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Catalysts and polymerization processes wherein these catalysts are used

Assignee: ExxonMobil Chemical Patents Inc
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Filing: 1988-01-27
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Granted: —
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Expires: 2008-01-27
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Abstract

Abstract A catalyst is prepared by combining a bis(cyclopentadienyl)zirconium compound which may be represented by one of the following general formulae: (A-Cp)MX 1 X2; (A-Cp)MX' 1 X' 2 ; (A-Cp)ML; and (Cp*)(CpR)MX 1 Wherein: M is a metal selected from the Group consisting of titanium (Ti), zirconium (Zr) and hafnium (Hf); (A-Cp) is either (Cp)(Cp * ) or Cp-A'-Cp * and Cp and Cp * are the same or different substituted or unsubstituted cyclopentadienyl radicals; A' is a covalent bridging group containing a Group IV-A element; L is an olefin, diolefin or aryne ligand: X 1 and X 2 are, independently, selected from the Group consisting of hydride radicals, hydrocarbyl radicals, substituted-hydrocarbyl radicals, organo-metalloid radicals and the like; X' 1 and X' 2 are joined and bound to the metal atom to form a metallacycle, in which the metal, X' 1 and X' 2 form a hydrocarbocyclic ring having from about 3 to about 20 carbon atoms; and R is a substituent on one of the cyclopentadienyl radicals which is also bound to the metal atom. With a second compound comprising a cation capable of donating a proton add a bulky, labile anion comprising a plurality of boron atoms capable of stabilizing the zirconium cation formally having a coordination number of 3 and a valence of +4 which is formed as a result of the combination, said second compound having one of the following general formulae: Wherein: L'-H is either H , ammonium or a substituted-ammonium radical having up to 3 hydrogen atoms replaced with a hydrocabyl or substituted-hydrocarbyl radical, a phosphonium or substituted-phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical and the like; B and C are, respectively, boron and carbon; X, X' and X" are radicals selected, independently, from the Group consisting of hydride radicals, halide radicals, hydrocarbyl or substituted-hydrocarbyl radicals, organo-metalloid radicals and the like; a and b are integers ≧ 0; c is an integer ≧ 1; a + b + c = an even-numbered integer from 2 to about 8; and m is an integer ranging from 5 to about 22. Wherein: L'-H is either H , ammonium or a substituted-ammonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical, a phosphonium or substituted-phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical and the like; B, C, M and H are, respectively, boron, carbon, a transition metal and hydrogen; X 3 , X 4 and X 5 are radicals selected, independently, from the Group consisting of hydride radicals, halide radicals, hydrocarbyl or substituted-hydrocarbyl radicals, organo-metalloid radicals and the like; a' and b' are the same or a different integer ≧ 0; c' is an integer ≧ 2; a' + b' + c' = an even-numbered integer from 4 to about 8; m' is an integer from 6 to about 12; n is an integer such that 2c' - n = d; and d is an integer 1. Many of the catalysts thus formed are stable and isolable and may be recovered and stored. The catalysts may be preformed and then used to polymerize olefins or the catalysts may be formed in situ during polymerization by adding the separate components to the polymerization reaction. The catalyst will be formed when the two components are combined at a temperature within the range from about -100°C to about 300 °C. The catalysts thus prepared afford better control of polymer molecular weight and are not subject to equilibrium reversal. The catalysts thus produced are also less pyrophoric than the more conventional Ziegler-Natta olefin polymerization catalysts.

Inventors

  • 👤 Howard William Turner
  • 👤 Gregory George Hlatry

Bibliographic Details

Application Number —
Jurisdiction EP
Data Source google_patents
Last Synchronized 2026-10-31 23:23
CPC Classifications
C; C08; C08F; C08F10/00; C07; C07F; C07F17/00; C08F4/00; C08F4/42; C08F4/44; C08F4/60; C08F4/62; C08F4/64; C08F4/659; C08F4/65908; C08F4/6592; C08F4/65922; Y; Y10; Y10S; Y10S526/00; Y10S526/943

