WO2024031216A1 - Plaque d'électrode négative et son procédé de préparation, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique - Google Patents

Plaque d'électrode négative et son procédé de préparation, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique Download PDF

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Publication number
WO2024031216A1
WO2024031216A1 PCT/CN2022/110769 CN2022110769W WO2024031216A1 WO 2024031216 A1 WO2024031216 A1 WO 2024031216A1 CN 2022110769 W CN2022110769 W CN 2022110769W WO 2024031216 A1 WO2024031216 A1 WO 2024031216A1
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negative electrode
buffer layer
current collector
lithium
active material
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PCT/CN2022/110769
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English (en)
Chinese (zh)
Inventor
陈兴布
孙信
吴李力
李璇
董苗苗
云亮
宋佩东
刘润蝶
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宁德时代新能源科技股份有限公司
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Priority to CN202280088146.9A priority Critical patent/CN118679593A/zh
Priority to PCT/CN2022/110769 priority patent/WO2024031216A1/fr
Publication of WO2024031216A1 publication Critical patent/WO2024031216A1/fr

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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
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof

Definitions

  • the present application relates to the field of secondary batteries, specifically to a negative electrode plate and its preparation method, secondary batteries, battery modules, battery packs and electrical devices.
  • lithium-ion batteries With the growth of new energy demand, the market has put forward increasingly higher requirements for the endurance and service life of secondary batteries such as lithium-ion batteries. As the number of cycles of a lithium-ion battery increases, the active lithium in the battery will gradually decrease, thus affecting its energy density and cycle life. Traditional technology usually presses metallic lithium onto the surface of the active material layer for lithium replenishment. However, because the lithium replenishment rate is too fast, a large amount of heat will be generated instantly, posing safety risks. At the same time, after the battery is filled with liquid, metal lithium is quickly replenished with lithium. If the amount of lithium supplement is large, lithium deposition will easily occur during the cycle, which will affect the cycle life of the battery.
  • this application provides a negative electrode plate and a preparation method thereof, a secondary battery, a battery module, a battery pack and a power device, which can improve the cycle performance of the secondary battery.
  • One aspect of the present application provides a negative electrode sheet, including a first negative active material layer, a first current collector, a lithium replenishing layer, a second current collector and a second negative active material layer that are stacked in sequence; the negative electrode
  • the pole pieces also include cushioning material;
  • At least one of the first current collector and the second current collector has a through hole; the buffer material is filled in the through hole of the first current collector and the through hole of the second current collector. At least one of them.
  • the negative electrode sheet further includes a first buffer layer, which is disposed between the first current collector and the lithium replenishing layer and partially embedded in the first current collector. In the through hole of the fluid, so that the buffer material is filled in the through hole of the first current collector;
  • the negative electrode piece further includes a second buffer layer, the second buffer layer is disposed between the second current collector and the lithium replenishing layer, and is partially embedded in the passage of the second current collector. hole, so that the buffer material is filled in the through hole of the second current collector.
  • the thickness of the first buffer layer is 3 ⁇ m ⁇ 10 ⁇ m; optionally, the thickness of the first buffer layer is 3 ⁇ m ⁇ 7 ⁇ m;
  • the thickness of the second buffer layer is 3 ⁇ m ⁇ 10 ⁇ m; optionally, the thickness of the second buffer layer is 3 ⁇ m ⁇ 7 ⁇ m.
  • the first buffer layer and the second buffer layer have lithium ion conductivity.
  • the first buffer layer and the second buffer layer each include an ion conductor material
  • the ion conductor material includes at least one of an ion conductor polymer, an ion conductor oxide, an ion conductor sulfide, and an ion conductor halide.
  • the ion conductor material has an ion conductivity of 10 -9 S/cm 2 to 10 -2 S/cm 2 .
  • the ion conductor polymer is selected from at least one of polyethylene oxide, polyvinylidene fluoride, and polyanionic conductor polymers;
  • the ion conductor oxide is selected from at least one selected from the group consisting of lithium lanthanum titanium oxide, lithium lanthanum zirconium oxide, and lithium titanium aluminum phosphate.
  • the mass percentage of the ion conductor material in the first buffer layer is 60% to 80%; and/or the mass percentage of the ion conductor material in the second buffer layer is 60% ⁇ 80%;
  • the mass percentage of the ion conductor material is 70% to 80%; and/or in the second buffer layer, the mass percentage of the ion conductor material is 70%. ⁇ 80%.
  • the porosity of the first buffer layer and the second buffer layer is 2% to 50%;
  • the porosity of the first buffer layer and the second buffer layer is 20% to 40%.
  • the total area occupied by the through holes of the first current collector accounts for 0.1% to 30% of the area on the first current collector
  • the total area occupied by the through holes of the first current collector accounts for 2% to 15% of the area on the first current collector.
  • the area ratio of the through holes of the second current collector on the second current collector is 0.1% to 30%;
  • the area ratio of the through holes of the second current collector on the second current collector is 2% to 15%.
  • the maximum pore diameter of the first current collector and/or the second current collector is 5 ⁇ m to 1 mm;
  • the maximum pore diameter of the through holes of the first current collector and/or the second current collector is 30 ⁇ m to 200 ⁇ m.
  • the negative electrode sheet of the present application can avoid the problem of avoiding the If the lithium replenishment layer is in direct contact with the negative active material, the lithium replenishment rate is too fast and there is a risk of heat generation; the buffer material can regulate the lithium replenishment rate of the lithium replenishment layer to avoid lithium dendrites caused by excessive lithium replenishment rate.
  • the secondary battery has a long lifespan. cycle life.
  • this application also provides a method for preparing a negative electrode sheet, including the following steps:
  • the present application also provides a secondary battery, including the above-mentioned negative electrode sheet or the negative electrode sheet prepared according to the above-mentioned preparation method of the negative electrode sheet.
  • the negative electrode sheet includes a first buffer layer and a second buffer layer;
  • the secondary battery includes a positive active material and a negative active material;
  • the first Coulombic efficiency of the positive active material is >90%, The first Coulombic efficiency of the negative active material is >90%;
  • the thickness of the first buffer layer is 4 ⁇ m to 7 ⁇ m;
  • the thickness of the second buffer layer is 4 ⁇ m to 7 ⁇ m;
  • the first Coulombic efficiency of the positive active material is ⁇ 90%, and/or the first Coulombic efficiency of the negative active material is ⁇ 90%;
  • the thickness of the first buffer layer is 3 ⁇ m to 5 ⁇ m; and the second buffer layer The thickness is 3 ⁇ m ⁇ 5 ⁇ m.
