InSb nanoparticles dispersion in Yb-filled Co4Sb12 improves the thermoelectric performance

Abstract

Out of several methods, one of the most explored strategies to decrease the lattice thermal conductivity of Co4Sb12-based materials are either filling suitable electropositive elements into the voids or the formation of nanocomposites. These two approaches were combined in this work by filling Yb into the void of Co4Sb12 and preparing nanocomposites of Yb0.2Co4Sb12 and InSb according to the formula (InSb)x + Yb0.2Co4Sb12 (where x = 0.1, 0.2, 0.3, 0.4), via ball-milling and spark plasma sintering. Yb2O3 and CoSb2 as impurity phases were found at the grain boundaries. EBSD and TEM micrographs showed nanocrystalline InSb phase (20–200 nm) dispersed in the matrix grains. The charge transfer from Yb filler with an oxidation state of +3 to Co4Sb12 yielded a low electrical resistivity (ρ) of the matrix. An increase in ρ and Seebeck coefficient (S) in the composites with x = 0.1 and 0.3 occurred due to the higher amount of oxide impurities in these two samples and the scattering of charge carriers at the interfaces induced by the secondary phases. The other two composites with x = 0.2 and 0.4 exhibited ρ(T) and S(T) similar to the Yb0.2Co4Sb12 matrix. The dispersion of the InSb and Yb2O3 phases at the grain boundaries combined with the anharmonicity introduced by the fillers (Yb) in the voids enhanced the scattering of phonons within a broad wavelength range and reduced the lattice thermal conductivity significantly. Hence, a highest zT of ~1.2 at 773 K with a thermoelectric efficiency of 8.89% and 8.28% (423–773 K) were obtained for (InSb)0.1 + Yb0.2Co4Sb12 and (InSb)0.2 + Yb0.2Co4Sb12 nanocomposites, respectively.