" in diameter by about 1/8" 
thick. The Dynatup test was performed under ASTM test procedure D3763-86 
using the Dynatup impact testing equipment by General Research 
Instruments. Briefly, the test procedure involves subjecting samples to a 
falling dart impact. The dart is about a 0.5" diameter rod about 1.5" long 
and has a rounded, blunt end, which is the end that impacts upon the 
sample. The molded sample is clamped in a holding device. The date is on a 
vertical sled or shaft, with weights added for energy impact 
determination. The test is designed to force failure of the sample in 
order to determine the type of failure occurring. The average velocity of 
the falling dart was about 11.3 feet per second, and the impact energy was 
100 foot-pounds, with a drop height of two feet. 
In the Dynatup impact test, the energy absorbed by the sample by the 
falling dart is plotted on a graph from the time the dart first hits the 
sample until it punctures through the sample. E(max) is the maximum energy 
absorbed by the sample at the peak of the graph, which is a chart of the 
energy absorbed by the sample. E(tot) is the total energy absorbed over 
the range of time the dart first hits the sample until it punctures 
through the sample. Generally, E(max) and E(tot) are the average of 
several samples for each formulation tested, as shown in the tables. 
The DOI test procedure was developed to determine the effect fillers in 
materials may have on specular gloss of the topcoat paint when no primer, 
sealer, surfacer, etc. is used. Some automobile parts are so prepared with 
topcoat only. Since DOI will vary depending on the paint color, a high 
gloss black automotive paint is used as the standard. This paint yields a 
DOI of 99+% when properly applied to unfilled materials, i.e. plastics 
without inorganic fillers such as glass, mica, clay, etc. Samples are all 
painted together with an automatic paint spraying machine (Spraymation 
#310740) to insure proper uniformity and repeatability of application 
parameters (flash time, paint thickness, etc.). When the paint is cured, 
the DOI is measured in several locations on each sample with a meter. An 
ATI model #1792 special gloss meter is used. The results are reported in 
the Tables below. 
The wollastonite of this invention employed in the Examples was NYGLOS 
wollastonite, having an average mean diameter based on number average of 
less than about 4.5 .mu.m and an average mean length of about 24 .mu.m. 
The wollastonite of the prior art employed in the Examples was NYAD G 
wollastonite, having an average mean diameter based on number average of 
about 16 .mu.m and an average mean length of about 90 .mu.m. Both 
wollastonites are from NYCO Company. The morphology of the NYGLOS and NYAD 
G wollastonites was determined on the raw material, i.e. before 
compounding with the particular resins and other additives to prepare the 
formulations set forth in the Tables. The method employed was light 
microscopy. Photomicrographs were made using transmitted bright field 
illumination on a Zeiss Photomicroscope interfaced to a Zeiss IBAS image 
analysis system. From the photomicrographs, particles were measured and 
number average mean results were obtained as reported above. Particle size 
distribution was also determined. 
The results of the above tests were as follows: 
TABLE 1 
______________________________________ 
Examples 1-4 
(parts) 
INGREDIENTS (by wt.) 
1 2 3 4 
______________________________________ 
PEIE (30) 37.2 37.2 37.2 37.2 
PBT 30.0 30.0 30.0 30.0 
IMP 12.0 12.0 12.0 12.0 
Stabilizer Package 
0.8 0.8 0.8 0.8 
NYGLOS 20.0 0 10.0 0 
Mica 0 0 10.0 10.0 
NYAD G 0 20.0 0 10.0 
PROPERTIES 
Notched, Izod foot-lbs/inch 
@ rm. temp. 10.8 7.2 4.1 4.3 
@ -30.degree. C. 
3.1 3.1 2.1 2.2 
Dynatup 
@ rm. temp. -- -- 2D 1D/1DSC 
.sup.E MAX/.sup.E TOT 16/18 14/16 
@ -30.degree. C. 
