Kinetics of Nitric Acid Uptake by Salt

Fenter, Frederick F.; Caloz, François; Rossi, Michel J.

doi:10.1021/j100090a014

Cited by 100 publications

(210 citation statements)

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“…The mass spectra of the species of interest in this study share common fragment peaks when using electron impact ionization ( Based on previous studies of the gaseous products of the HNO 3 -NaCl reaction, 12,13,17,18,29,32 HNO 3 generated in the N 2 O 5 hydrolysis reacts on the salt surface to form gaseous HCl. We denote the HCl produced in reaction (4) …”

Section: Experimental Methodsmentioning

confidence: 99%

“…This introduces substantial uncertainty regarding the available surface area of the salt to which the gas is exposed. 12,13,17,32,[46][47][48][49][50][51][52] In the limit of very fast gas uptake, the gas is removed before it can diffuse significantly into the underlying salt layers. In this case, the geometric surface area is a reasonable approximation for the available reactive surface area.…”

Section: à2mentioning

confidence: 99%

“…In the former case, the HNO 3 product can react further with NaCl [11][12][13][14][15][16][17][18]20,[22][23][24][25][26][27][28][29][30][31][32][33][34] to generate HCl.…”

Section: Introductionmentioning

confidence: 99%

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Knudsen cell studies of the reactions of N2O5 and ClONO2 with NaCl: development and application of a model for estimating available surface areas and corrected uptake coefficients

Hoffman

Gebel

Fox

et al. 2003

Phys. Chem. Chem. Phys.

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The reaction of gaseous N 2 O 5 with sea salt and its components is a potential source of halogen atoms in the marine boundary layer. There are two possible reaction paths when water is present on the salt surface. Reaction with the chloride ion forms nitryl chloride (ClNO 2 ), a photolyzable compound: N 2 O 5 + NaCl ! ClNO 2 + NaNO 3 , while hydrolysis of N 2 O 5 generates HNO 3 that can react further with NaCl to form gaseous HCl: N 2 O 5 + H 2 O (on NaCl) ! 2 HNO 3 , HNO 3 + NaCl ! HCl + NaNO 3 . We report here Knudsen cell studies at 23 C of the reaction of N 2 O 5 with NaCl, using less than one layer of salt particles. A model, which takes into account the effective salt surface area exposed to the gas, was applied, allowing for the determination of uptake coefficients without introducing uncertainties associated with diffusion into multiple layers of salt particles. The net uptake coefficient for the sum of both channels for the N 2 O 5 reaction was measured to be g N 2 O 5 ¼ (2.9 AE 1.7) Â 10 À3, where the error cited is the 2s statistical error. The cumulative error is estimated to be better than a factor of three. Both ClNO 2 and HCl were observed as gaseous products from the N 2 O 5 -salt reaction and the branching ratio for ClNO 2 was 0.73 AE 0.28 (2s). A limited number of experiments were carried out for the reaction with synthetic sea salt, resulting in an uptake coefficient of about an order of magnitude larger than for NaCl, and a ClNO 2 yield of 100%. We propose a mechanism for this reaction in which surfaceadsorbed water plays a key role in the competition between hydrolysis of N 2 O 5 to generate HNO 3 and the reaction with NaCl to generate ClNO 2 . Reaction with NaCl is shown to be a potentially important source of ClNO 2 , and thus, of highly reactive chlorine atoms in urban marine regions at dawn. Application of our model to previous data from this laboratory for the reaction of chlorine nitrate (ClONO 2 ) with fractional layers of NaCl gives a corrected uptake coefficient of g ClONO 2 ¼ (2.4 AE 1.2) Â 10 À2 (2s), which suggests that the ClONO 2 -NaCl reaction may contribute significantly to the observed concentrations of Cl 2 in the marine boundary layer.

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Section: Experimental Methodsmentioning

confidence: 99%

Section: à2mentioning

confidence: 99%

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Knudsen cell studies of the reactions of N2O5 and ClONO2 with NaCl: development and application of a model for estimating available surface areas and corrected uptake coefficients

Hoffman

Gebel

Fox

et al. 2003

Phys. Chem. Chem. Phys.

