JP5789890B2 - 高容量の正極活物質及びこれを含むリチウム二次電池 - Google Patents
高容量の正極活物質及びこれを含むリチウム二次電池 Download PDFInfo
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- 239000007774 positive electrode material Substances 0.000 title claims description 70
- 229910052744 lithium Inorganic materials 0.000 title claims description 59
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims description 56
- 229910000314 transition metal oxide Inorganic materials 0.000 claims description 53
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 36
- 239000004020 conductor Substances 0.000 claims description 18
- 230000002427 irreversible effect Effects 0.000 claims description 14
- 239000000126 substance Substances 0.000 claims description 14
- 238000007599 discharging Methods 0.000 claims description 11
- 229910002804 graphite Inorganic materials 0.000 claims description 11
- 239000010439 graphite Substances 0.000 claims description 11
- 229910052799 carbon Inorganic materials 0.000 claims description 10
- 229910002102 lithium manganese oxide Inorganic materials 0.000 claims description 8
- VLXXBCXTUVRROQ-UHFFFAOYSA-N lithium;oxido-oxo-(oxomanganiooxy)manganese Chemical compound [Li+].[O-][Mn](=O)O[Mn]=O VLXXBCXTUVRROQ-UHFFFAOYSA-N 0.000 claims description 8
- 239000000463 material Substances 0.000 claims description 7
- 239000013078 crystal Substances 0.000 claims description 6
- 229910044991 metal oxide Inorganic materials 0.000 claims description 6
- 150000004706 metal oxides Chemical class 0.000 claims description 6
- 229910052782 aluminium Inorganic materials 0.000 claims description 4
- QTHKJEYUQSLYTH-UHFFFAOYSA-N [Co]=O.[Ni].[Li] Chemical compound [Co]=O.[Ni].[Li] QTHKJEYUQSLYTH-UHFFFAOYSA-N 0.000 claims description 3
- OGCCXYAKZKSSGZ-UHFFFAOYSA-N [Ni]=O.[Mn].[Li] Chemical compound [Ni]=O.[Mn].[Li] OGCCXYAKZKSSGZ-UHFFFAOYSA-N 0.000 claims description 3
- 239000006230 acetylene black Substances 0.000 claims description 3
- 229910052787 antimony Inorganic materials 0.000 claims description 3
- 229910052797 bismuth Inorganic materials 0.000 claims description 3
- 229910052796 boron Inorganic materials 0.000 claims description 3
- 229910052791 calcium Inorganic materials 0.000 claims description 3
- 239000006231 channel black Substances 0.000 claims description 3
- 229910052804 chromium Inorganic materials 0.000 claims description 3
- 229910052802 copper Inorganic materials 0.000 claims description 3
- 239000006232 furnace black Substances 0.000 claims description 3
- 229910021389 graphene Inorganic materials 0.000 claims description 3
- 229910052742 iron Inorganic materials 0.000 claims description 3
- 239000003273 ketjen black Substances 0.000 claims description 3
- 239000006233 lamp black Substances 0.000 claims description 3
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 claims description 3
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 claims description 3
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 claims description 3
- 229910052749 magnesium Inorganic materials 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 3
- 229910052758 niobium Inorganic materials 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 229910052721 tungsten Inorganic materials 0.000 claims description 3
- 229910052720 vanadium Inorganic materials 0.000 claims description 3
- 229910052725 zinc Inorganic materials 0.000 claims description 3
- 229910052726 zirconium Inorganic materials 0.000 claims description 3
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical compound [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 claims description 2
- 239000006229 carbon black Substances 0.000 claims description 2
- BVPMZCWLVVIHKO-UHFFFAOYSA-N lithium cobalt(2+) manganese(2+) oxygen(2-) Chemical compound [O-2].[Mn+2].[Co+2].[Li+] BVPMZCWLVVIHKO-UHFFFAOYSA-N 0.000 claims description 2
- 238000000034 method Methods 0.000 description 10
- 239000002245 particle Substances 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 7
