Electrode application composite ceramic electrolyte particle coated with hydrophobic protective layer

Abstract

The invention discloses a hydrophobic protective layer coated composite ceramic electrolyte particle applied to an electrode, which comprises a plurality of composite LLZO particles, and each composite LLZO particle comprises: an LLZO particle; the outer surface of the LLZO particle is coated with a first hydroxide ion layer, so that a secondary LLZO particle is integrally formed; the secondary LLZO particle is coated with a first dopamine layer, so that the hydrophobic LLZO particle is formed; an outer hydrophobic layer is coated on the outer surface of the hydrophobic LLZO particle to form the composite LLZO particle; the outer hydrophobic layer is a plurality of peripheral composite particles, and the peripheral composite particles are a plurality of barium titanate composite particles or a plurality of zinc oxide composite particles or a combination of the barium titanate composite particles and the zinc oxide composite particles; each peripheral composite particle is formed by coating the periphery of each peripheral particle with a second hydroxide ion layer; and the periphery of each second hydroxide ion layer is coated with a corresponding second dopamine layer, and dopamine in each dopamine layer can generate copolymerization, so that the outer hydrophobic layer is coated on the outer surface of the hydrophobic LLZO particle and is naturally formed during stirring.

Description

Technical Field

[0001] This invention relates to the field of battery electrode materials technology, and in particular to a composite ceramic electrolyte particle for electrode application coated with a hydrophobic protective layer. Background Art

[0002] A battery is mainly formed by placing a positive electrode and a negative electrode in an electrolyte. In conventional technology, LLZO material is added to the negative electrode to increase ionic conductivity. LLZO material has high ionic conductivity for lithium ions. Therefore, when lithium ions pass through the negative electrode, the dispersed LLZO particles guide the lithium ions, thus allowing for a uniform distribution of lithium ions within the negative electrode. This prevents abnormal accumulation of lithium ions in the negative electrode slurry and avoids side reactions with the slurry.

[0003] However, moisture is present during the manufacturing process of the negative electrode. Since LLZO material is hydrophilic, it is prone to react with water, causing it to become damp and generate alkaline substances, which leads to the deterioration of the material in the negative electrode slurry. Summary of the Invention

[0004] This invention provides a composite ceramic electrolyte particle for electrode application coated with a hydrophobic protective layer to overcome the aforementioned deficiencies in the prior art.

[0005] The technical solution of this invention is as follows: An electrode application composite ceramic electrolyte particle with a hydrophobic protective layer is provided. This is achieved by coating the outer surface of LLZO particles with barium titanate composite particles or zinc oxide composite particles to form better ionic conductivity. Furthermore, because the multiple barium titanate particles or zinc oxide particles and the dopamine layer have hydrophobic properties, coating the outer surface of the secondary LLZO particles with the dopamine layer makes it more difficult for moisture to enter the LLZO particles, and the barium titanate composite particles or zinc oxide composite particles provide further hydrophobic protection. Moreover, nanoscale amorphous carbon and carbon nanotubes act as conductive aids. The nanoscale amorphous carbon is in the form of particles, while the carbon nanotubes are in the form of elongated strips. The addition of nanoscale amorphous carbon into the gaps contributes to the overall conductivity of the structure. In this invention, multiple barium titanate composite particles or zinc oxide composite particles, the dopamine layer, multiple carbon nanotubes, and nanoscale amorphous carbon are used to form a multilayer protection, so the entire composite LLZO particle structure has enhanced lithium conductivity, and avoids reaction with water during the electrode manufacturing process, thus achieving better battery electrode material manufacturing quality.

[0006] To achieve the above objectives, this invention proposes a composite ceramic electrolyte particle for electrode application coated with a hydrophobic protective layer. The composite ceramic electrolyte particle is composed of multiple composite LLZO particles, which are added to an electrode in a solid-state or near-solid-state battery. The electrode comprises: an electrode substrate and an electrode paste layer coated on the electrode substrate; each composite LLZO particle comprises:

[0007] LLZO particles are used to guide and disperse lithium ions through the electrode, thus enabling lithium ions to form a uniform channel distribution inside the electrode.

