Wearable thermoelectric generator based on flexible corrugated tellurium film and preparation method

Abstract

The application provides a wearable thermoelectric generator based on a flexible corrugated tellurium film and a preparation method, which comprises the following steps: realizing a flexible tellurium-based film with p-type and n-type thermoelectric units arranged alternately on a single-layer tellurium film, and then bending, folding and packaging the film; placing the exposed end of the pn junction of the corrugated tellurium film thermoelectric generator at the hot end and the other end in the air, so as to ensure that the cold and hot ends of the device generate a temperature difference, thereby making the multiple carriers of the p-type and n-type semiconductors migrate from the hot end to the cold end, and forming a consistent thermoelectric potential; the alternately arranged thermoelectric units are at least one pair of pn pairs, and when the thermoelectric unit pairs are connected in series, the stretchability of the device is significantly enhanced. The application can generate electricity in different common life heat sources, such as a human wrist, a hot water cup, a computer radiator and the like, and has the advantages of low cost, simple reproduction and replaceable use materials.

Description

TECHNICAL FIELD

[0001] The present application belongs to the field of nanobiological sensors, and particularly relates to a wearable thermoelectric generator based on a flexible corrugated tellurium film and a preparation method. BACKGROUND

[0002] Wearable electronic devices have become a research hotspot in recent years due to their application prospects in the fields of communication, medical care, sports detection, etc. The wearable electronic products on the market at present mainly rely on electrochemical energy storage batteries for power supply, but are limited by the battery life. Self-powered wearable electronic devices driven by human body heat through the thermoelectric effect are a very promising solution, which can directly convert waste heat into useful electrical energy. The principle of this Seebeck effect is that when there is a temperature difference between the two ends of a conductor, the majority of p-type and n-type semiconductors migrate from the hot end to the cold end, forming a consistent current. Therefore, the thermoelectric generator based on the Seebeck effect has the advantages of high reliability, long service life and maintenance-free, and has broad application prospects in the fields of aerospace, waste heat collection and human body heat collection.

[0003] However, the current thermoelectric generator is limited by the output voltage and power density, and its commercial application is very limited. How to reasonably design the structure of the device to achieve high output performance while having high stretchability so as to be suitable for various application scenarios has become a problem to be solved by researchers. Generally, people consider the optimization of thermoelectric materials and device structure design to achieve a thermoelectric device with high output performance and high stretchability. In terms of materials, the main consideration is to improve the dimensionless thermoelectric figure of merit of the thermoelectric material. In terms of device structure, researchers have proposed the idea of converting a two-dimensional planar structure into a three-dimensional structure. In recent years, a variety of three-dimensional structure thermoelectric generators utilizing the vertical temperature difference of the skin surface have been reported, including wave-shaped structures, spring structures, spiral structures, etc.

[0004] Among the existing thin-film-based three-dimensional structure thermoelectric generators, a power density output of 10.02 W m -2 has been achieved, but at the same time, complex processes and expensive equipment are also used. In many cases, p-type and n-type tellurium-based thin films need to be prepared separately, and then the p-type and n-type thermoelectric thin films are combined through a bonding step, and finally the device is folded to form a device, and the preparation process is complicated. However, the key to market competition lies in the cost-effectiveness and scalable manufacturing capability of the thermoelectric generator. Therefore, in order to meet the actual demand, it is necessary to efficiently utilize the temperature difference of the heat source while being able to be mass-integrated and meet certain wearing comfort. SUMMARY

[0005] In view of the above situation, the main purpose of the present application is to provide a wearable thermoelectric generator based on a flexible corrugated tellurium film and a preparation method to solve the above technical problems.

[0006] The application provides a wearable thermoelectric generator based on a flexible corrugated tellurium film, comprising a p-type tellurium film and an n-type tellurium-based film, the p-type tellurium film and the n-type tellurium-based film are both made of a single-layer tellurium film, and the p-type tellurium-based thermoelectric unit and the n-type tellurium-based thermoelectric unit are alternately arranged to form the p-type tellurium film and the n-type tellurium-based film.

[0007] The flexible film with the p-type tellurium-based thermoelectric unit and the n-type tellurium-based thermoelectric unit alternately arranged is bent, folded and packaged to obtain a corrugated tellurium-based film.

[0008] The exposed end of the pn junction of the thermoelectric generator in the corrugated tellurium-based film is arranged at the hot end, and the other end is arranged in the air, so that the carriers of the p-type semiconductor and the carriers of the n-type semiconductor migrate from the hot end to the cold end to generate a unified direction of thermoelectric potential.

[0009] The thermoelectric units generating the thermoelectric potential are connected in series to obtain the wearable thermoelectric generator.

[0010] The application further provides a preparation method of the wearable thermoelectric generator based on the flexible corrugated tellurium film, the method is used for preparing the wearable thermoelectric generator based on the flexible corrugated tellurium film, and the method comprises the following steps:

[0011] Tellurium nanowire powder and polyvinylidene fluoride powder are dissolved in an N,N-dimethylformamide solution to obtain a dissolution solution, and the dissolution solution is stirred to form a mixed solution.

[0012] The mixed solution is subjected to ultrasonic treatment to obtain a treatment solution.

[0013] The treatment solution is transferred to a glass sheet, and the glass sheet is placed on a hot plate for drying to obtain a dried p-type tellurium film.

[0014] The dried p-type tellurium film is transferred from the glass sheet to a single-sided polyimide adhesive tape as a substrate by using the single-sided polyimide adhesive tape as a substrate to obtain a flexible undoped p-type tellurium film with the single-sided polyimide adhesive tape as the substrate.

[0015] The single-sided polyimide adhesive tape is adhered to the p-type tellurium film as the substrate to obtain a completed tellurium film.

[0016] Silver nitrate and ethylene glycol are uniformly mixed to obtain a solution of uniformly mixed silver nitrate and ethylene glycol, the completed tellurium film is immersed in the solution of uniformly mixed silver nitrate and ethylene glycol for in-situ reaction doping modification, and is left overnight to obtain a silver-doped reaction film.

[0017] After sufficient reaction, the silver-doped reaction film is taken out and washed to remove excess raw materials and by-products on the surface of the film, and a cleaned film is obtained.

[0018] The cleaned film is dried to obtain a flexible film with p-type and n-type tellurium-based thermoelectric units arranged alternately;

[0019] The flexible film with p-type and n-type tellurium-based thermoelectric units arranged alternately is bent, folded and packaged to obtain a wave-shaped tellurium-based film;

[0020] The exposed end of the pn junction of the thermoelectric generator in the wave-shaped tellurium-based film is placed at the hot end, and the other end is placed in the air, so that the carriers of the p-type semiconductor and the carriers of the n-type semiconductor migrate from the hot end to the cold end to generate a unified direction of thermoelectric potential;

[0021] The thermoelectric units generating thermoelectric potential are connected in series to obtain a wearable thermoelectric generator.

