A single-walled carbon nanotube aqueous lithium-ion conductive paste and its preparation method

Abstract

This invention relates to the field of carbon nanotube technology, specifically disclosing a single-walled carbon nanotube aqueous lithium-ionized conductive slurry and its preparation method. The raw materials for this single-walled carbon nanotube aqueous lithium-ionized conductive slurry include single-walled carbon nanotubes, lithium hydroxide aqueous solution, hydrogen peroxide aqueous solution, 3,4-ethylenedioxythiophene, lithium bis(trifluoromethanesulfonylimide), ammonium persulfate, organic lithium salts, dispersant, and deionized water. This invention, through a multi-level structural innovation of "covalent grafting-core-shell coating-dual lithium source synergy," simultaneously solves problems such as the instability of high-capacity inorganic lithium supplementers in aqueous systems, high interfacial impedance between the conductive network and the lithium supplementation material, and the inability of a single lithium source to meet the needs of the entire battery lifecycle. The resulting slurry exhibits stable storage, excellent processability, and can significantly improve the initial coulombic efficiency and cycle life of batteries, making it easy to scale up industrially.

Description

Technical Field

[0001] This invention relates to the field of conductive agent technology, and more specifically, to a single-walled carbon nanotube aqueous lithium-ionized conductive slurry and its preparation method. Background Technology

[0002] Lithium-ion batteries, due to their high energy density and long cycle life, have been widely used in consumer electronics, electric vehicles, and large-scale energy storage. However, during the first charge of a lithium-ion battery, a solid electrolyte interface film forms on the surface of the negative electrode. This process irreversibly consumes active lithium from the positive electrode, leading to a decrease in initial coulombic efficiency and reversible capacity loss. To compensate for this loss of active lithium and improve the overall battery performance, pre-lithiation technology has become a research hotspot.

[0003] In the field of conductive agents, single-walled carbon nanotubes are considered ideal materials for constructing efficient conductive networks and reducing electrode internal resistance due to their excellent electronic conductivity, high aspect ratio, and low percolation threshold. Currently, "lithiated conductive pastes" that integrate lithium replenishment and conductivity, especially water-based environmentally friendly pastes, have become a leading direction in the industry. However, high-capacity inorganic lithium replenishers are sensitive to water and are prone to hydrolysis or decomposition reactions, rendering them ineffective and unsuitable for direct use in water-based pastes. Existing technologies typically employ expensive anhydrous organic solvent systems or can only use organic lithium salts with lower lithium replenishment capacity but relatively stable water properties, making it impossible to simultaneously achieve high lithium replenishment capacity and water-based environmentally friendly processing. Summary of the Invention

[0004] To address the shortcomings of existing technologies, the present invention aims to provide a single-walled carbon nanotube aqueous lithium-ionized conductive slurry and its preparation method.

[0005] To achieve the above objectives, the present invention provides the following technical solution: A single-walled carbon nanotube aqueous lithium-ion conductive paste, comprising the following raw materials by weight: 3-5 parts single-walled carbon nanotubes, 20-40 parts lithium hydroxide aqueous solution, 30-80 parts hydrogen peroxide aqueous solution, 1.5-2.5 parts 3,4-ethylenedioxythiophene, 1-2 parts lithium bis(trifluoromethanesulfonylimide), 1.5-2.5 parts ammonium persulfate, 0.5-1.5 parts organolithium salt, 0.3-0.5 parts dispersant, and 60-90 parts deionized water.

[0006] Furthermore, the single-walled carbon nanotubes have a diameter of 1~3 nm and a length of 10~30 μm.

[0007] Furthermore, the concentration of the lithium hydroxide aqueous solution is 15~30wt%.

[0008] Furthermore, the concentration of the hydrogen peroxide aqueous solution is 5-15 wt%.

[0009] Furthermore, the organic lithium salt includes at least one of lithium citrate, lithium polyacrylate, and lithium tartrate.

