Issue 20, 2012

Tuning the catalytic performance of metal–organic frameworks in fine chemistry by active site engineering

Abstract

The effect of a post-synthetic acid treatment on the catalytic performance of MOFs is evaluated for MIL-100(Fe), an iron-benzenetricarboxylate. The acid-treated frameworks are structurally robust as no differences have been found in XRD patterns after treatment. Porosity of the acid-treated MOFs gradually decreases, most probably as a consequence of anions remaining in the charged frameworks. Monitoring the modification of the MOFs by reactions of which the outcome depends on the acid properties of the catalyst suggests the presence of two types of active sites, with weak Brönsted acid sites in close vicinity to the Lewis acid open metal sites. This is supported by CO-chemisorption experiments which indicate a large increase of both Lewis and Brönsted acidity. In Diels–Alder reactions of oxygenated dienophiles with 1,3-cyclohexadiene, a strong increase of the activity is found for the acid-treated MOFs. This is explained by the enhanced activation of the dienophiles on the modified active sites.

Graphical abstract: Tuning the catalytic performance of metal–organic frameworks in fine chemistry by active site engineering

Supplementary files

Article information

Article type
Paper
Submitted
20 Nov 2011
Accepted
13 Feb 2012
First published
28 Mar 2012

J. Mater. Chem., 2012,22, 10313-10321

Tuning the catalytic performance of metal–organic frameworks in fine chemistry by active site engineering

F. Vermoortele, R. Ameloot, L. Alaerts, R. Matthessen, B. Carlier, E. V. R. Fernandez, J. Gascon, F. Kapteijn and D. E. De Vos, J. Mater. Chem., 2012, 22, 10313 DOI: 10.1039/C2JM16030G

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