Semi-solid gel electrolyte for fast-charging lithium battery and preparation method thereof

Abstract

The application discloses a kind of semi-solid gel electrolyte applied to fast charging lithium battery and preparation method thereof.The gel state covalent organic framework material PEG-TG is prepared by solvent thermal reaction with triamino guanidine hydrochloride and PEG2-CHO as raw material, water / 1,4-dioxane as solvent, acetic acid as catalyst Cl After liquid electrolyte is replaced into gel state COF, gel electrolyte PEG-TG Cl CGE is formed.The gel electrolyte PEG-TG Cl CGE of the application has excellent ionic conductivity, lithium ion transference number and wide electrochemical window, while having relatively good safety performance of semi-solid gel electrolyte, it shows excellent fast charging performance, and is suitable for lithium battery field.

Description

TECHNICAL FIELD

[0001] The application belongs to the field of lithium battery semi-solid gel electrolyte, and relates to a semi-solid gel electrolyte applied to fast-charging lithium batteries and a preparation method thereof. BACKGROUND

[0002] The liquid electrolyte used in traditional lithium batteries has defects such as flammability, strong corrosion and poor stability, and the emerging solid-state electrolyte has unsatisfactory electrochemical performance due to its poor interface contact and internal poor ion path. The gel electrolyte is a uniform system formed by a polymer network, a liquid plasticizer and a lithium salt, which provides a compromise solution to combine the high ion conductivity of the liquid electrolyte and the safety of the solid electrolyte, and is likely to become the next generation of high-performance safe electrolyte material. However, the structure of the traditional gel electrolyte is random and disordered, and it is difficult to form an internal smooth and stable ion transmission path, which limits its efficiency in high-rate charging and discharging. For example, a recently reported biomimetic gel battery has a working rate of 0.5C, and the experimental cycle number is within 300 cycles (Li H, Jing L, Wen G, et al. A Skin-Mimicked Polymer Gel Electrolyte for Stabilizing Lithium Metal Batteries [J]. Advanced Energy Materials, 2025.).

[0003] Covalent organic frameworks (COFs) are a class of crystalline materials with periodic structures, which are formed by the stacking of two-dimensional sheets in a microcosmic level, thus forming natural one-dimensional channels in the direction perpendicular to the sheets. Researchers have been trying to use these channels as transport pathways for small molecules, ions, and other substances. However, in the field of electrolyte materials, the difficulty in processing of covalent organic framework materials, which are usually insoluble crystalline powders, greatly limits their practical application. Using covalent organic framework materials as the polymer network of gel electrolyte not only avoids the problem of difficult processing, but also provides a clear structure and clear ion conduction path for the gel (Liu Z, Zhang K, Huang G, et al. Highly processable covalent organic framework gel electrolyte enabled by side-chain engineering for lithium-ion batteries [J]. Angewandte Chemie International Edition, 2022.). However, since this type of work does not design a covalent organic framework with a clear function of regulating ion conduction as a gel polymer network, but only provides a clear structure for the gel by relying on the regular channel characteristics of covalent organic frameworks, its rate performance is still not ideal. SUMMARY

[0004] One of the purposes of the present application is to provide a covalent organic framework material PEG-TG Cl -COF with the function of regulating anion and cation conduction.

[0005] The covalent organic framework material PEG-TG Cl -COF with the function of regulating anion and cation conduction according to the present application is a two-dimensional framework structure material formed by Schiff base condensation reaction of triaminoguanidine hydrochloride and PEG-linked aldehyde compound (PEG2-CHO), and its structural formula is as follows:

[0006]

[0007] The structural formula of triaminoguanidine hydrochloride according to the present application is as follows:

[0008]

[0009] The structural formula of PEG2-CHO according to the present application is as follows:

[0010]

[0011] The second purpose of the present application is to provide the covalent organic framework material PEG-TG ClThe preparation method of COF comprises the following steps:

[0012] The triaminoguanidine hydrochloride and PEG2-CHO are mixed in a molar ratio of 2:3, then a water / 1,4-dioxane mixed solution is added, and the mixture is dissolved by ultrasonic treatment, then an acetic acid solution is added, and then the mixture is treated by ultrasonic treatment until it is gelled, and then the mixture is rapidly frozen by liquid nitrogen and vacuumized, and the tube is sealed by a flame spray gun, and the reaction is heated at 120±10 DEG C until the gel-like COF material PEG-TG is obtained Cl The water / 1,4-dioxane mixed solution is prepared by mixing water and 1,4-dioxane in a volume ratio of 0.3:1, and the volume of the acetic acid solution is 1 / 20-1 / 5 of the volume of the water / 1,4-dioxane mixed solution, and the concentration of the acetic acid is 3-12 mol / L.

