Fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker mediated plasticity and preparation method and application thereof

Abstract

The invention provides a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker mediated plasticity and a preparation method thereof, and belongs to the field of transistor materials. According to the preparation method, firstly, the surface hydrophilicity and charge distribution of a fiber base material are improved by adopting a plasma sputtering technology, then two-dimensional layered structure MXene is compounded on the fiber surface to form a compact and continuous thin film, and organic semiconductor polymer monomers are uniformly adsorbed by utilizing the large specific surface area and rich functional groups of the thin film; inducing an in-situ polymerization reaction to obtain the artificial nerve fiber with a porous nano structure. Then, the fiber loaded with the biological recognition molecules on the artificial nerve fiber serves as a transistor grid electrode, the artificial nerve fiber serves as a transistor source drain electrode, and the assembled fiber-based synapse transistor is low in working voltage; 0.5 V), fast response speed (3s), high transconductance, low energy consumption (0.10 fJ / peak) and excellent synaptic plasticity.

Description

Technical Field

[0001] The present invention relates to the technical field of transistor materials, and in particular to a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity, and a preparation method and application thereof. Background Art

[0002] With the gradual development of wearable applications of smart fabrics, the preparation of fiber-based organic electrochemical transistors has gradually attracted widespread attention. However, when the conductive fibers prepared by existing technologies are applied to synaptic transistors, there is a problem of poor synaptic plasticity, so fiber-based synaptic transistors are still relatively rare.

[0003] Existing transistor synaptic devices can be divided into two types: thin-film transistors and fiber-based transistor synaptic devices. Thin-film transistor synaptic devices have poor structural biomimetic properties, poor mechanical stability, poor common fit and comfort. Fiber-based transistor synaptic devices can be divided into the following three categories: the first category is nanofiber membranes / wires. Although this type performs well in terms of energy consumption, it has poor mechanical fit with the substrate and is difficult to integrate over a large area. The second category is synaptic transistors integrated on a single fiber. This type often uses ferroelectric materials, so the operating voltage is too high. The third category is synaptic devices with dendritic network structures. This type successfully simulates the morphology of neural networks, but compared with the energy consumption of biological synapses, the energy consumption at the pj level is too high.

[0004] The patent with publication number CN114481603 B provides a polyester / boron nitride / polypyrrole composite conductive fiber and a fiber-based neurosynaptic transistor device. The neurosynaptic transistor includes a source, drain and gate arranged crosswise, and a gel electrolyte arranged between the intersections. The source, drain and gate use PET / BN / PPy composite conductive fibers, which are first impregnated with BN on the surface of polyester, and then pyrrole is polymerized and grown in situ on its surface to obtain a three-dimensional mesh and linear structure of conductive polymer composite fiber flexible electrode material. The fiber-based neurosynaptic transistor device has the advantages of softness, good biocompatibility and diversified integration methods. The high conductivity of the PET / BN / PPy channel material helps to improve the sensing performance of the device, but the energy consumption of the transistor device also increases, reaching 0.85pj / spike, which is far from the energy consumption of human brain synapses (1-10fJ / spike). In addition, the biochemical substances are unknown to mediate the plasticity of the neurosynaptic transistor. In summary, it is difficult for this device to achieve the coordinated optimization of high sensing performance and low energy consumption and has never achieved biochemical-mediated plasticity.

[0005] In view of this, it is necessary to design a fiber-based synaptic transistor with ultra-low energy consumption and fluid physiological marker-mediated plasticity, as well as its preparation method and application, to solve the above problems. Summary of the invention

[0006] In view of the technical problems existing in the background technology, the present application provides a fiber-based synaptic transistor with ultra-low energy consumption and plasticity mediated by body fluid physiological markers, and its preparation method and application. The preparation method first uses plasma sputtering technology to improve the hydrophilicity and charge distribution on the surface of the fiber substrate, and then composites the two-dimensional layered structure MXene on the fiber surface to form a dense and continuous film, and utilizes its large specific surface area and rich functional groups to uniformly adsorb organic semiconductor polymer monomers, inducing in situ polymerization reaction to obtain artificial nerve fibers with a porous nanostructure.

