Better understanding and applications of ammonium 12-molybdophosphate-based diffusive gradient in thin film techniques for measuring Cs in waters
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This study deals with further and systematic laboratory evaluation of the already known ammonium 12-molybdophosphate (AMP)-diffusive gradient in thin film (DGT) method, which is used for measuring total Cs concentration in environmental waters. This study confirms that the AMP-binding gel is not stable for pH > 6. In order to reveal a potential impact of AMP degradation on DGT application, time-series experiments were performed by deploying AMP-DGT samplers in Cs-doped moderately basic soft and hard water up to total AMP-binding gel degradation (60 and 175 h of deployment time, respectively). Linear accumulation of Cs by AMP-DGT samplers was observed up to 48 and 58 h in hard and soft waters, respectively. For this deployment time range, AMP-DGT measured over 77 ± 10 and 94 ± 16% of total Cs concentration in hard and soft water, respectively. The difference in DGT response was attributed to Ca2+ and Mg2+ competition reducing the uptake of AMP-DGT samplers in hard water. Shrinkage of agarose-polyacrylamide diffusive gel was experimentally observed only in hard water due to more intensive AMP-binding gel degradation in hard water. Even if the AMP-DGT response was not impacted in this study, it is recommended to use agarose hydrogel as standard diffusive gel. Based on the experience obtained from this detailed validation process, the authors propose a number of key requirements that need to be considered when developing DGT devices, with testing the performance over longer deployment times being critical.
KeywordsCesium Diffusive gradient in thin film (DGT) technique Binding gel stability Time-series accumulation Laboratory validation AMP degradation
Dr. Charlotte Cazala is gratefully acknowledged for her reading of the paper. Dr. Valérie Buard is also gratefully thanked for her help on the thickness measurement of diffusive gel with the optical microscope of laboratory LRMed (IRSN). This is PATERSON contribution 3.
This work has been supported by the ANR (French National Research Agency), under the “Investissement d’Avenir” framework program (number ANR-11-RSNR-0002).
- Bennett WW, Arsic M, Panther JG, Welsh DT, Teasdale PR (2016) Chapter 4 binding layer properties. In: Davison W (ed) Diffusive gradients in thin-films for environmental measurements. Cambridge environmental chemistry series. Cambridge University Press, Cambridge, pp 66–92Google Scholar
- Cambray RS, Cawse P, Garland J, Gibson JAB, Johnson P, Lewis G, Newton D, Salmon L, Wade B (1987) Observations on radioactivity from the Chernobyl accident. Nucl Energy 26:77–101Google Scholar
- Chang L-Y (1998) Development and application of diffusive gradients in thin-films (DGT) for the measurement of stable and radioactive caesium and strontium in surface waters, University of Lancaster, p. 227 ppGoogle Scholar
- Coughtrey P, Jackson D, Thorne M (1985) Radionuclide distribution and transport in terrestrial and aquatic ecosystems. A compendium of data, vol. 6. Balkema. AA Publishers, Rotterdam, The NetherlandsGoogle Scholar
- Eyrolle-Boyer F, Boyer P, Garcia-Sanchez L, Métivier J-M, Onda Y, De Vismes A, Cagnat X, Boulet B, Cossonnet C (2016) Behaviour of radiocaesium in coastal rivers of the Fukushima Prefecture (Japan) during conditions of low flow and low turbidity—insight on the possible role of small particles and detrital organic compounds. J Environ Radioact 151:328–340CrossRefGoogle Scholar
- Gonze M, Mourlon C, Calmon P, Manach E, Debayle C, Gurriaran R, Baccou J (2016): Assessment study of ambient dose rates dynamics in the Fukushima terrestrial regionGoogle Scholar
- Iwamoto R, Grimblot J (1999) Influence of phosphorus on the properties of alumina-based hydrotreating catalysts. Adv Catal 44:417–503Google Scholar
- Jolley DF, Mason S, Gao Y, Zhang H (2016) Practicalities of working with DGT. In: Davison W (Editor), Diffusive gradients in thin-films for environmental measurements. Cambridge environmental chemistry series. Cambridge University Press, Cambridge, pp. 263–290Google Scholar
- Matsunaga T, Nakanishi T, Atarashi-Andoh M, Takeuchi E, Muto K, Tsuduki K, Nishimura S, Koarashi J, Otosaka S, Sato T, Miyata Y, Nagao S (2016) Year-round variations in the fluvial transport load of particulate 137Cs in a forested catchment affected by the Fukushima Daiichi Nuclear Power Plant accident. J Radioanal Nucl Chem 310:679–693CrossRefGoogle Scholar
- Nagao S, Kanamori M, Ochiai S, Suzuki K, Yamamoto M (2014) Dispersion of Cs-134 and Cs-137 in river waters from Fukushima and Gunma prefectures at nine months after the Fukushima Daiichi NPP accident. J Nucl Sci Technol 4:13Google Scholar
- Parkhurst DL, Appelo C (2013) Description of input and examples for PHREEQC version 3: a computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations. 2328–7055, US Geological SurveyGoogle Scholar
- Povinec PP, Hirose K, Aoyama M (2013) Fukushima accident: radioactivity impact on the environment. NewnesGoogle Scholar
- Tsigdinos GA (1978): Heteropoly compounds of molybdenum and tungsten, Topics in current chemistry. Springer, pp. 1–64Google Scholar
- van Veen JR, Sudmeijer O, Emeis CA, de Wit H (1986) On the identification of molybdophosphate complexes in aqueous solution. J Chem Soc Dalton Trans:1825–1831Google Scholar
- Yasutaka T, Kawabe Y, Kurosawa A, Komai T (2013) Proceedings of the international symposium on environmental monitoring and dose estimation of residents after accident of TEPCO’s Fukushima Daiichi Nuclear Power Stations, Japan, pp 230Google Scholar