WO2010106749A1 - 導電物被覆アルミニウム材とその製造方法 - Google Patents
導電物被覆アルミニウム材とその製造方法 Download PDFInfo
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- WO2010106749A1 WO2010106749A1 PCT/JP2010/001490 JP2010001490W WO2010106749A1 WO 2010106749 A1 WO2010106749 A1 WO 2010106749A1 JP 2010001490 W JP2010001490 W JP 2010001490W WO 2010106749 A1 WO2010106749 A1 WO 2010106749A1
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- layer
- aluminum
- aluminum material
- organic
- conductive material
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- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 title claims abstract description 207
- 229910052782 aluminium Inorganic materials 0.000 title claims abstract description 206
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- 239000011347 resin Substances 0.000 claims abstract description 62
- 239000000126 substance Substances 0.000 claims abstract description 38
- 239000012044 organic layer Substances 0.000 claims abstract description 36
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- 239000007833 carbon precursor Substances 0.000 claims abstract description 28
- 229930195733 hydrocarbon Natural products 0.000 claims abstract description 28
- 150000002430 hydrocarbons Chemical class 0.000 claims abstract description 28
- 239000004215 Carbon black (E152) Substances 0.000 claims abstract description 22
- CAVCGVPGBKGDTG-UHFFFAOYSA-N alumanylidynemethyl(alumanylidynemethylalumanylidenemethylidene)alumane Chemical compound [Al]#C[Al]=C=[Al]C#[Al] CAVCGVPGBKGDTG-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000011368 organic material Substances 0.000 claims description 48
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 35
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Images
Classifications
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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
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/665—Composites
- H01M4/667—Composites in the form of layers, e.g. coatings
-
- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C8/00—Solid state diffusion of only non-metal elements into metallic material surfaces; Chemical surface treatment of metallic material by reaction of the surface with a reactive gas, leaving reaction products of surface material in the coating, e.g. conversion coatings, passivation of metals
- C23C8/60—Solid state diffusion of only non-metal elements into metallic material surfaces; Chemical surface treatment of metallic material by reaction of the surface with a reactive gas, leaving reaction products of surface material in the coating, e.g. conversion coatings, passivation of metals using solids, e.g. powders, pastes
- C23C8/62—Solid state diffusion of only non-metal elements into metallic material surfaces; Chemical surface treatment of metallic material by reaction of the surface with a reactive gas, leaving reaction products of surface material in the coating, e.g. conversion coatings, passivation of metals using solids, e.g. powders, pastes only one element being applied
- C23C8/64—Carburising
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/22—Electrodes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/22—Electrodes
- H01G11/24—Electrodes characterised by structural features of the materials making up or comprised in the electrodes, e.g. form, surface area or porosity; characterised by the structural features of powders or particles used therefor
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/22—Electrodes
- H01G11/26—Electrodes characterised by their structure, e.g. multi-layered, porosity or surface features
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/22—Electrodes
- H01G11/26—Electrodes characterised by their structure, e.g. multi-layered, porosity or surface features
- H01G11/28—Electrodes characterised by their structure, e.g. multi-layered, porosity or surface features arranged or disposed on a current collector; Layers or phases between electrodes and current collectors, e.g. adhesives
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/22—Electrodes
- H01G11/30—Electrodes characterised by their material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/66—Current collectors
- H01G11/68—Current collectors characterised by their material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/74—Terminals, e.g. extensions of current collectors
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/84—Processes for the manufacture of hybrid or EDL capacitors, or components thereof
- H01G11/86—Processes for the manufacture of hybrid or EDL capacitors, or components thereof specially adapted for electrodes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
- H01G9/04—Electrodes or formation of dielectric layers thereon
- H01G9/042—Electrodes or formation of dielectric layers thereon characterised by the material
- H01G9/045—Electrodes or formation of dielectric layers thereon characterised by the material based on aluminium
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
- H01G9/04—Electrodes or formation of dielectric layers thereon
- H01G9/048—Electrodes or formation of dielectric layers thereon characterised by their structure
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
- H01G9/04—Electrodes or formation of dielectric layers thereon
- H01G9/048—Electrodes or formation of dielectric layers thereon characterised by their structure
- H01G9/055—Etched foil 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
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
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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
- 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
- Y02E60/10—Energy storage using batteries
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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
- 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
- Y02E60/13—Energy storage using capacitors
-
- 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
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/24—Structurally defined web or sheet [e.g., overall dimension, etc.]
- Y10T428/24802—Discontinuous or differential coating, impregnation or bond [e.g., artwork, printing, retouched photograph, etc.]
