CN111129599A - Electrolyte and lithium ion battery - Google Patents
Electrolyte and lithium ion battery Download PDFInfo
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- CN111129599A CN111129599A CN201911415767.XA CN201911415767A CN111129599A CN 111129599 A CN111129599 A CN 111129599A CN 201911415767 A CN201911415767 A CN 201911415767A CN 111129599 A CN111129599 A CN 111129599A
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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
- 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
- H01M10/42—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
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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
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Abstract
The invention discloses an electrolyte and a lithium ion battery, wherein the electrolyte comprises lithium salt, an organic solvent, an additive A and an additive B; the content of the additive A is 0.1-10 percent, and the content of the additive B is 0.1-5 percent; the additive A has a structural formula shown as a formula (I) or (II): the additive B has a structural formula shown in the following formula (III). The oxidation potential of the additive B is low, and the additive B is oxidized and polymerized on the surface of the battery anode to form a compact CEI film to cover the surface of the anode, so that side reactions are prevented, the increase of the interface impedance of the anode is reduced, and the polarization of the electrode is reduced. And the additive A is reduced at the negative electrode of the battery, and the formed SEI film is compact and stable, and has a large effect of reducing the internal resistance of the negative electrode interface. Meanwhile, stable passive films generated on the anode and the cathode are mutually matched, so that the high-rate discharge performance of the battery can be remarkably improved, and higher discharge capacity can be still maintained under the high-rate discharge condition.
Description
Technical Field
The invention relates to the technical field of lithium batteries, in particular to an electrolyte and a lithium ion battery.
Background
The lithium ion battery has the remarkable advantages of high specific energy, large specific power, long cycle life, small self-discharge and the like, is popular with consumers, and is widely applied to 3C electronic products such as mobile communication, digital cameras, video cameras and the like. Although lithium ion batteries have been developed, consumers expect better batteries, and especially, higher and higher requirements are imposed on the charging and discharging speed of the batteries. For example, in the fields of unmanned aerial vehicles, aeromodelling, and the like, it is required that the lithium ion battery used can achieve sustained discharge with a high rate, but most commercial lithium ion batteries at present are difficult to meet such requirements.
Researchers have found that a key factor that restricts the high rate discharge of lithium ions is the internal resistance of the battery. The internal resistance of the battery is mainly determined by a current collector, an active material, an electrolyte and the like in the battery. At present, the research and use of the current collector and the active material of the battery are relatively mature, so that it is necessary to provide an electrolyte for a lithium ion battery, which can better realize a high-rate discharge function, starting from the electrolyte.
Disclosure of Invention
The present invention is directed to solving at least one of the problems of the prior art. Therefore, the invention provides an electrolyte which can meet the requirement of high-rate discharge of a lithium ion battery.
The invention also provides a lithium ion battery containing the electrolyte.
In a first aspect, an embodiment of the present invention provides an electrolyte including a lithium salt, an organic solvent, an additive a, and an additive B; based on the total weight of the electrolyte, the content of the additive A is 0.1-10 percent, and the content of the additive B is 0.1-5 percent;
the additive A has a structural formula shown as the following formula (I) or (II):
the additive B has a structural formula shown as the following formula (III):
wherein R is1、R2Are respectively and independently selected from C2-C6 alkyl; r3Selected from C1-C12 alkyl.
The electrolyte disclosed by the embodiment of the invention at least has the following beneficial effects:
the oxidation potential of the additive B is low, a compact solid electrolyte phase interface film (CEI) can be formed on the surface of the battery anode through oxidation polymerization and covers the surface of the anode, the CEI film is not easy to dissolve by an organic solvent and is more stable, side reactions of the anode material of the battery and an electrolyte on the surface of the anode can be effectively prevented, the increase amplitude of the interface impedance of the anode in the circulation process is reduced, and the electrode polarization phenomenon is reduced. And the additive A is reduced at the negative electrode of the battery, and the formed SEI film is compact and stable, and has a large effect of reducing the internal resistance of the negative electrode interface. Meanwhile, the inventors surprisingly found that when the additive a and the additive B are used in combination, stable passive films respectively generated on the positive electrode and the negative electrode cooperate with each other, so that the high-rate discharge performance of the battery can be remarkably improved, and a higher discharge capacity can be still maintained under a high-rate discharge condition.
