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CAMP Seminar: My Big Fat Greek Sabbatical: An Odyssey from Macroscopic Measurements to Atomic Design

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Angela D. Lueking, Pennsylvania State University
09 September 2014 from 3:30 PM to 4:30 PM
339 Davey Laboratory
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Hydrogen spillover involves addition of a catalyst to a high-surface area microporous support, such that the catalyst acts as a source for atomic hydrogen, the atomic hydrogen diffuses from the catalyst to the support, and ideally, the support provides a high number of tailored surface binding sites to maximize the number of atomic hydrogens interacting with the surface.  Hydrogen spillover has been proposed as a means to increase the operative adsorption temperature of nanoporous materials from cryogenic conditions to near ambient temperature.  However, this proposition has become highly controversial in the past few years, due largely to discrepancies between laboratories, and even variations of the magnitude of hydrogen uptake observed for materials prepared with near-identical techniques within the same laboratory.  These discrepancies have pointed to the fact that the hydrogen spillover mechanism is not understood on a molecular level.  Theoretical calculations exacerbated the controversy when they suggested an extremely narrow window for a thermodynamic incentive for hydrogen spillover, and a kinetic barrier that was virtually insurmountable. At Penn State, we published the first direct spectroscopic evidence of a reversible room temperature carbon-hydrogen wag mode that demonstrated some inconsistencies  with theoretical (DFT) calculations.  Amidst this controversy, I travelled to the University of Crete as a Marie Curie Fellow to reconcile these differences.  A combined experimental and theoretical approach was used to resolve the apparent discrepancies in the hydrogen spillover mechanism and propose potential surface sites and structures responsible for the high uptake in select materials. Applicable beyond the field of hydrogen storage, the results have implications to this elementary step in many catalytic reactions and in the design of new catalytic materials.