Understanding primary and secondary sources of ambient oxygenated volatile organic compounds in Shenzhen utilizing photochemical age-based parameterization method
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摘要
Oxygenated volatile organic compounds(OVOCs) are key intermediates in the atmospheric photooxidation process. To further study the primary and secondary sources of OVOCs,their ambient levels were monitored using a proton-transfer reaction mass spectrometer(PTR-MS) at an urban site in the Pearl River Delta of China. Continuous monitoring campaigns were conducted in the spring, summer, fall, and winter of 2016. Among the six types of OVOC species, the mean concentrations of methanol were the highest in each season(up to 13–20 ppbv), followed by those of acetone, acetaldehyde and acetic acid(approximately 2–4 ppbv), while those of formic acid and methyl ethyl ketone(MEK) were the lowest(approximately 1–2 ppbv). As observed from a diurnal variation chart, the OVOCs observed in Shenzhen may have been affected by numerous factors such as their primary and secondary sources and photochemical consumption. The photochemical age-based parameterization method was used to apportion the sources of ambient OVOCs. Methanol had significant anthropogenic primary sources but negligible anthropogenic secondary sources during all of the seasons. Acetone, MEK and acetic acid were mostly attributed to anthropogenic primary sources during each season with smaller contributions from anthropogenic secondary sources. Acetaldehyde had similar contributions from both anthropogenic secondary and anthropogenic primary sources throughout the year.Meanwhile, anthropogenic primary sources contributed the most to formic acid.
Oxygenated volatile organic compounds(OVOCs) are key intermediates in the atmospheric photooxidation process. To further study the primary and secondary sources of OVOCs,their ambient levels were monitored using a proton-transfer reaction mass spectrometer(PTR-MS) at an urban site in the Pearl River Delta of China. Continuous monitoring campaigns were conducted in the spring, summer, fall, and winter of 2016. Among the six types of OVOC species, the mean concentrations of methanol were the highest in each season(up to 13–20 ppbv), followed by those of acetone, acetaldehyde and acetic acid(approximately 2–4 ppbv), while those of formic acid and methyl ethyl ketone(MEK) were the lowest(approximately 1–2 ppbv). As observed from a diurnal variation chart, the OVOCs observed in Shenzhen may have been affected by numerous factors such as their primary and secondary sources and photochemical consumption. The photochemical age-based parameterization method was used to apportion the sources of ambient OVOCs. Methanol had significant anthropogenic primary sources but negligible anthropogenic secondary sources during all of the seasons. Acetone, MEK and acetic acid were mostly attributed to anthropogenic primary sources during each season with smaller contributions from anthropogenic secondary sources. Acetaldehyde had similar contributions from both anthropogenic secondary and anthropogenic primary sources throughout the year.Meanwhile, anthropogenic primary sources contributed the most to formic acid.
Oxygenated volatile organic compounds(OVOCs) are key intermediates in the atmospheric photooxidation process. To further study the primary and secondary sources of OVOCs,their ambient levels were monitored using a proton-transfer reaction mass spectrometer(PTR-MS) at an urban site in the Pearl River Delta of China. Continuous monitoring campaigns were conducted in the spring, summer, fall, and winter of 2016. Among the six types of OVOC species, the mean concentrations of methanol were the highest in each season(up to 13–20 ppbv), followed by those of acetone, acetaldehyde and acetic acid(approximately 2–4 ppbv), while those of formic acid and methyl ethyl ketone(MEK) were the lowest(approximately 1–2 ppbv). As observed from a diurnal variation chart, the OVOCs observed in Shenzhen may have been affected by numerous factors such as their primary and secondary sources and photochemical consumption. The photochemical age-based parameterization method was used to apportion the sources of ambient OVOCs. Methanol had significant anthropogenic primary sources but negligible anthropogenic secondary sources during all of the seasons. Acetone, MEK and acetic acid were mostly attributed to anthropogenic primary sources during each season with smaller contributions from anthropogenic secondary sources. Acetaldehyde had similar contributions from both anthropogenic secondary and anthropogenic primary sources throughout the year.Meanwhile, anthropogenic primary sources contributed the most to formic acid.
