Prediction of new stable compounds and promising thermoelectrics in the cu-Sb-Se system

Yongsheng Zhang, Vidvuds Ozoliniņš, Donald Morelli, C. Wolverton

Research output: Contribution to journalArticle

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Abstract

We study the phase stability and predict as-yet-unreported compounds in the thermoelectric Cu-Sb-Se ternary system. We use a combination of total energies obtained from density-functional-theory-based (DFT) calculations with vibrational entropies from phonon calculations (within the harmonic approximation) and configurational entropies, treated with cluster expansions (CE). The Cu-Sb-Se ternary phase diagram is determined (treating all phases as line compounds) using the grand-canonical linear programming method. We find the following results: (1) we predict the stability of a new previously unknown, zinc blende-based Cu4SbSe5 compound but find that it is thermodynamically stable up to only ∼300 K; (2) we also predict that a Cu12Sb4Se13 phase (isostructural with Cu 12Sb4S13, but unreported in the Cu-Sb-Se system) appears in the phase diagram at high temperatures (but below the temperatures where the observed Cu3SbSe3 phase is stable); (3) based on quasi-harmonic phonon and band structure calculations, we find that Cu12Sb4Se13 has thermal conductivity and an electronic structure that suggests it as a promising thermoelectric material.

LanguageEnglish (US)
Pages3427-3435
Number of pages9
JournalChemistry of Materials
Volume26
Issue number11
DOIs
StatePublished - Jun 10 2014

Profile

Phase diagrams
Entropy
Phase stability
Ternary systems
Band structure
Linear programming
Electronic structure
Density functional theory
Zinc
Thermal conductivity
Temperature

ASJC Scopus subject areas

  • Materials Chemistry
  • Chemical Engineering(all)
  • Chemistry(all)

Cite this

Prediction of new stable compounds and promising thermoelectrics in the cu-Sb-Se system. / Zhang, Yongsheng; Ozoliniņš, Vidvuds; Morelli, Donald; Wolverton, C.

In: Chemistry of Materials, Vol. 26, No. 11, 10.06.2014, p. 3427-3435.

Research output: Contribution to journalArticle

Zhang Y, Ozoliniņš V, Morelli D, Wolverton C. Prediction of new stable compounds and promising thermoelectrics in the cu-Sb-Se system. Chemistry of Materials. 2014 Jun 10;26(11):3427-3435. Available from, DOI: 10.1021/cm5006828
Zhang, Yongsheng ; Ozoliniņš, Vidvuds ; Morelli, Donald ; Wolverton, C./ Prediction of new stable compounds and promising thermoelectrics in the cu-Sb-Se system. In: Chemistry of Materials. 2014 ; Vol. 26, No. 11. pp. 3427-3435
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