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Molecular sieve catalysts for the regioselective and shape-selective oxyfunctionalization of alkanes in air

Molecular sieve catalysts for the regioselective and shape-selective oxyfunctionalization of alkanes in air
Molecular sieve catalysts for the regioselective and shape-selective oxyfunctionalization of alkanes in air
Framework-substituted, molecular-sieve, aluminophosphate, microporous solids are the centerpieces of a new approach to the aerobic oxyfunctionalization of saturated hydrocarbons. The sieves, and the few percent of the AlIII sites within them that are replaced by catalytically active, transition-metal ions in high oxidation states (CoIII, MnIII, FeIII), are designed so as to allow free access of oxygen in to and out of the interior of these high-area solids. Certain metal-substituted, molecular sieves permit only end-on approach of linear alkanes to the active centers, thereby favoring enhanced reactivity of the terminal methyl groups. By optimizing cage dimension, with respect to that of the hydrocarbon reactant, as well as adjusting the average separation of active centers within a cage, and by choosing the sieve with the appropriate pore aperture, highly selective conversions such as n-hexane to hexanoic acid or adipic acid, and cyclohexane to cyclohexanol, cyclohexanone, or adipic acid, may be effected at low temperature, heterogeneously in air.
hydrogen-peroxide, cyclohexane, acid catalysts, oxidation, radical chemistry, saturated-hydrocarbons, oxygen, linear alkanes, x-ray-absorption, gif chemistry
0001-4842
191-200
Thomas, John Meurig
f1d9bb61-4e2c-4c4b-8115-953d0f3d36bd
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Sankar, Gopinathan
31dc72ca-310b-407f-9d6c-856dbfb2e2d1
Bell, Robert G.
47951797-cf55-4b61-bc7a-25a1da365711
Thomas, John Meurig
f1d9bb61-4e2c-4c4b-8115-953d0f3d36bd
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Sankar, Gopinathan
31dc72ca-310b-407f-9d6c-856dbfb2e2d1
Bell, Robert G.
47951797-cf55-4b61-bc7a-25a1da365711

Thomas, John Meurig, Raja, Robert, Sankar, Gopinathan and Bell, Robert G. (2001) Molecular sieve catalysts for the regioselective and shape-selective oxyfunctionalization of alkanes in air. Accounts of Chemical Research, 34 (3), 191-200. (doi:10.1021/ar970020e).

Record type: Article

Abstract

Framework-substituted, molecular-sieve, aluminophosphate, microporous solids are the centerpieces of a new approach to the aerobic oxyfunctionalization of saturated hydrocarbons. The sieves, and the few percent of the AlIII sites within them that are replaced by catalytically active, transition-metal ions in high oxidation states (CoIII, MnIII, FeIII), are designed so as to allow free access of oxygen in to and out of the interior of these high-area solids. Certain metal-substituted, molecular sieves permit only end-on approach of linear alkanes to the active centers, thereby favoring enhanced reactivity of the terminal methyl groups. By optimizing cage dimension, with respect to that of the hydrocarbon reactant, as well as adjusting the average separation of active centers within a cage, and by choosing the sieve with the appropriate pore aperture, highly selective conversions such as n-hexane to hexanoic acid or adipic acid, and cyclohexane to cyclohexanol, cyclohexanone, or adipic acid, may be effected at low temperature, heterogeneously in air.

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More information

Published date: March 2001
Keywords: hydrogen-peroxide, cyclohexane, acid catalysts, oxidation, radical chemistry, saturated-hydrocarbons, oxygen, linear alkanes, x-ray-absorption, gif chemistry

Identifiers

Local EPrints ID: 54154
URI: http://eprints.soton.ac.uk/id/eprint/54154
ISSN: 0001-4842
PURE UUID: c4d4f8c5-6373-437d-9377-a57deec7d14b
ORCID for Robert Raja: ORCID iD orcid.org/0000-0002-4161-7053

Catalogue record

Date deposited: 29 Jul 2008
Last modified: 17 Dec 2019 01:45

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Contributors

Author: John Meurig Thomas
Author: Robert Raja ORCID iD
Author: Gopinathan Sankar
Author: Robert G. Bell

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