CN110994011A - Interlocking type all-solid-state lithium ion battery membrane blank and forming method and forming device thereof - Google Patents
Interlocking type all-solid-state lithium ion battery membrane blank and forming method and forming device thereof Download PDFInfo
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- CN110994011A CN110994011A CN201911058229.XA CN201911058229A CN110994011A CN 110994011 A CN110994011 A CN 110994011A CN 201911058229 A CN201911058229 A CN 201911058229A CN 110994011 A CN110994011 A CN 110994011A
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- 239000012528 membrane Substances 0.000 title claims abstract description 130
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 86
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 86
- 238000000034 method Methods 0.000 title claims abstract description 42
- 238000001125 extrusion Methods 0.000 claims abstract description 75
- 238000007666 vacuum forming Methods 0.000 claims abstract description 59
- 239000007784 solid electrolyte Substances 0.000 claims abstract description 56
- 229920000642 polymer Polymers 0.000 claims abstract description 54
- 238000013329 compounding Methods 0.000 claims abstract description 15
- 238000010345 tape casting Methods 0.000 claims abstract description 13
- 239000011888 foil Substances 0.000 claims description 10
- 229910052782 aluminium Inorganic materials 0.000 claims description 9
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical group [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 9
- 238000000465 moulding Methods 0.000 claims description 9
- 239000007787 solid Substances 0.000 claims description 9
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical group [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 6
- 239000011889 copper foil Substances 0.000 claims description 6
- 229910052744 lithium Inorganic materials 0.000 claims description 4
- 230000007246 mechanism Effects 0.000 claims description 4
- 150000001875 compounds Chemical class 0.000 claims 1
- 238000005086 pumping Methods 0.000 claims 1
- 238000004519 manufacturing process Methods 0.000 abstract description 9
- 239000000243 solution Substances 0.000 description 16
- 230000000694 effects Effects 0.000 description 13
- 238000004049 embossing Methods 0.000 description 13
- 238000007731 hot pressing Methods 0.000 description 10
- 239000000155 melt Substances 0.000 description 9
- 238000001291 vacuum drying Methods 0.000 description 8
- 238000005266 casting Methods 0.000 description 7
- 239000000853 adhesive Substances 0.000 description 6
- 230000001070 adhesive effect Effects 0.000 description 6
- 230000009977 dual effect Effects 0.000 description 6
- 238000007493 shaping process Methods 0.000 description 6
- 239000002904 solvent Substances 0.000 description 6
- 238000010586 diagram Methods 0.000 description 5
- 239000005518 polymer electrolyte Substances 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 239000002002 slurry Substances 0.000 description 4
- 239000006258 conductive agent Substances 0.000 description 3
- 238000013461 design Methods 0.000 description 3
- 238000012545 processing Methods 0.000 description 3
- 239000011149 active material Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 239000003792 electrolyte Substances 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
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- 239000000463 material Substances 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 230000002035 prolonged effect Effects 0.000 description 2
- 238000005096 rolling process Methods 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 1
- 239000013543 active substance Substances 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 210000001787 dendrite Anatomy 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000011244 liquid electrolyte Substances 0.000 description 1
- 238000003760 magnetic stirring Methods 0.000 description 1
- 210000001161 mammalian embryo Anatomy 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000007773 negative electrode material Substances 0.000 description 1
- -1 polytetrafluoroethylene Polymers 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000007774 positive electrode material Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 238000003672 processing method Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000010008 shearing Methods 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 238000004513 sizing Methods 0.000 description 1
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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
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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Abstract
The invention discloses an interlocking type all-solid-state lithium ion battery membrane blank, a forming method and a forming device thereof. The forming method comprises the steps of firstly adopting a co-extrusion mode to extrude and form the polymer solid electrolyte membrane, the anode active layer and the cathode active layer together, then adopting an imprinter to perform tape casting hot-press forming with the anode current collector and the cathode current collector, and forming a groove-shaped or convex integral interlocking structure while compounding. The device comprises a plurality of extruders, a multilayer co-extrusion die head, a positive and negative current collector sleeve and a stamping press, wherein the plurality of extruders are connected with the multilayer co-extrusion die head together, and a plurality of grooves are distributed on the surface of a vacuum forming roller in the stamping press. The invention can effectively shorten the production cycle of the lithium ion battery, and can effectively improve the structural stability of the lithium ion battery.
Description
Technical Field
The invention relates to the technical field of new energy lithium ion batteries, in particular to an interlocking type all-solid-state lithium ion battery membrane blank and a forming method and a forming device thereof.
