CN111834665A - High-nickel ternary lithium ion battery electrolyte and lithium ion battery - Google Patents
High-nickel ternary lithium ion battery electrolyte and lithium ion battery Download PDFInfo
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- CN111834665A CN111834665A CN202010585097.2A CN202010585097A CN111834665A CN 111834665 A CN111834665 A CN 111834665A CN 202010585097 A CN202010585097 A CN 202010585097A CN 111834665 A CN111834665 A CN 111834665A
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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
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0563—Liquid materials, e.g. for Li-SOCl2 cells
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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
- H01M2300/002—Inorganic 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 discloses a high-nickel ternary lithium ion battery electrolyte, which comprises a non-aqueous organic solvent, electrolyte lithium salt and an additive, wherein the additive comprises at least one sulfonate pyridinium additive with a specific structure. The invention also discloses a lithium ion battery comprising the positive plate, the isolating membrane, the negative plate and the high-nickel ternary lithium ion battery electrolyte. The reduction potential of the pyridine sulfonate additive is 1.6V vs Li+about/Li, which is reduced to form film in preference to solvent and conventional additive, plays a role in stabilizing the passive film of the negative electrode, and has the film forming function of the positive electrode with the oxidative decomposition potential of 4.35V vs Li+The Li has a promoting effect on the protection of the anode material, and can effectively improve the cycle performance, the high-temperature storage performance and the low-temperature performance of the ternary lithium ion battery.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to a high-nickel ternary lithium ion battery electrolyte and a lithium ion battery.
Background
The lithium ion battery has the advantages of high working voltage, high energy density, long service life, wide working temperature range, environmental friendliness and the like, and is widely applied to the fields of 3C digital products, electric tools, electric automobiles, aerospace and the like. Especially in the 3C digital field, mobile electronic devices, especially smart phones, have been rapidly developed in recent years toward lighter and thinner, and higher requirements are put forward on the energy density of lithium ion batteries.
In order to increase the energy density of the lithium ion battery, a common measure is to increase the charge cut-off voltage of the positive electrode material, such as the voltage of the commercialized ternary material lithium ion battery from 4.2V → 4.35V → 4.4V → 4.6V. Another method for increasing the energy density of lithium ion batteries is to increase the nickel content in the ternary material, such as the commercialized ternary material from NCM111 → NCM422 → NCM523 → NCM622 → NCM811, and the energy density of the battery can be further increased with the increase of the nickel content, but there are some negative effects, such as too high alkalinity of the material, lattice energy change during charge and discharge, material structure collapse and ion elution, and the like due to Ni4+Has stronger oxidizability, when the passive film of the positive electrode interface is damaged, Ni4+The oxidative decomposition of the electrolyte is rapidly catalyzed.
Chinese patent publication No. CN106099183A discloses a pyridinium propanesulfonate additive, wherein the additive amount of the pyridinium propanesulfonate accounts for 0.1-10% of the total mass of the electrolyte, and the additive can play a role in improving the high-temperature performance of the battery and reducing the internal resistance. The disadvantage is that the solubility of the pyridine propanesulfonate additive in the electrolyte is very low, and when the addition amount exceeds 1 percent of the total mass of the electrolyte, the substances can not be completely dissolved. When the amount added was 10% of the total mass of the electrolyte, the electrochemical performance of the battery was very poor when compared with the comparative group.
At present, the main method for solving the problems is to develop a new film forming additive, the new film forming additive is required to be capable of forming a passivation film on the interface of a positive electrode material and a negative electrode material through oxidation reduction, the formed passivation film is compact, good and elastic, and can expand and contract along with the expansion and contraction of the positive electrode material and the negative electrode material in the charging and discharging processes, so that the cracking degree of the passivation film is reduced, and the electrochemical performance of the high-nickel ternary lithium ion battery is improved.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to provide a high-nickel ternary lithium ion battery electrolyte and a lithium ion battery, wherein a pyridinium sulfonate additive in the high-nickel ternary lithium ion battery electrolyte has good film-forming performance, can form films on a positive electrode and a negative electrode, protects materials, and reduces interface impedance, so that the cycle performance, the rate capability, the low-temperature discharge performance and the like of the high-nickel ternary lithium ion battery are effectively improved.
