Enhanced Thermoelectric Performance of Yb-Filled Skutterudite with Bottom-Up Formed CoSi2 Nanoparticles

It is known that Yb-filled skutterudite with excellent thermoelectric performance is promising for a power generation device in the intermediate temperature region. Here we created a new approach to obtain nanostructured materials by adding Si to Co-overstoichiometric Yb-filled skutterudite through high-energy ball milling, which embedded bottom-up formed CoSi2 nanoparticles into grain-refining Yb0.25Co4Sb12, synergistically resulting in the enhanced thermoelectric properties and room-temperature hardness. On one hand, the abundant grain boundaries and phase interfaces effectively blocked the propagation of medium-low frequency phonons, resulting in a lower lattice thermal conductivity. On the other hand, phase interfaces barrier nicely screened a portion of low-energy electrons, leading to an improved power factor. As a result, an enhanced peak ZT value of ∼1.43 at 823 K and a promising average ZT of ∼1.00 between 300 and 823 K were achieved in the Yb0.25Co4Sb12/0.05CoSi2 sample. Meanwhile, such nanostructures also enhanced the hardness through the collective contributions of second phase and fine grain strengthening, which made skutterudite more competitive in practical application.