Incorporation of uranium into hematite during crystallization from ferrihydrite

Timothy A. Marshall, Katherine Morris, Gareth T.W. Law, Francis R. Livens, J. Frederick W. Mosselmans, Pieter Bots, Samuel Shaw

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Abstract

Ferrihydrite was exposed to U(VI)-containing cement leachate (pH 10.5) and aged to induce crystallization of hematite. A combination of chemical extractions, TEM, and XAS techniques provided the first evidence that adsorbed U(VI) (≈3000 ppm) was incorporated into hematite during ferrihydrite aggregation and the early stages of crystallization, with continued uptake occurring during hematite ripening. Analysis of EXAFS and XANES data indicated that the U(VI) was incorporated into a distorted, octahedrally coordinated site replacing Fe(III). Fitting of the EXAFS showed the uranyl bonds lengthened from 1.81 to 1.87 Å, in contrast to previous studies that have suggested that the uranyl bond is lost altogether upon incorporation into hematite the results of this study both provide a new mechanistic understanding of uranium incorporation into hematite and define the nature of the bonding environment of uranium within the mineral structure. Immobilization of U(VI) by incorporation into hematite has clear and important implications for limiting uranium migration in natural and engineered environments. © 2014 American Chemical Society.
Original languageEnglish
Pages (from-to)3724-3731
Number of pages8
JournalEnvironmental Science and Technology
Volume48
Issue number7
DOIs
Publication statusPublished - 3 Mar 2014

Fingerprint

Uranium
ferrihydrite
Crystallization
hematite
uranium
crystallization
ripening
immobilization
Minerals
leachate
incorporation
ferric oxide
transmission electron microscopy
Cements
cement
Agglomeration
Transmission electron microscopy
mineral

Keywords

  • uranium incorporation
  • hematite
  • crystallization
  • ferrihydrite
  • bonding environment
  • immobilization
  • immobilisation
  • radioactive waste disposal

Cite this

Marshall, T. A., Morris, K., Law, G. T. W., Livens, F. R., Mosselmans, J. F. W., Bots, P., & Shaw, S. (2014). Incorporation of uranium into hematite during crystallization from ferrihydrite. Environmental Science and Technology , 48(7), 3724-3731. https://doi.org/10.1021/es500212a
Marshall, Timothy A. ; Morris, Katherine ; Law, Gareth T.W. ; Livens, Francis R. ; Mosselmans, J. Frederick W. ; Bots, Pieter ; Shaw, Samuel. / Incorporation of uranium into hematite during crystallization from ferrihydrite. In: Environmental Science and Technology . 2014 ; Vol. 48, No. 7. pp. 3724-3731.
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Marshall, TA, Morris, K, Law, GTW, Livens, FR, Mosselmans, JFW, Bots, P & Shaw, S 2014, 'Incorporation of uranium into hematite during crystallization from ferrihydrite', Environmental Science and Technology , vol. 48, no. 7, pp. 3724-3731. https://doi.org/10.1021/es500212a

Incorporation of uranium into hematite during crystallization from ferrihydrite. / Marshall, Timothy A.; Morris, Katherine; Law, Gareth T.W.; Livens, Francis R.; Mosselmans, J. Frederick W.; Bots, Pieter; Shaw, Samuel.

In: Environmental Science and Technology , Vol. 48, No. 7, 03.03.2014, p. 3724-3731.

Research output: Contribution to journalArticle

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AU - Bots, Pieter

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