[0022] Compared with the prior art, the present application has the following advantages:

[0023] 1、The present application can generate thermoelectric potential in common different life heat sources, such as human wrist, hot water cup or computer heat sink, etc., and when the device is placed on the surface of the heat source, the higher the temperature difference between the cold and hot ends of the device, the greater the thermoelectric potential generated.

[0024] 2、The present application has low preparation cost and simple preparation process, and can be used for large-scale manufacturing. The p-type tellurium film is prepared by low-cost solvent thermal method and drop casting method, and through the ingenious use of single-sided adhesive polyimide tape, the conversion of p-type and n-type tellurium-based thermoelectric units arranged alternately can be realized on a single-layer flexible p-type tellurium film. The thermoelectric power factor (PF=S 2 σ, S is the Seebeck coefficient, and σ is the electrical conductivity) of the prepared p-type and n-type tellurium-based film can reach 19.07 μW m -1 K -2 and 25.99 μW m -1 K -2 .

[0025] 3、The thermoelectric generator of the present application has a three-dimensional wave-shaped structure configuration, which can effectively utilize the temperature difference perpendicular to the surface of the heat source. The wave-shaped structure TEG designed with 3 p-n pairs (TEG-3pn) realizes an open-circuit voltage output of 50.46 mV when the temperature difference is 60 K. In addition, the designed scalability is realized by using the characteristics of the wave-shaped structure, and the output performance can be further improved by adjusting the geometric parameters (such as height and area) of the device. At the same time, the configuration of the wave-shaped structure and the packaging of polydimethylsiloxane realize the super-high stretchability of the device up to 300%.

[0026] 4、The present application has low cost, simple and easy to reproduce, and the use of materials can be replaced.

[0027] Additional aspects and advantages of the present application will be set forth in part in the description which follows, and in part will be obvious from the description, or can be learned by practice of the application. BRIEF DESCRIPTION OF DRAWINGS

[0028] Figure 1 Schematic diagram of the wearable thermoelectric generator of the present application worn on the wrist of a human body;

[0029] Figure 2 Process schematic diagram of the preparation of p-type tellurium thin film by the solvothermal method and drop casting method of the present application;

[0030] Figure 3 Process schematic diagram of the preparation of silver-doped p-type and n-type tellurium-based thermoelectric unit alternating thin film by the in-situ reaction method of the present application;

[0031] Figure 4 Process schematic diagram of the wearable thermoelectric generator with high stretchability achieved by using bending and folding and packaging technology of the present application;

[0032] Figure 5 Thermoelectric performance diagram of p-type and n-type tellurium-based thin film of the present application;

[0033] Figure 6 Voltage-current-power curve diagram of wave-shaped structure TEG-3pn under different ΔT of the present application;

[0034] Figure 7 Open-circuit voltage and output power diagram of wave-shaped structure TEG-3pn under different ΔT of the present application;

[0035] Figure 8 Change relationship diagram of open-circuit voltage of wave-shaped structure TEG with the number of p-n pairs in series of the present application;

[0036] Figure 9 Change relationship diagram of voltage of TEG with device height under different ΔT of the present application;

[0037] Figure 10 Change relationship diagram of voltage of TEG with device area under different ΔT of the present application;

[0038] Figure 11 Relative resistance and relative voltage change of TEG of the present application when bending 1000 times at a bending radius r = 15 mm;

[0039] Figure 12 Relative resistance and relative voltage change of TEG of the present application when stretching 1000 times at a stretching strength of 80%;

[0040] Figure 13 Change of relative resistance of TEG of the present application with tensile strain;

[0041] Figure 14 A physical demonstration diagram of the wave-shaped TEG of the present application stretched to 300%;

[0042] Figure 15 A voltage output diagram of the TEG-4pn of the present application in sitting and walking states, wherein the inserted diagram is a stable voltage output diagram of the TEG-4pn worn on the wrist of a human body;

[0043] Figure 16 A voltage output diagram of the TEG-8pn of the present application in sitting and walking states, wherein the inserted diagram is a stable voltage output diagram of the TEG-8pn worn on the wrist of a human body;

[0044] Figure 17 A voltage output of the TEG-4pn and the TEG-8pn of the present application respectively placed on a hot water cup at 70°C. DETAILED DESCRIPTION

[0045] Embodiments of the present application are described in detail below with reference to the attached drawing figures, wherein the same or like reference numerals and characters in the drawing figures throughout the drawing figures denote the same or functionsally similar elements. The embodiments described below with reference to the attached drawing figures are exemplary only, and are merely intended to explain the present application, and should not be understood as a limitation of the present application.

[0046] These and other aspects of embodiments of the present application will become apparent from the following description and the accompanying drawing figures. In the description of embodiments of the present application below, some specific implementations of embodiments of the present application are specifically disclosed in order to represent the principles of embodiments of the present application, but it should be understood that the scope of embodiments of the present application is not limited thereto.

[0047] Embodiment 1

[0048] The present embodiment proposes a wearable thermoelectric generator based on a flexible wave-shaped tellurium film, comprising a p-type tellurium film and an n-type tellurium-based film, the p-type tellurium film and the n-type tellurium-based film are both made of a single-layer tellurium film, and the p-type tellurium-based thermoelectric unit and the n-type tellurium-based thermoelectric unit are alternately arranged to form the p-type tellurium film and the n-type tellurium-based film;

[0049] The flexible film with the p-type tellurium-based thermoelectric unit and the n-type tellurium-based thermoelectric unit alternately arranged is bent and folded and encapsulated to obtain a wave-shaped tellurium-based film;

[0050] The exposed end of the pn junction of the thermoelectric generator in the wave-shaped tellurium-based film is placed at the hot end, and the other end is placed in the air, so that the carriers of the p-type semiconductor and the carriers of the n-type semiconductor migrate from the hot end to the cold end to generate a unified direction of thermoelectric potential;

[0051] The thermoelectric units generating thermoelectric potential are connected in series to obtain a wearable thermoelectric generator.

