And Vanadium Containing Patents (Class 502/209)
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Patent number: 5422326Abstract: When a catalyst for producing methacrylic acid is prepared by shaping a catalyst component represented by the general formula P.sub.a Mo.sub.b V.sub.c X.sub.d Y.sub.e Z.sub.f O.sub.g wherein P, Mo, V, X, Y, Z, a, b, c, d, e, f and g are as defined in the specification, a catalyst capable of giving methacrylic acid in high yield is provided by adding one or more organic high-molecular weight compounds with an average particle size of 0.01-10 .mu.m, and carrying out heat treatment before use as a catalyst.Type: GrantFiled: February 8, 1993Date of Patent: June 6, 1995Assignee: Mitsubishi Rayon Co., Ltd.Inventors: Toru Kuroda, Motomu Ohkita
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Patent number: 5420091Abstract: A method of preparing a catalyst used for producing methacrylic acids through gas phase catalytic oxidation of methacrolein with molecular oxygen. The catalyst is represented by the formula:P.sub.a Mo.sub.b V.sub.c Ge.sub.d X.sub.e Y.sub.f Z.sub.g O.sub.hwherein P, Mo, V, Ge and O represent phosphorous, molybdenum, vanadium, germanium and oxygen, respectively; X represents at least one element selected from the group consisting of arsenic, antimony, bismuth, zirconium, tellurium, silver and boron; Y represents at lest one element selected from the group consisting of iron, copper, zinc, chromium, magnesium, tantalum, manganese, barium, gallium, cerium and lanthanum; Z represents at least one element selected from the group consisting of potassium, rubidium, cesium and thallium, and a, b, c, d, e, f, g and h represent the atomic ratios of the respective elements, and when b=12, then a=0.5-3, c=0.01-3, d=0.01-3, e=0-3, f=0-3, g=0.Type: GrantFiled: July 13, 1993Date of Patent: May 30, 1995Assignee: Mitsubishi Rayon Co., Ltd.Inventors: Toru Kuroda, Motomu Oh-Kita
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Patent number: 5401707Abstract: A vanadium/phosphorus oxide oxidation catalyst suitable for catalytic oxidation of C.sub.4 feed stock in the preparation of maleic anhydride is formed by calcining an intercalation complex of the formula VOHPO.sub.4 .multidot.0.5H.sub.2 O.multidot.({C.sub.n H.sub.2n+1 }--X).sub.z in which n has a value of from 0 to 20, z has a value of from about 1.5 to about 1.9; and X is an oxygen- or nitrogen-containing functional group operable to form hydrogen bonds with the structural P--OH and water groups of the complex.Type: GrantFiled: December 3, 1993Date of Patent: March 28, 1995Assignee: The Trustees of Princeton UniversityInventors: Jay B. Benziger, Vadim Guliants, Sankaran Sundaresan
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Patent number: 5391530Abstract: The present invention relates to a process for the production of a catalyst for the removal of nitrogen oxides from waste gases, in which the end of the catalyst on the gas-inlet side is coated with a compound selected from the group consisting of biphosphates, condensed phosphates, silicates, borates and mixtures thereof, and is subjected to thermal aftertreatment, where the end of the green element on the gas-inlet side is immersed into an aqueous preparation comprising biphosphates and/or condensed phosphates and/or silicates and/or borates, and the green element is subsequently calcined at temperatures of from 300.degree. to 700.degree. C.Type: GrantFiled: July 20, 1993Date of Patent: February 21, 1995Assignee: Huels Aktiengesellschaft - PB15Inventors: Bernd Nowitzki, Jurgen Jung, Helmut Kretschmer
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Patent number: 5366945Abstract: There is provided a catalyst comprising a heteropoly acid, such as phosphotungstic acid, supported on a mesoporous crystalline material, such as M41S. A particular form of this M41S support is designated as MCM-41. There is also provided a method for preparing this catalyst by impregnating the heteropoly acid on the support. There is also provided a process for using this catalyst to catalyze acid catalyzed reactions, such as the isomerization of paraffins and the alkylation of aromatics.Type: GrantFiled: December 22, 1992Date of Patent: November 22, 1994Assignee: Mobil Oil Corp.Inventors: Charles T. Kresge, David O. Marler, Gayatri S. Rav, Brenda H. Rose
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Patent number: 5364824Abstract: A phosphorus vanadium oxide catalyst for the oxidation of a C.sub.4 hydrocarbon. The catalyst comprises a shaped body having a volume, or a fixed bed comprising shaped bodies having an average volume, of at least about 0.02 cc, and contains a promoter selected from among Bi, Sb, Ge, Ti, Zr, La, Ce, Ni, Zn, U, Sn, Si or mixtures thereof. The promoter is present in a proportion that enables the catalyst to have a developed surface area of at least about 28 m.sup.2 /g, and to exhibit a weight/area productivity of at least about 3.5 mg maleic anhydride/m.sup.2 -hr and/or a weight/weight productivity of at least about 100 g maleic anhydride/kg.cat.-hr. when contacted with a gas containing 2.4% by volume n-butane in air, at a gas flow volume to catalyst weight ratio of 2180 cc/g-min., under a pressure of 1.055.times.10.sup.2 -kPa-G, and at a temperature sufficient to maintain a hydrocarbon conversion of 85 mole percent. Methods for the preparation of the catalyst include activation by ANST.Type: GrantFiled: December 8, 1992Date of Patent: November 15, 1994Assignee: Huntsman Specialty Chemicals CorporationInventors: William J. Andrews, Jerry R. Ebner, Timothy R. Felthouse
