Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Polymers from only ethylenic monomers or processes of...
Reexamination Certificate
1999-08-31
2002-07-09
Wu, David W. (Department: 1713)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Polymers from only ethylenic monomers or processes of...
C526S127000, C526S124100, C526S160000, C526S161000, C526S942000, C526S348600, C502S104000, C502S152000
Reexamination Certificate
active
06417298
ABSTRACT:
FIELD OF INVENTION
The present invention relates to a process utilizng a metallocene catalyst for producing ethylene/olefin interpolymers, which for a given melt index (MI) and density, have reduced melting peak temperatures (T
m
). Melting peak temperature (T
m
) is alternatively referred to as melt transition temperature or melting point. The present invention also relates to a process for reducing the melting peak temperature (T
m
) of ethylene/olefin interpolymers having a given melt index and density. Additionally, this invention relates to novel ethylene/olefin interpolymers, and films and articles of manufacture produced therefrom.
BACKGROUND OF INVENTION
Polyethylene and interpolymers of ethylene are well known and are useful in many applications. In particular linear interpolymers of ethylene, also known as copolymers, terpolymers, and the like of ethylene, possess properties which distinguish them from other polyethylene polymers, such as branched ethylene homopolymers commonly referred to as LDPE (low density polyethylene). Certain of these properties are described by Anderson et al, U.S. Pat. No. 4,076,698.
A particularly useful polymerization medium for producing polymers and interpolymers of ethylene is a gas phase process. Examples of such are given in U.S. Pat. Nos. 3,709,853; 4,003,712; 4,011,382; 4,302,566; 4,543,399; 4,882,400; 5,352,749 and 5,541,276 and Canadian Patent No. 991,798 and Belgian Patent No. 839,380.
Metallocene catalysts are known for polymerizing and interpolymerizing ethylene. Metallocene catalysts comprise at least one transition metal component having at least one moiety selected from substituted or unsubstituted cyclopentadienyl, substituted or unsubstituted pentadienyl, substituted or unsubstituted pyrrole, substituted or unsubstituted phosphole, substituted or unsubstituted arsole, substituted or unsubstituted boratabenzene, and substituted or unsubstituted carborane, and at least one co-catalyst component. Typical organometallic co-catalysts are alkyl aluminoxanes, such as methyl aluminokane, and boron containing compounds such as tris(perfluorophenyl)boron and salts of tetrakis(perfluorophenyl)borate.
The metallocene catalysts can be supported on an inert porous particulate carrier.
The use of internal electron donors with metallocene catalysts is disclosed in U.S. Pat. No. 5,106,804. The use of external electron donors with metallocene catalysts to control molecular weight is disclosed in U.S. Pat. No. 5,883,203.
Illustrative examples of electron donors include anhydrides, acid halides, ethers, thioethers, aldehydes, ketones, imines, amnines, amides, nitriles, isonitriles, cyanates, isocyanates, thiocyanates, isothiocyanates, thioesters, dithioesters, carbonic esters, hydrocarbyl carbamates, hydrocarbyl thiocarbamates, hydrocarbyl dithiocarbamates, urethanes, sulfoxides, sulfones, sulfonamides, organosilicon compounds containing at least one oxygen atom, and nitrogen, phosphorus, arsenic or antimony compounds connected to an organic group through a carbon or oxygen atom.
SUMMARY OF THE INVENTION
Applicants have unexpectedly found that the addition of at least one compound comprising at least one element from Group 15 and/or Group 16 of the Periodic Table of Elements, herein referred to as a modifier, in a process utilizing metallocene catalysts for preparing ethylene/olefin interpolymers, having a given melt index and density, reduces the melting peak temperature (T
m
) of the ethylene/olefin interpolymer. The melting peak temperature (T
m
) values herein are obtained by Differential Scanning Calorimetry in accordance with ASTM D 3418-97.
