WO2021108995A1 - 二次电池、电解液以及包括该二次电池的装置 - Google Patents
二次电池、电解液以及包括该二次电池的装置 Download PDFInfo
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- WO2021108995A1 WO2021108995A1 PCT/CN2019/122741 CN2019122741W WO2021108995A1 WO 2021108995 A1 WO2021108995 A1 WO 2021108995A1 CN 2019122741 W CN2019122741 W CN 2019122741W WO 2021108995 A1 WO2021108995 A1 WO 2021108995A1
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- 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
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- 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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- 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
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- H01M10/0567—Liquid materials characterised by the additives
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- 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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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
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- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/021—Physical characteristics, e.g. porosity, surface area
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
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- H01M2220/00—Batteries for particular applications
- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
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- H—ELECTRICITY
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- 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
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
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- H—ELECTRICITY
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- 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
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
- H01M2300/004—Three solvents
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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
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
- H01M2300/0042—Four or more solvents
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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
Definitions
- This application relates to the field of energy storage, in particular to a secondary battery, an electrolyte, and a device including the secondary battery.
- the first aspect of the application relates to a secondary battery
- the secondary battery includes an electrolyte, the electrolyte includes an organic solvent, and the organic solvent includes a cyclic carbonate and a chain carbonate; a cyclic carbonate and a chain carbonate
- the mass ratio of carbonate is 25:75 ⁇ 32:68; the chain carbonate includes dimethyl carbonate (also abbreviated as "DMC" in this text); the dimethyl carbonate is in the chain carbonate
- the mass percentage is greater than or equal to 9 wt% and less than 50 wt%; wherein, based on the total mass of the organic solvent, the mass percentage of the carboxylic acid ester in the organic solvent is less than 5 wt%.
- the second aspect of the application relates to an electrolyte, the electrolyte includes an organic solvent, the organic solvent includes a cyclic carbonate and a chain carbonate; the mass ratio of the cyclic carbonate to the chain carbonate is 25:75 ⁇ 32:68; the chain carbonate includes dimethyl carbonate; the mass percentage of the dimethyl carbonate in the chain carbonate is greater than or equal to 9wt% and less than 50wt%; wherein, based on the total organic solvent The mass percentage of the carboxylic acid ester in the organic solvent is less than 5 wt%.
- the third aspect of the present application relates to a device including the secondary battery of the first aspect of the present application.
- the inventors of the present application found that by specifically controlling the ratio of cyclic carbonate to chain carbonate in the electrolyte and at the same time specifically controlling the content of dimethyl carbonate in the chain carbonate, the secondary battery can be both excellent Low temperature power and 45°C cycle performance.
- the inventors found that when the electrolyte meets the above conditions, the amount of carboxylic acid ester needs to be strictly controlled. When the content of the carboxylic acid ester is not within the range given in this application, the cycle performance of the battery is seriously affected. It can be seen that in this application, by simultaneously controlling the ratio of cyclic carbonate to chain carbonate, the content of dimethyl carbonate in chain carbonate, and the amount of carboxylic acid ester, the secondary battery exhibits excellent low-temperature power. And cycle performance.
- the device of the present application includes the secondary battery provided by the present application, and thus has at least the same advantages as the secondary battery.
- Fig. 1 is a schematic diagram of an embodiment of a secondary battery of the present application.
- Fig. 2 is a schematic diagram of an embodiment of a battery module of the present application.
- Fig. 3 is a schematic diagram of an embodiment of a battery pack of the present application.
- Fig. 4 is an exploded view of the battery pack of Fig. 3.
- Fig. 5 is a schematic diagram of an embodiment of a device of the present application.
- composition is described as including or including specific components, it is expected that the composition does not exclude optional components not involved in the present invention, and it is expected that the composition may be composed or composed of the involved components, or Where a method is described as including or including specific process steps, it is expected that the method does not exclude optional process steps not involved in the present invention, and it is expected that the method can be constituted or composed of the involved process steps.
- any lower limit can be combined with any upper limit to form an unspecified range; and any lower limit can be combined with other lower limits to form an unspecified range, and any upper limit can be combined with any other upper limit to form an unspecified range.
- every point or single value between the end points of the range is included in the range. Therefore, each point or single numerical value can be used as its own lower limit or upper limit in combination with any other point or single numerical value or in combination with other lower or upper limits to form an unspecified range.
- the secondary battery provided by the first aspect of the present application includes an electrolyte, which is characterized in that the electrolyte includes an organic solvent, and the organic solvent includes a cyclic carbonate and a chain carbonate; the mass ratio of the cyclic carbonate to the chain carbonate is 25:75 ⁇ 32:68; the chain carbonate includes dimethyl carbonate; the mass percentage of the dimethyl carbonate in the chain carbonate is greater than or equal to 9wt% and less than 50wt%; wherein, based on For the total mass of the organic solvent, the mass percentage of the carboxylic acid ester in the organic solvent is less than 5 wt%.
