Ethylene oxide process

Claim 2

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with an oxygen-containing gas at ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° C in the presence of a fixed bed of a silver metal-containing catalyst, the improvement which comprises employing as said catalyst an article comprising a porous refractory support having deposited on its exterior and pore surfaces from about 2% by weight to about 20% by weight of silver and, coincidentally deposited with silver, a total of from about 4.0 × 10 - 5 gew per kilogram of total catalyst to about 8.0 × 10 - 3 gew per kilogram of total catalyst of alkali metal present in final form on the support in the form of an oxide in which said oxide consists of oxides of cesium or rubidium or mixtures thereof.

Claim 3

The process in accord with claim 1 wherein the among of alkali metal coincidentally deposited with the silver is in the range from about 2.0 × 10 - 4 to about 6.5 × 10 - 3 gew per kilogram of total catalyst.

Claim 4

The process in accord with claim 1 wherein the amount of alkali metal coincidentally deposited with the silver is in the range from about 3.0 × 10 - 4 to about 3.2 × 10 - 3 gew per kilogram of total catalyst.

Claim 5

The process in accord with claim 1 wherein the amount of alkali metal coincidentally deposited with the silver is in the range from about 5.0 × 10 - 4 to about 2.4 × 10 - 3 gew per kilogram of total catalyst.

Claim 6

The process in accord with claim 12 wherein the alkali metal coincidentally deposited with the silver is rubidium.

Claim 7

The process in accord with claim 2 wherein the alkali metal coincidentally deposited with the silver is cesium.

Claim 8

The process in accord with claim 4 wherein the alkali metal coincidentally deposited with the silver is rubidium.

Claim 9

The process in accord with claim 4 wherein the alkali metal coincidentally deposited with the silver is cesium.

Claim 10

The process in accord with claim 2 wherein the porous refractory support is alpha alumina and the alkali metal coincidentally deposited with the silver is rubidium.

Claim 11

The process in accord with claim 2 wherein the porous refractory support is alpha alumina and the alkali metal coincidentally deposited with the silver is cesium.

Claim 12

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with an oxygen-containing gas at ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° C in the presence of a fixed bed of a silver metal-containing catalyst, the improvement which comprises employing as said catalyst an article consisting essentially of a porous alpha alumina support having a surface area of from about 0.03 m 2 /g to about 2.0 m 2 /g and having deposited on its exterior and pore surfaces from about 2% by weight to about 20% by weight of silver and, coincidentally deposited with the silver, a total of from about 2.0 × 10 - 4 gew per kilogram of total catalyst to about 6.5 × 10 - 3 gew per kilogram of total catalyst of alkali metal present in final form on the support in the form of an oxide in which the said oxide consists of oxides of cesium or rubidium or mixtures thereof.

Claim 13

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with an oxygen-containing gas at ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° C in the presence of a fixed bed of a silver metal-containing catalyst, the improvement which comprises employing as said catalyst an article consisting essentially of a porous alpha alumina support having a surface area of from about 0.03 m 2 /g to about 2.0 m 2 /g and having deposited on its exterior and pore surfaces from about 2% by weight to about 20% by weight of silver and, coincidentally deposited with the silver, a total of from about 2.0 × 10 - 4 gew per kilogram of total catalyst to about 6.5 × 10 - 3 gew per kilogram of total catalyst of alkali metal present in final form on the support in the form of an oxide in which the said oxide consists of oxides of cesium or rubidium or mixtures thereof.

Claim 14

The process in accord with claim 11 wherein the surface area of the alpha alumina support is from about 0.1 m 2 /g to about 2.0 m 2 /g.

Claim 15

The process in accord with claim 12 wherein the silver is present in an amount of from about 3% by weight to about 15% by weight.

Claim 16

The process in accord with claim 12 wherein the alkali metal coincidentally deposited with the silver is rubidium.

Claim 17

The process in accord with claim 12 wherein the alkali metal coincidentally deposited with the silver is cesium.

Claim 18

The process in accord with claim 14 wherein the concentration of said rubidium is from about 5.0 × 10 - 4 to about 2.4 × 10 - 3 gew per kilogram of total catalyst.

Claim 19

The process in accord with claim 15 wherein the concentration of said cesium is from about 5.0 × 10 - 4 to about 2.4 × 10 - 3 gew per kilogram of total catalyst.

