High-temperature thermoelectric properties with Th${}_{3-x}$Te${}_4$

Th${}_3$Te${}_4$ materials are potential candidates for commercial thermoelectric (TE) materials at high-temperature due to their superior physical properties. We incorporate the multiband Boltzmann transport equations with firstprinciples calculations to theoretically investigate the TE properties of Th${}_3$Te${}_4$ materials. As a demonstration of our method, the TE properties of La${}_3$Te${}_4$ are similar with that of Ce${}_3$Te${}_4$ at low-temperature, which is consistent with the experiment. Then we systematically calculate the electrical conductivity, the Seebeck coefficient, and the power factor of the two materials above based on parameters obtained from first-principles calculations as well as several other fitting parameters. Our results reveal that for the electron–optical-phonon scattering at high temperatures, a linear dependence of optical phonon energy on temperature explains better the experimental results than a constant optical phonon energy. Based on this, we predict that the TE properties of Ce${}_3$Te${}_4$ is better than La${}_3$Te${}_4$ at high temperatures and the optimal carrier concentration corresponding to Ce${}_3$Te${}_4$ shifts upward with increasing temperature. The optimal carrier concentration of Ce${}_3$Te${}_4$ is around $1.6\times {10}^{21}$cm${}^{-3}$ with the peak power factor 13.07 $\mu$Wcm${}^{-1}$K${}^{-2}$ at $T=1200$K.