CN109786667B - Composite polymer three-dimensional structure metal lithium electrode and lithium ion battery - Google Patents
Composite polymer three-dimensional structure metal lithium electrode and lithium ion battery Download PDFInfo
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- CN109786667B CN109786667B CN201711131776.7A CN201711131776A CN109786667B CN 109786667 B CN109786667 B CN 109786667B CN 201711131776 A CN201711131776 A CN 201711131776A CN 109786667 B CN109786667 B CN 109786667B
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention provides a composite polymer three-dimensional structure metal lithium electrode which is characterized by comprising a polymer film, an electronic conductive material, an ionic conductive material and metal lithium, wherein the electronic conductive material and the ionic conductive material are doped in the polymer film, the polymer film is of a porous structure, and the metal lithium is filled in pores of the polymer film. The composite polymer three-dimensional structure metal lithium electrode provided by the invention can be directly used as a negative electrode, and can effectively avoid the problem of lithium death; ion conduction can be carried out by bypassing the hollow shell structure collapsed by the cathode material after dead lithium is formed; compared with the traditional cathode, the cathode has small volume and lighter weight, and can greatly improve the volumetric specific energy density and the mass specific energy density of the battery. In addition, the lithium ion battery can also be used as a lithium supplement material of a negative electrode, uniform lithium supplement is carried out, and the first-cycle charge-discharge efficiency of the battery is improved.
Description
Technical Field
The invention relates to the technical field of batteries, in particular to a composite polymer three-dimensional structure metal lithium electrode and a lithium ion battery.
Background
Compared with other secondary batteries, the lithium ion battery has the advantages of high voltage, high energy density, long cycle life, good safety performance and the like, and becomes a rechargeable battery with the most extensive application, for example, as a power supply of portable electronic products, a power battery of large-scale mobile equipment such as electric automobiles and the like. The current mature battery cathode material is mainly a graphite material, and after years of development, the energy density of the battery cathode material is developed to be close to a theoretical value level (the theoretical specific capacity is 372 mAh/g), so that the further improvement of the energy density of the battery is limited, and the requirement of the battery for high energy density in the future cannot be met.
Compared with graphite negative electrodes, the lithium metal has the characteristics of low density (0.53g/cm3), low standard electrode potential (-3.04V) and high theoretical specific capacity (3860mAh/g), and the energy density of the battery can be obviously improved when the lithium metal is used as the negative electrode. However, the uneven deposition of lithium metal during charging and discharging of the metallic lithium negative electrode results in the generation of a large amount of lithium dendrites, which pierce the battery separator to cause short-circuiting of the battery, and generate a large amount of heat to cause accidents such as ignition and even explosion. In addition, the growth of lithium dendrites also makes it difficult to form a stable Solid Electrolyte Interface (SEI) film on the surface of the electrode, resulting in the consumption of a large amount of lithium, and if the lithium dendrites are broken, dead lithium is formed, resulting in low coulombic efficiency and rapid capacity fading during battery cycling. In addition, the lithium metal negative electrode has the problems of electrode volume expansion in the circulation process, easy initiation of material internal pressure change, interface fluctuation and the like.
In order to solve the problem of lithium dendrites in the metallic lithium negative electrode, the prior art modifies the surface properties of the metallic lithium negative electrode by using an electrolyte additive; however, the single modification effect cannot reach the practical standard, and the problems of capacity loss, internal resistance increase, poor electrochemical performance and the like are easily caused, so that the problems of dendritic crystal growth, low coulombic efficiency, poor battery cyclicity and the like caused by the metal lithium electrode cannot be fundamentally solved.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to provide a composite polymer three-dimensional structure metal lithium electrode which can be directly used as a negative electrode and can effectively avoid the problem of lithium death; ion conduction can be carried out by bypassing the hollow shell structure collapsed by the cathode material after dead lithium is formed; compared with the traditional cathode, the cathode has small volume and lighter weight, and can greatly improve the volumetric specific energy density and the mass specific energy density of the battery. In addition, the lithium ion battery can also be used as a lithium supplement material of a negative electrode, uniform lithium supplement is carried out, and the first-cycle charge-discharge efficiency of the battery is improved.
In order to achieve the purpose, the invention adopts the following specific technical scheme:
the invention provides a composite polymer three-dimensional structure metal lithium electrode which is characterized by comprising a polymer film, an electronic conductive material, an ionic conductive material and metal lithium, wherein the electronic conductive material and the ionic conductive material are doped in the polymer film, the polymer film is of a porous structure, and the metal lithium is filled in pores of the polymer film.
Further, the polymer film is made of any one of single-layer polypropylene (PP), single-layer Polyethylene (PE), double-layer PP/PE, double-layer PP/PP or three-layer PP/PE/PP, PET, PI, aramid fiber, plant fiber and the like.
