title: In Situ Monitoring of Electrooxidation Processes at Gold Single Crystal Surfaces Using Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy.
abstract: 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.
authors.forename: Chao-Yu
authors.initials: CY
authors.lastname: Li
authors.forename: Jin-Chao
authors.initials: JC
authors.lastname: Dong
authors.forename: Xi
authors.initials: X
authors.lastname: Jin
authors.forename: Shu
authors.initials: S
authors.lastname: Chen
authors.forename: Rajapandiyan
authors.initials: R
authors.lastname: Panneerselvam
authors.affiliation: §Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, Bern CH-3012, Switzerland.
authors.forename: Alexander V
authors.initials: AV
authors.lastname: Rudnev
authors.forename: Zhi-Lin
authors.initials: ZL
authors.lastname: Yang
authors.affiliation: §Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, Bern CH-3012, Switzerland.
authors.forename: Jian-Feng
authors.initials: JF
authors.lastname: Li
authors.affiliation: §Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, Bern CH-3012, Switzerland.
authors.forename: Thomas
authors.initials: T
authors.lastname: Wandlowski
authors.forename: Zhong-Qun
authors.initials: ZQ
authors.lastname: Tian