JP2020103277A - Use of oxyhydrogen microorganisms for non-photosynthetic carbon capture and conversion of inorganic and/or c1 carbon sources into useful organic compounds - Google Patents

Abstract

To provide compositions and methods for a hybrid biological and chemical process that captures and converts carbon dioxide and/or other forms of inorganic carbon and/or C1 carbon sources (including but not limited to carbon monoxide, methane, methanol, formate, or formic acid, for example) and/or mixtures containing C1 chemicals (including but not limited to various syngas compositions, for example) into organic chemicals (biofuels or other valuable biomass, chemical, industrial, or pharmaceutical products.SOLUTION: The present invention, in certain embodiments, fixes inorganic carbon or C1 carbon sources into longer carbon chain organic chemicals by utilizing microorganisms capable of performing the oxyhydrogen reaction and the autotrophic fixation of CO2 in one or more steps of the process.SELECTED DRAWING: None

Description

RELATED APPLICATION This application is entitled 2010 "Use of Oxyhydrogen Microorganisms for Recovery and Conversion of Non-Photosynthetic Carbon from Inorganic Carbon Sources to Useful Organic Compounds" under the provisions of 35 USC 119(e). Claim priority based on US Provisional Patent Application No. 61/328,184 filed April 27, 2014. The present application is also 2010 entitled "Biochemical Process Utilizing Chemoautotrophic Microorganisms for the Chemosynthetic Fixation of Carbon Dioxide and/or Other Inorganic Carbon Sources to Organic Compounds and Other Useful Products". It is a continuation-in-part of international patent application PCT/US2010/001402 filed on May 12, which states: "Chemical synthetic immobilization of carbon dioxide and/or other inorganic carbon sources to organic compounds and other useful products. Is a continuation-in-part of US patent application Ser. No. 12/613,550 filed Nov. 6, 2009 entitled “Biochemical Process Utilizing Chemoautotrophic Microorganisms for the Production of Biochemical Process Utilizing Chemoautotrophic Microorganisms for Carbon Cycle by Chemical Synthesis from Carbon and Other Inorganic Carbon Sources to Biofuels and Other Useful Products" US provisional patent filed on November 6, 2008 Claim benefit based on application No. 61/111,794. Each of these applications is incorporated herein by reference in its entirety for all purposes.

The present invention is directed to biofuels, bioremediation, carbon capture, carbon dioxide fueling, carbon cycling, carbon sequestration, energy storage, gas liquefaction, waste energy fueling, syngas conversion, and renewable/alternative energy and/or low carbon dioxide. It belongs to the technical field of carbon source energy. In particular, the present invention relates to carbon dioxide and/or other forms of inorganic carbon sources and/or other C1 carbon sources in non-photosynthetic processes powered by low carbon emission energy sources and/or waste energy sources. It is a unique example of the use of biocatalysts in biochemical processes to immobilize carbon dioxide into organic chemicals with longer carbon chains. In addition, the invention includes the production of chemical co-products that are co-fed with carbon fixation reaction steps and/or non-biological reaction steps as part of a total carbon recovery and conversion process or syngas conversion process. The present invention provides an effective and economical recovery of carbon dioxide from the atmosphere or from point sources of carbon dioxide to produce liquid fuels for transportation and/or other organic chemicals, as well as a waste energy source. And/or may enable economical use of renewable energy sources and/or low carbon emission energy sources. This will help address climate change caused by greenhouse gases and contribute to domestic production of renewable liquid fuels for transport and/or other organic chemicals that have no dependence on agriculture.

Renewable energy or waste in the conversion of carbon dioxide or other low value carbon sources into useful organic chemicals to provide alternatives to chemicals, materials and fuels derived from petroleum or other fossil sources Much attention and effort has been devoted to the development of energy-using technologies. In the field of CO ₂ conversion, much emphasis has been placed on photosynthetic-based biological methods to fix CO ₂ into biomass or final products, while at the same time being completely abiotic for fixing CO _2. Some efforts have also been made in various chemical processes.

Relatively types of CO ₂ organic chemicals technique that have not received the attention is a hybrid chemical / biological process. In this case, the biological process is limited to CO ₂ fixation, which corresponds to the dark reaction of photosynthesis. Potential advantages of such a hybrid CO ₂ organic chemistry process include CO ₂ fixation enzyme function acquired through billions of years of evolution and solar PV, solar heat, wind power, geothermal, The ability to power a process in combination with hydroelectric power, or a wide array of abiotic technologies such as nuclear power, is included. Microbes that perform carbon fixation without the use of light should be confined to a more controlled and protected environment that is less susceptible to water and nutrient loss, pollution, and meteorological hazards than those that can be used to culture photosynthetic microorganisms. Is possible. Furthermore, the increase in bioreactor capacity can be matched to vertical rather than horizontal configurations, which can lead to even better land use efficiency. A hybrid chemical/biological system offers the potential for a CO ₂ organic chemical process that retains the complex biological functions of organic synthesis from CO ₂ and avoids many of the disadvantages of photosynthesis. ..

A chemoautotrophic microorganism is generally a microorganism capable of CO ₂ fixation as in the photosynthetic dark reaction, but this microorganism can obtain a reducing equivalent required for CO ₂ fixation from an external source. Yes, there is no need to internally generate it via the photosynthetic light reaction. Carbon-fixing biochemical pathways carried out in chemoautotrophic organisms include the reductive tricarboxylic acid cycle, the Calvin-Benson-Bassham cycle, and the Wood-Ljungdahl pathway.

Prior studies are known for the specific application of chemoautotrophic microorganisms in the recovery and conversion of CO ₂ gas to fixed carbon. However, many of these have suffered from the drawbacks of limited effectiveness, economic feasibility, practicality, and commercialization of the described process. The present invention, in certain aspects, addresses one or more of the above-mentioned disadvantages.

The present invention, which utilizes oxyhydrogen microorganisms for the chemical synthesis immobilization of CO ₂ under carefully controlled oxygen levels, is believed to have advantages in producing long chain organic compounds (eg, C _{5 and} above). Energy densities (energy per unit volume) are generally high for long chain organic compounds, and compatibility with current transport is generally large compared to short chain products such as C1 and C2 products. Therefore, the ability to produce long chain organic compounds is an important advantage of the present invention.

In response to the need in the art of the present inventors to carry out the present invention, a long-chain organic compound from an inorganic carbon source and/or a C1 carbon source is used through the use of an oxyhydrogen microorganism for carbon recovery and fixation. A novel combined biochemical process for recovery and conversion into compounds, particularly organic compounds with chain lengths of C5 and above, is described. In some embodiments, the process comprises efficient production of high value organic compounds such as liquid hydrocarbon fuels, waste treatment of waste carbon sources, and even CO ₂ capture that can provide an additional source of income. It is possible to combine.

In one aspect, biochemical methods for the recovery and conversion of inorganic carbon compounds and/or organic compounds containing only one carbon atom into organic chemicals are described. In some embodiments, the method is capable of retaining an inorganic carbon compound and/or an organic compound containing only one carbon atom, and/or retaining an extract of an oxyhydrogen microorganism. Inorganic carbon through introduction into a simple environment and at least one chemically synthesized carbon fixation reaction utilizing a cell extract containing an oxyhydrogen microorganism and/or an enzyme derived from the oxyhydrogen microorganism in the environment. Converting a compound and/or an organic compound containing only one carbon atom into an organic chemical and/or a precursor thereof. In some embodiments, the chemosynthesis immobilization reaction is at least in part chemically and/or electrochemically generated and/or electrons introduced into the environment from at least one external source outside the environment. It is driven by the chemical and/or electrochemical energy provided by the donor and electron acceptor.

In one aspect, a bioreactor is described. The bioreactor, in one group of embodiments, comprises a first column comprising an upper portion and a lower portion, and a second column comprising an upper portion and a lower portion, the upper portion of the second column being Are fluidly connected to the upper part of the first column and the lower part of the second column is fluidly connected to the lower part of the first column. In some embodiments, the bioreactor has a substantially constant volume of gas at the top of the first column and/or the second column when liquid is circulated between the first and second columns. Is constructed and arranged to be In some embodiments, the volume of gas occupies at least about 2% of the total volume of the column in which it is located.

In another aspect, a method of operating a bioreactor is provided. The method, in some embodiments, comprises circulating a liquid containing growth medium between the first column and the second column, and in operation, the volume of gas is such that the first column and/or the second column. Is maintained substantially constantly at the top of the column and the volume of gas accounts for at least about 2% of the total volume of the column in which it is located.

In one aspect, an electrolysis device is provided. In some embodiments, the electrolyzer is a chamber constructed and arranged to electrolyze water to produce oxygen and hydrogen, and separate at least a portion of oxygen in the stream from at least a portion of hydrogen in the stream. And an outlet comprising a separator constructed and arranged to ensure that the hydrogen content of the fluid leaving the separator is suitable for use as a feed stream to a reactor containing a culture of oxyhydrogen microorganisms. And a part.

In another aspect, a method of operating an electrolyzer is described. The method comprises, in some embodiments, electrolyzing water to produce a first stream containing oxygen and hydrogen and separating at least a portion of the oxygen from at least a portion of the hydrogen to produce a first stream. Producing a second stream that is relatively rich in hydrogen as compared to (wherein the second stream is suitable as a feed stream to a reactor containing a culture of oxyhydrogen microorganisms). Including.

The present invention, in certain embodiments, is a biochemical process utilizing a cell extract containing obligate or facultative oxyhydrogen microorganisms and/or enzymes derived from oxyhydrogen microorganisms in one or more carbon fixation process steps. Compositions and methods for recovering carbon dioxide from a carbon dioxide-containing gas stream and/or atmospheric carbon dioxide or carbon dioxide in dissolved, liquefied, or chemically bound form via.

The present invention, in certain embodiments, provides C1 carbon sources (such as, but not limited to, carbon monoxide, methane, methanol, formate, or formic acid) and/or C1 chemicals. A mixture containing (eg, but not limited to, various syngas compositions produced from various fixed carbon feedstocks that have been gasified, pyrolyzed, or steam reformed) is utilized. Thus, compositions and methods for converting the C1 chemistry to long chain organic compounds are provided.

The present invention, in a particular embodiment, recovers an organic compound produced by immobilizing an inorganic carbon source and/or a C1 carbon source into a long-chain organic compound by a chemical synthesis reaction carried out by an oxyhydrogen microorganism, Compositions and methods for treatment and use are provided. The present invention, in certain embodiments, provides for the maintenance and control of oxygen levels in a carbon fixation environment for enhanced (eg, optimal) production of C5 and higher organic compound products via carbon fixation. Compositions and methods are provided. The present invention, in certain embodiments, provides for the production, processing, and delivery of chemonutrients required for carbon fixation and maintenance of oxyhydrogen microbial cultures (e.g., electron donors required for non-photosynthetic carbon fixation and Compositions and methods for (including but not limited to providing electron acceptors). The present invention, in certain embodiments, provides compositions and methods for maintaining an environment useful for carbon sequestration and recovery and recycling of unused chemo-nutrients and process water.

The present invention, in certain embodiments, is a chemical process step performed in series and/or in parallel with a chemosynthesis reaction step, ie, a crude input chemical that is more purified than is suitable to support a chemosynthesis carbon fixation step. To produce chemicals, to convert energy input into chemical forms that can be used to drive chemical synthesis, specifically to chemical energy in the form of electron donors and electron acceptors, industrial sources, atmospheric sources , Or directing the inorganic carbon recovered from aquatic sources to the carbon fixation step of the process under conditions suitable to support chemosynthetic carbon fixation by oxyhydrogen microorganisms or enzymes, and/or long chain organic chemicals C1 chemicals derived from low-value or waste carbon sources such as carbon monoxide, methane, methanol, formate, or formic acid, which can be used by oxyhydrogen microorganisms as a carbon source and optional energy source for synthesizing And/or mixtures containing C1 chemicals (eg, but not limited to, various syngas compositions derived from gasification, pyrolysis, or steam reforming of carbon sources of various low value or waste products. Process, process, net reduction of gaseous CO ₂ released into the atmosphere and/or upgrade of low value or waste materials to finished chemicals, fuels or nutrition To further process the output product of the carbon fixation process into a form suitable for storage, transportation, and sale, and/or safe disposal. .. The fully chemical process step combined with the chemically synthesized carbon fixation step constitutes the total carbon capture and conversion process according to some embodiments of the present invention.

One of the features of certain embodiments of the present invention is a living body for immobilizing carbon dioxide in a carbon dioxide-containing gas stream or in air or water and/or dissolved or solid form of inorganic carbon into organic compounds. Incorporating one or more process steps into a chemical process for the recovery of inorganic carbon and the conversion to a fixed carbon product utilizing an oxyhydrogen microorganism and/or an enzyme derived from an oxyhydrogen microorganism as a catalyst. .. In some such embodiments, carbon dioxide containing flue gas, or process gas, or air, or as dissolved carbon dioxide, carbonate, or bicarbonate ions in a solution, including an aqueous solution such as seawater. Inorganic carbon, or inorganic carbon in a solid phase, such as, but not limited to, carbonates and bicarbonates, is placed in a tank or closed container containing a nutrient medium and oxyhydrogen microorganisms. , Pumped or otherwise added. In some such cases, the oxyhydrogen microorganisms may have chemical energy stored in molecular hydrogen and/or valence or conduction electrons in the solid electrode material, and/or pumped or otherwise into the nutrient medium. Provided by the following electron donors: ammonia, ammonium, carbon monoxide, dithionite, elemental sulfur, hydrocarbons, metabisulfite, nitric oxide, nitrite, thiosulfate (eg , Sodium thiosulfate (Na ₂ S ₂ O ₃ ) or calcium thiosulfate (CaS ₂ O ₃ ), but not limited to these, sulfides such as hydrogen sulfide, and sulfites. , Thionates, thionite, transition metals or sulfides, oxides, chalcogenides, halides, hydroxides, oxyhydroxides, phosphates, sulphates of soluble or solid phase, or Chemical synthesis is carried out using one or more of carbonates (but not limited to these) to immobilize inorganic carbon into organic compounds. In some embodiments, it is possible to use conduction band or valence band electrons in the solid electrode material. The electron donor can be oxidized by the electron acceptor in a chemical synthesis reaction. Electron acceptors that can be used in the chemical synthesis reaction step include oxygen and/or other electron acceptors (eg, the following: carbon dioxide, ferric ions or other transition metal ions, nitrates, nitrites). , Sulfate, oxygen, or one or more of holes in the valence band or conduction band in the solid electrode material, but not limited thereto).

One of the features of certain embodiments of the present invention is due to the conversion of C1 chemicals to long chain organic chemicals (ie, C2 and above, and in some embodiments C5 and above carbon chain molecules). C1 carbon source (for example, carbon monoxide, methane, methanol, formate, or formic acid, which utilizes an oxyhydrogen microorganism and/or an enzyme derived from an oxyhydrogen microorganism as a biocatalyst of And/or mixtures containing C1 chemistry (eg, various syngas compositions produced from various fixed carbon feedstocks that have been gasified, pyrolyzed, or steam reformed, including, but not limited to, (But not limited to) incorporating one or more process steps into the chemical process. In some such embodiments, C1-containing syngas, or process gas, or C1 chemicals in pure liquid form or dissolved in a solution, is placed in a tank or closed container containing a nutrient medium and oxyhydrogen microorganisms. , Pumped or otherwise added. In some such cases, the oxyhydrogen microorganisms have chemical energy stored in C1 chemicals and/or molecular hydrogen, and/or valence or conduction electrons in the solid electrode material, and/or nutrient medium. Pumped or otherwise provided to the following electron donors: ammonia, ammonium, carbon monoxide, dithionite, elemental sulfur, hydrocarbons, metabisulfite, nitric oxide, Sulfates, such as, but not limited to, nitrates, thiosulfates (eg, but not limited to sodium thiosulfate (Na ₂ S ₂ O ₃ ) or calcium thiosulfate (CaS ₂ O ₃ ), hydrogen sulfide Such as sulfides, sulfites, thionates, thionite, transition metals in soluble phase or in solid phase or their sulfides, oxides, chalcogenides, halides, hydroxides, oxyhydroxides, sulfuric acid Organic chemicals with longer carbon chains, using one or more of salts or carbonates, including but not limited to biochemical synthesis to extend C1 chemicals To The electron donor can be oxidized by the electron acceptor in a chemical synthesis reaction. Electron acceptors that may be used in this reaction step include oxygen and/or other electron acceptors (e.g., carbon dioxide, ferric ions or other transition metal ions, nitrates, nitrites, Oxygen, or one or more of the holes in the solid electrode material, but not limited to these).

