DE774468T1 - Additionspolymerisationskatalysator mit eingeschränkter Geometrie, Verfahren zur Herstellung davon, Vorläufer dafür, Verfahren zur Verwendung und daraus hergestellte Polymere - Google Patents

Additionspolymerisationskatalysator mit eingeschränkter Geometrie, Verfahren zur Herstellung davon, Vorläufer dafür, Verfahren zur Verwendung und daraus hergestellte Polymere

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DE774468T1
DE774468T1 DE0774468T DE96119530T DE774468T1 DE 774468 T1 DE774468 T1 DE 774468T1 DE 0774468 T DE0774468 T DE 0774468T DE 96119530 T DE96119530 T DE 96119530T DE 774468 T1 DE774468 T1 DE 774468T1
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coordination complex
metal coordination
catalyst
alkyl
metal
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DE19619530A1 (de
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George W. Lake Jackson Texas 77566 Knight
Shih-Yaw Sugar Land Texas 77479 Lai
Peter N. Midland Michigan 48640 Nickias
Robert K. Sugar Land Texas 77479 Rosen
Gregory F. Kennett Square Penn. 19348 Schmidt
James C. Richmond Texas 77469 Stevens
Francis J. Midland Michigan 48640 Timmers
David R. Midland Michigan 48640 Wilson
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Dow Chemical Co
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Dow Chemical Co
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Claims (44)

5373EPDE /SF/Fl/us, The Dow Chemical Company ANSPRÜCHE
1. Metallmonocyclopentadienyl-Koordinationskomplex entsprechend der
Formel I:
5
worin:
M Hafnium, Zirkon oder Titan ist,
Cp* eine Cyclopentadienyl- oder substituierte Cyclopenta dienylgruppe ist, die an M über eine &eegr;5-Bindung gebunden ist,
X bei jedem Auftreten eine anionische Ligandengruppe oder neutrale Lewis-Base Ligandengruppe mit bis zu 30 Nichtwasserstoffatomen ist,
n in Abhängigkeit der Valenz von M 1, 2, 3 oder 4 ist und
Y ein neutraler Zwei-Elektronen-Donorligand ausgewählt aus OR*, SR*. NR*2 und PR*2 ist,
Z SiR*2, CR*2, SiR*2SiR*2, CR*2CR*2, CR*= CR*. CR*2SiR*2, GeR*2, BR* oder BR*2 ist und
R* bei jedem Auftreten Wasserstoff oder eine Einheit ausgewählt aus Alkyl-, Aryl-, SiIyI -, halogenierten Alkyl-, halogenieren Aryl gruppen und Kombinationen daraus mit bis zu 20 Nichtwasserstoff atomen ist oder zwei oder mehr R*-Gruppen von Z oder sowohl von Y und Z ein kondensiertes Ringsystem bilden.
2. [Verfahren] Metall koordinationskomplex wie in Anspruch 1 beansprucht, worin M Titan ist.
3. Metall koordinationskomplex wie in Anspruch 1 beansprucht, worin die substituierte Cyclopentadienylgruppe Cyclopentadienyl ist, das mit einem oder mehreren C1- bis C20 - Kohl enwasserstoff-, C1- bis
5373EPDE /SF/Fl/us, The Dow Chemical Company
C20-Halogenkohlenwasserstoffresten, Halogen oder C1- bis C20-halogensubstituierten Resten von Gruppe-14-Metalloiden substituiert ist oder Indenyl, Tetrahydroindenyl, Fluorenyl oder Octahydrof1uorenyl ist.
4. Metall koordinationskomplex wie in einem der vorstehenden Ansprüche beansprucht, worin jedes X ausgewählt ist aus Hydrid, Halogen, Alkyl, Si IyI, Germyl, Aryl, Amid, Aryloxy, Alkoxy, SiI oxy, Phosphid, Sulfid, Acyl, Cyanid, Azid, Acetylacetonat und Kombinationen davon.
