CN113809401A - Non-aqueous electrolyte of lithium ion battery and application thereof - Google Patents
Non-aqueous electrolyte of lithium ion battery and application thereof Download PDFInfo
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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
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- 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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Abstract
The invention provides a lithium ion battery non-aqueous electrolyte and application thereof. The non-aqueous electrolyte of the lithium ion battery comprises an electrolyte, a non-aqueous solvent and an additive, wherein the additive comprises a first compound and a cyclic ester additive. The first compound contains a plurality of substituent groups rich in electron alkenyl, and the network dimension of the polymer formed by the first compound additive plays an important role in the conduction of lithium ions. Due to the multiolefin structure, the network structure formed by the polymer has different sizes, so that the transmission of lithium ions can be influenced. The invention can inhibit the reaction between the electrolyte and the anode in a high-temperature state by utilizing the synergistic effect of the first compound and the cyclic ester additive, thereby improving the high-temperature storage performance of the lithium ion battery.
Description
Technical Field
The invention belongs to the field of batteries, and particularly relates to a non-aqueous electrolyte of a lithium ion battery and application thereof.
Background
Compared with the traditional lead-acid battery, the lithium ion battery is taken as a rechargeable battery, has the advantages of high energy density, small self-discharge, long cycle life and the like, and is widely applied to the fields of electric automobiles, smart power grids, miniaturized electronic equipment and the like. At present, the use safety problem of the lithium ion battery is still an important factor for restricting the application development of the lithium ion battery.
The electrolyte of the lithium ion battery mostly adopts an organic solvent system, and when the charging current is large, the temperature of the battery system rises, so that potential safety hazards such as expansion and gas generation of the battery system are caused. In addition, in order to further improve the energy density of the lithium ion battery, researchers mostly adopt ternary cathode materials with high specific capacity and high reaction potential, and also put higher requirements on the electrolyte. In summary, improving the stability of the electrolyte is an effective method for improving the safety of the lithium ion battery, for example, adding some film-forming additives, conductive additives and multifunctional additives to the electrolyte can further improve the safety performance of the battery.
The Electrolyte additive is used in an amount of only a small part (usually less than 5 wt%) of the Electrolyte in the lithium ion battery, but a proper amount of the additive can form a Solid Electrolyte Interface (SEI) film on the surface of the negative electrode and/or the positive electrode. The SEI film can form a layer of protective film on the surfaces of the anode and cathode materials, so that the side reaction between the SEI film and the electrolyte is avoided. Cyclic carbon-and sulfur-containing compounds among these are currently the more widely used electrolyte additives, such as vinylene carbonate and fluoroethylene carbonate, which are better able to passivate graphite negative and/or positive electrodes. However, the SEI film has problems of unevenness, being broken down during cycling, and instability.
In view of the above, it is desirable in the art to develop an electrolyte for a lithium ion battery that is capable of not only forming a stable and thin SEI film, but also improving the electrochemical performance of the battery at high temperatures.
Disclosure of Invention
In view of the defects of the prior art, the invention aims to provide a lithium ion battery nonaqueous electrolyte and application thereof. The electrolyte provided by the invention can inhibit the reaction between the electrolyte and the anode at a high temperature, and is used in cooperation with the cyclic ester additive to prepare a stable SEI film, so that the high-temperature cycle performance of the lithium ion battery is improved.
In order to achieve the purpose, the invention adopts the following technical scheme:
in a first aspect, the present invention provides a nonaqueous electrolyte for a lithium ion battery, including an electrolyte, a nonaqueous solvent, and an additive, where the additive includes a first compound having a structure represented by formula 1 and a cyclic ester additive:
wherein R is1、R2、R3And R4Each independently selected from-CH-X, C2 to C6 straight chain alkyl groups or C2 to C6 branched chain alkyl groups.
The X is selected from linear alkyl of-H, C2 to C6 or branched alkyl of C2 to C6.
The R is1、R2、R3And R4At least one of which is selected from-CH ═ CH-X.
In the present invention, the first compound additive contains a plurality of electron-rich alkenyl substituent groups, and the network dimension of the polymer formed from the first compound additive plays an important role in the conduction of lithium ions. Due to the existence of the multiolefin structure, network structures formed by the polymers have different sizes, and therefore the size of an ion channel formed by the network structures can influence the transmission of lithium ions. In the present invention, the number of nodes is used to define the lithium ion transport channel formed by the polymerization of the first compound, for example: when the first compound contains only one vinyl group and the oxidative polymerization reaction is carried out, the number of nodes of the compound is 1 for one structural repeating unit; the first compound contains two vinyl groups, and for a structural repeat unit, the number of nodes in the compound is 2, and so on. In the present invention, when the number of nodes is too small, a polymer structure constituting the SEI film cannot form a dense protective film; when the number of nodes is too large, efficient transmission of lithium ions is hindered. Therefore, the invention adjusts the content of the olefin additive within a proper range, so that the number of nodes is between 2 and 2.5, and the high-temperature storage performance of the lithium ion battery is improved.
Preferably, the first compound includes a second compound having a structure shown in formula 2, a third compound having a structure shown in formula 3, a fourth compound having a structure shown in formula 4, and/or a fifth compound having a structure shown in formula 5:
preferably, the mass percentage of the first compound in the lithium ion battery nonaqueous electrolyte is 0.02% to 5%, for example, 0.02%, 0.1%, 0.5%, 1%, 2% or 5%, but not limited to the recited values, and other values not recited in the numerical range are also applicable.
