Enhanced Density of States Facilitates High Thermoelectric Performance in Solution-Grown Ge- and In-Codoped SnSe...

SnSe single crystals have gained great interest due to their excellent thermoelectric performance. However, polycrystalline SnSe is greatly desired due to facile processing, machinability, and scale-up application. Here, we report an outstanding high average ZT of 0.88 as well as a high peak ZT of 1.92 in solution-processed SnSe nanoplates. Nanosized boundaries formed by nanoplates and lattice strain created by lattice dislocations and stacking faults effectively scatter heat-carrying phonons, resulting in an ultralow lattice thermal conductivity of 0.19 W m^-1 K^-1 at 873 K. Ultraviolet photoelectron spectroscopy reveals that Ge and In incorporation produces an enhanced density of states in the electronic structure of SnSe, resulting in a large Seebeck coefficient. Ge and In codoping not only optimizes the Seebeck coefficient but also substantially increases the carrier concentration and electrical conductivity, helping to maintain a high power factor over a wide temperature range. Benefiting from an enhanced power factor and markedly reduced lattice thermal conductivity, high average ZT and peak ZT are achieved in Ge- and In-codoped SnSe nanoplates. This work achieves an ultrahigh average ZT of 0.88 in polycrystalline SnSe by adopting nontoxic element doping, potentially expanding its usefulness for various thermoelectric generator applications.