| 1. |
- Almeida, Joao, et al.
(författare)
-
Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere
- 2013
-
Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 502:7471, s. 359-
-
Tidskriftsartikel (refereegranskat)abstract
- Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei(1). Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes(2). Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases(2). However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere(3). It is thought that amines may enhance nucleation(4-16), but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid-amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid-dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.
|
|
| 2. |
- Lehtipalo, Katrianne, et al.
(författare)
-
The effect of acid-base clustering and ions on the growth of atmospheric nano-particles
- 2016
-
Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 7
-
Tidskriftsartikel (refereegranskat)abstract
- The growth of freshly formed aerosol particles can be the bottleneck in their survival to cloud condensation nuclei. It is therefore crucial to understand how particles grow in the atmosphere. Insufficient experimental data has impeded a profound understanding of nano-particle growth under atmospheric conditions. Here we study nano-particle growth in the CLOUD (Cosmics Leaving OUtdoors Droplets) chamber, starting from the formation of molecular clusters. We present measured growth rates at sub-3 nm sizes with different atmospherically relevant concentrations of sulphuric acid, water, ammonia and dimethylamine. We find that atmospheric ions and small acid-base clusters, which are not generally accounted for in the measurement of sulphuric acid vapour, can participate in the growth process, leading to enhanced growth rates. The availability of compounds capable of stabilizing sulphuric acid clusters governs the magnitude of these effects and thus the exact growth mechanism. We bring these observations into a coherent framework and discuss their significance in the atmosphere.
|
|
| 3. |
- Blichner, Sara M., 1989-, et al.
(författare)
-
Process-evaluation of forest aerosol-cloud-climate feedback shows clear evidence from observations and large uncertainty in models
- 2024
-
Ingår i: Nature Communications. - 2041-1723. ; 15
-
Tidskriftsartikel (refereegranskat)abstract
- Natural aerosol feedbacks are expected to become more important in the future, as anthropogenic aerosol emissions decrease due to air quality policy. One such feedback is initiated by the increase in biogenic volatile organic compound (BVOC) emissions with higher temperatures, leading to higher secondary organic aerosol (SOA) production and a cooling of the surface via impacts on cloud radiative properties. Motivated by the considerable spread in feedback strength in Earth System Models (ESMs), we here use two long-term observational datasets from boreal and tropical forests, together with satellite data, for a process-based evaluation of the BVOC-aerosol-cloud feedback in four ESMs. The model evaluation shows that the weakest modelled feedback estimates can likely be excluded, but highlights compensating errors making it difficult to draw conclusions of the strongest estimates. Overall, the method of evaluating along process chains shows promise in pin-pointing sources of uncertainty and constraining modelled aerosol feedbacks.
|
|
| 4. |
- Buchholz, Angela, et al.
(författare)
-
Insights into the O : C-dependent mechanisms controlling the evaporation of alpha-pinene secondary organic aerosol particles
- 2019
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:6, s. 4061-4073
-
Tidskriftsartikel (refereegranskat)abstract
- The volatility of oxidation products of volatile organic compounds (VOCs) in the atmosphere is a key factor to determine if they partition into the particle phase contributing to secondary organic aerosol (SOA) mass. Thus, linking volatility and measured particle composition will provide insights into SOA formation and its fate in the atmosphere. We produced alpha-pinene SOA with three different oxidation levels (characterized by average oxygen-to-carbon ratio; (O:C) over bar = 0.53, 0.69, and 0.96) in an oxidation flow reactor. We investigated the particle volatility by isothermal evaporation in clean air as a function of relative humidity (RH < 2 %, 40 %, and 80 %) and used a filter-based thermal desorption method to gain volatility and chemical composition information. We observed reduced particle evaporation for particles with increasing <(O:C )over bar> ratio, indicating that particles become more resilient to evaporation with oxidative aging. Particle evaporation was increased in the presence of water vapour and presumably particulate water; at the same time the resistance of the residual particles to thermal desorption was increased as well. For SOA with (O:C ) over bar = 0.96, the unexpectedly large increase in mean thermal desorption temperature and changes in the thermogram shapes under wet conditions (80 % RH) were an indication of aqueous phase chemistry. For the lower (O:C ) over bar cases, some water-induced composition changes were observed. However, the enhanced evaporation under wet conditions could be explained by the reduction in particle viscosity from the semi-solid to liquid-like range, and the observed higher desorption temperature of the residual particles is a direct consequence of the increased removal of high-volatility and the continued presence of low-volatility compounds.
|
|
| 5. |
- Crljenica, Ivica, et al.
