Formation, characterization, and stability of methaneselenolate monolayers on Au(111) : an electrochemical high-resolution photoemission spectroscopy and DFT study
We investigated the mechanism of formation and stability of self-assembled monolayers (SAMs) of methaneselenolate on Au(111) prepared by the immersion method in ethanolic solutions of dimethyl diselenide (DMDSe). The adsorbed species were characterized by electrochemical measurements and high-resolu...
Veröffentlicht in: | Langmuir : the ACS journal of surfaces and colloids. - 1992. - 30(2014), 13 vom: 08. Apr., Seite 3754-63 |
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1. Verfasser: | |
Weitere Verfasser: | , , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2014
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Zugriff auf das übergeordnete Werk: | Langmuir : the ACS journal of surfaces and colloids |
Schlagworte: | Journal Article Research Support, Non-U.S. Gov't Organoselenium Compounds Solutions Sulfhydryl Compounds methylmercaptan 2X8406WW9I Ethanol 3K9958V90M Gold |
Zusammenfassung: | We investigated the mechanism of formation and stability of self-assembled monolayers (SAMs) of methaneselenolate on Au(111) prepared by the immersion method in ethanolic solutions of dimethyl diselenide (DMDSe). The adsorbed species were characterized by electrochemical measurements and high-resolution photoelectron spectroscopy (HR-XPS). The importance of the headgroup on formation mechanism and the stability of the SAMs was addressed by comparatively studying methaneselenolate (MSe) and methanethiolate (MT) monolayers. Density Functional Theory (DFT) calculations were performed to identify the elementary reaction steps in the mechanisms of formation and decomposition of the monolayers. Reductive desorption and HR-XPS measurements indicated that a MSe monolayer is formed at short immersion times by the cleavage of the Se-Se bond of DMDSe. However, the monolayer decomposes at long immersion times at room temperature, as evidenced by the appearance of atomic Se on the surface. The decomposition is more pronounced for MSe than for MT monolayers. The MSe monolayer stability can be greatly improved by two modifications in the preparation method: immersion at low temperatures (-20 °C) and the addition of a reducing agent to the forming solution |
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Beschreibung: | Date Completed 13.04.2015 Date Revised 08.04.2014 published: Print-Electronic Citation Status MEDLINE |
ISSN: | 1520-5827 |
DOI: | 10.1021/la404996q |