WO2009098977A1 - 電解質および電池 - Google Patents
電解質および電池 Download PDFInfo
- Publication number
- WO2009098977A1 WO2009098977A1 PCT/JP2009/051315 JP2009051315W WO2009098977A1 WO 2009098977 A1 WO2009098977 A1 WO 2009098977A1 JP 2009051315 W JP2009051315 W JP 2009051315W WO 2009098977 A1 WO2009098977 A1 WO 2009098977A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- electrolyte
- lithium
- negative electrode
- battery
- carbon
- Prior art date
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 83
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 59
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 36
- XMWRBQBLMFGWIX-UHFFFAOYSA-N C60 fullerene Chemical class C12=C3C(C4=C56)=C7C8=C5C5=C9C%10=C6C6=C4C1=C1C4=C6C6=C%10C%10=C9C9=C%11C5=C8C5=C8C7=C3C3=C7C2=C1C1=C2C4=C6C4=C%10C6=C9C9=C%11C5=C5C8=C3C3=C7C1=C1C2=C4C6=C2C9=C5C3=C12 XMWRBQBLMFGWIX-UHFFFAOYSA-N 0.000 claims abstract description 33
- 229910003472 fullerene Inorganic materials 0.000 claims abstract description 30
- 150000003839 salts Chemical class 0.000 claims abstract description 26
- 239000007784 solid electrolyte Substances 0.000 claims abstract description 25
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 9
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 9
- -1 alkali metal salt Chemical class 0.000 claims description 33
- 239000002041 carbon nanotube Substances 0.000 claims description 11
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 11
- 229910021389 graphene Inorganic materials 0.000 claims description 10
- 229910052783 alkali metal Inorganic materials 0.000 claims description 9
- 150000004678 hydrides Chemical class 0.000 claims description 7
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 6
- 230000007547 defect Effects 0.000 claims description 6
- XAEFZNCEHLXOMS-UHFFFAOYSA-M potassium benzoate Chemical compound [K+].[O-]C(=O)C1=CC=CC=C1 XAEFZNCEHLXOMS-UHFFFAOYSA-M 0.000 claims description 3
- 159000000000 sodium salts Chemical class 0.000 claims description 3
- 239000007773 negative electrode material Substances 0.000 abstract description 29
- 150000001875 compounds Chemical class 0.000 abstract description 26
- 229920000642 polymer Polymers 0.000 abstract description 17
- 229920003171 Poly (ethylene oxide) Polymers 0.000 abstract description 9
- 239000007774 positive electrode material Substances 0.000 abstract description 9
- 229910052744 lithium Inorganic materials 0.000 description 42
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 40
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 24
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 23
- 238000000034 method Methods 0.000 description 23
- 239000000470 constituent Substances 0.000 description 20
- 239000011135 tin Substances 0.000 description 19
- 239000000463 material Substances 0.000 description 18
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 17
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 description 17
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- 230000000052 comparative effect Effects 0.000 description 8
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- 239000000126 substance Substances 0.000 description 7
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- VZSRBBMJRBPUNF-UHFFFAOYSA-N 2-(2,3-dihydro-1H-inden-2-ylamino)-N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]pyrimidine-5-carboxamide Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C(=O)NCCC(N1CC2=C(CC1)NN=N2)=O VZSRBBMJRBPUNF-UHFFFAOYSA-N 0.000 description 5
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- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 3
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- FUJCRWPEOMXPAD-UHFFFAOYSA-N lithium oxide Chemical compound [Li+].[Li+].[O-2] FUJCRWPEOMXPAD-UHFFFAOYSA-N 0.000 description 1
- 229910001947 lithium oxide Inorganic materials 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- ACFSQHQYDZIPRL-UHFFFAOYSA-N lithium;bis(1,1,2,2,2-pentafluoroethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)C(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)C(F)(F)F ACFSQHQYDZIPRL-UHFFFAOYSA-N 0.000 description 1
- QVXQYMZVJNYDNG-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)methylsulfonyl-trifluoromethane Chemical compound [Li+].FC(F)(F)S(=O)(=O)[C-](S(=O)(=O)C(F)(F)F)S(=O)(=O)C(F)(F)F QVXQYMZVJNYDNG-UHFFFAOYSA-N 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- CWQXQMHSOZUFJS-UHFFFAOYSA-N molybdenum disulfide Chemical compound S=[Mo]=S CWQXQMHSOZUFJS-UHFFFAOYSA-N 0.000 description 1
- 229910000476 molybdenum oxide Inorganic materials 0.000 description 1
- 239000000178 monomer Substances 0.000 description 1
- 239000004570 mortar (masonry) Substances 0.000 description 1
- 239000011331 needle coke Substances 0.000 description 1
- 229910021470 non-graphitizable carbon Inorganic materials 0.000 description 1
- 125000005151 nonafluorobutanesulfonyl group Chemical group FC(C(C(S(=O)(=O)*)(F)F)(F)F)(C(F)(F)F)F 0.000 description 1
- 239000003921 oil Substances 0.000 description 1
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
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- 230000000737 periodic effect Effects 0.000 description 1
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- 239000005011 phenolic resin Substances 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-N phosphoric acid Substances OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 1
- 238000005289 physical deposition Methods 0.000 description 1
- 239000006253 pitch coke Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 229920001197 polyacetylene Polymers 0.000 description 1
- 229920000570 polyether Polymers 0.000 description 1
- 239000002861 polymer material Substances 0.000 description 1
- 229920000128 polypyrrole Polymers 0.000 description 1
- 229920000123 polythiophene Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 239000002296 pyrolytic carbon Substances 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
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- 239000005060 rubber Substances 0.000 description 1