(författare)
-
Determining the saturation vapour pressures of keto-dicarboxylic acids in aqueous solutions
- 2013
-
Ingår i: NUCLEATION AND ATMOSPHERIC AEROSOLS. - : American Institute of Physics (AIP). - 9780735411524 ; , s. 468-471
-
Konferensbidrag (refereegranskat)abstract
- A two-compartment binary mass transport model with group contribution methods parametrizations for the physical properties of the organic acids (UNIFAC Dortmund method for activity coefficients, GCVOL-OL-60 method for the pure liquid acid density, GC-MG method for the pure acid surface tension at room temperature, Fuller et al. method for the diffusion coefficients) was used to interpret the evaporation experiments of 100 nm sized keto-dicarboxylic acid aqueous solutions droplets at ambient temperature. The determined values for the saturation vapour pressure of liquid 2-keto-glutaric acid are in the order of 10(-5) Pa.
|
|
| 6. |
- Hao, Liqing, et al.
(författare)
-
Combined effects of boundary layer dynamics and atmospheric chemistry on aerosol composition during new particle formation periods
- 2018
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:23, s. 17705-17716
-
Tidskriftsartikel (refereegranskat)abstract
- Characterizing aerosol chemical composition in response to meteorological changes and atmospheric chemistry is important to gain insights into new particle formation mechanisms. A BAECC (Biogenic Aerosols - Effects on Clouds and Climate) campaign was conducted during the spring 2014 at the SMEAR II station (Station for Measuring Forest Ecosystem-Aerosol Relations) in Finland. The particles were characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). A PBL (planetary boundary layer) dilution model was developed to assist interpreting the measurement results. Right before nucleation events, the mass concentrations of organic and sulfate aerosol species were both decreased rapidly along with the growth of PBL heights. However, the mass fraction of sulfate aerosol of the total aerosol mass was increased, in contrast to a decrease for the organic mass fraction. Meanwhile, an increase in LVOOA (low-volatility oxygenated organic aerosol) mass fraction of the total organic mass was observed, in distinct comparison to a reduction of SVOOA (semi-volatile OOA) mass fraction. Our results demonstrate that, at the beginning of nucleation events, the observed sulfate aerosol mass was mainly driven by vertical turbulent mixing of sulfate-rich aerosols between the residual layer and the newly formed boundary layer, while the condensation of sulfuric acid (SA) played a minor role in interpreting the measured sulfate mass concentration. For the measured organic aerosols, their temporal profiles were mainly driven by dilution from PBL development, organic aerosol mixing in different boundary layers and/or partitioning of organic vapors, but accurate measurements of organic vapor concentrations and characterization on the spatial aerosol chemical composition are required. In general, the observed aerosol particles by AMS are subjected to joint effects of PBL dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During aerosol growth periods in the nighttime, the mass concentrations of organic aerosols and organic nitrate aerosols were both increased. The increase in SVOOA mass correlated well with the calculated increase in condensed HOMs' (highly oxygenated organic molecules) mass. To our knowledge, our results are the first atmospheric observations showing a connection between increase in SVOOA and condensed HOMs during the nighttime.
|
|
| 7. |
- Heitto, Arto, et al.
(författare)
-
Analysis of atmospheric particle growth based on vapor concentrations measured at the high-altitude GAW station Chacaltaya in the Bolivian Andes
- 2024
-
Ingår i: Atmospheric Chemistry and Physics. - 1680-7316 .- 1680-7324. ; 24, s. 1315-1328
-
Tidskriftsartikel (refereegranskat)abstract
- Early growth of atmospheric particles is essential for their survival and ability to participate in cloud formation. Many different atmospheric vapors contribute to the growth, but even the main contributors still remain poorly identified in many environments, such as high-altitude sites. Based on measured organic vapor and sulfuric acid concentrations under ambient conditions, particle growth during new particle formation events was simulated and compared with the measured particle size distribution at the Chacaltaya Global Atmosphere Watch station in Bolivia (5240ma.s.l.) during April and May 2018, as a part of the SALTENA (Southern Hemisphere high-ALTitude Experiment on particle Nucleation and growth) campaign. Despite the challenging topography and ambient conditions around the station, the simple particle growth model used in the study was able to show that the detected vapors were sufficient to explain the observed particle growth, although some discrepancies were found between modeled and measured particle growth rates. This study, one of the first of such studies conducted on high altitude, gives insight on the key factors affecting the particle growth on the site and helps to improve the understanding of important factors on high-altitude sites and the atmosphere in general. Low-volatility organic compounds originating from multiple surrounding sources such as the Amazonia and La Paz metropolitan area were found to be the main contributor to the particle growth, covering on average 65% of the simulated particle mass in particles with a diameter of 30nm. In addition, sulfuric acid made a major contribution to the particle growth, covering at maximum 37% of the simulated particle mass in 30nm particles during periods when volcanic activity was detected on the area, compared to around 1% contribution on days without volcanic activity. This suggests that volcanic emissions can greatly enhance the particle growth.
|
|
| 8. |
- Henschel, Henning, et al.
