scholarly journals Hydration of the Sulfuric Acid–Methylamine Complex and Implications for Aerosol Formation

2014 ◽  
Vol 118 (35) ◽  
pp. 7430-7441 ◽  
Author(s):  
Danielle J. Bustos ◽  
Berhane Temelso ◽  
George C. Shields

2021 ◽  
pp. 53-60
Author(s):  
A. E. Aloyan ◽  
◽  
A. N. Yermakov ◽  
V. O. Arutyunyan ◽  
◽  
...  

The results of one-dimensional calculations of the height profiles of nucleated sulfate aerosol particles for the northern mid-latitudes and tropics in winter are presented. Numerical calculations were performed using a three-dimensional model of the transport and transformation of multicompo- nent gas and aerosol substances in the atmosphere, incorporating photochemistry, nucleation involving neutral molecules and ions, as well as condensation/evaporation and coagulation. It is found that the resulting dynamics of the formation of aerosol particle nuclei is not a simple sum of ion and binary (water vapor/sulfuric acid) nucleation rates. This dynamics is determined by the ratio of critical radii of nucleated particles due to binary and ion nucleation of these substances (rcr_bin and rcr_ion) depending on temperature, relative humidity, and ionization rate. This should be taken into account in modeling the gas and aerosol composition of the atmosphere and comparing calculated and observed data.



2016 ◽  
Vol 16 (4) ◽  
pp. 1955-1970 ◽  
Author(s):  
M. Dal Maso ◽  
L. Liao ◽  
J. Wildt ◽  
A. Kiendler-Scharr ◽  
E. Kleist ◽  
...  

Abstract. Aerosol formation from biogenic and anthropogenic precursor trace gases in continental background areas affects climate via altering the amount of available cloud condensation nuclei. Significant uncertainty still exists regarding the agents controlling the formation of aerosol nanoparticles. We have performed experiments in the Jülich plant–atmosphere simulation chamber with instrumentation for the detection of sulfuric acid and nanoparticles, and present the first simultaneous chamber observations of nanoparticles, sulfuric acid, and realistic levels and mixtures of biogenic volatile compounds (BVOCs). We present direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We directly measured particle formation rates separately from particle growth rates. From this, we established that in our experiments, the formation rate was proportional to the product of sulfuric acid and biogenic VOC emission strength. The formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid. The growth rate of nanoparticles immediately after birth was best correlated with estimated products resulting from BVOC ozonolysis.



1998 ◽  
Vol 29 ◽  
pp. S87-S88
Author(s):  
Martin Wilck ◽  
Frank Stratmann ◽  
Lars Asbjørn Larsen ◽  
Rita Van Dingenen ◽  
Frank Raes


2020 ◽  
Author(s):  
Xiaojing Shen ◽  
Junying Sun ◽  
Fangqun Yu ◽  
Xiaoye Zhang ◽  
Junting Zhong ◽  
...  

Abstract. Influenced by the spread of the global 2019 novel coronavirus (COVID-19) pandemic, primary emissions of particles and precursors associated with anthropogenic activities decreased significantly in China during the Chinese New Year of 2020 and the lockdown period (January 24–February 16, 2020), as indicated by approximately 50 % reduction of NOx emission nation-wide based on the open literature. Two-month measurements of the number size distribution of neutral particles and charged ions showed that during the lockdown (LCD) period, the number concentration of particles smaller than 100 nm decreased by approximately 40 % compared to the pre-LCD period in January. However, the accumulation mode particles increased by approximately 20 % as several polluted episodes contributed to secondary aerosol formation. In this study, new particle formation (NPF) events were found to be enhanced in the nucleation and growth processes during the LCD period, as indicated by higher formation (J2) and growth rate (GR), even as NPF occurrence frequency slightly decreased. The condensing vapors controlling the nucleation and growth process, sulfuric acid, and oxidation product of volatile organic compounds were estimated based on available information. The proxy values showed that sulfuric acid and organic oxidized vapors increased during the LCD period by approximately 35 % and 133 % on NPF days, respectively. Higher J2 and GR during the LCD period were favored by the increased concentration level of condensing vapors and decreased condensation sink. Several heavy haze episodes have been reported by other studies during the LCD period; however, the increase in nanoparticle number concentration should also be considered. Some typical NPF events produced a high number concentration of nanoparticles that intensified in the following days to create severe aerosol pollution. Our study confirms a significant enhancement of the nucleation and growth process of nanoparticles during the COVID-19 LCD in Beijing and highlights the necessity of controlling nanoparticles in current and future air quality management.



