scholarly journals Investigation of the connections between atmospheric new particle formation and organics at an urban site of Beijing

2013 ◽  
Vol 13 (2) ◽  
pp. 3419-3450 ◽  
Author(s):  
Z. B. Wang ◽  
M. Hu ◽  
Z. J. Wu ◽  
D. L. Yue ◽  
J. Zheng ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Correlation Coefficients ◽  
Particle Formation ◽  
Nucleation Theory ◽  
Urban Site ◽  
New Particle Formation ◽  
Organic Vapors ◽  
Data Set ◽  
High Background ◽  
Nucleation Mechanisms

Abstract. The role of low-volatility organic vapors in atmospheric new particle formation has been studied based on a data set of 17 nucleation events observed during the CAREBeijing 2008 campaign. The particle formation rates show good correlations with sulfuric acid and organic vapors implying that both play an important role in the atmospheric new particle formation. High correlation coefficients are observed in all investigated nucleation mechanisms. The best fit (R = 0.73, slope = 1.1) between the observed and modelled particle formation rates is achieved with the homogenous nucleation theory of sulfuric acid (both homomolecularly and hetermolecularly) with separate coefficients in J=KSA1[H2SO4]2+KSA2[H2SO4][Org]. The contributions of the sulfuric acid and the organics involving terms have been 43% and 57%, respectively. In addition, the higher particle formation rates are observed on polluted nucleation days, indicating the organic vapors should be involved in the new particle formation process in the polluted urban environment of Beijing with high background aerosol loading.

scholarly journals Climatology of new particle formation at Izaña mountain GAW observatory in the subtropical North Atlantic

2014 ◽  
Vol 14 (8) ◽  
pp. 3865-3881 ◽  
Author(s):  
M. I. García ◽  
S. Rodríguez ◽  
Y. González ◽  
R. D. García
Keyword(s):  
Sulfuric Acid ◽  
North Atlantic ◽  
Growth Rates ◽  
Particle Growth ◽  
Particle Formation ◽  
Dust Particles ◽  
New Particle Formation ◽  
Data Set ◽  
Mean Values ◽  
Condensation Sink

Abstract. A climatology of new particle formation (NPF) events at high altitude in the subtropical North Atlantic is presented. A 4-year data set (June 2008–June 2012), which includes number size distributions (10–600 nm), reactive gases (SO2, NOx, and O3), several components of solar radiation and meteorological parameters, measured at Izaña Global Atmosphere Watch (GAW) observatory (2373 m above sea level; Tenerife, Canary Islands) was analysed. NPF is associated with the transport of gaseous precursors from the boundary layer by orographic buoyant upward flows that perturb the low free troposphere during daytime. On average, 30% of the days contained an NPF event. Mean values of the formation and growth rates during the study period were 0.46 cm−3 s−1 and 0.42 nm h−1, correspondingly. There is a clearly marked NPF season (May–August), when these events account for 50–60% of the days per month. Monthly mean values of the formation and growth rates exhibit higher values in this season, 0.49–0.92 cm−3 s−1 and 0.48–0.58 nm h−1, respectively. During NPF events, SO2, UV radiation and upslope winds showed higher values than during non-events. The overall data set indicates that SO2 plays a key role as precursor, although other species seem to contribute during some periods. Condensation of sulfuric acid vapour accounts for most of the measured particle growth during most of the year (~70%), except for some periods. In May, the highest mean growth rates (~0.6 nm h−1) and the lowest contribution of sulfuric acid (~13%) were measured, suggesting a significant involvement of other condensing vapours. The SO2 availability seems also to be the most influencing parameter in the year-to-year variability in the frequency of NPF events. The condensation sink showed similar features to other mountain sites, showing high values during NPF events. Summertime observations, when Izaña is within the Saharan Air Layer, suggest that dust particles may play a significant role acting as coagulation sink of freshly formed nucleation particles. The contribution of dust particles to the condensation sink of sulfuric acid vapours seems to be modest (~8% as average). Finally, we identified a set of NPF events in which two nucleation modes, which may evolve at different rates, occur simultaneously and for which further investigations are necessary.

