Polymer compositions comprising linear alternating polymers of carbon monoxide and at least one ethylenically unsaturated hydrocarbon filled with mica are prepared without the use of a coupling agent.

FIELD OF THE INVENTION 
This invention relates to certain polymer compositions of improved 
mechanical properties. More particularly, the invention relates to a 
polyketone polymer filled with mica. 
BACKGROUND OF THE INVENTION 
Blending of organic polymers with inorganic fillers is well known. Blending 
typically serves to improve the mechanical properties of the polymer as 
well as to extend the polymer through use of generally less expensive 
fillers. Typical fillers include talc, mica, certain calcium carbonates, 
glass fibers, gypsum and others as disclosed in published Japanese Patent 
Application J59064647-A. The use of such fillers in polyolefins is 
disclosed in published Japanese Patent Application J59147035-A. The use of 
flaky fibers, particularly mica, in thermoplastic resins such as 
polyolefins is shown by Ueeda et al., U.S. Pat. No. 4,555,439. 
The ease with which blends of an organic polymer and an inorganic filler 
are produced and processed is greatly dependent upon the physical 
properties of the polymer and the filler as well as the extent of 
interaction between the components of the blend. Particularly important is 
the degree of adhesion between the polymer and the filler, especially when 
the polymer blend is to be employed in the production of shaped articles 
or articles which are to be subjected to mechanical or thermal stress. 
Improvement in important mechanical properties such as tensile strength, 
stiffness, ductility, and high heat distortion temperature result when a 
relatively high degree of adhesion occurs between the polymer and the 
filler. Lack of adhesion can be sufficiently troublesome so as to require 
the addition of cross-linking agents to overcome the problem and result in 
satisfactory mechanical properties. 
The above two published Japanese Patent Applications require the use of a 
silane cross-linking agent in order to obtain good mechanical properties 
when a number of inorganic fillers including mica are blended with 
polyolefins. Wang, U.S. Pat. No. 4,066,604 teaches the preferred use of 
nitrophenylenes or sulfonated polyphenylenes as cross-linking agents when 
mica is blended with certain branched polyphenylenes. 
An easily observed measure of the degree of adhesion, or lack of adhesion, 
is the phenomena of whitening of a polymer composition under stress or 
distortion. The above published Japanese Patent Applications teach that 
resistance to whitening is a desired property of the disclosed 
compositions which employ cross-linking agents. Ueeda, U.S. Pat. No. 
4,555,439 prepares rolled sheets of specific crystallinity and cites lack 
of whitening as an improved property. 
U.S. Pat. No. 4,317,765 to Gaylord teaches that about 23 different 
hydroxyl-containing fillers can be added to about 76 different 
thermoplastic polymers. Among the fillers is mica and among the polymers 
listed is a copolymer of carbon monoxide and ethylene, with the structure 
of the copolymers being omitted. Gaylord further states that the 
properties of polymer compositions are improved only if a coupling or 
compatibilizing agent is employed in the compositions. Having established 
the need for a coupling agent or compatibilization process, Gaylord sets 
forth two methods of accomplishing the desired compatibilization through 
the use of coupling agents. 
The class of polymers of carbon monoxide and olefin(s) has been known for 
some time. Brubaker, U.S. Pat. No. 2,495,286, produced such polymers of 
relatively low carbon monoxide content in the presence of free radical 
initiators, i.e., peroxy compounds. G.B. 1,081,304 produced similar 
polymers of higher carbon monoxide content in the in the presence of 
alkylphosphine complexes of palladium salts as catalyst. Nozaki extended 
this process to produce linear alternating polymers by the use of 
arylphosphine complexes of palladium moieties and certain inert solvents. 
See, for example, U.S. Pat. No. 3,694,412. 
More recently, the class of linear alternating polymers of carbon monoxide 
and at least one ethylenically unsaturated hydrocarbon, e.g., ethylene or 
ethylene and propylene, has become of greater interest in part because of 
the greater availability of the polymers. These polymers, often referred 
to as polyketones or polyketone polymers, have been shown to be of the 
repeating formula --CO--A-- where A is the moiety of unsaturated 
hydrocarbon polymerized through the ethylenic unsaturation. For example, 
when the hydrocarbon is ethylene the polymer is represented by the 
repeating formula --CO--CH.sub.2 --CH.sub.2 --. The general process for 
the more recent production of such polymers is illustrated by a number of 
published European Patent Applications including 121,965, 181,014, and 
their U.S. equivalents, U.S. Pat. No. 4,835,250 and U.S. Pat. No. 
