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Tin-Substituted Chalcopyrite: An n-Type Sulfide with Enhanced Thermoelectric Performance.

Sahil Tippireddy1, Feridoon Azough2, Vikram1

  • 1Department of Chemistry, University of Reading, Whiteknights, Reading RG6 6DX, United Kingdom.

Chemistry of Materials : a Publication of the American Chemical Society
|July 18, 2022
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Summary

Tin substitution in n-type chalcopyrite (CuFeS2) significantly enhances thermoelectric performance. This study demonstrates a 300% increase in the figure-of-merit (zT) for thermoelectric devices by optimizing material properties.

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Area of Science:

  • Materials Science
  • Solid State Physics
  • Thermoelectrics

Background:

  • N-type sulfides are scarce, hindering all-sulfide thermoelectric device fabrication.
  • Chalcopyrite (CuFeS2) is a rare n-type sulfide with potential for thermoelectric applications.

Purpose of the Study:

  • To enhance the thermoelectric performance of chalcopyrite (CuFeS2) via tin (Sn) substitution.
  • To investigate the mechanisms behind performance enhancement in Cu1-xSnxFeS2.

Main Methods:

  • Chemical substitution to synthesize Cu1-xSnxFeS2 (0 ≤ x ≤ 0.1).
  • Transmission electron microscopy (TEM) for microstructural analysis.
  • Density functional theory (DFT) calculations and X-ray photoelectron spectroscopy (XPS) for electronic structure analysis.

Main Results:

  • Tin substitution induced mass/strain fluctuations, lattice softening, and enhanced phonon scattering.
  • Substituted materials maintained high Seebeck coefficient and charge-carrier mobility, improving the power factor threefold.
  • Small polaron formation, confirmed by DFT and XPS, limited carrier concentration and reduced lattice thermal conductivity by up to 40%.

Conclusions:

  • Tin substitution in chalcopyrite effectively enhances thermoelectric properties.
  • Optimized Cu0.96Sn0.04FeS2 achieved a figure-of-merit (zT) of approximately 0.3 at 673 K, a 300% improvement.
  • This work provides a viable strategy for developing high-performance n-type sulfide thermoelectrics.