CN102282295A - Process for the production of chemicals - Google Patents

Process for the production of chemicals Download PDF

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CN102282295A
CN102282295A CN2009801545116A CN200980154511A CN102282295A CN 102282295 A CN102282295 A CN 102282295A CN 2009801545116 A CN2009801545116 A CN 2009801545116A CN 200980154511 A CN200980154511 A CN 200980154511A CN 102282295 A CN102282295 A CN 102282295A
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cathode compartment
negative electrode
anode
carbonic acid
microorganism
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R·罗森德尔
K·拉贝
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University of Queensland UQ
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University of Queensland UQ
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Priority claimed from AU2008906519A external-priority patent/AU2008906519A0/en
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    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B3/00—Electrolytic production of organic compounds
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/4618—Devices therefor; Their operating or servicing for producing "ionised" acidic or basic water
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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    • C12M35/00—Means for application of stress for stimulating the growth of microorganisms or the generation of fermentation or metabolic products; Means for electroporation or cell fusion
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    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
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    • C12P7/00—Preparation of oxygen-containing organic compounds
    • C12P7/02—Preparation of oxygen-containing organic compounds containing a hydroxy group
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    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
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    • C12P7/00—Preparation of oxygen-containing organic compounds
    • C12P7/40—Preparation of oxygen-containing organic compounds containing a carboxyl group including Peroxycarboxylic acids
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    • C12P7/00—Preparation of oxygen-containing organic compounds
    • C12P7/62—Carboxylic acid esters
    • C12P7/625—Polyesters of hydroxy carboxylic acids
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/20—Indirect fuel cells, e.g. fuel cells with redox couple being irreversible
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    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/4618—Devices therefor; Their operating or servicing for producing "ionised" acidic or basic water
    • C02F2001/4619—Devices therefor; Their operating or servicing for producing "ionised" acidic or basic water only cathodic or alkaline water, e.g. for reducing
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Abstract

A process for producing one or more chemical compounds comprising the steps of providing a bioelectrochemical system having an anode and a cathode separated by a membrane, the anode and the cathode being electrically connected to each other, causing oxidation to occur at the anode and causing reduction to occur at the cathode to thereby produce reducing equivalents at the cathode, providing the reducing equivalents to a culture of microorganisms, and providing carbon dioxide to the culture of microorganisms, whereby the microorganisms produce the one or more chemical compounds, and recovering the one or chemical compounds.

Description

Be used to produce the method for chemical
Technical field
The present invention relates to be used to produce the method for chemical.More specifically, the present invention relates to use the bioelectrochemistry system to produce the method for chemical.
Background technology
The consumption of fossil fuel resource and recognize that day by day artificial effect may drive people to the influence that climate change causes just more and more and reduce greenhouse gas emission and the more continuable society of development in the global range with increasing.Except reproducible electric energy, such sustainable society also needs the fuel and the chemical that obtain to produce renewablely.In order to reach real renewable, need be from reproducible starting material biological example matter or from waste product for example waste water and/or these chemical of carbon dioxide generating.
The bioelectrochemistry system has appearred recently, for example microbiological fuel cell and microorganism electrolysis cell, and described bioelectrochemistry system is used to produce the technology that the potential of the energy and product is paid close attention to.The bioelectrochemistry system is based on and uses the electrochemical activity microorganism, and it can anode provide electronics or can accept electronics from negative electrode.If the interaction on electrochemical activity microorganism and the anode generation electrochemistry, then this type of electrode is known as the biological anode of biological anode (biological anode), biological anode (bioanode) or microorganism.On the contrary, if the interaction on electrochemical activity microorganism and the negative electrode generation electrochemistry, then this type of electrode is known as the biological-cathode of biological negative electrode (biological cathode), biological-cathode (biocathode) or microorganism.The bioelectrochemistry system be generally considered to be used for from the energy-producing promising WeiLai Technology of organic substance that is present in aqueous waste stream stream (for example waste water) (people such as Rozendal, Trends Biotechnol.2008,26,450-459).Industry, agricultural and domestic waste water contain the dissolved organic substance of removing before need be in being discharged into environment usually.Usually, by the aerobic processing these organic pollutants are removed, aerobic is handled and can be consumed a large amount of electric energy to ventilate.Can carry out electrical coupling with the opposite electrode (negative electrode) that carries out reduction reaction by biological anode and realize the bioelectrochemistry wastewater treatment microorganism.Because this electrical connection the between anode and the negative electrode, can the generating electrodes reaction, electronics can flow to negative electrode from anode.In addition, transfer an electron to electrode (anode) in anodic electrochemical activity microorganism, they are with the organic pollutant oxidation in the aqueous waste stream stream (for example waste water) (and removing thus) simultaneously.The bioelectrochemistry system can be used as fuel cell move (produce electric energy in this case---Rabaey and Verstraete for example, Trends Biotechnol.2005,23,291-298) or as electrolyzer move (in this case, electric energy enters the bioelectrochemistry system---for example, and patent WO2005005981A2).
In 2003, Rozendal and Buisman obtained the electrolytic patent of biocatalysis, but it is the bioelectrochemistry system (WO2005005981, its whole disclosures are incorporated this paper into by the cross reference mode) that is used for from the material production hydrogen of bio-oxidation.But the material that is used for the electrolytic bio-oxidation of biocatalysis for example can be, the dissolved organic substance in the waste water.In their invention, but in Rozendal and Buisman the material importing reactor, anode and negative electrode are provided in the described reactor and have contained close anode (anodophilic) bacterium that is in the aqueous medium bio-oxidation; Apply the voltage of 0.1-1.5 volt between anode and the negative electrode, the pH that keeps aqueous medium simultaneously is between 3-9; And collect hydrogen from negative electrode.
