Release of NOx from sunlight‐irradiated midlatitude snow

Honrath, R. E.; Peterson, Matt A.; Dziobak, M. P.; Dibb, Jack E.; Arsenault, Matthew; Green, Sarah

doi:10.1029/1999gl011286

Cited by 154 publications

(145 citation statements)

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“…At the relative humidity of !40% observed during the measurement intensive, there should be at least several monolayers of water on the glass manifold wall surfaces [Svensson et al, 1987;Saliba et al, 2001]. Thus the produced NO 2(ads) may react rapidly with adsorbed H 2 O to produce HONO, which is then released from the surface into the air [Pitts et al, 1984] This mechanism is consistent with the recent observations of photochemical production of HONO [Zhou et al, 2001] and NO x [Honrath et al, 1999[Honrath et al, , 2000 in snowpack from nitrate/HNO 3 photolysis. These observations are also supportive of a recent hypothesis that the photolysis of adsorbed HNO 3 /nitrate on ground surfaces is a major daytime source of HONO and thus is responsible for the observed elevated HONO concentrations in the rural atmospheric boundary layer .…”

Section: Resultssupporting

confidence: 77%

Photochemical production of nitrous acid on glass sample manifold surface

Zhou

Huang

et al. 2002

Geophysical Research Letters

124

134

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[1] Significant production of HONO was observed on glass sample manifold wall surface when exposed to sunlight during the PROPHET 2000 summer measurement intensive. It is hypothesized that the artifact HONO was produced by photolysis of adsorbed nitric acid/nitrate on the manifold wall surfaces followed by the subsequent reaction of produced NO 2 and adsorbed H 2 O on surface. This observation suggests against the use of an unshielded glass manifold as a sampling inlet for the measurement of atmospheric HONO. It may also have some implications in interpreting field NO x data measured using similar glass inlet manifolds, especially from the clean remote environments where NO x is low and HNO 3 is a major fraction of NO y .

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Section: Resultssupporting

confidence: 77%

Photochemical production of nitrous acid on glass sample manifold surface

Zhou

Huang

et al. 2002

Geophysical Research Letters

124

134

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“…[22][23][24][25] Less is known about the photochemistry of nitrate in complex aerosol mixtures, such as in processed sea salt aerosols. Sea salt particles, whether processed or unprocessed, are likely to exist as concentrated aqueous droplets at ambient relative humidities.…”

Section: Introductionmentioning

confidence: 99%

Enhanced surface photochemistry in chloride–nitrate ion mixtures

Wingen

Moskun

Johnson

et al. 2008

Phys. Chem. Chem. Phys.

116

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Heterogeneous reactions of sea salt aerosol with various oxides of nitrogen lead to replacement of chloride ion by nitrate ion. Studies of the photochemistry of a model system were carried out using deliquesced mixtures of NaCl and NaNO 3 on a Teflon s substrate. Varying molar ratios of NaCl to NaNO 3 (1 : 9 Cl À : NO 3 À , 1 : 1 Cl À : NO 3 À , 3 : 1 Cl À : NO 3 À , 9 : 1 Cl À : NO 3 À) and NaNO 3 at the same total concentration were irradiated in air at 299 AE 3 K and at a relative humidity of 75 AE 8% using broadband UVB light (270-380 nm). Gaseous NO 2 production was measured as a function of time using a chemiluminescence NO y detector. Surprisingly, an enhanced yield of NO 2 was observed as the chloride to nitrate ratio increased. Molecular dynamics (MD) simulations show that as the Cl À : NO 3 À ratio increases, the nitrate ions are drawn closer to the interface due to the existence of a double layer of interfacial Cl À and subsurface Na + . This leads to a decreased solvent cage effect when the nitrate ion photodissociates to NO 2 +O À , increasing the effective quantum yield and hence the production of gaseous NO 2 . The implications of enhanced NO 2 and likely OH production as sea salt aerosols become processed in the atmosphere are discussed.

