CN110957532A - Electrolyte for lithium ion battery and lithium ion battery comprising same - Google Patents
Electrolyte for lithium ion battery and lithium ion battery comprising same Download PDFInfo
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- CN110957532A CN110957532A CN201911352862.XA CN201911352862A CN110957532A CN 110957532 A CN110957532 A CN 110957532A CN 201911352862 A CN201911352862 A CN 201911352862A CN 110957532 A CN110957532 A CN 110957532A
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- lithium ion
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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
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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
- H01M10/052—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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention provides an electrolyte for a lithium ion battery, which is more stable at high temperature, and a lithium ion battery comprising the same. The electrolyte for the lithium ion battery comprises an organic solvent, lithium salt, a first additive and a second additive; the first additive and the second additive have structural formulas shown in formulas (I) and (II) respectively. The oxidation potential of the first additive is lower than that of the organic solvent, and the first additive can be preferentially oxidized and polymerized on the surface of the positive electrode to form a compact solid electrolyte phase interface film, so that the oxidative decomposition gas generation is reduced, and the consumption of active substances is reduced. The nitrogen atoms of the second additive can be effectively complexed with high-valence transition metal atoms, so that the interface impedance of the anode is reduced, the migration of lithium ions on the interface of the anode is facilitated, the oxidation activity of the anode material on the electrolyte, particularly the oxidation of the anode material on the electrolyte under a high-temperature condition, the reduction dissolution of the transition metal caused by the change of the structure of the anode material is further inhibited, and the high-temperature performance of the lithium ion battery is improved.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to an electrolyte for a lithium ion battery and the lithium ion battery comprising the same.
Background
The lithium ion battery has the advantages of high working voltage, large energy density, long cycle life, safety and the like, and is the most widely used secondary battery of 3C electronic products at present. However, with the progress and development of society, the energy density and cycle life at high temperature of lithium ion batteries are increasingly required. For example, in the current mainstream game notebook computer, with the improvement of configuration, the battery temperature of the computer is as high as more than 40 ℃ under the condition of high-load work. Therefore, it is a trend of development of lithium ion batteries to improve the electrical properties of the lithium ion batteries in floating charge and storage at high temperatures.
The electrolyte is used as an important component of the lithium ion battery and plays a role in transmitting lithium ions in the charge and discharge processes. However, the electrolyte solvent conventionally used is easily oxidized and decomposed on the surface of the positive electrode under high temperature conditions. Moreover, the high temperature condition further aggravates the decomposition and re-film formation of the SEI film (Solid Electrolyte Interphase), and the consumption of the Electrolyte is continuously accelerated while high-impedance byproducts are generated, so that the performance of the lithium ion battery is greatly influenced. Therefore, it is necessary to improve the stability of the lithium ion battery electrolyte at high temperature and improve the high temperature performance of the battery.
Disclosure of Invention
The present invention is directed to solving at least one of the problems of the prior art. Accordingly, the present invention provides an electrolyte for a lithium ion battery that is more stable at high temperatures, and a lithium ion battery including the same.
In a first aspect, an embodiment of the present invention provides an electrolyte for a lithium ion battery, including an organic solvent, a lithium salt, a first additive, and a second additive;
the first additive has a formula as shown in formula (I):
the second additive has a formula as shown in formula (II):
wherein:
R1、R2are respectively and independently selected from C1-C12 alkyl, C1-C12 halogenated alkyl, C2-C12 alkenyl, C2-C12 halogenated alkenyl, C6-C26 aryl and C6-C26 halogenated aryl;
R3、R4、R5are respectively and independently selected from hydrogen atoms, halogen atoms, C1-C12 alkyl, C1-C12 halogenated alkyl, C1-C12 alkoxy, C1-C12 halogenated alkoxy, C2-C12 alkenyl, C2-C12 halogenated alkenyl, C6-C26 aryl and C6-C26 halogenated aryl;
R6、R7、R8are respectively and independently selected from hydrogen atoms, C1-C10 alkyl and C1-C10 halogenated alkyl.
