JPS60243032A - Conversion of hydrocarbon by zeolite nu-1 as catalyst - Google Patents

Abstract

(57) [Summary] This bulletin contains application data before electronic filing, so abstract data is not recorded.

Description

DETAILED DESCRIPTION OF THE INVENTION The present invention relates to a process for converting hydrocarbons using a zeolite material designated as zeolite nu(nu)-1 as a catalyst.

Zeolite Nu-1 used in the present invention is separately disclosed in Japanese Patent Application No. 51-117053 (Japanese Unexamined Patent Publication No. 52-1453).
The application has been filed as No. 99. As described in the same specification, Zeolite Nu-1 contains a silica source; an alumina source; and a methylated quaternary ammonium compound and/or its cationic decomposition product and/or a methylated quaternary ammonium compound. The resulting mixture is prepared from a synthetic mixture containing, for example, a mixture of trimethylamine and methanol (instead of which the corresponding phosphonium compounds may be used).

Zeolite Nuu 1 has a composition in the following range from 0.9 to
1.3 R20-Al2O3・20~15[]sio□
・0 to 40H20 (where R is hydrogen, ammonium, phosphonium, or 1/n of n-valent metal cations, and fc is more than 1)'lf: and when R is hydrogen, It has an X-ray diffraction pattern substantially as shown in Table 1.

The above definition includes Zeolite Nu1 in its as-prepared state (prepared!, ox state means the product that has undergone a synthesis reaction and a washing and optionally drying process) and dehydration and/or calcination. and/or ion 1
It includes New 1 in the form obtained by conversion.

In the prepared state of neutron 1, R is ammonium or phosphonium (hereinafter referred to as Q) selected from methylated quaternary ammonium and methylated quaternary phosphonium and their cationic decomposition products. , or such as ammonium or phosphonylamla, and may contain alkali metals, especially sodium. Although a certain portion of Q20 in the as-prepared Nyu-1 dissipates and some of it may be trapped in the zeolite structure, this more Q10 is It does not constitute part or all of the composition. The proportion of Q10 is typically A1□0
The amount is in the range of 50.5 to 2.5 moles per mole.

Preferably, the silica:alumina ratio is at least 4o.

Table 1 d(A) 100I/IOd(A) 100I/IO8
,8718'3.965 73 8°28 69 3.845 74 6.53 43 3.81 22 6.19 75 3.687 16 4.43 52 3.508 29 4.30 51 3.256 27 4.08 37 2.858 15 4.03 , 100 The H20 content of the prepared trench condition ♀Nuu 1 depends on the conditions under which it was dried after reaction.

In the calcined form of New 1, R can be an alkali metal but contains little or no ammonium or phosphonium compounds.

The reason for this is that these compounds burn out in the presence of air, leaving hydrogen as the equilibrating cation.

Among the ion exchange forms of New 1, ammonium (
The NH4'' form is important because it can be easily converted to the hydrogen form by calcination. The hydrogen form and forms containing metals introduced by ion exchange are discussed further below.

The takes shown in Table 1 include estimated measurement errors and are subject to certain ranges common in zeolite production due to ants, impurities, changes in the R cations involved, and variations in the microcrystalline structure within the main structure. It represents the change in -.

More specifically, the d spacing in Table 1 can range from +4% to -2%. The zeolite may contain a combination of new forms from a range of different d-spacings, and in some forms the 6.5-6.6 A line bifurcates into two. Sometimes. The attached figure shows a high d-spacing type with branched peaks.

Reference example related to hydrogen form 1. The data in Table 1 shown in
6 Of those lines, d (
A) The 194 line is fixed with the impurity kenyite, 617
and 6.19 lines were fixed with dalite.

Zeolite Nu-1 is further characterized by the dye adsorption properties described below.

