Sources of methacrolein and methyl vinyl ketone and their contributions to methylglyoxal and formaldehyde at a receptor site in Pearl River Delta
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摘要
Methacrolein(MACR) and methyl vinyl ketone(MVK) are two major intermediate products from the photochemical oxidation of isoprene, the most important biogenic volatile organic compound. In addition, MACR and MVK have primary emissions. Investigating the sources and evolution of MACR and MVK could provide helpful information for the oxidative capacity of the atmosphere. In this study, hourly measurements of isoprene, MACR, and MVK were conducted at a receptor site in the Pearl River Delta region(PRD), i.e., the Heshan site(HS), from 22 October to 20 November, 2014. The average mixing ratios of isoprene,MACR and MVK were 151 ± 17, 91 ± 6 and 79 ± 6 pptv, respectively. The daily variations and the ratios of MVK/MACR during daytime and nighttime suggested that other sources besides isoprene photooxidation influenced the MACR and MVK abundances at the HS.Positive matrix factorization was utilized to resolve the sources of MACR and MVK. Five sources were identified and quantified, including biogenic emissions, biomass burning,secondary formation, diesel, and gasoline vehicular emissions. Among them, secondary formation made the greatest contribution to observed MACR and MVK with average contributions of ～ 45% and ～ 70%, respectively. Through the yields of secondary products from the oxidation of MACR and MVK by the OH radical and the concentrations of MACR and MVK, it was found that methylglyoxal and formaldehyde were the main oxidation products of MACR and MVK at the HS site. Overall, this study evaluated the roles of primary emissions on ambient levels of MACR and MVK and advanced the understanding of photochemical oxidation of MACR and MVK in the PRD.
Methacrolein(MACR) and methyl vinyl ketone(MVK) are two major intermediate products from the photochemical oxidation of isoprene, the most important biogenic volatile organic compound. In addition, MACR and MVK have primary emissions. Investigating the sources and evolution of MACR and MVK could provide helpful information for the oxidative capacity of the atmosphere. In this study, hourly measurements of isoprene, MACR, and MVK were conducted at a receptor site in the Pearl River Delta region(PRD), i.e., the Heshan site(HS), from 22 October to 20 November, 2014. The average mixing ratios of isoprene,MACR and MVK were 151 ± 17, 91 ± 6 and 79 ± 6 pptv, respectively. The daily variations and the ratios of MVK/MACR during daytime and nighttime suggested that other sources besides isoprene photooxidation influenced the MACR and MVK abundances at the HS.Positive matrix factorization was utilized to resolve the sources of MACR and MVK. Five sources were identified and quantified, including biogenic emissions, biomass burning,secondary formation, diesel, and gasoline vehicular emissions. Among them, secondary formation made the greatest contribution to observed MACR and MVK with average contributions of ～ 45% and ～ 70%, respectively. Through the yields of secondary products from the oxidation of MACR and MVK by the OH radical and the concentrations of MACR and MVK, it was found that methylglyoxal and formaldehyde were the main oxidation products of MACR and MVK at the HS site. Overall, this study evaluated the roles of primary emissions on ambient levels of MACR and MVK and advanced the understanding of photochemical oxidation of MACR and MVK in the PRD.
Methacrolein(MACR) and methyl vinyl ketone(MVK) are two major intermediate products from the photochemical oxidation of isoprene, the most important biogenic volatile organic compound. In addition, MACR and MVK have primary emissions. Investigating the sources and evolution of MACR and MVK could provide helpful information for the oxidative capacity of the atmosphere. In this study, hourly measurements of isoprene, MACR, and MVK were conducted at a receptor site in the Pearl River Delta region(PRD), i.e., the Heshan site(HS), from 22 October to 20 November, 2014. The average mixing ratios of isoprene,MACR and MVK were 151 ± 17, 91 ± 6 and 79 ± 6 pptv, respectively. The daily variations and the ratios of MVK/MACR during daytime and nighttime suggested that other sources besides isoprene photooxidation influenced the MACR and MVK abundances at the HS.Positive matrix factorization was utilized to resolve the sources of MACR and MVK. Five sources were identified and quantified, including biogenic emissions, biomass burning,secondary formation, diesel, and gasoline vehicular emissions. Among them, secondary formation made the greatest contribution to observed MACR and MVK with average contributions of ～ 45% and ～ 70%, respectively. Through the yields of secondary products from the oxidation of MACR and MVK by the OH radical and the concentrations of MACR and MVK, it was found that methylglyoxal and formaldehyde were the main oxidation products of MACR and MVK at the HS site. Overall, this study evaluated the roles of primary emissions on ambient levels of MACR and MVK and advanced the understanding of photochemical oxidation of MACR and MVK in the PRD.
