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WO2017190367A1 - Batterie rechargeable et son procédé de préparation - Google Patents

Batterie rechargeable et son procédé de préparation Download PDF

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Publication number
WO2017190367A1
WO2017190367A1 PCT/CN2016/081349 CN2016081349W WO2017190367A1 WO 2017190367 A1 WO2017190367 A1 WO 2017190367A1 CN 2016081349 W CN2016081349 W CN 2016081349W WO 2017190367 A1 WO2017190367 A1 WO 2017190367A1
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WIPO (PCT)
Prior art keywords
battery
lithium
metal
positive electrode
secondary battery
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Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/CN2016/081349
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English (en)
Chinese (zh)
Inventor
唐永炳
季必发
张帆
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Shenzhen Institute of Advanced Technology of CAS
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Shenzhen Institute of Advanced Technology of CAS
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Priority to CN201680085080.2A priority Critical patent/CN109155433A/zh
Priority to PCT/CN2016/081349 priority patent/WO2017190367A1/fr
Publication of WO2017190367A1 publication Critical patent/WO2017190367A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
    • H01M10/0562—Solid materials
    • 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

Definitions

  • the present invention relates to the field of batteries, and in particular to a secondary battery and a method of fabricating the same.
  • a secondary battery also called a rechargeable battery, is a battery that can be repeatedly charged and discharged and used multiple times. Compared with a non-reusable primary battery, the secondary battery has the advantages of low cost of use and low environmental pollution.
  • the main secondary battery technologies are lead-acid batteries, nickel-chromium batteries, nickel-hydrogen batteries, and lithium-ion batteries. Among them, lithium ion batteries are the most widely used. Lithium-ion batteries have become the power source for electric vehicles and power tools because of their high power density, low self-discharge rate, no memory effect and stable discharge voltage.
  • the core components of a lithium ion battery usually contain a positive electrode, a negative electrode, an electrolyte, and a separator.
  • the organic electrolyte secondary battery needs to further reduce the volume, increase the specific capacity and voltage, and further reduce the thickness of the separator. Therefore, there is a need to provide a secondary battery to solve the problems of low-energy, easy-corrosion electrode materials, poor design and assembly, poor safety, low service life, and the necessity of using a separator.
  • the negative electrode of the conventional lithium ion battery must contain a negative active material and a negative current collector, wherein the negative active material occupies a large part of the volume and weight, which limits the battery capacity and energy density of the lithium ion battery.
  • the present invention provides a secondary battery and a preparation method thereof, which are intended to solve the problems of low specific energy, easy corrosion of electrode materials, poor design and assembly, poor safety, and low service life of existing liquid electrolytes. Problems such as diaphragms must be used.
  • the present invention directly solves the problem of low battery capacity and energy density by using the negative electrode current collector as the negative electrode.
  • the present invention provides a secondary battery including a battery negative electrode and a battery positive electrode; and further comprising an all-solid electrolyte layer, wherein
  • the negative electrode of the battery includes a negative current collector, and does not include a negative active material;
  • the negative current collector includes a metal, a metal alloy or a metal composite conductive material;
  • the all solid electrolyte layer includes an inorganic solid electrolyte
  • the positive electrode of the battery includes a positive current collector and a positive active material layer
  • the positive current collector includes a metal, a metal alloy or a metal composite conductive material
  • the positive active material layer includes a positive electrode capable of reversibly deintercalating lithium, sodium or magnesium ions. Active material.
  • the anode current collector comprises one of aluminum, magnesium, lithium, vanadium, copper, iron, tin, zinc, nickel, titanium, manganese or a composite of any one of them or an alloy of any one of them .
  • the anode current collector is aluminum.
  • the structure of the anode current collector is a multi-layer composite structure of porous aluminum or aluminum coated with aluminum foil or porous aluminum or carbon material.
  • the cathode current collector comprises one of aluminum, magnesium, lithium, vanadium, copper, iron, tin, zinc, nickel, titanium, manganese or a composite of any one of them or an alloy of any one of them .
