Thermoelectric driving fiber-based organic electrochemical synaptic transistor and preparation method and application thereof

Abstract

The invention provides a thermoelectric driving fiber-based organic electrochemical synapse transistor and a preparation method and application thereof, and the thermoelectric driving fiber-based organic electrochemical synapse transistor is composed of a thermoelectric energy supply device, a fiber-based organic electrochemical synapse transistor and wires for connecting all parts. The thermoelectric energy supply device comprises a P-type thermoelectric fiber and an N-type thermoelectric material, and the fiber-based organic electrochemical synaptic transistor comprises a source-drain fiber electrode, a grid fiber electrode and an ionic gel electrolyte. According to the thermoelectric energy supply device prepared based on the Seebeck effect, conversion from heat energy of the human body to electric energy can be achieved, and stable energy supply to the synaptic transistor can be achieved. The integration of the thermoelectric energy supply device and the fiber-based organic electrochemical synaptic transistor has a wide application prospect in the fields of medical treatment, intelligent materials and wearable equipment.

Description

Technical Field

[0001] The present invention relates to the field of electrochemical technology, and in particular to a thermoelectrically driven fiber-based organic electrochemical synaptic transistor and a preparation method and application thereof. Background Art

[0002] PEDOT:PSS (poly (3,4-ethylenedioxythiophene / polystyrene sulfonate)) is an electrically conductive polymer with good electrical conductivity and biocompatibility, which is widely used in the fields of flexible electronics and biomedicine. Thermoelectric effect refers to the phenomenon that when two different metals or semiconductor materials move charges under the action of temperature gradient, an electromotive force is generated. Thermoelectric effect can be applied to fields such as energy conversion and refrigeration technology. Organic electrochemical synaptic transistor is an electrochemical device based on ion gel electrolyte, which has signal transmission and processing functions similar to biological synapses and can simulate the signal processing mechanism in the human nervous system. In the prior art, thermoelectric effect, PEDOT:PSS and organic electrochemical synaptic transistor have been widely studied and applied, but there are the following problems in practical applications: 1. The conversion efficiency of thermoelectric power generation devices is not high, energy utilization is not sufficient, and it is difficult to achieve a stable energy supply; 2. The conductivity and biocompatibility of PEDOT:PSS need to be further improved to obtain better application effects; 3. Organic electrochemical synaptic transistors are prone to ion gel electrolyte failure, electrode breakage and other problems during long-term use, affecting the long-term stability and reliability of the device.

[0003] In view of this, it is necessary to design an improved thermoelectrically driven fiber-based organic electrochemical synaptic transistor and its preparation method and application to solve the above problems. Summary of the invention

[0004] In view of the defects of the above-mentioned prior art, the purpose of the present invention is to provide a thermoelectrically driven fiber-based organic electrochemical synaptic transistor and its preparation method and application. The thermoelectric energy supply device prepared based on the Seebeck effect can realize the conversion of human body thermal energy into electrical energy, and can realize stable energy supply to the synaptic transistor. The integration of the thermoelectric energy supply device and the organic electrochemical synaptic transistor has broad application prospects in the fields of medical care, smart materials, and wearable devices.

[0005] To achieve the above-mentioned purpose, the present invention provides a thermoelectrically driven fiber-based organic electrochemical synapse transistor, which is composed of a thermoelectric power supply device, a fiber-based organic electrochemical synapse transistor and wires connecting the various parts. The thermoelectric power supply device includes a P-type thermoelectric fiber and an N-type thermoelectric material. The P-type thermoelectric fiber is composed of a PEDOT:PSS aqueous dispersion, carbon nanotubes, an organic solvent and a polymer. The ratio of the added amount of the carbon nanotubes to the solid content of the PEDOT:PSS aqueous dispersion is (0.05-0.2):1; the added amount of the polymer is 1-10wt% of the PEDOT:PSS aqueous dispersion.

