The Research Of N-ligands/CuCl Used As Catalysts For The Reaction Of Oxidative Carbonylation

This thesis deals with the preparation, characterization and catalytic reactivity in the liquid phase oxidative carbonylation of polystyrene-supported catalyst (PS-Phen/CuCl), organic-inorganic hybrid-supported catalyst (OIH/CuCl) and the catalysts of the coordination with pyridine compounds and CuCl.The PS-Phen/CuCl materials were good catalysts for liquid phase oxidative carbonylation of methanol to form Dimethyl Carbonate (DMC). The catalyst (PS-Phen/CuCl) exhibited higher activity and selectivity than the unsupported CuCl and PS-Phen/CuCl2 catalysts. PS-Phen/CuCl could be separated easily and be reused several times, with slight loss of the active components. After recycling 6 times, the catalyst still showed high catalytic activity and selectivity, with the average conversion of methanol of 15.3% and the average of 96.4%, under the reaction conditions of [Cu(I)]=0.2mol/L, 3.0MPa(PCO:PO2=9:1), 2h, 120℃.For the reaction of oxidative carbonylation of methanol to dimethyl carbonate using the catalysts of the coordination with pyridine compounds and CuCl, The experiments showed that when pyridine compounds were used as ligands, the catalytic activities were increased remarkably,the catalytic capabilities of these pyridine compounds should be due to their pKa and their structural properties;Also it was found that the catalytic activities of bipyridine compounds were better than normal single-N pyridine compounds;For single-N pyridine compounds, it showed the best catalytic activity during the reaction while its pKa was approximate 6.7, whether higher or lower than it, their catalytic activities would gradual decrease.