[0010] Furthermore, the dispersant includes at least one of polyvinylpyrrolidone, polyvinyl alcohol, and polyethylene glycol p-isooctylphenyl ether.

[0011] Furthermore, the preparation method of the single-walled carbon nanotube aqueous lithium-ion conductive paste includes the following steps: (1) Weigh each raw material component according to its weight percentage; (2) Add single-walled carbon nanotubes and dispersant to 2 / 3 of deionized water and sonicate at 20~30℃ for 20~60 min to obtain a single-walled carbon nanotube aqueous dispersion.

[0012] (3) Cool the single-walled carbon nanotube aqueous dispersion to 0~10℃, stir at 100~400rpm and simultaneously add lithium hydroxide aqueous solution and hydrogen peroxide aqueous solution, the addition time is 30~90min, then add 3,4-ethylenedioxythiophene and lithium bis(trifluoromethanesulfonylimide), maintain the temperature at 0~10℃, continue stirring for 15~30min to obtain the reaction system; (4) Dissolve ammonium persulfate in the remaining 1 / 3 of the water and slowly add it dropwise into the reaction system over 45 to 120 minutes. After the addition is complete, raise the temperature to 15°C to 30°C, add the organic lithium salt, and continue stirring the reaction at 100 to 400 rpm for 4 to 8 hours to obtain the composite dispersion. (5) The composite dispersion is homogenized in a high-pressure micro-jet homogenizer 1 to 5 times to obtain a single-walled carbon nanotube aqueous lithium conductive slurry.

[0013] Furthermore, the conditions for ultrasonic treatment in step (2) are power 200~600W and frequency 20~40kHz.

[0014] Furthermore, the pressure of the homogenization process in step (5) is 500~2000 bar.

[0015] In summary, this application includes at least the following beneficial effects: (1) This invention utilizes a "one-pot aqueous phase method" to form a dense conductive polymer shell on the surface of lithium peroxide nanoparticles at the instant they are generated. This shell has excellent water-repellent and lithium-ion-conducting properties, completely isolating the highly active, high-capacity lithium peroxide core from water, fundamentally solving the problem that high-capacity inorganic lithium replenishing agents cannot exist stably in aqueous slurries. Compared to traditional lithium replenishing slurries that require expensive and toxic organic solvents, the slurry of this invention uses deionized water as the dispersion medium, which is not only green and environmentally friendly and inherently safe, but also seamlessly integrated into existing aqueous electrode coating production lines for lithium-ion batteries, significantly reducing production costs and environmental risks.

[0016] (2) In this invention, lithium peroxide is generated in situ by covalently grafting CO-Li chemical bonds onto oxygen-containing functional groups on the surface of single-walled carbon nanotubes. The contact between the single-walled carbon nanotubes and the lithium replenishment material is no longer physical, but rather a chemical bond at the atomic scale. This not only eliminates the electron transport barrier between the two, but also ensures that the composite structure remains stable under volume changes during slurry stirring, coating, and long-term battery cycling, avoiding particle agglomeration and desorption. At the same time, the single-walled carbon nanotubes themselves are excellent electronic conductors, while the covalently grafted lithium salt-doped conductive polymer shell is a good lithium-ion conductor. This unique core-shell grafting structure constructs a three-dimensional dual-continuous conductive network in situ inside the electrode. Electrons and lithium ions can reach the surface of the active material simultaneously through dedicated channels with the shortest path and minimum impedance, significantly improving the rate performance of the electrode and the utilization rate of the active material.