[0007] The artificial nerve fiber has a large volume capacitance and a short energy dissipation path. The fiber-based synaptic transistor assembled with the artificial nerve fiber as the source and drain of the transistor and the fiber carrying the biorecognition molecule on the artificial nerve fiber as the gate of the transistor has a low operating voltage (<0.5V), a fast response speed (3s), a high transconductance, a low energy consumption (0.10fJ / spike), and excellent synaptic plasticity.

[0008] This fiber-based synaptic transistor can be used in low-energy consumption, high-biochemical-mediated plasticity artificial synapses, brain-computer interfaces, sensory nerves and smart electronic fabrics.

[0009] In a first aspect, the present application provides a method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity, comprising the following steps:

[0010] S1, plasma etching the fiber substrate under nitrogen / hydrogen mixed gas conditions, the etching time is 3-30 minutes;

[0011] S2, fully immersing the fiber substrate obtained in step S1 in the MXene suspension for 6-8 hours, taking it out and drying it in a vacuum oven at 10-60° C.; repeating the above immersion and drying steps 2-6 times;

[0012] S3, placing the MXene composite fiber substrate obtained in step S2 in a conductive polymer monomer solution, and then preparing an artificial nerve fiber having a porous nano-needle, linear and mesh composite structure through a low-temperature in-situ polymerization reaction after infiltration;

[0013] S4, loading the biorecognition molecule onto the artificial nerve fiber obtained in step S3 to obtain a gate artificial nerve fiber;

[0014] S5, using the artificial nerve fiber obtained in step S3 as the source and drain of the transistor, and applying silver paste on both ends; dripping electrolyte at the middle position, waiting for it to dry slightly, and then dripping another drop, repeating this 2-3 times to build up to a certain height to form a gel electrolyte; placing the gate artificial nerve fiber obtained in step S4 on the gel electrolyte in a cross shape, and at the same time dripping another drop of gel electrolyte, also waiting for it to dry slightly, and then dripping another drop after it is slightly dried, so as to obtain a fiber-based synaptic transistor with ultra-low energy consumption and plasticity mediated by body fluid physiological markers.

[0015] In some embodiments, in step S2, the concentration of the MXene suspension is 0.1 to 12 mg / ml.

[0016] In some embodiments, in step S3, the low-temperature in-situ polymerization takes 12 to 72 hours.

[0017] In some embodiments, the MXene is Ti3C2T x 、Mo2CT x 、Mo2TiC2T x 、Cr2TiC2T x One or more of the above, the layer thickness is 1 to 10 nm.

[0018] In some embodiments, in step S4, the method of loading the biorecognition molecule onto the artificial nerve fiber is one or more of physical adsorption, chemical coupling, bioaffinity, physical embedding, and self-assembly technology.

[0019] In some embodiments, the conductive polymer is one of polyaniline, polypyrrole, polythiophene, poly-3-hexylthiophene, poly-3-cyclohexylthiophene, thiophenepyrrolopyrroledione, and polyethylene oxide; the fiber substrate is one or more of cotton, wool, silk, nylon, polyester, acrylic, vinylon, polypropylene, viscose, carbon fiber, and aramid fiber.

[0020] In some embodiments, the gel electrolyte is one of an ionic liquid gel electrolyte and a biomass gel electrolyte.

[0021] In the second aspect, an embodiment of the present application provides a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity, wherein the fiber-based synaptic transistor is composed of a source-drain artificial nerve fiber, a gate artificial nerve fiber, and an electrolyte; the source-drain artificial nerve fiber includes a fiber substrate, a conductive polymer and MXene loaded on the fiber substrate; the gate artificial nerve fiber includes a fiber substrate, a conductive polymer loaded on the fiber substrate, MXene, and a biorecognition molecule.

[0022] In some embodiments, the fiber-based synaptic transistor operates at a voltage of less than 0.5 V, has a transconductance of 7.0 mS, and has an energy consumption as low as 0.10 fJ / spike.

[0023] The fiber-based synaptic transistor is used in the fields of low-energy consumption, high-body fluid physiological marker material-mediated plasticity artificial synapses, brain-computer interfaces, sensory nerves, and intelligent electronic fabrics.