(Al Cationic Dyes Acrifurapine None Phenosafranine 1゜Methyl Red Very Strong Torylene Red None b) Other Dyes Alizarin Weak Aralin None Aluminone None Without TMA The adsorption was further characterized by each individual6. Lower F
(7) %W/W e, arrival i (P/PO= 0.5
) was measured for hydrogen form Nyu 1 in the diagnostic example, and is considered to be typical.

The slow adsorption of P-xylene means that although Nu-1 has an internal cavity large enough to accommodate P-xylene, the entrance hole to such a cavity is small (approximately 6.0
1).

From Table 2, it is clear that Zeolite Nu-1 adsorbs 1.5 to 4.0 times more water (by weight) than n-hexane. Therefore, Zeolite New 1
Although it is considered to belong to the class of so-called hydrophilic 1 zeolites, its silica:alumina ratio can exceed 6D, and this value therefore suggests a hydrophobic behavior (i.e., it adsorbs n-hexane more than water). It is at the same level as the value previously disclosed as characterized by

NuU 1 in its hydrogen form is characterized by high activity towards xylene isomerization and ethylbenzene conversion reactions and selective catalytic properties against xylene disproportionation reactions.

In producing Zeolite New 1 used in the present invention, at least one silica source;
and at least one methylated quaternary ammonium compound or methylated quaternary phosphonium compound; and an aqueous mixture having the following molar composition:

5102A1203 At least 10, preferably 20
~200, especially 40-100, Na O/Si0 0-0.4, especially l: 1.05-0
．． 25,2 (Na20-1(:120) AI0201-60, preferably 0.1-0.5, especially 0.2-03 H2O/'(Na20-I-Q20) 5-500, especially 100- 300, Q2o/(Na20-FQ20)0.
05-1.0, especially 0.4-0.7, where Q is methylated quaternary ammonium or methylated quaternary phosphor, =
ram, and N a 20 and Q20 are free N a
Only 20 and 020 are shown. “Free NazOJ” and “free Q20” generally refer to the hydroxide form;
Examples of extremely weak acids in which a20 and Q20 are effective in the zeolite synthesis reaction refer to the salt form of aluminic acid or silicic acid. When water glass is used as the silica source, free NaO and/or Q20
The content of can be reduced to the above-mentioned range by addition of acids or by addition of Q in the form of alumina or antacid salts (for example sulphates, nitrates or halides).

The silica source can be any perilla source commonly considered in the zeolite industry for zeolite synthesis. For example, powdered solid silica, silica, colloidal silica or fused silica. Among the powdered silicas that can be used, mention may be made of precipitated silicas, especially those prepared by precipitation from alkali metal silicate solutions. Examples of such products include AKZ O's rxs300J and similar products, Aeronor Silica, Fume 5i
lica ) and silica gel (preferably of the grade used as reinforcing pigment for rubber or silicone rubber). Colloidal silica of various particle sizes can be used, such as those of 10-15 microns or 40-50 microns sold under the trademarks rLUDox, rNALcOAJ and rsYTONJ.

Dissolved silica that can be used includes alkali metal dispersion 1
Commercial water glass containing 0.5 to 6.0 mol per mole, especially 2.0 to 4.0 mol of 3102; British Patent No. 119325
"Act" as defined in No. 4 Specification
ive) J alkali silica salts; and silicates made by dissolving Noriyoku in alkali metal oxides or quaternary hydroxides as a preliminary step in the preparation of synthetic mixtures.

Sources of alumina are most commonly sodium aluminate, but also aluminum salts (such as chlorides, nitrates or sulfates) or alumina itself (preferably colloidal alumina, punidoboehmite, boehmite, comma alumina). , trihydrated alpha alumina or trihydrated beta alumina, which should be in a hydrated state or in a hydrated state, or the like.

At least a portion of the alumina in the reaction mixture for the NuU 1 synthesis may be provided in the form of one or more aluminosilicates. The aluminosilicate compound accounts for at least 20% of the alumina source, especially from 50 to 1
Preferably, 00% is provided. If the aluminosilicate compound contains sufficient silica, it may provide all of the silica power source. However, zeolite
Since the silica:alumina ratio of New 1 is much higher than the silica:alumina ratio of commercially available aluminum aluminosilicates, an additional source of sonic power is usually included in the reaction mixture.