Preferably, the content of the cyclic ester additive in the non-aqueous electrolyte of the lithium ion battery is 0.05% to 20% by mass, for example, 0.05%, 0.5%, 1%, 5%, 10% or 20% by mass, but not limited to the recited values, and other values not recited in the numerical range are also applicable.
Preferably, the cyclic ester additive in the non-aqueous electrolyte solution of the lithium ion battery includes any one or a combination of at least two of a cyclic carbonate additive, a cyclic sultone additive or a cyclic sulfate additive, and may be, for example, a cyclic carbonate additive, a cyclic sultone additive and a cyclic sulfate additive, a cyclic carbonate additive and a cyclic sultone additive, a cyclic carbonate additive and a cyclic sulfate additive or a cyclic sultone additive and a cyclic sulfate, but is not limited to the listed species, and other species not listed within the scope of the cyclic ester additive are also applicable.
Preferably, the cyclic carbonate additive includes any one or a combination of at least two of vinylene carbonate, fluoroethylene carbonate or ethylene carbonate, such as vinylene carbonate, fluoroethylene carbonate and ethylene carbonate or ethylene carbonate, but not limited to the listed species, and other species not listed within the scope of the cyclic carbonate additive are also applicable.
Preferably, the cyclic sultone additive comprises any one or combination of two of 1, 3-propane sultone and 1, 3-propylene sultone, and can be 1, 3-propane sultone and 1, 3-propylene sultone, 1, 3-propane sultone or 1, 3-propylene sultone.
Preferably, the cyclic sulfate-based additive includes any one of or a combination of at least two of vinyl sulfate or propylene sulfate, and may be, for example, vinyl sulfate and propylene sulfate, vinyl sulfate or propylene sulfate.
Preferably, the electrolyte is a lithium salt.
Preferably, the lithium salt comprises lithium hexafluorophosphate.
Preferably, the concentration of lithium hexafluorophosphate in the non-aqueous electrolyte of the lithium ion battery is 0.5mol/L to 2mol/L, for example, 0.5mol/L, 1mol/L, 1.5mol/L or 2mol/L, but not limited to the enumerated values, and other unrecited values in the numerical range are also applicable.
Preferably, the additive further comprises a lithium salt additive.
Preferably, the lithium salt additive includes any one or a combination of at least two of lithium bis (oxalate) difluorophosphate, lithium difluoro (oxalate) borate, lithium bis (fluorosulfonyl) imide or lithium bis (trifluoromethyl) sulfonyl imide, such as lithium bis (oxalate) difluorophosphate and lithium difluorophosphate, lithium difluoro (oxalate) borate or lithium bis (trifluoromethanesulfonyl) imide, but not limited to the enumerated species, and other species not enumerated within the scope of the lithium salt additive are equally applicable.
Preferably, the lithium salt additive is contained in the lithium ion battery nonaqueous electrolyte in an amount of 0.05% to 20% by mass, for example, 0.05%, 0.5%, 1%, 5%, 10% or 20% by mass, but not limited to the recited values, and other values not recited in the numerical range are also applicable.
Preferably, the non-aqueous solvent includes any one or a combination of at least two of ethylene carbonate, dimethyl carbonate, ethyl methyl carbonate, propylene carbonate or diethyl carbonate, such as ethylene carbonate and dimethyl carbonate, ethyl methyl carbonate and propylene carbonate or diethyl carbonate, but is not limited to the listed species, and other species not listed in the non-aqueous solvent are also applicable.
Preferably, the content of the nonaqueous solvent in the nonaqueous electrolyte solution of the lithium ion battery is 60% to 85% by mass, for example, 60%, 65%, 70%, 75%, 80% or 85%, but not limited to the recited values, and other values not recited in the numerical range are also applicable.
In a second aspect, the invention provides a lithium ion battery, which comprises the lithium ion battery nonaqueous electrolyte solution of the first aspect.
Preferably, the lithium ion battery further comprises a positive electrode current collector, a positive electrode active material coated on the positive electrode current collector, a negative electrode active material coated on the negative electrode current collector, and a separator.
Preferably, the positive active material includes any one or a combination of at least two of lithium cobalt oxide, lithium nickel oxide, lithium manganese oxide, lithium nickel cobalt manganese oxide, or lithium nickel cobalt aluminum oxide, and may be, for example, lithium cobalt oxide and lithium nickel oxide, lithium manganese oxide and lithium nickel manganese oxide, lithium nickel cobalt manganese oxide, or lithium nickel cobalt aluminum oxide, but is not limited to the listed species, and other species not listed in the scope of the positive active material are also applicable.
Preferably, the negative electrode active material includes any one or a combination of at least two of soft carbon, hard carbon, artificial graphite, natural graphite, silicon oxide, silicon carbon compound or lithium titanate, for example, the soft carbon and hard carbon, artificial graphite and natural graphite, silicon oxide, silicon carbon compound or lithium titanate may be used, but not limited to the listed species, and other species not listed in the scope of the negative electrode active material may be equally applicable.
