WO2017009273A1 - Catalyseur et procédé permettant le couplage oxydatif de méthane - Google Patents

Catalyseur et procédé permettant le couplage oxydatif de méthane Download PDF

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Publication number
WO2017009273A1
WO2017009273A1 PCT/EP2016/066386 EP2016066386W WO2017009273A1 WO 2017009273 A1 WO2017009273 A1 WO 2017009273A1 EP 2016066386 W EP2016066386 W EP 2016066386W WO 2017009273 A1 WO2017009273 A1 WO 2017009273A1
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Prior art keywords
manganese
catalyst composition
methane
alkali metal
oxide compound
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PCT/EP2016/066386
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English (en)
Inventor
Hendrik Dathe
Sivaramakrishnan VENKATRAMAN
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Shell Internationale Research Maatschappij B.V.
Shell Oil Company
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Publication of WO2017009273A1 publication Critical patent/WO2017009273A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2/00—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms
    • C07C2/76—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen
    • C07C2/82—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen oxidative coupling
    • C07C2/84—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen oxidative coupling catalytic
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/32—Manganese, technetium or rhenium
    • B01J23/34—Manganese
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/04—Mixing
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/08—Heat treatment
    • B01J37/082—Decomposition and pyrolysis
    • B01J37/088—Decomposition of a metal salt
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2523/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00
    • C07C2523/02—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00 of the alkali- or alkaline earth metals or beryllium
    • C07C2523/04—Alkali metals
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2523/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00
    • C07C2523/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • C07C2523/32—Manganese, technetium or rhenium
    • C07C2523/34—Manganese
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/50—Improvements relating to the production of bulk chemicals
    • Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts

Definitions

  • the present invention relates to a catalyst and a process for the oxidative coupling of methane.
  • Methane is a valuable resource which is used not only as a fuel, but is also used in the synthesis of chemical compounds such as higher hydrocarbons .
  • the oxidative coupling of methane converts methane into saturated and unsaturated, non-aromatic hydrocarbons having 2 or more carbon atoms, including ethylene.
  • a gas stream comprising methane is
  • ethane molecules are first coupled into one ethane molecule, which is then dehydrogenated into ethylene.
  • Said ethane and ethylene may further react into saturated and unsaturated hydrocarbons having 3 or more carbon atoms, including propane, propylene, butane, butene, etc.
  • the gas stream leaving an OCM process contains a mixture of water, hydrogen, carbon monoxide, carbon dioxide, methane, ethane, ethylene, propane, propylene, butane, butene and saturated and unsaturated hydrocarbons having 5 or more carbon atoms .
  • the conversion that can be achieved in an OCM process is relatively low. Besides, at a higher conversion, the selectivity decreases so that it is generally desired to keep the conversion low. As a result, a relatively large amount of unconverted methane leaves the OCM process.
  • the proportion of unconverted methane in the OCM product gas stream may be as high as 50 to 60 mol% based on the total molar amount of the gas stream. This unconverted methane has to be recovered from the desired products, such as ethylene and other
  • a further difficulty with OCM processes is that a competing reaction that takes place is the oxidation of methane to carbon dioxide and water.
  • one of the best-performing catalysts that has been found to date in the OCM field comprises manganese, tungsten and sodium on a silica carrier.
  • the oxidative coupling of methane in the presence of said catalyst is studied in Applied Catalysis A: General 343 (2008) 142-148, Applied Catalysis A: General 425-426 (2012) 53-61, Fuel 106 (2013) 851-857, US 2014/0080699 Al and US 6596912 Bl .
  • US 4499322 A discloses catalyst compositions comprising (a) at least one reducible oxide of at least one metal selected from the group consisting of Mn, Sn, In, Ge, Pb, Sb and Bi; and (b) a promoting amount of at least one promoter selected from the group consisting of alkali metals and compounds thereof.
  • the stability of said catalyst compositions is further enhanced by
  • the support in said catalyst compositions may either be a conventional support material such as silica, alumina, titania or zirconia, or it may be the alkali promoter such as Na 2 0 or K 2 0. Examples 4, 5 and Comparative Example B in US
  • Example 4 tests a bulk oxide
  • NaMn oxide which comprises NaMn0 2 and NaO .7Mn0 2 and which was made by calcining sodium
  • Example 5 tests a bulk oxide designated as "LiMn oxide” which was prepared from Li 2 MnC>3 as precursor by calcining under similar conditions to those in Example 4; and Comparative Example B tests a bulk manganese oxide designated as "Mn oxide” which comprises Mn 2 0 3 and which was prepared by calcining manganese acetate under similar conditions to those in Example 4.
