科研之友
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摘要
The dimensionless figure of merit, ZT, of bulk thermoelectric materials depends mainly on the transport properties of charge carriers and heat-carrying phonons. PbTe-4 mol % SrTe doped with 2 mol % Na (Pbw(0.94)Na(0.02)Sr(0.04)Te) is a nanostructured material system that exhibits a ZT higher than 2. The precipitate size distribution of SrTe precipitates is believed to play a key role. This raises the question of whether its performance is limited by precipitate coarsening (Ostwald ripening) at elevated temperatures. Herein, we utilize an atom-probe tomography (APT) to study the number density and mean radii of precipitates in concert with partial radial distribution functions (RDFs) of individual atoms. We find that the SrTe precipitates actually contain oxygen: SrTe1-xOx. We correlate this information with the overall ZT performance, specifically focusing on the electrical and lattice thermal conductivities after isothermal, heat treatments at 300 and 400 degrees C for 7 days, followed by furnace cooling. Comparison of the samples annealed at 400 and 300 degrees C demonstrates significant coarsening of SrTe1-xOx precipitates as well as strong segregation of oxygen impurities in the SiTe1-xOx precipitates. Additionally, on the basis of the partial RDFs, the Na dopant atoms cluster with other Na atoms as well as with Pb, Te, and St atoms; clustering depends strongly on the annealing temperature and concomitantly affects the overall ZT values. We found that the coarsening slightly increases the lattice thermal conductivity and also increases the electrical conductivity, thereby having little or even a beneficial effect on the ZT values. Importantly, these findings demonstrate that APT enables quantitative analyses in three dimensions of the PbTe-4 mol %. SrTe samples in addition to correlation of their properties with the thermoelectric performance.
