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The application of inelastic neutron scattering to investigate iron-based Fischer-Tropsch to olefins catalysis

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The application of inelastic neutron scattering to investigate iron-based Fischer-Tropsch to olefins catalysis. / Davidson, Alisha L.; Gibson, Emma K.; Cibin, Giannantonio; van Rensburg, Hendrik; Parker, Stewart F.; Webb, Paul B.; Lennon, David.

In: Journal of Catalysis, Vol. 392, 12.2020, p. 197-208.

Research output: Contribution to journalArticlepeer-review

Harvard

Davidson, AL, Gibson, EK, Cibin, G, van Rensburg, H, Parker, SF, Webb, PB & Lennon, D 2020, 'The application of inelastic neutron scattering to investigate iron-based Fischer-Tropsch to olefins catalysis', Journal of Catalysis, vol. 392, pp. 197-208. https://doi.org/10.1016/j.jcat.2020.09.025

APA

Davidson, A. L., Gibson, E. K., Cibin, G., van Rensburg, H., Parker, S. F., Webb, P. B., & Lennon, D. (2020). The application of inelastic neutron scattering to investigate iron-based Fischer-Tropsch to olefins catalysis. Journal of Catalysis, 392, 197-208. https://doi.org/10.1016/j.jcat.2020.09.025

Vancouver

Davidson AL, Gibson EK, Cibin G, van Rensburg H, Parker SF, Webb PB et al. The application of inelastic neutron scattering to investigate iron-based Fischer-Tropsch to olefins catalysis. Journal of Catalysis. 2020 Dec;392:197-208. https://doi.org/10.1016/j.jcat.2020.09.025

Author

Davidson, Alisha L. ; Gibson, Emma K. ; Cibin, Giannantonio ; van Rensburg, Hendrik ; Parker, Stewart F. ; Webb, Paul B. ; Lennon, David. / The application of inelastic neutron scattering to investigate iron-based Fischer-Tropsch to olefins catalysis. In: Journal of Catalysis. 2020 ; Vol. 392. pp. 197-208.

Bibtex - Download

@article{1f02737b1b3e4ac59ab7087d19f69924,
title = "The application of inelastic neutron scattering to investigate iron-based Fischer-Tropsch to olefins catalysis",
abstract = "The technique of inelastic neutron scattering (INS) is used to investigate how hydrogen is partitioned within a series of Na and S promoted iron-based Fischer-Tropsch-to-olefin catalysts. Two reaction test regimes are examined. First, reaction testing at elevated temperature and pressure demonstrate how Na/S additions enhance short chain olefin selectivity and reduce methane formation under industrially relevant reaction conditions. For a fixed level of Na incorporation (2000 ppm), sulfur concentrations of ≤ 100 ppm result in only a modest improvement in olefin selectivity. However, for sulfur values of ≥ 100 ppm there is a noticeable and systematic increase in C2-C4 olefin selectivity; rising from ∼30.0 % to 35.2% at 250 ppm. Second, using ambient pressure CO hydrogenation as a test reaction in INS and micro-reactor configurations, catalyst samples are further analysed by TPR, TPO, XRD and S K-edge XANES. INS shows the formation of a hydrocarbonaceous overlayer to be significantly attenuated by the presence of the promoters, with increasing S levels significantly reducing the intensity of the sp2 and sp3 hybridised ν(C-H) modes of the overlayer, albeit to differing degrees. A probable role for how this combination of promoters is perturbing the form of the hydrocarbonaceous overlayer to subsequently moderate the product distribution is considered.",
keywords = "Fischer-Tropsch-to-olefins catalysis, Inelastic neutron scattering, XANES, Chemical modifiers",
author = "Davidson, {Alisha L.} and Gibson, {Emma K.} and Giannantonio Cibin and {van Rensburg}, Hendrik and Parker, {Stewart F.} and Webb, {Paul B.} and David Lennon",
note = "Sasol Ltd., the University of Glasgow and EPSRC [award reference EP/P505534/1.] are thanked for the provision of postgraduate studentship (ALD). The STFC Rutherford Appleton Laboratory is thanked for access to neutron beam facilities [RB 1520269/1610413]. Diamond Light Source is thanked for time on B18 beamline through the Catalysis Hub BAG application (SP15151 and rapid access beamtime SP18431). The Royal Society is thanked for the provision of an Industry Fellowship (PBW).",
year = "2020",
month = dec,
doi = "10.1016/j.jcat.2020.09.025",
language = "English",
volume = "392",
pages = "197--208",
journal = "Journal of Catalysis",
issn = "0021-9517",
publisher = "Academic Press Inc.",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - The application of inelastic neutron scattering to investigate iron-based Fischer-Tropsch to olefins catalysis

AU - Davidson, Alisha L.

