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United States Patent (19) 11 Patent Number: 4,716,143 Imai 45 Date of Patent: Dec

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United States Patent (19) 11 Patent Number: 4,716,143 Imai 45 Date of Patent: Dec United States Patent (19) 11 Patent Number: 4,716,143 Imai 45 Date of Patent: Dec. 29, 1987 (54) DEHYDROGENATION CATALYST Primary Examiner-Asok Pal COMPOSITION Attorney, Agent, or Firm-Thomas K. McBride; John F. Spears, Jr. (75) Inventor: Tamotsu Imai, Mt. Prospect, Ill. (73) Assignee: UOP Inc., Des Plaines, Ill. 57 ABSTRACT A novel catalytic composite comprising a platinum 21 Appl. No.: 18,541 group metal component; a modifier metal component 22 Filed: Feb. 25, 1987 selected from the group consisting of a tin component, germanium component, rhenium component and mix Related U.S. Application Data tures thereof; an alkali or alkaline earth metal compo 63) Continuation-in-part of Ser. No. 871,356, Jun. 6, 1986, nent or mixtures thereof, an optional halogen compo abandoned. nent, and an optional catalytic modifier component on a (51) Int. Cl." ....................... G01J 21/04; G01J 23/58; refractory oxide support having a nominal diameter of G01J 23/62 at least about 850 microns. The distribution of the plati (52) U.S. C. .................................... 502/326; 502/327; num group metal component is such that the platinum 502/328; 502/330; 502/349; 502/352; 502/514; group component is surface-impregnated where sub 502/523: 502/527; 585/660 stantially all of the platinum group metal component is 58 Field of Search ............... 502/326, 327, 328,330, located at most within a 400 micron exterior layer of the 502/349, 352, 514,523, 527 support. The effective amount of the modifier metal component may be uniformly impregnated throughout (56. References Cited the refractory oxide support, surface-impregnated, or U.S. PATENT DOCUMENTS located in any other appropriate fashion. The distribu 3,584,060 6/1971 Rausch ................................ 585/434 tion of the surface-impregnated modifier metal compo 3,86,344 6/1974 Shimizu et al. ..................... 502/257 nent is such that the modifier metal component is sub 3,878,131 4/1975 Hayes.................................. 502/330 stantially all located at most within a 400 micron exte 3,897,368 7/1975 Ohara et al. ... 252/466 PT rior layer of the support. The novel catalyst has particu 4,082,696 4/1978 Robinson ............................ 502/327 lar utility as a hydrocarbon dehydrogenation catalyst. A 4,255,253 3/1981 Herrington et al. ... ... 502/527 4,515,905 5/1985 Uytterhoeven et al. 502/309 method of preparing the catalyst is also disclosed. 4,547,486 10/1985 Shyr ....................... 502/.333 4,595,673 6/1986 Inai et al. ........................... 502/227 10 Claims, 5 Drawing Figures U.S. Patent Dec. 29, 1987 Sheet 2 of 4 4,716,143 pºOOº.009OOZ009009OO OOO/ Y (off oy - y ) 4,716,143 1. 2 ponent are uniformly distributed throughout the surface DEHYDROGENATION CATALYST and pores of the catalyst. COMPOSITION U.S. Pat. No. 3,897,368 describes a method for the production of a noble metal catalyst where the noble CROSS-REFERENCE TO RELATED metal is platinum and the platinum is deposited selec APPLICATION tively upon the external surface of the catalyst. How ever, this disclosure describes the advantages of impreg This application is a continuation-in-part of prior nating only platinum on the exterior layer and utilizes a copending application Ser. No. 871,356 filed June 6, specific type of surfactant to achieve the surface im 1986, now abandoned, the contents of which are incor 10 pregnation of the noble metal. Surprisingly, it has been porated herein by reference thereto. discovered that by incorporating into the outer layer of BACKGROUND OF THE INVENTION the catalyst support substantially all of both a platinum This invention relates to the conversion of hydrocar group metal component and a metal component se bons, especially the dehydrogenation of dehydrogena lected from the group comprising tin, germanium, and table hydrocarbons, in the presence of a catalyst com 15 rhenium, a catalyst displaying improved performance in posite. This invention also pertains to a new catalyst a dehydrogenation process is obtained. composite and a method of making it. OBJECTS AND EMBODIMENTS The dehydrogenation of hydrocarbons is an impor It is, therefore, an object of the present invention to tant commercial process because of the great demand 20 provide an improved catalytic composite and a method for dehydrogenated hydrocarbons for the manufacture of making the same. A corollary objective is to provide of various chemical products such as detergents, high an improved process for the conversion of hydrocar octane gasolines, pharmaceutical products, plastics, bons especially for the dehydrogenation of hydrocar synthetic rubbers, and other products well known to bons. those skilled in the art. One example of this process is 25 Accordingly, in a broad embodiment, the present dehydrogenating isobutane to produce isobutylene invention is a catalytic composite comprising a platinum