Catalysts for oxidative coupling of methane and solution combustion method for the production of the same

Patent metadata

Field	Value
Publication number	US-9610565-B2
Application number	US-201313971357-A
Country	US
Kind code	B2
Filing date	Aug 20, 2013
Priority date	Aug 20, 2012
Publication date	Apr 4, 2017
Grant date	Apr 4, 2017

Abstract

A method for making a metal oxide material and catalyzing the oxidative coupling of methane, including mixing a metal cation-containing oxidizer portion and a reducing fuel portion with water to define an aqueous solution, evaporatively removing water from the aqueous solution to yield a concentrated liquid, burning the concentrated liquid yield an homogeneous metal oxide powder, flowing methane from a first source and oxygen from a second source over the homogeneous metal oxide powder, and catalyzing an oxidative coupling of methane reaction with the homogeneous metal oxide powder. The homogeneous metal oxide powder contains metal oxides selected from the group including LaSrAlO 4 , LaAlO 3 , Sr 3 Al 2 O 6 , Na 2 WO 4 —Mn/SiO 2 , and combinations thereof.

First claim

We claim:

1. A method for producing metal oxide catalysts for oxidative coupling of methane reactions, comprising:
measuring predetermined stoichiometric amounts of metal cation contributors to define a predetermined metal cation precursor;
measuring a predetermined amount of reducing fuel;
mixing the predetermined amount of fuel, the predetermined metal cation precursor and water to define an aqueous solution;
evaporating water from the aqueous solution to define a concentrated solution;
igniting the concentrated solution;
combustively reacting the metal cation precursor with the fuel to yield a metal oxide;
flowing methane from a first source over the metal oxide;
flowing oxygen from a second source over the metal oxide;
mixing methane from the first source with oxygen from the second source in the presence of the metal oxide; and
catalyzing an oxidative coupling of methane reaction with the metal oxide;
wherein the methane from the first source and the oxygen from the second source are kept separate until they are introduced and mixed together in the presence of the metal oxide;
wherein the metal cation precursor is selected from the group consisting of strontium nitrate, aluminum nitrate nonahydrate, sodium tungsten oxide dihydrate, manganese nitrate tetrahydrate, tetraethoxysilane, and combinations thereof, and wherein the reducing fuel is selected from the group consisting of glycine, hydrazine, oxalates, and combinations thereof.

2. A method for making a metal oxide material, comprising:
mixing a metal cation-containing oxidizer portion and a reducing fuel portion with water to define an aqueous solution;
evaporatively removing water from the aqueous solution to yield a concentrated liquid;
burning the concentrated liquid to yield an homogeneous metal oxide powder;
mixing unblended methane and oxygen in the presence of the homogeneous metal oxide powder; and
catalyzing an oxidative coupling of methane reaction with the homogeneous metal oxide powder;
wherein the homogeneous metal oxide powder contains at least one metal oxide selected from the group consisting of LaSrAlO 4 , LaAlO 3 , Sr 3 Al 2 O 6 , Na 2 WO 4 —Mn/SiO 2 , and combinations thereof.

3. The method of claim 2 wherein metal cation containing portion is selected from the group consisting of lanthanum nitrate hexahydrate, strontium nitrate, aluminum nitrate nonahydrate, sodium tungsten oxide dihydrate, manganese nitrate tetrahydrate, tetraethoxysilane, and combinations thereof, and wherein the fuel portion is selected from the group including glycine, hydrazine, oxalates, and combinations thereof.

4. The method of claim 2 wherein the reducing fuel portion to metal-cation containing oxidizer portion ratio is between 0.5 and 2.0.

5. The method of claim 1 , and further comprising:
dissolving solids into the aqueous solution;
evaporating the concentrated solution to yield a paste; and
self-igniting the paste.

6. A method for producing metal oxide catalysts for oxidative coupling of methane reactions, comprising:
measuring predetermined stoichiometric amounts of metal cation contributors to define a predetermined metal cation precursor;
measuring a predetermined amount of reducing fuel;
mixing the predetermined amount of fuel, the predetermined metal cation precursor and water to define an aqueous solution;
evaporating water from the aqueous solution to define a concentrated solution;
igniting the concentrated solution;
combustively reacting the metal cation precursor with the fuel to yield a metal oxide;
flowing methane from a first source over the metal oxide at a first flow rate;
flowing oxygen from a second source over the metal oxide at a second flow rate;
introducing and mixing methane from the first source with oxygen from the second source in the presence of the metal oxide; and
catalyzing an oxidative coupling of methane reaction with the metal oxide;
wherein the methane from the first source and the oxygen from the second source are kept separate until they are introduced to one another in the presence of the metal oxide;
wherein the metal cation precursor is selected from the group consisting of strontium nitrate, aluminum nitrate nonahydrate, sodium tungsten oxide dihydrate, manganese nitrate tetrahydrate, tetraethoxysilane, and combinations thereof, and wherein the reducing fuel is selected from the group consisting of glycine, hydrazine, oxalates, and combinations thereof;
wherein the first and second flow rates may be varied independently of one another.

Assignees

• Purdue Research Foundation

Inventors

• Ghose Ranjita
• Hwang Hyun Tae
• Varma Arvind

Classifications

• C01F17/34

  Aluminates, e.g. YAlO3 or Y3-xGdxAl5O12 · CPC title

• B01J23/34 Primary

  Manganese · CPC title

• B01J2523/00

  Constitutive chemical elements of heterogeneous catalysts · CPC title

• B01J23/005

  Spinels · CPC title

• C01G41/02

  Oxides; Hydroxides · CPC title