CN109906528B - 制造适于高负载的二次电池的电极的方法 - Google Patents
制造适于高负载的二次电池的电极的方法 Download PDFInfo
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- CN109906528B CN109906528B CN201880004218.0A CN201880004218A CN109906528B CN 109906528 B CN109906528 B CN 109906528B CN 201880004218 A CN201880004218 A CN 201880004218A CN 109906528 B CN109906528 B CN 109906528B
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Abstract
本文提供一种制备二次电池的电极的方法。在一些实施方式中,该方法包括:用电极浆料涂布集流体以在集流体上形成涂布层,电极浆料包括粘合剂、电极活性材料、导电材料、无定形硒纳米颗粒和溶剂;以及干燥涂布层,其中该干燥使无定形硒纳米颗粒蒸发并在涂布层中形成通道。
Description
技术领域
本公开内容涉及一种制备二次电池的电极的方法。该制备二次电池的电极的方法包括:用电极浆料涂布集流体以在集流体上形成涂布层,电极浆料包括粘合剂、电极活性材料、导电材料、无定形硒纳米颗粒和溶剂;以及干燥涂布层以使无定形硒纳米颗粒蒸发并在涂布层中形成通道。
背景技术
随着移动装置的技术发展以及对移动装置需求的增加,对作为能源的二次电池的需求已迅猛增长。在二次电池之中,已对具有高能量密度和高放电电压的锂二次电池进行了大量的研究,并且锂二次电池已得到商业化并被广泛使用。
就电池的形状而言,对足够薄以便应用于诸如移动电话之类的产品的棱柱型二次电池和袋型二次电池的需求非常高。然而,就电池的材料而言,对诸如锂离子电池和锂离子聚合物电池之类的表现出高能量密度、高放电电压和高输出稳定性的锂二次电池的需求非常高。
根据其形状,二次电池可分为圆柱型电池单元、棱柱型电池单元以及袋型电池单元。在它们之中,圆柱型二次电池包括电极组件、包含电极组件的圆柱型罐以及结合至罐的顶部的盖组件。
在二次电池中,安装在电池壳体中的电极组件是电力产生元件,其由正极、隔膜和负极的堆叠结构构成,并且可以进行充放电。电极组件可大致分为:通过在施加有电极活性材料浆料的片型的正极和负极之间插置隔膜而卷绕的果冻卷(Jelly-roll)型;在隔膜插置在多个正极和负极之间的状态下顺序地层压的堆叠型;以及用堆叠型的单元电池卷绕到长的隔离膜上的堆叠/折叠型。在这些电极组件之中,果冻卷型电极组件具有诸如易于制造且具有高的每单位重量的能量密度之类的优势,由此被广泛使用。
果冻卷型电极组件由用正极、负极和插置在这两个电极之间的隔膜卷绕成圆柱形的果冻卷型构成,并且正极接片和负极接片各自从正极和负极引出。通常,正极接片引出至上部,而负极接片引出至下部。
罐是圆柱型二次电池中具有几乎是圆柱形状的金属材料的容器,并且通过诸如深拉伸(deep drawing)之类的制造方法来形成。因此,罐自身可以是端子。
盖组件具有这样的结构,即在其中顺序堆叠有形成正极端子的上端盖、配置成在电池内部的温度升高时极大增加电池的电阻以切断电流的PTC元件、配置成在电池内部的压力升高时切断电流或排出气体的安全排气部、配置成将安全排气部与除某些部分以外的盖板电隔离的衬垫、以及连接有与正极连接的正极端子的盖板。
电极组件的正极通过从正极向上引出的正极接片电连接至盖组件的一个部件,而负极通过从负极向下引出的负极接片连接至罐的底表面。当然,可通过改变极性来设计电极。
