CN116093427A - High-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte and lithium ion battery - Google Patents

High-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte and lithium ion battery Download PDF

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CN116093427A
CN116093427A CN202111323130.5A CN202111323130A CN116093427A CN 116093427 A CN116093427 A CN 116093427A CN 202111323130 A CN202111323130 A CN 202111323130A CN 116093427 A CN116093427 A CN 116093427A
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ion battery
lithium ion
lithium
cobalt oxide
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付向天
朱学全
黄慧聪
邱阳
张晓宇
赵倩
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Shanshan Advanced Materials Quzhou Co ltd
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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
    • 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
    • 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
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
    • 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
    • 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

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Abstract

The invention belongs to the technical field of lithium ion batteries, and discloses a high-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte and a lithium ion battery. The non-aqueous electrolyte of the high-voltage lithium cobalt oxide lithium ion battery comprises a non-aqueous organic solvent, electrolyte lithium salt and a film forming additive, wherein the film forming additive comprises an oxaphosphaheptacyclic additive with a specific structure and other additives. The phosphaheptaring additive with a specific structural formula in the nonaqueous electrolyte of the high-voltage lithium ion battery can form a phosphate CEI film stable under high voltage at the positive electrode, inhibit the reaction of the positive electrode and the electrolyte, complex positive electrode cobalt ions through the optimization of substituents and inhibit dissolution.

