CN111769260A - High specific energy lithium ion battery and preparation method thereof - Google Patents
High specific energy lithium ion battery and preparation method thereof Download PDFInfo
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- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
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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 high-specific energy lithium ion battery and a preparation method thereof. A high specific energy lithium ion battery comprises a positive electrode and a negative electrode, wherein the positive electrode comprises a positive active material, a positive conductive agent and a positive adhesive, and the negative electrode comprises a negative active material, a negative conductive agent and a negative adhesive; the positive electrode active substance is a mixed material of a lithium-rich manganese-based material and a nickel-cobalt-manganese ternary material, and the negative electrode active substance is a mixed material of a graphite material and a silicon-based material.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to a high-specific-energy lithium ion battery and a preparation method thereof.
Background
Among many cathode materials of lithium ion batteries, lithium-rich manganese-based materials are receiving increasing attention due to their high specific energy (> 250mAh/g), high potential (4.4V) and low price. The lithium-rich manganese-based material has the defects of low first charge-discharge efficiency, capacity attenuation caused by voltage attenuation, poor rate capability and the like, and the commercialization degree of the material is limited.
The negative electrode of a commercial lithium ion battery is generally made of graphite material, and the theoretical specific capacity of the negative electrode is only 372 mAh/g. The theoretical specific capacity of the graphite as the negative electrode material makes the graphite unable to alone play the big role of the new generation of negative electrode materials of lithium ion batteries. The silicon-based material severely limits its possibility of individual use due to excessive volume effects during its lithium intercalation.
Disclosure of Invention
The invention aims to provide a high-specific energy lithium ion battery and a preparation method thereof.
In order to solve the technical problems, the invention provides a high specific energy lithium ion battery, which comprises a positive electrode and a negative electrode, wherein the positive electrode comprises a positive active material, a positive conductive agent and a positive adhesive; the positive electrode active substance is a mixed material of a lithium-rich manganese-based material and a nickel-cobalt-manganese ternary material, and the negative electrode active substance is a mixed material of a graphite material and a silicon-based material.
Optionally, the mass ratio of the lithium-rich manganese-based material to the nickel-cobalt-manganese ternary material in the mixed material of the lithium-rich manganese-based material and the nickel-cobalt-manganese ternary material is (0.1-10):1, and the mass ratio of the graphite material to the silicon-based material in the mixed material of the graphite material and the silicon-based material is (0.1-50): 1.
Optionally, the nickel-cobalt-manganese ternary material is SnO2And (4) targeted coating.
Optionally, the mass ratio of the lithium-rich manganese-based material to the nickel-cobalt-manganese ternary material in the mixed material of the lithium-rich manganese-based material and the nickel-cobalt-manganese ternary material is (0.6-1.67):1, and the mass ratio of the graphite material to the silicon-based material in the mixed material of the graphite material and the silicon-based material is 24.28: 1.
Optionally, the mass of the positive electrode active material in the positive electrode is more than 95%, and the mass of the negative electrode active material in the negative electrode is more than 95%.
Optionally, the positive electrode conductive agent comprises particle conductive carbon black with the particle size of 30-40nm and carbon nanotubes, and the negative electrode conductive agent comprises particle conductive carbon black with the particle size of 30-40 nm.
The invention also provides a preparation method for manufacturing the high-specific-energy lithium ion battery, which comprises the following steps:
preparing a positive electrode: mixing the positive active substance, the positive conductive agent and the positive adhesive in proportion, uniformly stirring, coating on an aluminum foil, drying, rolling and slicing to obtain a positive electrode;
preparing a negative electrode: mixing and stirring a negative active material, a negative conductive agent and a negative adhesive uniformly according to a proportion, coating the mixture on a copper foil, drying the copper foil, and rolling and slicing the dried copper foil to obtain a negative electrode;
preparing a dry battery cell: preparing a dry battery cell by using the prepared negative electrode and the prepared positive electrode; and
and (5) preparing the battery.
Optionally, the preparation of the dry cell includes: and taking a polyethylene film as a diaphragm, stacking the anode, the diaphragm and the cathode in sequence, separating the anode and the cathode by the diaphragm, welding a tab on the outermost layer of the anode and the cathode to obtain the dry battery cell.
