Ethylene copolymer compositions

BACKGROUND OF THE INVENTION
Ethylene polymers, i.e., homopolymers and copolymers, are easily molded or extruded into shaped articles. Additives are frequently used to improve the strength of the polymers. Efforts have also been made to improve the flame and smoke resistance of such polymers by adding various flame and smoke retardants. However, many such retardants have a negative effect on mechanical properties, such as strength properties, and it is desirable to discover combinations of strength-enhancing additives and flame and smoke retardants that provide a good balance between strength properties and flame and smoke retardancy. This invention is directed to such combinations.
SUMMARY OF THE INVENTION
In its broad aspect, the compositions of this invention comprise:
(a) 20-100 parts of an ethylene polymer matrix comprising at least one thermoplastic ethylene copolymer of ethylene and at least one comonomer selected from vinyl acetate, esters of methacrylic acid or esters of acrylic acid;
(b) 10-80 parts, preferably 10-40 parts, of a copolymer selected from the class consisting of (i) an ethylene/propylene/diene copolymer grafted with 0.1 to 5 weight % anhydride functionality or (ii) at least one polyolefin grafted with 0.1 to 5 weight % anhydride functionality, or (iii) a mixture of both; and
(c) 75-130 parts, preferably 90-110, per 100 parts of polymeric components present, of magnesium hydroxide or alumina trihydrate, or a mixture of both.
(d) 0-80 parts of polyethylene, preferably medium density or linear low density polyethylene;
provided that the combined parts of components (a) and (d) is at least 80 parts.
When polyethylene is present, the preferred amount of component (a) present will be 30-40 parts.
In another embodiment, 3-20 parts of at least one ionomeric copolymer of ethylene and at least one alpha,beta-ethylenically unsaturated carboxylic acid of 3-6 carbons, such as methacrylic or acrylic acid can be present with components (a)-(c) or with components (a)-(c) that contain polyethylene.
Still another optional feature in any of the foregoing embodiments is the additional presence of an ethylene/propylene or ethylene/propylene/diene copolymer in amounts of up to 50 parts.
In still other embodiments, any one or more of the following copolymers may be present: a copolymer of ethylene/methacrylic or acrylic acid, a copolymer of ethylene/vinyl acetate grafted with anhydride functionality, a copolymer of ethylene and acrylic or methacylic acid esters of saturated aliphic alcohols grafted with anhydride functionality.
To add flame retardancy, magnesium hydroxide or alumina trihydrate, or a mixture of the two, is added.
To reduce low temperature brittleness, an ethylene/propylene/diene copolymer grafted with anhydride functionality or at least one polyolefin grafted with anhydride functionality, or a mixture of both, is added.
In addition, it was also found that an ionomeric copolymer of ethylene and a lower alkyl (meth)acrylic acid neutralized with metallic cations also provides resistance to low temperature brittleness, and these polymers can be used also.
It was also discovered that if an ethylene/propylene rubbery copolymer or ethylene/propylene/diene copolymer is added, the elongation properties of the compositions are enhanced.
DESCRIPTION OF THE INVENTION
The foregoing compositions are useful as flame retardant articles, or as insulation or protective coatings around electrical wire or cable.
The thermoplastic ethylene copolymer matrix has been found to more readily accept the magnesium hydroxide or alumina hydrate because of its polarity, and improves extrudability of the compositions. The ethylene copolymers are preferably copolymers of ethylene and vinyl acetate, but numerous other monomers may be used in place of vinyl acetate. For example, copolymers of ethylene with acrylic, methacrylic or methacrylic acid esters of saturated aliphatic alcohols can be used. The copolymers of ethylene and esters of acrylic acid and methanol or ethanol advantageously have a comonomer content of 9-49 wt. %.
It has been found that, preferably, polyethylene should be a component, and that preferably use of a medium density (i.e., maximum density 0.940 (ASTM D-1248, Type II)) polyethylene or linear low density polyethylene (maximum density 0.925) and use of a narrow molecular weight range polyethylene produces better mechanical properties in a wire or cable coating. Such polyethylenes are preferred.
