WO2012144189A1 - 二酸化炭素の吸着及び放出デバイス - Google Patents
二酸化炭素の吸着及び放出デバイス Download PDFInfo
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- WO2012144189A1 WO2012144189A1 PCT/JP2012/002629 JP2012002629W WO2012144189A1 WO 2012144189 A1 WO2012144189 A1 WO 2012144189A1 JP 2012002629 W JP2012002629 W JP 2012002629W WO 2012144189 A1 WO2012144189 A1 WO 2012144189A1
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- carbon dioxide
- porous body
- release device
- dioxide adsorption
- electrode
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- 0 CC(CC1(C)C)CC(C)(C)*1O Chemical compound CC(CC1(C)C)CC(C)(C)*1O 0.000 description 2
- FKNQCJSGGFJEIZ-UHFFFAOYSA-O Cc1cc[nH+]cc1 Chemical compound Cc1cc[nH+]cc1 FKNQCJSGGFJEIZ-UHFFFAOYSA-O 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1425—Regeneration of liquid absorbents
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- C—CHEMISTRY; METALLURGY
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- C08G73/00—Macromolecular compounds obtained by reactions forming a linkage containing nitrogen with or without oxygen or carbon in the main chain of the macromolecule, not provided for in groups C08G12/00 - C08G71/00
- C08G73/02—Polyamines
- C08G73/026—Wholly aromatic polyamines
- C08G73/0266—Polyanilines or derivatives thereof
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
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- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
- B01J20/205—Carbon nanostructures, e.g. nanotubes, nanohorns, nanocones, nanoballs
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
- B01J20/26—Synthetic macromolecular compounds
- B01J20/262—Synthetic macromolecular compounds obtained otherwise than by reactions only involving carbon to carbon unsaturated bonds, e.g. obtained by polycondensation
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/30—Processes for preparing, regenerating, or reactivating
- B01J20/34—Regenerating or reactivating
- B01J20/3441—Regeneration or reactivation by electric current, ultrasound or irradiation, e.g. electromagnetic radiation such as X-rays, UV, light, microwaves
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/60—Preparation of carbonates or bicarbonates in general
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- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G73/00—Macromolecular compounds obtained by reactions forming a linkage containing nitrogen with or without oxygen or carbon in the main chain of the macromolecule, not provided for in groups C08G12/00 - C08G71/00
- C08G73/06—Polycondensates having nitrogen-containing heterocyclic rings in the main chain of the macromolecule
- C08G73/0622—Polycondensates containing six-membered rings, not condensed with other rings, with nitrogen atoms as the only ring hetero atoms
- C08G73/0627—Polycondensates containing six-membered rings, not condensed with other rings, with nitrogen atoms as the only ring hetero atoms with only one nitrogen atom in the ring
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- C08L79/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing nitrogen with or without oxygen or carbon only, not provided for in groups C08L61/00 - C08L77/00
- C08L79/02—Polyamines
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L79/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing nitrogen with or without oxygen or carbon only, not provided for in groups C08L61/00 - C08L77/00
- C08L79/04—Polycondensates having nitrogen-containing heterocyclic rings in the main chain; Polyhydrazides; Polyamide acids or similar polyimide precursors
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/40—Capture or disposal of greenhouse gases of CO2
Definitions
- the present invention relates to a device capable of electrochemically adsorbing and releasing carbon dioxide.
- Carbon dioxide is a substance widely existing on the earth that occupies 0.04% in the atmosphere, and is a compound widely used in industry. Specific examples of industrial use of carbon dioxide include foaming gas such as carbonated drinks, bath additives, fire extinguishing agents, dry ice for cooling, and air for emergency replenishment of bicycles. Carbon dioxide in a supercritical state is used as an extraction solvent for caffeine, and is also used in a laser used for processing in an industrial field and a carbon dioxide laser used as a medical laser knife. Furthermore, it is used for a CO 2 refrigerant compressor or the like as an alternative to a fluorocarbon refrigerant.
- carbon dioxide is used for carbon dioxide fertilization to accelerate the growth of plants such as forcing cultivation of strawberries and aquatic plants in ornamental aquariums, and also used for CA storage (controlled atomosphere storage) of fresh produce. Yes.
- Patent Document 1 a compression adsorption technique for compressing and adsorbing carbon dioxide using zeolite, Or the thing which adsorb
- the present invention has been made in view of the above-described reasons, and an object thereof is to provide a carbon dioxide adsorption / release device having high adsorption ability and low energy consumption during adsorption / desorption.
