JP2011134704A - 蓄電デバイス用負極材料及びそれを用いた蓄電デバイス用負極 - Google Patents
蓄電デバイス用負極材料及びそれを用いた蓄電デバイス用負極 Download PDFInfo
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- 239000007773 negative electrode material Substances 0.000 title claims abstract description 156
- 238000003860 storage Methods 0.000 title claims abstract description 54
- 239000000463 material Substances 0.000 title description 5
- 229920001187 thermosetting polymer Polymers 0.000 claims abstract description 23
- 239000011230 binding agent Substances 0.000 claims abstract description 20
- 229920005989 resin Polymers 0.000 claims abstract description 18
- 239000011347 resin Substances 0.000 claims abstract description 18
- 238000004519 manufacturing process Methods 0.000 claims abstract description 12
- 150000001875 compounds Chemical class 0.000 claims abstract description 3
- 230000005611 electricity Effects 0.000 claims description 35
- 229920001721 polyimide Polymers 0.000 claims description 8
- 239000002482 conductive additive Substances 0.000 claims description 6
- 239000000203 mixture Substances 0.000 claims description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 5
- 239000012752 auxiliary agent Substances 0.000 claims description 4
- 239000009719 polyimide resin Substances 0.000 claims description 4
- 239000003795 chemical substances by application Substances 0.000 claims description 3
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- 238000000576 coating method Methods 0.000 claims 1
- 238000000034 method Methods 0.000 abstract description 4
- 229910001416 lithium ion Inorganic materials 0.000 description 35
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 27
- 125000004429 atom Chemical group 0.000 description 15
- 238000006243 chemical reaction Methods 0.000 description 14
- 239000013078 crystal Substances 0.000 description 11
- 239000002184 metal Substances 0.000 description 11
- 229910052751 metal Inorganic materials 0.000 description 11
- 239000000843 powder Substances 0.000 description 11
- 229910052718 tin Inorganic materials 0.000 description 11
- 239000003990 capacitor Substances 0.000 description 10
- 238000010438 heat treatment Methods 0.000 description 10
- 239000012298 atmosphere Substances 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 8
- 230000007423 decrease Effects 0.000 description 8
- 238000007599 discharging Methods 0.000 description 8
- 238000002844 melting Methods 0.000 description 8
- 230000008018 melting Effects 0.000 description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 7
- 238000003780 insertion Methods 0.000 description 7
- 230000037431 insertion Effects 0.000 description 7
- 229910052744 lithium Inorganic materials 0.000 description 7
- 239000002994 raw material Substances 0.000 description 7
- 239000003575 carbonaceous material Substances 0.000 description 6
- 150000002500 ions Chemical class 0.000 description 6
- 229910001128 Sn alloy Inorganic materials 0.000 description 5
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 5
- 238000000605 extraction Methods 0.000 description 5
- 239000011521 glass Substances 0.000 description 5
- 229920002312 polyamide-imide Polymers 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 4
- 239000002033 PVDF binder Substances 0.000 description 4
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 4
- 239000004962 Polyamide-imide Substances 0.000 description 4
- 239000004642 Polyimide Substances 0.000 description 4
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 4
- 239000002131 composite material Substances 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 229910052698 phosphorus Inorganic materials 0.000 description 4
- 239000011574 phosphorus Substances 0.000 description 4
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 4
- 239000007774 positive electrode material Substances 0.000 description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 3
- 239000011149 active material Substances 0.000 description 3
- 230000006866 deterioration Effects 0.000 description 3
