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Chemical and Physical Transformations of Aluminosilicate Clay Minerals Due to Acid Treatment and Consequences for Heterogeneous Ice Nucleation

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† Department of Chemistry, The Pennsylvania State University, 104 Chemistry Building, University Park, Pennsylvania 16802, United States
‡ CIRES and Department of Chemistry and Biochemistry, University of Colorado at Boulder, Boulder, Colorado 80309, United States
*(M.A.F.) E-mail: [email protected]
Cite this: J. Phys. Chem. A 2014, 118, 38, 8787–8796
Publication Date (Web):August 29, 2014
https://doi.org/10.1021/jp504846g
Copyright © 2014 American Chemical Society
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    Abstract

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    Mineral dust aerosol is one of the largest contributors to global ice nuclei, but physical and chemical processing of dust during atmospheric transport can alter its ice nucleation activity. In particular, several recent studies have noted that sulfuric and nitric acids inhibit heterogeneous ice nucleation in the regime below liquid water saturation in aluminosilicate clay minerals. We have exposed kaolinite, KGa-1b and KGa-2, and montmorillonite, STx-1b and SWy-2, to aqueous sulfuric and nitric acid to determine the physical and chemical changes that are responsible for the observed deactivation. To characterize the changes to the samples upon acid treatment, we use X-ray diffraction, transmission electron microscopy, and inductively coupled plasma–atomic emission spectroscopy. We find that the reaction of kaolinite and montmorillonite with aqueous sulfuric acid results in the formation of hydrated aluminum sulfate. In addition, sulfuric and nitric acids induce large structural changes in montmorillonite. We additionally report the supersaturation with respect to ice required for the onset of ice nucleation for these acid-treated species. On the basis of lattice spacing arguments, we explain how the chemical and physical changes observed upon acid treatment could lead to the observed reduction in ice nucleation activity.

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    Data for the high-defect kaolinite sample, KGa-2, the Na-rich montmorillonite sample, SWy-2, and control experiments for both montmorillonite samples (STx-1b and SWy-2) as described in the text. This material is available free of charge via the Internet at http://pubs.acs.org

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