CN116995191B - Negative electrode piece and lithium ion battery - Google Patents

Negative electrode piece and lithium ion battery Download PDF

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Publication number
CN116995191B
CN116995191B CN202311264099.1A CN202311264099A CN116995191B CN 116995191 B CN116995191 B CN 116995191B CN 202311264099 A CN202311264099 A CN 202311264099A CN 116995191 B CN116995191 B CN 116995191B
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negative electrode
silicon
coating
positive electrode
conductive agent
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CN116995191A (en
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沈志鹏
陈凯
冯玉川
李峥
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Suzhou Qingtao New Energy S&T Co Ltd
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Suzhou Qingtao New Energy S&T Co Ltd
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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
    • H01M4/134—Electrodes based on metals, Si or alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • 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
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • H01M4/366—Composites as layered products
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/386—Silicon or alloys based on silicon
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • H01M4/625—Carbon or graphite
    • 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
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/027—Negative electrodes

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Composite Materials (AREA)
  • Inorganic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

The application discloses a negative electrode plate and a lithium ion battery, wherein the negative electrode plate comprises a negative electrode current collector, a first coating arranged on the negative electrode current collector and a second coating arranged on the first coating; the first coating comprises a negative electrode active material, a first negative electrode conductive agent and a first negative electrode binder, wherein the negative electrode active material comprises a silicon-based negative electrode material and hard carbon-coated graphite; the second coating comprises graphite coated by hard carbon, a second negative electrode conductive agent and a second negative electrode binder; the silicon-based anode material comprises a silicon-containing compound and dopamine coated on the surface of the silicon-containing compound. The negative electrode plate and the lithium ion battery provided by the application can solve the problem that the high energy density and the quick charging capability of the lithium ion battery cannot be achieved in the prior art.

Description

Negative electrode piece and lithium ion battery
Technical Field
The application relates to the technical field of batteries, in particular to a negative electrode plate and a lithium ion battery.
Background
The lithium ion battery is widely used in products such as mobile phones, notebook computers, tablet computers, electric automobiles and the like due to the advantages of high working voltage, high energy density, low self-discharge rate, green environmental protection and the like. However, the lithium ion battery with high energy density cannot realize rapid charging due to the unsatisfactory rate performance of the negative electrode plate.
Therefore, how to obtain a negative electrode tab and a lithium ion battery with both high energy density and fast charging capability is a technical problem that needs to be solved by those skilled in the art.
Disclosure of Invention
The application provides a negative pole piece and a lithium ion battery to solve the problem that lithium ion battery high energy density and quick charge ability can not be concurrently among the prior art.
In order to solve one or more of the above technical problems, the technical solution adopted in the present application is:
in a first aspect, the present application provides a negative electrode tab comprising a negative electrode current collector, a first coating disposed on the negative electrode current collector, and a second coating disposed on the first coating;
the first coating comprises a negative electrode active material, a first negative electrode conductive agent and a first negative electrode binder, wherein the negative electrode active material comprises a silicon-based negative electrode material and hard carbon-coated graphite;
the second coating comprises graphite coated by hard carbon, a second negative electrode conductive agent and a second negative electrode binder.
Further, the silicon-based anode material comprises a silicon-containing compound and dopamine coated on the surface of the silicon-containing compound.
Further, the silicon-containing compound includes at least one of silicon oxide and silicon carbide.
Further, the thickness of the first coating layer is 50% -70% of the sum of the thicknesses of the first coating layer and the second coating layer, and the thickness of the second coating layer is 30% -50% of the sum of the thicknesses of the first coating layer and the second coating layer.
Further, the mass fraction of the silicon-containing compound in the anode active material is 5% -20%.
Further, the first negative electrode conductive agent comprises vapor grown carbon fibers, conductive carbon black and single-walled carbon nanotubes.
Further, the second negative electrode conductive agent includes single-walled carbon nanotubes and conductive carbon black.
Further, the first negative electrode binder includes at least one of polyacrylic acid or polyacrylonitrile;
and/or the number of the groups of groups,
the second negative electrode binder includes at least one of carboxymethyl cellulose, styrene-butadiene rubber, or polyacrylic acid.
Preferably, the first negative electrode binder is a mixture of polyacrylic acid and polyacrylonitrile.
Preferably, the second negative electrode binder is polyacrylic acid.
Further, the negative current collector includes a carbon coated copper foil.
In a second aspect, corresponding to the above-mentioned negative electrode plate, the present application provides a lithium ion battery, the lithium ion battery includes a positive electrode plate, a negative electrode plate and an electrolyte, and the negative electrode plate is the above-mentioned negative electrode plate.
According to a specific embodiment provided by the application, the application discloses the following technical effects:
the application provides a negative pole piece and lithium ion battery, improves the purpose that realizes lithium ion battery high energy density and quick charge ability and obtain through the structure to the negative pole piece. Specifically, the negative electrode active material in the first coating layer arranged on the negative electrode current collector comprises a silicon-based negative electrode material and hard carbon coated graphite, the second coating layer arranged on the first coating layer comprises hard carbon coated graphite, the silicon-based negative electrode material in the first coating layer can improve the energy density of the negative electrode plate, and the hard carbon coated graphite in the first coating layer and the second coating layer can improve the charging capacity of the negative electrode plate. The design of the two layers of coating on the negative electrode current collector can greatly improve the charging capacity of the battery while ensuring high energy density, so that the aim of achieving both high energy density and quick charging capacity of the lithium ion battery is fulfilled. In addition, the silicon-based anode material comprises a silicon-containing compound and dopamine coated on the surface of the silicon-containing compound. The dopamine-coated silicon-containing compound has hydroxyl and amino functional groups on the surface, so that dipole moment interacted with lithium ions can be improved, the diffusion coefficient of the lithium ions in the negative electrode is improved, and the compound conductive agent is matched for use, so that the compound conductive compound has better multiplying power performance.