Background
In recent years, lithium ion batteries with high energy density, high output voltage and long cycle life and low capacity fade have enjoyed tremendous success as the primary power source for electric vehicles and modern energy storage systems. However, lithium ion batteries containing organic liquid electrolytes are prone to dangerous phenomena such as chemical side reactions, lithium dendrites and leakage, internal short circuits, etc. All-solid-state lithium ion batteries containing solid polymer electrolytes are considered to be a very promising alternative due to their high safety.
The all-solid-state lithium ion battery mainly comprises a positive electrode, a negative electrode and a solid polymer electrolyte. At present, the all-solid-state lithium ion battery is mainly formed by cold press molding of a positive pole piece, a solid electrolyte membrane and a negative pole piece which are prepared by different processing methods, and each layer of structure is simply laminated in a plane shape. These planar all-solid-state lithium ion batteries have problems of small contact area, poor interfacial adhesion of the respective layers, and easy peeling of the respective layers when subjected to bending.
In the existing lithium ion battery manufacturing process, the solid polymer electrolyte membrane is usually prepared by a solution casting method. The method comprises the specific processes of quantitatively adding dried raw materials into a solvent, uniformly stirring by means of magnetic stirring or ultrasonic mixing and the like, casting the uniformly mixed solution into a polytetrafluoroethylene mold, and volatilizing the solvent under certain conditions to obtain the solid polymer electrolyte film. However, in practical application, the film prepared by the method inevitably has certain pores due to solvent volatilization, has poor surface flatness, needs to be subjected to hot pressing and sizing treatment, and has a complex process.
The positive and negative electrodes of the lithium ion battery are composed of positive and negative electrode materials, a conductive agent, an adhesive, a current collector and the like. The positive and negative electrode plates are prepared by respectively mixing a special solvent and an adhesive with powdery positive and negative active substances, uniformly stirring to prepare slurry positive and negative substances, respectively and uniformly coating the positive and negative slurries on the surface of a metal foil through an automatic coating machine, drying and shearing.
And finally, the prepared positive and negative pole pieces and the solid polymer electrolyte film are directly assembled into the all-solid-state lithium ion battery through cold pressing at room temperature by a glove box.
In the manufacturing process of the lithium ion battery, the battery is prepared by adopting a solution casting method, the production cycle of the battery is longer, the solid electrolyte film and the positive and negative pole pieces are in a two-dimensional solid-solid contact mode, and even if the improvement is realized by adopting measures of changing the formula of the adhesive, improving the content of the adhesive and the like, the interface contact area and the interface contact effect of the polymer solid electrolyte film and the positive and negative pole pieces are still not ideal, so that the preparation of the flexible battery and the overall performance of the whole battery are influenced.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provide an interlocking type full-solid-state lithium ion battery membrane blank, which has a three-dimensional interlocking structure, the interface contact area between a polymer solid electrolyte membrane and positive and negative electrode plates is larger, the contact structure is stable, and the phenomenon that the performance is influenced because the interface is easy to fall off when the battery is bent can be effectively avoided.
The invention also aims to provide a forming method of the interlocking type all-solid-state lithium ion battery membrane blank, which is a co-extrusion-stamping forming method, so that the production period of the lithium ion battery can be effectively shortened, and the structural stability of the lithium ion battery can be effectively improved.
The invention further aims to provide a forming device of the interlocking type all-solid-state lithium ion battery membrane blank.
The technical scheme of the invention is as follows: an interlocking type full-solid-state lithium ion battery membrane blank is an integrated multilayer structure with an integrated interlocking structure and comprises a positive pole piece and a polymer solid electrolyte membrane which are connected; the integral interlocking structure is a groove-shaped or bulge-shaped embedded structure with overlapped multilayer structures.
Furthermore, the lithium ion battery also comprises a negative pole piece, wherein the positive pole piece, the polymer solid electrolyte membrane and the negative pole piece are sequentially connected, and an integral interlocking structure is formed among the positive pole piece, the polymer solid electrolyte membrane and the negative pole piece.
In the structure, a groove-shaped or convex-shaped embedded structure is directly formed among the multilayer structures, so that a three-dimensional interlocking structure is formed between the polymer solid electrolyte membrane and the positive pole piece and the negative pole piece on two sides or one side of the polymer solid electrolyte membrane, a good interface contact effect is achieved, the contact structure is stable, the phenomenon that the interface falls off when the battery is bent can be effectively avoided, and a foundation is laid for the development of the flexible lithium ion battery.
The positive pole piece comprises a positive current collector and a positive active layer, the positive active layer is arranged between the polymer solid electrolyte membrane and the positive current collector, and the positive active layer and the polymer solid electrolyte membrane are jointly extruded to form an integral structure.
