Abstract: The invention relates to a continuous process to make and isolate methylal by reacting formaldehyde and methanol with an acid catalyst under at least partial formation of methylal and water, to form a mixture M2 comprising formaldehyde, methanol, methylal, and water, separating the said mixture M2 in a distillation column B into three distinct product streams, one being a distillate taken from the column head BH which is rich in methylal, one taken from the column bottom stream BB being almost pure water, and one taken from the side of the column B below the reaction zone which stream is rich in methanol, characterised in that the ratio of the amount of substance of methanol to the amount of substance of formaldehyde in the mixture M1 is at least 3 mol/mol, and to an apparatus to be used with this process.

Abstract: The invention relates to the use of monoliths as particle filters for limiting the deactivation of catalysts during catalytic reactions in multi-tubular reactors. The invention is particularly well-suited for catalytic oxidation reactions in the gaseous phase. The invention also relates to multi-tubular reactors including monoliths as particle filters.

Abstract: Provided is a process for producing aldehydes or ketones by oxidizing alcohols with oxygen, which comprises oxidizing alcohols to aldehydes or ketones in an organic solvent at room temperature with oxygen or air as an oxidant, wherein ferric nitrate (Fe(NO3)3.9H2O), 2,2,6,6-tetramethylpiperidine N-oxyl (TEMPO) and an inorganic chloride are used as catalysts, the reaction time is 1-24 hours, and the molar ratio of said alcohols, 2,2,6,6-tetramethylpiperidine N-oxyl and the inorganic chloride is 100:1˜10:1˜10:1˜10. The present process has the advantages of high yield, mild reaction conditions, simple operation, convenient separation and purification, recoverable solvents, substrates used therefor being various and no pollution, and therefore it is adaptable to industrialization.

Abstract: A process for the fixed bed oxidation of methanol to formaldehyde wherein the bed comprises at least two layers having different catalytic activity, wherein the layer of lower activity is comprised in the part of the bed from which the reactant gas mixture enters and its activity is calibrated so that the maximum hot spot temperature in the layer is comprised between 350° C. and 430° C. and is higher than the maximum hot spot temperature of the layer of greater activity formed by pure catalyst, and wherein during the period in which the situation of the maximum hot spot temperature of the layer of lower activity remains at the values cited above, the conversion of methanol is higher than 96% by mols.

Abstract: A method of preparing a catalyst for producing acrolein by oxidation of propylene at high space velocity, said catalyst is a Mo—Bi—Fe—Co based composite metal oxide. Producing unsaturated aldehyde via partial oxidation of lower unsaturated olefin at high space velocity using said catalyst is suitable for process with or without off-gas recirculating. Said catalyst is prepared by co-precipitation, the reaction conditions for using said catalyst to produce unsaturated aldehyde are, the space velocity of unsaturated lower olefin relative to catalyst being 120˜200 h-1(STP), reaction temperature being 300˜420° C. and absolute pressure being 0.1˜0.5 MPa; a single-stage unsaturated lower olefin conversion ratio of greater than 98.0% and carbon oxide yield of less than 3.3% with an overall yield of unsaturated lower aldehyde and acid of greater than 94.0% are obtained. The process to prepare the said catalyst is simple, easy to be repeated, and capable of industrial scale-up.

Abstract: A process for producing a ringlike oxidic shaped body by mechanically compacting a pulverulent aggregate introduced into the fill chamber of a die, wherein the outer face of the resulting compact corresponds to that of a frustocone.

Abstract: A process for the fixed bed oxidation of methanol to formaldehyde wherein the bed comprises at least two layers having different catalytic activity, wherein the layer of lower activity is comprised in the part of the bed from which the reactant gas mixture enters and its activity is calibrated so that the maximum hot spot temperature in the layer is comprised between 350° C. and 430° C. and is higher than the maximum hot spot temperature of the layer of greater activity formed by pure catalyst, and wherein during the period in which the situation of the maximum hot spot temperature of the layer of lower activity remains at the values cited above, the conversion of methanol is higher than 96% by mols.