4,818,810. The process typically involves a catalyst composition formed 
from a compound of a Group VIII metal selected from palladium, cobalt and 
nickel, the anion of a strong non-hydrohalogenic acid and a bidentate 
ligand of phosphorus, arsenic or antimony. 
The resulting polymers are relatively high molecular weight thermoplastics 
having established utility in the production of shaped articles, such as 
containers for the food and drink industry, which are produced by 
processing the polymer according to known methods. For some particular 
applications it has been found desirable to have properties for a 
polymeric composition which are somewhat different from those of the 
polyketone polymers. It would be of advantage to retain the desirable 
properties of the polyketone polymers and yet improve other properties. 
These advantages are often obtained through the provision of a polymer 
blend. Reinforcing a polymer with a filler often provides a less expensive 
product, in addition to desirable properties. 
It is an object of this invention to provide blends of a polyketone polymer 
filled with mica which exhibit desirable properties. It is a further 
object of this invention to prepare such mica-filled compositions without 
the use of a coupling or compatibilizing agent commonly used with other 
filled polymer compositions. 
SUMMARY OF THE INVENTION 
This invention relates to improved polymer compositions comprising an 
amount of a linear alternating polymer of carbon monoxide and at least one 
ethylenically unsaturated hydrocarbon filled with an amount of mica. The 
compositions exhibit good adhesion and mechanical properties without the 
addition of the coupling or compatibilizing agents often necessary in 
filled polymer blends. Muscovite is a preferred mica. 
DESCRIPTION OF THE INVENTION 
The polyketone polymers which are employed as the major component of the 
filled blends of the invention are linear alternating polymers of carbon 
monoxide and at least one ethylenically unsaturated hydrocarbon. Suitable 
ethylenically unsaturated hydrocarbons for use as precursors of the 
polyketone polymers have up to 20 carbon atoms inclusive, preferably from 
2 to 10 carbon atoms inclusive, and are aliphatic such as ethylene and 
other .alpha.-olefins including propylene, butylene, isobutylene, 
1-hexene, 1-octene and 1-dodecene, or are arylaliphtic containing an 
aromatic substituent on an otherwise aliphatic molecule, particularly an 
aryl substituent on a carbon atom of the ethylenic unsaturation. 
Illustrative of this latter class of ethylenically unsaturated 
hydrocarbons are styrene, p-methylstyrene, p-ethylstyrene and 
m-methylstyrene. Preferred polyketone polymers are copolymers of carbon 
monoxide and ethylene or are terpolymers of carbon monoxide, ethylene and 
a second hydrocarbon of at least 3 carbon atoms, particularly an 
.alpha.-olefin such as propylene. 
The structure of the polyketone polymers is that of a linear alternating 
polymer of carbon monoxide and ethylenically unsaturated hydrocarbon, and 
the polymer will contain substantially one molecule of carbon monoxide for 
each molecule of unsaturated hydrocarbon. When terpolymers of carbon 
monoxide, ethylene and a second hydrocarbon are employed in the blends of 
the invention, there will be within the terpolymer at least about two 
units incorporating a moiety of ethylene for each unit incorporating a 
moiety of second hydrocarbon, preferably from about 10 units to about 100 
units incorporating a moiety of ethylene per unit incorporating a moiety 
of the second hydrocarbon. The polymer chain is therefore represented by 
the formula 
##STR1## 
where G is the moiety obtained by polymerization of the second hydrocarbon 
through the ethylenic unsaturation. The --CO--(CH.sub.2 --CH.sub.2 units 
and the --CO--(G)-- units are found randomly throughout the polymer chain 
and the ratio of y:x is no more than about 0.5. In the modification of the 
invention where a copolymer of carbon monoxide and ethylene is employed as 
a blend component, there will be no second hydrocarbon and the polyketone 
polymer is represented by the above formula wherein y is 0. When y is 
other than 0, i.e., terpolymers are employed, ratios of y:x from about 
0.01 to about 0.1 are preferred. The end groups or "caps" of the polymer 
chain will depend on what materials are present during the production of 
the polyketone and whether and how the polyketone is purified. The precise 
properties of the polymer will not depend upon the particular end groups 
to any considerable extent so that the polymer is fairly represented by 
the above formula for the polymeric chain. 