The negative pole piece comprises a negative pole current collector and a negative pole active layer, the negative pole active layer is arranged between the polymer solid electrolyte membrane and the negative pole current collector, and the positive pole active layer, the polymer solid electrolyte membrane and the negative pole active layer are extruded together to form an integrated structure.
The positive current collector is an aluminum foil layer, and the negative current collector is a copper foil layer or a lithium metal layer.
The invention relates to a forming method of an interlocking type all-solid-state lithium ion battery membrane blank, which comprises the steps of firstly, co-extruding a polymer solid electrolyte membrane and a positive active layer to form a primary membrane blank; and compounding a positive current collector on one side of the positive active layer, and performing tape casting hot-press molding by using an imprinter to ensure that the primary film blank and the positive current collector form a groove-shaped or convex integral interlocking structure while being compounded.
Compounding a negative pole piece on one side of the polymer solid electrolyte membrane by adopting a glove box after the lithium ion battery membrane blank is formed; and the positive active layer and the positive current collector positioned on the other side of the polymer solid electrolyte membrane form a positive pole piece.
During the co-extrusion molding, the polymer solid electrolyte membrane is in a melt extrusion mode, and the positive active layer is in a melt extrusion or solution extrusion mode.
When the positive active layer adopts a solution extrusion mode, the positive current collector adopts an aluminum foil with a porous structure.
The invention discloses a forming method of an interlocking type full-solid-state lithium ion battery membrane blank, which comprises the steps of firstly, co-extruding and forming a positive electrode active layer, a polymer solid electrolyte membrane and a negative electrode active layer in a co-extrusion mode to form a primary membrane blank; and compounding a positive current collector on one side of the positive active layer, compounding a negative current collector on one side of the negative active layer, and performing tape casting hot press molding by using an imprinter to ensure that the positive current collector, the primary film blank and the negative current collector form a groove-shaped or convex integral interlocking structure while compounding.
During the co-extrusion molding, the polymer solid electrolyte membrane adopts a melt extrusion mode, the positive electrode active layer adopts a melt extrusion or solution extrusion mode, and the negative electrode active layer adopts a melt extrusion or solution extrusion mode.
When the positive active layer adopts a solution extrusion mode, the positive current collector adopts an aluminum foil with a porous structure; when the negative active layer adopts a solution extrusion mode, the negative current collector adopts copper foil with a porous structure.
In the two forming methods, the polymer solid electrolyte membrane is formed by adopting a melt extrusion mode, and the method has the advantages of short production period, flat and smooth surface of the electrolyte membrane, no gap generated by solvent volatilization, environmental friendliness and the like. In the co-extrusion process of the positive active layer and the negative active layer, a very good interface bonding effect can be achieved by adopting a melt extrusion mode; when the solution extrusion mode is adopted, the content of the adhesive can be effectively reduced, and the content of the active material and the conductive agent in the positive active layer and the negative active layer is improved, so that the performances of the positive pole piece and the negative pole piece are improved.
Meanwhile, in the two forming methods, the casting hot-press forming is carried out immediately after the co-extrusion is finished, at the moment, the polymer solid electrolyte membrane is in a molten state, the positive electrode active layer and the negative electrode active layer are in a slurry state or a molten state, and the material in the state can ensure a good interface contact effect through casting hot-press.
The interlocking type full-solid-state lithium ion battery membrane blank has a three-dimensional interlocking type structure after being formed, and can be curled and collected after being subjected to subsequent treatment such as vacuum drying.
The invention relates to a forming device of an interlocking type all-solid-state lithium ion battery membrane blank, which comprises a first extruder, a third extruder, a multilayer co-extrusion die head, a positive current collector sleeve and a stamping press, wherein the machine head of the first extruder and the machine head of the third extruder are connected with the multilayer co-extrusion die head together; a plurality of grooves are distributed on the surface of a vacuum forming roller in the stamping machine.
The invention discloses another forming device of an interlocking type full-solid lithium ion battery membrane blank, which comprises a first extruder, a second extruder, a third extruder, a multi-layer co-extrusion die head, a positive current collector sleeve, a negative current collector sleeve and a stamping press, wherein the machine head of the first extruder, the machine head of the second extruder and the machine head of the third extruder are connected with the multi-layer co-extrusion die head together; a plurality of grooves are distributed on the surface of a vacuum forming roller in the stamping machine.
In the forming device for the two interlocking type all-solid-state lithium ion battery membrane blanks, the hot-press forming roller set is arranged in the stamping machine and comprises a vacuum forming roller and an auxiliary forming roller which are matched with each other, and the surface of the auxiliary forming roller is a smooth surface or is distributed with a plurality of protrusions matched with grooves on the surface of the vacuum forming roller.
