JP2015513193A - 性能に優れたリチウム二次電池 - Google Patents
性能に優れたリチウム二次電池 Download PDFInfo
- Publication number
- JP2015513193A JP2015513193A JP2014560868A JP2014560868A JP2015513193A JP 2015513193 A JP2015513193 A JP 2015513193A JP 2014560868 A JP2014560868 A JP 2014560868A JP 2014560868 A JP2014560868 A JP 2014560868A JP 2015513193 A JP2015513193 A JP 2015513193A
- Authority
- JP
- Japan
- Prior art keywords
- secondary battery
- lithium secondary
- negative electrode
- positive electrode
- lithium
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 45
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 44
- 239000007773 negative electrode material Substances 0.000 claims abstract description 14
- 239000008151 electrolyte solution Substances 0.000 claims abstract description 11
- 239000012528 membrane Substances 0.000 claims abstract description 10
- 238000000926 separation method Methods 0.000 claims abstract description 10
- FDLZQPXZHIFURF-UHFFFAOYSA-N [O-2].[Ti+4].[Li+] Chemical compound [O-2].[Ti+4].[Li+] FDLZQPXZHIFURF-UHFFFAOYSA-N 0.000 claims abstract description 9
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 16
- 239000000126 substance Substances 0.000 claims description 16
- 239000002131 composite material Substances 0.000 claims description 12
- 239000010936 titanium Substances 0.000 claims description 12
- 239000007774 positive electrode material Substances 0.000 claims description 11
- 229910052782 aluminium Inorganic materials 0.000 claims description 10
- 239000011572 manganese Substances 0.000 claims description 9
- 229910052759 nickel Inorganic materials 0.000 claims description 9
- 229910052719 titanium Inorganic materials 0.000 claims description 9
- 239000010949 copper Substances 0.000 claims description 7
- KLARSDUHONHPRF-UHFFFAOYSA-N [Li].[Mn] Chemical compound [Li].[Mn] KLARSDUHONHPRF-UHFFFAOYSA-N 0.000 claims description 6
- 229910052802 copper Inorganic materials 0.000 claims description 6
- 229910052742 iron Inorganic materials 0.000 claims description 6
- ZYXUQEDFWHDILZ-UHFFFAOYSA-N [Ni].[Mn].[Li] Chemical compound [Ni].[Mn].[Li] ZYXUQEDFWHDILZ-UHFFFAOYSA-N 0.000 claims description 5
- 229910009109 Li1.33Ti1.67O4 Inorganic materials 0.000 claims description 4
- 229910052796 boron Inorganic materials 0.000 claims description 4
- 229910052596 spinel Inorganic materials 0.000 claims description 4
- 239000011029 spinel Substances 0.000 claims description 4
- 229910052725 zinc Inorganic materials 0.000 claims description 4
- 229910002099 LiNi0.5Mn1.5O4 Inorganic materials 0.000 claims description 3
- 229910012465 LiTi Inorganic materials 0.000 claims description 3
- 229910052804 chromium Inorganic materials 0.000 claims description 3
- 229910052749 magnesium Inorganic materials 0.000 claims description 3
- 150000001450 anions Chemical class 0.000 claims description 2
- 229910052787 antimony Inorganic materials 0.000 claims description 2
- 229910052797 bismuth Inorganic materials 0.000 claims description 2
- 229910052791 calcium Inorganic materials 0.000 claims description 2
- 229910052758 niobium Inorganic materials 0.000 claims description 2
- 238000003860 storage Methods 0.000 claims description 2
- 229910052721 tungsten Inorganic materials 0.000 claims description 2
- 229910052720 vanadium Inorganic materials 0.000 claims description 2
- 229910052726 zirconium Inorganic materials 0.000 claims description 2
- 229910012409 LiNi0.4Mn1.6O4 Inorganic materials 0.000 claims 1
- -1 Nickel metal hydride Chemical class 0.000 description 25
