CN116936938B - 3D printing continuous carbon fiber solid-state battery and preparation method thereof - Google Patents

3D printing continuous carbon fiber solid-state battery and preparation method thereof Download PDF

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CN116936938B
CN116936938B CN202310946011.8A CN202310946011A CN116936938B CN 116936938 B CN116936938 B CN 116936938B CN 202310946011 A CN202310946011 A CN 202310946011A CN 116936938 B CN116936938 B CN 116936938B
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continuous carbon
carbon fiber
battery
electrode active
negative electrode
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CN116936938A (en
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侯章浩
丁浩林
石会发
杜雨森
李志豪
杨乐怡
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Qingdao University of Technology
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Qingdao University of Technology
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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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B33—ADDITIVE MANUFACTURING TECHNOLOGY
    • B33Y—ADDITIVE MANUFACTURING, i.e. MANUFACTURING OF THREE-DIMENSIONAL [3-D] OBJECTS BY ADDITIVE DEPOSITION, ADDITIVE AGGLOMERATION OR ADDITIVE LAYERING, e.g. BY 3-D PRINTING, STEREOLITHOGRAPHY OR SELECTIVE LASER SINTERING
    • B33Y10/00—Processes of additive manufacturing
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B33—ADDITIVE MANUFACTURING TECHNOLOGY
    • B33Y—ADDITIVE MANUFACTURING, i.e. MANUFACTURING OF THREE-DIMENSIONAL [3-D] OBJECTS BY ADDITIVE DEPOSITION, ADDITIVE AGGLOMERATION OR ADDITIVE LAYERING, e.g. BY 3-D PRINTING, STEREOLITHOGRAPHY OR SELECTIVE LASER SINTERING
    • B33Y70/00—Materials specially adapted for additive manufacturing
    • B33Y70/10—Composites of different types of material, e.g. mixtures of ceramics and polymers or mixtures of metals and biomaterials
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B33—ADDITIVE MANUFACTURING TECHNOLOGY
    • B33Y—ADDITIVE MANUFACTURING, i.e. MANUFACTURING OF THREE-DIMENSIONAL [3-D] OBJECTS BY ADDITIVE DEPOSITION, ADDITIVE AGGLOMERATION OR ADDITIVE LAYERING, e.g. BY 3-D PRINTING, STEREOLITHOGRAPHY OR SELECTIVE LASER SINTERING
    • B33Y80/00—Products made by additive manufacturing
    • 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
    • H01M10/056—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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H01M4/1391—Processes of manufacture of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
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    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Abstract

The invention belongs to the technical field of solid-state batteries, and relates to a 3D printing continuous carbon fiber solid-state battery and a preparation method thereof. The positive and negative current collectors of the continuous carbon fiber solid-state battery are all continuous carbon fibers, and the continuous carbon fibers are impregnated through a presoaking device, so that positive active substances and negative active substances are respectively adhered to the surfaces of the continuous carbon fibers corresponding to the positive and negative electrodes; twisting by a twisting device, and fixing the positive electrode active material and the negative electrode active material to form a positive electrode and a negative electrode of the battery; the outer surfaces of the anode and the cathode of the battery are wrapped by solid electrolyte; the continuous carbon fiber solid-state battery adopts a manufacturing mode of stacking layers by 3D printing. The continuous carbon fiber solid-state battery developed by the invention can customize the shape according to the requirement, realizes individuation and high performance of the battery, is beneficial to reducing the weight of equipment in the fields of carrying and the like, has low production cost and has wide application prospect.

Description

3D printing continuous carbon fiber solid-state battery and preparation method thereof
Technical Field
The invention belongs to the technical field of solid-state batteries, and relates to a 3D printing continuous carbon fiber solid-state battery and a preparation method thereof.
