CN107994207B - Lithium ion battery and cathode plate thereof - Google Patents
Lithium ion battery and cathode plate thereof Download PDFInfo
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- CN107994207B CN107994207B CN201610942995.2A CN201610942995A CN107994207B CN 107994207 B CN107994207 B CN 107994207B CN 201610942995 A CN201610942995 A CN 201610942995A CN 107994207 B CN107994207 B CN 107994207B
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- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
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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
- H01M10/052—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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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention discloses a lithium ion battery cathode plate, which comprises a cathode current collector, an active material layer arranged on the cathode current collector, and a barrier layer arranged on the active material layer, wherein the barrier layer comprises a porous carbon material, a binder and a conductive agent, the aperture of the porous carbon material is 2-50 nm, and the specific surface area is 500-2000 m-2Per g, pore volume of 1.00-2.25cm3(ii) in terms of/g. The cathode plate of the lithium ion battery can not only obviously reduce the deposition of transition metal on the anode, but also can not influence the discharge capacity of the lithium ion battery at high and low temperatures, can obviously improve the cycle performance of the lithium ion battery and prolong the cycle life of the battery.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a lithium ion battery and a cathode plate thereof.
Background
In recent years, lithium ion batteries have been rapidly developed and the demand for such batteries has been increasing. Lithium ion batteries generally need to meet the following characteristics: (1) high energy and high power density (where HEV hybrid vehicles have higher power requirements and energy storage batteries have lower power requirements); (2) the working temperature range is wide, and the environmental suitability is strong; (3) long cycle life and service life; (4) outstanding safety and reliability.
For lithium ion batteries containing transition metals, the conductive salt L iPF in the electrolyte is present during cycling6Decomposition occurs to form L iF and PF5，PF5The electrolyte can generate hydrolysis reaction with residual trace water in the electrolyte to generate HF, and the HF is influenced by acidic gas and self structural stability, and the transition metal in the cathode material is easily dissolved into the electrolyte, diffuses to the anode along with circulation and catalyzes the decomposition of an SEI film on the surface of an anode plate to influence the stability of the SEI film, accelerate the consumption of active lithium, and simultaneously initiate other side reactions, thereby accelerating the capacity attenuation of the battery.
For example, in the case of a lithium ion battery containing a transition metal Mn, the valence state of Mn changes from +3 to +4 during charge and discharge, the Jahn-Teller effect is easily generated, lattice distortion occurs and volume contraction or expansion is caused, so that the structure becomes unstable and collapses. At high temperatures, in particular in high-voltage systems, in electrolytesTraces of HF cause Mn2+The dissolution of the compound causes the destruction of a spinel structure, greatly accelerates the attenuation of the battery capacity, and has the chemical reaction formula of 4HF + 2L iMn2O4→3γ-MnO2+MnF2+2LiF+2H2O。
The literature reports that the deposition of metal Mn on the surface of an anode can influence the insertion and extraction of L i, more Mn can be detected on the surface of an anode material along with the circulation, and the Mn reacts with SEI on the anode to destroy the stability of an SEI film, increase the impedance of the anode and accelerate the capacity loss of a lithium ion battery.
Therefore, in the circulation process of the existing lithium ion batteries such as NCM (nickel cobalt lithium manganate ternary material), NCA (nickel cobalt lithium aluminate ternary material), lithium manganate, lithium iron phosphate, lithium-rich manganese-based material and the like, some side reactions occur on the surface of the anode material continuously, some acid gases are generated and diffused to the cathode, and some transition metals are dissolved. In addition, during continuous charge and discharge, the structural stability of the cathode material is deteriorated, and a part of the transition metal is also dissolved out. The dissolved transition metal diffuses to the surface of the anode material, the stability of an SEI film is damaged, the consumption of active lithium is increased, the capacity attenuation of the lithium ion battery is accelerated, and finally the cycle life of the battery is reduced.