The grafted polymers of component b may be grafted with alpha,beta-ethylenically unsaturated carboxylic acids or anhydrides such as maleic acid, maleic anhydride, fumaric acid, itaconic acid, itaconic anhydride, and the like. Maleic anhydride is a preferred graft material for both the polyolefin polymers and the ethylene/propylene/diene (EPDM) copolymer. The amount of grafting, i.e., anhydride functionality, will be about 0.1 to 5 weight %. The grafted copolymers impart good resistance to low temperature (e.g., about -40.degree. or below, such as down to -60.degree. C.) brittleness. They also increase yield elongation, and yield and break tensile strength. The polyolefin polymers can be polyethylene or copolymers of ethylene and higher olefins (C.sub.3 -C.sub.6) such as propylene and/or butylene. Thus, they include both crystalline and elastomeric polymers, and can be employed with one another herein.
By the term "anhydride functionality" is meant the group ##STR1## The concentration of anhydride in the graft polymer may be measured by infrared spectroscopy of hot pressed films.
The graft copolymers may be prepared as described in Flexman, U.S. Pat. No. 4,026,067 or Caywood, U.S. Pat. No. 3,884,882 and U.S. Pat. No. 4,010,223. The diene component of the graft copolymer is nonconjugated and includes linear aliphatic dienes of at least six carbon atoms which have one terminal double bond and one internal double bond, and cyclic dienes wherein one or both of the carbon-to-carbon double bonds are part of a carbocyclic ring. Of the linear dienes, 1,4-hexadiene are especially preferred.
Classes of cyclic dienes useful for graft formation include alkylidene bicycloalkenes, alkenyl bicycloalkenes, bicycloalkadienes, and alkenyl cycloalkenes.
The magnesium hydroxide [Mg(OH).sub.2 ] and alumina trihydrate (Al.sub.2 O.sub.3.3H.sub.2 O) are used to impart smoke and flame retardation to the compositions. These materials may be surface treated to aid in compatibilizing them with the matrix polymer or polymers.
It has also been found that presence of an ethylenic ionomeric copolymer also aids in reducing brittleness at low temperatures. The ionomeric copolymer employed as a component of the blends of this invention is preferably a copolymer of ethylene and alpha,beta-ethylenically unsaturated carboxylic acids containing 3-6 carbon atoms. The alpha-olefin content of the copolymer is preferably at least 70 mole percent, based on copolymer. The carboxylic acid groups are randomly distributed over the copolymer molecules and can be 10-90%, preferably 40-80%, neutralized by metal cations distributed over the carboxylic acid groups of the copolymer. The metal cations can be derived from any metals, but preferably are Zn, Na, Mg or Ca. Illustrative of the alpha,beta-ethylenically unsaturated carboxylic acids useful in the preparation of said ionic copolymer are acrylic acid, methacrylic acid, ethacrylic acid, itaconic acid, maleic acid, fumaric acid, and monoesters of itaconic acid, maleic acid, and fumaric acid. Other monomers can, of course, be incorporated in the copolymer.
Finally, it has been found that if an ethylene/propylene (E/P) copolymer or ethylene/propylene/diene (EPDM) copolymer is added, the composition will have better elongation properties. Examples of EPDM copolymers are those ungrafted copolymers described previously.
Desired additives such as antioxidants, neutralizers, ultraviolet absorbers, antistatic agents, pigments, lubricants, slip agents, viscosity modifiers or the like can be added to the composition of this invention.
The components of the compositions of this invention can be blended by any of the conventional blending methods such as a roll mill, a Banbury mixer, a monoaxial extruder, biaxial extruder or the like. The compositions can be formed by any of the conventional methods such as compression molding, extrusion coating, injection molding, calendering, or the like.

