Hierarchical microphase separation strain enhanced ionic conductive elastomer fiber as well as preparation method and application thereof

Abstract

The invention relates to a hierarchical microphase separation strain enhanced ionic conductive elastomer fiber and a preparation method and application thereof, the interior of the ionic conductive elastomer fiber has a bicontinuous network structure, and the ionic conductive elastomer fiber comprises an EOEOEA / PAA continuous phase and a PEA / LiTFSI continuous phase which are interpenetrated. According to the fiber, a copolymer P (PEA-co-EOEOEA) is used as a structural framework, an EOEOEA / PAA continuous phase is constructed by an EOEOEA chain segment and PAA based on a hydrogen-bond interaction, a PEA / LiTFSI continuous phase is constructed by a PEA chain segment and LiTFSI based on a strong coordination interaction, the EOEOEA / PAA continuous phase is used as a mechanical reinforcement phase, and the PEA / LiTFSI continuous phase is used as an ion transport phase. Through hierarchical microphase separation engineering and a dual swelling process, a bicontinuous network structure with EOEOEA chain segment (soft segment) / PAA as a mechanical reinforcement phase and PEA chain segment (hard segment) / LiTFSI as an ion transport phase is constructed, collaborative optimization of mechanical properties and conductivity is realized, and the performance of the composite material is improved. The ionic conductive elastomer fiber with ultrahigh stretchability, toughness, rapid self-repairing property and strain-insensitive ionic conductivity is obtained, and meanwhile, simple and continuous preparation of the fiber is realized.

Description

Technical Field

[0001] This invention relates to the field of flexible conductive materials technology, and in particular to a layered microphase separation strain-enhanced ion-conductive elastomer fiber, its preparation method, and its application. Background Technology

[0002] The rapid development of flexible electronics technology has placed extremely high demands on stretchable conductive materials, requiring them to maintain stable electrical signal output under dynamic deformation. Ion-conductive elastomers, due to their absence of liquid electrolytes, have become a research hotspot in this field and are being widely explored for applications in wearable electronics, soft robots, conductive components, sensors, and electrodes.

[0003] Currently, researchers have proposed strategies such as constructing ridge structures and porous networks to reduce the strain sensitivity of ion-conducting elastomers, but these methods are mostly implemented only in thin film materials. Fibrous conductors, due to their flexibility, breathability, and weavability, are more valuable for wearable applications. However, existing ion-conducting fibers have many technical defects. Their resistance is highly sensitive to deformation, and signal drift easily occurs under dynamic deformation, severely affecting the working accuracy of wearable devices and sensors, resulting in poor dynamic conductivity stability. Furthermore, it is difficult to balance mechanical and conductivity properties; some materials have acceptable tensile strength but poor conductivity, while others meet conductivity standards but lack mechanical toughness and have a narrow stretching range, failing to meet the practical application requirements of flexible electronics. Moreover, the preparation of these fibers often employs complex processes such as template methods and multi-step encapsulation, making continuous and large-scale production difficult. The resulting fibers also suffer from insufficient self-healing ability and poor durability. In addition, it is difficult to achieve uniform microphase structure control in one-dimensional fiber structures, which not only restricts ion transport paths but also makes conductive pathways prone to breakage during stretching, further exacerbating the material's conductivity instability.

[0004] To address the signal drift problem under dynamic deformation of ion-conductive materials, current technological research focuses on fluid-free strain-insensitive conductive materials. For thin-film materials, strategies such as ridge structure construction and interface confinement have been developed, significantly improving conductivity stability. Meanwhile, fibrous conductive materials, due to their excellent mechanical flexibility, stress dispersion capabilities, and seamless integration into breathable textiles, have become a preferred direction in flexible electronics. Existing technologies have proposed various innovative solutions based on fiber structure design to mitigate resistance changes under deformation. The specific implementation paths are as follows: Microfluidic spinning to construct fibers with special structures: Conductive fibers with helical core structures are prepared by coaxial microfluidic spinning process. The special geometry of the fibers disperses tensile stress and reduces the damage of deformation to the internal conductive path, thereby reducing the magnitude of resistance change. However, the preparation process and technology of this route are complex, the core structure is prone to desorption during recycling, and the structural stability is not good. Polymerization-induced phase separation design of bicontinuous structure: Based on polymerization-induced phase separation technology, a solid-liquid bicontinuous structure is constructed inside the fiber. Phase separation optimizes the spatial distribution of the mechanical support phase and the ionic conductive phase, improving the conductivity stability during fiber deformation. However, the conductivity of the fiber prepared by this route will decrease significantly after multiple uses, and the long-term stability is insufficient. Channel adhesion and macro-corrugated structure modification: Adhesive channel strategy is used to enhance the stability of ion transport path inside the fiber, or macro-corrugated structure is constructed to use the elastic deformation of the structure to offset tensile stress and minimize resistance change under strain; however, adhesion or introduction of macro-structure is prone to defects such as insufficient interfacial bonding strength and local stress concentration, making it difficult to solve the signal stability problem under dynamic deformation from the root. Summary of the Invention

[0005] The purpose of this invention is to provide a hierarchical microphase separation strain-enhanced ion-conductive elastomer fiber, its preparation method and application. The ion-conductive elastomer fiber has excellent mechanical properties, electrical conductivity, strain insensitivity, and self-healing ability, and its preparation method is simple and can be carried out in continuous production.

[0006] The objective of this invention can be achieved through the following technical solutions: One objective of this invention is to provide a hierarchical microphase separation strain-enhanced ion-conductive elastomer fiber, which has a dual continuous network structure, including interpenetrating EOEOEA / PAA continuous phase and PEA / LiTFSI continuous phase.

[0007] Preferably, the ion-conductive elastomer fiber is a copolymer P(PEA- co -EOEOEA) forms the structural framework, in which the EOEOEA segments and PAA form the EOEOEA / PAA continuous phase based on hydrogen bonding, and the PEA segments and LiTFSI form the PEA / LiTFSI continuous phase based on strong coordination. The EOEOEA / PAA continuous phase serves as the mechanically reinforcing phase, and the PEA / LiTFSI continuous phase serves as the ion transport phase.

[0008] In this invention, PEA refers to 2-phenoxyethyl acrylate, and EOEOEA refers to 2-(2-ethoxyethoxy)ethyl acrylate.

[0009] More preferably, the copolymer P(PEA- co The structural formula of -EOEOEA is as follows: Where n ranges from 400 to 500, and m ranges from 100 to 125.

[0010] More preferably, the strong coordination effect refers to: on the one hand, Li in LiTFSI + Li forms a strong coordination bond with the ester group oxygen atom on the PEA segment through lithium bonds; on the other hand, Li + With TFSI - Stable ion coordination is formed between them, and the dual coordination synergistically confines LiTFSI to the PEA chain segment.

[0011] Preferably, the ion-conductive elastomer fiber has a diameter of 1.8~2.2 mm, a length of 10~120 cm, and an aspect ratio of 500:1~600:1.

