WO2018209762A1 - Anode de batterie au lithium et son procédé de préparation et son application - Google Patents

Anode de batterie au lithium et son procédé de préparation et son application Download PDF

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Publication number
WO2018209762A1
WO2018209762A1 PCT/CN2017/090252 CN2017090252W WO2018209762A1 WO 2018209762 A1 WO2018209762 A1 WO 2018209762A1 CN 2017090252 W CN2017090252 W CN 2017090252W WO 2018209762 A1 WO2018209762 A1 WO 2018209762A1
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negative electrode
layer
lithium
lithium battery
battery
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PCT/CN2017/090252
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English (en)
Chinese (zh)
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宋殿权
张春涛
王永鹤
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哈尔滨光宇电源股份有限公司
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Publication of WO2018209762A1 publication Critical patent/WO2018209762A1/fr

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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
    • 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
    • H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
    • 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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • H01M4/366—Composites as layered products
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/381—Alkaline or alkaline earth metals elements
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/381—Alkaline or alkaline earth metals elements
    • H01M4/382—Lithium
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/628—Inhibitors, e.g. gassing inhibitors, corrosion inhibitors
    • 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 invention relates to a method for preparing a negative electrode of a lithium battery. It belongs to the field of solid-state batteries and liquid batteries.
  • Lithium metal anodes can theoretically provide more capacity (3860mAh/g, graphite anode: 370mAh/g) compared to graphite anodes used in commercial lithium-ion batteries. Lithium metal anodes are expected to be in next-generation portable electronic devices. And large areas of applications such as electric vehicles. Lithium-sulfur batteries and lithium-ion batteries with lithium metal as the negative electrode have gradually attracted the attention of researchers, and have become a hot spot in academic and industrial research in recent years. However, there are still many problems in the research of lithium metal anodes, the most important of which is the growth of dendrites.
  • the dendrites are dendritic lithium deposits which appear in the negative electrode during the multiple deposition/precipitation of the lithium ion negative electrode. Dendritic growth brings two problems: (1) the dendrite will pierce the diaphragm and cause short circuit of the battery. The short-circuit current inside the positive and negative electrodes generates heat inside the battery, causing the battery system to run out of control, which may cause the battery to catch fire or even explode. A series of safety issues; (2) dendrites will increase the side reaction of electrolyte and metal lithium, consume lithium active substances, and reduce battery utilization. The lithium dendrites that are out of the current collector are dead lithium, and the presence of dead lithium reduces the available active materials, reducing the efficiency and cycle life of the battery.
  • Lithium batteries based on lithium metal anodes are still in the laboratory stage, and few industrial achievements have been made.
  • the invention is to solve the problem that the conventional graphite anode has a low specific capacity, a dendrite is easy to grow, a first coulombic efficiency is low, and a battery energy density is low, and a lithium battery anode preparation method is now provided.
  • the invention provides a method for preparing a negative electrode of a lithium battery, the method comprising the following steps:
  • Step 1 mixing a carbon material having a mass percentage of 75% to 90%, a conductive agent having a mass percentage of 5% to 20%, and a binder having a mass percentage of 5% to 10%.
  • Step 2 uniformly depositing a metal lithium layer or a metal sodium layer (2) having a thickness of 1 ⁇ m to 30 ⁇ m on the intermediate material layer (1);
  • Step 3 After completing the operations of Step 1 and Step 2, the tab (3) is connected to the current collector (4) to complete the preparation of the anode of the lithium battery.
  • the invention provides a lithium battery negative electrode, which comprises:
  • the intermediate material layer is composed of the following mass percentage components: carbon-based material 75% to 90%, conductive agent 5-20%, and binder 5-10%; the intermediate material layer has a thickness of 1 ⁇ m ⁇ 70 ⁇ m; the metal lithium layer or the metal sodium layer has a thickness of 1 ⁇ m to 30 ⁇ m.