Claim 20

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with an oxygen-containing gas at ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° in the presence of a fixed bed of a silver metal-containing catalyst, the improvement which comprises employing as said catalyst an article comprising a porous support of siliceous composition having a surface area of from about 0.03 m 2 /g to about 2.0 m 2 /g and having deposited on its exterior and pore surfaces from about 2% by weight to about 20% by weight of silver and, coincidentally deposited with the silver, a total of from about 2.0 × 10 - 4 gew per kilogram of total catalyst to about 6.5 × 10 - 3 gew per kilogram of total catalyst of alkali metal present in final form on the support in the form of an oxide in which the said oxide consists of oxides of cesium or rubidium or mixtures thereof.

Claim 21

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with an oxygen-containing gas at ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° in the presence of a fixed bed of a silver metal-containing catalyst, the improvement which comprises employing as said catalyst an article comprising a porous support of siliceous composition having a surface area of from about 0.03 m 2 /g to about 2.0 m 2 /g and having deposited on its exterior and pore surfaces from about 2% by weight to about 20% by weight of silver and, coincidentally deposited with the silver, a total of from about 2.0 × 10 - 4 gew per kilogram of total catalyst to about 6.5 × 10 - 3 gew per kilogram of total catalyst of alkali metal present in final form on the support in the form of an oxide in which the said oxide consists of oxides of cesium or rubidium or mixtures thereof.

Claim 22

The process in accord with claim 18 wherein the amount of alkali metal coincidentally deposited with the silver is in the range from about 5.0 × 10 - 4 to about 2.4 × 20 - 3 gew per kilogram of total catalyst.

Claim 23

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with an oxygen-containing gas at ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° in the presence of a fixed bed of silver metal-contaning catalyst, the improvement which comprises employing as said catalyst an article prepared by a process which comprises impregnating a porous refractory catalyst support with a solution comprising solvent, silver salt sufficient to deposit on said support from 2% by weight to 20% by weight of silver and salts of one or more higher alkali metals sufficient to deposit on said support a total of from about 4.0 × 10 - 5 gew per kilogram of total catalyst to about 8.0 × 10 - 3 gew per kilogram of total catalyst of at least one alkali metal in the form of a salt in which the said salt consists of salts of cesium or rubidium or mixtures thereof; separating the impregnated support from excess impregnating solution and thereafter reducing the silver salt to silver metal at a temperature of from about 100° to about 500° C.

Claim 24

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with an oxygen-containing gas at ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° in the presence of a fixed bed of silver metal-contaning catalyst, the improvement which comprises employing as said catalyst an article prepared by a process which comprises impregnating a porous refractory catalyst support with a solution comprising solvent, silver salt sufficient to deposit on said support from 2% by weight to 20% by weight of silver and salts of one or more higher alkali metals sufficient to deposit on said support a total of from about 4.0 × 10 - 5 gew per kilogram of total catalyst to about 8.0 × 10 - 3 gew per kilogram of total catalyst of at least one alkali metal in the form of a salt in which the said salt consists of salts of cesium or rubidium or mixtures thereof; separating the impregnated support from excess impregnating solution and thereafter reducing the silver salt to silver metal at a temperature of from about 100° to about 500° C.

Claim 25

The process in accord with claim 20 wherein the amount of alkali metal added to the catalyst support is in the range from about 5.0 × 10 - 4 to about 2.4 × 20 - 3 gew per kilogram of total catalyst.

Claim 26

The process in accord with claim 21 wherein the alkali metal coincidentally deposited with the silver is rubidium.

Claim 27

The process in accord with claim 21 wherein the alkali metal coincidentally deposited with the silver is cesium.

