CN110931866A - Lithium ion battery electrolyte - Google Patents
Lithium ion battery electrolyte Download PDFInfo
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- CN110931866A CN110931866A CN201911170479.2A CN201911170479A CN110931866A CN 110931866 A CN110931866 A CN 110931866A CN 201911170479 A CN201911170479 A CN 201911170479A CN 110931866 A CN110931866 A CN 110931866A
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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
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Abstract
The invention discloses a lithium ion battery electrolyte, which comprises a lithium salt electrolyte, a non-aqueous organic solvent and at least three combined electrolyte additives. The invention has the advantages that: (1) a negative electrode SEI film substance with lower relative impedance is formed, so that the interface performance and compatibility of the electrolyte and the negative electrode material of the lithium ion battery are improved; (2) the cycle life of the lithium ion battery is prolonged.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to a lithium ion battery electrolyte.
Background
Lithium ion batteries have been commercialized by Sony corporation of japan since 1990 to have a recent history of over 20 years. Because of higher volumetric energy, gravimetric energy and good environmental protection, the battery gradually replaces the traditional lead-acid battery, Ni-Cd and MH-Ni battery, and is widely used in portable 3C electronic equipment such as mobile phones, notebook computers and the like, thereby rapidly occupying a large market and rapidly developing. With the demand for smaller, lighter, and thinner electronic products becoming stronger in recent years, in addition to the pursuit of lower prices, the pursuit of higher energy density is a strong driving force for improving electronic products.
The electrolyte is an important component of the battery, and although the electrolyte does not contribute to the energy of the battery, the composition of the electrolyte directly affects the cycle capacity and the service life of the battery. The electrolyte with proper composition (related to selection and dosage of salt, solvent and additive) can effectively exert and improve the electrochemical properties of the anode and cathode materials of the lithium ion battery, such as cycle life, capacity maintenance, high-temperature storage, safety performance, rate discharge characteristic, discharge platform time, capacity exertion of the anode and cathode, and the like.
In general, during the first charge and discharge of a lithium ion battery, components such as a solvent or an additive in an electrolyte undergo reductive decomposition and the product is deposited on the surface of a negative electrode material graphite to form a solid electrolyte interface film (SEI film), or oxidative decomposition and the product is deposited on the surface of a positive electrode material to form a positive electrode interface protective film. The good and dense interface protective film can alleviate the decomposition of the electrolyte, thereby reducing the irreversible capacity of the battery and improving the cycle performance of the battery. Optimizing the electrolyte composition and selecting appropriate solvents, lithium salts, and additives are effective ways to improve the interfacial film.
Since the commercialization of lithium ion batteries 1990, it has been very extensive to develop additives for improving the film-forming properties of negative electrodes and to study their mechanism of action and film-forming components. For example, the inorganic additives currently used for improving the SEI performance of the negative electrode are mainly CO2, SO2, and the like. Organic additives which have been successfully developed include 1, 2-Vinylene Carbonate (VC), halogenated ethylene carbonate (X-EC, X ═ F, Cl, etc.), ethylene sulfite, and 1, 3-Propane Sultone (PS). The additives have the main functions of inhibiting the decomposition of the electrolyte by being subjected to reductive decomposition in preference to the electrolyte solvent, forming good SEI on a graphite negative electrode and improving the reversible capacity and stability of the electrode.
In fact, one of the most important factors in the life decay of lithium ion batteries is that lithium ions are continuously consumed by the regeneration of SEI during the cycle; although the volume expansion rate of the graphite negative electrode is lower than that of other negative electrodes with high energy density, the volume expansion rate is about 10%, the volume of the graphite negative electrode continuously expands along with the continuous circulation of the battery, the mechanical internal stress caused by the continuous expansion of the graphite negative electrode can cause the damage and continuous regeneration of a negative electrode SEI film, the lithium ions can be continuously consumed by the regenerated SEI film, and the cycle life of the battery is continuously reduced.
Therefore, it is important for the life of the battery to be affected by an effective electrolyte additive combination having excellent compatibility with the positive and negative electrode materials of the lithium ion battery to form an SEI film having a stable composition and a low impedance.
