CN110783535A - 用于具有高容量的锂二次电池的正极添加剂 - Google Patents
用于具有高容量的锂二次电池的正极添加剂 Download PDFInfo
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- CN110783535A CN110783535A CN201910751832.XA CN201910751832A CN110783535A CN 110783535 A CN110783535 A CN 110783535A CN 201910751832 A CN201910751832 A CN 201910751832A CN 110783535 A CN110783535 A CN 110783535A
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- lithium secondary
- secondary battery
- carbon
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Abstract
本发明涉及用于具有高容量的锂二次电池的正极添加剂,以及包含该正极添加剂的锂二次电池,其在正极活性材料中含有Li2NiO2以改善使用选自Si、SiC、SiOx(0<x<2)、Sn、SnO2、Sb、Ge及它们的混合物中的负极活性材料时容量保持率在初始循环期间降低的现象。根据本发明的锂二次电池可显著改善容量保持率在初始循环期间的降低,并伴随着电池容量的增加。
Description
本申请是申请日为2014年09月03日的PCT国际申请PCT/KR2014/008264的分案申请,原申请为发明专利申请,进入中国国家阶段的申请号为201480002937.0,名称为“用于具有高容量的锂二次电池的正极添加剂”。
技术领域
本申请要求2013年9月5日在韩国提交的韩国专利申请案第10-2013-0106746号及2014年9月3日在韩国提交的韩国专利申请案第10-2014-0116894号的优先权,其通过参照方式并入本文。
本公开内容涉及要用于具有高容量的锂二次电池、更具体地为正极含有Li2NiO2的锂二次电池的正极的添加剂,以便改善当使用非碳系材料作为负极活性材料时容量保持率在初始循环期间降低的现象。
背景技术
近来能量储存技术已渐受瞩目。由于能量储存技术的应用领域已延伸至移动装置如手机、摄录像机与笔记本电脑,以及电动车辆的能量,对具有高能量密度的作为电源的电池的需求已逐渐增加。锂二次电池被认为是能满足此需求的最佳电池,其研究早已积极展开。
目前使用的二次电池中,1990年代早期研发的锂二次电池包含由能嵌入或脱嵌锂离子的碳材料制成的负极、由含锂的氧化物制成的正极、以及使适量锂盐溶于混合有机溶剂所得的非水性电解质溶液。
已使用能嵌入及脱嵌锂离子的各种碳系材料,包括人造石墨、天然石墨及硬碳,作为锂二次电池的负极活性材料。这些碳系材料中,石墨相对于锂具有-0.2V的低放电电压,因而使用石墨作为负极活性材料的电池具有3.6V的高放电电压。因此,这种石墨活性材料由于可在锂电池能量密度方面提供优点且具有良好的可逆性以确保锂二次电池的长寿命,因而其已经被最广泛地运用。然而,制备电极时石墨活性材料具有提供低容量的低密度(理论密度2.2g/cc),其在电极的每单位体积能量密度上是不利的,且其在高放电电压下易于与所使用的有机电解质反应,这可能因电池的不正常操作或过度充电等而导致着火或爆炸。
近来由于锂二次电池的用途扩大,因此对在如高温和/或低温的严苛条件下能维持良好性能且即使在高电压下也能稳定充电的锂二次电池有逐渐增加的需求。
