Abstract

Evolution of nitrogen (N), a life-essential volatile element, in highly reduced magmatic systems is a key for the origin of N on rocky planets formed via accretion of reduced chondritic parent body materials, planetesimals, and embryos that underwent partial or complete differentiation. However, the storage capacity of N in phases relevant for reduced silicate systems undergoing thermal processing is poorly known. To investigate the stability of N-bearing phases in partially molten silicate-rich systems as well as solubility of nitrogen in silicate melts and minerals, we performed laboratory experiments on a 80:20 synthetic basalt-Si3N4 mixture at 1.5–3.0 GPa and 1300–1600 °C in graphite capsules, yielding oxygen fugacity ranging from ∼ IW– 3.0 to ∼ IW – 4.0. All experiments produced silicate melt + nierite + Fe-rich alloy melt + N-rich vapor ± sinoite ± cpx. Sinoite was restricted to above while cpx was restricted below 1400–1500 °C. Nitrogen solubility and Nitrogen Concentration at Silicon-Nitride Saturation (NCNS) in silicate melts increase with increasing pressure and temperature and range between 3.6 and 9.5 wt%. Using our high pressure N solubility data and similar data at ambient and lower pressures, we derived a new N solubility model in silicate melts. Solubility of nitrogen in cpx was between 1.51 and 2.05 wt% and resulted in cpx/silicate melt partition coefficients for nitrogen, DNcpx/silicatemelt of ∼ 0.4 to ∼ 0.2. These DNcpx/silicatemelt are distinctly higher than those previously estimated at more oxidizing conditions, suggesting N maybe much less incompatible during thermal processing of rocky reservoirs at highly reducing conditions. Partition coefficient of N between Fe-rich alloy melt and cpx, DNFe-richalloymelt/cpx was found to be between 1.6 and 2.1. The application of our N solubility data and model suggests that mobilization of N from the deeper, partially molten reservoirs to shallower reservoirs is possible in reduced planetesimals and internally differentiated meteorite parent bodies – leading to net loss of N via melt degassing or reprecipitation of N-bearing solid phases, depending on whether the surficial shell is oxidized or reduced, respectively. Similarly, comparison of the first measured DNcpx/silicatemelt values from our highly reducing experiments with those estimated at more oxidizing conditions suggest that N would be much less incompatible during internal and external magma ocean processing of rocky bodies under highly reducing conditions. Therefore, enrichment of N in the atmospheres of Earth and Venus is likely a result of more oxidizing penultimate phase of accretion, which would lead to N being more readily partitioned to residual liquid, which would also more readily degas at oxidizing conditions.

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