CN111883771A - Lithium ion battery positive electrode material, positive plate and lithium ion battery - Google Patents
Lithium ion battery positive electrode material, positive plate and lithium ion battery Download PDFInfo
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- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
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Abstract
The invention provides a lithium ion battery anode material, an anode plate and a lithium ion battery, belonging to the technical field of lithium ion batteries, wherein the anode material is prepared from the following raw materials in parts by weight: 50-90 parts of lithium manganese iron phosphate; 5-25 parts of nickel cobalt lithium manganate; 5-25 parts of lithium manganate. According to the lithium ion battery anode material provided by the invention, lithium manganese iron phosphate, lithium nickel cobalt manganese oxide and lithium manganese oxide are selected for scientific compounding, the lithium manganese iron phosphate is used as a main component, the lithium nickel cobalt manganese oxide and the lithium manganese oxide are used as auxiliary components, the particles are deeply compounded through ball milling, and further a double-platform discharging of the lithium manganese iron phosphate is changed into a smooth and gentle curve, and the double-platform discharging lithium manganese iron phosphate is used for preparing a lithium ion battery, so that the lithium battery with high energy density, good safety performance, long cycle life and low cost can be obtained.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a lithium ion battery positive electrode material, a positive plate and a lithium ion battery.
Background
With the continuous improvement of living standard of people, the demand of batteries is continuously increased, and particularly, the demand of reusable lithium ion batteries is gradually increased.
The lithium manganese iron phosphate is a common lithium ion battery anode material, has low cost and environmental protection, belongs to an olivine crystal form as lithium iron phosphate, has the same theoretical capacity and excellent safety performance, has the same theoretical capacity (170mAh/g) as lithium iron phosphate, has double discharge platforms (3.85V and 3.35V) relative to a graphite cathode, has potential high energy density due to 4.0V high potential, but has a pressure difference of nearly 0.5V on the double platforms, causes huge impact on electrical equipment due to higher pressure difference, and greatly limits the industrial application of the lithium manganese iron phosphate.
For example, CN106129365A discloses a high-safety lithium iron manganese phosphate battery, which mainly uses lithium nickel cobalt manganese oxide as a main material and uses lithium iron manganese phosphate as an auxiliary material, and improves and enhances the thermal stability of the lithium nickel cobalt manganese oxide material by simple mechanical and physical mixing, thereby enhancing the safety performance of the lithium nickel cobalt manganese oxide. However, the invention only uses lithium manganese iron phosphate as an auxiliary material, and cannot realize the batch industrialization of the lithium manganese iron phosphate.
CN105449269A discloses a lithium ion battery, which mixes lithium iron phosphate, lithium nickel cobalt manganese oxide and lithium manganese iron phosphate together, and improves the cycle performance, energy density and safety performance of the battery. However, the invention still uses lithium manganese iron phosphate as an auxiliary material, the voltage platforms of the lithium nickel cobalt manganese oxide and the lithium manganese iron phosphate are both higher than 3.6V, the discharge platform of the lithium iron phosphate is only 3.2V, the voltage platforms of the three materials are not well matched, and the battery cannot fully exert the best performance.
Disclosure of Invention
The invention provides a lithium ion battery anode material, an anode plate and a lithium ion battery, and aims to solve the technical problems.
The invention provides a lithium ion battery anode material which is prepared from the following raw materials in parts by weight:
50-90 parts of lithium manganese iron phosphate; 5-25 parts of nickel cobalt lithium manganate; 5-25 parts of lithium manganate;
wherein the total amount of the lithium iron manganese phosphate, the lithium nickel cobalt manganese oxide and the lithium manganese oxide is 100 parts.
Further, the D50 of the lithium manganese iron phosphate is 0.7-1.5 mu m; d50 of the nickel cobalt lithium manganate is 8.0-15.0 mu m; the D50 of the lithium manganate is 8.0-15.0 mu m.
