- Open Access
Nitrogen in the Earth: abundance and transport
© The Author(s). 2019
- Received: 29 November 2018
- Accepted: 30 April 2019
- Published: 20 May 2019
The terrestrial nitrogen budget, distribution, and evolution are governed by biological and geological recycling. The biological cycle provides the nitrogen input for the geological cycle, which, in turn, feeds some of the nitrogen into the Earth’s interior. A portion of the nitrogen also is released back to the oceans and the atmosphere via N2 degassing. Nitrogen in silicate minerals (clay minerals, mica, feldspar, garnet, wadsleyite, and bridgmanite) exists predominantly as NH4+. Nitrogen also is found in graphite and diamond where it occurs in elemental form. Nitrides are stable under extremely reducing conditions such as those that existed during early planetary formation processes and may still persist in the lower mantle. From experimentally determined nitrogen solubility in such materials, the silicate Earth is nitrogen undersaturated. The situation for the core is more uncertain, but reasonable Fe metal/silicate nitrogen partition coefficients (> 10) would yield nitrogen contents sufficient to account for the apparent nitrogen deficiency in the silicate Earth compared with other volatiles. Transport of nitrogen takes place in silicate melt (magma), water-rich fluids, and as a minor component in silicate minerals. In melts, the N solubility is greater for reduced nitrogen, whereas the opposite appears to be the case for N solubility in fluids. Reduced nitrogen species (NH3, NH2−, and NH2+) dominate in most environments of the modern Earth’s interior except the upper ~ 100 km of subduction zones where N2 is the most important species. Nitrogen in magmatic liquids in the early Earth probably was dominated by NH3 and NH2−, whereas in the modern Earth, the less reduced, NH2+ functional group is more common. N2 is common in magmatic liquids in subduction zones. Given the much lower solubility of N2 in magmatic liquids compared with other nitrogen species, nitrogen dissolved as N2 in subduction zone magmas is expected to be recycled and returned to the oceans and the atmosphere, whereas nitrogen in reduced form(s) likely would be transported to greater depths. This solubility difference, controlled primarily by variations in redox conditions, may be a factor resulting in increased nitrogen in the Earth’s mantle and decreasing abundance in its oceans and atmosphere during the Earth’s evolution. Such an abundance evolution has resulted in the decoupling of nitrogen distribution in the solid Earth and the hydrosphere and atmosphere.
Nitrogen has been used as a tracer with which to connect surface reservoirs (atmosphere and the oceans) to the solid Earth. Adequate characterization of the nitrogen exchange within and between reservoirs relies, however, on knowledge of bulk nitrogen contents, nitrogen distribution among various reservoirs, and on nitrogen transport mechanisms within and between the reservoirs as a function of temperature, pressure, redox conditions, and composition of condensed and volatile components.
The bulk terrestrial nitrogen abundance is not well established in part because it depends on the precursor material of the Earth, in part because the nitrogen content of the Earth’s core is not well constrained, and in part because the nitrogen concentration in the various nitrogen reservoirs may vary over geologic time (Bebout et al. 2013; Johnson and Goldblatt 2015; Dalou et al. 2017). It has been suggested, for example, that the terrestrial abundance of nitrogen resembles that of chondrites or combinations of different chondritic materials (Fogel and Steele 2013; Dauphas 2017). With a single precursor component such as, for example, chondrite, its nitrogen content depends on processing of this material prior to formation of the Earth. Another possibility is that the Earth was formed with contributions from different embryos with different elemental and isotopic compositions some of which might also be parents of chondritic components (Dauphas 2017). Here, the embryos include major contributions from both carbonaceous and enstatite chondrite as well as other components including ordinary chondrite and a late veneer. The contributions occurred at different stages during Earth formation. Again, however, the nitrogen contents of the individual contributors are uncertain factors.