- a carbon dioxide adsorption / release device includes a pair of electrodes 1 and 2 provided facing each other, and an electrolyte 3 filled between the electrodes 1 and 2 of the pair of electrodes. And a porous body 4 provided on one electrode 1 of the pair of electrodes, wherein the electrolytic solution 3 absorbs carbon dioxide and is absorbed into the electrolytic solution.
- the porous body 4 allows carbonate ions or hydrogen carbonate ions to be formed on the surface of the porous body 4 when a forward voltage is applied to the pair of electrodes 1 and 2. Is electrostatically adsorbed, and the carbonate ions or bicarbonate ions are electrostatically released from the surface of the porous body 4 when a reverse voltage is applied to the pair of electrodes.
- forward voltage application refers to a pair of electrodes 1 and 2 provided facing each other, an electrolytic solution 3 filled between the electrodes 1 and 2 of the pair of electrodes, and one electrode of the pair of electrodes.
- a voltage is applied by connecting a positive electrode of a DC power source to the electrode 1 and a negative electrode of a DC power source to the electrode 2.
- reverse voltage application means applying a voltage by connecting the negative electrode of the DC power source to the electrode 1 and connecting the positive electrode of the DC power source to the electrode 2 in the above configuration.
- the porous body 4 includes a unit A that can be reversibly oxidized and reduced by applying a voltage to the pair of electrodes 1 and 2, and the oxidation of the unit A It is preferable that either the reductant or the reductant is an organic polymer in a cationic state.
- the porous body 4 is preferably a polymer gel that swells in the electrolytic solution.
- the unit A in the porous body 4 composed of the polymer gel, is preferably represented by the following structural formula (Formula 1 or Formula 2).
- the porous body 4 is represented by the following structural formula (Chemical Formula 3 or Chemical Formula 4).
- the porous body 4 is a conductive polymer porous body.
- the unit A is preferably polyaniline represented by the following structural formula (Formula 5).
- the porous body 4 is a conductive inorganic porous body.
- the unit A is preferably graphene.
- the conductive inorganic porous body is composed of at least one selected from the group consisting of graphite, carbon nanotube, and carbon fiber (carbon fiber).
- the density of the unit A contained in the porous body 4 is preferably 0.0002 mol / g to 0.02 mol / g.
- the solvent of the electrolytic solution is water.
- the electrolytic solution contains a supporting salt.
- the cation of the supporting salt preferably has a molecular weight of 1000 or more.
- the anion of the support salt preferably has a molecular weight of 1000 or more.
- a pair of electrodes provided opposite to each other, an electrolytic solution filled between the electrodes of the pair of electrodes, a porous body provided on one electrode of the pair of electrodes,
- the electrolyte solution can absorb carbon dioxide and form carbon dioxide ions or hydrogen carbonate ions by dissolving carbon dioxide in the electrolyte solution.
- the porous body can form the pair of electrodes.
- the carbonate ions or hydrogen carbonate ions are electrostatically adsorbed on the surface of the porous body, and when a reverse voltage is applied to the pair of electrodes, the carbonate ions or Since hydrogen ions are electrostatically released, the storage and release of carbon dioxide is electrochemically controlled by applying forward and reverse voltages to the electrodes 1 and 2.
- carbon dioxide is adsorbed / released by applying a voltage and does not require large energy such as applying heat, so that it exhibits low energy and excellent adsorption / desorption performance. Therefore, according to the present invention, it is possible to provide a carbon dioxide adsorption / release device that has high adsorption capacity and low energy consumption during adsorption / desorption.
- FIG. 1 is a schematic cross-sectional view showing an embodiment of the present invention.
- FIG. 1 shows an example of a carbon dioxide adsorption / release device.
- the carbon dioxide adsorption / release device includes a pair of electrodes (electrode 1 and electrode 2), an electrolytic solution 3, and a porous body 4.
- the electrode 1 and the electrode 2 are disposed to face each other and are spaced apart from each other, and the electrolytic solution 3 and the porous body 4 exist between the electrode 1 and the electrode 2.
- the electrolytic solution 3 and the porous body 4 are in contact with each other, the electrolytic solution 3 is in contact with the electrode 2, and the porous body 4 is in contact with the electrode 1 so as to exchange electrons and holes.
- the electrode 1 is connected to an electric device such as an external power source, a secondary battery, or a capacitor, and can perform a discharge charging process on the carbon dioxide adsorption / release device.
