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In situ Raman spectroscopic evidence for oxygen reduction reaction intermediates at platinum single-crystal surfaces

Author

Listed:
  • Jin-Chao Dong

    (Xiamen University)

  • Xia-Guang Zhang

    (Xiamen University)

  • Valentín Briega-Martos

    (Universidad de Alicante)

  • Xi Jin

    (Xiamen University)

  • Ji Yang

    (Xiamen University)

  • Shu Chen

    (Xiamen University)

  • Zhi-Lin Yang

    (Xiamen University)

  • De-Yin Wu

    (Xiamen University)

  • Juan Miguel Feliu

    (Universidad de Alicante)

  • Christopher T. Williams

    (University of South Carolina)

  • Zhong-Qun Tian

    (Xiamen University)

  • Jian-Feng Li

    (Xiamen University
    Xiamen University
    Shenzhen Research Institute of Xiamen University)

Abstract

Developing an understanding of structure–activity relationships and reaction mechanisms of catalytic processes is critical to the successful design of highly efficient catalysts. As a fundamental reaction in fuel cells, elucidation of the oxygen reduction reaction (ORR) mechanism at Pt(hkl) surfaces has remained a significant challenge for researchers. Here, we employ in situ electrochemical surface-enhanced Raman spectroscopy (SERS) and density functional theory (DFT) calculation techniques to examine the ORR process at Pt(hkl) surfaces. Direct spectroscopic evidence for ORR intermediates indicates that, under acidic conditions, the pathway of ORR at Pt(111) occurs through the formation of HO2*, whereas at Pt(110) and Pt(100) it occurs via the generation of OH*. However, we propose that the pathway of the ORR under alkaline conditions at Pt(hkl) surfaces mainly occurs through the formation of O2−. Notably, these results demonstrate that the SERS technique offers an effective and reliable way for real-time investigation of catalytic processes at atomically flat surfaces not normally amenable to study with Raman spectroscopy.

Suggested Citation

  • Jin-Chao Dong & Xia-Guang Zhang & Valentín Briega-Martos & Xi Jin & Ji Yang & Shu Chen & Zhi-Lin Yang & De-Yin Wu & Juan Miguel Feliu & Christopher T. Williams & Zhong-Qun Tian & Jian-Feng Li, 2019. "In situ Raman spectroscopic evidence for oxygen reduction reaction intermediates at platinum single-crystal surfaces," Nature Energy, Nature, vol. 4(1), pages 60-67, January.
  • Handle: RePEc:nat:natene:v:4:y:2019:i:1:d:10.1038_s41560-018-0292-z
    DOI: 10.1038/s41560-018-0292-z
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    Citations

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    Cited by:

    1. Rubén Rizo & Julia Fernández-Vidal & Laurence J. Hardwick & Gary A. Attard & Francisco J. Vidal-Iglesias & Victor Climent & Enrique Herrero & Juan M. Feliu, 2022. "Investigating the presence of adsorbed species on Pt steps at low potentials," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    2. Tianyu Zhang & Jing Jin & Junmei Chen & Yingyan Fang & Xu Han & Jiayi Chen & Yaping Li & Yu Wang & Junfeng Liu & Lei Wang, 2022. "Pinpointing the axial ligand effect on platinum single-atom-catalyst towards efficient alkaline hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    3. Jiannan Du & Guokang Han & Wei Zhang & Lingfeng Li & Yuqi Yan & Yaoxuan Shi & Xue Zhang & Lin Geng & Zhijiang Wang & Yueping Xiong & Geping Yin & Chunyu Du, 2023. "CoIn dual-atom catalyst for hydrogen peroxide production via oxygen reduction reaction in acid," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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