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CoSb 3 -based skutterudite is a promising mid-temperature thermoelectric material. However, the high lattice thermal conductivity limits its further application. Filling is one of the most effective methods to reduce the lattice thermal conductivity. In this study, we investigate the Ce filling limit and its influence on thermoelectric properties of p-type Fe 3 CoSb 12 -based skutterudites grown by a temperature gradient zone melting (TGZM) method. Crystal structure and composition characterization suggests that a maximum filling fraction of Ce reaches 0.73 in a composition of Ce 0.73 Fe 2.73 Co 1.18 Sb 12  prepared by the TGZM method. The Ce filling reduces the carrier concentration to 1.03 × 10 20  cm −3  in the Ce 1.25 Fe 3 CoSb 12 , leading to an increased Seebeck coefficient. Density functional theory (DFT) calculation indicates that the Ce-filling introduces an impurity level near the Fermi level. Moreover, the rattling effect of the Ce fillers strengthens the short-wavelength phonon scattering and reduces the lattice thermal conductivity to 0.91 W m −1  K −1 . These effects induce a maximum Seebeck coefficient of 168 μV K −1  and a lowest  κ  of 1.52 W m −1  K −  1  at 693 K in the Ce 1.25 Fe 3 CoSb 12 , leading to a peak  zT  value of 0.65, which is 9 times higher than that of the unfilled Fe 3 CoSb 12 .

Ce Filling Limit and Its Influence on Thermoelectric Performance of Fe3CoSb12-Based Skutterudite Grown by a Temperature Gradient Zone Melting Method