One or more chemical synthesis reaction steps of the process, wherein carbon dioxide and/or inorganic carbon is fixed to organic carbon in the form of organic compounds and biomass, and/or C1 chemicals (eg carbon monoxide, methane, Mixtures (including, but not limited to, methanol, formate, or formic acid) and/or C1 chemicals (eg, gasified, pyrolyzed, or steam modified various fixed carbons). Biochemically long-chain organic chemicals (ie, C2 or higher, in some embodiments C5 or higher, including but not limited to various syngas compositions produced from feedstocks). The reaction process for converting C1 chemicals into long-chain organic chemicals, which are converted into carbon chain molecules of Can be implemented in. A facultative environment is considered to have an aerobic upper layer and an anaerobic lower layer due to the stratification of the water column.

Oxygen levels are controlled in some embodiments of the invention such that the production of target organic compounds by oxyhydrogen microorganisms via carbon fixation is controlled (eg, optimized). One of the goals of controlling oxygen levels is to control (eg, optimize) intracellular adenosine triphosphate (ATP) concentration through cellular reduction of oxygen and production of ATP by oxidative phosphorylation, while at the same time. Keeping the environment sufficiently reducing so that a high ratio of NADH (or NADPH) to NAD (or NADP) is also retained.

The advantage of using oxyhydrogen microorganisms over absolutely anaerobic acetogenic or methanogenic microorganisms for carbon capture and/or syngas conversion applications is that the oxygen tolerance of oxyhydrogen microorganisms is higher. is there.

An additional advantage of using oxyhydrogen microorganisms over acetogenic bacteria for carbon capture and/or syngas conversion applications and/or biofuel production is due to the production of ATP powered by the oxyhydrogen reaction. Produce a water product that can be easily incorporated into the process stream, rather than the generally undesirable acid-producing acetic acid and butyric acid products that can harm microorganisms by lowering the solution pH or accumulating to toxic levels Is.

A further feature of certain embodiments of the invention is the electron donation used by oxyhydrogen microorganisms to immobilize carbon dioxide to organic compounds and/or to synthesize longer carbon chain organic molecules from C1 chemicals. Related to body source, production, or recirculation. Electron donors used for carbon dioxide capture and carbon fixation are, in certain embodiments of the invention, photovoltaic, solar, wind, hydroelectric, nuclear, geothermal, enhanced geothermal, ocean heat, wave power, tidal power. Generate or recycle electrochemically or thermochemically using power based on a wide variety of renewable energy technologies and/or low carbon emission energy technologies including, but not limited to. Is possible. The electron donor may also be of mineral origin, including but not limited to minerals containing reduced forms of S and Fe. The electron donors used in certain embodiments of the invention can also be produced or recycled via chemical reaction with hydrocarbons, which may or may not be non-renewable fossil fuels, provided that The chemical reaction shall produce little or no carbon dioxide gas emissions. For example, an oxide reduction reaction that produces a carbonate product and a hydrogen product that can be used as electron donors in a carbon fixation reaction step according to certain embodiments of the invention is
2CH ₄ +Fe ₂ O ₃ +3H ₂ O→2FeCO ₃ +7H ₂
And/or CH ₄ +CaO+2H ₂ O→CaCO ₃ +4H ₂
including.

Further features of certain embodiments of the invention relate to the formation and recovery of organic compounds and/or biomass from one or more chemically synthesized carbon fixation steps. These organic compounds and/or biomass products can have a variety of uses.

A further feature of certain embodiments of the invention is one or more oxyhydrogen microorganisms modified to produce superior amounts and/or qualities of organic compounds, biochemicals, or biomass via chemical synthesis. Relevant for use in multiple carbon fixation steps. The oxyhydrogen microorganisms used in these steps may be accelerated mutagenesis (eg, using ultraviolet light treatment or chemical treatment), genetic engineering or modification, hybridization, synthetic biology, or traditional selective breeding ( However, the present invention can be modified through artificial means including, but not limited to, these. Possible modifications of oxyhydrogen microorganisms include, as biofuels or feedstocks for producing biofuels (eg JP-8 jet fuel, diesel oil, gasoline, biodiesel oil, butanol, ethanol, hydrocarbons, methane, And pseudo vegetable oils, or any other hydrocarbon suitable for use as a renewable/alternative fuel resulting in reduced greenhouse gas emissions, including but not limited to) Examples include, but are not limited to, those directed to the production of controlled amounts and/or qualities of organic compounds and/or biomass.

Also described are compositions and methods that reduce the risk of conducting gas fermentation utilizing a mixture of hydrogen and oxygen in the process of the present invention.

Also, water is used as a hydrogen electron donor or hydride electron with improved efficiency over current state-of-the-art electrolysis for the purpose of producing hydrogen electron donors or hydride electron donors and oxygen electron acceptors. Also described are compositions and methods that take advantage of the oxygen tolerance of oxyhydrogen microorganisms and the ability to use oxygen as an electron acceptor to enable systems for conversion to donors and oxygen electron acceptors.

Also described are process steps for recovery and further finishing of useful chemicals produced in both the biological carbon fixation steps of the process as well as the non-biological process steps.

Other advantages and novel features of the invention will be apparent from the following detailed description of various embodiments of the invention, including but not limited to, when considered in conjunction with the accompanying drawings. Will be. All publications, patent applications, and patents mentioned in this text are incorporated by reference in their entirety. If the specification and the documents incorporated by reference include conflicting and/or conflicting disclosures, the present specification shall control.

Embodiments of the present invention are described by way of example, and not by way of limitation, with reference to the accompanying drawings, which are schematic and are not intended to be drawn to scale. For purposes of clarity, not all elements are shown in all figures, and where an exemplification is not necessary for one of ordinary skill in the art to understand the invention, the elements of each embodiment of the invention are Not all are displayed.

1 is a general process flow diagram of one embodiment of the present invention for a carbon capture and fixation process. Others of the invention with CO ₂ recovery performed by a microorganism (eg, a hydrogen-oxidizing purple non-sulfur bacterium) capable of undergoing an oxyhydrogen reaction to produce a lipid-rich biomass that is converted to JP-8 jet fuel. It is a process flow diagram of an embodiment. By utilizing the low solubility of hydrogen and oxygen gas in water, and by providing oxygen and hydrogen required for cell energy and carbon fixation to oxyhydrogen microorganisms, dangerous mixing of hydrogen and oxygen can be avoided. Fig. 2 is a schematic drawing of a simple bioreactor. The relatively high solubility of carbon dioxide and the carbon enrichment mechanism (CCM) are used to remove CO2 from a lean gas stream to remove CO2 from the lean gas mixture and separate it from low solubility gases such as oxygen and nitrogen. FIG. 3 is a design diagram of a bioreactor that takes advantage of the fact that oxyhydrogen microbes have a high ability to recover carbon. It is an electrolysis technique specifically designed to take advantage of the resistance and need of oxyhydrogen microorganisms to specific oxygen concentrations by reducing the complete separation of hydrogen and oxygen produced from standard electrolysis.

The present invention, in certain embodiments, involves a biochemical process utilizing cell extracts containing obligate or facultative oxyhydrogen microorganisms and/or enzymes derived from oxyhydrogen microorganisms in one or more process steps. Thus, compositions and methods for recovering and fixing carbon dioxide from carbon dioxide-containing gas streams and/or atmospheric carbon dioxide or carbon dioxide in liquefied or chemically bound form are provided. Further, fixation of CO ₂ and / or other C1 inorganic carbon source other than the carbon source is also described. Cell extracts include, but are not limited to, lysates, extracts, fractions or purified products exhibiting chemosynthetic enzyme activity that can be produced from oxyhydrogen microorganisms by standard methods. In addition, the invention, in certain embodiments, extends one or more chemical synthesis reaction steps and/or C1 molecules performed by an oxyhydrogen microorganism to immobilize inorganic carbon into an organic compound. Compositions and methods are provided for the recovery, treatment, and use of chemical products of one or more synthetic reaction steps performed by oxyhydrogen microorganisms to produce longer carbon chain organic chemicals. Finally, the present invention provides, in certain embodiments, chemonutrients required for chemoautotrophic carbon fixation by oxyhydrogen microorganisms, in particular molecular hydrogen and/or to drive carbon fixation reactions. Generation and processing of electron donors, including but not limited to electrical power, and electron acceptors, including but not limited to oxygen and carbon dioxide, and Compositions and methods for delivery, compositions and methods for maintaining an environment useful for carbon fixation by oxyhydrogen microorganisms, and removal of chemical products of chemosynthesis from an oxyhydrogen culture environment and unused portion of chemonutrients Compositions and methods for the recovery and recycling of

"Molecular hydrogen", the term "two hydrogen" and "H _2" are used interchangeably throughout.

The terms "oxyhydrogen microorganism" and "detonation microorganism" are used interchangeably throughout. The oxyhydrogen microorganisms are reviewed in Chapter 5, Section III of the present "Thermophilic Bacteria" by Jakob Kristjansson, CRC Press, 1992, which is hereby incorporated by reference. Generally, oxyhydrogen microorganisms are capable of performing an oxyhydrogen reaction. Oxyhydrogen microorganisms generally have the ability to utilize hydrogenase to utilize molecular hydrogen, with some of the electrons donated from H ₂ being NAD ⁺ (and/or other cellular). The remaining part of the electron is used for aerobic respiration. In addition, oxyhydrogen microorganisms are generally capable of autotrophically fixing CO ₂ via pathways such as the reverse Calvin cycle and the reverse citric acid cycle.

In addition, the terms "oxyhydrogen reaction" and "detonation reaction" are used synonymously throughout to mean the microbial oxidation of molecular hydrogen by molecular oxygen. The oxyhydrogen reaction is generally
Expressed as 2H ₂ +O ₂ →2H ₂ O+ energy and/or by the stoichiometric equivalent equation of this reaction.

Exemplary oxyhydrogen microorganisms that can be used in one or more process steps according to certain embodiments of the invention include the following: purple non-sulfur photosynthetic bacteria (eg, Rhodopseudomonas palustris). ), Rod Pseudomonas Kapusurata (Rhodopseudomonas capsulata), Rod Pseudomonas Biridisu (Rhodopseudomonas viridis), Rhodopseudomonas Sur Fobi Ridisu (Rhodopseudomonas sulfoviridis), Rod Pseudomonas Burasuchika (Rhodopseudomonas blastica), Rhodopseudomonas sphaeroides (Rhodopseudomonas spheroides), Rod Rhodopseudomonas acidophila, and other species of Rhodopseudomonas, Rhodospirillum rubrum, and other species of Rhodospirillum rubrum, and other non-genus Rhodospirillum rubrum, and other species of Rhodospirillum rubrum, and other species of Rhodospirillum rubrum, and other Rhodospirrum ), Rhodococcus opacus and other species of Rhodococcus, Rhizobium japonica and other rhizobium species of Rhizobium japonica, and other Rhizobium spp. genus (Thiocapsa) species, Pseudomonas Hidorogenobora (Pseudomonas hydrogenovora), species of Pseudomonas hydrogenoformans Terumo Philadelphia (Pseudomonas hydrogenothermophila), and the other of the genus Pseudomonas (Pseudomonas), Hidorogenomonasu pan Totoro file (Hydrogenomonas pantotropha), Hidorogenomonasu eutropha (Hydrogenomonas eutropha), Hydrogenomomonas facilis, and other species of the genus Hydrogenomonas. , Hydrogenogenobacter thermophilus and other species of Hydrogenogenobacter, Hydrogenovibrio marinos and other species of Hydrogenovirobriogeno, and other species of Hydrogenobirobiliogen (Hybrogenobiroen). Pylori) and other Helicobacter species, Xanthobacter species, Hydrogenogenophaga species, Bradyrhizobium japonicum and other Bradyrhizobium japonicum species. (Bradyrrhizobium) species, Ralstonia eutropha and other Ralstonia species, Alcaligenes eutrophus and other Alcaligenes vorax (Valixa paradoxus), ) And other species of the genus Variovorax, Acidovorax facilis and other species of the genus Acidovorax, cyanobacteria (eg, Anabena ocilarianaes, Anabaena naesanari, anaeroanades). -Anaena spiroides, Anabaena cylindrica, and other Anabaena species, including, but not limited to, green algae (e.g., Senedesmus oblius sususus senus (Scudenus esmunus senus)). ) And other species of the genus Scenedesmus, Chlamydomonas reinhardii and other species of the genus Chlamydomonas morphaeum, Anchistrodes phyllum, Ankistrodes phyllum, Ankystrodesphium. And others Rhaphidium spp., but is not limited to these), and further includes one or more of a consortium of microorganisms, including, but not limited to, oxyhydrogen microorganisms. Not a thing.

Various oxyhydrogen microorganisms that can be used in certain embodiments of the present invention include hydrothermal vents, geothermal vents, hot springs, cold seeps, subterranean aquifers, salt lakes, salt water formations, mines, acid mine drainage, mines. Tailings, oil wells, refinery wastewater, oil, gas or hydrocarbon contaminated water, coal seams, deep subterranean formations, wastewater and sewage treatment plants, geothermal power plants, sulfur pore areas, soils (for example contaminated with hydrocarbons). Soils and/or soils located under or around oil or gas wells, oil refineries, oil pipelines, gas stations, etc.). It can be native to the environment (but not limited to). They may or may not be extremophiles, including (but not limited to) thermophiles, hyperthermophiles, acidophilic bacteria, halophilic bacteria, and psychrophilic bacteria. Good.

In some embodiments, it is possible to produce relatively long chain chemical products. For example, the organic chemical produced in some embodiments is at least C5, at least C10, at least C15, at least C20, about C5 to about C30, about C10 to about C30, about C15 to about C30, or about C20 to. Compounds with a carbon chain length of about C30 may be included.

FIG. 1 illustrates process steps for producing an electron donor (eg, a molecular hydrogen electron donor) suitable for supporting chemical synthesis from energy input and crude inorganic chemical input, followed by chemical step from the electron donor generation step. The step of collecting the co-products, the generated electron donor, together with the oxygen electron acceptor, water, nutrients, and CO ₂ from the industrial flue gas point source, are used to collect and fix carbon dioxide using oxyhydrogen microorganisms. Delivering to one or more chemical synthesis reaction steps that produce chemical and biomass co-products via a chemical synthesis reaction, followed by a process step of recovering both chemical and biomass products from the process stream; and FIG. 3 shows a general process flow diagram of an embodiment of the invention with the step of recycling unused nutrients and process water as well as the cell mass needed to maintain microbial culture back to the carbon fixation reaction step. There is.

