Method for constructing three-dimensional structure interface of all-solid-state lithium metal battery negative electrode and application thereof

Abstract

The application relates to a construction method and application of a full-solid-state lithium metal battery negative electrode three-dimensional structure interface, and comprises the following steps: a micro-nano scale coating preparation technology is used to accurately construct a three-dimensional structure lithiumophilic coating on a solid electrolyte surface, molten lithium is fully contacted with the lithiumophilic coating through intercalation, conversion, alloying and other lithiation reactions, so that a three-dimensional structure solid-solid interface with close contact is formed between the solid electrolyte and the lithium metal, and the three-dimensional structure solid-solid interface is matched with a high-capacity positive electrode and applied to a full-solid-state lithium metal battery. The application accurately controls the structure and components of the negative electrode interface in the micro-nano scale, solves the problem of poor solid-solid interface contact, significantly reduces the interface impedance, improves the uniformity of the electric field distribution and the lithium ion diffusion rate, inhibits the formation and growth of lithium dendrites, buffers the volume change of lithium metal deposition / peeling, enhances the stability of the interface structure, and realizes stable circulation under the conditions of a large current density and a high capacity.

Description

Technical Field

[0001] This invention belongs to the field of energy storage battery material technology, and in particular relates to a method for preparing and applying a solid-solid interface for the negative electrode of an all-solid lithium metal battery. Background Technology

[0002] With the rapid development of portable electronic devices, electric vehicles, and energy storage technologies, traditional lithium-ion batteries can no longer meet the urgent market demands. Their capacity and safety issues have driven the development of solid-state batteries. All-solid-state lithium batteries utilize solid electrolytes that can replace flammable organic electrolytes, offering extremely high safety. Furthermore, they combine lithium metal anodes and high-capacity cathodes to create all-solid-state lithium metal batteries, meeting the future demand for higher energy density in new energy development. Therefore, they are considered a crucial direction for the next generation of energy storage batteries. In recent years, significant progress has been made in the research of all-solid-state lithium batteries, developing inorganic solid electrolytes represented by oxides and sulfides, and polymer solid electrolytes represented by polyethylene oxide. However, the solid-solid interface between the solid electrolyte and the lithium metal anode is not uniform. Poor contact between the two leads to uneven current distribution and localized lithium deposition, which can cause high polarization or promote the formation and penetration of lithium dendrites into the solid electrolyte, resulting in a short circuit. In addition, during high current density and high-capacity stripping processes, the lack of timely replenishment of lithium at the interface can easily lead to the formation of interface voids or gaps, causing a rapid increase in battery impedance and shortening battery cycle life. The above problems seriously hinder the practical application of all-solid-state lithium metal batteries. Summary of the Invention

[0003] To address the aforementioned technical problems, this invention provides a method for constructing and applying a three-dimensional structural interface for the negative electrode of an all-solid-state lithium metal battery.

[0004] The technical solution adopted in this invention is: a method for constructing a three-dimensional structure interface of the negative electrode of an all-solid-state lithium metal battery. It adopts a micro-nano scale coating preparation technology that combines vapor deposition and micro-spraying to accurately prepare a lithiophilic coating with a three-dimensional structure on the surface of a solid electrolyte. The molten lithium is brought into full contact with the lithiophilic coating through a lithiation reaction, thereby forming a tightly contacted solid-solid interface between the solid electrolyte and the lithium metal.

[0005] Preferably, the specific steps are as follows:

[0006] Step 1: Deposit lithiophilic materials on the surface of structural materials using vapor deposition technology to form nanoscale lithiophilic structural materials;

[0007] Step 2: Using micro-spraying technology, the structural material with the modified lithiophilic layer is sprayed onto the surface of the solid electrolyte to form a three-dimensional lithiophilic coating at the micron scale;

[0008] Step 3: Completely wet the three-dimensional lithium-loving coating on the surface of the solid electrolyte with molten lithium. After cooling, a tight solid-solid interface is formed between the solid electrolyte and the lithium metal.