[0008] A first hydroxide ion layer is coated on the outer surface of the LLZO particles, forming a primary and secondary LLZO particle. The first hydroxide ion layer is formed by adding tris(hydroxymethyl)amine during the manufacturing process of the composite LLZO particles. Tris(hydroxymethyl)amine itself has three OH- bonds. Two of the OH- bonds in the tris(hydroxymethyl)amine are used to form hydrogen bonds with the oxidized functional groups of the LLZO particles. The third OH- bond on the tris(hydroxymethyl)amine extends towards the outer surface of the LLZO particles, thereby forming the first hydroxide ion layer. Tris(hydroxymethyl)amine can also be called tris(hydroxymethyl)aminomethane (Tris).

[0009] A first dopamine layer coats the exterior of the secondary LLZO particles, forming a hydrophobic LLZO particle; wherein the OH- bonds of the dopamine itself undergo a dehydration polymerization reaction with the third OH- bonds of the first hydroxide ion layer to form the first dopamine layer; the dopamine has hydrophobic properties, which can further protect the LLZO particles from moisture.

[0010] An outer hydrophobic layer is coated on the outer surface of the hydrophobic LLZO particles to form the composite LLZO particles; wherein the outer hydrophobic layer is composed of multiple peripheral composite particles, which are multiple barium titanate composite particles or multiple zinc oxide composite particles or a combination of both.

[0011] Each peripheral composite particle is formed by coating a second hydroxide ion layer on the periphery of each peripheral particle (which is a barium titanate particle or a zinc oxide particle), and each second hydroxide ion layer is further coated with a corresponding second dopamine layer.

[0012] The second hydroxyl ion layer is formed by adding tris(hydroxymethyl)amine during the manufacturing process of the composite LLZO particles. Tris(hydroxymethyl)amine itself has three OH- bonds. Two of these OH- bonds are used to form hydrogen bonds with the oxidative functional groups on the barium titanate or zinc oxide particles. The third OH- bond of the tris(hydroxymethyl)amine extends towards the outer surface of the barium titanate or zinc oxide particles, thus forming the second hydroxyl ion layer. During the manufacturing process of the entire composite LLZO particles, the OH- bonds of the dopamine in the second dopamine layer corresponding to each peripheral composite particle undergo a dehydration polymerization reaction with the OH- bonds on the second hydroxyl ion layer, forming the overall second dopamine layer.

[0013] When the outer hydrophobic layer coats the outer surface of the hydrophobic LLZO particles, the dopamine in the first dopamine layer and the second dopamine layer will undergo a copolymerization reaction. Therefore, the outer hydrophobic layer coats the outer surface of the hydrophobic LLZO particles and is formed naturally during the process stirring.

[0014] This invention coats the outer surface of an LLZO material with multiple barium titanate particles or multiple zinc oxide particles and dopamine material, giving it hydrophobic properties and making it less susceptible to moisture penetration. Furthermore, carbon nanotubes and nanoscale amorphous carbon are added to the outer surface of the LLZO material coated with barium titanate or zinc oxide and dopamine material to coat the negative electrode particles in the battery's negative electrode material, improving the overall conductivity of the negative electrode. Since the ionic conductivity of the multiple barium titanate particles is superior to that of the LLZO particles, a better overall ionic conductivity is also achieved. The zinc oxide particles improve negative electrode compatibility and the ion interface layer, and because they possess the functions of a negative electrode material, the capacity loss due to coating is reduced.

[0015] The features and advantages of the invention will be further understood from the following description, and please refer to the accompanying drawings while reading. Attached Figure Description

[0016] Figure 1 This invention is shown in a structural diagram.

[0017] Figure 2 Examples of applications of the present invention are shown.

[0018] Figure 3 This diagram shows an enlarged schematic of the hydroxide ion layer structure of the secondary LLZO particles of the present invention.

[0019] Figure 4 This diagram shows an enlarged schematic of the hydrophobic LLZO particle structure of the present invention, which illustrates the enlarged schematic and structural diagram of the dehydration polymerization reaction formed by the OH- bonds of the dopamine itself and the third OH- bond of the hydroxide ion layer.

[0020] Figure 5 This shows an enlarged schematic diagram of the barium titanate composite particle structure of the present invention.

[0021] Figure 6 This shows an enlarged schematic diagram of the zinc oxide composite particle structure of the present invention.

[0022] Figure 7 This diagram shows the three-level LLZO particle structure of the present invention.

[0023] Figure 8 A cross-sectional view of the structure of the present invention is shown.

[0024] Figure 9 This is an enlarged schematic diagram showing the structure of the present invention. Detailed Implementation

[0025] The present invention will now be described in detail with reference to the accompanying drawings and specific embodiments.