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“…Emissions of nitrogen oxides, NO x = NO + NO 2 , from snow to the overlying air as a result of photolysis of the nitrate anion, NO − 3 , within snow have been observed in polar (Jones et al, 2001;Beine et al, 2002) and midlatitude regions (Honrath et al, 2000). They were found to have a significant impact on the oxidising capacity of the atmospheric boundary layer, especially in remote areas, such as the polar regions, where anthropogenic pollution is small (Grannas et al, 2007).…”

Section: Introductionmentioning

confidence: 99%

Modelling the physical multiphase interactions of HNO3 between snow and air on the Antarctic Plateau (Dome C) and coast (Halley)

2018

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Abstract. Emissions of nitrogen oxide (NO x = NO + NO 2 ) from the photolysis of nitrate (NO − 3 ) in snow affect the oxidising capacity of the lower troposphere especially in remote regions of high latitudes with little pollution. Current air-snow exchange models are limited by poor understanding of processes and often require unphysical tuning parameters. Here, two multiphase models were developed from physically based parameterisations to describe the interaction of nitrate between the surface layer of the snowpack and the overlying atmosphere. The first model is similar to previous approaches and assumes that below a threshold temperature, T o , the air-snow grain interface is pure ice and above T o a disordered interface (DI) emerges covering the entire grain surface. The second model assumes that air-ice interactions dominate over all temperatures below melting of ice and that any liquid present above the eutectic temperature is concentrated in micropockets. The models are used to predict the nitrate in surface snow constrained by year-round observations of mixing ratios of nitric acid in air at a cold site on the Antarctic Plateau (Dome C; 75 • 06 S, 123 • 33 E; 3233 m a.s.l.) and at a relatively warm site on the Antarctic coast (Halley; 75 • 35 S, 26 • 39 E; 35 m a.s.l). The first model agrees reasonably well with observations at Dome C (C v (RMSE) = 1.34) but performs poorly at Halley (C v (RMSE) = 89.28) while the second model reproduces with good agreement observations at both sites (C v (RMSE) = 0.84 at both sites). It is therefore suggested that in winter air-snow interactions of nitrate are determined by non-equilibrium surface adsorption and cocondensation on ice coupled with solid-state diffusion inside the grain, similar to Bock et al. (2016). In summer, however, the air-snow exchange of nitrate is mainly driven by solvation into liquid micropockets following Henry's law with contributions to total surface snow NO − 3 concentrations of 75 and 80 % at Dome C and Halley, respectively. It is also found that the liquid volume of the snow grain and airmicropocket partitioning of HNO 3 are sensitive to both the total solute concentration of mineral ions within the snow and pH of the snow. The second model provides an alternative method to predict nitrate concentration in the surface snow layer which is applicable over the entire range of environmental conditions typical for Antarctica and forms a basis for a future full 1-D snowpack model as well as parameterisations in regional or global atmospheric chemistry models.

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Release of NO_x from sunlight‐irradiated midlatitude snow

Abstract: Abstract.Photochemical production and release of gas-

Cited by 154 publications

References 10 publications

Photochemical production of nitrous acid on glass sample manifold surface

Photochemical production of nitrous acid on glass sample manifold surface

Enhanced surface photochemistry in chloride–nitrate ion mixtures

Modelling the physical multiphase interactions of HNO<sub>3</sub> between snow and air on the Antarctic Plateau (Dome C) and coast (Halley)

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Release of NOx from sunlight‐irradiated midlatitude snow

Abstract: Abstract.Photochemical production and release of gas-

Cited by 154 publications

References 10 publications

Photochemical production of nitrous acid on glass sample manifold surface

Photochemical production of nitrous acid on glass sample manifold surface

Enhanced surface photochemistry in chloride–nitrate ion mixtures

Modelling the physical multiphase interactions of HNO&lt;sub&gt;3&lt;/sub&gt; between snow and air on the Antarctic Plateau (Dome C) and coast (Halley)

Contact Info

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Release of NO_x from sunlight‐irradiated midlatitude snow

Modelling the physical multiphase interactions of HNO<sub>3</sub> between snow and air on the Antarctic Plateau (Dome C) and coast (Halley)