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  • 1
    Electronic Resource
    Electronic Resource
    Springer
    Aquatic geochemistry 1 (1995), S. 355-374 
    ISSN: 1573-1421
    Keywords: aerosol dissolution ; atmosphere ; rainwater ; seawater ; trace metals ; speciation ; pH cycling ; photochemistry ; particulate load
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Previous work has shown that the type and pH history of an aerosol governs trace metal solubility in rainwater. This study concentrates on the crustal elements Al, Fe and Mn and identifies additional processes which affect dissolution not only in the atmosphere but also on mixing into seawater. Aerosol dissolution experiments (at aerosol concentrations of about 30 mg 1−1) show manganese exhibiting high solubility at the low pH values typical of clouds (54±2.5% at pH 2, with results expressed in mole percent units) with 85% of this increase occurring within 6 hours of acidification. The percentage dissolution decreases to 50% at pH values representative of rainwater (pH 5.5) and to 26±4% at pH 8, typical of seawater. No such dramatic solution phase removal occurs at pH 8 in the presence of inorganic anions (to a final solubility of 44±2%). Thus the extent of manganese dissolution depends strongly on whether aerosols are cycled through acidic environments and on subsequent inorganic complexation once rainwater mixes into sea. Aluminium shows highest dissolution (7.1±0.6%) at low pH with 78% of this increase occurring within 6 hours of acidification. Rapid solution phase removal occurs on increasing the pH to that representative of rainwater (to 0.9±0.4% with 87% of this decrease occurring within 15 min). As a consequence of acid cycling and aluminium's amphoteric nature, solubility is enhanced at seawater pH (2.3±0.3%) over that in rain. Iron shows a strong pH-solubility relationship with highest solubility at low pH (4.7±0.2%), 70% of this value being reached within 6 hours of acidification, and decreasing rapidly to 0.17% as pH is raised to 8. Addition of inorganic anions at pH 8 to simulate mixing into seawater causes a further decrease in solubility, perhaps due to anion induced colloid destabilisation. Photochemical reduction also effects solubility under low pH conditions with Fe(II) comprising 1% of the total iron in the Saharan Aerosol used and 8.4% in an Urban material at a pH of ≈ 2. This element shows rapid solution phase removal with increasing particulate load which is tentatively rationalised in terms of a simple Kd approach.
    Type of Medium: Electronic Resource
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  • 2
    Publication Date: 2019-05-22
    Type: Conference or Workshop Item , NonPeerReviewed
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  • 3
    Publication Date: 2014-01-27
    Description: Dissolved iron (dFe) distributions and atmospheric and vertical subduction fluxes of dFe were determined in the upper water column for two meridional transects of the Atlantic Ocean. The data demonstrate the disparity between the iron biogeochemistry of the North and South Atlantic Ocean and show well-defined gradients of size fractionated iron species in surface waters between geographic provinces. The highest dFe and lowest mixed layer residence times (0.4–2.5 years) were found in the northern tropical and subtropical regions. In contrast, the South Atlantic Gyre had lower dFe concentrations (〈0.4 nM) and much longer residence times (〉5 years), presumably due to lower atmospheric inputs and more efficient biological recycling of iron in this region. Vertical input fluxes of dFe to surface waters ranged from 20 to 170 nmol m–2 d–1 in the North Atlantic and tropical provinces, whereas average fluxes of 6–13 nmol m–2 d–1 were estimated for the South Atlantic. Our estimates showed that the variable dFe distribution over the surface Atlantic (〈0.1–2.0 nM) predominantly reflected atmospheric Fe deposition fluxes (〉50% of total vertical Fe flux to surface waters) rather than upwelling or vertical mixing. This demonstrates the strength of the connection between land-derived atmospheric Fe fluxes and the biological cycling of carbon and nitrogen in the Atlantic Ocean.
    Type: Article , PeerReviewed
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  • 4
    Publication Date: 2023-02-08
    Description: An ocean iodine cycling model is presented, which predicts upper ocean iodine speciation. The model comprises a three-layer advective and diffusive ocean circulation model of the upper ocean, and an iodine cycling model embedded within this circulation. The two primary reservoirs of iodine are represented, iodide and iodate. Iodate is reduced to iodide in the mixed layer in association with primary production, linked by an iodine to carbon (I:C) ratio. A satisfactory model fit with observations cannot be obtained with a globally constant I:C ratio, and the best fit is obtained when the I:C ratio is dependent on sea surface temperature, increasing at low temperatures. Comparisons with observed iodide distributions show that the best model fit is obtained when oxidation of iodide back to iodate is associated with mixed layer nitrification. Sensitivity tests, where model parameters and processes are perturbed, reveal that primary productivity, mixed layer depth, oxidation, advection, surface fresh water flux and the I:C ratio all have a role in determining surface iodide concentrations, and the timescale of iodide in the mixed layer is sufficiently long for non-local processes to be important. Comparisons of the modelled iodide surface field with parameterisations by other authors shows good agreement in regions where observations exist, but significant differences in regions without observations. This raises the question of whether the existing parameterisations are capturing the full range of processes involved in determining surface iodide, and shows the urgent need for observations in regions where there are currently none.