scholarly journals Evaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case

2011 ◽  
Vol 11 (8) ◽  
pp. 24165-24189 ◽  
Author(s):  
Z. B. Wang ◽  
M. Hu ◽  
D. L. Yue ◽  
J. Zheng ◽  
R. Y. Zhang ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Particle Number ◽  
Particle Formation ◽  
Urban Atmosphere ◽  
Limiting Factors ◽  
New Particle Formation ◽  
H2so4 Concentration ◽  
Nucleation Mechanisms ◽  
Better Than

Abstract. New particle formation (NPF) is considered as an important mechanism for gas-to-particle transformation, and gaseous sulfuric acid is believed as a curcial 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 the condensation sink of pre-existing particles is one of the limiting factors to determine the occurrence of nucleation 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 was adopted to explore the nucleation mechanism. The exponents range from 1 to 5. 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.

scholarly journals An improved criterion for new particle formation in diverse atmospheric environments

2010 ◽  
Vol 10 (17) ◽  
pp. 8469-8480 ◽  
Author(s):  
C. Kuang ◽  
I. Riipinen ◽  
S.-L. Sihto ◽  
M. Kulmala ◽  
A. V. McCormick ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Growth Rates ◽  
Particle Growth ◽  
Particle Formation ◽  
Balance Model ◽  
New Particle Formation ◽  
Data Set ◽  
Surface Areas ◽  
Recent Developments ◽  
Diverse Data

Abstract. A dimensionless theory for new particle formation (NPF) was developed, using an aerosol population balance model incorporating recent developments in nucleation rates and measured particle growth rates. Based on this theoretical analysis, it was shown that a dimensionless parameter LΓ, characterizing the ratio of the particle scavenging loss rate to the particle growth rate, exclusively determined whether or not NPF would occur on a particular day. This parameter determines the probability that a nucleated particle will grow to a detectable size before being lost by coagulation with the pre-existing aerosol. Cluster-cluster coagulation was shown to contribute negligibly to this survival probability under conditions pertinent to the atmosphere. Data acquired during intensive measurement campaigns in Tecamac (MILAGRO), Atlanta (ANARChE), Boulder, and Hyytiälä (QUEST II, QUEST IV, and EUCAARI) were used to test the validity of LΓ as an NPF criterion. Measurements included aerosol size distributions down to 3 nm and gas-phase sulfuric acid concentrations. The model was applied to seventy-seven NPF events and nineteen non-events (characterized by growth of pre-existing aerosol without NPF) measured in diverse environments with broad ranges in sulfuric acid concentrations, ultrafine number concentrations, aerosol surface areas, and particle growth rates (nearly two orders of magnitude). Across this diverse data set, a nominal value of LΓ=0.7 was found to determine the boundary for the occurrence of NPF, with NPF occurring when LΓ<0.7 and being suppressed when LΓ>0.7. Moreover, nearly 45% of measured LΓ values associated with NPF fell in the relatively narrow range of 0.1

scholarly journals An improved criterion for new particle formation in diverse atmospheric environments

2010 ◽  
Vol 10 (1) ◽  
pp. 491-521 ◽  
Author(s):  
C. Kuang ◽  
I. Riipinen ◽  
S.-L. Sihto ◽  
M. Kulmala ◽  
A. V. McCormick ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Growth Rates ◽  
Particle Growth ◽  
Particle Formation ◽  
Balance Model ◽  
New Particle Formation ◽  
Data Set ◽  
Surface Areas ◽  
Recent Developments ◽  
Diverse Data