Compared with the prior art, the invention has the following beneficial effects:
the invention provides a lithium ion battery non-aqueous electrolyte, which adopts a first compound with a multi-alkenyl structure, not only enhances the electron-donating effect, but also forms a lithium ion transmission channel in an obtained polymer network, adjusts the size of the channel by using the number of nodes, promotes the transmission of lithium ions, and simultaneously is used cooperatively with a cyclic ester additive to prepare a stable SEI film so as to optimize the high-temperature cycle performance of the battery.
Detailed Description
The technical solution of the present invention is further explained by the following embodiments. It should be understood by those skilled in the art that the examples are only for the understanding of the present invention and should not be construed as the specific limitations of the present invention.
In the prior art, the energy density of the lithium ion battery is improved by adopting a high-content nickel element anode material and improving the charge cut-off voltage. However, the solutions disclosed in the prior art all have adverse effects on the electrolyte, such as side reactions, gas generation and increased interfacial resistance.
In order to solve the technical problems, the invention provides a lithium ion battery nonaqueous electrolyte and application thereof.
Embodiments of the invention provide, in part, a lithium ion battery nonaqueous electrolyte comprising an electrolyte, a nonaqueous solvent, and an additive comprising a first compound having a structure represented by formula 1 and a cyclic ester additive:
wherein R is1、R2、R3And R4Each independently selected from-CH-X, C2 to C6 straight chain alkyl or C2 to C6 branched chain alkyl;
the X is selected from linear alkyl of-H, C2 to C6 or branched alkyl of C2 to C6;
the R is1、R2、R3And R4At least one of which is selected from-CH ═ CH-X.
The invention provides a lithium ion battery non-aqueous electrolyte, which adopts a first compound with a multi-alkenyl structure, an obtained polymer network forms a lithium ion transmission channel, the size of the channel is adjusted by using the number of nodes, the transmission of lithium ions is promoted, and meanwhile, the non-aqueous electrolyte is used in cooperation with a cyclic ester additive to prepare a stable SEI film, so that the high-temperature cycle performance of the battery is optimized.
In some embodiments, the first compound includes a second compound having a structure represented by formula 2, a third compound having a structure represented by formula 3, a fourth compound having a structure represented by formula 4, and/or a fifth compound having a structure represented by formula 5:
in some embodiments, the mass percentage of the first compound in the lithium ion battery nonaqueous electrolyte is 0.02% to 5%.
In some embodiments, the content of the cyclic ester additive in the nonaqueous electrolyte solution of the lithium ion battery is 0.05% to 20% by mass.
In some embodiments, the cyclic ester additive in the nonaqueous electrolyte solution of the lithium ion battery includes any one of or a combination of at least two of a cyclic carbonate additive, a cyclic sultone additive, or a cyclic sulfate additive.
In some embodiments, the cyclic carbonate-based additive includes any one of vinylene carbonate, fluoroethylene carbonate, or ethylene carbonate, or a combination of at least two thereof.
In some embodiments, the cyclic sultone-based additive comprises either or a combination of 1, 3-propane sultone or 1, 3-propene sultone.
In some embodiments, the cyclic sulfate-based additive includes any one of vinyl sulfate or propylene sulfate or a combination of at least two thereof.
In some embodiments, the electrolyte is a lithium salt.
In some embodiments, the lithium salt comprises lithium hexafluorophosphate.
In some embodiments, the concentration of lithium hexafluorophosphate in the lithium ion battery nonaqueous electrolyte is 0.5 to 2 mol/L.
In some embodiments, the additive further comprises a lithium salt additive.
In some embodiments, the lithium salt additive comprises any one of or a combination of at least two of lithium bis (oxalato) difluorophosphate, lithium difluorooxalato borate, lithium bis (fluorosulfonyl) imide, or lithium bis (trifluoromethylsulfonyl) imide.
In some embodiments, the lithium salt additive is present in the lithium ion battery nonaqueous electrolyte in an amount of 0.05 to 20% by mass.
In some embodiments, the non-aqueous solvent comprises any one of ethylene carbonate, dimethyl carbonate, ethyl methyl carbonate, propylene carbonate, or diethyl carbonate, or a combination of at least two thereof.
In some embodiments, the nonaqueous solvent in the nonaqueous electrolyte solution of the lithium ion battery is 60 to 85 mass percent.
In one embodiment, a lithium ion battery comprising the lithium ion battery non-aqueous electrolyte is provided, and the lithium ion battery comprises the lithium ion battery non-aqueous electrolyte.
In one embodiment, the lithium ion battery further includes a positive electrode current collector and a positive electrode active material coated on the positive electrode current collector, a negative electrode current collector and a negative electrode active material coated on the negative electrode current collector, and a separator.
In one embodiment, the positive active material includes any one of lithium cobalt oxide, lithium nickel oxide, lithium manganese oxide, lithium nickel cobalt manganese oxide, or lithium nickel cobalt aluminum oxide, or a combination of at least two thereof.
In one embodiment, the negative active material includes any one of soft carbon, hard carbon, artificial graphite, natural graphite, silicon oxy compound, silicon carbon compound, or lithium titanate, or a combination of at least two thereof.
Example 1
The embodiment provides a lithium ion battery nonaqueous electrolyte, which comprises 2.5% of a fourth compound, 2.5% of vinylene carbonate, 2.5% of 1, 3-propane sultone and 5% of an additive of vinyl sulfate by mass percentage, wherein the lithium salt comprises 1mol/L lithium hexafluorophosphate, 2.5% of lithium difluorophosphate, 2.5% of lithium difluorosulfonimide and 5% of lithium difluorophosphate by mass percentage, and the balance is a nonaqueous solvent, wherein the nonaqueous solvent consists of vinyl carbonate, ethyl methyl carbonate and diethyl carbonate in a mass ratio of 3:5: 2.
