Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Polymers from only ethylenic monomers or processes of...
Reexamination Certificate
2000-09-05
2002-02-05
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...
C502S113000, C502S103000, C502S117000, C502S154000, C502S153000, C526S348600, C526S943000, C526S113000, C526S348500, C526S348200
Reexamination Certificate
active
06344528
ABSTRACT:
FIELD OF THE INVENTION
The present invention relates to a catalyst for olefin (co)polymerization and to a process for the production of olefin (co)polymers. More particularly, the present invention relates to a catalyst for olefin (co)polymerization which has high polymerization activity and can produce olefin (co)polymers having a high molecular weight and a narrow molecular weight distribution and to a process for the production of olefin (co)polymers using the same.
By the term “(co)polymerization” as used herein is meant copolymerization or polymerization.
BACKGROUND OF THE INVENTION
Olefin polymers and copolymers such as polypropylene and polyethylene are excellent in mechanical properties and resistance to chemicals and very useful in view of well balanced economic advantages so that they are used widely in various plastic article fields. The olefin (co)polymers have hitherto been produced by (co)polymerization of olefins using a so-called Ziegler-Natta catalyst, which comprises a transition metal catalyst component, examples of which include titanium trichloride, titanium tetrachloride, and a carrier such as magnesium chloride carrying at least one above described titanium chlorides thereon, and an organoaluminum compound in combination.
On the other hand, in recent years, use of a catalyst which comprises a combination of metallocene and aluminoxane, different than conventional catalyst systems, in (co)polymerization of olefins gives olefin (co)polymers and the olefin (co)polymers obtained with the metallocene series catalyst have a narrow molecular weight distribution and in the case of copolymers comonomers are copolymerized uniformly; hence, it is known that more uniform olefin (co)polymers are obtained.
However, as described in Eur. Polym. J., 32, 331 (1966), the olefin (co)polymers obtained with metallocene catalysts have a low molecular weight and from practical reasons, catalyst for olefin (co)polymerization which can provide olefin (co)polymers having a higher molecular weight are desired.
Japanese Patent Application Laid-open Nos. 7-233210, 7-233211 and 7-233212 describe that the use of metallocene catalysts containing two or more kinds of transition metals gives rise to high molecular weight polymers. In this case, however, there is a problem that a plurality kinds of active species participate in polymerization of polymers with different molecular weights, so that the molecular weight distribution becomes broader and it is difficult to obtain homogeneous olefin (co)polymers.
SUMMARY OF THE INVENTION
The present invention has been made in view of the above and an object of the present invention is to provide a catalyst for olefin (co)polymerization which shows high polymerization activity and which can produce olefin (co)polymers having a high molecular weight and a narrow molecular weight distribution and a process for producing olefin (co)polymers using the same. More particularly, an object of the present invention is to provide a catalyst which can produce copolymers of ethylene and 1-hexene having a high molecular weight and a narrow molecular weight distribution and a process for producing copolymers of ethylene and 1-hexene using the same.
As a result of intensive investigation with view to achieving the above object, the present inventors have found that (co)polymerization of olefins with a metallocene compound having a specified structure and aluminoxane carried together on a fine particulate carrier as a catalyst in the presence of an organoaluminum compound gives rise to olefin (co)polymers having a high molecular weight and a narrow molecular weight distribution, thus completing the present invention.
That is, the present invention is to provide a catalyst for olefin (co)polymerization comprising a transition metal compound represented by general formula (I) or (II) below and aluminoxane carried on a fine particulate carrier.