Abstract: Two zone (11, 12; 21, 22; 31, 32; 41, 42) fluidized bed reactor (10, 20, 30, 40), wherein the upper zone (11, 21, 31, 41) presents a different section than the lower zone (12, 22, 32, 42). In one of the two zones (11, 12; 21, 22; 31, 32; 41, 42), a zone of reducing atmosphere is created and, in the other zone, a zone of oxidising atmosphere is created. In a preferred embodiment, the section of the upper zone (11, 21, 31, 41) is larger than that of the lower zone (12, 22, 32, 42), creating a reducing atmosphere in the upper zone (11, 21, 31, 41) and an oxidising atmosphere in the lower zone (12, 22, 32, 42). Rows of flow distributor tubes exist in the upper zone (11, 21, 31, 41) to avoid the appearance of dead zones.

Abstract: A process is disclosed for the synthesis of formaldehyde from methane starting with the oxychlorination of methane to produce methylene chloride. Hydrolysis of methylene chloride yields the product formaldehyde. Gaseous formaldehyde is condensed for shipment. Byproduct chloroform and carbon tetrachloride are recovered and hydrogenated to provide additional methylene chloride.

Abstract: The invention relates to the use of monoliths as particle filters for limiting the deactivation of catalysts during catalytic reactions in multi-tubular reactors. The invention is particularly well-suited for catalytic oxidation reactions in the gaseous phase. The invention also relates to multi-tubular reactors including monoliths as particle filters.

Abstract: Methods for controlling series or series-parallel reactions are described. Novel microchannel apparatus having mesoporous structures adjacent to bulk flow paths are described. Methods of synthesizing formaldehyde from methanol are also described.

Abstract: The invention relates to a coated catalyst, especially for oxidation of methanol to formaldehyde, which, on an inert, preferably essentially nonporous, support body, has at least one coating which comprises, before the removal of the organic fractions of components b) and c): (a) oxides, or precursor compounds convertible to the corresponding oxides, of molybdenum and iron, where the molar ratio of Mo:Fe is between 1:1 and 5:1, and optionally further metallic components or metal oxide components or precursor compounds convertible to the corresponding oxides, (b) at least one organic binder, preferably an aqueous dispersion of copolymers, especially selected from vinyl acetate/vinyl laurate, vinyl acetate/ethylene, vinyl acetate/acrylate, vinyl acetate/maleate, styrene/acrylate or mixtures thereof, and (c) at least one further component selected from the group consisting of SiO2 sol or precursors thereof, Al2O3 sol or precursors thereof, ZrO2 sol or precursors thereof, TiO2 sol or precursors thereof, waterglas

Abstract: A process is disclosed for the synthesis of formaldehyde from methane starting with the oxychlorination of methane to produce methylene chloride. Hydrolysis of methylene chloride yields the product formaldehyde. Byproduct chloroform and carbon tetrachloride are recovered and hydrogenated to provide additional methylene chloride.

Abstract: The present invention discloses a novel use of a catalyst with core-porous shell structure, which includes carrying out an oxidation of an alcohol in vapor phase and in the presence of the catalyst with core-porous shell structure to form an aldehyde or ketone, wherein the catalyst with core-porous shell structure is constituted of a core material and a porous shell material. The core material is a metal having a catalytic activity, and the shell material is a porous inorganic oxide.

Abstract: A process for preparing formaldehyde by gas-phase oxidation of methanol vapor by means of a gas stream comprising molecular oxygen in the presence of a fixed-bed catalyst comprising iron and molybdenum, wherein the process is carried out in a reactor (1) having heat-exchange plates (2) which are arranged in the longitudinal direction of the reactor (1) and have a spacing between them and through which a heat transfer medium flows, inlet and outlet facilities (3, 4) for the heat transfer medium to the heat-exchange plates (2) and also gaps (5) between heat-exchange plates (2) in which the fixed-bed catalyst is present and into which the methanol vapor and the gas stream comprising molecular oxygen are passed, is described.

Abstract: The present invention relates to a process of oxidation of alcohols selectively to aldehydes or ketones with molecular oxygen using a TEMPO based catalyst, Fe-bipyridyl or Fe-phenantroline co-catalyst and N-bromosuccinimide promoter in acetic acid solvent. The oxidation takes places at high rates and high aldehyde selectivity at temperatures in the range 45-50° C. and oxygen or air pressures of 0-15 psi. The alcohol conversion of 95-100% and aldehyde selectivity higher than 95% are achieved over 3-4 hours reaction time. Aldehydes such as 3,3-dimethyl-1-butanal can be produced efficiently using the present invention.

