Abstract
Alkaline metal (AM) atoms filled CoSb3 skutterudites are synthesized by melting method and sintered by spark plasma sintering. The maximal filling fraction or filling fraction limit (FFL) of AM (AM=Li, Na, K, Cs) in CoSb3 are estimated experimentally and show good agreement with our previous calculations based on density functional method. The effect of thermodynamics properties on FFL, crystallographic properties and microstructure are investigated. Among all the AM-filled CoSb3 systems, Na shows the highest experimental FFL of ~65% due to the relatively stable chemical properties of Na and NaSbx binary compounds. Furthermore, NayCo4Sb12 shows the best crystallization and purity under the same synthesis approach. In the cases of the end members Li and Cs, both our theoretical and experimental results show that the filling levels in CoSb3 are infinitesimal due to the extremely low formation enthalpies of LiSbx and CsSbx compounds.
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