Alkylation bimetallic catalysts

FIELD: process engineering.

SUBSTANCE: invention relates to alkylation catalysts. Particularly, it relates to solid acid catalyst to be used in paraffin's alkylation by olefins that comprises: (a) zeolite selected from the group including zeolite X, zeolite Y, ZSM-20, EMT and combination thereof; (b) multimetallic material added to zeolite wherein, at least, one metal is Pt or Pd, and, at least, second metal is Ni, Co, Mn, Cr, V, Ti, Fe, or Cu. Catalyst comprising above described components additionally includes binder selected from the group consisting of aluminium oxides, silicon oxides, silicon-aluminium oxides, zirconium oxides and clays. Invention covers also the method of alkylation of paraffin by olefins that comprises the following stages: (a) using above described solid acid catalyst and (b) mixing one or more alkylation paraffins with one or more alkylation reagents, olefins, in the presence of said catalyst in conditions bringing about alkylation to produce alkylation products and catalyst regeneration in H2 conditions.

EFFECT: new active catalyst for paraffins alkylation by olefins that features longer life.

16 cl, 14 dwg, 25 ex

 

The present application under §119(e) of Section 35 of the Code of laws of the United States claims the benefit of Provisional Patent Application No. 60/852380, filed October 17, 2006, which is shown here for information.

The technical FIELD TO WHICH the INVENTION RELATES.

The present invention relates to a solid acid catalysts for use in alkylation processes. Solid acid catalyst includes multimetallic (for example, bi-metal, tri-metal or tetramethylene) component, which produces a hydrogenating action to reactivate (or regenerated) catalyst in the presence of hydrogen. The invention also relates to processes of alkylation using a solid acid catalyst having multimetallic component for hydrogenation.

The LEVEL of TECHNOLOGY

"Alkylation" in General relates to the reaction of a hydrocarbon such as an aromatic or a saturated hydrocarbon with olefin. For example, in one type of reaction is of particular interest, branched saturated hydrocarbon, such as isobutane, may be subjected to alkylation of an olefin containing 2 to 6 carbon atoms, such as 2-butene, with the formation of alkylate, which has a higher octane number and which boils in the temperature range of the boiling gasoline fraction. In% SSH, directed to the alkylation of paraffins with olefins, the resulting molecule is branched hydrocarbons for gasoline components, such as isomers of octane, for example trimethylpentane (“TMP”), which are high octane number. Gasoline with a high octane number, often expressed as the octane number of gasoline by the research method (“RON”), can reduce detonation in the engine, than reduced the need to add harmful to the environment antiknock compounds, such as tetraethyl lead. The second octane indicator, motor octane number ("OCM", "MON"), also describes the anti-knock properties of gasoline. Motor octane number (MON) is measured when the test engine is running with high load (high speed), and the octane number of gasoline by the research method (RON) measured at low load (low speed).

The gasoline produced in the alkylation process, essentially does not contain impurities such as sulfur and nitrogen, which may be present in gasoline produced in other ways, such as the cracking of heavy oil fractions, for example, vacuum gas oil and the products of atmospheric distillation. Sulfur oxides (“SOx”), the product of combustion, are a primary cause of pollution. In addition to direct emissions of oxides with the market (SOx) sulfur oxides (SOx) can significantly reduce the performance of catalytic converters, thereby impairing the efficiency of absorption of emissions of sulphur oxides (SOx), nitrogen oxides (NOx) and carbon monoxide (CO). Sulphur oxides (SOx) are also involved in the formation of indirect particles - a combination of water and sulfur oxides (SOx) with the formation of sulphurous and sulphuric acids. These indirect contamination particles, which are usually in the 1-10 micron range, are the "respirable"particles, which have a deleterious effect on health, especially those people who suffer from asthma or emphysema. In addition, unlike gasoline, obtained by reforming naphtha or cracking of heavy oil fractions, the alkylate contains very little aromatic compounds or olefins or even without them. Aromatic compounds, particularly benzene, toxic, and olefins which are reactive in the photochemical reactions that form ozone and smog.

The alkylation reaction is kislotosoderjasimi. In alkylation processes typically used liquid acid catalysts such as sulfuric acid or hydrofluoric (HF) acid. The use of liquid acid catalysts has several shortcomings. Used liquid acids are vysokokorrozivnuyu, requiring the use of more expensive equipment special quality. Because the presence of these the acid in the final fuel is undesirable, any acid remaining in the alkylate, should be removed. This process is complicated and expensive. In addition, liquid acid, particularly hydrofluoric (HF) acid, dangerous when released into the environment.

To resolve these and other disadvantages of liquid acid catalysts, for use in alkylation processes were developed solid acid catalysts. In the solid catalysts are usually used solid acid catalyst and a metal, which performs the function of hydrogenation. For example, U.S. Patent No. 6855856 describes a catalyst comprising a solid acid, such as zeolite, and the execution of the function hydrogenation. Described solid acid has a specific range for the relationship of the pore volume of the catalyst to the specific length of the catalytic particles.

The lack of solid acid catalysts that are used in the prototypes, is that the catalyst can be quickly decontaminated due to the formation polyalkylated (for example, products C12+), which inhibit alkylation reaction is in some respects like a very soft coke. Once the catalyst will generate a certain level of content polyalkylated, the catalyst is essentially stops alkylation reaction. In the reactor with a fixed bed, often predpochtitel the second design, you can watch de-activated, which occurs as a stripe aging, area decontamination moving in the form of a strip through the layer up until most layer is not deactivated. This deactivation of the catalyst leads to the need for periodic regeneration of the catalyst to ensure a satisfactory yield of the desired product produced in the process. Regeneration of the catalyst usually requires stopping the alkylation at a certain period of time. This reduces productivity and increases costs in the alkylation process, in particular due to the reduction of "operational" factor of the process.

The preferred method of regeneration of the catalyst is a hydrogenation. Hydrogenating action is usually provided by the metal of Group VIII of the Periodic table of elements, in particular noble metals such as platinum (Pt) or palladium (Pd). In contrast to the classical bifunctional (metal/acid) hydrogenating catalyst effect plays a minor or indirect role in the alkylation reactions. On the contrary, it plays a crucial role in the effective reactivation by hydrogen (H2) (also referred to here as "regeneration") of the deactivated catalyst. Hydrogenating action is important in both the following regenerations, as for the so-called bottom of temperaturey (“low T”), and high-temperature (high-T) regeneration.

Made various attempts to develop improved solid acid catalysts. For example, the Patent Publication U.S. No. 2004/0162454 describes the alkylation catalyst comprising nanocrystalline zeolite Y and metal for hydrogenation. The pore size of the nanocrystalline zeolite Y ensures alkylate with higher values of octane number of gasoline on the research method and the motor octane number (RON/MON), as well as longer term catalyst. The catalyst based on nanocrystalline zeolite Y also includes a metal of Group VIII of the Periodic table of elements, such as platinum (Pt) or palladium (Pd), for performing the functions of hydrogenation.

To improve the effectiveness and efficiency of alkylation process using solid acid catalysts have been developed various methods of improving the process of regeneration of the solid acid catalysts. For example, U.S. Patent No. 7176340 describes a continuous process for the alkylation using, in General, at least four reactors containing the catalyst. However, the use of multiple reactors increases the cost of the process; this increased cost may be offset, at least partly, is by improving the overall efficiency of the overall process. U.S. patent No. 5986158 describes an alkylation process in which the catalyst is periodically subjected to the processing in the stage of regeneration by contact with a raw material containing a saturated hydrocarbon and hydrogen, and the regeneration is carried out at 90%or less passing the active catalytic cycle. While these methods of regeneration improve the overall efficiency of the alkylation process, relatively large amounts are needed for this solid acid catalysts and associated with these noble metals can be a problem, which makes the process of alkylation economically unacceptable.

It would be desirable to have a solid acid catalyst for the alkylation, which ensures a long service life before decontamination. It would also be desirable to have a solid acid catalyst, which uses metal for performing hydrogenation, which produces equal or superior action compared with platinum (Pt) or palladium (Pd) and which can be available at a low price. The present invention overcomes one or more of these and other disadvantages or difficulties caused by the use of solid acid catalysts in alkylation processes according to the prototypes.

The INVENTION

This isobuteneisoprene on solid acid catalysts for the alkylation of paraffins with olefins and the use of solid acid catalysts in the alkylation process. Solid acid catalyst includes zeolite and moisturizing action. The zeolite can be any zeolite, known qualified specialists in this field of technology for use in solid acid catalysts for alkylation processes. In a preferred embodiment, in the solid acid catalyst can be applied zeolites having the structure of tasita (faujasite). Extended family poasito may include varieties X, Y, ZSM-20 and EMT. In order to illustrate the present invention description of the preferred embodiments will focus on zeolite Y (including Y, ultrastable (with respect - “USY”, that is, having the size of the unit cell 24,50 Å or less (24,5×10-10m), zeolite X and combinations of zeolites X and Y.

Hydrogenating action often preferably provided bi-metal or tri-metal component. Traditionally, bi-metal or tri-metal component should include a variety of noble metals such as platinum (Pt) or palladium (Pd), in such combinations, as, for example, PtNi, PtCo, PtAg, PtAu, PtPdNi, PtPdAg, PtPdAu, PdNi, PdAg and PdAu. We also used a combination of platinum (Pt) or palladium (Pd) with ruthenium (Ru), iridium (Ir), rhodium (Rh), copper (Cu) and rhenium (Re). In some examples, can be used tetramethylene system (for example, PtPdAgAu or PtNiReIrAu).