- Y10T428/24851—Intermediate layer is discontinuous or differential
Definitions
- the present invention generally relates to a conductive material-coated aluminum material in which the surface of an aluminum material is coated with a conductive material, and a method for producing the same. Specifically, the current collectors and electrodes of various capacitors, the current collectors of various batteries, The present invention relates to a conductive material-coated aluminum material used for electrodes and the like and a method for producing the same.
- Patent Document 1 Japanese Patent Application Laid-Open No. 2000-164466
- a carbon intermediate film is provided on a current collector formed of aluminum, and activated carbon, carbon black, and a binder are formed thereon.
- an active material layer made of a paste-like mixed material mixed with methylcellulose as an adhesive is coated as a conductive material.
- the composite material obtained by the above method has a structure in which the conductive carbon particles themselves are supported on the surface of the aluminum material, which is the base material, and thus is exposed to a high temperature and high humidity atmosphere for a long time.
- moisture contained in the atmosphere enters between the carbon particles and causes a hydration reaction at the interface between the carbon particles and the aluminum material.
- this composite material is used for a capacitor or a battery, a corrosive component contained in the capacitor or the battery often accelerates the progress of the hydration reaction.
- Patent Document 1 Although carbon particles that are conductive materials are fixed using a binder, not only the properties of the binder itself deteriorate due to long-term use, but also the hydration reaction described above. As a result, the conductivity decreases.
- the object of the present invention is that the conductive material that ensures the conductivity of the surface does not peel off from the aluminum material even when used under high humidity conditions, and is preferably used as a material for a current collector or electrode. It is to provide a conductive material coated aluminum material and a method for manufacturing the same.
- the present inventor obtained the following knowledge as a result of earnest research.
- the conductive material-containing layer is configured to contain a substance exhibiting conductivity without using carbon particles, the above hydration reaction can be suppressed.
- the inventor thought that this could be done. That is, the inventor forms an organic material layer on the surface of an aluminum material as a conductive material-containing layer, and configures the conductive material-containing layer so that a carbon precursor is contained as a conductive material in the organic material layer. It came to the idea that it should be.
- a resin layer is formed on the surface of an aluminum material.
- the aluminum material having the resin layer formed on the surface thereof is heated in the space containing the hydrocarbon-containing substance, so that the resin layer formed on the surface of the aluminum material remains as an organic layer after the heating step.
- This organic layer has a very dense structure. This dense structure makes it possible to suppress the intrusion of moisture contained in the atmosphere when exposed to a high temperature and high humidity atmosphere for a long period of time.
- this organic substance layer contains a carbon precursor, it becomes possible to ensure electrical conductivity without supporting carbon particles on the surface of the aluminum material due to the presence of this carbon precursor.
- the conductive material-coated aluminum material according to the present invention includes an aluminum material, an organic material layer formed on the surface of the aluminum material, and at least a part of the surface of the aluminum material between the aluminum material and the organic material layer. And an organic layer containing a carbon precursor as a conductive material.
- an intervening layer containing an aluminum carbide formed between the aluminum material and the organic material layer was formed on the surface of the aluminum material and the surface of the aluminum material. It works to enhance the adhesion with the organic layer.
- the organic layer has a very dense structure, a hydration reaction with moisture in a high humidity atmosphere can be suppressed.
- the presence of the carbon precursor in the organic material layer can ensure electrical conductivity without supporting carbon particles on the surface of the aluminum material.
- the carbon precursor contained in the organic material layer preferably contains at least carbon and hydrogen elements, and contains a component similar to graphite or a component similar to amorphous carbon.
- the carbon precursor contained in the organic material layer contains at least carbon and hydrogen elements, and the Raman shift detected by Raman spectroscopy has a Raman shift of 1350 cm ⁇ . It is preferable to have a peak of Raman scattering intensity around 1 or 1580 cm ⁇ 1 .
- the organic material layer is preferably formed from a substance that does not volatilize by heating within a temperature range of 450 ° C. or higher and lower than 660 ° C. for 1 hour or longer and 100 hours or shorter.
- the organic material layer By forming the organic material layer from the above materials, it is possible to form a structure with few defects and cracks.
- the conductive material-covered aluminum material having any of the above-described characteristics according to the present invention is used for constituting an electrode structure.
- the above electrode structure is preferably used to constitute a current collector and an electrode of a capacitor.
- capacitance characteristic, internal resistance characteristic, charging / discharging characteristic, and lifetime of a capacitor can be improved.
- the capacitor include an electric double layer capacitor, an aluminum electrolytic capacitor, and a functional solid capacitor.
- the above electrode structure is preferably used for constituting a battery current collector and an electrode.
- capacitance characteristic, internal resistance characteristic, charging / discharging characteristic, and lifetime of a battery can be improved.
- the battery include a secondary battery such as a lithium ion battery.