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Patent number: 5364825Abstract: Multimetal oxide compositions of the formula I[X.sup.1.sub.a X.sup.2.sub.b O.sub.x ].sub.p [X.sup.3.sub.c X.sup.4.sub.d X.sup.5.sub.e X.sup.6.sub.f X.sup.7.sub.g X.sup.2.sub.h O.sub.y ].sub.q(I)whereX.sup.1 is bismuth, tellurium, antimony, tin and/or copper,X.sup.2 is molybdenum and/or tungsten,X.sup.3 is an alkali metal, thallium and/or samarium,X.sup.4 is an alkaline earth metal, nickel, cobalt, copper, manganese, zinc, tin, cadmium and/or mercury,X.sup.5 is iron, chromium, cerium and/or vanadium,X.sup.6 is phosphorus, arsenic, boron and/or antimony,X.sup.7 is a rare-earth metal, titanium, zirconium, niobium, tantalum, rhenium, ruthenium, rhodium, silver, gold, aluminum, gallium, indium, silicon, germanium, lead, thorium and/or uranium,a is from 0.01 to 8,b is from 0.Type: GrantFiled: May 21, 1993Date of Patent: November 15, 1994Assignee: BASF AktiengesellschaftInventors: Hans-Peter Neumann, Hans Martan, Hermann Petersen, Walter Doerflinger
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Patent number: 5354722Abstract: The present invention provides a composition of matter having the formulaA.sub.x B.sub.1-x V.sub.y C.sub.1-y P.sub.3 O.sub.10-15wherein A is Nb or Ta, B is Sb, C is Ti or Sn, and 0.ltoreq.x,y.ltoreq.1, a composition of matter having the formulaM.sub.z A.sub.x B.sub.1-x V.sub.y C.sub.1-y P.sub.3 O.sub.10-15wherein M is selected from the group consisting of Cu, Ag, Na, K, and Cs, A is Nb or Ta, B is Sb, C is Ti or Sn, and 0.ltoreq.x,y,z.ltoreq.1, a composition of matter having the formulaM.sub.z A.sub.x B.sub.1-x V.sub.y C.sub.1-y P.sub.3-n Si.sub.n O.sub.10-15wherein M is selected from the group consisting of Cu, Ag, Bi, Na, K, Rb, and Cs, A is Nb or Ta, B is Sb or As, C is Ti, Zr, Sn, or Ge, and 0.ltoreq.x,z.ltoreq.1, 0<y.ltoreq.1, and 0.ltoreq.n.ltoreq.2, and conversion processes catalyzed by at least one of the composition.Type: GrantFiled: April 22, 1993Date of Patent: October 11, 1994Assignee: Mobil Oil CorporationInventors: Pradyot A. Agaskar, Robert K. Grasselli
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Patent number: 5348927Abstract: A method of removing chloride from phosphorus/vanadium/oxygen mixed oxide oxidation catalysts comprising treating a chloride containing catalyst comprising phosphorus, vanadium and oxygen with a stream of gas comprising oxygen, steam and an inert gas at flow rate and temperature and for a period of time to substantially reduce the amount of chloride in the catalyst.Type: GrantFiled: March 1, 1993Date of Patent: September 20, 1994Assignee: Scientific Design Company, Inc.Inventor: Arie Bortinger
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Patent number: 5330954Abstract: A catalytic system based on oxygen, vanadium, phosphorus, and molybdenum corresponding to the formula H.sub.m X.sub.n Me.sub.p PMo.sub.12-x V.sub.x O.sub.40, wherein X represents the VO.sup.2+ cation with 0<n.ltoreq.2, H represents protons with 0.ltoreq.m<4, 0.ltoreq.x.ltoreq.3, Me is a metal ion, especially an ion of a transition metal, with 0.ltoreq.p.ltoreq.t, t depending on the charge of the corresponding ion, is useful for the oxydehydrogenation of saturated carboxylic acids to .alpha.,.beta.-unsaturated acids and for oxidizing aldehydes to acids.Type: GrantFiled: September 3, 1992Date of Patent: July 19, 1994Assignee: Elf Atochem, S.A.Inventors: Emmanuel Cadot, Franck Daubrege, Gilbert Herve, Andre Teze
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Patent number: 5329043Abstract: A method of preparing methacrolein and/or methacrylic acid by catalytic gas phase oxidation of isobutane in the presence of a catalyst, wherein said catalyst is a catalyst containing divanadyl pyrophosphate and represented by general formula (1)P.sub.a V.sub.b X.sub.c Y.sub.d Z.sub.e O.sub.x (1)wherein P, V, and O represent phosphorus, vanadium and oxygen, respectively; X represents at least one element selected from the group consisting of cobalt and nickel; Y represents at least one element selected from the group consisting of niobium, tantalum, manganese, iron, copper, zinc, lanthanum, neodymium, samarium, cerium, zirconium, chromium, magnesium, tungsten, tin, hafnium, uranium, indium, cadmium, molybdenum, antimony, bismuth, rhodium, silver and sulfur; Z represents at least one element selected from the group consisting of potassium, rubidium, cesium and thallium; a, b, c, d, e, and x represent atomic ratios, respectively, provided that when a is 1, b is 0.2 to 2, c is 0.Type: GrantFiled: May 26, 1993Date of Patent: July 12, 1994Assignee: Nippon Shokubai Co., Ltd.Inventors: Ikuya Matsuura, Yukio Aoki
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Patent number: 5302566Abstract: A process is described for preparing attrition resistant catalyst, particularly vanadium/phosphorus oxide catalyst, having an oxide rich surface layer. The oxide rich surface layer is obtained from a stable oxide-forming mixture which contains both colloidal oxide sol and a soluble oxide precursor.Type: GrantFiled: January 25, 1993Date of Patent: April 12, 1994Assignee: E. I. Du Pont de Nemours and CompanyInventor: Jo Ann T. Schwartz
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Patent number: 5300472Abstract: A catalyst for the selective reduction of nitrous oxide with ammonia contains, in addition to titanium oxide as component (A), at least one oxide of W, Si, B, Al, P, Zr, Ba, Y, La, Ce and at least one oxide of Y, Nb, Mo, Fe, Cu as component (B), whereby the atomic ratio between the elements of components (A) and (B) amounts to 1:0.001 up to 1. The catalyst can be obtained by kneading reactive titanium oxide with a high specific surface of predominantly anatase with the substances of component (B) or their preliminary stages, adding processing agents, winding up with a homogeneous kneaded mass, extruding the latter, drying the extrudate and calcining in air at 300.degree.-800.degree. C.Type: GrantFiled: December 31, 1992Date of Patent: April 5, 1994Assignee: Degussa AktiengesellschaftInventors: Reinhold Brand, Bernd Engler, Wolfgang Honnen, Edgar Koberstein, Johannes Ohmer
