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Secondary organic aerosol (SOA) formation from aqueous OH radical oxidation of dicarbonyl compounds in the atmosphere
Descriptive
TypeOfResource
Text
TitleInfo
(ID = T-1)
Title
Secondary organic aerosol (SOA) formation from aqueous OH radical oxidation of dicarbonyl compounds in the atmosphere
Identifier
ETD_2895
Identifier
(type = hdl)
http://hdl.rutgers.edu/1782.1/rucore10001600001.ETD.000056804
Language
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eng
Genre
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theses
Subject
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(authority = RUETD)
Topic
Environmental Sciences
Subject
(ID = SBJ-2);
(authority = ETD-LCSH)
Topic
Aerosols--Health aspects
Subject
(ID = SBJ-3);
(authority = ETD-LCSH)
Topic
Atmospheric aerosols--Research
Abstract
(type = abstract)
Secondary organic aerosols (SOA) affect visibility, health and global climate. Current chemical transport models cannot represent SOA in the free troposphere. Fog/cloud processing, which is the dominant source of atmospheric sulfate, has been recognized as a missing source of SOA globally. Aqueous photooxidation of water-soluble products (e.g., glyoxal and methylglyoxal) of gas-phase photochemistry yields low-volatility compounds including oxalic acid. When this chemistry takes place in clouds and fogs followed by droplet evaporation (or if this chemistry occurs in aerosol water) then products remain in part in the particle phase, forming SOA. However, current aqueous SOA formation mechanism has not shown how the starting concentrations of precursors and presence of acidic sulfate affect product formation. Aqueous phase photochemical batch reactions were conducted with glyoxal and methylglyoxal at cloud relevant concentrations, using hydrogen peroxide photolysis as the hydroxyl radical (∙OH) source. Experiments were repeated at higher concentrations and with/without sulfuric acid. Precursors and products were investigated using ion chromatography (IC), electrospray ionization mass spectrometry (ESI-MS), and IC-ESI-MS. Products included carboxylic acids and higher molecular weight compounds, which are major constituents of aerosols. Sulfuric acid shows little effect on product formation. Dilute aqueous chemistry models successfully reproduced product formation for glyoxal and methylglyoxal at cloud relevant conditions, but measurements deviated from predictions from predictions at elevated concentrations. Higher molecular weight products become increasingly important as precursor concentration increases. Aqueous radical-radical reactions provide explanations for observed higher molecular weight products. Additionally, acetic acid is identified as an SOA precursor for the first time. This work provides an improved understanding of aqueous phase dicarbonyl oxidation mechanism and the overall significance of aqueous SOA formation. Kinetic data are made available to regional and global atmospheric models, and the mechanism described in this work will help people to mitigate adverse aerosol effects.
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electronic resource
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xv, 219 p. : ill.
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application/pdf
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text/xml
Note
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Ph.D.
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Includes bibliographical references
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Includes vita
Note
(type = statement of responsibility)
by Yi Tan
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Tan
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Yi
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1983-
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author
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Yi Tan
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Barbara J.
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chair
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Advisory Committee
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Barbara J. Turpin
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Reinfelder
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John
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internal member
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Advisory Committee
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John Reinfelder
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Seitzinger
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Sybil P.
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internal member
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Advisory Committee
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Sybil P. Seitzinger
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Carlton
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(type = given)
Ann Marie
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outside member
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Advisory Committee
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Ann Marie Carlton
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Rutgers University
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degree grantor
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Graduate School - New Brunswick
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school
OriginInfo
DateCreated
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2010
DateOther
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2010-10
Place
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(type = code)
xx
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TitleInfo
Title
Rutgers University Electronic Theses and Dissertations
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ETD
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Title
Graduate School - New Brunswick Electronic Theses and Dissertations
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rucore19991600001
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NjNbRU
Identifier
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doi:10.7282/T3542N9P
Genre
(authority = ExL-Esploro)
ETD doctoral
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Rights
RightsDeclaration
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(ID = rulibRdec0006)
The author owns the copyright to this work.
Copyright
Status
Copyright protected
Availability
Status
Open
Reason
Permission or license
RightsHolder
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(type = personal)
Name
FamilyName
Tan
GivenName
Yi
Role
Copyright Holder
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Type
Permission or license
DateTime
2010-09-23 11:46:44
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Name
Yi Tan
Affiliation
Rutgers University. Graduate School - New Brunswick
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Author Agreement License
Detail
I hereby grant to the Rutgers University Libraries and to my school the non-exclusive right to archive, reproduce and distribute my thesis or dissertation, in whole or in part, and/or my abstract, in whole or in part, in and from an electronic format, subject to the release date subsequently stipulated in this submittal form and approved by my school. I represent and stipulate that the thesis or dissertation and its abstract are my original work, that they do not infringe or violate any rights of others, and that I make these grants as the sole owner of the rights to my thesis or dissertation and its abstract. I represent that I have obtained written permissions, when necessary, from the owner(s) of each third party copyrighted matter to be included in my thesis or dissertation and will supply copies of such upon request by my school. I acknowledge that RU ETD and my school will not distribute my thesis or dissertation or its abstract if, in their reasonable judgment, they believe all such rights have not been secured. I acknowledge that I retain ownership rights to the copyright of my work. I also retain the right to use all or part of this thesis or dissertation in future works, such as articles or books.
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Technical
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ETD
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application/pdf
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application/x-tar
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1638400
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