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Complexation and phase evolution at dimethylformamide-Ag(111) interfaces [electronic resource].

Published:
Washington, D.C. : United States. National Nuclear Security Administration, 2016.
Oak Ridge, Tenn. : Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy
Physical Description:
17 pages : digital, PDF file
Additional Creators:
Sandia National Laboratories, United States. National Nuclear Security Administration, and United States. Department of Energy. Office of Scientific and Technical Information
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Summary:
The interaction of solvent molecules with metallic surfaces impacts many interfacial chemical processes. We investigate the chemical and structure evolution that follows adsorption of the polar solvent dimethylformamide (DMF) on Ag(111). An Ag(DMF)2 coordination complex forms spontaneously by DMF etching of Ag(111), yielding mixed films of the complexes and DMF. Utilizing ultrahigh vacuum scanning tunneling microscopy (UHV-STM), in combination with X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) computations, we map monolayer phases from the 2-D gas regime, consisting of a binary mixture of DMF and Ag(DMF)2, through the saturation monolayer limit, in which these two chemical species phase separate into ordered islands. Structural models for the near-square DMF phase and the chain-like Ag(DMF)2 phase are presented and supported by DFT computation. Interface evolution is summarized in a surface pressure-composition phase diagram, which allows structure prediction over arbitrary experimental conditions. In conclusion, this work reveals new surface coordination chemistry for an important electrolyte-electrode system, and illustrates how surface pressure can be used to tune monolayer phases.
Report Numbers:
E 1.99:sand--2016-5593j
sand--2016-5593j
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Note:
Published through SciTech Connect.
09/15/2016.
"sand--2016-5593j"
"647404"
Journal of Physical Chemistry. C ISSN 1932-7447 AM
Wentao Song; Kevin Leung; Qian Shao; Karen J. Gaskell; Janice E. Reutt-Robey.
Funding Information:
AC04-94AL85000
View MARC record | catkey: 24046217