Furthermore, the vapor grown carbon fiber, the conductive carbon black and the single-walled carbon nanotube are adopted as the first conductive agent in the first coating, so that the conductivity of the whole coating can be improved, the second conductive agent in the second coating comprises the single-walled carbon nanotube and the conductive carbon black, the single-walled carbon nanotube can form a continuous conductive network more easily, the transmission of lithium ions can be promoted more easily by combining the use of the conductive carbon black, and the improvement of the multiplying power performance of the battery is more obvious.
Further, the negative electrode current collector in the application comprises the carbon-coated copper foil, and the carbon-coated copper foil is selected as the negative electrode current collector, so that the impedance of a negative electrode active substance and the negative electrode current collector can be reduced, the surface density and the compaction density of a negative electrode plate are optimized, the lithium ion transmission distance is shortened, and the quick charging capability of a battery can be improved.
Of course, not all of the above-described advantages need be achieved at the same time in practicing any one of the products of the present application.
Detailed Description
The following description of the technical solutions in the embodiments of the present application will be clear and complete, and it is obvious that the described embodiments are only some embodiments of the present application, but not all embodiments. All other embodiments obtained by a person of ordinary skill in the art based on the embodiments in the present application are within the scope of the protection of the present application.
As described in the background art, the lithium ion battery with high energy density cannot realize rapid charging due to the unsatisfactory rate performance of the negative electrode plate. In order to solve one or more of the problems, the application creatively provides a novel negative electrode plate and a lithium ion battery, and the aims of high energy density and quick charging capability of the lithium ion battery are achieved by improving the structure of the negative electrode plate.
The following is an optional technical scheme of the application, but not as a limitation to the technical scheme provided by the application, and the technical purpose and beneficial effect of the application can be better achieved and realized through the following optional technical scheme.
The application provides a negative electrode plate, which comprises a negative electrode current collector, a first coating layer arranged on the negative electrode current collector and a second coating layer arranged on the first coating layer, wherein the first coating layer comprises a negative electrode active substance, a first negative electrode conductive agent and a first negative electrode binder, and the negative electrode active substance comprises a silicon-based negative electrode material and hard carbon coated graphite; the second coating comprises graphite coated by hard carbon, a second negative electrode conductive agent and a second negative electrode binder. Specifically, the negative electrode active material in the first coating layer arranged on the negative electrode current collector comprises a silicon-based negative electrode material and hard carbon coated graphite, the second coating layer arranged on the first coating layer comprises hard carbon coated graphite, the silicon-based negative electrode material in the first coating layer can improve the energy density of the negative electrode plate, and the hard carbon coated graphite in the first coating layer and the second coating layer can improve the charging capacity of the negative electrode plate. The design of the two layers of coating on the negative electrode current collector can greatly improve the charging capacity of the battery while ensuring high energy density, so that the aim of achieving both high energy density and quick charging capacity of the lithium ion battery is fulfilled.
Further, the first negative electrode conductive agent comprises vapor grown carbon fibers, conductive carbon black and single-walled carbon nanotubes, and the vapor grown carbon fibers, the conductive carbon black and the single-walled carbon nanotubes are used as the composite conductive agent, so that the conductive performance of the whole coating can be improved. The second conductive agent comprises single-walled carbon nanotubes and conductive carbon black, the single-walled carbon nanotubes are easier to form a continuous conductive network, and the combination of the conductive carbon black is more beneficial to promoting the transmission of lithium ions, so that the improvement of the rate performance of the battery is more obvious.
Further, the first negative electrode binder includes at least one of polyacrylic acid or polyacrylonitrile, and preferably, the first negative electrode binder is a mixture of polyacrylic acid and polyacrylonitrile.
The second negative electrode binder includes at least one of carboxymethyl cellulose, styrene-butadiene rubber, or polyacrylic acid, and preferably, the second negative electrode binder is polyacrylic acid.
In this embodiment of the present application, the silicon-based anode material includes a silicon-containing compound and dopamine coated on a surface of the silicon-containing compound, and specifically, the silicon-containing compound includes at least one of silicon oxide and silicon carbide, and sizes of the silicon oxide and the silicon carbide are nano-scale. The surface of the dopamine-coated silicon-containing compound has hydroxyl and amino functional groups, so that dipole moment interacted with lithium ions can be improved, the diffusion coefficient of the lithium ions in the negative electrode is improved, and the compound conductive agent is matched for use, so that the lithium-ion-containing compound has better multiplying power performance. In addition, the silicon-containing compound can generate larger volume expansion after being combined with lithium ions, the internal structure of the expanded negative electrode material is destroyed, the cycle life of the lithium ion battery is further influenced, and the expansion of silicon in the silicon-containing compound is buffered by coating dopamine on the surface of the silicon-containing compound, so that the expansion of the silicon in the cycle process of the lithium ion battery is inhibited.