5D 1B/4* 5B 2B/3* 
.sup.E MAX/.sup.E TOT 
-- -- -- -- 
DOI (%) 99 73 87 73 
CTE (in./in./.degree. F. .times. 10.sup.-5 
3.24 6.47 5.06 4.97 
flow direction) 
______________________________________ 
PEIE (30) copolyetherimide ester LOMOD .RTM. JE630 by General Electric 
Company contains 30% by weight of polyethylene glycol 
PBT polybutylene terephthalate VALOX .RTM. 315 by General Electric 
Company 
IMP impact modifier BLENDEX .RTM. 338 ABS (70 wt. % butadiene, 22 wt. % 
styrene, 8 wt. % acrylonitrile) by General Electric Company 
Notched Izod ASTM D630A 
Dynatup ASTM D 376386 
Stabilizer Package tris nonyl phosphate (TNPP), Irganox 1010 (a phenolic 
anti oxident by Ciba Geigy, a thio ester and an epoxy) 
D ductile break 
B brittle break 
* star break 
Ductile break means penetration of the sample without cracks or breakaway 
fragments. 
Brittle means penetration of the sample with cracks and breakaway 
fragments. 
Star break means penetration of the sample with radial cracks like a star 
Mica Harco White Muscovite mica 
EXAMPLES 5-10 
Examples 1-4 were repeated, except that the ingredients and compositions 
were as reported in Table 2 below: 
TABLE 2 
__________________________________________________________________________ 
Examples 5-10 
(parts) 
INGREDIENTS (by wt.) 
5 6 7 8 9 10 
__________________________________________________________________________ 
PEIE (30) 44.5 44.5 21.7 
21.7 
0 0 
PEIE .sup.(1) 
0 0 0 0 74.3 
74.3 
PBT 37.7 37.7 17.5 
17.5 
0 0 
IMP 12.0 12.0 10.0 
10.0 
0 0 
NYGLOS 0 5.0 50.0 
0 0 25.0 
NYAD G 5.0 0 0 50.0 
25.0 
0 
Stabilizer Package 
0.8 0.8 0.8 0.8 0.7 0.7 
PROPERTIES 
Notched Izod (ft-lbs/in) 
@ rm. temp. 8.7 9.4 1.9 2.5 5.3 5.3 
@ -30.degree. C. 
4.6 9.4 1.3 1.7 4.0 2.7 
Dynatup 
@ rm. temp. -- -- -- -- -- -- 
.sup.E MAX/.sup.E TOT 
@ -30.degree. C. 
5B 5D 4B/1* 
5* 5B 5D 
.sup.E MAX/.sup.E TOT 
18.4/21.91 
16.9/31.61 
1.7/7.0 
2.5/9.8 
-- -- 
DOI (%) 85 98 91 44 73 99 
CTE (in/in/.degree. F. .times. 10.sup.-5 
5.95 5.42 2.37 
4.27 
5.99 
6.25 
flow direction) 
__________________________________________________________________________ 
PEIE .sup.(1) copolyetherimide ester LOMOD .RTM. J1013 by General 
Electric Company 
All other ingredients and tests run are the same as Table 1, except the 
Stabilizer Package of Examples 9 and 10 do not contain a thio ester. 
EXAMPLES 11-16 
Examples 1-4 were repeated, except that the formulations employed herein 
were as reported in Table 3, along with the results obtained. 
TABLE 3 
__________________________________________________________________________ 
Examples 11-16 
(parts) 
INGREDIENTS (by wt.) 
11 12 13 14 15 16 
__________________________________________________________________________ 
PET 32.1 32.1 15.0 
15.0 
0 0 
PBT 0 0 30.0 
30.0 
74.3 
74.3 
PC 32.0 32.0 19.1 
19.1 
0 0 
IMP 15.0 15.0 15.0 
15.0 
0 0 
NYGLOS 20.0 0 0 20.0 
25.0 
0 
NYAD G 0 20.0 20.0 
0 0 25.0 
Stabilizer Package 
0.9 0.9 0.9 0.9 0.7 0.7 
PROPERTIES 
Notched Izod (ft-lbs/in) 
@ rm. temp. 1.7 1.5 4.2 1.9 0.9 0.7 
@ -30.degree. C. 
0.7 0.9 0.6 0.6 0.7 0.7 
Dynatup 
@ rm. temp. 2B 2B 2B 2B 1B 1B 
.sup.E MAX/.sup.E TOT 
31/32 
6/6 19/21 
27/33 
2.0/2.0 
1.5/1.6 
@ -30.degree. C. 
