Journal
ADVANCED MATERIALS
Volume 32, Issue 16, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201908218
Keywords
acoustic phonon scattering; grain boundaries; Mg3Bi2; Mg3SbBi; weighted mobility
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Funding
- NASA Science Mission Directorate's Radioisotope Power Systems Thermoelectric Technology Development
- ERC [742068]
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [392228380]
- Cluster Fellowship from the Institute for Sustainability and Energy at Northwestern (ISEN)
- Alexander von Humboldt Foundation
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Mg-3(Sb,Bi)(2) alloys have recently been discovered as a competitive alternative to the state-of-the-art n-type Bi-2(Te,Se)(3) thermoelectric alloys. Previous theoretical studies predict that single crystals Mg-3(Sb,Bi)(2) can exhibit higher thermoelectric performance near room temperature by eliminating grain boundary resistance. However, the intrinsic Mg defect chemistry makes it challenging to grow n-type Mg-3(Sb,Bi)(2) single crystals. Here, the first thermoelectric properties of n-type Te-doped Mg3Sb2 single crystals, synthesized by a combination of Sb-flux method and Mg-vapor annealing, is reported. The electrical conductivity and carrier mobility of single crystals exhibit a metallic behavior with a typical T-1.5 dependence, indicating that phonon scattering dominates the charge carrier transport. The absence of any evidence of ionized impurity scattering in Te-doped Mg3Sb2 single crystals proves that the thermally activated mobility previously observed in polycrystalline materials is caused by grain boundary resistance. Eliminating this grain boundary resistance in the single crystals results in a large enhancement of the weighted mobility and figure of merit zT by more than 100% near room temperature. This work experimentally demonstrates the accurate understanding of charge-carrier scattering is crucial for developing high-performance thermoelectric materials and indicates that single-crystalline Mg-3(Sb,Bi)(2) solid solutions can exhibit higher zT compared to polycrystalline samples.
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