Iron Vacancies Accommodate Uranyl Incorporation into Hematite

Environmental Science & Technology
Martin E McBriartyEugene S Ilton

Abstract

Radiotoxic uranium contamination in natural systems and nuclear waste containment can be sequestered by incorporation into naturally abundant iron (oxyhydr)oxides such as hematite (α-Fe2O3) during mineral growth. The stability and properties of the resulting uranium-doped material are impacted by the local coordination environment of incorporated uranium. While measurements of uranium coordination in hematite have been attempted using extended X-ray absorption fine structure (EXAFS) analysis, traditional shell-by-shell EXAFS fitting yields ambiguous results. We used hybrid functional ab initio molecular dynamics (AIMD) simulations for various defect configurations to generate synthetic EXAFS spectra which were combined with adsorbed uranyl spectra to fit experimental U L3-edge EXAFS for U6+-doped hematite. We discovered that the hematite crystal structure accommodates a trans-dioxo uranyl-like configuration for U6+ that substitutes for structural Fe3+, which requires two partially protonated Fe vacancies situated at opposing corner-sharing sites. Surprisingly, the best match to experiment included significant proportions of vacancy configurations other than the minimum-energy configuration, pointing to the importance of incorpo...Continue Reading

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Citations

Jun 6, 2021·Chemosphere·Luke T TownsendSamuel Shaw
Jun 12, 2021·The Journal of Physical Chemistry Letters·Sebastian T MergelsbergEugene S Ilton
Jun 29, 2021·Environmental Science. Processes & Impacts·Pieter BotsJoanna C Renshaw
Aug 14, 2021·Journal of the American Chemical Society·Fabrizio OrtuLouise S Natrajan
Nov 7, 2019·Environmental Science & Technology·Eric J BylaskaEugene S Ilton
Nov 26, 2020·The Journal of Physical Chemistry Letters·Eugene S IltonEric J Bylaska
Nov 27, 2021·ACS Earth & Space Chemistry·Luke T TownsendKatherine Morris
Dec 10, 2021·Environmental Science & Technology·Olwen StaggSamuel Shaw

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