Catalytic (calcined catalyst and) preparation of linear polyethylenepolyamines (therewith)

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 containing titanium triphosphate and 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 phosphoric acid for a period of time ranging from about 0.5 to about 5 hours, thereafter water washing, recovering and drying the thus-treated pellets and then calcining the pellets at about 200° C. to about 800° C. for about 1 to about 24 hours, 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 the reaction product is fractionated to obtain at least a fraction comprising diethylenetriamine and wherein at least a portion of said diethylenetriamine is recycled to the reaction zone together with the said feedstock.

Claim 4

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 a catalyst prepared by treating titania pellets with phosphoric acid for a period of time within the range of about 0.5 to about 5 hours sufficient to thermally chemically bond from about 0.5 to about 10 wt.% of phosphorus to at least the surface of said pellets and to convert at least a portion of the titanium and phosphorous to titanium triphosphate, and thereafter water washing, recovering and drying the thus treated pellets and then calcining said pellets at about 500° to about 700° C. for about 4 to about 16 hours, continuously contacting a mixture of ethylenediamine 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 5

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 a catalyst prepared by treating titania pellets with phosphoric acid for a period of time within the range of about 0.5 to about 5 hours sufficient to thermally chemically bond from about 0.5 to about 10 wt.% of phosphorus to at least the surface of said pellets and to convert at least a portion of the titanium and phosphorous to titanium triphosphate, and thereafter water washing, recovering and drying the thus treated pellets and then calcining said pellets at about 500° to about 700° C. for about 4 to about 16 hours, continuously contacting a mixture of ethylenediamine 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 6

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 the catalyst, a catalyst composition consisting essentially of thermally activated calcined pelleted titania containing titanium triphosphate and 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 impregnating titania pellets with phosphoric acid, heating the impregnated pellets at about 100° to about 150° C. for a period of time ranging from about 0.5 to about 5 hours, thereafter water washing, recovering and drying the thus-treated pellets and then calcining the pellets at about 200° C. to about 800° C. for about 1 to about 24 hours, 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 7

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 the catalyst, a catalyst composition consisting essentially of thermally activated calcined pelleted titania containing titanium triphosphate and 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 impregnating titania pellets with phosphoric acid, heating the impregnated pellets at about 100° to about 150° C. for a period of time ranging from about 0.5 to about 5 hours, thereafter water washing, recovering and drying the thus-treated pellets and then calcining the pellets at about 200° C. to about 800° C. for about 1 to about 24 hours, 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 8

A method as in claim 4, wherein the reaction product is fractionated to obtain at least a fraction comprising diethylenetriamine and wherein at least a portion of said diethylenetriamine is recycled to the reaction zone together with the said feedstock.

Claim 9

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 a catalyst prepared by a process consisting of the steps of impregnating titania pellets with phosphoric acid, heating the impregnated pellets at a temperature of about 100° to about 150° C. for a period of time within the range of about 0.5 to about 5 hours sufficient to thermally chemically bond from about 0.5 to about 10 wt.% of phosphorus to at least the surface of said pellets and to convert at least a portion of the titanium and phosphorous to titanium triphosphate, and thereafter water washing, recovering and drying the thus treated pellets and then calcining said pellets at about 500° to about 700° C. for about 4 to about 16 hours, 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 300° to about 350° C. and a pressure of about 1000 to about 2000 psig. to obtain an essentially noncyclic reaction product.

Claim 10

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 a catalyst prepared by a process consisting of the steps of impregnating titania pellets with phosphoric acid, heating the impregnated pellets at a temperature of about 100° to about 150° C. for a period of time within the range of about 0.5 to about 5 hours sufficient to thermally chemically bond from about 0.5 to about 10 wt.% of phosphorus to at least the surface of said pellets and to convert at least a portion of the titanium and phosphorous to titanium triphosphate, and thereafter water washing, recovering and drying the thus treated pellets and then calcining said pellets at about 500° to about 700° C. for about 4 to about 16 hours, 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 300° to about 350° C. and a pressure of about 1000 to about 2000 psig. to obtain an essentially noncyclic reaction product.