Abstract
| Original language | English |
|---|---|
| Pages (from-to) | 2926-2934 |
| Number of pages | 9 |
| Journal | ACS Catalysis |
| Volume | 7 |
| Issue number | 4 |
| Early online date | 13 Mar 2017 |
| DOIs | |
| Publication status | Published - 7 Apr 2017 |
Cite this
Understanding the Role of Molecular Diffusion and Catalytic Selectivity in Liquid-Phase Beckmann Rearrangement. / Potter, Matthew E.; O’malley, Alexander J.; Chapman, Stephanie; Kezina, Julija; Newland, Stephanie H.; Silverwood, Ian P.; Mukhopadhyay, Sanghamitra; Carravetta, Marina; Mezza, Thomas M.; Parker, Stewart F.; Catlow, C. Richard A.; Raja, Robert.
In: ACS Catalysis, Vol. 7, No. 4, 07.04.2017, p. 2926-2934.Research output: Contribution to journal › Article
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TY - JOUR
T1 - Understanding the Role of Molecular Diffusion and Catalytic Selectivity in Liquid-Phase Beckmann Rearrangement
AU - Potter, Matthew E.
AU - O’malley, Alexander J.
AU - Chapman, Stephanie
AU - Kezina, Julija
AU - Newland, Stephanie H.
AU - Silverwood, Ian P.
AU - Mukhopadhyay, Sanghamitra
AU - Carravetta, Marina
AU - Mezza, Thomas M.
AU - Parker, Stewart F.
AU - Catlow, C. Richard A.
AU - Raja, Robert
PY - 2017/4/7
Y1 - 2017/4/7
N2 - 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.
AB - 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.
U2 - 10.1021/acscatal.6b03641
DO - 10.1021/acscatal.6b03641
M3 - Article
VL - 7
SP - 2926
EP - 2934
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
IS - 4
ER -