CN111725511B - Lithium ion secondary battery pole piece and lithium ion secondary battery - Google Patents
Lithium ion secondary battery pole piece and lithium ion secondary battery Download PDFInfo
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- CN111725511B CN111725511B CN202010602745.0A CN202010602745A CN111725511B CN 111725511 B CN111725511 B CN 111725511B CN 202010602745 A CN202010602745 A CN 202010602745A CN 111725511 B CN111725511 B CN 111725511B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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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
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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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
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- 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
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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a lithium ion secondary battery pole piece which comprises a current collector and an active substance layer coated on at least one surface of the current collector, wherein a porous insulating coating is coated on the surface of the active substance layer, the porous insulating coating comprises dopamine-coated inorganic particles and a first binder, and an organic coating is further coated on the surface of the porous insulating coating and is distributed in an island shape and/or a linear shape. The invention solves the problem that the performance of the battery is influenced by the inorganic porous layer coated on the surface of the diaphragm, and also solves the safety problem caused by the expansion of the negative electrode in the circulating process.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a lithium ion secondary battery pole piece and a lithium ion secondary battery.
Background
Since the commercialization of lithium ion secondary batteries was realized in the 90 s, lithium ion secondary batteries have been widely used in the fields of mobile phones, notebook computers, tablet computers, bluetooth headsets, MP3, digital cameras, and the like, due to their characteristics of high energy density, high operating voltage, light weight, and the like.
The lithium ion battery mainly comprises a positive pole piece, a negative pole piece and a diaphragm arranged between the positive pole piece and the negative pole piece, wherein the diaphragm is used for isolating the positive pole and the negative pole and preventing the positive pole and the negative pole from being in direct contact with each other to generate short circuit. At present, the diaphragm is mainly a porous medium composed of polyolefins such as polyethylene, polypropylene and the like, the polyolefin diaphragm has a melting point of 200 ℃ or lower, when the temperature of the battery is increased due to short circuit caused by internal or external factors, the contact short circuit of a positive electrode and a negative electrode caused by shrinkage is easy to occur, and even the thermal runaway of the battery is caused to cause fire accidents. In addition, the surface of the pole piece is uneven, or sharp foreign matters mixed in the battery assembly process are easy to damage the diaphragm to cause short circuit, and the battery is penetrated by a sharp object to cause short circuit.
In order to solve the above problems, a porous insulating layer made of inorganic particles has been coated on the surface of the separator, and the porous insulating layer can prevent the positive electrode and the negative electrode from directly contacting each other when the separator is shrunk or damaged, thereby preventing the occurrence of fire.
However, in the above-mentioned technology, since lithium ions need to pass through the porous layer to generate a battery path, the porous layer composed of inorganic particles has poor wettability of a polymer with an electrolyte solution, resulting in poor ion conductivity of the porous layer, and since the porous layer composed of inorganic particles is an insulating layer for improving safety, the interfacial resistance of the battery increases, affecting the dynamic performance and cycle performance of the battery.
In addition, the negative active material in the lithium ion battery has high expansion rate in the charging and discharging processes of the battery, so that the battery is seriously deformed, and the porous layer formed by inorganic particles is cracked due to the deformation of the battery in the charging and discharging use processes of the battery, so that the effect of inhibiting the internal short circuit is insufficient, and the safety problem of the battery is reduced.
Disclosure of Invention
One of the objects of the present invention is: aiming at the defects of the prior art, the lithium ion secondary battery pole piece is provided, which can avoid the influence of the inorganic porous layer coated on the surface of the diaphragm on the performance of the battery and can also avoid the safety problem caused by the expansion of the negative electrode in the circulating process.
In order to achieve the purpose, the invention adopts the following technical scheme:
the utility model provides a lithium ion secondary battery pole piece, includes the mass flow body, coats the active material layer on the at least one surface of mass flow body, the surface coating porous insulating coating on active material layer, porous insulating coating includes dopamine cladding's inorganic particle and first binder, porous insulating coating's surface still coats organic coating, organic coating is island and/or linear distribution.
It should be noted that, because dopamine has good imbibition capability, the imbibition performance of the porous insulating coating is further improved. The dopamine can be polymerized on the surface of the inorganic particle, the particle size of the dopamine particle is far smaller than that of the inorganic particle, and the dopamine particle attached to the surface of the inorganic particle is equivalent to increase of a pore channel of the porous insulating coating, so that the dopamine particle is more beneficial to the passing of lithium ions, especially the migration of the lithium ions under high multiplying power, and further the discharge performance of the battery is improved.
It should be noted that the amount of the dopamine particles accumulated on the surface of the inorganic particles cannot be too much, and the too much dopamine particles completely coat the inorganic particles, so that the pore channels and the pore diameters of the porous insulating coating are reduced, and the lithium ions are not facilitated to pass through.
As an improvement of the lithium ion secondary battery pole piece, the coating area ratio of the organic coating to the porous insulating coating is 0.5-0.95: 1. When the active material layer is the negative electrode active material layer and the negative electrode active material is selected from graphite, in the cycle process of the battery, the distribution of the island-shaped and/or linear organic coating provides a space required by the expansion of the negative electrode graphite, the deformation problem in the cycle process of the battery is solved, the porous insulating coating is prevented from cracking, and good safety performance is maintained. Among them, the organic coating layer cannot be coated in an excessive area because the organic coating layer has an ability to absorb an electrolyte, and the organic coating layer increases in area after imbibing and swelling, which may cause deformation of the addition-polymerization battery. The coating area of the organic coating cannot be too small, the amount of the electrolyte absorbed by the too small coating area is too small, the ion conductivity of the organic coating cannot be improved, and the cycle performance of the battery cannot be sufficiently improved.