In the embodiment illustrated in FIG. 1, CO ₂ containing flue gases is recovered from a point source or emitter. The electron donors needed for chemical synthesis (eg, H2) can be generated from input inorganic chemicals and energy. Flue gas is pumped into a bioreactor containing oxyhydrogen microorganisms with electron donors and electron acceptors required to drive chemical synthesis and a suitable medium to support carbon fixation through microbial culture and chemical synthesis. It is possible. Cell cultures can flow into and out of the bioreactor continuously. After the cell culture leaves the bioreactor, the cell mass can be separated from the liquid medium. The cell mass needed to supplement the cell culture population at the desired (eg, optimal) level can be recycled back to the bioreactor. The excess cell mass can be dried to form a dry biomass product, which can be further post-processed into various chemicals, fuels, or nutrients. Following the cell separation step, extracellular chemical products of the chemosynthesis reaction can be removed from the process flow and recovered. Then, any unwanted waste products that may be present are removed. After this, the liquid medium and any unused nutrients can be recycled back to the bioreactor.

Many of the reduced inorganic chemicals (eg, H ₂ , H ₂ S, ferrous iron, ammonium, Mn ²⁺ ) that grow chemoautotrophic organisms are electrochemical and/or known in the chemical arts. It can be easily produced using thermochemical processes, which in some cases can be used for a variety of carbon dioxide-free or low carbon and/or carbon dioxide and low carbon emissions, including wind, hydro, nuclear, photovoltaic, or solar heat. Alternatively, power can be supplied by a renewable power source.

In certain embodiments of the invention, one or more of the following: photovoltaic, solar heat, wind power, hydroelectric power, nuclear power, geothermal, enhanced geothermal, ocean heat, wave power, tidal power, where Carbon dioxide-free or low carbon emissions and/or renewable power sources, including but not limited to, are used to generate electron donors. In certain embodiments of the present invention, the oxyhydrogen microorganisms acts as a carbon source, by using a CO ₂ recovered from the flue gas or from the atmosphere or ocean, renewable energy and / or low carbon emission energy or unsubstituted It acts as a biocatalyst for converting carbon emission energy into liquid hydrocarbon fuels or generally high energy density organic compounds. These embodiments of the present invention use a renewable energy source to produce hydrogen gas, which must be stored in a relatively heavy weight storage system (eg, tank or storage material). Or it could provide a renewable energy technology with the ability to produce transportation fuels with significantly higher energy densities even when used to charge batteries, which have a relatively low energy density. is there. In addition, liquid hydrocarbon fuel products according to certain embodiments of the invention may be more compatible with current transportation infrastructure as compared to battery or hydrogen energy storage options.

The location of one or more process steps that produce electron donors (eg, molecular hydrogen electron donors) in the general process flow of certain embodiments of the present invention is shown in Box 3 of FIG. "Body generation"). Electron donors produced in certain embodiments of the present invention using electrochemical and/or thermochemical processes known in the chemical arts and/or electron donors produced from natural sources include: Molecular hydrogen and/or valence or conduction electrons in solid electrode materials and/or the following: ammonia, ammonium, carbon monoxide, dithionite, elemental sulfur, hydrocarbons, metabisulfite, oxidation Sulfates such as nitrogen, nitrites, thiosulfates (including but not limited to sodium thiosulfate (Na ₂ S ₂ O ₃ ) or calcium thiosulfate (CaS ₂ O ₃ )). , Sulfides such as hydrogen sulfide, sulfites, thionates, thionites, transition metals in soluble phase or in solid phase or their sulfides, oxides, chalcogenides, halides, hydroxides, oxyhydroxides And other reducing agents including, but not limited to, one or more of compounds, sulfates, or carbonates, but not limited thereto.

In a particular embodiment of the invention, molecular hydrogen is used as the electron donor. Hydrogen electron donors include, but are not limited to, the following: proton exchange membranes (PEM), liquid electrolytes such as KOH, high pressure electrolysis, and high temperature electrolysis of steam (HTES). ) Water electrolysis; iron oxide cycle, cerium (IV) oxide-cerium (III) oxide cycle, zinc-zinc oxide cycle, sulfur-iodine cycle, copper-chlorine cycle, calcium-bromine-iron cycle, hybrid sulfur cycle ( Thermochemical decomposition of water via methods including, but not limited to; electrolysis of hydrogen sulfide; thermochemical and/or electrochemical decomposition of hydrogen sulfide; carbon capture and sequestration Methane reforming, coal gasification enabling carbon capture and sequestration, Kvaerner process and other processes to produce carbon black products, biomass gasification or pyrolysis enabling carbon capture and sequestration, and ferrous iron Oxidation of (Fe ²⁺ ) to ferric iron (Fe ³⁺ ) or oxidation of sulfur compounds (wherein the oxidized iron or sulfur is a metal sulfide, hydrogen sulfide, or hydrocarbon (but not limited to these) (But not limited to) can be recycled back to the reduced state via additional chemical reactions with minerals, including (but not limited to). Produce hydrogen with low or no carbon dioxide emissions, including but not limited to half-cell reduction of H ⁺ to H ₂ with half-cell oxidation of electron sources Is produced by methods known in the art of the chemical process industry including, but not limited to, one or more of the other electrochemical or thermochemical processes known to be. ..

In certain embodiments of the present invention, hydrogen electron donors are not necessarily produced with low carbon dioxide emissions or carbon dioxide free emissions, but hydrogen is used in municipal waste, black liquor, agricultural waste, wood waste. Feedstocks, including but not limited to foodstuffs, stranded natural gas, biogas, sour gas, methane hydrate, tires, sewage, fertilizers, straw, and low-value high-lignocellulosic biomass in general (but not limited to). Waste energy sources or low-value energy using methods known in the chemical process industry, including but not limited to gasification, pyrolysis, or steam reforming of Generated from source.

In certain embodiments of the invention utilizing molecular hydrogen as an electron donor for carbon fixation reactions performed by oxyhydrogen microorganisms, the production of molecular hydrogen using renewable and/or CO ₂ -free energy input. There are chemical co-products that are sometimes formed. When water is used as the hydrogen source, oxygen can be a co-product of water splitting through processes including but not limited to electrolysis or thermochemical water splitting. In certain embodiments of the invention using water as a hydrogen source, some of the oxygen co-products are oxyhydrocarbon fixed for the production of intracellular ATP via an oxyhydrogen reaction enzymatically related to oxidative phosphorylation. It can be used in the process. In certain embodiments of the invention, the oxygen produced by water splitting is in excess of that required to maintain favorable (eg, optimal) conditions for carbon fixation and organic compound production by oxyhydrogen microorganisms. It can be processed into a form suitable for sale through process steps known in the field of commercial oxygen gas production science and technology. In certain embodiments of the invention where hydrogen sulfide is the hydrogen source, sulfur or sulfuric acid may be a co-product of molecular hydrogen production. In certain embodiments of the invention where sulfuric acid is a co-product of hydrogen production, a portion of the sulfuric acid is available for hydrolysis of biomass in the process step after carbon fixation. In certain embodiments of the invention, excess co-produced sulfuric acid and/or sulfur (eg, above the amount otherwise available for carbon capture and conversion processes according to certain embodiments of the invention). Can be processed into a form suitable for sale via process steps known in the art of commercial sulfuric acid and/or sulfur production. Also, process heat may be generated when hydrogen is produced from hydrogen sulfide. In certain embodiments of the present invention, the process heat generated during hydrogen production is recovered and elsewhere to the carbon capture and conversion process according to certain embodiments of the present invention to improve overall energy efficiency. Used. Chemical co-products and/or heat co-products and/or electric co-products may, in certain embodiments of the invention, be associated with the production of molecular hydrogen for use as an electron donor. The chemical and/or heat and/or co-products of molecular hydrogen production can be otherwise subjected to carbon capture and conversion processes according to certain embodiments of the invention to improve efficiency. It can be used as long as possible. In certain embodiments, additional chemical co-products (eg, above the amount available for the carbon capture and conversion process according to certain embodiments of the invention) are sold to produce additional revenue streams. It can be prepared for use. Excessive heat co-products or electric energy co-products during the production of molecular hydrogen (eg, beyond the amount available within the process) can, for example, convert process heat to a form of salable electricity (but not Use in other chemical and/or biological processes via means known in the scientific and technological fields of heat exchange and heat transfer and electricity generation and transfer, including (but not limited to). It can be delivered for sale as soon as possible.

In certain embodiments of the present invention, electrochemical energy stored in solid valence or conduction electrons in electrodes or capacitors or related devices is used alone or as a chemical electron donor and/or electron. In combination with a carrier, a reducing equivalent for a carbon fixation reaction is utilized by utilizing the direct exposure of the electrode material to the microbial culture environment and/or the immersion of the electrode material in the microbial culture medium. To provide.

A feature of certain embodiments of the invention is that electron donors (eg, reduced forms) produced from mineral sources that are also usable by certain oxyhydrogen microorganisms as a source of reducing equivalents in addition to or instead of hydrogen are also available. , But not limited to, electron donors produced from S and Fe containing minerals). Thus, the present invention may, in certain embodiments, allow the use of an almost untapped energy source (inorganic geochemical energy).

The electron donors used in certain embodiments of the present invention include the following: elemental Fe ⁰ , siderite (FeCO ₃ ), magnetite (Fe ₃ O ₄ ), pyrite or marcasite (FeS ₂ ), Pyrrhotite (Fe _(1-x) S (x=0 to 0.2)), nickel iron sulfate (Fe,Ni) ₉ S ₈ , purple nickel ore (Ni ₂ FeS ₄ ), pyrite nickel ore (Ni , Fe) S ₂ , arsenopyrite (FeAsS), or other iron sulfides, poultry (AsS, ox (As ₂ S ₃ ), cobaltite (CoAsS), rhodomanganese (MnCO ₃ ), chalcopyrite (CuFeS). ₂ ), chalcocite (Cu ₅ FeS ₄ ), copper indigo (CuS), tetrahedrite (Cu ₈ Sb ₂ S ₇ ), arsenopyrite (Cu ₃ AsS ₄ ), arbohemite (Cu ₁₂ As _4. S ₁₃ ). , Chalcopyrite (Cu ₂ S), or other copper sulfide, sphalerite (ZnS), sphalerite (ZnS), or other zinc sulfide, galena (PbS), ammonite (Pb ₅ ( Sb, As ₂ )S ₈ ), or other lead sulfide, molybdenum or goethite (Ag ₂ S), molybdenite (MoS ₂ ), goethite ore (NiS), polydymite (Ni ₃ S ₄ ), Or other nickel sulfides, pyroxene ore (Sb ₂ S ₃ ), Ga ₂ S ₃ , CuSe, Cooper ore (PtS), laura ore (RuS ₂ ), Bragg ore (Pt, Pd, Ni)S, FeCl ₂ It can be purified from natural mineral sources including one or more of these (but not limited to).

The production of electron donors from natural mineral sources, in certain embodiments of the invention, involves atomizing, crushing, or pulverizing mineral ore with a device such as a ball mill to increase the leached surface area and to wet the mineral ore. A pretreatment step, which may include, but is not limited to, producing a slurry. In these embodiments of the invention where the electron donor is produced from a natural mineral source, flotation methods such as dissolved air flotation or foam flotation using a flotation tower or mechanical flotation tank, gravity separation, magnetic separation, Methods known in the art, including but not limited to heavy liquid separation, selective flocculation, water separation, or fractional distillation, are used to determine the presence of sulfides and/or other sulfides present in the ore. It may be advantageous if the particle size is controlled so that the reducing agent can be concentrated. After formation of the crushed ore or slurry, the particulate matter in the leachate or concentrate may be filtered (eg, vacuum filtered), sedimented, or otherwise known prior to introducing the electron donor-containing solution into the chemoautotrophic culture environment. It can be separated by the solid/liquid separation technology of. In addition, any leaching of mineral ores that is toxic to chemoautotrophic organisms can be removed prior to exposing the chemoautotrophic organism to the leachate. The solids remaining after processing of the mineral ore may be concentrated by filter press, disposed of, retained for further processing, or sold, depending on the mineral ore used in certain embodiments of the present invention.

Also, electron donors, in certain embodiments of the invention, are: process gas, tail gas, enhanced oil recovery vent gas, biogas, acidic mine drainage, landfill leachate, landfill gas, geothermal. Gas, geothermal sludge or brine, metal pollutants, gangue, tailings, sulphides, disulfides, mercaptans (eg but not limited to methyl mercaptan and dimethyl mercaptan, ethyl mercaptan) , Carbonyl sulfide, carbon disulfide, alkane sulfonate, sulfurized dialkyl, thiosulfate, thiofuran, thiocyanate, isothiocyanate, thiourea, thiol, thiophenol, thioether, thiophene, dibenzothiophene, tetrathionate, dithionite, thionate, disulfide One or more of dialkyl, sulfone, sulfoxide, sulfolane, sulfonic acid, dimethylsulfoniopropionate, sulfonate, hydrogen sulfide, sulfate ester, organic sulfur, sulfur dioxide, and all other sour gases, provided , But not limited to these) and pollutants or waste products.

In addition to the mineral source, the electron donor may, in certain embodiments of the invention, be a hydrocarbon that may be of fossil origin but that is used in a chemical reaction that results in low or no carbon dioxide gas emissions. Is produced or recycled through the chemical reaction of. These reactions include thermochemical and electrochemical processes. Such chemistries used in these embodiments of the present invention include thermochemical reduction of sulfate reactions or TSR and Muller-Kuhne reactions, iron oxides, calcium oxides, or magnesium oxides, including but not limited to: Methane reforming-like reactions that utilize metal oxides such as (but not those) instead of water (where hydrocarbons, along with hydrogen electron donor products, produce little or no carbon dioxide gas emissions. Reacting to form a solid carbonate), but is not limited thereto.

Examples of reactions between metal oxides and hydrocarbons to produce hydrogen electron donor products and carbonates include:
2CH ₄ +Fe ₂ O ₃ +3H ₂ O→2FeCO ₃ +7H ₂
And/or CH ₄ +CaO+2H ₂ O→CaCO ₃ +4H ₂
However, the present invention is not limited to these.

In certain embodiments, the electron donor produced is carbon dioxide, oxygen, and/or: ferric ion or other transition metal ion, nitrate, nitrite, sulfate, or solid electrode. One or more chemical synthesis reaction steps depending on the electron acceptor including, but not limited to, one or more of valence band holes or conduction band holes in the material. Is oxidized by.

The location of one or more chemical synthesis steps and/or oxyhydrogen reaction steps in the general process flow of certain embodiments of the present invention is shown in FIG. 1 labeled "Bioreactor-Detonation Microorganisms". Illustrated by Box 4.

At each step of the process in which chemical synthesis and/or oxyhydrogen reaction is performed, one or more types of electron donors and one or more types of electron acceptors are added to the nutrient medium containing oxyhydrogen microorganisms. Pumped or otherwise added to the reaction vessel either bolus addition or either periodically or continuously. Chemical synthesis reactions driven by the transfer of electrons from an electron donor to an electron acceptor can immobilize inorganic carbon dioxide into organic compounds and biomass.

In a particular embodiment of the invention, an electron carrier is incorporated into the nutrient medium to kinetically accelerate the chemosynthetic reaction process, from an electron donor to an oxyhydrogenate in the presence of an electron acceptor and inorganic carbon. It is possible to facilitate the delivery of reducing equivalents to. This aspect of the invention provides anthraquinone-2,6-disulfonate (AQDS), cobalt seprate, cytochrome, formate, humic, iron, methyl viologen, NAD+/NADH, neutral red (NR), phenazine, and An electron carrier known in the art of electrical stimulation of microbial metabolism, including, but not limited to, quinone, is used to generate electrons (but not these) in H ₂ gas or solid electrode materials. Can be used to facilitate the transfer of reducing electrons from poorly soluble electron donors (such as, but not limited to) to oxyhydrogen microorganisms.