5B 5B 5B 5B -- -- 
.sup.E MAX/.sup.E TOT 
7.0/7.6 
1.1/4.9 
1.1/4.3 
1.9/3.8 
-- -- 
DOI (%) 98 46 49 77 99 73 
CTE (in/in/.degree. F. .times. 10.sup.-5 
3.02 5.00 5.99 
3.99 
3.64 
4.69 
flow direction) 
__________________________________________________________________________ 
PET polyethylene terephthalateDuPont's CRYSTAR 3948 having an IV 0.57 
dl/gram 
PC polycarbonate LEXAN .RTM. 140 resin by General Electric Company 
IMP impact modifier KM 330, a shell core polyacrylate by Rohm & Haas Co 
All other ingredients and tests run are the same as Table 1, except 
Examples 15 and 16 do not contain thio ester in the Stabilizer Package. 
EXAMPLES 17-24 
Examples 1-4 were repeated, except that the formulations employed herein 
were as reported in Table 4, along with the results. 
TABLE 4 
__________________________________________________________________________ 
Examples 17-24 
(parts) 
INGREDIENTS (by wt.) 
17 18 19 20 21 22 23 24 
__________________________________________________________________________ 
PBT 59.3 
59.3 
0 0 0 0 0 0 
ABS 15.0 
15.0 
12.0 
12.0 
0 0 19.1 
19.1 
SAN 0 0 16.0 
16.0 
0 0 60.0 
60.0 
PC 0 0 51.25 
51.25 
79.1 
79.1 
-- -- 
NYGLOS 25.0 
0 20.0 
0 20.0 
0 20.0 
-- 
NYAD G 0 25.0 
0 20.0 
-- 20.0 
-- 20.0 
Stabilizer Package 
0.7 0.7 0.75* 
0.75* 
0.9* 
0.9* 
0.75* 
0.75* 
PROPERTIES 
Notched Izod (ft lbs/in) 
@ rm. temp. 1.0 1.2 3.4 2.2 -- -- -- -- 
@ -30.degree. C. 
1.0 1.0 1.1 1.3 -- -- -- -- 
Dynatup 
@ rm. temp. 2B 2B 2B 2B 5B 5B 5B 5BP 
.sup.E MAX/.sup.E TOT 
13/13 
2/2 25/26 
2/13 
2.7/3.0 
1.4/1.5 
1.4/1.7 
3.8/5.2 
@ -30.degree. C. 
5B 5B 5B 5B 5B 5B 5B 5BP 
.sup.E MAX/.sup.E TOT 
1.6/3.1 
2.1/3.3 
3.4/4.0 
5.6/10.7 
2.1/2.2 
0.99/1.1 
1.6/1.9 
2.9/3.5 
DOI (%) 99 88 94 72 89 70 70 58 
CTE (in/in/.degree. F. .times. 10.sup.-5 
3.63 
3.85 
2.25 
3.00 
2.17 
2.69 
2.91 
3.81 
flow direction) 
__________________________________________________________________________ 
ABS BLENDEX .RTM. 338 ABS (70 wt. % butadiene, 22 wt. % styrene, 8 wt. 
acrylonitrile) by General Electric Company 
SAN styrene acrylonitrile copolymer SAN 580 by General Electric Company 
BP brittle punch out 
PC polycarbonate LEXAN .RTM. 140 resin by General Electric Company 
All other ingredients and tests run are the same as Table 1, except that 
Examples 17 and 18 do not contain a thio ester in the Stabilizer Package 
*Stabilizer Package Irganox 1076 (a phenolic antioxident by Ciba 
Geigy)/pentaertherytol tetrestearate/IRGAFOS 168 
EXAMPLES 25-33 
Several blends were prepared, each of which contained 49 parts by weight 
poly(2,6-dimethyl-1,4-phenylene ether) which had an intrinsic viscosity 
of, approximately, 0.45 dl/g as measured in chloroform at 25.degree. C., 
0.70 part citric acid monohydrate compatibilizing agent, 10 parts rubber 
modifier (Kraton, G-1651 Shell Chemical, a 
styrene-ethylene/butylene-styrene triblock copolymer), 0.30 part Irganox 
1076 hindered phenol stabilizer, 0.10 part KI stabilizer, and 10 parts of 
a specified nylon. 
The foregoing blended components of the composition were fed to the 
feedthroat of a 30 mm. Werner & Pfleiderer twin screw extruder which was 
fitted with a downstream addition port. The extruder was set at 
550.degree. F., and was fitted with a downstream addition port. 
An additional 31 parts of a nylon component specified in the table were fed 
at the downstream addition port. 
The resulting extruded strand was chopped into pellets, dried and molded 
into ASTM test parts in a Newbury 3 ounce injection molder having a 
550.degree. F. set temperature profile and a mold set temperature of 
150.degree. F. All test results described in Table 1 were performed in 
accordance with ASTM test specifications. 