As an improvement of the lithium ion secondary battery electrode plate of the present invention, the inorganic particles include at least one of calcium oxide, zinc oxide, magnesium oxide, titanium dioxide, silicon dioxide, zirconium dioxide, tin dioxide, cerium dioxide, aluminum oxide, calcium carbonate, and barium titanate, and the first binder includes at least one of styrene-butadiene polymer, polyvinylidene fluoride-hexafluoropropylene, polyacrylic acid, polymethacrylic acid, polyacrylate polymer, polymethyl acrylate, polyethyl acrylate, methyl methacrylate, polyacrylonitrile, sodium carboxymethylcellulose, butadiene-acrylonitrile polymer, polyvinylpyrrolidone, and polyacrylic acid-styrene polymer. The inorganic particles are not particularly limited as long as they are not oxidized or reduced in the lithium ion secondary battery and have excellent electronic insulation properties. The first binder is used for binding the inorganic particles with each other and ensuring the structural stability of the porous insulating coating.
As an improvement of the lithium ion secondary battery pole piece, the particle size of the inorganic particles is 0.001-20 μm, and the mass ratio of the inorganic particles to the first binder is 1: 99-99.9: 1. Preferably, the particle size of the inorganic particles is 0.1 to 10 μm. The too large particle size of the inorganic particles may result in too large pore size of the porous insulating coating.
As an improvement of the lithium ion secondary battery pole piece, the thickness of the porous insulating coating is 0.5-50 mu m, the aperture of the porous insulating coating is 0.001-10 mu m, and the porosity of the porous insulating coating is 5-95%. Preferably, the thickness of the porous insulating coating is 1-10 mu m, the aperture of the porous insulating coating is 0.1-5 mu m, and the porosity of the porous insulating coating is 30-60%. The too large thickness of the porous insulating coating can slow down the migration rate of lithium ions and the charge and discharge rate of the battery; the thickness of the porous insulating coating is too small, and the anode and the cathode of the battery still have the possibility of contact. The pore size of the porous insulating coating is too small, which also affects the migration rate of lithium ions.
As an improvement of the lithium ion secondary battery pole piece, the organic coating comprises organic particles and a second binder, the organic particles comprise at least one of polyvinylidene fluoride, vinylidene fluoride-hexafluoropropylene polymer, polyvinylidene fluoride-co-hexafluoropropylene, polyvinylidene fluoride-co-trichloroethylene, polymethyl methacrylate, polyethylene oxide, polyacrylonitrile, polyvinylpyrrolidone, polyvinyl acetate, polyimide, acrylonitrile-butadiene copolymer and acrylonitrile-styrene-butadiene copolymer, and the second binder comprises styrene-butadiene polymer, polyvinylidene fluoride-hexafluoropropylene, polyvinylpyrrolidone, polyacrylonitrile, sodium carboxymethylcellulose, polyacrylic acid, polymethyl acrylate, polymethyl methacrylate, polypropylene oxide, polyvinyl chloride, At least one of polyethylacrylate, methyl methacrylate, sodium polyacrylate, polyacrylic acid-styrene polymer, and ethyl acetate. The organic particles include, but are not limited to, the above-mentioned ones, as long as the organic particles can absorb the electrolyte and swell in the electrolyte. The second binder is used to bind the organic particles.
As an improvement of the lithium ion secondary battery pole piece, the particle size of the organic particles is 0.001-10 mm, and the mass ratio of the organic particles to the second binder is 1: 99-99.9: 0.1. Preferably, the particle size of the organic particles is 0.005um to 500 μm, and the mass ratio of the organic particles to the second binder is 30:99 to 99.9: 0.1.
As an improvement of the pole piece of the lithium ion secondary battery, the organic coating further comprises a fast ion conductor, and the fast ion conductor comprises at least one of an NASICON type oxide fast ion conductor, a LiPON type fast ion conductor and a garnet type fast ion conductor. The fast ion conductor is also called as solid electrolyte, and has relatively high ion conductivity in a solid state, and lithium ions can be directly transmitted through the fast ion conductor. The lithium ion battery has the advantages that the transmission of lithium ions is accelerated, and the charge and discharge rate of the lithium ion battery can be effectively improved. The fast ion conductor does not store or release lithium ions to participate in electrochemical reaction, and the fast ion conductor is used for conducting the lithium ions.
As an improvement of the lithium ion secondary battery pole piece, when the organic coating is in an island shape, the area of each island-shaped organic coating is 0.025 mu m2～500mm2The height of the organic coating is 0.05 um-100 um; when the organic coating is in the form of a wire, the organic layerThe width of coating is 0.05um ~10mm, the length of organic coating is 0.5um ~50mm, the height of organic coating is 0.5um ~100 um.
The invention also provides a lithium ion secondary battery, which comprises a positive plate, a negative plate and electrolyte, wherein the positive plate or the negative plate is the lithium ion secondary battery plate described in any one of the specifications. Wherein the electrolyte is liquid electrolyte. The lithium ion secondary battery can not comprise a diaphragm, and the porous insulating coating arranged on the surface of the active material layer can replace the diaphragm, so that the direct contact between the positive plate and the negative plate can be avoided, and the lithium ions can be transmitted between the positive electrode and the negative electrode.