In order to achieve the purpose, the invention adopts the technical scheme that: a high-nickel ternary lithium ion battery electrolyte comprises a non-aqueous organic solvent, an electrolyte lithium salt and an additive, wherein the additive comprises at least one sulfonate pyridinium additive with a structure shown in a formula (I):
wherein R is selected from any one of alkyl, fluoroalkyl, phenyl and cyclohexyl.
Preferably, the pyridinium sulfonate additive is selected from at least one of the compounds having the following structures:
preferably, the content of the pyridine sulfonate additive is 0.1-1.0% of the total mass of the electrolyte.
Preferably, the additive further comprises a conventional additive, which is one or more of Vinylene Carbonate (VC), fluoroethylene carbonate (FEC), vinylethylene carbonate (VEC), 1, 3-Propanesultone (PS), 1, 3-Propene Sultone (PST), vinyl sulfate (DTD), tris (trimethylsilane) borate (TMSB), tris (trimethylsilane) phosphate (TMSP), tripropynyl phosphate and tripropynyl phosphate.
More preferably, the conventional additive is a mixture of Vinylene Carbonate (VC), 1, 3-Propane Sultone (PS), vinyl sulfate (DTD).
Preferably, the content of the conventional additive is 0.5-10.0% of the total mass of the electrolyte.
Preferably, the electrolyte lithium salt is a mixture of lithium hexafluorophosphate, lithium bis-fluorosulfonyl imide and lithium difluorophosphate, and the mass ratio of lithium hexafluorophosphate, lithium bis-fluorosulfonyl imide and lithium difluorophosphate in the mixture is 6.5-12.5: 1: 0.75-2.5.
Preferably, the content of the electrolyte lithium salt is 12.5 to 17.0 percent of the total mass of the electrolyte.
In the present invention, the non-aqueous organic solvent includes a cyclic carbonate-based solvent selected from at least one of Ethylene Carbonate (EC) and Propylene Carbonate (PC), and a chain carbonate-based solvent selected from one or more of dimethyl carbonate (DMC), diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC). Preferably, the non-aqueous organic solvent is a mixture of Ethylene Carbonate (EC), Propylene Carbonate (PC), diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC). More preferably, the mass ratio of the ethylene carbonate, the propylene carbonate, the diethyl carbonate and the ethyl methyl carbonate is (10-30): (5-10): (5-20): (40-70), and the mass ratio is more preferably 25: 5: 10: 60.
the invention also discloses a lithium ion battery which comprises a positive plate, an isolating membrane, a negative plate and the high-nickel ternary lithium ion battery electrolyte.
Preferably, the charge cut-off voltage of the lithium ion battery is 4.2-4.35V.
Preferably, the positive electrode active material of the positive electrode sheet is LiNi1-x-y-zCoxMnyAlzO2Wherein: x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, z is more than or equal to 0 and less than or equal to 1, x + y + z is more than or equal to 0 and less than or equal to 1, the nickel content is more than or equal to 60 percent, and the negative active substance of the negative plate is artificial graphite, natural graphite or SiOwThe silicon-carbon composite material is compounded with graphite, wherein w is more than 1 and less than 2.