[0052] Example 2

[0053] Reference is made to Figure 2 , this embodiment provides the preparation process of p-type thin film on the basis of example 1, in this embodiment, the solvent thermal method and drop casting method are used for the preparation of p-type thin film, the method for preparing tellurium nanowire powder by the solvent thermal method in this embodiment includes method one, method two, method three or method four;

[0054] The specific steps of method one are as follows:

[0055] 1.5g of sodium tellurite and 7.5g of ascorbic acid powder were mixed in 120ml of ethylene glycol solution and stirred for 0.3h, after the solute was completely dissolved, a mixed solution was obtained, and the mixed solution was transferred to a 90℃ tetrafluoroethylene high-pressure reaction kettle with a stirring rate of 450rpm and stirred for 20h;

[0056] After the reaction was completed, the reaction product was obtained, the reaction product was cooled to room temperature, and three times of centrifugal washing were carried out in a centrifuge with a rotation speed of 5000rpm, each time for 5min, to remove by-products and excess raw materials, and ultrasonic cleaning was carried out for 4min after the centrifugation was completed.

[0057] After the ultrasonic cleaning was completed, the washed tellurium powder was obtained, and the washed tellurium powder was placed in a 60℃ oven and baked for 12h to obtain tellurium nanowire powder.

[0058] The specific steps of method two are as follows:

[0059] 1g of ascorbic acid and 0.1g of cetyltrimethylammonium bromide were dissolved in 40ml of distilled water to obtain a clear solution;

[0060] 0.052g of sodium tellurite powder was added to the solution, and the solution was stirred vigorously for 0.2h to form a white suspension, the suspension was heated to 90℃ and reacted for 20h to obtain a reaction mixture;

[0061] After the reaction mixture was cooled to room temperature, 50ml of ethanol was added to the reaction mixture to precipitate, and tellurium nanowires were obtained;

[0062] The tellurium nanowires were centrifuged by a centrifuge with a rotation speed of 5000rpm for 4min to recover the precipitate, and distilled water and anhydrous ethanol were used for washing to remove by-products and excess cetyltrimethylammonium bromide, to obtain washed tellurium nanowire powder, and the washed tellurium nanowire powder was placed in a 50℃ vacuum drying oven for 10h to obtain tellurium nanowire powder.

[0063] It should be noted that ascorbic acid is a reducing agent, sodium tellurite is a tellurium source, and cetyltrimethylammonium bromide is an anionic surfactant.

[0064] The specific steps of the third method are as follows:

[0065] Sodium tellurite with a molar ratio of 3 mmol was dissolved in 30 ml of ethylene glycol, and the solution was stirred vigorously at a temperature of 120°C to obtain a colorless solution;

[0066] 0.3 g of sodium borohydride was dissolved in 30 ml of ethylene glycol to obtain a dissolved solution, and the dissolved solution was added dropwise to the colorless solution of sodium tellurite to obtain a mixture;

[0067] The mixture was refluxed at 280°C for 19 h to obtain tellurium nanorods;

[0068] The tellurium nanorods were precipitated with isopropyl alcohol to obtain a precipitate, which was centrifuged by a 5000 rpm centrifuge for 4 min to collect the precipitate, and the precipitate was washed with acetone to obtain a cleaned tellurium powder;

[0069] The cleaned tellurium powder was placed in a 50°C oven and baked for 11 h to obtain a tellurium nanowire powder.

[0070] The specific steps of the fourth method are as follows:

[0071] 0.1884 g of sodium tellurite and 0.942 g of polyvinylpyrrolidone were dissolved in 66 ml of deionized water, and a uniform solution was obtained under strong magnetic stirring at room temperature;

[0072] 3.3 ml of hydrazine hydrate and 6.7 ml of ammonia water were added to the uniform solution, and the solution was stirred to obtain a stirred solution;

[0073] The stirred solution was poured into a sealed reactor, and the reaction was carried out at 170°C for 3 h;

[0074] After the reaction was completed, the reaction product was cooled to room temperature, and the precipitate was recovered by centrifugation using a 5000 rpm centrifuge for 6 min to obtain a recovered precipitate, which was washed three times with deionized water and ethanol to remove by-products and excess raw materials, and the centrifugation was followed by 4 min ultrasonic cleaning to obtain a cleaned tellurium powder;

[0075] The cleaned tellurium powder was placed in a 50°C oven and baked for 11 h to obtain a tellurium nanowire powder.

[0076] Example 3

[0077] Please refer to Figure 2 , this embodiment provides a preparation process for a p-type thin film based on example 1, in this embodiment, the solvent thermal method and drop casting method are used for the preparation of the p-type thin film, in this embodiment, the method for preparing the tellurium nanowire powder by the solvent thermal method includes method one, method two, method three or method four;

[0078] The specific steps of the method one are as follows:

[0079] 1.75 g of sodium tellurite and 8.5 g of ascorbic acid powder are mixed in 160 mL of ethylene glycol solution and stirred for 0.5 h, after the solute is completely dissolved, a mixed solution is obtained, and the mixed solution is transferred to a 95℃ tetrafluoroethylene high-pressure reaction kettle with a stirring rate of 475 rpm for stirring reaction for 22 h;

[0080] After the reaction is completed, a reaction product is obtained, the reaction product is cooled to room temperature, and three times of centrifugal washing is performed in a centrifuge with a rotating speed of 6000 rpm for 5 min each time to remove by-products and excess raw materials, and ultrasonic cleaning is performed for 6 min after the centrifugation is completed;

[0081] After the ultrasonic cleaning is completed, a washed tellurium powder is obtained, and the washed tellurium powder is placed in a 60℃ oven for baking for 11 h to obtain a tellurium nanowire powder, which is recorded as A1.

[0082] The specific steps of the method two are as follows:

[0083] 5.5 g of ascorbic acid and 0.63 g of cetyltrimethylammonium bromide are dissolved in 200 ml of distilled water to obtain a clear solution;

[0084] 0.32 g of sodium tellurite powder is added to the solution, and the solution is stirred vigorously for 0.4 h to form a white suspension, the suspension is heated to 95℃ for reaction for 22 h to obtain a reaction mixture;

[0085] After the reaction mixture is cooled to room temperature, 125 ml of ethanol is added to the reaction mixture for precipitation to obtain tellurium nanowires;

[0086] The tellurium nanowires are centrifuged by a centrifuge with a rotating speed of 6000 rpm for 5 min to recover the precipitate, and the precipitate is washed with distilled water and anhydrous ethanol to remove by-products and excess cetyltrimethylammonium bromide, to obtain a washed tellurium nanowire powder, and the washed tellurium nanowire powder is placed in a 60℃ vacuum drying oven for drying for 11 h to obtain a tellurium nanowire powder, which is recorded as A2.

