Closed all-solid-state lithium-oxygen battery, oxygen-containing composite positive electrode material and preparation method

Abstract

The invention discloses a closed all-solid-state lithium-oxygen battery, an oxidation composite positive electrode and a preparation method, the closed all-solid-state lithium-oxygen battery comprises an oxygen-containing compound and a catalyst, the oxygen-containing compound comprises one or more of Li2O, Li2O2, KO2, Li2CO3, Li3PO4 and LiNO3, and the catalyst comprises a transition metal oxide, a noble metal and an alloy thereof, a carbon-based material, a metal organic framework and a derivative thereof, a monatomic catalyst and a composite material. The catalyst comprises one or more of oxygen-containing compounds and one or more of non-metal catalysts, the mass ratio of the oxygen-containing compounds is 50%-80%, and the mass ratio of the catalyst is 20%-50%. According to the invention, the oxidation-reduction reaction of oxygen is immobilized, oxygen is not generated, and the problems of complex structure and low actual energy density of an open type lithium air battery are solved; the solid electrolyte is used for replacing electrolyte, so that the potential safety hazard of electrolyte permeation is solved, the electrochemical performance is improved, and a new path is provided for the ultrahigh-specific-energy all-solid-state battery.

Description

Technical Field

[0001] The present invention relates to the field of solid-state batteries, and in particular to a closed all-solid-state lithium-oxygen battery and a preparation method thereof. Background Art

[0002] Solid-state batteries have attracted significant attention in recent years due to their significant advantages, including high safety, high theoretical energy density, and wide operating temperature range. They hold broad application prospects, particularly in the fields of new energy and energy storage. It is predicted that solid-state lithium-ion power batteries will achieve large-scale commercial application between 2025 and 2030. However, the theoretical capacity of conventional cathode materials in existing technologies is relatively low, and the development of all-solid-state batteries with energy densities exceeding 500Wh / kg remains a significant challenge.

[0003] Lithium-oxygen batteries (Li-O2 batteries), a high-energy-density energy storage technology, are considered the "holy grail" of lithium secondary batteries due to their ultra-high theoretical energy density (approximately 3500Wh / kg). Li-O2 batteries generate capacity by reacting lithium metal with oxygen to form lithium peroxide (Li2O2). Significant progress has been made in some research, with lithium-air cells achieving energy densities of 780Wh / kg already reported.

[0004] Although lithium-oxygen batteries have significant theoretical advantages, they still have the following problems in existing technologies: (1) The open structure design is complex, which reduces the actual energy density. Lithium-oxygen batteries need to be equipped with air filters or oxygen storage devices and are usually designed as open structures. This design complicates the battery system, increases manufacturing costs, and takes up additional space, reducing the actual energy density. (2) Liquid electrolytes pose serious safety risks. Traditional lithium-oxygen batteries mostly use liquid electrolytes, and the open structure easily causes the electrolyte to volatilize, leak or degrade. This not only significantly reduces the safety of the battery, but may also cause safety accidents. (3) Side reactions are serious and the cycle life is short. In a liquid electrolyte environment, the lithium metal negative electrode easily reacts with the electrolyte or oxygen to generate unstable byproducts. This phenomenon will lead to a decrease in battery performance and coulombic efficiency, seriously affecting the cycle life of the battery. (4) It is difficult to balance energy density and safety. In the process of improving the energy density of lithium-oxygen batteries, safety performance often needs to be sacrificed. The existing technology has not yet achieved an effective balance between high specific energy and high safety.

[0005] All-solid-state batteries, due to their lack of liquid electrolytes, are considered a key approach for improving battery safety and energy density. Inorganic solid-state electrolytes (including oxides, sulfides, polymers, and halides) are becoming a research hotspot as alternatives to liquid electrolytes due to their excellent ionic conductivity and electrochemical stability. Combining solid-state battery and lithium-air battery technologies could provide an innovative path to developing batteries with high specific energy and safety performance.

[0006] Patent CN 113130920 A discloses an integrated composite oxygen electrode and its preparation and application. This patent involves dissolving polyoxyethylene in acetonitrile, adding a lithium salt and an inorganic electrolyte to form a uniform electrolyte membrane slurry; dissolving polyoxyethylene in N-methylpyrrolidone, adding a lithium salt and an inorganic electrolyte to form a composite binder slurry; grinding the composite binder slurry with a catalyst and uniformly coating it on a current collector to form a composite oxygen electrode; and pouring the electrolyte membrane slurry onto the composite oxygen electrode to form an integrated composite oxygen electrode. While this method reduces the oxygen electrode interfacial impedance and improves the charge-discharge cycle performance of solid-state lithium-oxygen batteries, the use of organic solvents poses environmental pollution and high solvent recovery costs. Furthermore, the preparation process is complex, and the overall energy density of the battery needs to be improved.

