CN106663551B - Capacitor nonaqueous electrolytic solution and capacitor - Google Patents

Capacitor nonaqueous electrolytic solution and capacitor Download PDF

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Publication number
CN106663551B
CN106663551B CN201580034821.XA CN201580034821A CN106663551B CN 106663551 B CN106663551 B CN 106663551B CN 201580034821 A CN201580034821 A CN 201580034821A CN 106663551 B CN106663551 B CN 106663551B
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alkyl
capacitor
mono
monovalence
electrolytic solution
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CN106663551A (en
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松村菜穗
岛本秀树
涩谷厚辉
渡边裕知
矢野亨
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Adeka Corp
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Asahi Denka Kogyo KK
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    • 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
    • H01G11/64—Liquid electrolytes characterised by additives
    • 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
    • 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

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

Abstract

A kind of capacitor includes with nonaqueous electrolytic solution: by Z- (SiR1R2F)nIt is at least one kind of in the compound of expression.Wherein, R1 and R2 is any one of hydrogen atom, monovalent hydrocarbon, the oxygen-containing alkyl of monovalence, monovalence sulfur-bearing alkyl, mono-valent halogenated alkyl, mono-valent halogenated oxygen-containing alkyl and mono-valent halogenated sulfur-bearing alkyl etc. respectively, Z is any one of ehter bond, thioether bond, univalent aliphatic series alkyl and divalent aliphatic hydrocarbon, and n is 1 or 2.

Description

Capacitor nonaqueous electrolytic solution and capacitor
Technical field
The present invention relates to a kind of nonaqueous electrolytic solution for capacitor and use the capacitor of the nonaqueous electrolytic solution.
Background technique
In recent years, as power supply high density electrical storage device, the secondary cell of high voltage and high-energy density is made extensively With.As it does so, being carried out the following studies to effectively utilize high density electrical storage device: by using can be with fast charging and discharging Capacitor is as power buffer, to effectively utilize the energy.
Wherein, it is proposed that use the capacitor of big charge capacity.The capacitor of the big charge capacity is by the master as electronic equipment Power supply of power supply and circuit etc. uses, for the capacitor, it is desirable that more high performance.Therefore, it is proposed to charging voltage Towards Higher Voltage is (referring for example to patent document 1.).
Secondary cell has anode and cathode, and has nonaqueous electrolytic solution.In order to improve the peace in relation to the secondary cell The performances such as qualitative and electrical characteristic have carried out various researchs to including additive in nonaqueous electrolytic solution.
Specifically, proposing as additive: 1,3-propane sultone is (referring for example to patent document 2,3.), ethylene Base ethylene carbonate is (referring for example to patent document 4,5.), vinylene carbonate is (referring for example to patent document 6,7.) and fourth sulfonic acid Lactone is (referring for example to patent document 3.) etc..Wherein, because good vinylene carbonate, the vinylene carbonate are extensive It uses.
These additives form on the surface of cathode and are referred to as solid electrolyte film (SEI:Solid Electrolyte Interface stable film).Because the surface of cathode is coated by the film, it is considered in charge and discharge, nonaqueous electrolytic solution Reduction decomposition be suppressed.
Existing technical literature
Patent document
Patent document 1: Japanese Unexamined Patent Publication 10-321479 bulletin
Patent document 2: Japanese Unexamined Patent Application 63-102173 bulletin
Patent document 3: Japanese Unexamined Patent Publication 10-050342 bulletin
Patent document 4: Japanese Unexamined Patent Publication 4-087156 bulletin
Patent document 5: Japanese Unexamined Patent Publication 2001-006729 bulletin
Patent document 6: Japanese Unexamined Patent Publication 5-074486 bulletin
Patent document 7: Japanese Unexamined Patent Publication 8-045545 bulletin
Summary of the invention
However, being not necessarily used as capacitor nonaqueous electrolytic solution to the effective additive of non-aqueous electrolyte for secondary battery Additive it is also effective.Accordingly, with respect to the additive of capacitor nonaqueous electrolytic solution, because having to secondary cell with non-aqueous The additive of electrolyte is separately inquired into, and it requires to the effective additive of capacitor nonaqueous electrolytic solution.
Accordingly, it is desired to provide a kind of capacitor nonaqueous electrolytic solution and capacitor that can steadily obtain excellent performance Device.
In order to achieve the above object, the present inventor is made by deeply extensive research, discovery by using specific compound To include the additive in capacitor nonaqueous electrolytic solution, can solve the above problem.
The present invention is based on the studies above as a result, the capacitor of one embodiment of the present invention with nonaqueous electrolytic solution include by It is at least one kind of in the compound that following formula (1) indicates.
[chemical formula 1]
(R1 and R2 are hydrogen atom (H), monovalent hydrocarbon, the oxygen-containing alkyl of monovalence, monovalence sulfur-bearing alkyl, mono-valent halogenated hydrocarbon respectively Any one in base, mono-valent halogenated oxygen-containing alkyl, mono-valent halogenated sulfur-bearing alkyl and a variety of univalent perssads being combined into them It is a.Z is any one of ehter bond (- O-), thioether bond (- S-), univalent aliphatic series alkyl and divalent aliphatic hydrocarbon, n be 1 or 2。)
In addition, the capacitor of one embodiment of the present invention has a pair of electrodes and nonaqueous electrolytic solution, the non-aqueous solution electrolysis Liquid includes at least one kind of in above-mentioned formula (1) compound represented.