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“…For this evaluation, sensitivity runs were carried out. The magnitude of γ HNO 3 ,ss has been investigated in many laboratory experiments (e.g., Fenter et al, 1994;Laux et al, 1994;Abbatt and Waschewsky, 1998;Davies and Cox, 1998;Guimbud et al, 2002;Ghosal and Hemminger, 2004;Tolocka et al, 2004;Saul et al, 2006;Liu et al, 2007). However, as shown in Table 4, γ HNO 3 ,ss ranges widely from ∼10 −1 to ∼10 −4 .…”

Section: Observations Vs Model-predictionsmentioning

confidence: 99%

Investigation of ship-plume chemistry using a newly-developed photochemical/dynamic ship-plume model

et al. 2009

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Abstract.A photochemical/dynamic ship-plume model, which can consider the ship-plume dynamics and ship-plume chemistry, simultaneously, was developed to gain a better understanding of atmospheric impact of ship emissions. The model performance was then evaluated by a comparison with the observation data measured on a NOAA WP-3D flight during the Intercontinental Transport and Chemical Transformation 2002 (ITCT 2K2) airborne field campaign. The simulation conditions and parameters, such as meteorological conditions, emission rates, and background gas and particulate species concentrations, were obtained directly and/or inferred indirectly from the ITCT 2K2 observation data. The model-predicted concentrations showed good agreement with the observed concentrations of five ambient species (NO x , NO y , ozone, HNO 3 , and H 2 SO 4 ) at the eight plume transects by the WP-3D flight with strong correlations around the 1:1 line (0.64≤R≤0.85). In addition, a set of tests were carried out to approximate the magnitude of the reaction probability of HNO 3 onto sea-salt particles in the model-observation comparison framework. These results suggest that the reaction probability of HNO 3 onto seasalt particles may be in the order of 0.05-0

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“…That storm brought in marine air, increasing Cl − to about 1500 ng/g. It can then be hypothesized that the reaction (2) led to HNO 3 deposition to the snow (Fenter et al, 1994). The rate obviously depends on the concentration of NaCl, and thus would be much more efficient at Ny-Ålesund, relative to pre-storm Alert.…”

Section: Sources Of Nomentioning

confidence: 99%

Fluxes of nitrates between snow surfaces and the atmosphere in the European high Arctic

Beine¹,

Dominé

Ianniello³

et al. 2003

Atmos. Chem. Phys.

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Abstract. Measurements of atmospheric and snow mixing ratios of nitrates and nitrites and their fluxes above the snow surface were made during two intensive campaigns during spring time 2001 at Ny-Ålesund, Svalbard as part of the EU project "The NItrogen Cycle and Effects on the oxidation of atmospheric trace species at high latitudes" (NICE).At this coastal site close to the unseasonably unfrozen fjord, of the measured nitrogen species, only HNO 3 showed a significant flux on to the snow surface; a mean deposition of −8.7 nmol h −1 m −2 was observed in late April / early May 2001. These fluxes may be due to the reaction of HNO 3 with sea salt, and especially NaCl, or may be simply uptake of HNO 3 by ice, which is alkaline because of the sea salt in our marine environment. During snowfall periods dry deposition of HNO 3 may contribute up to 10% of the N budget in the snow; however, the main source for N is wet deposition in falling snow.The surface snow at Ny-Ålesund showed very complex stratigraphy; the NO − 3 mixing ratio in snow varied between 65 and 520 ng g −1 , the total NO − 3 content of the snowpack was on the order of 2700 ng cm −2 . In comparison the atmospheric boundary layer column showed a NO − 3 content of only 8 ng cm −2 . The limited exchange, however, between the snow and the atmosphere was attributed to low mobility of NO − 3 in the observed snow. Contrary to other Arctic sites (i.e. Alert, Nunavut or Summit, Greenland) deposition of sea salt and crustal aerosols in this marine environment made the surface snow alkaline; snow NO − 3 was associated with heavier cations and was not readily available for physical exchange or photochemical reactions.

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Kinetics of Nitric Acid Uptake by Salt

Cited by 100 publications

References 9 publications

Knudsen cell studies of the reactions of N2O5 and ClONO2 with NaCl: development and application of a model for estimating available surface areas and corrected uptake coefficients

Knudsen cell studies of the reactions of N2O5 and ClONO2 with NaCl: development and application of a model for estimating available surface areas and corrected uptake coefficients

Investigation of ship-plume chemistry using a newly-developed photochemical/dynamic ship-plume model

Fluxes of nitrates between snow surfaces and the atmosphere in the European high Arctic

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