DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Mapping Metals Incorporation of a Whole Single Catalyst Particle Using Element Specific X-ray Nanotomography

Abstract

Full-field transmission X-ray microscopy has been used to determine the 3D structure of a whole individual fluid catalytic cracking (FCC) particle at high spatial resolution and in a fast, noninvasive manner, maintaining the full integrity of the particle. Using X-ray absorption mosaic imaging to combine multiple fields of view, computed tomography was performed to visualize the macropore structure of the catalyst and its availability for mass transport. We mapped the relative spatial distributions of Ni and Fe using multiple-energy tomography at the respective X-ray absorption K-edges and correlated these distributions with porosity and permeability of an equilibrated catalyst (E-cat) particle. Both metals were found to accumulate in outer layers of the particle, effectively decreasing porosity by clogging of pores and eventually restricting access into the FCC particle.

Authors:
 [1];  [2];  [1];  [2];  [2];  [1]
  1. Utrecht Univ. (The Netherlands)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1214384
Grant/Contract Number:  
AC03-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 1; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
02 PETROLEUM

Citation Formats

Meirer, Florian, Morris, Darius T., Kalirai, Sam, Liu, Yijin, Andrews, Joy C., and Weckhuysen, Bert M. Mapping Metals Incorporation of a Whole Single Catalyst Particle Using Element Specific X-ray Nanotomography. United States: N. p., 2015. Web. doi:10.1021/ja511503d.
Meirer, Florian, Morris, Darius T., Kalirai, Sam, Liu, Yijin, Andrews, Joy C., & Weckhuysen, Bert M. Mapping Metals Incorporation of a Whole Single Catalyst Particle Using Element Specific X-ray Nanotomography. United States. https://doi.org/10.1021/ja511503d
Meirer, Florian, Morris, Darius T., Kalirai, Sam, Liu, Yijin, Andrews, Joy C., and Weckhuysen, Bert M. Fri . "Mapping Metals Incorporation of a Whole Single Catalyst Particle Using Element Specific X-ray Nanotomography". United States. https://doi.org/10.1021/ja511503d. https://www.osti.gov/servlets/purl/1214384.
@article{osti_1214384,
title = {Mapping Metals Incorporation of a Whole Single Catalyst Particle Using Element Specific X-ray Nanotomography},
author = {Meirer, Florian and Morris, Darius T. and Kalirai, Sam and Liu, Yijin and Andrews, Joy C. and Weckhuysen, Bert M.},
abstractNote = {Full-field transmission X-ray microscopy has been used to determine the 3D structure of a whole individual fluid catalytic cracking (FCC) particle at high spatial resolution and in a fast, noninvasive manner, maintaining the full integrity of the particle. Using X-ray absorption mosaic imaging to combine multiple fields of view, computed tomography was performed to visualize the macropore structure of the catalyst and its availability for mass transport. We mapped the relative spatial distributions of Ni and Fe using multiple-energy tomography at the respective X-ray absorption K-edges and correlated these distributions with porosity and permeability of an equilibrated catalyst (E-cat) particle. Both metals were found to accumulate in outer layers of the particle, effectively decreasing porosity by clogging of pores and eventually restricting access into the FCC particle.},
doi = {10.1021/ja511503d},
journal = {Journal of the American Chemical Society},
number = 1,
volume = 137,
place = {United States},
year = {Fri Jan 02 00:00:00 EST 2015},
month = {Fri Jan 02 00:00:00 EST 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 68 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Visualization of the Equilibrium FCC Catalyst Surface by AFM and SEM–EDS
journal, October 2003


Imaging Catalysts at Work: A Hierarchical Approach from the Macro- to the Meso- and Nano-scale
journal, November 2012

  • Grunwaldt, Jan-Dierk; Wagner, Jakob B.; Dunin-Borkowski, Rafal E.
  • ChemCatChem, Vol. 5, Issue 1
  • DOI: 10.1002/cctc.201200356

Vanadium passivation of cracking catalysts by imaging secondary ion mass spectrometry
journal, January 1995


