CA2783297C - In-situ microbial oxygen generation and hydrocarbon conversion in a hydrocarbon containing formation - Google Patents
In-situ microbial oxygen generation and hydrocarbon conversion in a hydrocarbon containing formation Download PDFInfo
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- 229930195733 hydrocarbon Natural products 0.000 title claims abstract description 57
- 150000002430 hydrocarbons Chemical class 0.000 title claims abstract description 57
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 title claims abstract description 51
- 229910052760 oxygen Inorganic materials 0.000 title claims abstract description 48
- 239000001301 oxygen Substances 0.000 title claims abstract description 48
- 230000015572 biosynthetic process Effects 0.000 title claims abstract description 45
- 230000000813 microbial effect Effects 0.000 title claims abstract description 30
- 239000004215 Carbon black (E152) Substances 0.000 title claims abstract description 26
- 238000011065 in-situ storage Methods 0.000 title claims abstract description 21
- 238000006243 chemical reaction Methods 0.000 title claims description 20
- XTEGARKTQYYJKE-UHFFFAOYSA-M Chlorate Chemical compound [O-]Cl(=O)=O XTEGARKTQYYJKE-UHFFFAOYSA-M 0.000 claims abstract description 70
- 238000000034 method Methods 0.000 claims abstract description 62
- 244000005700 microbiome Species 0.000 claims abstract description 46
- 239000000203 mixture Substances 0.000 claims abstract description 17
- 239000012530 fluid Substances 0.000 claims abstract description 16
- 239000011148 porous material Substances 0.000 claims abstract description 14
- 241000894006 Bacteria Species 0.000 claims abstract description 13
- 241000205046 Archaeoglobus Species 0.000 claims abstract description 9
- 241000626621 Geobacillus Species 0.000 claims abstract description 6
- 241000589596 Thermus Species 0.000 claims abstract description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 30
- 239000003921 oil Substances 0.000 claims description 20
- 239000000356 contaminant Substances 0.000 claims description 14
- 235000014113 dietary fatty acids Nutrition 0.000 claims description 14
- 229930195729 fatty acid Natural products 0.000 claims description 14
- 239000000194 fatty acid Substances 0.000 claims description 14
- 150000004665 fatty acids Chemical class 0.000 claims description 14
- 239000010779 crude oil Substances 0.000 claims description 12
- 239000003345 natural gas Substances 0.000 claims description 11
- VLTRZXGMWDSKGL-UHFFFAOYSA-M perchlorate Inorganic materials [O-]Cl(=O)(=O)=O VLTRZXGMWDSKGL-UHFFFAOYSA-M 0.000 claims description 11
- 230000009467 reduction Effects 0.000 claims description 11
- 229910001919 chlorite Inorganic materials 0.000 claims description 10
- 229910052619 chlorite group Inorganic materials 0.000 claims description 10
- QBWCMBCROVPCKQ-UHFFFAOYSA-N chlorous acid Chemical compound OCl=O QBWCMBCROVPCKQ-UHFFFAOYSA-N 0.000 claims description 10
- VLTRZXGMWDSKGL-UHFFFAOYSA-N perchloric acid Chemical compound OCl(=O)(=O)=O VLTRZXGMWDSKGL-UHFFFAOYSA-N 0.000 claims description 9
- 238000011084 recovery Methods 0.000 claims description 9
- 238000002347 injection Methods 0.000 claims description 7
- 239000007924 injection Substances 0.000 claims description 7
- 239000000126 substance Substances 0.000 claims description 7
- 108090000790 Enzymes Proteins 0.000 claims description 5
- 102000004190 Enzymes Human genes 0.000 claims description 5
- 238000007323 disproportionation reaction Methods 0.000 claims description 5
- 229910052739 hydrogen Inorganic materials 0.000 claims description 5
- 239000001257 hydrogen Substances 0.000 claims description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 5
- 229910002651 NO3 Inorganic materials 0.000 claims description 4
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 4
- 230000000593 degrading effect Effects 0.000 claims description 4
- -1 poly thionates Chemical compound 0.000 claims description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 claims description 3
- FERIUCNNQQJTOY-UHFFFAOYSA-M Butyrate Chemical compound CCCC([O-])=O FERIUCNNQQJTOY-UHFFFAOYSA-M 0.000 claims description 3
- FERIUCNNQQJTOY-UHFFFAOYSA-N Butyric acid Natural products CCCC(O)=O FERIUCNNQQJTOY-UHFFFAOYSA-N 0.000 claims description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 3
- 150000002431 hydrogen Chemical class 0.000 claims description 3
- 241000531184 Ferroglobus Species 0.000 claims description 2
- 108090000913 Nitrate Reductases Proteins 0.000 claims description 2
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 2
- 241000205101 Sulfolobus Species 0.000 claims description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims description 2
- 241000605118 Thiobacillus Species 0.000 claims description 2
- 241000605261 Thiomicrospira Species 0.000 claims description 2
- 108010075269 chlorate reductase Proteins 0.000 claims description 2
- 108010055547 chlorite dismutase Proteins 0.000 claims description 2
- 241001148470 aerobic bacillus Species 0.000 claims 3
- 239000000370 acceptor Substances 0.000 claims 2
- 150000003464 sulfur compounds Chemical class 0.000 claims 2
- IOVCWXUNBOPUCH-UHFFFAOYSA-M Nitrite anion Chemical compound [O-]N=O IOVCWXUNBOPUCH-UHFFFAOYSA-M 0.000 claims 1
- 108090000854 Oxidoreductases Proteins 0.000 claims 1
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims 1
- 208000031513 cyst Diseases 0.000 claims 1
- 230000000694 effects Effects 0.000 claims 1
- 239000003344 environmental pollutant Substances 0.000 claims 1
- 239000002105 nanoparticle Substances 0.000 claims 1
- 230000037361 pathway Effects 0.000 claims 1
- 231100000719 pollutant Toxicity 0.000 claims 1
- 229920001021 polysulfide Polymers 0.000 claims 1
- 239000005077 polysulfide Substances 0.000 claims 1
- 150000008117 polysulfides Polymers 0.000 claims 1
- 235000011149 sulphuric acid Nutrition 0.000 claims 1
- 230000001939 inductive effect Effects 0.000 abstract description 4