[0012] More preferably, the diameter of the ion-conductive elastomer fiber is 2 mm.

[0013] Preferably, the ion-conductive elastomer fiber has a non-porous, dense structure.

[0014] The second objective of this invention is to provide a method for preparing the aforementioned hierarchical microphase separation strain-reinforced ion-conductive elastomer fiber, comprising the following steps: S1: Preparation of prepolymer solution: PEA (2-phenoxyethyl acrylate), EOEOEA (2-(2-ethoxyethoxy)ethyl acrylate) and photoinitiator A are mixed and stirred until dissolved, and then polymerized by ultraviolet light to obtain the prepolymer solution; S2: Reactive wet spinning: The prepolymer solution from step S1 is injected into a syringe. The prepolymer solution is extruded into a deionized water coagulation bath and photopolymerized by ultraviolet light irradiation to obtain P(PEA- co -EOEOEA) copolymer fibers; S3: First swelling: Prepare an aqueous solution of AA / photoinitiator B as the first swelling solution, and then apply the P(PEA-) obtained in step S2 to the solution. co -EOEOEA) copolymer fibers are immersed in the first swelling solution for light-protected swelling. After swelling, the fibers are removed and dried, and then subjected to ultraviolet light irradiation to cause AA (acrylic acid) to polymerize in situ on the fiber surface, yielding P(PEA- co -EOEOEA) composite fiber; S4: Second swelling: Prepare a LiTFSI (lithium bis(trifluoromethanesulfonyl)imide) / EA (ethyl acetate) solution as the second swelling solution, and then apply the P(PEA-) obtained in step S3 to the solution. co The ion-conductive elastomer fiber (-EOEOEA) composite fiber is immersed in the second swelling solution and swelled in the dark. After swelling is completed, the fiber is removed and dried to obtain the ion-conductive elastomer fiber.

[0015] Preferably, in step S1, the molar ratio of PEA to EOEOEA is 8:2 - 6:4.

[0016] More preferably, in step S1, the molar ratio of PEA to EOEOEA is 8:2.

[0017] Preferably, in step S1, the photoinitiator A is DMPA (2,2-dimethoxy-2-phenylacetophenone).

[0018] Preferably, in step S1, the mass of the photoinitiator accounts for 0.8 to 1.2 wt% of the sum of the masses of PEA and EOEOEA.

[0019] More preferably, in step S1, the mass of the photoinitiator accounts for 1.0 wt% of the sum of the masses of PEA and EOEOEA.

[0020] Preferably, in step S1, the process conditions for ultraviolet light-initiated polymerization are: irradiation with an ultraviolet light source with a wavelength of 365 nm for 10-15 seconds.

[0021] More preferably, in step S1, the process conditions for ultraviolet light-initiated polymerization are: irradiation with an ultraviolet light source with a wavelength of 365 nm for 12 seconds.

[0022] Preferably, in step S2, the extrusion flow rate of the prepolymer liquid is 4~6 mL / h.

[0023] More preferably, in step S2, the extrusion flow rate of the prepolymer liquid is 5 mL / h.

[0024] More preferably, in step S2, the syringe uses a 22G needle.

[0025] More preferably, in step S2, the 22G needle has a diameter of 0.9 mm, a length of 25 mm, and a maximum theoretical liquid extrusion flow rate of 31 mL / min.

[0026] Preferably, in step S2, the ultraviolet light irradiation-induced photopolymerization is carried out by irradiating with an ultraviolet light source with a wavelength of 365 nm for 30 to 60 seconds.

[0027] More preferably, in step S2, the ultraviolet light irradiation-induced photopolymerization is carried out by irradiating with an ultraviolet light source with a wavelength of 365 nm for 45 seconds.

[0028] More preferably, in step S2, the P(PEA- co The EOEOEA copolymer fiber has a diameter of 1.0 mm and is transparent.

[0029] Preferably, in step S3, the concentration of AA in the first swelling solution is 9.8 ~ 10.2 mol / L.

[0030] More preferably, in step S3, the concentration of AA in the first swelling solution is 10 mol / L.

[0031] Preferably, in step S3, the photoinitiator B is AKG (α-ketoglutarate).

[0032] Preferably, in step S3, the mass of the photoinitiator B is 0.4 to 0.6% of the mass of AA.

[0033] More preferably, in step S3, the mass of the photoinitiator B is 0.5% of the mass of AA.

[0034] Preferably, in step S3, the light-protected swelling time is 12 to 24 hours, and the first swelling solution is replaced every 2 to 4 hours during the swelling period.

[0035] More preferably, in step S3, the light-protected swelling time is 18 hours, and the first swelling solution is replaced every 3 hours during the swelling period.

[0036] Preferably, in step S3, the drying process is as follows: take out the fiber, absorb the surface solution with filter paper, and vacuum dry it for 15-20 minutes at 20~30℃ and -0.10~-0.12 MPa.

[0037] More preferably, in step S3, the drying process is as follows: take out the fiber, absorb the surface solution with filter paper, and vacuum dry at 25 °C and -0.10 MPa for 15 minutes.

[0038] Preferably, in step S3, the light source used for ultraviolet irradiation is an ultraviolet light source with a wavelength of 365 nm, and the irradiation time is 50~70 seconds.

[0039] More preferably, in step S3, the light source used for ultraviolet irradiation is an ultraviolet light source with a wavelength of 365 nm, and the irradiation time is 60 seconds.

[0040] Preferably, in step S3, the P(PEA- co The tensile toughness of the -EOEOEA composite fiber is not less than 8.0 MJ / m. 3 .

[0041] Preferably, in step S4, the concentration of LiTFSI in the second swelling solution is 0.08~0.12 g / mL, and the light-protected swelling time is 20~28 hours.

[0042] More preferably, in step S4, the concentration of LiTFSI in the second swelling solution is 0.10 g / mL, and the light-protected swelling time is 24 hours.

[0043] Preferably, in step S4, the drying process is as follows: take out the fiber and vacuum dry it at 20~30 ℃ and -0.10~-0.12 MPa for 12~24 hours.

[0044] More preferably, in step S4, the drying process is as follows: the fiber is taken out and vacuum dried at 25 °C and -0.10 MPa for 24 hours.

