US20130126336A1 - Carbon dioxide immobilization unit - Google Patents

Carbon dioxide immobilization unit Download PDF

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Publication number
US20130126336A1
US20130126336A1 US13/805,865 US201113805865A US2013126336A1 US 20130126336 A1 US20130126336 A1 US 20130126336A1 US 201113805865 A US201113805865 A US 201113805865A US 2013126336 A1 US2013126336 A1 US 2013126336A1
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Prior art keywords
carbon dioxide
electrode
immobilization unit
cathode
produced
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Abandoned
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US13/805,865
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English (en)
Inventor
Hideki Sakai
Hiroki Mita
Yuichi Tokita
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Sony Corp
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Sony Corp
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Assigned to SONY CORPORATION reassignment SONY CORPORATION ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: TOKITA, YUICHI, MITA, HIROKI, SAKAI, HIDEKI
Publication of US20130126336A1 publication Critical patent/US20130126336A1/en
Abandoned legal-status Critical Current

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    • C25B3/04—
    • 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
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C25B1/01—Products
    • C25B1/02—Hydrogen or oxygen
    • 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
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • 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
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B3/00—Electrolytic production of organic compounds
    • C25B3/20—Processes
    • C25B3/25—Reduction
    • C25B9/12—
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/30—Cells comprising movable electrodes, e.g. rotary electrodes; Assemblies of constructional parts thereof

