CN108735970B - Sandwich structure metal composite negative plate for secondary battery - Google Patents

Sandwich structure metal composite negative plate for secondary battery Download PDF

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CN108735970B
CN108735970B CN201810358099.0A CN201810358099A CN108735970B CN 108735970 B CN108735970 B CN 108735970B CN 201810358099 A CN201810358099 A CN 201810358099A CN 108735970 B CN108735970 B CN 108735970B
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metal
nanowire
copper
sheet
composite negative
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CN108735970A (en
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马延文
陈剑宇
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Nanjing University of Posts and Telecommunications
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Nanjing University of Posts and Telecommunications
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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
    • H01M4/134—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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Cell Electrode Carriers And Collectors (AREA)

Abstract

The invention relates to a sandwich structure metal composite negative plate for a secondary battery, which comprises an M metal plate and metal nanowire layers adhered to the upper surface and the lower surface of the M metal plate, wherein the M metal plate is a lithium metal plate, a sodium metal plate or a magnesium metal plate, the metal nanowire layer is composed of a group of metal nanowires adhered to the surface of the M metal plate, and the metal nanowires are copper nanowires, nickel nanowires or copper-nickel nanowires. The invention has the advantages that the surface current is dispersed through the network structure formed by the metal nanowires adhered on the upper surface and the lower surface of the M metal sheet, and the distribution of M metal ions is more uniform.