Optionally, the polyethylene film is coated on one side with a ceramic material.
Optionally, the preparing the battery includes preparing an electrolyte and packaging the battery, and the preparing the electrolyte includes: mixing and dissolving lithium hexafluorophosphate serving as lithium salt in a solvent with the mass ratio of ethylene carbonate, propylene carbonate and dimethyl carbonate being 1:1:1 to obtain electrolyte; the package of the battery includes: and injecting electrolyte, pre-sealing, standing, forming, secondary sealing, capacity grading and aging to obtain the high-specific-energy lithium ion battery.
In conclusion, the positive electrode of the high-specific-energy lithium ion battery provided by the invention utilizes the relatively stable structural characteristic of the nickel-cobalt-manganese NCM ternary material and the higher specific capacity of the lithium-rich manganese-based material, and the mixed positive electrode material has the characteristics of high specific capacity and long cycle performance and overcomes the serious defect of voltage attenuation of the lithium-rich manganese-based material to a certain extent. Meanwhile, the silicon-based material is matched to be used together with the cathode of the cathode additive, so that the capacity is improved.
Detailed Description
The following examples are given to further illustrate the embodiments of the present invention. The following examples are intended to illustrate the invention but are not intended to limit the scope of the invention.
Example one
Preparation of the positive electrode: mixing a lithium-rich manganese-based material, a nickel-cobalt-manganese NCM622 material, polyvinylidene fluoride PVDF HSV900 and 5130, small-particle conductive carbon black (Super P, the particle size is 30-40nm) and Carbon Nano Tubes (CNT) according to the mass ratio of 48%, 1% and 1%, and mixing, stirring and dispersing the mixture with N-methylpyrrolidone (NMP) to obtain uniform mixed slurry. And then coating the slurry on a carbon-coated aluminum foil (the thickness of the carbon-coated layer is 1 mu m) of a current collector with the thickness of 16 mu m, drying, rolling and slicing to obtain the required positive plate.
Preparation of a negative electrode: mixing artificial graphite, silicon monoxide, sodium carboxymethylcellulose (CMC), Styrene Butadiene Rubber (SBR) and small-particle conductive carbon black (Super P) according to the mass ratio of 91.05%, 3.75%, 1.2%, 2.5% and 1.5%, and mixing with ultrapure water, stirring and dispersing to obtain uniform mixed slurry. And then coating the slurry on a current collector copper foil with the thickness of 8 mu m, drying, rolling and slicing to obtain the required negative plate.
Preparing a dry battery core: taking a Polyethylene (PE) film with a single surface coated with a ceramic material as a diaphragm, and stacking a positive plate, the diaphragm and a negative plate in sequence, wherein the diaphragm separates the positive and negative plates of each layer, and the outermost layer is the negative plate; the naked electric core ultrasonic welding utmost point ear, anodal aluminium utmost point ear of using, the negative pole uses copper nickel plating utmost point ear. And (5) sticking the adhesive tape, and keeping the appearance of the battery cell to obtain the required dry battery cell.
Preparing a lithium ion battery: lithium hexafluorophosphate (LiPF6) 1M was used as a lithium salt, and was mixed and dissolved in a solvent in which Ethylene Carbonate (EC), Propylene Carbonate (PC) and dimethyl carbonate (DMC) were dissolved in a mass ratio of 1:1:1 to obtain a desired electrolyte. The aluminum-plastic film is punched to a proper size, in this embodiment, the size of the punched pits is 116mm by 227mm by 5.7mm, and the specific size is determined according to the requirement. And (3) packaging the top side, baking until the moisture is qualified, injecting the electrolyte into the battery, pre-packaging, standing, forming (charging to 4.2V at 0.05C and then charging to 4.6V at 0.15C), secondary packaging, grading and aging to obtain the required lithium ion battery. After the manufactured soft package lithium ion battery is subjected to 0.5C charging and 1C discharging cycle test for 600 weeks, the retention rate reaches 96.09%, and the first discharging specific capacity reaches 183.32 mAh/g.
