Atmospheric gas-to-particle conversion: why NPF events are observed in megacities?

2017 ◽  
Vol 200 ◽  
pp. 271-288 ◽  
Author(s):  
M. Kulmala ◽  
V.-M. Kerminen ◽  
T. Petäjä ◽  
A. J. Ding ◽  
L. Wang

In terms of the global aerosol particle number load, atmospheric new particle formation (NPF) dominates over primary emissions. The key for quantifying the importance of atmospheric NPF is to understand how gas-to-particle conversion (GTP) takes place at sizes below a few nanometers in particle diameter in different environments, and how this nano-GTP affects the survival of small clusters into larger sizes. The survival probability of growing clusters is tied closely to the competition between their growth and scavenging by pre-existing aerosol particles, and the key parameter in this respect is the ratio between the condensation sink (CS) and the cluster growth rate (GR). Here we define their ratio as a dimensionless survival parameter,P, asP= (CS/10−4s−1)/(GR/nm h−1). Theoretical arguments and observations in clean and moderately-polluted conditions indicate thatPneeds to be smaller than about 50 for a notable NPF to take place. However, the existing literature shows that in China, NPF occurs frequently in megacities such as in Beijing, Nanjing and Shanghai, and our analysis shows that the calculated values ofPare even larger than 200 in these cases. By combining direct observations and conceptual modelling, we explore the variability of the survival parameterPin different environments and probe the reasons for NPF occurrence under highly-polluted conditions.

2018 ◽  
Vol 18 (7) ◽  
pp. 4533-4548 ◽  
Author(s):  
Joonas Enroth ◽  
Jyri Mikkilä ◽  
Zoltán Németh ◽  
Markku Kulmala ◽  
Imre Salma

Abstract. Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20), 50, 75, 110 and 145 nm were determined in situ by using a volatility–hygroscopicity tandem differential mobility analyser (VH-TDMA) system with a relative humidity of 90 % and denuding temperature of 270 ∘C in central Budapest during 2 months in winter 2014–2015. The probability density function of the hygroscopic growth factor (HGF) showed a distinct bimodal distribution. One of the modes was characterised by an overall mean HGF of approximately 1.07 (this corresponds to a hygroscopicity parameter κ of 0.033) independently of the particle size and was assigned to nearly hydrophobic (NH) particles. Its mean particle number fraction was large, and it decreased monotonically from 69 to 41 % with particle diameter. The other mode showed a mean HGF increasing slightly from 1.31 to 1.38 (κ values from 0.186 to 0.196) with particle diameter, and it was attributed to less hygroscopic (LH) particles. The mode with more hygroscopic particles was not identified. The probability density function of the volatility GF (VGF) also exhibited a distinct bimodal distribution with an overall mean VGF of approximately 0.96 independently of the particle size, and with another mean VGF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV) and volatile (V) particles. The mean particle number fraction for the LV mode decreased from 34 to 21 % with particle diameter. The bimodal distributions indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. Particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic compounds such as non-hygroscopic hydrocarbon-like organics. The hygroscopic particles were ordinarily volatile. They could be composed of moderately transformed aged combustion particles consisting of partly oxygenated organics, inorganic salts and soot. The larger particles contained internally mixed non-volatile chemical species as a refractory residual in 20–25 % of the aerosol material (by volume).


2017 ◽  
Author(s):  
Joonas Enroth ◽  
Jyri Mikkilä ◽  
Zoltán Németh ◽  
Markku Kulmala ◽  
Imre Salma

Abstract. Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20), 50, 75, 110 and 145 nm were determined in situ by using a VH-TDMA system with a relative humidity of 90 % and denuding temperature of 270 °C in central Budapest during two months in winter 2014–2015. The probability density function of the hygroscopic growth factor (GF) showed a distinct bimodal distribution. One of the modes was characterized by an overall mean GF of approximately 1.07 (the corresponding hygroscopicity parameter κ of 0.033) independently of the particle size, and was assigned to nearly hydrophobic (NH) particles. Its mean particle number fraction was large, and it was decreasing monotonically from 71 % to 41 % with particle diameter. The other mode showed a mean GF increasing slightly from 1.31 to 1.38 (κ values from 0.186 to 0.196) with particle diameter, and it was attributed to less hygroscopic (LH) particles. These hygroscopicity values are low in general. The mode with more hygroscopic particles was not identified. The probability density function of the volatility GF also exhibited a distinct bimodal distribution with an overall mean volatility GF of approximately 0.96 independently of the particle size, and with another mean GF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV) and volatile (V) particles. The mean particle number fraction for the LV mode was decreasing from 34 % to 21 % with particle diameter. The bimodal distributions in the GF spectrum indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. The mean diurnal variability of the particle number fractions for the NH and LV modes, and of the volatility GF for the LV mode followed the diurnal pattern of the vehicular road traffic, while the mean diurnal variability of the hygroscopicity parameter for the NH, and of the particle number fractions for the V mode on workdays were inversely linked to the road traffic. The particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic compounds such as non-hygroscopic hydrocarbon-like organics. The particles related to the LH and V modes could be composed of moderately transformed aged combustion particles consisting of partly oxygenated organics, inorganic salts and soot. Both regional background sources and urban (local) emissions contribute to these particles. Dependency of the volatility GF and the volume fraction remaining after the thermal treatment on the mean hygroscopic GF suggested that the hygroscopic compounds were ordinarily volatile, and that the larger particles contained internally mixed non-volatile chemical species as refractory residuals in 20–25 % of the aerosol material (by volume), which could be core-like soot or organic polymers.