  • US 4,758,484 describes a positive-electrode material for a rechargeable battery prepared by heat treatment of a mixture of manganese dioxide and lithium salt in the temperature range of 300 °C-430 °C.
  • US 2012/0321954 and US 2013/0171525 describe a positive-electrode material for a rechargeable battery prepared by a molten salt method.
  • the present invention has surprisingly found that certain catalyst compositions display advantageous performance in the oxidative coupling of methane.
  • a catalyst composition comprising a ternary oxide compound, said ternary oxide compound comprising one or more alkali metals and manganese and having been prepared by reacting one or more alkali metal compounds selected from alkali metal hydroxide, alkali metal carbonate and alkali oxide with one or more manganese compounds selected from manganese oxides, manganese hydroxide, manganese acetate and manganese nitrate .
  • alkali metal compounds selected from alkali metal hydroxide, alkali metal carbonate and alkali oxide, and
  • manganese oxides manganese hydroxide, manganese acetate and manganese nitrate
  • a process for the oxidative coupling of methane comprising converting methane to one or more C2+ hydrocarbons, wherein said process comprises contacting a reactor feed comprising methane and oxygen with the afore-mentioned catalyst composition.
  • Figure 1 is a schematic diagram showing a typical reactor set-up for oxidative coupling of methane.
  • FIGS 2 to 4 show the results obtained for the various catalysts tested.
  • Figure 5 shows an X-ray diffraction (XRD) pattern of a Li 2 Mn0 3 catalyst composition according to the present disclosure .
  • methane (CH 4 ) conversion means the mole fraction of methane converted to product (s) .
  • Cx selectivity refers to the percentage of converted reactants that went to product (s) having carbon number x and “Cx+ selectivity” refers to the percentage of converted reactants that went to the specified product (s) having a carbon number x or more.
  • C2 selectivity refers to the percentage of converted methane that formed ethane and ethylene.
  • C2+ selectivity means the percentage of converted methane that formed compounds having carbon numbers of 2 or more.
  • Cx yield is used to define the percentage of products obtained with carbon number x relative to the theoretical maximum product obtainable. The Cx yield is calculated by dividing the amount of obtained product having carbon number x in moles by the theoretical yield in moles and multiplying the result by 100. “C2 yield” refers to the total combined yield of ethane and
  • the Cx yield may be calculated by multiplying the methane conversion by the Cx selectivity.
  • Space time yield Cx refers to the volume of products having carbon number x formed per volume of the reactor and time.
  • weight percent refers to the ratio of the total weight of the carrier, the metal-containing dopant or the metal in the dopant to the total weight of the catalyst composition the catalyst. Percentages of metals from the metal-containing dopants in the catalyst composition may be determined by XRF, as is known in the art. The metals content of catalyst composition may also be inferred or controlled via its synthesis.
  • the components of the catalyst composition are to be selected in an overall amount not to exceed 100 wt . %.
  • the term "compound” refers to the combination of a particular element with one or more different elements by surface and/or chemical bonding, such as ionic and/or covalent and/or coordinate bonding.
  • ion or “ionic” refers to an electrically chemical charged moiety; “cation” or “cationic” being positive, “anion” or “anionic” being negative, and
  • oxygen or “oxyanionic” being a negatively charged moiety containing at least one oxygen atom in combination with another element (i.e., an oxygen-containing anion) . It is understood that ions do not exist in vacuo, but are found in combination with charge-balancing counter ions when added.
  • oxidic refers to a charged or neutral species wherein an element in question is bound to oxygen and possibly one or more different elements by surface and/or chemical bonding, such as ionic and/or covalent and/or coordinate bonding.
  • an oxidic compound is an oxygen-containing compound which also may be a mixed, double or complex surface oxide.
  • Illustrative oxidic compounds include, but are not limited to, oxides
  • hydroxides, nitrates, sulfates, carboxylates, carbonates, bicarbonates , oxyhalides, etc. as well as surface species wherein the element in question is bound directly or indirectly to an oxygen either in the substrate or the surface .
  • the one or more alkali metals present in the catalyst composition of the present invention are preferably selected from lithium, sodium and potassium.
  • said catalyst composition is prepared by reacting one or more lithium compounds selected from lithium hydroxide, lithium carbonate and/or lithium oxide with one or more manganese compounds selected from manganese oxides, manganese hydroxide, manganese acetate and manganese nitrate.
