Formation of atmospheric molecular clusters consisting of methanesulfonic acid and sulfuric acid: Insights from flow tube experiments and cluster dynamics simulations

Wen, Hui; Wang, Chunyu; Wang, Zhongquan; Hou, Xiaofei; Han, Yajuan; Liu, Yi-Rong; Jiang, Shuai; Huang, Teng; Huang, Wei

doi:10.1016/j.atmosenv.2018.11.043

Cited by 12 publications

(2 citation statements)

References 103 publications

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“…Bork et al 40 studied SA–MSA–DMA clusters using quantum chemical methods. It was found that in marine environments MSA could enhance cluster formation between SA and dimethylamine up to a factor of 3 at 258.15 K. Applying a combination of flowtube experiments and quantum chemical calculations, Wen et al 41 demonstrated that adding MSA to newly formed SA - water particles led to a dual particle distribution, while adding SA to newly formed MSA–water particles did not show this behavior. In both cases, mixed SA–MSA–water particles emerged, but with highly different number concentrations and size distributions.…”

Section: Introductionmentioning

confidence: 99%

Clusteromics III: Acid Synergy in Sulfuric Acid–Methanesulfonic Acid–Base Cluster Formation

Elm

2022

ACS Omega

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Acid–base molecular clusters are an important stage in atmospheric new particle formation. While such clusters are most likely multicomponent in nature, there are very few reports on clusters consisting of multiple acid molecules and multiple base molecules. By applying state-of-the-art quantum chemical methods, we herein study electrically neutral (SA) 1 (MSA) 1 (base) 0–2 clusters with base = ammonia (A), methylamine (MA), dimethylamine (DMA), trimethylamine (TMA) and ethylenediamine (EDA). The cluster structures are obtained using a funneling approach employing the ABCluster program, semiempirical PM7 calculations and ωB97X-D/6-31++G(d,p) calculations. The final binding free energies are calculated at the DLPNO-CCSD(T 0 )/aug-cc-pVTZ//ωB97X-D/6-31++G(d,p) level of theory using the quasi-harmonic approximation. Based on the calculated cluster geometries and thermochemistry (at 298.15 K and 1 atm), we find that the mixed (SA) 1 (MSA) 1 (base) 1–2 clusters more resemble the (SA) 2 (base) 1–2 clusters compared to the (MSA) 2 (base) 1–2 clusters. Hence, some of the steric hindrance and lack of hydrogen bond capacity previously observed in the (MSA) 2 (base) 1–2 clusters is diminished in the corresponding (SA) 1 (MSA) 1 (base) 1–2 clusters. Cluster kinetics simulations reveal that the presence of an MSA molecule in the clusters enhances the cluster formation potential by up to a factor of 20. We find that the SA–MSA–DMA clusters have the highest cluster formation potential, and thus, this system should be further extended to larger sizes in future studies.

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Section: Introductionmentioning

confidence: 99%

Clusteromics III: Acid Synergy in Sulfuric Acid–Methanesulfonic Acid–Base Cluster Formation

Elm

2022

ACS Omega

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“…Bork et al 46 showed that at MSA concentrations relevant to the marine environment, cluster formation between SA and dimethylamine could be enhanced from 15 to 300% at 298 and 258 K, respectively, by the presence of MSA. Using a combination of flow tube experiments and quantum chemical calculations, Wen et al 47 recently showed that adding MSA to formed SA–water particles led to a bimodal particle distribution with an initial narrow peak that was attributed to MSA–water particles and a broad larger peak that was attributed to SA–water particles. Adding SA to formed MSA–water particles did not show this bimodal behavior.…”

Section: Introductionmentioning

confidence: 99%

New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals

Rosati

Christiansen

Jonge

et al. 2021

ACS Earth Space Chem.

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Dimethyl sulfide (DMS) is produced by plankton in oceans and constitutes the largest natural emission of sulfur to the atmosphere. In this work, we examine new particle formation from the primary pathway of oxidation of gas-phase DMS by OH radicals. We particularly focus on particle growth and mass yield as studied experimentally under dry conditions using the atmospheric simulation chamber AURA. Experimentally, we show that aerosol mass yields from oxidation of 50–200 ppb of DMS are low (2–7%) and that particle growth rates (8.2–24.4 nm/h) are comparable with ambient observations. An HR-ToF-AMS was calibrated using methanesulfonic acid (MSA) to account for fragments distributed across both the organic and sulfate fragmentation table. AMS-derived chemical compositions revealed that MSA was always more dominant than sulfate in the secondary aerosols formed. Modeling using the Aerosol Dynamics, gas- and particle-phase chemistry kinetic multilayer model for laboratory CHAMber studies (ADCHAM) indicates that the Master Chemical Mechanism gas-phase chemistry alone underestimates experimentally observed particle formation and that DMS multiphase and autoxidation chemistry is needed to explain observations. Based on quantum chemical calculations, we conclude that particle formation from DMS oxidation in the ambient atmosphere will most likely be driven by mixed sulfuric acid/MSA clusters clustering with both amines and ammonia.

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Nucleation in the Mediterranean Atmosphere

Sellegri

2022

Atmospheric Chemistry in the Mediterranean Region

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Formation of atmospheric molecular clusters consisting of methanesulfonic acid and sulfuric acid: Insights from flow tube experiments and cluster dynamics simulations

Cited by 12 publications

References 103 publications

Clusteromics III: Acid Synergy in Sulfuric Acid–Methanesulfonic Acid–Base Cluster Formation

Clusteromics III: Acid Synergy in Sulfuric Acid–Methanesulfonic Acid–Base Cluster Formation

New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals

Nucleation in the Mediterranean Atmosphere

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