US 3,939,061 AGranted

Process for reactivation of iridium-containing catalysts

AssigneeExxon Research & Engineering Co.

InventorsJohn D. Paynter, Richard R. Cecil

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Abstract

A process for reactivating a catalyst comprising iridium, or iridium as a component of a multimetallic combination, particularly one which includes both iridium and platinum admixed one with the other, and with other metal components, and halogen, composited with a refractory porous inorganic oxide, previously inactivated by coke deposition thereon, possible loss of halogen content and agglomeration of the metal, or metals, or oxides thereof, such as occurs in a reforming process wherein such catalyst is contacted with a hydrocarbon feed at reforming conditions, and subsequently regenerated by burning accumulated coke deposits therefrom. A bed of the coke-depleted catalyst, wherein up to about 70 weight percent of the iridium of the catalyst is present as agglomerates of crystallite sizes greater than about 50A, is contacted in a plurality of cycles, an initial cycle of which includes, in sequence, (i) reduction of the coke-depleted catalyst, as by contact thereof with a stream of reducing gas, e.g., hydrogen or hydrogen-containing gas, at temperature sufficient to reduce the said iridium component, or the iridium component in admixture with other components, and (ii) contact of the reduced catalyst, up to or not significantly beyond the time of halogen breakthrough, with a halogen, or halogen precursor, in the presence of insignificant concentrations of added molecular oxygen, if any, at temperature sufficient to redisperse the agglomerates, and subsequent cycles of which include, in sequence, reduction as defined in step (i), supra, and halogenation as defined in step (ii), supra, whether or not molecular oxygen is added.

Claims22

Dependent claims

In a process for the catalytic conversion of hydrocarbons wherein a hydrocarbon feedstock is contacted with a reforming catalyst comprising an iridium hydrogenation-dehydrogenation component composited with a refractory porous inorganic oxide support at conversion conditions, the catalyst having been at least partially deactivated during contact with said feedstock by the deposition of coke deposits thereon, a method for reactivating said catalyst after discontinuing contact of said catalyst with said feedstock comprising:

a. contacting a bed of said catalyst in a reaction zone with a gaseous mixture containing oxygen at an elevated temperature for a time sufficient to burn at least a substantial portion of said coke deposits therefrom, the duration of said contacting at said elevated temperature being insufficient to convert more than about 70 weight percent of the iridium on said catalyst to agglomerates having crystallite sizes greater than about 50A;
b. contacting a bed of said coke depleted catalyst without subsequent contact with a substantially halogen-free, oxygen-containing gas at temperature sufficient to agglomerate further the iridium on said catalyst, in a plurality of cycles, an initial cycle of which includes the steps of
i. contacting said coke depleted catalyst in a reaction zone with hydrogen or hydrogen-containing gas at an elevated temperature for a time sufficient to reduce a substantial portion of said iridium on said catalyst to its metallic form;
(ii) contacting said reduced catalyst having a substantial portion of the iridium contained thereon in the metallic form in a reaction zone with a substantially oxygen-free, halogen-containing gas at a temperature of at least about 850.degree.F., continuing said contacting not substantially beyond the point of halogen breakthrough from the exit side of the bed of said catalyst;
and one or more subsequent cycles which includes the steps of
iii. contacting said halogen-treated catalyst in a reaction zone with a hydrogen or hydrogen-containing gas at an elevated temperature for a time sufficient to convert a substantial portion of said iridium on said catalyst to its metallic form;
and then
iv. contacting said catalyst having a substantial portion of the iridium contained thereon in the metallic form in a reaction zone with a halogen-containing gas at a temperature of at least about 850.degree.F., continuing said contacting not substantially beyond the point of halogen breakthrough from the exit side of the bed of said catalyst.

5 more elements

In a process for the catalytic reforming of hydrocarbons wherein a hydrocarbon feedstock is contacted with a reforming catalyst comprising an iridium hydrogenation dehydrogenation component composited with an alumina support at reforming conditions, the catalyst having been at least partially deactivated during contact with said feedstock by the deposition of coke deposits thereon, a method for reactivating said catalyst after discontinuing contact of said catalyst with said feedstock comprising:

a. contacting a bed of said catalyst in a reaction zone with a gaseous mixture containing oxygen at partial pressures of at least about 0.1 psi at temperatures ranging from 575.degree.F. to about 850.degree.F. for a period ranging from about 0.1 to about 48 hours to burn at least a substantial portion of said coke deposits therefrom, the duration of said contacting at said elevated temperature being insufficient to convert more than about 70 weight percent of the iridium component of said catalyst to agglomerates having crystallite sizes greater than about 50A;
b. contacting a bed of said coke depleted catalyst, without subsequent contacting with a substantially halogen-free, oxygen-containing gas at temperature sufficient to reagglomerate the iridium on said catalyst in a plurality of cycles, an initial cycle of which includes the steps of
i. contacting said coke depleted catalyst in a reaction zone with hydrogen or a hydrogen-containing gas at temperature ranging from about 400.degree.F. to about 1100.degree.F. to reduce a substantial portion of said iridium component of said catalyst to its metallic form;
ii. contacting said reduced catalyst having a substantial portion of the iridium contained thereon in the metallic form in a reaction zone with a substantially oxygen-free gas which contains halogen in concentration ranging from about 0.01 mole percent to about 10 mole percent at a temperature of at least about 850.degree.F., continuing said contacting not substantially beyond the point of halogen breakthrough from the exit side of the bed of said catalyst;
and one or more subsequent cycles which includes
iii. contacting said halogen-treated catalyst in a reaction zone with a hydrogen or a hydrogen-containing gas at temperature ranging from about 400.degree.F. to about 1100.degree.F. for time sufficient to convert a substantial portion of said iridium component of said catalyst to its metallic form;
and then
iv. contacting said catalyst having a substantial portion of the iridium contained thereon in the metallic form in a reaction zone with a gas which contains halogen in concentration ranging from about 0.01 mole percent to about 10 mole percent at a temperature of at least about 850.degree.F., continuing said contacting not substantially beyond the point of halogen breakthrough from the exit side of the bed of said catalyst.

5 more elements

Dependencies are inferred from the claim text.