[0017] (3) This invention introduces a dual lithium source synergistic design of "main lithium source - auxiliary lithium source" to achieve precise compensation for the consumption of active lithium at different stages of the battery. When a solid electrolyte interface film is formed during the first charge, the organic lithium salt can quickly release lithium ions to accurately compensate for the first irreversible capacity loss and improve the battery's first coulombic efficiency; the covalently grafted core-shell lithium peroxide serves as a high-capacity main lithium source, and in subsequent cycles, as the battery's small side reactions gradually decompose, it continuously and stably replenishes active lithium, effectively delaying the battery capacity drop and extending the battery's cycle life. This sequential relay lithium replenishment strategy of "first-efficiency compensation" and "long-term slow release" realizes intelligent management of active lithium throughout the battery's entire life cycle. Detailed Implementation

[0018] It should be noted that, where there is no conflict, the embodiments and features described in this application can be combined with each other. The present invention will now be described in detail with reference to the embodiments.

[0019] It should be noted that, unless otherwise specified, all technical and scientific terms used in this application have the same meaning as commonly understood by one of ordinary skill in the art to which this application pertains.

[0020] This invention provides a method for preparing a single-walled carbon nanotube aqueous lithium-ion conductive paste, comprising the following steps: (1) Weigh out the following by weight: 3-5 parts of single-walled carbon nanotubes with a diameter of 1-3 nm and a length of 10-30 μm, 20-40 parts of lithium hydroxide aqueous solution with a concentration of 15-30 wt%, 30-80 parts of hydrogen peroxide aqueous solution with a concentration of 5-15 wt%, 1.5-2.5 parts of 3,4-ethylenedioxythiophene, 1-2 parts of lithium bis(trifluoromethanesulfonylimide), 1.5-2.5 parts of ammonium persulfate, 0.5-1.5 parts of organolithium salt, 0.3-0.5 parts of dispersant, and 60-90 parts of deionized water; (2) Add single-walled carbon nanotubes and dispersant to 2 / 3 of deionized water, and sonicate at 20-30℃ for 20-60 minutes under the conditions of power 200-600W and frequency 20-40kHz to obtain a single-walled carbon nanotube aqueous dispersion. (3) Cool the single-walled carbon nanotube aqueous dispersion to 0~10℃, stir at 100~400rpm and simultaneously add lithium hydroxide aqueous solution and hydrogen peroxide aqueous solution, the addition time is 30~90min, then add 3,4-ethylenedioxythiophene and lithium bis(trifluoromethanesulfonylimide), maintain the temperature at 0~10℃, continue stirring for 15~30min to obtain the reaction system; (4) Dissolve ammonium persulfate in the remaining 1 / 3 of the water and slowly add it dropwise into the reaction system over 45 to 120 minutes. After the addition is complete, raise the temperature to 15°C to 30°C, add the organic lithium salt, and continue stirring the reaction at 100 to 400 rpm for 4 to 8 hours to obtain the composite dispersion. (5) Place the composite dispersion in a high-pressure micro-jet homogenizer and homogenize it 1 to 5 times under a pressure of 500 to 2000 bar to obtain a single-walled carbon nanotube aqueous lithium conductive slurry.

[0021] The organic lithium salt includes at least one of lithium citrate, lithium polyacrylate, and lithium tartrate; the dispersant includes at least one of polyvinylpyrrolidone, polyvinyl alcohol, and polyethylene glycol p-isooctylphenyl ether.

[0022] The technical solutions provided by the present invention will be described in detail below with reference to the embodiments, but they should not be construed as limiting the scope of protection of the present invention.