另外,用于在电极组件与盖组件之间绝缘的上绝缘构件位于电极组件与盖组件之间,而用于在电极组件与罐的底表面之间绝缘的下绝缘构件位于电极组件与罐的底表面之间。
此外,锂二次电池包括含锂过渡金属氧化物作为电极活性材料的正极、含碳基活性材料的负极、和多孔隔膜。正极通过将正极浆料涂布至铝箔来制备,而负极通过将含碳基活性材料的负极浆料涂布至铜箔来制备。
正极浆料和负极浆料添加导电材料以改善活性材料的电导率。尤其是,用作正极活性材料的锂过渡金属氧化物本质上具有较低的电导率,由此正极浆料必须添加导电材料。
作为导电材料,主要使用碳基材料,例如,诸如天然石墨和人造石墨之类的石墨;诸如炭黑、乙炔黑、槽法炭黑、炉法炭黑、灯黑、夏黑之类的炭黑等等,并且,在一些情况下,使用诸如碳纤维、金属纤维等的导电纤维。市售的导电材料的具体示例可包括各种乙炔黑产品(可从Chevron Chemical Company获得)、Denka黑(可从Denka Singapore PrivateLimited获得)、可从Gulf Oil Company获得的各种产品、Vulcan XC-72(可从CabotCompany获得)、Super P(Timcal Co.,Ltd.)等等。
随着电力需求的增加,电池逐渐具有较高容量,并且出现了具有高能量密度的高负载电极。在高负载电极的情况下,与低负载电极相比,因为锂离子向电极中的箔的转移非常低,所以循环性能较低。
具体地,为了改善高负载电极中的锂离子的直行性,已经提出了诸如增加电极中的孔隙率或在制造电极之后在电极中机械地制备孔隙之类的方法。
然而,在增加电极中的孔隙率的情形中,由于厚度增加,因此能量密度降低,并且在制造电极之后在电极中制备孔隙的情形中,由于电极活性材料的减少和人造形状,因此可能会发生局部电极劣化。
发明内容
技术问题
为了解决上述问题,本公开内容提供了一种制备具有通道的电极的方法,该方法通过将无定形硒纳米颗粒添加到用于制备常规电极浆料的电极活性材料、导电材料和粘合剂的混合工序中,并且在施加和干燥电极浆料时使硒纳米颗粒蒸发。
技术方案
根据本公开内容的一个示例性实施方式,提供一种制备二次电池的电极的方法,包括:将粘合剂分散或溶解于溶剂中以制备粘合剂溶液;通过将所述粘合剂溶液与包含电极活性材料、导电材料和无定形硒纳米颗粒的电极材料混合来制备电极浆料;用所述电极浆料涂布集流体以在所述集流体上形成涂布层;以及干燥所述涂布层以使所述无定形硒纳米颗粒蒸发并在所述涂布层中形成通道。
根据本公开内容的另一个示例性实施方式,所述无定形硒纳米颗粒的尺寸可在500nm至1000nm的范围内。
根据本公开内容的再一个示例性实施方式,所述无定形硒纳米颗粒可在90℃至110℃下蒸发。
根据本公开内容的又一个示例性实施方式,所述涂布层的起泡可包括在所述涂布层中形成通道。
根据本公开内容的又一个示例性实施方式,提供一种二次电池的电极,所述电极由上述方法制造。
根据本公开内容的又一个示例性实施方式,提供一种包括所述电极的锂二次电池。
根据本公开内容的又一个示例性实施方式,所述电池可以是选自锂离子电池、锂聚合物电池和锂离子聚合物电池中的任一种。
根据本公开内容的又一个示例性实施方式,提供一种包括至少一个上述二次电池的电池组。
根据本公开内容的又一个示例性实施方式,提供一种包括所述电池组作为电源的装置。
根据本公开内容的又一个示例性实施方式,所述装置可以是选自移动电话、便携式计算机、智能电话、智能平板、上网本、可穿戴电子装置、轻型电动车(Light ElectronicVehicle,LEV)、电动汽车、混合电动汽车、插电式混合电动汽车和电力存储装置中的任一种。
有益效果