Description

Sandwich structure metal composite negative plate for secondary battery
Technical Field
The invention relates to a sandwich structure metal composite negative plate for a secondary battery, in particular to a sandwich structure lithium metal composite negative plate, and belongs to the technical field of secondary batteries.
Background
It is understood that lithium metal negative electrodes can theoretically provide more capacity (3860mAh g) than the graphite negative electrodes in existing commercially available secondary batteries, such as lithium ion batteries -1 ) And the most negative potential (-3.040V vs. standard hydrogen electrode), the lithium metal negative electrode is expected to realize larger application in the fields of next-generation portable electronic equipment, electric automobiles and the like. However, since the 1970 s, explosion accidents occurred soon since the first generation of commercial lithium metal full cells, because when lithium was deposited on the flat lithium sheet surface during cycling, the subsequently deposited lithium grew along the previously deposited lithium due to the tip deposition effect, forming lithium dendrites. Due to the generation of dendritic lithium, part of dendritic lithium is separated from a lithium substrate to become 'dead lithium', and can not be reused, the dendritic lithium continuously grows and accumulates to puncture a diaphragm to cause short circuit of the battery, the increase of the dead lithium can cause that more lithium can not participate in the utilization of the battery again to cause the reduction of coulombic efficiency, and the irreversible loss of capacity. These all cause problems in the life and safety of the lithium metal battery. Therefore, how to regulate the structure of the lithium surface and promote the uniform distribution of current and lithium ions on the surface of the negative electrode is a hot issue which needs to be intensively researched nowadays.
Disclosure of Invention
The invention aims to: aiming at the defects in the prior art, the sandwich-structure metal composite negative plate for the secondary battery is provided, which can disperse surface current without other current collectors and make metal ions uniformly distributed.
In order to achieve the above object, the present invention provides a metal composite negative electrode sheet with a sandwich structure for a secondary battery, comprising an M metal sheet and metal nanowire layers adhered to the upper and lower surfaces of the M metal sheet, wherein the M metal sheet is a lithium metal sheet, a sodium metal sheet or a magnesium metal sheet, the metal nanowire layer is composed of a group of metal nanowires adhered to the surface of the M metal sheet, the metal nanowires are copper nanowires, nickel nanowires or copper-nickel nanowires, and the metal nanowire layers on the upper and lower surfaces of the M metal sheet are made of the same material.
According to the invention, the metal nanowire layer is adhered to the upper surface and the lower surface of the M metal sheet, and the metal nanowire layer adhered to one surface of the M metal sheet is directly used as a current collector without other current collectors. The method is realized by wrapping the upper surface and the lower surface of the ultrathin metal sheet by the copper nanowires, the upper surface and the lower surface of the metal sheet are wrapped between two layers of copper nanowire films in the mode, and a copper nanowire network structure is formed on the metal surface layer, so that the distribution of current and metal ions on a negative electrode can be regulated and controlled, the formation and growth of dendritic crystal lithium caused by the fact that the current forms a tip effect at a certain point are avoided, the metal ions are uniformly distributed through the shunting action of the copper nanowire network, and the effect of inhibiting the dendritic crystal lithium is realized. In addition, the arrangement mode of the metal nanowires on the upper surface and the lower surface of the metal sheet is free dispersion arrangement, and the metal nanowires can form a network structure and are in cross connection according to the properties of the metal nanowires, so that the nanowire films (the nanowires on the upper surface and the lower surface are both a film) can form a good conductive network. Therefore, the pattern of the metal nanowire layer of the present invention is a network cross shape.
Preferably, the M metal sheet is a lithium metal sheet, and the metal nanowire is a copper nanowire.
The preferable scheme of the invention is that the sandwich structure metal composite negative plate for the lithium metal battery comprises a lithium metal plate and copper nanowire layers adhered to the upper surface and the lower surface of the lithium metal plate.
Preferably, the thickness of the lithium metal sheet is 10 to 500 μm. The diameter of the copper nanowire is 50-100 nm, and the length of the copper nanowire is 50-200 mu m.
The lithium metal sheet is an ultrathin metal lithium sheet, the waste of lithium resources is reduced due to the lithium sheet with the thickness, the surface of a negative electrode is more stable due to the composition of the lithium sheet and the copper nanowire, the cycle life of the battery is greatly prolonged, the coulombic efficiency is greatly improved, and the industrialization process of the lithium metal battery, particularly the lithium-sulfur battery and the lithium-air battery with high energy density is promoted. For a lithium metal battery, a network structure formed by metal nanowires is adhered to the upper surface and the lower surface of a lithium metal sheet, the structure inhibits dendritic lithium generation in the battery cycle process, stabilizes a lithium metal negative electrode, improves the coulombic efficiency of the battery, prolongs the service life of the battery, is very necessary for improving the safety performance of the lithium metal battery, and has important significance for constructing a high-energy-density lithium metal battery (such as a lithium sulfur battery and a lithium air battery) system.
Preferably, the metal nanowires are adhered in a pressurizing compounding manner, and the specific method is that the metal nanowires are pressed on the upper surface and the lower surface of the M metal sheet in a pressurizing manner, and the applied pressure is 0.1-10 MPa. The metal nanowires are adhered to the upper surface and the lower surface of the M metal sheet in a pressurizing mode, and the contact resistance of the metal nanowires and the M metal sheet is reduced in a composite mode.
Preferably, the diameter of the nickel nanowire is 50-100 nm, and the length of the nickel nanowire is 50-100 mu m.
Preferably, the copper-nickel nanowire is formed by mixing a copper nanowire and a nickel nanowire, and the mass ratio of the copper nanowire to the nickel nanowire is (1-9): (1-9); the diameter of the copper nanowire is 50-100 nm, and the length of the copper nanowire is 50-200 mu m; the diameter of the nickel nanowire is 50-100 nm, and the length of the nickel nanowire is 50-100 mu m.
Preferably, the thickness of the metal composite negative plate with the sandwich structure is 10-500 μm.
Preferably, the sandwich-structured metal composite negative electrode sheet is used in a secondary battery. The secondary battery is a lithium metal battery, a sodium metal battery or a magnesium metal battery.
The invention has the advantages that:
1. according to the sandwich-structure metal composite negative plate, the surface current is dispersed through the network structure formed by the metal nanowires adhered to the upper surface and the lower surface of the M metal sheet, and meanwhile, the distribution of M metal ions is more uniform;
2. the metal nanowires are adhered to the upper surface and the lower surface of the M metal sheet in a pressurizing mode, and the contact resistance of the metal nanowires and the M metal sheet is reduced in a composite mode;
3. according to the invention, the metal nanowire layers are adhered to the upper surface and the lower surface of the M metal sheet, and the metal nanowire layer adhered to one surface of the M metal sheet is directly used as a current collector without other current collectors.
Drawings
The invention will be further described with reference to the accompanying drawings.