Claims Analysis

Total Claims: 20
Claim 1
Independent Claim 91 words
An ionic polymerisation catalyst for olefin polymerisation including a cation having a coordination number of 3 and a valence of +4, derived from a hydrolysable, bis(cyclopentadienyl) compound of a metal of Group IVB of the Periodic Table of Elements or a catalytically active decomposition product thereof and a stabilising anion comprising a purality of boron atoms which does not transfer an anionic substituent or fragment to the cation to form a neutral four coordinate metallocene and sufficiently labile to permit displacement by an olefin and/or diolefin and/or unsaturated monomer during polymerisation.
Claim 2
Dependent Claim 91 words
An ionic polymerisation catalyst for olefin polymerisation including a cation having a coordination number of 3 and a valence of +4, derived from a hydrolysable, bis(cyclopentadienyl) compound of a metal of Group IVB of the Periodic Table of Elements or a catalytically active decomposition product thereof and a stabilising anion comprising a purality of boron atoms which does not transfer an anionic substituent or fragment to the cation to form a neutral four coordinate metallocene and sufficiently labile to permit displacement by an olefin and/or diolefin and/or unsaturated monomer during polymerisation.
Claim 3
Dependent Claim 181 words
Catalyst according to Claim 1 wherein said cation is derived from a compound represented by the following general formulae : or Wherein : M is a metal selected from the group consisting of titanium (Ti), zirconium (Zr) and hafnium (Hf) ; (A-Cp) is either (Cp)(Cp * ) or Cp-A'-Cp * and Cp and Cp * are the same or different substituted or unsubstituted cyclopentadienyl radicals, optionally two independently substituted or unsubstituted radicals ; A' is a covalent bridging group containing a Group IV-A element ; L is an olefin, diolefin or aryne ligand ; X 1 and X 2 are, independently, selected from the group consisting of hydride radicals, hydrocarbyl radicals, substituted-hydrocarbyl radicals, optionally two lower alkyl substituents or two hydrides or organo-metalloid radicals ; X'i and X 2 are joined and bound to the metal atom to form a metallacycle, in which the metal, X' i and X 2 form a hydrocarbocyclic ring containing from 3 to 20 carbon atoms ; and R is a substituent on one of the cyclopentadienyl radicals which is also bound to the metal atom.
Claim 4
Dependent Claim 26 words
Catalyst according to Claim 1 or Claim 2 wherein said stabilising anion is derived from a compound represented by one of the following general formulae :
Claim 5
Dependent Claim 124 words
Wherein : L'-H is either H+, ammonium or a substitued ammonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical, a phosphonium or substituted or substituted-phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical and the like ; B and C are, respectively, boron and carbon ; X, X' and X" are radicals selected, independently, from the group consisting of hydride radicals, halide radicals, hydrocarbyl radicals or organo-metalloid radicals ; a and b are integers ≧ 0 ; c is an integer ≧ 1 ; a + b + c = an even-numbered integer from 2 to 8 ; and m is an integer ranging from 5 to 22 to 22 ; and/or
Claim 6
Dependent Claim 124 words
Wherein : L'-H is either H+, ammonium or a substitued ammonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical, a phosphonium or substituted or substituted-phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical and the like ; B and C are, respectively, boron and carbon ; X, X' and X" are radicals selected, independently, from the group consisting of hydride radicals, halide radicals, hydrocarbyl radicals or organo-metalloid radicals ; a and b are integers ≧ 0 ; c is an integer ≧ 1 ; a + b + c = an even-numbered integer from 2 to 8 ; and m is an integer ranging from 5 to 22 to 22 ; and/or
Claim 7
Dependent Claim 143 words
Wherein : L'-H is either H+, ammonium or a substituted-ammonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical, a phosphonium or substituted-phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical ; B, C, M and H are, respectively, boron, carbon, a transition metal and hydrogen ; X 3 , X 4 and X 5 are radicals selected, independently, from the group consisting of hydride radicals, halide radicals, hydrocarbyl radicals or organo-metalloid radicals ; a' and b' are the same or a different integer ≧ 0 ; c' is an integer ≧ 2 ; a + b' + c' = an even-numbered integer from 4 to 8; m' is an integer from 6 to 12 ; n is an integer such that 2c'-n = d ; and d is an integer 1.
Claim 8
Dependent Claim 143 words
