WO2024008741A1 - Biosynthèse de méthane - Google Patents

Biosynthèse de méthane Download PDF

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Publication number
WO2024008741A1
WO2024008741A1 PCT/EP2023/068438 EP2023068438W WO2024008741A1 WO 2024008741 A1 WO2024008741 A1 WO 2024008741A1 EP 2023068438 W EP2023068438 W EP 2023068438W WO 2024008741 A1 WO2024008741 A1 WO 2024008741A1
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Prior art keywords
bioreactor
process according
hydrogen
reactor
microorganisms
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PCT/EP2023/068438
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English (en)
Inventor
Anker Jarl Jacobsen
Original Assignee
A J Inventing V/A Jarl Jacobsen
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Application filed by A J Inventing V/A Jarl Jacobsen filed Critical A J Inventing V/A Jarl Jacobsen
Publication of WO2024008741A1 publication Critical patent/WO2024008741A1/fr

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Classifications

    • 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
    • C12P5/00—Preparation of hydrocarbons or halogenated hydrocarbons
    • C12P5/02—Preparation of hydrocarbons or halogenated hydrocarbons acyclic
    • C12P5/023—Methane
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
    • C12M21/00—Bioreactors or fermenters specially adapted for specific uses
    • C12M21/04—Bioreactors or fermenters specially adapted for specific uses for producing gas, e.g. biogas
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
    • C12M23/00—Constructional details, e.g. recesses, hinges
    • C12M23/02—Form or structure of the vessel
    • C12M23/06—Tubular
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
    • C12M29/00—Means for introduction, extraction or recirculation of materials, e.g. pumps
    • C12M29/14—Pressurized fluid
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
    • C12M29/00—Means for introduction, extraction or recirculation of materials, e.g. pumps
    • C12M29/18—External loop; Means for reintroduction of fermented biomass or liquid percolate
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
    • C12M29/00—Means for introduction, extraction or recirculation of materials, e.g. pumps
    • C12M29/24—Recirculation of gas