  • the cathode current collector is aluminum.
  • the inorganic solid electrolyte comprises a perovskite crystalline electrolyte, an inverse perovskite crystalline electrolyte, a superionic conductor type crystalline electrolyte, a fast ion conductive crystalline electrolyte, a garnet crystalline electrolyte or nitrogen.
  • a lithium-type crystalline electrolyte a lithium phosphorus-oxygen-nitrogen amorphous electrolyte, an amorphous sulfide amorphous electrolyte, and a composite electrolyte.
  • the positive electrode active material comprises lithium cobaltate, lithium nickelate, lithium manganate, lithium iron phosphate, lithium nickel cobaltate binary material, spinel structure oxide, lithium nickel cobalt manganese ternary material, layer A composite material of one or more or any one of lithium-rich high manganese materials.
  • the positive electrode active material layer further comprises a conductive agent and a binder
  • the positive electrode active material is contained in an amount of 60 to 95% by weight
  • the conductive agent is contained in an amount of 0.1 to 30% by weight
  • the binder is contained in an amount of 0.1 to 10% by weight. %.
  • the present invention also provides a method for preparing a secondary battery, the method comprising:
  • Preparing a battery negative electrode cutting a metal, metal alloy or metal composite conductive material into a desired size, and then washing the surface of the cut metal, metal alloy or metal composite conductive material, the washed metal, a metal alloy or a metal composite conductive material as a battery negative electrode;
  • the positive electrode of the battery prepares the positive electrode of the battery, weigh the living positive material, the conductive agent and the binder according to a certain ratio, add it into a suitable slurry and fully grind it into a uniform slurry, and then uniformly apply it to the surface of the positive current collector, and then cut the slurry after it is completely dried. Cutting to obtain a positive electrode of a desired size, the positive active material being a metal oxide or a metal compound;
  • Assembly is performed using the battery negative electrode, the solid electrolyte layer, and the battery positive electrode.
  • the invention has the beneficial effects that the solid electrolyte layer is used instead of the common liquid organic electrolyte, the electrode material is not easily corroded, the chemical stability can be maintained over a wide temperature range, and the use of the battery is increased. Life expectancy and greatly improve the safety of the battery and reduce the battery
  • the cost of packaging, in addition to the cation diffusion rate (ion conductivity) in the solid state is higher than that of the liquid electrolyte, theoretically it can achieve higher output; because the solid electrolyte layer is used, no diaphragm is needed, which reduces the volume of the battery and reduces the volume.
  • the overall quality of the battery increases the energy density of the battery; at the same time, the secondary battery provided by the invention cancels the negative active material, and directly uses the metal or the metal alloy or the metal composite as the negative electrode and the current collector, thereby not only reducing the cost of the battery production, but also simplifying
  • the production process can also effectively improve the battery capacity and energy density of the battery, and exhibit good charge and discharge cycle performance.
  • FIG. 1 is a schematic structural view of a secondary battery according to an embodiment of the present invention.
  • FIG. 1 is a schematic structural diagram of a secondary battery according to an embodiment of the present invention.
  • a secondary battery provided by an embodiment of the present invention includes a battery negative electrode 4, an all-solid electrolyte layer 3, and a battery positive electrode, wherein the battery negative electrode includes a negative electrode current collector and does not include a negative electrode active material; the negative electrode current collector is metal, Metal alloy or metal composite conductive material.
  • the all-solid electrolyte layer includes an inorganic solid electrolyte;
  • the battery positive electrode includes a positive electrode current collector 1 and a positive electrode active material layer 2,
  • the positive electrode current collector is a metal, a metal alloy or a metal composite conductive material, and the positive electrode active material includes a reversible deintercalation lithium ion
  • a positive electrode active material of sodium ion or magnesium ion, as long as lithium ion, sodium ion or magnesium ion is allowed to freely escape and intercalate, such as lithium, sodium or magnesium transition metal oxide and its doped binary or ternary transition Metal oxides, etc.
