CN112151875A - Current collector-free battery core, preparation method thereof and lithium ion battery - Google Patents

Current collector-free battery core, preparation method thereof and lithium ion battery Download PDF

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CN112151875A
CN112151875A CN202011125847.4A CN202011125847A CN112151875A CN 112151875 A CN112151875 A CN 112151875A CN 202011125847 A CN202011125847 A CN 202011125847A CN 112151875 A CN112151875 A CN 112151875A
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material layer
area
polar
positive electrode
isolation
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CN112151875B (en
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徐洲
李涛
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Shenzhen Poly Lithium Energy Co ltd
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Shenzhen Poly Lithium Energy 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • 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
    • 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
    • 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

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  • Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Materials Engineering (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)

Abstract

The invention discloses a current collector-free battery core, a preparation method thereof and a lithium ion battery. The method comprises the following steps: 1) preparing a first material area and a first polar material layer of a first blank area positioned on one side of the first material area; 2) forming a first isolation material layer on the first polar material layer and the first blank region; 3) preparing a second polar material layer with a structure opposite to that of the first polar material layer on the first isolation material layer, wherein the second polar material layer comprises a second material area and a second blank area which is positioned on one side of the second material area and is opposite to the first blank area; the first material area and the second material area are partially overlapped in the horizontal projection direction; 4) forming a second isolation material layer in the second blank area, wherein the first isolation material layer and the second isolation material layer form an isolation structure, and the first polarity material layer and the second polarity material layer are isolated to obtain a cell unit; 5) and cutting along the edge of the battery cell unit to obtain the battery cell without the current collector.

Description

Current collector-free battery core, preparation method thereof and lithium ion battery
Technical Field
The invention belongs to the technical field of energy storage, and relates to a current collector-free battery core, a preparation method thereof and a lithium ion battery.
Background
In recent years, with the development of economy and the advancement of technology, energy problems and environmental problems have become important concerns of all people at present. The excessive consumption of fossil fuels and the growing demand for energy have made the development and utilization of clean energy extremely urgent.
The lithium ion secondary battery is used as a preferred power supply in the fields of digital products, electric automobile products and the like at present because of the advantages of high energy density, high working voltage, long cycle life, no pollution and the like. With the increasing popularity of portable intelligent devices, development of light and thin battery cells with portability, small size, high energy density and high safety has recently become a common research hotspot in academic and industrial circles. How to make portable intelligent equipment really meet the daily life needs of people, how to make intelligent equipment have not only less volume but also long-time endurance, it becomes one of the technical difficulties that the development of battery electric core corresponding to it is urgent to overcome.
CN109888168A discloses a positive electrode, a preparation method thereof and a battery with the positive electrode, wherein the positive electrode is a carbon fiber network structure loaded by a positive electrode material and nano titanium dioxide, and the preparation method of the positive electrode is as follows: soaking the paper in titanate solution, taking out and drying to obtain a composite paper, ultrasonically dispersing a positive electrode material and deionized water according to a certain proportion to obtain a dispersion liquid with a certain solubility, then mixing the composite paper with the dispersion liquid to perform hydrolysis reaction, taking out and drying to obtain a titanium dioxide and positive electrode material loaded complex; and then carrying out high-temperature heating treatment on the complex in the protective gas atmosphere to obtain a structure of loading nano titanium dioxide and a positive electrode material on a carbon fiber network, namely a positive electrode and a battery with the positive electrode. The technical scheme is used for preparing the self-supporting flexible anode without a bonding agent and a current collector, and can simplify the electrode preparation process, reduce the working procedures, reduce the cost, improve the energy density, and improve the conductivity and the safety. However, the invention requires that the electrode is prepared first and then assembled into the battery, the process is relatively complicated, and the electrode structure is not compact enough.
CN108807958A discloses a tin dioxide-graphene-carbon nanotube flexible negative electrode material, a preparation method and an application thereof, wherein the preparation method comprises: dissolving tin salt in pure water, heating to 90-230 ℃, preserving heat for 3-72 hours, cooling to room temperature, adding saccharides, stirring for dissolving, heating to 90-230 ℃, preserving heat for 1-72 hours, adding graphene oxide dispersion liquid, stirring and mixing uniformly, adding short single-walled carbon nanotubes, styrene-butadiene rubber and hydroiodic acid solution, stirring uniformly, performing ultrasonic treatment, performing reduced pressure filtration on the mixed solution to obtain a composite membrane, and drying to obtain the composite membrane. The preparation method of the flexible negative electrode material is simple, environment-friendly and low in cost, and the problem of volume expansion of tin dioxide is relieved by the structure of the three-dimensional carbon skeleton; the addition of SBR improves the mechanical property of the membrane so that the membrane can be directly used as a flexible electrode material under the condition of no current collector and no binder; the prepared composite membrane material has excellent cycle performance, high energy density, high rate performance and long service life. However, the preparation process of the flexible negative electrode is complex, and the tightness of the assembled battery is not good enough.
Aiming at the development trend of the lithium ion battery cell, at present, no mature technology and process are available in the industry to prepare products meeting the requirements, most devices only stay in the research stage, and the problems that the performance cannot meet the requirements, the energy density is low, the preparation cost is high, the preparation process is complex and the like need to be solved are really applied.
