CN112952199B - 一种电解液及包含其的锂离子电池 - Google Patents
一种电解液及包含其的锂离子电池 Download PDFInfo
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
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Abstract
本发明提供一种电解液及包含其的锂离子电池,所述电解液包含电解质、有机溶剂和添加剂,所述添加剂包含添加剂A和添加剂B,所述添加剂A为双氟磺酰亚胺金属盐和双三氟磺酰亚胺金属盐中的至少一种,所述添加剂B为三甲氧基(3,3,3‑三氟丙基)硅烷。本发明的电解液可以提高锂化硅的稳定性和三元正极材料的表面稳定性,从而改善了电池的寿命。
Description
技术领域
本发明属于电池技术领域,涉及一种电解液及包含其的锂离子电池。
背景技术
锂离子电池的被广泛应用于新能源汽车、消费电子产品、储能等各类移动或固定式能量储存场景,这些应用对下一代锂离子电池产品提出了更高的能量密度和寿命要求。业界在努力开发新的阴极材料和阳极材料,而通过提升阳极材料的克容量已被证明可以更为直接的提升电池的能量密度。目前主流的商业阳极材料为石墨,其具有优异的稳定性。但其相对较低的理论容量(372mAh/g)已成为制约锂离子电池能量密度进一步提升的因素。在地球上硅资源丰富,价格低廉,具有很高的理论容量(~3640毫安时/克),具有很好的作为锂离子电池负极材料的潜力。
尽管硅作为负极具有很高的克容量,但其在锂化后体积变化很大,使得固体电解质界面(SEI)容易被破坏而消耗活性锂,带来电池的容量损失。锂化后的硅与负极的粘合剂和电解液成分都具有高的反应活性,进一步减少了活性锂,消耗了电解液中的溶剂,破坏了粘合剂的粘结作用,并生成各种杂质相,导致电池内阻升高,容量下降。与此同时,为了发挥硅负极高克容量的优势,与其搭配的正极材料通常为三元或NCA,这类正极材料中的过渡金属离子在容易溶出到电解液,重新沉积在负极表面,催化生成更厚的SEI膜,消耗活性锂,导致电池容量的损失。
因此,在本领域,期望开发一种可以提高锂化硅的稳定性和三元正极材料的表面稳定性,从而改善电池寿命的电解液。
发明内容
针对现有技术的不足,本发明的目的在于提供一种电解液及包含其的锂离子电池。本发明的电解液可以提高锂化硅的稳定性和三元正极材料的表面稳定性,从而改善了电池的寿命。
为达此目的,本发明采用以下技术方案:
一方面,本发明提供一种电解液,所述电解液包含电解质、有机溶剂和添加剂,所述添加剂包含添加剂A和添加剂B,所述添加剂A为双氟磺酰亚胺金属盐和双三氟磺酰亚胺金属盐中的至少一种,所述添加剂B为三甲氧基(3,3,3-三氟丙基)硅烷。
在本发明中,通过添加剂A中的金属离子在锂离子进入Si材料后,与Si和Li形成Li-M-Si多元化合物(M为金属离子),大大提高了Si负极的稳定性,减少了Si负极与电解液的副反应,从而可以提高电池的库伦效率和循环寿命。电解液添加剂B三甲氧基(3,3,3-三氟丙基)硅烷可以同时在正极和负极表面形成稳定的保护膜,从而提高电池的循环寿命。二者配合,能够更好地提高锂化硅的稳定性和三元正极材料的表面稳定性,从而改善电池的寿命。
在本发明中,所述双氟磺酰亚胺金属盐可以用M(FSI)x表示,其中M为Mg、Ca或Al中的一种,x为2~3,FSI为双氟磺酸亚胺基团。
在本发明中,所述双三氟磺酰亚胺金属盐可以用M(TFSI)x表示,其中M为Mg、Ca或Al中的一种,x为2~3,TFSI为双三氟磺酰亚胺基团。
优选地,所述双氟磺酰亚胺金属盐为如下结构的双氟磺酰亚胺金属盐中的至少一种:
优选地,所述双三氟磺酰亚胺金属盐为如下结构的双三氟磺酰亚胺金属盐中的至少一种:
在本发明中,添加剂B的结构如下:
优选地,所述添加剂A在电解液中的浓度为0.05-0.3mol/L,例如0.05mol/L、0.08mol/L、0.1mol/L、0.15mol/L、0.18mol/L、0.2mol/L、0.25mol/L、0.28mol/L或0.3mol/L。
