Title of Invention

"UZM-5, UZM-5P AND UZM-6; CRYSTALLINE ALUMINOSILICATE ZEOLITES AND PROCESSES USING THE SAME"

Abstract

A new family of crystalline alumino-silicate zeolites has been synthesized. These zeolites are represented by the empirical formula. Where M is alkali or alkaline earth metal such as lithium and strontium, R is a nitrogen containing organic cation such as tetramethyl ammonium and E is a framework element such as gallium. They are also characterized by unique x-ray diffraction patterns and have catalytic properties for carrying out various hydrocarbon conversion processes, especially isomerization of aromatic compounds and alkylation of aromatic compounds.

Full Text

BACKGROUND OF THE INVENTION Zeolites are crystalline aluminosiiicate compositions which are mJcroporcus: and which have a three-dimensional oxide framework formed 'from corner sharing A1O2 and SiOa tetrahedra. Numerous zeolites:, both naturally occurring and synthetically prepared are used in various industrial processes. Zeolites are characterized by having pore openings of uniform dimensions, 'having a significant ion exchange capacity, and being capable of reversibly desorbing an 'adsorbed phase which is dispersed throughout the internal voids of • the- crystal without significantly displacing -any atoms which 'iriiake up. ythS .permanent zeolite .crystal structure. The number of synthetic zeolites is well.over a hundred as; evidenced by tne xtlas.. of Zeolite Structure Types published by the Internationa! Zeolite Associa'tiori (IZA). As is well known, zeolites are.distinguisfie'd .frc|rn;each other on tfhe basis of their composition, crystal .structure -and 'adsorption. properties,-One rnethod commonly used in the art to distinguish zeolites is x-ray diffraction, .. 'Applicants have synthesized a family of crystalline zeolitic composition's which have unique x-ray diffraction patterns and have an empirical formula on an. anhydrous bas-is in terms of molar ratios of: where M is at Jeast one exchangeable cation selected from the group consisting' of alkali and alkaline earth metals, "rn" is the mole ratio of i\/1 to (Al 4- h) and varies from 0 to-1,2, R is a nitrogen-containing organic cation selected from the group consisting of quaternary ammonium ions, protonated amines, protonated 'cliamines, protonated alkanolarnin.es, quaternary aikanolammonium ions, V • ' diquaternary ammonium ions, and mixtures thereof, "r" is.the mole ratio.of R to. {Al + E) and has. a value of 0.25 to 3.0, E is an element selected from the group consisting of Ga, Fe, In, Cr, and B, "x" is the mole fraction of E and varies from 0 to 0.5, "n" is the weighted average valence of M and has a value of +1 to +2, "p" is the weighted average valence of R and has a value of +1 to.-t-2, "y" is the mole ratio of Si to (Al + E) and varies from 5 to 12, and "z".is the mole ratio of O t'p (Al;-h E) and has a value determined by the equation: -. (Equatiion Removed) Specific members of this family of zeolites are: UZM-5, U2M-5P an DETAILED PESCRIPTIQN.OF THE INVENTION ; Applicants have synthesized a hew family of zeolites. In its as-synthesized form,: this family of zeolites ..has a composition on. an anhydrous basis that is represented by the formula: . . M is an exchangeable cation and is selected from the group consisting of alkali and alkaline earth metals..Specific examples of the M cations include but are not limited to lithium, sodium, potassium, cesium,- strontium-, calcium, magnesium, 'barium and mixtures thereof. The value of "m" which is the mole ratio of M to (At 4 E)-varies from 0 to 1,2. FJ is-a nitrogen containing organic cation and is selected 'from the group consisting of protonated amines, protonated diamines, protonaied aikanolamines, quaternary ammonium ions, diquaternary ammonium ions, quaternized alkanolammonium ions and mixtures thereof, The value of "r" .'•which is the mole ratio of R to (Al + E) varies f-rom 0,25 to 3.0, The value of "n" which-is; the weighted average vaience of M varies from +1'to '4-2; The -value of "p", which.-is the average weighted valence of the organic cation has a value from'-f 1 to +2, E is an element which is present in the framework and is selected from the group,consisting of gallium, iron,- boron chromium, indium and nnjxtures thereof. The value, of "x" which is the mole fraction-of E varies" from ;0 to 0.5, The ' ratio of silicon to (AkE) is represented by "y" which varies from 5;;to. 12, While -.the '• mole; .ratiO;;.pf O: to._(AI+.E) is represented by "'z" and '" has::a;value given;';t)y-"ttle;./. equation:,.. (Equatiion Removed) VVhen .M Is only one metal, "then the weighted average, 'valence is the: valence of,that one'metal, i.e. +1 -or +2,. However, when more".than, orie lyi metat;- '• :is present; the total,amount of:-' (Equatiion Removed)and the weighted average valence "n" is given by-the equation: (Equatiion Removed)ence is the valence of the single R cation, i,e./.-i-1 .or +2, When more than one R cation is present, the total amount'of R is given by the equation: (Equatiion Removed) arid the weighted average valence "p" is given by the equation: . (Equatiion Removed)These, aluminosilicate zeolites, are . prepared by a hydrothermal: crystallization of a reaction mixture prepared by combining reactive sources of R, aluminum, optionally E and/or M i . nitrate, indium chloride and indium nitrate. When R is a quaternary-ammonium cation, the sources include without limitation the hydroxide, and Halide compounds. Specific examples include without limitation tetramethylammonium hydroxide, tetraethylammoniurn ' hydroxide, hexamethonium bromide, tetramethylammonium chloride, methyltriethylamrnonium hydroxide, R may also •be neutral amines, diamines, and alkanoiamines, Specific examples are triethanolarnine, trtethyfamine, and N>J,N',N' tetramethyl-I.S-hexanediamine.' - The reaction mixture containing reactive sources of the desired components can be described in terms of molar ratios of the oxides by thev forrnufa: where "a" is the mole ratio of the oxide of M and has a value of 0 to 2, "fo" is -the mole ratio of the oxide of R and has a value of 1.5 to 30, "d" is the mole ratio of silica and has a value of 5 to 30, "c" .is the mole ratio of the oxide of E and.-has.a value from, 0 to;'d,-5,;and v"e":;is the mole, ratio of water and has a value of 30 'to1 .6000. The reaction ..mixture is now reacted at reaction conditions Including :a-temperature of 100°C to 175°C and preferably from 140°C to 160°C for a period ' .... ) -of 12 hours to 14 days and preferably for a time of 2 days to 5 days in a sealed reaction vessel under autogenous pressure. After crystallization is complete, the solid,! product is isolated from the heterogeneous mixture by means such as filtration or centrifugation, and then washed with de-ionized water and dried in air at ambient temperature up to 100°C. As synthesized, the zeolites will contain some of the exchangeable or ! ' charge balancing cations in its pores. These exchangeable cations can be exchanged for other cations, or in the case of organic cations, they can be removed by heating under controlled conditions. All of these methods are we!! known: in the art. The crystalline zeolites are' characterized by a three-dimensional - framework structure of at least'SiO2 and AlOa tetrahedra! units. These zeolites are further characterized by their unique x-ray diffraction pattern. The x-ray-diffraction pattern has at least two. peaks: one peak at a c/-spacing of 3,9±Q,12A and one peak at-a-c/-spacing of 8,6±0,20A. To allow for ready reference,, the different structure types and compositions of crystalline zeolites have been given arbitrary designation of UZM-h, where "h" is an integer starting at one and where for example "1" represents a framework of structure type "1", That is one .or more zeolitic. composition with different empirical formulas can have the same structure type "h", e.g. in .this respect,'"the following species can be identified by their.x-ray ;diffractidh patterns" which have at least the; d-spacing and relative, intensities ;set: j (Table Removed) The zeolites, of this, invention .are .capable