Method for preparing lithium metal-electrolyte composite structure, and lithium battery

Abstract

Disclosed is a method for preparing a lithium metal-electrolyte composite structure, comprising: providing a composite electrolyte dispersion, wherein a polymer and an oxide electrolyte are dispersed in the composite electrolyte dispersion; applying the composite electrolyte dispersion to the surface of a lithium metal sheet to form a liquid film on the surface of the lithium metal sheet; drying the liquid film to obtain a preformed composite structure; and performing rolling treatment on the preformed composite structure to obtain the lithium metal-electrolyte composite structure.

Description

Method for preparing lithium metal-electrolyte composite structure, lithium battery

[0001] Cross-reference to related applications

[0002] This application claims priority to Chinese Patent Application No. 202411348771.X, filed on September 26, 2024, the entire contents of which are incorporated herein by reference. TECHNICAL FIELD

[0003] The present disclosure relates to the field of new energy, and particularly relates to a method for preparing a lithium metal-electrolyte composite structure and a lithium battery. BACKGROUND

[0004] Solid-state batteries with high energy density and safety are ideal candidates for next-generation energy storage applications, promising to break through the technical bottlenecks of liquid lithium-ion batteries, achieving higher energy density, longer cycle life, and better safety performance. In addition, solid-state batteries can introduce a higher specific capacity lithium metal anode, with a theoretical specific capacity of 3680 mAh / g, much higher than the theoretical specific capacity of 372 mAh / g of carbon-based graphite material anodes, which is beneficial to improve the energy density of solid-state batteries. However, due to the high activity and soft texture of lithium metal, it is difficult to process it into thin and regular lithium foils like traditional electrode sheets through mechanical methods. The current production process of thin film lithium metal anodes mainly includes hot melting method, composite metal method and electrodeposition method. However, the hot melting method has high energy consumption, the composite metal method is prone to alloy segregation and has poor interface contact, and the electrodeposition method requires high precision control of process parameters and takes a long time, making it difficult to mass-produce. The production process of thin film lithium metal anodes still needs to be improved. SUMMARY

[0005] By using the method for preparing a lithium metal-electrolyte composite structure and the lithium battery of one or more embodiments of the present disclosure, the technical problems of high energy consumption, easy alloy segregation and poor interface contact in the production process of thin film lithium metal anodes are solved.

[0006] In a first aspect, the present disclosure provides a method for preparing a lithium metal-electrolyte composite structure, comprising the following steps: providing a composite electrolyte dispersion liquid, the composite electrolyte solution being dispersed with a polymer and an oxide electrolyte; coating the composite electrolyte dispersion liquid to the surface of a lithium metal sheet to form a liquid film on the surface of the lithium metal sheet; drying the liquid film to obtain a pre-prepared composite structure; and rolling the pre-prepared composite structure to obtain a lithium metal-electrolyte composite structure.

[0007] In a second aspect, the present disclosure provides a lithium battery comprising the lithium metal-electrolyte composite structure prepared by the method of any one of the first aspect. BRIEF DESCRIPTION OF DRAWINGS

[0008] The accompanying drawings, which are incorporated herein and form a part of the specification, illustrate the embodiments consistent with the present disclosure and, together with the description, further serve to explain the principles of the present disclosure.

[0009] In order to more clearly illustrate the technical solutions in the embodiments of the present disclosure or the related art, the accompanying drawings needed to be used in the embodiments or the related art description will be briefly introduced. Obviously, for those of ordinary skill in the art, other drawings can also be obtained without creative labor based on these drawings.

[0010] FIG. 1 shows a flowchart of a method for preparing a lithium metal-electrolyte composite structure according to some embodiments of the present disclosure. Embodiments of the present disclosure

[0011] In order to make the objects, technical solutions and advantages of the embodiments of the present disclosure clearer, the technical solutions in the embodiments of the present disclosure will be described clearly and completely below with reference to the drawings in the embodiments of the present disclosure. Obviously, the described embodiments are only some of the embodiments of the present disclosure, rather than all the embodiments. Based on the embodiments in the present disclosure, all other embodiments obtained by those of ordinary skill in the art without creative labor fall within the scope of protection of the present disclosure.

