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

    • 27 Citations

    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.

    Original languageEnglish (US)
    Pages (from-to)3427-3435
    Number of pages9
    JournalChemistry of Materials
    Volume26
    Issue number11
    DOIs
    StatePublished - Jun 10 2014

    Profile

    Community Psychiatry
    Acetanilides
    Cardenolides
    Hemophilia A
    Phase diagrams
    Entropy
    Temperature
    Joint Loose Bodies
    Bibliography of Medicine
    Dairying
    Saimiriine herpesvirus 2
    Traffic Accidents
    Ternary systems
    Band structure
    Linear programming
    Electronic structure
    Density functional theory
    Phase stability
    Thermal conductivity
    Zinc

    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, Vol. 26, No. 11, 10.06.2014, p. 3427-3435.

    Research output: Contribution to journalArticle

    @article{dbad49aa62554fe9b3dc88a3d352af47,
    title = "Prediction of new stable compounds and promising thermoelectrics in the cu-Sb-Se system",
    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.",
    author = "Yongsheng Zhang and Vidvuds Ozoliniņš and Donald Morelli and C. Wolverton",
    year = "2014",
    month = "6",
    doi = "10.1021/cm5006828",
    volume = "26",
    pages = "3427--3435",
    journal = "Chemistry of Materials",
    issn = "0897-4756",
    publisher = "American Chemical Society",
    number = "11",

    }

    TY - JOUR

    T1 - Prediction of new stable compounds and promising thermoelectrics in the cu-Sb-Se system

    AU - Zhang,Yongsheng

    AU - Ozoliniņš,Vidvuds

    AU - Morelli,Donald

    AU - Wolverton,C.

    PY - 2014/6/10

    Y1 - 2014/6/10

    N2 - 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.

    AB - 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.

    UR - http://www.scopus.com/inward/record.url?scp=84902189705&partnerID=8YFLogxK

    UR - http://www.scopus.com/inward/citedby.url?scp=84902189705&partnerID=8YFLogxK

    U2 - 10.1021/cm5006828

    DO - 10.1021/cm5006828

    M3 - Article

    VL - 26

    SP - 3427

    EP - 3435

    JO - Chemistry of Materials

    T2 - Chemistry of Materials

    JF - Chemistry of Materials

    SN - 0897-4756

    IS - 11

    ER -