[0026] Please refer to Figures 1 to 9 As shown, the electrode application of the present invention, coated with a hydrophobic protective layer, comprises composite ceramic electrolyte particles, wherein the particles are multiple composite LLZO (lithium lanthanum zirconium oxide) particles 100, which are mainly used in the electrodes of solid-state or near-solid-state batteries, especially the negative electrode 10 of such batteries. The LLZO is composed of lithium lanthanum zirconium oxide (Li7La3Zr2O) 12 Lithium lanthanum zirconium oxide (LLZO), or lithium lanthanum zirconium oxide doped with at least one metal element (e.g., Li 6.2 Ga 0.8 La3Zr2O 12 It is a gallium (Ga)-doped lithium lanthanum zirconium oxide compound, or it can be an aluminum (Al)-doped or barium (Ba)-doped lithium lanthanum zirconium oxide compound. The particle size of the composite LLZO particles 100 is between 50 nanometers and 200 nanometers.

[0027] The negative electrode 10 comprises: a negative electrode substrate 11, which is a carrier material for supporting the negative electrode 10; and a negative electrode slurry layer 13 coated on the negative electrode substrate 11, the negative electrode slurry layer 13 comprising a negative electrode slurry 12 as a binder. The negative electrode slurry 12 is a mixture of SBR (Styrene Butadiene Rubber), CMC (Carboxymethyl Cellulose), and a conductive agent (CNT (Carbon Nanotube) or Super-P (Conductive Carbon). Water is used as the solvent in the fabrication of the negative electrode slurry 12. The composite LLZO particles 100 are used to guide lithium ions. The proportion of the composite LLZO particles 100 in the electrode slurry layer (especially the negative electrode slurry layer) is between 0.5 wt% and 5 wt%.

[0028] The structure of a composite LLZO particle 100 according to the present invention is described below. The composite LLZO particle 100 comprises:

[0029] The LLZO particles 15 are mainly used because LLZO material has high ionic conductivity for lithium ions. Therefore, when lithium ions pass through the electrode, the multiple dispersed LLZO particles 15 can guide and disperse the lithium ion pathways, thus allowing the lithium ions to present a uniform channel distribution inside the electrode. This avoids abnormal accumulation of lithium ions in the electrode slurry and prevents side reactions with the electrode slurry.

[0030] Since moisture is present during the manufacturing process of this electrode, and the LLZO particles 15 are hydrophilic and therefore easily affected by moisture, causing a chemical reaction that produces alkaline substances, the outer layer of the LLZO particles 15 must be covered with a protective layer to prevent the LLZO particles 15 from becoming damp during the manufacturing process of this electrode.

[0031] A first hydroxide ion (OH-) layer 24 coats the outer surface of the LLZO particle 15, forming a primary and secondary LLZO particle 30 (e.g., Figure 3 The thickness of the first hydroxide ion layer 24 is between 0.5 nm and 2 nm. This first hydroxide ion layer 24 is formed by adding tris(hydroxymethyl)amine during the manufacturing process of the composite LLZO particles 100. The tris(hydroxymethyl)amine itself has three OH- bonds, two of which are hydrogen-bonded with the oxidized functional groups on the LLZO particles 15. The third OH- bond of the tris(hydroxymethyl)amine extends towards the outer surface of the LLZO particles 15, thus forming the first hydroxide ion layer 24. Only two tris(hydroxymethyl)amine molecules are shown in the figure; this number is for illustrative purposes only and is not intended to limit the scope of the invention.

[0032] A first dopamine layer 35 coats the exterior of the secondary LLZO particle 30, thereby forming a hydrophobic LLZO particle 40 (e.g., Figure 4 The dopamine's OH- bonds undergo a dehydration polymerization reaction with the third OH- bond of the first hydroxyl ion layer 24, allowing the dopamine to combine with the secondary LLZO particles 30 to form the hydrophobic LLZO particles 40. Due to the copolymerization reaction between dopamine molecules, a first dopamine layer 35 is formed. The thickness of the first dopamine layer 35 is between 1 nanometer and 10 nanometers.

[0033] The purpose of coating the secondary LLZO particles 30 with a first dopamine layer 35 is primarily because moisture is present during the manufacturing process of the electrode paste. Since the LLZO particles 15 are hydrophilic, they are easily affected by moisture, producing alkaline byproducts that compromise their lithium conductivity. Dopamine, on the other hand, is hydrophobic; therefore, coating the secondary LLZO particles 30 with the first dopamine layer 35 further protects them from moisture absorption.