[0024] Compared with the prior art, the present invention has the following beneficial effects:

[0025] (1) The present application provides a method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity. First, the fiber substrate is plasma etched under nitrogen / hydrogen mixed gas conditions to enhance the fiber's affinity for negatively charged MXene. Then, a two-dimensional layered structure MXene is composited on the fiber surface to form a dense and continuous film. The large specific surface area and rich functional groups of the MXene are utilized to uniformly adsorb organic semiconductor polymer monomers, thereby inducing an in situ polymerization reaction to obtain an artificial nerve fiber with a porous nanostructure.

[0026] (2) The artificial nerve fiber has a large volume capacitance and a short energy dissipation path. The fiber-based synaptic transistor assembled with the artificial nerve fiber as the source and drain of the transistor and the fiber loaded with biorecognition molecules on the artificial nerve fiber as the gate of the transistor has a low operating voltage (<0.5V), a fast response speed (3s), a high transconductance, an energy consumption as low as 0.10fJ / spike, and excellent synaptic plasticity.

[0027] (3) The fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity provided in this application successfully achieved selective and concentration-dependent synaptic behavior in both PBS and artificial urine environments, and had a significant memory effect, providing the possibility for the combination of artificial neuromorphic devices and biological sensory neural networks.

[0028] The above description is only an overview of the technical solution of the present application. In order to more clearly understand the technical means of the present application, it can be implemented in accordance with the contents of the specification. In order to make the above and other purposes, features and advantages of the present application more obvious and easy to understand, the specific implementation methods of the present application are listed below. BRIEF DESCRIPTION OF THE DRAWINGS

[0029] In order to more clearly illustrate the technical solution of the present application, the following is a brief introduction to the drawings used in the present application. Obviously, the drawings described below are only some embodiments of the present application, and for ordinary technicians in this field, other drawings can be obtained based on these drawings without creative work.

[0030] Figure 1This is a microscopic electron microscope image of the unmodified FPA6 fiber substrate in Example 1.

[0031] Figure 2 This is a microscopic electron microscope image of FPA6 / MXene / PANI fiber after plasma sputtering technology in Example 1.

[0032] Figure 3 The energy consumption of the fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity prepared in Example 1 under non-proton ionic liquid gel electrolyte and proton gel electrolyte respectively.

[0033] Figure 4 This is the excitatory postsynaptic current of the fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity prepared in Example 1 using proton gel electrolyte.

[0034] Figure 5 This is the EPSC of the fiber-based synaptic transistor with ultra-low energy consumption and humoral physiological markers mediated plasticity prepared in Example 1 under different UA concentrations.

[0035] Figure 6 The mediated plasticity of the fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological markers mediated plasticity prepared in Example 1 under different UA concentrations and interfering substances.

[0036] Figure 7 This is the electron microscope image of FPA6 / PANI fiber in comparative example 1. DETAILED DESCRIPTION

[0037] The following embodiments of the technical solution of the present application are described in detail in conjunction with the accompanying drawings. The following embodiments are only used to more clearly illustrate the technical solution of the present application, and are therefore only used as examples, and cannot be used to limit the scope of protection of the present application.

[0038] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by technicians in the technical field to which this application belongs; the terms used herein are only for the purpose of describing specific embodiments and are not intended to limit this application; the terms "including" and "having" in the specification and claims of this application and the above-mentioned figure descriptions and any variations thereof are intended to cover non-exclusive inclusions.

[0039] In the description of the embodiments of the present application, the technical terms "first", "second", etc. are only used to distinguish different objects, and cannot be understood as indicating or implying relative importance or implicitly indicating the number, specific order or primary and secondary relationship of the indicated technical features. In the description of the embodiments of the present application, the meaning of "multiple" is more than two, unless otherwise clearly and specifically defined.

[0040] Reference to "embodiments" herein means that a particular feature, structure, or characteristic described in conjunction with the embodiments may be included in at least one embodiment of the present application. The appearance of the phrase in various locations in the specification does not necessarily refer to the same embodiment, nor is it an independent or alternative embodiment that is mutually exclusive with other embodiments. It is explicitly and implicitly understood by those skilled in the art that the embodiments described herein may be combined with other embodiments.

