Atmospheric Fate of Monoethanolamine: Enhancing New Particle Formation of Sulfuric Acid as an Important Removal Process

Xie, Hong-Bin; Elm, Jonas; Halonen, Roope; Myllys, Nanna; Kurtén, Theo; Kulmala, Markku; Vehkamäki, Hanna

doi:10.1021/acs.est.7b02294

Cited by 110 publications

(181 citation statements)

References 78 publications

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“…In addition, the cluster growth might be hindered due to kinetic barriers. The addition of a monomer or a cluster to a pre-existing cluster might require cluster reorientation which in turn may lead to the breaking of intermolecular bonds, and thus non-negligible kinetic barriers (DePalma et al, 2014;Bzdek et al, 2017;Xu et al, 2017). The subsequent growth as well as the evaporation may be slower than our calculations assume, especially in the case of strongly bound cage-like clusters.…”

Section: Ion-mediated Particle Formationmentioning

confidence: 84%

Role of base strength, cluster structure and charge in sulfuric-acid-driven particle formation

et al. 2019

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Abstract. In atmospheric sulfuric-acid-driven particle formation, bases are able to stabilize the initial molecular clusters and thus enhance particle formation. The enhancing potential of a stabilizing base is affected by different factors, such as the basicity and abundance. Here we use weak (ammonia), medium strong (dimethylamine) and very strong (guanidine) bases as representative atmospheric base compounds, and we systematically investigate their ability to stabilize sulfuric acid clusters. Using quantum chemistry, we study proton transfer as well as intermolecular interactions and symmetry in clusters, of which the former is directly related to the base strength and the latter to the structural effects. Based on the theoretical cluster stabilities and cluster population kinetics modeling, we provide molecular-level mechanisms of cluster growth and show that in electrically neutral particle formation, guanidine can dominate formation events even at relatively low concentrations. However, when ions are involved, charge effects can also stabilize small clusters for weaker bases. In this case the atmospheric abundance of the bases becomes more important, and thus ammonia is likely to play a key role. The theoretical findings are validated by cluster distribution experiments, as well as comparisons to previously reported particle formation rates, showing a good agreement.

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Section: Ion-mediated Particle Formationmentioning

confidence: 84%

Role of base strength, cluster structure and charge in sulfuric-acid-driven particle formation

et al. 2019

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“…In addition of the commonly studied ammonia and amines, several studies have recently investigated possibilities of other bases to participate in new-particle formation. For instance, diamines, amineoxides and guanidine compounds have been suggested to have a role in the stabilization of sulfuric-acid-containing clusters (Xie et al, 2017;Jen et al, 2016;Elm et al, 2016;Myllys, 2017). In fact, these compounds are able to enhance particle formation much more effectively than ammonia or dimethylamine, however, their atmospheric abundances remain unclear.…”

Section: Introductionmentioning

confidence: 99%

Role of Base Strength, Cluster Structure and Charge in Sulfuric Acid-Driven Particle Formation

Myllys¹,

Kubečka²,

Besel³

et al. 2019

Preprint

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<p><strong>Abstract.</strong> In atmospheric sulfuric acid-driven particle formation, bases are able to stabilize the initial molecular clusters, and thus enhance particle formation. The enhancing potential of a stabilizing base is affected by different factors, such as the basicity and abundance. Here we use weak (ammonia), medium strong (dimethylamine) and very strong (guanidine) bases as representative atmospheric base compounds, and systematically investigate their ability to stabilize sulfuric acid clusters. Using quantum chemistry, we study proton transfer as well as intermolecular interactions and symmetry in clusters, of which the former is directly related to the base strength and the latter to the structural effects. Based on the theoretical cluster stabilities and cluster population kinetics modeling, we provide molecular-level mechanisms of cluster growth and show that in electrically neutral particle formation, guanidine can dominate formation events even at relatively low concentrations. However, when ions are involved, charge effects can stabilize small clusters also for weaker bases. In this case the atmospheric abundance of the bases becomes more important, and thus ammonia is likely to play a key role. The theoretical findings are validated by cluster distribution experiments, as well as comparisons to previously reported particle formation rates, showing a good agreement.</p>

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“…3,4 There is compelling evidence that sulfuric acid (SA), water (W), ammonia (A) or amines can play key roles in atmospheric new particle formation (NPF), but these compounds are still not e cient enough to explain NPF in all the environments where it has been observed. Recently, numerous atmospheric observations and theoretical studies have shown that organic acids can also enhance NPF, [5][6][7][8][9][10][11][12][13][14][15] However, there are potentially tens of thousands of di↵erent atmospheric organic species with varying properties, which makes the exact chemical composition of clusters containing organic molecules highly speculative. Furthermore, di↵erent organics have di↵erent chemical reactivities.…”

Section: Introductionmentioning

confidence: 99%

Clustering mechanism of oxocarboxylic acids involving hydration reaction: Implications for the atmospheric models

Liu

Kupiainen-Määttä

Zhang

et al. 2018

The Journal of Chemical Physics

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The formation of atmospheric aerosol particles from condensable gases is a dominant source of particulate matter in the boundary layer, but the mechanism is still ambiguous. During the clustering process, precursors with different reactivities can induce various chemical reactions in addition to the formation of hydrogen bonds. However, the clustering mechanism involving chemical reactions is rarely considered in most of the nucleation process models. Oxocarboxylic acids are common compositions of secondary organic aerosol, but the role of oxocarboxylic acids in secondary organic aerosol formation is still not fully understood. In this paper, glyoxylic acid, the simplest and the most abundant atmospheric oxocarboxylic acid, has been selected as a representative example of oxocarboxylic acids in order to study the clustering mechanism involving hydration reactions using density functional theory combined with the Atmospheric Clusters Dynamic Code. The hydration reaction of glyoxylic acid can occur either in the gas phase or during the clustering process. Under atmospheric conditions, the total conversion ratio of glyoxylic acid to its hydration reaction product (2,2-dihydroxyacetic acid) in both gas phase and clusters can be up to 85%, and the product can further participate in the clustering process. The differences in cluster structures and properties induced by the hydration reaction lead to significant differences in cluster formation rates and pathways at relatively low temperatures.

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Atmospheric Fate of Monoethanolamine: Enhancing New Particle Formation of Sulfuric Acid as an Important Removal Process

Cited by 110 publications

References 78 publications

Role of base strength, cluster structure and charge in sulfuric-acid-driven particle formation

Role of base strength, cluster structure and charge in sulfuric-acid-driven particle formation

Role of Base Strength, Cluster Structure and Charge in Sulfuric Acid-Driven Particle Formation

Clustering mechanism of oxocarboxylic acids involving hydration reaction: Implications for the atmospheric models

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