[0012] Unless otherwise specifically defined, the terms used herein are understood as having the meanings commonly used in the art. Therefore, unless otherwise defined, all technical and scientific terms used herein have the same meanings as generally understood by those skilled in the art to which the present disclosure belongs. If there is a contradiction, the present specification takes precedence.

[0013] Unless otherwise specifically stated, the various raw materials, reagents, instruments and equipment used in the present disclosure can be purchased from the market or can be prepared by existing methods.

[0014] The existing production process of thin film type lithium metal negative electrode has the technical problems of high energy consumption, easy alloy segregation and poor interface contact, which leads to the need for improvement of the production process of thin film type lithium metal negative electrode.

[0015] The technical solutions provided by the embodiments of the present disclosure are to solve the above technical problems, and the general idea is as follows.

[0016] FIG. 1 shows a flowchart of a method for preparing a lithium metal-electrolyte composite structure according to some embodiments of the present disclosure. In a first aspect, as shown in FIG. 1, the present disclosure provides a method for preparing a lithium metal-electrolyte composite structure, comprising the following steps:

[0017] S1: providing a composite electrolyte dispersion liquid, the composite electrolyte solution containing a polymer and an oxide electrolyte;

[0018] S2: coating the composite electrolyte dispersion liquid onto the surface of a lithium metal sheet to form a liquid film on the surface of the lithium metal sheet;

[0019] S3: drying the liquid film to obtain a pre-prepared composite structure; and

[0020] S4: roll-pressing the pre-prepared composite structure to obtain a lithium metal-electrolyte composite structure.

[0021] It is easy to understand that lithium is a relatively soft metal, which has small deformation resistance, strong ductility, and active properties. During the processing of lithium foil, stress concentration is prone to occur, which leads to irregular shape of the lithium foil, local wrinkles, and adhesion defects.

[0022] The composite electrolyte dispersion liquid provided in the embodiments of the present disclosure contains a polymer and an oxide electrolyte. After the composite electrolyte dispersion liquid is coated onto the surface of the lithium metal sheet, a liquid film can be formed on the surface of the lithium metal sheet. After drying, the liquid film forms an electrolyte pre-prepared film with certain toughness and softness. The electrolyte pre-prepared film is attached to the surface of the lithium metal sheet, so that the stress received by the lithium metal sheet during the roll-pressing process can be easily dispersed through the electrolyte pre-prepared film. In addition, the interface friction between the electrolyte pre-prepared film and the surface of the lithium metal sheet is small, which makes the lithium metal sheet not prone to local wrinkles and adhesion during the roll-pressing process.

[0023] In addition, the electrolyte pre-prepared film and the lithium metal sheet can be in closer contact during the roll-pressing process.

[0024] In some embodiments of the present disclosure, the polymer is at least one of polyvinylidene fluoride, polymethyl methacrylate, poly(vinylidene fluoride-co-hexafluoropropylene), polyimide, and aramid.

[0025] It is easy to understand that the above-mentioned polymers all have good toughness and film-forming properties, and can be easily purchased on the market, and have high applicability in the present disclosure.

[0026] In some embodiments of the present disclosure, the oxide electrolyte is at least one of lithium aluminum titanium phosphate, lithium lanthanum zirconium oxide, and lithium lanthanum zirconium titanium oxide.

[0027] It is easy to understand that the lithium titanium aluminum phosphate, lithium lanthanum zirconium oxide and lithium lanthanum titanium zirconium oxide all have good gel-forming performance, high electrical conductivity and strong stability, and are easy to be purchased from the market, and have high applicability in the present disclosure.

[0028] In some embodiments of the present disclosure, the particle size of the oxide electrolyte is 0.4 µm ~2.0 µm.