Background
The traditional lithium ion battery has the advantages of higher energy density and power density, high working voltage, long cycle life, capability of rapid charge and discharge and the like, and is widely applied to the fields of aerospace, electric vehicles, portable electronic equipment and the like. However, conventional lithium ion batteries are bulky and heavy, and the device requires a large storage space to be reserved. Furthermore, the liquid electrolyte used is at risk of thermal runaway explosion. In the global environment trend of low carbon economy, there is a need for a more efficient, lightweight, safe, green and environmentally friendly battery. Unlike the liquid ion battery generally used today, the solid-state battery is a battery using an ion-conductive solid-state material as an electrolyte, and can greatly improve the safety index and energy density of the battery. The continuous carbon fiber has the advantages of light weight and high strength, and the structural performance of the solid-state battery can be greatly improved when the continuous carbon fiber is used in the solid-state battery, so that the continuous carbon fiber solid-state battery can meet the requirements of high performance, multifunctional integration and light weight in the fields of aerospace and the like, and has wide application prospects.
The 3D printing technology, also called additive manufacturing technology, is used for directly manufacturing the three-dimensional entity which accords with the actual situation according to 3D model data by adding materials and manufacturing layer by layer. Compared with the traditional material removal-cutting processing technology, the method is a 'bottom-up' manufacturing method, and the 3D printing technology has been rapidly developed in the last twenty years. The 3D printing technology does not need traditional cutters, clamps and a plurality of processing procedures, and parts with any complex shape can be rapidly and precisely manufactured on one device, so that the free manufacturing of the parts is realized, the forming of a plurality of parts with complex structures is solved, the processing procedures are greatly reduced, and the processing period is shortened; 3D printing provides a new direction for integrated, low cost, short cycle manufacturing of continuous carbon fiber solid state batteries.
However, existing 3D printing devices lack complete electrical polarization of continuous carbon fibersThe equipment can not manufacture continuous carbon fiber solid-state batteries, and most of the existing spray heads are single fiber channels and can not print positive and negative electrodes at the same time 。 And no technology can replace 3D printing to manufacture continuous carbon fiber solid-state batteries so as to tightly combine the anode and the cathode with electrolyte. Therefore, development of a new 3D printing method is required to prepare a continuous carbon fiber solid state battery.
Disclosure of Invention
Aiming at the technical problems, the invention provides a 3D printing continuous carbon fiber solid-state battery and a preparation method thereof; the high performance of the battery is realized, the weight of equipment in the fields of carrying and the like is reduced, the production cost is low, and the battery has wide application prospect.
The invention is realized by the following technical scheme:
A3D printing continuous carbon fiber solid-state battery is characterized in that a battery anode and a battery cathode current collector of the continuous carbon fiber solid-state battery are both continuous carbon fibers,
the continuous carbon fibers are impregnated through a presoaking device, so that positive electrode active substances and negative electrode active substances are respectively adhered to the surfaces of the continuous carbon fibers corresponding to the positive electrode and the negative electrode; twisting by a twisting device, and fixing the positive electrode active material and the negative electrode active material to form a battery positive electrode and a battery negative electrode;
the outer surfaces of the anode and the cathode of the battery are wrapped by solid electrolyte;
the continuous carbon fiber solid-state battery adopts a manufacturing mode of stacking layers by 3D printing. The manufacturing method can finally integrally manufacture the battery with the complex structure. The continuous carbon fiber solid-state battery developed by the invention can customize the shape according to the requirement, realizes individuation and high performance of the battery, is beneficial to reducing the weight of equipment in the fields of carrying and the like, has low production cost and has wide application prospect.
Further, the positive electrode active material includes: potassium manganate, potassium cobaltate; the negative electrode active material includes: graphite, lithium titanate; the solid electrolyte material includes: polycarbonate, polyurethane.
Further, the battery anode and the battery cathode are arranged in parallel, so that the contact between the anode and the cathode can be effectively avoided, and the short circuit is prevented.
A method of preparing a 3D printed continuous carbon fiber solid state battery, the method comprising the steps of:
s1: respectively placing the positive electrode and the negative electrode on two fiber reels by using continuous carbon fibers; respectively injecting a positive electrode active material and a negative electrode active material into two impregnating devices, and adding a solid electrolyte material into an extruding device;
s2: setting a printing path and printing parameters of a 3D printer; in the step S2, a complete object is finally constructed by setting a 3D printing path and parameters and adopting a layer-by-layer stacking manufacturing mode; this layer-by-layer fabrication process enables 3D printing to print cells of almost any shape, conventional techniques being omitted here.