As an improvement of the lithium ion secondary battery of the present invention, a separator is further included between the positive electrode tab and the negative electrode tab. Preferably, the present invention may also include a separator, which may be specifically configured as any one of a polyethylene film, a polypropylene film, and a polyethylene-polypropylene composite film. Further preferably, the separator comprises a substrate layer and a functional coating layer compounded on at least one surface of the substrate layer, wherein the functional coating layer comprises a zeolite-like imidazole framework compound. Still more preferably, the zeolitic imidazolate framework compound is ZIF-21 or ZIF-67. Because the zeolite-like imidazole framework compound has good hydrophilic performance, the wettability of the diaphragm can be improved, and the cycle performance of the battery can be further improved. In addition, gaps with good connection are formed among zeolite-like imidazole framework compounds in the functional coating, so that the gaps can be filled with electrolyte, and good channels are provided for migration of lithium ions. The zeolite-like imidazole framework compound is tightly attached to the surface of the base material layer, so that the migration of lithium ions between the zeolite-like imidazole framework compound is facilitated, and the interface impedance between the diaphragm and the pole piece is reduced.
Compared with the prior art, the beneficial effects of the invention include but are not limited to:
1) the porous insulating coating can insulate the positive electrode and the negative electrode when the temperature of the battery is increased due to the internal or external factors and the positive electrode and the negative electrode are in direct contact due to the contraction of the diaphragm, so that the occurrence of short circuit is prevented, and the fire accident caused by the thermal runaway of the battery is prevented.
2) The dopamine is coated on the surface of the inorganic particles, and the dopamine has good imbibition capability, so that the imbibition performance of the porous insulating coating is improved. The dopamine can be polymerized on the surface of the inorganic particle, the particle size of the dopamine particle is far smaller than that of the inorganic particle, and the dopamine particle attached to the surface of the inorganic particle is equivalent to increase of a pore channel of the porous insulating coating, so that the dopamine particle is more beneficial to the passing of lithium ions, especially the migration of the lithium ions under high multiplying power, and further the discharge performance of the battery is improved.
3) The organic coating has good electrolyte absorption capacity, and improves the ion conductivity of the organic coating, so that the lithium ion battery has better cycle performance; in addition, under the pressure in the production process of the lithium ion battery, the organic coating and the diaphragm keep good bonding force, and interface impedance can be obviously reduced, so that the dynamic performance and the cycle performance of the battery are improved.
4) The organic coating is distributed in an island shape and/or a linear shape, so that a space required by the expansion of the negative electrode graphite is provided in the battery circulation process, the deformation problem in the battery circulation process is solved, the porous insulating coating is prevented from cracking, and the good safety performance of the battery is ensured.
Detailed Description
In order to make the technical solutions and advantages of the present invention clearer, the technical solutions of the present invention will be clearly and completely described below with reference to specific embodiments, and it is obvious that the described embodiments are some, but not all embodiments of the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The invention provides a lithium ion secondary battery pole piece which comprises a current collector and an active substance layer coated on at least one surface of the current collector, wherein the surface of the active substance layer is coated with a porous insulating coating, the porous insulating coating comprises dopamine-coated inorganic particles and a first binder, the surface of the porous insulating coating is also coated with an organic coating, and the organic coating is distributed in an island shape and/or a linear shape.
Furthermore, the coating area ratio of the organic coating to the porous insulating coating is 0.5-0.95: 1. Specifically, the coating area ratio of the organic coating layer to the porous insulating coating layer is 0.5:1, 0.6:1, 0.7:1, 0.8:1, 0.9:1, or 0.95: 1.
Further, the inorganic particles include at least one of calcium oxide, zinc oxide, magnesium oxide, titanium dioxide, silicon dioxide, zirconium dioxide, tin dioxide, cerium dioxide, aluminum oxide, calcium carbonate, and barium titanate, and the first binder includes at least one of styrene-butadiene polymer, polyvinylidene fluoride-hexafluoropropylene, polyacrylic acid, polymethacrylic acid, polyacrylate polymer, polymethyl acrylate, polyethyl acrylate, methyl methacrylate, polyacrylonitrile, sodium carboxymethylcellulose, butadiene-acrylonitrile polymer, polyvinylpyrrolidone, and polyacrylic acid-styrene polymer. The preparation method of the dopamine-coated inorganic particles comprises the following steps: adding dopamine into a Tris solution, adding inorganic particles, stirring, and evaporating the solution to prepare the inorganic particles with the surfaces modified by the dopamine.
Further, the particle size of the inorganic particles is 0.001-20 μm, and the mass ratio of the inorganic particles to the first binder is 1: 99-99.9: 1. Preferably, the particle size of the inorganic particles is 0.1 to 10 μm. Further preferably, the particle diameter of the inorganic particles is 1 μm, 2 μm, 3 μm, 4 μm, 5 μm, 6 μm, 7 μm, 8 μm, 9 μm or 10 μm.
Furthermore, the thickness of the porous insulating coating is 0.5-50 μm, the aperture of the porous insulating coating is 0.001-10 um, and the porosity of the porous insulating coating is 5-95%. Preferably, the thickness of the porous insulating coating is 1 μm, 2 μm, 3 μm, 4 μm, 5 μm, 6 μm, 7 μm, 8 μm, 9 μm or 10 μm.
