The Fe–C–O–H–N system at 6.3–7.8 GPa and 1200–1400 °C: implications for deep carbon and nitrogen cycles

Contributions to Mineralogy and Petrology(2018)

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摘要
Interactions in a Fe–C–O–H–N system that controls the mobility of siderophile nitrogen and carbon in the Fe 0 -saturated upper mantle are investigated in experiments at 6.3–7.8 GPa and 1200–1400 °C. The results show that the γ-Fe and metal melt phases equilibrated with the fluid in a system unsaturated with carbon and nitrogen are stable at 1300 °C. The interactions of Fe 3 C with an N-rich fluid in a graphite-saturated system produce the ε-Fe 3 N phase (space group P 6 3 / mmc or P 6 3 22) at subsolidus conditions of 1200–1300 °C, while N-rich melts form at 1400 °C. At IW- and MMO-buffered hydrogen fugacity ( f H 2 ), fluids vary from NH 3 - to H 2 O-rich compositions (NH 3 /N 2 > 1 in all cases) with relatively high contents of alkanes. The fluid derived from N-poor samples contains less H 2 O and more carbon which mainly reside in oxygenated hydrocarbons, i.e., alcohols and esters at MMO-buffered f H 2 and carboxylic acids at unbuffered f H 2 conditions. In unbuffered conditions, N 2 is the principal nitrogen host (NH 3 /N 2 ≤ 0.1) in the fluid equilibrated with the metal phase. Relatively C- and N-rich fluids in equilibrium with the metal phase (γ-Fe, melt, or Fe 3 N) are stable at the upper mantle pressures and temperatures. According to our estimates, the metal/fluid partition coefficient of nitrogen is higher than that of carbon. Thus, nitrogen has a greater affinity for iron than carbon. The general inference is that reduced fluids can successfully transport volatiles from the metal-saturated mantle to metal-free shallow mantle domains. However, nitrogen has a higher affinity for iron and selectively accumulates in the metal phase, while highly mobile carbon resides in the fluid phase. This may be a controlling mechanism of the deep carbon and nitrogen cycles.
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关键词
Mantle,Metal,Fluid,Carbon,Nitrogen,Hydrocarbons,Gas chromatography–mass spectrometry
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