Concentration and source rate of precursor vapors participating in particle formation and subsequent growth were investigated during the Pearl River Delta intensive campaign (PRD2004, October 2004) in southeastern C...Concentration and source rate of precursor vapors participating in particle formation and subsequent growth were investigated during the Pearl River Delta intensive campaign (PRD2004, October 2004) in southeastern China. Four new particle formation event days and a typical non-event day were selected for our analysis. Atmospheric sulphuric acid, the important precursor vapor in nucleation and growth, were simulated with a pseudo steady-state model based on the measurements of SO2, NOx, 03, CO, non-methane hydrocarbon (NMHC) and ambient particle number concentrations as well as modeled photolysis frequencies obtained from measurements. The maximum midday sulphuric acid concentrations vary from 4.53 × 10^7 to 2.17 × 10^8 molecules cm^-3, the corresponding source rate via reaction of OH and SO2 range between 2.37 × 10^6 and 1.16 × 10^7 molecules cm^-3 s^-1. Nucleation mode growth rate was derived from size spectral evolution during the events to be 6.8-13.8 nm h^-1. Based on the growth rate, concentration of the vapors participating in subsequent growth were estimated to vary from 1.32 × 10^8 to 2.80 × 10^8 molecules cm^-3 with corresponding source rate between 7.26 × 10^6 and 1.64 × 10^7 molecules cm^-3 s^-1. Our results show the degree of pollution is larger in PRD. Sulphuric acid concentrations are fairly high and have a close correlation with new particle formation events. Budget analysis shows that sulphuric acid alone is not enough for required growth; other nonvolatile vapors are needed. However, sulphuric acid plays an important role in growth; the contribution of sulphuric acid to growth in PRD is 12.4%-65.2%.展开更多
This study discusses the evolution of particle number size distribution during episodes of heavy pollution and new particle formation in the urban atmosphere of Beijing to quantify the effects of dynamic processes (co...This study discusses the evolution of particle number size distribution during episodes of heavy pollution and new particle formation in the urban atmosphere of Beijing to quantify the effects of dynamic processes (coagulation and condensation) on the particle number size distribution.During a heavy-pollution event,an extremely low number concentration of 3-10 nm particles (on average 46 cm-3) was observed.This is because nucleation-mode particles were easily removed by strong coagulational scavenging of larger particles under this condition.In addition,a large condensation sink (on average 0.13 s-1) restrained nucleation,which is one of the major sources of nucleation-mode particles.Conversely,during a new-particle formation event,the small condensation sink (0.01 s-1) of precursor facilitated nucleation.At the same time,preexisting particles had little ability to scavenge newly formed particles (around 1 nm) and allowed them to grow to a detectable size (larger than 3 nm currently).We suggest that the effects of dynamic processes (coagulation and condensation) on particle size distribution should be stressed under some extreme conditions of the relatively polluted urban atmosphere in addition to traffic and meteorological factors.展开更多
Formation of new atmospheric aerosol particles is a global phenomenon that has been observed to take place in even heavily-polluted environments. However, in all environments there appears to be a threshold value of t...Formation of new atmospheric aerosol particles is a global phenomenon that has been observed to take place in even heavily-polluted environments. However, in all environments there appears to be a threshold value of the condensation sink (due to pre-existing aerosol particles) after which the formation rate of 3 nm particles is no longer detected. In China new particle production has been observed at very high pollution levels (condensation sink about 0.1 s-1 ) m several megaclt es, including Beijing, Shanghai and Nanjing as well as in Pearl River Delta (PRD). Here we summarize the recent findings obtained from these studies and discuss the various implications these findings will have on future research and policy.展开更多
New particle formation is a key process in shaping the size distribution of aerosols in the atmosphere.We present here the measurement results of number and size distribution of aerosol particles (10–10000 nm in dia...New particle formation is a key process in shaping the size distribution of aerosols in the atmosphere.We present here the measurement results of number and size distribution of aerosol particles (10–10000 nm in diameter) obtained in the summer of 2008,at a suburban site in Beijing,China.We firstly reported the pollution level,particle number size distribution,diurnal variation of the particle number size distribution and then introduced the characteristics of the particle formation processes.The results showed that the number concentration of ultrafine particles was much lower than the values measured in other urban or suburban areas in previous studies.Sharp increases of ultrafine particle count were frequently observed at noon.An examination of the diurnal pattern suggested that the burst of ultrafine particles was mainly due to new particle formation promoted by photochemical processes.In addition,high relative humidity was a key factor driving the growth of the particles in the afternoon.During the 2-month observations,new particle formation from homogeneous nucleation was observed for 42.7% of the study period.The average growth rate of newly formed particles was 3.2 nm/hr,and varied from 1.2 to 8.0 nm/hr.The required concentration of condensable vapor was 4.4×10 7 cm-3,and its source rate was 1.2×10 6 cm-3 sec-1.Further calculation on the source rate of sulphuric acid vapor indicated that the average participation of sulphuric acid to particle growth rates was 28.7%.展开更多
基金China National Basic Research and Development Program (Grant Nos. 2002CB410801, 2002CB211605) National Natural Science Foundation of China (Grant No. 40405025).