Definitions

  • the present invention relates to a carbon dioxide immobilization unit using an oxidoreductase. More specifically, the invention relates to a carbon dioxide immobilization unit producing an organic acid or a carbohydrate from carbon dioxide.
  • Biofuel cells using an oxidoreductase as a reaction catalyst have been attracting an attention as next-generation fuel cells with high capacity and high safety, since the biofuel cells effectively extract electrons from glucose, ethanol, and the like which are not usable in fuel cells using a typical industrial catalyst.
  • FIG. 5 is a diagram schematically illustrating an electric power generation principle of a biofuel cell using an enzyme.
  • glucose in an anode 101 , glucose is decomposed by an enzyme immobilized on a surface thereof to extract electrons (e ⁇ ) and to produce protons (H + ).
  • protons H +
  • a cathode 102 water (H 2 O) is produced from the protons (H + ) transported from the anode 101 through a proton conductor 103 , the electrons (e ⁇ ) transmitted through an external circuit, and oxygen (O 2 ) in, for example, air.
  • oxygen oxygen
  • FIG. 6 is a diagram schematically illustrating an electric power generation principle of a methanol type biofuel cell.
  • a biofuel cell using methanol as a fuel to generate electric power has been proposed in related art (for example, refer to PTL 1).
  • alcohol dehydrogenase (ADH), formaldehyde genase (FalDH), and formate dehydrogenase (FateDH) are immobilized on the surface of the anode 101 .
  • the formic acid produced in the formic acid production section is decomposed into hydrogen and carbon dioxide by a catalyst for formic acid decomposition.
  • Hydrogen produced by this decomposition reaction is used for an arbitrary purpose such as a fuel cell.
  • carbon dioxide as a by-product is transmitted to the formic acid production section to be used for formic acid production.
  • a carbon dioxide immobilization unit includes at least: a first electrode decomposing water to produce protons; a second electrode producing an organic acid or a carbohydrate from the protons produced in the first electrode and carbon dioxide; and a proton conductor transferring the protons produced in the first electrode to the second electrode, in which an oxidoreductase is present on a surface of the first electrode or a surface of the second electrode, or both.
  • a surface of an electrode includes an outer surface of the electrode and an inner surface of a gap in an inside of the electrode.
  • the carbon dioxide immobilization unit may further include a carbon dioxide supply section supplying carbon dioxide to the second electrode.
  • the carbon dioxide supply section may supply a gas containing carbon dioxide in concentration of 0.028 to 100 vol % both inclusive.
  • the carbon dioxide immobilization unit may include an oxygen removal section removing oxygen produced in the first electrode; and a product recovery section extracting the organic acid or the carbohydrate produced in the second electrode.
  • the first electrode may be a dipping type electrode which is directly in contact with a liquid phase or is in contact with the liquid phase with a separator in between
  • the second electrode may be a semi-dipping type electrode which is directly in contact with the liquid phase or is in contact with the liquid phase with a separator in between, as well as is in contact with a vapor phase with a gas-liquid separator film in between.
  • first electrode or the second electrode, or both may be formed of, for example, a conductive porous material.
  • carbon dioxide is allowed to be easily immobilized in the form of an organic acid or a carbohydrate through only inputting electric power to the carbon dioxide immobilization unit without using hydrogen.
  • FIG. 1 is a diagram schematically illustrating a principle of a carbon dioxide immobilization unit according to an embodiment of the invention.
  • FIG. 2 is a diagram schematically illustrating an electrode configuration of an anode 1 illustrated in FIG. 1 which is of a dipping type.
  • FIG. 3 is a diagram schematically illustrating an electrode configuration of a cathode 2 illustrated in FIG. 1 which is of a semi-dipping type.
  • FIG. 4 is a diagram schematically illustrating a principle of a carbon dioxide immobilization unit according to a modification example of the above-described embodiment of the invention.
  • FIG. 5 is a diagram schematically illustrating an electric power generation principle of a biofuel cell using an enzyme.
  • FIG. 6 is a diagram schematically illustrating an electric power generation principle of a methanol type biofuel cell.
  • FIG. 1 is a diagram schematically illustrating a carbon dioxide immobilization unit according to an embodiment of the invention.
  • FIG. 2 is a diagram schematically illustrating an electrode configuration of an anode 1 (a first electrode) which is of a dipping type
  • FIG. 3 is a diagram schematically illustrating an electrode configuration of a cathode 2 (a second electrode) which is of a semi-dipping type.
  • the carbon dioxide immobilization unit according to the embodiment includes the anode 1 and the cathode 2 which are disposed to face each other with a proton conductor 3 in between.
  • an oxidoreductase is present on a surface of the anode 1 or a surface of the cathode 2 , or both, and an organic acid such as formic acid or a carbohydrate such as glucose is produced from carbon dioxide (CO 2 ) by reaction opposite to reaction in a biofuel cell in related art.
  • a surface of an electrode includes an outer surface of the electrode and an inner surface of a gap in an inside of the electrode.
  • the anode 1 In the anode 1 , water (H 2 O) is oxidatively decomposed to produce oxygen (O 2 ) and to extract protons (H + ) and electrons (e ⁇ ). Therefore, the anode 1 adopts a dipping type electrode configuration in which the anode 1 is directly in contact with a liquid phase such as an electrolytic solution 13 including a buffer substance or is in contact with the liquid phase with a separator 14 made of nonwoven or the like in between as illustrated in FIG. 2 . It is to be noted that, in the electrode configuration illustrated in FIG. 2 , the electrolytic solution 13 serves as the proton conductor 3 .
