JP6952247B2 - 正極活物質、および、電池 - Google Patents
正極活物質、および、電池 Download PDFInfo
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- JP6952247B2 JP6952247B2 JP2017235019A JP2017235019A JP6952247B2 JP 6952247 B2 JP6952247 B2 JP 6952247B2 JP 2017235019 A JP2017235019 A JP 2017235019A JP 2017235019 A JP2017235019 A JP 2017235019A JP 6952247 B2 JP6952247 B2 JP 6952247B2
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- Prior art keywords
- lithium composite
- positive electrode
- active material
- electrode active
- battery
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- 239000007774 positive electrode material Substances 0.000 title claims description 77
- 229910052744 lithium Inorganic materials 0.000 claims description 180
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 169
- 239000002131 composite material Substances 0.000 claims description 164
- 239000000203 mixture Substances 0.000 claims description 68
- 239000007773 negative electrode material Substances 0.000 claims description 21
- 239000013078 crystal Substances 0.000 claims description 20
- 229910052759 nickel Inorganic materials 0.000 claims description 19
- 239000007784 solid electrolyte Substances 0.000 claims description 19
- 229910052748 manganese Inorganic materials 0.000 claims description 16
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims description 14
- 229910052782 aluminium Inorganic materials 0.000 claims description 14
- 229910052742 iron Inorganic materials 0.000 claims description 14
- 229910001416 lithium ion Inorganic materials 0.000 claims description 14
- 229910052804 chromium Inorganic materials 0.000 claims description 12
- 229910052802 copper Inorganic materials 0.000 claims description 12
- 239000000463 material Substances 0.000 claims description 12
- 229910052719 titanium Inorganic materials 0.000 claims description 12
- 229910052720 vanadium Inorganic materials 0.000 claims description 12
- 229910052725 zinc Inorganic materials 0.000 claims description 12
- 239000011255 nonaqueous electrolyte Substances 0.000 claims description 11
- 229910052791 calcium Inorganic materials 0.000 claims description 8
- 239000003792 electrolyte Substances 0.000 claims description 8
- 229910052749 magnesium Inorganic materials 0.000 claims description 8
- 229910052750 molybdenum Inorganic materials 0.000 claims description 8
- 229910052758 niobium Inorganic materials 0.000 claims description 8
- 229910052721 tungsten Inorganic materials 0.000 claims description 8
- 229910052697 platinum Inorganic materials 0.000 claims description 7
- 229910052700 potassium Inorganic materials 0.000 claims description 7
- 229910052708 sodium Inorganic materials 0.000 claims description 7
- 229910052726 zirconium Inorganic materials 0.000 claims description 7
- 239000002245 particle Substances 0.000 claims description 6
- 229910052710 silicon Inorganic materials 0.000 claims description 5
- 229910052796 boron Inorganic materials 0.000 claims description 4
- 229910052757 nitrogen Inorganic materials 0.000 claims description 3
- 229910052698 phosphorus Inorganic materials 0.000 claims description 3
- 230000001376 precipitating effect Effects 0.000 claims description 3
- 229910052717 sulfur Inorganic materials 0.000 claims description 2
- 150000001875 compounds Chemical class 0.000 description 45
- 239000010410 layer Substances 0.000 description 29
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- 239000011572 manganese Substances 0.000 description 27
- -1 LiF Chemical class 0.000 description 26
- 238000000034 method Methods 0.000 description 25
- 230000000052 comparative effect Effects 0.000 description 23
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 23