- 238000005755 formation reaction Methods 0.000 description 28
- 230000008569 process Effects 0.000 description 11
- 229930192474 thiophene Natural products 0.000 description 6
- 150000003577 thiophenes Chemical class 0.000 description 6
- 238000010796 Steam-assisted gravity drainage Methods 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 241000203069 Archaea Species 0.000 description 4
- 150000001335 aliphatic alkanes Chemical class 0.000 description 4
- 239000003245 coal Substances 0.000 description 4
- 235000015097 nutrients Nutrition 0.000 description 4
- 241000205042 Archaeoglobus fulgidus Species 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 239000010426 asphalt Substances 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 239000000295 fuel oil Substances 0.000 description 3
- 238000009533 lab test Methods 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 238000012216 screening Methods 0.000 description 3
- JVTAAEKCZFNVCJ-UHFFFAOYSA-M Lactate Chemical compound CC(O)C([O-])=O JVTAAEKCZFNVCJ-UHFFFAOYSA-M 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000013073 enabling process Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 239000003079 shale oil Substances 0.000 description 2
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Chemical compound [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 description 2
- 230000004936 stimulating effect Effects 0.000 description 2
- 108020004465 16S ribosomal RNA Proteins 0.000 description 1
- 241000186216 Corynebacterium Species 0.000 description 1
- 241000283986 Lepus Species 0.000 description 1
- 241000186359 Mycobacterium Species 0.000 description 1
- 241000187644 Mycobacterium vaccae Species 0.000 description 1
- 108010025915 Nitrite Reductases Proteins 0.000 description 1
- 241000589517 Pseudomonas aeruginosa Species 0.000 description 1
- 241000589776 Pseudomonas putida Species 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006065 biodegradation reaction Methods 0.000 description 1
- 239000012267 brine Substances 0.000 description 1
- 239000011162 core material Substances 0.000 description 1
- 238000005202 decontamination Methods 0.000 description 1
- 230000003588 decontaminative effect Effects 0.000 description 1
- 230000001419 dependent effect Effects 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000011010 flushing procedure Methods 0.000 description 1
- 239000008398 formation water Substances 0.000 description 1
- 125000000524 functional group Chemical group 0.000 description 1
- 238000011534 incubation Methods 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 238000002955 isolation Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 230000007483 microbial process Effects 0.000 description 1
- 238000009629 microbiological culture Methods 0.000 description 1
- 238000012544 monitoring process Methods 0.000 description 1
- 239000004058 oil shale Substances 0.000 description 1
- 238000011946 reduction process Methods 0.000 description 1
- 235000010344 sodium nitrate Nutrition 0.000 description 1
- HPALAKNZSZLMCH-UHFFFAOYSA-M sodium;chloride;hydrate Chemical compound O.[Na+].[Cl-] HPALAKNZSZLMCH-UHFFFAOYSA-M 0.000 description 1
- 230000000638 stimulation Effects 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 239000011275 tar sand Substances 0.000 description 1
- 235000013619 trace mineral Nutrition 0.000 description 1
- 239000011573 trace mineral Substances 0.000 description 1
- 230000035899 viability Effects 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
- C12P1/00—Preparation of compounds or compositions, not provided for in groups C12P3/00 - C12P39/00, by using microorganisms or enzymes
- C12P1/04—Preparation of compounds or compositions, not provided for in groups C12P3/00 - C12P39/00, by using microorganisms or enzymes by using bacteria
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K8/00—Compositions for drilling of boreholes or wells; Compositions for treating boreholes or wells, e.g. for completion or for remedial operations
- C09K8/58—Compositions for enhanced recovery methods for obtaining hydrocarbons, i.e. for improving the mobility of the oil, e.g. displacing fluids
- C09K8/582—Compositions for enhanced recovery methods for obtaining hydrocarbons, i.e. for improving the mobility of the oil, e.g. displacing fluids characterised by the use of bacteria
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K8/00—Compositions for drilling of boreholes or wells; Compositions for treating boreholes or wells, e.g. for completion or for remedial operations
- C09K8/58—Compositions for enhanced recovery methods for obtaining hydrocarbons, i.e. for improving the mobility of the oil, e.g. displacing fluids
- C09K8/592—Compositions used in combination with generated heat, e.g. by steam injection
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K8/00—Compositions for drilling of boreholes or wells; Compositions for treating boreholes or wells, e.g. for completion or for remedial operations
- C09K8/60—Compositions for stimulating production by acting on the underground formation
-
- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
- C12P3/00—Preparation of elements or inorganic compounds except carbon dioxide
Abstract
A method for in-situ microbial oxygen generation in an underground hydrocarbon containing formation comprises : - injecting into the formation an oxygen generating composition comprising thermophilic chlorate reducing micro-organisms, such as bacteria of the genus Archaeoglobus, Geobacillus and/or Thermus, which multiply at a temperature of at least 60° C; and - inducing the multiplied micro-organisms to convert the hydrocarbons and/or other pore fluid components in-situ into transportable or disposable products
Description
IN-SITU MICROBIAL OXYGEN GENERATION AND HYDROCARBON CONVERSION IN A
HYDROCARBON CONTAINING FORMATION
BACKGROUND OF THE INVENTION
The invention relates to a method for in-situ oxygen generation in a hydrocarbon containing formation.
