Catalysts, methods of making catalysts, and methods of combustion
AssigneeVelocys, Inc.
InventorsBarry Lee-Mean Yang, Ruiqiang Long, Junko M. Watson, Abhishek Gupta
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Abstract
Catalysts are described in which an active catalyst is disposed on a low surface area, oxide support. Methods of forming catalysts are described in which a Cr-containing metal is oxidized to form a chromium oxide layer and an active catalyst is applied directly on the chromium oxide layer. Methods of making new catalysts are described in which the surface is sonicated prior to depositing the catalyst. Catalyst systems and methods of oxidation are also described. The inventive systems, catalysts and methods are, in some instances, characterized by surprisingly superior results.
Claims38
A method of combusting a carbon-containing compound, comprising:
- providing a gas mixture comprising CO or a hydrocarbon and an oxidant;
- and
- passing the gas mixture through a reaction chamber at a GHSV of at least 100,000 −1 and a temperature of 400 to 1100° C.;
- wherein the reaction chamber has an internal dimension of 1 cm or less;
- wherein a combustion catalyst is disposed in the reaction chamber;
- and
- wherein at least 20% of the CO or the hydrocarbon in the gas mixture is converted to CO2.
A method of oxidizing a carbon-containing compound, comprising:
- providing a gas mixture comprising CO or a hydrocarbon and an oxidant;
- and
- passing the gases through a reaction chamber at a GHSV of at least 10,000 h−1 and a temperature of 400 to 1100° C.;
- wherein the reaction chamber has an internal dimension of 1 cm or less;
- wherein a combustion catalyst is disposed in the reaction chamber;
- wherein pressure drop through the reaction chamber is 20 psi or less, or wherein the pressure drop through the reaction chamber is 3.0 psi per inch or less;
- and
- wherein at least 20% of the hydrocarbon in the gas mixture is converted to CO2.
A catalyst system, comprising:
- a metal substrate comprising chromium and cobalt;
- a chromium-containing oxide layer in direct contact with the metal substrate;
- wherein the chromium-containing oxide layer has a surface that is not adjacent to the metal substrate and wherein this surface has a Co:Cr ratio that is at least 50% less than the metal substrate;
- an active catalyst material on the chromium-containing oxide layer;
- wherein the combination of the metal substrate, the active catalyst material and the chromium-containing oxide layer define a catalyst, and wherein the catalyst has a low surface area of no more than 0.5 m2/g or no more than 1 m2/inch2 of geometric surface area.
The catalyst system of claim 16 wherein the reaction chamber is defined by a wall or walls that comprise the metal substrate.
A catalyst system, comprising:
- a reaction chamber and a catalyst, wherein the catalyst comprises:
- a metal substrate;
- an oxide layer disposed on the metal substrate;
- and
- a combustion catalyst on the oxide layer;
- wherein the reaction chamber has an internal dimension of 1 cm or less;
- wherein the combustion catalyst is disposed within the reaction chamber;
- and
- wherein the system is characterizable by a combustion activity selected from the group consisting of:
- when a gas mixture containing 9 volume % CH4, 1.9 vol. % O2, and 89 vol. % N2 is passed through the reaction chamber at a GHSV of 1.6×106 h−1 and a temperature in the reaction chamber of 835° C., there is a CH4 conversion of at least 9% and an O2 conversion of at least 50%;
- when a gas mixture containing 1.0 volume % CH4, 4.4 vol. % O2, 1.2 vol. % H2, 2.0 vol. % CO, and 91.4 vol. % N2 is passed through the reaction chamber at a GHSV of 1.1×106 h−1 and a temperature in the reaction chamber of 710° C., there is a CO conversion of at least 80%;
- and
- when a gas mixture containing 1.0 volume % CH4, 4.4 vol. % O2, 1.2 vol. % H2, 2.0 vol. % CO, and 91.4 vol. % N2 is passed through the reaction chamber at a GHSV of 1.1×106 h−1 and a temperature in the reaction chamber of 910° C., there is a CO conversion of at least 90%.