[0045] More preferably, the preparation method of the hierarchical microphase separation strain-reinforced ion-conductive elastomer fiber includes the following steps: S1: Preparation of prepolymer solution: Under light-protected conditions, PEA and EOEOEA were mixed at a molar ratio of 8:2; DMPA photoinitiator, accounting for 1.0 wt% of the total monomer mass, was added and stirred to dissolve; the mixture was irradiated with an ultraviolet light source with a wavelength of 365 nm for 12 seconds to obtain a viscous prepolymer solution. S2: Reactive wet spinning: The prepolymer solution is loaded into a syringe and extruded into a deionized water coagulation bath at a flow rate of 5 mL / h through a 22G needle; during extrusion, the fine stream is continuously irradiated with 365 nm ultraviolet light for 45 seconds to ensure complete polymerization, yielding transparent P(PEA- co -EOEOEA) copolymer fibers, with a diameter of approximately 1.0 mm; S3: First swelling enhancement: Prepare a 10 mol / L aqueous solution of AA and add 0.5 wt% (by weight of AA) of photoinitiator AKG; immerse the fiber obtained in step S2 in this solution and swell in the dark for 18 hours, changing the solution every 3 hours. Remove the fiber, blot the surface solution with filter paper, and vacuum dry at 25 ℃ and -0.1 MPa for 15 minutes; then irradiate with ultraviolet light for 60 seconds to cause the infiltrated AA to polymerize in situ, forming P(PEA- co -EOEOEA) / PAA composite fiber; S4: Second swelling and conductivity: Prepare a LiTFSI / EA solution with a concentration of 0.10 g / mL; immerse the composite fiber obtained in step S3 in this solution and soak it in the dark for 24 hours. After removal, vacuum dry it at 25 ℃ and -0.1 MPa for 24 hours to completely remove the solvent, and obtain the final ion-conductive elastomer fiber (labeled ICEF-1).

[0046] The third objective of this invention is to provide an application of the aforementioned hierarchical microphase separation strain-enhanced ion-conductive elastomer fiber in wearable electronic devices and soft robots.

[0047] Preferably, the ion-conductive elastomer fibers are woven into a mesh electrode, and the mesh electrode is assembled with an acrylic elastic dielectric layer to obtain a single-electrode mode triboelectric nanogenerator.

[0048] Preferably, the single-electrode mode triboelectric nanogenerator includes a mesh electrode based on ion-conductive elastomer fiber weaving, and both sides of the mesh electrode are provided with an acrylic elastic dielectric layer.

[0049] More preferably, an aluminum foil for reducing external electromagnetic interference to the device is also disposed between one side surface of the mesh electrode and the acrylic elastic dielectric layer.

[0050] More preferably, the weaving process is a plain weave weave.

[0051] More preferably, the weaving density is 50×30 threads / 10cm.

[0052] More preferably, the acrylic elastic dielectric layer has dimensions of 1.5 cm × 2 cm and a thickness of 90 μm.

[0053] More preferably, the mesh electrode has a size of 1 cm × 1.5 cm and a thickness of 3.6~4 mm.

[0054] More preferably, the aluminum foil has a size of 1 cm × 1.7 cm and a thickness of 500 μm.

[0055] More preferably, the mesh electrode and the acrylic elastic dielectric layer are assembled by adhesion.

[0056] More preferably, the single-electrode mode triboelectric nanogenerator can be used for material identification sensing.

[0057] More preferably, the single-electrode mode triboelectric nanogenerator can be used for material identification of skin, wood, nitrile rubber, glass, stainless steel, and rabbit fur.

[0058] More preferably, when the single-electrode mode triboelectric nanogenerator comes into contact with the above-mentioned material, it can generate different open-circuit voltage signals, thereby realizing material identification sensing.

[0059] To address the shortcomings of existing ion-conductive fibers, such as significant resistance changes and severe signal drift under dynamic deformation, difficulty in simultaneously achieving mechanical and conductive properties, complex fabrication processes, and insufficient self-healing capabilities, this invention provides a hierarchical microphase separation strain-reinforced ion-conductive elastomer fiber, its preparation method, and its applications. This invention utilizes hierarchical microphase separation engineering and a dual swelling process to construct a dual-continuous network structure (microphase separation structure) with PEOEOEA segments (soft segments) / PAA as the mechanical reinforcement phase and PEA segments (hard segments) / LiTFSI as the ion transport phase. This achieves synergistic optimization of mechanical and conductive properties, resulting in an ion-conductive elastomer fiber possessing ultra-high tensile strength, toughness, rapid self-healing, and strain-insensitive ion conductivity. Simultaneously, it enables simple and continuous fabrication of this fiber, solving the technical problems of difficult control of one-dimensional fiber microstructure and easy breakage of conductive pathways under dynamic deformation.

[0060] The principle of microphase separation structure formation of the ion-conductive elastomer fiber of the present invention is as follows: Firstly, copolymer P(PEA- co Using EOEOEA as the matrix, microphase separation occurs due to the incompatibility between PEA segments (hydrophobic) and EOEOEA segments (hydrophilic), forming a bicontinuous initial structural framework in which hydrophilic EOEOEA segment microregions (EOEOEA segments have flexible aliphatic long chains, serving as soft microregions) and hydrophobic PEA segment microregions (PEA segments contain rigid benzene ring structures, serving as hard microregions) interpenetrate each other. This provides a clear spatial partitioning basis for the selective construction of subsequent functional phases, laying the groundwork for the precise division of labor between mechanical enhancement and ion transport functions.

[0061] The first step, aqueous phase swelling, achieves mechanically reinforcing phase construction: P(PEA- co P(PEA-EOEOEA) copolymer fibers are immersed in an aqueous solution of amino acids (AA) for light-protected swelling. Due to the difference in chain segment polarity, AA monomers selectively accumulate in and swell the hydrophilic EOEOEA chain microregions. Following in-situ polymerization initiated by ultraviolet light, the resulting PAA molecular chains are tightly anchored to the EOEOEA chains through hydrogen bonding, forming a cross-linked, entangled polar network within the hydrophilic EOEOEA microregions. This results in a continuous PAA reinforcing phase that permeates the entire fiber. This PAA network within the hydrophilic microregions provides the fiber with excellent tensile toughness and structural stability. This step constructs P(PEA- co -EOEOEA) / PAA composite fiber.

[0062] The second step involves oil phase swelling to construct the ion transport phase: P(PEA- coWhen the LiTFSI (-EOEOEA) / PAA composite fiber is immersed in an oily organic solvent system (EA) containing LiTFSI, the hydrophobic PEA segments swell and open channels under the action of the organic solvent, and LiTFSI is selectively distributed along the micro-regions of the PEA segments; among which Li + With the ester oxygen atom on the PEA chain segment, TFSI - Anions form strong coordination interactions and are stably confined within the hydrophobic microregions composed of PEA segments, forming a continuous ion transport pathway within these hydrophobic microregions.

[0063] Since the PAA phase is firmly bonded to the EOEOEA segments through hydrogen bonds and is confined to the hydrophilic microregions in a polar environment, it mainly undertakes the mechanical reinforcement function; while the ion transport function is undertaken by the PEA / LiTFSI phase in the hydrophobic microregions. Ultimately, a dual continuous network structure is formed inside the fiber, in which the hydrophilic microregion mechanical reinforcement phase and the hydrophobic microregion ion transport phase are separate and functionally synergistic. This ensures that the fiber still has stable ionic conductivity under large strain at the microstructural level, while achieving a synergistic improvement in mechanical and electrical properties.