Though hydrogen is the interested chemical that produces at negative electrode, more interested is whether can produce the higher chemical substance of value, for example fuel and chemical.The example of this class A fuel A and chemical comprises, alcohol, for example methyl alcohol, ethanol, propyl alcohol, butanols etc.; Carboxylic acid, for example formic acid, acetate, propionic acid, butyric acid, lactic acid etc.; Biological polymer, for example Poly-(PHB) or the like.Yet, in order to need the high-grade catalyst mechanism in the generation reaction of this class complexity of cathode catalysis.Can develop chemical catalyst for this purpose, very complicated and very expensive but these chemical catalysts may become, because they may need to use precious metal.Alternately, can use close negative electrode (cathodophilic) microorganism to come the catalytic cathode reaction to produce valuable chemical.Parent's cathode microbial is such microorganism: it can interact with negative electrode: accept electronics or cathodic reaction product (for example hydrogen or reductive electron mediator) and utilize them to produce valuable chemical from negative electrode.This type of electrode is known as the biological-cathode of biological negative electrode, biological-cathode or microorganism.Electronics and cathodic reaction product (for example hydrogen or reductive electron mediator) are commonly referred to as reducing equivalent (reducing equivalent).Reducing equivalent allows the reduction electron acceptor(EA) and can be used as the electron donor of microbial metabolism.Electron mediator is the organic compound that redox active is arranged, and is well known by persons skilled in the art.They comprise compound for example quinone, toluylene red, methyl viologen etc.Electron mediator shuttles back and forth between electrode and microorganism.In this shuttled back and forth process, electron mediator continued to be reduced by electrode and subsequently again by microbiological oxidation, to produce chemical products.
The biological-cathode that has proved microorganism is used for oxygen reduction, and (for example, people such as Rabaey, ISME are J.2008,2,1387-1396), nitrate reduction (for example, people such as Clauwaert, Environ.Sci.Technol., 2007,41,7564-7569), dechlorination (for example, people such as Aulenta, Environ.Sci.Technol., 2007,41,2554-2559), the generation of hydrogen (for example, people such as Rozendal, Environ.Sci.Technol., 2008,42,629-634), generation (for example, people such as Clauwaert, Water Sci.Technol. with methane, 2008,57,575-579), be not used to produce aforesaid those more complicated molecules but describe it as yet.
Generally speaking, blended microorganisms cultures (being a plurality of species) can not be in large quantities, produce complicated chemical with high density or purity, because the natural end products in the blended microorganisms cultures is simple molecules normally, for example, under anaerobic be methane; Under aerobic conditions, be carbonic acid gas.Therefore, in practice, complicated molecule normally produces with the microorganisms cultures of determining, for example pure microorganisms cultures (being single species) or be completely specified coculture (that is two or more careful species of selecting) at least.Therefore, unless can suppress methanogenic activity, otherwise the biological-cathode that can produce the microorganism of complicated molecule also needs the microorganisms cultures (people such as Rozendal of the close cathode microbial determined, Trends Biotechnol.2008,26,450-459), this close cathode microbial can not be from for example enrichment natively the waste water of the inoculum of complexity.The microorganisms cultures of the close cathode microbial of determining should be through careful select or genetically engineered pure culture, but also can be the coculture of the careful selection of two or more careful pure growths that select or genetic modification.These pure growths or coculture should be made up of the microbial species that can catalysis produces the reaction of required complicated molecule.
Using the shortcoming of the culture of determining of close cathode microbial is that these cultures are easy to by other microbial contamination.So, unless can suppress these other microbic activity, these other microorganisms will be decomposed the product by the culture of the determining generation of close cathode microbial, limit the product output of bioelectrochemistry system thus.Can the bioelectrochemistry system be prevented by other microbial contamination by between anode and negative electrode, using ion-exchange membrane.Using of ion-exchange membrane makes negative electrode separate with the rest part of bioelectrochemistry system, and can make the culture of determining of close cathode microbial be difficult for contaminated.Further reason is: reducing equivalent is the microorganism that sterilely is delivered to close negative electrode basically, and its form is for being sent and come from first the form of anodic electronics by negative electrode.
Under the situation of microbiological fuel cell, people such as Torres (people such as Torres, Environ.Sci.Technol., 2008,42,8773-8777) a kind of method that is used for reducing the anode of microbiological fuel cell and the pH difference between the negative electrode has been proposed: between cathode compartment, place anion-exchange membrane and apply the carbonic acid gas platinum catalyst of oxygen (be used to reduce) to gaseous cathode.This carbonic acid gas and hydroxide ion reaction also form the carbonate kind.This can reduce the pH of negative electrode, and the carbonate kind also can be crossed over anion-exchange membrane to anode and increase the latter's pH from cathodic migration.Thereby reduce the pH difference between the two.
Summary of the invention
Aspect first, the invention provides the method that is used to produce one or more chemical compounds, comprise the following steps: to provide bioelectrochemistry system with the separated anode of tunicle and negative electrode, described anode and negative electrode are electrically connected to each other; Reduce in anode generation oxidation and at negative electrode, thereby produce reducing equivalent at negative electrode; Described reducing equivalent is provided and provides carbonic acid gas to microorganisms cultures to microorganisms cultures, thus one or more chemical compounds of described microorganisms; With described one or more chemical compounds of recovery.
In yet another aspect, the invention provides the method that is used to produce one or more chemical compounds, comprise the following steps: to provide bioelectrochemistry system with the separated anode of tunicle and negative electrode, described anode and negative electrode are electrically connected to each other, and described system has the microorganism that is provided at one or more chemical compounds of formation in the described cathode compartment in cathode compartment and the described cathode compartment; Reduce in anode generation oxidation and at negative electrode, wherein provide carbonic acid gas to described cathode compartment, and one or more chemical compounds of described microorganisms; With reclaim described one or more chemical compounds from described cathode compartment.
