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US4996363A Expired / Lapsed US ⏱️ 0.0 years remaining

Catalytic reforming of alkyleneamines to linearly-extended polyalkylenepolyamines

Assignee: Dow Chemical Co
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Filing: 1988-12-20
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Granted: 1991-02-26
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Expires: 2008-12-20
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Abstract

Abstract A process for reforming alkyleneamines to predominantly linearly-extended polyalkylenepolyamines comprising contacting an alkyleneamine or mixture thereof with a catalyst under conditions such that a mixture of polyalkylenepolyamines enriched in linearly-extended products is formed, said catalyst containing at least one compound selected from the group consisting of (a) Group VB metal oxides, (b) Group VB metal phosphates, (c) silicates of Groups IIA, IIIB, IVB, VB, and the lanthanide and actinide metals, and (d) tungsten oxides, with the proviso that the silicates and tungsten oxides are essentially free of aluminum. For example, ethylenediamine is contacted with a catalyst of niobium phosphate or niobic acid under reaction conditions to yield predominantly non-cyclic polyethylenepolyamines.

Inventors

  • 👤 Robert G. Bowman
  • 👤 David C. Molzahn
  • 👤 George E. Hartwell

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-11-08 17:52
CPC Classifications
C; C07; C07C; C07C209/00; C07C209/64

Claims Analysis

Total Claims: 25
Claim 1
Independent Claim 58 words
A process of reforming amines comprising contacting an alkyleneamine or mixture thereof with a catalytic amount of a catalyst consisting essentially of a Group IIA metal silicate, with the proviso that the silicate is essentially free of aluminum, the contacting occurring under reaction conditions such that a mixture of polyalkylenepolyamines is formed which is enriched in linearly-extended homologues.
Claim 2
Dependent Claim 58 words
A process of reforming amines comprising contacting an alkyleneamine or mixture thereof with a catalytic amount of a catalyst consisting essentially of a Group IIA metal silicate, with the proviso that the silicate is essentially free of aluminum, the contacting occurring under reaction conditions such that a mixture of polyalkylenepolyamines is formed which is enriched in linearly-extended homologues.
Claim 3
Dependent Claim 68 words
The process of claim 1 wherein the alkyleneamine is represented by the formula: ##STR3## wherein each B is independently NR or O; each R is independently hydrogen, amino, a C 1 -C 12 alkyl moiety or C 1 -C 12 aminoalkyl moiety, or a monocyclic aryl moiety; each x is independently an integer from 1 to about 12; and n is an integer from 0 to about 150.
Claim 4
Dependent Claim 15 words
The process of claim 2 wherein each B is NR and each R is hydrogen.
Claim 5
Dependent Claim 10 words
The process of claim 3 wherein the alkyleneamine is ethylenediamine.
Claim 6
Dependent Claim 10 words
The process of claim 3 wherein the alkyleneamine is diethylenetriamine.
Claim 7
Dependent Claim 11 words
The process of claim 1 wherein the catalyst is magnesium silicate.
Claim 8
Dependent Claim 32 words
The process of claim 1 wherein the quantity of catalyst is in the range from about 0.1 weight percent to about 20 weight percent based on the weight of the alkyleneamine reactant.
Claim 9
Dependent Claim 20 words
The process of claim 1 wherein the temperature is in the range from about 200° C. to about 400° C.
Claim 10
Dependent Claim 19 words
The process of claim 1 wherein the pressure is in the range from about atmospheric to about 4000 psig.
Claim 11
Dependent Claim 32 words
The process of claim 1 wherein the liquid hourly space velocity is in the range from about 0.1 g ml -1 hr -1 to about 10.0 g ml -1 hr -1 .
Claim 12
Dependent Claim 69 words
The process of claim 1 wherein the linearly-extended polyalkyleneopolyamines are represented by the formula: ##STR4## wherein each B is independently NR or O; each R is independently hydrogen, amino, a C 1 -C 12 alkyl moiety, a C 1 -C 12 aminoalkyl moiety, or a monocyclic aryl moiety; each x is independently an integer from 1 to about 12; and m is an integer from 1 to about 300.
Claim 13
Dependent Claim 24 words
The process of claim 11 wherein each R is hydrogen, each B is NR, x is 2, and m is 1, 2, or 3.
Claim 14
Dependent Claim 18 words
The process of claim 1 wherein the selectivity for linearly-extended polyalkylenepolyamines is at least about 45 weight percent.
Claim 15
Dependent Claim 18 words
The process of claim 13 wherein the selectivity for linearly-extended polyalkylenepolyamines is at least about 75 weight percent.
Claim 16
Dependent Claim 87 words
A process of preparing non-cyclic polyethylenepolyamines comprising contacting ethylenediamine, diethylenetriamine or mixtures thereof with a catalyst consisting essentially of magnesium silicate in a continuous flow reactor at a temperature in the range from about 250° C. to about 350° C., a pressure in the range from about 1000 psig to about 2000 psig, an a flow rate from about 0.5 g ml-1 hr-1 to about 5.0 g ml-1 hr-1 such that a mixture of linearly-extended polyethylenepolyamines is formed in a combined selectivity of about 75 weight percent.
Claim 17
Dependent Claim 87 words
A process of preparing non-cyclic polyethylenepolyamines comprising contacting ethylenediamine, diethylenetriamine or mixtures thereof with a catalyst consisting essentially of magnesium silicate in a continuous flow reactor at a temperature in the range from about 250° C. to about 350° C., a pressure in the range from about 1000 psig to about 2000 psig, an a flow rate from about 0.5 g ml-1 hr-1 to about 5.0 g ml-1 hr-1 such that a mixture of linearly-extended polyethylenepolyamines is formed in a combined selectivity of about 75 weight percent.
Claim 18
Dependent Claim 10 words
The process of claim 1 wherein a solvent is employed.
Claim 19
Dependent Claim 18 words
The process of claim 1 wherein the Group IIA silicate contains less than about 5 weight percent aluminum.
Claim 20
Dependent Claim 18 words
The process of claim 17 wherein the Group IIA silicate contains less than about 2 weight percent aluminum.
Claim 21
Dependent Claim 18 words
The process of claim 18 wherein the Group IIA silicate contains less than about 1 weight percent aluminum.
Claim 22
Dependent Claim 19 words
The process of claim 6 wherein the silicon to magnesium mole ratio varies from about 0.5 to about 20.
Claim 23
Dependent Claim 18 words
The process of claim 15 wherein the weight ratio of diethylenetriamine to piperazine is at least about 3/1.
Claim 24
Dependent Claim 21 words
The process of claim 15 wherein the weight percentage of triethylenetetramines which are non-cyclic is at least about 50 weight percent.
Claim 25
Dependent Claim 21 words
The process of claim 15 wherein the weight percentage of tetraethylenepentamines which are non-cyclic is at least about 50 weight percent.

USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1994-02-25 1994-08-27 1995-02-26 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1998-02-25 1998-08-27 1999-02-26 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 2002-02-25 2002-08-27 2003-02-26 $7700.00 Window Closed / Lapsed

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