Estimation of the rate constant for the reaction of acid sulphate aerosol with NH3 gas from atmospheric measurements

Harrison, Roy M.; Kitto, Abdul-Massih N.

doi:10.1007/bf00053755

Cited by 48 publications

(18 citation statements)

References 37 publications

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“…We hypothesise that away from significant terrestrial influence, any un-neutralised sulfate acidity in the atmosphere will A Harrison and Kitto [50] found kinetic control of aerosol sulfate neutralisation by NH 3 during a 'connected flow' study over S.E. England.…”

Section: Coupling Of Dms Emission and Nh 3 Fluxmentioning

confidence: 99%

“…We adopt a time constant for this process that results in 95% equilibration over ∼1 h, in keeping with the observations and models of Harrison and Kitto [50] and Quinn et al [22] Initial conditions and default parameter values are selected to represent typical 'average' conditions in the global remote ocean and MBL, particularly the Southern Ocean. The seawater ammonium concentration is taken as a high-latitude average concentration of 150 nM after Johnson [21] ; the sulfate input is considered as a per-unit area flux and is taken as the mean value of the Southern Ocean DMS flux observed by Shon et al [51] (1.3 µmol m −2 day −1 ), multiplied by their mean observed SO 2 conversion factor of 0.6, giving a sulfate input of 0.5 nmol m −2 min −1 .…”

Section: Model Descriptionmentioning

confidence: 99%

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Coupling between dimethylsulfide emissions and the ocean - atmosphere exchange of ammonia

Johnson

Bell

2008

Environ. Chem.

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Environmental context. Dimethylsulfide (DMS) is recognised as a potentially significant climate-forcing gas, owing to its role in particle and cloud formation in the marine atmosphere, where it is the dominant source of acidity. Ammonia, the dominant naturally occurring base in the atmosphere, plays an important role in neutralising particles formed from DMS oxidation products and may even enhance the formation rate of new particles. A biogeochemical coupling has previously been proposed between DMS and ammonia fluxes from the ocean to the atmosphere, in the form of coproduction of the two gases in seawater. We revise this suggestion by introducing the concept of 'co-emission' of the gases, where DMS emission controls the rate of emission of ammonia from the ocean by acidifying the atmosphere. Abstract.A strong correlation between aerosol ammonium and non-sea salt sulfate is commonly observed in the remote marine boundary layer. It has been suggested that this relationship implies a biogeochemical linkage between the nitrogen (N) and sulfur (S) cycles at the cellular biochemical level in phytoplankton in the ocean, or a linkage in the atmosphere (see P. S. Liss and J. N. Galloway, Interactions of C, N, P and S biogeochemical cycles and global change (Springer, 1993), and P. K. Quinn et al. in J. Geophys. Res. -Atmos. 1990, 95). We argue that an oceanic linkage is unlikely and draw on mechanistic and observational evidence to make the argument that the atmospheric connection is based on simple physical chemistry. Drawing on an established analogous concept in terrestrial trace gas biogeochemistry, we propose that any emission of dimethylsulfide (DMS) from the ocean will indirectly influence the flux of NH 3 from the ocean, through the neutralisation of acidic DMS oxidation products and consequent lowering of the partial pressure of NH 3 in the atmosphere. We present a simple numerical model to investigate this hypothesised phenomenon, using a parameterisation of the rate and thermodynamics of gas-to-particle conversion of NH x and explicitly modelled oceanatmosphere NH 3 exchange. The model indicates that emission of acidic sulfur to the atmosphere (e.g. as a product of DMS oxidation) may enhance the marine emission of NH 3 . It also suggests that the ratio of ammonium to non-sea salt sulfate in the aerosol phase is strongly dependent on seawater pH, temperature and wind speed -factors that control the ocean-atmosphere ammonia flux. Therefore, it is not necessary to invoke a stoichiometric link between production rates of DMS and ammonia in the ocean to explain a given ammonium to non-sea salt sulfate ratio in the aerosol. We speculate that this mechanism, which can provide a continuous resupply of ammonia to the atmosphere, may be involved in a series of biogeochemical-climate feedbacks. His research interests are biogeochemical cycles taking place both within and between the ocean and its overlying atmosphere, with a focus on biogenic trace gases. He is currently working with Peter Liss as part of the Surfac...

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Section: Coupling Of Dms Emission and Nh 3 Fluxmentioning

confidence: 99%

Section: Model Descriptionmentioning

confidence: 99%

Coupling between dimethylsulfide emissions and the ocean - atmosphere exchange of ammonia

Johnson

Bell

2008

Environ. Chem.

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“…Even so, Harrison and Kitto [100] carried out this determination by measuring the conversion of NH3 to NH4 + as the air mass traveled between three successive distant sampling points in rural England. They established that the sum of the concentrations [H++NH|] as well as the ratio [H++NHj]/[SO^_-l-NO^] remained constant indicating no significant ammonia input during travel.…”

Section: Reaction Of Ammonia With Sulfuric and Sulfate Aerosols Undermentioning

confidence: 99%

Fate of ammonia in the atmosphere?a review for applicability to hazardous releases

Renard

Calidonna

Henley³

2004

Journal of Hazardous Materials

141

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“…In principle it is possible to estimate these reaction rates from field experiments using the changes in the ratio NH $ :NH % + in air as a function of the vertical or horizontal distance Harrison & Kitto, 1992). However, many assumptions have to be made and results vary.…”

Section:  mentioning

confidence: 99%

Ammonia: emission, atmospheric transport and deposition

Asman¹,

Sutton

Schjørring³

1998

New Phytologist

517

292

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The global emission of ammonia (NH $ ) is about 54 Mt N. The major global sources are excreta from domestic animals and fertilizers, but oceans, biomass burning and crops are also important. About 60 % of the global NH $ emission is estimated to come from anthropogenic sources. NH $ -N emissions are of the same order as the NO x -N emissions on both global and European scales. Emitted NH $ returns to the surface mainly in the form of dry deposition of NH $ and wet deposition of ammonium (NH % + ). In countries with high NH $ emission densities, dry deposition of NH $ from local sources and wet deposition of NH % + from remote sources dominate the deposition. In countries with low NH $ emission densities only wet deposition of NH % + from remote sources dominates the deposition. Surface exchange of NH $ is essentially bi-directional, depending on the NH $ compensation point concentration of the vegetation and the airborne concentration. In general, the compensation point is larger for agricultural than semi-natural plants, and varies with plant growth stage. According to basic thermodynamics the leaf tissue or stomatal compensation point of NH $ doubles for each increase of 5 mC. However, exchange of NH $ does not only occur through the stomata, but it can also be deposited to leaf surfaces, as well as emitted back to the atmosphere from drying leaf surfaces. Atmospheric transport and deposition models can be used to interpolate NH $ concentrations and depositions in space and time, to calculate import\export balances and to estimate past or future situations. Adverse effects on sensitive ecosystems caused by high N deposition can be reduced by lowering the emissions and, to a limited extent, also by removing sources close to the ecosystem to be protected.

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Estimation of the rate constant for the reaction of acid sulphate aerosol with NH3 gas from atmospheric measurements

Cited by 48 publications

References 37 publications

Coupling between dimethylsulfide emissions and the ocean - atmosphere exchange of ammonia

Coupling between dimethylsulfide emissions and the ocean - atmosphere exchange of ammonia

Fate of ammonia in the atmosphere?a review for applicability to hazardous releases

Ammonia: emission, atmospheric transport and deposition

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