EXAMPLES
The Examples are shown in tabular form. The blends described in the tables were prepared by blending the indicated ingredients on a Banbury mixer or two-roll mill. Compounding on a two-mill roll was carried out on a 4".times.8" (10.2 cm.times.20.3 cm) two-roll mill heated with 165.degree. C. steam. All of the polymer components were added to the mill, melted and mixed. Flame retardants and other additives were then added. When incorporation was complete and a band formed on the mill, the component was cut and folded six times. After cigar rolling and rebanding six times, the compound was sheeted off the mill. Compression molding of these samples was carried out on a 8".times.8" (20.3 cm.times.20.3 cm) stainless steel mold. The bottom plate containing two 3".times.6".times.0.075 (7.6 cm.times.15.2 cm.times.0.2 cm) cavities was 3/4" (1.9 cm) thick; the solid top plate was 3/8" (0.95 cm) thick. The mold was heated to 177.degree. C. in a Pasedena Hydraulic Press. 7.6 cm.times.15.2 cm.times.0.23 cm sheets of compound were placed in the preheated mold, using 2 mil "Kapton" polyimide film sprayed with Freekote 33 mold release as a mold liner. The closed mold was placed in the press and heated for 10 minutes with the platens closed to touch pressure. The pressure was then increased to 30,000 pounds force on the 10.2 cm ram as read from the pressure gauge of the press for 1 minute. The pressure was momentarily released and then returned to 30,000 pounds (133 kN) force for 2 minutes. The closed mold was then removed from the heated press and placed in a water-cooled press. When the mold reached room temperature, the samples were removed from the mold.
When a Banbury mixer was used, the chamber was heated to 150.degree.-160.degree. F. (66.degree.-71.degree. C.) with the cooling water off. The polymers and then flame retardants were added. Mixing to 250.degree. F.-275.degree. F. (166.degree.-177.degree. C.) with the cooling water off was carried out, followed by sweeping. The cooling water was turned on after sweeping.
With the cooling water on, mixing was carried out until a temperature of 330.degree.-350.degree. F. was reached and then the contents were dumped from the chamber. The contents were cut and folded on a mill and sheeted for molding. The sheeted compositions were pressed between sheets of "Mylar" or aluminum foil. Mold temperatures of 177.degree. C. (350.degree. F.) were used. The contents were held at contact pressure for 10 minutes. The contents were held at full pressure for 1 minute; the pressure was momentarily released then quickly reestablished and held for an additional two minutes. The sheet was removed and cooled quickly on a cold bench top.
Each example and comparison in the Tables consists of 100 parts by weight matrix polymer. This matrix polymer consists of an ethylene copolymer, as indicated, at 20-100 parts, and polyethylene, 0-80 parts. Varying amounts of other ingredients were added, expressed as parts per 100 parts of the above resin ingredients.
Samples for testing were compression molded according to the procedure outlined above and tests performed according to the procedures outlined in the Table below.
Where blanks appear in the Table property data, the property value was not determined.
______________________________________Table of Test MethodsTest Procedure______________________________________Yield Strength ASTM D-638, D-412Elongation at Yield ASTM D-638, D-412Tensile Strength ASTM D-638, D-412Elongation at Break ASTM D-638, D-412Low Temp. Brittle- ASTM D-746ness (LTB)Limiting Oxygen ASTM D-862Index (LOI)*______________________________________ *Measured to nearest 1%.