[0013] Further, in the mixture, the concentration of the triaminoguanidine hydrochloride is 0.03-0.1 mol / L, and preferably 0.035 mol / L; and the concentration of the PEG2-CHO is 0.03-0.1 mol / L, and preferably 0.052 mol / L.

[0014] Further, the volume of the acetic acid solution is 1 / 10 of the volume of the water / 1,4-dioxane mixed solution, and the concentration of the acetic acid is 6 mol / L.

[0015] Further, the reaction time is 48-96 h, and preferably 72 h.

[0016] Further, the gel-like COF material PEG-TG is rapidly frozen by liquid nitrogen and vacuumized, and the tube is sealed by a flame spray gun, and the reaction is heated at 120±10 DEG C until the gel-like COF material PEG-TG is obtained Cl The COF is purified by Soxhlet extraction with water and tetrahydrofuran, and finally freeze-dried to obtain the COF material PEG-TG Cl The COF is a solid.

[0017] The third object of the present application is to provide a semi-solid gel electrolyte, which is the PEG-TG Cl The CGE comprises the COF material PEG-TG Cl The COF, a lithium salt and an organic solvent.

[0018] The lithium salt is a lithium salt commonly used in the field of lithium batteries, including but not limited to lithium hexafluorophosphate (LiPF6), lithium perchlorate (LiClO4) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), lithium bis(fluorosulfonyl)imide (LiFSI) and the like. In the specific embodiment of the present application, LiTFSI is taken as an example.

[0019] The organic solvent described in the present application is an organic solvent commonly used in the field of lithium batteries, preferably an organic solvent with a boiling point of ≥ 150℃, including but not limited to ethylene carbonate (EC), propylene carbonate (PC) and butylene carbonate (BC) and the like. In the specific embodiment of the present application, PC is taken as an example.

[0020] The fourth object of the present application is to provide a preparation method of the semi-solid gel electrolyte described above, comprising the following steps:

[0021] (1) Dissolve lithium salt powder in an organic solvent to prepare a lithium salt solution;

[0022] (2) Place the gel-like covalent organic framework material PEG-TG Cl -COF in the lithium salt solution, and replace it with fresh lithium salt solution at intervals, and repeat the process until the lithium salt solution completely replaces the gel-like covalent organic framework material PEG-TG Cl -COF.

[0023] (3) Place the covalent organic framework material PEG-TG Cl -COF obtained in step (2) in a lithium salt solution for high-temperature treatment, and use the boiling point difference between the low-boiling-point liquids (1,4-dioxane, water and acetic acid) remaining in the gel and the high-boiling-point organic solvent to completely remove the remaining low-boiling-point liquids, to prepare a semi-solid gel electrolyte PEG-TG Cl -CGE.

[0024] Further, in step (1), the concentration of the lithium salt solution is 1 mol / L; in step (2), the replacement frequency is more than three times; and in step (3), the high-temperature treatment temperature is 110-150℃, preferably 120℃.

[0025] The fifth object of the present application is to provide a semi-solid gel lithium battery, whose positive electrode is lithium iron phosphate (LFP), negative electrode is lithium, and electrolyte is a semi-solid gel electrolyte PEG-TG Cl -CGE.

[0026] The semi-solid gel lithium battery described in the present application can be a lithium ion battery or a lithium metal battery.

[0027] Compared with the prior art, the present application has the following advantages:

[0028] (1) The present application utilizes the high designability of covalent organic framework materials, introducing cationic skeletons and PEG side chains into the interior, and the synergistic effect of the two components enables them to be prepared in a gel state, thus overcoming the limitation of traditional covalent organic frameworks as difficult-to-process powder materials. As a result, based on the gel-like covalent organic framework material PEG-TG ClThe self-supporting semi-solid gel electrolyte prepared by COF can fully exert the regular channel characteristics of the covalent organic framework material for ion conduction.

