WO2021189406A1 - Dispositif électrochimique et dispositif électronique - Google Patents

Dispositif électrochimique et dispositif électronique Download PDF

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WO2021189406A1
WO2021189406A1 PCT/CN2020/081608 CN2020081608W WO2021189406A1 WO 2021189406 A1 WO2021189406 A1 WO 2021189406A1 CN 2020081608 W CN2020081608 W CN 2020081608W WO 2021189406 A1 WO2021189406 A1 WO 2021189406A1
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active material
negative electrode
electrochemical device
negative
ppm
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PCT/CN2020/081608
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English (en)
Chinese (zh)
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杜鹏
谢远森
董佳丽
范国凌
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宁德新能源科技有限公司
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Priority to PCT/CN2020/081608 priority Critical patent/WO2021189406A1/fr
Priority to CN202080098111.4A priority patent/CN115280567A/zh
Publication of WO2021189406A1 publication Critical patent/WO2021189406A1/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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • 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
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • 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
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • This application relates to the field of energy storage, in particular to an electrochemical device and an electronic device.
  • Electrochemical devices for example, lithium-ion batteries
  • Small-sized lithium-ion batteries are generally used as power sources for driving portable electronic communication devices (for example, camcorders, mobile phones, or notebook computers, etc.), especially high-performance portable devices.
  • portable electronic communication devices for example, camcorders, mobile phones, or notebook computers, etc.
  • medium-sized and large-sized lithium-ion batteries with high output characteristics have been developed for use in electric vehicles (EV) and large-scale energy storage systems (ESS).
  • EV electric vehicles
  • ESS large-scale energy storage systems
  • Improving the active material in the electrode is one of the research directions to solve the above problems.
  • this application attempts to solve at least one problem existing in the related field at least to some extent.
  • the present application provides an electrochemical device, which includes a positive electrode, a negative electrode, and an electrolyte, wherein the negative electrode includes a negative electrode current collector and a negative electrode active material layer disposed on the negative electrode current collector, so
  • the anode active material layer includes an anode active material
  • the anode active material includes crushed particles
  • a particle crushing rate of the anode active material is 20% to 80%.
  • the particle crushing rate of the negative active material is 30% to 60%.
  • the particle crushing rate of the negative active material is 40% to 50%.
  • the particle crushing rate of the negative active material is 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%. % Or 80%.
  • the broken particles have cracks or cracks with a width not greater than 4 ⁇ m. In some embodiments, the broken particles have cracks or cracks with a width not greater than 3.5 ⁇ m. In some embodiments, the broken particles have cracks or cracks with a width not greater than 2.5 ⁇ m. In some embodiments, the broken particles have cracks or cracks with a width not greater than 2 ⁇ m.
  • the roughness of the negative active material layer is not more than 6 ⁇ m. In some embodiments, the roughness of the negative active material layer is not greater than 5 ⁇ m. In some embodiments, the roughness of the negative active material layer is not more than 3 ⁇ m. In some embodiments, the roughness of the negative active material layer is not more than 1 ⁇ m. In some embodiments, the roughness of the negative active material layer is 0.5 ⁇ m, 1 ⁇ m, 2 ⁇ m, 3 ⁇ m, 4 ⁇ m, 5 ⁇ m, or 6 ⁇ m.
  • the cohesive strength of the negative active material is 5 N/m to 30 N/m. In some embodiments, the cohesive strength of the negative active material is 8N/m to 25N/m. In some embodiments, the cohesive strength of the negative active material is 5N/m, 10N/m, 15N/m, 20N/m, 25N/m, or 30N/m.
  • the binding force between the negative active material layer and the negative current collector is 5 N/m to 20 N/m. In some embodiments, the binding force between the negative active material layer and the negative current collector is 10 N/m to 15 N/m. In some embodiments, the binding force between the negative active material layer and the negative current collector is 5N/m, 8N/m, 10N/m, 12N/m, 14N/m, 16N/m, 18N. /m or 20N/m.
  • the half-height width Id of the peak appearing at 1345 cm -1 to 1355 cm -1 of the negative electrode active material measured by Raman spectroscopy and the peak appearing at 1595 cm -1 to 1605 cm -1 The ratio Id/Ig of the half-height peak width Ig is 0.7 to 1.5.
  • the Id/Ig of the negative active material measured by Raman spectroscopy is 1.0 to 1.2.
  • the Id/Ig of the negative active material measured by Raman spectroscopy is 0.7, 0.8, 0.9, 1.0, 1.1, 1.2, 1.3, 1.4, or 1.5.
  • the Id is 200 cm -1 to 1100 cm -1 . In some embodiments, Id of 2200cm -1 to 1000cm -1. In some embodiments, the Id is 2500 cm -1 to 900 cm -1 . In some embodiments, Id is 200cm -11, 300cm -1, 400cm -1 , 500cm -1, 550cm -1, 600cm -1, 700cm -1, 850cm -1, 900cm -1, 1000cm -1, 1100cm - 1 .
  • the negative active material includes at least one of a metal element or a non-metal element
  • the metal element includes gold, silver, platinum, zirconium, zinc, magnesium, calcium, barium, vanadium, iron, or At least one of aluminum, based on the total weight of the negative active material, the content of the metal element is 20 ppm to 400 ppm
  • the non-metal element includes at least one of phosphorus, boron, silicon, arsenic or selenium, based on The total weight of the negative active material and the content of the non-metal elements are 50 ppm to 400 ppm.