5. Metall koordinationskomplex wie in Anspruch 1 beansprucht, entsprechend der Formel II:
(ID
worin:
R' bei jedem Auftreten Wasserstoff oder eine Einheit
ausgewählt aus Alkyl, Aryl, SiIyI, Germyl, Cyano, Halogen oder Kombinationen davon mit bis zu 20 Nichtwasserstoffatomen ist oder ein benachbartes Paar von R1-Gruppen einen Kohlenwasserstoffring bilden, der an die Cyclopentadienyleinheit anelliert ist,
X bei jedem Auftreten Hydrid ist oder eine Einheit ist, die
ausgewählt ist aus Halogen, Alkyl, SiIyI, Germyl, Aryl, Amid, Aryloxy, Alkoxy, SiIoxy und Kombinationen daraus mit bis zu 20 Nichtwasserstoffatomen und neutralen Lewis-Base-Liganden mit bis zu 20 Nichtwasserstoffatomen und
M, n, Y und Z wie in Anspruch 1 definiert sind.
5373EPDE /SF/Fl/us, The Dow Chemical Company
••&idigr;&iacgr;&Egr;-y &iacgr;'&Rgr;'&Bgr; TX'46 8T1
6. Metall koordinationskomplex wie in Anspruch 5 beansprucht, worin M Titan ist.
7. MetalIkoordinationskomplex wie in Anspruch 1 oder 5 beansprucht, worin Y gleich NR*2 ist.
8. MetalIkoordinationskomplex wie in Anspruch 1 oder 5 beansprucht, worin Y gleich OR* ist.
9. MetalIkoordinationskompl ex wie in Anspruch 5 beansprucht, worin R' bei jedem Auftreten Wasserstoff oder ein Alkyl rest ist oder R' an der Cyclopentadienyleinheit einen Kohlenwasserstoffring bildet, der an die Cyclopentadienyleinheit anelliert it.
10. MetalIkoordinationskomplex wie in Anspruch 1 oder 5 beansprucht, worin X Alkyl ist.
11. MetalIkoordinationskomplex wie in Anspruch 1 oder 5 beansprucht, worin X Halogen ist.
12. MetalIkoordinationskomplex wie in Anspruch 1 oder 5 beansprucht, worin X Aralkyl ist.
13. MetalIkoordinationskomplex wie in Anspruch 1 oder 5 beansprucht, worin Z SiR*2 ist.
14. MetalIkoordinationskomplex wie in Anspruch 1 oder 5 beansprucht, worin &eegr; gleich 1 ist.
15. Metall koordinationskomplex wie in Anspruch 1 oder 5 beansprucht, worin &eegr; gleich 2 ist.
5373EPDE /SF/Fl/us, The Dow Chemical Company &eegr;&udigr;\&Ggr; j C.P.»Q 7"*I.4*.468Tt
16. Metallkoordinationskomplex wie in Anspruch 1 oder 5 beansprucht, worin &eegr; gleich 3 ist.
17. Metallkoordinationskompl ex wie in Anspruch 1 oder 5 beansprucht, worin R* Wasserstoff oder Alkyl ist.
18. (Tetramethyl -r|5-cyclopentadienyl) -dimethyl (1-methylethoxy) si 1 antitan-trichlorid.
19. Katalysator, der bei Additionspolymerisation verwendet werden kann, enthaltend
a) einen Metallkoordinationskompl ex wie in einem der Ansprüche 1 bis 18 beansprucht und
b) einen aktivierenden Cokatalysator.
20. Katalysator wie in Anspruch 19 beansprucht, worin der aktivierende Cokatalysator eine Aluminiumverbindung enthält.
21. Katalysator wie in Anspruch 19 beansprucht, worin die Alumini umverbindung ein Alkyl aluminoxan ist.
22. Katalysator wie in Anspruch 19 beansprucht, worin die Aluminiumverbindung kein Alkyl aluminoxan ist.
23. Katalysator wie in Anspruch 20 beansprucht, worin die Aluminiumverbindung ein Alkylaluminoxan, Aluminiumalkyl, Aluminiumhalogenid oder Aluminiumalkylhalogenid ist.
24. Katalysator wie in Anspruch 19 beansprucht, worin der aktivierende Cokatalysator aus Verbindungen ausgewählt ist, die der Formel
5373EPDE /SF/Fl/us, The Dow Chemical Company
entsprechen, worin:
R bei jedem Auftreten ein C1- bis C10 -Alkyl- oder Aralkylrest ist,
X" Halogen ist und
&eegr; gleich 1, 2 oder 3 ist.