The halogenated alkyl, halogenated alkenyl, halogenated alkoxy and halogenated aryl refer to alkyl, alkenyl, alkoxy and aryl which have one or more substituent groups, and the substituent groups are one or more of any halogen atoms.
The electrolyte for the lithium ion battery provided by the embodiment of the invention at least has the following beneficial effects:
the oxidation potential of the first additive is lower than that of the organic solvent, so that a compact solid electrolyte phase interface film (namely a CEI film) can be formed on the surface of the positive electrode through oxidation polymerization preferentially, the oxidative decomposition gas generation of the organic solvent at the positive electrode is effectively reduced, the consumption of the organic solvent on active substances is reduced, and the first additive is particularly beneficial to the performance of a secondary battery under the high-temperature condition. The second additive contains three nitrogen atoms, each nitrogen atom has a pair of lone-pair electrons, and can be effectively complexed with high-valence transition metal atoms, so that the interface impedance of the anode can be remarkably reduced, the migration of lithium ions on the interface of the anode is facilitated, and the complexation of the N atoms and the high-valence metal atoms (such as Ni, Co, Mn and the like) effectively reduces the oxidation activity of the anode material on the electrolyte, particularly the oxidation on the electrolyte under the high-temperature condition, and further can inhibit the dissolution of transition metals such as nickel, cobalt and the like caused by the structural change of the anode material due to the reduction reaction, so that the high-temperature performance of the lithium ion battery is improved.
Electrolyte for lithium ion batteries, R, according to some embodiments of the invention1、R2Are respectively provided withIndependently selected from C1-C6 alkyl, C1-C6 halogenated alkyl, C2-C6 alkenyl, C2-C6 halogenated alkenyl, phenyl and halogenated phenyl.
Electrolyte for lithium ion batteries, R, according to some embodiments of the invention3、R4、R5Are respectively and independently selected from hydrogen atoms, halogen atoms, C1-C6 alkyl, C1-C6 halogenated alkyl, C1-C6 alkoxy, C1-C6 halogenated alkoxy, C2-C6 alkenyl, C2-C6 halogenated alkenyl, phenyl and halogenated phenyl.
According to some embodiments of the electrolyte for a lithium ion battery of the present invention, the first additive is selected from the group consisting of:
according to some embodiments of the electrolyte for a lithium ion battery of the present invention, the second additive is selected from the group consisting of:
the electrolyte for a lithium ion battery according to some embodiments of the present invention may include 0.01 to 3% by weight of the first additive, based on the total weight of the electrolyte for a lithium ion battery. The addition of the first additive in a proper proportion can reduce the dissolution of transition metal, remarkably improve the floating charge capacity retention rate of the battery at high temperature, and control the thickness expansion in a small range.
The electrolyte for a lithium ion battery according to some embodiments of the present invention, the weight of the first additive is 0.05% to 1% based on the total weight of the electrolyte for a lithium ion battery.
The electrolyte for a lithium ion battery according to some embodiments of the present invention may include 0.01 to 3% by weight of the second additive, based on the total weight of the electrolyte for a lithium ion battery. Increasing the amount of the second additive can reduce the elution of the transition metal, but an excessive amount of the second additive causes a sharp increase in the internal resistance of the battery, thereby causing some deterioration in the capacity retention rate of the battery.
The electrolyte for a lithium ion battery according to some embodiments of the present invention may include 0.05 to 1% by weight of the second additive, based on the total weight of the electrolyte for a lithium ion battery.
According to some embodiments of the electrolyte for a lithium ion battery of the present invention, the organic solvent is selected from a cyclic carbonate, a linear carbonate, and a carboxylate.
According to the electrolyte for a lithium ion battery of some embodiments of the present invention, the cyclic carbonate is selected from Ethylene Carbonate (EC), Propylene Carbonate (PC), the linear carbonate is selected from dimethyl carbonate (DMC), Ethyl Methyl Carbonate (EMC), diethyl carbonate (DEC), and the carboxylate is selected from at least one of Propyl Propionate (PP), Ethyl Propionate (EP), and Methyl Propionate (MP).
