A method, device for preparing composite nanofiber assisted separator, zinc-based battery

Abstract

The application discloses a method and device for preparing a composite nanofiber auxiliary diaphragm, and a zinc-based battery for improving zinc negative electrode interface stability. The method comprises the following steps: preparing MXene powder; dissolving the MXene powder and PVDF powder respectively, and preparing MXene solution and PVDF spinning solution; preparing a PVDF fiber auxiliary diaphragm through electrostatic spinning using the PVDF spinning solution; and mixing and stirring the MXene solution and the PVDF spinning solution, and preparing a MXene / PVDF composite nanofiber auxiliary diaphragm through the mixed solution.

Description

Technical Field

[0001] This application relates to the field of electrical engineering, and more particularly to a method, apparatus, and zinc-based battery for preparing a composite nanofiber-assisted separator. Background Technology

[0002] Novel energy storage systems have become an important research direction in the energy field. Compared to traditional lithium-ion batteries, aqueous zinc-ion batteries (AZIBs) use non-flammable aqueous electrolytes, offering advantages such as high safety, high ionic conductivity, abundant zinc resources, low cost, and environmental friendliness. Meanwhile, the zinc anode has a high theoretical capacity and low redox potential, providing an important foundation for constructing high-performance aqueous energy storage devices. Therefore, the technology of aqueous zinc-ion batteries is constantly innovating. However, aqueous zinc-ion batteries (AZIBs) still face a key bottleneck in actual cycling: poor stability of the zinc anode interface. The reasons are as follows: First, Zn... 2+ During deposition / stripping, dendrite growth is easily induced by localized electric field concentration and uneven ion flux distribution, leading to the formation of "dead zinc," membrane puncture, and even battery short circuits. Secondly, parasitic reactions such as hydrogen evolution, corrosion, and byproduct deposition are unavoidable in aqueous environments, continuously consuming active zinc and electrolyte, and significantly increasing interfacial impedance. Furthermore, Zn... 2+ The high charge density and strong solvation effect result in high desolvation and migration energy barriers during cross-interface transport, further exacerbating deposition inhomogeneity and polarization deterioration. Therefore, the coupling between dendrite growth, side reactions, and high-barrier transport is the core reason for the poor interfacial stability of the zinc anode. Summary of the Invention

[0003] This application discloses a method, apparatus, and zinc-based battery for preparing composite nanofiber-assisted separators to improve the interface stability of zinc anodes.

[0004] Existing research mainly focuses on anode surface modification, electrolyte optimization, and separator functionalization. Among these, functional separator design, due to its multiple functions including physical isolation, ion transport regulation, and interfacial electric field optimization, is considered an effective strategy for improving the stability of zinc anodes. Meanwhile, electrospinning technology can construct ultrathin fiber membranes with high porosity, interconnected pores, and adjustable thickness, and can induce PVDF molecular chain orientation and β-phase formation, thereby endowing the separator with stronger polarization characteristics and ion regulation capabilities. Therefore, this application, based on the structural design of functional separators, utilizes electrospinning to prepare modified separators aimed at reshaping the electric field environment and ion transport behavior of the zinc anode surface. By guiding the directional and uniform deposition of zinc ions, this strategy can effectively delay dendrite growth, improve the interfacial stability of the zinc anode, and thus significantly improve the cycle life of the battery while ensuring high coulombic efficiency.

[0005] In a first aspect, embodiments of this application provide a method for preparing a composite nanofiber-assisted membrane, comprising: Preparation of MXene powder; MXene powder and PVDF powder were dissolved separately to prepare MXene solution and PVDF spinning solution; MXene solution and PVDF spinning solution were mixed and stirred, and MXene / PVDF composite nanofiber-assisted membranes were prepared by mixing the mixed solution.

[0006] Optionally, the step of mixing and stirring the MXene solution and the PVDF spinning solution to prepare the MXene / PVDF composite nanofiber-assisted membrane specifically includes: The MXene solution and PVDF spinning solution were mixed and magnetically stirred at a constant temperature to generate the first spinning precursor solution. MXene / PVDF composite nanofibers were prepared using a first spinning precursor solution and an electrospinning method.

[0007] Optionally, the steps of dissolving MXene powder and PVDF powder separately to prepare MXene solution and PVDF spinning solution specifically include: A predetermined mass of PVDF powder is dissolved in a predetermined DMAc / acetone mixed solvent and stirred under a predetermined temperature water bath to prepare a PVDF spinning solution. PVDF fiber-assisted membranes were prepared by electrospinning using PVDF spinning solution. A predetermined mass fraction of MXene powder was placed in a DMAc / acetone mixed solvent and ultrasonically treated under ice bath conditions to prepare an MXene solution.

[0008] Optionally, the steps for preparing MXene powder specifically include: Prepare the first mixture using hydrochloric acid and deionized water, and place the predetermined mass of lithium fluoride and the first mixture into centrifuge tube A; Add the predetermined mass of titanium aluminum carbide to centrifuge tube A in multiple batches and stir. Secure a pair of rubber gloves tightly to the cap of centrifuge tube A with a rubber band, and then place centrifuge tube A in an oil bath at a preset temperature to promote the reaction. After the reaction was completed, the mixed solution in centrifuge tube A was subjected to acid washing and water washing in sequence. The precipitate in the mixed solution was retained and refrigerated. After the refrigeration process is completed, the precipitate is dissolved in deionized water and subjected to ultrasonic and centrifugation treatment until the precipitate is completely separated to generate an MXene solution. The MXene solution was first frozen, and then freeze-dried to obtain MXene powder.

[0009] Optionally, after the step of mixing and stirring the MXene solution and the PVDF spinning solution, and preparing the MXene / PVDF composite nanofiber-assisted membrane from the mixed solution, the method further includes: An MXene / PVDF composite nanofiber-assisted diaphragm is placed between two copper sheets; Copper wires are attached to copper sheets to act as wires connecting to an electrochemical workstation. The assembly performance of pressure electronic devices is then tested using a pre-designed nanoengine and the electrochemical workstation.

[0010] Optionally, after the step of mixing and stirring the MXene solution and the PVDF spinning solution, and preparing the MXene / PVDF composite nanofiber-assisted membrane from the mixed solution, the method further includes: Preparation of MnO2-CNT cathode; Preparation of PV-assisted separators; MXene / PVDF composite nanofiber assisted separator and PV assisted separator were respectively combined with GF separator to form PVMX-F separator system and PV-F separator system. GF separator was used as reference separator system. The separator system was tested with the high potential side of PVMX-F assisted separator and PV-F separator close to zinc negative electrode. The MnO2-CNT cathode was assembled into a PVMX-F membrane system, a PV-F membrane system, and a reference membrane system to form a coin cell, and a test cell pack was generated. The test cell pack was then subjected to battery performance testing.

