CN114335687A - Lithium ion battery and preparation method thereof - Google Patents
Lithium ion battery and preparation method thereof Download PDFInfo
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Abstract
The invention provides a lithium ion battery and a preparation method thereof, wherein the lithium ion battery takes a ternary material as a positive active material and takes a mixture of a graphite material and silicon as a negative active material, the graphite material in the negative active material is of a sheet structure, and the silicon is of a spherical or spheroidal structure; the lithium ion battery provided by the invention adopts the combination of the positive electrode active material and the negative electrode active material, so that the obtained lithium ion battery has high capacity and excellent rate performance.
Description
Technical Field
The invention belongs to the field of battery materials, and relates to a lithium ion battery and a preparation method thereof.
Background
At present, the anode materials adopted in the lithium battery market are basically lithium cobaltate, which has the characteristic of high battery safety, but the voltage is too low, and the problem of insufficient capacity when the lithium battery is used on a mobile phone (the cut-off voltage of the mobile phone is generally about 3.4V) is obvious; the ternary lithium ion battery has the advantages of high voltage, high specific energy, wide working temperature range, high specific power, stable discharge and long storage time, but the application of the ternary lithium ion battery in high-capacity and high-rate charge and discharge is limited by the composition of the currently adopted negative active substance and electrolyte;
CN108258191A discloses a lithium ion battery, which includes: a housing; the positive plate and the negative plate are positioned in the shell, and a diaphragm is arranged between the positive plate and the negative plate; the negative plate comprises a plurality of side reaction active sites, wherein the side reaction active sites are formed by volatilizing volatile substances with boiling points lower than a preset boiling point in negative slurry in the process of forming the negative plate; the positive plate is internally provided with an over-charging gas production substance which generates gas when the charging voltage of the lithium ion battery reaches a preset charging voltage. According to the technical scheme provided by the invention, the side reaction active sites are formed in the negative plate, and the overcharge and gas production substance is arranged in the positive plate, so that a large amount of gas can be produced in the overcharge of the lithium ion battery, and the produced gas is discharged in time in a loosened winding core, and a current cut-off device in the lithium ion battery can be opened in time, so that the lithium ion battery is disconnected, and the safety performance of the high-rate lithium ion battery is improved; CN103199262A discloses a method for manufacturing a high-capacity, high-rate, high-safety lithium ion battery, which adopts a positive electrode material, a mesh current collector, a negative electrode material, a diaphragm, and an electrolyte, and coats the positive electrode material and the negative electrode material on the current collector to manufacture a pole piece, so as to manufacture a battery, wherein the current collector is manufactured by the following steps: (1) dissolving polyvinylidene fluoride or polytetrafluoroethylene in N-methyl pyrrolidone in a stirring pot or dissolving CMC in deionized water, adding SBR, stirring for 3-6h, adding one or a powder mixture of silicon dioxide and aluminum oxide to the mixture to obtain a powder with a concentration of 0.5-2%, and stirring to uniformly disperse the powder in a PVDF solution; (2) coating the glue solution of the powder on a reticular current collector by using a coating machine, and baking the powder in an oven, wherein the thickness of the powder on the reticular current collector is 0.5-3 mu m; the above documents give some structural schemes suitable for high-capacity and high-rate lithium ion batteries, but the structural schemes only improve the battery performance in terms of safety or current collector arrangement, and the obtained lithium ion battery still has the problems of insufficient capacity or incapability of being used for high-rate charge and discharge;
therefore, the development of a high-capacity and high-rate lithium ion battery and a preparation method thereof still have important significance.
Disclosure of Invention
The invention aims to provide a lithium ion battery and a preparation method thereof, wherein the lithium ion battery is a 18650 type lithium ion battery, the lithium ion battery takes a ternary material as a positive electrode active substance and takes a mixture of a graphite material and silicon as a negative electrode active substance, the graphite material in the negative electrode active substance is of a sheet structure, and the silicon is of a spherical or spheroidal structure; the lithium ion battery provided by the invention adopts the combination of the positive electrode active substance and the negative electrode active substance, so that the obtained lithium ion battery has high capacity and excellent rate capability, the capacity of the obtained lithium ion battery can reach 3.0mAh, and the discharge rate of the lithium ion battery can reach 10C-15C.