Definitions

  • the present invention relates to the field of green technologies, to carbon capture and to the energy field.
  • the present invention relates to the bioindustrial manufacture of methane from carbon dioxide and hydrogen.
  • Methane-producing microorganisms are thought to be among the earliest cellular life forms colonizing our planet, and are major contributors to the past and present global carbon cycle.
  • methanogens belong to the archaeal domain of life, and they utilize a variety of methanogenic metabolisms among a wide distribution of archaeal phyla.
  • Hydrogenotrophic methanogens are archaea that can grow on hydrogen and carbon dioxide with the production of methane, an important intermediate in the global carbon cycle. They reduce carbon dioxide to methane and water by using hydrogen as an electron donor.
  • the acetoclastic methanogens use acetate as an electron acceptor while the methylotropic methanogens use methanol or methylamines as an electron acceptor.
  • the present invention provides a process for reacting hydrogen with carbon dioxide to form methane in an aqueous medium catalysed by microorganisms, where said reaction takes place inside a bioreactor, characterised in that the solubility of hydrogen in the aqueous medium is enhanced by pressure combined with a flow induced residence time enabling the dissolution and reaction of at least 80% of the gaseous hydrogen mixed with the aqueous medium.
  • the bioreactor is a U-shaped or coaxial vertical bioreactor.
  • the microorganisms are archaea, i.e. hydrogenotrophic methanogens.
  • the present invention provides a bioreactor fitted for implementing the process as defined in the first aspect of the invention.
  • the bioreactor is a U-shaped or coaxial vertical bioreactor.
  • FIG. 1 Coaxial vertical bioreactor for reacting hydrogen with carbon dioxide to form methane using microorganisms as catalysts.
  • a process for reacting hydrogen with carbon dioxide to form methane in an aqueous medium catalysed by microorganisms where said reaction takes place inside a bioreactor, characterised in that the solubility of hydrogen in the aqueous medium is enhanced by pressure combined with a flow induced residence time enabling the dissolution and reaction of at least 80% of the gaseous hydrogen mixed with the aqueous medium.
  • Microorganisms used for methane synthesis according to the present invention are so-called hydrogenotropic methanogens.
  • Hydrogenotropic methanogens derive metabolic energy from the reaction : Methanogens presently all belong to the archae bacteria and they are found ubiquitu- ous in nature and off course in anaerobic digesters where they often establish as mixed cultures in more or less equilibrium with the feed streams of the digester and its operating mode.
  • Non-limiting examples of hydrogenotropic methanogens are Methanopyrus kandleri, Mathanococcus maripaludis, Methanobacterium thermoautotrophium, Methanosarcina mazei, Methanospirillum hungatei, and Methanocella paludicola.
  • the process of the present operation is conducted using specific methanogenic bacteria as inoculum.
  • the bioreactor is inoculated with methanogenic bacteria obtained from an anaerobic digester, such as the anaerobic digester producing a biogas used as a source of carbon dioxide.
  • the process of the present invention is a continuous process where a microbial feed continuously is fed to the bioreactor, e.g. from an anerobic digester such as a municipal waste water treatment facility or an animal effluent processing facility.
  • the fluid exit stream from the bioreactor may be discarded or it may be wholly or partly recycled to the anaerobic digester wherefrom it came in the first instance.
  • the carbon dioxide can be supplied as pure carbon dioxide or as part of the exit gas from an industrial process.
  • the hydrogen gas may be supplied as pure gas from e.g. electrolysis, or supplied from the exit gas of an industrial process.
  • the carbon dioxide is fed to the bioreactor as part of a gas which is the biogas from an anaerobic digestion, e.g. having about 40% of carbon dioxide and 60% of methane, while the hydrogen gas is fed as a pure gas, e.g. 95-100% hydrogen.
  • the hydrogen gas may be prepared on-site by e.g. electrolysis.
  • the feed of hydrogen gas is regulated so as to match on a molar basis the feed of carbon dioxide in the biogas from an anerobic digestion.
  • this feed ratio is about 2.5 volumes of biogas per 1.0 volume of hydrogen gas.
  • the carbon dioxide and hydrogen fed to the bioreactor when supplied from two different gasses may either be mixed prior to being fed to the reactor or may be fed as separate gasses that are mixed inside the bioreactor.
  • the bioreactor used for the process converting carbon dioxide and hydrogen into methane may be a U-shaped or coaxial bioreactor or it may be a pressurized continuous stirred tank reactor.
  • the U-shaped or coaxial vertical bioreactor is a continuous bioreactor having the inlets for liquid substrate, microorganisms and gaseous substrates (carbon dioxide and hydrogen) in the first end of the bioreactor and the exit for spent liquid and reacted gasses at the second end of the bioreactor.
  • the U-shaped or coaxial vertical bioreactor has partial recycling of the exit gas from the bioreactor.
  • the amount of the exit gas being recycled may be about 25%, about 35%, about 50% or about 75%.