Too low a mass fraction of the silicon-containing compound in the anode active material affects the energy density of the lithium ion battery, while too high a mass fraction of the silicon-containing compound in the anode active material affects the service life of the lithium ion battery and increases the cost. In order to achieve both the energy density and the service life of the lithium ion battery, in the embodiments of the present application, the mass fraction of the silicon-containing compound in the negative electrode active material is 5% -20%, more specifically, the mass fraction of the silicon-containing compound in the negative electrode active material may be 5%, 10%, 15%, 20%, and specific point values between the above point values, which are limited in space and for brevity, the present invention is not exhaustive to list the specific point values included in the range.
In a specific embodiment, the thickness of the first coating layer is 50% -70% of the sum of the thicknesses of the first coating layer and the second coating layer, more specifically, the thickness of the first coating layer is 50%,55%,60%,65%,70% of the sum of the thicknesses of the first coating layer and the second coating layer, and specific point values among the above point values are limited in space and for brevity, the present invention is not exhaustive of the specific point values included in the range. The thickness of the second coating layer is 30% -50% of the sum of the thicknesses of the first coating layer and the second coating layer, more specifically, the thickness of the second coating layer is 30%, 35%, 40%, 45%, 50% of the sum of the thicknesses of the first coating layer and the second coating layer, and specific point values among the above point values are limited in space and for the sake of brevity, the present invention does not exhaustively list the specific point values included in the range. The thickness ratio of the first coating to the second coating is reasonably controlled, so that the energy density and the expansion performance of the cathode can be better coordinated.
In a specific embodiment, the negative current collector comprises a carbon coated copper foil. The carbon-coated copper foil is selected as the negative current collector, so that the impedance of the negative active material and the negative current collector can be reduced, the surface density and the compaction density of the negative electrode plate are optimized, and the lithium ion transmission distance is shortened, thereby improving the quick charging capability of the battery. As a preferred embodiment, the thickness of the carbon coated copper foil is 1-50 μm, more specifically, the thickness of the carbon coated copper foil may be 1, 5, 10, 15, 20 or 50 μm, and specific point values between the above point values, are limited in space and for the sake of brevity, the present invention does not exhaustively list the specific point values included in the range.
Corresponding to the negative electrode plate, the application also provides a lithium ion battery, which comprises a positive electrode plate, a negative electrode plate and electrolyte. The relevant content of the negative electrode sheet can be referred to the above description, and will not be described in detail here.
In this embodiment of the application, the positive pole piece includes positive current collector and covers positive active material layer on positive current collector surface, positive active material layer includes positive active material, positive binder, positive conductive agent. And in the specific implementation, uniformly mixing the positive electrode active material, the positive electrode binder, the positive electrode conductive agent and the solvent to obtain positive electrode slurry, coating the positive electrode slurry on the surface of the positive electrode current collector, drying and rolling to obtain the positive electrode plate.
The positive electrode current collector in the embodiments of the present application is not particularly limited as long as it has conductivity without causing chemical changes in the battery. Specifically, the positive current collector includes, but is not limited to, any one of aluminum, nickel or stainless steel, such as aluminum foil. The shape of the positive electrode current collector includes, but is not limited to, metal foil, metal grid, metal mesh, etc., and the user may select according to actual needs, which is not particularly limited herein.
The positive electrode active material is a compound that reversibly intercalates and deintercalates lithium, and the positive electrode active material in this application may be known in the artAny positive electrode active material. For example: the positive electrode active material includes, but is not limited to, one of a layered oxide cathode, a spinel cathode, and an olivine-type cathode. For example, a layered oxide cathode (e.g., a rock salt layered oxide) comprises one or more lithium-based positive electroactive materials selected from the group consisting of: liCoO 2 (LCO)，LiNi x Mn y Co 1-x-y O 2 (wherein x is more than or equal to 0 and less than or equal to 1, and y is more than or equal to 0 and less than or equal to 1), and LiNi 1-x-y Co x Al y O 2 (wherein x is more than or equal to 0 and less than or equal to 1, and y is more than or equal to 0 and less than or equal to 1), and LiNi x Mn 1-x O 2 (wherein 0.ltoreq.x.ltoreq.1), and Li 1+x MO 2 (wherein M is one of Mn, ni, co and Al, and x is more than or equal to 0 and less than or equal to 1). The spinel cathode comprises one or more lithium-based positive electroactive materials selected from the group consisting of: liMn 2 O 4 (LMO) and LiNi x Mn 1.5 O 4 . Olivine-type cathodes comprising one or more lithium-based positive electroactive materials LiMPO 4 (wherein M is at least one of Fe, ni, co and Mn).
In a specific embodiment, the mass fraction of the positive electrode active material is 80% -99%, more specifically, the mass fraction of the positive electrode active material may be 80%, 85%, 90%, 95% or 99%, and specific point values between the above point values, are limited in terms of space and for brevity, the present invention is not exhaustive to list the specific point values included in the range. When the mass fraction of the positive electrode active material is 80% or less, the capacity of the lithium ion battery may be reduced due to a decrease in energy density.
The positive electrode binder is a component that contributes to adhesion between the positive electrode active material and the positive electrode conductive agent, and adhesion with the positive electrode current collector. In the embodiment of the present application, the positive electrode binder includes, but is not limited to, one or more of Polytetrafluoroethylene (PTFE), sodium carboxymethyl cellulose (CMC), styrene Butadiene Rubber (SBR), polyvinylidene fluoride (PVDF), nitrile Butadiene Rubber (NBR), styrene-butylene-styrene copolymer (SEBS), styrene-butadiene-styrene copolymer (SBS), lithium polyacrylate (LiPAA), sodium polyacrylate (NaPAA), sodium alginate, and lithium alginate. The user may select according to actual needs, and is not particularly limited herein.
