Aluminosilicate lithium ion solid electrolyte and preparation method thereof

Abstract

The present invention belongs to the technical field of solid electrolytes, and discloses a lithium aluminosilicate lithium solid electrolyte and a preparation method thereof. The lithium aluminosilicate lithium solid electrolyte is a spodumene and derivative system, and its chemical formula is Li 1‑x Al 1‑x Si 2+x O6; wherein, x = 0.5, 0.25, -0.25, -0.5, -0.75 or -1.00. Since the present invention adjusts the ratio of Al to Si in LiAlSi2O6 to predict Li 1‑x Al 1‑x Si 2+ x O6 material system. Compared with the original LiAlSi2O6, the Li 1‑x Al 1‑x Si 2+x O6 (x≠0) system provided by the present invention has better lithium ion conductivity at room temperature. A series of materials obtained by changing the ratio of Al to Si in LiAlSi2O6 of the present invention still maintain a good level of electrochemical stability, and the safety performance as a solid electrolyte is guaranteed. Substituting homologous elements for one or both of Al and Si in such materials can further improve the conductivity.

Description

Technical Field

[0001] The invention belongs to the technical field of solid electrolytes, and in particular relates to an aluminosilicate lithium ion solid electrolyte and a preparation method thereof. Background Art

[0002] At present, with the gradual popularization of new energy electric vehicles and the continuous development of portable electronic devices, people's requirements for the performance and safety of lithium-ion batteries are also increasing. As a representative of commercial secondary batteries, traditional lithium-ion batteries use organic liquid electrolytes with safety hazards such as leakage, spontaneous combustion, and even explosion, which is an important factor restricting the development of the new energy industry. As an important component of lithium-ion batteries, electrolytes directly affect the battery's capacity, internal resistance, rate charge and discharge performance, operating temperature range, cycle life and safety performance. Electrolytes with excellent performance can greatly improve the comprehensive performance of lithium batteries. In recent years, all-solid-state batteries based on solid electrolytes have attracted much attention. They can use lithium metal as an anode. In addition, solid electrolytes avoid the use of diaphragms and organic electrolytes, greatly improving the energy density and safety of secondary batteries. They are regarded as an important development direction for the new generation of energy storage systems.

[0003] Solid electrolytes are an extremely important part of all-solid-state batteries. They are currently divided into three categories: polymer electrolytes, sulfide electrolytes, and oxide electrolytes. Polymer solid electrolytes are mainly composed of polymer substrates and lithium salts. The most representative ones are polyethylene oxide (PEO) and its derivative-based polymer solid electrolytes, but their conductivity at room temperature is still low, which has become an obstacle to their large-scale commercialization. Sulfide solid electrolytes also have high lithium ion conductivity at room temperature, and they have good mechanical formability and are very suitable for processing into full batteries. However, sulfide materials easily react with moisture in the air to generate harmful H2S gas, and poor electrochemical stability has become the biggest obstacle to their widespread use in the production of safe all-solid-state batteries. Oxide solid electrolytes have many advantages, including low sensitivity to moisture in the air, high energy density, and good electrochemical stability, but their low lithium ion conductivity at room temperature hinders their widespread application. Therefore, studying solid electrolytes with excellent lithium ion conductivity and excellent stability at room temperature is of great significance to the development of all-solid-state batteries.

[0004] In recent years, lithium aluminosilicate material systems have been considered as lithium ion conductors, and thus are expected to be used as solid electrolytes. It is reported that spodumene (β-LiAlSi2O6) exhibits isotropic lithium ion conductivity, excellent thermal stability and mechanical stability. However, β-spodumene exhibits relatively low room temperature lithium ion conductivity (less than 10 -10S / cm) and a high lithium ion diffusion barrier (about 0.8 eV), which makes their performance less than ideal as solid electrolytes.

[0005] Through the above analysis, the problems and defects of the prior art are as follows:

[0006] (1) Existing polymer solid electrolytes and oxide solid electrolytes have low conductivity at room temperature.

[0007] (2) The sulfide materials of existing sulfide solid electrolytes easily react with moisture in the air to generate harmful H2S gas, and have poor electrochemical stability.

[0008] (3) β-LiAlSi2O6 material has excellent electrochemical stability and thermal stability, but its lithium ion conductivity is relatively low, which limits its further application. Summary of the invention

[0009] In view of the problems existing in the prior art, the present invention provides an aluminosilicate lithium ion solid electrolyte and a preparation method thereof.

