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Gas-Phase Hydrogen-Atom Measurement above Catalytic and Noncatalytic Materials during Ethane Dehydrogenation

Steinmetz, S.A.; DeLaRiva, Andrew T.; Riley, Christopher R.; Schrader, Paul E.; Datye, Abhaya; Spoerke, Erik D.; Kliewer, Christopher J.

The role of a solid surface for initiating gas-phase reactions is still not well understood. The hydrogen atom (H) is an important intermediate in gas-phase ethane dehydrogenation and is known to interact with surface sites on catalysts. However, direct measurements of H near catalytic surfaces have not yet been reported. Here, we present the first H measurements by laser-induced fluorescence in the gas-phase above catalytic and noncatalytic surfaces. Measurements at temperatures up to 700 °C show H concentrations to be at the highest above inert quartz surfaces compared to stainless steel and a platinum-based catalyst. Additionally, H concentrations above the catalyst decreased rapidly with time on stream. These newly obtained observations are consistent with the recently reported differences in bulk ethane dehydrogenation reactivity of these materials, suggesting H may be a good reporter for dehydrogenation activity.