(författare)
-
Hydration of Atmospherically Relevant Molecular Clusters : Computational Chemistry and Classical Thermodynamics
- 2014
-
Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 118:14, s. 2599-2611
-
Tidskriftsartikel (refereegranskat)abstract
- Formation of new particles through clustering of molecules from condensable vapors is a significant source for atmospheric aerosols. The smallest clusters formed in the very first steps of the condensation process are, however, not directly observable by experimental means. We present here a comprehensive series of electronic structure calculations on the hydrates of clusters formed by up to four molecules of sulfuric acid, and up to two molecules of ammonia or dimethylamine. Though clusters containing ammonia, and certainly dimethylamine, generally exhibit lower average hydration than the pure acid clusters, populations of individual hydrates vary widely. Furthermore, we explore the predictions obtained using a thermodynamic model for the description of these hydrates. The similar magnitude and trends of hydrate formation predicted by both methods illustrate the potential of combining them to obtain more comprehensive models. The stabilization of some clusters relative to others due to their hydration is highly likely to have significant effects on the overall processes that lead to formation of new particles in the atmosphere.
|
|
| 9. |
- Hirsikko, Anne, et al.
(författare)
-
Indoor and outdoor air ions and aerosol particles in the urban atmosphere of Helsinki : characteristics, sources and formation
- 2007
-
Ingår i: Boreal environment research. - 1239-6095 .- 1797-2469. ; 12:3, s. 295-310
-
Tidskriftsartikel (refereegranskat)abstract
- We measured air ion size distributions with an air ion spectrometer in the size range of 0.34-40.3 nm both indoors (in July) and outdoors (in August) in Helsinki, Finland in 2004. At the same time we measured particle number concentrations and size distributions with two condensation particle counters (indoors) and differential mobility particle sizer (outdoors). Our main focus was to study new-particle formation in an urban site. We observed new-particle formation indoors almost every day, even many times a day, and four times outdoors. Indoors, the observed growth rates were 2.3-4.9 nm h-' for 1.3-3-nm ions, 6.5-8.7 nm h(-1) for 3-7-nm ions and 5.1-8.7 nm h-' for 7-20-nm ions. Outdoor ions (3-7 nm) grew at rates as large as 15.4 nm h-'. Outdoor ion and particle number concentrations were dependent on the wind direction, whereas indoor concentrations were dependent on ventilation conditions. Secondary particle formation and growth affected concentrations both indoors and outdoors. We concluded, based on our measurement results and simulated penetration of outdoor particles through the ventilation system, that we had indoor sources for secondary particles.
|
|
| 10. |
- Huang, Wei, et al.