Such a method is known from US patent 5,163,510.
The method known from this prior art reference comprises:
- injecting into the formation a fluid comprising a source of oxygen that chemically releases oxygen into the formation;
- inducing micro-organisms present in the formation to multiply using the oil as their carbon source and the chemically produced oxygen in the injection water as their oxygen source; and - allowing the multiplied micro-organisms to convert oil from the environment.
In this known method the source of oxygen is provided by injecting water comprising an oxidizing compound selected from the group consisting of H202, NaC1O3, KC1O4, NaNO3 and combinations thereof, which are assumed to be chemically converted to result in oxygen. This assumption is based on the fact that oxygen generation from Microbial Chlorate Reduction was for the first time reported in 1996 by van Ginkel at al in 1996, Archives of Microbiology 166:321-326.
In accordance with the teachings of US patent 5,163,510 the chemically generated oxygen is then used by microbes to convert hydrocarbons.
Limitations of the use of the known oxidizing compounds known from US patent 5,163,510 for chemical oxygen generation are that H202 may dissociate during or shortly after the injection process, and that chemical
HYDROCARBON CONTAINING FORMATION
BACKGROUND OF THE INVENTION
The invention relates to a method for in-situ oxygen generation in a hydrocarbon containing formation.
Such a method is known from US patent 5,163,510.
The method known from this prior art reference comprises:
- injecting into the formation a fluid comprising a source of oxygen that chemically releases oxygen into the formation;
- inducing micro-organisms present in the formation to multiply using the oil as their carbon source and the chemically produced oxygen in the injection water as their oxygen source; and - allowing the multiplied micro-organisms to convert oil from the environment.
In this known method the source of oxygen is provided by injecting water comprising an oxidizing compound selected from the group consisting of H202, NaC1O3, KC1O4, NaNO3 and combinations thereof, which are assumed to be chemically converted to result in oxygen. This assumption is based on the fact that oxygen generation from Microbial Chlorate Reduction was for the first time reported in 1996 by van Ginkel at al in 1996, Archives of Microbiology 166:321-326.
In accordance with the teachings of US patent 5,163,510 the chemically generated oxygen is then used by microbes to convert hydrocarbons.
Limitations of the use of the known oxidizing compounds known from US patent 5,163,510 for chemical oxygen generation are that H202 may dissociate during or shortly after the injection process, and that chemical
2 -conversion of NaNO3r NaClO3 and KC1O4do not generate oxygen at temperatures lower than 1200 Celsius.
Moreover, the microbes Pseudomonas putida, Pseudomonas aeruginosa, Corynebacterium lepus, Mycobacterium rhodochrous and Mycobacterium vaccae disclosed in US patent 5,163,510 are non-thermophilic micro-organisms, which are unable to reduce chlorate and/or multiply at temperature of at least 60 C. This will prevent the method known from US patent 5,163,510 to be beneficial for application throughout an entire hydrocarbon containing formation as the ambient temperature in a hydrocarbon containing formation often exceeds 60 C.
The use of microbial chlorate reduction as mechanism for in-situ oxygen generation and thereby stimulating microbial activity using hydrocarbons as carbon and energy source has been reported for the bioremediation of hydrocarbon spills at ambient atmospheric temperatures in the following prior art references:
- Coates et al., 1998, Nature 396(6713): 730 - Coates et al., 1999, Applied Environmental Microbiology 65(12): 5234-5341 - Coates et al., 2004, US patent 2004/0014196A1 , which prior art references are collectively referred to as Coates et al (1998, 1999, 2004) - Tan et al., 2006, Biodegradation 17(1): 113-119 - Mehboob et al., 2009: Applied Microbiology and Biotechnology 83(4): 739-747 - Langenhoff et al., 2009, Bioremediation Journal, 13(4):
There is a need to provide an method for in-situ thermophilic microbial oxygen generation wherein a controlled amount of oxygen is microbiologically produced in-situ deeper in the hydrocarbon containing formation where the temperature is at least 60 C.
Moreover, the microbes Pseudomonas putida, Pseudomonas aeruginosa, Corynebacterium lepus, Mycobacterium rhodochrous and Mycobacterium vaccae disclosed in US patent 5,163,510 are non-thermophilic micro-organisms, which are unable to reduce chlorate and/or multiply at temperature of at least 60 C. This will prevent the method known from US patent 5,163,510 to be beneficial for application throughout an entire hydrocarbon containing formation as the ambient temperature in a hydrocarbon containing formation often exceeds 60 C.
The use of microbial chlorate reduction as mechanism for in-situ oxygen generation and thereby stimulating microbial activity using hydrocarbons as carbon and energy source has been reported for the bioremediation of hydrocarbon spills at ambient atmospheric temperatures in the following prior art references:
- Coates et al., 1998, Nature 396(6713): 730 - Coates et al., 1999, Applied Environmental Microbiology 65(12): 5234-5341 - Coates et al., 2004, US patent 2004/0014196A1 , which prior art references are collectively referred to as Coates et al (1998, 1999, 2004) - Tan et al., 2006, Biodegradation 17(1): 113-119 - Mehboob et al., 2009: Applied Microbiology and Biotechnology 83(4): 739-747 - Langenhoff et al., 2009, Bioremediation Journal, 13(4):
There is a need to provide an method for in-situ thermophilic microbial oxygen generation wherein a controlled amount of oxygen is microbiologically produced in-situ deeper in the hydrocarbon containing formation where the temperature is at least 60 C.
3 -There is furthermore a need to provide an enabling process for the stimulation of in-situ thermophilic microbial conversion of hydrocarbons wherein oxygen is microbiologically produced from the injected oxygen source only at high temperature locations in a hydrocarbon containing formation where injected or indigenous micro-organisms encounter the injected electron acceptor in addition to an electron donor, such as hydrocarbons, volatile fatty acids, etc.
