CN112751080B - 用于可再充电锂电池的电解质和可再充电锂电池 - Google Patents
用于可再充电锂电池的电解质和可再充电锂电池 Download PDFInfo
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- CN112751080B CN112751080B CN202011153536.9A CN202011153536A CN112751080B CN 112751080 B CN112751080 B CN 112751080B CN 202011153536 A CN202011153536 A CN 202011153536A CN 112751080 B CN112751080 B CN 112751080B
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- lithium battery
- active material
- rechargeable lithium
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- 229910052793 cadmium Inorganic materials 0.000 description 1
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- STASIHJVWFOIGF-UHFFFAOYSA-N carbonic acid;1-nitroethene Chemical compound OC(O)=O.[O-][N+](=O)C=C STASIHJVWFOIGF-UHFFFAOYSA-N 0.000 description 1
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- QWTKOKXIYQZOTL-UHFFFAOYSA-N phenoxycarbonylphosphonic acid Chemical compound OP(O)(=O)C(=O)OC1=CC=CC=C1 QWTKOKXIYQZOTL-UHFFFAOYSA-N 0.000 description 1
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Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- 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
- H01M10/0567—Liquid materials characterised by the additives
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07F—ACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
- C07F9/00—Compounds containing elements of Groups 5 or 15 of the Periodic Table
- C07F9/02—Phosphorus compounds
- C07F9/28—Phosphorus compounds with one or more P—C bonds
- C07F9/38—Phosphonic acids [RP(=O)(OH)2]; Thiophosphonic acids ; [RP(=X1)(X2H)2(X1, X2 are each independently O, S or Se)]
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07F—ACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
- C07F9/00—Compounds containing elements of Groups 5 or 15 of the Periodic Table
- C07F9/02—Phosphorus compounds
- C07F9/28—Phosphorus compounds with one or more P—C bonds
- C07F9/38—Phosphonic acids [RP(=O)(OH)2]; Thiophosphonic acids ; [RP(=X1)(X2H)2(X1, X2 are each independently O, S or Se)]
- C07F9/3804—Phosphonic acids [RP(=O)(OH)2]; Thiophosphonic acids ; [RP(=X1)(X2H)2(X1, X2 are each independently O, S or Se)] not used, see subgroups