Herein, monovalent hydrocarbon be the univalent perssad being made of carbon (C) and hydrogen (H) general name (comprising aliphatic alkyl and Aromatic hydrocarbyl), it can be straight-chain, or the branched with one or more side chains can be ring-type, can also be with For the ring-type with one or more side chains.The oxygen-containing alkyl of monovalence is the group that one or more ehter bonds are imported in monovalent hydrocarbon, The ehter bond can be directed in the end of carbochain, can also be imported in a manner of dividing carbochain midway.Monovalence sulfur-bearing alkyl be The group of one or more thioether bonds is imported in monovalent hydrocarbon, which can be directed in the end of carbochain, can also be with by carbon The mode of chain midway segmentation imports.
Mono-valent halogenated alkyl is the group that at least one hydrogen atom in monovalent hydrocarbon is replaced by halogen atom.It is mono-valent halogenated Oxygen-containing alkyl is the group that at least one hydrogen atom in the oxygen-containing alkyl of monovalence is replaced by halogen atom.Mono-valent halogenated sulfur-bearing alkyl It is the group that at least one hydrogen atom in monovalence sulfur-bearing alkyl is replaced by halogen atom.
Univalent aliphatic series alkyl is the general name for the monovalence non-aromatic group being made of carbon and hydrogen, can be straight-chain, Or the branched with one or more side chains, it can be ring-type, or the ring-type with one or more side chains. Divalent aliphatic hydrocarbon is the general name for the divalent non-aromatic group being made of carbon and hydrogen, can be straight-chain, or Branched with one or more side chains can be ring-type, or the ring-type with one or more side chains.
The capacitor nonaqueous electrolytic solution and capacitor of a kind of embodiment according to the present invention, because of nonaqueous electrolytic solution packet Containing at least one kind of in formula (1) compound represented, so excellent performance can be obtained steadily.
Detailed description of the invention
Fig. 1 is to indicate the perspective view after cutting off the structure division of the capacitor of one embodiment of the present invention.
Specific embodiment
One embodiment of the present invention is described in detail according to following order below.But it is for the present invention Detailed content is not limited solely to pattern described below, can be properly changed.
1. capacitor nonaqueous electrolytic solution
1-1. fluorine silicyl (Silyl) compound
1-2. other materials
1-2-1. solvent
1-2-2. electrolyte
2. capacitor
3. effect and effect
<1. capacitor nonaqueous electrolytic solution>
Firstly, being illustrated to the composition of the capacitor nonaqueous electrolytic solution of one embodiment of the present invention.
Capacitor described herein is with nonaqueous electrolytic solution (hereinafter referred merely to as " electrolyte ".) it include for example carbon materials for having The capacitor etc. of the electrode of material.But electrolyte can be used for the capacitor for the electrode for having comprising other materials.
<1-1. fluorine silyl compound>
The electrolyte include by following formula (1) indicate compound in it is any one or more.
[chemical formula 2]
(R1 and R2 are hydrogen atom (H), monovalent hydrocarbon, the oxygen-containing alkyl of monovalence, monovalence sulfur-bearing alkyl, mono-valent halogenated hydrocarbon respectively Any one in base, mono-valent halogenated oxygen-containing alkyl, mono-valent halogenated sulfur-bearing alkyl and a variety of univalent perssads being combined into them It is a.Z is any one of ehter bond (- O-), thioether bond (- S-), univalent aliphatic series alkyl and divalent aliphatic hydrocarbon, n be 1 or 2。)
Formula (1) compound represented is compound (hereinafter referred to as " the fluorine silicyl chemical combination comprising n fluorine silicyl Object ".).Why electrolyte includes fluorine silyl compound, is because can be improved the chemical stabilization of the electrolyte in this way Property.Accordingly, because the decomposition reaction of electrolyte is suppressed, so can aid in the performance for improving capacitor.
As long as the respective type hydrogen atom of R1 and R2, monovalent hydrocarbon, the oxygen-containing alkyl of monovalence, monovalence sulfur-bearing alkyl, monovalence In halogenation alkyl, mono-valent halogenated oxygen-containing alkyl, mono-valent halogenated sulfur-bearing alkyl and a variety of univalent perssads being combined into them Any one, there is no particular limitation.Further more, R1 and R2 can be identical group, or different groups.
Monovalent hydrocarbon can be straight-chain as described above, be the general name for the univalent perssad being made of carbon and hydrogen, or Branched with one or more side chains can be ring-type, or the ring-type with one or more side chains.
The monovalent hydrocarbon can be aliphatic alkyl, be also possible to aromatic hydrocarbyl.Aliphatic alkyl is, for example, alkyl, alkene Base, alkynyl and naphthenic base etc..Aromatic hydrocarbyl is, for example, aryl etc..Further more, monovalent hydrocarbon is also possible to above-mentioned aliphatic alkyl With a variety of univalent perssads being combined into aromatic hydrocarbyl.
The specific example of alkyl be methyl, ethyl, propyl, isopropyl, butyl, amyl, isopentyl, s- amyl, t- amyl, Isobutyl group, s- butyl, t- butyl, amyl, isopentyl, t- amyl, hexyl, s- hexyl, heptyl, s- heptyl, octyl, s- octyl, 2- methyl amyl and 2- ethylhexyl etc..The specific example of alkenyl is vinyl and acrylic etc..The specific example of alkynyl is second Alkynyl etc..The specific example of naphthenic base is cyclopropyl, cyclobutyl, cyclopenta, cyclohexyl, 4- methylcyclohexyl, suberyl and ring Octyl etc..The specific example of aryl is phenyl and naphthalene etc..