  • the amount of the exit gas being recycled to the bioreactor is from about 25% to 75%, from about 30% to 60%, from about 40% to about 50%.
  • the U-shaped or coaxial vertical bioreactor has partial recycling of the exit gas from the bioreactor, where the amount of gas being recycled is controlled in response to a measurement or estimation of the amount of carbon dioxide in the exit gas.
  • the height of the U-shaped or coaxial vertical bioreactor sets a minimum pressure that will be present at the bottom of the bioreactor where the part having downwards flow turns to the part having upward flow. For every 10 meters of bioreactor level (liquid height) the pressure is additionally approx. 1 bar as compared to the top of the bioreactor.
  • the U-shaped or coaxial bioreactor may also be pressurized at the inlet at the top, but if the reactor has a sufficient height it can have a sufficiently high hydrostatic pressure in the bottom part to quantitative drive the dissolution of gaseous hydrogen to dissolved hydrogen.
  • the solubility of hydrogen in water is much lower than the solubility of other gasses, such as oxygen, carbon dioxide (see Table 1). For instance, the solubility of hydrogen at 293 K is only 0.16 mg per 100 g of water, which amounts to 7% of the solubility of methane, and to 0.1% of the solubility of carbon dioxide.
  • solubility of gasses in water decreases with the temperature and since most hydrogenotropic methanogens are thermophiles, the solubility of hydrogen is very low and consequently the mass transfer of gaseous hydrogen to soluble hydrogen becomes the rate limiting step.
  • the U-shaped or coaxial vertical bioreactor may have any suitable shape as long as the unidirectional flow of the liquid and the gaseous phase are maintained.
  • the U-shaped or coaxial vertical bioreactor has a coaxial design, i.e. one vertical tubular structure placed inside a larger vertical structure having fluid and gaseous connection only in the bottom of the bioreactor.
  • the U-shaped or coaxial vertical bioreactor has the dimension of a pipe starting from the inlet end at the top, going vertically down to the buttom and turning up towards the exit also at the top, i.e. a U-shape.
  • the cross sectional area of the downward part of the bioreactor is the same as the cross sectional area of the upward part of the bioreactor.
  • the cross sectional area of the downward part of the bioreactor is smaller than the cross sectional area of the upward part of the bioreactor.
  • the bioreactor for implementing the process for reacting hydrogen with carbon dioxide to form methane may also be a continuous stirred tank reactor (CSTR) or a counterflow bioreactor which is pressurized.
  • CSTR continuous stirred tank reactor
  • counterflow bioreactor which is pressurized.
  • the counterflow bioreactor or CSTR is operated at a pressure of at least 2 bar, at least 3 bar, at least 6 bar or at least 10 bar.
  • the bioreactor is a counterflow bioreactor wherein the gaseous phase moves upwards and the aqueous phase moves downwards.
  • the bioreactor is a CSTR.
  • the CSTR reactor has a recirculation loop which recycles a part of the exit gas to the bioreactor.
  • the amount of the exit gas being recycled to the bioreactor is from about 25% to 75%, from about 30% to 60%, from about 40% to about 50%. In a further embodiment the amount of the exit gas being recycled is about 25%, about 35%, about 50% or about 75%.
  • the mean residence time of the liquid phase in the bioreactor is at least 10 seconds, at least 30 seconds, at least 1 minute, at least 5 minutes, at least 20 minutes, or at least 60 minutes.
  • the bioreactor according to item 14 wherein the inlet of aqueous medium comprising microorganisms and the inlet for hydrogen and carbon dioxide are both at the upper part of the bioreactor, whereby a downward flow mixes and transports the fluid and gas phases down past the buttom of the bioreactor and subsequently upward towards the outlet end of said bioreactor which is also at the upper part of the bioreactor.
  • said reactor is a continuously stirred tank reactor having a recirculating loop for recirculating at least part of the gaseous phase.
  • a U-shaped vertical bioreactor in the form of a tubular reactor having an inlet for liquid digestate obtained from a waste treatment facility containing hydrogenotropic methanogens, c.f. Figure 1 . Also at the inlet end of the bioreactor two separate gasses are fed into the digestate, the first gas supplying the hydrogen and the second gas supplying the carbon dioxide.
  • a counterflow bioreactor produces methane from a feed gas being made by mixing hydrogen with biogas from a waste treatment facility ( Figure 2).
  • the mixed inlet gas containing hydrogen and carbon dioxide is blown into a sparger ring at the buttom of the bioreactor and moving upwards through the liquid phase.
  • the liquid phase contains hydrogenotropic methanogens which catalyse the reaction forming methane.
  • the liquid phase moves downward against the flow of the gas phase, and at the bottom of the bioreactor the liquid phase is recirculated back to the top of the bioreactor.
  • the counterflow bioreactor is pressurized to enhance the rate of dissolution of the hydrogen gas into the aqueous phase.
  • the exit gas from the top of the bioreactor is a methane enriched biogas having a much lower carbon dioxide contents relative to the 40% CO2 in the biogas fed to the bioreactor. Also, the exit gas contains traces of remnant hydrogen.

