Patent US4356312A successfully refreshed from Google Patents.
US4356312A
Expired / Lapsed
US
⏱️ 0.0 years remaining
Ethylene oxide process
Assignee: Shell USA Inc
•
Filing: 1979-03-22
•
Granted: 1982-10-26
•
Expires: 1999-03-22
Abstract
Abstract When supported silver materials are being prepared, deposits of from about 4.0×10 -5 to about 8.0×10 -3 gram equivalent weights per kilogram of finished product of ionic, higher alkali metals, i.e., ionic potassium, rubidium or cesium simultaneously with the deposit of silver improves the selectivity of these materials as catalysts for ethylene oxide production. Particularly good results are obtained with potassium.
Inventors
- 👤 Robert P. Nielsen
- 👤 John H. La Rochelle
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-08 07:53
CPC Classifications
C; C07; C07D; C07D301/00; C07D301/02; C07D301/03; C07D301/04; C07D301/08; C07D301/10; B; B01; B01J; B01J23/00; B01J23/38; B01J23/54; B01J23/66; B01J35/00; B01J35/60; B01J35/61; B01J35/612; B01J35/63; B01J35/633; Y; Y02; Y02P; Y02P20/00; Y02P20/50; Y02P20/52
Claims Analysis
Total Claims: 31
Claim 1
Independent Claim
138 words
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° C. to about 285° C. in the presence of a fixed bed of 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 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -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 the oxide of potassium.
Claim 2
Dependent Claim
138 words
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° C. to about 285° C. in the presence of a fixed bed of 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 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -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 the oxide of potassium.
Claim 3
Dependent Claim
36 words
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 4
Dependent Claim
36 words
The process in accord with claim 1 wherein the amount of alkali metal coincidentally deposited with the silver is in the range from about 7.5×10 -4 to about 2.3×10 -3 gew per kilogram of total catalyst.
Claim 5
Dependent Claim
15 words
The process in accord with claim 1 wherein the porous refractory support is alpha alumina.
Claim 6
Dependent Claim
161 words
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° C. 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 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -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 the oxide of potassium.
Claim 7
Dependent Claim
161 words
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° C. 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 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -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 the oxide of potassium.
Claim 8
Dependent Claim
29 words
The process in accord with claim 5 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 9
Dependent Claim
26 words
The process in accord with claim 6 wherein the silver is present in an amount of from about 3% by weight to about 15% by weight.
Claim 10
Dependent Claim
28 words
The process in accord with claim 6 wherein the concentration of said potassium is from about 5.0×10 -4 to about 2.4×10 -3 gew per kilogram of total catalyst.
Claim 11
Dependent Claim
28 words
The process in accord with claim 6 wherein the concentration of said potassium is from about 7.5×10 -4 to about 2.3×10 -3 gew per kilogram of total catalyst.
Claim 12
Dependent Claim
160 words
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° C. 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 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 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -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 the oxide of potassium.
Claim 13
Dependent Claim
160 words
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° C. 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 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 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -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 the oxide of potassium.
Claim 14
Dependent Claim
36 words
The process in accord with claim 10 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 15
Dependent Claim
36 words
The process in accord with claim 10 wherein the amount of alkali metal coincidentally deposited with the silver is in the range from about 7.5×10 -4 to about 2.3×10 -3 gew per kilogram of total catalyst.
Claim 16
Dependent Claim
181 words
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° C. 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 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 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -3 gew per kilogram of total catalyst of alkali metal in the form of a salt in which the said salt consists of the salt of potassium; separating the impregnated support from excess impregnating solution and thereafter reducing the silver salt to silver metal at a temperature of from about 100° C. to about 500° C.
Claim 17
Dependent Claim
181 words
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° C. 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 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 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -3 gew per kilogram of total catalyst of alkali metal in the form of a salt in which the said salt consists of the salt of potassium; separating the impregnated support from excess impregnating solution and thereafter reducing the silver salt to silver metal at a temperature of from about 100° C. to about 500° C.
Claim 18
Dependent Claim
36 words
The process in accord with claim 13 wherein the amount of alkali metal added to the catalyst support is in the range from about 5.0×10 -4 to about 2.4×10 -3 gew per kilogram of total catalyst.
Claim 19
Dependent Claim
36 words
The process in accord with claim 13 wherein the amount of alkali metal added to the catalyst support is in the range from about 7.5×10 -4 to about 2.3×10 -3 gew per kilogram of total catalyst.
Claim 20
Dependent Claim
272 words
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° C. 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 solution comprising solvent, silver salt sufficient to deposit from 2% by weight to 20% by weight of silver on said support and salts of alkali metal in which said salt consists of the salt of potassium, sufficient to deposit an amount of the alkali metal in excess of 3.2×10 -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° C. 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 3.0×10 -4 to 3.2×10 -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 the oxide of potassium; (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 21
Dependent Claim
272 words
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° C. 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 solution comprising solvent, silver salt sufficient to deposit from 2% by weight to 20% by weight of silver on said support and salts of alkali metal in which said salt consists of the salt of potassium, sufficient to deposit an amount of the alkali metal in excess of 3.2×10 -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° C. 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 3.0×10 -4 to 3.2×10 -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 the oxide of potassium; (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 22
Dependent Claim
36 words
The process in accord with claim 16 wherein the amount of alkali metal added to the catalyst support is in the range from about 5.0×10 -4 to about 2.4×10 -3 gew per kilogram of total catalyst.
Claim 23
Dependent Claim
36 words
The process in accord with claim 16 wherein the amount of alkali metal added to the catalyst support is in the range from about 7.5×10 -4 to about 2.3×10 -3 gew per kilogram of total catalyst.
Claim 24
Dependent Claim
183 words
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° C. 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 catalyst and from about 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -3 gew per kilogram of total catalyst of alkali metal in the form of water-soluble salts in which said salts consist of salts of potassium, 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 25
Dependent Claim
183 words
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° C. 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 catalyst and from about 3.0×10 -4 gew per kilogram of total catalyst to about 3.2×10 -3 gew per kilogram of total catalyst of alkali metal in the form of water-soluble salts in which said salts consist of salts of potassium, 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 26
Dependent Claim
36 words
The process in accord with claim 19 wherein the amount of alkali metal added to the catalyst support is in the range from about 5.0×10 -4 to about 2.4×10 -3 gew per kilogram of total catalyst.
Claim 27
Dependent Claim
36 words
The process in accord with claim 19 wherein the amount of alkali metal added to the catalyst support is in the range from about 7.5×10 -4 to about 2.3×10 -3 gew per kilogram of total catalyst.
Claim 28
Dependent Claim
16 words
The process in accord with claim 19 wherein said alkaline aqueous solution contains an organic amine.
Claim 29
Dependent Claim
17 words
The process in accord with claim 22 wherein said silver salts are silver salts of carboxylic acids.
Claim 30
Dependent Claim
18 words
The process in accord with claim 19 wherein the porous refractory catalyst support consists essentially of alpha alumina.
Claim 31
Dependent Claim
17 words
The process in accord with claim 19 wherein the porous refractory catalyst support is a siliceous solid.
References Cited (Backward Citations)
USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
|---|---|---|---|---|---|
| 3.5 Years (Year 4) | 1985-10-25 | 1986-04-26 | 1986-10-26 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1989-10-25 | 1990-04-26 | 1990-10-26 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 1993-10-25 | 1994-04-26 | 1994-10-26 | $7700.00 | Window Closed / Lapsed |