Delivery of reducing equivalents from electron donors to oxyhydrogen microorganisms for one or more chemosynthesis reactions, in certain embodiments, hydrogen storage materials that may double as a solid carrier medium for microbial growth. Of the absorbed or adsorbed hydrogen electron donor in the vicinity of a hydrogen-oxidizing chemoautotrophic organism, and/or a solid carrier growth medium and an electron donor source or an electron acceptor source. Electrode material that can also have the function of (for example, graphite, graphite felt, activated carbon, carbon nanofiber, conductive polymer, steel, iron, copper, titanium, lead, tin, palladium, platinum, platinum coated titanium, other platinum coated Chemoautotrophy of metals, transition metals, transition metal alloys, transition metal sulfides, oxides, chalcogenides, halides, hydroxides, oxyhydroxides, phosphates, sulphates and/or carbonates) Kinetically and/or thermodynamically via means such as, but not limited to, placing the solid electrons in close proximity to the microorganism by introducing them directly into the culture environment. Can be promoted. Some such embodiments of the present invention provide reduction equivalents of poorly soluble electron donors such as, but not limited to, electrons in H ₂ gas or solid electrode materials to oxyhydrogen microorganisms. Can help to move.

The culture broth used in the chemical synthesis process according to certain embodiments of the present invention comprises suitable minerals, salts, vitamins, cofactors, buffers, and other components required for microbial growth known to those of skill in the art. [Bailey and Ollis, Biochemical Engineering Fundamentals, 2nd ed; pp 383-384 and 620-622; McGraw-Hill: New York (1986)]. These nutrients can be selected to maximize carbon fixation and promote carbon flow through the enzymatic pathway to the desired organic compounds. Selective growth environments, such as those used in the art of solid state fermentation or non-aqueous fermentation, can be used in certain embodiments. In certain embodiments utilizing water from an aqueous culture, broth, saline, seawater, and/or other natural aquatic bodies, or water from other sources of potable water, it can be used if it is resistant to oxyhydrogen microorganisms Is.

The biochemical pathways, in certain embodiments of the invention, generally relate to specific growth conditions (eg, trace amounts of micronutrients such as nitrogen, oxygen, phosphorus, sulfur, inorganic ions, and, if present,). Can be controlled and optimized for the production of chemical products (eg target organic compounds) and/or biomass by maintaining a level of any regulatory molecule that is not considered a nutrient or energy source. Depending on the embodiment of the invention, the broth can be maintained in aerobic, microaerobic, anoxic, anaerobic, facultative conditions. A facultative environment is considered to have an aerobic upper layer and an anaerobic lower layer due to the stratification of the water column.

Oxygen levels are controlled in certain embodiments of the invention. Oxygen levels can be controlled, for example, to facilitate the production of target organic compounds by oxyhydrogen microorganisms via carbon fixation. One of the purposes of controlling oxygen levels, in certain embodiments, is to control intracellular adenosine triphosphate (ATP) levels via cellular reduction of oxygen and production of ATP by oxidative phosphorylation (eg, Optimization). In some such embodiments, controlling the ATP concentration while at the same time maintaining the environment sufficiently reducing so that the intracellular ratio of NADH (or NADPH) to NAD (or NADP) is relatively high. But sometimes it is desirable. In some embodiments, ATP levels are as follows: cellular reduction of oxygen and/or other electron acceptors of oxidative strength sufficient to produce ATP via oxidative phosphorylation, ATP into the culture medium. And/or direct introduction of a chemical analogue of ATP into the culture medium by means of one or more, but not limited to, the oxyhydrogen microorganisms. Increased and/or optimized within.

The reduction of oxygen by hydrogen in the oxyhydrogen reaction is generally enzymatically related to the production of ATP via oxidative phosphorylation in oxyhydrogen microorganisms. The oxyhydrogen reaction may act as a substitute for the light reaction of photosynthesis in that it produces both NADPH and ATP. Generally, in oxyhydrogen microorganisms, the hydrogenase catalyzes the reduction of NAD to NADH by hydrogen (or, as an alternative, in some photosynthetic organisms that can perform the oxyhydrogen reaction, the hydrogenase is hydrogenated by H _{2 )} . It catalyzes the reduction of ferredoxin, which in turn reduces NADP to NADPH) [Chen, Gibbs, Plant Physiol. (1992) 100, 1361-1365]. NADH and/or NADPH can then be used as a reducing agent in the anabolic reaction or can be used to produce oxygen by reducing oxygen via oxidative phosphorylation [Bongers, J. et al. Bacteriology, (Oct 1970) 145-151]. Therefore, the following light-dependent photosynthetic reaction:
^{_{2H 2 O + 2NADP + + 2ADP}} + 2Pi + light ^{→ 2NADPH + 2H + + 2ATP +} O 2
Instead of,
1/2O ₂ +2NADP ⁺ +2ADP +2Pi +3H ₂ →2NADPH +2H ⁺ +2ATP +2H ₂ O
Given that it is possible to perform the oxyhydrogen reaction of H. in dark conditions (eg, in the substantial absence of visible electromagnetic radiation) and produce ₂ ATP per H ₂ consumed, hydrogen acts in place of photons [ Bongers, J. et al. Bacteriology, (Oct 1970) 145-151].

In certain embodiments of the invention, anabolic pathways and/or anabolic pathways that promote carbon fixation and also consume ATP in addition to consuming reducing equivalents and/or reduce the net ATP yield of chemically synthesized carbon fixation. Alternatively, the goal is to maintain high intracellular concentrations of ATP as well as NADH and/or NADPH to drive the solvent production pathway. Such biochemical pathways include the following: fatty acid synthesis, mevalonate pathway and terpenoid synthesis, butanol pathway and 1-butanol synthesis, acetolactate/α-ketovalerate pathway and 2-butanol synthesis, and Examples include, but are not limited to, the ethanol route. In some embodiments of the invention, it is possible to determine a preferred oxygen level. That is, if the oxygen level is too low, intracellular ATP may be reduced below the desired level in oxyhydrogen microorganisms, while if the oxygen level is too high, NADH (or NADPH) will be below the desired level. The ratio of NAD (or NADP) may be reduced.

In certain embodiments of the invention, the application of the ATP used in carbon fixation and the synthesis of organic compounds and the oxyhydrogen reaction to produce NADH and/or NADPH may be performed, for example, by the Wood-Ljungdahl pathway or the methanogenic pathway. Can provide advantages over alternative approaches using anaerobic biochemical pathways for carbon fixation of C. Carbon fixation via the Wood-Ljungdahl pathway or the methanogenic pathway generally produces C1 or C2 organic compounds, and it may be difficult to produce compounds above C4 via these pathways.

The Wood-Ljungdahl pathway is essentially capable of producing acetic acid, ethanol, butyric acid, and butanol, but butyric acid and butanol are generally byproducts of H ₂ and CO ₂ gas fermentation, and C 4 Chain lengths above typically do not occur [Lynd, Zeikus, J. et al. of Bacteriology (1983) 1415-1423; Eichler, Sink, Archives of Microbiology (1984) 140, 147-152]. The acetic acid production pathway to acetic acid and butyric acid produces net ATP, whereas the solvent production pathway to ethanol and butanol does not [Papoutsakis, Biotechnology & Bioengineering (1984) 26, 174-187, Heise, Muller, Gottschalk. , J. of Bacteriology (1989) 5473-5478, Lee, Park, Jang, Nielsen, Kim, Jung, Biotechnology & Bioengineering (2008) 101, 209-228]. Because ATP is required for cell maintenance, a certain amount of relatively undesired non-biofuel co-products (ie, organic acids) from acetogens that fix carbon through the Wood-Ljungdahl pathway are generally required. ) Will be present and the reducing equivalents and carbon will be wasted.

The production of hydrocarbons with a chain length above C4 is most commonly achieved biologically via fatty acid biosynthesis [Fischer, Klein-Marcuschamer, Stephanolpoulos, Metabolic Engineering (2008) 10, 295-304. ]. Unlike the solvent-producing pathways that derive from the Wood-Ljungdahl pathway, fatty acid synthesis is involved in net ATP consumption. For example, the net reaction for the synthesis of palmitic acid (C16) is given as follows, starting with acetyl CoA in this example.
8-acetyl _{-CoA + 7ATP + H 2 O +} 14NADPH + 14H + → palmitate ^{+ 8CoA + 14NADP + + 7ADP +} 7Pi

One challenge of the anaerobic pathway, such as methane generation and Wood-Ljungdahl in order to drive the fatty acid synthesis using the ATP generation, ATP produced per _{H 2} consumed is the relatively small, Methane [Thauer, R.; K. Kaster, A.; K. Seedorf, H.; Buckel, W.; & Hedderich, R Methanogenic archea: ecologically relevant differences in energy conservation. Nat Rev Microbiol 6,579-591, doi: nrmicro1931 [pii]] or 1 ATP per 4H _{2 in} the production of acetic acid and 1 ATP per 10H _{2 in} the production of butyric acid [Papoutsakis, Biotechnology 4 & Bio17(4)198(4)). -187, Heise, Muller, Gottschalk, J.; of Bacteriology (1989) 5473-5478, Lee, Park, Jang, Nielsen, Kim, Jung, Biotechnology & Bioengineering (2008) 101, 209-228]. In contrast, in the oxyhydrogen reaction, hydrogen-assimilating oxyhydrogen microorganisms can produce up to ₂ ATP per consumed H ₂ [Bongers, J. et al. Bacteriology, (Oct 1970) 145-151]. In other words, oxyhydrogen microorganisms are capable of producing up to 8 times more ATP per consumed H ₂ than methanogenic or acetogenic microorganisms. Furthermore, in the pathway of ATP production via the oxyhydrogen reaction, rather than the relatively undesired acetic acid or butyric acid product of acid formation, which can perturb the pH of the system and raise it to concentrations that are toxic to organisms, Produce water that can be easily incorporated into the process stream.

The highest energy density fuel that can actually be naturally reached via the Wood-Ljungdahl pathway by injecting inorganic carbon is typically 30 MJ/kg of ethanol, but 36.1 MJ/kg of butanol. There is a possibility. Diesel fuel (46.2 MJ/kg) or JP-8 aviation fuel (43.15 MJ/kg) was produced per ATP required for fatty acid synthesis using anaerobic pathways such as Wood-Ljungdahl. It can be generally difficult and generally less efficient as it increases the amount of H ₂ that needs to be consumed in the absolute anaerobic pathway of However, these high density infra compatible liquid fuels can be readily produced via the ATP, NADH, or NADPH driven liposynthesis pathway produced by the oxyhydrogen reaction.

The lipid content of biomass and the efficiency of lipid biosynthetic pathways contribute to the overall efficiency of certain embodiments of the invention in converting CO ₂ and other C1 compounds to long chain compounds (eg, infrastructure compatible fuels). There are two factors that can influence. The lipid content of biomass may determine the proportion of carbon and reducing equivalents that direct the synthesis of fuel products, as opposed to other components of biomass. Lipid content may determine the energy input from the reduction equivalents that can be recovered in the final fuel product. Similarly, the efficiency of metabolic pathways can determine the amount of reducing equivalents that must be consumed in converting CO ₂ and hydrogen to lipids along the lipid biosynthetic pathway. Many oxyhydrogen microorganisms contain species with high lipid content and containing an efficient pathway from H ₂ and CO ₂ to lipids. In certain embodiments of the invention, high lipid content species such as, but not limited to, Rhodococcus opacus, which may have a lipid content of greater than 70% [Guda, M. K. , Omar, S.; H. , Chekroud, Z.; A & Nour Eldin, H.A. M. Biomediation of kerosine I: A case study in liquid media. Chemosphere 69, 1807-1814, doi: S0045-6535(07)00738-2, Waltermann, M.; Luftmann, H.; Baumeister, D.; Kalscheuer, R.; & Steinbuchel, A.; Rhodococcus opacus strain PD630 as a new source of high-value single-cell oil? Isolation and characterization of triacylglycerols and other storage lipids. Microbiology 146 (Pt 5), 1143-1149 (2000). ] And/or species that utilize highly efficient metabolic pathways such as, but not limited to, the reverse tricarboxylic acid cycle [ie, the reverse citric acid cycle] for carbon fixation [Miura, A. et al. Kameiya, M.; , Arai, H.; , Ishii, M.; & Igarashi, Y.; A soluble NADH-dependent fumarate reductase in the reductive triboxylic acid acid cycle of Hydrogenobacter thermophilus TK-6. J Bacteriol 190, 7170-7177, doi: JB. 00747-08 [pii] 10.1128/JB. 00747-08 (2008). Shivery, J.; M. , Van Keulen, G.; & Meijer, W.M. G. Something from most noting: carbon dioxide fixation in chemautotrofs. Annu Rev Microbiol 52, 191-230, doi: 10.1146/annurev. micro. 5.2.1191 (1998). ] Is used. In terms of energy efficiency, the reverse tricarboxylic acid route can be a relatively advantageous route. The synthesis of palmitic acid from H ₂ and CO ₂ generally increases the ATP production per reduced equivalent consumed in the oxyhydrogen reaction by oxyhydrogen microorganisms, so generally, with respect to the reduced equivalent consumed, It is about 15% more efficient than palmitic acid synthesis in acetogenic bacteria.

Inorganic carbon sources used in the chemical synthesis reaction process steps according to certain embodiments of the present invention include: carbon dioxide-containing gas streams, which may be pure substances or mixtures, liquefied CO ₂ , dry ice, One or more of solid carbon dioxide, carbonate ions, or inorganic carbon in a solid form such as a carbonate ion, a carbonate or a mineral of bicarbonate, which is dissolved in a solution including an aqueous solution such as seawater. However, it is not limited thereto. Carbon dioxide and/or other forms of inorganic carbon can be introduced into the steps of the process where carbon fixation is performed, either bolus addition, periodic or continuous to the nutrient medium contained in the reactor Is. Organic compounds containing only one carbon atom that can be used in the synthetic reaction process steps according to certain embodiments of the present invention include: carbon monoxide, methane, methanol, formate salts, formic acid, And/or mixtures containing C1 chemistries including, but not limited to, various syngas compositions produced from various fixed carbon feedstocks that have been gasified or steam reformed. 1 or 2 or more of these, but not limited to these.

In certain embodiments, organic compounds and/or electron donors containing only one carbon atom are used as biomass and/or other organic matter (eg, biomass and/or other sources from waste or low value sources). It is produced via gasification and/or pyrolysis of organic matter) and provided as syngas to the culture of oxyhydrogen microorganisms. In this case, the ratio of hydrogen to carbon monoxide in the syngas may or may not be adjusted via means such as a water gas shift reaction prior to delivering the syngas to the microbial culture. In certain embodiments, the organic compound containing only one carbon atom and/or the electron donor is methane or natural gas (eg, stranded natural gas or otherwise natural gas that is burned or released to the atmosphere) or Produced via methane steam reforming from biogas or landfill gas and provided as syngas to cultures of oxyhydrogen microorganisms. In this case, the ratio of hydrogen to carbon monoxide in the syngas may or may not be adjusted via means such as a water gas shift reaction prior to delivering the syngas to the microbial culture.

In certain embodiments of the invention, carbon dioxide-containing flue gas is recovered from the chimney at temperatures, pressures, and gas compositions characteristic of untreated exhaust, and with minimal modification, carbon fixation. Directed into the reaction vessel in which it takes place. In some embodiments where no impurities harmful to chemoautotrophic organisms are present in the flue gas, modification of the flue gas as it enters the reaction vessel is required to pump the gas into the reactor system. It is possible to limit the compression and/or gas temperature to the heat exchange required to reduce the temperature to a temperature suitable for microorganisms.

Oxyhydrogen microorganisms generally have advantages over carbon anaerobic acetogenic or methanogenic microorganisms in carbon capture applications because they are more oxygen tolerant. Industrial flue gas is one of the CO ₂ sources contemplated for certain embodiments of the present invention, so that compared to obligate anaerobic methanogens or acetogens, since oxygen resistance is relatively high, it is possible to withstand typical flue 2-6% of O ₂ content found in the gas.

