CN110199414B - 锂二次电池用正极以及包含其的锂二次电池 - Google Patents
锂二次电池用正极以及包含其的锂二次电池 Download PDFInfo
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- CN110199414B CN110199414B CN201880007237.9A CN201880007237A CN110199414B CN 110199414 B CN110199414 B CN 110199414B CN 201880007237 A CN201880007237 A CN 201880007237A CN 110199414 B CN110199414 B CN 110199414B
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- Prior art keywords
- positive electrode
- secondary battery
- lithium secondary
- lithium
- active material
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- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 49
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 47
- 230000002427 irreversible effect Effects 0.000 claims abstract description 34
- 239000007774 positive electrode material Substances 0.000 claims abstract description 31
- 239000000463 material Substances 0.000 claims abstract description 28
- FUJCRWPEOMXPAD-UHFFFAOYSA-N lithium oxide Chemical compound [Li+].[Li+].[O-2] FUJCRWPEOMXPAD-UHFFFAOYSA-N 0.000 claims abstract description 11
- 229910001947 lithium oxide Inorganic materials 0.000 claims abstract description 8
- 239000000203 mixture Substances 0.000 claims description 20
- 239000002210 silicon-based material Substances 0.000 claims description 13
- 239000011255 nonaqueous electrolyte Substances 0.000 claims description 12
- 229910000676 Si alloy Inorganic materials 0.000 claims description 6
- 239000002131 composite material Substances 0.000 claims description 6
- 229910052710 silicon Inorganic materials 0.000 claims description 6
- 229910001323 Li2O2 Inorganic materials 0.000 claims description 4
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 4
- 239000007773 negative electrode material Substances 0.000 claims description 4
- 229910052760 oxygen Inorganic materials 0.000 claims description 4
- 239000001301 oxygen Substances 0.000 claims description 4
- 239000010703 silicon Substances 0.000 claims description 4
- 229910052814 silicon oxide Inorganic materials 0.000 claims description 4
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims description 3