of., separating mixtures of molecular species based on the molecular size (kinetic diameter): or;on .the ; . • . ' degree of polarity, of the. molecular species. When the separation of .molecular' species is based on molecular size, separation is accomplished by the smaller 1 ' molecular, species entering the intracrystalline void space while excluding larger species. The kinetic diameters of various molecules such as oxygen, nitrogen,' >• carbon dioxide, carbon monoxide are provided in D.W. Breck, Zeolite, Molecular Sieves, John Wiley and Sons (1974) p. 636. The crystalline rnicroporous compositions of the present invention either ias synthesized or after calcination can be used as catalysts-or catalyst supports In hydrocarbon, conversion processes. Hydrocarbon conversion processes are, i well known 'in the art and include cracking, hydrocracking, alkyiation of both aromatics and isoparaffins, isomerization, polymerization, reforming, dewaxing/ • h'ydrogenation, dehydrogenation,. transalkylation, 'dealkylation, hydration, dehydration, . hydrotreating, hydrodenitrogenation, hydrodesulfurization, methanation and .syngas shift .process. Specific reaction conditions and.the types of feeds which can be used in these processes are well,known in the art. Preferred hydrocarbon conversion processes are alkyiation of .aromatics, and isomerizatidn of xylenes, • ; :•••:Other'":feactibns-;may;,be.?eatalyzed by these crYStalline^^rnicrQporpus cornpositioqs,-including 'base-catalyzed side chain alkyiation pfi,alkylaromatiGS, aldo l-cpnderisations,,;.olefirv. double: bond isomerization and; isomerization. of. acetylenes,, alcohol; dehydrogenation, and o|efin dimerization,. oligomerization- ,and conversion;':,of alcohol to.'olefins.. Suitably ion. exchanged.:.forms ofi these; ' ' f mate rials- can catalyze the'; reduction of/NOX to N2.in, automotive and industrial, exhaust streams.. Some, of the reaction conditions and types of .feeds that can;: : be used in. these'processes are. set forth in US-A-5,015.,796 and in H. Pines, TH| CHEMISTRY -OF . CATALYTIC. HYDROCARBON CONVERSIONS,:. i ' " Academic/Press (1981.) pp. 123-154 and references contained.therein. : Although the zeolites can be used alone, it is preferable that the zeolite be mixed with a binder for convenient formation of catalyst particles in a proportion of. 5, to 100 mass % zeolite and 0 to 95 mass-% binder, with the zeolite preferably comprising from 10 to 90 mass-% of the composite. The binder should preferably be porous, have a surface area of 5 to 800 m2/g, and relatively ' refractory to the conditions utilized-in the hydrocarbon conversion process, Non-• limiting examples of binders are aluminas, titania, zirconia, .zinc oxide, magnesia, boria, silica-alumina, siiica-magnesia, chrornia-alumina, alumina-boria, silica-. zirconia, silica, silica gel, and clays. Preferred binders are amorphous silica and 1 alumina, including gamma-, .eta-, and theta-alumina,' with gamma- and eta-alumina being especially preferred. ,..;. . The zeolite with, or without a binder can be formed into various shape's " 'such as pills, pellets, extrudates, spheres, etc. Preferred shapes are extrudates .and spheres. Extrudates are prepared by conventional means which involves .mixing/of zeolitev either before or after adding metallic 'Components, with the :binde;r;and-a-'siuitable;'pe'ptizin'g agent to -form--a homod&hedus'-'dbugh: or'thick'1 paste :having.th§ cprr-eet moisture content to allow for the forrrfattorrof extrudates ' w/ith'. .•aeceptable:,-infegrity -to.-withstand direct calcination:"1' 'The"doiiigh' theri !is extruded through :;a -die to-give the shaped extrudate, A 'muititude of different extrudate-shapes are possible, .including, but not lirnited;to, cylinders, cloverleaf;,d;umbbeli and symmetrical 'and-.asymmetrical pdlylobates;- : It -is also within trie:' scope of this •.invention that the extrudates may be further shaped to any.desired '. fprm,jsuch as sphere's, by/any means known to the art;' ,..„ ..Spheres:can be prepared by the well known oil-drop method which .is described in.US-A-2,620,314 which is incorporated by reference. The method involves; dropping a mixture of zeolite, and for example, alumina sol, and gelling agent into an oil bath maintained at elevated temperatures. The droplets of the mixture remain in the oil bath until they set and form hydrogel spheres. The spheres are then continuously withdrawn from the oil bath and typically subjected to specific aging treatments In oil and an amrnoniacai solution to /further improve their physical characteristics. The resulting aged and gelled particles are then washed and dried at a relatively low temperature of 50-200°G and subjected to a calcination procedure at a temperature, of 450-700°C for a period of 1 to 20 hours. This treatment effects conversion of the hyciroge! to the corresponding alumina matrix.- A platinum-group metal, including one or more of platinum, palladium, rhodium, ruthenium, osmium, and iridium, is an optional component of .the present catalyst but necessary, for isqmerization and alkylation. The preferred platinum-group metal is.platinum.- The platinum-group.metal, component may . --exist within ther.final catalyst composite;,as a compound such as .an, oxide, sulfide,; f.vhaljdevoxysulfide^^ ."more, other ingredients, of. .the, catalyst.: corriposite. It, i.s, believe,^/that the,, best-.;: . results ;are.obtained when substantially .all the platin.urrh.grQup, metalcomponent, , - exists -in a .reduced state. .•,.The platinum-group metal.; component .generally ,. : oompris^s JromVO.01 to. 5 ,rnas$-%;: and preferably .from Q.fatp^g.% of.;thejinal -,-:. ^scatalyst-oQRipJQsite', -calculated on an ejemental basis.., The. platinum-group, metal., component may be ^incorporated .into.,the..,-. xoatalyst co.mposite: in any; suitable ...manner.. One. m.ethod., of preparing, the, " oatalysi involves the utilization.of a.-.water-soluble, .decomposable.compound.of .a, , platinum-group metal to Impregnate the calcined sieve/binder composite. -. . Alterhatively,: a platinum-group metal-compound may be added at the time of i compositing the zeolite and binder. Yet another method of effecting a suitable metal distribution is by compositing the metal component with the binder prior to co-extruding the zeolite and binder. Complexes of platinum-group metals which may be employee! according to the above or other known methods include ;' chloroplatinic acid, chloropailadic acid, ammonium ch'ioroplatinate, bromoplatinic •acid, platinum- trichloride, platinum tetrachioride hydrate, platinum 1 • • i ' dichlorocarbonyl dichloride, tetramine piatinic chloride, dinitrodiaminoplatinurn, ; sodium tetranitroplatinate (II), palladium chloride, palladium nitrate, palladium 'sulfate, diamminepalladium (II) hydroxide, tetramminepalladium (II1) chloride, and ' :the like.-- ' It .is within the scope of the present invention that the catalyst composite may contain other metal components known to modify the effect of thepfa'tihum-- group metsii component.;.:• Such metal modifiers may include rhenium, "tin, • 1 . germanium' '.'.(eadr cobalt,! nickel,' indium, gallium, ^zinc, uranium/: :dysp'rp"s'mrn; ; ^halliump Snd':;niixtU;pes'N,thereof:^ Gatalytically effective ;ambuhts: bFsUGfi;;"mefa:]:j modifiers;may;be.: incbrporated into the' catalyst by any means known" in the art 'fp effect a homogeneous, or.stralified-distribution. The;."catalyst! composite :of the: present invention'may contain a hai.bge'ri" " comppne'nt.:;•J:he.,halogeh-component .may -be either fluorine,; chlorine, 'bromine aa iodine or /mixtures' thereof, ^with.chlorine.; being'preferred.:; The h'.alogen" /.component is' generally-pre'sent :in a combined state with the inorganic-oxide: .suppbrt. :;.;;;^her' optional "halogen component is preferably weli-;dispeVsed'; throughout ,th:e -catalyst and may comprise- from1 mo.re than -0:2 to 15'wt.'