In some embodiments where carbon dioxide containing flue gas is transported into the system to dissolve carbon dioxide in solution (eg, as is well known in the carbon recovery arts), scrubbed flue gas ( In general, mainly containing inert gases such as nitrogen) can be released into the atmosphere.

Gases that are dissolved in solution and fed to the culture broth or directly dissolved in the culture broth in certain embodiments of the invention include a gaseous electron donor (eg, hydrogen gas) in addition to carbon dioxide. In certain embodiments of the invention, but not limited to, other components of carbon monoxide and syngas, hydrogen sulfide, and/or other electron donors such as, but not limited to, other sour gases. Can be included. It is also possible to maintain a controlled amount of oxygen in the culture broth according to some embodiments of the invention, and in certain embodiments oxygen is effectively present in the solution supplied to the culture broth. It will be lysed and/or directly in the culture broth.

Dissolution of oxygen, carbon dioxide, and/or an electron donor gas, such as, but not limited to, hydrogen and/or carbon monoxide, in some embodiments of the invention, Can be achieved using compressor, flow meter, and/or flow valve mechanisms known to those skilled in the art of bioreactor scale microbial culture, commonly used to pump gas into solution. The following features: sparging devices, diffusers (including but not limited to domes, tubes, discs, or donuts of any shape), coarse bubbles or fines It can be supplied to one or more of, but not limited to, a bubble aerator and/or a venturi device. In certain embodiments of the invention, paddle aerators and the like may also be used for surface aeration. In certain embodiments of the invention, mechanical mixing is used with an impeller and/or turbine to facilitate gas dissolution. In some embodiments, hydraulic shearing devices can be used to reduce bubble size.

In certain embodiments of the invention in which air or oxygen needs to be effectively pumped into the culture broth to maintain a beneficial (eg, optimal) oxygen loading level, oxygen bubbles are mixed and oxygen transferred. The desired (eg, optimal) diameter is injected into the broth. It has been shown to be 2 mm in certain embodiments [Environment Research Journal May/June 1999 pgs. 307-315]. In certain aerobic embodiments of the invention, a process of shearing oxygen bubbles is used to achieve this bubble diameter, as described in US Pat. No. 7,332,077. In some embodiments, the bubbles have an average diameter of 7.5 mm or less, and slugging is avoided.

In certain embodiments of the invention that utilize hydrogen as an electron donor, hydrogen gas is bubbled by bubbling it into the culture medium and/or through a membrane that is in contact with and impermeable to the culture medium. It is supplied to a chemoautotrophic culture vessel by diffusing it. The latter method is considered safer in many embodiments and may be preferred, as hydrogen accumulating in the gas phase can form explosive conditions (of explosive hydrogen concentrations in air The range is 4-74.5%, which can be avoided in certain embodiments of the invention). In some embodiments, the membrane is coated with a biofilm of oxyhydrogen microorganisms such that hydrogen must diffuse into the microorganism after passing through the membrane.

Additional chemicals known in the art that are necessary or useful for the maintenance and growth of oxyhydrogen microorganisms can be added to the culture broth according to certain embodiments of the invention. These chemicals include nitrogen sources such as ammonia, ammonium (eg, ammonium chloride (NH ₄ Cl), ammonium sulfate ((NH ₄ ) ₂ SO ₄ )), nitrates (eg potassium nitrate (KNO ₃ )), urea. Or an organic nitrogen source such as a phosphate (eg, disodium phosphate (Na ₂ HPO ₄ ), potassium phosphate (KH ₂ PO ₄ ), phosphoric acid (H ₃ PO ₄ ), potassium dithiophosphate (K ₃ PS ₂ O ₂ ), potassium orthophosphate (K ₃ PO ₄ ), dipotassium phosphate (K ₂ HPO ₄ )), sulfate, yeast extract, chelated iron, potassium (for example, potassium phosphate (KH ₂ PO ₄ ), Potassium nitrate (KNO ₃ ), potassium iodide (KI), potassium bromide (KBr)), as well as other inorganic salts, minerals, and micronutrients (eg, sodium chloride (NaCl), magnesium sulfate (MgSO ₄ 7H ₂ O)). Alternatively, magnesium chloride (MgCl ₂ ), calcium chloride (CaCl ₂ ), or calcium carbonate (CaCO ₃ ), manganese sulfate (MnSO ₄ 7H ₂ O) or manganese chloride (MnCl ₂ ), ferric chloride (FeCl ₃ ), sulfate sulfate Ferrous iron (FeSO ₄ 7H ₂ O), or ferrous chloride (FeCl ₂ 4H ₂ O), sodium bicarbonate (NaHCO ₃ ) or sodium carbonate (Na ₂ CO ₃ ), zinc sulfate (ZnSO ₄ ) or zinc chloride ( ZnCl ₂ ), ammonium molybdate (NH ₄ MoO ₄ ), or sodium molybdate (Na ₂ MoO ₄ 2H ₂ O), cuprous sulfate (CuSO ₄ ) or copper chloride (CuCl ₂ 2H ₂ O), cobalt chloride (CoCl) ₂ 6H ₂ O), aluminum chloride _(AlCl 3 _.6H 2 O), lithium chloride (LiCl), boric acid _{(H 3 BO 3), 2} 6H 2 O nickel chloride _(NiCl), tin chloride (SnCl ₂ H ₂ O ), barium chloride (BaCl ₂ 2H ₂ O), copper selenate (CuSeO ₄ 5H ₂ O) or sodium selenite (Na ₂ SeO ₃ ), sodium metavanadate (NaVO ₃ ), chromium salt). However, the present invention is not limited to these. In certain embodiments, mineral salt medium (MSM) formulated by Schlegel et al. may be used [Thermophilic bacteria, Jakob Kristjansson, Chapter 5, Section III, CRC Press, (1992)].

In certain embodiments, the concentration of nutritional chemicals (eg, electron donors and electron acceptors) is at a level (eg,) that favors enhanced (eg, maximal) carbon uptake and fixation and/or organic compound production. (For example, as close as possible to their respective optimum levels), which vary depending on the oxyhydrogen species utilized, but are known or without undue experimentation. It can be determined by those skilled in the art of microbial culture.

In certain embodiments of the present invention, nutrient levels as well as waste product levels, pH, temperature, salinity, dissolved oxygen and dissolved carbon dioxide, gas and liquid flow rates, agitation rates, and pressure in a microbial culture environment are controlled. To be done. Operating parameters that affect carbon fixation can be monitored using sensors (eg, dissolved oxygen and/or redox probes are used to measure electron donor/electron acceptor concentrations) and actuated valves. , Pumps, and agitators can be used to control manually or automatically based on feedback from sensors by using devices such as, but not limited to. The temperature of the inflow broth as well as the inflow gas can be adjusted by means such as, but not limited to, a heat exchanger.

Dissolution of gases and nutrients needed to maintain oxyhydrogen culture and promote carbon fixation, as well as removal of inhibitory waste products, can be facilitated by agitation of the culture broth. Oxyhydrogen microorganisms can carry out carbon fixation reaction over the entire volume of the reaction tank, including methods utilizing photosynthetic organisms (photosynthesis requires light, so it is limited to the surface area) It offers advantages over other approaches. The use of agitation may reduce microorganisms, nutrients, optimal growth environment, and/or CO2 in a reactor volume such that production is facilitated (eg, maximizing the reactor volume in which the carbon fixation reaction occurs at an optimal rate). It is possible to further increase this advantage by making the distribution as wide and uniform as possible throughout.

Agitation of the culture broth in certain embodiments of the invention includes recirculating the broth from the bottom of the vessel to the top through a recirculation conduit, carbon dioxide, electron donor gas (eg, H ₂ ), oxygen, and/or Or by means of air sparging and/or equipment such as, but not limited to, mechanical mixers such as, but not limited to, impellers (100-1000 rpm) and turbines (but not limited to). Achievable.

In certain embodiments of the present invention, the chemical environment, oxyhydrogen microorganisms, electron donors, electron acceptors, oxygen, pH, and/or temperature levels can be varied according to a wide variety of carbon fixation reactions and/or biogenic compounds leading to organic compounds. Varying, either spatially and/or temporally, across a series of bioreactors in fluid communication such that the chemical pathways take place sequentially or in parallel.

The nutrient medium containing oxyhydrogen microorganisms is, in certain embodiments of the invention, partially or completely, periodically or continuously removable from the bioreactor and, for example, exponentially growing the cell culture. To supplement the depleted nutrients in the growth medium in order to maintain the cell culture in growth phase (exponential phase or stationary phase) at an increased (eg optimal) carbon fixation rate in order to maintain phase And/or can be replaced with fresh cell-free medium to remove inhibitory waste products.

Due to the high growth rates achievable with oxyhydrogen species, it is possible to match or exceed the maximum rates of carbon fixation and/or biomass production per unit biomass abandoned achievable with photosynthetic microorganisms. As a result, in certain embodiments, it is possible to produce excess biomass. Cell mass overgrowth can be removed from the system to produce a biomass product. In some embodiments, the overgrowth of the cell mass is to maintain a desirable (eg, optimal) microbial population and cell density in the microbial culture so that a continuous high carbon capture fixation rate is obtained. , Can be removed from the system.

Another advantage of certain embodiments of the present invention relates to a vessel containing a carbon fixation reaction environment and used to carry out the culture in a carbon capture fixation process. Exemplary culture vessels that can be used in some embodiments of this invention to culture and grow oxyhydrogen microorganisms for carbon dioxide capture fixation include those known to those of skill in the art of large-scale microbial culture. Can be mentioned. Such culture tanks, which may be of natural or artificial origin, include airlift reactors, biological scrubber towers, bioreactors, bubble towers, caverns, caves, cisterns, continuous stirred tank reactors, countercurrent rise. Expanded bed reactors, digesters, in particular digester systems known in the prior art for sewage/wastewater treatment or bioremediation, filters such as trickle filters, rotating biological contactor filters, rotating disks, soil filters (but not (But not limited to these), fluidized bed reactor, gas lift fermentor, immobilized cell reactor, lagoon, membrane biofilm reactor, microbial fuel cell, ore shaft, pachuca tank, packed bed reactor, plug flow reactor, pond, pool , Quarries, storage tanks, static mixers, tanks, towers, trickle bed reactors, vats, vertical shaft bioreactors, and wells, but are not limited thereto. The bottom, siding, walls, lining, and/or top may be bitumen, cement, ceramics, clay, concrete, epoxy, fiberglass, glass, macadam, plastic, sand, sealant, soil, steel or other metals and their It can be constructed from one or more materials including, but not limited to, alloys, stone, tar, wood, and any combination thereof. In certain embodiments of the present invention, where the oxyhydrogen microorganisms require a corrosive growth environment and/or produce corrosive chemicals via carbon fixation reactions, inside the vessel where the corrosion resistant material is used to contact the growth medium. Can be lined.

Since oxyhydrogen microorganisms do not require sunlight to fix CO ₂ , they can be used in a carbon capture and fixation process that avoids many of the drawbacks associated with photosynthesis-based carbon capture and conversion techniques. For example, in order to maintain chemical synthesis, shallow and large ponds are not needed, nor are bioreactors with high surface-to-volume ratios and special features or transparent materials like solar collectors. Techniques such as certain embodiments of the invention that utilize oxyhydrogen microorganisms are not subject to the diurnal, geographical, meteorological, and seasonal constraints typically associated with photosynthesis-based systems.

In certain embodiments of the invention, a low shape such as, but not limited to, a cubic shape, a medium aspect ratio cylindrical shape, an ellipsoidal shape or “oval shape”, a hemispherical shape or a spherical shape. By using a chemical synthesis bath geometry with a surface area to volume ratio, material costs are minimized unless other design requirements (eg, land footprint) dominate material costs. In contrast to photosynthesis technology, which requires a large surface-to-volume ratio to provide sufficient light irradiation, the use of small reactor geometries is due to the lack of light-requiring chemical synthesis reactions. You can.

Also, because oxyhydrogen microbes have no light dependence, it allows for plant designs with much smaller footprints than are traditionally associated with photosynthetic techniques. For example, a long vertical shaft bioreactor system can be used for chemosynthetic carbon capture if it is assumed that plant footprint needs to be minimized due to limited land utilization. Long vertical shaft type bioreactors are disclosed, for example, in US Pat. Nos. 4,279,754, 5,645,726, 5,650,070, and 7,. 332,077.

Unless other requirements prevail, in certain embodiments of the present invention, the introduction of invading erosive food to the vessel surface and/or the reactor causing high loss of water, nutrients, and/or heat is minimized. It can be suppressed. The ability to minimize such surfaces may be due to the absence of a chemical synthesis requirement. Photosynthesis-based techniques generally require that the surface that causes high loss of water, nutrients, and/or heat, and that is lost by erosion, is generally the same as the surface that transmits the light energy required for photosynthesis. In general, such surfaces cannot be minimized.

The incubator according to the invention, in some embodiments, depending on the embodiment of the invention, maintains an aerobic, microaerobic, anoxic, anaerobic, or facultative environment, Reactor designs known to those skilled in the art of large scale microbial culture can be used. For example, similar to the design of many sewage treatment plants, certain embodiments of the present invention include tanks to perform multiple chemical synthesis process steps on a carbon dioxide waste stream, and in certain embodiments heterotrophic process steps. Are sequentially arranged in serial forward fluid communication, with certain tanks maintained in aerobic conditions and other tanks maintained in anaerobic conditions.

In a particular embodiment of the invention, the oxyhydrogen microorganisms are immobilized in their growth environment. The immobilization of microorganisms is carried out using any medium known in the art of culturing microorganisms that supports colonization by microorganisms, for example the following: glass wool, clay, concrete, wood fibers, inorganic oxides (eg , ZrO ₂ , Sb ₂ O ₃ , or Al ₂ O ₃ ), organic polymer polysulfone, or open-pore polyurethane foam having a high specific surface area, but not limited thereto (But not limited to) using a medium that grows microorganisms on matrices, meshes, or membranes made from any of a wide variety of natural and synthetic materials and polymers, including but not limited to: Not), achievable. Microorganisms in certain embodiments of the invention also include, but are not limited to, those that have not been distributed throughout the growth vessel as is known in the art of microbial culture. On the surface of the binding object, for example, the following: beads, sand, silicates, sepiolites, glasses, ceramics, small diameter plastic discs, spheres, tubes, particles or in the art. Other known shapes, shredded coconut hulls, crushed corncobs, activated carbon, granular coal, crushed corals, sponge balls, suspension media, small pieces of rubbery (elastomeric) polyethylene tubing of small diameter, porous cloth , Berl saddles, Raschig ring slings can be propagated on the surface of one or more objects, including but not limited to. The materials used in the microbial support medium may include hydrogen storage materials and/or electrode materials to enhance the transfer of reducing equivalents to oxyhydrogen microorganisms. Usable electrode materials include the following: graphite, activated carbon, carbon nanofibers, conductive polymers, steel, iron, copper, titanium, lead, tin, palladium, platinum, transition metals, transition metal alloys, transitions. One or more of metal sulfides, oxides, chalcogenides, halides, hydroxides, oxyhydroxides, phosphates, sulphates, or carbonates can be mentioned, but are not limited thereto. Not a thing. Examples of hydrogen storage materials that can be used in this application include titanium, graphite, activated carbon, carbon nanofibers, iron, copper, lead, tin, and metal hydrides (for example, TiFeH ₂ , TiH ₂ , VH ₂ , ZrH ₂ , NiH, Examples include, but are not limited to, NbH ₂ , PdH, and polymers known in the hydrogen storage art (eg, metal organic framework (MOF)). ), and nanoporous polymeric materials, but are not limited thereto. In certain embodiments, the hydrogen storage material does not react strongly with water and has no strong or rapid effect on the pH of the culture medium.