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Patent number: 5296436Abstract: An improvement in the oxidation catalyst used for the partial oxidation of n-butane and containing vanadium and phosphorus, zinc, lithium and molybdenum mixed oxides which comprises adding the molybdenum as a compound which is dissolved in a solvent during the manufacture of the catalyst.Type: GrantFiled: January 8, 1993Date of Patent: March 22, 1994Assignee: Scientific Design Company, Inc.Inventor: Arie Bortinger
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Patent number: 5288880Abstract: The present invention provides a process for the manufacture of maleic anhydride by the vapor phase catalytic oxidation of n-butane with molecular oxygen by the use of a specially prepared phosphorus vanadium-oxygen composite catalyst containing specific kind of a divalent metal. The catalyst used in the present invention is prepared from a mixture of vanadyl hydrogen orthophosphate and at least one compound selected from the group consisting of a divalent metal hydrogen orthophosphate (Divalent metal is selected from Mg, Ca, Ba, Mn, Fe, Co, Ni, Cu, and Zn.), a divalent metal ammonium orthophosphate (Divalent metal is the same as above.), and a divalent metal orthophosphate (Divalent metal is the same as above.), with the atomic ratio of the divalent metal/vanadium of 0.003-0.5, by calcining the mixture at 300.degree.-400.degree. C., and then pretreating said catalyst in an inert gas or a mixed gas containing n butane and molecular oxygen at 350.degree.-700.degree. C.Type: GrantFiled: March 15, 1993Date of Patent: February 22, 1994Assignee: Maruzen Petrochemical Co., Ltd.Inventor: Ikuya Matsuura
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Patent number: 5280003Abstract: An improvement in the oxidation catalyst used for the partial oxidation of n-butane and containing vanadium and phosphorus, zinc, lithium and molybdenum mixed oxides which comprises carrying out the crystallization step under static conditions which allows for more uniform conditions for crystal growth. The static conditions are maintained by refluxing the solvent during the period of crystallization.Type: GrantFiled: August 24, 1992Date of Patent: January 18, 1994Assignee: Scientific Design Company, Inc.Inventor: Arie Bortinger
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Patent number: 5275996Abstract: An activated porous phosphorus/vanadium oxide catalyst adapted for the catalytic oxidation of a hydrocarbon to produce a carboxylic acid anhydride. The catalyst comprises shaped bodies having a B.E.T. surface area of at least about 15 m.sup.2 /g, an average vanadium oxidation state of between about 4.0 and about 4.5, a total pore volume of at least about 0.15 cc/g, a normalized apparent shaped body density of between about 1.25 and about 2.0 g/cc, and a crush strength of at least about 4 pounds. At least about 5% of the pore volume of the catalyst is constituted of pores having a diameter of at least about 0.8 microns, and at least about 4% of the pore volume is constituted of pores having a diameter of at least about 10 microns.Type: GrantFiled: May 22, 1992Date of Patent: January 4, 1994Assignee: Monsanto CompanyInventors: William J. Andrews, Jerry R. Ebner, Timothy R. Felthouse
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Patent number: 5260241Abstract: A phosphate-Al.sub.2 O.sub.3 material is disclosed wherein the phosphate is homogeneously dispersed throughout, the specific surface area as measured by N.sub.2 BET method is at least about 50 m.sup.2 /g, and the average pore radius is no greater than about 200.ANG.. A method is disclosed for producing the material which comprises forming a precursor material by wet-mixing a phosphate yielding species and an aluminum oxide yielding species which can be aluminum oxide, aluminum hydroxylated oxides, aluminum hydroxide, aluminum alkoxides, and combinations thereof, in amounts sufficient to result in an AlPO.sub.4 content of about 3 to 12 percent by weight in the phosphate-Al.sub.2 O.sub.3, drying and heat-treating the precursor material at a temperature and for a time sufficient to form the phosphate- Al.sub.2 O.sub.3. The material is used as a support for catalyst metals.Type: GrantFiled: August 12, 1992Date of Patent: November 9, 1993Assignee: Corning IncorporatedInventors: William P. Addiego, Irwin M. Lachman, Mallanagouda D. Patil, Jimmie L. Williams
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Patent number: 5235071Abstract: The invention relates to a catalyst for producing phthalic anhydride by gas phase catalytic oxidation of o-xylene and/or naphthalene with molecular oxygen or gas containing molecular oxygen and, to a process for producing phthalic anhydride by using said catalyst. The catalyst is made by supporting, on a heat-resistant inorganic carrier, a catalytic active substance which comprises: vanadium oxide; anatase type titanium dioxide having specific surface area of 10 to 60 m.sup.2 /g; niobium; at least one element selected from potassium, cesium, rubidium and thallium; phosphorus; and antimony. The catalytic active substance is prepared by using a five-valent antimony compound as an antimony source. The process for producing phthalic anhydride comprises use of said catalyst.Type: GrantFiled: June 30, 1992Date of Patent: August 10, 1993Assignee: Nippon Shokubai Co., Ltd.Inventors: Kenji Ueda, Masaaki Okuno, Tatsuya Kawabata, Shinya Tanaka
