Alkane Activation at Catalytic Metal Surfaces: A Coupled Experimental and Theoretical Study of Reaction Dynamics and Energy Transfer at the Gas-Surface Interface

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The Chemical Structure, Dynamics and Mechanisms Program of the Chemistry Division supports Professor Ian Harrison, University of Virginia, for studies of Alkane Activation at Catalytic Metal Surfaces: A Coupled Experimental and Theoretical Study of Reaction Dynamics and Energy Transfer at the Gas-Surface Interface. A heated effusive molecular beam doser will be used to impinge C1-C9 alkane molecules at variable gas temperature onto a surface such that activation barriers for dissociative chemisorption can be surmounted. Dissociative sticking coefficients will be measured and the multidimensional experimental data will be used to test and develop theoretical models of gas-surface reactivity. Using the combination of the effusive molecular beam results to be measured here, existing supersonic molecular beam dissociative sticking measurements, electronic structure theory calculations, and kinetic modeling the effects of molecular rotation, vibrational efficacy, alkane complexity, surface structure, gas and surface temperatures, early/late transition state barrier position, and gas-surface energy transfer on dissociative sticking will be addressed.This research will experimentally characterize and theoretically model the activation of C1-C9 alkanes at catalytic metal surfaces. The research will be directed towards gaining a molecular-level understanding of the activated dissociation of alkanes at surfaces, which is oftentimes believed to be the rate limiting step in the catalytic transformations of alkanes into more valuable chemicals such as hydrogen, synthesis gas, alkenes, or fuels. Alkanes are a targeted product of biomass reforming and more energy efficient and selective catalysis of alkanes is desirable in the quest to efficiently convert renewable biomass to fuels. Importantly, a diverse group of young graduate and undergraduate students will be educated in the interdisciplinary fields of surface science, catalysis, and reaction dynamics through coupled experimental and theoretical work on basic science relevant to a key societal goal, namely, engineering a sustainable energy future. Minority undergraduates will be taught and hosted as part of a summer science encouragement program at the University of Virginia whereby students will learn about renewable energy research. Graduate students will be encouraged and continue in their outreach laboratory demonstrations at local elementary schools.