Cristian Blanco and Scott M. Auerbach,
``Simulating Non-Equilibrium Dynamics in Nanopores:
Microwave-Heated Diffusion of Methanol and Benzene
in DAY Zeolite,''
J. Comput. Theor. Nanosci. 1, 183-189 (2004).
Abstract
We have performed equilibrium molecular dynamics and microwave (MW) heated
molecular dynamics simulations to explore how MW heating influences
self-diffusion in zeolite nanopores. We have applied these simulations to
methanol and/or benzene in de-aluminated Y zeolite.
We find that even under the non-equilibrium conditions of MW heating,
center-of-mass motions can be associated with effective temperatures.
However, we find that the temperatures controlling kinetic and potential
energy distributions are not generally the same in MW-heated systems,
with potential temperatures generally exceeding kinetic ones.
This finding has a consequence for understanding MW-heated diffusion in
zeolites. In particular, when temperatures are sufficiently
high that diffusion is not strongly activated, MW-heated diffusivities
are equal to equilibrium diffusivities at the same kinetic temperature.
On the other hand, when diffusion becomes more strongly activated at lower
temperatures, MW-heated diffusivities consistently exceed equilibrium
diffusivities at
the same kinetic temperature, because the MW-heated potential
distributions enable more facile barrier crossing. This result shows
that in general, MW-heated diffusion is more complicated than simply
``different components diffusing at different temperatures.'' Instead,
we advocate the picture involving
different components diffusing at different kinetic and potential
temperatures.
Prof SM Auerbach
19 March 2004