The polymerization process of the present invention for producing an ethylene/olefin interpolymer having, at a given melt index and density, a reduced melting peak temperature (T
m
) comprises the introduction into a polymerization medium containing ethylene and at least one or more other olefin(s), at least one metallocene catalyst comprising at least one transition metal component having at least one moiety selected from substituted or unsubstituted cyclopentadienyl, substituted or unsubstituted pentadienyl, substituted or unsubstituted pyrrole, substituted or unsubstituted phosphole, substituted or unsubstituted arsole, substituted or unsubstituted boratabenzene, and substituted or unsubstituted carborane, and at least one co-catalyst component, and at least one modifier, wherein the modifier is present in the polymerization medium in an amount sufficient to reduce the melting peak temperature (T
m
) of the ethylene/olefin interpolymer to a level lower than would result in the same polymerization process in the absence of the modifier.
The present invention also relates to a process for reducing the melting peak temperature (T
m
) of an ethylene/olefin interpolymer having a given melt index (MI) and density. The process comprises introducing a modifier, into a polymerization process containing ethylene and at least one or more other olefin(s) and at least one metallocene catalyst comprising at least one transition metal component having at least one moiety selected from substituted or unsubstituted cyclopentadienyl, substituted or unsubstituted pentadienyl, substituted or unsubstituted pyrrole, substituted or unsubstituted phosphole, substituted or unsubstituted arsole, substituted or unsubstituted boratabenzene, and substituted or unsubstituted carborane, and at least one co-catalyst component, in an amount sufficient to reduce the melting peak temperature (T
m
).
In a further embodiment of the present invention, it has been found desirable to add at least one or more organometallic compounds, in addition to the metallocene catalyst(s), to the polymerization medium.
The present invention also relates to ethylene/olefin interpolymers, which for a given melt index and density, have a reduced melting peak temperature (T
m
).
All mention herein to elements of Groups of the Periodic Table are made in reference to the Periodic Table of the Elements, as published in “Chemical and Engineering News”, 63(5), 27, 1985. In this format, the Groups are numbered 1 to 18.
DETAILED DESCRIPTION OF THE INVENTION
Applicants have unexpectedly found that the addition of at least one compound comprising at least one element from Group 15 and/or Group 16 of the Periodic Table of Elements, herein referred to as a modifier, in a process utilizing metallocene catalysts for preparing ethylene/olefin interpolymers, having a given melt index and density, reduces the melting peak temperature (T
m
) of the ethylene/olefin interpolymer. The melting peak temperature (T
m
) values herein are obtained by Differential Scanning Calorimetry in accordance with ASTM D 3418-97.
The polymerization process of the present invention for producing an ethylene/olefin interpolymer having, at a given melt index and density, a reduced melting peak temperature (T
m
) comprises the introduction into a polymerization medium containing ethylene and at least one or more other olefin(s), at least one metallocene catalyst comprising at least one transition metal component having at least one moiety selected from substituted or unsubstituted cyclopentadienyl, substituted or unsubstituted pentadienyl, substituted or unsubstituted pyrrole, substituted or unsubstituted phosphole, substituted or unsubstituted arsole, substituted or unsubstituted boratabenzene, and substituted or unsubstituted carborane, and at least one co-catalyst component, and at least one modifier, wherein the modifier is present in the polymerization medium in an amount sufficient to reduce the melting peak temperature (T
m
) of the ethylene/olefin interpolymer to a level lower than would result in the same polymerization process in the absence of the modifier.
The present invention also relates to a process for reducing the melting peak temperature (T
m
) of an ethylene/olefin interpolymer having a given melt index (MI) and density. The process comprises introducing a modifier, into a polymerization process containing ethylene and at least one or more other olefin(s) and at least one
Ford Randal Ray
Vanderbilt Jeffrey James
Williams Darryl Stephen
Eastman Chemical Company
Graves, Jr. Bernard J.
Harlan R.
Wood Jonathan D.
Wu David W.
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