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CN107240721B - Bipolar electrode, lithium ion battery and manufacturing method of lithium ion battery - Google Patents

Bipolar electrode, lithium ion battery and manufacturing method of lithium ion battery Download PDF

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Publication number
CN107240721B
CN107240721B CN201710389586.9A CN201710389586A CN107240721B CN 107240721 B CN107240721 B CN 107240721B CN 201710389586 A CN201710389586 A CN 201710389586A CN 107240721 B CN107240721 B CN 107240721B
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lithium ion
current collector
conductive
layer
ion battery
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CN107240721A (en
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刘昌位
胡金丰
高鹏然
吕坤
张华农
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Shenzhen Center Power Tech Co Ltd
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Shenzhen Center Power Tech 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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • 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
    • 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
    • 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
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • 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
    • H01M4/13—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
    • 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
    • H01M4/136—Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • H01M4/667—Composites in the form of layers, e.g. coatings
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/668—Composites of electroconductive material and synthetic resins
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/403—Manufacturing processes of separators, membranes or diaphragms
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • 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
    • H01M2004/029—Bipolar electrodes
    • 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
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    • 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
    • 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
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Abstract

The invention relates to the technical field of lithium ion batteries, and particularly discloses bipolar electrodes, a lithium ion battery and a manufacturing method of the lithium ion battery, wherein each bipolar electrode comprises a current collector, a conducting layer and a positive active layer which are sequentially overlapped from the th surface outwards, a second conducting layer and a negative active layer which are sequentially overlapped from the second surface outwards, and sealant which is used for firmly sealing the th conducting layer, the current collector and the second conducting layer, wherein the sealant is overlapped on the th conducting layer, the current collector and the second conducting layer, the thickness of the th conducting layer is the same as that of the positive active layer, and the thickness of the second conducting layer is the same as that of the negative active layer.

Description

Bipolar electrode, lithium ion battery and manufacturing method of lithium ion battery
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to bipolar electrodes, a lithium ion battery and a manufacturing method of the lithium ion battery.
Background
Environmental pollution and oil shortage are difficult problems faced by various countries all over the world, and electric automobiles can be used as a scheme for relieving or even solving the two problems, namely the electric automobiles can meet the rigidity requirement of daily travel of people and cannot cause direct pollution to the environment, and which is a key technology for developing electric automobiles is a power battery.
Because the lithium ion battery has series advantages of high energy density, high working voltage, long cycle life, no memory effect and the like, the lithium ion battery is a power battery for electric automobiles and attracts much attention, a plurality of power batteries are required to be connected in series to ensure output power for the electric automobiles, however, the series connection has very high requirement on the consistency of the battery, and the consistency of the battery connected in series is difficult to guarantee according to the current battery manufacturing technology, so the consistency and the safety are technical bottlenecks which limit the development of the electric automobiles.
The bipolar lithium ion battery can output higher working voltage by a single battery, besides, each polar plate and each parts of each polar plates of the battery with the structure have equal current density, and the current density is very small, so that the balance problems of different reaction degrees and aging degrees of active substances do not exist in the battery, and the consistency of the battery can be effectively improved.
However, the bipolar current collector of the present bipolar battery has a large defect, for example, the conventional bipolar current collector is a copper-aluminum composite foil or an aluminum-nickel composite foil, the thickness of the foil is less than 100 μm, and holes are easily generated, and denier of the used foil has micropores, so that an electrolyte can easily enter, and the battery is short-circuited, when the aluminum foil has holes, the copper foil or the nickel foil on the other surface is easily oxidized and corroded, and these problems can cause potential safety hazards of the high-voltage bipolar battery.
The invention patent with the application number of CN103219521A discloses bipolar current collectors and a manufacturing method thereof, and particularly polymer barrier layers are added between an aluminum foil and a non-aluminum conducting layer, and then polymers filled with conducting particles are coated.
The invention patent No. CN101076915A discloses a bipolar battery, but it has a problem of liquid-to-liquid short circuit caused by electrolyte solution bleeding, and in order to solve this problem, a polymer gel electrolyte is used in the electrolyte layer.
