Catalyst – solid sorbent – or support therefor: product or process – Catalyst or precursor therefor – Plural component system comprising a - group i to iv metal...
Reexamination Certificate
2000-08-10
2004-05-18
Cheung, William (Department: 1713)
Catalyst, solid sorbent, or support therefor: product or process
Catalyst or precursor therefor
Plural component system comprising a - group i to iv metal...
C526S127000, C526S129000, C526S135000, C526S141000, C526S160000, C556S179000, C556S187000, C556S190000
Reexamination Certificate
active
06737379
ABSTRACT:
TECHNICAL FIELD
The present invention relates to a novel aluminum-oxy compound, a carrier for olefin polymerization catalyst comprising the aluminum-oxy compound, a catalyst component for olefin polymerization, and a method for producing polyolefins. More precisely, it relates to a novel aluminum-oxy compound having high polymerization activity and capable of giving polyolefins with good polymer morphology, a carrier for olefin polymerization catalysts comprising the aluminum-oxy compound, a catalyst component for olefin polymerization, and a method for producing polyolefins.
BACKGROUND OF THE INVENTION
In the field of polyolefin production, forwarded is the development of catalyst systems applicable to bulk polymerization, vapor-phase polymerization, slurry polymerization and others, for catalysts with transition metal compounds, typically IV Group transition metal compounds carried on inorganic porous carriers (these will be hereinafter referred to as transition metal-carrying catalysts).
The polymerization systems require high polymerization activity and good polymer morphology, for which is desired the development of high-activity catalysts capable of giving high bulk-density polyolefins.
On the other hand, it is known that aluminum-oxy compounds, especially methylalumoxane are useful promoters for metallocene catalysts. For example, various techniques of producing on-carrier catalysts have been disclosed, for example, using a solution of methylalumoxane in the step of carrying transition metal compounds on inorganic porous carriers. However, it is known that aluminum-oxy compounds produced from organoaluminums often contain impurities of non-reacted organoaluminiums and insoluble side products (gels). Therefore, the polymerization activity per aluminum atom of aluminum-oxy compounds is low, and a large amount of the compound must be used for polymerization, thereby inevitably resulting in the increase in the production costs. In addition, a large amount of aluminum will remain in the polymers produced. Such problems with aluminum-oxy compounds are serious for their industrial applications. To solve the problems, various proposals have heretofore been made (Japanese Patent Application Laid-Open Nos. 211307/1986, 130601/1988, 16803/1989, 167307/1990).
According to the techniques proposed, the activity per aluminum compound of aluminum-oxy compounds could be increased in some degree, but such aluminoxanes are still problematic in that they are poorly soluble and are difficult to handle, and, in addition, they often worsen the quality and even the tone of the polymers produced. Therefore, further improving the compounds is desired.
Also proposed is a method of combining methylaluminoxane and some other organoaluminum compounds (Japanese Patent Laid-Open Nos. 260602/1985, 130604/1985, 89506/1988, 178108/1988, 218707/1988, 9206/1989, 315407/1989, 22306/1990, 167310/1990).
According to the techniques proposed, the amount of methylaluminoxane to be used could be reduced in some degree, but the activity per aluminum of the combined systems is still unsatisfactory. Therefore, further improving them is desired.
Apart from the problems with aluminum-oxy compounds themselves noted above, there is still another problem with transition metal-carrying catalyst systems comprising a transition metal, an inorganic porous carrier and an aluminum-oxy compound in that their catalytic activity is much lower than that of non-carrier homogeneous-phase catalyst systems. To solve this problem, various proposals have been made.
For example, International Patent Publication No. 507515/1997 discloses a method of preparing an on-carrier catalyst, for which the alumoxane solution to be used is pre-treated to remove the gel component from it. The object of the technique disclosed is to improve polymer morphology, but, according to the method, it is difficult to increase the activity of the catalyst. In addition, the technique to improve polymer morphology is limited.
International Patent Publication Nos. 511044/1996, 503008/1997, 505340/1997 and 507517/1997 disclose various methods of using alumoxane solutions for producing on-carrier catalysts. However, the on-carrier catalysts produced according to the methods are problematic in that their catalytic activity is much lower than that of non-carrier homogeneous-phase catalysts.
U.S. Pat. No. 5,157,137 discloses a method of processing an alumoxane solution with alkali to remove the gel component from it. However, the technique disclosed is ineffective for increasing the activity of catalysts, and, in addition, the alkali treatment is problematic in that it increases the cost of alumoxanes.
As mentioned above, the current situation in the art regarding transition metal-carrying catalyst systems that comprise a transition metal compound, an inorganic porous carrier and an aluminium-oxy compound is that no one could obtain on-carrier catalysts of which the polymerization activity is on the same level as that of non-carrier homogeneous-phase catalysts and which could give high bulk-density polyolefins.
We, the present inventors have made the present invention from the viewpoints noted above, and the object of the invention is to provide a novel aluminum-oxy compound having high polymerization activity and capable of giving polyolefins with good polymer morphology, a carrier for olefin polymerization catalysts comprising the aluminum-oxy compound, a catalyst component for olefin polymerization, and a method for producing polyolefins.
We, the present inventors have assiduously studied, and, as a result, have found a specific aluminum-oxy compound which is obtained from a reaction product of an organoaluminum compound and water and which contains neither a residual organoaluminum component nor a gel compound; a carrier for olefin polymerization catalysts which is obtained from the aluminum-oxy compound and an inorganic compound; and an olefin polymerization catalyst which is obtained by contacting the carrier with a transition metal compound. We have further found that the olefin polymerization catalyst has high polymerization activity and that polyolefins with good polymer morphology can be obtained by the use of the catalyst. On the basis of these findings, we have completed the present invention.
Specifically, the invention provides an aluminum-oxy compound, a carrier for olefin polymerization catalysts, a catalyst component for olefin polymerization, and a method for producing polyolefins, which are as follows:
1. An aluminium-oxy compound obtained through reaction of an organoaluminum compound with water, which is soluble in hydrocarbon solvents and in which the amount of the organoaluminum compound remaining is at most 10% by weight as measured through
1
H-NMR.
2. A carrier for olefin polymerization catalysts, which comprises the aluminum-oxy compound of above 1 and an inorganic compound having at least one element selected from Groups 2 to 4 or Groups 12 to 14 of the Periodic Table.
3. The carrier for olefin polymerization catalysts of above 2, wherein the inorganic compound is an oxide.
4. A catalyst component for olefin polymerization, which comprises the carrier for olefin polymerization catalysts of above 2 or 3 and a transition metal compound.
5. The catalyst component for olefin polymerization of above 4, wherein the transition metal compound is selected from Group 4 or Groups 8 to 10 of the Periodic Table.
6. The catalyst component for olefin polymerization of above 4 or 5, wherein the transition metal compound of Group 4 of the Periodic Table is any one selected from transition metal compounds of the following general formulae (I) to (III):
where R
1
to R
6
each independently represent a hydrogen atom, a halogen atom, a hydrocarbon group having from 1 to 20 carbon atoms, or a halogen-containing hydrocarbon, group having from 1 to 20 carbon atoms; the groups of at least one pair of R
3
and R
4
, R
4
and R
5
, and R
5
and R
6
may be bonded to each other to form a ring; X
1
and X
2
each independently represent a hydrogen atom, a halogen ato
Kanzawa Mitsugu
Machida Shuji
Cheung William
Idemitsu Petrochemical Co. Ltd.
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