In order to solve the problems, currently adopted measures are that a porous carbon material with adsorbability is directly mixed in an active material layer to serve as a conductive agent, but the porous carbon material has extremely strong liquid absorption capacity, and the addition of the porous carbon material can reduce the binding force between an active material and a current collector, so that the power performance and the safety performance of the lithium ion battery are deteriorated.
In view of the above, there is a need for a cathode sheet of a lithium ion battery, which can reduce the deposition of transition metals on the anode and improve the cycle performance of the battery.
Disclosure of Invention
The invention aims to: provided are a lithium ion battery and a cathode sheet thereof, which can not only reduce deposition of transition metals on an anode, but also significantly improve cycle performance of the battery.
To is coming toThe invention realizes the aim, and provides a lithium ion battery cathode sheet, which comprises a cathode current collector, an active material layer arranged on the cathode current collector, and a barrier layer arranged on the active material layer, wherein the barrier layer comprises a porous carbon material, a binder and a conductive agent, the pore diameter of the porous carbon material is 2 nm-50 nm, and the specific surface area is 500-2000 m-2Per g, pore volume of 1.00-2.25cm3/g。
The barrier layer containing the porous carbon material is arranged outside the active substance layer, and the porous carbon material has excellent adsorption performance and also has good conductivity, chemical inertia and corrosion resistance, so that the abundant pore structure of the porous carbon material can be used for adsorbing the transition metal dissolved from the cathode material, and the dissolved transition metal is restrained at the cathode to prevent the transition metal from diffusing to the surface of the anode; in addition, the porous material has a large specific surface area, and can store a large amount of electrolyte, so that the cycle life of the battery can be prolonged.
As an improvement of the cathode plate of the lithium ion battery, the pore diameter of the porous carbon material is 15-50nm, and the specific surface area is 820-2000m2Per g, pore volume of 1.42-2.25cm3/g。
As an improvement of the cathode sheet of the lithium ion battery, the porous carbon material is one or more of activated carbon, carbon nano tubes, mesoporous carbon or carbide derived carbon.
As an improvement of the cathode plate of the lithium ion battery, the thickness of the barrier layer is 2-25 μm.
As an improvement of the cathode plate of the lithium ion battery, the thickness of the barrier layer is 15-25 μm.
As an improvement of the cathode plate of the lithium ion battery, the barrier layer comprises the following components in percentage by mass: 40-90% of a porous carbon material, 5-40% of a binder and 5-55% of a conductive agent.
As an improvement of the cathode sheet of the lithium ion battery, the conductive agent in the barrier layer is one or more of conductive carbon black SP, conductive graphite, SP-L i, ketjen black, carbon fiber and graphene.
As an improvement of the cathode sheet of the lithium ion battery, the binder in the barrier layer is one or more of polyvinylidene fluoride, sodium carboxymethylcellulose, sodium alginate, polyvinyl alcohol, polytetrafluoroethylene, polyurethane, polyacrylic acid and acrylic acid-acrylamide copolymer.
As an improvement of the cathode sheet of the lithium ion battery, the active material contained in the active material layer is one or more of nickel cobalt lithium manganate, nickel cobalt lithium aluminate, lithium manganate, lithium iron phosphate and lithium-rich manganese-based materials.
In order to achieve the above object, the present invention further provides a lithium ion battery, which includes a cathode sheet, an anode sheet, a separator arranged between the cathode sheet and the anode sheet, and an electrolyte, wherein the cathode sheet is the above-mentioned lithium ion battery cathode sheet.
Compared with the prior art, the cathode plate of the lithium ion battery has the following beneficial technical effects:
the barrier layer containing the porous carbon material is arranged outside the active substance layer, and the abundant pore structure of the porous carbon material is utilized, so that the deposition of transition metal on the anode can be obviously reduced, the discharge capacity of the lithium ion battery at high and low temperatures can not be influenced, the cycle performance of the lithium ion battery can be obviously improved, and the cycle life of the battery can be prolonged.
