Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates
NaCl in fresh sea-salt aerosol (SSA) particles can partially or fully react with atmospheric NO<sub>x</sub>/HNO<sub>3</sub>, so internally mixed NaCl and NaNO<sub>3</sub> aerosol particles can co-exist over a wide range of mixing ratios. Laboratory-generated, micr...
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doaj-c1339033a8e6490e863ccc75cefb18182020-11-24T23:45:12ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242015-03-011563379339310.5194/acp-15-3379-2015Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogatesD. Gupta0H. Kim1G. Park2X. Li3H.-J. Eom4C.-U. Ro5Department of Chemistry, Inha University, Incheon, 402-751, South KoreaDepartment of Chemistry, Inha University, Incheon, 402-751, South KoreaDepartment of Chemistry, Inha University, Incheon, 402-751, South KoreaDepartment of Chemistry, Inha University, Incheon, 402-751, South KoreaDepartment of Chemistry, Inha University, Incheon, 402-751, South KoreaDepartment of Chemistry, Inha University, Incheon, 402-751, South KoreaNaCl in fresh sea-salt aerosol (SSA) particles can partially or fully react with atmospheric NO<sub>x</sub>/HNO<sub>3</sub>, so internally mixed NaCl and NaNO<sub>3</sub> aerosol particles can co-exist over a wide range of mixing ratios. Laboratory-generated, micrometer-sized NaCl and NaNO<sub>3</sub> mixture particles at 10 mixing ratios (mole fractions of NaCl (<i>X</I><sub>NaCl</sub>) = 0.1 to 0.9) were examined systematically to observe their hygroscopic behavior, derive experimental phase diagrams for deliquescence and efflorescence, and understand the efflorescence mechanism. During the humidifying process, aerosol particles with the eutonic composition (<i>X</I><sub>NaCl</sub> = 0.38) showed only one phase transition at their mutual deliquescence relative humidity (MDRH) of 67.9 (±0.5)% On the other hand, particles with other mixing ratios showed two distinct deliquescence transitions; i.e., the eutonic component dissolved at MDRH, and the remainder in the solid phase dissolved completely at their DRHs depending on the mixing ratios, resulting in a phase diagram composed of four different phases, as predicted thermodynamically. During the dehydration process, NaCl-rich particles (<i>X</I><sub>NaCl</sub> > 0.38) showed a two stage efflorescence transition: the first stage was purely driven by the homogeneous nucleation of NaCl and the second stage at the mutual efflorescence RH (MERH) of the eutonic components, with values in the range of 30.0–35.5%. Interestingly, aerosol particles with the eutonic composition (<i>X</I><sub>NaCl</sub> = 0.38) also showed two-stage efflorescence, with NaCl crystallizing first followed by heterogeneous nucleation of the remaining NaNO<sub>3</sub> on the NaCl seeds. NaNO<sub>3</sub>-rich particles (<i>X</I><sub>NaCl</sub> ≤ 0.3) underwent single-stage efflorescence transitions at ERHs progressively lower than the MERH because of the homogeneous nucleation of NaCl and the almost simultaneous heterogeneous nucleation of NaNO<sub>3</sub> on the NaCl seeds. SEM/EDX elemental mapping indicated that the effloresced NaCl–NaNO<sub>3</sub> particles at all mixing ratios were composed of a homogeneously crystallized NaCl moiety in the center, surrounded either by the eutonic component (for <i>X</I><sub>NaCl</sub> > 0.38) or NaNO<sub>3</sub> (for <i>X</I><sub>NaCl</sub> ≤ 0.38). During the humidifying or dehydration process, the amount of eutonic composed part drives particle/droplet growth or shrinkage at the MDRH or MERH (second ERH), respectively, and the amount of pure salts (NaCl or NaNO<sub>3</sub> in NaCl- or NaNO<sub>3</sub>-rich particles, respectively) drives the second DRHs or first ERHs, respectively. Therefore, their behavior can be a precursor to the optical properties and direct radiative forcing for these atmospherically relevant mixture particles representing the coarse, reacted inorganic SSAs. In addition, the NaCl–NaNO<sub>3</sub> mixture aerosol particles can maintain an aqueous phase over a wider RH range than pure NaCl particles as SSA surrogate, making their heterogeneous chemistry more probable.http://www.atmos-chem-phys.net/15/3379/2015/acp-15-3379-2015.pdf |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
D. Gupta H. Kim G. Park X. Li H.-J. Eom C.-U. Ro |
spellingShingle |
D. Gupta H. Kim G. Park X. Li H.-J. Eom C.-U. Ro Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates Atmospheric Chemistry and Physics |
author_facet |
D. Gupta H. Kim G. Park X. Li H.-J. Eom C.-U. Ro |
author_sort |
D. Gupta |
title |
Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates |
title_short |
Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates |
title_full |
Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates |
title_fullStr |
Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates |
title_full_unstemmed |
Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates |
title_sort |
hygroscopic properties of nacl and nano<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates |
publisher |
Copernicus Publications |
series |
Atmospheric Chemistry and Physics |
issn |
1680-7316 1680-7324 |
publishDate |
2015-03-01 |
description |
NaCl in fresh sea-salt aerosol (SSA) particles can partially or fully react
with atmospheric NO<sub>x</sub>/HNO<sub>3</sub>, so internally mixed NaCl and NaNO<sub>3</sub>
aerosol particles can co-exist over a wide range of mixing ratios.