S3: the end parts of the continuous carbon fiber dry tows on the two fiber reels are respectively pulled out from the two fiber reels, sequentially pass through the impregnating device, the air drying device and the twisting device and reach the two fiber pipelines of the printing spray head;
s4: simultaneously pulling two bundles of continuous carbon fiber dry tows according to a set pulling speed; two bundles of continuous carbon fiber dry tows are impregnated by an impregnating device, then are dried by an electrode active substance acceleration dryer by a heating air dryer in an air drying device, and are twisted by a twisting device, and the two bundles of continuous carbon fiber dry tows are arranged in parallel and enter two fiber pipelines of a printing spray head;
s5: the extrusion device provides solid electrolyte materials for the printing spray head, and the printing spray head extrudes a battery anode and a battery cathode which are fully coated by the solid electrolyte materials;
s6: and printing according to the set printing parameters by the 3D printer to obtain the continuous carbon fiber battery extruded by the nozzle.
Further, the method further comprises step S7: and (5) using a cooling device to accelerate cooling, and gradually solidifying the continuous carbon fiber battery.
Further, the method further comprises step S8: and packaging the cooled continuous carbon fiber solid-state battery in a soft package mode.
Further, the printing speed is adjusted by adjusting the pulling speed of the continuous carbon fiber dry tow in step S4.
Further, the number of the impregnating devices is two, and the two impregnating devices are respectively used for containing the positive electrode active material and the negative electrode active material; the continuous carbon fiber is passed through a presoaking device, so that the positive electrode active material and the negative electrode active material are respectively adhered on the surfaces of the continuous carbon fiber for the positive electrode and the negative electrode, and the positive electrode and the negative electrode of the battery are formed.
Further, the number of the air drying devices is two, and the two air drying devices are respectively used for drying positive electrode active materials and negative electrode active materials impregnated on continuous carbon fibers for the positive electrode and the negative electrode;
the twisting devices are two in number and are respectively used for twisting the air-dried positive electrode and negative electrode which are impregnated with the positive and negative electrode active substances by using the continuous carbon fibers so as to fix the positive electrode active substances and the negative electrode active substances.
Further, the number of fiber pipelines in a printing nozzle in the 3D printer is two; the two fiber pipelines are parallel to each other, so that the battery anode and the battery cathode are arranged in parallel;
the extruding device is connected with the printing nozzle, solid electrolyte material is provided for the printing nozzle, and the printing nozzle extrudes the battery anode and the battery cathode which are fully coated by the solid electrolyte material.
The beneficial technical effects of the invention are as follows:
the continuous carbon fiber solid-state battery provided by the invention adopts the continuous carbon fiber impregnated electrode active material as the electrode, the continuous carbon fiber can distribute energy storage in the whole structure of the battery, the structural member and the energy storage system are combined, the mechanical property of the continuous carbon fiber is maintained, and meanwhile, excellent energy storage performance is given, so that the structural design of the power battery pack is simplified while the weight is reduced, and the continuous carbon fiber adopts a twisting structure to fix the electrode active material, thereby improving the energy efficiency and the structural efficiency. From new energy automobiles to small unmanned aerial vehicles, from artificial satellites to electric airplanes, the continuous carbon fiber solid-state batteries can distribute energy storage in the structure, can have both structural performance and energy storage function, and have huge market prospects.
The preparation method of the 3D printing continuous carbon fiber solid-state battery provided by the invention can be used for manufacturing the continuous carbon fiber solid-state battery with complex shape and high performance, and has the advantages of good structural stability, automatic production, electrochemical performance, production stability, low production cost and short production period. The invention can manufacture the continuous carbon fiber solid-state battery with small external dimension, good structural stability and low cost.
Drawings
Fig. 1 is a schematic flow chart of a preparation method for printing a continuous carbon fiber solid-state battery according to an embodiment of the invention;
fig. 2 is a schematic top view of a print head according to an embodiment of the present invention.
Fig. 3 is a schematic cross-sectional view of a continuous carbon fiber solid state battery positive electrode and a battery negative electrode in an embodiment of the invention.