Further, the organic coating includes organic particles and a second binder, the organic particles include at least one of polyvinylidene fluoride, vinylidene fluoride-hexafluoropropylene polymer, polyvinylidene fluoride-co-hexafluoropropylene, polyvinylidene fluoride-co-trichloroethylene, polymethyl methacrylate, polyethylene oxide, polyacrylonitrile, polyvinylpyrrolidone, polyvinyl acetate, polyimide, acrylonitrile-butadiene copolymer, and acrylonitrile-styrene-butadiene copolymer, the second binder comprises at least one of styrene-butadiene polymer, polyvinylidene fluoride-hexafluoropropylene, polyvinylpyrrolidone, polyacrylonitrile, sodium carboxymethylcellulose, polyacrylic acid, polymethyl acrylate, polyethyl acrylate, methyl methacrylate, sodium polyacrylate, polyacrylic acid-styrene polymer and ethyl acetate.
Furthermore, the particle size of the organic particles is 0.001-10 mm, and the mass ratio of the organic particles to the second binder is 1: 99-99.9: 0.1. Preferably, the particle size of the organic particles is 0.005um to 500 μm, and the mass ratio of the organic particles to the second binder is 30:99 to 99.9: 0.1. Further preferably, the particle size of the organic particles is 0.005. mu.m, 0.1. mu.m, 1. mu.m, 10. mu.m, 50. mu.m, 100. mu.m, 150. mu.m, 200. mu.m, 250. mu.m, 300. mu.m, 350. mu.m, 400. mu.m, 450. mu.m or 500. mu.m. Further preferably, the mass ratio of the organic particles to the second binder is 30:99, 50:99, 70:99, 99:70, 99:50, 99:30, 99:10, 99:1 or 99.1: 0.1.
Further, the organic coating layer further comprises fast ion conductors including NASICON type oxide fast ion conductors, LiPON type fast ion conductors, and garnet type fast ion conductors. The fast ion conductor is also called as solid electrolyte, and has relatively high ion conductivity in a solid state, and lithium ions can be directly transmitted through the fast ion conductor. The lithium ion battery has the advantages that the transmission of lithium ions is accelerated, and the charge and discharge rate of the lithium ion battery can be effectively improved.
Further, when the organic coating layer is in the form of islands, the area of each island-shaped organic coating layer is 0.025 μm2～500mm2The height of the organic coating is 0.05 um-100 um; when the organic coating is linear, the width of the organic coating is 0.05 um-10 mm, the length of the organic coating is 0.5 um-50 mm, and the height of the organic coating is 0.5 um-100 um. Preferably, when the organic coating is island-shaped, the area of the organic coating is 0.05mm2、1mm2、2mm2、3mm2、4mm2、5mm2、6mm2、7mm2、8mm2、9mm2Or 10mm2The height of the organic coating is 0.05um, 10um, 20um, 30um, 40um, 50um, 60um, 70um, 80um, 90um or 100 um. Preferably, when the organic coating is linear distribution, the width of the organic coating is 0.05um, 1um, 2um, 3um, 4um, 5um, 6um, 7um, 8um, 9um or 10um, the length of the organic coating is 0.5um, 5um, 10um, 15um, 20um, 25um, 30um, 35um, 40um, 45um or 50um, the height of the organic coating is 0.5um, 10um, 20um, 30um, 40um, 50um, 60um, 70um, 80um, 90um or 100 um.
The pole piece of the lithium ion secondary battery can be manufactured according to the following method, and the steps comprise the following steps: coating a porous insulating coating on the surface of the active material layer; and coating an organic coating on the surface of the porous insulating coating.
(1) Preparing a porous insulating coating: dissolving a first binder in a first solvent to form a polymer solution, adding dopamine-coated inorganic particles and mixing uniformly, uniformly coating the prepared mixture on the surface of an active material layer, and then drying to obtain a porous insulating coating. The first solvent that may be used is not particularly limited, and may be one that can dissolve the first binder and uniformly disperse the inorganic particles and can be easily removed in coating and drying, and includes, but is not limited to, tetrahydrofuran, methyl ethyl ketone, dimethylformamide, dimethylacetamide, tetramethylurea, tetramethylphosphate, acetone, dichloromethane, chloroform, dimethylamide, N-methylpyrrolidone (NMP), cyclohexane, water, and a mixture thereof. The concentration of the first binder is 1 to 99 wt%, preferably 30 to 60 wt%. For coating the mixture of dopamine-coated inorganic particles and a binder on the surface of the active material layer, any method known in the art may be used, and usable methods include: dip coating, die coating, roll coating, comma transfer coating, gravure coating, or combinations thereof.
