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Particle acidity and sulfate production during severe hazeevents in China cannot be reliably inferred by assuminga mixture of inorganic salts
Wang, GH(Wang, Gehui)1,2; Zhang,F(Zhang,Fang)4,5; Peng,JF(Peng,Jianfei)5,6; Duan,L(Duan,Lian)5,7; Ji,YM(Ji, Yuemeng)5,8; Wilmarie Marrero-Ortiz5; Wang,JY(Wang,Jiayuan)2; Li,JJ(Li,Jianjun)2; Wu,C(Wu, Can)2; Cao, C(Cao,Cong)2; Wang, Y(Wang,Yuan)9; Zheng, J(Zheng,Jun)10; Jeremiah Secrest5; Li,YX(Li,Yixin)5; Wang,YY(Wang,Yuying)4,5; Li,H(Li,Hong)11; Li,N(Li,Na)5,12; Zhang,RY(Zhang,Renyi)5,6; Wang, Gehui
Source PublicationAtmospheric Chemistry and Physics
AbstractAtmospheric measurements showed rapid sulfate formation during severe haze episodes in China, with fine particulate matter (PM) consisting of a multi-component mixture that is dominated by organic species. Several recent studies using the thermodynamic model estimated the particle acidity and sulfate production rate, by treating the PM exclusively as a mixture of inorganic salts dominated by ammonium sulfate and neglecting the effects of organic compounds. Noticeably, the estimated pH and sulfate formation rate during pollution periods in China were highly conflicting among the previous studies. Here we show that a particle mixture of inorganic salts adopted by the previous studies does not represent a suitable model system and that the acidity and sulfate formation cannot be reliably inferred without accounting for the effects of multi-aerosol compositions during severe haze events in China. Our laboratory experiments show that SO2 oxidation by NO2 with NH3 neutralization on fine aerosols is dependent on the particle hygroscopicity, phase-state, and acidity. Ammonium sulfate and oxalic acid seed particles exposed to vapors of SO2, NO2, and NH3 at high relative humidity (RH) exhibit distinct size growth and sulfate formation. Aqueous ammonium sulfate particles exhibit little sulfate production, in contrast to aqueous oxalic acid particles with significant sulfate production. Our field measurements demonstrate significant contribution of watersoluble organic matter to fine PM in China and indicate that the use of oxalic acid in laboratory experiments is representative of ambient organic dominant aerosols. While the particle acidity cannot be accurately determined from field measurements or calculated using the thermodynamic model, our results reveal that the pH value of ambient organics-dominated aerosols is sufficiently high to promote efficient SO2 oxidation by NO2 with NH3 neutralization under polluted conditions in China.
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Document Type期刊论文
Corresponding AuthorWang, Gehui
Affiliation1.Key Laboratory of Geographic Information Science of the Ministry of Education, School of Geographic Sciences,East China Normal University, Shanghai 200241, China
2.State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment,Chinese Academy of Sciences, Xi’an 710061, China
3.Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment,Chinese Academy of Science, Xiamen 361021, China
4.College of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, China
5.Departments of Atmospheric Sciences and Chemistry, Texas A&M University, College Station, TX, 77843, USA
6.State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciencesand Engineering, Peking University, Beijing 100871, China
7.State Environmental Protection Key Lab of Environmental Risk Assessment and control on Chemical Processes,East China University of Science and Technology, Shanghai 200237, China
8.School of Environmental Science and Engineering, Institute of Environmental Health and Pollution, Control,Guangdong University of Technology, Guangzhou 510006, China
9.Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA 91125, USA
10.Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control,Nanjing University of Information Science & Technology, Nanjing 210044, China
11.State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy ofEnvironmental Sciences, Beijing 100012, China
12.Key Laboratory of Songliao Aquatic Environment, Jilin Jianzhu University, Changchun, 130118, China
First Author AffilicationState Key Laboratory of Loess and Quaternary Geology
Recommended Citation
GB/T 7714
Wang, GH,Zhang,F,Peng,JF,et al. Particle acidity and sulfate production during severe hazeevents in China cannot be reliably inferred by assuminga mixture of inorganic salts[J]. Atmospheric Chemistry and Physics,2018,18(2018):10123-10132.
APA Wang, GH.,Zhang,F.,Peng,JF.,Duan,L.,Ji,YM.,...&Wang, Gehui.(2018).Particle acidity and sulfate production during severe hazeevents in China cannot be reliably inferred by assuminga mixture of inorganic salts.Atmospheric Chemistry and Physics,18(2018),10123-10132.
MLA Wang, GH,et al."Particle acidity and sulfate production during severe hazeevents in China cannot be reliably inferred by assuminga mixture of inorganic salts".Atmospheric Chemistry and Physics 18.2018(2018):10123-10132.
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