As an ecofriendly thermoelectric material with intrinsic low thermal conductivity, ternary diamond-like CuSnSe (CSS) has attracted much attention. Nevertheless, its figure of merit, ZT, is limited by its small thermopower () and power factor (PF). Here, we show that an increase in thermopower by 63% and a carrier-mobility rise of 81% at 300 K can be simultaneously achieved through 5% substitution of Fe for Sn due to both enhancement of electronic density of states and degeneracy of multiple valence band maxima, which lead to high PF = 10.3 μW·cm·K at 823 K for Fe-doped CSS (CSFS). Besides, an ultrahigh PF of 14.8 μW·cm·K (at 773 K) and 45% reduction of lattice thermal conductivity (at 823 K) are realized for CSFS-based composites with 0.125 wt % of MgO nanoinclusions, owing to further enhancement of via energy-dependent scattering and strong phonon scattering by the embedded nanoparticles. Consequently, a maximum ZT = 1 at 823 K is reached for the CSFS/ MgO composite samples with = 0.125 wt %, which is around 2.5 times larger than that of the CSS compound.
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