IP Library Granted Patent US 8,309,779
Granted Patent B2
US 8,309,779 · App. 12/733,156 · Granted Nov 13, 2012

Ethylene oligomerization catalyst systems having enhanced selectivity

View Patent ↗
Loading inventors, assignments & file history…
Monitor This Case
Get email alerts when status or documents change.
Order Certified Copies
Most orders are placed with the USPTO same day — all within 24 business hours.
Order via The Patent Place →
Pre-filled with this patent's details
Quick Facts
Patent No.
US 8,309,779
App. No.
12/733,156
Granted
Nov 13, 2012
Kind
B2
Abstract

Disclosed herein is a catalyst system for selective oligomerization of ethylene, which comprises a P—C—C—P frame-work ligand, which is (R 1 )(R 2 )P—(R 5 )CHCH(R 6 )—P(R 3 )(R 4 ), and a chromium-based metal compound. Also disclosed is a method of greatly enhancing the activity and selectivity of oligomerization, such as trimerization or tetramerization, using a ligand having a specific steric arrangement structure.

Claims (18)

1. A method of producing 1-hexene by selectively trimerizing ethylene using a catalyst system comprising a transition metal or transition metal precursor, a promoter and a ligand represented by any one of the following formulas 1 to 4, wherein the promoter is methylaluminoxane (MAO) or ethylaluminoxane (EAO) and the ligand is sterically asymmetric with respect to a plane of symmetry:

wherein R 1 , R 2 , R 3 and R 4 are each independently hydrocarbyl, substituted hydrocarbyl, heterohydrocarbyl or substituted heterohydrocarbyl, R 5 and R 6 are each independently hydrocarbyl or substituted hydrocarbyl, and A is hydrocarbylene, substituted hydrocarbylene, heterohydrocarbylene or substituted heterohydrocarbylene.

2. The method of claim 1 , wherein R 1 , R 2 , R 3 and R 4 in the ligand are each independently selected from the group consisting of phenyl, benzyl, naphthyl, anthracenyl, mesityl, xenyl, methyl, ethyl, ethylenyl, propyl, propenyl, propinyl, butyl, cyclohexyl, 4-methylcyclohexyl, 4-ethylcyclohexyl, 4-isopropylcyclohexyl, tolyl, xylyl, 4-methylphenyl, 4-ethylphenyl, 4-isopropylphenyl, 4-t-butylphenyl, 4-methoxyphenyl, 4-isopropoxyphenyl, cumyl, methoxy, ethoxy, phenoxy, tolyloxy, dimethylamino, thiomethyl, trimethylsilyl, dimethylhydrazine, 2-methylcyclohexyl, 2-ethylcyclohexyl, 2-isopropylcyclohexyl, o-methylphenyl, o-ethylphenyl, o-isopropylphenyl, o-t-butylphenyl, o-methoxyphenyl, and o-isopropoxyphenyl.

3. The method of claim 2 , wherein R1, R2, R3 and R4 in the ligand are each independently selected from the group consisting of phenyl, tolyl, xenyl, naphthyl, cyclohexyl, 4-methylphenyl, 4-ethylphenyl, 4-isopropylphenyl, 4-t-butylphenyl, 4-methoxyphenyl, 4-isopropoxyphenyl, 2-methylcyclohexyl, 2-ethylcyclohexyl, 2-isopropylcyclohexyl, o-methylphenyl, o-ethylphenyl, o-isopropylphenyl, o-t-butylphenyl, o-methoxyphenyl and o-isopropoxyphenyl.

4. The method of claim 1 , wherein R5 and R6 in the ligand are each independently selected from the group consisting of alkyl, substituted alkyl, aryl, substituted aryl, aryloxy, substituted aryloxy, alkoxycarbonyl, carbonyloxy, alkoxy, aminocarbonyl, carbonylamino, dialkylamino, silyl groups, derivatives thereof, and aryl substituted with one or more of these substituents.

