Capturing the Genesis of an Active Fischer–Tropsch Synthesis Catalyst with Operando X-ray Nanospectroscopy

Ilse K. van Ravenhorst; Charlotte Vogt; Heiko Oosterbeek; Koen W. Bossers; José G. Moya-Cancino; Alexander P. van Bavel; Ad M.J. van der Eerden; David Vine; Frank M.F. de Groot; Florian Meirer; Bert M. Weckhuysen

doi:10.1002/anie.201806354

Capturing the Genesis of an Active Fischer–Tropsch Synthesis Catalyst with Operando X-ray Nanospectroscopy

Ilse K. van Ravenhorst
, Charlotte Vogt
, Heiko Oosterbeek
, Koen W. Bossers
, José G. Moya-Cancino
, Alexander P. van Bavel
, Ad M.J. van der Eerden
, David Vine
, Frank M.F. de Groot
, Florian Meirer
, Bert M. Weckhuysen

Research output: Contribution to journal › Article › peer-review

Abstract

A state-of-the-art operando spectroscopic technique is applied to Co/TiO₂ catalysts, which account for nearly half of the world's transportation fuels produced by Fischer–Tropsch catalysis. This allows determination of, at a spatial resolution of approximately 50 nm, the interdependence of formed hydrocarbon species in the inorganic catalyst. Observed trends show intra- and interparticular heterogeneities previously believed not to occur in particles under 200 μm. These heterogeneities are strongly dependent on changes in H₂/CO ratio, but also on changes thereby induced on the Co and Ti valence states. We have captured the genesis of an active FTS particle over its propagation to steady-state operation, in which microgradients lead to the gradual saturation of the Co/TiO₂ catalyst surface with long chain hydrocarbons (i.e., organic film formation).

Original language	English
Pages (from-to)	11957-11962
Number of pages	6
Journal	Angewandte Chemie - International Edition
Volume	57
Issue number	37
DOIs	https://doi.org/10.1002/anie.201806354
State	Published - 10 Sep 2018
Externally published	Yes

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Keywords

Fischer–Tropsch synthesis
X-ray microspectroscopy
chemical imaging
heterogeneous catalysis
nanoparticles

ASJC Scopus subject areas

Catalysis
General Chemistry

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10.1002/anie.201806354

Cite this

van Ravenhorst, I. K., Vogt, C., Oosterbeek, H., Bossers, K. W., Moya-Cancino, J. G., van Bavel, A. P., van der Eerden, A. M. J., Vine, D., de Groot, F. M. F., Meirer, F., & Weckhuysen, B. M. (2018). Capturing the Genesis of an Active Fischer–Tropsch Synthesis Catalyst with Operando X-ray Nanospectroscopy. Angewandte Chemie - International Edition, 57(37), 11957-11962. https://doi.org/10.1002/anie.201806354

@article{c9c237893cb24ce3b13cad9f6920c185,

title = "Capturing the Genesis of an Active Fischer–Tropsch Synthesis Catalyst with Operando X-ray Nanospectroscopy",

abstract = "A state-of-the-art operando spectroscopic technique is applied to Co/TiO2 catalysts, which account for nearly half of the world's transportation fuels produced by Fischer–Tropsch catalysis. This allows determination of, at a spatial resolution of approximately 50 nm, the interdependence of formed hydrocarbon species in the inorganic catalyst. Observed trends show intra- and interparticular heterogeneities previously believed not to occur in particles under 200 μm. These heterogeneities are strongly dependent on changes in H2/CO ratio, but also on changes thereby induced on the Co and Ti valence states. We have captured the genesis of an active FTS particle over its propagation to steady-state operation, in which microgradients lead to the gradual saturation of the Co/TiO2 catalyst surface with long chain hydrocarbons (i.e., organic film formation).",

keywords = "Fischer–Tropsch synthesis, X-ray microspectroscopy, chemical imaging, heterogeneous catalysis, nanoparticles",

author = "\{van Ravenhorst\}, \{Ilse K.\} and Charlotte Vogt and Heiko Oosterbeek and Bossers, \{Koen W.\} and Moya-Cancino, \{Jos{\'e} G.\} and \{van Bavel\}, \{Alexander P.\} and \{van der Eerden\}, \{Ad M.J.\} and David Vine and \{de Groot\}, \{Frank M.F.\} and Florian Meirer and Weckhuysen, \{Bert M.\}",