- 229910001925 ruthenium oxide Inorganic materials 0.000 description 1
- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(iv) oxide Chemical compound O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 description 1
- VSZWPYCFIRKVQL-UHFFFAOYSA-N selanylidenegallium;selenium Chemical compound [Se].[Se]=[Ga].[Se]=[Ga] VSZWPYCFIRKVQL-UHFFFAOYSA-N 0.000 description 1
- 150000003377 silicon compounds Chemical class 0.000 description 1
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- 239000007790 solid phase Substances 0.000 description 1
- 239000006104 solid solution Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 239000004071 soot Substances 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 230000001629 suppression Effects 0.000 description 1
- 229920003051 synthetic elastomer Polymers 0.000 description 1
- 239000005061 synthetic rubber Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 1
- 238000002230 thermal chemical vapour deposition Methods 0.000 description 1
- 238000007751 thermal spraying Methods 0.000 description 1
- 150000003606 tin compounds Chemical class 0.000 description 1
- CFJRPNFOLVDFMJ-UHFFFAOYSA-N titanium disulfide Chemical compound S=[Ti]=S CFJRPNFOLVDFMJ-UHFFFAOYSA-N 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 230000002463 transducing effect Effects 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 238000007740 vapor deposition Methods 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 239000013585 weight reducing agent Substances 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
Images
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
- H01B1/06—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of other non-metallic substances
- H01B1/12—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of other non-metallic substances organic substances
- H01B1/122—Ionic conductors
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0562—Solid materials
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0088—Composites
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
- H01M50/109—Primary casings; Jackets or wrappings characterised by their shape or physical structure of button or coin shape
-
- 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
Definitions
- the present invention relates to an electrolyte containing an electrolyte salt and a battery using the same.
- a liquid electrolyte in which a lithium salt as an electrolyte salt is dissolved in a carbonate ester solvent is widely used.
- the electrolytic solution may leak, which may damage peripheral electronic components.
- a solid electrolyte instead of the electrolytic solution.
- the solid electrolyte include inorganic type and organic type.
- an organic type is used. The solid electrolyte has attracted attention.
- an electrolyte composed of a polymer compound and an electrolyte salt is widely known.
- Research on solid electrolytes using polyether compounds typified by polyethylene oxide as the polymer compound is actively conducted.
- Perfluorosulfonic acid resin is widely used as an electrolyte membrane having proton conductivity for use in fuel cells.
- technologies using carbon clusters such as fullerenes and carbon nanotubes having proton-dissociable groups, A technique using a polymer compound in which carbon clusters having dissociative functional groups are linked to each other via a linking group is known (for example, see Patent Documents 1 and 2).
- the above-described carbon cluster has been studied for a technique for using it as a material for a negative electrode active material or an additive for an electrolytic solution in a secondary battery (see, for example, Patent Documents 3 and 4).
- the lithium ion dissociated in the polymer compound moves due to the segment motion of the polymer chain, thereby having ion conductivity. Therefore, at low temperatures, the segment motion tends to decrease and the ionic conductivity tends to decrease significantly. For this reason, it has been difficult to maintain good battery characteristics over a wide temperature range.
- the present invention has been made in view of such problems, and an object thereof is to provide an electrolyte capable of ensuring good ionic conductivity at a low temperature and a battery using the same.
- the electrolyte of the present invention is a solid electrolyte and includes a carbon cluster and an electrolyte salt containing at least one of an alkali metal salt and an alkaline earth metal salt.
- the battery of the present invention is a battery including a positive electrode and a negative electrode and a solid electrolyte, and the solid electrolyte includes a carbon cluster and an electrolyte salt containing at least one of an alkali metal salt and an alkaline earth metal salt. It is a waste.
- the carbon cluster is included, good ionic conductivity can be ensured even at a low temperature even with a solid electrolyte.
- a decrease in the ionic conductivity of the electrolyte at a low temperature is suppressed, so that favorable battery characteristics can be maintained.
- FIG. 6 is a diagram showing temperature characteristics of ionic conductivity in electrolytes (Examples 1-1 to 1-4, Comparative Example 1). It is a figure showing the temperature characteristic of the ionic conductivity in another electrolyte (Examples 2-1 and 2-2, comparative example 1).
- An electrolyte according to an embodiment of the present invention is a solid electrolyte used for an electrochemical device such as a battery, and includes carbon clusters and an electrolyte salt.
- the “carbon cluster” refers to a material in which carbon is a main element and tens to hundreds of atoms are bonded, or a material formed by the bonding is agglomerated or crystallized.
- This electrolyte contains carbon clusters because it can maintain good ionic conductivity at low temperatures, unlike polymers containing polyethylene oxide or ethylene oxide in which cations are moved by segment movement of polymer chains. is there.