The reference numerals are: 1. a fiber reel; 2. continuous carbon fibers; 3. an impregnating device; 4. an air drying device; 5. a twisting device; 6. printing a spray head; 601. a first fiber conduit; 602. a second fiber tube; 7. an extrusion device; 8. a cooling device; 9. a positive electrode active material; 10. a negative electrode active material; 11. a solid electrolyte material; 12. a battery positive electrode; 13. and a battery negative electrode.
Detailed Description
The present invention will be described in further detail with reference to the drawings and examples, in order to make the objects, technical solutions and advantages of the present invention more apparent. It should be understood that the specific embodiments described herein are for purposes of illustration only and are not intended to limit the scope of the invention.
On the contrary, the invention is intended to cover any alternatives, modifications, equivalents, and variations as may be included within the spirit and scope of the invention as defined by the appended claims. Further, in the following detailed description of the present invention, certain specific details are set forth in order to provide a better understanding of the present invention. The present invention will be fully understood by those skilled in the art without the details described herein.
Example 1
The invention provides a 3D printing continuous carbon fiber solid state battery embodiment, wherein the 3D printing continuous carbon fiber solid state battery comprises a battery positive electrode 12 and a battery negative electrode 13 (shown in figure 3); the battery anode 12 and the battery cathode 13 current collectors of the continuous carbon fiber solid-state battery are all continuous carbon fibers, and the continuous carbon fibers are used for enhancing the structural performance of the continuous carbon fiber solid-state battery;
the continuous carbon fibers are impregnated through a presoaking device, so that positive electrode active substances and negative electrode active substances are respectively adhered to the surfaces of the continuous carbon fibers corresponding to the positive electrode and the negative electrode; then twisting by a twisting device to fix the positive electrode active material and the negative electrode active material to form a battery positive electrode 12 and a battery negative electrode 13 of the battery;
the outer surfaces of the battery anode 12 and the battery cathode 13 of the battery are wrapped by solid electrolyte;
the continuous carbon fiber solid-state battery adopts a manufacturing mode of stacking layers by 3D printing. The manufacturing method can finally integrally manufacture the battery with the complex structure. The continuous carbon fiber solid-state battery developed by the invention can customize the shape according to the requirement, realizes individuation and high performance of the battery, is beneficial to reducing the weight of equipment in the fields of carrying and the like, has low production cost and has wide application prospect.
In this embodiment, the positive electrode active material includes: potassium manganate, potassium cobaltate; the negative electrode active material includes: graphite, lithium titanate; the solid electrolyte material includes: polycarbonate, polyurethane.
In this embodiment, the positive electrode of the battery and the negative electrode of the battery are arranged in parallel, so that contact between the positive electrode and the negative electrode of the battery can be effectively avoided, and short circuit is prevented.
The positive and negative current collectors of the 3D printing continuous carbon fiber solid-state battery provided by the invention are all continuous carbon fibers, so that the structural performance of the battery can be enhanced, including the enhancement of tensile strength, high strength, impact resistance and flexibility; the continuous carbon fiber is passed through a presoaking device, so that the positive electrode active material and the negative electrode active material are respectively adhered to the surfaces of the continuous carbon fiber to form the positive electrode and the negative electrode of the battery; the outer surfaces of the positive electrode and the negative electrode are wrapped by solid electrolyte, and the positive electrode and the negative electrode have higher strength, stability and good flexibility. Compared with the solid-state battery in the prior art, the solid-state battery has higher strength and stability.
Example 2
The invention also provides a printing system for 3D printing of continuous carbon fiber solid-state batteries, as shown in fig. 1, comprising: a fiber pipeline 1, an impregnating device 3, an air drying device 4, a twisting device 5 and a 3D printer;
the number of the fiber pipelines 1 is two, and the two fiber pipelines 1 are respectively used for placing continuous carbon fibers 2 for the positive electrode and the negative electrode;
the number of the impregnating devices 3 is two, and the two impregnating devices 3 are respectively used for containing the positive electrode active material 9 and the negative electrode active material 10; the continuous carbon fiber 2 is passed through a presoaking device, and a positive electrode active material 9 and a negative electrode active material 10 are respectively adhered to the surfaces of the continuous carbon fiber for positive electrode and negative electrode to form a battery positive electrode 12 and a battery negative electrode 13;
the air drying device 4 is used for drying the electrode active substances impregnated on the continuous carbon fibers; preferably, the number of the air-drying devices 4 is two, and the two air-drying devices 4 are used for drying the positive electrode active material 9 and the negative electrode active material 10 impregnated on the continuous carbon fiber for the positive electrode and the negative electrode respectively; can accelerate the drying of the electrode active material, prevent the active material from losing, and facilitate the subsequent treatment.
