WO2004040679A1 - 多孔電極およびそれを用いた電気化学素子 - Google Patents
多孔電極およびそれを用いた電気化学素子 Download PDFInfo
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- WO2004040679A1 WO2004040679A1 PCT/JP2003/013979 JP0313979W WO2004040679A1 WO 2004040679 A1 WO2004040679 A1 WO 2004040679A1 JP 0313979 W JP0313979 W JP 0313979W WO 2004040679 A1 WO2004040679 A1 WO 2004040679A1
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/8605—Porous electrodes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
- H01M4/8652—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites as mixture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
- H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Definitions
- the present invention relates to a porous material used for electrochemical devices such as a battery and a capacitor.
- the present invention relates to a fuel cell, an air battery, a ⁇ ⁇ device, a gas sensor, an intense gas ⁇ device, and the like, which uses the porous material as a gas expansion mm electrode and uses it in combination with a reactant gas and a desorber.
- Fig. 3 shows a typical configuration of a fuel cell.
- a fuel electrode that generates electrons and protons by reacting a fuel such as hydrogen with the fuel, a TO material that transmits the generated protons, and oxygen that reacts the protons and oxygen with the electrons that arrive through an external circuit It consists of «.
- the ⁇ in the electrode section of the fuel cell plays the following role;
- liquid or gaseous fluid fuel reacts with the catalyst on the electrode, for example, H 2 ⁇ 2 H + + 2 e _, and the separated electrons are transmitted outside from the electrode, Protons are transferred to the proton conductive material.
- the electrolyte a substance that plays a role of only protons 31 and has a small decrease in efficiency due to diffusion of fuel or the like is used.
- the composition of ®g used in fuel cells is a gas or liquid fuel fluid, as shown in ⁇ , a reaction site that causes a reaction between electrons, protons and fuel, and g also carries an electron or proton charge. Requires electrode material and electrolyte. In this way, it is difficult to coexist with the space where the fuel flows and the charge transfer.
- the electrode is composed of a fluorine-based polymer having a sulfonic acid group in the side chain, which is a proton-conductive solid electrolyte as the orchid, the conductivity of carbon particles formed by carbon particles, etc.
- a porous material is coated with a material and aged, or embedded in a porous material (Japanese Unexamined Patent Application Publication No.
- the electrodes of the fuel cell are composed of: a) fuel gas, b) bandages for reaction, c) charge, and d) orchid.
- a porous body is used as the electrode.
- the catalyst is dispersed in the form of fine particles so as to have a specific surface area of 1 mm without being combined. It is preferable that protons react at the trace of time with the fuel gas force, and the generated electrons and protons are efficiently separated from the reaction site «to be ⁇ .
- water is generated from protons, it is preferable that electrons and protons reach the reaction site in an efficient manner and warp with oxygen.
- carbon particles 101 such as carbon black form the poles:!
- the polymer of the electrolyte 104 is applied so as to cover the surface of the particles, and the bandages are buried in the liver It has been done. Therefore, in practice, as shown in Fig. 4, the carbon ionization surface is partially covered with the solid polymer electrolyte 104 and partially covered, and in some cases, completely covered. Unexplained parts are formed.
- the fuel fluid is easily accessible.
- the electron and protons generated by the anti-J3 ⁇ 4T are not separated without charge separation because there is no nearby polymer electrolyte 104 that transmits the protons to the electrolyte membrane 105. Recombination enables efficient reaction.
- expensive metal such as platinum is inevitably used, as in the case of being covered with high liver quality, resulting in high cost.
- the electrode is made of carbon particles such as carbon black
- the black ink is formed in the step of applying S # to the carbon particles and in the step of combining with the polymer electrolyte. is there. If the material is fiber, the specific surface area of the rubber decreases and the rejection rate decreases. For this reason, it is necessary to use a lot of luras.
- the present invention has been made in view of the problems of the surgical technique, and has as its object to provide a reaction that proceeds efficiently. Further, an object of the present invention is to provide a use of an electrochemical device such as a fuel cell capable of efficiently causing a reaction.
- the present invention relates to the following porosity and electrification.
- An electrode made of a porous material having electron conductivity (1) A three-porous material is composed of three skeletons. (2) A material having a proton affinity group is not suitable.