Study of the accessibility effect on the irreversible deactivation of FCC catalysts from contaminant feed metals
journal, September 2007


Catalytic activity in individual cracking catalyst particles imaged throughout different life stages by selective staining
journal, September 2011

  • Buurmans, Inge L. C.; Ruiz-Martínez, Javier; Knowles, William V.
  • Nature Chemistry, Vol. 3, Issue 11
  • DOI: 10.1038/nchem.1148

Integrated Laser and Electron Microscopy Correlates Structure of Fluid Catalytic Cracking Particles to Brønsted Acidity
journal, December 2011

  • Karreman, Matthia A.; Buurmans, Inge L. C.; Geus, John W.
  • Angewandte Chemie International Edition, Vol. 51, Issue 6
  • DOI: 10.1002/anie.201106651

Multi Length Scale Microstructural Investigations of a Commercially Available Li-Ion Battery Electrode
journal, January 2012

  • Shearing, P. R.; Brandon, N. P.; Gelb, J.
  • Journal of The Electrochemical Society, Vol. 159, Issue 7
  • DOI: 10.1149/2.053207jes

Comparison of SOFC cathode microstructure quantified using X-ray nanotomography and focused ion beam–scanning electron microscopy
journal, June 2011

  • Nelson, George J.; Harris, William M.; Lombardo, Jeffrey J.
  • Electrochemistry Communications, Vol. 13, Issue 6
  • DOI: 10.1016/j.elecom.2011.03.016

3D Non-destructive morphological analysis of a solid oxide fuel cell anode using full-field X-ray nano-tomography
journal, November 2012


Nanoscale elemental sensitivity study of Nd 2 Fe 14 B using absorption correlation tomography : Nanoscale Elemental Sensitivity Study of N
journal, August 2013

  • Kao, Thomas L.; Shi, Crystal Y.; Wang, Junyue
  • Microscopy Research and Technique, Vol. 76, Issue 11
  • DOI: 10.1002/jemt.22273

Phase retrieval using polychromatic illumination for transmission X-ray microscopy
journal, January 2011

  • Liu, Yijin; Andrews, Joy C.; Wang, Junyue
  • Optics Express, Vol. 19, Issue 2
  • DOI: 10.1364/oe.19.000540

Works referencing / citing this record:

Spatial and temporal exploration of heterogeneous catalysts with synchrotron radiation
journal, August 2018


Non-empirical identification of trigger sites in heterogeneous processes using persistent homology
journal, February 2018


The frontiers of energy
journal, January 2016

  • Armstrong, Robert C.; Wolfram, Catherine; de Jong, Krijn P.
  • Nature Energy, Vol. 1, Issue 1
  • DOI: 10.1038/nenergy.2015.20

Micro-spectroscopy of HKUST-1 metal–organic framework crystals loaded with tetracyanoquinodimethane: effects of water on host–guest chemistry and electrical conductivity
journal, January 2019

  • Rivera-Torrente, Miguel; Filez, Matthias; Schneider, Christian
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 46
  • DOI: 10.1039/c9cp05082e

Nickel Poisoning of a Cracking Catalyst Unravelled by Single‐Particle X‐ray Fluorescence‐Diffraction‐Absorption Tomography
journal, January 2020

  • Gambino, Marianna; Veselý, Martin; Filez, Matthias
  • Angewandte Chemie International Edition, Vol. 59, Issue 10
  • DOI: 10.1002/anie.201914950

Chemical imaging of Fischer-Tropsch catalysts under operating conditions
journal, March 2017

  • Price, Stephen W. T.; Martin, David J.; Parsons, Aaron D.
  • Science Advances, Vol. 3, Issue 3
  • DOI: 10.1126/sciadv.1602838

Nickel Poisoning of a Cracking Catalyst Unravelled by Single‐Particle X‐ray Fluorescence‐Diffraction‐Absorption Tomography
journal, January 2020

