CN111370756A - High-voltage solid-state lithium battery and preparation method thereof - Google Patents
High-voltage solid-state lithium battery and preparation method thereof Download PDFInfo
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- 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
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- H01M10/00—Secondary cells; Manufacture thereof
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- H01M10/0427—Button cells
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- H—ELECTRICITY
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- 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
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M10/058—Construction or manufacture
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
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- Y02E60/10—Energy storage using batteries
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Abstract
The invention discloses a high-voltage solid-state lithium battery and a preparation method thereof. The high-voltage solid-state lithium battery comprises a plurality of battery units which are sequentially stacked and connected in series, can solve the problem of an electrode/electrolyte interface in the solid-state battery, and can greatly improve the safety of the battery. The preparation process of the high-voltage solid-state lithium battery is simple and easy to implement, can simply prepare high-voltage and high-safety solid-state button batteries in batch, and has good industrial application prospect.
Description
Technical Field
The invention belongs to the technical field of electrochemistry, and particularly relates to a high-voltage solid-state lithium battery and a preparation method thereof.
Background
With the large use and continuous depletion of fossil fuels, the development and effective utilization of green renewable energy sources and environmental protection become global common concerns. The development of secondary batteries capable of realizing efficient energy storage and conversion is not only related to national economic development and strategic safety, but also closely related to the life of people, and thus has received wide attention at home and abroad.
Lithium ion secondary batteries have been widely used in consumer electronics because of their high energy density, long cycle life, low self-discharge, no memory effect, wide operating temperature, and low cost. Conventional liquid batteries face serious safety problems due to electrolyte leakage, combustion, even explosion, etc. The solid-state battery based on the solid electrolyte greatly improves the safety problem of the battery, and the button type lithium battery is small, exquisite and portable, is convenient for circuit integration, and has wide application in portable electronic products. However, the output voltage of button cell is 1.5 and 3V, and the low output voltage greatly limits its application range. Therefore, how to improve the output voltage and the use safety of the button cell through a simple process, and further realize the industrialization of the high-voltage button cell faces a great challenge.
Disclosure of Invention
The invention aims to provide a high-voltage solid-state lithium battery and a preparation method thereof, which can solve the problem of an electrode/electrolyte interface in the solid-state battery and greatly improve the safety of the battery.
To this end, the present invention provides a high-voltage solid-state lithium battery including a battery case and a plurality of battery cells enclosed in the battery case, the plurality of battery cells being stacked in series in sequence, the battery cells including a solid electrolyte, a positive electrode tab, and a negative electrode tab.
Preferably, the high-voltage solid-state lithium battery is a button-type lithium battery, and the output voltage of the high-voltage solid-state lithium battery is greater than 3V; the battery case is one of 2016, 2025 and 2032 type button battery cases.
Preferably, the solid electrolyte comprises a polymer matrix, a lithium salt and a filler, and the mass ratio of the polymer matrix to the lithium salt to the filler is (10-20): (5-10): (0-0.1).
Preferably, the polymer matrix is one of polyethylene oxide (PEO), polyvinylidene fluoride (PVDF), polymethyl ethylene carbonate (PPC), and Polyacrylonitrile (PAN); the lithium salt is one of lithium (Li) -containing inorganic salts; the filler includes a sulfide solid electrolyte or an oxide solid electrolyte.
Preferably, the positive plate material comprises a lithium battery positive electrode material, a binder and an electronic conductive agent, and the mass ratio of the lithium battery positive electrode material to the binder to the electronic conductive agent is (70-90): (15-5): (15-5).
Preferably, the lithium battery positive electrode material is one of lithium iron phosphate (LFP), lithium manganese iron phosphate (LFMP), Lithium Cobaltate (LCO), Lithium Manganate (LMO) and ternary material (NCM); the binder is polyvinylidene fluoride (PVDF);
the electron conductive agent includes one of conductive carbon black (Super P), acetylene black and Ketjen black.
The invention also provides a preparation method of the high-voltage solid-state lithium battery, which comprises the following steps:
(1) uniformly dispersing the lithium battery positive electrode material, the binder and the electronic conductive agent into a first solvent to obtain positive electrode slurry; coating the positive electrode slurry on a current collector aluminum foil, and drying the positive electrode slurry to obtain a positive plate;
(2) uniformly dispersing the polymer matrix, the lithium salt and the filler into a second solvent to obtain solid electrolyte slurry, and coating the solid electrolyte slurry on the positive plate;
(3) after the solid electrolyte slurry is dried, cutting the positive plate with the solid electrolyte into a round shape for later use to obtain a positive wafer;
(4) rolling the lithium sheet onto the copper foil to serve as a negative plate;
(5) directly attaching the negative electrode sheet to the positive electrode wafer with the solid electrolyte to form an independent battery unit;
(6) sequentially stacking and connecting a plurality of battery units in series to form a series circuit; and packaging the plurality of battery units connected in series in a button battery shell to form the stacked multi-unit high-voltage solid-state lithium battery.
