Plutonium(IV) Sorption during Ferrihydrite Nanoparticle Formation

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http://hdl.handle.net/10138/308512

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Smith , K F , Morris , K , Law , G T W , Winstanley , E H , Livens , F R , Weatherill , J S , Abrahamsen-Mills , L G , Bryan , N D , Mosselmans , J F W , Cibin , G , Parry , S , Blackham , R , Law , K A & Shaw , S 2019 , ' Plutonium(IV) Sorption during Ferrihydrite Nanoparticle Formation ' , ACS Earth and Space Chemistry , vol. 3 , no. 11 , pp. 2437-2442 . https://doi.org/10.1021/acsearthspacechem.9b00105

Title: Plutonium(IV) Sorption during Ferrihydrite Nanoparticle Formation
Author: Smith, Kurt F.; Morris, Katherine; Law, Gareth T. W.; Winstanley, Ellen H.; Livens, Francis R.; Weatherill, Joshua S.; Abrahamsen-Mills, Liam G.; Bryan, Nicholas D.; Mosselmans, J. Frederick W.; Cibin, Giannantonio; Parry, Stephen; Blackham, Richard; Law, Kathleen A.; Shaw, Samuel
Contributor: University of Helsinki, Department of Chemistry
Date: 2019-11
Language: eng
Number of pages: 11
Belongs to series: ACS Earth and Space Chemistry
ISSN: 2472-3452
URI: http://hdl.handle.net/10138/308512
Abstract: Understanding interactions between iron (oxyhydr)oxide nanoparticles and plutonium is essential to underpin technology to treat radioactive effluents, in cleanup of land contaminated with radionuclides, and to ensure the safe disposal of radioactive wastes. These interactions include a range of adsorption, precipitation, and incorporation processes. Here, we explore the mechanisms of plutonium sequestration during ferrihydrite precipitation from an acidic solution. The initial 1 M HNO3 solution with Fe(III)((aq)) and Pu-242(IV)((aq)) underwent controlled hydrolysis via the addition of NaOH to pH 9. The majority of Fe(III)((aq)) and Pu(IV)((aq)) was removed from solution between pH 2 and 3 during ferrihydrite formation. Analysis of Pu-ferrihydrite by extended X-ray absorption fine structure (EXAFS) spectroscopy showed that Pu(IV) formed an inner-sphere tetradentate complex on the ferrihydrite surface, with minor amounts of PuO2 present. Best fits to the EXAFS data collected from Pu-ferrihydrite samples aged for 2 and 6 months showed no statistically significant change in the Pu(IV)-Fe oxyhydroxide surface complex despite the ferrihydrite undergoing extensive recrystallization to hematite. This suggests the Pu remains strongly sorbed to the iron (oxyhydr)oxide surface and could be retained over extended time periods.
Subject: Plutonium
ferrihydrite
hematite
nanoparticle
XAS
sorption
REDUCTION
ADSORPTION
IRON
SPECIATION
FERROZINE
MAGNETITE
HEMATITE
U(VI)
WASTE
116 Chemical sciences
114 Physical sciences
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