提供了一种制备具有通道结构的二次电池的电极的方法。制备二次电池的电极的方法包括:将粘合剂分散或溶解于溶剂中以制备粘合剂溶液;通过将所述粘合剂溶液与包含电极活性材料、导电材料和无定形硒纳米颗粒的电极材料混合来制备电极浆料;用所述电极浆料涂布集流体以在所述集流体上形成涂布层;以及干燥所述涂布层以使所述无定形硒纳米颗粒蒸发并在所述涂布层中形成通道。
另外,本公开内容提供了:通过上述方法制备并且适于高负载的电极;包括所述电极的二次电池;使用所述二次电池的电池组;以及使用所述电池组的装置。
附图说明
图1A是示出根据本公开内容示例性实施方式的干燥之前的涂布层的示意图。
图1B是示出根据本公开内容示例性实施方式的干燥之后的涂布层的示意图。
具体实施方式
下文中,将详细描述本公开内容的优选实施方式。另外,现有实施方式并非意在限制本公开内容的范围,而是仅仅作为示例进行展示,而且在不偏离技术主旨的情况下可做出各种改进。
本公开内容的一种制备二次电池的电极的方法包括将粘合剂分散或溶解于溶剂中以制备粘合剂溶液以及通过将该粘合剂溶液与包含电极活性材料、导电材料和无定形硒纳米颗粒的电极材料混合来制备电极浆料。如图1A所绘示,在集流体上涂布电极浆料以形成涂布层10,其中涂布层10具有设于其中的无定形硒纳米颗粒20。干燥涂布层以使无定形硒纳米颗粒20蒸发并在涂布层中形成通道30,如图1B所绘示。
下面将与根据本公开内容的二次电池一起描述粘合剂、电极活性材料、和导电材料的类型。
根据本公开内容,无定形硒纳米颗粒的尺寸可在500nm至1000nm的范围内。无定形硒纳米颗粒在蒸发时起到形成通道的作用。通道旨在增强锂离子的直行性,因此小于500nm的无定形硒纳米颗粒不会有助于锂离子通过,并且粒径超过1nm的无定形硒纳米颗粒起到空隙的作用,使得无定形硒纳米颗粒的能量密度随着电极孔隙率的增加而降低,这不是优选的。
将粘合剂、电极活性材料、导电材料和无定形硒纳米颗粒混合在一起以制备电极浆料,用该电极浆料涂布集流体。下面将用根据本公开内容的二次电池详细描述涂布的厚度。
当涂布的电极浆料在90至110℃下干燥时,无定形硒纳米颗粒蒸发以使涂布层起泡。使涂布层起泡意味着在涂布层中形成通道。一般的硒具有高熔点,从而在90至110℃的温度下不会蒸发。然而,由于无定形硒纳米颗粒由比结晶纳米颗粒更多的无序颗粒构成并由此具有微弱的分子间引力,无定形硒纳米颗粒可在90至110℃的温度下蒸发。
因此,由于无定形硒纳米颗粒难以蒸发的问题,低于90℃的温度不是优选的,并且由于电极浆料中的其他组分也可蒸发并由此可改变电极结构,超过110℃的温度也不是优选的。
通过上述方法制备的本公开内容的二次电池的电极具有适于高负载的结构,使得增强了锂离子的直行性并且不降低能量密度。
此外,本公开内容提供了一种包括以上述方法制备并且适于高负载的电极的二次电池。
根据本公开内容的二次电池配置成容纳其中不同极性的两个电极在被隔膜分离的状态下进行层压的电极组件,并且电极组件包括含正极活性材料的正极、含负极活性材料的负极和隔膜。
具体而言,例如,通过将正极活性材料、导电材料和粘合剂的混合物施加在正极集流体上然后干燥所得物来制备正极,并且根据需要可进一步将填料添加至混合物中。
根据本公开内容,正极活性材料可使用层状混合物,诸如锂钴氧化物(LiCoO2)、锂镍氧化物(LiNiO2)等,或者用一种或多种过渡金属取代的化合物;分子式Li1+xMn2-xO4(其中,x是0~0.33),诸如LiMnO3、LiMn2O3、LiMnO2等的锂锰氧化物(LiMnO2);锂铜氧化物(Li2CuO2);钒氧化物,诸如LiV3O8、LiFe3O4、V2O5、Cu2V2O7等;由分子式LiNi1-xMxO2(其中M=Co、Mn、Al、Cu、Fe、Mg、B或Ga,x=0.01~0.3)表示的镍位点型锂镍氧化物(lithiatednickel