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Recent advances in Raman spectroelectrochemistry on single-crystal surfaces

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Abstract

Benefiting from a principally contaminant-free and well-defined surface, single-crystal electrodes offer new insights into interfacial processes and are important in electrochemistry. The early impetus for using single-crystal electrodes in electro-catalysis was to investigate the surface structure at the atomic level for the reactions that are sensitive to the surface. These studies were usually performed in an ultra-high vacuum with atomic force microscopy (AFM), scanning tunneling microscope (STM), and X-ray methods to avoid the contamination. However, such characterizations are limited in their ability to identify chemical species definitively, a limitation that has similarly plagued the study of single-crystals. Recent advances in shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) have enabled the detection of reaction intermediates on single-crystal electrodes, in which shell-isolated nanoparticles on the single-crystal electrode can enhance the Raman signal from the surface, without changing the surface structure and electrochemical response. Thus, this work aims to review recent advances in Raman spectroelectrochemical studies on single-crystal electrode surfaces. The discussion focuses on how SHINERS technology has enabled the effective detection of intermediate species and, when combined with the electrochemical method, has yielded novel insights into the dynamic evolution of surface structure and electrocatalytic reaction mechanisms. Finally, the challenges and future of single-crystal electrodes are introduced.

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Acknowledgements

This work was supported by the National Key Research and Development Program of China (2020YFB1505800), the National Natural Science Foundation of China (21925404, 22005130, and 21991151), and the China Postdoctoral Science Foundation (BX20220187).

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Authors and Affiliations

  1. State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, College of Energy, iChEM, Xiamen University, Xiamen, 361005, China

    Quan-Feng He, Jin-Chao Dong & Jian-Feng Li

  2. Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen, 361005, China

    Quan-Feng He & Jian-Feng Li

  3. Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences, University of Chinese Academy of Sciences, Beijing, 100190, China

    Jia Yu

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  1. Quan-Feng He
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Correspondence to Jia Yu or Jian-Feng Li.

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He, QF., Yu, J., Dong, JC. et al. Recent advances in Raman spectroelectrochemistry on single-crystal surfaces. Sci. China Chem. 66, 3360–3371 (2023). https://doi.org/10.1007/s11426-023-1682-x

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