Olenius, T., Halonen, R., Kurtén, T., Henschel, H., Kupiainen‐Määttä, O., Ortega, I. K., Jen, C. N., Vehkamäki, H., and Riipinen, I. ( 2017), New particle formation from sulfuric acid and amines: Comparison of monomethylamine, dimethylamine, and trimethylamine, J. Geophys. Res. Atmos., 122, 7103– 7118, doi:10.1002/2017JD026501
New particle formation from sulfuric acid and amines : comparison of monomethylamine, dimethylamine, and trimethylamine
|Author:||Olenius, Tinja1; Halonen, Roope2; Kurtén, Theo3;|
1Department of Environmental Science and Analytical Chemistry (ACES) and Bolin Centre for Climate Research, Stockholm University, Stockholm, Sweden
2Department of Physics, University of Helsinki, Helsinki, Finland
3Department of Chemistry, University of Helsinki, Helsinki, Finland
4Now at Research Unit of Medical Imaging, Physics and Technology, University of Oulu, Oulu, Finland
5Now at ONERA-The French Aerospace Lab, Palaiseau, France
6Environmental Science, Policy, and Management, University of California, Berkeley, California, USA
|Online Access:||PDF Full Text (PDF, 1.4 MB)|
|Persistent link:|| http://urn.fi/urn:nbn:fi-fe2019062722210
American Geophysical Union,
|Publish Date:|| 2019-06-27
Amines are bases that originate from both anthropogenic and natural sources, and they are recognized as candidates to participate in atmospheric aerosol particle formation together with sulfuric acid. Monomethylamine, dimethylamine, and trimethylamine (MMA, DMA, and TMA, respectively) have been shown to enhance sulfuric acid‐driven particle formation more efficiently than ammonia, but both theory and laboratory experiments suggest that there are differences in their enhancing potentials. However, as quantitative concentrations and thermochemical properties of different amines remain relatively uncertain, and also for computational reasons, the compounds have been treated as a single surrogate amine species in large‐scale modeling studies. In this work, the differences and similarities of MMA, DMA, and TMA are studied by simulations of molecular cluster formation from sulfuric acid, water, and each of the three amines. Quantum chemistry‐based cluster evaporation rate constants are applied in a cluster population dynamics model to yield cluster concentrations and formation rates at boundary layer conditions. While there are differences, for instance, in the clustering mechanisms and cluster hygroscopicity for the three amines, DMA and TMA can be approximated as a lumped species. Formation of nanometer‐sized particles and its dependence on ambient conditions is roughly similar for these two: both efficiently form clusters with sulfuric acid, and cluster formation is rather insensitive to changes in temperature and relative humidity. Particle formation from sulfuric acid and MMA is weaker and significantly more sensitive to ambient conditions. Therefore, merging MMA together with DMA and TMA introduces inaccuracies in sulfuric acid‐amine particle formation schemes.
Journal of geophysical research. Atmospheres
|Pages:||7103 - 7118|
|Type of Publication:||
A1 Journal article – refereed
|Field of Science:||
ERC projects 278277‐ATMOGAIN, 257360‐MOCAPAF, and 692891‐DAMOCLES; Formas project 2015‐749; the Academy of Finland Center of Excellence program project 272041; and National Science Foundation AGS project 1524211 are acknowledged for funding. The authors thank CSC‐IT Center for Science in Espoo, Finland, for computing time.
©2017. American Geophysical Union.