Electrolytes according to other embodiments of the present invention, R3Specific examples thereof include, but are not limited to, straight-chain or straight-chain alkyl groups such as methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, tert-butyl, n-pentyl, isopentyl, sec-pentyl, tert-pentyl, n-hexyl, n-heptyl, n-octyl, isooctyl, sec-octyl, tert-octyl, n-nonyl, isononyl, n-decyl, and isodecyl groups.
Electrolytes according to other embodiments of the present invention, R1、R2Specific examples include, but are not limited to, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, tert-butyl, n-pentyl, isopentyl, sec-pentyl, tert-pentyl, and n-hexyl.
According to further embodiments of the electrolyte of the present invention, the additive a is selected from the group consisting of vinyl sulfate, propylene sulfate, vinyl sulfite, propylene sulfite.
According to other embodiments of the electrolyte of the present invention, additive B is pentafluorophenyl methanesulfonate.
According to other embodiments of the electrolyte, the additive a may be present in an amount ranging from 10%, 8%, 5%, 4% at the upper limit and 0.1%, 0.2%, 0.3%, 0.5%, 1% at the lower limit, based on the total weight of the electrolyte.
The electrolyte according to other embodiments of the present invention includes 0.3 to 5% of the additive a, based on the total weight of the electrolyte.
According to the electrolyte of other embodiments of the present invention, the additive B is included in an amount ranging from 5% to 3% at the upper limit and 0.1% to 0.2% at the lower limit, based on the total weight of the electrolyte.
The electrolyte according to other embodiments of the present invention includes 0.2 to 3% of the additive B, based on the total weight of the electrolyte.
According to other embodiments of the electrolyte of the present invention, the lithium salt is an organic lithium salt or an inorganic lithium salt or a mixture of both.
According to other embodiments of the electrolyte of the present invention, the lithium salt is a fluorine-containing lithium salt.
According to still further embodiments of the electrolyte of the present invention, the fluorine-containing lithium salt is selected from the group consisting of lithium hexafluorophosphate, lithium hexafluoroarsenate, lithium perchlorate, lithium trifluorosulfonyl, lithium difluoro (trifluoromethylsulfonyl) imide, lithium bis (fluorosulfonyl) imide, and lithium tris (trifluoromethylsulfonyl) methide.
According to other embodiments of the electrolyte of the present invention, the concentration of the lithium salt is 0.5mol/L to 2 mol/L. The concentration of the lithium salt is too low, the conductivity of the electrolyte is low, and the multiplying power and the cycle performance of the whole battery system can be influenced; and the concentration of the lithium salt is too high, so that the viscosity of the electrolyte is too high, and the multiplying power of the whole battery system is also influenced.
According to other embodiments of the electrolyte of the present invention, the organic solvent is selected from the group consisting of ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl formate, ethyl propionate, propyl propionate, methyl butyrate, tetrahydrofuran.
In a second aspect, embodiments of the present invention provide a lithium ion battery comprising a positive electrode sheet, a negative electrode sheet, a separator, and any one of the foregoing electrolytes.
The lithium ion battery of the embodiment of the invention has at least the following effects:
when a lithium ion battery formed by the electrolyte prepared by the formula works, stable passive films CEI and SEI can be generated at the positions of the positive electrode and the negative electrode. The two passive films are mutually matched, so that the high-rate discharge performance of the lithium ion battery is remarkably improved, and higher discharge capacity can be kept under the high-rate discharge condition.