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Patent number: 5223469Abstract: The present invention relates to a fluidized-bed catalyst for propylene ammoxidation to produce acrylonitrile, which consists of silica support and a composite of the formulaA.sub.a B.sub.b C.sub.c Ni.sub.d Co.sub.e Na.sub.f Fe.sub.g Bi.sub.h M.sub.i Mo.sub.j O.sub.xwherein A is potassium, rubidium, cesium samarium, thallium, or mixture thereof; B is manganese, magnesium, strontium, calcium, barium, lanthanum, rare earth, or mixture thereof; C is phosphorus, arsenic, boron, antimony, chromium, or mixture thereof; M is tungsten, vanadium, or mixture thereof. The catalyst of the present invention is highly active and selective for preparing acrylonitrile, more specifically, is suitable for catalyzing the reaction between air and propylene at a rather low ratio hence to greatly enlarge the processing capacity of the reactor. By using the catalyst of the present invention, the processing capacity of the reactor increases by 10-15 percent compared with that using conventional catalysts.Type: GrantFiled: October 31, 1991Date of Patent: June 29, 1993Assignee: China Petro-Chemical CorporationInventors: Xin Chen, Lianghua Wu
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Patent number: 5221767Abstract: Compositions of the formula IMo.sub.12 P.sub.a V.sub.b X.sub.c.sup.1 X.sub.d.sup.2 X.sub.e.sup.3 Sb.sub.f Re.sub.g S.sub.h O.sub.n (I),whereX.sup.1 is potassium, rubidium and/or cesium,X.sup.2 is copper and/or silver,X.sup.3 is cerium, boron, zirconium, manganese and/or bismuth,a is from 0.5 to 3.0,b is from 0.01 to 3.0,c is from 0.2 to 3.0,d is from 0.01 to 2.0,e is from 0 to 2.0,f is from 0.01 to 2.0,g is from 0 to 1.0,h is from 0.001 to 0.5 andn is a number determined by the valency and content of the elements different from oxygen in I, are used as catalysts for preparing methacrylic acid by gas-phase oxidation of methacrolein.Type: GrantFiled: August 12, 1992Date of Patent: June 22, 1993Assignee: BASF AktiengesellschaftInventors: Karl-Heinz Boehning, Gerd Duembgen, Ulrich Hammon, Richard Krabetz, Franz Merger, Matthias Schwarzmann, Fritz Thiessen, Herbert Vogel
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Patent number: 5215952Abstract: Method for making catalysts for gas phase oxidation reactions by admixing a catalytically active material comprising oxides of molybdenum, phosphorus, and vanadium with combustible natural or synthetic fibers, or with carbon fibers, forming shaped bodies from the mixture, and then calcining said shaped bodies at 100.degree. C. to 380.degree. C. in oxygen, whereby said fibers are burned out to leave channels in said shaped bodies; catalysts made by such methods; and methods for gas phase oxidation reactions using such catalysts.Type: GrantFiled: April 24, 1992Date of Patent: June 1, 1993Assignee: Rohm GmbHInventors: Ernst Bielmeier, Thomas Haeberle
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Patent number: 5206201Abstract: A catalyst for the production of a substituted benzaldehyde by catalytic vapor-phase oxidation of a substituted toluene, which catalyst has as a catalytically active substance being composed of an oxide represented by the general formula III:V.sub.a Mo.sub.b X.sub.c Y.sub.d O.sub.e (III)wherein V, Mo, and O are respectively for vanadium, molybdenum, and oxygen, X is at least one element selected from the group consisting of sodium, potassium, rubidium, cesium, and thallium, Y is at least one element selected from the group consisting of niobium, tantalum, phosphorus, antimony, bismuth, tellurium, tin, lead, boron, copper, and silver, and a, b, c, d, and e indicate the atomic ratios of relevant elements such that where a+b=1, then b=0.05 to 0.4, c=0.1 to 1, d=0 to 1, and e=the value determined by the state of oxidation of other elements.Type: GrantFiled: May 22, 1991Date of Patent: April 27, 1993Assignee: Nippon Shokubai Co., Ltd.Inventors: Nobuji Kishimoto, Isao Nakamura, Taizou Matsueda, Yoshitaka Arita
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Patent number: 5198403Abstract: A catalyst for the selective reduction of nitrous oxide with ammonia contains, in addition to titanium oxide as component (A), at least one oxide of W, Si, B, Al, P, Zr, Ba, Y, La, Ce and at least one oxide of V, Nb, Mo, Fe, Cu as component (B), whereby the atomic ratio between the elements of components (A) and (B) amounts to 1:0.001 up to 1. The catalyst can be obtained by kneading reactive titanium oxide with a high specific surface of predominantly anatase with the substances of component (B) or their preliminary stages, adding processing agents, winding up with a homogeneous kneaded mass, extruding the latter, drying the extrudate and calcining in air at 300.degree.-800.degree. C.Type: GrantFiled: November 5, 1991Date of Patent: March 30, 1993Assignee: Degussa AGInventors: Reinhold Brand, Bernd Engler, Wolfgang Honnen, Edgar Koberstein, Johannes Ohmer
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Patent number: 5183793Abstract: Catalysts having the general formula:V.sub.1 Bi.sub.a Sb.sub.b Fe.sub.c X.sub.d Y.sub.c Z.sub.f O.sub.gwherein,X=Mo, Cu, W, Nb, Te, P, Sn, Ge, AsY=Co, Ni, Ce, La, Mn, CrZ=Alkali, alkaline earth, B, Tl and,a=0.1-10,b=0.01-20,c=0.01-5,d=0-5,e=o-3,f=0-1, and g is determined by the valance requirements of the elements present,are produced by first forming and calcining an iron-antimony oxide composition which is subsequently combined with compounds of vanadium, bismuth and other elements. The catalysts are useful in the formation of phthalonitriles from the reaction of xylenes with oxygen and ammonia at elevated temperatures.Type: GrantFiled: November 13, 1991Date of Patent: February 2, 1993Assignee: The Standard Oil CompanyInventors: Christos Paparizos, Wilfrid G. Shaw
