Nitrogen distribution between aqueous fluids and silicate melts

Abstract

The partitioning of nitrogen between hydrous fluids and haplogranitic, basaltic, or albitic melts was studied at 1–15 kbar, 800–1200 °C, and oxygen fugacities (fO2) ranging from the Fe–FeO buffer to 3log units above the Ni–NiO buffer. The nitrogen contents in quenched glasses were analyzed either by electron microprobe or by secondary ion mass spectrometry (SIMS), whereas the nitrogen contents in fluids were determined by mass balance. The results show that the nitrogen content in silicate melt increases with increasing nitrogen content in the coexisting fluid at given temperature, pressure, and fO2. Raman spectra of the silicate glasses suggest that nitrogen species change from molecular N2 in oxidized silicate melt to molecular ammonia (NH3) or the ammonium ion (NH4+) in reduced silicate melt, and the normalized Raman band intensities of the nitrogen species linearly correlate with the measured nitrogen content in silicate melt. Elevated nitrogen contents in silicate melts are observed at reduced conditions and are attributed to the dissolution of NH3/NH4+. Measured fluid/melt partition coefficients for nitrogen (DNfluid/melt) range from 60 for reduced haplogranitic melts to about 10 000 for oxidized basaltic melts, with fO2 and to a lesser extent melt composition being the most important parameters controlling the partitioning of nitrogen. Pressure appears to have only a minor effect on DNfluid/melt in the range of conditions studied. Our data imply that degassing of nitrogen from both mid-ocean ridge basalts and arc magmas is very efficient, and predicted nitrogen abundances in volcanic gases match well with observations. Our data also confirm that nitrogen degassing at present magma production rates is insufficient to accumulate the atmosphere. Most of the nitrogen in the atmosphere must have degassed very early in Earth's history and degassing was probably enhanced by the oxidation of the mantle.