The twisting device 5 is used for twisting the air-dried positive electrode and negative electrode continuous carbon fibers respectively so as to fix the positive electrode active material 9 and the negative electrode active material 10; preferably, the number of the twisting devices 5 is two, and the two twisting devices 5 are respectively used for twisting the dried continuous carbon fiber dry tows for the positive electrode and the negative electrode which are impregnated with the positive electrode active substance 10 and air-dried; the electrode active material is immobilized to avoid the active material from escaping.
The printing nozzle 6 of the 3D printer comprises two fiber pipelines, and the two fiber pipelines are parallel to each other, so that the battery anode 12 and the battery cathode 13 are arranged in parallel; the extrusion device 7 of the 3D printer is connected with the printing spray head 6, the extrusion device 7 is arranged on one side of the printing spray head, a solid electrolyte material 11 is provided for the printing spray head 6, and the solid electrolyte material 11 is used for wrapping the surfaces of the battery anode 12 and the battery cathode 13 during printing.
The printing nozzle 6 comprises two fiber pipelines, and two bundles of dry fiber tows impregnated with the positive and negative electrode active substances 10 are respectively fed into one fiber pipeline, so that positive and negative electrode contact can be effectively avoided. Specifically, two fiber pipes are arranged in parallel so that the printed battery positive electrode 12 and the battery negative electrode 13 are arranged in parallel.
Example 3
The invention also provides a preparation method of the 3D printing continuous carbon fiber solid-state battery, which comprises the following steps:
s1: respectively placing the positive electrode and the negative electrode on two fiber pipelines 1 by using continuous carbon fibers; injecting a positive electrode active material 9 and a negative electrode active material 10 into the two impregnating devices 3, respectively, and adding a solid electrolyte material 11 into the extruding device 7;
s2: setting a printing path and printing parameters of a 3D printer; in the step S2, a complete object is finally constructed by setting a 3D printing path and parameters and adopting a layer-by-layer stacking manufacturing mode; this layer-by-layer fabrication process enables 3D printing to print cells of almost any shape, conventional techniques being omitted here.
S3: the end parts of the continuous carbon fiber dry tows on the two fiber pipelines 1 are respectively pulled out from the two fiber pipelines 1, sequentially pass through the impregnating device 3, the air drying device 4 and the twisting device 5 to reach the two fiber pipelines of the printing spray head 6;
specifically, a continuous carbon fiber dry tow is pulled out of the carbon fiber pipeline 1 by a threading needle to pass through a first fiber pipeline 601 of the impregnating device 3, the air drying device 4, the twisting device 5 and the printing spray head 6 in sequence; another continuous carbon fiber dry tow is pulled from the fiber reel 1 by a threading needle to sequentially pass through the impregnating device 3, the air drying device 4, the twisting device 5 and the second fiber pipeline 602;
s4: when two bundles of carbon fiber dry tows are in place at the same time (when reaching the first fiber pipeline 601 and the second fiber pipeline 602), two bundles of continuous carbon fiber dry tows are pulled at the same time according to a set pulling speed; two bundles of continuous carbon fiber dry tows are impregnated by an impregnating device 3, then are dried by an air drying device 4 by a heating air dryer to accelerate electrode active substances, and are twisted by a twisting device 5, and the two bundles of continuous carbon fiber dry tows are arranged in parallel and enter two fiber pipelines of a printing spray head 6;
specifically, the printing speed is adjusted by adjusting the pulling speed of the continuous carbon fiber dry tow in step S4.
S5: the extrusion device 7 provides the solid electrolyte material 11 for the printing nozzle 6, and sets the feeding amount of the solid electrolyte material 11 in the nozzle, so that the printing nozzle 6 extrudes the battery anode 12 and the battery cathode 13 fully covered by the solid electrolyte material 11;
s6: and printing according to the set printing parameters by the 3D printer to obtain the continuous carbon fiber battery extruded by the nozzle.