- the electrode 1 functions as a negative electrode (anode) of the carbon dioxide adsorption / release device.
- the electrode 1 and the electrode 2 may be formed of a single film made of a conductive material, or may be formed by laminating a conductive material on a base material.
- the conductive material include metals such as platinum, gold, silver, copper, aluminum, rhodium, and indium; carbon; indium-tin composite oxide, tin oxide doped with antimony, and tin oxide doped with fluorine.
- Conductive metal oxides such as: a composite of the metal or compound; a material in which the metal or compound is coated with silicon oxide, tin oxide, titanium oxide, zirconium oxide, aluminum oxide, or the like.
- the surface resistance of the electrode 1 is preferably as low as possible, but the surface resistance is preferably 200 ⁇ / ⁇ or less, more preferably 50 ⁇ / ⁇ or less.
- the surface resistance is 200 ⁇ / ⁇ or less, the voltage loss at the electrode 1 in the device of the present invention is reduced, and the device can be driven at a low voltage.
- the surface resistance is 50 ⁇ / ⁇ or less, the above effect is further improved, and device driving at a lower voltage becomes possible.
- the lower limit of the surface resistance is not particularly limited, but is usually 0.1 ⁇ / ⁇ . When the surface resistance is 0.1 ⁇ / ⁇ or more, the availability of electrodes and the low-voltage driving of the device are compatible.
- the electrode 1 When the electrode 1 is formed by depositing a transparent conductive oxide such as indium oxide, tin oxide, or zinc oxide on the substrate, a vacuum process such as sputtering or vapor deposition is employed on the substrate. The Further, a wet method such as a spin coating method, a spray method, or a screen printing method may be employed.
- a transparent conductive oxide such as indium oxide, tin oxide, or zinc oxide
- a vacuum process such as sputtering or vapor deposition is employed on the substrate.
- a wet method such as a spin coating method, a spray method, or a screen printing method may be employed.
- the electrode 2 functions as the positive electrode (cathode) of the carbon dioxide adsorption / release device.
- the electrode 2 may be formed of the same material as that of the electrode 1 and the same method as that of the electrode 1, for example.
- the electrode 2 is preferably made of a material having a catalytic action that gives electrons to the reductant in the electrolytic solution 3.
- materials include metals such as platinum, gold, silver, copper, aluminum, rhodium, and indium; carbon materials such as graphite, carbon nanotubes, and carbon carrying platinum; indium-tin composite oxide, doped with antimony Examples thereof include conductive metal oxides such as tin oxide and fluorine-doped tin oxide; and conductive polymers such as polyethylenedioxythiophene, polypyrrole, and polyaniline.
- platinum, graphite, polyethylenedioxythiophene and the like are particularly preferable.
- the electrolytic solution 3 includes a solvent and an electrolyte.
- the electrolyte is preferably present in a state dissolved in a solvent.
- the electrolyte is added to increase the ionic conductivity of the solvent, and the solvent dissolves carbon dioxide and becomes a medium for adsorption / desorption to the porous body 4.
- the solvent is filled or swollen in the porous body 4 to constitute a device.
- the solvent is preferably an electrochemically stable compound with a wide potential window.
- an aqueous solvent or an organic solvent can be used.
- water carbonate compounds such as dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, ethylene carbonate and propylene carbonate; ester compounds such as methyl acetate, methyl propionate and ⁇ -butyrolactone; diethyl ether, 1,2-dimethoxyethane, 1 Ether compounds such as 1,3-dioxosilane, tetrahydrofuran and 2-methyl-tetrahydrofuran; heterocyclic compounds such as 3-methyl-2-oxazodilinone and 2-methylpyrrolidone; nitrile compounds such as acetonitrile, methoxyacetonitrile and propionitrile; sulfolane, Examples include aprotic polar compounds such as dimethyl sulfoxide and dimethylformamide.
- carbonate compounds such as ethylene carbonate and propylene carbonate
- heterocyclic compounds such as ⁇ -butyrolactone, 3-methyl-2-oxazodilinone and 2-methylpyrrolidone
- acetonitrile methoxyacetonitrile
- propionitrile 3-methoxypropio Nitrile compounds
- nitrile and valeric nitrile are preferred.
- water is mixed from the viewpoint of the formation of hydrogen carbonate anions.
- the solvent may contain an ionic liquid (ionic liquid) or may consist only of an ionic liquid.
