High-temperature order/disorder transition in the thermoelectric Cu3SbSe3

Abstract

We report the results of an investigation on the structural evolution of a potential new thermoelectric material, Cu3SbSe3, as a function of temperature from 25 to 390 °C. From high-temperature x-ray diffraction data, the refined lattice parameters were seen to change nonlinearly, but continuously, with temperature, with an increased rate of thermal expansion in the a and b lattice parameters from around 125 °C to 175 °C and negative thermal expansion in the c axis from around 100 °C to 175 °C. Crystallographic charge flipping analysis indicated an increase in the disorder of the copper cations with temperature. This reversible order/disorder phase transition in Cu3SbSe3 affects the transport properties, as evidenced by thermal conductivity measurements, which change from negative to positive slope at the transition temperature. This structural change in Cu3SbSe3 has implications for its potential use in thermoelectric generators.

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ACKNOWLEDGMENTS

Sample synthesis at Michigan State University was supported by the National Science Foundation under award number NSH-CBET-0754029. Characterization research at Oak Ridge National Laboratory was sponsored by the Center on Revolutionary Materials for Solid State Energy Conversion, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001054 and by Oak Ridge National Laboratory’s High Temperature Materials Laboratory, sponsored by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program.

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Correspondence to Melanie Kirkham.

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Kirkham, M., Majsztrik, P., Skoug, E. et al. High-temperature order/disorder transition in the thermoelectric Cu3SbSe3. Journal of Materials Research 26, 2001–2005 (2011). https://doi.org/10.1557/jmr.2011.43

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