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Title: Hydrolysis of N{sub 2}O{sub 5} on submicron sulfuric acid aerosols

Abstract

The kinetics of reactive uptake of gaseous N{sub 2}O{sub 5} on submicron sulfuric acid aerosol particles has been investigated using a laminar flow reactor coupled with a differential mobility analyzer (DMA) to characterize the aerosol. The particles were generated by homogeneous nucleation of SO{sub 3}/H{sub 2}O mixtures. In the H{sub 2}SO{sub 4} concentration range 26.3--64.5 wt {degree} the uptake coefficient was {gamma} = 0.033 {+-} 0.004, independent of acid strength. For an acid strength of 45 wt % {gamma} was found to decrease with increasing temperature over the range 263--298 K. From this, temperature dependence values of {minus}115 {+-} 30 kJ/mol and {minus}25.5 {+-} 8.4 J/K mol were determined for the changes in enthalpy and entropy of the uptake process, respectively. The results are consistent with a previous model of N{sub 2}O{sub 5} hydrolysis involving both a direct and an acid catalyzed mechanism, with uptake under the experimental conditions limited by mass accommodation.

Authors:
; ; ;
Publication Date:
Research Org.:
Univ. of Cambridge (GB)
OSTI Identifier:
20034418
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry A: Molecules, Spectroscopy, Kinetics, Environment, amp General Theory
Additional Journal Information:
Journal Volume: 104; Journal Issue: 17; Other Information: PBD: 4 May 2000; Journal ID: ISSN 1089-5639
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; NITROGEN OXIDES; HYDROLYSIS; AEROSOLS; SULFURIC ACID; DROPLETS; TEMPERATURE DEPENDENCE; CHEMICAL REACTION KINETICS; ATMOSPHERIC CHEMISTRY

Citation Formats

Hallquist, M., Stewart, D.J., Baker, J., and Cox, R.A. Hydrolysis of N{sub 2}O{sub 5} on submicron sulfuric acid aerosols. United States: N. p., 2000. Web. doi:10.1021/jp9939625.
Hallquist, M., Stewart, D.J., Baker, J., & Cox, R.A. Hydrolysis of N{sub 2}O{sub 5} on submicron sulfuric acid aerosols. United States. doi:10.1021/jp9939625.
Hallquist, M., Stewart, D.J., Baker, J., and Cox, R.A. Thu . "Hydrolysis of N{sub 2}O{sub 5} on submicron sulfuric acid aerosols". United States. doi:10.1021/jp9939625.
@article{osti_20034418,
title = {Hydrolysis of N{sub 2}O{sub 5} on submicron sulfuric acid aerosols},
author = {Hallquist, M. and Stewart, D.J. and Baker, J. and Cox, R.A.},
abstractNote = {The kinetics of reactive uptake of gaseous N{sub 2}O{sub 5} on submicron sulfuric acid aerosol particles has been investigated using a laminar flow reactor coupled with a differential mobility analyzer (DMA) to characterize the aerosol. The particles were generated by homogeneous nucleation of SO{sub 3}/H{sub 2}O mixtures. In the H{sub 2}SO{sub 4} concentration range 26.3--64.5 wt {degree} the uptake coefficient was {gamma} = 0.033 {+-} 0.004, independent of acid strength. For an acid strength of 45 wt % {gamma} was found to decrease with increasing temperature over the range 263--298 K. From this, temperature dependence values of {minus}115 {+-} 30 kJ/mol and {minus}25.5 {+-} 8.4 J/K mol were determined for the changes in enthalpy and entropy of the uptake process, respectively. The results are consistent with a previous model of N{sub 2}O{sub 5} hydrolysis involving both a direct and an acid catalyzed mechanism, with uptake under the experimental conditions limited by mass accommodation.},
doi = {10.1021/jp9939625},
journal = {Journal of Physical Chemistry A: Molecules, Spectroscopy, Kinetics, Environment, amp General Theory},
issn = {1089-5639},
number = 17,
volume = 104,
place = {United States},
year = {2000},
month = {5}
}