- organic solvent may have a meaning commonly understood in the battery field.
- organic solvent can be understood as a non-aqueous aprotic solvent that can be used as a carrier of active ions in a battery.
- organic solvents include cyclic carbonates, chain carbonates, carboxylic acid esters, and the like.
- the cyclic carbonate includes ethylene carbonate (also abbreviated as “EC” herein), propylene carbonate (also abbreviated as “PC” herein) and butylene carbonate (also abbreviated as “PC” herein). It can be abbreviated as "BC”); preferably, the cyclic carbonate includes ethylene carbonate.
- the chain carbonate also includes one or more of diethyl carbonate (also abbreviated as "DEC” in this document) and ethyl methyl carbonate (also abbreviated as “EMC” in this document) ;
- the chain carbonate also includes ethyl methyl carbonate.
- the inventor of the present application found that the relative content of cyclic carbonate and chain carbonate needs to be limited to a specific range.
- the excessive proportion of cyclic carbonate not only causes the viscosity of the electrolyte to increase at low temperatures, affects the low temperature conductivity of the electrolyte, and reduces the low temperature charge and discharge power of the battery, but also excessive cyclic carbonate
- the ester can undergo oxidation reaction on the positive electrode, which leads to the increase of battery gas production, which affects the charging interface, deteriorates the charging ability, and then affects the cycle performance at 45°C.
- the proportion of cyclic carbonate is too small, which leads to the decomposition of the electrolyte salt by the electrolyte.
- the reduction in separation capacity will affect the high-temperature conductivity of the electrolyte, resulting in greater polarization during the 45°C cycle of the battery, and under the action of the expansion force, the cycle performance will deteriorate.
- the mass ratio of cyclic carbonate to chain carbonate should be controlled at 25:75 ⁇ 32:68, which can favorably balance the high and low temperature conductivity of the electrolyte, so that the battery can obtain better Excellent 45°C cycle performance and low temperature power performance.
- the mass percentage of ethylene carbonate in the cyclic carbonate is greater than 90%, preferably 92%-100%.
- ethylene carbonate has a film-forming protective effect on the negative electrode active material, and controlling its content within a given range can further improve the cycle performance of the battery.
- the mass percentage of ethylene carbonate in the cyclic carbonate is greater than or equal to 94%, and even more preferably greater than or equal to 98%.
- the mass percentage of ethylene carbonate in the cyclic carbonate even reaches 100%.
- the mass percentage of dimethyl carbonate in the chain carbonate is 10% to 48% by weight, more preferably 15% to 45% by weight. In an exemplary embodiment, the mass percentage of dimethyl carbonate in the chain carbonate may be about 14 wt%, 18 wt%, 20 wt%, 25 wt%, 30 wt%, 35 wt%, or 40 wt%. The inventor found that by using the amount of dimethyl carbonate defined herein, good low-temperature conductivity and 45°C cycle performance can be obtained.
- dimethyl carbonate in the electrolyte effectively alleviates the deterioration of the charging ability caused by the increase of the expansion force of the battery during the cycle, which is beneficial to inhibit the increase of the expansion force in the battery, and thus is beneficial to the improvement of the battery cycle performance.
- too much dimethyl carbonate causes the low temperature conductivity and low temperature power of the electrolyte to decrease significantly.
- the decomposition of excessive dimethyl carbonate at the interface of the positive electrode increases gas production, resulting in serious battery flatulence, especially severely deteriorating the 45°C cycle performance of the battery.
- the carboxylic acid ester may include one or more of methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate, and propyl propionate.
- the carboxylic acid ester may include one or more of ethyl acetate and ethyl propionate.
- carboxylic acid esters compared with chain carbonates, carboxylic acid esters have the advantages of low viscosity and high dielectric constant, and their conductivity at room temperature and low temperature is usually higher than that of carbonate solvents.
- the electrolyte includes 3 wt% or less of carboxylic acid ester. Even more preferably, based on the total mass of the organic solvent, the organic solvent does not include the carboxylic acid ester (that is, the mass percentage of the carboxylic acid ester in the organic solvent is 0 wt%).
- the conductivity of the electrolyte at -20°C is greater than or equal to 2.5 mS/cm. More preferably, the conductivity of the electrolyte at -20°C is 2.6 mS/cm to 3.5 mS/cm. For example, the conductivity of the electrolyte at -20°C may be about 2.6 mS/cm, 2.8 mS/cm, 3.0 mS/cm, 3.2 mS/cm, or 3.4 mS/cm.
- the electrolyte may further include additives.
- the additives include, but are not limited to, fluoroethylene carbonate (FEC), vinylene carbonate (VC), ethylene sulfate (DTD), tris(trimethylsilane) phosphate (TMSP), lithium difluorooxalate One or more of (LiDFOB) and lithium bis(fluorosulfonyl)imide (LiFSI).
