Transition metal complex, process for producing the same,...

Details Transition metal complex, process for producing the same,... Transition metal complex, process for producing the same,...

1999-04-30

2001-12-11

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...

C526S160000, C526S161000, C526S943000, C526S348600, C526S336000, C502S152000, C502S155000, C556S011000, C556S012000, C556S052000, C556S053000

Reexamination Certificate

active

06329478

ABSTRACT:

TECHNICAL FIELD
The present invention relates to a transition metal complex, a process for producing the same, a polymerization catalyst containing the transition metal complex and a process for producing polymers which uses the catalyst.
BACKGROUND ART
A number of reports have already been made on the process for producing olefin polymers using a metallocene complex. For example, JP-A-58-19309 discloses a process for producing olefin polymers which uses a metallocene complex and an aluminoxanone. The process has a problem in that when olefin is polymerized with the disclosed catalyst which uses bis(cyclopentadienyl)zirconium dichloride and methylaluminoxane, the molecular weight of the olefin polymer obtained is low. To improve this point, WO87/02370 discloses the use of a reaction product of an organic compound having at least two hydroxyl groups with a transition metal compound. However, the system disclosed in WO87/02370 which uses 2,2′-thiobis(6-tert-butyl-4-methylphenoxy)titanium dichloride and methylaluminoxane, and also a system disclosed in JP-A-5-230133 which uses 2,2′-thiobis(6-tert-butyl-4-methylphenoxy)titanium dichloride, triisobutylaluminum and triphenylmethyl tetrakis(pentafluorophenyl)borate involve a problem in that the catalytic activity is unsatisfactorily low from the industrial point of view although the molecular weight of the polymer produced is improved.
Moreover, known metallocene complexes, e.g., ethylenebis(indenyl)zirconium dichloride, isopropylidene(cyclopentadienyl) (fluorenyl)zirconium dichloride and dimethylsilyl(tert-butylamide)-(tetramethylcyclopentadienyl)titanium dichloride, have a problem in that they are insoluble in saturated hydrocarbon solvents although they are soluble in aromatic hydrocarbon solvents and resultantly polymerization catalysts containing such complexes cannot be used for producing polymers using saturated hydrocarbon solvents.
In recognition of the situation, the objects of the present invention are to provide a complex, important from the industrial viewpoint, which has a high activity at reaction temperatures efficient in the industrial process for olefin polymerization and is soluble in saturated hydrocarbon solvents, and to provide a highly active olefin polymerization catalyst containing the complex, and a process for producing olefin polymers which uses the catalyst.
DISCLOSURE OF THE INVENTION
The present inventors have made extensive study on transition metal complexes and olefin polymerization catalysts in order to attain the above-mentioned objects. As the result, the inventors have found a transition metal complex soluble in saturated hydrocarbon solvents which has a ligand comprising an aromatic ring having a hetero atom in the substituent and a cyclopentadienyl ring linked with each other through a covalent bonding group, and have accomplished the present invention on the basis of above finding.
Thus, according to the present invention, there are provided a transition metal complex represented by the formula (1) (hereinafter referred to as compound (1)) and a polymerization catalyst containing the complex:
wherein M
1
is a transition metal atom of the group 4 of the periodic table of elements, A is an atom of the group 16 of the periodic table of elements and B is an atom of the group 14 of the periodic table of elements; Cp
1
is a group having a cyclopentadiene type anionic skeleton; and X
1
, X
2
, R
1
, R
2
, R
3
, R
4
, R
5
and R
6