- the method for producing a conductive material-coated aluminum material according to the present invention includes the following steps.
- the organic material layer is made of an aluminum material by placing the aluminum material and the resin layer in a space containing a hydrocarbon-containing substance and heating them. Formed on the surface.
- the resin layer is heated in an atmosphere containing a hydrocarbon-containing substance, but is not completely oxidized or lost, and becomes an organic layer containing a carbon precursor.
- the organic layer formed on the surface of the aluminum material has a very dense structure, the hydration reaction with moisture in a high humidity atmosphere can be suppressed. Furthermore, the presence of the carbon precursor in the organic material layer can ensure electrical conductivity without supporting carbon particles on the surface of the aluminum material.
- the resin layer forming step preferably includes a step of mixing a resin and a solvent.
- the resin layer can be uniformly formed on the surface of the aluminum material, and the organic layer formed through the subsequent steps can be uniformly formed on the surface of the aluminum material.
- an organic material layer having a uniformly dense structure is formed on the surface of the aluminum material, and hydration reaction with moisture in a high humidity atmosphere can be suppressed at any location on the surface of the aluminum material. .
- the organic layer forming step is preferably performed in a temperature range of 450 ° C. or higher and lower than 660 ° C.
- the organic material layer is provided on the surface of the aluminum material, intrusion of moisture contained in the atmosphere can be suppressed when exposed to a high temperature and high humidity atmosphere for a long time. It becomes like this.
- this organic substance layer contains a carbon precursor, the presence of this carbon precursor makes it possible to ensure electrical conductivity without supporting carbon particles on the surface of the aluminum material. As a result, it is possible to ensure conductivity while suppressing the hydration reaction with moisture in a high-humidity atmosphere as compared with conventional conductive material-covered aluminum materials. Thus, it becomes possible to use the conductive material-coated aluminum material of the present invention for a long period of time.
- an organic material layer 2 is formed on the surface of an aluminum foil 1 as an example of an aluminum material.
- An intervening layer 3 containing an aluminum element and a carbon element is formed between the aluminum foil 1 and the organic material layer 2.
- the intervening layer 3 is formed in at least a part of the surface of the aluminum foil 1 and contains an aluminum carbide, for example, Al 4 C 3 .
- the organic layer 2 contains a carbon precursor.
- the organic layer 2 has a portion that is in direct contact with the aluminum foil 1 and a portion that is in close contact with the aluminum foil 1 through the intervening layer 3.
- the organic material layer 2 has sufficient adhesion by directly adhering to the aluminum foil 1, but the organic material layer 2 is more firmly adhered to the aluminum foil 1 due to the presence of the intervening layer 3. .
- the organic material layer 2 is attached on a partial region of the intervening layer 3.
- Part of the organic material layer 2 formed on the surface of the aluminum foil 1 adheres on the surface of a part of the intervening layer 3, and the other part of the organic material layer 2 is not on the surface of the interposing layer 3. Further, it may be directly attached on the surface of the aluminum foil 1 where the intervening layer 3 is not formed.
- the plurality of intervening layers 3 are formed in an island shape on the surface of the aluminum foil 1 at intervals, but are formed in an island shape adjacent to each other. Also good.
- an intervening layer 3 containing an aluminum carbide formed between the aluminum foil 1 and the organic material layer 2 is formed on the surface of the aluminum foil 1. It acts to increase the adhesion with the organic material layer 2 formed on the surface of the aluminum foil 1. As a result of this action, moisture can be prevented from entering between the aluminum foil 1 and the organic layer 2 even under high humidity conditions.
- the carbon precursor contained in the organic material layer 2 formed on the surface of the aluminum foil 1 preferably contains at least carbon and hydrogen elements, and contains a component similar to graphite or a component similar to amorphous carbon. Those are preferred. In addition, it is guessed that the resin layer formed in the surface of the aluminum foil 1 changes to a carbon precursor by the heating process mentioned later.
- the conductive material-coated aluminum material of the present invention having the above-described structure preferably has a longer time until the organic layer 2 is completely peeled from the aluminum foil 1 in the hydrochloric acid peeling test specified below.
- ⁇ Hydrochloric acid peel test> A strip-shaped conductive material-covered aluminum material having a width of 10 mm and a length of 100 mm is immersed in a hydrochloric acid solution at 80 ° C. and 1 M (M means volume molar concentration [mol / liter]). Measure the time until complete peeling.
- an aluminum material (aluminum foil 1 as an example in the above embodiment) as a substrate on which the organic layer 2 is formed is not particularly limited, and pure aluminum or an aluminum alloy is used. be able to.
- Such an aluminum material preferably has an aluminum purity of 98% by mass or more as a value measured according to the method described in “JIS H2111”.