[0041] In the description of the embodiments of the present application, the term "and / or" is only a description of the association relationship of the associated objects, indicating that there may be three relationships. For example, A and / or B can represent: A exists alone, A and B exist at the same time, and B exists alone. In addition, the character " / " in this article generally indicates that the associated objects before and after are in an "or" relationship.

[0042] In the description of the embodiments of the present application, the term "multiple" refers to more than two (including two). Similarly, "multiple groups" refers to more than two groups (including two groups), and "multiple pieces" refers to more than two pieces (including two pieces).

[0043] In the description of the embodiments of the present application, unless otherwise clearly specified and limited, technical terms such as "installed", "connected", "connected", "fixed" and the like should be understood in a broad sense. For example, it can be a fixed connection, a detachable connection, or an integral connection; it can be a mechanical connection or an electrical connection; it can be a direct connection or an indirect connection through an intermediate medium, and it can be the internal connection of two elements or the interaction relationship between two elements. For those of ordinary skill in the art, the specific meanings of the above terms in the embodiments of the present application can be understood according to the specific circumstances.

[0044] In order to realize low operating voltage of transistors while having low energy consumption, the present application embodiment provides a method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity, comprising the following steps:

[0045] S1, plasma etching the fiber substrate under nitrogen / hydrogen mixed gas conditions, the etching time is 3-30 minutes;

[0046] Among them, the fiber base material is one or more of cotton, wool, silk, nylon, polyester, acrylic, vinylon, polypropylene, viscose fiber, carbon fiber, and aramid fiber.

[0047] S2, fully immersing the fiber substrate obtained in step S1 in the MXene suspension for 6-8 hours, taking it out and drying it in a vacuum oven at 10-60° C.; repeating the above immersion and drying steps 2-6 times;

[0048] Among them, the concentration of MXene suspension is 0.1~12 mg / ml.

[0049] MXene is Ti3C2T x 、Mo2CT x 、Mo2TiC2T x 、Cr2TiC2T x One or more of the above, the layer thickness is 1 to 10 nm.

[0050] S3, placing the MXene composite fiber substrate obtained in step S2 in a conductive polymer monomer solution, and then preparing an artificial nerve fiber having a porous nano-needle, linear and mesh composite structure through a low-temperature in-situ polymerization reaction after infiltration;

[0051] The purity of the conductive high molecular polymer monomer is 99-100%.

[0052] The conductive polymer is one of polyaniline, polypyrrole, polythiophene, poly-3-hexylthiophene, poly-3-cyclohexylthiophene, thiophene diketopyrrolopyrrole, and polyethylene oxide;

[0053] The low-temperature in-situ polymerization process is as follows: add the conductive monomer to the acid solution, then immerse the MXene composite fiber substrate in the acid solution and stir; then dissolve ammonium persulfate ((NH4)2S2O8) in an equal volume of acid solution and drop it into the mixed solution. After polymerizing the conductive polymer at low temperature for 12 to 72 hours, wash the unattached conductive polymer and vacuum dry it at 25 to 60°C to obtain the source-drain artificial nerve fiber.

[0054] S4, loading the biorecognition molecule onto the artificial nerve fiber obtained in step S3 to obtain a gate artificial nerve fiber;

[0055] Specifically, the method of loading the biorecognition molecules onto the artificial nerve fibers is one or more of physical adsorption, chemical coupling, bioaffinity, physical embedding, and self-assembly technology.

[0056] The biorecognition molecules are one or more of glucose oxidase, uricase, lactate oxidase, acetylcholinesterase, lactate oxidase, horseradish peroxidase, metal nanoparticles, carbon nanotubes, rhodium single-atom nanozymes, magnetic Fe3O4 nanoparticles and graphene; the method of loading the biorecognition molecules is one or more of physical adsorption, chemical coupling, bioaffinity, physical embedding and self-assembly technology.