[0087] The specific steps of the method three are as follows:

[0088] Sodium tellurite with a molar ratio of 3.5 mmol is dissolved in 45 ml of ethylene glycol, and stirring is performed at a temperature of 130℃ to obtain a colorless solution;

[0089] 0.45 g of sodium borohydride is dissolved in 30 ml of ethylene glycol to obtain a dissolved solution, and the dissolved solution is added dropwise to the colorless solution of sodium tellurite to obtain a mixture;

[0090] The mixture is refluxed at 290℃ for 20h to obtain tellurium nanorods;

[0091] The tellurium nanorods are precipitated with isopropyl alcohol to obtain a precipitate, which is centrifuged by a 6000rpm centrifuge for 5min to collect the precipitate, and the tellurium powder is washed with acetone to obtain the washed tellurium powder;

[0092] The washed tellurium powder is placed in a 60℃ oven for baking for 12h to obtain the tellurium nanowire powder, which is denoted as A3.

[0093] The specific steps of Method Four are as follows:

[0094] 0.55g of sodium tellurite and 3g of polyvinylpyrrolidone are dissolved in 180ml of deionized water to obtain a uniform solution under strong magnetic stirring at room temperature;

[0095] 9.5ml of hydrazine hydrate and 22ml of ammonia water are added to the uniform solution and stirred to obtain a stirring solution;

[0096] The stirring solution is poured into a sealed reactor and reacted at 185℃ for 4h;

[0097] After the reaction is completed, the reaction product is cooled to room temperature and centrifuged by a 6000rpm centrifuge for 5min to recover the precipitate, which is washed with deionized water and ethanol three times to remove by-products and excess raw materials, and ultrasonic cleaning is performed for 6min after centrifugation to obtain the washed tellurium powder;

[0098] The washed tellurium powder is placed in a 60℃ oven for baking for 12h to obtain the tellurium nanowire powder, which is denoted as A4.

[0099] Example 4

[0100] Please refer to Figure 2 , this embodiment provides a preparation process of a p-type thin film based on Example 1, and in this embodiment, a solvent thermal method and a drop casting method are used to prepare the p-type thin film, and in this embodiment, the method for preparing the tellurium nanowire powder by the solvent thermal method includes Method One, Method Two, Method Three or Method Four;

[0101] The specific steps of Method One are as follows:

[0102] 2g of sodium tellurite and 10g of ascorbic acid powder are mixed in 200ml of ethylene glycol solution and stirred for 0.8h, and after the solute is completely dissolved, a mixed solution is obtained, which is transferred to a 100℃ tetrafluoroethylene high-pressure reaction kettle with a stirring rate of 500rpm for 24h of stirring reaction;

[0103] After the reaction is completed, the reaction product is obtained, the reaction product is cooled to room temperature, and three centrifugal washings are carried out in a centrifuge with a rotation speed of 7000 rpm for 6 min each time to remove by-products and excess raw materials. After the centrifugation is completed, ultrasonic cleaning is carried out for 8 min;

[0104] After the ultrasonic cleaning is completed, the washed tellurium powder is obtained, the washed tellurium powder is placed in a 70°C oven for baking for 12 h, and the tellurium nanowire powder is obtained, which is denoted as B1.

[0105] The specific steps of the second method are as follows:

[0106] 10 g of ascorbic acid and 1 g of cetyltrimethylammonium bromide are dissolved in 400 ml of distilled water to obtain a clear solution;

[0107] 0.52 g of sodium tellurite powder is added to the solution, and the solution is stirred vigorously for 0.5 h to form a white suspension. The suspension is heated to 100°C for a reaction of 24 h to obtain a reaction mixture;

[0108] After the reaction mixture is cooled to room temperature, 200 ml of ethanol is added to the reaction mixture for precipitation to obtain tellurium nanowires;

[0109] The tellurium nanowires are centrifuged by a centrifuge with a rotation speed of 7000 rpm for 6 min to recover the precipitate, and distilled water and anhydrous ethanol are used for washing to remove by-products and excess cetyltrimethylammonium bromide. The washed tellurium nanowire powder is obtained, and the washed tellurium nanowire powder is placed in a 70°C vacuum drying oven for drying for 12 h to obtain the tellurium nanowire powder, which is denoted as B2.

[0110] The specific steps of the third method are as follows:

[0111] Sodium tellurite with a molar ratio of 4 mmol is dissolved in 60 ml of ethylene glycol, and the solution is stirred vigorously at a temperature of 140°C to obtain a colorless solution;

[0112] 0.6 g of sodium borohydride is dissolved in 40 ml of ethylene glycol to obtain a dissolved solution, and the dissolved solution is added dropwise to the colorless solution of sodium tellurite to obtain a mixture;

[0113] The mixture is refluxed at 300°C for 21 h to obtain tellurium nanorods;

[0114] The tellurium nanorods are precipitated with isopropyl alcohol to obtain a precipitate, and the precipitate is collected by centrifugation by a centrifuge with a rotation speed of 7000 rpm for 6 min, and the washed tellurium powder is obtained by washing with acetone;

[0115] The washed tellurium powder is placed in a 70°C oven for baking for 13 h to obtain the tellurium nanowire powder, which is denoted as B3.

[0116] The specific steps of Method Four are as follows:

[0117] 0.942 g of sodium tellurite and 5 g of polyvinylpyrrolidone were dissolved in 330 ml of deionized water, and a uniform solution was obtained under strong magnetic stirring at room temperature;

[0118] 16.5 ml of hydrazine hydrate and 33.5 ml of ammonia water were added to the uniform solution, and stirring was performed to obtain a stirring solution;

[0119] The stirring solution was poured into a sealed reactor, and reaction was performed at 190°C for 5 h;

[0120] After the reaction was completed, the reaction product was cooled to room temperature, and a 7000 rpm centrifuge was used to centrifuge for 6 min to recover the precipitate, thereby obtaining recovered precipitate. The recovered precipitate was washed three times with deionized water and ethanol to remove byproducts and excess raw materials. After centrifugation, ultrasonic cleaning was performed for 8 min to obtain washed tellurium powder;

[0121] The washed tellurium powder was placed in a 70°C oven and baked for 13 h to obtain tellurium nanowire powder, which is denoted as B4.

