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CN-121985722-A - High-flexibility silver telluride thermoelectric film with pearl scallop structure and preparation method and application thereof

CN121985722ACN 121985722 ACN121985722 ACN 121985722ACN-121985722-A

Abstract

The invention relates to the technical field of thermoelectric materials, in particular to a high-flexibility silver telluride thermoelectric film with a pearl scallop structure, and a preparation method and application thereof. The silver telluride thermoelectric film with the non-stoichiometric ratio and the pearl scallop structure is rapidly prepared through an intermittent co-sputtering process under the conditions of room temperature and fixed working air pressure, the mechanical property and the thermoelectric property of the silver telluride thermoelectric film are remarkably improved through the pearl scallop structure, the surface of the silver telluride thermoelectric film is free of cracks after 5000 times of bending circulation, the resistance is only increased by 20%, excellent flexibility is shown, meanwhile, the power factor can reach 51.92 mu W m ‑1 K ‑2 under the condition of room temperature, the good thermoelectric property is achieved, the requirements of flexible wearable thermoelectric devices are met, and the potential commercial application prospect is provided.

Inventors

  • FENG XIAOBIN
  • NIU GUOWEI
  • LI WENJUAN
  • Niu Yuanbin
  • DUAN BO
  • LI GUODONG
  • ZHAI PENGCHENG

Assignees

  • 武汉理工大学

Dates

Publication Date
20260505
Application Date
20260225

Claims (10)

  1. 1. A high-flexibility silver telluride thermoelectric film with a pearl scallop structure is characterized in that the pearl scallop structure comprises pearl-shaped silver grains and radial silver telluride grains at the center of the bottom, the silver telluride grains are radially distributed by taking the pearl-shaped silver grains as the center, radial rib-shaped crystal boundaries are formed between adjacent radial silver telluride grains in the pearl scallop structure, and heterogeneous interfaces are formed between the pearl-shaped silver grains and the radial silver telluride grains.
  2. 2. The high-flexibility silver telluride thermoelectric film with a pearl scallop structure according to claim 1, wherein the atomic percentage ratio of silver to tellurium is 1.9-2.3:1 in the components of the high-flexibility silver telluride thermoelectric film with the pearl scallop structure, the size of the pearl silver crystal grain is 100-400 nm, and the size of the radial silver telluride crystal grain is 40-85 nm.
  3. 3. The preparation method of the high-flexibility silver telluride thermoelectric film with the pearl scallop structure is characterized by comprising the following steps of: the pretreated substrate is fixed on a substrate, then the substrate is put into a sputtering cavity, a silver simple substance target is fixed on a direct current power supply, a tellurium simple substance target is fixed on a radio frequency power supply, and the substrate is prepared by adopting an intermittent magnetron co-sputtering method in one step.
  4. 4. The method for preparing the high-flexibility silver telluride thermoelectric film with the pearl scallop structure according to claim 3, wherein the power of the direct current power supply is 20-30W.
  5. 5. The method for preparing the high-flexibility silver telluride thermoelectric film with the pearl scallop structure according to claim 3, wherein the temperature of the intermittent magnetron co-sputtering is 20-30 ℃.
  6. 6. The method for preparing the high-flexibility silver telluride thermoelectric film with the pearl scallop structure according to claim 3, wherein the intermittent magnetron co-sputtering method comprises the steps of sputtering and depositing for 12-17 minutes, then turning off a power supply for 10-15 minutes, and repeating for 3-5 periods.
  7. 7. The method of claim 6, wherein the sputtering parameters include pumping the air pressure in the cavity to below 5×10 -4 Pa, setting the argon flow to 30-40 sccm, setting the working air pressure to 1-1.5 Pa, setting the substrate rotation speed to 10-20 rpm, and setting the pulse duty ratio to 70-90%.
  8. 8. The method for preparing a high-flexibility silver telluride thermoelectric film with a pearl scallop structure according to claim 3, wherein the purity of the silver simple substance and the tellurium simple substance are more than or equal to 99.9%.
  9. 9. The method for preparing the high-flexibility silver telluride thermoelectric film with the pearl scallop structure according to claim 3, wherein the substrate comprises polyimide, and the pretreatment comprises ultrasonic cleaning and drying of the substrate.
  10. 10. Use of a highly flexible silver telluride thermoelectric film having a pearl scallop structure according to claim 1 or 2 in the manufacture of a thermoelectric device product.

