B. Wehner

Rapid aerosol particle growth and increase of cloud condensation nucleus activity by secondary aerosol formation and condensation: A case study for regional air pollution in northeastern China

[1] This study was part of the international field measurement Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing-2006). We investigated a new particle formation event in a highly polluted air mass at a regional site south of the megacity Beijing and its impact on the abundance and properties of cloud condensation nuclei (CCN). During the 1-month observation, particle nucleation followed by significant particle growth on a regional scale was observed frequently (~30%), and we chose 23 August 2006 as a representative case study. Secondary aerosol mass was produced continuously, with sulfate, ammonium, and organics as major components. The aerosol mass growth rate was on average 19 μg m -3 h -1 during the late hours of the day. This growth rate was observed several times during the 1-month intensive measurements. The nucleation mode grew very quickly into the size range of CCN, and the CCN size distribution was dominated by the growing nucleation mode (up to 80% of the total CCN number concentration) and not as usual by the accumulation mode. At water vapor supersaturations of 0.07-0.86%, the CCN number concentrations reached maximum values of 4000-19,000 cm -3 only 6-14 h after the nucleation event. During particle formation and growth, the effective hygroscopicity parameter κ increased from about 0.1-0.3 to 0.35-0.5 for particles with diameters of 40-90 nm, but it remained nearly constant at ~0.45 for particles with diameters of ~190 nm. This result is consistent with aerosol chemical composition data, showing a pronounced increase of sulfate.

Particle number size distributions in a street canyon and their transformation into the urban-air background: measurements and a simple model study

Abstract Car traffic is one of the main anthropogenic aerosol sources in modern cities. The characterization of these emissions is important for describing the quality of urban air. Measurements in a street canyon in a German urban area were made. Maximum number concentrations occurred during morning hours from Monday to Friday when the traffic density is highest. The maximum of the number size distribution measured during rush hour near a busy city street was at a particle diameter of 15 nm . This differs significantly from size distributions directly measured in vehicle exhaust (vehicles placed on chassis dynamometers used for vehicle emissions certification), typically about 50 nm . The size distributions measured in the urban area depended on the distance to the nearest road. With increasing distance, the maximum of the size distribution increased, and the total number concentration decreased. This seems to be a result of particle growth due to processes such as coagulation and condensation, and dilution with the surrounding air. To clarify the transformation of the particle number size distributions measured in a street canyon into the urban-air background, a sectional aerosol model was used to calculate the evolution of the number size distribution, and included the effect of condensation, coagulation, dilution, and continuous entrainment of freshly emitted particles yielding good agreement with measurements.

The effect of particle size on cardiovascular disorders — The smaller the worse

BACKGROUND Previous studies observed associations between airborne particles and cardio-vascular disease. Questions, however, remain as to which size of the inhalable particles (coarse, fine, or ultrafine) exerts the most significant impact on health. METHODS For this retrospective study, data of the total number of 23,741 emergency service calls, registered between February 2002 and January 2003 in the City of Leipzig, were analysed, identifying 5326 as being related to cardiovascular incidences. Simultaneous particle exposure was determined for the particle sizes classes <100 nm (UFP), <2.5 μm (PM2.5) and <10 μm (PM10). We used a time resolution of 1 day for both parameters, emergency calls and exposure. RESULTS Within the group of cardiovascular diseases, the diagnostic category of hypertensive crisis showed a significant association with particle exposure. The significant effect on hypertensive crisis was found for particles with a size of <100 nm in diameter and starting with a lag of 2 days after exposure. No consistent influence could be observed for PM2.5 and PM10. The Odds Ratios on hypertensive crisis were significant for the particle size <100 nm in diameter from day 2 post exposure OR=1.06 (95%CI: 1.02-1.10, p=0.002) up to day 7 OR=1.05 (95%CI 1.02-1.09, p=0.005). CONCLUSION Ultrafine particles affect cardiovascular disease adversely, particularly hypertensive crises. Their effect is significant compared with PM2.5 and PM10. It appears necessary, from a public health point of view, to consider regulating this type of particles using appropriate measurands as particle number.

