Enhancing the Thermoelectric Properties via Modulation of Defects in P-Type MNiSn-Based (M = Hf, Zr, Ti) Half-Heusler Materials

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Xin Ai - , Chair of Metallic Materials and Metal Physics, Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Binghua Lei - , University of Missouri (Author)
  • Magdalena O. Cichocka - , Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Lars Giebeler - , Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Ruben Bueno Villoro - , Max Planck Institute for Iron Research (Author)
  • Siyuan Zhang - , Max Planck Institute for Iron Research (Author)
  • Christina Scheu - , Max Planck Institute for Iron Research (Author)
  • Nicolás Pérez - , Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Qihao Zhang - , Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Andrei Sotnikov - , Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • David J. Singh - , University of Missouri (Author)
  • Kornelius Nielsch - , Chair of Metallic Materials and Metal Physics, Institute of Applied Physics, Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Ran He - , Leibniz Institute for Solid State and Materials Research Dresden (Author)

Abstract

The thermoelectric figure-of-merit (zT) of p-type MNiSn (M = Ti, Zr, or Hf) half-Heusler compounds is lower than their n-type counterparts due to the presence of a donor in-gap state caused by Ni occupying tetrahedral interstitials. While ZrNiSn and TiNiSn, have been extensively studied, HfNiSn remains unexplored. Herein, this study reports an improved thermoelectric property in p-type HfNi1−xCoxSn. By doping 5 at% Co at the Ni sites, the Seebeck coefficient becomes reaching a peak value exceeding 200 µV K−1 that breaks the record of previous reports. A maximum power factor of ≈2.2 mW m−1 K−2 at 973 K is achieved by optimizing the carrier concentration. The enhanced p-type transport is ascribed to the reduced content of Ni defects, supported by first principle calculations and diffraction pattern refinement. Concomitantly, Co doping also softens the lattice and scatters phonons, resulting in a minimum lattice thermal conductivity of ≈1.8 W m−1 K−1. This leads to a peak zT of 0.55 at 973 K is realized, surpassing the best performing p-type MNiSn by 100%. This approach offers a new method to manipulate the intrinsic atomic disorder in half-Heusler materials, facilitating further optimization of their electronic and thermal properties.

Details

Original languageEnglish
Article number2305582
JournalAdvanced functional materials
Volume33
Issue number48
Publication statusPublished - 23 Nov 2023
Peer-reviewedYes

Keywords

Keywords

  • half-Heusler, interstitial defects, mechanical alloying, p-type HfNiSn, thermoelectrics