Positive electrode sheet, solid-state battery, electric device and preparation method

Abstract

Provided are a positive electrode sheet, a solid-state battery, an electric device and a preparation method. The positive electrode sheet comprises a positive electrode current collector and an active film layer located on at least one side of the positive electrode current collector, wherein the active film layer comprises a positive electrode active region and a filling region located on at least part of the periphery of the positive electrode active region. The positive electrode active region comprises positive electrode active particles and a sulfide solid electrolyte, and the filling region comprises a positive electrode stabilizer. The positive electrode sheet has significantly improved air stability, and can also significantly inhibit the escape of hydrogen sulfide gas.

Description

Cathode electrode sheet, solid-state battery, power utilization device, and preparation method

[0001] Related applications

[0002] The present application claims priority to the Chinese patent application No.CN202410175721X, filed on February 7, 2024, entitled "Cathode electrode sheet, solid-state battery, power utilization device, and preparation method", the contents of which are hereby incorporated by reference in its entirety. TECHNICAL FIELD

[0003] The present application relates to the technical field of solid-state batteries, further relates to the technical field of all-solid-state batteries, and still further relates to a cathode electrode sheet, a solid-state battery, a power utilization device, and a preparation method, wherein the solid-state battery further relates to an all-solid-state battery. BACKGROUND

[0004] The statements herein are provided only to complement the present application and are not necessarily prior art.

[0005] Solid-state batteries use non-flammable solid electrolytes to replace organic electrolytes in traditional liquid secondary batteries, greatly improving the safety of the batteries and being considered as the closest new generation of batteries to industrialization. All-solid-state batteries are a type of battery that uses solid electrodes and solid-state electrolytes. All-solid-state batteries use solid-state electrolytes to replace the liquid electrolytes in traditional batteries, and the solid-state electrolytes can also simultaneously serve as separators for the positive and negative electrodes, thus eliminating the need for a separator film. Due to the advantages of all-solid-state batteries in safety, energy density, and the like, all-solid-state batteries have been widely concerned in recent years. Among solid-state electrolytes, sulfide electrolytes have attracted much attention due to their excellent ion conduction ability. However, sulfide electrolytes have poor air stability and are sensitive to moisture in the air, easily absorbing moisture in the air and reacting, resulting in the generation of toxic hydrogen sulfide gas and affecting the electrochemical performance of the battery, thus limiting the application of sulfide electrolytes.

[0006] SUMMARY

[0007] According to various embodiments and various examples of the present application, the present application provides a cathode electrode sheet, a solid-state battery, a power utilization device, a preparation method, and an application, wherein the solid-state battery further relates to an all-solid-state battery. The cathode electrode sheet has a positive electrode stabilizer arranged in the blank area of the overhang design, has significantly improved air stability, and the structural design can also significantly inhibit the escape of hydrogen sulfide gas.

[0008] In a first aspect of the application, a positive electrode tab is provided, the positive electrode tab comprising a positive electrode current collector and an active film layer located on at least one side of the positive electrode current collector, the active film layer comprising a positive electrode active region and a filler region located on at least a portion of a periphery of the positive electrode active region; wherein the positive electrode active region comprises positive electrode active particles and a sulfide solid electrolyte; and the filler region comprises a positive electrode stabilizer.

[0009] In some embodiments, the positive electrode stabilizer comprises at least one of a moisture absorbent and a hydrogen sulfide absorbent.

[0010] In some embodiments, a positive electrode tab is provided, the positive electrode tab comprising a positive electrode current collector and an active film layer located on at least one side of the positive electrode current collector, a thickness direction of the active film layer being denoted as a longitudinal direction, and a direction perpendicular to the longitudinal direction being denoted as a transverse direction;

[0011] In the transverse direction, the active film layer comprises a positive electrode active region and a filler region located on at least a portion of a periphery of the positive electrode active region;

[0012] wherein the positive electrode active region comprises positive electrode active particles and a positive electrode solid electrolyte, the positive electrode solid electrolyte comprising a sulfide solid electrolyte; and the filler region comprises a positive electrode stabilizer, the positive electrode stabilizer comprising at least one of a moisture absorbent and a hydrogen sulfide absorbent.

[0013] For the existing solid-state battery (the solid-state battery can be a full solid-state battery) with an overhang structure design, the width of the positive active material layer in the positive electrode layer is less than the width of the negative active material layer in the negative electrode layer. The positive electrode sheet provided by the first aspect of the present application is filled with a stabilizer (denoted as a positive stabilizer) that is beneficial to improving the air stability of the positive electrode material in the corresponding blank area on the positive side. The positive stabilizer includes at least one of a moisture absorber and a hydrogen sulfide absorber. During the preparation of the positive electrode sheet and the assembly of the battery, on the one hand, the filling area can play a certain physical isolation effect on the moisture in the air and the positive active area; on the other hand, the moisture absorber can reduce or avoid the contact probability of the sulfide electrolyte and the moisture, effectively reduce or delay the possibility of the reaction between the sulfide solid electrolyte and the moisture in the air during the process of the positive electrode sheet, inhibit the reaction between the sulfide solid electrolyte and the moisture in the air from the source, reduce or avoid the generation and escape of toxic hydrogen sulfide gas, in addition, the moisture absorber can also improve the material stability in the positive active area, reduce or avoid the adverse effects of the moisture in the air on the moisture-sensitive materials in the positive active area, promote the sulfide solid electrolyte to more stably and effectively play the role of rapid ion conduction, inhibit the increase of the interfacial impedance in the positive electrode sheet, fully exert the capacity of the positive active material and the ion conduction ability of the sulfide solid electrolyte, and thus be beneficial to improving the cycle performance of the assembled solid-state battery (the solid-state battery can be a full solid-state battery); on the other hand, the hydrogen sulfide absorber can absorb the toxic hydrogen sulfide gas generated by the reaction between the sulfide electrolyte and the moisture that may be contacted, and reduce or avoid the escape of the hydrogen sulfide gas.

[0014] In addition, by inhibiting the formation of hydrogen sulfide gas by the sulfide solid electrolyte, the formation of inert by-products in the sulfide solid electrolyte can be reduced, the impedance increase can be inhibited, and thus the rate performance of the battery can be improved.

[0015] In addition, the positive electrode sheet can also be used with a negative electrode sheet of the same size in the transverse direction, which is beneficial to avoiding the shearing of the negative electrode sheet by the positive electrode sheet during high-pressure treatment, and thus is beneficial to avoiding the fracture or powdering of the negative electrode sheet.

[0016] In some embodiments, the positive stabilizer satisfies one or more of the following characteristics:

[0017] The weight percentage of the positive stabilizer in the filling area is 30wt%-99.5wt%, which can be 45wt%-98wt%;

[0018] In the filling area, the mass ratio of the moisture absorber to the hydrogen sulfide absorber is 0-1, which can be 1:9 to 9:1;

[0019] The weight percentage of the moisture absorber in the filling area is 0wt%-99.5wt%, optionally 10wt%-90wt%, further optionally 40wt%-60wt%;

[0020] The weight percentage of the hydrogen sulfide absorber in the filling area is 0wt%-99.5wt%, optionally 10wt%-90wt%, further optionally 40wt%-60wt%.

[0021] By adjusting one or more of the following parameters: the weight percentage of the positive electrode stabilizer in the filling area (R0 M ), the mass ratio of the moisture absorber and the hydrogen sulfide absorber in the filling area (R H2O / H2S ), the weight percentage of the moisture absorber in the filling area (R1 H2O ), and the weight percentage of the hydrogen sulfide absorber in the filling area (R1 H2S ), the content of the positive electrode stabilizer in the positive electrode sheet can be adjusted, so as to better reduce or avoid the contact probability of the sulfide electrolyte with moisture, and further reduce or avoid the escape of hydrogen sulfide gas.

[0022] By controlling R1 H2O Within the aforementioned range, the content of the moisture absorber in the positive electrode sheet can be adjusted, which is not only conducive to better reducing or avoiding the contact probability of the sulfide electrolyte with moisture, reducing or avoiding the generation and escape of hydrogen sulfide gas, but also conducive to better enhancing the material stability of the positive active area, promoting the sulfide solid electrolyte to more effectively and stably play the role of rapid ion conduction, and more conducive to improving the electrochemical performance of the secondary solid-state battery (the solid-state battery can be a full solid-state battery) assembled by using the positive electrode sheet, such as being conducive to achieving better cycle performance.

[0023] By controlling R1 H2S Within the aforementioned range, it is conducive to better reducing or avoiding the escape of hydrogen sulfide gas.

[0024] In some embodiments, the positive electrode stabilizer satisfies one or more of the following characteristics:

[0025] The positive electrode stabilizer comprises the moisture absorber, and the moisture absorber comprises one or more of a physical water absorber and a chemical water absorber;

[0026] The positive electrode stabilizer comprises the hydrogen sulfide absorber, and the hydrogen sulfide absorber comprises one or more of a hydrogen sulfide physical absorber and a hydrogen sulfide chemical absorber.

[0027] In some embodiments, the positive electrode stabilizer satisfies one or more of the following characteristics:

[0028] The moisture absorbent includes a physical moisture absorbent, and the physical moisture absorbent includes one or more moisture absorbents selected from the group consisting of silica gel, molecular sieve, metal organic framework, and porous carbon; wherein the moisture absorbent of the porous carbon includes activated carbon;

[0029] The moisture absorbent includes a chemical moisture absorbent, and the chemical moisture absorbent includes one or more moisture absorbents selected from the group consisting of CaCl2, CaH2, anhydrous CuSO4, LiCl, FeCl3, FeO(OH), KMnO4, Na2CO3, Fe2O3, Fe(OH)3, ZnO, CuO, NiO, and Al2O3.

[0030] The hydrogen sulfide absorbent includes a hydrogen sulfide physical absorbent, and the hydrogen sulfide physical absorbent includes one or more hydrogen sulfide absorbents selected from the group consisting of activated carbon, molecular sieve, and metal organic framework.

[0031] The hydrogen sulfide absorbent includes a hydrogen sulfide chemical absorbent, and the hydrogen sulfide chemical absorbent includes one or more hydrogen sulfide absorbents selected from the group consisting of Fe2O3, ZnO, Bi2O3, CuO, and MnO.

[0032] The type of at least one of the moisture absorbent and the hydrogen sulfide absorbent can be flexibly selected to better achieve the effect of reducing or avoiding the escape of hydrogen sulfide gas. Among them, by flexibly selecting the moisture absorbent, the contact probability of the sulfide electrolyte and moisture can be better reduced or avoided, thereby reducing or avoiding the effect of hydrogen sulfide gas escaping, promoting the sulfide solid electrolyte to play a more stable and effective role, and better improving the cycle performance of the battery.

[0033] In some embodiments, the positive electrode stabilizer includes a dual absorbent, which refers to a substance that simultaneously serves as the moisture absorbent and the hydrogen sulfide absorbent.

[0034] The dual absorbent includes one or more of a dual physical absorbent and a dual chemical absorbent; the dual physical absorbent refers to a substance that simultaneously absorbs moisture and hydrogen sulfide based on physical action, and the dual chemical absorbent refers to a substance that simultaneously absorbs moisture and hydrogen sulfide based on chemical action.

[0035] In some embodiments, the positive electrode stabilizer satisfies one or more of the following characteristics:

[0036] The positive electrode stabilizer includes the dual physical absorbent, and the dual physical absorbent includes one or more selected from the group consisting of activated carbon, molecular sieve, and metal organic framework.

[0037] The positive electrode stabilizer includes the dual chemical absorbent, and the dual chemical absorbent includes one or more selected from the group consisting of ZnO and CuO.

[0038] When the positive electrode stabilizer includes a dual-absorbing agent, the water-absorbing agent and the hydrogen sulfide-absorbing agent can simultaneously play a role, which is conducive to more effectively reducing or avoiding the escape of hydrogen sulfide and improving the material and performance stability of the positive electrode active area, and better improving the cycle performance of the battery.

[0039] In some embodiments, the positive electrode stabilizer includes the dual chemical absorbing agent and the dual physical absorbing agent, and the dual physical absorbing agent includes one or more of activated carbon and molecular sieve.

[0040] When one or more of activated carbon and molecular sieve is used as a physical absorbing agent in combination with a dual chemical absorbing agent, the effect of simultaneously absorbing water and hydrogen sulfide is better.

[0041] In some embodiments, the filling area further includes a first binder; the first binder includes one or more of a rubber-based binder, carboxymethyl cellulose, a polyolefin-based binder, a polyurethane-based binder, a polyacrylate-based binder, a polyacrylic resin, polyvinylidene fluoride, polytetrafluoroethylene, a vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, a vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene terpolymer, and a tetrafluoroethylene-hexafluoropropylene copolymer.

[0042] The rubber-based binder includes at least one of a fluorinated rubber-based binder or a rubber-based binder without fluorine elements.

[0043] The polyacrylate-based binder includes at least one of a fluorine-containing acrylate resin or a polyacrylate-based binder without fluorine elements.

[0044] In some embodiments, the first binder includes one or more of styrene butadiene rubber, nitrile rubber, hydrogenated nitrile rubber, a polyacrylic resin, and a polyurethane-based binder.

[0045] In some embodiments, the weight percentage of the first binder in the filling area is 0.5wt% to 5wt%, which can be optionally 2wt% to 4wt%.

[0046] By arranging the binder in the filling area, the cohesion between the filling components in the filling area can be enhanced, so that the filling state of the positive electrode stabilizer and other components is more stable, and the filling area can function more durably and stably. Further, by adjusting the weight percentage of the binder in the filling area within the above range, the binder can fully and durably play a role while fully playing the above-mentioned role.

[0047] In some embodiments, the filling area includes the first binder, and the positive electrode active area includes a second binder; the first binder and the second binder are of the same type.

[0048] The filling area and the positive active area use the same kind of binder, which is conducive to improving the adhesion strength of the filling area on the positive current collector.

[0049] In some embodiments, the filling area further comprises an insulating material.

[0050] In some embodiments, the filling area satisfies one or more of the following characteristics:

[0051] The insulating material comprises one or more of inorganic oxide insulating material, boehmite, non-woven fabric fiber and fibrous resin; optionally, the inorganic oxide insulating material comprises one or more of Al2O3, MgO, SiO2, BaTiO3, BaCO3, Fe3O4, TiO2, Y2O3, Mn2O3 and Mn2O7;

[0052] The weight percentage of the insulating material in the filling area is less than or equal to 69wt%, and optionally 1wt% to 50wt%;

[0053] In the filling area, the mass ratio of the insulating material to the positive stabilizer is less than or equal to 2, and optionally 0.5 to 1.

[0054] By setting the insulating material in the filling area, on the one hand, the risk of internal short circuit can be better avoided, and on the other hand, the distribution concentration of the positive stabilizer can be adjusted, which can assist in adjusting the content of the positive stabilizer in the filling area. The type of insulating material can be flexibly selected accordingly.

[0055] By adjusting one or both of the "weight percentage of the insulating material in the filling area" and the "mass ratio of the insulating material to the positive stabilizer in the filling area" within the above range, it is conducive to better avoiding the risk of internal short circuit while flexibly setting the appropriate content of the positive stabilizer in the filling area.

[0056] In some embodiments, the positive active particles comprise a positive active body and a coating layer located on at least a part of the surface of the positive active body, the positive active body comprises one or more of lithium transition metal oxide and lithium-containing phosphate, and the coating layer comprises lithium oxide compound.

[0057] In some embodiments, the lithium oxide compound satisfies one or more of the following characteristics:

[0058] The lithium oxide compound comprises one or more elements of B, Nb, Zr, Si, P, Mn, Zn, Al, Fe and Na;

[0059] The weight percentage of the lithium oxide compound in the positive active particles is 0.1wt% to 5wt%.

[0060] In some embodiments, the lithium-oxygen compound satisfies one or more of the following characteristics:

[0061] The lithium-oxygen compound includes one or more of Li3BO3, LiNbO3, Li2ZrO3, Li2SiO3, LiPO3, and Li2MnO4;

[0062] The lithium-oxygen compound has a weight percentage in the positive electrode active particles of 0.1wt% to 2wt%.

[0063] By arranging the coating layer on the surface of the positive electrode active body, it is beneficial to physically isolate the positive electrode active body from the sulfide solid electrolyte while maintaining certain ion conductivity, which can inhibit the occurrence of side reactions due to space charge when the positive electrode active body and the sulfide solid electrolyte are in contact, inhibit the decomposition of the sulfide solid electrolyte, reduce the interface impedance, and help the positive electrode active body to fully exert its capacity, and more beneficial to improve the cycle performance of the battery.

[0064] By adjusting the weight percentage of the lithium-oxygen compound in the positive electrode active particles within the aforementioned range, it is beneficial to achieve higher energy density while fully exerting the improvement effect of the coating layer.

[0065] In some embodiments, the sulfide solid electrolyte includes at least one of a binary sulfide solid system and a ternary sulfide solid system;

[0066] The binary sulfide solid system includes one or more of Li2S-P2S5, Li2S-SiS2, Li2S-GeS2, and Li2S-B2S3;

[0067] The ternary sulfide solid system includes one or more of argyrodite-type sulfide electrolyte, Li2S-MeS2-P2S5 ternary sulfide electrolyte, lithium-germanium-phosphorus-sulfur type sulfide electrolyte, Li2S-P2S5-MS ternary sulfide electrolyte, Li2S-P2S5-MCl ternary sulfide electrolyte, and thio-LISICON type sulfide electrolyte; wherein Me includes one or more elements of Si, Ge, Sn, and Al; and M includes one or more elements of Ge, Al, Sn, Pb, Sb, Si, and As.

[0068] In the case of arranging the filling area, the selection of the sulfide solid electrolyte is not necessarily limited by the strength of hygroscopicity, and the type of sulfide solid electrolyte can be more flexibly selected according to the needs of one or more aspects such as ion conductivity, electrochemical window range, electrical conductivity, particle size, etc.

[0069] In some embodiments, the cathode stabilizer includes a moisture absorbent, and the cathode solid electrolyte further includes a halide solid electrolyte;

[0070] Optionally, the halide solid electrolyte includes lithium element, halogen and X element, wherein the X element includes one or more of Y, In, Zr, Sc, Ho, Mn, Cd and Pb, and the halogen includes one or more of Cl, Br and I.

[0071] In some embodiments, the halide solid electrolyte includes one or more of Li3X 1 Cl6, LiX 1 I4, LiX 1 I3 and Li3X 1 Br6, and X in the halide solid electrolyte includes one or more of Y, In, Sc, Ho, Mn, Cd and Pb. 1

[0072] When the cathode solid electrolyte further includes a halide solid electrolyte that is easy to physically absorb moisture, the cathode active material layer can face a more serious moisture absorption problem, and the moisture absorption caused by the halide solid electrolyte can further exacerbate the instability of the sulfide solid electrolyte. At this time, by adopting the cathode tab structure design of the first aspect of the present application and setting a moisture absorbent in the cathode stabilizer, more significant improvement in the air stability of the cathode tab can be achieved. The moisture absorbent can significantly reduce or avoid the absorption of moisture by the cathode active area, reduce or avoid the escape of hydrogen sulfide gas, and more significantly improve the material stability and performance stability of the cathode active area (including the sulfide solid electrolyte), which is more conducive to improving the electrochemical performance of the assembled solid-state battery (the solid-state battery can be a full solid-state battery), for example, the cycle performance of the battery can be better improved.