Description

High-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte and lithium ion battery
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to a high-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte and a lithium ion battery.
Background
With technological progress, people continuously increase the requirements on the quality of living environment, and the environmental pollution problem caused by the increasingly depleted and consumed fossil energy is more serious, so that the research and development of clean renewable new energy becomes urgent. A large amount of new energy sources such as solar energy, wind energy, tidal energy, geothermal energy and the like are developed and used at present, but the energy sources are limited in time and space and need to be properly converted and stored for use.
The lithium ion battery is used as a green environment-friendly high-energy battery and is the most ideal and potential rechargeable battery in the world at present. Compared with other batteries, the battery has a series of advantages of no memory effect, rapid charge and discharge, high energy density, long cycle life, no environmental pollution and the like, and is widely applied to small electronic equipment such as notebook computers, video cameras, mobile phones, electronic watches and the like. With the continuous improvement of the capacity requirements of pure electric vehicles, hybrid electric vehicles, portable energy storage devices and the like on lithium ion batteries, the development of lithium ion batteries with higher energy density and power density is expected to realize long-term endurance and energy storage. The energy density of the lithium ion battery can be improved by improving the working voltage, but the development of the high-voltage lithium ion battery is limited by the oxidative decomposition of the common electrolyte under high voltage. For example, the electrochemical window of the traditional carbonate electrolyte is narrow, and after the voltage is increased, the electrolyte can be decomposed; on the other hand, the oxidation capability of the positive electrode under high pressure is enhanced, a large amount of metal is dissolved, gas is separated out, and the phase change of the material causes the battery to fail and even be dangerous. Therefore, development of an electrolyte resistant to high pressure is required.
Disclosure of Invention
The invention aims to overcome the defects of the background technology and provide a high-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte and a lithium ion battery. According to the nonaqueous electrolyte for the high-voltage lithium ion battery, through optimizing the formula, under the combined action of multiple components of a unique combination, the electrolyte system has high energy density and high safety performance, and is beneficial to meeting the requirement of the electrolyte on the cycle performance under high voltage.
In order to achieve the purpose of the invention, the nonaqueous electrolyte of the high-voltage lithium cobalt oxide lithium ion battery comprises a nonaqueous organic solvent, electrolyte lithium salt and a film forming additive, wherein the film forming additive comprises a phosphaheptacyclic additive, and the phosphaheptacyclic additive has a structural formula shown in the formula (I):
Figure BDA0003340831430000021
/>
wherein R is selected from hydrogen atom, fluorine atom, alkyl group with 1-4 carbons, alkenyl group, alkynyl group, nitrile group, fluoroalkyl group or alkoxy group.
Further, in some embodiments of the present invention, the phosphaheptacyclic additive is selected from at least one of the compounds represented by the following structural formulas:
Figure BDA0003340831430000031
further, in some embodiments of the invention, the phosphaheptacyclic additive is 0.1-0.5% by mass of the nonaqueous electrolyte of the high-voltage lithium ion battery.
Preferably, in some embodiments of the present invention, the phosphaheptacyclic additive is 0.1-0.3% by mass of the nonaqueous electrolyte of the high-voltage lithium ion battery.
Further, in some embodiments of the present invention, at least one of 1, 3-Propane Sultone (PS), fluoroethylene carbonate (FEC), hexanetrinitrile (HTCN), vinyl sulfate (DTD), succinonitrile (SN) is also included in the film-forming additive.
Further, in some embodiments of the present invention, the mass percentage of 1, 3-Propane Sultone (PS), fluoroethylene carbonate (FEC), hexanetrinitrile (HTCN), ethylene sulfate (DTD), succinonitrile (SN) in the nonaqueous electrolyte of the high-voltage lithium ion battery is 0.2-2%.
Further, in some embodiments of the present invention, the electrolyte lithium salt may be selected from a mixture of lithium hexafluorophosphate with one or more of lithium bis-fluorosulfonyl imide, lithium bis-trifluoromethanesulfonyl imide, lithium difluorooxalato borate, and lithium difluorobis-oxalato phosphate.
Preferably, in some embodiments of the present invention, the mass percentage of the electrolyte lithium salt in the nonaqueous electrolyte solution of the high-voltage lithium ion battery is 10-20%.
Further, in some embodiments of the present invention, the non-aqueous organic solvent is selected from one or more of ethylene carbonate, fluoroethylene carbonate, propylene carbonate, diethyl carbonate, ethyl propionate, propyl propionate.
Preferably, in some embodiments of the present invention, the non-aqueous organic solvent is a mixture of ethylene carbonate, propylene carbonate, diethyl carbonate, propyl propionate.
Further, in some embodiments of the present invention, the volume ratio of the ethylene carbonate, propylene carbonate, diethyl carbonate, propyl propionate is 5-15:15-25:5-15:50-70.
Preferably, in some embodiments of the present invention, the volume ratio of the ethylene carbonate, propylene carbonate, diethyl carbonate, propyl propionate is 8-12:17-23:8-12:55-65.
On the other hand, the invention also provides a high-voltage lithium cobalt oxide lithium ion battery, which comprises a positive electrode, a negative electrode, a diaphragm and the non-aqueous electrolyte of the high-voltage lithium cobalt oxide lithium ion battery.
