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J Phys Chem Lett. 2018 Mar 15;9(6):1324-1328. doi: 10.1021/acs.jpclett.8b00094. Epub 2018 Mar 05.

Deactivation of Zeolite Catalyst H-ZSM-5 during Conversion of Methanol to Gasoline: Operando Time- and Space-Resolved X-ray Diffraction.

The journal of physical chemistry letters

Daniel Rojo-Gama, Lukasz Mentel, Georgios N Kalantzopoulos, Dimitrios K Pappas, Iurii Dovgaliuk, Unni Olsbye, Karl Petter Lillerud, Pablo Beato, Lars F Lundegaard, David S Wragg, Stian Svelle

Affiliations

  1. Center for Materials Science and Nanotechnology (SMN), Department of Chemistry , University of Oslo , P.O. Box 1033, Blindern , N-0315 Oslo , Norway.
  2. Haldor Topsøe A/S , Haldor Topsøes Allé 1 , 2800 Kgs. Lyngby , Denmark.
  3. Swiss-Norwegian Beamline, The European Synchrotron , European Synchrotron Radiation Facility , 6, Rue Jules Horowitz , 38000 Grenoble , France.

PMID: 29494162 DOI: 10.1021/acs.jpclett.8b00094

Abstract

The deactivation of zeolite catalyst H-ZSM-5 by coking during the conversion of methanol to hydrocarbons was monitored by high-energy space- and time-resolved operando X-ray diffraction (XRD) . Space resolution was achieved by continuous scanning along the axial length of a capillary fixed bed reactor with a time resolution of 10 s per scan. Using real structural parameters obtained from XRD, we can track the development of coke at different points in the reactor and link this to a kinetic model to correlate catalyst deactivation with structural changes occurring in the material. The "burning cigar" model of catalyst bed deactivation is directly observed in real time.

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