- the aluminum material used in the present invention has a composition of lead (Pb), silicon (Si), iron (Fe), copper (Cu), manganese (Mn), magnesium (Mg), chromium (Cr), zinc ( Zn alloy, titanium (Ti), vanadium (V), gallium (Ga), nickel (Ni), and aluminum alloy to which at least one alloy element is added within the necessary range, or the above inevitable It also includes aluminum with limited impurity element content.
- the thickness of the aluminum material is not particularly limited, but it is preferably 5 ⁇ m or more and 200 ⁇ m or less for a foil, and more than 200 ⁇ m and 3 mm or less for a plate.
- the above-mentioned aluminum material can be manufactured by a known method. For example, a molten aluminum or aluminum alloy having the above-mentioned predetermined composition is prepared, and an ingot obtained by casting this is appropriately homogenized. Thereafter, an aluminum material can be obtained by subjecting the ingot to hot rolling and cold rolling. In addition, you may perform an intermediate annealing process in the range of 150 degreeC or more and 400 degrees C or less in the middle of said cold rolling process.
- the conductive material-coated aluminum material having any of the above-described characteristics according to the present invention is preferably used for constituting an electrode structure.
- the above electrode structure is preferably used for constituting a current collector or an electrode of a capacitor. Thereby, the capacity
- the capacitor include an electric double layer capacitor, an aluminum electrolytic capacitor, and a functional solid capacitor.
- the above electrode structure is preferably used for constituting a current collector or electrode of a battery.
- capacitance characteristic, internal resistance characteristic, charging / discharging characteristic, and lifetime of a battery can be improved.
- the battery include a secondary battery such as a lithium ion battery.
- a resin layer is formed on the surface of the aluminum foil 1 (resin layer forming step).
- the aluminum foil 1 on which the resin layer is formed is placed in a space containing a hydrocarbon-containing substance and heated to form an organic substance layer containing a carbon precursor (organic substance layer forming step).
- organic substance layer forming step By this organic substance layer formation process, as shown in FIG. 1, the organic substance layer 2 is formed on the surface of the aluminum foil 1.
- the aluminum foil 1 can be covered with the organic layer 2 by a simple process of placing the aluminum foil 1 in a space containing a hydrocarbon-containing substance and heating it.
- an intervening layer 3 containing aluminum carbide can be formed between the aluminum foil 1 and the organic layer 2.
- the aluminum foil 1 and the resin layer are arranged in a space containing a hydrocarbon-containing substance in the organic layer forming step. Then, the organic layer 2 is formed on the surface of the aluminum foil 1 as shown in FIG.
- the resin layer is heated in an atmosphere containing a hydrocarbon-containing substance, but does not completely oxidize and disappear, and becomes an organic layer 2 containing a carbon precursor. Thereby, electroconductivity is provided to the organic layer 2.
- the organic layer 2 has a very dense structure, the presence of the organic layer 2 on the surface of the aluminum foil 1 can suppress a hydration reaction with moisture in a high humidity atmosphere. . This makes it possible to use the conductive material-coated aluminum material for a long period of time in a harsh atmosphere at a higher temperature and higher humidity than before.
- the resin layer forming step preferably includes a step of mixing a resin and a solvent (mixing step).
- a resin layer can be uniformly formed on the surface of the aluminum foil 1, and an organic layer 2 formed through subsequent steps can be uniformly formed on the surface of the aluminum foil 1. It becomes. Thereby, the organic substance layer 2 which has a dense structure uniformly on the surface of the aluminum foil 1 is formed, and the hydration reaction with moisture in a high humidity atmosphere is suppressed at any location on the surface of the aluminum foil 1. be able to.
- the mixing method and the mixing time are not particularly limited as long as the resin layer is uniformly formed.
- the amount of the solvent to be added is preferably 50% by mass or less with respect to the resin addition amount.
- the resin used in the resin layer forming step is not particularly limited, and examples thereof include resins having a cyclic structure such as polyvinyl alcohol, polyvinyl butyral, epoxy, and aromatic (for example, phenol) and acrylic resins. In particular, phenolic resins are preferred.
- the solvent appropriately used in the resin layer forming step is not particularly limited, but is preferably a resin solvent (a solvent in which the resin is easily dissolved).
- a resin solvent a solvent in which the resin is easily dissolved.
- an oil-soluble resin is used as the resin, methyl isobutyl ketone, toluene, methyl ethyl ketone and the like can be mentioned.
- a resin and an appropriate solvent are used to prepare a slurry or a liquid, by coating, dipping, etc. What is necessary is just to adhere what was prepared in the solid form on the surface of the aluminum foil 1 by spraying in the form of a powder, extrusion, thermocompression bonding, etc.
