Growth of Ammonium Bisulfate Clusters by Adsorption of Oxygenated Organic Molecules

DePalma, Joseph W.; Wang, Jian; Wexler, Anthony S.; Johnston, Murray V.

doi:10.1021/acs.jpca.5b07744

Title: Growth of Ammonium Bisulfate Clusters by Adsorption of Oxygenated Organic Molecules

Journal Article · 20 October 2015 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI: https://doi.org/10.1021/acs.jpca.5b07744 · OSTI ID:1239790

DePalma, Joseph W. ^[1]; Wang, Jian ^[2]; Wexler, Anthony S. ^[3]; Johnston, Murray V. ^[1]

Univ. of Delaware, Newark, DE (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Univ. of California, Davis, CA (United States)

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-98CH10886; SC0012704

OSTI ID:: 1239790

Report Number(s):: BNL-111698-2015-JA; KP1701000

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 45 Vol. 119; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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