  • An electrode configuring the anode 1 is not specifically limited; however, for example, an electrode including, on a surface of an electrode 11 made of a conductive porous material, an enzyme immobilization layer 12 where an oxidoreductase or the like is immobilized may be used.
  • a conductive porous material used in this case, a known material may be used, and in particular, a carbon-based material such as porous carbon, carbon pellets, carbon felt, carbon paper, or a laminate of carbon fiber or carbon microparticles is suitable.
  • examples of the oxidoreductase immobilized on the surface of the anode 1 include bilirubin oxidase (BOD), laccases, and ascorbate oxidase.
  • an electron mediator may be immobilized, together with the above-described enzyme, on the surface of the anode 1 to decompose water by reaction of the enzyme and the electron mediator.
  • the electron mediator a compound having a quinone skeleton is preferably used, and in particular, a compound having a naphthoquinone skeleton is suitable.
  • 2-amino-1,4-naphthoquinone ANQ
  • 2-amino-3-methyl-1,4-naphthoquinone AMNQ
  • 2-methyl-1,4-naphthoquinone VK3
  • 2-amino-3-carboxy-1,4-naphthoquinone ACNQ
  • the compound having the quinone skeleton in addition to the compound having the naphthoquinone skeleton, for example, anthraquinone or a derivative thereof may be used. Moreover, if necessary, one kind or two or more kinds of other compounds functioning as electron mediators may be immobilized together with the compound having the quinone skeleton.
  • the anode 1 is not limited to an electrode having a surface on which an oxidoreductase is immobilized, and, for example, an electrode to which a microorganism including an oxidoreductase and functioning as a reaction catalyst is attached may be used, as long as the oxidoreductase is present on a surface of the electrode.
  • the cathode 2 adopts an air-exposure type electrode configuration in which an electrode is directly in contact with a vapor phase to allow carbon dioxide to be sufficiently supplied thereto, or a semi-dipping type electrode configuration, as illustrated in FIG. 3 , in which an electrode is in contact with the vapor phase with a gas-liquid separation film 25 in between.
  • the cathode 2 is the semi-dipping type electrode
  • the cathode 2 is also directly in contact with the liquid phase such as the electrolytic solution 13 including the buffer substance, or is also in contact with the separator 24 made of nonwoven in between, as illustrated in FIG. 3 .
  • an electrode including an enzyme immobilization layer 22 on a surface of an electrode 21 made of a conductive porous material may be used.
  • a conductive porous material forming the cathode 2 a known material may be also used, and in particular, a carbon-based material such as porous carbon, carbon pellets, carbon felt, carbon paper, or a laminate of carbon fiber or carbon microparticles is suitable.
  • the enzyme immobilized on the surface of the cathode 2 is allowed to be appropriately selected depending on a product, and, for example, when formic acid is produced, formate dehydrogenase (FDH) may be used. Moreover, when glucose is produced, glucose dehydrogenase (GDH) may be used.
  • FDH formate dehydrogenase
  • GDH glucose dehydrogenase
  • electron transfer enzymes such as hexokinase, glucose phosphate isomerase, phosphofructokinase, fructose bisphosphate aldolase, triosephosphate isomerase, glyceraldehydephosphate dehydrogenase, phosphoglyceromutase, phosphopyruvate hydratase, pyruvate kinase, L-lactate dehydrogenase, D-lactate dehydrogenase, pyruvate dehydrogenase, citrate synthase, aconitase, isocitrate dehydrogenase, 2-oxoglutarate dehydrogenase, succinyl-CoA synthetase, succinate dehydrogenase, fumarase, and malonate dehydrogenase may be usable.
  • known enzymes such as hexokinase, glucose phosphate isomerase, phosphofructokina
  • coenzyme oxidase or an electron mediator is preferably immobilized, together with the enzyme such as FDH, on the surface of the cathode 2 .
  • the enzyme such as FDH
  • coenzyme used in this case include NADH and NADPH, and diaphorase reducing an oxidant thereof (such as NAD + or NADP + ).
  • examples of the electron mediator immobilized together with these enzymes include potassium hexacyanoferrate, potassium ferricyanide, and potassium octacyanotungstate.
  • the cathode 2 is also not limited to an electrode having a surface on which an oxidoreductase is immobilized, and, for example, an electrode to which a microorganism including an oxidoreductase and functioning as a reaction catalyst is attached may be used, as long as the oxidoreductase is present on a surface of the electrode.
  • a vapor-liquid coexistence layer 23 in which a vapor phase and a liquid phase coexist may be further formed on an outer side of the enzyme immobilization layer 22 where the enzyme or the like is immobilized.
  • the proton conductor 3 may be a material not having electronic conductivity and capable of transporting protons (H + ), and an electrolytic solution including a buffer substance is typically used.
  • an electrolytic solution including a buffer substance is typically used.
  • a separator for example, cellophane, nonwoven, or the like
  • a separator having proton conductivity such as an ion-exchange resin film having a fluorine-containing carbon sulfonic acid group may be used as the proton conductor 3 .
  • the carbon dioxide immobilization unit include a carbon dioxide supply section 5 supplying carbon dioxide or a gas containing carbon dioxide to the cathode 2 .
  • the carbon dioxide immobilization unit further include an oxygen removal section 4 removing oxygen produced in the anode 1 , and a product recovery section 6 extracting the organic acid or the carbohydrate produced in the cathode 2 .
  • the configuration of the oxygen removal section 4 is not specifically limited; however, for example, the oxygen removal section 4 may have a configuration in which a solution around the anode 1 is allowed to flow, and deoxidized water is supplied to emit a solution including oxygen.