  • the content of the metal element is 50 ppm to 300 ppm based on the total weight of the negative active material. In some embodiments, based on the total weight of the negative active material, the content of the metal element is 100 ppm to 200 ppm. In some embodiments, based on the total weight of the negative active material, the content of the metal element is 20 ppm, 50 ppm, 80 ppm, 100 ppm, 150 ppm, 200 ppm, 250 ppm, 300 ppm, 350 ppm, or 400 ppm.
  • the content of the non-metal elements is 100 ppm to 350 ppm based on the total weight of the negative active material. In some embodiments, based on the total weight of the negative active material, the content of the non-metal elements is 50 ppm, 60 ppm, 70 ppm, 80 ppm, 90 ppm, 100 ppm, 110 ppm, 120 ppm, 130 ppm, 140 ppm, 150 ppm, 160 ppm, 170 ppm, 180ppm, 190ppm, 210ppm, 240ppm, 280ppm, 310ppm, 380ppm or 400ppm.
  • the negative active material has pores, the pore diameter of the pores is not greater than 3 ⁇ m, and the inner wall of the pores has the metal element.
  • the negative electrode active material has pores, the pore diameter of the pores is not greater than 3 ⁇ m, and the inner wall of the pores has the non-metallic element.
  • the hole diameter is not greater than 2.5 ⁇ m. In some embodiments, the pore diameter of the pores is not greater than 2 ⁇ m. In some embodiments, the pore diameter of the hole is not greater than 1.5 ⁇ m. In some embodiments, the pore diameter is 0.5 ⁇ m, 1 ⁇ m, 1.5 ⁇ m, 2 ⁇ m, 2.5 ⁇ m, or 3 ⁇ m.
  • the anode current collector includes a region where the anode active material layer is not provided, and based on the total area of the anode current collector, the region where the anode active material layer is not provided does not exceed 10%. In some embodiments, based on the total area of the negative electrode current collector, the area where the negative electrode active material layer is not provided does not exceed 8%. In some embodiments, based on the total area of the negative electrode current collector, the area where the negative electrode active material layer is not provided does not exceed 5%. In some embodiments, based on the total area of the negative electrode current collector, the area where the negative electrode active material layer is not provided does not exceed 3%. In some embodiments, based on the total area of the negative electrode current collector, the area where the negative electrode active material layer is not provided is 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8% , 9% or 10%.
  • the present application provides an electronic device, which includes the electrochemical device according to the present application.
  • Fig. 1 is a scanning electron microscope (SEM) image of a negative active material with crushed particles according to an embodiment of the present application.
  • a list of items connected by the term "at least one of” can mean any combination of the listed items. For example, if items A and B are listed, then the phrase "at least one of A and B" means only A; only B; or A and B. In another example, if items A, B, and C are listed, then the phrase "at least one of A, B, and C" means only A; or only B; only C; A and B (excluding C); A and C (exclude B); B and C (exclude A); or all of A, B, and C.
  • Project A can contain a single element or multiple elements.
  • Project B can contain a single element or multiple elements.
  • Project C can contain a single element or multiple elements.
  • pore refers to a pore structure or pore structure in a single negative electrode active material particle.
  • pores refer to voids between a plurality of particles of the negative active material.
  • particle crushing rate refers to the percentage of the number of crushed particles in the negative active material to the total number of negative active material particles.
  • the active materials of the electrodes is one of the research directions.
  • the upper limit of the theoretical electrochemical capacity of the graphitized negative active material is 372 mAh/g, and it is difficult for the electrochemical capacity of the previously known graphitized negative active material to break through this upper limit.
  • the silicon anode active material has a high electrochemical capacity. With the increase in the content of the doped material in the silicon anode active material, the energy density of the electrochemical device can be significantly improved, but the anode active material will undergo significant volume expansion, which will decrease significantly. The performance of the electrochemical device, in particular, will significantly reduce the capacity retention rate during long cycles.
  • an electrochemical device which includes a positive electrode, a negative electrode, and an electrolyte, wherein the negative electrode includes a negative electrode current collector and a negative electrode active material layer disposed on the negative electrode current collector.
  • the active material layer contains a negative active material that contains a certain amount of crushed particles.
  • the particle crushing rate of the anode active material is 20% to 80%. In some embodiments, the particle crushing rate of the negative active material is 30% to 60%. In some embodiments, the particle crushing rate of the negative active material is 40% to 50%. In some embodiments, the particle crushing rate of the negative active material is 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%. % Or 80%.
  • the crushed particles can increase the specific surface area of the negative electrode active material and increase the contact points between the negative electrode active material and the electrolyte, thereby improving the cycle performance and energy density of the electrochemical device.
  • the broken particles have cracks or cracks with a width not greater than 4 ⁇ m. In some embodiments, the broken particles have cracks or cracks with a width not greater than 3.5 ⁇ m. In some embodiments, the broken particles have cracks or cracks with a width not greater than 2.5 ⁇ m. In some embodiments, the broken particles have cracks or cracks with a width not greater than 2 ⁇ m.
  • Figure 1 shows a scanning electron microscope (SEM) image of a negative active material with broken particles. The particles circled in solid circles are broken particles with cracks, and those circled in dotted circles are broken particles with cracks.
  • the roughness of the negative active material layer is not more than 6 ⁇ m. In some embodiments, the roughness of the negative active material layer is not greater than 5 ⁇ m. In some embodiments, the roughness of the negative active material layer is not more than 3 ⁇ m. In some embodiments, the roughness of the negative active material layer is not more than 1 ⁇ m. In some embodiments, the roughness of the negative active material layer is 0.5 ⁇ m, 1 ⁇ m, 2 ⁇ m, 3 ⁇ m, 4 ⁇ m, 5 ⁇ m, or 6 ⁇ m.