- C07F9/3826—Acyclic unsaturated acids
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07F—ACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
- C07F9/00—Compounds containing elements of Groups 5 or 15 of the Periodic Table
- C07F9/02—Phosphorus compounds
- C07F9/28—Phosphorus compounds with one or more P—C bonds
- C07F9/38—Phosphonic acids [RP(=O)(OH)2]; Thiophosphonic acids ; [RP(=X1)(X2H)2(X1, X2 are each independently O, S or Se)]
- C07F9/3804—Phosphonic acids [RP(=O)(OH)2]; Thiophosphonic acids ; [RP(=X1)(X2H)2(X1, X2 are each independently O, S or Se)] not used, see subgroups
- C07F9/3886—Acids containing the structure -C(=X)-P(=X)(XH)2 or NC-P(=X)(XH)2, (X = O, S, Se)
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- 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
- H01M10/052—Li-accumulators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- 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
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/364—Composites as mixtures
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- H01M4/00—Electrodes
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/366—Composites as layered products
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/386—Silicon or alloys based on silicon
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
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Abstract
用于可再充电锂电池的电解质和包括该电解质的可再充电锂电池,该电解质包括非水性有机溶剂;锂盐;和添加剂,其中添加剂包括由化学式1表示的化合物:[化学式1]在化学式1中,R1为氰基、取代的或未取代的C2至C10烯基或取代的或未取代的C2至C10炔基。
Description
技术领域
实施方式涉及用于可再充电锂电池的电解质和包括其的可再充电锂电池。
背景技术
可再充电锂电池可以再充电并且可具有铅蓄电池、镍镉电池、镍氢电池或镍锌电池等的三倍或更多倍高的每单位重量的能量密度,并且可高度充电且可在商业上被制造用于笔记本电脑、手机、电动工具和电动自行车等。已经考虑了能量密度的额外改善。
通过将电解质注入到电池单电池中制造可再充电锂电池,该电池单电池包括含有能够嵌入/脱嵌锂离子的正极活性物质的正电极和含有能够嵌入/脱嵌锂离子的负极活性物质的负电极。
发明内容
可通过提供用于可再充电锂电池的电解质来实现实施方式,电解质包括非水性有机溶剂;锂盐;和添加剂,其中添加剂包括由化学式1表示的化合物:
[化学式1]
在化学式1中,R1为氰基、取代的或未取代的C2至C10烯基或取代的或未取代的C2至C10炔基。
R1可为氰基、取代的或未取代的C2至C4烯基或取代的或未取代的C2至C4炔基。
R1可为氰基、乙烯基、丙烯基、乙炔基或丙炔基。
由化学式1表示的化合物可由化学式1A表示:
[化学式1A]
基于电解质的总重,由化学式1表示的化合物的含量可为约0.1wt%至约10wt%。
基于电解质的总重,由化学式1表示的化合物的含量可为约0.2wt%至约2.0wt%。
可通过提供可再充电锂电池来实现实施方式,可再充电锂电池包括:含有正极活性物质的正电极;含有负极活性物质的负电极;和根据实施方式的电解质。