[0122] Example 5

[0123] See Figure 3 , this embodiment provides a preparation process for a p-type tellurium thin film on the basis of Example 1. In this embodiment, the p-type tellurium thin film is prepared by a solvothermal method and a drop casting method. The p-type tellurium thin film is prepared by a drop casting method using the tellurium nanowire powder prepared in Example 3. The specific steps are as follows:

[0124] 0.26 g of the baked tellurium nanowire powder and 0.13 g of polyvinylidene fluoride powder were dissolved in 6 mL of N,N-dimethylformamide to obtain a mixed solution after stirring for 20 min;

[0125] The mixed solution was placed in an 18% power ultrasonic cell crusher for ultrasonic treatment for 30 min, with an ultrasonic interval of 1.6 s, to obtain a treatment liquid;

[0126] The treatment liquid was transferred to a glass sheet, and the glass sheet was placed on a heating plate at 60°C and baked for 1 h to obtain a p-type tellurium thin film.

[0127] Example 6

[0128] This embodiment provides a preparation process for a p-type tellurium thin film on the basis of Example 1. In this embodiment, the p-type tellurium thin film is prepared by a solvothermal method and a drop casting method. The p-type tellurium thin film is prepared by a drop casting method using the tellurium nanowire powder prepared in Example 4. The specific steps are as follows:

[0129] Take 0.39g of the dried tellurium nanowire powder and 0.195g of the polyvinylidene fluoride powder to form a nanocomposite solution in 9mL of N,N-dimethylformamide, stir for 30min to obtain a mixed solution;

[0130] Put the mixed solution into a 20% power ultrasonic cell crusher for 35min of ultrasonic treatment with an ultrasonic interval of 1.95s to obtain a treatment liquid;

[0131] Move the treatment liquid to a glass sheet and place the glass sheet on a heating plate at 70°C for 1.3h to obtain a p-type tellurium thin film.

[0132] Example 7

[0133] This example provides a process for preparing a p-type tellurium thin film based on Example 1. In this example, the p-type tellurium thin film is prepared using a solvothermal method and a drop casting method. The process for preparing a p-type tellurium thin film using the tellurium nanowire powder prepared in Example 5 by a drop casting method includes the following specific steps:

[0134] Take 0.52g of the dried tellurium nanowire powder and 0.26g of the polyvinylidene fluoride powder to form a nanocomposite solution in 12mL of N,N-dimethylformamide, stir for 40min to obtain a mixed solution;

[0135] Put the mixed solution into a 22% power ultrasonic cell crusher for 40min of ultrasonic treatment with an ultrasonic interval of 2.3s to obtain a treatment liquid;

[0136] Move the treatment liquid to a glass sheet and place the glass sheet on a heating plate at 80°C for 1.6h to obtain a p-type tellurium thin film.

[0137] Example 8

[0138] Please refer to Figure 3 , this example provides a process for preparing an n-type tellurium-based thin film based on Example 1, thereby realizing a flexible tellurium-based thin film with p-type tellurium-based thermoelectric units and n-type tellurium-based thermoelectric units arranged alternately on a single-layer p-type tellurium thin film. In this example, the n-type tellurium-based thin film is prepared using an in-situ reaction method. The process for preparing an n-type tellurium-based thin film using an in-situ reaction method, thereby realizing a flexible tellurium-based thin film with p-type tellurium-based thermoelectric units and n-type tellurium-based thermoelectric units arranged alternately on a single-layer p-type tellurium thin film includes the following specific steps:

[0139] Use a single-sided adhesive polyimide tape with a planar size of 25×75 mm 2 as a substrate to transfer the dried tellurium thin film from the glass sheet to the polyimide tape, obtaining a flexible p-type tellurium thin film with undoped polyimide tape as a substrate;

[0140] A single-sided adhesive polyimide tape with a planar size of 25x10 mm 2 was adhered at equal intervals on a p-type tellurium film with a planar size of 25x75 mm 2 as a substrate to obtain a tellurium film with completed adhesion;

[0141] It should be noted that the polyimide tape with a planar size of 25x10 mm 2 protects the surface of the adhered tellurium film from being eroded by the dopant;

[0142] 30 mL of silver nitrate with a concentration of 0.1 mol / L and 60 mL of ethylene glycol with a concentration of 98% were uniformly mixed to obtain a uniformly mixed solution of silver nitrate and ethylene glycol; the tellurium film with completed adhesion was immersed in the uniformly mixed solution of silver nitrate and ethylene glycol for in-situ reaction doping modification, and was left to stand for 12 h to obtain a silver-doped reaction film;

[0143] It should be noted that the volume ratio of silver nitrate to ethylene glycol is 2:1.

[0144] After sufficient reaction, the film was taken out and was subjected to cyclic flushing with ethanol for 15 min by using an ultrasonic machine, and the cycle was repeated three times to remove the excess raw materials and by-products on the surface of the film to obtain a cleaned film;

[0145] The cleaned film was placed in a vacuum drying oven at 55°C for 1 h to obtain a flexible tellurium-based film with p-type and n-type tellurium-based thermoelectric units arranged alternately.

[0146] Example 9

[0147] Please refer to Figure 1 and Figure 4 , this embodiment provides a preparation process of a wearable thermoelectric generator based on Example 1. In this embodiment, a bending and folding and packaging technology is used to prepare a wearable thermoelectric generator with high stretchability. The specific steps are as follows:

[0148] The p-type and n-type tellurium-based thermoelectric units arranged alternately on the film were coated with silver glue at both ends, and silver wires were used as electrodes to obtain a film with p-type and n-type tellurium-based thermoelectric units arranged alternately connected by electrodes;

[0149] The polydimethylsiloxane main agent and the curing agent were completely mixed at a mass ratio of 10:1 to prepare a polydimethylsiloxane precursor;

[0150] The thin film with p-type tellurium-based thermoelectric units and n-type tellurium-based thermoelectric units arranged alternately is curved in a wavy structure along the pn junction, and after the bending is completed, the device is placed in a 3D printed mold, polydimethylsiloxane precursor is poured into the mold, and then the mold is placed in an oven at 65°C for 4h, so as to fix the shape and package the device;

[0151] The device with fixed shape and packaging is taken out of the 3D printed mold, and a wearable wavy structure thermoelectric generator with high stretchability is obtained.

[0152] The heat source of the wearable thermoelectric generator is the human wrist, a hot water cup or a computer heat sink.

