Activation of co–mo–S hydrodesulfurization catalysts under refinery conditions: a combined SAXS/XAS study

Lennart van Haandel, Alessandro Longo, Wim Bras, Emiel J.M. Hensen, Thomas Weber (Corresponding author)

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Uittreksel

The activation of heterogeneous catalysts is challenging to follow experimentally and poorly understood in many cases. We combine in situ and time‐resolved X‐ray absorption spectroscopy and small‐angle X‐ray scattering to study the activation of Co‐Mo−S hydrotreating catalysts under conditions close to a refinery start‐up, i. e., 20 bar H2 pressure and gaseous H2S or liquid sulfiding agents. Formation of MoS2 nanoparticles involves three stages, namely aggregation (50–150 °C) and self‐assembly (150–250 °C) of two distinct amorphous MoSx intermediates, followed by a transition into layered structures that closely relate to the MoS2 structure. In stage III, these nuclei coalesce into the final MoS2 nanoparticles. Their growth distribution and stacking degree can be tailored by controlling the aggregation step, paving the way for the synthesis of better hydrotreating catalysts. Our experimental approach enables studying a broad range of supported amorphous nanomaterials at various length scales and operating conditions relevant to important catalytic processes.
TaalEngels
Pagina's5013-5017
Aantal pagina's5
TijdschriftChemCatChem
Volume11
Nummer van het tijdschrift20
DOI's
StatusGepubliceerd - 18 okt 2019

Vingerafdruk

Hydrodesulfurization
Chemical activation
activation
catalysts
Catalysts
Agglomeration
Metal refineries
Nanoparticles
nanoparticles
X ray absorption spectroscopy
X ray scattering
Nanostructured materials
Self assembly
self assembly
absorption spectroscopy
x rays
nuclei
Liquids
synthesis
liquids

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    Citeer dit

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    title = "Activation of co–mo–S hydrodesulfurization catalysts under refinery conditions: a combined SAXS/XAS study",
    abstract = "The activation of heterogeneous catalysts is challenging to follow experimentally and poorly understood in many cases. We combine in situ and time‐resolved X‐ray absorption spectroscopy and small‐angle X‐ray scattering to study the activation of Co‐Mo−S hydrotreating catalysts under conditions close to a refinery start‐up, i. e., 20 bar H2 pressure and gaseous H2S or liquid sulfiding agents. Formation of MoS2 nanoparticles involves three stages, namely aggregation (50–150 °C) and self‐assembly (150–250 °C) of two distinct amorphous MoSx intermediates, followed by a transition into layered structures that closely relate to the MoS2 structure. In stage III, these nuclei coalesce into the final MoS2 nanoparticles. Their growth distribution and stacking degree can be tailored by controlling the aggregation step, paving the way for the synthesis of better hydrotreating catalysts. Our experimental approach enables studying a broad range of supported amorphous nanomaterials at various length scales and operating conditions relevant to important catalytic processes.",
    keywords = "EXAFS, Heterogeneous catalyst, Hydrodesulfurization, Nanoparticle formation, SAXS",
    author = "{van Haandel}, Lennart and Alessandro Longo and Wim Bras and Hensen, {Emiel J.M.} and Thomas Weber",
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    doi = "10.1002/cctc.201901390",
    language = "English",
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    journal = "ChemCatChem",
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    Activation of co–mo–S hydrodesulfurization catalysts under refinery conditions : a combined SAXS/XAS study. / van Haandel, Lennart; Longo, Alessandro; Bras, Wim; Hensen, Emiel J.M.; Weber, Thomas (Corresponding author).

    In: ChemCatChem, Vol. 11, Nr. 20, 18.10.2019, blz. 5013-5017.

    Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

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    AU - Longo,Alessandro

    AU - Bras,Wim

    AU - Hensen,Emiel J.M.

    AU - Weber,Thomas

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    N2 - The activation of heterogeneous catalysts is challenging to follow experimentally and poorly understood in many cases. We combine in situ and time‐resolved X‐ray absorption spectroscopy and small‐angle X‐ray scattering to study the activation of Co‐Mo−S hydrotreating catalysts under conditions close to a refinery start‐up, i. e., 20 bar H2 pressure and gaseous H2S or liquid sulfiding agents. Formation of MoS2 nanoparticles involves three stages, namely aggregation (50–150 °C) and self‐assembly (150–250 °C) of two distinct amorphous MoSx intermediates, followed by a transition into layered structures that closely relate to the MoS2 structure. In stage III, these nuclei coalesce into the final MoS2 nanoparticles. Their growth distribution and stacking degree can be tailored by controlling the aggregation step, paving the way for the synthesis of better hydrotreating catalysts. Our experimental approach enables studying a broad range of supported amorphous nanomaterials at various length scales and operating conditions relevant to important catalytic processes.

    AB - The activation of heterogeneous catalysts is challenging to follow experimentally and poorly understood in many cases. We combine in situ and time‐resolved X‐ray absorption spectroscopy and small‐angle X‐ray scattering to study the activation of Co‐Mo−S hydrotreating catalysts under conditions close to a refinery start‐up, i. e., 20 bar H2 pressure and gaseous H2S or liquid sulfiding agents. Formation of MoS2 nanoparticles involves three stages, namely aggregation (50–150 °C) and self‐assembly (150–250 °C) of two distinct amorphous MoSx intermediates, followed by a transition into layered structures that closely relate to the MoS2 structure. In stage III, these nuclei coalesce into the final MoS2 nanoparticles. Their growth distribution and stacking degree can be tailored by controlling the aggregation step, paving the way for the synthesis of better hydrotreating catalysts. Our experimental approach enables studying a broad range of supported amorphous nanomaterials at various length scales and operating conditions relevant to important catalytic processes.

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