[0029] The beneficial effect of the particle size of the oxide electrolyte being 0.4 µm ~2.0 µm is that both the oxide electrolyte and the polymer can be uniformly mixed, and the electrolyte preform film formed after drying of the liquid film has high ionic conductivity, and the oxide electrolyte is not too small in particle size to cause high difficulty in preparation.

[0030] For example, the particle size of the oxide electrolyte can be 0.4 µm, 0.8 µm, 1.2 µm, 1.6 µm, 2.0 µm.

[0031] In some embodiments of the present disclosure, the weight percentage of the polymer in the composite electrolyte dispersion liquid is 1%~10%; and / or, the weight percentage of the oxide electrolyte in the composite electrolyte dispersion liquid is 20%~40%.

[0032] It is easy to understand that the beneficial effect of the weight percentage of the polymer being 1%~10% is that the polymer can be relatively uniformly dispersed in the composite electrolyte dispersion liquid, and the electrolyte preform film formed after drying of the liquid film has good moldability and toughness.

[0033] It is easy to understand that the beneficial effect of the weight percentage of the oxide electrolyte being 20%~40% is that the oxide electrolyte can be relatively uniformly dispersed in the composite electrolyte dispersion liquid, and the electrolyte preform film formed after drying of the liquid film has high electrical conductivity.

[0034] In some embodiments of the present disclosure, the thickness of the liquid film is 2 µm~5 µm.

[0035] The beneficial effect of the thickness of the liquid film being 2 µm ~5 µm is that the electrolyte preform film formed after drying of the liquid film has a suitable thickness, and when the preform composite structure is subjected to rolling treatment, the electrolyte preform film can both play a sufficient buffering role on the lithium metal sheet subjected to rolling treatment and make the lithium metal sheet be fully rolled.

[0036] For example, the thickness of the liquid film can be 2 µm, 3 µm, 4 µm, 5 µm.

[0037] In some embodiments of the present disclosure, the pressure of the rolling treatment is 1 MPa-6 MPa, the speed of the rolling treatment is 0.1 m / s-3 m / s, the time of the rolling treatment is 0.1 h-5 h, and the temperature of the rolling treatment is 25℃-100℃.

[0038] In some embodiments of the present disclosure, the thickness of the lithium metal sheet is 50 µm-60 µm.

[0039] The thickness of the lithium metal sheet is 50 µm-60 µm, which is beneficial to make the thickness of the lithium metal-electrolyte composite structure within a preset range after the rolling treatment of the pre-prepared composite structure, and to ensure that the lithium metal sheet forms a regular lithium foil shape after the rolling treatment, avoiding defects such as local wrinkles and adhesion.

[0040] In some embodiments of the present disclosure, the thickness of the lithium metal-electrolyte composite structure is 20 µm-30 µm.

[0041] The thickness of the lithium metal-electrolyte composite structure is 20 µm-30 µm, which is beneficial to make the lithium metal-electrolyte composite structure have sufficient flexibility, and to make the thickness of the lithium metal in the lithium metal-electrolyte composite structure also easy to maintain a uniform thickness.

[0042] For example, the thickness of the lithium metal-electrolyte composite structure is 20 µm, 22 µm, 24 µm, 26 µm, 28 µm, or 30 µm.

[0043] In a second aspect, the embodiments of the present disclosure provide a lithium battery, which comprises the lithium metal-electrolyte composite structure prepared by the preparation method of the lithium metal-electrolyte composite structure according to any one of the embodiments of the first aspect.

[0044] It is easy to understand that the lithium metal-electrolyte composite structure can act as a negative electrode and an electrolyte structure in a lithium battery.

[0045] The lithium battery is realized based on the lithium metal-electrolyte composite structure prepared by the preparation method of the lithium metal-electrolyte composite structure according to any one of the embodiments of the first aspect, and the specific embodiments of the lithium battery can refer to the above-mentioned embodiments and the common knowledge in the art. Since the lithium battery adopts part or all of the technical solutions of the above-mentioned embodiments, it at least has all the beneficial effects brought by the technical solutions of the above-mentioned embodiments, which will not be repeated here.