The contribution of sulfuric acid and non‐volatile compounds on the growth of freshly formed atmospheric aerosols

[1] The formation of atmospheric aerosol particles (homogeneous nucleation, forming of stable clusters ∼1 nm in size), their subsequent growth to detectable sizes (>3 nm), and to the size of cloud condensation nuclei, remains one of the least understood atmospheric processes upon which global climate change critically depends. However, a quantitative model explanation for the growth of freshly formed aerosols has been missing. In this study, we present observations explaining the nucleation mode (3-25 nm) growth. Aerosol particles typically grow from 3 nm to 60-70 nm during a day, while their non-volatile cores grow by 10-20 nm as well. The total particle growth rate is 2-8 nm/h while the non-volatile core material can explain 20-40%. According to our results, sulfuric acid can explain the remainder of the growth, until the particle diameter is around 10-20 nm. After that secondary organic compounds significantly take part in growth process.

Variability of the aerosol number size distribution in Beijing, China: New particle formation, dust storms, and high continental background

Continuous measurements of aerosol number size distributions from 3 nm to 10 μm have been first performed within the city area of Beijing since March 2004. Size distributions of the first 45 measurement days (March 05 to April 18, 2004) were investigated in terms of their high variability. Two dust storm events were observed indicated by high number concentrations greater than 1 μm and mass concentrations around 1 mg m -3 . Continental highly polluted air was observed during 12 days indicated by a number peak in the accumulation mode range, and submicrometer volume concentrations above 150 μm 3 cm -3 were observed. Newly formed particles with more than 100,000 cm -3 were observed on 25 days when the particle surface area concentration drops below a critical value (100-2000 μm 2 cm -3 ) because of clean air from the north. Measurements show only a slight growth (∼1 nm h -1 ) of the particles indicating that they are produced within the city area of Beijing.

Design and calibration of a thermodenuder with an improved heating unit to measure the size-dependent volatile fraction of aerosol particles

Separated measurements of volatile and non-volatile fractions of atmospheric aerosols have become more important due to possible effects of non-volatile particle on respiratory diseases. Measurements of non-volatile particle fractions with considerable size and time resolution are therefore needed. The combination of a thermodenuder (TD) with aerosol size spectrometers can provide size distributions of non-volatile particles. TDs usually consist of two units: a heating and a cooling tube. Unfortunately, available TDs have some disadvantages concerning the heated tube, where volatile material should be desorbed from the particles. The residence time in the heating zone might be too short to completely evaporate the volatile material or the temperature at the exit of the heating tube might be below the condensation temperature of the evaporated species. Here, a new TD was developed with a longer residence time at the requested temperature and a more effective insulation to prevent recondensation at the end of the heating unit. Additionally, the TD was calibrated for size-dependent particle losses at different heater temperatures.

Sub-micrometer particulate air pollution and cardiovascular mortality in Beijing, China

BACKGROUND While the link between particulate matter and cardiovascular mortality is well established, it is not fully investigated and understood which properties of the aerosol might be responsible for the health effects, especially in polluted mega-city areas. OBJECTIVES Our goal was to explore the association between daily cardiovascular mortality and different particle metrics in the sub-micrometer range in Beijing, China. METHODS We obtained daily counts of cause-specific cardiovascular deaths in the Beijing urban area for the period March 2004 to August 2005. Concurrently, continuous measurements of particle number size distributions were performed. Particle number concentrations (NC) between 0.003 μm and 0.8 μm were converted to particle mass and surface area concentrations assuming spherical particles. Semi-parametric Poisson regression models adjusting for trend, seasonality, day of the week, and meteorology were used to estimate immediate, delayed and cumulative particle effects. Additionally, effect modification by air mass origin was investigated. RESULTS We observed associations between daily cardiovascular mortality and particle NC for a 2-days delay. Moreover, nearly all particle metrics showed 2-days delayed associations with ischemic heart disease mortality. The strongest association was found for particle NC in the size range 0.03-0.1 μm (7.1% increase in daily mortality with a 95%-confidence interval of 2.9%-11.5%, per an increase of 6250 particles/cm3). Results for surface and mass concentrations with a lag of two days indicated effect modification by air mass origin, whereas effects of particle NC were not modified. CONCLUSIONS Results show an elevated risk of cardiovascular mortality in Beijing from short-term exposure to particulate air pollution in the sub-micrometer range. Results also indicate that locally produced smaller particles and regionally transported particles may exhibit different effects in Beijing.

