scholarly journals Methanesulfonic Acid-driven New Particle Formation Enhanced by Monoethanolamine: A Computational Study

2019 ◽  
Vol 53 (24) ◽  
pp. 14387-14397 ◽  
Author(s):  
Jiewen Shen ◽  
Hong-Bin Xie ◽  
Jonas Elm ◽  
Fangfang Ma ◽  
Jingwen Chen ◽  
...  
Keyword(s):  
Computational Study ◽  
Methanesulfonic Acid ◽  
Particle Formation ◽  
New Particle Formation

scholarly journals The Role of Oxalic Acid in New Particle Formation from Methanesulfonic Acid, Methylamine, and Water

2017 ◽  
Vol 51 (4) ◽  
pp. 2124-2130 ◽  
Author(s):  
Kristine D. Arquero ◽  
R. Benny Gerber ◽  
Barbara J. Finlayson-Pitts
Keyword(s):  
Oxalic Acid ◽  
Methanesulfonic Acid ◽  
Particle Formation ◽  
New Particle Formation

New Particle Formation Involving Charged Sulfuric Acid – Ammonia Clusters

2020 ◽  
Author(s):  
Vitus Besel ◽  
Jakub Kubečka ◽  
Theo Kurtén ◽  
Hanna Vehkamäki
Keyword(s):  
Sulfuric Acid ◽  
Computational Study ◽  
Cluster Formation ◽  
Chem Phys ◽  
Particle Formation ◽  
Empirical Method ◽  
Particle Nucleation ◽  
New Particle Formation ◽  
Charged Clusters ◽  
Ammonia Clusters

<div> <p>The bulk of aerosol particles in the atmosphere are formed by gas-to-particle nucleation (Merikanto et al., 2009). However, the exact process of single molecules forming cluster, which subsequently can grow into particles, remains largely unknown. Recently, sulfuric acid has been identified to play a key role in this new particle formation enhanced by other compounds such as organic acids (Zhang, 2010) or ammonia (Anttila et al., 2005). To identify the characteristics of cluster formation and nucleation involving sulfuric acid and ammonia in neutral, positive and negative modes, we conducted a computational study. We used a layered approach for configurational sampling of the molecular clusters starting from utilizing a genetic algorithm in order to explore the whole potential energy surface (PES) with all plausible geometrical minima, however, with very unreliable energies. The structures were further optimized with a semi-empirical method and, then, at the ωB97X-D DFT level of theory. After each step, the optimized geometries were filtered to obtain the global minimum configuration. Further, a high level of theory (DLPNO-CCSD(T)) was used for obtaining the electronic energies, in addition to performing DFT frequency analysis, to calculate the Gibbs free energies of formation. These were passed to the Atmospheric Cluster Dynamics Code (ACDC) (McGrath et al., 2012) for studying the evolution of cluster populations. We determined the global minima for the following sulfuric acid - ammonia clusters: (H<sub>2</sub>SO<sub>4</sub>)<sub>m</sub>(NH<sub>3</sub>)<sub>n</sub> with m=n, m=n+1 and n=m+1 for neutral clusters, (H<sub>2</sub>SO<sub>4</sub>)<sub>m</sub>(HSO<sub>4</sub>)<sup>−</sup>(NH<sub>3</sub>)<sub>n</sub> with m=n and n=m+1 for positively charged clusters, and (H<sub>2</sub>SO<sub>4</sub>)<sub>m</sub>(NH<sub>4</sub>)<sup>+</sup>(NH<sub>3</sub>)<sub>n</sub> with m=n and m=n+1 for negatively charged clusters. Further, we present the formation rates, steady state concentrations and fluxes of these clusters calculated using ACDC and discuss how a new configurational sampling procedure, more precise quantum chemistry methods and parameters, such as symmetry and a quasiharmonic approach, impact these ACDC results in comparison to previous studies.</p> </div><div> <p><em>References:<br></em><em>J. Merikanto, D. V. Spracklen, G. W. Mann, S. J. Pickering, and K. S. Carslaw (2009). Atmos. Chem.  Phys., 9, 8601-8616. <br>R. Zhang (2010). Science, 328, 1366-1367. <br>T. Anttila, H. Vehkamäki, I. Napari, M. Kulmala (2005). Boreal Env. Res., 10, 523. <br>M.J. McGrath, T. Olenius, I.K. Ortega, V. Loukonen, P.  Paasonen, T. Kurten, M. Kulmala (2012). Atmos. Chem. Phys., 12, 2355. <br></em></p> </div>

scholarly journals The Role of Organic Acids in New Particle Formation from Methanesulfonic Acid and Methylamine

2021 ◽  
Author(s):  
Rongjie Zhang ◽  
Jiewen Shen ◽  
Hong-Bin Xie ◽  
Jingwen Chen ◽  
Jonas Elm
Keyword(s):  
Organic Acids ◽  
Cluster Formation ◽  
Methanesulfonic Acid ◽  
Particle Formation ◽  
Structural Factors ◽  
Atmospheric Conditions ◽  
New Particle Formation ◽  
Free Energies ◽  
Limited Temperature

Abstract. Atmospheric organic acids (OAs) are expected to enhance methanesulfonic acid (MSA)-driven new particle formation (NPF). However, the exact role of OAs in MSA-driven NPF remains unclear. Here, we employed a two-step strategy to probe the role of OAs in MSA-methylamine (MA) NPF. Initially, we evaluated the enhancing potential of 12 commonly detected OAs in ternary MA-MSA-OA cluster formation by considering the formation free energies of the (MSA)1(MA)1(OA)1 clusters and the atmospheric concentrations of the OAs. It was found that formic acid (ForA) has the highest potential to stabilize the MA-MSA clusters. The high enhancing potential of ForA results from its acidity, structural factors such as no intramolecular H-bonds and high atmospheric abundance. The second step is to extend the MSA-MA-ForA system to larger cluster sizes. The results indicate that ForA can indeed enhance MSA-MA NPF at atmospheric conditions (the upper limited temperature is 258.15 K), indicating that ForA might have an important role in MSA-driven NPF. The enhancing effect of ForA is mainly caused by an increased formation of the (MSA)2(MA)1 cluster, which is involved in the pathway of binary MSA-MA nucleation. Hence, our results indicate that OAs might be required to facilitate MSA-driven NPF in the atmosphere.

scholarly journals Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation

2020 ◽  
Vol 54 (21) ◽  
pp. 13498-13508
Author(s):  
Jiewen Shen ◽  
Jonas Elm ◽  
Hong-Bin Xie ◽  
Jingwen Chen ◽  
Junfeng Niu ◽  
...  
Keyword(s):  
Methanesulfonic Acid ◽  
Particle Formation ◽  
New Particle Formation ◽  
Structural Effects

scholarly journals New particle formation and growth from methanesulfonic acid, trimethylamine and water

2015 ◽  
Vol 17 (20) ◽  
pp. 13699-13709 ◽  
Author(s):  
Haihan Chen ◽  
Michael J. Ezell ◽  
Kristine D. Arquero ◽  
Mychel E. Varner ◽  
Matthew L. Dawson ◽  
...  
Keyword(s):  
Methanesulfonic Acid ◽  
Particle Formation ◽  
New Particle Formation ◽  
Particle Formation And Growth

Water participates in the formation of initial clusters to enhance particle formation from methanesulfonic acid and trimethylamine.

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