ABSTRACT
Tetrahedrites, a class of earth-abundant minerals, exhibit extremely low thermal conductivity values making them promising candidates for thermoelectric applications at high temperatures. Herein, we extend investigations on these materials to specimens substituted on both the Cu and Sb sites by reporting on the thermoelectric properties of polycrystalline Cu12-xCoxSb4-yTeyS13 in a wide range of temperatures (2-700 K). All prepared samples exhibit p-type heavily-doped semiconducting behavior with relatively low electrical resistivity values. These substitutions have little influence on the thermal conductivity, which remains very low in the whole temperature range (â¼0.7 W m(-1) K(-1)). Although the double-substituted samples exhibit higher ZT values with respect to the parent tetrahedrite Cu12Sb4S13, the maximum ZT of 0.80 reached at 700 K for (x,y) = (0.82, 0.41) remains comparable to the values obtained in compounds solely substituted with Co or Te.
ABSTRACT
The ability of some materials with a perfectly ordered crystal structure to mimic the heat conduction of amorphous solids is a remarkable physical property that finds applications in numerous areas of materials science, for example, in the search for more efficient thermoelectric materials that enable to directly convert heat into electricity. Here, we unveil the mechanism in which glass-like thermal conductivity emerges in tetrahedrites, a family of natural minerals extensively studied in geology and, more recently, in thermoelectricity. By investigating the lattice dynamics of two tetrahedrites of very close compositions (Cu12Sb2Te2S13 and Cu10Te4S13) but with opposite glasslike and crystal thermal transport by means of powder and single-crystal inelastic neutron scattering, we demonstrate that the former originates from the peculiar chemical environment of the copper atoms giving rise to a strongly anharmonic excess of vibrational states.