%',' '[ -, ' " " ' ' ' ' -• • calculated on an-elemental basis, of ;the final catalyst. .The halogen component'1 may be incorporated' in the. catalyst composite in any suitable manner,'either ' during, the preparation of the inorganic-oxide support or before, while or after other catalytic components are incorporated. i ne catalyst composite is dried at a temperature of from 100° to 320°C for a period of from 2 to-24 or more hours and, usually, calcined at a temperature of . from 400°to 650°C in an air atmosphere for a period of from 1 to 10 hours until alkylaromatic hydrocarbons;, of the general formula C6N(6:njRnv\where n.,'is .an-v I • integer from 1 to 5 and R is CH3, C2H5, G3H7, or C4H9, in any combination and including all the isomers thereof to-obtain more valuable isomers of the . alkylaromatic. Suitable alkylaromatic hydrocarbons include without limitation* ortho-xyiene, meta-xylene, para-xyle.ne, ethylbenzene, ethyltoluenes, tri-methylbenzenes, di-ethylbenzenes, tri-ethyl-benzenes, methylpropylbenzenes, ethylpropylbenzenes, di-isopropyibenzenes, and .mixtures thereof. . Isomerization of a C8-aromatic mixture containing ethyibenzene and xyienes is a particularly preferred application for the zeolites, of the invention. Generally such mixture will have an ethylbenzene content in the approximate .fange of 5 to 50 rriass-%,"an ortho-xylene content in the approximate range'of.0 to- 35. mass-%, a--meta-xylene content in the approximate range of 20 to 95 mass-% and-a para-xylene content in the approximate range of 0 to 15 mass-%. l.t is preferred that the aforementioned C8 aromatics comprise a non-equilibrium mixfurey i.e., at least one Cg-aromatic isomer is present in a concentration "that : differs substantially (defined herein as a difference of at least 5 mass-%'.of the ' -totat Cj} aromatics')'- frbm the thermpdynamic equilibrium concentration of that" is'omer'atyisbmenfatibh cbhditibhs: • Usually the non-equilibrium'mixture is prep'ared""by' remoVaTbf 'para-'and/or ortho-xylene fr'om a'fresh' C3 aromatic • The alkyli'fo.rhatic; hydrocarbons may be utilized in the present invention as found, in appropriate^^ fractions from various -refinery petroleum streams, e.g., as inciividual'cbrripbhents. or' as. certain boiling-range fractions obtained by the selective fractibhatibn and distillation of catalytically cracked or reformed hydrocarbons. The Isome'rizabie aromatic hydrocarbons need not be •' concentrated; 'the process bf this invention allows the isomerization of ,! alkylarbmatic-containing streams such as catalytic reformate with or without subsequent aromatics extraction to produce specified xytene isomers and partieuiarly to produce para-xylene. A C8-aromatics feed to the present process may contain nonarornatic hydrocarbons,'i.e., naphtheries and paraffins, in an amount up to 30 rnass-%. Preferably the isomerizable hydrocarbons consist •essentially of arornatics, however, to ensure pure products from dovynstream .'.recovery processes. According to the process of the present invention, an aikylaromatic : hydrocarbon, feed mixture, preferably in admixture with hydrogens is contacted .with a catalyst of the type hereinafter described in an aikylaromatic hydrocarbon isomerizatio.n zone. Contacting may be effected using the catalyst.in a fixed-bed system, a moving-bed system, a fluidized-bed system, or. in .a batch-type ..operation; In view of the danger of attrition loss of the valuable catalyst,and of. . :the.sifT!p[er operation; .it is preferred to use a fixed-bed, system. In this system,.;a ; /•hyd.rpgenrriqri/gas; and the feed, mixture a^ •-. to :thS:.desired- reaction .temperature.and thenipassed into.-anp.isomerization-zon.e : -Containing, :a -fixed: bed;.of catalyst./, The conversion• zone.;• may be;,one or more -. separate reactors-with sijitable means therebetween;to ensure that the desired isqme'rizatioa temperature\is maint.ained at. the entrance;:;to/-each-.zone.- ..The',-;. • reactants .may ibe.'cpntacte.d1 with the catalyst bed in either^upwardTV;.downwa;rd?i:;.' or: radial-flow ;fashion,,.and..the.,reactants,may. be in the .liquid phase, a mixed. • ;•••.-•• ^ li.g.uidrVapor'phase,.or a vapor.phase,. when contacted withIhe.eatalyst, The aikylaromatic feed mixture.-preferably. a non-equilibrium mixture-of G8. .arpmlatics, is contacted with,the.isomerization catalyst,at suitable aikylaromatic- ' ' isomerization cohditions. Such conditions comprise.a temperature ranging-from 0° to.:600°C or more, and preferably is in the range of'from 100° to 500°C. The pressure generally is from 101 to 10132 kPa (1 to 100 atmospheres absolute) preferably less than 5066 kPa (50 atmospheres). Sufficient catalyst is ' contained in the isomerization zone to provide a liquid hourly space velocity with • respect to' the hydrocarbon feed mixture of from 0,1 to 30 hr~1; and preferably 0.5 to 10 hr"1. The hydrocarbon feed mixture optimally is reacted in admixture with hydrogen at a hydrogen/hydrocarbon mole ratio of 0.5:1 to 25:1 or more. Other inert diluents such as nitrogen, argon and light hydrocarbons may be present. .., The reaction proceeds via the. mechanism, described hereinabove, of .isomerizing xylenes while reacting ethylbenzene to form a xylene mixture via conversion to .and reconversion from naphthenes. The yield of xylenes in the product thus is.enhanced by forming xylenes from ethylbenzene. The loss of C8 ' arpmatics through.the-reaction thus is low: typically less than 4 rhass-% per pass of G8, arornatics.ih the feed tg. the.reactor/ preferably 3 mass-% or less, and:mbst : preferably.ho more^thah;2>:5::mass\-%:;VV / ,, .;!; • 'The particular :Seheme'•••'employed to -recover: 'an isomerized' product frdm' i the ^effluent of the reactors of the isomerization zone;is not deemed to be critical • j •••••• . to the. .instant invention, and any effective recovery'scheme known in the art may' be; used; Typically, the. reactor effluent will be condensed and the hydrogen ahd: Ali^h^hydrocarbon, components removed: therefrom by flash separation.' The condensed liquid product then is fractionated to remove light and/or .heavy' • :,^yp;r(Dducts and' obtain the isp'merized 'product. In some Instances, certain product species such as ortho-xylene may be "recovered from the .isomerized i product by . selective fractidnation. The product from isomerization of CQ aromatics usually is processed to selectively recover the para-xylene isomer, optionally by crystallization. Selective adsorption is preferred using crystalline alurninosilicates according to US-A-3,201,491. Improvements and alternatives within the preferred • adsorption recovery process are described in US-A- 3,626,020, US-A-3,696,107, US-A-4,039,599, US-A-4,1-84,943, US-A-4 ,-381,419 and US-A-4,402,832, N In •& separation/ispmsrization process combination relating.. to the processing of combined .-with isomerized product comprising CB aromatics and naphthenes from the isbmerization reaction zone and fed to a-para-xyleneseparation zone;. the para-xylene-depleted stream comprising a non-equilibrium mixture 'Of- C8 aromatics is fed to the isomerization reaction zone, where the Ga-aromatic isomers are "'isomerized to near-equilibrium levels to obtain the isomerized product. In this process scheme non-recovered Ca-aromatic:/isomers preferably 'are recycled to extinction until they are either converted tO'paVa-xylene'or lost.' due:t6's1de-reac1i6ns-;' Oriho-xylene separation, preferabiyr6y^ra^tibna1io'n,-;iisQ/: may^be effectidi:onf:the fresh 'C8-aromatic feed or isomeri2dd;pro:duct, :6vf.botrY:iri" cornbihatiori, prior to para-xylene separation. the alkylatibn and preferably the mbnoalkylation of aromatic compounds involves reacting an aromatic 'compound with ari' olefin using:;the above' described zeoiitic fcatalys't. The olefihs which can be used in the process are-any"" of those which cbntaih frorfi 2 up to 20 carbon atoms.'