具有高催化活性和水热稳定性的新型介孔分子筛催化材料-吉大.ppt

SBA-15 MAS-9 Wave number (cm-1) IR Spectroscopy 556 cm-1: 5-ring of T-O-T: Containing zeolite units Strong Acidity and Good Catalysis Summary of MAS-7 MAS-9 Novel Micro/mesoporous Materials High Hydrothermal Stability Strong Acidity Good Catalytic Properties Ordered Titanosilicates with Highly Catalytic Active Sites for Oxidation Reactions (MTS-9) --- J. Am. Chem. Soc., 124, 888, 2001. Applications in Oxidation Reactions Very Stable Highly Active Catalyst --- 1983, US Patent. Nature, 1988 1989 Shortage: Small pore Size: Limited for bulky! To Synthesize Mesoporous Titanosilicate? TS-1 Zeolite Ti-MCM-41: Novel Catalysts --- Chem. Commun. 1994 Olefins epoxidation: Small: TS-1 Ti-MCM-41 Bulky: Ti-MCM-41 TS-1 Phenol hydroxylation: Low conversion! --- low oxidation ability! Ordered Mesoporous Titanosilicates Shortages of Ordered Mesoporous Titanosilicates ? Low Hydrothermal stability! ? Low Oxidation Ability! --- Limitation for Wide Application ? Why? ---Amorphous Walls ? Preparation of nanosized TS-1 zeolite containing PSBU ? Assembly of nanosized zeolites with surfactant micella: ordered mesoporous titanosilicates. How to Synthesize Mesoporous Titanosilicates with High Active Sites? Two-Step Procedure! X-ray Diffraction A: MTS-9; B: Ti-MCM-41; C: Ti-SBA-15 --- MTS-9: More stable Boiling water for 120h Without treatment Ti-SBA-15 MTS-9 IV-Type isotherm The same mesopore size N2 Isotherms TEM of MTS-9 Phenol Hydroxylation MTS-9: Very Active, Similar to TS-1 Ti-MCM-41 Ti-HMS : Inactive UV-Vis MTS-9：215 nm, the same as TS-1. MTS-9 Ti-MCM-41 IR Spectroscopy Ti-MCM-41 MTS-9 550 cm-1 550 cm-1: 5-ring of T-O-T: Containing zeolite units (PSBU), which is similar to that of TS-1 UV-Raman Spectroscopy Ti-MCM-41 MTS-9 MTS-9: 1122 cm-1: characteristic of 4-coordinated Ti, similar to TS-1 (1125 cm-1) UV-Raman Spectra of TS-1 and Silicalite-I Characteristic of 4-coordinated Ti species --- Angew. Chem. Int. Ed., 1999, 38, 2220. Sum