Knowledge of particle number size distribution(PND) and new particle formation(NPF)events in Southern China is essential for mitigation strategies related to submicron particles and their effects on regional air q...Knowledge of particle number size distribution(PND) and new particle formation(NPF)events in Southern China is essential for mitigation strategies related to submicron particles and their effects on regional air quality,haze,and human health.In this study,seven field measurement campaigns were conducted from December 2013 to May 2015 using a scanning mobility particle sizer(SMPS) at four sites in Southern China,including three urban sites and one background site.Particles were measured in the size range of15-515 nm,and the median particle number concentrations(PNCs) were found to vary in the range of 0.3× 10~4-2.2 × 10~4 cn^(-3) at the urban sites and were approximately 0.2 × 10~4 cm^(-3) at the background site.The peak diameters at the different sites varied largely from 22 to 102 nm.The PNCs in the Aitken mode(25-100 nm) at the urban sites were up to 10 times higher than they were at the background site,indicating large primary emissions from traffic at the urban sites.The diurnal variations of PNCs were significantly influenced by both rush hour traffic at the urban sites and NPF events.The frequencies of NPF events at the different sites were0%-30%,with the highest frequency occurring at an urban site during autumn.With higher SO_2 concentrations and higher ambient temperatures being necessary,NPF at the urban site was found to be more influenced by atmospheric oxidizing capability,while NPF at the background site was limited by the condensation sink.This study provides a unique dataset of particle number and size information in various environments in Southern China,which can help understand the sources,formation,and the climate forcing of aerosols in this quickly developing region,as well as help constrain and validate NPF modeling.展开更多
Peroxyacetyl nitrate (PAN) is an important indicator of photochemical smog and has adverse effects on human health and vegetation growth. A rapid and h!ghly selective technique of thermal dissociation chemical ioniz...Peroxyacetyl nitrate (PAN) is an important indicator of photochemical smog and has adverse effects on human health and vegetation growth. A rapid and h!ghly selective technique of thermal dissociation chemical ionization mass spectrometry (TD-CIMS) was recently developed to measure the abundance of PAN in real time; however, it may be subject to artifact in the presence of nitric oxide (NO). In this study, we tested the interference of the PAN signal induced by NO, evaluated the performance of TD- CIMS in an urban environment, and investigated the concentration and formation of PAN in urban Hong Kong. NO caused a significant underestimation of the PAN signal in TD-CIMS, with the underestimation increasing sharply with NO concentration and decreasing slightly with PAN abundance. A formula was derived to link the loss of PAN signal with the concentrations of NO and PAN, which can be used for data correction in PAN measurements. The corrected PAN data from TD- CIMS were consistent with those from the commonly used gas chromatography with electron capture detection, which confirms the utility of TD-CIMS in an urban environment in which NO is abundant. In autumn of 2010, the hourly average PAN mixing ratio varied from 0.06 ppbv to 5.17 ppbv, indicating the occurrence of photochemical pollution in urban Hong Kong. The tbrmation efficiency of PAN during pollution episodes was as high as 3.9 to 5.9 ppbv per 100 ppbv ozone. The efficiency showed a near-linear increase with NO, concentration, suggesting a control policy of NO,. reduction for PAN pollution.展开更多
To better understand potential pollutant formations during combustion of conventional hydrocarbon fuels blended with oxygenated fuels, detailed influences of ethanol as fuel additive on small polycyclic aromatic hydro...To better understand potential pollutant formations during combustion of conventional hydrocarbon fuels blended with oxygenated fuels, detailed influences of ethanol as fuel additive on small polycyclic aromatic hydrocarbons(PAHs) precursors, aldehydes, ketene and other important intermediate species in premixed fuel-rich low-pressure ethylene flames are distinguished among dilution, thermal and chemical effects of additives. Dominant effects of ethanol addition on each species are underlined respectively. Ethylene oxidation process is delayed when ethylene is substituted by ethanol. The influence of ethanol dilution and thermal effects on ethylene consumption are larger than chemical effects. CO mole fractions slightly decrease mainly as a result of dilution and thermal effects of added ethanol. The reductions in small PAHs precursors(acetylene and propargyl) are attributed to dilution and thermal effects of ethanol addition instead of chemical effects. The ethanol chemical effects promote formations of hazardous pollutants formaldehyde and acetaldehyde, and especially are responsible for the significant increase of acetaldehyde. C2H6, C4H2 and C4H4 mole fractions decrease in a similar way with acetylene and propargyl as ethanol is added. Ethanol used here only serves as a prototype of oxygenated additive, and identification method in this work is more universal which can be easily extended for analyzing other fuel blends of hydrocarbon and oxygenated fuels.展开更多
基金supported by the National Natural Science Foundation of China(Nos.U1301234,21277003)the Shenzhen Science&Technology Plan,and the Ministry of Science and Technology of China(No.2013CB228503)
文摘Knowledge of particle number size distribution(PND) and new particle formation(NPF)events in Southern China is essential for mitigation strategies related to submicron particles and their effects on regional air quality,haze,and human health.In this study,seven field measurement campaigns were conducted from December 2013 to May 2015 using a scanning mobility particle sizer(SMPS) at four sites in Southern China,including three urban sites and one background site.Particles were measured in the size range of15-515 nm,and the median particle number concentrations(PNCs) were found to vary in the range of 0.3× 10~4-2.2 × 10~4 cn^(-3) at the urban sites and were approximately 0.2 × 10~4 cm^(-3) at the background site.The peak diameters at the different sites varied largely from 22 to 102 nm.The PNCs in the Aitken mode(25-100 nm) at the urban sites were up to 10 times higher than they were at the background site,indicating large primary emissions from traffic at the urban sites.The diurnal variations of PNCs were significantly influenced by both rush hour traffic at the urban sites and NPF events.The frequencies of NPF events at the different sites were0%-30%,with the highest frequency occurring at an urban site during autumn.With higher SO_2 concentrations and higher ambient temperatures being necessary,NPF at the urban site was found to be more influenced by atmospheric oxidizing capability,while NPF at the background site was limited by the condensation sink.This study provides a unique dataset of particle number and size information in various environments in Southern China,which can help understand the sources,formation,and the climate forcing of aerosols in this quickly developing region,as well as help constrain and validate NPF modeling.