.These"oliefins rhay.be branched or linear oiefihs and either terminal or internal olefins. •'• Preferred olefihsi are jethylene, propylene and those olefins which are known as detergent.range .. oiefins. Detergent range olefins are linear olefins containing from 6 up through 20 : 'carbbn atoms which have either internal or terminal double bonds. Linear, blefins containing from 8 to 16 carbon atoms are preferred and those containing from 10 up to 14 carbon atoms are especially preferred! The alkylatable aromatic compounds may be selected from the group consisting of benzene, naphthalene, anthracene, phenanthrene, and substituted derivatives thereof, with benzene and its derivatives being the most preferred i aromatic compound. By alkylatable is meant that the aromatic compound can be I alkylated by an olefinic compound, The aikylatabie aromatic compounds may-have i one or more of the substituents selected from the group consisting-of alkyl groups (having from 1 to 20 carbon atoms), hy.droxy! groups, and alkoxy groups .whose alky! group also contains from, 1 up to 20 carbon atoms. Where tha substituent is . an 'alky! or alkoxy group, a phenyl group can also can be substituted on the alky! chain. Although ..unsubstituted. and monosubstituted benzenes, naphthalenes, - . anthracenes,..,and phenanthrenes are most often. used in the ^practice of this; invention, rpqlys;wbstituted aromatics -also .may be. employed.. - ^camples of suitable^ . al,kylatab!e.aro.matic,cornp'ounds.in .addition to those .cited above include 'bipfteriyj,. toluene,. .;xylener .ethylbenzene, .propylbenzene, butylbenzehev-s.pentyib.enzene.,;; hexylbenzene-heptylbenzene, octylbenzene, etc.; phenol, cresoiv ariis^le, e'tPioxys propgxy-, butoxy-, pentoxy-,. hexoxybenzene, etc. The ••particular: conditions' under ..which the monoalkylation ^reaction ^i^'1' conducted .depends, upon the, aromatic compound and the olefin used. .'One necessary, condition is that, the .reaction be conducted under- at least partial liquid. •• phase conditions.. Therefore, the reaction pressure is adjusted to maintain the ' . ' olefin ;at least partially dissolved in the liquid phase. For higher olefins the reaction may b'e conducted at autogenous pressure. As a practical matter' the pressure normally is in the range between 1379 and 6985 kPa (200-1000 psig) but usually is in a,range between 2069-4137 kPa (300-600 psig). The alkylation of the alkylatable ' aromatic compounds with the olefins in the C2-C20 range can be carried out at a .temperature of 60°C to 400°C/and preferably from 90°C to 250°C, for a time : : sufficient to form the desired product, .in a continuous process this time can vary ;.. considerably, but is usually fronrQ.'i to 3 hrVeight hourly space velocity with i • respect to the oiefin. In particular, 'the alkylation of benzene with ethylene can be carried out at temperatures of 2QQ°C to 250°C and the aikylation of benzene by "propylene at a temperature of 90°G to 2QO°C, The ratio of alkylatable aromatic •compound;to oiefin used in the instant process will depend upon the degree of .selective, monoalkylation desired as well as the relative; costs of the aromatic and plefinio components of the reaction mixture. For alkylation of benzene by prdpylene, benzene-to-olefin ratios may be as.low as 1 and as high as 10; with a ratio of 2:5-8 being preferred/,;. Where benzene is':alkyiated with ethylene a ::benzene-toiolefin ratio between;- 1M -and'; 8:1 Js preferred: " For 'detergent ;ra'nge'" olefins of C6-G20; a benzene-to-olefin ratio'of between 5:1-up to--as high as 30;fls: ^generally sufficient, to ensure the: desired monoalkylation selectivity; with; a range1, . between 8:1 and 20:1 even more preferred., •/The zeolites.^of this invention can also.be used to catalyze 'transalkylati.dnV. B^.: "transalkylation" is'meant that process where an alkyl:grqup..;qh-bne aromatic nucleus.is-intermojecularly transferred to a second aromatic nucleus.-; A preferred . transalkylationvprpcess is one where one or more alkyl groups-of a polyalkylated' . aromatic compound is transferred to a nonalkylated arornatic;cbmpound, and is' - ',' ! •' ' " • ' exemplified by reaction of diisopropytbenzene with benzene to give .two molecules of cumene. Thus, transalkylation often is utilized to add to the selectivity of a ' 1 ! - - desired selective monoalkylation by reacting the polyafkylates invariably formed during alkylation with nonalkylated aromatic to form additional monoalkylated precincts. For the purposes of this process, the polyalkylated aromatic compounds * are those formed in the alkylation of alkyfatable aromatic compounds with olefins .;as described above,.and the nonalkyiated-aromatic compounds are benzene, .naphthalene, anthracene, and phenanthrene. The reaction conditions 'for i transalkylation are similar to those for alkylation, with temperatures being in the i'ange of 100 to 250°, pressures in the range of 6985 to 3447 kPa (100 to 750 ;psig), and the molar ratio of unalkylated. aromatic to polyalkylated aromatic in the range from 1 to 10. Examples,of poiyaikylated aromatics which may be reacted with, e.g., benzene .as. the ,nonalkyiated aromatic include diethylbenzene; diisopropylbenzene, dibutylbenzene, triethylbenzene, triisopropylbenzene etc. v :; -The .X-ray patterns presented in the following examples (and tables :' ab'ove,) were-obtained.using,standard Xrray.powder diffraetion techniques. -'The ' radiation source was r.ad-ia-tipn "spufce-^ ..The;.'diffraction .pattern' from, the copper alpha-radiation was obtained1 'by = , ..appropriate - computer jbased 'techniques. : Flat compressed' powder samples were continuously scanned at 2° (28) per minute from 2° to 70°(2e). "InterplariaV ' .;..spacings,(d)'in Angstrom units were obtained' from the position-of the diffraction .peaks' expressed as 20 where 6 is the Bragg angle as observed'-from digitized: ;. ' data. Intensities were determined from the integrated area'of 'diffraction peaks ... . " after subtracting background, "I0" being the intensity of the stro'ngestline or peak, , and:'T';being the intensity of each of the other peaks. ' As will be understood by those skilled in the art, the. determination of the , ,cal error, which in combination can impose an uncertainty of ±0.4 on each reported value of 20 and up to, ±0.5 on reported values for nanocrystalljne materials. This uncertainty is, of course, also manifested in the reported values of the d-spacings, which are alculated from the 0 values. This imprecision is general throughout the art and is not sufficient to preclude the differentiation of the present crystalline materials '.from each other and from the compositions of the prior art, In some of the X-ray patterns reported, the relative intensities of the c/-spacings are indicated by the notations vs, s, m and w which represent very strong, strong, medium, and i weak, respectively. In terms of 100 X !/!0, the above designations are defined as w:= 0-15; m = 15-60; s = 60-80 and vs = 80-100. In certain instances the purity a synthesized product may be assessed with reference to its X-ray powder : diffraction pattern. Thus, for example, if a sample is stated to be pure, it is 'iritended only that the X-ray pattern :of the sample is free/of lines attributable to . : -crystalline impurities"; not that there are no amorphous materials .presents In order: to more fully illustrate the invention; the following examples are ".set-forth. It is to be- understood that the-examples are only by way of illustration;/; ';:and are ndt:intended as an dndue limitation on the broad scope of the invention . 'as set forth in:the appended claims.- . .. An aluminosilicate reaction mixture was prepared in the following manner. 'Aluminum sec- butoxide (95+%), 58.75 g, was added to 836.34 g TEAOH (35%) with vigorous stirring. To this mixture, 294.73 g colloidal silica, (Ludox AS-40, ' 40% SiO2) was added, followed by the addition of 10.18 g distilled water. The rea'ction mixture was homogenized for 1 hr with a high-speed mechanical stirrer, -. and then aged in teflon bottles overnight at 95°C. After the aging step, the reaction mixture was recombined and analyzed, the analysis indicated a silicon i content of 4.67%. 50,0 g portion of this reaction mixture was treated with TMACI solution consisting of 11.77 g TMAC'i (97%) dissolved in 23.0 -g distilled water while applying vigorous mixing. After a naif-hour of homogenization the reaction mixture-was distributed among 8 teflon-lined autoclaves. The autoclaves were all placed in ovens set at 150°C, where the reaction mixtures were'.digested for 4 days •' at autogenous pressures. The solid products were recovered by centrifugation, washed, and dried at 95°C. . The composition of the isolated products consisted.of the mole ratios. Si/AI = 6,88,--N/AI = 0.83 and C/N = 6.05... Scanning-Electron Microscopy (SEM) showed the crystallites to consist of clustered platelets approximately 100 - 300 nm.across. Gharacterization. by powder X-ray diffraction (XRD)-showed the line's in .the.