引文
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Apel,E.C.,Riemer,D.D.,Hills,A.,Baugh,W.,Orlando,J.,Faloona,I.et al.,2002.Measurement and interpretation of isoprene fluxes and isoprene,methacrolein,and methyl vinyl ketone mixing ratios at the PROPHET site during the 1998 Intensive.J.Geophys.Res.107(D3),H1-H7.
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Atkinson,R.,Baulch,D.L.,Cox,R.A.,Crowley,J.N.,Hampson,R.F.,Hynes,R.G.,et al.,2006.Evaluated kinetic and photochemical data for atmospheric chemistry:volume II-gas phase reactions of organic species.Atmos.Chem.Phys.6,3625-4055.
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Carter,W.,1994.Development of ozone reactivity scales for volatile organic compounds.J.Air Waste Manage.Assoc.44,881-899.
Carter,W.,1998.Updated Maximum Incremental Reactivity Scale for Regulatory Applications,Preliminary Report to California Air Resources Board.University of California,Riverside,CA,USA.
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de Gouw,J.A.,Warneke,C.,2007.Measurement of volatile organic compounds in the Earth's atmosphere using proton-transfer-reaction mass spectrometry.Mass Spectrom.Rev.26,223-257.
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Friedfeld,S.,Fraser,M.,Ensor,K.,Tribble,S.,Rehle,D.,Leleux,D.,et al.,2002.Statistical analysis of primary and secondary atmospheric formaldehyde.Atmos.Environ.36,4767-4775.
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Legreid,G.,L??v,J.B.,Staehelin,J.,Hueglin,C.,Hill,M.,Buchmann,B.,et al.,2007.Oxygenated volatile organic compounds(OVOCs)at an urban background site in Zürich(Europe):seasonal variation and source allocation.Atmos.Environ.41,8409-8423.
Li,Y.,Shao,M.,Lu,S.,Chang,C.,Dasgupta,P.K.,2010.Variations and sources of ambient formaldehyde for the 2008 Beijing Olympic games.Atmos.Environ.44,2632-2639.
Liggio,J.,Li,S.M.,McLaren,R.,2005.Reactive uptake of glyoxal by particulate matter.J.Geophys.Res.-Atmos 110,D10304.
Lindinger,W.,Hansel,A.,Jordan,A.,1998.On-line monitoring of volatile organic compounds at pptv levels by means of protontransfer-reaction mass spectrometry(PTR-MS)-Medical applications,food control and environmental research.Int.J.Mass Spectrom.173(3),191-241.
Liu,Y.,Shao,M.,Kuster,W.C.,Goldan,P.D.,Li,X.H.,Lu,S.H.,et al.,2009.Source identification of reactive hydrocarbons and oxygenated VOCs in the summertime in Beijing.Environ.Sci.Technol.43,75-81.
Liu,R.L.,Huang,X.F.,He,L.Y.,Yuan,B.,Lu,S.H.,Feng,N.,2012.On-line measurements and source analysis of VOCs in the atmosphere using Proton Transfer Reaction-Mass Spectrometry:case study in summer of Shenzhen.Acta Sci.Circumst.32,2540-2547.
Liu,Y.,Yuan,B.,Li,X.,Shao,M.,Lu,S.,Li,Y.,et al.,2015.Impact of pollution controls in Beijing on atmospheric oxygenated volatile organic compounds(OVOCs)during the 2008 Olympic Games:observation and modeling implications.Atmos.Chem.Phys.15,3045-3062.
Lü,H.,Cai,Q.Y.,Wen,S.,Chi,Y.,Guo,S.,Sheng,G.,et al.,2010.Seasonal and diurnal variation of carbonyl compounds in the urban atmosphere of Guangzhou,China.Sci.Total Environ.408,3523-3529.
Ma,Y.,Diao,Y.,Zhang,B.,Wang,W.,Ren,X.,Yang,D.,et al.,2016.Detection of formaldehyde emissions from an industrial zone in the Yangtze River Delta region of China using a proton transfer reaction ion-drift chemical ionization mass spectrometer.Atmos.Meas.Tech.9,6101-6116.