[0006] As a further improvement of the present invention, the carbon nanotubes are one or more of carboxylated single-walled carbon nanotubes, hydroxylated single-walled carbon nanotubes, single-walled carbon nanotubes, carboxylated multi-walled carbon nanotubes, hydroxylated multi-walled carbon nanotubes, and multi-walled carbon nanotubes, and the polymer is one or two of polyvinyl alcohol and polypyrrole.

[0007] As a further improvement of the present invention, the organic solvent is one or both of dimethyl sulfoxide and ethylene glycol, and the amount of the organic solvent added is 1 to 5 vol% of the PEDOT:PSS aqueous dispersion.

[0008] As a further improvement of the present invention, the P-type thermoelectric fiber is prepared by one or more of wet spinning, electrospinning, and sea-island spinning.

[0009] As a further improvement of the present invention, the N-type thermoelectric material is one or more of constantan wire, PbTe, graphene, carbon nanotubes, fullerene derivatives and a mixed solution of ethanol and polyetherimide.

[0010] The P-type thermoelectric fiber and the N-type thermoelectric material are wound and woven into a flexible fabric substrate to form a power supply unit. The thermoelectric energy supply device is composed of a plurality of power supply units, and the power supply units are connected by electrodes.

[0011] As a further improvement of the present invention, the fiber-based organic electrochemical synaptic transistor includes a source-drain fiber electrode, a gate fiber electrode and an ion gel electrolyte, the source-drain fiber electrode and the gate fiber electrode are prepared from PEDOT:PSS composite fibers, and the preparation method of the PEDOT:PSS composite fibers includes the following steps:

[0012] S1. Fully blending a PEDOT:PSS aqueous dispersion with an antifreeze and a polymer to obtain a uniform PEDOT:PSS mixed solution, wherein the antifreeze is one or more of ethylene glycol, propylene glycol, glycerol, thiol, vinyl acetate and calcium chloride, and the content of the antifreeze in the PEDOT:PSS aqueous dispersion is 1 to 5 vol%, and the polymer is one or more of polyvinyl alcohol, polyethylene, polypropylene, polyvinyl chloride, polystyrene, polyurethane, polyoxymethylene and polyethylene glycol, and the content of the polymer in the PEDOT:PSS aqueous dispersion is 1 to 10%;

[0013] S2. Freeze the PEDOT:PSS mixed solution obtained in step S1 at -80°C to -30°C for 6 to 48 hours, thaw at room temperature for 2 to 6 hours, and repeat the above freezing cycle process 1 to 5 times to obtain a wet spinning solution;

[0014] S3. The wet spinning solution described in step S2 is spun into PEDOT:PSS composite fibers using wet spinning technology.

[0015] The present invention also provides an application of the above-mentioned thermoelectrically driven fiber-based organic electrochemical synapse transistor, and the thermoelectrically driven fiber-based organic electrochemical synapse transistor is applied in the fields of medical treatment, smart materials and wearable devices.

[0016] The beneficial effects of the present invention are:

[0017] (1) The present invention provides a thermoelectrically driven fiber-based organic electrochemical synaptic transistor and a preparation method and application thereof. The thermoelectrically driven fiber-based organic electrochemical synaptic transistor is composed of a thermoelectric energy supply device, a fiber-based organic electrochemical synaptic transistor, and a wire connecting the various parts. The thermoelectric energy supply device includes a P-type thermoelectric fiber and an N-type thermoelectric material. The fiber-based organic electrochemical synaptic transistor includes a source-drain fiber electrode, a gate fiber electrode, and an ion gel electrolyte. The thermoelectric energy supply device prepared based on the Seebeck effect can realize the conversion of human body thermal energy into electrical energy, and can realize stable energy supply to the synaptic transistor. The integration of the thermoelectric energy supply device and the fiber-based organic electrochemical synaptic transistor has broad application prospects in the fields of medical care, smart materials, and wearable devices.