-, -pattern;, tp be those for the material designated :UZM-5 Table, 1-below shows, lines, characteristic of the .phase. A portioh.-of the sarriple-was calcined by ramping to,540°C at.2°C/min in ;N2, holding at 540°C in N2 for 1hr followed by a i ' .. 7 hr.dweli ,in air, afso at 540°C. The BET surface area was found to be 530 m2/g .and.the,micropore volume was 0.2cc/g. Table (Table Removed)Example 2 ; An aluminosilicate reaction mixture was prepared in the fpllowing manner. Distilled water, 876.65 g was used to dilute 846.25 g TEAOH (35%) solution. Aluminum sec-butoxide (95+%), 49.54 g was added with vigorous stirring. This was.followed by the addition of 427,57 g of TEOS (98%). The reaction mixture was heated to 85°C overnight and then distilled to 95°C for 2 hr to remove solvent.' The reaction mixture was allowed to cool and was found to contain 3,34% Si by elemental analysis. A 300 g portion of this reaction mixture was i • placed-in a teflon beaker and mixed vigorously. A solution containing 3.8 g TMAG1 (97%), 0.3 g LiCI, and 1.!'g Sr(NO3)2 dissolved in 25 g distilled water was prepared and added slowly to the aluminosilicate concoction with mixing. After the'addition, the reaction mixture was homogenized for 2 hr and then split up i V. . . _ • among, four teflon-lined autoclaves. The autoclaves were placed in a 150°C .. oven, where the reaction mixtures were digested for 5 days at T50°C: at:• . autogenous pressures. The products were Tecombined, the solids isolated by: i . - ..centnfujgation,. washed,; and dried at 95oC Analysislby powderx-ray diffraction showed the product to.have the UZM-5..structure .A .portion of. the product was calcined .under a flow of nitrogen-'for 7: -. \ - .hr at;.5,80.°C;. The composition; of the calcined product exhibited the foilowihg -mole ratios as.determined by elemental. analysis:.Si/AI.= 7.6,' Sr/AI = 0.11, Li/AI = 0,06, The BET surface area of the calcined material wa's-.500':-nn2/g and the micropbre volume was 0.19cc/g. The SEM of the product showed -the crystals to : consist of a rosette morphology, the plate bundles usually on the order of 0.3!to;; : 0.8 p across. Characteristic lines in the x-ray diffraction pattern are shown below i in Table 2, . : Table 2 (Table Removed)Example 3 An. aluminosilicate reaction mixture was prepared by adding 1722 g of' Al(0sec-Bu)3 (95+%) to 470.69 g TEAOH (35%) with .vigorous stirring;;-Oe-ionized water was added, 8.41 g, followed by the addition of 103.67 g of Ludox AS-40 colloidal silica. The, reaction mixture was homogenized for an hour with a high-speed stirrer before it was placed in a teflon bottle and aged at 95°C for 2 35%) with vigorous stirring. De-ionized water, 2.92 g, was added to the stirring reaction mixture along with 698.62 g Ludox AS-40 coiioida! silica. The resulting mixture was homogenized for an hour with' a high-speed stirfer'before It -was placed, in teflon bottles and aged at 95°C for one day, .This alumina-silicate composition, Mixture A, contained 4.96% Si by analysis and a Si/A! ratio- of-9?53.;' v.-Mixture- B was'prebared by diluting 275.23 g TEAOH (SS^^with 275~23 g de-i.pnized water, To this vigorously stirring solution; 107.77 g Ludox AS-40 .colloidal silica and 36.2 g freshly precipitated Ga(OH)3«>xH20, 13.8% Ga; were added. After ap hour of. hompgenjzation, the reaction mixture" was placed':in a .; teflon bottle and aged at 95°O for'three days.'This vgallo'silicate combositiriri '; Mixture B, contained 3.21'% Si by analysis. . •'- - '"•'• •'"• -.-:";The.substituted.aluminosilicate was prepared by cornbihing 45;g'.IVlikture ; A-:wifh;.5,,g: Mixture B. in: a teflon' beaker whi;leyemploying h^h-speedvstirririg' A;:; •• splutipri.prepared'by:.dissolvjng; 1.1:7 9 "^^(-':(^'c^) in i^bvOt-'g" deHbhized wateV.% was :added to -the stirriPg mixture. .After a half-hour' of 'hompg.enizatioh,.^ the'S,was •distributed among-three autoclaves: anfe ^and:;B^a'ys; at1500G:;at autogenous; pre5surpsi-T:he:solid'prQdlj^ts;i;were isolated':'" ;; by ee'rjitrifugatipn, washedjwith-de-ionized water,;and dried'at";9|i°C^ ;.v.;^A!Lthree;, of the products were• shown^tohave"the; UZM-5:-'stmcture'by^;J .powder .x-ray 'diffraction. Elemental analysis -showed the' six day;sample.la'., consist-of the following mole ratios: Si/(AI-fGa)•= 7.35; N/(AWG^) = 1.11; Si/Gia!V';^ = 78.3';' AI/Ga =.: 15.0 and.C/N ='5.44'.. Characteristic lines in the x-ray diffraction pattern* are "given in table 4. days. After it was cooled it- was determined by elemental analysis that the reaction.mixture contained 3,46% Si. A 50 g portion of this reaction mixture was •treated with a. solution of TMACI-(97%), 0.71 g, dissolved in 10 g de-ionized water. The mixture was homogenized for 30 minutes with, a high-speed stirrer » ! arid'then split among 3 teflon-lined autoclaves and digested for 2, 4, and 6. days at; 150°C at autogenous pressures. The solid products were isolated 'by centrifugation, washed with distilled water, and dried at 95°C: The products of the reaction mixtures digested for 4 and 6 days were, shown to be UZM-5 by powder x-ray diffraction. Characteristic lines in the x-ray ' diffraction pattern for the* material observed after-6 days: are given in Table 3. Table 3 (Table Removed Example 4 This 'example, shows the substitution of gallium for some of the aluminum in the structure. Two .separate reaction mixtures, Mixture A, an aluminosilicate composition, and Mixture B, a gailosilicate composition, were prepared. Mixture A was prepared by adding 116.06 g AI(OsecBu)3 (95+%)-to 1982.41 g TEAOH Table 4 (Table Removed. Example 5 An aluminosilicate reaction mixture was prepared by adding 197.31 g A!(0sec-B'u)3 to 2808.74 g TEAOH (35%), followed by the addition of 989..82-,g colloidal silica (Ludox AS-40) while maintaining vigorous stirring, The reaction mixture was aged at 95°C for 16 hr and then allowed to cool. This aluminosilicate reaction mixture was designated Mixture C and was used again in Example 7, Elemental analysis .showed Mixture C to contain 4.79% Si, A portion of this reaction mixture, 110 g, was placed in a teflon beaker equipped with a highspeed stirrer, Separately, a solution was prepared, by dissolving 1.27 g TMAC!' (97%) and 0.68 g Nad in 6 g de-ionized water, This solution was added to the ' stirring aluminosilicate reaction mixture. After a half-hour of homogenization, the reaction mixture was divided among 4 teflon-lined .autoclaves which were ! • '" digested under a variety of conditions. The solid products were isolated'by' . t filtration, washed with de-ionized water, and dried at 95°G. i j The products of all of the reactions exhibited the x-ray diffraction pattern • .of .UZM-5. Characteristic .lines in the x-ray diffraction pattern of a'.sample • digested at 150°C for 4. days are shown in table 5. Scanning Electron ^Microscopy:showed' the. sample to 'be;-very uniform-,; cphsisting of rosettes'.of: i > - : small plate-like crystals with.the ;rosettes 'measuring from 0.5 to 2 p across." :T-he •' .B.ETi surf ace. area'for this material -was- found to be .553'm%; while!the: microp'ore'*' :.volume was -0.22 cc/g. Elemental -analysis-showed :the;:Si/A! ratio 'to be s;97, Na/A;l, = .0,19^ N/AI = 0.97, and. C/N/ =- 5.59. Characteristic lines in the x-ray ' .diffraction pattern for this material are given irvtabJe-5". Table 5 (Table Removed • :, Example 6 An aluminosilicate reaction mixture was prepared-using, the following procedure: Aluminum sec-butoxide (95+%), 987.54 g, was. added-to 14058 g TEAOH (35%) with vigorous stirring. This was followed by the addition of 4954 g colloidal silica, Ludox AS-40. The reaction mixture was aged with stirring at 95°C for 16 hr," After aging, the reaction mixture was found to contain 4.72% Si. This aiuminosilicate reaction mixture was identified