- FEC fluoroethylene carbonate
- VC vinylene carbonate
- DTD ethylene sulfate
- TMSP tris(trimethylsilane) phosphate
- LiDFOB lithium difluorooxalate
- LiFSI lithium bis(fluorosulfonyl)imide
- the above additives can further improve the chemical stability of the electrolyte, improve the stability of the film formation of the positive and negative interfaces, and at the same time modify the lithium ion transmission path of the interface film to have a lower interface impedance and repair the positive and
- the total amount of the additives does not exceed 10 wt% of the total mass of the electrolyte.
- the amount of each additive component may be 0.05-5wt%, preferably 0.1-3wt%.
- the amount of each additive component may be 0.1 wt%, 0.3 wt%, 0.5 wt%, 1 wt%, 1.5 wt%, 2 wt%, or 2.5 wt%. Too little additive content will result in incomplete film formation at the electrode interface and unstable structure; too much additive content will increase the resistance of the film formation or the residual redox decomposition will cause battery flatulence.
- the electrolyte described in this application also includes an electrolyte salt as a solute.
- the electrolyte salt may be selected from LiPF 6 (lithium hexafluorophosphate), LiBF 4 (lithium tetrafluoroborate), LiClO 4 (lithium perchlorate), LiAsF 6 (lithium hexafluoroarsenate), Li(CF 3 SO 2 ) 2 N, LiFSI (lithium bisfluorosulfonimide), LiTFSI (lithium bistrifluoromethanesulfonimide), LiTFS (lithium trifluoromethanesulfonate), LiDFOB (lithium difluorooxalate), LiBOB (two oxalate borate) Lithium), LiPO 2 F 2 (lithium difluorophosphate), LiDFOP (lithium difluorodioxalate phosphate) and LiTFOP (lithium tetrafluorooxalate phosphate) one
- the electrolyte salt one or more of LiPF 6 , LiFSI , LiPO 2 F 2 , LiDFOB, and LiDFOP can be used.
- LiPF 6 may be used as the electrolyte salt.
- the mass percentage of the total mass of the electrolyte salt in the total mass of the electrolyte is ⁇ 20%. More preferably, the mass percentage of the total mass of the electrolyte salt in the total mass of the electrolyte is 10%-15%.
- the secondary battery further includes a negative pole piece.
- the negative electrode piece includes a negative electrode active material, and the negative electrode active material may be selected from substances known in the art that can be used as a negative electrode active material.
- the negative electrode active material includes artificial graphite, and when the negative electrode active material includes artificial graphite, the improvement effect of the above-mentioned electrolyte is more obvious.
- the performance of the battery can be further improved.
- the surface of the artificial graphite does not have an amorphous carbon coating layer; when the surface of the artificial graphite does not have an amorphous carbon coating layer, it can further reduce its and electrolyte in the battery cycle process.
- the side reaction reduces the increase in the thickness of the SEI film, thereby reducing the cycle expansion of the battery.
- the artificial graphite of the I D / I G is preferably less than or equal to 0.25.
- artificial graphite I D / I G may be 0.23,0.2,0.18,0.16,0.15,0.12,0.1 or 0.08.
- the I D /I G of the artificial graphite is 0.1 to 0.2.
- artificial graphite I D / I G adapted to improve the stability of the surface, which reduce the side reactions of the electrolyte surface, thereby further reducing the battery volume expansion during cycling.
- the I D / I G peak D represents the peak intensity artificial graphite (the I D) to peak intensity of G peak (the I G) ratio.
- Peak D and Peak G are Raman characteristic peaks of graphite materials.
- the D peak and G peak of artificial graphite can be measured by laser Raman spectroscopy, such as the Advantage 785TM Raman spectrometer.
- the artificial graphite also satisfies the number average particle size D n 10 of 1 ⁇ m to 3 ⁇ m, preferably 1 ⁇ m to 2 ⁇ m.
- the gram capacity of the artificial graphite can be further increased; and in the negative pole piece prepared by the artificial graphite, the artificial graphite and the additives such as the binder can be uniformly dispersed.
- the overall adhesion of the pole piece is relatively high, which can further reduce the cycle expansion of the battery.
- the artificial graphite also satisfies the volume average particle size D v 50 of 15 ⁇ m to 20 ⁇ m, preferably 15 ⁇ m to 18 ⁇ m.
- the volume average particle size D v 10 of the artificial graphite is greater than or equal to 6 ⁇ m, preferably 6.5 ⁇ m to 10.5 ⁇ m.
- the D v 10 of artificial graphite may be 6 ⁇ m or more, 6.5 ⁇ m or more, 7 ⁇ m or more, or 7.5 ⁇ m or more.
- the artificial graphite with D v 50 and/or D v 10 in the above range has higher active ion and electron transport performance, reduces side reactions of the electrolyte in the negative electrode; at the same time, it is also beneficial to improve the powder compaction density of its own.
- the artificial graphite also satisfies a particle size distribution (D v 90-D v 10)/D v 50 of 1.1 to 1.8, preferably 1.2 to 1.5.
