CN107078340B - 非水电解质二次电池 - Google Patents
非水电解质二次电池 Download PDFInfo
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- CN107078340B CN107078340B CN201580060633.4A CN201580060633A CN107078340B CN 107078340 B CN107078340 B CN 107078340B CN 201580060633 A CN201580060633 A CN 201580060633A CN 107078340 B CN107078340 B CN 107078340B
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- Prior art keywords
- nonaqueous electrolyte
- positive electrode
- active material
- negative electrode
- secondary battery
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- 229910052751 metal Inorganic materials 0.000 claims abstract description 19
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- 239000007773 negative electrode material Substances 0.000 claims description 27
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 4
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- PMGBATZKLCISOD-UHFFFAOYSA-N methyl 3,3,3-trifluoropropanoate Chemical compound COC(=O)CC(F)(F)F PMGBATZKLCISOD-UHFFFAOYSA-N 0.000 claims description 4
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Abstract
提供:具有高输入输出特性和良好的循环特性的非水电解质二次电池。作为实施方式一例的非水电解质二次电池具备:正极,其包含正极活性物质,所述正极活性物质具有层状结构,且以Co的含量相对于除Li之外的金属元素的总量为1mol%~20mol%的锂过渡金属氧化物作为主成分;负极,其包含含有Si的负极活性物质;和,非水电解质,其包含氟化链状羧酸酯。
Description
技术领域
本公开涉及一种非水电解质二次电池。
背景技术
专利文献1公开了,包含选自氟化链状醚、氟化环状酯和氟化链状碳酸酯中的至少1种氟系溶剂的非水电解质二次电池。专利文献1中记载了,通过使用上述非水电解质,从而在负极表面形成牢固的覆膜,因此电池的充放电效率和长期的充放电循环耐性提高。
现有技术文献
专利文献
专利文献1:日本专利第5359163号公报
发明内容
发明要解决的问题
然而,对于非水电解质二次电池,例如以产业用、***用的蓄电***用途为中心,重要的是具有高输入输出特性和良好的循环特性(高耐久性)。然而,包括专利文献1在内的现有技术中,难以兼顾高输入输出特性和良好的循环特性,谋求上述特性的进一步改善。