as Mixture D, and was used again in example 9. A portion of Mixture D, .47,01 g, was placed in a beaker equipped . with a stirrer, Separately, a solution was prepared by dissolving 1,12 g TMAC! . - . (97%) in 1,87 g de-ionized water. While stirring the aluminosilicate reaction mixture, the TMACi solution was added, and the resulting mixture was further homogenized for 20 minutes. The reaction mixture was then placed in a 100 ml ; 'i ' • • • • Parr stirred ;autoclave. The temperature of the reaction mixture was ramped from - room temperature to 150°C over a period of 3 hr, before it was held at 1500C for 24;hr. The reaction mixture was digested at autogenous pressures. The.solid • reaction product was isolated by centrifugation, washed with'de-ionized water;" and-driedat 1009G. • , :--The-/product exhibited the diffraction pattern :-of UZM-5P The characteristic x-ray diffraction lines for this material are showr .'reaction mixture 'of ;the same formulation, but digested for,72 'hr insfead-bf'24 'hr," yie'lded;;•well-crystallized -\J2M-5. The morphology of UZM-5P was"plate-like: with i - - sub-micron dimensions .as determined by- Scanning- Eleptron •Micrbscibpy; • Elerriental analysis showed:the Si/AI ratio to be 6.0, N/AI = 1.00- Table 6 (Table Removed ' Example 7 ; .A UZM-5P-composition similar to.;,that... disclosed:; in example -6i was . " prepared in: the -following,manner: 40 .g .of. Mixture C (see- ExampI.e 5), was-'used.; as tne;alurninum and silicon source and,was placed in a beaker equipped-with a: high-speed stirrer. Separately, 0,92 g TMACI (97%) was dissolved in 40 g de-- ..ionized water. This solution was added to Mixture G with'yigorbus stirring,.-After ,20 minutes of agitation, the reaction .mixture was placed in a teflon-lined : autoclave and digested at-150°C for,4 days at autogenous pressures, The sdlid-products were isolated by. centrifugation, washed with; de-ionized' -water; :--:and -dried at 95°C . .The product exhibited an x-ray diffraction pattern indicative of UZM-5P,' Characteristic x-ray diffraction lines for this material are given in Table 7. Elemental analysis showed the material to have Si/A! = 6.03, M/AI = 1,07, and C/N = 6,11, Scanning Electron Microscopy showed the sample to consist of clusters of bent plate-like crystals forming rosettes 400 - 800 nm across. Table (Table Removed Example 8 ; An afuminosilicate reaction mixture was prepared in the following manner: TEAQH (35%), 846.25 g, was diluted with 876.65 g de-ionized; water;'Ai(O-secBu)3 (95+%), 49.54 g, was added to the hydroxide solution followed by the addition of TEOS (98%), 427.57 g, while maintaining vigorous stirring: After two hours 'of. hom.ogehizati.on, the reaction mixture was placed in a flask and age'd at: 75°C with light stirring overnight. After the aging, the flask was fitted with a distillation head and some of the alcoholic hydrolysis products were removed via distillation. After solvent removal, the reaction mixture contained 3.34% Si. A 200 g portion of this aiuminosilicate reaction mixture was placed in a beaker equipped with a high-speed mixer. Separately, a solution was prepared by dissolving 15 g TMACI (97%) in 30 g de-ionized water, This solution was added dropwise to the aiuminosilicate reaction mixture and further homogenized for a half -hour. The reaction mixture was then placed in a Parr 2-1 static autoclave equipped with a teflon-cup liner. The reaction mixture was digested at 150°CTor 9Q hrat autogenous pressures. The solid product was isolated by centrifugation, washed with de-ionized water, and dried at 95°C. .The product had an x-ray diffraction pattern consistent.with that of the UZM-5P material, most notably the peaks at d=8.68A and 3.89A. Elemental >: analysis showed the Si/Al-ratio = .10.05, while the BET surface area was 601 :-:rrif/g-;anel the;:-micrbpbre.-. volume '.0.21 cc/g. Scannings-Electron - Microscopy shqwed;:the;' material ter consist 'of uniform clusters-of ;plate-like crystals in a rosette^ form'atioh,' with ; the : -rosettes having a diameter -of 0.25: to'; a'5; µ /Characteristic lines in the "x-ray pattern for this rhateriaT are" given in fable 8. •below. • (Table Removed Table 8 Example 9 A series of zeolites were prepared in a similar manner as the zeolite in . example 6, In a beaker there were placed 47,01 g of mixture D (see Example 6) ar)d to it there was added with stirring a solution of 1.12g TMACl (97%) in T.87g ofide-ionized water. The resulting mixture .was homogenized for 20 minutes and i ' ! - ' " ' then transferred to a 100ml Parr stirred autoclave. Four other mixtures were. iprepared in a similar manner and the respective mixtures were heated to 150°C and held at 150°G for 12 hrs, 18-hrs, 24 hrs,'36 hrs, and 72 hrs under autogenous' pressure, ' Each solid reaction 'product was isolated; by •- ' ' 'centrifugation, washed with de-ionized water and then-dried"at1006C. The. x-ray diffraction .patterns of ..the.five .samples^are. presented in-Table. 9'.::.:-The; data show .that additional, diffraction, Jines are observed.- as 'the amount; of:, digestion ..time is, increased. It is .clear that the. peaks atd ~ 8;6A and: d = 3:9A (in: :' " '- ' . ., bold) are common to all the synthesized materials, i.e.. structures/ ./Without wishing to be' bound by dny particular theoryV the roiiowing .explanation; is proposed; UZiVI-5 can be indexed on. a tetragonal cell with';a;=i.. . 12.41A arid c = 28.6;A. Based, on a tetragonal cells the 8,6A.ahd 3.9A pe.ak's'; ' " r - . t. '- • ' • ' • haveijndices.of 1tO and 310 respectively. This suggest that'ordering: first occurs v in the a and b directions and then in the c-direction. It appears that a- large' i •• • . • • . ..number of structures can be prepared by stopping the reaction at various times > •until-36- hours where the UZM-5 structure is attained. By stopping the synthesis j at various times, one can obtain zeolites with a range of different surface area, . ! ' acidity and adsorption properties. (Table Removed Example 10 ' .An aluminosiiicate reaction mixture was prepared in the following manner: AJ(Osec-Bu}.3 (95+%), 116.09 g, was added to 1983/17 g TEAOH (35%) and • 1.-86g de-ionized water with vigorous stirring. Then 698.88 g Ludox AS-40 .was. added, with continued stirring. After an hour of homogenization, the ! • " ' . "aluminosiiicate reaction mixture was placed in several teflon bottles and aged:at i - • - \ ' - ,,. ./ .„•• . ;. ,-.'.. .95 fC for 3 days. After the aging process, elemental analysis showed the mixture r ' ' to Contain 5.01% Si and had a Si/AI ratio of 10.03. This reaction mixture is designated "Mixture E. A portion of this aluminosiiicate reaction mixture,'40.0 g, was: placed ;in- a .beaker where it was stirred vigorously/ Separately, 0./8 g • i ' • - - TMAGI (97%) was dissolved in 15.0 g.de-ionized water. This solution was added to the stirring aluminosilicate reaction mixture in a dropwise fashion The rriixtute : was allowed to homogenize furtrier for an hour. The reaction'-mixture was then : placed •,in'. a7:teflon-lined autbciave and digested, at :15:0°C for '6 days' at autogenous'pressures; the solid product'was isolated by;centrifugatibh, v^ashed'" with de-ionized.-water, and dried at 95°C i ' , The product had an ••x-ray .pattern consistent with UZM-6: Scannihg- Electrpn Microscopy (SEM) showed the'material to consist of plate-like crystals .,' O.-T - 0.4 u across and less than 0.05 u .thick. The Si/AI ratio of'the pro'ducf UZW- ; 6 wasi8.34 by elemental analysis. The ;BET surface area of the sample was 520 . 4 • - -'•'•. m2/g, with- a micropore volume of 0,21 cc/g. Characteristic lines in "the x-ray diffraction pattern are given in table 10. Table 10 (Table Removed Example 11 An aluminosilicate reaction mixture, was prepared in an identical manner to Mixture E described in example 10. However, the reaction mixture was determined to be slightly different by analysis, with a Si content of 4,79 wt % and a-Si/A! ratio of 9,59. A portion of this aluminosilicate reaction mixture, 1100 g,. -was placed in a large beaker equipped with a high-speed stirrer. Separately, a solution was prepared by dissolving 4.14 g LiCI and 21.43 g TMACI (97%) in 65 g de-ionized water. This solution was added drop wise to the aluminosilicate . reaction mixture with stirring and was homogenized for an hour. The reaction mixture was then transferred to a static 2-L Parr reactor and digested at 150°C for.13'days :at autogenous pressure. The solid product was' isolaied/by filtration, wash:ed-;withpe!