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  Treatment of crude oil fractions, fossil fuels, and products thereof with sonic energyUSPTO Application #: 20060157339Title: Treatment of crude oil fractions, fossil fuels, and products thereof with sonic energy Abstract: In crude oil fractions, fossil fuels, and organic liquids in general in which it is desirable to reduce the levels of sulfur-containing and nitrogen-containing components, the process reduces the level of these compounds via the application of sonic energy. The process can be performed both with and without the added presence of an oxidizing agent, and with or without elevated temperature and/or pressure. The invention is performed either as a continuous process or a batch process. (end of abstract) Agent: Stetina Brunda Garred & Brucker - Aliso Viejo, CA, US Inventor: Mark Cullen USPTO Applicaton #: 20060157339 - Class: 204157620 (USPTO) Related Patent Categories: Chemistry: Electrical And Wave Energy, Non-distilling Bottoms Treatment, Processes Of Treating Materials By Wave Energy, Process Or Preparing Desired Organic Product Containing At Least One Atom Other Than Carbon And Hydrogen, Using Sonic Or Ultrasonic Energy The Patent Description & Claims data below is from USPTO Patent Application 20060157339. Brief Patent Description - Full Patent Description - Patent Application Claims
CROSS-REFERENCE TO RELATED APPLICATIONS [0001] The present application is a continuation-in-part of pending United. States application Ser. No. 09/853,127, filed by Gunnerman et al., entitled A TREATMENT OF CRUDE OIL FRACTIONS, FOSSIL FUELS, AND PRODUCTS THEREOF WITH ULTRASOUND, the teachings of which are expressly incorporated herein by reference. STATEMENT RE: FEDERALLY SPONSORED RESEARCH/DEVELOPMENT [0002] Not Applicable BACKGROUND OF THE INVENTION [0003] 1. Field of the Invention [0004] This invention resides in the field of chemical processes for the treatment of crude oil fractions and the various types of products derived and obtained from these sources. In particular, this invention addresses reformation processes as ring-opening reactions and the saturation of double bonds, to upgrade fossil fuels and convert organic products to forms that will improve their performance and expand their utility. This invention also resides in the removal of sulfur-containing compounds, nitrogen-containing compounds, and other undesirable components from petroleum and petroleum-based fuels. [0005] 2. Description of the Prior Art [0006] Fossil fuels are the largest and most widely used source of power in the world, offering high efficiency, proven performance, and relatively low prices. There are many different types of fossil fuels, ranging from petroleum fractions to coal, tar sands, and shale oil, with uses ranging from consumer uses such as automotive engines and home heating to commercial uses such as boilers, furnaces, smelting units, and power plants. [0007] Fossil fuels and other crude oil fractions and products derived from natural sources contain a vast array of hydrocarbons differing widely in molecular weight, boiling and melting points, reactivity, and ease of processing. Many industrial processes have been developed to upgrade these materials by removing, diluting, or converting the heavier components or those that tend to polymerize or otherwise solidify, notably the olefins, aromatics, and fused-ring compounds such as naphthalenes, indanes and indenes, anthracenes, and phenanthracenes. A common means of effecting the conversion of these compounds is saturation by hydrogenation across double bonds. [0008] For fossil fuels in particular, a growing concern is the need to remove sulfur compounds. Sulfur from sulfur compounds causes corrosion in pipeline, pumping, and refining equipment, the poisoning of catalysts used in the refining and combustion of fossil fuels, and the premature failure of combustion engines. Sulfur poisons the catalytic converters used in diesel-powered trucks and buses to control the emissions of oxides of nitrogen (NO.sub.x). Sulfur also causes an increase in particulate (soot) emissions from trucks and buses by degrading the soot traps used on these vehicles. The burning of sulfur-containing fuel produces sulfur dioxide which enters the atmosphere as acid rain, inflicting harm on agriculture and wildlife, and causing hazards to human health. [0009] The Clean Air Act of 1064 and its various amendments have imposed sulfur emission standards that are difficult and expensive to meet. Pursuant to the Act, the United States Environmental Protection Agency has set an upper limit of 15 parts per million by weight (ppmw) on the sulfur content of diesel fuel, effective in mid-2006. This is a severs reduction from the standard of 500 ppmw in effect in the year 2000. For reformulated gasoline, the standard of 300 ppmw in the year 2000 has been lowered to 30 ppmw, effective Jan. 1, 2004. Similar changes have been enacted in the European Union, which will enforce a limit of 50 ppmw sulfur for both gasoline and diesel fuel in the year 2005. The treatment of fuels to achieve sulfur emissions low enough to meet these requirements is difficult and expensive, and the increase in fuel prices that this causes