[0011] Optionally, the steps for preparing the PV-assisted separator specifically include: A mixed solvent was prepared using N,N-dimethylacetamide and acetone; A predetermined mass of polyvinylidene fluoride is dissolved in a mixed solvent to generate a second mixture. The second mixture is placed in a water bath at a preset temperature and stirred to generate a second spinning precursor solution. The second spinning precursor solution is transferred to a syringe, and spinning is performed according to the preset spinning rate and pressure. The PV-assisted diaphragm is then collected.

[0012] Secondly, embodiments of this application provide an apparatus for preparing a composite nanofiber-assisted membrane, comprising: The MXene powder preparation unit is used to prepare MXene powder. The MXene solution and PVDF spinning solution preparation unit is used to dissolve MXene powder and PVDF powder respectively and prepare MXene solution and PVDF spinning solution. A PVDF fiber-assisted membrane generation unit is used to prepare a PVDF fiber-assisted membrane by electrospinning using the PVDF spinning solution. The MXene / PVDF composite nanofiber-assisted membrane generation unit is used to mix and stir MXene solution and PVDF spinning solution, and to prepare MXene / PVDF composite nanofiber-assisted membrane through the mixed solution.

[0013] Optionally, the MXene / PVDF composite nanofiber-assisted membrane generation unit specifically includes: The MXene solution and PVDF spinning solution were mixed and magnetically stirred at a constant temperature to generate the first spinning precursor solution. MXene / PVDF composite nanofibers were prepared using a first spinning precursor solution and an electrospinning method.

[0014] Optionally, the MXene solution and PVDF spinning solution configuration unit specifically includes: A predetermined mass of PVDF powder is dissolved in a predetermined DMAc / acetone mixed solvent and stirred under a predetermined temperature water bath to prepare a PVDF spinning solution. A predetermined mass fraction of MXene powder was placed in a DMAc / acetone mixed solvent and ultrasonically treated under ice bath conditions to prepare an MXene solution.

[0015] Optionally, the MXene powder preparation unit specifically includes: Prepare the first mixture using hydrochloric acid and deionized water, and place the predetermined mass of lithium fluoride and the first mixture into centrifuge tube A; Add the predetermined mass of titanium aluminum carbide to centrifuge tube A in multiple batches and stir. Secure a pair of rubber gloves tightly to the cap of centrifuge tube A with a rubber band, and then place centrifuge tube A in an oil bath at a preset temperature to promote the reaction. After the reaction was completed, the mixed solution in centrifuge tube A was subjected to acid washing and water washing in sequence. The precipitate in the mixed solution was retained and refrigerated. After the refrigeration process is completed, the precipitate is dissolved in deionized water and subjected to ultrasonic and centrifugation treatment until the precipitate is completely separated to generate an MXene solution. The MXene solution was first frozen, and then freeze-dried to obtain MXene powder.

[0016] Optionally, following the MXene / PVDF composite nanofiber-assisted membrane generation unit, the three-dimensional aerogel electrode fabrication device further includes: Placement unit for placing the MXene / PVDF composite nanofiber-assisted separator between two copper sheets; The assembly performance testing unit for pressure electronic devices is used to attach copper wires to a copper sheet to act as wires to connect to an electrochemical workstation, and to perform assembly performance testing of pressure electronic devices using a pre-set nanoengine and an electrochemical workstation.

[0017] Optionally, following the MXene / PVDF composite nanofiber-assisted membrane generation unit, the three-dimensional aerogel electrode fabrication device further includes: MnO2-CNT cathode fabrication unit, used to fabricate MnO2-CNT cathodes; PV-assisted membrane preparation unit, used to prepare PV-assisted membranes; The membrane system preparation unit is used to combine MXene / PVDF composite nanofiber assisted membrane and PV assisted membrane with GF membrane to form PVMX-F membrane system and PV-F membrane system, respectively. GF membrane is used as reference membrane system. The PVMX-F assisted membrane and PV-F assisted membrane are both formed with the side with higher potential close to the zinc negative electrode to form the membrane system for testing. The battery performance testing unit is used to assemble coin cells with MnO2-CNT cathodes, PVMX-F membrane systems, PV-F membrane systems, and reference membrane systems to generate test battery packs, and then to test the battery performance of the test battery packs.

[0018] Optionally, the PV-assisted membrane fabrication unit specifically includes: A mixed solvent was prepared using N,N-dimethylacetamide and acetone; A predetermined mass of polyvinylidene fluoride is dissolved in a mixed solvent to generate a second mixture. The second mixture is placed in a water bath at a preset temperature and stirred to generate a second spinning precursor solution. The second spinning precursor solution is transferred to a syringe, and spinning is performed according to the preset spinning rate and pressure. The PV-assisted diaphragm is then collected.

[0019] Thirdly, embodiments of this application provide a zinc-based battery, comprising a MnO2-CNT cathode, a GF separator, an MXene / PVDF composite nanofiber-assisted separator according to any one of the first aspects, and zinc sheets stacked sequentially, and impregnated with a mixed electrolyte composed of 2 M ZnSO4 and 0.1 M MnSO4.

[0020] As can be seen from the above technical solutions, the embodiments of this application have the following advantages: In this application, MXene powder is first prepared. MXene powder and PVDF powder are dissolved separately to prepare MXene solution and PVDF spinning solution, respectively. PVDF fiber-assisted membranes are prepared by electrospinning using the PVDF spinning solution. The MXene solution and PVDF spinning solution are mixed and stirred, and MXene / PVDF composite nanofiber-assisted membranes are prepared using the mixed solution.

