WO2018102070A2 - Bioélectrosynthèse de composés organiques - Google Patents

Bioélectrosynthèse de composés organiques Download PDF

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WO2018102070A2
WO2018102070A2 PCT/US2017/059912 US2017059912W WO2018102070A2 WO 2018102070 A2 WO2018102070 A2 WO 2018102070A2 US 2017059912 W US2017059912 W US 2017059912W WO 2018102070 A2 WO2018102070 A2 WO 2018102070A2
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microbial population
carbon
cathode chamber
cathode
organic compounds
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WO2018102070A3 (fr
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Harold D. May
Edward V. LABELLE
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MUSC Foundation for Research and Development
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MUSC Foundation for Research and Development
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    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12N—MICROORGANISMS OR ENZYMES; COMPOSITIONS THEREOF; PROPAGATING, PRESERVING, OR MAINTAINING MICROORGANISMS; MUTATION OR GENETIC ENGINEERING; CULTURE MEDIA
    • C12N1/00—Microorganisms; Compositions thereof; Processes of propagating, maintaining or preserving microorganisms or compositions thereof; Processes of preparing or isolating a composition containing a microorganism; Culture media therefor
    • C12N1/20—Bacteria; Culture media therefor
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12N—MICROORGANISMS OR ENZYMES; COMPOSITIONS THEREOF; PROPAGATING, PRESERVING, OR MAINTAINING MICROORGANISMS; MUTATION OR GENETIC ENGINEERING; CULTURE MEDIA
    • C12N1/00—Microorganisms; Compositions thereof; Processes of propagating, maintaining or preserving microorganisms or compositions thereof; Processes of preparing or isolating a composition containing a microorganism; Culture media therefor
    • C12N1/36—Adaptation or attenuation of cells
    • 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
    • C12P7/00—Preparation of oxygen-containing organic compounds
    • C12P7/40—Preparation of oxygen-containing organic compounds containing a carboxyl group including Peroxycarboxylic acids
    • C12P7/54—Acetic acid
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B3/00—Electrolytic production of organic compounds
    • C25B3/01—Products
    • C25B3/07—Oxygen containing compounds
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B3/00—Electrolytic production of organic compounds
    • C25B3/20—Processes
    • C25B3/25—Reduction
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel

Definitions

  • the present invention relates generally to the fields of electrochemical synthesis and microbiology. More particularly, it concerns methods for producing organic compounds, such as acetate, by bioelectric synthesis.
  • a method for bioelectric synthesis of H2 and organic compounds comprising: (a) culturing a microbial population in a media in a cathode chamber of an electrochemical cell; (b) maintaining the microbial population in the cathode chamber in the presence of: (i) constant current of between 0.1 and 100 A per liter (or between 0.1 and 50 A or 1 and 50 A per liter) of cathode chamber volume; (ii) CO2 gas; and (iii) a flow of media nutrients, thereby producing organic compounds; and (c) collecting the produced organic compounds.
  • maintaining the microbial population may be in the presence of between 1 and 20 A per liter of cathode chamber volume.
  • maintaining the microbial population may be in the presence of between 3 and 15 A per liter of cathode chamber volume.
  • maintaining the microbial population may be in the presence of a constant current for at least 10, 20, 30, 40, 50, 60, 120 or 180 days. In some specific aspects, maintaining the microbial population is in the presence of a constant current for 60 to 180 days. In additional aspects, the constant flow of media nutrients may be filtered to maintain the cells of the microbial population in the cathode chamber.
  • an electrochemical cell of the embodiments comprises a probe for measuring pH (e.g. , in the cathode chamber).
  • the media in the cathode chamber comprises a pH buffer system.
  • the pH buffer system is a phosphate or carbonate buffer system.
  • the method additionally comprises maintaining the media in the cathode chamber in a constant pH range, such as a pH of between 8.0 and 4.5 or between 6.0 and 4.5. In certain aspects, the constant pH range is maintained by an automated system.
  • the flow of media nutrients is constant. In other aspects, the flow of media nutrients is intermittent.