The invention patent with the application number of CN104577132A discloses bipolar current collectors and a manufacturing method thereof, and particularly relates to a bipolar current collector which comprises a conductive matrix film, a polymer barrier film layer and a conductive shunt layer, wherein the upper surface and the lower surface of the conductive matrix film are covered with the polymer barrier film layer and the conductive shunt layer, the polymer barrier film layer is positioned between the conductive matrix film and the conductive shunt layer and covers the upper surface and the lower surface of the conductive matrix film in a staggered and complementary manner.
Disclosure of Invention
The invention provides bipolar electrodes aiming at the problems of complex manufacturing process, uneven distribution of conductive particles, easy occurrence of holes and the like of the conventional bipolar electrode.
In order to achieve the above purpose, the technical solution of the embodiment of the present invention is as follows:
A bipolar electrode comprising a current collector having opposing and second surfaces;
the conductive layer and the positive active layer are sequentially overlapped from the surface to the outside;
the second conducting layer and the negative active layer are sequentially overlapped from the second surface to the outside;
the current collector is characterized by further comprising a sealant which is used for firmly sealing the th conducting layer, the current collector and the second conducting layer, wherein the sealant is stacked on the surfaces of the th conducting layer, the current collector and the second conducting layer, the thickness of the th conducting layer is the same as that of the positive active layer, and the thickness of the second conducting layer is the same as that of the negative active layer.
According to the bipolar electrode provided by the invention, conductive layers are uniformly coated on the surface of the bipolar current collector, so that barrier films can be formed on the surface of the current collector by using resin to block holes possibly formed in the current collector and prevent short circuit caused by electrolyte permeation, and conductive agents in the conductive layers can be uniformly distributed on the surface of the current collector, so that the uniformity of charge distribution on the surface of the bipolar current collector is improved, the contact resistance between positive and negative electrode materials and the current collector is greatly reduced, and the adhesion capability of the positive electrode material and the current collector, the negative electrode material and the current collector can be improved.
furthermore, the invention also provides lithium ion batteries.
lithium ion batteries comprise bipolar electrodes, diaphragms for isolating the positive and negative electrodes of the bipolar electrodes, electrolyte and battery cases, wherein the bipolar electrodes are the bipolar electrodes, and the diaphragms are polyvinylidene fluoride-hexafluoropropylene diaphragms, polyvinylidene fluoride-hexafluoropropylene/ceramic compound diaphragms and ceramic mixed glue diaphragms.
According to the lithium ion battery provided by the invention, conductive layers are uniformly coated on the surface of the bipolar current collector, so that not only can barrier films be formed on the surface of the current collector by using resin to prevent short circuit caused by electrolyte permeation, but also conductive agents in the conductive layers can be uniformly distributed on the surface of the current collector, so that the uniformity of charge distribution on the surface of the bipolar current collector is improved, the contact resistance between a positive/negative electrode material and the current collector is greatly reduced, the adhesion capability between the positive/negative electrode material and the current collector can be improved, the performance of the battery can be effectively improved when the battery is assembled, the diaphragm is a coated diaphragm containing polyvinylidene fluoride-hexafluoropropylene (P (VDF-HFP)), the P (VDF-HFP) is gelatinized by a heating and hot-cold pressing process, the free electrolyte is reduced, the possibility of liquid connection short circuit is reduced, and in addition, the sealant at the edge of the bipolar current collector is sealed by hot pressing, the short circuit at the edge.
, the invention also provides the manufacturing method of the lithium ion battery.
The method for manufacturing the lithium ion battery at least comprises the following steps:
respectively coating conductive slurry on the th surface and the second surface of a clean current collector, and drying to obtain a th conductive layer stacked on the th surface and a second conductive layer stacked on the second surface;
coating the positive electrode slurry on the surface of the th conductive layer, and drying to obtain a positive electrode active layer superposed on the surface of the th conductive layer;
coating the negative electrode slurry on the surface of the second conductive layer, and drying to obtain a negative electrode active layer stacked on the surface of the second conductive layer;
coating a sealant on the th conducting layer, the second conducting layer and the edge of the current collector, wherein the thickness of the sealant on the surface of the th conducting layer is the same as that of the positive active layer, and the thickness of the sealant on the surface of the second conducting layer is the same as that of the negative active layer;
stacking the bipolar electrode and the partition plate according to a positive electrode-diaphragm-negative electrode mode, injecting electrolyte into the partition plate during stacking, and then performing hot-pressing treatment on the sealant to obtain a pole group;
loading the pole group into a packaging film; standing the packaged battery for 24-48h at 45-60 ℃;
the laid battery is subjected to formation treatment according to a normal process; and performing hot-cold pressing treatment on the battery before or after formation, wherein the hot-cold pressing treatment is performed at a hot pressing temperature of 35-90 ℃ and a pressure of 0.1-10MPa, and the cold pressing treatment is performed at a cold pressing temperature of 5-20 ℃ and a pressure of 0.1-10 MPa.