[0021] MXene was uniformly incorporated into PVDF powder via electrospinning to construct a composite functional layer with oriented polarization characteristics, namely an MXene / PVDF composite nanofiber-assisted separator. By controlling the polarization direction of the MXene / PVDF composite nanofiber-assisted separator to align with the direction of the applied charging voltage, a localized electric field pointing towards the zinc surface was formed at the interface between the MXene / PVDF composite nanofiber-assisted separator and the zinc anode, thereby guiding the Zn... 2+ Rapid and uniform migration along a predetermined direction reduces local ion concentration differences and inhibits dendrite growth. Furthermore, the negatively charged functional groups on the surface of MXene materials affect Zn... 2+ It produces an adsorption and enrichment effect, while also affecting OH. - and SO4 2- The anions generate a repulsive effect, which greatly reduces side reactions and by-product deposition on the zinc anode surface and improves the stability of the zinc anode interface. Attached Figure Description

[0022] To more clearly illustrate the technical solutions in the embodiments of this application, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of this application. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0023] Figure 1 This is a schematic diagram of an embodiment of the method for preparing composite nanofiber-assisted membranes according to this application; Figure 2 This is a schematic diagram of an embodiment of the method for testing the assembly performance of pressure electronic devices according to this application; Figure 3 A schematic diagram of an embodiment of a method for testing the battery performance of the battery pack used in this application; Figure 4 A schematic diagram of an embodiment of the apparatus for preparing the composite nanofiber-assisted diaphragm according to this application; Figure 5 This is a schematic diagram of another embodiment of the apparatus for preparing the composite nanofiber-assisted diaphragm according to this application; Figure 6This is a schematic diagram of the structure / operating principle of zinc-based batteries formed by different types of auxiliary separators in this application; Figure 7 This is a schematic diagram of the morphology and internal structure of PVMX in this application; Figure 8 XRD patterns of different diaphragms in this application; Figure 9 This is a schematic diagram of the DC polarization curves and electrochemical impedance spectra before and after polarization of zinc-based batteries formed with different auxiliary separators according to this application. Figure 10 This is a schematic diagram of the output current signal spectrum of the piezoelectric electronic device based on the PVMX diaphragm in this application under forward and reverse connection. Figure 11 This is a schematic diagram illustrating the anodic stability analysis of the auxiliary separator applied in the electroplating / stripping process of a Zn||Zn symmetric cell. Figure 12 This is a schematic diagram illustrating the performance of Zn–MnO2 batteries using GF, PV, and PVMX separators in this application. Detailed Implementation

[0024] In the following description, specific details such as particular system architectures and techniques are set forth for illustrative purposes and not for limitation, in order to provide a thorough understanding of the embodiments of this application. However, those skilled in the art will understand that this application may also be implemented in other embodiments without these specific details. In other instances, detailed descriptions of well-known systems, apparatuses, circuits, and methods have been omitted so as not to obscure the description of this application with unnecessary detail.

[0025] It should be understood that, when used in this application specification and the appended claims, the term "comprising" indicates the presence of the described features, integrals, steps, operations, elements and / or components, but does not exclude the presence or addition of one or more other features, integrals, steps, operations, elements, components and / or a collection thereof.

[0026] It should also be understood that the term “and / or” as used in this application specification and the appended claims means any combination of one or more of the associated listed items and all possible combinations, and includes such combinations.

[0027] As used in this application specification and the appended claims, the term "if" may be interpreted, depending on the context, as "when," "once," "in response to determination," or "in response to detection." Similarly, the phrase "if determined" or "if detected [the described condition or event]" may be interpreted, depending on the context, as meaning "once determined," "in response to determination," "once detected [the described condition or event]," or "in response to detection [the described condition or event]."

[0028] Furthermore, in the description of this application and the appended claims, the terms "first," "second," "third," etc., are used only to distinguish descriptions and should not be construed as indicating or implying relative importance.

[0029] References to "one embodiment" or "some embodiments" as described in this specification mean that one or more embodiments of this application include a specific feature, structure, or characteristic described in connection with that embodiment. Therefore, the phrases "in one embodiment," "in some embodiments," "in other embodiments," "in still other embodiments," etc., appearing in different parts of this specification do not necessarily refer to the same embodiment, but rather mean "one or more, but not all, embodiments," unless otherwise specifically emphasized. The terms "comprising," "including," "having," and variations thereof mean "including but not limited to," unless otherwise specifically emphasized.

[0030] The technical solutions of this application will be clearly and completely described below with reference to the accompanying drawings of the embodiments. Obviously, the described embodiments are only some embodiments of this application, and not all embodiments. Based on the embodiments of this application, all other embodiments obtained by those of ordinary skill in the art without creative effort are within the scope of protection of this application.

[0031] The method described in this application can be applied to servers, devices, terminals, or other devices with logical processing capabilities; therefore, this application does not limit its application. For ease of description, the following description uses a terminal as the executing entity.

[0032] Please see Figure 1 This application provides an embodiment of a method for preparing a composite nanofiber-assisted membrane, comprising: 101. Preparation of MXene powder; In this embodiment, the terminal first prepares a first mixture using hydrochloric acid and deionized water. A predetermined mass of lithium fluoride and the first mixture are placed in centrifuge tube A. Next, a predetermined mass of titanium aluminum carbide is added to centrifuge tube A in multiple batches with stirring. A rubber glove is tightly secured to the cap of centrifuge tube A using a rubber band. Centrifuge tube A is then placed in an oil bath at a predetermined temperature to promote the reaction. After the reaction is complete, the mixture in centrifuge tube A is sequentially acid-washed and water-washed. The precipitate in the mixture is retained and refrigerated. After refrigeration, the precipitate is dissolved in deionized water and subjected to ultrasonic treatment and centrifugation until the precipitate is completely separated, generating an MXene solution. This MXene solution is then frozen and finally freeze-dried to obtain MXene powder.

[0033] Specifically, the following example illustrates the process: First, place 1 g of lithium fluoride (LiF) in centrifuge tube A. Separately, add 12 mL of hydrochloric acid (HCl) and 4 mL of deionized water to centrifuge tube B, and stir for 5 min in an ice bath until homogeneous. Then, transfer the entire mixture from centrifuge tube B to centrifuge tube A, and continue stirring in an ice bath for 10 min to ensure complete dissolution of the lithium fluoride. Weigh 0.45 g of titanium aluminum carbide (Ti3AlC2) and add it to centrifuge tube A in three portions (0.15 g each time). After each addition, stir in an ice bath for 3 min. After the final addition, continue stirring in an ice bath for 20 min. Secure a rubber glove tightly to the cap of centrifuge tube A with a rubber band (to regulate the gas pressure balance during the reaction and prevent gas leakage), and then place the centrifuge tube in a 40°C oil bath for 48 h. After the reaction is complete, measure 40 mL of hydrochloric acid and 40 mL of deionized water into a beaker, mix and stir for 5 min, and pour this solution into centrifuge tube A for acid washing. After vortexing and mixing, centrifuge at 4000 r / min for 5 min and discard the supernatant. Repeat this acid washing step three times. After acid washing, add deionized water and repeat the above centrifugation and washing operation. After washing three times with water, retain the precipitate and refrigerate it in a refrigerator for 10 h. After refrigeration, measure 100 mL of deionized water to dissolve the precipitate in a beaker and sonicate for 30 min. Then centrifuge at 4000 r / min for 5 min and collect the supernatant. Repeat this sonication-centrifugation separation step until the precipitate is completely separated, and finally obtain a set of raw material MXene solutions. Then freeze the MXene solutions and finally freeze-dry them to obtain MXene powder.

