Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM 2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study
In the southeastern US, substantial emissions of isoprene from deciduous trees undergo atmospheric oxidation to form secondary organic aerosol (SOA) that contributes to fine particulate matter (PM2.5). Laboratory studies have revealed that anthropogenic pollutants, such as sulfur dioxide (SO2), oxid...
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creator | Rattanavaraha, Weruka Chu, Kevin Budisulistiorini, Sri Hapsari Riva, Matthieu Lin, Ying-Hsuan Edgerton, Eric S. Baumann, Karsten Shaw, Stephanie L. Guo, Hongyu King, Laura Weber, Rodney J. Neff, Miranda E. Stone, Elizabeth A. Offenberg, John H. Zhang, Zhenfa Gold, Avram Surratt, Jason D. |
description | In the southeastern US, substantial emissions of isoprene from deciduous trees undergo atmospheric oxidation to form secondary organic aerosol (SOA) that contributes to fine particulate matter (PM2.5). Laboratory studies have revealed that anthropogenic pollutants, such as sulfur dioxide (SO2), oxides of nitrogen (NOx), and aerosol acidity, can enhance SOA formation from the hydroxyl radical (OH)-initiated oxidation of isoprene; however, the mechanisms by which specific pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected at the Birmingham, Alabama (BHM), ground site during the 2013 Southern Oxidant and Aerosol Study (SOAS). Sample extracts were analyzed by gas chromatography–electron ionization-mass spectrometry (GC/EI-MS) with prior trimethylsilylation and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS) to identify known isoprene SOA tracers. Tracers quantified using both surrogate and authentic standards were compared with collocated gas- and particle-phase data as well as meteorological data provided by the Southeastern Aerosol Research and Characterization (SEARCH) network to assess the impact of anthropogenic pollution on isoprene-derived SOA formation. Results of this study reveal that isoprene-derived SOA tracers contribute a substantial mass fraction of organic matter (OM) ( ∼ 7 to ∼ 20 %). Isoprene-derived SOA tracers correlated with sulfate (SO42−) (r2 = 0.34, n = 117) but not with NOx. Moderate correlations between methacrylic acid epoxide and hydroxymethyl-methyl-α-lactone (together abbreviated MAE/HMML)-derived SOA tracers with nitrate radical production (P[NO3]) (r2 = 0.57, n = 40) were observed during nighttime, suggesting a potential role of the NO3 radical in forming this SOA type. However, the nighttime correlation of these tracers with nitrogen dioxide (NO2) (r2 = 0.26, n = 40) was weaker. Ozone (O3) correlated strongly with MAE/HMML-derived tracers (r2 = 0.72, n = 30) and moderately with 2-methyltetrols (r2 = 0.34, n = 15) during daytime only, suggesting that a fraction of SOA formation could occur from isoprene ozonolysis in urban areas. No correlation was observed between aerosol pH and isoprene-derived SOA. Lack of correlation between aerosol acidity |
doi_str_mv | 10.5194/acp-16-4897-2016 |
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Laboratory studies have revealed that anthropogenic pollutants, such as sulfur dioxide (SO2), oxides of nitrogen (NOx), and aerosol acidity, can enhance SOA formation from the hydroxyl radical (OH)-initiated oxidation of isoprene; however, the mechanisms by which specific pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected at the Birmingham, Alabama (BHM), ground site during the 2013 Southern Oxidant and Aerosol Study (SOAS). Sample extracts were analyzed by gas chromatography–electron ionization-mass spectrometry (GC/EI-MS) with prior trimethylsilylation and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS) to identify known isoprene SOA tracers. Tracers quantified using both surrogate and