[0023] Example 1 The preparation method of the single-walled carbon nanotube aqueous lithium-ion conductive paste in this embodiment includes the following steps: (1) Weigh out the following by weight: 3 parts of single-walled carbon nanotubes with a diameter of 1 nm and a length of 10 μm, 20 parts of lithium hydroxide aqueous solution with a concentration of 15 wt%, 30 parts of hydrogen peroxide aqueous solution with a concentration of 5 wt%, 1.5 parts of 3,4-ethylenedioxythiophene, 1 part of lithium bis(trifluoromethanesulfonylimide), 1.5 parts of ammonium persulfate, 0.5 parts of lithium citrate, 0.3 parts of polyvinylpyrrolidone, and 60 parts of deionized water. (2) Add single-walled carbon nanotubes and polyvinylpyrrolidone to 2 / 3 of deionized water, and sonicate at 20°C for 20 min under the conditions of 200W power and 20kHz frequency to obtain a single-walled carbon nanotube aqueous dispersion. (3) Cool the single-walled carbon nanotube aqueous dispersion to 0°C, stir at 100 rpm and simultaneously add lithium hydroxide aqueous solution and hydrogen peroxide aqueous solution for 30 min, then add 3,4-ethylenedioxythiophene and lithium bis(trifluoromethanesulfonylimide), maintain the temperature at 0°C and continue stirring for 15 min to obtain the reaction system. (4) Dissolve ammonium persulfate in the remaining 1 / 3 of the water and slowly add it dropwise into the reaction system over 45 min. After the addition is complete, raise the temperature to 15°C, add lithium citrate, and continue stirring at 100 rpm for 4 h to obtain a composite dispersion. (5) The composite dispersion was placed in a high-pressure micro-jet homogenizer and homogenized once at a pressure of 500 bar to obtain a single-walled carbon nanotube aqueous lithium conductive slurry.

[0024] Example 2 The preparation method of the single-walled carbon nanotube aqueous lithium-ion conductive paste in this embodiment includes the following steps: (1) Weigh out the following by weight: 4 parts of single-walled carbon nanotubes with a diameter of 2 nm and a length of 20 μm, 30 parts of lithium hydroxide aqueous solution with a concentration of 20 wt%, 55 parts of hydrogen peroxide aqueous solution with a concentration of 10 wt%, 2 parts of 3,4-ethylenedioxythiophene, 1.5 parts of lithium bis(trifluoromethanesulfonylimide), 2 parts of ammonium persulfate, 1 part of lithium polyacrylate, 0.4 parts of polyvinyl alcohol, and 75 parts of deionized water. (2) Add single-walled carbon nanotubes and polyvinyl alcohol to 2 / 3 of deionized water, and sonicate at 25°C for 40 min under the conditions of power 400W and frequency 30kHz to obtain a single-walled carbon nanotube aqueous dispersion. (3) Cool the single-walled carbon nanotube aqueous dispersion to 5°C, stir at 250 rpm and simultaneously add lithium hydroxide aqueous solution and hydrogen peroxide aqueous solution for 60 min, then add 3,4-ethylenedioxythiophene and lithium bis(trifluoromethanesulfonylimide), maintain the temperature at 5°C and continue stirring for 20 min to obtain the reaction system. (4) Dissolve ammonium persulfate in the remaining 1 / 3 of the water and slowly add it dropwise into the reaction system over 80 min. After the addition is complete, raise the temperature to 20°C, add lithium polyacrylate, and continue stirring at 250 rpm for 6 h to obtain a composite dispersion. (5) The composite dispersion was placed in a high-pressure micro-jet homogenizer and homogenized three times under a pressure of 1200 bar to obtain a single-walled carbon nanotube aqueous lithium conductive slurry.

[0025] Example 3 The preparation method of the single-walled carbon nanotube aqueous lithium-ion conductive paste in this embodiment includes the following steps: (1) Weigh out the following by weight: 5 parts of single-walled carbon nanotubes with a diameter of 3 nm and a length of 30 μm, 40 parts of lithium hydroxide aqueous solution with a concentration of 30 wt%, 80 parts of hydrogen peroxide aqueous solution with a concentration of 15 wt%, 2.5 parts of 3,4-ethylenedioxythiophene, 2 parts of lithium bis(trifluoromethanesulfonylimide), 2.5 parts of ammonium persulfate, 1.5 parts of lithium tartrate, 0.5 parts of polyethylene glycol p-isooctylphenyl ether, and 90 parts of deionized water. (2) Add single-walled carbon nanotubes and polyethylene glycol p-isooctylphenyl ether to 2 / 3 of deionized water, and sonicate at 30°C for 60 min under the conditions of 600W power and 40kHz frequency to obtain a single-walled carbon nanotube aqueous dispersion. (3) Cool the single-walled carbon nanotube aqueous dispersion to 10°C, stir at 400 rpm and simultaneously add lithium hydroxide aqueous solution and hydrogen peroxide aqueous solution for 90 min, then add 3,4-ethylenedioxythiophene and lithium bis(trifluoromethanesulfonylimide), maintain the temperature at 10°C and continue stirring for 30 min to obtain the reaction system. (4) Dissolve ammonium persulfate in the remaining 1 / 3 of the water and slowly add it dropwise into the reaction system over 120 min. After the addition is complete, raise the temperature to 30°C, add lithium tartrate, and continue stirring at 400 rpm for 8 h to obtain a composite dispersion. (5) The composite dispersion was placed in a high-pressure micro-jet homogenizer and homogenized 5 times under a pressure of 2000 bar to obtain a single-walled carbon nanotube aqueous lithium conductive slurry.

