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Hydrogen partitioning as a function of time-on-stream for an unpromoted iron-based Fischer-Tropsch synthesis catalyst applied to CO hydrogenation

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Davidson_2019_IECR_Hydrogen_CC.pdf (1.743Mb)
Date
08/01/2020
Author
Davidson, Alisha L.
Webb, Paul B.
Parker, Stewart F.
Lennon, David
Keywords
QD Chemistry
Chemistry(all)
Chemical Engineering(all)
Industrial and Manufacturing Engineering
NDAS
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Abstract
Inelastic neutron scattering (INS) is employed to examine the evolution of a promoter-free iron-based Fischer-Tropsch synthesis catalyst (∼10 g catalyst charge) that is exposed to ambient pressure CO hydrogenation at 623 K for up to 10 days time-on-stream (T-o-S). The longer reaction time is selected to better understand how the formation of a previously described hydrocarbonaceous overlayer corresponds to the catalyst conditioning process. Although the onset of pseudo steady-state reactor performance is observed at approximately 9 h T-o-S, INS establishes that the intensity of the C-H stretching mode of the sp3-hybridized component of the hydrocarbonaceous overlayer saturates at about 24 h T-o-S, while the corresponding intensity of the C-H stretching mode of the sp2-hybridized component requires 100-200 h T-o-S to achieve saturation. This novel series of measurements reveal different aspects of the complex catalyst evolutionary process to be indirectly connected with catalytic turnover.
Citation
Davidson , A L , Webb , P B , Parker , S F & Lennon , D 2020 , ' Hydrogen partitioning as a function of time-on-stream for an unpromoted iron-based Fischer-Tropsch synthesis catalyst applied to CO hydrogenation ' , Industrial and Engineering Chemistry Research , vol. 59 , no. 1 , pp. 52-60 . https://doi.org/10.1021/acs.iecr.9b04636
Publication
Industrial and Engineering Chemistry Research
Status
Peer reviewed
DOI
https://doi.org/10.1021/acs.iecr.9b04636
ISSN
0888-5885
Type
Journal article
Rights
Copyright © 2019 American Chemical Society. This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
Description
Sasol Ltd., the EPSRC (award reference EP/P505534/1), and the University of Glasgow are thanked for the provision of a postgraduate studentship (ALD). The STFC Rutherford Appleton Laboratory is thanked for access to neutron beam facilities. The Royal Society is thanked for the provision of an Industry Fellowship (PBW).
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  • University of St Andrews Research
URI
http://hdl.handle.net/10023/19256

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