- 239000002994 raw material Substances 0.000 description 23
- 229910052760 oxygen Inorganic materials 0.000 description 18
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 15
- 239000001301 oxygen Substances 0.000 description 15
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- 238000006479 redox reaction Methods 0.000 description 11
- 235000002639 sodium chloride Nutrition 0.000 description 11
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- 229910003002 lithium salt Inorganic materials 0.000 description 10
- 159000000002 lithium salts Chemical class 0.000 description 10
- 239000003125 aqueous solvent Substances 0.000 description 9
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 9
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 8
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- 239000008151 electrolyte solution Substances 0.000 description 7
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- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 6
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- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 4
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- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 4
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- 229910012851 LiCoO 2 Inorganic materials 0.000 description 3
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- 239000004698 Polyethylene Substances 0.000 description 3
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 3
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- 239000012856 weighed raw material Substances 0.000 description 3
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 2
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 2
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- 229910008522 Li1.2Mn0.54Co0.13Ni0.13O2 Inorganic materials 0.000 description 2
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- QLOAVXSYZAJECW-UHFFFAOYSA-N methane;molecular fluorine Chemical compound C.FF QLOAVXSYZAJECW-UHFFFAOYSA-N 0.000 description 1
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- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 238000005191 phase separation Methods 0.000 description 1
- 125000000843 phenylene group Chemical group C1(=C(C=CC=C1)*)* 0.000 description 1
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 1
- 229920002647 polyamide Polymers 0.000 description 1
- 229920002312 polyamide-imide Polymers 0.000 description 1
- 229920000447 polyanionic polymer Polymers 0.000 description 1
- 229920000570 polyether Polymers 0.000 description 1
- 229920006393 polyether sulfone Polymers 0.000 description 1
- 229920001721 polyimide Polymers 0.000 description 1
- 239000004926 polymethyl methacrylate Substances 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 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
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 238000004611 spectroscopical analysis Methods 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 230000000087 stabilizing effect Effects 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 125000001424 substituent group Chemical group 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 230000002194 synthesizing effect Effects 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
- 238000012360 testing method Methods 0.000 description 1
- 125000005207 tetraalkylammonium group Chemical group 0.000 description 1
- 125000005497 tetraalkylphosphonium group Chemical group 0.000 description 1
- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
- 239000006234 thermal black Substances 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 229910021561 transition metal fluoride Inorganic materials 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 1