- XUCJHNOBJLKZNU-UHFFFAOYSA-M dilithium;hydroxide Chemical compound [Li+].[Li+].[OH-] XUCJHNOBJLKZNU-UHFFFAOYSA-M 0.000 claims description 3
- 238000004146 energy storage Methods 0.000 claims description 3
- 229910001416 lithium ion Inorganic materials 0.000 claims description 3
- RJCRUVXAWQRZKQ-UHFFFAOYSA-N oxosilicon;silicon Chemical compound [Si].[Si]=O RJCRUVXAWQRZKQ-UHFFFAOYSA-N 0.000 claims description 3
- -1 PO)4 Chemical class 0.000 description 20
- 239000010410 layer Substances 0.000 description 20
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 15
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 12
- 239000011248 coating agent Substances 0.000 description 12
- 238000000576 coating method Methods 0.000 description 12
- 230000000052 comparative effect Effects 0.000 description 11
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 10
- 229910052782 aluminium Inorganic materials 0.000 description 9
- 239000004020 conductor Substances 0.000 description 9
- 239000000654 additive Substances 0.000 description 8
- HPGPEWYJWRWDTP-UHFFFAOYSA-N lithium peroxide Chemical compound [Li+].[Li+].[O-][O-] HPGPEWYJWRWDTP-UHFFFAOYSA-N 0.000 description 8
- 229910052759 nickel Inorganic materials 0.000 description 8
- 239000003960 organic solvent Substances 0.000 description 8
- 230000000996 additive effect Effects 0.000 description 7
- 239000006183 anode active material Substances 0.000 description 7
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- 229910052802 copper Inorganic materials 0.000 description 7
- 239000010949 copper Substances 0.000 description 7
- 239000000126 substance Substances 0.000 description 7
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- 239000010936 titanium Substances 0.000 description 7
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 6
- 239000003575 carbonaceous material Substances 0.000 description 6
- 229910052742 iron Inorganic materials 0.000 description 6
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 6
- 238000002360 preparation method Methods 0.000 description 6
- 239000007784 solid electrolyte Substances 0.000 description 6
- 239000004698 Polyethylene Substances 0.000 description 5