Us is Aasee invention represents a real departure from the traditional use of catalysts based on noble metals. In the catalysts according to the present invention the effective function of the hydrogenation takes a combination of platinum (Pt) and at least one 3d-metals (i.e. Nickel (Ni), cobalt (Co), manganese (Mn), chromium (Cr), vanadium (V), iron (Fe) or titanium (Ti)). The authors of the present invention have found that a synergistic combination can provide excellent regeneration at lower levels of platinum (Pt) or palladium (Pd). This structure can reduce the total cost of the catalyst and to facilitate waste disposal. In one embodiment, the new catalyst can include one or two 3d metal together with one or two noble metals, provided that one noble metal is platinum (Pt) or palladium (Pd). In yet another embodiment, the catalyst includes platinum (Pt) or palladium (Pd) and three 3d-metal.

Optional solid acid catalytic component may include a matrix material such as alumina, silica, silica-alumina, zirconium oxide, clay or combinations thereof.

The catalyst may be used in the process of alkylation of paraffin-olefin, such as alkylation of isobutane with butylene (preferably 2-butene)to form a gasoline product having a high value of the octane number of gasoline by research is the method (RON) and motor octane number (MON).

One advantage of solid acid catalysts according to the present invention is that they include multimetallic materials that are less expensive than catalysts having only platinum (Pt) or palladium (Pd), at the same time providing equivalent or superior regeneration action. Other advantages of the present invention will be apparent by qualified professionals in this field of technology from the detailed description of preferred embodiments set forth below.

BRIEF DESCRIPTION of DRAWINGS

Figure 1 is a schematic drawing of the reactor system used in the processes described in Examples 8-14.

Figure 2 is a graph showing the breakthrough time of the olefin to the catalysts of examples 1 to 7 used in the processes of Examples 8-14.

Figure 3 is a chart summarizing the experimental techniques used in the procedures coking and regeneration of hydrogen (H2in the examples.

Figure 4 presents a table summarizing the characteristic absorption bands of vibrational spectra of coke and coke precursors.

Figure 5 represents a graph of the chemisorption of carbon monoxide (CO) on "sakakawea" USY catalyst (ultrastable (with respect to the Y-zeolite) to 0.35 wt%. platinum (Pt).

6 is a graph showing the s the formation of a "coke" on USY catalyst to 0.35 wt%. platinum (Pt).

Fig.7 is a graph showing the regeneration of hydrogen (H2) USY-catalyst to 0.35 wt%. platinum (Pt).

Fig is a graph showing the formation of a "coke" on USY catalyst with 0,105% weight. Nickel (Ni) and 0.35 wt%. platinum (Pt).

Fig.9 is a graph showing the regeneration of hydrogen (H2) USY-catalyst with 0,105% weight. Nickel (Ni) and 0.35 wt%. platinum (Pt).

Figure 10 is a graph showing the formation of a "coke" on USY catalyst with 0,105% weight. Nickel (Ni) and 0.12 wt%. platinum (Pt).

11 is a graph showing the regeneration of hydrogen (H2) USY-catalyst with 0,105% weight. Nickel (Ni) and 0.12 wt%. platinum (Pt).

Fig is a graph showing the chemisorption capacity for carbon monoxide (CO) at different catalysts after 60 minutes coking.

Fig is a graph showing the chemisorption capacity for carbon monoxide (CO) at different catalysts after 100 minutes of regeneration.

Fig is a graph showing the chemisorption capacity for carbon monoxide (CO) catalysts 0.15% weight. platinum (Pt), of 0.12 wt%. platinum (Pt) and 0.11 wt%. cobalt (Co) and 0.12 wt%. platinum (Pt) and 0.10 wt%. Nickel (Ni).

A DETAILED DESCRIPTION of the PREFERRED embodiments

The present invention relates to a catalyst for the application of the processes of alkylation of paraffin (for example, isobutane) olefin (for example, 2-butene) to obtain gasoline product. The catalyst comprises a solid acid zeolite and moisturizing action. The catalyst can also include a matrix or binder material. Hydrogenating action is provided multimetallic component, preferably bi-metal or tri-metal component, which is implemented mainly in the structure of the zeolite. However, the invention is not limited in this respect and a certain amount mentioned hydrogenating steps may be executed by a bonding material, and the outer surface of the zeolite. In the following description of preferred embodiments, in General, uses the term "bimetallic" in the description of the catalyst, but it should be understood that the invention is not limited to the use of the composite material and that any multimetallic material or combination multimetallic materials that provide moisturizing effect, can be introduced in solid acid catalyst.

In the technique for use in alkylation processes known to many solid acid zeolites. In the present invention any of these zeolites can be used as a solid acid catalyst. The preferred zeolite for use in the present invention is t is of Olite, with the structure poasito, such as zeolite Y or zeolite X. In an especially preferred zeolite Y. In a particularly preferred embodiment is applied nanocrystalline zeolite Y, such as nanocrystalline zeolite Y is described in U.S. Patent No. 6793911, and in the Patent Publications of the United States No. 2004/0162454 listed here for information.

As described in the Patent Publications of the United States No. 2004/0162454, nanocrystalline zeolite Y is primary when used in the alkylation process. Zeolite has the crystal size of the unit cell is not more than about 100 nanometers (nm). The maximum diffusion distance of many reactants and, more importantly, the products are limited. Coking and related deactivation of the catalyst is reduced by providing the possibility that 1) preferred8products leaving the catalyst to flow subsequent alkylation reactions, i.e. the formation of heavier products C12+, and 2) the coke precursors (e.g., heavier products C12+) leave the catalyst before you undergo retrogressive reactions of condensation. Catalysts based on nanocrystalline zeolite Y also exhibit higher activity than zeolite catalysts having larger crystal elementary is haunted cell, improved efficiency ratio.

Hydrogenating action in solid acid catalysts are preferably provided catalytically active bi-metal or tri-metal component. Bi-metal or tri-metal component preferably includes at least one metal from Group VIII of the Periodic Table of elements. Preferred multimetallic components, which include platinum (Pt) or palladium (Pd) as one of the metals, such as PtNi, PtCo, PtAg, PtAu, PdNi, PdAg and PdAu, or PtPdNi, PtPdAg, PtPdAu. Can also be used a combination of platinum (Pt) or palladium (Pd) with ruthenium (Ru), iridium (Ir), rhodium (Rh), copper (Cu) and rhenium (Re). The invention is not limited in this respect and may be applied to any multimetallic (especially bi-metal and tri-metal) component, which will provide hydrogenating action in the alkylation reaction. For example, metals of Group VIB, including, for example, molybdenum (Mo) and vanadium (V), can be used in multimetallic component and can be applied multimetallic materials that do not include platinum (Pt)or palladium (Pd), such as a combination TiNiHf.

Multimetallic (especially bi-metal or tri-metal) component is introduced into the zeolite by using obseo potrebitelny ways known for well-qualified specialists in this field of technology, such as ion exchange, impregnation of the zeolite or the introduction of multimetallic material in the synthetic material from which made the zeolite. The preferred method of implementation multimetallic material is ion exchange. Because zeolites are highly selective, to enhance absorption multimetallic component can be selected salt multimetall. For example, tetrammine salts (e.g. chlorides, nitrates or hydroxides) multimetallic can be prepared and used for the introduction of bimetallic component in the zeolite. Multimetall can also be entered using a consistent process, sometimes referred to as "double dipping," in which the zeolite is treated with a salt solution with subsequent drying and calcification for fixing multimetall in the zeolite, and the process is repeated until the zeolite is not entered the desired number of multimetall.

Solid acid catalyst preferably contains from about 0.01 wt%. up to about 2.0 wt%. multimetallic (for example, bi-metal or tri-metal) component, more preferably contains from about 0.02% weight. up to about 1.0% weight. multimetallic component, and even more preferably from the eye is about 0.05% weight. up to about 0.5% weight. multimetallic component.

Solid acid catalyst will generally include a matrix (also called a binder) components, in particular, to impart physical integrity (e.g., tensile crushing, education, fine particles and so on), and macro porosity. Being used, the matrix components can be combined with the zeolite before or after the process in which multimetallic component is introduced into the catalyst. Materials that can be used as matrix components are inorganic oxides, such as oxides of aluminum, oxides of silicon, oxides of silicon, aluminum, Zirconia, clay, etc. the Matrix can be in the form of Zola, hydrogel or gel, and it may be catalytically active or inert. If you use the matrix material, the matrix material may contain from about 2% to about 98 wt%. the matrix material based on the combined weight of the matrix material and zeolite. The amount of matrix material included in the solid acid catalyst is selected to achieve the desired strength crushing, at the same time maintaining sufficient catalytic activity, taking into account the dilution of the zeolite matrix component. Preferably the matrix material bude is contained in an amount of from about 5% weight. to about 70 wt%. in the calculation of the combined weight of the matrix material and zeolite, and more preferably from about 10 wt%. up to about 50% weight. In a particularly preferred embodiment, the matrix material is contained in an amount of from about 15 wt%. to about 30 wt%. in the calculation of the combined weight of the matrix material and zeolite.

Multimetallic solid acid catalyst preferably has a diameter of extrudate from about 0.08 mm to about 2.5 mm When used in a reactor with a fixed bed, the diameter of the extrudate is preferably at least about 0.5 mm, with an upper limit of about 1.8 mm Smaller diameters can be used in the fluidized bed reactor or a slurry reactor. The catalyst preferably has an average diameter of micropores of about 7,4Å (7,4×10-10m)when using zeolite X or Y.