- Examples of the carbon cluster include a spherical structure, a bowl-shaped structure, a planar structure, and a cylindrical structure. They may be used alone or in combination of two or more. Moreover, those single crystals may be sufficient and a polycrystal may be sufficient.
- Examples of the spherical structure include fullerene or a derivative thereof.
- guide_body is what was formed by introduce
- guide_body means the same also in the below-mentioned.
- Examples of fullerenes include C 36 , C 60 , C 70 , C 76 , C 78 , C 80 , C 82 , C 84 , C 86 , C 88 , C 90 , C 92 , C 94 or C 96. It is done.
- Examples of fullerene derivatives include oxides and hydrides of fullerenes described above. Among them, C 60 fullerene or an oxide thereof is preferable. This is because it can be obtained relatively easily and good ionic conductivity can be secured at a low temperature.
- bowl-shaped structures include spherical structure defects. Specifically, a deficiency of the above-mentioned fullerene or a derivative thereof can be mentioned. This “deficiency” is, for example, an open structure due to a deficiency of some atoms of a spherical structure, such as a by-product when a so-called soot structure is generated. That is. In addition, what this deficient means is the same also in the below-mentioned.
- planar structure examples include graphene, a derivative thereof, or a defect thereof.
- planar structure examples include graphene, a derivative thereof, or a defect thereof.
- deletions are mentioned, for example.
- This carbon cluster is composed of fullerene, carbon nanotube, graphene, fullerene hydride, carbon nanotube hydride, graphene hydride, fullerene oxide, carbon nanotube oxide, and graphene oxide, and their defects. It is preferably at least one member of the group consisting of This is because a high effect can be obtained.
- the electrolyte salt has, for example, a battery electrode reactant as a cation, and includes at least one of an alkali metal salt and an alkaline earth metal salt.
- alkali metal salt include lithium salt, sodium salt and potassium salt.
- Specific examples of the lithium salt include lithium hexafluorophosphate (LiPF 6 ), lithium tetrafluoroborate (LiBF 4 ), perchlorine.
- the ratio (molar ratio) M1 / M2 between the number of moles of carbon clusters (M1) and the number of moles of electrolyte salt (M2) in this electrolyte is arbitrary, but within a range of 1/4 or more and 4/1 or less. Preferably there is. This is because a high effect can be obtained.
- this electrolyte for example, it is preferable to produce it by mixing a predetermined amount of carbon clusters and an electrolyte salt while pulverizing them in a solid phase. This is because the above-described electrolyte can be easily manufactured.
- the electrolyte in the present embodiment is a solid electrolyte, and includes a carbon cluster and an electrolyte salt containing at least one of an alkali metal salt and an alkaline earth metal salt.
- the ionic conductivity is good over a wide temperature range, with no rapid decrease in ionic conductivity due to suppression of segmental motion of polymer chains at low temperatures Maintained.
- the electrolyte may be a powdery mixture containing carbon clusters and an electrolyte salt, or may be a solidified powdery mixture.
- the carbon cluster is included, even if it is a solid electrolyte, good ionic conductivity can be secured at a low temperature. Therefore, when this electrolyte is used in an electrochemical device such as a battery, it can contribute to maintaining good battery characteristics at low temperatures.
- the carbon cluster is fullerene, carbon nanotube, graphene, hydride of fullerene, hydride of carbon nanotube, hydride of graphene, fullerene oxide, oxide of carbon nanotube, oxide of graphene, and defects thereof If the electrolyte salt is at least one member selected from the group consisting of lithium salt, sodium salt and potassium salt, a high effect can be obtained.
- the electrolyte is used as follows.
- FIG. 1 shows a cross-sectional configuration of the first battery.
- This battery is, for example, a lithium ion secondary battery in which the capacity of the negative electrode is represented by the capacity based on insertion and extraction of lithium which is a battery reactant.
- This secondary battery is obtained by laminating a positive electrode 14 accommodated in an outer can 11 and a negative electrode 15 accommodated in an outer cup 12 via an electrolyte 16.
- the battery structure using the outer can 11 and the outer cup 12 is called a so-called coin type.
- the peripheral edges of the outer can 11 and the outer cup 12 are sealed by caulking through a gasket 13.
- the outer can 11 has a shallow dish shape that accommodates the positive electrode 14, a so-called petri dish shape, and serves as an external positive electrode of the secondary battery.
- the outer can 11 is made of, for example, stainless steel, aluminum (Al), or a metal having a structure in which aluminum, stainless steel, and nickel (Ni) are sequentially stacked in the thickness direction from the side of the accommodated positive electrode 14.
- the exterior cup 12 is a petri dish-like container that houses the negative electrode 15 and serves as an external negative electrode for the secondary battery.
- the exterior cup 12 is made of, for example, a metal such as stainless steel, aluminum, or iron (Fe) whose surface is nickel-plated.
- the gasket 13 is made of, for example, an insulating material.
- the positive electrode 14 is, for example, one in which a positive electrode active material layer 14B is provided on one surface of a positive electrode current collector 14A having a pair of opposed surfaces.
- the positive electrode current collector 14A is made of a metal material such as aluminum, nickel, or stainless steel.
- the positive electrode active material layer 14B includes, for example, one or more positive electrode materials capable of inserting and extracting lithium as an electrode reactant as a positive electrode active material.
