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

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

doi:10.1021/acs.jpcc.1c09955

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

Journal Article · Wed Feb 02 00:00:00 EST 2022 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.1c09955· OSTI ID:1855813

^[1]; DeLaRiva, Andrew T. ^[2]; ^[3]; Schrader, Paul ^[1]; ^[2]; ^[3]; Kliewer, Christopher J. ^[1]

Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Univ. of New Mexico, Albuquerque, NM (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

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. Furthermore, 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.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: NA0003525

OSTI ID:: 1855813

Report Number(s):: SAND2022-2755J; 704025

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 6 Vol. 126; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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