Design and evaluation of magnetic resonance experiments for catalysis

Abstract

The focus of this research was to develop and evaluate new experimental methods for NMR studies of catalysis with a mandate for the use of magic angle sample spinning for all techniques. As a part of this effort several advancements were made including the reduction of in situ MAS NMR variable temperature experimental time scales from tens of minutes (and sometimes hours) to tens of seconds via radio frequency inductive heating, development of an MAS imaging experiment that allows the rapid determination of the homogeneity of adsorbates on catalyst beds, and the application of fluorine containing probe molecules, as observed by proton-fluorine double resonance NMR, to study zeolite acid strength. Other advancements that grew out the catalysis effort were the use of laser heating to perform temperature jump experiments allowing solid-liquid correlated spectroscopy to be performed, the use of laser heating to study thermal degradation of materials, and the design of an experiment for freeze-trapping reactive species in solution that may have application in the study of enzymatic catalysis. Additionally an NMR instrument was constructed in order to provide an experimental platform that was versatile and isolated from the main laboratory for safety reasons.