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NOTES and CORRESPONDENCE Nitric Acid–Sea Salt Reactions MAY 2000 NOTES AND CORRESPONDENCE 725 NOTES AND CORRESPONDENCE Nitric Acid±Sea Salt Reactions: Implications for Nitrogen Deposition to Water Surfaces S. C. PRYOR Atmospheric Science Program, Department of Geography, Indiana University, Bloomington, Indiana L. L. SùRENSEN Department of Wind Energy and Atmospheric Physics, Risù National Laboratory, Roskilde, Denmark 23 August 1999 and 20 October 1999 ABSTRACT Many previous studies have indicated the importance of nitric acid (HNO3) reactions on sea salt particles for ¯ux divergence of HNO3 in the marine surface layer. The potential importance of this reaction in determining the spatial and temporal patterns of nitrogen dry deposition to marine ecosystems is investigated using models of sea spray generation and particle- and gas-phase dry deposition. Under horizontally homogeneous conditions 21 with near-neutral stability and for wind speeds between 3.5 and 10 m s , transfer of HNO3 to the particle phase to form sodium nitrate may decrease the deposition velocity of nitrogen by over 50%, leading to greater horizontal transport prior to deposition to the sea surface. Conversely, for wind speeds above 10 m s21, transfer of nitrogen to the particle phase would increase the deposition rate and hence decrease horizontal transport prior to surface removal. 1. Introduction spheric ¯ux is uncertain and highly variable spatially, Paerl (1995) summarizes data that suggest dry deposi- a. Nitrogen deposition to aquatic ecosystems tion is a signi®cant contributor to the atmospheric ¯ux Most oceanic primary production by phytoplankton to all of the major oceans (i.e., dry deposition is greater is limited by nutrient availability. The limiting nutrients than 20% of the total ¯ux), and model calculations for commonly are nitrogen (N) and phosphorous (P). In- the seas around Denmark indicate that one-third of the creasing N and P concentrations have profound impli- total N comes from the atmosphere and approximately cations for ecosystem health and productivity. For ex- three-®fths of the atmospheric deposition (via wet and ample, Paerl (1995) suggests ``nitrogen-limited estuar- dry pathways) comes from particulate matter (Asman ies, shallow coastal and continental shelf waters account et al. 1995). It also has been suggested that atmospheric for nearly half the global oceanic primary production.'' ¯uxes to midlatitude coastal areas may be largest in the 22 Typically, absorption of nitrate (NO32 ), nitrite ( NO ), late spring and summer months, when nutrient concen- 1 and ammonium (NH4 ) from ocean waters supplies N trations are generally at a minimum and hence the effect required by organisms. Human activity has increased of this ¯ux may be disproportionately large (Fisher and the concentration of these and other N compounds in Oppenheimer 1991; Rendell et al. 1993). coastal waters, leading in some cases to greatly en- Nitrogen deposition is determined largely by emis- hanced primary production or eutrophication (Paerl sions of the following N-containing gases: nitric oxide 1995). A number of studies indicate that between 10% (NO), nitrogen dioxide (NO2), ammonia (NH3), and ni- and more than 50% of coastal N loading is attributable trous oxide (N2O). Nitric acid (HNO3) is formed prin- to atmospheric ¯uxes (e.g., Paerl 1995; Rendell et al. cipally as a result of NO and NO2 and has been shown 1993). Although the contribution of wet and dry de- to make a signi®cant contribution to total N deposition position and gas- and particle-phase N to this atmo- in a number of diverse terrestrial and marine environ- ments [e.g., in the studies of Sievering et al. (1992), Pryor et al. (1999b), and Asman et al. (1995), HNO3 deposition contributed approximately 10% of the total Corresponding author address: S. C. Pryor, Atmospheric Science N ¯ux]. Program, Dept. of Geography, Indiana University, Bloomington, IN 47405. Nitrogen emissions to the atmosphere are currently E-mail: [email protected] twice ``natural background'' levels (Vitousek et al. q 2000 American Meteorological Society Unauthenticated | Downloaded 09/29/21 08:33 AM UTC 726 JOURNAL OF APPLIED METEOROLOGY VOLUME 39 1997) and are predicted to increase by 25%±50% in less-developed regions by 2020 (Galloway et al. 1994). These projections indicate the importance of improved understanding of atmosphere±surface exchange and the potential for an enhanced role of atmospheric deposition in eutrophication problems in the twenty-®rst century. b. Dry deposition processes Because of dif®culties in direct measurement of dry deposition ¯uxes of particles and some gases, dry de- position often is determined by the ``concentration method'' in which the ¯ux F is given by multiplication FIG. 1. A schematic of the particle deposition model, illustrating of the concentration at some