  • the negative electrode sheet includes a first buffer layer and a second buffer layer;
  • the secondary battery includes a positive active material and a negative active material;
  • the first Coulombic efficiency of the positive active material is >90%,
  • the first Coulombic efficiency of the negative active material is >90%;
  • the ion conductivity of the ion conductor material is 10 -9 S/cm 2 ⁇ 10 -5 S/cm 2 ;
  • the first Coulombic efficiency of the positive active material is ⁇ 90%, and/or the first Coulombic efficiency of the negative active material is ⁇ 90%; the ion conductivity of the ion conductor material is 10 -6 S/cm 2 ⁇ 10 -2 S/cm 2 .
  • the negative electrode sheet includes a first buffer layer and a second buffer layer;
  • the secondary battery includes a positive active material and a negative active material;
  • the first Coulombic efficiency of the positive active material is >90%,
  • the first Coulombic efficiency of the negative active material is >90%;
  • the porosity of the first buffer layer and the second buffer layer is 30% to 40%;
  • the first Coulombic efficiency of the positive active material is ⁇ 90%, and/or the first Coulombic efficiency of the negative active material is ⁇ 90%; the porosity of the first buffer layer and the second buffer layer is 20%. ⁇ 30%.
  • the present application also provides a battery module, including the above-mentioned secondary battery.
  • the present application further provides a battery pack, including at least one of the above-mentioned secondary battery and the above-mentioned battery module.
  • the present application further provides an electrical device, including at least one selected from the above-mentioned secondary battery, the above-mentioned battery module, or the above-mentioned battery pack.
  • Figure 1 is a schematic diagram of a secondary battery according to an embodiment of the present application.
  • Figure 2 is an exploded view of the secondary battery according to an embodiment of the present application shown in Figure 1;
  • FIG. 3 is a schematic diagram of a battery module according to an embodiment of the present application.
  • Figure 4 is a schematic diagram of a battery pack according to an embodiment of the present application.
  • FIG 5 is an exploded view of the battery pack according to an embodiment of the present application shown in Figure 4;
  • Figure 6 is a schematic diagram of an electrical device using a secondary battery as a power source according to an embodiment of the present application
  • the inventor of the present application has provided a negative electrode sheet with a special lithium replenishing structure, which can reasonably control the lithium replenishing rate of the lithium replenishing structure, so that the lithium replenishing rate ⁇ the active lithium loss rate of the secondary battery, so the secondary battery It has higher energy density and longer cycle life.
  • the present application provides a negative electrode plate, a secondary battery, a battery module, a battery pack and an electrical device using the negative electrode plate.
  • This kind of secondary battery is suitable for various electrical devices that use batteries, such as mobile phones, portable devices, laptops, battery cars, electric toys, power tools, electric cars, ships and spacecraft.
  • spacecraft include aircraft, rockets , space shuttles and spacecrafts, etc.
  • a secondary battery is provided.
  • a secondary battery typically includes a positive electrode plate, a negative electrode plate, an electrolyte and a separator.
  • active ions are inserted and detached back and forth between the positive and negative electrodes.
  • the electrolyte plays a role in conducting ions between the positive and negative electrodes.
  • the isolation film is placed between the positive electrode piece and the negative electrode piece. It mainly prevents the positive and negative electrodes from short-circuiting and allows ions to pass through.
  • a negative electrode piece in one embodiment of the present application, is provided.
  • the negative electrode sheet includes a first negative electrode active material layer, a first negative electrode current collector, a lithium replenishing layer, a second negative electrode current collector, and a second negative electrode active material layer that are stacked in sequence.
  • the negative electrode plate also includes buffer material. At least one of the first negative electrode current collector and the second negative electrode current collector has a through hole; the buffer material is filled in at least one of the through hole of the first negative electrode current collector and the through hole of the second negative electrode current collector.
  • a lithium replenishing layer is sandwiched between two negative electrode current collectors with through holes, the through holes are filled with buffer materials, and a negative electrode active material layer is provided on the surface of the negative electrode current collector away from the lithium replenishing layer. It can prevent the lithium replenishment layer from being in direct contact with the negative active material and the lithium replenishment rate is too fast; the buffer material can regulate the lithium replenishment rate of the lithium replenishment layer to avoid lithium dendrites caused by excessive lithium replenishment rate.
  • the secondary battery has a longer cycle life. .
  • the lithium supplement layer supplements lithium to the negative electrode active material layer on the side close to the through hole.
  • the buffer material has lithium ion conductivity.
  • the buffer material may be an ion conductor material.
  • the ion conductor material has the ability to conduct lithium ions. It fills the through holes of the negative electrode current collector and can conduct lithium ions, thus realizing the lithium replenishment of the negative electrode sheet.
  • the first negative electrode current collector has multiple through holes, and the buffer material fills part or all of the through holes.
  • the second negative electrode current collector has a plurality of through holes, and the buffer material fills part or all of the through holes. Further, the buffer material fills all the through holes.
  • the negative electrode sheet further includes a first buffer layer, which is disposed between the first negative electrode current collector and the lithium replenishing layer, and is partially embedded in the through hole of the first negative electrode current collector, so that The buffer material is filled in the through hole of the first negative electrode current collector.
  • the negative electrode sheet also includes a second buffer layer. The second buffer layer is disposed between the second negative electrode current collector and the lithium replenishing layer, and is partially embedded in the through hole of the second negative electrode current collector, so that the buffer material is filled in the second negative electrode. in the through hole of the current collector.
  • the first buffer layer may be a continuous film layer structure between the first negative electrode current collector and the lithium supplement layer, so as to completely isolate the first negative electrode current collector and the lithium supplement layer; or, A buffer layer may also be distributed discontinuously between the first negative electrode current collector and the lithium replenishing layer.
