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Laboratory Studies of the Thermal an...

Richards, Nicole K.

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Laboratory Studies of the Thermal and Photochemical Oxidation of Sea Salt Aerosols.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Laboratory Studies of the Thermal and Photochemical Oxidation of Sea Salt Aerosols./
Author:	Richards, Nicole K.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2011,
Description:	178 p.
Notes:	Source: Dissertations Abstracts International, Volume: 73-06, Section: B.
Contained By:	Dissertations Abstracts International73-06B.
Subject:	Physical chemistry. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3487066
ISBN:	9781267058171

Laboratory Studies of the Thermal and Photochemical Oxidation of Sea Salt Aerosols.
Richards, Nicole K.

Laboratory Studies of the Thermal and Photochemical Oxidation of Sea Salt Aerosols. - Ann Arbor : ProQuest Dissertations & Theses, 2011 - 178 p.

Source: Dissertations Abstracts International, Volume: 73-06, Section: B.

Thesis (Ph.D.)--University of California, Irvine, 2011.

This item is not available from ProQuest Dissertations & Theses.

Sea salt aerosols play an important role in the formation of inorganic halogen species in the troposphere and can play significant role during ozone depletion events at high and mid latitudes. The mechanisms of halogen production from sea salt oxidation are not well understood. In this dissertation the interactions of halide ions with other components present in sea salt (i.e., nitrate ions and organics) are explored and be shown to be vital in our understanding of halogen formation mechanisms. Through halide-nitrate ion photolysis experiments and computational models of aqueous mixed halide-nitrate systems, it was determined that NO2 and OH can more efficiently be produced, due to nitrate ions being drawn near the interface and experiencing a reduction in the solvent cage relative to neat NaNO3. It was determined that cations, can affect the distribution of NO3− in computational models and affect rates of NO2 from irradiated thin films of nitrate in the presence and absence of halide ions. It was shown that interfacial mechanisms of the photolysis of nitrate-halide mixtures also increased halogen production. Gas phase halogen yields increased with addition of Br− ions to synthetic sea salt. Results suggest that a new interhalogen reaction mechanism, HOCl− + Br−, may be contributing to the increase in Br 2 production at lower [Cl−]/[Br−] ratios. Yields of gas phase halogens were also strongly dependent on the acidity of the solution, while that of NO2 was not. High concentrations of NO were observed at low pH, suggesting an additional halogen formation mechanism involving H2ONO+ and Br− contributes. The observed Br2 and BrCl production initiated by the photolysis of NO3− may be contributing to tropospheric ozone destruction during the polar sunrise and at mid-latitudes. Studies were also conducted in collaboration with the Saltzman group on the photochemical production of Cl2 from NaCl/organic photosensitizer mixtures using antraquinone sulfonic acid (AQS) and natural organic matter (NOM) as the photosensitizer. These studies showed that 120 ppb of Cl2 was produced from 254 nm irradiation of thin films of NaCl/AQS mixtures and was undetected in NaCl/NOM. Lastly, studies were initiated on the generation of undecanol coated NaCl particles.

ISBN: 9781267058171Subjects--Topical Terms:

1981412
Physical chemistry.

Laboratory Studies of the Thermal and Photochemical Oxidation of Sea Salt Aerosols.
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245 1 0 $a Laboratory Studies of the Thermal and Photochemical Oxidation of Sea Salt Aerosols.
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300 $a 178 p.
500 $a Source: Dissertations Abstracts International, Volume: 73-06, Section: B.
500 $a Publisher info.: Dissertation/Thesis.
500 $a Finlayson-Pitts, Barbara J.
502 $a Thesis (Ph.D.)--University of California, Irvine, 2011.
506 $a This item is not available from ProQuest Dissertations & Theses.
506 $a This item must not be added to any third party search indexes.
506 $a This item must not be sold to any third party vendors.
520 $a Sea salt aerosols play an important role in the formation of inorganic halogen species in the troposphere and can play significant role during ozone depletion events at high and mid latitudes. The mechanisms of halogen production from sea salt oxidation are not well understood. In this dissertation the interactions of halide ions with other components present in sea salt (i.e., nitrate ions and organics) are explored and be shown to be vital in our understanding of halogen formation mechanisms. Through halide-nitrate ion photolysis experiments and computational models of aqueous mixed halide-nitrate systems, it was determined that NO2 and OH can more efficiently be produced, due to nitrate ions being drawn near the interface and experiencing a reduction in the solvent cage relative to neat NaNO3. It was determined that cations, can affect the distribution of NO3− in computational models and affect rates of NO2 from irradiated thin films of nitrate in the presence and absence of halide ions. It was shown that interfacial mechanisms of the photolysis of nitrate-halide mixtures also increased halogen production. Gas phase halogen yields increased with addition of Br− ions to synthetic sea salt. Results suggest that a new interhalogen reaction mechanism, HOCl− + Br−, may be contributing to the increase in Br 2 production at lower [Cl−]/[Br−] ratios. Yields of gas phase halogens were also strongly dependent on the acidity of the solution, while that of NO2 was not. High concentrations of NO were observed at low pH, suggesting an additional halogen formation mechanism involving H2ONO+ and Br− contributes. The observed Br2 and BrCl production initiated by the photolysis of NO3− may be contributing to tropospheric ozone destruction during the polar sunrise and at mid-latitudes. Studies were also conducted in collaboration with the Saltzman group on the photochemical production of Cl2 from NaCl/organic photosensitizer mixtures using antraquinone sulfonic acid (AQS) and natural organic matter (NOM) as the photosensitizer. These studies showed that 120 ppb of Cl2 was produced from 254 nm irradiation of thin films of NaCl/AQS mixtures and was undetected in NaCl/NOM. Lastly, studies were initiated on the generation of undecanol coated NaCl particles.
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710 2 $a University of California, Irvine. $b Chemistry - Ph.D.. $3 2094938
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