oxide);由分子式LiMn2-xMxO2(其中M=Co、Ni、Fe、Cr、Zn或Ta,x=0.01~0.1)或Li2Mn3MO8(其中M=Fe、Co、Ni、Cu或Zn)表示的锂锰复合氧化物、分子式的锂一部分被碱土金属离子取代的LiMn2O4;二硫化合物;具有诸如由Fe2(MoO4)3或它们的组合形成的复合氧化物之类的锂嵌入材料(lithiumintercalation material)作为主要组分的化合物。
正极集流体通常制备成具有3至500μm的厚度。对于正极集流体没有特别限制,只要其在制造的电池中不会引起化学变化并且具有导电性即可。例如,可使用不锈钢、铝、镍、钛、烧结碳、或者用碳、镍、钛或银进行表面处理的铝或不锈钢。集流体可在其表面上形成细微的无规则体,并且能够增加正极活性材料的粘合力,其可以是诸如膜、片、箔、网、多孔材料、泡沫体、无纺布体之类的各种形式。
通常可以以基于包含正极活性材料的混合物的总重量的1至50重量%的量添加导电材料。对于导电材料没有特别限制,只要其在制造的电池中不会引起化学变化并且具有导电性即可。例如,可使用石墨,诸如天然石墨或人造石墨;炭黑,诸如炭黑、乙炔黑、科琴黑、槽法炭黑、炉法炭黑、灯黑和热炭黑;导电纤维,诸如碳纤维和金属纤维;金属粉末,诸如氟化碳粉末、铝粉和镍粉;导电晶须,诸如氧化锌晶须和钛酸钾晶须;导电金属氧化物,诸如钛氧化物;导电材料,诸如聚苯撑衍生物等。
粘合剂是辅助活性材料和导电材料的粘合以及辅助与集流体的粘合的组分,通常以基于包含正极活性材料的混合物的总重量的1至50重量%添加粘合剂。粘合剂的示例为聚偏二氟乙烯、聚乙烯醇、羧甲基纤维素(CMC)、淀粉、羟丙基纤维素、再生纤维素、聚乙烯吡咯烷酮、四氟乙烯、聚乙烯、聚丙烯、乙烯-丙烯-二烯三元聚合物(EPDM)、磺化EPDM、丁苯橡胶、氟橡胶以及各种共聚物等。
填料可以是可选择地用作抑制正极膨胀的组分。填料没有特别限制,只要其是不会在制造的电池中引起化学变化的纤维材料即可。填料的示例包括烯烃类聚合物,诸如聚乙烯和聚丙烯;和纤维材料,诸如玻璃纤维和碳纤维等。
此外,通过涂布并干燥负极集流体上的负极材料来制备负极,并且可进一步包括上述的组分。
负极集流体通常可制造成3至500μm的厚度。对于负极集流体而言,可没有限制地使用不会诱发化学变化并且具有高导电性的材料。负极集流体的示例可包括铜、不锈钢、铝、镍、钛、烧结碳、或者用碳、镍、钛或银进行表面处理的铝或不锈钢。与正极集流体一样,负极集流体可在其表面上具有细微的无规则体以增加负极活性材料的粘合力,并且可具有诸如膜、片、箔、网、多孔体、泡沫体以及无纺布体等的各种形式。
负极材料包括无定形碳或结晶碳,具体而言,可使用碳,诸如非石墨化碳或石墨系碳;金属复合氧化物,诸如LixFe2O3(0≤x≤1)、LixWO2(0≤x≤1)、SnxMe1-xMe′yOz(Me:Mn、Fe、Pb、Ge;Me′:Al、B、P、Si、元素周期表第1、2、3族元素、卤素;0≤x≤1;1≤y≤3;1≤z≤8);锂金属;锂合金;硅系合金;锡系合金;氧化物,诸如SnO、SnO2、PbO、PbO2、Pb2O3、Pb3O4、Sb2O3、Sb2O4、Sb2O5、GeO、GeO2、Bi2O3、Bi2O4或Bi2O5;导电聚合物,诸如聚乙炔;或Li-Co-Ni系材料。
对于在正极和负极之间将电极绝缘的隔膜而言,可使用常规的聚烯烃类隔膜或者在烯烃类材料上形成有机和无机复合层的复合隔膜,但不限于此。
电解质可以是包含锂盐的非水电解液,并且可包括非水电解液和锂。非水电解液的示例可包括非水电解质、固体电解质、无机固体电解质等。