Further, in some embodiments of the invention, the active material of the positive electrode is lithium cobaltate; the negative electrode is one or more of natural graphite, artificial graphite, lithium titanate, silicon oxygen negative electrode and silicon negative electrode.
Further, in some embodiments of the invention, the upper cutoff voltage of the lithium ion battery is 4.35-4.5V.
Compared with the prior art, the invention has the following advantages:
(1) In the non-aqueous electrolyte of the high-voltage lithium ion battery, the functional group contained in the phosphaheptacyclic additive with a specific structural formula forms a phosphate CEI film which is stable under high voltage at the positive electrode, so that the reaction between the positive electrode and the electrolyte is inhibited, the cobalt ion of the positive electrode can be complexed through the optimization of the substituent, the dissolution is inhibited, the cycle life is further prolonged, the decomposition condition of the high-voltage electrolyte is improved, and the stability of the battery is ensured.
(2) According to the non-aqueous electrolyte for the high-voltage lithium ion battery, through optimizing a formula, improving a solvent and combining the combined action of the phosphaheptacyclic additive with a specific structural formula, the mixed lithium salt and other additives, the high-voltage lithium ion battery can be ensured to obtain excellent cycle performance, and the electrolyte system has high energy density and high stability.
Detailed Description
The present invention will be described in further detail with reference to the following examples in order to make the objects, technical solutions and advantages of the present invention more apparent. Additional aspects and advantages of the invention will be set forth in part in the description which follows, and in part will be obvious from the description, or may be learned by practice of the invention. It is to be understood that the following description is intended to be illustrative of the invention and not restrictive.
The terms "comprising," "including," "having," "containing," or any other variation thereof, as used herein, are intended to cover a non-exclusive inclusion. For example, a composition, step, method, article, or apparatus that comprises a list of elements is not necessarily limited to only those elements but may include other elements not expressly listed or inherent to such composition, step, method, article, or apparatus.
When an equivalent, concentration, or other value or parameter is expressed as a range, preferred range, or a range bounded by a list of upper preferable values and lower preferable values, this is to be understood as specifically disclosing all ranges formed from any pair of any upper range limit or preferred value and any lower range limit or preferred value, regardless of whether ranges are separately disclosed. For example, when ranges of "1 to 5" are disclosed, the described ranges should be construed to include ranges of "1 to 4", "1 to 3", "1 to 2 and 4 to 5", "1 to 3 and 5", and the like. When a numerical range is described herein, unless otherwise indicated, the range is intended to include its endpoints and all integers and fractions within the range.
The indefinite articles "a" and "an" preceding an element or component of the invention are not limited to the requirement (i.e. the number of occurrences) of the element or component. Thus, the use of "a" or "an" should be interpreted as including one or at least one, and the singular reference of an element or component includes the plural reference unless the amount clearly dictates otherwise.
Furthermore, the descriptions of the terms "one embodiment," "some embodiments," "examples," "particular examples," or "some examples," etc., described below mean that a particular feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the present invention. In this specification, schematic representations of the above terms are not necessarily for the same embodiment or example. The technical features of the respective embodiments of the present invention may be combined with each other as long as they do not collide with each other.
The phosphaheptacyclic additives in the examples and comparative examples are characterized as follows:
the structural formula of M1 is:
Figure BDA0003340831430000061
the structural formula of M2 is:
Figure BDA0003340831430000071
the structural formula of M3 is:
Figure BDA0003340831430000072
the structural formula of M4 is:
Figure BDA0003340831430000073
m5 has the structural formula:
Figure BDA0003340831430000081
the structural formula of M6 is:
Figure BDA0003340831430000082
example 1
Preparation of electrolyte: in a glove box filled with argon gas (oxygen content. Ltoreq.1 ppm, water content. Ltoreq.1 ppm), ethylene Carbonate (EC), propylene Carbonate (PC), diethyl carbonate (DEC), propyl Propionate (PP) were mixed at 10:20:10:60 to obtain a mixed solution, and adding 15% lithium hexafluorophosphate (LiPF) based on the total mass of the electrolyte 6 ) Subsequently, 0.2% of a phosphaheptacyclic additive M1 based on the total mass of the electrolyte, 4% of 1, 3-Propane Sultone (PS) based on the total mass of the electrolyte, 10% of fluoroethylene carbonate (FEC) based on the total mass of the electrolyte, 2% of Hexanetrinitrile (HTCN) based on the total mass of the electrolyte, and 1.5% of Succinonitrile (SN) based on the total mass of the electrolyte were added to the mixed solution and stirred to be completely dissolved, to obtain an electrolyte of example 1.
Example 2
Examples 2 to 12 are also specific examples of the preparation of the electrolyte, and the parameters and preparation method are the same as in example 1 except that the composition ratios of the components of the electrolyte are added as shown in Table 1. The electrolyte formulation is shown in table 1.
Comparative examples 1 to 9
Comparative examples 1 to 9 the procedure of example 1 was followed except that the electrolyte was added in the composition ratio shown in Table 1.
Table 1 electrolyte compositions of examples and comparative examples
Figure BDA0003340831430000091
/>
Figure BDA0003340831430000101
Note that: the content of each component in the lithium salt is the mass percentage content in the electrolyte;