Ou,J.,Zheng,J.,Li,R.,Huang,X.,Zhong,Z.,Zhong,L.,et al.,2015.Speciated OVOC and VOC emission inventories and their implications for reactivity-based ozone control strategy in the Pearl River Delta region,China.Sci.Total Environ.530,393-402.
Pang,X.,Mu,Y.,2006.Seasonal and diurnal variations of carbonyl compounds in Beijing ambient air.Atmos.Environ.40(33),6313-6320.
Perry,R.,Gee,I.L.,1995.Vehicle emissions in relation to fuel composition.Sci.Total Environ.34,577-584.
Seinfeld,J.H.,Pandis,S.N.,2006.Properties of the atmospheric aerosol.In:Seinfeld,J.H.,Pandis,S.N.(Eds.),Atmospheric Chemistry and Physics:From Air Pollution to Climate Change.Wiley-Interscience,New York,pp.350-389.
Shao,M.,Wang,B.,Lu,S.,Yuan,B.,Wang,M.,2011.Effects of Beijing Olympics control measures on reducing reactive hydrocarbon species.Environ.Sci.Technol.45,514-519.
Sin,D.W.M.,Wong,Y.C.,Louie,P.K.K.,2001.Trend of ambient carbonyl compounds in the urban environment of Hong Kong.Atmos.Environ.35,5961-5969.
Singh,H.B.,Kanakidou,M.,Crutzen,P.J.,Jacob,D.J.,1995.High concentrations and photochemical fate of oxygenated hydrocarbons in the global troposphere.Nature 378,50-54.
Stoji?,A.,Stoji?,S.S.,?o?tari?,A.,Miji?,Z.,Peri?i?,M.,Raj?i?,S.,2015.Characterization of VOC sources in an urban area based on PTR-MS measurements and receptor modelling.Environ.Sci.Pollut.Res.22,13137-13152.
Wang,M.,Shao,M.Z.,Chen,W.W.,Yuan,B.,Lu,S.,Zhang,Q.,et al.,2013a.Validation of emission inventories by measurements of ambient volatile organic compounds in Beijing,China.Atmos.Chem.Phys.13,26933-26979.
Wang,Q.,Chen,C.,Wang,H.L.,Zhou,M.,Lou,S.R.,Qiao,L.P.,et al.,2013b.Forming Potential of Secondary Organic Aerosols and Sources Apportionment of VOCs in Autumn of Shanghai,China.Environ.Sci.34(2),424-433.
WHO,2000.Air Quality Guidelines for Europe.second ed.WHORegional Publications,European Series No91.WHO,Copenhagen.
Yuan,B.,Shao,M.,de Gouw,J.,Parrish,D.D.,Lu,S.H.,Wang,M.,et al.,2012.Volatile organic compounds(VOCs)in urban air:how chemistry affects the interpretation of positive matrix factorization(PMF)analysis.J.Geophys.Res.-Atmos.117,D24302.
Zhang,Y.H.,Su,H.,Zhong,L.J.,Cheng,Y.F.,Zeng,L.M.,Wang,X.S.,et al.,2008.Regional ozone pollution and observation-based approach for analyzing ozone-precursor relationship during the PRIDE-PRD2004 campaign.Atmos.Environ.42,6203-6218.
Zhang,Y.,Wang,X.,Barletta,B.,Simpson,I.J.,Blake,D.R.,Fu,X.,et al.,2013.Source attributions of hazardous aromatic hydrocarbons in urban,suburban and rural areas in the Pearl River Delta(PRD)region.J.Hazard.Mater.250,403-411.
Zhang,H.,Li,H.,Zhang,Q.Z.,Zhang,Y.J.,Zhang,W.Q.,Wang,X.Z.,et al.,2017.Atmospheric volatile organic compounds in a typical urban area of Beijing pollution characterization,health risk assessment and source apportionment.Atmosphere 8,61.
Zheng,J.,Shao,M.,Che,W.,Zhang,L.,Zhong,L.,Zhang,Y.,et al.,2009.Speciated VOC emission inventory and spatial patterns of ozone formation potential in the Pearl River Delta,China.Environ.Sci.Technol.43(22),8580-8586.
