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Expanding beyond the micropore: active-site engineering in hierarchical architectures for Beckmann rearrangement

Expanding beyond the micropore: active-site engineering in hierarchical architectures for Beckmann rearrangement
Expanding beyond the micropore: active-site engineering in hierarchical architectures for Beckmann rearrangement
The ability to engineer discrete solid-acid centers within hierarchically porous architectures that contain micropores with interconnected mesopores offers the potential to overcome the spatial restraints and diffusional limitations imposed by conventional microporous zeotype catalysts, which often lead to decreased catalyst lifetimes and restricted substrate scope. By employing a one-step soft-templating approach, coupled with detailed physicochemical and spectroscopic characterization, isolated, solid-acid sites can be suitably tailored and discretely modulated within the micropores and mesopores. The design strategy facilitates a synergistic enhancement in catalytic activity, selectivity, substrate versatility, and longevity, compared to analogous microporous zeotypes that have been extensively employed in the chemical industry, as solid-acid catalysts, for the production of ?-caprolactam (precursor for Nylon-6).
2155-5435
6587-6593
Newland, Stephanie H.
4f4fef13-95ea-4cc5-9b45-13733eb6c06a
Sinkler, Wharton
20c463cb-85e9-4751-a092-9f0155f72cf7
Mezza, Thomas
c81e4984-d885-4a18-a1b5-64c5d5ca275e
Bare, Simon R.
74aea019-9076-4148-ab37-21d3197dc393
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Haies, Ibraheem M.
d14dce0d-4693-429a-8047-7770f3765d02
Levy, Alan
cefea37f-08a1-4c9d-8fff-11146908dba1
Keenan, Scott
253a86ed-c1b7-485c-bc59-22f30dda0174
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Newland, Stephanie H.
4f4fef13-95ea-4cc5-9b45-13733eb6c06a
Sinkler, Wharton
20c463cb-85e9-4751-a092-9f0155f72cf7
Mezza, Thomas
c81e4984-d885-4a18-a1b5-64c5d5ca275e
Bare, Simon R.
74aea019-9076-4148-ab37-21d3197dc393
Carravetta, Marina
1b12fa96-4a6a-4689-ab3b-ccc68f1d7691
Haies, Ibraheem M.
d14dce0d-4693-429a-8047-7770f3765d02
Levy, Alan
cefea37f-08a1-4c9d-8fff-11146908dba1
Keenan, Scott
253a86ed-c1b7-485c-bc59-22f30dda0174
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b

Newland, Stephanie H., Sinkler, Wharton, Mezza, Thomas, Bare, Simon R., Carravetta, Marina, Haies, Ibraheem M., Levy, Alan, Keenan, Scott and Raja, Robert (2015) Expanding beyond the micropore: active-site engineering in hierarchical architectures for Beckmann rearrangement. ACS Catalysis, 5 (11), 6587-6593. (doi:10.1021/acscatal.5b01595).

Record type: Article

Abstract

The ability to engineer discrete solid-acid centers within hierarchically porous architectures that contain micropores with interconnected mesopores offers the potential to overcome the spatial restraints and diffusional limitations imposed by conventional microporous zeotype catalysts, which often lead to decreased catalyst lifetimes and restricted substrate scope. By employing a one-step soft-templating approach, coupled with detailed physicochemical and spectroscopic characterization, isolated, solid-acid sites can be suitably tailored and discretely modulated within the micropores and mesopores. The design strategy facilitates a synergistic enhancement in catalytic activity, selectivity, substrate versatility, and longevity, compared to analogous microporous zeotypes that have been extensively employed in the chemical industry, as solid-acid catalysts, for the production of ?-caprolactam (precursor for Nylon-6).

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e-pub ahead of print date: 29 September 2015
Published date: 6 November 2015

Identifiers

Local EPrints ID: 394650
URI: http://eprints.soton.ac.uk/id/eprint/394650
ISSN: 2155-5435
PURE UUID: 686b09c2-a669-4e57-b030-c85479aa895c
ORCID for Marina Carravetta: ORCID iD orcid.org/0000-0002-6296-2104
ORCID for Robert Raja: ORCID iD orcid.org/0000-0002-4161-7053

Catalogue record

Date deposited: 23 May 2016 09:11
Last modified: 15 Mar 2024 03:26

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Contributors

Author: Stephanie H. Newland
Author: Wharton Sinkler
Author: Thomas Mezza
Author: Simon R. Bare
Author: Ibraheem M. Haies
Author: Alan Levy
Author: Scott Keenan
Author: Robert Raja ORCID iD

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