There is also a need for a method for thermophilic microbial oxygen generation through chlorate reduction at the oil water interface, in contrast to chemical generation of oxygen known from US patent 5,163,510 that can also occur in oil-poor parts of the reservoir.
Utilization of microbes to enhance hydrocarbon recovery is hampered by the limited bioavailability and biodegradability of the hydrocarbons under hot reservoir conditions.
Thus there is also a need to provide a way to improve bioavailability and biodegradability in hot hydrocarbon containing formations where the ambient temperature is at least 60 C.
SUMMARY OF THE INVENTION
In accordance with the invention there is provided a method for in-situ oxygen generation in an underground hydrocarbon containing formation, the method comprising injecting into the formation an oxygen generating composition which releases oxygen (02) by reduction of chlorate (C103-), wherein:
- the formation has a temperature of at least 60 C;
- the composition comprises thermophilic chlorate reducing micro-organisms, which multiply at an ambient temperature of at least 60 C,; and - the multiplied thermophilic chlorate reducing micro-
There is also a need for a method for thermophilic microbial oxygen generation through chlorate reduction at the oil water interface, in contrast to chemical generation of oxygen known from US patent 5,163,510 that can also occur in oil-poor parts of the reservoir.
Utilization of microbes to enhance hydrocarbon recovery is hampered by the limited bioavailability and biodegradability of the hydrocarbons under hot reservoir conditions.
Thus there is also a need to provide a way to improve bioavailability and biodegradability in hot hydrocarbon containing formations where the ambient temperature is at least 60 C.
SUMMARY OF THE INVENTION
In accordance with the invention there is provided a method for in-situ oxygen generation in an underground hydrocarbon containing formation, the method comprising injecting into the formation an oxygen generating composition which releases oxygen (02) by reduction of chlorate (C103-), wherein:
- the formation has a temperature of at least 60 C;
- the composition comprises thermophilic chlorate reducing micro-organisms, which multiply at an ambient temperature of at least 60 C,; and - the multiplied thermophilic chlorate reducing micro-
4 -organisms convert the hydrocarbons and/or other pore fluids in-situ into transportable or disposable products.
In an embodiment the thermophilic chlorate reducing micro-organisms comprise bacteria of the genus Archaeoglobus, Geobacillus and/or Thermus and use hydrogen (H) and electrons(e) provided by hydrocarbons, volatile fatty acids and/or other pore fluids in the formation followed by dismutation of chlorite(Cl02-) by the micro-organisms on the basis of the reactions:
C103 + 2H+ +2e -> C102- +H20 C102 -> Cl- +02 In a suitable embodiment the thermophilic chlorate reducing micro-organisms multiply at an ambient temperature of at least 800 C and comprise bacteria of the genus Archaeoglobus fulgidis.
Optionally, the method according to the invention furthermore comprises:
- injecting into the formation an oxygen generating composition, which comprise or generates chlorate in the formation and which releases oxygen (02) by thermophilic microbial reduction of chlorate(C103) by the micro-organisms, using hydrogen (H) and electrons (e) provided by the hydrocarbons, volatile fatty acids and/or other pore fluid components, such as oil & gas contaminants such as H2S, thiophenes and mercaptanes, followed by dismutation of chlorite (C102) by micro-organisms on the basis of the reactions:
C103 + 2H+ +2e -> C102- +H20 C102- -> Cl- +02;
- inducing multiplication of the thermophilic chlorate-reducing micro-organisms (Archaeoglobus, Geobacillus, Thermus), other chlorate-reducing thermophilic micro-organisms and other micro-organisms that can use the hydrocarbons, volatile fatty acids and/or other pore fluid
In an embodiment the thermophilic chlorate reducing micro-organisms comprise bacteria of the genus Archaeoglobus, Geobacillus and/or Thermus and use hydrogen (H) and electrons(e) provided by hydrocarbons, volatile fatty acids and/or other pore fluids in the formation followed by dismutation of chlorite(Cl02-) by the micro-organisms on the basis of the reactions:
C103 + 2H+ +2e -> C102- +H20 C102 -> Cl- +02 In a suitable embodiment the thermophilic chlorate reducing micro-organisms multiply at an ambient temperature of at least 800 C and comprise bacteria of the genus Archaeoglobus fulgidis.
Optionally, the method according to the invention furthermore comprises:
- injecting into the formation an oxygen generating composition, which comprise or generates chlorate in the formation and which releases oxygen (02) by thermophilic microbial reduction of chlorate(C103) by the micro-organisms, using hydrogen (H) and electrons (e) provided by the hydrocarbons, volatile fatty acids and/or other pore fluid components, such as oil & gas contaminants such as H2S, thiophenes and mercaptanes, followed by dismutation of chlorite (C102) by micro-organisms on the basis of the reactions:
C103 + 2H+ +2e -> C102- +H20 C102- -> Cl- +02;
- inducing multiplication of the thermophilic chlorate-reducing micro-organisms (Archaeoglobus, Geobacillus, Thermus), other chlorate-reducing thermophilic micro-organisms and other micro-organisms that can use the hydrocarbons, volatile fatty acids and/or other pore fluid
5 PCT/EP2010/070666 -components (e.g. oil & gas contaminants as H2S, thiophenes and mercaptanes) as their carbon source and/or electron donor and the injected composition or the oxygen generated by thermophilic chlorate reduction thereby as their electron 5 acceptor and/or oxygen source; and - inducing the multiplied micro-organisms to convert the hydrocarbons and/or other pore fluid components in-situ into transportable products, such as in Microbial Enhanced Oil Recovery(MEOR) and/or ECBM Enhanced Coal Bed Methane(ECBM) processes.
