Temperature Dependent n-Type Self Doping in Nominally 19-Electron Half-Heusler Thermoelectric Materials

Shashwat Anand, Kaiyang Xia, Tiejun Zhu, Chris Wolverton, Gerald Jeffrey Snyder*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

22 Scopus citations

Abstract

The discovery of a semiconducting ground state XyYZ (y = 0.8 or 0.75) in nominally 19-electron half-Heusler materials warrants a closer look at their apparently metallic properties that often make them good thermoelectric (TE) materials. By systematically investigating the temperature dependence of off-stoichiometry (x) in V0.8+ xCoSb, Nb0.8+ xCoSb, and Ti0.75+ xNiSb it is found that x invariably increases with increasing temperature, leading to an n-type self-doping behavior. In addition, there is also a large phase width (range of x) associated with each phase that is temperature dependent. Thus, unlike in typical 18-electron half-Heuslers (e,g, TiNiSn), the temperature dependence of vacancy and carrier concentration (n) in nominally 19-electron half-Heuslers links its transport properties to synthesis conditions. The temperature dependence of x and n are understood using density functional theory based defect energies (Ed) and phase diagrams. Ed are calculated for 21 systems which can be used in predicting solubility in this family of compounds. Using this simple strategy, suitable composition and temperature synthesis conditions are devised for obtaining an optimized n to engineer TE properties in phase-pure V0.8+ xCoSb, and the previously unexplored Ta0.8+ xCoSb.

Original languageEnglish (US)
Article number1801409
JournalAdvanced Energy Materials
Volume8
Issue number30
DOIs
StatePublished - Oct 25 2018

Keywords

  • 19-electron half-Heuslers
  • NbCoSb
  • VCoSb
  • defects
  • vacancy

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

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