Abstract
The reactions of methanethiol were studied on Mo(110) using temperature-programmed reaction. X-ray photoelectron, and high resolution electron energy loss spectroscopies. The SH bond in methanethiol is broken upon adsorption to form a methyl thiolate intermediate at 100 K. The CS bond of the intermediate is oriented along the surface normal based on vibrational data which indicates C 3v symmetry since only one methyl rock mode is observed at 905 cm −1. Electron energy loss spectra also indicate that the CS bond is weakened in the methyl thiolate intermediate compared to methanethiol. Methane is formed via CS bond hydrogenolysis of the thiolate in a peak centered at 315 K; nonselective decomposition to atomic carbon and sulfur with gaseous dihydrogen is a competing process. Approximately 40% of the thiolate produces methane and the remaining 60% nonselectively decomposes. The kinetics and selectivity are related to the CS bond strength in the thiolate and the lack of a stable gas-phase dehydrogenation product. The reactivity and structure of the thiolate is compared on Mo(110) and other metals.
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