- iifS is contained on a substance that contains ⁇ K in the negative electrode and separates it into protons and electrons, and has a ⁇ 0 ⁇ proton affinity group.
- ⁇ tait has been perforated ⁇ .
- Substantially all of the substance is fiJ-substituted on the substance that has a badly proton-affinity group.
- the substance having an unfavorable proton affinity group is linear ⁇ f
- the linear liver has a group having an affinity with an unfavorable three-porous material at one end. Having a hydrophilic group,
- Plural sickles H dislike 33 ⁇ 4 of fountain liver dislodged? Absorbs on the surface of L-form, and the proton-affinity groups of the plurality of linear molecules form a proton-affinity coated surface, iffS ⁇ l Porosity described in l
- porous electrode according to claim 1 wherein the substance having a proton affinity group is a spherical molecule having a proton affinity group.
- porous electrode according to item 4 wherein the spheroid liver is at least one of dendrimer and fullerene.
- Electrode made of? -L-electrode with electron conductivity the anamorphous porous body is composed of a three-dimensional skeleton, and the substance with a proton affinity group ⁇ T is not ⁇ B ⁇ ⁇ 3 ⁇ 4
- a method of using a porous cage in which hydrogen is further divided into protons and electrons, and wherein the substance is supported on the substance having a proton affinity group Or a method of using a porous cage in which hydrogen is further divided into protons and electrons, and wherein the substance is supported on the substance having a proton affinity group.
- the porous me method wherein the solution containing the sickle 3 3 and containing a substance having a proton affinity group includes a step of dispersing the multi-L form at the time of dispersing.
- An electrochemical element consisting of a fuel ⁇ ⁇ @, which produces protons from the fuel, and a fuel ⁇ ⁇ @, which reacts protons with oxygen, with a proton-conductive solid electrolyte interposed between them.
- One electrode is porous ⁇ described in 5 ⁇ 1
- FIG. 1 is a diagram showing an example of the porous electrode of the present invention.
- FIG. 2 is a diagram showing another example of the porosity according to the present invention.
- FIG. 3 is a diagram showing a typical US of a fuel cell.
- FIG. 4 is a view showing a multi-layer electrode of the present invention.
- FIG. 5 is a diagram showing another example of the porous electrode of the present invention.
- the porous electrode of the present invention is an electrode made of a porous body having electron conductivity
- the porous body is composed of three ⁇ skeletons, (2) a substance having a proton affinity group is located on a part or ⁇ of the surface of the three dimensional skeleton, and (3) further separates hydrogen into protons and electrons It is assumed that the substance is included on a substance containing a catalyst and having a proton affinity group.
- the material constituting the porous body is not weak as long as it has electronic conductivity.
- any material that can convert electrons or Si should be used.
- one or more conductive materials such as metal materials, oxides, semiconductors, conductive materials, and carbon materials may be used. Wear. More specifically, examples of the material include gold, platinum, nickel, iron, copper, aluminum, and stainless steel.
- the oxide conductor include titanium oxide, tin oxide, indium oxide, indium tin oxide, tungsten oxide, tantalum oxide, and sodium oxide.
- the half is exemplified by silicon, sulfurized dome, sulfur, and selenium lead.
- the highly conductive liver is exemplified by polypyrrole, polyaniline, polythiophene, and the like.
- the carbon material examples include carbon black (acetylene black, Ketjen black, etc.), activated carbon, artificial graphite, natural graphite, carbon, pyrolytic carbon, glassy carbon, invisible carbon, special carbon, coke, and the like. . It does not have to be crystal of force-pon material and may have either diamond structure or black 3 ⁇ 4 ⁇ . Also, as a carbon material, it is possible to perform ⁇ ffl on nanocarbon materials such as carbon nanotubes, carbon nanohorns, carbon nanoribbons, carbon nanocoils, and carbon nanocapsules.
- a composite material in which a conductive material is combined with a non-conductive material can be filtered.
- a porous body such as silica or alumina having a metal film formed by plating or the like, or a porous body such as silica or alumina coated with an oxide conductor or a highly conductive metal can be used.
- a carbon material By using a carbon material, carbon can be supported with a high specific surface area, and durability against acid or alkali can be obtained. Furthermore, processing and taste are not required, and cost can be reduced.