More preferably, the positive electrode active material is LiNi0.6Co0.2Mn0.2O2Or LiNi0.8Co0.1Mn0.1O2The preparation method of the positive plate comprises the following steps: LiNi as positive electrode active material0.6Co0.2Mn0.2O2Or LiNi0.8Co0.1Mn0.1O2The conductive agent acetylene black and the binder polyvinylidene fluoride (PVDF) are mixed according to the mass ratio of 96: 2.5: 1.5 fully stirring and uniformly mixing in an N-methyl pyrrolidone solvent system, coating on an aluminum foil, drying and cold pressing to obtain the positive plate, wherein the compaction density of the positive plate is 3.0-3.4 mg/cm3(ii) a The preparation method of the negative active material comprises the following steps: preparing negative active material artificial graphite, conductive agent acetylene black, binder Styrene Butadiene Rubber (SBR), and thickener carboxymethylcellulose sodium (CMC) according to a mass ratio of 96: 2: 1: 1, fully stirring and uniformly mixing in a deionized water solvent system, coating the mixture on a copper foil, drying and cold pressing to obtain a negative plate, wherein the compaction density of the negative plate is 1.5-1.6 mg/cm3。
Compared with the prior art, the invention has the beneficial effects that:
1. the pyridine sulfonate additive with the structure shown in formula (I) has the function of anode film formation, and the oxidative decomposition potential is 4.35V vs Li+Li, having a significant promoting effect on the protection of the positive electrode material (Ni)4+Has strong oxidizability, protects the anode and avoids Ni4+Oxidative decomposition of the electrolyte), thereby significantly improving the electrochemical performance of the battery;
2. the reduction potential of the pyridine sulfonate additive with the structure shown in formula (I) is 1.6vs Li/Li+On the left and right sides, the reduction can be performed on the cathode graphite interface in preference to the solvent and the conventional additives, and the reduction product is complemented and interacted with substances formed by reduction of the conventional additives such as Vinylene Carbonate (VC), vinyl sulfate (DTD) and 1, 3-Propane Sultone (PS), so that a passivation film formed after formation and capacity grading of the battery has more compact and stable characteristics, and the electrochemical performance of the battery is further improved;
3. the DTD and LiFSI in the electrolyte are combined, so that the corrosion hazard of LiFSI to the anode aluminum foil can be preferentially inhibited, an excellent interface protective film can be formed on the surface of an electrode, the reactivity of the electrode material and the electrolyte is reduced, the microstructure of the electrode material is stabilized, and the electrochemical performance of a lithium ion battery is improved.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail with reference to the following embodiments. It is to be understood that the following description is only illustrative of the present invention and is not to be construed as limiting the present invention.
The pyridine sulfonate-based additives of the examples and comparative examples are characterized as follows:
the structural formula of the compound (1) is as follows:
the structural formula of the compound (2) is as follows:
example 1
Preparing an electrolyte: in a glove box filled with argon, Ethylene Carbonate (EC), Propylene Carbonate (PC), diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC) were mixed in a mass ratio of EC: PC: DEC: EMC 25: 5: 10: 60 to obtain a mixed solution, and then slowly adding 12.5 wt% of lithium hexafluorophosphate (LiPF) based on the total mass of the electrolyte to the mixed solution6) 1.0 wt% of lithium difluorophosphate (LiPO) based on the total mass of the electrolyte2F2) And 2.5 wt% of lithium bis (fluorosulfonyl) imide (LiFSI) based on the total mass of the electrolyte, and finally adding a pyridinium sulfonate additive compound (2) accounting for 0.3 wt% of the total mass of the electrolyte, and uniformly stirring to obtain the lithium ion battery electrolyte of example 1.
Examples 2 to 6 and comparative examples 1 to 6
Examples 2 to 6 and comparative examples 1 to 6 were the same as example 1 except that the components of the electrolyte were added in the proportions shown in Table 1.
TABLE 1 composition ratios of the components of the electrolytes of examples 1-6 and comparative examples 1-6
Note: the concentration of each component in the lithium salt is the mass percentage content in the electrolyte;
the content of the pyridine sulfonate additive is the mass percentage content in the electrolyte;
the content of each component in the conventional additive is the mass percentage content in the electrolyte;
the proportion of each component in the nonaqueous organic solvent is mass ratio.
Performance testing
Preparing a lithium ion battery:
LiNi as positive electrode active material0.6Co0.2Mn0.2O2The conductive agent acetylene black and the binder polyvinylidene fluoride (PVDF) are mixed according to the mass ratio of 96: 2.5: 1.5 fully stirring and uniformly mixing in an N-methyl pyrrolidone solvent system, coating on an aluminum foil, drying, and cold pressing to obtain the positive plate.
Preparing negative active material artificial graphite, conductive agent acetylene black, binder Styrene Butadiene Rubber (SBR), and thickener carboxymethylcellulose sodium (CMC) according to a mass ratio of 96: 2: 1: 1, fully stirring and uniformly mixing in a deionized water solvent system, coating on a copper foil, drying, and cold pressing to obtain the negative plate.
Polyethylene (PE) is used as a base film, and a nano aluminum oxide coating is coated on the base film to be used as an isolating film.