- 238000007740 vapor deposition Methods 0.000 description 1
- 239000012808 vapor phase Substances 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
- 239000002759 woven fabric Substances 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
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Description
実施の形態1における正極活物質は、リチウム複合酸化物と、リチウム複合オキシフッ化物と、を含む。また、リチウム複合オキシフッ化物は、リチウム複合酸化物の表面の少なくとも一部を被覆している。
ここで、Me1は、Mn、Co、Ni、Fe、Al、Cu、V、Nb、Mo、Ti、Cr、Zr、Zn、Na、K、Ca、Mg、Pt、Au、Ru、Wからなる群より選択される一種または二種以上の元素であってもよい。
0.5≦x≦1.34、
0.5≦y≦1.0、
0≦z≦0.5、
1.5≦x+y+z≦2.0、
を満たしてもよい。
ここで、Me2は、Mn、Co、Ni、Fe、Al、Cu、V、Nb、Mo、Ti、Cr、Zr、Zn、Na、K、Ca、Mg、Pt、Au、Ru、Wからなる群より選択される一種または二種以上の元素であってもよい。
1.0≦α≦2.1、
0.8≦β≦1.3、
1.5≦γ≦2.9、
0.1≦δ≦1.5、
を満たしてもよい。
1.0≦α≦2.0、
β=1.0、
1.5≦γ≦2.0、
0.5≦δ≦1.0、
を満たしてもよい。
以下に、実施の形態1の正極活物質の製造方法の一例が、説明される。
以下、実施の形態2が説明される。なお、上述の実施の形態1と重複する説明は、適宜、省略される。
[リチウム複合酸化物の作製]
LiOH・H2OとNi0.85Co0.1Al0.05(OH)2とを、Li/(Ni+Co+Al)=1のモル比となるように秤量した。
また、得られたリチウム複合酸化物の組成を、ICP発光分光分析法および不活性ガス溶融−赤外吸収法およびイオンクロマトグラフィーにより求めた。
LiFとLiMnO2とを、Li/Mn/O/F=2/1/2/1のモル比となるように秤量した。
上述のように得られたリチウム複合酸化物とリチウム複合オキシフッ化物とを、100:5の質量比で(すなわち、リチウム複合オキシフッ化物が、リチウム複合酸化物に対して、5質量%含むように)秤量し、めのう乳鉢で10分間混合することで、正極活物質を得た。
次に、70質量部の上述の正極活物質と、20質量部の導電剤と、10質量部のポリフッ化ビニリデン(PVDF)と、適量の2−メチルピロリドン(NMP)とを、混合した。これにより、正極合剤スラリーを得た。
上述の実施例1から、リチウム複合酸化物およびリチウム複合オキシフッ化物を、表1に示す組成および質量比となるように変更した。
実施例1と同様の手法を用いて、リチウム複合酸化物(LiNi0.85Co0.1Al0.05O2)を得た。なお、リチウム複合オキシフッ化物は、用いなかった。
上述の比較例1から、リチウム複合酸化物を、表1に示す組成となるように変更した。これ以外は、上述の比較例1と同様にして、比較例2〜5の正極活物質を合成した。
正極に対する電流密度を0.2mA/cm2、充電終止電圧を4.3Vに設定し、実施例1および比較例1の電池を充電した。
11 ケース
12 正極集電体
13 正極活物質層
14 セパレータ
15 封口板
16 負極集電体
17 負極活物質層
18 ガスケット
21 正極
22 負極
Claims (13)
- リチウム複合酸化物と、
前記リチウム複合酸化物の少なくとも一部を被覆するリチウム複合オキシフッ化物と、を含み、
前記リチウム複合オキシフッ化物は、組成式LiαMe2βOγFδ(ここで、前記Me2は、Mn、Co、Ni、Fe、Al、Cu、V、Nb、Mo、Ti、Cr、Zr、Zn、Na、K、Ca、Mg、Pt、Au、Ru、及びWからなる群より選択される少なくとも一種であり、1.0≦α≦2.1、 0.8≦β≦1.3、 1.5≦γ≦2.9、かつ、0.1≦δ≦1.5)で表され、
前記リチウム複合オキシフッ化物の結晶構造は空間群Fm−3mに属し、
前記Me2は、Mn、Co、Ni、Fe、Cu、V、Ti、Cr、及びZnからなる群より選択される少なくとも一種を含む、
正極活物質。 - リチウム複合酸化物と、
前記リチウム複合酸化物の少なくとも一部を被覆するリチウム複合オキシフッ化物と、を含み、
前記リチウム複合オキシフッ化物は、組成式Li α Me2 β O γ F δ (ここで、前記Me2は、Mn、Co、Ni、Fe、Al、Cu、V、Nb、Mo、Ti、Cr、Zr、Zn、Na、K、Ca、Mg、Pt、Au、Ru、及びWからなる群より選択される少なくとも一種であり、1.0≦α≦2.0、 β=1.0、 1.5≦γ≦2.0、かつ、0.5≦δ≦1.0)で表され、
前記リチウム複合オキシフッ化物の結晶構造は空間群Fm−3mに属する、
正極活物質。 - 正極活物質であって、
リチウム複合酸化物と、
前記リチウム複合酸化物の少なくとも一部を被覆するリチウム複合オキシフッ化物と、を含み、
前記リチウム複合オキシフッ化物は、組成式Li α Me2 β O γ F δ (ここで、前記Me2は、Mn、Co、Ni、Fe、Al、Cu、V、Nb、Mo、Ti、Cr、Zr、Zn、Na、K、Ca、Mg、Pt、Au、Ru、及びWからなる群より選択される少なくとも一種であり、1.0≦α≦2.1、 0.8≦β≦1.3、 1.5≦γ≦2.9、かつ、0.1≦δ≦1.5)で表され、
前記リチウム複合オキシフッ化物の結晶構造は空間群Fm−3mに属し、
前記正極活物質は、前記リチウム複合酸化物を含有する複数の第1粒子と、前記リチウム複合オキシフッ化物を含有する複数の第2粒子との混合体であり、
前記複数の第1粒子の少なくとも1つが、前記複数の第2粒子の少なくとも1つと直接接触している、
正極活物質。 - 前記Me2は、Mn、Co、Ni、Fe、Cu、V、Ti、Cr、及びZnからなる群より選択される少なくとも一種を含む、請求項2又は3に記載の正極活物質。
- 前記リチウム複合酸化物は、組成式LixMe1yAzO2(ここで、前記Me1は、Mn、Co、Ni、Fe、Al、Cu、V、Nb、Mo、Ti、Cr、Zr、Zn、Na、K、Ca、Mg、Pt、Au、Ru、及びWからなる群より選択される少なくとも一種であり、前記Aは、B、P、Si、S、及びNからなる群より選択される少なくとも一種であり、0.5≦x≦1.34、 0.5≦y≦1.0、 0≦z≦0.5、かつ、1.5≦x+y+z≦2.0)で表される、
請求項1〜4のいずれか1項に記載の正極活物質。 - 前記Me2は、MnおよびNiからなる群より選択される少なくとも一種を含む、
請求項1から5のいずれか一項に記載の正極活物質。 - 前記正極活物質は、前記リチウム複合酸化物を、主成分として含む、
請求項1から6のいずれかに記載の正極活物質。 - 前記リチウム複合酸化物に対する前記リチウム複合オキシフッ化物の質量比が、0.001以上かつ0.1以下である、
請求項1から7のいずれか一項に記載の正極活物質。 - 前記質量比が、0.01以上かつ0.05以下である、
請求項8に記載の正極活物質。 - 請求項1から9のいずれか一項に記載の正極活物質を含む正極と、
負極と、
電解質と、
を備える、
電池。 - 前記正極は、前記正極活物質を主成分として含む正極活物質層を備える、
請求項10に記載の電池。 - 前記負極は、リチウムイオンを吸蔵および放出しうる負極活物質、または、リチウム金属を負極活物質として溶解および析出させうる材料を含み、
前記電解質は、非水電解液である、
請求項10または11に記載の電池。 - 前記負極は、リチウムイオンを吸蔵および放出しうる負極活物質、または、リチウム金属を負極活物質として溶解および析出させうる材料を含み、
前記電解質は、固体電解質である、
請求項10または11に記載の電池。
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