[0009] Preferably, the vapor deposition technology includes one or more combinations of atomic layer deposition, molecular layer deposition, or chemical vapor deposition; the micro-spraying technology includes one or more combinations of ultrasonic spraying, gas atomization spraying, or electrostatic spraying.

[0010] Preferably, molten lithium is brought into full contact with the lithiophilic coating by intercalation, conversion, or alloying methods.

[0011] Preferably, the solid electrolyte comprises one or more combinations of polymers, chlorides, sulfides, and oxides.

[0012] Preferably, the solid electrolyte is a perovskite oxide electrolyte, a garnet oxide electrolyte, or a polyoxyethylene polymer electrolyte.

[0013] Preferably, the structural material is one or more of the following: single-walled carbon nanotube oxide, multi-walled carbon nanotube oxide, graphite oxide, graphene oxide, graphdiyne oxide, carbon black oxide powder, zinc oxide, tin oxide, indium oxide, magnesium oxide, zirconium oxide, niobium oxide, tantalum oxide, aluminum oxide, lithium oxide powder, copper, aluminum, silver, iron, nickel, tantalum, magnesium, tin, zinc powder, garnet oxide, lithium nitride, and lithium fluoride powder; the diameter of the structural material powder particles is 0.1 μm–10 μm.

[0014] Preferably, the lithiophilic material includes one or more combinations of zinc oxide, magnesium oxide, indium oxide, tin oxide, titanium oxide, molybdenum oxide, lithium-rich organic thin films, zinc-rich organic thin films, aluminum-rich organic thin films, titanium-rich organic thin films, tin sulfide, zinc sulfide, molybdenum sulfide, rhodium, platinum, palladium, ruthenium, gold, and silver.

[0015] Preferably, the thickness of the lithiophilic modified coating is 1 nm–200 nm; the thickness of the three-dimensional structure coating is 0.5 μm–50 μm.

[0016] Preferably, the contact time between molten lithium and the three-dimensional lithium-loving coating is 1–60 min, the melting temperature is 181–350 °C, and the lithium metal thickness is 0.01 mm–2 mm.

[0017] A solid-state lithium metal battery is obtained by first constructing a composite structure of a solid electrolyte and a lithium metal anode according to the construction method of the three-dimensional structure interface of the anode of a solid-state lithium metal battery, and then combining it with a high-capacity cathode to obtain a solid-state lithium metal battery.

[0018] Preferably, the cathode material includes one or more combinations of lithium cobalt oxide, lithium iron phosphate, lithium manganese oxide, lithium nickel cobalt manganese oxide, and lithium nickel cobalt aluminum oxide.

[0019] The advantages and positive effects of this invention are: it precisely controls the structure and composition of the negative electrode solid-solid interface at the micro-nano scale, solves the problem of poor solid-solid interface contact, significantly reduces interface impedance, improves the uniformity of electric field distribution and lithium ion diffusion rate, inhibits the formation and growth of lithium dendrites, buffers the volume change of lithium metal deposition / stripping, enhances the stability of the interface structure, and achieves stable cycling under high current density and high capacity conditions.

[0020] This method is simple to operate, has universal applicability, can be applied to different battery fields and industries, and is easy to modify existing mature production lines, making it easy to promote. Attached Figure Description

[0021] Figure 1 This is a SEM image of the solid electrolyte surface after ultrasonic spraying and atomic layer deposition in Example 1;

[0022] Figure 2 The images shown are SEM and EDS images of the cross-section of the solid electrolyte after ultrasonic spraying and atomic layer deposition in Example 1.