{[&eegr;-C
5
R
1
5
M
1
X
1
2
][&mgr;-&eegr;-C
5
R
2
4
-SiR
3
2
-&eegr;-C
9
R
4
6
][&eegr;-C
5
R
5
5
M
1
X
2
2
]} (I)
{[&eegr;-C
5
R
6
5
M
2
X
3
2
][&mgr;-&eegr;-C
5
R
7
4
-B-&eegr;-C
5
R
8
4
][&eegr;-C
5
R
9
5
M
2
X
4
2
]} (II)
[In formulae (I) and (II) above, &eegr;-C
5
R
1
5
, &eegr;-C
5
R
2
4
, &eegr;-C
5
R
5
5
, &eegr;-C
5
R
6
5
, &eegr;-C
5
R
7
4
, &eegr;-C
5
R
8
4
, and &eegr;-C
5
R
9
5
represent substituted cyclopentadienyl groups, respectively. Each of R
1
, R
2
, R
5
, R
6
, R
7
, R
8
, and R
9
independently represents a hydrogen atom or a hydrocarbon group having 1 to 20 carbon atoms which may contain a silicon atom, all R
1
s, R
2
s, R
5
s, R
6
s, R
7
s, R
8
s, and R
9
s may be the same or different, respectively, and any two adjacent R
1
s, R
2
s, R
5
s, R
6
s, R
7
s, R
8
s, and R
9
s may combine to form at least one hydrocarbon ring which may contain a silicon atom around the cyclopentadienyl ring, respectively.
In formula (I) above, &eegr;-C
9
R
4
6
represents a substituted indenyl group. R
4
represents a hydrogen atom or a hydrocarbon group having 1 to 20 carbon atoms which may contain a silicon atom, all R
4
s may be the same or different, and any two adjacent R
4
s may combine to form at least one hydrocarbon ring which may contain a silicon atom around the indenyl ring. SiR
3
2
is a crosslinking group and R
3
is a hydrocarbon group having 1 to 20 carbon atoms.
In formula (II) above, B is a crosslinking group consisting of a hydrocarbon containing a silicon atom, its backbone chain containing at least one silicon atom and its chain length being 2 to 20 atoms.
In formulae (I) and (II) above, M
1
and M
2
represent transition metals selected from the group consisting of titanium, zirconium and hafnium, respectively.
Further, in formula (I) above, each of X
1
and X
2
independently and, in formula (II) above, each of X
3
and X
4
independently represents a hydrogen atom, a halogen atom or a hydrocarbon group having 1 to 20 carbon atoms.]
The present invention is also to provide a catalyst for copolymerization of ethylene and 1-hexene comprising a transition metal compound represented by general formula (I) or (II) above and aluminoxane carried on a fine particulate carrier.
Further, the present invention is to provide a process for olefin (co)polymerization by (co)polymerizing olefins in the presence of a catalyst and an organoaluminum compound, in which the catalyst is a catalyst comprising a transition metal compound represented by general formula (I) or (II) above and aluminoxane carried on a fine particulate carrier.
Further more, the present invention is to provide a process for polymerization of ethylene and 1-hexene by copolymerizing ethylene and 1-hexene in the presence of a catalyst and an organoaluminum compound, in which the catalyst is a catalyst comprising a transition metal compound represented by general formula (I) or (II) above and aluminoxane carried on a fine particulate carrier.
The catalyst for olefin (co)polymerization as described above shows a high polymerization activity in the production of olefin (co)polymers and the process for producing olefin (co)polymers using it can give olefin (co)polymers having a high molecular weight and a narrow molecular weight distribution.
DETAILED DESCRIPTION OF THE INVENTION
Hereafter, the present invention will be described in more detail. First, explanation will be made on the catalyst for olefin (co)polymerization of the present invention.
(1) Catalyst for Olefin (co)polymerization of the Present Invention
The catalyst for olefin (co)polymerization of the present invention is a carried type catalyst comprising a transition metal compound represented by general formula (I) or (II) above and aluminoxane carried on a fine particulate carrier.
The transition metal compound represented by general formula (I) above used in the catalyst for olefin (co)polymerization of the present invention is not limited particularly so far as it is a metallocene compound represented by general formula (I) above, but examples of the above transition meta
Saito Jun
Tsutsui Mototake
Ushioda Tsutomu
Cheung William K
Chisso Corporation
McDermott & Will & Emery
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