[0010] The present invention is achieved by providing an aluminosilicate lithium ion solid electrolyte, wherein the aluminosilicate lithium ion solid electrolyte is spodumene and its derivative system, and the chemical formula is: Li 1-x Al 1-x Si 2+x O6; wherein, the value range of x is -1.00 to 0.5 and x≠0.

[0011] Furthermore, when x is taken as -1.00, the aluminosilicate lithium ion solid electrolyte is Li2Al2SiO6.

[0012] Furthermore, when x is -0.75, the aluminosilicate lithium ion solid electrolyte is Li 1.75 Al 1.75 Si 1.25 O6.

[0013] Furthermore, when x is -0.5, the aluminosilicate lithium ion solid electrolyte is Li 1.5 Al 1.5 Si 1.5 O6.

[0014] Furthermore, when x is -0.25, the aluminosilicate lithium ion solid electrolyte is Li 1.25 Al 1.25 Si 1.75 O6.

[0015] Furthermore, when x is 0.25, the aluminosilicate lithium ion solid electrolyte is Li 0.75 Al 0.75 Si2.25 O6.

[0016] Furthermore, when x is 0.5, the aluminosilicate lithium ion solid electrolyte is Li 0.5 Al 0.5 Si 2.5 O6.

[0017] Furthermore, by replacing Al or Si with elements of the same group, Al can be replaced by B or Ga or In or Ta, and Si can be replaced by C or Ge or Sn or Pb, a solid electrolyte Li can be obtained. 1-x A 1-x B 2+x O6, A=B,Al,Ga,In,Ta; B=C,Si,Ge,Sn,Pb.

[0018] Another object of the present invention is to provide a primary lithium ion battery solid electrolyte, wherein the primary lithium ion battery solid electrolyte is made of the aluminosilicate lithium ion solid electrolyte.

[0019] Another object of the present invention is to provide a secondary lithium-ion battery solid electrolyte, wherein the secondary lithium-ion battery solid electrolyte is made from the aluminosilicate lithium-ion solid electrolyte.

[0020] Another object of the present invention is to provide a method for preparing the aluminosilicate lithium ion solid electrolyte, the method comprising: replacing the Al and Si elements in the original LiAlSi2O6, determining the ratio of the Al and Si elements, and obtaining the aluminosilicate lithium ion solid electrolyte as Li 1-x Al 1-x Si 2+x O6, x=0.5, 0.25, -0.25, -0.5, -0.75 or -1.00.

[0021] In combination with the above technical solutions and the technical problems solved, please analyze the advantages and positive effects of the technical solutions to be protected by the present invention from the following aspects:

[0022] First, in view of the technical problems existing in the above-mentioned prior art and the difficulty of solving the problems, the technical solutions to be protected by the present invention and the results and data during the research and development process are closely combined to analyze in detail and deeply how the technical solutions of the present invention solve the technical problems, and some creative technical effects brought about after solving the problems. The specific description is as follows:

[0023] Based on first principles and ab initio molecular dynamics, the present invention analyzes the influence of different content ratios of Al and Si in β-LiAlSi2O6 material on its lithium ion conductivity properties. In the field of energy, the present invention can be used as a solid electrolyte for lithium ion batteries, including primary batteries and secondary batteries.

[0024] The purpose of the present invention is to improve the lithium ion conductivity of β-LiAlSi2O6 by adjusting the content ratio of Al / Si elements in the material. In order to analyze the optimal ratio of Al / Si elements, the present invention replaces Al and Si elements in the original β-LiAlSi2O6, thereby constructing a material system, namely Li 1-x Al 1-x Si 2+x O6 (x = 0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00). The present invention adopts ab initio molecular dynamics simulation calculation method based on density functional theory to analyze Li 1-x Al 1-x Si 2+x Conductivity of lithium ions in O6.

[0025] It can be seen from the experimental results that the Li 1-x Al 1-x Si 2+x The band gap of O6 unit cell is generally large (greater than 3.5eV), indicating that its structure has good electrochemical stability. Its application in solid electrolyte can effectively inhibit the shuttle of electrons in it and avoid the occurrence of battery self-discharge. 1-x Al 1-x Si 2+x During the ab initio molecular dynamics simulation of the O6 material system at high temperature, the crystal structure skeleton remains intact, indicating that it has good thermal stability. 1-x Al 1-x Si 2+x The x value in O6 is negative, that is, the ratio of Al to Si increases. When the unit cell turns into a lithium-rich structure, the conductivity at room temperature is improved by several orders of magnitude compared with the original structure. Among them, Li2Al2SiO6 has the lowest lithium ion migration barrier and the best conductivity performance.