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery-grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the nonaqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the nonaqueous solvent, adding a fourth compound, 2.5% of vinylene carbonate, 2.5% of 1, 3-propane sultone and 5% of vinyl sulfate in mass percentage, respectively, and then adding 2.5% of lithium difluorophosphate, 2.5% of lithium difluorosulfonimide and 5% of lithium difluorophosphate in mass percentage to make the concentration of the lithium hexafluorophosphate be 1mol/L, thereby preparing the lithium ion battery nonaqueous electrolyte.
The preparation method of the lithium ion battery comprises the following steps:
LiNi as positive electrode active material0.8Co0.1Mn0.1O2The conductive agent acetylene black and the adhesive polyvinylidene fluoride are fully stirred and uniformly mixed in an N-methyl pyrrolidone solvent system according to the mass ratio of 95:3:2, coated on an aluminum foil, dried and cold-pressed to obtain the positive pole piece, and the compaction density of the positive pole piece is 3.5g/cm3。
Graphite as negative active material, acetylene black as conducting agent, styrene butadiene rubber as binder and carbon-methyl fiber as thickenerFully stirring and uniformly mixing the sodium ascorbate in a deionized water solvent system according to a mass ratio of 96:2:1:1, coating the mixture on a copper foil, drying and cold-pressing the mixture to obtain a negative pole piece, wherein the compaction density of the negative pole piece is 1.65g/cm3。
Polyethylene with the thickness of 9 mu m is taken as a base film, and a nano aluminum oxide coating with the thickness of 3 mu m is coated on the base film to obtain the diaphragm.
And stacking the positive pole piece, the diaphragm and the negative pole piece in sequence, so that the diaphragm is positioned between the positive pole piece and the negative pole piece to play an isolating role, and stacking the pieces to obtain the bare cell.
And (2) filling the bare cell into an aluminum plastic film, baking at 80 ℃ to remove water, injecting corresponding electrolyte, sealing, standing, hot-cold pressing, forming, clamping, capacity grading and other procedures to obtain the finished product of the flexibly-packaged lithium ion secondary battery.
Example 2
The embodiment provides a lithium ion battery nonaqueous electrolyte, which comprises 0.02 mass percent of a fourth compound, 0.025 mass percent of vinylene carbonate and 0.025 mass percent of an additive of 1, 3-propane sultone, wherein the lithium salt is lithium hexafluorophosphate with the concentration of 0.5mol/L, 5 mass percent of lithium difluorophosphate, 5 mass percent of lithium difluorosulfonimide and 10 mass percent of lithium difluorophosphate, and the balance is a nonaqueous solvent, wherein the nonaqueous solvent is composed of ethylene carbonate, ethyl methyl carbonate and diethyl carbonate in a mass ratio of 3:5: 2.
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the nonaqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the nonaqueous solvent, adding a fourth compound with the mass percentage of 0.02%, vinylene carbonate with the mass percentage of 0.025% and 1, 3-propane sultone with the mass percentage of 0.025%, adding lithium difluorophosphate with the mass percentage of 5%, lithium difluorosulfonimide with the mass percentage of 5% and lithium difluorophosphate with the mass percentage of 10% so that the concentration of the lithium hexafluorophosphate is 0.5mol/L, and preparing the lithium ion battery nonaqueous electrolyte.
The preparation method of the lithium ion battery comprises the following steps: the preparation method of the lithium ion battery of the present example is the same as that of example 1.
Example 3
The embodiment provides a lithium ion battery nonaqueous electrolyte, wherein the lithium ion nonaqueous electrolyte comprises, by taking the total mass of the nonaqueous electrolyte as 100%, 5% by mass of a fourth compound, 5% by mass of vinylene carbonate, 10% by mass of 1, 3-propane sultone and 5% by mass of an additive of vinyl sulfate, lithium salt is lithium hexafluorophosphate with a concentration of 2mol/L, lithium difluorophosphate with a mass percentage of 0.025% by mass and lithium difluorosulfonimide with a mass percentage of 0.025% by mass, and the balance is a nonaqueous solvent which is composed of vinyl carbonate, ethyl methyl carbonate and diethyl carbonate in a mass ratio of 3:5: 2.
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery-grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the non-aqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the non-aqueous solvent, adding a fourth compound with the mass percentage of 5%, vinylene carbonate with the mass percentage of 5%, 1, 3-propane sultone with the mass percentage of 10% and ethylene sulfate with the mass percentage of 5%, adding lithium difluorophosphate with the mass percentage of 0.025% and lithium difluorosulfonimide with the mass percentage of 0.025% respectively, and enabling the concentration of the lithium hexafluorophosphate to be 2mol/L to prepare the non-aqueous electrolyte of the lithium ion battery.
The preparation method of the lithium ion battery comprises the following steps: the preparation method of the lithium ion battery of the present example is the same as that of example 1.