- 239000002131 composite material Substances 0.000 description 4
- AMWRITDGCCNYAT-UHFFFAOYSA-L manganese oxide Inorganic materials [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 4
- 239000012528 membrane Substances 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 238000000926 separation method Methods 0.000 description 4
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000003792 electrolyte Substances 0.000 description 3
- 229910001416 lithium ion Inorganic materials 0.000 description 3
- 239000011572 manganese Substances 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 238000011160 research Methods 0.000 description 3
- 229910052723 transition metal Inorganic materials 0.000 description 3
- 150000003624 transition metals Chemical class 0.000 description 3
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 2
- -1 and summer black Substances 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 210000001787 dendrite Anatomy 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 229920000642 polymer Polymers 0.000 description 2
- 0 *=C1C=CC=C1 Chemical compound *=C1C=CC=C1 0.000 description 1
- 229910015645 LiMn Inorganic materials 0.000 description 1
- 229910015643 LiMn 2 O 4 Inorganic materials 0.000 description 1
- 229910014689 LiMnO Inorganic materials 0.000 description 1
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- SOXUFMZTHZXOGC-UHFFFAOYSA-N [Li].[Mn].[Co].[Ni] Chemical compound [Li].[Mn].[Co].[Ni] SOXUFMZTHZXOGC-UHFFFAOYSA-N 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 238000003915 air pollution Methods 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910021383 artificial graphite Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 239000006182 cathode active material Substances 0.000 description 1
- 210000004027 cell Anatomy 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- XEUFSQHGFWJHAP-UHFFFAOYSA-N cobalt(2+) manganese(2+) oxygen(2-) Chemical compound [O--].[O--].[Mn++].[Co++] XEUFSQHGFWJHAP-UHFFFAOYSA-N 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 229920001940 conductive polymer Polymers 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000004880 explosion Methods 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 230000001939 inductive effect Effects 0.000 description 1
- 229910021437 lithium-transition metal oxide Inorganic materials 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- PPNAOCWZXJOHFK-UHFFFAOYSA-N manganese(2+);oxygen(2-) Chemical class [O-2].[Mn+2] PPNAOCWZXJOHFK-UHFFFAOYSA-N 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 239000007773 negative electrode material Substances 0.000 description 1
- 229910000480 nickel oxide Inorganic materials 0.000 description 1
- 239000011255 nonaqueous electrolyte Substances 0.000 description 1
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229920001690 polydopamine Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 239000011163 secondary particle Substances 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
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- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- 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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- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
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- C01G45/1221—Manganates or manganites with a manganese oxidation state of Mn(III), Mn(IV) or mixtures thereof
- C01G45/125—Manganates or manganites with a manganese oxidation state of Mn(III), Mn(IV) or mixtures thereof of the type[MnO3]n-, e.g. Li2MnO3, Li2[MxMn1-xO3], (La,Sr)MnO3
- C01G45/1257—Manganates or manganites with a manganese oxidation state of Mn(III), Mn(IV) or mixtures thereof of the type[MnO3]n-, e.g. Li2MnO3, Li2[MxMn1-xO3], (La,Sr)MnO3 containing lithium, e.g. Li2MnO3, Li2[MxMn1-xO3
-
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- C01G53/00—Compounds of nickel
- C01G53/40—Nickelates
- C01G53/42—Nickelates containing alkali metals, e.g. LiNiO2
