Probing the Nature of the Active Phase of Molybdenum-Supported Catalysts for the Direct Synthesis of Methylmercaptan from Syngas and H2S

作者：Cordovan A; Blanchard P; Lancelot C; Fremy G; Lamonier C^*

来源：ACS Catalysis, 2015, 5(5): 2966-2981.

DOI：10.1021/cs502031f

• methyl mercaptan
• thiolation
• syngas
• molybdenum disulfide
• KMo-based catalysts
• sulfided catalysts
• potassium tetrathiomolybdate
• potassium tetraoxomolybdate

Alumina supported K-, Mo-, and K-Mo-based catalysts prepared from different precursors (ammonium heptamolybdate + KNO3, K2MoO4, K2MoS4) with the same loading were used to produce CH3SH by the simple syngas/H2S route. The simultaneous presence of Mo and K in the catalytic system allows the achievement of higher CO conversions and CH3SH selectivity and a decrease in CO2 selectivity. Through XPS analysis of sulfided catalysts, the presence of a new phase (named KxMoS2) with an unusual Mo 3d binding energy in which potassium cations are intercalated between the MoS2 layers is evidenced. The amount of this phase was well correlated with the catalytic performances of the corresponding catalysts in the reaction of methyl mercaptan production. Indeed, it was found that the higher the amount of KxMoS2 phase in the catalyst, the higher the CH3SH productivity. On the basis of these statements KxMoS2 is proposed as the active phase acting in the reaction of thiolation of syngas.

• 出版日期2015-5