Aerobic Epoxidation of Olefin by Platinum Catalysts Supported on Mesoporous Silica Nanoparticles

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• 作者：Dominik Munz ; Daoyong Wang ; Megan M. Moyer ; Michael S. Webster-Gardiner ; Pranaw Kunal ; David Watts ; Brian G. Trewyn ; Andrei N. Vedernikov ; T. Brent Gunnoe
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：July 1, 2016
• 年：2016
• 卷：6
• 期：7
• 页码：4584-4593
• 全文大小：627K
• 年卷期：0
• ISSN：2155-5435

文摘

We report platinum catalysts for the efficient aerobic oxidation of olefins to form epoxides and/or derived glycol monoethers. The catalysts—diaqua and dichloro Pt^II complexes supported by the ligand di(2-pyridine)methanesulfonate (dpms)—are most active when they are covalently tethered to mesoporous silica nanoparticles (MSNs). Supporting the molecular Pt complexes on the MSNs prevents bimolecular catalyst deactivation. Using this strategy, >40 000 turnovers are achieved for the aerobic oxidation of norbornene in 2,2,2-trifluoroethanol. The position of the tether and the nature of other ligands in the metal coordination sphere (aqua, hydroxo, or chloro) are shown to affect the catalyst activity. The new MSN-supported Pt materials were characterized by nuclear magnetic resonance (NMR) spectroscopy, nitrogen physisorption, powder X-ray diffraction (PXRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and thermogravimetric analysis (TGA).