用于解决问题的方案
作为本公开的一个方案的非水电解质二次电池的特征在于,具备:正极,其包含正极活性物质,所述正极活性物质具有层状结构,且以钴(Co)的含量相对于除锂(Li)之外的金属元素的总量为1mol%以上且低于20mol%的锂过渡金属氧化物作为主成分;负极,其包含含有硅(Si)的负极活性物质;和,非水电解质,其包含氟化链状羧酸酯。
发明的效果
根据本公开的一个方案,可以提供具有高输入输出特性和良好的循环特性(高耐久性)的非水电解质二次电池。
附图说明
图1为作为实施方式一例的非水电解质二次电池的截面图。
具体实施方式
认为利用作为本公开的一个方案的非水电解质二次电池,在充电时从正极溶出的Co在含有Si的负极活性物质的表面与氟化链状羧酸酯特异性地发生反应,形成离子透过性优异的优质的覆膜。由此,可以兼顾高输入输出特性和高耐久性。上述作用效果是仅在具备Co的含量相对于除Li之外的金属元素的总量为1mol%以上且低于20mol%的锂过渡金属氧化物、含有Si的负极活性物质和氟化链状羧酸酯的情况下才会得到的特异性效果。作为本公开的一个方案的非水电解质二次电池适合于例如重复数千次的充放电循环的产业用、***用的蓄电***用途。
以下,对实施方式的一例进行详细说明。
实施方式的说明中参照的附图是示意性地记载,附图中描绘的构成要素的尺寸比率等有时与实际物体不同。具体的尺寸比率等应参照以下的说明来判断。
图1为作为实施方式一例的非水电解质二次电池10的截面图。
非水电解质二次电池10具备:正极11、负极12和非水电解质。在正极11与负极12之间设置分隔件13是适合的。非水电解质二次电池10例如具有如下结构:正极11和负极12介由分隔件13卷绕而成的卷绕型的电极体14与非水电解质收纳于电池壳体。需要说明的是,也可以应用正极和负极介由分隔件交替地层叠而成的层叠型的电极体等其他形态的电极体来代替卷绕型的电极体14。作为收纳电极体14和非水电解质的电池壳体,可以举出:圆筒形、方形、硬币形、纽扣形等金属制壳体、层压树脂片而形成的树脂制壳体(层压型电池)等。图1所示的例子中,由有底圆筒形状的壳体主体15和封口体16构成电池壳体。
非水电解质二次电池10具备分别配置于电极体14的上下的绝缘板17、18。图1所示的例子中,安装于正极11的正极引线19通过绝缘板17的贯通孔向封口体16侧延伸,安装于负极12的负极引线20通过绝缘板18的外侧向壳体主体15的底部侧延伸。例如,正极引线19利用焊接等与作为封口体16的底板的过滤器22的下面连接,作为与过滤器22电连接的封口体16的顶板的盖26成为正极端子。负极引线20利用焊接等与壳体主体15的底部内面连接,壳体主体15成为负极端子。本实施方式中,在封口体16上设有电流切断机构(CID)和气体排出机构(安全阀)。需要说明的是,在壳体主体15的底部也设置气体排出阀(未作图示)是适合的。
壳体主体15例如为有底圆筒形状的金属制容器。在壳体主体15与封口体16之间设有垫片27,确保电池壳体内部的密闭性。壳体主体15例如适合地具有对侧面部从外侧加压而形成的、用于支撑封口体16的突出部21。突出部21优选沿着壳体主体15的圆周方向形成为环状,在其上面支撑封口体16。
