Catalytic preparation of linear polyethylenepolyamines [with supported catalyst]

Claim 2

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 which comprises: a. using, as a catalyst, a thermally activated pelleted composition consisting essentially of zirconium silicate having from about 0.5 wt.% to about 10 wt.% of phosphorous thermally chemically bonded thereto, b. continuously contacting a mixture of ethylenediamine and monoethanolamine in a molar ratio of about 1 to about 5 mols 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 product.

Claim 3

A method as in claim 1, wherein the source of phosphorus is phosphoric acid.

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 a catalyst, a thermally activated pelleted composition consisting essentially of zirconium silicate having from about 0.5 wt.% to about 10 wt.% of phosphorous chemically bonded thereto, said catalyst having been prepared by impregnating pellets of zirconium silicate with a liquid phosphorous compound, heating said impregnated pellets at a temperature of about 100° to about 150° C. for about 0.5 to about 5 hours and thereafter recovering and drying the thus treated pellets, b. continuously contacting a mixture of ethylenediamine and monoethanolamine in a molar ratio of about 1 to about 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 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 a catalyst, a thermally activated pelleted composition consisting essentially of zirconium silicate having from about 0.5 wt.% to about 10 wt.% of phosphorous chemically bonded thereto, said catalyst having been prepared by impregnating pellets of zirconium silicate with a liquid phosphorous compound, heating said impregnated pellets at a temperature of about 100° to about 150° C. for about 0.5 to about 5 hours and thereafter recovering and drying the thus treated pellets, b. continuously contacting a mixture of ethylenediamine and monoethanolamine in a molar ratio of about 1 to about 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

A method as in claim 3, wherein the source of the phosphorous is phosphoric acid.

Claim 7

In a method wherein monoethanolamine is reacted with ethylenediamine in a reaction zone 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 a catalyst, a thermally activated pelleted composition consisting essentially of zirconium silicate having from about 0.5 wt.% to about 10 wt.% of phosphorous chemically bonded thereto, said catalyst having been prepared by impregnating pellets of zirconium silicate with a liquid phosphorous compound, heating said impregnated pellets at a temperature of about 100° to about 150° C. for about 0.5 to about 5 hours and thereafter recovering and drying the thus treated pellets, b. continuously contacting a mixture of ethylenediamine and monoethanolamine in said reaction zone in a molar ratio of about 1 to about 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 1,000 to about 2,000 psig. to obtain an essentially noncyclic reaction product comprising diethylenetriamine, triethylenetetramine and tetraethylenepentamine, c. recovering a fraction comprising diethylenetriamine from said reaction product, and d. recycling at least a portion of said diethylenetriamine fraction to said reaction zone.

Claim 8

In a method wherein monoethanolamine is reacted with ethylenediamine in a reaction zone 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 a catalyst, a thermally activated pelleted composition consisting essentially of zirconium silicate having from about 0.5 wt.% to about 10 wt.% of phosphorous chemically bonded thereto, said catalyst having been prepared by impregnating pellets of zirconium silicate with a liquid phosphorous compound, heating said impregnated pellets at a temperature of about 100° to about 150° C. for about 0.5 to about 5 hours and thereafter recovering and drying the thus treated pellets, b. continuously contacting a mixture of ethylenediamine and monoethanolamine in said reaction zone in a molar ratio of about 1 to about 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 1,000 to about 2,000 psig. to obtain an essentially noncyclic reaction product comprising diethylenetriamine, triethylenetetramine and tetraethylenepentamine, c. recovering a fraction comprising diethylenetriamine from said reaction product, and d. recycling at least a portion of said diethylenetriamine fraction to said reaction zone.

Claim 9

A method as in claim 5, wherein the source of the phosphorous is phosphoric acid.