Simultaneous Suppression of Phonon Transport and Carrier Concentration for Efficient Rhombohedral GeTe Thermoelectric.

Superior electronic performance due to the highly degenerated Σ valence band (N(v)∼12) makes rhombohedral GeTe a promising low-temperature (<600 K) thermoelectric candidate. Minimizing lattice thermal conductivity (κ(L)) is an essential route for enhancing thermoelectric performance, but the temperature-dependent κ(L), corelated to T(-1), makes its reduction difficult at low temperature. In this work, a room-temperature κ(L) of ≈0.55 W m(-1)-K(-1), the lowest ever reported in GeTe-based thermoelectric, is realized in (Ge(1-) (y)Sb(y)Te)(1-) (x)(Cu(8)GeSe(6))(x), primarily due to strong phonon scattering induced by point defects and precipitates. Simultaneously, Cu(8)GeSe(6)-alloying effectively suppresses the precipitation of Ge, enabling the optimization of carrier concentration with the additional help of aliovalent Sb doping. As a result, an extraordinary peak zT of up to 2.3 and an average zT(avg.) of ≈1.2 within 300-625 K are achieved, leading to a conversion efficiency of ≈9% at a temperature difference of 282 K. This work robustly demonstrates its potential as a promising component in thermoelectric generator utilizing low-grade waste heat.