A variety of groups being combined into alkyl etc. are for example: group, alkyl and the naphthenic base that alkyl and aryl are combined into The group etc. that group, alkenyl and the aryl being combined into are combined into.The specific example for the group that alkyl and aryl are combined into is to first Phenyl, xylyl, benzyl, phenethyl, 2- phenyl-propane -2- base (2-phenylpropan-2-yl group), diphenylmethyl Base, trityl group and styryl etc..The specific example for the group that alkyl and naphthenic base are combined into is cyclohexyl methyl etc..Alkene The specific example for the group that base and aryl are combined into is cinnamyl group etc..
The oxygen-containing alkyl of monovalence is as described above, be the group for importing one or more ehter bonds in monovalent hydrocarbon.The ehter bond can be with It is directed in the end to form the carbochain of monovalent hydrocarbon, can also be imported so that one or many modes is divided in carbochain midway.
The specific example of the oxygen-containing alkyl of the monovalence is as described below.If importing 1 ehter bond in methyl, first is just formed Oxygroup (- O-CH3).If in ethyl (- CH2-CH3) end import 1 ehter bond, then just formed ethyoxyl (- O-CH2- CH3).If 1 ehter bond is imported in a manner of dividing carbochain in ethyl, with regard to formation-CH2-O-CH3.If propyl (- CH2-CH2-CH3) end import 1 ehter bond, then just formed propoxyl group (- O-CH2-CH2-CH3).If to divide in propyl The mode for cutting carbochain imports 2 ehter bonds, then with regard to formation-CH2-O-CH2-O-CH3。
Monovalence sulfur-bearing alkyl is as described above, be the group for importing one or more thioether bonds in monovalent hydrocarbon.The thioether bond It can be directed in the end to form the carbochain of monovalent hydrocarbon, can also be led so that one or many modes is divided in carbochain midway Enter.
The specific example of the monovalence sulfur-bearing alkyl is as described below.If importing 1 thioether bond in methyl, just formed Sulfidomethyl (- S-CH3).If importing 1 thioether bond in the end of ethyl, sulphur ethyl (- S-CH is just formed2-CH3).If 1 thioether bond is imported in a manner of dividing carbochain in ethyl, then with regard to formation-CH2-S-CH3。
Mono-valent halogenated alkyl is as described above, be the base that one or more hydrogen atoms in monovalent hydrocarbon are replaced by halogen atom Group, the type of the halogen atom can be a kind, or a variety of.
Halogen atom be such as fluorine (F), chlorine (C1), bromine (Br) and iodine (I) in it is any one or more.
The specific example of mono-valent halogenated alkyl is: chloromethyl, trifluoromethyl, 2- fluoro ethyl, 2- chloroethyl, 2,2,2- trifluoros Ethyl, 2,2,2- trichloroethyls, 1,1,2,2- tetra- fluoro ethyl, pentafluoroethyl group, five chloroethyls, 3- fluoropropyl, 2- chloropropyl, 3- chlorine The chloro- 1- Methylethyl of propyl, 1-, 3,3,3- trifluoro propyls, 2,2,3,3- tetra- fluoropropyls, heptafluoropropyl, 2- chlorobutyl, 3- neoprene The chloro- 2- butyl of base, 4- chlorobutyl, 3-, (1- chloromethyl) propyl, chloro- 1, the 1- dimethyl ethyl of 2-, 3- chloro-2-methyl propyl, 5- Chlorine amyl, 3- chloro-2-methyl propyl, chloro- 2, the 2- dimethyl propyl of 3-, 6- chlorine hexyl, five fluorine cyclohexyl, 4- fluorine cyclohexyl first Base, 2- chlorphenyl, 3- chlorphenyl, 4- chlorphenyl, 2- fluorophenyl, 3- fluorophenyl, 4- fluorophenyl and 2,4,6- chlorphenyls etc..
Mono-valent halogenated oxygen-containing alkyl is as described above, be one or more hydrogen atoms in the oxygen-containing alkyl of monovalence by halogen atom Displaced group.Mono-valent halogenated sulfur-bearing alkyl is as described above, be one or more hydrogen atoms in monovalence sulfur-bearing alkyl by halogen original The group of son displacement.
The specific example of mono-valent halogenated oxygen-containing alkyl is perfluoromethoxy (- O-CF3) etc..The tool of mono-valent halogenated sulfur-bearing alkyl Body example is perfluor sulfidomethyl (- S-CF3) etc..
The specific example of a variety of groups being combined into monovalent hydrocarbon etc. is the oxygen-containing alkyl of monovalence and monovalence sulfur-bearing alkyl The group (- CH being combined into2-O-CH2-S-CH3) etc..
As long as any one of the type ehter bond of Z, thioether bond, univalent aliphatic series alkyl and divalent aliphatic hydrocarbon are i.e. Can, there is no particular limitation.
Univalent aliphatic series alkyl, can be with as described above, be the general name for the monovalence non-aromatic group being made of carbon and hydrogen For straight-chain, or the branched with one or more side chains can be ring-type, or have one or more sides The ring-type of chain.
The univalent aliphatic series alkyl is for example: alkyl, alkenyl, alkynyl, naphthenic base and a variety of one be combined into them Valence group etc..Further more, explanation of the specific example of univalent aliphatic series alkyl such as about above-mentioned monovalent hydrocarbon.
Divalent aliphatic hydrocarbon, can be with as described above, be the general name for the divalent non-aromatic group being made of carbon and hydrogen For straight-chain, or the branched with one or more side chains can be ring-type, or have one or more sides The ring-type of chain.
The divalent aliphatic hydrocarbon is for example: alkylidene, alkenylene, alkynylene, cycloalkylidene and a variety of knots in them The group etc. of synthesis.
