Abstract
The structural and thermoelectric properties of the filled skutterudite (Sm,Gd)y(FexNi1-x)4Sb12 were investigated and critically compared to the ones in the Sm-containing system with the aim of unravelling the effect of double filling on filling fraction and thermal conductivity. Several samples (x = 0.50–0.90 and y = 0.15–0.48) were prepared by melting-sintering, and two of them were densified by spark plasma sintering in order to study their thermoelectric features. The crystallographic study enables the recognition of the role of the filler size in ruling the filling fraction and the compositional location of the p/n crossover: It has been found that the former lowers and the latter moves toward lower x values with the reduction of the filler ionic size, as a consequence of the progressively weaker interaction of the filler with the Sb12 cavity. The analysis of thermoelectric properties indicates that, despite the Sm3+/Gd3+ small mass difference, the contemporary presence of these ions in the 2a site significantly affects the thermal conductivity of both p- and n-compositions. This occurs by reducing its value with respect to the Sm-filled compound at each temperature considered, and making the overall thermoelectric performance of the system comparable to several multi-filled (Fe, Ni)-based skutterudites described in the literature.
Highlights
In the field of modern solid state chemistry and physics, thermoelectricity occupies a central role due to its relevance in the framework of energy conversion, in particular, refrigeration and electric power generation
According to SEM microphotographs, the EDS analyses and X-ray diffraction, the filled skutterudite results were by far the main phase for each formulation, even if small amounts of extra phases could be revealed in all the samples
The Sm and Gd amounts derive from the refinement of the occupancy factor of the 2a site, and they are in good agreement with the EDS results
Summary
In the field of modern solid state chemistry and physics, thermoelectricity occupies a central role due to its relevance in the framework of energy conversion, in particular, refrigeration and electric power generation. Materials 2019, 12, 2451 fulfilling several requirements, such as high electrical conductivity and low thermal conductivity. The need for decoupling thermal and electrical conductivity suggests that a two-fold strategy is pursued, consisting of mainly acting on the reduction of λph and the increase of σ. This goal can be achieved by addressing the search for valid thermoelectric materials for semiconductors
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