封口体16具有:形成有过滤器开口部22a的过滤器22、和配置于过滤器22上的阀体。阀体堵住过滤器22的过滤器开口部22a,由于内部短路等而产生的放热使电池的内压上升时阀体断裂。本实施方式中,作为阀体,设置有下阀体23和上阀体25,进一步设置有配置于下阀体23与上阀体25之间的绝缘构件24、和具有盖开口部26a的盖26。构成封口体16的各构件例如具有圆板形状或环形状,除绝缘构件24之外的各构件彼此电连接。具体而言,过滤器22与下阀体23在各周缘部彼此接合,上阀体25与盖26也在各周缘部彼此接合。下阀体23与上阀体25在各中央部彼此连接,在各周缘部之间夹设有绝缘构件24。需要说明的是,由于内部短路等而产生的放热使内压上升时,例如下阀体23在薄壁部断裂,由此上阀体25向盖26侧膨胀,从下阀体23脱离,从而两者的电连接被切断。
对于非水电解质二次电池10,例如体积能量密度为600Wh/L以上。如后述那样,对于非水电解质二次电池10,正极活性物质使用锂过渡金属氧化物,负极活性物质使用能够吸储·释放锂离子的材料。更详细而言,分别地,正极活性物质使用含有钴(Co)的锂过渡金属氧化物,负极活性物质使用含有硅(Si)的材料。进而,作为非水电解质,使用包含氟化链状羧酸酯的非水溶剂。
[正极]
正极例如由金属箔等正极集电体、和形成于正极集电体上的正极复合材料层构成。正极集电体可以使用铝等在正极的电位范围内稳定的金属的箔、表层配置有该金属的薄膜等。正极复合材料层适合的是,除正极活性物质之外还包含导电材料和粘结材料。正极例如可以如下制作:在正极集电体上涂布包含正极活性物质、粘结材料等的正极复合材料浆料,使涂膜干燥后,进行压延,在集电体的两面形成正极复合材料层。
正极活性物质具有层状结构,且以Co的含量相对于除Li之外的金属元素的总量为1mol%以上且低于20mol%的锂过渡金属氧化物(以下,记作“锂过渡金属氧化物A”)作为主成分。锂过渡金属氧化物A的晶体结构例如为六方晶,具有归属于空间群R-3m的对称性。正极活性物质也可以包含除锂过渡金属氧化物A之外的材料,锂过渡金属氧化物A相对于正极活性物质的总重量至少包含50重量%,优选包含80重量%以上,更优选包含90重量%以上。本实施方式中,对仅使用锂过渡金属氧化物A作为正极活性物质的情况进行说明。认为,通过使用含有Co的锂过渡金属氧化物A,在含有Si的负极活性物质的表面形成优质的覆膜,可以兼顾高输入输出特性和高耐久性。
锂过渡金属氧化物A中的Co的含量如上述那样为1mol%以上且低于20mol%、优选为2mol%~15mol%、更优选为3mol%~12mol%。锂过渡金属氧化物A在放电状态或未反应状态下例如由通式LiaCoxM1-xO2(0.9≤a≤1.2、0.01≤x<0.2、M为包含选自Ni、Mn、Al中的至少1种的金属元素)表示。作为金属元素M,例如可以举出:除Co、镍(Ni)、锰(Mn)之外的过渡金属元素、碱金属元素、碱土金属元素、第12族元素、除铝(Al)之外的第13族元素、和第14族元素。具体而言,可以举出:硼(B)、镁(Mg)、钛(Ti)、铬(Cr)、铁(Fe)、铜(Cu)、锌(Zn)、锆(Zr)、锶(Sr)、铌(Nb)、钼(Mo)、锡(Sn)、钽(Ta)、钨(W)、钠(Na)、钾(K)、钡(Ba)、钙(Ca)等。
锂过渡金属氧化物A优选Ni的含量相对于除Li之外的金属元素的总量为80mol%以上,更优选为85mol%以上。Ni的含量如果为80mol%以上,则输入输出特性和耐久性进一步提高。锂过渡金属氧化物A在放电状态或未反应状态下例如由通式LiaCoxNiyM1-x-yO2(0.9≤a≤1.2、0.01≤x<0.2、0.8≤y<1.0、0<x+y<1、M为包含选自Mn、Al中的至少1种的金属元素)表示。适合的锂过渡金属氧化物A的一例为Ni-Co-Al系、Ni-Co-Mn系的复合氧化物。
