Oceanic emissions of nitrous oxide (N2O) account for roughly one‐third of all natural sources to the atmosphere. Hot‐spots of N2O outgassing occur over oxygen minimum zones (OMZs), where the presence of steep oxygen gradients surrounding anoxic waters leads to enhanced N2O production from both nitrification and denitrification. However, the relative contributions from these pathways to N2O production and outgassing in these regions remains poorly constrained, in part due to shared intermediary nitrogen tracers, and the tight coupling of denitrification sources and sinks. To shed light on this problem, we embed a new, mechanistic model of the OMZ nitrogen cycle within a three‐dimensional eddy‐resolving physical‐biogeochemical model of the Eastern Tropical South Pacific (ETSP), tracking contributions from remote advection, atmospheric exchange, and local nitrification and denitrification. The model indicates that net N2O production from denitrification is approximately one order of magnitude greater than nitrification within the ETSP OMZ. However, only ∼32% of denitrification‐derived N2O production ultimately outgasses to the atmosphere in this region (contributing ∼36% of the air‐sea N2O flux on an annual basis), while the remaining is exported out of the domain. Instead, remotely produced N2O advected into the OMZ region accounts for roughly half (∼57%) of the total N2O outgassing, with smaller contributions from nitrification (∼7%). Our results suggests that, together with enhanced production by denitrification, upwelling of remotely derived N2O contributes the most to N2O outgassing over the ETSP OMZ.
The ocean is estimated to contribute up to ~20% of global fluxes of atmospheric nitrous oxide (N2O), an important greenhouse gas and ozone depletion agent. Marine oxygen minimum zones contribute disproportionately to this flux. To further understand the partition of nitrification and denitrification and their environmental controls on marine N2O fluxes, we report new relationships between oxygen concentration and rates of N2O production from nitrification and denitrification directly measured with15N tracers in the Eastern Tropical Pacific. Highest N2O production rates occurred near the oxic‐anoxic interface, where there is strong potential for N2O efflux to the atmosphere. The dominant N2O source in oxygen minimum zones was nitrate reduction, the rates of which were 1 to 2 orders of magnitude higher than those of ammonium oxidation. The presence of oxygen significantly inhibited the production of N2O from both nitrification and denitrification. These experimental data provide new constraints to a multicomponent global ocean biogeochemical model, which yielded annual oceanic N2O efflux of 1.7–4.4 Tg‐N (median 2.8 Tg‐N, 1 Tg = 1012 g), with denitrification contributing 20% to the oceanic flux. Thus, denitrification should be viewed as a net N2O production pathway in the marine environment.
more » « less- Award ID(s):
- 1657663
- PAR ID:
- 10459975
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Global Biogeochemical Cycles
- Volume:
- 32
- Issue:
- 12
- ISSN:
- 0886-6236
- Page Range / eLocation ID:
- p. 1790-1802
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
Abstract -
Abstract Marine oxygen deficient zones are dynamic areas of microbial nitrogen cycling. Nitrification, the microbial oxidation of ammonia to nitrate, plays multiple roles in the biogeochemistry of these regions, including production of the greenhouse gas nitrous oxide (N2O). We present here the results of two oceanographic cruises investigating nitrification, nitrifying microorganisms, and N2O production and distribution from the offshore waters of the Eastern Tropical South Pacific. On each cruise, high‐resolution measurements of ammonium ([NH4+]), nitrite ([NO2−]), and N2O were combined with15N tracer‐based determination of ammonia oxidation, nitrite oxidation, nitrate reduction, and N2O production rates. Depth‐integrated inventories of NH4+and NO2−were positively correlated with one another and with depth‐integrated primary production. Depth‐integrated ammonia oxidation rates were correlated with sinking particulate organic nitrogen flux but not with primary production; ammonia oxidation rates were undetectable in trap‐collected sinking particulate material. Nitrite oxidation rates exceeded ammonia oxidation rates at most mesopelagic depths. We found positive correlations between archaeal
amoA genes and ammonia oxidation rates and betweenNitrospina ‐like 16S rRNA genes and nitrite oxidation rates. N2O concentrations in the upper oxycline reached values of >140 nM, even at the western extent of the cruise track, supporting air‐sea fluxes of up to 1.71 μmol m−2 day−1. Our results suggest that a source of NO2−other than ammonia oxidation may fuel high rates of nitrite oxidation in the offshore Eastern Tropical South Pacific and that air‐sea fluxes of N2O from this region may be higher than previously estimated. -