Laboratory-generated, micrometer-sized NaCl and NaNO<sub>3</sub> mixture particles
at 10 mixing ratios (mole fractions of NaCl (<i>X</I><sub>NaCl</sub>) = 0.1 to 0.9)
were examined systematically to observe their hygroscopic behavior, derive
experimental phase diagrams for deliquescence and efflorescence, and
understand the efflorescence mechanism. During the humidifying process,
aerosol particles with the eutonic composition (<i>X</I><sub>NaCl</sub> = 0.38) showed
only one phase transition at their mutual deliquescence relative humidity
(MDRH) of 67.9 (±0.5)% On the other hand, particles with other
mixing ratios showed two distinct deliquescence transitions; i.e., the
eutonic component dissolved at MDRH, and the remainder in the solid phase
dissolved completely at their DRHs depending on the mixing ratios, resulting
in a phase diagram composed of four different phases, as predicted
thermodynamically. During the dehydration process, NaCl-rich particles
(<i>X</I><sub>NaCl</sub> > 0.38) showed a two stage efflorescence transition:
the first stage was purely driven by the homogeneous nucleation of NaCl and
the second stage at the mutual efflorescence RH (MERH) of the eutonic
components, with values in the range of 30.0–35.5%. Interestingly,
aerosol particles with the eutonic composition (<i>X</I><sub>NaCl</sub> = 0.38) also
showed two-stage efflorescence, with NaCl crystallizing first followed by
heterogeneous nucleation of the remaining NaNO<sub>3</sub> on the NaCl seeds.
NaNO<sub>3</sub>-rich particles (<i>X</I><sub>NaCl</sub> ≤ 0.3) underwent single-stage
efflorescence transitions at ERHs progressively lower than the MERH because
of the homogeneous nucleation of NaCl and the almost simultaneous
heterogeneous nucleation of NaNO<sub>3</sub> on the NaCl seeds. SEM/EDX elemental
mapping indicated that the effloresced NaCl–NaNO<sub>3</sub> particles at all
mixing ratios were composed of a homogeneously crystallized NaCl moiety in
the center, surrounded either by the eutonic component (for <i>X</I><sub>NaCl</sub>
> 0.38) or NaNO<sub>3</sub> (for <i>X</I><sub>NaCl</sub> ≤ 0.38). During the
humidifying or dehydration process, the amount of eutonic composed part
drives particle/droplet growth or shrinkage at the MDRH or MERH (second
ERH), respectively, and the amount of pure salts (NaCl or NaNO<sub>3</sub> in
NaCl- or NaNO<sub>3</sub>-rich particles, respectively) drives the second DRHs or
first ERHs, respectively. Therefore, their behavior can be a precursor to
the optical properties and direct radiative forcing for these
atmospherically relevant mixture particles representing the coarse, reacted
inorganic SSAs. In addition, the NaCl–NaNO<sub>3</sub> mixture aerosol particles
can maintain an aqueous phase over a wider RH range than pure NaCl particles
as SSA surrogate, making their heterogeneous chemistry more probable. |
url |
http://www.atmos-chem-phys.net/15/3379/2015/acp-15-3379-2015.pdf |
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