  • the negative electrode of the lithium battery of the present invention is composed of a bottom layer current collector, an intermediate material layer and a metal lithium layer or a metal sodium layer attached to the intermediate material layer, wherein the intermediate material layer is composed of a component represented by the following mass percentage: carbon 75% to 90% of the material, 5% to 20% of the conductive agent and 5% to 10% of the binder, the thickness of the intermediate layer is 1 ⁇ m to 70 ⁇ m; the metal lithium layer or the metal sodium layer can be vapor deposited with lithium metal in the middle The material layer is obtained, wherein the metal lithium layer or the metal sodium layer has a thickness of 1 ⁇ m to 30 ⁇ m, which is a dense and uniform metal lithium layer or a metal sodium layer.
  • the intermediate material layer is composed of a component represented by the following mass percentage: carbon 75% to 90% of the material, 5% to 20% of the conductive agent and 5% to 10% of the binder, the thickness of the intermediate layer is 1 ⁇ m to 70 ⁇ m; the metal lithium layer or the metal sodium layer can be
  • the lithium battery negative electrode of the invention can adjust the distribution of lithium ions on the surface of the negative electrode by using the intermediate substance layer, avoid the aggregation of the lithium ion battery in time and space, realize the uniform distribution of lithium ions on the surface of the negative electrode, thereby inhibiting the occurrence of lithium dendrites. Improves the safety performance of lithium metal batteries.
  • the negative electrode of the lithium battery is coupled with a positive electrode material having a high specific capacity such as sulfur, air, etc., and is important for constructing a lithium battery system with high energy density, high stability, and high safety.
  • the present invention provides the use of a lithium battery anode as described above in the preparation of a solid state battery or a liquid battery. Specifically, the present invention provides a lithium battery comprising a positive electrode and a negative electrode, wherein the negative electrode is the lithium battery negative electrode described above.
  • the lithium battery anode composed of the present application can be applied in the field of solid battery and liquid battery, and the evaporated lithium metal or metal sodium can inhibit the generation of lithium dendrites during charging and discharging of the battery, thereby improving the safety of the battery, and the new type
  • the negative electrode of the lithium battery can reduce the irreversible capacity loss of the battery during the formation process.
  • the first coulombic efficiency of the battery is improved, and the positive electrode material capacity is increased by 3%-20%.
  • the lithium battery anode of the present application and the nickel-cobalt-aluminum ternary cathode material are assembled into a button battery, and the first Coulomb efficiency of the battery is 97%, and the conventional graphite anode and the nickel-cobalt-aluminum ternary cathode material are assembled into a button battery, which is the first Coulomb battery. The efficiency is 92%.
  • the lithium battery negative electrode of the present application and the nickel cobalt aluminum ternary positive electrode material are assembled into a button battery, and the capacity is reduced by 1.8% in a cycle of 200 weeks, and the lithium metal plate is used as a negative electrode and the nickel cobalt aluminum ternary positive electrode material is assembled into a button battery.
  • the cycle capacity decays by 3.4% for 200 cycles.
  • the negative electrode of the lithium battery of the present application is matched with the same nickel-cobalt-aluminum ternary positive electrode material as compared with the conventional graphite negative electrode.
  • the quality of the negative electrode of the lithium battery of the present application is 10% to 80% lower than that of the conventional graphite negative electrode, and the thickness is thinner than that of the conventional negative electrode. % ⁇ 90%.
  • the quality of the negative electrode of the lithium battery constructed by the present application is 10% to 80% lower than that of the conventional graphite negative electrode, and the thickness is reduced by 10% to 90% compared with the conventional negative electrode, thereby greatly improving the gram capacity of the negative electrode material, and the battery can be
  • the energy density is increased by 1 to 4 times, which improves the energy utilization rate of the battery.