[0046] The present disclosure is further described below with reference to specific examples. It should be understood that these examples are intended to illustrate the present disclosure and are not intended to limit the scope of the present disclosure. The experimental methods in the following examples, unless otherwise specified, are generally determined according to the industry standards. If there is no corresponding industry standard, it is determined according to the general international standards, conventional conditions, or according to the conditions recommended by the manufacturer.

[0047] Example 1

[0048] The preparation method of the lithium metal-electrolyte composite structure provided in this example comprises the following steps:

[0049] S1: preparing a composite electrolyte dispersion liquid by using N-methyl pyrrolidone as a solvent and a polymer and an oxide electrolyte as solutes;

[0050] S2: coating the composite electrolyte dispersion liquid to the two side surfaces of the lithium metal sheet to form liquid films with a thickness of 3 µm on the two side surfaces of the lithium metal sheet, respectively;

[0051] S3: performing drying treatment on the liquid films to obtain a pre-prepared composite structure; and

[0052] S4: performing roll pressing treatment on the pre-prepared composite structure to obtain a lithium metal-electrolyte composite structure.

[0053] The polymer is poly(vinylidene fluoride-co-hexafluoropropylene). The oxide electrolyte is lithium aluminum titanium phosphate. The particle size of the oxide electrolyte is 1 µm. The weight percentage of the polymer in the composite electrolyte dispersion liquid is 2%. The weight percentage of the oxide electrolyte in the composite electrolyte dispersion liquid is 10%. The pressure of the roll pressing treatment is 1.5 MPa. The speed of the roll pressing treatment is 0.5 m / s. The time of the roll pressing treatment is 0.1 h. The temperature of the roll pressing treatment is 50°C.

[0054] The thickness of the lithium metal sheet is 50 µm.

[0055] The thickness of the prepared lithium metal-electrolyte composite structure is 25 µm.

[0056] Example 2

[0057] The preparation method of the lithium metal-electrolyte composite structure provided in this example comprises the following steps:

[0058] S1: preparing a composite electrolyte dispersion liquid by using N-methyl pyrrolidone as a solvent and a polymer and an oxide electrolyte as solutes;

[0059] S2: coating the composite electrolyte dispersion liquid to the two side surfaces of the lithium metal sheet to form liquid films with a thickness of 3 µm on the two side surfaces of the lithium metal sheet, respectively;

[0060] S3: drying the liquid film to obtain a pre-prepared composite structure; and

[0061] S4: roll-pressing the pre-prepared composite structure to obtain a lithium metal-electrolyte composite structure.

[0062] The polymer is poly(vinylidene fluoride-co-hexafluoropropylene). The oxide electrolyte is lithium aluminum titanium phosphate. The particle size of the oxide electrolyte is 1 µm. The weight percentage of the polymer in the composite electrolyte dispersion is 2%. The weight percentage of the oxide electrolyte in the composite electrolyte dispersion is 20%. The pressure of the roll-pressing is 1.5 MPa. The speed of the roll-pressing is 0.5 m / s. The time of the roll-pressing is 0.1 h. The temperature of the roll-pressing is 50℃.

[0063] The thickness of the lithium metal sheet is 50 µm.

[0064] The thickness of the prepared lithium metal-electrolyte composite structure is 26 µm.

[0065] Example 3

[0066] The present example provides a method for preparing a lithium metal-electrolyte composite structure, comprising the following steps:

[0067] S1: preparing a composite electrolyte dispersion by using N-methylpyrrolidone as a solvent and a polymer and an oxide electrolyte as solutes;

[0068] S2: coating the composite electrolyte dispersion to both sides of a lithium metal sheet to form a 3 µm-thick liquid film on both sides of the lithium metal sheet, respectively;

[0069] S3: drying the liquid film to obtain a pre-prepared composite structure; and

[0070] S4: roll-pressing the pre-prepared composite structure to obtain a lithium metal-electrolyte composite structure.