(2) Preparation of organic coating: dissolving a second binder in a second solvent to form a polymer solution, adding organic particles and mixing uniformly, uniformly coating the prepared mixture on the surface of the porous insulating coating, and drying to obtain the organic coating. The solvent that can be used is not particularly limited, and it is sufficient that the second binder can be dissolved and the organic particles can be uniformly dispersed and can be easily removed in coating and drying, and the second solvent includes, but is not limited to, tetrahydrofuran, methyl ethyl ketone, dimethylformamide, dimethylacetamide, tetramethylurea, tetramethylphosphate, acetone, dichloromethane, chloroform, dimethylformamide, N-methylpyrrolidone (NMP), cyclohexane, ethyl acetate, water, and a mixture thereof. The concentration of the second binder is 1 to 99 wt%, preferably 5 to 50 wt%. In order to coat the mixture of the organic particles and the second binder on the surface of the porous insulating coating layer to form island-like or line-like distribution, any method known in the art may be used, and usable methods include: dip coating, die coating, roll coating, comma transfer coating, gravure coating, screen printing, spray coating, cast coating, or combinations thereof.
Example 1
(1) Preparing a positive plate: mixing lithium cobaltate, conductive carbon and a binder polyvinylidene fluoride according to a mass ratio of 96: 2.0: 2.0 evenly mixing the raw materials in an N-methyl pyrrolidone (NMP) solvent to prepare anode slurry, then coating the anode slurry on an aluminum foil, drying the aluminum foil at 110 ℃ to obtain an anode plate, and cold pressing the anode plate for later use.
Preparing a porous insulating coating: adding 13 wt% of polyacrylate emulsion (40% of the aqueous solution) into deionized water, stirring for 1h, and adding 85 wt% of dopamine-coated Al2O3And after the particles are stirred for 2 hours, grinding the particles in a ball mill for 1 hour, adding 2 wt% of sodium carboxymethyl cellulose (CMC) into the ground slurry, and continuously stirring for 1 hour to prepare the slurry. And then, uniformly covering the prepared slurry on two surfaces of the cold-pressed positive electrode by using gravure coating, wherein the thickness of the two-surface coating is 5um respectively, and preparing the prepared pole piece for later use.
The preparation of the organic coating comprises the steps of firstly adding 40 wt% of ethyl acetate into an N-methylpyrrolidone (NMP) solvent, stirring for 1h, then adding 60 wt% of polyvinylidene fluoride (PVDF) powder, and uniformly stirring for 2h to obtain an organic glue solution. And coating the pole piece coated with the porous insulating coating by adopting a dip-coating mode. Organic coating on porous insulating coatingDistributed in island shape, and each island-shaped organic coating has an area of 1mm2And the height is 10 um. Then the pole piece is subjected to slitting, edge cutting and tab welding to prepare the positive plate.
(2) Preparing the negative plate by mixing graphite, conductive carbon, thickener sodium carboxymethyl cellulose and binder styrene butadiene rubber according to a mass ratio of 95: 2.0: 1.0: 2.0 evenly mixing in deionized water to prepare cathode slurry, then coating the cathode slurry on a copper foil, drying at 85 ℃, cold pressing, splitting, cutting edges, and welding tabs to prepare a cathode sheet.
(3) A diaphragm: a polyethylene microporous film with the thickness of 16um is taken as a separation film.
(4) The preparation of the battery comprises the steps of winding the positive plate, the isolating film and the negative plate into a battery core, then placing the battery core into an aluminum-plastic packaging bag, injecting an electrolyte (ethylene carbonate: dimethyl carbonate: methyl ethyl carbonate: 1:2:1, containing 1M lithium hexafluorophosphate), packaging, forming, capacity and the like to prepare the lithium ion secondary battery.
Example 2
(1) Preparing a positive plate: mixing lithium cobaltate, conductive carbon and a binder polyvinylidene fluoride according to a mass ratio of 96: 2.0: 2.0 mixing evenly in N-methyl pyrrolidone (NMP) solvent to prepare anode slurry, then coating on aluminum foil, drying at 110 ℃, cold pressing, splitting, cutting edges, and welding tabs to prepare the anode plate.
(2) Preparing the negative plate by mixing graphite, conductive carbon, thickener sodium carboxymethyl cellulose and binder styrene butadiene rubber according to a mass ratio of 95: 2.0: 1.0: 2.0 evenly mixing in deionized water to prepare cathode slurry, then coating the cathode slurry on a copper foil, drying at 85 ℃ and cold pressing for later use.
Preparing a porous insulating coating: adding 13 wt% of polyacrylate emulsion (40% of the aqueous solution) into deionized water, stirring for 1h, and adding 85 wt% of dopamine-coated Al2O3And after the particles are stirred for 2 hours, grinding the particles in a ball mill for 1 hour, adding 2 wt% of sodium carboxymethyl cellulose (CMC) into the ground slurry, and continuously stirring for 1 hour to prepare the slurry. Then the prepared slurry is uniformly covered on the two cold-pressed negative electrodes by gravure coatingOn the surface, the thickness of the two coating layers is respectively 5um, and the prepared pole piece is ready for use.
The preparation of the organic coating comprises the steps of firstly adding 40 wt% of ethyl acetate into an N-methylpyrrolidone (NMP) solvent, stirring for 1h, then adding 60 wt% of polyvinylidene fluoride (PVDF) powder, and uniformly stirring for 2h to obtain an organic glue solution. And coating the pole piece coated with the porous insulating coating by adopting a dip-coating mode. The organic matter coating is in linear distribution on porous insulating coating, and the width of linear coating is 1mm, and length is 10mm, and is highly 10 um. Then the pole piece is subjected to slitting, edge cutting and tab welding to manufacture the negative pole piece.
(3) A diaphragm: a polyethylene microporous film with the thickness of 16um is taken as a separation film.