authentic standards were compared with collocated gas- and particle-phase data as well as meteorological data provided by the Southeastern Aerosol Research and Characterization (SEARCH) network to assess the impact of anthropogenic pollution on isoprene-derived SOA formation. Results of this study reveal that isoprene-derived SOA tracers contribute a substantial mass fraction of organic matter (OM) ( ∼ 7 to ∼ 20 %). Isoprene-derived SOA tracers correlated with sulfate (SO42−) (r2 = 0.34, n = 117) but not with NOx. Moderate correlations between methacrylic acid epoxide and hydroxymethyl-methyl-α-lactone (together abbreviated MAE/HMML)-derived SOA tracers with nitrate radical production (P[NO3]) (r2 = 0.57, n = 40) were observed during nighttime, suggesting a potential role of the NO3 radical in forming this SOA type. However, the nighttime correlation of these tracers with nitrogen dioxide (NO2) (r2 = 0.26, n = 40) was weaker. Ozone (O3) correlated strongly with MAE/HMML-derived tracers (r2 = 0.72, n = 30) and moderately with 2-methyltetrols (r2 = 0.34, n = 15) during daytime only, suggesting that a fraction of SOA formation could occur from isoprene ozonolysis in urban areas. No correlation was observed between aerosol pH and isoprene-derived SOA. Lack of correlation between aerosol acidity and isoprene-derived SOA is consistent with the observation that acidity is not a limiting factor for isoprene SOA formation at the BHM site as aerosols were acidic enough to promote multiphase chemistry of isoprene-derived epoxides throughout the duration of the study. All in all, these results confirm previous studies suggesting that anthropogenic pollutants enhance isoprene-derived SOA formation.</description><identifier>ISSN: 1680-7324</identifier><identifier>ISSN: 1680-7316</identifier><identifier>EISSN: 1680-7324</identifier><identifier>DOI: 10.5194/acp-16-4897-2016</identifier><language>eng</language><publisher>Katlenburg-Lindau: Copernicus GmbH</publisher><subject>Acidity ; Aerosol acidity ; Aerosol formation ; Aerosol research ; Aerosols ; Anthropogenic factors ; Atmospheric chemistry ; Chromatography ; Correlation ; Deciduous trees ; Duration ; Epoxides ; Gas chromatography ; Human influences ; Hydroxyl radicals ; Ionization ; Ions ; Isoprene ; Limiting factors ; Liquid chromatography ; Mass spectrometry ; Mass spectroscopy ; Meteorological data ; Methacrylic acid ; Night ; Night-time ; Nighttime ; Nitrogen compounds ; Nitrogen dioxide ; Nitrogen oxides ; Organic matter ; Oxidation ; Oxides ; Oxidizing agents ; Ozone ; Ozonolysis ; Particulate emissions ; Particulate matter ; pH effects ; Pollutants ; Pollution ; Quadrupoles ; Scientific imaging ; Secondary aerosols ; Spectroscopy ; Sulfates ; Sulfur ; Sulfur dioxide ; Sulphur ; Suspended particulate matter ; Tracers ; Trimethylsilylation ; Urban areas</subject><ispartof>Atmospheric chemistry and physics, 2016-04, Vol.16 (8), p.4897-4914</ispartof><rights>Copyright Copernicus GmbH 2016</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c1823-7ca6f7f8f7a485a6fc9aef458bfe6050ac58be7c463dbcc118f95619c2fe472e3</citedby><cites>FETCH-LOGICAL-c1823-7ca6f7f8f7a485a6fc9aef458bfe6050ac58be7c463dbcc118f95619c2fe472e3</cites><orcidid>0000-0002-5715-9157 ; 0000-0003-4045-5539 ; 0000-0002-6833-1450 ; 0000-0001-8904-1287 ; 0000-0003-0765-8035</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,864,27924,27925</link.rule.ids></links><search><creatorcontrib>Rattanavaraha, Weruka</creatorcontrib><creatorcontrib>Chu, Kevin</creatorcontrib><creatorcontrib>Budisulistiorini, Sri Hapsari</creatorcontrib><creatorcontrib>Riva, Matthieu</creatorcontrib><creatorcontrib>Lin, Ying-Hsuan</creatorcontrib><creatorcontrib>Edgerton, Eric S.</creatorcontrib><creatorcontrib>Baumann, Karsten</creatorcontrib><creatorcontrib>Shaw, Stephanie L.