Disclosure of Invention
The invention aims to overcome the technical defects and provide the lithium ion battery electrolyte, which improves the interface performance and compatibility of the electrolyte and a lithium ion battery cathode material, effectively reduces battery impedance and prolongs the cycle life of the battery.
In order to solve the technical problems, the technical scheme provided by the invention is as follows: a lithium ion battery electrolyte comprises a lithium salt electrolyte, a non-aqueous organic solvent and at least three combined electrolyte additives.
The invention has the advantages that: (1) a negative electrode SEI film substance with lower relative impedance is formed, so that the interface performance and compatibility of the electrolyte and the negative electrode material of the lithium ion battery are improved; (2) the cycle life of the lithium ion battery is prolonged.
Preferably, a first of said combined electrolyte additives comprises at least: succinic anhydride, maleic anhydride, thiophene and antipyrine.
Preferably, a second of said combined electrolyte additives comprises at least: any one of allyl sulfate, 4-methyl vinyl sulfate, 4-ethyl vinyl sulfate and 4-propyl vinyl sulfate.
Preferably, a third of the combined electrolyte additives comprises lithium carbonate.
Compared with the prior electrolyte additive technology, the combined electrolyte additive is beneficial to the formation of an interfacial film with lower resistance, and finally the cycle life of the battery is improved.
Preferably, the lithium salt electrolyte is at least one of LiPF6, LiBF4, LiBOB, liddob, LiTFSi, and LiFSi; the mass concentration of the lithium salt electrolyte in the electrolyte is 0.2-2 mol/L; the nonaqueous organic solvent accounts for 76-87.5% of the total weight of the electrolyte; the combined electrolyte additive accounts for 0.5-10% of the total weight of the electrolyte.
Preferably, the lithium salt electrolyte has a mass concentration of 0.8 to 1.5mol/L in the electrolyte.
Preferably, the combined electrolyte additive accounts for 0.5-7% of the total weight of the electrolyte.
Preferably, the non-aqueous organic solvent is a mixture of at least two or more of ethylene carbonate, propylene carbonate, ethyl methyl carbonate, dimethyl carbonate and diethyl carbonate.
The composition of the electrolyte screens and combines the types of the additives aiming at the respective physicochemical characteristics of the nonaqueous organic solvent and the additives, and finds the proportion of the additives of the electrolyte, which can exert the respective advantages and mutually inhibit the respective disadvantages, thereby not only improving the compatibility of the nonaqueous organic solvent ethylene carbonate and methyl ethyl carbonate with the active electrode material, but also leading the active substance to exert the optimal electrochemical performance, forming an interface film with low impedance on the surface of the active substance, and improving the capacity and the cycle life of the battery.
Drawings
FIG. 1 is a graph showing the normal temperature 1C charge-discharge cycle performance test of the NCM523/AG 1Ah soft pack lithium ion battery of examples 1-3 and comparative examples 1-3 according to the present invention.
FIG. 2 is a graph of the AC impedance after the normal temperature 1C charge-discharge cycle to 100 weeks of the NCM523/AG 1Ah soft pack lithium ion batteries of examples 1-3 and comparative examples 1-3 according to the present invention.
Detailed Description
The present invention will be described in further detail with reference to the accompanying drawings.
Example 1:
the lithium ion battery electrolyte comprises the following specific formula: 25.45g of ethylene carbonate, 16.96g of ethylmethyl carbonate, 42.41g of dimethyl carbonate, 0.5g of succinic anhydride (CAS No.108-30-5), 1.5g of propylene sulfate (CAS No.1073-05-8) and 0.5g of lithium carbonate (99.9%). The electrolyte is LiPF 6; the preparation method comprises the following steps: preparing electrolyte in a BRAUN glove box, wherein the glove box is filled with argon with the purity of 99.999 percent, the water content in the glove box is controlled to be less than or equal to 5ppm, and the temperature is room temperature; uniformly mixing the ethylene carbonate, the ethyl methyl carbonate and the dimethyl carbonate solvent, cooling to-20 ℃, adding the electrolyte LiPF6, fully mixing to form 1.05mol/L LiPF6 electrolyte solution, and finally respectively adding the three additives in the weight parts, and uniformly mixing.