优选地,所述添加剂B在电解液中的质量百分比浓度为0.002%-3%,例如0.002%、0.005%、0.008%、0.01%、0.05%、0.1%、0.5%、1%、1.5%、2%、2.5%或3%。
优选地,所述电解质为锂盐,所述锂盐优选LiPF6、LiClO4、LiPO2F2、Li2PO3F、LiBF4、LiSO3F、LiTFMSB、LiN(SO2F)2、LiAsF6、LiN(SO2CF3)2、LiN(SO2C2F5)2、LiBOB、LiPFO或四氟[草酸根-O,O’]磷酸锂中的一种或至少两种的组合,进一步优选LiPF6、LiBOB、LiBF4、LiSO3F、LiPO2F2、LiN(SO2CF3)2或LiN(SO2F)2中的一种或至少两种的组合。
优选地,所述电解质在电解液中的浓度为0.5-2mol/L,例如0.5mol/L、0.6mol/L、0.7mol/L、0.8mol/L、0.9mol/L、1mol/L、1.2mol/L、1.5mol/L、1.8mol/L或2mol/L。
本发明所述的有机溶剂的种类没有特别限制,能够实现本发明的技术方案即可。作为例子,所述有机溶剂可选自碳酸乙烯酯、碳酸丙烯酯、碳酸甲乙酯、碳酸丁烯酯、碳酸二甲酯、碳酸二乙酯、氟代碳酸乙烯酯、碳酸二丙酯、1,4-丁内酯、碳酸甲丙酯、碳酸乙丙酯、丙酸甲酯、丁酸甲酯、乙酸乙酯、丙酸乙酯或丁酸乙酯中的一种或至少两种的组合。
优选地,所述有机溶剂在电解液中的质量百分含量为60%~90%,例如60%、63%、65%、68%、70%、75%、78%、80%、85%、88%或90%。
另一方面,本发明提供了一种锂离子电池,所述锂离子电池包括正极、负极、隔离膜以及如上所述的电解液。
优选地,所述正极包含的活性材料选自NCM和/NCA,所述负极包含的活性材料选自Si和石墨的物料复合物。
优选地,所述负极包含的活性材料中Si占复合物的质量百分比为5%-50%,例如5%、8%、10%、13%、15%、18%、20%、25%、28%、30%、35%、38%、40%、45%、48%或50%。
相对于现有技术,本发明具有以下有益效果:
在本发明中,通过添加剂A中的金属离子在锂离子进入Si材料后,与Si和Li形成Li-M-Si多元化合物(M为金属离子),大大提高了Si负极的稳定性,减少了Si负极与电解液的副反应,从而可以提高电池循环寿命。电解液添加剂B三甲氧基(3,3,3-三氟丙基)硅烷可以同时在正极和负极表面形成稳定的保护膜,从而提高电池的循环寿命。二者配合,能够更好地提高锂化硅的稳定性和三元正极材料的表面稳定性,从而改善电池的寿命。
附图说明
图1为对实施例1-3以及对比例1-3的锂离子电池循环寿命测试得到的容量保持率曲线图。
具体实施方式
下面通过具体实施方式来进一步说明本发明的技术方案。本领域技术人员应该明了,所述实施例仅仅是帮助理解本发明,不应视为对本发明的具体限制。
实施例1
配备一种电解液,其中溶剂为碳酸乙烯酯、碳酸丙烯酯、碳酸甲乙酯、碳酸二甲酯四种混合溶剂(混合比例为1.5:1.5:6:1),电解质为锂盐LiPF6,电解质浓度1mol/L,添加剂包含碳酸亚乙烯酯,亚硫酸丙烯酯,添加剂A和添加剂B三甲氧基(3,3,3-三氟丙基)硅烷,添加剂A在电解液中的含量为0.3mol/L,添加剂B在电解液中的质量百分比为0.1%。正极采用NCM材料,负极采用石墨和硅的复合物,其中硅含量为10%。将正极、负极、电解液装配成电芯进行测试。
实施例2
配备一种电解液,其中溶剂为碳酸乙烯酯、碳酸丙烯酯、碳酸甲乙酯、碳酸二甲酯四种混合溶剂(混合比例为1.5:1.5:6:1),电解质为锂盐LiPF6,电解质浓度2mol/L,添加剂包含碳酸亚乙烯酯,亚硫酸丙烯酯,添加剂和添加剂B三甲氧基(3,3,3-三氟丙基)硅烷,添加剂A在电解液中的含量为0.05mol/L,添加剂B在电解液中的质量百分比为0.005%。正极采用NCM材料,负极采用石墨和硅的复合物,其中硅含量为10%。将正极、负极、电解液装配成电芯进行测试。
实施例3