______________________________________TABLE OF COMPOSITION______________________________________EVA 1 28 wt. % VA, MI 3EVA 2 18 wt. % VA, MI 0.7EVA 3 9.5 wt. % VA, MI 0.8EEA 15 wt. % ethyl acrylate, MI 0.5E/nBA 30 wt. % n-butyl acrylateHDPE high density polyethyleneMDPE medium density polyethylene (Type II, ASTM D-1248)LLDPE linear low density polyethylene (Type I, ASTM D-1248)Graft Copolymer 1 Graft of maleic anhydride (about 1.7 wt. %) onto EPDM rubber, MI about 3Graft Copolymer 2 Graft of maleic anhydride (about 0.4 wt. %) onto polyethylene, MI about 13Graft Copolymer 3 Graft of maleic anhydride (about 1.0 wt. %) onto polyethylene, MI about 12Ionomer 1 Copolymer of ethylene with 15 wt. % methacrylic acid, 58% neutralized with zinc, MI 0.7Ionomer 2 Copolymer of ethylene with 10 wt. % isobutyl acrylate and 10 wt. % methacrylic acid, 74% neutralized with Zn, MI 1.0EPDM 1 Terpolymer of ethylene with 30 wt. % propylene and 3.7% hexadiene, Mooney viscosity, about 44, ASTM D-16467EPDM 2 Same as EPDM 1, except Mooney viscosity is about 60Melamine Resin "Cyrez" 963 from American Cyanamid CompanyAntioxidant "Irganox" 1010, which is from Ciba Geigy______________________________________ EVA = ethylene/vinyl acetate copolymer MI = melt index EEA = ethylene/ethyl acrylate copolymer E/nBA = ethylene/nbutyl acrylate copolymer EPDM rubber = ethylene/propylene/1,4hexadiene copolymer
Examples 1 and 2 and Comparative Examples C1 to C4, Table 1, show that when EVA, LLDPE, graft copolymer, and Mg(OH).sub.2 are present, the same exhibits superior LOI (at 125 parts Mg(OH).sub.2) to samples in which any of these components is missing. At higher Mg(OH).sub.2 levels, as shown in Examples 3 and 4, Table 2, better than expected LOI's are obtained even in the absence of the polyethylene. The letter L before the LOI value means "less than". Other properties are good, as seen in the Table.
Examples 5-9, Table 3, show that EVA containing 28 wt. % VA is superior to EVA containing only 18% or 9.5% VA. The EVA of higher vinyl acetate content gives compositions with generally higher elongation at break, when compared with the corresponding examples at lower VA levels. The EVA's of lower VA content still give acceptable properties for purposes of this invention.
Examples 10-13, Table 4, show that the presence of some polyethylene based graft copolymer gives significantly improved elongation at break compared to samples which use only the graft copolymer based on ethylene/propylene/diene rubber, at the same total levels of graft copolymer. In these preferred cases, the properties are even further improved when the polyethylene is LLDPE rather than MDPE
Examples 14-17, Table 5, show the advantage of replacing part of the graft copolymer with ethylene/propylene/diene rubber. While Example 14 already shows an excellent balance of properties, replacing progressively more and more of the graft copolymer with EPDM rubber results in still improved elongation, while maintaining tensile strength, and with only slight deterioration of low temperature properties. However, when high levels of EPDM rubber are added, at the expense of graft copolymer Examples 18 and 19 and Comparative Example C5, low temperature properties are compromised. Example 20, however, shows that at 10 parts graft copolymer, adequate low temperature properties can be obtained, provided that the amount of EPDM rubber is limited to about 10 parts.
Examples 21-29, Table 6, further illustrate the invention with compositions of EVA or EEA, LLDPE or MDPE, graft copolymer, and magnesium hydroxide or alumina trihydrate flame retardant. All samples give an acceptable spectrum of properties.
Examples 30-40, Table 7, further illustrate the invention with compositions which also include EPDM rubber.
Examples 41-47, Table 8, and Examples 48-54, Table 9, are similar to the examples in Tables 7 and 6, respectively, except that a small amount of ionomeric copolymer is also present. Examples 52-54 show the effect of adding ionomeric copolymer in increasing amounts. It is apparent from these examples that the presence of the ionomeric copolymer tends to give improved low temperature properties and tensile strength.
Comparative Examples C6 through C9, in Table 10, show that when the graft copolymer is left out of the composition, the elongation properties are greatly reduced. If EPDM rubber is present Comparative Examples C8 and C9, the elongation may be improved somewhat, but the low temperature properties are not improved.
Comparative Examples C-10 to C-12, Table 11, and C-3 and C-4, Table 1, show that when the ethylene copolymer is absent, the balance of properties is not maximized. (In Examples C-10 to C-12, the amount of copolymer plus polyethylene is less than 100 parts. The amounts of other ingredients have not been normalized.)