(4) The preparation of the battery comprises the steps of winding the positive plate, the isolating film and the negative plate into a battery core, then placing the battery core into an aluminum-plastic packaging bag, injecting an electrolyte (ethylene carbonate: dimethyl carbonate: methyl ethyl carbonate: 1:2:1, containing 1M lithium hexafluorophosphate), packaging, forming, capacity and the like to prepare the lithium ion secondary battery.
Comparative example 1
(1) Preparing a positive plate: mixing lithium cobaltate, conductive carbon and a binder polyvinylidene fluoride according to a mass ratio of 96: 2.0: 2.0 mixing evenly in N-methyl pyrrolidone (NMP) solvent to prepare anode slurry, then coating on aluminum foil, drying at 110 ℃, cold pressing, splitting, cutting edges, and welding tabs to prepare the anode plate.
(2) Preparing the negative plate by mixing graphite, conductive carbon, thickener sodium carboxymethyl cellulose and binder styrene butadiene rubber according to a mass ratio of 95: 2.0: 1.0: 2.0 evenly mixing in deionized water to prepare cathode slurry, then coating the cathode slurry on a copper foil, drying at 85 ℃, cold pressing, splitting, cutting edges, and welding tabs to prepare a cathode sheet.
(3) A diaphragm: a polyethylene microporous film with the thickness of 16um is taken as a separation film.
(4) The preparation of the battery comprises the steps of winding the positive plate, the isolating film and the negative plate into a battery core, then placing the battery core into an aluminum-plastic packaging bag, injecting an electrolyte (ethylene carbonate: dimethyl carbonate: methyl ethyl carbonate: 1:2:1, containing 1M lithium hexafluorophosphate), packaging, forming, capacity and the like to prepare the lithium ion secondary battery.
Comparative example 2
(1) Preparing a positive plate: mixing lithium cobaltate, conductive carbon and a binder polyvinylidene fluoride according to a mass ratio of 96: 2.0: 2.0 evenly mixing the raw materials in an N-methyl pyrrolidone (NMP) solvent to prepare anode slurry, then coating the anode slurry on an aluminum foil, drying the aluminum foil at 110 ℃ to obtain an anode plate, and cold pressing the anode plate for later use.
Preparing a porous insulating coating: adding 13 wt% of polyacrylate emulsion (the content of the aqueous solution is 40%) into deionized water, stirring for 1h, and then adding 85 wt% of Al2O3And after the particles are stirred for 2 hours, grinding the particles in a ball mill for 1 hour, adding 2 wt% of sodium carboxymethyl cellulose (CMC) into the ground slurry, and continuously stirring for 1 hour to prepare the slurry. And then, uniformly covering the two surfaces of the cold-pressed positive electrode with the prepared slurry by using gravure coating, wherein the thickness of each coating on the two surfaces is 5 micrometers, and then, carrying out strip division, edge cutting and tab welding on the pole piece to prepare the positive plate.
(2) Preparing the negative plate by mixing graphite, conductive carbon, thickener sodium carboxymethyl cellulose and binder styrene butadiene rubber according to a mass ratio of 95: 2.0: 1.0: 2.0 evenly mixing in deionized water to prepare cathode slurry, then coating the cathode slurry on a copper foil, drying at 85 ℃, cold pressing, splitting, cutting edges, and welding tabs to prepare a cathode sheet.
(3) A diaphragm: a polyethylene microporous film with the thickness of 16um is taken as a separation film.
(4) The preparation of the battery comprises the steps of winding the positive plate, the isolating film and the negative plate into a battery core, then placing the battery core into an aluminum-plastic packaging bag, injecting an electrolyte (ethylene carbonate: dimethyl carbonate: methyl ethyl carbonate: 1:2:1, containing 1M lithium hexafluorophosphate), packaging, forming, capacity and the like to prepare the lithium ion secondary battery.
Comparative example 3
(1) Preparing a positive plate: mixing lithium cobaltate, conductive carbon and a binder polyvinylidene fluoride according to a mass ratio of 96: 2.0: 2.0 mixing evenly in N-methyl pyrrolidone (NMP) solvent to prepare anode slurry, then coating on aluminum foil, drying at 110 ℃, cold pressing, splitting, cutting edges, and welding tabs to prepare the anode plate.
(2) Preparing the negative plate by mixing graphite, conductive carbon, thickener sodium carboxymethyl cellulose and binder styrene butadiene rubber according to a mass ratio of 95: 2.0: 1.0: 2.0 evenly mixing in deionized water to prepare cathode slurry, then coating the cathode slurry on a copper foil, drying at 85 ℃ and cold pressing for later use.
Preparing a porous insulating coating: adding 13 wt% of polyacrylate emulsion (the content of the aqueous solution is 40%) into deionized water, stirring for 1h, and then adding 85 wt% of Al2O3And after the particles are stirred for 2 hours, grinding the particles in a ball mill for 1 hour, adding 2 wt% of sodium carboxymethyl cellulose (CMC) into the ground slurry, and continuously stirring for 1 hour to prepare the slurry. And then, uniformly covering the two surfaces of the cold-pressed negative electrode with the prepared slurry by using gravure coating, wherein the thicknesses of the two coating layers are respectively 5 micrometers, and then, carrying out strip division, edge cutting and tab welding on the pole piece to prepare the negative pole piece.
(3) A diaphragm: a polyethylene microporous film with the thickness of 16um is taken as a separation film.
