Deng Rigui, Su Xianli, Zheng Zheng, Liu Wei, Yan Yonggao, Zhang Qingjie, Dravid Vinayak P, Uher Ctirad, Kanatzidis Mercouri G, Tang Xinfeng
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China.
Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.
Sci Adv. 2018 Jun 1;4(6):eaar5606. doi: 10.1126/sciadv.aar5606. eCollection 2018 Jun.
Several prominent mechanisms for reduction in thermal conductivity have been shown in recent years to improve the figure of merit for thermoelectric materials. Such a mechanism is a hierarchical all-length-scale architecturing that recognizes the role of all microstructure elements, from atomic to nano to microscales, in reducing (lattice) thermal conductivity. In this context, there have been recent claims of remarkably low (lattice) thermal conductivity in BiSbTe that are attributed to seemingly ordinary grain boundary dislocation networks. These high densities of dislocation networks in BiSbTe were generated via unconventional materials processing with excess Te (which formed liquid phase, thereby facilitating sintering), followed by spark plasma sintering under pressure to squeeze out the liquid. We reproduced a practically identical microstructure, following practically identical processing strategies, but with noticeably different (higher) thermal conductivity than that claimed before. We show that the resultant microstructure is anisotropic, with notable difference of thermal and charge transport properties across and along two orthonormal directions, analogous to anisotropic crystals. Thus, we believe that grain boundary dislocation networks are not the primary cause of enhanced through reduction in thermal conductivity. Instead, we can reproduce the purported high through a favorable but impractical and incorrect combination of thermal conductivity measured along the pressing direction of anisotropy while charge transport measured in the direction perpendicular to the anisotropic direction. We believe that our work underscores the need for consistency in charge and thermal transport measurements for unified and verifiable measurements of thermoelectric (and related) properties and phenomena.
近年来,已经发现了几种降低热导率的重要机制,以提高热电材料的品质因数。这样一种机制是一种层次化的全长度尺度结构设计,它认识到从原子尺度到纳米尺度再到微米尺度的所有微观结构元素在降低(晶格)热导率方面的作用。在这种背景下,最近有报道称,BiSbTe中的(晶格)热导率极低,这归因于看似普通的晶界位错网络。BiSbTe中这些高密度的位错网络是通过非常规材料加工产生的,即加入过量的Te(形成液相,从而促进烧结),然后在压力下进行放电等离子烧结以挤出液体。我们遵循几乎相同的加工策略,复制出了几乎相同的微观结构,但热导率明显不同(更高),与之前报道的不同。我们表明,所得的微观结构是各向异性的,在两个正交方向上的热传输和电荷传输特性存在显著差异,类似于各向异性晶体。因此,我们认为晶界位错网络不是通过降低热导率来提高品质因数的主要原因。相反,我们可以通过在各向异性的压制方向上测量热导率,同时在垂直于各向异性方向上测量电荷传输,以一种有利但不切实际且不正确的组合来重现所谓的高品质因数。我们认为,我们的工作强调了在热电(及相关)性质和现象的统一且可验证的测量中,电荷传输和热传输测量一致性的必要性。