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Surface Reconstruction for Forming the [IrO6]-[IrO6] Framework: Key Structure for Stable and Activated OER

Cheng-Long Ma1, Zhi-Qiang Wang2, Wei Sun3

  • 1School of Resources and Environmental Engineering, East China University of Science and Technology, 130 Mei Long Road, Shanghai 200237, China.

ACS Applied Materials & Interfaces
|June 21, 2021
PubMed
Summary

Surface reconstruction in iridium oxides (AIrO) enhances oxygen evolution reaction (OER) performance. Lu2Ir2O7 shows superior OER activity due to an improved [IrO6]-[IrO6] framework, boosting electron transport.

Keywords:
Lu2Ir2O7iridium-based derivativesoxygen evolution reactionpyrochloresurface reconstruction

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Iridium-based oxides (AIrO) are known for excellent oxygen evolution reaction (OER) performance, particularly in acidic media.
  • Understanding the electronic state changes during surface reconstruction is crucial for optimizing OER catalysts.
  • The role of specific iridium pyrochlores, like Lu2Ir2O7, in this process requires further investigation.

Purpose of the Study:

  • To synthesize and investigate the underestimated Lu2Ir2O7 for its OER performance.
  • To explore the electronic state changes during surface reconstruction using spectroscopy and computational methods.
  • To elucidate the relationship between electronic structure, surface reconstruction, and OER activity in iridium pyrochlores.

Main Methods:

  • Synthesis of Lu2Ir2O7 and other iridium pyrochlores (Pr2Ir2O7, Eu2Ir2O7).
  • Electrochemical characterization, including electrochemical impedance spectra (EIS).
  • Spectroscopic techniques (X-ray absorption near-edge structure - XANES) and computational methods (density of states - DOS).

Main Results:

  • Four forms of reconstructed pyrochlores were identified during OER, including an intact pyrochlore, a metastable [IrO6]-[IrO6] framework, and an amorphous outer layer.
  • The corner-shared [IrO6]-[IrO6] framework enhances electron transport efficiency, critical for acidic OER.
  • Lu2Ir2O7 exhibited the highest OER performance among the studied Ir-based pyrochlores, with a ninefold increase in Ir-mass activity compared to IrO2, attributed to enhanced Ir-O hybridization and a downshifted d-band center.

Conclusions:

  • The surface reconstruction process in iridium pyrochlores significantly impacts OER performance.
  • The metastable [IrO6]-[IrO6] framework plays a vital role in enhancing electron transport and catalytic activity.
  • Lu2Ir2O7 demonstrates exceptional OER activity, highlighting its potential for water-splitting applications.