非水电解质的示例,可使用诸如N-甲基-2-吡咯酮、碳酸丙烯酯、碳酸乙烯酯、碳酸丁烯酯、碳酸二甲酯、碳酸二乙酯、γ-丁内酯、1,2-二甲氧基乙烷、四羟基法兰克(franc)、2-甲基四氢呋喃、二甲亚砜、1,3-二氧戊环、甲酰胺、二甲基甲酰胺、二氧戊环、乙腈、硝基甲烷、甲酸甲酯、乙酸甲酯、磷酸三酯、三甲氧基甲烷、二氧戊环衍生物、环丁砜、甲基环丁砜、1,3-二甲基-2-咪唑烷酮、碳酸丙烯酯衍生物、四氢呋喃衍生物、醚、丙酸甲酯和丙酸乙酯。
有机固体电解质的示例可使用聚乙烯衍生物、聚环氧乙烷衍生物、聚环氧丙烷衍生物、磷酸酯聚合物、聚搅拌赖氨酸(agitation lysine)、聚酯硫化物、聚乙烯醇、聚偏二氟乙烯和含有离子解离基团的聚合物。
无机固体电解液的示例是锂(Li)的氮化物、卤化物和硫酸盐,诸如Li3N、LiI、Li5NI2、Li3N-LiI-LiOH、LiSiO4、LiSiO4-LiI-LiOH、Li2SiS3、Li4SiO4、Li4SiO4-LiI-LiOH和Li3PO4-Li2S-SiS2。
锂盐是一种在上述提及的非水电解液中迅速可溶的材料,并且可包括,例如,LiCl、LiBr、LiI、LiClO4、LiBF4、LiB10Cl10、LiPF6、LiCF3SO3、LiCF3CO2、LiAsF6、LiSbF6、LiAlCl4、CH3SO3Li、CF3SO3Li、(CF3SO2)2NLi、氯硼烷锂、低级脂肪族羧酸锂、四苯硼酸锂、以及酰亚胺。
此外,为了改善充电和放电特性以及阻燃性,例如,可将吡啶、亚磷酸三乙酯、三乙醇胺、环醚、乙二胺、n-乙二醇二甲醚(glyme)、六磷酸三酰胺、硝基苯衍生物、硫、醌亚胺染料、N-取代的恶唑烷酮、N,N-取代的咪唑啉、乙二醇二烷基醚、铵盐、吡咯、2-甲氧基乙醇、三氯化铝等添加至非水电解液中。根据具体情况,为了赋予不燃性,非水电解液可进一步包括含卤溶剂,诸如四氯化碳和三氟乙烯。而且,为了改善高温存储特性,非水电解液可进一步包括二氧化碳气体。
电池是选自锂离子电池、锂聚合物电池、锂离子聚合物电池当中的任一种。这是根据电解质的性质分类的,并且正极、负极和电解液如上所述。
此外,本公开内容提供一种包含一个或多个所述二次电池的电池组。
本公开内容还提供一种包含所述电池组的装置。该装置的示例包括移动电话、便携式计算机、智能电话、智能平板、可穿戴电子装置、平板电脑、上网本、轻型电动车(LightElectronic Vehicle,LEV)、电动汽车、混合电动汽车、插电式混合电动汽车或电力存储装置,且不限于此。
下文中,将参照以下示例详细描述本公开内容。然而,本文中提供的示例用于阐明本公开内容,并且本公开内容的范围不限于此。
<示例1>
使用混合的羟基氧化物MOOH(M=Ni4/15(Mn1/2Ni1/2)8/15Co0.2)作为过渡金属前驱体以制备锂-镍-锰-钴类活性材料,并将混合的羟基氧化物与Li2Co3以计量比(Li:M=1.02:1)混合,然后将混合物于空气中在900℃下烧结10小时以制备锂混合过渡金属氧化物。通过将95.1重量%的正极活性材料和0.9重量%的多孔导电材料与2重量%的作为粘合剂的聚偏二氟乙烯(polyvinylidene fluoride,PVdF)混合来制备正极混合物,该正极活性材料通过将锂混合过渡金属氧化物和Li2CoO2以20:80的比例混合得到,该多孔导电材料具有35nm的平均颗粒直径和360ml/100g的DBP吸附值,并将2重量%的500nm无定形硒纳米颗粒和N-甲基吡咯烷酮(N-methlypyrrolidone,NMP)加入至制得的正极混合物以制备正极混合物浆料。将正极混合物浆料施加在作为集流体的铝箔上,接着于真空烘箱中在100℃下干燥2小时或更久以制备正极。
<示例2>
