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- W2965720266 abstract "Recently, attention on pyridine adsorption and reaction at the electrode/electrolyte interface has been revitalized in the context of pyridine-mediated reactions such as CO2 reduction. Taking Pt as an example, although numerous efforts have been made, disagreements are still unresolved regarding the potential-dependent adsorption of pyridine on the Pt electrode, which further prevents an explicit understanding of the pyridine-mediated electrochemical process at a molecular level. Here, we employed an operando electrochemical surface-enhanced Raman spectroscopy method, in combination with the density functional theory calculation and isotopic labeling of the molecule, to thoroughly study how pyridine interacts with the Pt electrode/electrolyte interface. For the first time, it is corroborated that pyridine is adsorbed on the Pt electrode in both pyridine molecule (Py) and α-pyridyl radical (α-Pyl) states. On the basis of a systematic investigation of the potential-dependent vibrational spectra, we further explored how the coverage, configuration, and binding strength of both Py and α-Pyl adsorbates on the Pt electrode are tuned by electrode polarization and accordingly established a structural model at the electrochemical interface. Our work not only ends the long-time disputes on how pyridine interacts with the Pt electrode but also provides crucial information for the mechanistic research of pyridine-mediated reaction process." @default.
- W2965720266 created "2019-08-13" @default.
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- W2965720266 date "2019-08-04" @default.
- W2965720266 modified "2023-10-14" @default.
- W2965720266 title "Potential-Dependent Coadsorption of Pyridine Molecule and α-Pyridyl Radical at the Pt Electrode/Electrolyte Interface" @default.
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- W2965720266 doi "https://doi.org/10.1021/acs.jpcc.9b03752" @default.
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