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- All Subjects: Hydrogen
Description
Hydrogen is the main constituent of stars, and thus dominates the protoplanetary disc from which planets are born. Many planets may at some point in their growth have a high-pressure interface between refractory planetary materials and ahydrogen-dominated atmosphere. However, little experimental data for these materials at the relevant pressure-temperature conditions exists. I have experimentally explored the interactions between planetary materials and hydrogen at high P-T conditions utilizing the pulsed laser-heated diamond-anvil cell. First, I found that ferric/ferrous iron (as Fe2O3 hematite and (Mg,Fe)O ferropericlase) are reduced to metal by hydrogen: Fe2O3 + 4H2 → 2FeO + H2O + 3H2 → 2FeH + 3H2O and (Mg1−xFex) O + 3/2 xH2 → xFeH + (1 − x) MgO + xH2O respectively. This reduction of iron by hydrogen is important because it produces iron metal and water from iron oxide. This can partition H into the core (as FeH) or mantle (as H2O/OH−) of a growing planet.
Next, I expanded my starting materials to silicates. I conducted experiments on San Carlos Olivine at pressures of 5-42 GPa. In the presence hydrogen, I observed the breakdown of molten magnesium silicate and the reduction of both iron and silicon to metal, forming alloys of both Fe-H and Fe-Si: Mg2SiO4 + 2H2 + 3Fe →
2MgO + FeSi + 2FeH + 2H2O.
Similar experiments using natural fayalite (Fe2SiO4) as a starting material at pressures of 5-21 GPa yielded similar results. Hydrogen reduced iron to metal as it did in experiments with iron oxides. Unlike with San Carlos olivine, above 10 GPa silicon remained oxidized, implying the following reaction: Fe2SiO4 + 3H2 → 2FeH+2H2O +SiO2. However, below 7 GPa, silicon reduces and alloys with iron. The formation of Fe-Si alloys from silicates facilitated by hydrogen could have important effects for core composition in growing planets. I also observed at low pressures (<10 GPa), quenched iron melt can trap more hydrogen than previously thought (H/Fe nearly 2 instead of 1). This may have important effects for the chemical sequestration of a hydrogen atmosphere at shallow depths in an early magma ocean.
All of the experimental work presented herein show that the composition, chemical partitioning, and phase stability of the condensed portion of growing planets can be modified via interaction with overlaying or ingassed volatile species.
ContributorsAllen-Sutter, Harrison (Author) / Shim, Sang-Heon Dan (Thesis advisor) / Li, Mingming (Committee member) / Leinenweber, Kurt D (Committee member) / Tyburczy, James A (Committee member) / Gabriel, Travis S.J. (Committee member) / Arizona State University (Publisher)
Created2022
Description
Seismic observations have revealed two large low shear velocity provinces (LLSVPs) in the lowermost mantle beneath Pacific and Africa. One hypothesis for the origin of LLSVPs is that they are caused by accumulation of subducted oceanic crust on the core-mantle boundary (CMB). Here, I perform high resolution geodynamical calculations to test this hypothesis. The result shows that it is difficult for a thin (~ 6 km) subducted oceanic crust to accumulate on the CMB, and the major part of it is viscously stirred into the surrounding mantle. Another hypothesis for the origin of LLSVPs is that they are caused by thermochemical piles of more-primitive material which is remnant of Earth's early differentiation. In such case, a significant part of the subducted oceanic crust would enter the more-primitive reservoir, while other parts are either directly entrained into mantle plumes forming on top of the more-primitive reservoir or stirred into the background mantle. As a result, mantle plumes entrain a variable combination of compositional components including more-primitive material, old oceanic crust which first enters the more-primitive reservoir and is later entrained into mantle plumes with the more-primitive material, young oceanic crust which is directly entrained into mantle plumes without contacting the more-primitive reservoir, and depleted background mantle material. The result reconciles geochemical observation of multiple compositional components and varying ages of oceanic crust in the source of ocean-island basalts. Seismic studies have detected ultra-low velocity zones (ULVZs) in some localized regions on the CMB. Here, I present 3D thermochemical calculations to show that the distribution of ULVZs provides important information about their origin. ULVZs with a distinct composition tend to be located at the edges of LLSVPs, while ULVZs solely caused by partial melting tend to be located inboard from the edges of LLSVPs. This indicates that ULVZs at the edges of LLSVPs are best explained by distinct compositional heterogeneity, while ULVZs located insider of LLSVPs are better explained by partial melting. The results provide additional constraints for the origin of ULVZs.
ContributorsLi, Mingming (Author) / McNamara, Allen K (Thesis advisor) / Garnero, Edward J (Committee member) / Shim, Sang-Heon (Committee member) / Tyburczy, James (Committee member) / Clarke, Amanda (Committee member) / Arizona State University (Publisher)
Created2015
Description
The transport of hydrogen to the Earth’s deep interior remains uncertain. The upper mantle minerals have very low hydrogen solubilities (hundreds of ppm). The hydrogen storage capability in the transition zone minerals (2 wt%) is high compared to those of the upper mantle. The hydrogen storage in the lower mantle is not well known. The main minerals in the lower mantle bridgmanite and ferropericlase have very low hydrogen storage capacities (less than 20 ppm). In order to further understand the hydrogen storage in the lower mantle, a series of experiments had been conducted to simulate the environment similar to the Earth’s mantle. The experiments with hydrous Mg2SiO4 ringwoodite (Rw) show that it converts to crystalline dense hydrous silica, stishovite (Stv) or CaCl2-type SiO2(mStv), containing ∼1 wt% H2O together with bridgmanite (Brd) and MgO at the pressure-temperature conditions expected for lower mantle depths between approximately 660 to 1600 km. Brd would break down partially to dense hydrous silica (6–25 mol%) and(Mg,Fe)O in mid-mantle regions with 0.05–0.27 wt% H2O. The hydrous stishovite has a CaCl2 structure, which is common among hydrous minerals in the lower mantle. Based on this observation, I hypothesize the existence of hydrous phases in the lower mantle. The experiments found a new hexagonal iron hydroxide (η-Fe12O18+x/2Hx) between the stability fields of the epsilon and pyrite-type FeOOH at 60–80 GPa and high temperature. The new phase contains less H2O, limiting the H2O transport from the shallow to the deep mantle in the Fe–O–H system. Possible hydrogen storage in Ca-perovskite was studied. CaPv could contain 0.5–1 wt% water and the water in CaPv could distort the crystal structure of CaPv from cubic to tetragonal structure. In conclusion, hydrogen can be stored in hydrous stishovite in the shallower depth of the lower mantle. At greater depth, the new η phase and pyrite-type phase would take over the hydrogen storage. The role of CaPv in deep water storage needs to be considered in future studies.
ContributorsChen, Huawei (Author) / Shim, Sang-Heon (Thesis advisor) / Garnero, Edward (Committee member) / Bose, Maitrayee (Committee member) / Li, Mingming (Committee member) / Leinenweber, Kurt (Committee member) / Arizona State University (Publisher)
Created2019