[0023] Figure 3 This is the solid electrolyte morphology after wetting with molten lithium in Example 1;

[0024] Figure 4 This is a SEM image of the cross-section of molten lithium after contact with a solid electrolyte in Example 1;

[0025] Figure 5 The symmetric cell prepared in Example 1 operates at a current density of 0.5 mA / cm². -2 Capacity 0.25 mAh / cm³ -2 The potential-time curve measured under the given conditions;

[0026] Figure 6 The full cell prepared in Example 1 has a current density of 0.5 mA / cm² at the negative electrode surface. -2 The specific capacity and coulomb efficiency of the cycle are as follows;

[0027] Figure 7 This is a SEM image of the solid electrolyte surface after ultrasonic spraying and atomic layer deposition in Example 2;

[0028] Figure 8 The symmetric cell prepared for Comparative Example 1 was used at a current density of 0.5 mA / cm². -2 Capacity 0.25 mAh / cm³ -2 The potential-time curve measured under the given conditions;

[0029] Figure 9 The symmetric cell prepared for Comparative Example 2 was used at a current density of 0.5 mA / cm². -2 Capacity 0.25 mAh / cm³ -2 The potential-time curve was measured under the specified conditions. Detailed Implementation

[0030] The embodiments of the present invention will now be described with reference to the accompanying drawings.

[0031] This invention relates to a method for constructing and applying a three-dimensional structural interface for the negative electrode of an all-solid-state lithium metal battery. Specifically, it relates to a method for constructing a tightly contacting solid-solid interface and a method for precisely controlling the solid-solid interface. During construction, a three-dimensional lithiophilic coating is first formed on the surface of a solid electrolyte using micro-nano scale coating preparation techniques such as vapor deposition and micro-spraying. Then, molten lithium is used to wet the three-dimensional lithiophilic coating through lithiation reactions such as intercalation, conversion, and alloying, thereby forming a tightly contacting solid-solid interface on the solid electrolyte surface. Furthermore, during the construction process, the lithium affinity, lithium-ion conductivity, electronic conductivity, and lithium-ion diffusion coefficient of the solid electrolyte-lithium metal negative electrode interface can be precisely controlled by adjusting the thickness of the micron-sized three-dimensional coating and the thickness of the surface nano-lithhiophilic coating, thereby further constructing a high-performance all-solid-state lithium metal battery. By constructing a three-dimensional hybrid ion-electron conductive interface between the solid electrolyte and the lithium metal negative electrode, the solid-solid interface contact problem existing in solid-state batteries is solved.

[0032] When constructing a three-dimensional lithiophilic interface for a solid electrolyte, firstly, a lithiophilic material is deposited on the surface of a structural material using vapor deposition technology to form a nanoscale lithiophilic structural material; then, a micro-spraying technique is used to spray the modified lithiophilic structural material onto the surface of the solid electrolyte to form a micron-scale three-dimensional lithiophilic coating; next, the three-dimensional lithiophilic coating on the surface of the solid electrolyte is brought into close contact with molten lithium to prepare a three-dimensional mixed ion-electron conductive interface for the solid electrolyte; finally, the combined solid electrolyte / lithium metal anode is matched with a high-capacity cathode to form an all-solid-state lithium metal battery.

[0033] The construction method and application of the three-dimensional structure interface of the negative electrode in all-solid-state lithium metal batteries include the following steps:

[0034] Step 1: Deposit a lithiophilic material on the surface of the structural material using vapor deposition (VCD) to form a nanoscale lithiophilic structural material. The VCD technique can be atomic layer deposition (ALD), molecular layer deposition (MLD), or chemical vapor deposition (CVD). The lithiophilic material can be one or a combination of several of the following: zinc oxide, magnesium oxide, indium oxide, tin oxide, titanium oxide, molybdenum oxide, lithium-rich organic thin films, zinc-rich organic thin films, aluminum-rich organic thin films, titanium-rich organic thin films, tin sulfide, zinc sulfide, molybdenum sulfide, rhodium, platinum, palladium, ruthenium, gold, and silver. The structural material can be one or a combination of one or more of the following: single-walled carbon nanotubes (SWNTs), multi-walled carbon nanotubes (MWCs), graphite oxide, graphene oxide, graphynylene oxide, carbon black oxide, zinc oxide, tin oxide, indium oxide, magnesium oxide, copper, aluminum, silver, iron, nickel, magnesium, tin, and zinc. The thickness of the nanoscale lithiophilic structural material is 1 nm–200 nm, preferably 10 nm–50 nm. The thickness of the lithiophilic material is controlled by setting different deposition cycle numbers.