[0073] In some embodiments, the cathode active area has a first side and a second side facing away from each other, and the first side and the second side respectively intersect with the transverse direction;

[0074] The filling area is arranged outside the opposite regions of the first side and the second side, respectively.

[0075] By arranging the filling area on both sides of the transverse direction of the cathode active area, it is beneficial to better isolate the cathode active area from the contact with moisture in the air and reduce or avoid the escape of hydrogen sulfide gas when assembling the solid-state battery (the solid-state battery can be a full solid-state battery).

[0076] In some embodiments, the first side and the second side are completely covered by the filling area.

[0077] ​When the filling region completely covers two sides of the positive active region in the width direction, it is beneficial to better isolate the positive active region from the contact with moisture in the air when assembling the solid-state battery (the solid-state battery can be a full solid-state battery), and to reduce or avoid the escape of hydrogen sulfide gas.

[0078] In some embodiments, in the lateral direction, the positive active region is completely surrounded by the filling region.

[0079] When the filling region completely surrounds the positive active region in the lateral direction, it is beneficial to better isolate the positive active region from the contact with moisture in the air when assembling the solid-state battery (the solid-state battery can be a full solid-state battery), and to reduce or avoid the escape of hydrogen sulfide gas.

[0080] In some embodiments, the width of the filling region at different positions along the outer side of the positive active region is greater than or equal to 0.2 mm, optionally 0.2 mm to 10 mm, and further optionally 0.5 mm to 10 mm, in terms of the projected area of the filling region in the lateral direction.

[0081] By controlling the width of the filling region located outside the positive active region within a certain range, it is possible to reduce or avoid the contact of the positive active region with moisture in the air, and in addition, by further selecting a suitable range, it is also possible to achieve a higher energy density at the same time. In addition, the above width setting can effectively avoid internal short circuit caused by volume change of the electrode sheet, shear of the overhang region during charging and discharging, etc. during the battery cycle.

[0082] In some embodiments, the volume ratio of the filling region to the positive active region is greater than or equal to 0.2%, optionally 0.2% to 20%, and further optionally 0.5% to 10%.

[0083] By controlling one or both of the mass ratio and the volume ratio of the filling region in the positive active region within the aforementioned range, it is beneficial to reduce or avoid the contact of the positive active region with moisture in the air, and in addition, by further selecting a suitable range, it is also possible to achieve a higher energy density at the same time.

[0084] In some embodiments, the thickness of the active film layer at different lateral positions is equal.

[0085] When the thickness of the active film layer at different lateral positions is equal, there is no height difference between the positive active region and the filling region on the side surface of the active film layer away from the positive current collector, and therefore, when the positive electrode sheet is used in cooperation with the negative electrode sheet and subjected to high pressure treatment, it is beneficial to avoid the positive electrode sheet shearing the negative electrode sheet, and to avoid the negative electrode sheet breaking or powdering.

[0086] In a second aspect of the present application, a solid-state battery is provided, which comprises a positive electrode layer, a solid electrolyte layer and a negative electrode layer arranged in sequence, wherein the positive electrode layer comprises the positive electrode tab according to the first aspect of the present application.

[0087] In some embodiments, the solid-state battery is a full solid-state battery.

[0088] In some embodiments, a full solid-state battery is provided, which comprises a positive electrode layer, a solid electrolyte layer and a negative electrode layer arranged in sequence, wherein the positive electrode layer comprises the positive electrode tab according to the first aspect of the present application.

[0089] In some embodiments, the projection area of the positive electrode layer, the solid electrolyte layer and the negative electrode layer along the longitudinal direction is consistent.

[0090] By arranging the positive electrode layer, the solid electrolyte layer and the negative electrode layer in equal size and in alignment in the lateral direction, the projection area of the three layers along the longitudinal direction is consistent (at this time, the side surfaces of each structural layer are arranged in alignment), which is beneficial to reducing the structural layer fracture or powder dropping caused by interlayer shearing during high pressure treatment.

[0091] In a third aspect of the present application, an electric device is provided, which comprises the solid-state battery according to the second aspect of the present application.

[0092] In some embodiments, an electric device is provided, which comprises the full solid-state battery according to the second aspect of the present application.

[0093] In a fourth aspect of the present application, a preparation method of a full solid-state battery is provided, which comprises the following steps:

[0094] providing a substrate comprising a solid electrolyte layer and a negative electrode layer arranged in sequence, wherein the negative electrode layer is located on one side of the solid electrolyte layer;

[0095] compositing the positive electrode tab according to the first aspect of the present application on the side of the solid electrolyte layer away from the negative electrode layer to prepare a solid-state battery;

[0096] Optionally, the solid-state battery is a full solid-state battery.

[0097] In some embodiments, a preparation method of a full solid-state battery is provided, which comprises the following steps:

[0098] providing a substrate comprising a solid electrolyte layer and a negative electrode layer arranged in sequence, wherein the negative electrode layer is located on one side of the solid electrolyte layer;

[0099] compositing the positive electrode tab according to the first aspect of the present application on the side of the solid electrolyte layer away from the negative electrode layer to prepare a full solid-state battery.

[0100] The details of one or more implementations or embodiments of the application are set forth in the accompanying drawings and the description below. Other features, objects, and advantages of the application will be apparent from the description, drawings, and claims. BRIEF DESCRIPTION OF DRAWINGS

[0101] To better describe and illustrate the implementations, embodiments, or examples provided by the present application, reference can be made to one or more drawings. Additional details or examples used to describe the drawings should not be considered as limiting the scope of any of the disclosed applications, the presently described implementations, embodiments, or examples, and the best mode presently contemplated of these applications. It is also noted that each of the drawings is presented in a simplified form and is used only to facilitate the description of the present application. The various dimensions of each component shown in the drawings are arbitrarily shown and can be drawn to scale or not drawn to scale. For example, the dimensions of the components in some places in the drawings are exaggerated for the sake of clarity. Each component in the drawings is not drawn to scale unless specifically stated. The drawings of the present application do not limit the size of each component.

[0102] Moreover, in all the drawings, the same reference numbers are used to represent the same components.

[0103] In the drawings:

[0104] FIG. 1 is a schematic diagram of the structure and internal components of a positive electrode tab according to an embodiment of the present application, showing a longitudinal cross-section.

[0105] FIG. 2 is a schematic diagram of the structure of a positive electrode tab according to an embodiment of the present application, showing a longitudinal cross-section.

[0106] FIG. 3 is a schematic diagram of the structure and internal components of a positive electrode tab according to an embodiment of the present application, showing a longitudinal cross-section.

[0107] FIG. 4 is a schematic diagram of the structure and internal components of a positive electrode tab according to an embodiment of the present application, showing a longitudinal cross-section.

[0108] FIG. 5 is a schematic diagram of the structure of a positive electrode tab according to an embodiment of the present application, showing a transverse cross-section.

[0109] FIG. 6 is a schematic diagram of the structure of a positive electrode tab according to an embodiment of the present application, showing a transverse cross-section.

[0110] FIG. 7 is a schematic diagram of the structure of a full solid-state battery cell according to an embodiment of the present application.

[0111] FIG. 8 is a schematic diagram of the structure of a full solid-state battery cell according to an embodiment of the present application.

[0112] FIG. 9 is a schematic diagram of the structure of a full solid-state battery cell according to an embodiment of the present application.

[0113] FIG. 10 is a schematic view of an all-solid-state battery cell according to an embodiment of the present application.

[0114] FIG. 11 is an exploded view of the all-solid-state battery cell shown in FIG. 10 according to an embodiment of the present application.

[0115] FIG. 12 is a schematic view of a battery module according to an embodiment of the present application.

[0116] FIG. 13 is a schematic view of a battery pack according to an embodiment of the present application.

[0117] FIG. 14 is an exploded view of the battery pack shown in FIG. 13 according to an embodiment of the present application.

[0118] FIG. 15 is a schematic view of an electric device using an all-solid-state battery as a power source according to an embodiment of the present application.

[0119] Regarding reference numerals: 10, positive electrode tab; 110, positive electrode current collector; 120, positive electrode active region; 130, filling region; 121, positive electrode active particle; 122, positive electrode solid electrolyte; 131, positive electrode stabilizer; 132, first binder; 133, insulating material; 100, positive electrode layer; 200, solid electrolyte layer; 300, negative electrode layer; 310, negative electrode current collector; 320, negative electrode active material layer; Y, longitudinal direction; X1, width direction of the positive electrode active region in the lateral direction; X2, length direction of the positive electrode active region in the lateral direction; 1, battery pack; 2, upper case; 3, lower case; 4, battery module; 5, all-solid-state battery cell; 51, housing; 52, all-solid-state battery cell; 53, cover plate; 6, electric device; 10, positive electrode tab.

[0120] It can be understood that the drawing sizes of the positive electrode layer 100, the positive electrode current collector 110, the positive electrode active region 120, the filling region 130, the solid electrolyte layer 200, the negative electrode layer 300, the negative electrode current collector 310, and the negative electrode active material layer 320 in each drawing do not represent actual sizes. The shapes and sizes of the positive electrode active particle 121, the positive electrode solid electrolyte 122, the positive electrode stabilizer 131, the first binder 132, and the insulating material 133 involved in the drawings do not represent or limit the shapes and sizes of actual particles, and the illustrated number of each component does not represent or limit the actual number and number ratio. DETAILED DESCRIPTION

[0121] Hereinafter, some embodiments of the positive electrode tab, the solid-state battery, the all-solid-state battery, the power-using device, and the manufacturing method of the present application are described in detail with appropriate reference to the accompanying drawings. However, there are cases where unnecessary detailed explanations are omitted. For example, there are cases where detailed explanations of matters that are already well known, repeated explanations of actually identical structures are omitted. This is to avoid the following description from becoming unnecessarily lengthy and to facilitate understanding by those skilled in the art. Furthermore, the accompanying drawings and the following description are provided so that those skilled in the art can fully understand the present application, and are not intended to limit the subject matter recited in the claims.

[0122] The "ranges" disclosed in the present application can be defined in the form of a lower limit and an upper limit, a given range is defined by selecting a lower limit and an upper limit, and the selected lower limit and upper limit define the boundaries of the particular range. The ranges defined in this way can be inclusive or exclusive of the end values, either end value can be included or excluded independently, and can be arbitrarily combined, that is, any lower limit can be combined with any upper limit to form a range. For example, if the ranges 60-120 and 80-110 are listed for a particular parameter, it is understood that the ranges 60-110 and 80-120 are also contemplated. Furthermore, if the minimum range values 1 and 2 are listed, and if the maximum range values 3, 4, and 5 are also listed, the following ranges are all contemplated: 1-3, 1-4, 1-5, 2-3, 2-4, and 2-5. In the present application, unless otherwise specified, the numerical range "a-b" represents a shorthand notation for any real combination of numbers between a and b, where a and b are both real numbers. For example, the numerical range "0-5" means that all real numbers between "0-5" have been listed herein, and "0-5" is just a shorthand notation for these numerical combinations. In addition, when it is stated that a certain parameter is an integer ≥ 2, it is equivalent to listing the parameter as, for example, integer 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, and so on. For example, when it is stated that a certain parameter is an integer selected from "2-10", it is equivalent to listing the integers 2, 3, 4, 5, 6, 7, 8, 9, and 10.

[0123] In the present application, unless otherwise specified, "about" means within a reasonable range around the number, and the fluctuation range can vary depending on the type and value of the number. For example, a range of ±10%, ±5%, ±2%, ±1%, and so on can be allowed. For example, taking "about 20°C" with an approximation of ±1°C as an example, the approximation values of 19°C, 19.5°C, and so on within the approximation range indicated by "about 20°C" should also be included in the range indicated by "about 20°C".

[0124] In the present application, as no specific limitation, the term "a value" is intended to include the value itself and its reasonable approximation, and the definition of the "value" can be applied to discrete value points and also to the end points of a value range. In the present application, as no specific limitation, the term "a value" or "a value range" is intended to include the value itself and its reasonable approximation, and the definition of the "value" or "the value range" can be applied to discrete value points and also to the end points of a value range. It is understood by those skilled in the art that the range of acceptable fluctuations associated with the relevant approximation can be included in the definition of the "value" or "the value range". In the present application, as no specific limitation, "N1" can be reasonably understood as "about N1", and "N1-N2" can be reasonably understood as "about N1 to about N2", wherein N1 and N2 are two unequal values. For example, in some cases, due to one or more factors such as the reasonable deviation allowed in the art, the accuracy of instrument control, etc., it is reasonable to include the approximate values within the range of the approximation range in the range defined by the value range; for example, "temperature 20-30°C" can be understood as "about 20-30°C"; further, taking "20°C" as the end point and its approximation ±1°C as an example, the approximate values within the approximation range of 19°C, 19.5°C, etc. should also be included in the range indicated by 20-30°C. As a non-limiting example, the percentage "10%" can be reasonably understood as "about 10%". As another non-limiting example, the percentage "2%-10%" can be reasonably understood as "about 2%-about 10%". As another non-limiting example, the percentage "0%" at least includes "none", and can also include the case of "below the detection limit".

[0125] In the present application, as no specific limitation, the terms "a plurality of", "a plurality of kinds", "a plurality of items", "several", etc. mean more than two or equal to two in number. For example, "one or more" means one or ≥(greater than or equal to) two. It can be understood that, when referring to "any plurality" of items, it means any suitable combination of a plurality of items, i.e. in a manner that does not conflict and can implement the present application.

[0126] If not specifically stated, all embodiments and optional embodiments of the present application can be combined with each other to form new technical solutions.

[0127] In the present application, the phrase "embodiment" means that the specific features, structures or properties described in connection with the embodiment can be included in at least one embodiment or embodiment of the present application. The appearance of this phrase in various places in the specification does not necessarily mean the same embodiment, nor is it a separate or alternative embodiment independent of or alternative to other embodiments. It is explicitly and implicitly understood by those skilled in the art that the embodiments described herein can be combined with other embodiments. The term "embodiment" is similarly understood herein.

[0128] It is understood by those skilled in the art that the order of writing each step in the method of each embodiment or example does not mean a strict execution order and does not constitute any limitation on the implementation process. The detailed execution order of each step should be determined by its function and possible internal logic. If not specifically stated, all steps of the present application can be performed sequentially or randomly, and can be preferably performed sequentially. For example, method M includes steps (a) and (b), which means that the method can include sequentially performed steps (a) and (b), or sequentially performed steps (b) and (a). For example, method M also includes step (c), which means that step (c) can be added to method M in any order, for example, method M can include steps (a), (b) and (c), or steps (a), (c) and (b), or steps (c), (a) and (b), etc.

[0129] In the present application, the open technical features or technical solutions described with the words "containing", "including", "comprising" and the like do not exclude additional members other than the listed members, and can be regarded as providing both a closed feature or solution composed of the listed members and an open feature or solution including additional members in addition to the listed members. For example, A includes a1, a2 and a3, and unless otherwise specified, it can also include other members or can not include additional members, and can be regarded as providing both the feature or solution that "A is composed of a1, a2 and a3" or "A is selected from a1, a2 and a3", and the feature or solution that "A includes not only a1, a2 and a3, but also other members".

[0130] In the present application, A (such as B) means that B is a non-limiting example of A, and A can be understood as not limited to B, unless otherwise specified.

[0131] In the present application, "optionally", "optional" and "optional" mean that it can or can not be present, i.e. it can be selected from either of the two parallel solutions "yes" or "no". If there are multiple "options" in a technical solution, and unless otherwise specified, there is no contradiction or mutual restriction. Each "option" is independent. Unless otherwise specified, "optionally includes", "optionally contains" and the like are described in the present application, for example, "optionally includes" means "may include or not include".

[0132] In the present application, "and / or" corresponding features or solutions include any one of two or more related listed items, and also includes any and all combinations of related listed items, wherein any and all combinations include combinations of any two related listed items, any more related listed items, or all related listed items. For example, "A and / or B" represents a group consisting of A, B, and a combination of A and B. Wherein "including A and / or B" can represent "including A, including B, and including A and B", and can also represent "including A, including B, or including A and B", which can be properly understood according to the sentence.

[0133] As used herein, "combinations thereof", "any combination thereof", "any combination manner thereof" and the like include all suitable combination manners of any two or more listed items.

[0134] As used herein, "suitable combination manner", "suitable manner", "any suitable manner" and the like are subject to the implementation of the technical solutions of the present application.

[0135] As used herein, "preferred", "better", "better", "appropriate", "better", "better" are only to describe the implementation mode or embodiment with better effect, and it should be understood that it does not constitute a limitation on the protection scope of the present application. If there are multiple "preferred" in a technical solution, each "preferred" is independent of each other if there is no special description, and there is no contradictory relationship or mutual restriction.

[0136] In the present application, "further", "more further", "in particular", "for example", "such as", "example", "for example" are used for description purposes, indicating differences in content, but should not be understood as limiting the protection scope of the present application.

[0137] In the present application, in the "first aspect", "second aspect", "third aspect", "fourth aspect" and the like, the terms "first", "second", "third", "fourth" and the like are only for description purposes, and cannot be understood as indicating or implying relative importance or quantity, nor can it be understood as implicitly indicating the importance or quantity of the indicated technical features. Moreover, "first", "second", "third", "fourth" and the like only serve the purpose of non-exhaustive enumeration and description, and should be understood as not constituting a closed limitation on the quantity.

[0138] In the present application, unless specifically stated and limited otherwise, a first feature is "on" or "under" a second feature can mean that the first and second features are in direct contact, or the first and second features are in indirect contact through an intermediate medium. In the present application, unless specifically stated and limited otherwise, a first feature is "on" or "under" a second feature can mean a horizontal height reciprocal position relationship, or can only mean an existence of an attachment relationship without limiting the horizontal height reciprocal position relationship.

[0139] In the present application, the term "room temperature" generally refers to 4℃ to 35℃, and can refer to 20℃±5℃. In some embodiments or examples of the present application, room temperature refers to 20℃ to 30℃.

[0140] In the present application, the units related to the data range, if only the right end point is followed by a unit, it means that the units of the left end point and the right end point are the same. For example, 3-5h or 3-5h both mean that the units of the left end point "3" and the right end point "5" are both h (hour), and both have the same meaning as 3h-5h. In addition, similar descriptions of other parameters such as temperature, size, etc. are also understood in the same way.

[0141] The weight or mass of the related components mentioned in the embodiments or examples of the present application can not only refer to the content of each component, but also represent the proportional relationship between the weight or mass of each component, so as long as the content of the related components in the embodiments or examples of the present application is enlarged or reduced in proportion, it is within the scope described in the present application. Further, the mass involved in the embodiments or examples of the present application can be micrograms (μg), milligrams (mg), grams (g), kilograms (kg), etc. Mass units well known in the chemical field. If not otherwise stated, the mass ratio is numerically equal to the corresponding weight ratio, for example, the mass of substance A is m1, the weight is W1, the mass of substance B is m2, and the weight is W2. The mass ratio m1 / m2 is numerically equal to the corresponding weight ratio W1 / W2.

