Actieve zuurstof in metaalhoudende zeolieten voor de selectieve oxidatie van koolwaterstoffen.

The global industrial activity is facing a drastic change in raw material base. Efficient and sustainable utilization of residual resources becomes vital, while technological development and optimization to reduce greenhouse gas emissions are equally significant. Efficient use of remaining natural gas reservoirs, which are estimated to hold for another 60 years, is a major challenge. As storage and transportation of natural gas is complicated and often non-economical, new technology to convert natural gas onsite into liquid, such as methanol, would be highly desirable. It requires very selective catalysis with high activity at sufficiently low temperatures to avoid deep oxidation to CO and CO2. In the past, numerous groups have attempted this reaction with bio- and chemocatalysis, but the search for robust heterogeneous catalysts in partial methane oxidation has been elusive. Recently, COK identified in collaboration with the research group of professor E. Solomon, the formation of a unique very active [Cu(II)-O-Cu(II)]2+ core (PNAS, 2009). This core is easily formed upon contactin a Cu exchanged ZSM-5 zeolite with oxidants like O2 or the greenhouse gas N2O. The dicopper core is able to transform methane in methanol at temperatures below 150°C. The active core being identified very recently, the project will further search for the fundamental understanding of the role of various key parameters, i.e., size, composition. Al distribution, zeolite structure and transition metal type in the formation and (re)activity of the active cupper core. The project should provide detailed information concerning the mechanistic cycle of the oxidation process, and should ultimately accelerate the design process of novel high performance catalysts for selective methane oxidation.

Trefwoorden:Heterogeneous catalysis, Zeolite, Spectroscopy, Biomimicry, Selective oxidation, Methane oxidation