In summary, it is an urgent need to develop a method for ensuring the energy density of the battery cell, ensuring the safety performance of the battery cell during the production and use processes, and having a simple preparation process.
Disclosure of Invention
In view of the above problems, an object of the present invention is to provide a current collector-free battery cell, a method for manufacturing the same, and a lithium ion battery.
In order to achieve the purpose, the invention adopts the following technical scheme:
in a first aspect, the present invention provides a method for preparing a current collector-free battery cell, the method comprising the steps of:
(1) preparing a first polar material layer, wherein the first polar material layer comprises a first material area and a first blank area positioned on one side of the first material area;
(2) forming a first isolation material layer on the first polar material layer and the first blank region using an isolation material;
(3) preparing a second polarity material layer on the first isolation material layer, wherein the polarity of the second polarity material layer is opposite to that of the first polarity material layer, and the second polarity material layer comprises a second material area and a second blank area which is positioned on one side of the second material area and is opposite to the first blank area;
the first material area and the second material area are partially overlapped in the horizontal projection direction;
(4) forming a second isolation material layer in the second blank area by using an isolation substance, wherein the first isolation material layer and the second isolation material layer form an isolation structure, and the isolation structure separates the first polarity material layer from the second polarity material layer to obtain a battery cell unit of a lamination structure;
(5) and cutting along the edge of the battery cell unit to obtain the battery cell without the current collector.
In the method of the present invention, the isolation material layer formed in step (2) may be prepared at one time (e.g., one filling molding) or may be prepared multiple times (e.g., two filling molding).
The method of the invention adopts a lamination type process, a plurality of cell units can be obtained at one time, the working efficiency is improved, the shape and the size of the cell are controllable, and the prepared lithium ion battery has good safety, compact structure and energy density.
The manufacturing process is simple to operate, and meanwhile, the safety performance of the battery cell in the production and use processes can be guaranteed. The following is a preferred technical solution of the present invention, but not a limitation to the technical solution provided by the present invention, and the technical objects and advantageous effects of the present invention can be better achieved and achieved by the following preferred technical solution.
Preferably, the raw materials used for preparing the first polar material layer in the step (1) and the second polar material layer in the step (3) are electrode mixtures, and the electrode mixtures are positive electrode mixtures or negative electrode mixtures.
Preferably, the method of preparing the first polar material in step (1) and the second polar material in step (3) is independently selected from at least one of coating, preferably pressure coating, and filling, preferably deposition.
Pressure coating refers to a coating method that fixes raw materials to a surface to be coated under a certain pressure, including but not limited to at least one of 3D printing and spraying.
In the present invention, the forms of the first mixture and the second mixture are not limited, as long as the first polar material layer and the second polar material layer can be formed tightly by combining with a certain process, and the first polar material layer and the second polar material layer may be, for example, dry powder, dry particle, wet particle, slurry, or the like.
The invention does not limit the variety of the raw materials in the anode mixture and the cathode mixture, and the raw materials commonly used in the field for preparing the anode mixture and the cathode mixture can be used in the invention.
Preferably, the positive electrode mix includes a positive electrode active material, a binder, and a conductive agent.
Preferably, the anode mix includes an anode active material, a binder, and optionally a conductive agent. The "optional conductive agent" means: the negative electrode material layer may or may not contain a conductive agent, for example, when other components in the negative electrode material layer satisfy that the negative electrode material layer has good conductivity, no additional conductive agent is needed.
Preferably, the positive active material includes at least one of lithium cobaltate, lithium manganate, lithium iron phosphate, lithium manganese phosphate, a nickel-cobalt-manganese ternary material, and a nickel-cobalt-aluminum ternary material.
Preferably, the negative active material includes at least one of lithium titanate, natural graphite, artificial graphite, carbon fiber, soft carbon, hard carbon, mesocarbon microbeads, elemental silicon, a silicon oxy compound, and a silicon-carbon composite.
Preferably, the binder in the positive electrode mix and the negative electrode mix is independently selected from at least one of polyvinylidene fluoride, polytetrafluoroethylene, polyacrylic acid, and polyvinyl alcohol. Such as polyvinylidene fluoride, polytetrafluoroethylene, a combination of polyvinylidene fluoride and polyacrylic acid, a combination of polyvinylidene fluoride, polytetrafluoroethylene and polyvinyl alcohol, and the like. However, the above-mentioned binder is not limited thereto, and other binders commonly used in the art to achieve the same effect may be used in the present invention.
Preferably, the conductive agent in the positive electrode mixture and the negative electrode mixture is independently selected from at least one of conductive carbon black, acetylene black, ketjen black, Super P, Super S, carbon nanotube, graphene, porous carbon and carbon fiber. For example, conductive carbon black, ketjen black, a combination of acetylene black and Super P, a combination of Super P, carbon nanotube and porous carbon, etc., but not limited to the above-listed conductive agents, other conductive agents commonly used in the art to achieve the same effect may be used in the present invention.