Aluminosilicates may be synthetic or natural. When it is synthetic, it may be, for example, a crystalline compound (eg a zeolite), an amorphous compound (eg a gel or zeolite precursor) or a silica/alumina cranking catalyst. When it is a natural product, it may be, for example, kaolin (particularly 50% kaolin).
Clays such as metakaolin (in the form of metakaolin) calcined at 0-950 DEG C., especially 530-600 DEG C., or 1 t or more of attapulgite, diffukite, hallosite, illite or montmorillonite. Natural zeolites can be used if desired. Substances (natural or synthetic) such as nepheline and calunlite may also be used. In constructing the reaction mixture, reactants such as water and alkali metal compounds introduced as part of the aluminosilicate material should also be taken into account, and preferably reaction-interfering constituents such as Group I element compounds should be taken into account. should be virtually non-existent. The aluminosilicate compounds used may be those made by treating corresponding compounds containing interfering cations with acids''!, or with non-interfering cations. The aluminum may be removed by removing the aluminum.

For the use of aluminosilicate starting materials, such starting materials can be prepared as shaped granules (in particular with diameters of 1 to 1
(in the form of approximately spherical particles of cylindrical compressed pellets with 0 cavities or in the form of extrudates with a diameter of 2 to 10 bodies and a length of 5 to 20 mm)
Modification methods to be introduced become possible. and silica content,
The loading and the time can be selected such that the conversion to zeolite Nu-1 takes place only in the outer part of the particles. By this method Zeolite Nu-1 can be obtained directly on pre-formed particles, obviating the agglomeration process required to produce such particles from powder. force)
Typical conditions for the modified method are as follows.

SiO3/Al□03 12-25 Temperature 150-200°C Time 1.5-60 days Water content of the reaction mixture is 500% per mole of A1□03
The amount is preferably 1,000 to 4,000 moles or more.

The relative proportions of QO and Na 20 can be selected in relation to the desired sodium content of the produced zeolite; the lower the sodium content, ie the need for ion exchange, the lower the proportion of Na 20. The preferred range of 0.4 to 0.7 is generally useful in the production of zeolites requiring moderate ion exchange treatment, yet does not incur the costs of high proportions of O20.

The reaction should be continued until the zeolite product contains at least 50% W/W (but not beyond that point). Such time depends on the temperature and relative concentrations of the reactants, and on whether the reaction mixture is allowed to stand or is stirred. If the reaction time is exceeded, then Zeolite Nu-1 may transform into other substances. Preferably, the progress of the reaction is followed by sampling the mixture at intervals and testing it at intervals. A typical reaction time is 12
The reaction temperature is suitably from 80 to 600°C, preferably from 165 to 280°C and especially from 150 to 250°C.

In addition to the components already mentioned, the reaction mixture may also contain crystal-seeding zeolites and mineralizing agents, such as sulfates, nitrates or halides of alkali metals. Such mineralizing agents. (ri, which may be added as such or formed in situ by reaction of an alkali metal hydroxide, aluminate or silicate with a suitable acid or quaternary or aluminum salt) Good too.

Upon termination of the reaction, the solid phase is collected on a filter, washed, and the solid phase product is then ready for subsequent treatments such as drying, dehydration and ion exchange.

If alkali metal ions are present in the reaction products, they must be at least partially removed in order to produce the hydrogen form of Nu-1, and such removal can be accomplished using an acid, especially a strong acid such as hydrochloric acid. This can be done by ion exchange using a solution of an ammonium salt such as ammonium chloride, or by using an ammonium compound prepared by ion exchange using a solution of an ammonium salt such as ammonium chloride. Such ion exchange can be carried out by slurrying with an ion exchange solution once or several times (such treatment may be referred to below as slurry exchange). Zeolites are usually calcined after ion exchange, but may be calcined before or during the steps.