(författare)
-
Variation in chemical composition and volatility of oxygenated organic aerosol in different rural, urban, and mountain environments
- 2024
-
Ingår i: Atmospheric Chemistry and Physics. - 1680-7316 .- 1680-7324. ; 24:4, s. 2607-2624
-
Tidskriftsartikel (refereegranskat)abstract
- The apparent volatility of atmospheric organic aerosol (OA) particles is determined by their chemical composition and environmental conditions (e.g., ambient temperature). A quantitative, experimental assessment of volatility and the respective importance of these two factors remains challenging, especially in ambient measurements. We present molecular composition and volatility of oxygenated OA (OOA) particles in different rural, urban, and mountain environments (including Chacaltaya, Bolivia; Alabama, US; Hyytiälä, Finland; Stuttgart and Karlsruhe, Germany; and Delhi, India) based on deployments of a filter inlet for gases and aerosols coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (FIGAERO-CIMS). We find on average larger carbon numbers (nC) and lower oxygen-To-carbon (O:C) ratios at the urban sites (nC: 9.8±0.7; O:C: 0.76±0.03; average ±1 standard deviation) compared to the rural (nC: 8.8±0.6; O:C: 0.80±0.05) and mountain stations (nC: 8.1±0.8; O:C: 0.91±0.07), indicative of different emission sources and chemistry. Compounds containing only carbon, hydrogen, and oxygen atoms (CHO) contribute the most to the total OOA mass at the rural sites (79.9±5.2%), in accordance with their proximity to forested areas (66.2±5.5% at the mountain sites and 72.6±4.3% at the urban sites). The largest contribution of nitrogen-containing compounds (CHON) is found at the urban stations (27.1±4.3%), consistent with their higher NOx levels. Moreover, we parametrize OOA volatility (saturation mass concentrations, Csat) using molecular composition information and compare it with the bulk apparent volatility derived from thermal desorption of the OOA particles within the FIGAERO. We find differences in Csat values of up to 1/43 orders of magnitude and variation in thermal desorption profiles (thermograms) across different locations and systems. From our study, we draw the general conclusion that environmental conditions (e.g., ambient temperature) do not directly affect OOA apparent volatility but rather indirectly by influencing the sources and chemistry of the environment and thus the chemical composition. The comprehensive dataset provides results that show the complex thermodynamics and chemistry of OOA and their changes during its lifetime in the atmosphere. We conclude that generally the chemical description of OOA suffices to predict its apparent volatility, at least qualitatively. Our study thus provides new insights that will help guide choices of, e.g., descriptions of OOA volatility in different model frameworks such as air quality models and cloud parcel models.
|
|
| 11. |
- Isokääntä, Sini, et al.
(författare)
-
The effect of clouds and precipitation on the aerosol concentrations and composition in a boreal forest environment
- 2022
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:17, s. 11823-11843
-
Tidskriftsartikel (refereegranskat)abstract
- Atmospheric aerosol particle concentrations are strongly affected by various wet processes, including below and in-cloud wet scavenging and in-cloud aqueous-phase oxidation. We studied how wet scavenging and cloud processes affect particle concentrations and composition during transport to a rural boreal forest site in northern Europe. For this investigation, we employed air mass history analysis and observational data. Long-term particle number size distribution (∼15 years) and composition measurements (∼8 years) were combined with air mass trajectories with relevant variables from reanalysis data. Some such variables were rainfall rate, relative humidity, and mixing layer height. Additional observational datasets, such as temperature and trace gases, helped further evaluate wet processes along trajectories with mixed effects models.All chemical species investigated (sulfate, black carbon, and organics) exponentially decreased in particle mass concentration as a function of accumulated precipitation along the air mass route. In sulfate (SO4) aerosols, clear seasonal differences in wet removal emerged, whereas organics (Org) and equivalent black carbon (eBC) exhibited only minor differences. The removal efficiency varied slightly among the different reanalysis datasets (ERA-Interim and Global Data Assimilation System; GDAS) used for the trajectory calculations due to the difference in the average occurrence of precipitation events along the air mass trajectories between the reanalysis datasets.Aqueous-phase processes were investigated by using a proxy for air masses travelling inside clouds. We compared air masses with no experience of approximated in-cloud conditions or precipitation during the past 24 h to air masses recently inside non-precipitating clouds before they entered SMEAR II (Station for Measuring Ecosystem–Atmosphere Relations). Significant increases in SO4 mass concentration were observed for the latter air masses (recently experienced non-precipitating clouds).Our mixed effects model considered other contributing factors affecting particle mass concentrations in SMEAR II: examples were trace gases, local meteorology, and diurnal variation. This model also indicated in-cloud SO4 production. Despite the reanalysis dataset used in the trajectory calculations, aqueous-phase SO4 formation was observed. Particle number size distribution measurements revealed that most of the in-cloud SO4 formed can be attributed to particle sizes larger than 200 nm (electrical mobility diameter). Aqueous-phase secondary organic aerosol (aqSOA) formation was non-significant.
|
|
| 12. |
- Lampilahti, Janne, et al.
(författare)
-
Zeppelin-led study on the onset of new particle formation in the planetary boundary layer
- 2021
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:16, s. 12649-12663
-
Tidskriftsartikel (refereegranskat)abstract
- We compared observations of aerosol particle formation and growth in different parts of the planetary boundary layer at two different environments that have frequent new particle formation (NPF) events. In summer 2012 we had a campaign in Po Valley, Italy (urban background), and in spring 2013 a similar campaign took place in Hyytiälä, Finland (rural background). Our study consists of three case studies of airborne and ground-based measurements of ion and particle size distribution from ∼1 nm. The airborne measurements were performed using a Zeppelin inside the boundary layer up to 1000 m altitude. Our observations show the onset of regional NPF and the subsequent growth of the aerosol particles happening almost uniformly inside the mixed layer (ML) in both locations. However, in Hyytiälä we noticed local enhancement in the intensity of NPF caused by mesoscale boundary layer (BL) dynamics. Additionally, our observations indicate that in Hyytiälä NPF was probably also taking place above the ML. In Po Valley we observed NPF that was limited to a specific air mass.
|
|
| 13. |
- Leinonen, Ville, et al.