Of particular interest are those polyketones of number average molecular 
weight from about 1000 to about 200,000, especially those polymers of 
number average molecular weight from about 10,000 to about 90,000 and 
containing substantially equimolar quantities of carbon monoxide and 
ethylenically unsaturated hydrocarbon. 
Such polymers are produced by contacting the carbon monoxide and the 
ethylenically unsaturated hydrocarbon(s) under polymerization conditions 
in the presence of a catalytic quantity of a catalyst formed from a metal 
compound of palladium, cobalt or nickel, an anion of a non-hydrohalogenic 
acid having a pKa less than about 6, preferably less than about 2, and 
certain bidentate ligands of nitrogen or of phosphorus, arsenic or 
antimony. Although the scope of the polymerization process is extensive, 
for purposes of illustration, in a preferred method of producing the 
polyketone polymer, the metal compound is palladium acetate, the anion is 
the anion of tri-fluoroacetic acid or para-toluenesulfonic acid, and the 
bidentate ligand is 1,3-bis(diphenylphosphino)propane. 
Polymerization is typically carried out at elevated temperature and 
pressure, in the gaseous phase in the substantial absence of reaction 
diluent, or in the liquid phase in the presence of a reaction diluent such 
as a lower alkanol, e.g., methanol or ethanol. Suitable reaction 
temperatures are from about 20.degree. C. to about 150.degree. C. with 
preferred reaction temperatures being from about 50.degree. C. to about 
135.degree. C. Typical reaction pressures are from about 1 bar to about 
200 bar, more typically from about 10 bar to about 100 bar. 
The reactants and catalyst are contacted by conventional methods such as 
shaking or stirring and subsequent to reaction the polymer product is 
recovered as by filtration or decantation. The polymer product will, on 
occasion, contain metal or other residues of the catalyst which are 
removed, if desired, by treatment of the polymer product with a solvent 
which is selective for the residues. 
Production of this class of polymers is illustrated, for example, by 
published European Patent Applications 181,014 and 121,965, and their U.S. 
equivalents, U.S. Pat. No. 4,818,810 and U.S. Pat. No. 4,835,250. 
The physical properties of the polymer will be in part determined by the 
molecular weight and whether the polymer is a copolymer or terpolymer and 
what unsaturated hydrocarbons have been employed in its production. 
Typical melting points of the polyketone polymers are from about 
175.degree. C. to about 300.degree. C., more frequently from about 
210.degree. C. to about 260.degree. C. The polymers will have a limiting 
viscosity number (LVN), measured in a standard capillary viscosity 
measuring device in m-cresol at 60.degree. C., from about 0.5 to about 10, 
preferably from about 0.8 to about 4. 
The polymer compositions of the invention comprise the polyketone polymers 
above incorporating uniformly therein a proportion of mica. The 
compositions exhibit good adhesion and mechanical properties without the 
addition of the coupling or compatibilizing agents often necessary in 
filled polymer blends. The micas which are suitably used in the 
compositions of the invention are those silicate materials characterized 
physically as flat, six-sided monoclinic crystals which undergo a nearly 
perfect basal cleavage to yield thin, tough, flexible flakes. Such micas 
are characterized as high aspect ratio micas, having an aspect ratio of up 
to 20:1, preferably up to 100:1. The phrase, "the aspect ratio" of a mica 
particle is defined as the ratio of the length of a particle to the 
thickness of the particle. Larger particles tend to have higher aspect 
ratios. 
The actual chemical composition of the mica will vary over a range of 
specific types of mica. Muscovite is a preferred mica but other natural or 
synthetic micas such as phlogophite, biolite, fluorophlogopite, and barium 
fluorophlogopite and barium disilicate can be used. Micas are further 
described in Kirk-Othmer, Encyclopedia of Chemical Technology, Second 
Edition, Vol. 13, pp. 398-424, incorporated herein by reference. 
