CO hydrogenation reaction on sulfided molybdenum catalysts

Adsorption of reaction intermediates appearing during CO hydrogenation at the sulfur covered MoS2(1 0−1 0) surfaces, Mo-termination with 42% S coverage and S-termination with 50% S coverage, are investigated systematically using periodic density functional theory methods. Computed vibrational frequencies of all intermediates are compared with observed data from infrared (IR) spectroscopy allowing a detailed interpretation and assignment of the different features in the experimental spectra. The pathway for CO hydrogenation on both terminations has been studied in detail where the most likely reaction path involves C1 type surface species in the sequence CO → CHO → CH2O → CH2OH → CH2 → CH3 → CH4 in agreement with the experiment.

Graphical abstractCO hydrogenation mechanisms at sulfur covered MoS2(1 0−1 0) surfaces are investigated systematically using periodic density functional theory. Calculated energies of possible reaction steps and barriers are used to identify optimized reaction paths.Figure optionsDownload full-size imageDownload as PowerPoint slide