The comparisons of observed and simulated NOx, CO, O3, NH3, HNO3, SO2 and PM2.5 indicate that CMAQ model can simulate variations of pollutants over North China well.Moreover, the model results show that high NH3 is in...The comparisons of observed and simulated NOx, CO, O3, NH3, HNO3, SO2 and PM2.5 indicate that CMAQ model can simulate variations of pollutants over North China well.Moreover, the model results show that high NH3 is in Hebei, Henan and Shandong provinces,with average concentration of (30-35)×10-9. The results of the sensitive experiment indicate that high concentration of NH3 has the efficiency of the production of secondary sulfate aerosol increase by more than 30%, especially at the juncture of Handan, Anyang and Changzhi that increased by 50%. In addition, NH3 also produces secondary ammonia and nitrate aerosol, and the sum of them is approximately equal to sulfate aerosol. The height of planetary boundary layer (PBL) in Beijing is higher in daytime, with average height of 1500 m at noon. This makes SO2,NH3 and HNO3 transported into upper PBL of 850 hPa. The high secondary sulfate, and ammonia and nitrate aerosol happen in the upper and lower PBL, respectively. Because PM2.5 lifetime is relatively long, it can be transported into the middle troposphere to form a thick aerosol layer,which is the arched roof of aerosol. The model result suggests that if the aerosol concentration in North China would be controlled, the reduction of NH3 emission is one of efficient ways besides the reduction of primary SO2, NOx and aerosol emission.展开更多
This paper explores the role of the secondary inorganic aerosol （SIA） species ammonium,NH4＋,nitrate,NO3-,and sulfate,SO24-,during haze and fog events using hourly mass concentrations of PM2.5 measured at a suburban...This paper explores the role of the secondary inorganic aerosol （SIA） species ammonium,NH4＋,nitrate,NO3-,and sulfate,SO24-,during haze and fog events using hourly mass concentrations of PM2.5 measured at a suburban site in Hangzhou,China.A total of 546 samples were collected between 1 April and 8 May 2012.The samples were analyzed and classified as clear,haze or fog depending on visibility and relative humidity （RH）.The contribution of SIA species to PM2.5 mass increased to ～50％ during haze and fog.The mass contribution of nitrate to PM2.5 increased from 11％ during clear to 20％ during haze episodes.Nitrate mass exceeded sulfate mass during haze,while near equal concentrations were observed during fog episodes.The role of RH on the correlation between concentrations of SIA and visibility was examined,with optimal correlation at 60％-70％ RH.The total acidity during clear,haze and fog periods was 42.38,48.38 and 45.51 nmol m-3,respectively,indicating that sulfate,nitrate and chloride were not neutralized by ammonium during any period.The nitrate to sulfate molar ratio,as a function of the ammonium to sulfate molar ratio,indicated that nitrate formation during fog started at a higher ammonium to sulfate molar ratio compared to clear and haze periods.During haze and fog,the nitrate oxidation ratio increased by a factor of 1.6-1.7,while the sulfur oxidation ratio increased by a factor of 1.2-1.5,indicating that both gaseous NO2 and SO2 were involved in the reduced visibility.展开更多
The extremely high concentrations of PM2.5(particulate matter with an aerodynamic meter≤2.5 mm)during severe and persistent haze events in China have been closely related to the formation of secondary aerosols(SA).Ne...The extremely high concentrations of PM2.5(particulate matter with an aerodynamic meter≤2.5 mm)during severe and persistent haze events in China have been closely related to the formation of secondary aerosols(SA).New particle formation(NPF)is the critical initial step of SA formation.New particles are commonly formed from gas-phase precursors(e.g.,SO2,volatile organic compounds)via nucleation and initial growth,in which molecular clusters with a mobility diameter smaller than 3 nm(hereafter referred to nanoscale molecular clusters)will be involved throughout the whole process.Recently,significant breakthroughs have been obtained on NPF studies,which are mostly attributed to the technical development in the real-time analysis of size-resolved number concentration and chemical composition of nanoscale molecular clusters.Regarding the detection of size-resolved number concentrations of nanoscale molecular clusters,both methods and instruments have been well built up;practical application in laboratory-scale experiments and field measurements have also been successfully demonstrated.In contrast,real-time analysis of chemical composition of nanoscale molecular clusters has still encountered the great challenges caused by the complex organic compositions of the clusters,and improvement of present analytical strategies is urgently required.The better understanding in NPF will not only benefit the atmospheric modeling and climate predictions but also the source control of SA.展开更多
文摘The comparisons of observed and simulated NOx, CO, O3, NH3, HNO3, SO2 and PM2.5 indicate that CMAQ model can simulate variations of pollutants over North China well.Moreover, the model results show that high NH3 is in Hebei, Henan and Shandong provinces,with average concentration of (30-35)×10-9. The results of the sensitive experiment indicate that high concentration of NH3 has the efficiency of the production of secondary sulfate aerosol increase by more than 30%, especially at the juncture of Handan, Anyang and Changzhi that increased by 50%. In addition, NH3 also produces secondary ammonia and nitrate aerosol, and the sum of them is approximately equal to sulfate aerosol. The height of planetary boundary layer (PBL) in Beijing is higher in daytime, with average height of 1500 m at noon. This makes SO2,NH3 and HNO3 transported into upper PBL of 850 hPa. The high secondary sulfate, and ammonia and nitrate aerosol happen in the upper and lower PBL, respectively. Because PM2.5 lifetime is relatively long, it can be transported into the middle troposphere to form a thick aerosol layer,which is the arched roof of aerosol. The model result suggests that if the aerosol concentration in North China would be controlled, the reduction of NH3 emission is one of efficient ways besides the reduction of primary SO2, NOx and aerosol emission.