According to the manufacturing method of the lithium ion battery, the diaphragm is a coating diaphragm containing polyvinylidene fluoride-hexafluoropropylene (P (VDF-HFP)), and the P (VDF-HFP) is gelatinized through a heating, heating and cold-pressing process, so that free electrolyte is reduced, and the possibility of liquid-to-liquid short circuit is reduced; and the sealant at the edge of the bipolar current collector is sealed by hot pressing, so that the short circuit of the edge part of the bipolar current collector is prevented, the safety of the battery is improved, and the whole manufacturing method is simple in process and suitable for large-scale production.
Drawings
The invention will be further described with reference to the drawings and examples, in which:
FIG. 1 is a front view of a bipolar electrode provided by an embodiment of the present invention;
FIG. 2 is a cross-sectional view A-A of a bipolar electrode provided in accordance with an embodiment of the present invention;
FIG. 3 is an enlarged view of a portion B of a bipolar electrode provided in accordance with an embodiment of the present invention;
FIG. 4 is a schematic diagram of a lithium ion battery assembled by bipolar electrodes according to an embodiment of the present invention;
the solar cell comprises a current collector 1, a conductive layer 2, a conductive agent 21, a binder 22, a second conductive layer 3, a positive electrode active layer 4, a negative electrode active layer 5, a sealant 6 and a diaphragm 7.
Detailed Description
For purposes of making the objects, aspects and advantages of the present invention more apparent, the present invention will be described in detail below with reference to the accompanying drawings and examples.
1-3, the present example provides bipolar electrodes, including a current collector 1, the current collector 1 having a th and a second opposing surfaces;
the conductive layer and the positive electrode active layer 4 are sequentially overlapped from the surface to the outside;
and a second conductive layer 3 and a negative active layer 5 which are sequentially overlapped from the second surface to the outside;
the current collector further comprises a sealant 6 for firmly sealing the th conducting layer 2, the current collector 1 and the second conducting layer 3.
Specifically, the sealant 6 is stacked on the th conductive layer 2, the current collector 1 and the second conductive layer 3, and the thickness on the th conductive layer 2 is the same as that of the positive electrode active layer 4, and the thickness on the second conductive layer 3 is the same as that of the negative electrode active layer 5.
Preferably, in order to avoid a possibility of short circuit due to the contact of the positive and negative electrode active layers 4 and 5 with each other, the current collector 1 has an area larger than that of the positive and negative electrode active layers 4 and 5, respectively.
Similarly, when the negative active layer 5 is coated, a partial area is also reserved around the edge of the second surface of the current collector 1, and the negative active layer 5 in the reserved partial area cannot cover the partial area, the reserved area is used for coating the sealant 6, so that the sealant 6 covers the edge of the th surface and the edge of the second surface, and the sealant 6 forms concave structures buckled with the edge of the current collector 1, as shown in fig. 2 specifically.
preferably, in order to avoid short circuit caused by contact between the positive electrode active layer 4 and the negative electrode active layer 5 and avoid lithium deposition during assembly of the bipolar electrode into a battery, the area of the positive electrode active layer 4 is smaller than that of the negative electrode active layer 5. fig. 2 shows that the length of the cross section of the positive electrode active layer 4 is smaller than that of the cross section of the negative electrode active layer 5.
Preferably, the current collector 1 is any kinds of aluminum foil, copper foil, nickel foil, stainless steel foil, aluminum-nickel composite foil, and aluminum-copper composite foil.
Preferably, the thickness of the current collector 1 is 1 μm to 40 μm.
Preferably, the th conductive layer 2 has a thickness of 0.1 to 10.0 μm.
Preferably, the thickness of the second conductive layer 3 is 0.1 μm to 10.0 μm.
Preferably, the th conductive layer 2 and the second conductive layer 3 are coated by conductive paste, and the conductive paste of the th conductive layer 2 is the same as the conductive paste of the second conductive layer 3.