Zheng,J.,Zhang,R.,Garzón,J.P.,Huertas,M.E.,Levy,M.,Ma,Y.,et al.,2013.Measurements of formaldehyde at the U.S.-Mexico border during the Cal-Mex 2010 air quality study.Atmos.Environ.70,513-520.
Apel,E.C.,Riemer,D.D.,Hills,A.,Baugh,W.,Orlando,J.,Faloona,I.et al.,2002.Measurement and interpretation of isoprene fluxes and isoprene,methacrolein,and methyl vinyl ketone mixing ratios at the PROPHET site during the 1998 Intensive.J.Geophys.Res.107(D3),H1-H7.
Atkinson,R.,2000.Atmospheric chemistry of VOCs and NOx.Atmos.Environ.34,2063-2101.
Atkinson,R.,Arey,J.,2003.Atmospheric degradation of volatile organic compounds.Chem.Rev.103,4605-4638.
Atkinson,R.,Baulch,D.L.,Cox,R.A.,Crowley,J.N.,Hampson,R.F.,Hynes,R.G.,et al.,2006.Evaluated kinetic and photochemical data for atmospheric chemistry:volume II-gas phase reactions of organic species.Atmos.Chem.Phys.6,3625-4055.
Barletta,B.,Meinardi,S.,Simpson,I.J.,Zou,S.,Rowland,F.S.,Blake,D.R.,2008.Ambient mixing ratios of nonmethane hydrocarbons(NMHCs)in two major urban centers of the Pearl River Delta(PRD)region:Guangzhou and Dongguan.Atmos.Environ.42,4393-4408.
Bashkin,V.N.,2009.Environmental Chemistry:Asian Lessons.Kluwer Academic Pub.,Netherlands.
Baudic,A.,Gros,V.,Sauvage,S.,Locoge,N.,Sanchez,O.,SardaEstève,R.,et al.,2016.Seasonal variability and source apportionment of volatile organic compounds(VOCs)in the Paris megacity(France).Atmos.Chem.Phys.16(18),1-51.
Brocco,D.,Fratarcangeli,R.,Lepore,L.,Petricca,M.,Ventrone,I.,1997.Determination of aromatic hydrocarbons in urban air of Roma.Atmos.Environ.31,557-566.
Carter,W.,1994.Development of ozone reactivity scales for volatile organic compounds.J.Air Waste Manage.Assoc.44,881-899.
Carter,W.,1998.Updated Maximum Incremental Reactivity Scale for Regulatory Applications,Preliminary Report to California Air Resources Board.University of California,Riverside,CA,USA.
Chen,W.T.,Shao,M.,Lu,S.H.,Wang,M.,Zeng,L.M.,Yuan,B.,et al.,2014.Understanding primary and secondary sources of ambient carbonyl compounds in Beijing using the PMF model.Atmos.Chem.Phys.14,3047-3062.
de Gouw,J.A.,Warneke,C.,2007.Measurement of volatile organic compounds in the Earth's atmosphere using proton-transfer-reaction mass spectrometry.Mass Spectrom.Rev.26,223-257.
de Gouw,J.A.,Middlebrook,A.M.,Warneke,C.,Goldan,P.D.,Kuster,W.C.,Roberts,J.M.,et al.,2005.Budget of organic carbon in a polluted atmosphere:results from the New England Air Quality Study in 2002.J.Geophys.Res.-Atmos.110,D16305.
Fall,R.,1999.Biogenic emissions of volatile organic compounds from higher plants.In:Hewitt,C.N.(Ed.),Reactive Hydrocarbons in the Atmosphere.Elsevier,New York,pp.41-96.
Finlayson-Pitts,B.J.,Pitts,J.N.,1997.Tropospheric air pollution:ozone,airborne toxics,polycyclic aromatic hydrocarbons,and particles.Science 276,1045-1052.
Friedfeld,S.,Fraser,M.,Ensor,K.,Tribble,S.,Rehle,D.,Leleux,D.,et al.,2002.Statistical analysis of primary and secondary atmospheric formaldehyde.Atmos.Environ.36,4767-4775.