Nitrogen distribution among reservoirs reflects recycling mechanisms. A major contribution to nitrogen recycling is subduction zones (Goldblatt et al. 2009; Palya et al. 2011) where sediments comprising N-rich organic materials descend into the mantle. Redox conditions play a critical role in the descent process as oxygen fugacity governs the speciation of the nitrogen (Mysen and Fogel 2010). Redox conditions affect the initial recycling step, which is the breakdown of sedimentary organic materials. Redox conditions also govern subsequent nitrogen solubility in minerals, melts, and fluids because the solubility varies with nitrogen speciation. Some of the nitrogen in subducting materials is returned to the surface through devolatilization and nitrogen release. This occurs whenever conditions favor oxidized nitrogen (N2), which is not very soluble in magmatic liquids. However, nitrogen is not always oxidized. Under mildly reducing conditions, similar to those defined by the magnetite-wüstite (MW) to quartz-fayalite-magnetite (QFM) oxygen buffers, nitrogen can exist as various N–H complexes (Mysen et al. 2008), which can be significantly soluble in subduction zone silicate minerals (Honma and Itahara 1981; Watenphul et al. 2010) and silicate melt (magmatic liquids) (Mysen et al. 2008). Under such circumstances, nitrogen could be transported into the deep mantle. Therefore, there could be greater nitrogen input than output in the Earth, which accords with current observations (Sano et al. 2001; Mitchell et al. 2010; Busigny et al. 2011). Even when nitrogen output near mid-ocean ridges is taken into account, a large difference between nitrogen influx and outflux remains (Busigny et al. 2011). It follows that the nitrogen content of the Earth’s interior increased during Earth history while the nitrogen abundance of the oceans and atmosphere may have decreased. It also follows that with the redox-dependent nitrogen solubility in condensed and volatile components, nitrogen abundance (and isotopic compositions?) in the atmosphere, oceans, and crust is decoupled from nitrogen in the deep interior (mantle and core).
The factors that govern the nitrogen abundance and distribution in the Earth’s interior in time and space will be discussed in this review. To this end, observations of nitrogen abundance will be examined together with results from laboratory experiments relevant to nitrogen solubility and solution mechanisms in condensed (crystalline and molten materials) and volatile (C-O-H-N) fluids will be discussed. There will be particular emphasis on the consequences of redox-controlled nitrogen speciation as this may help understand the decoupling of terrestrial core and mantle versus crustal nitrogen reservoirs.
The condensed Earth includes its crust, mantle, and core. Additional reservoirs are the oceans and the atmosphere. To address how nitrogen is distributed, current knowledge of nitrogen recycling and speciation within reservoirs will be summarized briefly first. This will be followed by a discussion of experimental data on nitrogen solubility and solution mechanisms necessary to characterize nitrogen transport behavior in molten silicate (magma).
In terms of total mass, the main reservoir is the mantle (Table 1). However, the summary in Table 1 does not include the Earth’s core for which nitrogen estimates vary significantly (Dalou et al. 2017; Roskosz et al. 2013). Major uncertainties affecting assessment of the nitrogen abundance in the core are silicate/melt partition coefficients, the extent of pressure-dependent nitrogen partitioning between metal and silicate, and redox conditions during core separation. These variables are somewhat interdependent and are central factors governing nitrogen cycles in the Earth.
The agents for materials transfer within and between are silicate melts (magma) and sometimes COHN volatiles. Nitrogen and other volatiles would have been dissolved in the high-pressure silicate magma ocean of the early Earth in which the solubility of the volatile species likely greatly exceeded their abundance. This is because the solubility of volatiles in silicate melts, including nitrogen species, in the C-O-H-N system is on the order of several thousand ppm even at pressures corresponding to depths of a few kilometers. The solubility increases with increasing pressure (see Mysen and Richet 2019; Chapters 14–18, for detailed review of this information). A few thousand ppm is orders of magnitude greater than the content of these volatiles in the silicate Earth (Marty 2012; Halliday 2013; Armstrong et al. 2015).
Nitrogen in the crust
Much of the nitrogen in crustal igneous rocks may be returned to the Earth’s interior in subduction zones. The nitrogen concentration in the igneous rocks varies widely. For example, granite formed by partial melting of biomass precursors typically is ammonium-rich with up to more than 100 ppm N held in mica and feldspar minerals, whereas granite formed by fractional crystallization or melting of mafic rocks is nitrogen poor with only several ppm N (Hall 1999). Other igneous rocks such as gabbro and tonalite contain on average 10 ppm or less N (Johnson and Goldblatt 2015).