  • the negative active material layer is formed by randomly arranging negative active material particles, and its surface roughness depends on the unevenness of the particles with small spacing and minute peaks and valleys on the surface.
  • the roughness of the negative active material layer can be obtained by the following method: within the sampling length, the arithmetic mean of the absolute value of the distance from the point on the particle profile to the reference line is calculated, that is, the profile arithmetic mean deviation Ra.
  • the profile arithmetic mean deviation Ra The smaller the Ra, the smaller the roughness of the negative electrode active material layer, and the smoother the negative electrode active material layer.
  • the cohesive strength of the negative active material is 5 N/m to 30 N/m. In some embodiments, the cohesive strength of the negative active material is 8N/m to 25N/m. In some embodiments, the cohesive strength of the negative active material is 5N/m, 10N/m, 15N/m, 20N/m, 25N/m, or 30N/m. The presence of broken particles invalidates the contact sites of part of the active material and the binder, thereby reducing the cohesive strength of the negative active material. When the cohesive strength of the negative electrode active material is within the above range, the particles of the negative electrode active material have proper adhesion, which can avoid the phenomenon of powder falling during the rolling and winding process, and avoid the formation of the inside of the lithium ion battery.
  • the negative active material can also expand in volume during the charge and discharge process to avoid incomplete lithium insertion, thereby ensuring the capacity of the electrochemical device.
  • the cohesive strength of the negative electrode active material can be tested with the Instron (model 33652) tester: take the negative electrode sheet (width 30mm, length 100-160mm), use double-sided adhesive paper (model: 3M9448A, width 20mm, length (90-150mm) fix it on the steel plate, stick the adhesive tape on the surface of the negative active material layer, connect one side of the adhesive tape to the paper tape of equal width, adjust the limit block of the tensile machine to a suitable position, and attach the tape Folding and sliding up 40mm, the sliding rate was 50mm/min, and the polymerization strength between the particles in the negative active material layer was tested at 180° (that is, stretched in the opposite direction).
  • the binding force between the negative active material layer and the negative current collector is 5 N/m to 20 N/m. In some embodiments, the binding force between the negative active material layer and the negative current collector is 10 N/m to 15 N/m. In some embodiments, the binding force between the negative active material layer and the negative current collector is 5N/m, 8N/m, 10N/m, 12N/m, 14N/m, 16N/m, 18N. /m or 20N/m.
  • the binding force between the negative electrode active material layer and the negative electrode current collector is within the above range, it is possible to avoid film peeling or burrs during the rolling or slitting process, thereby avoiding potential safety hazards and ensuring the battery core
  • the internal resistance is within an acceptable range to ensure the dynamic performance and cycle performance of the electrochemical device.
  • the peeling strength between the negative electrode active material layer and the negative electrode current collector can be achieved by controlling the rolling process in the preparation process of the negative electrode.
  • the binding force between the negative electrode active material layer and the negative electrode current collector can be tested using an Instron (model 33652) tester: take the pole piece (width 30mm, length 100-160mm), use double-sided adhesive tape (Model: 3M9448A, width 20mm, length 90-150mm) Fix it on the steel plate, stick the adhesive tape on the surface of the negative active material layer, connect one side of the adhesive tape to the paper tape of equal width, adjust the tension machine Place the limit block to a suitable position, fold the paper tape upwards and slide it 40mm, with a slip rate of 50mm/min, and test the adhesion between the negative electrode active material layer and the negative electrode current collector at 180° (ie, stretching in the opposite direction) Knot force.
  • Instron model 33652
  • the half-height width Id of the peak appearing at 1345 cm -1 to 1355 cm -1 of the negative electrode active material measured by Raman spectroscopy and the peak appearing at 1595 cm -1 to 1605 cm -1 The ratio Id/Ig of the half-height peak width Ig is 0.7 to 1.5.
  • the Id/Ig of the negative active material measured by Raman spectroscopy is 1.0 to 1.2.
  • the Id/Ig of the negative active material measured by Raman spectroscopy is 0.7, 0.8, 0.9, 1.0, 1.1, 1.2, 1.3, 1.4, or 1.5.
  • the Id is 200 cm -1 to 1100 cm -1 . In some embodiments, Id of 2200cm -1 to 1000cm -1. In some embodiments, the Id is 2500 cm -1 to 900 cm -1 . In some embodiments, Id as 200cm -1, 300cm -1, 400cm -1 , 500cm -1, 550cm -1, 600cm -1, 700cm -1, 850cm -1, 900cm -1, 1000cm -1, 1100cm - 1 .
  • the negative active material includes at least one of a metal element or a non-metal element
  • the metal element includes gold, silver, platinum, zirconium, zinc, magnesium, calcium, barium, vanadium, iron, or At least one of aluminum, based on the total weight of the negative active material, the content of the metal element is 20 ppm to 400 ppm
  • the non-metal element includes at least one of phosphorus, boron, silicon, arsenic or selenium, based on The total weight of the negative active material and the content of the non-metal elements are 50 ppm to 400 ppm.
  • the content of the metal element is 50 ppm to 300 ppm based on the total weight of the negative active material. In some embodiments, based on the total weight of the negative active material, the content of the metal element is 100 ppm to 200 ppm. In some embodiments, based on the total weight of the negative active material, the content of the metal element is 20 ppm, 50 ppm, 80 ppm, 100 ppm, 150 ppm, 200 ppm, 250 ppm, 300 ppm, 350 ppm or 400 ppm.
