Atomic-defect-suppressed pristine p-type Bi0.3Sb1.7Te3 as robust high-performance thermoelectrics for power generation and cooling

High-strength high-performance p-type (Bi,Sb) 2 Te 3 are of pivotal importance for near-room-temperature thermoelectric conversions, the reliable synthesis and fabrication has been viewed of imperative priority. It is known that the energy-favorable formation of anti-site Sb Te ' and vacancy v Sb ''' acceptor defects from high-temperature syntheses results in additional charge carriers and scattering centers for electrical and phonon transport. However, how p-type (Bi,Sb) 2 Te 3 with minimal lattice defects function remains to be scrutinized. Herein, we present the synergistic enhancements of mechanical robustness and thermoelectric property in crystallographic-defect-suppressed pristine (Bi,Sb) 2 Te 3 through a simple mechanical alloying combined with spark-plasma-sintering (SPS) process. The Sb Te ' and v Sb ''' acceptor defects were efficiently restrained, contributing to markedly increased charge carrier mobilities. A slightly enlarged band gap of 0.24 eV underpinned enhanced thermoelectric performance for pristine Bi 0.3 Sb 1.7 Te 3 over a wide temperature range, delivering high zT 300 K of 1.16 and zT ave of 1.21 over 300–473 K. Interestingly, the confined in-situ grain coarsening during SPS with uniform dispersive nanopores readily endowed an ultra-high compressive strength of 206 MPa, surpassing that of reported (Bi,Sb) 2 Te 3 so far. A 7-pair module (coupled with n-Bi 2 Te 3 ) was fabricated, demonstrating a competitive Δ T over 70 K at T hot = 300 K. Furthermore, a power-generation module coupled with n-Mg 3 SbBi registered a cutting-edge thermoelectric conversion efficiency of 9.5% at a temperature gradient of 250 K. The strategy eliminates the need of complex processing nor extrinsic doping for pristine (Bi,Sb) 2 Te 3 , demonstrating great potentials in thermoelectric power generation and cooling applications. • Mechanical alloying and SPS under Ar suppress lattice defects, enabling high μ H of ∼251 cm 2 ⸱V –1 ⸱s –1 . • Pristine Bi 0.3 Sb 1.7 Te 3 shows zT 300 K of 1.16 and zT ave of 1.21 due to band-gap widening with optimized n H . • High mechanical compressive strength of 206 MPa is achieved from a single-step SPS processing. • Device-level cooling Δ T 303 K > 70 K and conversion efficiency of 9.5% (Δ T = 250 K) are delivered by respective modules.