Issue 5, 2014

Rationalising the role of solid-acid sites in the design of versatile single-site heterogeneous catalysts for targeted acid-catalysed transformations

Abstract

A versatile design strategy for rationalising the role of well-defined and isolated multifunctional solid-acid active centres, employing Mg(II)Si(IV)AlPO-5 nanoporous architectures has been demonstrated, with a view to affording structure–property correlations compared to its corresponding mono-substituted analogues (Mg(II)AlPO-5 and Si(IV)AlPO-5). The simultaneous incorporation of Mg(II) and Si(IV) ions, as isomorphous replacements for Al(III) and P(V) ions in the microporous architecture, plays an important role in modulating the nature and strength of the solid-acid active sites in the industrially-important, vapour-phase Beckmann rearrangement of cyclohexanone oxime to produce ε-caprolactam (the precursor for renewable nylon-6) and in the isopropylation of benzene to cumene. The structural integrity, coordination geometry and local environment of the active (Brønsted-acid) sites could be rationalised at the molecular level, using in situ spectroscopic techniques, for tailoring the catalytic synergy by adroit design of the framework architecture.

Graphical abstract: Rationalising the role of solid-acid sites in the design of versatile single-site heterogeneous catalysts for targeted acid-catalysed transformations

Supplementary files

Article information

Article type
Edge Article
Submitted
07 Nov 2013
Accepted
29 Jan 2014
First published
31 Jan 2014
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2014,5, 1810-1819

Author version available

Rationalising the role of solid-acid sites in the design of versatile single-site heterogeneous catalysts for targeted acid-catalysed transformations

E. Gianotti, M. Manzoli, M. E. Potter, V. N. Shetti, D. Sun, J. Paterson, T. M. Mezza, A. Levy and R. Raja, Chem. Sci., 2014, 5, 1810 DOI: 10.1039/C3SC53088D

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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