  • the cathode chamber may be flushed with CO2 or supplied with bicarbonate periodically. In more specific aspects, the cathode chamber is flushed with CO2 or supplied with bicarbonate on average every 3 to 10 days. In a certain aspect, the cathode chamber is supplied with a continuous in flow of CO2 or bicarbonate.
  • the CO2 is obtained from waste gas or captured from the anaerobic digestion of waste.
  • the produced organic compounds are removed periodically (e.g., hourly, daily, every two days, every three days or weekly) or continuously.
  • waste products in the media are removed periodically (e.g., hourly, daily, every two days, every three days or weekly) or continuously.
  • cathode chamber may be maintained at a temperature of between 15 and 40 °C. More specifically, the cathode chamber may be maintained at a temperature of between 20 and 30 °C.
  • the microbial population may comprise bacteria from at least two, three or four families selected from the group consisting of Eubaceriaceae, Campy lobacteraceae, Helicobacteraceae, Porphyromonadaceae, WCHBl-69, Spirochaetaceae, Deferribacteraceae, Rhodobacteraceae, Synergistaceae and Rhodocyclaceae.
  • the microbial population comprises two or more different species of bacteria.
  • the microbial population is essentially a pure culture of one species of bacteria.
  • the microbial population comprises Bacteria from the Helicobacteraceae, WCHBl-69, Spirochaetaceae, or Synergistaceae families.
  • the microbial population may comprise bacteria from the genus Acetobacterium, Sulfur ospirillum, Wolinella, Paludibacter, Spirochaeta, Geovibrio, Desulfovibrio or Azovibrio.
  • the microbial population comprises bacteria from the genera Acetobacterium, Sulfur ospirillum and/or, optionally, from the family Rhodobacteraceae.
  • the microbial population comprises Acetobacterium woodii, Acetobacterium weiringae, Sporomusa ovata, Clostridium ljugdahlii, Clostridium carboxydivorans, Clostridium autoethanogenum or a mixture thereof.
  • the microbial population comprises Acetobacterium sp., Sulfurospirillum sp., and Desulfovibrio sp.
  • the microbial population comprises the Electrobiome® mixture (see, Marshall et al, 2017, incorporated herein by reference). More specifically, the microbial population may comprise at least 85% Acetobacterium sp.
  • the microbial population comprises Acetobacterium woodii, Acetobacterium weiringae, Sporomusa ovata, Clostridium ljugdahlii, Clostridium autoethanogenum, Clostridium carboxydivorans either as an essentially pure culture or as mixture of two or more of these organisms.
  • the method does not involve the addition of compounds that inhibit methanogenic organisms.
  • the microbial population may be essentially free of methanogenic organisms.
  • a method of the embodiments uses a growth media that does not comprise yeast extract and/or does not comprise a reducing agent.
  • the media can be essentially free of methyl reductase inhibitors, such as 2-bromoethanesulfonic acid (BESA) or 2-chloroethanesulfonic acid (CESA).
  • the cathode may comprise reticulated vitreous carbon (RVC), carbon paper, carbon cloth, carbon felt, carbon wool, carbon foam, graphite, porous graphite, graphite powder, graphene, carbon nanotubes, electrospun carbon fibers, carbon coated stainless steel mesh, a conductive polymer, platinum, palladium, titanium, gold, silver, nickel, copper (e.g., copper foam or copper wool), tin, iron, cobalt, tungsten, stainless steel (e.g., steel foam or steal wool), and combinations thereof.
  • the cathode comprises RVC and the RVC may be coated with carbon nanotubes.
  • the cathode may be a porous material.
  • the cathode may comprise 10 to 1000 pores per inch (ppi).
  • the cathode comprises RVC having 10 to 100 or 10 to 200 pores per inch (ppi).
  • the electrochemical cell comprises an anode composed of carbon paper, carbon cloth, carbon felt, carbon wool, carbon foam, graphite, porous graphite, graphite powder, graphene, carbon nanotubes, electrically conductive woven fabric, electrospun carbon fibers, a conductive polymer, platinum, palladium, titanium, gold, silver, nickel, copper, tin, iron, cobalt, cobalt phosphate, tungsten, stainless steel, coated titanium, a mixed metal oxide or a combination thereof.