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Patent number: 5173468Abstract: Compositions of the formula IMO.sub.12 P.sub.a V.sub.b X.sup.1.sub.c X.sup.2.sub.d X.sup.3.sub.e Sb.sub.f Re.sub.g S.sub.h O.sub.n (I)whereX.sup.1 is potassium, rubidium and/or cesium,X.sup.2 is copper and/or silver,X.sup.3 is cerium, boron, zirconium, manganese and/or bismuth,a is from 0.5 to 3.0,b is from 0.01 to 3.0,c is from 0.2 to 3.0,d is from 0.01 to 2.0,e is from 0 to 2.0,f is from 0.01 to 2.0,g is from 0 to 1.0,h is from 0.001 to 0.5 andn is a number determined by the valency and content ofthe elements different from oxygen in I, are used as catalysts for preparing methacrylic acid by gas-phase oxidation of methacrolein.Type: GrantFiled: July 12, 1991Date of Patent: December 22, 1992Assignee: BASF AktiengesellschaftInventors: Karl-Heinz Boehning, Gerd Duembgen, Ulrich Hammon, Richard Krabetz, Franz Merger, Matthias Schwarzmann, Fritz Thiessen, Herbert Vogel
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Patent number: 5171876Abstract: Disclosed is a process for making an .alpha., .beta.-unsaturated mononitrile by the catalytic reaction of a paraffin containing 3-5 carbon atoms with molecular oxygen and ammonia by catalytic contact of the foregoing reactants in a reaction zone with a metal oxide catalyst containing the elements indicated by the empirical formula,Cr.sub.a Mo.sub.b Te.sub.c M.sub.d O.sub.x (formula 1)whereM=one or more of Mg, Ni, Sb, Ti, La, P, Ce, Fe, Nb, W, V, and Cu, each of a, b & c is 0.1 to 10d is zero to 10a+b+c>1.5d, andx is determined by the valence requirements of the other elements present, andwherein the reactants fed to the reaction zone contain a mole ratio of said paraffin:NH.sub.3 in the range from 2.5 to 16 and a mole ratio of said paraffin:O.sub.2 in the range from 1 to 10.Type: GrantFiled: September 16, 1991Date of Patent: December 15, 1992Assignee: The Standard Oil CompanyInventors: Dev D. Suresh, Michael J. Seeley, Jeanette R. Nappier, Maria S. Friedrich
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Patent number: 5169820Abstract: The invention presents catalysts for producing phthalic anhydride by vapor phase catalytic oxidation of orthoxylene and/or naphthalene with molecular oxygen or gas containing molecular oxygen. The catalyst is prepared by supporting a catalytic active substance comprising 1 to 20 parts by weight (hereinafter abbreviated "parts") of vanadium oxide as V.sub.2 O.sub.3, 99 to 80 parts of anatase type titanium dioxide with specific surface area of 10 to 60 m.sup.2 /g as TiO.sub.2 and per 100 parts of the sum of these two ingredients, 0.05 to 1.2 parts of at least one element selected from potassium, cesium, rubidium and thallium as oxide, and 0.05 to 2 parts of silver as Ag.sub.2 O on a heat resistant inorganic carrier. The catalyst may also contain, per 100 parts in total of vanadium oxide and titanium dioxide, 0 to 1 part of niobium as Nb.sub.2 O.sub.5, 0 to 1.2 parts of phosphorus as P.sub.2 O.sub.3, and 0 to 5 parts of antimony as Sb.sub.2 O.sub.Type: GrantFiled: March 6, 1991Date of Patent: December 8, 1992Assignee: Nippon Shokubai Kagaku Kogyo Co., Ltd.Inventors: Kenji Ueda, Tatsuya Kawabata, Masaaki Okuno, Chisako Nishio, Shinya Tanaka
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Patent number: 5168090Abstract: Shaped oxidation catalyst structures containing catalytic material comprised of mixed oxides of vanadium and phosphorus which are useful for the production of maleic anhydride via the partial oxidation of nonaromatic hydrocarbons, particularly n-butane, in the vapor phase with molecular oxygen or a molecular oxygen-containing gas are provided. Such structures are characterized by exhibiting (a) a geometric volume of from about 30 percent to about 67 percent of that exhibited by the void space-free solid geometric form, (b) an external geometric surface area/geometric volume ratio of at least about 20 cm.sup.-1, (c) a bulk density of from about 0.4 g/cm.sup.3 to about 1.4 g/cm.sup.3, and (d) a mechanical resistance sufficient to maintain substantially the structural integrity of the shaped structure under handling and use conditions.Type: GrantFiled: December 20, 1991Date of Patent: December 1, 1992Assignee: Monsanto CompanyInventors: Jerry R. Ebner, Robert A. Keppel
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Patent number: 5158923Abstract: An improvement in the oxidation catalyst used for the partial oxidation of n-butane and containing vanadium and phosphorus, zinc and lithium mixed oxides which comprises adding a molybdenum compound modifier in an amount of from about 0.005 to 0.025/1 Mo/V to the catalyst during the digestion of the reduced vanadium compound by concentrated phosphoric acid. The addition of Mo produces a catalyst which is very stable more active system and longer lived than the unmodified catalyst.Type: GrantFiled: July 22, 1991Date of Patent: October 27, 1992Assignee: Scientific Design Company, Inc.Inventor: Bruno J. Barone
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Patent number: 5155235Abstract: A catalyst for producing maleic anhydride by oxidation of n-butane comprising V,P and additionally Mg or Zr is prepared by(a) heating a pentavalent vanadium compound in an organic medium to reduce at least a part of the pentavalent vanadium to tetravalent vanadium,(b) reacting the resulting vanadium compound with phosphoric acid in the presence of at least one of a magnesium compound and a zirconium compound to form a catalyst precursor,(c) separating the resulting catalyst precursor from the organic medium, and(d) drying and calcining the catalyst precursor.Type: GrantFiled: July 5, 1991Date of Patent: October 13, 1992Assignee: Mitsui Toatsu Chemicals, Inc.Inventors: Jimbo Takashi, Tadamitsu Kiyoura, Yasuo Kogure, Kazuo Kanaya