Preferably, in the step (1), the first solvent is one of N-methylpyrrolidone (NMP) and Dimethylformamide (DMF), the drying temperature is 60-120 ℃, and the drying time is 12-48 h.
Preferably, in the step (2), the second solvent is one of N-methylpyrrolidone (NMP), Dimethylformamide (DMF) and Acetonitrile (ACN).
Preferably, in the step (3), the drying temperature is 60-80 ℃, the drying time is 24-48h, and the diameter of the anode wafer is 8-19 mm; in the step (4), the thickness of the lithium sheet is 50-1000 μm.
Compared with the prior art, the invention has the advantages and positive effects that: the invention provides a high-voltage solid-state lithium battery and a preparation method thereof. The high-voltage solid-state lithium battery comprises a plurality of battery units which are sequentially stacked and connected in series, can solve the problem of an electrode/electrolyte interface in the solid-state battery, and can greatly improve the safety of the battery. The preparation process of the high-voltage solid-state lithium battery is simple and easy to implement, can simply prepare high-voltage and high-safety solid-state button batteries in batch, and has good industrial application prospect.
Other features and advantages of the present invention will become more apparent from the following detailed description of the invention when taken in conjunction with the accompanying drawings.
Drawings
Fig. 1 is a charge and discharge curve of a high voltage solid state lithium battery of example 1 of the present invention.
Detailed Description
The following detailed description of specific embodiments of the present invention is provided to illustrate and explain the present invention and to be understood not to limit the present invention.
The high-voltage solid lithium battery comprises a battery shell and a plurality of battery units encapsulated in the battery shell, wherein the battery units are sequentially stacked and connected in series, and each battery unit comprises a solid electrolyte, a positive plate and a negative plate. The high-voltage solid-state lithium battery comprises a plurality of battery units which are sequentially stacked and connected in series, can solve the problem of an electrode/electrolyte interface in the solid-state battery, and can greatly improve the safety of the battery. The preparation process of the high-voltage solid-state lithium battery is simple and easy to implement, can simply prepare high-voltage and high-safety solid-state button batteries in batch, and has good industrial application prospect.
The high-voltage solid-state lithium battery is a button type lithium battery, and the output voltage of the high-voltage solid-state lithium battery is more than 3V; the battery case is one of 2016, 2025 and 2032 type button battery cases.
The solid electrolyte comprises a polymer matrix, lithium salt and a filler, wherein the polymer matrix and the lithium salt form the polymer solid electrolyte, and the filler and the polymer matrix can play a synergistic role and can further improve the ionic conductivity and the mechanical strength of the solid electrolyte. The mass ratio of the polymer matrix, the lithium salt and the filler is (10-20): (5-10): (0-0.1), the solid electrolyte has excellent ionic conductivity and mechanical strength under the condition of the mass ratio; if the lithium salt is too little, the prepared electrolyte has low ionic conductivity; if the amount of the lithium salt is too large, the ionic conductivity is high, but the viscosity of the electrolyte is remarkably increased, the electrolyte is easy to flow, and the mechanical strength is poor; if the amount of the filler is too small, the ionic conductivity of the prepared electrolyte is reduced, and the battery capacity is not favorably exerted; the mechanical strength is low, and lithium dendrite is easy to penetrate through to cause short circuit; if the amount of the filler is too large, the mechanical strength is improved, but the ionic conductivity is remarkably reduced.
The polymer matrix is one of polyethylene oxide (PEO), polyvinylidene fluoride (PVDF), polymethyl ethylene carbonate (PPC) and Polyacrylonitrile (PAN); the lithium salt is one of lithium (Li) -containing inorganic salts; the filler includes a sulfide solid electrolyte or an oxide solid electrolyte, such as Lithium Lanthanum Zirconium Oxide (LLZO), Lithium Lanthanum Titanium Oxide (LLTO), or lithium titanium aluminum phosphate (LATP). The pure polymer electrolyte has low ionic conductivity and low mechanical strength; after inorganic solid electrolyte filler (the inorganic filler is powder and is dissolved in a solvent together with lithium salt and high polymer to prepare electrolyte slurry) is added, the filler and the high polymer matrix can play a synergistic role, and the ionic conductivity and the mechanical strength of the solid electrolyte are further improved.