[0029] (2) The cationic framework of the covalent organic framework material of the present application restricts the migration of lithium salt anions through Coulomb interaction. The PEG side chain provides a jumping site for lithium ions, inducing directional transport of lithium ions and uniform deposition on the electrode surface. The coordination of the two components respectively regulates the transport of anions and cations, improving the ionic conductivity of the electrolyte while maintaining a high lithium ion transference number, greatly improving the ion conduction performance of the electrolyte.

[0030] (3) The semi-solid gel electrolyte based on the covalent organic framework material of the present application has excellent high-rate cycle performance (i.e. fast charging performance) in lithium batteries, for example Li|PEG-TG Cl The CGE|LFP battery can be stably operated at 10C rate for more than 2000 cycles. This performance almost surpasses all semi-solid gel electrolytes applied to this battery system, providing a design idea for gel electrolytes targeting fast charging performance. BRIEF DESCRIPTION OF DRAWINGS

[0031] Figure 1 XRD comparison chart of materials prepared with different solvent ratios.

[0032] Figure 2 PEG-TG Cl Infrared chart of COF.

[0033] Figure 3 PEG-TG Cl Digital chart of CGE.

[0034] Figure 4 PEG-TG Cl Variable temperature electrochemical impedance spectrum of CGE.

[0035] Figure 5 Li|PEG-TG Cl Electrochemical impedance spectrum and corresponding chronoamperogram of CGE|Li battery before and after polarization.

[0036] Figure 6 Li|PEG-TG Cl Cycle performance chart of CGE|Li battery at 0.2 mA cm -2 and 25°C.

[0037] Figure 7 Li|PEG-TG Cl Cycle curve of CGE|LFP battery at 10C rate and 25°C. DETAILED DESCRIPTION

[0038] In order to make the purpose, technical scheme and advantages of the present application more clear, the present application is further described in detail below by examples, and in combination with the drawings. It should be understood that the specific examples described herein are only used to explain the present application, and are not used to limit the present application.

[0039] The triaminoguanidine hydrochloride described in the present application can be commercially purchased. PEG2-CHO can be prepared by referring to the literature (Wu M, Huang H, Xu B, et al. Poly (ethylene glycol)-functionalized 3D covalent organic frameworks as solid-state polyelectlytes [J]. Rsc Advances, 2022.) and the specific synthesis route is as follows:

[0040]

[0041] The specific steps are as follows:

[0042] (1) Synthesis of 1,4-dibromo-2,5-bis(2-(2-methoxyethoxy)ethoxy)benzene: 2,5-dibromoparadichlorobenzene (2.14 g, 8.0 mmol), K2CO3(5.52 g, 40.0 mmol) and 1-bromo-2-(2-methoxyethoxy)ethane (2.4 mL, 17.5 mmol) were added into 100 mL Schlenk flask, respectively, which was purged with argon for three times using three-way tube, and then 40 mL of super dry acetonitrile was injected using a needle tube. The reaction was stirred at 90℃ for 12 hours. After the reaction was completed, the mixture was filtered and the solution was concentrated under vacuum, and then dissolved in dichloromethane and washed with water three times, and the aqueous phase and oil phase were separated by a separatory funnel. The oil phase was dried with anhydrous Na2SO4, filtered and concentrated. Silica gel column chromatography (petroleum ether / ethyl acetate: 1 / 1) was used to obtain transparent crystals of 1,4-dibromo-2,5-bis(2-(2-methoxyethoxy)ethoxy)benzene (yield: 70%).

[0043] (2) Synthesis of PEG2-CHO: 1,4-Dibromo-2,5-bis(2-(2-methoxyethoxy)ethoxy)benzene (2.36 g, 5 mmol), p-formylphenylboronic acid (2.26 g, 15 mmol), tetrakis(triphenylphosphine)palladium (340 mg) and K2CO3(2.07 g, 15 mmol) were added into a 100 mL Schlenk tube, which was purged with argon three times using a double-tube, then deoxygenated tetrahydrofuran (100 mL) and deoxygenated water (20 mL) were injected using a needle tube. The reaction was stirred at 80 °C overnight. After the reaction, the mixture was filtered and the solution was concentrated under vacuum, then redissolved in dichloromethane and washed with water three times, the aqueous and oil phases were separated by a separatory funnel. The oil phase was dried with Na2SO4, filtered and concentrated. The crude product was purified by column chromatography (petroleum ether / ethyl acetate: 1 / 1) to obtain PEG2-CHO as a light yellow powder (yield: 74%).