which can be polymerized to provide tackifying agents group metal component; a modifier metal component for adhesives, viscosity-index additives for motor oils selected from the group consisting of a tin component, and impact-resistant and anti-oxidant additives for plas germanium component, rhenium component and mix tics. 30 tures thereof; and an alkali metal component, or an alkaline earth metal component or mixtures thereof on a INFORMATION DISCLOSURE refractory oxide support having a nominal diameter of Numerous catalytic composites comprising a plati at least about 850 microns wherein the platinum group num group component and a modifier metal component component is surface-impregnated upon the refractory selected from the group consisting of a tin component, 35 oxide support where substantially all of the platinum germanium component, rhenium component, and mix group component is located within at most a 400 micron tures thereof are known. For example related U.S. Pat. wide exterior layer of the support. The effective amount Nos. 3,632,503, 3,755,481, and 3,878,131 disclose cata of the modifier metal component may be uniformly lysts comprising a platinum group component, a tin impregnated, surface-impregnated, or located in any component, and a germanium component on a porous other appropriate fashion. If the modifier metal compo carrier material. However, these references disclose nent is surface-impregnated, then substantially all of the that best results are achieved when a germanium com modifier metal component will be located within at ponent is uniformly distributed throughout the carrier most a 400 micron wide exterior layer of the support. material. However, the reference is silent as to any In an alternative embodiment, the invention is a advantage to be achieved by limiting the location of 45 method of preparing a catalytic composite comprising substantially all of the catalytic metals to an outer layer compositing a platinum group component, a modifier of the catalyst particle. In fact, it is indicated in these metal component selected from the group consisting of references that it is preferred that the catalytic compos a tin component, germanium component, rhenium com ite thereof be subjected to a substantially water-free ponent and mixtures thereof and an alkali or alkaline reduction step prior to its use in the conversion of hy 50 earth metal component on a refractory oxide support drocarbons. It is further disclosed that the step is de having a nominal diameter of at least about 850 microns signed to ensure a uniform and finely divided dispersion wherein the platinum group component is surface of metallic components throughout the carrier material. impregnated upon the refractory oxide support wherein Related U.S. Pat. Nos. 3,682,838 and 3,761,531 dis the platinum group component is substantially all lo close catalytic composites comprising a platinum group 55 cated within at most a 400 micron wide exterior layer of component, and a Group IVA metallic component. As the support and the effective amount of the modifier with the previous references it is disclosed therein that metal component may be uniformly impregnated, sur it is preferred that the catalysts are subjected to a reduc face-impregnated, or located in any other appropriate tion step prior to their use. It is further disclosed in these fashion. references that the reduction step is designed to assure In yet another embodiment, the invention is a hydro uniform distribution of the metallic particles throughout carbon conversion process comprising the steps of con the catalysts. tacting a hydrocarbon at hydrocarbon conversion con U.S. Pat. Nos. 3,558,477, 3,562,147, 3,584,060, and ditions with a catalytic composite comprising a plati 3,649,566 all disclose catalytic composites comprising a num group metal component; a modifier metal compo platinum group component, and a rhenium component 65 nent selected from the group consisting of a tin compo on a refractory oxide support. However, as before these nent, germanium component, rhenium component and references disclose that the best results are achieved mixtures thereof; and an alkali or alkaline earth metal when the platinum group component and rhenium com component on a refractory oxide support having a nom 4,716, 143 3 4. inal diameter of at least about 850 microns wherein the nent is best defined as being both surface-impregnated platinum group component is surface-impregnated and and substantially all located within at most the 400 wherein substantially all of the platinum group compo micron exterior layer of the support where "substan nent is located at most within a 400 micron wide exte tially all" is meant at least about 75% of the component. rior layer of the support and wherein the effective 5 As previously stated, the support material has a nomi amount of the modifier metal component may be either nal diameter of 850 microns. For a catalyst support uniformly impregnated, surface-impregnated, or lo material which approaches this diameter, the exterior cated in any other appropriate fashion.
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