[0035] Step 2: Using micro-spraying technology, the modified lithiophilic layer structural material is sprayed onto the surface of the solid electrolyte to form a micron-scale three-dimensional lithiophilic coating. The solid electrolyte is one or a combination of polymers, chlorides, sulfides, and oxides, preferably perovskite oxide electrolytes, garnet oxide electrolytes, or polyethylene oxide polymer electrolytes. The spraying technology is ultrasonic spraying, gas atomization spraying, or electrostatic spraying. The thickness of the micron-scale three-dimensional lithiophilic coating is 0.5 μm–50 μm, preferably 2 μm–20 μm. The thickness of the three-dimensional carbon material layer can be controlled by adjusting the amount of spraying slurry during preparation.

[0036] Step 3: Completely wet the three-dimensional lithium-loving coating on the surface of the solid electrolyte with molten lithium, and after cooling, form a tightly contacted solid-solid interface between the solid electrolyte and the lithium metal; wherein the contact time between the molten lithium and the three-dimensional lithium-loving coating is 1-60 min, preferably 5-30 min; the melting temperature is 181-350 ℃, preferably 200-300 ℃; and the lithium metal thickness is 0.01 mm-2 mm, preferably 0.1 mm-1.6 mm.

[0037] By adjusting different parameters in the construction process, the thickness of the micron-sized three-dimensional structure coating and the thickness of the surface nano-lithophile coating can be precisely controlled, thereby controlling the lithium affinity, lithium-ion conductivity, electronic conductivity, and lithium-ion diffusion coefficient at the interface between the solid electrolyte and the lithium metal anode.

[0038] Non-uniform contact at the solid-solid interface between the solid electrolyte and the lithium metal anode can easily lead to uneven current distribution and uneven lithium deposition, promoting the formation of lithium dendrites that penetrate into the solid electrolyte, ultimately causing a short circuit. The three-dimensional lithiophilic coating prepared by the above method, after reacting with molten lithium, can improve the contact between the solid electrolyte and lithium metal by filling the gaps between them and enhancing the interfacial lithiophilicity, effectively reducing interfacial impedance. Some solid electrolytes themselves have poor lithiophilicity, easily forming lithium carbonate on their surface, which is a lithiophore layer. Directly attaching the lithium anode to the solid electrolyte can easily create voids and pores. Constructing a lithiophilic coating can greatly improve lithiophilicity, improve the interfacial wetting of molten lithium and the electrolyte, achieve tight adhesion, and eliminate interfacial gaps and pores. The three-dimensional lithiophilic interface structure can guide a uniform and stable distribution of the electric field, thereby guiding uniform lithium deposition and promoting rapid lithium-ion transport at the interface, thus improving the cycle life of all-solid-state lithium metal batteries under high current density and high deposition / stripping capacity.

[0039] The above-described method for constructing a three-dimensional hybrid ion-electron conductive interface can be used to prepare all-solid-state lithium metal batteries. The three-dimensional structure interface of the all-solid-state lithium metal battery anode prepared through the above steps is a solid electrolyte / lithium metal anode that has been bonded together. It can be matched with a high-capacity cathode to form an all-solid-state lithium metal battery. The cathode material can be one or a combination of lithium cobalt oxide, lithium iron phosphate, lithium manganese oxide, lithium nickel cobalt manganese oxide, and lithium nickel cobalt aluminum oxide. In some embodiments of this invention, the components are assembled into coin cell half-cells or all-solid-state lithium metal batteries to test their performance. Experiments have shown that the strategy of modifying the surface of the solid electrolyte using vapor deposition and spraying techniques can effectively improve the contact between the solid electrolyte and lithium metal, reducing interfacial impedance. Furthermore, compared to the physical pressing of lithium sheets, molten lithium, in liquid metal form, contacts the electrolyte surface. Utilizing the wetting, spreading, and penetrating behavior of liquid lithium, it spontaneously fills surface irregularities, voids, and defects, resulting in a void-free interface and achieving atomic-level continuous contact. This leads to high interfacial bonding strength, effectively maintaining interface integrity during charge and discharge, inhibiting interface degradation and void formation, and significantly improving cycle life. In addition, the three-dimensional lithium-loving interface can guide a uniform and stable distribution of the electric field, thereby guiding uniform lithium deposition and promoting rapid lithium-ion transport at the interface. This further enhances the cycle life of all-solid-state lithium metal batteries under high current density and high deposition / stripping capacity.