will have a major influence on the world economy. [0010] The principal method of fossil fuel desulfurization in the prior art is hydrodesulfurization, i.e., the reaction between the fossil fuel and hydrogen gas at elevated temperature and pressure in the presence of a catalyst. This causes the reduction of organic sulfur to gaseous H.sub.2S, which is then oxidized to elemental sulfur by the Claus process. A considerable amount of unreacted H.sub.2S remains however, with its attendant health hazards. A further limitation of hydrodesulfurization is that it is not equally effective in removing all sulfur-bearing compounds. Mercaptans, thioethers, and disulfides, for example, are easily broken down and removed by the process, while aromatic sulfur compounds, cyclic sulfur compounds, and condensed multicyclic sulfur compounds are less responsive to the process. Thiophene, benzothiophene, dibenzothiophene, other condensed-ring thiophenes, and substituted versions of these compounds, which account for as much as 40% of the total sulfur content of crude oils from the Middle East and 70% of the sulfur content of West Texas crude oil, are particularly refractory to hydrodesulfurization. [0011] In light of the deficiencies associated with hydrodesulfurization, new processes have emerged, the most notable being oxidative desulfurization, that seek to effectuate sulfur removal with greater efficiency. Essentially, such process involves oxidizing sulfur species that may be present, typically through the use of an oxidizing agent, such as a hydroperoxide or peracid, to thus convert the sulfur compounds to sulfones. To facilitate such oxidative reaction, ultrasound may be applied as per the teachings of U.S. Pat. No. 6,402,939 issued to Yen et al., entitled OXIDATIVE DESULFURIZATION OF FOSSIL FUELS WITH ULTRASOUND; and U.S. Pat. No. 6,500,219 issued to Gunnerman, entitled CONTINUOUS PROCESS FOR OXIDATIVE DESULFURIZATION OF FOSSIL FUELS WITH ULTRASOUND AND PRODUCTS THEREOF, the teachings of each are expressly incorporated herein by reference. [0012] Advantageously, oxidative desulfurization can be performed under mild temperatures and pressures, and further typically does not require hydrogen. Additionally advantageous is the fact that oxidative desulfurization requires much less in terms of capital expenditures to implement. In this respect, oxidative desulfurization can be selectively deployed to treat only a single fraction of refined petroleum, such as diesel, and can be readily integrated as a finishing process into existing refinery facilities. Perhaps most advantageous is the fact that oxidative desulfurization can substantially eliminate all sulfur species present in a given amount of crude oil such that ultra-low sulfur levels can be attained, and in particular the lower standards being set forth in various legislative requirements regarding sulfur content levels. [0013] Despite such advantages, however, oxidative desulfurization is presently ineffectual for use in large scale refining operations insofar as currently deployed oxidative desulfurization techniques only partially oxidize the sulfur species present to sulfoxides, as opposed to sulfones. In this regard, present oxidative desulfurization techniques are too ineffectual and cannot achieve sufficient oxidation necessary to implement on a large scale basis. Moreover, to the extent the sulfur species is only partially oxidized (i.e., to sulfoxide), eventual removal of the sulfur species, which is typically accomplished either through solvent extraction or absorption based upon the differential polarity of the sulfones assumed to be present through such process, fails to facilitate the removal of the sulfoxide components based upon its lesser degree of polarity (i.e., as compared to sulfones). Accordingly, substantial refinements to oxidative desulfurization must be made before such technology can be practically implemented. [0014] In addition to sulfur-bearing compounds, nitrogen-bearing compounds are also sought to be removed from fossil fuels, since these compounds tend to poison the acidic components of the hydrocracking catalysts used in the refinery. The removal of nitrogen-bearing compounds is achieved by hydrodenitrogenation, which is a hydrogen treatment performed in the presence of metal sulfide catalysts. Both hydrodesulfurization and hydrodenitrogenation require expensive catalysts as well as high temperatures (typically 400.degree. F. to 850.degree. F., which is equivalent to 204.degree. C. to 254.degree. C.) and pressures (typically 50 psi to 3,500 psi). These processes require a source of hydrogen or an on-site hydrogen production unit, which entails high capital expenditures and operating costs. In both of these processes, there is also a risk of hydrogen leaking from the reactor. [0015] As such, there exists a substantial need in the art for systems and methods that are operative to effectuate the removal of sulfur from refined fossil fuels that is substantially effective in removing virtually all of the sulfur species present in the fossil fuel that is further extremely cost effective and can be readily integrated into conventional oil refining processes. There is likewise a need in the art for such a