A monovalent ion-conducting polymer based on organosilicate salt, and a preparation method and application thereof

Abstract

The application provides a single-ion conductive polymer based on an organic silicate salt and a preparation method and application thereof. The main raw material of the organic silicate salt polymer provided by the application is silicon tetrachloride which is low in price and polyethylene glycol with different molecular weights, and the single-ion conductive polymer of the organic silicate salt is obtained after polymerization, hydrolysis and lithiation. The structure of Si-O-C as the main chain improves the flexibility of the material, and a new anion group is adopted, so that the material selection is provided for a full-solid single-ion electrolyte.

Description

Technical Field

[0001] This invention belongs to the field of polymer solid electrolyte materials, and particularly relates to a single-ion conductive polymer based on organosilicon salts, its preparation method, and its application. Specifically, it relates to the preparation of one-dimensional chain, two-dimensional network, and three-dimensional cross-linked polymers of organosilicon salts and their application in single-ion organic polymer solid electrolytes. Background Technology

[0002] The rapid development of lithium-ion batteries has led to their dominance in portable devices and the consumer electronics market, and in recent years they have expanded into new energy vehicles and the power grid. At the same time, market demands for lithium-ion batteries to achieve both high rate performance and safety are constantly increasing. Traditional lithium-ion batteries use organic liquid electrolytes; however, organic solvents have drawbacks such as easy leakage, volatility, and flammability. Furthermore, the insertion and extraction of lithium ions in liquid batteries can lead to the formation of lithium dendrites, which can further cause short circuits and even explosions. Therefore, the development of solid-state electrolytes is of great significance for the development of efficient and safe lithium-ion batteries.

[0003] Common solid-state electrolyte materials mainly include inorganic solid-state electrolytes, organic solid-state electrolytes, and organic-inorganic composite electrolytes. Liang et al. reported the use of inorganic lithium iodide films as solid-state electrolytes in 1969, which attracted widespread attention. Subsequently, oxides and sulfides became the main inorganic materials studied. However, inorganic materials suffer from drawbacks such as poor flexibility and high interfacial impedance between the electrolyte and the electrode. Organic electrolytes typically use a polymer matrix as the solid matrix for lithium salts. Compared to inorganic materials, the presence of polymers can more effectively prevent the formation of lithium dendrites and reduce the interfacial impedance between the electrolyte and the electrode. Most organic polymer electrolytes mix lithium salts into the polymer matrix, but it is difficult to achieve the desired ionic conductivity. Organic-inorganic composite electrolytes are obtained by dispersing inorganic fillers with high surface activity or high ionic conductivity in a polymer electrolyte. Many inorganic fillers can be selected, such as SiO2, ZrO2, and ceramic powders. The addition of inorganic fillers significantly improves the conductivity of the electrolyte. However, the lithium ion transference number remains low, and the migration of anions leads to concentration polarization, thereby reducing the battery capacity and cycle performance.

[0004] In order to enable solid electrolytes to simultaneously possess high lithium-ion transference numbers (t) Li+ Due to their excellent properties such as ≈1 and low interfacial impedance, single-ion polymer solid electrolytes have become a research focus. The structural feature of single-ion polymers is that anions are fixed on the polymer chains, which restricts the movement of anions and thus increases the lithium-ion transference number, thereby improving the cycle performance of the battery.

[0005] Despite significant progress in the fundamental research of single-ion solid electrolytes, their applications are still in their early stages. The following aspects still require further research and exploration: (1) How to improve the efficiency of Li... + (2) How to improve the mechanical properties of the electrolyte and solve the problem of interface contact between the solid electrolyte and the electrode. Summary of the Invention

[0006] In view of this, the present invention aims to propose a single-ion conductive polymer based on organosilicon salts. This conductive polymer is a novel silicate-based anionic conductive polymer, and the anion reacts with Li... + The binding force is relatively weak, which is beneficial to Li + The ionization of the conductive polymer results in high conductivity at room temperature; moreover, the conductive polymer possesses excellent mechanical properties such as plasticity, flexibility, and tensile strength, which can solve the problem of interfacial contact between solid electrolytes and electrodes.