[0064] Under tensile strain, rigid PEA / Li + The enriched conductive microregions are gradually arranged along the stretching direction, thereby reducing the tortuosity of the ion transport path; at the same time, the hydrogen-bonded soft microregions do not disrupt the lithium coordination environment when subjected to mechanical deformation. This synergistic structural evolution mechanism enables efficient ion transport even under large deformation conditions and provides a structural basis for the strain-enhanced ion conductivity observed in the ion-conductive elastomer fibers of this invention.

[0065] Compared with the prior art, the present invention has the following beneficial effects: (1) This invention provides a hierarchical microphase separation strain-enhanced ion-conductive elastomer fiber, which forms a double continuous network structure by interpenetrating the EOEOEA / PAA continuous phase and the PEA / LiTFSI continuous phase. This ion-conductive elastomer fiber has excellent mechanical properties, electrical properties, strain insensitivity, self-healing ability, and is simple to prepare and can be produced continuously.

[0066] (2) This invention constructs a dual continuous network structure with EOEOEA chain segments (soft segments) / PAA as the mechanical reinforcement phase and PEA chain segments (hard segments) / LiTFSI as the ion transport phase by combining multi-level microphase separation engineering with dual swelling process. This solves the technical problem of limited ion transport path and easy breakage of conductive path during stretching in one-dimensional fiber structure. It enables conductive elastomer fiber to have both 834% ultra-high tensile strength and 0.019 S / m excellent ion conductivity, breaking through the bottleneck of mutual restriction between mechanical and conductive properties of traditional materials. Moreover, the fiber axial structure uniformity error is ≤5%.

[0067] (3) The ion-conductive elastomer fiber of the present invention also has unique strain insensitivity characteristics. The absolute value of the relative resistance change is ≤0.1 in the strain range of 0-800%, and the resistance decreases by only 0.11% under the maximum strain. It can effectively avoid signal drift in dynamic deformation and meet the precise signal transmission requirements of dynamic scenarios such as wearable devices. At the same time, relying on the dynamic non-covalent bond effect of hydrogen bond, lithium bond and other bonds, the fiber has a self-repair efficiency of 89% within 48h and a tensile toughness retention rate of ≥90% after repair, which greatly improves durability.

[0068] (4) The preparation method of the ion-conductive elastomer fiber of the present invention adopts the integrated process of reactive wet spinning and double swelling, without the need for complex steps such as pre-stretching. It can continuously prepare fibers with a length ≥120 cm and a diameter fluctuation ≤±10%, which has the potential for industrial promotion. The product has excellent mechanical adaptability, stable conductivity, self-healing ability and easy weaving integration characteristics. It has a wide and irreplaceable application prospect in flexible electronics fields such as high-fidelity signal transmission, wearable health monitoring, and soft robots.

[0069] (5) The present invention constructs a dual continuous network structure in situ through hierarchical microphase separation combined with a dual swelling process. The preparation process is simple and easy to control, and does not require complex spinning equipment and macroscopic structural modification. The internal mechanical reinforcement phase and ion transport phase are stably combined through hydrogen bonding and strong coordination, respectively, without problems such as structural desorption and insufficient interfacial bonding strength. At the same time, the hierarchical microphase separation structure can uniformly disperse tensile stress and avoid local stress concentration. In addition, LiTFSI is stably confined around the PEA chain segment to form a continuous and reliable ion transport pathway. The conductivity of the fiber does not decrease significantly after multiple cycles of service. It has both excellent structural stability and long-term conductivity stability under dynamic deformation. Attached Figure Description

[0070] Figure 1 The image shows the physical specimen of the ion-conductive elastomer fiber prepared in Example 1. Figure 2 This is a schematic diagram illustrating the preparation process and principle of the ion-conductive elastomer fiber of the present invention. Figure 2 In the diagram, 'a' represents the preparation process of steps S1-S2. Figure 2 In the diagram, b is a schematic diagram of the preparation principle of steps S1-S2; Figure 2 (C is a schematic diagram of the preparation principle of steps S3-S4). Figure 3 The image shows the AFM (atomic force microscopy) characterization of the ion-conductive elastomer fibers prepared in Example 1. Figure 3 a- Figure 3 c is P(PEA-) co -EOEOEA) copolymer fiber, P(PEA- coMorphology of EOEOEA) / PAA composite fiber and ion-conductive elastomer fiber ICEF-1. Figure 3 d- Figure 3 f is P(PEA-) in sequence co -EOEOEA) copolymer fiber, P(PEA- co Phase diagram of (EOEOEA) / PAA composite fiber and ion-conductive elastomer fiber ICEF-1). Figure 4 P(PEA-) was obtained from different monomer mass ratios in Examples 1-3 and Comparative Examples 4-7. co Stress-strain curve of EOEOEA copolymer fiber; Figure 5 The tensile toughness comparison diagrams are shown for the ion-conductive elastomer fibers in Examples 1-3 and Comparative Examples 1-4. Figure 6 This is a comparison of the relative resistance variation curves of the ion-conductive elastomer fibers in Examples 1-3 and Comparative Examples 1-4. Figure 7 This is a comparison of the relative conductivity curves of the ion-conductive elastomer fibers in Examples 1-3 and Comparative Examples 1-4. Figure 8 The ion-conductive elastomer fiber prepared in Example 1 and P(PEA- co Comparison of toughness and self-healing efficiency of -EOEOEA) copolymer fibers; Figure 9 The conductivity recovery curves of the ion-conductive elastomer fibers obtained in Example 1 at different healing times are shown. Figure 10 The curves showing the relative resistance and relative conductivity of the ion-conductive elastomer fiber obtained in Example 1 after 48 hours of self-healing under different strains are shown. Figure 11 The curves showing the relative resistance changes of the ion-conductive elastomer fiber obtained in Example 1 under different stretching cycles are shown. Figure 12 The output voltage waveforms of the ion-conductive elastomer fiber obtained in Example 1 when transmitting AC signals of different frequencies under constant strain are shown. Figure 13 The output voltage waveforms of the ion-conductive elastomer fiber obtained in Example 1 under different tensile strains are shown. Figure 14 Photographs showing the changes in LED brightness during the stretching process, powered by ion-conductive elastomer fiber (ICEF) obtained in Example 1 and ion-conductive elastomer fiber (ICEF (Blend)) obtained in Comparative Example 3 as conductors. Figure 15The open-circuit voltage output of the TENG device (single-electrode mode triboelectric nanogenerator) obtained in the application example when it is in contact with different materials; Figure 16 The open-circuit voltage output of the TENG device obtained in the application example when it is periodically in contact with nitrile rubber at different frequencies; Figure 17 The graph shows the stability of the output voltage of the TENG device obtained in the application example under contact separation cycle. Detailed Implementation

[0071] The present invention will now be described in detail with reference to the accompanying drawings and specific embodiments. These embodiments are based on the technical solution of the present invention and provide detailed implementation methods and specific operating procedures. However, the scope of protection of the present invention is not limited to the following embodiments.