- a particle size distribution D v 90-D v 10/D v 50 of 1.1 to 1.8, preferably 1.2 to 1.5.
- the proper particle size distribution is also conducive to the proper specific surface area (SSA) of artificial graphite, which enables it to have both higher electrochemical reaction activity and higher surface stability, thereby further improving the cycle performance.
- SSA specific surface area
- the D n 10, D v 10, D v 50, and D v 90 of the artificial graphite can be measured with a laser particle size analyzer (such as Malvern Master Size 3000) with reference to the standard GB/T19077.1-2016.
- a laser particle size analyzer such as Malvern Master Size 3000
- D n 10, D v 10, D v 50, and D v 90 are as follows:
- D n 10 the particle size corresponding to when the cumulative number distribution percentage of the material reaches 10%
- D v 10 The particle size when the cumulative volume distribution percentage of the material reaches 10%
- D v 50 the particle size when the cumulative volume distribution percentage of the material reaches 50%
- D v 90 The particle size when the cumulative volume distribution percentage of the material reaches 90%.
- the specific surface area of artificial graphite of 1.0m 2 /g ⁇ 1.5m 2 / g.
- artificial graphite has an appropriate specific surface area and can have high electrochemical reaction activity in secondary batteries, meeting the kinetic requirements of secondary batteries, and reducing side reactions of electrolyte on the surface of the material. Reduce gas production, which can reduce the volume expansion of the battery during the cycle.
- Artificial graphite with appropriate specific surface area also has a strong bonding force with the binder, which can improve the cohesion and adhesion of the pole piece, thereby further reducing the cycle expansion of the battery.
- the specific surface area of artificial graphite can be tested using methods known in the art. For example, you can refer to GB/T19587-2017, use the nitrogen adsorption specific surface area analysis test method to test, and use the BET (Brunauer Emmett Teller) method to calculate, wherein the nitrogen adsorption specific surface area analysis test can pass the Tri-Star 3020 type ratio test of Micromeritics, USA Surface area pore size analysis tester is performed.
- BET Brunauer Emmett Teller
- the graphitization degree G of the artificial graphite may be 90%-95%, preferably 92%-94%.
- a proper graphitization degree G can make the artificial graphite have a higher gram capacity, and at the same time make the bulk structure of the artificial graphite more stable.
- the degree of graphitization of artificial graphite can be tested using methods known in the art.
- the powder compaction density of the artificial graphite under a pressure of 2000 kg is 1.65 g/cm 3 to 1.85 g/cm 3 , preferably 1.68 g/cm 3 to 1.83 g/cm 3 .
- the artificial graphite has a higher powder compaction density under a pressure of 2000kg, and the negative pole piece using the artificial graphite can have a higher compaction density, so that the battery has a higher energy density.
- the powder compaction density of the artificial graphite can be tested by methods known in the art. For example, refer to GB/T 24533-2009 and use an electronic pressure testing machine (such as UTM7305) for testing.
- an electronic pressure testing machine such as UTM7305
- the compacted density of the negative electrode membrane is 1.55 g/cm 3 to 1.75 g/cm 3 ; more preferably, the compacted density of the negative electrode membrane is 1.6 g/cm 3 to 1.7 g/cm 3 .
- the negative electrode membrane can have a high-pressure compaction density and at the same time have a porosity suitable for full infiltration of the electrolyte. Therefore, the capacity of the battery can be used more effectively, and the battery can obtain better dynamic performance.
- the orientation OI value of the negative electrode piece is 8-15, more preferably 8-12.
- the OI value of the pole piece can have a higher degree of isotropy, so that the artificial graphite is dispersed in all directions during the expansion of the lithium intercalation in the pole piece, which can further reduce the pole piece and the The cyclic expansion of the battery.
- X-ray diffraction analysis refers to the standard JISK 0131-1996, using an X-ray diffractometer (such as Bruker D8 Discover X-ray diffractometer) for testing, using CuK ⁇ rays as the radiation source, and the ray wavelength
- the scanning 2 ⁇ angle range is 20° ⁇ 80°, and the scanning rate is 4°/min.
- the areal density of the negative electrode film of the present application is 7.5 mg/cm 2 -14.0 mg/cm 2 ; preferably 9.5 mg/cm 2 -12.0 mg/cm 2 .
- the areal density of the negative electrode film can represent the weight of the film per unit area on the electrode after cold pressing. The measurement may be performed according to the method described in the embodiment, or may be performed according to other well-known methods in the art. In some exemplary embodiments, the mass of the negative electrode film in a specific area is weighed by a standard balance, and then the mass of the negative electrode film per unit area, that is, the areal density, is calculated.
- the parameters of the negative electrode membrane (for example, the compaction density of the negative electrode membrane and the areal density) given in this application all refer to the parameter range of the single-sided membrane.
- the membrane parameters on any one of the surfaces meet the requirements of the present application, which is considered to fall within the protection scope of the present application.