Further, the lithium manganese iron phosphate is LiMnxFe(1-x)PO4Wherein x is more than or equal to 0.5 and less than or equal to 0.8;
the nickel cobalt lithium manganate is LiNixMnyCo(1-x-y)O2Wherein x is more than 0 and less than 1, y is more than 0 and less than 1, and 0 is more than 1-x-y and less than 1;
the lithium manganate is LiMn2O4。
The invention also provides a preparation method of the lithium ion battery anode material, which comprises the following steps: and mixing the raw materials of lithium manganese iron phosphate, lithium nickel cobalt manganese oxide and lithium manganate, placing the mixture in a ball milling tank, adding zirconium balls, and then carrying out ball milling to obtain the anode material.
Further, the diameter of the zirconium balls is 10-20 mm, and the mass ratio of the balls to the materials is 2: 1-4: 1; the ball milling time is 20-40 min.
The invention also provides a positive plate, which comprises a current collector and a positive active material layer coated on the current collector, wherein the positive active material layer comprises any one of the positive materials.
The invention also provides a lithium ion battery, comprising: the positive plate is the positive plate or comprises any one of the positive materials.
Furthermore, the diaphragm is made of polyethylene, polypropylene or polypropylene-polyethylene-polypropylene three-layer composite diaphragm.
The invention has the following advantages:
(1) according to the lithium ion battery anode material provided by the invention, lithium manganese iron phosphate, lithium nickel cobalt manganese oxide and lithium manganese oxide are selected for scientific compounding, the lithium manganese iron phosphate is used as a main component, the lithium nickel cobalt manganese oxide and the lithium manganese oxide are used as auxiliary components, and the particles are deeply compounded through ball milling, so that the discharging double platform of the lithium manganese iron phosphate is changed into a smooth and stable curve, and the lithium manganese iron phosphate is used for preparing a lithium ion battery, so that the lithium battery with high energy density, good safety performance, long cycle life and low cost can be obtained.
(2) According to the invention, the particle size D50 of lithium manganese iron phosphate is 0.7-1.5 μm, the particle sizes D50 of lithium nickel cobalt manganese oxide and lithium manganese oxide are 8-15 μm, and the olivine crystal lithium manganese iron phosphate with small particle size can be filled into gaps between the layered lithium nickel cobalt manganese oxide with large particle size and the spinel crystal lithium manganese oxide, so that the energy density, the safety performance and the cycle life of the battery are improved on the premise of solving the double-platform problem of lithium manganese iron phosphate discharge.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this specification, illustrate an embodiment of the invention and, together with the description, serve to explain the invention and not to limit the invention.
In the drawings:
FIG. 1 is a Scanning Electron Microscope (SEM) image of a composite material obtained in example 1 of the present invention;
FIG. 2 is a Transmission Electron Microscope (TEM) image of a composite material obtained in example 1 of the present invention;
FIG. 3 is a graph showing the discharge curves of example 3 of the present invention, comparative examples 3 and 4;
fig. 4 is a cycle curve of the battery of example 3 of the present invention.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the embodiments of the present invention and the accompanying drawings, 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. The embodiments and features of the embodiments of the present invention may be combined with each other without conflict.
In the prior art, the main component of the commonly used lithium ion battery anode material is nickel cobalt lithium manganate which has high energy density, but poor safety performance and high price. The other common positive electrode material component lithium manganese iron phosphate is low in cost and environment-friendly, has the same theoretical capacity and excellent safety performance as lithium iron phosphate, but can only be used as an auxiliary component and matched with lithium nickel cobalt manganese oxide due to the existence of a discharging double platform (the pressure difference of the double platform is nearly 0.5V), so that the application of the lithium manganese iron phosphate is severely limited.
According to the lithium ion battery anode material provided by the embodiment of the invention, the self performance and the discharge platform of different anode materials are comprehensively considered, lithium manganese iron phosphate (the discharge platforms are 3.85V and 3.35V), lithium nickel cobalt manganese (the discharge platform is 3.65V) and lithium manganese (the discharge platform is 3.85V) are selected for scientific compounding, the lithium manganese iron phosphate is used as a main component, the lithium nickel cobalt manganese and the lithium manganese are used as auxiliary components, the platform pressure difference and the electrical performance of each component are comprehensively considered, and finally the obtained anode material can effectively solve the problem of double platforms.