2005 ◽  
Vol 5 (11) ◽  
pp. 2989-3002 ◽  
Author(s):  
P. Guyon ◽  
G. P. Frank ◽  
M. Welling ◽  
D. Chand ◽  
P. Artaxo ◽  
...  

Abstract. As part of the LBA-SMOCC (Large-Scale Biosphere-Atmosphere Experiment in Amazonia - Smoke, Aerosols, Clouds, Rainfall, and Climate) 2002 campaign, we studied the emission of carbon monoxide (CO), carbon dioxide (CO2), and aerosol particles from Amazonian deforestation fires using an instrumented aircraft. Emission ratios for aerosol number (CN) relative to CO (ERCN/CO) fell in the range 14-32 cm-3 ppb-1 in most of the investigated smoke plumes. Particle number emission ratios have to our knowledge not been previously measured in tropical deforestation fires, but our results are in agreement with values usually found from tropical savanna fires. The number of particles emitted per amount biomass burned was found to be dependent on the fire conditions (combustion efficiency). Variability in ERCN/CO between fires was similar to the variability caused by variations in combustion behavior within each individual fire. This was confirmed by observations of CO-to-CO2 emission ratios (ERCO/CO2), which stretched across the same wide range of values for individual fires as for all the fires observed during the sampling campaign, reflecting the fact that flaming and smoldering phases are present simultaneously in deforestation fires. Emission factors (EF) for CO and aerosol particles were computed and a correction was applied for the residual smoldering combustion (RSC) fraction of emissions that are not sampled by the aircraft, which increased the EF by a factor of 1.5-2.1. Vertical transport of smoke from the boundary layer (BL) to the cloud detrainment layer (CDL) and the free troposphere (FT) was found to be a very common phenomenon. We observed a 20% loss in particle number as a result of this vertical transport and subsequent cloud processing, attributable to in-cloud coagulation. This small loss fraction suggests that this mode of transport is very efficient in terms of particle numbers and occurs mostly via non-precipitating clouds. The detrained aerosol particles released in the CDL and FT were larger than in the unprocessed smoke, mostly due to coagulation and secondary growth, and therefore more efficient at scattering radiation and nucleating cloud droplets. This process may have significant atmospheric implications on a regional and larger scale.


2017 ◽  
Vol 17 (24) ◽  
pp. 15007-15017 ◽  
Author(s):  
Imre Salma ◽  
Veronika Varga ◽  
Zoltán Németh

Abstract. Effects of a new aerosol particle formation (NPF) and particle diameter growth process as a single source of atmospheric particle number concentrations were evaluated and quantified on the basis of experimental data sets obtained from particle number size distribution measurements in the city centre and near-city background of Budapest for 5 years. Nucleation strength factors for a nucleation day (NSFNUC) and for a general day (NSFGEN) were derived separately for seasons and full years. The former characteristic represents the concentration increment of ultrafine (UF) particles specifically on nucleation days with respect to accumulation-mode (regional background) concentrations (particles with equivalent diameters of 100–1000 nm; N100−1000) due solely to the nucleation process. The latter factor expresses the contribution of nucleation to particle numbers on general days; thus, it represents a longer time interval such as season or year. The nucleation source had the largest effect on the concentrations around noon and early afternoon, as expected. During this time interval, it became the major source of particles in the near-city background. Nucleation increased the daily mean concentrations on nucleation days by mean factors of 2.3 and 1.58 in the near-city background and city centre, respectively. Its effect was largest in winter, which was explained by the substantially lower N100−1000 levels on nucleation days than those on non-nucleation days. On an annual timescale, 37 % of the UF particles were generated by nucleation in the near-city background, while NPF produced 13 % of UF particles in the city centre. The differences among the annual mean values, and among the corresponding seasonal mean values, were likely caused by the variability in controlling factors from year to year. The values obtained represent the lower limits of the contributions. The shares determined imply that NPF is a non-negligible or substantial source of particles in near-city background environments and even in city centres, where the vehicular road emissions usually prevail. Atmospheric residence time of nucleation-mode particles was assessed by a decay curve analysis, and a mean of 02:30 was obtained. The present study suggests that the health-related consequences of the atmospheric NPF and growth process in cities should also be considered in addition to its urban climate implications.


