Potter, ME;
O'Malley, AJ;
Chapman, S;
Kezina, J;
Newland, SH;
Silverwood, IP;
Mukhopadhyay, S;
... Raja, R; + view all
(2019)
Understanding the Role of Molecular Diffusion and Catalytic Selectivity in Liquid-Phase Beckmann Rearrangement.
ACS Catalysis
, 7
(4)
pp. 2926-2934.
10.1021/acscatal.6b03641.
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Abstract
Understanding the role of diffusion in catalysis is essential in the design of highly active, selective, and stable industrial heterogeneous catalysts. By using a combination of advanced in situ spectroscopic characterization tools, particularly quasi-elastic and inelastic neutron scattering, we outline the crucial differences in diffusion modes and molecular interactions of active sites within solid-acid catalysts. This, coupled with 2D solid-state NMR and probe-based FTIR spectroscopy, reveals the nature of the active site in our SAPO-37 catalyst and affords detailed information on the evolution of solid-acid catalysts that can operate at temperatures as low as 130 °C, for the Beckmann rearrangement of cyclohexanone oxime to ε-caprolactam (precursor for Nylon-6). The versatility of this approach leads to structure−property correlations that contrast the dynamics of the diffusion process in the different materials studied. Our results illustrate the power of these techniques in unravelling the interplay between active site and molecular diffusion in single-site heterogeneous catalysts, which can play a vital role in designing low-temperature, sustainable catalytic processes.
| Type: | Article |
|---|---|
| Title: | Understanding the Role of Molecular Diffusion and Catalytic Selectivity in Liquid-Phase Beckmann Rearrangement |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acscatal.6b03641 |
| Publisher version: | https://doi.org/10.1021/acscatal.6b03641 |
| Language: | English |
| Additional information: | Copyright © 2017 American Chemical Society. This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes. |
| Keywords: | Beckmann rearrangement; catalytic diffusion; heterogeneous catalysts; neutron scattering; nylon-6; operando spectroscopy |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10065159 |
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