Potential factors and mechanism of particulate matters explosive increase induced by free radicals oxidation
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摘要
Atmospheric particulate pollution in China has attracted much public attention.Occasionally, the particle number concentration increases sharply in a short time period,which is defined as a "particulate matter explosive increase". Heavy particulate matter pollution not only reduces visibility but also has an adverse effect on human health. Hence,there is an urgent need to discover the causes of particulate matter explosive increase.During this campaign, the particle number concentration and free radicals were measured at a tall building on the campus of Lanzhou University of Technology. Additionally, we examined a series of chemicals to reproduce the observed particulate matter explosive increase in a smog chamber to determine its potential factors. Then, we analyzed the mechanism of particulate matter explosive increase in the presence of free radicals. We found that, among the potential inorganic and organic sources analyzed, a mixture of organic and SO_2 in the research region had a major effect on particulate matter explosive increase. Moreover, free radical oxidation has a large effect, especially in the formation of organic particulates.
Atmospheric particulate pollution in China has attracted much public attention.Occasionally, the particle number concentration increases sharply in a short time period,which is defined as a "particulate matter explosive increase". Heavy particulate matter pollution not only reduces visibility but also has an adverse effect on human health. Hence,there is an urgent need to discover the causes of particulate matter explosive increase.During this campaign, the particle number concentration and free radicals were measured at a tall building on the campus of Lanzhou University of Technology. Additionally, we examined a series of chemicals to reproduce the observed particulate matter explosive increase in a smog chamber to determine its potential factors. Then, we analyzed the mechanism of particulate matter explosive increase in the presence of free radicals. We found that, among the potential inorganic and organic sources analyzed, a mixture of organic and SO_2 in the research region had a major effect on particulate matter explosive increase. Moreover, free radical oxidation has a large effect, especially in the formation of organic particulates.
Atmospheric particulate pollution in China has attracted much public attention.Occasionally, the particle number concentration increases sharply in a short time period,which is defined as a "particulate matter explosive increase". Heavy particulate matter pollution not only reduces visibility but also has an adverse effect on human health. Hence,there is an urgent need to discover the causes of particulate matter explosive increase.During this campaign, the particle number concentration and free radicals were measured at a tall building on the campus of Lanzhou University of Technology. Additionally, we examined a series of chemicals to reproduce the observed particulate matter explosive increase in a smog chamber to determine its potential factors. Then, we analyzed the mechanism of particulate matter explosive increase in the presence of free radicals. We found that, among the potential inorganic and organic sources analyzed, a mixture of organic and SO_2 in the research region had a major effect on particulate matter explosive increase. Moreover, free radical oxidation has a large effect, especially in the formation of organic particulates.
引文
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Zhou,J.B.,Xing,Z.Y.,Deng,J.J.,Du,K.,2016.Characterizing and sourcing ambient PM2.5over key emission regions in China I:water-soluble ions and carbonaceous fractions.Atmos.Environ.135,20-30.
Cao,J.J.,Chow,J.C.,Lee,S.C.,Li,Y.,Chen,S.W.,An,Z.S.,et al.,2005.Characterization and source apportionment of atmospheric organic and elemental carbon during fall and winter of 2003 in Xi'an,China.Atmos.Chem.Phys.5,3127-3137.
Chu,P.C.,Chen,Y.C.,Lu,S.H.,2008.Atmospheric effects on winter SO2pollution in Lanzhou,China.Atmos.Res.89,365-373.
Dominic,F.,Greenstone,M.,Sunstein,C.R.,2014.Particulate matter matters.Science 344,257-259.
Donahue,N.M.,Robinson,A.L.,Pandis,S.N.,2008.Atmospheric organic particulate matter:from smoke to secondary organic aerosol.Atmos.Environ.43,94-106.
Elser,M.,Huang,R.J.,Wolf,R.,Slowik,J.G.,Wang,Q.Y.,Canonaco,F.,et al.,2016.New insights into PM2.5chemical composition and sources in two major cities in China during extreme haze events using aerosol mass spectrometry.Atmos.Chem.and Phys.16,3207-3225.
Grundstr?m,M.,Hak,C.,Chen,D.,Hallquist,M.,Pleijel,H.,2015.Variation and co-variation of PM10,particle number concentration,NOx and NO2in the urban air-relationships with wind speed,vertical temperature gradient and weather type.Atmos.Environ.120,317-327.
Hirsikko,A.,Nieminen,T.,Gagne,S.,Lehtipalo,K.,Manninen,H.E.,Ehn,M.,et al.,2011.Atmospheric ions and nucleation:a review of observations.Atmos.Chem.Phys.11,767-798.