Guenther,A.,Hewitt,C.N.,Erickson,D.,Fall,R.,Geron,C.,Graedel,T.,et al.,1995.A global model of natural volatile organic compound emissions.J.Geophys.Res.100,8873-8892.
Harley,R.A.,Hannigan,M.P.,Cass,G.R.,1992.Respeciation of organic gas emissions and the detection of excess unburned gasoline in the atmosphere.Environ.Sci.Technol.26,2395-2408.
Huang,J.,Feng,Y.L.,Li,J.,Xiong,B.,Feng,J.L.,Wen,S.,et al.,2008.Characteristics of carbonyl compounds in ambient air of Shanghai,China.J.Atmos.Chem.61,1-20.
Huang,X.,Yun,H.,Gong,Z.,Li,X.,He,L.,Zhang,Y.,et al.,2014.Source apportionment and secondary organic aerosol estimation of PM2.5in an urban atmosphere in China.Sci.China Earth Sci.57,1352-1362.
Kristensson,A.,Johansson,C.,Westerholm,R.,Swietlicki,E.,Gidhagen,L.,Wideqvist,U.,et al.,2004.Real-world traffic emission factors of gases and particles measured in a road tunnel in Stockholm,Sweden.Atmos.Environ.38,657-673.
Legreid,G.,L??v,J.B.,Staehelin,J.,Hueglin,C.,Hill,M.,Buchmann,B.,et al.,2007.Oxygenated volatile organic compounds(OVOCs)at an urban background site in Zürich(Europe):seasonal variation and source allocation.Atmos.Environ.41,8409-8423.
Li,Y.,Shao,M.,Lu,S.,Chang,C.,Dasgupta,P.K.,2010.Variations and sources of ambient formaldehyde for the 2008 Beijing Olympic games.Atmos.Environ.44,2632-2639.
Liggio,J.,Li,S.M.,McLaren,R.,2005.Reactive uptake of glyoxal by particulate matter.J.Geophys.Res.-Atmos 110,D10304.
Lindinger,W.,Hansel,A.,Jordan,A.,1998.On-line monitoring of volatile organic compounds at pptv levels by means of protontransfer-reaction mass spectrometry(PTR-MS)-Medical applications,food control and environmental research.Int.J.Mass Spectrom.173(3),191-241.
Liu,Y.,Shao,M.,Kuster,W.C.,Goldan,P.D.,Li,X.H.,Lu,S.H.,et al.,2009.Source identification of reactive hydrocarbons and oxygenated VOCs in the summertime in Beijing.Environ.Sci.Technol.43,75-81.
Liu,R.L.,Huang,X.F.,He,L.Y.,Yuan,B.,Lu,S.H.,Feng,N.,2012.On-line measurements and source analysis of VOCs in the atmosphere using Proton Transfer Reaction-Mass Spectrometry:case study in summer of Shenzhen.Acta Sci.Circumst.32,2540-2547.
Liu,Y.,Yuan,B.,Li,X.,Shao,M.,Lu,S.,Li,Y.,et al.,2015.Impact of pollution controls in Beijing on atmospheric oxygenated volatile organic compounds(OVOCs)during the 2008 Olympic Games:observation and modeling implications.Atmos.Chem.Phys.15,3045-3062.
Lü,H.,Cai,Q.Y.,Wen,S.,Chi,Y.,Guo,S.,Sheng,G.,et al.,2010.Seasonal and diurnal variation of carbonyl compounds in the urban atmosphere of Guangzhou,China.Sci.Total Environ.408,3523-3529.
Ma,Y.,Diao,Y.,Zhang,B.,Wang,W.,Ren,X.,Yang,D.,et al.,2016.Detection of formaldehyde emissions from an industrial zone in the Yangtze River Delta region of China using a proton transfer reaction ion-drift chemical ionization mass spectrometer.Atmos.Meas.Tech.9,6101-6116.
Ou,J.,Zheng,J.,Li,R.,Huang,X.,Zhong,Z.,Zhong,L.,et al.,2015.Speciated OVOC and VOC emission inventories and their implications for reactivity-based ozone control strategy in the Pearl River Delta region,China.Sci.Total Environ.530,393-402.
