Landfill gas recovery

• US 5,681,360 A
• Filed: 01/11/1995
• Issued: 10/28/1997
• Est. Priority Date: 01/11/1995
• Status: Expired due to Term

• Current Assignee: Acrion Technologies, Inc.
• Original Assignee: Acrion Technologies, Inc.
• Inventors: Brown, William R., Cook, W. Jeffrey, Siwajek, Lawrence A.
• Primary Examiner(s): MCMAHON, TIMOTHY M
• Application Number:
  US08/371,136
• Time in Patent Office: 1,021 Days
• Field of Search: 48/127.3, 48/127.5, 48/198.3, 48/197 A, 62/17, 95/42, 95/149, 95/229
• US Class Current: 48/127.3
• CPC Class Codes: B01D 2258/05 Biogas
• CPC Class Codes: B01D 53/1418 Recovery of products
• CPC Class Codes: B01D 53/1475 Removing carbon dioxide
• CPC Class Codes: C01B 32/50 Carbon dioxide
• CPC Class Codes: C07C 7/005 Processes comprising at least two steps in series
• CPC Class Codes: C07C 9/04 Methane production by treatment of sewage C02F11/04; natural gas, synthetic natural gas C10L3/06
• CPC Class Codes: F25J 1/0022 Hydrocarbons, e.g. natural gas
• CPC Class Codes: F25J 1/0229 Integration with a unit for using hydrocarbons, e.g. consuming hydrocarbons as feed stock
• CPC Class Codes: F25J 1/023 for the combustion as fuels, i.e. integration with the fuel gas system
• CPC Class Codes: F25J 2200/74 Refluxing the column with at least a part of the partially condensed overhead gas
• CPC Class Codes: F25J 2200/94 Details relating to the withdrawal point
• CPC Class Codes: F25J 2205/50 using absorption, i.e. with selective solvents or lean oil, heavier CnHm and including generally a regeneration step for the solvent or lean oil
• CPC Class Codes: F25J 2210/04 Mixing or blending of fluids with the feed stream
• CPC Class Codes: F25J 2210/66 Landfill or fermentation off-gas, e.g. "Bio-gas"
• CPC Class Codes: F25J 2210/80 Carbon dioxide
• CPC Class Codes: F25J 2215/04 Recovery of liquid products
• CPC Class Codes: F25J 2220/62 Separating low boiling components, e.g. He, H2, N2, Air
• CPC Class Codes: F25J 2220/66 Separating acid gases, e.g. CO2, SO2, H2S or RSH
• CPC Class Codes: F25J 2220/80 Separating impurities from carbon dioxide, e.g. H2O or water-soluble contaminants
• CPC Class Codes: F25J 2220/82 Separating low boiling, i.e. more volatile components, e.g. He, H2, CO, Air gases, CH4
• CPC Class Codes: F25J 2220/84 : Separating high boiling, i.e. less volatile components, e.g. NOx, SOx, H2S
• CPC Class Codes: F25J 2230/04 : Compressor cooling arrangement, e.g. inter- or after-stage cooling or condensate removal
• CPC Class Codes: F25J 2230/30 : Compression of the feed stream
• CPC Class Codes: F25J 2245/02 : Recycle of a stream in general, e.g. a by-pass stream
• CPC Class Codes: F25J 2260/20 : Integration in an installation for liquefying or solidifying a fluid stream
• CPC Class Codes: F25J 2260/60 : Integration in an installation using hydrocarbons, e.g. for fuel purposes
• CPC Class Codes: F25J 2260/80 : Integration in an installation using carbon dioxide, e.g. for EOR, sequestration, refrigeration etc.
• CPC Class Codes: F25J 3/0209 : Natural gas or substitute natural gas
• CPC Class Codes: F25J 3/0233 : separation of CnHm with 1 carbon atom or more
• CPC Class Codes: F25J 3/0266 : separation of carbon dioxide production of carbon dioxide in general C01B32/00
• CPC Class Codes: Y02C 20/40 : of CO2
• CPC Class Codes: Y02E 50/30 : Fuel from waste, e.g. synthetic alcohol or diesel
• CPC Class Codes: Y02P 20/151 : Reduction of greenhouse gas [GHG] emissions, e.g. CO2
• CPC Class Codes: Y10S 62/927 : Natural gas from nitrogen
• CPC Class Codes: Y10S 62/929 : From natural gas

Abstract

A process for concentrating and recovering methane and carbon dioxide from landfill gas includes absorption of commonly occurring pollutants using a reduced amount of carbon dioxide absorbent which itself may be an in situ derived and recoverable constituent. Separated methane may be concentrated into a high heating value fuel, and a highly pure food-grade carbon dioxide product may also be recovered. Process streams may be used to provide fuel for compression and refrigeration and/or to regenerate carbon dioxide absorbent.

