Hierarchical Structure of NiMo Hydrodesulfurization Catalysts Determined by Ptychographic X-Ray Computed Tomography

J. Ihli (Corresponding author), L. Bloch, Frank Krumeich, K. Wakonig, M. Holler, M. Guizar-Sicairos, Thomas Weber, J. Cesar da Silva, Jeroen A. Van Bokhoven

Research output: Contribution to journalArticleAcademicpeer-review

18 Citations (Scopus)

Abstract


Hydrodesulphurization, the removal of sulphur from crude oils, is an essential catalytic process in the petroleum industry safeguarding the production of clean hydrocarbons. Sulphur removal is critical for the functionality of downstream processes and vital to the elimination of environmental pollutants. The effectiveness of such an endeavour is among other factors determined by the structural arrangement of the heterogeneous catalyst. Namely, the accessibility of the catalytically active molybdenum disulphide (MoS2) slabs located on the surfaces of a porous alumina carrier. Here, we examined a series of pristine sulfided Mo and NiMo hydrodesulphurization catalysts of increasing metal loading prepared on commercial alumina carriers using ptychographic X‐ray computed nanotomography. Structural analysis revealed a build consisting of two interwoven support matrix elements differing in nanoporosity. With increasing metal loading, approaching that of industrial catalysts, these matrix elements exhibit a progressively dissimilar MoS2 surface coverage as well as MoS2 cluster formation at the matrix element boundaries. This is suggestive of metal deposition limitations and/ or catalyst activation and following prohibitive of optimal catalytic utilization. These results will allow for diffusivity calculations, a better rationale of current generation catalyst performance as well as a better distribution of the active phase in next‐generation hydrodesulphurization catalysts.
Original languageEnglish
Pages (from-to)17266-17271
Number of pages6
JournalAngewandte Chemie - International Edition
Volume59
Issue number39
DOIs
Publication statusPublished - 21 Sept 2020

Funding

L.B. is supported by an ESRF Studentship. The work of J.I. is supported by funding from the Swiss National Science Foundation (SNF), Project No. 179886 and 153556. Ptychographic tomography instrumentation was supported by SNF R'Equip (Project No. 145056). Ptychography experiments were performed at the coherent small‐angle ‐ray scattering (cSAXS) beamline at the Swiss Light Source at the Paul Scherrer Institut in Villigen, Switzerland. We thank X. Donath for technical support at the cSAXS beamline. Electron microscopy and sample preparation for PXCT experiments were performed at the Scientific Centre for Optical and Electron Microscopy (ScopeM) ETH Zurich. We thank Arend‐Jan van Welsenes (Shell Technology Centre Amsterdam) for the preparation of the HDS catalysts and the bare alumina carrier. x L.B. is supported by an ESRF Studentship. The work of J.I. is supported by funding from the Swiss National Science Foundation (SNF), Project No. 179886 and 153556. Ptychographic tomography instrumentation was supported by SNF R'Equip (Project No. 145056). Ptychography experiments were performed at the coherent small-angle x-ray scattering (cSAXS) beamline at the Swiss Light Source at the Paul Scherrer Institut in Villigen, Switzerland. We thank X. Donath for technical support at the cSAXS beamline. Electron microscopy and sample preparation for PXCT experiments were performed at the Scientific Centre for Optical and Electron Microscopy (ScopeM) ETH Zurich. We thank Arend-Jan van Welsenes (Shell Technology Centre Amsterdam) for the preparation of the HDS catalysts and the bare alumina carrier.

FundersFunder number
SNF R'Equip145056
Shell Technology Centres
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung153556, 179886
ETH Zurich

    Keywords

    • heterogeneous catalysis
    • hydrodesulfurization
    • molybdenum disulphide
    • ptychographic tomography
    • supported catalyst

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