Alloy scattering to optimize carrier and phonon transport properties in PbBi2S4 thermoelectric

Ternary PbBi 2 S 4 compound with crustal S-rich element and low lattice thermal conductivity is considered as a potential thermoelectric candidate. However, its inferior thermoelectric properties are rooted in the low electrical transport performance. Generally, enhancing electrical transport performance (power factor, PF) primarily entails optimizing the interdependent relationship between carrier mobility μ (linked to electrical conductivity σ ) and effective mass m ∗ (related to Seebeck coefficient S ). In this work, we introduce the strategy of alloy scattering to independently enhance S without weakening μ and simultaneously reduce thermal conductivity, leading to a synergetic optimization of electron and phonon in PbBi 2 S 4 thermoelectric. Heavy Sn alloying in PbBi 2 S 4 presents uniform and orderly distribution on Pb sites as unclosed by the atomic-scale crystal structure observation. These massive Sn atom serves as scattering centers and turns the electron scattering mechanism to be dominated by alloy scattering, thus resulting in a ∼33% increment of S in Pb 0.6 Sn 0.4 Bi 2 S 4 . Meanwhile, Sn alloying aggravates phonon scattering further lowering lattice thermal conductivity and reaching an extremely low value of 0.34 W⋅m −1 ·K −1 at 773 K. Finally, a maximum zT of 0.68 at 773 K is obtained in Pb 0.6 Sn 0.4 Bi 2 S 4 , which is ∼ 45% higher than the pristine matrix. This study proves that the strategy of alloy scattering is effective in improving overall electrical transport properties as well as reducing lattice thermal conductivity, which paves a new way to develop high-performance thermoelectric materials. • Heavy Sn alloying changes the scattering mechanism of the pristine PbBi 2 S 4 . • Demonstrate the feasibility of alloy scattering. • The highest zT value 0.68 is achieved for PbBi 2 S 4 -based material in Pb 0.6 Sn 0.4 Bi 2 S 4 .