</creatorcontrib><creatorcontrib>Guo, Hongyu</creatorcontrib><creatorcontrib>King, Laura</creatorcontrib><creatorcontrib>Weber, Rodney J.</creatorcontrib><creatorcontrib>Neff, Miranda E.</creatorcontrib><creatorcontrib>Stone, Elizabeth A.</creatorcontrib><creatorcontrib>Offenberg, John H.</creatorcontrib><creatorcontrib>Zhang, Zhenfa</creatorcontrib><creatorcontrib>Gold, Avram</creatorcontrib><creatorcontrib>Surratt, Jason D.</creatorcontrib><title>Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM 2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study</title><title>Atmospheric chemistry and physics</title><description>In the southeastern US, substantial emissions of isoprene from deciduous trees undergo atmospheric oxidation to form secondary organic aerosol (SOA) that contributes to fine particulate matter (PM2.5). Laboratory studies have revealed that anthropogenic pollutants, such as sulfur dioxide (SO2), oxides of nitrogen (NOx), and aerosol acidity, can enhance SOA formation from the hydroxyl radical (OH)-initiated oxidation of isoprene; however, the mechanisms by which specific pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected at the Birmingham, Alabama (BHM), ground site during the 2013 Southern Oxidant and Aerosol Study (SOAS). Sample extracts were analyzed by gas chromatography–electron ionization-mass spectrometry (GC/EI-MS) with prior trimethylsilylation and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS) to identify known isoprene SOA tracers. Tracers quantified using both surrogate and authentic standards were compared with collocated gas- and particle-phase data as well as meteorological data provided by the Southeastern Aerosol Research and Characterization (SEARCH) network to assess the impact of anthropogenic pollution on isoprene-derived SOA formation. Results of this study reveal that isoprene-derived SOA tracers contribute a substantial mass fraction of organic matter (OM) ( ∼ 7 to ∼ 20 %). Isoprene-derived SOA tracers correlated with sulfate (SO42−) (r2 = 0.34, n = 117) but not with NOx. Moderate correlations between methacrylic acid epoxide and hydroxymethyl-methyl-α-lactone (together abbreviated MAE/HMML)-derived SOA tracers with nitrate radical production (P[NO3]) (r2 = 0.57, n = 40) were observed during nighttime, suggesting a potential role of the NO3 radical in forming this SOA type. However, the nighttime correlation of these tracers with nitrogen dioxide (NO2) (r2 = 0.26, n = 40) was weaker. Ozone (O3) correlated strongly with MAE/HMML-derived tracers (r2 = 0.72, n = 30) and moderately with 2-methyltetrols (r2 = 0.34, n = 15) during daytime only, suggesting that a fraction of SOA formation could occur from isoprene ozonolysis in urban areas. No correlation was observed between aerosol pH and isoprene-derived SOA. Lack of correlation between aerosol acidity and isoprene-derived SOA is consistent with the observation that acidity is not a limiting factor for isoprene SOA formation at the BHM site as aerosols were acidic enough to promote multiphase chemistry of isoprene-derived epoxides throughout the duration of the study. All in all, these results confirm previous studies suggesting that anthropogenic pollutants enhance isoprene-derived SOA formation.