- the structure of the porous body is composed of three skeletons.
- the ⁇ 5 skeleton is not particularly limited as long as it has a predetermined porosity.
- the porosity of the porous body can be determined according to the purpose and usage of the porous basket, but it is typically in the range of 10% to 98%, and is supplied in a liquid or gaseous state Considering the efficiency of the electrode reaction of the reactant and the bow of the electrode, it is preferable to set the force within the range of 20% and 80%.
- the specific surface area (B ET method) also P arm specifically at Nag usually can force it determined 3 ⁇ 4 ⁇ in the range of 2 0 0 0m 2 Zg from 5 ⁇ 2 ⁇ , considering that the efficiency and the electrode of the response 1 Om 2 / It is desirable to set the range of g to 500 m 2 Zg.
- the porous material method also requires ⁇ ffl be able to.
- these are formed into dogs of a predetermined shape I by H-shaped molding methods such as ffiii ⁇ , injection, m, printing, and coating. do it.
- H-shaped molding methods such as ffiii ⁇ , injection, m, printing, and coating. do it.
- three types of particles such as bubbles formed by a collection of powder particles, bubbles obtained by foaming, and entanglements obtained by entanglement of fineness, are obtained. Any of these can be used as the porous body of the present invention.
- the porous body can be formed by a method of making the material porous at the same time as the synthesis of the material.
- the sol-gel method can be suitably used.
- the reference gel obtained through the wet gel synthesized by the sol-gel method is preferable because it has a network skeleton structure and specific surface area.
- a fiber gel obtained by stiffening a wet gel, such as titanium oxide or sodium oxide, which is difficult to transmit an oxide, or a porous carbon material obtained by firing a carbon precursor sardine gel can be used.
- a substance having a proton-affinity group (hereinafter also referred to as “spiza”) is attached to “” ⁇ or ⁇ on the surface of the 3 ⁇ S skeleton.
- the spacer may be mainly one that can generate generated protons from electrons, that is, one that can isolate protons from a conductive material that performs electronic Si.
- the spacer may be composed of ⁇ having a proton affinity group.
- the above shape is not p-arm-like, but a linear liver, a spherical shape, etc. can be used for a basket.
- a single liver is preferable, and a) chemisorption with affinity for porous material by chemical reaction ⁇ ?, b) monolayer or bilayer with affinity by physical adsorption, etc. And the amphiphile used.
- the spherical ⁇ for example dendrimers one (e.g. polyamidoamine dendrimer, Polypropylene I Min dendrimer), fullerene (e.g. c 60, c 70, c 76 , c 78, c 82, c 84) is mosquitoes ⁇ up like.
- a dendrimer in the present invention.
- Examples of the proton affinity group include a sulfonic acid group, a hydroxyl group, a carboxylic acid group, an amine group, an amino group, an ammonium group, an amide group, a thio group, a silanol group, a phosphoric acid group, and an oxyethylene group.
- These proton affinity groups are One or more kinds may be contained in the molecule.
- the experiments containing two or more proton affinity groups may be the same or different.
- These proton affinity groups can be selected according to the material of the porous body and the like.
- a linear element is used as the element that constitutes the above-mentioned substance.
- ⁇ One end of an H-shaped molecule (chain: «element) consisting of an aralkylene group, a phenylene group, etc. It is possible to use a solid compound that has a proton-producing group and has at the other end an affinity with the surface of the porous material of one degree, which has a high affinity for the surface of the porous material.
- the group can be selected according to the properties of the surface of the porous body 51. For example, 1) the surface of the porous material is ⁇ T: ⁇ is an alkyl group, a fluoroalkyl group, a phenyl group, etc.
- the proton affinity group is introduced into the spherical surface (especially, the outer peripheral portion), which is difficult.
- the spherical molecule at least one of dendrimer and fullerene can be suitably used.
- dendrimers are most preferable because they can be designed relatively freely according to the size of the catalyst (particles) and can be fixed inside the spherical liver. These spherical livers are easily adsorbed by physical adsorption to create self-alignment on the surface.
- a dendrimer it is possible to suitably use a liver in which a functional group of the yarn 15 or a part which is polymerized in a fine filament form is a proton affinity group. Further, it is possible to use a metal in which a proton affinity group is further added to a functional group.