- 239000011261 inert gas Substances 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
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- -1 polytetrafluoroethylene Polymers 0.000 description 3
- 238000000634 powder X-ray diffraction Methods 0.000 description 3
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- 239000000126 substance Substances 0.000 description 3
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 3
- 229910001887 tin oxide Inorganic materials 0.000 description 3
- GEZAUFNYMZVOFV-UHFFFAOYSA-J 2-[(2-oxo-1,3,2$l^{5},4$l^{2}-dioxaphosphastannetan-2-yl)oxy]-1,3,2$l^{5},4$l^{2}-dioxaphosphastannetane 2-oxide Chemical compound [Sn+2].[Sn+2].[O-]P([O-])(=O)OP([O-])([O-])=O GEZAUFNYMZVOFV-UHFFFAOYSA-J 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- 229910020879 Sn-Li Inorganic materials 0.000 description 2
- 229910006404 SnO 2 Inorganic materials 0.000 description 2
- 229910008888 Sn—Li Inorganic materials 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 239000011889 copper foil Substances 0.000 description 2
- RKTYLMNFRDHKIL-UHFFFAOYSA-N copper;5,10,15,20-tetraphenylporphyrin-22,24-diide Chemical compound [Cu+2].C1=CC(C(=C2C=CC([N-]2)=C(C=2C=CC=CC=2)C=2C=CC(N=2)=C(C=2C=CC=CC=2)C2=CC=C3[N-]2)C=2C=CC=CC=2)=NC1=C3C1=CC=CC=C1 RKTYLMNFRDHKIL-UHFFFAOYSA-N 0.000 description 2
- 239000007772 electrode material Substances 0.000 description 2
- 239000008151 electrolyte solution Substances 0.000 description 2
- 125000005843 halogen group Chemical group 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 239000001989 lithium alloy Substances 0.000 description 2
- 239000000155 melt Substances 0.000 description 2
- 239000003960 organic solvent Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 2
- 239000010452 phosphate Substances 0.000 description 2
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 2
- 239000004810 polytetrafluoroethylene Substances 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
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- 229920005992 thermoplastic resin Polymers 0.000 description 2
- 239000011800 void material Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 229920003026 Acene Polymers 0.000 description 1
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 1
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 1
- 229910013733 LiCo Inorganic materials 0.000 description 1
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 1
- 229910015643 LiMn 2 O 4 Inorganic materials 0.000 description 1
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 1
- 229910013870 LiPF 6 Inorganic materials 0.000 description 1
- 239000004640 Melamine resin Substances 0.000 description 1
- 229920000877 Melamine resin Polymers 0.000 description 1
- 239000004743 Polypropylene Substances 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229920001807 Urea-formaldehyde Polymers 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910000905 alloy phase Inorganic materials 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- 239000010405 anode material Substances 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000005587 bubbling Effects 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 238000006482 condensation reaction Methods 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 238000004132 cross linking Methods 0.000 description 1
- 239000002178 crystalline material Substances 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000003822 epoxy resin Substances 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910052734 helium Inorganic materials 0.000 description 1
- 239000001307 helium Substances 0.000 description 1
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 1
- 239000004615 ingredient Substances 0.000 description 1
- 239000003273 ketjen black Substances 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