基金This work was supported by the Environment and Conservation Fund of Hung Kong (Project No. 2009-07), National Natural Science Foundation of China (Grant Nos. 41275123, 21407094 and 91544213), China Postdoctoral Science Foundation (No. 2014M561932), and the Jiangsu Collaborative Innovation Center for Climate Change. The authors thank Dr. Pamela Holt for proofreading the manuscript.
文摘Peroxyacetyl nitrate (PAN) is an important indicator of photochemical smog and has adverse effects on human health and vegetation growth. A rapid and h!ghly selective technique of thermal dissociation chemical ionization mass spectrometry (TD-CIMS) was recently developed to measure the abundance of PAN in real time; however, it may be subject to artifact in the presence of nitric oxide (NO). In this study, we tested the interference of the PAN signal induced by NO, evaluated the performance of TD- CIMS in an urban environment, and investigated the concentration and formation of PAN in urban Hong Kong. NO caused a significant underestimation of the PAN signal in TD-CIMS, with the underestimation increasing sharply with NO concentration and decreasing slightly with PAN abundance. A formula was derived to link the loss of PAN signal with the concentrations of NO and PAN, which can be used for data correction in PAN measurements. The corrected PAN data from TD- CIMS were consistent with those from the commonly used gas chromatography with electron capture detection, which confirms the utility of TD-CIMS in an urban environment in which NO is abundant. In autumn of 2010, the hourly average PAN mixing ratio varied from 0.06 ppbv to 5.17 ppbv, indicating the occurrence of photochemical pollution in urban Hong Kong. The tbrmation efficiency of PAN during pollution episodes was as high as 3.9 to 5.9 ppbv per 100 ppbv ozone. The efficiency showed a near-linear increase with NO, concentration, suggesting a control policy of NO,. reduction for PAN pollution.
基金supported by the National Natural Science Foundation of China(Grant No.51306091)the Jiangsu Provincial Natural Science Foundation of China(Grant Nos.BK20140034,BK20130758)+1 种基金the Fundamental Research Funds for the Central Universities(Grant No.30920140111005)the Jiangsu Provincial Project of"Six Talent Summit"(Grant No.2014-XNY-002)
文摘To better understand potential pollutant formations during combustion of conventional hydrocarbon fuels blended with oxygenated fuels, detailed influences of ethanol as fuel additive on small polycyclic aromatic hydrocarbons(PAHs) precursors, aldehydes, ketene and other important intermediate species in premixed fuel-rich low-pressure ethylene flames are distinguished among dilution, thermal and chemical effects of additives. Dominant effects of ethanol addition on each species are underlined respectively. Ethylene oxidation process is delayed when ethylene is substituted by ethanol. The influence of ethanol dilution and thermal effects on ethylene consumption are larger than chemical effects. CO mole fractions slightly decrease mainly as a result of dilution and thermal effects of added ethanol. The reductions in small PAHs precursors(acetylene and propargyl) are attributed to dilution and thermal effects of ethanol addition instead of chemical effects. The ethanol chemical effects promote formations of hazardous pollutants formaldehyde and acetaldehyde, and especially are responsible for the significant increase of acetaldehyde. C2H6, C4H2 and C4H4 mole fractions decrease in a similar way with acetylene and propargyl as ethanol is added. Ethanol used here only serves as a prototype of oxygenated additive, and identification method in this work is more universal which can be easily extended for analyzing other fuel blends of hydrocarbon and oxygenated fuels.