[0026] Comparative Example 1 The preparation method of this comparative example involves ball milling and mixing lithium peroxide powder, single-walled carbon nanotubes, and polyvinylpyrrolidone in water to prepare a conductive paste.

[0027] Comparative Example 2 The preparation method of this comparative example is roughly the same as that of Example 1, but the single-walled carbon nanotubes were not subjected to ultrasonic dispersion pretreatment, but were directly mixed with lithium hydroxide aqueous solution and hydrogen peroxide aqueous solution.

[0028] Comparative Example 3 The preparation method of this comparative example is roughly the same as that of Example 1, but no organic lithium salt is added to the formulation.

[0029] Experimental Example Slurry stability: The slurry samples prepared in Examples 1-3 and Comparative Examples 1-3 were left to stand at 25°C for 48 hours. The presence of stratification and sedimentation was observed and recorded to evaluate their storage stability.

[0030] Electrode resistivity: The resistivity of the electrode coating was measured by coating the slurry samples prepared in Examples 1-3 and Comparative Examples 1-3 onto an insulating substrate film and then drying them.

[0031] First coulombic efficiency: The slurry samples prepared in Examples 1-3 and Comparative Examples 1-3 were compounded with positive electrode active materials to prepare electrode sheets. After assembling half cells, they were discharged at a constant current of 0.1C to the cutoff voltage, and the ratio of the first discharge capacity to the charging capacity was calculated.

[0032] Capacity retention rate after 200 cycles: The slurry samples prepared in Examples 1-3 and Comparative Examples 1-3 were compounded with positive electrode active materials to prepare electrode sheets, and full cells were assembled. The cells were cycled 200 times at a 1C / 1C charge / discharge rate. The percentage of the discharge capacity of the 200th cycle divided by the discharge capacity of the 2nd cycle was used as the capacity retention rate.

[0033] 5C rate discharge capacity ratio: The slurry samples prepared in Examples 1-3 and Comparative Examples 1-3 were compounded with positive electrode active materials to prepare electrodes, and full cells were assembled. After being fully charged at 0.2C, the cells were discharged to the cutoff voltage at 0.2C and 5C, respectively. The 5C discharge capacity was divided by the 0.2C discharge capacity to characterize the effect of the slurry on the rate performance of the electrodes. The specific results are shown in Table 1.

[0034] Table 1. Performance test results of the examples and comparative examples

[0035] As shown in Table 1, Examples 1-3, through the "one-pot aqueous phase method," achieve in-situ polymerization of lithium peroxide nanoparticles on their surface to form a dense conductive polymer shell the instant the nanoparticles are generated. This shell possesses excellent water-repellent and lithium-ion-conducting properties, completely isolating the highly active, high-capacity lithium peroxide core from water, fundamentally solving the problem that high-capacity inorganic lithium replenishing agents cannot stably exist in aqueous slurries. Compared to traditional lithium replenishing slurries that require expensive and toxic organic solvents, the slurry of this invention uses deionized water as the dispersion medium, making it not only environmentally friendly and inherently safe, but also seamlessly integrated into existing aqueous electrode coating production lines for lithium-ion batteries, significantly reducing production costs and environmental risks.

