Methanol diffusion in zeolite HY: a combined quasielastic neutron scattering and molecular dynamics simulation study

Literature Information

Publication Date 2016-05-16
DOI 10.1039/C6CP01151A
Impact Factor 3.676
Authors

Victoria García Sakai, Ian P. Silverwood, Nikolaos Dimitratos


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Abstract

The diffusion of methanol in zeolite HY is studied using tandem quasielastic neutron scattering (QENS) experiments and molecular dynamics (MD) simulations at 300–400 K. The experimental diffusion coefficients were measured in the range 2–5 × 10−10 m2 s−1 and simulated diffusion coefficients calculated in the range of 1.6–3.2 × 10−9 m2 s−1. Activation energies were measured as 8.8 and 6.9 kJ mol−1 using QENS and MD respectively. Differences may be attributed predominantly to the experimental use of a dealuminated HY sample, containing significant defects such as strongly adsorbing silanol nests, compared to a perfect simulated crystal containing only evenly distributed Brønsted acid sites. Experimental and simulated diffusivities measured in this study are lower than those obtained from those previously calculated in siliceous faujasite, due to methanol H-bonding to Brønsted acid sites as observed in the MD simulations. However, both experimental and simulated diffusivities were significantly higher than those obtained in NaX, due to the higher concentration of extraframework cations present in the previously studied structures.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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