- the ionic liquid include all known ionic liquids. For example, imidazolium-based, pyridine-based, alicyclic amine-based, aliphatic amine-based, azonium amine-based ionic liquids, and European Patent No. No. 718288, pamphlet of International Publication No. 95/18456, Electrochemistry Vol. 65, No. 11, 923 (1997), J. Electrochem. Soc. 143, 10, pp. 3099 (1996), Inorg. Chem. Examples include ionic liquids having the structure described in 35, 1168 (1996). Thus, when the solvent has sufficient ionic conductivity, the electrolyte may not be present.
- the electrolyte may be gelled or immobilized, and may be formed from a gelled electrolyte (gelled electrolyte) or a polymer electrolyte.
- the gelling agent for gelling the electrolyte include a gelling agent utilizing a technique such as a polymer and a polymer crosslinking reaction, a polymerizable polyfunctional monomer, and an oil gelling agent.
- gelled electrolyte and polymer electrolyte commonly used substances can be applied.
- vinylidene fluoride polymers such as polyvinylidene fluoride, acrylic acid polymers such as polyacrylic acid, and acrylonitrile systems such as polyacrylonitrile.
- Polymers and polyether polymers such as polyethylene oxide, and compounds having an amide structure in the structure are preferred.
- the electrolytic solution 3 may contain a redox constituent that can be stably oxidized and reduced.
- the redox-based constituent material means a pair of substances that are present reversibly in the form of an oxidized form and a reduced form in a redox reaction.
- the redox constituents include solutions in which a redox couple is dissolved in a solvent, solid electrolytes such as molten salts, p-type semiconductors such as copper iodide, amine derivatives such as triphenylamine, polyacetylene, polyaniline, and polythiophene. And the like, and the like.
- the oxidation-reduction component include, for example, chlorine compound-chlorine, iodine compound-iodine, bromine compound-bromine, thallium ion (III) -thallium ion (I), mercury ion (II) -mercury ion (I ), Ruthenium ion (III) -ruthenium ion (II), copper ion (II) -copper ion (I), iron ion (III) -iron ion (II), nickel ion (II) -nickel ion (III), Examples thereof include, but are not limited to, vanadium ion (III) -vanadium ion (II), manganate ion-permanganate ion, and the like. In this case, these redox constituents function differently from the redox part in the porous body 4.
- This redox-based constituent material may be immobilized on the electrode 2.
- the immobilization method include a carbon electrode used in a secondary battery and the like, and a method in which the above-described constituent material is contained in a polymer gel.
- the solvent is preferably water that is widely present in the atmosphere.
- the electrolyte is dissolved in a solvent and added to improve the ionic conductivity of the electrolytic solution 3.
- electrolyte for example, tetrabutylammonium perchlorate, tetraethylammonium hexafluorophosphate, ammonium salts such as imidazolium salt and pyridinium salt, and alkali metal salts such as lithium perchlorate and potassium boron tetrafluoride are preferable.
- salts containing alkali metal or alkaline earth metal such as lithium, sodium, potassium, calcium, or an organic compound having an amino group as a cation and a halogen ion such as chlorine or bromine, or an anion as sulfonium or the like can be given.
- the electrolyte supporting salt stabilizes carbonate ions or bicarbonate ions and has a pH buffering ability.
- specific examples include sodium bicarbonate, sodium carbonate, acetic acid, sodium acetate and the like.
- these electrolytes may contain two or more simultaneously.
- the porous body 4 is electrochemically charged to a positive charge and has a function of adsorbing bicarbonate ions or carbonate ions.
- the porous body 4 is preferably a polymer gel body (gel layer 6) that swells in the electrolytic solution 3.
- the polymer gel body has a redox part and a gel part in the molecule.
- the redox moiety is a site where repeated redox is possible, that is, a site that can be reversibly oxidized and reduced in the redox reaction.
- This redox part should just be comprised by the site
- At least one of the oxidized form and reduced form of the redox moiety is preferably a cationic compound.
- the gel part is a part that swells into a gel containing the electrolyte solution.
- the redox moiety is chemically bonded to the gel site.
- the positional relationship between the redox moiety and the gel part in the molecule of the organic compound is not particularly limited.
- the redox part is the main chain as a side chain. It becomes a structure combined with.
- bonded alternately may be sufficient.
- the oxidation-reduction part and the gel part exist in the same molecule of the organic compound, the oxidation-reduction part is easily held in the gel layer 6 at a position where electrons are easily transported.
