Equal channel angular extrusion: An effective method to refine the microstructure of cast n-type Bi2Te3 based ingot to co-optimize thermoelectric and mechanical properties

Abstract

Although the mechanical strength of n-type polycrystalline Bi2Te3 based alloys prepared by conventional powder metallurgy technology is good, its thermoelectric properties have poor repeatability and contamination is introduced. In this work, n-type polycrystalline Bi2Te3 based alloys with uniform microstructure were fabricated by applying equal channel angular extrusion (ECAE) method to extrude the cast ingot directly for four passes at 783 K. The initial lamellae coarse grains with hundreds of microns were broken down efficiently and refined uniformly to only 10–20 μm. And the Vickers hardness was increased by 2.3 times due to the refined grains. On the other hand, it is noteworthy that the ECAE process is also an ideal method to improve the thermoelectric properties of cast ingot by boosting electrical transport properties due to the donor like effect induced by heavy deformation and reducing thermal transport properties due to the enhanced phonon scattering. In order to further optimize the thermoelectric performance, BiCl3 doping was used to precisely tune the carrier concentration to the best range. The intrinsic excitation temperature of Bi2Te3 based alloys gradually shifted from low temperature (below 303 K) to high temperature (463 K) owing to the increased carrier concentration. Finally, the extruded Bi2Te3 based alloy doped with 0.064 wt % BiCl3 obtained the maximum dimensionless figure of merit (ZT) of 0.68 at 423 K, which was far higher than the nearly zero of the initial cast ingot.