The development of thermoelectric (TE) materials to replace Bi2Te3 alloys is emerging as a hot issue with the potential for wider practical applications. In particular, layered Zintl-phase materials, which can appropriately control carrier and phonon transport behaviors, are being considered as promising candidates. However, limited data have been reported on the thermoelectric properties of metal-Sb materials that can be transformed into layered materials through the insertion of cations. In this study, we synthesized FeSb and MnSb, which are used as base materials for advanced thermoelectric materials. They were confirmed as single-phase materials by analyzing X-ray diffraction patterns. Based on electrical conductivity, the Seebeck coefficient, and thermal conductivity of both materials characterized as a function of temperature, the zT values of MnSb and FeSb were calculated to be 0.00119 and 0.00026, respectively. These properties provide a fundamental data for developing layered Zintl-phase materials with alkali/alkaline earth metal insertions.

The n-type Bi2-xSbxTe3 compounds have been of great interest due to its potential to achieve a high thermoelectric performance, comparable to that of p-type Bi2-xSbxTe3. However, a comprehensive understanding on the thermoelectric properties remains lacking. Here, we investigate the thermoelectric transport properties and band characteristics of n-type Bi2-xSbxTe3 (x = 0.1 – 1.1) based on experimental and theoretical considerations. We find that the higher power factor at lower Sb content results from the optimized balance between the density of state effective mass and nondegenerate mobility. Additionally, a higher carrier concentration at lower x suppresses bipolar conduction, thereby reducing thermal conductivity at elevated temperatures. Consequently, the highest zT of ~ 0.5 is observed at 450 K for x = 0.1 and, according to the single parabolic band model, it could be further improved by ~70 % through carrier concentration tuning.

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 Bi1.7Sb0.3Te3 (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.

High-temperature and high-pressure post-processing applied to sintered thermoelectric materials can create nanoscale defects, thereby enhancing their thermoelectric performance. Here, we investigate the effect of hot isostatic pressing (HIP) as a post-processing treatment on the thermoelectric properties of p-type Bi0.5Sb1.5Te3.0 compounds sintered via spark plasma sintering. The sample post-processed via HIP maintains its electronic transport properties despite the reduced microstructural texturing. Moreover, lattice thermal conductivity is significantly reduced owing to activated phonon scattering, which can be attributed to the nanoscale defects created during HIP, resulting in an ~18% increase in peak zT value, which reaches ~1.43 at 100oC. This study validates that HIP enhances the thermoelectric performance by controlling the thermal transport without having any detrimental effects on the electronic transport properties of thermoelectric materials.