In general, the cation of Zeolite New 1 is any metal cation, especially 1A, IB, IIA, ■B, l1l
(@Rareto M), Vll-A (including man-in)
Vllll (gold medal metals) group metals and substituted by lead and bismuth. (Here, the periodic table is based on that described in Abridium of Specifications 1 published by the British Patent Office).

To produce the catalyst, zeolite Nu-1 can be introduced into an inorganic matrix together with other substances, inert or catalytically active. The inorganic matrix may simply be present as a binder to hold the small zeolite particles (0.05-10 microns) together, or the reaction rate may be too high without the addition of a diluent and excessive carbon deposition may overwhelm the catalyst. It is added as a diluent to reduce the amount of reaction in reaction processes that may cause contamination.

Typical inorganic matrices and 1. So, alumina, silica, kaolin clay, bentonite, montmorillonite,
Sepiolite, attapulgite, Fuller's earth, synthetic porous materials (e.g. 51o2-A12o3゜5iO2-Zr
O□, 5iO2-The2.5iO2-Bed.

SiO□-T x O2'E or any combination of these chlorides. An efficient method of mixing Zeolite NuU 1 and such a diluent is to mix the appropriate aqueous slurries together in a mixing nozzle 12 and then spray dry the mixed slurry.

Other mixing methods also used1. sell.

Zeolite Nu-1, in either cationic form or in the form of a catalytic complex, can be used as a hydrogenation/dehydrogenation component (e.g.
Ni, Co, Pt, F'd, He, Rh)
Hydrotacking and reforming catalysts can be produced by replacing or impregnating with. (Particularly preferred when the Na 20 content is 0.03% W/W).

A preferred method of hydrocarbon conversion according to the invention is to convert an alkylbenzene or a mixture of alkylbenzenes into a catalyst consisting of Zeolite Nyu 1 (especially Zeolite Nyu 1 with a sodium oxide content of 0.15% W/W or less in good hydrogen form). and, under isomerization conditions, the gas phase primary is brought into contact with the liquid phase.

Appropriate isomerization conditions in the gas phase include 100 to 60
Temperature in the range of 0°C preferably 200-450° and 05-50 absolute atmospheric pressure (a ta ) preferably 1-5a
The pressure is in the range ta.

Appropriate isomerization conditions in the liquid phase include 0 to 350°C.
Temperature in the range of 1~20 D ata, speed 1° and 5
Pressures in the range ~7 Data and (in fluid systems) 1-100 W/Wy. < is 1
There are space velocities in the range of ~30 W/W/hr (higher space velocities are used at higher temperatures).

Optionally, a diluent may be present, suitably using one or more diluents having a critical temperature above the isomerization temperature, for example toluene, ethylbenzene, trimethylbenzene, naphthenes. and paraffins. Preferably, the diluent, if present, is in an amount representing 1 to 9 Qwt% of the isomerization reaction feed. In the above reaction method, the catalyst is preferably free of hydrogenation/dehydrogenation components. Optionally, the isomerization reaction can be carried out in the presence of hydrogen. Suitable molar ratios of hydrogen:alkylbenzene range from U3:1 to 1,60:1. When using hydrogen, the catalyst is
A mixture of group metals and zeolites is preferable. The Group I metal is preferably platinum. The amount of metal used ranges from 01 to 2 wt% metal based on the total weight of the catalyst. Preferably, the alkylbenzene is a xylene compound (eg m-xylene for conversion to xylene) or a xylene isomer. a mixture (often accompanied by ethylbenzene).

The amount of ethylbenzene present will depend in part on the source of the xylene mixture, but is typically at zero in the feedstock.
1, which may be ~25 wt%, some advanced xylene isomerization processes require limiting the amount of ethylbenzene present in the feed to relatively small amounts (e.g., 6% or less). The reason for this is that above this concentration the catalyst used is unable to decompose the ethylbenzene and the ethylbenzene therefore accumulates in the recycle stream. In the method of the present invention, a relatively large amount of ethylbenzene is lJt [6-25%]
Even feedstocks that are present can be treated similarly to feedstocks containing relatively small amounts of ethylbenzene.