配备一种电解液,其中溶剂为碳酸乙烯酯、碳酸丙烯酯、碳酸甲乙酯、碳酸二甲酯四种混合溶剂(混合比例为1.5:1.5:6:1),电解质为锂盐LiPF6,电解质浓度1mol/L,添加剂包含碳酸亚乙烯酯,亚硫酸丙烯酯,添加剂和添加剂B三甲氧基(3,3,3-三氟丙基)硅烷,添加剂A在电解液中的含量为0.2mol/L,添加剂B在电解液中的质量百分比为1%。正极采用NCM材料,负极采用石墨和硅的复合物,其中硅含量为10%。将正极、负极、电解液装配成电芯进行测试。
对比例1
在该对比例中,与实施例1不同之处仅在于,所述电解液中添加剂不包括添加剂A和添加剂B,其余添加剂用量相同。
对比例2
在该对比例中,与实施例1不同之处仅在于,所述电解液中添加剂不包括添加剂A,添加剂B的含量为3%,其余添加剂用量相同。
对比例3
在该对比例中,与实施例1不同之处仅在于,所述电解液中添加剂不包括添加剂B,添加剂A的含量为0.3mol/L,其余添加剂用量相同。
对实施例1-3以及对比例1-3的锂离子电池循环寿命的表征测试,其测试方法为对装配好的电池做1C/1C倍率的充放电循环,循环寿命=第N圈放电容量/第一圈放电容量。
测试结果如图1所示,由图1可以看出,在添加剂A和添加剂B同时添加到电解液中时,更有利于提高正负极界面的稳定性,对硅基电芯的的常温循环容量保持率有较大的提升。
申请人声明,本发明通过上述实施例来说明本发明的电解液及包含其的锂离子电池,但本发明并不局限于上述实施例,即不意味着本发明必须依赖上述实施例才能实施。所属技术领域的技术人员应该明了,对本发明的任何改进,对本发明产品各原料的等效替换及辅助成分的添加、具体方式的选择等,均落在本发明的保护范围和公开范围之内。
Claims (13)
1.一种电解液,其特征在于,所述电解液包含电解质、有机溶剂和添加剂,所述添加剂包含添加剂A和添加剂B,所述添加剂A为双氟磺酰亚胺金属盐和双三氟磺酰亚胺金属盐中的至少一种,所述添加剂B为三甲氧基(3,3,3-三氟丙基)硅烷;
所述双氟磺酰亚胺金属盐用M(FSI)x表示,其中M为Mg、Ca或Al中的一种,x为2~3,FSI为双氟磺酰亚胺基团;
所述双三氟磺酰亚胺金属盐用M(TFSI)x表示,其中M为Mg、Ca或Al中的一种,x为2~3,TFSI为双三氟磺酰亚胺基团。
4.根据权利要求1所述的电解液,其特征在于,所述添加剂A在电解液中的浓度为0.05-0.3mol/L。
5.根据权利要求1所述的电解液,其特征在于,所述添加剂B在电解液中的质量百分比浓度为0.002%-3%。
6.根据权利要求1所述的电解液,其特征在于,所述电解质为锂盐。
7.根据权利要求6所述的电解液,其特征在于,所述锂盐选自LiPF6、LiClO4、LiPO2F2、Li2PO3F、LiBF4、LiSO3F、LiTFMSB、LiN(SO2F)2、LiAsF6、LiN(SO2CF3)2、LiN(SO2C2F5)2、LiBOB、LiPFO或四氟[草酸根-O,O’]磷酸锂中的一种或至少两种的组合。
8.根据权利要求7所述的电解液,其特征在于,所述锂盐选自LiPF6、LiBOB、LiBF4、LiSO3F、LiPO2F2、LiN(SO2CF3)2或LiN(SO2F)2中的一种或至少两种的组合。
9.根据权利要求1所述的电解液,其特征在于,所述电解质在电解液中的浓度为0.5-2mol/L。
10.根据权利要求1所述的电解液,其特征在于,所述有机溶剂选自碳酸乙烯酯、碳酸丙烯酯、碳酸甲乙酯、碳酸丁烯酯、碳酸二甲酯、碳酸二乙酯、氟代碳酸乙烯酯、碳酸二丙酯、1,4-丁内酯、碳酸甲丙酯、碳酸乙丙酯、丙酸甲酯、丁酸甲酯、乙酸乙酯、丙酸乙酯或丁酸乙酯中的一种或至少两种的组合。
11.根据权利要求1所述的电解液,其特征在于,所述有机溶剂在电解液中的质量百分含量为60%~90%。
12.一种锂离子电池,其特征在于,所述锂离子电池包括正极、负极、隔离膜以及如权利要求1-11中任一项所述的电解液;
所述正极包含的活性材料选自NCM或NCA,所述负极包含的活性材料选自Si和石墨的物料复合物。
13.根据权利要求12所述的锂离子电池,其特征在于,所述负极包含的活性材料中Si占复合物的质量百分比为5%-50%。
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