  • the content of the non-metal elements is 100 ppm to 350 ppm based on the total weight of the negative active material. In some embodiments, based on the total weight of the negative active material, the content of the non-metal elements is 50 ppm, 60 ppm, 70 ppm, 80 ppm, 90 ppm, 100 ppm, 110 ppm, 120 ppm, 130 ppm, 140 ppm, 150 ppm, 160 ppm, 170 ppm, 180ppm, 190ppm, 210ppm, 240ppm, 280ppm, 310ppm, 380ppm or 400ppm.
  • the negative active material has pores, the pore diameter of the pores is not greater than 3 ⁇ m, and the inner wall of the pores has the metal element.
  • the negative electrode active material has pores, the pore diameter of the pores is not greater than 3 ⁇ m, and the inner wall of the pores has the non-metallic element.
  • the hole diameter is not greater than 2 ⁇ m. In some embodiments, the pore diameter of the hole is not greater than 1 ⁇ m. In some embodiments, the pore diameter of the hole is not greater than 0.5 ⁇ m. In some embodiments, the pore diameter is 0.5 ⁇ m, 1 ⁇ m, 1.5 ⁇ m, 2 ⁇ m, 2.5 ⁇ m, or 3 ⁇ m.
  • the negative electrode active material with pores has a larger specific surface area, and the inner wall of the pores can effectively adsorb lithium, which helps to increase the electrochemical capacity of the negative electrode active material. When the pore diameter is within the above range, the electrolyte can effectively infiltrate the negative electrode active material to form a solid-liquid interface.
  • the anode current collector includes a region where the anode active material layer is not provided, and based on the total area of the anode current collector, the region where the anode active material layer is not provided does not exceed 10%. In some embodiments, based on the total area of the negative electrode current collector, the area where the negative electrode active material layer is not provided does not exceed 8%. In some embodiments, based on the total area of the negative electrode current collector, the area where the negative electrode active material layer is not provided does not exceed 5%. In some embodiments, based on the total area of the negative electrode current collector, the area where the negative electrode active material layer is not provided does not exceed 3%. In some embodiments, based on the total area of the negative electrode current collector, the area where the negative electrode active material layer is not provided is 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8% , 9% or 10%.
  • the negative active material may include, but is not limited to, natural graphite, artificial graphite, mesophase carbon microspheres (referred to as MCMB for short), hard carbon, soft carbon, silicon, silicon-carbon composite, Li-Sn Alloy, Li-Sn-O alloy, Sn, SnO, SnO 2 , spinel structure lithiated TiO 2 -Li 4 Ti 5 O 12 or LI-l alloy.
  • Non-limiting examples of carbon materials include crystalline carbon, amorphous carbon, and mixtures thereof.
  • the crystalline carbon may be amorphous or flake-shaped, flake-shaped, spherical or fibrous natural graphite or artificial graphite.
  • Amorphous carbon can be soft carbon, hard carbon, mesophase pitch carbide, calcined coke, and the like.
  • the negative electrode further includes a conductive layer.
  • the conductive material of the conductive layer may include any conductive material as long as it does not cause a chemical change.
  • conductive materials include carbon-based materials (e.g., natural graphite, artificial graphite, carbon black, acetylene black, Ketjen black, carbon fibers, carbon nanotubes, graphene, etc.), metal-based materials (e.g., metal Powder, metal fibers, etc., such as copper, nickel, aluminum, silver, etc.), conductive polymers (e.g., polyphenylene derivatives), and mixtures thereof.
  • the negative electrode further includes a binder, and the binder is selected from at least one of the following: polyvinyl alcohol, carboxymethyl cellulose, hydroxypropyl cellulose, and diacetyl cellulose , Polyvinyl chloride, carboxylated polyvinyl chloride, polyvinyl fluoride, ethylene oxide-containing polymers, polyvinylpyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, poly Propylene, styrene butadiene rubber, acrylic (ester) styrene butadiene rubber, epoxy resin or nylon, etc.
  • the binder is selected from at least one of the following: polyvinyl alcohol, carboxymethyl cellulose, hydroxypropyl cellulose, and diacetyl cellulose , Polyvinyl chloride, carboxylated polyvinyl chloride, polyvinyl fluoride, ethylene oxide-containing polymers, polyvinylpyrrolidone
  • the negative electrode current collector used in the present application may be selected from copper foil, nickel foil, stainless steel foil, titanium foil, foamed nickel, foamed copper, polymer substrates coated with conductive metals, and combinations thereof.
  • the positive electrode includes a positive electrode current collector and a positive electrode active material provided on the positive electrode current collector.
  • the specific types of positive electrode active materials are not subject to specific restrictions, and can be selected according to requirements.
  • the positive electrode active material includes a positive electrode material capable of absorbing and releasing lithium (Li).
  • positive electrode materials capable of absorbing/releasing lithium (Li) may include lithium cobalt oxide, lithium nickel cobalt manganate, lithium nickel cobalt aluminate, lithium manganate, lithium iron manganese phosphate, lithium vanadium phosphate, lithium vanadyl phosphate, and phosphoric acid. Lithium iron, lithium titanate and lithium-rich manganese-based materials.
  • the chemical formula of lithium cobalt oxide can be as chemical formula 1:
  • M1 represents selected from nickel (Ni), manganese (Mn), magnesium (Mg), aluminum (A1), boron (B), titanium (Ti), vanadium (V), chromium (Cr), iron (Fe), Copper (Cu), zinc (Zn), molybdenum (Mo), tin (Sn), calcium (Ca), strontium (Sr), tungsten (W), yttrium (Y), lanthanum (La), zirconium (Zr) and For at least one of silicon (Si), the values of x, a, b, and c are within the following ranges: 0.8 ⁇ x ⁇ 1.2, 0.8 ⁇ a ⁇ 1, 0 ⁇ b ⁇ 0.2, -0.1 ⁇ c ⁇ 0.2.