锂过渡金属氧化物A的粒径(通过激光衍射法测定的体积平均粒径)没有限定,优选为2μm~30μm。锂过渡金属氧化物的颗粒例如为粒径50nm~10μm的一次颗粒结合而成的二次颗粒。在锂过渡金属氧化物A的颗粒表面可以固着例如氧化钨、磷酸锂等无机化合物颗粒。
上述导电材料用于提高正极复合材料层的导电性。作为导电材料的例子,可以举出:炭黑(CB)、乙炔黑(AB)、科琴黑、石墨等碳材料等。它们可以单独使用也可以组合2种以上使用。
上述粘结材料为了维持正极活性物质和导电材料间的良好的接触状态、且提高正极活性物质等对正极集电体表面的粘结性而使用。作为粘结材料的例子,可以举出:聚四氟乙烯(PTFE)、聚偏二氟乙烯(PVdF)等氟系树脂、聚丙烯腈(PAN)、聚酰亚胺系树脂、丙烯酸类树脂、聚烯烃系树脂等。另外,可以组合使用这些树脂与羧甲基纤维素(CMC)或其盐(可以为CMC-Na、CMC-K、CMC-NH4等、以及部分中和型的盐)、聚环氧乙烷(PEO)等。它们可以单独使用也可以组合2种以上使用。
[负极]
负极例如由包含金属箔等的负极集电体、和形成于该集电体上的负极复合材料层构成。负极集电体可以使用铜等在负极的电位范围内稳定的金属的箔、表层配置有该金属的薄膜等。负极复合材料层适合的是,除了负极活性物质之外还包含粘结材料。负极例如可以如下制作:在负极集电体上涂布包含负极活性物质、粘结材料等的负极复合材料浆料,使涂膜干燥后,进行压延,在集电体的两面形成负极复合材料层。
负极活性物质如上述那样可以使用含有Si的材料。Si与石墨等碳材料相比,能够吸储更多的锂离子,因此,通过用于负极活性物质可以实现电池的高容量化。另外,通过负极活性物质中含有Si,可以兼顾高输入输出特性和高耐久性。作为含有Si的材料,可以使用Si,优选使用硅氧化物(以下,记作“硅氧化物B”)。
硅氧化物B适合的是,为SiOx(0.8≤x≤1.5)所示的氧化物。SiOx例如具有非晶态的SiO2的基质中分散有微细的Si的结构。利用透射型电子显微镜(TEM)观察SiOx颗粒时,可以确认Si的存在。Si优选在SiO2的基质中以200nm以下的尺寸均匀地分散。需要说明的是,SiOx颗粒也可以包含硅酸锂(例如Li2SiO3、Li2Si2O5等)。硅氧化物B的粒径(通过激光衍射法测定的体积平均粒径)例如为1μm~15μm、优选为4μm~10μm。
硅氧化物B适合的是,在颗粒表面具有由导电性比SiOx高的材料构成的导电层。作为构成导电层的导电材料,优选电化学稳定的材料,优选为选自由碳材料、金属和金属化合物组成的组中的至少1种材料。构成导电层的碳材料中,与正极复合材料层的导电材料同样地,可以使用炭黑、乙炔黑、科琴黑、石墨、和它们的2种以上的混合物等。
考虑导电性的确保和锂离子对硅氧化物B的扩散性,上述导电层的厚度优选1nm~200nm、更优选5nm~100nm。导电层的厚度可以利用扫描型电子显微镜(SEM)等通过颗粒的截面观察来测量。导电层例如可以利用CVD法、溅射环法、镀覆法(电解电镀·化学镀)等以往公知的方法而形成。利用CVD法在硅氧化物B的颗粒表面形成由碳材料形成的导电层时,例如将硅氧化物B的颗粒和烃系气体在气相中加热,使由烃系气体的热分解而产生的碳在硅氧化物B的颗粒上堆积。
作为负极活性物质,考虑循环特性等,适合的是,组合使用硅氧化物B与石墨。即,负极活性物质由硅氧化物B与石墨的混合物形成。负极活性物质可以进一步包含除石墨之外的碳材料等,优选实质上仅由硅氧化物B和石墨构成。从提高电池容量、输入输出特性、循环特性等的观点出发,硅氧化物B的含量相对于负极活性物质的总重量优选为1重量%~20重量%。更优选为2重量%~15重量%、特别优选为3重量%~10重量%。石墨的含量例如相对于负极活性物质的总重量为80重量%~99重量%。即,硅氧化物B与石墨的比例(混合比)以重量比计、优选为99:1~80:20、更优选为98:2~85:15、特别优选为97:3~90:10。