Specifically, an embodiment of the invention provides a lithium ion battery cathode material, which is prepared from the following raw materials in parts by weight:
50-90 parts of lithium manganese iron phosphate; 5-25 parts of nickel cobalt lithium manganate; 5-25 parts of lithium manganate;
wherein the total amount of the lithium iron manganese phosphate, the lithium nickel cobalt manganese oxide and the lithium manganese oxide is 100 parts.
In one embodiment of the invention, D50 of the lithium manganese iron phosphate is 0.7-1.5 μm; d50 of the nickel cobalt lithium manganate is 8.0-15.0 mu m; the D50 of the lithium manganate is 8.0-15.0 mu m.
In an embodiment of the invention, the lithium iron manganese phosphate is LiMnxFe(1-x)PO4Wherein x is more than or equal to 0.5 and less than or equal to 0.8.
The nickel cobalt lithium manganate is LiNixMnyCo(1-x-y)O2Wherein 0 < xLess than 1, y is more than 0 and less than 1, and 0 is more than 1-x-y and less than 1; specifically, it may be NCM111, NCM523, NCM622, and NCM 811.
The lithium manganate is LiMn2O4。
Another embodiment of the present invention provides a method for preparing a lithium ion battery positive electrode material, including: and mixing the raw materials of lithium manganese iron phosphate, lithium nickel cobalt manganese oxide and lithium manganate, placing the mixture in a ball milling tank, adding zirconium balls, and then carrying out ball milling to obtain the anode material.
Specifically, the diameter of the zirconium ball is 10-20 mm. The mass ratio of the ball material is 2: 1-4: 1. The ball milling time is 20-40 min. Preferably, the diameter of the zirconium balls is 15 mm. The mass ratio of the ball material is 2: 1. The ball milling time is 30 min.
The embodiment of the invention also provides a positive plate, which comprises a current collector and a positive active material layer coated on the current collector, wherein the positive active material layer comprises the positive material.
Specifically, the positive active material layer comprises the following raw materials in parts by weight:
92-96 parts of a positive electrode material;
2-4 parts of a positive electrode conductive agent;
2-4 parts of a positive electrode binder;
preferably;
the positive conductive agent is at least one of conductive carbon black, conductive graphite, carbon nano tubes or graphene;
the positive electrode adhesive is at least one of Suwei PVDF 5130 and Achima PVDF 900.
An embodiment of the present invention further provides a lithium ion battery, including: the positive plate is any one of the positive plates or comprises any one of the positive materials.
Preferably, the negative electrode sheet comprises a current collector and a negative active material layer coated on the current collector, wherein the negative active material layer is composed of the following raw materials in parts by weight:
94-96 parts of a negative electrode material;
1-2 parts of a negative electrode conductive agent;
3-4 parts of a negative electrode binder.
More preferably, the negative electrode material is artificial graphite or natural graphite;
the negative adhesive is at least one of styrene butadiene rubber or sodium carboxymethylcellulose;
furthermore, the diaphragm is made of polyethylene, polypropylene or polypropylene-polyethylene-polypropylene three-layer composite diaphragm.
The present invention will be described in detail with reference to examples.
Example 1Lithium ion battery anode material and preparation method thereof
The positive electrode material includes:
the mass fraction of the lithium manganese iron phosphate is 70 parts, wherein LiMn is adopted as the lithium manganese iron phosphate0.6Fe0.4PO4；
The lithium nickel cobalt manganese oxide is 20 parts by mass, wherein the lithium nickel cobalt manganese oxide adopts LiNi0.5Mn0.3Co0.2O2；
The mass portion of the lithium manganate is 10 portions.