Further, the electronic conducting material is one or more of carbon black, chrysene, acetylene black, Super P, graphene oxide, COF, MOF, single-wall or multi-wall carbon nano tubes, carbon fibers, conducting high polymer materials, conducting graphite, copper powder, aluminum powder, nickel, cobalt, titanium, iron, ruthenium dioxide and molybdenum dioxide.
Further, the ion conductive material may be an inorganic solid state electrolyte material.
Further, the ion conducting material may also be a polymeric single lithium ion conductor material.
Further, the ion conductive material may also be a mixture of the material of the polymer film and a lithium salt.
Further, the lithium salt is one or more of lithium hexafluorophosphate (LiPF 6), lithium hexafluoroarsenate (LiAsF 6), lithium perchlorate (LiClO 4), lithium fluoroborate (LiBF 4), lithium bis (fluorosulfonyl) imide (LiFSI), lithium bis (trifluoromethanesulfonyl) imide (LiTFSI), lithium trifluoromethanesulfonate (LiOTF), lithium dioxalate borate (LiBOB) and lithium difluorooxalate borate (LiODFB).
Further, the porosity of the polymer film is 40% -95%.
Further, the thickness of the composite polymer three-dimensional structure metal lithium electrode is 1-50 μm.
Further, the metal lithium is filled in the hole by evaporation.
Further, the porous structure of the polymer membrane is manufactured by a weaving process, a non-woven fabric process or a track etching process.
The invention also provides a lithium ion battery which comprises a positive electrode, a negative electrode, an electrolyte, a diaphragm and the composite polymer three-dimensional structure metal lithium electrode, wherein the composite polymer three-dimensional structure metal lithium electrode is used as a lithium supplement material of the negative electrode.
Further, the battery is a liquid battery or a solid battery.
The invention has the beneficial effects that: the composite polymer three-dimensional structure metal lithium electrode provided by the invention is simple to prepare, good in performance and low in cost;
1) the composite polymer three-dimensional structure metal lithium electrode disclosed by the invention contains the electron conductive material and the ion conductive material, has the electron and ion conduction functions, can be directly used as a negative electrode, and can effectively avoid the problem of lithium death; ion conduction can be carried out by bypassing the hollow shell structure collapsed by the cathode material after dead lithium is formed;
2) the composite polymer three-dimensional structure metal lithium electrode adopts the polymer film as the matrix, has smaller thickness and lighter weight compared with the traditional electrode, and can effectively improve the volumetric specific energy density and the mass specific energy density of the battery;
3) the composite polymer three-dimensional structure metal lithium electrode also contains metal lithium, and can be used as a lithium supplement material of a negative electrode, so that the lithium can be uniformly supplemented, and the first-cycle charge-discharge efficiency of the battery is improved.
Drawings
Fig. 1 is a schematic view of the microstructure of the composite polymer three-dimensional structure metal lithium electrode of the present invention.
1-polymer film, 2-metallic lithium.
Detailed Description
In order to make the technical solutions of the present invention better understood by those skilled in the art, the present invention will be further described in detail with reference to specific examples. Note that the following described embodiments are illustrative only for explaining the present invention, and are not to be construed as limiting the present invention.
As shown in fig. 1, the composite polymer three-dimensional structure metal lithium electrode provided by the invention comprises a polymer film 1, an electronic conductive material, an ionic conductive material and metal lithium, wherein the polymer film is used as a matrix, and the electronic conductive material and the ionic conductive material are doped in the polymer film and are uniformly distributed; the polymer film is of a porous structure, and metal lithium 2 is filled in pores of the polymer film.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, the polymer film is made of any one of single-layer polypropylene (PP), single-layer Polyethylene (PE), double-layer PP/PE, double-layer PP/PP or three-layer PP/PE/PP, PET, PI, aramid fiber, plant fiber and the like.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, the electronic conductive material is one or more of carbon black, chrysene, acetylene black, Super P, graphene oxide, COF, MOF, single-wall or multi-wall carbon nano tubes, carbon fibers, conductive polymer materials, conductive graphite, copper powder, aluminum powder, nickel, cobalt, titanium, iron, ruthenium dioxide and molybdenum dioxide.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, the ion conductive material can be an inorganic solid electrolyte material.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, the ion conductive material can also be a polymer single lithium ion conductor material.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, the ion conductive material can also be a mixture of the material of the polymer film and lithium salt.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, the lithium salt is one or more of lithium hexafluorophosphate (LiPF 6), lithium hexafluoroarsenate (LiAsF 6), lithium perchlorate (LiClO 4), lithium fluoroborate (LiBF 4), lithium bis (fluorosulfonyl) imide (LiFSI), lithium bis (trifluoromethanesulfonyl) imide (LiTFSI), lithium trifluoromethanesulfonate (LiOTF), lithium bis (LiBOB) oxalate and lithium difluoro (LiODFB).