同时,可能通过将碳系负极活性材料改成非碳系材料如硅氧化物以改良锂二次电池的容量特性。然而,包括硅氧化物的一些负极材料是不可逆的。因此,一些负极材料在第一次充电时嵌入锂离子但在之后的放电中无法脱嵌约20%的锂离子。因此,在第一次充电循环后,第一次充电中所使用的正极活性材料的约20%无法参与接下来的充电及放电,而最终使锂二次电池的效率降低。
为解决此问题,已尝试制备由碳系材料及硅系材料组成的纳米粒子复合物并将其用作负极活性材料。通过将碳系材料用作电导体,此纳米粒子复合物能相当地改良电池的容量保持率。然而,碳系材料须以超过50重量%的量而过量存在于纳米粒子复合物中以对电池提供较佳的容量保持,这降低了电池容量。另外,尽管碳系材料如上所述过量存在,但仍存在容量在第50次循环或之后会进一步降低而小于1500mAh/g的问题。
因此,需要开发当使用非碳系材料作为负极材料时能改善初始循环期间容量保持率的降低的锂二次电池。
发明内容
技术问题
设计本公开内容以解决上述问题,因此本公开内容的目的是提供当使用非碳系材料作为负极材料时能改善初始循环期间容量保持率的降低的锂二次电池。
为此,本公开内容提供锂二次电池,其可在第一次充电时在负极供应充足的锂以及补充循环期间在负极消耗的锂。
技术方案
为了实现上述目的,根据本公开内容的一个方面,提供了锂二次电池,其包括正极、负极和隔膜,其中,正极活性材料含有化合物Li2NiO2,负极活性材料含有选自如下任一种:Si、SiC、SiOx(0<x<2)、Sn、SnO2、Sb、Ge及它们的混合物。
正极活性材料可含有1重量%~10重量%的量的化合物Li2NiO2。
负极活性材料可含有1重量%~30重量%的量的选自如下的任一种:Si、SiC、SiOx(0<x<2)、Sn、SnO2、Sb、Ge及它们的混合物。
除了Li2NiO2,正极活性材料可进一步含有选自如下的任一种:LixCoO2(0.5<x<1.3)、LixNiO2(0.5<x<1.3)、LixMnO2(0.5<x<1.3)、LixMn2O4(0.5<x<1.3)、Lix(NiaCobMnc)O2(0.5<x<1.3、0<a<1、0<b<1、0<c<1、a+b+c=1)、LixNi1-yCoyO2(0.5<x<1.3、0<y<1)、LixCo1- yMnyO2(0.5<x<1.3、0≤y<1)、LixNi1-yMnyO2(0.5<x<1.3、O≤y<1)、Lix(NiaCobMnc)O4(0.5<x<1.3、0<a<2、0<b<2、0<c<2、a+b+c=2)、LixMn2-zNizO4(0.5<x<1.3、0<z<2)、LixMn2-zCozO4(0.5<x<1.3、0<z<2)、LixCoPO4(0.5<x<1.3)、LixFePO4(0.5<x<1.3)及它们的混合物。
除了选自Si、SiC、SiOx(0<x<2)、Sn、SnO2、Sb、Ge及它们的混合物中的任一种,负极活性材料可进一步含有选自如下的任一种:软碳、硬碳、天然石墨、结晶石墨(Kishgraphite)、热解炭、中间相沥青基碳纤维、中间相碳微球、中间相沥青、石油衍生焦炭、煤焦油沥青衍生焦炭及它们的混合物。
该锂二次电池在50次循环后的容量保持率可为90%以上。
有益效果
根据本公开内容的锂二次电池可显着改善容量保持率在初始循环期间的降低,从而显示出优异的高容量保持率。
附图说明
伴随的附图与前述公开内容一起阐释本公开内容的优选实施方式,用于提供对本公开内容的技术主旨的进一步了解。然而,本公开内容不应理解为受限于所述附图。
图1显示本公开内容的实施例1及比较例1中制备的电池(单电池)的容量保持率(%)随循环的图。
具体实施方式
