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DOI | 10.5194/acp-18-6679-2018 |
NO2-initiated multiphase oxidation of SO2 by O-2 on CaCO3 particles | |
Yu, Ting1,2; Zhao, Defeng1,2,3,4; Song, Xiaojuan1,2; Zhu, Tong1,2 | |
2018-05-09 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2018 |
卷号 | 18期号:9页码:6679-6689 |
文章类型 | Article |
语种 | 英语 |
国家 | Peoples R China |
英文摘要 | The reaction of SO2 with NO2 on the surface of aerosol particles has been suggested to be important in sulfate formation during severe air pollution episodes in China. However, we found that the direct oxidation of SO2 by NO2 was slow and might not be the main reason for sulfate formation in ambient air. In this study, we investigated the multiphase reaction of SO2 with an O-2 / NO2 mixture on single CaCO3 particles using Micro-Raman spectroscopy. The reaction converted the CaCO3 particle to a Ca(NO3)(2) droplet, with CaSO4 center dot 2H(2)O solid particles embedded in it, which constituted a significant fraction of the droplet volume at the end of the reaction. The reactive uptake coefficient of SO2 for sulfate formation was on the order of 10(-5), which was higher than that for the multiphase reaction of SO2 directly with NO2 by 2-3 orders of magnitude. According to our observations and the literature, we found that in the multiphase reaction of SO2 with the O-2 / NO2 mixture, O-2 was the main oxidant of SO2 and was necessary for radical chain propagation. NO2 acted as the initiator of radical formation, but not as the main oxidant. The synergy of NO2 and O-2 resulted in much faster sulfate formation than the sum of the reaction rates with NO2 and with O-2 alone. We estimated that the multiphase oxidation of SO2 by O-2 initiated by NO2 could be an important source of sulfate and a sink of SO2, based on the calculated lifetime of SO2 regarding the loss through the multiphase reaction versus the loss through the gas-phase reaction with OH radicals. Parameterization of the reactive uptake coefficient of the reaction observed in our laboratory for further model simulation is needed, as well as an integrated assessment based on field observations, laboratory study results, and model simulations to evaluate the importance of the reaction in ambient air during severe air pollution episodes, especially in China. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000431763600005 |
WOS关键词 | HETEROGENEOUS REACTION ; SULFUR(IV) OXIDES ; SULFATE FORMATION ; PULSE-RADIOLYSIS ; NITROGEN-DIOXIDE ; AQUEOUS-SOLUTION ; S(IV) OXIDATION ; CARBON NUCLEI ; MINERAL DUST ; WINTER HAZE |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/19516 |
专题 | 地球科学 |
作者单位 | 1.Peking Univ, Coll Environm Sci & Engn, BIC ESAT, Beijing 100871, Peoples R China; 2.Peking Univ, Coll Environm Sci & Engn, SKL ESPC, Beijing 100871, Peoples R China; 3.Fudan Univ, Dept Atmospher & Ocean Sci, Shanghai 200438, Peoples R China; 4.Fudan Univ, Inst Atmospher Sci, Shanghai 200438, Peoples R China |
推荐引用方式 GB/T 7714 | Yu, Ting,Zhao, Defeng,Song, Xiaojuan,et al. NO2-initiated multiphase oxidation of SO2 by O-2 on CaCO3 particles[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(9):6679-6689. |
APA | Yu, Ting,Zhao, Defeng,Song, Xiaojuan,&Zhu, Tong.(2018).NO2-initiated multiphase oxidation of SO2 by O-2 on CaCO3 particles.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(9),6679-6689. |
MLA | Yu, Ting,et al."NO2-initiated multiphase oxidation of SO2 by O-2 on CaCO3 particles".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.9(2018):6679-6689. |
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