[0071] The polymer is poly(vinylidene fluoride-co-hexafluoropropylene). The oxide electrolyte is lithium aluminum titanium phosphate. The particle size of the oxide electrolyte is 1 µm. The weight percentage of the polymer in the composite electrolyte dispersion is 2%. The weight percentage of the oxide electrolyte in the composite electrolyte dispersion is 30%. The pressure of the roll-pressing is 1.5 MPa. The speed of the roll-pressing is 0.5 m / s. The time of the roll-pressing is 0.1 h. The temperature of the roll-pressing is 50℃. The thickness of the lithium metal sheet is 50 µm. The thickness of the prepared lithium metal-electrolyte composite structure is 27 µm.

[0072] Example 4

[0073] The embodiment provides a preparation method of a lithium metal-electrolyte composite structure, and the method comprises the following steps:

[0074] S1: preparing a composite electrolyte dispersion liquid by taking N-methyl pyrrolidone as a solvent and taking a polymer and an oxide electrolyte as solutes;

[0075] S2: coating the composite electrolyte dispersion liquid to two side surfaces of a lithium metal sheet to form liquid films with a thickness of 3 µm on the two side surfaces of the lithium metal sheet respectively;

[0076] S3: performing drying treatment on the liquid films to obtain a prefabricated composite structure; and

[0077] S4: performing roll pressing treatment on the prefabricated composite structure to obtain the lithium metal-electrolyte composite structure.

[0078] In the embodiment, the polymer is poly(vinylidene fluoride-co-hexafluoropropylene), the oxide electrolyte is lithium aluminum titanium phosphate, the particle size of the oxide electrolyte is 1 µm, the weight percentage of the polymer in the composite electrolyte dispersion liquid is 2%, the weight percentage of the oxide electrolyte in the composite electrolyte dispersion liquid is 20% to 40%, the pressure of the roll pressing treatment is 1.5 MPa, the speed of the roll pressing treatment is 0.5 m / s, the time of the roll pressing treatment is 0.1 h, the temperature of the roll pressing treatment is 50°C, the thickness of the lithium metal sheet is 50 µm, and the thickness of the prepared lithium metal-electrolyte composite structure is 29 µm.

[0079] Embodiment 5

[0080] The embodiment is different from the embodiment 1 only in that in the step S2, the composite electrolyte dispersion liquid is coated to one side surface of the lithium metal sheet.

[0081] Specifically as follows:

[0082] The embodiment provides a preparation method of a lithium metal-electrolyte composite structure, and the method comprises the following steps:

[0083] S1: preparing a composite electrolyte dispersion liquid by taking N-methyl pyrrolidone as a solvent and taking a polymer and an oxide electrolyte as solutes;

[0084] S2: coating the composite electrolyte dispersion liquid to one side surface of a lithium metal sheet to form a liquid film with a thickness of 3 µm on the one side surface of the lithium metal sheet;

[0085] S3: performing drying treatment on the liquid film to obtain a prefabricated composite structure; and

[0086] S4: performing roll pressing treatment on the prefabricated composite structure to obtain the lithium metal-electrolyte composite structure.

[0087] The polymer is poly(vinylidene fluoride-co-hexafluoropropylene). The oxide electrolyte is lithium aluminum titanium phosphate. The particle size of the oxide electrolyte is 1 µm. The weight percentage of the polymer in the composite electrolyte dispersion is 2%. The weight percentage of the oxide electrolyte in the composite electrolyte dispersion is 10%. The pressure of the rolling treatment is 1.5 MPa. The speed of the rolling treatment is 0.5 m / s. The time of the rolling treatment is 0.1 h. The temperature of the rolling treatment is 50℃. The thickness of the lithium metal sheet is 50 µm. The thickness of the prepared lithium metal-electrolyte composite structure is 23 µm.