Inoculation of the oxyhydrogen culture into the fermentor is effected in the transfer and/or incubator of the culture from existing oxyhydrogen cultures resident in other carbon capture fixation systems according to certain embodiments of the invention. Can be performed by methods including, but not limited to, transfer of culture from incubation of the inoculum stock. The inoculum stock of the oxyhydrogen strain may be in powder, liquid, frozen, or lyophilized form, as well as any other suitable form readily apparent to one of skill in the art, including, but not limited to. It can be transported and stored in its original form. In certain embodiments where the culture is established in a very large reactor, the growth and establishment of the culture can be done in successive scale vessels in intermediate scale vessels prior to inoculation of the phenylscale bath. ..

The location of one or more process steps that separate cell clumps from the process stream in the general process flow of certain embodiments of the present invention is illustrated by box 5 in FIG. 1, labeled “Cell Separation”. It

Separation of cell clumps from a liquid suspension is carried out by the following methods: centrifugation, flocculation, flotation, filtration using membrane type, hollow fiber type, spiral wound type, ceramic type filter system, vacuum filtration. , Tangential flow filtration, clarification, sedimentation, hydrocyclone, or one or more (but not limited to), by any method known in the art of microbial culture. There is an example of a cell mass collecting technique, WO 08/00558 pamphlet published on Jan. 8, 1998, US Pat. No. 5,807,722, US Pat. No. 5,593,886. , And US Pat. No. 5,821,111]. In certain embodiments where the cell clumps are immobilized on a matrix, they are harvested by methods including, but not limited to, gravity settling or filtration and separated from the growth substrate by liquid shear. It is possible.

In certain embodiments of the invention, when excess cell mass is removed from the culture, in combination with fresh broth such that sufficient biomass is retained in one or more chemosynthesis reaction steps, " It is possible to recirculate back into the cell culture as indicated by the process arrow marked "Recycled Cell Mass". This allows for continuous enhanced (eg, optimal) autotrophic carbon fixation production of organic compounds. The cell mass collected by the collection system can be recycled and returned to the culture tank using, for example, an air lift pump or an intermittent pump. In certain embodiments, the cell mass that is recirculated and returned to the culture tank is not exposed to the aggregating agent unless the aggregating agent is non-toxic to the microorganism.

In certain embodiments of the invention, microbial cultures and carbon fixation reactions use continuous influx removal of nutrient medium and/or biomass to determine cell population and environmental parameters (eg, cell density, chemical concentration) over time. It is maintained in a steady state, targeted at a constant (eg, optimal) level. Cell density can be monitored in certain embodiments of the invention by direct sampling, by correlation of optical density with cell density, and/or by a particle size analyzer. The hydraulic and biomass retention times can be separated so that both broth chemistry and cell density can be independently controlled. It is possible to keep the fluid pressure retention time relatively short compared to the biomass retention time and to keep the dilution high enough to allow a large replenishment of cell growth broth. The dilution rate is set to the optimum trade-off between supplementing the culture broth and increasing process cost from pumping, increased dosage, and other requirements associated with the dilution rate.

To assist in the processing of biomass products into biofuels or other useful products, for example, but not limited to, ball milling, cavitation pressure, sonication, or mechanical shearing after the cell recycling step. It is possible to destroy and release excess microbial cells in certain embodiments of the invention using methods including (but not limited to).

The biomass harvested in some embodiments may be processed in one or more process steps in box 7 labeled "Dryer" in the general process flow of the particular embodiment of the invention illustrated in FIG. It is possible to dry with.

In certain embodiments of the invention, drying excess biomass includes but is not limited to centrifugation, drum drying, evaporation, freeze drying, heating, spray drying, vacuum drying, and/or vacuum filtration. It is possible to implement it by using a technology such as (No). Waste heat from industrial sources of flue gas can be used to dry the biomass in certain embodiments. In addition, the chemosynthetic oxidation of electron donors is generally exothermic and generally produces waste heat. In a particular embodiment of the present invention, waste heat can be used to dry the biomass.

In certain embodiments of the invention, the biomass is further processed after drying to assist in the production of biofuels or other useful chemicals by separating lipid content or other target biochemicals from microbial biomass. .. Separation of lipids is carried out using a non-polar solvent for extracting lipids, for example, hexane, cyclohexane, ethyl ether, alcohol (isopropanol, ethanol, etc.), tributyl phosphate, supercritical carbon dioxide, trioctylphosphine oxide, secondary and It can be carried out using, but not limited to, tertiary amines or propane. Other useful biochemicals can be extracted with solvents including, but not limited to, chloroform, acetone, ethyl acetate, and tetrachloroethylene.

The extracted lipid content of the biomass may include, but is not limited to, one or more of the following: catalytic cracking and reforming, decarboxylation, hydrotreating, isomerization. Treated using methods known in the science and technology of biomass refining, including the following: JP-8 jet fuel, diesel oil, gasoline, and other alkanes, olefins, and aromatics It is possible to produce petroleum and petrochemical alternatives, including but not limited to one or more. In some embodiments, the extracted lipid content of the biomass is obtained via processes known in the science and technology of biomass purification, including, but not limited to, transesterification and esterification. It can be converted into ester fuels such as biodiesel oil (fatty acid methyl ester or fatty acid ethyl ester).

The broth remaining after removal of the cell mass can be pumped into a system for removing chemical products of chemosynthesis and/or spent nutrients which are recycled or possibly recovered and/or discarded.

The location of one or more process steps for recovering chemicals from the process stream in the general process flow of certain embodiments of the present invention is indicated by box 8 in FIG. 1, labeled "Chemical Co-Product Separation." It is illustrated in.

The recovery and/or recycling of chemosynthetic chemical products and/or spent nutrients from an aqueous broth solution is, in certain embodiments of the invention, known in the art of the process industry and specific practice of the invention. Using equipment and techniques targeted to obtain a chemical product in the form of, for example, solvent extraction, water extraction, distillation, fractional distillation, cementation, chemical precipitation, alkaline solution absorption, on activated carbon, ion exchange resins. Absorption or adsorption on, or on molecular sieves, modification of solution pH and/or redox potential, evaporators, fractional crystallisers, solid/liquid separators, nanofiltration, and all combinations thereof, but not both. But not limited to) can be achieved.

In certain embodiments of the invention, long chain organic compounds that are compatible with purification to free fatty acids, lipids, or other media, or biofuel products produced via chemical synthesis are labeled box 8 in FIG. Can be recovered from the process stream in the step of. These free organic molecules can be released from the oxyhydrogen microorganisms into the process stream solution via means including, but not limited to, cell excretion or secretion or cell lysis. is there. In certain embodiments of the invention, the recovered organic compound is one or more of, but not limited to, the following: catalytic cracking and reforming, decarboxylation, hydrotreating, isomerization. (But not necessarily) and methods known in the science and technology field of biomass refining. Such processes include, but are not limited to, one or more of JP-8 jet fuel, diesel oil, gasoline, and other alkanes, olefins, and aromatics. Can be used to produce petroleum and petrochemical alternatives, including (but not). Recovered fatty acids are biodiesel oil (fatty acid methyl ester or fatty acid ethyl ester) via processes known in the science and technology of biomass refining including, but not limited to, transesterification and esterification. ) And other ester-based fuels.

In some embodiments, after recovery of the chemicals from the process stream, removal of waste products is performed as indicated by box 9 labeled "waste removal" in FIG. Residual broth can be returned to the fermentor with exchanged water and/or exchanged nutrients.

In certain embodiments of the invention involving chemoautotrophic oxidation of electron donors extracted from mineral ores, the solution of metal oxide cations may remain after the chemical synthesis reaction step. Also, the solution rich in dissolved metal cations can be attributed, in particular, to fouling flue gas from the coal firing plant or the like being injected into the process. In some such embodiments of the invention, cementation of scrap iron, steel wool, copper, or zinc dust, chemical precipitation as precipitation of sulfides or hydroxides, electrowinning to plate certain metals, on activated carbon. Or stripping metal cations from the process stream by methods including, but not limited to, absorption onto ion exchange resins, modification of solution pH and/or redox potential, solvent extraction. It is possible. In particular embodiments of the invention, the recovered metal may be sold for additional revenue streams.

In certain embodiments, the chemicals used in the process of chemical product recovery, nutrient and water recycle, and waste removal processes have low toxicity to humans and are recycled and grown. It has low toxicity to the oxyhydrogen microorganisms used when exposed to the process stream returned to the container.

In a particular embodiment of the invention, the pH of the microbial culture is controlled. To counter the pH drop, a neutralization step can be performed to maintain the pH within the optimum range for microbial maintenance and growth before recycling the broth back into the fermentor. Neutralization of acids in broth is achieved by the addition of bases including, but not limited to limestone, lime, sodium hydroxide, ammonia, caustic potash, magnesium oxide, iron oxide. It is possible. In certain embodiments, the base is calcium oxide, magnesium oxide, iron oxide, iron ore, metal oxide-containing olivine, metal oxide-containing serpentine, metal oxide-containing ultrabasic deposits and subsurface basic saline zones. Produced from carbon dioxide-free sources such as naturally occurring basic minerals including, but not limited to, aqueous layers. Carbon dioxide will generally be released when limestone is used for neutralization. This carbon dioxide can be directed back into the growth vessel for uptake by chemical synthesis and/or otherwise sequestered rather than released into the atmosphere.

Further features of particular embodiments of the invention relate to the use of organic compounds and/or biomass produced via one or more chemical synthesis process steps according to particular embodiments of the invention. Examples of the use of the produced organic compound and/or biomass include JP-8 jet fuel, diesel oil, gasoline, octane, biodiesel oil, butanol, ethanol, propanol, isopropanol, propane, alkane, olefin, aromatic compound, and fat. Production of liquid fuels including alcohols, fatty acid esters, alcohols (but not limited to), 1,3-propanediol, 1,3-butadiene, 1,4-butanediol, 3-hydroxy Propionate, 7-ADCA/cephalosporin, ε-caprolactone, γ-valerolactone, acrylate, acrylic acid, adipic acid, ascorbate, aspartate, ascorbic acid, aspartic acid, caprolactam, carotenoids, citrate, citric acid , DHA, docetaxel, erythromycin, ethylene, gamma butyrolactone, glutamate, glutamic acid, HPA, hydroxybutyrate, isopentenol, isoprene, isoprenoids, itaconate, itaconic acid, lactate, lactic acid, lanosterol, levulinic acid, lycopene, lysine, apple Acid salt, malonic acid, peptide, ω-3DHA, ω fatty acid, paclitaxel, PHA, PHB, polyketide, polyol, propylene, pyrrolidone, serine, sorbitol, statin, steroids, succinate, terephthalate, terpene, THF, rubber , Wax esters, polymers, general-purpose chemicals, industrial chemicals, specialty chemicals, paraffin substitutes, additives, nutritional supplements, nutritional drugs, pharmaceuticals, pharmaceutical intermediates, personal care products (but not limited to these As raw materials and/or feedstocks for the production of organic chemicals, including but not limited to), manufacturing processes or chemical processes, alcohol fermentation or other biofuel fermentation and/or gasification and liquefaction processes and/or others Biofuel production processes including, but not limited to, catalytic cracking, direct liquefaction, Fisher Tropsch process, hydrogenation, methanol synthesis, pyrolysis, transesterification, or microbial syngas conversion. , As a biomass fuel for combustion, specifically as a fuel that is co-combusted with fossil fuels, as a source of medicinal, medicinal or nutritional substances, commercially available enzymes, antibiotics, amino acids, vitamins Kind, bio plastic Other microorganisms or organisms as carbon sources for large scale fermentations producing a variety of chemicals including, but not limited to, stick, glycerol, or 1,3-propanediol. As a dietary source for animals, including but not limited to cows, sheep, chickens, pigs, or fish, for the production of methane or biogas. Examples of the feedstock of the present invention include, but are not limited to, fertilizers, soil additives and soil stabilizers.

Further features of certain embodiments of the invention relate to the optimization of oxyhydrogen microorganisms for carbon dioxide capture, carbon sequestration to organic compounds, and the production of other valuable chemical co-products. This optimization includes, but is not limited to, accelerated mutagenesis (eg, using ultraviolet light or chemical treatment), genetic engineering or modification, hybridization, synthetic biology, or traditional selection breeding. No.) and other methods known in the technical field of artificial breeding. In certain embodiments of the invention that utilize a microbial consortium, the community is a target electron donor, including but not limited to hydrogen, oxygen, but not limited to. , Etc., and growth in the presence of environmental conditions can be enriched with the desired oxyhydrogen microorganisms using methods known in the art of microbiology.

A further feature of certain embodiments of the invention relates to modifying the biochemical pathways of oxyhydrogen microorganisms to produce target organic compounds. This modification may be by manipulating the growth environment and/or accelerated mutagenesis (eg, using UV light or chemical treatment), genetic engineering or modification, hybridization, synthetic biology, or traditional It can be achieved through methods known in the art of artificial breeding, including but not limited to selective breeding. Organic compounds produced through modification include the following: JP-8 jet fuel, diesel oil, gasoline, biodiesel oil, butanol, ethanol, long chain hydrocarbons, lipids, fatty acids, simulated vegetable oils, and To produce biofuels, including but not limited to methane produced from biological reactions in vivo, or biofuels and/or liquid fuels via chemical aftertreatment. The feedstock of the present invention includes, but is not limited to, one or more of optimized organic compounds and/or biomass. These forms of fuel can be used as renewable/alternative energy sources with cold room effect gas emissions.

Specific embodiments of the invention are now described to provide specific examples of total biochemical processes for recovering CO ₂ using oxyhydrogen microorganisms and producing biomass and other useful co-products. A process flow diagram is provided and described. This particular example should not be construed as limiting the invention in any way and is provided for illustrative purposes only.

FIG. 2 is an exemplary process flow diagram illustrating one embodiment of the present invention for the capture of CO ₂ by oxyhydrogen microorganisms and the production of lipid-rich biomass, which is converted to JP-8 jet fuel. including. In this group of embodiments, carbon dioxide-rich flue gas is recovered from an emission source such as a power plant, refinery, or cement manufacturer. Then, to compress the flue gas, Rod Pseudomonas pulse tris (Rhodopseudomonas palustris), Rod Pseudomonas Kapusurata (Rhodopseudomonas capsulata), Rod Pseudomonas Biridisu (Rhodopseudomonas viridis), Rhodopseudomonas Sur Fobi Ridisu (Rhodopseudomonas sulfoviridis), Rod Red non-sulfur photosynthetic bacteria, including but not limited to Rhodopseudomonas blastica, and other Rhodopseudomonas species, including but not limited to: It is possible to pump into a cylindrical anaerobic digester containing one or more oxyhydrogen microorganisms (e.g.

In some embodiments, Rhodopseudomonas capsulata can be used as the oxyhydrogen microorganism, and in some cases chemoautotrophic growth with hydrogen for a multiplication time of 6 hours. Can be achieved. For example, Madigan, Gest, J.; See Bacterology (1979) 524-530, which is hereby incorporated by reference. In some embodiments, the doubling time of the microorganism can be 6 hours or less. In some embodiments, the dry biomass concentration can be at least about 3 g/l, at least about 4 g/l, or at least 5 g/l at steady state. In some embodiments, the lipid content of the biomass in the oxyhydrogen microorganisms can be at least about 10%, at least about 20%, at least about 30%, at least about 35%, or at least about 40%. For example, in some embodiments, Rhodopseudomonas palustris can be used as an oxyhydrogen microorganism. For example, Carlozzi, Pintucci, Piccardi, Buccini, Minieri, Lambardi, Biotechnol. Lett. , (2009) DOI 10.1007/s10529-009-0183-2, which is hereby incorporated by reference. In certain embodiments, the biomass content of oxyhydrogen microorganisms is at least 40%, there is a steady state bioreactor cell density of at least 5 g/liter in a continuous process, and the doubling time of the microorganisms is up to 6 hours. And the process achieves an energy efficiency of at least 40% in the conversion of hydrogen to biomass and/or at least 60% of the biomass energy content is stored as lipids (which is about 40% by weight biomass. Corresponding to the lipid content of).