引文
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Carter,W.P.L.,Atkinson,R.,1996.Development and evaluation of a detailed mechanism for the atmospheric reactions of isoprene and NOx.In.J.Chem.Kinet.28,497-530.
Carvalho,L.R.F.,Vasconcellos,P.C.,Mantovani,W.,Pool,C.S.,Pisani,S.O.,2005.Measurements of biogenic hydrocarbons and carbonyl compounds emitted by trees from temperate warm Atlantic rainforest,Brazil.J.Environ.Monitor.7,493-499.
Chen,W.T.,Shao,M.,Lu,S.H.,Wang,M.,Zeng,L.M.,Yuan,B.,Liu,Y.,2013.Understanding primary and secondary sources of ambient carbonyl compounds in Beijing using the PMF model.Atmos.Chem.Phys.14,3047-3062.
Cheung,K.,Guo,H.,Ou,J.M.,Simpson,I.J.,Barletta,B.,Meinardi,S.,Blake,D.R.,2014.Diurnal profiles of isoprene,methacrolein and methyl vinyl ketone at an urban site in Hong Kong.Atmos.Environ.84,323-331.
Chew,A.A.,Atkinson,R.,Aschmann,S.M.,1998.Kinetics of the gas phase reaction of NO3radicals with a series of alcohols,glycolethers,ethers and chloroalkenes.J.Chem.Soc.Faraday Trans.94,1083-1089.
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Fan,J.,Zhang,R.,2004.Atmospheric oxidation mechanism of isoprene.Environ.Chem.1,140-149.
Fuchs,H.,Albrecht,S.,Acir,I.H.,Bohn,B.,Breitenlechner,M.,Dorn,H.,et al.,2018.Investigation of the oxidation of methyl vinyl ketone(MVK)by OH radicals in the atmospheric simulation chamber SAPHIR.Atmos.Chem.Phys.Discuss.18(11),8001-8016.https://doi.org/10.519/acp-2018-265.
Gillman,J.B.,Lerner,B.M.,Kuster,W.C.,Goldan,P.D.,Warneke,C.,Veres,P.R.,et al.,2015.Biomass burning emissions and potential air quality impacts of volatile organic compounds and other trace gases from fuels common in the US.Atmos.Chem.Phys.15,13915-13928.
Grosjean,D.,Grosjean,E.,Gertler,A.W.,2001.On-road emissions of carbonyls from light-duty and heavy-duty vehicles.Environ.Sci.Technol.35,45-53.
Guenther,A.,2008.Are plant emissions green?Nature 452,701-702.https://doi.org/10.1038/452701a.
Guenther,A.,Karl,T.,Harley,P.,Wiedinmyer,C.,Palmer,P.I.,Geron,C.,2006.Estimates of global terrestrial isoprene emissions using MEGAN(Model of Emissions of Gases and Aerosols from Nature).Atmos.Chem.Phys.6,3181-3210.
Guo,H.,Cheng,H.R.,Ling,Z.H.,Louie,P.K.K.,Ayoko,G.A.,2011.Which emission sources are responsible for the volatile organic compounds in the atmosphere of Pearl River Delta?J.Hazard.Mater.188,116-124.
Guo,H.,Ling,Z.H.,Simpson,I.J.,Blake,D.R.,Wang,D.W.,2012.Observations of isoprene,methacrolein(MAC)and methyl vinyl ketone(MVK)at a mountain site in Hong Kong.J.Geophys.Res.117,D19303 10.1029.2012JD017750.
Guo,H.,Ling,Z.H.,Cheng,H.R.,Simpson,I.J.,Lyu,X.P.,Wang,X.M.,et al.,2017.Tropospheric volatile organic compounds in China.Sci.Total Environ.574,1021-1043.
Guven,B.B.,Olaguer,E.,2011.Ambient formaldehyde source attribution in Houston during Tex AQS II and TRAMP.Atmos.Environ.45,4272-4280.
Hasa,E.,2015.The impact of isoprene and methacrolein chemistry on air quality in Europe Dissertation submitted to Department of Chemical Engineering of University of Patras.July 2015.
He,Z.R.,Ling,Z.H.,et al.,2018.Contribution of Different Anthropogenic NMHCs Sources to O3Formation at a Receptor Site in the Pearl River Delta Region and Policy Implication Submitted to Journal of Cleaner Production.