  • the second buffer layer may be a continuous film layer structure between the first negative electrode current collector and the lithium supplement layer, so as to completely isolate the second negative electrode current collector and the lithium supplement layer; or, The two buffer layers may also be distributed discontinuously between the first negative electrode current collector and the lithium replenishing layer.
  • the thickness of the first buffer layer ranges from 3 ⁇ m to 10 ⁇ m.
  • the thickness of the first buffer layer is 3 ⁇ m, 4 ⁇ m, 5 ⁇ m, 6 ⁇ m, 7 ⁇ m, 8 ⁇ m, 9 ⁇ m or 10 ⁇ m.
  • the thickness of the first buffer layer is 3 ⁇ m ⁇ 7 ⁇ m.
  • the thickness of the second buffer layer is 3 ⁇ m to 10 ⁇ m.
  • the thickness of the second buffer layer is 3 ⁇ m, 4 ⁇ m, 5 ⁇ m, 6 ⁇ m, 7 ⁇ m, 8 ⁇ m, 9 ⁇ m or 10 ⁇ m.
  • the thickness of the second buffer layer is 3 ⁇ m ⁇ 7 ⁇ m.
  • the thickness of the first buffer layer or the second buffer layer refers to the thickness of the buffer material filled in the first negative electrode current collector or the second negative electrode current collector through hole and the first buffer layer or the second buffer layer covering the first negative electrode current collector.
  • the thickness of the first buffer layer or the second buffer layer is the minimum distance between the lithium supplement layer and the first negative electrode active material layer or the second negative electrode active material layer.
  • the thickness of the first buffer layer or the second buffer layer can be obtained by observing the cross-section of the negative electrode piece using a scanning electron microscope (SEM).
  • SEM scanning electron microscope
  • the thickness of the buffer layer is too small, the lithium replenishment rate is too fast and lithium dendrites are formed, which affects the cycle life of the secondary battery; when the buffer layer thickness is too large, the lithium replenishment rate is slow and the energy density of the secondary battery is reduced.
  • Controlling the thickness of the buffer layer within the above range can control the appropriate lithium replenishment rate of the negative electrode sheet.
  • the lithium replenishment rate of the negative electrode plate is less than or equal to the active lithium loss rate of the secondary battery, so that the secondary battery can have both high energy density and long cycle life.
  • the active lithium loss rate of a secondary battery refers to the rate of active lithium loss during the cycle of the secondary battery. It can be estimated by the slope of the curve of the capacity of the secondary battery changing with the number of cycles during the cycle of the secondary battery, that is, the capacity fading rate. Specifically, the active lithium loss rate of the secondary battery can be estimated by the following equation.
  • the lithium replenishment rate is 0, and the secondary battery capacity decreases as the number of cycles increases; when the lithium replenishment rate ⁇ the active lithium loss rate, the slope of the curve of the capacity changing with the number of cycles is relative to The slope of the lithium replenishment rate is partially increased; when the lithium replenishment rate ⁇ the active lithium loss rate, the slope of the curve of capacity changing with the number of cycles mainly depends on the loss of the positive electrode active material's own lithium intercalation capacity; when the lithium replenishment rate > When the active lithium loss rate is high, compared to the situation where the lithium replenishment rate ⁇ the active lithium loss rate, the slope of the curve of capacity changing with the number of cycles cannot be further improved. Instead, lithium will be deposited on the surface of the negative electrode, which can easily lead to internal micro short circuits and self-discharge. Increased problems bring security risks.
  • the first Coulombic efficiency of the positive active material is >90%, and the first Coulombic efficiency of the negative active material is >90%; the thickness of the first buffer layer is 4 ⁇ m ⁇ 7 ⁇ m; the thickness of the second buffer layer is 4 ⁇ m ⁇ 7 ⁇ m .
  • the first Coulombic efficiency of the positive electrode refers to the first lithium insertion capacity/first lithium removal capacity of the positive electrode active material.
  • the first Coulombic efficiency of the negative electrode refers to the first lithium removal capacity/first lithium insertion capacity of the negative electrode active material. It can be determined by the positive electrode active material or the negative electrode active material alone. Prepare button cells for measurement.
  • the secondary battery has a slower active lithium loss rate, and the thickness of the buffer layer is controlled within the above range, the secondary battery has a more suitable lithium replenishment rate. speed, both high energy density and long cycle life.
  • the first Coulombic efficiency of cathode active materials such as lithium iron phosphate (LFP), lithium iron manganese phosphate (LMFP), lithium nickel cobalt manganese oxide (NCM), lithium manganate (LMO), lithium cobalt oxide (LCO), etc. >90%.
  • the first Coulombic efficiency of negative active materials such as natural graphite, artificial graphite, lithium titanate (LTO), soft carbon, etc. is >90%.
  • the first Coulombic efficiency of the positive active material is ⁇ 90%, and/or the first Coulombic efficiency of the negative active material is ⁇ 90%; the thickness of the first buffer layer is 3 ⁇ m to 5 ⁇ m; and the thickness of the second buffer layer is 3 ⁇ m ⁇ 5 ⁇ m.
  • the first Coulombic efficiency of the positive active material and the negative active material is low, the irreversible capacity of the positive active material and the negative active material is large and the loss rate of active lithium is large, the thickness of the buffer layer is controlled within the above range, and the secondary The battery has a more appropriate lithium replenishment rate, higher energy density and longer cycle life.
  • the first Coulombic efficiency of positive active materials such as lithium-rich lithium manganate, lithium-rich lithium nickelate, etc. is ⁇ 90%.
  • the first Coulombic efficiency of negative active materials such as silicon-based materials, tin-based materials, lithium metal negative electrodes, and some porous carbons is ⁇ 90%.
  • the first buffer layer and the second buffer layer have lithium ion conductivity.
  • both the first buffer layer and the second buffer layer include ion conductor materials.
  • the ion conductor material includes at least one of an ion conductor polymer, an ion conductor oxide, an ion conductor sulfide, and an ion conductor halide.
  • the ion conductor material has lithium ion conductivity and can conduct lithium ions on both sides of the negative electrode current collector to achieve lithium replenishment in the secondary battery.
  • the ion conductor polymer may be selected from at least one of, but not limited to, polyethylene oxide (PEO), polyvinylidene fluoride (PVDF), and polyanionic conductor polymers.