[0034] 102. Dissolve MXene powder and PVDF powder separately to prepare MXene solution and PVDF spinning solution; A predetermined mass of PVDF powder is dissolved in a predetermined DMAc / acetone mixed solvent and stirred under a predetermined temperature water bath to generate a PVDF spinning solution. A predetermined mass fraction of MXene powder is placed in a DMAc / acetone mixed solvent and ultrasonically treated under ice bath conditions to prepare an MXene solution.

[0035] Specifically, the following example illustrates this: First, 1.5 g of PVDF was dissolved in a DMAc / acetone mixed solvent with a volume ratio of 1:1, and stirred at 1000 rpm for 1 hour in a 60°C water bath. Simultaneously, 0.8% by mass of MXene powder was dispersed in the same DMAc / acetone mixed solvent and ultrasonically treated in an ice bath for 1 hour.

[0036] 103. PVDF fiber-assisted membranes were prepared by electrospinning using PVDF spinning solution; 104. Mix and stir the MXene solution and the PVDF spinning solution, and prepare an MXene / PVDF composite nanofiber assisted membrane through the mixed solution.

[0037] MXene solution and PVDF spinning solution were mixed and magnetically stirred to generate a first spinning precursor solution. MXene / PVDF composite nanofibers were prepared using this first spinning precursor solution and an electrospinning method.

[0038] Specifically, the following example illustrates this: MXene solution and PVDF spinning solution were mixed and magnetically stirred for 0.5 hours to obtain a spinning precursor solution. Finally, using electrospinning technology under the same conditions, an MXene / PVDF (PVMX) composite nanofiber-assisted membrane was successfully prepared.

[0039] In this application, MXene powder is first prepared. MXene powder and PVDF powder are dissolved separately to prepare MXene solution and PVDF spinning solution, respectively. PVDF fiber-assisted membranes are prepared by electrospinning using the PVDF spinning solution. The MXene solution and PVDF spinning solution are mixed and stirred, and MXene / PVDF composite nanofiber-assisted membranes are prepared using the mixed solution.

[0040] MXene was uniformly incorporated into PVDF powder via electrospinning to construct a composite functional layer with oriented polarization characteristics, namely an MXene / PVDF composite nanofiber-assisted separator. By controlling the polarization direction of the MXene / PVDF composite nanofiber-assisted separator to align with the direction of the applied charging voltage, a localized electric field pointing towards the zinc surface was formed at the interface between the MXene / PVDF composite nanofiber-assisted separator and the zinc anode, thereby guiding the Zn... 2+ Rapid and uniform migration along a predetermined direction reduces local ion concentration differences and inhibits dendrite growth. Furthermore, the negatively charged functional groups on the surface of MXene materials affect Zn... 2+ It produces an adsorption and enrichment effect, while also affecting OH. - and SO4 2- The anions generate a repulsive effect, which greatly reduces side reactions and by-product deposition on the zinc anode surface and improves the stability of the zinc anode interface.

[0041] Meanwhile, the introduction of MXene can improve membrane wettability, reduce interfacial contact resistance, and enhance ion transport kinetics and battery rate performance. Compared with existing technologies, this embodiment achieves a synergistic unity of interfacial electric field regulation, ion selective transport, and interfacial protection, simultaneously improving zinc deposition uniformity, cycle life, capacity retention, and rate performance. It provides a new membrane design scheme for the development of high-capacity, long-life aqueous zinc-ion batteries and can be extended to other metal anode energy storage devices.

[0042] Please see Figure 2 This application provides an embodiment of a method for testing the assembly performance of pressure electronic devices, comprising: 201. Place the MXene / PVDF composite nanofiber-assisted diaphragm between two copper sheets; 202. Copper wires are attached to copper sheets to act as wires to connect to the electrochemical workstation. The assembly performance of the pressure electronic device is tested using the preset nanoengine and electrochemical workstation.

[0043] In this embodiment, an MXene / PVDF composite nanofiber auxiliary diaphragm is placed between copper sheets at the top and bottom, and transparent tape is wrapped and fixed on a glass slide. Copper wires are attached to the copper sheets to act as wires connecting to the electrochemical workstation. The nanoengine and the electrochemical workstation are used for performance testing.

[0044] Please see Figure 3 This application provides an embodiment of a method for testing battery pack performance, comprising: 301. Preparation of MnO2-CNT cathode; 302. Preparation of PV-assisted separator; In this embodiment, a mixed solvent is first prepared by N,N-dimethylacetamide and acetone. Then, a preset mass of polyvinylidene fluoride is placed in the mixed solvent to dissolve and generate a second mixture. Next, the second mixture is placed in a water bath at a preset temperature and stirred to generate a second spinning precursor solution. Then, the second spinning precursor solution is transferred to a syringe, and spinning is performed according to a preset spinning rate and pressure. The PVDF fiber film is then collected.

[0045] Specifically, the following example illustrates the process: First, 1.5 g of polyvinylidene fluoride (PVDF) was dissolved in a mixed solvent consisting of 3 mL of N,N-dimethylacetamide and 3 mL of acetone. This mixture was then placed in a 60°C water bath and stirred at 1000 rpm for 1 h to obtain a homogeneous spinning precursor solution. The resulting solution was transferred to a syringe, and spinning was performed at a rate of 0.03 mL / min under a high voltage of 18 kV. The nanofibers were collected on a roller at a speed of 1520 rpm, with a receiving distance (needle tip to collector surface) of 15 cm. The ambient temperature was controlled at 25°C and the humidity at 48% during the spinning process. After spinning, the collected PVDF fiber film was peeled off from the release paper and dried in a 60°C oven for at least 6 h to obtain the second set of raw material, the PV-assisted separator.

[0046] 302. The MXene / PVDF composite nanofiber assisted separator and the PV assisted separator were respectively combined with the GF separator to form the PVMX-F separator system and the PV-F separator system. The GF separator was used as the reference separator system. The PVMX-F assisted separator and the PV-F assisted separator were both formed with the side with the higher potential close to the zinc negative electrode to form the separator system for testing. 303. Assemble coin cells with MnO2-CNT cathodes, PVMX-F membrane system, PV-F membrane system and reference membrane system respectively to generate test cell packs, and perform battery performance tests on the test cell packs.

