A Sulfide Electrolyte-Filled Interpenetrating Porous Network Ultra-Thin Interface Layer, Its Preparation Method and Application

Abstract

The present invention discloses a sulfide electrolyte-filled interpenetrating porous network ultra-thin interfacial layer, its preparation method and application, which relates to the field of sulfide all-solid-state battery materials. By modifying PVDF-HFP with carboxymethyl chitosan, the hydroxyl, carboxyl and amino groups in carboxymethyl chitosan can form hydrogen bonds and electrostatic interactions with the fluorocarbon chains of PVDF-HFP, optimizing the toughness and environmental friendliness of the film while retaining the excellent electrochemical stability of PVDF-HFP; then the film is subjected to anti-solvent induced phase separation treatment to form a uniform porous network structure; finally, the sulfide electrolyte dispersion is directionally deposited into the porous network structure of the ultra-thin film, and the distribution of the electrolyte in the pores is precisely controlled by the spraying process to construct a continuous lithium-ion transport channel, and the final composite ultra-thin interfacial layer is formed after drying. This interfacial layer has the characteristics of ultra-thin and high ionic conductivity, and can effectively reduce the interfacial impedance, improve the interfacial stability and long-cycle stability of sulfide all-solid-state batteries.

Description

Technical Field

[0001] The present invention relates to the field of sulfide all-solid-state battery materials, and particularly to a sulfide electrolyte-filled interpenetrating porous network ultrathin interfacial layer, its preparation method and application, and especially to a sulfide electrolyte directionally filled ultrathin interfacial layer of a carboxymethyl chitosan-modified PVDF-HFP composite biobased interpenetrating porous network structure, its preparation method and application. Background Art

[0002] With the development of new energy technologies, all-solid-state batteries have become a research hotspot for next-generation energy storage devices due to their advantages such as high energy density, high safety, and no risk of liquid leakage. Among them, sulfide electrolytes are widely used in all-solid-state battery systems due to their high ionic conductivity and excellent interfacial contact performance. However, compared with traditional liquid electrolytes, sulfide all-solid-state batteries still face many challenges in practical applications. Among them, the interfacial stability and cycle stability between the cathode material and the sulfide electrolyte are the key factors affecting the performance of all-solid-state batteries. Due to the high chemical activity of sulfide electrolytes, side reactions are likely to occur when they come into contact with cathode materials such as high-nickel ternary materials, lithium-rich oxides, and lithium iron phosphate, resulting in an increase in interfacial impedance and degradation of the interfacial structure, ultimately affecting the long-term stable operation of the battery. In addition, the contact between the sulfide electrolyte and the cathode active material particles is uneven, which may form high-impedance regions, further reducing the rate performance and cycle life of the battery. Summary of the Invention

[0003] In view of this, the purpose of the present invention is to provide a sulfide electrolyte-filled interpenetrating porous network ultrathin interfacial layer, its preparation method and application.

[0004] The purpose of the present invention is achieved by the following technical solutions:

[0005] <First Aspect>

[0006] The present invention provides a preparation method of a sulfide electrolyte-filled interpenetrating porous network ultrathin interfacial layer, comprising the following steps:

[0007] Mix a carboxymethyl chitosan-modified PVDF-HFP solution and a lithium salt solution evenly to obtain a precursor solution;

[0008] Coat the precursor solution on a substrate, and through anti-solvent phase separation treatment and drying treatment, obtain a porous structure ultrathin film with an interpenetrating network;

[0009] Deposit a sulfide electrolyte slurry evenly into the porous structure ultrathin film structure, and dry it to obtain the interfacial layer.

[0010] As an embodiment, the carboxymethyl chitosan-modified PVDF-HFP solution is a solution obtained by mixing a PVDF-HFP solution and a carboxymethyl chitosan solution.

[0011] As an embodiment, the ratio of the solute to the solvent in the carboxymethyl chitosan solution is (0.1~0.5) g : 20 mL.

[0012] As an embodiment, the solvent in the carboxymethyl chitosan solution is deionized water.

[0013] In some embodiments, the ratio of the solute to the solvent in the carboxymethyl chitosan solution is (0.2~0.3) g : 20 mL.

[0014] As an embodiment, the ratio of the solute to the solvent in the PVDF-HFP solution is (0.5~2) g : 10 mL.

