In-situ imaging of reacting single-particle zeolites by non-linear optical microscopy

Paul J. Wrzesinski, Mikhail N. Slipchenko, Taslima A. Zaman, Robert Martin Rioux, Jr., James R. Gord, Sukesh Roy

Research output: Chapter in Book/Report/Conference proceedingConference contribution

Abstract

Zeolite catalysis has been exploited by the petrochemical industry since the 1940's for catalytic cracking reactions of long chain hydrocarbons. The selectivity of zeolites strongly depends on a pore size, which is controlled by the chosen structure-directing agent (SDA) and by the SDA decomposition/removal process. Although zeolites are composed of micron-sized crystals, studies of zeolite materials typically focus on bulk (i.e., ensemble) measurements to elucidate structure-function information or to optimize catalysts and/or process parameters. To examine these phenomena on the microscale, non-linear optical microscopy is used to provide real-time imaging of chemical reactions in zeolites at temperatures exceeding 400°C. The template decomposition mechanism is studied, as elucidation of the mechanism is critical to understanding the relationship between the decomposition chemistry and the nanoscale features of the zeolite (topology, Si/Al ratio, added dopants). Forward stimulated Raman scattering (SRS), forward coherent anti-Stokes Raman scattering (CARS) and epi two-photon fluorescence (TPF) modalities are acquired simultaneously providing video-rate structural and chemical information. A high-temperature cell with gas inlet system is used for the study of reactions under various temperatures and gas environments. Examining the decomposition process with single-particle resolution enables access to ensemble-level and spatially-resolved behavior. Parallel experiments on bulk zeolite powders are conducted to enable comparison of ensemble and single-particle behavior during template decomposition. Our multi-technique approach has high potential for gaining insight into the link between nanoscale structure and catalytic activity and selectivity of zeolitic materials.

Original languageEnglish (US)
Title of host publicationFrontiers in Ultrafast Optics
Subtitle of host publicationBiomedical, Scientific, and Industrial Applications XV
EditorsMichel Meunier, Peter R. Herman, Stefan Nolte, Alexander Heisterkamp
PublisherSPIE
ISBN (Electronic)9781628414455
DOIs
StatePublished - Jan 1 2015
EventFrontiers in Ultrafast Optics: Biomedical, Scientific, and Industrial Applications XV - San Francisco, United States
Duration: Feb 8 2015Feb 10 2015

Publication series

NameProceedings of SPIE - The International Society for Optical Engineering
Volume9355
ISSN (Print)0277-786X
ISSN (Electronic)1996-756X

Other

OtherFrontiers in Ultrafast Optics: Biomedical, Scientific, and Industrial Applications XV
CountryUnited States
CitySan Francisco
Period2/8/152/10/15

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics
  • Computer Science Applications
  • Applied Mathematics
  • Electrical and Electronic Engineering

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