The Tables follow.
TABLE 1______________________________________ 1, C1, 2, C2, C3, C4______________________________________EVA #1 40 100 40LLDPE 60 100 60 100 100Graft Copol 1 30 30 30 40Graft Copol 2 10 10 10EPDM 1 40Mg(OH).sub.2 125 125 125 89 125 125Antioxidant 1 1 1 0.7 1 1Tensile Str, 1780 1925 1835 1437 1812 1651PSITensile Str, 12.27 13.27 12.65 9.91 12.49 11.38MPa% Retention** 96 98 98 96 102 90% Elong. at 376 414 503 570 307 677Break% Retention** 98 89 92 48 88 101Brittleness:Failures/10 @-45.degree. C. 1 * * * * *-60.degree. C. 5Limiting O.sub.2 31 24 24 26 25 24Index______________________________________ *Values uncertain machine was not working properly. **% Retention means retention of the property after aging the sample at 100.degree. C. for 48 hours in a circulating air oven.
TABLE 2______________________________________Example: 3, 4______________________________________EVA #1 100 100Graft Copolymer 1 30 30Graft Copolymer 2 10 10Mg(OH).sub.2 145 135Antioxidant 1 1Tensile Str, PSI 1589 1559Tensile Str, MPa 10.96 10.75% Retention 93 97% Elong. @ Break 439 422% Retention 80 87Brittleness:Failures/10 @-45.degree. C. 1 2-60.degree. C. 10 10Limiting O.sub.2 Index 32 29______________________________________
TABLE 3______________________________________ 5, 6, 7*, 8, 9______________________________________EVA #1 40 40EVA #2 40 40EVA #3 40MDPE 60 60 60LLDPE 60 60Graft Co- 30 30 30 30 30polymer 1Graft Co- 10 10 10 10 10polymer 2Mg(OH).sub.2 110 110 110 110 110Antioxidant 1 1 1 1Tensile Str, 2123 2071 1973 2386 1834PSITensile Str, 14.64 14.28 13.60 16.45 12.65MPa% Retention 105 98 105 106 103% Elong. @ 325 440 364 308 290Break% Retention 76 92 87 88 70Brittleness:Failures/10 @-45.degree. C. 1 0 0 0 0-60.degree. C. 0 0 2 0 4Limiting O.sub.2 27 26Index______________________________________ *Duplications of this Example resulted in Elongation to Break values of 347, 280, 387, 352, 425, 260. Other property values were in the range of those of Example 6.
TABLE 4______________________________________ 10, 11, 12, 13______________________________________EVA #2 40 40 40 40MDPE 60 60LLDPE 60 60Graft Co- 30 40 30 40polymer 1Graft Co- 10 10polymer 2Mg(OH).sub.2 110 110 110 110Antioxidant 1 1 1 1Tensile Str, 2017 2223 2195 2120PSITensile Str, 13.91 15.33 15.13 14.62MPa% Retention 102 110 100 121% Elong. @ Break 387 229 407 205% Retention 83 90 86 114Brittleness:Failures/10 @-45.degree. C. 1 0 0 0-60.degree. C. 4 1 0 0Limiting O.sub.2 26 26Index______________________________________
