Optimization of Bulk Thermoelectrics: Influence of Cu Insertion in Ag3.6Mo9Se11
Résumé
Currently, there is a resurgence of interest in thermoelectric materials with enhanced efficiency. Among investigated classes of bulk thermoelectrics such as partially filled skutterudites, Zn4Sb3-based materials, and clathrates, novel polycrystalline Mo-9 cluster-based chalcogenides were reported recently. Among those, Chevrel phase-derived Ag Mo9Se11 (with 3.4 <= y <= sign 3.9) compounds have shown interesting thermoelectric properties, in particular extremely low thermal conductivity allowing improved thermoelectric efficiency compared with reported Chevrel phases. They also possess a complex crystallographic structure where stacked Mo9Se11 units leave channels occupied by Ag atoms. Analysis of the structural determinants of the thermoelectric properties of Ag Mo9Se11 suggested that performance improvements could result from further Cu insertion. In this paper, we describe the synthesis route we used for preparing quaternary Ag-Cu-Mo-Se compositions by a combination of powder metallurgy and spark plasma sintering techniques. Characterization by x-ray diffraction, scanning electron microscopy, and electrical and thermal measurements has been performed. The results obtained for two compounds (Ag3.6Cu0.2Mo9Se11 and Ag3.6Cu0.4Mo9Se11) are discussed and compared with those of the parent ternary compound Ag3.6Mo9Se11.