HKEPD(Hong Kong Environmental Protection Department),2015.Characterisation of VOC sources and integrated photochemical ozone analysis in Hong Kong and the Pearl River Delta region.Final report.
Ho,K.F.,Lee,S.C.,Ho,W.K.,Blake,D.R.,et al.,2009.Vehicular emission of volatile organic compounds(VOCs)from a tunnel study in Hong Kong.Atmos.Chem.Phys.9,7491-7504.
Inomata,S.,Tanimoto,H.,Pan,X.L.,Taketani,F.,Komazaki,Y.,Miyakawa,T.,et al.,2014.Laboratory measurements of emission factors of nonmethane volatile organic compounds from burning of Chinese crop residues.J.Geophys.Res.120(10),5237-5252.https://doi.org/10.1002/2014JD022761.
Jardine,K.J.,Monson,R.K.,Abrell,L.,Saleska,S.R.,Arneth,A.,Jardine,A.,et al.,2011.Within-plant isoprene oxidation confirmed by direct emissions of oxidation products methyl vinyl ketone and methacrolein.Glob.Chang.Biol.18(3),973-984.https://doi.org/10.1111/j.1365-2486.2011.02610.x.
Jenkin,M.E.,Clemitshaw,K.C.,2000.Ozone and other secondary photochemical pollutants:chemical processes governing their formation in the planetary boundary layer.Atmos.Environ.34,2499-2527.
Jones,C.E.,Hopkins,J.R.,Lewis,A.C.,2011.In situ measurements of isoprene and monoterpenes within a south-east Asian tropical rainforest.Atmos.Chem.Phys.11,6971-6984.https://doi.org/10.5194/acp-11-6971-2011.
Karl,T.,Guenther,A.,Turnipseed,A.A.,Tyndall,G.S.,Artaxo,P.,Martin,S.T.,2009.Rapid formation of isoprene photooxidation products observed in Amazonia.Atmos.Chem.Phys.9,7753-7767.https://doi.org/10.5194/acp-9-7753-2009.
Kudo,S.,Tanimoto,H.,Inomata,S.,Saito,S.,Pan,X.,Kanaya,Y.,et al.,2013.Emissions of nonmethane volatile organic compounds from open crop residue burning in the Yangtze River Delta region.China.J.Geophys.Res.119(12),7684-7698.https://doi.org/10.1002/2003JD021044.
Lau,A.K.H.,Yuan,Z.,Yu,J.Z.,Louie,P.K.K.,2010.Source apportionment of ambient volatile organic compounds in Hong Kong.Sci.Total Environ.408,4138-4149.
Leung,D.Y.C.,Wong,P.,Cheung,B.K.H.,Guenther,A.,2010.Improved land cover and emission factor for modeling biogenic volatile organic compounds emissions from Hong Kong.Atmos.Environ.44,1456-1468.
Ling,Z.H.,Guo,H.,Chen,G.X.,Lam,S.H.M.,Fan,S.J.,2016.Formaldehyde and acetaldehyde at different elevations in mountainous areas in Hong Kong.Aerosol Air Qual.Res.16,1868-1878.
Ling,Z.H.,Zhao,J.,Fan,S.J.,Wang,X.M.,2017.Sources of formaldehyde and their contributions to photochemical O3formation at an urban site in the Pearl River Delta,southern China.Chemosphere 168,1293-1301.
Liu,Y.,Shao,M.,Fu,L.L.,Lu,S.H.,et al.,2008.Source profiles of volatile organic compounds(VOCs)measured in China:part I.Atmos.Environ.42,6247-6260.
Liu,Y.,Shao,M.,Kuster,W.C.,Goldan,P.D.,Li,X.H.,Lu,S.H.,de Gouw,J.A.,2009.Source identification of reactive hydrocarbons and oxygenated VOCs in the summertime in Beijing.Environ.Sci.Technol.43,75-81.
Makar,P.A.,Fuentes,J.D.,Wang,D.,Staebler,R.M.,Wiebe,H.A.,1999.Chemical processing of biogenic hydrocarbons within and above a temperate deciduous forest.J.Geophys.Res.104(D3),3581-3603.
Park,C.G.,Schade,W.,Boedeker,I.,2011.Characteristic of the flux of isoprene and its oxidation products in an urban area.J.Geophys.Res.116,D21303.https://doi.org/10.1029/2011JD015856.
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