A plurality of through holes are further distributed in the groove in the surface of the vacuum forming roller, and each through hole is externally connected with a vacuumizing mechanism through a flow passage in the vacuum forming roller. The flow channel design in the vacuum forming roller is the same as or similar to that of the existing vacuum roller. When the vacuum forming roller is vacuumized, the film blank close to the vacuum forming roller can be tightly attached to the vacuum forming roller under the dual actions of extrusion force and vacuum suction force, so that the structure on the surface of the vacuum forming roller is embossed and copied.
According to the actual requirement of the lithium ion battery, the grooves on the surface of the vacuum forming roller can be designed into various shapes such as hexagon, quadrangle, circle, honeycomb and the like. When a primary film blank formed by the multilayer co-extrusion die head, a positive current collector from the positive current collector sleeve and a negative current collector from the negative current collector sleeve enter the embossing machine together, the layers of the battery film blank are compacted under the tape casting hot-pressing effect of the embossing machine hot-pressing forming roller group. And vacuumizing the vacuum forming roller, wherein one side attached to the vacuum forming roller is subjected to dual functions of extrusion force and vacuum suction force, and after tape casting hot pressing of a stamping machine, the groove structure of the vacuum forming roller is reversely copied into a battery membrane blank, so that the interlocking type all-solid-state lithium ion battery membrane blank is prepared.
Compared with the prior art, the invention has the following beneficial effects:
the interlocking type all-solid-state lithium ion battery membrane blank has a three-dimensional interlocking structure, the interface contact area between the polymer solid electrolyte membrane and the positive and negative electrode plates is large, the contact structure is stable, the phenomenon that the performance is affected due to the fact that the interface is easy to fall off when the battery is bent can be effectively avoided, and a foundation is laid for research of flexible lithium ion batteries.
The forming method of the interlocking type full-solid-state lithium ion battery membrane blank adopts a co-extrusion-embossing forming mode, can realize continuous one-step forming of the lithium ion battery membrane blank with a three-dimensional interlocking structure, can effectively shorten the production period of the lithium ion battery, has higher production efficiency, firstly forms a polymer solid electrolyte membrane, an anode active layer and a cathode active layer in a co-extrusion mode, then laminates the primary membrane blank in a molten state or a molten-solution state with an anode current collector and a cathode current collector in a flow-delay embossing mode, and simultaneously embosses and forms the three-dimensional interlocking structure of the lithium ion battery membrane blank, so that the prepared lithium ion battery membrane blank has the advantages of good contact effect, stable contact structure and the like, and the overall performance of the lithium ion battery is effectively improved.
In the forming device of the interlocking type all-solid-state lithium ion battery membrane blank, the surface structure of the vacuum forming roller is improved, so that the polymer solid electrolyte membrane, the positive pole piece and the negative pole piece form a three-dimensional interlocking structure while being pressed and attached, and the device is matched with an extruder and a multilayer co-extrusion die head for use.
Drawings
Fig. 1 is a schematic structural diagram of the interlocking type all-solid-state lithium ion battery membrane blank.
Fig. 2 is a schematic diagram illustrating a method for forming a membrane blank of an interlocked all-solid-state lithium ion battery in accordance with example 2.
FIG. 3 is a schematic structural view of a vacuum forming roll.
Fig. 4 is a schematic diagram illustrating a method for forming a membrane blank of an interlocked all-solid-state lithium ion battery in accordance with example 3.
Fig. 5 is a schematic diagram illustrating a method for forming a membrane blank of an interlocked all-solid-state lithium ion battery in accordance with example 4.
Fig. 6 is a schematic diagram illustrating a method for forming a membrane blank of an interlocked all-solid-state lithium ion battery in accordance with example 5.
In the above figures, the components indicated by the respective reference numerals are as follows: 1 is anodal mass flow body, 2 is anodal active layer, 3 is polymer solid electrolyte membrane, 4 is the negative pole active layer, 5 is the negative pole mass flow body, 6 is integral interlocking structure, 7 is first extruder, 8 is the second extruder, 9 is the third extruder, 10 is multilayer coextrusion die head, 11 is the primary film embryo, 12 is the negative pole mass flow body sleeve, 13 is anodal mass flow body sleeve, 14 is the auxiliary forming roller, 15 is the vacuum forming roller, 16 is the collection roller, 17 is the recess, 18 is the vacuum drying case.
Detailed Description
The present invention will be described in further detail with reference to examples, but the embodiments of the present invention are not limited thereto.