In order to achieve the purpose, the invention adopts the following technical scheme:
in a first aspect, the invention provides a lithium ion battery, wherein a positive active material of the lithium ion battery is a ternary material, a negative active material of the lithium ion battery is a mixture of a graphite material and silicon, the graphite material is a sheet structure, and the silicon is a spherical or spheroidal structure.
The lithium ion battery adopts the ternary material as the anode active material, simultaneously adopts the mixture of the graphite material and the silicon as the cathode active material, and the combination of the two materials obviously improves the capacity and the rate capability of the obtained lithium ion battery.
In the invention, silicon in the mixture of the graphite material and the silicon can be alloyed with lithium at normal temperature, so that the lithium ion battery has high capacity which can reach 3.0 mAh.
In the invention, the silicon-based material with a spherical or quasi-spherical structure means that: the overall shape of the material is spherical or approximately spherical, and the material can be a silicon simple substance, a silicon-oxygen material, a silicide containing lithium or magnesium, and the like.
Preferably, the ternary material is nickel cobalt lithium manganate with high nickel content, and the molar content of nickel element in the nickel cobalt lithium manganate with high nickel content is more than 60%.
Preferably, the graphite material is carbonized artificial graphite.
Preferably, the silicon-based material is silicon oxide, and the silicon oxide has high first efficiency, so that the electrochemical performance of the battery is improved.
Preferably, the particle size D50 of the silicon-based material is 5um-6um, such as 5um, 5.2um, 5.3um, 5.5um, 5.7um, 5.8um or 6um, etc.
Preferably, the mass ratio of the graphite material to the silicon is (7-10): 1, e.g. 7: 1. 7.2: 1. 7.3: 1. 7.5: 1. 7.8: 1. 8: 1. 8.5: 1. 9: 1. 9.5: 1 or 10: 1, etc.
In the negative active material of the present invention, the mass ratio of the graphite material to the silicon is in the above range, which is advantageous for improving the rate capability of the lithium ion battery while increasing the capacity of the lithium ion battery.
Preferably, the preparation method of the mixture of the graphite material and the silicon-based material comprises the following steps: adding 40-50% (such as 40%, 42%, 43%, 44%, 45%, 47%, 48% or 50%) of graphite material, adding silicon-based material, stirring at 20-50 rpm (such as 20-52%, 53%, 54%, 55%, 56%, 58% or 60%) of graphite material, stirring at the original speed, and controlling the total stirring time at 10-15 min (such as 10min, 12min, 13min, 14min or 15 min).
Preferably, the separator of the lithium ion battery is a single-side coated ceramic separator.
Preferably, the ceramic-coated side of the single-side coated ceramic separator is opposite to the positive electrode.
Preferably, the electrolyte of the lithium ion battery contains a solvent, a lithium salt and a film-forming additive.
Preferably, the lithium salt includes LiODFB, LiFSI, LiPF2O2And LiPF6Preferably, LiODFB, LiFSI and LiPF6Combinations of (a) and (b).
Preferably, the film forming additive comprises VC and/or FEC.
Preferably, the solvent comprises EC, EMC and DMC, and EC: EMC: DMC ═ 1-2: 6-8 by mass ratio, wherein EC is selected in a range (1-2) such as 1, 1.2, 1.5, 1.7 or 2, EMC is selected in a range (1-2) such as 1, 1.2, 1.5, 1.7 or 2, and DMC is selected in a range (6-8) such as 6, 6.2, 6.5, 6.7, 7, 7.5, 7.8 or 8.
Preferably, the electrolyte comprises the following components by taking the total mass of the electrolyte as 100 percent:
in the preferred embodiment, LiPF6The content of (b) may be, for example, 15%, 15.2%, 15.5%, 16%, 17%, or the like; the content of VC may be, for example, 0.5%, 1%, 1.5%, 2%, or the like; the FEC content may be, for example, 5%, 5.5%, 6%, 6.5%, 7%, 8%, or the like; the content of LiODFB may be, for example, 0.5%, 0.6%, 0.7%, 0.8%, 1%, or the like; the content of LiFSI may be, for example, 0.5%, 0.6%, 0.7%, 0.8%, 1%, or the like.
