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

Understanding the structure and dynamic process of water at the solid-liquid interface is an extremely important topic in surface science, energy science and catalysis . As model catalysts, atomically flat single-crystal electrodes exhibit well-defined surface and electric field properties, and ther...

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Bibliographic Details
Published in:Nature (London) 2021-12, Vol.600 (7887), p.81-85A
Main Authors: Wang, Yao-Hui, Zheng, Shisheng, Yang, Wei-Min, Zhou, Ru-Yu, He, Quan-Feng, Radjenovic, Petar, Dong, Jin-Chao, Li, Shunning, Zheng, Jiaxin, Yang, Zhi-Lin, Attard, Gary, Pan, Feng, Tian, Zhong-Qun, Li, Jian-Feng
Format: Article
Language:English
Subjects:
Catalysts
Chemical bonds
Computer applications
Crystal surfaces
Dissociation
Electric fields
Electrochemistry
Electrodes
Electrolytes
Electron transfer
Hydrogen
Hydrogen bonding
Hydrogen evolution reactions
Liquid-solid interfaces
Raman spectroscopy
Single crystals
Sodium
Spectroscopy
Spectrum analysis
Water structure
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Summary:Understanding the structure and dynamic process of water at the solid-liquid interface is an extremely important topic in surface science, energy science and catalysis . 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 level . Hence, studying interfacial water behaviour on single-crystal surfaces provides a framework for understanding electrocatalysis . However, interfacial water is notoriously difficult to probe owing to interference from bulk water and the complexity of interfacial environments . 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.
ISSN:0028-0836
1476-4687
DOI:10.1038/s41586-021-04068-z