Kinetics of Adsorption ofn-butane on an Aggregate of Silicalite by Transient Non-equilibrium Molecular Dynamics

Numerical evidence for a thermal driving force during adsorption of butane in silicalite

“…Here we show, using non-equilibrium molecular dynamics simulations of n-butane in silicalite [6] that a significant temperature change accompanies adsorption and intra-crystalline transport, and leads to a significant varying thermal driving force across the crystal surface, in agreement with the proposition of Ruthven et al [7].…”

“…Butane was adsorbed and the temperature of the silicalite was recorded. A simple velocity rescaling thermostat was always on in the gas phase at the boundaries of the simulation box [6]. This situation mimics a real uptake-experiment.…”

“…Butane was described using the united atom model, where the methyl and the methylene groups are considered as one centre of force. Details on the model and the potential can be found in reference [6]. The non-equilibrium state of the system was simulated using a transient non-equilibrium molecular dynamics simulation technique [6].…”

“…Details on the model and the potential can be found in reference [6]. The non-equilibrium state of the system was simulated using a transient non-equilibrium molecular dynamics simulation technique [6]. Periodic boundary conditions were used.…”

Understanding Transport in MFI‐Type Zeolites on a Molecular Basis

“…The steps of sticking and trapping of the sorbate on the zeolite surface and of entering into the pore network are probably most controversially discussed. Simon et al reported estimated sticking probabilities of approximately one [74,75] for n-butane on silicalite-1 and Kärger et al [76] of around 10 −4 for benzene in silicalite-1 using PFG-NMR [76,77]. In contrast, our results on the basis of time-resolved infrared spectroscopy with ZSM5 [78] showed values of around 10 −7 for benzene, toluene, and xylene.…”