[0007] Patent CN 113948717 A discloses a composite solid electrolyte-cathode composite material, its preparation method, and a lithium-oxygen battery. The composite solid electrolyte-cathode composite material described in the patent comprises a porous, dense, porous skeleton material; a solid electrolyte composited within a porous layer on one side of the skeleton material; and a cathode material composited within a porous layer on the other side of the skeleton material. This structure integrates the solid electrolyte and cathode, effectively improving the interfacial contact and stability between the lithium anode and solid electrolyte. However, the preparation of the porous-dense-porous skeleton material using template or phase transfer methods requires high preparation conditions and results in poor product consistency.

[0008] Patent CN 115911680 A discloses an all-solid-state lithium-oxygen battery and its preparation method. The all-solid-state lithium-oxygen battery described in the patent includes a battery housing and a battery cell encapsulated within the housing. The battery cell comprises a solid electrolyte, a double-layer positive electrode, and a lithium sheet. The double-layer positive electrode comprises a nano-gold layer and a silver nanowire layer adjacent to the solid electrolyte. This all-solid-state lithium-oxygen battery improves the solid-solid interface between the positive electrode and the electrolyte, effectively enhancing battery cycle stability. However, the use of precious metals increases production costs, and the complex preparation process makes it difficult to commercialize in a short period of time.

[0009] In summary, it is necessary to develop a closed all-solid-state lithium-oxygen battery with high energy density and high safety. By controlling the redox products of the positive electrode and avoiding the use of an oxygen supply device, the battery structure and preparation process can be simplified, and the battery energy density and safety can be improved. At the same time, inorganic solid electrolytes and catalysts can be flexibly selected to achieve an all-solid-state battery with a wide application range, high energy density, high safety, simple preparation process and low cost. Summary of the Invention

[0010] To address the above-mentioned problems, the present invention aims to provide a closed all-solid-state lithium-oxygen battery and a method for preparing the same. In response to the above-mentioned technical deficiencies, the present invention optimizes the design of lithium-oxygen batteries through the following innovations, promoting the development of batteries with high energy density and high safety: The concept of oxygen-containing composite cathode materials is proposed for the first time, and successfully applied in closed all-solid-state batteries to achieve excellent electrochemical performance. The present invention aims to simplify the battery structure design by immobilizing the redox reaction of oxygen, limiting the existence of oxygen to Li2O, Li2O2, and LiO2, without generating oxygen, thereby eliminating the need for an oxygen supply device and achieving high actual energy density, thus solving the problems of complex structure and low actual energy density of open lithium-air batteries; replacing the electrolyte with a solid electrolyte solves the safety hazard of electrolyte penetration and improves electrochemical performance, providing a new path for ultra-high specific energy all-solid-state batteries, and applying oxygen-containing composite cathode materials in closed all-solid-state batteries solves problems such as electrolyte leakage and electrolyte side reactions, thereby improving safety and electrochemical performance.

[0011] The present invention is achieved through the following technical solutions:

[0012] Oxygen-containing composite positive electrode materials include oxygen-containing compounds and catalysts. The oxygen-containing compounds include one or more of Li2O, Li2O2, KO2, Li2CO3, Li3PO4, and LiNO3. The catalysts include one or more of transition metal oxides (such as MnO2, Co3O4), precious metals and their alloys (such as Pt, Ir), carbon-based materials (such as graphene, carbon nanotubes), metal-organic frameworks (MOFs) and their derivatives (such as Fe-NC), single-atom catalysts (SACs, such as single-atom Fe, Co), composite materials (such as metal oxide / carbon composites), and non-metallic catalysts (such as nitrides, phosphides). The mass proportion of the oxygen-containing compound is 50%-80%, and the mass proportion of the catalyst is 20%-50%.

[0013] The preparation methods of oxygen-containing composite positive electrode materials include solid phase and liquid phase methods.