- the resin layer After the resin layer is deposited on the surface of the aluminum foil 1, it may be dried at a temperature in the range of 20 ° C. or more and 300 ° C. or less before the heat treatment.
- the organic material layer 2 may be formed on at least one surface of the aluminum foil 1, and the thickness is preferably in the range of 0.01 ⁇ m to 10 mm.
- the organic material layer may be formed on the entire surface of the aluminum material, but a portion that does not form the organic material layer may be provided on a portion of the surface of the aluminum material depending on the intended use (for example, For example, if you want to provide a portion of the aluminum material where the organic layer is not formed to connect to the terminal).
- the type of the hydrocarbon-containing substance used is not particularly limited.
- the hydrocarbon-containing material include paraffinic hydrocarbons such as methane, ethane, propane, n-butane, isobutane and pentane, olefinic hydrocarbons such as ethylene, propylene, butene and butadiene, and acetylenes such as acetylene.
- examples thereof include hydrocarbons and derivatives of these hydrocarbons.
- paraffinic hydrocarbons such as methane, ethane, and propane are preferable because they become gaseous in the process of heating the aluminum material. More preferred is any one of methane, ethane and propane. The most preferred hydrocarbon is methane.
- the hydrocarbon-containing substance may be used in any state such as liquid or gas in the production method of the present invention.
- the hydrocarbon-containing material may be present in the space where the aluminum material is present, and may be introduced into the space where the aluminum material is disposed by any method.
- the hydrocarbon-containing substance is gaseous (methane, ethane, propane, etc.)
- the hydrocarbon-containing substance may be filled alone or together with an inert gas in a sealed space where the heat treatment of the aluminum material is performed.
- the hydrocarbon-containing substance is a liquid
- the hydrocarbon-containing substance may be filled alone or together with an inert gas so as to be vaporized in the sealed space.
- the pressure of the heating atmosphere is not particularly limited, and may be normal pressure, reduced pressure, or increased pressure. Further, the pressure adjustment may be performed at any time during the temperature rise to a certain heating temperature or during the temperature lowering from the certain heating temperature while the pressure is maintained at a certain heating temperature.
- the mass ratio of the hydrocarbon-containing substance introduced into the space for heating the aluminum material is not particularly limited. It is preferable to make it into the range of 0.5 mass part or more and 30 mass parts or less especially.
- the heating temperature may be appropriately set according to the composition of the aluminum material that is the object to be heated, but it is preferably within the range of 450 ° C. or higher and lower than 660 ° C. More preferably, it is carried out within the range of not more than ° C. However, in the production method of the present invention, heating the aluminum material at a temperature lower than 450 ° C. is not excluded, and the aluminum material may be heated at a temperature exceeding at least 300 ° C.
- the heating time is generally in the range of 1 hour to 100 hours, although it depends on the heating temperature and the like.
- the oxygen concentration in the heating atmosphere is preferably 1.0% by volume or lower.
- the thermal oxide film on the surface of the aluminum material may be enlarged, and the surface resistance value of the aluminum material may increase.
- the surface of the aluminum material may be roughened before the heat treatment.
- the surface roughening method is not particularly limited, and known techniques such as cleaning, etching, blasting and the like can be used.
- Examples 1 to 5 To 1 part by mass of various resins shown in “Resin used in resin layer forming step” in Table 1, 4 parts by mass of various solvents shown in “Solvent” in Table 1 are added, mixed and dissolved. A coating solution having a solid content of 20% by mass was obtained.
- a resin layer was formed by applying these coating solutions on both surfaces of an aluminum foil having a thickness of 50 ⁇ m and a purity of 99.3% by mass, and dried at a temperature of 150 ° C. for 30 seconds (resin layer forming step). The thickness of the resin layer after drying was 1 to 3 ⁇ m on one side. Then, the organic layer was formed by hold
- the cross section was observed using a scanning electron microscope (SEM).
- FIG. 2 shows a photograph of a cross section of a conductive material-coated aluminum material sample of Example 4 observed with a scanning electron microscope (SEM).
- SEM scanning electron microscope
- the organic material layer (relatively dark portion) has a very dense structure in the conductive material-covered aluminum material.
- FIG. 3 is a photograph of the back surface of the intervening layer 3 exposed by removing the aluminum foil 1 in FIG.
- the magnification of the photograph is 3000 times, 10000 times, and 15000 times in the order of the arrows.
- the components contained in the organic layer were confirmed by Raman spectrum detected by Raman spectroscopy (measurement device name: microscopic Raman device Ramascope1000 manufactured by RENISHAW). shift detecting a peak of the Raman scattering intensity corresponding to amorphous carbon in the vicinity of 1350 cm -1, further Raman shift detects a peak of the Raman scattering intensity corresponding to graphite in the vicinity of 1580 cm -1.