the content of the phosphaheptacyclic additive is the mass percentage content in the electrolyte;
the content of each component in other additives is the mass percentage content in the electrolyte;
the proportion of each component in the solvent is mass ratio.
Preparation of lithium cobaltate battery
LiCoO as positive electrode active material 2 And (3) fully stirring and uniformly mixing the conductive agent acetylene black and the binder polyvinylidene fluoride in an N-methyl pyrrolidone system according to a mass ratio of 95:3:2, coating the mixture on an aluminum foil, drying and cold pressing the aluminum foil, and thus obtaining the positive plate.
SiO as a negative electrode active material 1.02 (5%)/AG (95%), conductive agent super carbon black, thickener sodium carboxymethyl cellulose and binder styrene-butadiene rubber are fully stirred and uniformly mixed in a deionized water solvent system according to the mass ratio of 95:1:2:2, and then are coated on a copper foil for drying and cold pressing, so that the negative electrode plate is obtained.
Polyethylene is used as a base film, and a nano alumina coating is coated on the base film to be used as a diaphragm.
And sequentially stacking the positive plate, the diaphragm and the negative plate, enabling the diaphragm to be positioned between the positive plate and the negative plate to play a role in isolation, and winding to obtain the bare cell. And (3) placing the bare cell in an outer package, respectively injecting the electrolyte prepared in each example and each comparative example, and carrying out the procedures of packaging, placing, forming, aging, secondary packaging, capacity division and the like to obtain the lithium cobalt oxide silicon oxygen carbon lithium ion battery.
Lithium ion battery performance test
(1) Circulation at normal temperatureThe method can test: at 25 ℃, the LiCoO is added with 2 The silicon-oxygen-carbon lithium ion battery is charged to 4.5V according to a constant current and a constant voltage of 1C, the cut-off current is 0.05C, and then the lithium ion battery is discharged to 3.0V according to the constant current of 1C. The 500 th cycle capacity retention rate was calculated after 500 cycles of charge/discharge. The calculation formula is as follows:
500 th week capacity retention = 500 th week cycle discharge capacity/first week cycle discharge capacity x 100%.
(2) High temperature storage performance at 60 ℃): the LiCoO is treated at room temperature 2 The silicon oxygen carbon lithium ion battery is charged and discharged once according to 1C, the cut-off current is 0.05C, and the initial capacity is recorded. Then, the battery is fully charged according to the constant current and constant voltage of 1C, and the initial thickness and the initial internal resistance of the battery are tested; placing the full-charge battery in a constant temperature environment at 60 ℃ for 14 days, and calculating the thermal expansion rate; after the battery is cooled to normal temperature for 6 hours, discharging to 3.0V according to 1C, recording the residual capacity of the battery, and calculating the residual capacity of the battery according to the following calculation formula:
battery thermal state expansion ratio (%) = (thermal thickness-initial thickness)/initial thickness×100%;
battery capacity remaining rate (%) =remaining capacity/initial capacity×100%;
battery capacity recovery rate (%) =recovery capacity/initial capacity×100%
Table 2 battery performance of each of examples and comparative examples
Figure BDA0003340831430000111
/>
Figure BDA0003340831430000121
For LiCoO 2 Lithium ion battery of the silicon oxygen carbon system:
as can be seen from examples 1 to 12 and comparative examples 1 to 7, the lithium ion batteries using the electrolytes of examples 1 to 12 were superior to those of comparative examples 1 to 7 in both normal temperature cycle performance and high temperature storage performance. The nonaqueous electrolyte of the high-voltage lithium ion battery can stabilize CEI film and reduce the oxidation rate of electrolyte on the surface of positive electrode under high voltage by optimizing the formula and combining the unique combination of various components, especially by combining the phosphaseven-ring additive with specific structural formula with other additives, thereby ensuring that the high-capacity lithium cobalt oxide-silicon oxygen carbon battery has long cycle life and excellent high-temperature storage performance. Meanwhile, the optimal addition amount of the phosphaheptacyclic additive is 0.2-0.3%. Specifically, the optimal addition amount of M1, M2, M4 and M6 is 0.3%, and the optimal addition amount of M3 and M5 is 0.2%.
Comparative examples 1-6 data with only phosphaheptacyclic additives indicated that the effect of mono-phosphaheptacyclic additives was limited; in addition, compared with examples 1, 2, 4 and 6, the comparative example 7 without the phosphaheptacyclic additive has lower capacity retention rate after being cycled for 500 weeks at normal temperature, which proves that the CEI interface film formed by the part of phosphaheptacyclic additive is more excellent and stable and can improve the cycle performance of the battery; meanwhile, the relative ratio of the phosphaheptacyclic additives with different substituents shows that the M1, M2, M4 and M6 have better circulation performance and low DCR; m3 is excellent in storage performance and small in gas production. The best overall performance is M6.
In summary, the nonaqueous electrolyte for the high-voltage lithium ion battery can ensure high-voltage LiCoO by improving the carbonate solvent at the electrode/electrolyte interface and combining the combined action of the phosphaheptacyclic additive, the nitrile additive and other conventional additives with specific structural formula 2 The silicon oxygen carbon lithium ion battery has excellent cycle performance and high-temperature storage performance.
It will be readily appreciated by those skilled in the art that the foregoing is merely illustrative of the present invention and is not intended to limit the invention, but any modifications, equivalents, improvements or the like which fall within the spirit and principles of the present invention are intended to be included within the scope of the present invention.