(4) The preparation of the battery comprises the steps of winding the positive plate, the isolating film and the negative plate into a battery core, then placing the battery core into an aluminum-plastic packaging bag, injecting an electrolyte (ethylene carbonate: dimethyl carbonate: methyl ethyl carbonate: 1:2:1, containing 1M lithium hexafluorophosphate), packaging, forming, capacity and the like to prepare the lithium ion secondary battery.
The lithium ion batteries of the above comparative examples and examples were subjected to discharge rate test and cycle performance test, and the lithium ion batteries of the above comparative examples and examples were subjected to nail penetration safety test before and after cycle.
(1) Testing discharge multiplying power, namely firstly charging the lithium ion secondary battery at 25 ℃ by adopting multiplying power of 0.5C, discharging at 0.2C multiplying power, and recording discharge capacity; then charging at 0.5C multiplying power, discharging at 0.5C multiplying power, and recording the discharge capacity; then charging at 0.5C multiplying power, discharging at 1.0C multiplying power, and recording the discharge capacity; then charging at 0.5C multiplying power, discharging at 1.5C multiplying power, and recording the discharge capacity; and finally, charging at 0.5C multiplying power, discharging at 2.0C multiplying power, and recording the discharge capacity. Capacity retention rate at each different discharge rate (discharge capacity at each rate/discharge capacity at 0.2C rate) 100%. The results are shown in Table 1.
(2) And (3) cycle performance test, namely charging the lithium ion secondary battery at 25 ℃ by adopting a rate of 0.5C, discharging at a rate of 0.5C, sequentially performing 500 cycles, testing the battery capacity at the rate of 0.5C in each cycle, comparing the battery capacity at 25 ℃ with the battery capacity before the cycle, and calculating the capacity retention rate after the cycle, wherein the capacity retention rate is 100 percent (the capacity at the rate of 0.5C after the cycle/the capacity at 25 ℃ of the battery before the cycle). The thickness of the fully charged cell after 500 cycles was measured and compared with the thickness of the fully charged cell before cycle, and the thickness expansion rate of the cell was calculated as [ (thickness of the cell after full charge after cycle-thickness of the cell before cycle)/thickness of the fully charged cell before cycle ] × 100%. The results are shown in Table 2.
(3) And (3) nail penetration testing: the battery was fully charged and then tested according to UL1642 with a nail diameter of 2.5mm and a nail penetration speed of 100 mm/s. And respectively carrying out nail penetration safety test on the battery before circulation and the battery after 500 circulations. The test results are shown in Table 3.
TABLE 1 Capacity Retention ratio at different discharge rates for comparative example and example
| Group of | 0.2C | 0.5C | 1.0C | 1.5C | 2.0C |
| Comparative example 1 | 100％ | 98％ | 94％ | 88％ | 82％ |
| Comparative example 2 | 100％ | 96％ | 92％ | 85％ | 76％ |
| Comparative example 3 | 100％ | 96％ | 92％ | 86％ | 77％ |
| Example 1 | 100％ | 98％ | 95％ | 92％ | 86％ |
| Example 2 | 100％ | 98％ | 96％ | 91％ | 85％ |
TABLE 2 test results of the retention of cyclic capacity and the expansion of thickness for comparative and example
| Group of | Capacity retention rate | Rate of thickness expansion |
| Comparative example 1 | 85％ | 23％ |
| Comparative example 2 | 80％ | 25％ |
| Comparative example 3 | 81％ | 24％ |
| Example 1 | 87％ | 6％ |
| Example 2 | 88％ | 5％ |
Table 3 nail penetration test results of battery before and after cycle
As can be seen from table 1, the battery discharge rate performance is significantly improved by coating a porous insulating coating on the surface of the electrode plate, as compared with the comparative example, the lithium ion secondary battery of the present invention has a significantly improved discharge rate performance, because the dopamine-coated modified inorganic particles can increase the pore channels of the porous insulating coating, which is more conducive to the passage of lithium ions, especially to the migration of lithium ions at high rates, thereby improving the discharge performance of the battery.
As can be seen from table 2, after a layer of porous insulating coating is coated on the surface of the pole piece, the cycle performance of the battery will be deteriorated, but the cycle performance of the lithium ion secondary battery of the present invention is not affected, but is improved. In addition, the problem of large thickness expansion cannot be solved by coating a layer of porous insulating coating on the surface of the pole piece, and the battery can obviously reduce the thickness expansion of the battery. The organic coating has good electrolyte absorption capacity, and improves the ion conductivity of the organic coating, so that the lithium ion battery has better cycle performance; in addition, under the pressure in the production process of the lithium ion battery, the organic coating and the diaphragm keep good bonding force, and interface impedance can be obviously reduced, so that the dynamic performance and the cycle performance of the battery are improved. The organic coating is distributed in an island shape and/or a linear shape, so that a space required by the expansion of the negative electrode graphite is provided in the battery circulation process, the deformation problem in the battery circulation process is solved, the porous insulating coating is prevented from cracking, and the good safety performance of the battery is ensured.
As can be seen from table 3, after the surface of the pole piece is coated with a porous insulating coating, the safety performance of the battery is obviously improved, but the safety performance is reduced after 500 cycles. The battery of the present invention maintains high safety performance both before and after 500 cycles. The porous insulating coating can insulate the positive electrode and the negative electrode when the positive electrode and the negative electrode are in direct contact due to the contraction of the diaphragm when the short-circuit temperature of the battery is increased due to internal or external factors, so that the short circuit is prevented, and the fire accident caused by the thermal runaway of the battery is prevented.