[0142] In the present application, unless otherwise stated, wt% means weight percentage by weight, which is numerically equal to the corresponding mass percentage by mass. In the present application, for weight percentage, "0" has the same meaning as "0wt%" and can be used interchangeably.

[0143] In the present application, unless otherwise stated, the parameter units involved are nm for nanometer, μm for micrometer, V for volt, mPa·S for millipascal·second, mg / cm 2 mg / cm 2 g / cm 3 g / cm

[0144] In the present application, "greater than or equal to", "greater than or equal to" and "≥" have the same meaning and can be used interchangeably; "less than or equal to", "less than or equal to" and "≤" have the same meaning and can be used interchangeably; "greater than" can be equivalent to ">"; "less than" can be equivalent to "<". In the present application, unless otherwise stated, "greater than or equal to" and "≥" can be considered to provide both "greater than" and "equal to" options. In the present application, unless otherwise stated, "less than or equal to" and "≤" can be considered to provide both "less than" and "equal to" options.

[0145] In the present application, the exemplary description involving "in some embodiments (or examples)", "in one embodiment (or example)" and the like can cover but is not limited to the following meanings: these options can be combined with other options in a suitable manner to form new technical solutions.

[0146] In the present application, unless otherwise stated, the "solid-state battery" provided in the present application refers to a battery in which the electrolyte in the battery comprises a solid electrolyte; generally, the solid-state battery comprises a positive electrode layer, a solid electrolyte layer and a negative electrode layer. During the charging and discharging process of the battery, active ions are embedded and extracted between the positive electrode layer and the negative electrode layer. The solid electrolyte layer plays a role in conducting ions between the positive electrode layer and the negative electrode layer, and can also isolate the positive electrode layer from the negative electrode layer to prevent short circuiting of the positive and negative electrodes, therefore, the solid-state battery can not be provided with a separator film in the traditional lithium-ion battery. The solid-state battery uses a non-flammable solid electrolyte to replace the organic electrolyte in the traditional liquid lithium-ion battery, greatly improving the safety of the battery. In addition to improving safety, the solid-state battery can also better adapt to high-energy-density positive and negative electrode materials, and reduce system weight, which is conducive to improving energy density.

[0147] In the present application, unless otherwise stated, the "all-solid-state battery" provided in the present application refers to a battery in which the electrolyte in the battery comprises a solid electrolyte; generally, the all-solid-state battery comprises a positive electrode layer, a solid electrolyte layer and a negative electrode layer. During the charging and discharging process of the battery, active ions are embedded and extracted between the positive electrode layer and the negative electrode layer. The solid electrolyte layer plays a role in conducting ions between the positive electrode layer and the negative electrode layer, and can also isolate the positive electrode layer from the negative electrode layer to prevent short circuiting of the positive and negative electrodes, therefore, the all-solid-state battery can not be provided with a separator film in the traditional lithium-ion battery.

[0148] In the present application, unless otherwise stated, "solid electrolyte" refers to an electrolyte material or electrolyte substance that exists in a solid state during the storage and preparation of the solid-state battery and during the working process of the solid-state battery. It can be understood that the solid electrolyte exists in a solid state at room temperature, including but not limited to.

[0149] In the present application, the electrode layer is a functional layer containing active material, which can be a positive electrode layer or a negative electrode layer, and the "active material" in the electrode layer refers to a material capable of reversibly intercalating and deintercalating active ions. Unless otherwise specified, "negative electrode active material" refers to a material capable of reversibly intercalating and deintercalating active ions used in the negative electrode layer; "positive electrode active material" refers to a material capable of reversibly deintercalating and intercalating active ions used in the positive electrode layer. When the solid-state battery or the all-solid-state battery is charged, the active ions are deintercalated from the positive electrode, intercalated into the negative electrode through the solid electrolyte layer; and when the solid-state battery or the all-solid-state battery is discharged, the active ions are deintercalated from the negative electrode and intercalated into the positive electrode. The active ion is not particularly limited, and non-limitingly, the active ion in the solid-state battery can be lithium ion, which corresponds to a lithium ion solid-state battery; the active ion in the all-solid-state battery can be lithium ion, which corresponds to a lithium ion all-solid-state battery.

[0150] In the present application, "electrode active material", "electrode active substance", "active material" and "active substance" have the same meaning and can be used interchangeably; "positive electrode active material" and "positive electrode active material" have the same meaning and can be used interchangeably; "negative electrode active material" and "negative electrode active material" have the same meaning and can be used interchangeably. "Positive electrode active material" and "positive electrode active material" have the same meaning and can be used interchangeably; "negative electrode active material" and "negative electrode active material" have the same meaning and can be used interchangeably.

[0151] Regarding the positive electrode sheet in the solid-state battery, taking the positive electrode sheet in the all-solid-state battery as an example, it is usually necessary to add a solid electrolyte to promote the conduction of lithium ions. Among them, sulfide electrolyte has become a solid electrolyte material of great concern due to its excellent ion conduction ability. However, the air stability of sulfide electrolyte is poor, and it is sensitive to moisture in the air, which can easily absorb moisture in the air and react, resulting in the generation of toxic hydrogen sulfide gas. In the preparation process of the positive electrode sheet, it is inevitable to contact the moisture in the air. The air instability of sulfide electrolyte causes the positive electrode sheet to release highly toxic hydrogen sulfide gas during the preparation and assembly of the all-solid-state battery, which is not conducive to practical application and industrial production. In addition, the sulfide solid electrolyte is decomposed after reacting with the moisture that may be contacted, resulting in impaired ion conduction ability, which will increase the interface impedance between the positive electrode active particles and the solid electrolyte particles in the positive electrode, affecting the electrochemical performance of the assembled all-solid-state battery and damaging the cycle performance of the battery.

[0152] Exemplarily, a reaction formula between a sulfide solid electrolyte and moisture is as follows:

[0153] The existing structure research on all-solid-state batteries usually adopts the overhang structure design of traditional lithium ion batteries, that is, according to the projection along the stacking direction of each structure layer of the all-solid-state battery, the area of the positive active material layer is smaller than the area of the negative active material layer. When the electrode sheet is subjected to high pressure treatment, the size difference will cause the relatively small positive electrode sheet to shear the negative electrode sheet, which is easy to cause the negative electrode sheet to be broken or to fall off powder.

[0154] In the first aspect of the present application, a positive electrode sheet is provided, which is provided with a positive electrode stabilizer in the positive electrode blank area of the overhang structure.

[0155] In some embodiments, a positive electrode sheet is provided, which includes a positive electrode current collector and an active film layer located on at least one side of the positive electrode current collector, the active film layer including a positive active area and a filling area located on at least a part of the periphery of the positive active area; wherein the positive active area includes positive active particles and a sulfide solid electrolyte; and the filling area includes a positive electrode stabilizer.

[0156] In some embodiments, the positive electrode stabilizer includes at least one of a moisture absorber and a hydrogen sulfide absorber.

[0157] In some embodiments, a positive electrode sheet is provided, which is provided with a positive electrode stabilizer in the positive electrode blank area of the overhang structure, the positive electrode stabilizer including at least one of a moisture absorber and a hydrogen sulfide absorber.

[0158] The positive electrode sheet and solid-state battery (the solid-state battery can be an all-solid-state battery) provided by the present application ingeniously utilizes the traditional overhang structure design, fills the blank area of the positive electrode sheet with a stabilizer that is beneficial to improve the air stability of the positive electrode material, so that the positive electrode sheet has significantly improved air stability, and the structure design can also significantly inhibit the escape of hydrogen sulfide gas.

[0159] In some embodiments, a positive electrode sheet is provided, which includes a positive electrode current collector and an active film layer located on at least one side of the positive electrode current collector, the thickness direction of the active film layer is recorded as the longitudinal direction, and the direction perpendicular to the longitudinal direction is recorded as the transverse direction.

[0160] In the transverse direction, the active film layer includes a positive active area and a filling area located on at least a part of the periphery of the positive active area;

[0161] Wherein, the positive active area includes positive active particles and a positive solid electrolyte, the positive solid electrolyte includes a sulfide solid electrolyte; and the filling area includes a positive electrode stabilizer, the positive electrode stabilizer includes at least one of a moisture absorber and a hydrogen sulfide absorber.

[0162] In the present application, the "thickness direction of the active film layer" is referred to as the longitudinal direction (see Y direction in FIGS. 1-4) unless otherwise specified, and the direction perpendicular to the longitudinal direction is referred to as the lateral direction. Generally, the thickness direction of the positive electrode sheet coincides with the thickness direction of the active film layer, and also coincides with the thickness direction of the positive electrode active region.

[0163] In the present application, the "positive electrode active particle" refers to a particle containing a positive electrode active material, which has the ability to reversibly release and intercalate active ions, unless otherwise specified.

[0164] In the present application, the "positive electrode stabilizer" refers to an agent capable of improving the air stability of the positive electrode material, unless otherwise specified. The positive electrode stabilizer includes at least one of a moisture absorbent and a hydrogen sulfide absorbent, unless otherwise specified. The positive electrode stabilizer can include only the moisture absorbent, only the hydrogen sulfide absorbent, or both the moisture absorbent and the hydrogen sulfide absorbent. As to "absorption" in the moisture absorbent, it can be based on at least one of a physical action and a chemical action, as long as it can function to bind, fix, or eliminate moisture, and is within the meaning of the moisture absorbent in the present application. As to "absorption" in the hydrogen sulfide absorbent, it can be based on at least one of a physical action and a chemical action, as long as it can function to bind, fix, or eliminate hydrogen sulfide gas, and is within the meaning of the hydrogen sulfide absorbent in the present application. When the moisture absorbent and the hydrogen sulfide absorbent coexist, they can be the same substance or different substances, that is, the positive electrode stabilizer is allowed to function as both the moisture absorbent and the hydrogen sulfide absorbent.

[0165] The positive electrode tab provided in the first aspect of the present application is filled with a stabilizer (denoted as a positive electrode stabilizer) beneficial to improving the air stability of the positive electrode material in the corresponding blank area on the positive electrode side, and the positive electrode stabilizer includes at least one of a moisture absorber and a hydrogen sulfide absorber. During the preparation of the positive electrode tab and the assembly of the battery, on the one hand, the filled area can play a role in physically isolating the moisture in the air from the positive electrode active area; on the other hand, the moisture absorber can reduce or avoid the contact probability of the sulfide electrolyte and the moisture, effectively reduce or delay the possibility of the reaction between the sulfide solid electrolyte and the moisture in the air during the preparation process of the positive electrode tab, inhibit the reaction between the sulfide electrolyte and the moisture in the air from the source, reduce or avoid the generation and escape of toxic hydrogen sulfide gas, in addition, the moisture absorber can also improve the material stability in the positive electrode active area, reduce or avoid the adverse effects of the moisture in the air on the moisture-sensitive materials in the positive electrode active area, promote the sulfide solid electrolyte to more stably and effectively play the role of fast ion conduction, inhibit the increase of the interfacial impedance in the positive electrode tab, fully exert the capacity of the positive electrode active material and the ion conduction ability of the sulfide solid electrolyte, and thus be beneficial to improving the electrochemical performance of the assembled solid-state battery (the solid-state battery can be a full solid-state battery), for example, the cycle performance of the battery can be improved; on the other hand, the hydrogen sulfide absorber can absorb the toxic hydrogen sulfide gas generated by the reaction between the sulfide electrolyte and the moisture that may be contacted, and reduce or avoid the escape of the hydrogen sulfide gas.

[0166] In addition, by inhibiting the formation of hydrogen sulfide gas by the sulfide solid electrolyte, the formation of inert by-products in the sulfide solid electrolyte can be reduced, and the impedance increase can be inhibited, thereby the rate performance of the battery can be improved.

[0167] In addition, the positive electrode tab can also be used in cooperation with a negative electrode tab of the same size in the transverse direction, which is beneficial to avoiding the shearing of the negative electrode tab by the positive electrode tab during high-pressure treatment, and thus is beneficial to avoiding the fracture or powdering of the negative electrode tab.

[0168] In the present application, if no other instructions are given, the positive electrode tab sample can be obtained from the solid-state battery (the solid-state battery can be a full solid-state battery) in the following manner: the positive electrode active area sample and the filled area sample of the electrode tab can be obtained by disassembling the battery, and the chemical composition in the positive electrode active area and the filled area can be further analyzed in the following manner: the three-dimensional structure of the sample is reconstructed by using the nanospatial dynamic resolution and layer-by-layer cutting technology of FIB-SEM, the element distribution and proportion are obtained by combining EDS element spectrum analysis, and finally the composition and size of each part of the positive electrode tab are quantitatively analyzed by software to obtain the parameters.

[0169] In the present application, unless otherwise specified, the types and contents of substances in the positive active region of the positive electrode active film layer (including but not limited to positive active particles and positive solid electrolyte), and the types and contents of substances in the filling region (excluding but not limited to positive stabilizer) can be detected by the following method: the structure and composition analysis of the active film layer can be tested and analyzed by focused electron beam (FIB) technology, scanning electron microscope (SEM) and element analysis technology, etc. For example, it can be obtained by combining frozen focused ion beam (FIB) continuous slicing, cross-sectional SEM morphology observation, energy dispersive spectroscopy (EDS) element energy spectrum combination and three-dimensional reconstruction analysis software analysis. For example, the sample is finely sliced (the scale can reach nanoscale thin slices) layer by layer along the transverse direction at different thickness positions by using frozen focused ion beam (FIB), and different layer samples at different thickness positions are separated. The morphology, structure and element distribution of each layer cross section can be analyzed under FIB continuous slicing by scanning electron microscope (SEM) test, and the three-dimensional structure of the sample can be reconstructed by combining three-dimensional structure reconstruction software, and the mass and / or volume of different regions of the sample to be tested can be estimated. As a non-limiting example, the test analysis of the above parameters can use FEI Scios 2HiVac equipment.

[0170] In addition, for the types and contents of chemical components in the positive active region and the filling region, including but not limited to the positive stabilizer and the first binder, the insulating material, the positive active particle, the positive active body, the coating layer in the positive active particle, etc. described below, other suitable methods in other chemical component detection means, such as X-ray diffraction (XRD), inductively coupled plasma spectrometer (ICP), gas chromatography mass spectrometry (GC-MS), Fourier transform infrared spectrometer (FT-IR), Raman spectroscopy (Raman), etc. can be used for test analysis. Non-limitingly, the material components of the coating layer of different positive active particles can be detected and analyzed by XRD method, ICP method, etc. Element analysis method, the binder (first binder or second binder) can be analyzed by FT-IR method and Raman method, in addition, the area size of the filling region can be analyzed by SEM, FIB, etc.

[0171] In the present application, the weight percentage of the positive stabilizer in the filling region can be denoted as R0 M , the mass ratio of the moisture absorbent and the hydrogen sulfide absorbent in the filling region can be denoted as R H2O / H2S , the weight percentage of the moisture absorbent in the filling region can be denoted as R1 H2O , the weight percentage of the hydrogen sulfide absorbent in the filling region can be denoted as R1 H2S . For the positive stabilizer which can simultaneously play the dual role of moisture absorbent and hydrogen sulfide absorbent, R H2O / H2S , R1 H2O and R1 H2SWhen the same substance can be repeatedly calculated as the moisture absorbent and the hydrogen sulfide absorbent, for example, when the positive electrode stabilizer is only one substance and simultaneously plays the dual role of the moisture absorbent and the hydrogen sulfide absorbent, R0 H2O / H2S is 1, and further when R0 M is 95wt%, R1 H2O and R1 H2S are both 95wt%, see Examples 16-19, etc. When the positive electrode stabilizer is more than one substance and simultaneously plays the dual role of the moisture absorbent and the hydrogen sulfide absorbent, similarly, R0 H2O / H2S is 1, and R0 M , R1 H2O and R1 H2S are equal in value, see Examples 27-28, etc.

[0172] In some embodiments, the weight ratio (R0 M ) of the positive electrode stabilizer in the filling area satisfies 0wt% < R0 M ≤ 99.5wt%, which can be optionally 30wt% ~ 99.5wt%, further optionally 45wt% ~ 98wt%, and more further optionally 49wt% ~ 98wt%. The weight ratio of the positive electrode stabilizer in the filling area can also be any one of the following weight ratios: 5wt%, 10wt%, 15wt%, 20wt%, 25wt%, 30wt%, 35wt%, 40wt%, 45wt%, 49wt%, 50wt%, 55wt%, 60wt%, 65wt%, 70wt%, 75wt%, 80wt%, 85wt%, 90wt%, 95wt%, 98wt%, 99wt%, 99.5wt%, etc., and the weight ratio of the positive electrode stabilizer in the filling area can be selected from an interval formed by any two of the aforementioned weight ratios.

[0173] In some embodiments, the mass ratio (R H2O / H2S ) of the moisture absorbent and the hydrogen sulfide absorbent in the filling area is 0 ~ 1, which can be optionally 1:9 to 9:1 (also equivalent to 1 / 9 to 9), and can also be any one of the following mass ratios or selected from an interval formed by any two of the following mass ratios: 0, 0.05, 0.1, 1 / 9, 0.15, 0.2, 0.25, 0.3, 0.33, 1 / 3, 0.4, 0.5, 0.6, 0.75, 0.8, 0.9, 1, 1.05, 1.1, 1.2, 1.25, 1.3, 1.35, 1.4, 1.45, 1.5, 1.6, 1.75, 1.8, 2, 2.25, 2.4, 2.5, 3, 3.5, 3.6, 4, 4.5, 5, 5.5, 6, 6.5, 7, 7.5, 8, 8.5, 9, etc.

[0174] In the present application, when referring to a "numerical ratio", the ratio, percentage, numerical value, etc. can be used to describe it, unless otherwise specified. For example, "mass ratio of 9:1" and "mass ratio of 9" have the same meaning and can be used interchangeably. For another example, "volume ratio of 0.1", "volume ratio of 1:10" and "volume ratio of 10%" have the same meaning and can be used interchangeably.

[0175] In some embodiments, the weight percentage (R1 H2O ) of the moisture absorbent in the filling area is 0wt% to 99.5wt%, optionally 10wt% to 90wt%, further optionally 30wt% to 70wt%, and more further optionally 40wt% to 60wt%. The weight percentage of the moisture absorbent in the filling area can also be any one of the following weight percentages or selected from the interval consisting of any two of the following weight percentages: 0wt%, 1wt%, 2wt%, 4wt%, 5wt%, 6wt%, 8wt%, 10wt%, 15wt%, 20wt%, 25wt%, 30wt%, 35wt%, 40wt%, 45wt%, 50wt%, 55wt%, 60wt%, 65wt%, 70wt%, 75wt%, 80wt%, 85wt%, 90wt%, 95wt%, 98wt%, 99wt%, 99.5wt%, etc.

[0176] In some embodiments, the weight percentage (R1 H2S ) of the hydrogen sulfide absorbent in the filling area is 0wt% to 99.5wt%, optionally 10wt% to 90wt%, further optionally 30wt% to 70wt%, and more further optionally 40wt% to 60wt%. The weight percentage of the hydrogen sulfide absorbent in the filling area can also be any one of the following weight percentages or selected from the interval consisting of any two of the following weight percentages: 0wt%, 1wt%, 2wt%, 4wt%, 5wt%, 6wt%, 8wt%, 10wt%, 15wt%, 20wt%, 25wt%, 30wt%, 35wt%, 40wt%, 45wt%, 50wt%, 55wt%, 60wt%, 65wt%, 70wt%, 75wt%, 80wt%, 85wt%, 90wt%, 95wt%, 98wt%, 99wt%, 99.5wt%, etc.