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 13
- 230000003647 oxidation Effects 0.000 description 10
- 238000007254 oxidation reaction Methods 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 9
- 239000004020 conductor Substances 0.000 description 8
- 239000003792 electrolyte Substances 0.000 description 8
- 239000000203 mixture Substances 0.000 description 8
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 7
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 6
- 239000011230 binding agent Substances 0.000 description 6
- 229910052799 carbon Inorganic materials 0.000 description 6
- 229910003002 lithium salt Inorganic materials 0.000 description 6
- 159000000002 lithium salts Chemical class 0.000 description 6
- 239000007784 solid electrolyte Substances 0.000 description 6
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 5
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- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 3
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- 230000000694 effects Effects 0.000 description 3
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- 239000011701 zinc Substances 0.000 description 3
- WNXJIVFYUVYPPR-UHFFFAOYSA-N 1,3-dioxolane Chemical compound C1COCO1 WNXJIVFYUVYPPR-UHFFFAOYSA-N 0.000 description 2
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- 229910013063 LiBF 4 Inorganic materials 0.000 description 2
- 229910013684 LiClO 4 Inorganic materials 0.000 description 2
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 2
- 239000002033 PVDF binder Substances 0.000 description 2
- 239000004372 Polyvinyl alcohol Substances 0.000 description 2
- JUJWROOIHBZHMG-UHFFFAOYSA-N Pyridine Chemical compound C1=CC=NC=C1 JUJWROOIHBZHMG-UHFFFAOYSA-N 0.000 description 2
- KAESVJOAVNADME-UHFFFAOYSA-N Pyrrole Chemical compound C=1C=CNC=1 KAESVJOAVNADME-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 2
- 239000004917 carbon fiber Substances 0.000 description 2
- 239000003575 carbonaceous material Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
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- 150000001875 compounds Chemical class 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- LYCAIKOWRPUZTN-UHFFFAOYSA-N ethylene glycol Natural products OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
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- 229910002804 graphite Inorganic materials 0.000 description 2
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- 229910052736 halogen Inorganic materials 0.000 description 2
- 150000002367 halogens Chemical class 0.000 description 2
- 229910003480 inorganic solid Inorganic materials 0.000 description 2
- AMXOYNBUYSYVKV-UHFFFAOYSA-M lithium bromide Chemical compound [Li+].[Br-] AMXOYNBUYSYVKV-UHFFFAOYSA-M 0.000 description 2
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- TZIHFWKZFHZASV-UHFFFAOYSA-N methyl formate Chemical compound COC=O TZIHFWKZFHZASV-UHFFFAOYSA-N 0.000 description 2
- LQNUZADURLCDLV-UHFFFAOYSA-N nitrobenzene Chemical compound [O-][N+](=O)C1=CC=CC=C1 LQNUZADURLCDLV-UHFFFAOYSA-N 0.000 description 2
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- 238000011160 research Methods 0.000 description 2
- 229910052709 silver Inorganic materials 0.000 description 2
- 239000004332 silver Substances 0.000 description 2
- VZGDMQKNWNREIO-UHFFFAOYSA-N tetrachloromethane Chemical compound ClC(Cl)(Cl)Cl VZGDMQKNWNREIO-UHFFFAOYSA-N 0.000 description 2
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 2