正极活性物质可包括锂与钴、锰、镍或其组合的复合氧化物。
正极活性物质可由化学式4表示:
[化学式4]
Lix1M1 1-y1-z1M2 y1M3 z1O2
在化学式4中,x1、y1和z1可满足下述关系:0.9≤x1≤1.8,0≤y1≤1,0≤z1≤1,和0≤y1+z1≤1,且M1、M2和M3可各自独立地为Ni、Co、Mn、Al、Sr、Mg、La或其组合。
正极活性物质可由化学式5表示:
[化学式5]
Lix2Niy2Coz2Al1-y2-z2O2
在化学式5中,x2、y2和z2可满足下述关系:1≤x2≤1.2,0.6≤y2≤1,和0≤z2≤0.5(例如,0≤z2≤0.4或0≤z2<0.4)。
负极活性物质可包括含有Si活性物质和碳活性物质的Si-C复合材料。
负极活性物质可进一步包括结晶碳。
结晶碳可包括石墨,且石墨可包括天然石墨、人造石墨或其混合物。
Si-C复合材料可进一步包括壳,壳围绕Si-C复合材料的表面,且壳可包括非晶碳。
非晶碳可包括软碳、硬碳、中间相沥青碳化产物、煅烧焦炭或其混合物。
附图说明
通过参考附图详细地描述示例性实施方式,特征将对本领域技术人员来说是显而易见的,其中:
图1为根据实施方式的可再充电锂电池的分解透视图。
图2为当使用根据实施例1的电解质时形成在负电极的表面上的SEI膜的SEM图像。
图3为当使用根据比较例1的电解质时形成在负电极的表面上的SEI膜的SEM图像。
图4显示根据合成例的添加剂化合物的P-NMR谱。
具体实施方式
现在将在下文参考附图更充分描述示例实施方式;然而,它们可以以不同的形式来体现,并且不应被解释为限于本文阐述的实施方式。相反,提供这些实施方式使得本公开将是透彻和完整的,并且将向本领域技术人员充分传达示例性实施。
在附图中,为了图示的清楚起见,可放大层和区域的尺寸。还将理解,当层或元件被称为“在”另一个层或元件“上”时,它可直接在另一个层或元件上,或者也可存在中间层或元件。此外,还将理解,当层被称为“在”两个层“之间”时,它可为两个层之间的唯一层,或者也可存在一个或多个中间层。相同的附图标记通篇指相同的元件。
如本文使用的,当不另外提供定义时,“取代的”指化合物的氢被选自下述中的取代基替代:卤素原子(F、Br、Cl或I)、羟基、硝基、氰基、氨基、叠氮基、脒基、肼基、腙基、羰基、氨甲酰基、巯基、酯基、羧基或其盐、磺酸基或其盐、磷酸基或其盐、C1至C20烷基、C2至C20烯基、C2至C20炔基、C6至C30芳基、C7至C30芳基烷基、C1至C4烷氧基、C1至C20杂烷基、C3至C20杂芳基烷基、C3至C30环烷基、C3至C15环烯基、C6至C15环炔基、C2至C20杂环烷基和其组合。
下文描述根据实施方式的用于可再充电锂电池的电解质。
根据实施方式的用于可再充电锂电池的电解质可包括非水性有机溶剂、锂盐和添加剂。在实施中,添加剂可包括例如由化学式1表示的化合物。
[化学式1]
在化学式1中,R1可为或可包括例如氰基、取代的或未取代的C2至C10烯基或取代的或未取代的C2至C10炔基。
由化学式1表示的化合物(包括在根据实施方式的添加剂中)包括分子内部的锂源,且可在负电极的表面上被还原并在其上形成具有优异的离子导电性的强的固体电解质界面(SEI)膜。因此,由于初始形成的固体电解质界面(SEI)膜而可抑制在高温循环操作期间负电极表面的分解,并且因此可减小可再充电锂电池中的电阻增加率。
与包括一个–OLi的化合物相比,在实施中,其中包括两个–OLi作为锂源,并且化合物可具有改善高倍率性能的效果。
在实施中,具有不饱和键的官能团可包括在一个分子中,且可有助于引起包含锂源的化合物的聚合,且SEI膜可更牢固地形成在负电极的表面上。
形成在负电极的表面上的SEI膜的实施方式可见于图2中。
图2为当使用根据实施例1的电解质时形成在负电极的表面上的SEI膜的SEM图像。
图3为当使用根据比较例1的电解质时形成在负电极的表面上的SEI膜的SEM图像。
参考图2和图3,当使用包括根据实施方式的添加剂的电解质时,强的(例如,固体)SEI膜可形成在负电极的表面上(图2)。当使用不包括添加剂的电解质时,裂纹可发生在负电极的表面上(图3)。
在实施中,化学式1中的R1可为例如氰基、取代的或未取代的C2至C4烯基或取代的或未取代的C2至C4炔基。
随着含有不饱和键的官能团的碳数更少,聚合物可变得更致密,可再充电锂电池的电阻增加率可减少,并且可改善其在高温下存储期间的稳定性。
在实施中,化学式1中的R1可为例如氰基、乙烯基、丙烯基、乙炔基或丙炔基。
根据实施方式的添加剂,例如,由化学式1表示的化合物,可包括例如由化学式1A表示的化合物。
[化学式1A]
在实施中,基于用于可再充电锂电池的电解质的总重,由化学式1表示的化合物的含量可为例如约0.1wt%至约10wt%,约0.1wt%至约5.0wt%,或约0.2wt%至约2.0wt%,或约0.2wt%至约1.5wt%。
当在上述范围内包括由化学式1表示的化合物时,可实现(通过防止在高温下电阻的增加)具有改善的循环寿命特性的可再充电锂电池,并且同时,可改善可再充电锂电池的高温性能。