[0015] In some embodiments, the ratio of the solute to the solvent in the PVDF-HFP solution is (1~1.5) g : 10 mL.

[0016] As an embodiment, the solvent in the PVDF-HFP solution is a polar solvent.

[0017] As an embodiment, the solvent in the PVDF-HFP solution is one or more of N-methylpyrrolidone, dimethylacetamide, dimethylformamide, dimethyl sulfoxide, tetrahydrofuran, and acetone.

[0018] In some embodiments, the solvent in the PVDF-HFP solution is N-methylpyrrolidone.

[0019] As an embodiment, the solute in the lithium salt solution is lithium bis(oxalato)borate or lithium bis(trifluoromethanesulfonyl)imide.

[0020] As an embodiment, the solvent in the lithium salt solution is acetonitrile or tetrahydrofuran.

[0021] As an embodiment, the ratio of the solute to the solvent in the lithium salt solution is (0.2~0.8) g : 5 mL.

[0022] In some embodiments, the ratio of the solute to the solvent in the lithium salt solution is 0.5 g : 5 mL.

[0023] As an embodiment, the ratio of the solute to the solvent in the sulfide electrolyte slurry is (0.2~1.5) g : 10 mL.

[0024] In some embodiments, the ratio of the solute to the solvent in the sulfide electrolyte slurry is (0.5 - 1.0) g : 10 mL.

[0025] As an embodiment, the solute in the sulfide electrolyte slurry is Li6PS5Cl.

[0026] As an embodiment, the solvent in the sulfide electrolyte slurry is an ether solvent.

[0027] In some embodiments, the solvent in the sulfide electrolyte slurry is anisole.

[0028] As an embodiment, magnetic stirring is used for solution mixing in the preparation of the precursor solution.

[0029] As an embodiment, magnetic stirring and ultrasonic treatment are successively used for mixing in the preparation process of the carboxymethyl chitosan-modified PVDF-HFP solution.

[0030] As an embodiment, the precursor solution is coated on a substrate to form a film with a thickness of 0.3 - 1.0 μm.

[0031] As an embodiment, the substrate is made of glass.

[0032] As an embodiment, the anti-solvent phase separation treatment is to immerse the substrate with the coated film in deionized water for phase separation.

[0033] As an embodiment, the time of the anti-solvent phase separation treatment is 0.8 - 1.2 h.

[0034] As an embodiment, the deposition method is: using the spraying method, spraying the sulfide electrolyte slurry onto one side of the porous ultra-thin film structure.

[0035] As an embodiment, the spraying rate is 0.05 - 0.15 mL / min, and the spraying distance is 5 - 10 cm.

[0036] In some embodiments, the spraying rate is 0.1 mL / min, and the spraying distance is 8 cm.

[0037] As an embodiment, the drying parameters are a vacuum degree of 0.05 - 0.09 MPa and a temperature of 40 - 80 °C.

[0038] In some embodiments, the drying parameters are a vacuum degree of 0.08 MPa and a temperature of 50 - 60 °C.

[0039] <Second aspect>

[0040] The present invention provides a sulfide electrolyte-filled interpenetrating porous network ultra-thin interface layer, which includes a porous framework formed by a PVDF-HFP polymer modified with carboxymethyl chitosan, a lithium salt is distributed in the framework, and sulfides are distributed in the pores of the framework.

[0041] As an embodiment, the thickness of the interface layer is 0.5 to 5 μm.

[0042] In some embodiments, the thickness of the interface layer is 0.8 to 1.0 μm.

[0043] As an embodiment, the impedance of the interface layer is 17 to 20 Ω, and the ionic conductivity is 8.0 to 9 mS / cm.

[0044] In some embodiments, the impedance of the interface layer is 17.3 to 19.1 Ω, and the ionic conductivity is 8.0 to 8.9 mS / cm.

[0045] <Third aspect>

[0046] The present invention provides an application of a sulfide electrolyte-filled interpenetrating porous network ultra-thin interface layer in a all-solid-state battery.

[0047] As an embodiment, the application of the interface layer as an electrolyte layer.