[0072] A hierarchical microphase-separated strain-reinforced ion-conducting elastomer fiber has an internal double continuous network structure, including interpenetrating EOEOEA / PAA continuous phases and PEA / LiTFSI continuous phases. Specifically, the ion-conducting elastomer fiber is based on copolymer P(PEA- co The EOEOEA fiber forms the structural framework, with EOEOEA segments bonded to PAA via hydrogen bonding to form an EOEOEA / PAA continuous phase, and PEA segments bonded to LiTFSI via strong coordination to form a PEA / LiTFSI continuous phase. The EOEOEA / PAA continuous phase serves as the mechanical reinforcement phase, while the PEA / LiTFSI continuous phase serves as the ion transport phase. The diameter of this ion-conductive elastomer fiber is 1.8~2.2 mm, the length is 100~120 cm, and the aspect ratio is 500:1~600:1.

[0073] The method for preparing ion-conductive elastomer fibers, such as Figure 2 As shown, the specific steps include: S1: Preparation of prepolymer solution: PEA, EOEOEA, and photoinitiator A are mixed and stirred until dissolved, and then subjected to UV-initiated polymerization to obtain a prepolymer solution; wherein, the molar ratio of PEA to EOEOEA is 8:2-6:4, the photoinitiator A is DMPA, and the mass of the photoinitiator accounts for 0.8~1.2wt% of the sum of the masses of PEA and EOEOEA; the process conditions for UV-initiated polymerization are: irradiation with a UV light source with a wavelength of 365 nm for 10~15 seconds.

[0074] S2: Reactive wet spinning: The prepolymer solution from step S1 is injected into a syringe. The prepolymer solution is extruded into a deionized water coagulation bath and photopolymerized by ultraviolet light irradiation to obtain P(PEA- co-EOEOEA) copolymer fiber; wherein the extrusion flow rate of the prepolymer liquid is 4~6 mL / h, and the ultraviolet light irradiation-induced photopolymerization is carried out by irradiation with an ultraviolet light source with a wavelength of 365 nm for 30~60 seconds.

[0075] S3: First swelling: Prepare an aqueous solution of AA / photoinitiator B as the first swelling solution, and then apply the P(PEA-) obtained in step S2 to the solution. co -EOEOEA) copolymer fibers are immersed in the first swelling solution for light-protected swelling. After swelling, the fibers are removed and dried, and then subjected to ultraviolet light irradiation to cause AA to polymerize in situ on the fiber surface, yielding P(PEA- co -EOEOEA) / PAA composite fiber; wherein, the concentration of AA in the first swelling solution is 9.8~10.2 mol / L, the photoinitiator B is AKG, and the mass of the photoinitiator B is 0.4~0.6% of the mass of AA; the light-protected swelling time is 12~24 hours, and the first swelling solution is replaced every 2~4 hours during the swelling period; the drying process is as follows: take out the fiber, absorb the surface solution with filter paper, and vacuum dry at 20~30 ℃ and -0.10~-0.12 MPa for 15~20 minutes; the light source used for ultraviolet irradiation is an ultraviolet light source with a wavelength of 365 nm, and the irradiation time is 50~70 seconds.

[0076] S4: Second swelling: Prepare a LiTFSI / EA solution as the second swelling solution, and apply the P(PEA-) obtained in step S3 to the solution. co The -EOEOEA) / PAA composite fiber is immersed in a second swelling solution and swells in the dark. After swelling, the fiber is removed and dried to obtain the ion-conductive elastomer fiber. The concentration of LiTFSI in the second swelling solution is 0.08~0.12 g / mL, and the swelling time in the dark is 20~28 hours. The drying process is as follows: the fiber is removed and vacuum dried at 20~30 ℃ and -0.10~-0.12 MPa for 12~24 hours.

[0077] Unless otherwise specified, the reagents, methods, instruments, and equipment used in this invention are conventional in the art. Unless otherwise specified, the reagents and materials used in the following examples are all commercially available.

[0078] The reagents used in each example are described below: 2-Phenoxyethyl acrylate (PEA, >98%), 2-(2-ethoxyethoxy)ethyl acrylate (EOEOEA, >95%) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI, >99%): Shanghai Aladdin Biochemical Technology Co., Ltd. Acrylic acid (AA, AR, >99%), ethyl acetate (EA, AR, >99.5%) and α-ketoglutaric acid (AKG, >98%): Shanghai Ammas Reagent Co., Ltd. 2,2-Dimethoxy-2-phenylacetophenone (DMPA, 99%): Shanghai Maclean Biochemical Technology Co., Ltd.

[0079] Acrylic elastic dielectric layer: Shanghai Yixin tape is made of PET polyester film, acrylic resin and other materials. It has a dielectric constant of 3.5-3.8, an elongation of 50%, is transparent, has an adhesion of 1200 g / 25 mm, a tensile strength of 120 N / 25 mm, and a temperature resistance of 200℃.

[0080] Unified Specifications for Performance Testing Methods: Tensile properties: Tested using a universal testing machine according to ASTM D638 standard at a tensile rate of 50 mm / min. Strain (ε) is expressed as a percentage, and toughness is calculated by integrating the stress-strain curve.

[0081] Ionic conductivity (σ): The volumetric conductivity is calculated by measuring the volumetric conductivity using an electrochemical impedance spectroscopy method through a two-electrode system.

[0082] Strain insensitivity: Resistance (R) is measured simultaneously during the stretching process, with the relative resistance change ∆ as the metric. R / R 0=( R - R 0) / R 0 represents, where R 0 represents the initial resistance at zero strain.

[0083] Self-healing efficiency: The fiber was completely cut, the cut surfaces were brought into contact and left to stand at room temperature for 48 hours. The tensile strength (or breaking energy) before and after repair was tested respectively. Efficiency = (performance after repair / original performance) × 100%.

[0084] Example 1 This embodiment provides a method for preparing strain-reinforced ion-conductive elastomer fibers, the method comprising: Prepolymer preparation: Under light-protected conditions, PEA and EOEOEA were mixed at a molar ratio of 8:2. 1.0 wt% of photoinitiator DMPA was added and stirred until dissolved. The mixture was irradiated with a 365 nm UV light source for 12 seconds to obtain a viscous prepolymer.

[0085] Wet spinning: The prepolymer solution is loaded into a syringe and extruded into a deionized water coagulation bath at a flow rate of 5 mL / h through a 22G needle. During extrusion, the stream is continuously irradiated with 365 nm ultraviolet light for 45 seconds to ensure complete polymerization, yielding transparent P(PEA-) co -EOEOEA) copolymer fiber, with a diameter of approximately 1.0 mm.