The main influx of nitrogen to the Earth’s interior is from sediments in subduction zones (Busigny et al. 2011). Some nitrogen from the descending sediment column is released as N2 and returned to the oceans and the atmosphere. The proportion of nitrogen remaining in sedimentary and metamorphic rocks decreases with increasing depth (e.g., Plessen et al. 2010).
The extent to which release of N2 occurs instead of transport as NH4+ to greater depth in subduction zones depends on the thermal gradient and oxygen fugacity. Steep thermal gradients lead to N2 formation. Cold subduction zones lead to greater nitrogen loss (Bebout et al. 1999; Halama et al. 2014). Under oxidizing conditions such as those near the QFM-NNO range, which is typical for subduction zone magmatism (Carmichael and Ghiorso 1990), most of the nitrogen is released as N2. Under more reducing conditions, the nitrogen remains as NH4+ and descends into the deep mantle. Ammonia and derivative functional groups in this latter environment are retained in clay minerals, micas (phlogopite and phengite), and feldspars (Hall 1999; Elkins et al. 2006; Watenphul et al. 2009; Mitchell et al. 2010; Plessen et al. 2010; Palya et al. 2011; Yoshioka et al. 2018).
Nitrogen in the mantle
Nitrogen solubility as high as near 25 ppm in forsterite, pyroxene, and garnet have been reported in an experimental study in the 1.5–3.0 GPa range with the oxygen fugacity controlled at those of the NNO and IW buffer (Li et al. 2013). From least squares fitting to all the data obtained, Li et al. (2013) derived the following expressions for solubility;
where ∆NNO is the oxygen fugacity difference from that of the nickel/nickel oxide oxygen buffer [∆NNO = log fO2-logfO2(NNO)]. Partition coefficients among upper mantle minerals are summarized in Table 2.
Nitrogen partition coefficients
0.43 ± 0.11
0.38 ± 0.08
0.11 ± 0.04
0.85 ± 0.15
0.32 ± 0.16
Nitrogen partition coefficients among lower mantle silicate phases (data from Yoshioka et al. 2018)
5.1 ± 2.1
2.0 ± 1.2
4.2 ± 0.3
Nitrogen in the Earth’s core
Evolution of the terrestrial nitrogen reservoirs following their original composition and volume in the proto-Earth was accomplished by mass transfer with magma (silicate melt) and fluids in the C-O-H-N systems. Characterization of these processes rely on understanding nitrogen solubility, solution mechanisms, and nitrogen partitioning between coexisting minerals, melts, and fluids.
Solubility and solution mechanisms
The nitrogen solubility and speciation in magmatic melts and aqueous fluids are sensitive functions of redox conditions, temperature, pressure, silicate, and fluid composition. These variables will, therefore, affect the distribution of nitrogen in the Earth. For example, redox conditions are important because N2 is incompatible in silicate minerals, whereas reduced nitrogen is compatible (Bebout et al. 2013). In this latter case, during melting and fluid release in the mantle, some nitrogen will, therefore, remain in crystalline mantle. This feature together with oxygen fugacity variations are key factors controlling temporal changes in mantle (and core?) nitrogen content.
Oxidizing conditions are defined as an fO2 near that of the QFM oxygen buffer and above. Nitrogen in fluids and melts exists principally as molecular N2 under oxidizing conditions (Mysen et al. 2014; Li et al. 2015).
The N2 solubility commonly follows Henry’s Law with a Henry’s Law constant near 5•10−9 mol g−1 bar−1 (Javoy and Pineau 1991; Libourel et al. 2003; Roskosz et al. 2006). Some variations in the Henry’s Law constant may be ascribed to compositional dependence of the N2 solubility similar to the behavior of noble gases in silicate melts. These variables include extent of silicate polymerization (which is mostly linked to Si + Al contents), aluminum substitution of silicon, and the electronic properties and proportions of network-modifying cations (alkali metals and alkaline earths).
