期刊
LANGMUIR
卷 27, 期 22, 页码 13910-13917出版社
AMER CHEMICAL SOC
DOI: 10.1021/la202746y
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资金
- Nagasaki University
Phase transitions of an adsorption layer of dibenzyl viologen (dBV) as a typical diaryl viologen on a basal plane of a highly oriented pyrolytic graphite (HOPG) electrode are described using voltammetry, in situ electrochemical scanning tunneling microscopy (EC-STM), and electroreflectance (ER) spectroscopy. A monolayer redox process at less negative potential than the bulk redox process was found to be the first-order faradaic phase transition between a gaslike adsorption layer of dication (dBV(2+)) and a 2D condensed monolayer of radical cation (dBV(center dot+)). Comparison of the results of cyclic voltammetry and potential step chronoamperometry was made with those of heptyl viologen (HV), which also undergoes a faradaic phase transition of the first order. It suggested that the contribution of intermolecular pi-pi interaction between benzyl groups of dBV to the phase transition is minor and apparently equivalent to interchain interaction between the heptyl chains of HV. In situ EC-STM images of the 2D condensed monolayer demonstrated stripe patterns of the rows of dBV(center dot+) molecules forming 3-fold rotationally symmetric domains. The results of the ER measurements also revealed that the orientation of the longitudinal molecular axis of the bipyridinium moiety of dBV(center dot+) molecules lying flat on the HOPG electrode surface, most likely with a side-on configuration.
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