Example 4
The embodiment provides a lithium ion battery nonaqueous electrolyte, which comprises an additive containing a fifth compound 2.5% by mass, vinylene carbonate 2.5% by mass, 1, 3-propane sultone 2.5% by mass and vinyl sulfate 5% by mass, lithium salts including lithium hexafluorophosphate with a concentration of 1mol/L, lithium difluorophosphate 2.5% by mass, lithium bis-fluorosulfonylimide 2.5% by mass and lithium bis-difluorophosphate 5% by mass, and a nonaqueous solvent in the balance, wherein the nonaqueous solvent is composed of vinyl carbonate, ethyl methyl carbonate and diethyl carbonate in a mass ratio of 3:5:2, based on 100% by mass of the total mass of the nonaqueous electrolyte. .
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery-grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the nonaqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the nonaqueous solvent, adding a fifth compound with the mass percentage of 2.5%, vinylene carbonate with the mass percentage of 2.5%, 1, 3-propane sultone with the mass percentage of 2.5% and vinyl sulfate with the mass percentage of 5%, adding lithium difluorophosphate with the mass percentage of 2.5%, lithium bis-fluorosulfonimide with the mass percentage of 2.5% and lithium bis-difluorophosphate with the mass percentage of 5% respectively, and enabling the concentration of the lithium hexafluorophosphate to be 1mol/L to prepare the lithium ion battery nonaqueous electrolyte.
The preparation method of the lithium ion battery comprises the following steps: the preparation method of the lithium ion battery of the present example is the same as that of example 1.
Example 5
The embodiment provides a lithium ion battery nonaqueous electrolyte, which comprises an additive containing 0.02 mass percent of a fifth compound, 0.025 mass percent of vinylene carbonate and 0.025 mass percent of 1, 3-propane sultone, wherein the lithium salt is lithium hexafluorophosphate with the concentration of 0.5mol/L, 5 mass percent of lithium difluorophosphate, 5 mass percent of lithium difluorosulfonimide and 10 mass percent of lithium difluorophosphate, and the balance is a nonaqueous solvent, wherein the nonaqueous solvent is composed of ethylene carbonate, ethyl methyl carbonate and diethyl carbonate according to the mass ratio of 3:5:2, based on the total mass of the nonaqueous electrolyte as 100%.
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the nonaqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the nonaqueous solvent, adding a fifth compound with the mass percentage of 0.02%, vinylene carbonate with the mass percentage of 0.025% and 1, 3-propane sultone with the mass percentage of 0.025%, adding lithium difluorophosphate with the mass percentage of 5%, lithium difluorosulfonimide with the mass percentage of 5% and lithium difluorophosphate with the mass percentage of 10% so that the concentration of the lithium hexafluorophosphate is 0.5mol/L, and preparing the lithium ion battery nonaqueous electrolyte.
The preparation method of the lithium ion battery comprises the following steps: the preparation method of the lithium ion battery of the present example is the same as that of example 1.
Example 6
The embodiment provides a lithium ion battery nonaqueous electrolyte, which comprises an additive containing a fifth compound 5% by mass, vinylene carbonate 5%, 1, 3-propane sultone 10% by mass and vinyl sulfate 5% by mass, lithium salt including lithium hexafluorophosphate 2mol/L in concentration and lithium difluorophosphate 0.025% by mass and lithium difluorosulfonimide 0.025% by mass, respectively, and the balance of a nonaqueous solvent, wherein the nonaqueous solvent is composed of vinyl carbonate, ethyl methyl carbonate and diethyl carbonate in a mass ratio of 3:5:2, based on 100% by mass of the total mass of the nonaqueous electrolyte.
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery-grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the non-aqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the non-aqueous solvent, adding a fifth compound with the mass percentage of 5%, vinylene carbonate with the mass percentage of 5%, 1, 3-propane sultone with the mass percentage of 10% and ethylene sulfate with the mass percentage of 5%, adding lithium difluorophosphate with the mass percentage of 0.025% and lithium difluorosulfonimide with the mass percentage of 0.025% respectively, and enabling the concentration of the lithium hexafluorophosphate to be 2mol/L to prepare the non-aqueous electrolyte of the lithium ion battery.
The preparation method of the lithium ion battery comprises the following steps: the preparation method of the lithium ion battery of the present example is the same as that of example 1.
Example 7
The embodiment provides a lithium ion battery nonaqueous electrolyte, which comprises an additive containing 0.4% by mass of a fourth compound, 0.1% by mass of a fifth compound, 1% by mass of vinyl sulfate, 0.5% by mass of vinylene carbonate and 1% by mass of 1, 3-propane sultone, wherein the lithium salt comprises lithium hexafluorophosphate with the concentration of 1mol/L, 0.8% by mass of lithium difluorophosphate, 0.5% by mass of lithium difluorosulfonimide and 0.5% by mass of lithium difluorophosphate, and the balance of a nonaqueous solvent, wherein the nonaqueous solvent consists of vinyl carbonate, methyl ethyl carbonate and diethyl carbonate in a mass ratio of 3:5:2, based on the total mass of the nonaqueous electrolyte being 100%.
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery-grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the nonaqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the nonaqueous solvent, adding a fourth compound with the mass percentage of 0.4%, a fifth compound with the mass percentage of 0.1%, 1% of ethylene sulfate, 0.5% of vinylene carbonate and 1% of 1, 3-propane sultone, adding lithium difluorophosphate with the mass percentage of 0.8%, lithium difluorosulfonimide with the mass percentage of 0.5% and lithium difluorophosphate with the mass percentage of 0.5% to make the concentration of the lithium hexafluorophosphate be 1mol/L, and preparing the lithium ion battery nonaqueous electrolyte.
