# US 9,518,236 B2 · Synthetic fuels and chemicals production with in-situ CO2 capture

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- Number: US 9,518,236 B2
- Document ID: US9518236B2
- Status: Granted
- Kind: B2
- Application number: 13/394,396
- Filed: 2010-09-08
- Published: 2012-06-28
- Granted: 2016-12-13
- Earliest claimed: 2009-09-08
- Assignees: The Ohio State University Research Foundation
- Applicants: Liang-Shih Fan; Fanxing Li; Liang Zeng
- Inventors: Liang-Shih Fan; Fanxing Li; Liang Zeng
- Web page: https://patentgrep.com/patent/US9518236B2

## CPC

- C10G 1/02: by distillation
- C01B 3/344: {using non-catalytic solid particles}
- C10G 2/50: {from carbon dioxide with hydrogen}
- C10J 3/725: {Redox processes}
- C01B 2203/062: Hydrocarbon production, e.g. Fischer-Tropsch process
- C01B 2203/148: involving a recycle stream to the feed of the process for making hydrogen or synthesis gas
- C01B 2203/86: Carbon dioxide sequestration
- C10G 2300/1011: Biomass
- C10G 2300/807: Steam
- C10J 3/466: {Entrained flow processes}
- C10J 3/86: combined with waste-heat boilers
- C10J 2300/0916: Biomass
- C10J 2300/093: Coal
- C10J 2300/0959: Oxygen
- C10J 2300/1612: CO2-separation and sequestration, i.e. long time storage
- C10J 2300/1659: to liquid hydrocarbons
- C10J 2300/1678: with air separation
- C10J 2300/1807: Recycle loops, e.g. gas, solids, heating medium, water
- C10K 1/003: {of acid contaminants, e.g. acid gas removal}
- C10K 1/024: {by filtration}
- Y02P 20/145: the feedstock being materials of biological origin
- Y02P 30/00: Technologies relating to oil refining and petrochemical industry
- Y02P 30/20: using bio-feedstock
- C10G: CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION (cracking to hydrogen or synthesis gas C01B; cracking or pyrolysis of hydrocarbon gases to individual hydrocarbons or mixtures thereof of definite or specified constitution C07C; cracking to cokes C10B); RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- C10J: PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES (synthesis gas from liquid or gaseous hydrocarbons C01B; underground gasification of minerals E21B43/295); CARBURETTING AIR OR OTHER GASES
- C10K: PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

Novel redox based systems for fuel and chemical production with in-situ CO2 capture are provided. A redox system using one or more chemical intermediates is utilized in conjunction with liquid fuel generation via indirect Fischer-Tropsch synthesis, direct hydrogenation, or pyrolysis. The redox system is used to generate a hydrogen rich stream and/or CO2 and/or heat for liquid fuel and chemical production. A portion of the byproduct fuels and/or steam from liquid fuel and chemical synthesis is used as part of the feedstock for the redox system.

## Claims

### Claim 1

A method for producing synthetic liquid fuel from a carbonaceous fuel comprising:
indirectly gasifying the carbonaceous fuel using steam and optionally, an oxygen containing gas, and forming separate streams of carbon dioxide and hydrogen rich gases, wherein metal oxide particles containing Fe2O3 are used in an indirect gasification reaction, and the carbonaceous fuel is indirectly gasified by:
reducing the Fe2O3 containing particles with the carbonaceous fuel in a first reaction zone comprising a packed moving bed with a countercurrent gas-solids contacting pattern such that an average valence of iron is less than 1, wherein the first reaction zone is operated at a temperature of greater than or equal to 400° C. and less than or equal to 1200° C. and at a pressure of greater than or equal to 1.01×105 Pa and less than or equal to 8.10×106 Pa;
at least partially oxidizing a portion of the reduced iron oxide containing particles from the first reaction zone with steam to generate a hydrogen rich gas in a second reaction zone comprising countercurrent gas-solids contacting pattern such that the iron oxide containing particle is at least partially oxidized to contain Fe3O4;
directly sending a portion of the reduced iron oxide particles from the first reaction zone to a third reaction zone;
oxidizing the reduced iron oxide particles from the first reaction zone and the iron oxide containing particles from the second reaction zone with an oxygen containing gas in the third reaction zone, and returning the oxidized iron oxide containing particles to the first reaction zone; and
reacting the hydrogen rich gas and a portion of the carbon dioxide in a CO2 hydrogenation reaction to form a synthetic fuel, wherein remaining CO2 is sequestered.

### Claim 2 (depends on 1)

A method as claimed in claim 1 in which at least a portion of the steam is produced using heat generated from the CO2 hydrogenation reaction.

### Claim 3 (depends on 1)

A method as claimed in claim 1 in which the carbonaceous fuel comprises syngas, carbon monoxide, methane rich gas, light hydrocarbons, liquid carbonaceous fuels, coal, biomass, tar sand, oil shale, petroleum coke, heavy liquid hydrocarbons, wax, or a mixture thereof.

### Claim 4 (depends on 1)

A method as claimed in claim 1 in which at least a portion of the synthetic liquid fuel is used as a feed for the carbonaceous fuel.

### Claim 5 (depends on 1)

A method as claimed in claim 1 in which the metal oxide particles contain supporting material comprising a ceramic material selected from the group consisting of oxides of Al, Ti, Zr, Y, Si, La, Cr, Mg, Mn, Cu, Ca, carbides of Si and Ti, sepiolite, bentonite, and kaolin.

### Claim 6 (depends on 1)

A method as claimed in claim 1 in which gaseous species selected from CO2, H2O, or gaseous fuels from CO2 hydrogenation, are introduced to the bottom of the first reaction zone to enhance conversions of both the iron oxide particles and the carbonaceous fuel.

### Claim 7 (depends on 1)

A method as claimed in claim 1 in which the carbonaceous fuel comprises solid carbonaceous fuel particles which are suspended by the gases in a lower section of the first reaction zone until they are at least 50% converted before being elutriated towards the top of the first reaction zone.

### Claim 8 (depends on 1)

A method as claimed in claim 1 in which a calcium oxide containing CO2 sorbent is used to assist in the indirect gasification of the carbonaceous fuels.