According to the electrolyte for a lithium ion battery of some embodiments of the present invention, the lithium salt is an inorganic lithium salt.
According to some embodiments of the electrolyte for lithium ion batteries of the present invention, the lithium salt is selected from lithium hexafluorophosphate (LiPF)6) Lithium perchlorate (LiClO)4) Lithium hexafluoroarsenate (LiAsF)6) Lithium bis (fluorosulfonyl) imide (LiFSI) and lithium bis (trifluoromethylsulfonyl) imide (LiTFSI).
According to the electrolyte for the lithium ion battery of some embodiments of the present invention, the lithium salt is LiPF6The concentration is 0.5-2 mol/L.
According to the electrolyte for the lithium ion battery of some embodiments of the present invention, the concentration of the lithium salt is 0.9 to 1.2 mol/L.
The electrolyte for a lithium ion battery according to some embodiments of the present invention further includes a film forming additive.
According to the electrolyte for a lithium ion battery of some embodiments of the present invention, the film-forming additive is a negative electrode film-forming additive.
According to the electrolyte for the lithium ion battery of some embodiments of the present invention, the negative electrode film forming additive is fluoroethylene carbonate, vinylene carbonate, Vinyl Ethylene Carbonate (VEC), 1, 3-Propane Sultone (PS).
In a second aspect, an embodiment of the present invention provides a lithium ion battery to which the electrolyte for a lithium ion battery is applied.
The lithium ion battery provided by the embodiment of the invention at least has the following beneficial effects:
when the lithium ion battery prepared by the electrolyte for the lithium ion battery is subjected to floating charge under a high-temperature condition, the capacity retention rate can be controlled at a higher level, so that the performance of the battery cannot be greatly damaged under the high-temperature condition, and the electrolyte is suitable for wider application scenes.
The lithium ion battery according to some embodiments of the present invention includes the above-described electrolyte for a lithium ion battery, and a positive electrode sheet, a negative electrode sheet, and a separator in contact with the electrolyte.
Detailed Description
The concept and technical effects of the present invention will be clearly and completely described below in conjunction with the embodiments to fully understand the objects, features and effects of the present invention. It is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all embodiments, and those skilled in the art can obtain other embodiments without inventive effort based on the embodiments of the present invention, and all embodiments are within the protection scope of the present invention.
Example 1
The embodiment provides an electrolyte for a lithium ion battery, which comprises the following components based on the total weight of the electrolyte: 1 wt% of a first additive (selected from the compounds represented by the formula (III)), and 0.5 wt% of a second additive (selected from the compounds represented by the formula (IX)). The lithium salt in the electrolyte is lithium hexafluorophosphate, and the concentration of the lithium salt is 1.2 mol/L. The weight ratio of each solvent in the organic solvent adopted by the electrolyte is ethylene carbonate: propylene carbonate: diethyl carbonate: propyl propionate ═ 20: 20: 25: 35.
the present embodiment also provides a secondary battery. The secondary battery is a lithium ion battery and comprises a positive plate, a negative plate, a diaphragm and the electrolyte for the lithium ion battery.
The positive plate comprises a positive active material, a current collector, a conductive agent and a binder. The positive electrode active material is lithium cobaltate particles. The negative plate comprises a negative active material, a current collector, a conductive agent and a binder. The negative active material is graphite. The separator is a PE porous polymer isolating membrane.
The lithium ion battery is prepared by the following steps:
(1) preparing a positive plate:
the positive electrode is high-voltage lithium cobaltate particles, the conductive agent is Carbon Nano Tubes (CNT), the binder is polyvinylidene fluoride (PVDF), and the weight ratio of the high-voltage lithium cobaltate particles to the binder in the positive electrode is 96.5: 2: 1.5. the preparation method comprises the steps of fully stirring and uniformly mixing the raw materials in an N-methyl pyrrolidone (NMP) solvent to form uniform anode slurry with the viscosity of about 5000Pa.s, and uniformly coating the anode slurry on an anode current collector. The positive electrode current collector used was an aluminum foil 10 μm thick. Drying is then carried out in an oven at 110-120 ℃ and subsequent cold pressing to obtain the desired thickness. And finally, cutting the anode sheet into the required length and width according to the process requirements to obtain the anode sheet.