In some embodiments, described system also comprises power supply in circuit.Described power supply can comprise the DC power supply, for example battery or DC to AC transmodulator.
Power supply can be used for applying voltage to system, and it increases chemical production speed.The voltage that puts between anode and the negative electrode by power supply can be 0-10V, preferred 0-1.5V, more preferably 0-1.0V.This volume current density that can produce in the bioelectrochemistry electrolyzer is 0-10,000A/m 3The bioelectrochemistry electrolyzer, preferred 10-5,000A/m 3The bioelectrochemistry electrolyzer, more preferably 100-2500A/m 3The bioelectrochemistry electrolyzer, and/or area is 0-1 than current density, 000A/m 2The film surface-area, preferred 1-100A/m 2The film surface-area, more preferably 2-25A/m 2The film surface-area.
In embodiments of the present invention, be present in reducing equivalent and the carbonic acid gas that microorganism in the cathode compartment or accept reducing equivalent from cathode compartment utilizes negative electrode to produce and produce organic molecule.Therefore, carbonic acid gas is fed to microorganism as carbon raw material, and described microorganism is accepted reducing equivalent or is present in the cathode compartment from negative electrode.In fact, carbonic acid gas can be the unique carbon raw material composition that provides to described microorganism.In other embodiments, microorganism utilizes the chemical that carbonic acid gas and other organic substance produce to be needed.In this case, the example of suitable microorganism comprises chemoautotrophic bacteria.For example, when forming butanols, the chemoautotrophic bacteria of negative electrode will carry out according to following formula:
4CO 2+24H ++24e -→C 4H 9OH+7H 2O (2)
To recognize: utilize carbonic acid gas to have the desirable effect of minimizing Carbon emission (and therefore reducing greenhouse gas emission) to be converted into the chemical product that needs as carbonaceous material.
In one embodiment, in cathode compartment, provide or comprise definite microorganisms cultures from the microorganism that cathode compartment is accepted reducing equivalent, it comprises the microbial species of one or more selections.In one embodiment, described definite microorganisms cultures comprises the pure microorganisms cultures that contains the single microorganism species.In another embodiment, described definite microorganisms cultures comprises the coculture of two or more careful microbial species of selecting.Select such microbial species: described microbial species produces one or more chemical compounds.Aptly, described microbial species does not form the methane of significant quantity when negative electrode is grown.
Can form or select to comprise the microorganisms cultures of determining of the microbial species of one or more selections by suitable technique arbitrarily well known by persons skilled in the art.
In this embodiment, provide basically the microorganisms cultures of " pure " (in cathode compartment or be used for accepting reducing equivalent) from negative electrode.Select such microorganisms cultures of " pure " basically: one or more chemical compounds that need of described microorganism culturing deposits yields.For example, can select Clostridium carboxidivorans sp.nov. to produce hydrogen (people such as Liou, Int.J.Syst.Evol.Microbiol., 2005 from carbon dioxide generating acetate, ethanol, butyric acid and butanols and negative electrode ground, 55,2085-2091).Keep pure basically state in order to ensure described pure basically microorganisms cultures, any incoming flow that adds in microorganisms cultures should be substantially free of other microorganism.For example, the carbon-dioxide flow that adds in microorganisms cultures also should not contain the microorganism of contaminative.
The carbon-dioxide flow that adds in cathode compartment can be derived from the exhaust flow or the flue gas flow of roasting kiln or boiler.To recognize: this type of exhaust flow that produces from roasting kiln or boiler or the temperature of flue gas flow are very high, therefore, will be aseptic basically (being that they will not contain any contaminative microorganism).These stream can be cooled off simply and joins in the cathode compartment as carbonated incoming flow.If exhaust flow or flue gas flow contain deleterious other material of microorganism in the possible anticathode chamber, should before joining cathode compartment, described other material be removed.To recognize: can only part exhaust flow or flue gas flow be joined in the cathode compartment.
The carbon-dioxide flow that joins in the cathode compartment also can be the biogas that contains the mixture of methane and carbonic acid gas (with other gas of potential).
The carbonic acid gas that joins negative electrode also can be derived from colliery layer or coal seam, and the fluid that wherein will be rich in carbonate is from coal seam suction cathode compartment.
In another embodiment, the microorganism that provides in cathode compartment comprises the non-selected culture of blended, and described method further comprises the following steps: to produce one or more chemical and reclaim described one or more chemical from cathode compartment in cathode compartment, suppress the formation of methane in the cathode compartment simultaneously.Those skilled in the art will appreciate that the non-selected culture of blended comprises methanogen usually, and, do not operate cathode compartment if do not take specific preventive measures, then the product that finally produces from cathode compartment may be a methane.Therefore, in this embodiment, operate cathode compartment in the mode that suppresses methane formation.Can be by following one or the multinomial formation that suppresses methane:
● in cathode compartment, add the active chemical that one or more suppress the chemical of methane formation or suppress methanogen.For example, known 2-monobromethane sulfonate (BES) suppresses the activity of methanogen.Also can use the active chemical of other inhibition methanogen.
● the operation cathode compartment is so that use the short residence time in the cathode compartment.In this case, most methanogen poor growths use the short residence time will suppress the formation or the growth of methanogens in a large number in the cathode compartment in cathode compartment, because they can't obtain time enough fully to be grown to any big number.In this embodiment, can in cathode compartment, frequently or constantly provide fresh cathode compartment fluid.
● at low pH operation cathode compartment, for example below 5.5, below the preferred pH5.
● regularly cathode compartment is exposed to air or oxygen.
In one embodiment, provide CO by spreading or transporting to cathode compartment from the anode of bioelectrochemistry system 2This transportation can be undertaken by crossing over the film that separates anode and negative electrode, is perhaps undertaken by other pipeline.
