CN109742391B - High-nickel lithium ion battery, battery positive electrode material and preparation method thereof - Google Patents
High-nickel lithium ion battery, battery positive electrode material and preparation method thereof Download PDFInfo
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Abstract
The invention provides a high nickel lithium ion battery, a battery anode material and a preparation method thereof, wherein a high nickel ternary anode material, a conductive agent, a binder and a low-temperature activated molecular sieve are mixed to obtain a precursor, the precursor is dispersed in N-methyl pyrrolidone to obtain anode slurry, the anode slurry is coated on an aluminum foil, and the aluminum foil coated with the anode slurry is dried to obtain the battery anode material, because the low-temperature activated molecular sieve is added into the high nickel lithium ion battery anode material, the low-temperature activated molecular sieve can absorb trace moisture remained in the battery anode material and electrolyte, inhibit the reaction of water and the electrolyte, reduce the generation of hydrogen fluoride and the corrosion of hydrogen fluoride to the battery anode, enhance the interface stability of the battery anode and the electrolyte, improve the cycle performance, and because the molecular sieve can be activated at low temperature, the dehydration activation can be realized in the process of drying the aluminum foil coated with the anode slurry, simplifies the preparation process and is suitable for industrial production.
Description
Technical Field
The invention relates to the field of lithium ion batteries, in particular to a high-nickel lithium ion battery, a battery anode material and a preparation method thereof.
Background
At present, the high-nickel ternary cathode material is more and more widely applied to the preparation of lithium ion batteries, and has the advantages of high voltage, large energy density, long cycle life and the like compared with the traditional lithium ion battery cathode materials such as lithium iron phosphate, lithium cobaltate, lithium nickel cobalt manganese, lithium manganate and the like. However, in the storage and circulation processes of the high-nickel lithium ion battery, even a trace amount of moisture exists, the moisture and the electrolyte can generate side reaction, the electrolyte is consumed, hydrogen fluoride which has a corrosion effect on the anode material is generated, the stability of the electrode structure is poor, the circulation performance is reduced, and potential safety hazards exist at the same time.
The common methods for modifying the positive electrode of the lithium ion battery at present mainly comprise a coating method and an electrolyte additive method, wherein the coating method is to coat a layer of metal oxide, fluoride or phosphate and other substances on the surface of the positive electrode of the battery to prevent the positive electrode material from directly contacting with the electrolyte, but the coating method can cause the conductivity of the battery to be poor, hinder the transmission of ions in the battery and cause the reduction of the impedance and the rate capability of the battery. The electrolyte additive mainly has the function of improving the chemical stability of the electrolyte during circulation, but the electrochemical performance of the electrolyte is reduced due to the difference of the compatibility of the electrolyte additive and the anode and cathode.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides a high-nickel lithium ion battery, a battery anode material and a preparation method thereof.
In order to achieve the purpose, the invention adopts the following technical scheme:
in one general aspect, a high-nickel lithium ion battery positive electrode material is provided, which comprises an aluminum foil and a positive electrode membrane arranged on the aluminum foil, wherein the positive electrode membrane comprises a high-nickel ternary positive electrode material, a bonding agent, a conductive agent and a low-temperature activated molecular sieve, and the chemical general formula of the low-temperature activated molecular sieve is xRO. ySiO2·zAl2O3·P2O5In the general formula, 0<x≤0.9，0<y is less than or equal to 0.9, z is less than or equal to 1.0 and is less than or equal to 0.1, and R is one of Cu, Ca or Ba.
Preferably, the mass ratio of the high-nickel ternary cathode material to the adhesive to the conductive agent is 7.0-9.0 parts: 0.5-2.0 parts: 0.5-1.0 part by weight of the low-temperature activated molecular sieve, wherein the mass of the low-temperature activated molecular sieve is 0.1-2.0 wt% of the mass of the high-nickel ternary cathode material.
Preferably, the high-nickel ternary cathode material is one or a mixture of at least one of NCM622, NCM811 and NCA.
Preferably, the conductive agent is one of acetylene black, conductive carbon black, conductive graphite, or ketjen black.
