Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Polymers from only ethylenic monomers or processes of...
Reexamination Certificate
1998-05-13
2001-07-17
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...
C526S351000, C526S943000
Reexamination Certificate
active
06262203
ABSTRACT:
The present invention relates to thermoplastic elastomers such as polypropylene and related polyolefin types, being more specifically concerned with polypropylenes exhibiting elastomeric properties and catalysts for making the same.
BACKGROUND
Tullock and co-workers,
(Tullock, C. W.; Tebbe, F. N.; Mulhaupt, R.; Ovenall, D, W.; Saltarquist, R. A.; Ittel, S. D.
J. Polym. Sci. Part A
(1989) 27 3063; Collette, J. W.; Tullock, C. W.; MacDonald, R. N.; Buck, W. H.; Su. A. C. L.; Harrell, J. R.; Mulhaupt, R.; Anderson, B. C.
Macromolecules
(1989) 22 2851),
have obtained polypropylenes exhibiting elastomeric properties using alumina-supported bis(arene) Ti, Zr, and Hf catalysts with materials of heterogeneous composition comprising chains soluble in ethyl ether, hexane, heptane and octane, as well as octane-insoluble ones. Each fraction contains polypropylene chains considered to be uniform in structure. The total polymer exhibits poor elastomeric properties. Hysterisis effects showing 110% permanent set after 300% elongation were obtained.
Ewen et al. and Kaminsky et al.
(Ewen, J. A.
J. Am. Chem. Soc.
1984 106, 6355.; Ewen, J. A. “Ligand Effects on Metallocene Catalyzed Polymerizations”, in Catalytic Polymerization of Olefins; Keii, T.; Soga, K., Eds.; Elsevier, New York, 1986, p. 271; (c) Ewen, J. A.; Haspeslagh, L.; Atwood, J. L.; Zhang, H.
J. Am. Chem. Soc.
1987 109 6544; Kaminsky, W.; Kuiper, K.; Brintzinger, H. H.; Wild, F. R. W. P.
Angew. Chem. Int. Ed. Engl.
1985-24 507), described symmetrical
ansa
-metallocene compounds which also produce heterogenous mixture of polypropylenes; examples are
rac
-ethylene bis(indenyl) zirconium dichloride and
rac
-ethylene bis(tetrahydroindenyl) zirconium dichloride. We have discovered new nonsymmetric
ansa
-metellocene systems, exemplified by
rac
-ethylidene (1-&eegr;
5
-tetramethylcyclopentadienyl) (1-&eegr;
5
-indenyl)-dichlorotitanium (1) which produces homogeneous homopolypropylene having the attributes of a thermoplastic elastomeric (TPE) material, which properties are derived from intrinsic molecular characteristics of the macromolecular chain, and, unlike the hecerogenotis polymers of Tullock et al, which have poor elastomeric properties resulting from the blend of amorphous and stereo regular polypropylenes.
OBJECT OF THE INVENTION
A principal object of this invention, accordingly, is to provide a new thermoplastic elastomeric material of the olefin class and one that can be produced with a single monomer and a novel method of producing the same.
A further object is to provide a novel thermoplastic elastomeric polypropylene material.
Still a further object is to provide new catalysts for forming such novel products.
Other and further objects will be explained hereinafter and are more particularly delineated in the appended claims.
SUMMARY
In summary, however, from one of its important aspects, the invention embraces a novel catalytic new composition of matter of formula rac-ethylidene (1-&eegr;
5
terramethylcyclopencadienyl) (1-&eegr;
5
-indenyl) dichloro-M, where M is a metal selected from the group consisting of Ti, Zr and Hf. The invention also involves novel thermoplastic elastomeric olefin products including a thermoplastic elastomeric olefin polymer having alternate blocks of homopolymerized stereo regular crystallizable segments and of homopolymerized stereo irregular non-crystallizable amorphous segments, the former segment aggregating into crystalline domains to act as physical crosslinks, thus enabling elastic recovery of stretched specimens upon release of the strain. Preferred and best mode embodiments, formations and method for carrying out the same are hereinafter set forth in detail.
REFERENCES:
patent: 3175999 (1965-03-01), Natta et al.
patent: 3784502 (1974-01-01), Gobran et al.
patent: 4522982 (1985-06-01), Ewen
patent: 4849487 (1989-07-01), Kaminsky et al.
patent: 5594080 (1997-01-01), Waymouth et al.
patent: 5969070 (1999-10-01), Waymouth et al.
Chien James C. W.
Rausch Marvin D.
Rabago R.
Rines and Rines
The Academy of Applied Science
Wu David W.
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