The electrolyte adopts the lithium salt combination and the film forming additive combination with the content, which is beneficial to reducing the DCR of the lithium ion battery and further improving the high-rate discharge capability of the lithium ion battery.
Preferably, the positive electrode of the lithium ion battery comprises a positive electrode current collector and a positive electrode active material layer positioned on the surface of the positive electrode current collector.
Preferably, the positive electrode current collector is an aluminum foil with a thickness of 10um-12um, such as 10um, 10.5um, 11um, 11.5um, or 12 um.
Preferably, the positive electrode active material layer includes a positive electrode active material, a conductive agent, a binder, and an additive including lithium carbonate.
Preferably, the conductive agent in the positive electrode active material layer is a carbon nanotube.
Preferably, the binder in the positive electrode is polyvinylidene fluoride.
Preferably, the mass ratio of the positive electrode active material, the conductive agent, the binder and the additive in the positive electrode active material layer is (96-98): (1-1.5): (1-1.5): (0.3-1), wherein the positive electrode active material is selected from the range (96-98) such as 96, 97, 97.5 or 98, the conductive agent is selected from the range 1, 1.2, 1.3, 1.4 or 1.5, the binder is selected from the range 1, 1.2, 1.3, 1.4 or 1.5, and the additive is selected from the range 0.3, 0.4, 0.5, 0.6, 0.8 or 1.
Preferably, the negative electrode of the lithium ion battery comprises a negative electrode current collector and a negative electrode active material layer on the surface of the negative electrode current collector.
Preferably, the negative electrode current collector includes a copper foil.
Preferably, the anode active material layer includes an anode active material, a conductive agent, and a binder.
Preferably, the conductive agent in the negative electrode includes at least one of conductive carbon black and carbon nanotubes.
Preferably, the binder in the negative electrode includes at least one of sodium carboxymethyl cellulose and styrene butadiene rubber.
In a second aspect, the present invention provides a method for preparing a lithium ion battery according to the first aspect, the method comprising the steps of:
(1) preparing anode slurry and cathode slurry, wherein the anode slurry contains a ternary material, the cathode slurry contains a mixture of a graphite material and a silicon-based material, the graphite material is of a sheet structure, and the silicon-based material is of a spherical or spheroidal structure;
(2) coating the positive electrode slurry obtained in the step (1) on a positive electrode current collector to obtain a positive electrode;
(3) coating the negative electrode slurry obtained in the step (1) on a negative electrode current collector to obtain a negative electrode;
(4) and (3) winding the anode in the step (2), the cathode in the step (3) and the diaphragm into a pole group, and performing post-treatment to obtain the lithium ion battery.
Preferably, the solvent in the positive electrode slurry includes N-methylpyrrolidone (NMP).
Preferably, the preparation method of the cathode slurry in the step (1) includes mixing a ternary material, a conductive agent, a binder, an additive and a solvent to obtain the cathode slurry.
Preferably, the method of mixing is stirring.
Preferably, in the step (1), the negative electrode slurry comprises the following components by mass percent of 100% of the negative electrode slurry:
preferably, the preparation method of the negative electrode slurry comprises the step of mixing a graphite material with a mixture of silicon, a conductive agent, a binder and a solvent to obtain the negative electrode slurry.
Preferably, the step (2) further comprises drying, rolling, slitting and tabletting after coating.
Preferably, the step (3) further comprises drying, rolling, slitting and tabletting after coating.
Preferably, the step (4) further comprises the steps of entering a shell, injecting liquid and sealing after winding.
Preferably, the sealing is followed by priming, formation, aging and partial volume.