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- 230000007423 decrease Effects 0.000 description 5
- 239000003792 electrolyte Substances 0.000 description 5
- 229910003002 lithium salt Inorganic materials 0.000 description 5
- 159000000002 lithium salts Chemical class 0.000 description 5
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- 229910013292 LiNiO Inorganic materials 0.000 description 2
- 229910013872 LiPF Inorganic materials 0.000 description 2
- 229910001290 LiPF6 Inorganic materials 0.000 description 2
- 101150058243 Lipf gene Proteins 0.000 description 2
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- KAESVJOAVNADME-UHFFFAOYSA-N Pyrrole Chemical compound C=1C=CNC=1 KAESVJOAVNADME-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
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- 150000001450 anions Chemical class 0.000 description 2
- WMWLMWRWZQELOS-UHFFFAOYSA-N bismuth(iii) oxide Chemical compound O=[Bi]O[Bi]=O WMWLMWRWZQELOS-UHFFFAOYSA-N 0.000 description 2
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- 238000006243 chemical reaction Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
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- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明涉及一种锂二次电池用正极以及包含其的锂二次电池,所述正极包括正极集电体和在所述正极集电体的至少一个表面上涂覆并形成的正极活性材料层,其中,所述正极集电体包括未涂覆正极活性材料层的突出的未涂覆部,并且在所述未涂覆部上涂覆有由锂氧化物组成的不可逆材料。
Description
技术领域
相关申请的交叉引用
本申请要求于2017年11月30日向韩国知识产权局提交的韩国专利申请第10-2017-0163156号以及于2018年11月29日向韩国知识产权局提交的韩国专利申请第10-2018-0151235号的优先权权益,并通过援引将其内容完整并入本文。
本公开涉及锂二次电池用正极以及包含其的锂二次电池,更具体地,涉及高能量锂二次电池用正极以及包含其的锂二次电池。
背景技术
随着技术发展和对于各种装置的需求增加,对使用二次电池作为能源的需求迅速增加。在这些二次电池中,具有高能量密度和电压、长循环寿命和低自放电率的锂二次电池是可商购的并被广泛使用。
在这种锂二次电池中,作为正极活性材料,通常使用具有层状晶体结构的含锂的钴氧化物(LiCoO2)、具有层状晶体结构的LiMnO2、具有尖晶石晶体结构的LiMn2O4以及含锂的镍氧化物(LiNiO2)。并且,作为负极活性材料,主要使用碳材料。最近,由于对高能量锂二次电池的需求增加,正在考虑将有效容量为碳基材料的10倍以上的硅基材料或硅氧化物基材料混合使用。
同时,为了开发高能量锂二次电池,最近认为有必要使用以硅基材料作为负极活性材料的负极。然而,应用硅基材料的负极具有高的不可逆容量,因此存在充电/放电效率低的问题。
为了解决这些问题,已经提出了采用混合有具有高不可逆容量的添加剂(例如Li2O2)的正极来制造电池的方法。然而,当Li2O2通过首次充电分解以释放氧气时,在该位置产生孔隙,并且由于这些孔隙的产生,在首次充电后正极的密度降低,从而导致电池的能量密度降低的问题。
发明内容
[技术问题]