Mixing the three materials, placing the mixture into a 2L ball milling tank made of polyurethane, adding zirconium balls with the diameter of 15mm, wherein the ball-material ratio is 2:1, placing the ball milling tank into a ball mill, adjusting the frequency to be 30HZ, and performing ball milling for 30min to obtain the composite lithium iron manganese phosphate material for later use.
The scanning electron microscope topography is shown in figure 1, and the transmission electron microscope topography is shown in figure 2.
Example 2Lithium ion battery anode material and preparation method thereof
The positive electrode material includes:
the mass fraction of the lithium manganese iron phosphate is 80 parts, wherein the lithium manganese iron phosphate adopts LiMn0.6Fe0.4PO4；
The mass portion of the nickel cobalt lithium manganate is 10 portions, wherein the nickel cobalt lithium manganate adopts LiNi0.5Mn0.3Co0.2O2；
The mass portion of the lithium manganate is 10 portions.
Mixing the three materials, placing the mixture into a 2L ball milling tank made of polyurethane, adding zirconium balls with the diameter of 15mm, wherein the ball-material ratio is 2:1, placing the ball milling tank into a ball mill, adjusting the frequency to be 30HZ, and performing ball milling for 30min to obtain the composite lithium iron manganese phosphate material for later use.
Example 3Lithium ion battery
The lithium ion battery includes: the positive plate, the negative plate, the diaphragm and the electrolyte;
the positive plate comprises a current collector and a positive active material layer coated on the current collector; the positive active material layer comprises the following raw materials in parts by weight: 95 parts of the cathode material obtained in example 1; 3 parts of a positive electrode conductive agent; 2 parts of positive electrode binder (Suwei PVDF 5130);
the negative plate comprises a current collector and a negative active material layer coated on the current collector, wherein the negative active material layer comprises the following raw materials in parts by weight: 95 parts of a negative electrode material (artificial graphite); 1 part of negative electrode conductive agent; 4 parts of a negative electrode binder (styrene butadiene rubber).
The diaphragm is made of polyethylene.
Example 4Lithium ion battery
The difference from example 3 is that the positive electrode material obtained in example 2 was used.
Comparative example 1Lithium ion battery anode material and preparation method thereof
The difference from example 1 is that the positive electrode material only includes lithium manganese iron phosphate, that is, the mass fraction of lithium manganese iron phosphate is 100 parts.
Comparative example 2Lithium ion battery anode material and preparation method thereof
The difference from example 1 is that lithium iron phosphate (with a discharge plateau of 3.2V) is used as the positive electrode material to replace lithium nickel cobalt manganese oxide, i.e., lithium manganese iron phosphate (with LiMn as lithium manganese iron phosphate)0.6Fe0.4PO4) 70 parts of lithium iron phosphate, 20 parts of lithium manganate and 10 parts of lithium manganate.
Comparative example 3Lithium ion battery
The difference from example 3 was that the positive electrode material obtained in comparative example 1 was used.
Comparative example 4Lithium ion battery
The difference from example 4 was that the positive electrode material obtained in comparative example 2 was used.
Test example 1
The electric properties of the full cells obtained in the above examples 3 to 4 and comparative examples 3 to 4 were measured, and the results are shown in table 1.
TABLE 1
As can be seen from fig. 3, the discharge curves of comparative example 3 and comparative example 4 are clearly double-plateau curves, while the discharge curve of example 3 becomes smooth and gentle with respect to the pure lithium manganese iron phosphate of comparative example 3, and there is no clear double-plateau curve. Therefore, the three components are combined, so that the problem of double discharge platforms can be solved, and the electrical property test and the compaction density are excellent. If only the lithium iron manganese phosphate is compounded with one of lithium nickel cobalt manganese oxide or lithium manganese oxide, the comprehensive performance of the lithium iron manganese oxide is influenced certainly because lithium nickel cobalt manganese oxide or lithium manganese oxide has certain limitations (for example, lithium nickel cobalt manganese oxide has high cost and extremely poor safety performance, lithium manganese oxide has poor cycle performance and low capacity).