[0014] Among them, the specific solid phase method is to mechanically mix the oxygen-containing compound and the catalyst with a method of sintering, the mechanical mixing method is high-energy ball milling or ultra-high-energy ball milling, the ball-to-material ratio is 40:1, the rotation speed is 500-600rpm, and the ball milling time is 80-200h; the sintering is specifically: the mixed material is sintered, and during implementation, it can be placed in a tubular furnace or muffle furnace with O2, the sintering temperature is 200-500℃, and the sintering time is 2-8h.

[0015] The liquid phase preparation method includes the following steps: (1) preparing a mixed precursor solution, specifically including: selecting a lithium source (such as Li2O2, Li2O, etc.) and a transition metal salt compound (such as chloride, nitrate or other soluble metal salt) as precursors, mixing the lithium source with an ethanol solution of the transition metal salt, wherein the molar ratio of the lithium source to the transition metal salt is 1:n, n<10, wherein n is used to adjust the mass percentage of lithium oxide and transition metal oxide in the final completely oxidized product. Ultrasonic treatment can be performed during the mixing process to improve the dispersibility. The precursor solution is then stirred for reaction, filtered and dried, and sintered. The sintering treatment specifically includes: sintering the dried intermediate product at 200-500°C for 1-5 hours in an oxygen atmosphere to obtain a final product of the nanocomposite material and the transition metal oxide.

[0016] A positive electrode sheet includes the oxygen-containing composite positive electrode material as described above, an inorganic solid electrolyte material, and a conductive agent. The conductive agent includes one or more of conductive carbon black (SP), graphite, carbon fiber (VGCF), carbon nanotubes (CNTs), and graphene (GN).

[0017] Among them, the inorganic solid electrolyte material includes one or more of oxide solid electrolyte, sulfide solid electrolyte, polymer solid electrolyte and halide solid electrolyte.

[0018] A closed all-solid-state lithium-oxygen battery comprises the aforementioned positive electrode sheet, an inorganic solid electrolyte material and a negative electrode material.

[0019] The oxide solid electrolyte includes but is not limited to Li7La3Zr2O 12 (LLZO) and its doped derivatives; Li 1.3 Al 0.3 Ti 1.7 (PO4)3 (LATP) and its derivatives; Li4Ti5O 12 and its derivatives; Li3xLa 2 / 3 -xTiO3 (LLTO) and its derivatives; Li 10 GeP2O 12 and its derivatives.

[0020] The sulfide solid electrolyte includes but is not limited to Li6PS5X (X=F, Cl, Br, I or one or more thereof) and its derivatives; Li6+aSb1-aSiaS5I and its derivatives (0.1≤a≤0.75); Li 10 MP2S 12 (M=one or more of Si, Ge, Sn, Zn, Al) and its derivatives; Li3PS4 and its derivatives; Li7P3S 11and its derivatives; Li4MS4 (M=Si, Sn, Ge) and its derivatives.

[0021] The polymer solid electrolyte includes but is not limited to polyethylene oxide (PEO)-based electrolytes and their doped derivatives; polyvinylidene fluoride (PVDF)-based electrolytes and their composites; polyacrylonitrile (PAN)-based electrolytes and their derivatives; polymethacrylate (PMMA)-based electrolytes and their derivatives.

[0022] The halide solid electrolyte includes but is not limited to Li3MX6 (M=Y, In, Sc, X=F, Cl, Br, I) and its derivatives; LixMyN1-yClz (0<x≤3, 0<z≤6) and its derivatives; Li2ZrCl6 and its derivatives.

[0023] The negative electrode materials include but are not limited to Li metal, Li-In alloy, graphite, Si and alloys thereof.

[0024] When performing battery testing, the voltage test range is selected from 2.0V to 5V.

[0025] The test temperature is between 0° C. and 150° C. The battery test temperature of the present invention can reach 150° C., which raises the operating temperature of the battery to a higher level and improves the high temperature resistance of the battery.

[0026] Compared with the prior art, the present invention has the following advantages and beneficial effects:

[0027] 1. This invention proposes the concept of an oxygen-containing composite cathode material for the first time and successfully applies it in a closed all-solid-state battery, achieving excellent electrochemical performance. This invention aims to address the complex structure and low practical energy density of open-type lithium-air batteries by immobilizing the oxygen redox reaction, eliminating oxygen production. Replacing the electrolyte with a solid-state electrolyte addresses the safety risk of electrolyte penetration and improves electrochemical performance, providing a new path for ultra-high specific energy all-solid-state batteries.