- the positive electrode active material layer 14B may contain a conductive agent, a binder, or the like as necessary.
- positive electrode materials capable of inserting and extracting lithium include iron sulfide (FeS 2 ), titanium sulfide (TiS 2 ), molybdenum sulfide (MoS 2 ), niobium selenide (NbSe 2 ), and vanadium oxide (V Examples thereof include chalcogenides containing no lithium such as 2 O 5 ) or lithium-containing compounds containing lithium.
- lithium-containing compounds are preferable because some compounds can obtain a high voltage and a high energy density.
- a lithium-containing compound include a composite oxide containing lithium and a transition metal element, or a phosphoric acid compound containing lithium and a transition metal element.
- the group consisting of cobalt, nickel, manganese, and iron Those containing at least one of them are preferred. This is because a higher voltage can be obtained.
- the chemical formula is represented by, for example, Li x MIO 2 or Li y MIIPO 4 . In the formula, MI and MII represent one or more transition metal elements.
- the values of x and y vary depending on the charge / discharge state of the battery, and are generally 0.05 ⁇ x ⁇ 1.10 and 0.05 ⁇ y ⁇ 1.10.
- the composite oxide containing lithium and a transition metal element include lithium cobalt composite oxide (Li x CoO 2 ), lithium nickel composite oxide (Li x NiO 2 ), and lithium nickel cobalt composite oxide (Li x Ni 1-z Co z O 2 (z ⁇ 1)), lithium nickel cobalt manganese composite oxide (Li x Ni (1-vw) Co v Mn w O 2 (v + w ⁇ 1)), or a spinel structure Examples thereof include lithium manganese composite oxide (LiMn 2 O 4 ).
- a composite oxide containing nickel is preferable. This is because a high capacity can be obtained and excellent cycle characteristics can be obtained.
- the phosphate compound containing lithium and a transition metal element include, for example, a lithium iron phosphate compound (LiFePO 4 ) or a lithium iron manganese phosphate compound (LiFe 1-u Mn u PO 4 (u ⁇ 1)). Etc.
- examples of the positive electrode material include oxides such as titanium oxide, vanadium oxide, and manganese dioxide, and conductive polymers such as sulfur, polyaniline, and polythiophene.
- the negative electrode 15 is, for example, one in which a negative electrode active material layer 15B is provided on one surface of a negative electrode current collector 15A having a pair of opposed surfaces.
- the negative electrode current collector 15A is preferably made of a metal material having good electrochemical stability, electrical conductivity, and mechanical strength. Examples of the metal material include copper (Cu), nickel, and stainless steel. Among these, copper is preferable as the metal material. This is because high electrical conductivity can be obtained.
- the metal material constituting the negative electrode current collector 15A a material containing one or more metal elements that do not form an intermetallic compound with lithium is preferable.
- an intermetallic compound is formed with lithium, it is damaged by the influence of stress due to expansion and contraction of the negative electrode current collector 15A during charge / discharge, so that the current collecting property is reduced, or the negative electrode active material layer 15B is peeled off. It is easy to do.
- the metal element include copper, nickel, titanium (Ti), iron, and chromium (Cr).
- the negative electrode active material layer 15B contains one or more negative electrode materials capable of inserting and extracting lithium as a negative electrode active material.
- the negative electrode active material layer 15B may contain a conductive agent or a binder as necessary. Note that the charge capacity of the negative electrode material capable of inserting and extracting lithium is preferably larger than the charge capacity of the positive electrode active material.
- Examples of the negative electrode material capable of inserting and extracting lithium include a carbon material.
- Examples of such a carbon material include graphitizable carbon, non-graphitizable carbon having a (002) plane spacing of 0.37 nm or more, or graphite having a (002) plane spacing of 0.34 nm or less.
- coke includes pitch coke, needle coke, petroleum coke, and the like, and the organic polymer compound fired body is obtained by firing and carbonizing a phenol resin, a furan resin, or the like at an appropriate temperature.
- a carbon material is preferable because it has a very small change in crystal structure due to insertion and extraction of lithium, so that a high energy density is obtained and an excellent cycle characteristic is obtained, and it also functions as a conductive agent.
- Examples of the negative electrode material capable of occluding and releasing lithium include, for example, a material capable of occluding and releasing lithium and having at least one of a metal element and a metalloid element as a constituent element. Can be mentioned. Such a negative electrode material is preferable because a high energy density is obtained.
- This negative electrode material may be a single element or an alloy or a compound of a metal element or a metalloid element, or may have at least a part of one or more of these phases.
- the alloy herein includes an alloy containing one or more metal elements and one or more metalloid elements in addition to an alloy composed of two or more metal elements. Moreover, the alloy here may contain the nonmetallic element.
- This structure includes a solid solution, a eutectic (eutectic mixture), an intermetallic compound, or a mixture of two or more of them.
- Examples of the metal element or metalloid element constituting the negative electrode material include a metal element or metalloid element capable of forming an alloy with lithium.
- a metal element or metalloid element capable of forming an alloy with lithium.
- at least one of silicon and tin is particularly preferable. This is because a high energy density can be obtained because the ability to occlude and release lithium is large.