In this embodiment, the method further includes step S7: the cooling device 8 is used for accelerating the cooling, and the continuous carbon fiber battery is gradually solidified.
In this embodiment, the method further includes step S8: and packaging the dried continuous carbon fiber solid-state battery by using a soft package battery.
Specifically, the printing speed is adjusted by adjusting the pulling speed of the continuous carbon fiber dry tow in step S4.
In this embodiment, the number of the impregnating devices 3 is two, and the two impregnating devices 3 are respectively used for containing the positive electrode active material 9 and the negative electrode active material 10; the continuous carbon fibers are passed through a prepreg device, and the positive electrode active material 9 and the negative electrode active material 10 are adhered to the surfaces of the continuous carbon fibers for positive electrode and negative electrode, respectively, to form a battery positive electrode 12 and a battery negative electrode 13.
In this embodiment, the number of the air-drying devices 4 is two, and the two air-drying devices 4 are used for drying the positive electrode active material 9 and the negative electrode active material 10 impregnated on the continuous carbon fiber for the positive electrode and the negative electrode, respectively. The air drying device 4 is used for accelerating the drying of the electrode active substances, so that the active substances are not lost, and the subsequent treatment is convenient. Specifically, both air-drying devices 4 employ a heated air dryer.
In this embodiment, the number of the twisting devices 5 is two, and the two twisting devices are used for twisting the continuous carbon fibers for positive and negative electrodes impregnated with the positive and negative electrode active materials 10 and air-dried, respectively, so as to fix the positive electrode active material 9 and the negative electrode active material 10. The twisting device 5 is used for fixing the electrode active material and avoiding the active material from escaping.
In this embodiment, the number of fiber pipes in the printing nozzle 6 in the 3D printer is two; the two fiber pipes are parallel to each other so that the battery positive electrode 12 and the battery negative electrode 13 are arranged in parallel; the printing nozzle 6 comprises two fiber pipelines, and two bundles of dry fiber tows impregnated with the positive and negative electrode active substances 10 are respectively fed into one fiber pipeline, so that positive and negative electrode contact can be effectively avoided. Specifically, two fiber pipes are arranged in parallel so that the printed battery positive electrode 12 and the battery negative electrode 13 are arranged in parallel;
the extrusion device 7 is connected with the printing spray head 6, a solid electrolyte material 11 is provided for the printing spray head 6, and the printing spray head 6 extrudes a battery positive electrode 12 and a battery negative electrode 13 which are fully covered by the solid electrolyte material 11. The 3D printing method provided by the invention can be used for manufacturing continuous carbon fiber solid-state batteries with complex shapes.
The electrode of the 3D printing continuous carbon fiber is formed by uniformly mixing electrode active substances and fibers, wherein a solid electrolyte is used, positive electrodes and negative electrodes are arranged in parallel through a fixing device, the positive electrodes and the negative electrodes are fully coated by the electrolyte, and finally the electrode is printed through a printing device; the preparation method comprises the following steps: the method comprises the steps of respectively fully impregnating two bundles of fibers with positive electrode active substances and negative electrode active substances, accelerating drying of the electrode active substances by a heating air dryer, fixing the electrode active substances by a twisting device, enabling the two bundles of fibers to be arranged in parallel and respectively enter two fiber pipelines, extruding electrolyte from the pipelines at one side of a printing spray head, fully coating the two bundles of fibers by the electrolyte, extruding a continuous carbon fiber battery by the printing spray head, and accelerating cooling of the battery by a cooling device. The continuous carbon fiber solid-state battery developed by the invention realizes high performance of the battery, is beneficial to reducing the weight of equipment in the fields of carrying and the like, has low production cost and has wide application prospect.
The foregoing description of the preferred embodiments of the invention is not intended to limit the invention to the precise form disclosed, and any such modifications, equivalents, and alternatives falling within the spirit and scope of the invention are intended to be included within the scope of the invention.