- the Raman spectrum is shown in FIG.
- Comparative Example 1 By dispersing 1 part by mass of carbon black particles having an average particle diameter of 20 nm in butanol shown in “Solvent” in Table 1, carbon having a solid content of 20% by mass as a coating liquid having a solid content of 20% by mass is obtained. A coating solution containing black particles was obtained. This coating solution was applied to both sides of an aluminum foil having a thickness of 50 ⁇ m and a purity of 99.3% by mass, and dried at a temperature of 150 ° C. for 30 seconds (step corresponding to the resin layer forming step). The thickness of the carbon black particle-containing layer after drying was 1 ⁇ m on one side.
- the production method of this comparative example corresponds to a method in which a carbon black particle-containing layer in which carbon black particles are dispersed in a solvent is formed instead of the resin layer formation step in the production method of the present invention.
- Comparative Example 2 1 part by weight of 2 parts by weight of carbon black particles having an average particle diameter of 20 nm is a polyvinyl chloride resin (in this case, acting as a binder for the carbon black particles) shown in “Resin used in the resin layer forming step” in Table 1.
- a coating liquid used in the step corresponding to the resin layer forming step by mixing with a part and dispersing in a mixed solvent of toluene and methyl ethyl ketone (mixing ratio 1: 1) shown in “Solvent” in Table 1, A coating liquid containing carbon black particles having a solid content of 20% by mass was obtained.
- This coating solution was applied to both sides of an aluminum foil having a thickness of 50 ⁇ m and a purity of 99.3% by mass, and dried at a temperature of 150 ° C. for 30 seconds (step corresponding to the resin layer forming step).
- the thickness of the carbon black particle-containing layer after drying was 1 ⁇ m on one side.
- the carbon foil was formed by hold
- a conductor-coated aluminum material as Comparative Example 2 was produced.
- the production method of this comparative example corresponds to a method in which a carbon black particle-containing layer in which carbon black particles and a binder are dispersed in a solvent is formed instead of the resin layer formation step in the production method of the present invention.
- the conductive material-coated aluminum materials of Examples 1 to 5 have the following effects. That is, the conductive material-coated aluminum materials of Examples 1 to 5 do not contain carbon black particles as a conductive material, and the organic material layer 2 is formed on the surface of the aluminum foil 1. Since the organic layer 2 has a very dense structure, intrusion of moisture contained in the atmosphere can be suppressed when exposed for a long time in an atmosphere of high temperature and high humidity. Moreover, since this organic substance layer 2 contains a carbon precursor, it becomes possible to ensure conductivity even if carbon particles are not supported on the surface of the aluminum foil 1 due to the presence of this carbon precursor.