level above the surface by that the model is composed of two layers, a well-mixed turbulent a deposition velocity: layer in which gravitational settling and turbulent transport are re- sponsible for the transfer of particles toward the surface, and the F 52y d(z)[C(z) 2 C(0)], (1) quasi-laminar surface layer in which gravitational settling of ``wet'' particles and diffusional transport are the primary transport mecha- where C(z) is concentration at measurement height z; nisms. This ®gure is adapted from Hummelshùj et al. (1992). C(0) is concentration at the surface (which may be zero depending on surface uptake); y d(z) 5 deposition ve- locity, which may be computed as the inverse of the to the ¯ux at the surface). Flux divergence (i.e., violation sum of a number of resistances plus a gravitational set- of this assumption), however, may occur because of tling term for particles: advection, storage effects, or chemical reactions be- 1 tween the measurement height and the ground (Kramm y dg51y . (2) and Dlugi 1994). Reaction of HNO3 on sea salt (NaCl) rabc1 r 1 r particles to yield sodium nitrate (NaNO3) in the particle In Eq. (2) the following are true. phase and volatize hydrochloric acid vapor (HCl) is a potentially important source of ¯ux divergence of HNO3 1) ra is aerodynamic resistance. This term represents the resistance to transport by turbulence to the quasi- over the sea surface (Geernaert et al. 1998). This chem- laminar surface layer. ical reaction and others on and in sea salt aerosols also have been shown to play critical roles in halogen (par- 2) rb is quasi-laminar surface layer resistance. Very close to the surface, a laminar boundary layer forms ticularly chlorine and bromine) release in the marine (depth ø 100±1000 mm), which essentially is free boundary layer (Sander and Crutzen 1996), which has of turbulence. Transport across this layer is largely been linked to ozone depletion [e.g., the rapid decrease the result of Brownian diffusion. in ozone concentrations in Arctic air masses during the spring (Barrie et al. 1988)]. 3) rc is surface resistance. For highly reactive or soluble gases the surface resistance is small. We assume a In this note, the reaction of HNO3 on sea salt is con- surface resistance of zero and 100% ef®cient surface sidered from a different perspective. The rate constant capture for particle deposition to water surfaces. for the HNO3±NaCl reaction is thought to be rapid (Fen- ter et al. 1994), and the reaction has a large equilibrium 4) y g is gravitational settling velocity. For coarse-mode particles, the downward gravitational force exceeds constant (Seinfeld and Pandis 1998), so, given suf®cient the drag force from the viscosity of air, and hence particle surface area (and time), the reaction is expected to reach completion with near total transfer of N to the y g is important. This transport process is negligible for gases and ®ne particles, however. particle phase. Here a ®rst analysis of the potential role of this reaction in modifying atmosphere±surface ¯uxes Additional processes that may be of importance to of N is presented. It is demonstrated that this transfer particle dry deposition but are not considered here in- of N from the gas to the particle phase has the potential clude interception and inertial forces, electrical migra- to modify substantially the spatial and temporal patterns tion due to surface charge, and thermophoresis caused of the ¯ux of N to the sea surface. by temperature gradients (see Zufall and Davidson 1998). 2. Modeling particle dry deposition to water surfaces c. The focus of this note a. Description of the model The majority of studies of dry deposition ¯uxes to surfaces explicitly or implicitly rely upon the constant Here the model of particle dry deposition velocity ¯ux layer assumption (i.e., that the measured or deter- described by Pryor et al. (1999) and based on work by mined ¯ux at a given height above the surface is equal Williams (1982) and Hummelshùj et al. (1992) is used. Unauthenticated | Downloaded 09/29/21 08:33 AM UTC MAY 2000 NOTES AND CORRESPONDENCE 727 A schematic of the model is shown in Fig. 1. The form of the model is (y h1 y g,d)(y d 1 y g,w) y d 5 , (3) y h 1 y d 1 y g,d where y h is transfer velocity in the layer dominated by turbulent transfer, y g,d and y g,w are gravitational settling transfer velocities (subscripts d and w indicate dry and wet particles, respectively, where dry particles are those present in the marine atmosphere above the quasi-lam- inar surface layer, and wet particles refer to particles that have taken up water as they approach the surface and are subject to higher humidities), and y d is transfer velocity across laminar surface layer. These terms are given by the following equations. 1) Transfer velocity due to turbulent processes: 1 y h 5 , (4) 1 zzz ln rr0m 2Chh 1C FIG. 2.
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