</description><subject>Acidity</subject><subject>Aerosol acidity</subject><subject>Aerosol formation</subject><subject>Aerosol research</subject><subject>Aerosols</subject><subject>Anthropogenic factors</subject><subject>Atmospheric chemistry</subject><subject>Chromatography</subject><subject>Correlation</subject><subject>Deciduous trees</subject><subject>Duration</subject><subject>Epoxides</subject><subject>Gas chromatography</subject><subject>Human influences</subject><subject>Hydroxyl radicals</subject><subject>Ionization</subject><subject>Ions</subject><subject>Isoprene</subject><subject>Limiting factors</subject><subject>Liquid chromatography</subject><subject>Mass spectrometry</subject><subject>Mass spectroscopy</subject><subject>Meteorological data</subject><subject>Methacrylic acid</subject><subject>Night</subject><subject>Night-time</subject><subject>Nighttime</subject><subject>Nitrogen compounds</subject><subject>Nitrogen dioxide</subject><subject>Nitrogen oxides</subject><subject>Organic matter</subject><subject>Oxidation</subject><subject>Oxides</subject><subject>Oxidizing agents</subject><subject>Ozone</subject><subject>Ozonolysis</subject><subject>Particulate emissions</subject><subject>Particulate matter</subject><subject>pH effects</subject><subject>Pollutants</subject><subject>Pollution</subject><subject>Quadrupoles</subject><subject>Scientific imaging</subject><subject>Secondary aerosols</subject><subject>Spectroscopy</subject><subject>Sulfates</subject><subject>Sulfur</subject><subject>Sulfur dioxide</subject><subject>Sulphur</subject><subject>Suspended particulate matter</subject><subject>Tracers</subject><subject>Trimethylsilylation</subject><subject>Urban 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the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM 2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study</title><author>Rattanavaraha, Weruka ; Chu, Kevin ; Budisulistiorini, Sri Hapsari ; Riva, Matthieu ; Lin, Ying-Hsuan ; Edgerton, Eric S. ; Baumann, Karsten ; Shaw, Stephanie L. ; Guo, Hongyu ; King, Laura ; Weber, Rodney J. ; Neff, Miranda E. ; Stone, Elizabeth A. ; Offenberg, John H. ; Zhang, Zhenfa ; Gold, Avram ; Surratt, Jason D.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c1823-7ca6f7f8f7a485a6fc9aef458bfe6050ac58be7c463dbcc118f95619c2fe472e3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><topic>Acidity</topic><topic>Aerosol acidity</topic><topic>Aerosol formation</topic><topic>Aerosol research</topic><topic>Aerosols</topic><topic>Anthropogenic 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effects</topic><topic>Pollutants</topic><topic>Pollution</topic><topic>Quadrupoles</topic><topic>Scientific imaging</topic><topic>Secondary aerosols</topic><topic>Spectroscopy</topic><topic>Sulfates</topic><topic>Sulfur</topic><topic>Sulfur dioxide</topic><topic>Sulphur</topic><topic>Suspended particulate matter</topic><topic>Tracers</topic><topic>Trimethylsilylation</topic><topic>Urban areas</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Rattanavaraha, Weruka</creatorcontrib><creatorcontrib>Chu, Kevin</creatorcontrib><creatorcontrib>Budisulistiorini, Sri Hapsari</creatorcontrib><creatorcontrib>Riva, Matthieu</creatorcontrib><creatorcontrib>Lin, Ying-Hsuan</creatorcontrib><creatorcontrib>Edgerton, Eric S.</creatorcontrib><creatorcontrib>Baumann, Karsten</creatorcontrib><creatorcontrib>Shaw, Stephanie L.</creatorcontrib><creatorcontrib>Guo, Hongyu</creatorcontrib><creatorcontrib>King, Laura</creatorcontrib><creatorcontrib>Weber, Rodney 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Laura</au><au>Weber, Rodney J.</au><au>Neff, Miranda E.</au><au>Stone, Elizabeth A.</au><au>Offenberg, John H.</au><au>Zhang, Zhenfa</au><au>Gold, Avram</au><au>Surratt, Jason D.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM 2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study</atitle><jtitle>Atmospheric chemistry and physics</jtitle><date>2016-04-21</date><risdate>2016</risdate><volume>16</volume><issue>8</issue><spage>4897</spage><epage>4914</epage><pages>4897-4914</pages><issn>1680-7324</issn><issn>1680-7316</issn><eissn>1680-7324</eissn><abstract>In the southeastern US, substantial emissions of isoprene from deciduous trees undergo atmospheric oxidation to form secondary organic aerosol (SOA) that contributes to fine particulate