The thermoelectric effect, which converts waste heat into electricity, holds promise as a renewable energy technology. Recently, bismuth telluride (Bi2Te3)-based alloys are being recognized as important materials for practical applications in the temperature range from room temperature to 500 K. However, conventional sintering processes impose limitations on shape-changeable and tailorable Bi2Te3 materials. To overcome these issues, three-dimensional (3D) printing (additive manufacturing) is being adopted. Although some research results have been reported, relatively few studies on 3D printed thermoelectric materials are being carried out. In this study, we utilize extrusion 3D printing to manufacture n-type Bi_1.7Sb_0.3Te₃ (N-BST). The ink is produced without using organic binders, which could negatively influence its thermoelectric properties. Furthermore, we introduce graphene oxide (GO) at the crystal interface to enhance the electrical properties. The formed N-BST composites exhibit significantly improved electrical conductivity and a higher Seebeck coefficient as the GO content increases. Therefore, we propose that the combination of the extrusion 3D printing process (Direct Ink Writing, DIW) and the incorporation of GO into N-BST offers a convenient and effective approach for achieving higher thermoelectric efficiency.

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• Exploring Thermoelectric Transport Properties and Band Parameters of n-Type Bi2-xSbxTe3 Compounds Using the Single Parabolic Band Model
  Linh Ba Vu, Soo-ho Jung, Jinhee Bae, Jong Min Park, Kyung Tae Kim, Injoon Son, Seungki Jo
  journal of Korean Powder Metallurgy Institute.2024; 31(2): 119.     CrossRef

We fabricate fine (<20 μm) powders of Bi_0.5Sb_1.5Te₃ alloys using a large-scale production method and subsequently consolidate them at temperatures of 573, 623, and 673 K using a spark plasma sintering process. The microstructure, mechanical properties, and thermoelectric properties are investigated for each sintering temperature. The microstructural features of both the powders and bulks are characterized by scanning electron microscopy, and the crystal structures are analyzed by X-ray diffraction analysis. The grain size increases with increasing sintering temperature from 573 to 673 K. In addition, the mechanical properties increase significantly with decreasing sintering temperature owing to an increase in grain boundaries. The results indicate that the electrical conductivity and Seebeck coefficient (217 μV/K) of the sample sintered at 673 K increase simultaneously owing to decreased carrier concentration and increased mobility. As a result, a high ZT value of 0.92 at 300 K is achieved. According to the results, a sintering temperature of 673 K is preferable for consolidation of fine (<20 μm) powders.

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• Complex microstructure induced high thermoelectric performances of p-type Bi–Sb–Te alloys
  Eun-Ha Go, Babu Madavali, Min-Woo Shin, Sung Ho Song, Soon-Jik Hong
  Materials Chemistry and Physics.2023; 307: 128156.     CrossRef
• Role of sintering temperature on electronic and mechanical properties of thermoelectric material: A theoretical and experimental study of TiCoSb half-Heusler alloy
  Ajay Kumar Verma, Kishor Kumar Johari, Kriti Tyagi, Durgesh Kumar Sharma, Pawan Kumar, Sudhir Kumar, Sivaiah Bathula, S.R. Dhakate, Bhasker Gahtori
  Materials Chemistry and Physics.2022; 281: 125854.     CrossRef
• Enhanced thermoelectric properties of Li and Mg co−substituted Bi2Sr2Co2O fabricated by combined conventional sintering and spark plasma sintering
  K. Park, H.Y. Hong, S.Y. Gwon
  Inorganic Chemistry Communications.2022; 145: 110005.     CrossRef

Graphene oxide (GO) powder processed by Hummer's method is mixed with p-type Bi₂Te₃ based thermoelectric materials by a high-energy ball milling process. The synthesized GO-dispersed p-type Bi₂Te₃ composite powder has a composition of Bi_0.5Sb_1.5Te₃ (BSbT), and the powder is consolidated into composites with different contents of GO powder by using the spark plasma sintering (SPS) process. It is found that the addition of GO powder significantly decreases the thermal conductivity of the pure BSbT material through active phonon scattering at the newly formed interfaces. In addition, the electrical properties of the GO/BSbT composites are degraded by the addition of GO powder except in the case of the 0.1 wt% GO/BSbT composite. It is found that defects on the surface of GO powder hinder the electrical transport properties. As a result, the maximum thermoelectric performance (ZT value of 0.91) is achieved from the 0.1% GO/BSbT composite at 398 K. These results indicate that introducing GO powder into thermoelectric materials is a promising method to achieve enhanced thermoelectric performance due to the reduction in thermal conductivity.

Citations

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• Nanocomposite Strategy toward Enhanced Thermoelectric Performance in Bismuth Telluride
  Hua‐Lu Zhuang, Jincheng Yu, Jing‐Feng Li
  Small Science.2025;[Epub]     CrossRef
• Exploring Thermoelectric Transport Properties and Band Parameters of n-Type Bi2-xSbxTe3 Compounds Using the Single Parabolic Band Model
  Linh Ba Vu, Soo-ho Jung, Jinhee Bae, Jong Min Park, Kyung Tae Kim, Injoon Son, Seungki Jo
  journal of Korean Powder Metallurgy Institute.2024; 31(2): 119.     CrossRef
• Enhancing Electrical Properties of N-type Bismuth Telluride Alloys through Graphene Oxide Incorporation in Extrusion 3D Printing
  Jinhee Bae, Seungki Jo, Kyung Tae Kim
  journal of Korean Powder Metallurgy Institute.2023; 30(4): 318.     CrossRef
• Advancement of thermoelectric performances through the dispersion of expanded graphene on p-type BiSbTe alloys
  Eun-Ha Go, Rathinam Vasudevan, Babu Madavali, Peyala Dharmaiah, Min-Woo Shin, Sung Ho Song, Soon-Jik Hong
  Powder Metallurgy.2023; 66(5): 722.     CrossRef
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  Young Min Cho, Kyung Tae Kim, Gi Seung Lee, Soo Hyung Kim
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• The Preparation and Growth Mechanism of the Recovered Bi2Te3 Particles with Respect to Surfactants
  Hyeongsub So, Eunpil Song, Yong-Ho Choa, Kun-Jae Lee
  Journal of Korean Powder Metallurgy Institute.2017; 24(2): 141.     CrossRef

Bi2Te3 related compounds show the best thermoelectric properties at room temperature. However, n-type Bi2Te2.7Se0.3 showed no improvement on ZT values. To improve the thermolectric propterties of n-type Bi2Te2.7Se0.3, this research has Cu-doped n-type powder. This study focused on effects of Cu-doping method on the thermoelectric properties of n-type materials, and evaluated the comparison between the Cu chemical and mechanical doping. The synthesized powder was manufactured by the spark plasma sintering(SPS). The thermoelectric properties of the sintered body were evaluated by measuring their Seebeck coefficient, electrical resistivity, thermal conductivity, and hall coefficient. An introduction of a small amount of Cu reduced the thermal conductivity and improved the electrical properties with Seebeck coefficient. The authors provided the optimal concentration of Cu_0.1Bi_1.99Se_0.3Te_2.7. A figure of merit (ZT) value of 1.22 was obtained for Cu_0.1Bi_1.9Se_0.3Te_2.7 at 373K by Cu chemical doping, which was obviously higher than those of Cu_0.1Bi_1.9Se_0.3Te_2.7 at 373K by Cu mechanical doping (ZT=0.56) and Cu-free Bi₂Se_0.3Te_2.7 (ZT=0.51).