5. The method of claim 1 , wherein A in the ligand is selected from the group consisting of alkylene, alkoxylene, alkoxycarbonylene, carbonyloxy, aminocarbonylene, carbonylamino, alkylamino, derivatives thereof, and alkylene substituted with one or more of these substituents.

6. The method of claim 1 , wherein the ligand is selected from the group consisting of (S,S)- or (R,R)-(phenyl) 2 P—CH(methyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(methyl)CH(methyl)-P(4-methoxyphenyl) 2 , (S,S)- or (R,R)-(4-methylphenyl) 2 P—CH(methyl)CH(methyl)-P(4-methylphenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(methyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(ethyl)CH(methyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(ethyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(ethyl)CH(ethyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(phenyl) 2 P—CH(ethyl)CH(ethyl)-P(phenyl) 2 , (S,S)- or (R,R)-(phenyl) 2 P—CH(isopropyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(isopropyl)CH(methyl)-P(4-methoxyphenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(isopropyl)CH(methyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(phenyl) 2 P—CH(n-propyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(n-propyl)CH(methyl)-P(4-methoxyphenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(n-propyl)CH(methyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(phenyl) 2 P—CH(isopropyl)CH(ethyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(isopropyl)CH(ethyl)-P(4-methoxyphenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(isopropyl)CH(ethyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-trans-1,2-di-(P(phenyl) 2 )cyclohexane, (S,S)- or (R,R)-trans-1,2-di-(P(4-methoxyphenyl) 2 )cyclohexane, (S,S)- or (R,R)-trans-1,2-di-(P(4-ethylphenyl) 2 )cyclohexane, (S,S)- or (R,R)-trans-1,2-di-(P(phenyl) 2 )cyclopentane, (S,S)- or (R,R)-trans-1,2-di-(P(4-methoxyphenyl) 2 )cyclopentane, (S,S)- or (R,R)-1,2-di-(P(4-ethylphenyl) 2 )cyclopentane, (S,S)- or (R,R)-3,4-di-(P(phenyl) 2 )pyrrole, (S,S)- or (R,R)-3,4-di-(P(4-methoxyphenyl) 2 )pyrrole, (S,S)- or (R,R)-trans-3,4-di-(P(4-ethylphenyl) 2 )pyrrole, (S,S)- or (R,R)-trans-3,4-di-(P(4-ethylphenyl) 2 )imidazole, (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(dimethylamine)CH(dimethylamine)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(3-methoxyphenyl) 2 P—CH(methyl)CH(methyl)-P(3-methoxyphenyl) 2 , ((S,S)- or (R,R)-4-dimethylaminephenyl) 2 P—CH(methyl)CH(methyl)P(4-dimethylaminephenyl) 2 , (S,S)- or (R,R)-(4-ethylcyclohexyl) 2 PCH(methyl)CH(methyl)P(4-ethylcyclohexyl) 2 , (S,S)- or (R,R)-trans-3,4-di-(P(2-ethylphenyl) 2 )pyrrole, (S,S)- or (R,R)-trans-3,4-di-(P(2-ethylphenyl) 2 )imidazole, (S,S)- or (R,R)-(phenyl) 2 P—CH(phenyl)CH(phenyl)-P(phenyl) 2 , (1S,2S)- or (1R,2R)-trans-bis(diphenylphosphino)cyclohexane, and (1S,2S)- or (1R,2R)-trans-bis(di(4-methoxyphenyl)phosphino)cyclohexane.

7. The method of claim 1 , wherein said transition metal or transition metal precursor is chromium or a chromium precursor.

8. The method of claim 7 , wherein said chromium or chromium precursor is selected form the group consisting of chromium (III) acetylacetonate, tris(tetrahydrofuran) trichlorochromium, and chromium (III) 2-ethylhexanoate.