- the conductor-coated aluminum material of the present invention can be used for a long time in a harsh atmosphere.
- electrodes and current collectors of capacitors such as electric double layer capacitors, aluminum electrolytic capacitors and functional solid capacitors, current collectors and electrodes of secondary batteries such as lithium ion batteries, etc.
- capacitors such as electric double layer capacitors, aluminum electrolytic capacitors and functional solid capacitors, current collectors and electrodes of secondary batteries such as lithium ion batteries, etc.
Abstract
Description
このような炭素前駆体を有機物層中に含ませることにより、導電性を示す有機物層を形成することができる。
幅10mm、長さ100mmの短冊状の導電物被覆アルミニウム材を、80℃、1M(Mは、体積モル濃度[mol/リットル]を意味する)の塩酸溶液中に浸漬し、アルミニウム材から有機物層が完全に剥離するまでの時間を測定する。
表1の「樹脂層形成工程で用いる樹脂」に示された各種の樹脂1質量部に対して、表1の「溶媒」に示された各種の溶媒4質量部を加えて混合して溶解させ、固形分20質量%の塗工液を得た。なお、実施例2~5の「溶媒」であるトルエンとメチルエチルケトンとの混合溶媒の混合比は1:1である。
平均粒径が20nmのカーボンブラック粒子1質量部を、表1の「溶媒」に示されたブタノールに分散させることにより、固形分20質量%の塗工液として、固形分が20質量%のカーボンブラック粒子を含む塗工液を得た。この塗工液を厚みが50μmで純度が99.3質量%のアルミニウム箔の両面に塗布し、温度150℃で30秒間乾燥した(樹脂層形成工程に対応する工程)。なお、乾燥後のカーボンブラック粒子含有層の厚みは片面で1μmであった。その後、両面にカーボンブラック粒子含有層が形成されたアルミニウム箔を、メタンガス雰囲気中にて温度550℃で10時間保持することにより、炭素含有層を形成した(有機物層形成工程に対応する工程)。このようにして、比較例1としての導電物被覆アルミニウム材を作製した。本比較例の製造方法は、本発明の製造方法における樹脂層形成工程に代えて、カーボンブラック粒子を溶媒で分散させたカーボンブラック粒子含有層を形成する工程を行なったものに相当する。
平均粒径が20nmのカーボンブラック粒子2質量部を、表1の「樹脂層形成工程で用いる樹脂」に示されたポリ塩化ビニル系樹脂(この場合、カーボンブラック粒子のバインダーとして作用する)1質量部と混合し、表1の「溶媒」に示されたトルエンとメチルエチルケトンとの混合溶媒(混合比1:1)に分散させることにより、樹脂層形成工程に対応する工程で用いる塗工液として、固形分が20質量%のカーボンブラック粒子を含む塗工液を得た。この塗工液を厚みが50μmで純度が99.3質量%のアルミニウム箔の両面に塗布し、温度150℃で30秒間乾燥した(樹脂層形成工程に対応する工程)。なお、乾燥後のカーボンブラック粒子含有層の厚みは片面で1μmであった。その後、両面にカーボンブラック粒子含有層が形成されたアルミニウム箔を、メタンガス雰囲気中にて温度550℃で10時間保持することにより、炭素含有層を形成した(有機物層形成工程に対応する工程)。このようにして、比較例2としての導電物被覆アルミニウム材を作製した。本比較例の製造方法は、本発明の製造方法における樹脂層形成工程に代えて、カーボンブラック粒子とバインダーを溶媒で分散させたカーボンブラック粒子含有層を形成する工程を行なったものに相当する。
実施例1~5、比較例1~2で得られた、導電物被覆アルミニウム材における有機物層2(比較例1~2では炭素含有層)の導電性試験、導電物被覆アルミニウム材の経時信頼性試験(塩酸剥離試験、水和反応試験)の結果を表1に示す。なお、評価条件は以下に示す通りである。
作製した実施例1~5、比較例1~2の導電物被覆アルミニウム材の導電性を次のようにして評価した。まず、作製した実施例1~5、比較例1~2の導電物被覆アルミニウム材から、試験試料として、幅20mm、長さ100mmの矩形状に切断した試料を準備した。サンドペーパーを用いて、この試料の一部において表層の導電物層を削り落とした。このようにして作製された試験試料のアルミニウム部と導電物層の各表面に、テスター(三和電気計器(株)製DIGITAL MULTIMETER PM5)の導通チェックモードを使って、各端子を押し当て導電性を確認した。その評価結果を表1の「導電性」に示す。
まず、作製した実施例1~5、比較例1~2の導電物被覆アルミニウム材から、試験試料として、幅10mm、長さ100mmの短冊状に切断した試料を準備した。そして、この試験試料を、80℃、1M(Mは、体積モル濃度[mol/リットル]を意味する)の塩酸溶液中に浸漬し、有機物層2(比較例1~2においては炭素含有層)が完全に剥離するまでの時間を測定した。その測定された時間を表1の「塩酸剥離時間」に示す。
まず、作製した実施例1~5、比較例1~2の導電物被覆アルミニウム材から、試験試料として、幅65mm、長さ70mmのサイズに切り出した試料を準備した。そして、この試験試料を、80℃に加熱した純水に60分間浸漬し、水和反応により発生したガスを回収し、その体積を測定し、その測定された体積を水和反応の量と評価した。その量を表1の「水和反応量」に示す。
Claims (9)
- アルミニウム材(1)と、
前記アルミニウム材(1)の表面上に形成された有機物層(2)と、
前記アルミニウム材(1)と前記有機物層(2)との間で前記アルミニウム材(1)の表面の少なくとも一部の領域に形成された、アルミニウムの炭化物を含む介在層(3)とを備え、
前記有機物層(2)は炭素前駆体を含む、導電物被覆アルミニウム材。 - 前記炭素前駆体は、少なくとも炭素および水素の元素を含み、かつ、ラマン分光法によって検出されたラマンスペクトルにおいてラマンシフトが1350cm-1付近または1580cm-1付近にラマン散乱強度のピークを有する、請求項1に記載の導電物被覆アルミニウム材。
- 前記有機物層(2)は、450℃以上660℃未満の温度範囲で1時間以上100時間以下の範囲内での加熱により揮発しない物質から形成される、請求項1に記載の導電物被覆アルミニウム材。
- 当該導電物被覆アルミニウム材は、電極構造体を構成するために用いられる、請求項1に記載の導電物被覆アルミニウム材。
- 前記電極構造体はキャパシタの集電体および電極である、請求項4に記載の導電物被覆アルミニウム材。
- 前記電極構造体は電池の集電体および電極である、請求項4に記載の導電物被覆アルミニウム材。
- アルミニウム材(1)の表面に、樹脂層を形成する樹脂層形成工程と、