According to the lithium ion battery of other embodiments of the present invention, the positive plate includes a positive current collector and a positive membrane coated on the positive current collector, and the negative plate includes a negative current collector and a negative membrane coated on the negative current collector.
According to other embodiments of the present invention, a lithium ion battery includes a positive electrode membrane including a positive electrode active material, a binder, and a conductive agent, and a negative electrode membrane including a negative electrode active material, a binder, and a conductive agent.
According to other embodiments of the lithium ion battery of the present invention, the positive active material is selected from the group consisting of lithium cobaltate, lithium nickel cobalt manganese ternary material, lithium iron phosphate and lithium manganate.
According to other embodiments of the lithium ion battery of the present invention, the negative active material is graphite.
According to the lithium ion battery of other embodiments of the present invention, the upper charging limit voltage of the lithium ion battery is 4.5V.
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 present embodiment provides an electrolyte, wherein the weight ratio of each solvent in the electrolyte is ethylene carbonate: diethyl carbonate: 1 of propylene carbonate: 1: 1. the lithium salt was selected to be lithium hexafluorophosphate, which was present at a concentration of 1.1 mol/L. The electrolyte comprises the following two additives in a ratio based on the total weight of the electrolyte: 1 wt% of pentafluorophenyl house sulfonate and 1 wt% of vinyl sulfate.
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.
The lithium ion battery is prepared by the following steps:
(1) preparing a positive plate:
selecting high-voltage lithium cobaltate particles as a positive electrode active material, carbon nanotubes as a conductive agent, polyvinylidene fluoride (PVDF) as a binder, and mixing the materials in a ratio of 97: 1.5: 1.5 in N-methyl pyrrolidone solvent, fully stirring and uniformly mixing to form uniform anode slurry, and coating the uniform anode slurry on an anode current collector aluminum foil. And drying and cold pressing to obtain the positive plate.
(2) Preparing a negative plate:
selecting graphite as a negative electrode active substance, acetylene black as a conductive agent, styrene butadiene rubber as a binder and carboxymethyl cellulose as a thickening agent, wherein the weight ratio of the graphite to the acetylene black is 95: 2: 2: 1, fully stirring and uniformly mixing in deionized water to form uniform negative electrode slurry, and coating the uniform negative electrode slurry on a negative electrode current collector copper foil. And drying and cold pressing to obtain the required negative plate.
(3) And sequentially stacking and winding the positive plate, the diaphragm and the negative plate to form the naked battery cell. And placing the bare cell in an outer packaging bag, injecting the electrolyte, and performing vacuum packaging, standing, formation, shaping and other processes to complete the preparation of the lithium ion battery.
Example 2
High rate discharge test
Referring to example 1, the amounts of pentafluorophenyl methanesulfonate and vinyl sulfate were adjusted to obtain electrolytes of different ratios, and different lithium ion batteries were prepared according to the obtained electrolytes, wherein the specific numbers of the ratios are shown in the following table:
TABLE 1 content of additives for lithium ion batteries
Discharging each lithium ion battery obtained according to the electrolyte formula at 25 ℃ in a half-charge state to 3.0V by using 0.5C, fully charging at a constant current and a constant voltage of 0.5C, discharging to 3.0V by using currents of 0.5C, 1C, 3C, 5C and 10C with different multiplying factors, respectively recording discharge capacity, finishing reference (100%) by using 0.5C discharge capacity, and calculating discharge capacity under different multiplying factors to obtain discharge test data with different multiplying factors, wherein the discharge test data are specifically shown in the following table 2:
