The filling fraction
limitation (FFL) in n-type CoSb3 skutterudites is far below
that of p-type (Fe,Co)Sb3-based
skutterudites, and it is critical to increase FFL for accomplishing
high thermoelectric figure of merit (ZT
max). Here, a series of Yb
x
Co4–y
Fe
y
Sb12 alloys with x = 0.25–0.5 and y = 0.1–0.5 were synthesized, which demonstrate a clear increase
of the FFL of Yb from ∼0.3 in CoSb3 to 0.5. Ultralow
thermal conductivities of 2.0–2.5 W/m·K at 300 K and 1.75
W/m·K at ∼600 K have been achieved, which are the lowest
values reported among skutterudite materials and comparable with p-type
skutterudites. These ultralow thermal conductivities result from the
combination of secondary phase scattering and phonon scattering from
dynamic electron exchange between Fe2+ and Co3+. High ZT
max values of 1.28 at 740 K
and 1.34 at 780 K are obtained, which are among the best values reported
in the temperature range of 740–800 K. The temperature at which
maximum ZT
max appears is shifted below
850 K. These results are highly exciting toward the development of
multistage segmented and cascade thermoelectric power generators for
in-air operations.