Drawings
The cathode sheet of the lithium ion battery of the present invention is described in detail below with reference to the accompanying drawings and specific embodiments, wherein:
fig. 1 is a graph comparing the discharge capacities of the lithium ion batteries of example 1 and comparative example at different temperatures.
Fig. 2 is a graph comparing the cycle performance of the lithium ion batteries of example 1 of the present invention and the comparative example.
Detailed Description
In order to make the objects, technical solutions and technical effects of the present invention more clear, the present invention will be further described in detail with reference to the accompanying drawings and the detailed description. It should be understood that the detailed description and specific examples, while indicating the preferred embodiment of the invention, are intended for purposes of illustration only and are not intended to limit the scope of the invention.
The invention provides a lithium ion battery cathode sheet, which comprises a cathode current collector, an active material layer arranged on the cathode current collector, and a barrier layer arranged on the active material layer, wherein the barrier layer comprises a porous carbon material, a binder and a conductive agent, the pore diameter of the porous carbon material is 2-50 nm, and the specific surface area is 500-2000 m-2Per g, pore volume of 1.00-2.25cm3/g。
The porous carbon material can be any one or more of activated carbon, carbon nano-tubes, mesoporous carbon or carbide derived carbon, and the materials can achieve the aim of the invention.
The thickness of the barrier layer is 2-25 μm. If the thickness of the barrier layer is within a certain range, the mass percentage of the porous carbon material is within a proper range, so that the strong adsorption capacity on transition metal ions is ensured, the content of the transition metal deposited by the corresponding anode is low, and the capacity of the battery cannot be attenuated too fast; too thin or too thick a barrier layer may result in a decrease in the capacity of the battery, and may not achieve the desired effect.
The barrier layer comprises the following components in percentage by mass: 40-90% of a porous carbon material, 5-40% of a binder and 5-55% of a conductive agent. Because the proportion of the binder contained in the barrier layer is higher, after the hot pressing process, the binding power between the barrier layer and the active material layer and between the barrier layer and the isolation film can be increased, the good adhesion and the non-falling of the barrier layer and the active material layer in the circulation and storage processes of the battery cell are ensured, the good interface between the cathode sheet and the isolation film is realized, and the circulation and storage performance of the battery is improved.
The conductive agent in the barrier layer can be one or more selected from conductive carbon black SP, conductive graphite, SP-L i, guichen black, carbon fiber and graphene.
The binder in the barrier layer can be one or more selected from polyvinylidene fluoride, sodium carboxymethylcellulose, sodium alginate, polyvinyl alcohol, polytetrafluoroethylene, polyurethane, polyacrylic acid and acrylic acid-acrylamide copolymer.
The active material contained in the active material layer can be one or more of nickel cobalt lithium manganate, nickel cobalt lithium aluminate, lithium manganate, lithium iron phosphate and lithium-rich manganese-based materials.
Examples
Example 1:
1) preparation of cathode sheet
① preparation of active substance layer
Dissolving polyvinylidene fluoride (PVDF) in N-methylpyrrolidone (NMP) solvent according to a certain proportion, fully stirring to obtain a polyvinylidene fluoride polymer solution, and adding an active substance nickel-cobalt-manganese ternary material L iNi according to a formula comprising an active substance, a binder and a conductive agent in a mass ratio of 95:2:30.5Co0.2Mn0.3O2PVDF as a binder and SP (conductive carbon black SP) as a conductive agent, and finally vacuumizing to remove bubbles; filtering with a 150-mesh stainless steel screen to obtain the required cathode slurry; the obtained cathode slurry was uniformly coated on a cathode current collector, and then dried at 85 ℃ to form an active material layer having a thickness of 115 μm.
Wherein the active substance can be selected from nickel-cobalt-manganese ternary material L iNi0.5Co0.2Mn0.3O2In addition, lithium nickel cobalt manganese oxide ternary materials, lithium nickel cobalt aluminum oxide ternary materials, lithium manganese oxide, lithium iron phosphate and lithium-rich manganese-based materials with different transition metal element contents can be selected.
