Catalytic process for the preparation of linear polyethylenepolyamines with tungstophosphoric acid-or molybdophosphoric acid-on-titania catalysts

Claim 2

In a method wherein monoethanolamine is reacted with ethylenediamine in a reaction zone in the presence of a phosphorus-containing catalyst to provide an essentialy noncyclic product comprising polyethylenepolyamines, the improvement for conducting said process on a continuous basis which comprises: a. using, as a catalyst, titania pellets having deposited thereon a minor amount of a tungstophosphoric acid or a molybdophosphoric acid or a mixture thereof; b. 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 3

A method as in claim 1 wherein a minor amount of a tungstophosphoric acid is deposited on the titania pellets.

Claim 4

A method as in claim 1 wherein a minor amount of a molybdophosphoric acid is deposited on the titania pellets.

Claim 5

In a method wherein monoethanolamine is reacted with ethylenediamine in a reaction zone 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, a composition prepared by impregnating titania pellets with an aqueous solution of a tungstophosphoric acid or a molybdophosphoric acid or a salt thereof or a mixture thereof, and thereafter drying and calcining the titania pellets to thereby provide a catalyst composition composed of titania pellets having from about 0.01 to about 10 wt. % of phosphorus and about 0.1 to about 30 wt. % of tungsten or molybdenum or a mixture thereof deposited thereon; b. 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 270° to about 320° C. and a pressure of about 1,000 to about 2,000 psig. to obtain an essentially noncyclic reaction product.

Claim 6

In a method wherein monoethanolamine is reacted with ethylenediamine in a reaction zone 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, a composition prepared by impregnating titania pellets with an aqueous solution of a tungstophosphoric acid or a molybdophosphoric acid or a salt thereof or a mixture thereof, and thereafter drying and calcining the titania pellets to thereby provide a catalyst composition composed of titania pellets having from about 0.01 to about 10 wt. % of phosphorus and about 0.1 to about 30 wt. % of tungsten or molybdenum or a mixture thereof deposited thereon; b. 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 270° to about 320° C. and a pressure of about 1,000 to about 2,000 psig. to obtain an essentially noncyclic reaction product.

Claim 7

A method as in claim 4 wherein a minor amount of a tungstophosphoric acid is deposited on the titania pellets.

Claim 8

A method as in claim 5 wherein the tungstophosphoric acid is 12-tungstophosphoric acid.

Claim 9

A method as in claim 4 wherein a minor amount of a molybdophosphoric acid is deposited on the titania pellets.

Claim 10

A method as in claim 7 wherein the molybdophosphoric acid is 12-molybdophosphoric acid.

Claim 11

As a new composition of matter, a catalytically active pelleted composition, said composition having been prepared by impregnating titania pellets with an aqueous solution of a tungstophosphoric acid or a molybdophosphoric acid or a mixture thereof and by thereafter drying and calcining the thus-treated titania pellets to thereby provide a catalyst composition composed of titania pellets having from about 0.1 to about 10 wt. % of phosphorus and about 0.1 to about 30 wt. % of tungsten or molybdenum or a mixture thereof deposited thereon.

Claim 12

As a new composition of matter, a catalytically active pelleted composition, said composition having been prepared by impregnating titania pellets with an aqueous solution of a tungstophosphoric acid or a molybdophosphoric acid or a mixture thereof and by thereafter drying and calcining the thus-treated titania pellets to thereby provide a catalyst composition composed of titania pellets having from about 0.1 to about 10 wt. % of phosphorus and about 0.1 to about 30 wt. % of tungsten or molybdenum or a mixture thereof deposited thereon.

Claim 13

A composition as in claim 9 wherein a minor amount of tungstophosphoric acid is deposited on the titania pellets.

Claim 14

A composition as in claim 10 wherein the tungstophosphoric acid is 12-tungstophosphoric acid.

Claim 15

A composition as in claim 9 wherein a minor amount of a molybdophosphoric acid is deposited on the titania pellets.

Claim 16

A method as in claim 12 wherein the molybdophosphoric acid is 12-molybdophosphoric acid.

Claim 17

As a new composition of matter, a catalytically active pelleted composition, said composition having been prepared by immersing titania pellets in about a 1 wt. % to about a 50 wt. % aqueous solution of a tungstophosphoric acid or a molybdophosphoric acid or a sodium or a potassium salt thereof or a mixture thereof for about 0.1 to about 5 hours at a temperature of up to about 150° C. and by thereafter drying and calcining the thus-treated titania pellets at a temperature of about 200° to about 800° C. for about 2 to about 24 hours to thereby provide a catalyst composition composed of titania pellets having from about 0.1 to about 1.0 wt. % of phosphorus and about 0.1 to about 30 wt. % of tungsten or molybdenum or a mixture thereof deposited thereon.

Claim 18

As a new composition of matter, a catalytically active pelleted composition, said composition having been prepared by immersing titania pellets in about a 1 wt. % to about a 50 wt. % aqueous solution of a tungstophosphoric acid or a molybdophosphoric acid or a sodium or a potassium salt thereof or a mixture thereof for about 0.1 to about 5 hours at a temperature of up to about 150° C. and by thereafter drying and calcining the thus-treated titania pellets at a temperature of about 200° to about 800° C. for about 2 to about 24 hours to thereby provide a catalyst composition composed of titania pellets having from about 0.1 to about 1.0 wt. % of phosphorus and about 0.1 to about 30 wt. % of tungsten or molybdenum or a mixture thereof deposited thereon.

Claim 19

A composition as in claim 14 wherein the acid is a tungstophosphoric acid or a sodium or potassium salt thereof.

Claim 20

A composition as in claim 15 wherein the tungstophosphoric acid is 12-tungstophosphoric acid.

Claim 21

A composition as in claim 14 wherein the acid is a molybdophosphoric acid or a sodium or a potassium salt thereof.

Claim 22

A method as in claim 17 wherein the molybdophosphoric acid is 12-molybdophosphoric acid.