The positive electrode mixture and/or the negative electrode mixture of the invention may further comprise other additives suitable for preparing the positive electrode material layer and/or the negative electrode material layer, such as a surfactant or a pore-forming agent.
In the invention, the first polar material layer and the second polar material layer have opposite polarities and correspond to the positive electrode material layer and the negative electrode material layer. The first polar material layer can be an anode material layer, and the second polar material layer can be a cathode material layer; alternatively, the first polar material layer may be a negative electrode material layer, and the second polar material layer may be a positive electrode material layer.
Preferably, the first polar material layer is formed on the substrate table.
It should be noted that the above-defined preparation sequence of the first polarity material layer and the second polarity material layer is only for a single cell unit (which may be a single cell, or a multi-cell of a stack of multiple cells); for mass production of the cell units, a plurality of first polarity material layers may be simultaneously prepared on the substrate, and at this time, all of the first polarity material layers may be positive electrode material layers, all of the first polarity material layers may be negative electrode material layers, or both of the positive electrode material layers and the negative electrode material layers may be provided.
Preferably, the number of first polar material layers is at least 2, such as 2, 4, 5, 7, 8, 10, 12 or 20, etc.
Preferably, the number of the second polarity material layers is at least 2, such as 2, 4, 5, 7, 8, 10, 12 or 20, etc.
Preferably, the number of the second polar material layers is the same as that of the first polar material layers.
Preferably, the second material section is identical in shape and size to the first material section.
Preferably, the partial coincidence of the first material area and the second material area in the horizontal projection direction is realized by the following mode: the second material area is staggered along a single direction relative to the first material area.
Preferably, in the step (2), a material containing a spacer substance is filled and/or coated on the first polar material layer and the first empty area to form a first spacer material layer. When the second isolation material layer is actually prepared, the thickness of the second isolation material layer corresponding to the first blank area is higher than that of the second isolation material layer corresponding to the first polar material layer, so that a plane is obtained after filling and/or coating, and the plane is used for preparation of subsequent processes.
Preferably, in the step (4), in the second blank area, a material containing a separation substance is filled and/or coated to form a second separation material layer. In the actual preparation of the second isolating material layer, the height of the second isolating material layer should be substantially the same as the thickness of the second polarity material layer, so that a flat surface is obtained after filling and/or coating for the preparation of subsequent processes.
Preferably, in the step (2) and the step (4), the coating mode is a casting method.
In the present invention, the types of the spacer in the step (2) and the step (4) may be the same or different.
Preferably, the kinds of the separator in step (2) and step (4) independently include at least one of a solid electrolyte, a ceramic dielectric material, and a polyolefin.
Preferably, at least a portion of the separation structure located between the first polar material layer and the second polar material layer has a lithium ion conductivity, so as to ensure the transmission of lithium ions between the positive electrode and the negative electrode.
In order to obtain better effects of isolating the positive electrode and the negative electrode and transmitting lithium ions, the following preferred scheme can be adopted:
solid electrolytes such as oxide solid electrolytes, sulfide solid electrolytes or polymer solid electrolytes, more specifically, LLZO, LLZTO and the like, are directly used as a separator material for producing a separator structure, and the actual production may be performed by pressure coating using a dry powder, a granular dry material, a granular wet material of a solid electrolyte, such as spray coating or 3D printing.
② the isolation structure is prepared by adopting a porous polyolefin layer, such as a porous PP layer or a porous PE layer, and the actual preparation can adopt a fitting mode.
Thirdly, ceramic dielectric material is used as isolation material for preparing the isolation structure, and the ceramic dielectric material, adhesive and solvent are mixed and then pressure coating, such as spraying or 3D printing, is adopted for practical preparation.
(iv) mixing the polyolefin in molten or powdered form with a pore-forming agent, including but not limited to volatile solvents or metal oxide particles (e.g., Al)2O3、TiO2、SiO2MgO, CaO, etc.), wherein the metal particles increase stacking holes to provide transport channels for lithium ions, and have good thermal stability to improve the safety of the battery.
Preferably, the spacer material layer located between the first polar material layer and the second polar material layer has pores.
Preferably, in the cutting step in step (4), the cutting edge of the side corresponding to the first blank area is consistent with the edge of the second polar material layer, and the cutting edge of the side corresponding to the second blank area is consistent with the edge of the first polar material layer.
The present invention is not limited to the cutting method, including but not limited to laser cutting, linear cutting, and knife cutting.
As a preferable technical solution of the method of the present invention, the method further includes repeating steps (1) - (4) at least 1 time after step (4), so as to obtain the cell unit of the lamination structure. The cell unit formed in this condition is a multi-cell, that is, the cell unit includes at least 2 single cells in the form of stacked sheets.
Preferably, the method further comprises a step of drying before the cutting step.
Preferably, the method further includes, after the cutting step is completed, providing a conductive layer on end faces of a side corresponding to the first blank region and a side corresponding to the second blank region of the battery cell.
The form of the conductive layer is not limited in the present invention, and the conductive layer may be coated with conductive paste or bonded with conductive paste.
