Impact of dam flushing operations on sediment dynamics and quality in the upper Rhône River, France.

The Rhône River (France) has been used for energy production for decades and 21 dams have been built. To avoid problems due to sediment storage, dam flushing operations are periodically organized. The impacts of such operations on suspended particulate matter (SPM) dynamics (resuspension and fluxes) and quality (physico-chemical characteristics and contamination), were investigated during a flushing operation performed in June 2012 on 3 major dams from the Upper Rhône River. The concentrations of major hydrophobic organic contaminants (polychlorinated biphenyls, polycyclic aromatic hydrocarbons - PAHs, bis(2-ethylhexyl)phthalate [DEHP] and 4-n-nonylphenol), trace metal elements, particulate organic carbon (POC) and particle size distribution were measured on SPM samples collected during this event as well as on those obtained from 2011 to 2016 at a permanent monitoring station (150 km downstream). This allows to compare the SPM and contaminant concentrations and fluxes during the 2012 dam flushing operations with those during flood events and baseflow regime. At equal water discharge, mean SPM concentrations during flushing were on average 6-8 times higher than during flood events recorded from 2011 to 2016. While of short duration (19 days), the flushing operations led to the resuspension of SPM and contributed to a third of the mean annual SPM flux. The SPM contamination was generally lower during flushing than during baseflow or flood, probably due to the fact that flushing transports SPM only issued from resuspended sediment, with no autochtonous particles nor eroded soil. The only exception are PAHs and DEHP with higher concentrations during flushing, which must be issued from the resuspension of legacy-contaminated sediments stored behind the dams before the implementation of emission regulations. During flushing, the variations of POC and contaminant concentrations are also mostly driven by particle size. Finally, we propose a list of recommendations for the design of an adequate monitoring network to evaluate the impact of dam flushing operations on large river systems.

U isotopes distribution in the Lower Rhone River and its implication on radionuclides disequilibrium within the decay series.

The large rivers are main pathways for the delivery of suspended sediments into coastal environments, affecting the biogeochemical fluxes and the ecosystem functioning. The radionuclides from 238U and 232Th-series can be used to understand the dynamic processes affecting both catchment soil erosion and sediment delivery to oceans. Based on annual water discharge the Rhone River represents the largest river of the Mediterranean Sea. The Rhone valley also represents the largest concentration in nuclear power plants in Europe. A radioactive disequilibrium between particulate 226Ra(p) and 238U(p) was observed in the suspended sediment discharged by the Lower Rhone River (Eyrolle et al. 2012), and a fraction of particulate 234Th was shown to derive from dissolved 238U(d) (Zebracki et al. 2013). This extensive study has investigated the dissolved U isotopes distribution in the Lower Rhone River and its implication on particulate radionuclides disequilibrium within the decay series. The suspended sediment and filtered river waters were collected at low and high water discharges. During the 4-months of the study, two flood events generated by the Rhone southern tributaries were monitored. In river waters, the total U(d) concentration and U isotopes distribution were obtained through Q-ICP-MS measurements. The Lower Rhone River has displayed non-conservative U-behavior, and the variations in U(d) concentration between southern tributaries were related to the differences in bedrock lithology. The artificially occurring 236U was detected in the Rhone River at low water discharges, and was attributed to the liquid releases from nuclear industries located along the river. The (235U/238U)(d) activity ratio (=AR) in river waters was representative of the 235U natural abundance on Earth. The (226Ra/238U)(p) AR in suspended sediment has indicated a radioactive disequilibrium (average 1.3 ± 0.1). The excess of 234Th in suspended sediment =(234Thxs(p)) was apparent solely at low water discharges. The activity of 234Thxs(p) was calculated through gamma measurements and ranged from unquantifiable to 56 ± 14 Bq kg-1. The possibility of using 234Th as a tracer for the suspended sediment dynamics in large Mediterranean river was then discussed.

Tritium and 14C background levels in pristine aquatic systems and their potential sources of variability.