[0047] The batteries used for electrochemical performance testing in this application mainly include Zn||Zn symmetric cells, Zn||Cu half-cells, and Zn||MnO2-CNT cathode full cells. The batteries were assembled based on the MXene / PVDF composite nanofiber-assisted separator and other reference auxiliary separators, with the CR2032 coin cell type being the primary assembly method. Different electrolytes were selected for assembly and performance evaluation of different battery systems according to the testing objectives. It should be noted that during battery assembly, the side with the higher potential PV separator (MXene / PVDF composite nanofiber-assisted separator) was placed close to the zinc anode (PV-F is an electrospun separator attached to the outer surface of the collecting paper, exhibiting a lower potential on the upper surface) and assembled with GF to form the separator system. The Zn||Zn symmetric cells and Zn||Cu half-cells were tested in 2 M ZnSO4 electrolyte to characterize the deposition / stripping behavior and reversibility of the zinc anode. For Zn||MnO2-CNT full cells, a mixed electrolyte consisting of 2 M ZnSO4 and 0.1 M MnSO4 is used to meet the electrochemical reaction requirements of the MnO2-based cathode during charge and discharge, and to evaluate the overall energy storage performance of the full cell.

[0048] Specifically, the following example illustrates the assembly and testing of an aqueous zinc-ion battery. First, MXene / PVDF composite nanofiber-assisted separators and PV-assisted separators are combined with GF separators to form a separator system. This system is then assembled with positive and negative button cells, spacers, and spring sheets to create a zinc-based battery. Zn||Zn symmetric cell tests and Zn||Cu half-cell tests are then performed. (The side of the MXene / PVDF composite nanofiber-assisted separator facing the zinc negative electrode has the highest potential, PVMX-F, and PV-F is also the side with the highest potential.) Next, a simple one-step hydrothermal method was used to prepare MnO2-CNT composite materials. Specifically, 0.2 g of commercial multi-walled carbon nanotubes were first dispersed in 120 mL of deionized water, followed by the addition of 0.973 g of potassium permanganate and continuous stirring for 0.5 h. Separately, 2.27 g of manganese acetate tetrahydrate was dissolved in 20 mL of deionized water to prepare a homogeneous solution, which was then slowly added dropwise to the above mixture and ultrasonically stirred for 1 h to promote a complete reaction. The resulting mixture was transferred to an autoclave and subjected to hydrothermal reaction at 120 °C for 12 hours. After cooling to room temperature, the brownish-red product was collected by filtration, rinsed multiple times with deionized water, and then dried overnight under vacuum at room temperature to obtain the MnO2-CNT composite material. Subsequently, the electrode coating slurry was prepared: using N-methylpyrrolidone as a solvent, the active component, conductive carbon black, and PVDF were mixed in a mass ratio of 8:1:1 and mechanically stirred for 3 hours to promote thorough dispersion within the system and construct a homogeneous electrode slurry. The slurry was then uniformly coated onto the surface of carbon paper using a doctor blade coating method and dried under vacuum at 40°C, ultimately yielding an effective MnO2 loading of approximately 2.0 mg / cm³. -2 The MnO2-CNT cathode electrode was used. This cathode electrode was then assembled into a coin cell with a PVMX-F, PV-F, or GF separator system. To investigate the performance of the obtained cells, constant current charge-discharge (GCD), cyclic voltammetry (CV) curves, rate performance, and long-cycle performance were analyzed in subsequent zinc-based cell examples.

[0049] Please see Figure 4 This application provides an apparatus for preparing composite nanofiber-assisted membranes, comprising: MXene powder preparation unit 401 is used to prepare MXene powder; The MXene solution and PVDF spinning solution preparation unit 402 is used to dissolve MXene powder and PVDF powder respectively and prepare MXene solution and PVDF spinning solution. The PVDF fiber-assisted membrane generation unit 403 is used to prepare a PVDF fiber-assisted membrane by electrospinning using a PVDF spinning solution. The MXene / PVDF composite nanofiber-assisted membrane generation unit 404 is used to mix and stir the MXene solution and the PVDF spinning solution, and to prepare the MXene / PVDF composite nanofiber-assisted membrane through the mixed solution.

[0050] Optionally, the MXene / PVDF composite nanofiber-assisted membrane generation unit 404 specifically includes: The MXene solution and PVDF spinning solution were mixed and magnetically stirred to generate the first spinning precursor solution. MXene / PVDF composite nanofibers were prepared using a first spinning precursor solution and an electrospinning method.

[0051] Optionally, the MXene solution and PVDF spinning solution configuration unit 402 specifically includes: A PVDF spinning solution is prepared by dissolving a preset mass of PVDF powder in a preset DMAc / acetone mixed solvent and stirring it in a water bath at a preset temperature. A predetermined mass fraction of MXene powder was placed in a DMAc / acetone mixed solvent and ultrasonically treated under ice bath conditions to prepare an MXene solution.

[0052] Optionally, the MXene powder preparation unit 401 specifically includes: Prepare the first mixture using hydrochloric acid and deionized water, and place the predetermined mass of lithium fluoride and the first mixture into centrifuge tube A; Add the predetermined mass of titanium aluminum carbide to centrifuge tube A in multiple batches and stir. Secure a pair of rubber gloves tightly to the cap of centrifuge tube A with a rubber band, and then place centrifuge tube A in an oil bath at a preset temperature to promote the reaction. After the reaction was completed, the mixed solution in centrifuge tube A was subjected to acid washing and water washing in sequence. The precipitate in the mixed solution was retained and refrigerated. After the refrigeration process is completed, the precipitate is dissolved in deionized water and subjected to ultrasonic and centrifugation treatment until the precipitate is completely separated to generate an MXene solution. The MXene solution was first frozen, and then freeze-dried to obtain MXene powder.

[0053] Optionally, following the MXene / PVDF composite nanofiber-assisted membrane generation unit 403, the three-dimensional aerogel electrode fabrication device further includes: Placement unit for placing the MXene / PVDF composite nanofiber-assisted separator between two copper sheets; The assembly performance testing unit for pressure electronic devices is used to attach copper wires to a copper sheet to act as wires to connect to an electrochemical workstation, and to perform assembly performance testing of pressure electronic devices using a pre-set nanoengine and an electrochemical workstation.

