초록 |
Although chloride-ligated Pt compounds like (bpym)PtCl2, K2PtCl4 and (DMSO)2PtCl2 has been reported to be highly active catalysts for the methane oxidation to methyl bisulfate (MBS) in the oleum media, their applications is hampered by the catalyst deactivation to PtCl2. In this study, we investigated Pt-black catalyzed methane oxidation, which has no ligand. A MBS yield of 82.1% with a selectivity of 96.5% was obtained at a catalyst loading of 1.6 mM at 180 oC, which proved the highest catalytic activity of Pt-black for this reaction. The reaction was thought to proceed by the dissolved Pt species, and no deactivation was observed during four consecutive experiments. However, at a concentration of over 30 mM, MBS yield fell down due to the decomposition of MBS to CO2 on the surface of heterogeneous Pt(0). Vacuum distillation experiments showed the potential for isolating MBS from the oxidation product mixture as a major component. |