| Particle acidity and sulfate production during severe haze events in China cannot be reliably inferred by assuming a mixture of inorganic salts | |
| Wang, Gehui1,2,3; Zhang, Fang4,5,6; Peng, Jianfei5,6,7; Duan, Lian5,6,8; Ji, Yuemeng5,6,9; Marrero-Ortiz, Wilmarie5,6; Wang, Jiayuan2; Li, Jianjun2; Wu, Can2; Cao, Cong2; Wang, Yuan10; Zheng, Jun11; Secrest, Jeremiah5,6; Li, Yixin5,6; Wang, Yuying4,5,6; Li, Hong12; Li, Na5,6,13; Zhang, Renyi5,6,7 | |
| Corresponding Author | Wang, Gehui(ghwang@geo.ecnu.edu.cn) ; Zhang, Renyi(renyi-zhang@tamu.edu) |
| 2018-07-17 | |
| Source Publication | ATMOSPHERIC CHEMISTRY AND PHYSICS
 |
| ISSN | 1680-7316 |
| Volume | 18Issue:14Pages:10123-10132 |
| Abstract | Atmospheric 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 water-soluble 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. |
| DOI | 10.5194/acp-18-10123-2018 |
| WOS Keyword | DICARBOXYLIC-ACIDS ; ATMOSPHERIC AEROSOLS ; INLAND CHINA ; HETEROGENEOUS REACTIONS ; FORMATION MECHANISMS ; SIZE DISTRIBUTION ; AMMONIUM-SULFATE ; OXALIC-ACID ; AMINES ; PHASE |
| Indexed By | SCI ; SCI |
| Language | 英语 |
| Funding Project | National Key R&D Plan (Quantitative Relationship and Regulation Principle between Regional Oxidation Capacity of Atmospheric and Air Quality)[2017YFC0210000] ; China National Natural Science Funds for Distinguished Young Scholars[41325014] ; National Nature Science Foundation of China[41773117] ; Robert A. Welch Foundation[A-1417] ; National Science Foundation Graduate Research Fellowship Program |
| WOS Research Area | Meteorology & Atmospheric Sciences |
| Funding Organization | National Key R&D Plan (Quantitative Relationship and Regulation Principle between Regional Oxidation Capacity of Atmospheric and Air Quality) ; China National Natural Science Funds for Distinguished Young Scholars ; National Nature Science Foundation of China ; Robert A. Welch Foundation ; National Science Foundation Graduate Research Fellowship Program |
| WOS Subject | Meteorology & Atmospheric Sciences |
| WOS ID | WOS:000438945300001 |
| Publisher | COPERNICUS GESELLSCHAFT MBH |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.ieecas.cn/handle/361006/13253 |
| Collection | 粉尘与环境研究室 |
| Corresponding Author | Wang, Gehui; Zhang, Renyi |
| Affiliation | 1.East China Normal Univ, Sch Geog Sci, Minist Educ, Key Lab Geog Informat Sci, Shanghai 200241, Peoples R China 2.Chinese Acad Sci, Inst Earth Environm, State Key Lab Loess & Quaternary Geol, Xian 710061, Shaanxi, Peoples R China 3.Chinese Acad Sci, Inst Urban Environm, Ctr Excellence Reg Atmospher Environm, Xiamen 361021, Peoples R China 4.Beijing Normal Univ, Coll Global Change & Earth Syst Sci, Beijing 100875, Peoples R China 5.Texas A&M Univ, Dept Atmospher Sci, College Stn, TX 77843 USA 6.Texas A&M Univ, Dept Chem, College Stn, TX 77843 USA 7.Peking Univ, Coll Environm Sci & Engn, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100871, Peoples R China 8.East China Univ Sci & Technol, State Environm Protect Key Lab Environm Risk Asse, Shanghai 200237, Peoples R China 9.Guangdong Univ Technol, Sch Environm Sci & Engn, Inst Environm Hlth & Pollut, Control, Guangzhou 510006, Guangdong, Peoples R China 10.CALTECH, Jet Prop Lab, Pasadena, CA 91125 USA 11.Nanjing Univ Informat Sci & Technol, Jiangsu Key Lab Atmospher Environm Monitoring & P, Nanjing 210044, Jiangsu, Peoples R China 12.Chinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China 13.Jilin Jianzhu Univ, Key Lab Songliao Aquat Environm, Changchun 130118, Jilin, Peoples R China |
| Recommended Citation GB/T 7714 | Wang, Gehui,Zhang, Fang,Peng, Jianfei,et al. Particle acidity and sulfate production during severe haze events in China cannot be reliably inferred by assuming a mixture of inorganic salts[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(14):10123-10132. |
| APA | Wang, Gehui.,Zhang, Fang.,Peng, Jianfei.,Duan, Lian.,Ji, Yuemeng.,...&Zhang, Renyi.(2018).Particle acidity and sulfate production during severe haze events in China cannot be reliably inferred by assuming a mixture of inorganic salts.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(14),10123-10132. |
| MLA | Wang, Gehui,et al."Particle acidity and sulfate production during severe haze events in China cannot be reliably inferred by assuming a mixture of inorganic salts".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.14(2018):10123-10132. |
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