Mobility of Radionuclides in Fractured Carbonate Rocks: Lessons from a Field-Scale Transport Experiment

Tran, Emily; Reimus, Paul W.; Klein-BenDavid, Ofra; Teutsch, Nadya; Zavarin, Mavrik; Kersting, Annie B.; Weisbrod, Noam

doi:10.1021/acs.est.0c03008

Cited by 12 publications

(8 citation statements)

References 57 publications

(112 reference statements)

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“…Several physicochemical mechanisms have previously been considered and observed for the transport behavior of transuranic actinide isotopes in the environment. Such mechanisms include solution complexation to small inorganic ions, ,,,- complexation to small water-soluble organic chelators, - sorption onto mineral phases, ,, ion exchange with clay minerals, , as well as colloid-mediated transport. ,,, Given the growing inventory of spent nuclear fuel worldwide , and the necessity to understand, model, and predict the behavior of radiotoxic elements over thousands of years, it is imperative to be aware of the full range of mechanisms that may influence the environmental behavior of actinides. In this context, the recent discovery of the natural lanthanide-binding protein LanM in M.…”

Section: Environmental Implicationsmentioning

confidence: 99%

Impact of a Biological Chelator, Lanmodulin, on Minor Actinide Aqueous Speciation and Transport in the Environment

Deblonde,

Morrison,

Mattocks

et al. 2023

Environ. Sci. Technol.

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Minor actinides are major contributors to the long-term radiotoxicity of nuclear fuels and other radioactive wastes. In this context, understanding their interactions with natural chelators and minerals is key to evaluating their transport behavior in the environment. The lanmodulin family of metalloproteins is produced by ubiquitous bacteria and Methylorubrum extorquens lanmodulin (LanM) was recently identified as one of nature’s most selective chelators for trivalent f-elements. Herein, we investigated the behavior of neptunium, americium, and curium in the presence of LanM, carbonate ions, and common minerals (calcite, montmorillonite, quartz, and kaolinite). We show that LanM’s aqueous complexes with Am(III) and Cm(III) remain stable in carbonate-bicarbonate solutions. Furthermore, the sorption of Am(III) to these minerals is strongly impacted by LanM, while Np(V) sorption is not. With calcite, even a submicromolar concentration of LanM leads to a significant reduction in the Am(III) distribution coefficient (K d, from >104 to ∼102 mL/g at pH 8.5), rendering it even more mobile than Np(V). Thus, LanM-type chelators can potentially increase the mobility of trivalent actinides and lanthanide fission products under environmentally relevant conditions. Monitoring biological chelators, including metalloproteins, and their biogenerators should therefore be considered during the evaluation of radioactive waste repository sites and the risk assessment of contaminated sites.

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Section: Environmental Implicationsmentioning

confidence: 99%

Impact of a Biological Chelator, Lanmodulin, on Minor Actinide Aqueous Speciation and Transport in the Environment

Deblonde,

Morrison,

Mattocks

et al. 2023

Environ. Sci. Technol.

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“…Carbonate skeletons also preserve information about life histories (Gerringer et al, 2018;Mat et al, 2020;Posenato et al, 2022), ecological relationships between organisms (Fagerstrom, 1987;Mourguiart and Carbonel, 1994;Valchev, 2003), and past human interrelations (Gutieŕrez-Zugasti, 2011;Haour et al, 2016;Burchell et al, 2018). Furthermore, the contribution of calcifiers (organisms that mineralize calcium carbonate) to the rock record is of great commercial interest, for example for the extraction of building materials, as source rocks for water and hydrocarbons and as a storage rock for CO 2 (Hanshaw and Back, 1979;Izgec et al, 2008;Benavente et al, 2018;Tran et al, 2020).…”