[0007] To achieve the above objectives, the technical solution created by this invention is implemented as follows:

[0008] A single-ion conductive polymer based on an organosilicon ester salt has the following structural formula:

[0009]

[0010] Formula (1) is a one-dimensional chain-like single-ion conductive polymer; Formula (2) is a two-dimensional network-like single-ion conductive polymer; Formula (3) is a three-dimensional cross-linked single-ion conductive polymer.

[0011] In the above formulas, x = 1, 2, 3, 4...; n = 1, 2, 3, 4...; m = 1, 2, 3, 4...

[0012] Another objective of this invention is to provide a method for preparing a single-ion conductive polymer based on organosilicon salts.

[0013] To achieve the above objectives, the technical solution created by this invention is implemented as follows:

[0014] Preparation of one-dimensional chain-like single-ion conductive polymer (p-1SiOROLi):

[0015] In an organic solvent and under a gaseous atmosphere, SiCl4 with an S1:1:1 equivalent and polyethylene glycol with a fixed molecular weight undergo a polymerization reaction to obtain a polymer.

[0016] S2: Expose the polymer obtained in S1 to air for 1 hour. After complete hydrolysis, filter to obtain the hydrolysis product.

[0017] S3: The hydrolysis product obtained in S2 is lithiated using a lithiation reagent in an organic solvent and under a gaseous atmosphere to obtain a one-dimensional chain-like single-ion conductive polymer.

[0018] The organic solvents mentioned in step S1 include ethylene glycol dimethyl ether, diethylene glycol dimethyl ether, tetrahydrofuran, and 1,3-oxocyclopentane; the gas atmosphere is nitrogen or an inert gas.

[0019] The organic solvents mentioned in step S3 include dichloromethane, tetrahydrofuran, and ethylene glycol dimethyl ether; the gas atmosphere is nitrogen or an inert gas; the lithium-ionizing agents include n-butyllithium, tert-butyllithium, tert-butoxide lithium, phenyllithium, and lithium hydroxide.

[0020] Preparation of a two-dimensional network single-ion conductive polymer (p-2SiOROLi):

[0021] A polymer is obtained by polymerizing SiCl4 with an S1:1:1.5 equivalent ratio and polyethylene glycol with a fixed molecular weight in an organic solvent and under a gaseous atmosphere.

[0022] S2: Expose the polymer obtained in S1 to air for 1 hour. After complete hydrolysis, filter to obtain the hydrolysis product.

[0023] S3: The hydrolysis product obtained in S2 is lithiated using a lithiation reagent in an organic solvent and under a gaseous atmosphere to obtain a two-dimensional network single-ion conductive polymer.

[0024] The organic solvents mentioned in step S1 include ethylene glycol dimethyl ether, diethylene glycol dimethyl ether, tetrahydrofuran, and 1,3-oxocyclopentane; the gas atmosphere is nitrogen or an inert gas.

[0025] The organic solvents mentioned in step S3 include dichloromethane, tetrahydrofuran, and ethylene glycol dimethyl ether; the gas atmosphere is nitrogen or an inert gas; the lithium-ionizing agents include n-butyllithium, tert-butyllithium, tert-butoxide lithium, phenyllithium, and lithium hydroxide.

[0026] Preparation of a three-dimensional cross-linked single-ion conductive polymer (p-3SiOROLi):

[0027] In an organic solvent and under a gaseous atmosphere, SiCl4 with an S1:1:2 equivalent ratio and polyethylene glycol with a fixed molecular weight undergo a polymerization reaction to obtain a polymer.

[0028] S2: Expose the polymer obtained in S1 to air for 1 hour. After complete hydrolysis, filter to obtain the hydrolysis product.

[0029] S3: The hydrolysis product obtained in S2 is lithiated using a lithiation reagent in an organic solvent and under a gaseous atmosphere to obtain a two-dimensional network single-ion conductive polymer.

[0030] The organic solvents mentioned in step S1 include ethylene glycol dimethyl ether, diethylene glycol dimethyl ether, tetrahydrofuran, and 1,3-oxocyclopentane; the gas atmosphere is nitrogen or an inert gas.

[0031] The organic solvents mentioned in step S3 include dichloromethane, tetrahydrofuran, and ethylene glycol dimethyl ether; the gas atmosphere is nitrogen or an inert gas; the lithium-ionizing agents include n-butyllithium, tert-butyllithium, tert-butoxide lithium, phenyllithium, and lithium hydroxide.