[0177] By adjusting the weight percentage (R0 M ) of the positive electrode stabilizer in the filling area, the mass ratio (R H2O / H2S ) of the moisture absorbent and the hydrogen sulfide absorbent in the filling area, the weight percentage (R1 H2O ) of the moisture absorbent in the filling area, and the weight percentage (R1 H2S) can adjust the content of the positive electrode stabilizer in the positive electrode sheet, so as to better play the role of reducing or avoiding the contact probability between the sulfide electrolyte and moisture and thus reducing or avoiding the escape of hydrogen sulfide gas.

[0178] It should be noted that some positive electrode stabilizers can act as moisture absorbers and hydrogen sulfide absorbers at the same time, so R1 H2O With R1 H2S The sum of the M .

[0179] By controlling R1 H2O Within the aforementioned range, the content of the moisture absorber in the positive electrode plate can be adjusted, which is not only conducive to better reducing or avoiding the probability of contact between the sulfide electrolyte and moisture, reducing or avoiding the generation and escape of hydrogen sulfide gas, but also conducive to better enhancing the material stability of the positive electrode active area, promoting the sulfide solid electrolyte to more effectively and stably perform fast ion conduction, and is more conducive to improving the electrochemical properties of the solid-state battery (the solid-state battery can be an all-solid-state battery) assembled secondary using the positive electrode plate, such as achieving better cycle performance.

[0180] By controlling R1 H2S Within the aforementioned range, it is beneficial to better reduce or avoid the escape of hydrogen sulfide gas.

[0181] In some embodiments, the positive electrode stabilizer includes a moisture absorbent. Without limitation, the moisture absorbent may include one or more of a physical moisture absorbent and a chemical moisture absorbent. In some embodiments, the moisture absorbent may include, but is not limited to, a physical moisture absorbent. Non-limiting examples of physical moisture absorbents may include one or more moisture absorbents of silica gel, molecular sieve moisture absorbents, metal organic frameworks, and porous carbon, and the moisture absorbent of porous carbon includes activated carbon. In some embodiments, the moisture absorbent may include, but is not limited to, a chemical moisture absorbent. Non-limiting examples of chemical moisture absorbents may include, but are not limited to, one or more of CaCl2, CaH2, anhydrous CuSO4, lithium chloride (LiCl), FeCl3, FeO(OH), KMnO4, Na2CO3, Fe2O3, Fe(OH)3, ZnO, CuO, NiO, Al2O, etc.

[0182] In some embodiments, the positive electrode stabilizer includes a hydrogen sulfide absorber. Without limitation, the hydrogen sulfide absorber can include one or more of a hydrogen sulfide physical absorber and a hydrogen sulfide chemical absorber. In some embodiments, the hydrogen sulfide absorber includes, but is not limited to, a hydrogen sulfide physical absorber. Non-limiting examples of the hydrogen sulfide physical absorber can include one or more of activated carbon-based, molecular sieve-based, and metal organic framework-based hydrogen sulfide absorbers. In some embodiments, the hydrogen sulfide absorber can include, but is not limited to, a hydrogen sulfide chemical absorber. Non-limiting examples of the hydrogen sulfide chemical absorber can include one or more of Fe2O3, ZnO, Bi2O3, CuO, MnO, and the like.

[0183] The kind of at least one of the moisture absorber and the hydrogen sulfide absorber can be flexibly selected to better achieve the effect of reducing or avoiding the escape of hydrogen sulfide gas. Among them, by flexibly selecting the moisture absorber, the contact probability of the sulfide electrolyte with moisture can be better reduced or avoided, thereby reducing or avoiding the effect of the escape of hydrogen sulfide gas, and promoting the sulfide solid electrolyte to function more stably and effectively, and better improving the cycle performance of the battery.

[0184] The action mechanism of the above-mentioned various moisture absorbers can be understood by those skilled in the art from the relevant technical field according to the description in the present application, so that different kinds of moisture absorbers can be used in combination according to the needs, and moisture absorbers with different action mechanisms can also be used in combination.

[0185] The action mechanism of the above-mentioned various hydrogen sulfide absorbers can be understood by those skilled in the art from the relevant technical field according to the description in the present application, so that different kinds of hydrogen sulfide absorbers can be used in combination according to the needs, and hydrogen sulfide absorbers with different action mechanisms can also be used in combination. Taking the hydrogen sulfide chemical absorber ZnO as an example, the hydrogen sulfide gas can be eliminated by using the following chemical reaction: ZnO + H2S → ZnS + H2O; however, this reaction will produce water, and therefore, the moisture absorber can be used in combination.

[0186] In some embodiments, the positive electrode stabilizer comprises a dual-absorbing agent, which refers to a substance that simultaneously functions as a moisture-absorbing agent and a hydrogen sulfide-absorbing agent. The dual-absorbing agent can comprise one or more of a dual-physical-absorbing agent and a dual-chemical-absorbing agent; the dual-physical-absorbing agent refers to a substance that simultaneously absorbs moisture and hydrogen sulfide based on physical action; the dual-chemical-absorbing agent refers to a substance that simultaneously absorbs moisture and hydrogen sulfide based on chemical action. Without limitation, the dual-physical-absorbing agent can comprise one or more of an activated carbon type, a molecular sieve type, and a metal-organic framework type. Without limitation, the dual-chemical-absorbing agent can comprise one or more of ZnO, CuO, Fe2O3, CaO, and the like. In some embodiments, the dual-chemical-absorbing agent comprises at least one of ZnO and CuO. In some embodiments, the dual-chemical-absorbing agent comprises ZnO. Without limitation, the dual-absorbing agent can comprise one or more of ZnO, CuO, an activated carbon type, a molecular sieve type, and a metal-organic framework type.

[0187] In some embodiments, the positive electrode stabilizer comprises one or more of ZnO, CuO, Fe2O3, CaO, and the like, optionally, the positive electrode stabilizer comprises at least one of ZnO and CuO, further optionally, the positive electrode stabilizer comprises ZnO.

[0188] When the positive electrode stabilizer comprises a dual-absorbing agent, the dual-absorbing agent can simultaneously function as a moisture-absorbing agent and a hydrogen sulfide-absorbing agent, which is conducive to more effectively reducing or avoiding the escape of hydrogen sulfide and improving the material and performance stability of the positive electrode active area, and better improving the cycle performance of the battery.

[0189] In some embodiments, the positive electrode stabilizer comprises a dual-absorbing agent, which comprises a dual-physical-absorbing agent and a dual-chemical-absorbing agent.

[0190] When a physical-absorbing agent is used in combination with a dual-chemical-absorbing agent, the effect of simultaneously absorbing moisture and hydrogen sulfide is better.

[0191] In some embodiments, the positive electrode stabilizer comprises a dual-chemical-absorbing agent and a dual-physical-absorbing agent, and the dual-physical-absorbing agent comprises one or more of an activated carbon type and a molecular sieve type.

[0192] When the positive electrode stabilizer only contains a dual-absorbing agent, it means that the types and weights of the moisture-absorbing agent and the hydrogen sulfide-absorbing agent are completely the same, and R H2O / H2S is equal to 1, R1 H2O , R1 H2S , and R0 M are equal in value.

[0193] When an activated carbon type and a molecular sieve type are used as a physical-absorbing agent in combination with a dual-chemical-absorbing agent, the effect of simultaneously absorbing moisture and hydrogen sulfide is better.

[0194] In some embodiments, the filler region comprises a binder (denoted as a first binder), and in this case, the filler region comprises at least the cathode stabilizer and the first binder. Without limitation, the first binder can comprise one or more of a rubber-based binder, a carboxymethyl cellulose, a polyolefin-based binder, a polyurethane-based binder, a polyacrylate-based binder, a polyacrylic resin, a polyvinylidene fluoride, a polytetrafluoroethylene, a vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, a vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene terpolymer, a tetrafluoroethylene-hexafluoropropylene copolymer, and the like.

[0195] Without limitation, the rubber-based binder can comprise at least one of a fluorinated rubber-based or a rubber-based binder that does not contain fluorine elements. In some embodiments, the rubber-based binder comprises a fluorinated rubber-based, which can further be a fluorinated rubber-based binder. In other embodiments, the rubber-based binder comprises a rubber-based binder that does not contain fluorine elements. Without limitation, the polyacrylate-based binder can comprise at least one of a fluorine-containing acrylate resin or a polyacrylate-based binder that does not contain fluorine elements. In some embodiments, the polyacrylate-based binder comprises a fluorine-containing acrylate resin. In some embodiments, the polyacrylate-based binder comprises a polyacrylate-based binder that does not contain fluorine elements. Non-limiting examples of the first binder can comprise one or more of a styrene butadiene rubber, a nitrile butadiene rubber, a hydrogenated nitrile butadiene rubber, a polyacrylic resin, a polyurethane-based binder, and the like.

[0196] In the present application, unless otherwise specified, the "binder" in the filler region, denoted as a first binder, refers to a binder that can at least agglomerate the components in the filler region.

[0197] In some embodiments, the first binder has a weight percentage in the filler region of 0.5wt% to 5wt%, which can optionally be 1wt% to 4wt%, which can further be 2wt% to 4wt%, and which can also be any one of the following percentages or a range selected from any two of the following percentages: 0.5wt%, 0.6wt%, 0.8wt%, 1wt%, 1.2wt%, 1.5wt%, 1.6wt%, 1.8wt%, 2wt%, 2.5wt%, 3wt%, 3.5wt%, 4wt%, 4.5wt%, 5wt%, and the like.

[0198] In some embodiments, the positive electrode active area includes a binder (which may be referred to as a second binder). The types of the first binder and the second binder may be the same or different. The type of the second binder may refer to the description of the first binder. For example, the second binder may include, but is not limited to, one or more of a rubber binder, carboxymethyl cellulose, a polyolefin binder, a polyurethane binder, a polyacrylate binder, a polyacrylic resin, polyvinylidene fluoride, polytetrafluoroethylene, a vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, a vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene terpolymer, a tetrafluoroethylene-hexafluoropropylene copolymer, and the like. Non-limiting examples of the second binder may include one or more of styrene-butadiene rubber, nitrile rubber, hydrogenated nitrile rubber, polyacrylic resin, polyurethane binder, and the like. As one of the non-limiting examples, the second binder may include one or more of a rubber binder, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), a vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, a vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene terpolymer, a tetrafluoroethylene-hexafluoropropylene copolymer, and a fluorine-containing acrylate resin. In a non-limiting manner, the weight percentage of the second binder in the positive electrode active area can be 0-10wt%, further can be 0-8wt%, further can be 0.1wt%-5wt%, further can be 1wt%-5wt%, based on the total weight of the positive electrode active area. The weight percentage of the second binder in the positive electrode active area can also be 0.2wt%-5wt%, 0.5wt%-5wt%, 0.1wt%-3wt%, 0.3wt%-3wt%, 1wt%-3wt%, etc.

[0199] In the present application, the first binder located in the filling region and the second binder located in the positive electrode active region, when both are present, may be the same or different.

[0200] In some embodiments, the filling region includes a first binder, the positive electrode active region includes a second binder, and the first binder and the second binder are of the same type.

[0201] When the filling area and the positive electrode active area use the same type of binder, it is beneficial to improve the adhesion strength of the filling area on the positive electrode current collector.

[0202] The filling area may or may not include insulating material. The weight proportion of the insulating material in the filling area may be 0 wt % to 69 wt %, optionally 0 wt % to 66 wt %, further optionally 0 wt % to 60 wt %, further optionally 0 wt % to 50 wt %, but is not limited thereto.

[0203] In some embodiments, the filling region comprises an insulating material, and in this case, the filling region comprises at least the positive electrode stabilizer and the insulating material. In some of these embodiments, the filling region comprises the positive electrode stabilizer, the first binder, and the insulating material.

[0204] Without limitation, the insulating material can comprise one or more of inorganic oxide insulating material, boehmite, non-woven fabric fiber, and fibrous resin. Without limitation, the inorganic oxide insulating material can comprise one or more of Al2O3, MgO, SiO2, BaTiO3, BaCO3, Fe3O4, TiO2, Y2O3, Mn2O3, and Mn2O7.

[0205] By disposing the insulating material in the filling region, on the one hand, the risk of internal short circuit can be better avoided, and on the other hand, the distribution concentration of the positive electrode stabilizer can be adjusted, which can assist in adjusting the content of the positive electrode stabilizer in the filling region. The type of insulating material can be flexibly selected accordingly.

[0206] In some embodiments, the weight percentage of the insulating material in the filling region is 0wt% to 50wt%, further optionally 1wt% to 50wt%, more further optionally 1wt% to 10wt%, and more further optionally 3wt% to 7wt%.

[0207] Without limitation, the weight percentage of the insulating material in the filling region can be any one of the following suitable weight percentages or selected from a suitable interval consisting of any two of the following weight percentages: 0wt%, 1wt%, 2wt%, 4wt%, 5wt%, 6wt%, 8wt%, 10wt%, 15wt%, 20wt%, 25wt%, 30wt%, 35wt%, 40wt%, 45wt%, 50wt%, 55wt%, 60wt%, 66wt%, 69wt%, and the like.

[0208] In some embodiments, the mass ratio of the insulating material to the positive electrode stabilizer is less than or equal to 2, optionally 0 to 2, further optionally 0.5 to 2, more further optionally 0.5 to 1, and also 1 to 1.5. Without limitation, the mass ratio of the insulating material to the positive electrode stabilizer can also be any one of the following ratios or selected from an interval consisting of any one of the following ratios: 0, 0.05, 0.1, 1 / 9, 0.15, 0.2, 0.25, 0.3, 0.33, 1 / 3, 0.4, 0.5, 0.6, 0.75, 0.8, 0.9, 1, 1.05, 1.1, 1.2, 1.25, 1.3, 1.35, 1.4, 1.45, 1.5, 1.6, 1.75, 1.8, 2, and the like.

[0209] By adjusting one or both of the parameters of "insulating material weight percentage in the filling region" and "insulating material to positive electrode stabilizer mass ratio in the filling region" within the above ranges, it is beneficial to better avoid the risk of internal short circuit while flexibly setting a suitable content of positive electrode stabilizer in the filling region.

[0210] In some embodiments, the positive electrode active particle comprises at least a positive electrode active body, which can or can not comprise a coating layer on at least a part of its surface. As defined previously, the positive electrode active body comprises a positive electrode active substance.

[0211] Non-limitingly, the weight percentage of the positive electrode active substance in the positive electrode active body can be 95wt%~100wt%, and can also be any one of the following percentages or a range consisting of any two of the following percentages: 95wt%, 96wt%, 97wt%, 98wt%, 99wt%, 100wt%, etc.

[0212] When the positive electrode active particle comprises a coating layer, the coating layer can comprise a lithium oxide compound, but is not limited thereto. The weight percentage of the coating layer in the positive electrode active particle can be 0wt%~5wt%, can optionally be 0.1wt%~5wt%, can further optionally be 0.5wt%~5wt%, can also be 0.1wt%~2wt%, can also be 0.5wt%~2wt%, and can also be any one of the following weight percentages or a range consisting of any two of the following weight percentages: 0wt%, 0.1wt%, 0.2wt%, 0.4wt%, 0.5wt%, 0.6wt%, 0.8wt%, 1wt%, 1.5wt%, 2wt%, 2.5wt%, 3wt%, 4wt%, 4.5wt%, 5wt%, etc.

[0213] In the present application, unless otherwise specified, the "positive electrode active particle" can or can not comprise a coating layer. When comprising a coating layer, the coating layer is located on at least a part of the surface of the positive electrode active body. Non-limitingly, the weight percentage of the coating layer in the positive electrode active particle can be 0.1wt%~5wt%, can optionally be 0.5wt%~5wt%, and can also be 0.1wt%~2wt%, and can also refer to the previous definition. Non-limitingly, the thickness of the coating layer can be 0.1nm~50nm, can optionally be 0.5nm~10nm. It can also be any one of the following thicknesses or a range consisting of any two of the following thicknesses: 0.1nm, 0.2nm, 0.4nm, 0.5nm, 0.6nm, 0.8nm, 1nm, 2nm, 3nm, 4nm, 5nm, 6nm, 7nm, 8nm, 9nm, 10nm, 12nm, 15nm, 20nm, 25nm, 30nm, 35nm, 40nm, 45nm, 50nm, etc.

[0214] Non-limitingly, the weight percentage of the positive electrode active material in the positive electrode active particle can be 95wt% to 100wt%, and can also be any one of the following percentages or a range consisting of any two of the following percentages: 95wt%, 96wt%, 97wt%, 98wt%, 99wt%, 100wt%, etc.

[0215] The structure (e.g., whether there is a coating layer) and chemical composition of the positive electrode active particle can be detected by the aforementioned methods, such as X-ray diffraction (XRD), inductively coupled plasma spectrometer (ICP), etc., but are not limited thereto. The methods that can be used to detect the structure and chemical composition of the positive electrode active particle can be used in the present application.

[0216] In the present application, the D v 50 can be 1μm to 15μm, optionally 5μm to 15μm, further optionally 5μm to 12μm, and can also be any one of the following particle sizes or a range consisting of any two of the following particle sizes: 1μm, 2μm, 3μm, 4μm, 5μm, 6μm, 8μm, 10μm, 12μm, 15μm, etc.

[0217] In some embodiments, the D v 50 of the constituent particles in the coating layer is less than or equal to 1μm.

[0218] In some embodiments, the D v 50 of the lithium oxide compound in the coating layer is less than or equal to 1μm.

[0219] In the context of the present application, the particle size of a material can be characterized by the volume cumulative distribution particle size D v N (wherein N represents any numerical value selected from 0 to 100), which refers to the particle size corresponding to the cumulative volume distribution percentage of the material reaching N%, and the volume percentage of the material with a particle size less than or equal to D v N is N%. The D v N can be obtained from the volume cumulative distribution curve of the material particle size, and the volume cumulative distribution curve starts from zero on the small particle size side, unless otherwise specified. Take D v 50 as an example. In the present application, unless otherwise specified, D v 50 refers to the particle size corresponding to the cumulative volume distribution percentage of the material reaching 50%, which indicates that the particle size of the particles accounting for 50% of the volume of the material is less than or equal to D v 50, and the particle size of the particles accounting for 50% of the volume of the material is greater than D v 50. Those skilled in the art can understand that D v50, and can be measured using instruments and methods known in the art. For example, GB / T 19077-2016 Particle Size Distribution Laser Diffraction Method can be referred to, and a laser particle size analyzer can be conveniently used for measurement, such as a Mastersizer 2000E laser particle size analyzer from Malvern Instruments Ltd., UK, or an LS-909 laser particle size analyzer from Beckman Coulter.