The preparation method of the lithium ion battery comprises the following steps: the preparation method of the lithium ion battery of the present example is the same as that of example 1.
Example 8
The embodiment provides a lithium ion battery nonaqueous electrolyte, which comprises an additive containing 0.26 mass percent of a fourth compound, 0.13 mass percent of a fifth compound, 1 mass percent of ethylene sulfate, 0.5 mass percent of vinylene carbonate and 1 mass percent of 1, 3-propane sultone based on 100 mass percent of the total mass of the nonaqueous electrolyte, lithium salts comprise lithium hexafluorophosphate with the concentration of 1mol/L, 0.8 mass percent of lithium difluorophosphate, 0.5 mass percent of lithium difluorosulfonimide and 0.5 mass percent of lithium difluorophosphate, and the balance is a nonaqueous solvent, wherein the nonaqueous solvent consists of ethylene carbonate, methyl ethyl carbonate and diethyl carbonate in a mass ratio of 3:5: 2.
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery-grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the nonaqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the nonaqueous solvent, adding a fourth compound with the mass percentage of 0.26%, a fifth compound with the mass percentage of 0.13%, 1% of ethylene sulfate, 0.5% of vinylene carbonate and 1% of 1, 3-propane sultone, adding lithium difluorophosphate with the mass percentage of 0.8%, lithium difluorosulfonimide with the mass percentage of 0.5% and lithium difluorophosphate with the mass percentage of 0.5% to make the concentration of the lithium hexafluorophosphate be 1mol/L, and preparing the lithium ion battery nonaqueous electrolyte.
The preparation method of the lithium ion battery comprises the following steps: the preparation method of the lithium ion battery of the present example is the same as that of example 1.
Example 9
The embodiment provides a lithium ion battery nonaqueous electrolyte, which comprises an additive containing 0.16 mass percent of a fourth compound, 0.16 mass percent of a fifth compound, 1 mass percent of vinyl sulfate, 0.5 mass percent of vinylene carbonate and 1 mass percent of 1, 3-propane sultone based on 100 mass percent of the total mass of the nonaqueous electrolyte, lithium salts comprise lithium hexafluorophosphate with the concentration of 1mol/L, 0.8 mass percent of lithium difluorophosphate, 0.5 mass percent of lithium difluorosulfonimide and 0.5 mass percent of lithium difluorophosphate, and the balance is a nonaqueous solvent, wherein the nonaqueous solvent consists of vinyl carbonate, methyl ethyl carbonate and diethyl carbonate in a mass ratio of 3:5: 2.
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery-grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the nonaqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the nonaqueous solvent, adding a fourth compound with the mass percentage of 0.16%, a fifth compound with the mass percentage of 0.16%, 1% of ethylene sulfate, 0.5% of vinylene carbonate and 1% of 1, 3-propane sultone, adding lithium difluorophosphate with the mass percentage of 0.8%, lithium difluorosulfonimide with the mass percentage of 0.5% and lithium difluorophosphate with the mass percentage of 0.5% to make the concentration of the lithium hexafluorophosphate be 1mol/L, and preparing the lithium ion battery nonaqueous electrolyte.
The preparation method of the lithium ion battery comprises the following steps: the preparation method of the lithium ion battery of the present example is the same as that of example 1.
Example 10
The embodiment provides a lithium ion battery nonaqueous electrolyte, which comprises an additive containing 0.09 mass percent of a fourth compound, 0.18 mass percent of a fifth compound, 1 mass percent of vinyl sulfate, 0.5 mass percent of vinylene carbonate and 1 mass percent of 1, 3-propane sultone based on 100 mass percent of the total mass of the nonaqueous electrolyte, lithium salts comprise lithium hexafluorophosphate with the concentration of 1mol/L, 0.8 mass percent of lithium difluorophosphate, 0.5 mass percent of lithium difluorosulfonimide and 0.5 mass percent of lithium difluorophosphate, and the balance is a nonaqueous solvent, wherein the nonaqueous solvent consists of vinyl carbonate, methyl ethyl carbonate and diethyl carbonate in a mass ratio of 3:5: 2.
The preparation method of the non-aqueous electrolyte of the lithium ion battery comprises the following steps: the electrolyte was prepared in a glove box with a nitrogen content of 99.999%, an actual oxygen content of 0.1ppm and a moisture content of 0.1 ppm. Uniformly mixing ethylene carbonate, ethyl methyl carbonate and a diethyl carbonate battery-grade organic solvent in a mass ratio of 3:5:2 by taking the total mass of the nonaqueous electrolyte as 100%, adding fully dried lithium hexafluorophosphate into the nonaqueous solvent, adding a fourth compound with the mass percentage of 0.09%, a fifth compound with the mass percentage of 0.18%, 1% of ethylene sulfate, 0.5% of vinylene carbonate and 1% of 1, 3-propane sultone, adding lithium difluorophosphate with the mass percentage of 0.8%, lithium difluorosulfonimide with the mass percentage of 0.5% and lithium difluorophosphate with the mass percentage of 0.5% to make the concentration of the lithium hexafluorophosphate be 1mol/L, and preparing the lithium ion battery nonaqueous electrolyte.
