Nickel Poisoning of a Cracking Catalyst Unravelled by Single X-ray Fluorescence-Diffraction-Absorption Tomography

Marianna Gambino; Martin Veselý; Matthias Filez; Ramon Oord; Dario Ferreira Sanchez; Daniel Grolimund; Nikolai Nesterenko; Delphine Minoux; Marianne Maquet; Florian Meirer; Bert M. Weckhuysen

doi:10.1002/ANGE.201914950

Nickel Poisoning of a Cracking Catalyst Unravelled by Single X-ray Fluorescence-Diffraction-Absorption Tomography

Marianna Gambino, Martin Veselý, Matthias Filez, Ramon Oord, Dario Ferreira Sanchez, Daniel Grolimund, Nikolai Nesterenko, Delphine Minoux, Marianne Maquet, Florian Meirer^*, Bert M. Weckhuysen^*

^*Corresponding author for this work

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

Abstract

Ni contamination from crude oil in the fluid catalytic cracking (FCC) process is one of the primary sources of catalyst deactivation, thereby promoting dehydrogenation-hydrogenation and speeding up coke growth. Herein, single-particle X-ray fluorescence, diffraction and absorption (μXRF-μXRD-μXAS) tomography is used in combination with confocal fluorescence microscopy (CFM) after thiophene staining to spatially resolve Ni interaction with catalyst components and study zeolite degradation, including the processes of dealumination and Br0nsted acid sites distribution changes. The comparison between a Ni-lean particle, exposed to hydrotreated feedstock, and a Ni-rich one, exposed to non-hydrotreated feedstock, reveals a preferential interaction of Ni, found in co-localization with Fe, with the γ-Al₂O₃ matrix, leading to the formation of spinel-type hotspots. Although both particles show similar surface zeolite degradation, the Ni-rich particle displays higher dealumination and a clear Brønsted acidity drop.

Original language	English
Pages (from-to)	3950-3955
Number of pages	6
Journal	Advanced Materials
Volume	132
Issue number	10
DOIs	https://doi.org/10.1002/ANGE.201914950
Publication status	Published - Mar 2020

Bibliographical note

Funding Information:
B.M.W. thanks Total and an European Research Council (ERC) Advanced Grant (grant number 321140) for financial support for this project, while F.M. acknowledges a personal VIDI grant from the Netherlands Organization for Scientific Research (NWO). Total is thanked for providing the FCC samples. We also acknowledge the Swiss Light Source (SLS) for providing access to microXAS X05LA beamline.

Funding Information:
B.M.W, thanks Total and an European Research Council (ERC) Advanced Grant (grant number 321140) for financial support for this project, while F.M. acknowledges a personal VIDI grant from the Netherlands Organization for Scientific Research (NWO). Total is thanked for providing the FCC.

Publisher Copyright:
© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Funding

B.M.W. thanks Total and an European Research Council (ERC) Advanced Grant (grant number 321140) for financial support for this project, while F.M. acknowledges a personal VIDI grant from the Netherlands Organization for Scientific Research (NWO). Total is thanked for providing the FCC samples. We also acknowledge the Swiss Light Source (SLS) for providing access to microXAS X05LA beamline. B.M.W, thanks Total and an European Research Council (ERC) Advanced Grant (grant number 321140) for financial support for this project, while F.M. acknowledges a personal VIDI grant from the Netherlands Organization for Scientific Research (NWO). Total is thanked for providing the FCC.

Keywords

catalyst deactivation
fluid catalytic cracking (FCC)
heterogeneous catalysis
X-ray microscopy
zeolites

Access to Document

10.1002/ANGE.201914950

Angewandte Chemie - 2020 - Gambino - Nickel Poisoning of a Cracking Catalyst Unravelled by Single‐Particle X‐rayFinal published version, 2.74 MBLicence: Taverne

Cite this

@article{51842cb3105447efb9d6f5740f00b8be,

title = "Nickel Poisoning of a Cracking Catalyst Unravelled by Single X-ray Fluorescence-Diffraction-Absorption Tomography",

abstract = "Ni contamination from crude oil in the fluid catalytic cracking (FCC) process is one of the primary sources of catalyst deactivation, thereby promoting dehydrogenation-hydrogenation and speeding up coke growth. Herein, single-particle X-ray fluorescence, diffraction and absorption (μXRF-μXRD-μXAS) tomography is used in combination with confocal fluorescence microscopy (CFM) after thiophene staining to spatially resolve Ni interaction with catalyst components and study zeolite degradation, including the processes of dealumination and Br0nsted acid sites distribution changes. The comparison between a Ni-lean particle, exposed to hydrotreated feedstock, and a Ni-rich one, exposed to non-hydrotreated feedstock, reveals a preferential interaction of Ni, found in co-localization with Fe, with the γ-Al2O3 matrix, leading to the formation of spinel-type hotspots. Although both particles show similar surface zeolite degradation, the Ni-rich particle displays higher dealumination and a clear Br{\o}nsted acidity drop.",

keywords = "catalyst deactivation, fluid catalytic cracking (FCC), heterogeneous catalysis, X-ray microscopy, zeolites",