[0054] Optionally, following the MXene / PVDF composite nanofiber-assisted membrane generation unit 403, the three-dimensional aerogel electrode fabrication device further includes: MnO2-CNT cathode fabrication unit, used to fabricate MnO2-CNT cathodes; PV-assisted membrane preparation unit, used to prepare PV-assisted membranes; The membrane system preparation unit is used to combine MXene / PVDF composite nanofiber assisted membrane and PV assisted membrane with GF membrane to form PVMX-F membrane system and PV-F membrane system, respectively. GF membrane is used as reference membrane system. The PVMX-F assisted membrane and PV-F assisted membrane are both formed with the side with higher potential close to the zinc negative electrode to form the membrane system for testing. The battery performance testing unit is used to assemble coin cells with MnO2-CNT cathodes, PVMX-F membrane systems, PV-F membrane systems, and reference membrane systems to generate test battery packs, and then to test the battery performance of the test battery packs.

[0055] Optionally, the PV-assisted membrane fabrication unit specifically includes: A mixed solvent was prepared using N,N-dimethylacetamide and acetone; A predetermined mass of polyvinylidene fluoride is dissolved in a mixed solvent to generate a second mixture. The second mixture is placed in a water bath at a preset temperature and stirred to generate a second spinning precursor solution. The second spinning precursor solution is transferred into a syringe, and spinning is performed according to the preset spinning rate and pressure. The PVDF nanofiber membrane is then collected.

[0056] Please see Figure 5 This application provides an apparatus for preparing composite nanofiber-assisted membranes, comprising: Processor 501, memory 502, input / output unit 503, and bus 504.

[0057] The processor 501 is connected to the memory 502, the input / output unit 503, and the bus 504.

[0058] The memory 502 stores a program, and the processor 501 calls the program to execute it, such as... Figure 1 , Figure 2 and Figure 3 The method in the middle.

[0059] This application provides a computer-readable storage medium on which a program is stored, and when the program is executed on a computer, it performs the following... Figure 1 , Figure 2 and Figure 3 The method in the middle.

[0060] Please refer to Figure 6 , Figure 6 This diagram illustrates the structure and operating principle of a zinc-based battery with different types of auxiliary membranes. It shows a sequentially stacked structure consisting of a MnO2-CNT cathode, a GF membrane, an MXene / PVDF composite nanofiber auxiliary membrane, and zinc sheets, impregnated with a mixed electrolyte composed of 2 M ZnSO4 and 0.1 M M MnSO4. Figure 6 As can be seen, the GF separator is a GR-assisted separator, the PV-F separator is a combination of a PV-assisted separator and a GR-assisted separator, and the PVMX-F separator is a combination of an MXene / PVDF composite nanofiber-assisted separator and a GR-assisted separator. The battery has a zinc sheet at the bottom, a MnO2-CNT cathode at the top, and a mixed electrolyte consisting of 2 M ZnSO4 and 0.1 M MnSO4, filled with SO42-. 2- .

[0061] Please refer to the following. Figure 7 , Figure 7 This is a schematic diagram of the internal structure and operating principle of PVMX, where PVMX is an abbreviation for MXene / PVDF composite nanofiber-assisted membrane. Specifically, Figure 6 In Figure 7 (a) is a SEM image of MXene. Figure 7 (b) is a TEM image of MXene. Figure 7 (c) is a SEM image of the side of the PVMX membrane. Figure 7 (d) and Figure 7 (e) shows the SEM image and corresponding elemental distribution diagram of the PVMX membrane. Figure 7 (f) is a TEM image of the PVMX membrane.

[0062] Depend on Figure 7 It can be seen that MXene has a nanosheet structure and PVDF has a fiber channel structure. MXene was successfully exfoliated and embedded in the PVDF fiber network, and MXene can be seen to be uniformly dispersed in PVDF.

[0063] Figure 8 The XRD patterns of these three membranes show that the peak intensity of the α phase of PVMX is weakened after the introduction of MXene, while the peak intensity of the β phase is enhanced, indicating that the transformation from α phase to β phase is promoted and the polarization is enhanced.

[0064] Please refer to Figure 9 , Figure 9 This diagram illustrates the DC polarization curves and electrochemical impedance spectra before and after polarization of zinc-based batteries formed with different auxiliary separators. (Specific details...) Figure 9 (a) Figure 9 (b) and Figure 9 (c) shows the DC polarization curves and electrochemical impedance spectra of Zn||Zn symmetric cells with GF, PV-F and PVMX-F separators, respectively.

[0065] from Figure 9 As can be seen, ion transport number testing is used to characterize zinc ions. This is to accurately quantify the effect of different membranes on Zn. 2+ To investigate the impact of transport efficiency, this study used a combination of AC impedance spectroscopy and DC potentiostatic polarization to determine the transport number in a Zn||Zn symmetric cell. The experiment began with an initial EIS scan of the assembled battery within a scanning frequency range of 1 MHz–0.01 Hz to determine its initial interface impedance. Subsequently, a small voltage of 10 mV was applied to the battery for polarization. After the current evolved to steady-state equilibrium, an EIS spectrum was acquired again to obtain the corresponding steady-state impedance. Finally, combining the instantaneous current before and after polarization, the steady-state current, and relevant resistance parameters, the following formula was used to calculate... :

[0066] in The DC polarization potential applied to the battery. and These are the initial instantaneous current and the steady-state current, respectively. and These are the initial impedance and steady-state impedance, respectively. The liquid underwent cyclic charge-discharge testing. The current density was set to 0.5 mA / cm². 2 .

[0067] To investigate the effect of MXene introduction into the PVDF membrane on ion transport, electrochemical impedance spectroscopy (EIS) was measured to estimate the ion transport number of the membrane. ). Figure 9 It is evident that the PVMX film exhibits a higher ion transfer number (0.86) than both pure PVDF (0.73) and GF (0.42), demonstrating faster ion diffusion. Enhanced ionic conductivity and Zn... 2+ The transport number indicates that the introduction of MXene is beneficial for regulating the transport kinetics of ions through the membrane, resulting in more abundant and faster Zn transport. 2+ Transport. Negatively charged MXene will promote Zn transport through electrostatic interactions. 2+ The diffusion of MXene. Theoretical calculations also support the introduction of MXene, demonstrating lower Zn content.2+ Diffusion barrier.