TABLE 5______________________________________ 14 15, 16 17 18, C5 19, 20______________________________________EVA #1 40 40 40 40 40 40 30EVA #2 40LLDPE 60 60 60 60 60 60 70MDPE 60Graft Co- 30 20 15 10 10 10polymer 1Graft Co- 10 10 10 10 10polymer 2EPDM 1 10 15 20 30 40 20 10Mg(OH).sub.2 110 110 110 110 110 110 130 110Antioxidant 1 1 1 1 1 1 1 1Tensile Str, 1992 1992 1788 1977 2076 1853 1724 1715PSITensile Str, 13.73 13.73 12.33 13.63 14.31 11.89 11.83MPa% Retention 104 96 108 99 96 87 90% Elong. @ 453 567 535 664 764 754 643 506Break% Retention 92 85 105 97 96 93 90Brittleness:Failures/10 @-45.degree. C. 1 0 0 3 8 10 9 6-60.degree. C. 4 7 7 10 10 10 10 10______________________________________
TABLE 6______________________________________Example: 21, 22, 23, 24______________________________________EVA #1 40 30 40 40EVA #2EEALLDPE 60 70 60 60MDPEGraft Co- 30 30 30 30polymer 1Graft Co- 10 10polymer 2MoO.sub.3Melamine Resin 5Mg(OH).sub.2 125 130 140 130Antioxidant 1 1 1 1Tensile Str, 1848 1939 1805 1806PSITensile Str, 12.74 13.37 12.45 12.45MPa% Retention 99 97 95% Elong. @ 495 437 354 372Break% Retention 95 83 90Brittleness:Failures/10 @-45.degree. C. 1 0 * 1-60.degree. C. 4 6 * 9Limiting O.sub.2 30 L28 29 29Index______________________________________Example: 25, 26, 27 28, 29______________________________________EVA #1 40EVA #2 40 40 40EEA 60MDPE 60 60LLDPE 40 60 60Graft Co- 30 30 30 30 30polymer 1Graft Co- 10 10 10 10polymer 2MoO.sub.3 10Melamine Resin 5Mg(OH).sub.2 110 110 55 124Alumina 110 55 20TrihydrateAntioxidant 1 1 1 1Tensile Str, 1773 1872 1660 2143 2218PSITensile Str, 12.22 12.91 11.45 14.78 15.30MPa% Retention 95 104 113 106% Elong. @ 321 411 356 308 195Break% Retention 72 82 89 89Brittleness:Failures/10 @-45.degree. C. 1 0 0 1 2-60.degree. C. 1 0 2 0 5Limiting O.sub.2 L28 29 28Index______________________________________ *Values uncertain machine was not working properly.
TABLE 7__________________________________________________________________________Example: 30, 31 32, 33** 34, 35, 36, 37, 38 39, 40__________________________________________________________________________EVA #1 40 30 40 40 30 40 40 40 30 40EEA 40LLDPE 60 60 70 60 60 70 60 60 60 70 60Graft 15 20 10 20 30 15 20 20 10 20 10Copol 1Graft 10 10 15 15 10 15 10 10 10 15 15Copol 2EPDM 1 15 10 20 15 10 20 10 10 20 15 20Mg(OH).sub.2 135 135 145 150 150 150 110 154 135 150 145Antioxidant 1 1 1 1 1 1 1 1 1 1 1Tensile Str, 1834 1780 1800 1772 1762 1511 1979 1403 1700 1646 1658PSITensile Str, 12.65 12.27 12.41 12.22 12.15 10.42 13.65 9.67 11.72 11.35 11.43MPa% Retention 93 90 93 94 104 112 95 94% Elong. @ 552 435 599 482 418 446 550 309 599 349 549Break% Retention 94 77 89 85 97 123 91 103Brittleness:Failures/10 @-45' C. 1 2 8 2 * * 0 10 5 1 7-60' C. 10 8 9 10 4 10 10 8 10Limiting O.sub.2 30 L28 29 29 30 31 L28 L28 L28 L28 L28Index__________________________________________________________________________ *Brittleness Brittleness not accurately recorded due to machine malfunction. **When When graft copolymer 2 is replaced with an ethylene/methacrylic acid copolymer of MI 3, good results are obtained.