与硅氧化物B组合使用的石墨可以使用:以往作为非水电解质二次电池的负极活性物质使用的石墨、例如鳞片状石墨、块状石墨、土状石墨等天然石墨、块状人造石墨(MAG)、石墨化中间相碳微球(MCMB)等人造石墨等。石墨的粒径(通过激光衍射法测定的体积平均粒径)例如为5~30μm、优选为10~25μm。
作为上述粘结材料,与正极的情况同样地,可以使用氟系树脂、PAN、聚酰亚胺系树脂、丙烯酸类树脂、聚烯烃系树脂等。使用水系溶剂制备负极复合材料浆料时,优选使用:苯乙烯-丁二烯橡胶(SBR)、CMC或其盐、聚丙烯酸(PAA)或其盐(可以为PAA-Na、PAA-K等、以及部分中和型的盐)、聚乙烯醇(PVA)等。
[分隔件]
分隔件使用具有离子透过性和绝缘性的多孔性片。作为多孔性片的具体例,可以举出:微多孔薄膜、织布、无纺布等。作为分隔件的材质,适合的是,聚乙烯、聚丙烯等烯烃系树脂、纤维素等。分隔件也可以为具有纤维素纤维层和烯烃系树脂等热塑性树脂纤维层的层叠体。另外,也可以为包含聚乙烯层和聚丙烯层的多层分隔件,也可以使用在分隔件的表面涂布有芳纶系树脂等树脂的分隔件。
也可以在分隔件与正极和负极中至少一者的界面形成包含无机物的填料的填料层。作为无机物的填料,例如可以举出:含有Ti、Al、Si、Mg中的至少1种的氧化物、磷酸化合物等。填料层例如可以将含有该填料的浆料涂布于正极、负极或分隔件的表面而形成。
[非水电解质]
非水电解质包含:非水溶剂、和溶解于非水溶剂的电解质盐。非水溶剂如上述那样至少包含氟化链状羧酸酯。非水溶剂例如可以使用除氟化链状羧酸酯之外的酯类、醚类、腈类、二甲基甲酰胺等酰胺类、和它们的2种以上的混合溶剂等。另外,也可以使用丙磺酸内酯等含磺基化合物。非水溶剂也可以包含将这些溶剂的氢的至少一部分用氟等卤素原子取代而得到的卤素取代体。
上述氟化链状羧酸酯适合使用碳数3~5的氟化链状羧酸酯。作为具体例,可以举出:氟化丙酸甲酯、氟化丙酸乙酯、氟化乙酸甲酯、氟化乙酸乙酯、氟化乙酸丙酯等。其中,优选使用氟化丙酸甲酯(FMP),特别优选使用3,3,3-三氟丙酸甲酯。氟化链状羧酸酯的含量相对于构成非水电解质的非水溶剂的总体积优选为40体积%~90体积%。氟化链状羧酸酯的含量如果为该范围内,则容易在负极表面形成离子透过性优异的优质的覆膜。
作为上述酯类(除上述氟化链状羧酸酯之外)的例子,可以举出:碳酸亚乙酯(EC)、碳酸亚丙酯(PC)、碳酸亚丁酯、碳酸亚乙烯酯等环状碳酸酯、碳酸二甲酯(DMC)、碳酸甲乙酯(EMC)、碳酸二乙酯(DEC)、碳酸甲丙酯、碳酸乙丙酯、碳酸甲基异丙酯等链状碳酸酯、γ-丁内酯(GBL)、γ-戊内酯(GVL)等环状羧酸酯、将这些溶剂的氢的至少一部分用氟等卤素原子取代而得到的卤素取代体等。另外,非水溶剂也可以包含非氟化链状羧酸酯。
作为上述醚类的例子,可以举出:1,3-二氧戊环、4-甲基-1,3-二氧戊环、四氢呋喃、2-甲基四氢呋喃、环氧丙烷、1,2-环氧丁烷、1,3-二氧杂环己烷、1,4-二氧杂环己烷、1,3,5-三氧杂环己烷、呋喃、2-甲基呋喃、1,8-桉树脑、冠醚等环状醚、1,2-二甲氧基乙烷、二***、二丙醚、二异丙醚、二丁醚、二己醚、乙基乙烯醚、丁基乙烯醚、甲基苯醚、乙基苯醚、丁基苯醚、戊基苯醚、甲氧基甲苯、苄基***、二苯醚、二苄醚、邻二甲氧基苯、1,2-二乙氧基乙烷、1,2-二丁氧基乙烷、二乙二醇二甲醚、二乙二醇二***、二乙二醇二丁醚、1,1-二甲氧基甲烷、1,1-二乙氧基乙烷、三乙二醇二甲醚、四乙二醇二甲醚等链状醚类、将这些溶剂的氢的至少一部分用氟等卤素原子取代而得到的卤素取代体等。
