CN114050272A - Graphene substrate and thin film lithium battery with same - Google Patents
Graphene substrate and thin film lithium battery with same Download PDFInfo
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- CN114050272A CN114050272A CN202111363592.XA CN202111363592A CN114050272A CN 114050272 A CN114050272 A CN 114050272A CN 202111363592 A CN202111363592 A CN 202111363592A CN 114050272 A CN114050272 A CN 114050272A
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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
- H01M10/36—Accumulators not provided for in groups H01M10/05-H01M10/34
- H01M10/38—Construction or manufacture
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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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
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- 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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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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Abstract
A graphene substrate and a thin film lithium battery with the same are provided. The thickness of the graphene substrate is 0.5-10 μm, and the square resistance value of the graphene substrate is 0.1-2 omega/sq. The graphene substrate has extremely high conductivity, excellent mechanical strength and mechanical property, excellent thermal stability and super chemical stability, so when the graphene substrate is applied to a thin film lithium battery, perfect matching with a solid positive electrode material and a solid negative electrode material can be realized simultaneously, and the electrochemical corrosion defect of other metal collecting electrodes in the process of charging and discharging the battery for many times can be avoided. As an excellent adhesion substrate of a solid positive electrode material and a solid negative electrode material, the graphene substrate provided by the invention can provide an ultra-strong bonding force with the positive electrode material and the negative electrode material, and does not have any influence on normal vapor deposition of the positive electrode material, the solid electrolyte material and the negative electrode material of the thin film lithium battery.
Description
Technical Field
The invention relates to the field of large-scale energy storage and power energy, in particular to a graphene substrate and a thin film lithium battery with the graphene substrate.
Background
An all-solid-state lithium battery is also called an all-solid-state lithium secondary battery, that is, a lithium secondary battery in which each unit of the battery includes an anode, a cathode, and an electrolyte, all of which are made of solid materials. The structure of the all-solid-state lithium battery is simpler than that of the traditional lithium ion battery, the solid electrolyte not only conducts lithium ions, but also plays the role of a diaphragm, and the all-solid-state lithium battery has the advantages of high mechanical strength, no flammable and volatile components, no liquid leakage hidden danger, good temperature resistance and the like. The all-solid-state lithium battery can be made of inorganic materials, large-scale preparation is easy to realize so as to meet the requirement of a large-size battery, and the structural composition of the battery is simpler.
However, since the solid materials have certain rigidity and strength, when the battery is formed, the contact surfaces of different solid materials cannot be completely attached to each other without gaps, so that the contact surface resistance of the all-solid-state lithium battery is very high, and the performance of the battery is significantly reduced, which causes the energy density, specific energy, specific power, energy efficiency and energy conservation rate of the all-solid-state battery to be limited.
The inventors have recognized that the introduction of thin film fabrication techniques into an all solid-state lithium battery, to form an all solid-state battery in thin film form, can completely avoid the problem of interfacial contact within the battery. However, thin film lithium batteries require a suitable substrate. The common flexible plastic base material is non-conductive and not high temperature resistant, and has weak bonding force with the anode, the cathode and the like of the thin film lithium battery. The surfaces of common aluminum foils and copper foils are easy to oxidize, which can generate adverse effect on the binding force between the aluminum foils and the copper foils and the positive electrode, the negative electrode and the like of the thin film lithium battery, and cause large change of interface resistance. How to prepare a suitable substrate becomes a technical problem to be solved urgently by those skilled in the art.
The above information disclosed in this background section is only for enhancement of understanding of the background of the application and therefore it may comprise prior art that does not constitute known to a person of ordinary skill in the art.
Disclosure of Invention
An object of the present invention is to provide a graphene-based substrate and a thin film lithium battery having the same, which at least partially solve the above problems.
A further object of the present invention is to provide a novel graphene substrate for a thin film lithium battery, especially for a scheme of preparing an all-solid-state thin film lithium battery by a magnetron sputtering coating method.
Particularly, according to an aspect of the present invention, a graphene substrate for a thin film lithium battery is provided, wherein the thickness of the graphene substrate is 0.5 to 10 μm, and the sheet resistance of the graphene substrate is 0.1 to 2 Ω/sq.