In the invention, the first isolation material layer and the second isolation material layer form an isolation structure, and the isolation structure comprises an isolation layer positioned between the first isolation material layer and the second isolation material layer and an isolation part (the vertical section of the isolation structure is Z-shaped) positioned at the edge of the positive material layer and the negative material layer. The conductive layer can be used for connecting the positive electrode tab and the negative electrode tab.
In a second aspect, the present invention provides a current collector-free battery cell prepared by the method in the first aspect, where the current collector-free battery cell includes at least 1 cell unit with a lamination structure, the cell unit includes a first polar material layer, a second polar material layer, and an isolation structure filled between the first polar material layer and the second polar material layer, the isolation structure is in contact with the first polar material layer and the second polar material layer, respectively, a vertical cross section of the isolation structure is zigzag, where two parallel edges of the zigzag are located at an edge of a positive electrode material layer and an edge of a negative electrode material layer, respectively, and polarities of the first polar material layer and the second polar material layer are opposite.
The number of the cell units in the invention is at least 1, for example, 1, 2, 3, 5, 6, 8, 10, 12 or 15.
In the present invention, the "laminated structure" means: a structure formed by stacking layers upon one another.
In the battery core provided by the invention, the isolation structure effectively isolates the positive electrode and the negative electrode, the energy density of the battery is improved because of no current collector, and the safety performance of the battery core in the production and use processes is ensured because of the compact electrode structure.
As a preferred technical scheme of the battery core, the included angle of the Z shape is 90 ℃.
Preferably, in the vertical cross section, the thickness of the portion of the separator structure located between the positive electrode material layer and the negative electrode material layer is 10 μm to 300 μm, such as 10 μm, 20 μm, 30 μm, 40 μm, 50 μm, 60 μm, 70 μm, 85 μm, 100 μm, 150 μm, 200 μm, 240 μm, 265 μm, 300 μm, etc., preferably 20 μm to 200 μm.
Preferably, the thickness of the portions of the separator structure at the edges of the positive/negative electrode material layers is independently 100 μm-1000 μm, such as 100 μm, 150 μm, 200 μm, 300 μm, 400 μm, 500 μm, 600 μm, 650 μm, 750 μm, 800 μm, 900 μm or 1000 μm, etc., preferably 200 μm-500 μm.
In the battery cell of the invention, the isolation structure is partitioned. The isolation structure can be made of a single type or multiple types, so long as the effect of isolating the positive electrode from the negative electrode to avoid short circuit and ensuring lithium ions to be transmitted between the positive electrode and the negative electrode can be achieved, and insulating materials commonly used in the field can be used for the invention.
For example, the material of the portion of the isolation structure between the positive electrode material layer and the negative electrode material layer may be the same as or different from the material of the portion of the isolation structure at the edge of the positive electrode material layer/the negative electrode material layer.
In a third aspect, the present invention provides a lithium ion battery, which includes the current collector-free battery cell of the second aspect.
Compared with the prior art, the invention has the following beneficial effects:
the invention creatively adopts the lamination type process to construct the cell structure, the manufacturing process is simple to operate, a plurality of cell units can be obtained by one-time manufacturing, the manufacturing process is simplified, the working efficiency is improved, and the energy density of the battery can be effectively improved.
The lithium ion battery cell manufactured by the method has controllable shape, size and capacity, and is easy to realize commercial application. The electrode has the characteristics of compact structure and good safety.
Drawings
FIG. 1 is a schematic view of a positive electrode material layer region and a peripheral blank region according to a first embodiment;
FIG. 2 is a schematic view of a region of the negative electrode material layer and a peripheral blank region according to the first embodiment;
fig. 3 is a schematic cross-sectional view of a laminated cell unit according to the first embodiment;
FIG. 4 is a schematic view of a layer region and a peripheral blank region of the cathode material in the second embodiment;
fig. 5 is a schematic view of the negative electrode material layer region and the peripheral blank region in the second embodiment.
Detailed Description
The technical solutions of the present invention are further described by the following embodiments with reference to the accompanying drawings, but the present invention is not limited thereto.
The present invention will be described in detail by way of examples. The embodiments described below with reference to the drawings are exemplary and intended to be illustrative of the present invention and should not be construed as limiting the scope of the present invention. The specific process parameters and the like of the following examples are also only one example of suitable ranges, and a person skilled in the art can select the process parameters and the like within the suitable ranges through the description of the invention, and the specific selection of the following examples is not limited.