[0018] (2) The present invention sews thermoelectric fibers composed of PEDOT:PSS, carbon nanotubes, organic solvents and polymers and coated N-type thermoelectric materials onto a fabric substrate to form a thermoelectric power supply device, thereby further improving the wearability and integration of the device.

[0019] (3) The present invention uses PEDOT:PSS, antifreeze and polymer as the base material, and prepares a composite fiber electrode with high strength and stretchability through freeze-thaw pretreatment and wet spinning technology. The composite fiber electrode can meet the needs of devices of different shapes and sizes, and can also avoid problems such as breakage or failure of the electrode during operation. The prepared fiber-based organic electrochemical synaptic transistor has a high switching ratio, fast response rate, low energy consumption, excellent synaptic plasticity, and good pulse cycle stability, and can achieve high-precision and high-efficiency signal transmission and data processing. BRIEF DESCRIPTION OF THE DRAWINGS

[0020] Figure 1 This is a scanning electron microscope image of the P-type thermoelectric fiber provided in Example 1 of the present invention.

[0021] Figure 2 This is the Seebeck coefficient of the P-type thermoelectric fiber provided in Example 1 of the present invention.

[0022] Figure 3 The thermovoltage of the thermoelectric energy supply device under 0K temperature difference provided in Example 1 of the present invention.

[0023] Figure 4 Thermovoltage of the thermoelectric power supply device under a temperature difference of 4K provided in Example 1 of the present invention.

[0024] Figure 5 Thermovoltage of the thermoelectric energy supply device under a temperature difference of 5K provided in Example 1 of the present invention.

[0025] Figure 6 The thermoelectric energy supply device provided in Example 1 of the present invention is the post-synaptic response current and its peak value of the fiber-based organic electrochemical synapse transistor when the gate voltage is supplied.

[0026] Figure 7 It is a comparison chart of the Seebeck coefficients of Example 1 of the present invention and Comparative Example 3. DETAILED DESCRIPTION

[0027] In order to make the purpose, technical solutions and advantages of the present invention more clear, the present invention is described in detail below with reference to the accompanying drawings and specific embodiments.

[0028] It should also be noted that, in order to avoid obscuring the present invention due to unnecessary details, only structures and / or processing steps closely related to the scheme of the present invention are shown in the drawings, while other details that are not closely related to the present invention are omitted.

[0029] In addition, it should be noted that the terms "comprises", "includes" or any other variations thereof are intended to cover non-exclusive inclusion, so that a process, method, article or apparatus that includes a series of elements includes not only those elements, but also other elements not explicitly listed, or also includes elements inherent to such process, method, article or apparatus.

[0030] The present invention provides a thermoelectrically driven fiber-based organic electrochemical synaptic transistor, which is composed of a thermoelectric energy supply device, a fiber-based organic electrochemical synaptic transistor, and a wire connecting the various parts. The thermoelectric energy supply device includes a P-type thermoelectric fiber and an N-type thermoelectric material. The fiber-based organic electrochemical synaptic transistor includes a source-drain fiber electrode, a gate fiber electrode, and an ion gel electrolyte. Through the integrated thermoelectric energy supply device, the present invention can directly convert thermal energy into electrical energy, thereby providing power for the fiber-based organic electrochemical synaptic transistor, reducing dependence on an external power source. Due to the use of a fiber-based structure and a flexible fabric substrate, the synaptic transistor of the present invention has good flexibility and bendability, and is suitable for integration into wearable electronic products. The thermoelectric energy supply device can provide stable electrical energy for the synaptic transistor, ensuring the long-term stable operation of the device.