Abstract. A dimensionless theory for new particle formation (NPF) was developed, using an aerosol population balance model incorporating recent developments in nucleation rates and measured particle growth rates. Based on this theoretical analysis, it was shown that a dimensionless parameter LΓ, characterizing the ratio of the particle scavenging loss rate to the particle growth rate, exclusively determined whether or not NPF would occur on a particular day. This parameter determines the probability that a nucleated particle will grow to a detectable size before being lost by coagulation with the pre-existing aerosol. Cluster-cluster coagulation was shown to contribute negligibly to this survival probability under conditions pertinent to the atmosphere. Data acquired during intensive measurement campaigns in Tecamac (MILAGRO), Atlanta (ANARChE), Boulder, and Hyytiälä (QUEST II, QUEST IV, and EUCAARI) were used to test the validity of LΓ as an NPF criterion. Measurements included aerosol size distributions down to 3 nm and gas-phase sulfuric acid concentrations. The model was applied to seventy-seven NPF events and nineteen non-events (characterized by growth of pre-existing aerosol without NPF) measured in diverse environments with broad ranges in sulfuric acid concentrations, ultrafine number concentrations, aerosol surface areas, and particle growth rates (nearly two orders of magnitude). Across this diverse data set, a nominal value of LΓ=0.7 was found to determine the boundary for the occurrence of NPF, with NPF occurring when LΓ<0.7 and being suppressed when LΓ> 0.7. Moreover, nearly 45% of measured LΓ values associated with NPF fell in the relatively narrow range of 0.1<LΓ<0.3.

scholarly journals Evaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case

2011 ◽  
Vol 11 (24) ◽  
pp. 12663-12671 ◽  
Author(s):  
Z. B. Wang ◽  
M. Hu ◽  
D. L. Yue ◽  
J. Zheng ◽  
R. Y. Zhang ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Particle Formation ◽  
Urban Atmosphere ◽  
Limiting Factor ◽  
New Particle Formation ◽  
H2so4 Concentration ◽  
Nucleation Mechanisms ◽  
Source And Sink ◽  
Better Than

Abstract. 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.

Secondary new particle formation initiated by sulfuric acid-amine nucleation in Beijing

2021 ◽  
Author(s):  
Runlong Cai ◽  
Chao Yan ◽  
Jun Zheng ◽  
Lin Wang ◽  
Markku Kulmala ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Particle Formation ◽  
Nucleation Theory ◽  
Considerable Proportion ◽  
Free Energy Barrier ◽  
Initial Growth ◽  
New Particle Formation ◽  
Neutral Cluster ◽  
Atmospheric Measurements ◽  
Amine Concentration

&lt;p&gt;Secondary new particle formation is an important source of the number concentration of atmospheric aerosols. Despite relatively high coagulation sinks contributed by pre-existing aerosols, intensive new particle formation occurs frequently in polluted atmospheric environments such as in urban Beijing. Considering the measured concentrations of sulfuric acid and organic compounds, the contrast between the high coagulation sink and the frequent intensive NPF events in urban Beijing indicates an efficient nucleation mechanism. Based on long-term atmospheric measurements conducted at the campus of Beijing University of Chemical Technology, we show that sulfuric acid-amine nucleation is a governing mechanism to initiate new particle formation in urban Beijing. The molecular-level mechanism of sulfuric acid-amine nucleation, especially with low amine concentrations and high aerosol concentrations, are discussed. We present evidence for the existence of the missing amine molecules in the measured H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;-amine clusters. A neutral cluster needs to be ionized before it is detected by a mass spectrometer. Deprotonation or clustering with an additional reagent ion changes the stability of the original neutral cluster. Therefore, the amine molecules in neutral H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;-amine clusters may dissociate before detection. Combining measurements and cluster kinetic simulations, we show that although not directly detected, a considerable proportion of H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; monomers exist in the form of (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;)&lt;sub&gt;1&lt;/sub&gt;(amine)&lt;sub&gt;1&lt;/sub&gt;, where the amine is most likely to be dimethylamine or trimethylamine. The evaporation rate of (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;)&lt;sub&gt;1&lt;/sub&gt;(amine)&lt;sub&gt;1&lt;/sub&gt; is moderate and forming (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;)&lt;sub&gt;1&lt;/sub&gt;(amine)&lt;sub&gt;1&lt;/sub&gt; is a critical step for H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;-amine nucleation. According to nucleation theory, (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;)&lt;sub&gt;1&lt;/sub&gt;(amine)&lt;sub&gt;1&lt;/sub&gt; is the critical cluster at a low amine concentration, whereas H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;-amine nucleation may occur without a free energy barrier at a high amine concentration. The clustering between (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;)&lt;sub&gt;1&lt;/sub&gt;(amine)&lt;sub&gt;1&lt;/sub&gt; and (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;)&lt;sub&gt;n&lt;/sub&gt;(amine)&lt;sub&gt;n&lt;/sub&gt; is a major reaction pathway for the initial growth of H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;-amine clusters. These findings are supported by the measured H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; dimer concentration and its dependencies on amine concentrations and temperature in urban Beijing. Besides, the enhancement of cluster growth rate due to synergy between amines and ammonia are discussed.&lt;/p&gt;