[0044] Example 1

[0045] PEG-TG Cl The method for preparing PEG-TG-COF is as follows:

[0046] Trisamino guanidine hydrochloride (28 mg, 0.2 mmol) and PEG2-CHO (156.8 mg, 0.3 mmol) were mixed in a long neck Pyrex tube (tube length 18 cm, neck length about 9 cm, volume about 20 mL). A mixed solution of 1,4-dioxane (2 mL), deionized water (0.6 mL) and 6 mol / L acetic acid solution (260 μL) was added. Then the mixture was ultrasonically treated for 15 minutes until it gelled. After that, the mixture in the tube was quickly frozen with liquid nitrogen and evacuated. The neck of the tube was sealed with a flame gun. After waiting for the Pyrex tube to cool to room temperature, it was placed in an oven at 120 °C for 72 hours. The gel-like product covalent organic framework material PEG-TG-COF was obtained Cl The covalent organic framework material PEG-TG-COF was purified by Soxhlet extraction with water and tetrahydrofuran, then freeze-dried to obtain a yellow solid Cl The covalent organic framework material PEG-TG-COF was purified by Soxhlet extraction with water and tetrahydrofuran, then freeze-dried to obtain a yellow solid

[0047]

[0048] Figure 1 The XRD pattern of the material prepared in different solvent ratios was compared. The XRD image of the product prepared with a 1,4-dioxane / water volume ratio of 1 / 0.3 showed a weak characteristic peak at 3.1°, corresponding to the (100) crystal plane of the covalent organic framework. This proved the successful synthesis of the material from the crystal characteristics of the material.

[0049] Figure 2 PEG-TGCl -COF's infrared spectrum, it can be seen that there are two obvious peaks at 1094 and 2881 cm -1 , respectively, which are C-O and C-H from PEG chain; the peak at 1214 cm -1 is from C-N of backbone amino; the peak at 1615 cm -1 is from C=N. This proves the successful synthesis of the material from the molecular structure of the material.

[0050] Comparative Example 1

[0051] This comparative example is substantially the same as Example 1, except that the volume ratio of 1,4-dioxane and water is 1 / 0.1, i.e. 1,4-dioxane (2 mL) and deionized water (0.2 mL) are added, and the monomer concentration remains unchanged. The product is an orange-yellow gel, which is treated according to the steps in Example 1 and tested for XRD.

[0052] Figure 1 The XRD patterns of materials prepared at different solvent ratios, the XRD image of the product prepared at a 1,4-dioxane / water volume ratio of 1 / 0.1 does not exhibit characteristic peaks. This indicates that the product at this solvent ratio is amorphous and cannot synthesize the target covalent organic framework material.

[0053] Comparative Example 2

[0054] This comparative example is substantially the same as Example 1, except that the volume ratio of 1,4-dioxane and water is 1 / 0.5, i.e. 1,4-dioxane (2 mL) and deionized water (1 mL) are added, and the monomer concentration remains unchanged. The product is a yellow powder, which is treated according to the steps in Example 1 and tested for XRD.

[0055] Figure 1 The XRD patterns of materials prepared at different solvent ratios, the XRD image of the product prepared at a 1,4-dioxane / water volume ratio of 1 / 0.5 does not exhibit characteristic peaks. This indicates that the product at this solvent ratio is amorphous and cannot synthesize the target covalent organic framework material.

[0056] Example 2

[0057] Gel electrolyte PEG-TG Cl The preparation method of CGE is as follows:

[0058] 28.7 g of LiTFSI was weighed and dissolved in 100 mL of PC to prepare a liquid electrolyte, and the concentration of LiTFSI was 1 mol / L. The gel-like covalent organic framework material PEG-TG Cl-COF was left in the liquid electrolyte. Every 24 hours, fresh liquid electrolyte was used to replace it. This process was repeated three times, replacing most of the low boiling point liquids, including 1,4-dioxane, water, acetic acid, etc., and the residual monomers during the reaction. Finally, the gel was immersed in the liquid electrolyte and left overnight at 120°C, retaining the liquid electrolyte while completely removing the residual solvents during the synthesis process by the difference in boiling points.