Multimetallic solid acid catalyst may be used in several configurations process for alkylation catalysis of the reaction of paraffin and olefin with the formation of gasoline having a high value of the octane number of gasoline by the research method (RON) and motor octane number (MON). The alkylation process may be performed in any suitable form reaction system, known qualified specialists in this field of technology, so the th as processes with entrained fluidized bed, processes with a fixed fluidized bed, reactors, fluidized bed, slurry processes and processes with a fixed layer. For example, the alkylation process can represent this process, which is described in the Patent of the United States No. 6844479 or Patent Publications of the United States No. 2004/0162454 listed here for information.

Typically, the alkylation process is carried out in such conditions that at least part of the alkylating reagent and alkilirutego connection will be in liquid phase or in the supercritical phase. In General, the process is carried out at a temperature in the range from about -40° to about 250°C., preferably in the range of from about 50° to about 150°C., more preferably in the range of from about 70° to about 100°C. and a pressure of from about 1 to about 100 bar (0.1 to 10 MPa), preferably from about 10 to about 40 bar (1-4 MPa) and more preferably from about 15 to about 30 bar (1.5 to 3 MPa). The molar ratio alkilirutego compound to alkylating reagent in the total mass of raw material in the reactor is preferably higher than about 5:1 and more preferably higher than about 50:1. Higher molar ratios are considered as preferred for performance reasons, because they in General provide for increasing the octane number of the product and stability of the catalyst. In the of rhny limit for this ratio is determined by the type of process and economic factors of the process. The upper limit of the molar ratio is not critical and can reach a maximum of 5000:1. In General, economic reasons are the preferred molar ratio of, for example, at about 1000:1 or lower. In many modern versions use a molar ratio alkilirutego compound to alkylating reagent level 150-750:1 is considered as the most preferred. The feed rate of raw material (WHSV, average hourly feed rate) alkylating reagent in General ranges from about 0.01 to about 5, preferably in the range of from about 0.05 to about 0.5 and more preferably in the range of from about 0.1 to about 0.3 gram alkylating reagent per gram of catalyst per hour. The value of the average hourly feed rate of raw material (WHSV) alkilirutego saturated hydrocarbon preferably ranges from about 0.1 to about 500. It should be understood that the use of solid acid catalyst according to the present invention is not limited to any specific reaction conditions, and the above conditions are approximate.

The catalyst according to the invention particularly suitable for use in the alkylation of isoalkanes having 4-10 carbon atoms, such as isobutane, isopentane or isohexane, or mixtures thereof, olefins, having the mi 2-10 carbon atoms, preferably 2-6 carbon atoms and more preferably 3-5 carbon atoms. The alkylation of isobutane butane or a mixture of butenes is a particularly preferred variant implementation. The invention is not limited in this respect, and in the process of alkylation to produce a desired product may be used any suitable paraffin or olefin.

The catalyst according to the present invention can also be used for other types of alkylation processes, such as processes that are used cycloalkanes or arylalkenes. For example, the catalysts can be used in the processes for correcting cetane number some threads distillates. For example, light cycle Gasol (“LCO”), the product of the distillation process for Catalytic Cracking (“FCC”), contains unsubstituted cycle and a low degree of alkylated aromatic cycles; as such, its cetane number is quite low - typically 10-30. Hydrogenation of light cycle of gazala (LCO) only slightly increases the cetane number. Usually gidrirovanie components are in low-grade alkylated cycloalkanes, such as methylethylketon. In one embodiment, the catalyst may be used in the process for a combination of hydrogenated light cycle Gaza is I (LCO) flow roughing C4-C6-olefins to produce high-quality diesel fuel.

Regeneration of the catalyst may be carried out using a low-temperature method or the high-temperature method. Low-temperature method is often performed before a product is found olefins, preferably in a state of less than about 20% of the time active cycle of the catalyst. Active cycle of the catalyst is defined as the time from the beginning of the filing of the alkylating reagent to the moment when compared with the figures at the entrance to containing the catalyst section of the reactor is about 20% of the alkylating reagent out of the containing catalyst section of the reactor unreacted, not counting the isomerization within the molecule. Low-temperature regeneration can be executed in the most practical way of stopping the feed of olefin and the introduction of hydrogen enriched in isobutane hydrocarbon raw material, when the reaction temperature is from about 70° to about 100°C. to remove C12+ heavy hydrocarbons and coke. More rigid high-temperature reactivation is usually conducted after a large number of low-temperature regeneration, at temperatures of from about 175° to about 350°C. In the high temperature reactivation stop threads as paraffin, olefin, and hydrogen gas is passed over the catalyst to remove coke and heavy hydrocarbons.

The following paragraph shall emery illustrate features of the present invention. In Examples 8-14 used reactor system 100 shown in Figure 1. In a reactor system using recirculation flow R, which combines the commodity flows F-1 (olefin) and F 2 (isoparaffin). The olefin stream F-1 includes CIS-2-butene, and the flow of isoparaffin comprises isobutane. The combined flows through line 101 are sent to the reactor 110 for alkylation, which contains the fixed layer 111 of the catalyst according to the invention. Reactor for alkylation immersed in an oil bath 112 to maintain a predetermined reaction temperature. The sample for gas chromatographic (GC) analysis can be selected in the channel 103 from the waste stream 102 from the reactor 110 for alkylation. The exhaust stream is divided into recycle stream R, which is circulated by a pump P back to the reactor 110 for alkylation with the addition of fresh raw materials F-1 and F-2, and stream 104 that is directed into the separation drum 120, from which a pair of V derived from the upper part, and the alkylate And as a product (for example, isomeric trimethylpentane (TMP)) is withdrawn from the bottom part. The reactor 110 works as a recycle reactor with a fixed bed to maintain a high value relationships of isobutane to butene and modeling of the reactor constant mixing (CSTR). High values of the ratios of the isobutane/butene help to minimize the education of coke and high-boiling components, which inactivate the catalyst. Can be used in a reactor with a fixed bed having multiple channels for injection of butene in places that are located at different heights on the fixed layer, in order to maintain the desired ratio of isobutane/butene in any given place in the whole entire layer of catalyst. The reaction product was a mixture of various components and/or isomers. Preferred components of the alkylation represent isomers trimethylpentane (TSR) branched C8-hydrocarbons, each of which has a high value of the octane number of gasoline by the research method (“RON”). For example, 2,2,4-trimethylpentane (isooctane) has the value of the octane number of gasoline by the research method (RON)equal to 100. The overall octane number of gasoline by the research method (RON) alkylate obtained in the examples was obtained by summing the works of the weight fraction of each component (determined using gas chromatography (GC) analysis), multiplied by the octane number of the component. The experiments continued until, while in the reaction product did not appear olefins (disable when 0,012% weight. was defined as the moment of breakthrough). At this point olefinic peaks in gas chromatography analysis showed deactivation of the catalyst.

The USE of THE S

EXAMPLE 1

The control catalyst (containing metals)

Illustrated here as examples of the catalysts used conventional zeolite framework, namely a commercially available zeolite ultrastable (with respect to Y (“USY”) under the name CBV500 manufactured by the PQ Corp. Product CBV500 has approximately 80% of the weight. zeolite and 20% of alumina. The catalyst was sieved through a sieve with mesh size 18/25 mesh for use in testing performance of laboratory scale (described below). The finished catalyst was designated as catalyst "A".

EXAMPLE 2

Obtaining a catalyst containing 0.5 wt%. platinum (Pt)

Platinum (Pt) catalyst control (i.e. without second or third added metal) was prepared from commercially available zeolite ultrastable (with respect to Y (“USY”) under the name CBV500 described in Example 1. Platinum (Pt) was added with a solution of nitrate salt tetraammineplatinum entered a commonly used method of initial wetting. The catalyst was dried at a temperature of 110°C in air with subsequent calcification at a temperature of 400°C in air atmosphere. Used the amount of salt of platinum (Pt), sufficient to ensure that the final catalyst contained 0.5% weight. platinum (Pt). The catalyst was sieved through a sieve with mesh size 18/25 mesh for the use of the Finance in the benchmark tests at laboratory scale (described below). The finished catalyst was designated as catalyst "B".

EXAMPLE 3

Obtaining a catalyst containing 0.15% of the weight. platinum (Pt)

A second catalyst containing only platinum (Pt) (i.e., without the second or third added metal), prepared from commercially available zeolite ultrastable (with respect to Y (“USY”) under the name CBV500 described in Example 1. Platinum (Pt) was added with a solution of nitrate salt tetraammineplatinum entered a commonly used method of initial wetting. The catalyst was dried at a temperature of 110°C in air with subsequent calcification at a temperature of 400°C in air atmosphere. Used the amount of salt of platinum (Pt), sufficient to ensure that the final catalyst contained 0.15% of the weight. platinum (Pt). The catalyst was sieved through a sieve with mesh size 18/25 mesh for use in testing performance of laboratory scale (described below). The finished catalyst was designated as catalyst "C".

EXAMPLE 4

Getting a platinum-Nickel (Pt/Ni) comparative catalyst

Platinum-Nickel (Pt/Ni) catalyst was prepared from a commercially available zeolite ultrastable (with respect to Y (“USY”) under the name CBV500 described in Example 1. Platinum (Pt) was added with a solution of nitrate salt tetraammineplatinum entered common is the procedure of initial wetting. The catalyst was dried at a temperature of 110°C in air with subsequent calcification at a temperature of 400°C in air atmosphere. Used the amount of salt of platinum (Pt), sufficient to ensure that the final catalyst contained 0,12% weight. platinum (Pt). The stage of introduction of the second metal used to add Nickel (Ni). Nickel (Ni) was added with a solution of nitrate Nickel salts, introduced a commonly used method of initial wetting. The catalyst was dried at a temperature of 110°C in air with subsequent calcification at a temperature of 400°C in air atmosphere. Used the amount of salt Nickel (Ni), sufficient to ensure that the final catalyst contained 0.10% per weight. Nickel (Ni). The catalyst was sieved through a sieve with mesh size 18/25 mesh for use in testing performance of laboratory scale (described below). The finished catalyst was designated as catalyst D".