[0088] Related experiments and effect data:

[0089] The lithium metal-electrolyte composite structure prepared in Examples 1-5 is tested as a lithium battery anode. The specific test method is as follows:

[0090] The thickness of the lithium metal-electrolyte composite structure is measured by a micrometer;

[0091] The lithium metal-electrolyte composite structure and the stainless steel sheet are combined into a symmetrical battery. The ionic conductivity of the symmetrical battery is measured by an alternating current impedance spectrum method;

[0092] The lithium metal-electrolyte composite structure and the commercial lithium sheet are combined into a symmetrical battery. When the current density is 1 mA / cm 2 , the cycle capacity is 1 mAh / cm 2 , and the symmetrical battery is recorded at a stable polarization voltage after 50 cycles.

[0093] The ionic conductivity and polarization voltage obtained by testing are shown in Table 1.

[0094] Table 1: Test results of ionic conductivity and polarization voltage of Examples 1-5

[0095]

[0096] Examples 1-4 strictly control the variables, and only the content of the oxide electrolyte is different. As can be seen from Table 1, as the content of the oxide electrolyte increases, the thickness of the lithium metal-electrolyte composite structure and the ionic conductivity increase, and the polarization voltage decreases, which indicates that under the conditions of Examples 1-4, increasing the content of the oxide electrolyte is beneficial to increasing the ionic conductivity of the lithium metal-electrolyte composite structure and the diffusion ability of ions from the lithium metal surface to the electrolyte. The difference between Example 5 and Example 1 is only that Example 5 only coats a single layer of liquid film. The ionic conductivity and polarization voltage decrease relative to Example 1. Overall, the technical solution of coating only a single layer of liquid film has a decrease in the ionic conductivity of the lithium metal-electrolyte composite structure compared to the technical solution of coating on both sides.

[0097] Compared with related technologies, the preparation method of the lithium metal-electrolyte composite structure provided in the embodiments of the present disclosure has the following advantages.

[0098] The preparation method of the lithium metal-electrolyte composite structure provided in the embodiments of the present disclosure includes the following steps: preparing a composite electrolyte dispersion liquid containing a polymer and an oxide electrolyte; and coating the composite electrolyte dispersion liquid onto a surface of a lithium metal sheet to form a liquid film on the surface of the lithium metal sheet. After drying, the liquid film forms an electrolyte preformed film with toughness and relatively softness, which can easily disperse the stress of the lithium metal sheet in the rolling process. In addition, the interface friction between the electrolyte preformed film and the surface of the lithium metal sheet is small, which can prevent the lithium metal sheet from being easily locally wrinkled and adhered in the rolling process.

[0099] Various embodiments of the present disclosure can exist in the form of a range; it should be understood that the description in the form of a range is merely for the convenience and brevity, and should not be understood as a hard limit on the scope of the present disclosure; therefore, it should be considered that all possible sub-ranges and single values within the range have been specifically disclosed. For example, it should be considered that the range description from 1 to 6 has specifically disclosed sub-ranges, such as from 1 to 3, from 1 to 4, from 1 to 5, from 2 to 4, from 2 to 6, from 3 to 6, etc., as well as single numbers within the range, such as 1, 2, 3, 4, 5 and 6, which applies to any range. In addition, whenever a numerical range is indicated herein, it refers to any cited number (fraction or integer) within the indicated range.