- a dendrimer is a sphere-shaped, high liver that has been successfully dendritic-grown from high ⁇ ?, and is composed of a core, a branch skeleton, and elements on the outermost surface. , The branch skeleton can be polymerized sequentially. Thus, the polymerization Depending on the number of times, the dendrimer can be grown into ITO. By selecting each element such as growth, the ⁇ i and size of the dendrimer can be precisely controlled, and when «is formed inside, the size of the vehicle can be regulated and controlled.
- dendrimer there are various types of dendrimers such as polyamidoamine, polypropyleneimine, polyether, etc. Its size can be controlled by the size of the growth, but can range from approximately I nm to 100 nm. It is preferable not to be too large for the age at which the high-growth nanometeresis is formed, and it can be used more preferably in the range of about I nm to 50 nm.
- fullerene it is possible to use a fullerene having a surface coated with a strong proton affinity group such as a sulfonic acid group or a carboxylic acid group, in addition to a hydroxylated fullerene. Furthermore, it is a T ability to use a material that contains a metal that acts as a metal in the fullerene.
- ⁇ fl can also be obtained by the synthesis method.
- a liver having a proton affinity group added to an existing liver can be subjected to ⁇ ffl.
- the spacer may cover the surface of or the surface of the skeleton.
- bacteria can be prepared according to the purpose and usage of the L electrode.
- the spacer covers substantially the entire surface of the skeleton. Thereby, better healing performance can be achieved.
- the method of applying the spacer to the porous body is not particularly ⁇ -armed.
- it can be suitably applied by immersing a solution or dispersion obtained by dissolving or dispersing a spacer in a solvent in a porous material.
- the solvent may be water or a harmful medium.
- an anaerobic medium for example, alcohols such as methanol and ethanol, and charcoal such as hexane can convert elements.
- the amount of the spacer used in this case may be appropriately determined according to the type of the porous body to be used and the like.
- the porosity of the present invention includes a thigh that functions to split hydrogen into protons and electrons.
- ⁇ is preferably placed on the spacer contained in the porous material S, and it is more desirable that substantially all of the wakefulness is absorbed on the spacer. This results in the ability to achieve higher ⁇ s characteristics with less food. It should be noted that, as long as the effects of the present invention are not impaired, a portion of the spacer may be employed.
- hydrogen can be separated into protons and electrons by the reaction-( ⁇ tongue substance) can be MI.
- a porous electrode is stored in the fuel cell etc.
- metals such as platinum, palladium, ruthenium and gold, alloys such as platinum ruthenium and white, nickel-based and manganese-based oxides, etc. can be used. it can.
- the following method may be used. For example, a) a method of fijf using a colloid, b) a method of applying a metal salt or the like before or after a precursor is removed, and C) a baking of a precursor such as a metal salt.
- the catalyst may be applied at any stage. For example, a) a method of adding a solid to the surface of a porous body when forming a porous electrode, b) a method of introducing a spacer at the same time as applying a spacer to the body surface, and c) a method of preliminarily increasing the spacer.
- a method of applying the spacer to the surface of the porous body and a method of applying the spacer after the spacer is applied to the surface of the porous body. These methods may be selected according to the materials to be used, the view, and the like.
- the above method c) is preferable.
- virtually all of the 3 ⁇ 4 to be converted can be made to the spacer, and the ⁇ reaction can be performed more efficiently.
- the electrode of the present invention can be suitably made difficult.
- This method can be performed in accordance with a method of providing a hated spacer. In the above case, a spacer that does not carry a metal may be used together with a supported spacer.
- the porous electrode of the present invention is mainly composed of a porous body having electric conductivity, It can be composed of spacers and «.
- the spacer is formed on the surface of a three-dimensional skeleton constituting a poly-L body.
- a space is provided near the catalyst so that the reactant can easily reach the reaction site.
- separation or separation of the charged substance of» 0 ⁇ It makes it easier to supply your body to «.
- the contact between the surface of the porous body and the corresponding proto 11 compatible group of the coated spacer is set so as to be close to each of the transmissions. When you do, you get a better effect. Further, it is preferable that substantially all the particles are supported on the spacer in order to secure the standing position.