First, a basic scheme of materials used in the examples of the present invention is briefly described:
the invention provides a laminated current collector-free lithium ion battery cell and a manufacturing process thereof, wherein the manufacturing process of the cell comprises the following raw materials of a positive electrode material layer: selecting a positive electrode active material, a conductive agent and a binder to mix and prepare a dry powder material; raw materials of the anode material layer: selecting a negative electrode active material and a binder to mix to prepare a dry powder; isolating substance: at least one of a ceramic dielectric material, a solid electrolyte material and a polyolefin is selected. The method comprises the following steps:
selecting a positive electrode active material lithium cobaltate, a conductive agent acetylene black and a binder polyvinylidene fluoride to mix to prepare a dry powder, and spraying the dry powder on a designated area of a hydrophobic easily-stripped platform to obtain a positive electrode material layer, wherein the specific area is shown in figure 1 and comprises a positive electrode material layer area 111 and a peripheral blank area 112;
spraying an isolating material above the positive electrode material layer and in the blank area on the periphery, specifically, mixing a ceramic dielectric material with a binder and a solvent to prepare slurry, and spraying to obtain a plane full of the isolating material again;
thirdly, spraying a negative electrode material layer in a specified area above the plane of the step, wherein the specific area is as shown in fig. 2 and comprises a negative electrode material layer area 113 and a peripheral blank area 114, and the area is consistent with the area of the positive electrode material layer in shape and size, and most importantly, the two material layers must be staggered;
step four, spraying and filling the blank area 114 with an isolating substance material;
and fifthly, drying, cutting and peeling the prepared laminated material layer integrally to obtain the laminated current collector-free lithium ion battery cell.
Note that, the cutting process adopts a laser cutting machine, and the laminated material layer can be firstly cut into an integral strip shape, and then cut into bare cells with different shapes and sizes according to actual needs. The section of the bare cell unit after cutting is as shown in fig. 3, and the whole unit 1, the unit of this embodiment, includes a positive electrode material layer 11, a negative electrode material layer 12 and a separator material layer 13.
A plurality of units can be obtained by one-time manufacturing, and the working efficiency is improved.
The shape, the size and the capacity of the cell unit can be controlled.
The embodiment of the invention also provides a lithium ion battery, in particular to a laminated current collector-free lithium ion battery, which is prepared by adopting the prepared naked battery cell, and the specific implementation mode is as follows:
firstly, coating a layer of silver paste or other conductive substances on the cut electrode end surface of a cell unit comprising a positive electrode material layer, a negative electrode material layer and a separation material layer;
then, soaking the battery core with electrolyte to fill the battery core isolating substance material layer with the electrolyte;
then, assembling the battery cell filled with the electrolyte with a shell with a corresponding size to obtain a lithium ion battery; or, the battery core is packaged by using an insulating coating or a coating layer, and the tab is led out to obtain the lithium ion battery.
Example one
Selecting a positive electrode active material lithium cobaltate, a conductive agent acetylene black and a binder polyvinylidene fluoride to mix to prepare a dry powder, and spraying the dry powder on a designated area of a hydrophobic easily-stripped platform to obtain a positive electrode material layer with the thickness of 150 mu m and the surface density of 400g/m2Specific areas are shown in fig. 1, and include a positive electrode material layer area 111 and a peripheral blank area 112;
spraying an isolating material above the positive electrode material layer and in the blank area at the periphery, specifically, spraying a ceramic dielectric material Al2O3Mixing with a binder polyvinylidene fluoride and a solvent N-methyl pyrrolidone to prepare slurry, and spraying to obtain a plane full of the isolation material with the thickness of 30 mu m;
thirdly, spraying a negative electrode material layer in a specified area above the plane in the step, wherein the thickness of the negative electrode material layer is 150 mu m, and the area density of the negative electrode material layer is 200g/m2Specific regions include a negative electrode material layer region 113 and a peripheral blank region 114, as shown in fig. 2, and it is noted that the regions are in accordance with the shape and size of the regions of the positive electrode material layer, and the regions are shifted by 2mm in the horizontal direction compared with the regions of the positive electrode material layer;
step four, spraying and filling the blank area 114 with the thickness of 150 μm by using an isolating substance material;
and fifthly, drying, cutting and peeling the prepared laminated material layer integrally to obtain the laminated current collector-free lithium ion battery cell.
Note that, the cutting process adopts a laser cutting machine, linear cutting or cutter cutting, and the laminated material layer can be firstly cut into an integral strip shape, and then cut into bare cells with different shapes and sizes according to actual needs. The section of the bare cell unit after cutting is as shown in fig. 3, and the whole unit 1, the unit of this embodiment, includes a positive electrode material layer 11, a negative electrode material layer 12 and a separator material layer 13.
A plurality of units can be obtained by one-time manufacturing, and the working efficiency is improved.
The shape, the size and the capacity of the cell unit can be controlled.
Example two
The invention relates to a laminated current collector-free lithium ion battery cell and a manufacturing process thereof, wherein the manufacturing process of the cell basically has the same steps as the first embodiment, only the difference of specific areas is included, and the specific steps are as follows:
step one, spraying a positive electrode material layer on a designated area of a hydrophobic easily-stripped platform, wherein the specific area is shown in fig. 4 and comprises a positive electrode material layer area 211 and a peripheral blank area 212;
secondly, spraying an isolating substance material above the anode material layer and in the blank area on the periphery of the anode material layer to obtain a plane full of the isolating material again;
step three, spraying a negative electrode material layer in a specified area above the plane of the step, wherein the specific area is as shown in fig. 5 and comprises a negative electrode material layer area 213 and a peripheral blank area 214, and the area is in accordance with the area of the positive electrode material layer in shape and size and is displaced by 2mm in the horizontal direction compared with the area of the positive electrode material layer;
step four, spraying and filling the blank area 214 with an isolating substance material;
and fifthly, drying, cutting and peeling the prepared laminated material layer integrally to obtain the laminated current collector-free lithium ion battery cell.