EXAMPLE 5

Getting a platinum-Nickel (Pt/Ni) comparative catalyst (low content)

Platinum-Nickel (Pt/Ni) catalyst was prepared from a commercially available zeolite ultrastable (with respect to Y (“USY”) under the name CBV500 described in Example 1. Platinum (Pt) was added with a solution of nitrate salt tetraammineplatinum entered common way initially is about wetting. The catalyst was dried at a temperature of 110°C in air with subsequent calcification at a temperature of 400°C in air atmosphere. Used the amount of salt of platinum (Pt), sufficient to ensure that the final catalyst contained 0.06% of the weight. platinum (Pt). The stage of introduction of the second metal used to add Nickel (Ni). Nickel (Ni) was added with a solution of nitrate Nickel salts, introduced a commonly used method of initial wetting. The catalyst was dried at a temperature of 110°C in air with subsequent calcification at a temperature of 400°C in air atmosphere. Used the amount of salt Nickel (Ni), sufficient to ensure that the final catalyst contained 0.05% weight. Nickel (Ni). The catalyst was sieved through a sieve with mesh size 18/25 mesh for use in testing performance of laboratory scale (described below). The finished catalyst was designated as catalyst "E".

EXAMPLE 6

Receiving platinum-cobalt (Pt/Co) comparative catalyst

Based on the unexpected and synergistic beneficial properties of platinum-Nickel (Pt/Ni) catalyst prepared platinum-cobalt (Pt/Co) catalyst with a commercially available zeolite ultrastable (with respect to Y (“USY”) under the name CBV500 described in Example 1. Platinum (Pt) was added with a solution of nitrogen is the Isla salt tetraammineplatinum, put commonly used means the initial wetting. The catalyst was dried at a temperature of 110°C in air with subsequent calcification at a temperature of 400°C in air atmosphere. Used the amount of salt of platinum (Pt), sufficient to ensure that the final catalyst contained 0,12% weight. platinum (Pt). The stage of introduction of the second metal used to add cobalt (Co). Cobalt (Co) was added with a solution of nitrate salts of cobalt, introduced a commonly used method of initial wetting. The catalyst was dried at a temperature of 110°C in air with subsequent calcification at a temperature of 400°C in air atmosphere. Used the amount of salt of cobalt (Co), sufficient to ensure that the final catalyst contained 0,11% weight. cobalt (Co). The catalyst was sieved through a sieve with mesh size 18/25 mesh for use in testing performance of laboratory scale (described below). The finished catalyst was designated as catalyst "F".

EXAMPLE 7

Obtaining a catalyst containing 0.5 wt%. Nickel (Ni) (without including platinum (Pt))

The catalyst containing only Nickel (Ni), prepared from commercially available zeolite ultrastable (with respect to Y (“USY”) under the name CBV500 described in Example 1. Nickel (Ni) was added with a solution of nitrate salt is ikela (Ni), put commonly used means the initial wetting. The catalyst was dried at a temperature of 110°C in air with subsequent calcification at a temperature of 400°C in air atmosphere. Used the amount of salt Nickel (Ni), sufficient to ensure that the final catalyst contained 0.5% weight. Nickel (Ni). The catalyst was sieved through a sieve with mesh size 18/25 mesh for use in testing performance of laboratory scale (described below). The finished catalyst was designated as catalyst "G".

EXAMPLE 8

Test the performance of the alkylation and regeneration of the catalyst: the catalyst In

Test alkylation at laboratory scale were carried out in a reactor system 100, illustrated in Figure 1, at a temperature of 80°C and a total pressure of 400 psig (2,757 MPa (gauge)). Reactant was a mixture of 2-butene ("olefin" or "On") and isobutane ("I"), with the total molar ratio "I/O"equal to 16. Thanks recycling isobutane internal ratio “I/O” was about 750. The catalyst is pre-treated by heating from room temperature to 300°C with a rate of temperature rise of 1°C/min in air stream (flow rate of 75 ml/min/g catalyst), holding for 2 hours at this temperature, cooled back to room temperature the tours, then switch on the flow of hydrogen with a flow rate of 20 ml/min/gram of catalyst, at the same time, with temperatures up to 275°C with a rate of temperature rise of 1°C/min, holding for 2 hours and cooled to room temperature. Each test used 4 parts of catalyst and 0.27 parts/min above-mentioned mixture of the reactants. The composition of the product was monitored using gas chromatography (GC) and was calculated octane number (C5+)-gasoline (octane number of gasoline by the research method (RON)). Experimental conditions reflect those for industrial production, where the initial conversion of the olefin is 100% at the beginning of the process.

In this process the catalyst is subjected to "stripe" aging, that is, the accumulation of "coke" (heavy hydrocarbons) comes from the front of the reactor to the rear of the reactor. Deactivation of the catalyst occurs when the conversion of the olefin becomes incomplete. This effect is called "breakthrough olefin" or simply "the breakthrough". The cycle length is determined by the breakthrough time, after which the catalyst must be regenerated. In this experiment, breakthrough is defined as the time when the output of the olefin reaches 0,012% weight. from the amount of product and recycled isobutane.

After breakthrough, the catalyst was regenerated with p the power flow of the hydrogen with the speed of temperature rise of 1°C/min until a temperature of 275°C and then kept at the temperature for 2 hours.

After regeneration the catalyst was tested again under the same conditions as in the first test cycle, and monitor the breakthrough of the olefin. Upon reaching the end of the cycle, the catalyst was again regenerated and tested the performance of the third cycle.

The performance results shown in Figure 2. The catalyst showed the breakthrough times of 4.6 hours 3.9 hours and 4.7 hours for the three test cycles. Full recovery performance shows that the process of regeneration with hydrogen is a very effective.

EXAMPLE 9

Test the performance of the alkylation and Regeneration of the Catalyst: the Catalyst And

The catalyst And catalyst control without metal content, were tested in the same manner as in Example 8, except that he had only two cycles. Fresh catalyst had a breakthrough time of 4.5 hours, showing a performance equivalent to that of the catalyst C. This result, together with the equivalent octane product demonstrates that the metal did not play a significant role for the performance of the alkylation.

After high temperature regeneration of the catalyst was tested for the second cycle, the onset of the breakthrough of the olefin was pretty quick - 1.2 hours. This result demonstrates the crucial role of metal for the regeneration of hydrogen. Because productive is th second cycle was bad, the third cycle was considered inappropriate.

EXAMPLE 10

Test the performance of the alkylation and regeneration of the catalyst: the catalyst With

The catalyst, a catalyst with a low content of platinum (Pt), felt the equivalent way as a catalyst (example 8). Fresh catalyst had the first cycle of 4.5 hours before the breakthrough of the olefin - identical performance catalyst Century On the basis of his performance in the second and third cycle, cycle-to-cycle has been some degradation of about 10% in each cycle. In order to achieve complete regeneration, these results show that the critical content of platinum (Pt) lies above the 0.15 wt%, when there are no other metals.

EXAMPLE 11

Test the performance of the alkylation and regeneration of the catalyst: the catalyst D

Catalyst D catalyst with a content of 0.12 wt%. platinum (Pt) and 0.10 wt%. Nickel (Ni), felt the equivalent way as a catalyst (example 8). Fresh catalyst had the first cycle of 4.6 hours before the breakthrough of the olefin - identical performance catalyst Century, His second cycle also had a breakthrough time of 4.6 hours, with subsequent breakthrough time of 4.4 hours in his third cycle. These results demonstrate that the bimetallic catalyst had neo is commonly a good regeneration performance from cycle to cycle.

EXAMPLE 12

Test the performance of the alkylation and regeneration of the catalyst: the catalyst E

Catalyst E catalyst content is 0.06 wt%. platinum (Pt) and 0.05% weight. Nickel (Ni), felt the equivalent way as a catalyst (example 8). Fresh catalyst had the first cycle of 4.3 hours before the breakthrough of olefins is almost identical to the performance of the catalyst Century, However, the cycle-to-cycle has been some degradation of performance (second cycle had a breakthrough time of 3.7 hours, with subsequent breakthrough time of 3.3 hours in his third cycle). These results demonstrate that the bimetallic catalyst was saving performance by minor, low to bad level, but clearly superior not containing metal catalyst.

EXAMPLE 13

Test the performance of the alkylation and regeneration of the catalyst: the catalyst F

Catalyst F catalyst with a content of 0.12 wt%. platinum (Pt) and 0.11 weight. cobalt (Co), felt the equivalent way as a catalyst (example 8). Fresh catalyst had the first cycle of 4.7 hours before the breakthrough of olefins is identical to the performance of the catalyst Century, His second cycle had a breakthrough time of 4.9 hours, with subsequent breakthrough time of 4.4 hours in his third cycle. These results demonstrate that the boards the but-cobalt (PtCo) bimetallic catalyst also had a good recovery performance from cycle to cycle.

EXAMPLE 14

Test the performance of the alkylation and regeneration of the catalyst: the catalyst G

Catalyst G catalyst with a content of 0.50 wt%. Nickel (Ni), felt the equivalent way as a catalyst (example 8). Fresh catalyst had the first cycle of 3.9 hours before the breakthrough of olefins is 15% lower than the performance of the Catalyst Century, His second cycle had a breakthrough time of 2.4 hours, with subsequent breakthrough time 0.9 hours in his third cycle. These results demonstrate that the catalyst containing only Nickel (Ni), showed very poor recovery performance from cycle to cycle, indicating that for the purposes of regeneration requires the presence of at least one noble metal.