(2) Preparing a negative plate:
the negative electrode active substance is graphite, the conductive agent is super-p (small particle conductive carbon black), the binder is sodium carboxymethyl cellulose (CMC) and Styrene Butadiene Rubber (SBR), and the weight ratio of the above components in the negative electrode is 95: 1.5: 1.5: 2. the mixture is fully stirred and uniformly mixed in deionized water to form uniform negative electrode slurry with the viscosity of about 3000Pa.s, and then the uniform negative electrode slurry is uniformly coated on a negative electrode current collector. The negative current collector adopts 6 mu m copper foil. Drying is then carried out in an oven at 90-100 ℃ and subsequently cold pressing to give the desired thickness. And finally, cutting the anode sheet into required length and width according to the process requirements to obtain the anode sheet.
(3) And assembling the positive plate, the diaphragm and the negative plate into a soft package battery, and injecting the electrolyte to obtain the lithium ion battery.
Example 2
Float charge test
The types and contents of the first additive and the second additive in example 1 were adjusted to obtain each case group, see the following table, wherein the types of the first additive and the second additive are shown in the above formulas:
TABLE 1 comparison of various groups of additives
The 16 batteries were subjected to float charge test in a 55 ℃ incubator for 49 weeks. The specific test method is as follows: firstly, initializing the battery at normal temperature, and recording initial capacity, thickness and internal resistance.
Testing in a 55 ℃ constant temperature box, (1) carrying out multiplying power constant current constant voltage charging to full charge voltage at 0.5 ℃, cutting off current at 0.05 ℃, and standing for 22.8 hours; (2) then, the mixture was discharged at a constant current of 0.05C for 60 minutes and left for 10 minutes. And (3) repeating the steps (1) and (2) for 24 hours after the cycle for one week, testing the full-state voltage, the internal resistance and the thickness of the battery every 7 weeks, and testing the capacity retention rate until the test is finished for 49 weeks. The float test results are shown in the table below.
TABLE 2 Floating Charge test results
The high-temperature floating charge test is a test for higher requirements of the battery. During the test, the battery is always in a high SOC state. At this time, the positive electrode has high activity and is very likely to react with the electrolyte. In addition, transition metal elements such as high-valence Co, Ni and Mn can be precipitated from the surface of the positive active material, react with the electrolyte or diffuse to the surface of the negative electrode to damage the negative electrode; the high valence transition metal is dissolved out along with the release of oxygen, and further reacts with the electrolyte to generate gas. The content of the transition metal on the negative electrode sheet is an important index reference value for measuring the stability of the active material in the battery. Therefore, in the experiment, the content of the transition metal on the negative plate is tested besides the overall thickness expansion and the capacity retention rate of the battery are considered.
As can be seen from the thickness expansion, the capacity retention rate and the content of the transition metal in the negative electrode in the 55 ℃ floating charge test, the dissolution of the transition metal can be reduced by adding the first additive and the second additive in a proper proportion as in cases 1 to 11, and the floating charge capacity retention rate and the smaller thickness expansion of the battery at high temperature are obviously improved. The first additive can be preferentially oxidized and polymerized on the surface of the positive electrode to form a CEI film in the first charging process, and Si, O, P and other groups contained in the CEI can be well combined with trace water and fluorine ions in the electrolyte, so that HF and the SEI film or the CEI film are prevented from being combined to generate gas. Meanwhile, the second additive can be effectively complexed with high-valence transition metal atoms (Ni, Co, Mn and the like), so that the transition metals (such as Mn and Co) in the positive active material are prevented from dissolving out, the release of O is prevented, the O and the electrolyte are prevented from generating gas by oxidation, and the volume expansion of the secondary battery is further avoided. As can be seen from the negative electrode transition metal content, increasing the amount of the second additive can reduce the elution of the transition metal, but excessive amounts of the additive will cause a sharp increase in the internal resistance of the battery, and will also deteriorate the capacity retention rate of the battery.