前記樹脂層が形成されたアルミニウム材(1)を、炭化水素含有物質を含む空間に配置して、加熱することにより、炭素前駆体を含む有機物層(2)を形成する有機物層形成工程とを備える、導電物被覆アルミニウム材の製造方法。 - 前記樹脂層形成工程は、樹脂と溶媒とを混合する工程を含む、請求項7に記載の導電物被覆アルミニウム材の製造方法。
- 前記有機物層形成工程は、450℃以上660℃未満の温度範囲で行う、請求項7に記載の導電物被覆アルミニウム材の製造方法。
Priority Applications (3)
Application Number | Priority Date | Filing Date | Title |
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CN201080012506.4A CN102356176B (zh) | 2009-03-17 | 2010-03-04 | 导电物包覆铝材及其制造方法 |
EP10753246.7A EP2410071A4 (en) | 2009-03-17 | 2010-03-04 | Aluminum member covered with conductive coat and process for production of same |
US13/203,869 US20110318550A1 (en) | 2009-03-17 | 2010-03-04 | Electrically conductive substance coated aluminum material and method for manufacturing the same |
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JP2009-064187 | 2009-03-17 | ||
JP2009064187A JP5649285B2 (ja) | 2009-03-17 | 2009-03-17 | 導電物被覆アルミニウム材とその製造方法 |
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US (1) | US20110318550A1 (ja) |
EP (1) | EP2410071A4 (ja) |
JP (1) | JP5649285B2 (ja) |
KR (1) | KR101631838B1 (ja) |
CN (1) | CN102356176B (ja) |
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Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
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JP6167243B1 (ja) * | 2016-06-17 | 2017-07-19 | Tpr株式会社 | 電気二重層キャパシタ |
Families Citing this family (7)
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JP5325326B2 (ja) * | 2011-10-26 | 2013-10-23 | 株式会社神戸製鋼所 | 集電体、電極、二次電池、および二次電池の製造方法 |
KR101325633B1 (ko) * | 2011-12-21 | 2013-11-07 | 비나텍주식회사 | 리튬 이온 커패시터의 집전체 구조물, 이를 포함하는 전극 및 이를 포함하는 리튬 이온 커패시터 |
CN105579609B (zh) * | 2013-09-26 | 2019-04-12 | 东洋铝株式会社 | 包覆铝材及其制造方法 |
CN104347278A (zh) * | 2014-11-14 | 2015-02-11 | 深圳市今朝时代新能源技术有限公司 | 一种超级电容器用涂层铝箔的制备方法 |
CN109417158A (zh) * | 2016-05-06 | 2019-03-01 | 深圳中科瑞能实业有限公司 | 一种负极材料及其制备方法、含所述负极材料的负极及二次电池 |
CN106435494A (zh) * | 2016-08-12 | 2017-02-22 | 深圳市第四能源科技有限公司 | 一种改善锂电池正极集电极电性能的方法 |
CN114899409B (zh) * | 2022-05-18 | 2023-12-05 | 上海瑞浦青创新能源有限公司 | 一种碳纳米管纤维集流体的制备方法 |
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- 2010-03-04 EP EP10753246.7A patent/EP2410071A4/en active Pending
- 2010-03-04 US US13/203,869 patent/US20110318550A1/en not_active Abandoned
- 2010-03-04 KR KR1020117024123A patent/KR101631838B1/ko active IP Right Grant
- 2010-03-04 CN CN201080012506.4A patent/CN102356176B/zh active Active
- 2010-03-16 TW TW099107574A patent/TWI496684B/zh active
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JP6167243B1 (ja) * | 2016-06-17 | 2017-07-19 | Tpr株式会社 | 電気二重層キャパシタ |
US10636581B2 (en) | 2016-06-17 | 2020-04-28 | Tpr Co., Ltd. | Electric double layer capacitor |
Also Published As
Publication number | Publication date |
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JP5649285B2 (ja) | 2015-01-07 |
EP2410071A4 (en) | 2018-06-20 |
US20110318550A1 (en) | 2011-12-29 |
KR101631838B1 (ko) | 2016-06-20 |
TW201036811A (en) | 2010-10-16 |
JP2010215964A (ja) | 2010-09-30 |
CN102356176B (zh) | 2015-11-25 |
TWI496684B (zh) | 2015-08-21 |
KR20110133487A (ko) | 2011-12-12 |
CN102356176A (zh) | 2012-02-15 |
EP2410071A1 (en) | 2012-01-25 |
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