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Patent number: 5153162Abstract: A catalyst for the production of methacrylic acid composed of an inert carrier and a catalytically active substance. The catalytically active substance layer being composed of oxides represented by the following formula (I)Mo.sub.a P.sub.b a.sub.c B.sub.d C.sub.e D.sub.f O.sub.x (I)where Mo represents molybdenum, P represents phosphorus, A represents at least one element selected from arsenic, antimony, germanium, bismuth, zirconium, cerium and selenium, B is at least one element selected from copper, iron, chromium, nickel, maganese, cobalt, tin, silver, zinc, palladium, rhodium and tellurium, C represents at least one element selected from vanadium, tungsten and niobium, D represents at least one element selected from alkali metals, alkaline earth metals and thallium, and O represents oxygen, a, b, c, d, e, f and x respectively represent the atomic ratios of Mo, P, A, B, C, D and O, and when a=12, b=0.5-4, c=0-5, d=0-3, e=0-4, and f=0.Type: GrantFiled: August 29, 1990Date of Patent: October 6, 1992Assignee: Nippon Shokubai Kagaku Kogyo Co., Ltd.Inventors: Ikuo Kurimoto, Hideto Hashiba, Hideo Onodera, Yukio Aoki
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Patent number: 5139988Abstract: A composition which contains as essential components: crystalline iron antimonate and at least one element selected from the group consisting of vanadium, molybdenum, and tungsten; is useful as a catalyst in the oxidation reaction of organic compounds. Also, a process for producing the composition is disclosed.Type: GrantFiled: September 17, 1991Date of Patent: August 18, 1992Assignee: Nitto Chemical Industry Co., Ltd.Inventors: Yutaka Sasaki, Hiroshi Utsumi, Kenichi Miyaki
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Patent number: 5137860Abstract: Vanadium/phosphorus mixed oxide catalysts comprising vanadyl pyrophosphate, optionally containing a promoter component, are transformed from vanadium/phosphorus mixed oxide catalyst precursors comprising vanadyl hydrogen phosphate, optionally containing a promoter component, by subjecting the catalyst precursors to elevated temperatures in three stages--(a) an initial heat-up stage in an atmosphere selected from the group consisting of air, steam, an inert gas, and mixtures thereof, (b) a rapid heat-up stage at a programmed heat-up rate in a molecular oxygen/steam-containing atmosphere, and (c) a maintenance/finishing stage, first in a molecular oxygen/-steam-containing atmosphere, and thereafter in a nonoxidizing, steam-containing atmosphere. Such catalysts are useful for the production of maleic anhydride via the partial oxidation of nonaromatic hydrocarbons, particularly n-butane, in the vapor phase with molecular oxygen or a molecular oxygen-containing gas.Type: GrantFiled: June 27, 1991Date of Patent: August 11, 1992Assignee: Monsanto CompanyInventors: Jerry R. Ebner, William J. Andrews
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Patent number: 5134106Abstract: Novel maleic anhydride catalysts comprising phosphorus-vanadium oxides and phosphorus-vanadium-co-metal oxides which under reaction conditions for the manufacture of maleic anhydride from butane feedstock do not expand to the point of crushing and producing fines.Type: GrantFiled: February 19, 1991Date of Patent: July 28, 1992Assignee: Amoco CorporationInventors: Muin S. Haddad, William S. Eryman
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Patent number: 5128299Abstract: A process for producing a crystalline oxide of vanadium-phosphorus system, which comprises hydrothermally treating an aqueous medium containing (1) a tetravalent vanadium compound, (2) a pentavalent phosphorus compound, (3) a coordinate compound having at least two ligand atoms selected from the group consisting of oxygen atoms and nitrogen atoms and (4) a compound of at least one metal element selected from the group consisting of iron, nickel, cobalt and chromium, to form a crystalline oxide of vanadium-phosphorus system having an X-ray diffraction pattern shown in Table A:TABLE A ______________________________________ X-ray diffraction peaks (Anticathode: Cu--K.alpha.) 2.theta. (.+-.0.2.degree.) ______________________________________ 15.6.degree. 19.7.degree. 24.3.degree. 27.2.degree. 28.8.degree. 30.5.degree. 33.8.degree.Type: GrantFiled: December 6, 1990Date of Patent: July 7, 1992Assignee: Mitsubishi Kasei CorporationInventors: Masakatsu Hatano, Masayoshi Murayama, Kenji Shima, Masumi Ito
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Patent number: 5126307Abstract: A process for preparing a multi-component catalyst for producing methacrylic acid, containing phosphorus, molybdenum and vanadium, comprising mixing oxides of molybdenum and vanadium, water and materials for the other catalyst-constituting elements except potassium, rubidium, cesium and thallium to prepare a mixed solution, heating and reacting the mixed solution at 85.degree. C. or more for 1 to 10 hours, then cooling the mixed solution to 80.degree. C. or less, adding thereto a material for at least one element component selected from the group consisting of potassium, rubidium, cesium and thallium, adding further thereto at least one compound selected from the group consisting of ammonium nitrate, ammonium carbonate, ammonium hydrogencarbonate, ammonium sulfate and ammonium hydrogensulfate with the temperature of the mixed solution kept at 80.degree. C. or less, then removing water therefrom and heat-treating the residual product.Type: GrantFiled: April 22, 1991Date of Patent: June 30, 1992Assignee: Mitsubishi Rayon Co., Ltd.Inventors: Shinji Yamamoto, Motomu Oh-Kita