[0032] Another objective of this invention is to propose applications of single-ion conductive polymers based on organosilicon salts.

[0033] To achieve the above objectives, the technical solution created by this invention is implemented as follows:

[0034] A solid electrolyte film, characterized in that it comprises two layers of aluminum foil, with a single-ion conductive polymer based on an organosilicon ester salt sandwiched between the two layers of aluminum foil as described above.

[0035] Furthermore, the preparation method of the above-mentioned solid electrolyte thin film includes the following steps:

[0036] S1: Lay the single-ion conductive polymer flat on aluminum foil and cover the surface with another aluminum foil;

[0037] S2: Place the material obtained in S1 flat between the two heated aluminum blocks;

[0038] S3: The material obtained in S1 is heated to 100°C by applying pressure to it through two heating aluminum blocks and maintained for 10 minutes to obtain a single-ion conductive polymer solid electrolyte film.

[0039] Furthermore, the aforementioned solid electrolyte film can be applied to lithium solid-state batteries.

[0040] Furthermore, a lithium solid-state battery includes a positive electrode sheet, a negative electrode sheet, and a solid electrolyte film as described above, wherein the solid electrolyte film is located between the positive electrode sheet and the negative electrode sheet; the positive electrode sheet, the solid electrolyte film, and the negative electrode sheet are encapsulated in a battery casing composed of a positive electrode shell and a negative electrode shell.

[0041] The positive electrode material includes lithium iron phosphate, lithium cobalt oxide, lithium nickel oxide, lithium manganese oxide, ternary materials, lithium-rich materials, oxide materials, sulfur positive electrode, and air positive electrode; the negative electrode is metallic lithium.

[0042] Compared with existing technologies, the single-ion conductive polymer based on organosilicon ester salt, its preparation method, and its application described in this invention have the following advantages:

[0043] (1) The polymer solid electrolyte described in this invention has good conductivity at room temperature.

[0044] (2) The polymer solid electrolyte of the present invention has good flexibility to solve the problem of interface contact between solid electrolyte and electrode. Attached Figure Description

[0045] Figure 1 This is the synthetic route for the one-dimensional chain-like single-ion conductive polymer in this invention.

[0046] Figure 2 This is the synthetic route for the two-dimensional network single-ion conductive polymer in this invention.

[0047] Figure 3 This is the synthetic route for the three-dimensional cross-linked single-ion conductive polymer in this invention.

[0048] Figure 4 The infrared spectra of p-3SiOROH1, p-3SiOROH2, and p-3SiOROH3 in this invention are shown.

[0049] Figure 5 This is the DSC diagram of p-3SiOROH3 in this invention.

[0050] Figure 6 The images shown are actual pictures of p-3SiOROH1, p-3SiOROH2, and p-3SiOROH3 in this invention.

[0051] Figure 7 This is the X-ray photoelectron spectrum of the 1s and 2p orbitals of p-3SiOROLi2 in this invention.

[0052] Figure 8 This is the electrochemical impedance spectroscopy (EIS) spectrum of p-3SiOROLi1 in this invention.

[0053] Figure 9 This is a schematic diagram of a lithium solid-state battery structure according to the present invention. Detailed Implementation

[0054] Unless otherwise defined, the technical terms used in the following embodiments have the same meanings as commonly understood by those skilled in the art to which this invention pertains. Unless otherwise specified, the experimental reagents used in the following embodiments are conventional biochemical reagents; and the experimental methods described are conventional methods.

[0055] The present invention will now be described in detail with reference to embodiments and accompanying drawings. This description is intended to enable those skilled in the art to make and use the invention, and is provided in the context of specific applications and their requirements. It will be apparent to those skilled in the art that various modifications can be made to the disclosed embodiments. Furthermore, the general principles defined in this invention can be applied to other embodiments and application scenarios without departing from the spirit and scope of the invention. Therefore, the present invention is not limited to the disclosed embodiments, but should be given the broadest scope consistent with the scope of the invention patent.

