Realizing high-ranged thermoelectric performance in PbSnS₂ crystals

Great progress has been achieved in p-type SnS thermoelectric compound recently, while the stagnation of the n-type counterpart hinders the construction of thermoelectric devices. Herein, n-type sulfide PbSnS₂ with isostructural to SnS is obtained through Pb alloying and achieves a maximum ZT of ~1.2 and an average ZT of ~0.75 within 300–773 K, which originates from enhanced power factor and intrinsically ultralow thermal conductivity. Combining the optimized carrier concentration by Cl doping and enlarged Seebeck coefficient through activating multiple conduction bands evolutions with temperature, favorable power factors are maintained. Besides, the electron doping stabilizes the phase of PbSnS₂ and the complex-crystal-structure induced strong anharmonicity results in ultralow lattice thermal conductivity. Moreover, a maximum power generation efficiency of ~2.7% can be acquired in a single-leg device. Our study develops a n-type sulfide PbSnS₂ with high performance, which is a potential candidate to match the excellent p-type SnS.