Catalyst – solid sorbent – or support therefor: product or process – Catalyst or precursor therefor – Boron or compound containing same
Reexamination Certificate
1999-09-23
2002-09-24
Yildirim, Bekir L. (Department: 1764)
Catalyst, solid sorbent, or support therefor: product or process
Catalyst or precursor therefor
Boron or compound containing same
C502S202000, C502S334000, C502S349000, C423S279000
Reexamination Certificate
active
06455461
ABSTRACT:
FIELD OF THE INVENTION
This invention relates to a borate-containing composition which can be effective as a catalyst for hydrogenating aromatic hydrocarbons, to a process for producing the composition, and to a process for using the composition.
BACKGROUND OF THE INVENTION
In an alkylation process, complex saturated hydrocarbon molecules are formed by direct union of a saturated hydrocarbon molecule and an unsaturated hydrocarbon molecule. For example, light compounds such as isobutane and butylene are converted into heavier compounds through the control of temperature and pressure in the presence of an acid catalyst. Hydrofluoric acid is presently widely used as an alkylation catalyst.
Some undesirable aromatic compounds such as, for example, heavily substituted aromatic compounds, wherein each of the alkyl groups has about 3 to about 9 carbon atoms per alkyl group, are also produced in an alkylation process. When the alkylation products are used in household products, food-related applications, cosmetics, and lantern fuel, it is generally required that they be substantially free of any aromatic compounds. The concentration of aromatic compounds can generally be reduced to 0.03 weight % or higher by a hydrotreatment process using commercially available nickel catalysts. However, reduction of aromatic compounds to less than 0.03 weight % by such hydrotreatment has never been achieved with commercially available catalysts. Therefore, a more active catalyst is required to substantially reduce the content of aromatic compounds, especially from the heavy end of the alkylate fraction. It is also highly desirable to develop a new catalyst that can substantially reduce the concentration of the undesirable aromatic compounds.
Furthermore, sulfur or sulfur-containing compounds may be present in refining processes and potentially could be present in an alkylation process. Commercially available catalysts used in removing or reducing the aromatic compounds are normally prone to sulfur poisoning. Therefore, it appears there is an ever-increasing need to develop a catalyst which is not sensitive to sulfur or sulfur-containing compounds and still can substantially reduce the concentration of the undesirable aromatic compounds.
SUMMARY OF THE INVENTION
An object of this invention is to provide a metal borate-containing composition. Also an object of this invention is to provide a process for producing this composition. Another object of this invention is to employ this composition in a process for hydrogenating aromatic hydrocarbons which are present in a hydrocarbon-containing fluid. An advantage of the invention is that the aromatic hydrocarbons content can be substantially reduced. Other objects will become apparent from the detailed description and the appended claims.
According to a first embodiment of this invention, a composition is provided which comprises an inorganic support having incorporated therein a hydrogenation catalyst wherein the support comprises aluminum, zirconium, and borate.
According to a second embodiment of this invention, a process is provided which comprises: (1) contacting an aluminum salt, a zirconium salt, and an acidic boron compound under a condition sufficient to effect the production of a solid inorganic support material comprising aluminum, zirconium, and borate; and (2) combining the support with a hydrogenation catalyst precursor.
According to a third embodiment of this invention, a process which can be used for catalytically hydrogenating an aromatic compound with hydrogen to a more saturated hydrocarbon is provided. The process comprises contacting a hydrocarbon-containing fluid which contains an aromatic compound, in the presence of a catalyst, with hydrogen under a condition effective to substantially hydrogenate the aromatic compound to a saturated compound.
DETAILED DESCRIPTION OF THE INVENTION
According to the first embodiment of the invention, the hydrogenation catalyst of the composition of this invention can be any hydrogenation catalyst known to one skilled in the art. Preferably, such catalyst is one of the Group VIII metals, Group VIII metal-containing compounds, or combinations of two or more thereof. The term “Group VIII” refers to the Periodic Table of the Elements, CRC Handbook of Chemistry and Physics, 67th edition, 1986-1987, CRC Press, Boca Raton, Fla. The presently preferred hydrogenation catalyst is platinum or a platinum compound such as platinum oxide.
The support component of the composition of this invention comprises, consists essentially of, or consists of, aluminum, zirconium, and borate. Aluminum and zirconium in the composition are generally not in the metal form. Preferably the support material comprises, consists essentially of, or consists of aluminum borate and zirconium borate. More preferably the support material comprises, consists essentially of, or consists of a zirconium/aluminum/borate composite.
Generally, the component has a weight ratio of Al to Zr in the range of from about 0.1:1 to about 30:1, preferably about 1:1 to about 20:1, and most preferably about 4:1 to about 12:1 and a weight ratio of (Al+Zr) to B in the range of from about 0.1:1 to about 10:1, preferably about 1:1 to about 6:1, and most preferably about 1.5:1 to about 3:1. Generally, the support component has a surface area, measured by the BET method employing N
2
, of about 200 to about 400 m
2
/g and a pore volume, measured by a pore size distribution method employing N
2
, of about 0.2-1.5 cc/g. It can have any suitable shape such as spherical, cylindrical, trilobal or irregular, or combinations of two or more thereof. It also can have any suitable particle size. The presently preferred size is about 0.4 to about 0.8 mm. If particles of the support component have been compacted and extruded, the formed cylindrical extrudates generally have a diameter of about 1 to about 4 mm and a length of about 3 to about 10 mm. It is within the scope of this invention to have minor amounts of aluminum oxide and zirconium oxide, generally about 1 to about 5 weight % of each, present in the support component. The hydrogenation catalyst component of the composition can be present in the composition of this invention in any quantity as long as that quantity can effect the substantial reduction of aromatic compound concentration in the product stream of an alkylation reaction. Generally, the weight % of the hydrogenation catalyst component in the invention composition can be in the range of from about 0.01 to about 50, preferably about 0.05 to about 25, and most preferably 0.1 to 15.
Preferably, the inorganic support component is prepared by a method comprising coprecipitation. A first aqueous solution containing any water-soluble aluminum salt such as, for example, aluminum nitrate; any water-soluble zirconium salt such as, for example, zirconyl nitrate; and any water-soluble acidic boron compound (preferably a boric acid, more preferably H
3
BO
3
) is prepared. Any suitable concentrations of these compounds in the aqueous solution can be employed so long as the concentration can result in the production of the inorganic support component disclosed above. Generally about 0.02 to about 1 mole/l of each compound, depending on the desired Al:Zr:B ratio can be employed. The initial pH of this aqueous solution is generally about 1 to about 3.
An aqueous alkaline solution, preferably an aqueous solution of ammonia containing about 25 to about 28 weight % NH
3
, generally having a pH of about 10 to about 14, is then added to the first aqueous solution in an amount sufficient to raise the pH of the first solution to 7 or above 7, preferably to about 8-9, to afford the coprecipitation of borates of aluminum and zirconium.
The dispersion of the formed coprecipitate in the aqueous solution is then subjected to any suitable solid-liquid separation methods known to one skilled in the art such as, for example, filtration to substantially separate the coprecipitate from the aqueous solution. Preferably, the coprecipitate is washed with water to remove adhered solution
Anderson Jeffrey R.
Phillips Petroleum Company
Yildirim Bekir L.
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