WO2007013693A2 - Dispositif electrochimique - Google Patents

Dispositif electrochimique Download PDF

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Publication number
WO2007013693A2
WO2007013693A2 PCT/JP2006/315451 JP2006315451W WO2007013693A2 WO 2007013693 A2 WO2007013693 A2 WO 2007013693A2 JP 2006315451 W JP2006315451 W JP 2006315451W WO 2007013693 A2 WO2007013693 A2 WO 2007013693A2
Authority
WO
WIPO (PCT)
Prior art keywords
group
cation
polarizable electrode
activated carbon
ionic liquid
Prior art date
Application number
PCT/JP2006/315451
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English (en)
Japanese (ja)
Other versions
WO2007013693A3 (fr
Inventor
Atushi Nishino
Original Assignee
Koei Chemical Company, Limited
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Koei Chemical Company, Limited filed Critical Koei Chemical Company, Limited
Priority to KR1020087002258A priority Critical patent/KR101332081B1/ko
Publication of WO2007013693A2 publication Critical patent/WO2007013693A2/fr
Publication of WO2007013693A3 publication Critical patent/WO2007013693A3/fr

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-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
    • H01G11/32—Carbon-based
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-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, LIGHT-SENSITIVE OR TEMPERATURE-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
    • H01G11/32—Carbon-based
    • H01G11/38—Carbon pastes or blends; Binders or additives therein
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-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
    • H01G11/54—Electrolytes
    • H01G11/58—Liquid electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-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
    • H01G11/54—Electrolytes
    • H01G11/58—Liquid electrolytes
    • H01G11/60—Liquid electrolytes characterised by the solvent