[0026] Second, considering the technical solution as a whole or from the perspective of the product, the technical effects and advantages of the technical solution to be protected by the present invention are described in detail as follows:

[0027] (1) By adjusting the ratio of Al to Si in LiAlSi2O6, the Li 1-x Al 1-x Si 2+xO6 (x = 0.5, 0.25, 0, -0.25, -0.5, -0.75 or -1.00) material system, the present invention is compared with the original LiAlSi2O6, Li 1-x Al 1-x Si 2+x The O6 (x≠0) system has better lithium ion conductivity at room temperature.

[0028] (2) A series of materials obtained by changing the ratio of Al to Si in LiAlSi2O6 still maintain a good level of electrochemical stability, and their safety performance as solid electrolytes is guaranteed.

[0029] (3) Compared with the original spodumene LiAlSi2O6, when the Al / Si value is increased (i.e. Li 1-x Al 1-x Si 2+x O6) the migration barrier of lithium ions will be significantly reduced. The migration barrier of lithium ions in Li2Al2SiO6 is reduced by about 40%, which is a significant decrease. Its lithium ion conductivity at room temperature is also significantly improved.

[0030] Third, as auxiliary evidence of the inventiveness of the claims of the present invention, it is also reflected in the expected benefits and commercial value after the technical solution of the present invention is transformed into:

[0031] The invention provides a design method of a silicate solid electrolyte, which has high lithium ion conductivity and cheap raw materials, and can greatly reduce the manufacturing cost of the solid electrolyte. BRIEF DESCRIPTION OF THE DRAWINGS

[0032] In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the following briefly introduces the drawings required for use in the embodiments of the present invention. Obviously, the drawings described below are only some embodiments of the present invention. For ordinary technicians in this field, other drawings can be obtained based on these drawings without creative work.

[0033] Figure 1 is a flow chart of a design method of aluminosilicate lithium ion solid electrolyte provided by an embodiment of the present invention;

[0034] Figure 2 is Li provided in the embodiment of the present invention 1-x Al 1-x Si 2+x Crystal structure diagram of O6 (x=0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00) material system;

[0035] Figure 3 is Li provided in the embodiment of the present invention0.5 Al 0.5 Si 2.5 Total electronic state density diagram of O6 material;

[0036] Figure 4 is Li provided in the embodiment of the present invention 0.75 Al 0.75 Si 2.25 Total electronic state density diagram of O6 material;

[0037] Figure 5 is a total electronic state density diagram of the LiAlSi2O6 material provided by an embodiment of the present invention;

[0038] Figure 6 is Li provided in the embodiment of the present invention 1.25 Al 1.25 Si 1.75 Total electronic state density diagram of O6 material;

[0039] Figure 7 is Li provided in the embodiment of the present invention 1.5 Al 1.5 Si 1.5 Total electronic state density diagram of O6 material;

[0040] Figure 8 is Li provided in the embodiment of the present invention 1.75 Al 1.75 Si 1.25 Total electronic state density diagram of O6 material;

[0041] Fig. 9 is a total electronic state density diagram of the Li2Al2SiO6 material provided by an embodiment of the present invention;

[0042] Fig.10 is a graph of the average mean square displacement of lithium ions at different temperatures of the Li2Al2SiO6 material provided by an embodiment of the present invention;

[0043] Fig.11 is Li provided in the embodiment of the present invention 1-x Al 1-x Si 2+x The conductivity of the material system O6 (x=0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00) changes with temperature;

[0044] Fig.12 is Li provided in the embodiment of the present invention 1-x Al 1-x Si 2+xThe lithium ion migration barrier and room temperature conductivity of the O6 (x=0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00) material system vary with x value;

[0045] Fig.13 is Li provided in the embodiment of the present invention 1-x Al 1-x Si 2+x The trend of lithium ion diffusion channel size changing with x value in O6 (x=0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00) material system.

[0046] Fig.14 is Li provided in the embodiment of the present invention 1-x Al 1-x (Si 1-y Ge y ) 2+x The conductivity variation with temperature of O6 (x=0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00, 0≤y≤1) material system and the lithium ion migration barrier and conductivity variation with y value at room temperature; DETAILED DESCRIPTION

[0047] In order to make the purpose, technical solution and advantages of the present invention more clearly understood, the present invention is further described in detail below in conjunction with the embodiments. It should be understood that the specific embodiments described herein are only used to explain the present invention and are not used to limit the present invention.