[0036] Examples 1-3 describe the in-situ generation of lithium peroxide via CO-Li covalent grafting onto oxygen-containing functional groups on the surface of single-walled carbon nanotubes. The relationship between the single-walled carbon nanotubes and the lithium-filling material is no longer physical contact, but rather atomic-scale chemical bonding. This not only eliminates the electron transport barrier between them but also ensures the stability of the composite structure under volume changes during slurry stirring, coating, and long-term battery cycling, preventing particle agglomeration and desorption. Simultaneously, the single-walled carbon nanotubes themselves are excellent electronic conductors, while the covalently grafted lithium salt-doped conductive polymer shell is a good lithium-ion conductor. This unique core-shell grafting structure constructs a three-dimensional, dual-continuous conductive network in situ within the electrode. Electrons and lithium ions can simultaneously reach the surface of the active material through dedicated channels with the shortest path and lowest impedance, significantly improving the rate performance of the electrode and the utilization rate of the active material.

[0037] Meanwhile, Examples 1-3 introduce a dual-lithium-source synergistic design of "main lithium source - auxiliary lithium source," achieving precise compensation for the consumption of active lithium at different stages of the battery. During the initial charging, when a solid electrolyte interface film is formed, the organic lithium salt can rapidly release lithium ions, precisely compensating for the initial irreversible capacity loss and improving the battery's initial coulombic efficiency. The covalently grafted core-shell lithium peroxide serves as a high-capacity main lithium source, continuously and stably replenishing active lithium in subsequent cycles as the battery's minor side reactions gradually decompose, effectively delaying the battery's capacity drop and extending its cycle life. This sequential relay lithium replenishment strategy of "initial efficiency compensation" and "long-term slow release" achieves intelligent management of active lithium throughout the battery's entire life cycle.

[0038] Comparative Example 1 involved ball milling lithium peroxide powder, single-walled carbon nanotubes, and polyvinylpyrrolidone in water to prepare a conductive slurry. Because the lithium peroxide powder was not coated, it reacted directly with water, generating gas and failing, leading to slurry sedimentation and failure. The core-shell structure of Example 1 perfectly solved this problem. Example 1 achieved a first-cycle coulombic efficiency of 95.6%, far exceeding that of Comparative Example 1, demonstrating that the grafted core-shell lithium supplement can efficiently and controllably release lithium ions. Its overwhelming advantage in cycle retention and rate performance proves the decisive role of the integrated "electron-ion dual-pathway" network in reducing electrode internal resistance and improving kinetics.

[0039] The slurry sample of Comparative Example 2 showed significant flocculation, indicating that the non-covalently adsorbed core-shell particles easily detached from the carbon nanotubes during the reaction and stirring, agglomerating and hindering the conductive network. This resulted in an electrode resistivity much higher than that of Example 1, and the capacity retention rate of Comparative Example 2 after 200 cycles decreased to 88.3%, far lower than that of Example 1. This confirms that the CO-Li chemical bond in Example 1 provides a stable anchor for the lithium replenishment material during long-term cycling, which is the structural basis for its long-term slow-release lithium replenishment.

[0040] Comparative Example 3, without the addition of organic lithium salt, lacked a rapid lithium replenishment method, resulting in an initial coulombic efficiency of only 88.6%, significantly lower than Example 1. This reveals the significant advantage of organic lithium salt in the shell, which can "respond instantly" during the first charge, precisely compensating for the consumption of SEI film formation.

[0041] This invention provides a single-walled carbon nanotube aqueous lithium-ionized conductive slurry and its preparation method. All reactions are carried out in an open system at room temperature and pressure, requiring only conventional cooling water to maintain the nucleation temperature, completely eliminating the dependence of existing technologies on anhydrous and oxygen-free glove boxes and cryogenic equipment. Finally, a high-pressure microfluidic homogenization isothermal method is used for homogenization, obtaining a high-quality slurry without damaging the structure. This simple, mild, and integrated process design offers high batch reproducibility and has a very broad prospect for industrialization.