Preferably, the conductive paste consists of the following components by mass 100%:
0.1 to 15 percent of conductive agent;
1-10% of a binder;
the balance of solvent.
The conductive paste is coated on the surfaces of th conductive layer 2 and second conductive layer 3, and then dried to obtain the surface microstructure shown in fig. 3, wherein 21 is a conductive agent and 22 is an adhesive.
Preferably, the conductive agent 21 can be at least of graphite, carbon black, carbon nano tubes, carbon fibers and graphene, the binder 22 is at least of polyvinyl alcohol, polyvinyl acid, polyvinylidene fluoride, epoxy resin, phenolic resin and polyurethane, the solvent is deionized water or N-methyl pyrrolidone, the solvent plays a role in dissolving the conductive agent and the binder, and the solvent volatilizes in the process of drying the smear.
Preferably, the positive electrode material in the positive electrode active layer 4 is at least kinds of lithium cobaltate, lithium manganate, ternary lithium nickel cobalt manganese oxide material, ternary nickel cobalt aluminum material, lithium-rich manganese and lithium iron phosphate.
Preferably, the cell negative electrode material in the negative electrode active layer 5 is or more of artificial graphite, natural graphite, mesocarbon microbeads, hard carbon, silicon oxygen and metal alloy negative electrodes.
According to the bipolar electrode provided by the invention, the conductive layers are uniformly coated on the surface of the bipolar current collector, so that barrier films can be formed on the surface of the current collector by using resin to prevent short circuit caused by electrolyte permeation, and conductive agents in the conductive layers can be uniformly distributed on the surface of the current collector, so that the uniformity of the surface charge distribution of the bipolar current collector is improved, the contact resistance between a positive electrode material and a negative electrode material and the current collector is greatly reduced, the adhesion capacity between the positive electrode material and the current collector and between the negative electrode material and the current collector can be improved, and when the bipolar electrode provided by the invention is assembled into a lithium ion battery, the battery performance can be effectively improved.
On the premise of providing the bipolar electrode, steps are further provided, and lithium ion batteries are further provided.
In embodiment, kinds of lithium ion batteries comprise bipolar electrodes, diaphragms for isolating the positive and negative electrodes of the bipolar electrodes, electrolyte and battery cases, wherein the bipolar electrodes are the bipolar electrodes, and the diaphragms are kinds of polyvinylidene fluoride-hexafluoropropylene diaphragms, polyvinylidene fluoride-hexafluoropropylene/ceramic composite diaphragms and ceramic mixed glue diaphragms.
According to the lithium ion battery provided by the invention, conductive layers are uniformly coated on the surface of the bipolar current collector, so that not only can barrier films be formed on the surface of the current collector by using resin to prevent short circuit caused by electrolyte permeation, but also conductive agents in the conductive layers can be uniformly distributed on the surface of the current collector, so that the uniformity of the surface charge distribution of the bipolar current collector is improved, the contact resistance between a positive/negative electrode material and the current collector is greatly reduced, the adhesion capacity between the positive/negative electrode material and the current collector can be improved, and the performance of the battery can be effectively improved when the lithium ion battery is assembled.
, the invention also provides a method for preparing of the lithium ion battery.
In an embodiment, the method for manufacturing the lithium ion battery includes the following steps:
(1) coating conductive slurry on the th surface and the second surface of a clean current collector respectively, and drying to obtain a th conductive layer stacked on the th surface and a second conductive layer stacked on the second surface;
coating the positive electrode slurry on the surface of the th conductive layer, and drying to obtain a positive electrode active layer superposed on the surface of the th conductive layer;
coating the negative electrode slurry on the surface of the second conductive layer, and drying to obtain a negative electrode active layer stacked on the surface of the second conductive layer;
coating a sealant on the th conducting layer, the second conducting layer and the edge of the current collector, wherein the thickness of the sealant on the th conducting layer surface is the same as that of the positive electrode active layer, and the thickness of the sealant on the second conducting layer surface is the same as that of the negative electrode active layer, and obtaining the bipolar electrode through roll pressing treatment.
(2) Assembling the bipolar electrode into a lithium ion battery: stacking the bipolar electrode and the separator in a positive-diaphragm-negative mode, injecting electrolyte of a conventional lithium ion battery into the separator during stacking, and performing hot-pressing treatment on the sealant to obtain a pole group, wherein the pole group is shown in fig. 4; loading the pole group into a packaging film; and standing the packaged battery for 24-48h at the temperature of 45-60 ℃.
