Traitement d'effluents radioactifs par procédés membranaires : Positionnement de l'Osmose inverse (thèse: 2013 - 2016)
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Publications scientifiques au M2P2
2017
Nicolas Combernoux, L. Schrive, V. Labed, Yvan Wyart, Emilie Carretier, et al.. Treatment of radioactive liquid effluents by reverse osmosis membranes: From lab-scale to pilot-scale. Water today, 2017, 123, pp.311-320. ⟨10.1016/j.watres.2017.06.062⟩. ⟨hal-01656412⟩ Plus de détails...
The recent use of the reverse osmosis (RO) process at the damaged Fukushima-Daiichi nuclear power plant generated a growing interest in the application of this process for decontamination purposes. This study focused on the development of a robust RO process for decontamination of two kinds of liquid effluents: a contaminated groundwater after a nuclear disaster and a contaminated seawater during a nuclear accident. The SW30 HR membrane was selected among other in this study due to higher retentions (96% for Cs and 98% for Sr) in a true groundwater. Significant fouling and scaling phenomenon, attributed to calcium and strontium precipitation, were evidenced in this work: this underscored the importance of the lab scale experiment in the process. Validation of the separation performances on trace radionuclides concentration was performed with similar retention around 96% between surrogates Cs (inactive) and 137Cs (radioactive). The scale up to a 2.6 m2 spiral wound membrane led to equivalent retentions (around 96% for Cs and 99% for Sr) but lower flux values: this underlined that the hydrodynamic parameters (flowrate/cross-flow velocity) should be optimized. This methodology was also applied on the reconstituted seawater effluent: retentions were slightly lower than for the groundwater and the same hydrodynamic effects were observed on the pilot scale. Then, ageing of the membrane through irradiation experiments were performed. Results showed that the membrane active layer composition influenced the membrane resistance towards γ irradiation: the SW30 HR membrane performances (retention and permeability) were better than the Osmonics SE at 1 MGy. Finally, to supplement the scale up approach, the irradiation of a spiral wound membrane revealed a limited effect on the permeability and retention. This indicated that irradiation conditions need to be controlled for a further development of the process.
Nicolas Combernoux, L. Schrive, V. Labed, Yvan Wyart, Emilie Carretier, et al.. Treatment of radioactive liquid effluents by reverse osmosis membranes: From lab-scale to pilot-scale. Water today, 2017, 123, pp.311-320. ⟨10.1016/j.watres.2017.06.062⟩. ⟨hal-01656412⟩
Nicolas Combernoux, Luc Schrive, Véronique Labed, Yvan Wyart, Emilie Carretier, et al.. Irradiation effects on RO membranes: Comparison of aerobic and anaerobic conditions. Polymer Degradation and Stability, 2016, 134, pp.126-135. ⟨10.1016/j.polymdegradstab.2016.09.034⟩. ⟨hal-01461790⟩ Plus de détails...
In this study, the investigation of the degradation of polyamide composite reverse osmosis membrane under gamma irradiation was carried out in aerobic and anaerobic conditions. A gamma Co-60 source was used to reach irradiation doses ranging from 0.1 to 1 MGy, with a constant dose rate of 0.5 kGy h(-1). The RO membranes degradation was assessed using XPS and ATR-FTIR for the chemical modification of the membrane active layer. Ion chromatography, pH measurement and gas chromatography were also used to identify and quantify the species release in aqueous and gaseous phases. Results showed a difference in the degradation of the membrane active layer and support layer between aerobic and anaerobic conditions. The different analysis performed suggested that the breakage of amide bonds was significantly higher in aerobic conditions rather than in anaerobic. This observation was confirmed by the measurement of an increasing amount of release species in aqueous and gaseous phase in aerobic conditions. Ester bonds scissions were highlighted as soon as the dose reached the value of 0.1 MGy in both conditions indicating an important sensitivity of the PVA-type coating of the RO membrane towards irradiation. Nevertheless, investigation of the top 10 nm surface of the active layer composition by XPS showed that the scissions of amide and ester bonds were similar in both conditions. Finally, all these results underlined a difference in the degradation mechanisms of the RO membranes: in anaerobic conditions, the degradation was limited to the top surface of the membrane and reductive species were involved in the degradation reactions. (C) 2016 Elsevier Ltd. All rights reserved.