Optionally, the graphene substrate is configured to be coated or grown on a collector substrate, the collector substrate is a flexible film material, and the flexible film material is a plastic film, a copper foil, an aluminum foil, or a carbon nanotube.
Optionally, the graphene substrate is configured to deposit thereon a positive electrode material, a negative electrode material, a collector material, or a current collector material of the thin film lithium battery.
Optionally, the interface resistance between the graphene substrate and the positive electrode material of the thin film lithium battery is 0.1-2 Ω.
Optionally, the interface resistance between the graphene substrate and the negative electrode material of the thin film lithium battery is 0.1-2 Ω
Optionally, the interface resistance between the graphene substrate and the collector material of the thin film lithium battery is 0.1-0.3 Ω.
Optionally, the interface resistance between the graphene substrate and the current collector material of the thin film lithium battery is 0.1-0.3 Ω.
According to another aspect of the present invention, there is also provided a thin film lithium battery including: a graphene substrate according to any one of the preceding claims.
Optionally, the thin film lithium battery further comprises: a negative electrode material, a solid state electrolyte material, a positive electrode material, a current collector material, and/or a current collector material deposited on the graphene substrate.
According to the graphene substrate and the thin film lithium battery with the graphene substrate, the graphene substrate has extremely high conductivity, excellent mechanical strength and mechanical property, excellent thermal stability and super chemical stability, so that when the graphene substrate is applied to the thin film lithium battery, perfect matching with a solid positive electrode material and a solid negative electrode material can be simultaneously realized, and the electrochemical corrosion defect of other metal collecting electrodes in the process of charging and discharging the battery for many times can be avoided. As an excellent adhesion substrate of a solid positive electrode material and a solid negative electrode material, the graphene substrate provided by the invention can provide an ultra-strong bonding force with the positive electrode material and the negative electrode material, and does not have any influence on normal vapor deposition of the positive electrode material, the solid electrolyte material and the negative electrode material of the thin film lithium battery.
Furthermore, based on the graphene substrate, each layer of thin film material of the thin film lithium battery is deposited on the graphene substrate, so that the graphene substrate has excellent interface binding property and coordination, has very low interface internal resistance, reduces the contact surface resistance, is beneficial to improving the energy density, specific energy, specific power, energy efficiency and energy conservation rate of the battery, is also beneficial to improving the structural stability of the battery, reduces or avoids the internal structure cracking of the battery, and prolongs the service life of the battery.
The above and other objects, advantages and features of the present invention will become more apparent to those skilled in the art from the following detailed description of specific embodiments thereof, taken in conjunction with the accompanying drawings.
Drawings
Some specific embodiments of the invention will be described in detail hereinafter, by way of illustration and not limitation, with reference to the accompanying drawings. The same reference numbers in the drawings identify the same or similar elements or components. Those skilled in the art will appreciate that the drawings are not necessarily drawn to scale. In the drawings:
fig. 1 is a schematic view of a graphene substrate according to one embodiment of the present invention;
fig. 2 is a schematic view of a thin film lithium battery according to one embodiment of the present invention.
Detailed Description
Fig. 1 is a schematic diagram of a graphene substrate 120 according to one embodiment of the present invention.
In the present embodiment, the thickness of the graphene substrate 120 is 0.5 to 10 μm, and may be, for example, 0.5 μm, 1 μm, 5 μm, or 10 μm.
The sheet resistance value of the graphene substrate 120 is 0.1-2 Ω/sq, and may be, for example, 0.1 Ω/sq, 0.5 Ω/sq, 1 Ω/sq, or 2 Ω/sq.
By comprehensively designing the thickness and the square resistance of the graphene substrate 120, the graphene substrate 120 can be compatible with other layers of thin film materials of the thin film lithium battery 10 in good physical and chemical properties, maintain good interface consistency, reduce the interface resistance, and maintain the interface resistance within a reasonable range, thereby improving the performance of the thin film lithium battery 10.