When the polymer film is processed and manufactured, the molding material of the polymer film, the electronic conductive material and the ionic conductive material can be fully and uniformly mixed, so that the electronic conductive material and the ionic conductive material are uniformly distributed in the polymer film, and the polymer film has good electronic and ionic conduction functions. The material of the polymer film, the electron conductive material and the ion conductive material are not particularly limited, and may be appropriately selected according to actual needs.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, the porosity of the polymer film is 40-95%, and preferably 60-85%.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, the thickness of the composite polymer three-dimensional structure metal lithium electrode can be 1-50 μm, and is preferably 1-20 μm.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, metal lithium can be filled in the holes of the polymer film in an evaporation mode. By heating the lithium metal to an evaporation temperature, lithium metal vapor is passed through the polymeric membrane, and the vapor condenses within the pores of the polymeric membrane, thereby closing or filling the pores.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, the porous structure of the polymer film can be formed by processing through a weaving process and a non-woven fabric process during film preparation of the polymer film; or processing the hole by a track etching method after the film preparation is finished. The hole processing method is not particularly limited.
The composite polymer three-dimensional structure metal lithium electrode provided by the invention adopts the polymer film as the matrix, and compared with the traditional electrode containing copper foil, the thickness of the polymer film can be very small, for example 3 μm; meanwhile, the high molecular film material has lower density, so that the weight of the electrode is lighter, and the volumetric specific energy density and the mass specific energy density of the battery can be greatly improved.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, as the composite polymer three-dimensional structure metal lithium electrode has the electron and ion conduction functions, the composite polymer three-dimensional structure metal lithium electrode can be directly used as a negative electrode; due to the ion conduction function, the lithium ion conduction structure can bypass a hollow shell structure collapsed by a negative electrode material to conduct ion conduction after dead lithium is formed, so that the problem of the dead lithium is effectively solved; meanwhile, the composite polymer three-dimensional structure metal lithium electrode contains metal lithium and can also be used as a lithium supplement material of a negative electrode, after the lithium supplement is finished, the remaining material has no influence on the internal structure and performance of the battery along with the disappearance or reduction of the metal lithium, and the conduction of lithium ions between the positive electrode and the negative electrode can be ensured to be not influenced.
According to the composite polymer three-dimensional structure metal lithium electrode provided by the invention, due to the composite polymer three-dimensional structure with high specific surface area, the interface resistance can be reduced, the local current density can be reduced, the growth speed of dendrites can be reduced, the surface charge distribution can be regulated and controlled, and the deposition of lithium ions is more uniform. Meanwhile, the porous structure also has certain expansion resistance, so that the volume expansion of the metal lithium cathode is inhibited, and the reduction of internal pressure and interface fluctuation is facilitated.
The invention also provides a lithium ion battery manufactured by applying the composite polymer three-dimensional structure metal lithium electrode, and the lithium ion battery can be a liquid battery or a solid battery. When the composite polymer three-dimensional structure metal lithium electrode in the lithium ion battery is directly used as a negative electrode, the hollow shell structure collapsed by a negative electrode material can be bypassed for ion conduction, and the problem of lithium death is effectively inhibited; the battery has light weight and small volume, and effectively improves the volumetric specific energy density and the mass specific energy density of the battery, thereby greatly improving the performance of the battery. When the composite polymer three-dimensional structure metal lithium electrode in the lithium ion battery is used as a lithium supplement material, the purpose of uniformly supplementing lithium can be achieved, and the first-cycle charge-discharge efficiency of the battery is greatly improved.
Under the same experimental conditions, the composite polymer three-dimensional structure metal lithium electrode provided by the invention has good lithium stability and electrochemical stability; uniform lithium ion deposition, excellent cycle stability, high safety, and long life are achieved during cycling. Compared with other batteries in the prior art, the cycle performance of the lithium ion battery manufactured by applying the composite polymer three-dimensional structure metal lithium electrode can be improved by about 10%.
In conclusion, the composite polymer three-dimensional structure metal lithium electrode provided by the invention can be directly used as a negative electrode, so that the problem of lithium death can be effectively avoided; ion conduction can be carried out by bypassing the hollow shell structure collapsed by the cathode material after dead lithium is formed; compared with the traditional electrode, the battery has smaller thickness and lighter weight, and can effectively improve the volumetric specific energy density and the mass specific energy density of the battery. In addition, the lithium ion battery can also be used as a lithium supplement material between a positive electrode and a negative electrode, can uniformly supplement lithium, and improves the first-cycle charge-discharge efficiency of the battery; has the outstanding advantages of excellent performance, strong practicability, low cost and the like. In a word, the invention provides the composite polymer three-dimensional structure metal lithium electrode which is simple in structure and strong in practicability, can realize large-scale application, and has wide application prospects.