The positive electrode conductive agent is a material that provides conductivity without causing adverse chemical reactions in the battery. In embodiments of the present application, the positive electrode conductive agent may include a carbon-based material, powdered nickel or other metal particles, or a conductive polymer. The carbon-based material may include, for example, particles of carbon black, graphite, super-P, acetylene black (such as KETCHENTM black or denktatm black), carbon fibers and nanotubes, graphene, and the like. Examples of the conductive polymer include polyaniline, polythiophene, polyacetylene, polypyrrole, poly (3, 4-ethylenedioxythiophene) polysulfstyrene, and the like. Preferably, the positive electrode conductive agent comprises one or more of conductive carbon black (Super-P), acetylene black, ketjen black, carbon Nanotubes (CNTs), graphene (rGO), activated carbon and Carbon Nanofibers (CNFs).
In a specific embodiment, the mass fraction of the positive electrode conductive agent is 1% -20%, more specifically, the mass fraction of the positive electrode conductive agent may be 1%, 5%, 10%, 15% or 20%, based on the total weight of the solid components in the positive electrode slurry, and specific point values among the above point values are limited in length and are not exhaustive for the sake of brevity.
Solvents include water or organic solvents, such as: n-methyl-2-pyrrolidone (NMP) or alcohol in an amount such that a positive electrode slurry comprising a positive electrode active material, a positive electrode binder, and a positive electrode conductive agent attains a desired viscosity. In a specific embodiment, the solvent is present in an amount such that the mass fraction of the solid component in the positive electrode slurry is 15% -65%, more specifically, the mass fraction of the solid component in the positive electrode slurry may be 15%, 20%, 30%, 40%, 50% or 65%, and specific point values between the above point values, are limited in length and for the sake of brevity, the present invention is not exhaustive to list the specific point values included in the range.
In order to prevent short circuits inside the battery, a separator is also required to be included in the lithium ion battery, and the separator is located between the positive electrode tab and the negative electrode tab to block the transmission of electrons inside the battery. The separator in the present application is any one of various separators used in lithium ion batteries, and includes a material having low resistance to ion migration of an electrolyte and good electrolyte holding ability. In this embodiment of the present application, the separator includes, but is not limited to, one or more of polypropylene, polyethylene, polyvinylidene fluoride, polyimide, and polyacrylonitrile, and the user may select according to actual needs, which is not specifically limited herein. It is to be noted here that when a solid electrolyte is employed, the solid electrolyte functions as a separator, and a conventional separator is not required.
In a specific embodiment, the membrane has a pore size of 0.01 μm to 15 μm and a thickness of 10 μm to 400 μm.
The electrolyte includes a liquid electrolyte and a solid electrolyte. The liquid electrolyte comprises a lithium salt and a nonaqueous solvent, the lithium salt comprising LiPF 6 、LiBF 4 、LiAsF 6 、LiClO 4 、LiB(C 6 H 5 ) 4 、LiCH 3 SO 3 、LiCF 3 SO 3 、LiN(SO 2 CF 3 ) 2 、LiC (SO 2 CF 3 ) 3 、LiSiF 6 、LiBOB、LiBF 2 (C 2 O 4 ) One or more of these may be selected by the user according to actual needs, and are not particularly limited herein. In the embodiment of the application, the lithium salt is preferably LiPF 6 Because of LiPF 6 Can have high ion conductivity and can improve cycle characteristics of the battery.
The nonaqueous solvent comprises one or more of a carbonate compound, a carboxylate compound and an ether compound. Further, the carbonate compound includes a chain carbonate compound, a cyclic carbonate compound, and a fluorocarbonate compound. Specifically, the chain carbonate compounds include, but are not limited to, diethyl carbonate (DEC), dimethyl carbonate (DMC), dipropyl carbonate (DPC), methylpropyl carbonate (MPC), ethylpropyl carbonate (EPC), ethylmethyl carbonate (MEC), and the like; the cyclic carbonate compounds include, but are not limited to, ethylene Carbonate (EC), propylene Carbonate (PC), butylene Carbonate (BC), vinyl Ethylene Carbonate (VEC), and the like; the fluorocarbonate compounds include, but are not limited to, fluoroethylene carbonate (FEC), 1, 2-difluoroethylene carbonate, 1, 2-trifluoroethylene carbonate, 1, 2-tetrafluoroethylene carbonate, 1-fluoro-2-methylethylene carbonate, 1-fluoro-1-methylethylene carbonate, 1, 2-difluoro-1-methylethylene carbonate, 1, 2-trifluoro-2-methylethylene carbonate, trifluoromethyl ethylene carbonate, and the like.
The carboxylic acid ester compounds include, but are not limited to, methyl acetate, ethyl acetate, n-propyl acetate, t-butyl acetate, methyl propionate, ethyl propionate, gamma-butyrolactone, decalactone, valerolactone, mevalonic acid lactone, caprolactone, methyl formate, and the like.
The ether compounds include, but are not limited to, dibutyl ether, tetraglyme, diglyme, 1, 2-dimethoxyethane, 1, 2-diethoxyethane, ethoxymethoxyethane, 2-methyltetrahydrofuran, tetrahydrofuran, and the like.
Further, the nonaqueous solvent may further include one or more of dimethyl sulfoxide, 1, 2-dioxolane, sulfolane, methyl sulfolane, 1, 3-dimethyl-2-imidazolidinone, N-methyl-2-pyrrolidone, formamide, dimethylformamide, acetonitrile, trimethyl phosphate, triethyl phosphate, trioctyl phosphate, and phosphoric acid ester.