Author(s):  
Richard Pasteka ◽  
Joao Pedro Santos da Costa ◽  
Mathias Forjan

Dry powder inhalers are used by a large number of patients worldwide to treat respiratory diseases. The objective of this work is to experimentally investigate changes in aerosol particle diameter and particle number concentration of pharmaceutical aerosols generated by five dry powder inhalers under realistic inhalation and exhalation conditions. The active respiratory system model (xPULM™) was used as a model of the human respiratory system and to simulate a patient undergoing inhalation therapy. A mechanical upper airway model was developed, manufactured and introduced as a part of the xPULM™ to represent the human upper respiratory tract with high fidelity. Integration of optical aerosol spectrometry technique into the setup allowed for evaluation of pharmaceutical aerosols. The results show that the upper airway model increases the resistance of the overall system and act as a filter for bigger particles (>3 µm). Furthermore, there is a significant difference (p < 0.05) in mean particle diameter between inhaled and exhaled particles with the majority of the particles depositing in the lung. The minimum deposition is reached for particle size of 0.5 µm. The mean particle number concentrations exhaled are 2.94% (BreezHaler®), 2.66% (Diskus®), 10.24% (Ellipta®) 2.13% (HandiHaler®) and 6.22% (Turbohaler®). In conclusion, the xPULM™ active respiratory system model is a viable option for studying interactions of pharmaceutical aerosols and the respiratory tract in terms of applicable deposition mechanisms. The model can support the reduction of animal experimentation in aerosol research and provide an alternative to experiments with human subjects.


2021 ◽  
Vol 21 (14) ◽  
pp. 11289-11302
Author(s):  
Imre Salma ◽  
Wanda Thén ◽  
Máté Vörösmarty ◽  
András Zénó Gyöngyösi

Abstract. Collocated measurements using a condensation particle counter, differential mobility particle sizer and cloud condensation nuclei counter were realised in parallel in central Budapest from 15 April 2019 to 14 April 2020 to gain insight into the cloud activation properties of urban aerosol particles. The median total particle number concentration was 10.1 × 103 cm−3. The median concentrations of cloud condensation nuclei (CCN) at water vapour supersaturation (S) values of 0.1 %, 0.2 %, 0.3 %, 0.5 % and 1.0 % were 0.59, 1.09, 1.39, 1.80 and 2.5 × 103 cm−3, respectively. The CCN concentrations represented 7–27 % of all particles. The CCN concentrations were considerably larger but the activation fractions were systematically substantially smaller than observed in regional or remote locations. The effective critical dry particle diameters (dc,eff) were derived utilising the CCN concentrations and particle number size distributions. Their median values at the five supersaturation values considered were 207, 149, 126, 105 and 80 nm, respectively; all of these diameters were positioned within the accumulation mode of the typical particle number size distribution. Their frequency distributions revealed a single peak for which the geometric standard deviation increased monotonically with S. This broadening indicated high time variability in the activating properties of smaller particles. The frequency distributions also showed fine structure, with several compositional elements that seemed to reveal a consistent or monotonical tendency with S. The relationships between the critical S and dc,eff suggest that urban aerosol particles in Budapest with diameters larger than approximately 130 nm showed similar hydroscopicity to corresponding continental aerosol particles, whereas smaller particles in Budapest were less hygroscopic than corresponding continental aerosol particles. Only modest seasonal cycling in CCN concentrations and activation fractions was seen, and only for large S values. This cycling likely reflects changes in the number concentration, chemical composition and mixing state of the particles. The seasonal dependencies of dc,eff were featureless, indicating that the droplet activation properties of the urban particles remained more or less the same throughout the year. This is again different from what is seen in non-urban locations. Hygroscopicity parameters (κ values) were computed without determining the time-dependent chemical composition of the particles. The median values for κ were 0.15, 0.10, 0.07, 0.04 and 0.02, respectively, at the five supersaturation values considered. The averages suggested that the larger particles were considerably more hygroscopic than the smaller particles. We found that the κ values for the urban aerosol were substantially smaller than those previously reported for aerosols in regional or remote locations. All of these characteristics can be linked to the specific source composition of particles in cities. The relatively large variability in the hygroscopicity parameters for a given S emphasises that the individual values represent the CCN population in ambient air while the average hygroscopicity parameter mainly corresponds to particles with sizes close to the effective critical dry particle diameter.