后文中将详细说明本公开内容。在说明之前,应了解说明书及所附权利要求中所使用的术语不应理解为受限于一般的及字典中的意义,而是应基于本案发明人可为了最佳解释而适当定义术语的原则,依据相应于本公开内容的技术方面的意义与概念而解释。
本公开内容的正极包含由Li2NiO2表示的锂镍氧化物。Li2NiO2可在第一次充电中以1摩尔以上的量脱嵌锂离子,且然后可在第一次放电和之后以1摩尔以下的量嵌入及脱嵌锂离子。因此,正极中添加的Li2NiO2可提供足以补偿负极的不可逆性的锂离子,因而可补偿第一次放电中负极的极大的不可逆性。
正极活性材料中Li2NiO2的含量可为1重量%~10重量%。当Li2NiO2的量满足此范围时,充电及放电过程可在没有电池损伤的情况下进行且电池的循环特性可能不会劣化。更具体地,锂二次电池在第50次循环或之后的容量保持率可为90%以上。若Li2NiO2的用量超过该上限,则Li2NiO2会在第一次充电后相变成LiNiO2,因而使得电池安全性不利地劣化。通常,LiNiO2的稳定性低于LiCoO2的稳定性。
可与锂镍氧化物一起使用的其他正极活性材料并无特别限制,只要其为本领域中常规使用的即可。可用的正极活性材料的非限制性实例可包括含锂的过渡金属氧化物,例如,LixCoO2(0.5<x<1.3)、LixNiO2(0.5<x<1.3)、LixMnO2(0.5<x<1.3)、LixMn2O4(0.5<x<1.3)、Lix(NiaCobMnc)O2(0.5<x<1.3,0<a<1,0<b<1,0<c<1,a+b+c=1)、LixNi1-yCoyO2(0.5<x<1.3,0<y<1)、LixCo1-yMnyO2(0.5<x<1.3,0≤y<1)、LixNi1-yMnyO2(0.5<x<1.3,0≤y<1)、Lix(NiaCobMnc)O4(0.5<x<1.3,0<a<2,0<b<2,0<c<2,a+b+c=2)、LixMn2-zNizO4(0.5<x<1.3,0<z<2)、LixMn2-zCozO4(0.5<x<1.3,0<z<2)、LixCoPO4(0.5<x<1.3)、LixFePO4(0.5<x<1.3)及它们的混合物。这些含锂的过渡金属氧化物可涂覆有金属如铝(Al)或金属氧化物。并且,除了含锂的过渡金属氧化物,也可使用含锂的过渡金属的硫化物、硒化物及卤化物。
本公开内容的负极包含选自如下的负极活性材料:Si、SiC、SiOx(0<x<2)、Sn、SnO2、Sb、Ge及它们的混合物。
选自Si、SiC、SiOx(0<x<2)、Sn、SnO2、Sb、Ge及它们的混合物中的负极活性材料可与本领域中常规使用的其他负极活性材料一起使用,且在所有负极活性材料中含有的量可为1重量%~30重量%。
通常,可考虑设计因子(design factor)以制备电池,其包括正极与负极间的电化学平衡(electrochemical balance)。即,即使设计电池以纳入具高容量的正极与具高容量的负极,也并不表示此电池必然具有高容量。就此方面,为了制备具有高容量的电池,选自Si、SiC、SiOx(0<x<2)、Sn、SnO2、Sb、Ge及它们的混合物中的负极活性材料在所有负极活性材料中的含量优选为1重量%~15重量%。若负极活性材料的用量超过该上限,即使将Li2NiO2用于正极活性材料,仍难以补偿锂离子的不可逆性。若负极活性材料的用量少于该下限,提高容量的效果便不足。
本领域中常规使用的其他负极活性材料的非限制性实例可包括能嵌入及脱嵌锂离子的碳系材料、金属锂等等。碳系材料可为低结晶性碳或高结晶性碳。低结晶性碳的代表性实例包括软碳及硬碳,高结晶性碳的代表性实例包括天然石墨、结晶石墨(Kishgraphite)、热解炭、中间相沥青基碳纤维、中间相碳微球、中间相沥青,及高温烧结碳如石油或煤沥青(coal tar pitch)衍生焦炭。
