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Title: Nitrogen partitioning between silicate phases and aqueous fluid depends on concentration
The distribution of nitrogen in geologic systems is modulated by its partitioning between silicate (mineral and melt) and fluid phases. Under geologically applicable oxygen fugacity, pressure, and temperatures, nitrogen can be multiply-speciated, with N2 coexisting with reduced nitride (N􀀀 3) species. Non-polar, neutral species, including N2, tend to concentrate in fluids, while charged nitride species have a greater propensity to concentrate in silicate phases. The stoichiometry of converting N2 to single N atom nitride species implies that nitrogen speciation may depend on its concentration, and this leads to the hypothesis that the partitioning of nitrogen between silicate and fluid phases also depends on concentration, potentially biasing prior experimental work in doped systems and influencing the behavior of nitrogen in geologic systems. To test this hypothesis, we have completed a series high pressure (~1.75 GPa, 800 ◦C) experiments that react minerals, melts, and fluids with variable nitrogen concentrations (3.1–17.1 wt% N). Our results imply order-of-magnitude-scale increases in mineral/melt and melt/fluid partitioning as nitrogen concentrations decrease within natural ranges. For example, decreasing the N concentration from 2500 to 2 ppm increases predicted DN melt/fluid values by over an order of magnitude at constant PT conditions. This means that loss of nitrogen from a degassing magma or dehydrating slab is a self-limiting process that becomes increasingly inefficient as nitrogen concentration falls. Despite this, nitrogen remains highly concentrated in the atmosphere, which receives N from fluids exsolved from slabs and magmas. To maintain a nitrogen-rich atmosphere we therefore suggest that warm and oxidizing conditions have prevailed over subduction zones because warm slabs dehydrate under lower pressures where nitrogen is more easily partitioned into fluids, and oxidizing conditions also promote nitrogen partitioning into fluids. Concentration-dependent partitioning of nitrogen will also serve to moderate any initial variations of N/K in slab materials upon dehydration, and this may help to explain the relatively uniform N/K ratio of MORB mantle. We supplement our nitrogen concentration experiments with a temperature series (1.5–2 GPa, 750–950 ◦C). Our temperature series data reveal that at high temperature nitrogen favors melts over fluids, while temperature has no resolvable effect of biotite-fluid partitioning.  more » « less
Award ID(s):
1725315
PAR ID:
10483927
Author(s) / Creator(s):
;
Publisher / Repository:
Elsevier
Date Published:
Journal Name:
Geochimica et Cosmochimica Acta
Volume:
354
Issue:
C
ISSN:
0016-7037
Page Range / eLocation ID:
1 to 12
Subject(s) / Keyword(s):
nitrogen partitioning volatiles
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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