The high performance of a multistage thermoelectric cooler (multi-TEC) used in a wide low-temperature range depends on the optimized thermoelectric (TE) performance of materials during the corresponding working temperature range for each stage. Despite decades of research on the commercial TE materials of Bi2Te3, the main research is still focused on temperatures above 300 K, lacking suitable hierarchical low-temperature n-Bi2Te3 for multistage TEC. In this work, we systematically investigated the influence of doping concentration and matrix material compositions on the TE performance of n-Bi2Te3 below room temperature by the high-energy ball milling and hot deformation. Consequently, two hierarchical n-Bi2Te3 materials with excellent mechanical properties working below 248 and around 298 K, respectively, have been screened out. The Bi2Te2.7Se0.3 + 0.03 wt % TeI4 can be adopted in a low-temperature range that exhibits the high average figure of merit (zTave) of 0.61 within 173-248 K. Meanwhile, the Bi2Te2.7Se0.3 + 0.05 wt % TeI4 sample displays a competitive zTave of 0.85 within 248-298 K, which can be applied above 248 K. The research of hierarchical TE materials provides valuable insights into the high-performance design of multistage TE cooling devices.
Keywords: Bi2Te3; hot deformation; low-temperature performance; thermoelectric cooling; thermoelectric material.