如果由化学式1表示的化合物的量小于约0.1wt%,则高温存储特性可劣化,并且如果其大于约10wt%,则循环寿命可由于界面电阻的增加而减少。
非水性有机溶剂可用作用于传输参与电池的电化学反应的离子的介质。
非水性有机溶剂可包括例如碳酸酯溶剂、酯溶剂、醚溶剂、酮溶剂、醇溶剂或非质子溶剂。
碳酸酯溶剂可包括例如碳酸二甲酯(DMC)、碳酸二乙酯(DEC)、碳酸二丙酯(DPC)、碳酸甲丙酯(MPC)、碳酸乙丙酯(EPC)、碳酸甲乙酯(MEC)、碳酸亚乙酯(EC)、碳酸亚丙酯(PC)或碳酸亚丁酯(BC)等。酯溶剂可包括例如乙酸甲酯、乙酸乙酯、乙酸正丙酯、乙酸二甲酯、丙酸甲酯、丙酸乙酯、丙酸丙酯、γ-丁内酯、癸内酯、戊内酯、甲羟戊酸内酯或己内酯等。醚溶剂可包括例如二丁醚、四甘醇二甲醚、二甘醇二甲醚、二甲氧基乙烷、2-甲基四氢呋喃或四氢呋喃等。酮溶剂可包括例如环己酮等。醇溶剂包括例如乙醇或异丙醇等。非质子溶剂可包括,例如腈比如R-CN(其中R为C2至C20直链、支链或环状烃基、双键、芳族环或醚键),酰胺比如二甲基甲酰胺,或二氧戊环比如1,3-二氧戊环,或环丁砜等。
非水性有机溶剂可单独使用或以混合物使用。当非水性有机溶剂以混合物使用时,它们的混合比可按照期望的电池性能来控制。
碳酸酯溶剂可通过混合环状碳酸酯和直链碳酸酯来制备。环状碳酸酯和直链碳酸酯可以以约1:1至约1:9的体积比混合在一起。当混合物用作电解质时,其可具有增强的性能。
除了碳酸酯溶剂之外,非水性有机溶剂可进一步包括芳族烃溶剂。碳酸酯溶剂和芳族烃溶剂可以以约1:1至约30:1的体积比混合在一起。
芳族烃溶剂可为由化学式2表示的芳族烃化合物。
[化学式2]
在化学式2中,R2至R7可各自独立地为例如氢、卤素、C1至C10烷基、卤代烷基或其组合。
芳族烃溶剂的实例可包括苯、氟苯、1,2-二氟苯、1,3-二氟苯、1,4-二氟苯、1,2,3-三氟苯、1,2,4-三氟苯、氯苯、1,2-二氯苯、1,3-二氯苯、1,4-二氯苯、1,2,3-三氯苯、1,2,4-三氯苯、碘苯、1,2-二碘苯、1,3-二碘苯、1,4-二碘苯、1,2,3-三碘苯、1,2,4-三碘苯、甲苯、氟甲苯、2,3-二氟甲苯、2,4-二氟甲苯、2,5-二氟甲苯、2,3,4-三氟甲苯、2,3,5-三氟甲苯、氯甲苯、2,3-二氯甲苯、2,4-二氯甲苯、2,5-二氯甲苯、2,3,4-三氯甲苯、2,3,5-三氯甲苯、碘甲苯、2,3-二碘甲苯、2,4-二碘甲苯、2,5-二碘甲苯、2,3,4-三碘甲苯、2,3,5-三碘甲苯、二甲苯和其组合。
电解质可进一步包括碳酸亚乙烯酯或由化学式3表示的碳酸亚乙酯化合物以有助于改善循环寿命。
[化学式3]
在化学式3中,R8和R9可各自独立地为例如氢、卤素、氰基(CN)、硝基(NO2)或C1至C5氟烷基。在实施中,R8和R9中的至少一个可为卤素、氰基(CN)、硝基(NO2)或C1至C5氟烷基,且R8和R9不同时为氢。
碳酸亚乙酯化合物的实例可包括二氟代碳酸亚乙酯、氯代碳酸亚乙酯、二氯代碳酸亚乙酯、溴代碳酸亚乙酯、二溴代碳酸亚乙酯、硝基碳酸亚乙酯、氰基碳酸亚乙酯和氟代碳酸亚乙酯。用于改善循环寿命的添加剂的量可在适当的范围内使用。
锂盐可溶解在非水性有机溶剂中,可供应给电池锂离子,可基本地操作可再充电锂电池,且可有助于改善锂离子在正电极和负电极之间的传输。锂盐的实例可包括LiPF6、LiBF4、LiSbF6、LiAsF6、LiN(SO2C2F5)2、Li(CF3SO2)2N、LiN(SO3C2F5)2、Li(FSO2)2N(双(氟磺酰基)酰亚胺锂:LiFSI)、LiC4F9SO3、LiClO4、LiAlO2、LiAlCl4、LiN(CxF2x+1SO2)(CyF2y+1SO2)(其中x和y为自然数,例如,选自1至20的整数)、LiCl、LiI和LiB(C2O4)2(双(草酸)硼酸锂;LiBOB)。可以以范围为约0.1M至约2.0M的浓度使用锂盐。当在上述浓度范围包括锂盐时,由于最佳电解质导电性和粘度,电解质可具有优异的性能和锂离子迁移率。
另一实施方式提供了可再充电锂电池,该可再充电锂电池包括:含有正极活性物质的正电极;含有负极活性物质的负电极;和上述的电解质。
正电极可包括集电器和在集电器上的包括正极活性物质的正极活性物质层。
正极活性物质可包括可逆地嵌入和脱嵌锂离子的锂化的插层化合物。
在实施中,可使用锂与钴、锰、镍或其组合的复合氧化物。
正极活性物质的实例可包括由化学式中的一个表示的化合物。
