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ClNO2 Production from N2O5 Uptake on Saline Playa Dusts: New Insights into Potential Inland Sources of ClNO2

Cite this: Environ. Sci. Technol. 2019, 53, 13, 7442–7452
Publication Date (Web):May 22, 2019
https://doi.org/10.1021/acs.est.9b01112
Copyright © 2019 American Chemical Society
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    Abstract

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    Nitryl chloride (ClNO2), formed when dinitrogen pentoxide (N2O5) reacts with chloride-containing aerosol, photolyzes to produce chlorine radicals that facilitate the formation of tropospheric ozone. ClNO2 has been measured in continental areas; however, the sources of particulate chloride required to form ClNO2 in inland regions remain unclear. Dust emitted from saline playas (e.g., dried lakebeds) contains salts that can potentially form ClNO2 in inland regions. Here, we present the first laboratory measurements demonstrating the production of ClNO2 from playa dusts. N2O5 reactive uptake coefficients (γN2O5) ranged from ∼10–3 to 10–1 and ClNO2 yields (φClNO2) were >50% for all playas tested except one. In general, as the soluble ion fraction of playa dusts increases, γN2O5 decreases and φClNO2 increases. We attribute this finding to a transition from aerosol surfaces dominated by silicates that react efficiently with N2O5 and produce little ClNO2 to aerosols that behave like deliquesced chloride-containing salts that generate high yields of ClNO2. Molecular bromine (Br2) and nitryl bromide (BrNO2) were also detected, highlighting that playas facilitate the heterogeneous production of brominated compounds. Our results suggest that parameterizations and models should be updated to include playas as an inland source of aerosol chloride capable of efficiently generating ClNO2.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.9b01112.

    • Description of the playa samples, dust generation setup, gas-phase compound detection, and soluble ion detection; five figures (playa photos, playa locations, laboratory setup, representative aerosol size distributions, and example of linearity between S and khet) and four tables (sample coordinates, corrections to S measurements, γN2O5 and φ values for all samples, and IC data) are also included (PDF)

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