Since the graphene substrate 120 has very high electrical conductivity, excellent mechanical strength and mechanical properties, and also has excellent thermal stability and super chemical stability, when the graphene substrate is applied to the thin film lithium battery 10 and serves as a collector, perfect matching with the solid positive electrode material 150 and the solid negative electrode material 130 can be simultaneously realized, and the electrochemical corrosion defect of other metal collectors in the multiple charging and discharging processes of the battery can be avoided. As an excellent adhesion substrate for the solid-state cathode material 150 and the solid-state anode material 130, the graphene substrate 120 of the present invention can provide an ultra-strong bonding force with the cathode material 150 and the anode material 130, without any influence on the normal vapor deposition of the cathode material 150, the solid-state electrolyte material 140, and the anode material 130 of the thin-film lithium battery 10.
In some alternative embodiments, the graphene substrate 120 is configured to be coated or grown on the collector substrate 110. The collector substrate 110 is a flexible film material, and the flexible film material is a plastic film, a copper foil, an aluminum foil, or a carbon nanotube. That is, the material of the collector substrate 110 may be a plastic film, a copper foil, an aluminum foil, or a carbon nanotube or other soft film material.
The graphene substrate 120 is formed by a coating or growing method, so that the bonding force between the graphene substrate 120 and the collector substrate 110 can be improved, and the structural stability can be improved. By coating or growing the graphene substrate 120 on the collector substrate 110, the thickness and sheet resistance value of the graphene substrate 120 may be easily adjusted.
In some alternative embodiments, graphene substrate 120 is configured to have deposited thereon positive electrode material 150, negative electrode material 130, collector material 120, or current collector material 160 of thin film lithium battery 10. That is, the cathode material 150, the anode material 130, the collector material 120, or the collector material 160 may be selectively deposited on the graphene substrate 120. For example, in the process of preparing a single thin film lithium battery 10, the negative electrode material 130 may be deposited first, then the solid electrolyte material 140 is deposited, then the positive electrode material 150, the current collector material 160, the current collector material 120, and the like are deposited, and in the process of preparing a plurality of thin film lithium batteries 10 connected in series (or connected in parallel), the steps of depositing the negative electrode material 130, the solid electrolyte material 140, the positive electrode material 150, and the current collector material 120 may be repeatedly performed according to the structure of the series (or connected in parallel) batteries, and the current collector material 160 is deposited.
According to the graphene substrate 120 disclosed by the invention, each layer of thin film material of the thin film lithium battery 10 is deposited on the graphene substrate 120, so that the graphene substrate 120 has excellent interface binding property and coordination property, has very low interface internal resistance, reduces the contact surface resistance, is beneficial to improving the energy density, specific energy, specific power, energy efficiency and energy conservation rate of the battery, is also beneficial to improving the structural stability of the battery, reduces or avoids the internal structure cracking of the battery, and prolongs the service life of the battery.
The interface resistance between the graphene substrate 120 and the positive electrode material 150 of the thin film lithium battery 10 is 0.1-2 Ω. The graphene substrate 120 can achieve good physical and chemical compatibility with the positive electrode material 150 of any thin film lithium battery 10, and maintain good interface consistency. The graphene substrate 120 of the present embodiment can ensure that the interfacial resistance value between the graphene substrate and the positive electrode material 150 of any thin film lithium battery 10 is within a range of 0.1 to 2 Ω.
The interface resistance between the graphene substrate 120 and the negative electrode material 130 of the thin film lithium battery 10 is 0.1-2 Ω. The graphene substrate 120 can achieve good physical and chemical compatibility with the negative electrode material 130 of any thin film lithium battery 10, and maintain good interface consistency. The graphene substrate 120 of the present embodiment can ensure that the interface resistance value between the graphene substrate and the negative electrode material 130 of any thin film lithium battery 10 is within a range of 0.1 to 2 Ω.
The interface resistance between the graphene substrate 120 and the collector material 120 of the thin film lithium battery 10 is 0.1-0.3 Ω. The graphene substrate 120 can achieve good physical and chemical compatibility with the collector material 120 of any thin film lithium battery 10, and maintain good interface consistency. The graphene substrate 120 of the present embodiment can ensure that the interface resistance value between the graphene substrate 120 and the collector material 120 of any thin film lithium battery 10 is within a range of 0.1 to 0.3 Ω.