In addition, as can be seen from table 1, after the three cathode materials of examples 3 and 4 are compounded by a ball milling process according to a certain proportion, the compaction densities of the materials are greatly improved, and the compaction of example 3 can reach 3.2g/cm3. As can also be seen from fig. 1 and 2, the lithium iron manganese phosphate with a small particle size is coated and filled in the ternary lithium manganese oxide and the lithium manganese oxide with a large particle size, and the composite material has a higher volume energy density due to the appropriate particle composition and ball milling composite process.
In addition, the 0.2C discharge specific capacity of the material in the embodiment 3 is 152.1mAh/g, the median voltage is 3.6864V, and the specific capacity of the material is higher than the theoretical specific capacity compounded according to the proportion. Because the three materials are deeply compounded by ball milling, the contact nodes among the particles are more compact and uniform, Mn in the microcosmically compounded materials has +2, +3 and +4 valence states, the materials have a better discharge platform curve and higher energy density due to the synergistic effect of the composite materials, the capacity retention rate of the battery 1C in the cycle of 2000 cycles of the embodiment 3 is 86.8%, and the cycle performance is far better than that of nickel cobalt lithium manganate and lithium manganate (figure 4).
The present invention is not limited to the above preferred embodiments, and any modifications, equivalent substitutions, improvements, etc. within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (8)
1. A lithium ion battery anode material is characterized in that,
the compound is prepared from the following raw materials in parts by weight:
50-90 parts of lithium manganese iron phosphate; 5-25 parts of nickel cobalt lithium manganate; 5-25 parts of lithium manganate;
wherein the total amount of the lithium iron manganese phosphate, the lithium nickel cobalt manganese oxide and the lithium manganese oxide is 100 parts.
2. The positive electrode material according to claim 1,
d50 of the lithium manganese iron phosphate is 0.7-1.5 mu m; d50 of the nickel cobalt lithium manganate is 8.0-15.0 mu m; the D50 of the lithium manganate is 8.0-15.0 mu m.
3. The positive electrode material according to claim 1,
the lithium iron manganese phosphate is LiMnxFe(1-x)PO4Wherein x is more than or equal to 0.5 and less than or equal to 0.8;
the nickel cobalt lithium manganate is LiNixMnyCo(1-x-y)O2Wherein x is more than 0 and less than 1, y is more than 0 and less than 1, and 0 is more than 1-x-y and less than 1;
the lithium manganate is LiMn2O4。
4. A preparation method of the lithium ion battery cathode material as claimed in any one of claims 1 to 3, comprising the following steps: and mixing the raw materials of lithium manganese iron phosphate, lithium nickel cobalt manganese oxide and lithium manganate, placing the mixture in a ball milling tank, adding zirconium balls, and then carrying out ball milling compounding to obtain the cathode material.
5. The production method according to claim 4,
the diameter of the zirconium ball is 10-20 mm; the mass ratio of the ball materials is 2: 1-4: 1; the ball milling time is 20-40 min.
6. A positive electrode sheet comprising a current collector and a positive electrode active material layer coated on the current collector, wherein the positive electrode active material layer comprises the positive electrode material according to any one of claims 1 to 3.
7. A lithium ion battery comprising: the positive plate, the negative plate, the diaphragm and the electrolyte are characterized in that the positive plate is the positive plate in claim 6 or comprises the positive electrode material in any one of claims 1 to 3.
8. The lithium ion battery according to claim 7,
the diaphragm is made of polyethylene, polypropylene or polypropylene-polyethylene-polypropylene three-layer composite diaphragm.