EXAMPLE 15

Methodology characterizing platinum (Pt) and bimetallic catalysts for the alkylation

A series of catalysts was prepared for characterizing the chemisorption of carbon monoxide (CO) and removing the infrared spectra with Fourier transform (FTIR). Prepared sample to 0.35 wt%. platinum (Pt) on ultrastable (with respect to zeolite Y ("USY"), designated as "Catalyst H". A second sample, designated as "Catalyst I"included 0,105% weight. Nickel (Ni) and 0.35 wt%. platinum (Pt) on USY. The third sample, designated as Catalyst J"included 0,105% weight. Nickel (Ni) and 0.12 wt%. platinum (Pt) is as USY.

A variety of laboratory processing of these three catalysts are shown in Figure 3. These are:

Recovery of hydrogen (H2): processing at a temperature of 450°C and a partial pressure of hydrogen (H2) 30 Torr (30 mm Hg, 4,0 kPa) for 30 minutes. This restoration was performed with periodic repeat up to three times.

The formation of coke: the Catalyst was subjected to isobutane (partial pressure of 15 Torr) (2,0 kPa) and CIS-2-butene (partial pressure of 1 Torr) (133,32 PA) at a temperature of 80°C for 30 minutes with periodic repeat up to two times.

Regeneration with hydrogen (H2): Zakochany the catalyst was subjected to hydrogen (H2) with a partial pressure of 10 Torr (of 1.33 kPa) at 250°C for 50 minutes, with periodic repeat up to two times.

Measurement of carbon monoxide (CO): standard chemisorption of carbon monoxide (CO) characterized different treated catalysts. The dispersion of platinum (Pt) could be estimated using the stoichiometric relationship "Pt:" level 1:1. In addition, the catalyst was monitored using infrared spectroscopy with Fourier transform (FTIR), where it was possible to determine the dispersed particles of platinum (Pt).

Figure 4 shows the characteristic frequency of the absorption of carbon-carbon bonds in celibately the x spectra coke and coke precursors.

EXAMPLE 16

Chemisorption of carbon monoxide (CO) on "sakakawea" Catalyst H: 0.35% of the weight. platinum (Pt)/USY

Figure 5 shows measurements using infrared spectroscopy with Fourier transform (FTIR) catalyst H in three States: (a) recovered (b) after "coking" within 240 minutes, and (C) after regeneration with hydrogen (H2within 100 minutes. Sharp single peak at wave number 2065 cm-1for (a) and (C) shows that the regeneration of hydrogen (H2) restores platinum (Pt) to her well-defined active state. A broad peak for (b) indicates that the metal function of platinum (Pt) was worse.

EXAMPLE 17

Measurements using infrared spectroscopy with Fourier transform (FTIR): the Formation of coke on the catalyst H: 0.35% of the weight. platinum (Pt)/USY

6 shows three infrared spectrum with a Fourier transform (“FTIR”) for the catalyst to 0.35 wt%. platinum (Pt)/USY ("catalyst H") and hydrocarbon "coke". This includes not containing hydrocarbons, recovered catalyst (upper curve); catalyst, zakochany within thirty minutes (middle curve); and catalyst, zakochany within sixty minutes (the lower curve). A key area of interest is near the region of wave numbers 3000 cm-1that region, which is matched with the edge of aliphatic (i.e. paraffin) hydrocarbons. The recovered catalyst shows essentially no hydrocarbon, whereas both coked catalyst detect the presence of aliphatic hydrocarbons. Zakochany for a longer time the catalyst (lower curve) had a significantly higher content of the hydrocarbon material.

EXAMPLE 18

Measurements using infrared spectroscopy with Fourier transform (FTIR): regenerated with hydrogen (H2) catalyst H: 0.35% of the weight. platinum (Pt)/USY

Fig.7 shows three infrared spectrum with a Fourier transform (“FTIR”) for the catalyst to 0.35 wt%. platinum (Pt)/USY ("Catalyst H") and hydrocarbons. The upper curve (the same as the lower curve in Figure 6) corresponds to shestidesyatiletiyu coking Pt/USY-sample. This catalyst was regenerated in the hydrogen (H2within 50 minutes (middle curve) and 100 minutes (lower curve). While effective, were both regeneration, increased duration was more efficient to remove the greater part of coke.

EXAMPLE 19

Measurements using infrared spectroscopy with Fourier transform (FTIR): the Formation of coke on the catalyst I: 0,105% weight. Nickel (Ni) - 0.35% of the weight. platinum (Pt)/USY

Fig shows three infrared spectrum with a Fourier transform (“FTIR”) for catalyst I (0,105% ve is. Nickel (Ni) - 0.35% of the weight. platinum (Pt)/USY) and hydrocarbon "coke". This includes not containing hydrocarbons, recovered catalyst (upper curve); catalyst, zakochany within thirty minutes (middle curve); and catalyst, zakochany within sixty minutes (the lower curve). A key area of interest is near the region of wave numbers 3000 cm-1area which corresponds to the aliphatic (i.e. paraffin) hydrocarbons. The recovered catalyst shows essentially no hydrocarbon, whereas both coked catalyst detect the presence of aliphatic hydrocarbons. Zakochany for a longer time the catalyst (lower curve) had a significantly higher content of the hydrocarbon material. The main fact can be seen when comparing the lower curves in Fig.6 and 8: under the same conditions coking bimetallic catalyst I (Fig) had a lower accumulation of hydrocarbons than the Catalyst H "only with platinum (Pt)" (6), as shown in the region of wave numbers 3000 cm-1. This unexpected result suggests that the bimetallic catalyst has a higher activity in the hydrogenation than the catalyst only with platinum (Pt)".

EXAMPLE 20

Measurements using infrared spectroscopy with p is the education Fourier transform (FTIR): regenerated with hydrogen (H 2) Catalyst I: 0,105% weight. Nickel (Ni) - 0.35% of the weight. platinum (Pt)/USY

Fig.9 shows three infrared spectrum with a Fourier transform (“FTIR”) for catalyst 0,105% weight. Nickel (Ni)/0.35% of the weight. platinum (Pt)/USY ("catalyst I") and hydrocarbon residue ("coke"). The upper curve (the same as the lower curve in Figure 8) is shestidesyatiletiyu coking Pt/USY-sample. This catalyst was regenerated in the hydrogen (H2within 50 minutes (middle curve) and 100 minutes (lower curve). While effective, were both regeneration, increased duration was more efficient to remove the greater part of coke. The main fact can be seen when comparing the lower curves in Fig.7 and 9: under the same conditions of regeneration in the hydrogen (H2) bimetallic catalyst I (Fig.9) had a lower accumulation of hydrocarbons than the catalyst I "only with platinum (Pt)" (Fig.7), as shown in the region of wave numbers 3000 cm-1. This unexpected result suggests that the bimetallic catalyst has a higher activity in the hydrogenation than the catalyst only with platinum (Pt)". Since the bimetallic catalyst also generates fewer coke (see example 19), it is not clear whether the advantage of bimetallic material in (a) reduced the formation of coke or (b) as in, decreased the formation of coke, and the best regeneration in hydrogen (H2). Regardless of the mechanism (a) or (b), any of them is obviously excellent and unexpected results.

EXAMPLE 21

Measurements using infrared spectroscopy with Fourier transform (FTIR): the Formation of coke on the catalyst J: 0,105% weight. Nickel -(Ni) - 0,12% weight. platinum (Pt)/USY

Figure 10 shows three infrared spectrum with a Fourier transform (“FTIR”) for the catalyst 0,105% weight. Nickel (Ni)/0,12% weight. platinum (Pt)/USY) ("catalyst I") and hydrocarbon "coke". This includes not containing hydrocarbons, recovered catalyst (upper curve); catalyst, zakochany within thirty minutes (middle curve); and catalyst, zakochany within sixty minutes (the lower curve). A key area of interest is near the region of wave numbers 3000 cm-1area which corresponds to the aliphatic (i.e. paraffin) hydrocarbons. The recovered catalyst shows essentially no hydrocarbon, whereas both coked catalyst detect the presence of aliphatic hydrocarbons. Zakochany for a longer time the catalyst (lower curve) had a significantly higher content of the hydrocarbon material. The main fact can be seen when comparing the lower curves in Fig.6 and 8: Ave the same conditions coking bimetallic catalyst (Fig) had a lower accumulation of hydrocarbons, than the catalyst H "only with platinum (Pt)" (6), as shown in the region of wave numbers 3000 cm-1. This unexpected result suggests that the bimetallic catalyst had high activity in the hydrogenation than the catalyst H "only with platinum (Pt)". Moreover, as shown in Figure 10, the number of aliphatic coke was more for the catalyst 0,105% weight. Nickel -(Ni)/0,12% weight. platinum (Pt)/USY), catalyst (J. This fact suggests that either (a) the content of platinum (Pt) was below the critical level for efficiency, or that (b) molar ratio “Ni/Pt and the metal levels were too low to ensure that the majority of atoms of platinum (Pt) were surrounded by a sufficient amount of Nickel (Ni) to achieve the synergistic effect observed for catalyst I.

