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Tracing Catalytic Conversion on Single Zeolite Crystals in 3D with Nonlinear Spectromicroscopy

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† FOM Institute AMOLF, Science Park 104, NL-1098 XG Amsterdam, The Netherlands
‡ Inorganic Chemistry and Catalysis Group, Utrecht University, Universiteitsweg 99, NL-3584 CG Utrecht, The Netherlands
Department of Chemical and Biological Engineering, Chalmers University of Technology, SE-41296 Göteborg, Sweden
§ Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
[email protected]
Cite this: J. Am. Chem. Soc. 2012, 134, 2, 1124–1129
Publication Date (Web):November 28, 2011
https://doi.org/10.1021/ja2088025
Copyright © 2011 American Chemical Society
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    Abstract

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    The cost- and material-efficient development of next-generation catalysts would benefit greatly from a molecular-level understanding of the interaction between reagents and catalysts in chemical conversion processes. Here, we trace the conversion of alkene and glycol in single zeolite catalyst particles with unprecedented chemical and spatial resolution. Combined nonlinear Raman and two-photon fluorescence spectromicroscopies reveal that alkene activation constitutes the first reaction step toward glycol etherification and allow us to determine the activation enthalpy of the resulting carbocation formation. Considerable inhomogeneities in local reactivity are observed for micrometer-sized catalyst particles. Product ether yields observed on the catalyst are ca. 5 times higher than those determined off-line. Our findings are relevant for other heterogeneous catalytic processes and demonstrate the immense potential of novel nonlinear spectromicroscopies for catalysis research.

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    Synthesis of H-beta crystals; table of Raman bands and assignment; derivation of the apparent adsorption enthalpy of 1-octene on H-beta, ΔHapp0; reconstructed 3D videos of the fluorescent side product distribution; CARS and UV/vis results of 2 μm large H-beta crystals. This material is free of charge via the Internet at http://pubs.acs.org.

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