  • said catalyst composition is sodium
  • said catalyst composition is prepared by reacting one or more sodium compounds selected from sodium hydroxide, sodium carbonate and sodium oxide with one or more manganese compounds selected from manganese oxides, manganese hydroxide, manganese acetate and manganese nitrate.
  • the alkali metal in the catalyst composition is potassium
  • said catalyst composition is prepared by reacting one or more potassium compounds selected from potassium hydroxide, potassium carbonate and potassium oxide with one or more manganese compounds selected from manganese oxides, manganese hydroxide, and manganese acetate .
  • the alkali metal in the catalyst composition is lithium.
  • the catalyst composition of the present invention may be conveniently used without the need for a separate carrier. That is to say, in a preferred embodiment of the present invention, there is no separate carrier present in said composition.
  • the catalyst composition comprises a carrier.
  • Said carrier is not particularly limited and any carrier commonly used in the formulation of catalyst compositions for use in the oxidative coupling of methane may be used.
  • suitable carriers include silica, titania, zirconia and alumina.
  • the carrier When used in the catalyst composition of the present invention, the carrier may be present therein in an amount in the range of from 0 to 50 % by weight, relative to the total weight of the catalyst composition.
  • the ternary oxide compound has the composition M 1 M 2 Mn0 3 , wherein M 1 and M 2 are the same or different and are alkali metals selected from lithium, sodium and potassium.
  • the ternary oxide compound has the composition M 2 Mn0 3 , wherein M is an alkali metal selected from lithium, sodium and potassium. Preferably, M is lithium.
  • the manganese compound that is used in the present specification is the manganese compound that is used in the following description.
  • preparation of the ternary oxide compound is preferably selected from manganese oxides, manganese hydroxide, manganese acetate and manganese nitrate. More preferably, said manganese compound is manganese (III) oxide (Mn 2 0 3 ) .
  • the specific form of the manganese, one or more alkali metals, and any optional co-promoters and/or additional metal-containing dopants in the catalyst composition may be unknown .
  • the ternary oxide compound in the catalyst composition of the present invention is prepared by reacting one or more alkali metal compounds selected from alkali metal hydroxide, alkali metal carbonate and alkali metal oxide with one or more manganese compounds selected from manganese oxides, manganese hydroxide, manganese acetate and manganese nitrate at a reaction temperature in the range of from 700 to 1000 °C.
  • a reaction temperature in the range of from 700 to 1000 °C.
  • the mixture is a slurry comprising a suitable solvent, preferably an organic solvent, such as acetone, methanol, or ethanol .
  • a suitable solvent preferably an organic solvent, such as acetone, methanol, or ethanol .
  • the mixture or slurry is then calcined in air at a temperature in the range of from 700 to 1000 °C, in order to obtain the ternary oxide compound for use as a catalyst as disclosed herein.
  • the calcination temperature is at least 720 °C, more
  • the calcination temperature is at most 900 °C, more
  • the catalyst composition is:
  • the catalyst composition consists essentially of a ternary oxide compound as disclosed herein.
  • the ternary oxide compound has a single phase crystalline structure. Typically, said ternary oxide compound has a monoclinic structure.
  • the ternary oxide compound is single-phase monoclinic Li 2 Mn0 3 .
  • the catalyst composition of the present invention may further comprise one or more co-promoters and/or additional metal-containing dopants.
  • the catalyst composition of the present invention comprises a carrier in addition to the ternary oxide compound
  • the catalyst composition may, in principle, be prepared by any suitable technique known in the art for supported catalyst compositions.
  • Such "supported" catalyst compositions may be prepared by methods such as adsorption, impregnation, precipitation, co-precipitation, granulation, spray drying, or dry mixing.
  • calcination may take place at a temperature in the range of from 700 to 1000 °C .
  • the process of the present invention comprises utilising the catalyst composition as hereinbefore described in a reactor suitable for the oxidative coupling of methane.
  • the reactor may be any suitable reactor, such as a fixed bed reactor with axial or radial flow and with inter-stage cooling or a fluidized bed reactor equipped with internal and external heat exchangers.
  • the catalyst composition may be packed along with an inert packing material, such as quartz, into a fixed bed reactor having an appropriate inner diameter and length.
  • an inert packing material such as quartz
  • the catalyst composition may be
  • impurities at a temperature in the range of from 100 to 300 °C for about one hour in the presence of an inert gas such as nitrogen, helium or argon.
  • Suitable processes include those described in EP 0206042 Al, US 4443649 A, CA 2016675 A, US 6596912 Bl, US 2013/0023709 Al, WO 2008/134484 A2 and WO 2013/106771 A2.
