Enhancing n-type PbTe thermoelectric performance through Cd alloying and strategic defects management

The significant performance disparity between n-type and p-type PbTe hinders their commercial viability in thermoelectric (TE) applications. While conventional multi-element alloying has demonstrably improved n-type PbTe thermoelectrics, it introduces stability concerns and cost escalation. Here, we propose a simpler approach utilizing a single isovalent element alloying strategy with Cd and defect management to enhance the TE performance of n-type PbTe. Cd doping widens the bandgap, leading to an increased effective mass and Seebeck coefficient, particularly at higher temperatures due to improved Cd solubility. However, as documented in previous studies on the PbTe-Cd system, Cd introduction can potentially deteriorate TE performance by reducing carrier mobility. To address this, we implemented defect engineering to optimize carrier mobility. A small excess of Pb atoms was introduced to occupy intrinsic Pb vacancies, achieving a remarkable 65.5 % enhancement in carrier mobility. Consequently, the maximum power factor of Cd-alloyed Pb _1.01Te samples reaches 31.5 μW cm ⁻¹ K ⁻² , marking a significant 69.3 % improvement compared to pristine PbTe. Additionally, the Cd-induced bandgap widening effectively mitigates bipolar diffusion. This, combined with enhanced phonon scattering due to the secondary CdTe phase, results in a 34.3 % decrease in thermal conductivity. By leveraging the multifaceted effects of Cd alloying and defect management, the ZT value of Pb _1.01 Te-2 %Cd samples reaches 1.35 at 782 K. These findings offer a new perspective on the versatile use of single isovalent element alloying strategy and performance optimization in other TE materials.