Description

High-flexibility silver telluride thermoelectric film with pearl scallop structure and preparation method and application thereof Technical Field The invention relates to the technical field of thermoelectric materials, in particular to a high-flexibility silver telluride thermoelectric film with a pearl scallop structure, and a preparation method and application thereof. Background With the development of wearable electronic devices, the development of sustainable miniature energy sources has become a leading-edge research hotspot. The wearable thermoelectric device is based on the Seebeck effect, can utilize the natural temperature difference between a human body and the environment to continuously generate power, and provides a unique solution for solving the cruising problem of equipment. The traditional rigid thermoelectric device has lower efficiency under small temperature difference, and is difficult to be tightly attached to a complex curved surface of a human body, so that larger contact thermal resistance is caused. Therefore, there is a great interest in thinning thermoelectric materials to construct flexible thermoelectric devices. Among the materials, silver telluride, as a narrow bandgap semiconductor, exhibits excellent thermoelectric potential due to its high carrier mobility and low lattice thermal conductivity. By precisely regulating the stoichiometric ratio, the effective optimization of the carrier concentration and type can be realized. Related researches show that the introduction of the nano second phase not only can regulate electric transport through energy band engineering, but also can construct a multi-scale strengthening mechanism in mechanical dimension. The nanometer second phase can effectively inhibit the destabilization and the expansion of cracks in a brittle matrix by inducing a plurality of synergistic toughening effects such as crack bridging, crack branching, crack deflection and the like. The microstructure design can improve the fracture toughness of the material, and has great significance for developing thermoelectric devices with high thermoelectric performance and high flexibility. However, the existing preparation methods of the silver telluride thermoelectric film are mainly focused on preparing silver telluride nanowires by a chemical mode, and then forming the film by vacuum auxiliary filtration, hot pressing and other modes, and the methods have the problems that the preparation process needs to be carried out in multiple steps and the flexibility of the prepared film is low, so that the industrial mass production and practical flexible application of the silver telluride film are limited. The magnetron sputtering method is adopted to prepare the film, which requires high temperature and post annealing treatment, and has long time and high energy consumption. Therefore, how to rapidly prepare the silver telluride thermoelectric film with excellent mechanical property and thermoelectric property at room temperature (20-30 ℃) in the next step is of great significance to develop the wearable thermoelectric device with high flexibility. Disclosure of Invention In view of the above, the invention provides a high-flexibility silver telluride thermoelectric film with a pearl scallop structure, and a preparation method and application thereof. Under the conditions of room temperature (20-30 ℃) and fixed air pressure, the polyimide is taken as a substrate, and the high-flexibility silver telluride thermoelectric film with the pearl scallop structure is rapidly prepared in one step by an intermittent magnetron co-sputtering method, so that the mechanical property and the thermoelectric property of the silver telluride thermoelectric film are remarkably improved, and particularly, the proportion of silver and tellurium elements in the film is regulated and controlled mainly by controlling the power of a direct-current power supply, and the silver and tellurium elements have remarkable influence on the microstructure of the pearl scallop. The technical scheme of the invention is realized as follows: In a first aspect, the invention provides a high-flexibility silver telluride thermoelectric film with a pearl scallop structure, wherein the pearl scallop structure is a bionic nano composite structure and comprises pearl-shaped silver grains and radial silver telluride grains at the center of the bottom, the silver telluride grains are radially distributed by taking the pearl-shaped silver grains as the center, radial rib grain boundaries are formed between adjacent radial silver telluride grains in the pearl scallop structure, and heterogeneous interfaces are formed between the pearl-shaped silver grains and the radial silver telluride grains. On the basis of the technical scheme, preferably, in the components of the high-flexibility silver telluride thermoelectric film with the pearl scallop structure, the atomic percentage ratio of silver to tellurium elements is 1.9-