  • the ion conductor oxide may be selected from at least one of, but not limited to, lithium lanthanum titanium oxide (LLTO), lithium lanthanum zirconium oxide (LLZO), and lithium aluminum titanium phosphate (LATP).
  • LLTO lithium lanthanum titanium oxide
  • LLZO lithium lanthanum zirconium oxide
  • LATP lithium aluminum titanium phosphate
  • the ion conductor material has an ionic conductivity of 10 -9 S/cm 2 to 10 -2 S/cm 2 .
  • the buffer layer is assembled into a localized symmetrical battery.
  • L is the thickness of the buffer layer.
  • S is the effective contact area between the buffer layer and the electrode during testing.
  • the first Coulombic efficiency of the positive active material is >90%, and the first Coulombic efficiency of the negative active material is >90%;
  • the ionic conductivity of the ion conductor material is 10 -9 S/cm 2 ⁇ 10 -5 S/ cm 2 .
  • ion conductor materials such as polyethylene oxide (PEO), 42.5Li 2 O ⁇ 57.5B 2 O 3 , Li 2.9 PO 3.3 N 0.46 , Li 3.6 Si 0. 6P 0.4 O 0.4 , Li 3.25 Ge 0.25 P 0.75 S 4
  • the ionic conductivity is 10 -9 S/cm 2 to 10 -5 S/cm 2 .
  • the first Coulombic efficiency of the positive active material is ⁇ 90%, and/or the first Coulombic efficiency of the negative active material is ⁇ 90%;
  • the ionic conductivity of the ion conductor material is 10 -6 S/cm 2 ⁇ 10 - 2 S/cm 2 .
  • the ion conductivity of ion conductor materials such as lithium lanthanum titanium oxide (LLTO), lithium lanthanum zirconium oxide (LLZO), Li 6 PS 5 Cl, etc. is 10 -6 S/cm 2 to 10 -2 S/cm 2 .
  • the mass percentage of the ion conductor material in the first buffer layer is 60% to 90%.
  • the mass percentage of the ion conductor material is 60%, 62%, 64%, 65%, 68%, 70%, 72%, 75%, 78%, 80%, 82%, 84%, 85%, 88% or 90%.
  • the mass percentage of the ion conductor material in the first buffer layer is 70% to 80%.
  • the mass percentage of the ion conductor material in the second buffer layer is 60% to 90%.
  • the mass percentage of the ion conductor material in the second buffer layer is 60%, 62%, 64%, 65%, 68%, 70%, 72%, 75%, 78%, 80%, 82%, 84%, 85%, 88% or 90%.
  • the mass percentage of the ion conductor material is 70% to 80%.
  • the first buffer layer and/or the second buffer layer further includes an adhesive and a conductive agent.
  • the porosity of the first buffer layer and the second buffer layer is 2% to 50%.
  • the porosity of the first buffer layer and the second buffer layer is 2%, 5%, 10%, 15%, 20%, 25%, 30%, 35%, 40%, 45% or 50%. Further, the porosity of the first buffer layer and the second buffer layer is 20% to 40%.
  • the true density method is used to test the porosity, and the inert gas (helium) replacement method with a small molecular diameter is used, combined with Archimedes' principle and Bohr's law, to accurately measure the true volume of the material being tested, thereby obtaining the sample to be tested porosity.
  • the inventor's research found that the porosity of the buffer layer will affect its lithium ion conductivity. If the porosity of the buffer layer is smaller, the ion conductivity of the buffer layer will be lower, and the lithium replenishment rate of the secondary battery will be slower; the pores of the buffer layer If the ratio is larger, the ionic conductivity of the buffer layer is higher, and the lithium replenishment rate of the secondary battery is faster; by adjusting the porosity of the buffer layer, it can adapt to secondary battery systems with different active lithium loss rates.
  • the first Coulombic efficiency of the positive active material is >90%, and the first Coulombic efficiency of the negative active material is >90%; the porosity of the first buffer layer and the second buffer layer is 30% to 40%.
  • the first Coulombic efficiency of the positive active material is ⁇ 90%, and/or the first Coulombic efficiency of the negative active material is ⁇ 90%; the porosity of the first buffer layer and the second buffer layer is 20% to 30%. .
  • the total area of the through holes of the first negative electrode current collector accounts for 0.1% to 30% of the area of the first negative electrode current collector.
  • the function of the through hole is to allow lithium ions in the lithium replenishment layer to pass through the current collector to replenish lithium for the negative active material layer. If the area ratio of the through hole is within the above range, lithium ions can pass through. If the area ratio of the through holes is too low, the lithium replenishment rate will be too low; if the area ratio of the through holes is too high, the lithium replenishment rate will be too fast and the strength of the current collector will be reduced.
  • the total area occupied by the through holes of the first negative electrode current collector accounts for 0.1%, 0.5%, 1%, 2%, 5%, 10%, 15%, 20%, 25% or 30%. Further, the total area occupied by the through holes of the first negative electrode current collector accounts for 2% to 15% of the area of the first negative electrode current collector.
  • the area ratio of the through hole of the second negative electrode current collector on the second negative electrode current collector ranges from 0.1% to 30%.
  • the function of the through hole is to allow lithium ions in the lithium replenishment layer to pass through the current collector to replenish lithium for the negative active material layer. If the area ratio of the through hole is within the above range, lithium ions can pass through. If the area ratio of the through holes is too low, the lithium replenishment rate will be too low; if the area ratio of the through holes is too high, the lithium replenishment rate will be too fast.
  • the total area occupied by the through holes of the second negative electrode current collector accounts for 0.1%, 0.5%, 1%, 2%, 5%, 10%, 15%, 20%, 25% or 30%. Further, the area ratio of the through hole of the second negative electrode current collector on the second negative electrode current collector is 2% to 15%.
  • the maximum pore diameter of the first negative electrode current collector and/or the second negative electrode current collector is 5 ⁇ m to 1 mm.
  • the maximum pore diameter of the through hole of the first negative electrode current collector and/or the second negative electrode current collector is 5 ⁇ m, 10 ⁇ m, 30 ⁇ m, 50 ⁇ m, 100 ⁇ m, 150 ⁇ m, 200 ⁇ m, 400 ⁇ m, 500 ⁇ m, 800 ⁇ m or 1000 ⁇ m.