Claims (3)

1. A method for preparing a 3D printed continuous carbon fiber solid state battery, the method comprising the steps of:
s1: respectively placing the positive electrode and the negative electrode on two fiber reels by using continuous carbon fibers; respectively injecting a positive electrode active material and a negative electrode active material into two impregnating devices, and adding a solid electrolyte material into an extruding device; the solid electrolyte material includes: polycarbonate, polyurethane;
s2: setting a printing path and printing parameters of a 3D printer;
s3: the end parts of the continuous carbon fiber dry tows on the two fiber reels are respectively pulled out from the two fiber reels, sequentially pass through the impregnating device, the air drying device and the twisting device and reach the two fiber pipelines of the printing spray head;
s4: simultaneously pulling two bundles of continuous carbon fiber dry tows according to the set pulling speed, and adjusting the printing speed by adjusting the pulling speed of the continuous carbon fiber dry tows; two bundles of continuous carbon fiber dry tows are impregnated by an impregnating device, then are air-dried by an air-drying device and twisted by a twisting device, and are arranged in parallel and enter two fiber pipelines of a printing spray head; the two fiber pipelines are parallel to each other;
the air drying device adopts a heating air dryer to accelerate the drying of the electrode active substances; the two impregnating devices are respectively used for containing positive electrode active materials and negative electrode active materials; the continuous carbon fiber is used for enabling the positive electrode active material and the negative electrode active material to be respectively adhered to the surfaces of the continuous carbon fiber for the positive electrode and the negative electrode through the impregnating device, so that a battery positive electrode and a battery negative electrode are formed;
the number of the air drying devices is two, and the two air drying devices are respectively used for drying positive electrode active materials and negative electrode active materials impregnated on continuous carbon fibers for the positive electrode and the negative electrode;
the number of the twisting devices is two, and the two twisting devices are respectively used for twisting the air-dried positive electrode and negative electrode impregnated with the positive and negative electrode active substances by using continuous carbon fibers so as to fix the positive electrode active substances and the negative electrode active substances;
s5: the extrusion device is used for providing solid electrolyte materials for the printing spray head, and is connected with the printing spray head and arranged on one side of the printing spray head; extruding a battery anode and a battery cathode which are fully coated by the solid electrolyte material by a printing spray head;
s6: and the 3D printer prints and obtains the continuous carbon fiber solid-state battery extruded by the spray head according to the set printing parameters.
2. The method for manufacturing a 3D printed continuous carbon fiber solid state battery according to claim 1, further comprising step S7: and (5) using a cooling device to accelerate cooling, and gradually solidifying the continuous carbon fiber battery.
3. The method for manufacturing a 3D printed continuous carbon fiber solid state battery according to claim 2, further comprising step S8: and packaging the cooled continuous carbon fiber solid-state battery in a soft package mode.
CN202310946011.8A 2023-07-31 2023-07-31 3D printing continuous carbon fiber solid-state battery and preparation method thereof Active CN116936938B (en)

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Publication number Priority date Publication date Assignee Title
CN102473905A (en) * 2009-07-14 2012-05-23 川崎重工业株式会社 Electrical storage device provided with fiber electrodes, and method for producing same
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CN109950635A (en) * 2019-03-19 2019-06-28 西安交通大学 A kind of all solid state continuous fiber lithium ion battery structure and its 3D printing manufacturing process
CN113172853A (en) * 2021-04-16 2021-07-27 固纤(苏州)智能科技有限公司 3D prints with continuous carbon-fibre composite's dry and wet preparation facilities

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WO2019190729A1 (en) * 2018-03-29 2019-10-03 Battelle Energy Alliance, Llc Electrochemical cells comprising three-dimensional (3d) electrodes

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Publication number Priority date Publication date Assignee Title
CN102473905A (en) * 2009-07-14 2012-05-23 川崎重工业株式会社 Electrical storage device provided with fiber electrodes, and method for producing same
CN108183257A (en) * 2017-12-26 2018-06-19 深圳先进技术研究院 Organogel electrolyte, application, sodium base double ion organic solid-state battery and preparation method thereof
CN109950635A (en) * 2019-03-19 2019-06-28 西安交通大学 A kind of all solid state continuous fiber lithium ion battery structure and its 3D printing manufacturing process
CN113172853A (en) * 2021-04-16 2021-07-27 固纤(苏州)智能科技有限公司 3D prints with continuous carbon-fibre composite's dry and wet preparation facilities

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