9. A method of producing 1-octene by selectively tetramerizing ethylene using a catalyst system comprising a transition metal or transition metal precursor, a promoter and a ligand represented by any one of the following formulas 1 to 4, wherein the promoter is methylaluminoxane (MAO) or ethylaluminoxane (EAO) and the ligand is sterically asymmetric with respect to a plane of symmetry:

wherein R 1 , R 2 , R 3 and R 4 are each independently hydrocarbyl, substituted hydrocarbyl, heterohydrocarbyl or substituted heterohydrocarbyl, R 5 and R 6 are each independently hydrocarbyl or substituted hydrocarbyl, and A is hydrocarbylene, substituted hydrocarbylene, heterohydrocarbylene or substituted heterohydrocarbylene.

10. The method of claim 9 , wherein R1, R2, R3 and R4 in the ligand are each independently selected from the group consisting of phenyl, benzyl, naphthyl, anthracenyl, mesityl, xenyl, methyl, ethyl, ethylenyl, propyl, propenyl, propinyl, butyl, cyclohexyl, 4-methylcyclohexyl, 4-ethylcyclohexyl, 4-isopropylcyclohexyl, tolyl, xylyl, 4-methylphenyl, 4-ethylphenyl, 4-isopropylphenyl, 4-t-butylphenyl, 4-methoxyphenyl, 4-isopropoxyphenyl, cumyl, methoxy, ethoxy, phenoxy, tolyloxy, dimethylamino, thiomethyl, trimethylsilyl, dimethylhydrazine, 2-methylcyclohexyl, 2-ethylcyclohexyl, 2-isopropylcyclohexyl, o-methylphenyl, o-ethylphenyl, o-isopropylphenyl, o-t-butylphenyl, o-methoxyphenyl, and o-isopropoxyphenyl.

11. The method of claim 10 , wherein R1, R2, R3 and R4 in the ligand are each independently selected from the group consisting of phenyl, tolyl, xenyl, naphthyl, cyclohexyl, 4-methylphenyl, 4-ethylphenyl, 4-isopropylphenyl, 4-t-butylphenyl, 4-methoxyphenyl, 4-isopropoxyphenyl, 2-methylcyclohexyl, 2-ethylcyclohexyl, 2-isopropylcyclohexyl, o-methylphenyl, o-ethylphenyl, o-isopropylphenyl, o-t-butylphenyl, o-methoxyphenyl and o-isopropoxyphenyl.

12. The method of claim 9 , wherein R5 and R6 in the ligand are each independently selected from the group consisting of alkyl, substituted alkyl, aryl, substituted aryl, aryloxy, substituted aryloxy, alkoxycarbonyl, carbonyloxy, alkoxy, aminocarbonyl, carbonylamino, dialkylamino, silyl groups, derivatives thereof, and aryl substituted with one or more of these substituents.

13. The method of claim 9 , wherein A in the ligand is selected from the group consisting of alkylene, alkoxylene, alkoxycarbonylene, carbonyloxy, aminocarbonylene, carbonylamino, alkylamino, derivatives thereof, and alkylene substituted with one or more of these substituents.