[0040] The present invention will now be described with reference to the accompanying drawings. Experimental methods not specifically described in terms of operation steps are performed in accordance with the corresponding product manuals. Unless otherwise specified, the instruments, reagents, and consumables used in the embodiments can be purchased from commercial companies.

[0041] Example 1: Construction of a three-dimensional hybrid ion-electron conductive interface for all-solid-state batteries

[0042] Hydroxylated multi-walled carbon nanotubes were sonicated in ethanol for 20 min to obtain a slurry. The slurry was uniformly dropped onto a glass slide, and after the ethanol evaporated, the glass slide was placed in an atomic layer deposition system. The reaction chamber was heated to 150°C, and using diethylzinc and water as precursors and argon as carrier gas, 90-cycle zinc oxide was deposited on the surface of the carbon nanotubes to a thickness of approximately 18 nm, thus obtaining a nanoscale lithiophilic structure material. The thickness of the hydroxylated multi-walled carbon nanotubes was approximately 22 nm, and the thickness of the carbon nanotubes after zinc oxide deposition was approximately 40.8 nm, consistent with expectations, demonstrating a significant nanoscale control over the thickness of the lithiophilic coating.

[0043] Carbon nanotubes with deposited zinc oxide were scraped off from a glass slide and ultrasonicated in ethanol for 60 min to obtain a spray slurry. A garnet-type oxide solid electrolyte was placed on a heating stage and heated to 100 °C. The slurry was then quantitatively sprayed onto both the upper and lower surfaces of the electrolyte using a micro-atomization spraying technique. Ethanol rapidly evaporated from the electrolyte surface, resulting in a three-dimensional lithiophilic coating. Scanning electron microscopy (SEM) images of the resulting interface surface are shown below. Figure 1 As shown, the obtained scanning electron microscope (SEM) image of the interface section and the corresponding energy-dispersive X-ray spectrometer (EDS) image are as follows. Figure 2 As shown, the thickness of the three-dimensional carbon material layer is controlled by adjusting the amount of carbon nanotube spraying slurry. The carbon material layer thickness in the figure is 2.5 μm, demonstrating a significant controllable effect at the micrometer scale. Simultaneously, the corresponding elemental distribution in the EDS analysis shows that zinc oxide is uniformly deposited on the carbon nanotube surface. These figures demonstrate the successful preparation of a uniform, precisely controllable three-dimensional lithiophilic coating on the surface of a solid electrolyte.

[0044] A lithium sheet was placed on a heating stage and heated to 240°C. After removing surface impurities, molten spheres were formed, which then came into close contact with a lithiophilic coating on the surface of a solid electrolyte. Upon cooling, a three-dimensional hybrid ion-electron conductive interface was obtained. A photograph of the interface after contact is shown below. Figure 3 As shown, the molten lithium and the solid electrolyte make good contact, with a contact angle of less than 90 degrees. A scanning electron microscope (SEM) image of the cross-section after contact is shown below. Figure 4 As shown, the lithium metal is in very close contact with the lithiophilic coating, and no pores are generated.

[0045] Coin cells were assembled using methods known in the art. Molten lithium was contacted to both sides of a modified solid electrolyte, forming a three-dimensional mixed ion-electron conductive interface at both the positive and negative electrodes. The coin cells were assembled using a 2032 coin cell casing with molten lithium as the two electrodes. Long-cycle testing was conducted using the coin cells under the following conditions: a constant current density of 0.5 mA / cm². -2 The capacity is 0.25 mAh / cm³. -2 .like Figure 5As shown, under the above test conditions, the coin cell can cycle stably for over 680 hours and maintain a stable overpotential plateau. This demonstrates that the three-dimensional hybrid ion-electron conductive interface prepared by this method provides a protective shielding effect, promoting ion transfer and inhibiting lithium dendrite growth even at high current densities.

