Charged and neutral binary nucleation of sulfuric acid in free troposphere conditions

Recent research [Wang et al., Nature 581, 184–189 (2020)] indicates nitric acid (NA) can participate in sulfuric acid (SA)–ammonia (NH3) nucleation in the clean and cold upper free troposphere, whereas NA exhibits no obvious effects at the boundary layer with relatively high temperatures. Herein, considering that an SA–dimethylamine (DMA) nucleation mechanism was detected in megacities [Yao et al., Science 361, 278–281 (2018)], the roles of NA in SA-DMA nucleation are investigated. Different from SA-NH3 nucleation, we found that NA can enhance SA-DMA–based particle formation rates in the polluted atmospheric boundary layer, such as Beijing in winter, with the enhancement up to 80-fold. Moreover, we found that NA can promote the number concentrations of nucleation clusters (up to 27-fold) and contribute 76% of cluster formation pathways at 280 K. The enhancements on particle formation by NA are critical for particulate pollution in the polluted boundary layer with relatively high NA and DMA concentrations.

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Binary nucleation in acid–water systems. II. Sulfuric acid–water and a comparison with methanesulfonic acid–water

The Journal of Chemical Physics ◽

10.1063/1.460262 ◽

1991 ◽

Vol 94 (10) ◽

pp. 6842-6850 ◽

Cited By ~ 125

Author(s):

B. E. Wyslouzil ◽

J. H. Seinfeld ◽

R. C. Flagan ◽

K. Okuyama

Keyword(s):

Sulfuric Acid ◽

Methanesulfonic Acid ◽

Water Systems ◽

Acid Water ◽

Binary Nucleation

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Measurement of aerosol sulfuric acid: 2. Pronounced layering in the free troposphere during the second Aerosol Characterization Experiment (ACE 2)

Journal of Geophysical Research Atmospheres ◽

10.1029/2001jd000605 ◽

2001 ◽

Vol 106 (D23) ◽

pp. 31975-31990 ◽

Cited By ~ 23

Author(s):

J. Curtius ◽

B. Sierau ◽

F. Arnold ◽

M. de Reus ◽

J. Ström ◽

...

Keyword(s):

Sulfuric Acid ◽

Free Troposphere ◽

Aerosol Characterization

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Binary nucleation of water-sulfuric acid system: the effect of the shape of the free energy surface and compressibility of solution on the nucleation rate

Journal of Aerosol Science ◽

10.1016/s0021-8502(98)00552-7 ◽

1998 ◽

Vol 29 ◽

pp. S377-S378 ◽

Cited By ~ 2

Author(s):

M. Noppel

Keyword(s):

Free Energy ◽

Sulfuric Acid ◽

Nucleation Rate ◽

Energy Surface ◽

Acid System ◽

Free Energy Surface ◽

Binary Nucleation

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Roles of Organic Emissions in the Formation of Near Field Aircraft-Emitted Volatile Particulate Matter: A Kinetic Microphysical Modeling Study

Journal of Engineering for Gas Turbines and Power ◽

10.1115/1.4029366 ◽

2015 ◽

Vol 137 (7) ◽

Cited By ~ 3

Author(s):

Hsi-Wu Wong ◽

Mina Jun ◽

Jay Peck ◽

Ian A. Waitz ◽

Richard C. Miake-Lye

Keyword(s):

Sulfuric Acid ◽

Relative Humidity ◽

Ambient Temperature ◽

Near Field ◽

Water Soluble ◽

Acid Water ◽

Organic Vapors ◽

Nucleation Mode ◽

Ambient Relative Humidity ◽

Binary Nucleation

A kinetic microphysical modeling approach that describes the formation of volatile aerosols in the presence of organic emissions in near field aircraft emitted plumes at ground level is presented. Our model suggests that self nucleation of organic species, binary nucleation of water-soluble organic vapors with water, and multicomponent nucleation of water-soluble organic vapors with sulfuric acid and water all have very slow nucleation rates. The formation of new homogeneous particles in near field aircraft plumes is thus considered to be driven by binary nucleation of sulfuric acid and water. Volatile organic vapors emitted from aircraft engines primarily contribute to the nucleation process by condensing on existing homogeneous aerosols and only affect the size and the composition (not the number) of the homogeneous aerosols. Our model also shows that under low ambient relative humidity levels or high ambient temperatures, nucleation mode particles are more organic-rich than soot coatings. Organic mass fraction of nucleation mode particles is more sensitive to organic emissions levels compared to that of soot coatings. Ambient temperature and relative humidity were also predicted to affect the nucleation of sulfuric acid–water cores, where higher ambient relative humidity level and lower ambient temperature strongly favor binary sulfuric acid–water nucleation. The effect of ambient conditions on organic fractions was predicted to be relatively insignificant.

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