[0059] Figure 3 Gel electrolyte PEG-TG Cl - Digital photo of CGE, which can be seen as a gel electrolyte PEG-TG Cl - CGE presents an orange-yellow gel.

[0060] Example 3

[0061] Gel electrolyte PEG-TG Cl - Battery assembly with CGE as electrolyte and stainless steel (Ss) as electrodes on both sides and ion conductivity test, the specific steps are as follows:

[0062] In the argon-filled glove box, the stainless steel sheet, gel electrolyte PEG-TG Cl - Ss|PEG-TG was assembled in the order of CGE, stainless steel sheet Cl - CGE|Ss battery, the battery mold was sealed by wax sealing to ensure airtightness. The ion conductivity (σ) was calculated using equation (1), where L represents the thickness of the electrolyte, S represents the effective contact area between the electrolyte and the stainless steel, and R corresponds to the bulk electrolyte resistance. The ion conductivity of n%-EBTp-M was measured using electrochemical impedance spectroscopy (EIS) at a temperature range of 25-100°C, a frequency range of 0.1 Hz to 1 MHz, and an amplitude of 10 mV.

[0063]

[0064] Figure 4 Gel electrolyte PEG-TG Cl - Temperature-dependent electrochemical impedance spectroscopy of CGE. PEG-TG Cl - The ion conductivity of CGE is as high as 17.7 mS cm -1 Such high conductivity indicates that the electrolyte can have enough lithium ions participate in the electrode reaction at high current density, thus meeting the basic requirements of fast charging technology.

[0065] Example 4

[0066] Gel electrolyte PEG-TG Cl - Lithium symmetric battery assembly with CGE as electrolyte and lithium ion transference number test, the specific steps are as follows:

[0067] In an argon-filled glovebox, Li|PEG-TG Cl -CGE, Li symmetric cells were assembled in the order of Li|PEG-TG Cl -CGE|Li cells were sealed by wax sealing to ensure the air-tightness of the cell molds. The assembled Li|Li symmetric cells were tested using chronoamperometry, in which a polarization of 10 mV (AV) was applied to the cell for 3000 s. The polarization current, including the initial value (I bp ) and the steady-state value (I ap ), was recorded. The interfacial resistance before polarization (R bp ) and after polarization (R ap ) was measured using electrochemical impedance spectroscopy at a test temperature of 60 °C. Subsequently, the transference number of Li + (t Li + ) was calculated using the Bruce-Vincent-Evans equation (2).

[0068]

[0069] Figure 5 PEG-TG Cl -CGE before and after polarization and the corresponding chronoamperometry curves. PEG-TG Cl -CGE exhibits a high t Li + , indicating that the ion conduction within the electrolyte is mainly dominated by lithium ions, and the designed cation skeleton plays a key role therein. This improves the stability of the battery during cycling.

[0070] Example 5

[0071] PEG-TG Cl -CGE was used as the electrolyte, and the lithium symmetric battery was assembled and tested for cycling, with the specific steps as follows:

[0072] The assembly method of the lithium symmetric battery was consistent with that in Example 4, and the cycling performance of the battery was tested at a current density of 0.2 mA cm -2 and 25 °C in a blue cell test system.

[0073] Figure 6 The cycling performance of the lithium symmetric battery at 0.2 mA cm -2 and 25 °C. The results show that the lithium symmetric battery can be stably operated for more than 2800 hours, and the overpotential is as low as ±54 mV. This proves that the specially designed covalent organic framework structure has a positive effect on the uniform deposition of lithium ions.

[0074] Example 6

[0075] with gel electrolyte PEG-TG Cl The assembly and testing of the semi-solid gel full battery with CGE as electrolyte are as follows:

[0076] In an argon-filled glove box, Li|PEG-TG Cl The Li|PEG-TG Cl The CGE|LFP battery was sealed by wax sealing to ensure air tightness. The charge-discharge performance of the battery was tested in a blue cell test system at a charge-discharge rate of 10C and 25°C, and the voltage range was 2.5V-4.2V.

[0077] Figure 7 The Li|PEG-TG Cl The cycle curve of the CGE|LFP battery at a rate of 10C. It can be seen that even at a rate as high as 10C, the CGE|LFP battery with PEG-TG Cl The battery with CGE as electrolyte also has high specific capacity and cycle stability, and there is no obvious decay within 2000 cycles. This performance almost surpasses all semi-solid gel batteries used in this system, proving the superiority of the design of the present application.