[0031] Specifically, the P-type thermoelectric fiber is prepared from a PEDOT:PSS aqueous dispersion, carbon nanotubes, an organic solvent and a polymer, and is used to improve flexibility, conductivity, thermoelectric performance and power supply stability. The carbon nanotubes are preferably one or more of carboxylated single-walled carbon nanotubes, hydroxylated single-walled carbon nanotubes, single-walled carbon nanotubes, carboxylated multi-walled carbon nanotubes, hydroxylated multi-walled carbon nanotubes and multi-walled carbon nanotubes, and the ratio of the amount of carbon nanotubes added to the solid content of the PEDOT:PSS aqueous dispersion is preferably (0.05-0.2):1.

[0032] The polymer is one or both of polyvinyl alcohol and polypyrrole, and the added amount of the polymer is preferably 1-10wt% of the PEDOT:PSS aqueous dispersion; the organic solvent is one or both of dimethyl sulfoxide and ethylene glycol, and the added amount of the organic solvent is preferably 1-5vol% of the PEDOT:PSS aqueous dispersion.

[0033] The addition of carbon nanotubes significantly improves the conductivity of PEDOT:PSS composites, because carbon nanotubes have extremely high electrical conductivity and can form an effective conductive network. Carbon nanotubes can also optimize the thermoelectric properties of the material by changing its microstructure, thereby improving the thermoelectric conversion efficiency. The addition of polymers not only improves the flexibility of the material, but also enhances its mechanical strength, making the thermoelectric fibers more durable during wear. The selection and addition amount of organic solvents have an important influence on the processability of PEDOT:PSS composites. Appropriate solvents can make the material easier to handle during processing and help form a uniform fiber structure. By optimizing the material composition, the environmental stability of P-type thermoelectric fibers is improved, and they can maintain their performance under different temperature and humidity conditions.

[0034] The preparation method of the P-type thermoelectric fiber is preferably one or more of wet spinning, electrospinning, and sea-island spinning.

[0035] The N-type thermoelectric material is preferably one or more of constantan wire, PbTe, graphene, carbon nanotubes, fullerene derivatives, and a mixed solution of ethanol and polyetherimide.

[0036] The P-type thermoelectric fiber and the N-type thermoelectric material are wound and woven into a flexible fabric substrate to form a power supply unit. The thermoelectric energy supply device is composed of a plurality of power supply units, and the power supply units are connected by electrodes to achieve effective energy supply of the power supply units. The mass percentage of the P-type thermoelectric fiber to the N-type thermoelectric material is preferably 10 to 20%.

[0037] Materials such as constantan wire and PbTe combined with P-type thermoelectric fibers can form efficient thermoelectric conversion pairs, thereby improving the conversion efficiency of thermoelectric power supply devices. Through the woven structure, the electrode connection between the power supply units ensures the continuity and stability of the power supply and reduces performance fluctuations caused by mechanical deformation. The use of flexible fabric substrates makes the thermoelectric power supply device have good flexibility and can adapt to different application scenarios and wearable needs. The ratio of P-type thermoelectric fibers to N-type thermoelectric materials helps to balance the thermoelectric properties of the two materials and achieve the best thermoelectric conversion effect.

[0038] The source-drain fiber electrode and the gate fiber electrode in the fiber-based organic electrochemical synaptic transistor are prepared from PEDOT:PSS composite fibers. The preparation method of the PEDOT:PSS composite fibers comprises the following steps:

[0039] S1. Fully blend the PEDOT:PSS aqueous dispersion with an antifreeze and a polymer to obtain a uniform PEDOT:PSS mixed solution. The antifreeze is preferably one or more of ethylene glycol, propylene glycol, glycerol, thiol, vinyl acetate and calcium chloride. The content of the antifreeze in the PEDOT:PSS aqueous dispersion is preferably 1 to 5 vol%. The polymer is preferably one or more of polyvinyl alcohol, polyethylene, polypropylene, polyvinyl chloride, polystyrene, polyurethane, polyoxymethylene and polyethylene glycol. The mass ratio of the polymer in the PEDOT:PSS aqueous dispersion is preferably 1 to 10 wt%.