EXAMPLE 22

Measurements using infrared spectroscopy with Fourier transform (FTIR): regenerated with hydrogen (H2) catalyst J: 0,105% weight. Nickel -(Ni)/0,12% weight. platinum (Pt)/USY

11 shows three infrared spectrum with a Fourier transform (“FTIR”) for catalyst 0,105% weight. Nickel (Ni) and 0.12 wt%. platinum (Pt)/USY (catalyst J) and hydrocarbon "coke". The upper curve (the same as the lower curve for Fig) corresponds shestidesyatiletiyu coking of catalyst J This catalyst was regenerated in the hydrogen (H 2within 50 minutes (middle curve) and 100 minutes (lower curve). While effective, were both regeneration, increased duration was more efficient to remove the greater part of coke. The main fact can be seen when comparing the lower curves in Fig.7 and 9: under the same conditions of regeneration in the hydrogen (H2) bimetallic catalysts (figures 9 and 11) had a lower accumulation of hydrocarbons than the catalyst only with platinum (Pt)" (Fig.7), as shown in the region of wave numbers 3000 cm-1. This unexpected result suggests that the bimetallic catalyst had high activity in the hydrogenation than the catalyst only with platinum (Pt)". Since the bimetallic catalyst J of Example 21 also does not generate a smaller amount of coke than the catalyst I with 0,105% weight. Nickel (Ni) - 0.35% of the weight. platinum (Pt) (see example 19), it is clear that the advantage of bimetallic catalysts with a lower metal content is in the best regeneration in hydrogen (H2). This is obviously excellent and unexpected results.

EXAMPLE 23

Measurements using infrared spectroscopy with Fourier transform (FTIR): Chemisorption capacity in respect of carbon monoxide (CO) three coked catalysts

Fig shows infrared spectra with Fourier-transformed the eat (FTIR) for the three catalysts (N: 0.35% of the weight. platinum (Pt)/USY [UP], I: 0,105% weight. Nickel (Ni) - 0.35% of the weight. platinum (Pt)/USY [MIDDLE], and J: 0,105% weight. Nickel (Ni) and 0.12 wt%. platinum (Pt)/USY [NIH]) after 60 minutes of coking. It should be noted that zakochany catalyst H "only with platinum (Pt) on USY" had a broader peak of platinum (Pt) lower intensity. This means that platinum (Pt) is obviously less dispersed, and had a lower content of the recovered platinum (Pt). The curves for the two bimetallic catalysts showed that (a) the peak of platinum (Pt) was more intense, and (b) more clearly formed (more narrow). These results show that when the coking bimetallic catalysts retain the dispersion of platinum (Pt) and the action of the recovered platinum (Pt) is better than the catalyst only with platinum (Pt)". Again, this is an excellent and unexpected results.

EXAMPLE 24

Measurements using infrared spectroscopy with Fourier transform (FTIR): chemisorption capacity in respect of carbon monoxide (CO) three regenerated hydrogen (H2) catalysts

Fig shows infrared spectra with Fourier transform (FTIR) for the three catalysts (N: 0.35% of the weight. platinum (Pt)/USY [UP], I: 0,105% weight. Nickel (Ni) - 0.35% of the weight. platinum (Pt)/USY [MIDDLE], and J: 0,105% weight. Nickel (Ni) and 0.12 wt%. platinum (Pt)/USY [NIH]) after 100 minutes of regeneration in which oredom (H 2). It should be noted that the regenerated hydrogen (H2) catalyst H "only with platinum (Pt) on USY" had a broader peak of platinum (Pt) lower intensity. This means that platinum (Pt) is obviously less dispersed and had less restored platinum (Pt). The curves for the two bimetallic catalysts showed that (a) the peak of platinum (Pt) was more intense and (b) more clearly formed (more narrow). These results show that by regeneration with hydrogen (H2) bimetallic catalysts retain high dispersion of platinum (Pt) and function restored platinum (Pt) compared with the catalyst only with platinum (Pt)". Again, this is an excellent and unexpected results.

EXAMPLE 25

Measurements using infrared spectroscopy with Fourier transform (FTIR): chemisorption capacity in respect of carbon monoxide (CO) three regenerated hydrogen (H2) catalysts

Fig shows two infrared spectrum with Fourier transform (FTIR) for each of the three catalysts (:0.15% of the weight. platinum (Pt)/USY [UP], F: 0,11% weight. cobalt (Co)-0,12% weight. platinum (Pt)/USY [MID] and D: 0,10% weight. Nickel (Ni) and 0.12 wt%. platinum (Pt)/USY [NIH]) after 100 minutes regeneration with hydrogen (H2). For each catalyst shows the spectrum with the background on carbon monoxide (CO) is atmosferoi (1 Torr) (133,32 PA) and without it. Three spectrum without background appear quite similar, showing only the strong binding of carbon monoxide (CO) and platinum (Pt). Since all three catalyst are approximately equivalent levels of platinum (Pt), these results are consistent with each other. However, if we consider the three spectrum with background carbon monoxide (CO), PtCo and PtNi-catalysts absorb more carbon monoxide (CO)than the catalyst-only with platinum (Pt)". These results indicate that the bimetals are reinforced metal function than the catalyst only with platinum (Pt), which is consistent with the improved performance demonstrated bimetallic materials.

As will be obvious by qualified professionals in this field of technology based on these guidelines, a variety of changes and modifications of the above-described and other embodiments of the invention can be made without going beyond its scope defined in the attached claims. Accordingly, this detailed description of the preferred embodiments should be construed as illustrative, but do not have a restrictive sense.

1. Solid acid catalyst for use in processes for the alkylation of paraffins with olefins, including:
(a) a zeolite selected from the group consisting of zeolite X, zeolite Y, ZSM-20, EMT and their combinations;
(b) multimetallic material introduced into the zeolite in which at least one of metal is Pt or Pd, and at least the second metal is Ni, Co, Mn, CR, V, Ti, Fe, Cu.

2. The solid acid catalyst according to claim 1, further comprising a binder material.

3. The solid acid catalyst according to claim 1, in which the zeolite has the structure of poasito.

4. The solid acid catalyst according to claim 1, in which multimetallic material is selected from the group consisting of PtNi, PtCo, PtMn, PtCr, PtV, PtTi, PtFe, PtCu, PtNiAg, PtNiAu, PtNiRu, PtNiIr, PtNiRh, PtNiRe, PdNi, PdCo, PdCu, PdMn, PdCr, PdV, PdTi, PdFe, PtPdCo, PtPdNi, PtPdMn, PtPdCr, PtPdV, PtPdTi, PtPdFe, PtPdCu, PdNiAg, PdNiAu, PdNiRu, PdNiIr, PdNiRh, PdNiRe, PtNiCo, PdNiCo, PtPdNiCo, PtNiCoFe and combinations thereof.

5. The solid acid catalyst according to claim 4, in which multimetallic material contains from about 0.01 wt.% up to about 2.0 wt.% by weight of solid acid catalyst.

6. The solid acid catalyst according to claim 2, in which the binder contains from about 5 wt.% to about 70 wt.% by weight of solid acid catalyst.

7. The solid acid catalyst according to claim 6, in which the binder material is selected from the group consisting of oxides of aluminum, oxides of silicon, oxides of silicon, of aluminum, of zirconium oxides, clays and combinations thereof.

8. The solid acid catalyst according to claim 3, in which the zeolite is present which allows a nanocrystalline zeolite Y.

9. The solid acid catalyst according to claim 3, in which the zeolite is an ultrastable (with respect to Y ("USY").

10. Solid acid catalyst for use in processes for the alkylation of paraffins with olefins, including:
(a) nanocrystalline zeolite Y;
(b) one or more multimetallic materials introduced into the zeolite is selected from the group consisting of PtNi, PtCo, PtMn, PtCr, PtV, PtTi, PtFe, PtCu, PtNiAg, PtNiAu, PtNiRu, PtNiIr, PtNiRh, PtNiRe, PdNi, PdCo, PdCu, PdMn, PdCr, PdV, PdTi, PdFe, PtPdCo, PtPdNi, PtPdMn, PtPdCr, PtPdV, PtPdTi, PtPdFe, PtPdCu, PdNiAg, PdNiAu, PdNiRu, PdNiIr, PdNiRh, PdNiRe, PtNiCo, PdNiCo, PtPdNiCo, PtNiCoFe, which multimetallic material contains from about 0.01 wt.% up to about 2.0 wt.% the weight of the solid acid catalyst; and
(c) one or more binders selected from the group consisting of oxides of aluminum, oxides of silicon, oxides of silicon, of aluminum, of zirconium oxides and clays, in which the binder contains from 5 wt.% up to 70 wt.% by weight of solid acid catalyst.

11. A method of alkylation of paraffins with olefins, comprising the stage of:
(a) providing a solid acid catalyst comprising a zeolite selected from the group consisting of zeolite X, zeolite Y, ZSM-20, EMT and their combinations and multimetallic material introduced into the zeolite in which at least one of metal is Pt or Pd, and at least the second metal is Ni, Co, Mn, Cr, V, Ti, Fe, si, and (b) mixing one or more alkilirutmi hydrocarbon-paraffins with one or more alkylating reagents-olefins in the presence of the specified catalyst at conditions that lead to alkylation reaction with the formation of the alkylation product; and regeneration of the catalyst in terms of H2.

12. The method according to claim 11, in which the zeolite has the structure of poasito, and the metal material is selected from the group consisting of PtNi, PtCo, PtMn, PtCr, PtV, PtTi, PtFe, PtCu, PtNiAg, PtNiAu, PtNiRu, PtNiIr, PtNiRh, PtNiRe, PdNi, PdCo, PdCu, PdMn, PdCr, PdV, PdTi, PdFe, PtPdCo, PtPdNi, PtPdMn, PtPdCr, PtPdV, PtPdTi, PtPdFe, PtPdCu, PdNiAg, PdNiAu, PdNiRu, PdNiIr, PdNiRh, PdNiRe, PtNiCo, PdNiCo, PtPdNiCo, and PtNiCoFe their combinatii.