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Patent number: 5124302Abstract: A monolithic ceramic structure, useful as a support for catalytic material or as a fluid filter, has a high surface area phase which consists essentially of a porous metal oxide material, at least 50% by weight of which is alumina, titania, and/or zirconia, and phosphate dispersed substantially throughout the porous metal oxide material. The presence of the phosphate stabilizes the porous metal oxide material against thermal degradation during sintering or exposure to elevated temperatures encountered in catalytic service and thereby aids in the retention of higher overall surface area in the monolithic structure.Type: GrantFiled: April 9, 1991Date of Patent: June 23, 1992Assignee: Corning IncorporatedInventors: Irwin M. Lachman, Jimmie L. Williams, Kenneth E. Zaun
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Patent number: 5116796Abstract: The present invention discloses two polyoxoanion supported metal complexes found to be useful in olefin hydrogenation. The complexes are novel compositions of matter which are soluble in organic solvents. In particular, the compositions of matter comprise A.sub.x [L.sub.n Ir.sup.(I) .multidot.X.sub.2 M.sub.15 M'.sub.3 O.sub.62 ].sup.x- and A.sub.y [L.sub.n Ir.sup.(I) .multidot.X.sub.2 M.sub.9 M'.sub.3 O.sub.40 ].sup.y- where L is a ligand preferably chosen from 1,5-cyclooctadiene (COD), ethylene, cyclooctene, norbornadiene and other olefinic ligands; n=1 or 2 depending upon the number of double bonds present in the ligand L; X is a "hetero" atom chosen from B, Si, Ge, P, As, Se, Te, I, Co, Mn and Cu; M is either W or Mo; M' is preferably Nb or V but Ti, Zr, Ta, Hf are also useful; and A is a countercation preferably selected from tetrabutyl ammonium and alkali metal ions.Type: GrantFiled: October 26, 1988Date of Patent: May 26, 1992Assignee: The University of OregonInventors: David J. Edlund, Richard G. Finke, Robert J. Saxton
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Patent number: 5108974Abstract: Vanadium pentoxide can be reduced to the +4 oxidation state from the +5 state, in the manufacture of vanadium-phosphorus-oxide catalyst precursor, (VO).sub.2 H.sub.4 P.sub.2 O.sub.9, by using phosphoric acid as the reducing agent rather than benzyl alcohol. Use of an alkyl silicate with the phosphoric acid insures the correct crystalline species, (VO).sub.2 H.sub.4 P.sub.2 O.sub.9, as indicated by X-ray diffraction.Type: GrantFiled: December 19, 1990Date of Patent: April 28, 1992Assignee: Akzo N.V.Inventor: Gershon J. Davis
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Patent number: 5104844Abstract: A process for preparing a multi-component catalyst for producing methacrylic acid containing phosphorus, molybdenum and vanadium comprising using in preparing the catalyst, at least one number selected from the group consisting of the oxide, carbonates, acetates and hydroxides of each catalyst-constituting element as a source of the element; dissolving or dispersing the selected sources of the catalyst-constituting elements in water; adding at least one member selected from the group consisting of ammonium carbonate, ammonium hydrogen-carbonate, ammonium sulfate and ammonium hydrogen-sulfate to the resulting aqueous solution or dispersion; removing water therefrom and then heat-treating the residual product.Type: GrantFiled: February 13, 1991Date of Patent: April 14, 1992Assignee: Mitsubishi Rayon Co., Ltd.Inventors: Shinji Yamamoto, Yutaka Kinoshita, Motomu Oh-Kita
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Patent number: 5102846Abstract: In a process for producing a catalyst having a composition represented by the following formula usable to produce methacrylic acid by the gas-phase catalytic oxidation of methacrolein with molecular oxygen,P.sub.a Mo.sub.b Cu.sub.c V.sub.d X.sub.e Y.sub.f Z.sub.g O.sub.hwherein P, Mo, Cu, V and O are phosphorus, molybdenum, copper, vanadium and oxygen, respectively, X is at least one element selected from the group consisting of arsenic, antimony, bismuth, germanium, zirconium, tellurium and silver, Y is at least one element selected from the group consisting of iron, zinc, chromium, magnesium, tantalum, manganese, barium, boron, gallium, cerium and lanthanum, Z is at least one element selected from the group consisting of potassium, rubidium, cesium and thallium, a, b, c, d, e, f, g and h are an atomic ratio of each element, and when b is 12, a is 0.5 to 3, c is 0.01 to 2, d is 0.01 to 3, e is 0.01 to 3, f is 0 to 3, g is 0.Type: GrantFiled: October 16, 1990Date of Patent: April 7, 1992Assignee: Mitsubishi Rayon Co., Ltd.Inventors: Toru Kuroda, Motomu Oh-Kita, Kazuhiro Ishii
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Patent number: 5102847Abstract: In a process for preparing a catalyst for producing methacrylic acid represented by the formula,P.sub.a Mo.sub.b V.sub.c Cu.sub.d Bi.sub.e X.sub.f Y.sub.g O.sub.hwherein P, Mo, V, Cu, Bi and O are phosphorus, molybdenum, vanadium, copper, bismuth and oxygen, respectively, X is at least one element selected from the group consisting of potassium, rubidium, cesium and thallium, Y is at least one element selected from the group consisting of antimony, zinc, iron, cerium, magnesium, chromium, indium, tellurium, manganese, tin, germanium, arsenic, boron, silicon, selenium, zirconium, silver, tantalum and tungsten, a, b, c, d, e, f, g and h are an atomic ratio of each element, and when b is 12, a is 0.1 to 3, c is 0.01 to 2, d is 0.01 to 2, e is 0.05 to 1, f is 0.01 to 2 and g is 0.Type: GrantFiled: February 14, 1991Date of Patent: April 7, 1992Assignee: Mitsubishi Rayon Co., Ltd.Inventors: Shinji Yamamoto, Yutaka Kinoshita, Masako Usui, Motomu Oh-Kita