Claims

1. A process for separating carbon dioxide from a landfill gas feed stream containing carbon dioxide, methane and trace contaminants of relatively higher boiling gases, comprising the steps

compressing the landfill gas feed stream and removing water therefrom to produce a dehydrated gas stream containing said methane, carbon dioxide and trace contaminants,

introducing said dehydrated gas stream into an absorption column means for absorbing said contaminants with a carbon dioxide absorbent primarily comprising said carbon dioxide present in said landfill gas stream,

withdrawing from said absorption column means, at a first location, a spent absorbent stream containing no more than about 35% of the carbon dioxide contained in the landfill gas feed stream and substantially all of said gas contaminants, withdrawing from said absorption column at a second location above said first location, a carbon dioxide product stream substantially free of contaminants containing a substantial portion of the carbon dioxide originally present in said landfill gas feed stream, and

also withdrawing from said absorption column means a methane product stream substantially free of said contaminants and containing most of the methane originally contained in said landfill gas feed stream.

2. The process of claim 1, wherein said spent absorbent stream contains from about 25 to about 35% of the carbon dioxide originally contained in said landfill gas feed stream.

3. The process of claim 1, including combining the spent absorbent stream with additional landfill gas to form a combined flare stream containing sufficient methane to support combustion and flaring the combined flare stream.

4. The process of claim 1, including the further step of forming food grade carbon dioxide by separating the carbon dioxide in said carbon dioxide product stream from only methane and other relatively lower boiling contaminants.

5. The process of claim 1, wherein said carbon dioxide product stream is a side product stream and said methane product stream is a top product stream containing most of the methane;

and including the further stem of separating the carbon dioxide and methane of said side product stream to form a recycle methane enriched stream that is returned to the process.

6. The process of claim 5, wherein said step of separating the carbon dioxide and methane of the said side product stream includes stripping the methane from the carbon dioxide to form said recycle methane enriched stream and a food grade carbon dioxide product.

7. The process of claim 5, including the further step of forming food grade carbon dioxide by separating the carbon dioxide from only methane and other relatively higher boiling contaminants.

8. The process of claims 4, wherein the step of forming food grade carbon dioxide includes separating the carbon dioxide from methane and other relatively higher boiling contaminants by crystallization.

9. The process of claim 8, wherein the crystallization step is performed at the triple point conditions of carbon dioxide.

10. The process of claim 2, including the further step of reforming said methane enriched product stream to provide a synthesis gas and converting the synthesis gas to methanol.

11. The process of claim 1, wherein said absorption column means comprise first and second absorbers, and including the further steps of withdrawing from said first absorber a combined overhead product stream enriched in methane and containing carbon dioxide to be recovered, introducing said overhead product stream as a feed into said second absorber, withdrawing from said second absorber said methane product stream and said carbon dioxide product stream.

12. The process of claim 11, including the further step of forming food grade carbon dioxide by processing said carbon dioxide product stream to separate carbon dioxide from only methane and other relatively higher boiling contaminants.

13. The process of claim 5 or 11, including the further step of removing additional carbon dioxide from said methane product stream by contacting it with a second absorbent to form a second methane product stream suitable for liquefaction and a second spent absorbent stream containing carbon dioxide removed from said first mentioned methane product stream, liquefying said second methane product stream to form a liquid methane product and an overhead liquefaction gas stream substantially free of carbon dioxide and contaminants, and contacting said second spent absorbent with said overhead liquefaction gas to regenerate the second absorbent and form a stripping gas containing the carbon dioxide stripped from the second spent absorbent stream.

14. The process of claim 13, wherein said stripping gas is substantially free of contaminants and contains a sufficient amount of methane to enable its use as an engine fuel, and said stripping gas is used to provide compression and cooling required in the process.

15. The process of claim 14, wherein said second absorbent is methanol.

16. The process of claim 5 or 11, including the further step of removing additional carbon dioxide from said methane product stream by contact with a second absorbent to form a second methane product stream suitable for liquefaction and a second spent absorbent stream containing carbon dioxide removed from said first mentioned methane product stream, liquefying said second methane product stream to form a liquid methane product and an overhead liquefaction gas stream substantially free of carbon dioxide and contaminants, said overhead liquefaction gas stream being substantially free of contaminants and containing sufficient methane to enable its use as an engine fuel, and said overhead liquefaction gas stream is used to provide compression and cooling required in the process.

17. The process of claim 16, wherein said absorbent is methanol.

33. The process of claim 1, wherein said carbon dioxide product stream contains a majority of the carbon dioxide originally present in said landfill gas stream.