  • the oxygen concentration in the solution around the anode 1 is allowed to be reduced; therefore, a decline in anode reaction is preventable.
  • carbon dioxide CO 2
  • carbon dioxide or a gas containing carbon dioxide is supplied from the carbon dioxide supply section 5 to the cathode 2 or its surrounding.
  • the gas supplied from the carbon dioxide supply section 5 may be a gas containing carbon dioxide in concentration equivalent to or higher than the concentration of carbon dioxide in air, and, for example, in the case where the concentration of carbon dioxide in air is 0.028 vol %, a gas containing carbon dioxide in concentration of 0.028 to 100 vol % both inclusive may be supplied to the cathode 2 .
  • the concentration of carbon dioxide around the cathode 2 is allowed to be maintained at a high level, and reaction efficiency is allowed to be enhanced.
  • gas supplied from the carbon dioxide supply section 5 to the cathode 2 for example, exhaust from a thermal power station or a vehicle may be used, and dry ice, exhalation, and the like may be also used.
  • a gas containing a high concentration of carbon dioxide is easily obtainable through using such a gas, and the organic acid or the carbohydrate is efficiently obtainable.
  • the configuration of the product recovery section 6 is not specifically limited; however, for example, a method of recovering a product contained in a solution around the cathode 2 through allowing the solution to flow and converting the product into a salt to precipitate the salt, or a method of recovering the product through allowing an absorbent such as activated carbon to absorb the product is applicable.
  • the concentration of the product in the solution around the cathode 2 is allowed to be reduced, thereby preventing a decline in cathode reaction. It is to be noted that, in the case where such a product recovery section 6 is included, it is preferable that the cathode 2 be a semi-dipping type electrode. Therefore, as the solution around the cathode 2 flows, the product is allowed to be immediately removed from the cathode 2 and recovered.
  • water (H 2 O) is oxidized by the oxidoreductase in the enzyme immobilization layer 12 disposed on the surface to extract protons (H + ) and electrons (e ⁇ ).
  • the oxygen removal section 4 allows oxygen (O 2 ) produced by this reaction to exit from the carbon dioxide immobilization unit.
  • the protons (H + ) are transferred to the cathode 2 through the proton conductor 3 , and the electrons (e ⁇ ) are transmitted to the cathode 2 through an external circuit.
  • an organic acid or a carbohydrate is produced from the protons (H + ) and the electrons (e ⁇ ) produced in the anode 1 , and carbon dioxide (CO 2 ) which is supplied from, for example, the carbon dioxide supply section 5 and is present in a vapor phase or a liquid phase in contact with the cathode 2 .
  • the product recovery section 6 allows the organic acid or the carbohydrate produced by this reaction to exit from the carbon dioxide immobilization unit.
  • the organic acid or the carbohydrate is allowed to be easily produced through only inputting electric power to the carbon dioxide immobilization unit without using hydrogen.
  • the carbon dioxide immobilization unit is allowed to immobilize carbon dioxide more efficiently, and a useful carbon compound is obtainable.
  • the carbon dioxide immobilization unit is allowed to immobilize carbon dioxide as a useful compound while using energy (electric power), and has a small and simple configuration; therefore, the carbon dioxide immobilization unit is applicable to a wide range of fields.
  • the carbon dioxide immobilization unit producing formic acid from carbon dioxide is described; however, the present invention is not limited thereto, and the carbon dioxide immobilization unit is allowed to produce a carbohydrate such as methanol or glucose in addition to the organic acid such as formic acid.
  • FIG. 4 is a diagram schematically illustrating a principle of a carbon dioxide immobilization unit according to a modification example of the above-described embodiment. It is to be noted that, in FIG. 4 , like components are denoted by like numerals as of the carbon dioxide immobilization unit according to the first embodiment illustrated in FIG. 1 and will not be further described. As illustrated in FIG. 4 , the carbon dioxide immobilization unit according to the modification example also includes an anode 31 and a cathode 32 which are disposed to face each other with the proton conductor 3 in between.
  • methanol CH 3 OH
  • formic acid is produced from carbon dioxide by formate dehydrogenase (FateDH). Then, the formic acid is converted into formaldehyde by formaldehyde genase (FalDH), and then methanol is produced by alcohol dehydrogenase (ADH).
  • the following reaction proceeds. More specifically, in the anode 31 , water (H 2 O) is oxidized by the oxidoreductase existing on the enzyme immobilization layer 12 disposed on the surface to extract protons (H + ) and electrons (e ⁇ ).
  • the oxygen removal section 4 allows oxygen (O 2 ) produced by this reaction to exit from the carbon dioxide immobilization unit.
  • the protons (H + ) are transferred to the cathode 32 through the proton conductor 3 , and the electrons (e ⁇ ) are transmitted to the cathode 2 through an external circuit.
  • formic acid, formaldehyde, and methanol are produced from the protons (H + ) and the electrons (e ⁇ ) produced in the anode 31 , and carbon dioxide (CO 2 ) which is supplied from, for example, the carbon dioxide supply section 5 and is present in a vapor phase or a liquid phase in contact with the cathode 32 .
  • product recovery sections 36 a to 36 c allow formic acid, formaldehyde, and methanol produced in such a manner, respectively, to exit from the carbon dioxide immobilization unit.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Inorganic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Apparatus Associated With Microorganisms And Enzymes (AREA)
  • Carbon And Carbon Compounds (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)
US13/805,865 2010-07-16 2011-07-08 Carbon dioxide immobilization unit Abandoned US20130126336A1 (en)