- the ranges of compaction density, areal density, etc. in the present invention all refer to the parameter ranges after cold compaction and compaction for battery assembly.
- the above-mentioned artificial graphite of the present application can be prepared by the following method:
- step (3) Granulate the product obtained in step (2), wherein the amount of binder added in the granulation process does not exceed 5% of the total weight of the raw coke raw material;
- step (3) Perform graphitization treatment on the product obtained in step (3) at a temperature of 2800° C. to 3200° C. to obtain the artificial graphite.
- the raw coke raw material can be selected from one or more of raw petroleum coke and raw pitch coke; more preferably, it includes raw petroleum coke.
- the green coke is non-needle coke.
- the volatile content of the raw petroleum coke is 7%-10%; the volatile content of the raw coke raw material is appropriate, so that the artificial graphite has a higher structural strength.
- the sulfur content of the raw petroleum coke is ⁇ 2%.
- the raw coke raw material has a lower sulfur content, which can improve the surface stability of artificial graphite.
- step (2) preferably, after the shaping in step (2), the step of removing fine powder is further included, and D n 10 can be adjusted to the range given in this application.
- granulating the product obtained in step (2) without adding a binder can further increase the gram capacity and structural strength of the artificial graphite.
- the product obtained in step (3) is graphitized at a temperature of 2900°C to 3100°C.
- the secondary battery of the present application further includes a positive pole piece, the positive pole piece includes a positive electrode active material, and the positive electrode active material can be selected from substances known in the art that can be used as a positive electrode active material.
- the positive electrode active material includes one or more of lithium transition metal oxides and modified compounds thereof, and the modified compounds may be doping modification and/or coating modification of lithium transition metal oxides.
- the lithium transition metal oxide includes one or more of lithium nickel manganese oxide and lithium nickel cobalt aluminum oxide.
- the positive pole piece and the negative pole piece may also optionally include a binder.
- a binder This application does not specifically limit the types of binders, and those skilled in the art can make selections according to actual needs.
- the binder used for the positive pole piece may include one or more of polyvinylidene fluoride (PVDF) and polytetrafluoroethylene (PTFE).
- the positive pole piece and the negative pole piece may also optionally include a conductive agent.
- a conductive agent used for the positive pole piece may include one or more of artificial graphite, superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, artificial graphene, and carbon nanofibers.
- the conductive agent used for the positive pole piece may include one or more of artificial graphite, superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, artificial graphene, and carbon nanofibers. kind.
- the secondary battery of the present application also includes a separator film.
- the isolation film is arranged between the positive pole piece and the negative pole piece to play a role of isolation.
- the type of isolation membrane in this application, and any well-known porous structure isolation membrane with good chemical stability and mechanical stability can be selected.
- the material of the isolation membrane can be selected from one or more of glass fiber, non-woven fabric, polyethylene, polypropylene, and polyvinylidene fluoride.
- the isolation film can be a single-layer film or a multilayer composite film. When the isolation film is a multilayer composite film, the materials of each layer can be the same or different.
- the secondary battery of the present application can be prepared according to conventional methods in the art, for example, the negative electrode active material and optional conductive agent and binder are dispersed in a solvent (such as water) to form a uniform negative electrode slurry, and the negative electrode slurry Coated on the negative electrode current collector, after drying, cold pressing and other processes, the negative electrode piece is obtained; the positive electrode active material and optional conductive agent and binder are dispersed in a solvent (for example, N-methylpyrrolidone, abbreviated as In NMP), a uniform positive electrode slurry is formed, and the positive electrode slurry is coated on the positive electrode current collector.
- a solvent such as water
- NMP N-methylpyrrolidone
- the positive electrode piece After drying, cold pressing, etc., the positive electrode piece is obtained; the positive electrode piece, separator, and negative electrode piece are pressed Sequentially winding or lamination, so that the separator is placed between the positive pole piece and the negative pole piece for isolation, to obtain the electric core, place the electric core in the outer packaging, and inject the electrolyte of the present application to obtain the Secondary battery.
- the secondary battery may include an outer package and a battery cell and electrolyte packaged in the outer package.
- the number of battery cells in the secondary battery can be one or several, which can be adjusted according to requirements.
- the outer packaging of the secondary battery may be a soft bag (for example, a bag type, and the material may be plastic, such as polypropylene PP, polybutylene terephthalate PBT, polybutylene succinate Ester PBS, etc.), or a hard shell (for example, aluminum shell, etc.).
- a soft bag for example, a bag type
- the material may be plastic, such as polypropylene PP, polybutylene terephthalate PBT, polybutylene succinate Ester PBS, etc.
- a hard shell for example, aluminum shell, etc.
- Fig. 1 shows a secondary battery 5 with a square structure as an example.
- the secondary battery can be assembled into a battery module, and the number of secondary batteries contained in the battery module can be multiple, and the specific number can be adjusted according to the application and capacity of the battery module.