(författare)
-
Comparison of particle number size distribution trends in ground measurements and climate models
- 2022
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:19, s. 12873-12905
-
Tidskriftsartikel (refereegranskat)abstract
- Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol–cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability.
|
|
| 14. |
- Mohr, Claudia, et al.
(författare)
-
Molecular identification of organic vapors driving atmospheric nanoparticle growth
- 2019
-
Ingår i: Nature communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 10
-
Tidskriftsartikel (refereegranskat)abstract
- Particles formed in the atmosphere via nucleation provide about half the number of atmospheric cloud condensation nuclei, but in many locations, this process is limited by the growth of the newly formed particles. That growth is often via condensation of organic vapors. Identification of these vapors and their sources is thus fundamental for simulating changes to aerosol-cloud interactions, which are one of the most uncertain aspects of anthropogenic climate forcing. Here we present direct molecular-level observations of a distribution of organic vapors in a forested environment that can explain simultaneously observed atmospheric nanoparticle growth from 3 to 50nm. Furthermore, the volatility distribution of these vapors is sufficient to explain nanoparticle growth without invoking particle-phase processes. The agreement between observed mass growth, and the growth predicted from the observed mass of condensing vapors in a forested environment thus represents an important step forward in the characterization of atmospheric particle growth.
|
|
| 15. |
- Olenius, Tinja, et al.
(författare)
-
Modeling of exhaust gas cleaning by acid pollutant conversion to aerosol particles
- 2021
-
Ingår i: Fuel. - : Elsevier BV. - 0016-2361 .- 1873-7153. ; 290
-
Tidskriftsartikel (refereegranskat)abstract
- Sulfur and nitrogen oxides (SOx and NOx) are harmful pollutants emitted into the atmosphere by industry and transport sectors. In addition to being hazardous gases, SOx and NOx form sulfuric and nitric acids which contribute to the formation of airborne particulate matter through nucleation and condensation, hence magnifying the environmental impact of these species. In this work, we build a modeling framework for utilizing this phenomenon for low-temperature exhaust gas cleaning. It has been reported that ammonia gas can be used to facilitate particle formation from the aforementioned acids, and thus remove these gaseous pollutants by converting them into ammonium sulfate and nitrate particles. Here we provide comprehensive modeling tools for applying this idea to exhaust gas cleaning by combining detailed models for nucleation, gas-particle mass exchange and particle population dynamics. We demonstrate how these models can be used to find advantageous operating conditions for a cleaning unit. In particular, the full model is computationally cheap and enables optimization of the particle formation efficiency and particle growth, hence ensuring sufficient conversion of gaseous pollutants into collectable particulate matter. This constitutes a ground for future engineering tools for designing next-generation sustainable exhaust gas cleaners.
|
|
| 16. |
- Riipinen, Ilona, et al.
(författare)
-
The contribution of organics to atmospheric nanoparticle growth
- 2012
-
Ingår i: Nature Geoscience. - : Springer Science and Business Media LLC. - 1752-0894 .- 1752-0908. ; 5:7, s. 453-458
-
Tidskriftsartikel (refereegranskat)abstract
- Aerosols have a strong, yet poorly quantified, effect on climate. The growth of the smallest atmospheric particles from diameters in the nanometre range to sizes at which they may act as seeds for cloud droplets is a key step linking aerosols to clouds and climate. In many environments, atmospheric nanoparticles grow by taking up organic compounds that are derived from biogenic hydrocarbon emissions. Several mechanisms may control this uptake. Condensation of low-volatility vapours and formation of organic salts probably dominate the very first steps of growth in particles close to 1 nm in diameter. As the particles grow further, formation of organic polymers and effects related to the phase of the particle probably become increasingly important. We suggest that dependence of particle growth mechanisms on particle size needs to be investigated more systematically.
|
|
| 17. |
- Wang, Mingyi, et al.