作为上述腈类的例子,可以举出:乙腈、丙腈、丁腈、戊腈、正庚腈、琥珀腈、戊二腈、己二腈、庚二腈、1,2,3-丙烷三甲腈、1,3,5-戊烷三甲腈、将这些溶剂的氢的至少一部分用氟等卤素原子取代而得到的卤素取代体等。
作为非水溶剂,特别适合的是,将氟化链状羧酸酯与环状碳酸酯、特别是氟化环状碳酸酯组合使用。氟化链状羧酸酯和氟化环状碳酸酯的总计的含量相对于非水溶剂的总体积优选设为50体积%以上、更优选为80体积%以上。氟化链状羧酸酯的含量如上述那样相对于非水溶剂的总体积优选为40体积%~90体积%、更优选为50体积%~85体积%。氟化环状碳酸酯的含量相对于非水溶剂的总体积例如为3体积%~20体积%。作为与氟化链状羧酸酯组合使用的氟化环状碳酸酯,例如可以举出:4-氟碳酸亚乙酯(FEC)、4,5-二氟-1,3-二氧戊环-2-酮、4,4-二氟-1,3-二氧戊环-2-酮、4-氟-5-甲基-1,3-二氧戊环-2-酮、4-氟-4-甲基-1,3-二氧戊环-2-酮、4-三氟甲基-1,3-二氧戊环-2-酮、4,5-二氟-4,5-二甲基-1,3-二氧戊环-2-酮(DFBC)等。其中,特别优选FEC。
电解质盐优选为锂盐。作为锂盐的例子,可以举出:LiBF4、LiClO4、LiPF6、LiAsF6、LiSbF6、LiAlCl4、LiSCN、LiCF3SO3、LiC(C2F5SO2)、LiCF3CO2、Li(P(C2O4)F4)、Li(P(C2O4)F2)、LiPF6-x(CnF2n+1)x(1<x<6、n为1或2)、LiB10Cl10、LiCl、LiBr、LiI、氯硼烷锂、低级脂肪族羧酸锂、Li2B4O7、Li(B(C2O4)2)[锂-双草酸硼酸盐(LiBOB)]、Li(B(C2O4)F2)等硼酸盐类、LiN(FSO2)2、LiN(C1F2l+1SO2)(CmF2m+1SO2){l、m为1以上的整数}等酰亚胺盐类等。锂盐可以将它们单独使用1种,也可以混合多种而使用。其中,从离子传导性、电化学稳定性等观点出发,优选至少使用含氟锂盐,例如优选使用LiPF6。从即使高温环境下也在负极的表面形成稳定的皮膜的方面出发,特别适合的是,将组合使用含氟锂盐与以乙二酸盐络合物为阴离子的锂盐(例如LiBOB)。对于锂盐的浓度,相对于非水溶剂1L优选设为0.8~1.8mol。
实施例
以下,根据实施例对本公开进一步详细说明,但本公开不限定于这些实施例。
<实施例1>
[正极的制作]
将作为正极活性物质的LiNi0.88Co0.09Al0.03O2所示的锂镍钴铝复合氧化物100重量份、乙炔黑(AB)1重量份、和聚偏二氟乙烯(PVdF)1重量份混合,进而加入适量的N-甲基-2-吡咯烷酮(NMP),制备正极复合材料浆料。接着,将该正极复合材料浆料涂布于由铝箔形成的正极集电体的两面,使其干燥。将其切成规定的电极尺寸,使用辊进行压延,制作在正极集电体的两面形成有正极复合材料层的正极。需要说明的是,LiNi0.88Co0.09Al0.03O2的晶体结构为层状岩盐结构(六方晶、空间群R3-m)。
[负极的制作]
将作为负极活性物质的颗粒表面经过碳覆盖了的氧化硅(SiO)4重量份、石墨粉末(C)96重量份、羧甲基纤维素(CMC)1重量份、和苯乙烯-丁二烯橡胶(SBR)1重量份混合,进而加入适量的水,制备负极复合材料浆料。接着,将该负极复合材料浆料涂布于由铜箔形成的负极集电体的两面,使其干燥。将其切成规定的电极尺寸,使用辊进行压延,制作在负极集电体的两面形成有负极复合材料层的负极。
[非水电解质的制作]
