Zhang Jingwen, Li Song, Zhu Zhengyi, Wu Zhenwang, Zhang Jiuxing
School of Materials Science and Engineering, Hefei University of Technology, Hefei 230009, China.
Dalton Trans. 2021 Aug 4;50(30):10515-10523. doi: 10.1039/d1dt01725j.
SnTe is an emerging IV-VI metal chalcogenide, but its low Seebeck coefficient and high thermal conductivity mainly originating from the high hole concentration limit its thermoelectric performance. In this work, an amorphous carbon core-shell-coated PbTe nanostructure prepared by a "bottom-up" method is first incorporated into the Sn1-ySbyTe matrix to enhance the thermoelectric performance of SnTe. The square-like PbTe nanoparticles maintain their original cubic morphology and do not grow up obviously after the SPS process due to the coating of the C layer, bringing about the formation of nanopores locally, while Sb alloying induces Sb point defects and Sb-rich precipitates. All these unique hierarchical microstructures finally lead to an ultralow lattice thermal conductivity (∼0.48 W-1 m-1 K-1) approaching amorphous limits (∼0.40 W-1 m-1 K-1). In addition, the incorporation of PbTe@C core-shell nanostructures decreases the carrier mobility obviously with a slight loss in carrier concentration, resulting in the deterioration of electrical properties to a certain extent. As a result, a peak thermoelectric figure of merit (ZT) of 1.07 is achieved for Sn0.89Sb0.11Te-5%PbTe@C at 873 K, which is approximately 154.76% higher than that of pristine SnTe. This work provides a new strategy to enhance the thermoelectric performance of SnTe and also offers a new insight into other related thermoelectric systems.
SnTe是一种新兴的IV-VI族金属硫族化物,但其塞贝克系数低且热导率高,主要源于高空穴浓度,这限制了其热电性能。在这项工作中,首先将通过“自下而上”方法制备的非晶碳核壳包覆的PbTe纳米结构掺入Sn1-ySbyTe基体中,以提高SnTe的热电性能。由于C层的包覆,方形的PbTe纳米颗粒保持其原始的立方形态,在放电等离子烧结(SPS)过程后没有明显长大,导致局部形成纳米孔,而Sb合金化会诱导Sb点缺陷和富Sb沉淀。所有这些独特的分级微观结构最终导致超低的晶格热导率(约0.48W⁻¹m⁻¹K⁻¹)接近非晶极限(约0.40W⁻¹m⁻¹K⁻¹)。此外,PbTe@C核壳纳米结构的掺入明显降低了载流子迁移率,同时载流子浓度略有损失,导致电学性能在一定程度上恶化。结果,Sn0.89Sb0.11Te-5%PbTe@C在873K时实现了1.07的峰值热电优值(ZT),比原始SnTe高出约154.76%。这项工作为提高SnTe的热电性能提供了一种新策略,也为其他相关热电系统提供了新的见解。