Understanding Earth’s accretion and primary differentiation is a long-standing goal of geology. The segregation of FeNi metal from molten silicate to form Earth’s core is expected to deplete and fractionate the highly siderophile elements (HSEs). Estimates of the primitive upper mantle (PUM) composition however, reveal only modest HSE depletions and chondritic element ratios. Past experiments to determine if the mantle composition is set by high-temperature metal-silicate equilibrium have involved measuring the solubility of HSEs in silicate melt at conditions more reducing than the iron-wustite (IW) buffer. Accurate determination of solubilities at such conditions has been hindered by the formation of dispersed metal inclusions; this work describes methods to circumvent the problem. Results of three separate studies are presented which document the solubility of Re, Pt and Au in molten silicate which is demonstrably nugget-free. Data obtained from experiments done at 0.1 MPa–2 GPa, 1573–2573 K and ~ IW -1.5 to +3 reveal: 1) Re, Pt and Au solubility increases with increasing temperature, 2) Re solubility increases with increasing oxygen fugacity (fO2), consistent with dissolution as oxide species, 3) Below ~ IW +3, Pt and Au solubility increases with decreasing fO2, consistent with dissolution as neutral or silicide species, and 4) that Au is amongst the most soluble HSE in molten silicate, with values increasing with temperature, but insensitive to changes in P, fO2 and melt composition, making it well suited as a geothermometer for core formation. Partition coefficients calculated from these and previous solubility measurements indicate that metal-silicate equilibrium is unable to reproduce the Re/Os and Pt/Os ratios required by PUM Os isotope systematics if simultaneously accounting for the observed absolute element abundances. Instead, results support late accretion of material following core formation, elevating element abundances and endowing chondritic inter-element ratios. Experimental results are incorporated into a terrestrial accretion model, which differs from the standard approach by explicitly accounting for the distribution of oxygen. Model results show siderophile element abundances in PUM are best reproduced if the mantle undergoes oxidation during accretion and metal-silicate equilibrium occurs near the peridotite solidus.
| Identifer | oai:union.ndltd.org:LACETR/oai:collectionscanada.gc.ca:OTU.1807/65449 |
| Date | 19 June 2014 |
| Creators | Bennett, Neil |
| Contributors | Brenan, James |
| Source Sets | Library and Archives Canada ETDs Repository / Centre d'archives des thèses électroniques de Bibliothèque et Archives Canada |
| Language | en_ca |
| Detected Language | English |
| Type | Thesis |
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