  • the anode may be an electrically conductive woven fabric.
  • the electrically conductive woven fabric comprises polydimethyl siloxane hollow fiber membranes and carbon fiber.
  • the anode is a coated titanium anode.
  • the anode may be coated with a metal oxide or with IrC and/or Ta20s.
  • the organic compounds may comprise acetate, butyrate, isobutyrate, propionate, 3-hydroxypropionate, 3-hydroxybutyrate, formate or an alcohol (e.g., ethanol).
  • the organic compound comprises ethanol and the culture media includes tungsten.
  • the method may further comprise contacting the microbial culture with a methyl reductase inhibitor, thereby selectively promoting acetate production.
  • the methyl reductase inhibitor is 2-bromoethanesulfonic acid (BESA) or 2-chloroethanesulfonic acid (CESA).
  • the method may be further defined as a method for electrosynthesis of polyhydroxyalkanoate (PHA) bioplastics and further comprising (d) mixing the collected H2 or organic compound with oxygen in a reaction chamber that comprises a second microbial population, thereby producing a PHA bioplastic.
  • the second microbial population may be a methanotroph or methanotrophic community.
  • the second microbial population is comprised in a nitrogen- or phosphate- limited environment.
  • the media at the cathode comprises a potassium phosphate buffer.
  • the PHA bioplastic comprises polyhydroxybutyrate.
  • the second microbial population may comprise Ralstonia eutropha, Escherichia coli, or Cupriavidus.
  • the second microbial population is an essentially pure culture of Ralstonia eutropha, Escherichia coli, or Cupriavidus.
  • the reaction chamber that comprises the second microbial population may be directly connected to the electrochemical cell via an anion exchange membrane.
  • the method further comprises isolating the PHA bioplastic from the cells of the second chamber.
  • a method of producing a greater than C5 hydrocarbon comprising providing acetate to a culture of algae, dinoflagellate algae and/or Thraustochytrids capable of producing long-chain hydrocarbons and organic products, said acetate produced in an electroacetogenic bioreactor.
  • the acetate is produced by any of the embodiments or aspects described above.
  • a method comprises (a) generating acetate in a first reactor at a biocathode comprising an electroacetogenic microbial population at a cathode, CO2, and a voltage potential at the cathode to produce acetate; (b) providing the acetate produced into a second reactor containing the algae; and (c) allowing the algae to convert the acetate into the C5-C40 hydrocarbon or organic compound.
  • the method further comprises collecting and/or distilling the C5-C40 hydrocarbon from the second reactor.
  • the mixture further comprises a green microalga, such as a viable green microalga cell.
  • the mixture comprises trace amounts of acetate, such as at least 0.001, 0.01, 0.1 or even as much as 1%, 2%, 3%, 4% or 5% acetate.
  • the long-chain hydrocarbons in the mixture have a 14 C content not less than 10% of the 14 C content in atmospheric CC .
  • a second bioreactor of the embodiments comprises an organism, such as Crypthecodinium cohnii Chlamydomonas rheinhardtii Haematococcus pluvialis, Schizochytrium spp. or green microalga such as Botryococcus braunii.
  • an acetate source such as an algae can produce long-chain hydrocarbons greater than Cs, such as C5-C40 hydrocarbons, C20-C40 hydrocarbon or C23-C33 hydrocarbons.
  • the long-chain hydrocarbons produced are defined as a fuel.
  • algal culture produces an amount of hydrocarbon greater than 4, 5, 6, 7 or 8 gfuel/L (e.g., greater than 10 gfuel/L).
  • the rate of fuel production is about or greater than about 0.75 or 1.0 gfuel/gcdw/hr.
  • the algal culture the second bioreactor has a reaction energy efficiency of greater than 50%, 55%, 60%, 65%, 70%, 75%, 80% or 85%.
  • an algal culture has an average carbon yield from acetate of about or greater than about 50%, 55%, 60%, or 65% (e.g., such as about 67%).
  • methods concern providing acetate into a second reactor.
