# US 9,873,101 B2 · Catalytic microchannel reformer

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- Number: US 9,873,101 B2
- Document ID: US9873101B2
- Status: Granted
- Kind: B2
- Application number: 14/606,847
- Filed: 2015-01-27
- Published: 2015-06-25
- Granted: 2018-01-23
- Earliest claimed: 2006-12-21
- Assignees: Ceramatec, Inc.
- Applicants: Ceramatec, Inc.
- Inventors: Joseph J. Hartvigsen; Balakrishnan Nair; Merrill Wilson; Akash Akash
- Web page: https://patentgrep.com/patent/US9873101B2

## CPC

- B01J 19/0093: {Microreactors, e.g. miniaturised or microfabricated reactors (laboratory containers with capillary fluid transport in microfabricated channels or chambers B01L3/5027)}
- B01D 67/0044: {by chemical reaction}
- B01D 71/024: {Oxides}
- C01B 3/323: Catalytic reaction of gaseous or liquid organic compounds other than hydrocarbons with gasifying agents
- C01B 3/384: with external heating of the catalyst
- C01B 3/40: characterised by the catalyst
- C01B 3/48: followed by reaction of water vapour with carbon monoxide
- C01B 3/503: characterised by membranes
- B01D 2325/22: Thermal or heat-resistance properties
- B01D 2325/30: Chemical resistance
- B01J 2219/00783: Laminate assemblies, i.e. the reactor comprising a stack of plates
- B01J 2219/00824: Ceramic
- B01J 2219/00835: Comprising catalytically active material
- B01J 2219/00873: Heat exchange
- B01J 2219/00907: using membranes
- C01B 2203/0233: the reforming step being a steam reforming step
- C01B 2203/0283: containing a CO-shift step, i.e. a water gas shift step
- C01B 2203/041: In-situ membrane purification during hydrogen production
- C01B 2203/047: the impurity being carbon monoxide
- C01B 2203/0475: the impurity being carbon dioxide
- C01B 2203/048: the impurity being an organic compound
- C01B 2203/0495: the impurity being water
- C01B 2203/0811: by combustion of fuel
- C01B 2203/0822: the fuel containing hydrogen
- C01B 2203/0827: at least part of the fuel being a recycle stream
- C01B 2203/1023: Catalysts in the form of a monolith or honeycomb
- C01B 2203/1058: Nickel catalysts
- C01B 2203/1223: Methanol
- C01B 2203/1241: Natural gas or methane
- C01B 2203/1247: Higher hydrocarbons
- C01B 2203/141: At least two reforming, decomposition or partial oxidation steps in parallel
- C01B 2203/145: At least two purification steps in parallel
- C01B 2203/82: Several process steps of C01B2203/02 - C01B2203/08 integrated into a single apparatus
- Y02E 60/32: Hydrogen storage
- Y02P 20/10: Process efficiency
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01D: SEPARATION (separating solids from solids by wet methods B03B, B03D; by pneumatic jigs or tables B03B; by other dry methods B07; magnetic or electrostatic separation of solid materials from solid materials or fluids, separation by high-voltage electric fields B03C; centrifuges, vortex apparatus B04; presses per se for squeezing-out liquid from liquid-containing material B30B9/02; treatment of water C02F, e.g. softening by ion-exchange C02F1/42; {arrangements of air intake cleaners in gas turbine plants F02C7/05} ; arrangements or mounting of filters in air-conditioning, air-humidification or ventilation F24F13/28)
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

An apparatus and method for enhancing the yield and purity of hydrogen when reforming hydrocarbons is disclosed in one embodiment of the invention as including receiving a hydrocarbon feedstock fuel (e.g., methane, vaporized methanol, natural gas, vaporized diesel, etc.) and steam at a reaction zone and reacting the hydrocarbon feedstock fuel and steam in the presence of a catalyst to produce hydrogen gas. The hydrogen gas is selectively removed from the reaction zone while the reaction is occurring by selectively diffusing the hydrogen gas through a porous ceramic membrane. The selective removal of hydrogen changes the equilibrium of the reaction and increases the amount of hydrogen that is extracted from the hydrocarbon feedstock fuel.

## Claims

### Claim 1

An apparatus comprising:
material comprising alumina powder reacted with a phosphate-containing reagent, said material forming at least one ceramic microchannel within the apparatus;
a reaction zone, positioned within the apparatus and at least partially within at least one microchannel, the reaction zone configured to receive reactants comprising a hydrocarbon fuel and steam, the reactants reacting to produce reaction products comprising hydrogen gas;
a combustion zone, positioned within the apparatus, in fluid communication with the reaction zone, the combustion zone configured to receive at least one of a reactant and a reaction product;
a product zone; and
a porous membrane positioned between the reaction zone and the product zone, the porous membrane comprising pores of varying size, the porous membrane configured to allow hydrogen gas to diffuse through said pores of the porous membrane at a higher diffusion rate than diffusion rates of reactants within the reaction zone and any other reaction products.

### Claim 2 (depends on 1)

The apparatus of claim 1, comprising confined spaces having lateral dimensions of less than 1 mm.

### Claim 3 (depends on 1)

The apparatus of claim 1, wherein the at least one ceramic microchannel comprises a very high surface area and a continuous nanopore network.

### Claim 4 (depends on 1)

The apparatus of claim 1, wherein, the at least one ceramic microchannel comprises phosphate-bonded ceramic materials.

### Claim 5 (depends on 1)

The apparatus of claim 1, wherein the at least one ceramic microchannel comprises at least one of micro-sized pores and nano-sized pores.

### Claim 6 (depends on 5)

The apparatus of claim 5, wherein the at least one of micro-sized pores and nano-sized pores are located adjacent to a reaction zone.

### Claim 7

An apparatus comprising:
at least one microchannel formed within the apparatus in material comprising alumina powder reacted with a phosphate-containing reagent, said material comprising confined spaces having lateral dimensions of less than 1 mm;
a reaction zone, positioned within the apparatus and at least partially within at least one microchannel, the reaction zone configured to receive reactants comprising hydrocarbon and steam to produce reaction products comprising hydrogen gas;
a combustion zone, positioned within the apparatus, in fluid communication with the reaction zone, the combustion zone configured to receive at least one of a reactant and a reaction product;
a product zone; and
a porous membrane positioned between the reaction zone and the product zone, the porous membrane comprising pores of varying size, the porous membrane configured to allow hydrogen gas to diffuse through said pores of the porous membrane at a higher diffusion rate than diffusion rates of reactants within the reaction zone and any other reaction products, and wherein a first surface of the porous membrane is exposed to the reaction zone and a second surface of the porous membrane opposite the first surface is exposed to the product zone; and wherein at least one of micro-sized pores and nano-sized pores are located adjacent to the reaction zone.