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Is the uptake of alcohols by H2O droplets governed by equilibrium solvation dynamics?

Conference ·
OSTI ID:560452
;  [1]
  1. Pacific Northwest National Lab., Richland, WA (United States)

Heterogeneous processes are important components of the earth`s atmospheric system. Experiments suggest that the interaction of small gas phase molecules with the liquid/vapor interface of aqueous droplets and their subsequent accommodation into the bulk of droplet is an integral part of these processes. A recently devised, molecular-level model predicts that this mass accommodation process is solely dependent on the rates of solvation and desorption of the impinging molecule and that the molecule must cross a large energy barrier before becoming solvated in the bulk water. In this work, we are using molecular dynamics computer simulations to examine this model. Due to the availability of experimental data, the ethanol-water and ethylene glycol-water systems have been chosen as prototypes for the mass accommodation process of non-reacting molecules. The potential of mean force technique is used to explore the equilibrium free energy surface for inserting these alcohols into bulk water from its vapor. These free energy profiles do not correspond to those predicted by the above mentioned model. The non-equilibrium aspects of this process are also explored.

DOE Contract Number:
AC06-76RL01830
OSTI ID:
560452
Report Number(s):
CONF-970443--
Country of Publication:
United States
Language:
English

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