  • Gambino, Marianna; Veselý, Martin; Filez, Matthias
  • Angewandte Chemie, Vol. 132, Issue 10
  • DOI: 10.1002/ange.201914950

Magnetophoretic Sorting of Single Catalyst Particles
journal, August 2018

  • Solsona, Miguel; Nieuwelink, Anne‐Eva; Meirer, Florian
  • Angewandte Chemie International Edition, Vol. 57, Issue 33
  • DOI: 10.1002/anie.201804942

Tailoring and visualizing the pore architecture of hierarchical zeolites
journal, January 2015

  • Wei, Ying; Parmentier, Tanja E.; de Jong, Krijn P.
  • Chemical Society Reviews, Vol. 44, Issue 20
  • DOI: 10.1039/c5cs00155b

Visualization of the effect of additives on the nanostructures of individual bio-inspired calcite crystals
journal, January 2019

  • Ihli, Johannes; Clark, Jesse N.; Kanwal, Nasima
  • Chemical Science, Vol. 10, Issue 4
  • DOI: 10.1039/c8sc03733g

Fluid catalytic cracking technology: current status and recent discoveries on catalyst contamination
journal, December 2018


Materials characterization by synchrotron x-ray microprobes and nanoprobes
journal, June 2018


Oxygen-diffusion-driven oxidation behavior and tracking areas visualized by X-ray spectro-ptychography with unsupervised learning
journal, April 2019


Assessment of the Location of Pt Nanoparticles in Pt/zeolite Y/γ‐Al 2 O 3 Composite Catalysts
journal, October 2019

  • Oenema, Jogchum; Hofmann, Jan P.; Hensen, Emiel J. M.
  • ChemCatChem, Vol. 12, Issue 2
  • DOI: 10.1002/cctc.201901617

Fluid catalytic cracking: recent developments on the grand old lady of zeolite catalysis
journal, January 2015

  • Vogt, E. T. C.; Weckhuysen, B. M.
  • Chemical Society Reviews, Vol. 44, Issue 20
  • DOI: 10.1039/c5cs00376h

Magnetophoretic Sorting of Single Catalyst Particles
journal, August 2018

  • Solsona, Miguel; Nieuwelink, Anne‐Eva; Meirer, Florian
  • Angewandte Chemie, Vol. 130, Issue 33
  • DOI: 10.1002/ange.201804942

Nanoscale Chemical Imaging of an Individual Catalyst Particle with Soft X-ray Ptychography
journal, February 2016


FIB-SEM Tomography Probes the Mesoscale Pore Space of an Individual Catalytic Cracking Particle
journal, April 2016

  • de Winter, D. A. Matthijs; Meirer, Florian; Weckhuysen, Bert M.
  • ACS Catalysis, Vol. 6, Issue 5
  • DOI: 10.1021/acscatal.6b00302

Relating structure and composition with accessibility of a single catalyst particle using correlative 3-dimensional micro-spectroscopy
journal, August 2016

  • Liu, Yijin; Meirer, Florian; Krest, Courtney M.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12634

A three-dimensional view of structural changes caused by deactivation of fluid catalytic cracking catalysts
journal, October 2017


Fluid catalytic cracking: recent developments on the grand old lady of zeolite catalysis
journal, January 2015

  • Vogt, E. T. C.; Weckhuysen, B. M.
  • Chemical Society Reviews, Vol. 44, Issue 20
  • DOI: 10.1039/c5cs00376h

Visualization of the effect of additives on the nanostructures of individual bio-inspired calcite crystals
journal, January 2019

  • Ihli, Johannes; Clark, Jesse N.; Kanwal, Nasima
  • Chemical Science, Vol. 10, Issue 4
  • DOI: 10.1039/c8sc03733g

Life and death of a single catalytic cracking particle
journal, April 2015


Chemical imaging of Fischer-Tropsch catalysts under operating conditions
journal, March 2017

  • Price, Stephen W. T.; Martin, David J.; Parsons, Aaron D.
  • Science Advances, Vol. 3, Issue 3
  • DOI: 10.1126/sciadv.1602838