  • acetate can be provided by diffusion.
  • the first and second bioreactors may be separated by a membrane that allows acetate molecules to diffuse in the second reactor.
  • a diffusion membrane has a pore size that is sufficiently small to exclude long-chain hydrocarbons from diffusing into the first bioreactor.
  • a method of the embodiments comprises purification of organic compounds such as acetate from the culture system.
  • the purification may comprise by freeze concentration or electrodialysis.
  • the inorganic compounds are separated from the reactor (such as in an acetate production stream).
  • the inorganic compound can comprises struvite (IMI-U gPCU-ei-teO).
  • a method of the embodiments further comprises collecting a long-chain hydrocarbon from a second bioreactor.
  • collecting the hydrocarbon can comprise exposing the culture of the second reactor to a solvent, such as an organic solvent, to remove the hydrocarbon.
  • a solvent extracts greater than 50%, 60%, 70%, 80%, 90% or 95% of the hydrocarbon from the media.
  • a method comprises distilling the long chain hydrocarbons.
  • the hydrocarbons can be distilled to produce a diesel or gasoline composition.
  • organic compounds produced by the methods of the embodiments comprise omega 3 fatty acids, polyunsaturated fatty acids (PUFAs) or carotenoid compounds such as astaxanthin.
  • a microbial population for use according to the methods comprises at least a first acetogen.
  • an "acetogen” refers to a CO2 reducing acetogen microbe that uses the Acetyl CoA Pathway.
  • Acetogenic organisms are well recognized in the art see, e,g., Impkamp and Muller, "Acetogenic Bacteria” Encyclopedia of Life Sciences, 2007, incorporated herein by reference.
  • FIG. 1A-B A, Three dimensional rendering of the components of the bioelectrochemical reactor. This is also designed for modular construction.
  • B An example of a constructed continuous flow bioelectrochemical cell.
  • FIG. 2 ODeoonm of effluent from triplicate bioelectrochemical reactors.
  • FIG. 3 Growth of the Electrobiome on 45 ppi RVC. Left: uninoculated RVC.
  • FIG. 4 Space time yield for acetate in triplicate continuous flow/culture bioelectrochemical reactors.
  • FIG. 5 Hydrogen production by uninoculated electrochemical reactor.
  • FIG. 6 Coulombic efficiency of triplicate bioelectrochemical reactors.
  • FIG. 7 Energy efficiency of triplicate bioelectrochemical reactors.
  • FIG.9 Hydrogen production of an uninoculated abiotic reactor operated under the same conditions as biotic reactors.
  • FIG. 11A-H Further organic compound production systems of the embodiments. DESCRIPTION OF ILLUSTRATIVE EMBODIMENTS
  • Microbial electrosynthesis is a promising new technology that when developed could result in a sustainable supply of chemicals and fuels from renewable electricity and C02.
  • rates, yields, and efficiencies have been too low for commercial consideration.
  • Methods and systems disclosed herein provide for significantly enhanced synthesis of organic compounds such as acetate.
  • the bioreactors and methods provided here are designed for operation with the microbial community maintained in a two chamber electrochemical cell, and include one or more of the following features: 1) maintenance under Galvanostatic (constant current) control; 2) a continuous supply of nutrients, water, and CO2; 3) continuous removal of products and waste media; 4) on a reticulated vitreous carbon (RVC) foam cathode; and 5) with a mixed metal oxide (MMO) anode.
  • Galvanostatic control and the high surface area RVC reduces the electron limitation and the continuous flow eliminates the nutrient limitation and avoids the accumulation of toxic compounds.
  • a bioreactor which produces acetate and the produced acetate is supplied (e.g. , via diffusion) to a second reactor which comprises a microalga or other organism to process the acetate into long chain hydrocarbons.
  • the organisms in such a second bioreactor can utilize modified fatty acid biosynthetic pathways, which result in the production of a long chain hydrocarbon, such as omega 3 fatty acids and astaxanthin.
  • long chain hydrocarbons for production according to the instant embodiments has between 5 and 40 carbons.