Example 1
The interlocking type all-solid-state lithium ion battery membrane blank is an integral multi-layer structure with an integral interlocking structure 6, as shown in fig. 1, and comprises a positive pole piece, a polymer solid electrolyte membrane 3 and a negative pole piece, wherein the positive pole piece, the polymer solid electrolyte membrane and the negative pole piece are sequentially connected, and an integral interlocking structure is formed among the positive pole piece, the polymer solid electrolyte membrane and the negative pole piece; the integral interlocking structure is a groove-shaped or bulge-shaped embedded structure with a multilayer structure overlapped, and in the embodiment, the integral interlocking structure is a boss-shaped structure.
The positive pole piece comprises a positive current collector 1 and a positive active layer 2, wherein the positive active layer is arranged between the polymer solid electrolyte membrane and the positive current collector; the negative pole piece comprises a negative pole active layer 4 and a negative pole current collector 5, the negative pole active layer is arranged between the polymer solid electrolyte membrane and the negative pole current collector, and the positive pole active layer, the polymer solid electrolyte membrane and the negative pole active layer are extruded together to form an integrated structure.
In general, the positive electrode collector may use an aluminum foil layer, and the negative electrode collector may use a copper foil layer or a lithium metal layer.
In the interlocking type all-solid-state lithium ion battery membrane blank structure, a groove-shaped or protrusion-shaped embedded structure is directly formed among the multilayer structures, so that a three-dimensional interlocking structure is formed between the polymer solid electrolyte membrane and the positive pole piece and the negative pole piece on two sides or one side of the polymer solid electrolyte membrane, a good interface contact effect is achieved, meanwhile, the contact structure is stable, the phenomenon that the interface falls off when the battery is bent can be effectively avoided, and a foundation is laid for the development of flexible lithium ion batteries.
Example 2
The embodiment of the invention discloses a method and a device for forming an interlocking type all-solid-state lithium ion battery membrane blank, which are suitable for processing and forming a polymer solid electrolyte membrane, a positive pole piece and a negative pole piece together.
As shown in fig. 2, the forming device of the interlocking type all-solid-state lithium ion battery film blank comprises a first extruder 7, a second extruder 8, a third extruder 9, a multilayer co-extrusion die head 10, a negative current collector sleeve 12, a positive current collector sleeve 13 and a stamping press, wherein the machine head of the first extruder, the machine head of the second extruder and the machine head of the third extruder are connected with the multilayer co-extrusion die head together, the positive current collector sleeve and the negative current collector sleeve are respectively arranged at the outer sides of the multilayer co-extrusion die head, and a primary film blank 11 formed by the multilayer co-extrusion die head, a positive current collector 1 from the current collector positive sleeve and a negative current collector 5 from the negative current collector sleeve enter the stamping press together; the surface of the vacuum forming roller 15 in the embossing press is distributed with a plurality of grooves 17 (as shown in figure 3).
Be equipped with hot briquetting roller set in the coining mill, including matched with supplementary shaping roller 14 and vacuum forming roller 15, the surface of supplementary shaping roller is the smooth surface or distributes and have a plurality ofly and vacuum forming roller surface recess matched with arch, and in this embodiment, supplementary shaping roller adopts the surface to be the structure of smooth surface. In addition, the two sides of the vacuum forming roller are respectively provided with the auxiliary forming rollers, so that the bonding time between the primary film blank and the anode and cathode current collectors can be effectively prolonged, and the bonding effect is further ensured. And rolling the lithium ion battery membrane blank formed after the lamination by using a collection roller 16.
A plurality of through holes are also distributed in the groove on the surface of the vacuum forming roller, and each through hole is externally connected with a vacuumizing mechanism through a flow passage in the vacuum forming roller. The flow channel design in the vacuum forming roller is the same as or similar to that of the existing vacuum roller. When the vacuum forming roller is vacuumized, the film blank close to the vacuum forming roller can be tightly attached to the vacuum forming roller under the dual actions of extrusion force and vacuum suction force, so that the structure on the surface of the vacuum forming roller is embossed and copied.
According to the actual requirement of the lithium ion battery, the grooves on the surface of the vacuum forming roller can be designed into various shapes such as hexagon, quadrangle, circle, honeycomb and the like. When a primary film blank formed by the multilayer co-extrusion die head, a positive current collector from the positive current collector sleeve and a negative current collector from the negative current collector sleeve enter the embossing machine together, the layers of the battery film blank are compacted under the tape casting hot-pressing effect of the embossing machine hot-pressing forming roller group. And vacuumizing the vacuum forming roller, wherein one side attached to the vacuum forming roller is subjected to dual functions of extrusion force and vacuum suction force, and after tape casting hot pressing of a stamping machine, the groove structure of the vacuum forming roller is reversely copied into a battery membrane blank, so that the interlocking type all-solid-state lithium ion battery membrane blank is prepared. As shown in FIG. 3, the grooves on the surface of the vacuum forming roll are designed in the shape of regular hexagons in this embodiment.