13. The method according to item 12, in which the zeolite is a zeolite Y.

14. The method according to item 12, which alkiliruty hydrocarbon is a paraffin, and the alkylating agent is an olefin.

15. The method according to 14, in which the paraffin is an isobutane and the olefin is a butylene or a mixture of butylenes.

16. The method according to item 15, in which the paraffin comprises isobutane and isopentane, and olefin comprises a mixture of C3-C5-olefins.



 

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FIELD: chemistry.

SUBSTANCE: cascade of four bubbling reactors joined in series is made. A solvent, homogeneous catalyst, ethylene and a homogeneous cocatalyst are fed into the first reactor. An oligomerisation reaction takes place in the first reactor. Contents of the first reactor are moved into the second reactor of the cascade through a first system of pipes in which there is already ethylene and/or into which ethylene is simultaneously or successively added. An oligomerisation reaction takes place in the second reactor. Contents of the second reactor are moved into another second, series-connected reactor through a second system of pipes in which there is already ethylene and/or into which ethylene is simultaneously or successively added. Contents of the other second reactor are moved into the third reactor through a third system of pipes in which there is already ethylene and/or into which ethylene is simultaneously or successively added. An oligomerisation reaction takes place in the third reactor and linear oligomers of α-olefins are removed from the third reactor. The catalyst and cocatalyst are added not only into the first reactor but in one of the series-connected reactors of the cascade as well. Concentration of the catalyst and cocatalyst is controlled such that the highest concentration of the catalyst is in the first reactor, while that of the cocatalyst is in the last reactor.

EFFECT: invention enables to obtain oligomer without contamination with polymer or branched by-products.

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FIELD: chemistry.

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EFFECT: possibility of smaller heat exchangers or cooling devices, saving power and lowering expenses.

11 cl, 1 dwg

FIELD: chemistry.

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14 cl, 3 dwg, 3 tbl, 14 ex

FIELD: chemical industry; other industries; methods and devices for conversion of the methane by the plasma-catalytic oxidation.

SUBSTANCE: the invention is pertaining to the method for conversion of the methane by the plasma-catalytic oxidation and to the and devices fro the method realization. The method of conversion of methane is conducted by the super high frequency (SHF)radiation plasma-catalytic oxidation with production of ethylene. The method includes activation of the catalyst by the SHF radiation and formation of the non-equilibrium "cold" SHF plasma. Simultaneously exercise activation of the catalyst by the super high frequency radiation and by the SHF plasma and create the non-equilibrium "cold" super high frequency plasma simultaneously in the Е010 type resonator or on Е01 with the symmetry of rotation from the SHF generator and on the total wave Н11° with rotation of the polarization plane of the continuous SHF generator. In the device realizing the indicated process the round waveguide is smoothly transforms into the waveguide with the partial dielectric filling-up and contains the aligner used for reduction of the reflections of the super high frequency energy, the encapsulant for provision of vacuum in the SHF plasma-catalytic reactor and the SHF plasma generation on the butt of the quartz rod, with the located on it quartz plates and the catalyst. The batchers of the uniform feeding of the reactants (СН4 + О2 + Аг) are installed with the capability of rotation and movement with respect to the SHF plasma. The system of the reaction products withdrawal is located in symmetry to the axis of the with respect to the plasmatron. The invention stimulates the increase of efficiency of the conversion process of methane into ethylene.

EFFECT: the invention ensures stimulation of the increased efficiency of the conversion process of methane into ethylene.

9 cl, 2 ex, 4 dwg, 1 tbl

FIELD: chemical industry; petrochemical industry; other industries; methods and the devices for production of the oligomer of the linear alpha olefin.

SUBSTANCE: the invention is pertaining to the method of manufacture of the oligomer of the linear alpha olefin. The invention presents the method of production of the oligomer of the linear alpha olefin in the reactor containing the liquid and the gaseous phases including the phases of the catalytic oligomerization of ethylene in the presence of the complex of iron with the derivative of 2,6-bis(arylimino))pyridine up to oligomer of the alpha olefin with the average molecular-weight from 50 up to 350 with the heat release, and withdrawal of the heat by means of the heat exchanger, which is not in the direct contact with the liquid phase, with usage of at least, a part of the gaseous phase in the capacity of the coolant. The invention also presents the installation for realization of the above indicated method of production of the oligomer of the linear alpha olefin. The technical result of the invention is the effective cooling of the reaction mixture, prevention of the clogging of the cooling devices by the settlings of the paraffin and polyethylene.

EFFECT: the invention ensures the effective cooling of the reaction mixture, prevention of the clogging of the cooling devices by the settlings of the paraffin and polyethylene.

14 cl, 2 dwg

FIELD: petrochemical industry; methods of production of the polyolefin bases of the synthetic oils.

SUBSTANCE: the invention is pertaining to the method of production of the polyolefin bases of the synthetic oils by cationic oligomerization of the olefinic raw and may be used in petrochemical industry. The developed method contains: the stages of preparation of the olefinic raw, preparation and batching in the reactor of the solutions and suspensions of the components of the catalytic system Al(0)-HCl-(CH3)3CCl (TBX), isomerization of alpha-olefins and oligomerizations of the highest olefins and their mixtures under action of the catalytic system Al (0)-HCl-TBX, extractions of the dead catalyst, separation of the oligomerizate for fractions and hydrogenation of the extracted fractions under action of the catalytic agent Pd (0.2 mass %)/Al2O3+NaOH. The invention ensures improvement of the stages of the developed method. For prevention of the corrosion activity of the products the method additionally contains the stage of dechlorination of the present in the oligomerizate chlorine-containing oligoolefins by the metallic aluminum, triethylaluminum, the alcoholic solutions of KOH or using the thermal dehydrochlorination of the chlorine-containing polyolefins at the presence or absence of KOH. For improvement of the technical-and-economic indexes of the method at the expense of the increase of the output of the target fractions of polyolefins with the kinematic viscosity of 2-8 centistoke at 100°C the method additionally contains the stage of the thermal depolymerization of the restrictedly consumable high-molecular polyolefins with the kinematic viscosity of 10-20 centistoke at 100°C into the target polyolefins with the kinematic viscosity of 2-8 centistoke at 100°C.

EFFECT: the invention ensures improvement of all the stages of the developed method.

1 cl, 15 tbl

FIELD: petrochemical processes.

SUBSTANCE: feedstock is brought into contact with catalyst based on Pentasil family zeolite in at least two zones differing from each other in conditions of conversion of aliphatic hydrocarbons into aromatic hydrocarbons, first in low-temperature conversion zone to covert more active feedstock components to produce aromatic hydrocarbons containing product followed by recovering C5+-hydrocarbons therefrom and, then, contacting the rest of hydrocarbons produced in low-temperature conversion zone with catalyst in high-temperature conversion zone, wherein less active component(s) is converted into aromatic hydrocarbons containing product followed by recovering C5+-hydrocarbons therefrom.

EFFECT: enabled production of aromatic hydrocarbons under optimal conditions from feedstock containing aliphatic C1-C4-hydrocarbons with no necessity of separating the latter.

4 cl, 1 dwg, 1 tbl

FIELD: oil and gas production.

SUBSTANCE: invention refers to procedure for catalytic conversion of hydrocarbons. The procedure consists in contacting source hydrocarbons with catalyst of hydrocarbon conversion to ensure reaction of catalytic cracking in a reactor. Further, products of reaction are withdrawn from the reactor and are divided into fractions to produce light olefines, gasoline, diesel fuel, heavy diesel fuel and other saturated low-molecule hydrocarbons. Also, catalyst of hydrocarbons conversion contains (of total weight of catalyst): 1-60 % wt of mixture of zeolite, 5-99 % wt of heat-resistant non-organic oxide and 0-70 % wt of clay. Mixture of zeolite contains (from total weight of mixture): 1-75 % wt of beta-zeolite modified with phosphorus and transition metal M, 25-99 % wt of zeolite with MF-structure and 0-74 % wt of zeolite of large pores. Waterless chemical composition of beta-zeolite modified with phosphorus and transition metal M is of the following kind: (0-0.3)Na2O·(0.5-10)Al2O3·(1.3-10)P2O5·(0.7-15)MxOy·(64-97)SiO2 (in brackets there are indicated wt percents of oxides) where transition metal M is one or several metals chosen from a group consisting of Fe, Co, Ni, Cu, Mn, Zn and Sn; x is number of atoms of transition metal M, and y is number ensuring valence corresponding to a degree of transition metal M oxidation.

EFFECT: increased conversion of hydrocarbons of oil and higher output of light olefines, particularly, propylene.

17 cl, 43 ex, 8 tbl

FIELD: oil and gas production.

SUBSTANCE: invention refers to procedure for catalytic conversion of hydrocarbons. The procedure consists in contacting source hydrocarbons with catalyst of hydrocarbon conversion to ensure reaction of catalytic cracking in a reactor. Further, products of reaction are withdrawn from the reactor and are divided into fractions to produce light olefines, gasoline, diesel fuel, heavy diesel fuel and other saturated low-molecule hydrocarbons. Also, catalyst of hydrocarbons conversion contains (of total weight of catalyst): 1-60 % wt of mixture of zeolite, 5-99 % wt of heat-resistant non-organic oxide and 0-70 % wt of clay. Mixture of zeolite contains (from total weight of mixture): 1-75 % wt of beta-zeolite modified with phosphorus and transition metal M, 25-99 % wt of zeolite with MF-structure and 0-74 % wt of zeolite of large pores. Waterless chemical composition of beta-zeolite modified with phosphorus and transition metal M is of the following kind: (0-0.3)Na2O·(0.5-10)Al2O3·(1.3-10)P2O5·(0.7-15)MxOy·(64-97)SiO2 (in brackets there are indicated wt percents of oxides) where transition metal M is one or several metals chosen from a group consisting of Fe, Co, Ni, Cu, Mn, Zn and Sn; x is number of atoms of transition metal M, and y is number ensuring valence corresponding to a degree of transition metal M oxidation.

