CN101322266A - 基于具有高硅含量的非晶态合金的电极组合物 - Google Patents
基于具有高硅含量的非晶态合金的电极组合物 Download PDFInfo
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- 239000000203 mixture Substances 0.000 title claims abstract description 34
- 229910000808 amorphous metal alloy Inorganic materials 0.000 title claims abstract description 12
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 title description 4
- 229910052710 silicon Inorganic materials 0.000 title description 4
- 239000010703 silicon Substances 0.000 title description 4
- 229910001416 lithium ion Inorganic materials 0.000 claims abstract description 21
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims abstract description 20
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 16
- 229910052751 metal Inorganic materials 0.000 claims abstract description 16
- 239000002184 metal Substances 0.000 claims abstract description 15
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 11
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims abstract description 9
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims abstract description 9
- 229910052726 zirconium Inorganic materials 0.000 claims abstract description 9
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims abstract description 8
- 239000010949 copper Substances 0.000 claims abstract description 8
- 229910052719 titanium Inorganic materials 0.000 claims abstract description 8
- 239000010936 titanium Substances 0.000 claims abstract description 8
- 229910052802 copper Inorganic materials 0.000 claims abstract description 7
- 229910052742 iron Inorganic materials 0.000 claims abstract description 7
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- 239000011651 chromium Substances 0.000 claims abstract description 6
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- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims abstract description 5
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims abstract description 5
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- 239000010941 cobalt Substances 0.000 claims abstract description 5
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- 150000002739 metals Chemical class 0.000 claims abstract description 5
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- 239000010955 niobium Substances 0.000 claims abstract description 5
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims abstract description 5
- 229910052715 tantalum Inorganic materials 0.000 claims abstract description 5