The interface resistance between the graphene substrate 120 and the current collector material 160 of the thin film lithium battery 10 is 0.1-0.3 Ω. The graphene substrate 120 can achieve good physical and chemical compatibility with the current collector material 160 of any thin film lithium battery 10, and maintain good interface consistency. The graphene substrate 120 of the present embodiment can ensure that the interfacial resistance value between the graphene substrate and the current collector material 160 of any thin film lithium battery 10 is within a range of 0.1 to 0.3 Ω.
Fig. 2 is a schematic diagram of a thin film lithium battery 10 according to one embodiment of the present invention. The thin film lithium battery 10 of the present embodiment includes the graphene substrate 120 as in any of the above embodiments. The graphene substrate 120 may serve as a collector of the thin film lithium battery 10.
The thin film lithium battery 10 may further include a negative electrode material 130, a solid state electrolyte material 140, a positive electrode material 150, a current collector material 160, and/or a current collector material 120 deposited on the graphene substrate 120.
Fig. 2 shows the structure of a single-segment thin film lithium battery 10, where the thin film lithium battery 10 includes a graphene substrate 120, and a negative electrode material 130, a solid electrolyte material 140, a positive electrode material 150, a current collector material 160, and a current collector material 120 sequentially deposited on the graphene substrate 120. The graphene substrate 120 is attached on the collector substrate 110. For example, the positive electrode material 150 may be a lithium cobaltate positive electrode thin film 150 or a lithium manganate positive electrode thin film 150, the solid electrolyte material 140 may be a lithium phosphate solid electrolyte thin film 140, the negative electrode material 130 may be a tin alloy negative electrode thin film 130, the collector material 120 may be a graphene collector thin film 120, and the collector material 160 may be copper or aluminum. Here, the method of depositing the collector material 120 is the same as the method of forming the graphene substrate 120, and thus fig. 2 is illustrated with the same drawing numbers. The arrows in fig. 2 show the sequence of the formation of the layers of the film.
It should be noted that fig. 2 only illustrates the structure of a single thin film lithium battery 10, and those skilled in the art should understand that these embodiments can be easily extended and changed, and all such extensions and changes are within the scope of the present invention.
As to the method of manufacturing the thin film lithium battery 10, it will be further explained in accordance with the following examples 1 to 3.
Example 1:
the graphene substrate 120 prepared by the method is used for depositing the single-section graphene-based thin film lithium battery 10 by adopting a magnetron sputtering coating technology: a graphene substrate 120 with a thickness of 6 μm is coated on a surface of a copper foil of 1 square meter, and a negative electrode thin film 130, a solid electrolyte thin film 140, a positive electrode thin film 150, and a graphene collector thin film 120 are sequentially deposited on the graphene substrate 120. Wherein the thickness of the deposited negative electrode thin film 130 is 4.5 μm, the thickness of the deposited solid electrolyte thin film 140 is 1.5 μm, and the thickness of the deposited positive electrode thin film 150 is 15 μm. The thickness of the graphene collector electrode thin film 120 was 6 μm. The capacity of the resultant battery after formation was 12240(mA · h).
Example 2:
the graphene substrate 120 prepared by the method is used for depositing two graphene-based thin film lithium batteries 10 connected in series by adopting a magnetron sputtering coating technology: a graphene substrate 120 with a thickness of 7 μm is coated on a copper foil surface of 1 square meter, and a negative electrode thin film 130, a solid electrolyte thin film 140, a positive electrode thin film 150, a graphene collector thin film 120, a negative electrode thin film 130, a solid electrolyte thin film 140, a positive electrode thin film 150, and a graphene collector thin film 120 are sequentially deposited on the graphene substrate 120. The thickness of the deposited negative electrode film 130 of each battery is 5.5 μm, the thickness of the deposited solid electrolyte film 140 of each battery is 2.0 μm, the thickness of the deposited positive electrode film 150 of each battery is 18.5 μm, and the thickness of the deposited graphene collector electrode film 120 of each battery is 7 μm. The capacity of the resultant battery after formation was 15096(mA · h).