[0153] In order to verify the effectiveness of the present application, Example 8 uses a flexible thin film with p-type and n-type tellurium-based thermoelectric units arranged alternately realized on a single layer of tellurium film, wherein the p-type is undoped tellurium thin film and the n-type is silver-doped tellurium-based thin film, which is called tellurium-silver thin film. The thermoelectric properties of the p-type and n-type tellurium-based thermoelectric thin film are tested at room temperature, and the results are shown in Figure 5 It can be seen that the Seebeck coefficient of the p-type tellurium thin film reaches 334 μV K -1 -1 , but due to the strong coupling between the Seebeck coefficient, electrical conductivity and thermal conductivity inherent in the thermoelectric figure of merit, the electrical conductivity of the p-type tellurium thin film is relatively low. When the p-type tellurium thin film is converted into a tellurium-silver thin film (mainly silver telluride is generated by reaction) in situ, the Seebeck coefficient changes from positive to negative (-106 μV K -1 -1 ) and is modified, and the electrical conductivity is also greatly improved. Finally, the power factor of the p-type and n-type tellurium-based thin film reaches 19.07 μW m -1 K -2 -1 and 25.99 μW m -1 K -2 , respectively.

[0154] The present application uses Example 9 to prepare a wearable wavy structure thermoelectric generator (TEG) using a thin film with p-type (tellurium thin film) and n-type (tellurium-silver thin film) tellurium-based thermoelectric units arranged alternately as a substrate, and the power generation performance of the TEG is characterized. The output characteristic measurement results are shown in Figure 6 and Figure 7 . The TEG consisting of N p-n pairs is referred to as TEG-Npn, and the TEG consisting of 3 p-n pairs is referred to as TEG-3pn. Figure 6 The power generation characteristic curve of TEG-3pn is shown, depicting the temperature difference (ΔT) range of the upper and lower surfaces of the wavy structure TEG from 10 K to 60 K. It is obvious that the output voltage and output power of the device are greatly enhanced with the increase of ΔT. Figure 7 The open-circuit voltage ( ), and the output power was calculated using the formula ) test was about 4.5 kQ. It can be seen that the open-circuit voltage of the prepared wave-shaped structure TEG-3pn reached 50.46 mV at a temperature difference of 60 K, and the maximum output power reached 140 nW. The open-circuit voltage and the temperature difference were linearly correlated, and the output power changed quadratically with the increase of the temperature difference. In addition, the scalable integration of the generator is crucial for increasing the energy output of the device, and here, the simple device preparation process facilitates the scalable manufacturing of TEG. The open-circuit voltage of the TEG can be significantly increased with the increase of the number of p-n pairs in series, especially at a higher temperature difference. Please refer to Figure 8 , when the number of p-n pairs in series is 5 pairs, the open-circuit voltage value at a temperature difference of 60 K is further improved to 78.1 mV.

[0155] In addition, the adjustment of the geometric parameters of the device is a simple method to improve the performance output of the thermoelectric generator, thereby further improving the scalability of the design of the thermoelectric generator according to the present application. By changing the height and area of the wave-shaped structure of the device respectively, the voltage variation measurement results at different temperature differences are shown in Figure 9 and Figure 10 . It can be seen that when the area of the device remains unchanged, the output voltage of the TEG increases with the increase of the height of the device, especially at a temperature difference of 60 K ( Figure 9 ). The significant change should be attributed to the actual temperature difference between the cold and hot ends of the device and the internal resistance of the device, which is determined by the thermoelectric properties and the geometric parameters of the thermoelectric unit. When the area of the device is changed (the length of the thermoelectric unit is the variable) under the condition that the height of the device is constant, the output voltage of the TEG remains basically unchanged at the same temperature difference, at which time it is indicated that the voltage output of the TEG is only related to the temperature difference between the cold and hot ends of the device ( Figure 10 ).

[0156] In order to improve the comfort and flexibility between the wearable electronic device and the human tissue, the TEG also needs to have good flexibility and stretchability, so as to adapt to complex movements (such as joint rotation) and at the same time minimize the high thermal resistance or discomfort between the wearable TEG and the skin due to air gap. The curing and packaging of the device by polydimethylsiloxane improve the flexibility and comfort of the device. By measuring the relative performance change of the wave-shaped structure TEG when bending and stretching, the fatigue resistance and stability of the TEG are verified. When the TEG withstands 1000 bending tests under the condition that the bending radius is 15 mm, the relative resistance change (AR / R0) and the relative voltage change (AU / U0) of the TEG remain relatively stable, and the change amplitudes are both less than 6%, which indicates that the designed wave-shaped structure TEG has good reliability and fatigue resistance ( Figure 11 ​Tensile cycling results show that after 1000 cycles at 80% strain, the ΔR / R0 and ΔU / U0 of the TEG of this invention remain relatively stable. Figure 12 It is worth noting that the wave-shaped TEG structure of this invention can be easily stretched to over 300%. Figure 13 and Figure 14 This demonstrates extremely high stretchability.

[0157] To verify the practical application potential of this invention, the actual electrical output performance of the TEG was tested under different wearing conditions. When the ambient temperature was 22°C, the maximum open-circuit voltage measured by a multimeter when directly wearing the TEG-4pn was 9.5 mV. Meanwhile, the actual electrical output performance of the device was related to the wearer's movement state; the maximum output voltage reached 11.82 mV and 13.17 mV when the wearer was sitting and walking, respectively. Figure 15 Furthermore, to maximize comfort and output performance when worn by the human body, this invention uses the same length and width (25×128 mm) 2 A single-layer tellurium thin film with alternating p-type and n-type tellurium-based thermoelectric units was used. The width of these thermoelectric units was shortened from 10 mm to 6 mm, increasing the number of tandem pn pairs from 4 to 8 pairs (TEG-8pn). The results are as follows: Figure 16 As shown in the illustration, under the same ambient temperature, the maximum open-circuit voltage of the TEG-8pn, measured by a multimeter, reached 12.5 mV, approximately 3 mV higher than that of the TEG-4pn. Similarly, under the same conditions, its maximum open-circuit voltage while sitting and walking increased by approximately 4 mV and 5 mV respectively compared to the TEG-4pn. Figure 16 ).

[0158] This invention can also harvest energy from household heat sources (such as hot water cups). When TEG-4pn and TEG-8pn are installed on hot water cups at 70°C, the voltage test results are as follows... Figure 17 As shown, compared to TEG-4pn, TEG-8pn exhibits a significantly increased maximum open-circuit voltage under high temperature difference, reaching 90.7 mV. However, it should be noted that the voltage of TEG-8pn decays more rapidly after reaching its maximum value, due to its shorter height. The voltage of TEG-8pn reaches thermal equilibrium and stabilizes after approximately 20 seconds. In conclusion, this invention can effectively collect thermal energy in various scenarios, demonstrating its enormous potential in the field of wearable electronic devices.