[0040] S2. Freeze the PEDOT:PSS mixed solution obtained in step S1 at -80°C to -30°C for 6 to 48 hours, thaw at room temperature for 2 to 6 hours, and repeat the above freezing cycle process 1 to 5 times to obtain a wet spinning solution.

[0041] S3. The wet spinning solution in step S2 is spun into PEDOT:PSS composite fibers using wet spinning technology. The coagulation bath is preferably one or more of deionized water, methanol, ethanol, isopropanol, acetone, dimethyl sulfoxide, and N,N-dimethylformamide. The spinning needle is 14G to 26G thick, 4mm to 25mm long, the spinning extrusion speed is preferably 0.2mm / min to 2.0mm / min, the spinning winding speed is preferably 0.2mm / min to 4.0mm / min, and the winding method is winding in the coagulation bath.

[0042] The thermoelectrically driven fiber-based organic electrochemical synaptic transistor and the preparation method thereof provided by the present invention are described below in conjunction with specific embodiments.

[0043] Example 1

[0044] Embodiment 1 provides a thermoelectrically driven fiber-based organic electrochemical synaptic transistor, which is composed of a thermoelectric energy supply device, a fiber-based organic electrochemical synaptic transistor and wires connecting the various parts. The thermoelectric energy supply device is composed of a plurality of power supply units, and the power supply unit is prepared by winding and weaving a P-type thermoelectric fiber and an N-type thermoelectric material in a flexible fabric substrate. The P-type thermoelectric fiber is prepared by wet spinning a PEDOT:PSS aqueous dispersion, carbon nanotubes, dimethyl sulfoxide and polyvinyl alcohol, wherein the ratio of the added amount of carbon nanotubes to the solid content of the PEDOT:PSS aqueous dispersion is 0.15:1, the added amount of polyvinyl alcohol is 5% of the PEDOT:PSS aqueous dispersion, the added amount of dimethyl sulfoxide is 5% of the PEDOT:PSS aqueous dispersion, the N-type thermoelectric material is constantan wire, and the mass ratio of the P-type thermoelectric fiber to the N-type thermoelectric material is 10%. Pour the PEDOT:PSS aqueous dispersion into a mixing container, add the weighed carbon nanotubes, and use a stirrer to stir thoroughly to ensure that the carbon nanotubes are evenly dispersed in the PEDOT:PSS solution. Add polyvinyl alcohol and dimethyl sulfoxide, and continue stirring until all components are completely mixed. Degas the mixed solution to remove bubbles in the solution to ensure the uniformity of the fibers during the spinning process. Inject the degassed solution into the spinning device for wet spinning. The coagulation bath is deionized water, the spinning needle thickness is 16G, the spinning needle length is 10mm, the spinning extrusion speed is 1.0mm / min, the spinning winding speed is 2.0mm / min, and the winding method is winding in the coagulation bath.

[0045] The fiber-based organic electrochemical synaptic transistor comprises a source-drain fiber electrode, a gate fiber electrode and an ion gel electrolyte. The source-drain fiber electrode and the gate fiber electrode are prepared from PEDOT:PSS composite fibers. The preparation method of the PEDOT:PSS composite fibers is as follows: PEDOT:PSS is fully blended with ethylene glycol and polyvinyl alcohol to obtain a uniform PEDOT:PSS mixed solution; wherein the mass ratio of ethylene glycol in the PEDOT:PSS aqueous solution is 10%, and the volume ratio of polyvinyl alcohol in the PEDOT:PSS aqueous solution is 5%; the PEDOT:PSS mixed solution is frozen in a -30°C refrigerator for 12 hours, thawed at room temperature for 4 hours, and the above freezing cycle process is repeated 3 times to obtain a wet spinning solution; the wet spinning solution is spun into PEDOT:PSS composite fibers using wet spinning technology, the coagulation bath is deionized water, the spinning needle thickness is 16G, the spinning needle length is 10mm, the spinning extrusion speed is 1.0mm / min, the spinning winding speed is 2.0mm / min, and the winding method is winding in the coagulation bath. The ion gel electrolyte is prepared from P(VDF-HFP) (poly(vinylidene fluoride-hexafluoropropylene)), EMIM (1-ethyl-3-methylimidazole): TFSI (bis(trifluoromethanesulfonyl)imide) and acetone. The preparation method is as follows: the raw materials are mixed in a mass ratio of P(VDF-HFP):(EMIM:TFSI):acetone=1:4:7, and the mixture is continuously stirred in a water bath at 60°C until the particles are completely dissolved, and the ion gel electrolyte is obtained after cooling.