以与示例1中相同的方式制备正极,区别之处在于使用750nm无定形硒纳米颗粒。
<示例3>
以与示例1中相同的方式制备正极,区别之处在于使用1000nm无定形硒纳米颗粒。
<示例4>
以与示例1中相同的方式制备正极,区别之处在于使用750nm无定形硒纳米颗粒并在90℃下干燥。
<示例5>
以与示例1中相同的方式制备正极,区别之处在于使用750nm无定形硒纳米颗粒并在110℃下干燥。
<比较例1>
以与示例1中相同的方式制备正极,区别之处在于不使用无定形硒纳米颗粒。
测量在示例1至示例5和比较例1中制备的每一个正极的电导率,结果示出于表1中。
[表1]
电导率(Ωcm)<sup>-1</sup> | |
示例1 | 1.3×10<sup>-2</sup> |
示例2 | 1.2×10<sup>-2</sup> |
示例3 | 1.1×10<sup>-2</sup> |
示例4 | 1.1×10<sup>-2</sup> |
示例5 | 1.2×10<sup>-2</sup> |
比较例1 | 1.2×10<sup>-3</sup> |
如表1中所示,可以看出,使用根据本公开内容的通过混合无定形硒纳米颗粒制备的正极浆料而制备的示例1至示例5的正极的电导率,比使用常规方法制备的比较例1的正极的电导率高十倍以上。
如上所述,尽管已参照具体的实施方式和附图描述了本公开内容,但本公开内容不限于此。本领域技术人员可以清楚的是,在不偏离本公开内容的精神和范围以及随附权利要求书的等同的情况下可做出各种改进和修改。
Claims (9)
1.一种制备锂二次电池的电极的方法,包括:
用电极浆料涂布集流体以在所述集流体上形成涂布层,所述电极浆料包括粘合剂、电极活性材料、导电材料、无定形硒纳米颗粒和溶剂;以及
干燥所述涂布层以使所述无定形硒纳米颗粒蒸发并在所述涂布层中形成通道,
其中所述无定形硒纳米颗粒的尺寸在500nm至1000nm的范围内,并且
其中所述涂布层在90℃至110℃下干燥。
2.一种锂二次电池的电极,所述电极由根据权利要求1所述的方法制造。
3.一种锂二次电池,所述锂二次电池包括根据权利要求2所述的电极。
4.如权利要求3所述的锂二次电池,其中所述锂二次电池是锂离子电池。
5.如权利要求3所述的锂二次电池,其中所述锂二次电池是锂聚合物电池。
6.如权利要求3所述的锂二次电池,其中所述锂二次电池是锂离子聚合物电池。
7.一种电池组,所述电池组包括至少一个根据权利要求4至6中任一项所述的锂二次电池。
8.一种包括根据权利要求7所述的电池组作为电源的装置。
9.如权利要求8所述的装置,其中所述装置包括选自移动电话、便携式计算机、智能电话、可穿戴电子装置、轻型电动车、电动汽车、和电力存储装置中的任一种。
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EP3522269A1 (en) | 2019-08-07 |
CN109906528A (zh) | 2019-06-18 |
US20190379033A1 (en) | 2019-12-12 |
WO2018159946A1 (ko) | 2018-09-07 |
KR102246622B1 (ko) | 2021-04-30 |
PL3522269T3 (pl) | 2020-11-16 |
EP3522269B1 (en) | 2020-07-08 |
KR20180100857A (ko) | 2018-09-12 |
EP3522269A4 (en) | 2019-09-18 |
US10741827B2 (en) | 2020-08-11 |
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