Contribution of Atmospheric Oxygenated Organic Compounds to Particle Growth in an Urban Environment

2021 ◽  
Author(s):  
Xiaohui Qiao ◽  
Chao Yan ◽  
Xiaoxiao Li ◽  
YiShuo Guo ◽  
Rujing Yin ◽  
...  
Keyword(s):  
Urban Environment ◽  
Organic Compounds ◽  
Particle Growth

Volatile organic compounds in an urban environment: a comparison among Belgium, Vietnam and Ethiopia

2013 ◽  
Vol 93 (3) ◽  
pp. 298-314 ◽  
Author(s):  
Duc Hoai Do ◽  
Herman Van Langenhove ◽  
Christophe Walgraeve ◽  
Samuel Fekadu Hayleeyesus ◽  
Patrick De Wispelaere ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Urban Environment ◽  
Organic Compounds ◽  
Volatile Organic

scholarly journals Observation of new particle formation in subtropical urban environment

2011 ◽  
Vol 11 (8) ◽  
pp. 3823-3833 ◽  
Author(s):  
H. C. Cheung ◽  
L. Morawska ◽  
Z. D. Ristovski
Keyword(s):  
Growth Rate ◽  
Urban Environment ◽  
Size Distribution ◽  
Particle Number ◽  
Particle Growth ◽  
Particle Formation ◽  
Number Concentration ◽  
Particle Number Concentration ◽  
Industrial Emissions ◽  
Traffic Exhaust

Abstract. The aim of this study was to characterise the new particle formation events in a subtropical urban environment in the Southern Hemisphere. The study measured the number concentration of particles and its size distribution in Brisbane, Australia during 2009. The variation of particle number concentration and nucleation burst events were characterised as well as the particle growth rate which was first reported in urban environment of Australia. The annual average NUFP, NAitken and NNuc were 9.3×103, 3.7×103 and 5.6×103 cm−3, respectively. Weak seasonal variation in number concentration was observed. Local traffic exhaust emissions were a major contributor of the pollution (NUFP) observed in morning which was dominated by the Aitken mode particles, while particles formed by secondary formation processes contributed to the particle number concentration during afternoon. Overall, 65 nucleation burst events were identified during the study period. Nucleation burst events were classified into two groups, with and without particles growth after the burst of nucleation mode particles observed. The average particle growth rate of the nucleation events was 4.6 nm h−1 (ranged from 1.79–7.78 nm h−1). Case studies of the nucleation burst events were characterised including (i) the nucleation burst with particle growth which is associated with the particle precursor emitted from local traffic exhaust emission, (ii) the nucleation burst without particle growth which is due to the transport of industrial emissions from the coast to Brisbane city or other possible sources with unfavourable conditions which suppressed particle growth and (iii) interplay between the above two cases which demonstrated the impact of the vehicle and industrial emissions on the variation of particle number concentration and its size distribution during the same day.

scholarly journals Probing key organic substances driving new particle growth initiated by iodine nucleation in coastal atmosphere

2020 ◽  
Vol 20 (16) ◽  
pp. 9821-9835
Author(s):  
Yibei Wan ◽  
Xiangpeng Huang ◽  
Bin Jiang ◽  
Binyu Kuang ◽  
Manfei Lin ◽  
...  
Keyword(s):  
Organic Compounds ◽  
Unsaturated Fatty Acids ◽  
Cloud Condensation Nuclei ◽  
Deep Understanding ◽  
Surface Group ◽  
Particle Growth ◽  
Biologically Active ◽  
Ion Cyclotron Resonance ◽  
20 Nm ◽  
Ft Icr Ms

