Thermoelectric and mechanical properties of melt spun and spark plasma sintered n-type Yb- and Ba-filled skutterudites

Abstract

• N-type double filled skutterudites can be formed by a combination of melt spinning and spark plasma sintering, obviating annealing steps. • The consolidated billets have thermoelectric properties that are comparable to those produced using more time and energy intensive powder metallurgical methods. • We demonstrate that the here described preparation route is scalable to 80 g billets as evidenced by the comparable nature of the transport properties of specimens cuts from large samples to those of smaller lab-scale specimens. Here we present thermoelectric and mechanical properties of n-type filled-skutterudites produced by a combination of melt spinning of pre-melted charges with subsequent consolidation by spark plasma sintering, a process we refer to as MS-SPS. This combination of processing steps leads to phase-pure n-type filled-skutterudites and obviates more energy and time intensive annealing steps. We show that both the thermoelectric properties and the tensile fracture strength compare favorably to materials made by traditional methods. The process is scalable to at least 80 g billets, such that the transport properties measured on test bars harvested from these larger billets compare favorably to those measured on lab-scale billets (5 g total billet mass). ZT values approaching 1.1 at 750 K were observed in materials made by MS-SPS. In addition, the tensile fracture strength of test bars cut from an 80 g billet is ∼128 MPa at room temperature and decreases with increasing temperature. Fractography of the test bars reveals that the majority failed due to surface and edge flaws with few failures due to volume type flaws. This indicates that the powder metallurgical methods employed to produce these samples is mature.