[0048] In view of the problems existing in the prior art, the present invention provides an aluminosilicate lithium ion solid electrolyte and a design method thereof. The present invention is described in detail below in conjunction with the accompanying drawings.

[0049] 1. Explanatory Examples In order to enable those skilled in the art to fully understand how to implement the present invention, this section provides an illustrative example that expands and describes the technical solution of the claims.

[0050] The aluminosilicate lithium ion solid electrolyte provided in the embodiment of the present invention is spodumene and its derivative system, and the chemical formula is: Li 1-x Al 1-x Si 2+x O6; wherein x = 0.5, 0.25, -0.25, -0.5, -0.75 or -1.00.

[0051] The optimal ratio of the solid electrolyte provided by the embodiment of the present invention comprises the following components:

[0052] Li 0.5 Al 0.5 Si 2.5O6;

[0053] Li 0.75 Al 0.75 Si 2.25 O6;

[0054] Li 1.25 Al 1.25 Si 1.75 O6;

[0055] Li 1.5 Al 1.5 Si 1.5 O6;

[0056] Li 1.75 Al 1.75 Si 1.25 O6;

[0057] Li2Al2SiO6.

[0058] The present invention also provides a method for preparing aluminosilicate lithium ion solid electrolyte, comprising: constructing a material system by replacing Al and Si elements in the original β-LiAlSi2O6, and determining the optimal ratio of Al / Si element content: Li 1-x Al 1-x Si 2+x O6, x = 0.5, 0.25, 0, -0.25, -0.5, -0.75 or -1.00; the ab initio molecular dynamics simulation method based on density functional theory was used to analyze the Li 1-x Al 1-x Si 2+x Conductivity of lithium ions in O6.

[0059] Example 1

[0060] In the embodiment of the present invention, the content ratio of Al / Si in β-LiAlSi2O6 material is adjusted to improve the conductivity of lithium ions. In order to analyze the optimal ratio of Al / Si content, the present invention replaces Al and Si in the original β-LiAlSi2O6, thereby constructing a material system, namely Li 1-x Al 1-x Si 2+x O6 (x = 0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00). The ab initio molecular dynamics simulation method based on density functional theory was used to analyze the Li 1- x Al 1-x Si 2+x Conductivity of lithium ions in O6.

[0061] (1) Figure 1 As shown, the purpose of the present invention provided by the embodiment of the present invention is to provide Li 1-x Al 1-x Si 2+x The design method for the optimal ratio of O6 elements includes the following steps:

[0062] S101, establish Li with different Al / Si content 1-x Al 1-x Si 2+x O6 model, and the constructed models were structurally optimized, with the lattice parameters and ion positions fully relaxed;

[0063] S102, based on structural optimization, the electronic state density of the constructed unit cell model was calculated, and the Li 1-x Al 1-x Si 2+x Electrochemical stability of O6 as a solid electrolyte;

[0064] S103, calculate the conductivity properties of materials according to the Nernst-Einstein equation, and use the Zeo++ program to calculate the Li 1-x Al 1-x Si 2+x The lithium ion diffusion channel of the O6 system was measured.

[0065] (2) In step S101 provided in the embodiment of the present invention, the constructed model is structurally optimized, and the lattice parameters and ion positions are completely relaxed until the total energy and ion force are less than 10 -5 eV and Optimized Li 1- x Al 1-x Si 2+x The crystal structure of O6 is as follows Figure 2 shown.

[0066] (3) In step S102 provided in the embodiment of the present invention, in order to analyze Li 1-x Al 1-x Si 2+x The electrochemical stability of O6 as a solid electrolyte was analyzed from the perspective of the electronic structure of the material by calculating the electronic state density of the constructed unit cell model based on its structural optimization. Figures 3 to 9 As shown in Figure 2, the band gap of undoped LiAlSi2O6 is around 4.5 eV. The high band gap indicates that it has very good electrochemical stability. 1-x Al 1- x Si 2+xO6 can be divided into two cases. When x is greater than 0, that is, lithium-poor state, the band gap tends to decrease with the increase of x. When x is less than 0, that is, lithium-rich state, the band gap also decreases with the decrease of x value. However, the band gap of all materials is greater than 3.5eV, indicating that the Li obtained by adjusting the ratio of Al to Si in LiAlSi2O6 1-x Al 1-x Si 2+x O6 (x=0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00) materials all have good electrochemical stability.