  • Methods of the embodiments may also comprise purification (e.g., distillation) of long-chain hydrocarbon (e.g., for use as commercial fuel).
  • An autotrophic microbial community from brewery wastewater was selected on a cathode of a bioelectrochemical system.
  • Acetate was sustainably and reproducibly generated electrosynthetically using a cathode potential.
  • additional byproducts may also be produced by such a reactor, such as hydrogen.
  • Carbon dioxide is a substrate in the acetate production step while being a byproduct of the hydrocarbon producing step.
  • sustained rates of acetogenesis based on cathode volume surpassed what has thus far been discovered for electrosynthesis of these compounds by use of a constant current and constant flow of nutrients into the system. More details of such systems can be found in International Application WO 2014/043690 and in LaBelle and May 2017, each of which is incorporated herein by reference.
  • microbial communities are well known for the intricate interactions between microorganisms that frequently result in an efficient and productive process due to the natural selection of microorganisms that will operate in stable consortia. For example, when a potential of -590 mV was applied the result was a microbial community that would electrosynthesize acetate very efficiently.
  • a microbial population may be one of those described in PCT Application WO 2014/043690 and Marshall et al. 2017 each incorporated herein by reference.
  • Previous studies using a biocathode indicate that at least one member of the community will interact directly with the electrode. An Acetobacterium sp.
  • the other major active bacteria on the biocathode could include Sulfur ospir ilium and Rhodobacteraceae, consistent with the community in the original reactor generating acetate.
  • Sulfur ospir ilium and Rhodobacteraceae play despite their prevalence and continued presence in the biocathodes.
  • the reactor systems were operated in both the light and the dark, with no observable effect on current or product formation. Without being bound by theory, one possibility for the role of these two bacteria could be to draw electrons directly from the electrode and produce hydrogen.
  • the biocathode could contain other bacteria including Desulfovibrio.
  • Acetic acid is another valuable commodity chemical made from fossil fuels that is used in industrial processes to produce vinyl acetate for paints and adhesives (Cheung et al. 2005). Production for human consumption, e.g. food and cosmetics, requires a higher degree of purity, which is achieved by microbial fermentation of sugars to acetic acid (vinegar) (Drake et al. 2008; Parrondo et al. 2003). Acetate is also a key intermediate in the production of biofuels, as it has been shown to be a feedstock for a microbial community to produce ethanol in BESs using methyl viologen as an electron carrier (Steinbusch et al. 2010).
  • the carbon source for the process is plentiful and inexpensive, the electrons may be supplied from sustainable non-carbon based sources, land mass requirements are negligible and will not compete with food crop production, and being strictly carbon neutral electrosynthesis presents an attractive way to combat climate change.
  • Microbial electrosynthesis fixes carbon dioxide from electricity and microbial catalysts with a high Coulombic efficiency.
  • the fixed carbon products can be used as a feedstock in lieu of sugar, surpassing the efficiency of photosynthesis.
  • an algal culture such as culture comprising
  • the methods may incorporate a mutant with an optimized acetate feeding rate, medium composition, and/or temperature. In some embodiments, these mutants will have a cell growth and hydrocarbon secretion rate is expected to reach up to 1.2 h "1 . Additionally, in some embodiments, the microalga can be grown in the dark, which can stimulate growth (Tanoi, 2011). D. Hydrocarbons
  • alkane or “hydrocarbon” refers to the compound H-R, wherein R is alkyl as this term is defined above.
  • alkyl refers to a monovalent saturated aliphatic group with a carbon atom as the point of attachment, a linear or branched, cyclo, cyclic or acyclic structure, and no atoms other than carbon and hydrogen.
  • cycloalkyl is a subset of alkyl, with the carbon atom that forms the point of attachment also being a member of one or more non-aromatic ring structures wherein the cycloalkyl group consists of no atoms other than carbon and hydrogen.
  • the term does not preclude the presence of one or more alkyl groups (carbon number limitation permitting) attached to the ring or ring system.
