Once Upon a Lifetime: Dynamics of Raman Scattering and Luminescence of Solid Catalysts at Work

Research output: ThesisDoctoral thesis 1 (Research UU / Graduation UU)

Abstract

Industrial catalysis plays a key role in our society. Catalysis involves the use of a catalyst materials that facilitate and accelerate chemical reactions. We study the working and deactivation mechanisms of catalysts used for the conversion of hydrocarbons in fuels and chemicals. These types of catalysts suffer from the formation of carbon deposits on their surfaces. This process frustrates the continuous conversion of feedstock into valuable chemicals. We set out to study the formation of carbon deposits with multiple spectroscopy experiments on catalysts in chemical reactors. During these experiments, we shine laser light on the catalyst in action on which the carbon deposits form. The laser light undergoes several types of light-matter interactions with the catalyst and the carbon deposits, after which it reappears in a modulated form. Spectral measurements of this modulated light yield valuable, albeit overlapping spectral information. Besides the spectral properties, the modulated light also has dynamic properties depending on the type of light-matter interaction from which it originated. We explore and exploit these dynamic differences with time-resolved spectroscopy in this PhD Thesis. We recorded Raman spectra with fainter background signals, by filtering out slower background fluorescence. By doing so, we gained insights in the formation of carbon deposits. Likewise, we recorded spectra to determine the temperature of catalyst materials at work. Filtering out background signals, based on their dynamic differences made our measurements more precise.
Original languageEnglish
QualificationDoctor of Philosophy
Awarding Institution
  • Utrecht University
Supervisors/Advisors
  • Weckhuysen, Bert, Supervisor
  • Rabouw, Freddy, Co-supervisor
Award date18 Jun 2025
Place of PublicationUtrecht
Publisher
Print ISBNs978-94-6522-214-1
DOIs
Publication statusPublished - 18 Jun 2025

Keywords

  • Catalysis
  • spectroscopy
  • luminescence thermometry
  • time-gated Raman spectroscopy
  • fluorescence lifetime microscopy
  • propane dehydrogenation
  • fluid catalytic cracking
  • carbon deposits

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