[0046] Coin cells were assembled using methods known in the art. Molten lithium was used as the negative electrode, NCM as the positive electrode, and a 2032 coin cell casing was used to assemble the coin cells. The current density at the negative electrode surface was 0.5 mA / cm². -2 Cyclic performance testing was conducted under a voltage range of 2.6-4.2 V. For example... Figure 6 As shown, under the above test conditions, the first cycle capacity was 1.275 mAh / cm³. -2 After 160 cycles, the capacity is 1.104 mAh / cm³. -2 With a capacity retention rate of up to 86.6% and an average coulombic efficiency of over 99%, it exhibits excellent cycle stability and reversibility.

[0047] Example 2:

[0048] A three-dimensional hybrid ion-electron conductive interface for the all-solid-state battery was constructed using the same methods as in Example 1, except that the number of atomic-layer deposited zinc oxide periods was 30, and the thickness was approximately 6 nm. The resulting scanning electron microscope (SEM) image of the interface surface is shown below. Figure 7 As shown, the thickness of the carbon nanotubes after zinc oxide deposition is approximately 28.9 nm. Combined with Example 1, it can be found that the thickness of the carbon nanotubes increases proportionally with the increase of the atomic layer deposition cycle, indicating that this method has a precise control effect on the thickness of the surface lithiophilic coating.

[0049] Comparative Example 1:

[0050] Molten lithium was brought into contact with both sides of an unmodified solid electrolyte, with the molten lithium serving as the two electrodes. A coin cell half-cell was assembled using a 2032 coin cell casing. Long-cycle testing was conducted using the coin cell half-cell, under the same test conditions as in Example 1.

[0051] like Figure 8 As shown, under the above test conditions, the coin cell can only cycle for 160 hours, and its stability is greatly reduced compared to Example 1. This indicates that the three-dimensional lithium-loving interface prepared by the present invention between the solid electrolyte and the lithium metal anode greatly solves the solid-solid interface contact problem existing in solid-state batteries, improves the uniformity and stability of the electric field distribution, enhances the diffusion ability of lithium at the solid-solid interface, and thus improves the cycle life of all-solid-state lithium metal batteries under high current density.

[0052] Comparative Example 2:

[0053] The three-dimensional hybrid ion-electron conductive interface of the all-solid-state battery was constructed using the same method as in Example 1, except that lithium sheets were directly attached to the surface of the solid electrolyte instead of molten lithium contacting the lithium-loving coating.

[0054] A coin cell half-cell is assembled using lithium sheets as electrodes on both sides and a 2032 coin cell casing.

[0055] Long-cycle testing was performed using button half-cells, under the same conditions as in Example 1.

[0056] like Figure 9 As shown, for solid-state batteries fabricated using the lithium-on-a-sheet process, the electrolyte and lithium metal remain in a solid-solid contact, exhibiting extremely poor cycle stability and high electrochemical polarization. The battery experiences a short circuit in the first cycle, with a charge / discharge overpotential as high as 1.7V, failing to complete stable cycling. This phenomenon directly reflects the extremely poor physical contact between the lithium sheet and the solid electrolyte, severe discontinuity in the ion transport path, and huge interfacial impedance. This contrasts sharply with the excellent electrochemical performance of solid-state batteries prepared using the molten lithium process, clearly demonstrating that molten lithium technology can significantly optimize the interfacial contact between the lithium anode and the solid electrolyte, improving interfacial stability and ion transport kinetics, making it a key strategy for achieving high-performance, long-life solid-state batteries.

[0057] The embodiments of the present invention have been described in detail above, but the content described is only a preferred embodiment of the present invention and should not be considered as limiting the scope of the present invention. All equivalent changes and improvements made in accordance with the scope of the present invention should still fall within the patent coverage of the present invention.