- the spacer sgii When the spacer forms a monolayer, the spacer sgii is in molecular order, and the electrons are tunneled or hopped to the source or from the electrode material. It is transmitted to Oki. And protons are transmitted to the surface by proton affinity conduction and hopping conduction to the electrolyte, and vice versa. If this health is too poor, it will be difficult to transmit between the thigh and the den and the efficiency will be reduced.
- the thickness of the single liver layer is preferably in the range of 0.1 nm to 100 nm in order for electrons and protons to be transmitted efficiently as described above. In particular, considering the electron tunneling conductivity, the range of 0.5 nm to 2 O nm is more preferable. This range may be determined according to the size of the liver or the size of the part, etc.
- the hydrogen that becomes the fuel has high diffusivity, reaches hydrogen, and the reaction proceeds.
- the electrochemical of the present invention is an electrochemical cell in which a fuel electrode that generates protons from a fuel and an oxygen electrode that reacts protons with oxygen are opposed to each other with a proton-conductive solid electrolyte therebetween. At least one of the electrodes is the porous electrode of the present invention. Therefore, in addition to using the present invention as a view, it is possible to refer to the components (rnm, container, separator, etc.) of the electrochemical element (fuel cell).
- an electrolyte having a p-ton conductivity may be used.
- a fluorine-based high-molecular weight film having a sulfonic acid group in a side chain; a hydrated oxide such as tungsten oxide or molybdenum oxide; a solid or body such as polyphosphoric acid or polytungstic acid can be used.
- the substrate is in the form of a film or a sheet.
- the porous cage with the electrolyte it can be applied to the porous electrode by a method of printing or coating.
- Electrochemical eaves are used as fuel tanks.
- the fuels used are, for example, alcohols such as methanol and ethanol; ethers such as dimethyl ether and getyl ether; methane, ethane, and propane.
- Gasoline and the like can be used in addition to carbon and teK, such as butane.
- hydrogen can be preferably ⁇ ffl.
- methanol is also preferable as an electrochemical element composed of a fuel pond, since the rate of generating hydrogen is high for the reaction performed directly by the porous electrode.
- porous and electrochemical devices according to the present invention can take various variations, and a typical embodiment thereof will be described.
- FIG. 1 shows an example of an embodiment of the porous electrode of the present invention.
- the porous electrode 10 of the present invention is made of an electron conductive porous body 1 made of conductive particles.
- the surface of the porous body forms a proton-affinity-coated surface 3 with proton-affinity groups 23 via the spacers 2.
- the spacer 2 is adsorbed on the porous body 1 at an affinity portion (affinity portion) 21 of the porous body 1, and the chain-shaped single liver portion 22 contains fine particles 4 therein. It is included.
- this porous electrode as an electrochemical eave, use the fuel pond example in Fig. 3.
- the pores 10 are arranged to face the proton conductive solid 5 so as to be used by supplying fuel and performing communication between the fuel cell and an external circuit.
- the marauder 4 used for the porosity 10 it is possible to select a suitable accessory for the reaction generated in each 1
- Hydrogen diffuses into the voids of the porous body 1 having the porous electrode 10 and reaches the surface thereof. On surfaces covered with spacer 2, ⁇ elements can easily rise 4. The hydrogen that reaches the thigh 4 reacts to give electrons (e _) and ptons (H +).
- the spacer of the single liver layer spacer 2 2 is a nucleus capable of transferring electrons secretly to the porous body 1 by tunnel conduction leakage, so that efficient separation of electrons and protons can be achieved. it can.
- protons easily move from the thigh 4 to the proton affinity group 23 by the hopping mechanism. On this surface 3, protons move by hopping conduction leakage to orchid 5. Then, the material 5 is applied to the electrode facing t3 ⁇ 4r to react with oxygen.
- the structure is formed by the organic layer of “fibre-like”; however, the same effect can be obtained by the spherical spacer 30 as in the second embodiment.
- the spherical spacer 30 is composed of a spacer portion 33 and a proton affinity base portion 32.
- the fine particles of Ra 34 are located inside the organic layer or between the spherical livers.
- spherical liver in addition to a spherical dendrimer obtained by dendritic growth of a high liver, spherical carbon such as Ripbon 60 and Rippon 70 are preferable.
