Local structure of the zeolitic catalytically active site during reaction.
The structural changes of the catalytic active site that occur during catalytic reaction in an acidic zeolite are detected. The local structure of the zeolitic Brønsted active site is a distorted tetrahedrally coordinated aluminum that has three short and one long aluminum-oxygen bond. Using in situ Al K edge X-ray absorption spectroscopy, the adsorption of a reactive intermediate in the oligomerization of ethene changed the local structure of the catalytic active site; the long aluminum oxygen bond is partially relaxed. At increasingly higher temperature, extensive coking of the catalyst frees the Brønsted acid site from the reactive intermediate, restoring the asymmetric coordination. These measurements show that application of in situ Al K edge spectroscopy provides fundamental insight into the structure of zeolitic catalytically active sites during catalytic action.
van Bokhoven
Jeroen A
JA
Swiss Federal Institute of Technology (ETH) Zurich, CH-8093, Zurich, Switzerland. j.a.vanbokhoven@tech.chem.ethz.ch
van der Eerden
Ad M J
AM
Prins
Roel
R