Carbon Deposit Analysis in Catalyst Deactivation, Regeneration, and Rejuvenation

Eelco T.C. Vogt; Donglong Fu; Bert M. Weckhuysen

doi:10.1002/anie.202300319

Carbon Deposit Analysis in Catalyst Deactivation, Regeneration, and Rejuvenation

Eelco T.C. Vogt^*, Donglong Fu, Bert M. Weckhuysen^*

^*Corresponding author for this work

Sub Inorganic Chemistry and Catalysis

Research output: Contribution to journal › Review article › peer-review

Abstract

Hydrocarbon conversion catalysts suffer from deactivation by deposition or formation of carbon deposits. Carbon deposit formation is thermodynamically favored above 350 °C, even in some hydrogen-rich environments. We discuss four basic mechanisms: a carbenium-ion based mechanism taking place on acid sites of zeolites or bifunctional catalysts, a metal-induced formation of soft coke (i.e., oligomers of small olefins) on bifunctional catalysts, a radical-mediated mechanism in higher-temperature processes, and fast-growing carbon filament formation. Catalysts deactivate because carbon deposits block pores at different length scales, or directly block active sites. Some deactivated catalysts can be re-used, others can be regenerated or have to be discarded. Catalyst and process design can mitigate the effects of deactivation. New analytical tools allow for the direct observation (in some cases even under in situ or operando conditions) of the 3D-distribution of coke-type species as a function of catalyst structure and lifetime.

Original language	English
Article number	e202300319
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	29
DOIs	https://doi.org/10.1002/anie.202300319
Publication status	Published - 17 Jul 2023

Bibliographical note

Funding Information:
BMW acknowledges funding from the Netherlands Research Council (NWO) in the frame of a Gravitation Program (Multiscale Catalytic Energy Conversion, MCEC), the Advanced Research Consortium (ARC) Chemical Building Blocks Consortium (CBBC), as well as the European Research Council (ERC) Advanced Grant (no. 321140) and ERC Proof‐of‐Concept grant (no. 862283). The authors thank Dr. Thomas Hartman (Utrecht University) for the help with the design of some of the figures.

Publisher Copyright:
© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

Funding

BMW acknowledges funding from the Netherlands Research Council (NWO) in the frame of a Gravitation Program (Multiscale Catalytic Energy Conversion, MCEC), the Advanced Research Consortium (ARC) Chemical Building Blocks Consortium (CBBC), as well as the European Research Council (ERC) Advanced Grant (no. 321140) and ERC Proof‐of‐Concept grant (no. 862283). The authors thank Dr. Thomas Hartman (Utrecht University) for the help with the design of some of the figures.

Funders	Funder number
Netherlands Research Council (NWO)
Advanced Research Consortium (ARC) Chemical Building Blocks Consortium
European Research Council (ERC)	321140
ERC	862283

Keywords

Carbon Deposition
Catalyst Deactivation
Catalyst Design
Coke
Coke Analysis

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Angew Chem Int Ed - 2023 - Vogt - Carbon Deposit Analysis in Catalyst Deactivation Regeneration and Rejuvenation (1)Final published version, 21.2 MBLicence: CC BY

Cite this

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title = "Carbon Deposit Analysis in Catalyst Deactivation, Regeneration, and Rejuvenation",

abstract = "Hydrocarbon conversion catalysts suffer from deactivation by deposition or formation of carbon deposits. Carbon deposit formation is thermodynamically favored above 350 °C, even in some hydrogen-rich environments. We discuss four basic mechanisms: a carbenium-ion based mechanism taking place on acid sites of zeolites or bifunctional catalysts, a metal-induced formation of soft coke (i.e., oligomers of small olefins) on bifunctional catalysts, a radical-mediated mechanism in higher-temperature processes, and fast-growing carbon filament formation. Catalysts deactivate because carbon deposits block pores at different length scales, or directly block active sites. Some deactivated catalysts can be re-used, others can be regenerated or have to be discarded. Catalyst and process design can mitigate the effects of deactivation. New analytical tools allow for the direct observation (in some cases even under in situ or operando conditions) of the 3D-distribution of coke-type species as a function of catalyst structure and lifetime.",

keywords = "Carbon Deposition, Catalyst Deactivation, Catalyst Design, Coke, Coke Analysis",

author = "Vogt, {Eelco T.C.} and Donglong Fu and Weckhuysen, {Bert M.}",

note = "Funding Information: BMW acknowledges funding from the Netherlands Research Council (NWO) in the frame of a Gravitation Program (Multiscale Catalytic Energy Conversion, MCEC), the Advanced Research Consortium (ARC) Chemical Building Blocks Consortium (CBBC), as well as the European Research Council (ERC) Advanced Grant (no. 321140) and ERC Proof‐of‐Concept grant (no. 862283). The authors thank Dr. Thomas Hartman (Utrecht University) for the help with the design of some of the figures. Publisher Copyright: {\textcopyright} 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.",

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N1 - Funding Information: BMW acknowledges funding from the Netherlands Research Council (NWO) in the frame of a Gravitation Program (Multiscale Catalytic Energy Conversion, MCEC), the Advanced Research Consortium (ARC) Chemical Building Blocks Consortium (CBBC), as well as the European Research Council (ERC) Advanced Grant (no. 321140) and ERC Proof‐of‐Concept grant (no. 862283). The authors thank Dr. Thomas Hartman (Utrecht University) for the help with the design of some of the figures. Publisher Copyright: © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

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N2 - Hydrocarbon conversion catalysts suffer from deactivation by deposition or formation of carbon deposits. Carbon deposit formation is thermodynamically favored above 350 °C, even in some hydrogen-rich environments. We discuss four basic mechanisms: a carbenium-ion based mechanism taking place on acid sites of zeolites or bifunctional catalysts, a metal-induced formation of soft coke (i.e., oligomers of small olefins) on bifunctional catalysts, a radical-mediated mechanism in higher-temperature processes, and fast-growing carbon filament formation. Catalysts deactivate because carbon deposits block pores at different length scales, or directly block active sites. Some deactivated catalysts can be re-used, others can be regenerated or have to be discarded. Catalyst and process design can mitigate the effects of deactivation. New analytical tools allow for the direct observation (in some cases even under in situ or operando conditions) of the 3D-distribution of coke-type species as a function of catalyst structure and lifetime.

AB - Hydrocarbon conversion catalysts suffer from deactivation by deposition or formation of carbon deposits. Carbon deposit formation is thermodynamically favored above 350 °C, even in some hydrogen-rich environments. We discuss four basic mechanisms: a carbenium-ion based mechanism taking place on acid sites of zeolites or bifunctional catalysts, a metal-induced formation of soft coke (i.e., oligomers of small olefins) on bifunctional catalysts, a radical-mediated mechanism in higher-temperature processes, and fast-growing carbon filament formation. Catalysts deactivate because carbon deposits block pores at different length scales, or directly block active sites. Some deactivated catalysts can be re-used, others can be regenerated or have to be discarded. Catalyst and process design can mitigate the effects of deactivation. New analytical tools allow for the direct observation (in some cases even under in situ or operando conditions) of the 3D-distribution of coke-type species as a function of catalyst structure and lifetime.

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Carbon Deposit Analysis in Catalyst Deactivation, Regeneration, and Rejuvenation

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