method that is effective in removing nitrogen-containing compounds that is further cost-effective and substantially effective in removing virtually all of the nitrogen species present in such fossil fuel. Still further, there is a need for such a process that is capable of enhancing the quality of the refined fossil fuel treated thereby and that can be readily utilized in either large scale or small scale refinery operations. BRIEF SUMMARY OF THE INVENTION [0016] It has now been discovered that fossil fuels, crude oil fractions, and may of the components that are derived from these sources can undergo a variety of beneficial conversions and be upgraded in a variety of ways by a process that applies sonic energy to these materials in a reaction medium. The organic material is combined with an aqueous phase to form an emulsion, placing the phases in intimate contact during the exposure to sonic energy. Hydrogen gas is not required, nor are the high temperature and pressure that are commonly needed for hydrogenations of the prior art. In certain embodiments of the invention, the treatment with sonic energy is performed in the presence of a hydroperoxide, and in certain embodiments as well, a transition metal catalyst is used. One of the surprising discoveries associated with certain embodiments of this invention, however, is that the conversions achieved by this invention can be achieved without the inclusion of a hydroperoxide in the reaction mixture. [0017] Included among the conversions achieved by the present invention are the removal of organic sulfur compounds, the removal of organic nitrogen compounds, the saturation of double bonds and aromatic rings, and the opening of rings in fused-ring structures. The invention thus resides in part in the process of using sonic energy to achieve these conversions. The invention further resided in processes for converting aromatics to cycloparaffins, and opening one or more rings in a fused-ring structure, thereby for example converting naphthalenes to monocyclic aromatics, anthracenes to naphthalenes, fused heterocyclic rings such as benzothiophenes, dibenzothiophenes, benzofurans, quinolines, indoles, and the like to substituted benzenes, acenaphthalenes and acenaphthenes to indanes and indenes, and monocyclic aromatics to noncyclic structures. Further still, the invention resides in processes for converting olefins to paraffins, and in processes for breaking carbon-carbon bonds, carbon-sulfur bonds, carbon-metal bonds, and carbon-nitrogen bonds. [0018] In addition to the foregoing, API gravities of fossil fuels and crude oil fractions are raised (i.e., the densities lowered) as a result of treatments in accordance with the invention. Moreover, the invention raises the cetane index of petroleum fractions and cracking products whose boiling points or ranges are in the diesel range. The term "diesel range" is used herein in the industry sense to denote the portion of crude oil that distills out after naphtha, and generally within the temperature range of approximately 200.degree. C. (392.degree. F.) to 370.degree. C. (698.degree. F.). Fractions and cracking products whose boiling ranges are contained in this range, as well as those that overlap with this range to a majority extent, are included. Examples of refinery fractions and streams within the diesel range are fluid catalytic cracking (FCC) cycle oil fractions, coker distillate fractions, straight run diesel fractions, and blends. The invention also imparts other beneficial changes such as a lowering of boiling pints and a removal of components that are detrimental to the performance of the fuel and those that affect refinery processes and increase the cost of production of the fuel. Thus, for example, FCC cycle oils can be treated in accordance with the invention to sharply reduce their aromatics content. [0019] A further group of crude oil fractions for which the invention is particularly useful are gas oils, which term is used herein as it is in the petroleum industry, to denote liquid petroleum distillates that have higher boiling points than naphtha. The initial boiling point may be as low as 400.degree. F. (200.degree. C.), but the preferred boiling range is about 500.degree. F. to about 1100.degree. F. (Approximately equal to 260.degree. C. to 595.degree. C.). Examples of fractions boiling within this range are FCC slurry oil, light and heavy gas oils, so termed in view of their different boiling points, and coker gas oils. All terms in this and the preceding paragraph are used herein as they are in the petroleum art. [0020] By virtue of the conversions that occur as a result of the process of this invention, hydrocarbon streams experience changes in their cold flow properties, including their pour points, cloud points, and freezing points. Sulfur compounds, nitrogen compounds, and metal-containing compounds are also reduced, and the use of a process in accordance with this invention significantly lessens the burden on conventional processes such as hydrodesulfurization, hydro-denitrogenation, and hydrodemetallization, which can therefore be performed with greater effectiveness and efficiency. Continue reading... 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