Thermodynamics of Liquid Immiscibility in Iron-Silicate Melt Systems: A Study of Nuclear Fallout Glass
Source abstract
Abstract
In a ground-interacting nuclear explosion, elements derived from environmental and anthropogenic material, such as iron, silicon, and aluminum, can be incorporated into the fireball. When significant amounts of metals are entrained, the resulting melt may display immiscible textures. The composition of these textures is a record of the temperature of formation and cooling rates (or thermodynamic stability) of the melts and can provide unique constraints on the early cooling conditions of these events. Here, a thermodynamic approach using calculated phase diagrams, the CALPHAD method, is used to predict temperature and composition ranges where stable liquid immiscibility might result in the textures observed in nuclear fallout glass. Sensitivity of the immiscibility to the presence of relative Al, Ca, and Mg content is also explored and compared to fallout samples, and partition coefficients are introduced to understand the preferred distribution of components into each liquid phase.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Nuclear Materials and Properties · High-pressure geophysics and materials · Thermal and Kinetic Analysis
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Lawrence Livermore National Laboratory, Livermore, CA 94551-0808, USA
Department of Nuclear Engineering, University of California, Berkeley, CA 94720-5800, USA
Funding
Lawrence Livermore National Laboratory
References (44)
Show source-provided references
1. The compositions, structures and origins of radioactive fall-out particles10.1016/0016-7037(60)90016-8 ↗
2. Characterizing major and trace element compositions in fallout melt glass from a near-surface nuclear test10.1016/j.jenvrad.2021.106796 ↗
3. Iron-rich microstructure records of high temperature multi-component silicate melt behavior in nuclear fallout10.1016/j.jenvrad.2021.106700 ↗
4. Chemical and structural characterization of particulate fallout isolated from air-filters10.1007/s10967-022-08442-7 ↗
5. When the dust settles: Stable xenon isotope constraints on the formation of nuclear fallout10.1016/j.jenvrad.2014.06.011 ↗
6. Diffusive mass transport in agglomerated glassy fallout from a near-surface nuclear test10.1016/j.gca.2017.12.011 ↗
7. Deposition of vaporized species onto glassy fallout from a near-surface nuclear test10.1016/j.gca.2016.10.036 ↗
8. Trinitite redux: Mineralogy and petrology10.2138/am-2015-4921 ↗
9. Nuclear forensics: Searching for nuclear device debris in trinitite-hosted inclusions10.1007/s10967-012-1654-9 ↗
10. Very high-temperature impact melt products as evidence for cosmic airbursts and impacts 12,900 years ago10.1073/pnas.1204453109 ↗
11. Genda, T. (2022). Nuclear Fallout Formation in Iron Rich Environments, University of California.
12. Constraints on fallout melt glass formation from a near-surface nuclear test10.1007/s10967-014-3293-9 ↗
13. A geochemical approach to constraining the formation of glassy fallout debris from nuclear tests10.1007/s00410-016-1320-2 ↗
14. Silicate liquid immiscibility in magmas and in the system K2O-FeO-AI2O3-SiO2: An example of serendipity10.1016/0016-7037(78)90250-8 ↗
15. Kaufman, L., and Bernstein, H. (1970). Computer Calculation of Phase Diagrams. With Special Reference to Refractory Metals, Academic Press.
16. Saunders, N., and Miodownik, A.P. (1998). CALPHAD (Calculation of Phase Diagrams): A Comprehensive Guide, Elsevier.
17. Sundman, B., Lukas, H., and Fries, S. (2007). Computational Thermodynamics: The Calphad Method, Cambridge University Press.
18. Genda, T., Moore, E., Perron, A., and Knight, K. (2020). Phase Formation in Nuclear Fallout, Lawrence Livermore National Lab.(LLNL).
19. Thermodynamic reassessment of the Y2O3–Al2O3–SiO2 system and its subsystems10.1016/j.calphad.2008.03.003 ↗
20. Linking first-principles energetics to CALPHAD: An application to thermodynamic modeling of the Al-Ca binary system10.1007/s11661-005-0133-0 ↗
21. An assessment of the entire Al–Fe system including D03 ordering10.1016/j.actamat.2009.02.046 ↗
22. Experimental investigation and thermodynamic calculation of the central part of the Mg–Al phase diagram
23. A re-evaluation of the liquid phases in the CaO–Al2O3 and MgO–Al2O3 systems10.1016/j.calphad.2004.09.001 ↗
24. Thermodynamic calculation of the ternary system Al-Si-C10.1016/S0364-5916(96)00027-2 ↗
25. Thermodynamic reassessment of the Si3N4–AlN–Al2O3–SiO2 system—Modeling of the SiAlON and liquid phases10.1016/j.calphad.2006.11.002 ↗
26. A reassessment of the Ca-Fe-O system10.1016/S0364-5916(96)00039-9 ↗
27. Contribution to the experimental and thermodynamic assessment of the Al-Ca-Fe-Si system—I. Al-Ca-Fe, Al-Ca-Si, Al-Fe-Si and Ca-Fe-Si systems10.1016/0364-5916(94)90034-5 ↗
28. Thermodynamic calculation of the CaO-MgO system10.1016/0364-5916(89)90006-0 ↗
29. Thermodynamic modelling of the Cr–Fe–Ni–O system10.1016/j.calphad.2008.04.005 ↗
30. An assessment of the Ca-Fe-O-Si system10.1007/s11663-997-0030-6 ↗
31. An assessment of the Fe-C-Si system10.1007/BF02664987 ↗
32. The Magnesium—Oxygen system10.1016/0364-5916(93)90006-W ↗
33. A study of the thermodynamic properties of MgO-SiO2 system10.1016/0364-5916(89)90005-9 ↗
34. Thermodynamic calculation of some subsystems of the Al-Ca-Mg-Si-O system10.1007/BF02667878 ↗
35. An Assessment of the Fe-O-Si System10.1007/s11663-997-0029-z ↗
36. Experimental study of ternary Ca–Mg–Si phase equilibria and thermodynamic assessment of Ca–Si and Ca–Mg–Si systems10.1016/j.intermet.2003.07.001 ↗
37. A two-sublattice model for molten solutions with different tendency for ionization10.1007/BF02816052 ↗
38. Modification of the two-sublattice model for liquids10.1016/0364-5916(91)90010-H ↗
39. (2023, January 20). Thermodynamics of Advanced Fuels-International Database (TAF-ID). Nucl. Energy Agency NEA (n.d.). Available online: https://www.oecd-nea.org/jcms/pl_24703/thermodynamics-of-advanced-fuels-international-database-taf-id.
40. Liquid Immiscibility in Silicate Melts and Related Systems10.2138/rmg.2007.65.4 ↗
41. The nature of phase separation in binary oxide melts and glasses. I. Silicate systems10.1016/S0022-3093(02)01043-8 ↗
42. Gaskell, D.R. (2008). Introduction to the Thermodynamics of Materials, Taylor & Francis Group, LLC.. [5th ed.].
43. The system FeO-Al2O3-SiO210.2465/ganko1941.37.83 ↗
44. Verteilung eines Stoffes zwischen zwei Lösungsmitteln und zwischen Lösungsmittel und Dampfraum10.1515/zpch-1891-0806 ↗