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims abstract description 5
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims abstract description 5
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- 239000010937 tungsten Substances 0.000 claims abstract description 5
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- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims abstract description 5
- 229910052727 yttrium Inorganic materials 0.000 claims abstract description 5
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 claims abstract description 5
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- 229910052744 lithium Inorganic materials 0.000 description 6
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 4
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- -1 poly(ethylene oxide) Polymers 0.000 description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 3
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- 239000004411 aluminium Substances 0.000 description 3
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- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
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- UONOETXJSWQNOL-UHFFFAOYSA-N tungsten carbide Chemical compound [W+]#[C-] UONOETXJSWQNOL-UHFFFAOYSA-N 0.000 description 2
- XESSXNRXAYFGSO-UHFFFAOYSA-N B([O-])([O-])[O-].[Li+].C(C(=O)O)(=O)O.[Li+].[Li+] Chemical compound B([O-])([O-])[O-].[Li+].C(C(=O)O)(=O)O.[Li+].[Li+] XESSXNRXAYFGSO-UHFFFAOYSA-N 0.000 description 1
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- 229910005516 Si55Al29.3Fe15.7 Inorganic materials 0.000 description 1
- 229910005722 Si62Al18Fe16Zr4 Inorganic materials 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
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- 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
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- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 1
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Abstract
一种用于锂离子电池的电极组合物,包括如式SixMyAlz所示的非晶态合金,其中x、y和z代表原子百分比值,且(a)x+y+z=100,(b)x≥55,(c)y<22,(d)z>0,和(e)M为选自锰、钼、铌、钨、钽、铁、铜、钛、钒、铬、镍、钴、锆、钇及其组合的一种或多种金属。
Description
技术领域
本发明涉及适用于锂离子电池的电极组合物。
背景技术
已经建议将含硅、铝及各种过渡金属元素的熔体旋铸合金用于锂离子电池的电极。这些合金具有能延长循环寿命并因此提高整体电池性能的非晶态微结构。不过,随着硅含量的增加,产生具有非晶态微结构的组合物越来越难。这一问题的一种建议解决方案需要使用相对较多数量(按原子百分比)和/或种类的过渡金属元素与硅和铝组合。不过,这一建议的解决方案存在着使材料电化学失活的风险。
发明内容
这里描述一种用于锂离子电池的包括非晶态合金的电极组合物,所述非晶态合金如式SixMyAlz所示,其中x、y和z代表原子百分比值,且(a)x+y+z=100,(b)x≥55,(c)y<22,(d)z>0,(e)M为选自锰、钼、铌、钨、钽、铁、铜、钛、钒、铬、镍、钴、锆、钇及其组合的一种或多种金属。非晶态合金可以为单相的形式。“非晶态合金”是一种缺乏长程原子秩序并且其X射线衍射图缺乏尖锐、明确界定峰的合金。