Preferably, the binder is one or a mixture of at least one of polyvinylidene fluoride, polytetrafluoroethylene and sodium carboxymethyl cellulose.
Preferably, the aperture of the low-temperature activated molecular sieve is 0.3 nm-2 nm, and the particle size of the low-temperature activated molecular sieve is 3 μm-4 μm.
In another general aspect, a high nickel lithium ion battery is provided, which comprises a positive electrode, a negative electrode, a separator arranged between the positive electrode and the negative electrode, and an electrolyte, wherein the positive electrode is made of the high nickel lithium ion battery positive electrode material.
In another general aspect, there is also provided a method for preparing a high nickel lithium ion battery cathode material, where the high nickel lithium ion battery cathode material is the above-mentioned high nickel lithium ion battery cathode material, and the method for preparing the high nickel lithium ion battery cathode material includes the following steps:
mixing a high-nickel ternary positive electrode material, a conductive agent, a binder and a low-temperature activated molecular sieve to obtain a precursor;
dispersing the precursor in N-methyl pyrrolidone to obtain positive electrode slurry;
and coating the positive electrode slurry on an aluminum foil, and drying the aluminum foil coated with the positive electrode slurry to obtain the battery positive electrode material.
Preferably, the drying environment for drying the aluminum foil coated with the positive electrode slurry is a vacuum environment.
Preferably, the drying temperature range for drying the aluminum foil coated with the anode slurry is 100-120 ℃, and the drying time is 10-12 hours.
The invention provides a high nickel lithium ion battery, a battery anode material and a preparation method thereof, wherein a low-temperature activated molecular sieve is added in the high nickel lithium ion battery anode material, and can adsorb residual trace moisture in the battery anode material and electrolyte, inhibit the reaction of water and the electrolyte, reduce the generation of hydrogen fluoride and the corrosion of the hydrogen fluoride to the battery anode, enhance the interface stability of the battery anode and the electrolyte, and improve the cycle performance.
Drawings
In order to more clearly illustrate the technical solutions in the embodiments of the present invention, the drawings needed to be used in the description of the embodiments will be briefly introduced below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and it is obvious for those skilled in the art to obtain other drawings based on these drawings without creative efforts.
FIG. 1 is a flow chart of a method for preparing the high nickel lithium ion battery anode material of the invention;
FIG. 2 is a schematic microstructural representation of a low temperature activated molecular sieve in an example of the invention;
FIG. 3 is a graph showing the cycle performance of the battery in example 1 of the present invention;
FIG. 4 is a graph showing the cycle performance of the battery in example 2 of the present invention;
FIG. 5 is a schematic view of the cycle performance curve of the battery of comparative example 1 according to the present invention;
FIG. 6 is a schematic diagram showing the cycle performance of the battery of comparative example 2 according to the present invention;
FIG. 7 is a graphical representation of the temperature activation curves for the low temperature activated molecular sieve of the present invention and a conventional molecular sieve.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example 1
Fig. 1 is a flow chart of a method for preparing a high nickel lithium ion battery positive electrode material of the present invention, and as shown in fig. 1, the method for preparing a high nickel lithium ion battery positive electrode material of the present embodiment includes the following steps:
s01, mixing the high-nickel ternary positive electrode material, the conductive agent, the binder and the low-temperature activated molecular sieve to obtain a precursor;
in step S01 of the present embodiment, mixing the high-nickel ternary cathode material, the conductive agent, the binder, and the low-temperature activated molecular sieve specifically includes: weighing 8 parts of: 1: 1, weighing a low-temperature activated molecular sieve with the mass of 0.5 wt% of the high-nickel ternary cathode material, dry-mixing the high-nickel ternary cathode material, the conductive agent, the binder and the low-temperature activated molecular sieve, and uniformly mixing to obtain a precursor.
It is noted that the mass ratio of the high-nickel ternary cathode material, the conductive agent and the binder can also be 9.0: 0.5: 0.5 or 7.0: 2.0: 1.0, namely the selection range of the mass ratio of the components of the high-nickel ternary positive electrode material, the adhesive and the conductive agent is 7.0-9.0 parts: 0.5-2.0 parts: 0.5-1.0 part, wherein the content of the adhesive cannot be too high, otherwise, the conductivity of the battery electrode can be reduced.