  • a reactor feed comprising methane and oxygen is introduced into the reactor.
  • the reactor feed may further comprise one or more of a diluent gas, together with minor components of the methane feed (ethane, propane etc.) or the methane recycle stream (e.g. ethane, ethylene, propane, propylene, CO, C0 2 , H 2 , H 2 0) .
  • the diluent represents the balance of the feed gas and is an inert gas. Examples of suitable inert gases are nitrogen, argon or helium.
  • the reactor feed is often comprised of a combination of one or more gaseous stream(s), such as a methane stream, an oxygen stream, a recycle gas stream, a diluent stream, etc.
  • the methane and oxygen added to the reactor as mixed feed, optionally comprising further components therein, at the same reactor inlet.
  • the methane and oxygen may be added in separate feeds, optionally comprising further components therein, to the reactor at separate inlets.
  • Methane may be present in the reactor feed in a concentration of at least 35 mole-%, and most preferably at least 40 mole-%, relative to the total reactor feed. Similarly, methane may be present in the reactor feed in a concentration of at most 90 mole-%, and most preferably at most 85 mole-%, relative to the total reactor feed.
  • methane may be present in the reactor feed in a
  • concentration in the range of from 35 to 90 mole-%, and most preferably in the range of from 40 to 85 mole-%, relative to the total reactor feed.
  • the reactor feed further comprises oxygen, which may be provided either as pure oxygen or air.
  • oxygen which may be provided either as pure oxygen or air.
  • high-purity at least 95 mole-%) oxygen or very high purity (at least
  • the oxygen concentration in the reactor feed should be less than the concentration of oxygen that would form a flammable mixture at either the reactor inlet or the reactor outlet under the prevailing
  • the oxygen concentration in the reactor feed may be no greater than a pre-defined percentage (e.g., 95%, 90%, etc.) of oxygen that would form a flammable mixture at either the reactor inlet or the reactor outlet at the prevailing operating conditions .
  • the oxygen concentration in the reactor feed may vary over a wide range, the oxygen concentration in the reactor feed is typically at least 7 mole-%, or at least 10 mole-%, relative to the total reactor feed.
  • the oxygen concentration of the reactor feed is typically at most 25 mole-%, or at most 20 mole-%, relative to the total reactor feed.
  • oxygen may be present in the reactor feed in a concentration in the range of from 7 to 25 mole-%, and preferably in the range of from 10 to 20 mole-%, relative to the total reactor feed.
  • methane : oxygen volume ratio in the process of the present invention is in the range of from 2/1 to 10/1, and more preferably in the range of from 3/1 to 6/1.
  • the reactor feed optionally may further comprise a diluent gas, such as helium, argon, nitrogen or a combination thereof.
  • a diluent gas such as helium, argon, nitrogen or a combination thereof.
  • the order and manner in which the components of the reactor feed are combined prior to contacting the catalyst composition is not limited, and they may be combined simultaneously or sequentially. However, as will be recognized by one skilled in the art, it may be desirable to combine certain components of the inlet feed gas in a specified order for safety reasons. For example, oxygen may be added to the inlet feed gas after the addition of a dilution gas for safety reasons. Similarly, as will be understood by one of skill in the art, the concentration of various feed components present in the inlet feed gas may be adjusted throughout the process, for example, to maintain a desired productivity, optimize the process, etc. Accordingly, the above-defined
  • concentration ranges were selected to cover the widest possible variations in the composition of the reactor feed during normal operation.
  • Figure 1 is a schematic representation showing a typical reactor and product separation set-up for the oxidative coupling of methane.
  • Feed gas comprising methane and oxygen (or air) is introduced into the OCM reactor 101, via lines 107 and 108, respectively.
  • the methane may consist of fresh feed and recycled methane (derived from the separation stage of the process) .
  • the product mixture exiting the OCM reactor is passed to condensation vessel 102, where the majority of the water by-product of OCM is removed.
  • the product from 102 is then sent to the separation section 103, wherein the desired C2+ hydrocarbons are separated (stream 104 ) , either as a mixed hydrocarbon stream or as separated streams of ethylene, ethane, propylene and other hydrocarbons .
  • Unreacted methane separated from the OCM product mixture in 103 may optionally be recycled, as stream 106, which is combined with fresh feed stream 107, before entering the reactor.
  • Undesired products of OCM such as CO and C0 2 , as well as N 2 in the case of OCM with air feed, are also separated from the product mixture in 103 and leave the process as stream 105.
  • the separation section may also include a section for conversion of alkanes to olefins (e.g. ethane cracker) .
