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

Rationalising the role of solid-acid sites in the design of versatile single-site heterogeneous catalysts for targeted acid-catalysed transformations
Rationalising the role of solid-acid sites in the design of versatile single-site heterogeneous catalysts for targeted acid-catalysed transformations
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 ?-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.
1478-6524
1810-1819
Gianotti, Enrica
2496d8d3-780f-4fe0-a43e-147e68331078
Manzoli, Maela
a17ae924-77c3-47b3-8c3b-d1b29cac758a
Potter, Matthew
34dee7dc-2f62-4022-bb65-fc7b7fb526d2
Shetti, Vasudev N.
a928ca6f-6cae-4fdc-aff4-43463be2c4db
Sun, Danni
b99cc371-82b3-4ac7-b83c-8cbc53434500
Paterson, James
bf6ad53e-007e-41c9-8ef0-551a7a0d53ce
Mezza, Thomas M.
a77c484c-a79f-4283-90c3-b049b63bdb1c
Levy, Alan
cefea37f-08a1-4c9d-8fff-11146908dba1
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Gianotti, Enrica
2496d8d3-780f-4fe0-a43e-147e68331078
Manzoli, Maela
a17ae924-77c3-47b3-8c3b-d1b29cac758a
Potter, Matthew
34dee7dc-2f62-4022-bb65-fc7b7fb526d2
Shetti, Vasudev N.
a928ca6f-6cae-4fdc-aff4-43463be2c4db
Sun, Danni
b99cc371-82b3-4ac7-b83c-8cbc53434500
Paterson, James
bf6ad53e-007e-41c9-8ef0-551a7a0d53ce
Mezza, Thomas M.
a77c484c-a79f-4283-90c3-b049b63bdb1c
Levy, Alan
cefea37f-08a1-4c9d-8fff-11146908dba1
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b

Gianotti, Enrica, Manzoli, Maela, Potter, Matthew, Shetti, Vasudev N., Sun, Danni, Paterson, James, Mezza, Thomas M., Levy, Alan and Raja, Robert (2014) Rationalising the role of solid-acid sites in the design of versatile single-site heterogeneous catalysts for targeted acid-catalysed transformations. Chemical Science, 5 (5), 1810-1819. (doi:10.1039/C3SC53088D).

Record type: Article

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 ?-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.

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e-pub ahead of print date: 31 January 2014
Published date: 1 May 2014
Organisations: Chemistry

Identifiers

Local EPrints ID: 367161
URI: http://eprints.soton.ac.uk/id/eprint/367161
ISSN: 1478-6524
PURE UUID: 99c22f25-741a-4acf-a024-ab0a21bf55cd
ORCID for Matthew Potter: ORCID iD orcid.org/0000-0001-9849-3306
ORCID for Robert Raja: ORCID iD orcid.org/0000-0002-4161-7053

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Date deposited: 23 Jul 2014 11:27
Last modified: 18 Feb 2021 17:16

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