[0159] In the description of the present specification, the description of the terms "one embodiment", "some embodiments", "an example", "a specific example", or "some examples" and the like means that the specific features, structures, materials or characteristics described in connection with the embodiment or example are included in at least one embodiment or example of the present application. In the present specification, the illustrative expressions of the above terms do not necessarily refer to the same embodiment or example. Furthermore, the specific features, structures, materials or characteristics described can be combined in any one or more embodiments or examples in a suitable manner.

[0160] The above-described embodiments only express several implementation manners of the present application, which are described in a more specific and detailed manner, but cannot be understood as a limitation on the patent scope of the present application. It should be noted that, for those of ordinary skill in the art, several modifications and improvements can be made without departing from the concept of the present application, which are all within the protection scope of the present application. Therefore, the protection scope of the patent of the present application should be subject to the appended claims.

Claims

1. A method for fabricating a wearable thermoelectric generator based on a flexible corrugated tellurium film, characterized in that, The method includes: Tellurium nanowire powder and polyvinylidene fluoride powder were dissolved in N,N-dimethylformamide solution to obtain a solution, and the solution was stirred to form a mixed solution. The mixed solution was subjected to ultrasonic treatment to obtain a treated solution; The treatment solution was transferred to a glass slide, and the glass slide was placed on a heating plate to dry, thus obtaining a dried p-type tellurium film. Using a single-sided adhered polyimide tape as a substrate, a dried p-type tellurium film was transferred from a glass slide onto the polyimide tape to obtain a flexible, undoped p-type tellurium film with the polyimide tape as a substrate. The polyimide tape, which is adhered to one side, is then adhered at equal intervals to a p-type tellurium film serving as a substrate to obtain a tellurium film that has been fully adhered. Silver nitrate and ethylene glycol are uniformly mixed to obtain a solution of silver nitrate and ethylene glycol. The adhering tellurium film is immersed in the solution of silver nitrate and ethylene glycol for in-situ reaction doping modification and left to stand overnight to obtain a silver-doped film. After the reaction is complete, the silver-doped film is taken out and rinsed to remove excess raw materials and by-products from the film surface, resulting in a cleaned film. The cleaned film is dried to obtain a flexible film with alternating p-type and n-type tellurium-based thermoelectric units; A flexible thin film with alternating p-type and n-type tellurium-based thermoelectric units is bent, folded, and encapsulated to obtain a wavy tellurium-based thin film. In a corrugated tellurium-based thin film, the exposed end of the pn junction of the thermoelectric generator is placed at the hot end, while the other end is placed in the air, so that the charge carriers of the p-type semiconductor and the n-type semiconductor migrate from the hot end to the cold end to generate a thermoelectric potential in a unified direction. By connecting the thermoelectric units that generate thermoelectric potential in series, a wearable thermoelectric generator is obtained.

2. The method for fabricating a wearable thermoelectric generator based on a flexible corrugated tellurium film according to claim 1, characterized in that, Tellurium nanowire powder is prepared using method one, method two, method three, or method four. The specific steps for preparing tellurium nanowire powder using Method 1 are as follows: Sodium tellurite and ascorbic acid powder were mixed in ethylene glycol solution and stirred until the solutes were completely dissolved to obtain a mixture. The mixture was then transferred to a polytetrafluoroethylene high-pressure reactor and stirred for reaction. After the reaction is complete, the reaction product is obtained. The reaction product is cooled to room temperature and centrifuged in a centrifuge to recover the precipitate. The product is washed three times with deionized water and ethanol to remove by-products and excess raw materials. After centrifugation, the product is ultrasonically cleaned. After ultrasonic cleaning, the cleaned tellurium powder is obtained. The cleaned tellurium powder is then placed in an oven and baked to obtain tellurium nanowire powder. The specific steps for preparing tellurium nanowire powder using method two are as follows: Ascorbic acid and hexadecyltrimethylammonium bromide were dissolved in distilled water to obtain a clear solution; Sodium tellurite was added to the solution and stirred vigorously to form a white suspension. The suspension was then heated to carry out the reaction to obtain the reaction mixture. After cooling the reaction mixture to room temperature, ethanol was added to the reaction mixture to precipitate tellurium nanowires. The tellurium nanowires were centrifuged to recover the precipitate, and then washed with distilled water and anhydrous ethanol to remove byproducts and excess hexadecyltrimethylammonium bromide, resulting in clean tellurium nanowire powder. The clean tellurium nanowire powder was then placed in a vacuum drying oven for drying to obtain tellurium nanowire powder. The specific steps for preparing tellurium nanowire powder using method three are as follows: Sodium tellurite was dissolved in ethylene glycol and stirred vigorously to obtain a colorless solution; Sodium borohydride was dissolved in ethylene glycol to obtain a solution, and the solution was added dropwise to a colorless sodium tellurite solution to obtain a mixture. The mixture was refluxed to obtain tellurium nanorods; Tellurium nanorods were precipitated with isopropanol to obtain a precipitate, which was then collected by centrifugation. The collected precipitate was then washed with acetone to obtain cleaned tellurium powder. The washed tellurium powder was placed in an oven and baked overnight to obtain tellurium nanowire powder; The specific steps for preparing tellurium nanowire powder using method four are as follows: Sodium tellurite and polyvinylpyrrolidone were dissolved in deionized water and a homogeneous solution was obtained under strong magnetic stirring at room temperature. Add hydrazine hydrate and ammonia to a homogeneous solution and stir to obtain a stirred solution; The stirred solution is poured into a sealed reactor to carry out the reaction; After the reaction is complete, the reaction product is obtained. The reaction product is cooled to room temperature and centrifuged to recover the precipitate. The recovered precipitate is washed three times with deionized water and ethanol to remove by-products and excess raw materials. After centrifugation, ultrasonic cleaning is performed to obtain cleaned tellurium powder. The washed tellurium powder was baked in an oven overnight to obtain tellurium nanowire powder.