- the gel state of the gel layer 6 is preferably, for example, konjac or an external shape such as an ion exchange membrane, but is not particularly limited thereto.
- the gel layer 6 becomes a cation state in either the oxidation state or the reduction state, and when it becomes the cation state, it adsorbs carbon dioxide in the form of carbonate ions or hydrogen carbonate ions. Can do.
- the degree of swelling is a physical index that affects the size of the reaction interface formed in the gel layer 6.
- Gel dried body refers to a dried gel layer 6.
- the drying of the gel layer 6 refers to the removal of the solution contained in the gel layer 6, especially the removal of the solvent.
- Examples of the method for drying the gel layer 6 include heating, removal of the solution or solvent in a vacuum environment, removal of the solution or solvent contained in the gel layer 6 with another solvent, and the like.
- a solvent having a high affinity with the solution or solvent to be contained and easily removed in a heated or vacuum environment may be selected. It is preferable for efficient removal of the solution or solvent contained in the gel layer 6.
- the degree of swelling of the gel layer 6 is preferably 110 to 3000%, and more preferably 150 to 500%.
- the degree of swelling is less than 110%, the electrolyte component in the gel layer 6 is reduced, and thus there is a possibility that the oxidation-reduction part is not sufficiently stabilized.
- the degree of swelling exceeds 3000%, the redox part in the gel layer 6 is reduced and the carbon dioxide adsorption ability may be reduced. For this reason, in any case, the performance of the carbon dioxide adsorption / release device is lowered.
- An organic compound having a redox moiety and a gel part in one molecule is represented by the following general formula, for example.
- (X i ) nj : Y k (X i ) n represents a gel site, and X i represents a monomer of a compound that forms the gel site.
- the gel part is formed of, for example, a polymer skeleton.
- Y represents a redox moiety bonded to (X i ) n .
- J and k are each an arbitrary integer representing the number of (X i ) n and Y contained in one molecule, and both are preferably in the range of 1 to 100,000.
- the redox moiety Y may be bonded to any part of the polymer backbone constituting the gel part (X i ) n .
- examples of the redox part of the polymer gel structure include structures represented by the following chemical formulas (6) and (7).
- Counter anion A in formula (6) as, for example a bromine ion, a chlorine ion, perchlorate ion, hexafluorophosphate ion, and an anion selected from tetrafluoroborate and the like.
- N + nitro cation
- N ⁇ nitro radical
- carbonate ion or hydrogen carbonate ion is contained in the polymer gel structure as a counter anion. Is done.
- Electropolymerization can be mentioned as a method for synthesizing the polymer gel represented by the chemical formula (6).
- the organic compound thus obtained has a pyridium structural unit represented by chemical formula (6) as a redox moiety.
- This pyridium structural unit is M by electropolymerization from a portion having a structure represented by chemical formula (8) of the precursor (where M is a halogen group such as fluorine, chlorine, bromine or iodine, or a cyano group). And a position where the substituent represented by M at this site is eliminated is bonded to each other.
- M is a halogen group such as fluorine, chlorine, bromine or iodine, or a cyano group.
- the organic compound when the pyridinium diradical is oxidized by one electron, a pyridinium cation radical is generated, and when further oxidized by one electron, the original pyridium structural unit is restored.
- the organic compound repeatedly exhibits stable redox ability.
- an organic compound undergoes a radical state during oxidation and reduction, a very fast self-electron exchange reaction occurs, and electrons are easily transferred between the organic compounds.
- the radical state at the time of oxidation reduction of the organic compound is observed by, for example, ESR (electron spin resonance).
- the precursor has a plurality of sites having the structure represented by the chemical formula (8) in one molecule, a high molecular weight organic compound can be generated by electrolytic polymerization of the precursor.
- the precursor has 2 or more, more preferably 3 or more sites per molecule having the structure represented by the chemical formula (8).
- the organic compound produced by electrolytic polymerization of the precursor is deposited on the electrode 1, thereby forming the porous body 4.
- the electrode 1 is first immersed in a solution containing the precursor. In this state, the precursor is polymerized on the electrode 1 by electrolytic polymerization to produce an organic compound, whereby the porous body 4 is formed on the electrode 1.
- the electrode potential of the electrode 1 during this electropolymerization is made lower than the reduction potential of the precursor. As a result, electrons can move within the organic compound having the properties of an n-type semiconductor on the electrode 1, and electrolytic polymerization proceeds.