The multiplied thermophilic micro-organisms generated in accordance with the method according to present invention may be used for in-situ conversion of coal, shale oil, oilshale, bitumen and/or a viscous crude oil into a synthetic crude oil with a reduced viscosity and/or to convert associated contaminants, such as H2S, thiophenes and mercaptanes, into oxidized sulfur fractions that remain within the reservoir brine.
The method according to the invention may be used to improve bioavailability and biodegradability of hydrocarbons at thermophilic (60 - 120 C) & anaerobic conditions in underground formations containing hydrocarbons, volatile fatty acids and other pore fluid components and micro-organisms, by the process of Thermophilic Microbial Chlorate Reduction. The process will generate oxygen in-situ that will enhance bioavailability and biodegradability, which subsequently will enables enhanced recovery of hydrocarbons (of improved quality) via other process like Microbial Enhanced Oil Recovery (MEOR), Microbial Enhanced Coalbed Methane (MECBM) or pretreatment of heavy hydrocarbon crudes (heavy oil, bitumen) prior to processes as Steam Assisted Gravity Drainage (SAGD).
The oxygen generating composition may comprise
The multiplied thermophilic micro-organisms generated in accordance with the method according to present invention may be used for in-situ conversion of coal, shale oil, oilshale, bitumen and/or a viscous crude oil into a synthetic crude oil with a reduced viscosity and/or to convert associated contaminants, such as H2S, thiophenes and mercaptanes, into oxidized sulfur fractions that remain within the reservoir brine.
The method according to the invention may be used to improve bioavailability and biodegradability of hydrocarbons at thermophilic (60 - 120 C) & anaerobic conditions in underground formations containing hydrocarbons, volatile fatty acids and other pore fluid components and micro-organisms, by the process of Thermophilic Microbial Chlorate Reduction. The process will generate oxygen in-situ that will enhance bioavailability and biodegradability, which subsequently will enables enhanced recovery of hydrocarbons (of improved quality) via other process like Microbial Enhanced Oil Recovery (MEOR), Microbial Enhanced Coalbed Methane (MECBM) or pretreatment of heavy hydrocarbon crudes (heavy oil, bitumen) prior to processes as Steam Assisted Gravity Drainage (SAGD).
The oxygen generating composition may comprise
6 -perchlorate (Cl04-) from which chlorate(Cl03-) is generated using electrons released by hydrocarbons, volatile fatty acids and/or other pore fluid components (e.g. oil & gas contaminants as H2S, thiophenes and mercaptanes) as electron donor on the basis of the following reaction:
C104- + 2H+ + 2e -> C103 + H20.
The hydrocarbons may comprise viscous crude oil, coal and/or other long chain hydrocarbons and the micro-organisms may comprise thermophilic (per)chlorate-reducing bacteria or archaea, such as archaea and bacteria of the genus Archaeoglobus, Geobacillus, Thermus and/or other thermophilic genera able to reduce chlorate and convert fatty acids or long chain hydrocarbons into short chain hydrocarbons being indigenous to the formation or introduced by injection.
The other pore fluid components may comprise fatty acids, natural gas contaminants; H2S, thiophenes, and mercaptanes, in which case the micro-organisms may comprise archaea and bacteria of the genus Archaeoglobus, Sulfolobus, Ferroglobus, Thiobacillus, Thiomicrospira or other genera able to convert natural gas contaminants.
These and other features, embodiments and advantages of the method according to the invention are described in the accompanying claims, abstract and the following detailed description of a non-limiting hypothetical example.
The present invention novelty compared to the inventions previously reported resides in:
Providing a microbial chlorate-reducing and oxygen-generating process (i.e. different from the invention of US patent 5,163,510, in which oxygen is assumed to be chemically produced (not by chlorate-reducing
C104- + 2H+ + 2e -> C103 + H20.
The hydrocarbons may comprise viscous crude oil, coal and/or other long chain hydrocarbons and the micro-organisms may comprise thermophilic (per)chlorate-reducing bacteria or archaea, such as archaea and bacteria of the genus Archaeoglobus, Geobacillus, Thermus and/or other thermophilic genera able to reduce chlorate and convert fatty acids or long chain hydrocarbons into short chain hydrocarbons being indigenous to the formation or introduced by injection.
The other pore fluid components may comprise fatty acids, natural gas contaminants; H2S, thiophenes, and mercaptanes, in which case the micro-organisms may comprise archaea and bacteria of the genus Archaeoglobus, Sulfolobus, Ferroglobus, Thiobacillus, Thiomicrospira or other genera able to convert natural gas contaminants.
These and other features, embodiments and advantages of the method according to the invention are described in the accompanying claims, abstract and the following detailed description of a non-limiting hypothetical example.
The present invention novelty compared to the inventions previously reported resides in:
Providing a microbial chlorate-reducing and oxygen-generating process (i.e. different from the invention of US patent 5,163,510, in which oxygen is assumed to be chemically produced (not by chlorate-reducing
7 -microorganisms) and only assumes microbial utilization of oxygen);
Providing such microbial chlorate-reducing and oxygen-releasing process that can operate at high temperatures in the range from 60 C up to 120 C
relevant to hydrocarbon containing reservoirs.
The microbial method according to the invention can operate at an elevated temperature of at least 600 C and is therefore different from the bioremediation method disclosed in US patent application 2004/0014196 Al (Coates), which releases oxygen at temperatures < 40 C
and the method known from US patent 5,163,510 that enables the use of micro-organisms at a temperature below 60 C (but not higher) and therefore seriously limits the application of the known method in hot hydrocarbon containing formations.