EFFECT: increased conversion of hydrocarbons of oil and higher output of light olefines, particularly, propylene.

17 cl, 43 ex, 8 tbl

FIELD: oil and gas production.

SUBSTANCE: invention refers to procedure for catalytic conversion of hydrocarbons. The procedure consists in contacting source hydrocarbons with catalyst of hydrocarbon conversion to ensure reaction of catalytic cracking in a reactor. Further, products of reaction are withdrawn from the reactor and are divided into fractions to produce light olefines, gasoline, diesel fuel, heavy diesel fuel and other saturated low-molecule hydrocarbons. Also, catalyst of hydrocarbons conversion contains (of total weight of catalyst): 1-60 % wt of mixture of zeolite, 5-99 % wt of heat-resistant non-organic oxide and 0-70 % wt of clay. Mixture of zeolite contains (from total weight of mixture): 1-75 % wt of beta-zeolite modified with phosphorus and transition metal M, 25-99 % wt of zeolite with MF-structure and 0-74 % wt of zeolite of large pores. Waterless chemical composition of beta-zeolite modified with phosphorus and transition metal M is of the following kind: (0-0.3)Na2O·(0.5-10)Al2O3·(1.3-10)P2O5·(0.7-15)MxOy·(64-97)SiO2 (in brackets there are indicated wt percents of oxides) where transition metal M is one or several metals chosen from a group consisting of Fe, Co, Ni, Cu, Mn, Zn and Sn; x is number of atoms of transition metal M, and y is number ensuring valence corresponding to a degree of transition metal M oxidation.

EFFECT: increased conversion of hydrocarbons of oil and higher output of light olefines, particularly, propylene.

17 cl, 43 ex, 8 tbl

FIELD: process engineering.

SUBSTANCE: invention relates to catalyst used in hydrogen cracking of paraffin hydrocarbons and to method of producing fuel main component. Proposed catalyst comprises USY zeolite produced from NaY that makes the initial compound and features intensity maximum of 30 or less displaying on surface 111 in analysing diffraction of X rays, binder and noble metal of VIII-group of periodic table. Invention covers also the method of producing fuel main component including hydrocracking of paraffin hydrocarbons using above described catalyst.

EFFECT: high cracking activity to allow high yield of medium fraction with low temperature of fuel main component congelation.

9 cl, 1 tbl, 9 ex

FIELD: process engineering.

SUBSTANCE: invention relates to catalyst and method of hydrocarbon treatment. Catalyst is intended for treatment of VGO/DMO to transform VGO/DMO into useful hydrocarbon products with shorter chains. Note here that VGO/DMO mix comprises less than that 10 % by volume of DMO while catalyst comprises: catalytic carrier material containing mesoporous material MCM-41 wherein major portion of pores inside catalytic material feature diametre varying from 20 to 50 A, catalytic material with which catalytic carrier material is impregnated, and promoter metal on catalytic carrier material intended for increasing catalytic conversion. Note here that said catalytic carrier material with catalytic metal and promoter metal serve to convert catalytically VGO/DMO into hydrocarbon products with shorter carbon chains. Invention covers also method of catalytic conversion of VGO/DMO in the presence of above described catalyst.

EFFECT: possibility to process hydrocarbon VGO/DMO mixes into products with shorter carbon mixes.

30 cl, 5 tbl, 1 dwg, 5 ex

FIELD: chemistry.

SUBSTANCE: invention relates to a method of producing indene dimmers through catalytic dimerisation of indene, characterised by that the catalyst used is zeolite ZSM-12 in H-form in amount of 10-30 wt % and the reaction is carried out at 100-200°C in aliphatic hydrocarbons in ratio indene: solvent equal to 1:1-4 (vol).

EFFECT: method simplifies production of indene dimers.

1 cl, 1 tbl, 8 ex

FIELD: chemistry.

SUBSTANCE: invention relates to a method of producing indene oligomers through catalytic oligomerisation of indene, characterised by that the catalysts used are zeolites Y and Beta, taken in amount of 10-30 wt % with respect to indene. The reaction is carried out at 80-200°C in a solvent medium or without.

EFFECT: method simplifies production of indene oligomers.

3 cl, 13 ex, 1 tbl

FIELD: chemistry.

SUBSTANCE: invention relates to a method of producing indene oligomers through catalytic oligomerisation of indene, characterised by that the catalysts used are zeolites Y and Beta, taken in amount of 10-30 wt % with respect to indene. The reaction is carried out at 80-200°C in a solvent medium or without.

EFFECT: method simplifies production of indene oligomers.

3 cl, 13 ex, 1 tbl

FIELD: chemistry.

SUBSTANCE: invention relates to a catalytic cracking composition. The composition contains: a) from approximately 12 to approximately 60 wt % zeolite Y; b) from 0.5 to 6 wt % rare-earth element, measured in form of an oxide of a rare-earth element; c) at least approximately 10 wt % pentasil, where the weight ratio of pentasil to zeolite Y is equal to at least 0.25 but not more than 3.0; and d) zeolite Y and pentasil make up at least approximately 35 wt % of the weight of the entire catalyst composition. The invention also discloses catalytic cracking methods.

EFFECT: invention increases output of light olefins.

81 cl, 8 ex, 8 tbl

FIELD: chemistry.

SUBSTANCE: present invention relates to improved catalysts, methods of preparing catalysts and methods for transalkylation of alkylaromatic hydrocarbons using catalysts. Described is a catalyst for transalkylation of alkylaromatic hydrocarbons containing a mordenite component, an acid molecular sieve component MFI, having molar ratio Si/Al2 less than 40, a rhenium component in range of 0.05-5% of the weight of the catalyst and a dispersing binding agent which is an inorganic oxide. The invention describes a method of preparing a transalkylation catalyst which involves the following steps: a) formation of a catalyst containing a mordenite component, an acid molecular sieve component MFI, having molar ratio Si/Al2 less than 40, a rhenium component in the range of 0.05-5% of the weight of the catalyst, and a dispersing binding agent which is an inorganic oxide; b) oxidation of the formed catalyst in conditions where atmospheric oxygen is present, temperature lies between 370°C and 650°C and for a period of time between 0.5 and 10 hours; and c) reduction of the oxidised catalyst in a reducing gas containing at least one gas selected from: hydrogen and hydrocarbon, in conditions where temperature lies between 100°C and 650°C. Described also is a method of producing xylene, involving the following steps: bringing a supply stream containing aromatic hydrocarbons, having at least seven carbon atoms, into contact with a catalyst in conditions for converting aromatic hydrocarbons, including presence of hydrogen and obtaining a stream of a product having high concentration of xylene, in which the catalyst contains a mordenite component; an acid molecular sieve component MFI, having molar ratio Si/Al2 less than 40, a rhenium component in the range of 0.05 to 5% of the weight of the catalyst; and a dispersing binding agent which is an inorganic oxide.

EFFECT: possibility of obtaining a transalkylation product with low content of components which boil together with benzene.

17 cl, 2 ex, 2 tbl

FIELD: process engineering.

SUBSTANCE: invention relates to carbon oxide catalyst, to method of manufactured gas production, to method of producing carbon dioxide reforming catalyst and carrier for said catalyst. Said catalyst converts initial hydrocarbon gaseous stock by carbon dioxide and is used for production of synthesis gas containing carbon monoxide and hydrogen. Note here that carbon dioxide reforming catalyst comprises main component representing mix of carrier containing carbonate of, at least, one alkaline-earth metal selected from the group consisting of Ca, Sr and Ba, and catalytic metal to promote reaction of decomposition of initial hydrocarbon gaseous stock. Method of producing carbon dioxide reforming catalyst comprises stages of mixing carrier containing carbonate of, at least, one alkaline-earth metal selected from the group consisting of Ca, Sr and Ba, titanium oxide and catalytic metal to promote reaction of decomposition of initial hydrocarbon gaseous stock and calcination to produce alkaline-earth metal composite oxide/Ti that can absorb carbon dioxide, and reaction of carbon dioxide absorption by said alkaline-earth metal composite oxide/Ti. Method of producing carbon dioxide reforming catalyst comprises stage of calcination in the presence of barium carbonate of, at least, one material selected from (a) wet ceramic film, (b) wet ceramic film wastes, (c) laminar wet ceramic film wastes and (d) those of wet ceramic film precursors. Note here that, at least, one of (a) to (d) is used in production of electronic component and, at least one of (a) to (d) contains, at least, one alkaline-earth metal selected from group consisting of Ca, Sr, Ba, and Ti at alkaline metal-to-Ti ratio making 0.9-1.1 that comprises the perovskite-structure metal as the main substance and catalytic metal. Method of producing synthesis gas comprising carbon monoxide and hydrogen in carbon dioxide reforming of gaseous hydrocarbon initial stock comprises the stages of carbon dioxide reforming of gaseous hydrocarbon initial stock containing methane as main component in using aforesaid carbon dioxide reforming catalyst and carbon dioxide reforming catalyst carrier used for production of synthesis gas containing carbon monoxide and hydrogen via reforming of gaseous hydrocarbon initial stock in using carbon dioxide. Note here that said carrier comprises carbonate of, at least, one alkaline-earth metal selected from the group consisting of Ca, Sr and Ba.

EFFECT: catalyst facilitates reaction of gaseous hydrocarbon initial stock with carbon dioxide and efficient production of hydrogen and carbon monoxide.

8 cl, 8 ex, 1 tbl, 2 dwg

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