[0034] An outer hydrophobic layer 41 is coated on the outer surface of the hydrophobic LLZO particles 40 to form the composite LLZO particles 100 (e.g., Figure 1 The outer hydrophobic layer 41 consists of multiple peripheral composite particles 20 and 22, which are multiple barium titanate composite particles 20 or multiple zinc oxide composite particles 22, or a combination of both. The distribution of the peripheral composite particles 20 and 22 on the outer surface of the hydrophobic LLZO particles 40 is naturally formed during the process stirring.

[0035] like Figure 5 and Figure 6 As shown, each peripheral composite particle 20, 22 has a second hydroxide ion layer 21 coated around its periphery (the peripheral particle is a barium titanate particle 201 or a zinc oxide particle 221); and each second hydroxide ion layer 21 is further coated around its periphery with a corresponding second dopamine layer 36. The particle size of each barium titanate composite particle 20 or zinc oxide composite particle 22 is between 10 nanometers and 20 nanometers.

[0036] like Figure 5 and Figure 6 As shown, the second hydroxide ion layer 21 is formed by adding tris(hydroxymethyl)amine during the manufacturing process of the composite LLZO particles 100. The tris(hydroxymethyl)amine itself has three OH- bonds, two of which are hydrogen-bonded with the oxidized functional groups of the barium titanate particles 201 or zinc oxide particles 221. The third OH- bond of the tris(hydroxymethyl)amine extends towards the outer surface of the barium titanate particles 201 or zinc oxide particles 221, thus forming the second hydroxide ion layer 21. During the manufacturing process of the entire composite LLZO particles 100, the OH- bonds of the dopamine in the second dopamine layer 36 corresponding to each of the peripheral composite particles 20 and 22 undergo a dehydration polymerization reaction with the OH- bonds on the second hydroxide ion layer 21, forming the second dopamine layer 36 as a whole. Only two tris(hydroxymethyl)amine molecules are shown in the figure; this number is for illustrative purposes only and is not intended to limit the scope of the invention.

[0037] The weight ratio of the total weight of the outer hydrophobic layer 41 to the total weight of the hydrophobic LLZO particles 40 is between 1 / 25 and 1 / 10 (4% to 10%), i.e., between 0.04 and 0.1. The thickness of the second hydroxide ion layer 21 is between 0.5 nanometers and 2 nanometers; the thickness of the second dopamine layer 36 is between 1 nanometer and 10 nanometers.

[0038] When the outer hydrophobic layer 41 covers the outer surface of the hydrophobic LLZO particles 40, the dopamine in the first dopamine layer 35 and the second dopamine layer 36 will undergo a chain copolymerization reaction. Therefore, the outer hydrophobic layer 41 can cover the outer surface of the hydrophobic LLZO particles 40, and it is formed naturally during the process stirring.

[0039] The purpose of coating the outer hydrophobic layer 41 is that the barium titanate particles 201 and the zinc oxide particles 221 are themselves hydrophobic. Therefore, when the multiple barium titanate composite particles 20 or the multiple zinc oxide composite particles 22 are coated on the outer surface of the hydrophobic LLZO particles 40, moisture can be further isolated to prevent the hydrophobic LLZO particles 40 from getting damp. Moreover, since the ionic conductivity of the barium titanate particles 201 is better than that of the LLZO particles 15, the overall ionic conductivity can also be better. The zinc oxide particles 221 can improve electrode compatibility and ion interface layer. Also, because they have the functions of electrode materials, the reduction in capacitance due to coating can be minimized.

[0040] The purpose of applying the second hydroxide ion layer 21 to coat the outer surface of the surrounding particles is that the barium titanate particles 201 or the zinc oxide particles 221 are insoluble in water, and hydroxide ions (OH-) are polar. Therefore, by coating the second hydroxide ion layer 21, they can react with the dopamine material of the corresponding second dopamine layer 36, so that the dopamine material can better adhere to the barium titanate particles 201 or the zinc oxide particles 221.

[0041] The present invention also includes:

[0042] Multiple carbon nanotubes 42 (CNTs) and multiple nanoscale amorphous carbon 45 are coated on the composite LLZO particles 100 to form a tertiary LLZO particle 50 (e.g. Figure 7 The carbon nanotubes 42 have a size ranging from 200 nm to 500 nm, while the amorphous carbon 45 at this nanoscale has a size ranging from 10 nm to 40 nm. This amorphous carbon 45 at this nanoscale is, for example, a super P conductive agent.