  • the maximum pore diameter of the through hole of the first negative electrode current collector and/or the second negative electrode current collector is 30 ⁇ m to 200 ⁇ m.
  • the maximum pore diameter of the through holes is within the above range.
  • the first negative electrode current collector and/or the second negative electrode current collector have through holes with smaller pore diameters and a larger number, which can make the lithium replenishment diffuse more uniformly.
  • the total area ratio and pore diameter of the through holes of the first negative electrode current collector and/or the second negative electrode current collector can be analyzed by observing the surface of the negative electrode sheet where the current collector is located with a scanning electron microscope (SEM).
  • SEM scanning electron microscope
  • the negative electrode current collector may be a metal foil or a composite current collector.
  • the metal foil copper foil can be used.
  • the composite current collector may include a polymer material base layer and a metal layer formed on at least one surface of the polymer material base material.
  • the composite current collector can be formed by forming metal materials such as copper, copper alloy, nickel, nickel alloy, titanium, titanium alloy, silver and silver alloy on a polymer material substrate.
  • Polymer material substrates include polypropylene (PP), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE) ) and other base materials.
  • the negative active material may be a negative active material known in the art for batteries.
  • the negative active material may include at least one of the following materials: artificial graphite, natural graphite, soft carbon, hard carbon, silicon-based materials, tin-based materials, lithium titanate, and the like.
  • the silicon-based material may be selected from at least one of elemental silicon, silicon oxide compounds, silicon carbon composites, silicon nitrogen composites and silicon alloys.
  • the tin-based material may be selected from at least one of elemental tin, tin oxide compounds and tin alloys.
  • the present application is not limited to these materials, and other traditional materials that can be used as battery negative electrode active materials can also be used. Only one type of these negative electrode active materials may be used alone, or two or more types may be used in combination.
  • the negative active material layer optionally further includes a binder.
  • the binder can be selected from styrene-butadiene rubber (SBR), polyacrylic acid (PAA), sodium polyacrylate (PAAS), polyacrylamide (PAM), polyvinyl alcohol (PVA), sodium alginate (SA), polymethyl At least one of acrylic acid (PMAA) and carboxymethyl chitosan (CMCS).
  • the negative active material layer optionally further includes a conductive agent.
  • the conductive agent may be selected from at least one of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene and carbon nanofibers.
  • the negative active material layer optionally includes other auxiliaries, such as thickeners (such as sodium carboxymethylcellulose (CMC-Na)) and the like.
  • thickeners such as sodium carboxymethylcellulose (CMC-Na)
  • Another embodiment of the present application also provides a method for preparing a negative electrode piece, including steps S110 to S140.
  • Step S110 Coat the negative electrode slurry on one surface of the negative electrode current collector to prepare a negative electrode active material layer.
  • Step S120 Drill holes into the negative electrode current collector from the surface of the negative electrode current collector away from the negative electrode active material layer to form a through hole.
  • the drilling step in step S120 may use laser drilling, roller pinning, or other methods to form through holes.
  • Step S130 Coat the buffer material slurry on the surface of the negative electrode current collector away from the negative electrode active material layer, so that the buffer material fills the through holes to obtain a sub-negative electrode piece.
  • Step S140 Take two sub-negative electrode sheets and prepare a lithium replenishing layer on the surface of the buffer material of at least one of the sub-negative electrode sheets, and connect the sub-negative electrode sheet with the lithium replenishing layer to the surface of the lithium replenishing layer of the other sub-negative electrode sheet.
  • the surfaces of the buffer material of the negative electrode piece are bonded together to prepare the negative electrode piece.
  • the two sub-negative electrode plates may be the same or different.
  • lithium replenishing layers can be separately prepared on the surfaces of the buffer materials of the two sub-negative electrode plates to prepare two sub-negative electrode plates with lithium replenishing layers; The surfaces of the sub-negative electrode pieces with the lithium-supplementing layer are bonded together to prepare the negative electrode piece.
  • a through hole may be formed in one of the negative current collectors of the two sub-negative electrode pieces.
  • the positive electrode sheet includes a positive current collector and a positive active material layer disposed on at least one surface of the positive current collector.
  • the positive active material layer includes a positive active material.
  • the positive electrode current collector has two surfaces opposite in its own thickness direction, and the positive electrode active material layer is disposed on any one or both of the two opposite surfaces of the positive electrode current collector.
  • the positive current collector may be a metal foil or a composite current collector.
  • the metal foil aluminum foil can be used.
  • the composite current collector may include a polymer material base layer and a metal layer formed on at least one surface of the polymer material base layer.
  • the composite current collector can be formed by forming metal materials such as aluminum, aluminum alloy, nickel, nickel alloy, titanium, titanium alloy, silver and silver alloy on a polymer material substrate.
  • Polymer material substrates include polypropylene (PP), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE) ) and other base materials.
  • the cathode active material may be a cathode active material known in the art for batteries.
  • the cathode active material may include at least one of the following materials: an olivine-structured lithium-containing phosphate, a lithium transition metal oxide, and their respective modified compounds.
  • the present application is not limited to these materials, and other traditional materials that can be used as positive electrode active materials of batteries can also be used. Only one type of these positive electrode active materials may be used alone, or two or more types may be used in combination.
  • lithium transition metal oxides may include, but are not limited to, lithium cobalt oxides (such as LiCoO 2 ), lithium nickel oxides (such as LiNiO 2 ), lithium manganese oxides (such as LiMnO 2 , LiMn 2 O 4 ), lithium Nickel cobalt oxide, lithium manganese cobalt oxide, lithium nickel manganese oxide, lithium nickel cobalt manganese oxide (such as LiNi 1/3 Co 1/3 Mn 1/3 O 2 (also referred to as NCM 333 ), LiNi 0.5 Co 0.2 Mn 0.3 O 2 (can also be abbreviated to NCM 523 ), LiNi 0.5 Co 0.25 Mn 0.25 O 2 (can also be abbreviated to NCM 211 ), LiNi 0.6 Co 0.2 Mn 0.2 O 2 (can also be abbreviated to NCM 622 ), LiNi At least one of 0.8 Co 0.1 Mn 0.1 O 2 (also referred to as NCM 811 ), lithium nickel cobalt aluminum oxide (such as Li Li
  • the olivine structure contains Examples of lithium phosphates may include, but are not limited to, lithium iron phosphate (such as LiFePO 4 (also referred to as LFP)), composites of lithium iron phosphate and carbon, lithium manganese phosphate (such as LiMnPO 4 ), lithium manganese phosphate and carbon. At least one of composite materials, lithium iron manganese phosphate, and composite materials of lithium iron manganese phosphate and carbon.