The size of the particles of mica which are useful in the present invention 
can vary but particles from about 50 mesh to about 600 mesh are suitable 
with particles from about 80 mesh to about 200 mesh being preferred for 
some applications, and all based on U.S. Bureau of Standards mesh sizes. 
The amount of mica to be incorporated into the compositions of the 
invention can vary widely. Preferably, a lesser amount of mica on a volume 
basis, relative to the polymer which is present as the major component in 
the total blend, is used. Amounts of mica from about 1% by volume to about 
35% by volume, or from about 2% by weight to about 56% by weight, based on 
the total composition, are satisfactory with amounts from about 2% by 
volume to about 30% by volume, or from about 5% by weight to about 51% by 
weight, based on the total composition, being preferred, and amounts of 
from about 5% by volume to about 30% by volume, or from about 11% by 
weight to about 51% by weight, being more preferred. 
The method of forming the polymer compositions is not critical so long as 
the method results in a substantially uniform blend of the composition 
components. The components are dry blended and converted to a 
substantially uniform composition by application of elevated temperature 
and pressure. Alternatively, the polymer is heated until molten and the 
mica mixed therewith through the use of a high-shear mixer, extruder or 
kinetic compounder. 
The composition of the invention, in addition to polymer and mica, may 
incorporate conventional additives such as plasticizers, mold release 
agents, antioxidants, fire retarding chemicals, pigments, and other 
materials to improve the processability or properties of the polymer 
blend. Such additives may be added by blending or other conventional 
methods together with or separately from the mica. 
The resulting compositions are processed by conventional methods such as 
injection molding, pressure forming, thermoforming, sheet extrusion and 
sheet casting which do not serve to degrade the polymer or the 
composition. 
The compositions are characterized by improved mechanical properties of 
stiffness, high heat distortion temperature, and strength, and by 
resistance to stress-whitening in molded articles, even those articles 
which incorporate rather sharp angles in their physical shape. 
The novel blend compositions have particular utility in the production of 
containers and mechanical parts, particularly those having a large and 
continuous surface where strength, uniformity, and appearance are 
important. Moreover, the compositions of the invention exhibit improved 
paint adhesion which, together with a high heat distortion temperature, 
offer significant advantages when paints requiring baking are employed, 
e.g., in exterior automobile parts. Other applications in which the 
compositions of the invention offer significant advantages are those 
applications having high temperature requirements.

The compositions of the invention are further illustrated by the following 
Examples which should not be construed as limiting the invention. 
EXAMPLE 1 
A linear alternating polyketone terpolymer of carbon monoxide, ethylene and 
propylene was prepared in the presence of a catalyst formed from palladium 
acetate, the anion of trifluoroacetic acid, and 
1,3-bis(diphenylphosphino)propane. The polymer had a melting point of 
215.degree.-220.degree. C. 
EXAMPLE 2 
The polymer of Example 1 was blended with 15% by weight of mica by use of a 
30 mm twin-screw extruder, extruded and pelletized to produce nibs. The 
nibs were dried, then injection molded into plaques of dimensions 
approximately 4 in. by 4 in. by 0.05 in. These plaques were deformed by 
Solid Phase Pressure Forming into shallow 2 oz. cups. There was no visual 
evidence of stress whitening. The nibs were also molded into test bars 
having dimensions approximately 4.5 in.times.0.5 in.times.0.12 in. These 
bars were evaluated for tensile properties according to ASTM D-638. The 
results are shown in Table 1. 
EXAMPLE 3 
Blends of 20% by weight of mica and the polymer of Example 1 were prepared 
by use of a 30 mm twin-screw extruder to produce nibs. The nibs were 
molded into plaques of dimensions approximately 4 in..times.4 
in..times.0.05 in. by injection molding. These plaques were formed into 
shallow trays and 2 oz. cups which exhibited high stiffness and good 
appearance without visual evidence of whitening under stress. The nibs 
were also molded into test bars having dimensions approximately 4.5 
in.times.0.5 in.times.0.12 in. These bars were evaluated for tensile 
properties according to ASTM D-638. The blends were also tested for 
Notched Izod using ASTM D-256, and for heat deflection temperature (at 264 
psi). The results are shown in Table 1. 
