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Nanostructured Co1-XNixSb3 Skutterudites: Synthesis, Thermoelectric Properties and Theoretical Modeling (Articolo in rivista)
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- Nanostructured Co1-XNixSb3 Skutterudites: Synthesis, Thermoelectric Properties and Theoretical Modeling (Articolo in rivista) (literal)
- Anno
- 2003-01-01T00:00:00+01:00 (literal)
- Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#doi
- 10.1063/1.1529077 (literal)
- Alternative label
Bertini L., Stiewe C., Toprak M., Williams S., Platzek D., Mrotzec A., Zhang Y., Gatti C., Müller E., Mamoun M., Rowe M. (2003)
Nanostructured Co1-XNixSb3 Skutterudites: Synthesis, Thermoelectric Properties and Theoretical Modeling
in Journal of applied physics; AIP, American institute of physics, Melville, NY (Stati Uniti d'America)
(literal)
- Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#autori
- Bertini L., Stiewe C., Toprak M., Williams S., Platzek D., Mrotzec A., Zhang Y., Gatti C., Müller E., Mamoun M., Rowe M. (literal)
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- ISI Web of Science (WOS) (literal)
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- Luca Bertinia)Istituto di Scienze e Tecnologie Molecolari (ISTM), Via Camillo Golgi 19, 20133 Milano, Italy
Christian Stiewe German Aerospace Center (DLR), Linder Hoehe, 51147 Cologne, Germany
Muhammet Toprak Royal Institute of Technology (KTH), Stockholm, Sweden
Simon Williams NEDO Laboratory for Thermoelectric Engineering (NEDO), Cardiff, United Kingdom
Dieter Platzek and Antje Mrotzek German Aerospace Center (DLR), Linder Hoehe, 51147 Cologne, Germany
Yu Zhang Royal Institute of Technology (KTH), Stockholm, Sweden
Carlo Gatti Istituto di Scienze e Tecnologie Molecolari (ISTM), Via Camillo Golgi 19, 20133 Milano, Italy
Eckhard Muller German Aerospace Center (DLR), Linder Hoehe, 51147 Cologne, Germany
Mamoun Muhammed Royal Institute of Technology (KTH), Stockholm, Sweden
Michael Rowe NEDO Laboratory for Thermoelectric Engineering (NEDO), Cardiff, United Kingdom (literal)
- Titolo
- Nanostructured Co1-XNixSb3 Skutterudites: Synthesis, Thermoelectric Properties and Theoretical Modeling (literal)
- Abstract
- Nanostructured skutterudite Co12xNixSb3 has been synthesized by chemical alloying with Ni
substitution for Co up to 27.5 at. %. High concentration of grain boundaries provided by
nanostructuring is expected to lower the thermal conductivity of thermoelectric materials and could
thus increase their thermoelectric dimensionless figure-of-merit ZT. Material preparation comprises
two key stages, coprecipitation of the precursor, and thermal processing to produce the skutterudite.
By modeling the chemistry of the metal ions in aqueous solution, optimum coprecipitation
conditions were achieved. The precipitated precursor consists of a solid solution of the different
intermediate compounds, and exhibits high reactivity. Calcination and reduction of the precursor
resulted in the alloying of these elements and in the formation of skutterudite at a temperature as low
as 723-773 K. Unfilled CoSb3 skutterudites were prepared by chemical precipitation from aqueous
solutions to achieve powders with a very small grain size ~;40 nm!. Compacted samples were
produced from this powder by uniaxial pressing under various conditions. Thermal conductivity,
electrical resistivity and Seebeck coefficient of the resulting compacts were measured in a
temperature range from 150 to 575 K. Measurement procedures were standardized for absolute
accuracy and reproducibility between the DLR, Cologne and NEDO, Cardiff Laboratories. It was
found that the thermal conductivity can be decreased by almost an order of magnitude at the highest
concentration of grain boundaries compared to highly annealed CoSb3 . Scanning Seebeck
microthermoprobe examination, facilitated spatially resolved measurement of Seebeck coefficient S,
providing information on samples' homogeneity and on its effect on local S. Indications on the
formation of an additional Ni containing phase were found. The electronic structure of Ni-doped
skutterudites has been investigated by means of fully periodic density functional theory calculations
and a topological analysis of the resulting electron densities. Ni substitution for Co doubles the
electronic charge transfer from the pnicogen ring to the metal frame and fills the region of the CoSb3
band gap with occupied states, thus explaining the increase of electrical conductivity observed
experimentally. The effect of the Ni substitution on the thermal conductivity is analyzed. The computed changes of the cell parameter with rising Ni content differ with those found by x-ray
powder diffraction, thereby suggesting that the structural hypothesis of Ni replacing Co in the cubic
frame of the skutterudite is only approximate or possibly incorrect. (literal)
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