  • lithium iron phosphate such as LiFePO 4 (also referred to as LFP)
  • composites of lithium iron phosphate and carbon such as LiMnPO 4
  • LiMnPO 4 lithium manganese phosphate and carbon.
  • At least one of composite materials, lithium iron manganese phosphate, and composite materials of lithium iron manganese phosphate and carbon At least one of composite materials, lithium iron manganese phosphate, and composite materials of lithium iron manganese phosphate and carbon.
  • the positive active material layer optionally further includes a binder.
  • the binder may include polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene tripolymer. At least one of a meta-copolymer, a tetrafluoroethylene-hexafluoropropylene copolymer and a fluorine-containing acrylate resin.
  • the positive active material layer optionally further includes a conductive agent.
  • the conductive agent may include at least one of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers.
  • the positive electrode sheet can be prepared in the following manner: the above-mentioned components used to prepare the positive electrode sheet, such as positive active materials, conductive agents, binders and any other components, are dispersed in a solvent (such as N-methylpyrrolidone) to form a positive electrode slurry; the positive electrode slurry is coated on the positive electrode current collector, and after drying, cold pressing and other processes, the positive electrode piece can be obtained.
  • a solvent such as N-methylpyrrolidone
  • the electrolyte plays a role in conducting ions between the positive and negative electrodes.
  • the type of electrolyte in this application can be selected according to needs.
  • the electrolyte can be liquid, gel, or completely solid.
  • the electrolyte is an electrolyte solution.
  • the electrolyte solution includes electrolyte salts and solvents.
  • the electrolyte salt may be selected from the group consisting of lithium hexafluorophosphate, lithium tetrafluoroborate, lithium perchlorate, lithium hexafluoroarsenate, lithium bisfluorosulfonimide, lithium bistrifluoromethanesulfonimide, lithium trifluoromethane At least one of lithium methanesulfonate, lithium difluorophosphate, lithium difluoroborate, lithium dioxaloborate, lithium difluorodioxalate phosphate and lithium tetrafluoroxalate phosphate.
  • the solvent may be selected from the group consisting of ethylene carbonate, propylene carbonate, methylethyl carbonate, diethyl carbonate, dimethyl carbonate, dipropyl carbonate, methylpropyl carbonate, and ethylpropyl carbonate.
  • butylene carbonate fluoroethylene carbonate, methyl formate, methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate, propyl propionate, methyl butyrate, butyric acid
  • ethyl ester 1,4-butyrolactone, sulfolane, dimethyl sulfone, methyl ethyl sulfone and diethyl sulfone.
  • the electrolyte optionally further includes additives.
  • additives may include negative electrode film-forming additives, positive electrode film-forming additives, and may also include additives that can improve certain properties of the battery, such as additives that improve battery overcharge performance, additives that improve battery high-temperature or low-temperature performance, etc.
  • the secondary battery further includes a separator film.
  • a separator film There is no particular restriction on the type of isolation membrane in this application. Any well-known porous structure isolation membrane with good chemical stability and mechanical stability can be used.
  • the material of the isolation membrane can be selected from at least one selected from the group consisting of glass fiber, non-woven fabric, polyethylene, polypropylene and polyvinylidene fluoride.
  • the isolation film can be a single-layer film or a multi-layer composite film, with no special restrictions. When the isolation film is a multi-layer composite film, the materials of each layer can be the same or different, and there is no particular limitation.
  • the positive electrode piece, the negative electrode piece, and the separator film can be formed into an electrode assembly through a winding process or a lamination process.
  • the secondary battery may include an outer packaging.
  • the outer packaging can be used to package the above-mentioned electrode assembly and electrolyte.
  • the outer packaging of the secondary battery may be a hard shell, such as a hard plastic shell, an aluminum shell, a steel shell, etc.
  • the outer packaging of the secondary battery may also be a soft bag, such as a bag-type soft bag.
  • the material of the soft bag may be plastic, and examples of the plastic include polypropylene, polybutylene terephthalate, polybutylene succinate, and the like.
  • FIG. 5 shows a square-structured secondary battery 5 as an example.
  • the outer package may include a housing 51 and a cover 53 .
  • the housing 51 may include a bottom plate and side plates connected to the bottom plate, and the bottom plate and the side plates enclose a receiving cavity.
  • the housing 51 has an opening communicating with the accommodation cavity, and the cover plate 53 can cover the opening to close the accommodation cavity.
  • the positive electrode piece, the negative electrode piece and the isolation film can be formed into the electrode assembly 52 through a winding process or a lamination process.
  • the electrode assembly 52 is packaged in the containing cavity.
  • the electrolyte soaks into the electrode assembly 52 .
  • the number of electrode assemblies 52 contained in the secondary battery 5 can be one or more, and those skilled in the art can select according to specific actual needs.
  • the secondary batteries can be assembled into battery modules, and the number of secondary batteries contained in the battery module can be one or more. The specific number can be selected by those skilled in the art according to the application and capacity of the battery module.
  • FIG. 7 shows the battery module 4 as an example.
  • a plurality of secondary batteries 5 may be arranged in sequence along the length direction of the battery module 4 .
  • the plurality of secondary batteries 5 can be fixed by fasteners.
  • the battery module 4 may further include a housing having a receiving space in which a plurality of secondary batteries 5 are received.
  • the above-mentioned battery modules can also be assembled into a battery pack.
  • the number of battery modules contained in the battery pack can be one or more. The specific number can be selected by those skilled in the art according to the application and capacity of the battery pack.
  • the battery pack 1 may include a battery box and a plurality of battery modules 4 disposed in the battery box.
  • the battery box includes an upper box 2 and a lower box 3 .
  • the upper box 2 can be covered with the lower box 3 and form a closed space for accommodating the battery module 4 .