LiaA1-bXbD2(0.90≤a≤1.8,0≤b≤0.5);LiaA1-bXbO2-cDc(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05);LiaE1-bXbO2-cDc(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05);LiaE2-bXbO4-cDc(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05);LiaNi1-b-cCobXcDα(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.5,0<α≤2);LiaNi1-b-cCobXcO2-αTα(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05,0<α<2);LiaNi1-b-cCobXcO2-αT2(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05,0<α<2);LiaNi1-b-cMnbXcDα(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05,0<α≤2);LiaNi1-b-cMnbXcO2-αTα(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05,0<α<2);LiaNi1-b-cMnbXcO2-αT2(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05,0<α<2);LiaNibEcGdO2(0.90≤a≤1.8,0≤b≤0.9,0≤c≤0.5,0.001≤d≤0.1);LiaNibCocMndGeO2(0.90≤a≤1.8,0≤b≤0.9,0≤c≤0.5,0≤d≤0.5,0.001≤e≤0.1);LiaNiGbO2(0.90≤a≤1.8,0.001≤b≤0.1);LiaCoGbO2(0.90≤a≤1.8,0.001≤b≤0.1);LiaMn1-bGbO2(0.90≤a≤1.8,0.001≤b≤0.1);LiaMn2GbO4(0.90≤a≤1.8,0.001≤b≤0.1);LiaMn1-gGgPO4(0.90≤a≤1.8,0≤g≤0.5);QO2;QS2;LiQS2;V2O5;LiV2O5;LiZO2;LiNiVO4;Li(3-f)J2(PO4)3(0≤f≤2);Li(3-f)Fe2(PO4)3(0≤f≤2);LiaFePO4(0.90≤a≤1.8)。
在上述化学式中,A可选自Ni、Co、Mn和其组合;X可选自Al、Ni、Co、Mn、Cr、Fe、Mg、Sr、V、稀土元素和其组合;D可选自O、F、S、P和其组合;E选自Co、Mn和其组合;T可选自F、S、P和其组合;G可选自Al、Cr、Mn、Fe、Mg、La、Ce、Sr、V和其组合;Q可选自Ti、Mo、Mn和其组合;Z可选自Cr、V、Fe、Sc、Y和其组合;并且J可选自V、Cr、Mn、Co、Ni、Cu和其组合。
正极活性物质可包括具有涂层的正极活性物质,或正极活性物质和涂布有涂层的正极活性物质的混合物。涂层可包括下述中的涂布元素化合物:涂布元素的氧化物或氢氧化物、涂布元素的羟基氧化物、涂布元素的氧碳酸盐或涂布元素的羟基碳酸盐。用于涂层的化合物可为非晶的或结晶的。涂层中包括的涂布元素可为Mg、Al、Co、K、Na、Ca、Si、Ti、V、Sn、Ge、Ga、B、As、Zr或其混合物。涂布方法可包括不对正极活性物质的性质引起任何副作用的合适的方法(例如,喷涂、浸渍)。
正极活性物质的实例可为由化学式4表示的化合物。
[化学式4]
Lix1M1 1-y1-z1M2 y1M3 z1O2
在化学式4中,
x1、y1和z1可满足下述关系:0.9≤x1≤1.8,0≤y1≤1,0≤z1≤1,0≤y1+z1≤1。M1、M2和M3可各自独立地为例如Ni、Co、Mn、Al、Sr、Mg、La或其组合。
在实施中,正极活性物质可包括锂与钴、锰、镍、铝或其组合的复合氧化物。在实施中,正电极活性物质相应可为化学式5的化合物。
[化学式5]
Lix2Niy2Coz2Al1-y2-z2O2
在化学式5中,x2、y2和z2可满足下述关系:1≤x2≤1.2,0.6≤y2≤1,和0≤z2≤0.5。
基于正极活性物质层的总重,正极活性物质的量可为约90wt%至约98wt%。
在实施中,正极活性物质层可包括粘结剂和导电材料。在实施中,基于正极活性物质层的总重,粘结剂和导电材料的各自量可为约1wt%至约5wt%。
粘结剂可有助于改善正极活性物质颗粒彼此的结合性质以及正极活性物质颗粒与集电器的结合性质。其实例可包括聚乙烯醇、羧甲基纤维素、羟丙基纤维素、二乙酰基纤维素、聚氯乙烯、羧化的聚氯乙烯、聚氟乙烯、含环氧乙烷的聚合物、聚乙烯吡咯烷酮、聚氨酯、聚四氟乙烯、聚偏二氟乙烯、聚乙烯、聚丙烯、苯乙烯-丁二烯橡胶、丙烯酸酯化的苯乙烯-丁二烯橡胶、环氧树脂和尼龙等。
可包括导电材料以有助于改善电极导电性。不引起化学变化的合适的电导性材料可用作导电材料。导电材料的实例可包括碳材料,比如天然石墨、人造石墨、炭黑、乙炔黑、科琴黑和碳纤维等;包括铜、镍、铝和银等的金属粉末或金属纤维的金属材料;导电聚合物,比如聚亚苯衍生物;或其混合物。
在实施中,集电器可为例如Al。
负电极可包括集电器和在集电器上的包括负极活性物质的负极活性物质层。
负极活性物质可为可逆地嵌入/脱嵌锂离子的材料、锂金属、锂金属合金、能够掺杂和去掺杂锂的材料或过渡金属氧化物。
