N2O production in the eastern South Atlantic: Analysis of N2O stable isotopic and concentration data

被引:42
作者
Frame, Caitlin H. [1 ]
Deal, Eric [2 ]
Nevison, Cynthia D. [3 ]
Casciotti, Karen L. [4 ]
机构
[1] Univ Basel, Dept Environm Sci, Basel, Switzerland
[2] Univ Grenoble 1, Inst Sci Terre, Grenoble, France
[3] Univ Colorado, Inst Arctic & Alpine Res, Boulder, CO 80309 USA
[4] Stanford Univ, Dept Environm Earth Syst Sci, Palo Alto, CA 94304 USA
基金
美国国家科学基金会;
关键词
nitrous oxide (N2O); isotopomer; nitrification; denitrification; nitrifier denitrification; coastal upwelling; ATMOSPHERIC NITROUS-OXIDE; TROPICAL NORTH PACIFIC; OXYGEN-MINIMUM; CARBON-DIOXIDE; NITRIC-OXIDE; EXPERIMENTAL DROUGHT; NITRIFICATION RATES; GLOBAL DISTRIBUTION; SOIL EMISSIONS; DENITRIFICATION;
D O I
10.1002/2013GB004790
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The stable isotopic composition of dissolved nitrous oxide (N2O) is a tracer for the production, transport, and consumption of this greenhouse gas in the ocean. Here we present dissolved N2O concentration and isotope data from the South Atlantic Ocean, spanning from the western side of the mid-Atlantic Ridge to the upwelling zone off the southern African coast. In the eastern South Atlantic, shallow N2O production by nitrifier denitrification contributed a flux of isotopically depleted N2O to the atmosphere. Along the African coast, N2O fluxes to the atmosphere of up to 46 mu mol/m(2)/d were calculated using satellite-derived QuikSCAT wind speed data, while fluxes at the offshore stations averaged 0.04 mu mol/m(2)/d. Comparison of the isotopic composition of the deeper N2O in the South Atlantic (800m to 1000m) to measurements made in other regions suggests that water advected from one or more of the major oxygen deficient zones contributed N2O to the mesopelagic South Atlantic via the Southern Ocean. This deeper N2O was isotopically and isotopomerically enriched (N-15(bulk) - N2O = 8.70.1, O-18 - N2O = 46.50.2, and Site Preference = 18.7 +/- 0.6 parts per thousand) relative to the shallow N2O source, indicating that N2O consumption by denitrification influenced its isotopic composition. The N2O concentration maximum was observed between 200m and 400m and reached 49 nM near the Angolan coast. The depths of the N2O concentration maximum coincided with those of sedimentary particle resuspension along the coast. The isotopic composition of this N2O (N-15(bulk) - N2O = 5.8 +/- 0.1 parts per thousand, O-18 - N2O = 39.7 +/- 0.1 parts per thousand, and Site Preference = 9.8 +/- 1.0 parts per thousand) was consistent with production by diffusion-limited nitrate (NO3-) reduction to nitrite (NO2-), followed by NO2- reduction to N2O by denitrification and/or nitrifier denitrification, with additional N2O production by NH2OH decomposition during NH3 oxidation. The sediment surface, benthic boundary layer, or particles resuspended from the sediments are likely to have provided the physical and chemical conditions necessary to produce this N2O.
引用
收藏
页码:1262 / 1278
页数:17
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