The preparation method of the lithium ion battery comprises the following steps: the preparation method of the lithium ion battery of the present example is the same as that of example 1.
Example 11
This example is different from example 1 in that the fourth compound is replaced with a tetravinylsilane, and the rest is the same as example 1.
Example 12
This example is different from example 1 in that the fourth compound was replaced with the third compound, and the rest was the same as example 1.
Example 13
This example differs from example 1 in that the fourth compound was replaced with diethyldivinylsilane, and the rest was the same as example 1.
Example 14
This example is different from example 1 in that the fourth compound was replaced with the second compound, and the rest was the same as example 1.
Comparative example 1
The comparative example is different from example 1 in that the content of the fourth compound by mass is 20% based on 100% of the total mass of the nonaqueous electrolytic solution, the amount of the nonaqueous solvent is adjusted to 100% of the total amount of the electrolytic solution, and the other raw materials, the compounding ratio, and the content by mass of each component are the same as those of example 1.
Comparative example 2
The comparative example is different from example 4 in that the content of the fifth compound by mass is 20% based on 100% of the total mass of the nonaqueous electrolytic solution, the amount of the nonaqueous solvent is adjusted to 100% of the total amount of the electrolytic solution, and the other raw materials, the compounding ratio, and the content by mass of each component are the same as those of example 4.
Comparative example 3
The comparative example is different from example 7 in that the fourth compound and the fifth compound additive are not added, the amount of the non-aqueous solvent is adaptively adjusted to make the total amount of the electrolyte be 100%, and other raw materials, mixture ratios and mass percentage contents of the components are the same as those of example 7.
Comparative example 4
The comparative example is different from example 7 in that the amount of the fourth compound was 20% by mass and the amount of the fifth compound was 20% by mass based on 100% by mass of the total mass of the nonaqueous electrolytic solution, and the amount of the nonaqueous solvent was adjusted to 100% by mass of the total amount of the electrolytic solution, and the other raw materials, the compounding ratios, and the mass percentages of the respective components were the same as those of example 7.
Comparative example 5
The comparative example is different from example 7 in that the fourth compound and the fifth compound additive are not added, tetraethylsilane is added in an amount of 0.5% by mass based on 100% by mass of the total nonaqueous electrolyte, the amount of the nonaqueous solvent is adaptively adjusted so that the total amount of the electrolyte is 100%, and the other raw materials, the mixture ratio and the mass percentage of each component are the same as those in example 7.
Comparative example 6
The comparative example is different from example 7 in that the fourth compound and the fifth compound additive are not added, tetraethylsilane is added in an amount of 10% by mass based on 100% by mass of the total nonaqueous electrolyte, the amount of the nonaqueous solvent is adaptively adjusted to make the total amount of the electrolyte 100%, and the other raw materials, the mixture ratio and the mass percentage of each component are the same as those in example 7.
Test conditions
The lithium ion batteries prepared in examples 1 to 14 and comparative examples 1 to 6 were respectively subjected to a high-temperature storage performance test, the test method was as follows:
charging the lithium ion battery to 4.2V at a constant current of 1C at 25 ℃, then charging to a constant voltage of 4.2V until the current is less than 0.05C, and then discharging to 3.0V at a constant current of 0.5C, testing the discharge capacity of the lithium ion battery at the moment and recording the discharge capacity as D0(ii) a Charging to 4.2V at a constant current of 1C, then charging to a current of less than 0.05C at a constant voltage of 4.2V, then storing the lithium ion battery at 60 ℃ for 30 days, and after the storage is finished, discharging to 3.0V at a constant current of 1C; charging to 4.2V at constant current of 1C, charging to current less than 0.05C at constant voltage of 4.2V, discharging to 3.0V at constant current of 0.5C, testing discharge capacity of the lithium ion battery at the moment, and recording as D1. The capacity retention rate relative to the lithium ion battery before storage was calculated according to the following formula:
capacity retention (%) - (D)1/D0)×100％。
Charging the lithium ion battery to 4.2V at a constant current of 1C at 25 ℃, then charging the lithium ion battery to a constant voltage of 0.05C, testing the thickness of the lithium ion battery before storage and recording the thickness as h0. Then the battery in the full charge state is placed in a 60 ℃ oven for storage for 30 days, and the thickness after storage is tested and recorded as h1The thickness expansion rate with respect to the lithium ion battery before storage is calculated according to the following formula:
thickness expansion ratio (%) - (h)1-h0)/h0×100％。
The results of the test are shown in table 1:
table 1:
as can be seen from the data in tables 1 and 2, the additive-containing nonaqueous electrolyte is adopted in the invention, and the lithium ion batteries prepared in the above examples are tested for high-temperature storage performance, compared with comparative examples 1 to 4, the capacity retention rate of the lithium ion batteries provided in examples 1 to 14 is as high as 86% or more, and particularly the capacity retention rate of the lithium ion battery provided in example 10 is as high as 98.9%, which further illustrates that the lithium ion batteries prepared by using the electrolyte of the invention have the advantages of high capacity retention rate and high-temperature stability; compared with examples 7-10, the change of the proportion of the mono-alkenyl silane fourth compound additive and the trienyl silane fifth compound additive shows that the number of formed compound nodes can be changed, and when the additive content is proper and the number of the nodes reaches 2-2.5, the electrolyte provided by the invention can relieve the volume expansion of the battery, so that the electrolyte provided by the invention has excellent high-temperature long-cycle stability and high-temperature storage stability and good safety performance when being applied to a lithium ion battery.