将4-氟碳酸亚乙酯(FEC)与3,3,3-三氟丙酸甲酯(FMP)以15:85的体积比进行混合。在该混合溶剂中使LiPF6以成为1.2mol/L的浓度的方式溶解而制作非水电解质。需要说明的是,相对于电解液100重量份,添加碳酸亚乙烯酯0.5重量份、和丙烯磺内酯1重量份。
[电池的制作]
分别地,在上述正极上安装铝引线,在上述负极上安装镍引线,介由分隔件将正极和负极以漩涡状卷绕,从而制作卷绕型的电极体。分隔件使用的是,在聚乙烯制的微多孔膜的单面形成有使聚酰胺和氧化铝的填料分散而成的耐热层。将该电极体收纳于外径18.2mm、高度65mm的有底圆筒形状的电池壳体主体,注入上述非水电解液后,通过垫片和封口体将电池壳体主体的开口部封口,制作18650型的圆筒形非水电解质二次电池X1。
<比较例1>
使用EMC代替FMP,制作非水电解质,,除此之外,与实施例1同样地制作电池Y1。
<比较例2>
作为负极活性物质,不使用氧化硅而仅使用石墨,除此之外,与实施例1同样地制作电池Y2。
<比较例3>
使用EMC代替FMP,制作非水电解质,除此之外,与比较例2同样地制作电池Y3。
<比较例4>
使用LiNi0.50Co0.20Mn0.30O2代替LiNi0.88Co0.09Al0.03O2,制作正极,除此之外,与实施例1同样地制作电池Y4。
<比较例5>
使用EMC代替FMP,制作非水电解质,除此之外,与比较例4同样地制作电池Y5。
<比较例6>
作为负极活性物质,不使用氧化硅而仅使用石墨,除此之外,与比较例4同样地制作电池Y6。
<比较例7>
使用EMC代替FMP,制作非水电解质,除此之外,与比较例6同样地制作电池Y7。
[输入输出特性的评价]
对于上述各电池,测定重复下述充放电循环后的电阻值,作为输入输出特性的评价。
以0.3It(1000mA)充电至额定容量的100%〔即,充电深度(SOC)变为100%〕后,在25℃的条件下,从开路电压以0.5It(1500mA)的电流值进行20秒放电。根据放电开始20秒后的电压与放电即将开始前的电压,使用下述式1,算出25℃下的电阻值。需要说明的是,电池Y1~Y7的各电池的电阻值用将电池X1的电阻值设为100%时的相对值来表示。
[循环特性(耐久性)的评价]
对于上述各电池,测定重复下述充放电循环后的容量维持率,作为循环特性(耐久性)的评价。
在25℃的温度环境下,对各电池以0.3It(1000mA)mA的恒定电流进行充电直至电池电压变为4.2V,电池电压达到4.2V后,以恒定电压进行充电。接着,以0.3It(1000mA)mA的恒定电流进行放电直至电池电压变为3.0V,求出此时的放电容量(初始容量)。重复进行该充放电循环,将100个循环后的放电容量除以初始容量而得到的值乘以100,算出容量维持率。
[表1]
电池 | 正极活性物质 | 负极活性物质 | FMP | 电阻值(%) | 容量维持率(%) |
X1 | LiNi<sub>0.88</sub>Co<sub>0.09</sub>Al<sub>0.03</sub>O<sub>2</sub> | C+SiO | 有 | 100 | 93.7 |
Y1 | LiNi<sub>0.88</sub>Co<sub>0.09</sub>Al<sub>0.03</sub>O<sub>2</sub> | C+SiO | 无 | 109 | 91.6 |
Y2 | LiNi<sub>0.88</sub>Co<sub>0.09</sub>Al<sub>0.03</sub>O<sub>2</sub> | C | 有 | 129 | - |
