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Practical advice on monitoring of U and Pu with marine bivalve mollusks near the Fukushima Daiichi Nuclear Power Plant
2020
Zuykov, Michael | Fowler, Scott W. | Archambault, Philippe | Spiers, Graeme | Schindler, Michael
Following the Fukushima Daiichi nuclear power plant accident in 2011, some marine radionuclide monitoring studies report a lack of evidence for contamination of Japanese coastal waters by U and Pu, or state that marine contamination by them was negligible. Nevertheless, Fukushima-derived U and Pu were reported as associated with Cs-rich microparticles (CsMPs) found in local soil, vegetation, and river/lake sediments. Over time, CsMPs can be transported to the sea via riverine runoff where actinides, as expected, will leach. We recommend establishing a long-term monitoring of U and Pu in the nearshore area of the Fukushima Prefecture using marine bivalve mollusks; shells, byssal threads and soft tissues should all be analyzed. Here, based on results from Th biosorption experiments, we propose that U and Pu could be present at concentrations several times higher in shells with a completely destroyed external shell layer (periostracum) than in shells with intact periostracum.
Show more [+] Less [-]Selectivity in the complexation of actinides by humic substances
1997
Zhang, Y.J. | Bryan, N.D. | Livens, F.R. | Jones, M.N. (Department of Chemistry, University of Manchester, Manchester M13 9PL (United Kingdom))
Fate of Lu(III) sorbed on 2-line ferrihydrite at pH 5.7 and aged for 12 years at room temperature. I: insights from ICP-OES, XRD, ESEM, AsFlFFF/ICP-MS, and EXAFS spectroscopy
2019
Finck, Nicolas | Bouby, Muriel | Dardenne, Kathy
Two-line ferrihydrite (2LFh) was aged for 12 years under ambient conditions and sheltered from light in the presence of Lu(III) used as surrogate for trivalent actinides. 2LFh aging produced hematite rhombohedra with overgrown acicular goethite particles. Analysis of the homogeneous suspension by asymmetrical flow field-flow fractionation (AsFlFFF) coupled to ICP-MS indicated that particles have a mean hydrodynamic diameter of about 140 nm and the strong correlation of the Fe and Lu fractograms hinted at a structural association of the lanthanide with the solid phase(s). Unfortunately, recoveries were low and thus results cannot be considered representative of the whole sample. The suspension was centrifuged and X-ray absorption spectroscopy (XAS) at the Lu L₃-edge on the settled particles indicated that Lu(III) is sixfold coordinated by oxygen atoms, pointing to a retention by structural incorporation within particles. This result is consistent with AsFlFFF results on the same suspension without centrifugation. The detection of next nearest Fe and O atoms were consistent with the structure of goethite, ruling out incorporation within hematite. After centrifugation of the suspension, only nanoparticulate needle-like particles, very likely goethite, could be detected in the supernatant by ESEM. AsFlFFF data of the supernatant were comparable to that obtained for the homogeneous suspension, whereas XAS indicated that Lu(III) is predominantly present as dissolved species in the supernatant. Results from both techniques can be interpreted as a major fraction of Lu present as aqueous ions and a minor fraction as structurally incorporated. Findings from this study are corroborated by STEM-HAADF data and results from DFT calculations in a companion paper.
Show more [+] Less [-]Geochemical behaviour of dissolved trace elements in a monsoon-dominated tropical river basin, Southwestern India
2014
The study presents a 3-year time series data on dissolved trace elements and rare earth elements (REEs) in a monsoon-dominated river basin, the Nethravati River in tropical Southwestern India. The river basin lies on the metamorphic transition boundary which separates the Peninsular Gneiss and Southern Granulitic province belonging to Archean and Tertiary–Quaternary period (Western Dharwar Craton). The basin lithology is mainly composed of granite gneiss, charnockite and metasediment. This study highlights the importance of time series data for better estimation of metal fluxes and to understand the geochemical behaviour of metals in a river basin. The dissolved trace elements show seasonality in the river water metal concentrations forming two distinct groups of metals. First group is composed of heavy metals and minor elements that show higher concentrations during dry season and lesser concentrations during the monsoon season. Second group is composed of metals belonging to lanthanides and actinides with higher concentration in the monsoon and lower concentrations during the dry season. Although the metal concentration of both the groups appears to be controlled by the discharge, there are important biogeochemical processes affecting their concentration. This includes redox reactions (for Fe, Mn, As, Mo, Ba and Ce) and pH-mediated adsorption/desorption reactions (for Ni, Co, Cr, Cu and REEs). The abundance of Fe and Mn oxyhydroxides as a result of redox processes could be driving the geochemical redistribution of metals in the river water. There is a Ce anomaly (Ce/Ce*) at different time periods, both negative and positive, in case of dissolved phase, whereas there is positive anomaly in the particulate and bed sediments. The Ce anomaly correlates with the variations in the dissolved oxygen indicating the redistribution of Ce between particulate and dissolved phase under acidic to neutral pH and lower concentrations of dissolved organic carbon. Unlike other tropical and major world rivers, the effect of organic complexation on metal variability is negligible in the Nethravati River water.
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