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- ItemEvaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case(München : European Geopyhsical Union, 2011) Wang, Z.B.; Hu, M.; Yue, D.L.; Zheng, J.; Zhang, R.Y.; Wiedensohler, A.; Wu, Z.J.; Nieminen, T.; Boy, M.New particle formation (NPF) is considered as an important mechanism for gas-to-particle transformation, and gaseous sulfuric acid is believed as a crucial precursor. Up to now few field-based studies on nucleation mechanisms and the role of sulfuric acid were conducted in China. In this study, simultaneously measurements of particle number size distributions and gaseous sulfuric acid concentrations were performed from July to September in 2008. Totally, 22 new particle formation events were observed during the entire 85 campaign days. The results show that in the case of both higher source and sink values, the result of the competition between source and sink is more likely the key limiting factor to determine the observation of NPF events in Beijing. The concentrations of gaseous sulfuric acid show good correlations with freshly nucleated particles (N3-6 and formation rates (J3 and J1.5. The power-law relationship between H2SO4 concentration and N3-6 or J is adopted to explore the nucleation mechanism. The exponents are showed a great range (from 1 to 7). More than half of the NPF events exhibit an exponent larger than 2.5. For these cases, the thermodynamic process works better than the activation or kinetic nucleation theories to explain the nucleation events in urban atmosphere of Beijing.
- ItemChemical mass balance of 300 °c non-volatile particles at the tropospheric research site Melpitz, Germany(München : European Geopyhsical Union, 2014) Poulain, L.; Birmili, W.; Canonaco, F.; Crippa, M.; Wu, Z.J.; Nordmann, S.; Wiedensohler, A.; Held, A.; Spindler, G.; Prévôt, A.S.H.; Wiedensohler, A.; Herrmann, H.In the fine-particle mode (aerodynamic diameter < 1 μm) non-volatile material has been associated with black carbon (BC) and low-volatile organics and, to a lesser extent, with sea salt and mineral dust. This work analyzes non-volatile particles at the tropospheric research station Melpitz (Germany), combining experimental methods such as a mobility particle-size spectrometer (3–800 nm), a thermodenuder operating at 300 °C, a multi-angle absorption photometer (MAAP), and an aerosol mass spectrometer (AMS). The data were collected during two atmospheric field experiments in May–June 2008 as well as February–March 2009. As a basic result, we detected average non-volatile particle–volume fractions of 11 ± 3% (2008) and 17 ± 8% (2009). In both periods, BC was in close linear correlation with the non-volatile fraction, but not sufficient to quantitatively explain the non-volatile particle mass concentration. Based on the assumption that BC is not altered by the heating process, the non-volatile particle mass fraction could be explained by the sum of black carbon (47% in summer, 59% in winter) and a non-volatile organic contribution estimated as part of the low-volatility oxygenated organic aerosol (LV-OOA) (53% in summer, 41% in winter); the latter was identified from AMS data by factor analysis. Our results suggest that LV-OOA was more volatile in summer (May–June 2008) than in winter (February–March 2009) which was linked to a difference in oxidation levels (lower in summer). Although carbonaceous compounds dominated the sub-μm non-volatile particle mass fraction most of the time, a cross-sensitivity to partially volatile aerosol particles of maritime origin could be seen. These marine particles could be distinguished, however from the carbonaceous particles by a characteristic particle volume–size distribution. The paper discusses the uncertainty of the volatility measurements and outlines the possible merits of volatility analysis as part of continuous atmospheric aerosol measurements.
- ItemCharacteristics of regional new particle formation in urban and regional background environments in the North China Plain(München : European Geopyhsical Union, 2013) Wang, Z.B.; Hu, M.; Sun, J.Y.; Wu, Z.J.; Yue, D.L.; Shen, X.J.; Zhang, Y.M.; Pei, X.Y.; Cheng, Y.F.; Wiedensohler, A.Long-term measurements of particle number size distributions were carried out both at an urban background site (Peking University, PKU) and a regional Global Atmospheric Watch station (Shangdianzi, SDZ) from March to November in 2008. In total, 52 new particle formation (NPF) events were observed simultaneously at both sites, indicating that this is a regional phenomenon in the North China Plain. On average, the mean condensation sink value before the nucleation events started was 0.025 s−1 in the urban environment, which was 1.6 times higher than that at regional site. However, higher particle formation and growth rates were observed at PKU (10.8 cm−3 s−1 and 5.2 nm h−1) compared with those at SDZ (4.9 cm−3 s−1 and 4.0 nm h−1). These results implied that precursors were much more abundant in the polluted urban environment. Different from the observations in cleaner environments, the background conditions of the observed particle homogeneous nucleation events in the North China Plain could be characterized as the co-existing of a stronger source of precursor gases and a higher condensational sink of pre-existing aerosol particles. Secondary aerosol formation following nucleation events results in an increase of particle mass concentration, particle light scattering coefficient, and cloud condensation nuclei (CCN) number concentration, with consequences on visibility, radiative effects, and air quality. Typical regional NPF events with significant particle nucleation rates and subsequent particle growth over a sufficiently long time period at both sites were chosen to investigate the influence of NPF on the number concentration of "potential" CCN. As a result, the NPF and the subsequent condensable growth increased the CCN number concentration in the North China Plain by factors in the range from 5.6 to 8.7. Moreover, the potential contribution of anthropogenic emissions to the CCN number concentration was more than 50%, to which more attention should be drawn in regional and global climate modeling, especially in the polluted urban areas.