Further, the chemical component of the high-nickel ternary cathode material is LiNi0.6Co0.2Mn0.2(NCM622), of course, the chemical composition of the high-nickel ternary cathode material can be replaced by LiNi according to actual production requirements0.8Co0.1Mn0.1(NCM811)、LiNi0.8Co0.15Al0.05O2(NCA) or other ternary positive electrode materials with similar properties.
Further, the chemical general formula of the low-temperature activated molecular sieve is xRO. ySiO2·zAl2O3·P2O5In the general formula, 0<x≤0.9，0<y is less than or equal to 0.9, z is less than or equal to 1.0 and 0.1 is less than or equal to 1.0, R is one of Cu, Ca or Ba, in the embodiment of the invention, the low-temperature activated molecular sieve containing Cu is adopted, the low-temperature activated molecular sieve can adsorb trace moisture remained in the battery anode material and the electrolyte, inhibit the reaction of water and the electrolyte, reduce the generation of hydrogen fluoride and the corrosion of hydrogen fluoride to the battery anode, enhance the interface stability of the battery anode and the electrolyte and improve the cycle performance, and the activated molecular sieve adopted in the embodiment is at a warm temperatureThe dehydration can be achieved even at a low degree.
FIG. 2 is a schematic diagram of the microstructure of the low-temperature activated molecular sieve in the embodiment of the present invention, as shown in FIG. 2, the pore diameter of the low-temperature activated molecular sieve in the embodiment is 0.3nm to 2nm, and the particle diameter of the low-temperature activated molecular sieve is 3 μm to 4 μm.
Further, the conductive agent of the present embodiment is one of acetylene black, conductive carbon black, conductive graphite, or ketjen black.
Further, the adhesive of the present embodiment is one or a mixture of at least one of polyvinylidene fluoride, polytetrafluoroethylene, and sodium carboxymethyl cellulose.
S02, dispersing the precursor in N-methyl pyrrolidone to obtain positive electrode slurry;
in step S02 of this embodiment, when dispersing the precursor in N-methylpyrrolidone, the precursor is wetted with N-methylpyrrolidone, and after adding the precursor into N-methylpyrrolidone, the solution is stirred and mixed uniformly to form the positive electrode slurry.
S03, coating the positive electrode slurry on an aluminum foil, and drying the aluminum foil coated with the positive electrode slurry to obtain a battery positive electrode material;
in step S03 of this embodiment, the aluminum foil is a current collector commonly used for the positive electrode material, the coating method for coating the positive electrode slurry on the aluminum foil in this embodiment is a roll coating method, which can ensure uniform coating of the positive electrode slurry, and the drying environment for drying the aluminum foil coated with the positive electrode slurry in this embodiment is a vacuum environment, the drying temperature range is 100-120 ℃, the drying time is 10-12 hours, after the positive electrode slurry is dried, a positive electrode membrane can be formed on the surface of the aluminum foil, in the vacuum environment, the moisture in the environment is less, and because the low-temperature activated molecular sieve of this embodiment can also separate the moisture in the interior at a low temperature, the activation process of the low-temperature activated molecular sieve and the drying process of the battery positive electrode material can be performed simultaneously, and as the temperature rises, when the temperature reaches 120 ℃, the low-temperature activated molecular sieve completes dehydration activation, and then the battery positive electrode material is subjected to heat preservation, the drying process is completed.
Example 2
As still another embodiment of the present specification, unlike example 1, in step S01 of the present example, the mass of the low-temperature activated molecular sieve is 2.0wt% of the high-nickel ternary cathode material.
Comparative example 1
As a comparative example of the present specification, unlike example 1, in step S01 of the present comparative example, the low temperature activated molecular sieve of the examples of the present invention was not added.