Claims

1. A method for constructing a three-dimensional structure interface for the negative electrode of an all-solid-state lithium metal battery, characterized in that: A micro-nano scale coating preparation technology combining vapor deposition and micro-spraying was used to precisely prepare a three-dimensional lithiophilic coating on the surface of a solid electrolyte. The molten lithium was brought into full contact with the lithiophilic coating through a lithiation reaction, thereby forming a tight solid-solid interface between the solid electrolyte and the lithium metal.

2. The method for constructing a three-dimensional structure interface of an all-solid-state lithium metal battery anode according to claim 1, characterized in that: The specific steps are as follows: Step 1: Deposit lithiophilic materials on the surface of structural materials using vapor deposition technology to form nanoscale lithiophilic structural materials; Step 2: Using micro-spraying technology, the structural material with the modified lithiophilic layer is sprayed onto the surface of the solid electrolyte to form a three-dimensional lithiophilic coating at the micron scale; Step 3: Completely wet the three-dimensional lithium-loving coating on the surface of the solid electrolyte with molten lithium. After cooling, a tight solid-solid interface is formed between the solid electrolyte and the lithium metal.

3. The method for constructing a three-dimensional structure interface of an all-solid-state lithium metal battery anode according to claim 1 or 2, characterized in that: Vapor deposition technology includes one or more combinations of atomic layer deposition, molecular layer deposition, or chemical vapor deposition; micro-spraying technology includes one or more combinations of ultrasonic spraying, gas atomization spraying, or electrostatic spraying.

4. The method for constructing a three-dimensional structure interface of an all-solid-state lithium metal battery anode according to claim 1 or 2, characterized in that: Solid electrolytes include one or more of polymers, chlorides, sulfides, and oxides.

5. A method for constructing a three-dimensional structure interface of an all-solid-state lithium metal battery anode according to claim 1 or 2, characterized in that: The structural material is one or more of the following: single-walled carbon nanotube oxide, multi-walled carbon nanotube oxide, graphite oxide, graphene oxide, graphdiyne oxide, carbon black oxide powder, zinc oxide, tin oxide, indium oxide, magnesium oxide, zirconium oxide, niobium oxide, tantalum oxide, aluminum oxide, lithium oxide powder, copper, aluminum, silver, iron, nickel, tantalum, magnesium, tin, zinc powder, garnet oxide, lithium nitride, and lithium fluoride powder; the diameter of the structural material powder particles is 0.1 μm–10 μm.

6. The method for constructing a three-dimensional structure interface of an all-solid-state lithium metal battery anode according to claim 5, characterized in that: Lithophile materials include one or more of the following: zinc oxide, magnesium oxide, indium oxide, tin oxide, titanium oxide, molybdenum oxide, lithium-rich organic films, zinc-rich organic films, aluminum-rich organic films, titanium-rich organic films, tin sulfide, zinc sulfide, molybdenum sulfide, rhodium, platinum, palladium, ruthenium, gold, and silver.

7. The method for constructing a three-dimensional structure interface of an all-solid-state lithium metal battery anode according to claim 6, characterized in that: The thickness of the lithophile-modified coating is 1 nm–200 nm; the thickness of the three-dimensional structure coating is 0.5 μm–50 μm.

8. The method for constructing a three-dimensional structure interface of an all-solid-state lithium metal battery anode according to claim 2, characterized in that: The contact time between molten lithium and the three-dimensional lithium-loving coating was 1–60 min, the melting temperature was 181–350 ℃, and the lithium metal thickness was 0.01 mm–2 mm.

9. An all-solid-state lithium metal battery, characterized in that: First, a composite structure of solid electrolyte and lithium metal anode is constructed according to the construction method of the three-dimensional structure interface of the all-solid-state lithium metal battery anode as described in any of claims 1-8. Then, it is combined with a high-capacity cathode to obtain an all-solid-state lithium metal battery.

10. The all-solid-state lithium metal battery according to claim 9, characterized in that: The cathode material includes one or more combinations of lithium cobalt oxide, lithium iron phosphate, lithium manganese oxide, lithium nickel cobalt manganese oxide, and lithium nickel cobalt aluminum oxide.

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