Abstract

Defect engineering is the core strategy for improving thermoelectric properties. Herein, cation doping along with modulation of cation vacancy have been developed in GeTe based materials as an effective method to induce vacancy-based defects to boost its thermoelectric performance. A series of ternary compounds of Ge9Sb2Te12-x (x = 0, 0.03, 0.06, 0.09, 0.12, 0.15) was prepared by vacuum melting and annealing combined with the SPS process. The role of Sb doping and the cation vacancy on the thermoelectric properties were systematically investigated. It is found that alloying Sb2Te3 with GeTe increases the concentration of cation vacancies, which is corroborated by both positron annihilation measurements and theoretical calculations. The vacancies, stacking faults and planar defects interaction determines the thermoelectric transport properties. Adjusting the deficiency of Te effectively tunes the concentration of cation vacancies and dopant defects in the structure. In turn, this tunes the carrier concentration close to its optimum. A high power factor of 32.6 μW cm-1 K-2 is realized for Ge9Sb2Te11.91 at 725 K. Moreover, large strains induced by the defect structures including Sb dopant, vacancy, staking faults as well as planar defects intensify phonon scattering, leading to a significant decrease in the lattice thermal conductivity from 7.6 W m-1 K-1 for pristine GeTe to 1.18 W m-1 K-1 for Ge9Sb2Te11.85 at room temperature. All the above contribute to a high ZT value of 2.1 achieved for Ge9Sb2Te11.91 sample at 775 K.

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