[0068] Please refer to Figure 10 , Figure 10 The output current signal spectra of a PVMX-based piezoelectric device under forward (a) and reverse (b) connections are shown. To detect the difference between the two sides of the PVDF film, the It curve was measured (…). Figure 10 The spun membrane appears identical on both sides. When the two electrodes are connected in opposite directions, the output signals are the same. However, the diagram shows a clear difference between the two, indicating they are not the same. The side facing the spinneret exhibits a more negative potential.

[0069] by Figure 11 Inspired by this analysis, this embodiment applies GF, PV-F, and PVMX-F auxiliary separators to Zn||Zn symmetric cells to further explore anodic stability during the electroplating / stripping process. Figure 11 As shown in (a), the symmetric Zn||Zn cell with a GF separator can only operate normally for a very short time. Even at 1 mA cm⁻¹ -2 The current density and 0.25 mAh cm⁻¹ -2 Under low cycle capacity conditions, the battery exhibited poor cycle performance, experiencing a short circuit due to severe dendrite formation after only 470 hours of cycling, resulting in drastic voltage fluctuations. In contrast, the symmetric battery using a PV-F separator achieved a cycle life of 1600 hours under the same conditions (1 mA cm⁻², 0.25 mAh cm⁻²). This demonstrates the positive effect of the PV-F separator on the reversibility of zinc electrode deposition / dissolution, primarily due to its ability to regulate the electrolyte environment. Notably, the symmetric battery using a PVMX-F separator achieved a higher cycle life at 1 mA cm⁻². -2 Stable cycling for more than 4300 hours under certain conditions. Figure 11 (b) at 5 mA cm -2 and 2.5 mAh cm -2 Under higher current conditions, the battery with PVMX-F separator also exhibits a longer cycle life (2600 hours), which is significantly better than the battery with PV-F separator (300 hours) or GF separator (110 hours). Figure 11 (c) even at 10 mA cm -2 and 5mAh cm -2 Under extremely harsh conditions, batteries using PVMX-F separators still achieve excellent cycle life (2200 hours), which is more than 10 times that of PV-F separators (200 hours) under the same conditions, and more than 40 times that of GF separators (50 hours).

[0070] Please refer to Figure 12 , Figure 12A schematic diagram showing the performance of Zn–MnO2 cells using GF, PV, and PVMX separators. Figure 12 (a) 0.1 mV s for three types of diaphragms -1 The cyclic current-voltage curve below, Figure 12 (b) is 0.1 A g -1 Constant current charge-discharge test curves under current density, Figure 12 (c) is a schematic diagram of the rate capability. Figure 12 (d) is 4 A g -1 Schematic diagram of long-cycle performance at current density To further explore the practical applications of PVMX-F, in this embodiment, a Zn–MnO2 coin cell was assembled with zinc as the anode and MnO2-CNT as the cathode. The MnO2-CNT was synthesized via a one-step hydrothermal method, and its successful preparation was confirmed by XRD and SEM. Cyclic voltammetry curves show that at 0.1 mV s... -1 At the scan rate, for the three membranes GF, PV, and PVMX, two sets of redox peaks showed similar patterns (please refer to...). Figure 12 (a)), which is related to Mn 4+ and Mn 2 + The two-step reverse redox process of valence state transition corresponds to each other, further verifying the consistency of charge storage. In the PVMX-F system, the potential difference of the redox peaks (0.136 V) is significantly lower than that of the PV-F system (0.177 V) and the GF system (0.19 V). Furthermore, Figure 12 (b) at 0.1 A g -1 At current densities of up to 330 mAh g, the discharge capacity of the full-cell system using the PVMX-F separator reaches 330 mAh g. -1 (Based on the mass of active material), it is also significantly higher than that using a GF membrane (184 mAh g). -1 ), and a full-cell system using a PV-F separator (126 mAh g), -1 The galvanostatic charge-discharge curves of the three full-cell systems (GF, PV, and PVMX) exhibit similar characteristic plateaus, which is consistent with previous cyclic voltammetry test results. Figure 12 (c) demonstrates the excellent rate performance of the PVMX membrane full cell, as the current density increases from 0.1 A g. -1 up to 1 A g -1 The PVMX membrane-coated full cell still maintained a capacity retention of 41.8%, significantly higher than the GF membrane system's 29.7% and the PV membrane system's 26.04%. When the current density returned to 1 A g... -1The PVMX-F exhibits a capacity retention rate of 96.7% relative to its initial state, significantly exceeding that of the PV-F (71.7%) and GF systems (42.4%), demonstrating superior stability. Figure 12 (d) It can be seen that the PVMX membrane at 4 A g -1 After 2000 cycles at a current density, it still maintains a capacity retention of 72% and a coulombic efficiency of nearly 100%, which is higher than that of GF membrane (13.4%) and PV (65.6%), demonstrating excellent long-cycle stability.

[0071] This embodiment introduces MXene into a PVDF nanofiber membrane to construct a composite functional layer with oriented polarization characteristics. This layer synergistically exerts interfacial electric field modulation, zinc-loving adsorption, and rapid ion transport, thereby improving the membrane's wettability, interfacial polarization capability, and Zn content. 2+ Transport dynamics.

[0072] This embodiment can effectively guide Zn 2+ Uniform migration and deposition reduce the local current density and nucleation energy barrier on the zinc anode surface, inhibit zinc dendrite growth, hydrogen evolution corrosion and by-product deposition, and significantly improve the reversibility and interface stability of the zinc anode deposition / stripping process.

[0073] This embodiment can significantly improve the cycle life, coulombic efficiency, rate performance and capacity retention of aqueous zinc-ion batteries. In particular, it exhibits excellent stability under high current density and long cycle conditions, and can be extended to other metal anode energy storage systems.

[0074] Those skilled in the art will clearly understand that, for the sake of convenience and brevity, the specific working processes of the systems, devices, and units described above can be referred to the corresponding processes in the foregoing method embodiments, and will not be repeated here.

[0075] In the several embodiments provided in this application, it should be understood that the disclosed systems, apparatuses, and methods can be implemented in other ways. For example, the apparatus embodiments described above are merely illustrative; for instance, the division of units is only a logical functional division, and in actual implementation, there may be other division methods. For example, multiple units or components may be combined or integrated into another system, or some features may be ignored or not executed. Furthermore, the coupling or direct coupling or communication connection shown or discussed may be an indirect coupling or communication connection between apparatuses or units through some interfaces, and may be electrical, mechanical, or other forms.

[0076] The units described as separate components may or may not be physically separate. The components shown as units may or may not be physical units; that is, they may be located in one place or distributed across multiple network units. Some or all of the units can be selected to achieve the purpose of the embodiments of this application, depending on actual needs.

