Process for reactivation of iridium-containing catalysts

Claim 2

In a process for reactivating a reforming catalyst, which includes an iridium component composited with a refractory porous inorganic oxide, previously inactivated by coke deposition thereon during contact with a hydrocarbon feed at hydrocarbon conversion conditions and subsequently regenerated by burning at elevated temperatures in the presence of oxygen containing gases to remove accumulated coke deposits therefrom, the improved combination which comprises: contacting, without interim contact with a substantially halogen-free, oxygen-containing gas at temperatures in excess of about 775°F., a bed of the coke-depleted catalyst in a cycle which includes, in sequence, the steps of i. contacting the coke-depleted catalyst with hydrogen or a hydrogen-containing gas at a temperature sufficient to reduce the said iridium component and then ii. contacting said reduced catalyst at an elevated temperature from about 550°F to about 1150°F in a reaction zone provided with exposed ferrous metal surfaces with a gas comprising elemental halogen or halogen precursor and water in amount ranging from about 0.1:1 to 15:1 molar ratio of water:halogen, in a non-oxygen containing atmosphere, sufficient to suppress corrosion of the ferrous metal surfaces of the reaction zone and to effect redispersion of the iridium.

Claim 3

The process of claim 1 wherein the water and halogen are added to the reaction zone in concentration ranging from about 1:1 to 2:1 molar ratio of water: halogen.

Claim 4

The process of claim 2 wherein the molar ratio of water:halogen ranges from about 0.4:1 to about 3.0:1.

Claim 5

The process of claim 1 wherein water is preintroduced into the reaction zone prior to the introduction of the admixture of halogen and water into the reaction zone.

Claim 6

The process of claim 4 wherein the molar ratio of the water:halogen admixture ranges from about 1:1 to about 2:1.

Claim 7

The process of claim 4 wherein the molar ratio of the water:halogen admixture ranges from about 1.2:1 to about 1.6:1.

Claim 8

The process of claim 1 wherein the halogen is chlorine.

Claim 9

In a process for reactivating reforming catalyst, comprised of halogen and iridium composited with a refractory porous inorganic oxide, previously inactivated by coke deposition thereon during contact with a hydrocarbon feed at reforming conditions, and subsequently contacted with oxygen at an elevated temperature to burn accumulated coke deposits therefrom, a method for reactivating said coke depleted catalyst by contacting a bed of the said coke-depleted catalyst without intermediate contact with a substantially halogen-free, oxygencontaining gas at temperatures in excess of about 775°F., which includes the sequence of steps comprising i. contacting said coke-depleted catalyst in a reaction zone with hydrogen or a hydrogen-containing gas at an elevated temperature for a time sufficient to reduce at least a portion of the iridium of said catalyst to its metallic state; ii. contacting said reduced catalyst at an elevated temperature from about 550°F to about 1150°F in a reaction zone, in a non-oxygen atmosphere, with a gas comprising elemental halogen or elemental halogen precursor and water in concentration ranging from about 0.1:1 to 15:1 molar ratio of water:halogen to effect redispersion of the iridium; iii. contacting said treated catalyst from step (ii) in said reaction zone, with hydrogen or a hydrogen-containing gas at an elevated temperature for a time sufficient to further reduce at least a portion of said iridium to its metallic state; and iv. contacting said treated catalyst from step (iii) in said reaction zone, in a non-oxygen-atmosphere with a gas comprising elemental halogen or elemental halogen precursor and water at an elevated temperature from about 550°F to about 1150°F in concentration ranging from about 0.1:1 to 15:1 molar ratio of water:halogen to effect redispersion of the iridium.

Claim 10

In a process for reactivating reforming catalyst, comprised of halogen and iridium composited with a refractory porous inorganic oxide, previously inactivated by coke deposition thereon during contact with a hydrocarbon feed at reforming conditions, and subsequently contacted with oxygen at an elevated temperature to burn accumulated coke deposits therefrom, a method for reactivating said coke depleted catalyst by contacting a bed of the said coke-depleted catalyst without intermediate contact with a substantially halogen-free, oxygencontaining gas at temperatures in excess of about 775°F., which includes the sequence of steps comprising i. contacting said coke-depleted catalyst in a reaction zone with hydrogen or a hydrogen-containing gas at an elevated temperature for a time sufficient to reduce at least a portion of the iridium of said catalyst to its metallic state; ii. contacting said reduced catalyst at an elevated temperature from about 550°F to about 1150°F in a reaction zone, in a non-oxygen atmosphere, with a gas comprising elemental halogen or elemental halogen precursor and water in concentration ranging from about 0.1:1 to 15:1 molar ratio of water:halogen to effect redispersion of the iridium; iii. contacting said treated catalyst from step (ii) in said reaction zone, with hydrogen or a hydrogen-containing gas at an elevated temperature for a time sufficient to further reduce at least a portion of said iridium to its metallic state; and iv. contacting said treated catalyst from step (iii) in said reaction zone, in a non-oxygen-atmosphere with a gas comprising elemental halogen or elemental halogen precursor and water at an elevated temperature from about 550°F to about 1150°F in concentration ranging from about 0.1:1 to 15:1 molar ratio of water:halogen to effect redispersion of the iridium.