[0043] In each of the three-level LLZO particles 50, the weight ratio of the total weight of the corresponding [multiple carbon nanotubes 42 and multiple nanoscale amorphous carbon 45] to the total weight of the LLZO particle 15 (i.e., the single LLZO particle 15) is 0.2 to 2: 99.8 to 98.

[0044] The nanoscale amorphous carbon 45, like the carbon nanotubes 42, serves as a conductive agent. Because the nanoscale amorphous carbon 45 is in particulate form, while the carbon nanotubes 42 are elongated, gaps are formed between the crisscrossing nanotubes 42. These gaps cannot conduct current. Therefore, adding the nanoscale amorphous carbon 45 into these gaps allows charge to be conducted to the next carbon nanotube 42 through the bridging of the nanoscale amorphous carbon 45 particles, thus further increasing current transfer. When the carbon nanotubes 42 are attached to the composite LLZO particles 100, they form a shape resembling a ball of yarn (e.g., ...). Figure 7 ).

[0045] The advantage of the carbon nanotubes 42 is that lithium ions can be easily stabilized between them. Therefore, the electrode slurry in this invention can stabilize a large number of lithium ions, thus improving the overall lithium ion conductivity. Furthermore, electrons can be easily fixed between the carbon nanotubes 42, thereby improving the overall lithium ion conductivity. Moreover, because the ion conductivity is very high, it facilitates rapid charging and discharging of the battery, and also reduces the amount of cobalt used, thus lowering the overall production cost.

[0046] In this invention, the outer surface of the LLZO particles is coated with barium titanate composite particles or zinc oxide composite particles to form better ionic conductivity. Furthermore, because the multiple barium titanate particles or zinc oxide particles and the dopamine layer have hydrophobic properties, coating the outer surface of the secondary LLZO particles with the dopamine layer makes it more difficult for moisture to penetrate the LLZO particles, and the barium titanate composite particles or zinc oxide composite particles provide further hydrophobic protection. The nanoscale amorphous carbon and carbon nanotubes act as conductive aids. The nanoscale amorphous carbon is in the form of particles, while the carbon nanotubes are in the form of elongated strips; the addition of nanoscale amorphous carbon into the gaps contributes to the overall conductivity of the structure. In this invention, multiple barium titanate composite particles or zinc oxide composite particles 22, the dopamine layer, and the multiple carbon nanotubes and nanoscale amorphous carbon form a multi-layered protective layer, so the entire composite LLZO particle structure has enhanced lithium conductivity, and reactions with water are avoided during electrode manufacturing, achieving better battery electrode material manufacturing quality.

[0047] In summary, the human-centered and considerate design of this invention is highly suitable for practical needs. Its specific improvements over existing deficiencies represent a significant breakthrough compared to conventional technology, offering substantial efficiency gains that are not easily achieved.

[0048] The above detailed description is a specific description of one feasible embodiment of the present invention. However, this embodiment is not intended to limit the patent scope of the present invention. All equivalent implementations or modifications that do not depart from the spirit of the present invention should be included in the patent scope of the present invention.

