Dielectric films for all-solid and semi-solid lithium batteries

Abstract

We provide dielectric films for all-solid-state and semi-solid-state lithium batteries. [Solution] The dielectric film for all-solid and semi-solid lithium batteries comprises a first film layer connected to the positive electrode of the lithium battery, a third film layer connected to the negative electrode of the lithium battery, and a second film layer connected between them. The first film layer includes a first polymer material used in part as a plasticizer and a first lithium salt dispersed in the first polymer material. The second film layer includes a second polymer material used in part as a plasticizer, a second lithium salt dispersed in the second polymer material, and a second inorganic ceramic dispersed in the second polymer material. The third film layer includes a third polymer material used in part as a plasticizer, a third lithium salt dispersed in the third polymer material, and a third inorganic ceramic dispersed in the third polymer material.

Description

Technical Field

[0001] The present invention relates to a dielectric film for a battery, and more particularly to a dielectric film for all-solid and semi-solid lithium batteries.

Background Art

[0002] Solid and semi-solid battery structures in the prior art are composed of a negative electrode, a positive electrode, and a dielectric film located between the positive electrode and the negative electrode. The negative electrode is filled with a negative electrode slurry as a binder and a plurality of negative electrode particles distributed in the negative electrode slurry. The positive electrode is filled with a positive electrode slurry as a binder and a plurality of positive electrode particles distributed in the positive electrode slurry. The dielectric film is used to isolate and bond the negative electrode and the positive electrode.

Summary of the Invention

Problems to be Solved by the Invention

[0003] In conventional solid or semi-solid electrolytes, the positive electrode slurry and the negative electrode slurry are used to guide lithium ions. However, the positive electrode slurry and the negative electrode slurry are likely to cause side reactions with lithium ions staying in the positive electrode slurry and the negative electrode slurry, resulting in dead lithium and lithium consumption. This is an irreversible chemical reaction. As the number of lithium ions in the battery decreases, the power storage capacity of the battery decreases. In addition, due to the low lithium ion capacity of the plurality of positive electrode particles and negative electrode particles in the positive electrode slurry and the negative electrode slurry, lithium ions in the positive electrode slurry and the negative electrode slurry are likely to concentrate on the surfaces of the positive electrode particles and the negative electrode particles, causing side reactions between these lithium ions and molecules in the positive electrode slurry and the negative electrode slurry. After long-term use, the capacitances of the positive electrode and the negative electrode decrease, the quantity of lithium ions decreases due to side reactions, and the power storage capacity of the battery decreases.

[0004] Furthermore, conventional dielectric films have a single-layer structure, are biased towards a rigid structure, and have a low lithium salt concentration. As a result, when bonding the dielectric film to the positive electrode, the lamination between them is not tightly bonded, leading to a decrease in the overall structure and bonding strength. In addition, conventional dielectric film materials cannot fill the gaps between them, making them prone to short circuits and reducing yield.

[0005] Furthermore, conventional single-layer dielectric films contain lithium salts at only a specific single concentration, resulting in a high required conduction energy level for lithium ions, low ionic conductivity, and a decrease in overall battery performance. When a single-layer dielectric film is bonded to the negative electrode, its low ionic conductivity makes it prone to dead lithium deposition on the negative electrode, increasing the formation of lithium crystals, raising the risk of puncture, and reducing the battery's energy storage capacity.

[0006] Therefore, the inventors believed that the above-mentioned shortcomings could be improved, and after diligent research, arrived at the present invention, which effectively improves the above-mentioned problems through a rational design.

