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Development and Application of an Ox...

Palm, Brett Brian,

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Development and Application of an Oxidation Flow Reactor to Study Secondary Organic Aerosol Formation from Ambient Air /

Record Type:	Electronic resources : Monograph/item
Title/Author:	Development and Application of an Oxidation Flow Reactor to Study Secondary Organic Aerosol Formation from Ambient Air // Brett Brian Palm.
Author:	Palm, Brett Brian,
Description:	1 electronic resource (223 pages)
Notes:	Source: Dissertations Abstracts International, Volume: 78-12, Section: B.
Contained By:	Dissertations Abstracts International78-12B.
Subject:	Atmospheric sciences. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10271219
ISBN:	9781369785678

Development and Application of an Oxidation Flow Reactor to Study Secondary Organic Aerosol Formation from Ambient Air /
Palm, Brett Brian,

Development and Application of an Oxidation Flow Reactor to Study Secondary Organic Aerosol Formation from Ambient Air /Brett Brian Palm. - 1 electronic resource (223 pages)

Source: Dissertations Abstracts International, Volume: 78-12, Section: B.

Secondary organic aerosols (SOA) in the atmosphere play an important role in air quality, human health, and climate. However, the sources, formation pathways, and fate of SOA are poorly constrained. In this dissertation, I present development and application of the oxidation flow reactor (OFR) technique for studying SOA formation from OH, O3, and NO3 oxidation of ambient air. With a several-minute residence time and a portable design with no inlet, OFRs are particularly well-suited for this purpose. I first introduce the OFR concept, and discuss several advances I have made in performing and interpreting OFR experiments. This includes estimating oxidant exposures, modeling the fate of low-volatility gases in the OFR (wall loss, condensation, and oxidation), and comparing SOA yields of single precursors in the OFR with yields measured in environmental chambers. When these experimental details are carefully considered, SOA formation in an OFR can be more reliably compared with ambient SOA formation processes. I then present an overview of what OFR measurements have taught us about SOA formation in the atmosphere. I provide a comparison of SOA formation from OH, O3, and NO3 oxidation of ambient air in a wide variety of environments, from rural forests to urban air. In a rural forest, the SOA formation correlated with biogenic precursors (e.g., monoterpenes). In urban air, it correlated instead with reactive anthropogenic tracers (e.g., trimethylbenzene). In mixed-source regions, the SOA formation did not correlate well with any single precursor, but could be predicted by multilinear regression from several precursors. Despite these correlations, the concentrations of speciated ambient VOCs could only explain approximately 10-50% of the total SOA formed from OH oxidation. In contrast, ambient VOCs could explain all of the SOA formation observed from O3 and NO3 oxidation. Evidence suggests that lower-volatility gases (semivolatile and intermediate-volatility organic compounds; S/IVOCs) were present in ambient air and were the likely source of SOA formation that could not be explained by VOCs. These measurements show that S/IVOCs likely play an important intermediary role in ambient SOA formation in all of the sampled locations, from rural forests to urban air.

English

ISBN: 9781369785678Subjects--Topical Terms:

3168354
Atmospheric sciences.
Subjects--Index Terms:

Aerosol

Development and Application of an Oxidation Flow Reactor to Study Secondary Organic Aerosol Formation from Ambient Air /
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300 $a 1 electronic resource (223 pages)
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500 $a Source: Dissertations Abstracts International, Volume: 78-12, Section: B.
500 $a Publisher info.: Dissertation/Thesis.
500 $a Advisors: Jimenez, Jose-Luis Committee members: Brown, Steven S.; Browne, Eleanor; Hodzic, Alma; Ziemann, Paul J.
502 $b Ph.D. $c University of Colorado at Boulder $d 2017.
520 $a Secondary organic aerosols (SOA) in the atmosphere play an important role in air quality, human health, and climate. However, the sources, formation pathways, and fate of SOA are poorly constrained. In this dissertation, I present development and application of the oxidation flow reactor (OFR) technique for studying SOA formation from OH, O3, and NO3 oxidation of ambient air. With a several-minute residence time and a portable design with no inlet, OFRs are particularly well-suited for this purpose. I first introduce the OFR concept, and discuss several advances I have made in performing and interpreting OFR experiments. This includes estimating oxidant exposures, modeling the fate of low-volatility gases in the OFR (wall loss, condensation, and oxidation), and comparing SOA yields of single precursors in the OFR with yields measured in environmental chambers. When these experimental details are carefully considered, SOA formation in an OFR can be more reliably compared with ambient SOA formation processes. I then present an overview of what OFR measurements have taught us about SOA formation in the atmosphere. I provide a comparison of SOA formation from OH, O3, and NO3 oxidation of ambient air in a wide variety of environments, from rural forests to urban air. In a rural forest, the SOA formation correlated with biogenic precursors (e.g., monoterpenes). In urban air, it correlated instead with reactive anthropogenic tracers (e.g., trimethylbenzene). In mixed-source regions, the SOA formation did not correlate well with any single precursor, but could be predicted by multilinear regression from several precursors. Despite these correlations, the concentrations of speciated ambient VOCs could only explain approximately 10-50% of the total SOA formed from OH oxidation. In contrast, ambient VOCs could explain all of the SOA formation observed from O3 and NO3 oxidation. Evidence suggests that lower-volatility gases (semivolatile and intermediate-volatility organic compounds; S/IVOCs) were present in ambient air and were the likely source of SOA formation that could not be explained by VOCs. These measurements show that S/IVOCs likely play an important intermediary role in ambient SOA formation in all of the sampled locations, from rural forests to urban air.
546 $a English
590 $a School code: 0051
650 4 $a Atmospheric sciences. $3 3168354
650 4 $a Environmental science. $3 677245
650 4 $a Atmospheric chemistry. $3 544140
653 $a Aerosol
653 $a Gas phase oxidation
653 $a Organic aerosol
653 $a Oxidation flow reactor
653 $a Potential aerosol mass
653 $a Secondary organic aerosol
690 $a 0371
690 $a 0725
690 $a 0768
710 2 $a University of Colorado at Boulder. $b Chemistry. $e degree granting institution. $3 3824215
720 1 $a Jimenez, Jose-Luis $e degree supervisor.
773 0 $t Dissertations Abstracts International $g 78-12B.
790 $a 0051
791 $a Ph.D.
792 $a 2017
856 4 0 $u https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10271219