Comparative example 2
As still another comparative example in this specification, unlike example 1, in step S01 of this comparative example, a conventional high temperature activated molecular sieve was added, and this comparative example used a UOP molecular sieve whose chemical composition was NaO. SiO2·Al2O3. The mass of the high-temperature activated molecular sieve is 0.5 wt% of the high-nickel ternary cathode material.
Test experiments
Fig. 3 is a schematic diagram of a cycle performance curve of a battery in example 1 of the present invention, fig. 4 is a schematic diagram of a cycle performance curve of a battery in example 2 of the present invention, fig. 5 is a schematic diagram of a cycle performance curve of a battery in comparative example 1 of the present invention, fig. 6 is a schematic diagram of a cycle performance curve of a battery in comparative example 2 of the present invention, and positive electrode materials of lithium ion batteries prepared in example 1, example 2, comparative example 1, and comparative example 2 are respectively assembled into a high nickel lithium ion battery, the high nickel lithium ion battery includes a positive electrode, a negative electrode, a separator disposed between the positive electrode and the negative electrode, and an electrolyte, and the positive electrode of the high nickel lithium ion battery is composed of the above positive electrode material of the high nickel lithium ion battery.
The assembled high nickel lithium ion battery is subjected to charge-discharge cycle under the voltage environment of 2.75V-4.5V at normal temperature, the cycle number is 500 circles, and the battery cycle performance curve diagrams shown in figures 3 to 6 are obtained.
After 500 cycles of continuous charge and discharge, the specific discharge capacity retention rate of the battery made of the battery cathode material in example 1 was 62.37%, and the specific discharge capacity retention rate of the battery made of the battery cathode material in example 2 was 61.27%.
The specific discharge capacity retention rate of the battery made of the battery cathode material which is not modified by the low-temperature activated molecular sieve in the comparative example 1 is 38.29%, and the cycle performance of the battery is obviously reduced compared with the battery made of the battery cathode material which is modified by the low-temperature activated molecular sieve, while the specific discharge capacity retention rate of the battery made of the battery cathode material which is modified by the high-temperature activated molecular sieve in the comparative example 2 is 56%, although the high-temperature activated molecular sieve also maintains a certain specific discharge capacity, compared with the batteries made of the battery cathode material which is modified by the low-temperature activated molecular sieve in the examples 1 and 2, the cycle performance of the battery is relatively poor.
Fig. 7 is a schematic diagram of temperature activation curves of the low-temperature activated molecular sieve of the present invention and a conventional molecular sieve, and as shown in fig. 7, more than 80% of the adsorbed water can be desorbed by the low-temperature activated molecular sieve at 60 ℃. In addition, in the preparation process, the environment temperature is required to reach 200 ℃ for completely dehydrating the high-temperature activated molecular sieve, so that dehydration cannot be completed when the electrode is dried, the high-temperature activated molecular sieve is required to be subjected to dehydration operation independently, and the dehydration temperature of the low-temperature activated molecular sieve is not high, so that dehydration can be completed in the electrode drying process, the electrode manufacturing process is simplified, and the electrode manufacturing time is saved.
In summary, the embodiment of the invention provides a high-nickel lithium ion battery anode material and a preparation method thereof, because the low-temperature activated molecular sieve is added in the high-nickel lithium ion battery anode material, the low-temperature activated molecular sieve can adsorb trace moisture remained in the battery anode material and electrolyte, inhibit the reaction of water and the electrolyte, reduce the generation of hydrogen fluoride and the corrosion of hydrogen fluoride to the battery anode, enhance the interface stability of the battery anode and the electrolyte, and improve the cycle performance.
The foregoing description has been directed to specific embodiments of this disclosure. Other embodiments are within the scope of the following claims. In some cases, the actions or steps recited in the claims may be performed in a different order than in the embodiments and still achieve desirable results. In addition, the processes depicted in the accompanying figures do not necessarily require the particular order shown, or sequential order, to achieve desirable results. In some embodiments, multitasking and parallel processing may also be possible or may be advantageous.
It should be noted that, for those skilled in the art, without departing from the principle of the present application, several improvements and modifications can be made, and these improvements and modifications should also be construed as the protection scope of the present application.