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Description
[化1]
xMnO2・(1-x)Li2MnO3(0<x<1) (1)
[化2]
xMnO2・(1-x)Li2MnO3(0<x<1) (1)
[化3]
Li2NixCu1-xO2(0≦x≦1) (2)
下記式(1)で表されるリチウムマンガン酸化物(第1遷移金属酸化物)と、
4.3V〜2.5Vの電圧範囲で充放電を行う場合、初サイクルでの充電容量と放電容量の差(非可逆容量)が200mAh/g以上のリチウム含有遷移金属酸化物(第2遷移金属酸化物)とを含む正極活物質を提供する。
[化4]
xMnO2・(1-x)Li2MnO3(0<x<1) (1)
[化5]
Li2NixCu1-xO2(0≦x≦1) (2)
正極の製造
正極活物質として、0.9MnO2-0.1Li2MnO3(60重量%)とLi2NiO2(40重量%)からなる混合物90重量%、導電材のデンカブラック6重量%、バインダーのPVDF 4重量%と共にNMPに添加してスラリーを製造した。これを正極集電体のアルミニウム(Al)箔上にコーティングし、圧延及び乾燥してリチウム二次電池用正極を製造した。
前記のように製造された正極と黒鉛系負極の間に多孔性ポリエチレンの分離膜を介在し、リチウム電解液を注入し、ポリマータイプのリチウム二次電池を製造した。
正極活物質として0.9MnO2-0.1Li2MnO3のみを用い、負極としてリチウム金属を用いてハーフセル(half-cell)を製造したことを除いては、実施例と同様の方法で充放電に伴う容量を測定した。
正極活物質としてLi2NiO2のみを用いたことを除いては、実施例と同様の方法で充放電に伴う容量を測定した。
前記実施例及び比較例1、2に係るリチウム二次電池に対し、4.3V〜2.5Vの電圧範囲で充放電しながら電池の容量を評価した結果を、図1から図3に記載した。
Claims (12)
- 下記式(1)で表されるリチウムマンガン酸化物(第1遷移金属酸化物)と、
4.3V〜2.5Vの電圧範囲で充放電を行う場合、初サイクルでの充電容量と放電容量の差(非可逆容量)が200mAh/g以上であり、下記式(2)で表されるリチウム含有遷移金属酸化物(第2遷移金属酸化物)とを含む正極活物質であって、
前記第2遷移金属酸化物は、正極活物質100重量部に対し20から40重量部で含まれる正極活物質。
[化1]
xMnO2・(1−x)Li2MnO3(0<x<1) (1)
[化2]
Li 2 NixCu 1−x O 2 (0≦x≦1) (2) - 前記第2遷移金属酸化物は、250mAh/g以上の非可逆容量を有することを特徴とする請求項1に記載の正極活物質。
- 前記正極活物質は、導電材をさらに含むことを特徴とする請求項1または2に記載の正極活物質。
- 前記導電材は、黒鉛及び導電性炭素からなることを特徴とする請求項3に記載の正極活物質。
- 前記導電材は、前記正極活物質100重量部に対し0.5から15重量部で含まれることを特徴とする請求項3又は4に記載の正極活物質。
- 前記導電性炭素は、アセチレンブラック、ケッチェンブラック、チャンネルブラック、ファーネスブラック、ランプブラック、及びサーマルブラックからなる群から選択されるカーボンブラック、又は結晶構造がグラフェンやグラファイトを含む物質からなる群から選択される一つ又はそれ以上が混合された物質であることを特徴とする請求項4に記載の正極活物質。
- 前記正極活物質は、リチウムコバルト酸化物、リチウムニッケル酸化物、リチウムマンガン酸化物、リチウムコバルト−ニッケル酸化物、リチウムコバルト−マンガン酸化物、リチウムマンガン−ニッケル酸化物、リチウムコバルト−ニッケル−マンガン酸化物、及びこれらにAl、Mg、Ni、Co、Fe、Cr、V、Ti、Cu、B、Ca、Zn、Zr、Nb、Mo、Sr、Sb、W及びBiからなる群から選択される1種以上の他元素(等)が置換又はドーピングされた酸化物からなる群から選択される1種以上のリチウム含有金属酸化物がさらに含まれたことを特徴とする請求項1から6の何れか1項に記載の正極活物質。
- 前記リチウム含有金属酸化物は、前記正極活物質100重量部に対し50重量部以内に含まれることを特徴とする請求項7に記載の正極活物質。
- 請求項1から8の何れか1項に記載の正極活物質を含む正極。
- 請求項9に記載の正極を含むリチウム二次電池。
- 請求項10に記載のリチウム二次電池を2以上含む電池モジュール。
- 前記電池モジュールは、パワーツール(power tool);電気車(Electric Vehicle、EV)、ハイブリッド電気車(Hybrid Electric Vehicle、HEV)及びプラグインハイブリッド電気車(Plug−in Hybrid Electric Vehicle、PHEV)を含む電気車;イーバイク(E−bike)、イースクーター(E−scooter)を含む電気二輪車;電気ゴルフカート(Electric golf cart);電気トラック;電気商用車又は電力貯蔵用システムのうち何れか一つの電源に利用されることを特徴とする請求項11に記載の電池モジュール。
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KR1020110094797A KR101444510B1 (ko) | 2011-09-20 | 2011-09-20 | 고용량의 양극활물질 및 이를 포함하는 리튬 이차전지 |
PCT/KR2012/007541 WO2013042957A1 (ko) | 2011-09-20 | 2012-09-20 | 고용량의 양극활물질 및 이를 포함하는 리튬이차전지 |
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JP2015118901A (ja) * | 2013-11-12 | 2015-06-25 | 信越化学工業株式会社 | リチウムイオン二次電池用正極活物質及びその製造方法並びにリチウムイオン二次電池 |
DE102015217745A1 (de) | 2015-09-16 | 2017-03-16 | Robert Bosch Gmbh | Aktivmaterial für eine positive Elektrode einer Batteriezelle, positive Elektrode und Batteriezelle |
CN106410188A (zh) * | 2016-12-06 | 2017-02-15 | 先进储能材料国家工程研究中心有限责任公司 | 锂离子电池正极浆料及其制备方法 |
CN110036509B (zh) * | 2017-06-27 | 2022-04-26 | 株式会社Lg新能源 | 锂二次电池用正极和包含其的锂二次电池 |
KR20190062209A (ko) | 2017-11-27 | 2019-06-05 | 주식회사 엘지화학 | 양극 첨가제, 이의 제조 방법, 이를 포함하는 양극 및 리튬 이차 전지 |
US11876158B2 (en) * | 2019-06-25 | 2024-01-16 | Enevate Corporation | Method and system for an ultra-high voltage cobalt-free cathode for alkali ion batteries |
CN111600013A (zh) * | 2020-05-12 | 2020-08-28 | 武汉工程大学 | 锰源前驱体和锰基锂电池正极材料及其制备方法 |
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JP2631998B2 (ja) * | 1988-05-17 | 1997-07-16 | 三洋電機株式会社 | 非水系二次電池用正極の製造法 |
JP2692932B2 (ja) * | 1989-02-20 | 1997-12-17 | 三洋電機株式会社 | 非水系二次電池 |
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EP2541654B1 (en) * | 2010-02-24 | 2014-11-19 | LG Chem, Ltd. | High-capacity positive electrode active material and lithium secondary battery comprising same |
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US9698413B2 (en) | 2017-07-04 |
US20140147727A1 (en) | 2014-05-29 |
KR101444510B1 (ko) | 2014-09-25 |
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