[0057] S5, using the artificial nerve fiber obtained in step S3 as the source and drain of the transistor, and applying silver paste on both ends; dripping electrolyte at the middle position, waiting for it to dry slightly, and then dripping another drop, repeating this process 2-3 times to form a gel electrolyte of a certain height; placing the gate artificial nerve fiber obtained in step S4 on the gel electrolyte in a cross shape, and dripping another drop of gel electrolyte at the same time, also waiting for it to dry slightly, and then dripping another drop after it is dried slightly, thereby obtaining a fiber-based synaptic transistor with ultra-low energy consumption and plasticity mediated by body fluid physiological markers.

[0058] The gel electrolyte is one of an ionic liquid gel electrolyte and a biomass gel electrolyte.

[0059] Ionic liquid gel electrolytes are composed of polymers, ionic liquids, and solvents.

[0060] The polymer is one or more of polyvinylidene fluoride (PVDF), poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), polyethylene oxide (PEO), polyvinylidene fluoride-hexafluoropropylene copolymer (P(VDF-TrFE)), polyvinyl alcohol (PVA), polyacrylonitrile (PAN), polyacrylamide (PAM), and polymethyl methacrylate (PMMA).

[0061] The ionic liquid is one or more of [DEME][BF4], [EMI][TFSA], [BMIM][PF6], [EIM][TFSI], [EMIM][TFSI], [LITFSI], [NaTFSI], and [KTFSI].

[0062] The solvent is one or more of acetone, ethanol, methanol, isopropanol, dimethyl carbonate, diethyl carbonate, ethylene glycol, and propylene glycol.

[0063] The biomass gel electrolyte is one or more of gelatin, alginate, starch, agar, cellulose, chitosan and the like.

[0064] The preparation method of the present application first uses plasma sputtering technology to improve the hydrophilicity and charge distribution of the fiber substrate surface, and then composites the two-dimensional layered structure MXene on the fiber surface to form a dense and continuous film, and uses its large specific surface area and rich functional groups to uniformly adsorb organic semiconductor polymer monomers, inducing in-situ polymerization to obtain artificial nerve fibers with porous nanostructures. The obtained artificial nerve fibers have large volume capacitance and short energy dissipation paths.

[0065] Then, the fiber loaded with biorecognition molecules on the artificial nerve fiber is used as the transistor gate, and the artificial nerve fiber is used as the transistor source and drain. The assembled fiber-based synaptic transistor has low operating voltage (<0.5V), fast response speed (3s), high transconductance, low energy consumption (0.10fJ / spike), and excellent synaptic plasticity.

[0066] In the second aspect, the embodiment of the present application provides a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity, which is prepared by the above-mentioned preparation method. The fiber-based synaptic transistor is composed of a source-drain artificial nerve fiber, a gate artificial nerve fiber, and an electrolyte; the source-drain artificial nerve fiber includes a fiber substrate, a conductive polymer loaded on the fiber substrate, and MXene; the gate artificial nerve fiber includes a fiber substrate, a conductive polymer loaded on the fiber substrate, MXene, and a biorecognition molecule.

[0067] The fiber-based synaptic transistor operates at less than 0.5V, has a transconductance of 7.0mS, and has an energy consumption as low as 0.10fJ / spike.

[0068] The fiber-based synaptic transistor can be used in the fields of low-energy consumption, high biochemical-mediated plasticity artificial synapses, brain-computer interfaces, sensory nerves, and smart electronic fabrics.

[0069] Some specific embodiments are listed below. It should be noted that the embodiments described below are exemplary and are only used to explain the present application, and should not be construed as limiting the present application. If specific techniques or conditions are not specified in the embodiments, the techniques or conditions described in the literature in this area or the product specifications are used. The reagents or instruments used without specifying the manufacturer are all conventional products that can be obtained commercially.