The positive plate material comprises a lithium battery positive electrode material, a binder and an electronic conductive agent, wherein the mass ratio of the lithium battery positive electrode material to the binder to the electronic conductive agent is (70-90): (15-5): (15-5). The binder can ensure that the positive electrode material of the lithium battery is bonded with the electronic conductive agent, and the electronic conductive agent can improve the electronic conductivity of the positive electrode plate.
The lithium battery positive electrode material comprises one of lithium iron phosphate (LFP), lithium manganese iron phosphate (LFMP), Lithium Cobaltate (LCO), Lithium Manganate (LMO) and ternary material (NCM); the binder is polyvinylidene fluoride (PVDF); the electronic conductive agent includes one of conductive carbon black (Super P), acetylene black and Ketjen black.
The preparation method of the high-voltage solid-state lithium battery comprises the following steps:
(1) uniformly dispersing the lithium battery positive electrode material, the binder and the electronic conductive agent into a first solvent to obtain positive electrode slurry; coating the positive electrode slurry on a current collector aluminum foil, and drying the positive electrode slurry to obtain a positive plate; the drying temperature is 60-120 ℃, and the drying time is 12-48 h; the first solvent is one of N-methylpyrrolidone (NMP) and Dimethylformamide (DMF);
(2) uniformly dispersing the polymer matrix, the lithium salt and the filler into a second solvent to obtain solid electrolyte slurry, and coating the solid electrolyte slurry on the positive plate; the second solvent is one of N-methylpyrrolidone (NMP), Dimethylformamide (DMF) and Acetonitrile (ACN);
(3) after the solid electrolyte slurry is dried, cutting the positive plate with the solid electrolyte into a round shape for later use to obtain a positive wafer with the diameter of 8-19 mm; the drying temperature is 60-80 ℃, and the drying time is 24-48 h;
(4) rolling a lithium sheet with the thickness of 50-1000 mu m onto the copper foil to serve as a negative plate;
(5) directly attaching the negative electrode sheet to the positive electrode wafer with the solid electrolyte to form an independent battery unit;
(6) sequentially stacking and connecting a plurality of battery units in series to form a series circuit; and packaging the plurality of battery units connected in series in a button battery shell to form the stacked multi-unit high-voltage solid-state lithium battery.
Example 1
The method for preparing the high-voltage solid-state lithium battery of the embodiment comprises the following steps:
(1) uniformly dispersing 0.8g of LFP positive electrode powder, 0.1g of PVDF binder and 0.1g of Super P electronic conductive agent in an NMP solvent, and magnetically stirring for 6 hours to obtain positive electrode slurry; coating the positive electrode slurry on a current collector aluminum foil, and drying the positive electrode slurry to obtain a positive plate; the drying temperature is 60 ℃, and the drying time is 24 hours;
(2) uniformly dispersing 0.5g of PEO, 0.2g of Lithium Trifluoromethanesulfonimide (LTFSI) and 0.1g of Lithium Lanthanum Zirconium Tantalum Oxygen (LLZTO) powder into a DMF solvent, magnetically stirring for 12 hours to obtain solid electrolyte slurry, and coating the solid electrolyte slurry on a positive plate;
(3) after the solid electrolyte slurry is dried, cutting the positive plate with the solid electrolyte into a round shape for later use to obtain a positive wafer with the diameter of 16 mm; the drying temperature is 60 ℃, and the drying time is 24 hours;
(4) rolling a lithium sheet with the thickness of 100 mu m onto the copper foil to serve as a negative plate;
(5) directly attaching a negative electrode sheet to the positive electrode wafer with the solid electrolyte to form an independent battery unit;
(6) and packaging one battery unit in a 2032 type button battery case to obtain a high-voltage solid-state lithium battery with the output voltage of 3V.
Fig. 1 is a charge/discharge curve of the high-voltage solid-state lithium battery of example 1, and it can be seen from fig. 1 that the high-voltage solid-state lithium battery of example 1 can be normally charged and discharged, and has a small overpotential and high battery safety.
Example 2
The method for manufacturing the high-voltage solid-state lithium battery of this embodiment is substantially the same as that of embodiment 1, except that step (6) of this embodiment is: two battery units are sequentially stacked and connected in series, and the positive electrode of one battery unit is in contact with the negative electrode of the other battery unit to form a series circuit; and packaging the two battery units connected in series in a button battery shell to obtain the high-voltage solid-state lithium battery with the output voltage of 6V.
Example 3
The method for manufacturing the high-voltage solid-state lithium battery of this embodiment is substantially the same as that of embodiment 1, except that step (6) of this embodiment is: sequentially stacking and connecting three battery units in series, wherein the positive electrode of the first battery unit is contacted with the negative electrode of the second battery unit, and the positive electrode of the second battery unit is contacted with the positive electrode of the third battery unit to form a series circuit; and packaging the three battery units connected in series in a button battery shell to obtain the high-voltage solid-state lithium battery with the output voltage of 9V.