可逆地嵌入/脱嵌锂离子的材料可包括碳材料。碳材料可为用于可再充电锂离子电池的合适的碳负极活性物质。碳材料的实例包括结晶碳、非晶碳和其组合。结晶碳可为不定形的或片状、鳞片状、球状或纤维状的天然石墨或人造石墨。非晶碳可为软碳、硬碳、中间相沥青碳化产物和烧制焦炭等。
锂金属合金可包括锂与Na、K、Rb、Cs、Fr、Be、Mg、Ca、Sr、Si、Sb、Pb、In、Zn、Ba、Ra、Ge、Al或Sn。
能够掺杂和去掺杂锂的材料可包括Si、SiOx(0<x<2)、Si-Q合金(其中Q为碱金属、碱土金属、第13族元素、第14族元素、第15族元素、第16族元素、过渡金属、稀土元素或其组合,且不为Si)、Sn、SnO2和Sn-R合金(其中R为碱金属、碱土金属、第13族元素、第14族元素、第15族元素、第16族元素、过渡元素、稀土元素或其组合,且不为Sn)等。它们中的至少一种可与SiO2混合。元素Q和R可为Mg、Ca、Sr、Ba、Ra、Sc、Y、Ti、Zr、Hf、Rf、V、Nb、Ta、Db、Cr、Mo、W、Sg、Tc、Re、Bh、Fe、Pb、Ru、Os、Hs、Rh、Ir、Pd、Pt、Cu、Ag、Au、Zn、Cd、B、Al、Ga、Sn、In、Tl、Ge、P、As、Sb、Bi、S、Se、Te、Po或其组合。
过渡金属氧化物可为例如氧化钒或氧化锂钒等。
根据实施方式的负极活性物质可包括含有Si活性物质和碳活性物质的Si-C复合材料。
Si活性物质的平均颗粒直径可为约50nm至约200nm。
当Si活性物质的平均颗粒直径在上述范围内时,可抑制在充电和放电期间发生的体积膨胀,且可防止在充电和放电期间由于颗粒碰撞引起的导电路径的断开。
基于Si-C复合材料的总重,Si活性物质的含量可为约1wt%至约60wt%,例如,约3wt%至约60wt%。
根据另一实施方式的负极活性物质可进一步包括结晶碳以及上述的Si-C复合材料。
当负极活性物质一起包括Si-C复合材料和结晶碳时,可以以混合物的形式包括Si-C复合材料和结晶碳,且在该情况下,可以以约1:99至约50:50的重量比包括Si-C复合材料和结晶碳。在实施中,可以以约5:95至约20:80的重量比包括Si-C复合材料和结晶碳。
结晶碳可包括例如石墨。在实施中,结晶碳可包括例如天然石墨、人造石墨或其混合物。
结晶碳可具有约5μm至约30μm的平均颗粒直径。
如本文使用的,平均颗粒直径可为累积尺寸-分布曲线中体积比为50%处的颗粒尺寸(D50)。
Si-C复合材料可进一步包括壳,壳围绕Si-C复合材料的表面,且壳可包括非晶碳。
非晶碳可包括软碳、硬碳、中间相沥青碳化产物、煅烧焦炭或其混合物。
基于100重量份的碳活性物质,非晶碳的含量可为约1重量份至约50重量份,例如,约5重量份至约50重量份,或约10重量份至约50重量份。
在负极活性物质层中,基于负极活性物质层的总重,负极活性物质的含量可为约95wt%至约99wt%。
在实施中,负极活性物质层可包括粘结剂和任选的导电材料。在负极活性物质层中,基于负极活性物质层的总重,粘结剂的量可为约1wt%至约5wt%。当其进一步包括导电材料时,其可包括约90wt%至约98wt%的负极活性物质、约1wt%至约5wt%的粘结剂和约1wt%至约5wt%的导电材料。
粘结剂可有助于改善负极活性物质颗粒彼此的结合性质以及负极活性物质颗粒与集电器的结合性质。粘结剂可为非水溶性粘结剂、水溶性粘结剂或其组合。
非水溶性粘结剂可包括例如聚氯乙烯、羧化的聚氯乙烯、聚氟乙烯、含环氧乙烷的聚合物、聚乙烯吡咯烷酮、聚氨酯、聚四氟乙烯、聚偏二氟乙烯、聚乙烯、聚丙烯、聚酰胺酰亚胺、聚酰亚胺或其组合。
水溶性粘结剂可包括橡胶粘结剂或聚合物树脂粘结剂。橡胶粘结剂可包括苯乙烯-丁二烯橡胶、丙烯酸酯化的苯乙烯-丁二烯橡胶(SBR)、丙烯腈-丁二烯橡胶、丙烯酸橡胶、丁基橡胶、氟橡胶或其组合。聚合物树脂粘结剂可包括聚四氟乙烯、聚乙烯、聚丙烯、乙烯丙烯共聚物、聚环氧乙烷、聚乙烯吡咯烷酮、聚环氧氯丙烷、聚磷腈、聚丙烯腈、聚苯乙烯、乙烯-丙烯二烯共聚物、聚乙烯吡啶、氯磺化聚乙烯、乳胶、聚酯树脂、丙烯酸树脂、酚醛树脂、环氧树脂、聚乙烯醇或其组合。
当水溶性粘结剂用作负电极粘结剂时,可进一步包括纤维素化合物作为增稠剂以提供或调整粘度。纤维素化合物可包括羧甲基纤维素、羟丙甲基纤维素、甲基纤维素或其碱金属盐。碱金属可为Na、K或Li。基于100重量份的负极活性物质,这种增稠剂的含量可为约0.1重量份至约3重量份。
包括导电材料以提供电极导电性。不引起化学变化的合适的电导性材料可用作导电材料。其实例可包括:碳材料,比如天然石墨、人造石墨、炭黑、乙炔黑、科琴黑和碳纤维等;金属材料,比如铜、镍、铝和银等的金属粉末或金属纤维等;导电聚合物,比如聚亚苯衍生物等;或其混合物。
集电器可包括铜箔、镍箔、不锈钢箔、钛箔、镍泡沫、铜泡沫、涂布有导电金属的聚合物基板,或其组合。
根据再充电锂电池的类型,可再充电锂电池可进一步包括负电极和正电极之间的隔板。合适的隔板材料的实例可包括聚乙烯、聚丙烯、聚偏二氟乙烯和它们的多层,比如聚乙烯/聚丙烯双层隔板、聚乙烯/聚丙烯/聚乙烯三层隔板和聚丙烯/聚乙烯/聚丙烯三层隔板。