[0048] Compared with the prior art, the present invention has the following beneficial effects:

[0049] The present invention provides a preparation method of a sulfide electrolyte-filled interpenetrating porous network ultra-thin interface layer, and this method has the following characteristics:

[0050] 1) Bio-based material modification

[0051] The present invention selects the renewable biopolymer carboxymethyl chitosan to modify PVDF-HFP. The hydroxyl, carboxyl, and amino groups in the carboxymethyl chitosan molecule can form hydrogen bonds and electrostatic interactions with the fluorocarbon chains of PVDF-HFP, improving its environmental friendliness while completely retaining the excellent electrochemical stability of PVDF-HFP itself.

[0052] 2) Porous structure construction

[0053] The modified film is subjected to anti-solvent induced phase separation treatment to form uniform, high specific surface area, and interconnected micro-nano scale pores, creating favorable conditions for subsequent electrolyte filling and ion transport.

[0054] 3) Electrolyte deposition

[0055] Using a spraying process, the sulfide electrolyte dispersion is precisely and directionally deposited into the porous network of the PVDF-HFP / carboxymethyl chitosan composite membrane. By regulating the spraying parameters, it is ensured that the electrolyte particles uniformly fill the pores, improving the interface stability, reducing the interface impedance, and making close contact with the positive electrode. Furthermore, a continuous lithium-ion transport channel is successfully constructed at the interface. After drying, a composite ultra-thin interface layer is finally obtained.

[0056] The sulfide electrolyte-filled interpenetrating porous network ultra-thin interface layer prepared by the above method has outstanding performance advantages, which are specifically as follows:

[0057] 1) High-efficiency ion transport

[0058] The interpenetrating porous network structure provides an efficient channel for ion transport, greatly enhancing the ion transport ability, effectively reducing the interface impedance, enabling the interface layer to have a high ionic conductivity, and ensuring that lithium ions can achieve rapid transport at the interface.

[0059] 2) Good compatibility

[0060] The composite interface layer significantly enhances the compatibility between the polymer membrane and the sulfide electrolyte, further promoting ion conduction and at the same time improving the interface stability of the composite membrane.

[0061] 3) Ultra-thin design

[0062] This interface layer adopts the ultra-thin design concept. While ensuring interface stability, it does not significantly increase the overall thickness of the battery, which helps to maintain the high energy density of the battery and is especially suitable for the fields of high-performance energy storage devices and power batteries.

[0063] 4) Application value

[0064] The ultra-thin interface layer prepared by the present invention can effectively solve the long-existing interface problem between the positive electrode and the electrolyte of the sulfide all-solid-state battery, significantly improving the interface stability and long-cycle stability of the battery. This innovative achievement provides an efficient and easily scalable solution for improving the performance of sulfide all-solid-state batteries, which is of crucial significance for promoting the commercial application process of all-solid-state batteries. Description of the drawings

[0065] By reading the detailed description of the non-limiting embodiments with reference to the following drawings, other features, objectives, and advantages of the present invention will become more obvious:

[0066] Figure 1 SEM image of the interface layer prepared in Example 1 of the present invention, with a magnification of ×2000;

[0067] Figure 2SEM image of the interfacial layer prepared in Example 1 of the present invention, with a magnification of ×10,000;

[0068] Figure 3 Electrochemical EIS impedance diagram of the sample of Example 1;

[0069] Figure 4 Electrochemical EIS impedance diagram of the sample of Example 2;

[0070] Figure 5 Electrochemical EIS impedance diagram of the sample of Comparative Example 1;

[0071] Figure 6 Electrochemical EIS impedance diagram of the sample of Comparative Example 2. Detailed implementation manners

[0072] The present invention will be described in detail below with reference to the embodiments. The following embodiments will help those skilled in the art to further understand the present invention, but do not limit the present invention in any form. It should be noted that those of ordinary skill in the art can make several adjustments and improvements without departing from the concept of the present invention. These all belong to the protection scope of the present invention.

[0073] For easy understanding, the abbreviations or nouns mentioned in the following text are first explained:

[0074] PVDF-HFP: Polyvinylidene fluoride - hexafluoropropylene copolymer.