A plurality of units can be obtained by one-time manufacturing, and the working efficiency is improved.
The shape and the size of the battery cell unit can be controlled when the material layer is sprayed.
In this embodiment, the thickness and the areal density of the positive electrode material layer and the negative electrode material layer are the same as those in the first embodiment.
EXAMPLE III
The laminated current collector-free lithium ion battery of the embodiment is manufactured by the bare cell prepared in the first embodiment and the bare cell prepared in the second embodiment, and the specific implementation manner is as follows:
firstly, coating a layer of silver paste on the end face of a cut electrode of the cell unit containing the positive electrode material layer, the negative electrode material layer and the isolating substance material layer obtained in the first embodiment and the second embodiment;
then, soaking the battery core with electrolyte to fill the battery core isolating substance material layer with the electrolyte;
and then assembling the battery cell filled with the electrolyte with a shell with a corresponding size to obtain the lithium ion battery.
In this embodiment, the thickness and the areal density of the positive electrode material layer and the negative electrode material layer are the same as those in the first embodiment.
Example four
The laminated current collector-free lithium ion battery of the embodiment is manufactured by the bare cell prepared in the first embodiment and the bare cell prepared in the second embodiment, and the specific implementation manner is as follows:
firstly, coating a layer of silver paste on the end face of a cut electrode of the cell unit containing the positive electrode material layer, the negative electrode material layer and the isolating substance material layer obtained in the first embodiment and the second embodiment;
then, soaking the battery core with electrolyte to fill the battery core isolating substance material layer with the electrolyte;
and then, packaging the battery cell by using an insulating coating or a coating layer, and leading out a tab to obtain the lithium ion battery.
In this embodiment, the thickness and the areal density of the positive electrode material layer and the negative electrode material layer are the same as those in the first embodiment.
EXAMPLE five
Selecting a positive electrode active material lithium cobaltate, a conductive agent acetylene black, a binder polyvinylidene fluoride and a solvent N-methyl pyrrolidone, mixing to prepare slurry, and 3D printing the slurry on a specified area of a hydrophobic easily-stripped platform to obtain a positive electrode material layer with the thickness of 150 mu m and the surface density of 400g/m2Drying and shaping;
coating isolation material above the positive electrode material layer and in the peripheral blank area, specifically, coating ceramic dielectric material Al2O3With a binder of polyvinylidene fluorideMixing ethylene and solvent N-methyl pyrrolidone to prepare slurry, performing 3D printing to obtain a plane full of the isolation material with the thickness of 30 mu m, and drying and shaping;
step three, coating a negative electrode material layer in a specified area above the plane of the step, wherein the thickness of the negative electrode material layer is 150 mu m, and the area density of the negative electrode material layer is 200g/m2The region is displaced by 2mm in the horizontal direction compared with the region of the positive electrode material layer;
filling the blank area with an isolating substance material, wherein the thickness of the blank area is 150 mu m;
and fifthly, drying, cutting and peeling the prepared laminated material layer integrally to obtain the laminated current collector-free lithium ion battery cell.
The cutting process of the embodiment adopts laser cutting.
A plurality of units can be obtained by one-time manufacturing, and the working efficiency is improved.
The shape, the size and the capacity of the cell unit can be controlled.
EXAMPLE six
Selecting a positive electrode active material lithium cobaltate, a conductive agent acetylene black and a binder polyvinylidene fluoride to mix to prepare a dry powder, and spraying the dry powder on a designated area of a hydrophobic easily-stripped platform to obtain a positive electrode material layer with the thickness of 150 mu m and the surface density of 400g/m2，；
Spraying an isolating material above the positive electrode material layer and in the blank area at the periphery, specifically, spraying a ceramic dielectric material Al2O3Mixing with a binder polyvinylidene fluoride and a solvent N-methyl pyrrolidone to prepare slurry, and spraying to obtain a plane full of the isolation material with the thickness of 40 mu m;
thirdly, spraying a negative electrode material layer in a specified area above the plane in the step, wherein the thickness of the negative electrode material layer is 150 mu m, and the area density of the negative electrode material layer is 200g/m2The region is displaced by 2mm in the horizontal direction compared with the region of the positive electrode material layer;
step four, spraying and filling the blank area with the thickness of 150 mu m by using an isolating substance material;
and fifthly, drying, cutting and peeling the prepared laminated material layer integrally to obtain the laminated current collector-free lithium ion battery cell.
A plurality of units can be obtained by one-time manufacturing, and the working efficiency is improved.
The shape, the size and the capacity of the cell unit can be controlled.