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- 229910006555 Li—Co—Ni Inorganic materials 0.000 description 1
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- 239000004472 Lysine Substances 0.000 description 1
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 1
- ZHGDJTMNXSOQDT-UHFFFAOYSA-N NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O Chemical compound NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O.NP(N)(N)=O ZHGDJTMNXSOQDT-UHFFFAOYSA-N 0.000 description 1
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- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 1
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- RSNHXDVSISOZOB-UHFFFAOYSA-N lithium nickel Chemical compound [Li].[Ni] RSNHXDVSISOZOB-UHFFFAOYSA-N 0.000 description 1
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 1
- VROAXDSNYPAOBJ-UHFFFAOYSA-N lithium;oxido(oxo)nickel Chemical compound [Li+].[O-][Ni]=O VROAXDSNYPAOBJ-UHFFFAOYSA-N 0.000 description 1
- VLXXBCXTUVRROQ-UHFFFAOYSA-N lithium;oxido-oxo-(oxomanganiooxy)manganese Chemical compound [Li+].[O-][Mn](=O)O[Mn]=O VLXXBCXTUVRROQ-UHFFFAOYSA-N 0.000 description 1
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- 229910000480 nickel oxide Inorganic materials 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- LYGJENNIWJXYER-UHFFFAOYSA-N nitromethane Chemical compound C[N+]([O-])=O LYGJENNIWJXYER-UHFFFAOYSA-N 0.000 description 1
- 229910021470 non-graphitizable carbon Inorganic materials 0.000 description 1
- 238000010943 off-gassing Methods 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 1
- 230000000737 periodic effect Effects 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
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 229920001197 polyacetylene Polymers 0.000 description 1
- 229920000728 polyester Polymers 0.000 description 1
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- 229920000036 polyvinylpyrrolidone Polymers 0.000 description 1
- 239000001267 polyvinylpyrrolidone Substances 0.000 description 1
- 235000013855 polyvinylpyrrolidone Nutrition 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
- 239000000843 powder Substances 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
- 239000001008 quinone-imine dye Substances 0.000 description 1
- 239000004627 regenerated cellulose Substances 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 230000001568 sexual effect Effects 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000008107 starch Substances 0.000 description 1
- 235000019698 starch Nutrition 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 229920005608 sulfonated EPDM Polymers 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 1
- TXEYQDLBPFQVAA-UHFFFAOYSA-N tetrafluoromethane Chemical compound FC(F)(F)F TXEYQDLBPFQVAA-UHFFFAOYSA-N 0.000 description 1
- 239000006234 thermal black Substances 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- BDZBKCUKTQZUTL-UHFFFAOYSA-N triethyl phosphite Chemical compound CCOP(OCC)OCC BDZBKCUKTQZUTL-UHFFFAOYSA-N 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
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- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
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- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
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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
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
