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DOI | 10.5194/acp-19-6737-2019 |
Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing; China | |
Qiu X.; Ying Q.; Wang S.; Duan L.; Zhao J.; Xing J.; Ding D.; Sun Y.; Liu B.; Shi A.; Yan X.; Xu Q.; Hao J. | |
发表日期 | 2019 |
ISSN | 16807316 |
起始页码 | 6737 |
结束页码 | 6747 |
卷号 | 19期号:10 |
英文摘要 | Comprehensive chlorine heterogeneous chemistry is incorporated into the Community Multiscale Air Quality (CMAQ) model to evaluate the impact of chlorinerelated heterogeneous reaction on diurnal and nocturnal nitrate formation and quantify the nitrate formation from gasto-particle partitioning of HNO3 and from different heterogeneous pathways. The results show that these heterogeneous reactions increase the atmospheric Cl2 and ClNO2 level (∼ 100 %), which further affects the nitrate formation. Sensitivity analyses of uptake coefficients show that the empirical uptake coefficient for the O3 heterogeneous reaction with chlorinated particles may lead to the large uncertainties in the predicted Cl2 and nitrate concentrations. The N2O5 uptake coefficient with particulate Cl- concentration dependence performs better in capturing the concentration of ClNO2 and nocturnal nitrate concentration. The reaction of OH and NO2 in the daytime increases the nitrate by ∼ 15% when the heterogeneous chlorine chemistry is incorporated, resulting in more nitrate formation from HNO3 gas-to-particle partitioning. By contrast, the contribution of the heterogeneous reaction of N2O5 to nitrate concentrations decreases by about 27% in the nighttime, when its reactions with chlorinated particles are considered. However, the generated gas-phase ClNO2 from the heterogeneous reaction of N2O5 and chlorine-containing particles further reacts with the particle surface to increase the nitrate by 6 %. In general, this study highlights the potential of significant underestimation of daytime concentrations and overestimation of nighttime nitrate concentrations for chemical transport models without proper chlorine chemistry in the gas and particle phases. © Author(s) 2019. |
语种 | 英语 |
scopus关键词 | atmospheric chemistry; atmospheric transport; chlorine; concentration (composition); diurnal variation; heterogeneity; seasonal variation; sensitivity analysis; Beijing [Beijing (ADS)]; Beijing [China]; China |
来源期刊 | Atmospheric Chemistry and Physics |
文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/144394 |
作者单位 | State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing, 100084, China; State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, School of Environment, Tsinghua University, Beijing, 100084, China; Zachry Department of Civil Engineering, Texas A and M University, College Station, TX 77843-3138, United States; State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, 100029, China; Beijing Environmental Monitoring Center, Beijing, 100048, China; Beijing Municipal Research Institute of Environmental Protection, Beijing, 100037, China |
推荐引用方式 GB/T 7714 | Qiu X.,Ying Q.,Wang S.,et al. Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing; China[J],2019,19(10). |
APA | Qiu X..,Ying Q..,Wang S..,Duan L..,Zhao J..,...&Hao J..(2019).Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing; China.Atmospheric Chemistry and Physics,19(10). |
MLA | Qiu X.,et al."Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing; China".Atmospheric Chemistry and Physics 19.10(2019). |
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