In the embodiments of the present application, the solid electrolyte includes, but is not limited to, a polymer solid electrolyte, an oxide solid electrolyte, a sulfide solid electrolyte, and the like.
Wherein the polymer solid electrolyte comprises at least one of polyvinyl chloride (PVC), polyacrylonitrile (PAN), polymethyl methacrylate (PMMA) and polyethylene oxide (PEO).
The oxide solid electrolyte may include one or more garnet ceramics, LISICON-type oxides, NASICON-type oxides, and perovskite-type ceramics, among others. For example, the one or more garnet ceramics may be selected from the group consisting of: li (Li) 6.5 La 3 Zr 1.75 Te 0.25 O 12 、Li 7 La 3 Zr 2 O 12 、Li 6.2 Ga 0.3 La 2.95 Rb 0.05 Zr 2 O 12 、Li 6.85 La 2.9 Ca 0.1 Zr 1.75 Nb 0.25 O 12 、Li 6.25 Al 0.25 La 3 Zr 2 O 12 、Li 6.75 La 3 Zr 1.75 Nb 0.25 O 12 、Li 6.75 La 3 Zr 1.75 Nb 0.25 O 12 And combinations thereof. The one or more LISICON-type oxides may be selected from the group comprising: li (Li) 14 Zn(GeO 4 ) 4 、Li 3+x (P 1−x Si x )O 4 (wherein 0<x<1）、Li 3+x Ge x V 1-x O 4 (wherein 0<x<1) And combinations thereof. One or more NASICON type oxides can be selected from LiMM ʹ (PO 4 ) 3 Definition, wherein M and M ʹ are independently selected from Al, ge, ti, sn, hf, zr and La. For example, in certain variations, the one or more NASICON-type oxides may be selected from the group consisting of: li (Li) 1+x Al x Ge 2-x (PO 4 ) 3 (LAGP) (wherein 0.ltoreq.x.ltoreq.2), li 1+x Al x Ti 2-x (PO 4 ) 3 (LATP) (where 0.ltoreq.x.ltoreq.2), li 1+x Y x Zr 2-x (PO 4 ) 3 (LYZP) (wherein 0.ltoreq.x.ltoreq.2), li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 、LiTi 2 (PO 4 ) 3 、LiGeTi(PO 4 ) 3 、LiGe 2 (PO 4 ) 3 、LiHf 2 (PO 4 ) 3 And combinations thereof. The one or more perovskite ceramics may be selected from the group comprising: li (Li) 3.3 La 0.53 TiO 3 、LiSr 1.65 Zr 1.3 Ta 1.7 O 9 、Li 2x-y Sr 1-x Ta y Zr 1-y O 3 (wherein x=0.75 y and 0.60<y<0.75）、Li 3/8 Sr 7/16 Nb 3/4 Zr 1/4 O 3 、Li 3x La (2/3-x) TiO 3 (wherein 0<x<0.25 A) and combinations thereof.
Wherein the sulfide-based solid state electrolyte may include one or more sulfide-based materials selected from the group consisting of: li (Li) 2 S-P 2 S 5 、Li 2 S-P 2 S 5 -MS x (wherein M is Si, ge and Sn and 0.ltoreq.x.ltoreq.2), li 3.4 Si 0.4 P 0.6 S 4 、Li 10 GeP 2 S 11.7 O 0.3 、Li 9.6 P 3 S 12 、Li 7 P 3 S 11 、Li 9 P 3 S 9 O 3 、Li 10.35 Si 1.35 P 1.65 S 12 、Li 9.81 Sn 0.81 P 2.19 S 12 、Li 10 (Si 0.5 Ge 0.5 )P 2 S 12 、Li(Ge 0.5 Sn 0.5 )P 2 S 12 、Li(Si 0.5 Sn 0.5 )PsS 12 、Li 10 GeP 2 S 12 （LGPS）、Li 6 PS 5 X (wherein X is Cl, br or I), li 7 P 2 S 8 I、Li 10.35 Ge 1.35 P 1.65 S 12 、Li 3.25 Ge 0.25 P 0.75 S 4 、Li 10 SnP 2 S 12 、Li 10 SiP 2 S 12 、Li 9.54 Si 1.74 P 1.44 S 11.7 C l0.3 、 (1-x) P 2 S 5-x Li 2 S (wherein 0.5.ltoreq.x.ltoreq.0.7) and combinations thereof.
The above materials are merely illustrative examples of selected positive electrode materials, and it is understood that any known positive electrode materials including positive electrode active materials, positive electrode binders, positive electrode conductive agents, and other additives can be used in the present application without departing from the inventive concepts of the present application.
Embodiments of the present invention will be described more specifically below with reference to examples and comparative examples. However, embodiments of the present invention are not limited to these examples only.
Example 1
The embodiment of the application provides a lithium ion battery, which comprises a negative electrode plate, a positive electrode plate and electrolyte.