  • the chemical formula of lithium nickel cobalt manganate or lithium nickel cobalt aluminate can be as chemical formula 2:
  • M2 represents selected from cobalt (Co), manganese (Mn), magnesium (Mg), aluminum (Al), boron (B), titanium (Ti), vanadium (V), chromium (Cr), iron (Fe), At least one of copper (Cu), zinc (Zn), molybdenum (Mo), tin (Sn), calcium (Ca), strontium (Sr), tungsten (W), zirconium (Zr), and silicon (Si),
  • the values of y, d, e, and f are in the following ranges: 0.8 ⁇ y ⁇ 1.2, 0.3 ⁇ d ⁇ 0.98, 0.02 ⁇ e ⁇ 0.7, -0.1 ⁇ f ⁇ 0.2.
  • the chemical formula of lithium manganate can be as chemical formula 3:
  • M3 represents selected from cobalt (Co), nickel (Ni), magnesium (Mg), aluminum (Al), boron (B), titanium (Ti), vanadium (V), chromium (Cr), iron (Fe), At least one of copper (Cu), zinc (Zn), molybdenum (Mo), tin (Sn), calcium (Ca), strontium (Sr) and tungsten (W), with z, g and h values in the following ranges respectively Inner: 0.8 ⁇ z ⁇ 1.2, 0 ⁇ g ⁇ 1.0 and -0.2 ⁇ h ⁇ 0.2.
  • the weight of the positive electrode active material layer is 1.5 to 15 times the weight of the negative electrode active material layer. In some embodiments, the weight of the positive active material layer is 3 to 10 times the weight of the negative active material layer. In some embodiments, the weight of the positive active material layer is 5 to 8 times the weight of the negative active material layer. In some embodiments, the weight of the positive active material layer is 1.5 times, 2 times, 3 times, 4 times, 5 times, 6 times, 7 times, 8 times, 9 times the weight of the negative active material layer. , 10 times, 11 times, 12 times, 13 times, 14 times or 15 times.
  • the positive active material layer may have a coating on the surface, or may be mixed with another compound having a coating.
  • the coating may include oxides of coating elements, hydroxides of coating elements, oxyhydroxides of coating elements, oxycarbonates of coating elements, and hydroxycarbonates of coating elements ( At least one coating element compound selected from hydroxycarbonate).
  • the compound used for the coating may be amorphous or crystalline.
  • the coating element contained in the coating may include Mg, Al, Co, K, Na, Ca, Si, Ti, V, Sn, Ge, Ga, B, As, Zr, F, or a mixture thereof.
  • the coating can be applied by any method as long as the method does not adversely affect the performance of the positive electrode active material.
  • the method may include any coating method well-known to those of ordinary skill in the art, such as spraying, dipping, and the like.
  • the positive active material layer further includes a binder, and optionally further includes a positive conductive material.
  • the binder can improve the binding of the positive electrode active material particles to each other, and also improve the binding of the positive electrode active material to the current collector.
  • binders include polyvinyl alcohol, hydroxypropyl cellulose, diacetyl cellulose, polyvinyl chloride, carboxylated polyvinyl chloride, polyvinyl fluoride, ethylene oxide-containing polymers, polyvinyl chloride Vinylpyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, styrene butadiene rubber, acrylic (ester) styrene butadiene rubber, epoxy resin, nylon, etc.
  • the positive electrode active material layer includes a positive electrode conductive material, thereby imparting conductivity to the electrode.
  • the positive electrode conductive material may include any conductive material as long as it does not cause a chemical change.
  • Non-limiting examples of positive electrode conductive materials include carbon-based materials (e.g., natural graphite, artificial graphite, carbon black, acetylene black, Ketjen black, carbon fiber, etc.), metal-based materials (e.g., metal powder, metal fiber, etc., Including, for example, copper, nickel, aluminum, silver, etc.), conductive polymers (for example, polyphenylene derivatives), and mixtures thereof.
  • the positive electrode current collector used in the electrochemical device according to the present application may be aluminum (Al), but is not limited thereto.
  • the electrolyte that can be used in the embodiments of the present application may be an electrolyte known in the prior art.
  • the electrolyte that can be used in the electrolyte in the embodiments of the present application includes, but is not limited to: inorganic lithium salts, such as LiClO 4 , LiAsF 6 , LiPF 6 , LiBF 4 , LiSbF 6 , LiSO 3 F, LiN(FSO 2 ) 2, etc.; Fluorine-containing organic lithium salts, such as LiCF 3 SO 3 , LiN(FSO 2 )(CF 3 SO 2 ), LiN(CF 3 SO 2 ) 2 , LiN(C 2 F 5 SO 2 ) 2 , cyclic 1,3- Lithium hexafluoropropane disulfonimide, lithium cyclic 1,2-tetrafluoroethane disulfonimide, LiN (CF 3 SO 2 ) (C 4 F 9 SO 2 ), LiC (CF 3 SO 2 ) 3.
  • inorganic lithium salts such as LiClO 4 , LiAsF 6 , LiPF 6 , Li
  • Lithium salt containing dicarboxylic acid complex such as bis(oxalato) lithium borate, difluorooxalic acid Lithium borate, tris(oxalato) lithium phosphate, diflu
  • the electrolyte includes a combination of LiPF 6 and LiBF 4.