  • reference numeral 1 is a schematic view showing the external structure of a negative electrode of a lithium battery, wherein reference numeral 1 denotes an intermediate substance layer, reference numeral 2 denotes a metallic lithium layer or a metallic sodium layer, and reference numeral 3 denotes a tab;
  • reference numeral 1 denotes an intermediate substance layer
  • reference numeral 2 denotes a metallic lithium layer or a metallic sodium layer
  • reference numeral 4 denotes a current collector (copper foil).
  • Step 1 mixing a carbon material having a mass percentage of 75% to 90%, a conductive agent having a mass percentage of 5% to 20%, and a binder having a mass percentage of 5% to 10%.
  • Step 2 uniformly depositing a metal lithium layer or a metal sodium layer (2) having a thickness of 1 ⁇ m to 30 ⁇ m on the intermediate material layer (1);
  • Step 3 After completing the operations of Step 1 and Step 2, the tab (3) is connected to the current collector (4) to complete the preparation of the anode of the lithium battery.
  • the distribution of lithium ions on the surface of the negative electrode can be regulated by using the intermediate substance layer, the aggregation of the lithium ion battery in time and space is avoided, and the uniform distribution of lithium ions on the surface of the negative electrode is achieved, thereby suppressing the occurrence of lithium dendrites.
  • the vapor-deposited metal lithium layer is realized by an intermediate substance layer which strongly adsorbs lithium ions.
  • the structure of the negative electrode of the lithium battery can effectively inhibit the generation of lithium dendrites, improve the safety of the battery, and improve the energy utilization rate of the battery. For example, the use of a high specific capacity positive electrode material will help promote the new high energy density lithium battery. Practical process.
  • the carbon material having a mass percentage of 75% to 90% means that the ratio of the mass of the carbon material to the total mass of the intermediate material layer (1) is 75% to 90%; the mass percentage is 5 % to 20% of the conductive agent means that the ratio of the mass of the conductive agent to the total mass of the intermediate substance layer (1) is 5% to 20%; the binder having a mass percentage of 5% to 10% means the binder The ratio of the mass to the total mass of the intermediate substance layer (1) is 5% to 10%.
  • Embodiment 2 This embodiment further describes a method for preparing a negative electrode of a lithium battery according to the first embodiment.
  • an intermediate material layer formed by mixing carbon materials coated on the current collector (4) (1)
  • Step 1 metal lithium or metal sodium evaporated on the intermediate material layer (1). See step 2 for details.
  • the third embodiment of the present invention is to further describe the method for preparing a negative electrode of a lithium battery according to the first embodiment.
  • the carbon-based material in the first step includes soft carbon, hard carbon, silicon carbon, and graphite.
  • the conductive agent and the binder in the first step may be those commonly used in the art, and the present invention is not particularly limited.
  • the conductive agent may be conductive carbon black (ie, super-P, SUPER-P).
  • the binder may be polyvinylidene fluoride (PVDF).
  • This embodiment further describes a method for preparing a negative electrode of a lithium battery according to the first embodiment.
  • the intermediate material layer (1), the metal lithium layer, and the metal sodium layer are both lithium battery negative electrodes. Active substance.
  • the invention provides a lithium battery negative electrode, which comprises:
  • the intermediate material layer is composed of the following mass percentage components: 75% to 90% of the carbon material, 5% to 20% of the conductive agent, and 5% to 10% of the binder; the thickness of the intermediate layer is 1 ⁇ m to 70 ⁇ m; the metal lithium layer or the metal sodium layer has a thickness of 1 ⁇ m to 30 ⁇ m.
  • a negative electrode of a lithium battery provided by an embodiment of the present invention includes a current collector (4), which is usually located on the bottom layer; and a copper foil well known in the art can be used as a current collector.
  • the current collector is connected to a tab (3).
  • the lithium battery negative electrode provided by the embodiment of the present invention includes an intermediate substance layer (1) which is formed by coating an intermediate substance layer mixed component on the current collector (4).
  • the intermediate substance layer is composed of 75% to 90% of a carbonaceous material, 5% to 20% of a conductive agent, and 5% to 10% of a binder according to a mass percentage.