  • the working principle of the secondary battery provided by the embodiment of the present invention is: the secondary battery provided by the embodiment of the present invention does not contain the negative current collector, and during the charging process, the positive active material is delithiated, sodium or magnesium, and directly connected with the all solid electrolyte layer.
  • the metal or metal alloy of the negative electrode reacts to form a lithium-metal alloy, a sodium-metal alloy or a magnesium-metal alloy; during discharge, the lithium-metal alloy of the negative electrode, the sodium-metal alloy or the delithium, sodium or magnesium
  • the charge and discharge process is realized by embedding an all-solid electrolyte layer in the positive electrode active material.
  • the secondary battery provided by the embodiment of the invention replaces the common liquid organic electrolyte by using the all-solid electrolyte layer, and is not easy to corrode the electrode material, can maintain chemical stability over a wide temperature range, and increases the service life of the battery, and The safety performance of the battery is greatly improved, and the packaging cost of the battery is lowered.
  • the diffusion speed (ion conductivity) of the cation in the solid state is higher than that of the liquid electrolyte, which can achieve higher output;
  • the diaphragm is required, the battery volume is reduced, the overall quality of the battery is reduced, and the energy density of the battery is increased.
  • the secondary battery provided by the invention cancels the negative active material, and directly uses a metal or a metal alloy or a metal composite as a negative electrode and a set.
  • the fluid not only reduces the cost of battery production, but also simplifies the production process, and at the same time effectively increases the battery capacity and energy density of the battery, and exhibits good charge and discharge cycle performance.
  • the anode current collector comprises one or a combination of any one of aluminum, magnesium, lithium, vanadium, copper, iron, tin, zinc, nickel, titanium, manganese or any one of them. Several alloys. Further, the anode current collector is preferably aluminum.
  • the anode current collector is a multi-layer composite material of porous aluminum and other aluminum coated with aluminum foil or porous aluminum or carbon material.
  • the lithium ion which uses the porous aluminum foil to remove the positive active material is more fully reacted with the metal aluminum alloy to increase the battery capacity; and the carbon layer coated porous aluminum foil structure maintains the capacity of the battery, and the aluminum foil is maintained by the protection of the carbon layer.
  • the structure further improves the cycle stability of the battery; the use of the multi-layer aluminum composite material is also advantageous for suppressing and improving the volume expansion effect of the aluminum foil and improving the cycle performance of the battery.
  • the cathode current collector comprises one or a combination of any one of aluminum, magnesium, lithium, vanadium, copper, iron, tin, zinc, nickel, titanium, manganese or any one of them. Several alloys. Further, the cathode current collector is preferably aluminum.
  • the inorganic solid electrolyte comprises a perovskite crystalline electrolyte, an inverse perovskite crystalline electrolyte, a superionic conductor crystalline electrolyte, a fast ion conductive crystalline electrolyte, and a garnet crystal.
  • the positive electrode active material in the positive electrode active layer is also not particularly limited as long as the anion can be reversibly extracted or embedded.
  • the positive electrode active material is selected from lithium cobaltate (LiCoO 2 ), lithium nickelate (LiNiO 2 ), lithium manganate (LiMn 2 O 4 ), lithium iron phosphate (LiFePO 4 ).
  • lithium nickel cobaltate binary material LiNi 1-x Co x O 2
  • lithium cobalt cobalt manganate ternary Material Li(Ni,Co,Mn)O 2
  • layered lithium-rich high manganese material Li 2 MnO 3 -Li(NiCoMn)O 2
  • the positive electrode active material may be a sodium phosphate polyanion compound, a ferricyanide and a Prussian blue complex, an active redox polymer, a tunnel structure compound, a spinel oxide, One or more of the layered transition metal oxides.