2017 ◽  
Author(s):  
Filippo Xausa ◽  
Pauli Paasonen ◽  
Risto Makkonen ◽  
Mikhail Arshinov ◽  
Aijun Ding ◽  
...  

Abstract. Climate models are important tools that are used for generating climate change projections, in which aerosol-climate interactions are one of the main sources of uncertainties. In order to quantify aerosol-radiation and aerosol-cloud interactions, detailed input of anthropogenic aerosol number emissions is necessary. However, the anthropogenic aerosol number emissions are usually converted from the corresponding mass emissions in precompiled emission inventories through a very simplistic method depending uniquely on chemical composition, particle size and density, which are defined for a few very wide main source sectors. In this work, the anthropogenic particle number emissions converted from the AeroCom mass in the ECHAM-HAM climate model were replaced with the recently-formulated number emissions from the Greenhouse Gas and Air Pollution Interactions and Synergies (GAINS)-model, where the emission number size distributions vary, for example, with respect to the fuel and technology. A special attention in our analysis was put on accumulation mode particles (particle diameter dp > 100 nm) because of (i) their capability of acting as cloud condensation nuclei (CCN), thus forming cloud droplets and affecting Earth's radiation budget, and (ii) their dominant role in forming the coagulation sink and thus limiting the concentration of sub-100 nanometers particles. In addition, the estimates of anthropogenic CCN formation, and thus the forcing from aerosol-climate interactions are expected to be affected. Analysis of global particle number concentrations and size distributions reveal that GAINS implementation increases CCN concentration compared with AeroCom, with regional enhancement factors reaching values as high as 10. A comparison between modeled and observed concentrations shows that the increase in number concentration for accumulation mode particle agrees well with measurements, but it leads to a consistent underestimation of both nucleation mode and Aitken mode (dp > 100 nm) particle number concentrations. This suggests that revisions are needed in the new particle formation and growth schemes currently applied in global modeling frameworks.


2020 ◽  
Vol 20 (19) ◽  
pp. 11329-11348 ◽  
Author(s):  
Jenni Kontkanen ◽  
Chenjuan Deng ◽  
Yueyun Fu ◽  
Lubna Dada ◽  
Ying Zhou ◽  
...  

Abstract. The climate and air quality effects of aerosol particles depend on the number and size of the particles. In urban environments, a large fraction of aerosol particles originates from anthropogenic emissions. To evaluate the effects of different pollution sources on air quality, knowledge of size distributions of particle number emissions is needed. Here we introduce a novel method for determining size-resolved particle number emissions, based on measured particle size distributions. We apply our method to data measured in Beijing, China, to determine the number size distribution of emitted particles in a diameter range from 2 to 1000 nm. The observed particle number emissions are dominated by emissions of particles smaller than 30 nm. Our results suggest that traffic is the major source of particle number emissions with the highest emissions observed for particles around 10 nm during rush hours. At sizes below 6 nm, clustering of atmospheric vapors contributes to calculated emissions. The comparison between our calculated emissions and those estimated with an integrated assessment model GAINS (Greenhouse Gas and Air Pollution Interactions and Synergies) shows that our method yields clearly higher particle emissions at sizes below 60 nm, but at sizes above that the two methods agree well. Overall, our method is proven to be a useful tool for gaining new knowledge of the size distributions of particle number emissions in urban environments and for validating emission inventories and models. In the future, the method will be developed by modeling the transport of particles from different sources to obtain more accurate estimates of particle number emissions.


2021 ◽  
Vol 21 (22) ◽  
pp. 17185-17223
Author(s):  
Clémence Rose ◽  
Martine Collaud Coen ◽  
Elisabeth Andrews ◽  
Yong Lin ◽  
Isaline Bossert ◽  
...  

Abstract. Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50 % and 60 % were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (∼ 102 cm−3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day–night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (∼ 103–104 cm−3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (∼ 102–103 cm−3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on the order of ∼ 10 to 1000 cm−3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol–cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate.


2020 ◽  
Vol 11 (4) ◽  
pp. 803-814 ◽  
Author(s):  
Jan Mertens ◽  
H. Lepaumier ◽  
P. Rogiers ◽  
D. Desagher ◽  
L. Goossens ◽  
...  

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