The specific example of alkylidene is: methane -1,1- diyl, ethane -1,2- diyl, propane -1,3- diyl, butane -1, 4- diyl, ethane -1,1- diyl, propane -1,2- diyl, butane -1,2- diyl, butane -1,3- diyl, butane -2,3- diyl, Pentane -1,5- diyl, hexane -1,6- diyl, heptane -1,7- diyl, octane -1,8- diyl, nonane -1,9- diyl, decane -1, 10- diyl and hexamethylene-Isosorbide-5-Nitrae-diyl etc..Wherein, preferably ethane -1,2- diyl, propane -1,3- diyl and butane-Isosorbide-5-Nitrae-two Base etc..The specific example of alkenylene is ethenylidene etc..The specific example of alkynylene is ethynylene etc..Cycloalkylidene it is specific Example is cyclopropylidene, sub- cyclobutyl and cyclohexylidene etc..
As long as the value 1 or 2 of n, there is no particular limitation.The value of the n is determined according to the type of Z.Specifically, In the case that Z is univalent aliphatic series alkyl, the value of n is 1.In addition, being in ehter bond, thioether bond and divalent aliphatic hydrocarbon in Z In the case where any one, the value of n is 2.
Respectively as the carbon atom number of monovalent hydrocarbon of R1 and R2, there is no particular limitation, preferably should not be terrifically excessive, Wherein, preferably 1~20.In particular, the carbon atom number of the aromatic hydrocarbyl is excellent in the case where monovalent hydrocarbon is aromatic hydrocarbyl Select 6~20.Because can be improved dissolubility and compatibility of fluorine silyl compound etc. in this way.
As the respective carbon atom number of univalent aliphatic series alkyl and divalent aliphatic hydrocarbon of Z, there is no particular limitation, excellent Choosing should not be terrifically excessive, wherein preferably 1~8.Because can be improved the dissolubility and compatibility of fluorine silyl compound in this way Property etc..
The specific example of the fluorine silyl compound is following a series of compound (No.1~No.41) etc..But As long as fluorine silyl compound has structure shown in formula (1), it is also possible to the other chemical combination not illustrated here Object.
[chemical formula 3]
[chemical formula 4]
There is no particular limitation for the amount of fluorine silyl compound in electrolyte, and e.g. 0.005 mass %~ 10 mass %, preferably 0.02 mass of mass %~5 %, the more preferable 0.05 mass mass of %~3 %.This is because being easy hair in this way The function of above-mentioned fluorine silyl compound is waved, so higher effect can be obtained.
Further more, in the case where electrolyte includes a variety of fluorine silyl compounds, above-mentioned fluorine silyl compound Amount is the summation of the amount of various fluorine silyl compounds.
<1-2. other materials>
It in the electrolytic solution, can also be together with above-mentioned fluorine silyl compound, comprising in other materials described below It is any one or more.
<1-2-1. solvent>
Other materials be, for example, in the solvents such as organic solvent it is any one or more.
There is no particular limitation for the type of organic solvent, e.g. cyclic carbonate compound, cyclic ester compounds, sulfoxide Compound, sulphones, amide compound, linear carbonate compound, chain ether compound, cyclic ether compounds, chain esterification Close object and phosphorous organic solvent etc..
Wherein, preferably cyclic carbonate compound, cyclic ester compounds, sulfoxide compound, sulphones and amide compound Object, more preferable cyclic carbonate compound.This is because relative dielectric constant is high, so the dielectric that can be improved electrolyte is normal Number.
Alternatively, it is preferred that linear carbonate compound, chain ether compound, cyclic ether compounds and chain ester compounds, more excellent Select chain shape carbonate products.Because the viscosity of electrolyte reduces, the mobility of ion can be improved.Therefore, in capacitor In device, the electric power storages characteristic such as power density can be improved.Particularly because the viscosity of linear carbonate compound significantly reduces, institute Also can be improved the performance of electrolyte in low temperature environment.
The specific example of cyclic carbonate compound is: ethylene carbonate, 1,2- propene carbonate, 1,3- propylene carbonate Ester, 1,2- butylene, 1,3- butylene, 1,1 ,-dimethyl ethylene carbonate, fluorine ethylene carbonate and difluoro carbonic acid Vinyl acetate etc..
The specific example of cyclic ester compounds is: gamma-butyrolacton, gamma-valerolactone, γ-hexalactone, δ-caprolactone and δ-are pungent Lactone etc..
The specific example of sulfoxide compound is: dimethyl sulfoxide, diethyl sulfoxide, dipropyl sulfoxide, diphenyl sulfoxide and thiophene Deng.
The specific example of sulphones is: methyl sulfone, diethyl sulfone, dipropyl sulfone, diphenyl sulphone (DPS), sulfolane (also referred to as four Hydrogen thiophene sulfone), 3- methyl sulfolane, 3,4- dimethylsulfolane, 3,4- benzhydryl sulfolane, cyclobufene sultone, 3- methyl ring Butylene sulfone, 3- ethylcyclobuten sulfone and 3- bromomethyl cyclobufene sultone etc..Wherein, preferably sulfolane and tetramethyl sulfolane etc..
The specific example of amide compound is: N-Methyl pyrrolidone, dimethylformamide and dimethyl acetamide etc..
The specific example of linear carbonate compound is: dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), carbon Diethyl phthalate (DEC), ethyl butyl carbonate, methyl-t-butyl carbonic ester, diisopropyl carbonate and t- butyl propyl carbonate Deng.
Chain ether compound and the respective specific example of cyclic ether compounds are: dimethoxy-ethane (DME), ethyoxyl methoxy Bis- (methoxycarbonyl group oxygen) ethane of base ethane, diethoxyethane, tetrahydrofuran, dioxolanes, dioxane, 1,2-, 1,2- are bis- Bis- (ethoxycarbonyl-oxygen) propane of (ethoxycarbonyl-oxygen) ethane, 1,2-, bis- (trifluoroethyl) ethers of ethylene glycol, bis- (the trifluoro second of propylene glycol Base) ether, bis- (trifluoromethyl) ethers of ethylene glycol and bis- (trifluoroethyl) ethers of diethylene glycol etc..Wherein, preferred dioxolanes.