Definitions

  • the present invention relates to an electrochemical element, and more particularly to an electric double layer capacitor and a polarizable electrode that can be used therefor.
  • Electric double layer capacitors which are representative of electrochemical devices, use a technology that accumulates electrical energy in an electric double layer formed at the interface between a polarizable electrode such as activated carbon and an electrolyte, and is rapidly It is a capacitor that can be charged and has a long charge / discharge cycle life.
  • Applications of this electric double layer capacitor include memory backup, electric vehicle power assist, and power storage battery replacement, and are being widely studied from small-capacity products to large-capacity products.
  • the quaternary ammonium salt (ionic liquid, ionic liquid, or room temperature melting) exists as a stable liquid in a wide temperature range including near room temperature in order to maintain high temperature stability in the electrolyte.
  • ionic liquid ionic liquid, or room temperature melting
  • polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PTFE) and poly (vinylidene fluoride) are used for polarizable electrodes to maintain their shape and strength.
  • PTFE polytetrafluoroethylene
  • PTFE polyvinylidene fluoride
  • PVDF activated carbon containing polyfluorinated olefins
  • the time required for impregnation of the ionic liquid into the polarizable electrode is relatively long, which is not yet satisfactory for industrial production of the above-described electrochemical device.
  • the above-mentioned electrochemical element cannot be sufficiently impregnated with an ionic liquid, it is also satisfactory in terms of stability at high temperatures, which is likely to cause leakage of the ionic liquid, particularly at high temperatures where the viscosity of the ionic liquid decreases. It is difficult. Disclosure of the invention
  • An object of the present invention is to provide an electrochemical device in which the above-mentioned drawbacks are improved.
  • Another object of the present invention is to provide a polarizable electrode suitable for use in such an electrochemical device.
  • a polarizable electrode can be impregnated into a polarizable electrode in a short time by using rubber as a binder for a polarizable electrode.
  • the inventors have also found that the use of a polarizable electrode improves the productivity and high-temperature stability of the electrochemical device, and the present invention has been completed.
  • the present invention relates to an electrochemical element comprising at least an ionic liquid as an electrolyte and a polarizable electrode, wherein the polarizable electrode is an activated carbon containing rubber, and
  • the present invention relates to a polarizable electrode characterized by containing at least rubber, an ionic liquid and activated carbon.
  • the electric double layer capacitor of the present invention includes a polarizable electrode, an electrolytic solution, a current collector, and a separator overnight as constituent elements.
  • the electric double layer capacitor of the present invention has a current collector and a separator electrode sandwiched between two polarizable electrodes impregnated with the electrolytic solution of the present invention, and impregnated with the electrolytic solution of the present invention. It is manufactured by being housed in a stainless steel outer case.
  • the configuration of a polarizable electrode is usually composed of activated carbon as an electrode active material, rubber as a binder material, and a conductive agent, and is used as a thin coating film, a sheet-like or plate-like molded body.
  • the specific surface area of the activated carbon cannot be generally stated due to the decrease in the bulk density associated with the increase in specific surface area due to the carbonaceous species, the capacitance (F / m 2 ), and the increase in the specific surface area.
  • the specific surface area determined by the BET method is preferably from 500 to 300 m 2 Z g, and in particular, the activated carbon having a specific surface area of from 10 Q to 200 m 2 Z g
  • the electrostatic capacity is large and preferable.
  • the method for producing such activated carbon is particularly limited.
  • the activation method includes a gas activation method in which the carbonized raw material is brought into contact with water vapor, carbon dioxide gas, oxygen, and other oxidizing gas at high temperature, and the carbonized raw material is mixed with zinc chloride, phosphoric acid, sodium phosphate, Calcium chloride, potassium sulfide, hydroxylating power Liu soot, sodium hydroxide, potassium carbonate, sodium carbonate, sodium sulfate soot, potassium sulfate, calcium carbonate, boric acid, nitric acid, etc. are evenly impregnated in an inert gas atmosphere.
  • a chemical activation method that heats and obtains activated carbon for dehydration and oxidation reaction of chemicals, both of which can be used.
  • the activated carbon after the activation treatment is heat-treated at 500 to 2500 ° C, preferably 700 to 1500 ° C in an inert gas atmosphere such as nitrogen, argon, helium, xenon, etc. to remove unnecessary surface functional groups.
