The Coking of a Solid Catalyst Rationalized with Combined Raman and Fluorescence Lifetime Microscopy

Author:

Vogel Robin1,Versluis Caroline1,Frijsen Rowie1,Prins P. Tim1,Vogt Eelco T. C.1,Rabouw Freddy T.12,Weckhuysen Bert M.1ORCID

Affiliation:

1. Inorganic Chemistry and Catalysis Group Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials Science Utrecht University Universiteitsweg 99 3584 CG Utrecht The Netherlands

2. Soft Condensed Matter Group Debye Institute for Nanomaterials Science Utrecht university Princetonplein 1 3584 CC Utrecht The Netherlands

Abstract

AbstractThe formation of carbon deposits is a major deactivation pathway for solid catalysts. Studying coking on industrially relevant catalysts is, however, often challenging due to the sample heterogeneity. That is especially true for zeolite‐containing catalysts where fluorescence often hampers their characterization with Raman spectroscopy. We turned this disadvantage into an advantage and combined Raman and fluorescence (lifetime) microscopy to study the coking behavior of an equilibrium catalyst material used for fluid catalytic cracking of hydrocarbons. The results presented illustrate that this approach can yield new insights in the physicochemical processes occurring within zeolite‐containing catalyst particles during their coking process. Ex situ analyses of single catalyst particles revealed considerable intra‐sample heterogeneities. The sample‐averaged Raman spectra showed a higher degree of graphitization when the sample was exposed to more hexane, while the sample‐averaged fluorescence lifetime showed no significant trend. Simultaneous in situ Raman and fluorescence (lifetime) microscopy, used to follow the coking and the regeneration of single particles, gave more insights in the changing fluorescence dynamics. During the coking, the rise and decline of the average fluorescence lifetime suggested the prolonged presence of smaller coke species that are quenched more and more by adjacent larger polyaromatics acting as Förster‐resonance‐energy‐transfer acceptors.

Funder

Nederlandse Organisatie voor Wetenschappelijk Onderzoek

Publisher

Wiley

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