As chain ester compounds, preferably carbon atom number is 2~8 monoester compound and diester compound etc..Mono-esterification Closing object and the respective specific example of diester compound can enumerate: methyl formate, Ethyl formate, methyl acetate, ethyl acetate, second Propyl propionate, isobutyl acetate, butyl acetate, methyl propionate, ethyl propionate, methyl butyrate, methyl isobutyrate, trimethylace tonitric first Ester, tri-methyl ethyl acetate, methylmalonate, malonic ester, succinic acid methyl esters, ethyl succinate, 3- methoxypropionic acid first Ester, 3- methoxypropionate, ethylene glycol diacetyl, propylene glycol diacetyl etc. are: methyl formate, Ethyl formate, acetic acid first Rouge, ethyl acetate, propyl acetate, isobutyl acetate, butyl acetate, methyl propionate and ethyl propionate etc..
The specific example of phosphorous organic solvent is for example: phosphoric acid ester, phosphorous acid esters, phosphinoxides and phosphonitrile class etc.. The specific example of phosphoric acid ester is: trimethyl phosphate, triethyl phosphate and triphenyl phosphate etc..The specific example of phosphorous acid esters It is: Trimethyl phosphite, triethyl phosphite and triphenyl phosphite etc..The specific example of phosphinoxides is trimethyl oxidation Phosphine, triethyl group phosphine oxide and triphenylphosphine oxide etc..
Further more, organic solvent is also possible to other compounds other than the above.Other compounds such as acetonitrile, propionitrile, nitre The derivative etc. of methylmethane and they.
<1-2-2. electrolyte>
In addition, other materials be in electrolyte it is any one or more, the electrolyte include cation and anion.Just The type of ion can be a kind, be also possible to a variety of.Type about anion is also the same.
As long as the cation of any valence mumber of the type of cation, there is no particular limitation, e.g.: quaternary ammonium from Sub-, quaternary phosphine (Phosphonium) ion, imidazoles (Imidazolium) ion, pyridine (Pyridinium) ion, pyrroles (Pyrrolidinium) ion, piperidines (Piperidinium) ion and metal ion etc..
Quaternary ammonium ion is such as tetraalkyl ammonium ion.The specific example of the tetraalkyl ammonium ion is: tetramethyl ammonium, Ethyl-trimethyl ammonium ion, diethyldimethylammonium ion, triethyl methyl ammonium ion, tetraethyl ammonium ion and thmethylpropyl Ammonium ion etc..
Quaternary phosphine ion is such as Si Wan Ji phosphonium ion.The specific example of the Si Wan Ji phosphonium ion is: tetramethyl phosphonium ion, Tetraethylphosphonium ion, 4-butyl-phosphonium ion, methyl San Yi Ji phosphonium ion, methyl San Ding Ji phosphonium ion and dimethyl Er Yi Ji Phosphonium from Son etc..
The specific example of imidazol ion is: 1,3- methylimidazole, 1- ethyl-3-methylimidazole, 1,3- diethyl Base imidazoles, 1,2,3- tri-methylimidazoliums, 1,2,3,4- tetramethyl imidazoles, 1,3,4- trimethyl -2- ethyl imidazol(e)s, 1, 3- dimethyl -2,4- diethyl imidazolium, 1,2- dimethyl -3,4- diethyl imidazolium, 1- methyl -2,3,4- triethyl methyl Imidazoles, 1,2,3,4- tetraethyl imidazoles, 1,3- dimethyl -2- ethyl imidazol(e), 1- ethyl -2,3- methylimidazole and 1,2,3- triethyl group imidazoles etc..
The specific example of pyridinium ion is: 1- picoline, 1- ethylpyridine, 1- butyl-pyridinium, 1- methyl- 3- picoline, 1- methyl -4- picoline, 1- methyl -3,4- lutidines, 1- methyl -3,5- dimethyl pyrazole Pyridine and 1- methyl -3,4,5- trimethylpyridine etc..
The specific example of pyrrolidinium ion is: 1- dimethyl pyrrole, 1- ethyl -1- methylpyrrole, 1- diethyl pyrrole Cough up with 1- butyl -1- methylpyrrole etc..
The specific example of piperidines ion is: 1- lupetidine, 1- ethyl -1- methyl piperidine, 1- diethyl piperazine Pyridine and 1- butyl -1- methyl piperidine etc..
Metal ion is for example: alkali metal ion and alkaline-earth metal ions etc..The specific example of alkali metal ion is: lithium from Son, sodium ion and potassium ion etc..The specific example of alkaline-earth metal ions is magnesium ion and calcium ion etc..
But the type of cation is also possible to other cations other than the above.
As long as the anion of any valence mumber of the type of anion, there is no particular limitation, e.g.: BF4 -、 PF6 -、AsF6 -、SbF6 -、N(RfSO3)2 -、C(RfSO2)3 -、RfSO3 -(Rf is the fluoroalkyl that carbon atom number is 1~12), N (FSO2)2 -、F-、Cl-、Br-、I-、NO3 -、NO2 -、ClO4 -、AlCl4 -、AlF4 -、TaF6 -、NbF6 -、SiF6 -、CN-And CH3BF3 -Deng. But the type of anion is also possible to other anion other than the above.