(3) Formation and other subsequent treatment of the lithium ion battery: carrying out formation treatment on the shelved battery according to a normal process; and performing hot-cold pressing treatment on the battery before or after formation, wherein the hot-cold pressing treatment is performed at a hot pressing temperature of 35-90 ℃ and a pressure of 0.1-10MPa, and the cold pressing treatment is performed at a cold pressing temperature of 5-20 ℃ and a pressure of 0.1-10 MPa.
Specifically, when the lithium ion battery is assembled, any of polyvinylidene fluoride-hexafluoropropylene diaphragms, polyvinylidene fluoride-hexafluoropropylene/ceramic composite diaphragms and ceramic mixed glue diaphragms are adopted, the diaphragms can reduce short circuit caused by permeation of electrolyte through holes of a current collector, swell after hot pressing treatment, and cross-link with binders in active layers of a positive electrode and a negative electrode, and P (VDF-HFP) is gelatinized through cold pressing, so that the effect of reducing free electrolyte is achieved.
Preferably, the time of the hot pressing treatment is 1-10 min; the time of the cold pressing treatment is 1-10 min.
According to the manufacturing method of the lithium ion battery provided by the embodiment of the invention, conductive layers are uniformly coated on the surface of the bipolar current collector, so that not only can barrier films be formed on the surface of the current collector by using resin to prevent short circuit caused by electrolyte permeation, but also conductive agents in the conductive layers can be uniformly distributed on the surface of the current collector, the uniformity of the surface charge distribution of the bipolar current collector is improved, meanwhile, the contact resistance between a positive/negative electrode material and the current collector is greatly reduced, the adhesion capability between the positive/negative electrode material and the current collector can be improved, the performance of the battery can be effectively improved when the lithium ion battery is assembled, the diaphragm is a coated diaphragm containing polyvinylidene fluoride-hexafluoropropylene (P (VDF-HFP)), the P (VDF-HFP) is gelatinized by a heating, heating and cold pressing process, the bipolar free electrolyte is reduced, the possibility of liquid connection short circuit is reduced, the sealant at the edge of the current collector is subjected to hot pressing and sealing, the edge part of the current collector is prevented from being short circuit, the safety.
In order to better illustrate the technical scheme of the bipolar electrode of the present invention and the technical scheme of the lithium ion battery manufactured by the bipolar electrode, the principle, the action and the achieved efficacy of the lithium ion battery are illustrated by a plurality of embodiments below.
Example 1
kinds of lithium ion batteries are made up as follows
(1) Production of electroconductive paste
The conductive paste is calculated by the mass of 100%
2% of carbon black (SP);
4% of epoxy resin;
94% of NMP solvent;
the components of the formula are mixed and stirred into conductive slurry.
(2) Manufacturing a bipolar electrode:
as shown in fig. 2, a 20 μm copper-aluminum composite foil is used as a current collector 1 of a bipolar electrode, the conductive paste obtained in step (1) is uniformly coated on the front and back surfaces of the current collector according to the surface density of , and the current collector is dried to obtain a th conductive layer 2 and a second conductive layer 3
LiCoO is a positive electrode active material2Mixing the conductive agent SP and the binder PVDF in NMP, stirring to obtain uniformly dispersed anode slurry, coating the anode slurry on the surface coated with the th conducting layer 2, reserving a blank on the surface of the th conducting layer 2 close to the edge, and drying to obtain an anode active layer 4;
then mixing and stirring the negative active material artificial graphite, the conductive agent SP, the binder SBR and the thickening agent CMC in water to obtain uniformly dispersed negative slurry, coating the negative slurry on the surface coated with the second conductive layer 3, reserving a blank on the surface of the second conductive layer 3 close to the edge, and drying to obtain a negative active layer 5;
coating sealant 6 on the edge of the bipolar current collector and the reserved blank edges of the th conducting layer 2 and the second conducting layer 3, and drying to obtain the bipolar electrode;
(3) assembling the lithium ion battery:
as shown in figure 4, a P (VDF-HFP) diaphragm 7 with the area larger than that of a positive active layer 4 and that of a negative active layer 5 are placed between the adjacent positive and negative electrodes, electrolyte is added to be overlapped into 4 layers, wherein the end is an electrode only with a positive electrode, the other end is an electrode only with a negative electrode, the battery core is sealed by a sealant 6 at the hot-pressing edge, then the battery core is arranged in an outer packaging film, the battery core is placed still for 36h at the 45 ℃ environment, a hot-cold press is used for hot-pressing for 2min at the 80 ℃ under the pressure of 0.2MPa, then the cold-pressing is carried out for 2min at the 18 ℃ under the pressure of 0.2MPa, a condensed battery is obtained, formation is carried out, and the bipolar lithium ion battery with the nominal voltage of 14.8V and the nominal capacity of.