scholarly journals Open ocean and coastal new particle formation from sulfuric acid and amines around the Antarctic Peninsula

2021 ◽  
Author(s):  
James Brean ◽  
Manuel Dall’Osto ◽  
Rafel Simó ◽  
Zongbo Shi ◽  
David C. S. Beddows ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Antarctic Peninsula ◽  
Particle Formation ◽  
Open Ocean ◽  
New Particle Formation ◽  
The Antarctic

Connection of organics to atmospheric new particle formation and growth at an urban site of Beijing

2015 ◽  
Vol 103 ◽  
pp. 7-17 ◽  
Author(s):  
Z.B. Wang ◽  
M. Hu ◽  
X.Y. Pei ◽  
R.Y. Zhang ◽  
P. Paasonen ◽  
...  
Keyword(s):  
Particle Formation ◽  
Urban Site ◽  
New Particle Formation ◽  
Particle Formation And Growth

scholarly journals Modelling studies of HOMs and their contributions to new particle formation and growth: comparison of boreal forest in Finland and a polluted environment in China

2018 ◽  
Vol 18 (16) ◽  
pp. 11779-11791 ◽  
Author(s):  
Ximeng Qi ◽  
Aijun Ding ◽  
Pontus Roldin ◽  
Zhengning Xu ◽  
Putian Zhou ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Boreal Forest ◽  
Environmental Conditions ◽  
Eastern China ◽  
Particle Growth ◽  
Particle Formation ◽  
Forest Site ◽  
Polluted Environment ◽  
New Particle Formation ◽  
Multifunctional Compounds

Abstract. Highly oxygenated multifunctional compounds (HOMs) play a key role in new particle formation (NPF), but their quantitative roles in different environments of the globe have not been well studied yet. Frequent NPF events were observed at two “flagship” stations under different environmental conditions, i.e. a remote boreal forest site (SMEAR II) in Finland and a suburban site (SORPES) in polluted eastern China. The averaged formation rate of 6 nm particles and the growth rate of 6–30 nm particles were 0.3 cm−3 s−1 and 4.5 nm h−1 at SMEAR II compared to 2.3 cm−3 s−1 and 8.7 nm h−1 at SORPES, respectively. To explore the differences of NPF at the two stations, the HOM concentrations and NPF events at two sites were simulated with the MALTE-BOX model, and their roles in NPF and particle growth in the two distinctly different environments are discussed. The model provides an acceptable agreement between the simulated and measured concentrations of sulfuric acid and HOMs at SMEAR II. The sulfuric acid and HOM organonitrate concentrations are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower at SORPES compared to SMEAR II. The model simulates the NPF events at SMEAR II with a good agreement but underestimates the growth of new particles at SORPES, indicating a dominant role of anthropogenic processes in the polluted environment. HOMs from monoterpene oxidation dominate the growth of ultrafine particles at SMEAR II while sulfuric acid and HOMs from aromatics oxidation play a more important role in particle growth. This study highlights the distinct roles of sulfuric acid and HOMs in NPF and particle growth in different environmental conditions and suggests the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas like eastern China.

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