[0075] Example 1

[0076] This example provides a method for preparing a sulfide electrolyte-filled interpenetrating porous network ultrathin interfacial layer, including the following steps:

[0077] S1. Prepare a modified PVDF-HFP solution using carboxymethyl chitosan

[0078] Mix the PVDF-HFP solution and the carboxymethyl chitosan solution, stir magnetically at room temperature for 3 h, and ultrasonically treat in an ultrasonic bath at 40 kHz for 45 min to form a uniform mixed solution, obtaining a carboxymethyl chitosan-modified PVDF-HFP solution;

[0079] S2. Prepare a precursor solution

[0080] Add a lithium bis(oxalato)borate solution to the modified PVDF-HFP solution, stir magnetically at room temperature for 2 h to make the solution uniformly mixed, obtaining a precursor solution;

[0081] S3. Coat and dry to prepare an interpenetrating network porous structure ultra-thin film

[0082] The precursor solution was uniformly coated on a glass substrate to form an ultra-thin film with a thickness of about 0.8 μm. Then, the film was immersed in 100 mL of deionized water for 1 h, and the anti-solvent effect was used to induce the phase separation of PVDF-HFP to form a connected porous structure film. The film was taken out of the water and dried in a vacuum drying oven at 50 °C (vacuum degree 0.08 MPa) for 12 h to ensure the stability of the porous structure and remove the residual moisture, obtaining an ultra-thin film with an interpenetrating network porous structure;

[0083] S4. Preparation of a sulfide electrolyte-filled interpenetrating porous network ultra-thin interfacial layer

[0084] Using the directional spraying method, the sulfide electrolyte slurry was uniformly sprayed on one side of the porous structure film, controlling the spraying rate at 0.1 mL / min and the spraying distance at 8 cm to ensure that the electrolyte uniformly penetrated into the porous network structure. Then, it was dried in a vacuum drying oven at 60 °C (vacuum degree 0.08 MPa) for 6 h to remove the solvent, and finally a PVDF-HFP / carboxymethyl chitosan-sulfide electrolyte composite ultra-thin interfacial layer with a thickness of about 1.0 μm was formed, and the pore diameter of its porous structure was about 50 - 200 nm, as Figure 1 and Figure 2 shown.

[0085] It should be noted that in this embodiment, unilateral spraying is adopted, and it is necessary to try to avoid leaving a covering layer on the surface of the porous structure film by the sulfide electrolyte slurry. However, in actual operation, it is inevitable that there will be some residues. Therefore, the sulfide electrolyte layer on the surface of the spraying side of the porous structure film should not exceed 300 nm.

[0086] In this embodiment, the volume dosages of the PVDF-HFP solution, the carboxymethyl chitosan solution, and the lithium bis(oxalato)borate solution are 5 mL, 10 mL, and 2 mL respectively.

[0087] PVDF-HFP solution: 1.0 g of PVDF-HFP was dissolved in 10 mL of N-methylpyrrolidone (NMP), and magnetically stirred in a water bath at 70 °C for 5 h until completely dissolved to form a uniform and transparent solution with a concentration of about 8.86 wt.% (the density of NMP was calculated as 1.028 g / mL at 25 °C).

[0088] Carboxymethyl chitosan solution: 0.2 g of carboxymethyl chitosan was dissolved in 20 mL of deionized water to prepare an aqueous solution, and magnetically stirred at room temperature for 5 h until a uniform carboxymethyl chitosan solution was formed, and the mass fraction of carboxymethyl chitosan was about 0.99 wt.%.

[0089] Lithium bis(oxalato)borate solution: 0.5 g of lithium bis(oxalato)borate was dissolved in 5 mL of acetonitrile and magnetically stirred at room temperature for 30 min to form a uniform lithium bis(oxalato)borate solution.

[0090] Sulfide electrolyte slurry: 0.5 g of sulfide electrolyte Li6PS5Cl was added to 10 mL of ether solvent anisole, ball-milled for 30 min under an argon protection environment, and then ultrasonically stirred for 30 min under an argon environment to form a uniform electrolyte slurry.

[0091] Example 2

[0092] This example provides a method for preparing a sulfide electrolyte-filled interpenetrating porous network ultra-thin interface layer, including the following steps:

[0093] S1. Prepare a modified PVDF-HFP solution using carboxymethyl chitosan

[0094] The PVDF-HFP solution and the carboxymethyl chitosan solution were mixed, magnetically stirred at room temperature for 3 h and ultrasonically treated in a 40 kHz ultrasonic bath for 40 min to form a uniform mixed solution, obtaining a carboxymethyl chitosan-modified PVDF-HFP solution;

[0095] S2. Prepare a precursor solution

[0096] Lithium bis(trifluoromethanesulfonyl)imide solution was added to the modified PVDF-HFP solution and magnetically stirred at room temperature for 2 h to make the solution uniformly mixed, obtaining a precursor solution;

