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Near-Surface Imagin...
Near-Surface Imaging of the Multicomponent Gas Phase above a Silver Catalyst during Partial Oxidation of Methanol
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- Zhou, Bo (author)
- Southern University of Science and Technology,Sandia National Laboratories
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- Huang, Erxiong (author)
- Sandia National Laboratories
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- Almeida, Raybel (author)
- Sandia National Laboratories
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- Gurses, Sadi (author)
- University of California, Davis
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- Ungar, Alexander (author)
- Sandia National Laboratories
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- Zetterberg, Johan (author)
- Lund University,Lunds universitet,Förbränningsfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Combustion Physics,Department of Physics,Departments at LTH,Faculty of Engineering, LTH
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- Kulkarni, Ambarish (author)
- University of California, Davis
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- Kronawitter, Coleman X. (author)
- University of California, Davis
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- Osborn, David L. (author)
- Sandia National Laboratories
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- Hansen, Nils (author)
- Sandia National Laboratories
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- Frank, Jonathan H. (author)
- Sandia National Laboratories
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(creator_code:org_t)
- 2020-12-15
- 2021
- English 14 s.
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In: ACS Catalysis. - : American Chemical Society (ACS). - 2155-5435. ; 11:1, s. 155-168
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http://dx.doi.org/10...
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https://www.osti.gov...
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Abstract
Subject headings
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- Fundamental chemistry in heterogeneous catalysis is increasingly explored using operando techniques in order to address the pressure gap between ultrahigh vacuum studies and practical operating pressures. Because most operando experiments focus on the surface and surface-bound species, there is a knowledge gap of the near-surface gas phase and the fundamental information the properties of this region convey about catalytic mechanisms. We demonstrate in situ visualization and measurement of gas-phase species and temperature distributions in operando catalysis experiments using complementary near-surface optical and mass spectrometry techniques. The partial oxidation of methanol over a silver catalyst demonstrates the value of these diagnostic techniques at 600 Torr (800 mbar) pressure and temperatures from 150 to 410 °C. Planar laser-induced fluorescence provides two-dimensional images of the formaldehyde product distribution that show the development of the boundary layer above the catalyst under different flow conditions. Raman scattering imaging provides measurements of a wide range of major species, such as methanol, oxygen, nitrogen, formaldehyde, and water vapor. Near-surface molecular beam mass spectrometry enables simultaneous detection of all species using a gas sampling probe. Detection of gas-phase free radicals, such as CH3 and CH3O, and of minor products, such as acetaldehyde, dimethyl ether, and methyl formate, provides insights into catalytic mechanisms of the partial oxidation of methanol. The combination of these techniques provides a detailed picture of the coupling between the gas phase and surface in heterogeneous catalysis and enables parametric studies under different operating conditions, which will enhance our ability to constrain microkinetic models of heterogeneous catalysis.
Subject headings
- TEKNIK OCH TEKNOLOGIER -- Kemiteknik -- Kemiska processer (hsv//swe)
- ENGINEERING AND TECHNOLOGY -- Chemical Engineering -- Chemical Process Engineering (hsv//eng)
- NATURVETENSKAP -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)
Keyword
- catalytic partial oxidation of methanol
- molecular beam mass spectrometry
- planar laser-induced fluorescence
- pressure gap
- Raman scattering
Publication and Content Type
- art (subject category)
- ref (subject category)
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- By the author/editor
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Zhou, Bo
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Huang, Erxiong
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Almeida, Raybel
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Gurses, Sadi
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Ungar, Alexander
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Zetterberg, Joha ...
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show more...
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Kulkarni, Ambari ...
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Kronawitter, Col ...
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Osborn, David L.
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Hansen, Nils
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Frank, Jonathan ...
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- About the subject
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- ENGINEERING AND TECHNOLOGY
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ENGINEERING AND ...
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and Chemical Enginee ...
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and Chemical Process ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Physical Science ...
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and Atom and Molecul ...
- Articles in the publication
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ACS Catalysis
- By the university
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Lund University