18. A process for separating carbon dioxide from a landfill gas feed stream containing carbon dioxide, methane and trace contaminants of relatively higher boiling gases comprising the steps of:

compressing the landfill gas feed stream and removing water therefrom to produce a dehydrated gas stream containing said methane, carbon dioxide and trace contaminants,

introducing said dehydrated gas stream into an absorption column for absorbing said contaminants with a carbon dioxide absorbent comprising a portion of said carbon dioxide present in said landfill gas stream, and

withdrawing from said absorption column, at a first location, a spent absorbent stream comprising no more than about about 35% of the carbon dioxide contained in the landfill gas feed stream and substantially all of said gas contaminants, withdrawing from said absorption column, at a second location above said first location, a side product stream containing a substantial portion of the carbon dioxide originally contained in said landfill gas feed stream, and withdrawing from said absorption column a methane product stream containing most of the methane originally contained in the landfill gas feed stream.

19. The process of claim 18, wherein said spent absorbent stream contains from about 25 to about 35% of the carbon dioxide originally contained in said landfill gas feed stream.

20. The process of claim 19, wherein said contaminants comprise at least one member selected from the group consisting of toluene, trichloroethylene, methyl ethyl ketone, acetone, methyl mercaptan, vinyl chloride, methyl chloride, Freon-12 and Freon-22, and said spent absorbent stream contains a flow of carbon dioxide just sufficient to achieve an L/KV ratio greater than one for the one or more contaminants present in the landfill gas feed stream.

21. The process of claim 18, including the further step of forming food grade carbon dioxide by separating the carbon dioxide from substantially only methane and other relatively higher boiling contaminants.

22. The process of claims 21, wherein the step of forming food grade carbon dioxide includes separating the carbon dioxide from methane and other relatively higher boiling contaminants by crystallization.

23. The process of claim 22, wherein the crystallization step is performed at the triple point conditions of carbon dioxide.

24. The process of claim 18, including the further step of reforming said methane enriched product stream to provide a synthesis gas and converting the synthesis gas to methanol.

25. The process of claim 20, including the further step of removing additional carbon dioxide from said methane product stream by contact with a second absorbent to form a second methane product stream suitable for liquefaction and a second spent absorbent stream containing carbon dioxide removed from said first mentioned methane product stream, liquefying said second methane product stream to form a liquid methane product and an overhead liquefaction gas stream substantially free of carbon dioxide and contaminants, and contacting said second spent absorbent with said overhead liquefaction gas to regenerate the second absorbent and form a stripping gas containing the carbon dioxide stripped from the second spent absorbent.

26. The process of claim 25, wherein said stripping gas is substantially free of contaminants and contains a sufficient amount of methane to enable its use as an internal combustion engine fuel, and said stripping gas is used to provide compression and cooling required in the process.

27. A process for separating carbon dioxide from a landfill gas feed stream containing carbon dioxide, methane and trace contaminants of relatively higher boiling gases comprising the steps of:

compressing the landfill gas feed stream and removing water therefrom to produce a dehydrated gas stream containing said methane, carbon dioxide and trace contaminants,

introducing said dehydrated gas stream into a first absorption column for absorbing said contaminants with a carbon dioxide absorbent comprising a portion of said carbon dioxide present in said landfill gas feed stream,

withdrawing from said first absorption column absorber, at a first location, a spent absorbent stream comprising no more than about about 35% of the carbon dioxide contained in the landfill gas feed stream and substantially all of said gas contaminants, and a combined overhead product stream enriched in methane and containing carbon dioxide to be recovered,

introducing said combined overhead product stream from said first absorption column, as a feed, into a second absorption column to separate carbon dioxide from methane using a carbon dioxide absorbent to form a bottom product containing methane and a substantial portion of the carbon dioxide originally present in the landfill gas feed stream and a methane product stream substantially free of said contaminants and containing most of the methane originally present in the landfill gas stream.

28. The process of claim 27, wherein said spent absorbent stream contains from about 25 to about 35% of the carbon dioxide originally contained in said landfill gas feed stream.

29. The process of claim 28, wherein said contaminants comprise at least one member selected from the group consisting of toluene, trichloroethylene, methyl ethyl ketone, acetone, methyl mercaptan, vinyl chloride, methyl chloride, Freon-12 and Freon-22, and said spent absorbent stream contains a flow of carbon dioxide just sufficient to achieve an L/KV ratio greater than one for the one or more contaminants present in the landfill gas feed stream.

30. The process of claim 27, including the further step of forming food grade carbon dioxide by separating the carbon dioxide from only methane and other relatively higher boiling contaminants.

31. The process of claim 27, including the further step of removing additional carbon dioxide from said methane product stream by contact with a second absorbent to form a second methane product stream suitable for liquefaction and a second spent absorbent containing carbon dioxide removed from said first mentioned methane product stream, liquefying said second methane product stream to form a liquid methane product and an overhead liquefaction gas stream substantially free of carbon dioxide and contaminants, and contacting said second spent absorbent with said overhead liquefaction gas to regenerate the absorbent and form a stripping gas containing the carbon dioxide stripped from the second spent absorbent.

32. The process of claim 31, wherein said stripping gas is substantially free of contaminants and contains a sufficient amount of methane to enable its use as an engine fuel, and said stripping gas is used to provide substantially all of the compression and cooling required in the process.