[0100] In the present disclosure, the orientation words such as "upper" and "lower" are specifically the directions of the drawing surface in the drawings unless otherwise stated. In addition, in the description of the present disclosure, the terms "comprise", "contain" and the like mean "including but not limited to". Moreover, the terms "comprise", "contain" or any other variant thereof are intended to cover non-exclusive inclusion, so that a process, method, article or device including a series of elements not only includes those elements, but also includes other elements not explicitly listed or inherent to such a process, method, article or device. Without more limitations, the elements defined by the statement "comprise" do not exclude the presence of other identical elements in the process, method, article or device including the elements. In this paper, the relationship terms such as "first" and "second" are only used to distinguish one entity or operation from another entity or operation, and do not necessarily require or imply any such actual relationship or order between the entities or operations. In this paper, the "and / or" describes the association relationship of the associated objects, which means that there can be three relationships, for example, A and / or B can represent the following cases: A exists alone, A and B exist together, and B exists alone. For the association relationship of more than three associated objects described by "and / or", it means that any one of the three associated objects can exist alone, or any at least two of them exist together, for example, for A, and / or B, and / or C, it means that any one of A, B and C exists alone, or any two of them exist together, or all three of them exist together. In this paper, "at least one" means one or more, and "multiple" means two or more. "At least one", "at least one of the following" or similar expressions mean any combination of these items, including any combination of single or multiple items. For example, "at least one of a, b, or c", or "at least one of a, b, and c", can mean a, b, c, a-b (i.e. a and b), a-c, b-c, or a-b-c, where a, b, and c can be single or multiple.

[0101] The above description is only a specific embodiment of the present disclosure, which enables those skilled in the art to understand or implement the present disclosure. Various modifications of these embodiments will be apparent to those skilled in the art, and the general principles defined herein can be implemented in other embodiments without departing from the spirit or scope of the present disclosure. Therefore, the present disclosure will not be limited to these embodiments shown herein, but will conform to the widest scope consistent with the principles and novel features disclosed herein.

Claims

1. A method for preparing a lithium metal-electrolyte composite structure, comprising the following steps: providing a composite electrolyte dispersion solution, wherein a polymer and an oxide electrolyte are dispersed in the composite electrolyte solution; coating the composite electrolyte dispersion solution to a surface of a lithium metal sheet to form a liquid film on the surface of the lithium metal sheet; performing a drying treatment on the liquid film to obtain a pre-prepared composite structure; and performing a rolling treatment on the pre-prepared composite structure to obtain the lithium metal-electrolyte composite structure.

2. The method of preparing a lithium metal-electrolyte composite structure according to claim 1, wherein, The polymer is at least one of polyvinylidene fluoride, polymethyl methacrylate, poly (vinylidene fluoride-co-hexafluoropropylene), polyimide and aramid.

3. The method of preparing a lithium metal-electrolyte composite structure according to claim 1, wherein, The oxide electrolyte is at least one of lithium aluminum titanium phosphate, lithium lanthanum zirconium oxide and lithium lanthanum zirconium titanium oxide.

4. The method of preparing a lithium metal-electrolyte composite structure according to claim 1, wherein, The particle size of the oxide electrolyte is 0.4 µm ~ 2.0 µm.

5. The method of producing a lithium metal-electrolyte composite structure according to claim 1, wherein, The weight percentage of the polymer in the composite electrolyte dispersion solution is 1% ~ 10%; and / or The weight percentage of the oxide electrolyte in the composite electrolyte dispersion solution is 20% ~ 40%.

6. The method of preparing a lithium metal-electrolyte composite structure according to claim 1, wherein, The thickness of the liquid film is 2 µm ~ 5 µm.

7. The method of producing a lithium metal-electrolyte composite structure according to claim 1, wherein, The pressure of the rolling treatment is 1 MPa ~ 6 MPa, the speed of the rolling treatment is 0.1 m / s ~ 3.0 m / s, the time of the rolling treatment is 0.1 h ~ 5.0 h, and the temperature of the rolling treatment is 25℃ ~ 100℃.

8. The method of producing a lithium metal-electrolyte composite structure according to claim 1, wherein, The thickness of the lithium metal sheet is 50 µm ~ 60 µm.

9. The method of producing a lithium metal-electrolyte composite structure according to any one of claims 1 to 8, wherein, The thickness of the lithium metal-electrolyte composite structure is 20 µm ~ 30 µm. 10.A lithium battery comprising the lithium metal-electrolyte composite structure prepared by the method for preparing a lithium metal-electrolyte composite structure according to any one of claims 1 ~ 9.

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