Phase Stability, Crystal Structure, and Thermoelectric Properties of Cu12Sb4S13–xSex Solid Solutions

Lu, Xu; Morelli, Donald T.; Wang, Yuxing; Lai, Wei; Xia, Yi; Ozolins, Vidvuds

doi:10.1021/acs.chemmater.5b04796

Title: Phase Stability, Crystal Structure, and Thermoelectric Properties of Cu₁₂Sb₄S_13–xSe_x Solid Solutions

Journal Article · Fri Feb 19 00:00:00 EST 2016 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.5b04796· OSTI ID:1370337

Lu, Xu ^[1]; Morelli, Donald T. ^[2]; Wang, Yuxing ^[2]; Lai, Wei ^[2]; Xia, Yi ^[3]; Ozolins, Vidvuds ^[3]

Chongqing Univ. (China); Michigan State Univ., East Lansing, MI (United States)
Michigan State Univ., East Lansing, MI (United States)
Univ. of California, Los Angeles, CA (United States)

The solubility of selenium on the sulfur site in tetrahedrite Cu₁₂Sb₄S₁₃ has been explored by theoretical calculations here, and the results have been verified by X-ray diffraction and X-ray synchrotron studies on Cu₁₂Sb₄S_13–xSe_x with x ranging from zero to 3. Density-functional theory calculations predict that Se substitution on the tetrahedral 24g site is preferred, and this is found to be consistent with Rietveld refinement of the crystal structure. High temperature thermoelectric property measurements on Cu₁₂Sb₄S_13-xSe_x reveal that Se substitution results in a decrease in electrical resistivity without diminution of the Seebeck coefficient. The “decoupling” of these parameters leads to a 30% enhancement in power factor of the x = 1 sample compared to that of pure Cu₁₂Sb₄S₁₃. Furthermore, in spite of an increased electronic thermal conductivity, alloy scattering of phonons caused by Se substitution reduces both the lattice and total thermal conductivities, leading to a large increase in the thermoelectric figure of merit.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001054; AC02-06CH11357; AC02-05CH11231

OSTI ID:: 1370337

Journal Information:: Chemistry of Materials, Vol. 28, Issue 6; Related Information: RMSSEC partners with Michigan State University (lead); University of California, Los Angeles; University of Michigan; Northwestern University; Oak Ridge National Laboratory; Ohio State University; Wayne State University; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 73 works

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