Pang,X.,Mu,Y.,2006.Seasonal and diurnal variations of carbonyl compounds in Beijing ambient air.Atmos.Environ.40(33),6313-6320.
Perry,R.,Gee,I.L.,1995.Vehicle emissions in relation to fuel composition.Sci.Total Environ.34,577-584.
Seinfeld,J.H.,Pandis,S.N.,2006.Properties of the atmospheric aerosol.In:Seinfeld,J.H.,Pandis,S.N.(Eds.),Atmospheric Chemistry and Physics:From Air Pollution to Climate Change.Wiley-Interscience,New York,pp.350-389.
Shao,M.,Wang,B.,Lu,S.,Yuan,B.,Wang,M.,2011.Effects of Beijing Olympics control measures on reducing reactive hydrocarbon species.Environ.Sci.Technol.45,514-519.
Sin,D.W.M.,Wong,Y.C.,Louie,P.K.K.,2001.Trend of ambient carbonyl compounds in the urban environment of Hong Kong.Atmos.Environ.35,5961-5969.
Singh,H.B.,Kanakidou,M.,Crutzen,P.J.,Jacob,D.J.,1995.High concentrations and photochemical fate of oxygenated hydrocarbons in the global troposphere.Nature 378,50-54.
Stoji?,A.,Stoji?,S.S.,?o?tari?,A.,Miji?,Z.,Peri?i?,M.,Raj?i?,S.,2015.Characterization of VOC sources in an urban area based on PTR-MS measurements and receptor modelling.Environ.Sci.Pollut.Res.22,13137-13152.
Wang,M.,Shao,M.Z.,Chen,W.W.,Yuan,B.,Lu,S.,Zhang,Q.,et al.,2013a.Validation of emission inventories by measurements of ambient volatile organic compounds in Beijing,China.Atmos.Chem.Phys.13,26933-26979.
Wang,Q.,Chen,C.,Wang,H.L.,Zhou,M.,Lou,S.R.,Qiao,L.P.,et al.,2013b.Forming Potential of Secondary Organic Aerosols and Sources Apportionment of VOCs in Autumn of Shanghai,China.Environ.Sci.34(2),424-433.
WHO,2000.Air Quality Guidelines for Europe.second ed.WHORegional Publications,European Series No91.WHO,Copenhagen.
Yuan,B.,Shao,M.,de Gouw,J.,Parrish,D.D.,Lu,S.H.,Wang,M.,et al.,2012.Volatile organic compounds(VOCs)in urban air:how chemistry affects the interpretation of positive matrix factorization(PMF)analysis.J.Geophys.Res.-Atmos.117,D24302.
Zhang,Y.H.,Su,H.,Zhong,L.J.,Cheng,Y.F.,Zeng,L.M.,Wang,X.S.,et al.,2008.Regional ozone pollution and observation-based approach for analyzing ozone-precursor relationship during the PRIDE-PRD2004 campaign.Atmos.Environ.42,6203-6218.
Zhang,Y.,Wang,X.,Barletta,B.,Simpson,I.J.,Blake,D.R.,Fu,X.,et al.,2013.Source attributions of hazardous aromatic hydrocarbons in urban,suburban and rural areas in the Pearl River Delta(PRD)region.J.Hazard.Mater.250,403-411.
Zhang,H.,Li,H.,Zhang,Q.Z.,Zhang,Y.J.,Zhang,W.Q.,Wang,X.Z.,et al.,2017.Atmospheric volatile organic compounds in a typical urban area of Beijing pollution characterization,health risk assessment and source apportionment.Atmosphere 8,61.
Zheng,J.,Shao,M.,Che,W.,Zhang,L.,Zhong,L.,Zhang,Y.,et al.,2009.Speciated VOC emission inventory and spatial patterns of ozone formation potential in the Pearl River Delta,China.Environ.Sci.Technol.43(22),8580-8586.
Zheng,J.,Zhang,R.,Garzón,J.P.,Huertas,M.E.,Levy,M.,Ma,Y.,et al.,2013.Measurements of formaldehyde at the U.S.-Mexico border during the Cal-Mex 2010 air quality study.Atmos.Environ.70,513-520.