New filled P-based skutterudites—promising materials for thermoelectricity?

Physics

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Scientific paper

The crystal structure, thermodynamic stability and electronic structure of the 75 filled and unfilled skutterudite compounds MxCo4- yFeyP12, with M being La, Y and Sc, x = {0, 0.125, 0.25, 0.50, 1} and y={0, 1, 2, 3, 4} are predicted from periodic density functional calculations. The rattling amplitude of the filling atom M, which is important for the thermal conductivity of the compounds, is found to depend mostly on the type of filling element and only to a small extent on the filling fraction, or the fraction of Fe in the structure. The calculated ground state stabilities show that none of the Sc-filled skutterudites are thermodynamically stable at 0 K, while the only stable combination of x and y among the studied Y-filled ones is YCoFe3P12. The La-filled skutterudites, on the other hand, are thermodynamically stable in a variety of combinations, with maximum stability when y=3x, that is three Fe atoms per filling atom. Based on the calculated electronic structure we also expect filled skutterudites with y=3x to be most interesting for thermoelectric applications.

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