Serveur d'exploration sur Pittsburgh

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Secondary Organic Aerosol Formation from in-Use Motor Vehicle Emissions Using a Potential Aerosol Mass Reactor

Identifieur interne : 004F61 ( Main/Exploration ); précédent : 004F60; suivant : 004F62

Secondary Organic Aerosol Formation from in-Use Motor Vehicle Emissions Using a Potential Aerosol Mass Reactor

Auteurs : Daniel S. Tkacikt [États-Unis] ; Andrew T. Lambe [États-Unis] ; Shantanu Jathar [États-Unis] ; XIANG LI [États-Unis] ; Albert A. Presto [États-Unis] ; YUNLIANG ZHAO [États-Unis] ; Donald Blake [États-Unis] ; Simone Meinardi [États-Unis] ; John T. Jayne [États-Unis] ; Philip L. Croteau [États-Unis] ; Allen L. Robinson [États-Unis]

Source :

RBID : Pascal:15-0037256

Descripteurs français

English descriptors

Abstract

Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ˜0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ˜2.9 ± 1.6 Tg SOA yr-1 in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.


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<title xml:lang="en" level="a">Secondary Organic Aerosol Formation from in-Use Motor Vehicle Emissions Using a Potential Aerosol Mass Reactor</title>
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<name sortKey="Croteau, Philip L" sort="Croteau, Philip L" uniqKey="Croteau P" first="Philip L." last="Croteau">Philip L. Croteau</name>
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<inist:fA14 i1="03">
<s1>Aerodyne Research, Inc.</s1>
<s2>Billerica, Massachusetts 01821</s2>
<s3>USA</s3>
<sZ>2 aut.</sZ>
<sZ>9 aut.</sZ>
<sZ>10 aut.</sZ>
</inist:fA14>
<country>États-Unis</country>
<wicri:noRegion>Billerica, Massachusetts 01821</wicri:noRegion>
</affiliation>
</author>
<author>
<name sortKey="Robinson, Allen L" sort="Robinson, Allen L" uniqKey="Robinson A" first="Allen L." last="Robinson">Allen L. Robinson</name>
<affiliation wicri:level="4">
<inist:fA14 i1="02">
<s1>Center for Atmospheric Particle Studies, Carnegie Mellon University</s1>
<s2>Pittsburgh, Pennsylvania 15213</s2>
<s3>USA</s3>
<sZ>1 aut.</sZ>
<sZ>4 aut.</sZ>
<sZ>5 aut.</sZ>
<sZ>6 aut.</sZ>
<sZ>11 aut.</sZ>
</inist:fA14>
<country>États-Unis</country>
<placeName>
<settlement type="city">Pittsburgh</settlement>
<region type="state">Pennsylvanie</region>
</placeName>
<orgName type="university">Université Carnegie-Mellon</orgName>
</affiliation>
<affiliation wicri:level="4">
<inist:fA14 i1="05">
<s1>Mechanical Engineering, Carnegie Mellon University</s1>
<s2>Pittsburgh, Pennsylvania 15213</s2>
<s3>USA</s3>
<sZ>4 aut.</sZ>
<sZ>5 aut.</sZ>
<sZ>6 aut.</sZ>
<sZ>11 aut.</sZ>
</inist:fA14>
<country>États-Unis</country>
<placeName>
<settlement type="city">Pittsburgh</settlement>
<region type="state">Pennsylvanie</region>
</placeName>
<orgName type="university">Université Carnegie-Mellon</orgName>
</affiliation>
</author>
</analytic>
<series>
<title level="j" type="main">Environmental science & technology</title>
<title level="j" type="abbreviated">Environ. sci. technol.</title>
<idno type="ISSN">0013-936X</idno>
<imprint>
<date when="2014">2014</date>
</imprint>
</series>
</biblStruct>
</sourceDesc>
<seriesStmt>
<title level="j" type="main">Environmental science & technology</title>
<title level="j" type="abbreviated">Environ. sci. technol.</title>
<idno type="ISSN">0013-936X</idno>
</seriesStmt>
</fileDesc>
<profileDesc>
<textClass>
<keywords scheme="KwdEn" xml:lang="en">
<term>Aerosols</term>