The method comprises the following steps of sequentially laminating a positive plate, an isolating membrane and a negative plate, winding the positive plate, the isolating membrane and the negative plate along the same direction to obtain a bare cell, placing the bare cell in an outer package, respectively injecting electrolyte prepared in examples 1-6 and comparative examples 1-6, carrying out procedures of packaging, shelving at 45 ℃, forming by a high-temperature clamp, secondary packaging, capacity grading and the like to obtain the high-nickel ternary lithium ion battery, and carrying out performance test, wherein the test result is shown in table 2:
1) and (3) testing the normal-temperature cycle performance of the high-nickel ternary lithium ion battery: and (3) charging the battery after capacity grading to 4.3V at a constant current and a constant voltage of 1C and stopping the current to 0.05C at 25 ℃, then discharging to 3.0V at a constant current of 1C, and calculating the capacity retention rate of the 1000 th cycle after 1000 cycles of cycle of charge/discharge according to the cycle. The calculation formula is as follows:
the 1000 th cycle capacity retention ratio (%) (1000 th cycle discharge capacity/first cycle discharge capacity) × 100%.
2) Testing the gas production rate and the capacity residual rate of the high-nickel ternary lithium ion battery at a constant temperature of 60 ℃: firstly, the battery is circularly charged and discharged for 1 time (4.3V-3.0V) at the normal temperature at 0.5C, and the discharge capacity C of the battery before storage is recorded0Then charging the battery to 4.3V full-voltage state at constant current and constant voltage, and testing the thickness V of the battery before high-temperature storage by using a drainage method1Then the battery is put into a thermostat with the temperature of 60 ℃ for storage for 7 days, the battery is taken out after the storage is finished, and the volume V of the battery after the storage is tested after the battery is cooled for 8 hours2Calculating the gas production rate of the battery after the battery is stored for 7 days at the constant temperature of 60 ℃; after the battery is cooled for 24 hours at room temperature, the battery is discharged to 3.0V at constant current of 0.5C again, and the discharge capacity C after the battery is stored is recorded1And calculating the capacity residual rate of the battery after 7 days of constant-temperature storage at 60 ℃, wherein the calculation formula is as follows:
the gas production of the battery is V after 7 days of storage at 60 DEG C2-V1；
Capacity remaining rate after 7 days of constant temperature storage at 60 ═ C1/C0)*100％。
3) And (3) testing the 45 ℃ cycle performance of the high-nickel ternary lithium ion battery: and (3) charging the battery after capacity grading to 4.3V at a constant current and a constant voltage of 1C at 45 ℃, stopping the current to 0.05C, then discharging to 3.0V at a constant current of 1C, and calculating the capacity retention rate of the 500 th cycle after the battery is cycled according to the cycle and is charged/discharged for 500 cycles. The calculation formula is as follows:
the 500 th cycle capacity retention ratio (%) (500 th cycle discharge capacity/first cycle discharge capacity) × 100%.
Table 2 results of testing cycle performance and high-temperature storage performance of batteries of examples and comparative examples
As can be seen from the comparison of the results of the cell performance test of comparative example 1 and examples 1-3 in Table 2: the pyridine sulfonate additive with a specific structure can obviously improve the cycle performance of the battery and the capacity retention rate after high-temperature storage. Through Cyclic Voltammetry (CV), the substance can be reduced to form a film in a negative electrode graphite interface preferentially by a solvent/other additives, and the reduction potential is 1.6V vs Li+and/Li or so.
As can be seen from the comparison of comparative examples 3 to 4 with examples 1 to 3 in Table 2, the results of the cell performance test: the addition amount of the pyridine sulfonate additive is preferably 0.1-1.0%, when the addition amount is too small, a passive film formed by the substance on an interface of a positive electrode material and a negative electrode material is not stable enough, and when the addition amount is too large, the passive film becomes thick, the impedance is increased, and the electrochemical performance of the ternary lithium ion battery is poor.
As can be seen from the comparison of the results of the cell performance tests of comparative examples 5 to 6 in Table 2: the DTD has an obvious effect of improving the performance of the battery, and the reason is that the combination of the DTD and the LiFSI can preferentially inhibit corrosion damage of LiFSI to the anode aluminum foil, and meanwhile, an excellent interface protective film can be formed on the surface of an electrode, so that the reactivity of the electrode material and electrolyte is reduced, and the microstructure of the electrode material is stabilized, thereby improving the electrochemical performance of the lithium ion battery.