The above examples are only intended to illustrate the technical solution of the present invention, but not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be apparent to those skilled in the art that various changes may be made and equivalents may be substituted for elements thereof; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions.
Claims (10)
1. A high voltage solid state lithium battery is characterized in that,
the high-voltage solid lithium battery comprises a battery shell and a plurality of battery units packaged in the battery shell, wherein the battery units are sequentially stacked and connected in series, and each battery unit comprises a solid electrolyte, a positive plate and a negative plate.
2. A high voltage lithium solid state battery according to claim 1,
the high-voltage solid-state lithium battery is a button type lithium battery, and the output voltage of the high-voltage solid-state lithium battery is more than 3V;
the battery case is one of 2016, 2025 and 2032 type button battery cases.
3. A high voltage lithium solid state battery according to claim 1,
the solid electrolyte comprises a polymer matrix, lithium salt and a filler,
the mass ratio of the polymer matrix to the lithium salt to the filler is (10-20): (5-10): (0-0.1).
4. A high voltage lithium solid state battery according to claim 3,
the polymer matrix is one of polyethylene oxide (PEO), polyvinylidene fluoride (PVDF), polymethyl ethylene carbonate (PPC) and Polyacrylonitrile (PAN);
the lithium salt is one of lithium (Li) -containing inorganic salts;
the filler includes a sulfide solid electrolyte or an oxide solid electrolyte.
5. A high voltage lithium solid state battery according to claim 1,
the positive plate material comprises a lithium battery positive electrode material, a binder and an electronic conductive agent,
the mass ratio of the lithium battery positive electrode material to the binder to the electronic conductive agent is (70-90): (15-5): (15-5).
6. A high voltage lithium solid state battery according to claim 5,
the lithium battery positive electrode material is one of lithium iron phosphate (LFP), lithium manganese phosphate (LFMP), Lithium Cobaltate (LCO), Lithium Manganate (LMO) and ternary material (NCM);
the binder is polyvinylidene fluoride (PVDF);
the electron conductive agent includes one of conductive carbon black (Super P), acetylene black and Ketjen black.
7. A method of manufacturing a high voltage solid state lithium battery as claimed in any one of claims 1 to 6,
the method comprises the following steps:
(1) uniformly dispersing the lithium battery positive electrode material, the binder and the electronic conductive agent into a first solvent to obtain positive electrode slurry; coating the positive electrode slurry on a current collector aluminum foil, and drying the positive electrode slurry to obtain a positive plate;
(2) uniformly dispersing the polymer matrix, the lithium salt and the filler into a second solvent to obtain solid electrolyte slurry, and coating the solid electrolyte slurry on the positive plate;
(3) after the solid electrolyte slurry is dried, cutting the positive plate with the solid electrolyte into a round shape for later use to obtain a positive wafer;
(4) rolling the lithium sheet onto the copper foil to serve as a negative plate;
(5) directly attaching the negative electrode sheet to the positive electrode wafer with the solid electrolyte to form an independent battery unit;
(6) sequentially stacking and connecting a plurality of battery units in series to form a series circuit; and packaging the plurality of battery units connected in series in a button battery shell to form the stacked multi-unit high-voltage solid-state lithium battery.
8. The method of manufacturing a high voltage solid lithium battery according to claim 7,
in the step (1), the first solvent is one of N-methylpyrrolidone (NMP) and Dimethylformamide (DMF),
the drying temperature is 60-120 ℃, and the drying time is 12-48 h.
9. The method of manufacturing a high voltage solid lithium battery according to claim 7,
in the step (2), the second solvent is one of N-methylpyrrolidone (NMP), Dimethylformamide (DMF) and Acetonitrile (ACN).
10. The method of manufacturing a high voltage solid lithium battery according to claim 7,
in the step (3), the drying temperature is 60-80 ℃, the drying time is 24-48h, and the diameter of the anode wafer is 8-19 mm;
in the step (4), the thickness of the lithium sheet is 50-1000 μm.
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| CN113258127A (en) * | 2021-05-31 | 2021-08-13 | 浙江大学 | Current collector-negative electrode integrated bipolar lithium secondary battery and method thereof |
| CN113258127B (en) * | 2021-05-31 | 2023-09-15 | 浙江大学 | Current collector-negative electrode integrated bipolar lithium secondary battery and method thereof |
| WO2023047064A1 (en) * | 2021-09-27 | 2023-03-30 | Arkema France | Cathode coating for li-ion battery |
| FR3127635A1 (en) * | 2021-09-27 | 2023-03-31 | Arkema France | CATHODE COATING FOR LI-ION BATTERY |
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