This isomerization reaction is carried out for example by
~10000 ppm preferably 1000-5000
It may be carried out in the presence of water vapor at a degree of ppm.

In each of the examples below, the ingredients had the following characteristics.

Silica AKZO rxs300. , +98.9%5
102゜11%Na 20 Sodium aluminate (formula) 1.25Na20・A1
゜03rTMAOH1 represents tetramethylammonium hydroxide. The solution used is 25% W/W
It contained TMAOH.

Metakaolin C formula) Al□03@2S102 (Kaolin calcined in air at 550°C for 17 hours I).

(made by)

Example 1 Preparation of Zeolite Nu-1 in Na-Q Form The synthesis mixture for its preparation had the following composition.

Al2O3・59ROS], 02” 12.65 Na
2O・10.760+・36.06oH−・3580.
3 H20 solid silica (66v K S 3 n O:
(manufactured by AKZO) with 6927 TMAOH bath solution and 500
1.82% solid sodium aluminate and 8.6% sodium hydroxide were then dissolved in 1152% water. Then, stir and mix into the above silica suspension for 10 minutes. The resulting slurry was heated at 170° C. for 8 days without stirring in a 1 ton Pyrex liner in a 5 ton autoclave. Approximately 60
After cooling to 120°C, the slurry was washed with filtered 12.500°C hot water and dried at 120°C.

The product Zeolite Nu-1 shows the X-ray diffraction data shown in Table 1 (7, its composition is o, 7 Na2O.0
．． 6Q20・A1□03・52 S IO2・6H20
(0-tetramethylammonium), and the crystal size was approximately 5 microns. This product was left in the air for 55 minutes overnight.
Calcinate at 0°C. This calcined product has an X-ray diffraction pattern that is substantially the same as the hydrated tetramethylammonium-containing zeolite Nu-1. Ta.

Table 6.
A) 100I/IOa (A,) 100I/IOK
19.4 2.5 4.01 10011.33 2.
5 3.95' 388.80 8.0 3.83 6
2 8.23 41 3.51 35 6.94 2.5 3.42 24 6.49 32 3.24 11 s-16A7 55 s 3.19 115.6L 1
1 3.08 11 5.34 10 2.98 11 4.41 46 2.94 5 4.28 49 2.85 8 2.76 8 2.73 4 2.67- ' 10 In Table 6, K is Kenyite , S indicates a line fixed at sodalite and 17, s-
1 indicates a Nyu 1 line reinforced by a nearby Ndalite line.

Preparation of zeolite (hydrogen form)-New 1
The slurry was exchanged three times at °C. Each exchange process lasted 1 hour. The product was heated in air at 550°C overnight.
When fired, the first Zeolite New 1 made
Virtually the same as X#! It was found to have a diffraction pattern.

It was found to have a crystal size of approximately 5 microns and to have the following composition:

0, C1I Na20-Al□03-553 io□ This hydrogen form New 1 zeolite has a water absorption capacity (p/p□==o, 7, 25 °C) of 6.5% W/W, and 3 %W/W of n-hexane (P/Po=0.6.
25°C). However, it did not absorb significantly P-xylene. These results indicate that the inlet hole size is at least 5A, but as small as 6 prongs.

Isomerization of Xylene Compounds The hydrogen form zeolite NYU 1 was used as a catalyst for the isomerization of a xylene mixture containing only 7% paraxylene and 11% ethylbenzene. It has been found that the catalyst exhibits a very low degradation rate K and virtually complete and highly advantageous conversion of ethylbenzene to gold diethylbenzene. It was also found that the xylene loss was very low.

An increase in the equilibrium concentration of xylene on zeolite 9 NYU1 was obtained at a temperature of 200 °C, which compared to that on the xylene isomerization catalyst of S 102/A l□03. low.

