Well-defined, supported epoxidation catalysts from molecular precursors

Justin M. Notestein*, Natalia Morlanes-Sanchez, Nicholas Schoenfeldt, Andrew Korinda, Randall Meyer, Zhenjuan Ni

*Corresponding author for this work

Research output: Contribution to journalConference articlepeer-review

Abstract

Supported oxides are ubiquitous heterogeneous catalysts, and synthetic control over oxide domains offers to improve our understanding of mechanisms at the atomic level and ultimately to control catalyst activities and selectivities. Two routes are presented to well-defined, supported oxides utilizing precursor inorganic complexes with some of the desired atomic connectivity built in. In the first, calixarene-Ta complexes are synthesized and grafted to SiO 2 for a one-pot route to ligand-capped, isolated sites. These catalysts have higher direct epoxidation selectivity for cyclohexene and less H 2O 2 decomposition than their bare oxide analogues. Epoxide hydrolysis can be lessened by simple capping with octanol. In the second, triazacyclononane manganese oxide catalysts are supported on functionalized surfaces for alkene epoxidation / dihydroxylation. These reactions occur at <25°C and epoxidation vs. dihydroxylation selectivity is controlled by the supported co-catalyst. Spectroscopic (principally XAS and UV-vis) and mechanistic studies give additional insight.

Original languageEnglish (US)
JournalACS National Meeting Book of Abstracts
StatePublished - 2011
Event242nd ACS National Meeting and Exposition - Denver, CO, United States
Duration: Aug 28 2011Sep 1 2011

ASJC Scopus subject areas

  • General Chemistry
  • General Chemical Engineering

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