  • the electrolyte includes a combination of an inorganic lithium salt such as LiPF 6 or LiBF 4 and a fluorine-containing organic lithium salt such as LiCF 3 SO 3 , LiN(CF 3 SO 2 ) 2 , and LiN(C 2 F 5 SO 2 ) 2 .
  • the electrolyte includes LiPF 6 .
  • the concentration of the electrolyte is in the range of 0.8-3 mol/L, for example, in the range of 0.8-2.5 mol/L, in the range of 0.8-2 mol/L, in the range of 1-2 mol/L, for example It is 1mol/L, 1.15mol/L, 1.2mol/L, 1.5mol/L, 2mol/L or 2.5mol/L.
  • Solvents that can be used in the electrolyte of the embodiments of the present application include, but are not limited to: carbonate compounds, ester-based compounds, ether-based compounds, ketone-based compounds, alcohol-based compounds, aprotic solvents, or combinations thereof.
  • carbonate compounds include, but are not limited to, linear carbonate compounds, cyclic carbonate compounds, fluorocarbonate compounds, or combinations thereof.
  • chain carbonate compounds include, but are not limited to, diethyl carbonate (DEC), dimethyl carbonate (DMC), dipropyl carbonate (DPC), methyl propyl carbonate (MPC), ethylene propyl carbonate ( EPC), ethyl methyl carbonate (MEC) and their combinations.
  • DEC diethyl carbonate
  • DMC dimethyl carbonate
  • DPC dipropyl carbonate
  • MEC methyl propyl carbonate
  • EPC ethylene propyl carbonate
  • MEC ethyl methyl carbonate
  • cyclic carbonate compound are ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), vinyl ethylene carbonate (VEC), and combinations thereof.
  • fluorocarbonate compound examples include fluoroethylene carbonate (FEC), 1,2-difluoroethylene carbonate, 1,1-difluoroethylene carbonate, 1,1,2-trifluoroethylene carbonate Fluoroethylene, 1,1,2,2-tetrafluoroethylene carbonate, 1-fluoro-2-methylethylene carbonate, 1-fluoro-1-methylethylene carbonate, 1,2 carbonate -Difluoro-1-methylethylene, 1,1,2-trifluoro-2-methylethylene carbonate, trifluoromethylethylene carbonate, and combinations thereof.
  • FEC fluoroethylene carbonate
  • 1,2-difluoroethylene carbonate 1,1-difluoroethylene carbonate
  • 1,1,2-trifluoroethylene carbonate Fluoroethylene, 1,1,2,2-tetrafluoroethylene carbonate, 1-fluoro-2-methylethylene carbonate, 1-fluoro-1-methylethylene carbonate, 1,2 carbonate -Difluoro-1-methylethylene, 1,1,2-trifluoro-2-methylethylene carbonate, trifluor
  • ester-based compounds include, but are not limited to, methyl acetate, ethyl acetate, n-propyl acetate, tert-butyl acetate, methyl propionate, ethyl propionate, ⁇ -butyrolactone, decanolide, Valerolactone, mevalonolactone, caprolactone, methyl formate, and combinations thereof.
  • ether-based compounds include, but are not limited to, dibutyl ether, tetraglyme, diglyme, 1,2-dimethoxyethane, 1,2-diethoxyethane Alkanes, ethoxymethoxyethane, 2-methyltetrahydrofuran, tetrahydrofuran, and combinations thereof.
  • ketone-based compounds include, but are not limited to, cyclohexanone.
  • alcohol-based compounds include, but are not limited to, ethanol and isopropanol.
  • aprotic solvents include, but are not limited to, dimethyl sulfoxide, 1,2-dioxolane, sulfolane, methyl sulfolane, 1,3-dimethyl-2-imidazolidinone, N-methyl- 2-pyrrolidone, formamide, dimethylformamide, acetonitrile, nitromethane, trimethyl phosphate, triethyl phosphate, trioctyl phosphate, and phosphate esters and combinations thereof.
  • a separator is provided between the positive electrode and the negative electrode to prevent short circuits.
  • the material and shape of the isolation film that can be used in the embodiments of the present application are not particularly limited, and they can be any technology disclosed in the prior art.
  • the isolation membrane includes a polymer or an inorganic substance formed of a material that is stable to the electrolyte of the present application, or the like.
  • the isolation film may include a substrate layer and a surface treatment layer.
  • the substrate layer is a non-woven fabric, film or composite film with a porous structure, and the material of the substrate layer is selected from at least one of polyethylene, polypropylene, polyethylene terephthalate and polyimide.
  • a polypropylene porous film, a polyethylene porous film, a polypropylene non-woven fabric, a polyethylene non-woven fabric, or a polypropylene-polyethylene-polypropylene porous composite film can be selected.
  • the porous structure can improve the heat resistance, oxidation resistance and electrolyte infiltration performance of the isolation membrane, and enhance the adhesion between the isolation membrane and the pole piece.
  • a surface treatment layer is provided on at least one surface of the substrate layer.
  • the surface treatment layer may be a polymer layer or an inorganic substance layer, or a layer formed by a mixed polymer and an inorganic substance.
  • the inorganic layer includes inorganic particles and a binder.
  • the inorganic particles are selected from alumina, silica, magnesium oxide, titanium oxide, hafnium dioxide, tin oxide, ceria, nickel oxide, zinc oxide, calcium oxide, zirconium oxide, One or a combination of yttrium oxide, silicon carbide, boehmite, aluminum hydroxide, magnesium hydroxide, calcium hydroxide, and barium sulfate.