[0086] First swelling enhancement: Prepare a 10 mol / L aqueous solution of AA and add 0.5 wt% (by weight of AA) of photoinitiator AKG. Immerse the fibers obtained in step 2 in this solution and allow them to swell in the dark for 18 hours, changing the solution every 3 hours. Remove the fibers, blot the surface solution with filter paper, and vacuum dry at 25°C and -0.1 MPa for 15 minutes. Then irradiate with ultraviolet light for 60 seconds to induce in-situ polymerization of the infiltrated AA, forming P(PEA- co -EOEOEA) / PAA composite fiber.

[0087] Second swelling and conductivity: Prepare a LiTFSI / EA solution with a concentration of 0.10 g / mL. Immerse the composite fiber obtained in step 3 in this solution and soak it in the dark for 24 hours. After removal, vacuum dry it at 25℃ and -0.1 MPa for 24 hours to completely remove the solvent, obtaining the final ion-conductive elastomer fiber (labeled ICEF-1).

[0088] Figure 1 The image shown is of the sample prepared in Example 1, demonstrating the successful preparation of the fiber structure.

[0089] The microstructure of the ion-conductive elastomer fiber sample prepared in Example 1 was characterized. Figure 3 AFM characterization images of this ion-conductive elastomer fiber at different preparation stages. Figure 3 a- Figure 3 In the middle, c represents the morphological diagram. Figure 3 d- Figure 3 f is the phase diagram; from left to right, they are P(PEA- co -EOEOEA) copolymer matrix, P(PEA- co -EOEOEA) / PAA composite fiber, P(PEA- co -EOEOEA) / PAA / LiTFSI ion-conductive elastomer fibers. As shown in the figure, P(PEA- co After the EOEOEA copolymer fiber was swelled in the first aqueous phase to introduce PAA, the phase separation was significantly enhanced, and the mechanically reinforcing phase was constructed. After the LiTFSI was swelled in the second oil phase to introduce LiTFSI, a bicontinuous phase structure was formed. This proves that the present invention successfully constructed a bicontinuous network in which the mechanically reinforcing phase and ion transport are interpenetrated through hierarchical microphase separation and double swelling process.

[0090] Example 2-3 Example 2 (PEA:EOEOEA=7:3) Except for adjusting the monomer molar ratio to 7:3 in step 1, the remaining steps and parameters are exactly the same as in Example 1. The resulting fiber is labeled ICEF-2.

[0091] Example 3 (PEA:EOEOEA=6:4) Except for adjusting the monomer molar ratio to 6:4 in step 1, the remaining steps and parameters are exactly the same as in Example 1. The resulting fiber is labeled ICEF-3.

[0092] Comparative Example 1 (physical blending, no microphase separation) Solution preparation: PEA, EOEOEA, AA, and LiTFSI are mixed in a single batch at a mass ratio (calculated) similar to the final product of Example 1. DMPA and AKG are added and dissolved in an appropriate amount of EA. The mixture is stirred to form a homogeneous solution.

[0093] Spinning and curing: The above mixed solution was injected into a deionized water coagulation bath using a syringe pump, and then irradiated with strong ultraviolet light for a long time in the bath and immediately after removal, in an attempt to make all monomers polymerize simultaneously and rapidly.

[0094] Drying: The resulting fibers were dried under vacuum. The resulting fibers were labeled D-1.

[0095] Compared with Example 1, Comparative Example 1 uses physical blending instead of microphase separation engineering to prepare ion-conductive elastomer fibers. The results show that physical blending cannot achieve selective distribution of the EOEOEA / PAA continuous phase and the PEA / LiTFSI continuous phase, and cannot form a double continuous network structure. The mechanical properties and ion conductivity of the resulting fibers are comprehensively degraded.

[0096] Comparative Example 2 (single swelling, enhancement only) The difference between Comparative Example 2 and Example 1 is that step 4 is omitted, and the second swelling and conductivity treatment with LiTFSI / EA solution is not performed. The remaining steps and parameters are the same, and the resulting fiber is labeled as D-2.

[0097] Compared with Example 1, Comparative Example 2 only performed the first swelling step and did not perform the second swelling step to prepare ion-conductive elastomer fibers. The results showed that constructing only the EOEOEA / PAA mechanical reinforcing phase could not form an effective ion-conductive network. The resulting fibers only had certain mechanical properties, but the ion-conductive properties were significantly lacking, and the synergistic optimization of mechanical and conductive properties could not be achieved.

[0098] Comparative Example 3 (single swelling, only electrical conductivity) The difference between Comparative Example 3 and Example 1 is that step 3 is omitted and AA swelling reinforcement treatment is not performed. The remaining steps and parameters are the same, and the resulting fiber is marked as D-3.

[0099] Compared with Example 1, this comparative example only performed a second swelling step and did not perform the first swelling step to prepare ion-conductive elastomer fibers. The results showed that by constructing only the PEA / LiTFSI ion-conductive phase and not constructing the EOEOEA / PAA mechanical reinforcing phase, the mechanical properties of the resulting fibers, especially the toughness, were significantly reduced. In addition, the LiTFSI was unevenly distributed inside the fibers, and it was impossible to achieve a synergistic improvement in mechanical properties and ion-conductive properties.

[0100] Comparative Example 4 (Microphase Separation Ratio Imbalance) Except for adjusting the monomer molar ratio to 2:8 (PEA:EOEOEA) in step 1, the remaining steps and parameters are exactly the same as in Example 1. The resulting fibers are labeled D-4.

[0101] When the monomer ratio exceeds the design range of this invention, the microphase separation structure is not ideal, and a double continuous network structure cannot be formed. The mechanical properties and ionic conductivity of the resulting fibers are significantly reduced.

[0102] Comparative Example 5 (PEA:EOEOEA=5:5) Except for adjusting the monomer molar ratio to 5:5 in step 1, the remaining steps and parameters are exactly the same as in Example 1. The resulting fibers are labeled D-5.

[0103] At this ratio, the electrical performance decreases significantly.

[0104] Comparative Example 6 (PEA:EOEOEA=4:6) Except for adjusting the monomer molar ratio to 4:6 in step 1, the remaining steps and parameters are exactly the same as in Example 1. The resulting fibers are labeled D-6.

[0105] At this ratio, the mechanical properties decrease significantly.

[0106] Comparative Example 7 (PEA:EOEOEA=3:7) Except for adjusting the monomer molar ratio to 3:7 in step 1, the remaining steps and parameters are exactly the same as in Example 1. The resulting fibers are labeled D-7.

[0107] At this ratio, the mechanical properties decrease significantly.