As a preferable technical scheme of the invention, the preparation method of the lithium ion battery comprises the following steps:
(a) stirring and mixing the ternary material, the conductive agent, the binder, the additive and the solvent to obtain anode slurry, then coating the anode slurry on an anode current collector, and drying, rolling, slitting and tabletting to obtain an anode;
wherein the mass ratio of the ternary material, the conductive agent, the binder and the additive is (96-98): (1-1.5): (1-1.5): (0.3-1);
(b) mixing a graphite material with a mixture of silicon, a conductive agent, a binder and a solvent to obtain negative electrode slurry, then coating the negative electrode slurry on a negative electrode current collector, and drying, rolling, slitting and tabletting to obtain a negative electrode;
the negative electrode slurry comprises the following components by taking the mass of the negative electrode slurry as 100 percent:
the balance of solvent; (c) and (c) winding the positive electrode in the step (a), the negative electrode in the step (b) and the single-side coated ceramic diaphragm, putting the positive electrode into a shell, injecting liquid and sealing to obtain the lithium ion battery.
The lithium ion battery is 18650 lithium ion battery.
Compared with the prior art, the invention has the following beneficial effects:
the lithium ion battery adopts the ternary material as the positive active material, adopts the mixture of the graphite material and the silicon as the negative active material, the graphite material is of a sheet structure, the silicon is of a spherical or sphere-like structure, and adopts the combination of the positive active material and the negative active material, so that the obtained lithium ion battery has high capacity, the high rate capability of the lithium ion battery is also obviously improved, the capacity of the lithium ion battery can reach 3.0mAh, and the discharge rate of the lithium ion battery can reach 10C-15C.
Drawings
Fig. 1 is an SEM image of a graphite material.
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 embodiment of the present invention, the silicon-based material is available from Violin light technology Co.
Example 1
The positive active material used in the lithium ion battery described in this embodiment is a ternary material (LiNi)0.8Co0.1Mn0.1O2) The negative active material is a mixture of a graphite material and a silicon-based material in a mass ratio of 9: 1; the graphite material is artificial graphite after carbonization, and is a sheet structure, the silica-based material is spherical or spherical-like silicon oxide, and the particle size D50 of the silica-based material is 5 um.
The preparation method of the mixture of the graphite material and the silicon-based material comprises the following steps: adding a graphite material accounting for 50% of the total mass of the graphite material according to the ratio, adding all silicon-based materials, stirring for 5min at a stirring speed of 20rpm, finally adding the graphite material accounting for 50% of the total mass of the graphite material, and continuously stirring for 10min at a stirring speed of 20 rpm.
The electrolyte in the lithium ion battery comprises the following components:
wherein the solvent comprises EC, EMC and DMC, and the mass ratio of EC to EMC to DMC is 2:1: 7.
In the positive electrode of the lithium ion battery in this embodiment, a positive electrode current collector is an aluminum foil (with a thickness of 12um), a conductive agent is a carbon nanotube, a binder is polyvinylidene fluoride, and an additive is lithium carbonate; wherein the mass ratio of the positive electrode active substance to the conductive agent to the binder to the additive is 97: 1.5: 1.2: 0.3;
in the negative electrode of the lithium ion battery, a negative electrode current collector is a copper foil, and a conductive agent is a mixture of conductive carbon black and carbon nanotubes according to a mass ratio of 1: 1, and the binder is sodium carboxymethylcellulose and styrene butadiene rubber in a mass ratio of 1: 1;
the preparation method of the lithium ion battery in the embodiment comprises the following steps:
(a) stirring and mixing the ternary material, the conductive agent, the binder, the additive and the solvent to obtain anode slurry, then coating the anode slurry on an anode current collector, and drying, rolling, slitting and tabletting to obtain an anode;
(b) mixing a mixture of a graphite material and a silicon-based material, a conductive agent, a binder and a solvent to obtain a negative electrode slurry, then coating the negative electrode slurry on a negative electrode current collector, and drying, rolling, slitting and tabletting to obtain a negative electrode;
the negative electrode slurry comprises the following components by taking the mass of the negative electrode slurry as 100 percent:
(c) and (c) winding the positive electrode in the step (a), the negative electrode in the step (b) and the single-side coated ceramic diaphragm, filling the positive electrode into a shell, injecting liquid, sealing, pre-charging, forming, aging and grading to obtain the lithium ion battery.
Example 2
The present example differs from example 1 in that the mass ratio of graphite material to silicon is 8: 1, other conditions were exactly the same as in example 1.