  • the binder is selected from polyvinylidene fluoride, vinylidene fluoride-hexafluoropropylene copolymer, polyamide, polyacrylonitrile, polyacrylate, polyacrylic acid, polyacrylate, polyvinylpyrrolidone, polyvinyl ether, One or a combination of polymethyl methacrylate, polytetrafluoroethylene and polyhexafluoropropylene.
  • the polymer layer contains a polymer, and the material of the polymer is selected from polyamide, polyacrylonitrile, acrylate polymer, polyacrylic acid, polyacrylate, polyvinylpyrrolidone, polyvinyl ether, polyvinylidene fluoride, poly At least one of (vinylidene fluoride-hexafluoropropylene).
  • the present application also provides an electrochemical device, which includes a positive electrode, an electrolyte, and a negative electrode.
  • the positive electrode includes a positive electrode active material layer and a positive electrode current collector.
  • the negative electrode includes a negative electrode active material layer and a negative electrode current collector.
  • the material layer includes the negative active material according to the present application.
  • the electrochemical device of the present application includes any device that undergoes an electrochemical reaction, and specific examples thereof include all kinds of primary batteries, secondary batteries, fuel cells, solar cells, or capacitors.
  • the electrochemical device is a lithium secondary battery, including a lithium metal secondary battery, a lithium ion secondary battery, a lithium polymer secondary battery, or a lithium ion polymer secondary battery.
  • the application also provides an electronic device, which includes the electrochemical device according to the application.
  • the use of the electrochemical device of the present application is not particularly limited, and it can be used in any electronic device known in the prior art.
  • the electrochemical device of the present application can be used in, but not limited to, notebook computers, pen-input computers, mobile computers, e-book players, portable phones, portable fax machines, portable copiers, portable printers, and headsets.
  • Stereo headsets video recorders, LCD TVs, portable cleaners, portable CD players, mini discs, transceivers, electronic notebooks, calculators, memory cards, portable recorders, radios, backup power supplies, motors, cars, motorcycles, power assistance Bicycles, bicycles, lighting equipment, toys, game consoles, clocks, power tools, flashlights, cameras, large household storage batteries and lithium-ion capacitors, etc.
  • the same amount of hydrochloric acid as zinc acetate is added to the zinc oxide sol-gel solution to obtain a second solution. 1000 mL of the second solution was added to the first solution, and stirring was continued at 50° C. for 90 minutes to obtain the third solution. Then, the obtained third solution was allowed to stand for 180 minutes, dried at 70° C. for 10 hours to remove the solvent, and then heat-treated at 1000° C. in an argon atmosphere to remove impurities to obtain a negative electrode active material.
  • the negative electrode active material obtained in this step is prepared into a pole piece, and the negative electrode active material with the desired particle crushing rate can be formed by controlling the rolling pressure and/or the rolling time control. Controlling the content of the second solution in the third solution can also realize the control of the particle crushing rate.
  • the negative active material, the binder styrene-butadiene rubber (SBR) and the thickener sodium carboxymethyl cellulose (CMC) prepared above are fully stirred and mixed in an appropriate amount of deionized water at a weight ratio of 97:1:2 to make it A uniform negative electrode slurry is formed, wherein the solid content of the negative electrode slurry is 54 wt%.
  • This slurry was coated on a negative electrode current collector (copper foil), dried at 85°C, and then cold pressed, cut into pieces, and cut, and dried under vacuum conditions at 120°C for 12 hours to obtain a negative electrode.
  • the positive electrode slurry wherein the solid content of the positive electrode slurry is 72 wt%.
  • the slurry was coated on the positive electrode current collector aluminum foil, dried at 85°C, and then cold-pressed, cut into pieces, and cut, and dried under vacuum at 85°C for 4 hours to obtain a positive electrode.
  • a polyethylene (PE) porous polymer film with a thickness of 7 ⁇ m was used as the separator.
  • the electrolyte is vacuum packaged, standing, forming, shaping, capacity testing and other processes to obtain a soft-packed lithium-ion battery.
  • Cycle capacity retention ratio (discharge capacity at the 200th cycle/discharge capacity at the first cycle) ⁇ 100%.
  • the lithium-ion battery is fully charged and placed in a high temperature box at 150°C.
  • the time when the lithium-ion battery starts to show flames is recorded as the thermal shock endurance time. Five samples were tested for each example or comparative example, and the average value was taken.
  • the lithium-ion battery was overcharged at a current density of 1C, and the surface temperature of the lithium-ion battery was tested. Five samples were tested for each example or comparative example, and the average value was taken.
  • the lithium-ion battery is charged at a constant current of 0.5C to a voltage of 4.3V, and then charged at a constant voltage of 4.3V to a current of 0.05C.
  • the UL1642 test standard is adopted.
  • the weight of the weight is 9.8kg and the diameter is 15.8mm, drop height of 61 ⁇ 2.5cm, impact test on lithium ion battery.
  • Instron (model 33652) tester to test: take the pole piece (width 30mm, length 100-160mm), and fix it with double-sided adhesive paper (model: 3M9448A, width 20mm, length 90-150mm) On the steel plate, stick the tape on the surface of the negative active material layer, connect one side of the tape to the paper tape of the same width, adjust the limit block of the tension machine to a suitable position, fold the tape upwards and slide 40mm, The slip rate was 50 mm/min, and the polymerization strength between particles inside the negative active material layer at 180° (that is, stretched in the opposite direction) was tested.