[0007] This invention has been made in view of these circumstances, and its objective is to provide dielectric films for all-solid-state and semi-solid-state lithium batteries. [Means for solving the problem]

[0008] To solve the above problems, the present invention employs the following means. That is, A dielectric film for all-solid and semi-solid lithium batteries according to one aspect of the present invention is provided, wherein the lithium battery comprises a negative electrode and a positive electrode, the dielectric film is located between the positive electrode and the negative electrode, the negative electrode is filled with a negative electrode slurry and a plurality of negative electrode particles as a binder, the positive electrode is filled with a positive electrode slurry and a plurality of positive electrode particles as a binder, and the dielectric film is provided, It includes a first film layer, a second film layer, and a third film layer, wherein the first film layer is connected to the positive electrode, the third film layer is connected to the negative electrode, and the second film layer is connected between the first film layer and the third film layer. The first film layer is A first polymer material used as a substrate for the first film layer, wherein the first polymer material is a mixture of PVDF-HFP (Polyvinylidene luoride - hexafluoropropylene copolymer), ADN (Adiponitrile), GLN (Glutaronitrile), and SN (Succinonitrile), wherein the ADN, GLN, and SN of the first polymer material are used as plasticizers and are dispersed in the PVDF-HFP, and their function is to disperse the entire first polymer material, thereby reducing the precipitation of crystalline material in the first polymer material, assisting in the dissociation of lithium salts, allowing the first film layer to easily conduct lithium ions, and facilitating plastic processing. The first lithium salt dispersed in the first polymer material comprises a first lithium salt which is a mixture of LiBOB (LiB(C2O4)2, Lithium bis(oxalate)borate), LiTFSI (LiN(CF3SO2)2, Lithium bis(trifluoromethanesulfonyl)imide), and LiFSI (F2LiNO4S2, Lithium bis(fluorosulfonyl)imide), The second film layer is A second polymer material used as a substrate for the second film layer, wherein the second polymer material is a mixture of PVDF-HFP, PAN (Polyacrylonitrile), and SN, and the PAN and SN of the second polymer material are used as plasticizers and are dispersed in the PVDF-HFP, and the PAN and SN are used to assist in the dissociation of the lithium salt of the second film layer and to increase the ionic conductivity of the second polymer material, A second lithium salt dispersed in the second polymer material, wherein the second lithium salt comprises a second lithium salt containing LiFSI and LiTSFI, The second inorganic ceramic dispersed in the second polymer material is a plurality of first LLZO particles coated on the outside with a first dopamine layer, and each of the first LLZO particles is lithium lanthanum zirconium oxide (Li7La3Zr2O 12 ) or a second inorganic ceramic composed of lithium lanthanum zirconium oxide doped with at least one metallic element, The third film layer is A third polymer material used as a substrate for the third film layer, wherein the third polymer material is a mixture of PEO (Poly(ethylene Oxide)) and PAN, the PEO has high stability at the reduction potential of the negative electrode and moderate ionic conductivity, the PAN has good electronic and ionic conductivity and further improves the overall performance of the PEO, the PAN of the third polymer material is used as a plasticizer, and the third polymer material dispersed in the PEO, A third lithium salt dispersed in the third polymer material, wherein the third lithium salt is a LiTFSI, A third inorganic ceramic dispersed in the third polymer material, wherein the third inorganic ceramic is a plurality of second LLZO particles coated on the outside with a second dopamine layer, and each of the second LLZO particles is lithium lanthanum zirconium oxide (Li7La3Zr2O 12 The third inorganic ceramic is composed of lithium lanthanum zirconium oxide doped with at least one metallic element, and the third inorganic ceramic is used to enhance ionic conductivity. [Effects of the Invention]

[0009] The present invention forms a three-layer dielectric film by adding a first film layer and a third film layer to both sides of a conventional single-layer dielectric film. Since the first and third film layers have a flexible structure, they can fill the gap between the positive and negative electrodes of a lithium battery, improving the gap when adhering to the positive and negative electrodes, enhancing battery performance, reducing the risk of short circuits, and improving battery yield.

[0010] The following information will become clear from the description in the specification and drawings described later. [Brief explanation of the drawing]

[0011] [Figure 1] This is an explanatory diagram showing a dielectric film for all-solid and semi-solid lithium batteries according to one embodiment of the present invention. [Figure 2] This is a schematic diagram showing a dielectric film for all-solid and semi-solid lithium batteries according to one embodiment of the present invention. [Figure 3] This is a schematic diagram showing a first LLZO particle according to one embodiment of the present invention. [Figure 4] This is a schematic diagram showing a second LLZO particle according to one embodiment of the present invention. [Modes for carrying out the invention]

[0012] Embodiments of the present invention will be described in detail below. However, the present invention is not limited thereto, and various modifications are possible within the scope described. Embodiments obtained by appropriately combining the technical means disclosed in different embodiments are also included within the technical scope of the present invention.

