In Situ Monitoring of Electrooxidation Processes at Gold Single Crystal Surfaces Using Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy

Identifying the intermediate species in an electrocatalytic reaction can provide a great opportunity to understand the reaction mechanism and fabricate a better catalyst. However, the direct observation of intermediate species at a single crystal surface is a daunting challenge for spectroscopic tec...

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Veröffentlicht in:Journal of the American Chemical Society 2015-06, Vol.137 (24), p.7648-7651
Hauptverfasser: Li, Chao-Yu, Dong, Jin-Chao, Jin, Xi, Chen, Shu, Panneerselvam, Rajapandiyan, Rudnev, Alexander V, Yang, Zhi-Lin, Li, Jian-Feng, Wandlowski, Thomas, Tian, Zhong-Qun
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Sprache:eng
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Zusammenfassung:Identifying the intermediate species in an electrocatalytic reaction can provide a great opportunity to understand the reaction mechanism and fabricate a better catalyst. However, the direct observation of intermediate species at a single crystal surface is a daunting challenge for spectroscopic techniques. In this work, electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy (EC-SHINERS) is utilized to in situ monitor the electrooxidation processes at atomically flat Au­(hkl) single crystal electrode surfaces. We systematically explored the effects of crystallographic orientation, pH value, and anion on electrochemical behavior of intermediate (AuOH/AuO) species. The experimental results are well correlated with our periodic density functional theory calculations and corroborate the long-standing speculation based on theoretical calculations in previous electrochemical studies. The presented in situ electrochemical SHINERS technique offers a unique way for a real-time investigation of an electrocatalytic reaction pathway at various well-defined noble metal surfaces.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.5b04670