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In situ speciation measurements and bioavailability determination of plutonium in natural waters of a karst system using diffusion in thin film technique (DGT)

Applicant Froidevaux Pascal
Number 140230
Funding scheme Project funding (Div. I-III)
Research institution Institut de Radiophysique Département de Radiologie Université de Lausanne/CHUV
Institution of higher education University of Lausanne - LA
Main discipline Geochemistry
Start/End 01.10.2012 - 30.09.2015
Approved amount 188'488.00
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All Disciplines (3)

Discipline
Geochemistry
Hydrology, Limnology, Glaciology
Environmental Research

Keywords (9)

bioavailability; karst; dissolved organic matter; colloidal transport; speciation; plutonium; bryophytes; diffusion in thin film (DGT); sf-ICP-MS

Lay Summary (English)

Lead
Lay summary

We propose a field study of the speciation and bioavailability of plutonium in freshwater using the novel techniques of diffusion in thin film of labile species of metal ions. After a calibration of the method in the laboratory it will be applied in two sites of a karst system in the Swiss Jura Mountains (a spring and a brook).

Our goal is a broad understanding of the speciation of plutonium in two chemically different environments (a mineral spring and an organic-rich brook) of a karst region in the Jura Mountains, Switzerland. Speciation will be carried out using the determination of labile species by DGT experiments. Colloidal fractions will be determined by ultra-filtration experiments. The focus of the study will be on the plutonium determination by sensitive sf-ICP-MS on the DGT and colloidal fractions of the studied waters. Together, the determination of labile (DGT) and colloidal plutonium will allow constructing a realistic model of plutonium speciation. We are particularly interested in the bioavailable fraction that could be taken up by mosses, which were shown in a previous study to accumulate plutonium in an intra-cellular compartment.

As most significant outcomes of this study we expect:

  • The determination of the diffusion coefficient in APA-gel for plutonium. With this calibration, the DGT technique will be available for a wide range of future plutonium studies.
  • The determination of the labile fraction of plutonium in freshwaters, one with a low content of DOM, one with a high content of DOM.
  • A better understanding of the accumulation of plutonium in the intra-cellular fraction of mosses.
  • The integration of all measured parameters into a suitable speciation model (e.g. WHAM model, (Tipping, 1994), which will allow to improve the understanding of 239Pu uptake and toxicity in the biosphere.

 

The significance of this study is beyond the freshwaters of the karst of the Jura Mountains, which will serve as a model of many other freshwaters. This work will contribute to our understanding of the mobility of plutonium in the environment and its toxicity for the biota.

Direct link to Lay Summary Last update: 21.02.2013

Responsible applicant and co-applicants

Employees

Publications

Publication
Evidence of plutonium bioavailability in pristine freshwaters of a karst system of the Swiss Jura Mountains
Cusnir Ruslan, Christl Marcus, Steinmann Philipp Bochud François, Froidevaux Pascal (2017), Evidence of plutonium bioavailability in pristine freshwaters of a karst system of the Swiss Jura Mountains, in Geochimica et Cosmochimica Acta, 206, 30-39.
Probing the Kinetic Parameters of Plutonium−Naturally Occurring Organic Matter Interactions in Freshwaters Using the Diffusive Gradients in Thin Films Technique
Ruslan Cusnir Maud Jaccard Claude Bailat Marcus Christl Philipp Steinmann Max Haldimann, Francois Bochud and Pascal Froidevaux (2016), Probing the Kinetic Parameters of Plutonium−Naturally Occurring Organic Matter Interactions in Freshwaters Using the Diffusive Gradients in Thin Films Technique, in Environmental Science and Technology, 50(10), 5103-5110.
A DGT Technique for Plutonium Bioavailability Measurements
Cusnir Ruslan, Steinmann Philipp, Bochud Francois, Froidevaux Pascal (2014), A DGT Technique for Plutonium Bioavailability Measurements, in ENVIRONMENTAL SCIENCE & TECHNOLOGY, 48(18), 10829-10834.
Speciation and bioavailability measurements of environmental plutonium using diffusion in thin films
Cusnir Ruslan, Steinmann Philipp, Christl Marcus, Bochud François, Froidevaux Pascal, Speciation and bioavailability measurements of environmental plutonium using diffusion in thin films, in Journal of Visualized Experiment, 105.

Collaboration

Group / person Country
Types of collaboration
Laboratory of Ion Beam Physics/ ETHZ Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
International Conference on Radioecology and Environmental Radioactivity Talk given at a conference Development of the DGT Technique for in-situ Pu Speciation Measurements 08.09.2014 Barcelona, Spain Cusnir Ruslan;
Conference on DGT and the Environment Poster Development of the DGT Technique for Pu Speciation Measurements 08.07.2013 Lancaster, Great Britain and Northern Ireland Cusnir Ruslan;


Associated projects

Number Title Start Funding scheme
175492 Development and application of diffusive gradients in thin films (DGT) and cross-flow ultrafiltration techniques for determining actinides (Pu, Am, U) speciation and availability at a marine site contaminated by the Sellafield (UK) nuclear discharges 01.10.2018 Project funding (Div. I-III)

Abstract

We propose a field study of the speciation and bioavailability of plutonium in freshwater using the novel techniques of diffusion in thin film of labile species of metal ions. After a calibration of the method in the laboratory it will be applied in two sites of a karst system in the Swiss Jura Mountains (a spring and a brook).Our goal is a broad understanding of the speciation of plutonium in two chemically different environments (a mineral spring and a organic-rich brook) of the karst of the Jura Mountains. Speciation will be carried out using the determination of labile species by DGT experiments. Colloidal fractions will be determined by ultra-filtration experiments. The focus of the study will be on the plutonium determination by sensitive sf-ICP-MS on the DGT and colloidal fractions of the spring waters. Together, the determination of labile (DGT) and colloidal plutonium will allow constructing a realistic model of plutonium speciation. We are particularly interested in the bioavailable fraction that could be taken up by mosses, which were shown in a previous study to accumulate plutonium in an intra-cellular compartment. As most significant outcomes of this study we expect:• The determination of the diffusion coefficient in APA-gel for plutonium. With this calibration the DGT technique will be available for a wide range of future Pu studies.• The determination of the labile fraction of plutonium in freshwaters, one with a low content of DOM, one with a high content of DOM.• A better understanding of the accumulation of plutonium in the intra-cellular fraction of mosses.• The integration of all measured parameters into a suitable speciation model (e.g. WHAM model, (Tipping, 1994), which will allow to improve the understanding of 239Pu uptake and toxicity in the biosphere. The significance of this study is beyond the freshwaters of the karst of the Jura Mountains, which will serve as a model of many other freshwaters. This work will contribute to our understanding of the mobility of plutonium in the environment and its toxicity for the biota.
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