# US 8,784,687 B2 · Methane steam reforming using fibrous composite catalytic structures having at least three solid phases

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- Number: US 8,784,687 B2
- Document ID: US8784687B2
- Status: Granted
- Kind: B2
- Application number: 13/680,510
- Filed: 2012-11-19
- Published: 2013-04-18
- Granted: 2014-07-22
- Earliest claimed: 2007-08-17
- Applicants: Juzer Jangbarwala
- Inventors: Juzer Jangbarwala
- Web page: https://patentgrep.com/patent/US8784687B2

## CPC

- C01B 3/40: characterised by the catalyst
- B01J 21/18: Carbon
- B01J 21/185: {Carbon nanotubes (carbon nanotubes per se C01B32/15)}
- B01J 23/24: Chromium, molybdenum or tungsten
- B01J 23/38: of noble metals
- B01J 23/74: Iron group metals
- B01J 23/80: with zinc, cadmium or mercury
- B01J 27/1856: {with platinum group metals}
- B01J 35/19: {Catalysts containing parts with different compositions}
- B01J 35/33: Electric or magnetic properties
- B01J 35/40: characterised by dimensions, e.g. grain size (in a colloidal state B01J35/23; crystallite size B01J35/77)
- B01J 35/58: Fabrics or filaments
- B01J 35/59: Membranes
- B01J 35/613: {10-100 m2/g}
- B01J 35/615: {100-500 m2/g}
- B01J 35/618: {more than 1000 m2/g}
- B01J 37/0201: {Impregnation}
- B82Y 30/00: Nanotechnology for materials or surface science, e.g. nanocomposites
- C01B 3/326: characterised by the catalysts
- H01M 8/0631: {Reactor construction specially adapted for combination reactor/fuel cell (hydrogen C01B3/00; reactors for physicochemical processes B01J19/00)}
- B01J 21/04: Alumina
- B01J 37/343: {of ultrasonic wave energy}
- 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 2203/0405: Purification by membrane separation
- C01B 2203/043: Regenerative adsorption process in two or more beds, one for adsorption, the other for regeneration
- C01B 2203/0445: Selective methanation
- C01B 2203/066: with fuel cells
- C01B 2203/1017: characterised by the form of the structure
- C01B 2203/1041: Composition of the catalyst
- C01B 2203/1058: Nickel catalysts
- C01B 2203/1064: Platinum group metal catalysts
- C01B 2203/1076: Copper or zinc-based catalysts
- C01B 2203/1223: Methanol
- C01B 2203/142: At least two reforming, decomposition or partial oxidation steps in series
- Y02E 60/50: Fuel cells
- Y02P 20/52: using catalysts, e.g. selective catalysts
- Y10S 977/734: Fullerenes, i.e. graphene-based structures, such as nanohorns, nanococoons, nanoscrolls or fullerene-like structures, e.g. WS2 or MoS2 chalcogenide nanotubes, planar C3N4, etc.
- Y10S 977/742: Carbon nanotubes, CNTs
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B82Y: SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
- Y10S: TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS

## Abstract

A methane steam reforming process for converting a syngas in the presence of permeable composite fibrous catalytic sheets comprised of at least three distinct solid phases. A first solid phase is a 3-dimensional porous network of a non-conductive porous ceramic material. A second solid phase is an electrically conductive phase comprised of randomly oriented electrically conductive fibers. A third phase is comprised of methane steam reforming catalytic particles dispersed on said 3-dimensional porous network, said conductive fibers, or both. A fourth phase can be present, which fourth phase is comprised one or more conductive species or one or more non-conductive species embedded in said first solid phase.

## Claims

### Claim 1

A process of performing methane steam reforming to produce a syngas comprised predominantly of hydrogen and carbon monoxide, which process comprising reacting methane by passing it through a permeable composite catalytic sheet-like structure in the form selected from sheet, board and block, comprised of at least three distinct solid phases wherein: i) a first solid phase is comprised of a 3-dimensional substantially continuous network of a non-conductive porous ceramic material; ii) a second solid phase is comprised of a plurality of electrically conductive fibers, having a bulk density that will provide substantially continuous electrical conductivity from one end of said sheet-like structure to an opposing end, and integrated throughout the 3-dimensional substantially continuous network of non-conductive porous ceramic material; iii) a third solid phase comprised of an effective amount of methane steam reforming catalyst particles dispersed throughout the non-conductive porous ceramic material, the plurality of electrically conductive fibers, or both, at methane reforming reaction conditions.

### Claim 2 (depends on 1)

The process of claim 1 wherein the methane steam reforming catalyst contains at least one active metal or metal oxide of Group 6 or Group 8 to 10 of the Periodic Table of the Elements.

### Claim 3 (depends on 2)

The process of claim 2 wherein the methane steam reforming conditions include temperatures from about 500° C. to about 1,200° C. and gas hourly space velocities of about 300 to about 9,000/h.

### Claim 4 (depends on 1)

The process of claim 1 wherein the methane steam reforming process conditions include temperatures from about 500° C. to about 1,200° C. and gas hourly space velocities of about 300 to about 9,000/h.

### Claim 5 (depends on 1)

The process of claim 1 wherein the methane steam reforming catalyst is comprised of about 3 wt % to about 40 wt % of at least one Group 6 or Group 8 to 10 metal, based on total weight of the catalyst.

### Claim 6 (depends on 1)

The process of claim 1 wherein there is a fourth solid phase comprised of a plurality of one or more conductive or non-conductive materials embedded within said first solid phase.

### Claim 7 (depends on 6)

The process of claim 6 wherein the fourth solid phase is comprised of one or more conductive materials selected from the group consisting of graphene, carbon, and graphitic nanostructures.

### Claim 8 (depends on 7)

The process of claim 7 wherein the graphitic nanostructures are selected from the group consisting of nanofibers, nanotubes, and nanoribbons.

### Claim 9 (depends on 6)

The process of claim 6 wherein the fourth solid phase is a non-conductive phase comprised of a non-conductive material selected from the group consisting of ceramic fibers, zirconia fibers, alumina fibers, aluminosilica fibers, aluminoboro silicate fibers, ceramic nanostructures, and silicon carbide fibers.

### Claim 10 (depends on 9)

The process of claim 9 wherein the non-conductive phase is comprised of ceramic fibers selected from the group consisting of ceramic nanostructures and silicon carbide fibers.

### Claim 11 (depends on 1)

The process of claim 1 wherein the conductive fibers are selected from the group consisting of carbon fibers and graphitic fibers.

### Claim 12 (depends on 11)

The process of claim 11 wherein the conductive fibers are graphitic fibers.

### Claim 13 (depends on 1)

The process of claim 1 wherein the conductive fibers are graphitic fibers.

### Claim 14 (depends on 1)

The process of claim 1 wherein the ceramic material of the first solid phase is selected from the group consisting of alumina, silica, silica-alumina, titania, zirconia, and magnesia.

### Claim 15 (depends on 14)

The process of claim 14 wherein the ceramic material is alumina.

### Claim 16 (depends on 1)

The process of claim 1 wherein conductive fibers are comprised of polymer fibers enhanced with a carbon material selected from the group consisting of graphene, graphite, and graphitic nanostructures.

### Claim 17 (depends on 16)

The process of claim 16 wherein the graphitic nanostructures are selected from the group consisting of nanofibers, nanotubes, and nanoribbons.