Claims (10)
1. The high-nickel lithium ion battery anode comprises an aluminum foil and an anode membrane arranged on the aluminum foil, and is characterized in that the anode membrane comprises a high-nickel ternary anode material, an adhesive, a conductive agent and a low-temperature activated molecular sieve, the mass of the low-temperature activated molecular sieve is 0.1-2.0 wt% of that of the high-nickel ternary anode material, and the chemical general formula of the low-temperature activated molecular sieve is xRO. ySiO2·zAl2O3·P2O5In the general formula, 0<x≤0.9，0<y is not more than 0.9, z is not less than 0.1 and not more than 1.0, R is one of Cu, Ca or Ba, the low-temperature activated molecular sieve completes dehydration activation in the process of drying the battery anode, and the temperature range of drying is 100-120 ℃.
2. The high-nickel lithium ion battery positive electrode according to claim 1, wherein the mass ratio of the high-nickel ternary positive electrode material to the binder to the conductive agent is 7.0-9.0 parts: 0.5-2.0 parts: 0.5 to 1.0 portion.
3. The high-nickel lithium ion battery positive electrode according to claim 1, wherein the high-nickel ternary positive electrode material is LiNi0.8Co0.15Al0.05O2。
4. The high-nickel lithium ion battery positive electrode according to claim 1, wherein the conductive agent is one of acetylene black, conductive graphite, or ketjen black.
5. The high-nickel lithium ion battery positive electrode according to claim 1, wherein the binder is at least one of polyvinylidene fluoride, polytetrafluoroethylene, and sodium carboxymethylcellulose.
6. The high-nickel lithium ion battery positive electrode according to claim 1, wherein the low-temperature activated molecular sieve has a pore size of 0.3nm to 2nm, and a particle size of 3 μm to 4 μm.
7. A high nickel lithium ion battery, comprising a positive electrode, a negative electrode, a separator arranged between the positive electrode and the negative electrode, and an electrolyte, wherein the positive electrode is the high nickel lithium ion battery positive electrode according to any one of claims 1 to 6.
8. A preparation method of a high-nickel lithium ion battery anode is characterized in that the high-nickel lithium ion battery anode is the high-nickel lithium ion battery anode of any one of claims 1 to 6, and the preparation method of the high-nickel lithium ion battery anode comprises the following steps:
mixing a high-nickel ternary positive electrode material, a conductive agent, a binder and a low-temperature activated molecular sieve to obtain a precursor;
dispersing the precursor in N-methyl pyrrolidone to obtain positive electrode slurry;
and coating the positive electrode slurry on an aluminum foil, and drying the aluminum foil coated with the positive electrode slurry to obtain the battery positive electrode.
9. The method for preparing the high-nickel lithium ion battery positive electrode according to claim 8, wherein the drying environment for drying the aluminum foil coated with the positive electrode slurry is a vacuum environment.
10. The method for preparing the high-nickel lithium ion battery positive electrode according to claim 8, wherein the drying temperature for drying the aluminum foil coated with the positive electrode slurry is 100 ℃ to 120 ℃, and the drying time is 10 to 12 hours.
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| CN110416540A (en) * | 2019-07-26 | 2019-11-05 | 陕西科技大学 | A kind of nickelic tertiary cathode material and preparation method thereof |
| CN110931774B (en) * | 2019-11-21 | 2021-05-14 | 广东邦普循环科技有限公司 | Composite Ni 65-coated nickel-cobalt-manganese ternary cathode material and preparation method and application thereof |
| CN113675400B (en) * | 2020-05-15 | 2023-07-14 | 比亚迪股份有限公司 | Positive electrode, preparation method thereof and lithium ion battery |
| CN113991053B (en) * | 2021-10-27 | 2023-05-05 | 深圳市量能科技有限公司 | Battery positive electrode and lithium ion battery comprising same |
| CN116646610B (en) * | 2023-06-28 | 2024-01-30 | 武汉中科先进材料科技有限公司 | Method for improving long-cycle stability of high-nickel NMC811 ternary lithium ion battery |
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