Section: Introductionmentioning

confidence: 99%

Tracing timing of growth in cultured molluscs using strontium spiking

et al. 2023

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IntroductionGrowth experiments present a powerful tool for determining the effect of environmental parameters on growth and carbonate composition in biogenic calcifiers. For successful proxy calibration and biomineralization studies, it is vital to identify volumes of carbonate precipitated by these organisms at precise intervals during the experiment. Here, we investigate the use of strontium labelling in mollusc growth experiments.MethodsThree bivalve species (Cerastoderma edule, Mytilus edulis and Ostrea edulis) were grown under monitored field conditions. The bivalves were regularly exposed to seawater with elevated concentrations of dissolved strontium chloride (SrCl2). In addition, the size of their shells was determined at various stages during the experiment using calliper measurements and digital photography. Trace element profiles were measured in cross sections through the shells of these molluscs using laser ablation ICPMS and XRF techniques.ResultsOur results show that doses of dissolved strontium equivalent to 7-8 times the background marine value (~0.6 mmol/L) are sufficient to cause reproducible peaks in shell-incorporated strontium in C. edule and M. edulis shells. No negative effects were observed on shell calcification rates. Lower doses (3-5 times background values) resulted in less clearly identifiable peaks, especially in M. edulis. Strontium spiking labels in shells of O. edulis are more difficult to detect, likely due to their irregular growth.DiscussionStrontium spiking is a useful technique for creating time marks in cultured shells and a reproducible way to monitor shell size during the growing season while limiting physical disturbance of the animals. However, accurate reconstructions of growth rates at high temporal resolution require frequent spiking with high doses of strontium.

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“…It is also possible to reconstruct life histories (Gerringer et al, 2018;Mat et al, 2020;Posenato et al, 2022), ecological relationships between organisms (Fagerstrom, 1987;Mourguiart and Carbonel, 1994;Valchev, 2003), and past human interrelations (Gutiérrez-Zugasti, 2011;Haour et al, 2016;Burchell et al, 2018). The contribution of calcifiers (organisms that mineralize calcium carbonate) to the rock record is also of great commercial interest, for example for the extraction of building materials, as source rocks for water and hydrocarbons and as a storage rock for CO 2 (Hanshaw and Back, 1979;Izgec et al, 2008;Benavente et al, 2018;Tran et al, 2020).…”

Section: Introductionmentioning

confidence: 99%

Tracing timing of growth in cultured mollusks using strontium spiking

Winter¹,

Sikkeleras²,

Goudsmit-Hazevoort³

et al. 2022

Preprint

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Growth experiments present a powerful tool for determining the effect of environmental parameters on growth and carbonate composition in biogenic calcifiers. For successful proxy calibration and biomineralization studies, it is vital to exactly identify volumes of carbonate precipitated at precise intervals during the experiment. Here, we investigate the use of strontium labelling in mollusk growth experiments. Three bivalve species (C. edule, M. edulis and O. edulis) were grown under monitored field conditions. The bivalves were regularly exposed to seawater with elevated concentrations of dissolved strontium. In addition, the size of the shells was determined at various stages during the experiment using calliper measurements and digital photography. Trace element profiles were measured in cross sections through the shells of these mollusks using laser ablation ICP-MS and XRF techniques. Our results show that doses of dissolved strontium equivalent to 7-8 times the background marine value are sufficient to produce reproducible peaks in shell incorporated strontium in C. edule and M. edulis shells. No negative effects were observed on shell calcification rates. Lower doses (3-5 times background values) resulted in less clearly identifiable peaks, especially in M. edulis. Strontium spiking labels in shells of O. edulis are more difficult to detect, likely due to their irregular growth. Nevertheless, strontium spiking seems a useful technique for creating time marks in cultured shells and a reproducible way to monitor shell height along the growing season while limiting physical disturbance of the animals. However, accurate reconstructions of growth rates at high time resolution require frequent spiking with high doses of strontium.

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Mobility of Radionuclides in Fractured Carbonate Rocks: Lessons from a Field-Scale Transport Experiment

Cited by 12 publications

References 57 publications

Impact of a Biological Chelator, Lanmodulin, on Minor Actinide Aqueous Speciation and Transport in the Environment

Impact of a Biological Chelator, Lanmodulin, on Minor Actinide Aqueous Speciation and Transport in the Environment

Tracing timing of growth in cultured molluscs using strontium spiking

Tracing timing of growth in cultured mollusks using strontium spiking

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