参考图1,根据一个实施方式的可再充电锂电池100可包括:电池单电池,该电池单电池包括负电极112,面向负电极112的正电极114,负电极112和正电极114之间的隔板113,以及浸渍负电极112、正电极114和隔板113的电解质(未显示);容纳电池单电池的电池壳体120;和密封电池壳体120的密封构件140。
提供下述实施例和比较例以便强调一个或多个实施方式的特性,但是将理解,实施例不解释为限制实施方式的范围,比较例也不解释为在实施方式的范围之外。此外,将理解,实施方式不限于在实施例和比较例中描述的特定细节。
可再充电锂电池单电池的生产
合成例:乙烯基磷酸锂(VPLi)的合成
在Ar气氛下将乙烯基膦酸(VPA,0.1g,1.02mmol)添加至5ml的其中溶解有LiH(0.03g,3.8mmol)的无水碳酸二甲酯。搅拌反应混合物1小时,并过滤以去除残留的LiH,以获得由化学式1A表示的目标产物。
[化学式1A]
31P NMR(300MHz,DMSO):δ9.60(s,1P)。
图4显示根据合成例的添加剂化合物的P-NMR谱。
参考图4,乙烯基膦酸(VPA)的反应物的P-NMR谱的化学位移确认产物为乙烯基磷酸锂(VPLi)。
比较合成例:由化学式b表示的化合物
在Ar气氛下将苯氧基羰基膦酸(1mmol)添加至10ml的其中溶解有LiH(3mmol)的无水碳酸二甲酯。搅拌反应混合物2小时,并且然后过滤以去除残留的LiH,以获得由化学式b表示的目标产物。
[化学式b]
31P NMR(300MHz,DMSO):从δ-3.40(s,1P)至δ-3.90(s,1P)发生化学位移。
实施例1
以98:1:1的重量比分别将作为正极活性物质的LiNi0.88Co0.105Al0.015O2、作为粘结剂的聚偏二氟乙烯和作为导电材料的炭黑混合,并且然后分散在N-甲基吡咯烷酮中,以制备正极活性物质浆料。
在Al箔上将正极活性物质浆料涂布成20μm厚,并且在100℃下干燥并压制以制造正电极。
制备重量比为89:11的人造石墨和Si-C复合材料的混合物作为负极活性物质,并且将负极活性物质、作为粘结剂的苯乙烯-丁二烯橡胶和羧甲基纤维素(作为粘度调节剂)以98:1:1的重量比分散在蒸馏水中,以制备负极活性物质浆料。
Si-C复合材料具有包括人造石墨和硅颗粒的核,以及涂布在核的表面上的煤沥青,基于Si-C复合材料的总重,硅的含量为3wt%。
将负极活性物质浆料涂布在10μm厚的Cu箔上,在100℃下干燥,并压制,以制造负电极。
使用制造的正电极和负电极、25μm厚的聚乙烯隔板和电解质来制造可再充电锂电池单电池。
电解质具有下述组成。
(电解质组成)
盐:1.15M LiPF6
溶剂:碳酸亚乙酯:碳酸甲乙酯:碳酸二甲酯(EC:MEC:DMC=2:4:4的体积比)
添加剂:1wt%的由化学式1A表示的化合物
(在电解质组成中,“wt%”是基于电解质(锂盐+非水性有机溶剂+添加剂)的总重)
实施例2
根据与实施例1相同的方法制造可再充电锂电池单电池,不同的是将添加剂的含量改变成0.5wt%。
实施例3
根据与实施例1相同的方法制造可再充电锂电池单电池,不同的是将添加剂的含量改变成0.2wt%。
比较例1
根据与实施例1相同的方法制造可再充电锂电池单电池,不同的是不包括添加剂。
比较例2
根据与实施例1相同的方法制造可再充电锂电池单电池,不同的是包括1wt%的氟代碳酸亚乙酯作为添加剂,而不是由化学式1A表示的化合物。
比较例3
根据与实施例1相同的方法制造可再充电锂电池单电池,不同的是添加剂为由化学式b表示的化合物,而不是由化学式1A表示的化合物。
单电池特性的评估
评估1:初始电阻的评估
将根据实施例1至3和比较例1至3的单电池在4A和4.2V下充电并在100mA下截止,并且然后,在25℃下暂停30分钟。随后,将单电池分别在10A下放电10秒,在1A下放电10秒,和在10A下放电4秒,并且然后,在18秒和23秒的每个点处测量单电池的电流和电压,以根据ΔR=ΔV/ΔI计算初始电阻(在18秒和23秒的点处的电阻的差)。结果显示在表1和表2中。
评估2:评估高倍率性能
将根据实施例1至3和比较例1至3的可再充电锂电池单电池在恒定电流(0.1C)和恒定电压(1.0V,0.01C截止)下充电,暂停10分钟,并通过将恒定电流改变成0.2C、1.0C、2.0C和5.0C来放电至2.5V,以评估高倍率放电特性(倍率性能)。结果显示在表1和表2中。
评估3:室温循环寿命特性的评估
通过在1C下恒定电流-恒定电压-充电将根据实施例1至3和比较例1至3的可再充电锂电池单电池充电和放电250次,在4.2V和0.05C下截止,并且在25℃下在1.0C的恒定电流下放电至3.0V以测量每次循环时的放电容量,并计算相对于第一次循环时的放电容量的第200次循环时的容量保持率。结果显示在表1和表2中。
[表1]
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[表2]