Abstract: Process for removing methanol from formaldehyde-containing solutions. The present invention relates to a process for removing methanol from formaldehyde-containing solutions, with methanol being converted into formaldehyde dimethyl acetal by reactive distillation in the presence of an acidic fixed-bed catalyst, and the resultant mixture comprising methanol, formaldehyde dimethyl acetal and possibly other impurities being distilled off.

Abstract: A method wherein a methanol-containing gas stream is passed in contact with a catalyst comprising a supported or unsupported bulk vanadate catalyst in the presence of an oxidizing agent for a time sufficient to convert at least a portion of the methanol to formaldehyde (CH2O).

Abstract: A method for formaldehyde production through catalytic oxidation of methanol, comprising the steps of feeding to a first oxidation catalytic bed (2) a gas flow comprising methanol and oxygen at a predetermined crossing linear flow rate, obtaining at the outlet of said first catalytic bed (2) a flow of gaseous reaction products comprising unreacted methanol, and feeding the flow of gaseous products to a second oxidation catalytic bed (6) is distinguished by the fact that the flow of gaseous reaction products comprising unreacted methanol is fed to the second catalytic bed (6) with a crossing linear flow rate substantially equal to said predetermined first catalytic bed (2) feeding flow rate.

Abstract: A process is provided for the manufacture of formaldehyde from methyl bromide. In the process, methyl bromide is oxidized with air over a catalyst to give formaldehyde and hydrogen bromide. In a preferred embodiment of the invention, a mixture of two different catalysts are employed, one to promote hydrolysis of methyl bromide to methyl alcohol and the other to promote the oxidation of methyl alcohol to formaldehyde.

Abstract: Feeds comprising methanol, dimethyl ether or a mixture of the two are oxidized by contacting the feed with an oxygen-containing gas and a supported heteropolyacid catalyst containing molybdenum or molybdenum and vanadium. The primary products are methylal (dimethoxymethane) and methyl formate. Production of dimethyl ether from methanol can be inhibited by partial deactivation of acid sites on the Keggin catalyst.

Abstract: A method for formaldehyde production through catalytic oxidation of methanol, comprising the steps of feeding to a first oxidation catalytic bed (2) a gas flow comprising methanol and oxygen at a predetermined crossing linear flow rate, obtaining at the outlet of said first catalytic bed (2) a flow of gaseous reaction products comprising unreacted methanol, and feeding the flow of gaseous products to a second oxidation catalytic bed (6) is distinguished by the fact that the flow of gaseous reaction products comprising unreacted methanol is fed to the second catalytic bed (6) with a crossing linear flow rate substantially equal to said predetermined first catalytic bed (2) feeding flow rate.

Abstract: The present invention relates to a process of oxidation of alcohols selectively to aldehydes or ketones with NaOCl using a TEMPO—borate catalyst system. It is shown that the oxidation can be efficiently carried out without KBr additives under solvent free conditions. Aldehydes such as 3,3-dimethylbutyraldehyde can be produced efficiently using the present invention.

Abstract: The method of the present invention involves the in situ formation of metal-molybdate catalyst particles active for methanol oxidation to formaldehyde, with iron as an example, the catalyst is made by mixing particulate forms of Fe2O3 and MoO3 which form an active Fe2(MoO4)3/MoO3 component inside the reactor during methanol oxidation.

Abstract: A process and apparatus for oxidizing methanol in a gas stream into formaldehyde in a fixed bed reactor. The process first introduces a gas stream into a fixed bed reactor. The fixed bed reactor contains a catalyst bed having a depth, a width, a length, an inlet, an upstream region, a downstream region and an outlet. Preferably, the inlet, the upstream region, the downstream region and the outlet are provided in the order stated. A vanadia-titania catalyst is provided in the upstream region and a molybdena-titania catalyst is provided in the downstream region. The vanadia-titania catalyst in the upstream region is substantially free of MoO3 and initially (i.e., during oxidation some V2O5 may sublime and migrate to the downstream region) the molybdena-titania catalyst in the downstream region is substantially free of V2O5. Next, the gas stream is contacted with the vanadia-titania catalyst under oxidizing conditions.