In one embodiment, can operate the present invention with biological anode and biological-cathode.In the embodiment of operating as anode with biological anode, one of product that may form in biological anolyte compartment is a carbonic acid gas.This carbonic acid gas can be as the raw material of cathode compartment.This carbonic acid gas can for example separate and be transported to subsequently negative electrode from the anode effluent.
In the embodiment of operating as anode with biological anode, can with waste streams for example waste water stream as joining the anodic charging.Then, anodic reaction is by microorganism electrochemical activity microorganism catalysis for example, and produces electronics (e -) and proton and/or carbonic acid gas and/or other oxidation products (for example sulphur):
Organic (or inorganic) material → x HCO 3 -+ y H ++ z e -+ other product (3)
Anode can be positioned at the anolyte compartment, and anolyte compartment and cathode compartment are separated by film.In the anolyte compartment, the organic and/or inorganic components in the waste streams is oxidized to discharge electronics, and electronics flows to negative electrode by electrical connection then.
In one embodiment, anion-exchange membrane is separated anolyte compartment and cathode compartment.Anion-exchange membrane is well known by persons skilled in the art, comprises for example AMI-7001 (Membranes International) of film, Neosepta AMX (ASTOM Corporation), and fumasep
Figure BDA0000075646630000071
(fumatech).
In some embodiments, in cathode compartment, form bicarbonate ion, move to the anolyte compartment by anion-exchange membrane subsequently.This can be favourable, because also obtained the pH control in the cathode compartment by add carbonic acid gas in cathode compartment.In this embodiment, carbonic acid gas is used to produce chemical compound as raw material as tectonic block, and is used for the pH of control cathode chamber.To understand: can produce hydroxide ion by the reaction that takes place at negative electrode.Hydroxide ion can react to form bicarbonate ion with carbonic acid gas, and this bicarbonate ion can pass through anion-exchange membrane then.In this way, undesirable pH increase in the cathode compartment (it has the potential possibility of kill microorganisms culture) can be avoided, and the running balance condition in the cathode compartment can be kept.Carbonic acid gas apply the salt concn that can significantly not increase in the cathode compartment.This is favourable, can reach dynamic balance state in the bioelectrochemistry system because this means.
In another embodiment, the film of separation anode and negative electrode comprises porous-film.Porous-film can allow liquid and ion from wherein passing through, but stops microorganism from wherein passing through.In one embodiment, can operate anode with biological anode, waste streams for example waste water stream can be as joining the anodic raw material.As mentioned above, the aperture of porous-film can be enough little of to stop microorganism to pass through film.These films are well known by persons skilled in the art, and comprise micro-filtration and ultra-filtration membrane.In course of normal operation, liquid enters cathode compartment from anode by porous-film.The hydroxide ion reaction that the proton that produces according to reaction formula (3) at anode enters cathode compartment and produced according to formula (4) and cathodic reaction by the film transportation:
H ++OH -→H 2O (4)
The result is: the undesirable pH in the cathode compartment raises and is able to Be Controlled, need not to apply in cathode compartment acid.It is stable that pH in the cathode compartment and salt concn keep, and keep running balance.Dissolved or gasiform CO 2Can be along with fluid is transferred to negative electrode from anode.
In another embodiment, the present invention can only operate with biological-cathode.In this embodiment, anode can comprise conventional basically anode.In this embodiment, can provide acid solution (for example sulfuric acid) in the anode chamber, anodic reaction can be the reaction (for example from water generates oxygen) that produces proton.Film can comprise cationic exchange membrane.Cationic exchange membrane is well known by persons skilled in the art, and comprises for example CMI-7000 (Membranes International) of film, Neosepta CMX (ASTOM Corporation),
Figure BDA0000075646630000081
FKB (Fumatech) and Nafion (DuPont).In this embodiment, proton moves by cationic exchange membrane, and the hydroxide ion that is produced with cathodic reaction reaction.The result is: need not to apply acid in cathode compartment, and the pH in the cathode compartment and salt concn keep stable, and keep running balance.
In another embodiment, be used to provide the reductive current source of negative electrode from the light anode.The light anode is well known by persons skilled in the art, and it is caught sunlight and will go back proper energy and is transferred to circuit.
In another embodiment, being used to of being provided drives current source that biochemicals produces from renewable energy source, for example sun power, water energy or other energy well known by persons skilled in the art.
In another embodiment, the film of separation anode and negative electrode comprises bipolar membrane.Bipolar membrane is well known by persons skilled in the art, and comprise film for example NEOSEPTA BP-1E (ASTOM Corporation) and
Figure BDA0000075646630000091
FBM (Fumasep).Bipolar membrane is formed by being positioned at the vertical cationic exchange layer of anionresin layer, and depends on following principle: be proton and hydroxide ion according to formula (5) with water decomposition between the ion exchange layer of film:
H 2O→H ++OH - (5)
In using the embodiment of bipolar membrane as the film of bioelectrochemistry system, the anionresin layer is towards the anolyte compartment, and the cationic exchange layer is towards cathode compartment.When electric current flowed, water diffused between the layer of bipolar membrane and is broken down into proton and hydroxide ion.Hydroxide ion enters anolyte compartment, the proton that produces in the anodic reaction of their offset types (3) there by the migration of anionresin layer; And proton enters cathode compartment by the migration of cationic exchange layer, and they offset the hydroxide ion (or proton consumption) that produces in the cathodic reaction there.The result is: need not to apply acid in cathode compartment, and the pH in the cathode compartment and salt concn keep stable, and keep running balance.
In yet another embodiment of the present invention, the anodic effluent for example can be transported to gas and carry post or film unit to reclaim gaseous carbon dioxide.This carbonic acid gas can be used as gas and provides to negative electrode.
