Previous results indicated that acceptor doping was considered an effective clue to substantially suppress electronic thermal conductivity and in the meanwhile hold a rather low lattice thermal conductivity in high Yb-filled skutterudites. However, the strength of ionized impurity scattering needs to be regulated elaborately to balance the enhanced Seebeck coefficient and the deteriorated carrier mobility. In this work, Ge doping not only synergistically modulates the Fermi energy level and strength of ionized impurity scattering to an optimal range and attains a benign power factor but also offers a valuable opportunity to further suppress κe and κ in the classic Yb0.3Co4Sb12 alloy. Since the Yb0.3Co4Sb11.75Ge0.25 sample is endowed with the most highlighted ZT value in the device application temperature range, a promising average ZT value of 1.00 across the 300-823 K is achieved, reaching up to the level of a typical triple-filled skutterudite, which is highly desirable for achieving a satisfactory theoretical conversion efficiency of ∼14.5%. Our work corroborates that the ionized impurity strength is an extremely critical benchmark to obtain desirable thermoelectric performance in the high Yb-filled skutterudites.
Keywords: Ge doping; carrier concentration; electronic thermal conductivity; ionized impurity scattering; skutterudites; thermoelectric properties.