The negative electrode sheet comprises a carbon-coated copper foil with the thickness of 10 mu m, a first coating layer arranged on the carbon-coated copper foil and a second coating layer arranged on the first coating layer, wherein the first coating layer comprises a negative electrode active substance, a first negative electrode conductive agent (vapor phase grown carbon fiber, conductive carbon black and single-wall carbon nano tubes) and a first negative electrode binder polyacrylic acid, the negative electrode active substance comprises a silicon-containing compound (silicon-containing compound is a mixture of silicon carbide and silicon oxide, the mass ratio of the silicon carbide to the silicon oxide is 1:1) and graphite coated with hard carbon, the mass fraction of the silicon-containing compound in the negative electrode active substance is 20%, and the mass ratio of the negative electrode active substance, the first negative electrode conductive agent and the first negative electrode binder in the first coating layer is 95:2:3, the second coating comprises graphite coated by hard carbon, a second negative electrode conductive agent (single-wall carbon nano tube and conductive carbon black) and a second negative electrode binder polyacrylic acid, wherein the mass ratio of the graphite coated by hard carbon to the second negative electrode conductive agent to the second negative electrode binder is 95:2:3, a step of; the positive electrode plate comprises a positive electrode current collector aluminum foil with the thickness of 10 mu m, and a positive electrode active material layer arranged on the positive electrode current collector aluminum foil, wherein the positive electrode active material layer comprises a positive electrode active material NCM-NI90, a positive electrode conductive agent super-P and a positive electrode binder PVDF, and the mass ratio of the positive electrode active material NCM-NI90 to the positive electrode conductive agent super-P to the positive electrode binder PVDF is 96:2:2.
the electrolyte comprises electrolyte and lithium salt, wherein the electrolyte is EC: DEC=1:1, and the lithium salt is LiPF 6 The concentration was 1mol/L.
The preparation method of the silicon-containing compound with the dopamine coated on the surface comprises the following steps:
3L of 0.1mol/L Tris buffer solution and 0.3L absolute ethyl alcohol are added into a vacuum stirring tank, then 30g of dopamine hydrochloride is added, and a mixed solution is formed after the dopamine hydrochloride is completely dissolved.
To the resulting mixed solution, 1.5kg of a mixture of silicon carbide and silicon oxide was added, and stirring was performed at a low temperature in an aerobic atmosphere and then at a low temperature in a nitrogen atmosphere. Stirring temperature is 5+/-2 ℃, stirring speed is 1200r/min, aerobic environment reaction is carried out for 5h, and nitrogen environment reaction is carried out for 12h.
The product was filtered and then dried under vacuum at 55 ℃ for 24 hours to obtain a silicon-containing compound having dopamine coated on the surface.
Example 2
Embodiment 2 differs from embodiment 1 in that the negative electrode sheet is different, and in embodiment 2, the first binder is polyacrylonitrile.
The embodiment provides a lithium ion battery, which comprises a negative electrode plate, a positive electrode plate and electrolyte.
The negative electrode sheet comprises a carbon-coated copper foil with the thickness of 10 mu m, a first coating layer arranged on the carbon-coated copper foil and a second coating layer arranged on the first coating layer, wherein the first coating layer comprises a negative electrode active substance, a first negative electrode conductive agent (vapor phase grown carbon fiber, conductive carbon black and single-walled carbon nano tubes) and a first negative electrode binder polyacrylonitrile, the negative electrode active substance comprises a silicon-containing compound (silicon-containing compound is a mixture of silicon carbide and silicon oxide, the mass ratio of the silicon carbide to the silicon oxide is 1:1) with dopamine coated on the surface and graphite coated with hard carbon, the mass fraction of the silicon-containing compound in the negative electrode active substance is 20%, and the mass ratio of the negative electrode active substance, the first negative electrode conductive agent and the first negative electrode binder in the first coating layer is 95:2:3, the second coating comprises graphite coated by hard carbon, a second negative electrode conductive agent (single-wall carbon nano tube and conductive carbon black) and a second negative electrode binder polyacrylic acid, wherein the mass ratio of the graphite coated by hard carbon to the second negative electrode conductive agent to the second negative electrode binder is 95:2:3.
the positive electrode plate comprises a positive electrode current collector aluminum foil with the thickness of 10 mu m, and a positive electrode active material layer arranged on the positive electrode current collector aluminum foil, wherein the positive electrode active material layer comprises a positive electrode active material NCM-NI90, a positive electrode conductive agent super-P and a positive electrode binder PVDF, and the mass ratio of the positive electrode active material NCM-NI90 to the positive electrode conductive agent super-P to the positive electrode binder PVDF is 96:2:2.
the electrolyte comprises electrolyte and lithium salt, wherein the electrolyte is EC: DEC=1:1, and the lithium salt is LiPF 6 The concentration was 1mol/L.
Example 3
Example 3 differs from example 1 in that in example 3, the first negative electrode binder is a mixture of polyacrylonitrile and polyacrylic acid.
The embodiment provides a lithium ion battery, which comprises a negative electrode plate, a positive electrode plate and electrolyte.
The negative electrode sheet comprises a carbon-coated copper foil with the thickness of 10 mu m, a first coating layer arranged on the carbon-coated copper foil and a second coating layer arranged on the first coating layer, wherein the first coating layer comprises a negative electrode active substance, a first negative electrode conductive agent (vapor phase grown carbon fiber, conductive carbon black and single-walled carbon nano tubes) and a mixture of a first negative electrode binder polyacrylonitrile and polyacrylic acid, the negative electrode active substance comprises a silicon-containing compound (the silicon-containing compound is a mixture of silicon carbide and silicon oxide, the mass ratio of the silicon carbide to the silicon oxide is 1:1) and graphite coated with hard carbon, the mass ratio of the silicon-containing compound in the negative electrode active substance is 20%, and the mass ratio of the negative electrode active substance, the first negative electrode conductive agent and the first negative electrode binder in the first coating layer is 95:2:3, the second coating comprises graphite coated by hard carbon, a second negative electrode conductive agent (single-wall carbon nano tube and conductive carbon black) and a second negative electrode binder polyacrylic acid, wherein the mass ratio of the graphite coated by hard carbon to the second negative electrode conductive agent to the second negative electrode binder is 95:2:3.