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- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
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Abstract
Description
Mは、Al、Mg、Ni、Co、Fe、Cr、V、Ti、Cu、B、Ca、Zn、Zr、Nb、Mo、Sr、Sb、W、Ti及びBiからなる群から選択される一つ以上の元素であり、
Aは、−1または−2価の一つ以上のアニオンである。
負極活物質(Li1.33Ti1.67O4)、導電材(Denka black)、バインダー(PVdF)を90:5:5の重量比でNMPに入れ、ミキシングして負極合剤を製造し、20μmの厚さのアルミニウムホイルに前記負極合剤をコーティングした後、圧延及び乾燥して、6.6mg/cm2の負極を製造した。
上記実施例1において、負極の重量を6.6mg/cm2、正極の重量を7.8mg/cm2になるように製造したこと以外は、実施例1と同様の方法でリチウム二次電池を製造した。
上記実施例1において、負極の重量を6.6mg/cm2、正極の重量を7.1mg/cm2になるように製造したこと以外は、実施例1と同様の方法でリチウム二次電池を製造した。
上記実施例1、2及び比較例1に係る二次電池のカットオフ電圧を3.5Vに設定し、カットオフ電圧に到達時に、負極の電位及び正極の電位をそれぞれ測定して、下記表1に示す。
二次電池の寿命特性の評価
上記実施例1、2及び比較例1の二次電池を1C、600mAで2〜3.35Vの範囲で充放電を進行し、これを常温で50サイクル反復実施しながら電池の充電容量の変化を測定し、その結果を図1に示す。
二次電池のガス発生量の測定
上記実施例1、2及び比較例1の二次電池を、1C、600mAで2〜3.35Vの範囲で充放電を進行し、これを常温で50サイクル反復実施した後、50サイクル下でガス発生量を測定して、図2に示す。
Claims (15)
- 正極、負極、前記正極と前記負極との間に配置される分離膜で構成された電極組立体及び電解液を含むリチウム二次電池であって、
前記負極が、負極活物質としてリチウムチタン酸化物(Lithium Titanium Oxide:LTO)を含んでおり、
前記リチウム二次電池は、3.3〜4Vの範囲の充電カットオフ電圧(cut−off voltage)を有し、前記カットオフ電圧に到達時に、負極の電位は、正極の電位が4.95Vを超えない範囲で0.75〜1.545Vであることを特徴とする、リチウム二次電池。 - 前記リチウム二次電池のカットオフ電圧(cut−off voltage)は3.3〜3.5Vであり、前記カットオフ電圧に到達時に、前記負極の電位は、正極の電位が4.95Vを超えない範囲で1.2〜1.545Vであることを特徴とする、請求項1に記載のリチウム二次電池。
- 前記リチウムチタン酸化物(LTO)は、下記化学式1で表されることを特徴とする、請求項1に記載のリチウム二次電池:
LiaTibO4(1)
上記式中、0.5≦a≦3、1≦b≦2.5である。 - 前記リチウムチタン酸化物は、Li1.33Ti1.67O4またはLiTi2O4であることを特徴とする、請求項3に記載のリチウム二次電池。
- 前記正極は高電圧正極であることを特徴とする、請求項1に記載のリチウム二次電池。
- 前記正極は、正極活物質として、下記化学式2で表されるスピネル構造のリチウムマンガン複合酸化物を含むことを特徴とする、請求項5に記載のリチウム二次電池:
LixMyMn2−yO4−zAz(2)
上記式中、0.9≦x≦1.2、0<y<2、0≦z<0.2であり、
Mは、Al、Mg、Ni、Co、Fe、Cr、V、Ti、Cu、B、Ca、Zn、Zr、Nb、Mo、Sr、Sb、W、Ti及びBiからなる群から選択される一つ以上の元素であり、
Aは、−1または−2価の一つ以上のアニオンである。 - 前記化学式2で表されるリチウムマンガン複合酸化物は、下記化学式3で表されるリチウムニッケルマンガン複合酸化物であることを特徴とする、請求項6に記載のリチウム二次電池:
LixNiyMn2−yO4(3)
上記式中、0.9≦x≦1.2、0.4≦y≦0.5である。 - 前記リチウムニッケルマンガン複合酸化物は、LiNi0.5Mn1.5O4またはLiNi0.4Mn1.6O4であることを特徴とする、請求項7に記載のリチウム二次電池。
- 前記負極の容量は、前記正極の容量と同一または小さいことを特徴とする、請求項1に記載のリチウム二次電池。
- 前記負極の容量が、前記正極の容量を基準として80〜100%であることを特徴とする、請求項9に記載のリチウム二次電池。
- 前記負極の容量が、前記正極の容量を基準として90〜100%であることを特徴とする、請求項10に記載のリチウム二次電池。
- 請求項1に記載のリチウム二次電池を単位電池として含むことを特徴とする、電池モジュール。
- 請求項12に記載の電池モジュールを含むことを特徴とする、電池パック。
- 請求項13に記載の電池パックを含むことを特徴とする、デバイス。
- 前記デバイスは、電気自動車、ハイブリッド電気自動車、プラグインハイブリッド電気自動車、または電力貯蔵用システムであることを特徴とする、請求項14に記載のデバイス。
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JP2010067496A (ja) * | 2008-09-11 | 2010-03-25 | National Univ Corp Shizuoka Univ | 電解液およびその利用 |
JP2012043709A (ja) * | 2010-08-20 | 2012-03-01 | Toshiba Corp | 非水電解質電池 |
WO2013100081A1 (ja) * | 2011-12-28 | 2013-07-04 | 三菱化学株式会社 | 非水系電解液及び非水系電解液二次電池 |
Cited By (3)
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JP2021518988A (ja) * | 2018-06-08 | 2021-08-05 | エルジー・ケム・リミテッド | リチウム二次電池用負極スラリー、及びこの製造方法 |
JP7114155B2 (ja) | 2018-06-08 | 2022-08-08 | エルジー エナジー ソリューション リミテッド | リチウム二次電池用負極スラリー、及びこの製造方法 |
US11581531B2 (en) | 2018-06-08 | 2023-02-14 | Lg Energy Solution, Ltd. | Negative electrode slurry for lithium secondary battery, and preparation method thereof |
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KR20130117709A (ko) | 2013-10-28 |
WO2013157853A1 (ko) | 2013-10-24 |
EP2811570B1 (en) | 2016-09-14 |
US9825293B2 (en) | 2017-11-21 |
EP2811570A4 (en) | 2015-06-24 |
CN104170149A (zh) | 2014-11-26 |
CN104170149B (zh) | 2017-07-18 |
JP6240100B2 (ja) | 2017-11-29 |
KR101507450B1 (ko) | 2015-03-31 |
US20140377656A1 (en) | 2014-12-25 |
EP2811570A1 (en) | 2014-12-10 |
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