Hydro-climatic drivers of land-based organic and inorganic particulate micropollutant fluxes: The regime of the largest river water inflow of the Mediterranean Sea.

Land-based micropollutants are the largest pollution source of the marine environment acting as the major large-scale chemical sink. Despite this, there are few comprehensive datasets for estimating micropollutant fluxes released to the sea from river mouths. Hence, their dynamics and drivers remain poorly understood. Here, we address this issue by continuous measurements throughout the Rhône River basin (∼100,000 km2) of 1) particulate micropollutant concentrations (persistant organic micropollutants: polychlorobiphenyls [PCBi] and polycyclic aromatic hydrocarbons [PAHs]; emerging compounds: glyphosate and aminomethylphosphonic acid [AMPA]; and trace metal elements [TME]), 2) suspended particulate matter [SPM], and 3) water discharge. From these data, we computed daily fluxes for a wide range of micropollutants (n = 29) over a long-term period (2008-2018). We argue that almost two-thirds of annual micropollutant fluxes are released to the Mediterranean Sea during three short-term periods over the year. The watershed hydro-climatic heterogeneity determines this dynamic by triggering seasonal floods. Unexpectedly, the large deficit of the inter-annual monthly micropollutant fluxes inputs (tributaries and the Upper Rhône River) compared to the output (Beaucaire station) claims for the presence of highly contaminated missing sources of micropollutants in the Rhône River watershed. Based on a SPM-flux-averaged micropollutant concentrations mass balance of the system and the estimates of the relative uncertainty of the missing sources concentration, we assessed their location within the Rhône River catchment. We assume that the potential missing sources of PAHs, PCBi and TME would be, respectively, the metropolitan areas, the alluvial margins of the Rhône River valley, and the unmonitored Cevenol tributaries.

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.

Estimating and restoring bedload transport through a run-of-river reservoir.

Weirs or run-of-river dams can disrupt bedload transfer with negative ecological effects downstream due to sediment starvation. The way and the degree to which bedload is trapped is nevertheless not straightforward and few studies have examined this topic. This study focuses on a 13-km-long reservoir of the Rhône River, France, created by a diversion dam equipped with bottom gates. Our main objective was to determine the degree of alteration of the bedload transfer downstream and to identify to which extent the implementation of Ecomorphogenic Flows (EmF), defined as environmental flows whose objective is specifically to increase bedload transfer through the reservoir to promote downstream habitat diversity, could increase bed mobility. The results show that the potential for morphological adjustments in the reservoir was already low before dam completion (1968) in response to a substantial decrease in coarse sediment supply, but that this potential was progressively reduced due to the impoundment. However, the bedload transfer continuity has been at least partially maintained since dam completion. According to numerical simulations, only particles smaller than medium gravels (d < 14 mm) could be exported downstream of the dam for relatively rare discharge (50-years return-interval flood). Implementation of EmF could neatly improve the bedload transfer since it would allow to strongly increase the competence: for a 2-years and a 50-years return-interval floods, the maximum particle size exportable downstream is respectively 9 and 4 times larger than for normal the reservoir operation.

Combining flux monitoring and data reconstruction to establish annual budgets of suspended particulate matter, mercury and PCB in the Rhône River from Lake Geneva to the Mediterranean Sea.

Long term and high resolution data on water discharge, suspended particulate matter (SPM) and contaminant concentrations in rivers are required for a better understanding of particulate transfers from the continental areas to the seas. The aim of this study was to provide a novel estimation of annual fluxes of SPM and related pollutants in the Rhône River from Lake Geneva to the Mediterranean Sea by combining high frequency or time-integrative monitoring and novel relations between SPM concentration (Cs) and water discharge (Q). At six stations of the Rhône Sediment Observatory (OSR), SPM fluxes were calculated over the 2000-2016 period by combining observational data and Cs-Q relations. Monthly average concentrations of mercury (Hg) and PCB 180 were obtained by analysis of SPM samples collected in time integrative particle traps between 2011 and 2016. These pollutants were selected because of the well documented contamination of the Rhône watershed by these substances. Inter-annual fluxes at the Rhône River outlet averaged 6.6 Mt. yr-1 for SPM, 572 kg yr-1 for Hg and 14 kg yr-1 for PCB 180. The Isère and Durance tributaries were found to be the main contributors of SPM fluxes. Annual SPM budgets were not balanced, suggesting deposition, remobilization of bottom sediments and/or contributions from non-monitored tributaries. The SPM sampled at the outlet was more contaminated than the combined SPM inputs from the monitored tributaries, suggesting that intermediate sources of contamination were not captured in the budget.