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Activation of surface oxygen sites on an iridium-based model catalyst for the oxygen evolution reaction

Author

Listed:
  • Alexis Grimaud

    (Chimie du Solide et de l’Energie
    Réseau sur le Stockage Electrochimique de l’Energie (RS2E))

  • Arnaud Demortière

    (Réseau sur le Stockage Electrochimique de l’Energie (RS2E)
    Laboratoire de Réactivité et Chimie des Solides)

  • Matthieu Saubanère

    (Chimie du Solide et de l’Energie
    Réseau sur le Stockage Electrochimique de l’Energie (RS2E)
    Institut Charles Gerhardt, CNRS UMR 5253, Université Montpellier)

  • Walid Dachraoui

    (Réseau sur le Stockage Electrochimique de l’Energie (RS2E)
    Laboratoire de Réactivité et Chimie des Solides)

  • Martial Duchamp

    (Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons (ER-C) and Peter Grünberg Institute (PGI))

  • Marie-Liesse Doublet

    (Réseau sur le Stockage Electrochimique de l’Energie (RS2E)
    Institut Charles Gerhardt, CNRS UMR 5253, Université Montpellier)

  • Jean-Marie Tarascon

    (Chimie du Solide et de l’Energie
    Réseau sur le Stockage Electrochimique de l’Energie (RS2E)
    ALISTORE-European Research Institute
    Sorbonne Universités—UPMC Univ Paris 06)

Abstract

The oxygen evolution reaction (OER) is of prime importance in multiple energy storage devices; however, deeper mechanistic understanding is required to design enhanced electrocatalysts for the reaction. Current understanding of the OER mechanism based on oxygen adsorption on a metallic surface site fails to fully explain the activity of iridium and ruthenium oxide surfaces, and the drastic surface reconstruction observed for the most active OER catalysts. Here we demonstrate, using La2LiIrO6 as a model catalyst, that the exceptionally high activity found for Ir-based catalysts arises from the formation of active surface oxygen atoms that act as electrophilic centres for water to react. Moreover, with the help of transmission electron microscopy, we observe drastic surface reconstruction and iridium migration from the bulk to the surface. Therefore, we establish a correlation between surface activity and surface stability for OER catalysts that is rooted in the formation of surface reactive oxygen.

Suggested Citation

  • Alexis Grimaud & Arnaud Demortière & Matthieu Saubanère & Walid Dachraoui & Martial Duchamp & Marie-Liesse Doublet & Jean-Marie Tarascon, 2017. "Activation of surface oxygen sites on an iridium-based model catalyst for the oxygen evolution reaction," Nature Energy, Nature, vol. 2(1), pages 1-10, January.
    • Handle: RePEc:nat:natene:v:2:y:2017:i:1:d:10.1038_nenergy.2016.189
    DOI: 10.1038/nenergy.2016.189
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    Cited by:

    1. Siran Xu & Sihua Feng & Yue Yu & Dongping Xue & Mengli Liu & Chao Wang & Kaiyue Zhao & Bingjun Xu & Jia-Nan Zhang, 2024. "Dual-site segmentally synergistic catalysis mechanism: boosting CoFeSx nanocluster for sustainable water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Gyu Rac Lee & Jun Kim & Doosun Hong & Ye Ji Kim & Hanhwi Jang & Hyeuk Jin Han & Chang-Kyu Hwang & Donghun Kim & Jin Young Kim & Yeon Sik Jung, 2023. "Efficient and sustainable water electrolysis achieved by excess electron reservoir enabling charge replenishment to catalysts," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Fan Liao & Kui Yin & Yujin Ji & Wenxiang Zhu & Zhenglong Fan & Youyong Li & Jun Zhong & Mingwang Shao & Zhenhui Kang & Qi Shao, 2023. "Iridium oxide nanoribbons with metastable monoclinic phase for highly efficient electrocatalytic oxygen evolution," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    4. Shu-Pei Zeng & Hang Shi & Tian-Yi Dai & Yang Liu & Zi Wen & Gao-Feng Han & Tong-Hui Wang & Wei Zhang & Xing-You Lang & Wei-Tao Zheng & Qing Jiang, 2023. "Lamella-heterostructured nanoporous bimetallic iron-cobalt alloy/oxyhydroxide and cerium oxynitride electrodes as stable catalysts for oxygen evolution," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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