- These spherical ⁇ are suitable for the purpose of the present invention because a proton affinity group or a hydrophilic group compatible with a porous body can be easily introduced into the surface thereof.
- the fine particles 34 can be formed inside the spherical liver, or can be formed in the space where the spherical particles come into contact with each other.
- FIG. 2 (1) shows an example of a dendrimer having a spherical shape.
- the diameter of the catalyst 34 fixed inside can be controlled by the size of the dendrimer because the diameter of the sphere can be controlled by growing the layer from the center one by one. With this, it is possible to arrange a note with a specific surface area.
- the ability to mix a catalyst-carrying dendrimer with a catalyst-free dendrimer and adjust the mixture to an S * value by mixing the two is essential. As a result, efficient power response can be achieved.
- Figure 2 (2) shows an example of a spherical force.
- the spherical carbon spacer portion 322 is, for example, a skeleton of carbon fiber 60, and is formed by crimping a proton affinity base portion 332 on the surface. Water proton, sulfone, etc. are provided as proton affinity groups. Luo 34 can be inserted into the gap where carbon 60 is lined up. Since this part is hidden by a space formed by carbon 60 with a diameter of about 0.7 nm, it can be made even smaller due to its structure, and it is possible to obtain a high specific surface area. These features allow efficient electrode operation.
- the porous electrode 10 having the structure shown in Difficult Form 1 or ⁇ S Form 2 is used as the proton conductive solid 5.
- the space of the porous electrode 10 contributes to the difficult reaction due to the diffusion of the fuel, and proton conduction on the surface 3 is performed.
- the porous body need not be a void as long as both functions described above can be provided.
- minute voids are formed in the filled portion 300 filled with a sphere having a proton affinity group on the surface: ⁇ . Since hydrogen can diffuse into such voids, an electrode reaction takes place up to the concealment.
- the protons can move not only on the surface 3 but also on the filling portion 300, the resistance of the fiber becomes small.
- the spacer 2 need not be formed first. That is, many Porous body 1 was filled with spherical ⁇ : The interface with ⁇ is spherical, and has the same function as forming the surface of the monolayer. If ⁇ is filled into the spherical liver, extra parts may be required more than necessary.
- a porous body having a specific surface area of about 50 m 2 / g was obtained by increasing the key of 0.1 m of carbon black.
- a spherical molecule used as a spacer was prepared as follows.
- a dendrimer was obtained, and the resulting dendrimer and a polyamidoamine dendrimer having a lipoxyl group on the surface (4.5th generation) (available from Aldrich recitation) in a molar ratio of 1: A mixed solution added to water was obtained at a ratio of 50.
- the size of the dendrimer used here was in the range of about 3 nm to 5 nm in diameter.
- the porous body was immersed in the above-mentioned ffig mixture at room temperature, and a dendrimer was adsorbed on the porous body surface to obtain a porous electrode A. At this time, it was about 0.1 mg m 2 .
- a porous electrode A was attached to a fluorinated high-quality film having a sulfonic acid group (trade name “Naphion” Dupont: ⁇ ) to form an electrochemical film.
- a porous electrode B was formed by applying a perfluoropolymer having a sulfonic acid group to the porous material thus mitered. This was combined with Naphion to form an electrochemical eave.
- porous body As the porous body was formed with an average pore size 0. lm, specific surface area 2 0 0m 2 / g, a density 4 0 0 k gZm 3 porous silica material having a thickness of about 2 0 nm electroless plated layer of gold on the surface of the I prepared something.
- a disulfide compound having a molecular structure of (S— (CH 2 ) 15 —COOH) 2 was added to acetone such that its content became 5 Ommo 1 / L, and a nighttime was prepared.
- the dendrimer having M in Example 1 was added to the same condition as the above.
- the dis-J sulfide group forms a monolayer on the surface of the porous body to be distributed to gold by itself.
- the surface of the obtained porous electrode is covered with a lipoxyl group.
- the dendrimer containing is contained in the organic layer composed of one (CH 2 ) 15 — part of the single film of the dis-J It is thought that it is taken in. Note that Tatsuko Hakuhaku as a participant was confirmed on the electron microscopic fiber, and there was no sign of ®® between each other because it was included in the dendrimer. Danji amount at this time was about 0. lmgZm 2.