EXAMPLE 4 
Blends of 30% by weight of mica and the polymer of Example 1, were prepared 
in the manner described in Example 3. Nibs were were molded into test bars 
having dimensions approximately 4.5 in.times.0.5 in.times.0.12 in. These 
bars were evaluated for tensile properties according to ASTM D-638. The 
blends were also tested for Notched Izod, using ASTM D-256, and heat 
deflection temperature (at 264 psi). The results are shown below in Table 
1. 
TABLE 1 
__________________________________________________________________________ 
Notched Izod 
1% Secant Stress at 
Elongation at 
(ft-lb/in) 
Heat Deflection 
Wt % Mica 
Modulus (psi) 
Yield (psi) 
Failure (%) 
23.degree. C. 
-40.degree. C. 
Temperature (.degree.C.) 
__________________________________________________________________________ 
0 200,00-250,000 
7,000-8,000 
60-120 4.3 -- 96 
15 521,000 3988 33.6 -- -- -- 
20 418,000 9070 11.0 1.04 
0.56 148 
30 548,000 9610 6.9 0.84 
0.56 159 
__________________________________________________________________________ 
EXAMPLE 5 
For comparative purposes, three specific "neat" novel polyketones, noted 
hereafter as Control A, Control B, and Control C were prepared into test 
plaques and test samples and evaluated for flexural modulus (in psi), 
tensile strength (in psi), and Notched Izod (in ft-lb/in) at room 
temperature and at -29.degree. F. Additionally, Control B was evaluated 
for its heat deflection temperature. Flexural modulus was determined using 
ASTM D-790. Tensile strength was determined using ASTM D-638. Notched Izod 
determination was made using ASTM D-256. The results of the analyses are 
shown in Table 2. 
More specifically, Control A was a linear alternating terpolymer prepared 
in the presence of a catalyst formed from palladium acetate, the anion of 
a trifluoroacetic acid and 1,3-bis(diphenylphosphino) propane. The polymer 
had a melting point of 220.degree. C. and a limiting viscosity number 
(LVN) of 1.96 dl/g, measured in m-cresol at 60.degree. C. 
Control B was a blend of two linear alternating polymers. Control B 
comprised 33% of the polyketone polymer 088/005 and 67% of the polyketone 
polymer 088/006. Polymer 088/005 was a linear alter-nating terpolymer of 
ethylene and 7 wt % propylene prepared by employing a catalyst composition 
formed from palladium acetate, the anion of trifluoroacetic acid and 
1,3-bis[di(methoxy-phenol)phosphino]propane. Polymer 088/005 had a melting 
point of 220.degree. C. and an LVN of 1.79 dl/g, measured in m-cresol at 
60.degree. C. Polymer 088/006 was a linear alternating polymer prepared in 
a manner identical to the 088/005 polymer. The 088/006 polymer had a 
melting point of 223.degree. C. and an LVN of 1.62 dl/g. The neat polymer 
blend of Control B was formed by dry mixing pellets of the two polymers 
088/005 with 088/006 in a conventional manner. The blended mixture was 
then melt blended in a 30 mm co-rotating twin screw extruder having seven 
zones and a total L/D of 27/1. The melt temperature at the die exit was 
260.degree. C. 
Control C was linear alternating polyketone polymer known as 088/008, 
prepared in the presence of a catalyst formed from palladium acetate, the 
anion of trifluoroacetic acid and 1,3-bis(diphenyl phosphino)propane. The 
polymer had a melting point of 223.degree. C. and an LVN of 1.73 dl/g 
measured in m-cresol at 60.degree. C. 
EXAMPLE 6 
The polymers of Example 5, Controls A, B, and C, were used to prepare 
several filled blend samples by compounding the polymer with filler(s) on 
a 30 mm, 27/1 L/D twin screw extruder. The fillers used included mica, 
glass fiber, and a mica/glass fiber blend. The mica used was a 
phyllosilicate mica, Asprapearl. The blends were extruded into water and 
pelletized. The pellets were dried and injection molded. An Engel (8 oz.) 
injection molder equipped with a 2.2/1 compression ratio screw was used 
for several moldings. The molder formed standard family test specimens 
which were tested using the ASTM tests noted above. The results of the 
tests are shown in Table 2. 