[0220] Without limitation, the positive electrode active material in the positive electrode active particle can use a positive electrode active material for a battery known in the art. As non-limiting examples, the positive electrode active material can include one or more of: lithium-containing phosphates, lithium transition metal oxides, and modified compounds of each thereof, further, the positive electrode active material can include one or more of: lithium-containing phosphates of olivine structure, lithium transition metal oxides, and modified compounds of each thereof. However, the present application is not limited to these materials, and other conventional materials that can be used as positive electrode active materials for batteries can also be used. These positive electrode active materials can be used alone only, or two or more can be used in combination. Among them, examples of the lithium transition metal oxide can include, but are not limited to, one or more of: lithium cobalt oxide, lithium nickel oxide, lithium manganese oxide, lithium nickel cobalt oxide, lithium manganese cobalt oxide, lithium nickel manganese oxide, lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminum oxide, and modified compounds thereof. Non-limiting examples of the lithium-containing phosphates of olivine structure can include, but are not limited to, one or more of: lithium iron phosphate, a composite of lithium iron phosphate and carbon, lithium manganese phosphate, a composite of lithium manganese phosphate and carbon, lithium manganese iron phosphate, a composite of lithium manganese iron phosphate and carbon. Non-limiting examples of the lithium cobalt oxide can include LiCoO2; non-limiting examples of the lithium nickel oxide can include LiNiO2; non-limiting examples of the lithium manganese oxide can include LiMnO2, LiMn2O4, and the like; non-limiting examples of the lithium nickel cobalt manganese oxide can include LiNi 1 / 3 Co 1 / 3 Mn 1 / 3 O2(also referred to as NCM 333 )、LiNi 0.5 Co 0.2 Mn 0.3 O2(also referred to as NCM 523 )、LiNi 0.5 Co 0.25 Mn 0.25 O2(also referred to as NCM 211 )、LiNi 0.6 Co 0.2 Mn 0.2 O2(also referred to as NCM 622 )、LiNi 0.8 Co 0.1 Mn 0.1O2(also can be referred to as NCM 811 ) and the like. Non-limiting examples of lithium nickel cobalt aluminum oxides can include LiNi 0.80 Co 0.15 Al 0.05 O2. Examples of lithium iron phosphates include LiFePO4(also can be referred to as LFP). Examples of lithium manganese phosphates include LiMnPO4.

[0221] With reference to solid-state batteries including active ions such as lithium ions, and with reference to all-solid-state batteries including active ions such as lithium ions, it can be understood that the all-solid-state batteries will be accompanied by lithium (Li) deintercalation and consumption during charging and discharging, and the content of Li in the positive electrode layer is different when the battery is discharged to different states. In the exemplary description of the positive electrode active material in this application, unless otherwise stated, the content of Li can be the initial state of the material or the non-initial state after charging and discharging cycles. When the positive electrode active material is applied to the positive electrode layer in the all-solid-state battery system, the content of Li in the positive electrode active material contained in the positive electrode layer will usually change after charging and discharging cycles. The content of Li can be measured by atomic molar content, but is not limited thereto. With reference to the content of Li in the initial state of the material, the initial state of the material refers to the state before being placed in the positive electrode layer. It can be understood that new materials or new substances obtained by appropriately modifying the listed positive electrode active materials are also within the scope of positive electrode active materials, and the aforementioned appropriate modification refers to acceptable modification methods for the positive electrode active material, and non-limiting examples include coating modification. In the exemplary description of the positive electrode active material in this application, the content of oxygen (O) is usually the theoretical state value, and the release of oxygen from the crystal lattice will cause the atomic molar content of oxygen to change, and the actual content of O will fluctuate. The content of O can be measured by atomic molar content, but is not limited thereto.

[0222] In some embodiments, the positive electrode active particles include a positive electrode active body and a coating layer located on at least a portion of the surface of the positive electrode active body, the positive electrode active body includes one or more of a lithium transition metal oxide and a lithium-containing phosphate, and the coating layer includes a lithium oxygen compound.

[0223] The coating layer of the positive electrode active particles can or can not include a lithium oxygen compound.

[0224] Non-limitingly, the weight percentage of the lithium oxide compound in the positive electrode active particle can be 0wt%~5wt%. When the positive electrode active particle comprises a coating layer, and the coating layer comprises the lithium oxide compound, the weight percentage of the lithium oxide compound in the positive electrode active particle can be selected from 0.1wt%~5wt%, further selected from 0.5wt%~5wt%, also can be 0.1wt%~2wt%, also can be 0.5wt%~2wt%. The weight percentage of the lithium oxide compound in the positive electrode active particle can also be any one of the following weight percentages or an interval formed by any two of the following weight percentages: 0wt%, 0.1wt%, 0.2wt%, 0.4wt%, 0.5wt%, 0.6wt%, 0.8wt%, 1wt%, 1.5wt%, 2wt%, 2.5wt%, 3wt%, 4wt%, 4.5wt%, 5wt%, etc.

[0225] In some embodiments, the positive electrode active particle comprises a positive electrode active body and a coating layer located on at least a part of the surface of the positive electrode active body, and the coating layer comprises a lithium oxide compound. The weight percentage of the lithium oxide compound in the coating layer can be 90wt%~100wt%, and can also be any one of the following percentages or an interval formed by any two of the following percentages: 90wt%, 92wt%, 94wt%, 95wt%, 96wt%, 97wt%, 98wt%, 99wt%, 100wt%, etc., but is not limited thereto.

[0226] Non-limitingly, the lithium oxide compound in the coating layer can comprise one or more elements selected from B, Nb, Zr, Si, P, Mn, Zn, Al, Fe, Na, etc. In some embodiments, the lithium oxide compound in the coating layer can comprise one or more of Li3BO3, LiNbO3, Li2ZrO3, Li2SiO3, LiPO3, Li2MnO4, etc.

[0227] By providing the coating layer on the surface of the positive electrode active body and introducing the compound component (such as the lithium oxide compound) which is not sensitive to water and has certain ion conductivity into the coating layer, it is beneficial to maintain certain ion conductivity while physically isolating the positive electrode active body from the sulfide solid electrolyte, to inhibit the side reaction caused by space charge when the positive electrode active body and the sulfide solid electrolyte are in contact, to inhibit the decomposition of the sulfide solid electrolyte, to reduce the interface impedance, to benefit the full capacity of the positive electrode active body, and to further improve the cycle performance of the battery.

[0228] In the present application, the following methods can be used to prepare the positive electrode active particles provided with a coating layer: (1) preparing a positive electrode active body according to the element composition and atomic stoichiometric ratio, which can be prepared by sol-gel, atomic layer deposition (ALD), molecular layer deposition (MLD), melt coating, dry coating, hydrothermal method, coprecipitation method, spray drying method, etc.; (2) according to the material composition of the coating layer, a physical coating or chemical coating method is used to form a coating layer with a certain weight percentage on the surface of the positive electrode active body. Those skilled in the art can select a suitable method to prepare the positive electrode active body and realize surface coating according to the structure and element composition of the positive electrode active particles in the present application. By adjusting the input amount of the coating layer material in the coating operation, the weight percentage of the coating layer in the positive electrode active particles can be controlled.

[0229] Non-limitingly, the weight percentage of lithium oxide compounds in the coating layer in the positive electrode active particles is 0.1wt%-5wt%, which can be optionally 0.5wt%-5wt%, and can also be 0.1wt%-2wt%, and can also be 0.5wt%-2wt%, and can also refer to the definition in the foregoing. Adjusting the "weight percentage of lithium oxide compounds in the positive electrode active particles" within the foregoing range is beneficial to achieving higher energy density while fully exerting the improvement of the coating layer.

[0230] Non-limitingly, when the positive electrode active particles or the positive electrode active body contain lithium transition metal oxides, the lithium transition metal oxides can include lithium transition metal oxides commonly known in the art that can be used as positive electrode active materials in solid-state batteries (which can be full solid-state batteries), but are not limited thereto. Examples of lithium transition metal oxides can include, but are not limited to, one or more of lithium cobalt oxides, lithium nickel oxides, lithium manganese oxides, lithium nickel cobalt oxides, lithium manganese cobalt oxides, lithium nickel manganese oxides, lithium nickel cobalt manganese oxides, lithium nickel cobalt aluminum oxides, and modified compounds thereof, etc. Examples of various lithium transition metal oxides can be referred to in the foregoing. For example, non-limiting examples of lithium nickel cobalt manganese oxides can include NCM 333 , NCM 523 , NCM 211 , NCM 622 , NCM 811 , etc. Non-limiting examples of lithium nickel cobalt aluminum oxides can include LiNi 0.80 Co 0.15 Al 0.05 O2.

[0231] In some embodiments, the positive electrode active body includes lithium-containing phosphates. The types of lithium-containing phosphates can be referred to in the foregoing definition. At this time, it is beneficial to reduce the chemical potential difference between the positive electrode active particles and the electrolyte material in the positive electrode active region, reduce the interface side reaction, reduce the interface impedance, improve the material stability, and improve the cycle performance.

[0232] In some embodiments, the sulfide solid electrolyte includes at least one of a binary sulfide solid state system and a ternary sulfide solid state system. Without limitation, the binary sulfide solid state system can include one or more of Li2S-P2S5, Li2S-SiS2, Li2S-GeS2, and Li2S-B2S3. Without limitation, the ternary sulfide solid state system can include one or more of argyrodite-type sulfide electrolyte, Li2S-MeS2-P2S5 ternary sulfide electrolyte, lithium-germanium-phosphorus-sulfur type sulfide electrolyte, Li2S-P2S5-MS ternary sulfide electrolyte, Li2S-P2S5-MCl ternary sulfide electrolyte, and thio-LISICON-type sulfide electrolyte; wherein Me can include one or more elements of Si, Ge, Sn, and Al; and M can include one or more elements of Ge, Al, Sn, Pb, Sb, Si, and As. In some embodiments, Me is selected from one or more elements of Si, Ge, Sn, and Al. In some embodiments, M is selected from one or more elements of Ge, Al, Sn, Pb, Sb, Si, and As.

[0233] With the filling area provided, the selection of the sulfide solid electrolyte is not necessarily limited by the strength of the hygroscopicity, and the type of the sulfide solid electrolyte can be more flexibly selected according to the needs of one or more aspects of the ion conduction ability, the electrochemical window range, the electrical conductivity, the particle size, and the like.

[0234] In some embodiments, the positive electrode stabilizer includes a moisture absorbing agent, and the positive electrode solid electrolyte further includes a halide solid electrolyte. Without limitation, the halide solid electrolyte can include lithium elements, halogens, and X elements, wherein the X elements can include one or more of Y, In, Zr, Sc, Ho, Mn, Cd, Pd, and the like, and can also be selected from one or more of the foregoing elements. Without limitation, the halogens can include one or more of Cl, Br, and I, and can also be selected from one or more of the foregoing elements. In some embodiments, the halogens are selected from one or both of Cl and Br, and can further be Cl or Br.

[0235] In some embodiments, the halide solid electrolyte can include Li3X 1 Cl6, LiX 1 I4, LiX 1 I3, Li3X 1 Br6, and the like, and optionally, the X 1 in the halide solid electrolyte can include one or more of Y, In, Zr, Sc, Ho, Mn, Cd, Pd, and the like, and can also be selected from one or more of the foregoing elements.

[0236] When the positive electrode solid electrolyte further includes a halide solid electrolyte which is prone to physical water absorption, the positive electrode active material layer can be subjected to a more serious water absorption problem, and the water absorption caused by the halide solid electrolyte can further exacerbate the instability of the hydrogen sulfide solid electrolyte. At this time, by adopting the positive electrode tab structure design of the first aspect of the present application and arranging the moisture absorber in the positive electrode stabilizer, more significant improvement in the air stability of the positive electrode tab can be achieved. The moisture absorber can significantly reduce or avoid the absorption of moisture by the positive electrode active area, reduce or avoid the escape of hydrogen sulfide gas, and more significantly improve the material stability and performance stability of the positive electrode active area (including the sulfide solid electrolyte), which is more conducive to improving the electrochemical performance of the assembled solid-state battery (the solid-state battery can be a full solid-state battery), for example, the cycle performance of the battery can be better improved.

[0237] In some embodiments, the positive electrode active area has a first side and a second side facing away from each other, and the first side and the second side respectively intersect with the transverse direction;

[0238] A filling area is arranged outside the opposite regions of the first side and the second side, respectively;

[0239] One example can be seen in FIG. 5. In FIG. 5, for example, in the width direction X1 of the positive electrode active area in the transverse direction, the positive electrode active area is provided with a filling area on both sides; in the length direction X2 of the positive electrode active area in the transverse direction, the positive electrode active area is not provided with a filling area on both sides. Taking a winding structure as an example, the X2 direction can correspond to the winding direction when assembling the solid-state battery (the solid-state battery can be a full solid-state battery), at this time, the length direction of a single layer of positive electrode active area can not be in contact with air on both sides.

[0240] By arranging the filling area on both sides of the positive electrode active area in the transverse direction, it is conducive to better isolating the positive electrode active area from the contact with moisture in the air and reducing or avoiding the escape of hydrogen sulfide gas when assembling the solid-state battery (the solid-state battery can be a full solid-state battery).

[0241] In some embodiments, the positive electrode tab includes a positive electrode current collector 110 and an active film layer located on one side of the positive electrode current collector 110, the active film layer includes a positive electrode active area 120, the positive electrode active area 120 has a first side and a second side facing away from each other, and the first side and the second side respectively intersect with the transverse direction, and a filling area 130 is arranged outside the opposite regions of the first side and the second side, respectively; wherein the positive electrode active area 120 includes positive electrode active particles 121 and a positive electrode solid electrolyte 122, and the filling area 130 includes a positive electrode stabilizer 131. One example can be seen in FIG. 1. In FIG. 1, the first side and the second side are exemplarily perpendicular to the transverse direction, i.e., parallel to the longitudinal direction Y. Among them, the positive electrode solid electrolyte includes a sulfide solid electrolyte; the positive electrode stabilizer includes at least one of a moisture absorber and a hydrogen sulfide absorber.

[0242] In some embodiments, based on the positive electrode tab shown in FIG. 1, the filling region 130 further comprises a first binder 132. One example can be seen in FIG. 3.

[0243] In some embodiments, based on the positive electrode tab shown in FIG. 1, the filling region 130 further comprises a first binder 132 and an insulating material 133. One example can be seen in FIG. 4.

[0244] In some embodiments, the positive electrode tab comprises a positive electrode current collector 110 and active film layers on both sides of the positive electrode current collector 110, and the active film layer on either side independently comprises a positive electrode active region 120, and the positive electrode active region 120 on either side independently has two sides facing away from each other, where the two sides on one side are denoted as a first side and a second side, and the two sides on the other side are denoted as a third side and a fourth side, and the first side, the second side, the third side and the fourth side are respectively transversely intersected, and the filling region 130 is respectively arranged on the outer side of the opposite regions of the first side and the second side, and the filling region 130 is respectively arranged on the outer side of the opposite regions of the third side and the fourth side. One example can be seen in FIG. 2. In FIG. 2, the first side, the second side, the third side and the fourth side are exemplarily perpendicular to the transverse direction, i.e. parallel to the longitudinal direction Y. Among them, the positive electrode active region comprises positive electrode active particles and a positive electrode solid electrolyte, and the positive electrode solid electrolyte comprises a sulfide solid electrolyte; the filling region comprises a positive electrode stabilizer, and the positive electrode stabilizer comprises at least one of a moisture absorbent and a hydrogen sulfide absorbent.

[0245] In some embodiments, the first side and the second side are completely covered by the filling region.

[0246] When the filling region completely covers the two sides of the positive electrode active region in the width direction, it is beneficial to better isolate the positive electrode active region from the contact with moisture in the air when assembling the solid-state battery (the solid-state battery can be a full solid-state battery), and to reduce or avoid the escape of hydrogen sulfide gas.

[0247] In some embodiments, in the transverse direction, the positive electrode active region is completely surrounded by the filling region. One example can be seen in FIG. 6.

[0248] When the filling region completely surrounds the positive electrode active region in the transverse direction, it is beneficial to better isolate the positive electrode active region from the contact with moisture in the air when assembling the solid-state battery (the solid-state battery can be a full solid-state battery), and to reduce or avoid the escape of hydrogen sulfide gas.

[0249] In some embodiments, the width of the filling region at different locations along the outer side of the positive active region is greater than or equal to 0.2 mm, optionally 0.2 mm to 10 mm, further optionally 0.25 mm to 10 mm, more further optionally 0.5 mm to 10 mm, and / or any one of the following or a range defined by any two of the following: 0.2 mm, 0.25 mm, 0.3 mm, 0.4 mm, 0.5 mm, 0.6 mm, 0.8 mm, 1 mm, 1.2 mm, 1.4 mm, 1.5 mm, 1.6 mm, 1.8 mm, 2 mm, 2.5 mm, 3 mm, 4 mm, 5 mm, 6 mm, 8 mm, 10 mm (corresponding to 1 cm), etc., in terms of the projected area of the filling region in the lateral direction.

[0250] By controlling the width of the filling region outside the positive active region within a certain range, the positive active region can be reduced or prevented from contacting moisture in the air, and in addition, a higher energy density can be achieved by further selecting a suitable range.

[0251] In some embodiments, the volume ratio of the filling region to the positive active region is greater than or equal to 0.2%, optionally 0.2% to 20%, further optionally 0.5% to 10%, more further optionally 1% to 10%, and / or any one of the following or a range defined by any two of the following: 0.2%, 0.4%, 0.5%, 0.6%, 0.8%, 1%, 1.2%, 1.4%, 1.6%, 1.8%, 2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 6%, 6.5%, 7%, 7.5%, 8%, 9%, 10%, etc., and / or a suitable range of the following: 0.5% to 20%, 0.2% to 10%, 3% to 7%, etc.

[0252] By controlling one or both of the mass ratio and the volume ratio of the filling region to the positive active region within the aforementioned ranges, the positive active region can be reduced or prevented from contacting moisture in the air, and in addition, a higher energy density can be achieved by further selecting a suitable range.

[0253] In some embodiments, the thickness of the active film layer is equal at different lateral positions.

[0254] When the thickness of the active film layer is equal at different transverse positions, there is no height difference between the positive active area and the filling area on the side surface of the active film layer away from the positive current collector, so when the positive electrode sheet is used with the negative electrode sheet and subjected to high pressure treatment, it is beneficial to avoid the positive electrode sheet shearing the negative electrode sheet, and it is beneficial to avoid the negative electrode sheet breaking or powdering.

[0255] Non-limitingly, the single-side thickness of the active film layer, the positive active area, or the filling area on the positive current collector can be 30 μm to 200 μm, optionally 60 μm to 130 μm, and can also be any one of the following thicknesses or a range consisting of any two of the following thicknesses: 30 μm, 40 μm, 50 μm, 60 μm, 80 μm, 100 μm, 120 μm, 130 μm, 140 μm, 150 μm, 160 μm, 180 μm, 200 μm, etc.; and can also be any one of the following ranges: 40 μm to 150 μm, 40 μm to 130 μm, 40 μm to 120 μm, 50 μm to 150 μm, 50 μm to 130 μm, 50 μm to 120 μm, 60 μm to 150 μm, 60 μm to 120 μm, etc.

[0256] Non-limitingly, the weight percentage of the positive active particles in the positive active area can be ≥ 80 wt%, and further can be ≥ 90 wt%.