Example 2:
the lithium ion battery electrolyte comprises the following specific formula: 25.45g of ethylene carbonate, 16.96g of ethylmethyl carbonate, 42.11g of dimethyl carbonate, 0.8g of succinic anhydride (CAS No.108-30-5), 1.5g of propylene sulfate (CAS No.1073-05-8) and 0.5g of lithium carbonate (99.9%). The electrolyte is LiPF 6; the preparation method comprises the following steps: preparing electrolyte in a BRAUN glove box, wherein the glove box is filled with argon with the purity of 99.999 percent, the water content in the glove box is controlled to be less than or equal to 5ppm, and the temperature is room temperature; uniformly mixing the ethylene carbonate, the ethyl methyl carbonate and the dimethyl carbonate solvent, cooling to-20 ℃, adding the electrolyte LiPF6, fully mixing to form 1.05mol/L LiPF6 electrolyte solution, and finally respectively adding the three additives in the weight parts, and uniformly mixing.
Example 3:
the lithium ion battery electrolyte comprises the following specific formula: 25.45g of ethylene carbonate, 16.96g of ethylmethyl carbonate, 41.91g of dimethyl carbonate, 0.5g of succinic anhydride (CAS No.108-30-5), 2.0g of propylene sulfate (CAS No.1073-05-8) and 0.5g of lithium carbonate (99.9%). The electrolyte is LiPF 6; the preparation method comprises the following steps: preparing electrolyte in a BRAUN glove box, wherein the glove box is filled with argon with the purity of 99.999 percent, the water content in the glove box is controlled to be less than or equal to 5ppm, and the temperature is room temperature; uniformly mixing the ethylene carbonate, the ethyl methyl carbonate and the dimethyl carbonate solvent, cooling to-20 ℃, adding the electrolyte LiPF6, fully mixing to form 1.05mol/L LiPF6 electrolyte solution, and finally respectively adding the three additives in the weight parts, and uniformly mixing.
Comparative example 1 (no lithium carbonate):
preparing electrolyte in a BRAUN glove box, wherein the glove box is filled with argon with the purity of 99.999 percent, the water content in the glove box is controlled to be less than or equal to 5ppm, and the temperature is room temperature; evenly mixing 25.45g of ethylene carbonate, 16.96g of ethyl methyl carbonate and 42.41g of dimethyl carbonate, cooling to-20 ℃, then adding an electrolyte LiPF6, fully mixing to form a 1.05mol/L LiPF6 electrolyte solution, and finally respectively adding 0.5g of succinic anhydride (CAS No.108-30-5) and 1.5g of propylene sulfate (CASNO.1073-05-8) and evenly mixing.
Comparative example 2 (no first additive):
preparing electrolyte in a BRAUN glove box, wherein the glove box is filled with argon with the purity of 99.999 percent, the water content in the glove box is controlled to be less than or equal to 5ppm, and the temperature is room temperature; after 25.45g of ethylene carbonate, 16.96g of ethyl methyl carbonate and 42.41g of dimethyl carbonate are uniformly mixed, the mixture is cooled to the temperature of minus 20 ℃, then an electrolyte LiPF6 is added and fully mixed to form a LiPF6 electrolyte solution of 1.05mol/L, and finally 0.5g of lithium carbonate and 1.5g of propylene sulfate (CAS No.1073-05-8) are respectively added and uniformly mixed.
Comparative example 3 (no second additive):
preparing electrolyte in a BRAUN glove box, wherein the glove box is filled with argon with the purity of 99.999 percent, the water content in the glove box is controlled to be less than or equal to 5ppm, and the temperature is room temperature; after 25.45g of ethylene carbonate, 16.96g of ethyl methyl carbonate and 42.41g of dimethyl carbonate are uniformly mixed, the mixture is cooled to-20 ℃, then electrolyte LiPF6 is added and fully mixed to form 1.05mol/L LiPF6 electrolyte solution, and finally 0.5g of succinic anhydride (CAS No.108-30-5) and 0.5g of lithium carbonate are respectively added and uniformly mixed.
