摘要
MWW type titanosilicate, Ti-MWW, has been synthesized by the dry-gel conversion (DGC) method, and its physicochemical properties and catalytic performance in the liquid-phase epoxidation of alkene have been compared with that of hydrothermally synthesized (HTS) Ti-MWW. The roles in the crystallization of silica source, alkali cation, cyclic amine as a structure-directing agent (SDA), and boric acid structure-supporting agent have been investigated. The crystallization of Ti-MWW did not occur for the dry gels free of boric acid, but was feasible at a Si/B molar ratio as high as 12 in marked contrast to the ratio of 0.75 required in the hydrothermal synthesis. The sodium as a mineralization agent was not necessary and on the contrary inhibited the crystallization particularly at a high content. The seeding technique using deboronated MWW effectively accelerated the crystallization speed and reduced the amount of boric acid required. As-synthesized Ti-MWW-DGC lamellar precursors contained both tetrahedral and octahedral species but the latter was selectively removed by acid treatment. Ti-MWW-DGC catalysts showed lower intrinsic activity than Ti-MWW-HTS in the epoxidation of hex-1-ene with hydrogen peroxide probably because the crystal size of the former was 10–20 times as large as that of the latter and then imposed significant diffusion problems for both the substrates and the products.