Tritium and (14)C are currently the two main radionuclides discharged by nuclear industry. Tritium integrates into and closely follows the water cycle and, as shown recently the carbon cycle, as does (14)C (Eyrolle-Boyer et al., 2014a, b). As a result, these two elements persist in both terrestrial and aquatic environments according to the recycling rates of organic matter. Although on average the organically bound tritium (OBT) activity of sediments in pristine rivers does not significantly differ today (2007-2012) from the mean tritiated water (HTO) content on record for rainwater (2.4 ± 0.6 Bq/L and 1.6 ± 0.4 Bq/L, respectively), regional differences are expected depending on the biomass inventories affected by atmospheric global fallout from nuclear testing and the recycling rate of organic matter within watersheds. The results obtained between 2007 and 2012 for (14)C show that the levels varied between 94.5 ± 1.5 and 234 ± 2.7 Bq/kg of C for the sediments in French rivers and across a slightly higher range of 199 ± 1.3 to 238 ± 3.1 Bq/kg of C for fish. This variation is most probably due to preferential uptake of some organic carbon compounds by fish restraining (14)C dilution with refractory organic carbon and/or with old carbonates both depleted in (14)C. Overall, most of these ranges of values are below the mean baseline value for the terrestrial environment (232.0 ± 1.8 Bq/kg of C in 2012, Roussel-Debet, 2014a) in relation to dilution by the carbonates and/or fossil organic carbon present in aquatic systems. This emphasises yet again the value of establishing regional baseline value ranges for these two radionuclides in order to account for palaeoclimatic and lithological variations. Besides, our results obtained from sedimentary archive investigation have confirmed the delayed contamination of aquatic sediments by tritium from the past nuclear tests atmospheric fallout, as recently demonstrated from data chronicles (Eyrolle-Boyer et al., 2014a,b). Thus Sedimentary archives can be successfully used to reconstruct past (14)C and OBT levels. Additionally, sediment repositories potentially represent significant storages of OBT that may account for in case of further remobilisation. We finally show that floods can significantly affect the OBT and (14)C levels within suspended particles or sediments depending on the origin of particles reinforcing the need to acquire baseline value range at a regional scale.

Tracing the origin of suspended sediment in a large Mediterranean river by combining continuous river monitoring and measurement of artificial and natural radionuclides.

Delivery of suspended sediment from large rivers to marine environments has important environmental impacts on coastal zones. In France, the Rhone River (catchment area of 98,000 km(2)) is by far the main supplier of sediment to the Mediterranean Sea and its annual solid discharge is largely controlled by flood events. This study investigates the relevance of alternative and original fingerprinting techniques based on the relative abundances of a series of radionuclides measured routinely at the Rhone River outlet to quantify the relative contribution of sediment supplied by the main tributaries during floods. Floods were classified according to the relative contribution of the main subcatchments (i.e., Oceanic, Cevenol, extensive Mediterranean and generalised). Between 2000 and 2012, 221 samples of suspended sediment were collected at the outlet and were shown to be representative of all flood types that occurred during the last decade. Three geogenic radionuclides (i.e., (238)U, (232)Th and (40)K) were used as fingerprints in a multivariate mixing model in order to estimate the relative contribution of the main subcatchment sources-characterised by different lithologies-in sediment samples collected at the outlet. Results showed that total sediment supply originating from Pre-Alpine, Upstream, and Cevenol sources amounted to 10, 7 and 2.10(6)tons, respectively. These results highlight the role of Pre-Alpine tributaries as the main sediment supplier (53%) to the Rhone River during floods. Other fingerprinting approaches based on artificial radionuclide activity ratios (i.e., (137)Cs/(239+240)Pu and (238)Pu/(239+240)Pu) were tested and provided a way to quantify sediment remobilisation or the relative contributions of the southern tributaries. In the future, fingerprinting methods based on natural radionuclides should be further applied to catchments with heterogeneous lithologies. Methods based on artificial radionuclides should be further applied to catchments characterised by heterogeneous post-Chernobyl (137)Cs deposition or by specific releases of radioactive effluents.