The thermophilic microbial chlorate-reducing and oxygen-releasing method according to the invention enhances bioavailability and biodegradability of hydrocarbons, which subsequently enables enhanced recovery of upgraded hydrocarbons from hydrocarbon containing formations optionally by:
a) enhanced oil recovery from oil bearing formations (MEOR), b) enhanced methane production of coal reservoirs (ECBM), c) pretreatment of heavy oil deposits before SAGD
operation; and d) in-situ conversion of oil and natural gas contaminants; H2S, thiophenes and mercaptanes, which conversion involves decontamination of hydrocarbons and is therefore different from US patent 2004/0014196A1, which aims to bioremediate hydrocarbons in a shallow low temperature environment or US patent 5,163,510, which aims to stimulate MEOR only.
Providing such microbial chlorate-reducing and oxygen-releasing process that can operate at high temperatures in the range from 60 C up to 120 C
relevant to hydrocarbon containing reservoirs.
The microbial method according to the invention can operate at an elevated temperature of at least 600 C and is therefore different from the bioremediation method disclosed in US patent application 2004/0014196 Al (Coates), which releases oxygen at temperatures < 40 C
and the method known from US patent 5,163,510 that enables the use of micro-organisms at a temperature below 60 C (but not higher) and therefore seriously limits the application of the known method in hot hydrocarbon containing formations.
The thermophilic microbial chlorate-reducing and oxygen-releasing method according to the invention enhances bioavailability and biodegradability of hydrocarbons, which subsequently enables enhanced recovery of upgraded hydrocarbons from hydrocarbon containing formations optionally by:
a) enhanced oil recovery from oil bearing formations (MEOR), b) enhanced methane production of coal reservoirs (ECBM), c) pretreatment of heavy oil deposits before SAGD
operation; and d) in-situ conversion of oil and natural gas contaminants; H2S, thiophenes and mercaptanes, which conversion involves decontamination of hydrocarbons and is therefore different from US patent 2004/0014196A1, which aims to bioremediate hydrocarbons in a shallow low temperature environment or US patent 5,163,510, which aims to stimulate MEOR only.
8 -The method according to the invention generates oxygen in-situ that will enhance bioavailability and biodegradability, which subsequently will enable enhanced recovery of hydrocarbons (of improved quality) via other process like Microbial Enhanced Oil Recovery (MEOR), Microbial Enhanced Coalbed Methane (MECBM) or pretreatment of heavy hydrocarbon crudes (heavy oil, bitumen) prior to processes as Steam Assisted Gravity Drainage (SAGD). The process can also enable in-situ natural gas contaminant removal resulting in upgraded hydrocarbons. The invention should therefore be considered as a strong enabling process for other subsurface thermophilic microbial processes.
When used in this specification and claims the term thermophilic chlorate reducing micro-organisms means that these micro-organisms multiply at an ambient temperature of at least 60 C.
These and other features, embodiments and advantages of the method according to the invention are described in the accompanying claims, abstract and the following detailed description of non-limiting embodiments depicted in the accompanying drawing.
BRIEF DESCRIPTION OF THE DRAWING
FIG.1 shows the consumption of lactate as an electron donor and conversion of chlorate to chloride at 85 C by the thermophilic Archaeoglobus fulgidus DSM4139 microorganism in laboratory experiment that demonstrates the viability of the method according to the invention at an elevated temperature.
DETAILED DESCRIPTION OF THE DEPICTED EMBODIMENT
FIG.1 shows the results of a laboratory experiments which demonstrated that Archaea from the genus Archaeoglobus can perform chlorate reduction at temperatures up to 85-95 C.
When used in this specification and claims the term thermophilic chlorate reducing micro-organisms means that these micro-organisms multiply at an ambient temperature of at least 60 C.
These and other features, embodiments and advantages of the method according to the invention are described in the accompanying claims, abstract and the following detailed description of non-limiting embodiments depicted in the accompanying drawing.
BRIEF DESCRIPTION OF THE DRAWING
FIG.1 shows the consumption of lactate as an electron donor and conversion of chlorate to chloride at 85 C by the thermophilic Archaeoglobus fulgidus DSM4139 microorganism in laboratory experiment that demonstrates the viability of the method according to the invention at an elevated temperature.
DETAILED DESCRIPTION OF THE DEPICTED EMBODIMENT
FIG.1 shows the results of a laboratory experiments which demonstrated that Archaea from the genus Archaeoglobus can perform chlorate reduction at temperatures up to 85-95 C.
9 -Archaeoglobus have often been encountered in hydrocarbon containing high temperature reservoirs as evident from molecular and cultivation experiments.
Moreover, members of this genus have been shown to be able to convert fatty acids and alkanes. Members of this genus therefore are one of the most relevant candidates for the thermophilic microbial chlorate-reduction process.
FIG.1 illustrates the results of a laboratory experiment in which lactate was consumed as electron donor and chlorate was converted into chloride at 85 C
by the micro-organism comprising bacteria of the genus Archaeoglobus fulgidus DSM4139.
It is observed that thermophilic microbial (Per)Chlorate Reduction at a temperature of at least 60 C
has never been described in the prior art for hot hydrocarbon containing environments with fatty acids or hydrocarbons as electron donor and that the experiment revealed that bacteria of the genus Archaeoglobus fulgidus DSM4139 will have an unexpectedly good performance for thermophilic microbial (Per)Chlorate Reduction in a hot hydrocarbon containing formation at an ambient temperature of at least 60 C.
EXAMPLE
A suitable embodiment of the method according to the invention, comprises the following steps:
a)Screening whether a target underground crude oil and/or natural gas containing reservoir formation has features, such as temperature, salinity, heterogeneity, oil characteristics, micro-organisms, volatile fatty acids, hydrogen ions, acetate, propionate or butyrate and/or other potential electron donors, etc., which allow use of the method according to the invention;
Moreover, members of this genus have been shown to be able to convert fatty acids and alkanes. Members of this genus therefore are one of the most relevant candidates for the thermophilic microbial chlorate-reduction process.