Nicolas Combernoux, Luc Schrive, Véronique Labed, Yvan Wyart, Emilie Carretier, et al.. Irradiation effects on RO membranes: Comparison of aerobic and anaerobic conditions. Polymer Degradation and Stability, 2016, 134, pp.126-135. ⟨10.1016/j.polymdegradstab.2016.09.034⟩. ⟨hal-01461790⟩
Nicolas Combernoux, Véronique Labed, Luc Schrive, Yvan Wyart, Emilie Carretier, et al.. Effect of gamma irradiation at intermediate doses on the performance of reverse osmosis membranes. International Journal for Radiation Physics and Chemistry, 2015, ⟨10.1016/j.radphyschem.2015.11.017⟩. ⟨hal-01294902⟩ Plus de détails...
The goal of this study is to explain the degradation of Polyamide (PA) composite reverse osmosis membrane (RO) in function of the irradiation dose. Irradiations were performed with a gamma 60Co source in wet conditions and under oxygen atmosphere. For different doses of 0.2 and 0.5 MGy with a constant dose rate of 0.5 kGy h−1, RO membranes performances (NaCl retention, permeability) were studied before and after irradiation. ATR-FTIR, ion chromatography and gas chromatography were used to characterize structural modification. Results showed that the permeability of RO membranes irradiated at 0.2 MGy exhibited a small decrease, related to scissions of the PVA coating. However, retention did not change at this dose. At 0.5 MGy, permeability showed a large increase of a factor around 2 and retention began to decrease from 99% to 95%. Chromatography measurements revealed a strong link between permselectivity properties variation, ion leakage and oxygen consumption. Add to ATR-FTIR observations, these results emphasized that the cleavages of amide and ester bonds were observed at 0.5 MGy, more precisely the loss of hydrogen bonds between polyamide chains. By different analysis, modifications of the polysulfone layer occur until a dose of 0.2 MGy.
Nicolas Combernoux, Véronique Labed, Luc Schrive, Yvan Wyart, Emilie Carretier, et al.. Effect of gamma irradiation at intermediate doses on the performance of reverse osmosis membranes. International Journal for Radiation Physics and Chemistry, 2015, ⟨10.1016/j.radphyschem.2015.11.017⟩. ⟨hal-01294902⟩
Journal: International Journal for Radiation Physics and Chemistry
Nicolas Combernoux, Luc Schrive, Véronique Labed, Yvan Wyart, Emilie Carretier, et al.. Study of polyamide composite reverse osmosis membrane degradation in water under gamma rays. Journal of Membrane Science, 2015, 480 (2), pp.64-73. ⟨10.1016/j.memsci.2015.01.019⟩. ⟨hal-01295140⟩ Plus de détails...
This study aims to investigate the impact of irradiation on the behavior of Polyamide (PA) composite reverse osmosis (RO) membranes. Irradiations were performed for two doses (0.1 and 1 MGy) in wet conditions under an oxygen atmosphere, with a gamma 60Co source. Irradiation effect on RO membranes performances (NaCl rejection, permeability) was studied before and after irradiation. ATR-FTIR, XPS, AFM, FESEM microscopy, ion chromatography were also used to characterize structural modifications. Results show that NaCl rejection of RO membranes irradiated at 1 MGy decreased until 64% and permeability increased by a factor of three. Nevertheless, membranes irradiated at 0.1 MGy did not exhibit any change in theirs permselectivity properties. Advanced analysis techniques confirmed that the firsts effects of gamma rays on RO membranes occurred between 0.1 and 1 MGy. Results emphasize that gamma rays effects on the RO membranes led to the breaking of amide and ester bonds at 1 MGy. These breakings resulted in loss of hydrogen bonds between polyamide chains, and consequently to a relaxation of the polyamide network. Finally, modifications of the polysulfone layer underneath were highlighted. Both relaxation of the polyamide network and modifications of the polysulfone layer could be involved in the drop of the permselectivity properties.
Nicolas Combernoux, Luc Schrive, Véronique Labed, Yvan Wyart, Emilie Carretier, et al.. Study of polyamide composite reverse osmosis membrane degradation in water under gamma rays. Journal of Membrane Science, 2015, 480 (2), pp.64-73. ⟨10.1016/j.memsci.2015.01.019⟩. ⟨hal-01295140⟩