[0056] Example 1: Synthesis of a one-dimensional chain-like single-ion conductive polymer (p-1SiOROLi1)

[0057] When using polyethylene glycol (PEG150) with a molecular weight of 150, the degree of polymerization of polyethylene glycol is 3. The specific synthesis method is as follows:

[0058] 0.75 g (5 mmol) of PEG150 was added to a two-necked round-bottom flask under a nitrogen atmosphere, followed by 20 mL of dimethyl ethylene glycol ether (DME) solvent. After elution with nitrogen three times, SiCl4 (0.57 mL, 5 mmol) was slowly added dropwise while stirring at 0 °C. After reacting for 4 hours, the flask was exposed to air for 1 hour (Si-Cl bonds can be hydrolyzed in trace amounts of water). After complete hydrolysis, the mixture was filtered to obtain 0.6 g of white solid as the hydrolysis product p-1SiOROH1. The hydrolysis product was transferred to a two-necked flask and dried under vacuum at 60 °C for 12 hours. 20 mL of anhydrous dichloromethane (DCM) was added, and after elution with nitrogen three times, 2.2 mL of n-butyllithium (2.5 mol / L n-hexane solution) was slowly added dropwise while stirring at 0 °C. After reacting for 12 hours, the solvent was removed under reduced pressure under anhydrous and oxygen-free conditions to obtain the white solid as the target product p-1SiOROLi1.

[0059] The preparation method of p-1SiOROLi1 single-ion solid electrolyte is as follows:

[0060] Approximately 50 mg of p-1SiOROLi1 polymer was spread evenly on an aluminum foil, and the surface was covered with another aluminum foil. The aluminum foil was then placed flat between two heated aluminum blocks. While applying pressure, the two heated aluminum blocks were heated to 100°C and maintained for 10 minutes to obtain a p-1SiOROLi1 solid electrolyte film.

[0061] Example 2: Synthesis of a two-dimensional network single-ion conductive polymer (p-2SiOROLi1)

[0062] When polyethylene glycol (PEG150) with a molecular weight of 150 was used, the degree of polymerization of polyethylene glycol was 3. The specific synthesis method is as follows:

[0063] 0.9 g (6 mmol) of PEG150 was added to a two-necked round-bottom flask under a nitrogen atmosphere, followed by 20 mL of dimethyl ethylene glycol ether (DME) solvent. After elution with nitrogen three times, SiCl4 (0.46 mL, 4 mmol) was slowly added dropwise while stirring at 0 °C. After reacting for 4 hours, the flask was exposed to air for 1 hour (Si-Cl bonds can be hydrolyzed in trace amounts of water). After complete hydrolysis, the mixture was filtered to obtain 0.6 g of white solid as the hydrolysis product p-2SiOROH1. The hydrolysis product was transferred to a two-necked flask and dried under vacuum at 60 °C for 12 hours. 20 mL of anhydrous dichloromethane (DCM) was added, and after elution with nitrogen three times, 0.8 mL of n-butyllithium (2.5 mol / L n-hexane solution) was slowly added dropwise while stirring at 0 °C. After reacting for 12 hours, the solvent was removed under reduced pressure under anhydrous and oxygen-free conditions to obtain the white solid as the target product p-2SiOROLi1.

[0064] The preparation method of p-2SiOROLi1 single-ion solid electrolyte is as follows:

[0065] Approximately 50 mg of p-2SiOROLi1 polymer was spread evenly on an aluminum foil, and the surface was covered with another aluminum foil. The aluminum foil was then placed flat between two heated aluminum blocks. While applying pressure, the two heated aluminum blocks were heated to 100°C and maintained for 10 minutes to obtain a p-2SiOROLi1 solid electrolyte film.

[0066] Example 3: Synthesis of a three-dimensional cross-linked single-ion conductive polymer (p-1SiOROLi1)

[0067] When using polyethylene glycol (PEG150) with a molecular weight of 150, the degree of polymerization of polyethylene glycol is 3. The specific synthesis method is as follows:

[0068] 0.9 g (6 mmol) of PEG150 was added to a two-necked round-bottom flask under an argon atmosphere, followed by 20 mL of dimethyl ethylene glycol (DME) solvent. After elution with nitrogen three times, SiCl4 (0.35 mL, 3 mmol) was slowly added dropwise while stirring at 0 °C. After reacting for 4 hours, the flask was exposed to air for 1 hour (Si-Cl bonds can be hydrolyzed in trace amounts of water). After complete hydrolysis, the mixture was filtered to obtain 0.5 g of white solid as the hydrolysis product p-3SiOROH1. The hydrolysis product was transferred to a two-necked flask and dried under vacuum at 60 °C for 12 hours. 20 mL of anhydrous dichloromethane (DCM) was added, and after elution with nitrogen three times, 0.9 mL of n-butyllithium (2.5 mol / L n-hexane solution) was slowly added dropwise while stirring at 0 °C. After reacting for 12 hours, the solvent was removed under reduced pressure under anhydrous and oxygen-free conditions to obtain the white solid as the target product p-3SiOROLi1.