基金supported by the National Natural Science Foundation of China (Grant Nos. 21190053 and 21177025)the Shanghai Science and Technology Commission of Shanghai Municipality (Grant Nos. 12DJ1400100 and 13XD 1400700)the Priority Fields for Ph.D. Programs Foundation of the Ministry of Education of China (Grant No.20110071130003)
文摘This paper explores the role of the secondary inorganic aerosol （SIA） species ammonium,NH4＋,nitrate,NO3-,and sulfate,SO24-,during haze and fog events using hourly mass concentrations of PM2.5 measured at a suburban site in Hangzhou,China.A total of 546 samples were collected between 1 April and 8 May 2012.The samples were analyzed and classified as clear,haze or fog depending on visibility and relative humidity （RH）.The contribution of SIA species to PM2.5 mass increased to ～50％ during haze and fog.The mass contribution of nitrate to PM2.5 increased from 11％ during clear to 20％ during haze episodes.Nitrate mass exceeded sulfate mass during haze,while near equal concentrations were observed during fog episodes.The role of RH on the correlation between concentrations of SIA and visibility was examined,with optimal correlation at 60％-70％ RH.The total acidity during clear,haze and fog periods was 42.38,48.38 and 45.51 nmol m-3,respectively,indicating that sulfate,nitrate and chloride were not neutralized by ammonium during any period.The nitrate to sulfate molar ratio,as a function of the ammonium to sulfate molar ratio,indicated that nitrate formation during fog started at a higher ammonium to sulfate molar ratio compared to clear and haze periods.During haze and fog,the nitrate oxidation ratio increased by a factor of 1.6-1.7,while the sulfur oxidation ratio increased by a factor of 1.2-1.5,indicating that both gaseous NO2 and SO2 were involved in the reduced visibility.
基金supported by the National Natural Science Foundation of China(No.21107066)National Instrumentation Program(No.2011YQ170067)Young Teachers Program of Universities in Shanghai(2012).
文摘The extremely high concentrations of PM2.5(particulate matter with an aerodynamic meter≤2.5 mm)during severe and persistent haze events in China have been closely related to the formation of secondary aerosols(SA).New particle formation(NPF)is the critical initial step of SA formation.New particles are commonly formed from gas-phase precursors(e.g.,SO2,volatile organic compounds)via nucleation and initial growth,in which molecular clusters with a mobility diameter smaller than 3 nm(hereafter referred to nanoscale molecular clusters)will be involved throughout the whole process.Recently,significant breakthroughs have been obtained on NPF studies,which are mostly attributed to the technical development in the real-time analysis of size-resolved number concentration and chemical composition of nanoscale molecular clusters.Regarding the detection of size-resolved number concentrations of nanoscale molecular clusters,both methods and instruments have been well built up;practical application in laboratory-scale experiments and field measurements have also been successfully demonstrated.In contrast,real-time analysis of chemical composition of nanoscale molecular clusters has still encountered the great challenges caused by the complex organic compositions of the clusters,and improvement of present analytical strategies is urgently required.The better understanding in NPF will not only benefit the atmospheric modeling and climate predictions but also the source control of SA.