AU - Gibson, Emma K.

AU - Cibin, Giannantonio

AU - van Rensburg, Hendrik

AU - Parker, Stewart F.

AU - Webb, Paul B.

AU - Lennon, David

N1 - Sasol Ltd., the University of Glasgow and EPSRC [award reference EP/P505534/1.] are thanked for the provision of postgraduate studentship (ALD). The STFC Rutherford Appleton Laboratory is thanked for access to neutron beam facilities [RB 1520269/1610413]. Diamond Light Source is thanked for time on B18 beamline through the Catalysis Hub BAG application (SP15151 and rapid access beamtime SP18431). The Royal Society is thanked for the provision of an Industry Fellowship (PBW).

PY - 2020/12

Y1 - 2020/12

N2 - The technique of inelastic neutron scattering (INS) is used to investigate how hydrogen is partitioned within a series of Na and S promoted iron-based Fischer-Tropsch-to-olefin catalysts. Two reaction test regimes are examined. First, reaction testing at elevated temperature and pressure demonstrate how Na/S additions enhance short chain olefin selectivity and reduce methane formation under industrially relevant reaction conditions. For a fixed level of Na incorporation (2000 ppm), sulfur concentrations of ≤ 100 ppm result in only a modest improvement in olefin selectivity. However, for sulfur values of ≥ 100 ppm there is a noticeable and systematic increase in C2-C4 olefin selectivity; rising from ∼30.0 % to 35.2% at 250 ppm. Second, using ambient pressure CO hydrogenation as a test reaction in INS and micro-reactor configurations, catalyst samples are further analysed by TPR, TPO, XRD and S K-edge XANES. INS shows the formation of a hydrocarbonaceous overlayer to be significantly attenuated by the presence of the promoters, with increasing S levels significantly reducing the intensity of the sp2 and sp3 hybridised ν(C-H) modes of the overlayer, albeit to differing degrees. A probable role for how this combination of promoters is perturbing the form of the hydrocarbonaceous overlayer to subsequently moderate the product distribution is considered.

AB - The technique of inelastic neutron scattering (INS) is used to investigate how hydrogen is partitioned within a series of Na and S promoted iron-based Fischer-Tropsch-to-olefin catalysts. Two reaction test regimes are examined. First, reaction testing at elevated temperature and pressure demonstrate how Na/S additions enhance short chain olefin selectivity and reduce methane formation under industrially relevant reaction conditions. For a fixed level of Na incorporation (2000 ppm), sulfur concentrations of ≤ 100 ppm result in only a modest improvement in olefin selectivity. However, for sulfur values of ≥ 100 ppm there is a noticeable and systematic increase in C2-C4 olefin selectivity; rising from ∼30.0 % to 35.2% at 250 ppm. Second, using ambient pressure CO hydrogenation as a test reaction in INS and micro-reactor configurations, catalyst samples are further analysed by TPR, TPO, XRD and S K-edge XANES. INS shows the formation of a hydrocarbonaceous overlayer to be significantly attenuated by the presence of the promoters, with increasing S levels significantly reducing the intensity of the sp2 and sp3 hybridised ν(C-H) modes of the overlayer, albeit to differing degrees. A probable role for how this combination of promoters is perturbing the form of the hydrocarbonaceous overlayer to subsequently moderate the product distribution is considered.

KW - Fischer-Tropsch-to-olefins catalysis

KW - Inelastic neutron scattering

KW - XANES

KW - Chemical modifiers

U2 - 10.1016/j.jcat.2020.09.025

DO - 10.1016/j.jcat.2020.09.025

M3 - Article

VL - 392

SP - 197

EP - 208

JO - Journal of Catalysis

JF - Journal of Catalysis

SN - 0021-9517

ER -

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