EXAMPLE seven
Selecting a positive active material lithium manganate, a conductive agent acetylene black and a binder polyvinylidene fluoride to mix to prepare a dry powder, and spraying the dry powder on a designated area of a hydrophobic easily-stripped platform to obtain a positive material layer with the thickness of 150 mu m and the surface density of 400g/m2；
Secondly, spraying an isolating substance material above the anode material layer and in a peripheral blank area, specifically, directly spraying a solid electrolyte to obtain a plane full of the isolating material, wherein the thickness of the plane is 30 microns;
thirdly, spraying a negative electrode material layer in a specified area above the plane in the step, wherein the thickness of the negative electrode material layer is 150 mu m, and the area density of the negative electrode material layer is 200g/m2The region is displaced by 2mm in the horizontal direction compared with the region of the positive electrode material layer;
step four, spraying and filling the blank area with the thickness of 150 mu m by using an isolating substance material;
and fifthly, drying, cutting and peeling the prepared laminated material layer integrally to obtain the laminated current collector-free lithium ion battery cell.
A plurality of units can be obtained by one-time manufacturing, and the working efficiency is improved.
The shape, the size and the capacity of the cell unit can be controlled.
Comparative example 1
Selecting a positive electrode active material lithium cobaltate, a conductive agent acetylene black and a binder polyvinylidene fluoride to mix to prepare a dry powder, and spraying the dry powder on a designated area of a hydrophobic easily-stripped platform to obtain a positive electrode material layer with the thickness of 150 microns;
step two, on the positive electrode material layer andspraying isolation material on the peripheral blank region, specifically, spraying ceramic dielectric material Al2O3Mixing with a binder polyvinylidene fluoride and a solvent N-methyl pyrrolidone to prepare slurry, and spraying to obtain a plane full of the isolation material with the thickness of 30 mu m;
thirdly, spraying a negative electrode material layer with the thickness of 150 μm in a specified area above the plane of the step, and noting that the area completely corresponds to the area of the positive electrode material layer without dislocation;
step four, spraying and filling the blank area with the thickness of 150 mu m by using an isolating substance material;
and fifthly, drying, cutting and peeling the prepared laminated material layer integrally to obtain the laminated current collector-free lithium ion battery cell.
The battery core prepared by the embodiment has defects in structure, and cannot lead out a tab and form a lithium ion battery.
Comparative example No. two
And preparing positive electrode slurry by adopting the positive electrode active material, the conductive agent and the binder with the same type and content as those in the first embodiment, coating the positive electrode slurry on the surface of the aluminum foil, and drying to obtain the positive electrode piece.
And preparing negative electrode slurry, coating the negative electrode slurry on the surface of the copper foil, and drying to obtain a negative electrode plate, wherein the composition of a negative electrode material layer in the negative electrode plate is the same as that in the first embodiment.
And (3) adopting a positive pole piece and a negative pole piece, isolating the positive pole piece and the negative pole piece by using a diaphragm, and laminating to obtain the battery core.
And (3) effect analysis:
firstly, the energy density is high, and the electrochemical performance is good:
in the existing typical cell structure, as in comparative example two, the ratio of the weight occupied by the copper foil and the aluminum foil to the positive and negative active materials is about 1:5 (about 1:8 for positive electrode and about 1:2 for negative electrode). While copper foil and aluminum foil do not contribute energy.
In the embodiment of the application, no copper foil or aluminum foil exists, and under the condition of the same ratio of the conductive agent to the binder, the weight of the battery cell is reduced, and the energy density of the battery cell is improved.
Even if the proportion of the conductive agent and the adhesive is increased, the capacity and the energy density of the battery cell can be improved under the condition that the increasing proportion is lower than the specific gravity of copper foil and aluminum foil in the existing battery cell structure (for example, the increasing proportion is not more than 5 percent), the weight of the battery cell can be reduced by about 15 percent, and the energy density is converted into the energy density, namely the energy density is increased by about 15 percent.
Secondly, the safety is good:
compared with the existing battery cell structure, the diaphragm made of the traditional PP/PE material is cancelled, and after the diaphragm is replaced by the inorganic oxide material, the diaphragm does not shrink and burn at high temperature, so that the safety guarantee is improved.
The foregoing is merely an exemplary embodiment of the invention and other variations may be readily made without departing from the true scope of the invention as described in the following claims.
The applicant states that the present invention is illustrated in detail by the above examples, but the present invention is not limited to the above detailed methods, i.e. it is not meant that the present invention must rely on the above detailed methods for its implementation. It should be understood by those skilled in the art that any modification of the present invention, equivalent substitutions of the raw materials of the product of the present invention, addition of auxiliary components, selection of specific modes, etc., are within the scope and disclosure of the present invention.

Claims (10)

1. A preparation method of a current collector-free battery core is characterized by comprising the following steps:
(1) preparing a first polar material layer, wherein the first polar material layer comprises a first material area and a first blank area positioned on one side of the first material area;
(2) forming a first isolation material layer on the first polar material layer and the first blank region using an isolation material;
(3) preparing a second polarity material layer on the first isolation material layer, wherein the polarity of the second polarity material layer is opposite to that of the first polarity material layer, and the second polarity material layer comprises a second material area and a second blank area which is positioned on one side of the second material area and is opposite to the first blank area;
the first material area and the second material area are partially overlapped in the horizontal projection direction;
(4) forming a second isolation material layer in the second blank area by using an isolation substance, wherein the first isolation material layer and the second isolation material layer form an isolation structure, and the isolation structure separates the first polarity material layer from the second polarity material layer to obtain a battery cell unit of a lamination structure;
(5) and cutting along the edge of the battery cell unit to obtain the battery cell without the current collector.