[0013] First, embodiments of the dielectric film 30 for all-solid and semi-solid lithium batteries according to the present invention will be described with reference to Figures 1 to 4. The lithium battery comprises a negative electrode 10 and a positive electrode 20, and as shown in Figure 2, the dielectric film 30 according to the present invention is located between the positive electrode 20 and the negative electrode 10. The negative electrode 10 is filled with a negative electrode slurry 12 as a binder and a plurality of negative electrode particles 15 (for example, SiC (silicon carbide) particles having a tin layer) distributed within the negative electrode slurry 12. The outer surface of the negative electrode particles 15 has the function of accommodating lithium ions and allowing lithium ions in the negative electrode to flow evenly. The negative electrode particles 15 cause a partial side reaction with lithium ions, reducing the number of usable lithium ions and, in the long term, reducing the overall capacitance of the battery. The positive electrode 20 is filled with a positive electrode slurry 22 as a binder and a plurality of positive electrode particles 26 distributed within the positive electrode slurry 22. The positive electrode slurry 22 and the positive electrode particles 26 generate side reactions with passing lithium ions, thus consuming the available lithium ions.

[0014] In this case, as shown in Figures 1 and 2, the dielectric film 30 of the present invention is located between the negative electrode 10 and the positive electrode 20 and is used to isolate and join the negative electrode 10 and the positive electrode 20. The dielectric film 30 comprises a first film layer 31, a second film layer 32, and a third film layer 33. The first film layer 31 is connected to the positive electrode 20, the third film layer 33 is connected to the negative electrode 10, and the second film layer 32 is connected between the first film layer 31 and the third film layer 33.

[0015] The first film layer mainly comprises the following components. Each component will be described below.

[0016] First, the first polymer material 311 serves as the base material of the first film layer 31. The first polymer material is a mixture of PVDF-HFP (Polyvinylidene luoride-hexafluoropropylene copolymer), ADN (Adiponitrile), GLN (Glutaronitrile), and SN (Succinonitrile), and the first polymer material 311 forms the base material of the first film layer 31. In the first polymer material 311, the ratio of the weight of the PVDF-HFP to the "total weight of the ADN, the GLN, and the SN" is in the range of 12:1 to 8:1.

[0017] The ADN, GLN, and SN in the first polymer material 311 act as plasticizers, are dispersed in the PVDF-HFP, disperse the overall structure of the first polymer material 311, reduce the precipitation of the crystalline quality of the first polymer material, and are used to assist the dissociation of the lithium salt (i.e., the following first lithium salt 312). By doing so, the entire first film layer 31 easily conducts lithium ions and facilitates plastic processing. The weight ratio of the ADN, the GLN, and the SN is in the range of 1:2:7 to 0.5:1:9.5.

[0018] Next, the first lithium salt 312 is dispersed in the first polymer material 311. The first lithium salt 312 includes a mixture of LiBOB (LiB(C2O4)2, Lithium bis(oxalate)borate), LiTFSI (LiN(CF3SO2)2, Lithium bis(trifluoromethanesulfonyl)imide), and LiFSI (F2LiNO4S2, Lithium bis(fluorosulfonyl)imide). The weight ratio of the total weight of the first lithium salt 312 to the total weight of the first polymer material 311 ranges from 1:2.5 to 1:5. The LiTFSI and the LiFSI are used to enhance lithium ion conductivity. The LiBOB is used to prevent the situation where the LiTFSI and the LiFSI are eroded by water, and to prevent the situation where the performance of the entire battery deteriorates due to the attack of HF (hydrofluoric acid) generated by the reaction of water and LiTFSI, enabling the first lithium salt 312 to withstand a high voltage difference. In this way, the first polymer material 311 is stable even under the high voltage action of the positive electrode 20. The LiBOB enhances the stability of the first polymer material 311. In the first film layer 31, the ratio of "the total weight of the LiTFSI and the LiFSI" to the weight of the LiBOB is 2:3 (weight ratio). The weight ratio of the LiFSI to the LiTFSI is 2:1.