[0108] Figure 4 P(PEA-) was obtained from different monomer mass ratios in Examples 1-3 and Comparative Examples 4-7. co Stress-strain curves of EOEOEA copolymer fibers. Figure 5 , Figure 6 , Figure 7 The charts presented are, in order, a comparison of the tensile toughness, relative resistance variation curves, and relative conductivity curves of the ion-conductive elastomer fibers in Examples 1-3 and Comparative Examples 1-4. (Summary) Figures 4-7It can be seen that the ion-conductive elastomer fiber (ICEF-1) obtained in Example 1 achieves the best balance of comprehensive performance when the ratio of PEA to EOEOEA monomers is 8:2. The tensile properties (ultra-high tensile strength of 834%, fiber fracture strain can reach more than 1200%) and strain insensitivity (absolute value of relative resistance change ≤0.1 in the strain range of 0-800%, and resistance decreases by only 0.11% at maximum strain) are all the best, achieving an excellent balance between excellent mechanical properties and excellent performance. Figure 7 In the medium strain, the relative conductivity change σ / σ0 = (strain + 1)^2 / (R / R0). Under medium and low strain, σ / σ0 is relatively small, and as the strain increases, σ / σ0 gradually increases.

[0109] Figure 8 This is a comparison of the toughness and self-healing efficiency of the ion-conductive elastomer fiber prepared in Example 1 and the P(PEA-co-EOEOEA) copolymer fiber. As shown in the figure, P(EOEOEA- co The P(PEA) copolymer itself possesses self-healing properties; after 48 hours of healing, the stress-strain ratio recovered from 1223% (0.73 MPa) to 1092% (0.65 MPa). ICEF-1, after two swelling cycles, retained this property, recovering its stress-strain ratio from 834% (1.9 MPa) to 682% (1.56 MPa) after 48 hours of healing. The self-healing efficiency is calculated as the ratio of the values ​​before and after self-healing. This is because P(PEA- co The EOEOEA unit in PEA contains a long ethoxy chain, and these ether oxygen atoms are excellent hydrogen bond acceptors. Furthermore, if the PEA moiety contains carbonyl oxygen, it also acts as a hydrogen bond acceptor. The hydrogen bonds have moderate bond energies and can be broken and reformed relatively easily at room temperature or slightly higher temperatures. When the material fractures, the exposed ether oxygen atoms and potential ester carbonyl oxygen atoms on the fracture surface can reform hydrogen bonds with polar groups on the opposite fracture surface. This continuous breaking and rebuilding of the hydrogen bond network is one of the key driving forces for achieving self-healing. The two swelling processes not only do not destroy the self-healing properties, but may even construct this property in a new dimension, indicating that the material can still maintain structural integrity after repair. The large number of carboxyl groups introduced by the first swelling and formed in situ photopolymerization in PAA, along with P(PEA- co The ether oxygen on the -EOEOEA) chain forms strong hydrogen bonds, which greatly enriches the hydrogen bond formation capability in the polymer network. The introduction of secondary swelling LiTFSI forms dynamic ionic clusters and physical cross-linking points. Due to the retention of ion migration and chain segment movement, the self-healing capability formed by the recombination of ionic coordination bonds is maintained.

[0110] Figure 9The conductivity recovery curves of the ion-conductive elastomer fiber obtained in Example 1 at different healing times are shown. The results show that after 48 hours of self-healing, the fiber conductivity can be restored to near the original level, confirming that the self-healing process can also effectively restore the electrical function of ICEF, providing support for the long-term service stability of the material.

[0111] Figure 10 The figures show the relative resistance and relative conductivity changes of the ion-conductive elastomer fiber obtained in Example 1 after 48 hours of self-healing under different strains. As can be seen from the figures, the self-healed fiber still maintains excellent strain-insensitive ion-conductive properties, and its electrical performance is stable under large strain conditions with no obvious signal drift.

[0112] Figure 11 The curves showing the relative resistance changes of the ion-conductive elastomer fiber obtained in Example 1 under different stretching cycles demonstrate that it still maintains stable signal transmission function after 2000 stretching cycles. Figure 12 and Figure 13 The figures show the output voltage waveforms of the ion-conductive elastomer fiber obtained in Example 1 when transmitting AC signals of different frequencies under constant strain and the output voltage waveforms under different tensile strains, respectively. The results demonstrate that the ion-conductive elastomer fiber, as a conductor, can stably transmit AC voltages of different frequencies, and the signal does not drift under high tensile strain. Furthermore, when connected in series with an LED bulb, it was found that the bulb brightness remained essentially unchanged during stretching, further demonstrating the strain-insensitive characteristics of ICEF-1. Figure 14 ).

[0113] Application examples This application example provides a single-electrode mode triboelectric nanogenerator (TENG device). The specific fabrication process is as follows: Using an acrylic elastomer as the bottom substrate, a mesh electrode (using a plain weave process; weave density of 50×30 fibers / 10cm) constructed by ion-conducting elastomer fibers (ICEF-1) prepared in Example 1 is tightly stacked on the acrylic elastomer. Then, an aluminum foil is attached to the surface of the mesh electrode as a single electrode layer. Finally, another layer of acrylic elastomer is covered on the aluminum foil electrode. By assembling the layers in a tight bonding manner, the single-electrode mode triboelectric nanogenerator is obtained.

[0114] In this application example, the acrylic elastic dielectric layer has dimensions of 1.5 cm × 2 cm and a thickness of 500 μm, the mesh electrode has dimensions of 1 cm × 1.5 cm, and the aluminum foil has dimensions of 1 cm × 1.7 cm and a thickness of 500 μm.

[0115] The TENG device obtained in the application examples exhibits excellent sensing and recognition performance and long-term service stability: the device can generate differentiated electrical signal responses when in contact with objects of six different materials. Figure 15 This enables precise material identification and sensing; after 2000 contact-separation cycles, the device's output voltage shows no significant attenuation, and its output performance remains highly stable throughout the cycle. Figure 17 ).

[0116] Figure 16 The open-circuit voltage output of the TENG device under periodic contact with nitrile rubber at different frequencies was measured. The results show that the device has stable output performance in the 1-3Hz frequency range, which can meet the application requirements of mechanical energy harvesting and self-powered sensing devices. Simultaneously, the fiber can stably transmit AC signals without distortion or attenuation under 0-500% tensile strain, and the signal fidelity remains unchanged at different transmission frequencies (0.5-5Hz). This meets the stable transmission requirements of physiological signals in wearable health monitoring devices, fully verifying the excellent strain-insensitive conductivity and practical application potential of the fiber of this invention.

[0117] The test results of the above embodiments and comparative examples are summarized as follows: Table 1: Comparison of the overall performance of fibers from the examples and comparative examples .