[0070] 1. Preparation method

[0071] Example 1

[0072] This embodiment provides a method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity, comprising the following steps:

[0073] S1, plasma etching the fiber substrate PA6 in a low-pressure cylindrical plasma reactor under nitrogen / hydrogen mixed gas conditions (volume ratio of 85% N2 / 15% H2) for 30 min to obtain functional PA6 (FPA6);

[0074] S2, fully immerse the FPA6 obtained in step S1 in 1 mg / mL Ti3C2T x The suspension was immersed in the solution for 8 h at a temperature of 4 °C. After being taken out, it was dried in a vacuum oven at 40 °C to obtain FPA6 / Ti3C2Tx Fiber; repeat the above soaking and drying steps 6 times;

[0075] S3, 1.14 mL of aniline monomer was added to 25 mL of 1 mol / L perchloric acid solution, and then the FPA6 / Ti3C2T x The fiber was immersed in the acid solution and stirred for 10 minutes; then 0.728g of ammonium persulfate ((NH4)2S2O8) was dissolved in an equal volume (25mL) of the acid solution and added dropwise to the mixed solution. Polyaniline was polymerized at 0°C for 48h, and the unattached polyaniline was washed and vacuum dried at 40°C to obtain PANI / MXene / PA6 fiber. The scanning electron microscope image is shown in FIG. Figure 2 shown.

[0076] Figure 1 In the figure, from left to right are the electron microscope images of the unmodified FPA6 fiber substrate, plasma functionalized PA6 (FPA6), and FPA6 / MXene electrode. It can be seen that the surface of the unmodified FPA6 fiber substrate is smooth and the active sites on the fiber surface are limited; the fiber surface of the plasma functionalized PA6 (FPA6) becomes rough; after MXene (Ti3C2T x ) after modification, the fiber surface is loaded with a large amount of Ti3C2T x , Ti3C2T x The large number of hydrophilic functional groups on the surface and their intercalated structures provide abundant sites for the attachment of aniline monomers. Compared with the smooth FPA6 surface, the surface of the FPA6 / MXene / PANI fiber composited with the two-dimensional layered MXene has nanoneedles, nanowires or nanonet structures (such as Figure 2 shown).

[0077] S4, soaking the PANI / MXene / PA6 fiber obtained in step S3 in a PBS solution containing urate oxidase (UOx) for 2 hours and then drying at 4°C, repeating twice to obtain a FPA6 / MXene / PANI / UOx gate fiber electrode;

[0078] S5, using the PANI / MXene / PA6 fiber obtained in step S3 as the transistor source and drain, applying silver paste on both ends; dripping electrolyte in the middle position, waiting for it to dry slightly, and then dripping another drop, repeating this three times to form a gel electrolyte of a certain height; placing the FPA6 / MXene / PANI / UOx gate fiber electrode obtained in step S4 on the gel electrolyte in a cross shape, and dripping another drop of gel electrolyte at the same time, waiting for it to dry slightly, and then dripping another drop of gel electrolyte to dry slightly, and then obtaining a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity. Wherein, the gel electrolyte is a gel electrolyte composed of polyvinyl alcohol (PVA): phosphoric acid (H3PO4): deionized water (DI) = 1:1:10.

[0079] Figure 3 The energy consumption of the fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity obtained in Example 1 in non-protonic ionic liquid gel electrolyte (volume ratio of PVA: phosphoric acid: water = 1: 1: 10) and proton gel electrolyte (mass ratio of polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP): 1-ethyl-3-methylimidazolium bistrifluoromethanesulfonyl imide salt (EMIM: TFSI): acetone = 1: 4: 7) respectively. It can be seen that the corresponding energy consumption in the non-protonic ionic liquid gel electrolyte (left figure) and the proton gel electrolyte (right figure) are 0.10fJ / spike and 1.21fJ / spike, respectively, which are much lower than 0.85pj / spike in the prior art.

[0080] Figure 4 The excitatory postsynaptic current (EPSC) of the fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity obtained in Example 1 under the use of proton gel electrolyte. When a negative pulse stimulus is applied to the gate of the device, the source-drain current of the device increases immediately, and gradually returns to the initial state after the stimulus is removed, forming EPSC. When the pulse intensity is gradually increased, EPSCs are significantly enhanced.

[0081] Figure 5 The EPSC of the fiber-based synaptic transistor with ultra-low energy consumption and humoral physiological markers mediated plasticity obtained in Example 1 at different UA concentrations.

