Startseite Ab initio calculations of uranium and thorium storage in CaSiO3-perovskite in the Earth’s lower mantle
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Ab initio calculations of uranium and thorium storage in CaSiO3-perovskite in the Earth’s lower mantle

  • Samuel N. Perry EMAIL logo , Jeffrey S. Pigott und Wendy R. Panero
Veröffentlicht/Copyright: 9. Februar 2017
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American Mineralogist
Aus der Zeitschrift American Mineralogist Band 102 Heft 2

Abstract

Earth’s mantle convection is powered in part by the radiogenic heat released by the decay of 238U, 235U, 232Th, and 40K. We present ab initio calculations of uranium and thorium incorporation in CaSiO3-perovskite with and without aluminum, and propose that aluminous calcium silicate perovskite is the likely host of uranium and thorium in the lower mantle. At 15 GPa, the enthalpies of solution into aluminum-free CaSiO3-perovskite are 10.34 kJ/mol for U4+ and 12.52 kJ/mol for Th4+ in SiO2 saturated systems, while the enthalpies are 17.09 kJ/mol and 19.27 kJ/mol, respectively, in CaO saturated systems. Coupled substitution of U4+ and Th4+ with aluminum is thermodynamically favored, with the enthalpies of solution negative for U4+ and near 0 kJ/mol for Th4+ throughout the stability field of CaSiO3-perovskite. Therefore, U incorporation into CaSiO3-perovskite is spontaneous in the presence of aluminum while Th forms a near ideal solid solution, implying these elements are potentially compatible with respect to partial melting in the transition zone and lower mantle. Furthermore, the solid solution reactions of U4+ and Th4+ are broadly similar to each other, suggesting a restriction on the fractionation of these actinides between the upper and lower mantle. U and Th compatibility in the presence of Al has implications regarding actinide transport into the deep mantle within subducting slabs and the geochemical content of seismic anomalies at the core-mantle boundary.

Keywords: Density functional theory; calcium-silicate perovskite; lower mantle mineralogy; uranium; thorium
† Present address: Department of Civil & Environmental Engineering; University of Notre Dame, Notre Dame, IN 46556, U.S.A

Acknowledgments

Support to S.N.P. from the Ohio State Undergraduate Research Scholarship, the Friends of Orton Hall fund grant and the Columbus Rock and Mineral Society scholarship. Further support for this research comes from NSF EAR 09-55647 and NSF EAR-PF 14-52545 to W.R.P. and J.S.P., respectively. All calculations were run at the Ohio Supercomputer Center, under computing award PAS0238-1 to W.R.P. We thank Bethany Chidester, Alexandre Corgne, and Razvan Caracas for their insightful reviews of this manuscript and their constructive feedback.

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Received: 2015-4-18
Accepted: 2015-9-19
Published Online: 2017-2-9
Published in Print: 2017-2-1

© 2017 by Walter de Gruyter Berlin/Boston

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https://doi.org/10.2138/am-2017-5816
Schlagwörter für diesen Artikel
Density functional theory; calcium-silicate perovskite; lower mantle mineralogy; uranium; thorium

Artikel in diesem Heft

  1. Highlights & Breakthroughs
  2. Rover observations in Gusev Crater: Evidence for a style of weathering unique to Mars?
  3. Special collection: Martian rocks and minerals: perspectives from rovers, orbiters, and meteorites
  4. Wishstone to Watchtower: Amorphous alteration of plagioclase-rich rocks in Gusev crater, Mars
  5. Special collection: geology and geobiology of lassen volcanic national park
  6. Oxygen isotope geochemistry of mafic phenocrysts in primitive mafic lavas from the southernmost Cascade Range, California
  7. Special collection: Dynamics of magmatic processes
  8. Geochemical and radiogenic isotope probes of Ischia volcano, Southern Italy: Constraints on magma chamber dynamics and residence time
  9. Fluids In The Crust
  10. Experimental tests on achieving equilibrium in synthetic fluid inclusions: Results for scheelite, molybdenite, and gold solubility at 800 °C and 200 MPa
  11. Special collection: Earth analogs for martian geological materials and processes
  12. Mineralogy and chemistry of San Carlos high-alkali basalts: Analyses of alteration with application for Mars exploration
  13. Special collection: Water in nominally hydrous and anhydrous minerals
  14. Effect of iron and trivalent cations on OH defects in olivine
  15. Chemistry and Mineralogy of Earth’s Mantle
  16. SiC-dominated ultra-reduced mineral assemblage in carbonatitic xenoliths from the Dalihu basalt, Inner Mongolia, China
  17. Chemistry and Mineralogy of Earth’s Mantle
  18. Ab initio calculations of uranium and thorium storage in CaSiO3-perovskite in the Earth’s lower mantle
  19. Spinels renaissance: The past, present, and future of those ubiquitous minerals and materials
  20. Raman spectroscopy and the inversion degree of natural Cr-bearing spinels
  21. Spinels Renaissance: The Past, Present, and Future of Those Ubiquitous Minerals and Materials
  22. Chromium influence on Mg-Al intracrystalline exchange in spinels and geothermometric implications
  24. Adakite metasomatism in a back-arc mantle peridotite xenolith from the Sea of Japan
  26. Effects of fluorine content on the elastic behavior of topaz [Al2SiO4(F,OH)2]
  28. Equation of state and hyperfine parameters of high-spin bridgmanite in the Earth’s lower mantle by synchrotron X-ray diffraction and Mössbauer spectroscopy
  30. Calibration of Fe XANES for high-precision determination of Fe oxidation state in glasses: Comparison of new and existing results obtained at different synchrotron radiation sources
  32. Bacterially mediated morphogenesis of struvite and its implication for phosphorus recovery
  34. High-pressure high-temperature Raman spectroscopy of kerogen: Relevance to subducted organic carbon
  36. Determination of pressure in aqueo-carbonic fluid inclusions at high temperatures from measured Raman frequency shifts of CO2
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  48. New Mineral Names
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