In the variant of above embodiment, can flow through film unit to allow separating carbon dioxide from the anode effluent from the anodic effluent, described film unit has liquid fluid at the opposite side of film.In this way, separated carbonic acid gas can enter in the fluidic solution of opposite side of film.Can provide carbonic acid gas to negative electrode with solubilized form.The fluid of film unit of opposite side of anode fluid of flowing through can be a cathode fluid.
In another embodiment, the anode effluent can betransported by film unit and flow to second fluid with the organic composition that allows carbonic acid gas and anode effluent.For example, can betransported from the effluent of fermentation reactor and to pass through anode, the anodic effluent can betransported and pass through film unit, there, except carbonic acid gas, lipid acid for example propionic acid, butyric acid and other lipid acid well known by persons skilled in the art is hunted down by film and in second fluid.Can there organic reduction can take place with this fluid transport to negative electrode.In this embodiment, carbonic acid gas and other organic substance are provided for by the raw material of microbial transformation for the chemical product of needs.
In one embodiment, provide the generation of organic molecule to negative electrode with auxiliary biochemicals.The example of this type of organic molecule has: glycerine, glucose, lactic acid, butyric acid and other molecule well known by persons skilled in the art.Can add these compounds and think that microorganism provides the source that forms Triphosaden (ATP), this can promote the generation of microorganism growth and product.
Under the situation of adding glycerine, the product of formation can comprise 1, ammediol or butanols.Can add glycerine to cathode compartment, add anolyte compartment or the two to.Also can before entering the bioelectrochemistry system glycerine (partly) be converted into propionic acid, the form with the mixture of glycerine and propionic acid is added to negative electrode then.
In one embodiment, the process of the microorganism in cathode compartment genetic modification is to accept electronics from negative electrode.The example of modifying comprises: add hydrogenase, cytopigment, transpeptidase (sortase) and other enzyme complex in cell.Perhaps, can provide conductive structure to negative electrode, nano wire for example is so that microorganism is connected with cathodic electricity.
In another embodiment, can in cathode fluid, add redox mediators, be transported to microorganism from negative electrode to allow electronics.The example of redox mediators has methyl viologen, toluylene red, azophenlyene methane amide, amino black and other amboceptor well known by persons skilled in the art.In some embodiments, redox is shuttled back and forth allow to increase NADH/NAD in the microorganism pond +Ratio, this can drive the generation of reductive molecule.
In some embodiments of method of the present invention, can in cathode compartment, form the mixture of the chemical that needs.In this type of embodiment, the present invention also comprises the following steps: to discharge from cathode compartment the mixture of chemical compound, and is two or more streams with the mixture separation of described chemical compound.Known arbitrarily other isolation technique that can use for example ion-exchange of known separation techniques, liquid-liquid extraction, absorption, absorption, gas stripping, distillation, reverse osmosis, membrane sepn, low temperature separation process or be suitable for those skilled in the art is come the mixture of separation chemistry compound.In some embodiments, one or more chemical compounds can react and be easier to the another kind of chemical compound removed with formation from remaining chemical compound.In some embodiments, one or more chemical compounds that form in the cathode compartment can comprise solid chemical compound.In this type of embodiment, can use the solid/liquid separation technology of any appropriate, comprise centrifugal, filtration, sedimentation, clarification, flotation etc.In other embodiments, one or more chemical compounds that form in the cathode compartment can comprise gaseous compound.In this type of embodiment, can collect product easily by the using gas collection device, for example use gas-liquid trap well known by persons skilled in the art.
In some embodiments of the present invention, the microorganisms cultures of packing in the cathode compartment.Microorganisms cultures is the part of the aqueous mixture in the cathode compartment normally.In other embodiment of the present invention, microorganisms cultures is grown at electrode surface.In other embodiment of the present invention, the part of packing in cathode compartment microorganisms cultures, another part microorganisms cultures is grown at electrode surface.
In some embodiments of the present invention, cathode compartment can comprise first Room that holds negative electrode, and described first Room comprises that redox shuttles back and forth; Also comprise second Room of containing one or more microorganisms, wherein said redox is shuttled back and forth and is reduced in first Room, and the reductive redox shuttled back and forth to be provided to second Room, and the microorganism that comprises in second Room utilizes described reductive redox to shuttle back and forth as electron donor to promote the formation of one or more chemical.The reductive redox redox that is converted into oxidation in second Room of shuttling back and forth is shuttled back and forth.The redox of oxidation is shuttled back and forth and can be back to first Room.
Can use the example of the chemical compound that the present invention forms to comprise:
---alcohol, for example methyl alcohol, ethanol, propyl alcohol, butanols, isopropylcarbinol etc.;
---carboxylic acid, for example formic acid, acetate, propionic acid, butyric acid, lactic acid etc.;
---glycol, for example 1, ammediol and 1,2-propylene glycol;
---biological polymer, for example Poly-(PHB) etc.;
---any organic chemicals that other can be under the situation that has or do not exist organic chemicals produces from carbonic acid gas and reducing equivalent by microorganism.
Description of drawings
Fig. 1 has shown the synoptic diagram of the bioelectrochemistry system that is suitable for embodiments of the present invention.
Fig. 2 has shown the synoptic diagram of the equipment that is suitable for another embodiment of the invention.
Fig. 3 has shown the synoptic diagram of the equipment that is suitable for another embodiment of the invention.
Fig. 4 has shown the synoptic diagram of the equipment that is suitable for another embodiment of the invention.
Accompanying drawing describes in detail
To recognize: it is in order to explain preferred implementation of the present invention that accompanying drawing is provided.Therefore, will understand: the present invention should not be considered to be limited to the feature that shows in the accompanying drawing.
Show among Fig. 1 bioelectrochemistry system 10 comprise anolyte compartment 12 and cathode compartment 14.Anolyte compartment 12 comprises anode 16.Cathode compartment 14 comprises negative electrode 18.Anode and negative electrode are electrically connected by circuit 20 each other, and circuit 20 comprises power supply 22.Separate by anion-exchange membrane 24 and cathode compartment 14 anolyte compartment 12.