As can be seen from the comparison of the results of the battery performance tests of examples 1-3 and examples 4-6 in Table 2: the combined action of the uniquely combined conventional additive and the sulfonate pyridine salt additive with a specific structure effectively improves the cycle performance, the high-temperature storage performance and the low-temperature performance of the ternary lithium ion battery.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (10)
1. The high-nickel ternary lithium ion battery electrolyte comprises a non-aqueous organic solvent, an electrolyte lithium salt and an additive, and is characterized in that the additive comprises at least one sulfonate pyridinium additive with the structure shown in the formula (I):
wherein R is selected from any one of alkyl, fluoroalkyl, phenyl and cyclohexyl.
2. The high-nickel ternary lithium ion battery electrolyte of claim 1, wherein the pyridinium sulfonate additive is selected from at least one of the compounds having the following structures:
3. the high-nickel ternary lithium ion battery electrolyte of claim 1, wherein the content of the pyridinium sulfonate additive is 0.1-1.0% of the total mass of the electrolyte.
4. The high-nickel ternary lithium ion battery electrolyte of claim 1, wherein the additives further comprise conventional additives, and the conventional additives are one or more of vinylene carbonate, fluoroethylene carbonate, vinyl ethylene carbonate, 1, 3-propane sultone, 1, 3-propene sultone, vinyl sulfate, tris (trimethylsilane) borate, tris (trimethylsilane) phosphate, tripropylene phosphate, and tripropylene phosphate.
5. The high-nickel ternary lithium ion battery electrolyte of claim 4, wherein the conventional additives are vinylene carbonate, 1, 3-propane sultone, sulfur
Mixtures of vinyl esters of acids.
6. The high-nickel ternary lithium ion battery electrolyte according to claim 4, wherein the content of the conventional additive is 0.5-10.0% of the total mass of the electrolyte.
7. The high-nickel ternary lithium ion battery electrolyte solution according to claim 1, wherein the electrolyte lithium salt is a mixture of lithium hexafluorophosphate, lithium bis-fluorosulfonyl imide and lithium difluorophosphate, and the mass ratio of the lithium hexafluorophosphate, the lithium bis-fluorosulfonyl imide and the lithium difluorophosphate in the mixture is 6.5-12.5: 1: 0.75-2.5.
8. The high-nickel ternary lithium ion battery electrolyte according to claim 1, wherein the content of the electrolyte lithium salt is 12.5-17.0% of the total mass of the electrolyte.
9. The high nickel ternary lithium ion battery electrolyte of claim 1 wherein the non-aqueous organic solvent is a mixture of ethylene carbonate, propylene carbonate, diethyl carbonate and ethyl methyl carbonate.
10. A lithium ion battery, characterized in that the lithium ion battery comprises a positive plate, a separation film, a negative plate and the high nickel ternary lithium ion battery electrolyte of any of claims 1-9.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112687956A (en) * | 2020-12-28 | 2021-04-20 | 远景动力技术(江苏)有限公司 | Non-aqueous electrolyte of lithium battery and lithium ion battery based on same |
| CN114006044A (en) * | 2021-10-25 | 2022-02-01 | 惠州亿纬锂能股份有限公司 | High-voltage electrolyte and application thereof |
| CN114552001A (en) * | 2020-11-24 | 2022-05-27 | 中国科学院大连化学物理研究所 | Electrolyte for improving high-temperature shelving performance of ternary lithium ion battery and application |
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| CN114006044A (en) * | 2021-10-25 | 2022-02-01 | 惠州亿纬锂能股份有限公司 | High-voltage electrolyte and application thereof |
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Effective date of registration: 20230928 Address after: No.62 Huayin North Road, Kecheng District, Quzhou City, Zhejiang Province Patentee after: New Asia Shanshan New Material Technology (Quzhou) Co.,Ltd. Address before: 523073 plant 5, plant 2, shuilian Pengdong Industrial Zone, Nancheng District, Dongguan City, Guangdong Province Patentee before: DONGGUAN SHANSHAN BATTERY MATERIALS Co.,Ltd. |