<term>Air pollution</term>
<term>Emission measure</term>
<term>Exhaust gas</term>
<term>Motor vehicle</term>
<term>Pennsylvania</term>
<term>Pollutant formation</term>
<term>Road traffic</term>
<term>Road tunnel</term>
<term>Secondary pollutant</term>
<term>Urban area</term>
</keywords>
<keywords scheme="Pascal" xml:lang="fr">
<term>Formation polluant</term>
<term>Polluant secondaire</term>
<term>Aérosol</term>
<term>Trafic routier</term>
<term>Véhicule à moteur</term>
<term>Gaz échappement</term>
<term>Mesure émission</term>
<term>Tunnel routier</term>
<term>Zone urbaine</term>
<term>Pollution air</term>
<term>Pennsylvanie</term>
</keywords>
<keywords scheme="Wicri" type="topic" xml:lang="fr">
<term>Aérosol</term>
<term>Véhicule à moteur</term>
<term>Zone urbaine</term>
</keywords>
</textClass>
</profileDesc>
</teiHeader>
<front>
<div type="abstract" xml:lang="en">Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ˜0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ˜2.9 ± 1.6 Tg SOA yr
<sup>-1</sup>
in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.</div>
</front>
</TEI>
<affiliations>
<list>
<country>
<li>États-Unis</li>
</country>
<region>
<li>Pennsylvanie</li>
</region>
<settlement>
<li>Pittsburgh</li>
</settlement>
<orgName>
<li>Université Carnegie-Mellon</li>
</orgName>
</list>
<tree>
<country name="États-Unis">
<region name="Pennsylvanie">
<name sortKey="Tkacikt, Daniel S" sort="Tkacikt, Daniel S" uniqKey="Tkacikt D" first="Daniel S." last="Tkacikt">Daniel S. Tkacikt</name>
</region>
<name sortKey="Blake, Donald" sort="Blake, Donald" uniqKey="Blake D" first="Donald" last="Blake">Donald Blake</name>
<name sortKey="Croteau, Philip L" sort="Croteau, Philip L" uniqKey="Croteau P" first="Philip L." last="Croteau">Philip L. Croteau</name>
<name sortKey="Jathar, Shantanu" sort="Jathar, Shantanu" uniqKey="Jathar S" first="Shantanu" last="Jathar">Shantanu Jathar</name>
<name sortKey="Jayne, John T" sort="Jayne, John T" uniqKey="Jayne J" first="John T." last="Jayne">John T. Jayne</name>
<name sortKey="Lambe, Andrew T" sort="Lambe, Andrew T" uniqKey="Lambe A" first="Andrew T." last="Lambe">Andrew T. Lambe</name>
<name sortKey="Meinardi, Simone" sort="Meinardi, Simone" uniqKey="Meinardi S" first="Simone" last="Meinardi">Simone Meinardi</name>
<name sortKey="Presto, Albert A" sort="Presto, Albert A" uniqKey="Presto A" first="Albert A." last="Presto">Albert A. Presto</name>
<name sortKey="Presto, Albert A" sort="Presto, Albert A" uniqKey="Presto A" first="Albert A." last="Presto">Albert A. Presto</name>
<name sortKey="Robinson, Allen L" sort="Robinson, Allen L" uniqKey="Robinson A" first="Allen L." last="Robinson">Allen L. Robinson</name>
<name sortKey="Robinson, Allen L" sort="Robinson, Allen L" uniqKey="Robinson A" first="Allen L." last="Robinson">Allen L. Robinson</name>
<name sortKey="Tkacikt, Daniel S" sort="Tkacikt, Daniel S" uniqKey="Tkacikt D" first="Daniel S." last="Tkacikt">Daniel S. Tkacikt</name>
<name sortKey="Xiang Li" sort="Xiang Li" uniqKey="Xiang Li" last="Xiang Li">XIANG LI</name>
<name sortKey="Xiang Li" sort="Xiang Li" uniqKey="Xiang Li" last="Xiang Li">XIANG LI</name>
<name sortKey="Yunliang Zhao" sort="Yunliang Zhao" uniqKey="Yunliang Zhao" last="Yunliang Zhao">YUNLIANG ZHAO</name>
<name sortKey="Yunliang Zhao" sort="Yunliang Zhao" uniqKey="Yunliang Zhao" last="Yunliang Zhao">YUNLIANG ZHAO</name>
</country>
</tree>
</affiliations>
</record>

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