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Factors Influencing Methyl Iodide Production in the Ocean and Its Flux to the Atmosphere

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Factors Influencing Methyl Iodide Production in the Ocean and Its Flux to the Atmosphere Factors influencing methyl iodide production in the ocean and its flux to the atmosphere Dissertation zur Erlangung des Doktorgrades der Mathematisch-Naturwissenschaftlichen Fakultät der Christian-Albrechts-Universität zu Kiel vorgelegt von Uwe Richter Kiel 2003 1 Referent: Prof. Dr. D.W.R. Wallace Korreferent: Prof. Dr. A. Körtzinger Tag der mündlichen Prüfung: 5.2.2004 Zum Druck genehmigt: 15.3.2004 gez. Prof. Dr. Wulf Depmeier 2 Table of contents Abstract ................................................................................................................6 Zusammenfassung ...............................................................................................7 1. Introduction .....................................................................................................8 1.1 Natural halocarbons ....................................................................................8 1.2 Methyl iodide in the atmosphere................................................................10 1.2.1 Sources for the atmosphere....................................................................................... 10 1.2.2 Sinks in the atmosphere............................................................................................ 12 1.3 Methyl iodide in the ocean .........................................................................13 1.3.1 Sources for the ocean................................................................................................ 14 1.3.2 Oceanic sinks............................................................................................................ 15 1.4 Goal of the present study............................................................................16 2. Data collecting methods................................................................................17 2.1 Cruise tracks...............................................................................................17 2.2 Methods for halocarbon measurements.....................................................18 2.3 Equilibrator................................................................................................20 2.4 Traps...........................................................................................................23 2.4.1 Traps for removing water ......................................................................................... 23 2.4.2 Traps for concentration of analytes .......................................................................... 23 2.5 Gas chromatographic system.....................................................................25 2.6 Water samples ............................................................................................27 2.7 Air samples .................................................................................................28 2.8 Standards....................................................................................................28 3 2.9 Water vapour correction ............................................................................30 2.10 Chlorophyll measurements.......................................................................31 3. Underway data...............................................................................................32 3.1 Air samples .................................................................................................32 3.2 Surface water samples................................................................................34 3.2.1 Henry’s law constant ................................................................................................ 34 3.2.2 Surface water concentrations.................................................................................... 35 3.3 Flux calculations ........................................................................................36 3.3.1 Transfer velocity....................................................................................................... 38 3.3.2 Schmidt number........................................................................................................ 40 3.3.3 Wind speed corrections ............................................................................................ 42 3.3.4 Concentration anomaly............................................................................................. 43 3.3.5 Methyl iodide flux calculations ................................................................................ 43 3.4 Discussion of the underway data ...............................................................48 4. Incubation experiments ................................................................................57 4.1 Introduction................................................................................................57 4.2 Methods ......................................................................................................59 4.2.1 Incubation flasks....................................................................................................... 59 4.2.2 Experimental protocol .............................................................................................. 61 4.3 Results.........................................................................................................63 4.4 Discussion...................................................................................................72 4.4.1 Freshwater controls................................................................................................... 76 4.4.2 Production rates ........................................................................................................ 77 5. Discussion.......................................................................................................82 5.1 Flux calculations ........................................................................................82 5.1.1 Proxies for methyl iodide?........................................................................................ 83 5.1.2 Global ocean atmosphere flux .................................................................................. 86 4 5.2 Global budget of methyl iodide..................................................................90 5.2.1 Sources and sinks of oceanic methyl iodide ............................................................. 92 5.3 Future research ..........................................................................................97 5.4 Conclusions ................................................................................................98 6. Literature .......................................................................................................99 Abbreviations and symbols ............................................................................111 List of figures ...................................................................................................114 List of tables.....................................................................................................115 5 Abstract Methyl iodide is an atmospheric trace gas and a major source of atmospheric iodine. Recent estimates of methyl iodide sources and sinks indicate that anthropogenic sources are neglectible. The major source of atmospheric methyl iodide are emissions from the ocean. The production pathways of methyl iodide in the ocean are, however, poorly understood. The known oceanic sources can only account for about 10 % of the ocean-atmosphere flux, whereas the sources for the remaining 90 % are not known. In this work a measuring system, consisting of an equilibrator connected to a 2-dimensional gas chromatograph, equipped with two electron capture detectors, was developed. This system was used on four cruises in the tropical and North Atlantic to measure the seawater concentrations and the atmospheric dry gas mole fractions of methyl iodide, and the ocean- atmosphere flux was calculated. A mean flux of ~22 nmol m-2 d-1 was calculated from all cruises. A global annual flux of 2.89 Gmol a-1 was estimated using this flux. The limiting factor for the methyl iodide flux seems to be the production in the ocean, because the measured fluxes were relatively uniform and independent from observed changes in the surface water concentrations and wind speeds. Incubation experiments were done in the tropical Atlantic to test the hypothesis that methyl iodide is produced in the surface water by a photochemical pathway, instead direct biological production by phytoplankton or bacteria. During the experiments untreated, filtered and poisoned seawater was incubated at ambient water temperature, either in the sunlight or in the dark. The production of methyl iodide observed in all incubations kept in the sunlight was five times higher than the production from incubations kept in the dark. No significant difference was observed between untreated, filtered and poisoned samples. This strongly indicates a photochemical production with no direct influence by biota. The mean photochemical production rate from all incubations was 0.12 nmol m-3 h-1. A layer of 14 m with this production rate is needed to balance the methyl iodide sinks from the halogen exchange reaction with chloride in the mixed layer and the flux to the atmosphere, based on model calculations. The global photochemical production of methyl iodide was estimated to be 5.3 Gmol a-1, using the measured production rate and a the calculated layer depth of 14 m. From these results the photochemical production of methyl
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