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Formation mechanism of methanesulfonic acid and ammonia clusters: A kinetics simulation study
https://orcid.org/0000-0002-9462-701X
https://orcid.org/0000-0002-5466-596X
Abstract The formation mechanism of methanesulfonic acid (MSA) and ammonia (NH3) clusters is investigated using density functional theory (DFT) and Atmospheric Cluster Dynamic Code (ACDC) in different conditions. The results suggest that hydrogen bonding and electrostatic interactions induced by proton transfer could provide the primary driving force that forms these clusters. NH3 can effectively promote the formation of MSA-based clusters at pptv levels, but high concentrations of precursors ([MSA] ≥ 2 × 107 molecules cm−3 and [NH3] ≥ 1 ppbv) is necessary for effective formation. The formation of the initial (MSA)2 dimer is a rate-determining step of cluster growth. The formation rate is proportional to the monomer concentration and inversely proportional to the temperature in the troposphere. Hydration has a great influence on the evaporation rate, formation rate, and nucleation mechanism of the MSA-NH3 system. The relative evaporation rate of all clusters is significantly affected by humidity, especially for the (MSA)(NH3) dimer. The evaporation rate of the (MSA)(NH3) dimer can be reduced by approximately a factor of 10−5 at a relative humidity (RH) ≥ 40%. The formation rate increases significantly with RH and reached up to a factor of 105 at RH = 100%. The formation of the initial (MSA)(NH3) dimer is the rate-determining step, which indicates that the nucleation mechanism is fundamentally different from anhydrous cases. In addition, the results showed that the formation of MSA-NH3 molecular clusters is relatively weak under typical atmospheric conditions. In addition to the high concentration of precursors and atmospheric humidity, the formation of MSA-based ternary clusters through the participation of other species such as SA that may be more important in promoting effective nucleation of MSA-NH3 system in the coastal atmosphere.
Graphical abstract Display Omitted
Highlights Hydrogen bonding is the primary driving force that forms the MSA-NH3 clusters. NH3 effectively promotes the formation of MSA-based clusters at ppt levels. Formation of (MSA)2 is a rate-determining step under anhydrous condition. Formation of (MSA)(NH3) is a rate-determining step under hydrous condition. The formation rate increases with RH, reaching up to a factor of 105 at RH = 100%.
Formation mechanism of methanesulfonic acid and ammonia clusters: A kinetics simulation study
https://orcid.org/0000-0002-9462-701X
https://orcid.org/0000-0002-5466-596X
Abstract The formation mechanism of methanesulfonic acid (MSA) and ammonia (NH3) clusters is investigated using density functional theory (DFT) and Atmospheric Cluster Dynamic Code (ACDC) in different conditions. The results suggest that hydrogen bonding and electrostatic interactions induced by proton transfer could provide the primary driving force that forms these clusters. NH3 can effectively promote the formation of MSA-based clusters at pptv levels, but high concentrations of precursors ([MSA] ≥ 2 × 107 molecules cm−3 and [NH3] ≥ 1 ppbv) is necessary for effective formation. The formation of the initial (MSA)2 dimer is a rate-determining step of cluster growth. The formation rate is proportional to the monomer concentration and inversely proportional to the temperature in the troposphere. Hydration has a great influence on the evaporation rate, formation rate, and nucleation mechanism of the MSA-NH3 system. The relative evaporation rate of all clusters is significantly affected by humidity, especially for the (MSA)(NH3) dimer. The evaporation rate of the (MSA)(NH3) dimer can be reduced by approximately a factor of 10−5 at a relative humidity (RH) ≥ 40%. The formation rate increases significantly with RH and reached up to a factor of 105 at RH = 100%. The formation of the initial (MSA)(NH3) dimer is the rate-determining step, which indicates that the nucleation mechanism is fundamentally different from anhydrous cases. In addition, the results showed that the formation of MSA-NH3 molecular clusters is relatively weak under typical atmospheric conditions. In addition to the high concentration of precursors and atmospheric humidity, the formation of MSA-based ternary clusters through the participation of other species such as SA that may be more important in promoting effective nucleation of MSA-NH3 system in the coastal atmosphere.
Graphical abstract Display Omitted
Highlights Hydrogen bonding is the primary driving force that forms the MSA-NH3 clusters. NH3 effectively promotes the formation of MSA-based clusters at ppt levels. Formation of (MSA)2 is a rate-determining step under anhydrous condition. Formation of (MSA)(NH3) is a rate-determining step under hydrous condition. The formation rate increases with RH, reaching up to a factor of 105 at RH = 100%.
Formation mechanism of methanesulfonic acid and ammonia clusters: A kinetics simulation study
https://orcid.org/0000-0002-9462-701X
https://orcid.org/0000-0002-5466-596X
Abstract The formation mechanism of methanesulfonic acid (MSA) and ammonia (NH3) clusters is investigated using density functional theory (DFT) and Atmospheric Cluster Dynamic Code (ACDC) in different conditions. The results suggest that hydrogen bonding and electrostatic interactions induced by proton transfer could provide the primary driving force that forms these clusters. NH3 can effectively promote the formation of MSA-based clusters at pptv levels, but high concentrations of precursors ([MSA] ≥ 2 × 107 molecules cm−3 and [NH3] ≥ 1 ppbv) is necessary for effective formation. The formation of the initial (MSA)2 dimer is a rate-determining step of cluster growth. The formation rate is proportional to the monomer concentration and inversely proportional to the temperature in the troposphere. Hydration has a great influence on the evaporation rate, formation rate, and nucleation mechanism of the MSA-NH3 system. The relative evaporation rate of all clusters is significantly affected by humidity, especially for the (MSA)(NH3) dimer. The evaporation rate of the (MSA)(NH3) dimer can be reduced by approximately a factor of 10−5 at a relative humidity (RH) ≥ 40%. The formation rate increases significantly with RH and reached up to a factor of 105 at RH = 100%. The formation of the initial (MSA)(NH3) dimer is the rate-determining step, which indicates that the nucleation mechanism is fundamentally different from anhydrous cases. In addition, the results showed that the formation of MSA-NH3 molecular clusters is relatively weak under typical atmospheric conditions. In addition to the high concentration of precursors and atmospheric humidity, the formation of MSA-based ternary clusters through the participation of other species such as SA that may be more important in promoting effective nucleation of MSA-NH3 system in the coastal atmosphere.
Graphical abstract Display Omitted
Highlights Hydrogen bonding is the primary driving force that forms the MSA-NH3 clusters. NH3 effectively promotes the formation of MSA-based clusters at ppt levels. Formation of (MSA)2 is a rate-determining step under anhydrous condition. Formation of (MSA)(NH3) is a rate-determining step under hydrous condition. The formation rate increases with RH, reaching up to a factor of 105 at RH = 100%.
Formation mechanism of methanesulfonic acid and ammonia clusters: A kinetics simulation study
Chen, Dongping (author) / Li, Danfeng (author) / Wang, Changwei (author) / Liu, Fengyi (author) / Wang, Wenliang (author)
Atmospheric Environment ; 222
2019-11-16
Article (Journal)
Electronic Resource
English
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