FIG. 1 is a flow chart of the present invention.
Detailed Description
Example 1
And (3) cleaning and drying 1g of a copper nanowire sample, and placing the sample in 10ml of n-hexane for uniform ultrasonic dispersion to obtain a copper nanowire dispersion liquid, wherein the diameter of the copper nanowire is 100nm, and the length of the copper nanowire is 100 micrometers. And (3) preparing the copper nanowire dispersion liquid into a film by adopting a spraying method, wherein the thickness of the film is 1 mu m. The pattern of the film should be a network cross shape.
The lithium metal sheet was cut into a pole piece having a diameter of 12mm and a thickness of 10 μm by a microtome.
And (3) respectively rolling the upper surface and the lower surface of the pole piece with the copper nanowire film under the pressure of 0.1MPa to obtain the lithium metal-copper nanowire composite negative electrode with the sandwich structure, wherein the thickness of the composite negative electrode piece is 10 microns. The copper nanowires are arranged on the upper and lower surfaces of the lithium metal sheet in a freely dispersed manner, and because the copper nanowires can form network structures which are connected in a cross manner according to the properties of the copper nanowires, the copper nanowires can form a good conductive network on the nanowire film.
The prepared sandwich-structure lithium metal-copper nanowire composite cathode is assembled into a symmetrical battery to test the stability of the battery, the current density is 200 muA, and the voltage hysteresis value after 1000 cycles of cycle is 30 mV.
Example 2
And (3) cleaning and drying 1g of a copper nanowire sample, and placing the sample in 10ml of n-hexane for uniform ultrasonic dispersion to obtain a copper nanowire dispersion liquid, wherein the diameter of the copper nanowire is 100nm, and the length of the copper nanowire is 200 microns. And preparing the copper nanowire dispersion liquid into a film by adopting a spraying method, wherein the thickness of the film is 2 mu m.
The lithium metal sheet was cut into a pole piece having a diameter of 12mm and a thickness of 20 μm by a microtome.
And (3) respectively rolling the upper surface and the lower surface of the pole piece with the copper nanowire film under the pressure of 0.5MPa to obtain the sandwich-structure lithium metal-copper nanowire composite negative electrode, wherein the thickness of the composite negative electrode piece is 20 micrometers.
The prepared sandwich-structure lithium metal-copper nanowire composite cathode is assembled into a symmetrical battery to test the stability of the battery, the current density is 1mA, and the voltage hysteresis value after 1000 cycles of cycle is measured to be 50 mV.
Example 3
And (3) cleaning and drying 1g of nickel nanowire sample, and placing the sample in 10ml of n-hexane for uniform ultrasonic dispersion to obtain a nickel nanowire dispersion liquid, wherein the diameter of the nickel nanowire is 50nm, and the length of the nickel nanowire is 50 microns. The nickel nanowire dispersion liquid is made into a film by a spraying method, and the thickness of the film is 0.5 mu m.
The lithium metal sheet was cut into a pole piece having a diameter of 12mm and a thickness of 10 μm by a microtome.
And (3) respectively rolling the upper surface and the lower surface of the pole piece with the nickel nanowire film under the pressure of 1MPa to obtain the lithium metal-nickel nanowire composite negative electrode with the sandwich structure, wherein the thickness of the composite negative pole piece is 11 microns.
The prepared sandwich-structure lithium metal-nickel nanowire composite cathode is assembled into a symmetrical battery to test the stability of the battery, the current density is 200 muA, and the voltage hysteresis value after 1000 cycles of cycle is 500 mV.
Example 4
Cleaning and drying 1g of copper nanowire and nickel nanowire samples, and placing the samples in 10ml of normal hexane for uniform ultrasonic dispersion to obtain copper-nickel nanowire dispersion liquid, wherein the diameter of the copper nanowire is 50nm, and the length of the copper nanowire is 100 micrometers; the diameter of the nickel nanowire is 50nm, and the length of the nickel nanowire is 100 micrometers; the mass ratio of the copper nanowire to the nickel nanowire is 1: 1. and preparing the copper-nickel nanowire dispersion liquid into a film by adopting a spraying method, wherein the thickness of the film is 2 mu m.
The lithium metal sheet was cut into a pole piece having a diameter of 12mm and a thickness of 10 μm by a microtome.
And (3) respectively rolling the upper surface and the lower surface of the pole piece with the copper-nickel nanowire film under the pressure of 1MPa to obtain the lithium metal-copper-nickel nanowire composite negative electrode with the sandwich structure, wherein the thickness of the composite negative electrode piece is 14 microns.
The prepared sandwich-structure lithium metal-copper-nickel nanowire composite cathode is assembled into a symmetrical battery to test the stability of the battery, the current density is 200 muA, and the voltage hysteresis value is 200mV after 1000 cycles of cycle.
Example 5
And (3) cleaning and drying 1g of a copper nanowire sample, and placing the sample in 10ml of n-hexane for uniform ultrasonic dispersion to obtain a copper nanowire dispersion liquid, wherein the diameter of the copper nanowire is 100nm, and the length of the copper nanowire is 100 micrometers. And preparing the copper nanowire dispersion liquid into a film by adopting a spraying method, wherein the thickness of the film is 1 mu m.
The lithium metal sheet was cut into a pole piece having a diameter of 12mm and a thickness of 10 μm by a microtome.
And (3) respectively rolling the upper surface and the lower surface of the pole piece with the copper nanowire film under the pressure of 1MPa to obtain the lithium metal-copper nickel nanowire composite negative electrode with the sandwich structure, wherein the thickness of the composite negative electrode piece is 12 microns.
The prepared sandwich-structured lithium metal-copper nanowire composite cathode is assembled into a symmetrical battery to test the stability of the battery, the current density is 1mA, and the voltage hysteresis value after 1000 cycles of circulation is 10 mV.
The prepared sandwich-structure lithium metal-copper nanowire composite negative electrode is assembled into a full battery to be used as a negative electrode, a lithium iron phosphate pole piece is used as a positive electrode, and the capacity of the battery after 200 cycles is measured to be kept to be 160 mAh.g -1 The coulombic efficiency was 97%.
Example 6
And (3) cleaning and drying 1g of a copper nanowire sample, and placing the sample in 10ml of n-hexane for uniform ultrasonic dispersion to obtain a copper nanowire dispersion liquid, wherein the diameter of the copper nanowire is 100nm, and the length of the copper nanowire is 100 micrometers. And preparing the copper nanowire dispersion liquid into a film by adopting a spraying method, wherein the thickness of the film is 5 mu m.
The lithium metal sheet was cut into a pole piece having a diameter of 12mm and a thickness of 10 μm by a microtome.
And (3) respectively rolling the upper surface and the lower surface of the pole piece with the copper nanowire film under the pressure of 0.5MPa to obtain the sandwich-structure lithium metal-copper-nickel nanowire composite negative electrode, wherein the thickness of the composite negative electrode piece is 15 mu m.
The prepared sandwich-structure lithium metal-copper nanowire composite cathode is assembled into a symmetrical battery to test the stability of the battery, the current density is 1mA, and the voltage hysteresis value after 1000 cycles of cycle is 10 mV.
The prepared sandwich-structure lithium metal-copper nanowire composite negative electrode is assembled into a full battery to be used as a negative electrode, a sulfur pole piece is used as a positive electrode, and the capacity of the battery after 200 cycles is measured to be kept at 1000 mAh.g -1 The coulombic efficiency was 99.3%.
In addition to the above embodiments, the present invention may have other embodiments. All technical solutions formed by adopting equivalent substitutions or equivalent transformations fall within the protection scope of the claims of the present invention.

