Sauerschnig Philipp, Saitou Noriyuki, Koshino Masanori, Ishida Takao, Yamamoto Atsushi, Ohta Michihiro
Global Zero Emission Research Center, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8569, Japan.
Advanced Manufacturing Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8564, Japan.
ACS Appl Mater Interfaces. 2024 Sep 4;16(35):46421-46432. doi: 10.1021/acsami.4c07148. Epub 2024 Aug 2.
Nanostructured lead telluride PbTe is among the best-performing thermoelectric materials, for both p- and n-types, for intermediate temperature applications. However, the fabrication of power-generating modules based on nanostructured PbTe still faces challenges related to the stability of the materials, especially nanoprecipitates, and the bonding of electric contacts. In this study, in situ high-temperature transmission electron microscopy observation confirmed the stability of nanoprecipitates in p-type PbNaGeTe up to at least ∼786 K. Then, a new architecture for a packaged module was developed for improving durability, preventing unwanted interaction between thermoelectric materials and electrodes, and for reducing thermal stress-induced crack formation. Finite element method simulations of thermal stresses and power generation characteristics were utilized to optimize the new module architecture. Legs of nanostructured p-type PbNaGeTe (maximum ∼ 2.2 at 795 K) and nanostructured n-type PbGaTe (maximum ∼ 1.5 at 748 K) were stacked with flexible Fe-foil diffusion barrier layers and Ag-foil-interconnecting electrodes forming stable interfaces between electrodes and PbTe in the packaged module. For the bare module, a maximum conversion efficiency of ∼6.8% was obtained for a temperature difference of ∼480 K. Only ∼3% reduction in output power and efficiency was found after long-term operation of the bare module for ∼740 h (∼31 days) at a hot-side temperature of ∼673 K, demonstrating good long-term stability.
纳米结构碲化铅(PbTe)是用于中温应用的p型和n型最佳热电材料之一。然而,基于纳米结构PbTe的发电模块制造仍面临与材料稳定性相关的挑战,特别是纳米沉淀物以及电接触的键合。在本研究中,原位高温透射电子显微镜观察证实了p型PbNaGeTe中纳米沉淀物在至少约786 K的温度下具有稳定性。然后,开发了一种用于封装模块的新架构,以提高耐用性、防止热电材料与电极之间的不必要相互作用,并减少热应力引起的裂纹形成。利用热应力和发电特性的有限元方法模拟来优化新的模块架构。纳米结构的p型PbNaGeTe(在795 K时最大值约为2.2)和纳米结构的n型PbGaTe(在748 K时最大值约为1.5)的腿与柔性铁箔扩散阻挡层和银箔互连电极堆叠在一起,在封装模块中形成电极与PbTe之间的稳定界面。对于裸模块,在约480 K的温差下获得了约6.8%的最大转换效率。在约673 K的热侧温度下对裸模块进行约740小时(约31天)的长期运行后,发现输出功率和效率仅降低了约3%,表明具有良好的长期稳定性。