Title:
Chemical tuning of thermal expansion in oxides
Chemical tuning of thermal expansion in oxides
Author(s)
Ruschman, Chad
Advisor(s)
Wilkinson, Angus P.
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Abstract
This work focuses on the chemical substitution of cations and anions in the frameworks of materials that have been known to exhibit negative thermal expansion (NTE). Zr2(PO4)2(SO4) is a member of the A(2)M(3)O(12) family which has been known to exhibit NTE. We have shown that Zr2(PO4)2(SO4) exhibits anisotropic positive thermal expansion. We have also shown that this material has been characterized in the wrong space group. Hf2(PO4)2(SO4) behaves similarly to Zr2(PO4)2(SO4) and follows this trend. Under pressure, Hf2(PO4)2(SO4) appears to undergo a phase transition. We have still yet to determine what space group the materials transitions to. While many members of the AX(2)O(7) family of frameworks have been fully characterized, the thermal expansion of PbP2O7 has yet to be reported. We were unable to obtain a reproducible procedure for synthesis of PbP2O7 from its precursor. Finally, variable temperature and variable pressure studies were performed on ZrMo2O8 in an attempt to learn more about the local structure. We found that space groups P213 and Pa-3 gave poor fits of the local structure at low r. Behavior of the nearest neighbor Zr-Mo distance was very similar to the bulk CTE. On compression, pressure induced amorphization is observed in ZrMo2O8. All interatomic correlations above 4 angstroms are washed out. Zr-O-Mo linkages remain well defined and do not massively deform as the pressure is increased. Finally, we we observed that Zr-O-Mo linkages change geometry reversibly as the pressure is increased.
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Date Issued
2010-05-20
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