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US3941682A Expired / Lapsed US ⏱️ 0.0 years remaining

Regeneration procedure

Assignee: ExxonMobil Technology and Engineering Co
•
Filing: 1973-08-16
•
Granted: 1976-03-02
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Expires: 1993-08-16
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Abstract

Abstract Supported iridium-containing hydrocarbon conversion catalysts which are at least partially deactivated due to the deposition of carbonaceous residues thereon during contact with hydrocarbons are regenerated by (1) contacting the catalyst in a reaction zone with oxygen to burn at least a portion of the carbonaceous residues from the catalyst, (2) contacting the carbonaceous residuedepleted catalyst in a reaction zone with hydrogen at an elevated temperature to reduce a substantial portion of the iridium present on the catalyst to its metallic form, (3) contacting the treated catalyst in a reaction zone with an elemental halogen-containing gas in a reaction zone with an elemental halogen-containing gas at a temperature greater than about 850°F., said gas being introduced into said reaction zone at a rate such that the halogen concentration of the treating gas at the outlet of said reaction zone is at least 50% of the inlet halogen concentration within at least 15 minutes from the time of the introduction of said treating gas into the inlet of said reaction zone, (4) contacting the treated catalyst in a reaction zone with hydrogen at an elevated temperature to reduce a substantial portion of the iridium present in the catalyst to its metallic form, and (5) contacting the catalyst from step (4) in a reaction zone with an elemental halogen-containing gas at a temperature of at least about 850°F. Steps (4) and (5) may be repeated, in sequence, at least one additional time to redisperse the iridium catalyst component to a highly active, high surface area state.

Inventors

  • 👤 Walter S. Kmak
  • 👤 David J. C. Yates

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-11-01 01:10
CPC Classifications
B; B01; B01J; B01J23/00; B01J23/90; B01J23/96; B01J37/00; B01J37/22; B01J37/24; C; C10; C10G; C10G35/00; C10G35/04; C10G35/06; C10G35/085; C10G35/09