3. The method for fabricating a wearable thermoelectric generator based on a flexible corrugated tellurium film according to claim 2, characterized in that, In the process of preparing tellurium nanowire powder using Method 1, sodium tellurite is used as the tellurium source, ascorbic acid is used as the reducing agent, and ethylene glycol is used as the reaction solvent and weak reducing agent. The mass of sodium tellurite and ascorbic acid powder is 1.5g-2.0g and 7.5g-10g respectively, the volume of ethylene glycol is 120mL-200mL, and the magnetic stirring time is 0.3h-0.8h. The reaction temperature set in the polytetrafluoroethylene high-pressure reactor is 90℃~100℃, the reaction time is 20h~24h, and the stirring speed is 450rpm~500rpm. The centrifuge speed is 5000rpm~7000rpm, the centrifugation time is 4 min~6 min, and the cleaning time in the ultrasonic cleaner is 4 min~8 min; Set the oven temperature to 50℃~70℃ and the baking time to 10h~12h; In the process of preparing tellurium nanowire powder using method two, ascorbic acid is used as a reducing agent, sodium tellurite is used as a tellurium source, and hexadecyltrimethylammonium bromide is used as an anionic surfactant. The mass of ascorbic acid is 1g to 10g, the mass of hexadecyltrimethylammonium bromide is 0.1g to 1g, the mass of sodium tellurite is 0.052g to 0.52g, the volume of distilled water is 40mL to 400mL, and the stirring time is 0.2h to 0.5h. The suspension is heated at 90℃~100℃, and the reaction time is 20h~24h; The volume of ethanol added for precipitation is 50 mL to 200 mL, the centrifuge speed is 5000 rpm to 7000 rpm, and the centrifugation time is 4 min to 6 min. The oven temperature is 50℃~70℃, and the baking time is 10h~12h; In the process of preparing tellurium nanowire powder using method three, the molar mass of sodium tellurite is 3 mmol to 4 mmol, and the temperature at which sodium tellurite is dissolved in ethylene glycol and vigorously stirred is 120℃ to 140℃. The mass of sodium borohydride is 0.3g to 0.6g, and the volume of ethylene glycol used for dissolving it is 20 mL to 40 mL. The mixture was refluxed at a temperature of 280℃~300℃ for 19h~21h. The centrifuge speed was set to 5000 rpm to 7000 rpm, and the centrifugation time was 4 min to 6 min. The oven temperature is 50℃~70℃, and the baking time is 11h~13h; In the process of preparing tellurium nanowire powder using method four, hydrazine hydrate is used as a reducing agent and polyvinylpyrrolidone is used as a surfactant. The mass of sodium tellurite is 0.1884 g to 0.942 g, the mass of polyvinylpyrrolidone is 1 g to 5 g, and the volume of deionized water is 66 mL to 330 mL. When adding hydrazine hydrate and ammonia water to a homogeneous solution, the volume of hydrazine hydrate added is 3.3 mL to 16.5 mL, and the volume of ammonia water added is 6.7 mL to 33.5 mL. The reaction temperature of the stirred solution poured into the sealed reactor is 170℃~190℃, and the reaction time is 3h~5h; The centrifuge speed is 5000rpm~7000rpm, the centrifugation time is 4 min~6 min, and the cleaning time in the ultrasonic cleaner is 4 min~8 min; The oven temperature is 50℃~70℃, and the baking time is 11h~13h.

4. The method for fabricating a wearable thermoelectric generator based on a flexible corrugated tellurium film according to claim 3, characterized in that, In the process of preparing p-type tellurium thin films, the mass of tellurium powder and polyvinylidene fluoride is 0.26g~0.52g and 0.13g~0.26g respectively, the volume of N,N-dimethylformamide is 6mL~12mL, and the magnetic stirring time is 20min~40min. The power of the ultrasonic cell disruptor is 18%–22%, the ultrasonic interval is 1.6s–2.3s, and the ultrasonic time is 30min–40min. The heating plate is set to a temperature of 60℃~80℃, and the baking time is 1h~1.6h.

5. The method for fabricating a wearable thermoelectric generator based on a flexible corrugated tellurium film according to claim 4, characterized in that, In the process of using single-sided adhered polyimide tape as a substrate, the polyimide tape and the glass slide have the same dimensions, with a planar size of 25 × 75 mm. 2 ; During the process of adhering single-sided polyimide tape to a p-type tellurium film as a substrate at equal intervals, the planar dimensions of the polyimide tape are 25 × 10 mm. 2 ; In the preparation of p-type tellurium thin films, the volume ratio of silver nitrate solution to ethylene glycol solution is 2~5:1, the reaction temperature is room temperature, and the reaction time is 11h~14h. The ultrasonic cleaning time is 10-20 minutes, the vacuum drying oven is set at 50℃-60℃, and the drying time is 1-3 hours.

6. The method for fabricating a wearable thermoelectric generator based on a flexible corrugated tellurium film according to claim 5, characterized in that, A flexible thin film with alternating p-type and n-type tellurium-based thermoelectric units is bent, folded, and encapsulated to obtain a wavy tellurium-based thin film. The specific steps include: Silver paste was applied to both ends of a film with alternating p-type and n-type tellurium-based thermoelectric units after drying, and silver wires were used as electrodes to obtain a film with electrodes connected to alternating p-type and n-type tellurium-based thermoelectric units. The polydimethylsiloxane main agent and the curing agent are completely mixed at a mass ratio of 10:1 to prepare the polydimethylsiloxane precursor; A thin film with alternating p-type and n-type tellurium thermoelectric units connected to electrodes is bent in a wavy structure along the pn junction. After bending, it is placed in a 3D printed mold, and polydimethylsiloxane precursor is poured into the mold to fix the shape and encapsulate it, thus obtaining a device with a fixed shape and encapsulation. The device, whose shape is fixed and encapsulated, is removed from the 3D-printed mold to obtain a wearable wave-shaped thermoelectric generator with high stretchability.

7. The method for fabricating a wearable thermoelectric generator based on a flexible corrugated tellurium film according to claim 6, characterized in that, The heat source for wearable thermoelectric generators can be the human wrist, a hot water cup, or a computer heat sink.

8. A wearable thermoelectric generator based on a flexible corrugated tellurium film, characterized in that, The wearable thermoelectric generator is prepared using the method for preparing a wearable thermoelectric generator based on a flexible corrugated tellurium film as described in any one of claims 1-7. The wearable thermoelectric generator includes: a p-type tellurium thin film and an n-type tellurium-based thin film. Both the p-type tellurium thin film and the n-type tellurium-based thin film are made of a single layer of tellurium film, and the p-type tellurium-based thermoelectric units and the n-type tellurium-based thermoelectric units are arranged alternately to form the p-type tellurium thin film and the n-type tellurium-based thin film. A corrugated tellurium-based thin film is obtained by bending, folding and encapsulating a flexible thin film with alternating p-type and n-type tellurium-based thermoelectric units. In a corrugated tellurium-based thin film, the exposed end of the pn junction of the thermoelectric generator is placed at the hot end, while the other end is placed in the air, so that the charge carriers of the p-type semiconductor and the n-type semiconductor migrate from the hot end to the cold end to generate a thermoelectric potential in a unified direction. By connecting the thermoelectric units that generate thermoelectric potential in series, a wearable thermoelectric generator is obtained.

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