Example two
The other conditions are consistent with the embodiment, and the only difference is that the positive electrode formula is changed into a lithium-rich manganese-based material, an NCM532 material, PVDF (HSV900 and 5130), small-particle conductive carbon black (Super P) and a Carbon Nano Tube (CNT) to be mixed, the retention rate of the prepared soft package lithium ion battery reaches 96.49 percent after being subjected to 0.5C charging and 1C discharging cycle test for 600 weeks, and the first discharging specific capacity reaches 178.52 mAh/g.
EXAMPLE III
The other conditions are consistent with the embodiment, the only difference is that the positive electrode formula is changed to mix the lithium-rich manganese-based material, the NCM622 material, PVDF (HSV900 and 5130), small-particle conductive carbon black (Super P) and Carbon Nano Tubes (CNT), the mass ratio is respectively 60%, 36%, 1% and 1%, the retention rate of the prepared soft package lithium ion battery reaches 95.01% after being subjected to 0.5C charging and 1C discharging cycle test for 600 weeks, and the first discharging specific capacity reaches 190.28 mAh/g.
Example four
The other conditions are consistent with the embodiment, the only difference is that the positive electrode formula is changed to mix a lithium-rich manganese-based material, an NCM622 material, PVDF (HSV900 and 5130), small-particle conductive carbon black (Super P) and Carbon Nano Tubes (CNT), the mass ratio is 36%, 60%, 1% and 1%, the retention rate of the prepared soft package lithium ion battery reaches 96.41% after being subjected to 0.5C charging and 1C discharging cycle test for 600 weeks, and the first discharging specific capacity reaches 177.09 mAh/g.
EXAMPLE five
The other conditions are consistent with the embodiment, the only difference is that the negative electrode formula is changed into the mixture of artificial graphite, micron silicon, sodium carboxymethylcellulose (CMC), Styrene Butadiene Rubber (SBR) and small-particle conductive carbon black (Super P), the retention rate of the prepared soft-package lithium ion battery reaches 94.28% after 0.5C charging and 1C discharging cycle test for 350 weeks, and the first discharging specific capacity reaches 181.78 mAh/g.
EXAMPLE six
The other conditions are consistent with the embodiment, the only difference is that the positive electrode formula is changed to mix a lithium-rich manganese-based material, an NCM622 material, PVDF (HSV900 and 5130), small-particle conductive carbon black (Super P) and carbon fiber (VGCF), the mass ratio is 36%, 60%, 1% and 1%, the retention rate of the prepared soft package lithium ion battery reaches 97.07% after being subjected to 0.5C charging and 1C discharging cycle test for 400 weeks, and the first discharging specific capacity reaches 182.85 mAh/g.
EXAMPLE seven
The other conditions are consistent with the embodiment, the only difference is that the positive electrode formula is changed to mix a lithium-rich manganese-based material, an NCM622 material, PVDF (HSV900 and 5130), small-particle conductive carbon black (Super P) and Graphene (Graphene), the mass ratio is respectively 36%, 60%, 1% and 1%, the retention rate of the prepared soft package lithium ion battery reaches 97.17% after being subjected to 0.5C charging and 1C discharging cycle testing for 400 weeks, and the first discharging specific capacity reaches 185.42 mAh/g.
Example eight
The other conditions are consistent with the embodiment, the only difference is that the positive electrode formula is changed to mix the lithium-rich manganese-based material, the NCM622 material, the PVDF (5130), the small-particle conductive carbon black (Super P) and the Carbon Nano Tube (CNT), the mass ratio is respectively 60%, 36.5%, 1.5%, 1% and 1%, the retention rate of the prepared soft package lithium ion battery reaches 95.01% after being subjected to 0.5C charging and 1C discharging cycle test for 600 weeks, and the first discharging specific capacity reaches 191.34 mAh/g.
Example nine
The other conditions are consistent with the embodiment, the only difference is that the negative electrode formula is changed into mixing of artificial graphite, silicon monoxide, sodium carboxymethylcellulose (CMC), Styrene Butadiene Rubber (SBR), Polyimide (PI) and small-particle conductive carbon black (Super P), the mass ratio is 91.05%, 3.75%, 1.2%, 2%, 0.5% and 1.5%, the retention rate of the prepared soft package lithium ion battery reaches 98.38% after being subjected to 0.5C charging and 1C discharging cycle test for 400 weeks, and the first discharging specific capacity reaches 185.86 mAh/g.