[0046] See also Figure 1 As shown, it is a scanning electron microscope image of the P-type thermoelectric fiber provided in Example 1, and the microstructure of the fiber can be clearly seen. The fiber surface in the left picture is smooth and has a certain toughness. The cross-section of the fiber can be seen in the right picture. Due to the addition of ionic solution, the fiber cross-section shrinks and presents an elliptical shape. Smooth fibers are convenient for making separate power generation devices and have the possibility of being used in wearable devices.

[0047] See also Figure 2 As shown, it is the Seebeck coefficient of the P-type thermoelectric fiber provided in Example 1, and it can be seen that its Seebeck coefficient is 23μV / K. As an important indicator for measuring the performance of thermoelectric materials, the Seebeck coefficient can reflect the ability of the material to convert thermal energy into electrical energy. The P-type thermoelectric fiber in this application shows excellent thermoelectric performance.

[0048] See also Figures 3 to 5 As shown, the thermovoltage of the thermoelectric energy supply device provided in Example 1 at different temperature differences, it can be seen that as the temperature increases, the thermovoltage gradually increases, indicating that thermal energy is converted into electrical energy. At the same temperature, the thermovoltage remains stable, indicating that the thermoelectric energy supply device has good stability.

[0049] See also Figure 6 As shown, the postsynaptic response current of the fiber-based organic electrochemical synapse transistor when the thermoelectric power supply device provided in Example 1 supplies energy for the gate voltage, as the gate voltage value increases, the peak value of the excitatory postsynaptic response current gradually increases, and conforms to the doping law of P-type semiconductors, indicating that the thermoelectric power supply unit can successfully drive the fiber-based organic electrochemical synapse transistor to work.

[0050] Example 2-3 and Comparative Example 1-2

[0051] Examples 2-3 and Comparative Examples 1-2 respectively provide a thermoelectrically driven fiber-based organic electrochemical synaptic transistor. Compared with Example 1, the only difference is that the ratio of the added amount of carbon nanotubes to the solid content of the PEDOT:PSS aqueous dispersion is different, which are 0.05:1, 0.10:1, 0, and 0.25:1, respectively. Other experimental parameters and conditions are basically the same as those in Example 1 and will not be repeated here.

[0052] As shown in Table 1, the conductivity of Comparative Example 1 is low, which is 2.6 S·cm, because carbon nanotubes are not added. -1 , the Seebeck coefficient is 15.6μV / K; in comparative example 2, although the conductivity is improved by adding excessive carbon nanotubes, the wet-spun fibers cannot be continuously spun and have no use value; the experimental results of examples 2-3 and comparative examples 1-2 show that adding carbon nanotubes can effectively increase the Seebeck coefficient and conductivity, but excessive carbon nanotubes will destroy the continuity of the fibers. Therefore, the ratio of the amount of carbon nanotubes added to the solid content of PEDOT:PSS is controlled at (0.05-0.2):1, ensuring the conductivity while not reducing the toughness of the fibers.

