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In situ Raman spectroscopy reveals the structure and dissociation of interfacial water

Author

Listed:
  • Yao-Hui Wang

    (Xiamen University)

  • Shisheng Zheng

    (Peking University, Shenzhen Graduate School)

  • Wei-Min Yang

    (Xiamen University)

  • Ru-Yu Zhou

    (Xiamen University)

  • Quan-Feng He

    (Xiamen University)

  • Petar Radjenovic

    (Xiamen University)

  • Jin-Chao Dong

    (Xiamen University)

  • Shunning Li

    (Peking University, Shenzhen Graduate School)

  • Jiaxin Zheng

    (Peking University, Shenzhen Graduate School)

  • Zhi-Lin Yang

    (Xiamen University)

  • Gary Attard

    (University of Liverpool)

  • Feng Pan

    (Peking University, Shenzhen Graduate School)

  • Zhong-Qun Tian

    (Xiamen University
    Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM))

  • Jian-Feng Li

    (Xiamen University
    Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM)
    China Jiliang University)

Abstract

Understanding the structure and dynamic process of water at the solid–liquid interface is an extremely important topic in surface science, energy science and catalysis1–3. As model catalysts, atomically flat single-crystal electrodes exhibit well-defined surface and electric field properties, and therefore may be used to elucidate the relationship between structure and electrocatalytic activity at the atomic level4,5. Hence, studying interfacial water behaviour on single-crystal surfaces provides a framework for understanding electrocatalysis6,7. However, interfacial water is notoriously difficult to probe owing to interference from bulk water and the complexity of interfacial environments8. Here, we use electrochemical, in situ Raman spectroscopic and computational techniques to investigate the interfacial water on atomically flat Pd single-crystal surfaces. Direct spectral evidence reveals that interfacial water consists of hydrogen-bonded and hydrated Na+ ion water. At hydrogen evolution reaction (HER) potentials, dynamic changes in the structure of interfacial water were observed from a random distribution to an ordered structure due to bias potential and Na+ ion cooperation. Structurally ordered interfacial water facilitated high-efficiency electron transfer across the interface, resulting in higher HER rates. The electrolytes and electrode surface effects on interfacial water were also probed and found to affect water structure. Therefore, through local cation tuning strategies, we anticipate that these results may be generalized to enable ordered interfacial water to improve electrocatalytic reaction rates.

Suggested Citation

  • Yao-Hui Wang & Shisheng Zheng & Wei-Min Yang & Ru-Yu Zhou & Quan-Feng He & Petar Radjenovic & Jin-Chao Dong & Shunning Li & Jiaxin Zheng & Zhi-Lin Yang & Gary Attard & Feng Pan & Zhong-Qun Tian & Jian, 2021. "In situ Raman spectroscopy reveals the structure and dissociation of interfacial water," Nature, Nature, vol. 600(7887), pages 81-85, December.
  • Handle: RePEc:nat:nature:v:600:y:2021:i:7887:d:10.1038_s41586-021-04068-z
    DOI: 10.1038/s41586-021-04068-z
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