  • Instron (model 33652) tester to test: take the pole piece (width 30mm, length 100-160mm), and fix it with double-sided adhesive paper (model: 3M9448A, width 20mm, length 90-150mm) On the steel plate, stick the tape on the surface of the negative active material layer, connect one side of the tape to the paper tape of the same width, adjust the limit block of the tension machine to a suitable position, fold the tape upwards and slide 40mm, The slip rate was 50 mm/min, and the binding force between the negative electrode active material layer and the negative electrode current collector at 180° (that is, stretched in the opposite direction) was tested.
  • Table 1 shows the impact of the particle crushing rate of the negative active material and Id/Ig on the cycle performance and safety of the lithium ion battery.
  • the width of the cracks or cracks of the crushed particles in Table 1 is not greater than 4 ⁇ m.
  • the results show that, compared to the comparative example, when the negative electrode active material contains crushed particles and the particle crushing rate is 20% to 80%, the cycle capacity retention rate of the lithium ion battery is significantly increased, the thermal shock endurance time is significantly extended, and the battery is overcharged.
  • the surface temperature in the test, nail penetration test, and impact test is significantly reduced, that is, the cycle performance and safety of the lithium-ion battery are significantly improved.
  • controlling the Id/Ig of the negative electrode active material within the range of 0.7 to 1.5 can further improve the cycle capacity retention rate of lithium-ion batteries, extend the thermal shock endurance time, and reduce the overcharge test, nail penetration test and impact test.
  • the surface temperature in the. On the basis of Id / Ig of 0.7 to 1.5 on the control Id 200cm -1 to 1100cm -1, it helps to further improve the cycle characteristics and safety of the lithium ion battery.
  • Table 2 shows the influence of metallic elements, non-metallic elements and pores in the negative active material on the cycle performance and safety of lithium-ion batteries. Except for the parameters listed in Table 2, the other settings of Embodiments 13-40 are consistent with those of Embodiment 3, and the other settings of Embodiment 41 are consistent with those of Embodiment 2.
  • the negative electrode active material contains 20 ppm to 400 ppm of metal elements and/or 50 ppm to 400 ppm of non-metal elements, it helps to further improve the cycle performance and safety of the lithium ion battery.
  • the negative electrode active material has pores and the inner wall of the pores has metal elements and/or non-metal elements, it helps to further improve the cycle performance and safety of the lithium ion battery.
  • Table 3 shows the influence of the properties of the negative electrode active material on the cycle performance and safety of lithium-ion batteries. Except for the parameters listed in Table 3, Examples 42-54 are consistent with the other settings of Example 3.
  • the results show that when the roughness of the negative electrode active material layer is not greater than 6 ⁇ m, the cohesive strength of the negative electrode active material is in the range of 5N/m to 30N/m, and/or the binding force between the negative electrode active material layer and the negative electrode current collector When it is in the range of 5N/m to 20N/m, it helps to further improve the cycle performance and safety of the lithium ion battery.
  • Table 4 shows the influence of the proportion of the area of the negative electrode current collector where the negative electrode active material layer is not provided on the cycle performance and safety of the lithium ion battery. Except for the parameters listed in Table 4, the other settings of Examples 55-58 are the same as those of Example 3.
  • references to “embodiments”, “partial examples”, “one embodiment”, “another example”, “examples”, “specific examples” or “partial examples” throughout the specification mean that At least one embodiment or example in this application includes the specific feature, structure, material, or characteristic described in the embodiment or example. Therefore, descriptions appearing in various places throughout the specification, such as: “in some embodiments”, “in an example”, “in one example”, “in another example”, “in an example “In”, “in a specific example” or “exemplified”, which are not necessarily quoting the same embodiment or example in this application.
  • the specific features, structures, materials or characteristics herein can be combined in one or more embodiments or examples in any suitable manner.

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Abstract

La présente invention porte sur un dispositif électrochimique et sur un dispositif électronique. Spécifiquement, la présente invention concerne un dispositif électrochimique comprenant une électrode positive, une électrode négative et un électrolyte. L'électrode négative comprend un collecteur de courant d'électrode négative et un couche de matériau actif d'électrode négative disposée sur le collecteur de courant d'électrode négative. La couche de matériau actif d'électrode négative comprend un matériau actif d'électrode négative. Le matériau actif d'électrode négative comprend des particules de fragment, et le taux de fragmentation de particule du matériau actif d'électrode négative est de 20 % à 80 %. Le dispositif électrochimique de la présente invention améliore les performances de cycle et les performances de sécurité.
PCT/CN2020/081608 2020-03-27 2020-03-27 Dispositif électrochimique et dispositif électronique WO2021189406A1 (fr)

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WO2024041206A1 (fr) * 2022-08-25 2024-02-29 珠海冠宇电池股份有限公司 Électrolyte de batterie et batterie

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CN103367703A (zh) * 2013-07-18 2013-10-23 东莞新能源科技有限公司 一种锂离子电池的负极极片及包含该极片的电池
CN110316714A (zh) * 2019-06-17 2019-10-11 西安交通大学苏州研究院 基于稻壳的三维多孔类石墨烯结构碳材料及其制备方法和应用

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CN103367703A (zh) * 2013-07-18 2013-10-23 东莞新能源科技有限公司 一种锂离子电池的负极极片及包含该极片的电池
CN110316714A (zh) * 2019-06-17 2019-10-11 西安交通大学苏州研究院 基于稻壳的三维多孔类石墨烯结构碳材料及其制备方法和应用

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2024041206A1 (fr) * 2022-08-25 2024-02-29 珠海冠宇电池股份有限公司 Électrolyte de batterie et batterie

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