Example 3
The present example differs from example 1 in that the mass ratio of graphite material to silicon is 9.6: 1, other conditions were exactly the same as in example 1.
Example 4
This example differs from example 1 in the lithium salt (LiPF) in the electrolyte6LiODFB and LiFSI) with an equimolar amount of LiPF2O2Other conditions were exactly the same as in example 1.
Comparative example 1
The present comparative example is different from example 3 in that only a graphite material is contained in the negative active material, and other conditions are exactly the same as those in example 3.
Comparative example 2
The comparative example is different from example 3 in that lithium cobaltate is used as the positive electrode active material, and other conditions are completely the same as those in example 3.
And (3) performance testing:
the lithium ion batteries prepared in examples 1 to 4 and comparative examples 1 to 2 were tested for capacity and rate capability, and the test method was: charging the monomer battery cell at a constant current of 0.5C in an environment of 25 +/-2 ℃, standing for 10min, discharging at a constant current of 0.2C, stopping the current at 0.02C, and recording the capacity and the temperature rise; then, the battery cell is charged at a constant current of 0.5C, stands for 10min, discharges at a constant current of 0.5C, stops current of 0.02C, and records capacity and temperature rise; by analogy, the capacity and the temperature rise of 20A/30A/45A are respectively recorded, and the test results are shown in Table 1;
TABLE 1
The applicant declares that the above description is only a specific embodiment of the present invention, but the scope of the present invention is not limited thereto, and it should be understood by those skilled in the art that any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present invention are within the scope and disclosure of the present invention.
Claims (10)
1. A lithium ion battery is characterized in that a positive electrode active substance of the lithium ion battery is a ternary material, a negative electrode active substance is a mixture of a graphite material and a silicon-based material, the graphite material is of a sheet structure, and the silicon-based material is of a spherical or spheroidal structure.
2. The lithium ion battery of claim 1, wherein the ternary material is high nickel content nickel cobalt lithium manganate, and the molar content of nickel element in the high nickel content nickel cobalt lithium manganate is more than 60%;
preferably, the graphite material is carbonized artificial graphite;
preferably, the silicon-based material is silicon oxide;
preferably, the particle size D50 of the silicon-based material is 5um-6 um;
preferably, the mass ratio of the graphite material to the silicon-based material is (7-10): 1;
preferably, the preparation method of the mixture of the graphite material and the silicon-based material comprises the following steps: adding a graphite material accounting for 40-50% of the total mass of the graphite material according to the proportion, then adding all silicon-based materials, stirring at a stirring speed of 20-50 rpm, finally adding the graphite material accounting for 50-60% of the total mass of the graphite material, and continuously stirring at the original speed, wherein the total stirring time is controlled within 10-15 min.
3. The lithium ion battery according to claim 1 or 2, wherein the separator of the lithium ion battery is a single-side coated ceramic separator;
preferably, the ceramic-coated side of the single-side coated ceramic separator is opposite to the positive electrode.
4. The lithium ion battery of any one of claims 1-3, wherein the electrolyte of the lithium ion battery comprises a solvent, a lithium salt, and a film forming additive;
preferably, the lithium salt includes LiODFB, LiFSI, LiPF2O2And LiPF6Preferably, LiODFB, LiFSI and LiPF6A combination of (1);
preferably, the film forming additive comprises VC and/or FEC;
preferably, the solvent comprises EC, EMC and DMC, and in terms of mass ratio, EC: EMC: DMC ═ 1-2: (1-2): 6-8;
preferably, the electrolyte comprises the following components by taking the total mass of the electrolyte as 100 percent:
5. the lithium ion battery according to any one of claims 1 to 4, wherein the positive electrode of the lithium ion battery comprises a positive electrode current collector and a positive electrode active material layer on the surface of the positive electrode current collector;
preferably, the positive current collector is an aluminum foil with the thickness of 10um-12 um;
preferably, the positive electrode active material layer comprises a positive electrode active material, a conductive agent, a binder and an additive, wherein the additive comprises lithium carbonate;
preferably, the conductive agent in the positive electrode active material layer is carbon nanotubes;
preferably, the binder in the positive electrode active material layer is polyvinylidene fluoride;
preferably, the mass ratio of the positive electrode active material, the conductive agent, the binder and the additive in the positive electrode active material layer is (96-98): (1-1.5): (1-1.5): (0.3-1).