    Type: Article , PeerReviewed
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  • 5
    Publication Date: 2019-05-22
    Type: Conference or Workshop Item , NonPeerReviewed
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  • 6
    Publication Date: 2024-02-07
    Description: Reaction with iodide (I-) at the sea surface is an important sink for atmospheric ozone, and causes sea-air emission of reactive iodine which in turn drives further ozone destruction. To incorporate this process into chemical transport models, improved understanding of the factors controlling marine iodine speciation, and especially sea-surface iodide concentrations, is needed. The oxidation of I- to iodate (IO3-) is the main sink for oceanic I-, but the mechanism for this remains unknown. We demonstrate for the first time that marine nitrifying bacteria mediate I- oxidation to IO3-. A significant increase in IO3- concentrations compared to media-only controls was observed in cultures of the ammonia-oxidising bacteria Nitrosomonas sp. (Nm51) and Nitrosoccocus oceani (Nc10) supplied with 9-10 mM I-, indicating I- oxidation to IO3-. Cell-normalised production rates were 15.69 (+/- 4.71) fmol IO3- cell(-1) d(-1) for Nitrosomonas sp., and 11.96 (+/- 6.96) fmol IO3- cell(-1) d(-1) for Nitrosococcus oceani, and molar ratios of iodate-to-nitrite production were 9.2 +/- 4.1 and 1.88 +/- 0.91 respectively. Preliminary experiments on nitrite-oxidising bacteria showed no evidence of I- to IO3- oxidation. If the link between ammonia and I oxidation observed here is representative, our ocean iodine cycling model predicts that future changes in marine nitrification could alter global sea surface I fields with potential implications for atmospheric chemistry and air quality.
    Type: Article , PeerReviewed
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  • 7
    Publication Date: 2024-02-07
    Description: The discovery of atmospheric micro(nano)plastic transport and ocean–atmosphere exchange points to a highly complex marine plastic cycle, with negative implications for human and ecosystem health. Yet, observations are currently limited. In this Perspective, we quantify the processes and fluxes of the marine-atmospheric micro(nano)plastic cycle, with the aim of highlighting the remaining unknowns in atmospheric micro(nano)plastic transport. Between 0.013 and 25 million metric tons per year of micro(nano)plastics are potentially being transported within the marine atmosphere and deposited in the oceans. However, the high uncertainty in these marine-atmospheric fluxes is related to data limitations and a lack of study intercomparability. To address the uncertainties and remaining knowledge gaps in the marine-atmospheric micro(nano)plastic cycle, we propose a future global marine-atmospheric micro(nano)plastic observation strategy, incorporating novel sampling methods and the creation of a comparable, harmonized and global data set. Together with long-term observations and intensive investigations, this strategy will help to define the trends in marine-atmospheric pollution and any responses to future policy and management actions.
    Type: Article , PeerReviewed
    Format: other
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  • 8
    Publication Date: 2022-11-03
    Description: The discovery of atmospheric micro(nano)plastic transport and ocean–atmosphere exchange points to a highly complex marine plastic cycle, with negative implications for human and ecosystem health. Yet, observations are currently limited. In this Perspective, we quantify the processes and fluxes of the marine-atmospheric micro(nano)plastic cycle, with the aim of highlighting the remaining unknowns in atmospheric micro(nano)plastic transport. Between 0.013 and 25 million metric tons per year of micro(nano)plastics are potentially being transported within the marine atmosphere and deposited in the oceans. However, the high uncertainty in these marine-atmospheric fluxes is related to data limitations and a lack of study intercomparability. To address the uncertainties and remaining knowledge gaps in the marine-atmospheric micro(nano)plastic cycle, we propose a future global marine-atmospheric micro(nano)plastic observation strategy, incorporating novel sampling methods and the creation of a comparable, harmonized and global data set. Together with long-term observations and intensive investigations, this strategy will help to define the trends in marine-atmospheric pollution and any responses to future policy and management actions.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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