College of Materials Science and Engineering, Shenzhen Key Laboratory of Special Functional Materials, Guangdong Research Center for Interfacial Engineering of Functional Materials, Guangdong Provincial Key Laboratory of Deep Earth Sciences and Geothermal Energy Exploitation and Utilization, Institute of Deep Earth Sciences and Green Energy, Shenzhen University, Shenzhen 518060, China.
College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, China.
ACS Appl Mater Interfaces. 2023 Apr 19;15(15):19250-19257. doi: 10.1021/acsami.3c02586. Epub 2023 Apr 5.
Manipulating and integrating the microstructures at different scales is crucial to tune the electrical and thermal properties of a given compound. High-pressure sintering can modify the multiscale microstructures and thus empower the cutting-edge thermoelectric performance. In this work, the high-pressure sintering technique followed by annealing is adopted to prepare Gd-doped -type (BiSb)(TeSe) alloys. First, the high energy of high-pressure sintering promotes the reduction of grain size, thus increasing the content of 2D grain boundaries. Next, high-pressure sintering induces strong interior strain, where 1D dense dislocations are generated near the strain field. More interestingly, the rare-earth element Gd with a high melting temperature is dissolved into the matrix via high-pressure sintering, thus promoting the formation of 0D extrinsic point defects. This concurrently improves the carrier concentration and density-of-state effective mass, resulting in an enhanced power factor. In addition, the integrated 0D point defects, 1D dislocations, and 2D grain boundaries by high-pressure sintering strengthen phonon scattering, thereby achieving a low lattice thermal conductivity of 0.5 Wm K at 348 K. Consequently, a maximum value of ∼1.1 at 348 K is achieved in the 0.4 at % Gd-doped (BiSb)(TeSe) sample. This work demonstrates that high-pressure sintering enables microstructure modification to enhance the thermoelectric performance of BiTe-based and other bulk materials.
在不同尺度上操纵和整合微观结构对于调整给定化合物的电和热性能至关重要。高压烧结可以改变多尺度微观结构,从而赋予前沿的热电性能。在这项工作中,采用高压烧结技术结合退火来制备 Gd 掺杂的 -型(BiSb)(TeSe)合金。首先,高压烧结的高能量促进晶粒尺寸减小,从而增加 2D 晶界的含量。其次,高压烧结诱导强烈的内部应变,在应变场附近产生 1D 密集位错。更有趣的是,具有高熔点的稀土元素 Gd 通过高压烧结溶解到基体中,从而促进 0D 外点缺陷的形成。这同时提高了载流子浓度和态密度有效质量,从而提高了功率因子。此外,高压烧结形成的 0D 点缺陷、1D 位错和 2D 晶界增强了声子散射,从而在 348 K 时实现了低晶格热导率 0.5 Wm K。因此,在 0.4 at% Gd 掺杂(BiSb)(TeSe)样品中在 348 K 时实现了最大 值约为 1.1。这项工作表明,高压烧结能够通过改变微观结构来提高 BiTe 基和其他块状材料的热电性能。