[0069] The specific method for preparing p-3SiOROLi1 single-ion solid electrolyte is as follows:

[0070] Approximately 50 mg of p-3SiOROLi1 polymer was spread evenly on an aluminum foil, and the surface was covered with another aluminum foil. The aluminum foil was then placed flat between two heated aluminum blocks. While applying pressure, the two heated aluminum blocks were heated to 100°C and maintained for 10 minutes to obtain a p-3SiOROLi1 solid electrolyte film.

[0071] Example 4: Synthesis of a three-dimensional cross-linked single-ion conductive polymer (p-3SiOROLi2)

[0072] When using polyethylene glycol (PEG400) with a molecular weight of 400, the degree of polymerization of polyethylene glycol is approximately 8. The specific synthesis method is as follows:

[0073] Under a nitrogen atmosphere, 2.4 g (6 mmol) of PEG400 was added to a two-necked round-bottom flask and heated to melt. Then, 20 mL of dimethyl ethylene glycol ether (DME) was added to the flask. After eluting with nitrogen three times, SiCl4 (0.35 mL, 3 mmol) was slowly added dropwise while stirring at 0 °C. After reacting for 4 hours, the flask was exposed to air for 1 hour (Si-Cl bonds can be hydrolyzed in trace amounts of water). After complete hydrolysis, the mixture was filtered to obtain 1.8 g of a white solid as the hydrolysis product p-3SiOROH2. The hydrolysis product was transferred to a two-necked flask and dried under vacuum at 60 °C for 12 hours. 20 mL of anhydrous dichloromethane (DCM) was added, and after eluting with nitrogen three times, 1.1 mL of n-butyllithium (2.5 mol / L n-hexane solution) was slowly added dropwise while stirring at 0 °C. After reacting for 12 hours, the solvent was removed under reduced pressure under anhydrous and oxygen-free conditions to obtain the white solid as the target product p-3SiOROLi2. XPS analysis of the ashed samples confirmed that the p-3SiOROH2 polymer was successfully lithiated.

[0074] The specific method for preparing p-3SiOROLi2 single-ion solid electrolyte is as follows:

[0075] Approximately 50 mg of p-3SiOROLi2 polymer was spread evenly on an aluminum foil, and the surface was covered with another aluminum foil. The aluminum foil was then placed flat between two heated aluminum blocks. While applying pressure, the two heated aluminum blocks were heated to 100°C and maintained for 10 minutes to obtain a p-3SiOROLi2 solid electrolyte film.

[0076] Example 5: Synthesis of a three-dimensional cross-linked single-ion conductive polymer (p-3SiOROLi3)

[0077] When using polyethylene glycol (PEG1000) with a molecular weight of 1000, the degree of polymerization of polyethylene glycol is approximately 20. The specific synthesis method is as follows:

[0078] 3 g (3 mmol) of PEG1000 was added to a two-necked round-bottom flask under an argon atmosphere and heated to melt. Then, 20 mL of dimethyl ethylene glycol (DME) solvent was added to the flask. After eluting with nitrogen three times, SiCl4 (0.18 mL, 1.5 mmol) was slowly added dropwise while stirring at 0 °C. After reacting for 4 hours, the flask was exposed to air for 1 hour (Si-Cl bonds can be hydrolyzed in trace amounts of water). After complete hydrolysis, the mixture was filtered to obtain 2.2 g of a white solid, which was the hydrolysis product p-3SiOROH3. The hydrolysis product was transferred to a two-necked flask and dried under vacuum at 60°C for 12 hours. 20 mL of anhydrous dichloromethane (DCM) was added, and the mixture was eluted three times with nitrogen. Then, 1.5 mL of n-butyllithium (2.5 mol / L n-hexane solution) was slowly added dropwise while stirring at 0°C. After reacting for 12 hours, the solvent was removed under reduced pressure under anhydrous and oxygen-free conditions to obtain a white solid, which was the target product p-3SiOROLi3.

