Date of Award

1-1-2018

Document Type

Dissertation

Degree Name

Ph.D.

Organizational Unit

Chemistry and Biochemistry

First Advisor

Brian J. Majestic, Ph.D.

Second Advisor

Shannon M. Murphy, Ph.D.

Third Advisor

Keith Miller

Fourth Advisor

Alex Huffman

Keywords

Atmospheric processing, Humic-like substances, Photochemistry, Polycyclic aromatic hydrocarbons, Soluble iron

Abstract

The details of the work presented in this dissertation focus on simulated reactions in the atmosphere and water systems between persistent aromatic compounds and varying species of metals with an emphasis on iron. Bulk water suspensions of a standard soil and polycyclic aromatic hydrocarbons (PAH) were analyzed for soluble iron by inductively-coupled plasma mass spectroscopy (ICP-MS) following a 16 hour reaction period using simulated sunlight. Significant increases in soluble iron were only seen with 2-3 ring linear PAH and carboxylic acids.

A two-stage study was conducted to investigate the potential for and possible mechanisms involving the photo-oxidation of PAH into humic-like substances (HULIS). Aqueous suspensions of PAH and oxidized PAH products are illuminated by a bench solar simulator and resulting samples are analyzed by high-pressure liquid chromatography (HPLC), UV-Vis, attenuated total reflectance Fourier transformer infrared spectroscopy (ATR-FTIR), solid-phase extraction (SPE), and electrospray ionization/atmospheric pressure chemical ionization mass spectroscopy (ESI/APCI-MS). HULIS production is based on comparison to SRFA and is observed in short chain PAH following a surface dependent path through naphthalene derivative intermediate structures. These results help explain brown carbon and health effects observed in areas affected by urban emissions.

Publication Statement

Copyright is held by the author. User is responsible for all copyright compliance.

Rights Holder

John P. Haynes

Provenance

Received from ProQuest

File Format

application/pdf

Language

en

File Size

124 p.

Discipline

Atmospheric chemistry, Analytical chemistry

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