matter (PM2.5). Laboratory studies have revealed that anthropogenic pollutants, such as sulfur dioxide (SO2), oxides of nitrogen (NOx), and aerosol acidity, can enhance SOA formation from the hydroxyl radical (OH)-initiated oxidation of isoprene; however, the mechanisms by which specific pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected at the Birmingham, Alabama (BHM), ground site during the 2013 Southern Oxidant and Aerosol Study (SOAS). Sample extracts were analyzed by gas chromatography–electron ionization-mass spectrometry (GC/EI-MS) with prior trimethylsilylation and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS) to identify known isoprene SOA tracers. Tracers quantified using both surrogate and authentic standards were compared with collocated gas- and particle-phase data as well as meteorological data provided by the Southeastern Aerosol Research and Characterization (SEARCH) network to assess the impact of anthropogenic pollution on isoprene-derived SOA formation. Results of this study reveal that isoprene-derived SOA tracers contribute a substantial mass fraction of organic matter (OM) ( ∼ 7 to ∼ 20 %). Isoprene-derived SOA tracers correlated with sulfate (SO42−) (r2 = 0.34, n = 117) but not with NOx. Moderate correlations between methacrylic acid epoxide and hydroxymethyl-methyl-α-lactone (together abbreviated MAE/HMML)-derived SOA tracers with nitrate radical production (P[NO3]) (r2 = 0.57, n = 40) were observed during nighttime, suggesting a potential role of the NO3 radical in forming this SOA type. However, the nighttime correlation of these tracers with nitrogen dioxide (NO2) (r2 = 0.26, n = 40) was weaker. Ozone (O3) correlated strongly with MAE/HMML-derived tracers (r2 = 0.72, n = 30) and moderately with 2-methyltetrols (r2 = 0.34, n = 15) during daytime only, suggesting that a fraction of SOA formation could occur from isoprene ozonolysis in urban areas. No correlation was observed between aerosol pH and isoprene-derived SOA. Lack of correlation between aerosol acidity and isoprene-derived SOA is consistent with the observation that acidity is not a limiting factor for isoprene SOA formation at the BHM site as aerosols were acidic enough to promote multiphase chemistry of isoprene-derived epoxides throughout the duration of the study. All in all, these results confirm previous studies suggesting that anthropogenic pollutants enhance isoprene-derived SOA formation.</abstract><cop>Katlenburg-Lindau</cop><pub>Copernicus GmbH</pub><doi>10.5194/acp-16-4897-2016</doi><tpages>18</tpages><orcidid>https://orcid.org/0000-0002-5715-9157</orcidid><orcidid>https://orcid.org/0000-0003-4045-5539</orcidid><orcidid>https://orcid.org/0000-0002-6833-1450</orcidid><orcidid>https://orcid.org/0000-0001-8904-1287</orcidid><orcidid>https://orcid.org/0000-0003-0765-8035</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | Acidity Aerosol acidity Aerosol formation Aerosol research Aerosols Anthropogenic factors Atmospheric chemistry Chromatography Correlation Deciduous trees Duration Epoxides Gas chromatography Human influences Hydroxyl radicals Ionization Ions Isoprene Limiting factors Liquid chromatography Mass spectrometry Mass spectroscopy Meteorological data Methacrylic acid Night Night-time Nighttime Nitrogen compounds Nitrogen dioxide Nitrogen oxides Organic matter Oxidation Oxides Oxidizing agents Ozone Ozonolysis Particulate emissions Particulate matter pH effects Pollutants Pollution Quadrupoles Scientific imaging Secondary aerosols Spectroscopy Sulfates Sulfur Sulfur dioxide Sulphur Suspended particulate matter Tracers Trimethylsilylation Urban areas |
title | Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM 2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study |
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