TABLE 2 results of the Large Rate discharge experiment
| Battery numbering | 0.5C | 1C | 3C | 5C | 10C |
| L1# | 100％ | 85.40％ | 70.10％ | 35.60％ | 1.00％ |
| L2# | 100％ | 87.10％ | 73.50％ | 40.30％ | 5.00％ |
| L3# | 100％ | 87.50％ | 74.00％ | 45.40％ | 10.00％ |
| L4# | 100％ | 88.00％ | 75.30％ | 46.70％ | 16.70％ |
| L5# | 100％ | 88.40％ | 75.90％ | 47.50％ | 23.80％ |
| L6# | 100％ | 92.30％ | 80.40％ | 56.20％ | 30.40％ |
| L7# | 100％ | 94.10％ | 81.30％ | 60.30％ | 40.00％ |
| L8# | 100％ | 96.30％ | 85.60％ | 65.60％ | 50.40％ |
| L9# | 100％ | 93.60％ | 80.60％ | 58.70％ | 45.70％ |
| L10# | 100％ | 91.40％ | 78.40％ | 53.10％ | 31.20％ |
| L11# | 100％ | 92.50％ | 80.65％ | 54.20％ | 33.10％ |
| L12# | 100％ | 94.80％ | 81.20％ | 61.50％ | 35.60％ |
| L13# | 100％ | 95.60％ | 81.70％ | 62.30％ | 38.70％ |
From the above test results, it is understood that the discharge capacity at a discharge rate of 5C/10C is significantly increased for L6# -L13 # as compared with that for battery L1# -L5 # as a comparative example. Compared with L6# to L9#, the 5C/10C discharge capacity is increased along with the increase of the content of the pentafluorophenyl methanesulfonate, but when the content of the pentafluorophenyl methanesulfonate additive is more than 3%, the film formation becomes thicker, the impedance is increased, and the 5C/10C discharge is worsened. Similarly, when the content of ethylene sulfate (DTD) is greater than 5%, the film thickness is increased, the impedance is increased, and the deterioration effect on 5C/10C discharge is caused by comparing L4# with L10# -L13 #.
In addition, compared with L1#, L2#, L3# and L12#, the electrolyte proportioning schemes of no additive, 3 wt% additive A, 1 wt% additive B, 3 wt% additive A and 1 wt% additive B are respectively as follows:
(1) after the additive A is singly added in an amount of 3 wt%, the discharge capacity at the discharge rate of 5C is increased by about 5%, and the discharge capacity at the discharge rate of 10C is increased by 4%;
(2) after 1 wt% of the additive B is added alone, the discharge capacity at 5C discharge rate is increased by about 10%, and the discharge capacity at 10C discharge rate is increased by 9%;
(3) the addition of the combination of 3 wt% additive a and 1 wt% additive B increased the discharge capacity at 5C discharge rate by 26% (well above 5% + 10%) and at 10C discharge rate by 35% (well above 4% + 9%).
Therefore, the two additives are combined and matched with each other, so that the discharge capacity under the condition of high-rate discharge can be obviously improved, and the requirements of some existing products on the high-rate discharge performance can be effectively met.
Example 3
Low temperature discharge test
The cells of example 2 in each half-charge state were discharged to 3.0V at 25 ℃ at 0.5C, then charged to 4.45V at 0.5C with constant current and constant voltage, and discharged to 3.0V at 0.5C, and the initial capacity was recorded. Then the cell was placed in a constant humidity cabinet at-40 ℃ for 4 hours, and then discharged to 3.0V with 0.5C, and the discharge capacity was recorded.
Capacity retention (%) of-40 ℃ discharge capacity (mAh)/initial capacity (mAh) × 100%
The results of the low temperature discharge test of each cell are shown in table 3.
TABLE 3 Low temperature discharge test results
From the test results, compared with the batteries L1# -L5 # of the electrolyte of the comparative example, the discharge capacity of the battery cells L6# -L13 # adopting the technical scheme of the application is obviously increased at the temperature of-40 ℃. As can be seen from comparison of L6# to L9#, the discharge capacity at-40 ℃ is increased with the increase of the content of pentafluorophenyl methanesulfonate, but when the content of the pentafluorophenyl methanesulfonate additive is more than 3%, the film formation becomes thicker, the impedance is increased, and the deterioration effect on low-temperature discharge is caused. Similarly, when the content of vinyl sulfate is greater than 5%, the film becomes thicker and the impedance increases, which adversely affects the deterioration of low-temperature discharge, in comparison with L4# and L10-L13 #.
