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Published on: December 5, 2019
On the oxidation of EuFe4Sb12 and EuRu4Sb12
Jessica M Peddle1, Michael W Gaultois, Andrew P Grosvenor
1Department of Chemistry, University of Saskatchewan, Saskatoon, Saskatchewan, Canada S7N 5C9.
Substituting elements in rare-earth-filled skutterudites enhances thermal stability. Larger elements like Europium (Eu) and Ruthenium (Ru) improve oxidation resistance in these thermoelectric materials.
Area of Science:
- Materials Science
- Solid State Chemistry
- Thermoelectric Materials
Background:
- Rare-earth-filled transition-metal pnictides with skutterudite structures are promising for high-temperature thermoelectric applications, such as waste heat recovery.
- Previous studies on CeFe(4)Sb(12) revealed oxidation at temperatures below operational limits, hindering practical use.
- Improving the thermal stability of these materials is crucial for their widespread adoption.
Purpose of the Study:
- To investigate the effect of substituting larger rare-earth (Eu) and transition-metal (Ru) elements for Ce and Fe in skutterudite materials.
- To determine if these substitutions enhance the oxidation resistance and thermal stability compared to CeFe(4)Sb(12).
- To understand the underlying mechanisms responsible for improved thermal stability.
Main Methods:
- Thermogravimetric Analysis (TGA) to assess weight changes due to oxidation.
- Powder X-ray Diffraction (XRD) to analyze structural changes.
- X-ray Absorption Near Edge Structure (XANES) spectroscopy to probe electronic structure and bonding.
Main Results:
- Substitution of Eu(2+) and Ru(2+) for Ce(3+) and Fe(2+) significantly increased the oxidation temperature compared to CeFe(4)Sb(12).
- The enhanced thermal stability is attributed to increased orbital overlap from larger Eu and Ru atoms, leading to stronger chemical bonds.
- The study demonstrated improved thermal stability in the modified skutterudite materials.
Conclusions:
- Selective elemental substitution is an effective strategy to enhance the thermal stability of rare-earth-filled skutterudites.
- Europium (Eu) and Ruthenium (Ru) substituted skutterudites exhibit superior oxidation resistance, making them more suitable for high-temperature applications.
- These findings pave the way for developing more robust thermoelectric materials for waste heat recovery systems.
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