The specific reinforcing components provided different strength and modulus 
values when blended with the Controls A, B, and C. Certain of these 
components appear to act synergistically with the polyketone causing a 
definite change in the properties of the polyketone with each blend. Mica 
provided a polymer with strength characteristics that were better than the 
neat polymer control, but which were not as good as the glass fibers alone 
or the mica/glass combination. High aspect ratio mica platelets provided 
good heat deflection temperature, but not quite as good strength as the 
glass fibers. 
TABLE 2 
__________________________________________________________________________ 
Heat 
Flexural 
Tensile Deflection 
Modulus 
Strength 
Notched Izod (ft-lb/in) 
Temperature 
(psi) 
(psi) Room Temperature 
29.degree. C. 
(.degree.F.) 
__________________________________________________________________________ 
Controls 
Control A 240,000 
7000-8000 
4.8 1.2 -- 
Control B 263,000 
7000-8000 
3.0 -- 205 
Control C 200,000- 
7000-8500 
4.3 1.1 -- 
250-000 
Mica Blends 
10 wt % 310,000 
8500 0.6-0.75 -- 250-260 
1 wt % 265,000 
6500 3.75-5 -- -- 
Mica/Glass Fiber Blends 
10 wt % mica + 5 wt %/glass 
400,000 
8200-7500 
1.8 0.9 240 
Glass Fiber Blends 
9.9 wt % (polar sized) 
304,000 
10,300 
2.1 0.9 -- 
9.9 wt % (not polar sized) 
230,000 
8300 1.7 0.8 -- 
__________________________________________________________________________ 
EXAMPLE 7 
Linear alternating terpolymers of carbon monoxide, ethylene, and propylene 
(89/054 and 89/056) were produced in the presence of a catalyst 
composition formed from palladium acetate, trifluoracetic acid and 
1,3-bis[di(2-methoxyphenyl)phosphino]propane. The polyketone polymers had 
melting points of about 220.degree.-222.degree. C. and LVNs of about 1.08 
dl/g when measured in m-cresol at 60.degree. C. The polyketone polymers 
also contained 0.5% Ethanox 330 and 0.5% Nucrel 535, both conventional 
additives. 
EXAMPLE 8 
The relative importance of a surface coating on the mica employed was 
investigated by preparing blends of polyketone polymers and micas with and 
without surface coatings. Filled blend compositions were prepared by 
combining the polymers of Example 7 with two different types of mica. The 
two micas used were: Aspraflex 100, muscovite mica with no surface 
treatment and Aspralok 100, muscovite mica with a coupling agent suitable 
for polyethylene, both obtained from J. M. Huber. The micas had comparable 
particle size ranges. 
The filled blends were prepared by dry blending polyketone polymer powder 
with the micas at the prescribed composition, and subsequently melt 
compounding the samples in a Haake 30 mm co-rotating, fully intermeshing, 
twin-screw extruder operating at about 200 rpm and a melt temperature of 
about 250.degree. C. Test specimens were prepared using an Arburg 
injection molding machine with a 25 mm diameter and a 20 ton clamp. All 
compounds were dried prior to molding, and molded specimens were stored 
over dessicant prior to testing. 
The samples were tested for mechanical and impact properties, as well as 
heat deflection temperature (at 264 psi). The results are shown in Table 
3. 
TABLE 3 
__________________________________________________________________________ 
Mica Content 
Flexural 
Tensile 
Notched Izod @ 
Gardner Impact @ 
Heat Deflection 
Mica Type 
vol % 
wt % 
Modulus (psi) 
Strength (psi) 
RT (ft-lb/in) 
RT (in-lb) 
Temperature 
__________________________________________________________________________ 
(.degree.C.) 
Control 
0 0 259,000 
9130 1.93 126 103 
Aspraflex 100 
10 22 606,000 
8500 0.86 8 159 
20 38 994,000 
9830 0.61 3 181 
Aspralok 100 
10 22 533,000 
8870 0.92 8 162 
20 38 849,000 
9140 0.61 5 172 
30 51 1,209,000 
9990 0.61 4 -- 
__________________________________________________________________________ 
The results in Table 3 indicate that the untreated mica produced stiffer 
blends, as measured by flexural modulus, than the mica with a surface 
coating, at similar mica loadings. The untreated mica also produced 
compounds with the greatest strength and with a higher heat deflection 
temperature at the 20% by volume loading. As expected, Notched Izod and 
Gardner impact values were better for the control than for the filled 
systems. 