② preparation of Barrier layer
The porous carbon material has the selected average pore diameter of 20nm and the specific surface area of 1020m2Per g, pore volume 1.62cm3The conductive carbon comprises active carbon per gram, polyvinylidene fluoride (PVDF) as a binder and conductive carbon black SP as a conductive agent; adding activated carbon into an NMP (N-methylpyrrolidone) solution, stirring for 4-12h, then adding SP, stirring for 4-12h, and finally adding PVDF into the solution to form slurry, wherein the mass ratio of the activated carbon to the PVDF to the SP is 80: 10: 10; the slurry was applied to an active material layer to form a barrier layer having a thickness of 3 μm. And drying to obtain the cathode sheet.
2) Preparation of Anode sheets
Styrene Butadiene Rubber (SBR) is dissolved in water solution, the mixture is fully stirred to form SBR water solution, then a certain amount of artificial graphite, SP and sodium carboxymethylcellulose (CMC) are added into the SBR water solution, the weight ratio of the artificial graphite to the CMC to the SBR is 96:1:1:2, the mixture is evenly stirred and coated on copper foil with the thickness of 8 mu m, and the copper foil is dried at the temperature of 110 ℃. And (4) carrying out cold pressing and cutting on the dried pole piece to obtain the anode piece.
3) Diaphragm
The separator used was a polypropylene (PP)/Polyethylene (PE)/polypropylene (PP) three-layer composite porous film having a thickness of 12 μm.
4) Preparation of the electrolyte
Uniformly mixing equal volume of Ethylene Carbonate (EC), Ethyl Methyl Carbonate (EMC) and diethyl carbonate (DEC) to obtain a mixed solvent, and adding lithium hexafluorophosphate (L iPF)6) Wherein L iPF6Has a concentration of 1 mol/L.
5) Battery fabrication
And forming the cathode sheet, the anode sheet and the diaphragm into a battery core through a winding or lamination process, then placing the battery core into a packaging bag, injecting electrolyte, and then forming, packaging and the like to assemble the battery.
Example 2:
example 2 is essentially the same as example 1, except that: the porous carbon material is mesoporous carbon with average pore diameter of 2nm and specific surface area of 500m2G, pore volume 1.00cm3/g。
Example 3:
example 3 is essentially the same as example 1, except that: the average pore diameter of the activated carbon is 50nm, and the specific surface area is 2000m2G, pore volume 2.25cm3/g。
Example 4:
example 4 is essentially the same as example 1, except that: the thickness of the barrier layer was 15 μm, and the average pore diameter of the activated carbon was 15nm and the specific surface area was 820m2G, pore volume 1.42cm3/g。
Example 5:
example 5 is essentially the same as example 1, except that: the thickness of the barrier layer was 25 μm, and the average pore diameter of the activated carbon was 30nm and the specific surface area was 1350m2G, pore volume 1.82cm3/g。
Example 6:
example 6 is essentially the same as example 1, except that: the mass ratio of the activated carbon to the PVDF to the SP in the barrier layer is 90: 5: 5.
comparative example:
the comparative example is substantially the same as example 1 except that: and (5) preparing the cathode sheet.
The preparation method of the cathode sheet comprises the steps of dissolving polyvinylidene fluoride (PVDF) in an N-methyl pyrrolidone (NMP) solvent according to a certain proportion, fully stirring to obtain a polyvinylidene fluoride polymer solution, and adding an active substance nickel-cobalt-manganese ternary material L iNi according to a formula comprising the active substance, a binder and a conductive agent in a mass ratio of 95:2:30.5Co0.2Mn0.3O2PVDF as a binder and SP as a conductive agent, and finally vacuumizing to remove bubbles; filtering with a 150-mesh stainless steel screen to obtain the required cathode slurry; the obtained cathode slurry was uniformly coated on a current collector to a thickness of 115 μm, and then dried at 85 ℃. And (4) carrying out cold pressing and cutting on the dried pole piece to prepare the cathode piece.
