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Molecular behaviour of phenol in zeolite Beta catalysts as a function of acid site presence: a quasielastic neutron scattering and molecular dynamics simulation study

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Abstract

Quasielastic neutron scattering (QENS) experiments complemented by classical molecular dynamics (MD) simulations at 393–443 K were employed in a study of the mobility and interactions of phenol in acidic zeolite H-Beta, to understand systems relevant to potential routes for the depolymerization and hydrodeoxygenation of lignin. QENS experiments observed isotropic phenol rotation with a fraction of static molecules, yielding rotational diffusion coefficients between 2.60 × 1010 and 3.33 × 1010 s−1 and an activation energy of rotation of 7.2 kJ mol−1. The MD simulations of phenol in the acidic and all-silica zeolite corroborate the experimental results, where molecules strongly adsorbed to the acidic sites behave as an immobile fraction with minimal contribution to the rotational diffusion, and the mobile molecules yield similar rotational diffusion coefficients to experiment. Translational diffusion is too slow to be detected in the instrumental time window of the QENS experiments, which is supported by MD-calculated activation energies of translation larger than 25 kJ mol−1. The study illustrates the effect of active sites in potential catalyst structures on the dynamical behaviour of molecules relevant to biomass conversion.

Graphical abstract: Molecular behaviour of phenol in zeolite Beta catalysts as a function of acid site presence: a quasielastic neutron scattering and molecular dynamics simulation study

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Publication details

The article was received on 02 Aug 2019, accepted on 19 Sep 2019 and first published on 04 Nov 2019


Article type: Paper
DOI: 10.1039/C9CY01548E
Catal. Sci. Technol., 2019, Advance Article
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    Molecular behaviour of phenol in zeolite Beta catalysts as a function of acid site presence: a quasielastic neutron scattering and molecular dynamics simulation study

    C. Hernandez-Tamargo, A. O'Malley, I. P. Silverwood and N. H. de Leeuw, Catal. Sci. Technol., 2019, Advance Article , DOI: 10.1039/C9CY01548E

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