Reactivation process for iridium-containing catalysts using low halogen flow rates

Claim 2

A process for reactivating an agglomerated catalyst containing metallic iridium comprising the steps of: (a) pretreating said catalyst by contact with a substantially elemental oxygen-free atmosphere comprising a halide-providing compound at elevated temperature for a sufficient time to provide about 1.3 weight percent and above halide to the catalyst, taken as the coke-free, dry catalyst; and (b) redispersing the metallic iridium from step (a) while maintaining said 1.3 weight percent and above halide provided to the catalyst by contact with an atmosphere comprising elemental halogen and a redispersing aid selected from elemental oxygen or elemental oxygen and water wherein said halogen and oxygen are present in a halogen to oxygen volume ratio in the range of about 0.05 to 10, at elevated temperature, at a halogen mass flow rate of about one-tenth gram or less of elemental halogen per 100 grams of catalyst per hour for a total halogen amount of up to 0.5 gram halogen per 100 grams catalyst, for a time sufficient to effect about a 75 to 100 percent redispersion of said metallic iridium.

Claim 3

The process of claim 1 wherein said catalyst is initially present substantially as agglomerated metallic iridium.

Claim 4

The process of claim 1 wherein said agglomerated iridium-containing catalyst is present on a catalyst support selected from silica, zeolite, alumina, silica-alumina, zirconia, alumina-zirconia, and mixtures thereof.

Claim 5

The process of claim 1 wherein said iridium-containing catalyst further contains a metal co-catalyst selected from platinum, rhodium, rhenium, palladium and mixtures thereof.

Claim 6

The process of claim 1 wherein said halide-providing compound is one which generates a hydrogen halide in the presence of hydrogen gas.

Claim 7

The process of claim 5 wherein said halide-providing compound is selected from carbon tetrachloride, chloroform, methylene chloride, methyl chloride, 1,2-dichloroethane, hexachloroethane, and mixtures thereof in the presence of hydrogen gas.

Claim 8

The process of claim 1 wherein said halide-providing compound is hydrogen chloride.

Claim 9

The process of claim 1 wherein said halide is present on the catalyst after step (a) in an amount of about 1.4 to 2.5 weight percent, taken as the coke-free, dry catalyst.

Claim 10

The process of claim 1 wherein said catalyst after completion of step (a) is saturated with halide.

Claim 11

The process of claim 1 wherein said agglomerated catalyst is platinum-iridium supported on alumina.

Claim 12

The process of claim 1 wherein said catalyst is platinum-iridium-rhenium supported on alumina.

Claim 13

The process of claim 1 wherein the temperatures in step (a) is in the range of about 250° to 600° C.

Claim 14

The process of claim 1 wherein said elemental halogen in step (b) in chlorine.

Claim 15

The process of claim 1 wherein said temperature in step (b) is in the range of about 450° to 600° C.

Claim 16

The process of claim 1 wherein said catalyst contains iridium oxide which is contacted with a reducing atmosphere at elevated temperature to substantially convert said iridium oxide to metallic iridium prior to or concurrently with step (a).

Claim 17

The process of claim 15 wherein said reducing atmosphere comprises hydrogen gas.

Claim 18

The process of claim 15 wherein the temperature of said contacting with said reducing atmosphere is in the range of about 250° to 600° C.

Claim 19

A process for reactivating a partially or completely decoked agglomerated platinum-iridium on alumina catalyst containing platinum and iridium oxides, comprising the steps of: (a) contacting said agglomerated catalyst with a hydrogen atmosphere at a temperature in the range of about 300° to 540° C., and a pressure of about 0.1 to 2.0 MPa, for a sufficient time to substantially reduce said oxides of platinum and iridium to the respective metals; (b) pretreating said catalyst from step (a) by contact with an elemental oxygen-free and elemental halogen-free atmosphere comprising hydrogen chloride at a temperature in the range of about 300° to 540° C. and a pressure of about 0.1 to 2.0 MPa for a sufficient time to saturate the catalyst with chloride; and (c) redispersing the metallic iridium and platinum while maintaining a saturated catalyst chloride level with an atmosphere comprising elemental chlorine and elemental oxygen in a halogen to oxygen volume ratio of about 0.05 to 10 at a temperature in the range of about 500° to 540° C., a pressure of about 0.1 to 2.0 MPa, at a halogen mass flow rate of about 0.05 to 0.1 gram halogen per 100 grams catalyst per hour, for a total halogen amount of up to 0.5 gram halogen per 100 grams catalyst, for a sufficient time to effect about 75 to 100 percent redispersion of both metallic platinum and iridium.

Claim 20

A process for reactivating a partially or completely decoked agglomerated platinum-iridium on alumina catalyst containing platinum and iridium oxides, comprising the steps of: (a) contacting said agglomerated catalyst with a hydrogen atmosphere at a temperature in the range of about 300° to 540° C., and a pressure of about 0.1 to 2.0 MPa, for a sufficient time to substantially reduce said oxides of platinum and iridium to the respective metals; (b) pretreating said catalyst from step (a) by contact with an elemental oxygen-free and elemental halogen-free atmosphere comprising hydrogen chloride at a temperature in the range of about 300° to 540° C. and a pressure of about 0.1 to 2.0 MPa for a sufficient time to saturate the catalyst with chloride; and (c) redispersing the metallic iridium and platinum while maintaining a saturated catalyst chloride level with an atmosphere comprising elemental chlorine and elemental oxygen in a halogen to oxygen volume ratio of about 0.05 to 10 at a temperature in the range of about 500° to 540° C., a pressure of about 0.1 to 2.0 MPa, at a halogen mass flow rate of about 0.05 to 0.1 gram halogen per 100 grams catalyst per hour, for a total halogen amount of up to 0.5 gram halogen per 100 grams catalyst, for a sufficient time to effect about 75 to 100 percent redispersion of both metallic platinum and iridium.