Comparative example 1
The other conditions are consistent with the embodiment, the only difference is that the positive electrode formula is changed to mix the lithium-rich manganese-based material, PVDF (HSV900 and 5130), small-particle conductive carbon black (Super P) and Carbon Nano Tubes (CNT), the mass ratio is respectively 96%, 1% and 1%, the retention rate of the prepared soft package lithium ion battery is attenuated to 90.23% after being subjected to 0.5C charging and 1C discharging cycle test for 400 weeks, and the first discharging specific capacity reaches 215.25 mAh/g.
Comparative example No. two
The other conditions are consistent with the embodiment, the only difference is that the positive electrode formula is changed to mix the NCM622 material, PVDF (HSV900 and 5130), small-particle conductive carbon black (Super P) and Carbon Nano Tubes (CNT), the mass ratio is respectively 96%, 1% and 1%, the retention rate of the prepared soft package lithium ion battery reaches 97.12% after being subjected to 0.5C charging and 1C discharging cycle test for 600 weeks, and the first discharging specific capacity reaches 164.35 mAh/g.
Comparative example No. three
The other conditions are consistent with the embodiment, the only difference is that the negative electrode formula is changed into mixing of artificial graphite, sodium carboxymethylcellulose (CMC), Styrene Butadiene Rubber (SBR) and small-particle conductive carbon black (Super P), the mass ratio of the mixture is 94.8%, 1.2%, 2.5% and 1.5%, the soft package lithium ion battery prepared by the method has a low-capacity phenomenon (less than 58Ah), and the lithium precipitation phenomenon occurs after 100 weeks of 0.5C charging and 1C discharging cycle test, so that the battery core has potential safety hazards.
Comparative example No. four
The other conditions are consistent with the embodiment, the only difference is that the particle size of the conductive carbon black is 100nm-200nm, the retention rate of the prepared soft package lithium ion battery is attenuated to 94.23% after being subjected to 0.5C charging and 1C discharging cycle test for 400 weeks, and the first discharging specific capacity reaches 181.25 mAh/g.
Example ten
The other conditions were kept consistent with the examples, the only difference being that SnO was prepared by a plasma-assisted ball milling technique2Targeting packageA nickel cobalt manganese coated material. Wherein the nickel cobalt manganese material and SnO2And performing plasma-assisted ball milling on the powder according to the mass ratio of 98:2, and performing ball milling for 8 hours to obtain the required material. After the prepared soft package lithium ion battery is subjected to 0.5C charging and 1C discharging cycle test for 400 weeks, the retention rate is attenuated to 98.73%, and the first discharging specific capacity reaches 193.24 mAh/g.
By comparing the first embodiment, the third embodiment and the fourth embodiment, when the mass ratio of the lithium-rich manganese-based material to the nickel-cobalt-manganese material is 5:3, the specific capacity of the lithium ion battery is optimal, and the cycle performance is worst; when the mass ratio of the lithium-rich manganese-based material to the nickel-cobalt-manganese material is 1:1, the specific capacity of the lithium ion battery is reduced to some extent and the cycle performance is improved to some extent; when the mass ratio of the lithium-rich manganese-based material to the nickel-cobalt-manganese material is 3:5, the specific capacity of the lithium ion battery is the minimum and the cycle performance is optimal.
By comparing examples one to nine with comparative examples one to three, the positive electrode made of the lithium-rich manganese-based material and the nickel-cobalt-manganese material and the negative electrode made of the mixture of the graphite material and the silicon-based material have synergistic effects with each other. The positive electrode made of the lithium-rich manganese-based material and the nickel-cobalt-manganese material is poor in electric cycle performance. Or the cathode is only made of the mixture of graphite materials and silicon-based materials, and the specific discharge capacity is not high.
By comparing examples one to nine with comparative examples one and comparative example two, in the positive electrode, both the absence of the lithium-rich manganese-based material and the absence of the NCM have an effect on the performance of the battery. The lithium ion batteries in the first to ninth embodiments all have a retention rate of over 95% after being subjected to 0.5C charging and 1C discharging cycle test for 400 weeks, a first discharging specific capacity of over 180mAh/g, and very good specific capacity and cycle performance.