[0257] In some embodiments, the positive active area includes a conductive agent (which can be referred to as a positive conductive agent). As a non-limiting example, the positive conductive agent can be a carbon conductive agent. Non-limitingly, the positive carbon conductive agent can include one or more of super-P, acetylene black, carbon black, ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers. Non-limitingly, the weight percentage of the positive conductive agent in the positive active area can be 0 to 10 wt%, further can be 0 to 8 wt%, further can be 0 to 5 wt%, further can be 0.1 wt% to 3 wt%, based on the total weight of the positive active area. The weight percentage of the positive conductive agent in the positive active area can also be 0.2 wt% to 5 wt%, 0.5 wt% to 5 wt%, 0.1 wt% to 3 wt%, etc.

[0258] As a non-limiting example, the positive current collector has two surfaces facing away from each other in the thickness direction of the positive current collector, and the active film layer is disposed on any one or both of the two surfaces of the positive current collector facing away from each other.

[0259] In some embodiments, the positive electrode current collector can employ a metal foil or a composite current collector. For example, as the metal foil, an aluminum foil can be employed. In the positive electrode current collector, the composite current collector can include a polymer material base layer and a metal layer formed on at least one surface of the polymer material base layer. In the positive electrode current collector, the composite current collector can be obtained by forming a metal material on a polymer material base material. In the positive electrode current collector, non-limiting examples of the metal material can include at least one of aluminum, an aluminum alloy, nickel, a nickel alloy, titanium, a titanium alloy, silver, a silver alloy, and the like. In the positive electrode current collector, non-limiting examples of the polymer material base material can include one or more of polypropylene (PP), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), and the like.

[0260] The positive electrode tab can be prepared by a dry method or a wet method. For example, a dry method can be employed to press into a film. For another example, a wet method can be employed to coat into a film.

[0261] In some embodiments, the positive electrode active region can be compounded with the positive electrode current collector by dry mixing the components described above for preparing the positive electrode active region, such as the positive electrode active particles, the positive electrode solid electrolyte, the second binder, the positive electrode conductive agent, and other optional components, and then heating and press kneading the mixed material into a mass, performing hot rolling to form a self-supporting positive electrode active sheet, and hot rolling the self-supporting positive electrode active sheet with the positive electrode current collector, the self-supporting positive electrode active sheet being compoundable to at least one side (single side or double sides) of the positive electrode current collector to obtain a base sheet including the positive electrode active region. Non-limitingly, a double planetary mixer can be employed for dry mixing. Non-limitingly, a banbury mixer can be employed for heating and press kneading. Non-limitingly, the temperature for performing hot rolling can be 75°C to 85°C, further such as 78°C, 80°C, 82°C, and the like. The method for assembling the solid-state battery (which can be a full solid-state battery) using the positive electrode tab can be suitable for industrial mass production.

[0262] In the present application, the width of the positive electrode active region (see X1 direction) can be 50 mm to 500 mm, but is not limited thereto, and can be any one of the following widths or an interval formed by any two of the following widths: 50 mm, 100 mm, 200 mm, 300 mm, 400 mm, 500 mm, and the like.

[0263] In some embodiments, the substrate including the positive electrode active region can be prepared by dispersing the components described above for preparing the positive electrode active region, such as the positive electrode active particles, the positive electrode solid electrolyte, the second binder, the positive electrode conductive agent, and other optional components, in an organic solvent to form a positive electrode slurry. Further, the positive electrode slurry is coated on at least one side surface of the positive electrode current collector, and after processes such as drying, cold pressing, etc., the positive electrode active region is obtained, and the substrate including the positive electrode active region is obtained. The cold pressing can be performed using a cold rolling machine. The type of organic solvent in the positive electrode slurry can include one or two of p-xylene, mesitylene, butyl butyrate, heptane, etc., and further can be p-xylene. The positive electrode slurry can be coated on a single surface of the positive electrode current collector, or on both surfaces of the positive electrode current collector. The solid content of the positive electrode slurry can be 40 wt% to 80 wt%. The viscosity of the positive electrode slurry at room temperature can be adjusted to 5000 mPa·s to 25000 mPa·s. The positive electrode sheet can have a compacted density of 3.0 g / cm 3 to 3.6 g / cm 3 , and optionally 3.3 g / cm 3 to 3.5 g / cm 3 .

[0264] As used herein, “compact density” has the meaning commonly known in the art and is one of the reference indicators of the energy density of a material. In the present application, unless otherwise specified, the compact density of an electrode sheet refers to the ratio of the mass of the electrode active material layer to its volume. The compact density of a positive electrode sheet refers to the ratio of the mass of the positive electrode active region to its volume, and the compact density of a negative electrode sheet refers to the ratio of the mass of the negative electrode active material layer to its volume.

[0265] Without limitation, the material of the filling region can be disposed on the target area of the positive electrode current collector by coating. Without limitation, the positive electrode stabilizer, the first binder, and optional other components (such as insulating materials) can be mixed with an organic solvent to form a stabilizer slurry, and then an appropriate amount of the stabilizer slurry can be coated on the target area, and after drying and cold pressing, the filling region can be formed, wherein the cold pressing can achieve densification. The solid content of the stabilizer slurry can be 40 wt% to 80 wt%. The type of organic solvent in the stabilizer slurry can include one or two of p-xylene, mesitylene, butyl butyrate, heptane, etc., and further can be p-xylene.

[0266] In the present application, the cold pressing process for preparing the positive electrode active region and the cold pressing process for preparing the filling region can be simultaneously achieved using the same process: the structure layer formed by coating and drying of the positive electrode slurry and the structure layer formed by coating and drying of the stabilizer slurry can be cold pressed together, thereby simultaneously obtaining the positive electrode active region and the filling region, and at this time, the positive electrode active region and the filling region have high consistency in the thickness direction, and the surface of the active film layer in the positive electrode sheet is more uniform as a whole.

[0267] In still another aspect of the present application, there is provided a use of the aforementioned positive electrode tab in the preparation of a solid-state battery.

[0268] In a second aspect of the present application, there is provided a solid-state battery comprising a positive electrode layer, a solid electrolyte layer and a negative electrode layer which are sequentially stacked, wherein the positive electrode layer comprises the positive electrode tab described in the first aspect of the present application.

[0269] In some embodiments, the solid-state battery is a full solid-state battery.

[0270] In some embodiments, there is provided a full solid-state battery comprising a positive electrode layer, a solid electrolyte layer and a negative electrode layer which are sequentially stacked, wherein the positive electrode layer comprises the positive electrode tab described in the first aspect of the present application.

[0271] Unless otherwise specified, the solid-state battery provided in the present application is a solid-state secondary battery.

[0272] Unless otherwise specified, the full solid-state battery provided in the present application is a full solid-state secondary battery.

[0273] In the present application, the full solid-state battery comprises a solid-state battery monomer, and the solid-state battery monomer comprises the positive electrode tab described in the first aspect of the present application.

[0274] In the present application, unless otherwise specified, the "solid-state battery monomer" refers to a basic unit capable of realizing the mutual conversion between chemical energy and electrical energy, and all the components are solid. In some embodiments, the solid-state battery monomer can be a full solid-state battery monomer.

[0275] In the present application, the full solid-state battery comprises a full solid-state battery monomer, and the full solid-state battery monomer comprises the positive electrode tab described in the first aspect of the present application.

[0276] In the present application, unless otherwise specified, the "full solid-state battery monomer" refers to a basic unit capable of realizing the mutual conversion between chemical energy and electrical energy, and all the components are solid. At this time, the solid-state battery monomer in which the electrolyte in the battery is a solid-state battery monomer with solid-state electrolyte, at this time, the positive electrode layer, the negative electrode layer and the electrolyte part all adopt solid materials, and no liquid electrolyte is arranged in the battery monomer, and thus it can be called a "full solid-state battery monomer".

[0277] Without limitation, the solid-state battery monomer (which can be a full solid-state battery monomer) can comprise a positive electrode layer, a solid electrolyte layer and a negative electrode layer, and the solid electrolyte layer is located between the positive electrode layer and the negative electrode layer. In the charging and discharging process of the battery, active ions are embedded and extracted between the positive electrode layer and the negative electrode layer. The solid electrolyte layer plays a role in conducting ions between the positive electrode layer and the negative electrode layer, and can also isolate the positive electrode layer from the negative electrode layer to prevent short circuiting of the positive and negative electrodes.

[0278] In some embodiments, the positive electrode layer, the solid electrolyte layer, and the negative electrode layer have the same projected area in the longitudinal direction.

[0279] By arranging the positive electrode layer, the solid electrolyte layer, and the negative electrode layer to have the same size in the lateral direction and aligning them, the projected areas of the three layers in the longitudinal direction are made the same (in this case, the side surfaces of the respective layers are aligned), which is advantageous in reducing layer breakage or powdering caused by interlayer shearing during high-pressure processing.

[0280] Some descriptions regarding the negative electrode layer are provided below.

[0281] The negative electrode layer can be provided by a negative electrode sheet that is known in the art for use in solid-state batteries (which can be all-solid-state batteries), or the constituent materials of the negative electrode layer can be pressed into a film on one side surface of the solid electrolyte layer.

[0282] The negative electrode layer can be prepared by a dry method or a wet method. For example, a dry method can be used to press the layer into a film. For another example, a wet method can be used to coat the layer into a film.

[0283] The negative electrode layer includes a negative electrode active material layer, and the negative electrode active material layer includes a negative electrode active substance.

[0284] Non-limitingly, the weight percentage of the negative electrode active substance in the negative electrode active material layer can be ≥ 80 wt%, and further can be ≥ 90 wt%.

[0285] In some embodiments, the negative electrode active substance is an indium-lithium alloy (InLi alloy).

[0286] In some embodiments, the negative electrode layer is an InLi alloy film.

[0287] In some embodiments, the negative electrode active substance can also be a negative electrode active substance known in the art for use in solid-state batteries (which can be all-solid-state batteries). As non-limiting examples, the negative electrode active substance can include one or more of the following materials: one or more of elemental silicon, elemental tin, silicon-carbon negative electrode, silicon monoxide, graphite, and metallic lithium. However, the present application is not limited to these materials or substances, and other conventional materials that can be used as negative electrode active substances for batteries can also be used. These negative electrode active substances can be used alone or in combination with two or more kinds.

[0288] In some embodiments, the negative active material comprises one or more of a carbon-based material, a silicon-based material, a tin-based material, and a lithium titanate, and a modified form of any of the foregoing, wherein the modified form comprises one or more of a doping modification and a coating modification. Both the doping modification and the coating modification can be made by or with reference to the modification methods known in the art, including but not limited to the selection of the element species and the doping amount. The carbon-based material can include but is not limited to one or more of a graphite material, a soft carbon, and a hard carbon. The graphite material can include one or more of an artificial graphite and a natural graphite.

[0289] In some embodiments, the negative active material comprises a carbon-based material and a silicon-based material. Without limitation, the total weight of the carbon-based material and the silicon-based material can account for ≥ 80%, optionally ≥ 90%, further optionally ≥ 95%, still further optionally ≥ 96%, and so on, and still further optionally 100%, and so on, of the total weight of the negative active material. The total weight of the graphite material and the silicon-based material can also account for any one of the following percentages, or greater than or equal to any one of the following percentages and less than or equal to 100%, or selected from the interval formed by any two of the following percentages: 80%, 82%, 83%, 84%, 85%, 86%, 88%, 90%, 92%, 94%, 95%, 96%, 98%, and so on, of the total weight of the negative active material. The carbon-based material can be defined as described above, for example, the carbon-based material can be a graphite material. The content of the carbon-based material can also be defined according to any suitable embodiment in the context.

[0290] In some embodiments, the negative active material comprises a carbon-based material and a silicon-based material in a mass ratio of 1:(1-3). The mass ratio of the carbon-based material and the silicon-based material can also be 1:(1-2), 1:(1.5-2), and so on.

[0291] In some embodiments, the negative electrode layer can include a negative electrode current collector and a negative electrode active material layer disposed on at least one surface of the negative electrode current collector, the negative electrode active material layer including a negative electrode active material. As a non-limiting example, the negative electrode current collector has two surfaces facing away from each other in a thickness direction thereof, and the negative electrode active material layer is disposed on either one or both of the two surfaces of the negative electrode current collector. In some embodiments, the negative electrode current collector can employ a metal foil or a composite current collector. For example, as the metal foil, a copper foil can be employed. In the negative electrode current collector, the composite current collector can include a polymer material base layer and a metal layer formed on at least one surface of the polymer material base layer. In the negative electrode current collector, the composite current collector can be formed by forming a metal material on the polymer material base layer. In the negative electrode current collector, non-limiting examples of the metal material can include one or more of copper, copper alloy, nickel, nickel alloy, titanium, titanium alloy, silver, silver alloy, and the like. In the negative electrode current collector, non-limiting examples of the polymer material base layer can include one or more of polypropylene (PP), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), and the like.

[0292] In some embodiments, the negative electrode active material layer includes a binder (which can be referred to as a negative electrode binder). Non-limiting examples of the negative electrode binder can include one or more of a rubber-based binder, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), a vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, a vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene terpolymer, a tetrafluoroethylene-hexafluoropropylene copolymer, a fluorine-containing acrylate resin, polyacrylic acid (PAA), sodium polyacrylate (PAAS), polyacrylamide (PAM), polyvinyl alcohol (PVA), sodium alginate (SA), polymethacrylic acid (PMAA), carboxymethyl chitosan (CMCS), and the like. Non-limiting examples of the weight percentage of the negative electrode binder in the negative electrode active material layer can be 0-10 wt%, more further can be 0-5 wt%, more further can be 1-5 wt%, and more further can be 1-3 wt%. Non-limiting examples of the rubber-based binder can include one or more of styrene butadiene rubber, nitrile butadiene rubber, hydrogenated nitrile butadiene rubber, and the like. In some embodiments, non-limiting examples of the negative electrode binder can include one or more of styrene butadiene rubber (SBR), polyacrylic acid (PAA), sodium polyacrylate (PAAS), polyacrylamide (PAM), polyvinyl alcohol (PVA), sodium alginate (SA), polymethacrylic acid (PMAA), and carboxymethyl chitosan (CMCS).

[0293] In some embodiments, the negative active material layer comprises a conductive agent (which can be referred to as a negative conductive agent). Without limitation, the negative conductive agent can comprise a carbon conductive agent. Without limitation, the negative carbon conductive agent can comprise one or more of super-P, acetylene black, carbon black, ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers. The weight percentage of the negative conductive agent in the negative active material layer can be 0-15 wt%, further optionally 0-10 wt%, further optionally 0-5 wt%, further optionally 0.1-5 wt%. The weight percentage of the negative conductive agent in the negative active material layer can also be 0.2-5 wt%, 0.5-5 wt%, 0.1-3 wt%, etc.

[0294] In some embodiments, the negative active material layer optionally comprises other auxiliary agents, such as thickening agents (e.g., sodium carboxymethyl cellulose (CMC-Na)) and the like. The weight percentage of the other auxiliary agents in the negative active material layer can be 0-15 wt%, further optionally 0-10 wt%, further optionally 0-5 wt%, further optionally 0-3 wt%, further optionally 0-2 wt%.

[0295] In some embodiments, the negative electrode layer can be prepared by dispersing the components described above for preparing the negative electrode layer, such as the negative active material, the negative conductive agent, the negative binder, and other optional components, in a solvent to form a negative electrode slurry. In some examples, the solvent is a non-aqueous solvent, and a non-limiting example of a non-aqueous solvent is N-methyl pyrrolidone (NMP). Further, the negative electrode slurry is coated on at least one side surface of the negative current collector, and after processes such as drying, cold pressing, and the like, a negative electrode sheet is obtained. The cold pressing can be performed using a cold rolling machine. The surface of the negative current collector to which the negative electrode slurry is coated can be a single surface of the negative current collector, or can be both surfaces of the negative current collector. The solid content of the negative electrode slurry can be 30-70 wt%, optionally 40-60 wt%. The viscosity of the negative electrode slurry at room temperature can be adjusted to 2000-10000 mPa·s, optionally 3000-10000 mPa·s. The compaction density of the negative electrode sheet can be 1.0-2.0 g / cm 3 3 3 3

[0296] The following is some description regarding the solid electrolyte layer.

[0297] The solid electrolyte layer functions to conduct ions between the positive electrode layer and the negative electrode layer, and also functions to isolate the positive electrode layer from the negative electrode layer to prevent short circuiting between the positive electrode and the negative electrode. ​​​​

[0298] The solid electrolyte layer includes a solid electrolyte. The solid electrolyte in the solid electrolyte layer can employ a solid electrolyte known in the art that can be used in a solid-state battery (which can be a full solid-state battery). As a non-limiting example, the solid electrolyte in the solid electrolyte layer can include one or more of the following materials: one or more of a sulfide solid electrolyte, a halide solid electrolyte, an oxide solid electrolyte, a polymer solid electrolyte, etc. The kind of the sulfide solid electrolyte in the solid electrolyte layer can be the same as or different from the sulfide solid electrolyte in the positive electrode layer.

[0299] In some embodiments, the solid electrolyte layer can be pressed from a solid electrolyte material into a solid electrolyte film.

[0300] In some embodiments, the solid electrolyte layer can have a thickness of 0.1 pm to 1000 pm, optionally 10 pm to 100 pm.

[0301] In this application, the assembly of the positive electrode layer, the solid electrolyte layer, and the negative electrode layer can be stacked in at least one of a stacking manner and a winding manner.

[0302] Without limitation, the positive electrode sheet, the solid electrolyte film, and the negative electrode sheet can be sequentially stacked (stacking manner assembly), the solid electrolyte is placed between the positive electrode sheet and the negative electrode sheet, and a solid-state battery cell (which can be a full solid-state battery cell) is prepared by hot rolling.

[0303] In some embodiments, the solid-state battery cell includes a solid-state battery cell.

[0304] In some embodiments, the solid-state battery cell is a full solid-state battery cell.

[0305] In some embodiments, the full solid-state battery cell includes a full solid-state battery cell.

[0306] In some embodiments, referring to FIG. 7, the solid-state battery cell (which can be a full solid-state battery cell) includes a positive electrode layer 100, a solid electrolyte layer 200, and a negative electrode layer 300 that are sequentially stacked. As an example, the positive electrode layer 100 in FIG. 7 is provided by the positive electrode sheet 10 shown in FIG. 2.

[0307] In some embodiments, the negative electrode layer 300 includes a negative electrode current collector 310 and negative electrode active material layers 320 located on both sides of the negative electrode current collector 310.

[0308] In some embodiments, based on the full solid-state battery cell shown in FIG. 7, the negative electrode layer 300 includes a negative electrode current collector 310 and negative electrode active material layers 320 located on both sides of the negative electrode current collector 310. As an example, refer to FIG. 8.

[0309] In some embodiments, the solid-state battery (which can be a full solid-state battery) includes at least one solid-state battery cell. The solid-state battery can include one or more solid-state battery cells.

[0310] In some embodiments, the solid-state battery (which can be a full solid-state battery) includes at least one solid-state battery cell. The solid-state battery can include one or more solid-state battery cells.