Size-Segregated Particle Number Concentrations and Respiratory Emergency Room Visits in Beijing, China

Background The link between concentrations of particulate matter (PM) and respiratory morbidity has been investigated in numerous studies. Objectives The aim of this study was to analyze the role of different particle size fractions with respect to respiratory health in Beijing, China. Methods Data on particle size distributions from 3 nm to 1 μm; PM10 (PM ≤ 10 μm), nitrogen dioxide (NO2), and sulfur dioxide concentrations; and meteorologic variables were collected daily from March 2004 to December 2006. Concurrently, daily counts of emergency room visits (ERV) for respiratory diseases were obtained from the Peking University Third Hospital. We estimated pollutant effects in single- and two-pollutant generalized additive models, controlling for meteorologic and other time-varying covariates. Time-delayed associations were estimated using polynomial distributed lag, cumulative effects, and single lag models. Results Associations of respiratory ERV with NO2 concentrations and 100–1,000 nm particle number or surface area concentrations were of similar magnitude—that is, approximately 5% increase in respiratory ERV with an interquartile range increase in air pollution concentration. In general, particles < 50 nm were not positively associated with ERV, whereas particles 50–100 nm were adversely associated with respiratory ERV, both being fractions of ultrafine particles. Effect estimates from two-pollutant models were most consistent for NO2. Conclusions Present levels of air pollution in Beijing were adversely associated with respiratory ERV. NO2 concentrations seemed to be a better surrogate for evaluating overall respiratory health effects of ambient air pollution than PM10 or particle number concentrations in Beijing.

Size-fractioned particulate air pollution and cardiovascular emergency room visits in Beijing, China.

BACKGROUND Although short-term exposure to ambient particulate matter has increasingly been linked with cardiovascular diseases, it is not quite clear how physical characteristics of particles, such as particle size may be responsible for the association. This study aimed at investigating whether daily changes in number or mass concentrations of accurately size-segregated particles in the range of 3nm-10μm are associated with daily cardiovascular emergency room visits in Beijing, China. METHODS Cardiovascular emergency room visit counts, particle size distribution data, and meteorological data were collected from Mar. 2004 to Dec. 2006. Particle size distribution data was used to calculate particle number concentration in different size fractions, which were then converted to particle mass concentration assuming spherical particles. We applied a time-series analysis approach. We evaluated lagged associations between cardiovascular emergency room visits and particulate number and mass concentration using distributed lag non-linear models up to lag 10. We calculated percentage changes of cardiovascular emergency room visits, together with 95% confidence intervals (CI), in association with an interquartile range (IQR, difference between the third and first quartile) increase of 11-day or 2-day moving average number or mass concentration of particulate matter within each size fraction, assuming linear effects. We put interaction terms between season and 11-day or 2-day average particulate concentration in the models to estimate the modification of the particle effects by season. RESULTS We observed delayed associations between number concentration of ultrafine particles and cardiovascular emergency room visits, mainly from lag 4 to lag 10, mostly contributed by 10-30nm and 30-50nm particles. An IQR (9040cm(-3)) increase in 11-day average number concentration of ultrafine particles was associated with a 7.2% (1.1-13.7%) increase in total, and a 7.9% (0.5-15.9%) increase in severe cardiovascular emergency room visits. The delayed effects of particulate mass concentration were small. Regarding immediate effects, 2-day average number concentration of Aitken mode (30-100nm) particles had strongest effects. An IQR (2269cm(-3)) increase in 2-day average number concentration of 30-50nm particles led to a 2.4% (-1.5-6.5%) increase in total, and a 1.7% (-2.9-6.5%) increase in severe cardiovascular emergency room visits. The immediate effects of mass concentration came mainly from 1000-2500nm particles. An IQR (11.7μgm(-3)) increase in 2-day average mass concentration of 1000-2500nm particles led to an around 2.4% (0.4-4.4%) increase in total, and a 1.7% (-0.8-4.2%) increase in severe cardiovascular emergency room visits. The lagged effect curves of number and mass concentrations of 100-300nm particles or 300-1000nm particles were quite similar, indicating that using particulate number or mass concentrations seemed not to affect the cardiovascular effect (of particles within one size fraction). The effects of number concentration of ultrafine particles, sub-micrometer particles (3-1000nm) and 10-30nm particles were substantially higher in winter comparing with in summer. CONCLUSIONS Elevated concentration levels of sub-micrometer particles were associated with increased cardiovascular morbidity. Ultrafine particles showed delayed effects, while accumulation mode (100-1000nm) particles showed immediate effects. Using number or mass concentrations did not affect the particle effects.

SUBMICROMETER AEROSOL SIZE DISTRIBUTIONS AND MASS CONCENTRATION OF THE MILLENNIUM FIREWORKS 2000 IN lEIPZIG, GERMANY

In this technical note, we present submicrometer aerosol number and volume size distribution as well as mass concentration during the Millennium fireworks measured at the Institute of Tropospheric Research (IfT) in Leipzig and their correlation with simultaneous measurements.