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Environmentally friendly Mg 3 Sb 2 -based materials have drawn intensive attention owing to their promising thermoelectric performance. In this work, the electrical properties of p-type Mg 3 Sb 2  are dramatically optimized by the regulation of Mg deficiency. Then, we, for the first time, found that Zn substitution at the Mg2 site leads to the alignment ofp    x  ,  yandp    zorbital, resulting in a high band degeneracy and the dramatically enhanced Seebeck coefficient, demonstrated by the DFT calculations and electronic properties measurement. Moreover, Zn alloying decreases Mg1 (Zn) vacancies formation energy and in turn increases Mg (Zn) vacancies and optimizes the carrier concentration. Simultaneously, the Mg/Zn substitutions, Mg vacancies, and porosity structure suppress the phonon transport in a broader frequency range, leading to a low lattice thermal conductivity of ~0.47 W m -1  K -1  at 773 K. Finally, a high  ZT  of ~0.87 at 773 K was obtained for Mg 1.95 Na 0.01 Zn 1 Sb 2 , exceeding most of the previously reported p-type Mg 3 Sb 2  compounds. Our results further demonstrate the promising prospects of p-type Mg 3 Sb 2 -based material in the field of mid-temperature heat recovery.

research

Electronic Orbital Alignment and Hierarchical Phonon Scattering Enabling High Thermoelectric Performance p-Type Mg <sub>3</sub> Sb <sub>2</sub> Zintl Compounds

Electronic Orbital Alignment and Hierarchical Phonon Scattering Enabling High Thermoelectric Performance p-Type Mg 3 Sb 2 Zintl Compounds

Electronic Orbital Alignment and Hierarchical Phonon Scattering Enabling High Thermoelectric Performance p-Type Mg ₃ Sb ₂ Zintl Compounds