  • the groups -CH 3 (Me), -CH2CH3 (Et), -CH2CH2CH3 (w-Pr or propyl), -CH(CH 3 ) 2 (z-Pr, Tr or isopropyl), -CH(CH 2 ) 2 (cyclopropyl), -CH2CH2CH2CH3 (w-Bu), -CH(CH 3 )CH 2 CH 3 (sec- butyl), -CH 2 CH(CH 3 )2 (isobutyl), -C(CH 3 ) 3 (fert-butyl, r-butyl, f-Bu or T3u), -CH 2 C(CH 3 ) 3 (weo-pentyl), cyclobutyl, cyclopentyl, cyclohexyl, and cyclohexylmethyl are non-limiting examples
  • a "long chain hydrocarbon” is a subset of “hydrocarbon” wherein the aliphatic group is a linear chain.
  • the following parenthetical subscripts further define the number of carbon atoms contained within that term as follows: "(Cn)” defines the exact number (n) of carbon atoms in the group/class. "(C ⁇ n)” defines the maximum number (n) of carbon atoms that can be in the group/class, with the minimum number as small as possible for the group in question.
  • alkyl(c ⁇ io) designates those alkyl groups having from 1 to 10 carbon atoms.
  • (Cn-n') defines both the minimum (n) and maximum number ( ⁇ ') of carbon atoms in the group.
  • alkyl(C2-io) designates those alkyl groups having from 2 to 10 carbon atoms.
  • Electrochemical Reactor The anode compartment consisted of a polypropylene spacer and a mixed metal oxide (Ir0 2 /Ta 2 05) catalyzed titanium anode (MMO) (Magneto, NL).
  • MMO mixed metal oxide
  • the cathode was a 45 ppi reticulated vitreous carbon foam (KR Reynolds Company, CA), 0.6x6x8 cm. It was pretreated in 2 N nitric acid and rinsed thoroughly with MilliQ water.
  • the catholyte was 50 mL of a phosphate-based medium described in LaBelle 2014. It contained salts, vitamins and trace metals and minerals. 50 mM NaCl was used instead of sodium bromoethanesulfonate. No yeast extract, sulfide or cysteine was used. The medium was filter sterilized and flowed through the reactors at 250 mL/day using a peristaltic pump and Pharmed BPT tubing.
  • the cells used to inoculate the reactors were obtained from an electroacetogenic reactor (LaBelle 2014). They were concentrated using tangential flow filtration using a 0.2 ⁇ poly ether sulfone filter, spun at 5000 (RCF) for 10 minutes and re-suspended in fresh medium.
  • the reactor was operated in constant current at 8 A/Lcathoiyte with current supplied from a VMP3 Potentiostat (Biologic) set in Galvanostatic mode and the voltage monitored by EC Lab software. 100% CC was passed through the headspace at an initially set rate of 25 mL/min. Medium was flowed though the reactor at a rate of 250 mL/day using a peristaltic pump.
  • VMP3 Potentiostat Biologic
  • Green microalga Botryococcus braunii
  • Botryococcus naturally secretes hydrocarbons outside the cell and stores hydrocarbons in the extracellular matrix where cells are connected to form colonies. The secreted hydrocarbons can be recovered through short contact with solvent. This process does not impair hydrocarbon yield of subsequent cultures, allowing continuous cultivation and milking of B. braunii for hydrocarbon production without major increase in cell biomass.
  • B. braunii To further increase cell yield and hydrocarbon production, B.
  • braunii mutants generated through chemical mutagenesis will be adapted and screened on the acetate-containing medium for mutants with improved phenotype.
  • Selected mutants will be grown in bioreactors and optimized for acetate feeding rate, medium composition, and temperature.
  • Cell growth and hydrocarbon secretion rate is expected to reach up to 1.2 h "1 .
  • a phosphate buffered medium and carbon dioxide is continuously flowed through a bioelectrochemical cell under a constant current.
  • the Electrobiome® or other acetogen(s) reside in the cathode compartment whereby the electrons and carbon dioxide are converted to acetate.
  • the bacterial cells are separated from the effluent to produce a cell-free acetate stream.