In the group of embodiments shown in Figure 2, hydrogen electron donors and oxygen and carbon dioxide electron acceptors are required for chemical synthesis and maintenance and growth of cultures that are pumped into digesters. , Nutrients, and added continuously to the growth broth. In a particular embodiment, the hydrogen source is a carbon dioxide free emission process. Exemplary carbon dioxide-free emissions processes include, but are not limited to, photovoltaics, solar heat, wind power, hydroelectric power, nuclear power, geothermal, enhanced geothermal, ocean heat, wave power, tidal power. ) And other electro-chemical or thermochemical processes powered by energy technologies. In the group of embodiments shown in FIG. 2, oxygen functions as an electron acceptor in the chemosynthetic reaction of intracellular production of ATP via the oxyhydrogen reaction associated with oxidative phosphorylation. Oxygen can be generated from flue gas, it can be generated from the water splitting reaction used to produce hydrogen, and/or it can be extracted from air. In FIG. 2, carbon dioxide from the flue gas is combined with ATP produced via the oxyhydrogen reaction and NADH and/or NADPH produced from the intracellular enzyme-catalyzed reduction of NAD ⁺ or NADP ⁺ by H ₂ . Acts as an electron acceptor for the synthesis of organic compounds via a biochemical pathway utilizing The culture broth can be separated from the broth by continuously removing it from the digester and allowing it to flow through a membrane filter. The cell mass can then be recycled back to the digester and/or pumped for work-up to perform lipid extraction according to methods known to those of skill in the art. The lipids are then processed by methods known to those of ordinary skill in the art of biomass purification (eg, US DOE Energy Efficiency & Renewable Energy Biomass Program, "National Algal Biofuels Technology," in its entirety, see Chapter 10 of its book, Romology, Vol. It is possible to convert into JP-8 jet fuel by using the above). The cell-free broth that has been passed through the cell debris filter can then be subjected to any necessary additional waste removal treatment depending on the flue gas source. The residual water and nutrients can then be pumped back into the digester.

Some of the species of Rhodopseudomonas have a very general metabolism, which allows them to be photoautotrophic, photoheterotrophic, heterotrophic, and even chemoautotrophic, aerobic Viable in both environmental and anaerobic environments [Madigan, Gest, J. et al. Bacteriology (1979) 524-530]. In certain embodiments of the invention, the heterotrophic function of Rhodopseudomonas species is exploited to further improve the efficiency of energy and carbon conversion to lipid products. The non-lipid biomass residue after lipid extraction is mainly composed of proteins and carbohydrates. In a particular embodiment of the invention, as shown in Figure 2, a portion of the carbohydrate and/or protein residue after lipid extraction is acid hydrolyzed to monosaccharides and/or amino acids to neutralize the acid. , And a solution of monosaccharides and/or amino acids is fed to a second heterotrophic bioreactor containing species of Rhodopseudomonas that consumes the biomass input to produce additional lipid products.

The genome of Rhodopseudomonas palustris was sequenced by the DOE Joint Genome Institute [Larimer et. al (2003) Nature Biotechnology 22, 55-61]. It has been reported that the genetic system can be modified particularly easily. In one group of embodiments of the invention, the one or more carbon fixation reactions are of the following: accelerated mutagenesis, genetic engineering or modification, hybridization, synthetic biology, or traditional selection breeding. Improved fixation of carbon dioxide and/or other forms of inorganic carbon and/or improved organic compounds via methods including one or more of, but not limited to, Is produced by a species of the genus Rhodopseudomonas that has been modified, optimized, or engineered to produce such production.

FIG. 3 includes an exemplary schematic diagram of a bioreactor 300 that can be used in certain embodiments. The bioreactor 300 is, for example, as the reactor illustrated as box 4 in FIG. 1 labeled “Bioreactor-Detonation Microorganisms” and/or in FIG. 2 labeled “Bioreactor-Red Nonsulfur Bacteria”. It can be used as the reactor illustrated as Box 4. The bioreactor 300 illustrated in FIG. 3 can be manipulated to take advantage of the low solubility of hydrogen gas and oxygen gas in water, avoiding dangerous mixing of hydrogen gas and oxygen gas. In addition, the bioreactor provides oxygen and hydrogen needed for cell energy and carbon fixation, for example by sparging, bubbling, or diffusing oxygen or air upwards into a vertical liquid column filled with culture medium. It is possible to provide to oxyhydrogen microorganisms.

Bioreactor 300 includes a first column 302 and a second column 304. In the group of embodiments shown in FIG. 3, oxygen is introduced into the first column 302, while hydrogen or syngas is introduced into the second column 304, while in other embodiments their order. May be reversed. Oxygen and/or hydrogen and/or syngas can be introduced into their respective columns, for example by sparging, bubbling, and/or diffusing so as to move upward through the culture medium. The bioreactor 300 may include a horizontal liquid connection 312 at the top of the tower and a horizontal liquid connection 314 at the bottom of the tower.

In some embodiments, the level of liquid medium in column 302 is maintained such that gas headspace 316 is formed above the liquid. In addition, in some cases, the level of liquid medium in column 304 can be arranged such that gas headspace 318 is formed above the liquid medium. In some embodiments, the headspace 316 and/or the headspace 318 is at least about 2%, at least about 10%, at least about 25%, 2% to about 80%, of the total volume of the column in which they are located. It can comprise 10% to about 80%, or about 25% to about 80%. Headspaces 316 and 318 can be isolated from each other by liquid culture. In some embodiments, the low solubility of the gas in the liquid medium allows the gas to be collected at the top of the columns after bubbling or spreading the gas upwards through each of those columns. is there. By establishing an isolated headspace, it is possible to prevent dangerous amounts of hydrogen gas and oxygen gas from mixing with each other. For example, it is possible to prevent hydrogen gas in one column from mixing with oxygen gas in the other column (and vice versa). Prevention of mixing of hydrogen gas and oxygen gas is achieved, for example, by maintaining the connection between the two columns so as to prevent the transport of gas from one column to the other by filling the liquid. It is possible. In some embodiments, the liquid medium is circulated between the first and second columns so that the headspaces 316 and/or 318 can be maintained substantially constant at the top of each of those columns. ..

In FIG. 3, the horizontal liquid connection 312 at the top of the column and the horizontal liquid connection 314 at the bottom of the column are such that the liquid medium flows upward in one column in the direction of oxygen gas with the horizontal liquid connection constantly filled. , And the other column so as to flow downwards against hydrogen gas and/or syngas. In another embodiment, the liquid culture medium flows upwards through a column containing hydrogen gas and/or syngas and downwards (countercurrent to the gas) through the other column containing oxygen gas. Is possible.

In some embodiments, the gas on one side or the other side (but not both sides simultaneously) causes the particular column to act as an airlift reactor, driving the circulation of the culture medium between the two columns, You can force bubbling. Also, in some embodiments, fluid circulation can be assisted by impellers, turbines, and/or pumps.

In some such embodiments, any unused hydrogen gas and/or syngas (which may terminate in the headspace) that has passed through the culture medium without being taken up by the microorganisms will remove gas from the headspace. It is possible to recycle by pumping, optionally compressing it and returning it into the medium at the bottom of the liquid column on the hydrogen side and/or the syngas side. In some embodiments, oxygen and/or air may likewise be recirculated on each side thereof, or, alternatively, vented after passing through the headspace.

The oxyhydrogen microorganisms, in certain embodiments, are freely circulated with the liquid medium between the first and second columns. In other embodiments, oxyhydrogen microorganisms are limited to the hydrogen side, for example, using a microfilter that allows the liquid medium to pass through but keeps the microorganisms on the hydrogen side.

FIG. 4 includes exemplary schematics of other methods of operating the bioreactor 300 that can be used in certain embodiments. The bioreactor arrangement of FIG. 4 can take advantage of the relatively high solubility of carbon dioxide and/or the high ability of oxyhydrogen microorganisms to recover carbon dioxide from relatively dilute streams. The procedure illustrated in FIG. 4 can take advantage of the carbon enrichment mechanism unique to oxyhydrogen microorganisms. Flue gas and/or air containing carbon dioxide can be transported via the oxygen side of the bioreactor. Carbon dioxide can be dissolved in the solution and/or can be taken up by oxyhydrogen microorganisms and then, for example, via the horizontal liquid connection 312 at the top of the column, through the hydrogen side of the reactor. Can be shipped to. On the hydrogen side, it is possible to provide a reducing equivalent that drives the fixation of carbon. In some embodiments, other gases that are pumped to the oxygen side (eg, oxygen, nitrogen, etc.) have low solubilities in contrast to CO ₂ and are not brought to the hydrogen side. Rather than being sent from column 302 to column 304, the low solubility gas can be transported to headspace 316. In some embodiments, it is possible to vent the gas after it has been transported to the headspace 316.

FIG. 5 includes an exemplary schematic diagram of an electrolyzer 500 that can be used in certain embodiments. The electrolysis device 500 may be, for example, as a unit illustrated as box 3 in FIG. 1 labeled “Electron Donor Generation” and/or as a unit illustrated as box 3 in FIG. 2 labeled “Electrolysis”. It can be used. The electrolyzer 500 is characterized by reducing or eliminating the complete separation of hydrogen and oxygen produced from the electrolysis process as compared to separation schemes utilized in conventional electrolysis systems designed for the production of pure hydrogen. It can be designed to take advantage of the tolerance and need of oxyhydrogen microorganisms to oxygen concentrations of. The apparatus 500 includes an electrolysis unit 502 configured to produce H ₂ and O ₂ from water. Any suitable electrolysis unit 502 can be utilized to carry out the electrolysis step. In some embodiments, the following is used: removing the separator used in standard electrolyzers to prevent gas crossover and/or using a relatively short distance between the positive and negative electrodes. Reducing electrical resistance in the electrolysis unit 502 at the expense of complete separation of hydrogen and oxygen by means including one or more of these (but not limited to). Is possible.

The device 500 may include an outlet 504 capable of transporting hydrogen and oxygen produced by the electrolysis unit 502. The outlet section 504 can include a separator 506 that can be used to separate at least a portion of hydrogen from at least a portion of oxygen. In certain embodiments, a semipermeable membrane, such as a polymeric membrane designed for H2 separation, can be utilized as the separator 506. In certain embodiments, the separator 506 may include palladium, palladium alloys, vanadium, niobium, tantalum, and their alloys, and/or other metals and/or hydrogens that are permeable to hydrogen but less permeable to other gases such as oxygen. Alternatively, it may include metal foils including, but not limited to, foils made from alloys. In some embodiments, a separator can be used to separate hydrogen from oxygen so that the hydrogen content of one gas product exiting the separator is enriched to the desired level for oxyhydrogen microorganisms. The gas product can then be transported to the bioreactor and used as a feedstock. In certain embodiments, the hydrogen content of one of the gas products exiting the separator can be set to a level that maximizes oxyhydrogen microbial activity and minimizes the loss of hydrogen produced through electrolyzer 500. ..

The following references are incorporated herein by reference in their entireties for all purposes. US Provisional Patent Application No. 61/328,184 filed April 27, 2010 entitled "Use of Oxyhydrogen Microorganisms for Recovery and Conversion of Non-Photosynthetic Carbon from Inorganic Carbon Source to Useful Organic Compounds" Filed May 12, 2010, entitled "Biochemical process utilizing chemoautotrophic microorganisms for chemical synthetic immobilization of carbon dioxide and/or other inorganic carbon sources to organic compounds and production of other useful products" International Application No. PCT/US2010/001402, and "Chemical synthesis fixation of carbon dioxide and/or other inorganic carbon sources to organic compounds and the production of other useful products by utilizing chemoautotrophic microorganisms. U.S. Patent Application Publication No. 2010/0120104, filed Nov. 6, 2009, entitled Process).

The following examples are intended to illustrate particular embodiments of the present invention and are not intended to exemplify the full scope of the invention.

Example 1
In this example, oxyhydrogen microorganisms accumulating high lipid content and/or other valuable compounds such as polyhydroxybutyrate (PHB) are treated with CO ₂ as a carbon source in the form that oxygen provides an electron acceptor. And grown in mineral medium with hydrogen acting as an electron donor. Such oxyhydrogen microorganisms can be used in certain embodiments of the present invention for the conversion of C1 chemicals such as carbon dioxide into long chain organic chemicals.

A static anaerobic reactor was inoculated with Cupriavidus necator DSM531, which is capable of accumulating a high percentage of cell mass as PHB. DSM medium no. maintained under aerobic conditions of 28 degrees Celsius. Inoculum was obtained from 1 agar plate. Each anaerobic reaction _{vessel, 80% H 2, 10%} CO 2, and liquid medium DSMno of 10ml with 10% _{O 2} in the headspace. Had 81. The culture was incubated at 28 degrees Celsius. The Capriavidus necator reached an optical density (OD) of 0.98 at 600 nm and a cell density of 4.7×10 ⁸ cells/ml after 8 days.

Another proliferation experiment was performed with Capriavidus necator (DSM531). The medium used for growth was Mineral Salt Medium (MSM) formulated by Schlegel et al. MSM medium was formed by mixing 1000 ml of medium A, 10 ml of medium B, and 10 ml of medium C. Medium A contained 9 g/l Na ₂ HPO ₄ . _{12H 2 O, 1.5g / l KH} 2 PO 4, 1.0g / l, 0.2g / l MgSO 4. Included 7H ₂ O, and 1.0 ml trace element medium. The trace element medium was 1000 ml distilled water, 100 mg/l ZnSO ₄ . _{7H 2 O, 30mg / l MnCl} 2. 4 H ₂ O, 300 mg/l H ₃ BO3, 200 mg/l COCl ₂ . 6H ₂ O, 10 mg/l CuCl ₂ . _{2H2O, 20mg / l NiCl2.6H 2 O} , and 30mg _/ l Na 2 _MoO 4. It contained 2H ₂ O. Medium B contained 100 ml distilled water, 50 mg ferric ammonium citrate, and 100 mg CaCl ₂ . Medium C contained 100 ml distilled water and 5 g NaHCO ₃ .

The culture was grown in 20 ml MSM medium in a closed serum vial with a 150 ml lid with the following gas mixture in the headspace: 71% hydrogen, 4% oxygen, 16% nitrogen, 9% carbon dioxide. Headspace pressure was 7 psi. The culture was grown for 8 days at 30 degrees Celsius. The Capriavidus necator reached an OD of 0.86 at 600 nm.

It is known that faster growth rates and higher cell densities can be reached in larger scale bioreactor devices. Therefore, it is believed that higher growth rates and cell densities may be achieved simply by scaling up the system described above. For example, Alcaligenes eutrophus (Alcaligenes eutrophus), Ralstonia eutropha (Ralstonia eutropha), Hidorogenomonasu eutropha (Hydrogenomona eutropha) Cupriavidus - also known as Nekatoru (Cupriavidus necator) and the bioreactor based on _{H 2 /} CO 2 _{/ O} 2 Up to a cell density of more than 90 grams/liter [Tanaka, Ishizaki; Biotech. And Bioeng. , Vol. 45, 268-275 (1995)], and with a doubling time of less than 2 hours [Ammann, Reed, Durichek, Appl. Microbio. , (1968) 822-826].