Claims Analysis

Total Claims: 27
Claim 1
Independent Claim 149 words
In a process for the catalytic reforming of hydrocarbons wherein a hydrocarbon feed stock is contacted with a catalyst comprising from about 0.01 to about 3.0 wt. % of an iridium component contained on a refractory inorganic oxide support at reforming conditions, the catalyst having been at least partially deactivated during contact with said feed stock by the deposition of carbonaceous residues, a method for regenerating said catalyst after discontinuing said contact of said catalyst with said feed stock comprising: 1. contacting said catalyst in a reaction zone with a gaseous mixture containing oxygen at an elevated temperature for a time sufficient to burn a substantial portion of said carbonaceous residues from said catalyst, the duration of said contacting at said elevated temperature being insufficient to convert more than about 70 wt. % of the iridium on said catalyst to agglomerates having crystalline sizes greater than about 50A; 2.
Claim 2
Dependent Claim 149 words
In a process for the catalytic reforming of hydrocarbons wherein a hydrocarbon feed stock is contacted with a catalyst comprising from about 0.01 to about 3.0 wt. % of an iridium component contained on a refractory inorganic oxide support at reforming conditions, the catalyst having been at least partially deactivated during contact with said feed stock by the deposition of carbonaceous residues, a method for regenerating said catalyst after discontinuing said contact of said catalyst with said feed stock comprising: 1. contacting said catalyst in a reaction zone with a gaseous mixture containing oxygen at an elevated temperature for a time sufficient to burn a substantial portion of said carbonaceous residues from said catalyst, the duration of said contacting at said elevated temperature being insufficient to convert more than about 70 wt. % of the iridium on said catalyst to agglomerates having crystalline sizes greater than about 50A; 2.
Claim 3
Dependent Claim 234 words
contacting said carbonaceous residue-depleted catalyst in said reaction zone with a hydrogen-containing gas at an elevated temperature for a time sufficient to convert a substantial portion of said iridium to its metallic form, said step (2) being effected prior to contact with a substantially halogen-free, oxygen-containing gas at a temperature sufficient to agglomerate further the iridium on said catalyst; 3. contacting said treated catalyst having a substantial portion of the iridium contained thereon in the metallic form in said reaction zone with an elemental halogen-containing gas at a temperature greater than about 850° F., said gas being introduced into said reaction zone at a rate such that the halogen concentration of the treating gas at the outlet of said reaction zone is at least 50% of the inlet halogen concentration within at least 15 minutes from the time of the introduction of said treating gas into the inlet of said reaction zone; 4. contacting said halogen treated catalyst in said reaction zone with a hydrogen-containing gas at an elevated temperature for a time sufficient to convert a substantial portion of said iridium to its metallic form; and 5. contacting said treated catalyst having a substantial portion of the iridium contained thereon in the metallic form in said reaction zone with an elemental halogen-containing gas at a temperature of at least about 850° F. for a time sufficient to redisperse at least a portion of
Claim 4
Dependent Claim 234 words
contacting said carbonaceous residue-depleted catalyst in said reaction zone with a hydrogen-containing gas at an elevated temperature for a time sufficient to convert a substantial portion of said iridium to its metallic form, said step (2) being effected prior to contact with a substantially halogen-free, oxygen-containing gas at a temperature sufficient to agglomerate further the iridium on said catalyst; 3. contacting said treated catalyst having a substantial portion of the iridium contained thereon in the metallic form in said reaction zone with an elemental halogen-containing gas at a temperature greater than about 850° F., said gas being introduced into said reaction zone at a rate such that the halogen concentration of the treating gas at the outlet of said reaction zone is at least 50% of the inlet halogen concentration within at least 15 minutes from the time of the introduction of said treating gas into the inlet of said reaction zone; 4. contacting said halogen treated catalyst in said reaction zone with a hydrogen-containing gas at an elevated temperature for a time sufficient to convert a substantial portion of said iridium to its metallic form; and 5. contacting said treated catalyst having a substantial portion of the iridium contained thereon in the metallic form in said reaction zone with an elemental halogen-containing gas at a temperature of at least about 850° F. for a time sufficient to redisperse at least a portion of
Claim 5
Dependent Claim 56 words
the iridium on the catalyst. 2. The process of claim 1 wherein, after completion of said step (1), said catalyst is contacted with an inert purge gas at a temperature of below about 750° F. for a time sufficient to remove substantially all of the carbon dioxide, carbon monoxide and oxygen present in said reaction zone.
Claim 6
Dependent Claim 20 words
The process of claim 1 wherein said steps (4) and (5) are repeated, in sequence, at least one additional time.
Claim 7
Dependent Claim 19 words
The process of claim 1 wherein said halogen-containing gas employed in steps (3) and (5) is a chlorine-containing gas.
Claim 8
Dependent Claim 20 words
The process of claim 2 wherein said halogen-containing gas employed in said steps (3) and (5) is a chlorine-containing gas.
Claim 9
Dependent Claim 23 words
The process of claim 1 wherein said steps (2) and (4) are conducted at a temperature varying from about 650° to 950° F.
Claim 10
Dependent Claim 23 words
The process of claim 2 wherein said steps (2) and (4) are conducted at a temperature varying from about 650° to 950° F.
Claim 11
Dependent Claim 23 words
The process of claim 5 wherein said steps (2) and (4) are conducted at a temperature varying from about 650° to 950° F.
Claim 12
Dependent Claim 156 words
In a process for the catalytic reforming of a naphtha feed stock wherein said naphtha feed stock and hydrogen are contacted with a catalyst comprising from about 0.01 to about 3.0 wt. % of an iridium component and a halogen component contained on an alumina support at naphtha reforming conditions, the catalyst having been at least partially deactivated during contact with said naphtha feed stock by the deposition of carbonaceous residues, a method for regenerating said catalyst after discontinuing contact of said catalyst with said feed stock comprising; 1. contacting said catalyst in a reaction zone with a gaseous mixture containing oxygen at an elevated temperature for a time sufficient to burn a substantial portion of said carbonaceous residues from said catalyst, the duration of said contacting at said elevated temperature being insufficient to convert more than about 70 wt. % of the iridium on said catalyst to agglomerates having crystallite sizes greater than about 50A;
Claim 13
Dependent Claim 156 words