可以选择x值,使x≥60。可以选择y值,使y≤20。
M优选代表不超过两种的金属。特别有用的金属的具体例子包括铁、钛、锆及其组合。
可以将该电极组合物用于锂离子电池的阳极,所述锂离子电池还包括阴极和电解质。电解质可以包括氟代碳酸亚乙酯。优选的是,阳极的形式为包括电极组合物与粘结剂(如聚酰亚胺)和导电稀释剂(如炭黑)组合的复合体。
该电极组合物在最少化金属M含量的同时显示出高容量和良好的循环寿命。最少化金属M的能力产生适合作为锂离子电池电极的电化学活性材料。
下文的附图和描述中给出了本发明的一个或多个实施例的详情。从描述和附图以及从权利要求中可以显而易见本发明的其它特征、目的及优点。
附图说明
图1为实例1中描述的熔体旋铸合金的X射线衍射外形图。
图2所示为结合了实例1中描述的熔体旋铸合金的电化学电池的循环性能。
图3为实例2中描述的熔体旋铸合金的X射线衍射外形图。
图4所示为结合了实例2中描述的熔体旋铸合金的电化学电池的循环性能。
具体实施方式
所描述的电极组合物特别适合用于锂离子电池的阳极。该电极组合物的特征为如式SixMyAlz所示的非晶态合金,其中x、y和z代表原子百分比值,且(a)x+y+z=100,(b)x≥55,(c)y<22,(d)z>0,(e)M为选自锰、钼、铌、钨、钽、铁、铜、钛、钒、铬、镍、钴、锆、钇及其组合的一种或多种金属。特别适用的组合物为其中x≥60、y≤20并且M代表不超过两种的金属的那些。
优选通过激冷块熔体旋铸法制备电极组合物。这种方法例如在“Amorphous Metallic Alloys”(F.E.Luborsky编辑,第2章,Butterworth & Co.,Ltd.(London),1983)一书中有一般性描述。按照这一方法,在射频场中使含硅和金属元素的锭熔化,然后通过喷嘴将其喷射到旋转的金属轮(例如,铜或铜合金轮)的表面上。由于轮的表面温度大大低于熔体温度,与轮表面的接触使熔体骤冷。骤冷可防止形成对电极性能不利的大晶粒。通过采用大于40m/s的轮表面速度和直径小于0.5mm的喷嘴可以制备出非晶态组合物。
该电极组合物特别适合用于锂离子电池的阳极。阳极优选为复合体,其中电极组合物与粘结剂和导电稀释剂结合。合适粘结剂的例子包括聚酰亚胺和聚偏二氟乙烯。合适的导电稀释剂的例子包括炭黑。
为制备电池,需将阳极与电解质和阴极(对电极)结合。电解质的形式可以为液体、固体或凝胶。固体电解质的例子包括聚合物电解质,例如聚环氧乙烷、含氟聚合物和共聚物(例如,聚四氟乙烯)及其组合。液体电解质的例子包括碳酸亚乙酯、碳酸二乙酯、碳酸亚丙酯、氟代碳酸亚乙酯(FEC)及其组合。向电解质提供锂电解质盐。合适盐的例子包括LiPF6、LiBF4、双(乙二酸)硼酸锂、LiN(CF3SO2)2、LiN(C2F5SO2)2、LiAsF6、LiC(CF3SO2)3和LiClO4。合适的阴极组合物的例子包括LiCoO2、LiCo0.2Ni0.8O2和LiMn2O4。另外的例子包括在下列文献中描述的阴极组合物:(1)Lu等人,美国专利申请公开2004/0121234;(2)Dahn等人,美国专利申请公开2003/0108793;(3)Eberman等人,美国专利申请公开2005/0112054;(4)Dahn等人,美国专利申请公开2004/0179993;(5)Lu等人,美国专利6,964,828;(6)Lu等人,美国专利7,078,128;(7)Obrovac等人,美国专利6,680,145;和(8)Dahn等人,美国专利5,900,385。
实例
实例1
在称量皿中称量出13.93g铝、49.960g硅、25.637g铁和10.469g锆(均为99.8%或更高的纯度),然后置于ARC炉中(购自AdvancedVacuum Systems,Ayer,MA)。在Ar气氛中使混合物熔化,生成具有Si62Al18Fe16Zr4组成的锭,其中所有的量均为原子百分比。
使用金刚石刃湿锯将锭切割成带,从而形成20g用于熔体旋铸的带。熔体旋铸装置由特征为圆柱形石英玻璃坩埚的真空室构成。坩埚具有16mm的内径、140mm长度和0.28mm的喷嘴。将坩埚置于厚度10mm、直径203mm的旋转冷却轮(Ni-Si-Cr-Cu C18000合金,含0.45重量%Cr、2.4重量%Ni、0.6重量%Si,余为铜)之上。运转之前使用打磨膏(购自3M,St.Paul,MN的IMPERIALMICROFINISHING)对轮的边缘表面抛光,接着用矿物油进行擦拭,留下一层薄膜。
为进行熔体旋铸,将20g锭带放入到坩埚中,此后将系统抽空至80mTorr,然后充He气至200mTorr的压力。采用RF感应熔化锭。当温度达到1275℃时,对熔融合金的表面施加400mTorr的He压力,以通过喷嘴将合金挤出到以5,031rpm(53m/s)旋转的转动轮上。制备出宽1mm、厚10微米的条带。使用配备了铜靶X射线管及衍射光束单色器的Siemens Model Kristalloflex 805 D500衍射仪收集典型带子的X射线衍射图。结果示于图1中。缺少尖峰表明组合物是非晶态的。
将1.70g熔体旋铸的条、150mg的Super P碳(导电稀释剂)、0.750g聚酰亚胺涂布溶液(PYRALIN PI2555,在N-甲基吡咯烷酮(NMP)中浓度20%,购自HD Microsystems,Parlink NJ)和3.75g的NMP加入到包含10mm直径和10.3mm直径的碳化钨球的40ml碳化钨碾磨容器中。将容器放入到行星式碾磨机(PULVERISETTE 7,购自Fritsch GmbH,Idon-Oberstein,Germany)中,在设置为8的条件下碾磨一小时。