Performance testing
The following tests were performed on the examples 1-6 and comparative cells:
1) discharge capacity test at different temperatures
The test temperature was: -40 ℃, 0 ℃, 10 ℃, 25 ℃, 45 ℃, 55 ℃; the charging rate is 1C, the discharging rate is 1C, the charging and discharging interval is 2.8V-4.2V, and the discharging capacity of the battery at the temperature is tested.
2) Cycle performance test at Normal temperature
Testing the capacity retention rate of the battery after 1000 cycles at 25 ℃, wherein the charging step comprises the steps of firstly carrying out constant current charging to 4.20V at a charging rate of 2C, and then carrying out constant voltage charging until the current is reduced to 0.05C; the discharging step is to discharge the mixture to 2.8V at constant current with the discharge rate of 3C.
3) Mass percent test of transition metals in anode sheets
After the battery is subjected to 1000 cycles at normal temperature, the battery is disassembled, and the mass percentage of the transition metal in the anode sheet after the cycle is tested by adopting an inductively coupled plasma mass spectrometer (ICP) method. Table 1 is a comparison of mass percent transition metal in anode sheets after cycling for examples 1-6 and comparative batteries.
As can be seen from the test results in Table 1, the room temperature capacity of the batteries of examples 1-6 is not significantly different from that of the comparative example, and is slightly improved compared with that of the comparative example; after 1000 cycles, the transition metal contents in the anode sheets of examples 1-6 were significantly reduced compared to the comparative examples, wherein the content of Ni was reduced to within 0.005%, the content of Co was reduced to within 0.005%, and the content of Mn was also reduced to within 0.0072%. The cathode plate of the lithium ion battery can not obviously influence the normal temperature capacity of the lithium ion battery, and can obviously reduce the deposition of transition metal on the corresponding anode, thereby further improving the cycle performance of the battery.
TABLE 1 mass percent of transition metals in the anode sheets
| Sample (I) | Normal temperature capacity (Ah) | Ni(wt.％) | Co(wt.％) | Mn(wt.％) |
| Example 1 | 38.83 | 0.0012 | 0.0015 | 0.0040 |
| Example 2 | 38.86 | 0.0043 | 0.0050 | 0.0072 |
| Example 3 | 38.90 | 0.0009 | 0.0012 | 0.0010 |
| Example 4 | 38.86 | 0.0014 | 0.0018 | 0.0050 |
| Example 5 | 38.78 | 0.0011 | 0.0013 | 0.0028 |
| Example 6 | 38.81 | 0.0011 | 0.0010 | 0.0024 |
| Comparative example | 38.77 | 0.0200 | 0.0170 | 0.0670 |
The barrier layer contains active carbon or mesoporous carbon which has excellent adsorption performance and also has good conductivity, chemical inertness and corrosion resistance, so that the abundant pore structure of the barrier layer can be used for adsorbing the transition metal dissolved from the cathode material, and the dissolved transition metal is restrained at the cathode and prevented from diffusing to the surface of the anode, thereby obviously reducing the deposition of the transition metal on the anode.
Fig. 1 is a graph comparing the discharge capacities of the lithium ion batteries of example 1 and comparative example at different temperatures. The results show that the capacity retention rates of example 1 and comparative example are substantially consistent at different temperatures. The cathode sheet of the lithium ion battery provided by the invention is provided with the barrier layer on the active material layer, so that the discharge capacity of the battery at high and low temperatures is basically not influenced.
Fig. 2 is a graph comparing the cycle performance of the lithium ion batteries of example 1 of the present invention and the comparative example. The results show that the cycle performance of the cell of example 1 using the present invention is significantly better than that of the comparative example. The lithium ion battery cathode plate can obviously improve the cycle performance of the battery.