Abstract Nitrous oxide (N2O) is a powerful greenhouse gas, and oceanic sources account for up to one third of the total natural flux to the atmosphere. In oxygen‐deficient zones (ODZs) like the Eastern Tropical North Pacific (ETNP), N2O can be produced and consumed by several biological processes. In this study, the concentration and isotopocule ratios of N2O from a 2016 cruise in the ETNP were analyzed to examine sources of and controls on N2O cycling across this region. Along the north‐south transect, three distinct biogeochemical regimes were identified: background, core‐ODZ, and high‐N2O stations. Background stations were characterized by smaller variations in N2O concentration and isotopic profiles relative to the other regimes. Core‐ODZ stations were characterized by co‐occurring N2O production and consumption at anoxic depths, indicated by high δ18O‐N2O (>90‰) and low δ15N2Oβ(<−10‰) values, and confirmed by a time‐dependent model, which indicated that N2O production via denitrification was significant and may occur with a nonzero site preference. High‐N2O stations, located at the periphery of a mesoscale eddy, were defined by N2O reaching 126.07 ± 12.6 nM and low oxygen concentrations expanding into near‐surface isopycnals. At these stations, model results indicated significant N2O production from ammonia‐oxidizing archaea and denitrification from nitrate at the N2O maximum within the oxycline, while bacterial nitrification and denitrification from nitrite were insignificant. This study also represents the first in the ETNP to link N2O production mechanisms to a mesoscale eddy through isotopocule measurements, suggesting the importance of eddies to spatiotemporal variability in N2O cycling and emissions from this region.
-
Abstract Nitrous oxide (N2O), a potent greenhouse gas, is produced disproportionately in marine oxygen deficient zones (ODZs). To quantify spatiotemporal variation in N2O cycling in an ODZ, we analyzed N2O concentration and isotopologues along a transect through the eastern tropical North Pacific (ETNP). At several stations along this transect, N2O concentrations reached a near surface maximum that exceeded prior measurements in this region, of up to 226.1 ± 20.5 nM at the coast. Above the
σ θ = 25.0 kg/m3isopycnal, Keeling plot analysis revealed two sources to the near‐surface N2O maximum, with different δ15N2Oαand δ15N2Oβvalues, but each with a site preference (SP) of 6‰–8‰. Given expected SPs for nitrification and denitrification, each of these sources could be comprised of 17%–26% nitrification (bacterial or archeal), and 74%–83% denitrification (or nitrifier‐denitrification). Below theσ θ = 25.0 kg/m3isopycnal, box model analysis indicated that the observed 46‰–50‰ SPs in the anoxic core of the ODZ cannot be reproduced in a steady state context without an SP for N2O production by denitrification, and may indicate instead a transient net consumption of N2O. Furthermore, time‐dependent model results indicated that while δ15N2Oαand δ18O‐N2O reflect both N2O production and consumption in the anoxic core of the ODZ, δ15N2Oβpredominantly reflects N2O sources. Finally, we infer that the high (N2O) observed at some stations derive from a set of conditions supporting high rates of N2O production that have not been previously encountered in this region. -
Microorganisms in marine oxygen minimum zones (OMZs) drive globally impactful biogeochemical processes. One such process is multistep denitrification (NO3–→NO2–→NO→N2O→N2), which dominates OMZ bioavailable nitrogen (N) loss and nitrous oxide (N2O) production. Denitrification-derived N loss is typically measured and modeled as a single step, but observations reveal that most denitrifiers in OMZs contain subsets (“modules”) of the complete pathway. Here, we identify the ecological mechanisms sustaining diverse denitrifiers, explain the prevalence of certain modules, and examine the implications for N loss. We describe microbial functional types carrying out diverse denitrification modules by their underlying redox chemistry, constraining their traits with thermodynamics and pathway length penalties, in an idealized OMZ ecosystem model. Biomass yields of single-step modules increase along the denitrification pathway when organic matter (OM) limits growth, which explains the viability of populations respiring NO2–and N2O in a NO3–-filled ocean. Results predict denitrifier community succession along environmental gradients: Pathway length increases as the limiting substrate shifts from OM to N, suggesting a niche for the short NO3–→NO2–module in free-living, OM-limited communities, and for the complete pathway in organic particle-associated communities, consistent with observations. The model captures and mechanistically explains the observed dominance and higher oxygen tolerance of the NO3–→NO2–module. Results also capture observations that NO3–is the dominant source of N2O. Our framework advances the mechanistic understanding of the relationship between microbial ecology and N loss in the ocean and can be extended to other processes and environments.