FIG.1 illustrates the results of a laboratory experiment in which lactate was consumed as electron donor and chlorate was converted into chloride at 85 C
by the micro-organism comprising bacteria of the genus Archaeoglobus fulgidus DSM4139.
It is observed that thermophilic microbial (Per)Chlorate Reduction at a temperature of at least 60 C
has never been described in the prior art for hot hydrocarbon containing environments with fatty acids or hydrocarbons as electron donor and that the experiment revealed that bacteria of the genus Archaeoglobus fulgidus DSM4139 will have an unexpectedly good performance for thermophilic microbial (Per)Chlorate Reduction in a hot hydrocarbon containing formation at an ambient temperature of at least 60 C.
EXAMPLE
A suitable embodiment of the method according to the invention, comprises the following steps:
a)Screening whether a target underground crude oil and/or natural gas containing reservoir formation has features, such as temperature, salinity, heterogeneity, oil characteristics, micro-organisms, volatile fatty acids, hydrogen ions, acetate, propionate or butyrate and/or other potential electron donors, etc., which allow use of the method according to the invention;
- 10 -b)Analyzing the composition of the water, oil and/or natural gas in the formation, for example by screening a sample taken from the formation;
c)Identification of potentially interesting micro-organisms with molecular DNA technologies using either general (16S rRNA-related) primer sets or enzyme/functional group specific primer sets (nitrate/nitrite-reductase, (per)chlorate reductases, chlorite dismutase, or hyrdrocarbon (alkane) degrading enzymes or using metagenomics;
d)Isolation of potentially interesting indigenous microbes from available core, formation water, and oil samples using VFA's (acetate, proprionate, butyrate,etc.), hydrocarbon components (e.g. long chain alkanes) or typical gas contaminants (e.g. H2S) as electron donor and nitrate, oxygen or perchlorate, chlorate or chlorite as electron acceptor.
e)Determination of the optimal nutrient mix (electron donor, N/P nutrient, trace elements, SRB-inhibiting chemicals, etc.) using the identified and/or cultivated micro-organisms;
f)Microbial incubations using the potential successful nutrient compositions and gas contaminants, VFA's or oil components (e.g. long chain alkanes) to prove microbial activity on lab scale;
g)Optional middle phase could be to verify chance of success by core flood experiments; and e)The following actual chemical injection and in-situ conversion procedure:
el) Shut-in and clean-up of a near wellbore area of the crude oil, tar sand, shale oil, natural gas and/or other hydrocarbon containing reservoir formation (either chemically or by flushing);
c)Identification of potentially interesting micro-organisms with molecular DNA technologies using either general (16S rRNA-related) primer sets or enzyme/functional group specific primer sets (nitrate/nitrite-reductase, (per)chlorate reductases, chlorite dismutase, or hyrdrocarbon (alkane) degrading enzymes or using metagenomics;
d)Isolation of potentially interesting indigenous microbes from available core, formation water, and oil samples using VFA's (acetate, proprionate, butyrate,etc.), hydrocarbon components (e.g. long chain alkanes) or typical gas contaminants (e.g. H2S) as electron donor and nitrate, oxygen or perchlorate, chlorate or chlorite as electron acceptor.
e)Determination of the optimal nutrient mix (electron donor, N/P nutrient, trace elements, SRB-inhibiting chemicals, etc.) using the identified and/or cultivated micro-organisms;
f)Microbial incubations using the potential successful nutrient compositions and gas contaminants, VFA's or oil components (e.g. long chain alkanes) to prove microbial activity on lab scale;
g)Optional middle phase could be to verify chance of success by core flood experiments; and e)The following actual chemical injection and in-situ conversion procedure:
el) Shut-in and clean-up of a near wellbore area of the crude oil, tar sand, shale oil, natural gas and/or other hydrocarbon containing reservoir formation (either chemically or by flushing);
- 11 -e2)Injection of microbial cultures (single species or consortia derived from enrichments inoculated with production fluids from the treated reservoir) into the formation to boost the required indigenous microbial species;
e3) Injection of optimized nutrient mixture (main components being: oxygen, perchlorate and or chlorate and/or nitrate possibly continuously but more likely push-wise to avoid the development of a chlorate-utilizing biofilm limited to the wellbore to ensure deep placement into the reservoir formation and thereby stimulating the required indigenous microbial community;
and e4) Monitoring of the in-situ conversion method according to the invention based on increase in oil production, change in water-cut, change in produced oil and/or natural characteristics and/or composition, detection of target micro-organism(s) using molecular DNA technologies and/or cultivation dependent screening.
e3) Injection of optimized nutrient mixture (main components being: oxygen, perchlorate and or chlorate and/or nitrate possibly continuously but more likely push-wise to avoid the development of a chlorate-utilizing biofilm limited to the wellbore to ensure deep placement into the reservoir formation and thereby stimulating the required indigenous microbial community;
and e4) Monitoring of the in-situ conversion method according to the invention based on increase in oil production, change in water-cut, change in produced oil and/or natural characteristics and/or composition, detection of target micro-organism(s) using molecular DNA technologies and/or cultivation dependent screening.
Claims (23)
1. A method for in-situ oxygen generation in an underground hydrocarbon containing formation, the method comprising injecting into the formation an oxygen generating composition which releases oxygen (O2) by reduction of chlorate (ClO3-), wherein:
- the formation has a temperature of at least 60°C;
- the composition comprises thermophilic chlorate reducing micro-organisms which multiply at an ambient temperature of at least 60° C; and - the multiplied thermophilic chlorate reducing micro-organisms convert the hydrocarbons and/or other pore fluids in-situ into transportable or disposable products, wherein the thermophilic chlorate reducing micro-organisms comprise bacteria of the genus Archaeoglobus, Geobacillus and/or Thermus, which use hydrogen (H) and electrons(e) provided by hydrocarbons, volatile fatty acids and/or other pore fluids in the formation followed by dismutation of chlorite(01O2-) by the micro-organisms on the basis of the reactions:
ClO3- + 2H+ +2e .fwdarw. ClO2- +H2O
ClO2- .fwdarw. Cl- +O2 .