[0019] Next, the second film layer 32 is the second polymer material 321 serving as the base material of the second film layer 32. The second polymer material 321 includes a mixture of PVDF-HFP, PAN (Polyacrylonitrile), and SN, and is provided with the second polymer material 321 as the base material. In the second polymer material 321, the weight ratio of the weight of PVDF-HFP, the weight of PAN, and the weight of SN ranges from 8:1.2:1 to 8:1:1.6.

[0020] The PAN and SN in the second polymer material 321 are plasticizers dispersed in the PVDF-HFP, and their function is to disperse the overall structure of the second polymer material 321 and reduce the precipitation of crystalline material in the second polymer material 321. The PAN and SN are used to assist in the dissociation of the lithium salt of the second film layer 32 (i.e., the second lithium salt 322 described below) and to increase the ionic conductivity.

[0021] Next, the second lithium salt 322 is dispersed in the second polymer material 321 and contains LiFSI and LiTSFI. In the second film layer 32, the weight ratio of the weight of LiFSI to the weight of LiTSFI is 1:2. The second lithium salt 322 is used to lower the energy level and increase stability when conducting lithium ions in each of the polymer materials, thereby improving conductivity. The weight ratio of the total weight of the second lithium salt 322 to the total weight of the second polymer material 321 is in the range of 1:3 to 1:9.

[0022] Next, the second inorganic ceramic 323 is dispersed in the second polymer material 321 and consists of a plurality of first LLZO particles 326 coated on the outside with a first dopamine layer 324 (see Figure 3). In the second film layer 32, the overall radial length of each of the first LLZO particles 326 is less than 100 nm. The second inorganic ceramic 323 is used to increase the ionic conductivity and the overall mechanical strength of the second film layer 32. The weight percentage of the total weight of the second inorganic ceramic 323 in the second polymer material 321 is in the range of 8% wt to 20% wt.

[0023] The first LLZO particle 326 is lithium lanthanum zirconium oxide (Li7La3Zr2O 12) or lithium lanthanum zirconium oxide doped with at least one metallic element may be composed of the first LLZO particles 326. Preferably, the first LLZO particles 326 are composed of Cu-LLZO (copper-doped lithium lanthanum zirconium oxide).

[0024] Because the PVDF-HFP of the second polymer material 321 readily reacts with the first LLZO particles 326, making it difficult for the entire material to form a film, the outer surface of the first LLZO particles 326 is coated with the first dopamine layer 324 to protect them. Furthermore, when the first LLZO particles 326 become wet, they readily generate alkaline byproducts, which cause a lithium fluoride reaction with the PVDF-HFP. Since dopamine is hydrophobic, coating the outer surface of the first LLZO particles 326 with the first dopamine layer 324 makes it difficult for moisture to penetrate the first LLZO particles 326, and the functional groups of dopamine are compatible with the PAN of the second polymer material 321. In each of the first LLZO particles 326, the weight percentage of the weight of the first dopamine layer 324 relative to the weight of the first LLZO particle 326 is less than 5% wt. The thickness of the first dopamine layer 324 is less than 3 nm.

[0025] Next, the third film layer 33 comprises a third polymer material 331 which serves as the substrate for the third film layer 33. The third polymer material 331 is The mixture contains PEO (Poly(ethylene oxide), polyethylene oxide) and PAN. The weight ratio of PEO to PAN is in the range of 5:1 to 8:1, and the PEO has high stability at the reduction potential of the negative electrode 10 and moderate ionic conductivity. Since the PAN has good electronic and ionic conductivity, the overall performance of the PEO is further improved by mixing it with PAN.

[0026] The PAN in the third polymer material 331 is used as a plasticizer and is dispersed in the PEO.

[0027] Additive 332 is FEC (fluoroethylene carbonate), which is dispersed in the third polymer material 331 and used to help the negative electrode 10 form a good ASEI (artificial solid electrolyte interphase). The weight percentage of additive 332 in the third polymer material 331 is less than 10% wt.