[0053] Examples 4-5 and Comparative Examples 3-4

[0054] Examples 4-5 and Comparative Examples 3-4 respectively provide a thermoelectrically driven fiber-based organic electrochemical synapse transistor. Compared with Example 1, the only difference is that the volume fraction of the organic solvent added to the P-type thermoelectric fiber is different, which is 1%, 3%, and 0.7%, respectively. The other experimental parameters and conditions are basically the same as those in Example 1 and will not be repeated here.

[0055] As shown in Table 1 and Figure 7 As shown, in Comparative Example 3, no dimethyl sulfoxide was added, and the conductivity and Seebeck coefficient were both low. In Comparative Example 4, excessive dimethyl sulfoxide was added, and the conductivity and Seebeck coefficient decreased compared with Example 1. The test results of Experimental Examples 4 and 5 show that with the increase of doping level, the fiber conductivity and Seebeck increased to varying degrees. Therefore, adding 1 to 5 vol% of dimethyl sulfoxide can maintain a high fiber conductivity and Seebeck coefficient.

[0056] Examples 6-7 and Comparative Examples 5-6

[0057] Examples 6-7 and Comparative Examples 5-6 respectively provide a thermoelectrically driven fiber-based organic electrochemical synaptic transistor. Compared with Example 1, the only difference is that the amount of polymer added in the P-type thermoelectric fiber is different, which is 3%, 8%, 0, and 15% respectively. The other experimental parameters and conditions are basically the same as those in Example 1 and will not be repeated here.

[0058] As shown in Table 1, in Example 6-7 and Comparative Example 5-6, with the addition of polyvinyl alcohol, the conductive components in the spinning solution are diluted, resulting in a decrease in the overall conductivity. The addition of polyvinyl alcohol may destroy the conductive network originally formed in the fiber and reduce the migration path of the charge carriers. The Seebeck coefficient decreases with the increase of polyvinyl alcohol. The addition of polyvinyl alcohol changes the composite properties of the fiber material and the electron density inside the fiber, resulting in a weakening of the Seebeck effect. Controlling the amount of polymer added to 1-10wt% of the PEDOT:PSS aqueous dispersion can balance the conductivity and mechanical properties of the fiber and realize its application in the field of wearable electronics.

[0059] Table 1 Performance test data of embodiments and comparative examples

[0060] project Seebeck coefficient (μV / K) <![CDATA[Conductivity (S·cm -1 )]]> Example 1 23.0 30.3 Example 2 17.8 11.5 Example 3 20.8 25.1 Example 4 7.9 7.5 Example 5 20.1 28.7 Example 6 24.5 32 Example 7 19.8 24.3 Comparative Example 1 15.6 2.6 Comparative Example 2 27.1 60.1 Comparative Example 3 6.6 6.6 Comparative Example 4 19.7 29.2 Comparative Example 5 23.5 35.1 Comparative Example 6 8.9 5.6

[0061] In summary, the present invention provides a thermoelectrically driven fiber-based organic electrochemical synaptic transistor and its preparation method and application. The thermoelectric energy supply device prepared based on the Seebeck effect can realize the conversion of human body thermal energy into electrical energy, and can realize stable energy supply to the synaptic transistor. The integration of the thermoelectric energy supply device and the fiber-based organic electrochemical synaptic transistor has broad application prospects in the fields of medical care, smart materials, and wearable devices.

[0062] The above embodiments are only used to illustrate the technical solution of the present invention rather than to limit it. Although the present invention has been described in detail with reference to the preferred embodiments, those skilled in the art should understand that the technical solution of the present invention may be modified or replaced by equivalents without departing from the spirit and scope of the technical solution of the present invention.

Claims

1. A thermoelectrically driven fiber-based organic electrochemical synaptic transistor, characterized in that: It is composed of a thermoelectric energy supply device, a fiber-based organic electrochemical synaptic transistor, and a wire connecting the various parts. The thermoelectric energy supply device includes a P-type thermoelectric fiber and an N-type thermoelectric material. The P-type thermoelectric fiber is prepared from a PEDOT:PSS aqueous dispersion, carbon nanotubes, an organic solvent and a polymer. The ratio of the amount of the carbon nanotubes added to the solid content of the PEDOT:PSS aqueous dispersion is (0.05-0.2):1; the amount of the polymer added is 1-10wt% of the PEDOT:PSS aqueous dispersion.

