Process for producing cyclic olefin based polymers, cyclic olefi

Details Process for producing cyclic olefin based polymers, cyclic olefi Process for producing cyclic olefin based polymers, cyclic olefi

1992-06-05

1997-05-13

Teskin, Fred

Synthetic resins or natural rubbers -- part of the class 520 ser

Synthetic resins

Polymers from only ethylenic monomers or processes of...

526113, 526115, 526116, 526117, 526118, 526119, 526126, 526127, 526132, 526134, 526148, 526151, 526160, 526161, 526170, 526172, 526308, 525210, 525211, 524553, 524554, C08F23204, C08F 464

Patent

active

056293984

DESCRIPTION:

BRIEF SUMMARY
FIELD OF THE INVENTION

The present invention relates to a process for producing a cyclic olefin based polymer, and particularly relates to a process for producing a cyclic olefin polymer and a cyclic olefin/alpha-olefin copolymer without opening rings of the cyclic olefin.
Further, the present invention relates to a novel cyclic olefin/alpha-olefin copolymer, and a composition and a molded article comprising the copolymer.


RELATED ART

It is known that cyclic olefins can be polymerized in the presence of a Ziegler-Natta catalyst. In most of the cases, the cyclic olefins suffer ring opening during the polymerization to give polymers with opened rings.
On the contrary to this process, cyclic olefins can be polymerized without suffering ring opening in accordance with the following methods (a) to (e).
(a) Japanese Patent Application Laid-Open Gazette (Kokai) No. Sho 64-66216 describes a process for polymerizing a cyclic olefin without suffering ring opening to obtain an isotactic polymer, in the presence of a catalyst composed of a stereo-rigid metallocene compound, particularly ethylenebis(indenyl)zirconium dichloride, and aluminoxane.
(b) Kokai No. Sho 61-271308 discloses a process for copolymerizing a cyclic olefin and an alpha-olefin without suffering ring opening, in the presence of a catalyst composed of a soluble vanadium compound and an organoaluminum compound.
(c) Kokai No. Sho 61-221206 and Kokai No. 64-106 describe a process for copolymerizing a cyclic olefin and an alpha-olefin without suffering ring opening, in the presence of a catalyst composed of a transition metal compound and aluminoxane.
(d) Kokai No. Sho 62-252406 describes a process for producing an ethylene/cyclic,olefin random copolymer having an ethylene content of 40 to 90 mol % with the use of a catalyst composed of a soluble vanadium compound and an organoaluminum compound.
(e) Kokai No. Hei 3-45612 discloses a process for producing a homopolymer and a copolymer of a polycyclic olefin with the use of a catalyst composed of a specific metallocene compound and aluminoxane.
However, the polymerization processes (a), (c) and (d) require use of a great amount of aluminoxane. Thus, a substantial amount of a metal will remain in the polymerized products, resulting in deterioration and coloring of the products. In these processes, after polymerization, deashing treatment of the resultant products should be sufficiently conducted. Thus, these processes have a problem in productivity.
Further, the catalysts used in the processes (b) and (d) are inferior due to extremely poor catalytic activities. In addition, an ethylene-rich copolymer obtained by the process (d) shows clear melting point and poor random configuration. Furthermore, in Kokai No. Sho 3-45612 (Process (e)), it is not proved in the working examples that a copolymer having a cyclic olefin content of 40 mol % or more can be produced.
On the other hand, studies on olefin polymerization with use of a cationic transition metal complex, have been made since many years ago. There are many reports as indicated as follows. However, each process has some problems.
(f) Natta et al. reported that ethylene can be polymerized in the presence of a catalyst composed of titanocene dichloride and triethylaluminum (J. Polymer Sci., 26, 120 (1964). Further, Breslow et al. reported polymerization of ethylene with use of a titanocene dichloride/dimethylaluminum chloride catalyst (J. Am. Chem. Soc., 79, 5072 (1957). Furthermore, Dyachkovskii et al. suggested that polymerization activities in ethylene polymerization using a titanocene dichloride/dimethylaluminum chloride catalyst are derived from a titanocenemonomethyl cation (J. Polymer Sci., 16, 2333 (1967).
However, the ethylene activities in these processes are extremely low.
(g) Jordan et al. reported synthesis and isolation of [biscyclopentadienylzirconium methyl(tetrahydrofuran)][tetraphenylboric acid] resulting from the reaction of zirconocenedimethyl and silver tetraphenylborate, and ethylene polymerization using the thus synthesized compoun

REFERENCES:
patent: 4948856 (1990-08-01), Minchak et al.
patent: 5066741 (1991-11-01), Campbell, Jr.
patent: 5087677 (1992-02-01), Brekner et al.
patent: 5153157 (1992-10-01), Hlatky et al.
Zdunneck et al, J. Organometal. Chem., 22 (1970) 659-663.
English Language Translation of Japanese Kokai Pat. No. 61-221206, published Oct. 1, 1986.
Tadnor et al, Principles of Polymer Processing, Wiley-Interscience, N.Y., 36-7, 1979.

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