- ItemLong-term measurements of particle number size distributions and the relationships with air mass history and source apportionment in the summer of Beijing(München : European Geopyhsical Union, 2013) Wang, Z.B.; Hu, M.; Wu, Z.J.; Yue, D.L.; He, L.Y.; Huang, X.F.; Liu, X.G.; Wiedensohler, A.A series of long-term and temporary measurements were conducted to study the improvement of air quality in Beijing during the Olympic Games period (8–24 August 2008). To evaluate actions taken to improve the air quality, comparisons of particle number and volume size distributions of August 2008 and 2004–2007 were performed. The total particle number and volume concentrations were 14 000 cm−3 and 37 μm−3 cm−3 in August of 2008, respectively. These were reductions of 41% and 35% compared with mean values of August 2004–2007. A cluster analysis on air mass history and source apportionment were performed, exploring reasons for the reduction of particle concentrations. Back trajectories were classified into five major clusters. Air masses from the south direction are always associated with pollution events during the summertime in Beijing. In August 2008, the frequency of air mass arriving from the south was 1.3 times higher compared to the average of the previous years, which however did not result in elevated particle volume concentrations in Beijing. Therefore, the reduced particle number and volume concentrations during the 2008 Beijing Olympic Games cannot be only explained by meteorological conditions. Four factors were found influencing particle concentrations using a positive matrix factorization (PMF) model. They were identified as local and remote traffic emissions, combustion sources as well as secondary transformation. The reductions of the four sources were calculated to 47%, 44%, 43% and 30%, respectively. The significant reductions of particle number and volume concentrations may attribute to actions taken, focusing on primary emissions, especially related to the traffic and combustion sources.
- ItemHygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their influence on the water uptake of ammonium sulfate(München : European Geopyhsical Union, 2011) Wu, Z.J.; Nowak, A.; Poulain, L.; Herrmann, H.; Wiedensohler, A.The hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their effects on ammonium sulfate were investigated using a hygroscopicity tandem differential mobility analyzer (H-TDMA). No hygroscopic growth is observed for disodium oxalate, while ammonium oxalate shows slight growth (growth factor = 1.05 at 90%). The growth factors at 90% RH for sodium acetate, disodium malonate, disodium succinate, disodium tartrate, diammonium tartrate, sodium pyruvate, disodium maleate, and humic acid sodium salt are 1.79, 1.78, 1.69, 1.54, 1.29, 1.70, 1.78, and 1.19, respectively. The hygroscopic growth of mixtures of organic salts with ammonium sulfate, which are prepared as surrogates of atmospheric aerosols, was determined. A clear shift in deliquescence relative humidity to lower RH with increasing organic mass fraction was observed for these mixtures. Above 80% RH, the contribution to water uptake by the organic salts was close to that of ammonium sulfate for the majority of investigated compounds. The observed hygroscopic growth of the mixed particles at RH above the deliquescence relative humidity of ammonium sulfate agreed well with that predicted using the Zdanovskii-Stokes-Robinson (ZSR) mixing rule. Mixtures of ammonium sulfate with organic salts are more hygroscopic than mixtures with organic acids, indicating that neutralization by gas-phase ammonia and/or association with cations of dicarbonxylic acids may enhance the hygroscopicity of the atmospheric particles.