- Examples of the material having at least one of silicon and tin include at least one selected from the group consisting of a simple substance, an alloy and a compound of silicon, and a simple substance, an alloy and a compound of tin. That is, it is a material having at least a part of a simple substance, an alloy or a compound of silicon, a simple substance, an alloy or a compound of tin, or one or more phases thereof.
- Examples of the silicon alloy include tin, nickel, copper, iron, cobalt (Co), manganese (Mn), zinc, indium, silver, titanium, germanium, bismuth and antimony (second constituent elements other than silicon).
- Examples include those containing at least one of the group consisting of Sb) and chromium.
- As an alloy of tin for example, as a second constituent element other than tin, among the group consisting of silicon, nickel, copper, iron, cobalt, manganese, zinc, indium, silver, titanium, germanium, bismuth, antimony and chromium The thing containing at least 1 sort (s) of these is mentioned.
- silicon compound or tin compound examples include those containing oxygen (O) or carbon (C), and may contain the second constituent element described above in addition to silicon or tin.
- a material having at least one of silicon and tin a material containing tin as a first constituent element and a second constituent element and a third constituent element in addition to the tin is preferable.
- the second constituent element is cobalt, iron, magnesium, titanium, vanadium (V), chromium, manganese, nickel, copper, zinc, gallium, zirconium, niobium (Nb), molybdenum (Mo), silver, indium, cerium ( Ce), hafnium, tantalum (Ta), tungsten (W), bismuth and silicon.
- the third constituent element is at least one selected from the group consisting of boron, carbon, aluminum, and phosphorus. This is because the cycle characteristics are improved by including the second and third constituent elements.
- tin, cobalt and carbon are included as constituent elements, and the carbon content is in the range of 9.9 mass% to 29.7 mass%, and the ratio of cobalt to the total of tin and cobalt (Co / (Sn + Co)) Is preferably a CoSnC-containing material in the range of 30% by mass to 70% by mass. This is because a high energy density can be obtained in such a composition range.
- This CoSnC-containing material may further contain other constituent elements as necessary.
- other constituent elements for example, silicon, iron, nickel, chromium, indium, niobium, germanium, titanium, molybdenum, aluminum, phosphorus, gallium, or bismuth are preferable, and two or more of them may be included. This is because a higher effect can be obtained.
- the CoSnC-containing material has a phase containing tin, cobalt and carbon, and the phase preferably has a low crystalline structure or an amorphous structure.
- the CoSnC-containing material it is preferable that at least a part of carbon that is a constituent element is bonded to a metal element or a metalloid element that is another constituent element. This is because tin or the like is suppressed from aggregation or crystallization.
- X-ray photoelectron spectroscopy can be mentioned.
- XPS X-ray photoelectron spectroscopy
- the peak of 1s orbit (C1s) of carbon appears at 284.5 eV in the case of graphite. .
- it is surface contamination carbon, it will appear at 284.8 eV.
- the charge density of the carbon element is high, for example, when carbon is bonded to a metal element or a metalloid element, the peak of C1s appears in a region lower than 284.5 eV.
- the peak of the synthetic wave of C1s obtained for the CoSnC-containing material appears in a region lower than 284.5 eV
- at least a part of the carbon contained in the CoSnC-containing material is a metal element or a half of other constituent elements. Combined with metal elements.
- the peak of C1s is used to correct the energy axis of the spectrum.
- the C1s peak of the surface-contaminated carbon is set to 284.8 eV, which is used as an energy standard.
- the waveform of the C1s peak is obtained as a form including the surface contamination carbon peak and the carbon peak in the CoSnC-containing material. For example, by analyzing using commercially available software, the surface contamination The carbon peak and the carbon peak in the CoSnC-containing material are separated. In the waveform analysis, the position of the main peak existing on the lowest bound energy side is used as the energy reference (284.8 eV).
- examples of the negative electrode material capable of inserting and extracting lithium include metal oxides and polymer compounds capable of inserting and extracting lithium.
- examples of the metal oxide include iron oxide, ruthenium oxide, and molybdenum oxide.
- examples of the polymer compound include polyacetylene, polyaniline, and polypyrrole.
- the conductive agent examples include carbon materials such as graphite, carbon black, and ketjen black. These may be used alone or in combination of two or more. Note that the conductive agent may be a metal material or a conductive polymer as long as it is a conductive material.
- binder examples include synthetic rubbers such as styrene butadiene rubber, fluorine rubber or ethylene propylene diene, and polymer materials such as polyvinylidene fluoride. These may be used alone or in combination of two or more.
- the electrolyte 16 is composed of the above-described electrolyte. This is because good battery characteristics can be maintained at low temperatures. Further, since the electrolyte 16 is a solid electrolyte, unlike the case of using a liquid electrolyte (electrolytic solution) or an electrolyte (gel electrolyte) in which the electrolytic solution is held in a polymer compound, liquid leakage, decomposition of the electrolyte, etc. Does not occur, and excellent safety and cycle characteristics can be obtained.
- the positive electrode 14, the electrolyte 16 and the negative electrode 15 are stacked and accommodated in the outer can 11, and the outer cup is disposed on the peripheral portion of the outer can 11 via the gasket 13. 12 is fixed by caulking. Thereby, the secondary battery shown in FIG. 1 is completed.