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  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Wood Science & Technology (AREA)
  • Zoology (AREA)
  • Bioinformatics & Cheminformatics (AREA)
  • Genetics & Genomics (AREA)
  • General Health & Medical Sciences (AREA)
  • Microbiology (AREA)
  • Biochemistry (AREA)
  • Biotechnology (AREA)
  • General Engineering & Computer Science (AREA)
  • Biomedical Technology (AREA)
  • Sustainable Development (AREA)
  • Molecular Biology (AREA)
  • General Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Clinical Laboratory Science (AREA)
  • Preparation Of Compounds By Using Micro-Organisms (AREA)
  • Apparatus Associated With Microorganisms And Enzymes (AREA)

Abstract

La présente invention propose un procédé et un bioréacteur pour faire réagir l'hydrogène avec le dioxyde de carbone pour constituer du méthane dans un milieu aqueux catalysé par des micro-organismes, où ladite réaction a lieu à l'intérieur d'un bioréacteur, caractérisé en ce que la solubilité de l'hydrogène dans le milieu aqueux est renforcée par la pression combinée à un temps de séjour induit par le débit permettant la dissolution et la réaction d'au moins 80 % de l'hydrogène gazeux mélangé avec le milieu aqueux.
PCT/EP2023/068438 2022-07-04 2023-07-04 Biosynthèse de méthane WO2024008741A1 (fr)

Applications Claiming Priority (2)

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DKPA202270358 2022-07-04
DKPA202270358 2022-07-04

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2014060740A1 (fr) * 2012-10-15 2014-04-24 Perlemax Limited Génération de bulles pour éliminer des constituants d'un liquide
WO2018052295A1 (fr) * 2016-09-15 2018-03-22 Kwr Water B.V. Bioréacteur servant à la fermentation aérobie hydrogénotrophe
US20190352592A1 (en) * 2017-01-10 2019-11-21 Calysta, Inc. Gas-fed fermentation reactors, systems and processes utilizing a vertical flow zone
US20210087523A1 (en) * 2015-11-09 2021-03-25 Unibio A/S Fermentation tank with an inlet for injecting carbon dioxide

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2014060740A1 (fr) * 2012-10-15 2014-04-24 Perlemax Limited Génération de bulles pour éliminer des constituants d'un liquide
US20210087523A1 (en) * 2015-11-09 2021-03-25 Unibio A/S Fermentation tank with an inlet for injecting carbon dioxide
WO2018052295A1 (fr) * 2016-09-15 2018-03-22 Kwr Water B.V. Bioréacteur servant à la fermentation aérobie hydrogénotrophe
US20190352592A1 (en) * 2017-01-10 2019-11-21 Calysta, Inc. Gas-fed fermentation reactors, systems and processes utilizing a vertical flow zone

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
DAVIS RUSMANIS ET AL: "Biological hydrogen methanation systems - an overview of design and efficiency", BIOENGINEERED, vol. 10, no. 1, 1 January 2019 (2019-01-01), US, pages 604 - 634, XP055701670, ISSN: 2165-5979, DOI: 10.1080/21655979.2019.1684607 *
MATTHEW R. MARTIN ET AL: "A Single-Culture Bioprocess of Methanothermobacter thermautotrophicus to Upgrade Digester Biogas by CO2-to-CH4 Conversion with H2", ARCHAEA, vol. 74, no. 5, 1 January 2013 (2013-01-01), CA, pages 450 - 11, XP055264723, ISSN: 1472-3646, DOI: 10.1155/2013/157529 *

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