Wherein : L'-H is either H+, ammonium or a substituted-ammonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical, a phosphonium or substituted-phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical ; B, C, M and H are, respectively, boron, carbon, a transition metal and hydrogen ; X 3 , X 4 and X 5 are radicals selected, independently, from the group consisting of hydride radicals, halide radicals, hydrocarbyl radicals or organo-metalloid radicals ; a' and b' are the same or a different integer ≧ 0 ; c' is an integer ≧ 2 ; a + b' + c' = an even-numbered integer from 4 to 8; m' is an integer from 6 to 12 ; n is an integer such that 2c'-n = d ; and d is an integer 1.
Claim 9
Dependent Claim 23 words
Catalyst according to any of the preceding claims wherein said stabilising anion is derived from a compound represented by the general formula :
Claim 10
Dependent Claim 85 words
Wherein : L'-H is either H+, ammonium or a substituted-ammonium optionally tri-substituted radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical, a phosphonium or substituted-phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical ; B, C and H are, respectively, boron, carbon and hydrogen ; ax is either 0 or 1 ; cx is either 2 or 1 ; ax + cx = 2; and bx is an integer ranging from 10 to 12.
Claim 11
Dependent Claim 85 words
Wherein : L'-H is either H+, ammonium or a substituted-ammonium optionally tri-substituted radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical, a phosphonium or substituted-phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical ; B, C and H are, respectively, boron, carbon and hydrogen ; ax is either 0 or 1 ; cx is either 2 or 1 ; ax + cx = 2; and bx is an integer ranging from 10 to 12.
Claim 12
Dependent Claim 46 words
Catalyst according to Claim 5 wherein said stabilising anion is derived from a compound selected from the group consisting of bis[tri(n-butyl)ammonium]dodecaborate and tri(n-butyl)ammonium 1-carbaun- deca or 1-carbadodecaborate and said first cation is derived from the group consisting of bis-(pentamethylcyclopentadienyl)zirconium dimethyl, (pentamethylcyclopentadienyl) (cyclopentadienyl)-zirconium dimethyl, and [1,3-bis(trimethylsilyl)cyclopentadienyl]zirconium dimethyl.
Claim 13
Dependent Claim 123 words
Catalyst according to any of the preceding claims wherein stabilising anion is derived from a compound represented by the following general formula : Wherein : L'-H is either H +, ammonium or a substituted-ammonium, optionally tri-substituted, radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical, a phosphonium or substituted-phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted-hydrocarbyl radical ; B, C and H are, respectively, boron, carbon and hydrogen ; ay is an integer from 0 to 2 ; by is an integer from 0 to 3 ; cy is an integer from 0 to 3 ; ay + by + cy = 4 and mx is an integer from 9 to 18.
Claim 14
Dependent Claim 65 words
Catalyst according to Claim 6 wherein said stabilising anion is derived from a compound selected from the group consisting of tri(n-butyl)ammonium 7,8-dicarbaundecaborate and tri(n-butyl)ammonium tridecahydrido-7-carbaundecaborate in which case preferably the cation is derived from bis-(pentamethylcyclopentadienyl)zirconium dimethyl and/or wherein L'-H is H+, preferably 7,8-dicarbaundecaborane (13) or octadecaborane (22) in which case optionally said cation is derived from the group consisting of bis(pentamethylcyclopentadienyl)zirconium dimethyl and bis-(ethyltetramethylcyclopentadienyl)zirconium dimethyl.
Claim 15
Dependent Claim 140 words
Catalyst according to any of the preceding claims wherein said stabilising anion is derived from a compound represented by the following general formula : Wherein : L'-H is either H+, ammonium or a substituted ammonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted hydrocarbyl radical, a phosphonium or substituted phosphonium radical having up to 3 hydrogen atoms replaced with a hydrocarbyl or substituted hydrocarbyl radical ; B, C, H and MZ are, respectively, boron, carbon, hydrogen and a transition metal ; az is an integer from 0 to 2 ; bz is an integer from 0 to 2 ; cz is either 2 or 3; mz is an integer from 9 to 11 ; az + bz + cz = 4 ; and nz and dz are, respectively, 2 & 2 or 3 & 1.
Claim 16
Dependent Claim 72 words
Catalyst according to Claim 8 wherein said stabilising anion is derived from N,N-dimethylanilinium bis-(undecahydrido-7,8-dicarbaundecaborato) cobaltate(III) and/or wherein said cation is derived from the group consisting of 1-bis(cyclopentadienyl)titana-3-dimethylsilacyclobutane, 1-bis(cyclopentadienyl)-zircona-3-dimethyl-silacyclobutane,and 1-bis(cyclopentadienyl)hafna-3-dimethylsilacyclobutane, bis-(cyclopentadienyl) zirconium (2,3-dimethyl-1,3-butadiene) and bis(cyclopentadienyl) hafnium(2,3-dimethyl-1,3-butadiene), (pentamethylcyclopentadienyl) (tetramethylcyclopentadienyl-methylene)-zirconium phenyl and (pentamethylcyclopentadienyl) (tetramethylcyclopentadienylmethylene) hafnium benzyl ; or said cation is derived from the group consisting of N,N-dimethylanilinium bis (7,8-dicarbaundecaborato)nickelate(ill) and N,N-dimethylanilinium bis(7,8-dicarbaundecaborato) ferrate(III) in which case preferably said cation is derived from bis(pentamethyl-cyclopentadienyl)zirconium dimethyl.