[0042] Based on the above-described preferred embodiments of the present invention, and through the foregoing description, those skilled in the art can make various changes and modifications without departing from the inventive concept. The technical scope of this invention is not limited to the contents of the specification, but must be determined according to the scope of the claims.

Claims

1. A single-walled carbon nanotube aqueous lithium-ion conductive paste, characterized in that, The raw materials, by weight, include: 3-5 parts single-walled carbon nanotubes, 20-40 parts lithium hydroxide aqueous solution, 30-80 parts hydrogen peroxide aqueous solution, 1.5-2.5 parts 3,4-ethylenedioxythiophene, 1-2 parts lithium bis(trifluoromethanesulfonylimide), 1.5-2.5 parts ammonium persulfate, 0.5-1.5 parts organolithium salt, 0.3-0.5 parts dispersant, and 60-90 parts deionized water.

2. The aqueous lithium-ion conductive paste for single-walled carbon nanotubes according to claim 1, characterized in that, The single-walled carbon nanotubes have a diameter of 1~3nm and a length of 10~30μm.

3. The aqueous lithium-ion conductive paste for single-walled carbon nanotubes according to claim 1, characterized in that, The concentration of the lithium hydroxide aqueous solution is 15~30wt%.

4. The aqueous lithium-ion conductive paste for single-walled carbon nanotubes according to claim 1, characterized in that, The concentration of the hydrogen peroxide aqueous solution is 5~15wt%.

5. The aqueous lithium-ion conductive paste for single-walled carbon nanotubes according to claim 1, characterized in that, The organic lithium salt includes at least one of lithium citrate, lithium polyacrylate, and lithium tartrate.

6. The aqueous lithium-ion conductive paste for single-walled carbon nanotubes according to claim 1, characterized in that, The dispersant includes at least one of polyvinylpyrrolidone, polyvinyl alcohol, and polyethylene glycol p-isooctylphenyl ether.

7. A method for preparing a single-walled carbon nanotube aqueous lithium-ionized conductive paste as described in claims 1-6, characterized in that, Includes the following steps: (1) Weigh each raw material component according to its weight percentage; (2) Add single-walled carbon nanotubes and dispersant to 2 / 3 of deionized water and sonicate at 20~30℃ for 20~60 min to obtain a single-walled carbon nanotube aqueous dispersion. (3) Cool the single-walled carbon nanotube aqueous dispersion to 0~10℃, stir at 100~400rpm and simultaneously add lithium hydroxide aqueous solution and hydrogen peroxide aqueous solution for 30~90min, add 3,4-ethylenedioxythiophene and lithium bis(trifluoromethanesulfonylimide), maintain the temperature at 0~10℃, continue stirring for 15~30min to obtain the reaction system; (4) Dissolve ammonium persulfate in the remaining 1 / 3 of the water and slowly add it dropwise into the reaction system over 45 to 120 minutes. After the addition is complete, raise the temperature to 15°C to 30°C, add the organic lithium salt, and continue stirring the reaction at 100 to 400 rpm for 4 to 8 hours to obtain the composite dispersion. (5) The composite dispersion is homogenized in a high-pressure micro-jet homogenizer 1 to 5 times to obtain a single-walled carbon nanotube aqueous lithium conductive slurry.

8. The method for preparing a single-walled carbon nanotube aqueous lithium-ion conductive paste according to claim 7, characterized in that, The conditions for ultrasonic treatment in step (2) are power 200~600W and frequency 20~40kHz.

9. The method for preparing a single-walled carbon nanotube aqueous lithium-ion conductive paste according to claim 7, characterized in that, The homogenization pressure in step (5) is 500~2000 bar.

Images