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  • 1
    Online Resource
    Online Resource
    Oceanic consumption of CH 3 CCl 3 : Implications for tropospheric OH
    American Geophysical Union (AGU) ; 1991
    In:  Journal of Geophysical Research: Atmospheres Vol. 96, No. D12 ( 1991-12-20), p. 22347-22355
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 96, No. D12 ( 1991-12-20), p. 22347-22355
    Abstract: Strong and extensive negative saturation anomalies for CH 3 CCl 3 were observed in the mid‐Pacific Ocean during the spring of 1990. Anomalies were largest at the equator, where upwelling and biological activity were greatest, but present virtually everywhere in our sampling range of 15°S to 20°N. The mean saturation anomaly for all of our data, corrected for physical effects, was −11.0%, implying that the ocean is a significant sink for CH 3 CCl 3 . The loss rate to maintain this anomaly is supported roughly by known hydrolysis rates, but contributions from other processes cannot be ruled out at this time. If hydrolysis and mixing are the only processes removing CH 3 CCl 3 from seawater, then about 6% of atmospheric CH 3 CCl 3 is removed by consumption in the oceans. Our data show that losses to the ocean most probably would range from 5 to 11% of the CH 3 CCl 3 removed from the atmosphere. This range translates to a partial residence time of 59–128 years for atmospheric CH 3 CCl 3 relative to oceanic consumption. Although these data indicate that the ocean is not an overwhelmingly large sink, its neglect does represent a systematic error in the calculation of tropospheric OH concentration from CH 3 CCl 3 production, growth, and distribution in the atmosphere.
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/91JD02126
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 1991
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  • 2
    Online Resource
    Online Resource
    Atmospheric hydrogen sulfide over the equatorial Pacific (SAGA 3)
    American Geophysical Union (AGU) ; 1993
    In:  Journal of Geophysical Research: Atmospheres Vol. 98, No. D9 ( 1993-09-20), p. 16979-16983
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 98, No. D9 ( 1993-09-20), p. 16979-16983
    Abstract: Atmospheric H 2 S concentrations were measured over the equatorial Pacific on leg 1 of the third Soviet‐American Gases and Aerosols (SAGA 3) cruise during February and March 1990. Five N‐S transects were made across the equator between Hawaii and American Samoa. The concentrations ranged from below the detection limit of 0.4 ± 0.5 (1 σ) to 14.4 ppt with an average value of 3.6 ± 2.3 ppt (1σ, n = 72). The highest concentrations were found on the easternmost two transects just south of the equator. The average concentration of 3.6 ppt observed on this cruise is the lowest reported value for background atmospheric H 2 S over the tropical oceans. A lack of correlation between 222 Rn and H 2 S rules out a significant continental source. Model calculations indicate that the oceanic source of H 2 S in this region is in the range of 9 to 21 × 10 −8 mol m −2 d −1 . From this flux the concentration of free sulfide (H 2 S + S = ) in the surface mixed layer of the ocean is estimated to be in the range of 32 to 67 pmol L −1 . In the atmosphere the oxidation of H 2 S produces SO 2 at a rate of 2.1 to 4.4 × 10 −11 mol m −3 d −1 which is only a small fraction of that estimated from the oxidation of dimethyl sulfide (DMS) in this region. A diurnal cycle was not observed in the H 2 S data recorded during this cruise.
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/92JD00451
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 1993
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  • 3
    Online Resource
    Online Resource
    A comprehensive estimate for loss of atmospheric carbon tetrachloride (CCl〈sub〉4〈/sub〉) to the ocean
    Copernicus GmbH ; 2016
    In:  Atmospheric Chemistry and Physics Vol. 16, No. 17 ( 2016-09-01), p. 10899-10910
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 17 ( 2016-09-01), p. 10899-10910
    Abstract: Abstract. Extensive undersaturations of carbon tetrachloride (CCl4) in Pacific, Atlantic, and Southern Ocean surface waters indicate that atmospheric CCl4 is consumed in large amounts by the ocean. Observations made on 16 research cruises between 1987 and 2010, ranging in latitude from 60° N to 77° S, show that negative saturations extend over most of the surface ocean. Corrected for physical effects associated with radiative heat flux, mixing, and air injection, these anomalies were commonly on the order of −5 to −10 %, with no clear relationship to temperature, productivity, or other gross surface water characteristics other than being more negative in association with upwelling. The atmospheric flux required to sustain these undersaturations is 12.4 (9.4–15.4) Gg yr−1, a loss rate implying a partial atmospheric lifetime with respect to the oceanic loss of 183 (147–241) yr and that  ∼  18 (14–22)  % of atmospheric CCl4 is lost to the ocean. Although CCl4 hydrolyzes in seawater, published hydrolysis rates for this gas are too slow to support such large undersaturations, given our current understanding of air–sea gas exchange rates. The even larger undersaturations in intermediate depth waters associated with reduced oxygen levels, observed in this study and by other investigators, strongly suggest that CCl4 is ubiquitously consumed at mid-depth, presumably by microbiota. Although this subsurface sink creates a gradient that drives a downward flux of CCl4, the gradient alone is not sufficient to explain the observed surface undersaturations. Since known chemical losses are likewise insufficient to sustain the observed undersaturations, this suggests a possible biological sink for CCl4 in surface or near-surface waters of the ocean. The total atmospheric lifetime for CCl4, based on these results and the most recent studies of soil uptake and loss in the stratosphere is now 32 (26–43) yr.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-16-10899-2016
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
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  • 4
    Online Resource
    Online Resource
    Composite global emissions of reactive chlorine from anthropogenic and natural sources: Reactive Chlorine Emissions Inventory
    American Geophysical Union (AGU) ; 1999
    In:  Journal of Geophysical Research: Atmospheres Vol. 104, No. D7 ( 1999-04-20), p. 8429-8440
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 104, No. D7 ( 1999-04-20), p. 8429-8440
    Abstract: Emission inventories for major reactive tropospheric Cl species (particulate Cl, HCl, ClNO 2 , CH 3 Cl, CHCl 3 , CH 3 CCl 3 , C 2 Cl 4 , C 2 HCl 3 , CH 2 Cl 2 , and CHClF 2 ) were integrated across source types (terrestrial biogenic and oceanic emissions, sea‐salt production and dechlorination, biomass burning, industrial emissions, fossil‐fuel combustion, and incineration). Composite emissions were compared with known sinks to assess budget closure; relative contributions of natural and anthropogenic sources were differentiated. Model calculations suggest that conventional acid‐displacement reactions involving S (IV) + O 3 , (IV) + O 3 H 2 O 2 , and H 2 SO 4 and HNO 3 scavenging account for minor fractions of sea‐salt dechlorination globally. Other important chemical pathways involving sea‐salt aerosol apparently produce most volatile chlorine in the troposphere. The combined emissions of CH 3 Cl from known sources account for about half of the modeled sink, suggesting fluxes from known sources were underestimated, the OH sink was overestimated, or significant unidentified sources exist. Anthropogenic activities (primarily biomass burning) contribute about half the net CH 3 Cl emitted from known sources. Anthropogenic emissions account for only about 10% of the modeled CHCl 3 sink. Although poorly constrained, significant fractions of tropospheric CH 2 Cl 2 (25%), C 2 HCl 3 (10%), and C 2 Cl 4 (5%) are emitted from the surface ocean; the combined contributions of C 2 Cl 4 and C 2 HCl 3 from all natural sources may be substantially higher than the estimated oceanic flux.
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/1998JD100084
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 1999
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