Claims (9)

1. The utility model provides a sandwich structure metal composite negative pole piece for secondary battery which characterized in that: the current collector comprises an M metal sheet and metal nanowire layers adhered to the upper surface and the lower surface of the M metal sheet, wherein the metal nanowire layer adhered to one surface of the M metal sheet is directly used as a current collector, the M metal sheet is a lithium metal sheet, a sodium metal sheet or a magnesium metal sheet, the metal nanowire layer is composed of a group of metal nanowires adhered to the surface of the M metal sheet, the metal nanowires are arranged on the upper surface and the lower surface of the metal sheet in a free dispersion manner and form a metal nanowire network structure on the metal surface layer, and the metal nanowires are copper nanowires, nickel nanowires or copper-nickel nanowires; and pressing the metal nanowires on the upper surface and the lower surface of the M metal sheet in a pressurizing manner, wherein the applied pressure is 0.1-1 MPa, and the metal nanowire layers on the upper surface and the lower surface of the M metal sheet are the same in material.
2. The metal composite negative electrode sheet with a sandwich structure for a secondary battery according to claim 1, wherein: the M metal sheet is a lithium metal sheet, and the metal nanowire is a copper nanowire.
3. The metal composite negative electrode sheet with a sandwich structure for a secondary battery according to claim 2, wherein: the thickness of the lithium metal sheet is 10-500 mu m.
4. The metal composite negative electrode sheet with a sandwich structure for a secondary battery according to claim 2, wherein: the diameter of the copper nanowire is 50-100 nm, and the length of the copper nanowire is 50-200 mu m.
5. The metal composite negative electrode sheet with a sandwich structure for a secondary battery according to claim 1, wherein: the diameter of the nickel nanowire is 50-100 nm, and the length of the nickel nanowire is 50-100 mu m.
6. The metal composite negative electrode sheet with a sandwich structure for a secondary battery according to claim 1, wherein: the copper-nickel nanowire is formed by mixing a copper nanowire and a nickel nanowire, wherein the mass ratio of the copper nanowire to the nickel nanowire is (1-9): (1-9); the diameter of the copper nanowire is 50-100 nm, and the length of the copper nanowire is 50-200 mu m; the diameter of the nickel nanowire is 50-100 nm, and the length of the nickel nanowire is 50-100 mu m.
7. The metal composite negative electrode sheet with a sandwich structure for a secondary battery according to claim 1, wherein: the thickness of the metal composite negative plate with the sandwich structure is 10-500 mu m.
8. The metal composite negative electrode sheet with a sandwich structure for a secondary battery according to claim 7, wherein: the metal composite negative plate with the sandwich structure is used in a secondary battery.
9. The metal composite negative electrode sheet with a sandwich structure for a secondary battery according to claim 8, wherein: the secondary battery is a lithium metal battery, a sodium metal battery or a magnesium metal battery.
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CN112164804A (en) * 2020-09-29 2021-01-01 贵州梅岭电源有限公司 Preparation method of composite modified lithium metal soft package battery
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