- ItemThe roles of sulfuric acid in new particle formation and growth in the mega-city of Beijing(München : European Geopyhsical Union, 2010) Yue, D.L.; Hu, M.; Zhang, R.Y.; Wang, Z.B.; Zheng, J.; Wu, Z.J.; Wiedensohler, A.; He, L.Y.; Huang, X.F.; Zhu, T.Simultaneous measurements of gaseous sulfuric acid and particle number size distributions were performed to investigate aerosol nucleation and growth during CAREBeijing-2008. The analysis of the measured aerosols and sulfuric acid with an aerosol dynamic model shows the dominant role of sulfuric acid in new particle formation (NPF) process but also in the subsequent growth in Beijing. Based on the data of twelve NPF events, the average formation rates (2–13 cm−3 s−1) show a linear correlation with the sulfuric acid concentrations (R2=0.85). Coagulation seems to play a significant role in reducing the number concentration of nucleation mode particles with the ratio of the coagulation loss to formation rate being 0.41±0.16. The apparent growth rates vary from 3 to 11 nm h−1. Condensation of sulfuric acid and its subsequent neutralization by ammonia and coagulation contribute to the apparent particle growth on average 45±18% and 34±17%, respectively. The 30% higher concentration of sulfate than organic compounds in particles during the seven sulfur-rich NPF events but 20% lower concentration of sulfate during the five sulfur-poor type suggest that organic compounds are an important contributor to the growth of the freshly nucleated particles, especially during the sulfur-poor cases.
- ItemVariation of particle number size distributions and chemical compositions at the urban and downwind regional sites in the Pearl River Delta during summertime pollution episodes(München : European Geopyhsical Union, 2010) Yue, D.L.; Hu, M.; Wu, Z.J.; Guo, S.; Wen, M.T.; Nowak, A.; Wehner, B.; Wiedensohler, A.; Takegawa, N.; Kondo, Y.; Wang, X.S.; Li, Y.P.; Zeng, L.M.; Zhang, Y.H.In order to characterize the features of particulate pollution in the Pearl River Delta (PRD) in the summer, continuous measurements of particle number size distributions and chemical compositions were simultaneously performed at Guangzhou urban site (GZ) and Back-garden downwind regional site (BG) in July 2006. Particle number concentration from 20 nm to 10 μm at BG was (1.7±0.8)×104 cm−3, about 40% lower than that at GZ, (2.9±1.1)×104 cm−3. The total particle volume concentration at BG was 94±34 μm3 cm−3, similar to that at GZ, 96±43 μm3 cm−3. More 20–100 nm particles, significantly affected by the traffic emissions, were observed at GZ, while 100–660 nm particle number concentrations were similar at both sites as they are more regional. PM2.5 values were similar at GZ (69±43 μg m−3) and BG (69±58 μg m−3) with R2 of 0.71 for the daily average PM2.5 at these two sites, indicating the fine particulate pollution in the PRD region to be regional. Two kinds of pollution episodes, the accumulation pollution episode and the regional transport pollution episode, were observed. Fine particles over 100 nm dominated both number and volume concentrations of total particles during the late periods of these pollution episodes. Accumulation and secondary transformation are the main reasons for the nighttime accumulation pollution episode. SO42−, NO3− accounted for about 60% in 100–660 nm particle mass and PM2.5 increase. When south or southeast wind prevailed in the PRD region, regional transport of pollutants took place. Regional transport contributed about 30% to fine particulate pollution at BG during a regional transport case. Secondary transformation played an important role during regional transport, causing higher increase rates of secondary ions in PM1.0 than other species and shifting the peaks of sulfate and ammonium mass size distributions to larger sizes. SO42−, NO3−, and NH4+ accounted for about 70% and 40% of PM1.0 and PM2.5, respectively.
- ItemRelating particle hygroscopicity and CCN activity to chemical composition during the HCCT-2010 field campaign(München : European Geopyhsical Union, 2013) Wu, Z.J.; Poulain, L.; Henning, S.; Dieckmann, K.; Birmili, W.; Merkel, M.; van Pinxteren, D.; Spindler, G.; Müller, K.; Stratmann, F.; Herrmann, H.; Wiedensohler, A.Particle hygroscopic growth at 90% RH (relative humidity), cloud condensation nuclei (CCN) activity, and size-resolved chemical composition were concurrently measured in the Thüringer Wald mid-level mountain range in central Germany in the fall of 2010. The median hygroscopicity parameter values, κ, of 50, 75, 100, 150, 200, and 250 nm particles derived from hygroscopicity measurements are respectively 0.14, 0.14, 0.17, 0.21, 0.24, and 0.28 during the sampling period. The closure between HTDMA (Hygroscopicity Tandem Differential Mobility Analyzers)-measured (κHTDMA) and chemical composition-derived (κchem) hygroscopicity parameters was performed based on the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. Using size-averaged chemical composition, the κ values are substantially overpredicted (30 and 40% for 150 and 100 nm particles). Introducing size-resolved chemical composition substantially improved closure. We found that the evaporation of NH4NO3, which may happen in a HTDMA system, could lead to a discrepancy in predicted and measured particle hygroscopic growth. The hygroscopic parameter of the organic fraction, κorg, is positively correlated with the O : C ratio (κorg = 0.19 × (O : C) − 0.03). Such correlation is helpful to define the κorg value in the closure study. κ derived from CCN measurement was around 30% (varied with particle diameters) higher than that determined from particle hygroscopic growth measurements (here, hydrophilic mode is considered only). This difference might be explained by the surface tension effects, solution non-ideality, gas-particle partitioning of semivolatile compounds, and the partial solubility of constituents or non-dissolved particle matter. Therefore, extrapolating from HTDMA data to properties at the point of activation should be done with great care. Finally, closure study between CCNc (cloud condensation nucleus counter)-measured (κCCN) and chemical composition (κCCN, chem) was performed using CCNc-derived κ values for individual components. The results show that the κCCN can be well predicted using particle size-resolved chemical composition and the ZSR mixing rule.