Abstract. Unlike the deep understanding of highly oxygenated organic molecules (HOMs) driving continental new particle formation (NPF), little is known about the organic compounds involved in coastal and open-ocean NPF. On the coastline of China we observed intense coastal NPF events initiated by iodine nucleation, but particle growth to cloud condensation nuclei (CCN) sizes was dominated by organic compounds. This article reveals a new group of C18,30HhOoNn and C20,24,28,33HhOo compounds with specific double-bond equivalents and oxygen atom numbers in new sub 20 nm coastal iodine particles by using ultrahigh-resolution Fourier transform–ion cyclotron resonance mass spectrometry (FT-ICR-MS). We proposed these compounds are oxygenated or nitrated products of long-chain unsaturated fatty acids, fatty alcohols, nonprotein amino acids or amino alcohols emitted mutually with iodine from coastal biota or biologically active sea surface. Group contribution method estimated that the addition of –ONO2, –OH and –C=O groups to the precursors reduced their volatility by 2–7 orders of magnitude and thus made their products condensable onto new iodine particles in the coastal atmosphere. Nontarget MS analysis also provided a list of 440 formulas of iodinated organic compounds in size-resolved aerosol samples during the iodine NPF days, which facilitates the understanding of unknown aerosol chemistry of iodine.

scholarly journals Model for acid-base chemistry in nanoparticle growth (MABNAG)

2013 ◽  
Vol 13 (3) ◽  
pp. 7175-7222 ◽  
Author(s):  
T. Yli-Juuti ◽  
K. Barsanti ◽  
L. Hildebrandt Ruiz ◽  
A.-J. Kieloaho ◽  
U. Makkonen ◽  
...  
Keyword(s):  
Particle Size ◽  
Sulfuric Acid ◽  
Gas Phase ◽  
Organic Compounds ◽  
Particle Growth ◽  
Particle Phase ◽  
Vapor Pressures ◽  
Salt Formation ◽  
Acid Base ◽  
Nanoparticle Growth

Abstract. Climatic effects of newly-formed atmospheric secondary aerosol particles are to a large extent determined by their condensational growth rates. However, all the vapors condensing on atmospheric nanoparticles and growing them to climatically relevant sizes are not identified yet and the effects of particle phase processes on particle growth rates are poorly known. Besides sulfuric acid, organic compounds are known to contribute significantly to atmospheric nanoparticle growth. In this study a particle growth model MABNAG (Model for Acid-Base chemistry in NAnoparticle Growth) was developed to study the effect of salt formation on nanoparticle growth, which has been proposed as a potential mechanism lowering the equilibrium vapor pressures of organic compounds through dissociation in the particle phase and thus preventing their evaporation. MABNAG is a model for monodisperse aqueous particles and it couples dynamics of condensation to particle phase chemistry. Non-zero equilibrium vapor pressures, with both size and composition dependence, are considered for condensation. The model was applied for atmospherically relevant systems with sulfuric acid, one organic acid, ammonia, one amine and water in the gas phase allowed to condense on 3–20 nm particles. The effect of dissociation of the organic acid was found to be small under ambient conditions typical for a boreal forest site, but considerable for base-rich environments (gas phase concentrations of about 1010 cm−3 for the sum of the bases). The contribution of the bases to particle mass decreased as particle size increased, except at very high gas phase concentrations of the bases. The relative importance of amine versus ammonia did not change significantly as a function of particle size. While our results give a reasonable first estimate on the maximum contribution of salt formation to nanoparticle growth, further studies on, e.g. the thermodynamic properties of the atmospheric organics, concentrations of low-volatility organic acids and amines, along with studies investigating the applicability of thermodynamics for the smallest nanoparticles are needed to truly understand the acid-base chemistry of atmospheric nanoparticles.

scholarly journals The roles of sulfuric acid in new particle formation and growth in the mega-city of Beijing

2010 ◽  
Vol 10 (10) ◽  
pp. 4953-4960 ◽  
Author(s):  
D. L. Yue ◽  
M. Hu ◽  
R. Y. Zhang ◽  
Z. B. Wang ◽  
J. Zheng ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Organic Compounds ◽  
Dominant Role ◽  
Formation Rate ◽  
Particle Growth ◽  
Particle Formation ◽  
New Particle Formation ◽  
Average Formation ◽  
Subsequent Neutralization