[0311] In some embodiments, the solid-state battery (which can be a full solid-state battery) includes at least one solid-state battery cell. The solid-state battery can include one or more solid-state battery cells.

[0312] In some embodiments, the solid-state battery (which can be a full solid-state battery) includes at least one solid-state battery cell. The solid-state battery can include one or more solid-state battery cells.

[0313] In some embodiments, the solid-state battery (which can be a full solid-state battery) includes at least one solid-state battery cell. The solid-state battery can include one or more solid-state battery cells.

[0314] In some embodiments, the solid-state battery (which can be a full solid-state battery) includes at least one solid-state battery cell. The solid-state battery can include one or more solid-state battery cells.

[0315] In some embodiments, the solid-state battery (which can be a full solid-state battery) includes at least one solid-state battery cell. The solid-state battery can include one or more solid-state battery cells.

[0316] In some embodiments, the solid-state battery (which can be a full solid-state battery) includes at least one solid-state battery cell. The solid-state battery can include one or more solid-state battery cells.

[0317] In some embodiments, referring to FIG. 11, the outer package can include a housing 51 and a cover plate 53. The housing 51 can include a bottom plate and side plates connected to the bottom plate, which enclose a receiving cavity. The housing 51 has an opening communicating with the receiving cavity, and the cover plate 53 can be arranged on the opening to close the receiving cavity. The all-solid-state battery cell 52 is packaged in the receiving cavity. The number of all-solid-state battery cells 52 contained in the all-solid-state battery cell 5 can be one or more, which can be selected by those skilled in the art according to actual needs.

[0318] The solid-state battery can be a battery module 4 or a battery pack 1.

[0319] The all-solid-state battery can be a battery module 4 or a battery pack 1.

[0320] The battery module includes at least one solid-state battery cell.

[0321] In some embodiments, the battery module includes at least one all-solid-state battery cell. The number of all-solid-state battery cells contained in the battery module can be one or more, which can be selected by those skilled in the art according to the application and capacity of the battery module.

[0322] In some embodiments, in the battery module, the plurality of solid-state battery cells can be arranged sequentially along the length direction of the battery module. Of course, they can also be arranged in any other manner. Further, the plurality of solid-state battery cells can be fixed by fasteners. Alternatively, the battery module can also include a housing having a receiving space, and the plurality of solid-state battery cells are received in the receiving space.

[0323] FIG. 12 is a battery module 4 as an example. Referring to FIG. 12, in the battery module 4, the plurality of all-solid-state battery cells 5 can be arranged sequentially along the length direction of the battery module 4. Of course, they can also be arranged in any other manner. Further, the plurality of all-solid-state battery cells 5 can be fixed by fasteners.

[0324] Alternatively, the battery module 4 can also include a housing having a receiving space, and the plurality of all-solid-state battery cells 5 are received in the receiving space.

[0325] In some embodiments, the above-mentioned battery module can also be assembled into a battery pack, and the number of battery modules contained in the battery pack can be one or more, which can be selected by those skilled in the art according to the application and capacity of the battery pack.

[0326] Figs. 13 and 14 are a battery pack 1 as an example. Referring to Figs. 13 and 14, a battery case and a plurality of battery modules 4 provided in the battery case can be included in the battery pack 1. The battery case includes an upper case 2 and a lower case 3, and the upper case 2 can be provided to cover the lower case 3 and form an enclosed space for accommodating the battery modules 4. The plurality of battery modules 4 can be arranged in the battery case in any manner.

[0327] In a third aspect of the present application, a power consuming device is provided, which includes the solid-state battery of the second aspect of the present application.

[0328] In some embodiments, a power consuming device is provided, which includes the all-solid-state battery of the second aspect of the present application.

[0329] In a fourth aspect of the present application, a method for preparing an all-solid-state battery is provided, which includes the following steps:

[0330] providing a substrate including a solid electrolyte layer and a negative electrode layer stacked thereon, the negative electrode layer being located on one side of the solid electrolyte layer;

[0331] compositing the positive electrode sheet of the first aspect of the present application on the side of the solid electrolyte layer away from the negative electrode layer to prepare a solid-state battery.

[0332] In some embodiments, a method for preparing an all-solid-state battery is provided, which includes the following steps:

[0333] providing a substrate including a solid electrolyte layer and a negative electrode layer stacked thereon, the negative electrode layer being located on one side of the solid electrolyte layer;

[0334] compositing the positive electrode sheet of the first aspect of the present application on the side of the solid electrolyte layer away from the negative electrode layer to prepare an all-solid-state battery.

[0335] In some embodiments, the power consuming device includes the all-solid-state battery of any of the embodiments provided in the present application.

[0336] Without limitation, the solid-state battery (which can be an all-solid-state battery) can be used as a power source of a power consuming device, or as an energy storage unit of a power consuming device. The power consuming device can include a mobile device, an electric vehicle, an electric train, a ship and a satellite, an energy storage system, etc., but is not limited thereto. Among them, the mobile device can be a mobile phone, a notebook computer, etc.; the electric vehicle can be a pure electric vehicle, a hybrid electric vehicle, a plug-in hybrid electric vehicle, an electric bicycle, an electric scooter, an electric golf cart, an electric truck, an electric motorcycle, an electric tool, etc., but is not limited thereto. The power consuming device can also be applied to military equipment, aerospace, etc., and can also be applied to hydroelectric, thermal, wind and solar power stations, etc. energy storage power systems.

[0337] As the power consuming device, a solid-state battery (which can be a full solid-state battery) can be selected according to the use requirement thereof.

[0338] FIG. 15 is a power consuming device 6 as an example. The power consuming device is a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle, etc. In order to meet the requirement of high power and high energy density of the solid-state battery or the full solid-state battery for the power consuming device, a battery pack or a battery module can be used.

[0339] The device as another example can be a mobile phone, a tablet computer, a notebook computer, etc. The device usually requires thinning, and a solid-state battery (which can be a full solid-state battery) can be used as a power source.

[0340] Hereinafter, some embodiments of the present application will be described. The embodiments described below are exemplary and are only used to explain the present application, and cannot be understood as a limitation of the present application. The technology or condition not mentioned in the embodiments is carried out according to the description in the foregoing, or according to the technology or condition described in the literature in the art, or according to the product instruction. The reagent or instrument not mentioned by the manufacturer is a conventional product that can be obtained by market purchase, or can be synthesized by a conventional method according to the market product.

[0341] In the following examples, room temperature refers to 20-30°C.

[0342] It should be noted that the full solid-state battery is used as a non-limiting example of the solid-state battery in each of the following embodiments and examples.

[0343] Unless otherwise specified, the D50 of the mixed particles in each example refers to the particle size (D50) of the mixed particles measured by the laser diffraction method according to GB / T 19077-2016. v 50, according to GB / T 19077-2016 particle size distribution laser diffraction method, using Mastersizer 2000E type laser particle size analyzer of British Malvern Instruments Co., Ltd. to test and obtain.

[0344] The positive active particles used in the following examples can be prepared by the method described above. For example, in Example 1, the positive active material NCM811 (LiNi 0.8 Co 0.1 Mn 0.1 O2), the coating layer is Li3BO3, the positive active body is NCM811, the weight percentage of the coating layer in the positive active particles is 0.2wt%, and the thickness of the coating layer is about 5nm.

[0345] (1) Preparation of the positive active body: according to LiNi 0.8 Co 0.1 Mn 0.1O2 corresponding atomic molar ratio, after mixing lithium chloride, nickel oxide, cobalt oxide and manganese sulfate uniformly, pure water is added, the solid content of the slurry is adjusted to about 30wt%, then it is put into a beater to mix for 30min, a mixed solution is prepared, the mixed solution is further put into a ball mill, 0.1mm zirconium oxide grinding balls are used to ball mill at a speed of 1000rpm for 12h, the obtained slurry is put into a spray dryer to dry and granulate to obtain a positive electrode material precursor; an air flow type spray drying method is used for atomization, the air inlet temperature of the equipment is set to 250°C, the air outlet temperature is 80°C, and the compressed air pressure is 0.7MPa; finally, the obtained positive electrode material precursor is put into a tube furnace, high temperature calcination is carried out at 950°C for 13h in an oxygen atmosphere, after calcination, air flow crushing and 300 mesh sieving, a powder-like ternary NCM positive electrode material composed of a positive electrode active body is obtained, which can be denoted as NCM body.

[0346] (2) Preparation of coating layer material. Mix Li2CO3 and B2O3 in a molar ratio of 3:1, heat at 600°C in air for 10h to obtain LBO powder. Ball mill the LBO powder at a speed of 400rpm, grind for 10min, then pause for 20min, repeat the "grind / pause" operation 99 times. Then perform a crushing treatment to reduce the D v 50of the LBO powder to less than or equal to 1μm, obtaining LBO coating material.

[0347] (3) Forming a coating layer on the surface of the positive electrode active body. Mix LBO coating material and NCM body in a mass ratio of 3:7, ball mill at 400rpm for 30min, then calcine in air at 800°C for 2h. Prepare to obtain the positive electrode active particles of Example 1.

[0348] Preparation Example

[0349] Example 1

[0350] (1) Preparation of binder glue containing binder.

[0351] Mix p-xylene and nitrile rubber (NBR) to make glue, wherein the mass ratio of xylene to NBR is 95:5; after weighing the above solid and liquid raw materials, stir at 25°C at a speed of 1000rpm for 300min, and finally obtain a uniform binder glue.

[0352] In this example, NBR is used as both the first binder in the filling area and the second binder in the positive electrode active area.

[0353] (2) Preparation of positive electrode substrate including positive electrode active area.

[0354] The positive electrode active material NCM811 (LiNi 0.8 Co0.1 Mn 0.1 O2) as the positive active particles, the weight ratio of the Li3BO3 coating layer in the positive active particles is 0.2wt%; Li6PS5Cl is used as the positive solid electrolyte, vapor grown carbon fiber (VGCF) is used as the positive conductive agent, the second binder is provided by the binder glue solution prepared in the first step, the positive active particles, the positive solid electrolyte, the positive conductive agent and the second binder are mixed in a mass ratio of 78:19:1:2, and a mixed slurry is obtained; the slurry solid content is controlled to 60wt% by adding dimethylbenzene in the above-mentioned mixed slurry, and a positive electrode slurry is obtained. The gap coating method is used to coat the double sides of the carbon-coated aluminum foil, wherein the size of the positive active area is 5cmx8.5cm, the coating gap is 1cm, the reserved tab side blank is 5cm, and the total blank width at the position of the prepared filling area is 1cm (the volume ratio of the filling area to the positive active area is 20%, the thickness and length of the filling area and the positive active area are the same, and the volume ratio and the width ratio are equal in value), and after coating, drying is performed at a drying temperature of 120°C, and a positive electrode substrate including a positive active area is obtained after drying. The compaction density of the positive active area is 3.5g / cm 3 .

[0355] (3) Preparation of stabilizer slurry.

[0356] The binder NBR (first binder) is mixed with the positive stabilizer CaCl2, wherein the mass ratio of CaCl2 to NBR is 95:5; wherein NBR is added in the form of the binder glue solution prepared in the first step, and the solid content of the filler slurry is controlled by adjusting the amount of solvent dimethylbenzene added, and the solid content is adjusted to 50wt%. The above-mentioned materials are stirred at a stirring speed of 1000rpm for 300min at 25°C to make the mixture uniform, and a stabilizer slurry is obtained.

[0357] (4) Preparation of a positive electrode tab including a filling area and a positive active area.

[0358] The gap coating method is used, and the stabilizer slurry prepared in the third step is used to coat the positive electrode substrate including the positive active area again, and the stabilizer slurry is coated around the positive active area, i.e. the 5mm area outside the positive active area is coated, and the total width of both sides is 1cm.

[0359] Since the coating gap of the positive active area of the positive electrode substrate is 1 cm during preparation, the stabilizer slurry can be coated at the gap of the positive active area. The tab side and the opposite side need to be coated with the stabilizer slurry in the 5 mm area outside the positive active area. After coating, drying is performed at a temperature of 120°C. After drying, the positive electrode sheet including the filling area and the positive active area is obtained. The positive electrode sheet is die-cut using a custom-made knife die. The transverse size of the active film layer corresponding to the knife die is 6 cm x 9.5 cm.

[0360] (5) Preparation of a solid electrolyte slurry for preparing a solid electrolyte layer.

[0361] The binder NBR is mixed with the solid electrolyte Li6PS5Cl to prepare the electrolyte slurry. The mass ratio of Li6PS5Cl to NBR is 98:2. The NBR is added in the form of the binder glue prepared in step (1). The solid content of the slurry is controlled by adjusting the amount of the solvent dimethylbenzene. The solid content is adjusted to 50 wt%. The slurry is stirred at 25°C for 300 min at a speed of 1000 rpm. After mixing, the solid electrolyte slurry is obtained.

[0362] (6) Preparation of a negative electrode sheet.

[0363] Nanosilicon, graphite, VGCF, and the binder polyvinylidene fluoride (PVDF) are mixed in a solvent N-methylpyrrolidone (NMP) according to a mass ratio of 55:30:12:3. The PVDF is dissolved in NMP. The binder glue and other components are mixed and stirred to form a uniform slurry. The solid content of the slurry is controlled by adding NMP to the mixed slurry. The solid content is adjusted to 30 wt%. The above materials are mixed and stirred to obtain a negative electrode slurry. The negative electrode slurry is continuously coated on both sides of a copper foil. The coating width of the electrode sheet is 9.5 cm. After coating, drying is performed at a temperature of 80°C. After drying, rolling is performed. Finally, the negative electrode sheet is obtained. The compaction density of the negative electrode sheet is 2.1 g / cm 3 .

[0364] (7) Preparation of a solid electrolyte-coated negative electrode sheet.

[0365] The solid electrolyte slurry is continuously coated on the negative electrode sheet. After coating, drying is performed at a temperature of 80°C. After drying, rolling is performed. Finally, the solid electrolyte-coated negative electrode sheet is obtained. The negative electrode active material layer corresponding to the knife die has a size of 6 cm x 9.5 cm.

[0366] (8) Assembly of a full solid-state battery.

[0367] The die-cut pieces in the above steps (4) and (7) are aligned and packaged by stacking, and after packaging, isostatic pressing is performed at 550 MPa and 90°C for 30 min. After the pressure is applied, the above battery cell is welded, packaged, and the like, and finally a full solid-state battery is obtained.

[0368] Examples 2-6. Changing the coating layer composition of the positive active particles.

[0369] A full solid-state battery is prepared by substantially the same method as in Example 1, except that the coating layer of the positive active particles in the positive active region is different. In the preparation process of step (2), the coating layer material for coating the positive active material is replaced with LiNbO3, Li2ZrO3, Li2SiO3, LiPO3, and Li2MnO4, respectively, and the basic coating layer thickness is controlled, and the other conditions are the same as in Example 1.

[0370] Examples 7-11. Changing the solid electrolyte type in the solid electrolyte layer.

[0371] A full solid-state battery is prepared by substantially the same method as in Example 1, except that the solid electrolyte type for preparing the solid electrolyte layer is different. In the process of preparing the solid electrolyte slurry in step (5), the solid electrolyte material is replaced with Li3YCl6, Li 10 GeP2S 12 , Li7La3Zr2O 12 , Li2S-P2S5, and LiI-LiBr-Li2S-P2S5, and the remaining operation conditions are the same as in Example 1.

[0372] Examples 12-21. Changing the positive stabilizer.

[0373] A full solid-state battery is prepared by substantially the same method as in Example 1, except that the positive stabilizer type is different. In the process of preparing the stabilizer slurry in step (3), the positive stabilizer is replaced with CaH2, anhydrous CuSO4, silica gel, lithium chloride, imidazole acid molecular sieve, porous carbon (activated carbon), Fe2O3, ZnO, Bi2O3, and CuO, respectively, and the other conditions are the same as in Example 1.

[0374] Examples 22-26. Changing the positive stabilizer, including a dual adsorbent.

[0375] A full solid-state battery is prepared by substantially the same method as in Example 1, except that the positive stabilizer type is different, and is replaced with a combination of anhydrous CuSO4 and ZnO with mass ratios of 2:8, 4:6, 5:5, 6:4, and 8:2, respectively. In the process of preparing the stabilizer slurry in step (3), the positive stabilizer is replaced according to the above ratios, and the other conditions are the same as in Example 1.

[0376] Examples 27-28. Change the positive electrode stabilizer to a dual physical absorption agent and a dual chemical absorption agent.

[0377] A full solid-state battery was prepared using a method substantially the same as that of Example 1, except that the type of positive electrode stabilizer was changed. In Example 27, the positive electrode stabilizer was replaced with imidazole acid molecular sieve and ZnO at a mass ratio of 1:1; in Example 28, the positive electrode stabilizer was replaced with activated carbon and CuO at a mass ratio of 1:1.

[0378] Example 29. Change the positive electrode stabilizer.

[0379] A full solid-state battery was prepared using a method substantially the same as that of Example 1, except that the type of positive electrode stabilizer was changed. The positive electrode stabilizer was replaced with anhydrous CuSO4 and Bi2O3 at a mass ratio of 1:1.

[0380] Example 30. Add an insulating material to the filling area.

[0381] A full solid-state battery was prepared using a method substantially the same as that of Example 1, except that an insulating material, Al2O3, was added to the filling area. In step (3), a stabilizer slurry was prepared by mixing a binder NBR (first binder), a positive electrode stabilizer CaCl2, and the insulating material Al2O3, at a mass ratio of 49:2:49. The remaining steps were the same as those of Example 1.

[0382] Example 31. The positive electrode active particles were not provided with a coating layer.

[0383] A full solid-state battery was prepared using a method substantially the same as that of Example 1, except that the positive electrode active particles were different. Lithium iron phosphate (LFP) without a coating layer was used as the positive electrode active particles. The remaining steps were the same as those of Example 1.

[0384] Example 32. Change the positive electrode stabilizer and the content of the first binder in the filling area.

[0385] A full solid-state battery was prepared using a method substantially the same as that of Example 1, except that the positive electrode stabilizer and the content of the first binder in the filling area were different. In step (3), the mass ratio of CaCl2 to NBR was controlled to be 98:2. The remaining steps were the same as those of Example 1.

[0386] Example 33.

[0387] A full solid-state battery was prepared using a method substantially the same as that of Example 1, except that the warm isostatic pressing conditions in step (8) were changed. The warm isostatic pressing conditions were adjusted as follows: the pressure was 350 MPa, the holding temperature was 60°C, and the holding time was 10 min. The other conditions were the same as those of Example 1.

[0388] Examples 34-35. The positive electrode solid electrolyte further comprises a halide solid electrolyte.

[0389] The all-solid-state battery was prepared by substantially the same method as in Example 1, except that the positive electrode solid electrolyte further comprises a halide solid electrolyte, and in step (5) for preparing the solid electrolyte slurry, a portion of the sulfide solid electrolyte was replaced with a halide solid electrolyte Li3YCl6, and the mass ratio of the sulfide solid electrolyte to the halide solid electrolyte in Example 34 and Example 35 was 8:2 and 5:5, respectively.

[0390] Examples 36-37.