The forming method of the interlocking type all-solid-state lithium ion battery membrane blank realized by the device comprises the following steps: as shown in fig. 2, a co-extrusion method is firstly adopted to extrude and form the positive active layer, the polymer solid electrolyte membrane and the negative active layer together to form a primary membrane blank 11; and then compounding a positive current collector 1 on one side of the positive active layer, compounding a negative current collector 5 on one side of the negative active layer, and performing tape casting hot press molding by using an imprinter to ensure that the positive current collector, the primary film blank and the negative current collector form a groove-shaped or convex integral interlocking structure while compounding.
In the above molding method, the polymer solid electrolyte membrane is melt-extruded, the positive electrode active layer is melt-extruded or solution-extruded, and the negative electrode active layer is melt-extruded or solution-extruded during co-extrusion molding. When the positive active layer adopts a solution extrusion mode, the positive current collector adopts an aluminum foil with a porous structure; when the negative active layer adopts a solution extrusion mode, the negative current collector adopts copper foil with a porous structure.
The polymer solid electrolyte membrane is formed by adopting a melt extrusion mode, and has the advantages of short production period, flat and smooth surface of the electrolyte membrane, no gap generated by solvent volatilization, environmental friendliness and the like. In the co-extrusion process of the positive active layer and the negative active layer, a very good interface bonding effect can be achieved by adopting a melt extrusion mode; when the solution extrusion mode is adopted, the content of the adhesive can be effectively reduced, and the content of the active material and the conductive agent in the positive active layer and the negative active layer is improved, so that the performances of the positive pole piece and the negative pole piece are improved.
Meanwhile, in the forming method, the casting hot-press forming is carried out immediately after the co-extrusion is finished, at the moment, the polymer solid electrolyte membrane is in a molten state, the positive electrode active layer and the negative electrode active layer are in a slurry state or a molten state, and the material in the state can ensure a good interface contact effect through casting hot-press.
Example 3
Compared with the embodiment 2, the forming method and the forming device of the interlocking type all-solid-state lithium ion battery membrane blank have the following differences: as shown in fig. 4, a vacuum drying oven 18 is further arranged between the stamping press and the collecting roller, the interlocking type full-solid-state lithium ion battery membrane blank has a three-dimensional interlocking structure after being formed, and is further dried by the vacuum drying oven and then collected. The forming device is more suitable for forming the positive active layer and the negative active layer in a solution extrusion mode. Wherein, each extruder, the multilayer co-extrusion die head, other components of the embossing press except the vacuum forming roller, the vacuum drying box and the like can all use the traditional corresponding devices.
Example 4
The embodiment of the invention discloses a method and a device for forming an interlocking type all-solid-state lithium ion battery membrane blank, which are suitable for processing and forming a polymer solid electrolyte membrane and a positive pole piece together, and then processing and attaching a negative pole piece subsequently.
As shown in fig. 5, the forming device of the interlocking type all-solid-state lithium ion battery membrane blank comprises a first extruder 7, a third extruder 9, a multilayer co-extrusion die head 10, a positive current collector sleeve 13 and an embossing press, wherein the machine head of the first extruder and the machine head of the third extruder are connected with the multilayer co-extrusion die head together, the positive current collector sleeve is arranged on the outer side of the multilayer co-extrusion die head, and a primary membrane blank formed by the multilayer co-extrusion die head and a positive current collector from the positive current collector sleeve enter the embossing press together; a plurality of grooves are distributed on the surface of a vacuum forming roller in the stamping machine.
Be equipped with hot briquetting roller set in the coining press, including matched with vacuum forming roller and supplementary shaping roller, the surface of supplementary shaping roller is the smooth surface or distributes and has a plurality of archs with vacuum forming roller surface recess matched with, and in this embodiment, supplementary shaping roller adopts the surface to be the structure of smooth surface. In addition, the two sides of the vacuum forming roller are respectively provided with the auxiliary forming rollers, so that the bonding time between the primary film blank and the anode and cathode current collectors can be effectively prolonged, and the bonding effect is further ensured. And rolling the lithium ion battery membrane blank formed after the lamination by using a collecting roller.