Abstract: A process and a catalyst reaction zone comprising one or more fixed bed reactors for oxidizing methanol in a reactant gas feed stream to formaldehyde. According to one embodiment, the process comprises introducing the reactant gas feed stream into an upstream region containing a vanadia-titania first catalyst (substantially free of a volatile MoO3 species) under oxidizing conditions to form a partially oxidized reactant gas feed stream which is then introduced under oxidizing conditions into a downstream region containing a metal molybdate second catalyst to further oxidize any residual methanol contained therein. According to another embodiment, a fixed bed reactor comprising an upstream region and a downstream region containing the aforementioned vanadia-titania and metal molybdate catalysts, respectively, is utilized to implement the inventive process to yield a product gas stream containing formaldehyde preferably at a conversion of 85% or more and a selectivity of 90% or more.

Abstract: In a process for preparing formaldehyde from methanol by dehydrogenation in a reactor in the presence of a catalyst at a temperature in the range from 300 to 1000° C., the catalyst is generated spatially separately from the reactor and at a temperature above the dehydrogenation temperature.

Abstract: Processes for the preparation of 3-alkoxyalkanols useful as solvents for coating materials, photoresists, or the like.

Abstract: A process and fixed bed reactor for oxidizing methanol in a reactant gas feed stream to formaldehyde. The process comprises introducing the reactant gas feed stream into an upstream region containing a first metal molybdate catalyst (substantially free of a volatile Mo/MoO3 species) under oxidizing conditions to form a partially oxidized reactant gas feed stream which is then introduced under oxidizing conditions into a downstream region containing a second metal molybdate catalyst to further oxidize any residual methanol contained therein. A fixed bed reactor comprising an upstream region and a downstream region containing the aforementioned first and second metal molybdate catalysts, respectively, is utilized to implement the inventive process to yield a product gas stream containing formaldehyde preferably at a conversion of 85% or more and a selectivity of 90% or more.

Abstract: Processes for producing citraconic anhydride and citraconic acid using porous materials with specific surface acidities and surface areas are described. The preferred catalyst is a porous gamma alumina. Itaconic acid is produced from citraconic acid. Itaconic acid is an intermediate to a variety of compounds including polymers.

Abstract: In a process for preparing formaldehyde from methanol by dehydrogenation in a reactor in the presence of a catalyst at a temperature in the range from 300 to 1000° C., a carrier gas stream which has a temperature above the dehydrogenation temperature is fed to the reactor.

Abstract: A process for selectively oxidizing an organic molecule by reacting said organic molecule and oxygen in the presence of a selective oxidation catalyst supported on a mesh-like structure.

Abstract: Preparing an aldehyde from an alcohol by contacting the alcohol in the presence of oxygen with a catalyst prepared by contacting an intimate mixture containing metal oxide support particles and particles of a catalytically active metal oxide from Groups VA, VIA, or VIIA, with a gaseous stream containing an alcohol to cause metal oxide from the discrete catalytically active metal oxide particles to migrate to the metal oxide support particles and to form a monolayer of catalytically active metal oxide on said metal oxide support particles.

Abstract: A particularly useful process which includes the steps of providing a feedstream comprising methanol, a soluble condensation promoting component capable of activating a heterogeneous acidic catalyst and a source of formaldehyde formed by conversion of methanol in the presence of a catalyst comprising copper and zinc; and heating this feedstream with the heterogeneous acidic catalyst in a catalytic distillation column to convert methanol and formaldehyde present to methylal and higher polyoxymethylene dimethyl ethers and to separate the methylal from the higher polyoxymethylene dimethyl ethers is disclosed. Advantageously, methylal and higher polyoxymethylene dimethyl ethers are formed and separated in a catalytic distillation column. By including within the column a section containing an anion exchange resin, an essentially acid-free product is obtained.

Abstract: Alkylene glycol is oxidized in a vapor phase in the presence of alcohol (a), oxygen, and a catalyst (a) (primary reaction). &agr;-oxoaldehyde, and alcohol (b) or olefin, are oxidized in a vapor phase in the presence of oxygen and a catalyst (b) (secondary reaction). A molar ratio of the alkylene glycol to the alcohol (a) is preferably in a range of 1/100 to 5/1. It is preferable that one same compound is used as the alcohol (a) and the alcohol (b). In the case where the primary and secondary reactions are successively executed, a reaction device in which a primary reactor and a secondary reactor are connected in a two-stage connection type is preferably used. This ensures that a method is provided that is capable of producing &agr;-oxoaldehyde at a higher yield than conventionally, and further, that is capable of stably obtaining an &agr;-oxoaldehyde solution or gas with a higher concentration than conventionally.