In combination with the above detailed description of the cathode sheet of the lithium ion battery of the present invention, it can be seen that, compared with the prior art, the present invention has at least the following beneficial technical effects:
the barrier layer containing the porous carbon material is arranged outside the active substance layer, and the abundant pore structure of the porous carbon material is utilized, so that the deposition of transition metal on the anode can be obviously reduced, the discharge capacity of the lithium ion battery at high and low temperatures can not be influenced, the cycle performance of the lithium ion battery can be obviously improved, and the cycle life of the battery can be prolonged.
The present invention can be modified and adapted appropriately from the above-described embodiments, according to the principles described above. Therefore, the present invention is not limited to the specific embodiments disclosed and described above, and some modifications and variations of the present invention should fall within the scope of the claims of the present invention. Furthermore, although specific terms are employed herein, they are used in a generic and descriptive sense only and not for purposes of limitation.
Claims (10)
1. The utility model provides a lithium ion battery cathode plate, its includes the cathode current collector, sets up the active material layer on the cathode current collector to and set up the barrier layer on the active material layer, its characterized in that: the barrier layer comprises a porous carbon material, a binder and a conductive agent, wherein the pore diameter of the porous carbon material is 2-50 nm, and the specific surface area is 500-2000m2Per g, pore volume of 1.00-2.25cm3/g。
2. The lithium ion battery cathode sheet according to claim 1, wherein: the pore diameter of the porous carbon material is 15-50nm, and the specific surface area is 820-2000m2Per g, pore volume of 1.42-2.25cm3/g。
3. The lithium ion battery cathode sheet according to claim 1, wherein: the porous carbon material is one or more of activated carbon, carbon nanotubes, mesoporous carbon or carbide derived carbon.
4. The lithium ion battery cathode sheet according to claim 1, wherein: the thickness of the barrier layer is 2-25 μm.
5. The lithium ion battery cathode sheet according to claim 1, wherein: the thickness of the barrier layer is 15-25 μm.
6. The lithium ion battery cathode sheet according to claim 1, wherein: the barrier layer comprises the following components in percentage by mass: 40-90% of a porous carbon material, 5-40% of a binder and 5-55% of a conductive agent.
7. The lithium ion battery cathode sheet according to claim 1, wherein the conductive agent in the barrier layer is one or more of conductive carbon black SP, conductive graphite, SP-L i, ketjen black, carbon fiber and graphene.
8. The lithium ion battery cathode sheet according to claim 1, wherein: the adhesive in the barrier layer is one or more of polyvinylidene fluoride, sodium carboxymethylcellulose, sodium alginate, polyvinyl alcohol, polytetrafluoroethylene, polyurethane, polyacrylic acid and acrylic acid-acrylamide copolymer.
9. The lithium ion battery cathode sheet according to claim 1, wherein: the active substance contained in the active substance layer is one or more of nickel cobalt lithium manganate, nickel cobalt lithium aluminate, lithium manganate, lithium iron phosphate and lithium-rich manganese-based materials.
10. The utility model provides a lithium ion battery, includes negative pole piece, positive pole piece, the diaphragm of interval between negative pole piece and positive pole piece to and electrolyte, its characterized in that: the cathode sheet is the lithium ion battery cathode sheet according to any one of claims 1 to 9.
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| JP2023520126A (en) * | 2020-03-20 | 2023-05-16 | ジーアールエスティー・インターナショナル・リミテッド | Cathodes and cathode slurries for secondary batteries |
| WO2023225797A1 (en) * | 2022-05-23 | 2023-11-30 | 宁德时代新能源科技股份有限公司 | Positive electrode sheet used for secondary battery, and secondary battery |
| CN115838163A (en) * | 2022-07-12 | 2023-03-24 | 宁德时代新能源科技股份有限公司 | Porous carbon material and preparation method thereof, negative electrode plate and lithium ion battery |
| CN116565293A (en) * | 2023-07-06 | 2023-08-08 | 宁德新能源科技有限公司 | Electrochemical device and electronic device |
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