Abstract. 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.

scholarly journals Molecular insights into new particle formation in Barcelona, Spain

2020 ◽  
Vol 20 (16) ◽  
pp. 10029-10045 ◽  
Author(s):  
James Brean ◽  
David C. S. Beddows ◽  
Zongbo Shi ◽  
Brice Temime-Roussel ◽  
Nicolas Marchand ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Organic Compounds ◽  
Radiative Forcing ◽  
Cloud Condensation Nuclei ◽  
Sulfuric Acid Concentration ◽  
Particle Growth ◽  
Particle Formation ◽  
Necessary Condition ◽  
New Particle Formation ◽  
High Concentrations

Abstract. Atmospheric aerosols contribute some of the greatest uncertainties to estimates of global radiative forcing and have significant effects on human health. New particle formation (NPF) is the process by which new aerosols of sub-2 nm diameter form from gas-phase precursors and contributes significantly to particle numbers in the atmosphere, accounting for approximately 50 % of cloud condensation nuclei globally. Here, we study summertime NPF in urban Barcelona in north-eastern Spain utilising particle counting instruments down to 1.9 nm and a Nitrate Chemical Ionisation Atmospheric Pressure interface Time of Flight Mass Spectrometer (CI-APi-ToF). The rate of formation of new particles is seen to increase linearly with sulfuric acid concentration, although particle formation rates fall short of chamber studies of H2SO4–DMA–H2O while exceeding those of H2SO4–BioOxOrg–H2O nucleation, although a role of highly oxygenated molecules (HOMs) cannot be ruled out. The sulfuric acid dimer : monomer ratio is significantly lower than that seen in experiments involving sulfuric acid and dimethylamine (DMA) in chambers, indicating that stabilisation of sulfuric acid clusters by bases is weaker in this dataset than in chambers, either due to rapid evaporation due to high summertime temperatures or limited pools of stabilising amines. Such a mechanism cannot be verified in these data, as no higher-order H2SO4–amine clusters nor H2SO4–HOM clusters were measured. The high concentrations of HOMs arise from isoprene, alkylbenzene, monoterpene and polycyclic aromatic hydrocarbon (PAH) oxidation, with alkylbenzenes providing greater concentrations of HOMs due to significant local sources. The concentration of these HOMs shows a dependence on temperature. The organic compounds measured primarily fall into the semivolatile organic compound (SVOC) volatility class arising from alkylbenzene and isoprene oxidation. Low-volatility organic compounds (LVOCs) largely arise from oxidation of alkylbenzenes, PAHs and monoterpenes, whereas extremely low-volatility organic compounds (ELVOCs) arise from primarily PAH and monoterpene oxidation. New particle formation without growth past 10 nm is also observed, and on these days oxygenated organic concentrations are lower than on days with growth by a factor of 1.6, and thus high concentrations of low-volatility oxygenated organics which primarily derive from traffic-emitted volatile organic compounds (VOCs) appear to be a necessary condition for the growth of newly formed particles in Barcelona. These results are consistent with prior observations of new particle formation from sulfuric acid–amine reactions in both chambers and the real atmosphere and are likely representative of the urban background of many European Mediterranean cities. A role for HOMs in the nucleation process cannot be confirmed or ruled out, and there is strong circumstantial evidence of the participation of HOMs across multiple volatility classes in particle growth.