因此,本发明致力于解决当使用将高容量不可逆添加剂与正极活性材料混合的正极时出现的问题,并且本公开的目的是提供一种锂二次电池用正极以及包含其的锂二次电池,其中,在正极集电体中,高容量不可逆材料仅涂覆在未涂覆活性材料层而形成的突出的未涂覆部上。
[技术方案]
根据本公开的一个方面,提供了一种锂二次电池用正极,其包括正极集电体和在所述正极集电体的至少一个表面上涂覆并形成的正极活性材料层,其中,所述正极集电体包括未涂覆正极活性材料层的突出的未涂覆部,并且其中,在所述未涂覆部上涂覆有由锂氧化物组成的不可逆材料。
此时,在包含所述锂二次电池用正极的锂二次电池的首次充电后,所述不可逆材料可以消失。
不可逆材料可以是Li2O2、Li2O或其混合物。
同时,根据本公开的另一方面,提供了一种锂二次电池,其包括:电极组件,其包括正极、负极和位于正极和负极之间的隔膜;用于浸渍所述电极组件的非水性电解液;以及包含所述电极组件和所述非水电解液的电池壳体,其中,所述正极是本公开的上述锂二次电池用正极。
这里,负极可以包括硅(Si)基材料作为负极活性材料。
硅基材料可以是:硅-硅氧化物复合材料;硅合金;或硅氧化物复合材料和硅合金。
此外,根据本公开,提供了一种包括本公开的锂二次电池作为单元电池的电池模组(battery module)以及包含其的电池组(battery pack),以及包括该电池组作为电源的装置。
这里,装置可以是电动车辆、混合动力电动车辆、插电式混合动力电动车辆或储能系统。
[有益效果]
根据本公开,在正极集电体的未涂覆部上涂覆由锂氧化物组成的不可逆材料,因此可以增加电池的能量密度。
特别地,由于不可逆材料仅涂覆在正极集电体的未涂覆部上,因此可以解决在现有技术的混合有不可逆添加剂的正极中可能出现的空隙生成问题,以及电池的能量密度降低现象。
附图说明
附图示出了本公开的优选实施方式,并且与详细描述一起,用于提供对本公开的技术精神的进一步理解。然而,本公开不应被解释为局限于附图。另一方面,为了突出更明确的说明,本说明书中所收录的附图中的要素的形状、尺寸、比例尺或比例可以夸大。
图1a和1b分别示意性地示出了常规正极的平面图和侧视图。
图2a和2b分别示意性地示出了本公开的实施方式的正极的平面图和侧视图。
图3示意性地示出了本公开的实施方式的充电后的正极的侧视图。
具体实施方式
应当理解,在本说明书和所附权利要求书中使用的术语或词语不应被解释为局限于一般和词典含义,而是基于发明人可以适当地定义术语以最佳地解释本发明的原则,将其解释为与本公开的技术方面相对应的含义和概念。因此,本说明书中公开的实施方式和附图中示出的结构仅仅是本公开的最优选实施方式,它们并不代表本公开的所有技术构思,因此,应该理解,在提交本申请时可存在能够替代它们的各种等同物和变形例。
为了开发满足工业需要的高能量锂二次电池,需要使用其中应用硅基材料作为负极活性材料的负极。然而,由于这种负极具有高的不可逆容量并因此具有低的充电/放电效率,因此已使用混合有高容量不可逆添加剂的正极来解决这些问题。
图1a和1b分别示意性地示出了常规正极的平面图和侧视图。根据所述图,将高容量不可逆添加剂混合在形成于正极集电体11上的正极活性材料层12中。通过首次充电,分散在正极活性材料层12内的高容量不可逆添加剂分解,从而在该位置产生空隙。结果,正极活性材料层12的密度降低,最终,电池的能量密度降低。
在本公开中,通过仅在正极集电体的未涂覆部上涂覆不可逆材料,而不是将正极活性材料和高容量不可逆添加剂混合,可以解决现有技术的问题。
图2a和2b分别示意性地示出了本公开的实施方式的正极的平面图和侧视图。图3示意性地示出了本公开的实施方式的充电后的正极的侧视图。
现将参考所述附图更详细地描述本公开。锂二次电池用正极100包括正极集电体110和在正极集电体110的至少一个表面上涂覆并形成的正极活性材料层120,其中,正极集电体110包括未涂覆有正极活性材料层120的突出的未涂覆部130,并且其中,在未涂覆部130上涂覆有由锂氧化物组成的不可逆材料140。
由于由锂氧化物组成的不可逆材料140仅涂覆在未涂覆部130上并且未包含在正极活性材料层120中,因此不需要将正极活性材料和不可逆材料混合的过程。特别地,由锂氧化物组成的不可逆材料140在包含锂二次电池用正极100的锂二次电池的首次充电后消失。因此,在首次充电后,其以未涂覆部130上没有涂层的形式存在。此时,由锂氧化物组成的不可逆材料140可以分解成锂离子和氧气并消失。
此时,不可逆材料可以是Li2O2、Li2O或其混合物。
不可逆材料140可以在溶解于有机溶剂中的状态下仅涂覆在未涂覆部130上,然后干燥。可以将不可逆材料在正极活性材料层120上涂覆至相应的厚度,例如10至300μm,或50至250μm,然后干燥以去除有机溶剂。
当将不可逆材料140涂覆并干燥至这样的厚度时,即使在将硅基材料用于负极的情况下,也可以有效地抵消两个电极的不可逆容量的不平衡,同时可以减少正极特性的劣化。
同时,包含在正极活性材料层中的正极活性材料可以包括由以下化学式1或2表示的锂过渡金属氧化物。
LixMyMn1-yO2-zAz (1)