25. Katalysator wie in Anspruch 19 beansprucht, worin der aktivierende Cokatalysator eine Lewis-Säure, ein Ammoniumsalz oder ein nichtwechselwirkendes Oxidationsmittel enthält, unter der Voraussetzung, daß der Katalysator nicht der Formel B
CpMXn +A"
15
entspricht, worin
Cp* eine einzelne r|5-Cyclopentadienyl- oder substituierte &eegr;5-Cyclopentadienylgruppe ist, die fakultativ kovalent über einen Substituenten an M gebunden ist,
M Hafnium, Titan oder Zirkonium ist und über eine r|5-Bindung an die &eegr;5-Cyclopentadienyl - oder substituierte r|5-Cyclopentadienylgruppe gebunden ist,
X unabhängig bei jedem Auftreten Halogen, Alkyl, Aryl, -NR2, Aryloxy oder Alkoxy mit bis zu 20 Kohlenstoffatomen ist, oder zwei oder mehr X-Gruppen zusammen einen Metal 1ocyclus mit M bilden,
R Alkyl oder Aryl mit bis zu 10 Kohlenstoffatomen ist,
n in Abhängigkeit der Valenz von M gleich 1 oder 2 ist und
A~ ein nichtkoordinierendes kompatibles Anion eines Bronsted-Säure-Salzes ist.
30
26. Verfahren zur Herstellung eines Metall koordinationskomplexes wie in Anspruch 1 beansprucht, umfassend Inberührungbringen einer
5373EPDE /SF/Fl/us, The Dow Chemical Company ..&Pgr; &Ggr; / «jr. &Bgr;·. &Pgr; ,^.l't / &bgr; Q Tl
: _____ — — ^^"&iacgr; »' a as« &agr;&lgr;&lgr; ^^ · "
Metall verbindung der Formel MXn+2 oder einem koordinierten Addukt davon mit einer dianionischen Salzverbindung entsprechend der Formel
(L+x)y(CP*-Z-Y)·2 oder (LX")+x)y(CP*-Z-Y)·2,
worin:
n, CP*. M, X, Y und Z wie in Anspruch 1 definiert sind,
L ein Metall der Gruppe 1 oder 2 des Periodischen Systems der Elemente ist,
&khgr; und y entweder 1 oder 2 sind und das Produkt von &khgr; und y 2 entspricht und
X" Fluor, Brom, Chlor oder Iod ist,
in einem inerten Lösungsmittel.
15
27. Verfahren zur Herstellung eines Metallkoordinationskompl exes wie in Anspruch 1 beansprucht, umfassend
(a) Inberührungbringen einer Metall verbindung der Formel MXn+1 oder eines koordinierten Addukts davon mit einer dianionischen Salzverbindung entsprechend der Formel
(L+x)y(CP*-Z-Y)"2 oder (LX")+x)y(CP*-Z-Y)-2,
worin:
n, CP*. M, X, Y und Z wie in Anspruch 1 definiert sind,
L ein Metall der Gruppe 1 oder 2 des Periodischen Systems der Elemente ist,
&khgr; und y entweder 1 oder 2 sind und das Produkt von &khgr; und y 2 entspricht und
X" Fluor, Brom, Chlor oder Iod ist,
in einem inerten Lösungsmittel und
5373EPDE /SF/Fl/us, The Dow Chemical Company
1EiBB-Q^ZiO 6 8 &Pgr;
(b) Inberührungbringen des Produkts von (a) mit einem nichtwechselwirkenden Oxidationsmittel, um die Oxidationsstufe des Metalls zu erhöhen.
28. Verfahren wie in Anspruch 26 oder Anspruch 27 beansprucht, worin das Lösungsmittel aus Cyclohexan, Tetrahydrofuran, Methylcycl&ogr;-hexan, Pentan, Hexan, Heptan, Benzol, Toluol, Xylol und Ethylbenzol ausgewählt ist.
29. Verfahren wie in Anspruch 28 beansprucht, worin das Lösungsmittel Toluol oder Tetrahydrofuran ist.
30. Verfahren zur Herstellung eines Katalysators wie in Anspruch 19 beansprucht, umfassend Inberührungbringen eines Komplexes wie in einem der Ansprüche 1 bis 18 definiert mit einem aktivierenden Cokatalysator.
