Effect of HPT processing on the structure, thermoelectric and mechanical properties of Sr0.07Ba0.07Yb0.07Co4Sb12

Author(s)
Gerda Rogl, Zainul Aabdin, Erhard Schafler, Jelena Horky, Daria Setman, Michael Zehetbauer, Martin Kriegisch, Oliver Eibl, Andrij Grytsiv, Ernst Bauer, Marius Reinecker, Wilfried Schranz, Peter Franz Rogl
Abstract

N-type skutterudite Sr0.07Ba0.07Yb0.07Co4Sb12 with ZT = 1.4 at 800 K was processed by high pressure torsion (HPT), a technique of severe plastic deformation (SPD) to produce a nanocrystalline material with many deformation induced lattice defects like dislocations and vacancies. As already shown previously, after HPT processing ZT similar to 1.8 was reached mainly due to a significantly reduced thermal conductivity (the lattice thermal conductivity reached almost the theoretical calculated minimum) although the electrical resistivity was higher. In this paper, the microstructural changes after HPT leading to such high ZT values were investigated. X-ray line profile analysis (XPA) before and after HPT was used to detect a smaller crystallite size and a high number of defects (dislocations and vacancies) resulting in an increase of the electrical resistivity but a significant decrease of the thermal conductivity after HPT processing. The decrease of the crystallite size could also be identified as the reason for enhanced microhardness, which means that Hall-Petch strengthening applies. In addition, for the first time, energy filtered transmission electron microscopy (TEM) was employed for the investigation of HPT processed skutterudites. Dislocations as well as grain boundaries of two types (polarised dipole walls and polarised tilt walls) could be directly observed, confirming what so far was assumed. Also for the first time thermal expansion was measured below and above room temperature and compared with the results before HPT revealing a slightly lower thermal expansion coefficient, the same Debye temperature but an Einstein temperature only half of that before HPT, the latter indicating lower frequencies of the filler atoms after HPT processing. Furthermore it could be shown that the decrease of the electrical resistivity after reaching a maximum runs parallel with a shrinking of the sample during thermal expansion measurements, proving that annealing out and closing of microcracks are responsible for this behaviour.

Organisation(s)
Department of Physical Chemistry, Physics of Nanostructured Materials, Physics of Functional Materials
External organisation(s)
Eberhard Karls Universität Tübingen, Technische Universität Wien
Journal
Journal of Alloys and Compounds
Volume
537
Pages
183-189
No. of pages
7
ISSN
0925-8388
DOI
https://doi.org/10.1016/j.jallcom.2012.05.011
Publication date
2012
Peer reviewed
Yes
Austrian Fields of Science 2012
104017 Physical chemistry, 103018 Materials physics
Portal url
https://ucrisportal.univie.ac.at/en/publications/effect-of-hpt-processing-on-the-structure-thermoelectric-and-mechanical-properties-of-sr007ba007yb007co4sb12(38f2aba5-aaca-4160-b8a3-db1c845e9ae3).html