- Fig. 2 is a battery module 4 as an example.
- a plurality of secondary batteries 5 may be arranged in sequence along the length direction of the battery module 4. Of course, it can also be arranged in any other manner. Furthermore, the plurality of secondary batteries 5 can be fixed by fasteners.
- the battery module 4 may further include a housing having an accommodating space, and a plurality of secondary batteries 5 are accommodated in the accommodating space.
- the above-mentioned battery modules can also be assembled into a battery pack, and the number of battery modules contained in the battery pack can be adjusted according to the application and capacity of the battery pack.
- Figures 3 and 4 show the battery pack 1 as an example. 3 and 4, the battery pack 1 may include a battery box and a plurality of battery modules 4 provided in the battery box.
- the battery box includes an upper box body 2 and a lower box body 3.
- the upper box body 2 can be covered on the lower box body 3 and forms a closed space for accommodating the battery module 4.
- a plurality of battery modules 4 can be arranged in the battery box in any manner.
- the present application also provides an electrolyte, the electrolyte includes an organic solvent, the organic solvent includes a cyclic carbonate and a chain carbonate; the mass ratio of the cyclic carbonate to the chain carbonate is 25:75 ⁇ 32:68; the chain carbonate includes dimethyl carbonate; the mass percentage of the dimethyl carbonate in the chain carbonate is greater than or equal to 9wt% and less than 50wt%;
- the mass percentage of the carboxylic acid ester in the organic solvent is less than 5 wt%.
- the electrolyte can be prepared according to conventional methods in the art.
- the organic solvent and the electrolyte salt and optional additives can be mixed uniformly to obtain the electrolyte.
- the order of addition of each material is not particularly limited.
- the electrolyte salt and optional additives are added to the organic solvent and mixed uniformly to obtain the electrolyte.
- the electrolyte salt can be added to the organic solvent first, and then the optional additives can be added to the organic solvent separately or at the same time.
- a device in a second aspect of the present application, includes the secondary battery of the first aspect of the present application, and the secondary battery provides power to the device.
- the device can be, but is not limited to, mobile devices (such as mobile phones, laptop computers, etc.), electric vehicles (such as pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf Vehicles, electric trucks, etc.), electric trains, ships and satellites, energy storage systems, etc.
- the device can select a secondary battery, a battery module, or a battery pack according to its usage requirements.
- Figure 5 is a device as an example.
- the device is a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle.
- a battery pack or a battery module can be used.
- the device may be a mobile phone, a tablet computer, a notebook computer, and the like.
- the device is generally required to be thin and light, and a secondary battery can be used as a power source.
- Artificial graphite A has the following characteristics: the gram capacity is about 354mAh/g, the volume average particle size D v 50 is about 12.8 ⁇ m, the volume average particle size D v 10 is about 6.9 ⁇ m, and the particle size distribution (D v 90-D v 10 ) / D v 50 approximately 1.26, a number average particle size D n 10 is about 4.3 ⁇ m, I D / I G of about 0.32, SSA about 0.95m 2 / g.
- Artificial graphite B has the following characteristics: the gram capacity is about 354mAh/g, the volume average particle size D v 50 is about 16.2 ⁇ m, the volume average particle size D v 10 is about 7.2 ⁇ m, and the particle size distribution (D v 90-D v 10 ) / D v 50 approximately 1.37, a number average particle size D n 10 is about 1.5 ⁇ m, I D / I G of about 0.18, SSA about 1.25m 2 / g.
- the positive electrode active material LiNi 0.5 Co 0.2 Mn 0.3 O 2 , the conductive agent (Super P), and the binder polyvinylidene fluoride (PVDF) are fully in N-methylpyrrolidone (NMP) at a mass ratio of 94:3:3 Stir and mix evenly to prepare positive electrode slurry. Then, the positive electrode slurry is uniformly coated on the current collector Al foil, dried and cold pressed to obtain a positive electrode pole piece.
- NMP N-methylpyrrolidone
- the negative active material artificial graphite A conductive agent (Super P), binder styrene-butadiene rubber (SBR), thickener sodium carboxymethyl cellulose (CMC-Na) in accordance with the mass ratio of 95:2:2:1 Stir and mix thoroughly in the deionized water solvent system to form a negative electrode slurry. Then, the negative electrode slurry is coated on the current collector Cu foil, dried and cold pressed to obtain a negative electrode piece.
- the compacted density of the negative electrode piece is 1.65 g/cm 3
- the areal density is 10.7 mg/cm 2
- the orientation OI value of the negative electrode piece is 22.
- the PE porous polymer film is used as the isolation membrane.
- Example 9-16 the same preparation steps as in Examples 1-8 were used, except that the artificial graphite B was replaced with artificial graphite A during the preparation of the negative pole piece.
- the specific experimental parameters and results are shown in Table 2. It is worth noting that in the preparation process of the negative pole piece, when the artificial graphite B is used, the orientation OI value of the obtained negative pole piece is 10.5.