[0028] Next, the third lithium salt 333 is dispersed in the third polymer material 331, and the third lithium salt 333 is LiTFSI. During formation or charge / discharge processes, the fluorine (F) and free lithium (Li) ions of the LiTFSI deposit on the surface of the negative electrode 10 to form LiF (lithium fluoride), which has the effect of protecting the negative electrode 10 and assisting in the formation of the ASEI. The third lithium salt 333 is used to lower the energy level and improve conductivity when conducting lithium ions in each of the polymer materials. The weight ratio of the total weight of the third lithium salt 333 to the weight ratio of the third polymer material 331 is in the range of 1:3 to 1:9.

[0029] Finally, the third inorganic ceramic 334 is dispersed in the third polymer material 331, and the third inorganic ceramic 334 is a plurality of second LLZO particles 336 coated on the outside with a second dopamine layer 335 (see Figure 4). In the third film layer 33, the overall radial size of each of the second LLZO particles 336 is in the range of 200 nm to 300 nm, and the third inorganic ceramic 334 is used to increase ionic conductivity. In this way, the negative electrode 10 has good ionic conductivity, reduces dead lithium deposition, suppresses the formation of lithium crystals, reduces the risk of puncture, improves mechanical performance, suppresses partial negative electrode expansion, and provides a stress source. The weight percentage of the total weight of the third inorganic ceramic 334 in the third polymer material 331 is in the range of 10% wt to 20% wt. In each of the second LLZO particles 336, the weight percentage of the second dopamine layer 335 relative to the weight of the second LLZO particle 336 is less than 5% wt. The thickness of the second dopamine layer 335 is less than 3 nm.

[0030] The second LLZO particle 336 is lithium lanthanum zirconium oxide (Li7La3Zr2O 12 ) or lithium lanthanum zirconium oxide doped with at least one metallic element may be composed of ) or lithium lanthanum zirconium oxide. Preferably, the second LLZO particle 336 is composed of Cu-LLZO (copper-doped lithium lanthanum zirconium oxide).

[0031] The first film layer 31 does not contain ceramic particles and is made of a flexible material, thus exhibiting high adhesion to the positive electrode. The first polymer material 311 of the first film layer 31 is a flexible material and can be filled into the gap between the dielectric film 30 and the positive electrode 20. Furthermore, the lithium salt selected for the first film layer 31 can reduce the energy level difference and increase the conductivity of lithium ions.

[0032] The concentration of the first lithium salt 312 in the first film layer 31 is higher than the concentrations of the lithium salts in the second film layer 32 and the third film layer 33 (i.e., the second lithium salt 322 and the third lithium salt 333), primarily to lower the boundary energy level that lithium ions must overcome in each polymer material of the film layer and to improve conductivity.

[0033] The lithium salt concentration in each film layer according to the present invention gradually decreases from the first film layer 31 to the third film layer 33. That is, the concentration of the first lithium salt 312 in the first film layer 31 is higher than the concentration of the second lithium salt 322 in the second film layer 32, and the concentration of the second lithium salt 322 in the second film layer 32 is higher than the concentration of the third lithium salt 333 in the third film layer 33. This reduces the energy level when lithium ions are conducted, thereby increasing conductivity.

[0034] If the concentration of a single polymer material is too high, crystalline precipitation is likely to occur, preventing the polymer from effectively forming a film through chain bonding. However, the plasticizer in the polymer material can prevent the precipitation of each of the polymer material's crystals, and the plasticizer supports each of the polymer material's structures, thereby enhancing the overall structural integrity of the polymer material. The plasticizer is a highly polar plasticizer, and its highly polar nature further facilitates the dissociation of each of the lithium salts, increasing the number of free lithium ions and further enhancing the lithium ion conductivity. In addition, inorganic ceramic materials may be added to the second film layer 32 and the third film layer 33 to enhance the conductivity and mechanical properties of lithium ions.

[0035] The sum of the thicknesses of the first film layer 31, the second film layer 32, and the third film layer 33 is in the range of 12 μm to 24 μm. The thickness of the second film layer 32 is in the range of 10 μm to 18 μm. The thicknesses of the first film layer 31 and the third film layer 33 are each in the range of 1 μm to 3 μm.