Huang,X.J.,Liu,Z.R.,Liu,J.Y.,Hu,B.,Wen,T.X.,Tang,G.Q.,et al.,2017.Chemical characterization and source identification of PM2.5at multiple sites in the Beijing-Tianjin-Hebei region,China.Atmos.Chem.Phys.17,12941-12962.
Jayaratnel,R.,Pushpawelal,B.,He,C.,Li,H.,Gao,J.,Chai,F.,et al.,2017.Observations of particles at their formation sizes in Beijing,China.Atmos.Chem.Phys.17,8825-8835.
Johansson,K.O.,Head-Gordon,M.P.,Schrader,P.E.,Wilson,K.R.,Michelsen,H.A.,2018.Resonance-stabilized hydrocarbonradical chain reactions may explain soot inception and growth.Science 361(6406),997-1000.
Landis,M.S.,Pancras,J.P.,Graney,J.R.,White,E.M.,Edgerton,E.S.,Legge,A.,et al.,2017.Source apportionment of ambient fine and coarse particulate matter at the Fort McKay community site,in the Athabasca Oil Sands Region,Alberta,Canada.Sci.Total Environ.585,105-117.
Li,H.,Ma,Y.L.,Duan,F.K.,He,K.B.,Zhu,L.D.,Huang,T.,et al.,2017.Typical winter haze pollution in Zibo,an industrial city in China:Characteristics,secondary formation,and regional contribution.Environ.Pollut.229,339-349.
Liu,B.S.,Li,T.K.,Yang,J.M.,Wu,J.H.,Wang,J.,Gao,J.X.,et al.,2017.Source apportionment and a novel approach of estimating regional contributions to ambient PM2.5in Haikou,China.Environ.Pollut.223,334-345.
Mentel,T.F.,Springer,M.,Ehn,M.,Kleist,E.,Pullinen,I.,Kurtén,T.,et al.,2015.Formation of highly oxidized multifunctional compounds:autoxidation of peroxy radicals formed in the ozonolysis of alkenes deduced from structure-product relationships.Atmos.Chem.Phys.15,6745-6765.
Molteni,U.,Bianchi,F.,Klein,F.,Haddad1,Carla,Frege,I.E.,Rossi,M.J.,Dommen,J.,et al.,2018.Formation of highly oxygenated organic molecules from aromatic compounds.Atmos.Chem.Phys.18,1909-1921.
Tan,J.,Zhang,L.,Zhou,X.,Duan,J.,Li,Y.,Hu,J.,et al.,2017.Chemical characteristics and source apportionment of PM2.5in Lanzhou,China.Sci.Total Environ.601(602),1743-1752.
Wagner,R.,Yan,C.,Lehtipalo,K.,Duplissy,J.,Nieminen,T.,Kangasluoma,J.,et al.,2017.The role of ions in new particle formation in the CLOUD chamber.Atmos.Chem.Phys.17,15181-15197.
Wang,S.G.,Feng,X.Y.,Zeng,X.Q.,Ma,Y.X.,Shang,K.Z.,2009.A study on variations of concentrations of particulate matter with different sizes in Lanzhou,China.Atmos.Environ.43,2823-2828.
Wang,G.Y.,Jia,S.M.,Niu,X.L.,Tian,H.Q.,Liu,Y.R.,Chen,X.F.,et al.,2017.Total free radical species and oxidation equivalent in polluted air.Sci.Total Environ.609,1103-1113.
Yao,L.,Garmash,O.,Federico,Bianchi,Jun,Zheng,Yan,C.,Kontkanen,J.,et al.,2018.Atmospheric new particle formation from sulfuric acid and amines in a Chinese megacity.Science366(6399),278-281.
Zhang,X.Y.,Wang,Y.Q.,Niu,T.,Zhang,X.C.,Gong,S.L.,Zhang,Y.M.,et al.,2012.Atmospheric aerosol compositions in China:spatial/temporal variability,chemical signature,regional haze distribution and comparisons with global aerosols.Atmos.Chem.Phys.12,779-799.
Zhang,R.Y.,Wang,G.,Guo,S.,Zamora,M.L.,Ying,Q.,Lin,Y.,et al.,2015.Formation of urban fine particulate matter.Chem.Rev.115,3803-3855.
Zhou,J.B.,Xing,Z.Y.,Deng,J.J.,Du,K.,2016.Characterizing and sourcing ambient PM2.5over key emission regions in China I:water-soluble ions and carbonaceous fractions.Atmos.Environ.135,20-30.