[0028] 2. The closed all-solid-state lithium oxygen battery provided by the present invention can realize the conversion of Li2O, Li2O2, and LiO2 without the intervention of O2. Under the premise of ensuring high discharge specific capacity, no additional oxygen supply device is required, thereby simplifying the battery structure design and having broad application prospects.

[0029] 3. The closed all-solid-state lithium-oxygen battery provided by this invention utilizes a variety of catalysts to address the electron transport problem within the composite cathode. Furthermore, by designing a rational composite cathode ratio, ion transport regulation is achieved, resolving the conflict between electron and ion transport and the porous structure of the electrode in open systems, demonstrating its great potential for application.

[0030] 4. The cathode provided by this invention can be used in a variety of inorganic solid-state batteries, offering advantages such as high energy density, high safety, simple preparation process, and low cost, with the potential for wide operating temperature range. The enclosed all-solid-state lithium-oxygen battery provided by this invention has significant application value in the field of lithium-air batteries. BRIEF DESCRIPTION OF THE DRAWINGS

[0031] The drawings described herein are used to provide a further understanding of the embodiments of the present invention, constitute a part of this application, and do not constitute a limitation of the embodiments of the present invention. In the drawings:

[0032] Figure 1 This is the first cycle charge and discharge curve of Example 1 of the present invention.

[0033] Figure 2 This is the charge and discharge curve of the first cycle of Example 2.

[0034] Figure 3 This is the electrochemical curve of Example 3.

[0035] Figure 4 This is the charge and discharge curve of the first cycle of Example 4.

[0036] Figure 5 This is the charge and discharge curve of the first cycle of Example 5.

[0037] Figure 6 This is the first cycle charge and discharge curve of comparative example 1. DETAILED DESCRIPTION

[0038] In order to make the objectives, technical solutions and advantages of the present invention more clearly understood, the present invention is further described in detail below in conjunction with examples and drawings. The exemplary embodiments of the present invention and their descriptions are only used to explain the present invention and are not intended to limit the present invention.

[0039] Example 1

[0040] (1) Preparation method of oxygen-containing composite positive electrode in this embodiment:

[0041] Step 1: Mix the oxygen-containing compound Li2O and the catalyst MnO2 in a mass ratio of 1:3, and grind them by hand in a mortar for 30 minutes to achieve uniform mixing.

[0042] Step 2 The mixed oxygen-containing composite positive electrode was subjected to high-energy ball milling at a ball-to-material ratio of 40:1 at a rotation speed of 600 rpm for 80 hours to obtain the oxygen-containing composite positive electrode in this embodiment.

[0043] (2) Assembly method of the all-solid-state battery in this embodiment:

[0044] The oxygen-containing composite cathode, Li3InCl6, and CNT were ground in a mortar at a ratio of 50:45:5 for 10 minutes to achieve a uniform mixture. The mixed cathode material was evenly spread throughout a solid-state battery mold and maintained at a pressure of 3 tons for 3 minutes to produce a positive electrode sheet that can be directly used in all-solid-state batteries. The resulting positive electrode sheet was assembled with the Li3InCl6 and Li6PS5Cl electrolyte layers and the Li-In alloy anode to form the all-solid-state battery used in this example.

[0045] The all-solid-state battery in this embodiment was subjected to charge and discharge cycle tests at a rate of 0.05C and a cut-off voltage of 2.0 V to 4.3 V. The test temperature was room temperature. Figure 1 shown.

[0046] Example 2

[0047] (1) Preparation method of oxygen-containing composite positive electrode in this embodiment:

[0048] Step 1: Mix the oxygen-containing compound Li2O and the catalyst MnO2 in a mass ratio of 1:3, and grind them by hand in a mortar for 30 minutes to achieve uniform mixing.

[0049] Step 2 The mixed oxygen-containing composite positive electrode was subjected to high-energy ball milling at a ball-to-material ratio of 40:1 at a rotation speed of 600 rpm for 80 hours to obtain the oxygen-containing composite positive electrode in this embodiment.

[0050] (2) Assembly method of the all-solid-state battery in this embodiment:

[0051] The oxygen-containing composite cathode, Li3InCl6, and CNT were ground in a mortar at a ratio of 50:45:5 for 10 minutes to achieve a uniform mixture. The mixed cathode material was evenly spread throughout a solid-state battery mold and maintained at a pressure of 3 tons for 3 minutes to produce a positive electrode sheet that can be directly used in all-solid-state batteries. The resulting positive electrode sheet was assembled with the Li3InCl6 and Li6PS5Cl electrolyte layers and the Li-In alloy anode to form the all-solid-state battery used in this example.