- the formation has a temperature of at least 60°C;
- the composition comprises thermophilic chlorate reducing micro-organisms which multiply at an ambient temperature of at least 60° C; and - the multiplied thermophilic chlorate reducing micro-organisms convert the hydrocarbons and/or other pore fluids in-situ into transportable or disposable products, wherein the thermophilic chlorate reducing micro-organisms comprise bacteria of the genus Archaeoglobus, Geobacillus and/or Thermus, which use hydrogen (H) and electrons(e) provided by hydrocarbons, volatile fatty acids and/or other pore fluids in the formation followed by dismutation of chlorite(01O2-) by the micro-organisms on the basis of the reactions:
ClO3- + 2H+ +2e .fwdarw. ClO2- +H2O
ClO2- .fwdarw. Cl- +O2 .
2. The method of claim 1, wherein the thermophilic chlorate reducing micro-organisms multiply at an ambient temperature of at least 80°C and comprise bacteria of the species Archaeoglobus fulgidis.
3. The method of claim 1 or 2, wherein the oxygen generating composition comprises perchlorate (ClO4) from which chlorate is generated using electrons released by the volatile fatty acids, hydrocarbons or other pore fluid components as electron donor on the basis of the following reaction:
ClO4- + 2H+ + 2e -> ClO3- + H2O.
ClO4- + 2H+ + 2e -> ClO3- + H2O.
4. The method of claim 3, wherein the hydrocarbons comprise at least one of viscous crude oil and other long chain hydrocarbons and the oxygen generating composition comprises crude oil degrading aerobic bacteria.
5. The method of claim 4, wherein the crude oil degrading aerobic bacteria are at least one of the genus Geobacillus or Thermus, the crude oil degrading aerobic bacteria being indigenous to the formation or introduced by injection.
6. The method of claim 3, wherein the multiplied bacteria dissociate crude oil from the formation by microbial dismutation of chlorite for the partial biotic and abiotic aerobic conversion of oil.
7. The method of claim 3 or 4, wherein the multiplied bacteria dissociate viscous crude oil from the formation by microbial dismutation of chlorite for the partial biotic and abiotic aerobic conversion of oil and the method is used to enhance crude oil recovery from the formation.
8. The method of claim 1, wherein the other pore fluids comprise natural gas contaminants and the micro-organisms comprise bacteria of the genus Sulfolobus, Ferroglobus, Thiobacillus, Thiomicrospira or other genera able to convert natural gas contaminants.
9. The method of claim 8, wherein the natural gas contaminant is at least one of CO2 and H2S.
10. The method of claim 8 or 9, wherein the formation comprises a H2S containing pollutant from which the oxygen generates more oxidized sulfur compounds.
11. The method of claim 10, wherein the oxidized sulfur compounds are elemental sulfur, poly sulfide, poly thionates, H2SO4, or combinations thereof.
12. The method of claim 1, wherein the other pore fluid components comprise at least one of hydrogen ions, acetate, propionate or butyrate and other volatile fatty acids.
13. The method of claim 1, wherein the injected chemical comprises at least one of perchlorate, chlorate and chlorite and another chemical, which can serve as electron acceptor or oxygen source in order to ensure deep placement of the at least one of perchlorate, chlorate and chlorite into the formation.
14. The method of any one of claims 10 to 13, wherein the composition is injected either continuously or pulse-wise into the formation to ensure deep placement of nitrate, nitrite, oxygen, perchlorate, chlorate or alternative electron acceptors into the formation.
15. The method of claim 1, wherein the micro-organisms comprise a single species microorganism or a mixture and/or consortia of micro-organisms.
16. The method of claim 1, wherein the micro-organisms are after a period of time substituted by single or multiple enzyme samples that can be water soluble or added as immobilized structures.
17. The method of claim 1, wherein the micro-organisms are introduced into the formation as highly active microbes.
18. The method of claim 1, wherein the micro-organisms are introduced into the formation as spores, cysts or encapsulated micro-organisms.
19. The method of claim 16, wherein the immobilized structures are bio-nano particles.
20. The method of claim 1, wherein the micro-organisms perform the microbial conversion of perchlorate via chlorate and chlorite to chloride and oxygen.
21. The method of claim 1, wherein the micro-organisms comprise both the perchlorate/chlorate/chlorite as well as the hydrocarbon conversion/natural gas contaminant conversion activity.
22. The method of claim 1, wherein the micro-organisms contain key enzymes from a nitrate-reduction and/or chlorate-reduction pathway.
23. The method of claim 22, wherein the key enzymes are perchlorate reductase, chlorate reductase, chlorite dismutase, nitrate reductase or combinations thereof.
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US20150075776A1 (en) * | 2013-07-24 | 2015-03-19 | D. Jack Adams | Optimization of biogenic methane production from hydrocarbon sources |
WO2016040844A1 (en) * | 2014-09-12 | 2016-03-17 | The Regents Of The University Of California | Specific inhibitors of (per)chlorate respiration as a means to enhance the effectiveness of (per)chlorate as a souring control mechanism in oil reservoirs |
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US5753122A (en) * | 1995-08-15 | 1998-05-19 | The Regents Of The University Of California | In situ thermally enhanced biodegradation of petroleum fuel hydrocarbons and halogenated organic solvents |
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