- lithium ions are released from the positive electrode 14 and inserted in the negative electrode 15 through the electrolyte 16.
- discharging for example, lithium ions are extracted from the negative electrode 15 and inserted into the positive electrode 14 through the electrolyte 16.
- the capacity of the negative electrode 15 is expressed by a capacity component based on insertion and extraction of lithium
- a decrease in ion conductivity at a low temperature of the electrolyte 16 is suppressed. Therefore, good battery characteristics can be maintained.
- the electrolyte 16 is a solid electrolyte, there is no liquid leakage, which is a concern when using a liquid electrolyte or an electrolyte in which an electrolytic solution is held in a polymer compound, and the electrolyte is decomposed even after repeated charge and discharge. It is suppressed. Therefore, it can contribute to the improvement of safety and cycle characteristics.
- the weight of the entire battery can be reduced as compared with the case where a liquid electrolyte or an inorganic solid electrolyte is used.
- the second battery has the same configuration, operation, and effect as the first battery except that the configuration of the negative electrode 15 is different, and is manufactured by the same procedure. Description of components common to the first battery is omitted.
- the negative electrode 15 is formed by providing a negative electrode active material layer 15B on one surface of a negative electrode current collector 15A, as in the first battery.
- the negative electrode active material layer 15B contains, for example, a material containing silicon or tin as a constituent element as a negative electrode active material. Specifically, for example, it contains a silicon simple substance, an alloy or a compound, or a tin simple substance, an alloy or a compound, and may contain two or more of them.
- This negative electrode active material layer 15B is formed by using a vapor phase method, a liquid phase method, a thermal spraying method or a firing method, or two or more of them, and the negative electrode active material layer 15B and the negative electrode current collector It is preferable that 15A is alloyed in at least a part of the interface. Specifically, the constituent elements of the negative electrode current collector 15A are diffused into the negative electrode active material layer 15B at the interface, the constituent elements of the negative electrode active material layer 15B are diffused into the negative electrode current collector 15A, or these constituent elements are It is preferable that they diffuse to each other. This is because breakage due to expansion and contraction of the negative electrode active material layer 15B due to charge / discharge can be suppressed, and electronic conductivity between the negative electrode active material layer 15B and the negative electrode current collector 15A can be improved. .
- vapor phase method for example, physical deposition method or chemical deposition method, specifically, vacuum vapor deposition method, sputtering method, ion plating method, laser ablation method, thermal chemical vapor deposition (CVD) method Or a plasma chemical vapor deposition method etc. are mentioned.
- liquid phase method a known method such as electroplating or electroless plating can be used.
- the firing method is, for example, a method in which a particulate negative electrode active material is mixed with a binder and dispersed in a solvent and then heat treated at a temperature higher than the melting point of the binder.
- a known method can also be used for the firing method, for example, an atmospheric firing method, a reactive firing method, or a hot press firing method.
- Example 1-1 to 1-3 The above-described electrolyte was produced using fullerene oxide as a carbon cluster.
- fullerene oxide was synthesized.
- 300 cm 3 of a toluene solution (1 mmol / dm 3 ) of fullerene C 60 (manufactured by Frontier Carbon; non-purple purity 99% or more) is placed in a three- neck flask equipped with a thermometer, and the three- neck flask is oil The bath was heated to 80 ° C.
- ozone gas (concentration 30 g / m 3 ) was introduced into a three- necked flask at a flow rate of 1.0 dm 3 / min, and the toluene solution was bubbled for 300 seconds to cause C 60 to oxidize. .
- the temperature of the reacted toluene solution was lowered to about 71 ° C. to 73 ° C. Subsequently, by introducing nitrogen gas into the three-necked flask for 300 seconds, the ozone gas in the three-necked flask was removed, the reaction was stopped, and the toluene solution was stirred at 80 ° C. for 30 minutes. Thereafter, by cooling to room temperature, a toluene solution containing fullerene oxide was obtained. Next, 1 dm 3 of toluene was added to this fullerene oxide-containing toluene solution, refluxed for 1 hour, and then cooled to room temperature.
- the refluxed toluene solution containing fullerene oxide was separated from insoluble components and soluble components by a polytetrafluoroethylene (PTFE) membrane filter having a pore size of 1.0 ⁇ m.
- PTFE polytetrafluoroethylene
- the insoluble component contains C 60 O x (x> 6) which is an oxidized fullerene
- the soluble component contains C 60 O x (0 ⁇ x ⁇ 6) which is an oxidized fullerene. It was.
- the insoluble matter was vacuum-dried at 80 ° C. to obtain C 60 O x (x> 6).
- LiTFSI; LiTFSI; electrolyte salt bis (trifluoromethanesulfonyl) imido lithium
- a mortar for about 10 minutes to prepare an electrolyte.
- mixing was performed so that the ratio (molar ratio) M1 / M2 of the number of moles M1 of C 60 O x (x> 6) as a carbon cluster and the number of moles M2 of LiTFSI as an electrolyte salt was 1/1. .
- Example 1-2 and 1-3 A procedure similar to that of Example 1-1 was performed except that the molar ratio M1 / M2 was changed to 1/1 (1/2) (Example 1-2) or 1/4 (Example 1-3). Passed.