Example 2 Preparation from a Reaction Mixture with Sodium Content 0.92% sodium aluminate powder and 2.22% sodium hydroxide pellets were dissolved in 100% water. 294g TMA
An OH bath was added to the solution and 182 finely divided phosphoric acid was stirred into it. The resulting suspension was stirred at 60°C for 1 hour and then kept at 170°C in an autoclave for 65 days. The reaction mixture thus had the following molar ratio composition:

S10□/Al2O3 vessel 0; Na2O/5102-01
1; (Na20+Q20)/5102-0,25;H2
0/(Na20+Q20)=250;Q20/(Na2
0+Q20)=05g; where Q is trimethylammonium. After cooling the mixture to room temperature, it was filtered, washed with water and dried in air at 120°C. The resulting fine solid was suspended in a solution of 202 ammonium chloride dissolved in 600 °C of water, and the slurry was exchanged at 50°C for 05 hours. The generated zeolite was filtered and washed with water. At this stage, the sodium content of the zeolite was 14% Na (by weight). This was then calcined at 500°C for 16 hours. Three further treatments with ammonium chloride solution reduced the sodium content to 0.08% Na.

Xylene isomerization yielded pellets consisting of 67% hydrogen form zeolite and 66% pseudoboehmite alumina (25% moisture). 7f pellets were charged to a laboratory scale reactor for xylene isomerization. Mixed xylene raw material (composition is in Table 4)
) was passed through the catalyst pellets at varying flow rates from 10 cc to 15 cc/hr. Three experiments (total of 24 hours in each experiment) were carried out at 450°C. The catalyst showed no loss of activity during each experiment. A 1° inspection of the catalyst at the end of each experiment revealed only very slight carbon deposits on the catalyst. Table 4 shows the composition of the raw materials and the composition of the gas produced in the three experiments.

Table 4 Be/Zen 0.05 0.90 0.71. 0.69
Toluene 0.27. 0.74 0.58 0.60
Ethylbenzene 5,80 4. s 3 464 4.
77 Baraxylene 8.38 18.92 17.94
17.57 meta-xylene 54.77 47.94
48.4748.65 Orthoxylene 29.30 2
5.94 26.4326.54 Aromatic 09 class 0.3
, -0.53-Aromatic C1o 0.05 - 0
．． 05 -n-c9 paraffin 120 Not measured 0
．． 75 The loss of xylenes due to the disproportionation reaction in the unmeasured Tani experiment was about 0.7% based on the toluene produced.In the conventional isomerization reaction method using a silica/alumina catalyst, the loss was usually about 2%. loss occurs, and the activity of such catalysts declines in similar experiments.

Example 6 The xylene isomerization operation of Example 2 was repeated using the same catalyst and under the same conditions, but this time the feedstock contained relatively multineedle ethylbenzene.

The composition of the raw material and the product composition in the two experiments are shown in Table 5.

Table 5 - Benzene -1,311,42 Toluene 0.2'7 C1,59[160n-nonane 1.35 1.09 '1.16 Ethylbenzene 1
2,20 9.46 942 Baraxylene 7.58
16.52 16.47 Meta-xylene 51.27 4
5.18 46.07 Ortho-xylene 2734 24
．． 18 24.86 Aromatic C90,34 Aromatic C□. 0.05 This example shows that feedstocks containing relatively large amounts of ethylbenzene can be treated using a catalyst made of Nuu 1 zeolite. In this case, ethylbenzene decomposes to benzene.

The activity and selectivity of the hydrogen form zeolite Nyu-1 of Example 2 was also superior to that of Nyu-1 Niji made in Example 1. The reason for this is not completely clear, but the following factors are thought to play an important role.

