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. 2018 Jan 16;8(6):3250-3263.
doi: 10.1039/c7ra12064h. eCollection 2018 Jan 12.

Hydration of the methanesulfonate-ammonia/amine complex and its atmospheric implications

Shou-Kui Miao  1   2 , Shuai Jiang  2 , Xiu-Qiu Peng  1   2 , Yi-Rong Liu  2 , Ya-Juan Feng  2 , Yan-Bing Wang  1   2 , Feng Zhao  1   2 , Teng Huang  1 , Wei Huang  1   2   3
Affiliations

Hydration of the methanesulfonate-ammonia/amine complex and its atmospheric implications

Shou-Kui Miao et al. RSC Adv. .

Abstract

Methanesulfonate (MSA-), found in substantial concentrations in the atmosphere, is expected to enhance aerosol nucleation and the growth of nanoparticles, but the details of methanesulfonate clusters are poorly understood. In this study, MSA- was chosen along with ammonia (NH3) or three common amines and water (H2O) to discuss the roles of ternary homogeneous nucleation and ion-induced nucleation in aerosol formation. We studied the structural characteristics and thermodynamics of the clusters using density functional theory at the PW91PW91/6-311++G(3df,3pd) level. The analysis of noncovalent interactions predicts that the amines can form more stable clusters with MSA- than NH3, in agreement with the results from structures and thermodynamics; however, the enhancement in stability for amines is not large enough to overcome the difference in the concentrations of NH3 and amines under typical atmospheric conditions. In addition, the favorable free energies of formation for the (MSA-)(NH3/amines)(H2O) n (n = 0-3) clusters at 298.15 K show that MSA- could contribute to the aerosol nucleation process with binding NH3/amines and H2O up to n = 3. There are strong temperature and humidity dependences for the formation of complexes; higher humidity and temperature promote the formation of larger hydrates. Finally, for the (MSA-)(NH3/amines)(H2O) n clusters, the evaporation rates were determined to further investigate the atmospheric implications.

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Conflict of interest statement

There are no conflicts to declare.

Figures

Fig. 1
Fig. 1. The global minima for (MSA−)(NH3/amines)(H2O)n (n = 0–3) optimized at the PW91PW91/6-311++G(3df,3pd) level.
Fig. 2
Fig. 2. Noncovalent interactions (NCI) analysis among the global minima for (MSA−)(NH3) (a), (MSA−)(MA) (b), (MSA−)(DMA) (c), (MSA−)(TMA) (d).
Fig. 3
Fig. 3. Hydrate distributions of (MSA−)(NH3/amines)(H2O)n (n = 0–3) clusters at three different relative humidities (RHs) with the temperature of 298.15 K (a), and three different temperatures with the RH of 50% (b).
Fig. 4
Fig. 4. Evaporation rates of MSA−, NH3/amines, H2O and (MSA−)(NH3/amines) from (MSA−)(NH3)(H2O)n (n = 0–3) clusters (a), (MSA−)(MA)(H2O)n (n = 0–3) clusters (b), (MSA−)(DMA)(H2O)n (n = 0–3) clusters (c) and (MSA−)(TMA)(H2O)n (n = 0–3) clusters (d), respectively.
Fig. 5
Fig. 5. Evaporation rates from the (MSA−)(NH3/amines)(H2O)n (n = 0–3) clusters. The top left (a), top right (b), bottom left (c) and bottom right (d) panels give the results for evaporation of MSA−, NH3/MA/DMA/TMA, H2O and (MSA−)(NH3)/(MSA−)(MA)/(MSA−)(DMA)/(MSA−)(TMA), respectively.
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