期刊
ACS NANO
卷 5, 期 7, 页码 5662-5672出版社
AMER CHEMICAL SOC
DOI: 10.1021/nn201307g
关键词
SHINERS; surface-enhanced Raman spectroscopy; core-shell nanoparticles; viologen; single crystal surfaces; electrochemistry
类别
资金
- Swiss National Science Foundation [200021_124643
- 200020_122069, CR5112_126969, NFP 62 406240_126 108]
- FUNMOLS
We reported the first application of in situ shell-isolated nanoparticle enhanced Raman spectroscopy (SHINERS) to an interfacial redox reaction under electrochemical conditions. We construct gap-mode sandwich structures composed of a thiol-terminated HS-6V6H viologen adlayer immobilized on a single crystal Au(111)-(1x1) electrode and covered by Au(60 nm)@SlO(2) core shell nanoparticles acting as plasmonic antennas. We observed high-quality, potential-dependent Raman spectra of the three viologen species V2+,V+center dot and V-0 on a well-defined Au(111) substrate surface and could map their potential-dependent evolution. Comparison with experiments on powder samples revealed an enhancement factor of the nonresonant Raman modes of similar to 3 x 10(5), and up to 9 x 10(7) for the resonance modes. The study illustrates the unique capability of SHINERS and its potential in the entire field of electrochemical surface science to explore structures and reaction pathways on well-defined substrate surfaces, such as single crystals, for molecular, (electro-)- catalytic, bioelectrochemical systems up to fundamental double layer studies at electrified solid/liquid interfaces.
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