  • carbon conductivity may be developed to increase electron conductivity.
  • the shape of the activated carbon can be used without any particular limitation, such as crushing, granulation, granule, fiber, ferrule, woven fabric, and sheet shape, but in the case of granular, the improvement of the bulk density of the electrode, the internal resistance In terms of reduction, the average particle size is preferably 30 im or less.
  • the average pore diameter is preferably 2.5 nm or less.
  • the average pore size of activated carbon is measured by the BET method with nitrogen adsorption.
  • Examples of the rubber used as a binder material of the polarizable electrode of the present invention include conjugated digens, acrylates, methacrylic compounds disclosed in, for example, JP-A No. 200-076731, JP-A No. 2005-064288, and the like.
  • a copolymer cross-linked polymer or the like derived from at least 1 layer selected from acid esters and the like is used.
  • the amount of binder contained in the polarizable electrode depends on the type and form of carbonaceous material The amount of activated carbon decreases and the capacity decreases when it is too much, but when it is too small, the binding strength is poor and the strength is lowered, so 0.5 to 30% of the weight of the activated carbon is preferable. ⁇ 30% is particularly preferred.
  • a polarizable electrode that can be impregnated with a ionic liquid in a short time can be produced. Moreover, you may mix and use a fluorine-type binder etc. as needed.
  • the conductive agent is at least selected from the group consisting of carbon black such as acetylene black and ketjen black, natural graphite, thermally expanded graphite, carbon fiber, ruthenium oxide, titanium oxide, aluminum, nickel, and the like.
  • a kind of conductive agent is preferred.
  • Acetylene black and ketjen black are particularly preferred in that the conductivity is effectively improved with a small amount.
  • the amount of activated carbon varies depending on the bulk density of the activated carbon, but if the amount is too large, the proportion of activated carbon decreases and the capacity decreases. Therefore, ⁇ 50% of the weight of the activated carbon is preferable, especially 3 to 30%.
  • the polarizable electrode can be formed by a conventionally known method, for example, by rolling, extruding, coating, or the like. Specifically, for example, it is obtained by adding rubber to a mixture of activated carbon and a conductive agent and then press-molding. In addition, activated carbon and rubber are mixed and molded, and then heat-treated in an inert atmosphere to obtain a sintered body. Furthermore, it is also possible to sinter activated carbon and rubber into an electrode.
  • the film thickness of the shaped polarizable electrode is usually preferably about 80 to 3000 m.
  • an electrolytic solution containing an ionic liquid as a main component is used.
  • an ionic liquid a known one can be used and is not particularly limited.
  • Q + represents a quaternary ammonium cation, A— (mabis (Rifrutal Lomethanesulfonyl) imidazole ion [N (S0 2 CF 3 ) ⁇ ]) [BF 4 -] or to Kisafuru old Rofosufue one Bok ion [PF 6 -].. represented will leave quaternary salt (hereinafter ,, ⁇ (1) in which are shown)) can be mentioned.
  • Examples of the quaternary ammonium cation represented by Q + include formula (2):
  • R 1 to R 4 may be the same or different from each other, and each represents an optionally substituted alkyl group.
  • Aliphatic ammonium cation (2) formula (3):
  • Q 1 represents an optionally substituted nitrogen-containing aliphatic cyclic group.
  • R 1 and R 2 are the same as above.
  • An alicyclic ammonium cation hereinafter referred to as alicyclic
  • Q 2 represents an optionally substituted nitrogen-containing heteroaromatic ring group.
  • R 1 is the same as described above.
  • alkyl group which may be substituted include, for example, methyl group, ethyl group, propyl group, isopropyl group, butyl group, isobutyl group, sec-butyl group, tert-butyl group, pentyl group, pentyl group, neopentyl group, and A linear, branched or cyclic unsubstituted alkyl group having 1 to 18 carbon atoms, such as a xyl group, an isohexyl group, a decyl group, a dodecyl group, a tectadecyl group, a cyclopentyl group, and a cyclohexyl group;
  • one or two or more hydrogen atoms constituting such an unsubstituted alkyl group are, for example, an aryl group such as a phenyl group, a disubstituted amino group such as a dimethylamino group
  • Examples of the optionally substituted nitrogen-containing aliphatic cyclic group include pyrrolidyl group, 2-methylpyrrolidyl group, 3-methylpyrrolidyl group, 2-ethylpyrrolidyl group, 3-ethylpyrrolidyl group, 2,2-dimethylpyrrolidyl group.
  • nitrogen-containing heteroaromatic group examples include pyridyl group, 2-methylpyridyl group, 3-methylpyridyl group, 4-methylpyridyl group, 2,6-dimethylpyridyl group, 2-methyl- 6-Ethylpyridyl group, 1-methylimidazolyl group, 1,2-dimethylimidazolyl group, 1-ethylimidazolyl group, 1-propylimidazolyl group, 1-pentylimidazolyl group, 1-pentylimidazolyl group, 1-hexylimidazolyl group Groups and the like.
  • Examples of the aliphatic ammonium cation (2) include tetrapentylmonium cation, tetrahexylammonium cation, trimethylpolypyrammonium cation, tert-butyl triethylammonium cation, benzyltrimethyl.