The polyamide component designated as nylon 6,6 was NP-10,000 from Nylon 
Polymers. The nylon 6 was Nycoa 471 from Nylon Corp. of America. 
The filled compositions were prepared in the same fashion as set forth in 
the previous paragraph, 
TABLE 5 
__________________________________________________________________________ 
Examples 25-33 
PROPERTIES 
25 26 27 28 29 30 31 32 33 
__________________________________________________________________________ 
Filler 0 Nicron 
Polyfil 
NYGLOS 
NYGLOS 
Talc PPG Clay 
M-XF 
500 talc 
EDL silane 
no MP 12-50 
3634 
EDL mica 
silane 
Clay 
treated 
treatment 
no glass 
300-L 
treated treatment 
fibers 
Notched Izod 
(ft-lbs/in) 
@ rm. temp. 
5.6 
0.7 0.9 2.2 2.4 1.0 0.9 2.0 1.0 
@ -30.degree. C. 
2.3 
0.7 0.6 1.5 1.6 0.6 0.6 1.5 0.8 
Tensile 98.0 
7.0 8.0 54.0 48.0 8.0 0.9 44.0 
12.0 
Elongation 
CTE 4.4 
3.2 3.2 3.6 4.0 3.3 2.4 3.8 3.6 
DOI 97.0 
99.0 
97.6 
99.0 99.0 99.0 96.6 
94.3 
89.0 
Dynatup (ft-lbs) 
@ rm. temp. 
45.0 
2.0 3.0 33.0 30.0 3.0 3.0 22.0 
1.0 
@ -22.degree. C. 
35.0 
1.0 2.0 11.0 14.0 1.0 3.0 7.0 1.0 
__________________________________________________________________________ 
except the filled compositions consisted of a blend of 40 parts of the 
poly(2,6dimethyl -1,4-phenylene ether), 36 parts of the nylon 6/6, 10 
parts of the Kraton G-1651, 0.7 parts of citric acid, and 14 parts of the 
filler, which is as set forth in Table 5 below with the results of the 
tests run on the Examples, namely Dynatup Impact, coefficient of thermal 
expansion (CTE), DOI and tensile elongation. Tensile elongation was 
determined in accordance with ASTM test procedure D638. The other test 
procedures are as described in Examples 1-4. 
TABLE 6 
______________________________________ 
Examples 34-39 AND 40C-45C 
EX D L DOI CTE 
______________________________________ 
40C Glass Fiber - A 
10 300 70 -- 
41C Wollastonite 
8 80 80 -- 
42C PMF 204C 5 50 80 -- 
43C Milled glass 
7 110 80 -- 
44C Milled glass 
4 110 80 -- 
45C Milled glass 
13 65 90 -- 
34 Milled ceramic 
3 15 99 -- 
35 CaSO.sub.4 2 20 99 -- 
36 Poly(calcium 
0.5 15 99 5.0 
terephthalate) 
37 Titanate 1.0 50 99 4.4 
38 TiO.sub.2 0.16 1.7 99 6.5 
39 Norphil 0.4 1.6 85 -- 
______________________________________ 
The above examples were materials tested for their suitability for painted 
automotive bodypanels. D means number average diameter of the fibers. L 
means number average length of the fibers. The compositions comprised 70% 
by weight polybutylene terephthalate, 20 percent by weight polyetherimide 
ester resin, and 10 percent by weight reinforcing fiber based on the 
entire weight of the composition. A DOI value of at least 95% is necessary 
for a composition to be suitable for the automotive body panels, 
preferably having a DOI of at least 99%. Examples 40.degree. C.-45.degree. 
C. are comparative examples. Examples 34-38 exhibit sufficiently high DOI 
values. DOI is measured after exposure of the composition to 280.degree. 
F. Preferably the coefficient of thermal expansion is between 
3.times.10.sup.-5 inches/inch/.degree.F. and 5.times.10.sup.-5 
inches/inch/.degree.F., more preferably between 4.times.10.sup.-5 
inches/inch/.degree.F. and 5.times.10.sup.-5 inches/inch/.degree.F. 
Therefore, in the present invention, it is to be understood by those 
skilled in the art that various changes may be made in the particular 
embodiments described above without departing from the spirit and scope of 
the invention as defined in the appended claims