The Effect of Structural Vacancies on the Thermoelectric Properties of (Cu2Te)1-x(Ga2Te3)x

Journal Article · Tue Jan 01 00:00:00 EST 2013 · Journal of Solid State Chemistry

DOI:https://doi.org/10.1016/j.jssc.2013.02.008· OSTI ID:1087468

Ye, Zuxin ^[1]; Cho, Jung Y ^[2]; Tessema, Misle ^[1]; Salvador, James R. ^[2]; Waldo, Richard ^[2]; Wang, Hsin ^[3]; Cai, Wei ^[3]

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1. GM Research and Development Center
2. GM R&D and Planning, Warren, Michigan
3. ORNL

We have studied the effects of structural vacancies on the thermoelectric properties of the ternary compounds (Cu2Te)1-x(Ga2Te3)x (x = 0.5, 0.55, 0.571, 0.6, 0.625, 0.667 and 0.75), which are solid solutions found in the pseudo-binary phase diagram for Cu2Te and Ga2Te3. This system possesses tunable structural vacancy concentrations. The x= 0.5 phase, CuGaTe2, is nominally devoid of structural vacancies, while the rest of the compounds contain varying amounts of these features, and the volume density of vacancies increases with Ga2Te3 content. The sample with x = 0.5, 0.55, 0.571, 0.6, 0.625 crystallize in the chalcopyrite structure while the x = 0.667 and 0.75 adopt the Ga2Te3 defect zinc blende structure. Strong scattering of heat carrying phonons by structural defects, leads to the reduction of thermal conductivity, which is beneficial to the thermoelectric performance of materials. On the other hand, these defects also scatter charge carriers and reduce the electrical conductivity. All the samples investigated are p-type semiconductors as inferred by the signs of their respective Hall (RH) and Seebeck (S) coefficients. The structural vacancies were found to scatter phonons strongly, while a combination of increased carrier concentration, and vacancies decreases the Hall mobility ( H), degrading the overall thermoelectric performance. The room temperature H drops from 90 cm2/V s for CuGaTe2 to 13 cm2/V s in Cu9Ga11Te21 and 4.6 cm2/V s in CuGa3Te5. The low temperature thermal conductivity decreases significantly with higher Ga2Te3 concentrations (higher vacancy concentration) due to increased point defect scattering which dominate thermal resistance terms. At high temperatures, the dependence of thermal conductivity on the Ga2Te3 content is less significant. The presence of strong Umklapp scattering leads to low thermal conductivity at high temperatures for all samples investigated. The highest ZT among the samples in this study was found for the defect-free CuGaTe2 with ZT ~ 1.0 at 840K.

• Research Organization: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
• Sponsoring Organization: Work for Others (WFO)
• DOE Contract Number: DE-AC05-00OR22725
• OSTI ID: 1087468
• Journal Information: Journal of Solid State Chemistry, Vol. 201; ISSN 0022-4596
• Country of Publication: United States
• Language: English

Related Subjects

thermoelectric