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Enhanced electronic conductivity by controlled self-doping in pyrochlores.

Haiyan Xiao1, Yanwen Zhang, William J Weber

  • 1Department of Materials Science & Engineering, University of Tennessee, Knoxville, TN 37996, USA. hxiao@utk.edu

Physical Chemistry Chemical Physics : PCCP
|March 30, 2012
PubMed
Summary

Introducing excess titanium interstitials into Y(2)Ti(2)O(7) pyrochlores induces a semiconductor-to-metal transition. This finding offers a new method for tuning pyrochlore oxides for applications like solid oxide fuel cells.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Condensed Matter Physics

Background:

  • Most 5d transition-metal (TM) pyrochlores are metallic.
  • 3d and 4d TM pyrochlores typically behave as semiconductors or insulators.
  • Controlling electronic conductivity in pyrochlores is crucial for applications.

Purpose of the Study:

  • To investigate the semiconductor-to-metal transition in Y(2)Ti(2)O(7) pyrochlores.
  • To understand the role of titanium interstitials in altering electronic properties.
  • To explore methods for tuning pyrochlore conductivity for electrochemical devices.

Main Methods:

  • Synthesis of Y(2)Ti(2)O(7) with excess Ti interstitials.
  • Characterization of interstitial site preference (anion vacant 8a or <010> bridge sites).
  • Density functional theory (DFT) calculations to model electronic structure and conductivity.

Main Results:

  • Excess Ti interstitials were successfully introduced into Y(2)Ti(2)O(7).
  • Ti interstitials preferentially occupy specific crystallographic sites.
  • DFT calculations confirmed that Ti interstitials enhance electronic conductivity through cation interactions.
  • A semiconductor-to-metal transition was observed.

Conclusions:

  • Introducing Ti interstitials is an effective strategy to induce metallic behavior in semiconducting pyrochlore oxides.
  • The electronic interplay between Ti interstitials and neighboring cations drives the conductivity enhancement.
  • This approach provides a pathway for tuning pyrochlore electronic properties for solid oxide fuel cells and other electrochemical applications.