[0082] Experiments show that when a constant negative gate pulse is applied to the device, the electrons generated by the UA oxidation reaction will be pushed to the PANI postsynaptic channel, thereby increasing the conductance. The current change (I / I0) with increasing UA concentration on the nanomolar and micromolar scales shows that different UA concentrations can sensitively mediate postsynaptic channel currents, and EPSC is significantly enhanced with increasing UA concentration.

[0083] Figure 6The fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological markers mediated plasticity obtained in Example 1 mediated plasticity under different UA concentrations and interfering substances.

[0084] Biologically, pain is sensitized by repeated stimulation due to cumulative changes in synaptic weight. To simulate this process, continuous negative gate pulses were applied to the nerve fiber-based OECT, and the current change was slightly enhanced under periodic negative pulses due to the doping of anions driven by the negative pulses in the channel. Then it returned to its initial state after the pulse was removed. No significant memory effect was found. When UA was present, a significant current enhancement occurred due to the doping of additional anions in the UA redox products. Long-term current retention was observed after 5 consecutive identical pulses, indicating that UA permanently regulates synaptic weight. High concentrations of interferons such as glucose, DA, and AA were also introduced to study their biological specificity. The current change of 10μM interferon was much smaller than that of 1nM UA, that is, the current change caused by high concentrations of interferons such as glucose, DA, and AA on the device was much smaller than the current change caused by low concentrations of UA on the device. Synaptic plasticity can only be selectively regulated by UA, indicating that the device has the potential to selectively convert biochemical signals into brain-like synaptic signals in a complex environment.

[0085] Comparative Example 1

[0086] Comparative Example 1 provides a method for preparing a fiber-based synaptic transistor. Compared with Example 1, the difference is that step S2 is not performed, that is, the two-dimensional layered structure MXene is not compounded on the fiber substrate. The rest is basically the same as Example 1 and will not be repeated here.

[0087] The experiment shows that a large number of PANI particles agglomerated and unevenly distributed appear on the surface of the fiber substrate, such as Figure 7 shown.

[0088] Comparative Example 2

[0089] Comparative Example 2 provides a method for preparing a fiber-based synaptic transistor. Compared with Example 1, the difference is that step S1 is not performed, that is, the fiber substrate is not plasma etched. The rest is roughly the same as Example 1 and will not be repeated here.

[0090] The test results are as follows: the fiber substrate was not plasma etched, resulting in uneven distribution of MXene sheets on PA6.

[0091] Examples 2-4 and Comparative Examples 3-5

[0092] Examples 2-4 and Comparative Examples 3-5 provide a method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity. Compared with Example 1, the difference is that the etching time in step S1 and the concentration of the MXene suspension in step S2 are changed, as shown in the following table. The rest is roughly the same as Example 1 and will not be repeated here.

[0093] Etching time (min) Concentration of MXene suspension (mg / ml) Example 1 30 1 Example 2 30 0.1 Example 3 3 12 Example 4 15 10 Comparative Example 3 30 0.2 Comparative Example 4 1 12 Comparative Example 5 40 0.1

[0094] Experiments show that when the concentration of the MXene suspension is lower than 0.1 mg / ml, it is difficult to form a continuous MXene composite film with uniform performance on the fiber surface.

[0095] When the etching time is 1 min, the functional group grafting efficiency is low and MXene is difficult to load evenly on the fiber electrode surface. When the etching time is 40 min, the fiber strength is significantly reduced.

[0096] Experiments show that MXene can also be Mo2CT x 、Mo2TiC2T x 、Cr2TiC2T x The conductive polymer may also be one of polypyrrole, polythiophene, poly-3-hexylthiophene, poly-3-cyclohexylthiophene, thiophene diketopyrrolopyrrole, and polyethylene oxide.

[0097] The fiber substrate can also be one or more of cotton, wool, silk, polyester, acrylic, vinylon, polypropylene, viscose fiber, carbon fiber, and aramid fiber.

[0098] It should be noted that the present application is not limited to the above-mentioned embodiments. The above-mentioned embodiments are only examples, and the embodiments having the same structure as the technical idea and exerting the same effect within the scope of the technical solution of the present application are all included in the technical scope of the present application. In addition, without departing from the scope of the main purpose of the present application, various modifications that can be thought of by those skilled in the art to the embodiments and other methods of combining some of the constituent elements in the embodiments are also included in the scope of the present application.

