Robustly Boosting Thermoelectric Performance of N‐Type PbSe via Lattice Plainification and Dynamic Doping

Abstract Ideal thermoelectrics shall possess a high average ZT , which relies on high carrier mobility and appropriate carrier density at operating temperature. However, conventional doping usually results in a temperature‐independent carrier concentration, making performance optimization over a wide temperature range be challenging. This work demonstrates the combination of lattice plainification and dynamic doping strategies is an effective route to boost the average ZT of N‐type PbSe. Because Sn and Pb have similar ionic radii and electronegativity, this allows Sn to fill the intrinsic Pb vacancies and effectively improves the carrier mobility of PbSe to 1300 cm 2 V −1 s −1 . Furthermore, a trace amount of Cu is introduced into the Sn‐filled PbSe to optimize the carrier concentration. The extra Cu is situated in the interstitial sides of the lattice, which undergoes a dissolution‐precipitation process with temperature, leading to a strongly temperature‐dependent carrier density in the material. This dynamic doping effectively improves the electrical transport properties and is also valid to suppress the lattice thermal conductivity. Ultimately, the resulting PbSn 0.004 Se+3‰Cu obtains a maximum ZT of ≈1.7 at 800 K and an average ZT of ≈1.0, with a 7.7% power generation efficiency in a single‐arm device, showing significant potential for commercial application.