- the porous body 4 formed by the electropolymerization of the precursor exhibits high durability. Moreover, this porous body 4 is formed in high density by being formed through electrolytic polymerization. For this reason, it is expected that the carbon dioxide adsorption performance in the porous body 4 is improved.
- the polymer gel body is encapsulated in a highly conductive substance called a collector electrode having a high porosity.
- the collector electrode When the collector electrode is present, the low electron transport property of the polymer gel body is ensured by the highly conductive material, so that the film can be made thicker and the amount of carbon dioxide adsorption per device can be improved. become.
- Materials constituting the collector electrode include metals such as platinum, gold, silver, copper, aluminum, rhodium and indium; carbon materials such as graphite, carbon nanotubes and carbon carrying platinum; indium-tin composite oxide, antimony Examples thereof include conductive metal oxides such as doped tin oxide and fluorine-doped tin oxide; and conductive polymers such as polyethylenedioxythiophene, polypyrrole, and polyaniline. These particles may be spherical. More preferably, it has a high aspect ratio. If it has a high aspect ratio, it can have a structure with a high current collection effect with a high porosity.
- the porous body 4 is preferably a conductive polymer porous body.
- a conductive polymer is formed in a porous state on the electrode 1, and carbonate ions or hydrogen carbonate ions are adsorbed on cation sites generated by electrochemical oxidation or reduction.
- the Examples of the porous polymer include conductive polymers such as polyaniline and polypyrrole. Polyaniline is extremely excellent in stability against air oxidation as compared with a linear conjugated polyacetylene, and is practically used as a positive electrode material using lithium aluminum as a counter electrode of a secondary battery, for example.
- Other applications include electrochromic materials, immobilized enzyme carriers, surface coating materials that suppress photodissolution of semiconductors, transistors, semiconductor electrode coating materials using electron transfer catalysis, and carbon dioxide photoelectrochemical reduction catalysts. Further, various applications such as use as an electrode material exhibiting a photoelectric response have been studied.
- Examples of the synthesis method include the method shown in Japanese Patent Application No. 4-11458.
- the production method of polyaniline is preferably electrolytic polymerization. If the film is formed by electropolymerization, the film formation proceeds in a state where a conductive path is secured, and a polyaniline film in which all aniline sites are active can be obtained.
- the electrolytic polymerization method may be a constant potential method or a potential scrambling method.
- the counter anion that ensures the cation site in the porous polymer body is preferably a bicarbonate ion or a carbonate ion.
- the ratio is preferably 10 to 99, more preferably 100 to 10,000, assuming that the total number of moles of other counter anions is 1.
- the porous body 4 may be an inorganic porous body.
- an inorganic porous body when a voltage is applied, the porous surface is filled with a positive or negative charge, and carbon dioxide is adsorbed on the inorganic porous body as a counter anion in the form of hydrogen carbonate ions or carbonate ions. Detach from the body.
- constituent material examples include a carbon-based electrode using activated carbon or carbon fiber, a high porosity electrode using a needle-like conductive material, or a carbon nanotube. These may be used in combination.
- a predetermined catalyst may be supported on these conductive materials.
- a platinum catalyst for example, a platinum catalyst, a silver catalyst, a platinum / ruthenium catalyst, a cobalt catalyst, or the like can be used.
- the thickness of the porous body 4 is preferably in the range of 0.001 to 10 cm. If it is less than this, the amount of carbon dioxide absorption will be insufficient, and if it is more than this, the absorption / release rate of carbon dioxide may be reduced.
- the porous body 4 has excellent carbon dioxide adsorption performance, and the electrolytic solution 3 is rapidly filled with carbonate ions or hydrogen carbonate ions. .
- the porous body 4 is filled with carbon dioxide in the form of hydrogen carbonate ions or carbonate ions and adsorbed. When applied, carbon dioxide is released from the porous body 4 into the electrolytic solution 3, so that carbon dioxide can be released.
- Example 1 A conductive glass substrate (manufactured by Asahi Glass Co., Ltd., 10 ⁇ / ⁇ ) having a thickness of 1 mm, a length of 21 mm, and a width of 24 mm having a fluorine-doped tin oxide film was prepared. This fluorine-doped tin oxide film was used as the electrode 1. 1 ⁇ m of polyaniline was deposited on the substrate 1 as the porous body 4 using an electrochemical oxidation method (electrolytic polymerization method).