In addition, compared with L1#, L2#, L3# and L12#, the electrolyte proportioning schemes of no additive, 3 wt% additive A, 1 wt% additive B, 3 wt% additive A and 1 wt% additive B are respectively as follows:
(1) after the additive A with the weight percentage of 3 percent is added independently, the low-temperature discharge capacity is increased by 5.6 percent;
(2) after 1 wt% of additive B is added independently, the low-temperature discharge capacity is increased by 15.3%;
(3) the low temperature discharge capacity retention increased by 29.4% (well above 5.6% + 15.3%) after the addition of the combination of 3 wt% additive a and 1 wt% additive B.
Therefore, the two additives are combined and matched with each other, so that the discharge capacity under the low-temperature discharge condition can be obviously improved, and the requirement of the existing product on the low-temperature discharge performance is met.
Example 4
An electrolyte is provided, which is different from the electrolyte in example 1 in that an additive A is propylene sulfite, and an additive B is a compound of the following structural formula:
the lithium ion battery is prepared by the electrolyte according to the method of the embodiment 1, and the discharge capacity of the lithium ion battery can still be kept above 30% at the rate of 10C by the test of the embodiment 2.
Example 5
An electrolyte was provided, which differs from example 1 in that the additive a was propylene sulfate. The lithium ion battery prepared by the electrolyte according to the method of the embodiment 1 and tested by the method of the embodiment 2 can still keep the discharge capacity of more than 30% at the rate of 10C.
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, comprising a lithium salt, an organic solvent, an additive A and an additive B; based on the total weight of the electrolyte, the content of the additive A is 0.1-10%, and the content of the additive B is 0.1-5%;
the additive A has a structural formula shown as the following formula (I) or (II):
the additive B has a structural formula shown as the following formula (III):
wherein R is1、R2Are respectively and independently selected from C2-C6 alkyl; r3Selected from C1-C12 alkyl.
2. The electrolyte of claim 1, wherein the additive A is selected from the group consisting of vinyl sulfate, propylene sulfate, vinyl sulfite, and propylene sulfite.
3. The electrolyte of claim 1, wherein additive B is pentafluorophenyl methanesulfonate.
4. The electrolyte of claim 1, wherein the additive a is present in an amount of 0.3% to 5% based on the total weight of the electrolyte.
5. The electrolyte of claim 1, wherein the additive B is present in an amount of 0.2% to 3% based on the total weight of the electrolyte.
6. The electrolyte of any one of claims 1 to 5, wherein the lithium salt is a fluorine-containing lithium salt.
7. The electrolyte of claim 6, wherein the fluorine-containing lithium salt is selected from the group consisting of lithium hexafluorophosphate, lithium hexafluoroarsenate, lithium perchlorate, lithium trifluorosulfonyl, lithium difluoro (trifluoromethylsulfonyl) imide, lithium bis (fluorosulfonyl) imide, and lithium tris (trifluoromethylsulfonyl) methide.
8. The electrolyte of any one of claims 1 to 5, wherein the concentration of the lithium salt is 0.5mol/L to 2 mol/L.
9. The electrolyte according to any one of claims 1 to 5, wherein the organic solvent is selected from ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl formate, ethyl propionate, propyl propionate, methyl butyrate, tetrahydrofuran.
10. A lithium ion battery comprising a positive electrode sheet, a negative electrode sheet, a separator and an electrolyte, wherein the electrolyte is the electrolyte according to any one of claims 1 to 9.
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Cited By (1)
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| CN115513528A (en) * | 2022-11-21 | 2022-12-23 | 广州天赐高新材料股份有限公司 | Nonaqueous electrolyte solution and secondary battery |
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Application publication date: 20200508 |