Integrative Graduate
Education and
Research Traineeship

Highlight

Research on C-H Bond Activation by Pd-substituted ceria

Sychrotron diffraction from catalysts.

Projects:

IGERT: ConvEne--Conversion of Energy Through Molecular...

Institution:

University of California at Santa Barbara

Primary Strategic Goal:

Discovery: Foster research that will advance the frontiers of knowledge, emphasizing areas of greatest opportunity and potential benefit and establishing the Nation as a global leader in fundamental transformational science and engineering.

Secondary Strategic Goal:

Learning: Build the Nation's research capability through critical investments in advanced instrumentation, facilities, cyber infrastructure, and experimental tools.

Achievement/Results

The study of methane activation reactions has important energy applications. While large reserves of methane exist, and a considerable portion of these reserves are currently used to heat homes and generate hydrogen for other synthetic processes, it is widely accepted that the conversion of methane to liquid hydrocarbon fuels, efficiently with an inexpensive and robust catalyst, would be a substantial contribution to alternative energy research. The usual Fischer-Tropsch strategy requires oxidation to mixtures of carbon monoxide and hydrogen, which are then converted to higher hydrocarbons. Alternate partial oxidation strategies could be a more direct route to valuable products. For example, dry reforming of methane is of value because recovered methane is often found in the presence of carbon dioxide. As large-scale separations are expensive, it would be convenient to identify a catalyst that efficiently converts methane to useful products in the presence of carbon dioxide.IGERT Fellow Lauren Misch has investigated Pd-substituted ceria for C-H bond activation reactions including the partial oxidation and dry reforming of methane. The studies, including post-catalytic synchrotron diffraction, suggest that the single-phase Pd-substituted ceria material is not the active species and that catalysis occurs instead over the reduced two-phase palladium-on-ceria system. This observation has been further confirmed by verifying the activity of the reduced catalysts for ethylene hydrogenation, a reaction that is known to require elemental palladium.

Address Goals

The reactions tested are of crucial importance for energy independence from liquid petroleum resources, and instead focus on more available natural gas resources. The work, a collaboration between the IGERT fellow, two IGERT associates, and three IGERT faculty members, is also highly interdisciplinary, bringing skills of chemical engineering, chemistry, and materials science to this important problem.