Claim 17
Dependent Claim 277 words
Composition of matter containing compounds represented by the following general formula : Wherein : M is a metal selected from the group consisting of titanium (Ti), zirconium (Zr) and hafnium (Hf) ; (A-Cp) is either (Cp)(Cp * ) or Cp-A'-Cp * and Cp and Cp * are the same or different substituted or unsubstituted cyclopentadienyl radicals ; A' is a covalent bridging group containing a Group IV-A element ; X 1 is selected from the group consisting of hydride radicals, hydrocarbyl radicals, organo-metalloid radicals ; and B' is a compatible non-coordinating anion which may be represented by one of the following general formulae : Wherein : B and C are, respectively, boron and carbon ; X, X' and X" are radicals selected, independently, from the group consisting of hydride radicals, halide radicals, hydrocarbyl radicals or organo-metalloid radicals, a and b are integers ≧ 0 ; c is an integer ≧ 1 ; a + b + c = an even-numbered integer from 2 to 8 ; and m is an integer ranging from 5 to 22 ; and 34 Wherein : B, C and M are, respectively, boron, carbon and a transition metal ; X 3 , X 4 and X 5 are radicals selected, independently, from the group consisting of hydride radicals, halide radicals, hydrocarbyl radicals, organo-metalloid radicals ; a' and b' are the same or a different integer ≧ 0 ; c' is an integer 2 ; a + b' + c' = an even-numbered integer from 4 to 8 ; m' is an integer from 6 to 12; n is an integer such that 2c'-n = d ; and d is an integer 1.
Claim 18
Dependent Claim 277 words
Composition of matter containing compounds represented by the following general formula : Wherein : M is a metal selected from the group consisting of titanium (Ti), zirconium (Zr) and hafnium (Hf) ; (A-Cp) is either (Cp)(Cp * ) or Cp-A'-Cp * and Cp and Cp * are the same or different substituted or unsubstituted cyclopentadienyl radicals ; A' is a covalent bridging group containing a Group IV-A element ; X 1 is selected from the group consisting of hydride radicals, hydrocarbyl radicals, organo-metalloid radicals ; and B' is a compatible non-coordinating anion which may be represented by one of the following general formulae : Wherein : B and C are, respectively, boron and carbon ; X, X' and X" are radicals selected, independently, from the group consisting of hydride radicals, halide radicals, hydrocarbyl radicals or organo-metalloid radicals, a and b are integers ≧ 0 ; c is an integer ≧ 1 ; a + b + c = an even-numbered integer from 2 to 8 ; and m is an integer ranging from 5 to 22 ; and 34 Wherein : B, C and M are, respectively, boron, carbon and a transition metal ; X 3 , X 4 and X 5 are radicals selected, independently, from the group consisting of hydride radicals, halide radicals, hydrocarbyl radicals, organo-metalloid radicals ; a' and b' are the same or a different integer ≧ 0 ; c' is an integer 2 ; a + b' + c' = an even-numbered integer from 4 to 8 ; m' is an integer from 6 to 12; n is an integer such that 2c'-n = d ; and d is an integer 1.
Claim 19
Dependent Claim 76 words
Composition of matter according to Claim 10 wherein (A-Cp) is a bis(peralkyl-substituted cyclopentadienyl) ; X is an alkyl group ; B' is (dodecahydrido-7,8-dicarbaundecaborato) and M is zirconium and wherein each of the alkyl groups in the peralkyl-substituted cyclopentadienyl radicals are, independently, C 1 -C 20 alkyl radicals and the alkyl group is a C 1 -C 20 alkyl radical, the peralkyl substitution being preferably pentamethyl or ethyltetramethyl and the alkyl radical being preferably a methyl radical.
Claim 20
Dependent Claim 137 words
Process for polymerizing an alpha-olefin, a diolefin and/or an acetylenically unsaturated compound containing from 2 to 18 carbon atoms either alone or in combination with one or more other monomers comprising the steps of: (a) contacting at a temperature within the range from -100°C to 300 °C and at a pressure within the range from 0 to 3500 Bar (45,000 psig.) an olefin, diolefin and/or an acetylenically unsaturated monomer either alone or in combination with one or more other monomers in a suitable carrier, solvent or diluent with a catalyst or composition of matter according to any of the preceding claims prepared previously or in situ during polymlerization ; (b) continuing the contacting of step (a) for a sufficient period of time to polymerize at least a portion of said olefin ; (c) recovering a polymer product.

References Cited (Backward Citations)

US3231593A Cited
EP0200351A2 Cited

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