- Capacity retention rate at the Nth cycle (discharge capacity at the Nth cycle/discharge capacity at the first cycle) ⁇ 100%.
- the cycle capacity retention rate drops to 80%, the number of cycles of the battery is recorded.
- the battery is kept at -20°C for 120 minutes to keep the temperature inside and outside the battery constant at -20°C. Then discharge with 400W power for 10 seconds, and measure the discharge end voltage V.
- the current power is the power value of the battery, expressed in W.
- the battery will be readjusted to a 20% SOC capacity at room temperature and discharged with a higher power at a low temperature. If the terminal voltage V is less than 2.1 ⁇ 0.05V, the battery will be readjusted to 20% SOC capacity at normal temperature, and discharged with lower power at low temperature.
- Comparing Examples 1-2, Examples 4-6 with Comparative Example 1 it can be seen that adding DMC to the electrolyte is beneficial to alleviate the deterioration of the charging ability caused by the increase in expansion force, thereby suppressing to a certain extent The expansion force is further increased, thereby improving the 45°C cycle performance.
- Comparative Examples 2-3 it can be seen from Comparative Examples 2-3 that as the content of DMC further increases, the low-temperature viscosity of the electrolyte increases, resulting in a significant decrease in conductivity and low-temperature power at low temperatures; in addition, the decomposition of DMC at the positive electrode interface increases, This results in serious battery flatulence, which affects the charging ability on the battery interface, and severely deteriorates the 45°C cycle performance.
- the mass percentage of DMC in the chain carbonate is controlled to at least 9 wt% and less than 50 wt%, good low-temperature conductivity and 45°C cycle performance are obtained.
- the amount of DMC in the chain carbonate is further controlled to be 15 wt% to 45 wt%, more preferably 25 wt% to 43 wt%, and at the same time, better low temperature power and 45°C cycle performance are obtained.
- Example 4 Comparing Example 4 with Example 7, and Comparative Example 8, it can be seen that adding a small amount of PC to the cyclic carbonate can increase the low-temperature conductivity, thereby improving the low-temperature power, but the PC content is further increased, and the PC will cause graphite to peel off. As a result, the swelling force of the battery increases and the cycle performance deteriorates.
- the inventor also surprisingly found that the use of artificial graphite B has fewer defects on the graphite surface, and the SEI film of the electrolyte on the graphite surface is broken and repaired. At the same time With the use of the electrolyte composition amount discussed above, the 45°C cycle performance and low-temperature power performance of the battery are further improved.
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Abstract
Description
Claims (16)
- 一种二次电池,包括电解液,其特征在于,所述电解液包括有机溶剂,所述有机溶剂包括环状碳酸酯和链状碳酸酯;所述环状碳酸酯与所述链状碳酸酯的质量比为25:75~32:68;所述链状碳酸酯包括碳酸二甲酯;所述碳酸二甲酯在所述链状碳酸酯中的质量百分数大于或等于9wt%且小于50wt%;其中,基于所述有机溶剂的总质量,所述有机溶剂中羧酸酯的质量百分数小于5wt%。
- 根据权利要求1所述的二次电池,其特征在于,所述碳酸二甲酯在所述链状碳酸酯中的质量百分数为15wt%~45wt%,优选为25wt%~43wt%。