the positive electrode plate comprises a positive electrode current collector aluminum foil with the thickness of 10 mu m, and a positive electrode active material layer arranged on the positive electrode current collector aluminum foil, wherein the positive electrode active material layer comprises a positive electrode active material NCM-NI90, a positive electrode conductive agent super-P and a positive electrode binder PVDF, and the mass ratio of the positive electrode active material NCM-NI90 to the positive electrode conductive agent super-P to the positive electrode binder PVDF is 96:2:2.
the electrolyte comprises electrolyte and lithium salt, wherein the electrolyte is EC: DEC=1:1, and the lithium salt is LiPF 6 The concentration was 1mol/L.
Example 4
Example 4 differs from example 2 in that in example 4, the second negative electrode binder is styrene-butadiene rubber.
The embodiment provides a lithium ion battery, which comprises a negative electrode plate, a positive electrode plate and electrolyte.
The negative electrode sheet comprises a carbon-coated copper foil with the thickness of 10 mu m, a first coating layer arranged on the carbon-coated copper foil and a second coating layer arranged on the first coating layer, wherein the first coating layer comprises a negative electrode active substance, a first negative electrode conductive agent (vapor phase grown carbon fiber, conductive carbon black and single-walled carbon nano tubes) and a first negative electrode binder polyacrylonitrile, the negative electrode active substance comprises a silicon-containing compound (silicon-containing compound is a mixture of silicon carbide and silicon oxide, the mass ratio of the silicon carbide to the silicon oxide is 1:1) with dopamine coated on the surface and graphite coated with hard carbon, the mass fraction of the silicon-containing compound in the negative electrode active substance is 20%, and the mass ratio of the negative electrode active substance, the first negative electrode conductive agent and the first negative electrode binder in the first coating layer is 95:2:3, the second coating comprises graphite coated by hard carbon, a second negative electrode conductive agent (single-wall carbon nano tube and conductive carbon black) and a second negative electrode binder styrene-butadiene rubber, wherein the mass ratio of the graphite coated by the hard carbon to the second negative electrode conductive agent to the second negative electrode binder is 95:2:3.
the positive electrode plate comprises a positive electrode current collector aluminum foil with the thickness of 10 mu m, and a positive electrode active material layer arranged on the positive electrode current collector aluminum foil, wherein the positive electrode active material layer comprises a positive electrode active material NCM-NI90, a positive electrode conductive agent super-P and a positive electrode binder PVDF, and the mass ratio of the positive electrode active material NCM-NI90 to the positive electrode conductive agent super-P to the positive electrode binder PVDF is 96:2:2.
the electrolyte comprises electrolyte and lithium salt, wherein the electrolyte is EC: DEC=1:1, and the lithium salt is LiPF 6 The concentration was 1mol/L.
Comparative example 1
Comparative example 1 differs from example 1 in that the negative electrode sheet in comparative example 1 includes a carbon-coated copper foil having a thickness of 10 μm, and a negative electrode active material layer including graphite, a negative electrode conductive agent (vapor-grown carbon fiber, conductive carbon black, and single-walled carbon nanotube), a negative electrode binder polyacrylic acid, wherein the mass ratio of graphite, the negative electrode conductive agent (vapor-grown carbon fiber, conductive carbon black, and single-walled carbon nanotube), and the negative electrode binder polyacrylic acid is 95:2:3.
comparative example 2
Comparative example 2 is different from example 1 in that the negative electrode sheet in comparative example 2 includes a carbon-coated copper foil having a thickness of 10 μm, and a negative electrode active material layer including hard carbon-coated graphite, a negative electrode conductive agent (vapor-phase grown carbon fiber, conductive carbon black, and single-walled carbon nanotube), a negative electrode binder cmc+sbr, wherein the mass ratio of the hard carbon-coated graphite, the negative electrode conductive agent (vapor-phase grown carbon fiber, conductive carbon black, and single-walled carbon nanotube), the negative electrode binder cmc+sbr is 95:2:3.
comparative example 3
Comparative example 3 differs from example 2 in that the negative electrode sheet, the silicon-containing compound thereof, was not subjected to dopamine coating.
The comparative example provides a lithium ion battery comprising a negative electrode sheet, a positive electrode sheet and an electrolyte.
The negative electrode sheet comprises a carbon-coated copper foil with the thickness of 10 mu m, a first coating layer arranged on the carbon-coated copper foil and a second coating layer arranged on the first coating layer, wherein the first coating layer comprises a negative electrode active substance, a first negative electrode conductive agent (vapor phase grown carbon fiber, conductive carbon black and single-walled carbon nano tubes) and a first negative electrode binder polyacrylonitrile, the negative electrode active substance comprises a silicon-containing compound (the silicon-containing compound is a mixture of silicon carbide and silicon oxide, the mass ratio of the silicon carbide to the silicon oxide is 1:1) and graphite coated by hard carbon, the mass fraction of the silicon-containing compound in the negative electrode active substance is 20%, and the mass ratio of the negative electrode active substance, the first negative electrode conductive agent and the first negative electrode binder in the first coating layer is 95:2:3, the second coating comprises graphite coated by hard carbon, a second negative electrode conductive agent (single-wall carbon nano tube and conductive carbon black) and a second negative electrode binder polyacrylic acid, wherein the mass ratio of the graphite coated by hard carbon to the second negative electrode conductive agent to the second negative electrode binder is 95:2:3.