文摘Concentration and source rate of precursor vapors participating in particle formation and subsequent growth were investigated during the Pearl River Delta intensive campaign (PRD2004, October 2004) in southeastern China. Four new particle formation event days and a typical non-event day were selected for our analysis. Atmospheric sulphuric acid, the important precursor vapor in nucleation and growth, were simulated with a pseudo steady-state model based on the measurements of SO2, NOx, 03, CO, non-methane hydrocarbon (NMHC) and ambient particle number concentrations as well as modeled photolysis frequencies obtained from measurements. The maximum midday sulphuric acid concentrations vary from 4.53 × 10^7 to 2.17 × 10^8 molecules cm^-3, the corresponding source rate via reaction of OH and SO2 range between 2.37 × 10^6 and 1.16 × 10^7 molecules cm^-3 s^-1. Nucleation mode growth rate was derived from size spectral evolution during the events to be 6.8-13.8 nm h^-1. Based on the growth rate, concentration of the vapors participating in subsequent growth were estimated to vary from 1.32 × 10^8 to 2.80 × 10^8 molecules cm^-3 with corresponding source rate between 7.26 × 10^6 and 1.64 × 10^7 molecules cm^-3 s^-1. Our results show the degree of pollution is larger in PRD. Sulphuric acid concentrations are fairly high and have a close correlation with new particle formation events. Budget analysis shows that sulphuric acid alone is not enough for required growth; other nonvolatile vapors are needed. However, sulphuric acid plays an important role in growth; the contribution of sulphuric acid to growth in PRD is 12.4%-65.2%.
基金supported by National Natural Science Foundation of China (Grant No. 20977001,21025728)
文摘This study discusses the evolution of particle number size distribution during episodes of heavy pollution and new particle formation in the urban atmosphere of Beijing to quantify the effects of dynamic processes (coagulation and condensation) on the particle number size distribution.During a heavy-pollution event,an extremely low number concentration of 3-10 nm particles (on average 46 cm-3) was observed.This is because nucleation-mode particles were easily removed by strong coagulational scavenging of larger particles under this condition.In addition,a large condensation sink (on average 0.13 s-1) restrained nucleation,which is one of the major sources of nucleation-mode particles.Conversely,during a new-particle formation event,the small condensation sink (0.01 s-1) of precursor facilitated nucleation.At the same time,preexisting particles had little ability to scavenge newly formed particles (around 1 nm) and allowed them to grow to a detectable size (larger than 3 nm currently).We suggest that the effects of dynamic processes (coagulation and condensation) on particle size distribution should be stressed under some extreme conditions of the relatively polluted urban atmosphere in addition to traffic and meteorological factors.
基金The work in this manuscript is supported by Academy of Finland via Center of Excellence in Atmospheric Sciences (Project No. 272041) and the Finnish Funding Agency for Technology and Innovation TEKES via Beautiful Beijing project (No. 3667/31/2013) and European Research Council Advanced Grant (ATMNUCLE, 227463) and InGOS DEFROST and CRAICC (No. 26060) and Nordforsk CRAICC-PEEX (amendment to contact 26060) funded by Nordforsk. The SORPES station was supported by Nanjing University and the Collaborative Innovation Center of Climate Change in Jiangsu Province, China. Part of Aijun Ding's work was supported by the excellent young scientist fund of National Natural Science Foundation of China (No. D0512/41422504).
文摘Formation of new atmospheric aerosol particles is a global phenomenon that has been observed to take place in even heavily-polluted environments. However, in all environments there appears to be a threshold value of the condensation sink (due to pre-existing aerosol particles) after which the formation rate of 3 nm particles is no longer detected. In China new particle production has been observed at very high pollution levels (condensation sink about 0.1 s-1 ) m several megaclt es, including Beijing, Shanghai and Nanjing as well as in Pearl River Delta (PRD). Here we summarize the recent findings obtained from these studies and discuss the various implications these findings will have on future research and policy.
基金supported by the National Department Public Benefit Research Foundation of China (No.201009001)the National Natural Science Foundation of China (No.41005065)the Basic Foundation for Public Benefit-Research Academies from the Central Government (No.2008KYYW01)
文摘New particle formation is a key process in shaping the size distribution of aerosols in the atmosphere.We present here the measurement results of number and size distribution of aerosol particles (10–10000 nm in diameter) obtained in the summer of 2008,at a suburban site in Beijing,China.We firstly reported the pollution level,particle number size distribution,diurnal variation of the particle number size distribution and then introduced the characteristics of the particle formation processes.The results showed that the number concentration of ultrafine particles was much lower than the values measured in other urban or suburban areas in previous studies.Sharp increases of ultrafine particle count were frequently observed at noon.An examination of the diurnal pattern suggested that the burst of ultrafine particles was mainly due to new particle formation promoted by photochemical processes.In addition,high relative humidity was a key factor driving the growth of the particles in the afternoon.During the 2-month observations,new particle formation from homogeneous nucleation was observed for 42.7% of the study period.The average growth rate of newly formed particles was 3.2 nm/hr,and varied from 1.2 to 8.0 nm/hr.The required concentration of condensable vapor was 4.4×10 7 cm-3,and its source rate was 1.2×10 6 cm-3 sec-1.Further calculation on the source rate of sulphuric acid vapor indicated that the average participation of sulphuric acid to particle growth rates was 28.7%.