碾磨以后将溶液转移至槽口涂覆棒,在15微米厚的铜箔上涂覆出25mm宽、125微米厚的带。涂层在150℃下真空固化2.5小时形成电极。然后通过使电极与金属锂阳极、两层平片聚丙烯膜隔板(CELGARD 2400,购自Celgard Inc.,Charlotte,NC)和作为电解质的在碳酸亚乙酯与碳酸二乙酯的1∶2混合物中的1M LiPF6结合,构造2225硬币式电池。使用电池循环器(MACCOR,4000型,购自Maccor,Tulsa,OK)对电池进行循环试验,第一循环为0.9V与0.005V之间恒流0.125mA,所有其余的循环为0.9V与0.005V之间恒流0.5mA。结果示于图2。如图所示,电池显示出良好的循环性能。
实例2
按照实例1中描述的步骤制备熔体旋铸锭。合金的成分为Si55Al29.3Fe15.7,其中所有的量均为原子百分比。图3所示的X射线衍射结果表明缺少尖峰,说明组合物是非晶态的。
使用高速剪切混合器将0.8g熔体旋铸条、4.16g的Super P碳(导电稀释剂)的3重量%分散体、3重量%聚偏二氟乙烯、94%的N-甲基吡咯烷酮(NMP)和1g NMP在一起混合15分钟。
混合以后把浆料转移至槽口涂覆棒,在15微米厚的铜箔上涂覆出25mm宽、125微米厚的带。涂层在150℃下真空固化2.5小时形成电极。然后,通过使电极与金属锂阳极、作为隔板的两层CELGARD 2400和作为电解质的在碳酸亚乙酯与碳酸二乙酯的1∶2混合物中的1M LiPF6结合,构造2225硬币式电池。使用MACCOR循环器按照表1中所述的方案对电池进行循环试验。结果示于图4。如图所示,电池显示出良好的循环性能。
表1
循环 | 电流 | 电位 | 涓流 |
锂化#1 | 70mA/g | 5mV | 7mA/g |
脱锂#1 | 70mA/g | 0.9V | 7mA/g |
锂化#2 | 70mA/g | 5mV | 14mA/g |
脱锂#2 | 70mA/g | 0.9V | 无 |
锂化#3+ | 140mA/g | 5mV | 14mA/g |
脱锂#3+ | 140mA/g | 0.9V | 无 |
实例3和4
按照实例1中描述的步骤制备具有表2中给出的成分的样品。X射线衍射数据显示在这两个例子中均缺少尖峰,表明组合物是非晶态的。采用每个组合物制备的电化学电池的循环容量也在表2中给出。结果表明每个电池都显示出良好的循环性能。
表2
已经描述了本发明的多个实施例。不过应当理解的是,在不偏离本发明的精神和范围的情况下可以作出各种修改。因此,其它的实施例是在以下的权利要求范围之内的。
Claims (18)
1.一种用于锂离子电池的电极组合物,包括如式SixMyAlz所示的非晶态合金,其中x、y和z代表原子百分比值,并且:
(a)x+y+z=100;
(b)x≥55;
(c)y<22;
(d)z>0;和
(e)M为选自由锰、钼、铌、钨、钽、铁、铜、钛、钒、铬、镍、钴、锆、钇及其组合组成的组中的一种或多种金属。
2.根据权利要求1所述的电极组合物,其中x≥60。
3.根据权利要求1所述的电极组合物,其中y≤20。
4.根据权利要求1所述的电极组合物,其中M为不超过两种的金属。
5.根据权利要求1所述的电极组合物,其中M选自铁、钛、锆及其组合。
6.根据权利要求1所述的电极组合物,其中x≥60,y≤20,M为不超过两种的金属。
7.根据权利要求1所述的电极组合物,其中所述非晶态合金的形式为单相。
8.一种锂离子电池,包括:
(a)阳极;
(b)阴极;和
(c)电解质,
其中所述阳极包含如式SixMyAlz所示的非晶态合金,其中x、y和z代表原子百分比值,并且:
(i)x+y+z=100;
(ii)x≥55;
(iii)y<22;
(iv)z>0;和
(v)M为选自由锰、钼、铌、钨、钽、铁、铜、钛、钒、铬、镍、钴、锆、钇及其组合组成的组中的一种或多种金属。
9.根据权利要求8所述的锂离子电池,其中x≥60。
10.根据权利要求8所述的锂离子电池,其中y≤20。
11.根据权利要求8所述的锂离子电池,其中M为不超过两种的金属。
12.根据权利要求8所述的锂离子电池,其中M选自铁、钛、锆及其组合。
13.根据权利要求8所述的锂离子电池,其中x≥60,y≤20,M为不超过两种的金属。
14.根据权利要求8所述的锂离子电池,其中所述非晶态合金的形式为单相。
15.根据权利要求8所述的锂离子电池,其中所述阳极进一步包含粘结剂和导电稀释剂。
16.根据权利要求15所述的锂离子电池,其中所述粘结剂包括聚酰亚胺。
17.根据权利要求15所述的锂离子电池,其中所述导电稀释剂包括炭黑。
18.根据权利要求8所述的锂离子电池,其中所述电解质包括氟代碳酸亚乙酯。
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US7972727B2 (en) | 2011-07-05 |
US20100167126A1 (en) | 2010-07-01 |
KR101354336B1 (ko) | 2014-01-22 |
TWI389374B (zh) | 2013-03-11 |
JP5302003B2 (ja) | 2013-10-02 |
US20070128517A1 (en) | 2007-06-07 |
EP1955393A1 (en) | 2008-08-13 |
US7732095B2 (en) | 2010-06-08 |
JP2009517850A (ja) | 2009-04-30 |
EP1955393A4 (en) | 2010-01-20 |
TW200746514A (en) | 2007-12-16 |
KR20080072025A (ko) | 2008-08-05 |
WO2007064531A1 (en) | 2007-06-07 |
EP1955393B1 (en) | 2014-08-27 |
CN101322266B (zh) | 2011-09-28 |
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