其中,M是选自由Al、Mg、Ni、Co、Fe、Cr、V、Ti、Cu、B、Ca、Zn、Zr、Nb、Mo、Sr、Sb、W、Ti和Bi组成的组的至少一种元素;
A是-1或-2或更高价的阴离子;
0.9≤x≤1.2,0<y<1,并且0≤z<0.2。
(1-x)LiM’O2-yAy-xLi2MnO3-y’Ay’ (2)
其中,M’是MnaMb;
M是选自由Ni、Ti、Co、Al、Cu、Fe、Mg、B、Cr、Zr、Zn和第二过渡系过渡金属组成的组的至少一种;
A是选自由阴离子(例如PO4、BO3、CO3、F和NO3)组成的组的至少一种;
0<x<1,0<y≤0.02,0<y’≤0.02,0.5≤a≤1.0,0≤b≤0.5,a+b=1。
同时,正极活性材料层还可包含粘合剂和导电材料。
此外,通过将电极合剂(正极活性材料、导电材料和粘合剂的混合物)涂覆在正极集电体的除未涂覆部之外的部分上来制造正极,并且需要时可以进一步向混合物中添加填料。
除了由化学式1或2表示的锂过渡金属氧化物之外,正极活性材料可包括:层状化合物,例如锂钴氧化物(LiCoO2)或锂镍氧化物(LiNiO2)或取代有一种以上过渡金属的化合物;锂锰氧化物,例如式Li1+xMn2-xO4(其中,x为0至0.33)、LiMnO3、LiMn2O3和LiMnO2;锂铜氧化物(Li2CuO2);钒氧化物,例如LiV3O8、LiFe3O4、V2O5和Cu2V2O7;由式LiNi1-xMxO2(其中,M=Co、Mn、Al、Cu、Fe、Mg、B或Ga,x=0.01至0.3)表示的Ni位型锂镍氧化物;由式LiMn2-xMxO2(其中M=Co、Ni、Fe、Cr、Zn或Ta,x=0.01至0.1)或Li2Mn3MO8(其中,M=Fe、Co、Ni、Cu或Zn)表示的锂锰复合氧化物;由LiNixMn2-xO4表示的具有尖晶石结构的锂锰复合氧化物;其中的一些Li原子被碱土金属离子取代的LiMn2O4;二硫化物;和Fe2(MoO4)3等,但不限于此。
正极集电体通常制造成具有3至500μm的厚度。这种正极集电体没有特别限制,只要其具有高导电性且不引起电池中的任何化学变化即可。例如,可以使用不锈钢、铝、镍、钛、煅烧碳,或用碳、镍、钛或银等表面处理的铝或不锈钢材料。集电体可在其表面上形成微观不规则物以增加正极活性材料的粘附强度,并且其可以以各种形状使用,例如膜、片、箔、网、多孔体、泡沫和无纺布等。
基于包含正极活性材料的混合物的总重量,导电材料的添加量通常为1重量%至50重量%。导电材料没有特别限制,只要其具有导电性且不引起电池中的任何化学变化即可。作为导电材料,可以使用例如:石墨,例如天然石墨或人造石墨;炭黑,例如炭黑、乙炔黑、科琴黑、槽黑、炉黑、灯黑或夏黑;导电纤维,例如碳纤维或金属纤维;金属粉末,例如氟化碳粉末、铝粉末或镍粉末;导电晶须,例如氧化锌或钛酸钾;导电金属氧化物,例如氧化钛;或聚亚苯基衍生物。
此外,粘合剂是辅助活性材料与导电材料等之间的粘合以及对集电体的粘合的成分,并且基于包含正极活性材料的混合物的总重量,粘合剂的添加量通常为1重量%至50重量%。这些粘合剂的实例包括聚偏二氟乙烯、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-二烯三元共聚物(EPDM)、磺化EPDM、丁苯橡胶、氟橡胶和各种共聚物。
此外,可选地使用填料作为抑制正极膨胀的成分。填料没有特别限制,只要其是不引起电池中的化学变化的纤维状材料即可。填料的实例包括:烯烃类聚合物,例如聚乙烯和聚丙烯;以及纤维状材料,例如玻璃纤维和碳纤维。
正极活性材料层可以通过将包含上述各成分的电极合剂以浆料的状态涂覆在集电体上并干燥来制造。
更具体地,这种活性材料层可以通过将上述合剂涂覆至10至300μm或50至250μm的厚度然后将其干燥以去除有机溶剂而形成,从而表现出适当的特性。
同时,根据本公开的另一方面,锂二次电池包括:电极组件,其包括正极、负极和位于正极和负极之间的隔膜;用于浸渍电极组件的非水性电解液;以及包含电极组件和非水性电解液的电池壳体,其中,正极是如上所述的本发明的正极。
此时,负极可以包括硅(Si)基材料作为负极活性材料,并且这种硅基材料可以是硅-硅氧化物复合材料和/或硅合金。硅基材料的更具体实例包括选自由SiOx(0≤x<2)、纯Si和Si合金组成组的至少一种。
此外,负极活性材料还可包括碳基材料,并且基于负极活性材料的总重量,碳基材料的含量可以为70重量%以上且99.9重量%以下。并且,碳基材料可以是选自由结晶人造石墨、结晶天然石墨、无定形硬碳、低结晶软碳、炭黑、乙炔黑、科琴黑、Super-P、石墨烯和纤维状碳组成的组的至少一种。特别地,其可以是结晶人造石墨和/或结晶天然石墨。
另一方面,除了碳基材料和硅基材料之外,负极活性材料可以包括:金属复合氧化物,例如LixFe2O3(0≤x≤1)、LixWO2(0≤x≤1)、SnxMe1-xMe’yOz(Me:Mn,Fe,Pb,Ge;Me’:Al,B,P,Si,1、2和3族元素,卤素;0<x≤1;1≤y≤3;1≤z≤8);锂金属;锂合金;硅基合金;锡基合金;金属氧化物,例如SnO、SnO2、PbO、PbO2、Pb2O3、Pb3O4、Sb2O3、Sb2O4、Sb2O5、GeO、GeO2、Bi2O3、Bi2O4和Bi2O5;导电聚合物,例如聚乙炔;Li-Co-Ni基材料;钛氧化物;和锂钛氧化物等,但不限于此。