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Patent number: 5093521Abstract: A process for producing methacrylic acid which includes subjecting methacrolein to gaseous phase catalytic oxidation using molecular oxygen and a catalyst represented by the general formula:P.sub.a Mo.sub.b V.sub.c Fe.sub.d Ce.sub.e (NH.sub.4).sub.f X.sub.g Y.sub.h Z.sub.i O.sub.jwherein P, Mo, V, Fe, Ce, NH.sub.4 and O represent phosphorus, molybdenum, vanadium, iron, cerium, ammonium group and oxygen, respectively; X represents at least one element selected from the group consisting of copper, zinc, bismuth, chromium, magnesium, silver, tantalum and lanthanum; Y represents at least one element selected from the group consisting of arsenic, antimony, zirconium, barium, manganese, germanium and tellurium; Z represents at least one element selected from the group consisting of potassium, rubidum, cesium and thallium; a, b, c, d, e, g, h, i and j each represents an atomic ratio of each element, and b is 12, a is in a range of 0.5-3, c is in a range of 0.01-3, d is in a range of 0.01-2, e is in a range of 0.Type: GrantFiled: July 6, 1989Date of Patent: March 3, 1992Assignee: Mitsubishi Rayon Co., Ltd.Inventors: Motomu Oh-Kita, Toru Kuroda, Yutaka Kinoshita, Kazuhiro Ishii
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Patent number: 5093298Abstract: Novel maleic anhydride catalysts comprising phosphorus-vanadium oxides and phosphorus-vanadium-co-metal oxides and the process for making such catalysts are disclosed. These catalysts under reaction conditions for the manufacture of maleic anhydride from butane feedstock do not expand to the point of crushing and producing fines. Moreover, the halogen level of such a catalyst is reduced.Type: GrantFiled: July 31, 1990Date of Patent: March 3, 1992Assignee: Amoco CorporationInventors: Muin S. Haddad, William S. Eryman
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Patent number: 5091354Abstract: Site-specific, framework substituted heteropolyacid or a polyoxoanion catalysts useful in alkane oxidation processes.Type: GrantFiled: July 11, 1990Date of Patent: February 25, 1992Assignee: Sun Refining and Marketing CompanyInventors: Paul E. Ellis, Jr., James E. Lyons
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Patent number: 5079207Abstract: Disclosed is a process for making an .alpha., .beta.-unsaturated monoitrile by the catalytic reaction of a paraffin containing 3-5 carbon atoms with molecular oxygen and ammonia by catalytic contact of the foregoing reactants in a reaction zone with a metal oxide catalyst containing the elements indicated by the empirical formula,V.sub.v A.sub.a D.sub.d Sn.sub.m Sb.sub.n Cu.sub.c O.sub.x (formula 1)in the relative atomic proportions indicated by the subscripts, whereA is selected from Te and BiD is one or more optional elements selected from Mo, W, Ti, Ge, Ce, La, Cr, Mn, Mg, Ca, Co, Ni, Fe, Nb, Ta, Ag, Zn, Cd, B, P, Na, K and Cs, anda is 0.001 to 30d is zero to 30c is 0.001 to 30m is 0.1 to 60n is 0.1 to 60n/v is>12 and<100m+n is.gtoreq.v+a+c+d, andx is determined by the valence requirements of the elements present, andwherein the reactants fed to the reaction zone contain a mole ratio of said paraffin:NH.sub.3 in the range from 2 to 16 and a mole ratio of said paraffin:O.sub.Type: GrantFiled: December 3, 1990Date of Patent: January 7, 1992Assignee: The Standard Oil CompanyInventors: James F. Brazdil, Linda C. Glaeser, Mark A. Toft
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Patent number: 5070060Abstract: An improvement in the oxidation catalyst used for the partial oxidation of n-butane and containing vanadium and phosphorus, zinc and lithium mixed oxides which comprises adding a molybdenum compound modifier in an amount of from about 0.0005 to 0.025/1 Mo/V to the catalyst during the digestion of the reduced vanadium compound by concentrated phosphoric acid. The addition of Mo produces a catalyst which is very stable more active system and longer lived than the unmodified catalyst.Type: GrantFiled: May 21, 1990Date of Patent: December 3, 1991Assignee: Scientific Design Company, Inc.Inventor: Bruno J. Barone
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Patent number: 5070061Abstract: Catalysts containing molybdenum, vanadium, phosphorus, and oxygen, optionally together with one or more metal ions, as their active constituents, are preferably disposed on an inert carrier for the oxidative dehydrogenation of isobutyric acid or its lower esters to methacrylic acid or its lower esters.Type: GrantFiled: December 7, 1990Date of Patent: December 3, 1991Assignee: Rohm GmbHInventor: Klaus Langerbeins
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Patent number: 5068215Abstract: A multi-component oxide catalyst comprising zinc and an alkali metal is described which is useful particularly for converting methane and/or natural gas to higher molecular weight hydrocarbon products such as ethane and ethylene. The catalyst is characterized by the formulaZn.sub.a A.sub.b M.sub.c M'.sub.d O.sub.xwhereinA is Li, Na, K, or mixtures thereof;M is Al, Ga, Cr, La, Y, Sc, V, Nb, Ta, Cu or mixtures thereof;M' is Cs, Rb, Mg, Ca, Sr, Ba, Sm, Pb, Mn, Sb, P, Sn, Bi, Ti, Zr, Hf, or mixtures thereof;a is from about 1 to about 20;b is from about 0.1 to about 20;c is from about 0 to about 5;d is from about 0 to about 20; andx is a number needed to fulfill the valence requirements of the other elements; provided that(i) at least one of c and d is at least 0.1; and(ii) when M' is Sn, c must be at least 0.1.Type: GrantFiled: December 11, 1989Date of Patent: November 26, 1991Assignee: Standard Oil CompanyInventors: Joseph P. Bartek, James F. Brazdil, Jr., John M. Hupp, Robert K. Grasselli