-i9hized: water and dried at'95°C.' Powder x-ray diffraction on a sample of the product showed the pattern to \beephsiste-nt.with that for UZM-6. The Si/AI ratio was 7.58: The' BET surface area was 51'2' m2/g, while the micropore volume was found to be O.i'8 cc/g. SEM of.the;calcined product show.ed it to consist of bent plate^crystals,-sometimes:- '. stacked, up to 0.1 - 0.4 p across and less that 0.05 u thick. Characteristic linas in: .:. the x-ray diffraction pattern are given in table 11.Table 11 (Table Removed Example 12 It is: known that zeolites are capable of a .variety of hydrocarbon conversion processes and find much of their utility in this regard. This example 4 [ " demonstrates the capability of UZM-5, UZM-5P, and UZM-6 to convert heptane ( to a; variety of products. Calcined samples of these " materials and for comparison, a steam-stabilized" Y zeolite (SSY) were tested in a microreactor operating at atmospheric pressure. The UZM-5 from example 5 and the UZM-6 from example 11 were ammonium ion-exchanged after calcination to remove alkali and obtain the acid form. The feed was heptane, saturated at 0°C in an H2 carrier gas. The catalyst loading was 250 mg of 40-60 mesh particulates. The samples were pretreated at 550°C for SO minutes in H2. The feed was introduced at a constant flow rate of 125 cc/min. The products were hydrogenated before going to the gas chromatograph. In this variable temperature program, the product stream was sampled at the following temperatures/times on stream:' ,25'^.C/O hr, 450°C/0.33 hr, 500°C/ 1.10 hr and 1.45 hr, and 550°C/2.20 hr .and 2,55 hr. The selectivjties to the major products for each sample are given in Table 12 for the last data point collected at 550°C. The data show that UZM-5," . . . - and.UZM -5P are.corriparable to SSY in ability to convert heptane, while UZM-6 is clearly; much-more active; thah: SSY in heptane conversion.UZM-6 sfiftws • - ' ( much more conversion to; aromatic products than the other rhateriars. Table 12 (Table Removed -Example 13. Another,distinguishing "feature'of zeolites is the ability to adsorb molecules • in their micropores .Such; properties enable the utilityof zeolites in adsorbent 'separation, and selective: catalytic applications. Adsorptioh measurements were performed using a standard McBain-Bakr gravimetric adsorption apparatus. The samples were calcined at 560°C to remove organic templates' before they were loaded into the tubes. The samples were then activated at 350°C overnight to remove adsorbed water from the pores. The samples were then exposed to a gas at several specific partial pressures and the amount of the gas adsorbed is expressed in terms of the weight percent of the sarnpla, The data in the tables below demonstrate the ability of UZM-5 and UZM-5P.to adsorb n-butane, i • ' • isobuiane, O2) and SFS (Table Removed (Table Removed Adsorption of isobutane T = 22°C (Table Removed (Table Removed -Example:14 .Another method for examining .adsorption properties .is. to use TGA or .",'-Thermal Gravimetric Analysis . In such an apparatus,, adsprption, information-at elevated temperatures is easy to acquire, as-well ;as controlled;-delivery'of- the, ' adsorption, .gasses.' This is. especially convenient foKi-ilarger-;-,-le'ssj,volatile': adsgrbates that are more/easily studied and handled at.,highem'tennperatures.; The tests were conducted on calcined, samples. Approximately :50 mg of'sample was'placed in the TGA sample holder. The sample was then activated for 2 hr at 500°;C in.a iM2 stream flowing at 127 cc/min. After the pretreatment, -the-.'sample, was brought to .120°C and an additional feed was cut in consisting of N2 saturated with cis 1,2-dimethyIcyclohexane at 25°C,'which flows at 72 cc/min. Hencev the total flow rate past the sample was 200 cc/min. The adsorption of the cis 1,2-dimethyicyclohexane was then monitored by TGA at 120°"C for an additional 250-minutes, The cis 1,2-dimethylcyclohexane adsorption after 5 and 250 minutes are given in terms of.wt.% of the sample in table 14, The table 't ' snows that UZiVI-6 picks up the iarge cis 1,2-dimethy!cyciohexane much more •readily than UZM-5. . . Table 14 (Table Removed 'Example "i'5 .Samples from examples 1 to 3 were tested for alkyiation activity by 'using an eth'ylb'enzene disproportionation test. The materials were converted to" )he .proton form before/testing. The UZM-6 from.example 3 was calcined in air at y350°C'for 1.5 hours; 450°C for 1.5 Hours: and'-7 hoars; at 580°C and ion ; ; 'exchanged with ammonium chloride, three,times at;80°C. for 2-'hours-The UZM-6 ffromrexample 2 was calcined at 520°C for t hour in N2-, followed "by 19 hours' in air The UZM-5 from example 1 was calcined' at :520°C ,for 10 :hr: The calcihed samples were sized to 40 - 60 mesh and loaded (250-mg) into a quartz tube (11mm i.d.) reactor residing in a furnace. The outlet pressure at the reactor inlet was atmospheric pressure. The samples were pretreateci'at 250°C in a flow of ; N2. The temperature was brought down to. 150°C and then the feed was introduced. The feed consisted of the N2 flow passing through an ethylbenzene saturator held at 0°C, with the N2 flow controlled at 150 cc/miri. While the flow remained constant, the sample was exposed to the feed and reaction products x. Were examined at 150°C, 150°C, 125°C, 175°C, 200°C, 230°C, and 175°C; The j product -effluents are analyzed by an on-iine GC .to measure activity and selectivity. Results from the second 150°C and the 230°C product collections are" given in Table 15. (Table Removed Example 16 .This example' demonstrates the. capability of UZM-6 to catalyze the synthesis of ethyibenzene from benzene and ethylene. The zeolite from example 3 w.as converted to the proton by the same procedure as .in .example 15. The zeolite was then bound with Plural SB alumina in a 70%-zeolite/30% alumina i ' . - formulation and formed into 1/16" diameter extrudates. The.'extrudates• were then i . , calcined, at.550°C. for 2 hr. The test employs a 7/8" diameter stainless'steel-' reactor which is. loaded with 40 cc of the catalyst. The benzene and ethylene are mixed on-line to a 3/1 benzene/ethylene ratio and then'pre-heated: before entering the reactor. The plef in was added at a rate of 0.45; hr"1 LHSV.-The testing was done with an effluent recycle-.to control the f fee-olef ih;at the:reactor inlet The reaction was carried out at 500 psog . Activity and selectivity data were collected..at 200°C and 230°C..The selectivities to alkvlated products are shown in Table:.16; Table 16 ' (Table Removed Example 17 An aluminosilicate reaction mixture was prepared in an identical manner to Mixture B described in example 3. However, the reaction mixture was determined to be slightly different by analysis, with a Si content of 4,79 wt % and 1 a; Si/Al ratio of 9.59, A portion of this aluminosilicate reaction mixture, 1100 g, was placed in a large beaker equipped with a high-speed stirrer. Separately, a .solution was prepared by dissolving 4.14 g Lid and 21,43 g'"TMAC! (97%) in 65 g-de-iohized water. This solution 'was added dropwise to the aruminosjlicate '( reaction mixture with stirring and was,homogenized for an hour. The reaction mixture was,,then transferred to a static'2-L Parr reactor and digested aM5.06G .for!3; days at autogenous pressure; The solid product was isolated by filtration, washed with de^ionized water and dried at 95°C. :• \-., .i,.. Powder x-ray diffraction on\a:5arnpleiOf:the/pr.oduGf;shdwed the pattern to. i. • ' ' - , • ' - • .-,'. be.consistent with that known for UZM-6. The Si/Al::~ratioWas:%:58'. The'-BET— Surface:area was 512 m2/g, whileV-the micrcipore vblume ,was' found to be '0:18' "ccVg SEM. of :the calcined product- showed1 it tojcon,sist;oi^benf'p!ate bry^tai's,;' sprnetimes stacked, up to 0,1 .