Example 2
kinds of lithium ion batteries are made up as follows
(1) Production of electroconductive paste
The conductive paste is calculated by the mass of 100%
2% of carbon black (SP);
4% of epoxy resin;
NMP solvent 94%
The components of the formula are mixed and stirred into conductive slurry.
(2) Manufacturing a bipolar electrode:
as shown in fig. 2, a 20 μm copper-aluminum composite foil is used as a current collector 1 of a bipolar electrode, the conductive paste obtained in step (1) is uniformly coated on the front and back surfaces of the current collector according to the surface density of , and the current collector is dried to obtain a th conductive layer 2 and a second conductive layer 3
LiCoO is a positive electrode active material2Mixing the conductive agent SP and the binder PVDF in NMP, stirring to obtain uniformly dispersed anode slurry, coating the anode slurry on the surface of the th conducting layer 2, reserving a blank on the surface of the th conducting layer 2 close to the edge, and drying to obtain an anode active layer 4;
then mixing and stirring the negative active material artificial graphite, the conductive agent SP, the binder SBR and the thickening agent CMC in water to obtain uniformly dispersed negative slurry, coating the negative slurry on the surface coated with the second conductive layer 3, reserving a blank on the surface of the second conductive layer 3 close to the edge, and drying to obtain a negative active layer 5;
coating sealant 6 on the edge of the bipolar current collector and the reserved blank edges of the th conducting layer 2 and the second conducting layer 3, and drying to obtain the bipolar electrode;
(3) assembling the lithium ion battery:
as shown in figure 4, a P (VDF-HFP) diaphragm 7 with the area larger than that of a positive electrode active layer 4 and that of a negative electrode active layer 5 are placed between the adjacent positive and negative electrodes, electrolyte is added to be overlapped into 4 layers, wherein the end is an electrode with only a positive electrode, the end is an electrode with only a negative electrode, the battery core is sealed through a sealant 6 at the hot pressing edge, then the battery core is arranged in an outer packaging film, the battery core is placed and stands for 36 hours in an environment with the temperature of 45 ℃, then the battery core is formed, the formation is finished, a hot and cold press is used for hot pressing at the temperature of 80 ℃ for 2 minutes under the pressure of 0.2MPa, then cold pressing at the temperature of 18 ℃ for 2 minutes under the pressure of 0.2MPa to obtain a condensed battery, and the lithium ion battery with the nominal bipolar voltage of 14.8V and the nominal capacity.
Example 3
kinds of lithium ion batteries are made up as follows
(1) Production of electroconductive paste
The conductive paste is calculated by the mass of 100%
2% of carbon black (SP);
4% of polyvinylidene fluoride;
94% of NMP solvent;
the components of the formula are mixed and stirred into conductive slurry.
