The flexible thermoelectric energy conversion technology can convert the environment or human body temperature difference into electrical energy to realize the self-power supply of electronic devices, and has broad application prospects in wearable and other fields. Traditional inorganic thermoelectric materials have excellent thermoelectric properties, but do not have flexible functions; while organic thermoelectric materials have good flexibility and bending properties, but the thermoelectric properties are extremely low. Organic/inorganic composite thermoelectric materials can integrate the thermoelectric performance of inorganic materials and the good bending properties of organic materials, and have become a research hotspot in recent years. Carbon nanotubes or metal nanowires with a one-dimensional structure can form a tightly connected conductive network with one-dimensional molecular chains of organic materials, and provide highly conductive channels along the chain network, so they are often used in organic/inorganic composite thermoelectric materials. . However, the extremely low Zebeck coefficient of carbon nanotubes or metal nanowires makes it difficult to increase the Zebeck coefficient of composite materials. Although the inorganic thermoelectric material has a high Zebeck coefficient, its shape is usually in the form of flakes or particles, resulting in low electrical transport performance of the composite material. Therefore, how to select matching organic/inorganic materials to obtain good electrical transport has become a key scientific issue in the research of organic/inorganic composite thermoelectric materials. Recently, Shi Xun, Chen Lidong, Associate Researchers Qiu Pengfei, Qu Sanyin, etc., researchers at the Shanghai Institute of Ceramics, Chinese Academy of Sciences, and He Jian, a professor at Clemson University in the United States, proposed a new dimension matching thermoelectric composite design strategy Even using inorganic semiconductor materials that also have a one-dimensional structure to prepare high-performance PVDF/Ta4SiTe4 organic/inorganic flexible thermoelectric composite films, the normalized maximum power density of the prototype device at a temperature difference of 35.5K is the highest among the currently reported flexible thermoelectric devices value. Related research results are published in Energy & Environmental Science under the title of Conformal organic–inorganic semiconductor composites for flexible thermoelectrics. The organic material polyvinylidene fluoride (PVDF) has a one-dimensional chain structure and is an insulator with excellent flexibility. Based on the design idea of ​​dimensional matching, the team chose Ta4SiTe4 inorganic material which also has a one-dimensional structure and PVDF to prepare an organic/inorganic flexible composite film. Through the chemical vapor transport reaction, Ta4SiTe4 one-dimensional whiskers doped with 0.5% Mo in the Ta site were obtained. Then, using N,N-dimethylformamide (DMF) as a dispersant, PVDF/Ta4SiTe4 composite film was obtained by the method of drop coating. Scanning electron microscopy found that Ta4SiTe4 whiskers were evenly dispersed in the PVDF matrix to form a network structure. Transmission electron microscopy showed that Ta4SiTe4 whiskers and PVDF formed a tightly bonded two-phase interface. The thermoelectric performance characterization found that PVDF/50 wt% Ta4SiTe4 has excellent electrical transport performance, with a power factor as high as 1060 μWm-1K-2 at 220 K. In particular, at the same conductivity, the Zebeck coefficient of PVDF/50 wt% Ta4SiTe4 film is much higher than that of organic/inorganic composite films based on carbon nanotubes or metal nanowires. Ta4SiTe4's own semiconductor transport characteristics and one-dimensional structure jointly produce the above-mentioned excellent electrical transport performance. While achieving excellent electrical transport performance, the organic/inorganic composite film formed by dimensionally matched PVDF and Ta4SiTe4 also has good flexibility. After repeated bending 5000 times on a curved surface with a diameter of 9 mm, the PVDF/50 wt% Ta4SiTe4 film resistance did not change significantly. The research team preliminarily prepared a prototype thermoelectric device containing 4 PVDF/50 wt% Ta4SiTe4 thermocouples. At a temperature difference of 35.5K, the normalized maximum power density of the device reached 0.13 Wm-1, which is the current reported flexible thermoelectric device. The maximum value. The research work has received funding and support from the National Key R&D Project, the National Natural Science Foundation of China, the Youth Innovation Promotion Association of the Chinese Academy of Sciences, and the Shanghai Youth Science and Technology Star Project. Figure a) Schematic diagram of PVDF/Ta4SiTe4 flexible composite film. b) Comparison of thermoelectric properties between PVDF/Ta4SiTe4 composite film and the reported one-dimensional organic-inorganic composite film. c) Comparison of the normalized maximum power density of the PVDF/Ta4SiTe4-based prototype thermoelectric device and the reported flexible thermoelectric device.
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