2. The method according to claim 1, wherein the raw materials used for preparing the first polar material layer in the step (1) and the second polar material layer in the step (3) are electrode mixtures, and the electrode mixtures are anode mixtures or cathode mixtures;
preferably, the method of preparing the first polar material in step (1) and the second polar material in step (3) is independently selected from at least one of coating, preferably pressure coating, and filling, preferably deposition; preferably, the positive electrode mix includes a positive electrode active material, a binder, and a conductive agent;
preferably, the anode mix comprises an anode active material, a binder, and optionally a conductive agent;
preferably, the positive active material comprises at least one of lithium cobaltate, lithium manganate, lithium iron phosphate, lithium manganese phosphate, a nickel-cobalt-manganese ternary material and a nickel-cobalt-aluminum ternary material;
preferably, the negative active material comprises at least one of lithium titanate, natural graphite, artificial graphite, carbon fiber, soft carbon, hard carbon, mesocarbon microbeads, elemental silicon, silicon oxide and silicon-carbon composite;
preferably, the binder in the positive electrode mixture and the negative electrode mixture is independently selected from at least one of polyvinylidene fluoride, polytetrafluoroethylene, polyacrylic acid and polyvinyl alcohol;
preferably, the conductive agent in the positive electrode mixture and the negative electrode mixture is independently selected from at least one of conductive carbon black, acetylene black, ketjen black, Super P, Super S, carbon nanotube, graphene, porous carbon and carbon fiber.
3. The method of claim 1 or 2, wherein the first polar material layer is a positive electrode material layer, and the second polar material layer is a negative electrode material layer; or, the first polar material layer is a negative electrode material layer, and the second polar material layer is a positive electrode material layer;
preferably, the first polar material layer is formed on the substrate table.
4. The method according to any one of claims 1 to 4, wherein the number of the first polar material layers is at least 2;
preferably, the number of the second polarity material layers is at least 2;
preferably, the number of the second polar material layers is the same as that of the first polar material layers;
preferably, the shape and size of the second material area are consistent with those of the first material area;
preferably, the partial coincidence of the first material area and the second material area in the horizontal projection direction is realized by the following mode: the second material area is staggered along a single direction relative to the first material area.
5. The method according to any one of claims 1 to 4, wherein in step (2), a first isolating material layer is formed by filling and/or coating a material containing isolating substances on the first polar material layer and the first empty area;
preferably, in the step (4), in the second blank area, filling and/or coating a material containing a separation substance to form a second separation material layer;
preferably, in the step (2) and the step (4), the coating mode is a casting method;
preferably, the isolating substances of step (2) and step (4) are the same or different in kind;
preferably, the kinds of the separator in the steps (2) and (4) independently include at least one of a solid electrolyte, a ceramic dielectric material, and a polyolefin;
preferably, at least a portion of the isolation structure located between the first polar material layer and the second polar material layer has lithium ion conductivity;
preferably, the spacer material layer located between the first polar material layer and the second polar material layer has pores.
6. The method according to any one of claims 1 to 5, wherein in the cutting step of step (4), the cutting edge of the corresponding side of the first blank area coincides with the edge of the second polarity material layer, and the cutting edge of the corresponding side of the second blank area coincides with the edge of the first polarity material layer;
preferably, the cutting of step (4) includes at least one of laser cutting, wire cutting and cutter cutting.
7. The method of any one of claims 1 to 6, further comprising repeating steps (1) to (4) at least 1 time after step (4) to obtain a laminated structure of the cell units.
8. The method according to any one of claims 1 to 7, further comprising a step of drying before the cutting step;
preferably, after the cutting step is completed, providing conductive layers on end faces of a side corresponding to the first blank area and a side corresponding to the second blank area of the battery cell;
preferably, the disposing manner includes at least one of coating conductive paste or attaching conductive paste.
9. The current collector-free cell prepared by the method of any one of claims 1 to 8, wherein the current collector-free cell comprises at least 1 cell unit of a lamination structure, the cell unit comprises a first polar material layer, a second polar material layer and an isolation structure filled between the first polar material layer and the second polar material layer, the isolation structure is in contact with the first polar material layer and the second polar material layer respectively, the isolation structure has a zigzag vertical cross section, wherein two parallel edges of the zigzag are located at an edge of the positive electrode material layer and an edge of the negative electrode material layer respectively, and polarities of the first polar material layer and the second polar material layer are opposite;
preferably, the included angle of the Z shape is 90 ℃;
preferably, in the vertical cross section, the thickness of the part of the isolation structure between the positive electrode material layer and the negative electrode material layer is 10 μm to 300 μm, preferably 20 μm to 200 μm;
preferably, the thickness of the portions of the separator structure located at the edges of the positive electrode material layer/negative electrode material layer is independently 100 μm to 1000 μm, preferably 200 μm to 500 μm.
10. A lithium ion battery comprising the current collector-less cells of claim 9.
CN202011125847.4A 2020-10-20 2020-10-20 Current collector-free battery core, preparation method thereof and lithium ion battery Active CN112151875B (en)

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