author = "Marianna Gambino and Martin Vesel{\'y} and Matthias Filez and Ramon Oord and Sanchez, {Dario Ferreira} and Daniel Grolimund and Nikolai Nesterenko and Delphine Minoux and Marianne Maquet and Florian Meirer and Weckhuysen, {Bert M.}",

note = "Funding Information: B.M.W. thanks Total and an European Research Council (ERC) Advanced Grant (grant number 321140) for financial support for this project, while F.M. acknowledges a personal VIDI grant from the Netherlands Organization for Scientific Research (NWO). Total is thanked for providing the FCC samples. We also acknowledge the Swiss Light Source (SLS) for providing access to microXAS X05LA beamline. Funding Information: B.M.W, thanks Total and an European Research Council (ERC) Advanced Grant (grant number 321140) for financial support for this project, while F.M. acknowledges a personal VIDI grant from the Netherlands Organization for Scientific Research (NWO). Total is thanked for providing the FCC. Publisher Copyright: {\textcopyright} 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.",

year = "2020",

month = mar,

doi = "10.1002/ANGE.201914950",

language = "English",

volume = "132",

pages = "3950--3955",

journal = "Advanced Materials",

issn = "0935-9648",

publisher = "Wiley-Blackwell",

number = "10",

}

TY - JOUR

T1 - Nickel Poisoning of a Cracking Catalyst Unravelled by Single X-ray Fluorescence-Diffraction-Absorption Tomography

AU - Gambino, Marianna

AU - Veselý, Martin

AU - Filez, Matthias

AU - Oord, Ramon

AU - Sanchez, Dario Ferreira

AU - Grolimund, Daniel

AU - Nesterenko, Nikolai

AU - Minoux, Delphine

AU - Maquet, Marianne

AU - Meirer, Florian

AU - Weckhuysen, Bert M.

N1 - Funding Information: B.M.W. thanks Total and an European Research Council (ERC) Advanced Grant (grant number 321140) for financial support for this project, while F.M. acknowledges a personal VIDI grant from the Netherlands Organization for Scientific Research (NWO). Total is thanked for providing the FCC samples. We also acknowledge the Swiss Light Source (SLS) for providing access to microXAS X05LA beamline. Funding Information: B.M.W, thanks Total and an European Research Council (ERC) Advanced Grant (grant number 321140) for financial support for this project, while F.M. acknowledges a personal VIDI grant from the Netherlands Organization for Scientific Research (NWO). Total is thanked for providing the FCC. Publisher Copyright: © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

PY - 2020/3

Y1 - 2020/3

N2 - Ni contamination from crude oil in the fluid catalytic cracking (FCC) process is one of the primary sources of catalyst deactivation, thereby promoting dehydrogenation-hydrogenation and speeding up coke growth. Herein, single-particle X-ray fluorescence, diffraction and absorption (μXRF-μXRD-μXAS) tomography is used in combination with confocal fluorescence microscopy (CFM) after thiophene staining to spatially resolve Ni interaction with catalyst components and study zeolite degradation, including the processes of dealumination and Br0nsted acid sites distribution changes. The comparison between a Ni-lean particle, exposed to hydrotreated feedstock, and a Ni-rich one, exposed to non-hydrotreated feedstock, reveals a preferential interaction of Ni, found in co-localization with Fe, with the γ-Al2O3 matrix, leading to the formation of spinel-type hotspots. Although both particles show similar surface zeolite degradation, the Ni-rich particle displays higher dealumination and a clear Brønsted acidity drop.

AB - Ni contamination from crude oil in the fluid catalytic cracking (FCC) process is one of the primary sources of catalyst deactivation, thereby promoting dehydrogenation-hydrogenation and speeding up coke growth. Herein, single-particle X-ray fluorescence, diffraction and absorption (μXRF-μXRD-μXAS) tomography is used in combination with confocal fluorescence microscopy (CFM) after thiophene staining to spatially resolve Ni interaction with catalyst components and study zeolite degradation, including the processes of dealumination and Br0nsted acid sites distribution changes. The comparison between a Ni-lean particle, exposed to hydrotreated feedstock, and a Ni-rich one, exposed to non-hydrotreated feedstock, reveals a preferential interaction of Ni, found in co-localization with Fe, with the γ-Al2O3 matrix, leading to the formation of spinel-type hotspots. Although both particles show similar surface zeolite degradation, the Ni-rich particle displays higher dealumination and a clear Brønsted acidity drop.

KW - catalyst deactivation

KW - fluid catalytic cracking (FCC)

KW - heterogeneous catalysis

KW - X-ray microscopy

KW - zeolites

UR - http://www.scopus.com/inward/record.url?scp=85134881961&partnerID=8YFLogxK

U2 - 10.1002/ANGE.201914950

DO - 10.1002/ANGE.201914950

M3 - Article

AN - SCOPUS:85134881961

SN - 0935-9648

VL - 132

SP - 3950

EP - 3955

JO - Advanced Materials

JF - Advanced Materials

IS - 10

ER -

Nickel Poisoning of a Cracking Catalyst Unravelled by Single X-ray Fluorescence-Diffraction-Absorption Tomography

Abstract

Bibliographical note

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this