[0052] The all-solid-state battery in this embodiment was subjected to charge and discharge cycle tests at a rate of 0.05C and a cut-off voltage of 2.0 V to 4.8 V. The test temperature was room temperature. Figure 2 shown.

[0053] Example 3

[0054] (1) Preparation method of oxygen-containing composite positive electrode in this embodiment:

[0055] Step 1: Mix the oxygen-containing compound Li2O and the catalyst Co3O4 in a mass ratio of 65:35, and grind them by hand in a mortar for 30 minutes to achieve uniform mixing.

[0056] Step 2 The mixed oxygen-containing composite positive electrode was subjected to high-energy ball milling at a ball-to-material ratio of 40:1 at a rotation speed of 600 rpm for 80 hours to obtain the oxygen-containing composite positive electrode in this embodiment.

[0057] (2) Assembly method of the all-solid-state battery in this embodiment:

[0058] The oxygen-containing composite cathode, Li3InCl6, and CNT were ground in a mortar at a ratio of 50:45:5 for 10 minutes to achieve a uniform mixture. The mixed cathode material was evenly spread throughout a solid-state battery mold and maintained at a pressure of 3 tons for 3 minutes to produce a positive electrode sheet that can be directly used in all-solid-state batteries. The resulting positive electrode sheet was assembled with the Li3InCl6 and Li6PS5Cl electrolyte layers and the Li-In alloy anode to form the all-solid-state battery used in this example.

[0059] The all-solid-state battery in this embodiment was subjected to charge and discharge cycle tests at a rate of 0.05C and a cut-off voltage of 2.0 V to 3.3 V. The test temperature was room temperature. Figure 3 shown.

[0060] Example 4

[0061] (1) Preparation method of oxygen-containing composite positive electrode in this embodiment:

[0062] Step 1: Mix the oxygen-containing compound Li2O and the catalyst MnO2 in a mass ratio of 1:3, and grind them by hand in a mortar for 30 minutes to achieve uniform mixing.

[0063] Step 2 The mixed oxygen-containing composite positive electrode was subjected to high-energy ball milling at a ball-to-material ratio of 40:1 at a rotation speed of 600 rpm for 80 hours to obtain the oxygen-containing composite positive electrode in this embodiment.

[0064] (2) Assembly method of the all-solid-state battery in this embodiment:

[0065] The oxygen-containing composite cathode, Li6PS5Cl, and CNT were ground in a mortar at a ratio of 50:45:5 for 10 minutes to achieve a uniform mixture. The mixed cathode material was evenly spread throughout a solid-state battery mold and maintained at a pressure of 3 tons for 3 minutes to produce a positive electrode sheet that can be directly used in all-solid-state batteries. The resulting positive electrode sheet was assembled with the Li3InCl6 and Li6PS5Cl electrolyte layers and the Li-In alloy anode to form the all-solid-state battery used in this example.

[0066] The all-solid-state battery in this embodiment was subjected to charge and discharge cycle tests at a rate of 0.05C and a cut-off voltage of 2.0 V to 4.3 V. The test temperature was room temperature. Figure 4 shown.

[0067] Example 5

[0068] (1) Preparation method of oxygen-containing composite positive electrode in this embodiment:

[0069] Step 1: Mix the oxygen-containing compound Li2O and the catalyst Co3O4 in a mass ratio of 65:35, and grind them by hand in a mortar for 30 minutes to achieve uniform mixing.

[0070] Step 2 The mixed oxygen-containing composite positive electrode was subjected to high-energy ball milling at a ball-to-material ratio of 40:1 at a rotation speed of 600 rpm for 80 hours to obtain the oxygen-containing composite positive electrode in this embodiment.

[0071] (2) Assembly method of the all-solid-state battery in this embodiment:

[0072] The oxygen-containing composite cathode, Li3InCl6, and CNT were ground in a mortar at a ratio of 50:45:5 for 10 minutes to achieve a uniform mixture. The mixed cathode material was evenly spread throughout a solid-state battery mold and maintained at a pressure of 3 tons for 3 minutes to produce a positive electrode sheet that can be directly used in all-solid-state batteries. The resulting positive electrode sheet was assembled with the Li3InCl6 and Li6PS5Cl electrolyte layers and the Li-In alloy anode to form the all-solid-state battery used in this example.

[0073] The all-solid-state battery in this embodiment was subjected to charge and discharge cycle tests at a rate of 0.05C, a cut-off voltage of 2.0 V to 3.3 V, and a test temperature of 150°C. Figure 5 shown.