Cathode compartment 14 comprises microorganisms cultures (schematically being shown as ellipse or circular 17 and 19 in Fig. 1).In embodiment shown in Figure 1, microorganisms cultures comprises definite culture.The microorganisms cultures of determining of the microorganism of parent's negative electrode should be through careful pure culture that select or genetic modification, but also can be that two or more are through the careful coculture of selecting of the process of careful pure growth that select or genetic modification.These pure growths or coculture should be made up of the microbial species that can catalysis produces the reaction of the complicated molecule that needs.Microorganisms cultures in the cathode compartment 14 is contained in aqueous medium (seeing numerical markings 17) and/or is attached on the electrode (sees numerical markings 19).
Gas inlet 26 and pneumatic outlet 28 are provided in the cathode compartment 14.The stream that will contain carbonic acid gas joins gas inlet 26, and unnecessary gas is discharged by pneumatic outlet 28.The stream that contains carbonic acid gas that joins in the cathode compartment is the stream that contains aseptic carbonic acid gas, does not promptly contain the contaminative microorganism.This type of a kind of possible source of containing the stream of carbonic acid gas is the exhaust flow from boiler or smelting furnace.This type of exhaust flow leaves pyritous boiler or smelting furnace, therefore, does not contain microorganism (microorganism will be killed by the high temperature in the exhaust flow).Exhaust flow can be cooled off (carry out in the mode of in air-flow, not introducing any contaminative bacterium, for example use indirect heat exchange), join subsequently in the cathode compartment 14.
Liquid from cathode compartment 14 circulates by fluid pipeline 30.Pump 32 is used to keep this liquid circulation.Separator 34 is used to separate the valuable product from liquid, and reclaims valuable product at 36 places.The character of separator will be by valuable product decision to be separated from liquid.Those skilled in the art will readily appreciate that the suitable separator that how to be designed for formed every kind of product.
Fig. 2 has shown the synoptic diagram that is suitable for substituting equipment of the present invention.The equipment that shows among Fig. 2 comprises the anolyte compartment 112 of containing anode 116.This equipment also comprises the cathode compartment 114 that contains negative electrode 118.Film 124 is separated anolyte compartment and cathode compartment.The circuit 120 that comprises power supply 122 (form of DC power supply, for example battery or AC to DC transmodulator) makes anode 116 be electrically connected with negative electrode 118.
This equipment also comprises independent container 130.Container 130 has inlet 132, carbonic acid gas and oxygen can be provided or comprise the gas of oxygen by this inlet.Can oxygen and carbonic acid gas be transported to chamber 114 by pipeline 134.Pipeline 136 is back to container 130 with fluid and unnecessary gas.Can also provide aqueous medium in the container 130, carbonic acid gas and oxygen can be dissolved in the described aqueous medium, and the aqueous medium that contains carbon dioxide dissolved and oxygen is transported to cathode compartment 114.
Fig. 3 has shown the synoptic diagram that is suitable for substituting equipment of the present invention.The equipment that shows among Fig. 3 comprises the anolyte compartment 212 of containing anode 216.This equipment also comprises the cathode compartment 214 that contains negative electrode 218.Film 224 is separated anolyte compartment and cathode compartment.The circuit 220 that comprises power supply 222 (form of DC power supply, for example battery or AC to DC transmodulator) makes anode 216 be electrically connected with negative electrode 218.
Equipment shown in Figure 3 also comprises other container 230.Container 230 has inlet 232 and enters container 230 to accept carbonic acid gas.In embodiment shown in Figure 3, redox is shuttled back and forth and is reduced in cathode compartment 214.By pipeline 236 redox being shuttled back and forth provides to outside cabin 230.Microorganisms cultures in the container 230 uses the reductive redox to shuttle back and forth as electron donor with reducing carbon dioxide.Then, oxidized redox is shuttled back and forth and is back to cathode compartment 214 by pipeline 238.
Fig. 4 has shown the synoptic diagram that is suitable for substituting equipment of the present invention.The equipment that shows among Fig. 4 comprises the anolyte compartment 312 of containing anode 316.This equipment also comprises the cathode compartment 314 that contains negative electrode 318.Film 324 is separated anolyte compartment and cathode compartment.The circuit 320 that comprises power supply 322 makes anode 316 be electrically connected with negative electrode 318.
This equipment also comprises container 330, and it has inlet 332 with to wherein providing oxygen (with other carbonic acid gas, if desired).Pipeline 350 is transported to cathode compartment 314 with oxygen and carbonic acid gas, and pipeline 352 is back to container 330 with unnecessary oxygen and carbonic acid gas.Oxygen and carbonic acid gas can be used as gas stream or are dissolved in the liquid flow and betransported.
In embodiment shown in Figure 4, produce carbonic acid gas being reflected in the anolyte compartment 312 of anode generation.The outlet 340 of anolyte compartment is discharged from the anolyte compartment and is contained the waterborne liquid of carbonic acid gas, and makes it carry post 342 by gas.Carry in the post at this gas, carbonic acid gas is separated from waterborne liquid.Waterborne liquid is back to anolyte compartment 312 by pipeline 344.The carbonic acid gas of being stripped from is transported to the inlet 334 of container 330 by pipeline 346.Carbonic acid gas in the container 330 and oxygen are transported to cathode compartment 314, and there, the culture of the selection of microorganism is converted into carbonic acid gas other chemical compound.The favourable part of this embodiment is to be hunted down and to be used as the raw material of cathode compartment at the carbonic acid gas that anode forms, thereby has reduced emission of carbon-dioxide.