参考表1,与包括由化学式b表示的化合物作为添加剂的比较例3的单电池相比,包括由化学式1A表示的化合物作为添加剂的实施例1的可再充电锂电池单电池呈现低的初始电阻。原因可能是有效形成了初始SEI膜并防止了负电极和电解质的副反应。
另外,与比较例1至3的可再充电锂电池单电池相比,实施例1的可再充电锂电池单电池具有优异的高倍率性能。
另外,与比较例1的可再充电锂电池单电池(不包括添加剂)和比较例2的单电池(包括氟代碳酸亚乙酯作为添加剂)相比,实施例1的可再充电锂电池单电池呈现改善的恢复容量。
如表2中可见,实施例1至3的可再充电锂电池单电池有助于减小初始电阻并实现优异的循环寿命特性和高倍率性能。
通过总结和回顾,电解质可包括其中溶解有锂盐的有机溶剂,且可决定可再充电锂电池的稳定性和性能。
LiPF6可用作电解质的锂盐,且可与电解质溶剂反应以促进溶剂的消耗并产生大量的气体。当LiPF6分解时,其产生LiF和PF5,这导致电池中的电解质消耗,造成高温性能劣化和差的安全性。
一个或多个实施方式可提供电解质,该电解质抑制这种锂盐的副反应并改善电池的性能。
一个或多个实施方式可提供用于可再充电锂电池的电解质,该用于可再充电锂电池的电解能够通过降低初始电阻来确保高倍率性能和改善循环寿命特性。
一个或多个实施方式可提供可再充电锂电池,该可再充电锂电池具有较低的初始电阻和改善的高倍率性能以及改善的循环寿命特性。
在本文中已公开了示例实施方式,并且尽管采用了具体术语,但它们仅以一般性和描述性意义使用和解释,而不是为了限制的目的。在一些情况下,如本领域普通技术人员在提交本申请时将显而易见的,结合特定实施方式描述的特征、特性和/或元件可以单独使用或与结合其他实施方式描述的特征、特性和/或元件组合使用,除非另有具体指示。因此,本领域技术人员将理解,在不脱离如所附权利要求中阐述的本发明的精神和范围的情况下,可以进行形式和细节上的各种改变。
Claims (13)
1.一种用于可再充电锂电池的电解质,所述电解质包括:
非水性有机溶剂;
锂盐;和
添加剂,
其中:
所述添加剂包括由化学式1表示的化合物:
[化学式1]
在化学式1,R1为氰基、取代的或未取代的C2至C10烯基或取代的或未取代的C2至C10炔基,
其中取代的C2至C10烯基或取代的C2至C10炔基的取代基选自卤素原子、羟基、硝基、氰基、氨基、叠氮基、脒基、肼基、腙基、羰基、氨甲酰基、巯基、酯基、羧基或其盐、磺酸基或其盐、磷酸基或其盐、C1至C20烷基、C2至C20烯基、C2至C20炔基、C6至C30芳基、C7至C30芳基烷基、C1至C4烷氧基、C1至C20杂烷基、C3至C20杂芳基烷基、C3至C30环烷基、C3至C15环烯基、C6至C15环炔基、C2至C20杂环烷基和其组合,并且
其中,基于所述电解质的总重,由化学式1表示的所述化合物的含量为0.2wt%至2.0wt%。
2.根据权利要求1所述的电解质,其中,R1为氰基、取代的或未取代的C2至C4烯基或取代的或未取代的C2至C4炔基。
3.根据权利要求1所述的电解质,其中,R1为氰基、乙烯基、丙烯基、乙炔基或丙炔基。
4.根据权利要求1所述的电解质,其中,由化学式1表示的所述化合物由化学式1A表示:
[化学式1A]
5.一种可再充电锂电池,包括:
含有正极活性物质的正电极;
含有负极活性物质的负电极;和
根据权利要求1至权利要求4中任一项所述的电解质。
6.根据权利要求5所述的可再充电锂电池,其中,所述正极活性物质包括锂与钴、锰、镍或其组合的复合氧化物。
7.根据权利要求5所述的可再充电锂电池,其中:
所述正极活性物质由化学式4表示:
[化学式4]
Lix1M1 1-y1-z1M2 y1M3 z1O2
在化学式4中,
x1、y1和z1满足下述关系:0.9≤x1≤1.8,0≤y1≤1,0≤z1≤1,和0≤y1+z1≤1,且
M1、M2和M3各自独立地为Ni、Co、Mn、Al、Sr、Mg、La或其组合。
8.根据权利要求5所述的可再充电锂电池,其中:
所述正极活性物质由化学式5表示:
[化学式5]
Lix2Niy2Coz2Al1-y2-z2O2
在化学式5中,x2、y2和z2满足下述关系:1≤x2≤1.2,0.6≤y2≤1,和0≤z2≤0.5。
9.根据权利要求5所述的可再充电锂电池,其中,所述负极活性物质包括含有Si活性物质和碳活性物质的Si-C复合材料。
10.根据权利要求9所述的可再充电锂电池,其中,所述负极活性物质进一步包括结晶碳。
11.根据权利要求10所述的可再充电锂电池,其中:
所述结晶碳包括石墨,且
所述石墨包括天然石墨、人造石墨或其混合物。
12.根据权利要求9所述的可再充电锂电池,其中:
所述Si-C复合材料进一步包括围绕所述Si-C复合材料的表面的壳,且
所述壳包括非晶碳。
13.根据权利要求12所述的可再充电锂电池,其中所述非晶碳包括软碳、硬碳、中间相沥青碳化产物、煅烧焦炭或其混合物。
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