期刊
ACS APPLIED ENERGY MATERIALS
卷 6, 期 1, 页码 580-587出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.2c03958
关键词
argyrodites; entropy engineering; thermoelectric performance; lattice thermal conductivity; phase transition
By employing the entropy engineering strategy through S alloying on the Se site, the phase transition temperature of Cu8GeSe6 is lowered, maintaining a stable cubic phase throughout the operating temperature region. The cubic Cu8GeSe6 exhibits improved carrier mobility and electrical performance due to its favorable electronic structure. Additionally, it possesses an ultralow thermal conductivity, making it a promising candidate for thermoelectric applications.
Argyrodite-type semiconductors, as prototypes of the phonon-liquid electron crystal concept, have attracted intensive attention due to their intrinsically low thermal conductivity. Like other members of this family, Cu8GeSe6 undergoes structural phase transition at 330 K from a low-temperature hexagonal phase to a high-temperature hexagonal phase. Here, by employing the entropy engineering strategy through S alloying on the Se site, the phase transition temperature is lowered to below room temperature, so that the stable cubic phase is maintained in the whole operating temperature region. Cubic Cu8GeSe6 exhibits a favorable electronic structure, which leads to improved carrier mobility and electrical performance. In addition, benefiting from the weak chemical bonding between Cu atoms and the [GeSe6] sublattice and the disordered cation occupancy, cubic Cu8GeSe6 possesses an ultralow thermal conductivity, and the sample with a nominal composition of Cu8GeSe4.2S1.8 reaches a zT value of 0.5 at 627 K. These results provide insights for suppressing phase transition in argyrodite-type thermoelectrics.
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