There is no particular limitation for the amount of electrolyte in electrolyte, wherein preferred 0.5mol/dm3(=mol/l)~ 2mol/dm3.This is because can ensure the capacitor of capacitor in this way, while internal resistance can be pressed very low.In detail It says, if amount ratio 0.5mol/dm3It is few, then because the absolute magnitude of the ion in electrolyte is insufficient, it is possible that leading to electricity The decline of appearance.On the other hand, if amount ratio 2mol/dm3It is more, then because the absolute magnitude of the ion in electrolyte became It is surplus, it is possible that leading to the increase of internal resistance.
Further more, other materials be also possible in flame retardant it is any one or more.This is because imparting resistance to electrolyte Combustion property, so the electrolyte becomes nonflammable.
There is no particular limitation for the amount of flame retardant in electrolyte, wherein preferably, opposite organic solvent is 1 matter Measure the mass of %~50 %, the more preferable 3 mass mass of %~10 %.It is brought this is because can avoid in this way to the performance of electrolyte Adverse effect, while sufficient anti-flammability can be obtained.
There is no particular limitation for the type of the flame retardant, e.g. halogen system flame retardant and phosphorus system flame retardant etc..Halogen system The specific example of flame retardant is: two (2,2,2- trifluoroethyl) carbonic esters, two (2,2,3,3- tetra- fluoropropyl) carbonic esters, two (2, 2,3,3,4,4,5,5- octafluoro amyls) carbonic ester and 2,2,3,3,3- pentafluoropropyl groups -1,1,2,2- tetrafluoro ethylethers etc..Phosphorus system is anti- The specific example for firing agent is trimethyl phosphate and triethyl phosphate etc..But the type of flame retardant be also possible to it is other than the above Other flame retardant.
<2. capacitor>
Secondly, being illustrated to the structure for the capacitor for using above-mentioned electrolyte.
Fig. 1 shows the stereochemical structures of the capacitor of one embodiment of the present invention.But in Fig. 1, in order to be easy to see The internal structure for examining capacitor, the state after indicating a part excision by shell 7.
Capacitor described herein is for example winding-type double layer capacitor.The capacitor is for example in the inside of shell 7 Have: capacitor element 1 and sealing part 6.
Shell 7 is for example open with one end (opening portion) and the shape of the other end (closure) closed bottomed tube Shape is formed by aluminium etc..In the inside of shell 7, it is accommodated with capacitor element 1, and the opening portion 7 of the shell 7 is by sealing part 6 Sealing.
Capacitor element 1 is by a pair of electrodes (anode and cathode) by winding after the stacking of partition (separator) 5 At.In the capacitor element 1, it is impregnated with above-mentioned electrolyte.
The anode such as polarizable electrode layer 4 comprising: collector 3 and the surface that the collector 3 is arranged in, the collector 3 connect It is connected to lead 2.Collector 3 is, for example, aluminium foil etc..Polarizable electrode layer 4 is for example comprising that can adsorb the active material with maldi ion In (positive active material) it is any one or more, the active material is including, for example, carbon material and organic semiconductor etc..
Carbon material is for example: active carbon, carbon nanotube, graphite and graphene etc., which is such as wood powder class, coconut The material that the raw materials such as shell class, phenolic resin class, petroleum coke class, coal coke class, pitch (pitch) class are activated.It is organic partly to lead Body is such as polyacene and its derivative.
Cathode has such as same structure with above-mentioned anode.That is, cathode includes: being connected with the current collection of lead 2 Body 3 and polarizable electrode layer 4, the polarizable electrode layer 4 include the active material (negative electrode active material that can be adsorbed with maldi ion Matter).
As long as the above-mentioned carbon material of the type of active material and organic semiconductor etc., there is no particular limitation.Wherein, Preferably, one or both in positive active material and negative electrode active material includes carbon material.This is because can hold in this way Easily and steadily absorption and maldi ion, so excellent performance can be obtained.
Further more, in polarizable electrode layer 4, can also together with active material, comprising adhesive and conductive auxiliary agent etc. other In material it is any one or more.
In the capacitor, it is preferred that being inserted into partition 5 between positive electrode and negative electrode.The partition 5 is, for example, The microporous membrane etc. formed by high-molecular compound, the microporous membrane can be single layer, be also possible to multilayer (multilayer film).
Forming the type of high-molecular compound of microporous membrane, there is no particular limitation, e.g.: polyethylene, polypropylene, Polyvinylidene fluoride, polyvinylidene chloride, polyacrylonitrile, polyacrylamide, polytetrafluoroethylene (PTFE), polysulfones, polyether sulfone, poly- carbonic acid Ester, polyamide, polyimides and poly- (methyl) acrylic acid etc..In addition, high-molecular compound may is that polyethylene oxide and polycyclic The polyethers such as Ethylene Oxide, are also possible to: the cellulose families such as carboxymethyl cellulose and hydroxypropyl cellulose.In addition, macromolecule chemical combination Object can be ester of above-mentioned a succession of high-molecular compound etc. and its derivative, be also possible to above-mentioned a succession of high-molecular compound In a variety of copolymer and mixture.Wherein, preferably polyethylene, polypropylene, polyvinylidene fluoride, polysulfones and cellulose etc..
Further more, can also in high-molecular compound containing in additive it is any one or more.The type of the additive There is no particular limitation with amount.
The film of partition 5 is formed as described above, it is preferred to micro- porosity.This is because electrolyte in this way easily infiltrates into partition 5, institute It is become easy with ion through the partition 5.