Applications Claiming Priority (3)

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JP2010-162130 2010-07-16
JP2010162130A JP2012021216A (ja) 2010-07-16 2010-07-16 二酸化炭素固定化装置
PCT/JP2011/065681 WO2012008376A1 (ja) 2010-07-16 2011-07-08 二酸化炭素固定化装置

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WO (1) WO2012008376A1 (ja)

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102014016894A1 (de) * 2014-11-17 2016-05-19 Gensoric Gmbh Verfahren und Vorrichtung zur Umwandlung gasförmiger Kohlenstoffverbindungen
EP3075884A1 (en) * 2015-03-31 2016-10-05 Wageningen Universiteit System and method for bio-electrochemical water oxidation
CN107250436A (zh) * 2014-11-02 2017-10-13 百奥堪引赛股份有限公司 改进的电化学生物反应器模块及其用途
US10626509B2 (en) 2017-02-02 2020-04-21 Kabushiki Kaisha Toshiba Electrolysis cell and electrolytic device for carbon dioxide
WO2023137278A1 (en) * 2022-01-11 2023-07-20 University Of Maryland, Baltimore Applications of o2-insensitive formate dehydrogenase

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US20180265899A1 (en) * 2017-03-16 2018-09-20 Kabushiki Kaisha Toshiba Carbon dioxide fixation device and fuel production system
JP7355559B2 (ja) 2019-08-28 2023-10-03 住友理工株式会社 燃料電池用ラジカル硬化性シール部材
CN113265670B (zh) * 2021-04-20 2022-11-18 复旦大学 含有支撑薄膜的电解池及电化学系统
JP7207672B1 (ja) 2022-01-18 2023-01-18 飯田グループホールディングス株式会社 蟻酸生成装置

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CN107250436A (zh) * 2014-11-02 2017-10-13 百奥堪引赛股份有限公司 改进的电化学生物反应器模块及其用途
US20170335473A1 (en) * 2014-11-02 2017-11-23 Biocheminsights, Inc. Improved Electrochemical Bioreactor Module and Use Thereof
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DE102014016894A1 (de) * 2014-11-17 2016-05-19 Gensoric Gmbh Verfahren und Vorrichtung zur Umwandlung gasförmiger Kohlenstoffverbindungen
EP3221458A2 (de) * 2014-11-17 2017-09-27 Gensoric GmbH Verfahren und vorrichtung zur herstellung von kohlendioxid
EP3075884A1 (en) * 2015-03-31 2016-10-05 Wageningen Universiteit System and method for bio-electrochemical water oxidation
US10626509B2 (en) 2017-02-02 2020-04-21 Kabushiki Kaisha Toshiba Electrolysis cell and electrolytic device for carbon dioxide
WO2023137278A1 (en) * 2022-01-11 2023-07-20 University Of Maryland, Baltimore Applications of o2-insensitive formate dehydrogenase

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CN102985598A (zh) 2013-03-20
EP2594664A4 (en) 2014-02-26
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EP2594664A1 (en) 2013-05-22
WO2012008376A1 (ja) 2012-01-19

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