Understanding how water and solutes enter and propagate through freshwater landscapes in the Anthropocene is critical to protecting and restoring aquatic ecosystems and ensuring human water security. However, high hydrochemical variability in headwater streams, where most carbon and nutrients enter river networks, has hindered effective modelling and management. We developed an analytical framework informed by landscape ecology and catchment hydrology to quantify spatiotemporal variability across scales, which we tested in 56 headwater catchments, sampled periodically over 12 years in western France. Unexpectedly, temporal variability in dissolved carbon, nutrients and major ions was preserved moving downstream and spatial patterns of water chemistry were stable on annual to decadal timescales, partly because of synchronous variation in solute concentrations. These findings suggest that while concentration and flux cannot be extrapolated among subcatchments, periodic sampling of headwaters provides valuable information about solute sources and subcatchment resilience to disturbance.

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The binding of rare earth elements (REE) to humic acid (HA) was studied by combining ultrafiltration and Inductively Coupled Plasma Mass Spectrometry techniques. REE­HA complexation experiments were performed at various pH conditions (ranging from 2 to 10.5) using a standard batch equilibration method. Results show that the amount of REE bound to HA strongly increases with increasing pH. Moreover, a Middle-REE (MREE) downward concavity is evidenced by REE distribution patterns at acidic pH. Modelling of the experimental data using Humic Ion Binding Model VI provided a set of log KMA values (i.e., the REE­HA complexation constants specific to Model VI) for the entire REE series. The log KMA pattern obtained displays a MREE downward concavity. Log KMA values range from 2.42 to 2.79. These binding constants are in good agreement with the few existing datasets quantifying the binding of REE with humic substances but quite different from a recently published study which evidence a lanthanide contraction effect (i.e., continuous increase of the constant from La to Lu). The MREE downward concavity displayed by REE­HA complexation pattern determined in this study compares well with results from REE­fulvic acid (FA) and REE­acetic acid complexation studies. This similarity in the REE complexation pattern suggests that carboxylic groups are the main binding sites of REE in HA. This conclusion is further illustrated by a detailed review of published studies for natural, organic-rich, river- and ground-waters which show no evidence of a lanthanide contraction effect in REE pattern. Finally, application of Model VI using the new, experimentally determined log KMA values to World Average River Water confirms earlier suggestions that REE occur predominantly as organic complexes (= 60%) in the pH range between 5­5.5 and 7­8.5 (i.e., in circumneutral pH waters). The only significant difference as compared to earlier model predictions made using estimated log KMA values is that the experimentally determined log KMA values predict a significantly higher amount of Light-REE bound to organic matter under alkaline pH conditions

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International audienceIncreasing dissolved organic carbon (DOC) concentrations have been reported during the last 15 years in streams from the United Kingdom, Northern Europe and North America. Identifying the sources of DOC and the controls of the delivery to the stream is important to understand the significance of these trends. This relies on the availability of observations of DOC dynamics during storm events, since much of the DOC export from soils to streams occurs during high flows. This study analyses DOC data for eight storm events during winter 2005-2006 in a small agricultural experimental catchment - the Kervidy-Naizin experimental catchment - located in Western France. A four end-member mixing approach was applied to the eight monitored storm events to identify DOC sources and quantify their respective contribution to DOC stream fluxes, using DOC, nitrate, sulphate and chloride as tracers. The results show that DOC concentrations in the stream at the outlet of this catchment increase markedly during storm events. The slope of the linear regression between DOC concentration and discharge was not constant for the eight events and depended on pre-event hydrological conditions. Between 64 and 86% of the DOC that enter the stream during storms originated from the upper layers of the riparian wetland soils. The variation of the delivery of DOC seems to be controlled by hydrological processes only, the wetland soils acting as a non-limiting store

[1] To obtain better constraints on the control of seasonal hydrological variations on dissolved organic carbon (DOC) dynamics in headwater catchments, we combined hydrometric monitoring with high-frequency analyses of DOC concentration and DOC chemical composition (specific UV adsorption, 13 C) in soil and stream waters during one complete hydrological cycle in a small lowland catchment of western France. We observed a succession of four hydrological periods, each corresponding to specific DOC signatures. In particular, the rise of the upland water table at the end of the rewetting period yielded to a strong increase of the specific UV absorbance (from 2.5 to 4.0 L mg C À1 m À1 ) and of the 13 C values (from À29 to À27%) of the soil DOC. Another striking feature was the release of large amounts of DOC during reduction of soil Fe-oxyhydroxides at the end of the highflow period. Comparison of hydrometric data with DOC composition metrics showed that soils from the upland domains were rapidly DOC depleted after the rise of the water table in these domains, whereas wetland soils acted as quasi-infinite DOC sources. Results from this study showed that the composition and ultimate source of the DOC exported to the stream will depend on the period within the annual hydrological cycle. However, we found that the aromatic DOC component identified during the high-flow period will likely represent the dominant DOC component in stream waters on an annual basis, because most of the annual stream DOC flux is exported during such periods.Citation: Lambert, T., A.-C. Pierson-Wickmann, G. Gruau, A. Jaffrezic, P. Petitjean, J.-N Thibault, and L. Jeanneau (2013), Hydrologically driven seasonal changes in the sources and production mechanisms of dissolved organic carbon in a small lowland catchment, Water Resour. Res., 49,[5792][5793][5794][5795][5796][5797][5798][5799][5800][5801][5802][5803]

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