  • it can be Na 2 V 3 (PO 4 ) 3 , Na 2 Zn 3 [Fe(CN) 6 ] 2 ⁇ xH 2 O, Na 2 Fe(SO 4 ) 2 , NaMn 2 O 4 , Na 0.61 [Mn 0.27 One or more of Fe 0.34 Ti 0.39 ]O 2 and NaCoO 2 .
  • the positive electrode active material layer further includes a conductive agent and a binder
  • the content of the positive electrode active material is 60-95 wt%
  • the content of the conductive agent is 0.1-30 wt%
  • the content of the binder is 0.1-10 wt%.
  • the conductive agent and the binder are not particularly limited and may be used in the art.
  • the conductive agent is one or more of conductive carbon black, Super P conductive carbon sphere, conductive graphite KS6, carbon nanotube, conductive carbon fiber, graphene, and reduced graphene oxide.
  • the binder is one or more of polyvinylidene fluoride, polytetrafluoroethylene, polyvinyl alcohol, carboxymethyl cellulose, SBR rubber, and polyolefin.
  • the embodiment of the invention further provides a method for preparing the above secondary battery, comprising:
  • Step 101 Prepare a battery negative electrode.
  • the metal, metal alloy or metal composite conductive material comprises one or a combination of any one of aluminum, magnesium, lithium, vanadium, copper, iron, tin, zinc, nickel, titanium, manganese or Any alloy may be a metal or metal alloy foil.
  • Step 102 preparing a solid electrolyte, and cutting the inorganic solid electrolyte layer into a certain shape and size for use;
  • Step 103 preparing a battery positive electrode.
  • the preparation of the positive electrode of the battery comprises: weighing the positive positive electrode material, the conductive agent and the binder according to a certain ratio, adding the appropriate slurry to the uniform slurry, and uniformly coating the surface of the positive current collector, and then performing the slurry completely after drying.
  • the battery is cut to obtain a positive electrode of a desired size, and the positive electrode active material is a metal oxide or a metal compound.
  • LiCoO 2 lithium cobaltate
  • LiNiO 2 lithium nickelate
  • LiMn 2 O 4
  • Step 104 assembling using the battery negative electrode, the all-solid electrolyte layer, and the battery positive electrode.
  • the prepared negative electrode, solid or gel electrolyte layer, and battery positive electrode are sequentially closely stacked in an inert gas or anhydrous oxygen-free environment, and then packaged into a battery case to complete battery assembly.
  • steps 101-103 describe the operation of the preparation method of the present invention in a specific order, it is not required or implied that these operations must be performed in this particular order.
  • the preparation of steps 101-103 can be performed simultaneously or in any order.
  • the secondary battery preparation method and the foregoing secondary battery are based on the same inventive concept, and the secondary battery obtained by the secondary battery preparation method has all the effects of the foregoing secondary battery, and details are not described herein again.
  • Preparation of battery negative electrode Take aluminum foil with a thickness of 0.02 mm, cut into a 12 mm diameter disc, wash the aluminum foil with ethanol, and dry it as a negative current collector for use.
  • a solid electrolyte is prepared, and the Li 0.5 La 0.5 TiO 3 electrolyte layer is cut into a certain shape and size for use;
  • Preparation of battery positive electrode 0.4 g of lithium cobaltate, 0.05 g of carbon black, 0.05 g of polyvinylidene fluoride was added to a 2 m] nitromethylpyrrolidone solution, and fully ground to obtain a uniform slurry; then the slurry was uniformly coated on the surface of the aluminum foil. And dried in a vacuum. The electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery positive electrode.
  • Battery assembly In the inert gas-protected glove box, the prepared negative electrode current collector, The solid electrolyte layer and the positive electrode of the battery are closely stacked in sequence, and then the stacked portion is packaged into a button battery case to complete battery assembly.
  • the battery negative electrode take 0.4g graphite, 0.05g carbon black, 0.05g polyvinylidene fluoride into 2ml nitromethylpyrrolidone solution, fully grind to obtain a uniform slurry; then uniformly apply the slurry on the surface of aluminum foil and vacuum dry .
