skip to main content


Title: Melting of the Fe‐C‐H System and Earth's Deep Carbon‐Hydrogen Cycle
Abstract

The occurrences and cycling of slab‐originated carbon and hydrogen are considered to be controlled by their reactions with metallic iron from mantle disproportionation and slab serpentinization, to form Fe alloys containing carbon and hydrogen. Here we show experimental results on the phase relations and melting of the Fe‐C‐H system using laser‐heated diamond anvil cell and X‐ray diffraction techniques up to 72 GPa. The incorporation of hydrogen was found to lower the eutectic melting temperatures of Fe‐C alloy by ∼50–178 K at 20–70 GPa, facilitating the formation of metallic liquids in the deep mantle and thus enhancing the mobility and deep cycling of subducted carbon and hydrogen. Hydrogen also substitutes with carbon in Fe‐C metal to form hydride and diamond at relatively high‐temperature conditions (e.g., 42.6 GPa, >1885 K and 71.8 GPa, >1798 K). The hydrogen‐carbon‐enriched metallic liquids provide the necessary fluid environment for superdeep diamond growth.

 
more » « less
Award ID(s):
1829273 1555388 1565708
NSF-PAR ID:
10369962
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  
Publisher / Repository:
DOI PREFIX: 10.1029
Date Published:
Journal Name:
Geophysical Research Letters
Volume:
49
Issue:
13
ISSN:
0094-8276
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Nitrogen is considered to be transported from Earth′s surface to the top of the lower mantle through subduction. However, little is known on the transportation and fate of subducted nitrogen to the Earth′s interior during slab‐mantle interactions. In this study, the stability of subducted sedimentary nitrogen in the reduced mantle was investigated to 35 GPa and 1600 K by laser‐heated diamond anvil cell experiments and first‐principles calculations. Our results showed that subducted nitrogen‐bearing silicates and fluids could not coexist with the metallic iron or iron‐rich alloys, and reacted with them to form different products at high pressure‐temperature conditions. Combining our results with previous data, we re‐determined the relative stability of iron‐light element binary compounds to 35 GPa and 1600 K to be Fe‐O > Fe‐N > Fe‐S > Fe‐C. This stability sequence contributes to explaining the observation that iron nitrides are trapped as inclusions in sulfur‐depleted lower‐mantle diamonds and are absent in sulfur‐rich ones. The recycling efficiency of subducted sedimentary nitrogen is strongly related to the availability of the metallic iron of the reduced mantle. Hydration of the metallic iron limits the storage of nitrogen in it and contributes to recycling nitrogen to Earth′s surface. Therefore, unlike subducted continental sediments, subducted marine sediments are unlikely to transport a large amount of surficial nitrogen to the metallic iron of the reduced mantle in which nitrogen could reside over long geologic periods.

     
    more » « less
  2. Abstract

    The carbon and water cycles in the Earth's interior are linked to key planetary processes, such as mantle melting, degassing, chemical differentiation, and advection. However, the role of water in the carbon exchange between the mantle and core is not well known. Here, we show experimental results of a reaction between Fe3C and H2O at pressures and temperatures of the deep mantle and core‐mantle boundary (CMB). The reaction produces diamond, FeO, and FeHx, suggesting that water can liberate carbon from the core in the form of diamond (“core carbon extraction”) while the core gains hydrogen, if subducted water reaches to the CMB. Therefore, Earth's deep water and carbon cycles can be linked. The extracted core carbon can explain a significant amount of the present‐day mantle carbon. Also, if diamond can be collected by mantle flow in the region, it can result in unusually high seismic‐velocity structures.

     
    more » « less
  3. Abstract

    Iron‐dominant metallic phases are likely the primary hosts for nitrogen in the reduced deep Earth, hence the storage of nitrogen in the lower mantle and the core is governed by the behavior of the Fe‐N‐C system at high temperatures and pressures. In this study, phase transitions and thermoelastic properties of iron carbonitrides were investigated at high pressure‐temperature conditions by diamond anvil cell experiments and first‐principles calculations. Experimental data revealed no phase transition inε‐type Fe4(N0.6C0.4) or Fe7(N0.75C0.25)3up to 60 GPa at room temperature. At high temperature, Fe7(N0.75C0.25)3transforms into the Fe3C‐type phase at ∼27 GPa, and then into the Fe7C3‐type phase at ∼45 GPa, which is also corroborated by our theoretical calculations. We found that the phase stability of iron carbonitrides mainly depends on the N/C ratio, and the elastic properties of iron carbonitrides are dominantly affected by the Fe/(N+C) ratio. Iron carbonitrides with diverse structures may be the main host for nitrogen in the deep mantle. Some iron carbonitride inclusions in lower mantle diamonds could be the residue of the primordial mantle or originate from subducted nitrogen‐bearing materials, rather than iron‐enriched phases of the outer core. In addition, our experiments confirmed the existence of Fe7C3‐type Fe7C3‐Fe7N3solid solutions above 40 GPa. Fe7C3‐type Fe7(C, N)3has comparable density and thermoelastic properties to its isostructural endmembers and may be a promising candidate constituent of the Earth's inner core.