the positive electrode plate comprises a positive electrode current collector aluminum foil with the thickness of 10 mu m, and a positive electrode active material layer arranged on the positive electrode current collector aluminum foil, wherein the positive electrode active material layer comprises a positive electrode active material NCM-NI90, a positive electrode conductive agent super-P and a positive electrode binder PVDF, and the mass ratio of the positive electrode active material NCM-NI90 to the positive electrode conductive agent super-P to the positive electrode binder PVDF is 96:2:2.
the electrolyte comprises electrolyte and lithium salt, wherein the electrolyte is EC: DEC=1:1, and the lithium salt is LiPF 6 The concentration was 1mol/L.
Test methods and conditions
1. The testing method of the maximum charging rate comprises the following steps:
and (3) fully charging the batteries prepared in the examples and the comparative examples with xC at 25 ℃ and fully discharging the batteries with 1C for 10 times, fully charging the batteries with xC, disassembling the negative pole piece, observing the lithium precipitation condition of the surface of the negative pole piece, and if the lithium is not precipitated on the surface of the negative pole piece, gradually increasing the charging rate xC with 0.1C as a gradient to test again until the lithium is precipitated on the surface of the negative pole, stopping the test, wherein the charging rate (x-0.1) C is the maximum charging rate of the batteries.
2. The method for testing the cycle performance comprises the following steps:
(1) Charging at 1C or a specified current to a final voltage, cutting off the current by 0.05C, and standing for 30min;
(2) Discharging at 1C to discharge final pressure, recording discharge capacity, and standing for 30min;
(3) And (3) testing the capacity retention rate of the normal temperature circulation 500 weeks after the circulation (1) - (2).
TABLE 1
From the test results of table 1, it can be seen that:
1. according to the embodiment and the comparative example, the arrangement of the plurality of anode active material layers is beneficial to the improvement of the overall performance of the battery, and meanwhile, the dopamine-coated silicon-containing compound serving as a silicon-based anode material can improve the maximum charging rate of the lithium ion battery, because the surface of the dopamine-coated silicon-containing compound is provided with hydroxyl and amino functional groups, the dipole moment interacted with lithium ions can be improved, so that the diffusion coefficient of the lithium ions in the anode is improved, and the maximum charging rate of the lithium ion battery is further improved.
2. The test results of the examples and the comparative examples show that the cycle performance of the battery can be further improved by adopting polyacrylonitrile or a mixture of polyacrylonitrile and polyacrylic acid as the binder, on the one hand, due to the interaction of the binders in the first coating and the second coating, on the other hand, the dopamine coating has better promotion effect on the binder system consisting of polyacrylonitrile and polyacrylic acid, the performance of the battery is further improved, and the cycle performance and the maximum charging rate of the lithium ion battery prepared by adopting the scheme are better.
From the above, the embodiment of the application provides a negative electrode plate and a lithium ion battery, which can effectively solve the problem that the high energy density and the rapid charging capability of the lithium ion battery in the prior art cannot be achieved.
The foregoing has described in detail a negative electrode tab and a lithium ion battery provided in the present application, and specific examples have been applied herein to illustrate the principles and embodiments of the present application, where the foregoing examples are provided to assist in understanding the methods of the present application and the core ideas thereof; also, as will occur to those of ordinary skill in the art, many modifications are possible in view of the teachings of the present application, both in the detailed description and the scope of its applications. In view of the foregoing, this description should not be construed as limiting the application.

Claims (7)

1. The negative electrode plate is characterized by comprising a negative electrode current collector, a first coating arranged on the negative electrode current collector and a second coating arranged on the first coating;
the first coating comprises a negative electrode active material, a first negative electrode conductive agent and a first negative electrode binder, wherein the negative electrode active material comprises a silicon-based negative electrode material and hard carbon-coated graphite;
the second coating comprises graphite coated by hard carbon, a second negative electrode conductive agent and a second negative electrode binder;
the silicon-based anode material comprises a silicon-containing compound and dopamine coated on the surface of the silicon-containing compound;
the first negative electrode conductive agent comprises vapor grown carbon fibers, conductive carbon black and single-walled carbon nanotubes, and the second negative electrode conductive agent comprises single-walled carbon nanotubes and conductive carbon black.
2. The negative electrode tab of claim 1 wherein the silicon-containing compound comprises at least one of silicon oxide, silicon carbide.
3. The negative electrode tab of claim 1, wherein the first coating has a thickness of 50% -70% of the sum of the thicknesses of the first coating and the second coating, and the second coating has a thickness of 30% -50% of the sum of the thicknesses of the first coating and the second coating.
4. The negative electrode sheet according to claim 1, wherein the mass fraction of the silicon-containing compound in the negative electrode active material is 5% -20%.
5. The negative electrode tab of claim 1, wherein the first negative electrode binder comprises at least one of polyacrylic acid or polyacrylonitrile;
and/or the number of the groups of groups,
the second negative electrode binder includes at least one of carboxymethyl cellulose, styrene-butadiene rubber, or polyacrylic acid.
6. The negative electrode tab of claim 1, wherein the negative current collector comprises a carbon coated copper foil.
7. A lithium ion battery comprising a positive electrode sheet, a negative electrode sheet and an electrolyte, wherein the negative electrode sheet is the negative electrode sheet according to any one of claims 1 to 6.
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