In situ sum-frequency vibrational spectroscopy of electrochemical interfaces with surface plasmon resonance

Electrochemical (EC) reactions are crucial in many applications, yet most EC analytical tools lack the sensitivity to access molecular-level information of reactants and products. By combining sum-frequency vibrational spectroscopy and surface plasmon resonance at EC interfaces, we demonstrate the f...

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Bibliographic Details
Published in:Proceedings of the National Academy of Sciences - PNAS 2014-01, Vol.111 (4), p.1293-1297
Main Authors: Liu, Wei-Tao, Shen, Y. Ron
Format: Article
Language:English
Subjects:
Aqueous solutions
Chemical reactions
Desorption
Electrocatalysis
Electrochemistry
Electrodes
Gold
Infrared radiation
Light beams
Material films
Oxidation
Physical Sciences
Spectroscopy
Spectrum analysis
Thiols
Vibrational spectra
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Summary:Electrochemical (EC) reactions are crucial in many applications, yet most EC analytical tools lack the sensitivity to access molecular-level information of reactants and products. By combining sum-frequency vibrational spectroscopy and surface plasmon resonance at EC interfaces, we demonstrate the feasibility of measuring in situ and real-time vibrational spectra during EC reactions at noble metal electrodes. Application of the technique to EC reactions at a gold surface helps in understanding how the surface in a basic solution is oxidized and reduced during a cyclic voltammetry cycle. Study of desorption of a thiol self-assembled monolayer from gold through EC reactions in a basic solution shows that the desorbed thiols by reductive reaction remain as an ordered layer near the gold interface, but do diffuse away if they are desorbed oxidatively from gold.
ISSN:0027-8424
1091-6490
DOI:10.1073/pnas.1317290111