A plurality of through holes are also distributed in the groove on the surface of the vacuum forming roller, and each through hole is externally connected with a vacuumizing mechanism through a flow passage in the vacuum forming roller. The flow channel design in the vacuum forming roller is the same as or similar to that of the existing vacuum roller. When the vacuum forming roller is vacuumized, the film blank close to the vacuum forming roller can be tightly attached to the vacuum forming roller under the dual actions of extrusion force and vacuum suction force, so that the structure on the surface of the vacuum forming roller is embossed and copied.
According to the actual requirement of the lithium ion battery, the grooves on the surface of the vacuum forming roller can be designed into various shapes such as hexagon, quadrangle, circle, honeycomb and the like. When a primary film blank formed by the multilayer co-extrusion die head, a positive current collector from the positive current collector sleeve and a negative current collector from the negative current collector sleeve enter the embossing machine together, the layers of the battery film blank are compacted under the tape casting hot-pressing effect of the embossing machine hot-pressing forming roller group. And vacuumizing the vacuum forming roller, wherein one side attached to the vacuum forming roller is subjected to dual functions of extrusion force and vacuum suction force, and after tape casting hot pressing of a stamping machine, the groove structure of the vacuum forming roller is reversely copied into a battery membrane blank, so that the interlocking type all-solid-state lithium ion battery membrane blank is prepared. The grooves on the surface of the vacuum forming roller in the embodiment are also designed into a regular hexagon shape.
The forming method of the interlocking type all-solid-state lithium ion battery membrane blank realized by the device comprises the following steps: firstly, co-extruding the polymer solid electrolyte membrane and the positive active layer to form a primary membrane blank; and compounding a positive current collector on one side of the positive active layer, and performing tape casting hot-press molding by using an imprinter to ensure that the primary film blank and the positive current collector form a groove-shaped or convex integral interlocking structure while being compounded.
After the lithium ion battery membrane blank is formed, compounding a negative pole piece on one side of the polymer solid electrolyte membrane by using a glove box (the step can be carried out by adopting a traditional process); and the positive active layer and the positive current collector positioned on the other side of the polymer solid electrolyte membrane form a positive pole piece.
In the above molding method, the polymer solid electrolyte membrane is melt-extruded and the positive electrode active layer is melt-extruded or solution-extruded during co-extrusion molding. When the positive active layer adopts a solution extrusion mode, the positive current collector adopts an aluminum foil with a porous structure.
Example 5
Compared with the embodiment 4, the forming method and the forming device of the interlocking type all-solid-state lithium ion battery membrane blank have the following differences: as shown in fig. 6, a vacuum drying oven 18 is further arranged between the stamping press and the collecting roller, the interlocking type full-solid-state lithium ion battery membrane blank has a three-dimensional interlocking structure after being formed, and is further dried by the vacuum drying oven and then collected. The forming device is more suitable for forming the positive active layer in a solution extrusion mode. Wherein, each extruder, the multilayer co-extrusion die head, other components of the embossing press except the vacuum forming roller, the vacuum drying box and the like can all use the traditional corresponding devices.
As mentioned above, the present invention can be better realized, and the above embodiments are only preferred embodiments of the present invention, and are not intended to limit the scope of the present invention; all equivalent changes and modifications made according to the present disclosure are intended to be covered by the scope of the claims of the present invention.
Claims (16)
1. The interlocking type full-solid-state lithium ion battery membrane blank is characterized by being of an integral multi-layer structure with an integral interlocking structure and comprising a positive pole piece and a polymer solid electrolyte membrane which are connected; the integral interlocking structure is a groove-shaped or bulge-shaped embedded structure with overlapped multilayer structures.
2. The interlocking type all-solid-state lithium ion battery membrane blank according to claim 1, wherein the lithium ion battery further comprises a negative electrode plate, and the positive electrode plate, the polymer solid electrolyte membrane and the negative electrode plate are sequentially connected to form an integral interlocking structure.
3. The interlocked type all-solid-state lithium ion battery membrane blank according to claim 2, wherein the positive electrode piece comprises a positive electrode current collector and a positive electrode active layer, the positive electrode active layer is arranged between the polymer solid electrolyte membrane and the positive electrode current collector, and the positive electrode active layer and the polymer solid electrolyte membrane are extruded together to form an integral structure.
4. The interlocked type all-solid-state lithium ion battery membrane blank according to claim 3, wherein the negative electrode plate comprises a negative electrode current collector and a negative electrode active layer, the negative electrode active layer is arranged between the polymer solid electrolyte membrane and the negative electrode current collector, and the positive electrode active layer, the polymer solid electrolyte membrane and the negative electrode active layer are extruded together to form an integral structure.