A minimum set of ozone precursor volatile organic compounds in an urban environment

2018 ◽  
Vol 9 (2) ◽  
pp. 369-378 ◽  
Author(s):  
Cleyton M. da Silva ◽  
Luane L. da Silva ◽  
Sergio M. Corrêa ◽  
Graciela Arbilla
Keyword(s):  
Volatile Organic Compounds ◽  
Urban Environment ◽  
Organic Compounds ◽  
Volatile Organic ◽  
Ozone Precursor

scholarly journals Model for acid-base chemistry in nanoparticle growth (MABNAG)

2013 ◽  
Vol 13 (24) ◽  
pp. 12507-12524 ◽  
Author(s):  
T. Yli-Juuti ◽  
K. Barsanti ◽  
L. Hildebrandt Ruiz ◽  
A.-J. Kieloaho ◽  
U. Makkonen ◽  
...  
Keyword(s):  
Particle Size ◽  
Sulfuric Acid ◽  
Gas Phase ◽  
Organic Compounds ◽  
Growth Rates ◽  
Particle Growth ◽  
Particle Phase ◽  
Salt Formation ◽  
Acid Base ◽  
Nanoparticle Growth

Abstract. Climatic effects of newly-formed atmospheric secondary aerosol particles are to a large extent determined by their condensational growth rates. However, all the vapours condensing on atmospheric nanoparticles and growing them to climatically relevant sizes are not identified yet and the effects of particle phase processes on particle growth rates are poorly known. Besides sulfuric acid, organic compounds are known to contribute significantly to atmospheric nanoparticle growth. In this study a particle growth model MABNAG (Model for Acid-Base chemistry in NAnoparticle Growth) was developed to study the effect of salt formation on nanoparticle growth, which has been proposed as a potential mechanism lowering the equilibrium vapour pressures of organic compounds through dissociation in the particle phase and thus preventing their evaporation. MABNAG is a model for monodisperse aqueous particles and it couples dynamics of condensation to particle phase chemistry. Non-zero equilibrium vapour pressures, with both size and composition dependence, are considered for condensation. The model was applied for atmospherically relevant systems with sulfuric acid, one organic acid, ammonia, one amine and water in the gas phase allowed to condense on 3–20 nm particles. The effect of dissociation of the organic acid was found to be small under ambient conditions typical for a boreal forest site, but considerable for base-rich environments (gas phase concentrations of about 1010 cm−3 for the sum of the bases). The contribution of the bases to particle mass decreased as particle size increased, except at very high gas phase concentrations of the bases. The relative importance of amine versus ammonia did not change significantly as a function of particle size. While our results give a reasonable first estimate on the maximum contribution of salt formation to nanoparticle growth, further studies on, e.g. the thermodynamic properties of the atmospheric organics, concentrations of low-volatility organics and amines, along with studies investigating the applicability of thermodynamics for the smallest nanoparticles are needed to truly understand the acid-base chemistry of atmospheric nanoparticles.

scholarly journals Development of a protocol for the auto-generation of explicit aqueous-phase oxidation schemes of organic compounds

2019 ◽  
Vol 19 (14) ◽  
pp. 9209-9239 ◽  
Author(s):  
Peter Bräuer ◽  
Camille Mouchel-Vallon ◽  
Andreas Tilgner ◽  
Anke Mutzel ◽  
Olaf Böge ◽  
...  
Keyword(s):  
Organic Compounds ◽  
Aqueous Phase ◽  
Rate Constants ◽  
Particle Growth ◽  
Chemical Mechanism ◽  
Estimation Methods ◽  
Radical Reactivity ◽  
Chemical Complexity ◽  
Model Studies ◽  
Phase Chemistry