- 0.4.,µ across and less;that 0.0.5 'µ thick; ;Charactenstic lines in the x-ray diffraction pattern :are;giyeh'ln;;table 17. Table 17 (Table Removed: . . Example; 18 The' zeolites from examples• 1- to-3 and 17 were tested-for xylene isomerization. The materials were converted to an acid form'before testihg.-Material isolated from the procedure of example 1 was tested after calcination at 550°C in air for 5 hr. This sample was designated UZM-5, Ex.1. A portion of the same'material-was acid washed (9g sample, 2 g H2SO4 (98%) in 60 g de-ionized water, 90°C, 2 hr), washed with water, and ammonium ion exchanged (1 N NH4CI,! 90°C, 1.5 hr) before .calcination at 55.0°C for 5 hr, This sample was designated UZM-5, Ex.1-AW, The material from example 2 was calcined at 550°C for 5 hr, ammonium ion exchanged 3 times (1 N NH4CI, 75°C), and calcined at 550°C for 2 hr, This sample was designated UZM-5, Ex. 2. The-UZM-6 from example 3 was calcined in M2 for 1 hr and 19 hr in. air at 520°C and was designated UZM-6, Ex. 3: The UZM-6 from example 17 was obtained in a proton form ;by calcination at 350°G for 1.5.hr, then 450°C for 1.5 hr, and 580°C for 1 hr . in N2, .followed by 6 hr.calcination in air. Then 85 g of the calcined material was : exchanged in 2L of 10% NH4CI solution at 80°C for 2 hr, which was repeated 3 -times.. Finally, the sample was .calcined, for 2 hrat-500°C in 'am, This sample ,was: .••designated. UZM-6,,Ex.17 Fprmicror.eactor testing, the :samples were sized to ;40-60 .mesh and:.actiyated in, a muffle furnace in a: flow of air at 550°C for 2 hr. :Thef:meshed samples, 1 25-mg were' loaded'into an;l 1: ;,mm id. quartz':;reactpn. sitting in;a,fufroacej the, outlet of the reactor was atiatijiosptiericvpressure.The •• samples-were preheated-to 375°C in-a flow of HS. The-folw of ;H2 was;;theh :. directed, through a saturator,; where, it was. saturated with either m-xylene or .. xylene .at 0°C: The .flow.-of-:H2 was -controlled;' at 50 cc/min:.-The furnace . stepped hrough, temperatures;.of .375°C, 400°Ci 425°-C; 450°C, 475oe; and 425°€-.,Product:.effluents at.each -temperature were directed, to an on-ling :GC obtaitn activity1, and selectivity measurements/ The. results :from m-xylene::and - xyleneJsomerization are shown in Tables 18a and 18b, respectively. . Table ISA, m-Xylene Isomerization Data, (Table Removed"able 18A (cont), m-Xylene lsomerization Data. (Table RemovedTabla I8B. o-Xylene lsomerization Data. (Table Removed 1 Amicropous crystailine zeolite having a compositin in the as synthesized form on an anhydrous basis in terms of mole ratios of the elements of: (Equation Removed) where M is at least one exchangeable cation selected from the group consisting of alkaii and alkaline earth metals, "m" is the mole ratio of M to (Ai + E) and varies from 0 to 1.2, R is a nitrogen-containing organic cation selected from the group consisting of protonated amines, protonated diamines, protonated alkanoiamines, quaternary ammonium ions, diquaternaryammonium ions, quaternized alkanolarnines and mixtures thereof, "r" is the mole ratio of R to (A! + E) and has a value of 0.25 to 3.0, E is at least one element selected from the group consisting of Ga, Fe, Cr, In and B, "x" is the moie fraction of E and varies from 0 to 0.5, "n" is the weighted average valence of M and has a value of +1 to +2, "p" is the weighted average valence of R and has a value of +1 to +2, "y" is the mole ratio of Si to (Ai + E) and varies from 5 to 12 and "z" is the mole ratio of O to (AI + E) and has a value determined by the equation: (Equation Removed) me zeolite characterized in that it has at least two x-ray diffraction peaks, •me at a rf-spacings of 3,9±G,1'2A and one at a d-spacing of 8.6±0,20A. 2. The zeolite of claim 1 characterized in that it has a x-ray powder diffraction pattern which contains at least the d-spacings and relative intensities of one of Tables A to C. 3. The zeolite of claims 1 or 2 where M is at least one metal selected from the group consisting of lithium, cesium, sodium, potassium, strontium, barium, calcium, magnesium and R is a quaternary ammonium cation. 4. A process for preparing the microporous crystalline zeolite of any of claims 1-3 which comprises forming a reaction mixture containing reactive sources of R, Al, Si and optionally E and/or M and reacting the reaction mixture at reaction conditions which include a temperature of 100°C to 175°C for a period of 12 hr to 2 weeks, the reaction mixture having a composition expressed in terms of mole ratios of the oxides of: (Equation Removed) ere "a" has a value of 0 to 2, "b" has a value of 1.5 to 30, "c" has a value of 0 to 0.5, "d" has a value of 5 to 30, and "e" has a value of 30 to 6000. 5. The process of claim 4 where the source of E is selected from the group consisting of alkali borates, boric acid, precipitated gallium oxyhydroxide, gallium sulfate, ferric sulfate, ferric chloride, chromium chloride, chromium nitrate, indium chloride and indium nitrate. 6. The process of claim 4 .where the aluminum source is selected from.the group consisting of .aluminum isopropoxide, aluminum sec-butoxide, precipitated alumina, AI(OH)3, aluminura metal and aluminum salts. hydrocarbon conversion process comprising contacting B, hydrocarbon stream with the microporous crystalline zeolite at hydrocarbon conversion conditions to give a converted product, 9. A process for the isomerization of a non-equilibrium feed mixture comprising xylenes and eihylbenzene comprising contacting the feed mixture in the presence of hydrogen in an isomerization zone with a catalyst composite comprising an effective amount of at least one platinum-group metal component and the crystalline aluminosilicate zeolite of any of claims 1-3 at isomerization conditions to obtain an isomerized product comprising a higher proportion of p-xylene than in the feed mixture. 10. The process of Claim 9 wherein the platinum-group metal component is present in an amount from 0.01 to 5 mass-% on an elemental basis, 11. The process of Claim 9 wherein ortho-xylene is recovered from one or both of the isomerized product and fresh feed mixture. 12. The process of Claim 9 further comprising recovery of para-xylene by selective adsorption from the isomerized product and a fresh feed 14 A process for monoaikylating aromatic compounds comprising reacting under alkyiation conditions an oiefin with an aikylatabie aromatic compound to provide an alkylated compound in the presence of a catalyst comprising the crystalline aluminosilicate zeolite of any of claims 1-3. 15. The process of Claim 14 where the oiefin contains from 2 up to 20 carbon atoms. 16. The process of claim 14 where the process is carried out under at least partial liquid phase conditions. 17. A process for preparing cumene by the alkyiation of benzene with propylene comprising reacting propyiene with benzene at a temperature between 90°C and 200°C at a pressure sufficient to maintain at least a partial liquid phase in the presence of a catalyst comprising the crystalline aluminosilicate zeolite of any of claims 1-3, 18. A transalkylation process comprising reacting under transalkyfation reaction conditions a polyalkylated aromatic compound with a nonalkylated aromatic compound, wherein at least one alkyl group is transferred from Hie polyalkylated aromatic compound to the nonalkylated aromatic compound in the presence of the rnicroporous crystalline zeolite of any of claims 1-3.

Documents:

713-delnp-2003-abstract.pdf

713-delnp-2003-assigment.pdf

713-delnp-2003-claims.pdf

713-delnp-2003-correspondence-others.pdf

713-delnp-2003-correspondence-po.pdf

713-delnp-2003-description (complete).pdf

713-delnp-2003-form-1.pdf

713-delnp-2003-form-18.pdf

713-delnp-2003-form-2.pdf

713-delnp-2003-form-26.pdf

713-delnp-2003-form-3.pdf

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713-delnp-2003-gpa.pdf

713-delnp-2003-pct-101.pdf

713-delnp-2003-pct-102.pdf

713-delnp-2003-pct-105.pdf

713-delnp-2003-pct-199.pdf

713-delnp-2003-pct-210.pdf

713-delnp-2003-pct-301.pdf

713-delnp-2003-pct-304.pdf

713-delnp-2003-pct-401.pdf

713-delnp-2003-pct-402.pdf

713-delnp-2003-petition 137.pdf