[0097] S3. Coat and dry to prepare an interpenetrating network porous structure ultra-thin film

[0098] The precursor solution was uniformly coated on a glass substrate to form an ultra-thin film with a thickness of about 0.5 μm, and then the film was immersed in 80 mL of deionized water for 0.5 h. The anti-solvent effect was used to induce phase separation of PVDF-HFP to form a connected porous structure film. The film was taken out of the water and dried in a vacuum drying oven at 60 °C for 18 h to ensure the stability of the porous structure and remove residual moisture, obtaining an interpenetrating network porous structure ultra-thin film;

[0099] S4. Prepare a sulfide electrolyte-filled interpenetrating porous network ultra-thin interface layer

[0100] Using the spraying method, the sulfide electrolyte slurry was uniformly sprayed on one side of the porous film structure, and the spraying rate was controlled at 0.15 mL / min to ensure that the electrolyte was uniformly filled into the porous network structure. Then it was dried in a vacuum drying oven at 80 °C for 8 hours to remove the solvent, and finally a PVDF-HFP / carboxymethyl chitosan-sulfide electrolyte composite ultra-thin interface layer with a thickness of about 0.8 μm and a pore diameter of about 50 - 200 nm in its porous structure was formed.

[0101] In this embodiment, the volume dosages of the PVDF-HFP solution, the carboxymethyl chitosan solution, and the lithium bis(oxalato)borate solution are 8 mL, 8 mL, and 3 mL respectively.

[0102] PVDF-HFP solution: Dissolve 1.8 g of PVDF-HFP in 12 mL of N-methylpyrrolidone (NMP), and magnetically stir for 4 hours under a water bath condition of 60 °C until completely dissolved to form a uniform and transparent solution with a concentration of approximately 12.73 wt.%.

[0103] Carboxymethyl chitosan solution: Dissolve 0.3 g of carboxymethyl chitosan in 20 mL of deionized water to prepare an aqueous solution, and magnetically stir for 4 hours at room temperature until a uniform carboxymethyl chitosan solution is formed, with the mass fraction of carboxymethyl chitosan being approximately 1.48 wt.%.

[0104] Lithium bis(trifluoromethanesulfonyl)imide solution: Dissolve 0.5 g of lithium bis(trifluoromethanesulfonyl)imide in 5 mL of tetrahydrofuran, and magnetically stir for 40 min at room temperature to form a uniform lithium bis(trifluoromethanesulfonyl)imide solution.

[0105] Sulfide electrolyte slurry: Add 1.0 g of sulfide electrolyte Li6PS5Cl to 15 mL of anisole, ball mill for 60 min under an argon protection environment, and then ultrasonically stir for 40 min under an argon environment to form a uniform electrolyte slurry.

[0106] Comparative Example 1

[0107] In this comparative example, an unmodified PVDF-HFP is used to prepare a method for fabricating an interpenetrating porous network ultra-thin interfacial layer filled with sulfide electrolyte. The steps are basically the same as those in Example 1, except that:

[0108] Step S1 is cancelled;

[0109] In Step S2, a PVDF-HFP solution is used to prepare a precursor solution.

[0110] An unmodified PVDF-HFP interfacial layer filled with sulfide electrolyte is prepared, with a thickness of approximately 1 μm.

[0111] Comparative Example 2

[0112] In this comparative example, a method for fabricating an interpenetrating porous network ultra-thin interfacial layer is provided, that is, referring to Example 1, a porous structure ultra-thin film with an interpenetrating network is fabricated through Steps S1, S2, and S3, with a thickness of approximately 0.8 μm.

[0113] Comparative Example 3

[0114] This comparative example provides a method for fabricating an ultra-thin interfacial layer. The steps are basically the same as those in Example 1, except that:

[0115] In step S1 and step S2, the three solutions, namely the PVDF-HFP solution, the carboxymethyl chitosan solution, and the lithium bis(oxalato)borate solution, are mixed together and then magnetically stirred to fully mix the solutions.

[0116] However, a porous structure film was not formed in the subsequent steps.

[0117] Performance detection

[0118] The electrochemical performance of the interface layers prepared in each example and comparative example was tested respectively.

