Tracing Catalytic Conversion on Single Zeolite Crystals in 3D with Nonlinear Spectromicroscopy
Artikel i vetenskaplig tidskrift, 2012

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.

microscopy

stokes-raman scattering

beta zeolites

solids

acid catalysts

Författare

K. F. Domke

FOM Institute for Atomic and Molecular Physics - AMOLF

T. A. Riemer

FOM Institute for Atomic and Molecular Physics - AMOLF

G. Rago

FOM Institute for Atomic and Molecular Physics - AMOLF

A. N. Parvulescu

Universiteit Utrecht

P. C. A. Bruijnincx

Universiteit Utrecht

Annika Enejder

Chalmers, Kemi- och bioteknik, Molekylär mikroskopi

B. M. Weckhuysen

Universiteit Utrecht

M. Bonn

FOM Institute for Atomic and Molecular Physics - AMOLF

Max Planck-institutet

Journal of the American Chemical Society

0002-7863 (ISSN) 1520-5126 (eISSN)

Vol. 134 1124-1129

Ämneskategorier

Kemi

DOI

10.1021/ja2088025