The selective activation of C-H bonds is fundamental to fuel conversion chemistry. We have developed a new approach to C-H bond activation using supported transition- and post-transition metals. Through the use of in situ XANES and EXAFS, in conjunction with IR and EPR spectroscopies, it has been possible to determine the nuclearity, coordination environment, and oxidation state of catalyst active sites during the dehydrogenation of propane at 550�C and the hydrogenation of propylene at 200�C. Such investigation has revealed that the active species are single, coordinatively unsaturated metal centers, and that these centers undergo neither oxidation nor reduction while catalyzing C-H bond activation reactions. The improved understanding of the structure and oxidation state of the catalytic active site provided by x-ray spectroscopic analysis, combined with organometallic synthesis techniques, has enabled the subsequent synthesis of single site catalysts capable of hydrogenating propylene at room temperature.

Investigation of supported catalysts for C-H bond activation by X-ray spectroscopic techniques

248th National Meeting (2014)

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