Abstract: A particularly useful process which includes the steps of providing a feedstream comprising a soluble condensation promoting component capable of activating a heterogeneous acidic catalyst and a source of formaldehyde formed by conversion of dimethyl ether in the presence of a catalyst comprising silver as an essential catalyst component; and heating the feedstream with the heterogeneous acidic catalyst in a catalytic distillation column to convert methanol and formaldehyde present to methylal and higher polyoxymethylene dimethyl ethers and to separate the methylal from the higher polyoxymethylene dimethyl ethers is disclosed. Advantageously, methylal and higher polyoxymethylene dimethyl ethers are formed and separated in a catalytic distillation column.

Abstract: A method wherein a methanol-containing waste gas stream, such as a pulp mill waste stream which contains methanol and other waste products, including methyl mercaptans, is passed in contact with a catalyst comprising a supported or unsupported bulk metal oxide catalyst in the presence of an oxidizing agent; preferably the gas stream is contacted with the catalyst, in the presence of the oxidizing agent, for a time sufficient to convert at least a portion of the methanol to formaldehyde (CH2O).

Abstract: Quadridentate Cu.sup.II and Zn.sup.II phenoxyl complexes and phenoxyl radical complexes thereof, in which one ligand L is bonded to each metal atom and H.sub.2 L stands for the general formula ##STR1## in which the bridge-unit Q stands for --S--, --O--, --N(R.sup.3)--, --P(R.sup.4)--, or ortho-NH--C.sub.6 H.sub.4 --NH-- and R.sup.1 and R.sup.2 stand for radical-stabilizing residues.Preferred radical complexes include ##STR2## The radical complexes are oxidation catalysts for oxidizing organic substrates with O.sub.2 in the course of which H.sub.2 O.sub.2 is also formed.

Abstract: A process for the catalytic conversion of methanol to formaldehyde wherein a gas stream containing methanol and oxygen is contacted with a silver catalyst in a first conversion zone containing a silver catalyst to produce an effluent containing formaldehyde, unreacted methanol, and oxidation byproducts; and contacting the first zone effluent with a copper catalyst in a second conversion zone for further conversion of the unreacted methanol. No molecular oxygen is added to the first stage effluent or to the second conversion zone.

Abstract: In a process for preparing carbonyl compounds of the formula ##STR1## where R.sup.1 is a hydrogen atom or an alkyl radical having from 1 to 3 carbon atoms, R.sup.2 is a hydrogen atom or a radical of the formula ##STR2## where R.sup.3 is a hydrogen atom or together with R.sup.4 is an oxygen atom, R.sup.4 is the radical OR.sup.6 or together with R.sup.3 is an oxygen atom, R.sup.5 is a hydrogen atom, an alkyl radical having from 1 to 8 carbon atoms or a cyclohexyl or cyclopentyl radical and R.sup.6 is an alkyl radical having from 1 to 4 carbon atoms, a cyclohexyl or cyclopentyl radical or a radical of the formula --CH.sub.2 --CHO or --CH.sub.2 --CH.sub.2 --O--CH.sub.2 --CHO, by gas-phase oxidation of methanol or alcohols of the formula ##STR3## where R.sup.1 and R.sup.5 are as defined above and R.sup.7 is a hydrogen atom or a radical OR.sup.8 and R.sup.8 is a hydrogen atom, an alkyl radical having from 1 to 4 carbon atoms, a cyclohexyl or cyclopentyl radical or a radical for the formula --CH.sub.2 --CH.sub.

Abstract: The present invention relates to a process for the preparation of carbonyl compounds of the formula ##STR1## in which R.sup.1 denotes a hydrogen atom or an alkyl radical containing from 1 to 3 carbon atoms, R.sup.2 denotes a hydrogen atom or a radical of the formula ##STR2## in which R.sup.3 denotes a hydrogen atom or, together with R.sup.4, an oxygen atom, R.sup.4 denotes the radical OR.sup.6 or, together with R.sup.3, an oxygen atom, R.sup.5 denotes a hydrogen atom or an alkyl radical containing from 1 to 8 carbon atoms or a cyclohexyl or cyclopentyl radical, and R.sup.6 denotes an alkyl radical containing from 1 to 4 carbon atoms, a cyclohexyl or cyclopentyl radical or a radical of the formula--CH.sub.2 --CHO or --CH.sub.2 --CH.sub.2 --O--CH.sub.2 --CHO,by gas-phase oxidation of methanol or alcohols of the formula ##STR3## in which R.sup.1 and R.sup.5 have the meanings specified above and R.sup.7 denotes a hydrogen atom or a radical OR.sup.8, and R.sup.