In case 12, no additive component was added, and in case 13 and case 14, 1 wt% of the second additive and 2 wt% of the first additive were added, respectively, it can be seen that the capacity retention ratio after 49 weeks was hardly improved, and the thickness expansion and the transition metal content of the negative electrode sheet were not significantly reduced by adding either of the first additive and the second additive alone.
In case 2, the first additive accounts for 2 wt% and the second additive accounts for 1 wt%, and comparison with cases 12, 13 and 14 shows that after the two types of additives are combined, the thickness expansion and the transition metal content of the negative plate are reduced remarkably, and the capacity retention rate is improved greatly. The ratio of the reduction and the increase is far higher than the improvement of the effect brought by independently adding the first additive and the second additive, and the method has unexpected technical effect. In comparison with other cases, it can be seen that the combination of the first additive and the second additive in proper proportion can bring about a very outstanding effect improvement.
While the embodiments of the present invention have been described in detail, the present invention is not limited to the embodiments, and various changes can be made without departing from the spirit of the present invention within the knowledge of those skilled in the art. Furthermore, the embodiments of the present invention and the features of the embodiments may be combined with each other without conflict.
Claims (10)
1. An electrolyte for a lithium ion battery is characterized by comprising an organic solvent, a lithium salt, a first additive and a second additive;
the first additive has a formula as shown in formula (I):
the second additive has a formula as shown in formula (II):
wherein:
R1、R2are respectively and independently selected from C1-C12 alkyl, C1-C12 halogenated alkyl, C2-C12 alkenyl, C2-C12 halogenated alkenyl, C6-C26 aryl and C6-C26 halogenated aryl;
R3、R4、R5are respectively and independently selected from hydrogen atoms, halogen atoms, C1-C12 alkyl, C1-C12 halogenated alkyl, C1-C12 alkoxy, C1-C12 halogenated alkoxy, C2-C12 alkenyl, C2-C12 halogenated alkenyl, C6-C26 aryl and C6-C26 halogenated aryl;
R6、R7、R8are respectively and independently selected from hydrogen atoms, C1-C10 alkyl and C1-C10 halogenated alkyl.
2. The electrolyte for lithium ion batteries according to claim 1, wherein R is1、R2Are respectively and independently selected from C1-C6 alkyl, C1-C6 halogenated alkyl, C2-C6 alkenyl, C2-C6 halogenated alkenyl, phenyl and halogenated phenyl.
3. The electrolyte for lithium ion batteries according to claim 1, wherein R is3、R4、R5Are respectively and independently selected from hydrogen atoms, halogen atoms, C1-C6 alkyl, C1-C6 halogenated alkyl, C1-C6 alkoxy, C1-C6 halogenated alkoxy, C2-C6 alkenyl, C2-C6 halogenated alkenyl, phenyl and halogenated phenyl.
4. The electrolyte for a lithium ion battery according to claim 1, wherein the first additive is selected from the group consisting of:
5. the electrolyte for a lithium ion battery according to claim 1, wherein the second additive is selected from the group consisting of:
6. the electrolyte for lithium ion batteries according to any one of claims 1 to 5, wherein the weight of the first additive is 0.01% to 3% based on the total weight of the electrolyte for lithium ion batteries.
7. The electrolyte for lithium ion batteries according to any one of claims 1 to 5, wherein the weight of the second additive is 0.01% to 3% based on the total weight of the electrolyte for lithium ion batteries.
8. The electrolyte for a lithium ion battery according to any one of claims 1 to 5, wherein the organic solvent is selected from a cyclic carbonate, a linear carbonate, and a carboxylate.
9. The electrolyte for a lithium ion battery according to any one of claims 1 to 5, further comprising a film forming additive.
10. A lithium ion battery comprising the electrolyte for a lithium ion battery according to any one of claims 1 to 9.
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Application publication date: 20200403 |