(2) Manufacturing a bipolar electrode:
as shown in fig. 2, a 16 μm aluminum foil is used as a current collector 1 of a bipolar electrode, the conductive paste of step (1) is uniformly coated on the front and back surfaces of the current collector according to the surface density of , and the current collector is dried to obtain a th conductive layer 2 and a second conductive layer 3
LiNi is a positive electrode active material0.5Co0.2Mn0.3O2Mixing the conductive agent CNTs and the binder PVDF in NMP, stirring to obtain uniformly dispersed anode slurry, coating the anode slurry on the surface coated with the th conductive layer 2, reserving a blank on the surface of the th conductive layer 2 close to the edge, and drying to obtain an anode active layer 4;
then the negative active material Li4Ti5O12Mixing the conductive agent SP, the binder SBR and the thickening agent CMC in water, stirring to obtain uniformly dispersed negative electrode slurry, coating the negative electrode slurry on the surface coated with the second conductive layer 3, reserving a blank on the surface of the second conductive layer 3 close to the edge, and drying to obtain a negative electrode active layer 5;
coating sealant 6 on the edge of the bipolar current collector and the reserved blank edges of the th conducting layer 2 and the second conducting layer 3, and drying to obtain the bipolar electrode;
(3) assembling the lithium ion battery:
as shown in figure 4, a P (VDF-HFP) diaphragm 7 with the area larger than that of a positive active layer 4 and that of a negative active layer 5 are placed between the adjacent positive and negative electrodes, electrolyte is added to be overlapped into 4 layers, 4 layers of positive electrodes and 4 layers of negative electrodes are provided in total, wherein the end is an electrode with only a positive electrode, and the end is an electrode with only a negative electrode, the battery core is sealed through a sealant 6 at the hot pressing edge, then the battery core is put into an outer packaging film, the battery core is placed at 45 ℃ and stands still for 36h, a hot-cold press is used for carrying out hot pressing at 80 ℃ for 2min under the pressure of 0.2MPa, then cold pressing is carried out at 18 ℃ for 2min under the pressure of 0.2MPa, a condensed battery is obtained, formation is carried out, and the lithium ion battery with the bipolar nominal voltage of 9.6V and.
Example 4
kinds of lithium ion batteries are made up as follows
(1) Production of electroconductive paste
The conductive paste is calculated by the mass of 100%
CNTs 1％；
3% of polyvinylidene fluoride;
96% of NMP solvent;
the components of the formula are mixed and stirred into conductive slurry.
(2) Manufacturing a bipolar electrode:
as shown in fig. 2, a 16 μm aluminum foil is used as a current collector 1 of a bipolar electrode, the conductive paste of step (1) is uniformly coated on the front and back surfaces of the current collector according to the surface density of , and the current collector is dried to obtain a th conductive layer 2 and a second conductive layer 3
LiNi is a positive electrode active material0.5Co0.2Mn0.3O2Mixing the conductive agent CNTs and the binder PVDF in NMP, stirring to obtain uniformly dispersed anode slurry, coating the anode slurry on the surface coated with the th conductive layer 2, reserving a blank on the surface of the th conductive layer 2 close to the edge, and drying to obtain an anode active layer 4;
then the negative active material Li4Ti5O12Mixing the conductive agent SP, the binder SBR and the thickening agent CMC in water, stirring to obtain uniformly dispersed negative electrode slurry, coating the negative electrode slurry on the surface coated with the second conductive layer 3, reserving a blank on the surface of the second conductive layer 3 close to the edge, and drying to obtain a negative electrode active layer 5;
coating sealant 6 on the edge of the bipolar current collector and the reserved blank edges of the th conducting layer 2 and the second conducting layer 3, and drying to obtain the bipolar electrode;
(3) assembling the lithium ion battery:
as shown in figure 4, a P (VDF-HFP) diaphragm 7 with the area larger than that of a positive active layer 4 and that of a negative active layer 5 are placed between the adjacent positive and negative electrodes, electrolyte is added to be overlapped into 4 layers, 4 layers of positive electrodes and 4 layers of negative electrodes are provided in total, wherein the end is an electrode with only a positive electrode, and the end is an electrode with only a negative electrode, the battery cell is sealed through a sealant 6 at the hot pressing edge, then the battery cell is arranged in an outer packaging film, the battery cell is placed at 45 ℃ for standing for 36h to be formed, after the formation, a hot-cold press is used for hot pressing at 80 ℃ for 10min, the pressure is 0.3MPa, then the cold pressing is carried out at 18 ℃ for 10min, the pressure is 0.3MPa, a condensed battery is obtained, and the lithium ion battery with the nominal voltage of 9.6V and the nominal capacity of.
Comparative example 1:
the foil used for the control group of bipolar electrodes was a conventional foil without a coating, the diaphragm was a conventional PE-based film, and other preparation conditions were maintained at compared with example 1, the nominal voltage was 14.8V, and the nominal capacity was 90 mAh.
Comparative example 2:
the foil used for the control group of bipolar electrodes was a conventional foil without a coating, the separator was a conventional PE-based film, and other preparation conditions were maintained at deg.f as in example 4, the nominal voltage of the battery was 9.6V, and the nominal capacity was 65 mAh.
The internal resistance, the leakage and the self-discharge of the lithium ion batteries prepared in the above examples 1 to 4 and comparative examples 1 to 2 were counted, as shown in table 1.