此外,构成负极的负极集电体通常制造成具有3至500μm的厚度。这种负极集电体没有特别限制,只要其具有高导电性且不引起电池中的任何化学变化即可。例如,可以使用铜、不锈钢、铝、镍、钛、煅烧碳,用碳、镍、钛或银等表面处理的铜或不锈钢材料,和铝-镉合金等。此外,与正极集电体类似,负极集电体可在其表面上形成微观不规则物以增加负极活性材料的粘附力,并且其可以以各种形状使用,例如膜、片、箔、网、多孔体、发泡体、无纺布等。
同时,隔膜位于正极和负极之间,并且使用具有高离子渗透性和机械强度的绝缘薄膜。隔膜的孔径通常为0.01至10μm,并且其厚度通常为5至300μm。作为隔膜的实例,例如,可以使用:烯烃类聚合物,例如聚丙烯,其具有耐化学性和疏水性;由玻璃纤维或聚乙烯等制成的片材或无纺布。当固体电解质(例如聚合物)用作电解质时,固体电解质也可以充当隔膜。
非水性电解液由非水性电解质和锂盐组成。作为非水性电解质,使用非水性有机溶剂、有机固体电解质、无机固体电解质等,但是本公开不限于此。
作为非水性有机溶剂的实例,可提及非质子有机溶剂,例如N-甲基-2-吡咯烷酮、碳酸亚丙酯、碳酸亚乙酯、碳酸亚丁酯、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、碳酸亚丙酯衍生物、四氢呋喃衍生物、醚、丙酸甲酯和丙酸乙酯。
此外,有机固体电解质的实例包括聚乙烯衍生物、聚环氧乙烷衍生物,聚环氧丙烷衍生物、磷酸酯聚合物、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。
此外,无机固体电解质的实例包括锂(Li)的氮化物、卤化物和硫酸盐,例如Li3N、LiI、Li5NI2、Li3N-LiI-LiOH、LiSiO4、LiSiO4-LiI-LiOH、Li2SiS3、Li4SiO4、Li4SiO4-LiI-LiOH和Li3PO4-Li2S-SiS2。
此外,锂盐是易溶于非水性电解质的材料。其实例包括但不限于LiCl、LiBr、LiI、LiClO4、LiBF4、LiB10Cl10、LiPF6、LiCF3SO3、LiCF3CO2、LiAsF6、LiSbF6、LiAlCl4、CH3SO3Li、(CF3SO2)2NLi、氯硼烷锂、低级脂肪族羧酸锂、四苯基硼酸锂和亚胺化物等。
另外,为了改善充电/放电特性和阻燃性,可以将例如吡啶、亚磷酸三乙酯、三乙醇胺、环醚、乙二胺、正甘醇二甲醚、六磷酸三酰胺、硝基苯衍生物、硫、醌亚胺染料、N-取代的噁唑烷酮、N,N-取代的咪唑烷、乙二醇二烷基醚、铵盐、吡咯、2-甲氧基乙醇或三氯化铝等添加到含锂盐的非水性电解质中。如果需要,为了赋予不燃性,电解质还可以包括含卤素的溶剂,例如四氯化碳和三氟化乙烯。此外,为了提高高温储存性,电解质还可以包含二氧化碳气体,并且还可以包括氟代碳酸亚乙酯(FEC)和丙烯磺酸内酯(PRS)等。
在一个具体实例中,将诸如LiPF6、LiClO4、LiBF4和LiN(SO2CF3)2等锂盐添加到作为高介电溶剂的环式碳酸酯EC或PC与作为低粘度溶剂的线性碳酸酯DEC、DMC或EMC的混合溶剂中,由此制备含有锂盐的非水性电解质。
同时,根据本公开的另一方面,提供一种包括所述锂二次电池作为单元电池的电池模组、包含该电池模组的电池组以及包括该电池组作为电源的装置。
这里,装置的实例可以是电动车辆、混合动力电动车辆、插电式混合动力电动车辆或储能系统,但不限于此。
在下文中,将通过实施例详细描述本公开以帮助理解本公开。然而,根据本公开的实施例可以以各种不同的形式修改,并且应当理解,本公开范围的解释不限于以下实施例。本公开的实施例是为了向本领域普通技术人员最佳地解释而提供的。
实施例1
(1)正极合剂的制备
将正极活性材料Li(Ni0.8Co0.1Mn0.1)O2、导电材料(炭黑,商品名:Super C65,Timcal)和粘合剂(PVDF,商品名:KF1100,Kureha)以80:8:12的重量比混合,并在研钵中干混,以制备实施例1的正极合剂。
(2)正极的制备
将有机溶剂(NMP)添加到实施例1的正极合剂中以形成浆料相,然后将其在铝集电体上涂覆至200μm的厚度,并在120℃的真空烘箱中真空干燥12小时。
然后,将过氧化锂(L2O2)和有机溶剂(NMP)的混合溶液(在100重量%的混合溶液总重量中,L2O2的含量为80重量%)涂覆在集电体的未涂覆部上至200μm的厚度,并在120℃的真空烘箱中真空干燥12小时。结果,获得实施例1的正极。
(3)锂二次电池的制备
将重量比为15:85的硅基活性材料SiO和人造石墨的负极活性材料混合物、导电材料(炭黑,商品名:Super C65,Timcal)、粘合剂(SBR,商品名A544,ZEON)和增稠剂(CMC,Daicell 2200,Daicell)以94.2:2:2.5:1.3的重量比混合,并干混以制备负极合剂。