  • the carbon-based material includes one or more of all kinds of soft carbon, hard carbon, silicon carbon, and graphite.
  • the conductive agent and the binder are both generally used in the art, and the invention is not particularly limited.
  • the intermediate substance layer has a porous structure and has an adsorption effect.
  • the intermediate substance layer has a thickness of from 1 ⁇ m to 70 ⁇ m.
  • the invention utilizes the intermediate substance layer to regulate the distribution of lithium ions on the surface of the negative electrode, avoids the aggregation of the lithium ion battery in time and space, realizes the uniform distribution of lithium ions on the surface of the negative electrode, and thereby inhibits the occurrence of lithium dendrites.
  • the negative electrode of the lithium battery provided by the embodiment of the invention comprises a metal lithium layer or a metal sodium layer (2) attached to the intermediate material layer (1) and formed by evaporation.
  • the metal lithium layer or the metal sodium layer has a thickness of from 1 ⁇ m to 30 ⁇ m; and its density is uniform.
  • the evaporated lithium metal or sodium metal can inhibit the generation of lithium dendrites during charging and discharging of the battery, further improving the safety of the battery.
  • the structure of the negative electrode of the lithium battery of the invention can effectively inhibit the generation of lithium dendrites, improve the safety of the battery, and improve the energy utilization rate of the battery.
  • the quality of the negative electrode of the lithium battery of the invention is lighter than that of the conventional graphite negative electrode, and the thickness is thinner than that of the conventional negative electrode, which greatly increases the gram capacity of the negative electrode material.
  • the method for preparing the lithium battery anode described above may include the following steps:
  • Step 1 Mix carbon materials with a mass percentage of 75% to 90%, a conductive agent with a mass percentage of 5% to 20%, and a binder with a mass percentage of 5% to 10%, according to 1 ⁇ m. a thickness of ⁇ 70 ⁇ m is coated on the current collector (4) to form a porous intermediate material layer (1);
  • Step 2 uniformly depositing a metal lithium layer or a metal sodium layer (2) having a thickness of 1 ⁇ m to 30 ⁇ m on the intermediate material layer (1);
  • Step 3 After completing the operations of Step 1 and Step 2, the tab (3) is connected to the current collector (4) to complete the preparation of the anode of the lithium battery.
  • the invention also provides the use of a lithium battery anode as described above in the preparation of a solid state battery or a liquid battery.
  • the present invention provides a lithium battery comprising a positive electrode and a negative electrode, wherein the negative electrode is the lithium battery negative electrode described above.
  • the active material in the positive electrode is selected from sulfur or air; the negative electrode of the lithium battery is coupled with a high specific capacity positive electrode material such as sulfur and air for constructing high energy density, high stability, and high safety.
  • the lithium battery system is of great significance.
  • the active material in the positive electrode is a nickel-cobalt-aluminum ternary positive electrode material; the button battery or the like can be assembled according to a conventional method, and the lithium battery has a high first coulombic efficiency and a high Battery energy density and excellent cycle performance.
  • the lithium battery negative electrode provided by the present invention and a preparation method and application thereof will be specifically described below in conjunction with the embodiments.
  • Step 1 Mixing 90% by mass of graphite, 5% by weight of SUPER-P and 5% by mass of PVDF, and coating the current collector copper foil with a thickness of 70 ⁇ m (4) a porous intermediate material layer (1);
  • Step 2 uniformly depositing a metal lithium layer (2) having a thickness of 3 ⁇ m on the intermediate material layer (1);
  • Step 3 After completing the operations of Step 1 and Step 2, the tab (3) is connected to the current collector (4) to complete the preparation of the anode of the lithium battery.
  • the lithium battery anode of the present application and the nickel-cobalt-aluminum ternary cathode material are assembled into a button battery, and the first Coulomb efficiency of the battery is 97%, and the conventional graphite anode and the nickel-cobalt-aluminum ternary cathode material are assembled into a button battery, which is the first Coulomb battery. The efficiency is 92%.