14. The method of claim 9 , wherein the ligand is selected from the group consisting of (S,S)- or (R,R)-(phenyl) 2 P—CH(methyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(methyl)CH(methyl)-P(4-methoxyphenyl) 2 , (S,S)- or (R,R)-(4-methylphenyl) 2 P—CH(methyl)CH(methyl)-P(4-methylphenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(methyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(ethyl)CH(methyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(ethyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(ethyl)CH(ethyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(phenyl) 2 P—CH(ethyl)CH(ethyl)-P(phenyl) 2 , (S,S)- or (R,R)-(phenyl) 2 P—CH(isopropyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(isopropyl)CH(methyl)-P(4-methoxyphenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(isopropyl)CH(methyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(phenyl) 2 P—CH(n-propyl)CH(methyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(n-propyl)CH(methyl)-P(4-methoxyphenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(n-propyl)CH(methyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(phenyl) 2 P—CH(isopropyl)CH(ethyl)-P(phenyl) 2 , (S,S)- or (R,R)-(4-methoxyphenyl) 2 P—CH(isopropyl)CH(ethyl)-P(4-methoxyphenyl) 2 , (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(isopropyl)CH(ethyl)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-trans-1,2-di-(P(phenyl) 2 )cyclohexane, (S,S)- or (R,R)-trans-1,2-di-(P(4-methoxyphenyl) 2 )cyclohexane, (S,S)- or (R,R)-trans-1,2-di-(P(4-ethylphenyl) 2 )cyclohexane, (S,S)- or (R,R)-trans-1,2-di-(P(phenyl) 2 )cyclopentane, (S,S)- or (R,R)-trans-1,2-di-(P(4-methoxyphenyl) 2 )cyclopentane, (S,S)- or (R,R)-1,2-di-(P(4-ethylphenyl) 2 )cyclopentane, (S,S)- or (R,R)-3,4-di-(P(phenyl) 2 )pyrrole, (S,S)- or (R,R)-3,4-di-(P(4-methoxyphenyl) 2 )pyrrole, (S,S)- or (R,R)-trans-3,4-di-(P(4-ethylphenyl) 2 )pyrrole, (S,S)- or (R,R)-trans-3,4-di-(P(4-ethylphenyl) 2 )imidazole, (S,S)- or (R,R)-(4-ethylphenyl) 2 P—CH(dimethylamine)CH(dimethylamine)-P(4-ethylphenyl) 2 , (S,S)- or (R,R)-(3-methoxyphenyl) 2 P—CH(methyl)CH(methyl)-P(3-methoxyphenyl) 2 , ((S,S)- or (R,R)-4-dimethylaminephenyl) 2 P—CH(methyl)CH(methyl)P(4-dimethylaminephenyl) 2 , (S,S)- or (R,R)-(4-ethylcyclohexyl) 2 PCH(methyl)CH(methyl)P(4-ethylcyclohexyl) 2 , (S,S)- or (R,R)-trans-3,4-di-(P(2-ethylphenyl) 2 )pyrrole, (S,S)- or (R,R)-trans-3,4-di-(P(2-ethylphenyl) 2 )imidazole, (S,S)- or (R,R)-(phenyl) 2 P—CH(phenyl)CH(phenyl)-P(phenyl) 2 , (1S,2S)- or (1R,2R)-trans-bis(diphenylphosphino)cyclohexane, and (1S,2S)- or (1R,2R)-trans-bis(di(4-methoxyphenyl)phosphino)cyclohexane.

15. The method of claim 9 , wherein said transition metal or transition metal precursor is chromium or a chromium precursor.

16. The method of claim 15 , wherein said chromium or chromium precursor is selected form the group consisting of chromium (III) acetylacetonate, tris(tetrahydrofuran) trichlorochromium, and chromium (III) 2-ethylhexanoate.

Assignments (5)
CHANGE OF ADDRESS Recorded Sep 2, 2022
From: SK GLOBAL CHEMICAL CO., LTD
To: SK GLOBAL CHEMICAL CO., LTD
Reel/Frame 061371/0328 →
CHANGE OF NAME Recorded Sep 2, 2022
From: SK GLOBAL CHEMICAL CO., LTD
To: SK GEO CENTRIC CO., LTD.
Reel/Frame 061371/0332 →
CORRECTIVE ASSIGNMENT TO CORRECT THE INCORRECT PATENT NUMBER 7448700 AND REPLACE IT WITH 7488700 PREVIOUSLY RECORDED ON REEL 026619 FRAME 0330. ASSIGNOR(S) HEREBY CONFIRMS THE CHANGE OF NAME. Recorded Apr 11, 2016
From: SK ENERGY CO., LTD.
To: SK INNOVATION CO., LTD.
Reel/Frame 038406/0201 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jul 15, 2011
From: SK INNOVATION CO., LTD.
To: SK GLOBAL CHEMICAL CO., LTD.
Reel/Frame 026598/0963 →
CHANGE OF NAME Recorded Jul 14, 2011
From: SK ENERGY CO., LTD.
To: SK INNOVATION CO., LTD.
Reel/Frame 026619/0330 →