  • Multiple battery modules 4 can be arranged in the battery box in any manner.
  • the present application also provides an electrical device, which includes at least one of the secondary battery, battery module, or battery pack provided by the present application.
  • the secondary battery, battery module, or battery pack can be used as a power source for the power-consuming device, or as an energy storage unit of the power-consuming device.
  • Electrical devices may include mobile equipment, electric vehicles, electric trains, ships and satellites, energy storage systems, etc., but are not limited to these.
  • mobile devices can be, for example, mobile phones, laptops, etc.; electric vehicles can be, for example, pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf carts, electric trucks, etc. , but not limited to this.
  • secondary batteries, battery modules or battery packs can be selected according to its usage requirements.
  • FIG. 10 shows an electrical device 6 as an example.
  • the electric device 6 is a pure electric vehicle, a hybrid electric vehicle, a plug-in hybrid electric vehicle, or the like.
  • a battery pack or battery module can be used.
  • the device may be a mobile phone, a tablet, a laptop, etc.
  • the device is usually required to be thin and light, and a secondary battery can be used as a power source.
  • holes are evenly drilled on the surface of the copper foil of the single-sided negative electrode piece that is not coated with negative electrode slurry.
  • the depth of the hole channel is equal to the thickness of the copper foil.
  • the cathode active material LiNi 0.8 Co 0.1 Mn 0.1 O 2 (can also be referred to as NCM 811 ), the conductive agent superconducting carbon and the binder polyvinylidene fluoride are mixed and dispersed in the NMP slurry in a mass ratio of 96:2:2
  • the material is coated on one side of the aluminum foil, and after drying, it is cold pressed and cut to obtain the positive electrode piece.
  • Isolation film 12 ⁇ m thick polyethylene separator, coated with 3 ⁇ m thick ceramic layer on both sides.
  • the electrolyte is 1M LiPF 6 /EC:EMC:DEC (volume ratio 1:1:1)
  • the bare cells are prepared by stacking them in the order of positive electrode piece/isolation film/double-sided negative electrode piece/isolation film/positive electrode piece. After hot pressing, the bare battery core is assembled with the top cover and shell, and then the electrolyte is injected and formed. , exhaust, sealing, testing and other processes to obtain secondary batteries.
  • Example 2 The difference between Examples 2 to 6 and Example 1 is that the thickness of the buffer layer in Examples 2 to 6 is different.
  • Example 7 to 12 The difference between Examples 7 to 12 and Example 2 is that the porosity of the buffer layer in Examples 7 to 12 is different.
  • Example 2 The difference between Examples 13 to 17 and Example 2 is that the content of the ion conductor material in the buffer layer of Examples 13 to 17 is different.
  • Example 13 the mass ratio of the ion conductor material LLZO, the conductive agent superconducting carbon, and the binder polyvinylidene fluoride is 58:32:10.
  • Example 14 the mass ratio of the ion conductor material LLZO, the conductive agent superconducting carbon, and the binder polyvinylidene fluoride is 60:30:10.
  • Example 15 the mass ratio of the ion conductor material LLZO, the conductive agent superconducting carbon, and the binder polyvinylidene fluoride is 70:20:10.
  • Example 16 the mass ratio of the ion conductor material LLZO, the conductive agent superconducting carbon, and the binder polyvinylidene fluoride is 90:5:5.
  • Example 17 the mass ratio of the ion conductor material LLZO, the conductive agent superconducting carbon, and the binder polyvinylidene fluoride is 95:2.5:2.5.
  • Embodiments 18 to 23 The difference between Embodiments 18 to 23 and Embodiment 2 is that the area ratio of the through holes on the current collector in Embodiments 18 to 23 is different.
  • Example 24 to 28 The difference between Examples 24 to 28 and Example 2 is that the diameters of the through holes in Examples 24 to 28 are different.
  • Example 29 The difference between Example 29 and Example 1 is that the ion conductor material of the buffer layer in Example 29 is different.
  • Example 30 The difference between Example 30 and Example 29 is that the porosity of the buffer layer in Example 30 is different.
  • Embodiment 31 differs.
  • Embodiment 32 differs from Embodiment 31.
  • Example 33 The difference between Example 33 and Example 32 is that the thickness of the metallic lithium layer in Example 33 is different.
  • Embodiment 34 and Embodiment 1 The difference between Embodiment 34 and Embodiment 1 is that the first buffer layer and the second buffer layer have different compositions.
  • the first buffer layer is the same as the buffer layer of Embodiment 1
  • the second buffer layer is the same as the buffer layer of Embodiment 29.
  • the layers are the same.
  • the structure of the negative electrode plate in Embodiment 35 is basically the same as that in Embodiment 1. The difference is that in Embodiment 35, the second current collector is not punched and is a copper foil without through holes; the first current collector is the same as that in Embodiment 1. Current collector.
  • Embodiments 36 to 38 are identical to Embodiments 36 to 38:
  • Examples 36 to 38 and Example 1 The difference between Examples 36 to 38 and Example 1 is that the negative active material is artificial graphite, and accordingly, the structural composition of the negative electrode sheet is also different.
  • Embodiments 39 to 41 are identical to Embodiments 39 to 41:
  • Examples 39-41 and Examples 36-38 The difference between Examples 39-41 and Examples 36-38 is that the positive active material is lithium iron phosphate (LFP), and accordingly, the structural composition of the negative electrode sheet is also different.
  • LFP lithium iron phosphate
  • Comparative Example 1 The difference between Comparative Example 1 and Example 1 is that the negative electrode piece is bonded to the copper foil used to prepare the negative electrode piece in step (1) of Example 1.
  • Comparative Example 2 The difference between Comparative Example 2 and Example 1 is that the buffer layer is omitted from the negative electrode piece.
  • Comparative Example 3 The difference between Comparative Example 3 and Example 36 is that the negative electrode sheet is bonded to the copper foil used to prepare the negative electrode sheet in step (1) of Example 7.
  • Comparative Example 4 The difference between Comparative Example 4 and Example 36 is that the buffer layer is omitted from the negative electrode piece.
  • Comparative Example 5 The difference between Comparative Example 5 and Example 39 is that the negative electrode piece is bonded to the copper foil prepared in step (1) of Example 9.