Variations and modifications to the above-described embodiments may also occur to those skilled in the art, which fall within the scope of the invention as disclosed and taught herein. Therefore, the present invention is not limited to the above-mentioned embodiments, and any obvious improvement, replacement or modification made by those skilled in the art based on the present invention is within the protection scope of the present invention. Furthermore, although specific terms are employed herein, they are used in a generic and descriptive sense only and not for purposes of limitation.
Claims (9)
1. A lithium ion secondary battery pole piece is characterized by comprising a current collector and an active material layer coated on at least one surface of the current collector, wherein a porous insulating coating is coated on the surface of the active material layer, the porous insulating coating comprises dopamine-coated inorganic particles and a first binder, an organic coating is further coated on the surface of the porous insulating coating, and the organic coating is distributed in an island shape and/or a linear shape; the coating area ratio of the organic coating to the porous insulating coating is 0.5-0.95: 1.
2. The lithium ion secondary battery pole piece of claim 1, wherein the inorganic particles comprise at least one of calcium oxide, zinc oxide, magnesium oxide, titanium dioxide, silicon dioxide, zirconium dioxide, tin dioxide, cerium dioxide, aluminum oxide, calcium carbonate, and barium titanate, and the first binder comprises at least one of styrene-butadiene polymer, polyvinylidene fluoride-hexafluoropropylene, polyacrylic acid, polymethacrylic acid, polyacrylate polymer, polymethyl acrylate, polyethyl acrylate, methyl methacrylate, polyacrylonitrile, sodium carboxymethylcellulose, butadiene-acrylonitrile polymer, polyvinylpyrrolidone, and polyacrylic acid-styrene polymer.
3. The pole piece of the lithium ion secondary battery according to claim 2, wherein the inorganic particles have a particle size of 0.001 to 20 μm, and the mass ratio of the inorganic particles to the first binder is 1:99 to 99.9: 1.
4. The pole piece of the lithium ion secondary battery of claim 1, wherein the thickness of the porous insulating coating is 0.5-50 μm, the pore diameter of the porous insulating coating is 0.001-10 um, and the porosity of the porous insulating coating is 5-95%.
5. The lithium ion secondary battery pole piece of claim 1, wherein the organic coating comprises organic particles comprising at least one of polyvinylidene fluoride, vinylidene fluoride-hexafluoropropylene polymer, polyvinylidene fluoride-co-hexafluoropropylene, polyvinylidene fluoride-co-trichloroethylene, polymethyl methacrylate, polyethylene oxide, polyacrylonitrile, polyvinylpyrrolidone, polyvinyl acetate, polyimide, acrylonitrile-butadiene copolymer, and acrylonitrile-styrene-butadiene copolymer, and a second binder comprising styrene-butadiene polymer, polyvinylidene fluoride-hexafluoropropylene, polyvinylpyrrolidone, polyacrylonitrile, sodium carboxymethylcellulose, polyacrylic acid, polyacrylonitrile, a polyvinyl alcohol, and a second binder, At least one of polymethyl acrylate, polyethyl acrylate, methyl methacrylate, sodium polyacrylate, polyacrylic acid-styrene polymer and ethyl acetate, wherein the particle size of the organic particles is 0.001-10 mm, and the mass ratio of the organic particles to the second binder is 1: 99-99.9: 0.1.
6. The lithium ion secondary battery pole piece of claim 5, wherein the organic coating further comprises a fast ion conductor comprising at least one of a NASICON type oxide fast ion conductor, a LiPON type fast ion conductor, and a garnet type fast ion conductor.
7. The pole piece of claim 1, wherein when the organic coating is in the form of islands, the area of each island of the organic coating is 0.025 μm2~500mm2The height of the organic coating is 0.05 um-100 um; when the organic coating is linear, the width of the organic coating is 0.05um ~10mm, the length of the organic coating is 0.5um ~50mm, the height of the organic coating is 0.5um ~100 um.
8. A lithium ion secondary battery, which is characterized by comprising a positive plate, a negative plate and electrolyte, wherein the positive plate or the negative plate is the lithium ion secondary battery plate of any one of claims 1 to 7.
9. The lithium ion secondary battery according to claim 8, further comprising a separator disposed between the positive electrode sheet and the negative electrode sheet, wherein the separator comprises a substrate layer and a functional coating layer compounded on at least one surface of the substrate layer, and the functional coating layer comprises a zeolite-like imidazole framework compound.
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| WO2022110225A1 (en) * | 2020-11-30 | 2022-06-02 | 宁德时代新能源科技股份有限公司 | Isolation membrane, secondary battery comprising same, and related battery module, battery pack and device |
| CN113629357A (en) * | 2021-07-23 | 2021-11-09 | 恒大新能源技术(深圳)有限公司 | Battery diaphragm, preparation method thereof and secondary battery |
| CN114421094A (en) * | 2022-01-11 | 2022-04-29 | 宁德新能源科技有限公司 | Electrochemical device, method for manufacturing the same, and electronic device |
| CN115377609A (en) * | 2022-08-11 | 2022-11-22 | 浙江大象新能源科技有限公司 | Polymer insulating coating and preparation method thereof |
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