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Catalytic synthesis of methanethiol from hydrogen sulfide and carbon monoxide over vanadium-based catalysts |
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| Authors: | Guido Mul Israel E Wachs Albert S Hirschon |
| Affiliation: | a SRI-International, Department of Chemistry and Chemical Engineering, 333 Ravenswood Ave, Menlo Park, CA 94025, USA b Lehigh University, Department of Chemical Engineering, Zettlemoyer Center for Surface Studies, 7 Asa Drive, Bethlehem, PA 18015, USA c Delft University of Technology, Delft-ChemTech, R&CE, Julianalaan 136, 2628 BL, Delft, The Netherlands |
| Abstract: | The direct synthesis of methanethiol, CH3SH, from CO and H2S was investigated using sulfided vanadium catalysts based on TiO2 and Al2O3. These catalysts yield high activity and selectivity to methanethiol at an optimized temperature of 615 K. Carbonyl sulfide and hydrogen are predominant products below 615 K, whereas above this temperature methane becomes the preferred product. Methanethiol is formed by hydrogenation of COS, via surface thioformic acid and methylthiolate intermediates. Water produced in this reaction step is rapidly converted into CO2 and H2S by COS hydrolysis. Titania was found to be a good catalyst for methanethiol formation. The effect of vanadium addition was to increase CO and H2S conversion at the expense of methanethiol selectivity. High activities and selectivities to methanethiol were obtained using a sulfided vanadium catalyst supported on Al2O3. The TiO2, V2O5/TiO2 and V2O5/Al2O3 catalysts have been characterized by temperature programmed sulfidation (TPS). TPS profiles suggest a role of V2O5 in the sulfur exchange reactions taking place in the reaction network of H2S and CO. |
| Keywords: | Methanethiol Carbon monoxide Hydrogen sulfide COS Hydrolysis TPS Catalysts Supported Vanadium oxide Vanadium sulfide Titania Alumina |
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