  • Comparative Example 6 The difference between Comparative Example 6 and Example 39 is that the buffer layer is omitted from the negative electrode piece.
  • first buffer layer and the second buffer layer of the negative electrode plate of the embodiment in Table 1 are the same, and the first current collector and the second current collector are the same.
  • Lithium replenishment amount test In an environment with RH ⁇ 2%, disassemble a fresh battery core, scrape a sample per unit area of the lithium replenishment layer between the two negative electrode current collectors and weigh it. Calculate the replenishment amount per unit area of the negative electrode piece. Amount of lithium.
  • Cycle performance test At 25°C, charge the lithium-ion battery to 4.25V (NCM811) or 3.65V (LFP) at a rate of 0.5C, then charge it at a constant voltage until the current is less than 0.05C, and then discharge it to 2.5V using a rate of 1C.
  • the cycle test is carried out in this form of full and full discharge until the discharge capacity of the lithium-ion battery decays to 80% of the initial capacity, and the number of cycles at this time is recorded.
  • Self-discharge voltage drop test Fully charge the battery, let it stand for 1 day, connect the positive and negative electrodes of the secondary battery through an electrochemical workstation (or multimeter), and record the open circuit voltage V1, record the open circuit voltage V2 after letting it stand for 2 days, as follows Calculate the self-discharge voltage drop in mV/h.
  • Example 1 1164 0.165
  • Example 2 1485 0.078
  • Example 3 1327 0.075
  • Example 4 1186 0.074
  • Example 5 982 0.072
  • Example 6 903 0.07
  • Example 7 1295 0.093
  • Example 8 1369 0.086
  • Example 9 1457 0.079
  • Example 10 1438 0.071
  • Example 12 1301 0.061
  • Example 13 1286 0.062 Example 14 1317 0.063
  • Example 15 1425 0.074
  • Example 16 Example 16 1352 0.093
  • Example 17 1267 0.118
  • Example 18 1173 0.058
  • Example 19 1296 0.062
  • Example 20 1425 0.066
  • Example 21 1483 0.072
  • Example 22 1251 0.149
  • Example 23 1086 0.201
  • Example 24 1579 0.057
  • Example 25 1431 0.082
  • Example 26 1309 0.095
  • Example 27 1176 0.131
  • Example 28 1042 0.173
  • Example 29 1276 0.068
  • Example 30 1193 0.065
  • Example 31 1089 0.062
  • Example 32 956 0.057
  • Example 33 904 0.056
  • Example 34 1210 0.082
  • Example 35 1134 0.146
  • Example 36 3381 0.051
  • Example 37 3176 0.049
  • Example 38 2459 0.045
  • Example 39 5493 0.038
  • Comparing Examples 1 to 35 with Comparative Example 1 it can be seen that compared with the secondary battery without a lithium replenishing layer, the cycle performance of the secondary battery of Examples 1 to 35 is significantly improved; and compared with Comparative Example 2, which does not have a buffer It can be seen from the comparison of secondary batteries with different layers that the buffer layer provided in Examples 1 to 35 can reduce the self-discharge voltage drop of the secondary battery and prevent the lithium supplement layer from depositing lithium on the surface of the negative electrode plate, causing a micro short circuit, thus preventing secondary Battery deterioration, cycle performance is better.
  • the porosity of the buffer layer in Examples 7 to 12 is different from that in Example 2. Different porosity of the buffer layer will affect the self-discharge voltage drop and the number of cycles of the secondary battery. The number of cycles in Example 2 and Examples 9 and 10 is relatively different. Most of them are above 1400. It can be seen that controlling the porosity of the buffer layer between 20% and 40% will have a better effect on improving the cycle life of the secondary battery.
  • the buffer layer ion conductor material content in Examples 13 to 17 is different from that in Example 2. It can be seen from the data in Table 2 that the secondary battery has better cycle performance when the buffer material mass content is 70% to 80%.
  • the area ratio of the through holes on the current collector in Examples 18 to 23 is different from that in Example 2.
  • the through hole area ratio of Examples 22 to 23 is 20% to 30%, the lithium replenishment rate is faster, and the self-discharge voltage drop is higher than that of Examples 2 and 18 to 21.
  • the through hole area ratio of Example 18 is 0.1%, the lithium replenishment rate is slow, the self-discharge voltage drop is small, but the number of cycles is smaller than that of Examples 2 and 19-22. Therefore, the through-hole area ratio is 2% to 15%, and the secondary battery cycle performance is better.
  • Examples 24 to 28 are different from Example 2 in the diameter of the through holes. It can be seen from the data in Table 2 that the secondary battery cycle performance is better when the through hole diameter is 30 ⁇ m ⁇ 200 ⁇ m.
  • the battery systems of Examples 36 to 38 and 38 to 41 are different from those of Examples 1 to 35.
  • the secondary batteries of Examples 36 to 41 It has a low self-discharge voltage drop, which can prevent the lithium replenishment layer from depositing lithium on the surface of the negative electrode sheet, causing micro short circuit, thereby avoiding the deterioration of the secondary battery and having a better cycle life.

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  • Engineering & Computer Science (AREA)
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Abstract

La présente invention concerne une plaque d'électrode négative, comprenant une première couche de matériau actif négatif, un premier collecteur de courant, une couche de supplément de lithium, un second collecteur de courant et une seconde couche de matériau actif négatif, qui sont empilés en séquence, la plaque d'électrode négative comprenant en outre un matériau tampon ; au moins l'un du premier collecteur de courant et du second collecteur de courant étant pourvu d'un trou traversant ; et le matériau tampon étant rempli dans le trou traversant du premier collecteur de courant et/ou le trou traversant du second collecteur de courant.
PCT/CN2022/110769 2022-08-08 2022-08-08 Plaque d'électrode négative et son procédé de préparation, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique WO2024031216A1 (fr)

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PCT/CN2022/110769 WO2024031216A1 (fr) 2022-08-08 2022-08-08 Plaque d'électrode négative et son procédé de préparation, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique

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JP2010027891A (ja) * 2008-07-22 2010-02-04 Meidensha Corp 電気化学素子
CN103022413A (zh) * 2012-12-28 2013-04-03 东莞新能源科技有限公司 锂电池用负极片及其制备方法及包含该负极片的锂电池
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