- Example 1-4 A procedure similar to that of Example 1-1 was performed except that lithium hexafluoroarsenate (LiAsF 6 ) was used instead of LiTFSI as the electrolyte salt. At this time, the ratio (molar ratio) M1 / M2 between the number of moles M1 of C 60 O x (x> 6) that is a carbon cluster and the number of moles M2 of LiAsF 6 that is an electrolyte salt is 1/1. Mixed.
- LiAsF 6 lithium hexafluoroarsenate
- the electrolytes of Examples 1-1 to 1-4 and Comparative Example 1 were subjected to impedance measurement at ⁇ 20 ° C. to 80 ° C., and the temperature characteristics of ionic conductivity were examined.
- the impedance was measured, the ionic conductivity ( ⁇ ; S / cm) was measured after holding the electrolyte in the dry room for 1 hour after the temperature reached a predetermined temperature.
- the Arrhenius plot was made based on the value of the ionic conductivity at each temperature, the result shown in FIG. 2 was obtained.
- the vertical axis represents the ionic conductivity ⁇ in logarithm
- the horizontal axis represents the reciprocal T ⁇ 1 (K ⁇ 1 ) of the temperature T (absolute temperature; K).
- the solid electrolyte can ensure good ionic conductivity at low temperatures by including a fullerene derivative and a lithium salt. Therefore, it is considered that a battery including such an electrolyte can maintain good battery characteristics at low temperatures.
- Example 1-1 to 1-3 when Examples 1-1 to 1-3 are compared, the ionic conductivity increases as the ratio (molar ratio) of LiTFSI in the electrolyte increases at 50 ° C. or higher, and C 60 O x (x> 6) It was found that when the molar ratio M1 / M2 of LiTFSI to 1/2 is 1/2, a high and stable ionic conductivity can be obtained in a wide temperature range. Further, from comparison between Example 1-1 and Example 1-4, in the electrolyte containing fullerene oxide, higher ionic conductivity was obtained when LiAsF 6 was used as the electrolyte salt than when LiTFSI was used. It was suggested that
- Example 2-1 and 2-2 A procedure similar to that in Example 1-1 or Example 1-4 was performed except that C 60 as a fullerene was used in place of C 60 O x (x> 6) as a carbon cluster.
- LiTFSI (Example 2-1) or LiAsF 6 (Example 2-2) is used as the electrolyte salt, and the molar ratio M1 / M2 between the carbon cluster and the electrolyte salt in that case is 1 / 1.
- Example 2-1 and 2-2 when the temperature characteristics of the ionic conductivity were examined in the same manner as in Example 1-1, the results shown in FIG. 3 were obtained.
- FIG. 3 also shows the result of Comparative Example 1.
- the solid electrolyte can ensure good ionic conductivity at low temperature by containing fullerene and lithium salt. Therefore, it is considered that a battery including such an electrolyte can maintain good battery characteristics at low temperatures.
- Example 2-1 the higher ionic conductivity is obtained when LiAsF 6 is used as the electrolyte salt than when LiTFSI is used. It has been suggested.
- the present invention has been described with reference to the embodiments and examples, the present invention is not limited to the modes described in the above embodiments and examples, and various modifications can be made.
- the usage application of the electrolyte of the present invention is not necessarily limited to a battery, but may be an electrochemical device other than a battery.
- Other applications include, for example, capacitors.
- the lithium ion secondary battery in which the capacity of the negative electrode is represented by a capacity component based on insertion and extraction of lithium has been described as the battery of the present invention.
- the battery of the present invention is a lithium metal secondary battery in which the capacity of the negative electrode is represented by a capacity component based on the precipitation and dissolution of lithium, and the charge capacity of the negative electrode material capable of inserting and extracting lithium is the charge capacity of the positive electrode.
- the capacity of the negative electrode includes a capacity based on insertion and extraction of lithium and a capacity based on precipitation and dissolution of lithium, and also applies to secondary batteries expressed by the sum of these capacities. Is possible.
- the case of using lithium as an electrode reactant has been described as an example for the battery of the present invention.
- other long-period periodic table such as sodium (Na) or potassium (K) is used.
- Other light metals such as aluminum and group 1 elements such as magnesium or calcium (Ca) may be used.
- the negative electrode material described in the above embodiment can be used as the negative electrode active material.
- the battery of the present invention has been described by taking the case where the battery structure is a coin type as an example.
- the battery of the present invention can be a cylindrical type, a laminated film type, a square type, or a button type.
- the present invention can be similarly applied to the case of having other battery structures such as the above, and the case where the battery element has a structure such as a laminated structure or a wound structure.
- the battery of the present invention is not limited to the secondary battery, but can be similarly applied to other types of batteries such as a primary battery.