[0077] Furthermore, the functional units in the various embodiments of this application can be integrated into one processing unit, or each unit can exist physically separately, or two or more units can be integrated into one unit. The integrated unit can be implemented in hardware or as a software functional unit.

[0078] If the integrated unit is implemented as a software functional unit and sold or used as an independent product, it can be stored in a computer-readable storage medium. Based on this understanding, the technical solution of this application, in essence, or the part that contributes to the prior art, or all or part of the technical solution, can be embodied in the form of a software product. This computer software product is stored in a storage medium and includes several instructions to cause a computer device (which may be a personal computer, server, or network device, etc.) to execute all or part of the steps of the methods described in the various embodiments of this application. The aforementioned storage medium includes various media capable of storing program code, such as USB flash drives, portable hard drives, read-only memory (ROM), random access memory (RAM), magnetic disks, or optical disks.

Claims

1. A method for preparing a composite nanofiber-assisted membrane, characterized in that, include: Preparation of MXene powder; The MXene powder and PVDF powder were dissolved separately to prepare MXene solution and PVDF spinning solution; A PVDF fiber-assisted membrane was prepared by electrospinning using the PVDF spinning solution. The MXene solution and the PVDF spinning solution were mixed and stirred, and the MXene / PVDF composite nanofiber assisted membrane was prepared by mixing the solution.

2. The method according to claim 1, characterized in that, The step of mixing and stirring the MXene solution and the PVDF spinning solution to prepare the MXene / PVDF composite nanofiber-assisted membrane specifically includes: The MXene solution and the PVDF spinning solution are mixed and subjected to constant temperature magnetic stirring to generate a first spinning precursor solution. MXene / PVDF composite nanofibers were prepared using the first spinning precursor solution and electrospinning method.

3. The method according to claim 2, characterized in that, The steps of dissolving the MXene powder and PVDF powder separately to prepare MXene solution and PVDF spinning solution specifically include: A predetermined mass of PVDF powder is dissolved in a predetermined DMAc / acetone mixed solvent and stirred under a predetermined temperature water bath to prepare a PVDF spinning solution. The MXene powder of a predetermined mass fraction was placed in a DMAc / acetone mixed solvent and ultrasonically treated under ice bath conditions to prepare an MXene solution.

4. The method according to claim 1, characterized in that, The specific steps for preparing MXene powder include: The first mixture was prepared using hydrochloric acid and deionized water. A predetermined mass of lithium fluoride and the first mixture were placed into centrifuge tube A. Take a preset mass of titanium aluminum carbide and add it to the centrifuge tube A in multiple batches while stirring. Secure a pair of rubber gloves tightly to the cap of centrifuge tube A with a rubber band, and then place centrifuge tube A in an oil bath at a preset temperature to promote the reaction. After the reaction is complete, the mixed solution in centrifuge tube A is subjected to acid washing and water washing treatment in sequence; The precipitate in the mixed solution is retained and subjected to refrigeration. After the refrigeration process is completed, the precipitate is dissolved in deionized water and subjected to ultrasonic and centrifugation treatment until the precipitate is completely separated to generate an MXene solution. The MXene solution was first frozen, and then freeze-dried to obtain MXene powder.

5. The method according to any one of claims 1 to 4, characterized in that, After the step of mixing and stirring the MXene solution and the PVDF spinning solution, and preparing the MXene / PVDF composite nanofiber-assisted membrane through the mixed solution, the method further includes: An MXene / PVDF composite nanofiber-assisted diaphragm is placed between two copper sheets; Copper wires are attached to a copper sheet to act as wires to connect to an electrochemical workstation. The assembly performance of the pressure electronic device is tested using a pre-designed nanoengine and the electrochemical workstation.

6. The method according to any one of claims 1 to 4, characterized in that, After the step of mixing and stirring the MXene solution and the PVDF spinning solution, and preparing the MXene / PVDF composite nanofiber-assisted membrane through the mixed solution, the method further includes: Preparation of MnO2-CNT cathode; Preparation of PV-assisted separators; MXene / PVDF composite nanofiber assisted separator and PV assisted separator were respectively combined with GF separator to form PVMX-F separator system and PV-F separator system. GF separator was used as reference separator system. The separator system was tested with the high potential side of PVMX-F assisted separator and PV-F separator close to zinc negative electrode. The MnO2-CNT cathode is assembled into a button cell with the PVMX-F membrane system, the PV-F membrane system and the reference membrane system to generate a test battery pack, and the battery performance of the test battery pack is tested.

7. The method according to claim 6, characterized in that, The specific steps for preparing the PV-assisted separator include: A mixed solvent was prepared using N,N-dimethylacetamide and acetone; A predetermined mass of polyvinylidene fluoride is dissolved in the mixed solvent to generate a second mixture; The second mixture is placed in a water bath at a preset temperature and stirred to generate a second spinning precursor solution. The second spinning precursor solution is transferred to a syringe, and spinning is performed according to a preset spinning rate and pressure. The PV-assisted diaphragm is then collected.

8. An apparatus for preparing a composite nanofiber-assisted membrane, characterized in that, include: The MXene powder preparation unit is used to prepare MXene powder. An MXene solution and PVDF spinning solution preparation unit is used to dissolve the MXene powder and PVDF powder respectively and prepare them into MXene solution and PVDF spinning solution; A PVDF fiber-assisted membrane generation unit is used to prepare a PVDF fiber-assisted membrane by electrospinning using the PVDF spinning solution. The MXene / PVDF composite nanofiber-assisted membrane generation unit is used to mix and stir the MXene solution and the PVDF spinning solution, and to prepare the MXene / PVDF composite nanofiber-assisted membrane through the mixed solution.

9. The three-dimensional aerogel electrode fabrication apparatus according to claim 8, characterized in that, The MXene / PVDF composite nanofiber-assisted membrane generation unit specifically includes: The MXene solution and the PVDF spinning solution are mixed and subjected to constant temperature magnetic stirring to generate a first spinning precursor solution. MXene / PVDF composite nanofibers were prepared using the first spinning precursor solution and electrospinning method.

10. A zinc-based battery, characterized in that, The membrane consists of a MnO2-CNT cathode, a GF membrane, an MXene / PVDF composite nanofiber-assisted membrane as described in any one of claims 1 to 7, and a zinc sheet stacked sequentially, and is impregnated with a mixed electrolyte composed of 2 M ZnSO4 and 0.1 M MnSO4.

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