Y3 | LiNi<sub>0.88</sub>Co<sub>0.09</sub>Al<sub>0.03</sub>O<sub>2</sub> | C | 无 | 116 | - |
Y4 | LiNi<sub>0.50</sub>Co<sub>0.20</sub>Mn<sub>0.30</sub>O<sub>2</sub> | C+Si0 | 有 | 110 | - |
Y5 | LiNi<sub>0.50</sub>Co<sub>0.20</sub>Mn<sub>0.30</sub>O<sub>2</sub> | C+SiO | 无 | 105 | - |
Y6 | LiNi<sub>0.50</sub>Co<sub>0.20</sub>Mn<sub>0.30</sub>O<sub>2</sub> | C | 有 | 181 | - |
Y7 | LiNi<sub>0.50</sub>Co<sub>0.20</sub>Mn<sub>0.30</sub>O<sub>2</sub> | C | 无 | 167 | - |
由表1的结果可知,对于分别作为正极活性物质使用LiNi0.88Co0.09Al0.03O2所示的复合氧化物、作为负极活性物质使用含有Si的材料、非水电解质中包含FMP的电池X1,与比较例的各电池相比,电阻值低、且容量维持率高。即,电池X1与比较例的各电池相比,具有高输入输出特性和良好的循环特性。认为其结果是由于,在充电时从正极溶出的Co在含有Si的负极活性物质的表面与氟化链状羧酸酯特异性地发生反应,形成包含Co和Si的离子透过性优异的优质的覆膜。另一方面,负极活性物质中不含有Si的情况下(电池Y2、3、6、7)、Co的含量为20mol%以上的情况下(电池Y4~7),电阻值高,无法得到良好的输入输出特性。认为,负极活性物质中不含Si的情况下,形成于负极表面的覆膜中也不含Si,不会形成电池X1那样的覆膜,电阻值增加。认为,Co量过多时,与形成于含有Si的负极活性物质的表面的FMP的覆膜变得过厚,电阻值增加。另外,认为,Co量过少(例如低于1mol%)时,为了充分形成优质的覆膜所需的Co少。需要说明的是,比较例的各电池中,通过添加FMP,电阻值反而上升。即,仅应用上述本公开的特征的情况下,可以特异性获得能够兼顾高输入输出特性和长寿命化这样的作用效果。
附图标记说明
10非水电解质二次电池、11正极、12负极、13分隔件、14电极体、15壳体主体、16封口体、17,18绝缘板、19正极引线、20负极引线、22过滤器、22a过滤器开口部、23下阀体、24绝缘构件、25上阀体、26盖、26a盖开口部、27垫片
Claims (3)
1.一种非水电解质二次电池,其具备:
正极,其包含正极活性物质,所述正极活性物质具有层状结构,且以钴(Co)的含量相对于除锂(Li)之外的金属元素的总量为1mol%以上且低于12mol%的锂过渡金属氧化物作为主成分;
负极,其包含含有硅(Si)的负极活性物质;和,
3,3,3-三氟丙酸甲酯,
所述负极活性物质由0.8≤x≤1.5的SiOx所示的硅氧化物与石墨的混合物组成,
所述硅氧化物的含量相对于所述负极活性物质的总重量为1重量%~20重量%,所述石墨的含量为80重量%~99重量%。
2.根据权利要求1所述的非水电解质二次电池,其中,所述锂过渡金属氧化物的镍(Ni)的含量相对于除锂(Li)之外的金属元素的总量为80mol%以上。
3.根据权利要求1或2所述的非水电解质二次电池,其中,所述3,3,3-三氟丙酸甲酯的含量相对于构成所述非水电解质的非水溶剂的总体积为40体积%~90体积%。
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