  • the reactor feed comprising methane and oxygen may be conveniently contacted with a catalyst composition as hereinbefore described in order to effect the conversion of methane to one or more C2+ hydrocarbons at a reactor temperature in the range of from 500 to 1000 °C.
  • said conversion is effected at a reactor temperature in the range of from 650 to 900 °C.
  • the conversion is effected at a reactor temperature of less than 850 °C. More preferably, the reactor temperature is preferably in the range of from
  • 650 to 850 °C even more preferably in the range of from 650 to 800 °C and most preferably in the range of from 700 to 775 °C.
  • the conversion of methane to one or more C2+ hydrocarbons is effected at a reactor pressure in the range of from 1 to 25 MPa. More preferably, said reactor pressure is in the range of from 2 to 10 MPa.
  • the gas hourly space velocity (GHSV) in the process of the present invention is the entering volumetric flow rate of the reactor feed divided by the catalyst bed volume at standard conditions.
  • said gas hourly space velocity is in the range of from 10000 to 300000 h _1 , and most preferably in the range of from 20000 to 70000 hT 1 .
  • the process of the present invention has a C2+ hydrocarbon selectivity of greater than 40 %, and more preferably greater than 60 %. In a preferred embodiment, the process of the present invention results in an ethane : ethene weight ratio of less than 1.6, and more preferably less than 0.6.
  • the afore-mentioned C2+ hydrocarbon selectivity, C2 hydrocarbon selectivity and ethane : ethene ratio values are determined at a reactor temperature of less than 850 °C, more preferably at a reactor
  • Li 2 Mn0 3 catalyst composition according to the present invention was prepared by conventional solid state reaction. 3.947 g of Mn 2 0 3 was mixed with 4.197 g of LiOH.H 2 0 in a mortar and pestle. The mixture was ground for 30 minutes. Acetone was added during the grinding to form a slurry. The final intimate mixture was transferred to an alumina boat or crucible.
  • Figure 5 displays an X-ray diffraction (XRD) pattern of the catalyst composition, showing a monoclinic single phase of Li 2 Mn0 3 .
  • the reference catalyst used for comparison purposes in the testing was 2% Mn/2% Na 2 W0 4 /Si0 2 which is the best performing catalyst for oxidative coupling of methane (OCM) based on open literature publications .
  • Catalysts were tested in accordance with the following general testing procedure.
  • the active test was carried out in a quartz fixed- bed microreactor with an isothermal zone of 4 cm and internal diameter of 2 mm.
  • the reagents of CH 4 (>99.9 %) and 0 2 (99.9 %) were used without further purification.
  • the reactor feed comprised methane and oxygen in a mole ratio of 4:1, with 5 mol . % nitrogen as inert gas.
  • the catalyst composition was evaluated at 700 °C, 725 °C, 750 °C and 800 °C, and 3.5 barg (350 kPa) pressure with a flow of 4.8 Nl/h.
  • reaction products were then analysed with an on ⁇ line GC device equipped with a 2 TCD and 2 FID using different columns for the separation of CH 4 , C0 2 , C 2 H X , C 3 H X , C 4 H X , CsH x , O 2 , 2 , CO.
  • Tables 1-4 and Figures 2-4 summarize the results of the testing.
  • the Li 2 Mn0 3 catalyst of the present invention displays advantageous activity for oxidative coupling of methane (OCM) at a lower
  • the Li 2 Mn0 3 catalyst of the present invention displays very similar performance compared to reference catalyst - showing 26.3% methane conversion and 60.4% selectivity for C2+ under these test conditions.
  • the Li 2 Mn0 3 catalyst of the present invention shows remarkably higher space time yield (STY) compared to the reference catalyst.

Abstract

L'invention concerne une composition de catalyseur comprenant un composé d'oxyde ternaire, ledit composé d'oxyde ternaire comprenant un ou plusieurs métaux alcalins et du manganèse et ayant été préparé par réaction d'un ou plusieurs composés de métal alcalin choisis parmi l'hydroxyde de métal alcalin, le carbonate de métal alcalin et l'oxyde de métal alcalin avec un ou plusieurs composés de manganèse choisis parmi des oxydes de manganèse, l'hydroxyde de manganèse, l'acétate de manganèse et le nitrate de manganèse ; et un procédé pour le couplage oxydatif de méthane à l'aide de ladite composition de catalyseur.
PCT/EP2016/066386 2015-07-13 2016-07-11 Catalyseur et procédé permettant le couplage oxydatif de méthane WO2017009273A1 (fr)

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Cited By (1)

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