In this specification, certain preferred embodiments of the invention have been described in sufficient detail to enable those skilled in the art to practice the full scope of the invention. However, many possible variations of the invention not specifically described are still considered to be within the scope of the invention and the appended claims. Therefore, these descriptions provided herein are merely added as examples and are not intended to limit the scope of the invention in any way. More generally, one of ordinary skill in the art would appreciate that all parameters, dimensions, materials, and configurations described herein are considered exemplary and that actual parameters, dimensions, materials, and/or It will be readily appreciated that the construction will depend on the particular application or applications for which the teachings of the invention are used. One of ordinary skill in the art would know, and be able to ascertain, many equivalent forms to the particular embodiments of the invention described herein without departing from routine experimentation. .. Accordingly, the embodiments described above are provided by way of example only, and the invention may be practiced otherwise than as specifically described and claimed within the scope of the appended claims and equivalents thereof. Please understand what you can do. The present invention is directed to each individual feature, system, article, material, kit, and/or method described herein. In addition, any combination of two or more such features, systems, articles, materials, kits, and/or methods may be the combination of such features, systems, articles, materials, kits, and/or methods with each other. If not inconsistent, it is included in the scope of the present invention.

As used in this specification and claims, the indefinite articles "a" and "an" are to be considered to mean "at least one" unless explicitly stated to the contrary.

As used in the specification and claims, the expression "and/or" refers to "one or both" of the elements so conjoined, that is to say in some cases concatenated. It shall be considered to mean an element that is present and that is otherwise present separately. In other instances, other than the elements specifically identified by the phrase "and/or", whether or not related to the specifically identified elements, unless expressly specified to the contrary May exist. Thus, for example, the reference term "A and/or B" when used in combination with an open-ended language such as "comprising", in one embodiment, is not A but A (and optionally B (Including elements other than A), in other embodiments B instead of A (optionally including elements other than A), and in yet other embodiments both A and B (optionally including other elements), etc. Can mean

As used herein in the specification and in the claims, "or" shall have the same meaning as "and/or" as specified above. For example, when separating listed items, "or" or "and/or" shall be inclusive. That is, some elements or at least one of the listed elements are included, as well as more than one and optionally additional items not listed. Obvious, such as "only one of" or "exactly one of" or "consisting of" as used in the claims Only terms that are not otherwise indicated are meant to include an element or exactly one of the listed elements. Generally, the term "or" as used herein refers to "either", "one of", "only one of", Or, if an exclusive term such as "exactly one of" is prepended, then only an exclusive choice (ie, "one or local rather than both") shall be considered. As used in the claims, "consisting essentially of" shall have its ordinary meaning as used in the field of patent law.

In the claims, as in the case of the above specification, “including”, “including”, “carrying”, “having”, All transitional phrases such as "containing", "including", "holding", etc. shall be open-ended. That is, it is meant to be included without limitation. Only the transitional phrases "consisting of" and "consisting essentially of" shall be closed or semi-closed transitional phrases, respectively.

Claims (40)

A biochemical process for the recovery and conversion of inorganic carbon compounds and/or organic compounds containing only one carbon atom into organic chemicals, comprising:
Introducing an inorganic carbon compound and/or an organic compound containing only one carbon atom into an environment suitable for retaining oxyhydrogen microorganisms and/or capable of retaining an extract of oxyhydrogen microorganisms,
In the environment, at least one chemically synthesized carbon fixation reaction utilizing the oxyhydrogen microorganism and/or a cell extract containing an enzyme derived from the oxyhydrogen microorganism, through the inorganic carbon compound and/or one Converting the organic compound containing only carbon atoms into the organic chemical and/or a precursor thereof,
Including
Electron donors and electrons in which the chemically synthesized immobilization reaction is at least partially chemically and/or electrochemically generated and/or introduced into the environment from at least one external source outside the environment. Such a method driven by chemical and/or electrochemical energy provided by a receptor. The method of claim 1, wherein the inorganic carbon compound comprises carbon dioxide. 3. The method according to claim 1 or 2, wherein the carbon dioxide comprises carbon dioxide gas alone and/or dissolved in a mixture or solution further comprising carbonate ions and/or bicarbonate ions. The method according to any one of claims 1 to 3, wherein the inorganic carbon comprises an inorganic carbon contained in a solid phase. 5. The method according to any one of claims 1 to 4, wherein the organic compound containing only one carbon atom comprises carbon monoxide, methane, methanol, formate, and/or formic acid. Electron donors and/or organic compounds containing only one carbon atom are produced via gasification and/or pyrolysis of organic matter and are provided as syngas to oxyhydrogen microorganisms. The method according to any one of 1. 6. An electron donor and/or an organic compound containing only one carbon atom is produced via methane steam reforming and provided to the oxyhydrogen microorganisms as syngas, 6. The method described in. 8. The method of claim 6 or 7, wherein the ratio of hydrogen to carbon monoxide in syngas is adjusted via a water gas shift reaction prior to delivering the syngas to oxyhydrogen microorganisms. 9. The oxyhydrogen microorganism comprises an oxyhydrogen microorganism selected from one or more of the following categories: purple non-sulfur photosynthetic bacteria, cyanobacteria, and/or green algae. The method described in the section. The method according to any one of claims 1 to 9, wherein the oxyhydrogen microorganism comprises an oxyhydrogen microorganism selected from cyanobacteria and/or green algae. The oxyhydrogen microorganisms are the following genera: Rhodopseudomonas species, Rhodospirillum species, Rhodococcus species, Rhizothioca species. Species, Pseudomonas spp, Hydrogenomomonas spp, Hydrogenogenobacter spp, Hydrogenovibrio spp, Hydrogenovibrio spp, Helicobacter bloc (Xanthobacterium) species, Hydrogenophaga species, Bradyrhizobium species, Ralstonia species, Alcaligenes species, and Variovorax species or Variovorax species , Species of Acidovorax, species of Anabaena, species of Scenedesmus, species of Chlamydomonas, species of Anchistrodesmus, and species of Ankistrodesmus, 10. The method according to any one of claims 1 to 9, comprising an oxyhydrogen microorganism selected from one or more of the species Rhaphidium). The oxyhydrogen microorganisms are the following genera: Rhodospirillum species, Rhizobium species, Thiocapsa species, Hydrogenovibrio ter species, Helicobacter. Species, Xanthobacter species, Hydrogenophaga species, Bradyrhizobium species, Variovorax species, Acidovorax species (Acidovora) Species, Anabaena species, Scenedesmus species, Chlamydomonas species, Anchistrodesmus species, and Raffidium species (Rhaphidium) species The method according to any one of claims 1 to 9, which comprises an oxyhydrogen microorganism selected from two or more. The electron donor is one of the following reducing agents: ammonia, ammonium, carbon monoxide, dithionite, elemental sulfur, hydrocarbons, hydrogen, metabisulfite, nitric oxide, nitrites such as sodium thiosulfate ( Na ₂ S ₂ O ₃ ) or calcium thiosulfate (CaS ₂ O ₃ ), but is not limited thereto. Sulfates such as thiosulfates, sulfides such as hydrogen sulfide, sulfites, and thionic acid. Salts, thionous acid, transition metals or sulfides in the dissolved or solid phase, oxides, chalcogenides, halides, hydroxides, oxyhydroxides, phosphates, sulfates or carbonates, 13. The method of any one of claims 1-12, including but not limited to one or more of the conduction band electrons or valence band electrons in the solid electrode material. The electron acceptor is one of the following: carbon dioxide, oxygen, nitrite, nitrate, ferric ions or other transition metal ions, sulfates, or valence band holes or conduction band positives in the solid electrode material. 14. The method of any one of claims 1-13, comprising one or more of the holes. Prior to the conversion step, electron donors and/or electron acceptors are produced and/or purified from at least one input chemical and/or chemicals produced during the fixing step and/or other industrial processes. 1. One or more chemical pretreatment steps are carried out for recycling from chemicals derived from waste streams from mining, agricultural, sewage or waste generation processes. 15. The method according to any one of 14. After the conversion step, the chemically synthesized organic and/or inorganic chemical products are separated from the process stream produced during the conversion step to produce the product in a form suitable for storage, transportation, and sale. Biomass in a form suitable for storage, transportation, and sale, wherein one or more process steps to be treated, as well as cell masses, are separated from said process stream and recycled to the environment and/or collected. 16. The method of any one of claims 1-15, wherein one or more process steps are performed that process to produce a. The conversion step is followed by one or more process steps of removing waste products and/or impurities and/or pollutants from the process stream produced during the fixing step for disposal. 16. The method according to any one of 16. 18. The method of claim 17, wherein the waste product comprises waste product from the nutrient medium used to maintain the oxyhydrogen reaction. After the conversion step, any unused nutrients and/or remaining after removing the oxyhydrogen cell mass and/or co-products of chemical synthesis and/or waste products or contaminants of the process stream generated during the fixation step. 19. The method according to any one of claims 1-18, wherein one or more process steps are carried out in which the process water is recycled and returned to the environment to support further chemical synthesis. Electron donors and/or electron acceptors are generated or recycled using renewable power sources, alternative power sources, or conventional power sources with low greenhouse gas emissions, and the power sources are photovoltaic, solar 20. The method of any one of claims 1-19, selected from at least one of: wind power, hydroelectric power, nuclear power, geothermal, enhanced geothermal, ocean heat, wave power, and tidal power. The electron donors are as follows: simple substance Fe ⁰ , siderite (FeCO ₃ ), magnetite (Fe ₃ O ₄ ), pyrite or marcasite (FeS ₂ ), pyrrhotite (Fe _(1-x) S( x=0 to 0.2)), iron nickel sulfate ore (Fe,Ni) ₉ S ₈ , purple nickel ore (Ni ₂ FeS ₄ ), pyrite nickel ore (Ni,Fe)S ₂ , arsenopyrite (FeAsS). , Or other iron sulfides, caplin (AsS, ox (As ₂ S ₃ ), cobaltite (CoAsS), rhodochrosite (MnCO ₃ ), chalcopyrite (CuFeS ₂ ), chalcopyrite (Cu ₅ FeS ₄ ). , covellite (CuS), tetrahedral chalcocite _{(Cu 8 Sb 2 S 7)} , enargite _(Cu 3 _AsS 4),砒tetrahedral chalcocite _{(Cu 12 As 4. S 13)} , chalcocite _(Cu 2 S) or other, Copper sulfide, sphalerite (ZnS), sphalerite (ZnS), or other zinc sulfide, galena (PbS), ammonite (Pb ₅ (Sb,As ₂ )S ₈ ), or others Lead sulphide, molybdenum or goethite (Ag ₂ S), molybdenite (MoS ₂ ), goethite ore (NiS), polydymium ore (Ni ₃ S ₄ ), or other nickel sulfide, molybdenum (Sb) ₂ S ₃ ), Ga ₂ S ₃ , CuSe, Cooper ore (PtS), Laura ore (RuS ₂ ), Bragg ore (Pt, Pd, Ni)S, FeCl ₂ natural selected from one or more of 21. A method according to any one of claims 1 to 20, produced from a mineral of origin. The electron donors are: process gas, tail gas, enhanced oil recovery vent gas, biogas, acid mine drainage, landfill leachate, landfill gas, geothermal gas, geothermal sludge or brine, metal contaminants, Mercaptan selected from one or more of gangue, tailings, sulfides, disulfides, methyl mercaptans and dimethyl mercaptans and ethyl mercaptans, carbonyl sulfides, carbon disulfides, alkane sulfonates, dialkyl sulfides, thiosulfates, thiofurans , Thiocyanate, isothiocyanate, thiourea, thiol, thiophenol, thioether, thiophene, dibenzothiophene, tetrathionate, dithionite, thionate, dialkyl disulfide, sulfone, sulfoxide, sulfolane, sulfonic acid, dimethylsulfonio Produced from a pollutant or waste product selected from one or more of propionate, sulfonate ester, hydrogen sulfide, sulfate ester, organic sulfur, sulfur dioxide, and all other sour gases. Item 22. The method according to any one of items 1 to 21. Delivery of reduced equivalents from electron donors to oxyhydrogen microorganisms for one or more chemosynthetic reactions during the immobilization step places absorbed or adsorbed hydrogen electron donors in close proximity to chemoautotrophic organisms Introducing a hydrogen storage material into the environment in the form of a solid carrier medium for microbial growth that facilitates microbial growth, from a poorly soluble electron donor containing electrons in H ₂ gas or solid electrode material to a chemoautotrophic culture medium Introducing electron mediators that help transfer reducing power and electrode materials in the form of solid growth carrier media that facilitate the placement of solid electrons in close proximity to chemoautotrophic organisms directly into the environment 23. The method of any one of claims 1-22, which is kinetic and/or thermodynamically enhanced by one or more of: 24. The method of any one of claims 1-23, wherein the organic chemical comprises a compound having a carbon chain length of C5 to C30. At least one chemical synthesis reaction via a method comprising one or more of the following: accelerated mutagenesis, genetic engineering or modification, hybridization, synthetic biology, and traditional selective breeding. The immobilization of inorganic carbon compounds and/or organic compounds containing only one carbon atom and the production of organic compounds is carried out by modified, optimized or engineered oxyhydrogen microorganisms. The method according to any one of 1. A first tower including an upper portion and a lower portion,
A second tower including an upper portion and a lower portion,
An upper portion of the second column is fluidly connected to an upper portion of the first column, and a lower portion of the second column is fluidly connected to a lower portion of the first column. A bioreactor,
When circulating a liquid between said first and said second column, the construction of such that the volume of gas is substantially constant at the top of said first column and/or said second column and A bioreactor arranged and in which the volume of gas occupies at least about 2% of the total volume of the column in which it is located. 27. The bioreactor of claim 26, wherein the bioreactor contains liquid medium. 27. The bioreactor of claim 26, wherein the bioreactor contains oxyhydrogen microorganisms. In operation, circulating a liquid containing a growth medium between a first column and a second column such that the volume of gas is substantially at the top of said first column and/or said second column. A method of operating a bioreactor, which is constantly maintained and the volume of gas accounts for at least about 2% of the total volume of the column in which it is located. 30. The method of claim 29, wherein the gas volume comprises hydrogen and/or oxygen. 30. The method of claim 29, wherein the gas volume comprises hydrogen. 30. The method of claim 29, wherein the volume of gas comprises about 2% to about 10% of the total volume of the column in which it is located. The first and/or second column comprises an inlet and at least a portion of the gas located at the top of the column is recovered from the volume via the inlet of said first and/or said second column. 30. The method according to claim 29, which is recycled and returned to the first and/or the second column. 30. The method of claim 29, wherein the bioreactor contains oxyhydrogen microorganisms. A chamber constructed and arranged to electrolyze water to produce oxygen and hydrogen;
At least a portion of the oxygen in the stream is separated from at least a portion of the hydrogen in the stream and the hydrogen content of the fluid leaving the separator is used as a feed stream to a reactor containing a culture of oxyhydrogen microorganisms. An outlet section that includes a separator that is constructed and arranged to be suitable for
And an electrolysis device. 36. The electrolyzer of claim 35, wherein the outlet of the electrolyzer is coupled in fluid communication with the bioreactor. 37. The electrolyzer of claim 36, wherein the bioreactor is constructed and arranged for recovery and conversion of inorganic carbon compounds and/or organic compounds containing only one carbon atom into organic chemicals by oxyhydrogen microorganisms. .. A method of operating an electrolyzer, comprising electrolyzing water to produce a first stream containing oxygen and hydrogen; and separating at least a portion of the oxygen from at least a portion of the hydrogen, Producing a second stream relatively rich in hydrogen as compared to one stream,
The process wherein the second stream is suitable as a feed stream to a reactor containing a culture of oxyhydrogen microorganisms. 39. The method of claim 38, comprising feeding a second stream to the bioreactor. 40. The method of claim 39, wherein the bioreactor contains oxyhydrogen microorganisms.