- a conductive glass substrate made by Asahi Glass, 10 ⁇ / ⁇ having a thickness of 1 mm, a length of 21 mm, and a width of 24 mm having a fluorine-doped tin oxide film is prepared, and platinum is deposited on the fluorine-doped tin oxide film by sputtering.
- Electrode 2 The porous body 4 and the electrode 2 were disposed so as to face each other, and a hot melt adhesive (Bunel, manufactured by DuPont) having a width of 1 mm and a thickness of 50 ⁇ m was interposed in an outer edge portion between the porous body 4 and the electrode 2.
- Example 2 In Example 2, only the porous body 4 is different from the structure of Example 1, and the other structure is the same as that of Example 1.
- the porous body 4 was produced by the following method. Electrolytic manganese dioxide (MnO 2 , positive electrode active material) heat-treated at 400 ° C., acetylene black (conductive agent), polyethylene oxide having an average molecular weight of 100,000 as a binder (viscosity average molecular weight 100,000, manufactured by Sigma-Aidrich) and LiN (CF 3 SO 2 ) 2 was dissolved or dispersed in acetonitrile and kneaded to prepare a paste-like positive electrode mixture.
- Electrolytic manganese dioxide MnO 2 , positive electrode active material
- acetylene black conductive agent
- polyethylene oxide having an average molecular weight of 100,000 as a binder viscosity average molecular weight 100,000, manufactured by Sigma-Aidrich
- LiN (CF 3 SO 2 ) 2 was dissolved or dispersed in aceton
- the mass of the polymer electrolyte was a mass in terms of solid content.
- the obtained paste-like positive electrode mixture was applied to an electrode, dried at 1200 ° C. for 24 hours, and then rolled with a roll press to prepare a porous body 4.
- the obtained device was evaluated for carbon dioxide adsorption / desorption performance in the same manner as in Example 1.
- Example 1 The porous body 4 in Example 1 was formed using zeolite. Ferrilite (peak of pore size distribution is about 4.5 angstrom, SiO 2 / Al 2 O 3 molar ratio is about 90) was used as zeolite. This was supported on the electrode at 50 g / m 2 to form a porous body 4.
- the porous body 4, the size of the electrodes 1 and 2, the distance between the electrode 2 and the porous body 4 and the like are the same as those in the first embodiment.
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Abstract
Description
したがって、本発明によれば、高吸着能であり、かつ吸着脱離時のエネルギー消費が少ない二酸化炭素吸着・放出デバイスを提供することができる。
多孔質体4は、電解液3に膨潤する高分子ゲル体(ゲル層6)であることが好ましい。
膨潤度=(ゲルの重量)/(ゲル乾燥体の重量)×100
(Xi)nj:Yk
