Dimeric 1,4,7-triazacyclononane manganese oxides are known to be efficient and highly active homogeneous oxidation catalysts whose selectivity toward epoxidation and cis-dihydroxylation can be controlled by the addition of various acid co-catalysts.  Here we present synthetic routes to supported triazacyclononane manganese oxides by a number of methods including impregnation, direct grafting and surface self-assembly.  Impregnation and self-assembly are found to be the most facile techniques.  Self-assembly from MeCN/H2O2 solutions onto organo-functionalized oxide supports provides the inherent advantage of supplying a co-catalyst as the tethering method, while direct grafting allows the control of tether length and rigidity.  The catalysts are characterized by diffuse reflectance UV-visible and X-ray spectroscopies with an emphasis on comparing and contrasting the metal oxide surface structures obtained by the various heterogenization methods.  Finally, the activity and selectivity of the catalysts prepared by the various heterogenization methods are compared for cyclooctene oxidation with aqueous H2O2.

Heterogenization and characterization of 1,4,7-triazacyclononane based manganese oxides for low temperature oxidation

239th National Meeting (2010)

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