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| CN112885996A (en) * | 2021-04-13 | 2021-06-01 | 江苏力泰锂能科技有限公司 | Positive electrode active material, preparation method thereof, positive electrode and lithium ion battery |
| CN113054157A (en) * | 2021-03-15 | 2021-06-29 | 星恒电源股份有限公司 | Double-composite modified spinel lithium manganate positive plate, preparation method thereof and lithium ion battery |
| CN113224277A (en) * | 2021-05-03 | 2021-08-06 | 星恒电源股份有限公司 | High-safety long-cycle-life positive pole piece for lithium ion battery |
| WO2022100626A1 (en) * | 2020-11-11 | 2022-05-19 | 比亚迪股份有限公司 | Lithium-ion battery |
| WO2022199681A1 (en) * | 2021-03-25 | 2022-09-29 | 比亚迪股份有限公司 | Lithium-ion battery and motorized vehicle |
| CN115832224A (en) * | 2023-01-05 | 2023-03-21 | 厦门海辰储能科技股份有限公司 | Positive plate and preparation method thereof, electrode assembly, energy storage device and electric device |
| CN116706030A (en) * | 2023-07-10 | 2023-09-05 | 安徽得壹能源科技有限公司 | Composite positive electrode material, electrode system and battery |
| CN116759560A (en) * | 2023-08-14 | 2023-09-15 | 中创新航科技集团股份有限公司 | Lithium iron manganese phosphate battery |
| EP4089767A4 (en) * | 2021-03-25 | 2023-11-29 | Contemporary Amperex Technology Co., Limited | Lithium manganate positive electrode active material and positive pole piece containing same, secondary battery, battery module, battery pack and powered device |
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| WO2022100626A1 (en) * | 2020-11-11 | 2022-05-19 | 比亚迪股份有限公司 | Lithium-ion battery |
| CN113054157A (en) * | 2021-03-15 | 2021-06-29 | 星恒电源股份有限公司 | Double-composite modified spinel lithium manganate positive plate, preparation method thereof and lithium ion battery |
| EP4089767A4 (en) * | 2021-03-25 | 2023-11-29 | Contemporary Amperex Technology Co., Limited | Lithium manganate positive electrode active material and positive pole piece containing same, secondary battery, battery module, battery pack and powered device |
| US12021232B2 (en) | 2021-03-25 | 2024-06-25 | Contemporary Amperex Technology Co., Limited | Lithium manganate positive electrode active material as well as positive electrode sheet, secondary battery, battery module, battery pack and powered device comprising the same |
| WO2022199681A1 (en) * | 2021-03-25 | 2022-09-29 | 比亚迪股份有限公司 | Lithium-ion battery and motorized vehicle |
| CN112885996A (en) * | 2021-04-13 | 2021-06-01 | 江苏力泰锂能科技有限公司 | Positive electrode active material, preparation method thereof, positive electrode and lithium ion battery |
| CN112885996B (en) * | 2021-04-13 | 2022-07-12 | 江苏力泰锂能科技有限公司 | Positive electrode active material, preparation method thereof, positive electrode and lithium ion battery |
| CN113224277B (en) * | 2021-05-03 | 2022-04-01 | 星恒电源股份有限公司 | High-safety long-cycle-life positive pole piece for lithium ion battery |
| CN113224277A (en) * | 2021-05-03 | 2021-08-06 | 星恒电源股份有限公司 | High-safety long-cycle-life positive pole piece for lithium ion battery |
| CN115832224A (en) * | 2023-01-05 | 2023-03-21 | 厦门海辰储能科技股份有限公司 | Positive plate and preparation method thereof, electrode assembly, energy storage device and electric device |
| CN115832224B (en) * | 2023-01-05 | 2023-12-22 | 厦门海辰储能科技股份有限公司 | Positive plate and preparation method thereof, electrode assembly, energy storage device and electric equipment |
| CN116706030A (en) * | 2023-07-10 | 2023-09-05 | 安徽得壹能源科技有限公司 | Composite positive electrode material, electrode system and battery |
| CN116759560A (en) * | 2023-08-14 | 2023-09-15 | 中创新航科技集团股份有限公司 | Lithium iron manganese phosphate battery |
| CN116759560B (en) * | 2023-08-14 | 2023-11-10 | 中创新航科技集团股份有限公司 | Lithium iron manganese phosphate battery |
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| Publication number | Publication date |
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| CN111883771B (en) | 2023-03-31 |
| CN116111085A (en) | 2023-05-12 |
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