# US 8,771,388 B2 · Method to produce methane rich fuel gas from carbonaceous feedstocks using a steam hydrogasification reactor and a water gas shift reactor

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- Number: US 8,771,388 B2
- Document ID: US8771388B2
- Status: Granted
- Kind: B2
- Application number: 12/783,228
- Filed: 2010-05-19
- Published: 2011-06-02
- Granted: 2014-07-08
- Earliest claimed: 2002-02-05
- Assignees: The Regents of the University of California
- Applicants: Joseph M. Norbeck; Chan Seung Park; Arun S K Raju
- Inventors: Joseph M. Norbeck; Chan Seung Park; Arun S K Raju
- Web page: https://patentgrep.com/patent/US8771388B2

## CPC

- C01B 3/12: by reaction of water vapour with carbon monoxide
- C10G 1/06: by destructive hydrogenation
- C10G 2/30: {from carbon monoxide with hydrogen}
- C10J 3/00: Production of combustible gases containing carbon monoxide from solid carbonaceous fuels (destructive distillation processes C10B)
- C10K 1/004: {Sulfur containing contaminants, e.g. hydrogen sulfide}
- C10K 3/04: reducing the carbon monoxide content {, e.g. water-gas shift [WGS]}
- C10L 3/08: Production of synthetic natural gas
- C10L 3/102: {of acid contaminants}
- C01B 2203/0283: containing a CO-shift step, i.e. a water gas shift step
- C01B 2203/04: containing a purification step for the hydrogen or the synthesis gas
- 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 2203/06: Integration with other chemical processes
- C01B 2203/0805: Methods of heating the process for making hydrogen or synthesis gas
- C01B 2203/1241: Natural gas or methane
- C01B 2203/1258: Pre-treatment of the feed
- C01B 2203/127: Catalytic desulfurisation
- C01B 2203/148: involving a recycle stream to the feed of the process for making hydrogen or synthesis gas
- C01B 2203/84: Energy production
- C10J 2300/0916: Biomass
- C10J 2300/0946: Waste, e.g. MSW, tires, glass, tar sand, peat, paper, lignite, oil shale
- C10J 2300/0966: Hydrogen
- C10J 2300/0973: Water
- C10J 2300/1659: to liquid hydrocarbons
- C10J 2300/1662: to methane
- C10J 2300/1807: Recycle loops, e.g. gas, solids, heating medium, water
- Y02E 50/30: Fuel from waste, e.g. synthetic alcohol or diesel
- Y02P 20/145: the feedstock being materials of biological origin
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- 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
- 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
- C10L: FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
- 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

A method for producing high levels of methane based on a combination of steam hydrogasification and a shift reactor is provided. Hydrogen produced by the shift reactor can be recycled back into the steam hydrogasifier.

## Claims

### Claim 1

A process for converting carbonaceous material into methane-rich fuel gas, comprising:
simultaneously heating in a steam hydrogasification reactor the carbonaceous material in the presence of both hydrogen and steam, at a temperature and pressure sufficient to generate a stream of methane and carbon monoxide rich product gas;
subjecting the methane and carbon monoxide rich produce gas in a shift reactor to a shift reaction to thereby form a shifted methane rich produce gas, wherein steam for the shift reaction is provided by the unreacted steam from the steam hydrogasification reactor;
wherein the carbon monoxide in the product reacts in the shift reactor with steam to produce hydrogen, and wherein the steam used to react with the carbon monoxide in the shift reactor is obtained only from the steam hydrogasification reactor; and
separating the hydrogen from the shifted methane rich product gas, and recycling at least part of the separated hydrogen to the steam hydrogasification reactor.

### Claim 2 (depends on 1)

The process of claim 1, wherein the carbonaceous material is provided in slurry form.

### Claim 3 (depends on 1)

The process of claim 1, whereby methane content of the methane and carbon monoxide rich product gas is between 10 to 40% on a mole basis.

### Claim 4 (depends on 1)

The process of claim 1, whereby methane content of the methane and carbon monoxide rich product gas is between 30-40% on a dry mole basis.

### Claim 5 (depends on 1)

The process of claim 1, wherein all of the separated hydrogen is recycled back into the steam hydrogasification reactor.

### Claim 6 (depends on 1)

The process of claim 1, wherein the heating is performed without a catalyst.

### Claim 7 (depends on 1)

The process of claim 1, wherein the heating is performed without the injection of oxygen.

### Claim 8 (depends on 1)

The process of claim 1, further comprising a step of removing sulfurous contaminants from the product gas before the step of subjecting the methane and carbon monoxide rich product gas in a shift reactor to a shift reaction.

### Claim 9 (depends on 8)

The process of claim 8, wherein the step of simultaneously heating is carried out at a temperature between 700-1000° C., and wherein the step of removing the sulfurous contaminants is performed at a temperature that is above a dew point of water.

### Claim 10 (depends on 1)

The process of claim 1, further comprising a step of controlling the composition of the product gas from the steam hydrogasification reaction by varying the steam to carbon and the H2 to carbon ratio of the feed.

### Claim 11 (depends on 1)

The process of claim 1 wherein the carbonaceous material comprises municipal waste, biomass, wood, coal, biosolids, or a natural or synthetic polymer.

### Claim 12

A process for converting a slurry of carbonaceous material in water into methane-rich fuel gas, comprising:
simultaneously heating in a hydrogasification reactor the carbonaceous material in the presence of both hydrogen and steam, at a temperature and pressure sufficient to generate a stream of methane and carbon monoxide rich product gas,
wherein all of the steam required for the hydrogasification is formed from the water in the slurry, and
feeding the product gas to a shift reactor, wherein the carbon monoxide of the product gas reacts with unreacted steam from the steam hydrogasification reactor at a temperature of between 200 to 450° C. to produce hydrogen, and wherein the methane is insert at the temperature in the shift reactor to thereby form a methane rich shifted product gas.

### Claim 13

A process for converting a slurry of carbonaceous material in water into methane-rich fuel gas, comprising:
simultaneously heating in a steam hydrogasification reactor the carbonaceous material in the presence of both hydrogen and steam, at a temperature and pressure sufficient to generate a stream of methane and carbon monoxide rich product gas that further contains unreacted steam:
wherein all of the steam required for the hydrogasification is formed from the water in the slurry;
removing sulfurous contaminants from the product gas in the presence of the unreacted steam;
subjecting the carbon monoxide in the produce gas in a shift reactor to a shift reaction at a temperature at which methane is inert to thereby form a shifted methane rich produce gas, wherein steam for the shift for shift reaction is provided by the unreacted steam; and
separating hydrogen from the shifted methane rich product gas, and recycling at least part of the separated hydrogen to the steam hydrogasification reactor.