The test method comprises the following steps:
the method comprises the steps of taking a nickel-cobalt-manganese 523 material as a positive electrode and taking Artificial Graphite (AG) as a negative electrode to manufacture a soft package lithium ion battery dry cell with the capacity of 1Ah, drying the dry cell in an oven at the temperature of 80-85 ℃ for 48h, and then moving the dry cell into a glove box for standby.
Respectively injecting the electrolyte obtained in each of the examples 1-3 and the comparative examples 1-3 into the dried dry cell, standing for 24h, pre-charging for one time, sealing, and performing secondary formation to obtain experimental batteries of the examples 1-3 and the comparative examples 1-3; the normal temperature charge and discharge performance of the material is compared with that of the material shown in figure 1. It is apparent that the discharge capacities of examples 1 to 3 were still stable at a high level when the number of cycles was close to 300 weeks, while the curves of comparative examples 1 to 3 exhibited a tendency to gradually decrease. In addition, after testing each battery and cycling for 100 weeks at normal temperature, testing the respective AC impedance spectrum (0.1 Hz-0.1 MHz10mV) in comparison with that shown in FIG. 2, referring to the relevant equivalent simulation circuit diagram model, it can be seen that the SEI film impedance (RSEI) and the charge transfer impedance (Rct) formed by examples 1-3 are significantly lower than those of comparative examples 1-3. Therefore, the application of the lithium ion battery electrolyte additive combination finally improves the cycle life of the battery and reduces the impedance of the battery.
The present invention and its embodiments have been described above, and the description is not intended to be limiting, and the drawings are only one embodiment of the present invention, and the actual structure is not limited thereto. In summary, those skilled in the art should appreciate that they can readily use the disclosed conception and specific embodiments as a basis for designing or modifying other structures for carrying out the same purposes of the present invention without departing from the spirit and scope of the invention as defined by the appended claims.
Claims (8)
1. A lithium ion battery electrolyte is characterized in that: comprises lithium salt electrolyte, non-aqueous organic solvent and at least three combined electrolyte additives.
2. The lithium ion battery electrolyte of claim 1, wherein: a first of said combined electrolyte additives comprises at least: succinic anhydride, maleic anhydride, thiophene and antipyrine.
3. The lithium ion battery electrolyte of claim 1, wherein: a second of the combined electrolyte additives comprises at least: any one of allyl sulfate, 4-methyl vinyl sulfate, 4-ethyl vinyl sulfate and 4-propyl vinyl sulfate.
4. The lithium ion battery electrolyte of claim 1, wherein: a third one of the combined electrolyte additives comprises lithium carbonate.
5. The lithium ion battery electrolyte of claim 1, wherein: the lithium salt electrolyte is at least one of LiPF6, LiBF4, LiBOB, LiDFOB, LiTFSi and LiFSI; the mass concentration of the lithium salt electrolyte in the electrolyte is 0.2-2 mol/L; the nonaqueous organic solvent accounts for 76-87.5% of the total weight of the electrolyte; the combined electrolyte additive accounts for 0.5-10% of the total weight of the electrolyte.
6. The lithium ion battery electrolyte of claim 1, wherein: the mass concentration of the lithium salt electrolyte in the electrolyte is 0.8-1.5 mol/L.
7. The lithium ion battery electrolyte of claim 1, wherein: the combined electrolyte additive accounts for 0.5-7% of the total weight of the electrolyte.
8. The lithium ion battery electrolyte of claim 1, wherein: the non-aqueous organic solvent is a mixture of at least two or more of ethylene carbonate, propylene carbonate, ethyl methyl carbonate, dimethyl carbonate and diethyl carbonate.
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| CN107706455A (en) * | 2017-09-20 | 2018-02-16 | 惠州亿纬锂能股份有限公司 | A kind of high voltage multiplying power electrolyte for taking into account high temperature performance and the lithium ion battery using the electrolyte |
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2019
- 2019-11-26 CN CN201911170479.2A patent/CN110931866A/en active Pending
Patent Citations (8)
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| CN101138125A (en) * | 2005-07-21 | 2008-03-05 | 松下电器产业株式会社 | Nonaqueous electrolyte secondary battery and its manufacturing method |
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