The fluid/melt partition coefficient for reduced nitrogen is temperature-dependent just as it is N2 (Fig. 14). The temperature-dependence results in a ∆H-value of − 5.9 ± 0.9 kJ/mol under the assumption of no pressure-dependence in the 0.6–1.4 GPa pressure range of those experiments (Mysen 2018a). This ∆H-value is significantly less than in the case of molecular N2 with its enthalpy value at − 20 ± 4 kJ/mol (Mysen 2018b) suggesting, perhaps, greater structural similarity between reduced nitrogen species in fluids and melts than is the case for molecular N2.
The oxygen fugacity is the most important factor affecting nitrogen abundance and distribution in the Earth because nitrogen speciation depends on fO2 in the oxygen fugacity range of the Earth’s interior. The different nitrogen species, in turn, exhibit significantly different solubility behavior and partitioning behavior among minerals, melts, and fluids. These features need attention when the role of nitrogen in Earth formation and evolution is under consideration.
In this expression, the NH2+ and H+ are linked to nonbridging oxygen in the silicate tetrahedra and serve, therefore, as network-modifiers.
The structural role of NH2− groups in Eq. (8) differs, therefore, from the behavior of NH2+ groups in expression (9). In Eq. (8), an Si-O-Si bridge is cleaved and the oxygen formerly forming a bridge is replaced by an OH− group and an NH2− group. In Eq. (9), which describes moderately reducing conditions, replacement of a network-modifying cation with NH2+ as a modifier has no effect on the overall degree of polymerization of the silicate.
Expressions (8)–(10) illustrate mechanisms of nitrogen solubility and solution mechanisms in most magmatic environments in planetary interiors, be they modern or primordial. The nitrogen solubility in magma depends significantly on which of those solution mechanisms dominate.
The effect of solution mechanisms on nitrogen solubility, governed primarily by fo2, is well illustrated by the behavior of nitrogen in subduction zones in which the oxygen fugacity ranges from oxidizing to quite reducing. Subduction zones are major venues for nitrogen flux into and out of the Earth (Busigny et al. 2011) with oxygen fugacity during nitrogen release a major factor determining the fate of nitrogen (Li and Keppler 2014; Mallik et al. 2018). Under oxidizing conditions such as those defined by the QFM buffer and above [Eq. (10)], which is common in the upper 100 km of subduction zones (Carmichael and Ghiorso 1990), N2 is a principal nitrogen species. Nitrogen dissolved as N2 in subduction zone magmas likely is recycled and returned to the oceans and the atmosphere because molecular N2 is incompatible in silicate melts and minerals and is released, therefore, to a fluid phase, which ascends to the surface. Under more reducing conditions such as those of the MW buffer and below [Eq. (8) and (9)], nitrogen exists in reduced form where it dissolves in minerals as described above (mica, feldspar, garnet, pyroxene and shallow depth, and wadsleyite and bridgmanite at greater depth). This nitrogen descends into the lithosphere and below likely will not be released back into the oceans and the atmosphere. The different solubility behavior of oxidized (N2) and reduced (NH3, NH2+, NH2−) nitrogen in mantle melts and minerals in the Earth’s interior would lead to an increase in mantle nitrogen through Earth history and a decrease in nitrogen abundance in its oceans and atmosphere. Because the Earth’s interior is undersaturated with respect to nitrogen (e.g., Yoshioka et al. 2018), this nitrogen is not returned to the Earth’s surface even during melting or fluid release because of the compatible nature of reduced nitrogen in silicate minerals at high temperature and pressure (Busigny et al. 2011). This is why nitrogen at or near the Earth’s surface cannot be used to characterize the behavior of nitrogen and its isotopes in the deep interior of the Earth.
Instrument, electronics, and library support was provided by Geophysical Laboratory technical staff. The manuscript also was reviewed by Dionysis Foustoukos and two external reviewers.
The research in this review was supported by endowment funds from the Carnegie Institution of Washington, and grants EAR-1212754 and EAR-1250449 from the National Science Foundation.
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