In the description of the present invention, it is to be understood that the terms "first", "second" and the like are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implying any number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature. In the description of the present invention, "a plurality" means two or more unless specifically defined otherwise.
In the present invention, unless otherwise expressly stated or limited, the terms "mounted," "connected," "secured," and the like are to be construed broadly and can, for example, be fixedly connected, detachably connected, or integrally formed; can be mechanically or electrically connected; either directly or indirectly through intervening media, either internally or in any other relationship. The specific meanings of the above terms in the present invention can be understood by those skilled in the art according to specific situations.
Although embodiments of the present invention have been shown and described, it is understood that the embodiments are illustrative and not restrictive, that various changes, modifications, substitutions and alterations may be made herein without departing from the spirit and scope of the invention as defined by the appended claims.
Claims (10)
1. The composite polymer three-dimensional structure metal lithium electrode is characterized by comprising a polymer film, an electronic conductive material, an ionic conductive material and metal lithium, wherein the electronic conductive material and the ionic conductive material are doped in the polymer film, the polymer film is of a porous structure, and the metal lithium is filled in pores of the polymer film;
the porosity of the polymer film is 40% -95%;
the metal lithium is filled in the holes through evaporation;
the porous structure of the polymer film is prepared by a weaving process, a non-woven fabric process or a track etching process.
2. The composite polymeric three-dimensional structure metal lithium electrode according to claim 1, wherein the polymeric film is made of any one of a single layer polypropylene (PP), a single layer Polyethylene (PE), a double layer PP/PE, a double layer PP/PP or a triple layer PP/PE/PP, PET, PI, aramid, and plant fiber.
3. The composite polymeric three-dimensional structure metal lithium electrode according to claim 1, wherein the electron conductive material is one or more of carbon black, graphene oxide, COF, MOF, single-walled or multi-walled carbon nanotubes, carbon fibers, conductive polymer materials, conductive graphite, copper powder, aluminum powder, nickel, cobalt, titanium, iron, ruthenium dioxide, and molybdenum dioxide.
4. The composite polymeric three-dimensional structure metal lithium electrode according to claim 1, wherein the ionic conductive material is an inorganic solid electrolyte material.
5. The composite polymeric three-dimensional structure metal lithium electrode according to claim 1, wherein the ionic conductive material is a polymeric single lithium ion conductor material.
6. The composite polymeric three-dimensional structure metal lithium electrode according to claim 1, wherein the ionic conductive material is a mixture of a material of the polymeric membrane and a lithium salt.
7. The lithium metal electrode with a composite polymer three-dimensional structure according to claim 6, wherein the lithium salt is lithium hexafluorophosphate (LiPF)6) Lithium hexafluoroarsenate (LiAsF)6) Lithium perchlorate (LiClO)4) Lithium fluoroborate (LiBF)4) One or more of lithium bis (fluorosulfonyl) imide (LiFSI), lithium bis (trifluoromethanesulfonyl) imide (LiTFSI), lithium trifluoromethanesulfonate (LiOTF), lithium dioxalate borate (LiBOB) and lithium difluorooxalate borate (LiODFB).
8. The lithium metal electrode with the composite polymer three-dimensional structure according to claim 1, wherein the thickness of the lithium metal electrode with the composite polymer three-dimensional structure is 1-50 μm.
9. A lithium ion battery comprising a positive electrode, a negative electrode, an electrolyte and a separator, wherein the lithium ion battery further comprises the composite polymer three-dimensional structure metal lithium electrode according to any one of claims 1 to 8, and the composite polymer three-dimensional structure metal lithium electrode is used as a lithium supplement material of the negative electrode.
10. The lithium ion battery of claim 9, wherein the battery is a liquid battery or a solid state battery.
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| CN113782823B (en) * | 2021-08-12 | 2023-07-04 | 浙江锋锂新能源科技有限公司 | Preparation method of lithium supplementing functional electrolyte membrane for solid-state lithium battery |
| CN113764667B (en) * | 2021-08-12 | 2023-07-14 | 浙江锋锂新能源科技有限公司 | Lithium supplementing functional electrolyte membrane for solid lithium battery |
| CN114583302B (en) * | 2022-05-05 | 2022-08-02 | 华中科技大学 | MOF-based monatomic lithium-supplement composite material, preparation method thereof, positive electrode material and battery |
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