ICCAS OpenIR
The influence of relative humidity on the heterogeneous oxidation of sulfur dioxide by ozone on calcium carbonate particles
Zhang, Ying1,2; Tong, Shengrui1; Ge, Maofa1,2,3; Jing, Bo1; Hou, Siqi1,2; Tan, Fang1,2; Chen, Yi1,2; Guo, Yucong1; Wu, Lingyan4
2018-08-15
Source PublicationSCIENCE OF THE TOTAL ENVIRONMENT
ISSN0048-9697
Volume633Pages:1253-1262
AbstractHeterogeneous reactions of SO2 and O-3 with CaCO3 particles were investigated at a series of relative humidity (RH, 1% to 90%) and 298 K using a diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The uptake coefficients of SO2 on CaCO3 at different RHs were obtained for the first time. Our results proved that high RH could substantially promote the formation of sulfate, for which the highest concentration (80% RH and reaction time of 200 min) and highest formation rate in stable stage (85% RH) were 14 times and 43 times that at 1% RH, respectively. The surface products, increment of concentration and formation rate of sulfate changed with RH which were due to the surface adsorbed water (SAW) on the particles. SAW could increase the reactive sites on the particles and thus accelerate the conversion of SO2 into sulfite, and sulfite could be oxidized rapidly. Liquid-like water layers formed on the particle surface could enhance the ion mobility and promote the aggregation of CaSO4 hydrates, which could expose more reactive sites and result in additional adsorption of SO2. Piece-wise equations of uptake coefficient with RH were given and could be referred by model simulation. The results are of importance in understanding the explosive growth of sulfate during severe haze episodes accompanied with high RH. (C) 2018 Elsevier B.V. All rights reserved.
KeywordHeterogeneous Reactions Sulfate Formation Uptake Coefficient Rh
DOI10.1016/j.scitotenv.2018.03.288
Indexed BySCI
Language英语
WOS IDWOS:000432475300122
PublisherELSEVIER SCIENCE BV
Citation statistics
Cited Times:7[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.iccas.ac.cn/handle/121111/42688
Collection中国科学院化学研究所
Corresponding AuthorTong, Shengrui; Ge, Maofa
Affiliation1.Chinese Acad Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Inst Chem, CAS Res Educ Ctr Excellence Mol Sci, Beijing 100190, Peoples R China
4.Chinese Acad Meteorol Sci, State Key Lab Severe Weather, Beijing 100081, Peoples R China
5.Chinese Acad Meteorol Sci, Key Lab Atmospher Chem CMA, Beijing 100081, Peoples R China
Recommended Citation
GB/T 7714
Zhang, Ying,Tong, Shengrui,Ge, Maofa,et al. The influence of relative humidity on the heterogeneous oxidation of sulfur dioxide by ozone on calcium carbonate particles[J]. SCIENCE OF THE TOTAL ENVIRONMENT,2018,633:1253-1262.
APA Zhang, Ying.,Tong, Shengrui.,Ge, Maofa.,Jing, Bo.,Hou, Siqi.,...&Wu, Lingyan.(2018).The influence of relative humidity on the heterogeneous oxidation of sulfur dioxide by ozone on calcium carbonate particles.SCIENCE OF THE TOTAL ENVIRONMENT,633,1253-1262.
MLA Zhang, Ying,et al."The influence of relative humidity on the heterogeneous oxidation of sulfur dioxide by ozone on calcium carbonate particles".SCIENCE OF THE TOTAL ENVIRONMENT 633(2018):1253-1262.
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