  • a stoichiometric amount of ammonium hydroxide matching the phosphate content is added to the acetate stream, the pH is raised to pH ⁇ 8-9, and a stoichiometric amount of a magnesium salt matching the phosphate is added and struvite is precipitated out and separated as a value added product (a slow release fertilizer).
  • the acetate stream is subjected to electrodialysis to generate concentrated acetic acid and a sodium hydroxide stream, the latter of which can be recycled into the struvite precipitation step.
  • a freeze concentration step can be performed before or after the electrodialysis step to achieve a desired strength of acetic acid.
  • the acetic acid is fed by a pH auxostat system along with the anodic oxygen (and air) to heterotrophic or mixotrophic algae (e.g.
  • a bicarbonate buffer is used with the Electrobiome® in place of the phosphate.
  • struvite production is avoided and the sodium hydroxide produced during electrodialysis is used to scrub carbon dioxide from the bioelectrochemical cell, purifying the hydrogen and regenerating the sodium bicarbonate buffer.
  • the scrubber could also remove carbon dioxide from the air, or from other process steps such as the heterotrophic algal production or the HTL step. See, FIG. 1 IB.
  • Electrobiome® is again operated with a phosphate buffer and acetate and struvite are produced as in example #1.
  • the acetic acid produced after electrodialysis is used to heterotrophically grow Haematococcus pluvialis, which is then exposed to stress by light, low nitrogen, or high concentrations of acetate from the Electrobiome® to induce the production of the highly valuable carotenoid, astaxanthin.
  • the latter is then extracted in dimethyl ether and the residual algal biomass plus Electrobiome® biomass is subjected to HTL and hydrotreatment to produce liquid fuels. See, FIG. l lC. D. Production of Astaxathin and Hydrocarbon Fuels from CO2 and Electricity.
  • the phosphate medium is replaced with a carbonate buffer, similar as done in B above, and struvite production is avoided.
  • Carbon dioxide is scrubbed while using sodium hydroxide produced during electrodialysis (as described in B).
  • Acetate is used to heterotrophically grow H. pluvialis and produce astaxanthin and fuels as described for C above. See. FIG. 11D.
  • the phosphate medium is once again used with the Electrobiome® so struvite is produced.
  • the acetic acid produced after electrodialysis is used to heterotrophically grow Crypthecodinium cohnii to produce omega 3 fatty acids (the acetic acid may also be supplied to the omega 3 producing thraustochytrid Schizochytrium).
  • the residual Electrobiome and algae biomass is used to produce liquid fuels. See, FIG. HE. F. Production of Omega 3 Fatty Acids and Hydrocarbon Fuels from CO2 and Electricity.
  • the carbonate based medium is used with the Electrobiome® and struvite production is avoided. Otherwise, the steps are as described in example #5 and omega 3 fatty acids and liquid hydrocarbon fuels are produced. See, FIG. 1 IF.
  • the phosphate based medium is used with the Electrobiome® to again produce acetate to grow algae heterotrophically (similar to A). Struvite is produced. However, the algae are saponified to carboxylates, which are then converted into hydrocarbons, fatty alcohols, and esters by Kolbe electrolsysis or the Hofer- Moest reaction. In addition to these products, NaHC03 is generated. Once again, the residual Electrobiome® and algal biomass is converted to liquid fuels by HTL and hydrotreatment. See, FIG. 11G.
  • the carbonate based medium is used with the Electrobiome® and the algae produced are saponified to carboxylates as described in G for Kolbe or Hofer-Moest conversion to hydrocarbons, fatty alcohols, and esters. Again, residual biomass is converted to liquid fuel by HTL. See, FIG. 11H.
  • Botryococcus braunii (Race A)," Eukaryotic Cell , 12: 1132-1141, 2013.

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Abstract

Selon certains aspects, la présente invention concerne un procédé de production bioélectrique de composés organiques tels que l'acétate. Selon d'autres aspects, la présente invention concerne également des procédés de production d'un combustible à base d'hydrocarbure au moyen de CO2 en tant que source de carbone.
PCT/US2017/059912 2016-11-03 2017-11-03 Bioélectrosynthèse de composés organiques Ceased WO2018102070A2 (fr)

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