  • Ammonium cation benzyl triethyl moncation, dimethyl (2-methichetil) Ammon cation, dimethylethyl (2-methichetil) Ammon cation, methyl methyl (2-methichetil) ammonium cation , Limethyl [2-(2-Methyloxy) ethyl] Ammonium Cation, Dimethylethyl [2— (2-Mexoxy) Ethyl] Ammonium Cation, Jetylmethyl [2— (2-Methoxyoxy) ) Echiru] Ammonyu Kachi ON, diallylmethylhexyl ammonium cation, diallyl-methyl-octyl-monoxide-cation, and the like.
  • Examples of the alicyclic ammonium cation (3) include 1,1-dimethylpyrrolidinium cation, 1,1-jetylpyrrolidinium cation, 1-ethyl-1-methylpyrrolidinium cation, 1-propyl monocation.
  • Nitrogen-containing heteroaromatic ammonium cations (4) include, for example, 1-methylpyridinium cation, 1-ethylpyridinium cation, 1,2-dimethylpyridinium cation, 1,3-dimethylpyridinium cation, 1, 4-dimethylpyridinium cation, ⁇ , 2, 6-trimethylpyridini Cations, 1—propylpyridinium cations, 1-pentylpyridinium cations, 1—pentylpyridinium cations, 1-hexylpyridinium cations, 1,3-dimethylimidazolium cations, 1, 3 —Jetyl imidazolium cation, 1-ethyl 3-methyl imidazolium cation, 1 —Butyl 3-methyl imidazolium cation, 1-hexyl 3—Methyl imidazolium cation, 1-year-old kutiru 3—Methyl imida
  • Quaternary salts (1) include, for example, 1-ptyl-1-methylpyrrolidinium
  • Moisture contained in the ionic liquid causes a decrease in the withstand voltage of the electric double layer capacitor, so the water content is usually 1% or less, preferably 100 ppm or less, more preferably 500 ppm. Below, particularly below 100 ppm.
  • the electrolytic solution used in the present invention usually does not contain a solvent, but if necessary, an organic solvent such as propylene carbonate or acetonitrile may be added. However, as described above, when these addition amounts are large, it is disadvantageous to the safety and stability of the electric double layer capacitor. In addition, an additive such as a surfactant may be added.
  • the material of the separator used for the capacitor element of the present invention paper, polypropylene, polyethylene, glass fiber, etc. are used.
  • the shape of the electric double layer capacitor may be any shape such as a coin shape, a winding shape, a square shape, and an aluminum laminar shape, and is not limited to these shapes.
  • the current collector is preferably a material with excellent conductivity and electrochemical durability, such as valve metals such as aluminum and titanium, stainless steel, precious metals such as gold and platinum, carbon materials such as graphite, Examples include conductive rubber mixed with conductive material.
  • Aluminum wire is preferred because it is particularly lightweight, excellent in electrical conductivity, and electrochemically stable.
  • the activated carbon and the molding method of the positive electrode and the negative electrode may be the same or different, and any material may be used as long as the negative electrode and the positive electrode have the same specific surface area.
  • coconut shell activated carbon with a specific surface area of 1 50 O m 2 Z g, carbon black, CMC and BM—400 B (manufactured by Nippon Zensain Co., Ltd .; butadiene rubber-based binder) in a weight ratio of 8 6 Ethanol was added to the mixture weighed so as to have a ratio of 9: 1: 4, kneaded, molded into a sheet and dried to obtain a 2 mm thick polarizable electrode sheet.
  • This polarizable electrode sheet was joined to one side of a current collector made of electrolytically etched aluminum foil (2), and then pressed and heat-treated to obtain a polarizable electrode having a current collector.
  • the polarizable electrode having a current collector obtained as described above was bent 10 times along a stainless rod shape having a diameter of 2 mm, and a test for determining the adhesive strength between the current collector and the polarizable electrode was performed. The results are shown in Table 2. 10 Bending R test, ⁇ indicates no peeling or cracking, ⁇ is 1-2 occurrences, X is 3 or more occurrences.
  • a tape peeling test was conducted by attaching 3 cm of a 10 mm wide scotch to the surface of the polarizable electrode having the current collector obtained as described above. The results are shown in Table 2. ⁇ indicates no peeling, X indicates cracking or partial peeling.
  • Example 1 The binder and the ionic liquid in Example 1 were replaced as shown in Table 1, and the ionic liquid was replaced with a fluorosurfactant (produced by Daikin Industries, Ltd.) or propylene force one pone cake (PC). The same procedure as in Example 1 was performed except that the amount shown in Table 1 was added to the ionic liquid. The results are shown in Table 2. Table 1
  • Binder AD 1 8 1: Acrylic rubber binder (manufactured by Nippon Zeon Co., Ltd.)
  • Ionic liquid B 1, 1 —Dimethyl-1-ethyl-1-ethyl [2— (2-Methyl Shechoxy) -ethyl]
  • Ammonium Full-fledged Robola (viscosity 22 5 m Pa ⁇ s 25 ° C) Table 2
  • the polarizable electrode which can be impregnated with the ionic liquid which is electrolyte solution in a short time can be provided.
  • a polarizable electrode since such a polarizable electrode is used, it is possible to provide an electrochemical device that is impregnated with an ionic liquid in a short time, further reduces leakage of the ionic liquid at high temperatures, and has improved productivity and high-temperature stability. .