Abstract. This paper presents a new CAPRAM–GECKO-A protocol for mechanism auto-generation of aqueous-phase organic processes. For the development, kinetic data in the literature were reviewed and a database with 464 aqueous-phase reactions of the hydroxyl radical with organic compounds and 130 nitrate radical reactions with organic compounds has been compiled and evaluated. Five different methods to predict aqueous-phase rate constants have been evaluated with the help of the kinetics database: gas–aqueous phase correlations, homologous series of various compound classes, radical reactivity comparisons, Evans–Polanyi-type correlations, and structure–activity relationships (SARs). The quality of these prediction methods was tested as well as their suitability for automated mechanism construction. Based on this evaluation, SARs form the basis of the new CAPRAM–GECKO-A protocol. Evans–Polanyi-type correlations have been advanced to consider all available H atoms in a molecule besides the H atoms with only the weakest bond dissociation enthalpies (BDEs). The improved Evans–Polanyi-type correlations are used to predict rate constants for aqueous-phase NO3 and organic compounds reactions. Extensive tests have been performed on essential parameters and on highly uncertain parameters with limited experimental data. These sensitivity studies led to further improvements in the new CAPRAM–GECKO-A protocol but also showed current limitations. Biggest uncertainties were observed in uptake processes and the estimation of Henry's law coefficients as well as radical chemistry, in particular the degradation of alkoxy radicals. Previous estimation methods showed several deficits, which impacted particle growth. For further evaluation, a 1,3,5-trimethylbenzene oxidation experiment has been performed in the aerosol chamber “Leipziger Aerosolkammer” (LEAK) at high relative humidity conditions and compared to a multiphase mechanism using the Master Chemical Mechanism (MCMv3.2) in the gas phase and using a methylglyoxal oxidation scheme of about 600 reactions generated with the new CAPRAM–GECKO-A protocol in the aqueous phase. While it was difficult to evaluate single particle constituents due to concentrations close to the detection limits of the instruments applied, the model studies showed the importance of aqueous-phase chemistry in respect to secondary organic aerosol (SOA) formation and particle growth. The new protocol forms the basis for further CAPRAM mechanism development towards a new version 4.0. Moreover, it can be used as a supplementary tool for aerosol chambers to design and analyse experiments of chemical complexity and help to understand them on a molecular level.

scholarly journals Analysis of new particle formation (NPF) events at nearby rural, urban background and urban roadside sites

2019 ◽  
Vol 19 (8) ◽  
pp. 5679-5694 ◽  
Author(s):  
Dimitrios Bousiotis ◽  
Manuel Dall'Osto ◽  
David C. S. Beddows ◽  
Francis D. Pope ◽  
Roy M. Harrison
Keyword(s):  
Urban Environment ◽  
Growth Rates ◽  
General Pattern ◽  
Particle Growth ◽  
Particle Formation ◽  
Atmospheric Conditions ◽  
New Particle Formation ◽  
Urban Background ◽  
Air Masses ◽  
Condensation Sink

Abstract. New particle formation (NPF) events have different patterns of development depending on the conditions of the area in which they occur. In this study, particle size distributions in the range of 16.6–604 nm (7 years of data) were analysed and NPF events occurring at three sites of differing characteristics – rural Harwell (HAR), urban background North Kensington (NK), urban roadside Marylebone Road (MR), London, UK – were extracted and studied. The different atmospheric conditions in each study area not only have an effect on the frequency of the events, but also affect their development. The frequency of NPF events is similar at the rural and urban background locations (about 7 % of days), with a high proportion of events occurring at both sites on the same day (45 %). The frequency of NPF events at the urban roadside site is slightly less (6 % of days), and higher particle growth rates (average 5.5 nm h−1 at MR compared to 3.4 and 4.2 nm h−1 at HAR and NK respectively) must result from rapid gas-to-particle conversion of traffic-generated pollutants. A general pattern is found in which the condensation sink increases with the degree of pollution of the site, but this is counteracted by increased particle growth rates at the more polluted location. A key finding of this study is that the role of the urban environment leads to an increment of 20 % in N16–20 nm in the urban background compared to that of the rural area in NPF events occurring at both sites. The relationship of the origin of incoming air masses is also considered and an association of regional events with cleaner air masses is found. Due to lower availability of condensable species, NPF events that are associated with cleaner atmospheric conditions have lower growth rates of the newly formed particles. The decisive effect of the condensation sink in the development of NPF events and the survivability of the newly formed particles is underlined, and influences the overall contribution of NPF events to the number of ultrafine particles in an area. The other key factor identified by this study is the important role that pollution, both from traffic and other sources in the urban environment (such as heating or cooking), plays in new particle formation events.

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