TABLE 8______________________________________Example: 41, 42, 43, 44 45, 46, 47______________________________________EVA #1 40 40 40 40 50 40 30LLDPE 60 60 60 60 50 60 70Graft Co- 10 10 20 20 15 15 35polymer 1Graft Co- 10 10 10 10 10polymer 2Graft Co- 10polymer 3Ionomer 1 3 3 3 3 3 5Ionomer 2 3EPDM 1 20 20 10 10 15 15 10Melamine ResinMoO.sub.3 4 4 4 4 4 4Mg(OH).sub.2 135 135 135 135 135 135 100Antioxidant 1 1 1 1 1 1 0.2Carbon Black 2Tensile Str, 1624 1496 1844 1635 1424 1589 2400PSITensile Str, 11.20 10.31 12.71 11.27 9.82 10.96 16.55MPa% Retention 100 103 90 99% Elong. @ 502 527 503 375 434 502 392Break% Retention 106 79 87 99Brittleness:Failures/10 @-45.degree. C. 3 1 2 0-60.degree. C. 10 7 10 1Limiting O.sub.2 31 30 29 30 29 29Index______________________________________
TABLE 9______________________________________Example: 48, 49, 50 51 52, 53, 54______________________________________EVA #1 40 40EVA #2 40 40 40 40 40MDPE 60 60 60 60LLDPE 60 60 60Graft Co- 20 30 30 30 20 20 20polymer 1Graft Co- 10 10 20 20 20polymer 2Ionomer 1 5 5 3Ionomer 2 5 3 10MoO.sub.3 4Mg(OH).sub.2 110 152 110 145 110 110 110Antioxidant 1 1.4 1 1 1Carbon Black 2 2.8Tensile Str, 2560 2700 1870 2088 1908 2149 2175PSITensile Str, 17.65 18.62 12.89 14.40 13.16 14.82 15.00MPa% Retention 106 99 101% Elong. @ 223 199 395 193 287 415 337Break% Retention 90 59 77Brittleness:Failures/10 @-45.degree. C. 0 0 1 0 2 0 1-60.degree. C. 0 0 8 3 7 0 1LOI 32______________________________________
TABLE 10______________________________________Example: C6, C7, C8, C9______________________________________EVA #2 40 33EVA #3 40EEAE/nBA 40MDPE 60 60 60LLDPE 67EPDM 2 20 11Mg(OH).sub.2 110 110 110 110Antioxidant 1 1 1 1Carbon Black 2 2 2Tensile Str, 2440 1600 1520 1510PSITensile Str, 16.82 11.03 10.48 10.41MPa% Retention% Elong. @ 6 8 514 72Break% RetentionBrittleness:Failures/10 @-45.degree. C. 10 10-60.degree. C. 10Limiting O.sub.2 Index______________________________________
TABLE 11______________________________________Example: C10, C11, C12______________________________________MDPE 60 50HDPE 60Graft Copol 1 10 10EPDM 1 40EPDM 2 30 40Mg(OH).sub.2 110 110 110Antioxidant 1 1 1Carbon Black 2 2 2Tensile Str, 1480 1210 1500PSITensile Str, 10.20 8.34 10.34MPa% Elong. @ 199 394 8BreakBrittleness:Failures/10 @ 10 10-45.degree. C.______________________________________
TABLE 12______________________________________Example: 55, 56, 57______________________________________EVA #1 40 40 40LLDPE 60 60 60Graft Co- 20 20 20Polymer 1Graft Copolymer of 15 -- --Maleic Anhydride(1.1 wt %) on EVA(18 wt % VA) MI 2.6Graft Copolymer of -- 15 --Maleic Anhydride(0.9 wt %) on EVA(9 wt % EVA) MI 0.8E/MAA (9%), MI 3 -- -- 15Antioxidant 1 1 1Carbon Black -- -- 3.4Mg(OH).sub.2 135 150 150Tensile Str. PSI 1688.0 1750.0 1846.0Tensile Str. MPa 11.6 12.1 12.7% Elong. @ Break 405.0 475.0 233.0Brittleness:Failures/10 @ -45 C. 0.0Failures/10 @ -60 C. 0.0Limiting O.sub.2 Index 29.0 30.0 27.0______________________________________

Number	Date	Country
131358	May 1983	EPX
0207734	Jun 1986	EPX
0013718	Jan 1980	JPX
0002358	Jan 1983	JPX
0184237	May 1983	JPX

Ethylene copolymer compositions

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