  • the lithium battery negative electrode of the present application and the nickel cobalt aluminum ternary positive electrode material are assembled into a button battery for circulation
  • the 200-week capacity is attenuated by 1.8%, and a pure metal lithium plate is used as a negative electrode and a nickel-cobalt-aluminum ternary positive electrode material is assembled into a button battery, and the cycle capacity is reduced by 3.4% in 200 cycles.
  • the quality of the negative electrode of the lithium battery formed by the present application is 40% lower than that of the conventional graphite negative electrode, and the thickness is reduced by 35% compared with the conventional negative electrode, which greatly increases the gram capacity of the negative electrode material, and can increase the energy density of the battery by 1.5 times, thereby improving the energy density of the battery. Battery energy utilization.
  • Step 1 Mixing 90% by mass of graphite, 5% by weight of SUPER-P and 5% by mass of PVDF, and coating the current collector copper foil according to a thickness of 40 ⁇ m (4) a porous intermediate material layer (1);
  • Step 2 uniformly depositing a metal sodium layer (2) having a thickness of 10 ⁇ m on the intermediate material layer (1);
  • Step 3 After completing the operations of Step 1 and Step 2, the tab (3) is connected to the current collector (4) to complete the preparation of the anode of the lithium battery.
  • the lithium battery negative electrode of the present application and the nickel cobalt aluminum ternary positive electrode material are assembled into a button battery, and the first coulombic efficiency of the battery is 98%.
  • the lithium battery negative electrode of the present application and the nickel-cobalt-aluminum ternary positive electrode material were assembled into a coin cell battery, and the capacity was reduced by 1.6% in a cycle of 200 weeks.
  • the quality of the negative electrode of the lithium battery formed by the present application is 60% lower than that of the conventional graphite negative electrode, and the thickness is reduced by 50% compared with the conventional negative electrode, which greatly increases the gram capacity of the negative electrode material, and can increase the energy density of the battery by 2 times, thereby improving the energy density of the battery. Battery energy utilization.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Composite Materials (AREA)
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Abstract

Un procédé de préparation d'une anode de batterie au lithium concerne le domaine des piles à électrolyte solide et des batteries à l'état liquide. Les problèmes actuels de faible capacité spécifique en gramme d'une électrode négative en graphite classique, de croissance dendritique rapide, de faible efficacité coulombienne initiale et de faible densité d'énergie de batterie sont résolus en conséquence. Le procédé comprend : l'étape 1, consistant à mélanger de 75 % à 90 % en masse d'un matériau carboné, de 5 % à 20 % en masse d'un agent conducteur, et de 5 % à 10 % en masse d'un agent de liaison pour former une couche intermédiaire absorbante ou poreuse (1), et à revêtir la couche intermédiaire (1) à une épaisseur de 1 à 70 µm sur un collecteur de courant (4) ; l'étape 2, consistant à déposer en phase vapeur une couche de métal de lithium ou une couche de métal de sodium (2) à une épaisseur de 1 à 30 µm uniformément sur la couche intermédiaire (1) ; et l'étape 3, consistant à connecter une languette de batterie (3) au collecteur de courant (4) après la réalisation de l'étape 1 et de l'étape 2 pour terminer la préparation d'une électrode négative de batterie au lithium. L'électrode négative de batterie au lithium peut être appliquée dans le domaine des piles à électrolyte solide et le domaine des batteries à l'état liquide.
PCT/CN2017/090252 2017-05-15 2017-06-27 Anode de batterie au lithium et son procédé de préparation et son application WO2018209762A1 (fr)

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CN112750978B (zh) * 2020-12-30 2022-03-15 珠海冠宇电池股份有限公司 极片及电池
WO2022143210A1 (fr) * 2020-12-30 2022-07-07 珠海冠宇电池股份有限公司 Pièce d'électrode et batterie

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