  • the electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery negative electrode.
  • the polymer polyethylene was cut into a disk having a diameter of 16 mm, and dried for use as a separator.
  • the electrolyte was prepared: 0.75 g of lithium hexafluorophosphate was weighed and added to 2.5 ml of ethylene carbonate and 2.5 ml of dimethyl carbonate, and the mixture was thoroughly stirred until lithium hexafluorophosphate was completely dissolved, and then it was used as an electrolyte.
  • Preparation of battery positive electrode 0.4 g of lithium cobaltate positive electrode material, 0.05 g of carbon black, 0.05 g of polyvinylidene fluoride was added to 2 ml of nitromethylpyrrolidone solution, and fully ground to obtain a uniform slurry; then the slurry was uniformly coated on aluminum foil. The surface was dried under vacuum. The electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery positive electrode.
  • the prepared negative electrode current collector, separator, and battery positive electrode are closely stacked in sequence, and the electrolyte is dripped to completely infiltrate the separator, and then the stacked portion is packaged into the button battery case. , complete battery assembly.
  • the secondary battery prepared in the above embodiment of the secondary battery preparation method was charged by a constant current of 100 mA/g of the positive electrode active material until its voltage reached 4.8 V, and then discharged at the same current until the voltage reached 3V, measuring its battery capacity and energy density, testing its cycle stability, expressed in cycles, the number of cycles is the number of times the battery is charged and discharged when the battery capacity is attenuated to 85%.
  • Example 6 uses a carbon layer to coat porous aluminum as a cathode current collector.
  • the number of cycles of the battery was optimized, in contrast to Example 5 using porous aluminum as the negative electrode material and Example 1 using aluminum foil as the negative electrode material to obtain a larger battery capacity.
  • Examples 7-12 used different positive electrode active materials, and in combination with the corresponding inorganic solid electrolyte, good battery capacity and cycle performance of the battery were achieved.

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  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
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  • General Chemical & Material Sciences (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

La présente invention concerne le domaine des batteries et, en particulier, une batterie rechargeable et son procédé de préparation. La batterie secondaire comprend une électrode négative de batterie, une électrode positive de batterie et une couche d'électrolyte tout solide, l'électrode négative de batterie comprenant un collecteur de courant d'électrode négative et ne comprenant pas un matériau actif d'électrode négative, la couche d'électrolyte tout solide étant un électrolyte solide inorganique, l'électrode positive de batterie comprenant un collecteur de courant d'électrode positive et une couche de matériau actif d'électrode positive, la couche de matériau actif d'électrode positive comprenant un matériau actif d'électrode positive qui désintercale librement et de façon réversible des ions lithium, des ions sodium ou des ions magnésium. En utilisant la couche d'électrolyte tout solide, la batterie secondaire ne corrode pas aisément des matériaux d'électrode et est capable de maintenir une stabilité chimique dans une large plage de température, ce qui augmente la durée de vie de la batterie; par ailleurs, en utilisant la couche d'électrolyte tout solide, la batterie rechargeable n'a pas besoin de séparateur, ce qui réduit le volume et la masse totale de la batterie, et augmente la densité d'énergie de la batterie; et en excluant la substance active d'électrode négative, la batterie rechargeable réduit non seulement le coût de production de la batterie, mais en outre, améliore efficacement la capacité et la densité d'énergie de la batterie, et présente de bonnes performances de cycle de charge et de décharge.
PCT/CN2016/081349 2016-05-06 2016-05-06 Batterie rechargeable et son procédé de préparation Ceased WO2017190367A1 (fr)

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CN201680085080.2A CN109155433A (zh) 2016-05-06 2016-05-06 一种二次电池及其制备方法
PCT/CN2016/081349 WO2017190367A1 (fr) 2016-05-06 2016-05-06 Batterie rechargeable et son procédé de préparation

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