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A broad tunability of the thermoelectric and mechanical properties of CoSb3 has been demonstrated by adjusting the composition with the addition of an increasing number of elements. However, such a strategy may negatively impact processing repeatability and composition control. In this work, single-element-filled skutterudite is engineered to have high thermoelectric and mechanical performances. Increased Yb filling fraction is found to increase phonon scattering, whereas cryogenic grinding contributes additional microstructural scattering. A peak zT of 1.55 and an average zT of about 1.09, which is comparable to the reported results of multiple-filled SKDs, are realized by the combination of simple composition and microstructure engineering. Furthermore, the mechanical properties of Yb single-filled CoSb3 skutterudite are improved by manipulation of the microstructure through cryogenic grinding. These findings highlight the realistic prospect of producing high-performance thermoelectric materials with reduced compositional complexity.
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