(Xi)nはゲル部位を示し、Xiはゲル部位を形成する化合物のモノマーを示す。ゲル部位は例えばポリマー骨格で形成される。モノマーの重合度nは、n=1~10万の範囲が好ましい。Yは(Xi)nに結合している酸化還元部を示す。またj,kはそれぞれ1分子中に含まれる(Xi)n、Yの数を表す任意の整数であり、いずれも1~10万の範囲が好ましい。酸化還元部Yはゲル部位(Xi)nを構成するポリマー骨格のいかなる部位に結合していてもよい。
多孔質体4は、導電性高分子多孔質体であることが好ましい。
多孔質体4は、無機多孔質体であってもよい。
[実施例1]
フッ素ドープ酸化スズ膜を有する厚み1mm、縦21mm、横24mmの導電性ガラス基板(旭硝子製、10Ω/□)を用意した。このフッ素ドープ酸化スズ膜を電極1とした。電気化学酸化法(電解重合法)を用いて多孔質体4としてポリアニリンを基板1上にlμm析出させた。一方、フッ素ドープ酸化スズ膜を有する厚み1mm、縦21mm、横24mmの導電性ガラス基板(旭硝子製、10Ω/□)を用意し、フッ素ドープ酸化スズ膜上に白金をスパッタ法で堆積させ、これを電極2とした。多孔質体4と電極2とを対向するように配置し、両者の間の外縁部分に幅1mm、厚み50μmの熱溶融性接着剤(デュポン社製、バイネル)を介在させた。この熱溶融性接着剤を加熱しながら加圧することで、多孔質体4と電極2とを熱溶融性接着剤を介して接合した。さらに、水にOH-TEMPO(4-ヒドロキシ-2, 2, 6, 6-テトラメチルピペリジン1-オキシル)を0.5Mの濃度で、塩化カリウムを0.5mol/lの濃度で溶解させて、電解質溶液を調製した。この電解質溶液を二酸化炭素注入・放出用の孔から、電極2と多孔質体4との間に注入した。これにより素子を作製した。なお、この場合のポリアニリンの合成法(電気化学酸化法)はE. M. Genies, Mol. Cryst. Liq. Cryst.,121,181-186 (1985)に記載された方法に従って行なった。得られた素子について、二酸化炭素吸着脱離性能を評価した。
実施例2は、多孔質体4のみ実施例1の構成と異なり、その他の構成は実施例1と同様である。
多孔質体4を、以下の方法で作製した。
400℃で熱処理した電解二酸化マンガン(MnO2、正極活物質)、アセチレンブラック(導電剤)、結着剤である平均分子量10万のポリエチレンオキシド(粘度平均分子量10万、Sigma-AIdrich社製)およびLiN(CF3SO2)2をアセトニトリルに溶解または分散させて混練し、ペースト状の正極合剤を調製した。ここで、MnO2:アセチレンブラック:ポリマー電解質=70質量%:20質量%:10質量%になるように配合した。なお、ポリマー電解質の質量は、固形分換算の質量とした。得られたペースト状の正極合剤を電極に塗布し、1200℃で24時間乾燥させた後、ロールプレスで圧延することにより、多孔質体4を作製した。得られた素子について実施例1と同様に、二酸化炭素吸着脱離性能を評価した。
実施例1における多孔質体4をゼオライトを用いて形成した。
ゼオライトとしてはフェリエライト(細孔径分布のピークが約4.5オングストローム、SiO2/Al2O3モル比が約90)を用いた。これを、電極上に50g/m2で担持させて、多孔質体4を形成した。多孔質体4、電極1、2の大きさ、電極2と多孔質体4との間隔等は実施例1と同一である。
放出量=(焼成前の重量)-(焼成後の重量)
2 電極
3 電解液
4 多孔質体
Claims (14)
- 対向して設けられた一対の電極と、上記一対の電極の各電極間に充填された電解液と、上記一対の電極の一方の電極上に設けられた多孔質体と、を有してなる二酸化炭素吸着・放出デバイスであって、
上記電解液は、二酸化炭素を吸収し当該電解液に二酸化炭素が溶解されることにより炭酸イオン又は炭酸水素イオンを形成可能であり、
上記多孔質体により、上記一対の電極への順方向電圧印加時に多孔質体の表面に上記炭酸イオンまたは炭酸水素イオンが静電的に吸着され、上記一対の電極への逆方向電圧印加時に多孔質体の表面から上記炭酸イオンまたは炭酸水素イオンが静電的に放出される二酸化炭素吸着・放出デバイス。 - 上記多孔質体は、一対の電極への電圧印加によって可逆的に酸化還元可能である単位Aを含み、かつ、単位Aの酸化体もしくは還元体のどちらか一方がカチオン状態となる有機高分子である請求項1記載の二酸化炭素吸着・放出デバイス。
- 上記多孔質体が上記電解液に膨潤する高分子ゲルである請求項2に記載の二酸化炭素吸着・放出デバイス。
- 上記多孔質体が、導電性高分子多孔質体である請求項2記載の二酸化炭素吸着・放出デバイス。
- 上記多孔質体が、導電性無機多孔質体である請求項1記載の二酸化炭素吸着・放出デバイス。
- 上記導電性無機多孔質体が、グラファイト、カーボンナノチューブ、炭素繊維(カーボンファイバー)からなる群から選択された少なくとも1つから構成される請求項8に記載の二酸化炭素吸着・放出デバイス。
- 上記多孔質体に含まれる単位Aの密度が、0.0002mol/g~0.02mol/gである請求項2に記載の二酸化炭素吸着・放出デバイス。
- 上記電解液の溶媒が水である請求項1に記載の二酸化炭素吸着・放出デバイス。
- 上記電解液が、支持塩を含む請求項1に記載の二酸化炭素吸着・放出デバイス。
- 上記支持塩のカチオンが、分子量1000以上である請求項12に記載の二酸化炭素吸着・放出デバイス。
- 上記支持塩のアニオンが、分子量1000以上である請求項12に記載の二酸化炭素吸着・放出デバイス。
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JP2018001131A (ja) * | 2016-07-07 | 2018-01-11 | 株式会社クラレ | 二酸化炭素分離装置 |
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