[0119] Test of ionic conductivity: Using a sulfide electrolyte of the Li6PS5Cl type, in a pressure cell mold, first load 100 mg of the sulfide electrolyte, press it under a pressure of 1 ton, hold the pressure for 1 minute, then lay the prepared interface layer flat on the electrolyte respectively, and then load 100 mg of the sulfide electrolyte, press it under a pressure of 1 ton, hold the pressure for 1 minute. Using an electrochemical workstation with the model CHI660E, in a normal atmospheric atmosphere at room temperature, perform an alternating current impedance test (as Figures 3 to 6 shown), and calculate the ionic conductivity. The results are shown in Table 1.

[0120] Table 1 Electrochemical performance data of the interface layer

[0121]

[0122] The interpenetrating porous network interface layer of the present invention has the characteristics of being ultrathin and having excellent interfacial compatibility, which can effectively reduce the interfacial impedance. At the same time, by directionally filling the sulfide electrolyte, the interfacial ionic conductivity is improved, and the lithium ion transport channel is optimized, thereby significantly improving the rate performance and cycle life of the sulfide all-solid-state battery. The preparation method of the present invention has a simple process, strong controllability, and is suitable for large-scale production, and has broad application prospects in the field of high-energy-density all-solid-state batteries.

[0123] The specific embodiments of the present invention have been described above. It should be understood that the present invention is not limited to the above specific embodiments, and those skilled in the art can make various deformations or modifications within the scope of the claims, which does not affect the essence of the present invention.

Claims

1. A preparation method of a sulfide electrolyte-filled interpenetrating porous network ultrathin interfacial layer, characterized in that It includes the following steps: Mix the carboxymethyl chitosan-modified PVDF-HFP solution and the lithium salt solution evenly to obtain a precursor solution; Coat the precursor solution on a substrate, and through anti-solvent phase separation treatment and drying treatment, obtain a porous structure ultra-thin film with an interpenetrating network; Evenly deposit the sulfide electrolyte slurry into the porous structure ultra-thin film structure, and dry it to obtain the interface layer; The solute in the lithium salt solution is lithium bis(oxalato)borate or lithium bis(trifluoromethanesulfonyl)imide, and the solvent is acetonitrile or tetrahydrofuran; The solute in the sulfide electrolyte slurry is Li6PS5Cl, and the solvent is an ether solvent.

2. The preparation method according to claim 1, characterized in that, The carboxymethyl chitosan-modified PVDF-HFP solution is a solution obtained by mixing the PVDF-HFP solution and the carboxymethyl chitosan solution.

3. The preparation method according to claim 2, characterized in that, It also includes one or more of the following technical features: A. The ratio of the solute to the solvent in the carboxymethyl chitosan solution is (0.1~0.5) g : 20 mL; B. The solvent in the carboxymethyl chitosan solution is deionized water; C. The ratio of the solute to the solvent in the PVDF-HFP solution is (0.5~2) g : 10 mL; D. The solvent in the PVDF-HFP solution is one or more of N-methylpyrrolidone, dimethylacetamide, dimethylformamide, dimethyl sulfoxide, tetrahydrofuran, and acetone.

4. The preparation method according to claim 1, characterized in that, It also includes one or more of the following technical features: A. The ratio of the solute to the solvent in the lithium salt solution is (0.2~0.8) g : 5 mL; B. The ratio of the solute to the solvent in the sulfide electrolyte slurry is (0.2~1.5) g : 10 mL.

5. The preparation method according to claim 1, characterized in that, The precursor solution is coated on the substrate to form a film with a thickness of 0.3~1.0 μm.

6. The preparation method according to claim 1, characterized in that, The anti-solvent phase separation treatment is to soak the substrate with the coated film in deionized water for phase separation.

7. The preparation method according to claim 1, characterized in that, The deposition method is: using the spraying method, spraying the sulfide electrolyte slurry on one side of the porous structure ultra-thin film structure.

8. A sulfide electrolyte-filled interpenetrating porous network ultra-thin interfacial layer, characterized in that, It is prepared by the preparation method according to any one of claims 1 to 7.

9. The interface layer according to claim 8, wherein It also includes one or more of the following technical features: A. The thickness of the interface layer is 0.5~5 μm; B. The impedance of the interface layer is 17~20 Ω, and the ionic conductivity is 8.0~9 mS / cm.

10. Application of the interface layer according to any one of claims 8 to 9 in a all-solid-state battery.

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