[0079] Figure 5 The image shows a differential scanning calorimetry (DSC) curve of p-3SiOROH3. The curve reveals that the material has a low glass transition temperature (Tg), which confirms that the material theoretically possesses good mechanical properties and low-temperature ion conductivity.

[0080] The specific method for preparing p-3SiOROLi3 single-ion solid electrolyte is as follows:

[0081] Approximately 50 mg of p-3SiOROLi3 polymer was spread evenly on an aluminum foil, and the surface was covered with another aluminum foil. The aluminum foil was then placed flat between two heated aluminum blocks. While applying pressure, the two heated aluminum blocks were heated to 100°C and maintained for 10 minutes to obtain a p-3SiOROLi3 solid electrolyte film.

[0082] Application Example 1

[0083] Application method of single-ion polymer solid electrolyte film based on three-dimensional cross-linked single-ion conductor p-3SiOROLi1 in Example 3:

[0084] 1) Electrolytic impedance spectroscopy was used to measure the ionic conductivity (σ) of p-3SiOROLi1 electrolyte at different temperatures.

[0085] Inside a glove box (high-purity Ar atmosphere, H2O and O2 both less than 1 ppm), the prepared p-3SiOROLi3 thin film was placed between two stainless steel sheets (SS), and an SS|polymer electrolyte|SS coin cell was assembled. AC impedance testing was performed at 60℃ and 80℃ (e.g., Figure 7 According to the formula (In the formula, L is the sample thickness (cm), R is the sample impedance (Ω), and S is the sample area (cm²). 2 The ionic conductivity of the electrolyte was calculated. The ionic conductivity of the p-3SiOROLi1 thin film prepared in Example 3 was 5.87 × 10⁻⁶. -7 S·cm -1 and 2.05×10 -4 S·cm -1 .

[0086] 2) Application of p-3SiOROLi1 single-ion polymer solid electrolyte film in lithium solid-state batteries

[0087] First, the positive electrode active material (LiFePO4), conductive carbon (Super P), and binder (PVDF in NMP) were weighed according to a certain mass ratio (6-9:0.5-3:0.5-1), and an appropriate amount of NMP was added. The mixture was thoroughly mixed using a homogenizer and then transferred to aluminum foil. A coater was used to ensure uniform thickness spreading. The foil was then transferred to a vacuum drying oven and dried at 65°C for 12 hours. Finally, the dried electrode was cut into circular electrodes with a diameter of 10 mm, which became the LiFePO4 positive electrode. Next, in a glove box, using LiFePO4 as the positive electrode, Li as the negative electrode, and the prepared p-3SiOROLi1 polymer membrane as the separator and electrolyte, a CR2032 standard coin cell was assembled. This battery is an all-solid-state battery without the addition of any liquid organic solvents.

[0088] The above description is merely a preferred embodiment of the present invention and is not intended to limit the present invention. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the protection scope of the present invention.

Claims

1. A single-ion-conducting polymer based on an organosilicate salt, characterized in that, The structural formula is shown in the following formula: Formula (1) is a one-dimensional chain-like single-ion conducting polymer; formula (2) is a two-dimensional network-like single-ion conducting polymer; formula (3) is a three-dimensional cross-linked single-ion conducting polymer; In the above formula, x=3, 4…; n=2, 3, 4…; and m=2, 3, 4… 2. A method for preparing the one-dimensional chain-like single-ion-conducting polymer as claimed in claim 1, characterized by, Comprising the following steps: S1: 1:1 equivalent of SiCl4 and fixed molecular weight polyethylene glycol in an organic solvent and under a gas atmosphere, polymerization reaction to obtain a polymer; S2: The polymer obtained in S1 is exposed to air for 1 hour, and after complete hydrolysis, the hydrolysis product is obtained by suction filtration; S3: Using lithiation reagent in organic solvent and under gas atmosphere, the hydrolysis product obtained in S2 is lithiated to obtain a one-dimensional chain-like single-ion conducting polymer; The organic solvent in step S1 includes ethylene glycol dimethyl ether, diethylene glycol dimethyl ether, tetrahydrofuran, 1,3-oxolane; the gas atmosphere is inert gas; The organic solvent in step S3 includes dichloromethane, tetrahydrofuran, ethylene glycol dimethyl ether; the gas atmosphere is inert gas; the lithiation reagent includes n-butyllithium, tert-butyllithium, lithium tert-butoxide, phenyllithium, lithium hydroxide.