Claim 11

The process of claim 8 wherein the water and halogen are added to the reaction zone in steps (ii) and (iv) in concentration ranging from about 1:1 to to 2:1 molar ratio of water:halogen.

Claim 12

The process of claim 9 wherein the molar ratio of water:halogen ranges from about 0.4:1 to 3.0:1.

Claim 13

The process of claim 8 wherein the water and halogen are admixed prior to the introduction of these components into the reaction zone.

Claim 14

The process of claim 11 wherein the molar ratio of water:halogen in the admixture ranges from about 1:1 to about 2:1.

Claim 15

The process of claim 11 wherein the molar ratio of water:halogen ranges from about 1.2:1 to about 1.6:1.

Claim 16

The process of claim 8 wherein the halogen is chlorine.

Claim 17

The process of claim 8 wherein the catalyst is comprised of a composite of iridium and platinum.

Claim 18

In a process for reactivating a reforming catalyst, comprised of halogen and iridium composited with a refractory porous inorganic oxide, previously inactivated by coke deposition thereon during contact with a hydrocarbon feed at reforming conditions, and subsequently contacted with oxygen at an elevated temperature to burn accumulated coke deposits therefrom, a method for reactivating said coke-depleted catalysts by contacting a bed of the said coke-depleted catalyst in a plurality of cycles without intermediate contact with a substantially halogen-free, oxygen-containing gas at temperatures in excess of about 775°F., a cycle of which includes the sequence of steps comprising i. contacting said coke-depleted catalyst in a reaction zone with hydrogen or a hydrogen-containing gas at an elevated temperature for a time sufficient to reduce at least a portion of the iridium of said catalyst to its metallic state; and then ii. contacting said reduced catalyst at an elevated temperature from about 550°F to about 1150°F in a reaction zone, in a non-oxygen containing atmosphere, with a gas comprising elemental halogen or elemental halogen precursor and water in concentration ranging from about 0.1:1 to 15:1 molar ratio of water:halogen up to, but not substantially beyond, the point of halogen breakthrough to effect redispersion of the iridium.

Claim 19

In a process for reactivating a reforming catalyst, comprised of halogen and iridium composited with a refractory porous inorganic oxide, previously inactivated by coke deposition thereon during contact with a hydrocarbon feed at reforming conditions, and subsequently contacted with oxygen at an elevated temperature to burn accumulated coke deposits therefrom, a method for reactivating said coke-depleted catalysts by contacting a bed of the said coke-depleted catalyst in a plurality of cycles without intermediate contact with a substantially halogen-free, oxygen-containing gas at temperatures in excess of about 775°F., a cycle of which includes the sequence of steps comprising i. contacting said coke-depleted catalyst in a reaction zone with hydrogen or a hydrogen-containing gas at an elevated temperature for a time sufficient to reduce at least a portion of the iridium of said catalyst to its metallic state; and then ii. contacting said reduced catalyst at an elevated temperature from about 550°F to about 1150°F in a reaction zone, in a non-oxygen containing atmosphere, with a gas comprising elemental halogen or elemental halogen precursor and water in concentration ranging from about 0.1:1 to 15:1 molar ratio of water:halogen up to, but not substantially beyond, the point of halogen breakthrough to effect redispersion of the iridium.

Claim 20

The process of claim 16 wherein the water and halogen are added to the reaction zone in step (ii) in concentration ranging from about 1:1 to 2:1 molar ratio of water:halogen.

Claim 21

The process of claim 17 wherein the molar ratio of water:halogen ranges from about 0.4:1 to 3.0:1.

Claim 22

The process of claim 16 wherein the water and halogen are admixed prior to introduction of these components into the reaction zone.

Claim 23

The process of claim 16 wherein the molar ratio of water:halogen ranges from about 1.2:1 to about 1.6:1.

Claim 24

The process of claim 16 wherein the halogen is chlorine.

Claim 25

The process of claim 16 wherein the catalyst is comprised of a composite of iridium and platinum.

Claim 26

The process of claim 16 wherein the catalyst is treated in a series of from 2 to about 5 cycles of said sequential hydrogen reduction and halogenation treatments.