Chemistry of hydrocarbon compounds – Aromatic compound synthesis – From nonhydrocarbon feed
Reexamination Certificate
2002-01-10
2002-12-03
Dang, Thuan D. (Department: 1754)
Chemistry of hydrocarbon compounds
Aromatic compound synthesis
From nonhydrocarbon feed
C585S408000, C585S409000
Reexamination Certificate
active
06489528
ABSTRACT:
BACKGROUND OF THE INVENTION
The present invention relates to the field of hydrocarbon upgrading processes. In another aspect, the invention relates to the conversion of oxygenated hydrocarbons to aromatics.
Developments in zeolite catalysts useful in hydrocarbon conversion processes have led to the use of zeolite catalysts for the conversion of oxygenated hydrocarbons to aromatics. The term “oxygenated hydrocarbons” as employed herein is defined to include hydrocarbons containing aliphatic moieties such as, but not limited to, alcohols, halides, mercaptans, sulfides, amines, ethers, and carbonyl compounds (aldehydes, ketones, carboxylic acids and the like) or mixtures thereof.
It is known to convert oxygenated hydrocarbons to olefins and aromatics in the presence of catalysts which contain a zeolite, as is described in U.S. Pat. No. 4,049,573. However, there are ever present incentives, including the selectivity to specific aromatics such as xylene, for the development of new, more effective and/or more practical catalyst systems and methods of preparing them.
SUMMARY OF THE INVENTION
It is an object of this invention to provide a novel hybrid catalyst system effective for converting at least a portion of a hydrocarbon feedstock comprising at least one oxygenated hydrocarbon to a reaction product comprising at least one aromatic.
It is yet another object of this invention to provide a method for making a novel hybrid catalyst system effective for converting at least a portion of a hydrocarbon feedstock comprising at least one oxygenated hydrocarbon to a reaction product comprising at least one aromatic.
Yet another object of this invention is to provide an improved process for the conversion of at least a portion of a hydrocarbon feedstock comprising at least one oxygenated hydrocarbon to a reaction product comprising at least one aromatic.
It is yet another object of this invention to provide a novel hybrid catalyst system which when used in the conversion of oxygenated hydrocarbons results in preferential production of aromatics.
A further object of this invention is to provide a novel hybrid catalyst system which when used in the conversion of oxygenated hydrocarbons results in preferential production of xylenes.
According to a first embodiment of the present invention, a catalyst system which can be used in the conversion of oxygenated hydrocarbons to aromatics is provided. The novel catalyst system comprises a first solid material comprising a silicoaluminophosphate and a second solid material comprising a zeolite, a zinc component and a metal selected from the group consisting of Group IIIA and Group VIB of the CAS version of the Periodic Table of the Elements, Hawley's Condensed Chemical Dictionary, 11th edition and combinations of any two or more thereof.
According to a second embodiment of the present invention, a method is provided for preparing a catalyst system, which can be used in the conversion of oxygenated hydrocarbons to aromatics, comprising blending the first solid material and the second solid material from the first embodiment.
According to a third embodiment of the present invention, a method is provided for preparing a catalyst system, which can be used in the conversion of oxygenated hydrocarbons to aromatics, comprising placing the first solid material from the first embodiment into a contacting vessel and placing the second solid material from the first embodiment into the contacting vessel such that a hydrocarbon feedstock comprising at least one oxygenated hydrocarbon charged to the contacting vessel contacts the first solid material prior to contacting the second solid material.
According to a fourth embodiment of the present invention, a method is provided for preparing a catalyst system, which can be used in the conversion of oxygenated hydrocarbons to aromatics, comprising placing the first solid material from the first embodiment into a first contacting vessel, placing the second solid material from the first embodiment into a second contacting vessel, and operating the catalyst system such that a hydrocarbon feedstock comprising at least one oxygenated hydrocarbon charged to the catalyst system contacts the first solid material prior to contacting the second solid material.
According to a fifth embodiment of the present invention, a process is provided for the conversion of at least a portion of a hydrocarbon feedstock comprising at least one oxygenated hydrocarbon to aromatics by contacting under conversion conditions the hydrocarbon feedstock with the novel catalyst system of the first embodiment prepared by the method of the second, third or fourth embodiment.
Other objects and advantages of the invention will become apparent from the detailed description and the appended claims.
DETAILED DESCRIPTION OF THE INVENTION
According to the first embodiment of the present invention the inventive catalyst system can comprise, consist essentially of, or consist of a first solid material comprising a catalytically effective amount of a silicoaluminophosphate (SAPO) and a second solid material comprising a catalytically effective amount of a zeolite, a catalytically effective amount of a zinc component and a catalytically effective amount of a metal selected from the group consisting of Group IIIA and Group VIB, and combinations of any two or more thereof.
The SAPO material used in preparing the first solid material can be any SAPO that, when used in conjunction with a zeolite material, is effective in the conversion of oxygenated hydrocarbons to aromatics.
SAPO materials exhibit properties of both aluminosilicate zeolites and aluminophosphates. The SAPO's have a three-dimensional microporous crystal framework structure comprising PO
2
, AlO
2
and SiO
2
tetrahedral units. The chemical composition (anhydrous) is:
mR:(Si
x
Al
y
P
z
)O
2
wherein “R” represents at least one organic templating agent present in the intracrystalline pore system: “m” represents the moles of “R” present per mole of (Si
x
Al
y
P
z
)O
2
and has a value of from zero to 0.3, the maximum value in each case depending upon the molecular dimensions of the templating agent and the available void volume of the pore system of the particular SAPO species involved, and “x”, “y” and “z” represent the mole fractions of silicon, aluminum and phosphorus, respectively.
Examples of such templating agents include, but are not limited to, tetramethylammonium hydroxide, tetraethylammonium hydroxide, and tetrapropylammonium hydroxide. Further details relating to the formation of SAPO compositions, including molar amounts of each oxide source, can be found in the Lok et al. U.S. Pat. No.4,440,871, the entire disclosure of which is expressly incorporated herein by reference.
SAPO compositions useful in the present invention include, but are not limited to, SAPO-4, SAPO-5, SAPO-11, SAPO-16, SAPO-17, SAPO-20, SAPO-31, SAPO-34, SAPO-35, SAPO-37, SAPO-40, SAPO-41, SAPO-42, and SAPO-44, described in Lok et al. referenced above. The presently more preferred SAPO is SAPO-34.
The SAPO can be combined or mixed with a binder material in a liquid such as water or a hydrocarbon, by any means known to one skilled in the art such as stirring, blending or kneading following which the resulting mixture can be extruded into pellets or tablets by any method known to those skilled in the art. The mixture can then be dried in air at a temperature in the range of from about 20° C. to about 125° C., for a time period in the range of from about 0.5 hour to about 4 hours under any pressures that accommodate the temperatures, preferably atmospheric pressure.
Any binders known to one skilled in the art for use with a SAPO are suitable for use herein. Examples of suitable binders include, but are not limited to, aluminas such as for example &agr;-alumina and &ggr;-alumina; silicas; alumina-silica; aluminum phosphate; aluminum chlorohydrate; clays such as kaolinite, halloysite, vermiculite, chlorite, attapulgite, smectite, montmorillonite, illite, saconite, sepiolite, palygorskite, and combinations of any tw
Drake Charles A.
Wu An-hsiang
Dang Thuan D.
Lee Michael E.
Phillips Petroleum Company
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