31. Verfahren zur Herstellung eines Katalysators wie in Anspruch 30 beansprucht, worin der aktivierende Cokatalysator wie in einem der
20 Ansprüche 20 bis 25 definiert ist.
32. Additionspolymerisationsverfahren zur Herstellung eines Polymers durch Inberührungbringen eines oder mehrerer additionspolymerisierbarer Monomere mit einem Katalysator unter Additionspolymerisationsbedingungen, dadurch gekennzeichnet, daß der Katalysator wie in einem der Ansprüche 19 bis 25 definiert ist.
33. Verfahren wie in Anspruch 32 beansprucht, worin die additionspolymerisierbaren Monomere aus ethylenisch ungesättigten Monomeren, acetylenisehen Verbindungen, konjugierten oder nichtkonjugierten Dienen und Polyenen mit 2 bis 20 Kohlenstoffatomen ausgewählt sind.
5373EPDE /SF/Fl/us, The Dow Chemical Company
«JVC" &igr; F» TV« &Lgr; *&PSgr;&EEgr; ·» I es &Lgr; f
! «&Igr;&mgr; fjPA 3#.4j 4 6 8 T
34. Verfahren wie in Anspruch 33 beansprucht, worin ein &agr;-Olefin mit einem aromatischen Vinylidenmonomer oder einem gehinderten aliphatischen Vinyl monomer copolymerisiert wird.
35. Verfahren wie in Anspruch 34 beansprucht, worin ein Ethylen mit Styrol oder Vinylcyclohexen copolymerisiert wird.
36. Verfahren zur Herstellung eines Copolymers aus einem gehinderten aliphatischen Vinylidenmonomer und einem a-01efin, worin das gehinderte aliphatische Vinylidenmonomer mit dem &agr;-Olefin unter Polyerisationsbedingungen in Gegenwart eines Katalysators in Berührung gebracht wird, der
a) einen Metall koordinationskomplex wie in einem der Ansprüche 1 bis 18 und
b) einen aktivierenden Cokatalysator
enthält.
37. Verfahren wie in Anspruch 36 beansprucht, worin der aktivierende Cokatalysator wie in einem der Ansprüche 20 bis 25 definiert ist.
38. Verfahren wie in Anspruch 36 oder 37 beansprucht, worin das gehinderte aliphatische Vinylidenmonomer eines ist, in dem die Kohlenstoffatome, die die ethylenisehe Unsättigung tragen, tertiär
25 oder quartär substituiert ist.
39. Verfahren wie in Anspruch 38 beansprucht, worin das Kohlenstoffatom mit einer cyclischen aliphatischen Gruppe substituiert ist.
40. Verfahren wie in Anspruch 39 beansprucht, worin das gehinderte aliphatische Vinylidenmonomer 1-, 3- oder 4-Vinylcyclohexen oder 5-Ethyliden-2-norbornen ist.
5373EPDE /SF/Fl/us, The Dow Chemical Company
41. Verfahren wie in einem der Ansprüche 32 bis 40 beansprucht, worin der Katalysator in situ gebildet wird.
42. Heterogener Katalysator auf einem Träger, der einen Metallkoordinationskompl ex entsprechend der Formel I wie in Anspruch 1 definiert und einen aktivierenden Cokatalysator enthält.
43. Heterogener Katalysator auf einem Träger wie in Anspruch 42 beansprucht, worin der Metallkoordinationskompl ex wie in einem der Ansprüche 2 bis 7 definiert ist.
44. Heterogener Katalysator auf einem Träger wie in Anspruch 43 beansprucht, worin der Träger aus Aluminiumoxid, MgCl2 und Siliciumdioxid ausgewählt ist.
DE0774468T 1989-08-31 1990-08-30 Additionspolymerisationskatalysator mit eingeschränkter Geometrie, Verfahren zur Herstellung davon, Vorläufer dafür, Verfahren zur Verwendung und daraus hergestellte Polymere Pending DE774468T1 (de)

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US42827689A 1989-10-27 1989-10-27
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