(författare)
-
Rapid growth of new atmospheric particles by nitric acid and ammonia condensation
- 2020
-
Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 581:7807, s. 184-
-
Tidskriftsartikel (refereegranskat)abstract
- A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog(1,2), but how it occurs in cities is often puzzling(3). If the growth rates of urban particles are similar to those found in cleaner environments (1-10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below -15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid-base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms(4,5).
|
|
| 18. |
- Yli-Juuti, Taina, et al.
(författare)
-
Effect Of Salt Formation On Condensation Of Organic Compounds On Atmospheric Nanoparticles
- 2013
-
Ingår i: NUCLEATION AND ATMOSPHERIC AEROSOLS. - : AIP. - 9780735411524 ; , s. 445-448
-
Konferensbidrag (refereegranskat)abstract
- Freshly formed atmospheric nanoparticles have been observed to contain also such organic compounds which have too high saturation vapor pressure to condense on nanoparticles reversibly. The condensation of these compounds on the particles may be facilitated by particle phase processes that transform the compounds into less-volatile form. Here we use particle growth model MABNAG to study the effect of particle phase acid-base chemistry on the condensation of organic acids and bases.
|
|
| 19. |
- Yli-Juuti, Taina, et al.
(författare)
-
Volatility of Organic Aerosol : Evaporation of Ammonium Sulfate/Succinic Acid Aqueous Solution Droplets
- 2013
-
Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:21, s. 12123-12130
-
Tidskriftsartikel (refereegranskat)abstract
- Condensation and evaporation modify the properties and effects of atmospheric aerosol particles. We studied the evaporation of aqueous succinic acid and succinic acid/ammonium sulfate droplets to obtain insights on the effect of ammonium sulfate on the gas/particle partitioning of atmospheric organic acids. Droplet evaporation in a laminar flow tube was measured in a Tandem Differential Mobility Analyzer setup. A wide range of droplet compositions was investigated, and for some of the experiments the composition was tracked using an Aerosol Mass Spectrometer. The measured evaporation was compared to model predictions where the ammonium sulfate was assumed not to directly affect succinic acid evaporation. The model captured the evaporation rates for droplets with large organic content but overestimated the droplet size change when the molar concentration of succinic acid was similar to or lower than that of ammonium sulfate, suggesting that ammonium sulfate enhances the partitioning of dicarboxylic acids to aqueous particles more than currently expected from simple mixture thermodynamics. If extrapolated to the real atmosphere, these results imply enhanced partitioning of secondary organic compounds to particulate phase in environments dominated by inorganic aerosol.
|
|
| 20. |
- Ylisirniö, Arttu, et al.
(författare)
-
Composition and volatility of secondary organic aerosol (SOA) formed from oxidation of real tree emissions compared to simplified volatile organic compound (VOC) systems
- 2020
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:9, s. 5629-5644
-
Tidskriftsartikel (refereegranskat)abstract
- Secondary organic aerosol (SOA) is an important constituent of the atmosphere where SOA particles are formed chiefly by the condensation or reactive uptake of oxidation products of volatile organic compounds (VOCs). The mass yield in SOA particle formation, as well as the chemical composition and volatility of the particles, is determined by the identity of the VOC precursor(s) and the oxidation conditions they experience. In this study, we used an oxidation flow reactor to generate biogenic SOA from the oxidation of Scots pine emissions. Mass yields, chemical composition and volatility of the SOA particles were characterized and compared with SOA particles formed from oxidation of alpha-pinene and from a mixture of acyclic-monocyclic sesquiterpenes (farnesenes and bisabolenes), which are significant components of the Scots pine emissions. SOA mass yields for Scots pine emissions dominated by farnesenes were lower than for a-pinene but higher than for the artificial mixture of farne-senes and bisabolenes. The reduction in the SOA yield in the farnesene- and bisabolene-dominated mixtures is due to exocyclic C =C bond scission in these acyclic-monocyclic sesquiterpenes during ozonolysis leading to smaller and generally more volatile products. SOA particles from the oxi- dation of Scots pine emissions had similar or lower volatility than SOA particles formed from either a single precursor or a simple mixture of VOCs. Applying physical stress to the Scots pine plants increased their monoterpene, especially monocyclic beta-phellandrene, emissions, which further decreased SOA particle volatility and increased SOA mass yield. Our results highlight the need to account for the chemical complexity and structure of real-world biogenic VOC emissions and stress-induced changes to plant emissions when modelling SOA production and properties in the atmosphere. These results emphasize that a simple increase or decrease in relative monoterpene and sesquiterpene emissions should not be used as an indicator of SOA particle volatility.
|
|