By the method for the micro- porous of film, there is no particular limitation, e.g. phase separation method and pulling method etc..In phase separation method In, such as after modulating the solution comprising high-molecular compound and organic solvent etc., make the solution microphase-separated on one side, on one side Film.Then, by extracting to remove the organic solvent in film, to make the film porous.In pulling method, such as in high capacity After the lower high-molecular compound that will be dissolved is squeezed out and is film-made, which is heat-treated.Then, make the crystalline arrangement in film After a direction, the film is stretched.Accordingly, because gap is formed between the crystallization in film, so the film porous.This is micro- The method of porous can suitably be selected according to the type etc. of the film for example used as partition 5.
Sealing part 6 is, for example, rubber etc., is embedded in the opening portion of shell 7.In the manufacturing process of capacitor, by opening The side of shell 7 near oral area forms drawing portion (recess portion), between the medial surface of the shell 7 and the lateral surface of sealing part 6 Gap sealed.Further more, in order to export lead 2 from the interior of shell 7, being provided with for wearing in sealing part 6 Cross the insertion hole of the lead 2.
Further more, electrode also may include in order to improve safety: phenol antioxidant, phosphorus antioxidants, thioether class are anti- The additives such as oxidant and hindered amine compound.It can also like this include additive about partition 5 and electrolyte.
<3. effects and effect>
According to above-mentioned electrolyte and capacitor, because electrolyte includes fluorine silyl compound, as described above, It is able to suppress the decomposition reaction of electrolyte.Therefore, even if saving in the high temperature environment using capacitor or in the high temperature environment Capacitor, is also able to suppress the increase of resistance (internal resistance), and obtains high capacitance.Furthermore, it is also possible to make charging voltage height Voltage.Therefore, excellent performance can be obtained.
Further more, in the explanation about above-mentioned capacitor, it is of the invention although double layer capacitor has been illustrated Capacitor is not limited to double layer capacitor, is readily applicable to other capacitors such as mixed capacitor.In these capacitors, One or both in a pair of electrodes can preferably adsorb the electrode with maldi ion.Even in this case, it can also obtain Obtain same effect.
[embodiment]
Hereinafter, the embodiment of the present invention is described in detail according to following order.But pattern of the invention is not limited to Pattern described herein.
1. the production of capacitor
2. the evaluation of capacitor
<production of 1. capacitors>
According to the following steps, capacitor shown in FIG. 1 has been made.
(experimental example 1~6)
Initially, polarizable electrode layer 4 is formed on the surface of collector 3, obtains a pair of electrodes (anode and cathode).As collection Electric body 3 uses the aluminium foil for implementing overetch processing.In the composition of polarizable electrode layer 4, active material (active carbon) is 88 weights Measure %, adhesive (polytetrafluoroethylene (PTFE)) is 6 weight %, conductive auxiliary agent (acetylene black) is 6 weight %.Then, in each electrode Aluminum lead 2 is installed on collector 3.Then, by partition 5 make anode and cathode stacking after, wind the anode, cathode and Partition 5 forms capacitor element 1.As the partition 5, use cellulose nonwoven fabric (35 μ m-thick).
Then, after capacitor element 1 is stored in the inside of the cylindrical case of aluminum 7, electrolyte is made to impregnate the capacitor Element 1.In the case where modulating the electrolyte, make electrolyte (tetraethyl ammonium tetrafluoroborate: N (C2H5)4 +BF4 -) be dissolved in After obtaining solution in organic solvent (gamma-butyrolacton), as needed, fluorine silyl compound is added in the solution. In this case, make the amount 1mol/dm of the electrolyte in electrolyte3.The presence or absence of fluorine silyl compound, type It is as shown in table 1 with amount (weight %).Further more, the water content in electrolyte is less than or equal to 100ppm.
[table 1]
Finally, forming the shell 7, and form drawing portion after sealing part 6 is stored in the inside of shell 7.At this In the case of kind, by the insertion hole being arranged in sealing part 6, lead 2 is exported from the inside of shell 7 to outside.Because logical The forming processes are crossed, the shell 7 for being accommodated with capacitor element 1 is sealed, so capacitor has been made.
<evaluations of 2. capacitors>
According to the following steps, the performance of capacitor is had rated.
Initially, in -30 DEG C of environment, make capacitor charging/discharging.In charging, charge when with the constant current of 1.5A After so that voltage is reached 2.8V, charged state is made to keep 7 points of kinds under the constant voltage of 2.8V.In electric discharge, electricity is determined with 1.35A Stream, which carries out electric discharge, makes voltage become 0V.Then, according to above-mentioned charge and discharge electric condition etc., capacitor is calculated using following formula (2), and make Resistance (DCR) is calculated with following formula (3).In this case, the height (mm) of capacitor is determined using vernier caliper.The electricity The height of container is as shown in Figure 1, be the full-size H of the length direction of shell 7.
Capacitor=Id×t(80-40)/V(80-40)......(2)
(IdCurrent value (1.35A) when being electric discharge.t(80-40)It is voltage from the voltage (2.8V) when being equivalent to fully charged 80% value (2.8V × 0.8=2.24V) drop to be equivalent to 40% value (2.8V × 0.4=1.12V) needed for the time. V(80-40)Be it is above-mentioned be equivalent to 80% value (2.24V) and be equivalent to 40% value (1.12V) difference (2.24V-1.12V= 1.12V)。)
Resistance=Δ V/Id......(3)
(Δ V be in the start time that will discharge as 0 second, from 0.5 second~2 seconds in the range of discharge curve calculate it is primary Near linear after, acquired since the primary near linear cut square current potential Vs with discharge when current potential V0 difference (V0-Vs)。IdCurrent value (1.35A) when being above-mentioned electric discharge.)
Then, in 60 DEG C of environment, make capacitor charging/discharging.In this case, when with the constant current of 1.5A to electricity Container charge after making voltage reach 2.8V, and the capacitor of charged state is saved 1250 hours.Later, 1.35A is used Constant current to capacitor carry out electric discharge make voltage become 0V.