- ItemThe simulations of sulfuric acid concentration and new particle formation in an urban atmosphere in China(München : European Geopyhsical Union, 2013) Wang, Z.B.; Hu, M.; Mogensen, D.; Yue, D.L.; Zheng, J.; Zhang, R.Y.; Liu, Y.; Yuan, B.; Li, X.; Shao, M.; Zhou, L.; Wu, Z.J.; Wiedensohler, A.; Boy, M.Simulations of sulfuric acid concentration and new particle formation are performed by using the zero-dimensional version of the model MALTE (Model to predict new Aerosol formation in the Lower TropospherE) and measurements from the Campaign of Air Quality Research in Beijing and Surrounding areas (CAREBeijing) in 2008. Chemical reactions from the Master Chemical Mechanism version 3.2 (MCM v3.2) are used in the model. High correlation (slope = 0.72, R = 0.74) between the modelled and observed sulfuric acid concentrations is found during daytime (06:00–18:00). The aerosol dynamics are simulated by the University of Helsinki Multicomponent Aerosol (UHMA) model including several nucleation mechanisms. The results indicate that the model is able to predict the on- and offset of new particle formation in an urban atmosphere in China. In addition, the number concentrations of newly formed particles in kinetic-type nucleation including homogenous homomolecular (J=K[H2SO4]2) and homogenous heteromolecular nucleation involving organic vapours (J=Khet[H2SO4][Org]) are in satisfactory agreement with the observations. However, the specific organic compounds that possibly participate in the nucleation process should be investigated in further studies. For the particle growth, only a small fraction of the oxidized total organics condense onto the particles in polluted environments. Meanwhile, the OH and O3 oxidation mechanism contribute 5.5% and 94.5% to the volume concentration of small particles, indicating the particle growth is more controlled by the precursor gases and their oxidation by O3.
- ItemTraffic restrictions in Beijing during the Sino-African Summit 2006: Aerosol size distribution and visibility compared to long-term in situ observations(München : European Geopyhsical Union, 2008) Cheng, Y.F.; Heintzenberg, J.; Wehner, B.; Wu, Z.J.; Su, H.; Mao, J.T.Based on the long-term in-situ observations of aerosol particle number size distributions and meteorological parameters, the measures of traffic restriction during the Sino-African Summit (4–6 November 2006) in Beijing, China have been found to be efficient in reducing the number concentration of aerosol particles, in particular Aitken and accumulation mode particles, and in improving the visibility when local emissions dominated. The influence of traffic restrictions on the particle concentrations differed for different particle sizes. More significant effects on fine particles with diameters ranging from 40 to 500 nm have been found. Based on statistical analysis of long-term observations, under comparable weather conditions, the number concentrations of the particles in Aitken and accumulation modes seemingly were reduced by 20–60% when the traffic restrictions were in place. This change may be mainly due to the reduction of secondary particle contributions. However, it is worth to notice that the reduction of 60% might overestimate the effect of the measures of traffic control, due to the inherent data shortage with very high wind speeds in the comparison data population. Our size-dependent aerosol data also indicate that measures led to reductions in particulate air pollution in the optically most important diameter range, whereas further vehicle restriction measures might lead to an increase in ultrafine particle formation if the condensational sink further decreased. Assuming that there were no traffic restrictions and with normal levels of the vehicle emissions, the visibilities during the Summit would have been lower by about 20–45%. The fact that over 95% cases with visibility range lower than 5 km during 2004 to 2007 occurred when the local wind speed was lower than 3 m s−1 may suggest that the importance of the emission restrictions is highest when the wind speed is lower than 3 m s−1, concerning the improvement of serious low visibility situations in Beijing.