Example 3:
the graphene substrate 120 prepared by the method is used for depositing two sections of graphene-based thin film lithium batteries 10 connected in parallel by adopting a magnetron sputtering coating technology: a graphene substrate 120 with a thickness of 7 μm is coated on a copper foil surface of 1 square meter, and a negative electrode thin film 130, a solid electrolyte thin film 140, a positive electrode thin film 150, a graphene collector thin film 120, a positive electrode thin film 150, a solid electrolyte thin film 140, a negative electrode thin film 130, and a graphene collector thin film 120 are sequentially deposited on the graphene substrate 120. The thickness of the deposited negative electrode film 130 of each battery is 6.5 μm, the thickness of the deposited solid electrolyte film 140 of each battery is 2.5 μm, the thickness of the deposited positive electrode film 150 of each battery is 22 μm, and the thickness of the deposited graphene collector electrode film 120 of each battery is 7 μm. The capacity of the resultant battery after formation was 35904(mA · h).
In the above examples 1 to 3, the cathode thin film 150, the solid electrolyte thin film 140, and the anode thin film 130 were all prepared by the magnetron sputtering method. For example, the positive electrode thin film 150 may be lithium cobaltate, the negative electrode thin film 130 may be a tin alloy, and the solid electrolyte thin film 140 may be lithium phosphate. The graphene collector film 120 is formed by coating or growing. Since the graphene collector thin film 120 and the graphene substrate 120 are both graphene thin films, they are denoted by the same reference numerals.
According to the graphene substrate 120 disclosed by the invention, each layer of thin film material of the thin film lithium battery 10 is deposited on the graphene substrate 120, so that the graphene substrate 120 has excellent interface binding property and coordination property, has very low interface internal resistance, reduces the contact surface resistance, is beneficial to improving the energy density, specific energy, specific power, energy efficiency and energy conservation rate of the battery, is also beneficial to improving the structural stability of the battery, reduces or avoids the internal structure cracking of the battery, and prolongs the service life of the battery.
Thus, it should be appreciated by those skilled in the art that while a number of exemplary embodiments of the invention have been illustrated and described in detail herein, many other variations or modifications consistent with the principles of the invention may be directly determined or derived from the disclosure of the present invention without departing from the spirit and scope of the invention. Accordingly, the scope of the invention should be understood and interpreted to cover all such other variations or modifications.
Claims (9)
1. A graphene substrate of a thin film lithium battery is characterized in that,
the thickness of the graphene substrate is 0.5-10 mu m, and the square resistance value of the graphene substrate is 0.1-2 omega/sq.
2. The graphene substrate according to claim 1,
the graphene substrate is configured to be coated or grown on a collector substrate, the collector substrate is a soft film material, and the soft film material is a plastic film, a copper foil, an aluminum foil or a carbon nanotube.
3. The graphene substrate according to claim 1,
the graphene substrate is configured to deposit thereon a positive electrode material, a negative electrode material, a collector material, or a current collector material of a thin film lithium battery.
4. The graphene substrate according to claim 1,
the interface resistance between the graphene substrate and the positive electrode material of the thin-film lithium battery is 0.1-2 omega.
5. The graphene substrate according to claim 1,
the interface resistance between the graphene substrate and the negative electrode material of the thin-film lithium battery is 0.1-2 omega.
6. The graphene substrate according to claim 1,
the interface resistance between the graphene substrate and the collector material of the thin film lithium battery is 0.1-0.3 omega.
7. The graphene substrate according to claim 1,
the interface resistance between the graphene substrate and a current collector material of the thin-film lithium battery is 0.1-0.3 omega.
8. A thin film lithium battery comprising:
the graphene substrate of any one of claims 1-7.
9. The thin film lithium battery of claim 8 further comprising:
a negative electrode material, a solid state electrolyte material, a positive electrode material, a current collector material, and/or a current collector material deposited on the graphene substrate.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114927765A (en) * | 2022-05-18 | 2022-08-19 | 鄂尔多斯市紫荆创新研究院 | All-solid-state battery and preparation method thereof |
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