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Incorporation of chlorine in nuclear waste glasses using high-pressure vitrification: Solubility, speciation, and local environment of chlorine

  • Valentin Jolivet , Yann Morizet , Nicolas Trcera , Vincent Fernandez and Tomo Suzuki-Muresan
Published/Copyright: May 31, 2023
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American Mineralogist
From the journal American Mineralogist Volume 108 Issue 6

Abstract

The solubility, speciation, and local atomic environment of chlorine have been determined for aluminoborosilicate glasses equilibrated with various sources of chlorine (NaCl and PdCl2) at high pressure (0.5–1.5 GPa) and high temperature (1350–1400 °C). The Cl solubility reaches up to 11 mol% in borosilicate glass and appears to be strongly influenced by the concentration of network-modifying cations (Ca and Na) and increases with increasing CaO + Na2O content. The Cl solubility is enhanced in Ca-bearing rather than Na-bearing borosilicate glass, suggesting a higher affinity of chlorine for alkaline-earth cations. Cl K-edge XANES and Cl 2p XPS spectra reveal that chlorine dissolves in glasses only as chloride species (Cl–) and no evidence of oxidized species is observed. Using PdCl2 as a chlorine source leads to a pre-edge signal for PdCl2 in the XANES spectra. The EXAFS simulations show that the Cl– local environment is charge compensated by Na+ or Ca2+ at a distance to first neighbor on the order of 2.7 Å, which is comparable to the observed distances in crystalline chloride compounds. The coordination to charge compensating cation is lower in the case of Ca2+ (~1.1) than Na+ (~4.3).

Keywords: High-pressure; chlorine; nuclear waste glasses; spectroscopy; Experimental Halogens in Honor of Jim Webster

† Special collection papers can be found online at http://www.minsocam.org/MSA/AmMin/special-collections.html

Acknowledgments and funding

We thank Don Baker for handling our manuscript and the two anonymous reviewers for their fruitful comments that helped to improve the quality of the manuscript. The authors are grateful to the Région Pays de la Loire, which financed the current work through the Pari Scientifque “CIPress.” The authors thank the Laboratoire de Planétologie et Géosciences, the Institut des Matériaux Jean Rouxel, the Nantes Université, and the CNRS for providing access to the analytical facilities. We acknowledge SOLEIL for the provision of synchrotron radiation facilities, and we thank LUCIA staff for assistance in using the beamline. We also thank Nicolas Stéphant for support on the SEM/EDS analytical platform.

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Received: 2022-05-18
Accepted: 2022-08-02
Published Online: 2023-05-31
Published in Print: 2023-06-27

© 2023 by Mineralogical Society of America

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  1. A shallow salt pond analog for aqueous alteration on ancient Mars: Spectroscopy, mineralogy, and geochemistry of sediments from Antarctica’s Dry Valleys
  2. Incorporation of chlorine in nuclear waste glasses using high-pressure vitrification: Solubility, speciation, and local environment of chlorine
  3. Experimental constraints on miscibility gap between apatite and britholite and REE partitioning in an alkaline melt
  4. Thermal expansion of minerals in the tourmaline supergroup
  5. Viscosity of Earth’s inner core constrained by Fe–Ni interdiffusion in Fe–Si alloy in an internal-resistive-heated diamond anvil cell
  6. The distribution of carbonate in apatite: The environment model
  7. Low-temperature crystallography and vibrational properties of rozenite (FeSO4·4H2O), a candidate mineral component of the polyhydrated sulfate deposits on Mars
  8. Hydrothermal fluid signatures of the Yulong porphyry Cu-Mo deposit: Clues from the composition and U-Pb dating of W-bearing rutile
  9. Magnetic contributions to corundum-eskolaite and corundum-hematite phase equilibria: A DFT cluster expansion study
  10. Microchemistry and magnesium isotope composition of the Purang ophiolitic chromitites (SW Tibet): New genetic inferences
  11. Pyrite geochemistry in a porphyry-skarn Cu (Au) system and implications for ore formation and prospecting: Perspective from Xinqiao deposit, Eastern China
  12. UV/Vis single-crystal spectroscopic investigation of almandine-pyrope and almandinespessartine solid solutions: Part I. Spin-forbidden Fe2+,3+ and Mn2+ electronic-transition energies, crystal chemistry, and bonding behavior
  13. Single-crystal UV/Vis optical absorption spectra of almandine-bearing and spessartine garnet: Part II. An analysis of the spin-forbidden bands of Fe2+, Mn2+, and Fe3+
  14. Single-crystal UV/Vis absorption spectroscopy of aluminosilicate garnet: Part III. {Fe2+} + [Fe3+] → {Fe3+} + [Fe2+] intervalence charge transfer
  15. A novel method for experiments in a one-atmosphere box furnace
https://doi.org/10.2138/am-2022-8599
Keywords for this article
High-pressure; chlorine; nuclear waste glasses; spectroscopy; Experimental Halogens in Honor of Jim Webster

Articles in the same Issue

  1. A shallow salt pond analog for aqueous alteration on ancient Mars: Spectroscopy, mineralogy, and geochemistry of sediments from Antarctica’s Dry Valleys
  2. Incorporation of chlorine in nuclear waste glasses using high-pressure vitrification: Solubility, speciation, and local environment of chlorine
  3. Experimental constraints on miscibility gap between apatite and britholite and REE partitioning in an alkaline melt
  4. Thermal expansion of minerals in the tourmaline supergroup
  5. Viscosity of Earth’s inner core constrained by Fe–Ni interdiffusion in Fe–Si alloy in an internal-resistive-heated diamond anvil cell
  6. The distribution of carbonate in apatite: The environment model
  7. Low-temperature crystallography and vibrational properties of rozenite (FeSO4·4H2O), a candidate mineral component of the polyhydrated sulfate deposits on Mars
  8. Hydrothermal fluid signatures of the Yulong porphyry Cu-Mo deposit: Clues from the composition and U-Pb dating of W-bearing rutile
  9. Magnetic contributions to corundum-eskolaite and corundum-hematite phase equilibria: A DFT cluster expansion study
  10. Microchemistry and magnesium isotope composition of the Purang ophiolitic chromitites (SW Tibet): New genetic inferences
  11. Pyrite geochemistry in a porphyry-skarn Cu (Au) system and implications for ore formation and prospecting: Perspective from Xinqiao deposit, Eastern China
  12. UV/Vis single-crystal spectroscopic investigation of almandine-pyrope and almandinespessartine solid solutions: Part I. Spin-forbidden Fe2+,3+ and Mn2+ electronic-transition energies, crystal chemistry, and bonding behavior
  13. Single-crystal UV/Vis optical absorption spectra of almandine-bearing and spessartine garnet: Part II. An analysis of the spin-forbidden bands of Fe2+, Mn2+, and Fe3+
  14. Single-crystal UV/Vis absorption spectroscopy of aluminosilicate garnet: Part III. {Fe2+} + [Fe3+] → {Fe3+} + [Fe2+] intervalence charge transfer
  15. A novel method for experiments in a one-atmosphere box furnace
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