Claims

1. A composite ceramic electrolyte particle for electrode application coated with a hydrophobic protective layer, characterized in that, include: The electrode coated with the hydrophobic protective layer uses composite ceramic electrolyte particles, which are multiple composite LLZO particles. The LLZO is lithium lanthanum zirconium oxide or lithium lanthanum zirconium oxide doped with at least one metal element. These composite LLZO particles are added to an electrode in a solid-state or near-solid-state battery. The electrode comprises: an electrode substrate and an electrode paste layer coated on the electrode substrate; each composite LLZO particle contains: LLZO particles are used to guide and disperse lithium ions through the electrode, thus enabling lithium ions to form a uniform channel distribution inside the electrode. A first hydroxide ion layer is coated on the outer surface of the LLZO particles, forming a first- and second-order LLZO particles. The first hydroxide ion layer is formed by adding tris(hydroxymethyl)amine during the manufacturing process of the composite LLZO particles. The tris(hydroxymethyl)amine itself has three OH- bonds. Two of the OH- bonds in the tris(hydroxymethyl)amine are used to form hydrogen bonds with the oxidized functional groups of the LLZO particles themselves. The third OH- bond on the tris(hydroxymethyl)amine extends towards the outer surface of the LLZO particles, thereby forming the first hydroxide ion layer. A first dopamine layer coats the exterior of the secondary LLZO particles, forming a hydrophobic LLZO particle; wherein the OH- bonds of the dopamine itself undergo a dehydration polymerization reaction with the third OH- bonds of the first hydroxide ion layer to form the first dopamine layer; the dopamine has hydrophobic properties, which can further protect the LLZO particles from moisture. An outer hydrophobic layer is coated on the outer surface of the hydrophobic LLZO particles to form the composite LLZO particles; wherein the outer hydrophobic layer is composed of multiple peripheral composite particles, which are multiple barium titanate composite particles or multiple zinc oxide composite particles or a combination of both. Each peripheral composite particle is formed by coating a second hydroxide ion layer on the periphery of each peripheral particle, wherein the peripheral particle is a barium titanate particle or a zinc oxide particle; and each second hydroxide ion layer is further coated with a corresponding second dopamine layer. The second hydroxide ion layer is formed by adding tris(hydroxymethyl)amine during the manufacturing process of the composite LLZO particles. Tris(hydroxymethyl)amine itself has three OH- bonds. Two of the OH- bonds in the tris(hydroxymethyl)amine are used to form hydrogen bonds with the oxidative functional groups on the barium titanate particles or zinc oxide particles. The third OH- bond of the tris(hydroxymethyl)amine extends towards the outer surface of the barium titanate particles or zinc oxide particles, thereby forming the second hydroxide ion layer. During the manufacturing process of the entire composite LLZO particles, the OH- bonds of the dopamine in the second dopamine layer corresponding to each of the peripheral composite particles undergo a dehydration polymerization reaction with the OH- bonds on the second hydroxide ion layer, forming the second dopamine layer as a whole. When the outer hydrophobic layer coats the outer surface of the hydrophobic LLZO particles, the dopamine in the first dopamine layer and the second dopamine layer will undergo a copolymerization reaction. Therefore, the outer hydrophobic layer coats the outer surface of the hydrophobic LLZO particles and is formed naturally during the process stirring.

2. The electrode application composite ceramic electrolyte particles coated with a hydrophobic protective layer according to claim 1, characterized in that, The LLZO particles are selected from lithium lanthanum zirconium oxide, or lithium lanthanum zirconium oxide doped with at least one metal element.

3. The electrode application composite ceramic electrolyte particles coated with a hydrophobic protective layer according to claim 1, characterized in that, The weight ratio of the total weight of the outer hydrophobic layer to the total weight of the hydrophobic LLZO particles is between 0.04 and 0.

1.

4. The electrode application composite ceramic electrolyte particles coated with the hydrophobic protective layer according to claim 1, characterized in that, The composite LLZO particles are used in a negative electrode.

5. The electrode application composite ceramic electrolyte particles coated with the hydrophobic protective layer according to claim 1, characterized in that, The particle size of the composite LLZO particles ranges from 50 nanometers to 200 nanometers.

6. The electrode application composite ceramic electrolyte particles coated with the hydrophobic protective layer according to claim 1, characterized in that, The particle size of each barium titanate composite particle or zinc oxide composite particle is between 10 nanometers and 20 nanometers.

7. The electrode application composite ceramic electrolyte particles coated with the hydrophobic protective layer according to claim 1, characterized in that, The thickness of the first hydroxide ion layer and the second hydroxide ion layer are each between 0.5 nanometers and 2 nanometers.

8. The electrode application composite ceramic electrolyte particles coated with the hydrophobic protective layer according to claim 1, characterized in that, The thickness of the first dopamine layer and the second dopamine layer are each between 1 nanometer and 10 nanometers.

9. The electrode application composite ceramic electrolyte particles coated with the hydrophobic protective layer according to claim 1, characterized in that, It also includes: multiple carbon nanotubes and multiple nanoscale amorphous carbon coatings on the outer surface of the composite LLZO particles to form tertiary LLZO particles.

10. The electrode application composite ceramic electrolyte particles coated with a hydrophobic protective layer according to claim 9, characterized in that, The size of the carbon nanotubes ranges from 200 nanometers to 500 nanometers; the size of the nanoscale amorphous carbon ranges from 10 nanometers to 40 nanometers.

11. The electrode application composite ceramic electrolyte particles coated with a hydrophobic protective layer according to claim 9, characterized in that, In each of the three-level LLZO particles, the weight ratio of the corresponding "total weight of multiple carbon nanotubes and multiple nanoscale amorphous carbon" to the total weight of the LLZO particles is 0.2-2:99.8-98.

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