In a process for the catalytic reforming of a naphtha feed stock wherein said naphtha feed stock and hydrogen are contacted with a catalyst comprising from about 0.01 to about 3.0 wt. % of an iridium component and a halogen component contained on an alumina support at naphtha reforming conditions, the catalyst having been at least partially deactivated during contact with said naphtha feed stock by the deposition of carbonaceous residues, a method for regenerating said catalyst after discontinuing contact of said catalyst with said feed stock comprising; 1. contacting said catalyst in a reaction zone with a gaseous mixture containing oxygen at an elevated temperature for a time sufficient to burn a substantial portion of said carbonaceous residues from said catalyst, the duration of said contacting at said elevated temperature being insufficient to convert more than about 70 wt. % of the iridium on said catalyst to agglomerates having crystallite sizes greater than about 50A;
Claim 14
Dependent Claim 307 words
contacting said carbonaceous residue-depleted catalyst in said reaction zone with a gas mixture containing hydrogen at a temperature varying from about 650° - 950° F. for a time sufficient to convert a substantial portion of said iridium to its metallic form, wherein said step (2) is effected prior to contact with a substantially halogen-free, oxygen-containing gas at a temperature sufficient to agglomerate further the iridium on said catalyst; 3. contacting said treated catalyst having a substantial portion of the iridium contained thereon in the metallic form in said reaction zone with a gas mixture containing chlorine at a temperature of greater than about 850° F., said gas mixture being introduced into said reaction zone at a rate such that the chlorine concentration of the treating gas at the outlet of said reaction zone is at least 50% of the inlet chlorine concentration within at least 15 minutes from the time of the introduction of said treating gas into the inlet of said reaction zone; 4. contacting said chlorine treated catalyst in a reaction zone with a gas mixture containing hydrogen at a temperature varying from about 650° to 950° F. for a time sufficient to convert a substantial portion of said iridium to its metallic form; 5. contacting said treated catalyst having a substantial portion of the iridium contained thereon in the metallic form in said reaction zone with a gas mixture containing chlorine at a temperature greater than about 850° F. for a time sufficient to redisperse at least a portion of the iridium on the catalyst; and 6. contacting said treated catalyst from step (5) in a reaction zone with said naphtha feed stock and hydrogen at naphtha reforming conditions, wherein said step is effected prior to contact with a substantially halogen-free, oxygen-containing gas at a temperature sufficient to agglomerate the iridium on said catalyst.
Claim 15
Dependent Claim 307 words
contacting said carbonaceous residue-depleted catalyst in said reaction zone with a gas mixture containing hydrogen at a temperature varying from about 650° - 950° F. for a time sufficient to convert a substantial portion of said iridium to its metallic form, wherein said step (2) is effected prior to contact with a substantially halogen-free, oxygen-containing gas at a temperature sufficient to agglomerate further the iridium on said catalyst; 3. contacting said treated catalyst having a substantial portion of the iridium contained thereon in the metallic form in said reaction zone with a gas mixture containing chlorine at a temperature of greater than about 850° F., said gas mixture being introduced into said reaction zone at a rate such that the chlorine concentration of the treating gas at the outlet of said reaction zone is at least 50% of the inlet chlorine concentration within at least 15 minutes from the time of the introduction of said treating gas into the inlet of said reaction zone; 4. contacting said chlorine treated catalyst in a reaction zone with a gas mixture containing hydrogen at a temperature varying from about 650° to 950° F. for a time sufficient to convert a substantial portion of said iridium to its metallic form; 5. contacting said treated catalyst having a substantial portion of the iridium contained thereon in the metallic form in said reaction zone with a gas mixture containing chlorine at a temperature greater than about 850° F. for a time sufficient to redisperse at least a portion of the iridium on the catalyst; and 6. contacting said treated catalyst from step (5) in a reaction zone with said naphtha feed stock and hydrogen at naphtha reforming conditions, wherein said step is effected prior to contact with a substantially halogen-free, oxygen-containing gas at a temperature sufficient to agglomerate the iridium on said catalyst.
Claim 16
Dependent Claim 21 words
The process of claim 9 wherein said step (1) operation is conducted at a temperature of less than about 850° F.
Claim 17
Dependent Claim 23 words
The process of claim 9 wherein said steps (3) and (5) are conducted at a temperature varying from about 850° to 1150° F.
Claim 18
Dependent Claim 50 words
The process of claim 9 wherein, after completion of said step (1), said catalyst is contacted with an inert purge gas at a temperature of below about 750° F. for a time sufficient to remove substantially all of the carbon dioxide, carbon monoxide and oxygen present in said reaction zone.
Claim 19
Dependent Claim 20 words
The process of claim 9 wherein said steps (4) and (5) are repeated, in sequence, at least one additional time.
Claim 20
Dependent Claim 52 words
The process of claim 9 wherein said hydrogen-containing gas is substantially removed from the reaction zone prior to each of said subsequent steps wherein said catalyst is contacted with a chlorine-containing gas and said chlorine-containing gas is substantially removed from said reaction zone prior to contacting said catalyst with said hydrogen-containing gas.
Claim 21
Dependent Claim 52 words
The process of claim 12 wherein said hydrogen-containing gas is substantially removed from the reaction zone prior to each of said subsequent steps wherein said catalyst is contacted with a chlorine-containing gas and said chlorine-containing gas is substantially removed from said reaction zone prior to contacting said catalyst with said hydrogen-containing gas.
Claim 22
Dependent Claim 52 words
The process of claim 13 wherein said hydrogen-containing gas is substantially removed from the reaction zone prior to each of said subsequent steps wherein said catalyst is contacted with a chlorine-containing gas and said chlorine-containing gas is substantially removed from said reaction zone prior to contacting said catalyst with said hydrogen-containing gas.
Claim 23
Dependent Claim 31 words
The process of claim 1 wherein the halogen-containing gas of steps (3) and (5) contains water in amounts ranging from about 0.02 to 1.0% by volume, based on total treat gas.
Claim 24
Dependent Claim 33 words
The process of claim 1 wherein the halogen-containing gas in steps (3) and (5) contains oxygen, the molar ratio of oxygen to elemental halogen in said halogen-containing gas being less than about 10;1.
Claim 25
Dependent Claim 34 words
The process of claim 9 wherein the gas mixture in steps (3) and (5) comprises chlorine and oxygen, the molar ratio of oxygen to chlorine in said gas mixture being less than about 10:1.
Claim 26
Dependent Claim 32 words
The process of claim 9 wherein the contacting in steps (3) and (5) is continued for a time sufficient to introduce from 0.1 to 4.0 wt. % additional chlorine onto the catalyst.
Claim 27
Dependent Claim 23 words
The process of claim 1 wherein said steps (2) and (4) are conducted at a temperature varying from about 400° to 1100° F.

References Cited (Backward Citations)

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USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1979-03-02 1979-09-01 1980-03-02 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1983-03-02 1983-09-01 1984-03-02 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 1987-03-02 1987-09-01 1988-03-02 $7700.00 Window Closed / Lapsed

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