A method of making a catalyst, comprising:
- oxidizing a new metal substrate to form a metal with a layer of low surface area surface oxide;
- wherein the new metal substrate has not previously been part of a catalyst structure;
- sonicating the metal substrate with the low surface area surface oxide;
- and
- depositing an active catalyst material on the sonicated metal substrate with the low surface area oxide layer.
A method of making a catalyst, comprising:
- step (a) oxidizing a nickel-based, chromium-containing metal by heating the metal to a temperature of at least 850° C. in the absence of oxygen and then exposing the metal to an oxygen-containing atmosphere at a temperature of at least 850° C. to form a nickel-based, chromium-containing metal with a chromium-containing metal oxide surface layer;
- and step (b) depositing an active catalyst material directly on the chromium-containing metal oxide surface layer of step (a).
A method of combusting a fuel to heat an adjacent stream, comprising:
- providing a gas mixture comprising CO or a hydrocarbon and an oxidant;
- and
- passing the gas mixture into at least one reaction chamber at a GHSV of at least 10,000 h−1 and a temperature of 400 to 1100° C.;
- wherein the at least one reaction chamber has an internal dimension of 1 cm or less;
- wherein a combustion catalyst is disposed in the at least one reaction chamber and is adjacent to at least one reaction chamber wall and further wherein a bulk flow path is present though the at least one reaction chamber;
- wherein the at least one reaction chamber has an internal surface area that is defined by the area of the at least one reaction chamber wall that is coextensive with the combustion catalyst;
- wherein at least one coolant chamber is adjacent to said at least one reaction chamber wall;
- wherein the at least one reaction chamber and the at least one coolant chamber define an integrated combustion reactor;
- and
- combusting the CO or a hydrocarbon with the oxidant to produce heat sufficient to create a heat flux, at steady-state, of at least 10 W per cm2 of the integrated combustion reactor.
A catalyst system, comprising:
- at least one reaction chamber comprising at least one reaction chamber wall:
- wherein the at least one reaction chamber has an internal dimension of 1 cm or less;
- wherein a combustion catalyst is disposed in the at least one reaction chamber and is adjacent to the at least one reaction chamber wall and further wherein a bulk flow path is present though the at least one reaction chamber;
- wherein the at least one reaction chamber has an internal surface area that is defined by the area of the at least one reaction chamber wall that is coextensive with the combustion catalyst;
- wherein at least one coolant chamber is adjacent to said at least one reaction chamber wall;
- wherein the at least one reaction chamber and the at least one coolant chamber define an integrated combustion reactor;
- and
- wherein the system is characterizable by a combustion activity such that, when a gas mixture comprising 8.7% methane and 91.3% air is passed into the at least one reaction chamber at a gas feed rate/ICR volume of 2000 h−1 and an endothermic gas stream passed through the coolant stream at a rate such that thermal equilibrium is obtained;
- sufficient heat is produced to create a heat flux, at steady-state, of at least 1 W per cc of the integrated combustion reactor.
A catalyst system, comprising:
- a nickel-based, chromium-containing, metal substrate;
- a chromium-containing oxide layer in direct contact with the metal substrate;
- an active catalyst material on the chromium-containing oxide layer;
- wherein prior to depositing the active catalyst material thereon, the surface of the oxide layer comprises at least 90 weight % chromia and has a Ni:Cr ratio of less than 0.005 as measured by XPS;
- wherein the combination of the metal substrate, the active catalyst material and the chromium-containing oxide layer define a catalyst, and wherein the catalyst has a low surface area of no more than 0.5 m2/g or no more than 1 m2/inch2 of geometric surface area.
A catalyst system, comprising:
- a reaction chamber comprising an outlet;
- a process stream in the reaction chamber;
- a gas stream passing through the outlet comprising CO2 wherein the atomic ratio of C in the CO2 to C in all molecules in the gas stream is at least 0.2;
- a metal substrate;
- a chromium- or aluminum-containing oxide layer in direct contact with the metal substrate;
- and
- an active catalyst material on the chromium- or aluminum-containing oxide layer;
- wherein the combination of the metal substrate, the active catalyst material and the chromium- or aluminum-containing oxide layer define a catalyst, and wherein the catalyst has a low surface area of no more than 0.5 m2/g or no more than 1 m2/inch2 of geometric surface area.
Dependencies are inferred from the claim text.