3. A method of preparing a two-dimensional network of single-ion conducting polymer as claimed in claim 1, characterized in that, Comprising the following steps: S1: 1:1.5 equivalent of SiCl4 and fixed molecular weight polyethylene glycol in an organic solvent and under a gas atmosphere, polymerization reaction to obtain a polymer; S2: The polymer obtained in S1 is exposed to air for 1 hour, and after complete hydrolysis, the hydrolysis product is obtained by suction filtration; S3: Using lithiation reagent in organic solvent and under gas atmosphere, the hydrolysis product obtained in S2 is lithiated to obtain a two-dimensional network-like single-ion conducting polymer; The organic solvent in step S1 includes ethylene glycol dimethyl ether, diethylene glycol dimethyl ether, tetrahydrofuran, 1,3-oxolane; the gas atmosphere is inert gas; The organic solvent in step S3 includes dichloromethane, tetrahydrofuran, ethylene glycol dimethyl ether; the gas atmosphere is inert gas; the lithiation reagent includes n-butyllithium, tert-butyllithium, lithium tert-butoxide, phenyllithium, lithium hydroxide.

4. A process for the preparation of the three-dimensional crosslinked single-ion conducting polymer as claimed in claim 1, characterized in that, Comprising the following steps: S1: 1:2 equivalent of SiCl4 and fixed molecular weight polyethylene glycol in an organic solvent and under a gas atmosphere, polymerization reaction to obtain a polymer; S2: The polymer obtained in S1 is exposed to air for 1 hour, and after complete hydrolysis, the hydrolysis product is obtained by suction filtration; S3: Using lithiation reagent in organic solvent and under gas atmosphere, the hydrolysis product obtained in S2 is lithiated to obtain a three-dimensional cross-linked single-ion conducting polymer; The organic solvent in step S1 includes ethylene glycol dimethyl ether, diethylene glycol dimethyl ether, tetrahydrofuran, 1,3-oxolane; the gas atmosphere is inert gas; The organic solvent in step S3 includes dichloromethane, tetrahydrofuran, ethylene glycol dimethyl ether; the gas atmosphere is inert gas; the lithiation reagent includes n-butyllithium, tert-butyllithium, lithium tert-butoxide, phenyllithium, lithium hydroxide.

5. A solid-state electrolyte film, characterized by: Comprising two layers of aluminum foil paper, and the two layers of aluminum foil paper are sandwiched with the single-ion conducting polymer based on organosilicate salt as claimed in claim 1.

6. A method of preparing the solid-state electrolyte film according to claim 5, characterized by, Comprising the following steps: S1: The single-ion conducting polymer is laid flat on the aluminum foil paper, and the surface is covered with another aluminum foil paper; S2: the material obtained in S1 is placed between two heated aluminum blocks; S3: the material obtained in S1 is heated to 100 DEG C while being pressed by the two heated aluminum blocks for 10 min, to obtain a single-ion conducting polymer solid-state electrolyte film.

7. Use of a solid-state electrolyte film according to claim 5, characterized in that: The solid-state electrolyte film is applied to a lithium solid-state battery.

8. A lithium solid state battery, characterized by: The lithium solid-state battery comprises a positive electrode sheet, a negative electrode sheet, and the solid-state electrolyte film of claim 5, wherein the solid-state electrolyte film is located between the positive electrode sheet and the negative electrode sheet; and the positive electrode sheet, the solid-state electrolyte film, and the negative electrode sheet are encapsulated in a battery shell composed of a positive shell and a negative shell. The positive electrode sheet material comprises lithium iron phosphate, lithium cobaltate, lithium nickelate, lithium manganate, a ternary material, a lithium-rich material, an oxide material, a sulfur positive electrode, and an air positive electrode; and the negative electrode sheet is metallic lithium.

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