are each independently a hydrogen atom, halogen atom, alkyl group with the number of carbon atoms of 1-20 optionally substituted with at least one halogen atom, aralkyl group with the number of carbon atoms of 7-20 optionally substituted with at least one halogen atom, aryl group with the number of carbon atoms of 6-20 optionally substituted with at least one halogen atom, substituted silyl group with the number of carbon atoms of 1-20 optionally substituted with at least one halogen atom, alkoxy group with the number of carbon atoms of 1-20 optionally substituted with at least one halogen atom, aralkyloxy group with the number of carbon atoms of 7-20 optionally substituted with at least one halogen atom, aryloxy group with the number of carbon atoms of 6-20 optionally substituted with at least one halogen atom, or di-substituted amino group with the number of carbon atoms of 2-20; provided that R
1
, R
2
, R
3
, R
4
, R
5
and R
6
may optionally combine with each other to form a ring.
[Transition metal complex]
In the compound [1], the transition metal atom represented by M
1
refers to a transition metal atom of the group 4 of the periodic table of elements (Nomenclature of Inorganic Chemistry, IUPAC, revised ed., 1989) and may be, for example, a titanium atom, zirconium atom and hafnium atom.
The atom of the group 16 of the periodic table of elements represented by A may be, for example, an oxygen atom, sulfur atom and selenium atom, and is preferably an oxygen atom.
The atom of the group 14 of the periodic table of elements represented by B may be, for example, a carbon atom, silicon atom and germanium atom.
The group having a cyclopentadiene type anionic skeleton represented as the substituent Cp
1
may be, for example, the &eegr;
5
-cyclopentadienyl group, &eegr;
5
-methylcyclopentadienyl group, &eegr;
5
-dimethylcyclopentadienyl group, &eegr;
5
-trimethylcyclopentadienyl group, &eegr;
5
-tetramethylcyclopentadienyl group, &eegr;
5
-ethylcyclopentadienyl group, &eegr;
5
-n-propylcyclopentadienyl group, &eegr;
5
-isopropylcyclopentadienyl group, &eegr;
5
-n-butylcyclopentadienyl group, &eegr;
5
-sec-butylcyclopentadienyl group, &eegr;
5
-tert-butylcyclopentadienyl group, &eegr;
5
-n-pentylcyclopentadienyl group, &eegr;
5
-neopentylcyclopentadienyl group, &eegr;
5
-n-hexylcyclopentadienyl group, &eegr;
5
-n-octylcyclopentadienyl group, &eegr;
5
-phenylcyclopentadienyl group, &eegr;
5
-naphthylcyclopentadienyl group, &eegr;
5
-trimethylsilylcyclopentadienyl group, &eegr;
5
-triethylsilylcyclopentadienyl group, &eegr;
5
-tert-butyldimethylsilylcyclopentadienyl group, &eegr;
5
-indenyl group, &eegr;
5
-methylindenyl group, &eegr;
5
-dimethylindenyl group, &eegr;
5
-ethylindenyl group, &eegr;
5
-n-propylindenyl group, &eegr;
5
-isopropylindenyl group, &eegr;
5
-n-butylindenyl group, &eegr;
5
-sec-butylindenyl group, &eegr;
5
-tert-butylindenyl group, &eegr;
5
-n-pentylindenyl group, &eegr;
5
-neopentylindenyl group, &eegr;
5
-n-hexylindenyl group, &eegr;
5
-n-octylindenyl group, &eegr;
5
-n-decylindenyl group, &eegr;
5
-phenylindenyl group, &eegr;
5
-methylphenylindenyl group, &eegr;5-naphthylindenyl group, &eegr;
5
-trimethylsilylindenyl group, &eegr;
5
-triethylsilylindenyl group, &eegr;
5
-tert-butyldimethylsilylindenyl group, &eegr;
5
-tetrahydroindenyl group, &eegr;
5
-fluorenyl group, &eegr;
5
-methylfluorenyl group, &eegr;
5
-dimethylfluorenyl group, &eegr;
5
-ethylfluorenyl group, &eegr;
5
-diethylfluorenyl group, &eegr;
5
-n-propylfluorenyl group, &eegr;
5
-di-n-propylfluorenyl group, &eegr;
5
-isopropylfluorenyl group, &eegr;
5
-diisopropylfluorenyl group, &eegr;
5
-n-butylfluorenyl group, &eegr;
5
-sec-butylfluorenyl group, &eegr;
5
-tert-butylfluorenyl group, &eegr;
5
-di-n-butylfluorenyl group, &eegr;
5
-di-sec-butylfluorenyl group, &eegr;
5
-di-tert-butylfluorenyl group, &eegr;
5
-n-pentyfluorenyl group, &eegr;
5
-neopentylfluorenyl group, &eegr;
5
-n-hexylfluorenyl group, &eegr;
5
-n-octylfluorenyl group, &eegr;
5
-n-decylfluorenyl group, &eegr;
5
-n-dodecylfluorenyl group, &eegr;
5
-phenylfluorenyl group, &eegr;
5
-di-phenylfluorenyl group, &eegr;
5
-methylphenylfluorenyl group, &eegr;
5
-naphthylfluorenyl group, &eegr;
5
-trimethylsilylfluorenyl group, &eegr;
5
-bis-trimethylsilylfluorenyl group, &eegr;
5
-triethylsilylfluorenyl group and &eegr;
5
-tert-butyldimethylsilylfluorenyl group, preferred among them being, for example, the &eegr;
5
-cyclopentadienyl group, &eegr;
5
-methylcyclopentadienyl group, &eegr;
5
-tert-butylcyclopentadienyl group, &eegr;
5
-tetramethylcyclopentadienyl group, &eegr;
5
-indenyl group and &

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