Claims

1. Covalent organic framework material PEG-TG with regulated anion and cation conduction function Cl -COF, characterized in that, The structural formula of the PEG2-CHO is as follows: was prepared by the following steps: Mixing trisamino guanidine hydrochloride and PEG2-CHO with a molar ratio of 2:3, then adding a water / 1,4-dioxane mixed solution, ultrasonic dissolution, adding an acetic acid solution, then ultrasonic treatment until the mixture gels, then rapid freezing with liquid nitrogen and vacuumizing, sealing the tube with a flame spray gun, heating the reaction at 120±10 ℃ until a gel-like covalent organic framework material PEG-TG is obtained Cl -COF; in the water / 1,4-dioxane mixed solution, the volume ratio of water to 1,4-dioxane is 0.3:1, the volume of the acetic acid solution is 1 / 20-1 / 5 of the volume of the water / 1,4-dioxane mixed solution, and the concentration of the acetic acid is 3-12 mol / L; The structural formula of the PEG2-CHO is as follows: 。 2. The covalent organic framework material PEG-TG according to claim 1 Cl -COF characterized by In the mixture, the concentration of the triaminoguanidine hydrochloride is 0.03-0.1 mol / L, and the concentration of the PEG2-CHO is 0.03-0.1 mol / L; the volume of the acetic acid solution is 1 / 10 of the volume of the water / 1,4-dioxane mixed solution, and the concentration of the acetic acid is 6 mol / L; and the reaction time is 48-96 h.

3. The covalent organic framework material PEG-TG according to claim 1 Cl -COF characterized by In the mixture, the concentration of the triaminoguanidine hydrochloride is 0.035 mol / L, and the concentration of the PEG2-CHO is 0.052 mol / L; and the reaction time is 72 h.

4. The covalent organic framework material PEG-TG according to claim 1 Cl -COF characterized by The gel-like covalent organic framework material PEG-TG Cl -COF was purified by Soxhlet extraction with water and tetrahydrofuran and finally freeze-dried to obtain the covalent organic framework material PEG-TG Cl -COF solid.

5. A semi-solid gel electrolyte PEG-TG Cl -CGE characterized in that, The constituent ingredients include the covalent organic framework material PEG-TG of claim 1 Cl -COF, lithium salt, and organic solvent.

6. The semi-solid gel electrolyte PEG-TG according to claim 5 Cl - CGE, characterized in that, The lithium salt is LiPF6, LiClO4, LiTFSI or LiFSI; and the organic solvent is ethylene carbonate, propylene carbonate or butylene carbonate.

7. The semi-solid gel electrolyte PEG-TG of claim 5 or 6 Cl A method for producing a CGE, characterized by, The method comprises the following steps: (1) dissolving the lithium salt powder in the organic solvent to prepare a lithium salt solution; (2) The gel-like covalent organic framework material PEG-TG Cl -COF is left to stand in the lithium salt solution and replaced with fresh lithium salt solution at intervals, and the process is repeated until the lithium salt solution completely replaces the gel-like covalent organic framework material PEG-TG Cl - most of the liquid and unreacted monomers remaining in the COF; (3) Covalent organic framework material PEG-TG obtained in step (2) is subjected to high-temperature treatment in a lithium salt solution Cl The COF gel is placed in a lithium salt solution for high-temperature treatment, and the difference between the boiling points of the low-boiling-point liquids, such as 1,4-dioxane, water, and acetic acid, and the high-boiling-point organic solvent remaining in the gel is used to completely remove the low-boiling-point liquids, to obtain a semi-solid gel electrolyte PEG-TG Cl CGE.

8. The production method according to claim 7, characterized by, In step (1), the concentration of the lithium salt solution is 1 mol / L; in step (2), the replacement is performed more than three times; and in step (3), the high-temperature treatment temperature is 110-150 DEG C.

9. The preparation method according to claim 7, characterized in that, In step (3), the high-temperature treatment temperature is 120 DEG C.

10. A semi-solid gel lithium battery, characterized by, The positive electrode is lithium iron phosphate, the negative electrode is lithium, and the electrolyte is the semi-solid gel electrolyte PEG-TG described in claim 5 or 6 Cl -CGE.

11. The semi-solid gel lithium battery of claim 10, wherein, The lithium battery is a lithium ion battery or a lithium metal battery.

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