[0074] Comparative Example 1

[0075] Li2O without a catalyst was subjected to high-energy ball milling under the same conditions as in Examples 1 and 2. It was then ground in a mortar with Li3InCl6 and CNT at a ratio of 50:45:5 for 10 minutes to achieve uniform mixing. The mixed positive electrode material was evenly spread across a solid-state molded cell and maintained at a pressure of 3 tons for 3 minutes to produce a positive electrode sheet that can be directly used in all-solid-state batteries. The resulting positive electrode sheet was assembled with the Li3InCl6 and Li6PS5Cl electrolyte layers and a Li-In alloy anode to create the all-solid-state battery described in the comparative example.

[0076] The all-solid-state battery in this comparative example was subjected to charge and discharge cycle tests at a rate of 0.05C and a cut-off voltage of 2.0 V to 4.8 V. The test temperature was room temperature. Figure 6 shown.

[0077] Comparing Examples 1-4 with Comparative Example 1, while Comparative Example 1 fails to achieve its full capacity without a catalyst, the Li2O exhibits extremely high discharge capacity after using different selected catalysts, and this discharge capacity is related to the type of catalyst. Example 5 demonstrates the system's high-temperature operation advantage, potentially expanding its application under extreme conditions.

[0078] The specific implementation methods described above further illustrate the objectives, technical solutions and beneficial effects of the present invention in detail. It should be understood that the above description is only a specific implementation method of the present invention and is not intended to limit the scope of protection of the present invention. Any modifications, equivalent substitutions, improvements, etc. made within the spirit and principles of the present invention should be included in the scope of protection of the present invention.

Claims

1. An oxygen-containing composite cathode material, characterized in that: It includes oxygen-containing compounds and catalysts. The oxygen-containing compounds include one or more of Li2O, Li2O2, KO2, Li2CO3, Li3PO4, and LiNO3. The catalysts include one or more of transition metal oxides, precious metals and their alloys, carbon-based materials, metal-organic frameworks and their derivatives, single-atom catalysts, composite materials, and non-metallic catalysts. The mass proportion of the oxygen-containing compounds is 50%-80%, and the mass proportion of the catalyst is 20%-50%.

2. The method for preparing an oxygen-containing composite cathode material according to claim 1, wherein: It is a solid phase preparation method, including mechanical mixing or sintering methods.

3. The preparation method according to claim 2, characterized in that The mechanical mixing method is high-energy ball milling or ultra-high-energy ball milling, the ball-to-material ratio is 40:1, the rotation speed is 500-600 rpm, and the ball milling time is 80-200 hours; the sintering is specifically: sintering the mixed material, the sintering temperature is 200-500° C., and the sintering time is 2-8 hours.

4. The preparation method according to claim 1, characterized in that The invention is a liquid phase preparation method, which specifically includes the following steps: (1) preparing a mixed precursor solution, specifically including: selecting a lithium source and a transition metal salt compound as precursors, mixing the lithium source with an ethanol solution of the transition metal salt, wherein the molar ratio of the lithium source to the transition metal salt is 1:n, n<10, wherein n is used to adjust the mass percentage of lithium oxide and transition metal oxide in the final completely oxidized product, and then stirring the precursor solution for reaction, filtering and drying, and sintering treatment. The sintering treatment specifically includes: sintering the dried intermediate product at 200-500°C for 1-5 hours in an oxygen atmosphere to obtain a final product of the nanocomposite material and the transition metal oxide.

5. A positive electrode sheet, characterized in that: The invention comprises the oxygen-containing composite positive electrode material as claimed in claim 1, an inorganic solid electrolyte material and a conductive agent.

6. The positive electrode sheet according to claim 5, characterized in that: The conductive agent includes one or more of conductive carbon black, graphite, carbon fiber, carbon nanotube and graphene.

7. The positive electrode sheet according to claim 5, characterized in that: The inorganic solid electrolyte material includes one or more of oxide solid electrolyte, sulfide solid electrolyte, polymer solid electrolyte and halide solid electrolyte.

8. A closed all-solid-state lithium-oxygen battery, characterized in that: The invention comprises the positive electrode sheet as claimed in claim 5, an inorganic solid electrolyte material and a negative electrode material.

9. The sealed all-solid-state lithium-oxygen battery according to claim 8, characterized in that: The test temperature is between 0°C and 150°C.

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