Claims (10)

1. The high-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte is characterized by comprising a nonaqueous organic solvent, electrolyte lithium salt and a film-forming additive, wherein the film-forming additive comprises a phosphaheptacyclic additive, and the phosphaheptacyclic additive has a structural formula shown in formula (I):
Figure FDA0003340831420000011
wherein R is selected from hydrogen atom, fluorine atom, alkyl group with 1-4 carbons, alkenyl group, alkynyl group, nitrile group, fluoroalkyl group or alkoxy group.
2. The high voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte according to claim 1, wherein the phosphaheptacyclic additive is selected from at least one of the compounds represented by the following structural formulas:
Figure FDA0003340831420000012
/>
Figure FDA0003340831420000021
3. the high-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte according to claim 1, wherein the mass percentage of the phosphaheptacyclic additive in the high-voltage lithium ion battery nonaqueous electrolyte is 0.1-0.5%; preferably, the mass percentage of the phosphaheptacyclic additive in the nonaqueous electrolyte of the high-voltage lithium ion battery is 0.1-0.3%.
4. The high voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte according to claim 1, wherein the film forming additive further comprises at least one of 1, 3-propane sultone, fluoroethylene carbonate, hexanetrinitrile, vinyl sulfate and succinonitrile; preferably, the film-forming additive comprises 1, 3-propane sultone, fluoroethylene carbonate, hexanetrinitrile and succinonitrile; preferably, the mass percentage of the 1, 3-propane sultone, fluoroethylene carbonate, hexanetrinitrile, ethylene sulfate and succinonitrile in the nonaqueous electrolyte of the high-voltage lithium ion battery in the film-forming additive is 0.2-2%.
5. The high-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte according to claim 1, wherein the electrolyte lithium salt is selected from one or more of lithium hexafluorophosphate, lithium bis (fluorosulfonyl) imide, lithium bis (trifluoromethanesulfonyl) imide, lithium difluorooxalato borate, and lithium difluorobis (oxalato) phosphate; preferably, the mass percentage of the electrolyte lithium salt in the nonaqueous electrolyte of the high-voltage lithium ion battery is 10-20%.
6. The high-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte according to claim 1, wherein the nonaqueous organic solvent is one or more selected from the group consisting of ethylene carbonate, fluoroethylene carbonate, propylene carbonate, diethyl carbonate, ethyl propionate, and propyl propionate; preferably, the nonaqueous organic solvent is a mixture of ethylene carbonate, propylene carbonate, diethyl carbonate, propyl propionate.
7. The nonaqueous electrolyte of the high-voltage lithium cobalt oxide lithium ion battery according to claim 1, wherein the volume ratio of the ethylene carbonate, the propylene carbonate, the diethyl carbonate and the propyl propionate is 5-15:15-25:5-15:50-70 parts; preferably, the volume ratio of the ethylene carbonate to the propylene carbonate to the diethyl carbonate to the propyl propionate is 8-12:17-23:8-12:55-65.
8. A high voltage lithium cobalt oxide lithium ion battery comprising a positive electrode, a negative electrode, a separator, and the high voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte of any one of claims 1-7.
9. The high voltage lithium cobalt oxide lithium ion battery according to claim 8, wherein the active material of the positive electrode is lithium cobalt oxide; the negative electrode is one or more of natural graphite, artificial graphite, lithium titanate, silicon oxygen negative electrode and silicon negative electrode.
10. The high voltage lithium cobalt oxide lithium ion battery of claim 8, wherein the upper cutoff voltage of the lithium ion battery is 4.35-4.5V.
CN202111323130.5A 2021-11-05 2021-11-05 High-voltage lithium cobalt oxide lithium ion battery nonaqueous electrolyte and lithium ion battery Pending CN116093427A (en)

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