[0118] In summary, the ion-conductive elastomer fiber (ICEF-1) obtained in Example 1 achieves the best overall performance balance when the ratio of PEA to EOEOEA monomers is 8:2, exhibiting optimal tensile properties and ionic conductivity. Furthermore, it gradually forms a hierarchical microphase separation structure during the subsequent two swelling processes. When the monomer ratio deviates from this optimal value (e.g., decreasing to 6:4 or becoming unbalanced to 2:8), the fiber's tensile toughness and conductive stability both decline. At a monomer ratio of 2:8, the microphase separation structure is severely damaged, and the decrease in conductivity is particularly significant, fully demonstrating the necessity of limiting the monomer ratio range in this invention. Combining the experimental results of Comparative Example 1 (physical blend), Comparative Example 2 (reinforcement only, no conductivity), and Comparative Example 3 (conductivity only, no reinforcement), it is evident that D-1 (physical blend) is significantly inferior to ICEF-1 in all performance indicators, especially in conductivity, strain insensitivity, and self-healing properties. This indicates that simple physical mixing cannot construct the "reinforcement-conductivity" dual network proposed in this invention, highlighting the core value of microphase separation engineering. While D-2 (reinforced only) possesses excellent tensile strength and toughness, its electrical conductivity is extremely low, failing to meet the practical application requirements of conductive materials. D-3 (conductive only) not only has significantly lower conductivity than this invention, but its mechanical properties and self-healing properties are also poor. The above comparisons fully demonstrate that the "reinforced first, conductive later" dual swelling sequential process of this invention is a necessary condition for simultaneously achieving excellent mechanical properties and a stable, high-conductivity ion pathway.

[0119] The ICEF-1 obtained in Example 1 exhibits a resistance change rate of only 0.22% under a huge strain of 500%, which can effectively avoid signal drift during dynamic wear and meet the actual application requirements of wearable devices. It also maintains stable signal transmission function after 2000 stretching cycles. In contrast, the fibers obtained in Comparative Examples 1, 3, and 4 all have a resistance change rate exceeding 6.5% under the same strain conditions, which can easily lead to signal distortion and cannot meet the usage requirements of dynamic wearable scenarios.

[0120] The above description of the embodiments is provided to enable those skilled in the art to understand and use the invention. It will be apparent to those skilled in the art that various modifications can be made to these embodiments, and the general principles described herein can be applied to other embodiments without inventive effort. Therefore, the present invention is not limited to the above embodiments, and any improvements and modifications made by those skilled in the art based on the disclosure of the present invention without departing from the scope of the invention should be within the protection scope of the present invention.

Claims

1. A hierarchical microphase separation strain-reinforced ion-conductive elastomer fiber, characterized in that, It has a dual continuous network structure, including the interpenetrating EOEOEA / PAA continuous phase and the PEA / LiTFSI continuous phase.

2. The hierarchical microphase separation strain-reinforced ion-conductive elastomer fiber according to claim 1, characterized in that, The ion-conductive elastomer fiber is a copolymer P(PEA- co -EOEOEA) forms the structural framework, in which the EOEOEA segments and PAA form the EOEOEA / PAA continuous phase based on hydrogen bonding, and the PEA segments and LiTFSI form the PEA / LiTFSI continuous phase based on strong coordination. The EOEOEA / PAA continuous phase serves as the mechanically reinforcing phase, and the PEA / LiTFSI continuous phase serves as the ion transport phase.

3. The hierarchical microphase separation strain-reinforced ion-conductive elastomer fiber according to claim 1, characterized in that, The ion-conductive elastomer fiber has a diameter of 1.8~2.2 mm, a length of 100~120 cm, and an aspect ratio of 500:1~600:

1.

4. A method for preparing a hierarchical microphase separation strain-reinforced ion-conductive elastomer fiber as described in any one of claims 1 to 3, characterized in that, Includes the following steps: S1: Prepolymer preparation: PEA, EOEOEA and photoinitiator A are mixed and stirred until dissolved, and then polymerized by ultraviolet light to obtain the prepolymer; S2: Reactive wet spinning: The prepolymer solution from step S1 is injected into a syringe. The prepolymer solution is extruded into a deionized water coagulation bath and photopolymerized by ultraviolet light irradiation to obtain P(PEA- co -EOEOEA) copolymer fibers; S3: First swelling: Prepare an aqueous solution of AA / photoinitiator B as the first swelling solution, and then apply the P(PEA-) obtained in step S2 to the solution. co -EOEOEA) copolymer fibers are immersed in the first swelling solution for light-protected swelling. After swelling, the fibers are removed and dried, and then subjected to ultraviolet light irradiation to cause AA to polymerize in situ on the fiber surface, yielding P(PEA- co -EOEOEA) composite fiber; S4: Second swelling: Prepare a LiTFSI / EA solution as the second swelling solution, and apply the P(PEA-) obtained in step S3 to the solution. co The ion-conductive elastomer fiber (-EOEOEA) composite fiber is immersed in the second swelling solution and swelled in the dark. After swelling is completed, the fiber is removed and dried to obtain the ion-conductive elastomer fiber.

5. The method for preparing hierarchical microphase separation strain-reinforced ion-conductive elastomer fibers according to claim 4, characterized in that, In step S1, the molar ratio of PEA to EOEOEA is 8:2-6:4, the photoinitiator A is DMPA, and the mass of the photoinitiator accounts for 0.8-1.2 wt% of the sum of the masses of PEA and EOEOEA; the process conditions for ultraviolet light-initiated polymerization are: irradiation with an ultraviolet light source with a wavelength of 365 nm for 10-15 seconds.

6. The method for preparing hierarchical microphase separation strain-reinforced ion-conductive elastomer fibers according to claim 4, characterized in that, In step S2, the extrusion flow rate of the prepolymer liquid is 4~6 mL / h, and the photopolymerization initiated by ultraviolet light irradiation uses an ultraviolet light source with a wavelength of 365 nm for 30~60 seconds.

7. The method for preparing hierarchical microphase separation strain-reinforced ion-conductive elastomer fibers according to claim 4, characterized in that, In step S3, the concentration of AA in the first swelling solution is 9.8~10.2 mol / L, the photoinitiator B is AKG, and the mass of the photoinitiator B is 0.4~0.6% of the mass of AA; the light-protected swelling time is 12~24 hours, and the first swelling solution is replaced every 2~4 hours during the swelling period; the drying process is as follows: take out the fiber, absorb the surface solution with filter paper, and vacuum dry at 20~30 ℃ and -0.10~-0.12 MPa for 15~20 minutes; the light source used for ultraviolet irradiation is an ultraviolet light source with a wavelength of 365 nm, and the irradiation time is 50~70 seconds.

8. The method for preparing hierarchical microphase separation strain-reinforced ion-conductive elastomer fibers according to claim 4, characterized in that, In step S4, the concentration of LiTFSI in the second swelling solution is 0.08~0.12 g / mL, and the light-protected swelling time is 20~28 hours; the drying process is as follows: take out the fiber and vacuum dry it at 20~30 ℃ and -0.10 ~ -0.12 MPa for 12~24 hours.

9. The application of a hierarchical microphase separation strain-enhanced ion-conductive elastomer fiber as described in any one of claims 1 to 3 in wearable electronic devices and soft robots.

10. The application according to claim 9, characterized in that, The ion-conductive elastomer fibers are woven into a mesh electrode, which is then assembled with an acrylic elastic dielectric layer to obtain a single-electrode mode triboelectric nanogenerator.

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