Embodiment
Embodiment 1: the generation of biological polymer
In this embodiment, use equipment shown in Figure 2, bacterium in the cathode compartment use carbonic acid gas and from the electronics of negative electrode as carbon source and energy, they can produce the biological polymer of Poly-(PHB) form in this case.Mode with the pure growth that keeps bacterium or definite culture provides CO 2Provide oxygen to support synthesizing of PHB.Electronics hydrogen direct or that produce by for example negative electrode arrives bacterium indirectly.If desired, external power source can provide negative electrode required extra also proper energy.
The example of the biology of negative electrode is: hookworm is coveted copper bacterium (Cupriavidus necator) and (was called alcaligenes eutrophus (Alcaligenes eutrophus, or Ralstonia eutropha) in the past.
Embodiment 2: provide also proper energy indirectly to the biology that produces biochemicals.
Use equipment shown in Figure 3 in this embodiment, redox is shuttled back and forth and is reduced in cathode compartment.The redox that is reduced is shuttled back and forth and is transported to outside chamber (can pass through permeable membrane), and microorganism utilizes the redox that is reduced to shuttle back and forth as electron donor with reduction electron acceptor(EA), i.e. CO there 2, and from described CO 2Produce chemical.If desired, external power source can provide negative electrode required extra also proper energy.
Embodiment 3: the CO that huge profit produces with anode 2Drive the reaction of negative electrode
This embodiment carries out in equipment shown in Figure 4.Anode comprises the microorganism that makes the carbon source oxidation.Peel off the CO that is produced in position or in the stripping reaction device externally 2, be transported to cathode compartment then, make cathode compartment can contain the completely specified culture of microorganism or blended culture to form the chemical of needs.
The present invention has presented the cathod system that the biological-cathode that uses microorganism produces complicated molecule, and it has prevented the problem that pH raises and/or the salinity rising is relevant in above-described and undesirable microbial contamination and/or the cathode compartment.

Claims (40)

1. be used to produce the method for one or more chemical compounds, comprise the following steps: to provide the bioelectrochemistry system with the separated anode of tunicle and negative electrode, described anode and negative electrode are electrically connected to each other; Reduce in anode generation oxidation and at negative electrode, thereby produce reducing equivalent at negative electrode; Described reducing equivalent is provided and provides carbonic acid gas to microorganisms cultures to microorganisms cultures, thus one or more chemical compounds of described microorganisms; With described one or more chemical compounds of recovery.
2. the method for claim 1, the microorganism that wherein forms one or more chemical compounds is present in the cathode compartment, and described method comprises: reduce in anode generation oxidation and at negative electrode, wherein provide carbonic acid gas to described cathode compartment, and one or more chemical compounds of described microorganisms; With reclaim one or more chemical from described cathode compartment.
3. the method for claim 1 or claim 2, wherein said bioelectrochemistry system comprises power supply in circuit.
4. each method of claim 1 to 3, wherein carbonic acid gas is fed in the microorganism as carbon raw material, described microorganism is accepted reducing equivalent or is present in the cathode compartment from negative electrode, and carbonic acid gas is the unique carbon raw material composition that provides to described microorganism.
5. each method of claim 1 to 3, wherein carbonic acid gas is as the carbon raw material of microorganism, and described microorganism is accepted reducing equivalent or is present in the cathode compartment from negative electrode, and carbonic acid gas is united other organic substance and utilized to produce chemical by microorganism.
6. each method of aforementioned claim, wherein in cathode compartment, provide or comprise definite microorganisms cultures from the microorganism that cathode compartment is accepted reducing equivalent, it comprises the microbial species of one or more selections.
7. each method of aforementioned claim, wherein said microbial species does not form the methane of significant quantity when negative electrode is grown.
8. each method of claim 1-6, wherein said microorganism comprises the non-selected culture of blended, and described method further comprises the following steps: to produce one or more chemical and reclaim described one or more chemical from cathode compartment in cathode compartment, suppress the formation of methane in the cathode compartment simultaneously.
9. the method for claim 8 is wherein by following one or the multinomial formation that suppresses methane: add one or more and suppress chemical that methane form or the active chemical that suppress methanogen in cathode compartment; The operation cathode compartment is so that use the short residence time in the cathode compartment; At low pH operation cathode compartment, for example below 5.5; Or regularly cathode compartment is exposed to air, oxygen or hydrogen peroxide.
10. each method of aforementioned claim, wherein said bioelectrochemistry system comprises biological anode and biological-cathode.
11. each method of aforementioned claim, one of product that wherein forms in the anolyte compartment is a carbonic acid gas, and this carbonic acid gas is as the raw material of cathode compartment.
12. each method of aforementioned claim, wherein anolyte compartment and cathode compartment are separated by anion-exchange membrane.
13. the method for claim 12 wherein forms bicarbonate ion in cathode compartment, move to the anolyte compartment by anion-exchange membrane subsequently, thus avoid may the cathode compartment of kill microorganisms in pH and/or salinity raise.
14. each method of claim 1-11, the film of wherein separating anode and negative electrode comprises porous-film, and described porous-film allows liquid and ion from wherein passing through, but stops microorganism from wherein passing through.
15. the method for claim 14, wherein operate anode with biological anode, waste streams is as the anodic raw material, in course of normal operation, liquid enters cathode compartment from anode by porous-film, and the proton that produces in anodic reaction enters cathode compartment by the film transportation and reacts according to the hydroxide ion that produces in reaction formula (4) and the cathodic reaction:
H ++OH -→H 2O (4)
Thereby avoid the undesirable pH in the cathode compartment to raise.
16. the method for claim 15, wherein pH in the cathode compartment and salt concn keep stable, and keep running balance.
17. each method of claim 1-9 is wherein only with biological-cathode operation bioelectrochemistry system.