6. The lithium ion battery according to any one of claims 1 to 5, wherein the negative electrode of the lithium ion battery comprises a negative electrode current collector and a negative electrode active material layer on a surface of the negative electrode current collector;
preferably, the negative electrode current collector includes a copper foil;
preferably, the anode active material layer includes an anode active material, a conductive agent, and a binder.
7. A method of making a lithium ion battery according to any of claims 1 to 6, comprising the steps of:
(1) preparing anode slurry and cathode slurry, wherein the anode slurry contains a ternary material, the cathode slurry contains a mixture of a graphite material and a silicon-based material, the graphite material is of a sheet structure, and the silicon-based material is of a spherical or spheroidal structure;
(2) coating the positive electrode slurry obtained in the step (1) on a positive electrode current collector to obtain a positive electrode;
(3) coating the negative electrode slurry obtained in the step (1) on a negative electrode current collector to obtain a negative electrode;
(4) and (3) winding the anode in the step (2), the cathode in the step (3) and the diaphragm into a pole group, and performing post-treatment to obtain the lithium ion battery.
8. The method of claim 7, wherein the solvent in the positive electrode slurry comprises N-methyl pyrrolidone;
preferably, the preparation method of the cathode slurry in the step (1) includes mixing a ternary material, a conductive agent, a binder, an additive and a solvent to obtain the cathode slurry;
preferably, the method of mixing is stirring.
9. The method according to claim 7 or 8, wherein in the step (1), the negative electrode slurry comprises the following components by mass based on 100% of the mass of the negative electrode slurry:
preferably, the solvent of the anode slurry includes water;
preferably, the preparation method of the negative electrode slurry comprises the steps of mixing a graphite material with a mixture of silicon, a conductive agent, a binder and a solvent to obtain the negative electrode slurry;
preferably, the step (2) further comprises drying, rolling, slitting and tabletting after coating;
preferably, the step (3) further comprises drying, rolling, slitting and tabletting after coating;
preferably, the step (4) further comprises the steps of entering a shell, injecting liquid and sealing after winding;
preferably, the sealing is followed by priming, formation, aging and partial volume.
10. A method according to any of claims 7-9, characterized in that the method comprises the steps of:
(a) stirring and mixing the ternary material, the conductive agent, the binder, the additive and the solvent to obtain anode slurry, then coating the anode slurry on an anode current collector, and drying, rolling, slitting and tabletting to obtain an anode;
wherein the mass ratio of the ternary material, the conductive agent, the binder and the additive is (96-98): (1-1.5): (1-1.5): (0.3-1);
(b) mixing a graphite material with a mixture of silicon, a conductive agent, a binder and a solvent to obtain negative electrode slurry, then coating the negative electrode slurry on a negative electrode current collector, and drying, rolling, slitting and tabletting to obtain a negative electrode;
the negative electrode slurry comprises the following components by taking the mass of the negative electrode slurry as 100 percent:
(c) and (c) winding the positive electrode in the step (a), the negative electrode in the step (b) and the single-side coated ceramic diaphragm, putting the positive electrode into a shell, injecting liquid and sealing to obtain the lithium ion battery.
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| CN110600696A (en) * | 2019-09-10 | 2019-12-20 | 深圳市比克动力电池有限公司 | Quick-charging type long-circulation cylindrical lithium ion battery with high low-temperature discharge capacity |
| CN111769260A (en) * | 2020-03-20 | 2020-10-13 | 浙江南都电源动力股份有限公司 | High specific energy lithium ion battery and preparation method thereof |
| CN111554903A (en) * | 2020-05-12 | 2020-08-18 | 宁德新能源科技有限公司 | Negative electrode material, negative electrode sheet, electrochemical device, and electronic device |
| CN113363428A (en) * | 2021-07-07 | 2021-09-07 | 远景动力技术(江苏)有限公司 | Silicon-based negative electrode conductive network system and preparation method and application thereof |
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