Phonon scattering by nanostructures and point defects has become the primary strategy for minimizing the lattice thermal conductivity (κ ) in thermoelectric materials. However, these scatterers are only effective at the extremes of the phonon spectrum. Recently, it has been demonstrated that dislocations are effective at scattering the remaining mid-frequency phonons as well. In this work, by varying the concentration of Na in Pb Eu Te, it has been determined that the dominant microstructural features are point defects, lattice dislocations, and nanostructure interfaces. This study reveals that dense lattice dislocations (≈4 × 10 cm ) are particularly effective at reducing κ . When the dislocation concentration is maximized, one of the lowest κ values reported for PbTe is achieved. Furthermore, due to the band convergence of the alloyed 3% mol. EuTe the electronic performance is enhanced, and a high thermoelectric figure of merit, zT, of ≈2.2 is achieved. This work not only demonstrates the effectiveness of dense lattice dislocations as a means of lowering κ , but also the importance of engineering both thermal and electronic transport simultaneously when designing high-performance thermoelectrics.
Compared to commercially available p-type PbTe thermoelectrics, SnTe has a much bigger band offset between its two valence bands and a much higher lattice thermal conductivity, both of which limit its peak thermoelectric figure of merit, zT of only 0.4. Converging its valence bands or introducing resonant states is found to enhance the electronic properties, while nanostructuring or more recently introducing interstitial defects is found to reduce the lattice thermal conductivity. Even with an integration of some of the strategies above, existing efforts do not enable a peak zT exceeding 1.4 and usually involve Cd or Hg. In this work, a combination of band convergence and interstitial defects, each of which enables a ≈150% increase in the peak zT, successfully accumulates the zT enhancements to be ≈300% (zT up to 1.6) without involving any toxic elements. This opens new possibilities for further improvements and promotes SnTe as an environment-friendly solution for conventional p-PbTe thermoelectrics.
To minimize the lattice thermal conductivity in thermoelectrics, strategies typically focus on the scattering of low-frequency phonons by interfaces and high-frequency phonons by point defects. In addition, scattering of mid-frequency phonons by dense dislocations, localized at the grain boundaries, has been shown to reduce the lattice thermal conductivity and improve the thermoelectric performance. Here we propose a vacancy engineering strategy to create dense dislocations in the grains. In Pb1−xSb2x/3Se solid solutions, cation vacancies are intentionally introduced, where after thermal annealing the vacancies can annihilate through a number of mechanisms creating the desired dislocations homogeneously distributed within the grains. This leads to a lattice thermal conductivity as low as 0.4 Wm−1 K−1 and a high thermoelectric figure of merit, which can be explained by a dislocation scattering model. The vacancy engineering strategy used here should be equally applicable for solid solution thermoelectrics and provides a strategy for improving zT.
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