State Key Laboratory of Advanced Technology for Materials Synthesis and Processing , Wuhan University of Technology , Wuhan 430070 , China.
Department of Materials Science and Engineering , University of Michigan , Ann Arbor , Michigan 48109 , United States.
ACS Appl Mater Interfaces. 2018 Aug 1;10(30):25519-25528. doi: 10.1021/acsami.8b07255. Epub 2018 Jul 19.
MnTe compounds show great potential for thermoelectric applications in the intermediate temperature range (500-800 K) because of their large Seebeck coefficient and intrinsically low thermal conductivity. So far, the existing methods for the synthesis of MnTe compounds remain constrained to multistep processes that are time- and energy-intensive. Herein, we demonstrate ultrafast synthesis of high-density bulk MnTe compounds using a combination of self-propagating high-temperature synthesis (SHS) and plasma activated sintering. The entire synthesis and processing procedure takes less than 1 h. The thermodynamic consideration suggests that the SHS process includes two steps: (1) Mn + 2Te → MnTe + Q and (2) MnTe → MnTe + Te. With the heat released by step (1), the process moved in cycle and finished in a rather short time. The effect of extra Mn content on the structure and thermoelectric properties was investigated. There is some solubility limit of extra Mn in the MnTe compound. The extra Mn occupy interstitial sites, leading to a decrease of carrier concentration while enhancing Seebeck coefficient and decreasing thermal conductivity. Low-temperature heat capacity data indicates that the MnTe compound has a high effective mass of 8.34 m and a low Debye temperature of 186 K, which are beneficial for the large Seebeck coefficient and low thermal conductivity. Therefore, the maximum ZT value reaches 0.57 at 850 K for the MnTe compound.
MnTe 化合物由于其较大的塞贝克系数和本征低热导率,在中温范围(500-800K)显示出在热电应用方面的巨大潜力。到目前为止,MnTe 化合物的现有合成方法仍然局限于多步过程,这些过程既耗时又耗能。在此,我们展示了使用自蔓延高温合成(SHS)和等离子体激活烧结相结合的方法,在不到 1 小时的时间内快速合成高密度块状 MnTe 化合物。整个合成和加工过程不到 1 小时。热力学考虑表明,SHS 过程包括两个步骤:(1)Mn + 2Te → MnTe + Q;(2)MnTe → MnTe + Te。通过步骤(1)释放的热量,该过程以循环的方式进行,并在相当短的时间内完成。额外 Mn 含量对结构和热电性能的影响也进行了研究。MnTe 化合物中有一定的额外 Mn 溶解度极限。额外的 Mn 占据间隙位置,导致载流子浓度降低,同时提高了塞贝克系数并降低了热导率。低温热容数据表明,MnTe 化合物具有高的有效质量 8.34m 和低的德拜温度 186K,这有利于大的塞贝克系数和低的热导率。因此,MnTe 化合物在 850K 时的最大 ZT 值达到 0.57。