Catalytic synthesis of linear polyethylenepolyamines (polyethylenepolyamine preparation and catalyst)

Claim 2

In a method wherein monoethanolamine is reacted with ethylenediamine in the presence of a phosphorus containing catalyst to provide an essentially noncyclic product comprising polyethylenepolyamines, the improvement for conducting said process on a continuous basis which comprises: a. using, as a catalyst, thermally activated calcined pelleted titania having thermally chemically bonded to at least the surface thereof about 0.5 to about 10 wt. % of phosphorus, said catalyst having been prepared by treating titania pellets with polyphosphoric acid for a period of time ranging from about 0.5 to about 5 hours, and thereafter water washing, recovering and drying the thus-treated pellets, b. continuously contacting a mixture of ethylene diamine and monoethanolamine in a molar ratio of about 1 to 5 moles of ethylenediamine per mole of monoethanolamine with said pelleted catalyst at a temperature of about 250° to about 400° C. and a pressure of about 500 to about 3000 psig. to obtain an essentially noncyclic reaction product.

Claim 3

A method as in claim 1, wherein at least a portion of the diethylenetriamine reaction product is recycled to the reaction zone.

Claim 4

In a method wherein monoethanolamine is reacted with ethylenediamine in the presence of a phosphorous containing catalyst to provide an essentially noncyclic product comprising polyethylenepolyamines, the improvement for conducting said process on a continuous basis which comprises: a. using, as the catalyst, a catalyst composition consisting essentially of thermally activated calcined pellets of titania having thermally chemically bonded to at least the surface thereof about 0.5 to about 10 wt. % of phosphorous, said catalyst having been prepared by impregnating titania pellets with polyphosphoric acid, heating said impregnated pellets at a temperature of about 100° to about 150° C. for a period of time ranging from about 0.5 to 5 hours, and thereafter water washing, recovering and drying the thus-treated pellets, b. continuously contacting a mixture of ethylenediamine and monoethanolamine in a molar ratio of about 2 to 5 moles of ethylenediamine per mole of monoethanolamine with said pelleted catalyst at a temperature of about 250° to about 400° C. and a pressure of about 500 to about 3000 psig to obtain an essentially noncyclic reaction product comprising diethylenetriamine.

Claim 5

In a method wherein monoethanolamine is reacted with ethylenediamine in the presence of a phosphorous containing catalyst to provide an essentially noncyclic product comprising polyethylenepolyamines, the improvement for conducting said process on a continuous basis which comprises: a. using, as the catalyst, a catalyst composition consisting essentially of thermally activated calcined pellets of titania having thermally chemically bonded to at least the surface thereof about 0.5 to about 10 wt. % of phosphorous, said catalyst having been prepared by impregnating titania pellets with polyphosphoric acid, heating said impregnated pellets at a temperature of about 100° to about 150° C. for a period of time ranging from about 0.5 to 5 hours, and thereafter water washing, recovering and drying the thus-treated pellets, b. continuously contacting a mixture of ethylenediamine and monoethanolamine in a molar ratio of about 2 to 5 moles of ethylenediamine per mole of monoethanolamine with said pelleted catalyst at a temperature of about 250° to about 400° C. and a pressure of about 500 to about 3000 psig to obtain an essentially noncyclic reaction product comprising diethylenetriamine.

Claim 6

A method as in claim 3, wherein at least a portion of the diethylenetriamine reaction product is recycled to the reaction zone.

Claim 7

In a method wherein monoethanolamine is reacted with ethylenediamine in the presence of a phosphorous containing catalyst to provide an essentially noncyclic product comprising polyethylenepolyamines, the improvement for conducting said process on a continuous basis which comprises: a. using a catalyst prepared by a process consisting essentially of the steps of impregnating pellets of titania with polyphosphoric acid, heating said impregnated pellets at a temperature of about 100° to about 150° C. for a period of time ranging from about 0.5 to about 5 hours to thermally chemically bond from about 0.5 to about 10 wt. % of phosphorous to at least the surface of said pellets, and thereafter water washing, recovering and drying the thus-treated pellets, b. continuously contacting a mixture of ethylenediamine and monoethanolamine in a molar ratio of about 2 to 5 moles of ethylenediamine per mole of monoethanolamine with said pelleted catalyst at a temperature of about 300° to about 350° C. and a pressure of about 1000 to about 2000 psig to obtain an essentially noncyclic reaction product comprising diethylenetriamine.

Claim 8

In a method wherein monoethanolamine is reacted with ethylenediamine in the presence of a phosphorous containing catalyst to provide an essentially noncyclic product comprising polyethylenepolyamines, the improvement for conducting said process on a continuous basis which comprises: a. using a catalyst prepared by a process consisting essentially of the steps of impregnating pellets of titania with polyphosphoric acid, heating said impregnated pellets at a temperature of about 100° to about 150° C. for a period of time ranging from about 0.5 to about 5 hours to thermally chemically bond from about 0.5 to about 10 wt. % of phosphorous to at least the surface of said pellets, and thereafter water washing, recovering and drying the thus-treated pellets, b. continuously contacting a mixture of ethylenediamine and monoethanolamine in a molar ratio of about 2 to 5 moles of ethylenediamine per mole of monoethanolamine with said pelleted catalyst at a temperature of about 300° to about 350° C. and a pressure of about 1000 to about 2000 psig to obtain an essentially noncyclic reaction product comprising diethylenetriamine.

Claim 9

A method as in claim 5, wherein the dried pellets are calcined at a temperature of about 200° to about 800° C. for a period of time within the range of about 2 to 24 hours.