In Situ SHINERS at Electrochemical Single-Crystal Electrode/Electrolyte Interfaces: Tuning Preparation Strategies and Selected Applications

Li, Jian-Feng; Rudnev, Alexander; Fu, Yongchun; Bodappa, Nataraju; Wandlowski, Thomas (2013). In Situ SHINERS at Electrochemical Single-Crystal Electrode/Electrolyte Interfaces: Tuning Preparation Strategies and Selected Applications. ACS nano, 7(10), pp. 8940-8952. American Chemical Society 10.1021/nn403444j

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We have studied Au(55 nm)@SiO2 nanoparticles (NPs) on two low-index phases of gold and platinum single crystal electrodes in ClO4– and SO42– ion-containing electrolytes by both electrochemical methods and in-situ shell-isolated nanoparticle enhanced Raman spectroscopy (SHINERS). We showed the blocking of the electrode with surfactants originating from the synthesis of as-prepared SHINERS NPs. We introduce an efficient procedure to overcome this problem, which provides a fundamental platform for the application of SHINERS in surface electrochemistry and beyond. Our method is based on a hydrogen evolution treatment of the SHINERS-NP-modified single-crystal surfaces. The reliability of our preparation strategy is demonstrated in electrochemical SHINERS experiments on the potential-controlled adsorption and phase formation of pyridine on Au(hkl) and Pt(hkl). We obtained high-quality Raman spectra on these well-defined and structurally carefully characterized single-crystal surfaces. The analysis of the characteristic A1 vibrational modes revealed perfect agreement with the interpretation of single-crystal voltammetric and chronoamperometric experiments. Our study demonstrates that the SHINERS protocol developed in this work qualifies this Raman method as a pioneering approach with unique opportunities for in situ structure and reactivity studies at well-defined electrochemical solid/liquid interfaces.

Item Type:

Journal Article (Original Article)

Division/Institute:

08 Faculty of Science > Departement of Chemistry and Biochemistry

UniBE Contributor:

Li, Jianfeng; Rudnev, Alexander; Fu, Yongchun; Bodappa, Nataraju and Wandlowski, Thomas

Subjects:

500 Science > 540 Chemistry

ISSN:

1936-0851

Publisher:

American Chemical Society

Language:

English

Submitter:

Alexander Rudnev

Date Deposited:

16 Jan 2014 10:32

Last Modified:

02 Sep 2015 11:23

Publisher DOI:

10.1021/nn403444j

Uncontrolled Keywords:

single-crystal electrodes, surface-enhanced Raman, SHINERS, Au@SiO2, nanoparticles, cyclic voltammetry, pyridine

BORIS DOI:

10.7892/boris.39820

URI:

https://boris.unibe.ch/id/eprint/39820

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