These results indicate that superior blends of polyketone polymers and mica 
may be obtained without the use of conventional coupling or 
compatibilizing agents. 
EXAMPLE 9 
Two different types of mica were evaluated by preparing blends of the 
polyketone polymers of Example 7 and both muscovite mica and phlogopite 
mica. The muscovite micas were Aspraflex 100, obtained from J. M. Huber, 
and WG-325.TM., obtained from KMG Minerals. The phlogopite mica was 
Suzorite.RTM. 325-HK, obtained from Suzorite Mica Products. None of the 
micas had a surface treatment, and all had comparable particle size 
ranges. 
The filled blends were prepared as described in Example 8. The samples were 
then tested for mechanical and impact properties, as well as heat 
deflection temperature (at 264 psi). The results are shown in Table 4. 
The muscovite micas provided better reinforcement than the phlogopite mica 
at comparable levels in the polyketone polymer. The muscovite-filled 
blends exhibited greater tensile strength and stiffness (measured by 
flexural modulus) than the phlogopite-filled blends at comparable 
loadings. 
TABLE 4 
__________________________________________________________________________ 
Mica Content 
Flexural 
Tensile 
Notched Izod @ 
Gardner Impact 
Heat Deflection 
Mica Type vol % 
wt % 
Modulus (psi) 
Strength (psi) 
RT (ft-lb/in) 
RT (in-lb) 
Temperature 
(.degree.C.) 
__________________________________________________________________________ 
Control 0 0 259,000 
9130 1.93 126 103 
Aspraflex 100 
10 22 606,000 
8500 0.86 8 159 
20 38 994,000 
9830 0.61 3 181 
WG-325 .TM. 
10 22 526,000 
8260 0.97 10 148 
20 38 859,000 
8410 0.68 3 175 
30 51 1,138,000 
8300 0.60 4 181 
Suzorite .RTM. 325-HK 
20 38 723,000 
7700 0.62 6 167 
__________________________________________________________________________ 
EXAMPLE 10 
The relative importance of particle size was investigated by preparing 
blends with micas having several particle sizes. Filled blend compositions 
were prepared by combining the polymers of Example 7 with three different 
micas, using the methods described in Example 8. 
The micas used were all phlogopite micas obtained from Suzorite Mica 
Products: (1) Suzorite.RTM.150-S, a coarse grind mica with 60% of the 
particles greater than 200 mesh (74 microns), (2) Suzorite.RTM. 200-HK, 
with 44-63% of the particles less than 325 mesh (44 microns), and (3) 
Suzorite.RTM. 325-HK, with 92% of the particles less than 325 mesh. The 
samples were all tested for mechanical and impact properties, as well as 
heat deflection temperature (at 264 psi). The results are shown in Table 
5. 
The results indicate that the more coarsely ground micas provide filled 
blends with greater stiffness than the micas that are more finely ground. 
The particles size of the mica also relates to its aspect ratio. Larger 
particles have higher aspect ratios, and a higher aspect ratio would be 
expected to provide superior stiffness for mica-filled compounds. However, 
the higher Notched Izod values for the blends containing the more coarsely 
ground mica is an unexpected result. Generally, one would expect a smaller 
particle size to be more effective at providing the toughness measured by 
Notched Izod. 
TABLE 5 
__________________________________________________________________________ 
Mica Content 
Flexural 
Tensile 
Notched Izod @ 
Gardner Impact 
Heat Deflection 
Mica Type vol % 
wt % 
Modulus (psi) 
Strength (psi) 
RT (ft-lb/in) 
RT (in-lb) 
Temperature 
(.degree.C.) 
__________________________________________________________________________ 
Control 0 0 259,000 
9130 1.93 126 103 
Suzorite .RTM. 150-S 
20 38 897,000 
7140 0.90 8 172 
Suzorite .RTM. 200-HK 
20 38 796,000 
7440 0.74 6 172 
Suzorite .RTM. 325-HK 
20 38 723,000 
7700 0.62 6 167 
__________________________________________________________________________