Comparative examples 1 and 2 show that the addition of an excessive amount of the olefin additive increases the impedance thereof, which hinders the improvement of the battery performance; comparative example 3, in which no additive was added, exhibited the worst cell performance; comparative example 4, in which an excessive amount of the fourth compound and the fifth compound were added at the same time, also had negative effects on the performance of the battery, as in comparative examples 1 and 2; comparative examples 5 and 6, in which the tetraethylsilane additive was added, provided batteries that exhibited poor effects in both capacity retention and thickness expansion under high-temperature storage conditions, because a stable SEI film could not be formed on the surface of an electrode by means of oxidative polymerization.
The applicant states that the present invention is illustrated by the above examples of the process of the present invention, but the present invention is not limited to the above process steps, i.e. it is not meant that the present invention must rely on the above process steps to be carried out. It will be apparent to those skilled in the art that any modification of the present invention, equivalent substitutions of selected materials and additions of auxiliary components, selection of specific modes and the like, which are within the scope and disclosure of the present invention, are contemplated by the present invention.
Claims (10)
1. A lithium ion battery non-aqueous electrolyte solution is characterized by comprising an electrolyte, a non-aqueous solvent and an additive, wherein the additive comprises a first compound with a structure shown in a formula 1 and a cyclic ester additive:
wherein R is1、R2、R3And R4Each independently selected from-CH-X, C2 to C6 straight chain alkyl or C2 to C6 branched chain alkyl;
the X is selected from linear alkyl of-H, C2 to C6 or branched alkyl of C2 to C6;
the R is1、R2、R3And R4At least one of which is selected from-CH ═ CH-X.
2. The nonaqueous electrolyte solution for lithium-ion batteries according to claim 1, wherein the first compound comprises a second compound having a structure represented by formula 2, a third compound having a structure represented by formula 3, a fourth compound having a structure represented by formula 4, and/or a fifth compound having a structure represented by formula 5:
preferably, the mass percentage of the first compound in the lithium ion battery nonaqueous electrolyte is 0.02% to 5%.
3. The nonaqueous electrolyte solution for lithium ion batteries according to claim 1 or 2, wherein the content of the cyclic ester additive in the nonaqueous electrolyte solution for lithium ion batteries is 0.05 to 20% by mass.
4. The nonaqueous electrolyte solution for a lithium ion battery according to any one of claims 1 to 3, wherein the cyclic ester additive in the nonaqueous electrolyte solution for a lithium ion battery includes any one of a cyclic carbonate additive, a cyclic sultone additive, or a cyclic sulfate additive, or a combination of at least two thereof.
5. The nonaqueous electrolyte solution for lithium ion batteries according to claim 4, wherein the cyclic carbonate additive comprises any one of vinylene carbonate, fluoroethylene carbonate or ethylene carbonate or a combination of at least two of them;
preferably, the cyclic sultone additive comprises any one or a combination of two of 1, 3-propane sultone and 1, 3-propylene sultone.
6. The nonaqueous electrolyte solution for lithium ion batteries according to claim 4 or 5, wherein the cyclic sulfate-based additive comprises any one of vinyl sulfate or propylene sulfate or a combination of at least two of the vinyl sulfate and the propylene sulfate.
7. The nonaqueous electrolyte solution for a lithium ion battery according to any one of claims 1 to 6, wherein the electrolyte is a lithium salt;
preferably, the lithium salt comprises lithium hexafluorophosphate;
preferably, the concentration of lithium hexafluorophosphate in the lithium ion battery nonaqueous electrolyte is 0.5mol/L to 2 mol/L;
preferably, the additive further comprises a lithium salt additive;
preferably, the lithium salt additive comprises any one of or a combination of at least two of lithium bis (oxalate) difluorophosphate, lithium difluorooxalate borate, lithium bis (fluorosulfonyl) imide or lithium bis (trifluoromethylsulfonyl) imide;
preferably, the lithium salt additive in the lithium ion battery non-aqueous electrolyte is 0.05 to 20 mass percent.
8. The nonaqueous electrolyte for a lithium ion battery according to any one of claims 1 to 7, wherein the nonaqueous solvent includes any one of ethylene carbonate, dimethyl carbonate, ethyl methyl carbonate, propylene carbonate, or diethyl carbonate, or a combination of at least two thereof;
preferably, the mass percentage of the nonaqueous solvent in the nonaqueous electrolyte of the lithium ion battery is 60-85%.
9. A lithium ion battery, characterized in that the lithium ion battery comprises the lithium ion battery nonaqueous electrolytic solution according to any one of claims 1 to 8.
10. The lithium ion battery of claim 9, further comprising a positive electrode current collector and a positive electrode active material coated on the positive electrode current collector, a negative electrode current collector and a negative electrode active material coated on the negative electrode current collector, and a separator;
preferably, the positive active material includes any one or a combination of at least two of lithium cobalt oxide, lithium nickel oxide, lithium manganese oxide, lithium nickel cobalt manganese oxide, or lithium nickel cobalt aluminum oxide;
preferably, the negative active material includes any one of soft carbon, hard carbon, artificial graphite, natural graphite, silicon oxy compound, silicon carbon compound, or lithium titanate, or a combination of at least two thereof.
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