Claims

1. A method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity, characterized in that: The following steps are involved: S1, plasma etching the fiber substrate under nitrogen / hydrogen mixed gas conditions, the etching time is 3-30 minutes; S2, fully immersing the fiber substrate obtained in step S1 in the MXene suspension for 6-8 hours, taking it out and drying it in a vacuum oven at 10-60° C.; repeating the above immersion and drying steps 2-6 times; S3, placing the MXene composite fiber substrate obtained in step S2 in a conductive polymer monomer solution, and then preparing an artificial nerve fiber having a porous nano-needle, linear and mesh composite structure through a low-temperature in-situ polymerization reaction after infiltration; S4, loading the biorecognition molecule onto the artificial nerve fiber obtained in step S3 to obtain a gate artificial nerve fiber; S5, using the artificial nerve fiber obtained in step S3 as the source and drain of the transistor, and applying silver paste on both ends; dripping electrolyte at the middle position, waiting for it to dry slightly, and then dripping another drop, repeating this 2-3 times to build up to a certain height to form a gel electrolyte; placing the gate artificial nerve fiber obtained in step S4 on the gel electrolyte in a cross shape, and at the same time dripping another drop of gel electrolyte, also waiting for it to dry slightly, and then dripping another drop after it is slightly dried, so as to obtain a fiber-based synaptic transistor with ultra-low energy consumption and plasticity mediated by body fluid physiological markers.

2. The method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity according to claim 1, characterized in that: In step S2, the concentration of the MXene suspension is 0.1 to 12 mg / ml.

3. The method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity according to claim 1, characterized in that: In step S3, the low-temperature in-situ polymerization is carried out for 12 to 72 hours.

4. The method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity according to claim 1, characterized in that: The MXene is Ti3C2T x 、Mo2CT x 、Mo2TiC2T x 、Cr2TiC2T x One or more of the above, the layer thickness is 1 to 10 nm.

5. The method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity according to claim 1, characterized in that: In step S4, the method of loading the biorecognition molecule onto the artificial nerve fiber is one or more of physical adsorption method, chemical coupling method, bioaffinity method, physical embedding method, and self-assembly technology.

6. The method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity according to claim 1, characterized in that: The conductive polymer is one of polyaniline, polypyrrole, polythiophene, poly-3-hexylthiophene, poly-3-cyclohexylthiophene, thiophenepyrrolopyrroledione, and polyethylene oxide; the fiber substrate is one or more of cotton, wool, silk, nylon, polyester, acrylic, vinylon, polypropylene, viscose, carbon fiber, and aramid fiber.

7. The method for preparing a fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity according to claim 1, characterized in that: The gel electrolyte is one of an ionic liquid gel electrolyte and a biomass gel electrolyte.

8. A fiber-based synaptic transistor with ultra-low energy consumption and fluid physiological marker-mediated plasticity, characterized in that: Prepared by the preparation method described in any one of claims 1-7; the fiber-based synaptic transistor consists of a source-drain artificial nerve fiber, a gate artificial nerve fiber and an electrolyte; the source-drain artificial nerve fiber includes a fiber substrate, a conductive polymer loaded on the fiber substrate and MXene; the gate artificial nerve fiber includes a fiber substrate, a conductive polymer loaded on the fiber substrate, MXene and a biorecognition molecule.

9. The fiber-based synaptic transistor with ultra-low energy consumption and body fluid physiological marker-mediated plasticity according to claim 8, characterized in that: The fiber-based synaptic transistor operates at a voltage of less than 0.5V and has an energy consumption as low as 0.10 fJ / spike.

10. An application of a fiber-based synaptic transistor prepared by the preparation method according to any one of claims 1 to 7 or a fiber-based synaptic transistor according to claims 8 to 9, characterized in that: The fiber-based synaptic transistor is used in the fields of low-energy consumption, high-body fluid physiological marker material-mediated plasticity artificial synapses, brain-computer interfaces, sensory nerves, and intelligent electronic fabrics.

Images