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Abstract
Description
図1は、第1の電池の断面構成を表している。この電池は、例えば、負極の容量が電池反応物質であるリチウムの吸蔵および放出に基づく容量により表されるリチウムイオン二次電池である。
第2の電池は、負極15の構成が異なる点を除き、第1の電池と同様の構成、作用および効果を有していると共に同様の手順により製造される。第1の電池と共通の構成要素については、その説明は省略する。
炭素クラスターとして酸化フラーレンを用いて上記した電解質を作製した。
モル比M1/M2を1/1に代えて、1/2(実施例1-2)あるいは1/4(実施例1-3)にしたことを除き、実施例1-1と同様の手順を経た。
電解質塩としてLiTFSIに代えて、六フッ化ヒ酸リチウム(LiAsF6 )を用いたことを除き、実施例1-1と同様の手順を経た。なお、この際、炭素クラスターであるC60Ox(x>6)のモル数M1と電解質塩であるLiAsF6 のモル数M2との比(モル比)M1/M2が1/1になるように混合した。
ポリエチレンオキサイド(PEO)とLiTFSIとからなる電解質を、PEOのモノマー単位であるエチレンオキサイド(EO)のモル数と、LiTFSIが含むリチウム(Li)のモル数との比(EO:Li)が10:1になるように作製した。この場合には、アルゴン雰囲気下のグローブボックス内において、0.5gのポリエチレンオキサイド(分子量100000;シグマアルドリッチ社製)と、0.0326gのLiTFSIとを50cm3のアセトニトリルに溶解させ、その溶液を12時間撹拌した。次に、その撹拌した溶液をPTFEからなるシャーレに入れ、アルゴン雰囲気下で風乾させたのち、80℃で真空乾燥することにより、電解質を作製した。
炭素クラスターとしてC60Ox (x>6)に代えて、フラーレンであるC60を用いたことを除き、実施例1-1あるいは実施例1-4と同様の手順を経た。この際には、電解質塩としてはLiTFSI(実施例2-1)、あるいはLiAsF6(実施例2-2)を用い、その場合の炭素クラスターと電解質塩とのモル比M1/M2はいずれも1/1とした。
Claims (4)
- 固体電解質であって、
炭素クラスターと、アルカリ金属塩およびアルカリ土類金属塩のうちの少なくとも1種を含有する電解質塩とを含む
電解質。 - 前記炭素クラスターは、フラーレン、カーボンナノチューブ、グラフェン、フラーレンの水素化物、カーボンナノチューブの水素化物、グラフェンの水素化物、フラーレンの酸化物、カーボンナノチューブの酸化物、およびグラフェンの酸化物、ならびにそれらの欠損物からなる群のうちの少なくとも1種である
請求項1記載の電解質。 - 前記電解質塩は、アルカリ金属塩を含有し、
前記アルカリ金属塩は、リチウム塩、ナトリウム塩およびカリウム塩のうちの少なくとも1種である
請求項1記載の電解質。 - 正極および負極と共に固体電解質を備えた電池であって、
前記固体電解質は、炭素クラスターと、アルカリ金属塩およびアルカリ土類金属塩のうちの少なくとも1種を含有する電解質塩とを含む
電池。
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CN2009801034750A CN101933190A (zh) | 2008-02-06 | 2009-01-28 | 电解质和电池 |
US12/865,051 US8492034B2 (en) | 2008-02-06 | 2009-01-28 | Electrolyte and battery |
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JP5446309B2 (ja) * | 2009-02-20 | 2014-03-19 | ソニー株式会社 | ゲル状電解質及びこれを用いた電池とその使用方法、並びにゲル状電解質の製造方法 |
CN103165937B (zh) * | 2011-12-17 | 2015-07-29 | 清华大学 | 固体电解质及使用该固体电解质的锂基电池 |
TWI445739B (zh) * | 2011-12-27 | 2014-07-21 | Ind Tech Res Inst | 固態電解質、鋰電池、與電化學載具結構 |
CN102426921A (zh) * | 2011-12-30 | 2012-04-25 | 北京交通大学 | 一种超级电容器及其电解液的制备方法 |
CN102891335B (zh) * | 2012-10-11 | 2014-08-13 | 同济大学 | 一种全固态纳米复合聚合物电解质的制备方法 |
US9959949B2 (en) | 2013-06-04 | 2018-05-01 | Savannah River Nuclear Solutions, Llc | Solid state electrolyte composites based on complex hydrides and metal doped fullerenes/fulleranes for batteries and electrochemical applications |
FR3033328A1 (fr) * | 2015-03-05 | 2016-09-09 | Arkema France | Composition liquide de nanocharges carbonees pour les formulations utilisees dans les batteries au plomb. |
WO2017149405A1 (en) * | 2016-03-02 | 2017-09-08 | Semiconductor Energy Laboratory Co., Ltd. | Graphene compound, method for forming graphene compound, and lithium-ion storage battery |
KR101865383B1 (ko) | 2016-06-03 | 2018-06-07 | 울산과학기술원 | 이차 전지 모듈 및 이차 전지 모듈 제조 방법 |
KR101909890B1 (ko) | 2016-09-01 | 2018-10-19 | 울산과학기술원 | 이온 함유 용액을 이용하는 이차 전지 모듈 |
CN108321391B (zh) * | 2018-01-24 | 2020-05-19 | 安徽安凯汽车股份有限公司 | 一种石墨烯基全固体金属锂电池及其工作方法 |
CN110190326B (zh) * | 2019-05-29 | 2021-08-31 | 华中科技大学 | 富勒烯衍生物作为电解液添加剂的应用及相应金属电池 |
US20210189578A1 (en) * | 2019-12-18 | 2021-06-24 | Georgia Tech Research Corporation | Systems and Methods for Concentrating Ions |
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