Abstract: A process for preparing formaldehyde by oxidative dehydrogenation of methanol comprises passing a gas mixture (i) comprisinga) from 0.1 to 50% by volume of methanol,b) from 0.1 to 30% by volume of oxygen,c) from 0 to 50% by volume of nitrogen oxide andd) from 0 to 60% by volume of water at from 150 to 800.degree. C. through a phosphorus-doped silver catalyst fixed bed (a) and applying from 0.01 to 100 ppm by weight of phosphorus, based on the phosphorus-doped silver catalyst fixed bed, in the form of a finely divided phosphorus compound having a melting point or decomposition temperature of more than 500.degree. C. (phosphorus compound P) to the phosphorus-doped silver catalyst fixed bed (a) per kg of methanol which is passed through in the form of the gas mixture (i) per cm.sup.2 of the cross-sectional area of the phosphorus-doped silver catalyst fixed bed (a).

Abstract: A process for the heterogeneous exothermic synthesis of formaldehyde, in particular in a reactor of the type comprising a plurality of adiabatic catalytic beds connected in series, provides the step of feeding to the reactor the methanol necessary for the synthesis distributed in at least two portions, each fed to respective distinct catalytic beds.

Abstract: A process for the heterogeneous exothermic synthesis of formaldehyde, in particular in reactors of the type comprising a plurality of adiabatic catalytic beds connected in series, provides the step of flowing the gaseous reagents across at least one of the catalytic beds with substantially radial flow.

Abstract: A method wherein a methanol-containing waste gas stream, such as a pulp mill waste stream which contains methanol and other waste products, including methyl mercaptans, is passed in contact with a catalyst comprising certain supported metal oxides in the presence of an oxidizing agent; preferably the gas stream is contacted with the catalyst, in the presence of the oxidizing agent, for a time sufficient to convert at least a portion of the methanol to formaldehyde (CH.sub.2 O).

Abstract: The process uses a supply column and additional heat exchangers associated with absorption columns. Air and methanol from outside and a subcurrent of methanol, originating from a cold methanol current exiting from the supply column, are fed to the supply column. This exiting current recirculates through the additional heat exchangers and is divided into the subcurrent which returns to the supply column and another subcurrent which is fed to an evaporator. A methanol-air mixture exits from the head of the supply column and is fed to an evaporator. The cold methanol is cooled in the supply column by evaporation of the methanol forming part of the methanol-air mixture.

Abstract: A process including a first stage wherein a feed gas stream containing acrolein originating, for example from the gas-phase oxidation of propylene to acrolein, is fractionated into a gaseous effluent and a liquid stream in a cooling column operating such that the temperature of the liquid stream at the bottom of the column is lower than or equal to the condensation temperature of the feed gas stream, the difference in temperature not exceeding 20.degree. C. and, a second stage, wherein the gaseous effluent is condensed at a temperature that is lower than 20.degree. C., to give a liquid fraction and a purified gaseous fraction, is disclosed. An apparatus for carrying on the purification process is also disclosed.

Abstract: A configuration of cylindrical catalyst granules displays a trilobed or triangular cross-section provided with three through-bores equidistant from each other, each of which through-bores has its axis parallel to the axis of the cylindrical granule.

Abstract: A configuration of cylindrical catalyst granules displays a trilobed or triangular cross-section provided with three through-bores equidistant from each other, each of which through-bores has its axis parallel to the axis of the cylindrical granule (FIG. 1).

Abstract: A method for preparing methacrolein comprises subjecting isobutylene or a tertiary butanol to gas phase catalytic oxidation with molecular oxygen in the presence of a catalyst which comprises a mixture of a composition (I) represented by the following general formula I:Mo.sub.a Bi.sub.b Fe.sub.c X.sub.d Y.sub.e Z.sub.f O.sub.g Iwherein X represents at least one element selected from the group consisting of Ni and Co; Y represents at least one element selected from the group consisting of K, Rb, Cs and Tl; Z represents at least one element selected from the group consisting of those belonging to Group 2, 3, 4, 5, 6, 7, 11, 12, 13, 14, 15 and 16 of Periodic Table in accordance with IUPAC nomenclature (1989); and a, b, c, d, e, f and g each represents an atomic ratio of each corresponding element, when a is assumed to be 12, b is 0.