[0067] (4) In step S103 provided in the embodiment of the present invention, the lithium ion conductivity property of the material is calculated according to the following Nernst-Einstein equation:

[0068]

[0069] Among them, σ is the conductivity, n is the number density of lithium ions, e is the charge of the elementary charge, Z is the valence state of a single lithium ion, k B is the Boltzmann constant, T is the temperature, and D is the diffusion coefficient of lithium ions. All physical quantities except the diffusion coefficient D can be obtained from the unit cell parameters and the calculation simulation parameters. Where MSD is the average mean square displacement of lithium ion diffusion, which can be calculated by ab initio molecular dynamics simulation. The larger the ratio of the average mean square displacement value to time, the larger the diffusion coefficient of lithium ions and the corresponding greater the lithium ion conductivity.

[0070] (5) Fig.10 Shows Li 1-x Al 1-x Si 2+x When x in O6 is -1 (i.e. Li2Al2SiO6), the average mean square displacement of lithium ions changes with time at different temperatures. The results show that the higher the temperature, the greater the ratio of the average mean square displacement to time, that is, the greater the diffusion coefficient of lithium ions, indicating that the conductivity of lithium ions is affected by temperature. The higher the temperature, the greater the conductivity of lithium ions.

[0071] (6) For the Nernst-Einstein equation Taking the logarithm of both sides and transforming them, we get in Plotting The lithium ion migration barrier E is calculated from the slope of the graph. aThe value of, where the smaller the slope, the larger the migration barrier; set the simulation temperature to 1073K ~ 2273K, the temperature interval is 200K; plot the data of multiple temperature points, and deduce the size of the migration barrier from the size of the slope. The migration barrier is the energy required for lithium ion migration. The larger the migration barrier, the more difficult it is for lithium ions to migrate, and the correspondingly lower the lithium ion conductivity. The smaller the migration barrier of lithium ions, the better the conductivity of lithium ions.

[0072] (7) Ionic conductivity is a key factor in determining the internal resistance and rate performance of batteries. 1-x Al 1-x Si 2+x The lithium ion conductivity of the O6 material system in the temperature range of 1073K to 2273K is linearly extrapolated from the high temperature data to the lithium ion conductivity at room temperature 300K; the original LiAlSi2O6 has the lowest calculated lithium ion conductivity at room temperature, and when x is positive, the lithium ion conductivity at room temperature increases; when x is negative, the lithium ion concentration of the material increases, and the lithium ion conductivity at room temperature increases significantly; among them, Li2Al2SiO6 has the best lithium ion conductivity performance at room temperature.

[0073] (8) Fig.12 Summarizes Li 1-x Al 1-x Si 2+x The lithium ion migration barrier of the O6 (x=0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00) system and the change trend of lithium ion conductivity at room temperature with the value of x. The lithium ion migration barrier is the highest in the original LiAlSi2O6. When x is a positive value (i.e., the Si / Al ratio increases), the migration barrier decreases as the Si / Al ratio increases. When x is a negative value (i.e., the Al / Si ratio increases), the migration barrier decreases as the Al / Si ratio increases, and the minimum value appears at x=-1.0, indicating that the barrier that needs to be overcome for the diffusion of lithium ions in Li2Al2SiO6 is the lowest, and lithium ions are easier to migrate in this material, so the lithium ion conductivity performance of this material is the best.

[0074] (9) The size of the lithium ion transmission channel also affects the conductivity of lithium ions. Fig.13 To use Zeo++ program to 1-x Al 1-x Si 2+x The measurement results of the lithium ion diffusion channel of the O6 (x=0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00) system. As shown in the figure, compared with the original LiAlSi2O6, the lithium ion transmission channel of Li2Al2SiO6 (i.e. when x=-1.0) is significantly improved, which is also the reason why it has higher lithium ion conductivity.

[0075] (10) After adopting the above technical solution, the ratio of Al to Si in LiAlSi2O6 was adjusted to predict the Li 1-x Al 1- x Si 2+x O6 (x = 0.5, 0.25, 0, -0.25, -0.5, -0.75, -1.00) material system, compared with the original LiAlSi2O6, Li 1-x Al 1-x Si 2+x The O6 (x≠0) system has better lithium ion conductivity at room temperature.