2021 ◽  
Author(s):  
Narcisse Tsona Tchinda ◽  
Lin Du ◽  
Ling Liu ◽  
Xiuhui Zhang

Abstract. The role of pyruvic acid (PA), one of the most abundant α-keto carboxylic acids in the atmosphere, was investigated both in the SO3 hydrolysis reaction to form sulfuric acid (SA) and in SA-based aerosol particle formation using quantum chemical calculations and a cluster dynamics model. We found that the PA-catalyzed SO3 hydrolysis is a thermodynamically driven transformation process, proceeding with a negative Gibbs free energy barrier, ca. −1 kcal mol−1 at 298 K, ~6.50 kcal mol−1 lower than that in the water-catalyzed SO3 hydrolysis. Results indicated that the PA-catalyzed reaction can potentially compete with the water-catalyzed SO3 reaction in SA production, especially in dry and polluted areas, where it is found to be ~two orders of magnitude more efficient that the water-catalyzed reaction. Given the effective stabilization of the PA-catalyzed SO3 hydrolysis product as SA•PA cluster, we proceeded to examine the PA clustering efficiency in sulfuric acid-pyruvic acid-ammonia (SA-PA-NH3) system. Our thermodynamic data used in the Atmospheric Cluster Dynamics Code indicated that under relevant tropospheric temperatures and concentrations of SA (106 cm3), PA (1010 cm3) and NH3 (1011 and 5 × 1011 cm3), of the PA-containing clusters, only clusters with one PA molecule, namely (SA)2•PA•(NH3)2, can participate to the particle formation, contributing by ~100 % to the net flux to aerosol particle formation at 238 K, exclusively. At higher temperatures (258 K and 278 K), however, the net flux to the particle formation is dominated by pure SA-NH3 clusters, while PA would rather evaporate from the clusters at high temperatures and not contribute to the particle formation. The enhancing effect of PA of examined by evaluating the ratio of the ternary SA-PA-NH3 cluster formation rate to binary SA-NH3 cluster formation rate. Our results show that while the enhancement factor of PA to the particle formation rate is almost insensitive to investigated temperatures and concentrations, it can be as high as 4.7 × 102 at 238 K and [NH3] = 1.3 × 1011 molecule cm−3. This indicates that PA may actively participate in aerosol formation, only in cold regions of the troposphere and highly NH3-polluted environments. The inclusion of this mechanism in aerosol models may definitely reduce uncertainties that prevail in modeling the aerosol impact on climate.



2021 ◽  
Author(s):  
Tuija Jokinen ◽  
Katrianne Lehtipalo ◽  
Kimmo Neitola ◽  
Nina Sarnela ◽  
Totti Laitinen ◽  
...  

<p>One way to form aerosol particles is the condensation of oxidized atmospheric trace gases, such as sulfuric acid (SA) into small molecular clusters. After growing to larger particles by condensation of low volatile gases, they can affect the planets climate directly by scattering light and indirectly by acting as cloud condensation nuclei. Observations of low-volatility aerosol precursor gases have been reported around the world but long-term measurement series and Arctic data sets showing seasonal variation are close to non-existent. In here, we present ~7 months of aerosol precursor gas measurements performed with the nitrate based chemical ionization mass spectrometer (CI-APi-TOF). We deployed our measurements ~250 km above the Arctic Circle at the Finnish sub-Arctic field station, SMEAR I in Värriö. We report concentration measurements of the most common new particle formation related compounds; sulfuric acid, methanesulfonic acid (MSA), iodic acid (IA) and highly oxygenated organic compounds, HOMs. At this remote measurement site, surrounded by a strict nature preserve, that gets occasional pollution from a Russian city of Murmansk, SA is originated both from anthropogenic and biological sources and has a clear diurnal cycle but no significant seasonal variation, while MSA as an oxidation product of purely biogenic sources is showing a more distinct seasonal cycle. Iodic acid concentrations are the most stable throughout the measurement period, showing almost identical peak concentrations for spring, summer and autumn. HOMs are abundant during the summer months and due to their high correlation with ambient air temperature, we suggest that most of HOMs are products of monoterpene oxidation. New particle formation events at SMEAR I happen under relatively low temperatures, low relative humidity, high ozone concentration, high SA concentration in the morning and high MSA concentrations in the afternoon. The role of HOMs in aerosol formation will be discussed. All together, these are the first long term measurements of aerosol forming precursor from the sub-arctic region helping us to understand atmospheric chemical processes and aerosol formation in the rapidly changing Arctic.</p><p> </p><p> </p>





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