2. The thermoelectrically driven fiber-based organic electrochemical synaptic transistor according to claim 1, characterized in that: The carbon nanotubes are one or more of carboxylated single-walled carbon nanotubes, hydroxylated single-walled carbon nanotubes, single-walled carbon nanotubes, carboxylated multi-walled carbon nanotubes, hydroxylated multi-walled carbon nanotubes, and multi-walled carbon nanotubes.

3. The thermoelectrically driven fiber-based organic electrochemical synaptic transistor according to claim 1, characterized in that: The polymer is one or both of polyvinyl alcohol and polypyrrole.

4. The thermoelectrically driven fiber-based organic electrochemical synaptic transistor according to claim 1, characterized in that: The organic solvent is one or both of dimethyl sulfoxide and ethylene glycol; the added amount of the organic solvent is 1-5 vol% of the PEDOT:PSS aqueous dispersion.

5. The thermoelectrically driven fiber-based organic electrochemical synaptic transistor according to claim 1, characterized in that: The P-type thermoelectric fiber is prepared by one or more of wet spinning, electrostatic spinning, and sea-island spinning.

6. The thermoelectrically driven fiber-based organic electrochemical synaptic transistor according to claim 1, characterized in that: The N-type thermoelectric material is one or more of constantan wire, PbTe, graphene, carbon nanotube, fullerene derivative and a mixed solution of ethanol and polyetherimide.

7. The thermoelectrically driven fiber-based organic electrochemical synaptic transistor according to claim 6, characterized in that: The P-type thermoelectric fiber and the N-type thermoelectric material are wound and woven into a flexible fabric substrate to form a power supply unit. The thermoelectric energy supply device is composed of a plurality of power supply units, and the power supply units are connected by electrodes.

8. The thermoelectrically driven fiber-based organic electrochemical synaptic transistor according to claim 1, characterized in that: The fiber-based organic electrochemical synapse transistor comprises a source-drain fiber electrode, a gate fiber electrode and an ion gel electrolyte.

9. The thermoelectrically driven fiber-based organic electrochemical synaptic transistor according to claim 8, characterized in that: The source-drain fiber electrode and the gate fiber electrode are prepared from PEDOT:PSS composite fibers. The preparation method of the PEDOT:PSS composite fibers comprises the following steps: S1. Fully blending a PEDOT:PSS aqueous dispersion with an antifreeze and a polymer to obtain a uniform PEDOT:PSS mixed solution, wherein the antifreeze is one or more of ethylene glycol, propylene glycol, glycerol, thiol, vinyl acetate and calcium chloride, and the content of the antifreeze in the PEDOT:PSS aqueous dispersion is 1 to 5 vol%, and the polymer is one or more of polyvinyl alcohol, polyethylene, polypropylene, polyvinyl chloride, polystyrene, polyurethane, polyoxymethylene and polyethylene glycol, and the content of the polymer in the PEDOT:PSS aqueous dispersion is 1 to 10 wt%; S2. Freeze the PEDOT:PSS mixed solution obtained in step S1 at -80°C to -30°C for 6 to 48 hours, thaw at room temperature for 2 to 6 hours, and repeat the above freezing cycle process 1 to 5 times to obtain a wet spinning solution; S3. The wet spinning solution described in step S2 is spun into PEDOT:PSS composite fibers using wet spinning technology.

10. An application of the thermoelectric driven fiber-based organic electrochemical synapse transistor according to any one of claims 1 to 9, characterized in that: The thermoelectrically driven fiber-based organic electrochemical synaptic transistor is used in the fields of medical treatment, smart materials and wearable devices.

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