[0076] The embodiments of the present invention obtain a series of materials by changing the ratio of Al to Si in LiAlSi2O6, and their electrochemical stability still maintains a good level, and their safety performance as solid electrolytes is guaranteed.

[0077] Compared with the original spodumene LiAlSi2O6, the present invention increases the value of Al / Si (i.e. Li 1-x Al 1-x Si 2+x O6) the migration barrier of lithium ions will be significantly reduced. The migration barrier of lithium ions in Li2Al2SiO6 is reduced by about 40%, which is a significant decrease. Its lithium ion conductivity at room temperature is also significantly improved.

[0078] Example 2

[0079] The implementation method is similar to that of Example 1, except that Li 1-x Al 1-x Si 2+x The Si element in O6 is partially or completely replaced by its homologous elements to obtain Li 1-x Al 1-x (Si 1-y Ge y ) 2+x O6(x=0.5,0.25,0,-0.25,-0.5,-0.75,-1.00,0≤y≤1). Fig.14 As shown in Figure 2, with the increase of Ge content, the conductivity of the electrolyte can be improved by nearly 1 order of magnitude.

[0080] The above description is only a specific implementation mode of the present invention, but the protection scope of the present invention is not limited thereto. Any modifications, equivalent substitutions and improvements made by any technician familiar with the technical field within the technical scope disclosed by the present invention and within the spirit and principle of the present invention should be covered by the protection scope of the present invention.

Claims

1. A lithium-ion aluminosilicate solid electrolyte, characterized in that: The aluminosilicate lithium ion solid electrolyte is a spodumene derivative system, and the chemical formula is: Li 1-x Al 1-x Si 2+x O6; where x ranges from -1.00 to 0.5, and x≠0.

2. The aluminosilicate lithium ion solid electrolyte according to claim 1, characterized in that When the value of x is -1.00, the aluminosilicate lithium ion solid electrolyte is Li2Al2SiO6.

3. The aluminosilicate lithium ion solid electrolyte according to claim 1, characterized in that x is -0.75, then the aluminosilicate lithium ion solid electrolyte is Li 1.75 Al 1.75 Si 1.25 O6.

4. The aluminosilicate lithium ion solid electrolyte according to claim 1, characterized in that x is -0.5, then the aluminosilicate lithium ion solid electrolyte is Li 1.5 Al 1.5 Si 1.5 O6.

5. The aluminosilicate lithium ion solid electrolyte according to claim 1, characterized in that x is -0.25, then the aluminosilicate lithium ion solid electrolyte is Li 1.25 Al 1.25 Si 1.75 O6.

6. The aluminosilicate lithium ion solid electrolyte according to claim 1, characterized in that When x is 0.25, the aluminosilicate lithium ion solid electrolyte is Li 0.75 Al 0.75 Si 2.25 O6.

7. The aluminosilicate lithium ion solid electrolyte according to claim 1, characterized in that When x is 0.5, the aluminosilicate lithium ion solid electrolyte is Li 0.5 Al 0.5 Si 2.5 O6.

8. The aluminosilicate lithium ion solid electrolyte according to claim 1, characterized in that By replacing Al or Si with elements of the same group, replacing Al with B or Ga or In or Ta, and replacing Si with C or Ge or Sn or Pb, a solid electrolyte Li is obtained. 1-x A 1- x B 2+x O6, A=B,Al,Ga,In,Ta; B=C,Si,Ge,Sn,Pb.

9. A solid electrolyte for a primary lithium-ion battery, characterized in that: The primary lithium-ion battery solid electrolyte is made of the aluminosilicate lithium-ion solid electrolyte according to any one of claims 1 to 8.

10. A solid electrolyte for a secondary lithium-ion battery, characterized in that: The secondary lithium-ion battery solid electrolyte is made of the aluminosilicate lithium-ion solid electrolyte according to any one of claims 1 to 8.

11. A method for preparing the aluminosilicate lithium ion solid electrolyte according to any one of claims 1 to 8, characterized in that: The preparation method of the aluminosilicate lithium ion solid electrolyte comprises: replacing the Al and Si elements in the original LiAlSi2O6, determining the ratio of the Al and Si elements, and obtaining the aluminosilicate lithium ion solid electrolyte as Li 1-x Al 1-x Si 2+x O6, x=0.5, 0.25, -0.25, -0.5, -0.75 or -1.00.

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