- 根据权利要求1或2所述的二次电池,其特征在于,所述有机溶剂中羧酸酯的质量百分数小于3wt%,优选地,所述有机溶剂中羧酸酯的质量百分数为0wt%。
- 根据权利要求1-3中任一项所述的二次电池,其特征在于,所述环状碳酸酯包括碳酸亚乙酯和碳酸亚丙酯中的一种或几种。
- 根据权利要求1-4中任一项所述的二次电池,其特征在于,所述碳酸亚乙酯在所述环状碳酸酯中的质量百分数大于90%,优选为92%~100%。
- 根据权利要求1-5中任一项所述的二次电池,其特征在于,所述链状碳酸酯还包括碳酸二乙酯和碳酸甲乙酯中的一种或几种。
- 根据权利要求1-6中任一项所述的二次电池,其特征在于,所述羧酸酯包括乙酸甲酯、乙酸乙酯、乙酸丙酯、丙酸甲酯、丙酸乙酯和丙酸丙酯中的一种或几种;优选地,所述羧酸酯包括乙酸乙酯和丙酸乙酯中的一种或几种。
- 根据权利要求1-7中任一项所述的二次电池,其特征在于,所述电解液还包括添加剂,所述添加剂包括氟代碳酸乙烯酯、碳酸亚乙烯酯、硫酸亚乙酯、 三(三甲基硅烷)磷酸酯、二氟草酸硼酸锂、和双氟磺酰亚胺锂的一种或几种。
- 根据权利要求8所述的二次电池,其特征在于,所述添加剂的总量不超过所述电解液总质量的10wt%。
- 根据权利要求1-9中任一项所述的二次电池,其特征在于,所述电解液在-20℃下的电导率≥2.5mS/cm,优选为2.6mS/cm~3.5mS/cm。
- 根据权利要求1-10所述的二次电池,所述二次电池还包括负极极片,所述负极极片包括负极活性材料,其特征在于,所述负极活性材料包括人造石墨,所述人造石墨满足下述(1)–(8)中的一种或几种:(1)所述人造石墨的克容量为350mAh/g~358mAh/g,;(2)所述人造石墨的D峰强度I D与G峰强度I G之间满足:I D/I G≤0.25,优选地,0.1≤I D/I G≤0.2(3)所述人造石墨负极材料的数量平均粒径D n10为1μm~3μm,优选为1μm~2μm;(4)所述人造石墨负极材料的体积平均粒径D v10≥6μm,优选为6.5μm~10.5μm;(5)所述人造石墨负极材料的体积平均粒径D v50为15μm~20μm,优选为15μm~18μm;(6)所述人造石墨负极材料的粒径分布(D v90﹣D v10)/D v50为1.1~1.8,优选为1.2~1.5;(7)所述人造石墨的比表面积为1.0m 2/g~1.5m 2/g;(8)所述人造石墨的石墨化度G为90%~95%,优选为92%~94%。
- 根据权利要求11所述的二次电池,其特征在于,所述负极极片的压实密度为1.55g/cm 3~1.75g/cm 3,优选为1.6g/cm 3~1.7g/cm 3。
- 根据权利要求12所述的二次电池,其特征在于,所述负极极片的取向OI值为8~15,优选为8~12;其中,所述负极极片的取向OI值为负极极片的X射线衍射图谱中负极活性材料的004衍射峰的峰面积与110衍射峰的峰面积的比值。
- 根据权利要求1-13中任一项所述的二次电池,其特征在于,所述二次电池还包括正极极片,所述正极极片包括正极活性材料,所述正极活性材料包括锂过渡金属氧化物及其改性化合物中的一种或几种;优选地,所述正极活性材料包括锂镍钴锰氧化物和锂镍钴铝氧化物中的一种或几种。
- 一种电解液,其特征在于,所述电解液包括有机溶剂,所述有机溶剂包括环状碳酸酯和链状碳酸酯;所述环状碳酸酯与所述链状碳酸酯的质量比为25:75~32:68;所述链状碳酸酯包括碳酸二甲酯;所述碳酸二甲酯在所述链状碳酸酯中的质量百分数大于或等于9wt%且小于50wt%;其中,基于所述有机溶剂的总质量,所述有机溶剂中羧酸酯的质量百分数小于5wt%。
- 一种装置,其特征在于,所述装置包括根据权利要求1-14任一项所述的二次电池。
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ES19954946T ES2934127T3 (es) | 2019-12-03 | 2019-12-03 | Batería secundaria, electrolito y dispositivo que contiene dicha batería secundaria |
EP19954946.0A EP3913721B1 (en) | 2019-12-03 | 2019-12-03 | Secondary battery, electrolyte, and device containing said secondary battery |
PL19954946.0T PL3913721T3 (pl) | 2019-12-03 | 2019-12-03 | Akumulator, elektrolit i urządzenie zawierające wspomniany akumulator |
PCT/CN2019/122741 WO2021108995A1 (zh) | 2019-12-03 | 2019-12-03 | 二次电池、电解液以及包括该二次电池的装置 |
KR1020227007000A KR20220038494A (ko) | 2019-12-03 | 2019-12-03 | 이차 전지, 전해액 및 이차 전지를 포함하는 장치 |
JP2022512712A JP7357769B2 (ja) | 2019-12-03 | 2019-12-03 | 二次電池、電解液及び二次電池を備える装置 |
CN201980066194.6A CN113207318A (zh) | 2019-12-03 | 2019-12-03 | 二次电池、电解液以及包括该二次电池的装置 |
US17/402,672 US11735775B2 (en) | 2019-12-03 | 2021-08-16 | Secondary battery, electrolyte, and apparatus comprising the secondary battery |
US18/208,898 US20230327209A1 (en) | 2019-12-03 | 2023-06-13 | Secondary battery, electrolyte, and apparatus comprising the secondary battery |
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Also Published As
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ES2934127T3 (es) | 2023-02-17 |
KR20220038494A (ko) | 2022-03-28 |
PL3913721T3 (pl) | 2023-02-27 |
EP3913721A4 (en) | 2022-03-30 |
EP3913721B1 (en) | 2022-11-23 |
CN113207318A (zh) | 2021-08-03 |
JP7357769B2 (ja) | 2023-10-06 |
EP3913721A1 (en) | 2021-11-24 |
US20230327209A1 (en) | 2023-10-12 |
US11735775B2 (en) | 2023-08-22 |
US20220123366A1 (en) | 2022-04-21 |
JP2022545896A (ja) | 2022-11-01 |
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