将有机溶剂(NMP)添加到实施例1的负极合剂中以形成浆料相,然后将其涂覆在铜集电体上并在150℃的真空烘箱中真空干燥12小时。由此制备负极。
在所制备的负极和正极之间为厚度为9μm且孔隙率为42vol的由PP/PE材料制成的隔膜,将它们插入电池容器中,并将电解液注入其中。根据常规的制造方法,以2032全电池的形式制造锂二次电池。
作为电解液,使用将1M(LiPF6)溶解在体积比为1:2:1的EC:DMC:DEC混合溶剂中(EC:DMC:DEC=1:2:1(v/v/v)中的1M LiPF6)得到的电解液。
比较例1
(1)正极合剂的制备
将正极活性材料Li(Ni0.8Co0.1Mn0.1)O2、过氧化锂(Li2O2)、导电材料(炭黑,商品名:Super C65,Timcal)和粘合剂(PVDF,商品名:KF1100,Kureha)以64:16:8:12的重量比混合,并在研钵中干混,以制备比较例1的正极合剂。
(2)正极的制备
将有机溶剂(NMP)添加到比较例1的正极合剂中以形成浆料相,然后将其涂覆在铝集电体上并在120℃的真空烘箱中真空干燥12小时。结果,获得比较例1的正极。
(3)正极和锂二次电池的制备
使用比较例1的正极代替实施例1的正极,并且其余操作以与实施例1中相同的方式进行,以制备正极和锂二次电池。
实验例1:电池的初始充电和放电特性的评价I
在室温下在以下条件下评价实施例1和比较例1的电池的初始充电和放电特性。
充电:0.01C,CC/CV,4.6V,5%截止
放电:0.01C,CC,2.5V,截止
作为该评价的结果,确认了实施例1的初始充电容量为904mAh/g,比较例1的初始充电容量为254mAh/g。
在比较例1和实施例1中,总体上可将过氧化锂(Li2O2)应用到正极上以补偿负极的不可逆添加剂容量。
过氧化锂(Li2O2)是理论上能够基于以下反应式1以每摩尔过氧化锂(Li2O2)不可逆地释放出2摩尔锂离子和1摩尔氧气的化合物。
[反应式1]Li2O2→2Li++O2
然而,根据初始充电容量评价结果,可以确认,在例如4.3V以上的高电压范围内,与将过氧化锂(Li2O2)与正极活性材料混合的状态涂覆的比较例1相比,将过氧化锂(Li2O2)涂覆在未涂覆部上的实施例1的电池具有更高的正极初始充电容量。
在实施例1中,由于在未涂覆部中进行过氧化锂(Li2O2)的还原分解反应,其并不影响正极活性材料层(即,在正极活性材料层内不形成空隙),并且随着未涂覆部上的涂层的消失而终止。因此,正极活性材料层的电极密度损失和整个电池的能量密度降低可以为零或非常小。
相反,在比较例1中,由于在正极活性材料层中发生过氧化锂(Li2O2)的还原分解反应,因此在正极活性材料层中形成了空隙,并且可能发生电极密度的降低和能量密度的降低。
结果,与比较例1相比,在实施例1中,有效地抵消了两个电极的不可逆容量的不平衡,同时正极的初始充电容量高,正极的能量密度损失小,并且可以获得优异的寿命特性。
[符号说明]
10、100:锂二次电池用正极
11、110:正极集电体
12、120:正极活性材料层
13、130:未涂覆部
140:不可逆材料。
Claims (13)
1.一种锂二次电池用正极,其包括:正极集电体,和在所述正极集电体的至少一个表面上涂覆并形成的正极活性材料层,
其中,所述正极集电体包括未涂覆所述正极活性材料层的突出的未涂覆部,并且
其中,在所述未涂覆部上涂覆有由锂氧化物组成的不可逆材料;
其中,所述不可逆材料在包含所述锂二次电池用正极的锂二次电池的首次充电后分解成锂离子和氧气并消失。
2.如权利要求1所述的锂二次电池用正极,其中,所述不可逆材料是Li2O2、Li2O或其混合物。
3. 如权利要求1所述的锂二次电池用正极,其中,所述不可逆材料在所述未涂覆部上被涂覆至10至300 μm的厚度。
4.一种锂二次电池,其包括:
电极组件,其包括正极、负极和位于所述正极和所述负极之间的隔膜;
用于浸渍所述电极组件的非水性电解液;以及
包含所述电极组件和所述非水性电解液的电池壳体,
其中,所述正极是权利要求1至3中任一项所述的锂二次电池用正极。
5.如权利要求4所述的锂二次电池,其包括硅(Si)基材料作为负极活性材料。
6.如权利要求5所述的锂二次电池,其中,所述硅基材料是:硅-硅氧化物复合材料;硅合金;或者硅氧化物复合材料和硅合金。
7.一种电池模组,其包括权利要求4所述的锂二次电池作为单元电池。
8.一种电池组,其包括权利要求7所述的电池模组。
9.一种包括权利要求8所述的电池组作为电源的装置。
10.如权利要求9所述的装置,其中,所述装置是电动车辆。
11.如权利要求9所述的装置,其中,所述装置是混合动力电动车辆。
12.如权利要求9所述的装置,其中,所述装置是插电式混合动力电动车辆。
13.如权利要求9所述的装置,其中,所述装置是储能系统。
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