5. The interlocking type all-solid-state lithium ion battery membrane blank according to claim 4, wherein the positive electrode current collector is an aluminum foil layer, and the negative electrode current collector is a copper foil layer or a lithium metal layer.
6. The forming method of the interlocking type full-solid-state lithium ion battery membrane blank is characterized in that a co-extrusion mode is adopted to extrude and form a polymer solid electrolyte membrane and a positive active layer together to form a primary membrane blank; and compounding a positive current collector on one side of the positive active layer, and performing tape casting hot-press molding by using an imprinter to ensure that the primary film blank and the positive current collector form a groove-shaped or convex integral interlocking structure while being compounded.
7. The forming method of the interlocked type all-solid-state lithium ion battery membrane blank according to claim 6, wherein after the lithium ion battery membrane blank is formed, a glove box is adopted to compound a negative electrode plate on one side of the polymer solid electrolyte membrane; and the positive active layer and the positive current collector positioned on the other side of the polymer solid electrolyte membrane form a positive pole piece.
8. The method for forming the interlocked type all-solid-state lithium ion battery membrane blank according to claim 6, wherein the polymer solid electrolyte membrane is melt-extruded and the positive electrode active layer is melt-extruded or solution-extruded during the co-extrusion.
9. The method for forming the interlocked type all-solid-state lithium ion battery membrane blank according to claim 8, wherein when the positive electrode active layer is formed by solution extrusion, an aluminum foil with a porous structure is adopted as a positive electrode current collector.
10. The forming method of the interlocking type full-solid-state lithium ion battery membrane blank is characterized in that a co-extrusion mode is adopted to jointly extrude and form the positive active layer, the polymer solid electrolyte membrane and the negative active layer to form a primary membrane blank; and compounding a positive current collector on one side of the positive active layer, compounding a negative current collector on one side of the negative active layer, and performing tape casting hot press molding by using an imprinter to ensure that the positive current collector, the primary film blank and the negative current collector form a groove-shaped or convex integral interlocking structure while compounding.
11. The method for forming the interlocked type all-solid-state lithium ion battery membrane blank according to claim 10, wherein the polymer solid electrolyte membrane is melt-extruded, the positive electrode active layer is melt-extruded or solution-extruded, and the negative electrode active layer is melt-extruded or solution-extruded during the co-extrusion.
12. The method for forming the interlocked type all-solid-state lithium ion battery membrane blank according to claim 11, wherein when the positive electrode active layer is formed by solution extrusion, an aluminum foil with a porous structure is adopted as a positive electrode current collector; when the negative active layer adopts a solution extrusion mode, the negative current collector adopts copper foil with a porous structure.
13. The forming device of the interlocking type full-solid lithium ion battery membrane blank is characterized by comprising a first extruder, a third extruder, a multilayer co-extrusion die head, a positive current collector sleeve and a stamping press, wherein the machine head of the first extruder and the machine head of the third extruder are connected with the multilayer co-extrusion die head together, the positive current collector sleeve is arranged on the outer side of the multilayer co-extrusion die head, and a primary membrane blank formed by the multilayer co-extrusion die head and a positive current collector from the positive current collector sleeve enter the stamping press together; a plurality of grooves are distributed on the surface of a vacuum forming roller in the stamping machine.
14. The forming device of the interlocking type full-solid lithium ion battery membrane blank is characterized by comprising a first extruder, a second extruder, a third extruder, a multilayer co-extrusion die head, a positive current collector sleeve, a negative current collector sleeve and a stamping press, wherein the machine head of the first extruder, the machine head of the second extruder and the machine head of the third extruder are connected with the multilayer co-extrusion die head together, the positive current collector sleeve and the negative current collector sleeve are respectively arranged on the outer sides of the multilayer co-extrusion die head, and a primary membrane blank formed by the multilayer co-extrusion die head, a positive current collector from the positive current collector sleeve and a negative current collector from the negative current collector sleeve enter the stamping press together; a plurality of grooves are distributed on the surface of a vacuum forming roller in the stamping machine.
15. The forming device of the interlocked type all-solid-state lithium ion battery membrane blank according to claim 13 or 14, wherein the stamping press is provided with a hot press forming roller set, which comprises a vacuum forming roller and an auxiliary forming roller which are matched with each other, and the surface of the auxiliary forming roller is smooth or is distributed with a plurality of protrusions matched with the grooves on the surface of the vacuum forming roller.
16. The forming device of the interlocked type all-solid-state lithium ion battery membrane blank according to claim 13 or 14, wherein a plurality of through holes are further distributed in the groove on the surface of the vacuum forming roller, and each through hole is externally connected with a vacuum pumping mechanism through a flow channel inside the vacuum forming roller.
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