note = "Funding Information: B.M.W. thanks the Netherlands Organization for Scientific Research (NWO) and Shell Global Solutions International B.V. for a CHIPP research grant as well as NWO for a Gravitation program (Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC)). Dr. B. Morana and Dr. G. Pandraud (Else Kooi Lab, TUDelft, The Netherlands) are acknowledged for providing the nanoreactors and useful insights. Dr. S. R. Bare (SLAC, USA) is thanked for carefully reading the manuscript before submission. Prof. A. P. Hitchcock (McMaster University, Canada) is thanked for help with the assignment of XAS features. Publisher Copyright: {\textcopyright} 2018 Wiley-VCH Verlag GmbH \& Co. KGaA, Weinheim",

year = "2018",

month = sep,

day = "10",

doi = "10.1002/anie.201806354",

language = "English",

volume = "57",

pages = "11957--11962",

journal = "Angewandte Chemie - International Edition",

issn = "1433-7851",

publisher = "John Wiley and Sons Ltd",

number = "37",

}

van Ravenhorst, IK, Vogt, C, Oosterbeek, H, Bossers, KW, Moya-Cancino, JG, van Bavel, AP, van der Eerden, AMJ, Vine, D, de Groot, FMF, Meirer, F & Weckhuysen, BM 2018, 'Capturing the Genesis of an Active Fischer–Tropsch Synthesis Catalyst with Operando X-ray Nanospectroscopy', Angewandte Chemie - International Edition, vol. 57, no. 37, pp. 11957-11962. https://doi.org/10.1002/anie.201806354

TY - JOUR

T1 - Capturing the Genesis of an Active Fischer–Tropsch Synthesis Catalyst with Operando X-ray Nanospectroscopy

AU - van Ravenhorst, Ilse K.

AU - Vogt, Charlotte

AU - Oosterbeek, Heiko

AU - Bossers, Koen W.

AU - Moya-Cancino, José G.

AU - van Bavel, Alexander P.

AU - van der Eerden, Ad M.J.

AU - Vine, David

AU - de Groot, Frank M.F.

AU - Meirer, Florian

AU - Weckhuysen, Bert M.

N1 - Funding Information: B.M.W. thanks the Netherlands Organization for Scientific Research (NWO) and Shell Global Solutions International B.V. for a CHIPP research grant as well as NWO for a Gravitation program (Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC)). Dr. B. Morana and Dr. G. Pandraud (Else Kooi Lab, TUDelft, The Netherlands) are acknowledged for providing the nanoreactors and useful insights. Dr. S. R. Bare (SLAC, USA) is thanked for carefully reading the manuscript before submission. Prof. A. P. Hitchcock (McMaster University, Canada) is thanked for help with the assignment of XAS features. Publisher Copyright: © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2018/9/10

Y1 - 2018/9/10

N2 - A state-of-the-art operando spectroscopic technique is applied to Co/TiO2 catalysts, which account for nearly half of the world's transportation fuels produced by Fischer–Tropsch catalysis. This allows determination of, at a spatial resolution of approximately 50 nm, the interdependence of formed hydrocarbon species in the inorganic catalyst. Observed trends show intra- and interparticular heterogeneities previously believed not to occur in particles under 200 μm. These heterogeneities are strongly dependent on changes in H2/CO ratio, but also on changes thereby induced on the Co and Ti valence states. We have captured the genesis of an active FTS particle over its propagation to steady-state operation, in which microgradients lead to the gradual saturation of the Co/TiO2 catalyst surface with long chain hydrocarbons (i.e., organic film formation).

AB - A state-of-the-art operando spectroscopic technique is applied to Co/TiO2 catalysts, which account for nearly half of the world's transportation fuels produced by Fischer–Tropsch catalysis. This allows determination of, at a spatial resolution of approximately 50 nm, the interdependence of formed hydrocarbon species in the inorganic catalyst. Observed trends show intra- and interparticular heterogeneities previously believed not to occur in particles under 200 μm. These heterogeneities are strongly dependent on changes in H2/CO ratio, but also on changes thereby induced on the Co and Ti valence states. We have captured the genesis of an active FTS particle over its propagation to steady-state operation, in which microgradients lead to the gradual saturation of the Co/TiO2 catalyst surface with long chain hydrocarbons (i.e., organic film formation).

KW - Fischer–Tropsch synthesis

KW - X-ray microspectroscopy

KW - chemical imaging

KW - heterogeneous catalysis

KW - nanoparticles

UR - https://www.scopus.com/pages/publications/85052744175

U2 - 10.1002/anie.201806354

DO - 10.1002/anie.201806354

M3 - Article

C2 - 30070756

SN - 1433-7851

VL - 57

SP - 11957

EP - 11962

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 37

ER -

Capturing the Genesis of an Active Fischer–Tropsch Synthesis Catalyst with Operando X-ray Nanospectroscopy

Abstract

UN SDGs

Keywords

ASJC Scopus subject areas

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