Claim 28

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with an oxygen-containing gas at ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° C in the presence of a fixed bed of a silver metal-containing catalyst, the improvement which comprises employing as said catalyst an article prepared by a process which comprises a. impregnating a porous refractory catalyst support with a solution comprising solvent, silver salt sufficient to deposit from 2 by weight to 20% by weight of silver on said support and salts of one or more higher alkali metals in which the said salts consist of salts of cesium or rubidium or mixtures thereof sufficient to deposit an amount of said alkali metal in excess of 8.0 × 10 - 3 gew per kilogram of total catalyst on said support; b. separating the impregnated support; c. reducing the silver salt present on said impregnated support to silver metal at a temperature of from about 100° to about 500° C; d. contacting said impregnated support wherein silver is present as silver metal one or more times with an alkanol of 1 or 2 carbon atoms to selectively remove an amount of higher alkali metal present on said impregnated support such that the impregnated support so contacted contains 4.0 × 10 - 5 to 8.0 × 10 - 3 gew of higher alkali metal per kilogram of catalyst present in final form on the support in the form of an oxide in which the said oxide consists of oxides of cesium or rubidium or mixtures thereof; and e. separating the impregnated support from the alkanol contacting solution and drying to substantially remove the residual alkanol present in and on the impregnated support.

Claim 29

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with an oxygen-containing gas at ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° C in the presence of a fixed bed of a silver metal-containing catalyst, the improvement which comprises employing as said catalyst an article prepared by a process which comprises a. impregnating a porous refractory catalyst support with a solution comprising solvent, silver salt sufficient to deposit from 2 by weight to 20% by weight of silver on said support and salts of one or more higher alkali metals in which the said salts consist of salts of cesium or rubidium or mixtures thereof sufficient to deposit an amount of said alkali metal in excess of 8.0 × 10 - 3 gew per kilogram of total catalyst on said support; b. separating the impregnated support; c. reducing the silver salt present on said impregnated support to silver metal at a temperature of from about 100° to about 500° C; d. contacting said impregnated support wherein silver is present as silver metal one or more times with an alkanol of 1 or 2 carbon atoms to selectively remove an amount of higher alkali metal present on said impregnated support such that the impregnated support so contacted contains 4.0 × 10 - 5 to 8.0 × 10 - 3 gew of higher alkali metal per kilogram of catalyst present in final form on the support in the form of an oxide in which the said oxide consists of oxides of cesium or rubidium or mixtures thereof; and e. separating the impregnated support from the alkanol contacting solution and drying to substantially remove the residual alkanol present in and on the impregnated support.

Claim 30

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with a oxygen-containing gas an ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° C in the presence of a fixed bed of a silver metal-containing catalyst, the improvement which comprises employing as said catalyst an article prepared by a process which comprises a. simultaneously adding to a porous refractory catalyst support from about 3% by weight to about 15% by weight of silver in the form of silver salts and from about 2.0 × 10 - 4 gew per kilogram of total catalyst to about 6.5 × 10 - 3 gew per kilogram of total catalyst of higher alkali metals in the form of water-soluble salts in which the said salts consist of salts of cesium or rubidium or mixtures thereof, by contacting said support with an alkaline aqueous solution of said silver and higher alkali metal salts; and b. maintaining the product of step (a) at a temperature of from about 100° C to about 500° C in the presence of a reducing agent, thereby converting the silver salts to silver metal.

Claim 31

In the process for the production of ethylene oxide wherein ethylene is contacted in vapor phase with a oxygen-containing gas an ethylene oxide forming conditions at an elevated temperature of from 210° to about 285° C in the presence of a fixed bed of a silver metal-containing catalyst, the improvement which comprises employing as said catalyst an article prepared by a process which comprises a. simultaneously adding to a porous refractory catalyst support from about 3% by weight to about 15% by weight of silver in the form of silver salts and from about 2.0 × 10 - 4 gew per kilogram of total catalyst to about 6.5 × 10 - 3 gew per kilogram of total catalyst of higher alkali metals in the form of water-soluble salts in which the said salts consist of salts of cesium or rubidium or mixtures thereof, by contacting said support with an alkaline aqueous solution of said silver and higher alkali metal salts; and b. maintaining the product of step (a) at a temperature of from about 100° C to about 500° C in the presence of a reducing agent, thereby converting the silver salts to silver metal.

Claim 32

The process in accord with claim 25 wherein said alkaline aqueous solution contains an organic amine.

Claim 33

The process in accord with claim 26 wherein said silver salts are silver salts of carboxylic acids.

Claim 34

The process in accord with claim 25 wherein the porous refractory catalyst support consists essentially of alpha alumina.

Claim 35

The process in accord with claim 25 wherein the porous refractory catalyst support is a siliceous solid.