Comparing the first example with the tenth example, SnO is prepared by adopting a plasma-assisted ball milling technology2The lithium ion battery made of the target coated nickel-cobalt-manganese material has better specific capacity and cycle performance.
Although the present invention has been described with reference to the preferred embodiments, it should be understood that various changes and modifications can be made therein by those skilled in the art without departing from the spirit and scope of the invention as defined by the appended claims.
Claims (10)
1. The high-specific-energy lithium ion battery is characterized by comprising a positive electrode and a negative electrode, wherein the positive electrode comprises a positive active material, a positive conductive agent and a positive adhesive, and the negative electrode comprises a negative active material, a negative conductive agent and a negative adhesive; the positive active substance is a mixed material of a lithium-rich manganese-based material and a nickel-cobalt-manganese ternary material, and the negative active substance is a mixed material of a graphite material and a silicon-based material.
2. The high specific energy lithium ion battery of claim 1, wherein the mass ratio of the lithium-rich manganese-based material to the nickel-cobalt-manganese ternary material in the mixed material of the lithium-rich manganese-based material and the nickel-cobalt-manganese ternary material is (0.1-10): 1; the mass ratio of the graphite material to the silicon-based material in the mixed material of the graphite material and the silicon-based material is (0.1-50): 1.
3. The high specific energy lithium ion battery of claim 2, wherein the mass ratio of the lithium-rich manganese-based material to the nickel-cobalt-manganese ternary material in the mixed material of the lithium-rich manganese-based material and the nickel-cobalt-manganese ternary material is (0.6-1.67):1, and the mass ratio of the graphite material to the silicon-based material in the mixed material of the graphite material and the silicon-based material is 24.28: 1.
4. The high specific energy lithium ion battery of claim 3, wherein the nickel cobalt manganese ternary material is formed from SnO2And (4) targeted coating.
5. The high specific energy lithium ion battery according to any one of claims 1 to 4, wherein the positive electrode active material accounts for 95% or more by mass of the positive electrode, and the negative electrode active material accounts for 95% or more by mass of the negative electrode.
6. The high specific energy lithium ion battery of any one of claims 1 to 4, wherein the positive electrode conductive agent comprises particulate conductive carbon black having a particle size of 30-40nm and carbon nanotubes, and the negative electrode conductive agent comprises particulate conductive carbon black having a particle size of 30-40 nm.
7. A method of manufacturing a high specific energy lithium ion battery according to any of claims 1 to 6, comprising:
preparing a positive electrode: mixing the positive active substance, the positive conductive agent and the positive adhesive in proportion, uniformly stirring, coating on an aluminum foil, drying, rolling and slicing to obtain a positive electrode;
preparing a negative electrode: mixing and stirring a negative active material, a negative conductive agent and a negative adhesive uniformly according to a proportion, coating the mixture on a copper foil, drying the copper foil, and rolling and slicing the dried copper foil to obtain a negative electrode;
preparing a dry battery cell: preparing a dry battery cell by using the prepared negative electrode and the prepared positive electrode; and
and (5) preparing the battery.
8. The high specific energy lithium ion battery of claim 7, wherein the preparation of the dry cell comprises: and taking a polyethylene film as a diaphragm, stacking the anode, the diaphragm and the cathode in sequence, separating the anode and the cathode by the diaphragm, welding a tab on the outermost layer of the anode and the cathode to obtain the dry battery cell.
9. The high specific energy lithium ion battery of claim 8, wherein said polyethylene film is single coated with a ceramic material.
10. The high specific energy lithium ion battery of any of claims 8 to 9, wherein the preparing the battery comprises preparing an electrolyte and packaging the battery, wherein the preparing the electrolyte comprises: mixing and dissolving lithium hexafluorophosphate serving as lithium salt in a solvent with the mass ratio of ethylene carbonate, propylene carbonate and dimethyl carbonate being 1:1:1 to obtain electrolyte; the package of the battery includes: and injecting electrolyte, pre-sealing, standing, forming, secondary sealing, capacity grading and aging to obtain the high specific energy lithium ion battery.
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| CN114335687A (en) * | 2021-12-30 | 2022-04-12 | 横店集团东磁股份有限公司 | Lithium ion battery and preparation method thereof |
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