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Fast vacancy-mediated oxygen ion incorporation across the ceria–gas electrochemical interface

Author

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  • Zhuoluo A. Feng

    (Stanford University
    Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory)

  • Farid El Gabaly

    (Sandia National Laboratories)

  • Xiaofei Ye

    (Stanford University)

  • Zhi-Xun Shen

    (Stanford University
    Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory)

  • William C. Chueh

    (Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory
    Sandia National Laboratories
    Stanford University)

Abstract

Electrochemical incorporation reactions are ubiquitous in energy storage and conversion devices based on mixed ionic and electronic conductors, such as lithium-ion batteries, solid-oxide fuel cells and water-splitting membranes. The two-way traffic of ions and electrons across the electrochemical interface, coupled with the bulk transport of mass and charge, has been challenging to understand. Here we report an investigation of the oxygen-ion incorporation pathway in CeO2-δ (ceria), one of the most recognized oxygen-deficient compounds, during hydrogen oxidation and water splitting. We probe the response of surface oxygen vacancies, electrons and adsorbates to the electrochemical polarization at the ceria–gas interface. We show that surface oxygen-ion transfer, mediated by oxygen vacancies, is fast. Furthermore, we infer that the electron transfer between cerium cations and hydroxyl ions is the rate-determining step. Our in operando observations reveal the precise roles of surface oxygen vacancy and electron defects in determining the rate of surface incorporation reactions.

Suggested Citation

  • Zhuoluo A. Feng & Farid El Gabaly & Xiaofei Ye & Zhi-Xun Shen & William C. Chueh, 2014. "Fast vacancy-mediated oxygen ion incorporation across the ceria–gas electrochemical interface," Nature Communications, Nature, vol. 5(1), pages 1-9, September.
    • Handle: RePEc:nat:natcom:v:5:y:2014:i:1:d:10.1038_ncomms5374
    DOI: 10.1038/ncomms5374
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    Cited by:

    1. Xin Chen & Junxiang Chen & Huayu Chen & Qiqi Zhang & Jiaxuan Li & Jiwei Cui & Yanhui Sun & Defa Wang & Jinhua Ye & Lequan Liu, 2023. "Promoting water dissociation for efficient solar driven CO2 electroreduction via improving hydroxyl adsorption," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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