正极和/或负极可包含粘合剂,可使用包括聚偏二氟乙烯-六氟丙烯共聚物(PVDF-co-HFP)、聚偏二氟乙烯、聚丙烯腈及聚甲基丙烯酸甲酯的各种粘合剂聚合物作为粘合剂。
通过将非水性电解质溶液引入由正极、负极和插置于其间的隔膜所组成的电极组而制备上述本公开内容的锂二次电池。作为构成电极组的正极、负极和隔膜,可使用常规用于制备锂二次电池的正极、负极和隔膜。
再者,隔膜可由惯常为单独使用或为常规隔膜层压形式的多孔聚合物膜获得,例如,由聚烯烃系聚合物如乙烯均聚物、丙烯均聚物、乙烯/丁烯共聚物、乙烯/己烯共聚物以及乙烯/甲基丙烯酸酯共聚物所制成的多孔聚合物膜。并且,亦可使用常规多孔无纺布例如由高熔点玻璃纤维或聚对酞酸乙二酯纤维所制成的无纺布作为隔膜,但不限于此。
本公开内容所使用的非水性电解质溶液包括锂盐作为电解质盐。锂盐可为任何常用于锂二次电池的电解质溶液者。例如,锂盐的阴离子可为选自如下的任一种:F-、Cl-、Br-、I-、NO3 -、N(CN)2 -、BF4 -、ClO4 -、PF6 -、(CF3)2PF4 -、(CF3)3PF3 -、(CF3)4PF2 -、(CF3)5PF-、(CF3)6P-、CF3SO3 -、CF3CF2SO3 -、(CF3SO2)2N-、(FSO2)2N-、CF3CF2(CF3)2CO-、(CF3SO2)2CH-、(SF5)3C-、(CF3SO2)3C-、CF3(CF2)7SO3 -、CF3CO2 -、CH3CO2 -、SCN-及(CF3CF2SO2)2N-。
本公开内容所使用的非水性电解质溶液包括常规用于锂二次电池的电解质溶液的有机溶剂,例如,醚类、酯类、酰胺类、直链碳酸酯、环状碳酸酯、及它们的混合物。
其中,典型地使用碳酸酯化合物如直链碳酸酯、环状碳酸酯或其混合物。环状碳酸酯的具体实例可包括碳酸亚乙酯(EC)、碳酸亚丙酯(PC)、1,2-碳酸亚丁酯、2,3-碳酸亚丁酯、1,2-碳酸亚戊酯、2,3-碳酸亚戊酯、碳酸亚乙烯酯、其卤化物及它们的混合物。直链碳酸酯的具体实例可包括碳酸二甲酯(DMC)、碳酸二乙酯(DEC)、碳酸二丙酯、碳酸甲乙酯(EMC)、碳酸甲丙酯、碳酸乙丙酯及它们的混合物,但不限于此。
特别地,上述碳酸酯系有机溶剂中,优选使用环状碳酸酯例如碳酸亚乙酯及碳酸亚丙酯,因为其具有高黏度及高介电常数而更易在电解质中解离(dissociate)锂盐。更优选地,这种环状碳酸酯可与具有低黏度及低介电常数的直链碳酸酯如碳酸二甲酯和碳酸二乙酯以适当比例混合以提供具有高导电性的电解质溶液。
再者,可用作有机溶剂的醚选自如下的任一种:二甲醚、二乙醚、二丙醚、甲基乙基醚、甲基丙基醚、乙基丙基醚及它们的混合物,但不限于此。
此外,可用作有机溶剂的酯选自如下的任一种:乙酸甲酯、乙酸乙酯、乙酸丙酯、丙酸甲酯、丙酸乙酯、γ-丁内酯、γ-戊内酯、γ-己内酯、σ-戊内酯、ε-己内酯及它们的混合物,但不限于此。
此外,本公开内容的电化学装置对其形状并无限制。例如,电化学装置的形状可为筒状例如罐、棱柱、袋状或硬币。
本发明的实施方式
为了更好地理解,以下将详述本公开内容的优选实例。然而本公开内容的实例可以各种方式修饰且不应解释为限制本发明的范围。本公开内容的实例仅用于使本领域的普通技术人员更好地理解本发明。
实施例1
提供由Al-掺杂的LiNiCoO2(LiNi0.8Co0.15Al0.05O2)及Li2NiO2以95:5的重量比组成的正极活性材料。接着,将正极活性材料、作为粘合剂的聚偏二氟乙烯、以及作为导电材料的碳以8:1:1的重量比混合,将混合物分散于N-甲基-吡咯烷酮以获得正极浆液。将该浆液涂覆于铝制成的集电器上,接着进行干燥及压制,以制备正极。