[0036] The first film layer 31 and the third film layer 33 may serve as boundary adhesive layers, with the first film layer 31 bonded to the positive electrode 20 and the third film layer 33 bonded to the negative electrode 10.

[0037] The present invention is not limited to the embodiments described above, and various modifications are possible within the scope of the claims. Embodiments obtained by appropriately combining the technical means disclosed in different embodiments are also included in the technical scope of the present invention. [Explanation of Symbols]

[0038] 10 negative electrode 12. Negative electrode slurry 15 Negative electrode particles 20 positive electrode 22 Positive electrode slurry 24 Positive electrode particles 30 Dielectric film 31. First film layer 32 Second film layer 33 Third film layer 311 First Polymer Material 312 Lithium salt 321 Second Polymer Material 322 Lithium salt 323 Second Inorganic Ceramics 324 Dopamine Layer 1 326 First LLZO particle 331 Third Polymer Materials 332 Additives 333 Third Lithium Salt 334 Third-generation inorganic ceramics 335 Second Dopamine Layer 336 2nd LLZO particle

Claims

1. A dielectric film for all-solid and semi-solid lithium batteries, wherein the lithium battery comprises a negative electrode and a positive electrode, the dielectric film is located between the positive electrode and the negative electrode, the negative electrode is filled with a negative electrode slurry and a plurality of negative electrode particles as a binder, the positive electrode is filled with a positive electrode slurry and a plurality of positive electrode particles as a binder, and the dielectric film is, It includes a first film layer, a second film layer, and a third film layer, wherein the first film layer is connected to the positive electrode, the third film layer is connected to the negative electrode, and the second film layer is connected between the first film layer and the third film layer. The first film layer is A first polymer material to be used as a substrate for the first film layer, wherein the first polymer material is a mixture of PVDF-HFP (Polyvinylidene luoride-hexafluoropropylene copolymer), ADN (Adiponitrile), GLN (Glutaronitrile), and SN (Succinonitrile), wherein the ADN, GLN, and SN of the first polymer material are used as plasticizers and are dispersed in the PVDF-HFP, and their function is to disperse the entire first polymer material, thereby reducing the precipitation of crystalline material in the first polymer material, assisting in the dissociation of lithium salts, allowing the first film layer to easily conduct lithium ions, and facilitating plastic processing. A first lithium salt dispersed in the first polymer material, wherein the first lithium salt is LiBOB (LiB(C 2 O 4 ), 2 , Lithium bis(oxalate)borate, lithium bis(oxalate)borate), LiTFSI (LiN(CF 3 SO 2 ), 2 , Lithium bis(trifluoromethanesulfonyl)imide, lithium bis(trifluoromethanesulfonyl)imide), and LiFSI (F 2 LiNO 4 S 2 , Lithium bis(fluorosulfonyl)imide, lithium bis(fluorosulfonyl)imide) mixture, and a first lithium salt, The second film layer is A second polymer material used as a substrate for the second film layer, wherein the second polymer material is a mixture of PVDF-HFP, PAN (Polyacrylonitrile), and SN, and the PAN and SN of the second polymer material are used as plasticizers and are dispersed in the PVDF-HFP, and the PAN and SN are used to assist in the dissociation of the lithium salt of the second film layer and to increase the ionic conductivity of the second polymer material, A second lithium salt dispersed in the second polymer material, wherein the second lithium salt comprises a second lithium salt containing LiFSI and LiTSFI, The second inorganic ceramic dispersed in the second polymer material is a plurality of first LLZO particles coated on the outside with a first dopamine layer, and each of the first LLZO particles is lithium lanthanum zirconium oxide (Li 7 La 3 Zr 2 O 12 ) or a second inorganic ceramic composed of lithium lanthanum zirconium oxide doped with at least one metallic element, The third film layer is A third polymer material used as a substrate for the third film layer, wherein the third polymer material is a mixture of PEO (Poly(ethylene Oxide)) and PAN, wherein the PEO has high stability at the reduction potential of the negative electrode and has moderate ionic conductivity, and the PAN has good electronic and ionic conductivity and further improves the overall performance of the PEO, and the PAN of the third polymer material is used as a plasticizer, and the third polymer material dispersed in the PEO, A third lithium salt dispersed in the third polymer material, wherein the third lithium salt is a LiTFSI third lithium salt, A third inorganic ceramic dispersed in the third polymer material, wherein the third inorganic ceramic is a plurality of second LLZO particles coated on the outside with a second dopamine layer, and each of the second LLZO particles is lithium lanthanum zirconium oxide (Li 7 La 3 Zr 2 O 12 A dielectric film for all-solid and semi-solid lithium batteries, characterized in that it comprises a third inorganic ceramic, which is composed of a lithium lanthanum zirconium oxide doped with at least one metal element, and the third inorganic ceramic is used to increase ionic conductivity.