     
    more » « less
  4. Abstract

    Many lines of evidence from high P–T experiments, thermodynamic models, and natural observations suggest that slab-derived aqueous fluids, which flux mantle wedges contain variable amounts of dissolved carbon. However, constraints on the effects of H2O–CO2 fluids on mantle melting, particularly at mantle wedge P–T conditions, are limited. Here, we present new piston cylinder experiments on fertile and depleted peridotite compositions with 3.5 wt.% H2O and XCO2 [= molar CO2 / (CO2 + H2O)] of 0.04–0.17. Experiments were performed at 2–3 GPa and 1350°C to assess how temperature, peridotite fertility, and XCO2 of slab-derived fluid affects partial melting in mantle wedges. All experiments produce olivine + orthopyroxene +7 to 41 wt.% partial melt. Our new data, along with previous lower temperature data, show that as mantle wedge temperature increases, primary melts become richer in SiO2, FeO*, and MgO and poorer CaO, Al2O3, and alkalis when influenced by H2O–CO2 fluids. At constant P–T and bulk H2O content, the extent of melting in the mantle wedge is largely controlled by peridotite fertility and XCO2 of slab-fluid. High XCO2 depleted compositions generate ~7 wt.% melt, whereas, at identical P–T, low XCO2 fertile compositions generate ~30 to 40 wt.% melt. Additionally, peridotite fertility and XCO2 have significant effects on peridotite partial melt compositions. At a constant P–T–XCO2, fertile peridotites generate melts richer in CaO and Al2O3 and poorer in SiO2, MgO + FeO, and alkalis. Similar to previous experimental studies, at a constant P–T fertility condition, as XCO2 increases, SiO2 and CaO of melts systematically decrease and increase, respectively. Such distinctive effects of oxidized form of dissolved carbon on peridotite partial melt compositions are not observed if the carbon-bearing fluid is reduced, such as CH4-bearing. Considering the large effect of XCO2 on melt SiO2 and CaO concentrations and the relatively oxidized nature of arc magmas, we compare the SiO2/CaO of our experimental melts and melts from previous peridotite + H2O ± CO2 studies to the SiO2/CaO systematics of primitive arc basalts and ultra-calcic, silica-undersaturated arc melt inclusions. From this comparison, we demonstrate that across most P–T–fertility conditions predicted for mantle wedges, partial melts from bulk compositions with XCO2 ≥ 0.11 have lower SiO2/CaO than all primitive arc melts found globally, even when correcting for olivine fractionation, whereas partial melts from bulk compositions with XCO2 = 0.04 overlap the lower end of the SiO2/CaO field defined by natural data. These results suggest that the upper XCO2 limit of slab-fluids influencing primary arc magma formation is 0.04 < XCO2 < 0.11, and this upper limit is likely to apply globally. Lastly, we show that the anomalous SiO2/CaO and CaO/Al2O3 signatures observed in ultra-calcic arc melt inclusions can be reproduced by partial melting of either CO2-bearing hydrous fertile and depleted peridotites with 0 < XCO2 < 0.11 at 2–3 GPa, or from nominally CO2-free hydrous fertile peridotites at P > 3 GPa.

     
    more » « less
  5. Abstract

    The viscosity of iron alloy liquids is the key for the core dynamo and core‐mantle differentiation of terrestrial bodies. Here we measured the viscosity of Fe‐Ni‐C liquids up to 7 GPa using the floating sphere viscometry method and up to 330 GPa using first‐principles calculations. We found a viscosity increase at ∼3–5 GPa, coincident with a structural transition in the liquids. After the transition, the viscosity reaches ∼14–27 mPa·s, a factor of 2–4 higher than that of Fe and Fe‐S liquids. Our computational results from 5 to 330 GPa also indicate a high viscosity of the Fe‐Ni‐C liquids. For a carbon‐rich core in large terrestrial body, the level of turbulence in the outer core would be lessened approaching the inner core boundary. It is also anticipated that Fe‐Ni‐C liquids would percolate in Earth's deep silicate mantle at a much slower speed than Fe and Fe‐S liquids.

     
    more » « less