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 239000011255 nonaqueous electrolyte Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000005011 phenolic resin Substances 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 239000006253 pitch coke Substances 0.000 description 1
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- 239000004814 polyurethane Substances 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- QGKLPGKXAVVPOJ-UHFFFAOYSA-N pyrrolidin-3-one Chemical compound O=C1CCNC1 QGKLPGKXAVVPOJ-UHFFFAOYSA-N 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
- 238000003980 solgel method Methods 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 229920001169 thermoplastic Polymers 0.000 description 1
- 239000004416 thermosoftening plastic Substances 0.000 description 1
- 229920006337 unsaturated polyester resin Polymers 0.000 description 1
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- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/621—Binders
- H01M4/622—Binders being polymers
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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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Abstract
【解決手段】少なくともSnOとP2O5を含有する化合物からなる負極活物質と、熱硬化性樹脂からなる結着剤を含有することを特徴とする蓄電デバイス用負極材料、および当該蓄電デバイス用負極材料が集電体表面に塗布されてなる蓄電デバイス用負極。さらに、前記蓄電デバイス用負極を製造する方法であって、蓄電デバイス用負極材料を集電体表面に塗布した後、減圧下にて150〜400℃で熱処理することを特徴とする蓄電デバイス用負極の製造方法。
【選択図】なし
Description
Sn+yLi++ye-←→LiySn ・・・(2)
表1〜3に実施例1〜14および比較例1〜8を示す。各負極活物質は以下のようにして作製した。
上記で得られた負極活物質に対し、表1〜3に示す組成となるように導電助剤と結着剤を秤量し、N−メチルピロリドン(NMP)に分散した後、自転・公転ミキサーで十分に撹拌してスラリー化した。ここで、表1および2に示す実施例1〜14の負極材料には導電助剤にケッチャンブラック(以下、「KB」と略す)を用い、結着剤に実施例1〜12ではポリイミド樹脂(以下、「PI」と略す)、実施例13ではイミド化されたポリイミド樹脂(以下、「イミド化PI」と略す)、実施例14ではイミド化されたポリアミドイミド樹脂(以下、「イミド化PAI」と略す)をそれぞれ用いた。表3に示す比較例1〜8は導電助剤にKB、結着剤に熱可塑性樹脂であるポリフッ化ビニリデン(以下、「PVDF」と略す)を用いた。
コインセルの下蓋に、上記作用極を銅箔面を下に向けて載置し、その上に60℃で8時間減圧乾燥した直径16mmのポリプロピレン多孔質膜(ヘキストセラニーズ社製 セルガード#2400)からなるセパレータ、および対極である金属リチウムを積層し、試験電池を作製した。電解液としては、1M LiPF6溶液/EC:DEC=1:1(EC=エチレンカーボネート、DEC=ジエチルカーボネート)を用いた。なお試験電池の組み立ては露点温度−60℃以下の環境で行った。
充電(負極材料へのリチウムイオンの吸蔵)は、0.2mAで2Vから0VまでCC(定電流)充電を行った。次に、放電(負極材料からのリチウムイオンの放出)は、0.2mAの定電流で0Vから2Vまで放電させた。この充放電サイクルを繰り返し行った。
Claims (10)
- 少なくともSnOとP2O5を含有する化合物からなる負極活物質と、熱硬化性樹脂からなる結着剤を含有することを特徴とする蓄電デバイス用負極材料。
- さらに、導電助剤を含有することを特徴とする請求項1に記載の蓄電デバイス用負極材料。
- 質量%で、負極活物質 55〜90%、結着剤 5〜30%、導電助剤 3〜20%を含有することを特徴とする請求項2に記載の蓄電デバイス用負極材料。
- 負極活物質が、モル%で、SnO 45〜95%、P2O5 5〜55%の組成を含有す
ることを特徴とする請求項1〜3のいずれかに記載の蓄電デバイス用負極材料。 - 負極活物質が実質的に非晶質であることを特徴とする請求項1〜4のいずれかに記載の蓄電デバイス用負極材料。
- 熱硬化性樹脂がポリイミド樹脂であることを特徴とする請求項1〜5のいずれかに記載の蓄電デバイス用負極材料。
- 導電助剤が高導電性カーボンブラックであることを特徴とする請求項1〜6のいずれかに記載の蓄電デバイス用負極材料。
- 蓄電デバイスが、非水二次電池であることを特徴とする請求項1〜7のいずれかに記載の蓄電デバイス用負極材料。
- 請求項1〜8のいずれかに記載の蓄電デバイス用負極材料が集電体表面に塗布されてなる蓄電デバイス用負極。
- 請求項9に記載の蓄電デバイス用負極を製造する方法であって、蓄電デバイス用負極材料を集電体表面に塗布した後、減圧下にて150〜400℃で熱処理することを特徴とする蓄電デバイス用負極の製造方法。
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JP2009266473A (ja) * | 2008-04-23 | 2009-11-12 | Sony Corp | 負極および二次電池 |
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US5618640A (en) | 1993-10-22 | 1997-04-08 | Fuji Photo Film Co., Ltd. | Nonaqueous secondary battery |
JP3498380B2 (ja) | 1994-02-28 | 2004-02-16 | 宇部興産株式会社 | 非水二次電池 |
US5707756A (en) | 1994-11-29 | 1998-01-13 | Fuji Photo Film Co., Ltd. | Non-aqueous secondary battery |
JP3890671B2 (ja) | 1997-04-22 | 2007-03-07 | 宇部興産株式会社 | 非水電解質二次電池用負極材料の製造方法およびこれを用いた負極と電池 |
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JPH08236158A (ja) * | 1995-02-27 | 1996-09-13 | Fuji Photo Film Co Ltd | 非水二次電池 |
JPH08298121A (ja) * | 1995-04-25 | 1996-11-12 | Fuji Photo Film Co Ltd | 非水二次電池 |
JP2002231209A (ja) * | 2001-01-31 | 2002-08-16 | Matsushita Electric Ind Co Ltd | 非水電解液二次電池 |
JP2004349016A (ja) * | 2003-05-20 | 2004-12-09 | Matsushita Electric Ind Co Ltd | 非水電解質二次電池の充放電方法 |
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JP2009266473A (ja) * | 2008-04-23 | 2009-11-12 | Sony Corp | 負極および二次電池 |
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WO2011065307A1 (ja) | 2011-06-03 |
US9017870B2 (en) | 2015-04-28 |
US20120276448A1 (en) | 2012-11-01 |
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