- Example 1 E was measured using this porous electrode as a fuel cell. The output at this time was about 0.85 V, and it was confirmed that an efficient reaction was performed.
- porous body a sintered body obtained by inverting titanium oxide particles having an average particle diameter of about 100 nm and burning the body was used.
- Silane Cup Link J T- (2-aminoethyl) aminopropylmethoxysilane was added to isopropyl alcohol to a concentration of 5 Ommo 1 to prepare a vigorous night. This humid 3 ⁇ 4 [2 nm diameter platinum colloid was dispersed.
- a porous layer S was formed on the surface of which a monolayer having a silyl group chemically aged with titanium oxide was formed.
- the porous electrode of Example 1 was filled with a polyamine amine dendrimer having a carboxyl group on its surface (4.5th-century) to fill the space of the porous electrode.
- a porous amine D was obtained by filling a polyamine amine dendrimer (4.5th generation) having a lipoxyl group on the surface thereof into the space of the porous electrode B of Example 1.
- Example 6 Using the porous electrode D described above, an electrochemical device was obtained in the same manner as in Example 1. Hydrogen was introduced into one side of this electrochemical element, and air was introduced into the opposite side to form a fuel cell. When this output was measured, a value of 0.85 V was obtained, and it was confirmed that a more efficient reaction occurred than in the case of using the conventional porous electrode B in Example 1. ⁇ Example 6 >>
- polyhydroxycarbon 60 water mffd fullerene having a folloWing number of 60 and having a m-group formed on the surface was used.
- the liquid obtained by adding the hydroxylated fullerene to tetrahydrofuran was carbon-distilled at room temperature.
- a porous material having a hydroxylated fullerene adsorbed on the surface of the porous material as a spacer was obtained.
- the porous body was immersed in platinum ammonia water, and the platinum ammonium was inserted and hydrogenated at 180 ° C. to form platinum fine particles having an average diameter of about 2 nm, thereby obtaining an electrode.
- the platinum fine particles are not removed, so it is considered that they are formed in the gaps where the molecules gather.
- M * at this time was about 0.2 mg / m 2 .
- the porous electrode was attached to Nafion, which is a fluorine-based high-quality film having a sulfonic acid group, to form a mounted chemical element. Hydrogen was introduced into one surface of the chemical element, and air was introduced into the opposite surface to form a fuel tank. The output of this fuel cell was a voltage of 0.9 V, which was almost the same as that of the multi-electrode A in Example 1, and it was confirmed that an efficient reaction occurred.
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- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Composite Materials (AREA)
- Inert Electrodes (AREA)
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Abstract
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AU2003280670A AU2003280670A1 (en) | 2002-10-31 | 2003-10-31 | Porous electrode and electrochemical device using the same |
JP2004548097A JP3709484B2 (ja) | 2002-10-31 | 2003-10-31 | 多孔電極およびそれを用いた電気化学素子 |
US10/879,759 US7662505B2 (en) | 2002-10-31 | 2004-06-30 | Porous electrode, and electrochemical element made using the same |
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US10196748B2 (en) | 2013-05-29 | 2019-02-05 | Kabushiki Kaisha Toshiba | Reduction catalyst and chemical reactor |
WO2015136776A1 (ja) * | 2014-03-14 | 2015-09-17 | 株式会社 東芝 | 酸化電極および光電気化学装置 |
JP2015175020A (ja) * | 2014-03-14 | 2015-10-05 | 株式会社東芝 | 酸化電極および光電気化学装置 |
US10100418B2 (en) | 2014-03-14 | 2018-10-16 | Kabushiki Kaisha Toshiba | Oxidation electrode and photoelectrochemical device |
Also Published As
Publication number | Publication date |
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CN100347889C (zh) | 2007-11-07 |
US20050014060A1 (en) | 2005-01-20 |
US7662505B2 (en) | 2010-02-16 |
AU2003280670A1 (en) | 2004-05-25 |
JPWO2004040679A1 (ja) | 2006-03-02 |
CN1708869A (zh) | 2005-12-14 |
JP3709484B2 (ja) | 2005-10-26 |
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