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Thermoelectric Properties of CoSb3-Based Skutterudites

Thesis advisor: Zhifeng Ren / Solid state cooling and power generation based on thermoelectric principles are regarded as one of the technologies with the potential of solving the current energy crisis. Thermoelectric devices could be widely used in waste heat recovery, small scale power generation and refrigeration. It has no moving parts and is environmental friendly. The limitation to its application is due to its low efficiency. Most of the current commercialized thermoelectric materials have figure of merit (ZT) around 1. To be comparable with kitchen refrigerator, ZT is required at room temperature. Skutterudites have emerged as member of the novel materials, which potentially have a higher ZT. In the dissertation, my investigation will be focused on the optimization of CoSb<sub>3</sub> &ndash based skutterudites. Starting with Co and Sb elements, CoSb<sub>3</sub> will form through a high energy ball mill. Unfortunately, even after 20 hours, only a small percentage of the powders have transformed in into CoSb<sub>3</sub>. Then the powders will be compacted into bulk samples by DC-controlled hot press. CoSb<sub>3</sub> single phase will form after press. Characterization of the structure and thermoelectric properties will be presented with details. The effects of synthesis conditions on thermoelectric properties of skutterudites were studied and discussed. Several possible methods of improving the ZT of N type skutterudites were applied. The highest obtained ZT thus far is about 1.2 from Yb doped CoSb<sub>3</sub>. For a group of samples with nominal composition Yb<sub>x</sub>Co<sub>4</sub>Sb<sub>12</sub>, the increased Yb concentration in our samples not only enhanced the power factor due to electron doping effect but also decreased the thermal conductivity due to a stronger rattling effect. In addition, the increased grain boundary density per unit volume due to the small grains in our bulk skutterudite materials may have also helped to enhance the phonon scattering and thus to reduce the thermal conductivity. Single and double doping methods with different combinations were also tried. So far, none of them have surpassed ZT of 1.2. Mixing different materials with Yb<sub>0.35</sub>Co<sub>4</sub>Sb<sub>12</sub> so far to increase the phonon scattering was also performed. No dramatic thermal conductivity reduction was observed. Small amounts of Fe/Mn substitution on Co sites will decrease the power factor to undesired degrees. Some results with Nd filled P type sample will be briefly introduced. P type samples are also obtained through substitution on Sb site. Preliminary work on preparing the electrode for CoSb<sub>3</sub> will be presented in the dissertation. CoSi<sub>2</sub> has low resistivity, and a similar coefficient of thermal expansion (CTE) as of doped CoSb<sub>3</sub>. It is good electrode candidate. DC controlled hot press is used to make the contact. Thermal stability of the contact was tested. Small cracks will form in the contact area, further improvement is necessary. Finally, my previous work on ZnO nanowire growth is briefly introduced. Large throughput of ZnO nanowire could be obtained with NaCl as the support to promote the conversion of Zn powder to ZnO. / Thesis (PhD) — Boston College, 2010. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.

Identiferoai:union.ndltd.org:BOSTON/oai:dlib.bc.edu:bc-ir_101841
Date January 2010
CreatorsYang, Jian
PublisherBoston College
Source SetsBoston College
LanguageEnglish
Detected LanguageEnglish
TypeText, thesis
Formatelectronic, application/pdf
RightsCopyright is held by the author, with all rights reserved, unless otherwise noted.

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