同样,提供由石墨及SiO以9:1的重量比组成的负极活性材料。接着,将负极活性材料、苯乙烯丁二烯橡胶(SBR)、及羧甲基纤维素(CMC)以90:5:5的重量比混合,将混合物分散于水中以获得负极浆液。将该浆液涂覆于铜制成的集电器上,接着进行干燥及压制,以制备负极。
使用包含体积比为1:2的碳酸亚乙酯及碳酸甲乙酯的1M LiPF6溶液作为电解质溶液。
然后,通过常规方法将如上所得的正极和负极与聚乙烯(PE)隔膜组合以制备硬币型全电池,其中引入电解质溶液。由此,最终制得硬币型全电池。
比较例1
重复实施例1的程序以制备硬币型全电池,不同之处在于不使用Li2NiO2。
试验实施例:测量每循环的容量保持率
在0.5C充电及1C放电的条件下,对实施例1及比较例1中制备的硬币型全电池进行充放电循环的试验,其结果示于图1。
如图1所示,与比较例1的锂二次电池相比,实施例1的锂二次电池展现并维持对初始循环期间的容量保持率(%)降低现象的显着改善。
Claims (10)
1.一种锂二次电池,其包含正极、负极和隔膜,并且是筒状电池,其中:
所述正极包含正极活性材料,所述正极活性材料含有1重量%~10重量%的化合物Li2NiO2,以及
所述负极包含负极活性材料,所述负极活性材料由如下材料构成:
1重量%~15重量%的SiO,以及
碳系材料,
其中,所述锂二次电池在50个循环后的容量保持率为90%以上,并且循环测试在0.5C充电和1C放电的条件下进行。
2.如权利要求1所述的锂二次电池,其中,SiO在所述负极活性材料中的含量为10重量%~15重量%。
3.如权利要求1所述的锂二次电池,其中,所述正极活性材料还含有选自如下材料中的任一种含锂的过渡金属氧化物:
LixCoO2,其中0.5<x<1.3;
LixNiO2,其中0.5<x<1.3;
LixMnO2,其中0.5<x<1.3;
LixMn2O4,其中0.5<x<1.3;
Lix(NiaCobMnc)O2,其中0.5<x<1.3,0<a<1,0<b<1,0<c<1,a+b+c=1;
LixNi1-yCoyO2,其中0.5<x<1.3,0<y<1;
LixCo1-yMnyO2,其中0.5<x<1.3,0≤y<1;
LixNi1-yMnyO2,其中0.5<x<1.3,0≤y<1;
Lix(NiaCobMnc)O4,其中0.5<x<1.3,0<a<2,0<b<2,0<c<2,a+b+c=2;
LixMn2-zNizO4,其中0.5<x<1.3,0<z<2;
LixMn2-zCozO4,其中0.5<x<1.3,0<z<2;
LixCoPO4,其中0.5<x<1.3;
LixFePO4,其中0.5<x<1.3;以及
它们的混合物。
4.如权利要求3所述的锂二次电池,其中,所述含锂的过渡金属氧化物涂覆有金属或金属氧化物。
5.如权利要求4所述的锂二次电池,其中,所述含锂的过渡金属氧化物涂覆有铝(Al)金属。
6.如权利要求1所述的锂二次电池,其中,所述碳系材料为选自如下材料中的任一种:软碳、硬碳、天然石墨、结晶石墨、热解炭、中间相沥青基碳纤维、中间相碳微球、中间相沥青、石油衍生焦炭、煤焦油沥青衍生焦炭及它们的混合物。
7.如权利要求6所述的锂二次电池,其中,所述碳系材料为天然石墨或结晶石墨。
8.如权利要求1所述的锂二次电池,其中,所述锂二次电池具有罐的形状。
9.如权利要求1所述的锂二次电池,其中,所述正极活性材料由LiNi0.8Co0.15Al0.05O2和Li2NiO2组成,并且所述负极活性材料由石墨和SiO组成。
10.如权利要求1所述的锂二次电池,其中,所述正极活性材料由重量比为95:5的LiNi0.8Co0.15Al0.05O2和Li2NiO2组成,并且所述负极活性材料由重量比为9:1的石墨和SiO组成。
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