(~ The zeolite of Example 2 has /JS smaller crystal size (the size of most crystals is 1 micron or less)
(b) Relatively low sodium content of the zeolite of Example 2; (C) Modified process; (i) In Example 1, the zeolite was washed, dried at 120°C, calcined at 550°C, and ammonium chloride Slurry exchange with solution and then calcination again, but in Example 2 calcination was carried out only after slurry exchange with ammonium chloride solution; and (11) Example 2
In this case, a higher Q20/Na2O ratio than that used in Example 1 was used.

In the present invention, not only the Zeolite New 1 used in the above Examples, but all Zeolite New 1 within the range defined above can be used as a catalyst. Examples of Zeolite Nu-1 with other compositions are shown below as reference examples.

Discussion Example Preparation of Zeolite Nu-1 in Na-Q form Example 1
However, in this example, the synthesis reaction was carried out using 20 at of nitrogen.
1. without stirring to keep it stationary under a. Ta. The product had the following composition.

0,7 Na20-2.5 Q20-Al□03-52
SiO-10,5H20, approximately 2.0 mol of Q
20 is non-structural and does not include brass in the final configuration. Crystal size was 6-5 microns. The X-ray diffraction pattern was typical of Zeolite Nu-1.

Preparation of the hydrogen form of Nu-1 The above product (1,3% W/WNa20) f::,
The product was mixed with 2 tnl of 5% W/W hydrochloric acid per vol.

The mixture was boiled under reflux conditions for 5 hours. It was then filtered and washed with deionized water. Washing product (0,3% W/
W Na2O) at 0.3 of 60 fnl per 12 solids.
Reslurried in 65% W/W hydrochloric acid and maintained at 50 °C for 1 hour, then filtered, washed with deionized water and dried. The dry product wJH contained 0,019% Na of the order of 20 Then, it was calcined at 450° C. overnight 17 to control and burn off the tetramethylammonium it contained without raising the temperature excessively.The composition of the calcined product was as follows.

0.91 Na2o ・A1203 ・50s 102
The adsorption capacity (%W/W) of this product for water, n-hexane, etc. was measured at 25°C and P/Po=0.5, and the following results were obtained.

Water 6.8 Isobutane 0.9 N-hexane 2.7 p-xylene 0 after 2 hours, 1.9 after 24 hours According to these adsorption takes, the pores in the zeolite structure are 6. O
It is determined that the amount does not exceed A.

The X-ray diffraction take of this hydrogen form New 1 is shown in Table 6.

The zeolite sample of this example was more active and selective than that of example 2 when tested as in example 2 and e.

Claims (1)

[Claims] (1) The following general formula % (where R is one or more of 1/n of hydrogen, ammonium, phosphonium, or n-valent cation)
and when R is in the hydrogen form, substantially d(A) 100I/Io d(A) 100I/I. 8.87 18 3.965 73 8.28 69 3.845 74 6.53 43 3.81 22 6.19 75 3.687 16 4.43 52 3.508 29 4.30 51 3.256 27 4. 08 37 2.858 15 4.03 100 A method for converting hydrocarbons in the presence of a catalyst consisting of zeolite Nu-1 having an X-ray diffraction pattern such as: (2) The method according to claim 1, which comprises isomerizing an alkylbenzene compound and uses a zeolite whose only substantial portion is hydrogen. (3) the reactants are present in the gas phase, there is substantially no added free hydrogen, the temperature is in the range 200-450°C, the pressure is in the range 1-5 atm absolute, and the catalyst is hydrogenating. /The method according to claim 2, which does not contain a dehydrogenation component. (4) The alkylbenzene compound exists in a liquid phase, there is substantially no added free hydrogen, the temperature is in the range of 0 to 650°C, the pressure is in the range of 5 to 70 atm absolute, and the catalyst is hydrogenating. /Claim 2 that does not contain a dehydrogenation component
The method described in section. (5) The method according to claim 1, which comprises isomerizing an alkylbenzene compound, R contains a metal from Group 1 of the periodic table, and hydrogen is present. (6) A process according to any one of claims 2 to 5, wherein the starting materials include xylenes and ethylbenzene and the reaction conditions are selected to result in conversion of ethylbenzene.