The self-discharge test method comprises the steps of firstly charging the battery to a half-electric state, measuring to obtain voltage values V1, then standing at normal temperature for 72 hours, measuring to obtain voltage values V2, and measuring to obtain self-discharge K ═ V1-V2)/72.
TABLE 1 data of cell performance test for examples 1-4 and comparative examples 1-2
Examples of the invention Internal resistance of Whether or not to leak liquid Self-discharge K value
Example 1 3.1mΩ Whether or not 0.082mV/h
Example 2 2.8mΩ Whether or not 0.073mV/h
Example 3 2.9mΩ Whether or not 0.057mV/h
Example 4 3.0mΩ Whether or not 0.065mV/h
Comparative example 1 4.8mΩ Is not obvious 0.180mV/h
Comparative example 2 5.2mΩ Is not obvious 0.242mV/h
As can be seen from table 1, when a foil with a conductive coating and a coating separator containing polyvinylidene fluoride-hexafluoropropylene (P (VDF-HFP)) are used, P (VDF-HFP) is gelled by a hot-cold-pressing process, so that internal resistance can be effectively reduced, the risk of leakage can be reduced, and the self-discharge of the prepared battery is small.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.

Claims (8)

1, kinds of lithium ion battery's preparation method, characterized by, include the following step at least:
respectively coating conductive slurry on the th surface and the second surface of a clean current collector, and drying to obtain a th conductive layer stacked on the th surface and a second conductive layer stacked on the second surface;
coating the positive electrode slurry on the surface of the th conductive layer, and drying to obtain a positive electrode active layer superposed on the surface of the th conductive layer;
coating the negative electrode slurry on the surface of the second conductive layer, and drying to obtain a negative electrode active layer stacked on the surface of the second conductive layer;
coating a sealant on the th conducting layer, the second conducting layer and the edge of the current collector, wherein the thickness of the sealant on the surface of the th conducting layer is the same as that of the positive active layer, and the thickness of the sealant on the surface of the second conducting layer is the same as that of the negative active layer;
stacking the bipolar electrode and the diaphragm in a positive-diaphragm-negative mode, injecting electrolyte into the diaphragm during stacking, and then performing hot-pressing treatment on the sealant to obtain a pole group;
loading the pole group into a packaging film; standing the packaged battery for 24-48h at 45-60 ℃;
the laid battery is subjected to formation treatment according to a normal process; performing hot-cold pressing treatment on the battery before or after formation, wherein the hot-cold pressing treatment is performed at a hot pressing temperature of 35-90 ℃ and a pressure of 0.1-10MPa, and the cold pressing temperature of 5-20 ℃ and a pressure of 0.1-10MPa;
the diaphragm is any kinds of polyvinylidene fluoride-hexafluoropropylene diaphragm, polyvinylidene fluoride-hexafluoropropylene/ceramic compound diaphragm and ceramic mixed glue diaphragm.
2. The method of manufacturing a lithium ion battery according to claim 1, wherein: the time of the hot pressing treatment is 1-10 min; the time of the cold pressing treatment is 1-10 min.
3. The method of manufacturing a lithium ion battery according to claim 1, wherein: the conductive paste comprises the following components by mass percent of 100 percent:
0.1 to 15 percent of conductive agent;
1 to 10 percent of binder
The balance of solvent;
the binder is at least of polyvinyl alcohol, polyvinyl acid, polyvinylidene fluoride, epoxy resin, phenolic resin and polyurethane;
the current collector is any kinds of aluminum foil, copper foil, nickel foil, stainless steel foil, aluminum-nickel composite foil and aluminum-copper composite foil.
4. The method of claim 3, wherein the conductive agent is at least types selected from graphite, carbon black, carbon nanotubes, carbon fibers and graphene, and the solvent is deionized water or N-methylpyrrolidone.
5. The method according to claim 1, wherein the th conductive layer has a thickness of 0.1 to 10.0 μm and/or the second conductive layer has a thickness of 0.1 to 10.0 μm.
6. The method for manufacturing the lithium ion battery according to claim 1, wherein the sealant is any of polypropylene, maleic anhydride grafted polypropylene and modified polyethylene.
7. The method of manufacturing a lithium ion battery according to claim 1, wherein: the thickness of the current collector is 1-40 μm.
8, lithium ion batteries manufactured by the manufacturing method of any of claims 1-7.
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