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  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)

Abstract

Dispositif électrochimique comportant au moins un liquide ionique utilisé comme solution d'électrolyte et une électrode polarisable. Ce dispositif électrochimique est caractérisé en ce que l'électrode polarisable se compose d'un charbon actif contenant un caoutchouc. En outre, l'invention concerne une électrode polarisable qui est caractérisée en ce qu'elle contient au moins un caoutchouc, un liquide ionique et un charbon actif.
PCT/JP2006/315451 2005-07-29 2006-07-28 Dispositif electrochimique WO2007013693A2 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
KR1020087002258A KR101332081B1 (ko) 2005-07-29 2006-07-28 전기 화학 소자

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2005219841 2005-07-29
JP2005-219841 2005-07-29

Publications (2)

Publication Number Publication Date
WO2007013693A2 true WO2007013693A2 (fr) 2007-02-01
WO2007013693A3 WO2007013693A3 (fr) 2007-04-19

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JP (1) JP2007059899A (fr)
KR (1) KR101332081B1 (fr)
CN (1) CN101228602A (fr)
WO (1) WO2007013693A2 (fr)

Cited By (1)

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WO2013073526A1 (fr) * 2011-11-14 2013-05-23 住友電気工業株式会社 Electrode pour dispositifs de stockage d'électricité, dispositif de stockage d'électricité et procédé de production d'électrode pour dispositifs de stockage d'électricité

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WO2008120439A1 (fr) * 2007-03-28 2008-10-09 Sanyo Chemical Industries, Ltd. Electrolyte, et solution électrolytique ou élément électrochimique le comprenant
JP5063172B2 (ja) * 2007-04-18 2012-10-31 大塚化学株式会社 電気二重層キャパシタ用電解液
JP5173460B2 (ja) * 2008-02-01 2013-04-03 太陽誘電株式会社 電気化学デバイス及びその製造方法
WO2009101806A1 (fr) * 2008-02-13 2009-08-20 Panasonic Corporation Condensateur à double couche électrique et son procédé de fabrication
CN102760578B (zh) * 2011-04-27 2016-05-18 海洋王照明科技股份有限公司 一种电容器电解液以及使用该电解液的电容器
CN102760576B (zh) * 2011-04-27 2015-09-23 海洋王照明科技股份有限公司 一种双电层电容器电解液以及使用该电解液的双电层电容器
CN102956361A (zh) * 2011-08-17 2013-03-06 海洋王照明科技股份有限公司 电解液以及双电层电容器
CN102956363A (zh) * 2011-08-17 2013-03-06 海洋王照明科技股份有限公司 一种电解液以及双电层电容器
US20130052525A1 (en) * 2011-08-24 2013-02-28 Sumitomo Chemical Company, Limited Sodium secondary battery
WO2013029236A1 (fr) * 2011-08-30 2013-03-07 海洋王照明科技股份有限公司 Liquide ionique au sel d'ammonium quaternaire à double centre, procédé de préparation de ce dernier et utilisation correspondante
JPWO2017090553A1 (ja) * 2015-11-27 2018-09-13 積水化学工業株式会社 キャパシタ用電極材及びキャパシタ

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2013073526A1 (fr) * 2011-11-14 2013-05-23 住友電気工業株式会社 Electrode pour dispositifs de stockage d'électricité, dispositif de stockage d'électricité et procédé de production d'électrode pour dispositifs de stockage d'électricité
JPWO2013073526A1 (ja) * 2011-11-14 2015-04-02 住友電気工業株式会社 蓄電デバイス用電極、蓄電デバイスおよび蓄電デバイス用電極の製造方法
US9048025B2 (en) 2011-11-14 2015-06-02 Sumitomo Electric Industries, Ltd. Electrode for electric storage device, electric storage device and manufacturing method of electrode for electric storage device

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CN101228602A (zh) 2008-07-23
WO2007013693A3 (fr) 2007-04-19
JP2007059899A (ja) 2007-03-08
KR101332081B1 (ko) 2013-11-22
KR20080031911A (ko) 2008-04-11

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