화학공학소재연구정보센터
Applied Catalysis A: General, Vol.194-195, 375-381, 2000
Shape-selective N-methylation of melamine with methanol by use of Ru/mordenite catalyst in the liquid phase
A Ru/mordenite (Ru/M) catalyst with catalytically-active ruthenium species retained in the mordenite pores has been prepared by the ion-exchange of Na-mordenite with [Ru(NH3)(6)](3+), followed by a very mild thermal treatment. While ex tended X-ray absorption fine structure (EXAFS) analysis showed the presence of both Ru-N and Ru-Ru bonds, HRTEM photographs evidenced the absence of metal particles larger than the diameter of a mordenite pore. The remaining NH3 ligand was also observed from the characteristic IR bands appearing at 1640:and 1356 cm(-1); the IR spectrum of adsorbed CO indicated the presence of multicarbonyl-type surface species (such as Run+(CO)(3)), consistent with the well-dispersed or coordinatively-unsaturated nature of ruthenium species. After the complete preparation procedure, a high degree of crystallinity-was maintained for mordenite (XRD), and the decrease of S-BET from 32 to 313 m(2) g(-1) ensured the existence of ruthenium species in the mordenite pores. It was demonstrated that, by using this catalyst, N-methylation of melamine with methanol was able to proceed in a moderately shape-selective manner (suppression of the formation of N,N,N''-tri methylated melamine (3) as compared to thar of N-methylated or N,N'-di-methylated melamine (1 or 2)) which is in harmony with the sizes of relevant molecules relative to the size of a mordenite pore.