Then, according to the step same as the case where measuring above-mentioned capacitor, resistance and height, in -30 DEG C of environment again The secondary capacitor for determining capacitor, resistance and height.
Capacitor sustainment rate (%), resistance increment rate (%) and expansion (mm) below have been calculated from these results, and has been obtained Result shown in table 1 is arrived.
Capacitor sustainment rate (%)=(capacitor before capacitor/preservation after preservation) × 100
Resistance increment rate (%)=(resistance before resistance/preservation after preservation) × 100
The height before height-preservation after expanding (mm)=preservation
The case where electrolyte includes fluorine silyl compound under (experimental example 1~5), fluorine first is not included compared to electrolyte The case where silane-based compound (experimental example 6), do not depend on the type of fluorine silyl compound, and capacitor sustainment rate increases and Resistance increment rate and expansion are reduced.The result indicates: if in the electrolytic solution including fluorine silyl compound, because It can be improved the chemical stability of the electrolyte, so being able to suppress the decomposition reaction of electrolyte in the high temperature environment. Therefore, in the capacitor, because capacitor becomes to be not easy to reduce and resistance becomes to be not easy to increase, and become to be not easy to expand, so It can be improved durability (service life).
As can be known from these results: if the electrolyte for capacitor includes fluorine silyl compound, because of energy Durability is enough improved, so excellent performance can be obtained steadily.
Although enumerating embodiments and examples above, the present invention is described, the present invention is not limited to The pattern illustrated in embodiments and examples can make various modifications.
Further more, there is no particular limitation for the purposes of capacitor of the invention.Wherein, because such as the various systems of automobile The demanding reliability in high current condition and cold environmental conditions etc., the preferably use as capacitor of the invention One example on way.
In addition, the purposes of electrolyte of the invention is not necessarily limited to capacitor, it is also possible to other electrochemical devices.
The disclosure contains the Japanese Priority Patent Application for relating to submit on July 7th, 2014 in Japanese Patent Office Purport disclosed in JP2014-139644, entire contents include here, for reference.
It should be appreciated by those skilled in the art, although according to design requirement and other factors be likely to occur various modifications, Combination, sub-portfolio and replaceable item, but they are all contained in the range of appended claims or its equivalent.

Claims (7)

1. a kind of capacitor nonaqueous electrolytic solution comprising: by following formula (1) indicate compound in it is at least one kind of,
[chemical formula 1]
Wherein, as n=1, R1 and R2 are hydrogen atom (H), monovalent hydrocarbon, the oxygen-containing alkyl of monovalence, monovalence sulfur-bearing alkyl, one respectively In valence halogenation alkyl, mono-valent halogenated oxygen-containing alkyl, mono-valent halogenated sulfur-bearing alkyl and a variety of univalent perssads being combined into them Any one of, Z is univalent aliphatic series alkyl；As n=2, R1 and R2 are hydrogen atom (H), monovalence sulfur-bearing alkyl, monovalence respectively Any one of the oxygen-containing alkyl of halogenation, mono-valent halogenated sulfur-bearing alkyl and a variety of univalent perssads being combined into them, Z is sulphur Ehter bond (- S-).
2. capacitor nonaqueous electrolytic solution according to claim 1, wherein
The monovalent hydrocarbon is in alkyl, alkenyl, alkynyl, naphthenic base, aryl and a variety of univalent perssads being combined into them Any one of,
The mono-valent halogenated alkyl, the mono-valent halogenated oxygen-containing alkyl and the mono-valent halogenated sulfur-bearing alkyl separately include halogen original It is at least one kind of in son,
The halogen atom includes fluorine atom (F), chlorine atom (Cl), bromine atom (Br) and iodine atom (I),
The univalent aliphatic series alkyl is in alkyl, alkenyl, alkynyl, naphthenic base and a variety of univalent perssads being combined into them Any one of.
3. capacitor nonaqueous electrolytic solution according to claim 1 or 2, wherein
Carbon atom number respectively as the monovalent hydrocarbon of the R1 and R2 is 1~20,
The carbon atom number of the univalent aliphatic series alkyl as the Z is 1~8.
4. capacitor nonaqueous electrolytic solution according to claim 1 or 2, wherein using having the electrode comprising carbon material Capacitor.
5. capacitor nonaqueous electrolytic solution according to claim 3, wherein use the electricity for having the electrode comprising carbon material Container.
6. a kind of capacitor, wherein have: a pair of electrodes and nonaqueous electrolytic solution,
The nonaqueous electrolytic solution, comprising at least one kind of in the compound that is indicated by following formula (1),
[chemical formula 2]
Wherein, as n=1, R1 and R2 are hydrogen atom (H), monovalent hydrocarbon, the oxygen-containing alkyl of monovalence, monovalence sulfur-bearing alkyl, one respectively In valence halogenation alkyl, mono-valent halogenated oxygen-containing alkyl, mono-valent halogenated sulfur-bearing alkyl and a variety of univalent perssads being combined into them Any one of, Z is univalent aliphatic series alkyl；As n=2, R1 and R2 are hydrogen atom (H), monovalence sulfur-bearing alkyl, monovalence respectively Any one of the oxygen-containing alkyl of halogenation, mono-valent halogenated sulfur-bearing alkyl and a variety of univalent perssads being combined into them, Z is sulphur Ehter bond (- S-).
7. capacitor according to claim 6, wherein at least one party in the pair of electrode includes carbon material.
CN201580034821.XA 2014-07-07 2015-06-29 Capacitor nonaqueous electrolytic solution and capacitor Expired - Fee Related CN106663551B (en)

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