Can Mineral Growth by Oriented Attachment Lead to Incorporation of Uranium into the Structure of Fe(oxyhydr)oxides?
EMSL Project ID
49800
Abstract
Previous laboratory work has shown that uranium can be incorporated into the structure of hematite and goethite during co-precipitation and redox transformation of ferrihydrite, respectively. However, it is becoming increasingly apparent that a preferred mechanism of growth for low solubility phases such as the Fe(III)-(oxyhydr)oxides is oriented aggregation (OA) of nano-particles instead of classical mechanisms involving atom by atom attachment. Consequently, we propose to study whether uranium can be incorporated into the structure of goethite (hematite) during oriented aggregation of nano-particles (~1-2 nm) that eventually form single crystal goethite rods on the order of 50 nm long and 10 nm in width. U(VI) will be adsorbed to the nano-particles at different stages of growth and characterized with a number of advanced techniques such as aberration corrected scanning transmission electron microscopy (ACSTEM), Cryo-TEM, X-ray photoelectron spectroscopy (XPS), and X-ray absorption spectroscopy (EXAFS and XANES). Ab initio molecular dynamic (AIMD) informed EXAFS will be used to determine the coordination environment of U and correlated to ACSTEM micrographs showing the location of individual uranium atoms. The laboratory results, in conjunction with the same high-powered methods discussed above, will be used to interpret the mode of uranium association with Fe(III)-(oxyhydr)oxides from natural systems where uranium has shown closed system behavior over millennia despite ongoing advection of water.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2017-10-01
End Date
2019-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Bylaska E.J., J.G. Catalano, S.T. Mergelsberg, S.A. Saslow, O. Qafoku, M.P. Prange, and E.S. Ilton. 2019. "Association of Defects and Zinc in Hematite." Environmental Science & Technology 53, no. 23:13687-13694. PNNL-SA-144849. doi:10.1021/acs.est.9b04323
McBriarty M.E., S.N. Kerisit, E.J. Bylaska, S. Shaw, K. Morris, and E.S. Ilton. 2018. "Iron Vacancies Accommodate Uranyl Incorporation into Hematite." Environmental Science & Technology 52, no. 11:6282-6290. PNNL-SA-131768. doi:10.1021/acs.est.8b00297
Prange M.P., X. Zhang, E.S. Ilton, L. Kovarik, M.H. Engelhard, and S.N. Kerisit. 2018. "Electronic Response of Aluminum-Bearing Minerals." Journal of Chemical Physics 149, no. 2:024502. PNNL-SA-132258. doi:10.1063/1.5037104
Soltis J.A., M.E. McBriarty, O. Qafoku, S.N. Kerisit, E. Nakouzi, J.J. De Yoreo, and E.S. Ilton. 2019. "Can Mineral Growth by Oriented Attachment Lead to Incorporation of Uranium(VI) into the Structure of Goethite?." Environmental Science Nano 6, no. 10:3000-3009. PNNL-SA-145133. doi:10.1039/c9en00779b