[0391] The all-solid-state battery was prepared by substantially the same method as in Example 1, except that the positive electrode stabilizer, the first binder, the insulating material, the volume ratio of the filling area to the positive electrode active area (numerically equal to the width ratio of the filling area to the positive electrode active area), and the weight ratio of the coating layer in the positive electrode active particles were different, which can be referred to Tables 1-3.

[0392] When adjusting the volume ratio of the filling area to the positive electrode active area, the positive electrode active area width remained unchanged (5 cm), and the relative volume ratio of the filling area was changed by changing the width of the filling area on both sides of the positive electrode active area. In addition, the width of the filling area on both sides of the positive electrode active area was made consistent.

[0393] Comparative Example 1. The overhang design was not used (no filling area was set), and the size of the positive electrode active area and the negative electrode active material layer was the same.

[0394] This comparative example used the same material formulation for each layer as in Example 1, except that during the preparation of the positive electrode sheet, the coating process of the hygroscopic agent slurry was omitted, and the die cutting size of the positive and negative electrode sheets remained consistent, with the corresponding transverse size of the die being 5 cm x 8.5 cm, and the other conditions being the same as in Example 1.

[0395] Comparative Example 2. No filling area was set, and the size of the positive electrode active area was smaller than that of the negative electrode active material layer.

[0396] This comparative example used the same material formulation for each layer as in Comparative Example 1, and during the preparation of the positive electrode sheet, step (4) of coating the stabilizer slurry was omitted, and the positive electrode sheet including the positive electrode active area was used to assemble the all-solid-state battery, with the die cutting size of the positive electrode being 5 cm x 8.5 cm and the size of the composite negative electrode and electrolyte layer being 6 cm x 9.5 cm, and the battery preparation process method being consistent with Example 1, while the hygroscopic agent slurry was coated on the outside of the battery, and the other test methods and conditions were the same as in Example 1.

[0397] Comparative Example 3. The positive electrode stabilizer was replaced with an insulating material.

[0398] A full solid-state battery was prepared by substantially the same method as in Example 1, except that in step (3), the positive electrode stabilizer in the filling area was replaced by TiO2.

[0399] Comparative Example 4. The positive electrode stabilizer was replaced by the first binder.

[0400] A full solid-state battery was prepared by substantially the same method as in Example 1, except that in step (3), the positive electrode stabilizer in the filling area was replaced by NBR; in step (4), the binder glue prepared in step (1) was diluted to about 2000 mPa·S with xylene, and the diluted binder glue was used to replace the stabilizer slurry in Example 1 to coat the corresponding blank area outside the positive electrode active area, and then dried.

[0401] Comparative Example 5. The positive electrode stabilizer was replaced by a water-stable solid electrolyte.

[0402] A full solid-state battery was prepared by substantially the same method as in Example 1, except that in step (3), the positive electrode stabilizer in the filling area was replaced by lithium-containing electrolyte LATP (Li 1.3 Al 0.3 Ti 1.7 (PO4)3).

[0403] Comparative Examples 6-7. The positive electrode stabilizer was replaced by an insulating material.

[0404] A full solid-state battery was prepared by substantially the same method as in Examples 34-35, except that in step (3), the positive electrode stabilizer in the filling area was replaced by insulating material Al2O3. Comparative Example 6 corresponds to Example 34, and Comparative Example 7 corresponds to Example 5.

[0405] The preparation parameters of Examples 1-37 and Comparative Examples 6-7 can also be referred to Tables 1-3.

[0406] Table 1.

[0407] Table 2.

[0408] Table 3.

[0409] II. Test of Related Parameters of Full Solid-state Batteries

[0410] The test process of some battery performance parameters of the full solid-state batteries prepared in each example and each comparative example is as follows.

[0411] 1. Test of open circuit voltage and internal resistance of battery

[0412] The test procedure of open circuit voltage of battery is as follows: at 25℃, the full solid battery to be tested is tested for voltage and internal resistance by using a multimeter.

[0413] 2. Measurement of sulfide generation amount of full solid battery

[0414] The full solid battery sample which has been subjected to warm isostatic pressing but has not been subjected to tab welding packaging and the like is placed in a sealed bag in a glove box which is replaced by Ar gas (dew point below -60℃) after being sufficiently dried. Thereafter, a polyacrylic acid material box having a volume capacity of 1755 cm 3 is placed in a constant temperature and humidity tank which is kept at room temperature (25℃) and humidity of 30% RH in an atmospheric atmosphere, and kept until the inside of the polyacrylic acid material box is the same as the environment in the constant temperature and humidity tank, after which the sealed bag in which the sample is placed is opened in the constant temperature and humidity tank, and the sample is quickly disposed in the polyacrylic acid material box. The hydrogen sulfide generated in 300 seconds immediately after the sample is disposed in the polyacrylic acid material box is measured for hydrogen sulfide concentration by using a hydrogen sulfide sensor (Riken Keiki Manufacturing GX-2009). The volume V (unit: cubic centimeter) of hydrogen sulfide at 25℃ and standard atmospheric pressure is calculated from the hydrogen sulfide concentration after 300 seconds, and divided by the mass m (unit: g) of all sulfide electrolyte materials in the solid battery, and the hydrogen sulfide generation amount is calculated as V / m, unit: cm 3 ·g -1 , which represents the hydrogen sulfide gas volume per gram of sulfide solid electrolyte parameter.

[0415] 3. Test of battery capacity retention rate

[0416] The test procedure of battery capacity retention rate is as follows: at 25℃, the full solid battery to be tested is charged at 1 / 3C constant current to 4.3V, then charged at 4.3V constant voltage until the current is 0.05C, left for 5 min, then discharged at 1 / 3C to 2V, and the obtained capacity is recorded as initial capacity Co. The above steps are repeated for the same battery, and the discharge capacity Cn of the battery after the nth cycle is recorded at the same time, then the battery capacity retention rate Pn = Cn / Co x 100% after each cycle; the data measured after 100 cycles under the above test conditions, i.e. the value of P100, can be recorded as "capacity retention rate after 100 cycles".

[0417] III. Test analysis results

[0418] The test results can be referred to Tables 4 and 5.

[0419] Examples 1-37 all set a filling area containing a positive electrode stabilizer in the positive electrode tab under overhang design, all have low internal resistance, low hydrogen sulfide production and good cycle performance.

[0420] Comparative Examples 1-7 all do not contain a filling area of a positive electrode stabilizer, wherein Comparative Example 1 does not use overhang design, Comparative Example 2 does not fill the overhang design blank area with material, Comparative Examples 3, 6-7 replace the positive electrode stabilizer with an insulating material, Comparative Example 4 replaces the positive electrode stabilizer with a first binder, and Comparative Example 5 replaces the positive electrode stabilizer with a water-stable solid electrolyte. It is found that the internal resistance of Comparative Examples 1-7 is significantly increased, the hydrogen sulfide production is significantly increased, and the cycle performance is all deteriorated to a certain extent.

[0421] Table 4.

[0422] Table 5.

[0423] The above description of the various embodiments tends to emphasize differences between the various embodiments, and the same or similar parts can be referred to each other, and for the sake of brevity, will not be described here.

[0424] The technical features of the above-described embodiments can be combined in any manner. For the sake of brevity, not all possible combinations of the technical features of the above-described embodiments are described, however, as long as the combination of the technical features does not contradict, it should be considered within the scope of the present specification.

[0425] It should be noted that the present application is not limited to the above-described embodiments. The above-described embodiments are merely examples, and embodiments having substantially the same configuration and playing the same role and effect as the technical idea within the scope of the technical solutions of the present application are all included in the technical scope of the present application. The above-described embodiments only express several embodiments of the present application, and the description is relatively detailed, but it should not be construed as limiting the scope of the patent. In addition, within the scope of the present application, various modifications that can be thought of by those skilled in the art, combinations of part of the components of the embodiments or other ways are also included in the scope of the present application.

Claims

1. A positive electrode tab, comprising a positive electrode current collector and an active film layer located on at least one side of the positive electrode current collector, wherein a thickness direction of the active film layer is defined as a longitudinal direction, and a direction perpendicular to the longitudinal direction is defined as a transverse direction; in the transverse direction, the active film layer comprises a positive electrode active region and a filling region located on at least a part of a periphery of the positive electrode active region; wherein the positive electrode active region comprises positive electrode active particles and a positive electrode solid electrolyte, the positive electrode solid electrolyte comprises a sulfide solid electrolyte; the filling region comprises a positive electrode stabilizer, the positive electrode stabilizer comprises at least one of a moisture absorbent and a hydrogen sulfide absorbent.

2. The cathode sheet of claim 1, wherein, the positive electrode stabilizer satisfies one or more of the following characteristics: a weight percentage of the positive electrode stabilizer in the filling region is 30wt%-99.5wt%; in the filling region, a mass ratio of the moisture absorbent to the hydrogen sulfide absorbent is 0-1; a weight percentage of the moisture absorbent in the filling region is 0wt%-99.5wt%; a weight percentage of the hydrogen sulfide absorbent in the filling region is 0wt%-99.5wt%.

3. The cathode sheet of claim 1 or 2, wherein, the positive electrode stabilizer satisfies one or more of the following characteristics: a weight percentage of the positive electrode stabilizer in the filling region is 45wt%-98wt%; in the filling region, a mass ratio of the moisture absorbent to the hydrogen sulfide absorbent is selected from 1:9 to 9:1; a weight percentage of the moisture absorbent in the filling region is 10wt%-90wt%, which can be 40wt%-60wt%; a weight percentage of the hydrogen sulfide absorbent in the filling region is 10wt%-90wt%, which can be 40wt%-60wt%.

4. The cathode sheet of any one of claims 1-3, wherein, the positive electrode stabilizer satisfies one or more of the following characteristics: the positive electrode stabilizer comprises the moisture absorbent, and the moisture absorbent comprises one or more of a physical moisture absorbent and a chemical moisture absorbent; the positive electrode stabilizer comprises the hydrogen sulfide absorbent, and the hydrogen sulfide absorbent comprises one or more of a hydrogen sulfide physical absorbent and a hydrogen sulfide chemical absorbent.

5. The cathode sheet of claim 4, wherein, the positive electrode stabilizer satisfies one or more of the following characteristics: the moisture absorbent comprises a physical moisture absorbent, and the physical moisture absorbent comprises one or more of a silica gel type, a molecular sieve type, a metal organic framework type, and a porous carbon type, wherein the porous carbon type comprises activated carbon; the moisture absorbent comprises a chemical moisture absorbent, and the chemical moisture absorbent comprises one or more of CaCl2, CaH2, anhydrous CuSO4, LiCl, FeCl3, FeO(OH), KMnO4, Na2CO3, Fe2O3, Fe(OH)3, ZnO, CuO, NiO, and Al2O; the hydrogen sulfide absorbent comprises a hydrogen sulfide physical absorbent, and the hydrogen sulfide physical absorbent comprises one or more of an activated carbon type, a molecular sieve type, and a metal organic framework type; the hydrogen sulfide absorbent comprises a hydrogen sulfide chemical absorbent, and the hydrogen sulfide chemical absorbent comprises one or more of Fe2O3, ZnO, Bi2O3, CuO, and MnO.

6. The cathode sheet of claim 4 or 5, wherein, The positive electrode stabilizer comprises a dual-absorbing agent, which refers to a substance that simultaneously functions as the moisture-absorbing agent and the hydrogen sulfide-absorbing agent; The dual-absorbing agent comprises one or more of a dual-physical absorbing agent and a dual-chemical absorbing agent; The dual-physical absorbing agent refers to a substance that simultaneously absorbs moisture and hydrogen sulfide based on physical action, and the dual-chemical absorbing agent refers to a substance that simultaneously absorbs moisture and hydrogen sulfide based on chemical action.

7. The cathode sheet of claim 6, wherein, The positive electrode stabilizer satisfies one or more of the following characteristics: The positive electrode stabilizer comprises the dual-physical absorbing agent, which comprises one or more of activated carbon, molecular sieves, and metal-organic frameworks; The positive electrode stabilizer comprises the dual-chemical absorbing agent, which comprises one or more of ZnO and CuO.

8. The cathode sheet of claim 6 or 7, wherein, The positive electrode stabilizer comprises the dual-chemical absorbing agent and the dual-physical absorbing agent, which comprises one or more of activated carbon and molecular sieves.

9. The cathode sheet of any one of claims 1-8, wherein, The filling region further comprises a first binder; the first binder comprises one or more of a rubber-based binder, carboxymethyl cellulose, a polyolefin-based binder, a polyurethane-based binder, a polyacrylate-based binder, a polyacrylic resin, polyvinylidene fluoride, polytetrafluoroethylene, a vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, a vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene terpolymer, and a tetrafluoroethylene-hexafluoropropylene copolymer; The rubber-based binder comprises at least one of a fluorinated rubber-based binder or a rubber-based binder without fluorine elements; The polyacrylate-based binder comprises at least one of a fluorine-containing acrylate resin or a polyacrylate-based binder without fluorine elements.

10. The cathode sheet of Claim 9, wherein, The first binder comprises one or more of styrene butadiene rubber, nitrile rubber, hydrogenated nitrile rubber, a polyacrylic resin, and a polyurethane-based binder.

11. The cathode sheet of claim 9 or 10, wherein, The weight percentage of the first binder in the filling region is 0.5wt% to 5wt%.

12. The cathode sheet of claim 9 or 10, wherein, The weight percentage of the first binder in the filling region is 2wt% to 4wt%.

13. The cathode sheet of any one of claims 9-12, wherein, The filling region comprises the first binder, and the positive electrode active region comprises a second binder; the first binder and the second binder are of the same type.

14. The cathode sheet of any one of claims 1-13, wherein, The filling region further comprises an insulating material.

15. The cathode sheet of Claim 14, wherein, The filling region satisfies one or more of the following characteristics: The insulating material comprises one or more of inorganic oxide insulating materials, boehmite, non-woven fabric fibers, and fibrous resins; optionally, the inorganic oxide insulating materials comprise one or more of Al2O3, MgO, SiO2, BaTiO3, BaCO3, Fe3O4, TiO2, Y2O3, Mn2O3, and Mn2O7; The weight percentage of the insulating material in the filling region is less than or equal to 69wt%; In the filling region, the mass ratio of the insulating material to the positive electrode stabilizer is less than or equal to 2.

16. The cathode sheet of Claim 15, wherein, The filling region satisfies one or more of the following characteristics: The weight percentage of the insulating material in the filling region is 1wt% to 50wt%; In the filling region, the mass ratio of the insulating material to the positive electrode stabilizer is 0.5 to 1.

17. The cathode sheet of any one of claims 1-16, wherein, The positive electrode active particle includes a positive electrode active body and a coating layer located on at least a part of the surface of the positive electrode active body, the positive electrode active body includes one or more of lithium transition metal oxide and lithium-containing phosphate, and the coating layer includes a lithium oxide compound.

18. The cathode sheet of Claim 17, wherein, The lithium oxide compound satisfies one or more of the following characteristics: The lithium oxide compound includes one or more of B, Nb, Zr, Si, P, Mn, Zn, Al, Fe and Na; The weight proportion of the lithium oxide compound in the positive electrode active particle is 0.1wt%-5wt%.

19. The cathode sheet of claim 17 or 18, wherein, The lithium oxide compound satisfies one or more of the following characteristics: The lithium oxide compound includes one or more of Li3BO3, LiNbO3, Li2ZrO3, Li2SiO3, LiPO3 and Li2MnO4; The weight proportion of the lithium oxide compound in the positive electrode active particle is 0.1wt%-2wt%.

20. The cathode sheet of any one of claims 1-19, wherein, The sulfide solid electrolyte includes at least one of a binary sulfide solid system and a ternary sulfide solid system; The binary sulfide solid system includes one or more of Li2S-P2S5, Li2S-SiS2, Li2S-GeS2 and Li2S-B2S3; The ternary sulfide solid system includes one or more of argyrodite-type sulfide electrolyte, Li2S-MeS2-P2S5 ternary sulfide electrolyte, lithium-germanium-phosphorus-sulfur type sulfide electrolyte, Li2S-P2S5-MS ternary sulfide electrolyte, Li2S-P2S5-MCl ternary sulfide electrolyte and thio-LISICON type sulfide electrolyte; wherein Me includes one or more of Si, Ge, Sn and Al; and M includes one or more of Ge, Al, Sn, Pb, Sb, Si and As.

21. The cathode sheet of any one of claims 1-20, wherein, The positive electrode stabilizer includes a moisture absorber, and the positive electrode solid electrolyte further includes a halide solid electrolyte; The halide solid electrolyte includes lithium element, halogen and X element, wherein the X element includes one or more of Y, In, Zr, Sc, Ho, Mn, Cd and Pb, and the halogen includes one or more of Cl, Br and I.

22. The cathode sheet of Claim 21, wherein, The halide solid electrolyte includes Li3X 1 Cl6, LiX 1 I4, LiX 1 I3 and Li3X 1 one or more of Br6, X in the halide solid electrolyte 1 includes one or more of Y, In, Sc, Ho, Mn, Cd, and Pb.

23. The cathode sheet of any one of claims 1-22, wherein, The positive electrode active region has a first side and a second side facing away from each other, and the first side and the second side respectively intersect with the transverse direction; The filling region is arranged outside the opposite regions of the first side and the second side, respectively.

24. The cathode sheet of Claim 23, wherein, The first side and the second side are completely covered by the filling region.

25. The cathode sheet of any one of claims 1-24, wherein, In the transverse direction, the positive electrode active region is completely surrounded by the filling region.

26. The cathode sheet of any one of claims 1-25, wherein, The width of the filling region at different positions along the outer side of the positive electrode active region is greater than or equal to 0.2mm in terms of the projection area of the filling region in the transverse direction.

27. The cathode sheet of Claim 25, wherein, The width of the filling region at different positions along the outer side of the positive electrode active region is 0.2mm-10mm, and optionally 0.5mm-10mm, in terms of the projection area of the filling region in the transverse direction.

28. The cathode sheet of any one of claims 1-27, wherein, The volume ratio of the filling region to the positive electrode active region is greater than or equal to 0.2%.

29. The cathode sheet of Claim 28, wherein, The volume ratio of the filling area to the positive active area is 0.2% to 20%, or 0.5% to 10%.

30. The cathode sheet of any one of claims 1-29, wherein, The thickness of the active film layer is equal at different lateral positions.

31. A solid-state battery comprising a positive electrode layer, a solid electrolyte layer, and a negative electrode layer, which are sequentially stacked, wherein The positive electrode layer comprises the positive electrode tab of any one of claims 1 to 30.

32. The solid-state battery of claim 31, wherein, The solid-state battery is a full solid-state battery.

33. The solid-state battery of claim 31 or 32, wherein, The projection areas of the positive electrode layer, the solid electrolyte layer and the negative electrode layer along the longitudinal direction are consistent.

34. An electrical device comprising the solid-state battery of any one of claims 31 to 33.

35. A method for preparing a solid-state battery, comprising the following steps: providing a substrate comprising a solid electrolyte layer and a negative electrode layer arranged in a stack, the negative electrode layer being located on one side of the solid electrolyte layer; compositing the positive electrode tab of any one of claims 1 to 30 on the side of the solid electrolyte layer away from the negative electrode layer to prepare a solid-state battery; Optionally, the solid-state battery is a full solid-state battery.

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