18. the method for claim 17, wherein the anode chamber provides acid solution, and anodic reaction comprises the reaction that produces proton, and film comprises cationic exchange membrane, and proton moves by cationic exchange membrane, and with cathodic reaction in the hydroxide ion reaction that produces.
19. each method of aforementioned claim, the film of wherein separating anode and negative electrode comprises bipolar membrane.
20. the method for claim 19, wherein bipolar membrane is formed by being positioned at the vertical cationic exchange layer of anionresin layer, described anionresin layer is towards the anolyte compartment, and described cationic exchange layer is towards cathode compartment, thereby when electric current flows, water diffuses between the layer of bipolar membrane and is broken down into proton and hydroxide ion, and hydroxide ion enters the anolyte compartment by the migration of anionresin layer, and their offset the proton that produces in anodic reaction there; And proton enters cathode compartment by the migration of cationic exchange layer, and they offset the hydroxide ion (or proton consumption) that produces in the cathodic reaction there.
21. each method of aforementioned claim, wherein the anodic effluent comprises carbonic acid gas and is transported to gas from the anodic effluent and carries post or film unit to reclaim gaseous carbon dioxide, to provide to negative electrode as gas.
22. the method for claim 21, wherein carbonic acid gas is separated with the anode effluent allowing from the anodic effluent film unit of flowing through, described film unit has liquid flow at the opposite side of film, thereby separated carbonic acid gas enters in the fluidic solution of opposite side of film, provides carbonic acid gas with solubilized form to negative electrode.
23. the method for claim 22, the fluid of the film unit of the opposite side of the anode fluid of wherein flowing through comprises cathode fluid.
24. the method for claim 22 wherein the transportation of anode effluent is flow to second fluid by film unit with the organic composition that allows carbonic acid gas and anode effluent, and described second fluid is transported to the reductive negative electrode that organic substance takes place.
25. each method of aforementioned claim, wherein form the mixture of chemical at cathode compartment, and described method also comprises the following steps: to discharge from cathode compartment the mixture of chemical compound, and is two or more streams with the mixture separation of described chemical compound.
26. each method of aforementioned claim, the microorganisms cultures of wherein packing in the cathode compartment, described microorganisms cultures is the part of the aqueous mixture in the cathode compartment, perhaps described microorganisms cultures is grown at electrode surface, and perhaps pack in the cathode compartment part microorganisms cultures and another part microorganisms cultures are grown at electrode surface.
27. each method of aforementioned claim, wherein cathode compartment comprises first Room that holds negative electrode, and described first Room comprises that redox shuttles back and forth; Cathode compartment also comprises second Room of containing one or more microorganisms, wherein said redox shuttles back and forth to be reduced in first Room and the reductive redox shuttled back and forth to be provided to second Room, and the microorganism that comprises in second Room utilizes described reductive redox to shuttle back and forth as electron donor to promote the formation of one or more chemical.
The redox that is converted into oxidation in second Room is shuttled back and forth 28. the method for claim 27, wherein said reductive redox are shuttled back and forth, and the redox of described oxidation is shuttled back and forth and is back to first Room.
29. each method of aforementioned claim, wherein formed chemical compound comprises:
---alcohol, for example methyl alcohol, ethanol, propyl alcohol, butanols, isopropylcarbinol;
---carboxylic acid, for example formic acid, acetate, propionic acid, butyric acid, lactic acid;
---glycol, for example 1, ammediol and 1,2-propylene glycol;
---biological polymer, for example Poly-(PHB).
30. each method of aforementioned claim, wherein formed chemical compound comprises butanols, and described bioelectrochemistry system is included in negative electrode produces butanols according to formula (2) chemosynthetic bacteria:
4CO 2+24H ++24e -→C 4H 9OH+7H 2O (2)。
31. each method of aforementioned claim wherein joins exhaust flow or flue gas flow that carbon-dioxide flow in the cathode compartment is derived from roasting kiln or boiler.
32. each method of aforementioned claim wherein applies 0-10V between anode and negative electrode, preferred 0-1.5V, the more preferably voltage of 0-1.0V; And the volume current density that obtains in the bioelectrochemistry electrolyzer is 0-10,000A/m 3The bioelectrochemistry electrolyzer, preferred 10-5,000A/m 3The bioelectrochemistry electrolyzer, more preferably 100-2500A/m 3The bioelectrochemistry electrolyzer, and/or area is 0-1 than current density, 000A/m 2The film surface-area, preferred 1-100A/m 2The film surface-area, more preferably 2-25A/m 2The film surface-area.
33. each method of aforementioned claim, wherein join carbon-dioxide flow in the cathode compartment and contain the biogas of the mixture that comprises methane and carbonic acid gas, the carbonic acid gas that perhaps joins negative electrode is derived from colliery layer or coal seam, and the fluid that wherein will be rich in carbonate is from coal seam suction cathode compartment.
34. each method of aforementioned claim wherein provides carbonic acid gas from the anodic of bioelectrochemistry system to cathode compartment by diffusion or transportation.
35. each method of aforementioned claim wherein also provides the generation of organic molecule with auxiliary biochemicals to negative electrode.
36. the method for claim 35, wherein said organic molecule is selected from: glycerine, glucose, lactic acid, propionic acid and butyric acid.
37. the method for claim 36, the product that wherein adds glycerine and formation comprises 1, ammediol or butanols, and to cathode compartment or anode chamber or the two interpolation glycerine.
38. the method for claim 37, wherein said glycerine also can part be converted into propionic acid before entering the bioelectrochemistry system, the mixture as glycerine and propionic acid adds negative electrode to subsequently.
39. each method of aforementioned claim is wherein added redox mediators in cathode fluid, be transported to microorganism to allow electronics from negative electrode.
40. the method for claim 39, wherein said redox mediators are selected from methyl viologen, toluylene red, azophenlyene methane amide, amino black or wherein two or more multinomial mixture.
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