Growth of Ammonium Bisulfate Clusters by Adsorption of Oxygenated Organic Molecules
Abstract
Quantum chemical calculations were employed to model the interactions of the [(NH4+)4(HSO4-)4] ammonium bisulfate cluster with one or more molecular products of monoterpene oxidation. A strong interaction was found between the bisulfate ion of the cluster and a carboxylic acid, aldehyde or ketone functionality of the organic molecule. Free energies of adsorption for carboxylic acids were in the -70 to -73 kJ/mol range, while those for aldehydes and ketones were in the -46 to -50 kJ/mol range. These values suggest that a small ambient ammonium bisulfate cluster, such as the [(NH4+)4(SO4-)4] cluster, is able to adsorb an oxygenated organic molecule. Although adsorption of the first molecule is highly favorable, adsorption of subsequent molecules is not, suggesting that sustained uptake of organic molecules does not occur, and thus is not a pathway for continuing growth of the cluster. This result is consistent with ambient measurements showing that particles below ~1 nm grow slowly, while those above 1 nm grow at an increasing rate presumably due to a lower surface energy barrier enabling the uptake of organic molecules. This work provides insight into the molecular level interactions which affect sustained cluster growth by uptake of organic molecules.
- Authors:
-
- Univ. of Delaware, Newark, DE (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Univ. of California, Davis, CA (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1239790
- Report Number(s):
- BNL-111698-2015-JA
Journal ID: ISSN 1089-5639; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000
- Grant/Contract Number:
- SC0012704; DE-AC02- 98CH10886
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
- Additional Journal Information:
- Journal Volume: 119; Journal Issue: 45; Journal ID: ISSN 1089-5639
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES
Citation Formats
DePalma, Joseph W., Wang, Jian, Wexler, Anthony S., and Johnston, Murray V. Growth of Ammonium Bisulfate Clusters by Adsorption of Oxygenated Organic Molecules. United States: N. p., 2015.
Web. doi:10.1021/acs.jpca.5b07744.
DePalma, Joseph W., Wang, Jian, Wexler, Anthony S., & Johnston, Murray V. Growth of Ammonium Bisulfate Clusters by Adsorption of Oxygenated Organic Molecules. United States. https://doi.org/10.1021/acs.jpca.5b07744
DePalma, Joseph W., Wang, Jian, Wexler, Anthony S., and Johnston, Murray V. Wed .
"Growth of Ammonium Bisulfate Clusters by Adsorption of Oxygenated Organic Molecules". United States. https://doi.org/10.1021/acs.jpca.5b07744. https://www.osti.gov/servlets/purl/1239790.
@article{osti_1239790,
title = {Growth of Ammonium Bisulfate Clusters by Adsorption of Oxygenated Organic Molecules},
author = {DePalma, Joseph W. and Wang, Jian and Wexler, Anthony S. and Johnston, Murray V.},
abstractNote = {Quantum chemical calculations were employed to model the interactions of the [(NH4+)4(HSO4-)4] ammonium bisulfate cluster with one or more molecular products of monoterpene oxidation. A strong interaction was found between the bisulfate ion of the cluster and a carboxylic acid, aldehyde or ketone functionality of the organic molecule. Free energies of adsorption for carboxylic acids were in the -70 to -73 kJ/mol range, while those for aldehydes and ketones were in the -46 to -50 kJ/mol range. These values suggest that a small ambient ammonium bisulfate cluster, such as the [(NH4+)4(SO4-)4] cluster, is able to adsorb an oxygenated organic molecule. Although adsorption of the first molecule is highly favorable, adsorption of subsequent molecules is not, suggesting that sustained uptake of organic molecules does not occur, and thus is not a pathway for continuing growth of the cluster. This result is consistent with ambient measurements showing that particles below ~1 nm grow slowly, while those above 1 nm grow at an increasing rate presumably due to a lower surface energy barrier enabling the uptake of organic molecules. This work provides insight into the molecular level interactions which affect sustained cluster growth by uptake of organic molecules.},
doi = {10.1021/acs.jpca.5b07744},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 45,
volume = 119,
place = {United States},
year = {Wed Oct 21 00:00:00 EDT 2015},
month = {Wed Oct 21 00:00:00 EDT 2015}
}
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Cited by: 12 works
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Figures / Tables:
Table 1: Thermodynamic potentials (in kJ/mol) for adsorption of various α-pinene oxidation products to the [(NH4+)4(HSO4-)4] cluster. Values are computed for the gas phase standard state of 1 atmosphere and 298 K.
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