2. In the first film layer, The weight ratio of ADN, GLN, and SN is in the range of 1:2:7 to 0.5:1:9.

5. The ratio of the weight of the PVDF-HFP to the "total weight of the ADN, GLN, and SN" is in the range of 12:1 to 8:

1. The weight ratio of the total weight of the first lithium salt to the total weight of the first polymer material is in the range of 1:2.5 to 1:

5. The dielectric film for all-solid and semi-solid lithium batteries according to claim 1, characterized in that the ratio of the total weight of the LiTFSI and LiFSI to the weight of the LiBOB is 2:3, and the weight ratio of the LiFSI to the LiTFSI is 2:

1.

3. In the second film layer, The weight ratio of the PVDF-HFP, PAN, and SN in the second polymer material is in the range of 8:1.2:1 to 8:1:1.

6. The weight ratio of the LiFSI to the LiTSFI is 1:

2. The weight ratio of the total weight of the second lithium salt to the total weight of the second polymer material is in the range of 1:3 to 1:

9. The dielectric film for all-solid and semi-solid lithium batteries according to claim 1, characterized in that the weight percentage of the total weight of the second inorganic ceramics in the second polymer material is in the range of 8% wt to 20% wt.

4. The radial size of each of the first LLZO particles is less than 100 nm. The dielectric film for all-solid and semi-solid lithium batteries according to claim 1, characterized in that, in each of the first LLZO particles, the weight percentage of the weight of the first dopamine layer in the first LLZO particle is less than 5% wt, and the thickness of the first dopamine layer is less than 3 nm.

5. In the third film layer, The weight ratio of the PEO to the PAN is in the range of 5:1 to 8:

1. The dielectric film for all-solid and semi-solid lithium batteries according to claim 1, characterized in that the weight ratio of the total weight of the third lithium salt to the weight of the third polymer material is in the range of 1:3 to 1:

9.

6. The dielectric film for all-solid and semi-solid lithium batteries according to claim 1, characterized in that the third film layer further comprises an additive, the additive being FEC (fluoroethylene carbonate) dispersed in the third polymer material, and used to assist the anode in forming a good ASEI (artificial solid electrolyte interphase).

7. The dielectric film for all-solid and semi-solid lithium batteries according to claim 6, characterized in that the weight percentage of the additive in the third polymer material is less than 10% wt.

8. The dielectric film for all-solid and semi-solid lithium batteries according to claim 1, characterized in that the first LLZO particles and the second LLZO particles are composed of Cu-LLZO, and the Cu-LLZO is copper-doped lithium lanthanum zirconium oxide.

9. The overall radial size of each of the second LLZO particles is in the range of 200 nm to 300 nm. The dielectric film for all-solid and semi-solid lithium batteries according to claim 1, characterized in that the weight percentage of the total weight of the third inorganic ceramic in the third polymer material is in the range of 10% wt to 20% wt.

10. The dielectric film for all-solid and semi-solid lithium batteries according to claim 1, characterized in that the sum of the thicknesses of the first film layer, the second film layer, and the third film layer is in the range of 12 μm to 24 μm, the thickness of the second film layer is in the range of 10 μm to 18 μm, and the thicknesses of the first film layer and the third film layer are each in the range of 1 μm to 3 μm.

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