JP5303947B2 - 固体電解質および電池 - Google Patents
固体電解質および電池 Download PDFInfo
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- JP5303947B2 JP5303947B2 JP2008026356A JP2008026356A JP5303947B2 JP 5303947 B2 JP5303947 B2 JP 5303947B2 JP 2008026356 A JP2008026356 A JP 2008026356A JP 2008026356 A JP2008026356 A JP 2008026356A JP 5303947 B2 JP5303947 B2 JP 5303947B2
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- Prior art keywords
- lithium
- electrolyte
- salt
- carbon
- fullerene
- Prior art date
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- 239000007784 solid electrolyte Substances 0.000 title claims abstract description 31
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 82
- 239000003792 electrolyte Substances 0.000 claims abstract description 80
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 43
- 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 42
- 229910003472 fullerene Inorganic materials 0.000 claims abstract description 40
- 150000003839 salts Chemical class 0.000 claims abstract description 31
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 10
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 10
- 229910052744 lithium Inorganic materials 0.000 claims description 46
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 44
- -1 alkali metal salt Chemical class 0.000 claims description 43
- 239000002041 carbon nanotube Substances 0.000 claims description 20
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 20
- 229910021389 graphene Inorganic materials 0.000 claims description 19
- 150000004678 hydrides Chemical class 0.000 claims description 13
- 229910052783 alkali metal Inorganic materials 0.000 claims description 9
- 230000007547 defect Effects 0.000 claims description 9
- 125000001889 triflyl group Chemical group FC(F)(F)S(*)(=O)=O 0.000 claims description 8
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 6
- 239000007790 solid phase Substances 0.000 claims description 6
- 229950003332 perflubutane Drugs 0.000 claims description 4
- 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
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
- 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 claims description 2
- 125000005151 nonafluorobutanesulfonyl group Chemical group FC(C(C(S(=O)(=O)*)(F)F)(F)F)(C(F)(F)F)F 0.000 claims description 2
- 229960004065 perflutren Drugs 0.000 claims description 2
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims 2
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims 2
- 229910015013 LiAsF Inorganic materials 0.000 claims 1
- 229910013075 LiBF Inorganic materials 0.000 claims 1
- 229910013872 LiPF Inorganic materials 0.000 claims 1
- 101150058243 Lipf gene Proteins 0.000 claims 1
- 150000001875 compounds Chemical class 0.000 abstract description 26
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- 230000002349 favourable effect Effects 0.000 abstract description 2
- 239000006183 anode active material Substances 0.000 abstract 1
- 239000006182 cathode active material Substances 0.000 abstract 1
- 239000007773 negative electrode material Substances 0.000 description 29
- 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
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- 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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- 150000001721 carbon Chemical class 0.000 description 13
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 description 13
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- 239000008151 electrolyte solution Substances 0.000 description 8
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 7
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- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 5
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- 230000000694 effects Effects 0.000 description 5
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- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 5
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- 239000000374 eutectic mixture Substances 0.000 description 1
- 230000005496 eutectics Effects 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- UQSQSQZYBQSBJZ-UHFFFAOYSA-N fluorosulfonic acid Chemical compound OS(F)(=O)=O UQSQSQZYBQSBJZ-UHFFFAOYSA-N 0.000 description 1
- 239000012634 fragment Substances 0.000 description 1
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- 229910052737 gold Inorganic materials 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical group [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910021469 graphitizable carbon Inorganic materials 0.000 description 1
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- 239000003273 ketjen black Substances 0.000 description 1
- 238000000608 laser ablation Methods 0.000 description 1
- 125000005647 linker group Chemical group 0.000 description 1
- 150000002641 lithium Chemical class 0.000 description 1
- RSNHXDVSISOZOB-UHFFFAOYSA-N lithium nickel Chemical compound [Li].[Ni] RSNHXDVSISOZOB-UHFFFAOYSA-N 0.000 description 1
- 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
- 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
- 229910052748 manganese Inorganic materials 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
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- 230000008018 melting Effects 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
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- 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
- 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
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- 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
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- 238000010298 pulverizing process Methods 0.000 description 1
- 239000002296 pyrolytic carbon Substances 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
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- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 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
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000007787 solid 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
- 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
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- 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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0088—Composites
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
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- Battery Electrode And Active Subsutance (AREA)
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)
- 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み、
前記炭素クラスターおよび前記電解質塩は、固相において粉砕混合されており、
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、
固体電解質。 - 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記載の固体電解質。 - 前記リチウム塩は、六フッ化リン酸リチウム(LiPF 6 )、四フッ化ホウ酸リチウム(LiBF 4 )、過塩素酸リチウム(LiClO 4 )、六フッ化ヒ酸リチウム(LiAsF 6 )、テトラフェニルホウ酸リチウム(LiB(C 6 H 5 ) 4 )、ビス(トリフルオロメタンスルホニル)イミドリチウム(LiN(CF 3 SO 2 ) 2 )、ビス(ペンタフルオロエタンスルホニル)イミドリチウム(LiN(C 2 F 5 SO 2 ) 2 )、(トリフルオロメタンスルホニル)(ペンタフルオロエタンスルホニル)イミドリチウム(LiN(CF 3 SO 2 )(C 2 F 5 SO 2 ))、(トリフルオロメタンスルホニル)(ヘプタフルオロプロパンスルホニル)イミドリチウム(LiN(CF 3 SO 2 )(C 3 F 7 SO 2 ))、(トリフルオロメタンスルホニル)(ノナフルオロブタンスルホニル)イミドリチウム(LiN(CF 3 SO 2 )(C 4 F 9 SO 2 ))、1,2−パーフルオロエタンジスルホニルイミドリチウム、1,3−パーフルオロプロパンジスルホニルイミドリチウム、1,3−パーフルオロブタンジスルホニルイミドリチウム、1,4−パーフルオロブタンジスルホニルイミドリチウム、およびリチウムトリス(トリフルオロメタンスルホニル)メチド(LiC(CF 3 SO 2 ) 3 )のうちの少なくとも1種である、
請求項2記載の固体電解質。 - 正極および負極と共に固体電解質を備え、
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み、
前記炭素クラスターおよび前記電解質塩は、固相において粉砕混合されており、
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、
電池。
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JP2008026356A JP5303947B2 (ja) | 2008-02-06 | 2008-02-06 | 固体電解質および電池 |
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 |
PCT/JP2009/051315 WO2009098977A1 (ja) | 2008-02-06 | 2009-01-28 | 電解質および電池 |
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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 |
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JP2008300173A (ja) * | 2007-05-31 | 2008-12-11 | Equos Research Co Ltd | リチウムイオン電池 |
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2008
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2009
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- 2009-01-28 WO PCT/JP2009/051315 patent/WO2009098977A1/ja active Application Filing
- 2009-01-28 CN CN2009801034750A patent/CN101933190A/zh active Pending
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US8492034B2 (en) | 2013-07-23 |
US20100323247A1 (en) | 2010-12-23 |
WO2009098977A1 (ja) | 2009-08-13 |
CN101933190A (zh) | 2010-12-29 |
JP2009187783A (ja) | 2009-08-20 |
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